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Article Natural Recovery and Liming Eects in Acidified Forest Soils in SW-Germany Lelde Jansone *, Klaus von Wilpert and Peter Hartmann Department of Soil and Environment, Forest Research Institute of Baden-Württemberg, D-79100 Freiburg, Germany; [email protected] (K.v.W.); [email protected] (P.H.) * Correspondence: [email protected]; Tel.: +49-761-4018-217 Received: 15 May 2020; Accepted: 23 June 2020; Published: 30 June 2020 Abstract: In the state of Baden-Wuerttemberg, Southwest-Germany, a large-scale forest liming trial was government-funded in 1983 and a lime treatment was carried out in autumn 1983 until early winter 1984. Repeated liming was applied in 2003. The limed sites and adjacent control plots were surveyed repeatedly: in 2003 before the second lime application and again in 2010 and 2015. Research of this scope presents a rare opportunity to evaluate firstly the long-term development of acidified soils with their potential for natural recovery on established control plots, and secondly the long-term eects of repeated lime application—at a collective of study sites of various growth regions and soil properties. A natural recovery in soil pH was observed since 2003, on average limited to an increase of 0.2–0.4 pH units in the forest floor and 0.1–0.3 pH units in the mineral soil until 2015. The majority of the organic layers still show very strong or extreme acidity with a pH value 3.9 on average and in the mineral soil with pH values between 3.8 and 4.6 on average. The exchangeable cations calcium and magnesium slightly increased also, although the base saturation remained <20% by 2015. The exchangeable acid cation concentrations indicated no significant changes and thus no recovery. The lime treatment greatly accelerated the rise in pH by 1.2–1.3 units and base saturation by 40–70% in the organic layer, as well as 0.3–1.2 pH units and base saturation by 7–50% in mineral soil. These eects were decreasing (yet still significant) with depth in the measured soil profile as well as with time since last treatment. Changes in soil cation exchange capacity after liming were significant in 0–5 cm mineral soil, below that they were negligible as the significant increase in base cations were accompanied by decreasing acid cations aluminum and iron (III) especially in the upper soil profile. Additionally, a decrease of forest floor and an enrichment of organic carbon and nitrogen in the mineral topsoil tended to follow liming at some sites. Overall the liming eects had a high variability among the study sites, and were more pronounced in the more acidic and coarser textured sites. Liming of acidified forest soils significantly adds to natural recovery and therefore helps to establish greater buering capacities and stabilize forest nutrition for the future. Keywords: acid deposition recovery; forest soil; liming 1. Introduction Forest soils in Central Europe underwent acidification in the 20th century, which was primarily due to anthropogenic emissions of SO 2 and NO X that became acidic compounds in precipitation as well as dry deposition, and depletion of organic matter from topsoil [1,2]. In the 1970s–1980s a phenomenon of “forest dieback”—a new challenge due to deteriorating forest crown condition—was identified. Over time, several ecological eects of the acidifying agents sulfur, nitrogen as well as ozone have been identified: harmfully aected assimilation organs of trees, damaged tree roots with declining fine root biomass, changes in ectomycorrhizal associations and in fine root distributions, magnesium deficiencies in acidified soil and nutrient imbalances due to nitrogen eutrophication [35] Soil Syst. 2020, 4, 38; doi:10.3390/soilsystems4030038 www.mdpi.com/journal/soilsystems
Transcript
Page 1: Natural Recovery and Liming E ects in Acidified Forest ...

Article

Natural Recovery and Liming Effects in AcidifiedForest Soils in SW-Germany

Lelde Jansone Klaus von Wilpert and Peter Hartmann

Department of Soil and Environment Forest Research Institute of Baden-WuumlrttembergD-79100 Freiburg Germany klausvon-wilpertonlinede (KvW) PeterHartmannForstbwlde (PH) Correspondence LeldeJansoneForstbwlde Tel +49-761-4018-217

Received 15 May 2020 Accepted 23 June 2020 Published 30 June 2020

Abstract In the state of Baden-Wuerttemberg Southwest-Germany a large-scale forest liming trialwas government-funded in 1983 and a lime treatment was carried out in autumn 1983 until earlywinter 1984 Repeated liming was applied in 2003 The limed sites and adjacent control plots weresurveyed repeatedly in 2003 before the second lime application and again in 2010 and 2015 Researchof this scope presents a rare opportunity to evaluate firstly the long-term development of acidifiedsoils with their potential for natural recovery on established control plots and secondly the long-termeffects of repeated lime applicationmdashat a collective of study sites of various growth regions and soilproperties A natural recovery in soil pH was observed since 2003 on average limited to an increaseof 02ndash04 pH units in the forest floor and 01ndash03 pH units in the mineral soil until 2015 The majorityof the organic layers still show very strong or extreme acidity with a pH value 39 on average and inthe mineral soil with pH values between 38 and 46 on average The exchangeable cations calciumand magnesium slightly increased also although the base saturation remained lt20 by 2015 Theexchangeable acid cation concentrations indicated no significant changes and thus no recovery Thelime treatment greatly accelerated the rise in pH by 12ndash13 units and base saturation by 40ndash70 inthe organic layer as well as 03ndash12 pH units and base saturation by 7ndash50 in mineral soil Theseeffects were decreasing (yet still significant) with depth in the measured soil profile as well as withtime since last treatment Changes in soil cation exchange capacity after liming were significantin 0ndash5 cm mineral soil below that they were negligible as the significant increase in base cationswere accompanied by decreasing acid cations aluminum and iron (III) especially in the upper soilprofile Additionally a decrease of forest floor and an enrichment of organic carbon and nitrogenin the mineral topsoil tended to follow liming at some sites Overall the liming effects had a highvariability among the study sites and were more pronounced in the more acidic and coarser texturedsites Liming of acidified forest soils significantly adds to natural recovery and therefore helps toestablish greater buffering capacities and stabilize forest nutrition for the future

Keywords acid deposition recovery forest soil liming

1 Introduction

Forest soils in Central Europe underwent acidification in the 20th century which was primarilydue to anthropogenic emissions of SO2 and NOX that became acidic compounds in precipitationas well as dry deposition and depletion of organic matter from topsoil [12] In the 1970sndash1980s aphenomenon of ldquoforest diebackrdquomdasha new challenge due to deteriorating forest crown conditionmdashwasidentified Over time several ecological effects of the acidifying agents sulfur nitrogen as well asozone have been identified harmfully affected assimilation organs of trees damaged tree roots withdeclining fine root biomass changes in ectomycorrhizal associations and in fine root distributionsmagnesium deficiencies in acidified soil and nutrient imbalances due to nitrogen eutrophication [3ndash5]

Soil Syst 2020 4 38 doi103390soilsystems4030038 wwwmdpicomjournalsoilsystems

Soil Syst 2020 4 38 2 of 33

(p 30) Earthwormsmdashimportant ecosystem engineersmdashare also known to avoid acidic (pH lt 36) andhigh aluminum content soils [6] The overall functioning of the forest ecosystems has been shown tobe impeded in acidified conditions [7]

The acid-base status of forest soils is typically evaluated by the pH base saturation and reciprocalto it the exchangeable acid cations Al Fe Mn and H Acidified soils experience a reduction in theirnatural acid neutralization capacity (ANC) as the pH decreases and with it the soilsrsquo buffering rangeshifts [8] For forest soils in Southwest Germany a distinct change of pH values between the years1927 and 1997 was reported with a pH reduction of up to 2 pH units in the top-soils [9] Manysoils have left the silicate buffer range and reached pH values buffered by aluminum-oxides andaluminum-hydroxides with potentially adverse effects on plant roots and soil organisms as well ashampered phosphorus availability [10ndash12] (pp 94ndash96) Since the long-term buffering of acids in soilsdepends on the weathering rate of primary minerals in carbonate-free soils the base cations Ca Mg Kand Namdashalso important tree nutrientsmdashare being released from silicate and clay minerals and leachedleading to further nutrient imbalances in already base poor soils [813]

Due to legislative measures such as the Convention on Long-Range Transboundary Air Pollution ofthe United Nations Economic Commission for Europe [14] the emissions of SO2 have been successfullyreduced however a legacy of S compounds is still stored in soil and delays the recovery fromacidification On the other hand in many regions the deposition on N compounds NO3- and NH4+

remains high and continues to impact the forest ecosystems Meanwhile also Ca and Mg depositionrates have been decreasing [21315] Forest soil inventories in Germany prove that soil acidificationstill is an ongoing process with decreasing base saturations in the mineral subsoil (below 5 cm) whilepH values showed a slight recovery in the topsoils and no changes in the subsoils at unlimed sites [12](pp 93ndash116)

Since natural soil development and in this case recovery is expected to be a slow processforest soil liming may be an effective counter-measure to help alleviate the consequences of soilacidification [16] Liming is the application of buffering compoundsmdashmost commonly calcite (calciumcarbonate limestone and CaCO3) and dolomite (CaMg(CO3)2)mdashin order to restore acid depositionimpaired soils [17] In Finland and Sweden liming was studied extensively already in 1950s for itspotential to accelerate N-mineralization in the organic soil [18] In Germany lime application has beena wide-spread forestry practice since the mid-1980s to compensate acid inputs and remediate acidifiedsoils in order to improve the forest stand vitality [5] (pp 38ndash39) A great number of studies haveattempted to characterize the effects of liming In a meta-study on liming and wood-ash treatmenteffects on forest ecosystems Reid and Watmough [17] showed that the most significant impacts ofliming were on soil pH and foliar Ca concentrations best predicted by the soil type and time sincetreatment and by the treatment dose and type respectively Other important indicators of limingsuccess were base-saturation as well as various tree growth measures Meanwhile a number of studiesreported no significant liming effect at all Šraacutemek et al [19] showed significant increase of soil pHas well as exchangeable Ca and Mg up to five years after liming in upper soil horizons with theeffect decreasing ten years after treatment Ouimet and Moore [20] found similar effects seven yearsafter liming along with a slight decrease in exchangeable K and strongly decreased exchangeableaciditymdashwith an increased lime dose In a study that found increased soil profile pH as well as changesin sorption complex of the forest floor 16 years since last liming Draacutepelovaacute et al [10] pointed out therole of site soil properties climate and tree species composition in the outcome of liming in a studywhich found increased soil profile pH as well as changes in sorption complex of the forest floor 16 yearssince treatment Saarsalmi et al [18] showed decreased acidity and improved base saturation in theorganic layer and topsoil of Norway spruce and Scots pine stands even 20 years after liming SimilarlyCourt et al [13] observed a trend of increased pH base saturation Ca Mg as well as decreasingexchangeable Al more than 20 years after lime application in beech stands Increased tree growth wasalso noted in this study likely due to the improved soil chemical and biological properties even 40years after In Germany the results of the second national forest soil inventory (NFSI) of 2006ndash2008 also

Soil Syst 2020 4 38 3 of 33

showed overall positive liming effects on forest soil acid-base as well as nutrient status since the firstsurvey in 1987ndash1992 noting also a decrease in N stocks in the organic layer with an increase in the0ndash30 cm mineral soil [21] (p 157) This observation was attributed to increased soil pH stimulating themicrobial activity and decomposition of organic matter with no notable change in the CN ratio

Thus the relevance of forest liming lies in its potential to both restore and preserve the sustainabilityof soilsrsquo functionality acid buffer capacity nutrient supply for forest growth leading to improvedstructural integrity of the ecosystem Meanwhile as the acid deposition distinctly decreased since the1980s it might currently be sufficiently counteracted and buffered by natural soil weathering wherebya trend reversal from deposition driven acidification to a natural recovery might have taken placeWith this in mind the soil chemical parameters and their temporal development were studied at tenlong-term lime treated research sites in the Southwest-German state of Baden-Wuerttemberg in orderto answer the following questions

1 Has natural recovery of acidified forest soils taken place since 1980s and to what extent2 Has liming been an effective counter-measure to forest soil acidification3 What site parameters dictate the extent of change in soil acidity status in case of (1) and (2)

2 Materials and Methods

21 Site Description

The ten study sites are located in the SW-German state of Baden-Wuerttemberg first describedby Littek [22] (pp 1ndash8 14) and Wilpert et al [23] (pp 1 7ndash22) They were initially selected in 1983according to the following criteria porous non-waterlogged severely acidified soils on sandstonesubstrates in the regions of Black Forest Forest of Odes and Neckarland as well as on Pleistocenedeposits in Alpine foothills with larger homogeneous stands (10ndash50 ha) of Norway spruce (Picea abies)in pure stands or mixed with Silver fir (Abies alba) Scots pine (Pinus sylvestris) Douglas fir (Pseudotsugamenziesii) and European beech (Fagus sylvatica) with the age of the stand being 40ndash90 years Excludedwere the areas of nature conservation water protection special biotopes (eg capercaillie habitats)protected forests other study sites as well as previously limed areas With regard to the tree vitalityseverely damaged stands with tree needle loss gt40 were also excluded from selection Directlyadjacent to an untreated ldquocontrolrdquo plot a ldquolimedrdquo plot was established by applying a calcium carbonateCaCO3 in mixture with 4ndash8 MgO 3 P2O5 and 6ndash10 K2O (ldquoKohlensaurer Kalk 121123127rdquo limegrade 95 lt 315 mm and 70 lt 10 mm) from autumn 1983 until early winter 1984 The dose wasestablished site-specific according to the pH humus form and tree species surveyed in 1983 and wasno higher than 35 Mg haminus1 in most cases between 25 and 3 Mg haminus1 This comparably low dosagewas chosen in order to avoid overly high mobilization of the humus layer and undesirable nutrientleaching in the groundwater and surface waters This also meant that any changes in the soil aciditystatus were expected to progress slowly over several years

In 2003 a second treatment of 6 Mg haminus1 dolomite lime with 55 CaCO3 and 35 MgCO3

(ldquoCaMg(CO3)2 5535rdquo lime grade 90 lt 01 mm) was applied The dolomite lime was seen to bufferacid deposition effectively and to react slower than the previously applied calcium carbonate mixturewith milder effects on humus and was therefore chosen to be applied in larger doses

It is important to note that the study sites have been considered as praxis-fertilization trialsmeaning that the scientific investigations have accompanied the regular forest management practices(moderate thinning of stands storm damage response natural regeneration or planting etc) A recentcomprehensive inventory of these sites was conducted in 2015 and their updated description is shownin Table 1 A map of study site locations is shown in Appendix A (Figure A1)

Soil Syst 2020 4 38 4 of 33

Table 1 Study sites and their key parameters in 2015

SiteLatitude

()Longitude

()Altitude(m asl)

Plot Size (ha)Substrate Soil Type 1 Texture 2 Humus

Type 3StandType 4

StandAge Grouping 5

Control Limed

BadWaldsee 4750prime 941prime 580 4 22 Glacial till cambisol LS

mull -modermull

PI-FA 70 G1

Ellwangen 4901prime 1010prime 490 10 15 Sandstone stagnosol SL mull PI 100 G1Freuden-

stadt 4826prime 825prime 740 8 21 Sandstone cambisol SL mull - mormoder AB-PI 100 G1

Heidelberg 4930prime 847prime 490 2 3 Sandstone podsol SL mull PI 70 G1

Ochsen-hausen 4806prime 1002prime 620 5 17 Periglacial

gravel cambisol Lmull -modermull

PI 90 G1

Herzogen-weiler 4801prime 820prime 950 8 20 Sandstone stagnosol LS-SL

mull -modermull

AB-PI 90 G2

Horb 4828prime 832prime 630 8 21 Sandstone cambisol LS mull AB-PI 100 G2

Hospital 4807prime 941prime 650 3 5 Glacial till stagnosol SiL-L mull - mormoder PI-FA 110 G2

Wangen 4747prime 945prime 710 6 22 Glacial till umbrisol SiL-L mormoder PI 100 G2

Weithard 4758prime 917prime 630 1 6 Glacial till stagnosol CL-L mull - mormoder PI 100 G2

1 dominating soil type according to FAO 2014 (World Reference Base For Soil Classification) 2 mean textural classes according to FAO [24] (pp 25ndash29) LS = Loamy sand SL = Sandy loamL = Loam SiL = Silty loam CL = Clay loam 3 dominating humus forms according to Ad-hoc-Arbeitsgruppe Boden (German soil classification) [25] (pp 303ndash310) 4 PI = Picea abies AB-PI= mixed Abies alba and Picea abies PI-FA= mixed Picea abies and Fagus sylvatica 5 Grouping according to K-means Cluster Analysis (see statistical analyses)

Soil Syst 2020 4 38 5 of 33

22 Soil Sampling and Laboratory Methods

The sampling methods of the different sampling periods of 1985ndash2015 are described in Table 2

Table 2 Soil sampling design in the 1980s (as described in Wilpert et al [23]) 2003 2010 and 2015

198586 and 1989 2003 2010 2015

Sample layoutwithin plot

3-10 (O-layer) and6ndash10 (mineral soil)samples in 10 mdistance along a

random diagonalline

1 sample at 5randomly distributedpoints plus 5 samplesat 0 80 160 240 and320 gradian in 5 mdistance from a soil

profile

1 sample at 5randomly

distributed points

1 sample at 5randomly

distributed points

Sampled soillayers

O-layer a

0ndash4 cm b

5ndash10 cm a

O-layer c

0ndash5 cm d

5ndash10 cm d

10ndash30 cm d

30ndash60 cm d

O-layer c

0ndash5c m d

5ndash10 cm d

10ndash30 cm d

30ndash60 cm d

O-layer c

0ndash5 cm d

5ndash10 cm d

10ndash20 cm d

20ndash30 cm d

30ndash60 cm d

Instrumenta scraper

b 100 cm3 soilsample ring

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8 cm

length 15 cm)

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8cm length 15 cm)

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8cm length 15 cm)

No of replicates 1 mixed sample 1 mixed sample 4 individualsamples

5 individualsamples

The first sampling period was 1985 and 1986 a further sampling campaign was completed in198990 Three to ten samples of O-layer and six to ten samples of the mineral soil were collected and thenmixed into a single sample for the laboratory analysis The results comparing the development at controland limed plots between these two sampling campaigns have been published in Wilpert et al [23](pp 30ndash45) The control plot pH-KCl in mineral topsoil was pH 30 ie in the Al and Al-Fe bufferrange meanwhile at limed plots it had increased by average 09 pH units in 198586 and 02 pH unitsby 198990 in 0ndash4 cm topsoil while in 4ndash10 cm topsoil only by 198990 an increase by 02 pH unitswas observed The pH-H2O was reported to be 05ndash1 pH units higher than pH-KCl with 10ndash20 lesschange after treatment While at control plots the O-layer thickness tended to increase at limed plots ithad decreased and liming had increased the variability of C-content in 4ndash10 cm mineral soil with littlechange in average C-content Control plot exchangeable cations (CEC) and exchangeable cations wereanalyzed only in 198990 samples where base saturation improved significantly by 17 after limetreatment (though with high variance) especially exchangeable Ca and slightly less exchangeable Mgwith little change in exchangeable K Meanwhile exchangeable Al and H had decreased Limed plotCEC had overall increased by 14

The second sampling was carried out in April until October 2003 ie twenty years after thefirst liming and before the second treatment campaign A soil sample per depth class was taken atfive randomly distributed points across a plot as well as in five directions from an established soilprofile then mixed into a single sample In MarchndashOctober 2010mdashseven years after the second limingeventmdashsoil sampling was done at four randomly distributed points per treatment plot The final soilsampling campaign was carried out in March until June 2015mdashtwelve years since the second limeapplicationmdashat five randomly distributed points per plot

The soil samples were dried at 60 C and ground in a mill with a 2 mm sieveThe following soil chemical parameters were considered in our investigation pH-H2O and

pH-KCl were measured with a glass electrode in 15 (mineral soil) and 110 (O-layer) solution withH2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (micromolc gminus1) and theirsum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation

Soil Syst 2020 4 38 6 of 33

() were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OEStotal N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al andFe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1)were calculated form dried soil samples of defined sampled area The methodology of our laboratoryanalyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA)by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as TablesS1ndashS3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different samplingperiods at the study sites and therefore the element concentrations may be directly comparedbetween the sampling years and between the directly adjacent treatment variants without consideringelement stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pHvalues were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversioninto pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volumeweight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019)First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity

of sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated samplingcampaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations werecalculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimalnumber of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBadWaldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 thesites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionallya principal component analysis (PCA) was run in order to confirm the CA results as well as determinethe most relevant soil chemical principal components (PC) of these site groups The first two PCsexplained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot

(t haminus1) and CEC (micromolc gminus1 PC-2 Figure 1)Group 1 (G1) includes the sites with predominantly ldquosandy soilsrdquo and is characterized with lower

CEC lower Ctot stocks lower K+ stocks and higher Al3+ stocks in the upper mineral soil comparedto Group 2 (G2) of predominantly finer textured ldquosiltyclay loam soilsrdquo For both study site groupspH-H2O of 40ndash44 was similar in 0-30 cm mineral soil whereas pH-KCl was 33ndash36 at G1 and 35ndash37at G2 sites ie comparably higher

The statistical analysis was applied to both site groups separately Due to small sample size in thesampling campaigns (n lt 30 per depth class) as well as a lack of normal distribution in some of thedata non-parametric statistical tests were chosen In order to compare the difference in group-meansbetween sampling years (separately for control and lime treatments) Friedman test for repeated(dependent) measurements was applied To find differences between control and lime treatmentswithin a sampling year MannndashWhitney U test for independent samples was used The significancelevel was chosen p lt 005

Soil Syst 2020 4 38 7 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 6 of 35

H2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (μmolc gminus1) and their sum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation () were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OES total N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000 in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al and Fe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1) were calculated form dried soil samples of defined sampled area The methodology of our laboratory analyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA) by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as Table S1 S2 and S3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different sampling periods at the study sites and therefore the element concentrations may be directly compared between the sampling years and between the directly adjacent treatment variants without considering element stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into 10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pH values were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversion into pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volume weight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019) First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity of

sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated sampling campaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations were calculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimal number of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBad Waldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 the sites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionally a principal component analysis (PCA) was run in order to confirm the CA results as well as determine the most relevant soil chemical principal components (PC) of these site groups The first two PCs explained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot (t haminus1) and CEC (μmolc gminus1 PC-2 Figure 1)

(a)

(b)

Figure 1 Principal component analysis (PCA) to characterize study site grouping parameters (a) studysites and (b) principal components

To estimate the natural recovery as well as the effects of lime application over time ie thedifference between two sampling periods within a study site group a relative response ratio (RRr) wascalculated for each of the relevant site parameters based on methodology in Hedges et al [29] andReid and Watmough [17]

RRr = (t2t1) minus 1 (1)

where t1 = site plot average (arithmetic mean) in previous sampling period t2 = site plot average infollowing sampling period In case of already relative (CN) log-transformed (pH) and discontinuous(base saturation) variables an absolute RRa was calculated as difference between previous and followingsampling year or limed and control treatment

RRa = t2 minus t1 (2)

3 Results

Since the 1980s sampling design and data set was not comparable with the subsequent campaignsfrom 2003 until 2015 we were not able to analyze statistically the changes in soil chemical propertiesof the entire measured soil profile of our studied sites for the period 1980s until 2003 Neverthelesswith the sampling data of 2003 we can evaluate the liming effects in this initial study period on soilproperties with the direct comparison of control and limed plots From 2003 on we can describe thedevelopment of soil chemical properties with respect to liming effects in great detail In this contextwe will first of all present the changes in soil acidity status with focus on pH values base saturationand cation exchange capacities as well as the exchangeable cations concentrations Secondly thedevelopment of soil nutrient status with focus on carbon and nitrogen are outlined A complete list ofparameter means (with standard deviations) as they developed over time and after lime treatment isavailable as Table S4 (G1) and S5 (G2) in Supplementary Materials The parameter response ratio (RR)means SD and ranges are fully detailed in Tables S6 (G1) and S7 (G2) of Supplementary Materials

31 Liming Effects in 2003

In 2003mdashtwenty years after the first lime treatment in 1983mdashno significant differences could beseen in soil pH or base saturation between the control and limed plots The mean values at limed plotstended to be higher for both parameters especially in the O-layer (pH) and 0ndash5 cm mineral soil (BS)

Soil Syst 2020 4 38 8 of 33

however the confidence intervals of both control and lime treatment overlap Similarly sum CECby 2003 was comparable throughout the entire soil profile also G2 site 0ndash5 cm mineral soil sampleexchangeable Ca as well as Ctot and Ntot were significantly increasedmdasha potential residual effect oflime application in 1983mdashyet even here the increase in CEC was only slight and not significant G1 sitelimed plot O-layer total Al and total Fe concentrations were significantly higher compared to controlalthough again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in theentire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer andfrom pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pHunits) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pHunits) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however thisrecovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layerand from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

Soil Syst 2020 4 x FOR PEER REVIEW 8 of 35

significant G1 site limed plot O-layer total Al and total Fe concentrations were significantly higher compared to control although again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in the entire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer and from pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in 0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pH units) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pH units) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however this recovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layer and from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1 and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pH units at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010 and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots with group average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in the O-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the difference between the control and limed plots was significant in all G1 measured soil profile depths in 2010 the treatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 years since the last lime application At G2 sites the liming effect reached significance only down to 10 cm mineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

(a)

(b)

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites(b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 38 9 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 9 of 35

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Similar development in both natural recovery and liming effects over time was seen also in pH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronounced in the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect only down to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen across all study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) The average RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in 2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below 20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significant increase in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime application This liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa 4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the 0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in both the 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pHunits at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots withgroup average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in theO-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the differencebetween the control and limed plots was significant in all G1 measured soil profile depths in 2010 thetreatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 yearssince the last lime application At G2 sites the liming effect reached significance only down to 10 cmmineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

Similar development in both natural recovery and liming effects over time was seen also inpH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronouncedin the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect onlydown to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen acrossall study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) Theaverage RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in

Soil Syst 2020 4 38 10 of 33

2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significantincrease in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime applicationThis liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa

4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in boththe 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just a 1ndash3 increasein group average BS Compared to the control plots both G1 and G2 limed plot BS was significantlyhigher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plotbase saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and9ndash12 in 30ndash60 cm mineral soil

Soil Syst 2020 4 x FOR PEER REVIEW 10 of 35

a 1ndash3 increase in group average BS Compared to the control plots both G1 and G2 limed plot BS was significantly higher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80 in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plot base saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and 9ndash12 in 30ndash60 cm mineral soil

(a)

(b)

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 studysites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differencesbetween current and previous sampling campaign

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 2: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 2 of 33

(p 30) Earthwormsmdashimportant ecosystem engineersmdashare also known to avoid acidic (pH lt 36) andhigh aluminum content soils [6] The overall functioning of the forest ecosystems has been shown tobe impeded in acidified conditions [7]

The acid-base status of forest soils is typically evaluated by the pH base saturation and reciprocalto it the exchangeable acid cations Al Fe Mn and H Acidified soils experience a reduction in theirnatural acid neutralization capacity (ANC) as the pH decreases and with it the soilsrsquo buffering rangeshifts [8] For forest soils in Southwest Germany a distinct change of pH values between the years1927 and 1997 was reported with a pH reduction of up to 2 pH units in the top-soils [9] Manysoils have left the silicate buffer range and reached pH values buffered by aluminum-oxides andaluminum-hydroxides with potentially adverse effects on plant roots and soil organisms as well ashampered phosphorus availability [10ndash12] (pp 94ndash96) Since the long-term buffering of acids in soilsdepends on the weathering rate of primary minerals in carbonate-free soils the base cations Ca Mg Kand Namdashalso important tree nutrientsmdashare being released from silicate and clay minerals and leachedleading to further nutrient imbalances in already base poor soils [813]

Due to legislative measures such as the Convention on Long-Range Transboundary Air Pollution ofthe United Nations Economic Commission for Europe [14] the emissions of SO2 have been successfullyreduced however a legacy of S compounds is still stored in soil and delays the recovery fromacidification On the other hand in many regions the deposition on N compounds NO3- and NH4+

remains high and continues to impact the forest ecosystems Meanwhile also Ca and Mg depositionrates have been decreasing [21315] Forest soil inventories in Germany prove that soil acidificationstill is an ongoing process with decreasing base saturations in the mineral subsoil (below 5 cm) whilepH values showed a slight recovery in the topsoils and no changes in the subsoils at unlimed sites [12](pp 93ndash116)

Since natural soil development and in this case recovery is expected to be a slow processforest soil liming may be an effective counter-measure to help alleviate the consequences of soilacidification [16] Liming is the application of buffering compoundsmdashmost commonly calcite (calciumcarbonate limestone and CaCO3) and dolomite (CaMg(CO3)2)mdashin order to restore acid depositionimpaired soils [17] In Finland and Sweden liming was studied extensively already in 1950s for itspotential to accelerate N-mineralization in the organic soil [18] In Germany lime application has beena wide-spread forestry practice since the mid-1980s to compensate acid inputs and remediate acidifiedsoils in order to improve the forest stand vitality [5] (pp 38ndash39) A great number of studies haveattempted to characterize the effects of liming In a meta-study on liming and wood-ash treatmenteffects on forest ecosystems Reid and Watmough [17] showed that the most significant impacts ofliming were on soil pH and foliar Ca concentrations best predicted by the soil type and time sincetreatment and by the treatment dose and type respectively Other important indicators of limingsuccess were base-saturation as well as various tree growth measures Meanwhile a number of studiesreported no significant liming effect at all Šraacutemek et al [19] showed significant increase of soil pHas well as exchangeable Ca and Mg up to five years after liming in upper soil horizons with theeffect decreasing ten years after treatment Ouimet and Moore [20] found similar effects seven yearsafter liming along with a slight decrease in exchangeable K and strongly decreased exchangeableaciditymdashwith an increased lime dose In a study that found increased soil profile pH as well as changesin sorption complex of the forest floor 16 years since last liming Draacutepelovaacute et al [10] pointed out therole of site soil properties climate and tree species composition in the outcome of liming in a studywhich found increased soil profile pH as well as changes in sorption complex of the forest floor 16 yearssince treatment Saarsalmi et al [18] showed decreased acidity and improved base saturation in theorganic layer and topsoil of Norway spruce and Scots pine stands even 20 years after liming SimilarlyCourt et al [13] observed a trend of increased pH base saturation Ca Mg as well as decreasingexchangeable Al more than 20 years after lime application in beech stands Increased tree growth wasalso noted in this study likely due to the improved soil chemical and biological properties even 40years after In Germany the results of the second national forest soil inventory (NFSI) of 2006ndash2008 also

Soil Syst 2020 4 38 3 of 33

showed overall positive liming effects on forest soil acid-base as well as nutrient status since the firstsurvey in 1987ndash1992 noting also a decrease in N stocks in the organic layer with an increase in the0ndash30 cm mineral soil [21] (p 157) This observation was attributed to increased soil pH stimulating themicrobial activity and decomposition of organic matter with no notable change in the CN ratio

Thus the relevance of forest liming lies in its potential to both restore and preserve the sustainabilityof soilsrsquo functionality acid buffer capacity nutrient supply for forest growth leading to improvedstructural integrity of the ecosystem Meanwhile as the acid deposition distinctly decreased since the1980s it might currently be sufficiently counteracted and buffered by natural soil weathering wherebya trend reversal from deposition driven acidification to a natural recovery might have taken placeWith this in mind the soil chemical parameters and their temporal development were studied at tenlong-term lime treated research sites in the Southwest-German state of Baden-Wuerttemberg in orderto answer the following questions

1 Has natural recovery of acidified forest soils taken place since 1980s and to what extent2 Has liming been an effective counter-measure to forest soil acidification3 What site parameters dictate the extent of change in soil acidity status in case of (1) and (2)

2 Materials and Methods

21 Site Description

The ten study sites are located in the SW-German state of Baden-Wuerttemberg first describedby Littek [22] (pp 1ndash8 14) and Wilpert et al [23] (pp 1 7ndash22) They were initially selected in 1983according to the following criteria porous non-waterlogged severely acidified soils on sandstonesubstrates in the regions of Black Forest Forest of Odes and Neckarland as well as on Pleistocenedeposits in Alpine foothills with larger homogeneous stands (10ndash50 ha) of Norway spruce (Picea abies)in pure stands or mixed with Silver fir (Abies alba) Scots pine (Pinus sylvestris) Douglas fir (Pseudotsugamenziesii) and European beech (Fagus sylvatica) with the age of the stand being 40ndash90 years Excludedwere the areas of nature conservation water protection special biotopes (eg capercaillie habitats)protected forests other study sites as well as previously limed areas With regard to the tree vitalityseverely damaged stands with tree needle loss gt40 were also excluded from selection Directlyadjacent to an untreated ldquocontrolrdquo plot a ldquolimedrdquo plot was established by applying a calcium carbonateCaCO3 in mixture with 4ndash8 MgO 3 P2O5 and 6ndash10 K2O (ldquoKohlensaurer Kalk 121123127rdquo limegrade 95 lt 315 mm and 70 lt 10 mm) from autumn 1983 until early winter 1984 The dose wasestablished site-specific according to the pH humus form and tree species surveyed in 1983 and wasno higher than 35 Mg haminus1 in most cases between 25 and 3 Mg haminus1 This comparably low dosagewas chosen in order to avoid overly high mobilization of the humus layer and undesirable nutrientleaching in the groundwater and surface waters This also meant that any changes in the soil aciditystatus were expected to progress slowly over several years

In 2003 a second treatment of 6 Mg haminus1 dolomite lime with 55 CaCO3 and 35 MgCO3

(ldquoCaMg(CO3)2 5535rdquo lime grade 90 lt 01 mm) was applied The dolomite lime was seen to bufferacid deposition effectively and to react slower than the previously applied calcium carbonate mixturewith milder effects on humus and was therefore chosen to be applied in larger doses

It is important to note that the study sites have been considered as praxis-fertilization trialsmeaning that the scientific investigations have accompanied the regular forest management practices(moderate thinning of stands storm damage response natural regeneration or planting etc) A recentcomprehensive inventory of these sites was conducted in 2015 and their updated description is shownin Table 1 A map of study site locations is shown in Appendix A (Figure A1)

Soil Syst 2020 4 38 4 of 33

Table 1 Study sites and their key parameters in 2015

SiteLatitude

()Longitude

()Altitude(m asl)

Plot Size (ha)Substrate Soil Type 1 Texture 2 Humus

Type 3StandType 4

StandAge Grouping 5

Control Limed

BadWaldsee 4750prime 941prime 580 4 22 Glacial till cambisol LS

mull -modermull

PI-FA 70 G1

Ellwangen 4901prime 1010prime 490 10 15 Sandstone stagnosol SL mull PI 100 G1Freuden-

stadt 4826prime 825prime 740 8 21 Sandstone cambisol SL mull - mormoder AB-PI 100 G1

Heidelberg 4930prime 847prime 490 2 3 Sandstone podsol SL mull PI 70 G1

Ochsen-hausen 4806prime 1002prime 620 5 17 Periglacial

gravel cambisol Lmull -modermull

PI 90 G1

Herzogen-weiler 4801prime 820prime 950 8 20 Sandstone stagnosol LS-SL

mull -modermull

AB-PI 90 G2

Horb 4828prime 832prime 630 8 21 Sandstone cambisol LS mull AB-PI 100 G2

Hospital 4807prime 941prime 650 3 5 Glacial till stagnosol SiL-L mull - mormoder PI-FA 110 G2

Wangen 4747prime 945prime 710 6 22 Glacial till umbrisol SiL-L mormoder PI 100 G2

Weithard 4758prime 917prime 630 1 6 Glacial till stagnosol CL-L mull - mormoder PI 100 G2

1 dominating soil type according to FAO 2014 (World Reference Base For Soil Classification) 2 mean textural classes according to FAO [24] (pp 25ndash29) LS = Loamy sand SL = Sandy loamL = Loam SiL = Silty loam CL = Clay loam 3 dominating humus forms according to Ad-hoc-Arbeitsgruppe Boden (German soil classification) [25] (pp 303ndash310) 4 PI = Picea abies AB-PI= mixed Abies alba and Picea abies PI-FA= mixed Picea abies and Fagus sylvatica 5 Grouping according to K-means Cluster Analysis (see statistical analyses)

Soil Syst 2020 4 38 5 of 33

22 Soil Sampling and Laboratory Methods

The sampling methods of the different sampling periods of 1985ndash2015 are described in Table 2

Table 2 Soil sampling design in the 1980s (as described in Wilpert et al [23]) 2003 2010 and 2015

198586 and 1989 2003 2010 2015

Sample layoutwithin plot

3-10 (O-layer) and6ndash10 (mineral soil)samples in 10 mdistance along a

random diagonalline

1 sample at 5randomly distributedpoints plus 5 samplesat 0 80 160 240 and320 gradian in 5 mdistance from a soil

profile

1 sample at 5randomly

distributed points

1 sample at 5randomly

distributed points

Sampled soillayers

O-layer a

0ndash4 cm b

5ndash10 cm a

O-layer c

0ndash5 cm d

5ndash10 cm d

10ndash30 cm d

30ndash60 cm d

O-layer c

0ndash5c m d

5ndash10 cm d

10ndash30 cm d

30ndash60 cm d

O-layer c

0ndash5 cm d

5ndash10 cm d

10ndash20 cm d

20ndash30 cm d

30ndash60 cm d

Instrumenta scraper

b 100 cm3 soilsample ring

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8 cm

length 15 cm)

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8cm length 15 cm)

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8cm length 15 cm)

No of replicates 1 mixed sample 1 mixed sample 4 individualsamples

5 individualsamples

The first sampling period was 1985 and 1986 a further sampling campaign was completed in198990 Three to ten samples of O-layer and six to ten samples of the mineral soil were collected and thenmixed into a single sample for the laboratory analysis The results comparing the development at controland limed plots between these two sampling campaigns have been published in Wilpert et al [23](pp 30ndash45) The control plot pH-KCl in mineral topsoil was pH 30 ie in the Al and Al-Fe bufferrange meanwhile at limed plots it had increased by average 09 pH units in 198586 and 02 pH unitsby 198990 in 0ndash4 cm topsoil while in 4ndash10 cm topsoil only by 198990 an increase by 02 pH unitswas observed The pH-H2O was reported to be 05ndash1 pH units higher than pH-KCl with 10ndash20 lesschange after treatment While at control plots the O-layer thickness tended to increase at limed plots ithad decreased and liming had increased the variability of C-content in 4ndash10 cm mineral soil with littlechange in average C-content Control plot exchangeable cations (CEC) and exchangeable cations wereanalyzed only in 198990 samples where base saturation improved significantly by 17 after limetreatment (though with high variance) especially exchangeable Ca and slightly less exchangeable Mgwith little change in exchangeable K Meanwhile exchangeable Al and H had decreased Limed plotCEC had overall increased by 14

The second sampling was carried out in April until October 2003 ie twenty years after thefirst liming and before the second treatment campaign A soil sample per depth class was taken atfive randomly distributed points across a plot as well as in five directions from an established soilprofile then mixed into a single sample In MarchndashOctober 2010mdashseven years after the second limingeventmdashsoil sampling was done at four randomly distributed points per treatment plot The final soilsampling campaign was carried out in March until June 2015mdashtwelve years since the second limeapplicationmdashat five randomly distributed points per plot

The soil samples were dried at 60 C and ground in a mill with a 2 mm sieveThe following soil chemical parameters were considered in our investigation pH-H2O and

pH-KCl were measured with a glass electrode in 15 (mineral soil) and 110 (O-layer) solution withH2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (micromolc gminus1) and theirsum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation

Soil Syst 2020 4 38 6 of 33

() were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OEStotal N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al andFe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1)were calculated form dried soil samples of defined sampled area The methodology of our laboratoryanalyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA)by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as TablesS1ndashS3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different samplingperiods at the study sites and therefore the element concentrations may be directly comparedbetween the sampling years and between the directly adjacent treatment variants without consideringelement stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pHvalues were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversioninto pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volumeweight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019)First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity

of sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated samplingcampaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations werecalculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimalnumber of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBadWaldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 thesites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionallya principal component analysis (PCA) was run in order to confirm the CA results as well as determinethe most relevant soil chemical principal components (PC) of these site groups The first two PCsexplained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot

(t haminus1) and CEC (micromolc gminus1 PC-2 Figure 1)Group 1 (G1) includes the sites with predominantly ldquosandy soilsrdquo and is characterized with lower

CEC lower Ctot stocks lower K+ stocks and higher Al3+ stocks in the upper mineral soil comparedto Group 2 (G2) of predominantly finer textured ldquosiltyclay loam soilsrdquo For both study site groupspH-H2O of 40ndash44 was similar in 0-30 cm mineral soil whereas pH-KCl was 33ndash36 at G1 and 35ndash37at G2 sites ie comparably higher

The statistical analysis was applied to both site groups separately Due to small sample size in thesampling campaigns (n lt 30 per depth class) as well as a lack of normal distribution in some of thedata non-parametric statistical tests were chosen In order to compare the difference in group-meansbetween sampling years (separately for control and lime treatments) Friedman test for repeated(dependent) measurements was applied To find differences between control and lime treatmentswithin a sampling year MannndashWhitney U test for independent samples was used The significancelevel was chosen p lt 005

Soil Syst 2020 4 38 7 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 6 of 35

H2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (μmolc gminus1) and their sum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation () were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OES total N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000 in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al and Fe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1) were calculated form dried soil samples of defined sampled area The methodology of our laboratory analyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA) by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as Table S1 S2 and S3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different sampling periods at the study sites and therefore the element concentrations may be directly compared between the sampling years and between the directly adjacent treatment variants without considering element stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into 10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pH values were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversion into pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volume weight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019) First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity of

sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated sampling campaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations were calculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimal number of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBad Waldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 the sites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionally a principal component analysis (PCA) was run in order to confirm the CA results as well as determine the most relevant soil chemical principal components (PC) of these site groups The first two PCs explained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot (t haminus1) and CEC (μmolc gminus1 PC-2 Figure 1)

(a)

(b)

Figure 1 Principal component analysis (PCA) to characterize study site grouping parameters (a) studysites and (b) principal components

To estimate the natural recovery as well as the effects of lime application over time ie thedifference between two sampling periods within a study site group a relative response ratio (RRr) wascalculated for each of the relevant site parameters based on methodology in Hedges et al [29] andReid and Watmough [17]

RRr = (t2t1) minus 1 (1)

where t1 = site plot average (arithmetic mean) in previous sampling period t2 = site plot average infollowing sampling period In case of already relative (CN) log-transformed (pH) and discontinuous(base saturation) variables an absolute RRa was calculated as difference between previous and followingsampling year or limed and control treatment

RRa = t2 minus t1 (2)

3 Results

Since the 1980s sampling design and data set was not comparable with the subsequent campaignsfrom 2003 until 2015 we were not able to analyze statistically the changes in soil chemical propertiesof the entire measured soil profile of our studied sites for the period 1980s until 2003 Neverthelesswith the sampling data of 2003 we can evaluate the liming effects in this initial study period on soilproperties with the direct comparison of control and limed plots From 2003 on we can describe thedevelopment of soil chemical properties with respect to liming effects in great detail In this contextwe will first of all present the changes in soil acidity status with focus on pH values base saturationand cation exchange capacities as well as the exchangeable cations concentrations Secondly thedevelopment of soil nutrient status with focus on carbon and nitrogen are outlined A complete list ofparameter means (with standard deviations) as they developed over time and after lime treatment isavailable as Table S4 (G1) and S5 (G2) in Supplementary Materials The parameter response ratio (RR)means SD and ranges are fully detailed in Tables S6 (G1) and S7 (G2) of Supplementary Materials

31 Liming Effects in 2003

In 2003mdashtwenty years after the first lime treatment in 1983mdashno significant differences could beseen in soil pH or base saturation between the control and limed plots The mean values at limed plotstended to be higher for both parameters especially in the O-layer (pH) and 0ndash5 cm mineral soil (BS)

Soil Syst 2020 4 38 8 of 33

however the confidence intervals of both control and lime treatment overlap Similarly sum CECby 2003 was comparable throughout the entire soil profile also G2 site 0ndash5 cm mineral soil sampleexchangeable Ca as well as Ctot and Ntot were significantly increasedmdasha potential residual effect oflime application in 1983mdashyet even here the increase in CEC was only slight and not significant G1 sitelimed plot O-layer total Al and total Fe concentrations were significantly higher compared to controlalthough again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in theentire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer andfrom pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pHunits) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pHunits) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however thisrecovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layerand from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

Soil Syst 2020 4 x FOR PEER REVIEW 8 of 35

significant G1 site limed plot O-layer total Al and total Fe concentrations were significantly higher compared to control although again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in the entire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer and from pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in 0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pH units) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pH units) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however this recovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layer and from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1 and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pH units at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010 and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots with group average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in the O-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the difference between the control and limed plots was significant in all G1 measured soil profile depths in 2010 the treatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 years since the last lime application At G2 sites the liming effect reached significance only down to 10 cm mineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

(a)

(b)

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites(b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 38 9 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 9 of 35

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Similar development in both natural recovery and liming effects over time was seen also in pH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronounced in the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect only down to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen across all study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) The average RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in 2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below 20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significant increase in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime application This liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa 4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the 0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in both the 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pHunits at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots withgroup average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in theO-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the differencebetween the control and limed plots was significant in all G1 measured soil profile depths in 2010 thetreatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 yearssince the last lime application At G2 sites the liming effect reached significance only down to 10 cmmineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

Similar development in both natural recovery and liming effects over time was seen also inpH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronouncedin the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect onlydown to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen acrossall study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) Theaverage RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in

Soil Syst 2020 4 38 10 of 33

2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significantincrease in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime applicationThis liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa

4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in boththe 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just a 1ndash3 increasein group average BS Compared to the control plots both G1 and G2 limed plot BS was significantlyhigher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plotbase saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and9ndash12 in 30ndash60 cm mineral soil

Soil Syst 2020 4 x FOR PEER REVIEW 10 of 35

a 1ndash3 increase in group average BS Compared to the control plots both G1 and G2 limed plot BS was significantly higher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80 in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plot base saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and 9ndash12 in 30ndash60 cm mineral soil

(a)

(b)

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 studysites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differencesbetween current and previous sampling campaign

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 3: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 3 of 33

showed overall positive liming effects on forest soil acid-base as well as nutrient status since the firstsurvey in 1987ndash1992 noting also a decrease in N stocks in the organic layer with an increase in the0ndash30 cm mineral soil [21] (p 157) This observation was attributed to increased soil pH stimulating themicrobial activity and decomposition of organic matter with no notable change in the CN ratio

Thus the relevance of forest liming lies in its potential to both restore and preserve the sustainabilityof soilsrsquo functionality acid buffer capacity nutrient supply for forest growth leading to improvedstructural integrity of the ecosystem Meanwhile as the acid deposition distinctly decreased since the1980s it might currently be sufficiently counteracted and buffered by natural soil weathering wherebya trend reversal from deposition driven acidification to a natural recovery might have taken placeWith this in mind the soil chemical parameters and their temporal development were studied at tenlong-term lime treated research sites in the Southwest-German state of Baden-Wuerttemberg in orderto answer the following questions

1 Has natural recovery of acidified forest soils taken place since 1980s and to what extent2 Has liming been an effective counter-measure to forest soil acidification3 What site parameters dictate the extent of change in soil acidity status in case of (1) and (2)

2 Materials and Methods

21 Site Description

The ten study sites are located in the SW-German state of Baden-Wuerttemberg first describedby Littek [22] (pp 1ndash8 14) and Wilpert et al [23] (pp 1 7ndash22) They were initially selected in 1983according to the following criteria porous non-waterlogged severely acidified soils on sandstonesubstrates in the regions of Black Forest Forest of Odes and Neckarland as well as on Pleistocenedeposits in Alpine foothills with larger homogeneous stands (10ndash50 ha) of Norway spruce (Picea abies)in pure stands or mixed with Silver fir (Abies alba) Scots pine (Pinus sylvestris) Douglas fir (Pseudotsugamenziesii) and European beech (Fagus sylvatica) with the age of the stand being 40ndash90 years Excludedwere the areas of nature conservation water protection special biotopes (eg capercaillie habitats)protected forests other study sites as well as previously limed areas With regard to the tree vitalityseverely damaged stands with tree needle loss gt40 were also excluded from selection Directlyadjacent to an untreated ldquocontrolrdquo plot a ldquolimedrdquo plot was established by applying a calcium carbonateCaCO3 in mixture with 4ndash8 MgO 3 P2O5 and 6ndash10 K2O (ldquoKohlensaurer Kalk 121123127rdquo limegrade 95 lt 315 mm and 70 lt 10 mm) from autumn 1983 until early winter 1984 The dose wasestablished site-specific according to the pH humus form and tree species surveyed in 1983 and wasno higher than 35 Mg haminus1 in most cases between 25 and 3 Mg haminus1 This comparably low dosagewas chosen in order to avoid overly high mobilization of the humus layer and undesirable nutrientleaching in the groundwater and surface waters This also meant that any changes in the soil aciditystatus were expected to progress slowly over several years

In 2003 a second treatment of 6 Mg haminus1 dolomite lime with 55 CaCO3 and 35 MgCO3

(ldquoCaMg(CO3)2 5535rdquo lime grade 90 lt 01 mm) was applied The dolomite lime was seen to bufferacid deposition effectively and to react slower than the previously applied calcium carbonate mixturewith milder effects on humus and was therefore chosen to be applied in larger doses

It is important to note that the study sites have been considered as praxis-fertilization trialsmeaning that the scientific investigations have accompanied the regular forest management practices(moderate thinning of stands storm damage response natural regeneration or planting etc) A recentcomprehensive inventory of these sites was conducted in 2015 and their updated description is shownin Table 1 A map of study site locations is shown in Appendix A (Figure A1)

Soil Syst 2020 4 38 4 of 33

Table 1 Study sites and their key parameters in 2015

SiteLatitude

()Longitude

()Altitude(m asl)

Plot Size (ha)Substrate Soil Type 1 Texture 2 Humus

Type 3StandType 4

StandAge Grouping 5

Control Limed

BadWaldsee 4750prime 941prime 580 4 22 Glacial till cambisol LS

mull -modermull

PI-FA 70 G1

Ellwangen 4901prime 1010prime 490 10 15 Sandstone stagnosol SL mull PI 100 G1Freuden-

stadt 4826prime 825prime 740 8 21 Sandstone cambisol SL mull - mormoder AB-PI 100 G1

Heidelberg 4930prime 847prime 490 2 3 Sandstone podsol SL mull PI 70 G1

Ochsen-hausen 4806prime 1002prime 620 5 17 Periglacial

gravel cambisol Lmull -modermull

PI 90 G1

Herzogen-weiler 4801prime 820prime 950 8 20 Sandstone stagnosol LS-SL

mull -modermull

AB-PI 90 G2

Horb 4828prime 832prime 630 8 21 Sandstone cambisol LS mull AB-PI 100 G2

Hospital 4807prime 941prime 650 3 5 Glacial till stagnosol SiL-L mull - mormoder PI-FA 110 G2

Wangen 4747prime 945prime 710 6 22 Glacial till umbrisol SiL-L mormoder PI 100 G2

Weithard 4758prime 917prime 630 1 6 Glacial till stagnosol CL-L mull - mormoder PI 100 G2

1 dominating soil type according to FAO 2014 (World Reference Base For Soil Classification) 2 mean textural classes according to FAO [24] (pp 25ndash29) LS = Loamy sand SL = Sandy loamL = Loam SiL = Silty loam CL = Clay loam 3 dominating humus forms according to Ad-hoc-Arbeitsgruppe Boden (German soil classification) [25] (pp 303ndash310) 4 PI = Picea abies AB-PI= mixed Abies alba and Picea abies PI-FA= mixed Picea abies and Fagus sylvatica 5 Grouping according to K-means Cluster Analysis (see statistical analyses)

Soil Syst 2020 4 38 5 of 33

22 Soil Sampling and Laboratory Methods

The sampling methods of the different sampling periods of 1985ndash2015 are described in Table 2

Table 2 Soil sampling design in the 1980s (as described in Wilpert et al [23]) 2003 2010 and 2015

198586 and 1989 2003 2010 2015

Sample layoutwithin plot

3-10 (O-layer) and6ndash10 (mineral soil)samples in 10 mdistance along a

random diagonalline

1 sample at 5randomly distributedpoints plus 5 samplesat 0 80 160 240 and320 gradian in 5 mdistance from a soil

profile

1 sample at 5randomly

distributed points

1 sample at 5randomly

distributed points

Sampled soillayers

O-layer a

0ndash4 cm b

5ndash10 cm a

O-layer c

0ndash5 cm d

5ndash10 cm d

10ndash30 cm d

30ndash60 cm d

O-layer c

0ndash5c m d

5ndash10 cm d

10ndash30 cm d

30ndash60 cm d

O-layer c

0ndash5 cm d

5ndash10 cm d

10ndash20 cm d

20ndash30 cm d

30ndash60 cm d

Instrumenta scraper

b 100 cm3 soilsample ring

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8 cm

length 15 cm)

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8cm length 15 cm)

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8cm length 15 cm)

No of replicates 1 mixed sample 1 mixed sample 4 individualsamples

5 individualsamples

The first sampling period was 1985 and 1986 a further sampling campaign was completed in198990 Three to ten samples of O-layer and six to ten samples of the mineral soil were collected and thenmixed into a single sample for the laboratory analysis The results comparing the development at controland limed plots between these two sampling campaigns have been published in Wilpert et al [23](pp 30ndash45) The control plot pH-KCl in mineral topsoil was pH 30 ie in the Al and Al-Fe bufferrange meanwhile at limed plots it had increased by average 09 pH units in 198586 and 02 pH unitsby 198990 in 0ndash4 cm topsoil while in 4ndash10 cm topsoil only by 198990 an increase by 02 pH unitswas observed The pH-H2O was reported to be 05ndash1 pH units higher than pH-KCl with 10ndash20 lesschange after treatment While at control plots the O-layer thickness tended to increase at limed plots ithad decreased and liming had increased the variability of C-content in 4ndash10 cm mineral soil with littlechange in average C-content Control plot exchangeable cations (CEC) and exchangeable cations wereanalyzed only in 198990 samples where base saturation improved significantly by 17 after limetreatment (though with high variance) especially exchangeable Ca and slightly less exchangeable Mgwith little change in exchangeable K Meanwhile exchangeable Al and H had decreased Limed plotCEC had overall increased by 14

The second sampling was carried out in April until October 2003 ie twenty years after thefirst liming and before the second treatment campaign A soil sample per depth class was taken atfive randomly distributed points across a plot as well as in five directions from an established soilprofile then mixed into a single sample In MarchndashOctober 2010mdashseven years after the second limingeventmdashsoil sampling was done at four randomly distributed points per treatment plot The final soilsampling campaign was carried out in March until June 2015mdashtwelve years since the second limeapplicationmdashat five randomly distributed points per plot

The soil samples were dried at 60 C and ground in a mill with a 2 mm sieveThe following soil chemical parameters were considered in our investigation pH-H2O and

pH-KCl were measured with a glass electrode in 15 (mineral soil) and 110 (O-layer) solution withH2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (micromolc gminus1) and theirsum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation

Soil Syst 2020 4 38 6 of 33

() were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OEStotal N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al andFe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1)were calculated form dried soil samples of defined sampled area The methodology of our laboratoryanalyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA)by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as TablesS1ndashS3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different samplingperiods at the study sites and therefore the element concentrations may be directly comparedbetween the sampling years and between the directly adjacent treatment variants without consideringelement stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pHvalues were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversioninto pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volumeweight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019)First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity

of sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated samplingcampaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations werecalculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimalnumber of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBadWaldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 thesites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionallya principal component analysis (PCA) was run in order to confirm the CA results as well as determinethe most relevant soil chemical principal components (PC) of these site groups The first two PCsexplained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot

(t haminus1) and CEC (micromolc gminus1 PC-2 Figure 1)Group 1 (G1) includes the sites with predominantly ldquosandy soilsrdquo and is characterized with lower

CEC lower Ctot stocks lower K+ stocks and higher Al3+ stocks in the upper mineral soil comparedto Group 2 (G2) of predominantly finer textured ldquosiltyclay loam soilsrdquo For both study site groupspH-H2O of 40ndash44 was similar in 0-30 cm mineral soil whereas pH-KCl was 33ndash36 at G1 and 35ndash37at G2 sites ie comparably higher

The statistical analysis was applied to both site groups separately Due to small sample size in thesampling campaigns (n lt 30 per depth class) as well as a lack of normal distribution in some of thedata non-parametric statistical tests were chosen In order to compare the difference in group-meansbetween sampling years (separately for control and lime treatments) Friedman test for repeated(dependent) measurements was applied To find differences between control and lime treatmentswithin a sampling year MannndashWhitney U test for independent samples was used The significancelevel was chosen p lt 005

Soil Syst 2020 4 38 7 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 6 of 35

H2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (μmolc gminus1) and their sum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation () were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OES total N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000 in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al and Fe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1) were calculated form dried soil samples of defined sampled area The methodology of our laboratory analyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA) by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as Table S1 S2 and S3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different sampling periods at the study sites and therefore the element concentrations may be directly compared between the sampling years and between the directly adjacent treatment variants without considering element stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into 10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pH values were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversion into pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volume weight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019) First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity of

sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated sampling campaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations were calculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimal number of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBad Waldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 the sites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionally a principal component analysis (PCA) was run in order to confirm the CA results as well as determine the most relevant soil chemical principal components (PC) of these site groups The first two PCs explained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot (t haminus1) and CEC (μmolc gminus1 PC-2 Figure 1)

(a)

(b)

Figure 1 Principal component analysis (PCA) to characterize study site grouping parameters (a) studysites and (b) principal components

To estimate the natural recovery as well as the effects of lime application over time ie thedifference between two sampling periods within a study site group a relative response ratio (RRr) wascalculated for each of the relevant site parameters based on methodology in Hedges et al [29] andReid and Watmough [17]

RRr = (t2t1) minus 1 (1)

where t1 = site plot average (arithmetic mean) in previous sampling period t2 = site plot average infollowing sampling period In case of already relative (CN) log-transformed (pH) and discontinuous(base saturation) variables an absolute RRa was calculated as difference between previous and followingsampling year or limed and control treatment

RRa = t2 minus t1 (2)

3 Results

Since the 1980s sampling design and data set was not comparable with the subsequent campaignsfrom 2003 until 2015 we were not able to analyze statistically the changes in soil chemical propertiesof the entire measured soil profile of our studied sites for the period 1980s until 2003 Neverthelesswith the sampling data of 2003 we can evaluate the liming effects in this initial study period on soilproperties with the direct comparison of control and limed plots From 2003 on we can describe thedevelopment of soil chemical properties with respect to liming effects in great detail In this contextwe will first of all present the changes in soil acidity status with focus on pH values base saturationand cation exchange capacities as well as the exchangeable cations concentrations Secondly thedevelopment of soil nutrient status with focus on carbon and nitrogen are outlined A complete list ofparameter means (with standard deviations) as they developed over time and after lime treatment isavailable as Table S4 (G1) and S5 (G2) in Supplementary Materials The parameter response ratio (RR)means SD and ranges are fully detailed in Tables S6 (G1) and S7 (G2) of Supplementary Materials

31 Liming Effects in 2003

In 2003mdashtwenty years after the first lime treatment in 1983mdashno significant differences could beseen in soil pH or base saturation between the control and limed plots The mean values at limed plotstended to be higher for both parameters especially in the O-layer (pH) and 0ndash5 cm mineral soil (BS)

Soil Syst 2020 4 38 8 of 33

however the confidence intervals of both control and lime treatment overlap Similarly sum CECby 2003 was comparable throughout the entire soil profile also G2 site 0ndash5 cm mineral soil sampleexchangeable Ca as well as Ctot and Ntot were significantly increasedmdasha potential residual effect oflime application in 1983mdashyet even here the increase in CEC was only slight and not significant G1 sitelimed plot O-layer total Al and total Fe concentrations were significantly higher compared to controlalthough again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in theentire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer andfrom pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pHunits) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pHunits) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however thisrecovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layerand from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

Soil Syst 2020 4 x FOR PEER REVIEW 8 of 35

significant G1 site limed plot O-layer total Al and total Fe concentrations were significantly higher compared to control although again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in the entire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer and from pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in 0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pH units) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pH units) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however this recovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layer and from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1 and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pH units at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010 and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots with group average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in the O-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the difference between the control and limed plots was significant in all G1 measured soil profile depths in 2010 the treatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 years since the last lime application At G2 sites the liming effect reached significance only down to 10 cm mineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

(a)

(b)

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites(b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 38 9 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 9 of 35

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Similar development in both natural recovery and liming effects over time was seen also in pH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronounced in the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect only down to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen across all study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) The average RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in 2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below 20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significant increase in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime application This liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa 4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the 0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in both the 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pHunits at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots withgroup average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in theO-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the differencebetween the control and limed plots was significant in all G1 measured soil profile depths in 2010 thetreatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 yearssince the last lime application At G2 sites the liming effect reached significance only down to 10 cmmineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

Similar development in both natural recovery and liming effects over time was seen also inpH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronouncedin the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect onlydown to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen acrossall study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) Theaverage RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in

Soil Syst 2020 4 38 10 of 33

2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significantincrease in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime applicationThis liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa

4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in boththe 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just a 1ndash3 increasein group average BS Compared to the control plots both G1 and G2 limed plot BS was significantlyhigher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plotbase saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and9ndash12 in 30ndash60 cm mineral soil

Soil Syst 2020 4 x FOR PEER REVIEW 10 of 35

a 1ndash3 increase in group average BS Compared to the control plots both G1 and G2 limed plot BS was significantly higher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80 in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plot base saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and 9ndash12 in 30ndash60 cm mineral soil

(a)

(b)

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 studysites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differencesbetween current and previous sampling campaign

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 4: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 4 of 33

Table 1 Study sites and their key parameters in 2015

SiteLatitude

()Longitude

()Altitude(m asl)

Plot Size (ha)Substrate Soil Type 1 Texture 2 Humus

Type 3StandType 4

StandAge Grouping 5

Control Limed

BadWaldsee 4750prime 941prime 580 4 22 Glacial till cambisol LS

mull -modermull

PI-FA 70 G1

Ellwangen 4901prime 1010prime 490 10 15 Sandstone stagnosol SL mull PI 100 G1Freuden-

stadt 4826prime 825prime 740 8 21 Sandstone cambisol SL mull - mormoder AB-PI 100 G1

Heidelberg 4930prime 847prime 490 2 3 Sandstone podsol SL mull PI 70 G1

Ochsen-hausen 4806prime 1002prime 620 5 17 Periglacial

gravel cambisol Lmull -modermull

PI 90 G1

Herzogen-weiler 4801prime 820prime 950 8 20 Sandstone stagnosol LS-SL

mull -modermull

AB-PI 90 G2

Horb 4828prime 832prime 630 8 21 Sandstone cambisol LS mull AB-PI 100 G2

Hospital 4807prime 941prime 650 3 5 Glacial till stagnosol SiL-L mull - mormoder PI-FA 110 G2

Wangen 4747prime 945prime 710 6 22 Glacial till umbrisol SiL-L mormoder PI 100 G2

Weithard 4758prime 917prime 630 1 6 Glacial till stagnosol CL-L mull - mormoder PI 100 G2

1 dominating soil type according to FAO 2014 (World Reference Base For Soil Classification) 2 mean textural classes according to FAO [24] (pp 25ndash29) LS = Loamy sand SL = Sandy loamL = Loam SiL = Silty loam CL = Clay loam 3 dominating humus forms according to Ad-hoc-Arbeitsgruppe Boden (German soil classification) [25] (pp 303ndash310) 4 PI = Picea abies AB-PI= mixed Abies alba and Picea abies PI-FA= mixed Picea abies and Fagus sylvatica 5 Grouping according to K-means Cluster Analysis (see statistical analyses)

Soil Syst 2020 4 38 5 of 33

22 Soil Sampling and Laboratory Methods

The sampling methods of the different sampling periods of 1985ndash2015 are described in Table 2

Table 2 Soil sampling design in the 1980s (as described in Wilpert et al [23]) 2003 2010 and 2015

198586 and 1989 2003 2010 2015

Sample layoutwithin plot

3-10 (O-layer) and6ndash10 (mineral soil)samples in 10 mdistance along a

random diagonalline

1 sample at 5randomly distributedpoints plus 5 samplesat 0 80 160 240 and320 gradian in 5 mdistance from a soil

profile

1 sample at 5randomly

distributed points

1 sample at 5randomly

distributed points

Sampled soillayers

O-layer a

0ndash4 cm b

5ndash10 cm a

O-layer c

0ndash5 cm d

5ndash10 cm d

10ndash30 cm d

30ndash60 cm d

O-layer c

0ndash5c m d

5ndash10 cm d

10ndash30 cm d

30ndash60 cm d

O-layer c

0ndash5 cm d

5ndash10 cm d

10ndash20 cm d

20ndash30 cm d

30ndash60 cm d

Instrumenta scraper

b 100 cm3 soilsample ring

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8 cm

length 15 cm)

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8cm length 15 cm)

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8cm length 15 cm)

No of replicates 1 mixed sample 1 mixed sample 4 individualsamples

5 individualsamples

The first sampling period was 1985 and 1986 a further sampling campaign was completed in198990 Three to ten samples of O-layer and six to ten samples of the mineral soil were collected and thenmixed into a single sample for the laboratory analysis The results comparing the development at controland limed plots between these two sampling campaigns have been published in Wilpert et al [23](pp 30ndash45) The control plot pH-KCl in mineral topsoil was pH 30 ie in the Al and Al-Fe bufferrange meanwhile at limed plots it had increased by average 09 pH units in 198586 and 02 pH unitsby 198990 in 0ndash4 cm topsoil while in 4ndash10 cm topsoil only by 198990 an increase by 02 pH unitswas observed The pH-H2O was reported to be 05ndash1 pH units higher than pH-KCl with 10ndash20 lesschange after treatment While at control plots the O-layer thickness tended to increase at limed plots ithad decreased and liming had increased the variability of C-content in 4ndash10 cm mineral soil with littlechange in average C-content Control plot exchangeable cations (CEC) and exchangeable cations wereanalyzed only in 198990 samples where base saturation improved significantly by 17 after limetreatment (though with high variance) especially exchangeable Ca and slightly less exchangeable Mgwith little change in exchangeable K Meanwhile exchangeable Al and H had decreased Limed plotCEC had overall increased by 14

The second sampling was carried out in April until October 2003 ie twenty years after thefirst liming and before the second treatment campaign A soil sample per depth class was taken atfive randomly distributed points across a plot as well as in five directions from an established soilprofile then mixed into a single sample In MarchndashOctober 2010mdashseven years after the second limingeventmdashsoil sampling was done at four randomly distributed points per treatment plot The final soilsampling campaign was carried out in March until June 2015mdashtwelve years since the second limeapplicationmdashat five randomly distributed points per plot

The soil samples were dried at 60 C and ground in a mill with a 2 mm sieveThe following soil chemical parameters were considered in our investigation pH-H2O and

pH-KCl were measured with a glass electrode in 15 (mineral soil) and 110 (O-layer) solution withH2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (micromolc gminus1) and theirsum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation

Soil Syst 2020 4 38 6 of 33

() were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OEStotal N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al andFe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1)were calculated form dried soil samples of defined sampled area The methodology of our laboratoryanalyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA)by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as TablesS1ndashS3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different samplingperiods at the study sites and therefore the element concentrations may be directly comparedbetween the sampling years and between the directly adjacent treatment variants without consideringelement stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pHvalues were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversioninto pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volumeweight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019)First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity

of sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated samplingcampaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations werecalculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimalnumber of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBadWaldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 thesites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionallya principal component analysis (PCA) was run in order to confirm the CA results as well as determinethe most relevant soil chemical principal components (PC) of these site groups The first two PCsexplained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot

(t haminus1) and CEC (micromolc gminus1 PC-2 Figure 1)Group 1 (G1) includes the sites with predominantly ldquosandy soilsrdquo and is characterized with lower

CEC lower Ctot stocks lower K+ stocks and higher Al3+ stocks in the upper mineral soil comparedto Group 2 (G2) of predominantly finer textured ldquosiltyclay loam soilsrdquo For both study site groupspH-H2O of 40ndash44 was similar in 0-30 cm mineral soil whereas pH-KCl was 33ndash36 at G1 and 35ndash37at G2 sites ie comparably higher

The statistical analysis was applied to both site groups separately Due to small sample size in thesampling campaigns (n lt 30 per depth class) as well as a lack of normal distribution in some of thedata non-parametric statistical tests were chosen In order to compare the difference in group-meansbetween sampling years (separately for control and lime treatments) Friedman test for repeated(dependent) measurements was applied To find differences between control and lime treatmentswithin a sampling year MannndashWhitney U test for independent samples was used The significancelevel was chosen p lt 005

Soil Syst 2020 4 38 7 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 6 of 35

H2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (μmolc gminus1) and their sum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation () were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OES total N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000 in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al and Fe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1) were calculated form dried soil samples of defined sampled area The methodology of our laboratory analyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA) by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as Table S1 S2 and S3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different sampling periods at the study sites and therefore the element concentrations may be directly compared between the sampling years and between the directly adjacent treatment variants without considering element stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into 10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pH values were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversion into pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volume weight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019) First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity of

sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated sampling campaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations were calculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimal number of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBad Waldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 the sites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionally a principal component analysis (PCA) was run in order to confirm the CA results as well as determine the most relevant soil chemical principal components (PC) of these site groups The first two PCs explained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot (t haminus1) and CEC (μmolc gminus1 PC-2 Figure 1)

(a)

(b)

Figure 1 Principal component analysis (PCA) to characterize study site grouping parameters (a) studysites and (b) principal components

To estimate the natural recovery as well as the effects of lime application over time ie thedifference between two sampling periods within a study site group a relative response ratio (RRr) wascalculated for each of the relevant site parameters based on methodology in Hedges et al [29] andReid and Watmough [17]

RRr = (t2t1) minus 1 (1)

where t1 = site plot average (arithmetic mean) in previous sampling period t2 = site plot average infollowing sampling period In case of already relative (CN) log-transformed (pH) and discontinuous(base saturation) variables an absolute RRa was calculated as difference between previous and followingsampling year or limed and control treatment

RRa = t2 minus t1 (2)

3 Results

Since the 1980s sampling design and data set was not comparable with the subsequent campaignsfrom 2003 until 2015 we were not able to analyze statistically the changes in soil chemical propertiesof the entire measured soil profile of our studied sites for the period 1980s until 2003 Neverthelesswith the sampling data of 2003 we can evaluate the liming effects in this initial study period on soilproperties with the direct comparison of control and limed plots From 2003 on we can describe thedevelopment of soil chemical properties with respect to liming effects in great detail In this contextwe will first of all present the changes in soil acidity status with focus on pH values base saturationand cation exchange capacities as well as the exchangeable cations concentrations Secondly thedevelopment of soil nutrient status with focus on carbon and nitrogen are outlined A complete list ofparameter means (with standard deviations) as they developed over time and after lime treatment isavailable as Table S4 (G1) and S5 (G2) in Supplementary Materials The parameter response ratio (RR)means SD and ranges are fully detailed in Tables S6 (G1) and S7 (G2) of Supplementary Materials

31 Liming Effects in 2003

In 2003mdashtwenty years after the first lime treatment in 1983mdashno significant differences could beseen in soil pH or base saturation between the control and limed plots The mean values at limed plotstended to be higher for both parameters especially in the O-layer (pH) and 0ndash5 cm mineral soil (BS)

Soil Syst 2020 4 38 8 of 33

however the confidence intervals of both control and lime treatment overlap Similarly sum CECby 2003 was comparable throughout the entire soil profile also G2 site 0ndash5 cm mineral soil sampleexchangeable Ca as well as Ctot and Ntot were significantly increasedmdasha potential residual effect oflime application in 1983mdashyet even here the increase in CEC was only slight and not significant G1 sitelimed plot O-layer total Al and total Fe concentrations were significantly higher compared to controlalthough again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in theentire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer andfrom pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pHunits) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pHunits) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however thisrecovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layerand from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

Soil Syst 2020 4 x FOR PEER REVIEW 8 of 35

significant G1 site limed plot O-layer total Al and total Fe concentrations were significantly higher compared to control although again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in the entire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer and from pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in 0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pH units) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pH units) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however this recovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layer and from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1 and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pH units at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010 and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots with group average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in the O-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the difference between the control and limed plots was significant in all G1 measured soil profile depths in 2010 the treatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 years since the last lime application At G2 sites the liming effect reached significance only down to 10 cm mineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

(a)

(b)

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites(b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 38 9 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 9 of 35

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Similar development in both natural recovery and liming effects over time was seen also in pH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronounced in the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect only down to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen across all study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) The average RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in 2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below 20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significant increase in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime application This liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa 4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the 0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in both the 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pHunits at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots withgroup average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in theO-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the differencebetween the control and limed plots was significant in all G1 measured soil profile depths in 2010 thetreatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 yearssince the last lime application At G2 sites the liming effect reached significance only down to 10 cmmineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

Similar development in both natural recovery and liming effects over time was seen also inpH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronouncedin the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect onlydown to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen acrossall study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) Theaverage RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in

Soil Syst 2020 4 38 10 of 33

2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significantincrease in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime applicationThis liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa

4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in boththe 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just a 1ndash3 increasein group average BS Compared to the control plots both G1 and G2 limed plot BS was significantlyhigher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plotbase saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and9ndash12 in 30ndash60 cm mineral soil

Soil Syst 2020 4 x FOR PEER REVIEW 10 of 35

a 1ndash3 increase in group average BS Compared to the control plots both G1 and G2 limed plot BS was significantly higher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80 in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plot base saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and 9ndash12 in 30ndash60 cm mineral soil

(a)

(b)

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 studysites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differencesbetween current and previous sampling campaign

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 5: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 5 of 33

22 Soil Sampling and Laboratory Methods

The sampling methods of the different sampling periods of 1985ndash2015 are described in Table 2

Table 2 Soil sampling design in the 1980s (as described in Wilpert et al [23]) 2003 2010 and 2015

198586 and 1989 2003 2010 2015

Sample layoutwithin plot

3-10 (O-layer) and6ndash10 (mineral soil)samples in 10 mdistance along a

random diagonalline

1 sample at 5randomly distributedpoints plus 5 samplesat 0 80 160 240 and320 gradian in 5 mdistance from a soil

profile

1 sample at 5randomly

distributed points

1 sample at 5randomly

distributed points

Sampled soillayers

O-layer a

0ndash4 cm b

5ndash10 cm a

O-layer c

0ndash5 cm d

5ndash10 cm d

10ndash30 cm d

30ndash60 cm d

O-layer c

0ndash5c m d

5ndash10 cm d

10ndash30 cm d

30ndash60 cm d

O-layer c

0ndash5 cm d

5ndash10 cm d

10ndash20 cm d

20ndash30 cm d

30ndash60 cm d

Instrumenta scraper

b 100 cm3 soilsample ring

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8 cm

length 15 cm)

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8cm length 15 cm)

c 200 cm3 soilsample ring

d Eijkelkamp rootauger (diameter 8cm length 15 cm)

No of replicates 1 mixed sample 1 mixed sample 4 individualsamples

5 individualsamples

The first sampling period was 1985 and 1986 a further sampling campaign was completed in198990 Three to ten samples of O-layer and six to ten samples of the mineral soil were collected and thenmixed into a single sample for the laboratory analysis The results comparing the development at controland limed plots between these two sampling campaigns have been published in Wilpert et al [23](pp 30ndash45) The control plot pH-KCl in mineral topsoil was pH 30 ie in the Al and Al-Fe bufferrange meanwhile at limed plots it had increased by average 09 pH units in 198586 and 02 pH unitsby 198990 in 0ndash4 cm topsoil while in 4ndash10 cm topsoil only by 198990 an increase by 02 pH unitswas observed The pH-H2O was reported to be 05ndash1 pH units higher than pH-KCl with 10ndash20 lesschange after treatment While at control plots the O-layer thickness tended to increase at limed plots ithad decreased and liming had increased the variability of C-content in 4ndash10 cm mineral soil with littlechange in average C-content Control plot exchangeable cations (CEC) and exchangeable cations wereanalyzed only in 198990 samples where base saturation improved significantly by 17 after limetreatment (though with high variance) especially exchangeable Ca and slightly less exchangeable Mgwith little change in exchangeable K Meanwhile exchangeable Al and H had decreased Limed plotCEC had overall increased by 14

The second sampling was carried out in April until October 2003 ie twenty years after thefirst liming and before the second treatment campaign A soil sample per depth class was taken atfive randomly distributed points across a plot as well as in five directions from an established soilprofile then mixed into a single sample In MarchndashOctober 2010mdashseven years after the second limingeventmdashsoil sampling was done at four randomly distributed points per treatment plot The final soilsampling campaign was carried out in March until June 2015mdashtwelve years since the second limeapplicationmdashat five randomly distributed points per plot

The soil samples were dried at 60 C and ground in a mill with a 2 mm sieveThe following soil chemical parameters were considered in our investigation pH-H2O and

pH-KCl were measured with a glass electrode in 15 (mineral soil) and 110 (O-layer) solution withH2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (micromolc gminus1) and theirsum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation

Soil Syst 2020 4 38 6 of 33

() were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OEStotal N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al andFe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1)were calculated form dried soil samples of defined sampled area The methodology of our laboratoryanalyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA)by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as TablesS1ndashS3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different samplingperiods at the study sites and therefore the element concentrations may be directly comparedbetween the sampling years and between the directly adjacent treatment variants without consideringelement stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pHvalues were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversioninto pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volumeweight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019)First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity

of sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated samplingcampaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations werecalculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimalnumber of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBadWaldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 thesites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionallya principal component analysis (PCA) was run in order to confirm the CA results as well as determinethe most relevant soil chemical principal components (PC) of these site groups The first two PCsexplained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot

(t haminus1) and CEC (micromolc gminus1 PC-2 Figure 1)Group 1 (G1) includes the sites with predominantly ldquosandy soilsrdquo and is characterized with lower

CEC lower Ctot stocks lower K+ stocks and higher Al3+ stocks in the upper mineral soil comparedto Group 2 (G2) of predominantly finer textured ldquosiltyclay loam soilsrdquo For both study site groupspH-H2O of 40ndash44 was similar in 0-30 cm mineral soil whereas pH-KCl was 33ndash36 at G1 and 35ndash37at G2 sites ie comparably higher

The statistical analysis was applied to both site groups separately Due to small sample size in thesampling campaigns (n lt 30 per depth class) as well as a lack of normal distribution in some of thedata non-parametric statistical tests were chosen In order to compare the difference in group-meansbetween sampling years (separately for control and lime treatments) Friedman test for repeated(dependent) measurements was applied To find differences between control and lime treatmentswithin a sampling year MannndashWhitney U test for independent samples was used The significancelevel was chosen p lt 005

Soil Syst 2020 4 38 7 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 6 of 35

H2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (μmolc gminus1) and their sum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation () were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OES total N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000 in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al and Fe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1) were calculated form dried soil samples of defined sampled area The methodology of our laboratory analyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA) by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as Table S1 S2 and S3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different sampling periods at the study sites and therefore the element concentrations may be directly compared between the sampling years and between the directly adjacent treatment variants without considering element stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into 10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pH values were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversion into pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volume weight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019) First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity of

sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated sampling campaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations were calculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimal number of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBad Waldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 the sites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionally a principal component analysis (PCA) was run in order to confirm the CA results as well as determine the most relevant soil chemical principal components (PC) of these site groups The first two PCs explained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot (t haminus1) and CEC (μmolc gminus1 PC-2 Figure 1)

(a)

(b)

Figure 1 Principal component analysis (PCA) to characterize study site grouping parameters (a) studysites and (b) principal components

To estimate the natural recovery as well as the effects of lime application over time ie thedifference between two sampling periods within a study site group a relative response ratio (RRr) wascalculated for each of the relevant site parameters based on methodology in Hedges et al [29] andReid and Watmough [17]

RRr = (t2t1) minus 1 (1)

where t1 = site plot average (arithmetic mean) in previous sampling period t2 = site plot average infollowing sampling period In case of already relative (CN) log-transformed (pH) and discontinuous(base saturation) variables an absolute RRa was calculated as difference between previous and followingsampling year or limed and control treatment

RRa = t2 minus t1 (2)

3 Results

Since the 1980s sampling design and data set was not comparable with the subsequent campaignsfrom 2003 until 2015 we were not able to analyze statistically the changes in soil chemical propertiesof the entire measured soil profile of our studied sites for the period 1980s until 2003 Neverthelesswith the sampling data of 2003 we can evaluate the liming effects in this initial study period on soilproperties with the direct comparison of control and limed plots From 2003 on we can describe thedevelopment of soil chemical properties with respect to liming effects in great detail In this contextwe will first of all present the changes in soil acidity status with focus on pH values base saturationand cation exchange capacities as well as the exchangeable cations concentrations Secondly thedevelopment of soil nutrient status with focus on carbon and nitrogen are outlined A complete list ofparameter means (with standard deviations) as they developed over time and after lime treatment isavailable as Table S4 (G1) and S5 (G2) in Supplementary Materials The parameter response ratio (RR)means SD and ranges are fully detailed in Tables S6 (G1) and S7 (G2) of Supplementary Materials

31 Liming Effects in 2003

In 2003mdashtwenty years after the first lime treatment in 1983mdashno significant differences could beseen in soil pH or base saturation between the control and limed plots The mean values at limed plotstended to be higher for both parameters especially in the O-layer (pH) and 0ndash5 cm mineral soil (BS)

Soil Syst 2020 4 38 8 of 33

however the confidence intervals of both control and lime treatment overlap Similarly sum CECby 2003 was comparable throughout the entire soil profile also G2 site 0ndash5 cm mineral soil sampleexchangeable Ca as well as Ctot and Ntot were significantly increasedmdasha potential residual effect oflime application in 1983mdashyet even here the increase in CEC was only slight and not significant G1 sitelimed plot O-layer total Al and total Fe concentrations were significantly higher compared to controlalthough again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in theentire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer andfrom pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pHunits) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pHunits) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however thisrecovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layerand from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

Soil Syst 2020 4 x FOR PEER REVIEW 8 of 35

significant G1 site limed plot O-layer total Al and total Fe concentrations were significantly higher compared to control although again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in the entire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer and from pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in 0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pH units) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pH units) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however this recovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layer and from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1 and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pH units at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010 and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots with group average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in the O-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the difference between the control and limed plots was significant in all G1 measured soil profile depths in 2010 the treatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 years since the last lime application At G2 sites the liming effect reached significance only down to 10 cm mineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

(a)

(b)

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites(b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 38 9 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 9 of 35

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Similar development in both natural recovery and liming effects over time was seen also in pH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronounced in the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect only down to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen across all study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) The average RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in 2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below 20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significant increase in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime application This liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa 4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the 0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in both the 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pHunits at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots withgroup average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in theO-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the differencebetween the control and limed plots was significant in all G1 measured soil profile depths in 2010 thetreatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 yearssince the last lime application At G2 sites the liming effect reached significance only down to 10 cmmineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

Similar development in both natural recovery and liming effects over time was seen also inpH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronouncedin the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect onlydown to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen acrossall study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) Theaverage RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in

Soil Syst 2020 4 38 10 of 33

2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significantincrease in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime applicationThis liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa

4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in boththe 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just a 1ndash3 increasein group average BS Compared to the control plots both G1 and G2 limed plot BS was significantlyhigher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plotbase saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and9ndash12 in 30ndash60 cm mineral soil

Soil Syst 2020 4 x FOR PEER REVIEW 10 of 35

a 1ndash3 increase in group average BS Compared to the control plots both G1 and G2 limed plot BS was significantly higher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80 in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plot base saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and 9ndash12 in 30ndash60 cm mineral soil

(a)

(b)

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 studysites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differencesbetween current and previous sampling campaign

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 6: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 6 of 33

() were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OEStotal N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al andFe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1)were calculated form dried soil samples of defined sampled area The methodology of our laboratoryanalyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA)by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as TablesS1ndashS3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different samplingperiods at the study sites and therefore the element concentrations may be directly comparedbetween the sampling years and between the directly adjacent treatment variants without consideringelement stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pHvalues were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversioninto pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volumeweight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019)First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity

of sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated samplingcampaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations werecalculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimalnumber of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBadWaldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 thesites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionallya principal component analysis (PCA) was run in order to confirm the CA results as well as determinethe most relevant soil chemical principal components (PC) of these site groups The first two PCsexplained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot

(t haminus1) and CEC (micromolc gminus1 PC-2 Figure 1)Group 1 (G1) includes the sites with predominantly ldquosandy soilsrdquo and is characterized with lower

CEC lower Ctot stocks lower K+ stocks and higher Al3+ stocks in the upper mineral soil comparedto Group 2 (G2) of predominantly finer textured ldquosiltyclay loam soilsrdquo For both study site groupspH-H2O of 40ndash44 was similar in 0-30 cm mineral soil whereas pH-KCl was 33ndash36 at G1 and 35ndash37at G2 sites ie comparably higher

The statistical analysis was applied to both site groups separately Due to small sample size in thesampling campaigns (n lt 30 per depth class) as well as a lack of normal distribution in some of thedata non-parametric statistical tests were chosen In order to compare the difference in group-meansbetween sampling years (separately for control and lime treatments) Friedman test for repeated(dependent) measurements was applied To find differences between control and lime treatmentswithin a sampling year MannndashWhitney U test for independent samples was used The significancelevel was chosen p lt 005

Soil Syst 2020 4 38 7 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 6 of 35

H2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (μmolc gminus1) and their sum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation () were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OES total N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000 in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al and Fe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1) were calculated form dried soil samples of defined sampled area The methodology of our laboratory analyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA) by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as Table S1 S2 and S3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different sampling periods at the study sites and therefore the element concentrations may be directly compared between the sampling years and between the directly adjacent treatment variants without considering element stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into 10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pH values were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversion into pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volume weight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019) First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity of

sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated sampling campaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations were calculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimal number of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBad Waldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 the sites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionally a principal component analysis (PCA) was run in order to confirm the CA results as well as determine the most relevant soil chemical principal components (PC) of these site groups The first two PCs explained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot (t haminus1) and CEC (μmolc gminus1 PC-2 Figure 1)

(a)

(b)

Figure 1 Principal component analysis (PCA) to characterize study site grouping parameters (a) studysites and (b) principal components

To estimate the natural recovery as well as the effects of lime application over time ie thedifference between two sampling periods within a study site group a relative response ratio (RRr) wascalculated for each of the relevant site parameters based on methodology in Hedges et al [29] andReid and Watmough [17]

RRr = (t2t1) minus 1 (1)

where t1 = site plot average (arithmetic mean) in previous sampling period t2 = site plot average infollowing sampling period In case of already relative (CN) log-transformed (pH) and discontinuous(base saturation) variables an absolute RRa was calculated as difference between previous and followingsampling year or limed and control treatment

RRa = t2 minus t1 (2)

3 Results

Since the 1980s sampling design and data set was not comparable with the subsequent campaignsfrom 2003 until 2015 we were not able to analyze statistically the changes in soil chemical propertiesof the entire measured soil profile of our studied sites for the period 1980s until 2003 Neverthelesswith the sampling data of 2003 we can evaluate the liming effects in this initial study period on soilproperties with the direct comparison of control and limed plots From 2003 on we can describe thedevelopment of soil chemical properties with respect to liming effects in great detail In this contextwe will first of all present the changes in soil acidity status with focus on pH values base saturationand cation exchange capacities as well as the exchangeable cations concentrations Secondly thedevelopment of soil nutrient status with focus on carbon and nitrogen are outlined A complete list ofparameter means (with standard deviations) as they developed over time and after lime treatment isavailable as Table S4 (G1) and S5 (G2) in Supplementary Materials The parameter response ratio (RR)means SD and ranges are fully detailed in Tables S6 (G1) and S7 (G2) of Supplementary Materials

31 Liming Effects in 2003

In 2003mdashtwenty years after the first lime treatment in 1983mdashno significant differences could beseen in soil pH or base saturation between the control and limed plots The mean values at limed plotstended to be higher for both parameters especially in the O-layer (pH) and 0ndash5 cm mineral soil (BS)

Soil Syst 2020 4 38 8 of 33

however the confidence intervals of both control and lime treatment overlap Similarly sum CECby 2003 was comparable throughout the entire soil profile also G2 site 0ndash5 cm mineral soil sampleexchangeable Ca as well as Ctot and Ntot were significantly increasedmdasha potential residual effect oflime application in 1983mdashyet even here the increase in CEC was only slight and not significant G1 sitelimed plot O-layer total Al and total Fe concentrations were significantly higher compared to controlalthough again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in theentire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer andfrom pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pHunits) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pHunits) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however thisrecovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layerand from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

Soil Syst 2020 4 x FOR PEER REVIEW 8 of 35

significant G1 site limed plot O-layer total Al and total Fe concentrations were significantly higher compared to control although again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in the entire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer and from pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in 0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pH units) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pH units) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however this recovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layer and from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1 and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pH units at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010 and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots with group average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in the O-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the difference between the control and limed plots was significant in all G1 measured soil profile depths in 2010 the treatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 years since the last lime application At G2 sites the liming effect reached significance only down to 10 cm mineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

(a)

(b)

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites(b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 38 9 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 9 of 35

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Similar development in both natural recovery and liming effects over time was seen also in pH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronounced in the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect only down to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen across all study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) The average RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in 2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below 20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significant increase in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime application This liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa 4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the 0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in both the 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pHunits at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots withgroup average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in theO-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the differencebetween the control and limed plots was significant in all G1 measured soil profile depths in 2010 thetreatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 yearssince the last lime application At G2 sites the liming effect reached significance only down to 10 cmmineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

Similar development in both natural recovery and liming effects over time was seen also inpH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronouncedin the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect onlydown to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen acrossall study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) Theaverage RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in

Soil Syst 2020 4 38 10 of 33

2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significantincrease in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime applicationThis liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa

4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in boththe 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just a 1ndash3 increasein group average BS Compared to the control plots both G1 and G2 limed plot BS was significantlyhigher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plotbase saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and9ndash12 in 30ndash60 cm mineral soil

Soil Syst 2020 4 x FOR PEER REVIEW 10 of 35

a 1ndash3 increase in group average BS Compared to the control plots both G1 and G2 limed plot BS was significantly higher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80 in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plot base saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and 9ndash12 in 30ndash60 cm mineral soil

(a)

(b)

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 studysites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differencesbetween current and previous sampling campaign

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 7: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 7 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 6 of 35

H2O and 1 M KCl mineral soil exchangeable cations Ca2+ Mg2+ K+ Al3+ Fe3+ (μmolc gminus1) and their sum CEC (including cations Na+ Mn2+ and H+) as well as the calculated mineral soil base saturation () were determined via percolation with 1 M NH4Cl-solution and extract analysis with ICP-OES total N and total C (g kgminus1) were measured in dry combustion (Woumlsthoff in 1980s Leco CN 2000 in 2003 Vario Max Elementar in 2010ndash2015) and CN ratio was calculated total Ca Mg K Al and Fe (g kgminus1) in the O-layer only were determined in aqua regia extract organic layer stocks (t haminus1) were calculated form dried soil samples of defined sampled area The methodology of our laboratory analyses was according to ldquoHandbuch Forstliche Analytikrdquo (ldquoHandbook of Forest Analysisrdquo HFA) by the Forest Analysis Advisory Committee (GAFA) [26ndash28] Our original data is available as Table S1 S2 and S3 in Supplementary Materials

It was assumed that the mineral soil bulk density remained stable during the different sampling periods at the study sites and therefore the element concentrations may be directly compared between the sampling years and between the directly adjacent treatment variants without considering element stocks

The element concentrations in 2015 were aggregated from 10ndash20 to 20ndash30 cm depth samples into 10ndash30 cm according to fine earth stocks for better comparison with the previous sampling periods pH values were aggregated after conversion into H+ concentration (mol Lminus1) and subsequent reconversion into pH Bulk density and fine earth stocks were estimated only in 2015 from soil sample volume weight and coarse soil fraction

23 Statistical Analysis

The statistical evaluations were conducted using R 363 (R Core Team 2019) First of all a K-means cluster analysis (CA) was conducted in order to explore the similarity of

sites by their soil chemical parameters at 0-30 cm control plot mineral soil (aggregated sampling campaign 2015 n = 49) whereby the exchangeable cation as well as Ctot and Ntot concentrations were calculated in stocks (t haminus1) according to fine earth stocks for better site comparability The optimal number of clusters ie groups of sites was determined to be 2 Group 1 contains the study sites ldquoBad Waldseerdquo ldquoEllwangenrdquo ldquoFreudenstadtrdquo ldquoHeidelbergrdquo and ldquoOchsenhausenrdquo (n = 5) and Group 2 the sites ldquoHerzogenweilerrdquo ldquoHorbrdquo ldquoHospitalrdquo ldquoWangenrdquo and ldquoWeithardrdquo (n = 5 Table 1) Additionally a principal component analysis (PCA) was run in order to confirm the CA results as well as determine the most relevant soil chemical principal components (PC) of these site groups The first two PCs explained 649 of the variability in data and were pH-H2O pH-KCl and K+ (t haminus1 PC-1) Ctot (t haminus1) and CEC (μmolc gminus1 PC-2 Figure 1)

(a)

(b)

Figure 1 Principal component analysis (PCA) to characterize study site grouping parameters (a) studysites and (b) principal components

To estimate the natural recovery as well as the effects of lime application over time ie thedifference between two sampling periods within a study site group a relative response ratio (RRr) wascalculated for each of the relevant site parameters based on methodology in Hedges et al [29] andReid and Watmough [17]

RRr = (t2t1) minus 1 (1)

where t1 = site plot average (arithmetic mean) in previous sampling period t2 = site plot average infollowing sampling period In case of already relative (CN) log-transformed (pH) and discontinuous(base saturation) variables an absolute RRa was calculated as difference between previous and followingsampling year or limed and control treatment

RRa = t2 minus t1 (2)

3 Results

Since the 1980s sampling design and data set was not comparable with the subsequent campaignsfrom 2003 until 2015 we were not able to analyze statistically the changes in soil chemical propertiesof the entire measured soil profile of our studied sites for the period 1980s until 2003 Neverthelesswith the sampling data of 2003 we can evaluate the liming effects in this initial study period on soilproperties with the direct comparison of control and limed plots From 2003 on we can describe thedevelopment of soil chemical properties with respect to liming effects in great detail In this contextwe will first of all present the changes in soil acidity status with focus on pH values base saturationand cation exchange capacities as well as the exchangeable cations concentrations Secondly thedevelopment of soil nutrient status with focus on carbon and nitrogen are outlined A complete list ofparameter means (with standard deviations) as they developed over time and after lime treatment isavailable as Table S4 (G1) and S5 (G2) in Supplementary Materials The parameter response ratio (RR)means SD and ranges are fully detailed in Tables S6 (G1) and S7 (G2) of Supplementary Materials

31 Liming Effects in 2003

In 2003mdashtwenty years after the first lime treatment in 1983mdashno significant differences could beseen in soil pH or base saturation between the control and limed plots The mean values at limed plotstended to be higher for both parameters especially in the O-layer (pH) and 0ndash5 cm mineral soil (BS)

Soil Syst 2020 4 38 8 of 33

however the confidence intervals of both control and lime treatment overlap Similarly sum CECby 2003 was comparable throughout the entire soil profile also G2 site 0ndash5 cm mineral soil sampleexchangeable Ca as well as Ctot and Ntot were significantly increasedmdasha potential residual effect oflime application in 1983mdashyet even here the increase in CEC was only slight and not significant G1 sitelimed plot O-layer total Al and total Fe concentrations were significantly higher compared to controlalthough again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in theentire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer andfrom pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pHunits) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pHunits) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however thisrecovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layerand from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

Soil Syst 2020 4 x FOR PEER REVIEW 8 of 35

significant G1 site limed plot O-layer total Al and total Fe concentrations were significantly higher compared to control although again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in the entire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer and from pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in 0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pH units) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pH units) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however this recovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layer and from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1 and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pH units at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010 and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots with group average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in the O-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the difference between the control and limed plots was significant in all G1 measured soil profile depths in 2010 the treatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 years since the last lime application At G2 sites the liming effect reached significance only down to 10 cm mineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

(a)

(b)

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites(b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 38 9 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 9 of 35

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Similar development in both natural recovery and liming effects over time was seen also in pH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronounced in the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect only down to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen across all study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) The average RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in 2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below 20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significant increase in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime application This liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa 4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the 0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in both the 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pHunits at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots withgroup average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in theO-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the differencebetween the control and limed plots was significant in all G1 measured soil profile depths in 2010 thetreatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 yearssince the last lime application At G2 sites the liming effect reached significance only down to 10 cmmineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

Similar development in both natural recovery and liming effects over time was seen also inpH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronouncedin the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect onlydown to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen acrossall study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) Theaverage RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in

Soil Syst 2020 4 38 10 of 33

2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significantincrease in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime applicationThis liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa

4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in boththe 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just a 1ndash3 increasein group average BS Compared to the control plots both G1 and G2 limed plot BS was significantlyhigher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plotbase saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and9ndash12 in 30ndash60 cm mineral soil

Soil Syst 2020 4 x FOR PEER REVIEW 10 of 35

a 1ndash3 increase in group average BS Compared to the control plots both G1 and G2 limed plot BS was significantly higher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80 in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plot base saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and 9ndash12 in 30ndash60 cm mineral soil

(a)

(b)

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 studysites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differencesbetween current and previous sampling campaign

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 8: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 8 of 33

however the confidence intervals of both control and lime treatment overlap Similarly sum CECby 2003 was comparable throughout the entire soil profile also G2 site 0ndash5 cm mineral soil sampleexchangeable Ca as well as Ctot and Ntot were significantly increasedmdasha potential residual effect oflime application in 1983mdashyet even here the increase in CEC was only slight and not significant G1 sitelimed plot O-layer total Al and total Fe concentrations were significantly higher compared to controlalthough again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in theentire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer andfrom pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pHunits) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pHunits) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however thisrecovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layerand from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

Soil Syst 2020 4 x FOR PEER REVIEW 8 of 35

significant G1 site limed plot O-layer total Al and total Fe concentrations were significantly higher compared to control although again without any notable influence on the pH or CEC

32 Soil Acidity Status Development between 2003 and 2015

321 pH Values

A tendency towards natural recovery of soil pH-H2O was observed between 2003 and 2015 in the entire soil profile of G1 study sites (Figure 2a) from group average pH 35 to pH 39 in the O-layer and from pH 35ndash43 to pH 39ndash46 in the 0ndash60 cm mineral soil The rate of response (RR) was significant in 0ndash5 cm and 10ndash60 cm mineral soil by 2010 (RRa 01ndash02 pH units) and in the O-layer by 2015 (RRa 03 pH units) (Figure 3a) At G2 sites (Figure 2b) the natural recovery was significant in O-layer (RRa 02 pH units) and 10ndash30 cm mineral soil (RRa 03 pH units) between 2003 and 2010 By 2015 however this recovery was no longer significant The G2 group average shifted from pH 37 to pH 39 in the O-layer and from pH 36ndash43 to pH 38ndash46 in the 0ndash60 cm mineral soil in the period from 2003 until 2015

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1 and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pH units at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010 and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots with group average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in the O-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the difference between the control and limed plots was significant in all G1 measured soil profile depths in 2010 the treatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 years since the last lime application At G2 sites the liming effect reached significance only down to 10 cm mineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

(a)

(b)

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites(b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 38 9 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 9 of 35

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Similar development in both natural recovery and liming effects over time was seen also in pH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronounced in the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect only down to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen across all study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) The average RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in 2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below 20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significant increase in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime application This liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa 4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the 0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in both the 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pHunits at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots withgroup average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in theO-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the differencebetween the control and limed plots was significant in all G1 measured soil profile depths in 2010 thetreatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 yearssince the last lime application At G2 sites the liming effect reached significance only down to 10 cmmineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

Similar development in both natural recovery and liming effects over time was seen also inpH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronouncedin the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect onlydown to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen acrossall study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) Theaverage RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in

Soil Syst 2020 4 38 10 of 33

2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significantincrease in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime applicationThis liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa

4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in boththe 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just a 1ndash3 increasein group average BS Compared to the control plots both G1 and G2 limed plot BS was significantlyhigher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plotbase saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and9ndash12 in 30ndash60 cm mineral soil

Soil Syst 2020 4 x FOR PEER REVIEW 10 of 35

a 1ndash3 increase in group average BS Compared to the control plots both G1 and G2 limed plot BS was significantly higher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80 in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plot base saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and 9ndash12 in 30ndash60 cm mineral soil

(a)

(b)

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 studysites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differencesbetween current and previous sampling campaign

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 9: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 9 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 9 of 35

Figure 2 pH-H2O in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Similar development in both natural recovery and liming effects over time was seen also in pH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronounced in the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect only down to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen across all study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) The average RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in 2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below 20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significant increase in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime application This liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa 4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the 0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in both the 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just

Figure 3 pH-H2O site average response ratio (RRa) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

At lime treated plots pH-H2O has been increasing significantly in the entire soil profile of both G1and G2 sites between 2003 and 2010 ie in the first 7 years since second lime application by 02ndash22 pHunits at G1 and 02ndash17 pH units at G2mdashthe RR decreasing with depth (Figure 3ab) Between 2010and 2015 the rise in limed mineral soil pH-H2O was again comparable to that of control plots withgroup average 01ndash03 (G1) and 01ndash02 (G2) pH unit increase in the mineral soil profile although in theO-layer the pH is once again decreasing by mean 10 (G1) and 05 (G2) pH units While the differencebetween the control and limed plots was significant in all G1 measured soil profile depths in 2010 thetreatment effect has lost its significance in 30ndash60 cm mineral soil by 2015 ie the period 7ndash12 yearssince the last lime application At G2 sites the liming effect reached significance only down to 10 cmmineral soil by 2010 moving further down in the soil profile to 30 cm mineral soil by 2015

Similar development in both natural recovery and liming effects over time was seen also inpH-KCl (see Appendix B Tables A3 and A4) The effect of lime treatment was even more pronouncedin the O-layer and topsoil 0ndash5 cm but overall the limed plots had a significant treatment effect onlydown to 10 cm topsoil at G1 and just down to 5 cm at G2

322 Base Saturation

From 2003 on a tendency towards slight natural recovery of base saturation (BS) was seen acrossall study sites although significant only in case of G2 site 0ndash5 cm topsoil (Figures 4 and 5) Theaverage RRa in the 0ndash60 cm soil profile was 1ndash5 in 2003ndash2010 and 4ndash9 (G1) and 05ndash7 (G2) in

Soil Syst 2020 4 38 10 of 33

2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significantincrease in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime applicationThis liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa

4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in boththe 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just a 1ndash3 increasein group average BS Compared to the control plots both G1 and G2 limed plot BS was significantlyhigher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plotbase saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and9ndash12 in 30ndash60 cm mineral soil

Soil Syst 2020 4 x FOR PEER REVIEW 10 of 35

a 1ndash3 increase in group average BS Compared to the control plots both G1 and G2 limed plot BS was significantly higher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80 in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plot base saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and 9ndash12 in 30ndash60 cm mineral soil

(a)

(b)

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 studysites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differencesbetween current and previous sampling campaign

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 10: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 10 of 33

2010ndash2015 Except for some of the sites of G1 in 2015 the control plot base saturation remained below20 ie poor

The liming effect after 2003 was especially strong at G1 sites with an average 30ndash60 significantincrease in 0ndash10 cm topsoil BS and 7ndash11 in 10ndash60 cm in the first 7 years after second lime applicationThis liming effect continuedmdashwith a 0ndash10 cm topsoil reduction in RRa to just 6ndash20 and 10ndash60 cm RRa

4ndash8mdashalso until 2015 At G2 sites the lime treatment effect was comparably lower 15ndash30 in the0ndash10 cm topsoil and 4ndash7 in 10ndash60 cm between 2003 and 2010 By 2015 the RRa had dropped in boththe 0ndash10 cm topsoil to 7ndash15 as well as in the deeper soil horizons 10ndash60 cm to just a 1ndash3 increasein group average BS Compared to the control plots both G1 and G2 limed plot BS was significantlyhigher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plotbase saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and9ndash12 in 30ndash60 cm mineral soil

Soil Syst 2020 4 x FOR PEER REVIEW 10 of 35

a 1ndash3 increase in group average BS Compared to the control plots both G1 and G2 limed plot BS was significantly higher in the entire mineral soil profile both 7 and 12 years since the second lime application 75ndash80 in 0ndash5 cm 35ndash55 in 5ndash10 cm 15ndash25 in 10ndash30 cm and 12ndash15 in 30ndash60 cm mineral soil G2 limed plot base saturation was generally lower 45ndash55 in 0ndash5 cm 20ndash30 in 5ndash10 cm 11ndash12 in 10ndash30 cm and 9ndash12 in 30ndash60 cm mineral soil

(a)

(b)

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 study sites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

Figure 4 Base saturation in the soil profiles of control and lime treated plots in 2003ndash2015 (a) G1 studysites (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differencesbetween current and previous sampling campaign

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 11: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 11 of 33Soil Syst 2020 4 x FOR PEER REVIEW 11 of 35

(a)

(b)

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stable throughout the following sampling periods in the mineral soil profiles at both G1 and G2 study sites with no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010 (RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notably decreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronounced increase in base cations appeared to balance out the decrease in acid cations so that the CEC did not change significantly at the limed plots No significant lime treatment effect on total CEC could be observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in 0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acid cations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cation concentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantly greater than control progressively with time

Figure 5 Base saturation site average response ratio (RRa) seven years after (2003ndash2010) and twelveyears after the second lime treatment (2010ndash2015) (a) G1 study sites (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

323 Cation Exchange Capacities

From 2003 the sum of the control plot exchangeable cations (CEC Figure 6) has remained stablethroughout the following sampling periods in the mineral soil profiles at both G1 and G2 study siteswith no significant differences between the sampling years

At limed plots the 0ndash5 cm upper topsoil CEC at G1 sites was significantly higher in 2010(RR 073)mdashmainly due to greatly increased availability of Ca and Mg base cations and despite notablydecreased Al and Fe-III acid cation concentrations At G1 5ndash30 cm this similar but less pronouncedincrease in base cations appeared to balance out the decrease in acid cations so that the CEC didnot change significantly at the limed plots No significant lime treatment effect on total CEC couldbe observed in the topsoil G2 sites (although from 2010 to 2015 CEC did increase significantly in0ndash5 cm topsoil RRr 015) where Ca and Mg cation concentrations increased distinctly and the acidcations decreased Since the base cation increase reached down to 60 cm mineral soil and acid cationconcentration only decreased in the upper 10 cm due to liming G2 limed plot CEC became significantlygreater than control progressively with time

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 12: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 12 of 33Soil Syst 2020 4 x FOR PEER REVIEW 12 of 35

(a)

(b)

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots 2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeable Ca2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010 and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in the first seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1 RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010 the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong at G1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1 (RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developed similarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg 2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionally the liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2 study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B) What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between 2010 and 2015 irrespective of treatment

Figure 6 Control plot exchangeable cations (CEC) in the soil profile of the control and limed plots2003ndash2015 (a) G1 sites and (b) G2 sites mdashlimed plots significantly different from control mdashsignificantdifferences between current and previous sampling campaign

At the control plots there was a tendency for an increase of total Ca in the O-layer and exchangeableCa2+ in the mineral soil (Figure 7) which was significant at G1 sites until 10 cm topsoil between 2010and 2015 (RRr 08ndash56) and at G2 sites 0ndash5 cm between 2003 and 2010 (RRr 071)

The effect of lime treatment on forest floor total Ca-concentration is a significant increase in thefirst seven years after the second lime application (RRr 305ndash733) and a decrease (significant for G1RRr minus034) ie the reverse process between 2010 and 2015 across all study sites Between 2003 and 2010the mineral soils experienced a significant increase of exchangeable Ca in 0ndash30 cm especially strong atG1 sites (RRr 572ndash1861) Afterwards Ca concentrations increased significantly only in 0ndash10 cm at G1(RRr 106ndash16) and just slightly at G2 sites

Both organic layer total Mg and mineral soil exchangeable Mg2+ (see Appendix B) developedsimilarly to Ca The difference was a significant recovery at G2 control plots in the O-layer Mg2003ndash2015 (RRr 034 and 025) without any significant improvement further down Additionallythe liming effect significance reached down to 60 cm mineral soil in 2003ndash2010 at both G1 and G2study sites

There was little change in the concentrations of the other base cations K and Na (see Appendix B)What is notable is the significant reduction of exchangeable K in 30ndash60 cm depth at G2 sites between2010 and 2015 irrespective of treatment

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

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2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 13: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 13 of 33Soil Syst 2020 4 x FOR PEER REVIEW 13 of 35

(a)

(b)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differences between current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in the control plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soil exchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time (G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in 2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr -01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed a trend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sites between 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067 and G2 RRr minus037)

Figure 7 Calcium response ratio (RRr) in the soil profile seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 sites and (b) G2 sites mdashsignificant differencesbetween current and previous sampling campaign

It became obvious that Al was the strongly dominant exchangeable cation and remained so in thecontrol plots throughout the entire sampling period 2003ndash2015 Forest floor total Al and mineral soilexchangeable Al concentrations (Figure 8) at the control plots showed no significant change over time(G1 RRr minus009ndash133 and G2 RRr minus013ndash034) only the G2 site O-layer Al was significantly higher in2010 compared to 2003 (RRr 022) and in 10ndash30 cm significantly lower (RRr minus01)

In response to the second liming treatment in 2003 mineral topsoilsrsquo exchangeable Al followed atrend opposite to that of Ca and Mg and was distinctly reduced in 0ndash10 cm at both G1 and G2 sitesbetween 2003 and 2010 at G1 and G2 though significantly only in 0ndash5 cm topsoil by 2010 (G1 RRr minus067and G2 RRr minus037)

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cmmineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Feconcentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in thelimed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed justwith low absolute values which however resulted in significant RR-values whereby Fe-concentrationsincreased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 14: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 14 of 33Soil Syst 2020 4 x FOR PEER REVIEW 14 of 35

(a)

(b)

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

Soil Fe concentrations (see Appendix B) were obviously present at all sites especially in the 0ndash10 cm mineral soils Significant changes over time in the topsoil occurred at G2 sites only where total Fe concentrations increased in the control plot O-layer (RRr 037) and exchangeable Fe decreased in the limed plot 0ndash5 cm (RRr minus036) in the period 2003ndash2010 The subsoil Fe concentrations changed just with low absolute values which however resulted in significant RR-values whereby Fe-concentrations increased in 2003ndash2010 and slightly decreased in 2010ndash2015mdashmore or less significantly at all study sites

Across all study sites forest floor total Mn concentrations were significantly higher at limed plots relative to control 7 and 12 years since the last lime application in addition after liming also the exchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots compared to control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2) in 2015

33 O-layer stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to be considered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly) lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limed plot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at control

Figure 8 Aluminum site average response ratio (RRr) seven years after (2003ndash2010) and twelve yearsafter the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificantdifferences between current and previous sampling campaign

Across all study sites forest floor total Mn concentrations were significantly higher at limed plotsrelative to control 7 and 12 years since the last lime application in addition after liming also theexchangeable Mn in 0ndash5 cm topsoil was significantly higher at G1 sites (see Appendix B)

Exchangeable protons H (also see Appendix B) were significantly lower at limed plots comparedto control in 0ndash5 cm topsoil in 2010 for both G1 and G2 as well as in 0ndash10 cm (G1) and 0ndash5 cm (G2)in 2015

33 O-layer Stocks Carbon and Nitrogen

For the evaluation of changes in carbon concentrations the humus layer stocks have to beconsidered too (Figure 9) At both G1 and G2 study sites the O-layer stocks were (not significantly)lower at limed plots relative to control in 2003 and in 2010 they were comparable In 2015 the limedplot O-layer stocks were significantly lower due to a tendency of increasing O-layer stocks at controlplots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significantand G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus thechanges of the concentrations could be compared directly

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 15: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 15 of 33

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b)G2 study sites mdashlimed plots significantly different from control mdashsignificant differences betweencurrent and previous sampling campaign

Soil Syst 2020 4 x FOR PEER REVIEW 15 of 35

plots (G1 RRr 015 ns and G2 RRr 032 ns) and a decrease at limed plots (G1 RRr minus03 significant and G2 RRr minus025 ns Figure 10) In the mineral soil we assumed constant fine earth stocks thus the changes of the concentrations could be compared directly

(a)

(b)

Figure 9 Organic layer stocks of control and lime treated plots in 2003ndash2015 (a) G1 study sites and (b) G2 study sites mdashlimed plots significantly different from control mdashsignificant differences between current and previous sampling campaign

(a)

(b)

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) and twelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sites mdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015 (see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparable to that of the control At G1 sites Ctot remained comparable between the control and limed except for the significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrations rose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained on average unchanged since 2003 with a tendency to increase in the entire measured mineral soil

Figure 10 Organic layer stock site average response ratio (RRr) seven years after (2003ndash2010) andtwelve years after the second lime treatment (2010ndash2015) (a) G1 study sites and (b) G2 study sitesmdashsignificant differences between current and previous sampling campaign

The control plots show little significant change in carbon concentrations between 2003 and 2015(see Appendix B) Only the G1 site O-layer Ctot significantly decreased in 2010ndash2015 (RRr minus012)

Between 2003 and 2010 this Ctot was significantly decreasing however and was again comparableto that of the control At G1 sites Ctot remained comparable between the control and limed except forthe significantly lower O-layer Ctot in 2010 In 0ndash10 cm topsoil of limed G1 sites Ctot concentrationsrose significantly in the period 2003ndash2010 (RRr 028ndash061)

At the control plots the total nitrogen in the soil profile of G1 sites (see Appendix B) remained onaverage unchanged since 2003 with a tendency to increase in the entire measured mineral soil profileSimilarly at G2 sites except for significantly increased Ntot in 0ndash5 cm between 2010 and 2015 (RRr 034)

At limed plots the only significant rise in Ntot concentrations occurred in 0ndash5 cm topsoil At G1the RR was 065 between 2003 and 2010 leading to significantly higher Ntot between limed and controlplots in 2010 G2 site Ntot concentrations significantly dropped (RRr -032) only to once again increasein 2010ndash2015 (RRr 032 overall similar development to Ctot)

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 16: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 16 of 33

While at G2 sites the CN ratio remained comparable between the sampling periods 2003ndash2015and between both control and limed plots at G1 sites CN significantly increased in the limed plotO-layer between 2010 and 2015 so that lime treated site CN was 27 and control CN was 24 in 2015Meanwhile in 0ndash5 cm mineral soil limed plot CN decreased (ns) and limed plot CN of 19 wassignificantly lower than the control plot CN of 21

4 Discussion

After a short discussion on methodological characteristics and boundary conditions of our studywe will discuss the temporal development of soil chemistry at the control plots which will allow us toevaluate the extent of natural recovery Afterwards we will assess the effects of lime treatment as theintended counter-measure to soil acidification We differentiated our study sites by their soil chemicaland physical properties to identify those site parameters which affect both the rate of natural recoveryand response to liming

41 Discussion on Methods and Boundary Conditions of the Study

The soil sampling in the campaigns of 2003 and 2010 were focused upon element concentrationsbeing analyzed at disturbed bulk samples which did not allow for calculation of element stocks Onlyin the last campaign 2015 volumetric soil samples were taken allowing for determination of bulkdensity of fine earth and volumetric content of the coarse soil fraction However also the volumetricreference is somehow unsharp because the samples were taken with an auger and artificial compactionof the soil samples cannot be excluded Due to that uncertainty and above all because of comparabilityamong the results of the sampling campaigns we decided to perform all evaluations on the basis ofelement concentrations

The dosage of the lime application between the liming campaigns in 198384 and 2003 weredifferentmdashthe latter was with 6 Mg haminus1 roughly double the dosage of the first campaign Vice versawere the ldquoreaction timesrdquo of both liming campaigns The effect of the first campaign was observed in2003 20 years after liming Between 1983 and 2003 the highest acid load from deposition in CentralEurope occurred [30] Therefore it is probable that a high proportion of the buffer capacity from thefirst campaign was neutralized by deposition before 2003 Both observation periods 2003ndash2010 and2010ndash2015 with a length of 7 and 5 years were more or less comparable but much shorter than 20years The fact that this study is based on data from three sampling campaigns provides some insightin the dynamics of both the natural recovery as well as the lime treatment effects which can be derivedpredominantly from the RR plots However the assessment of the exact temporal dynamics of theliming effects are incriminated with uncertainty and may only been derived as tendencies

42 Natural Recovery of Acidified Soils

A natural recovery of soil pH that we found was overall slight and comparable in both H2O andKCl throughout the entire soil profile Between 2003 and 2015 pH-H2O rose by 06ndash07 pH units in theorganic horizon and by 02ndash03 pH units in mineral soil In the O-layer and 0ndash10 cm topsoil the pH-H2Oremained le 42 and pH-KCl le 35 ie extremely acidic until 2015 The average pH-KCl of 30 in themineral topsoil samples of our study sites in the 1980s [23] (pp 36ndash37) thus has seen little improvementover three decades In the comparison between Germanyrsquos 1st and 2nd National Forest Soil Inventory(NFSI) at acidification-sensitive unlimed sites Meesenburg et al [12] (p 100) found pH-H2O hadincreased in the O-layer and 0ndash10 cm mineral soil from 1987ndash1992 until 2006ndash2008 although without asignificant change in pH-KCl An effect of increasing pH values in the subsoil which we found inour study has not yet been reported (to our knowledge) as a consequence of reduced acid depositionWhile at G1 sitesmdashwhich had overall lower pH-KCl lower CEC and higher exchangeable Al stocks inthe topsoil as well as predominantly coarser soil-fractionsmdasha distinct recovery was already seen from2003 until 60 cm in the soil profile at G2 sites the natural recovery was significant only to the depth of30 cm mineral soil

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 17: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 17 of 33

After 2003 only slight changes in the mineral soil base saturation could be observed at the controlplots which for the most part remained at lt 20 BS The comparison between NFSI I and II foundprevailing low topsoil base saturation in almost every region in Germany and loss of BS in 5ndash90 cm soilprofiles of unlimed acid-sensitive soils noting that the base cation uptake as tree nutrients as well asremobilization of S and nitrification processes may have contributed to this trend [12] (p 102) In ourstudy we found the base cations Ca and Mg tended towards natural recovery which was however onlysignificant in the O-layer (Mg) or in topsoil (Ca) No improvement was found for K concentrationswhich irrespective of treatment even declined in the 30ndash60 cm subsoil between 2010 and 2015 All-in-alldespite the slight recovery we observed at our study sites pH values and base saturation are still farfrom pre-industrial values which are reported or modeled to have been distinctly higher [9]

Since the control plot pH-H2O of le 42 in the topsoil is still predominantly in the Al and Al-Febuffer range [12] (p 95) which Wilpert et al [23] (pp 37ndash38) found already in our 1980s samples andthe base saturation remained low the lack of reduction in the acid cation Al and Fe concentrations thatwe found is not surprising Thus there has been little change in control plot CEC and the exchangeablecation concentrations over time

While in Wilpert et al [23] (pp 31ndash34) increased O-layer thickness at the control plots from198586 to 198990 was reported from 2003 on neither O-layer stocks or Ctot and Ntot concentrationschanged significantly at our control plots except for a significant decrease in the O-layer Ctot at G1 anda significant increase of 0ndash5 cm topsoil Ntot at G2 between 2010 and 2015 There was no noticeablechange in the CN ratio

43 Effects of Liming

The depth gradient of liming was obvious whereby a downward movement of lime treatmenteffects in the soil profile over time occurred A simplified interpretation of the RR-values gives theimpression that the liming effects are very strong in the first period and hardly significant in the secondperiod and thus have lessened substantially However this could also mean that the strong effectsof liming in the first observation period are still ongoing but with no further strong amplificationDolomite limestone has principally low solubility which is likely an important factor in our studyThe solution rate of limestone is controlled by the factors humidity CO2 partial pressure and pHvalue [31] (pp 195ndash197) Humidity and CO2 partial pressure are on the mid-term constant factorsand thus limiting the solution rate constantly Low pH values on heavily acidified soils acceleratethe dissolution rate As we found distinctly increased pH values as a direct effect of liming in thereverse one can conclude that this pH increase should decelerate the further dissolution rate Thus wecannot assume whether the liming effects of the second high-dosed liming campaign have weakenedessentially or dissolution rates are reduced and thus the liming effects have not yet developed fully inthe last observation period 2010ndash2015

Li et al [16] identified increased liming rate as the main driver in soil pH improvements whichmight explain why the first lime application of 3 t haminus1 in 1980s no longer had a significant effectcompared to control plot pH by 2003 Wilpert et al [23] (pp 36ndash38) saw the liming effect on topsoil pHdecline already 5ndash6 years after treatment with an increase of just 02 pH units then compared to 09 pHunits 1ndash2 years after The second lime dose of 6 t haminus1 made a notable difference both 7 and 12 yearsafter application Similar to the findings of Pabian et al [32] Court et al [13] and Meesenburg et al [12](p 100) our study showed that liming greatly accelerated the rise in soil pH-H2O compared to controlplots by 06ndash22 units down to 10 cm topsoil and a decreasing (yet still significant) effect with depthin the entire measured soil profile during the first 7 years since 2003 treatment In the followingyearsmdashbetween 2010 and 2015mdashthe limed plot forest floor pH was again decreasing though thepositive difference to control remained significant Draacutepelovaacute et al [10] also found reacidification oflimed Ol-horizon 12 years after treatment while the deeper horizons did still show decreased aciditycompared to the control

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 18: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 18 of 33

The effect of liming appears to have reached greater depthmdashup to 60 cmmdashin the soil profiles of G1sites in less time compared to G2 where below 30 cm mineral soil the limed treatment was no longersignificantly different from the control in the first 7 years since last lime treatment In the 7ndash12 yearperiod the pH change at both G1 and G2 plots was lower and comparable to natural regeneration(although limed plot pH still remained significantly higher than the control) Li et al [16] saw themaximum effect of lime in the first 3 years after application although the different environmental andecological conditions potentially delay or reduce liming effects Their study found that lower initialsoil pH led to stronger liming effects as well as increased variances Reid and Watmough [17] alsoshowed that initially extremely acidic sites treated with high doses showed the highest increase in pHIn our case from 2003 on the soil pH-H2O values were comparable at G1 and G2 sites while pH-KClwas lower at G1 indicating that perhaps the soil texture differences (a higher sand fraction in G1 soilprofiles) had impact on the site-specific development in soil pH-KCl

The temporal change in soil pH-KCl due to lime application was similar in the O-layer and0ndash10 cm (G1) and 0ndash5 cm (G2) topsoil while further down in the soil profiles no significant limingeffect was observed Huber et al [33] found similar results While pH-H2O is a measure of the effectivesoil acidity and shows seasonal fluctuations pH-KCl takes into account also the potential acidity ofreleased exchangeable Al and H in soil and therefore is a long-term measure of soil pH [12] (p 97)Indeed we found no significant reduction in exchangeable Al or proton concentrations below 10 cmdepth at our limed plots which indicates that the subsoil of limed plots has not yet fully recoveredfrom acidification

The total Al and Fe concentrations were significantly higher in the O-layer of G1 limed plotsin 2003 ie 20 years after the 1st lime treatment in the 1980s We presumed this resulted frombioturbation and subsequent mixing of mineral soil with the organic soil material notably lower Ctot

concentrations in the limed plot O-layer support this assumption The 2nd lime treatment in 2003obviously limitedmdashand even reversedmdashthe extent to which Al Fe and H cations were increasing atour study sites in the upper 0ndash10 cm soil profile by 2015 compared to the control A difference thatMeesenburg et al [12] (pp 99ndash100) found between NFSI I and II was a reduction in Al and Al-Fe bufferrange and an increase in the exchange buffer and even silicate buffer ranges at limed plots in 0ndash30 cmmineral soil

The 1st lime application in the 1980s improved topsoil base saturation at our study sites by 17after 5 years [23] (p 43) While by 2003 there was no significant difference between the limed andcontrol plot BS any more (except for still significantly higher exchangeable Ca in 0ndash5 cm topsoil)afterwards the 2nd lime treatment again made a significant impact improving base saturation in theentire 0ndash60 cm mineral soil profile of all study sitesmdashby 40ndash70 in the organic layer and by 7ndash50in mineral soil Specifically the concentrations of base cations Ca and Mgmdashthe main constituentsof dolomite limemdashrose significantly until 30 cm and 60 cm mineral soil respectively in the first 7years after last lime treatment Meanwhile neither Wilpert et al [23] (pp 44ndash45) nor we observeda distinct liming effect on K concentrations similar to findings of Huber et al [33] Court et al [13]found a BS of 9 at the control and 41 at the limed plots 16 years after treatment and significantlyincreased exchangeable Ca Mg and K in 0ndash15 cm topsoil Guckland et al [34] also found a significantlyincreased BS in 0ndash40 cm mineral soil 28 years after lime application with a mean increase of 11Meesenburg et al [12] (pp 102 110) showed an increase in 0ndash30 cm mineral soil BS between NFSI Iand II at limed sites especially on largely base-depleted plots

Our study found the limed plot BS response ratio was double in the soil profile of G1 sitescompared to G2 sites in 2003ndash2010 period despite the Ca concentrations being significantly higher inthe 0ndash5 cm topsoil of G2 limed sites compared to control in 2003 already (after the 1st lime applicationin 1980s) After 2010 ie 7ndash12 years since 2nd liming in both site groups the RRa of BS was declininghowever This is in agreement with findings of several studies that liming effects reached theirmaximum in the first decade after treatment [1335] and Reid and Watmough [17] who showed thattime since treatment has a major influence on BS response to liming Reid and Watmough [17] noted

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 19: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 19 of 33

that also soil type as well as the tree species would have an impact on the intensity and dynamic ofliming effects At our study sites we could not differentiate a stand effect as both groups contain amixture of stand types with varying dominance of Norway spruce The effect of soil types could alsonot be proven as they were from similar classes in our study however the texture seems to play adistinct role in differentiating G1 and G2 study site liming effect on BS This effect was also shown byLi et al [16] who found 32 higher liming effects in sandy soils than clayey soils His argument wasthat fine textured soils show a greater buffering capacity to changes in soil chemical properties thancoarse-textured soils

While at G1 sites limed plot CEC significantly increased compared to the control in the 0ndash5 cmtopsoil where as discussed the increase in BS as well as the decrease in Al and Fe was of greatermagnitude at G2 sites a significant rise in CEC was found in 10ndash60 cm subsoil where especially in30ndash60 cm the exchangeable Ca and Mg limed plot RRr still exceeded natural regeneration RRr by 2015Guckland et al [34] reported similarly increased CEC after liming due to increased exchangeable Caand Mg replacing exchangeable acidity andor Al3+ in the upper mineral soil meanwhile withouteffect on CEC in the 20ndash40 cm mineral soil These different reactions on liming at G1 and G2 sitesindicate different processes triggered on these site groups by lime application These processes couldbe on the one hand replacement of Al3+ with Ca2+ and Mg2+ as the statement of Guckland et al [34]suggests This process reduces the activity of Al-ions in the soil solution which generates protonsthrough hydrolysis [31] (pp 190ndash191) On the other hand the high increase of pH-H2O throughout thesoil profile down to 30ndash60 cm and the partially increased CEC suggest that according to the theory ofvariable charges of exchanger surfaces in the soil [31] (pp 170ndash173) the amount of negative charges undthus CEC increases with increasing pH The process behind that is an increase in pH-H2O functionalgroups of metal hydroxides (OH) of alumo-silicates (SiOH AlOH) and of carboxyl groups (COOH)that get de-protonized and thus increase the negative charge of the exchanger surfaces as well as CECThe third process that could explain changes of CEC is a translocation of carbon from the O-layerto the mineral soil This can generate new organic exchanger surfaces [31] (p 175) The significantincrease of CEC at G1 sites in 0ndash5 cm was accompanied by a significant and over-proportionally strongincrease of pH-H2O and indeed a significant increase of Ctot This suggests that in the more sandysoils of G1 sites the increase of organic carbon in combination with increased pH might have creatednew exchanger places and thus were the dominating process explaining increasing CEC there Thedescribed processes might also have occurred in 5ndash10 cm where similar changes were observed whichhowever were not as strong and overall not significant

At G2 sites with more loamy texture and higher colloid content and higher CEC at control plots aweak but significant increase of CEC occurred after liming in mineral soil layers below 10 cm Theonly predictor that shows at G2 sites a substantially higher reaction on liming in that depth layers isbase saturation This is due to a higher amount of Al being mobilized from the exchanger surfacesand replaced by Ca and Mg This depletion of Al is visible in Figure 8 to the depth of 30 cm At thedepth layer 30ndash60 cm Figure 8 shows no depletion of Al rather than a possible increase indicatingpartial resorption of Al mobilized in the upper soil layers It is somehow an unexpected finding thatat the more loamy G2 sites the liming effect on CEC reaches deeper than at G1 sites where a higherwater permeability could be expected according to the more sandy texture The explanation might bethe higher natural sorption capacity of G2 sites and perhaps preferential flow paths enhancing theldquoshort-cutrdquo like transport of Ca- and Mg-ions to deeper soil layers

We also found few distinct effects of liming on carbon and nitrogen properties of the studied siteswhich allow a further ecological discussion The limed plot O-layer stocks were comparable to those ofthe control in the 2003ndash2010 period Afterwards in 2010ndash2015 they were significantly lowermdashsimilar towhat Wilpert et al [23] (pp 31ndash34) observed 1 and 5 years after the 1980s lime treatment at our studysites Court et al [13] also found decreasing O-layer dry weight mid to long term after liming likelydue to enhanced microbial activity and accelerated decomposition rates Meanwhile Ctot decreasedin the O-layer and increased in the 0ndash10 cm topsoil of G1 sites in the first 7 years after 2nd lime

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 20: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 20 of 33

application Additionally Ntot concentrations rose in the 0ndash5 cm topsoil after liming Kreutzer (1995)showed changed O-layer morphology with increased mineral content in the O-layer and organic mattertransported downward as a result of earthworm activity at limed plotsmdashprobably this also occurred atour G1 study sites

At G2 sites 0ndash5 cm Ctot and Ntot were significantly higher at limed plots in 2003 potentially apersisting effect of the 1st lime treatment in 1980s where by the end of the 1980s increased varianceof the limed plot C-content in the topsoil was observed [23] (pp 34ndash35) After 2003 though bothcontrol and limed treatment Ctot and Ntot concentrations were comparable Ouimet and Moore [20]also observed no significant change in forest floor Ctot and Ntot concentrations after lime treatmentindicating no obvious change in mineralization rates

Despite G1 limed plot CN significantly increasing in the O-layer and significantly decreasingin 0ndash5 cm mineral topsoil between 2010 and 2015 CN ratio remained in the range typically underNorway spruce in cambisols podsols and stagnosols according to Cools et al [36]

5 Conclusions

Lime treatment has had notable positive effects on our soilrsquos recovery that are visible in theentire studied soil profile Thus in soils with proven soil acidificationmdashwhere it exceeds naturalacidificationmdashwe recommend liming to be established as a long-term forestry management practiceSite characteristics like soil texture and acidity status have to be taken into account when consideringthe site-specific outcomes of both natural and aided soil recovery

In order to evaluate even further the mechanisms of soil development in the process of recoveryfrom acidification over time it would be beneficial to expand the research at our study sites in thefuture Further measured ecosystem parameters could be evaluated eg possible changes in soilphysics and water budget that impact our soilrsquos hydrological functions as well as the biological activityof soil fauna plant root distributions and nutrients in plant biomass as important indicators of overallrecovery and stabilization of biodiversity and ecosystem functionality

Supplementary Materials The following are available online at httpwwwmdpicom2571-87894338s1Table S1 Original data O-layer chemistry 2003ndash2015 Table S2 Original data Mineral soil chemistry 2003ndash2015Table S3 Original data Mineral soil chemistry 2015 with stock calculations Table S4 G1 study site historicdevelopment in 2003ndash2015 (full version) Table S5 G2 study site historic development in 2003ndash2015 (full version)Table S6 G1 study site parameter response ratios (RR) to time in 2003ndash2015 (full version) Table S7 G2 study siteparameter response ratios (RR) to time in 2003ndash2015 (full version)

Author Contributions Conceptualization PH and KvW Data curation LJ PH and KvW Formal analysisLJ and PH Funding acquisition KvW Investigation LJ PH and KvW Methodology PH and KvWProject administration PH and KvW Software LJ Supervision PH and KvW Validation PH VisualizationLJ Writingmdashoriginal draft LJ Writingmdashreview and editing LJ PH and KvW All authors have read andagreed to the published version of the manuscript

Funding This research was funded by Bundesministerium fuumlr Ernaumlhrung und Landwirtschaft (BMEL) grantnumber 22028914 (2015ndash2017) and grant number 28W-B-4-075-02 (2018ndash2021)

Acknowledgments We would like to thank our predecessors who have set up and managed our long-termresearch sites and those many colleagues who have assisted in the field campaigns in sample preparationlaboratory analysis and lent advice and moral support throughout the many hours of data analysis

Conflicts of Interest The authors declare no conflict of interest The funders had no role in the design of thestudy in the collection analyses or interpretation of data in the writing of the manuscript or in the decision topublish the results

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 21: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 21 of 33

Appendix ASoil Syst 2020 4 x FOR PEER REVIEW 21 of 35

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015 given are group means with standard deviations Marked boldmdashsignificant differences between current and previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015 CN O-layer Control 2648 (148) 246 (263) 2441 (342) CN O-layer Limed 2398 (236) 2427 (18) 2716 (474) CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571) CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192) CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472) CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275) CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429) CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278) CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573) CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396) Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653) Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094) Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884) Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755) Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314) Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308) Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81) Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668) Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385) Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503) Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)

Figure A1 Study site location

Appendix B

Table A1 G1 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003ndash2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2648 (148) 246 (263) 2441 (342)CN O-layer Limed 2398 (236) 2427 (18) 2716 (474)CN 0ndash5 cm Control 2074 (348) 2096 (219) 2141 (571)CN 0ndash5 cm Limed 2068 (35) 2009 (312) 1872 (192)CN 5ndash10 cm Control 2152 (217) 2144 (357) 2143 (472)CN 5ndash10 cm Limed 1882 (357) 2041 (28) 1946 (275)CN 10ndash30 cm Control 2064 (457) 1814 (248) 1853 (429)CN 10ndash30 cm Limed 1728 (221) 1893 (297) 1799 (278)CN 30ndash60 cm Control 1782 (728) 1352 (299) 1345 (573)CN 30ndash60 cm Limed 1292 (261) 1533 (39) 1364 (396)Ctot gkg O-layer Control 40364(8113) 38575 (4488) 33814 (6653)Ctot gkg O-layer Limed 286 (10416) 30156 (8134) 32293 (6094)Ctot gkg 0ndash5 cm Control 4243 (2947) 4562 (2502) 5217 (2884)Ctot gkg 0ndash5 cm Limed 379 (1532) 5612 (2277) 6119 (2755)Ctot gkg 5ndash10 cm Control 2363 (1414) 2412 (1085) 2701 (1314)Ctot gkg 5ndash10 cm Limed 2208 (1114) 2676 (1046) 3201 (1308)Ctot gkg 10ndash30 cm Control 1249 (829) 1294 (604) 1314 (81)Ctot gkg 10ndash30 cm Limed 1437 (754) 1491 (623) 1565 (668)

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 22: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 22 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ctot gkg 30ndash60 cm Control 552 (419) 619 (398) 594 (385)Ctot gkg 30ndash60 cm Limed 658 (464) 745 (448) 73 (503)Fe gkg O-layer Control 252 (095) 35 (15) 431 (206)Fe gkg O-layer Limed 554 (192) 567 (258) 408 (201)

Fe3+ micromolcg 0ndash5 cm Control 891 (668) 1278 (954) 739 (356)Fe3+ micromolcg 0ndash5 cm Limed 687 (295) 472 (536) 155 (149)Fe3+ micromolcg 5ndash10 cm Control 39 (454) 783 (423) 439 (241)Fe3+ micromolcg 5ndash10 cm Limed 429 (317) 643 (487) 24 (285)Fe3+ micromolcg 10ndash30 cm Control 134 (173) 141 (152) 077 (071)Fe3+ micromolcg 10ndash30 cm Limed 077 (048) 181 (188) 078 (073)Fe3+ micromolcg 30ndash60 cm Control 033 (062) 098 (066) 023 (027)Fe3+ micromolcg 30ndash60 cm Limed 008 (006) 113 (158) 036 (074)H+ micromolcg 0ndash5 cm Control 1187 (316) 1777 (799) 1816 (1102)H+ micromolcg 0ndash5 cm Limed 135 (636) 455 (59) 303 (405)H+ micromolcg 5ndash10 cm Control 711 (564) 769 (462) 905 (644)H+ micromolcg 5ndash10 cm Limed 688 (495) 51 (417) 378 (378)H+ micromolcg 10ndash30 cm Control 242 (147) 247 (316) 211 (185)H+ micromolcg 10ndash30 cm Limed 171 (065) 136 (136) 17 (165)H+ micromolcg 30ndash60 cm Control 117 (056) 069 (101) 072 (062)H+ micromolcg 30ndash60 cm Limed 085 (082) 058 (064) 062 (058)K gkg O-layer Control 086 (022) 099 (015) 105 (028)K gkg O-layer Limed 117 (026) 129 (022) 122 (037)

K+ micromolcg 0ndash5 cm Control 083 (042) 074 (035) 103 (063)K+ micromolcg 0ndash5 cm Limed 07 (031) 096 (033) 096 (041)K+ micromolcg 5ndash10 cm Control 052 (022) 049 (015) 057 (018)K+ micromolcg 5ndash10 cm Limed 052 (021) 059 (027) 056 (017)K+ micromolcg 10ndash30 cm Control 042 (027) 043 (013) 045 (016)K+ micromolcg 10ndash30 cm Limed 047 (018) 048 (02) 049 (015)K+ micromolcg 30ndash60 cm Control 068 (059) 065 (036) 075 (068)K+ micromolcg 30ndash60 cm Limed 07 (058) 072 (039) 061 (037)Mn gkg O-layer Control 085 (069) 087 (051) 121 (096)Mn gkg O-layer Limed 094 (06) 212 (13) 184 (119)

Mn2+ micromolcg 0ndash5 cm Control 092 (143) 105 (146) 139 (131)Mn2+ micromolcg 0ndash5 cm Limed 17 (116) 366 (315) 48 (327)Mn2+ micromolcg 5ndash10 cm Control 209 (304) 153 (131) 148 (147)Mn2+ micromolcg 5ndash10 cm Limed 233 (177) 233 (171) 236 (195)Mn2+ micromolcg 10ndash30 cm Control 112 (138) 273 (182) 209 (214)Mn2+ micromolcg 10ndash30 cm Limed 19 (116) 264 (141) 212 (147)Mn2+ micromolcg 30ndash60 cm Control 085 (101) 214 (078) 126 (077)Mn2+ micromolcg 30ndash60 cm Limed 117 (098) 221 (129) 157 (151)

Na gkg O-layer Control 01 (002) 016 (003) 014 (007)Na gkg O-layer Limed 01 (003) 016 (004) 015 (014)

Na+ micromolcg 0ndash5 cm Control 024 (005) 082 (047) 106 (042)Na+ micromolcg 0ndash5 cm Limed 031 (021) 068 (027) 126 (059)Na+ micromolcg 5ndash10 cm Control 027 (01) 07 (033) 08 (034)Na+ micromolcg 5ndash10 cm Limed 021 (007) 062 (026) 09 (038)Na+ micromolcg 10ndash30 cm Control 019 (018) 048 (027) 051 (022)Na+ micromolcg 10ndash30 cm Limed 017 (008) 045 (028) 065 (032)Na+ micromolcg 30ndash60 cm Control 031 (017) 045 (023) 049 (021)Na+ micromolcg 30ndash60 cm Limed 02 (016) 06 (045) 057 (064)Ntot gkg O-layer Control 1526 (314) 1577 (183) 1391 (243)Ntot gkg O-layer Limed 118 (386) 1208 (327) 1205 (233)Ntot gkg 0ndash5 cm Control 202 (136) 212 (108) 252 (144)Ntot gkg 0ndash5 cm Limed 177 (051) 279 (1) 327 (151)

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 23: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 23 of 33

Table A1 Cont

Parameter Unit Depth Treatment 2003 2010 2015

Ntot gkg 5ndash10 cm Control 11 (064) 112 (049) 126 (056)Ntot gkg 5ndash10 cm Limed 113 (042) 13 (041) 162 (064)Ntot gkg 10ndash30 cm Control 061 (037) 07 (031) 069 (033)Ntot gkg 10ndash30 cm Limed 081 (036) 077 (024) 085 (03)Ntot gkg 30ndash60 cm Control 034 (024) 043 (021) 041 (019)Ntot gkg 30ndash60 cm Limed 05 (032) 045 (02) 049 (022)

pH-KCl O-layer Control 263 (054) 282 (034) 309 (077)pH-KCl O-layer Limed 301 (046) 556 (046) 43 (07)pH-KCl 0ndash5 cm Control 289 (013) 297 (014) 294 (062)pH-KCl 0ndash5 cm Limed 29 (019) 372 (098) 373 (107)pH-KCl 5ndash10 cm Control 311 (033) 325 (027) 317 (032)pH-KCl 5ndash10 cm Limed 318 (023) 347 (032) 36 (072)pH-KCl 10ndash30 cm Control 347 (035) 362 (034) 366 (026)pH-KCl 10ndash30 cm Limed 369 (017) 383 (022) 378 (02)pH-KCl 30ndash60 cm Control 378 (028) 394 (025) 392 (018)pH-KCl 30ndash60 cm Limed 384 (028) 396 (023) 397 (019)

Table A2 G2 study site historic development of pH-KCl Mg K Na Fe Mn H C and N in 2003-2015given are group means with standard deviations Marked boldmdashsignificant differences between currentand previous sampling campaign underlinemdashlimed plots significantly different from control

Parameter Unit Depth Treatment 2003 2010 2015

CN O-layer Control 2553 (456) 254 (353) 2415 (378)CN O-layer Limed 2612 (317) 2363 (278) 2369 (36)CN 0ndash5 cm Control 1886 (368) 1916 (449) 1748 (175)CN 0ndash5 cm Limed 1812 (137) 1782 (202) 1773 (185)CN 5ndash10 cm Control 179 (397) 1782 (597) 168 (185)CN 5ndash10 cm Limed 1786 (173) 1723 (17) 1729 (191)CN 10ndash30 cm Control 1552 (204) 1463 (334) 1411 (154)CN 10ndash30 cm Limed 1496 (256) 1486 (198) 1462 (221)CN 30ndash60 cm Control 1076 (126) 947 (273) 998 (21)CN 30ndash60 cm Limed 1118 (154) 107 (278) 1047 (316)Ctot gkg O-layer Control 40222 (5168) 36585 (8695) 33514 (7908)Ctot gkg O-layer Limed 36533 (1588) 30449 (8466) 29165 (6161)Ctot gkg 0ndash5 cm Control 4442 (669) 4906 (2227) 5797 (2958)Ctot gkg 0ndash5 cm Limed 6202 (1352) 3911 (1221) 5058 (1843)Ctot gkg 5ndash10 cm Control 2422 (333) 2415 (828) 2771 (924)Ctot gkg 5ndash10 cm Limed 2796 (664) 2502 (559) 2724 (995)Ctot gkg 10ndash30 cm Control 1394 (376) 1181 (393) 1373 (353)Ctot gkg 10ndash30 cm Limed 1316 (391) 1433 (538) 1384 (601)Ctot gkg 30ndash60 cm Control 498 (128) 498 (376) 595 (388)Ctot gkg 30ndash60 cm Limed 658 (508) 655 (473) 646 (569)Fe gkg O-layer Control 403 (226) 571 (398) 535 (326)Fe gkg O-layer Limed 493 (172) 744 (353) 749 (319)

Fe3+ micromolcg 0ndash5 cm Control 922 (63) 1322 (792) 837 (497)Fe3+ micromolcg 0ndash5 cm Limed 1537 (755) 964 (768) 356 (273)Fe3+ micromolcg 5ndash10 cm Control 381 (53) 37 (254) 246 (237)Fe3+ micromolcg 5ndash10 cm Limed 542 (482) 382 (271) 137 (115)Fe3+ micromolcg 10ndash30 cm Control 045 (043) 061 (036) 03 (02)Fe3+ micromolcg 10ndash30 cm Limed 044 (049) 107 (078) 03 (026)Fe3+ micromolcg 30ndash60 cm Control 005 (003) 035 (016) 008 (003)Fe3+ micromolcg 30ndash60 cm Limed 006 (006) 054 (046) 01 (009)H+ micromolcg 0ndash5 cm Control 1104 (725) 128 (847) 136 (963)H+ micromolcg 0ndash5 cm Limed 1826 (418) 58 (46) 489 (375)

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

1 Paces T Weathering rates of gneiss and depletion of exchangeable cations in soils under environmentalacidification J Geol Soc Lond 1986 143 673ndash677 [CrossRef]

2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
Page 24: Natural Recovery and Liming E ects in Acidified Forest ...

Soil Syst 2020 4 38 24 of 33

Table A2 Cont

Parameter Unit Depth Treatment 2003 2010 2015

H+ micromolcg 5ndash10 cm Control 484 (328) 323 (201) 46 (447)H+ micromolcg 5ndash10 cm Limed 699 (375) 284 (148) 294 (166)H+ micromolcg 10ndash30 cm Control 193 (097) 085 (052) 116 (068)H+ micromolcg 10ndash30 cm Limed 2 (097) 112 (054) 13 (067)H+ micromolcg 30ndash60 cm Control 134 (083) 096 (078) 067 (053)H+ micromolcg 30ndash60 cm Limed 153 (071) 108 (053) 112 (072)K gkg O-layer Control 141 (102) 159 (08) 124 (046)K gkg O-layer Limed 169 (067) 204 (088) 161 (072)

K+ micromolcg 0ndash5 cm Control 08 (018) 112 (073) 146 (117)K+ micromolcg 0ndash5 cm Limed 1 (043) 1 (034) 122 (066)K+ micromolcg 5ndash10 cm Control 07 (031) 071 (022) 084 (02)K+ micromolcg 5ndash10 cm Limed 071 (031) 09 (032) 085 (034)K+ micromolcg 10ndash30 cm Control 064 (023) 078 (024) 078 (026)K+ micromolcg 10ndash30 cm Limed 078 (041) 098 (041) 089 (034)K+ micromolcg 30ndash60 cm Control 102 (029) 116 (031) 097 (031)K+ micromolcg 30ndash60 cm Limed 11 (061) 143 (058) 113 (043)Mn gkg O-layer Control 085 (081) 108 (079) 101 (094)Mn gkg O-layer Limed 135 (112) 225 (132) 228 (13)

Mn2+ micromolcg 0ndash5 cm Control 293 (213) 35 (361) 328 (275)Mn2+ micromolcg 0ndash5 cm Limed 357 (349) 427 (346) 53 (416)Mn2+ micromolcg 5ndash10 cm Control 452 (341) 65 (453) 419 (422)Mn2+ micromolcg 5ndash10 cm Limed 404 (204) 544 (303) 461 (339)Mn2+ micromolcg 10ndash30 cm Control 37 (241) 468 (325) 316 (224)Mn2+ micromolcg 10ndash30 cm Limed 347 (138) 488 (306) 383 (271)Mn2+ micromolcg 30ndash60 cm Control 2 (144) 314 (243) 241 (192)Mn2+ micromolcg 30ndash60 cm Limed 178 (105) 371 (216) 245 (169)

Na gkg O-layer Control 01 (006) 013 (005) 013 (005)Na gkg O-layer Limed 01 (006) 018 (005) 013 (005)

Na+ micromolcg 0ndash5 cm Control 043 (022) 083 (057) 111 (029)Na+ micromolcg 0ndash5 cm Limed 041 (016) 072 (024) 104 (04)Na+ micromolcg 5ndash10 cm Control 043 (034) 068 (034) 086 (036)Na+ micromolcg 5ndash10 cm Limed 036 (021) 057 (021) 08 (032)Na+ micromolcg 10ndash30 cm Control 031 (014) 033 (018) 048 (015)Na+ micromolcg 10ndash30 cm Limed 024 (008) 044 (024) 056 (026)Na+ micromolcg 30ndash60 cm Control 04 (01) 046 (027) 037 (013)Na+ micromolcg 30ndash60 cm Limed 02 (012) 044 (028) 043 (02)Ntot gkg O-layer Control 1598 (238) 1453 (327) 1388 (277)Ntot gkg O-layer Limed 1409 (11) 1292 (35) 1247 (273)Ntot gkg 0ndash5 cm Control 238 (022) 257 (114) 328 (152)Ntot gkg 0ndash5 cm Limed 346 (091) 219 (062) 289 (111)Ntot gkg 5ndash10 cm Control 137 (014) 137 (035) 165 (053)Ntot gkg 5ndash10 cm Limed 157 (037) 145 (03) 158 (059)Ntot gkg 10ndash30 cm Control 09 (024) 083 (028) 098 (027)Ntot gkg 10ndash30 cm Limed 089 (023) 095 (03) 094 (035)Ntot gkg 30ndash60 cm Control 046 (01) 05 (022) 056 (025)Ntot gkg 30ndash60 cm Limed 056 (036) 057 (029) 056 (032)

pH-KCl O-layer Control 277 (043) 296 (039) 297 (062)pH-KCl O-layer Limed 306 (064) 453 (079) 437 (079)pH-KCl 0ndash5 cm Control 295 (029) 31 (022) 309 (032)pH-KCl 0ndash5 cm Limed 283 (011) 342 (039) 354 (066)pH-KCl 5ndash10 cm Control 329 (031) 353 (018) 342 (029)pH-KCl 5ndash10 cm Limed 318 (028) 359 (015) 362 (022)pH-KCl 10ndash30 cm Control 368 (018) 387 (014) 38 (016)pH-KCl 10ndash30 cm Limed 363 (017) 379 (014) 38 (015)pH-KCl 30ndash60 cm Control 374 (023) 38 (018) 388 (019)pH-KCl 30ndash60 cm Limed 363 (019) 376 (014) 38 (019)

Soil Syst 2020 4 38 25 of 33

Table A3 G1 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003-2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus188 188 minus397ndash074CN O-layer 2003ndash2010 Limed 029 328 minus361ndash523CN O-layer 2010ndash2015 Control minus019 177 minus296ndash17CN O-layer 2010ndash2015 Limed 289 384 004ndash908CN 0ndash5 cm 2003ndash2010 Control 022 225 minus19ndash392CN 0ndash5 cm 2003ndash2010 Limed minus059 152 minus318ndash08CN 0ndash5 cm 2010ndash2015 Control 045 424 minus228ndash79CN 0ndash5 cm 2010ndash2015 Limed minus137 263 minus489ndash21CN 5ndash10 cm 2003ndash2010 Control minus008 243 minus225ndash335CN 5ndash10 cm 2003ndash2010 Limed 159 206 minus035ndash425CN 5ndash10 cm 2010ndash2015 Control minus001 374 minus463ndash545CN 5ndash10 cm 2010ndash2015 Limed minus095 187 minus313ndash185CN 10ndash30 cm 2003ndash2010 Control minus25 415 minus88ndash07CN 10ndash30 cm 2003ndash2010 Limed 165 209 minus198ndash307CN 10ndash30 cm 2010ndash2015 Control 039 204 minus192ndash281CN 10ndash30 cm 2010ndash2015 Limed minus094 26 minus354ndash272CN 30ndash60 cm 2003ndash2010 Control minus43 668 minus1457ndash26CN 30ndash60 cm 2003ndash2010 Limed 241 418 minus29ndash732CN 30ndash60 cm 2010ndash2015 Control minus007 308 minus351ndash46CN 30ndash60 cm 2010ndash2015 Limed minus168 23 minus43ndash12Ctot gkg O-layer 2003ndash2010 Control 0 026 minus024ndash038Ctot gkg O-layer 2003ndash2010 Limed 028 081 minus036ndash152Ctot gkg O-layer 2010ndash2015 Control minus012 009 minus022ndashminus001Ctot gkg O-layer 2010ndash2015 Limed 012 03 minus025ndash058Ctot gkg 0ndash5 cm 2003ndash2010 Control 031 046 minus033ndash097Ctot gkg 0ndash5 cm 2003ndash2010 Limed 061 051 01ndash135Ctot gkg 0ndash5 cm 2010ndash2015 Control 028 052 minus022ndash111Ctot gkg 0ndash5 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 5ndash10 cm 2003ndash2010 Control 019 036 minus022ndash064Ctot gkg 5ndash10 cm 2003ndash2010 Limed 028 023 001ndash064Ctot gkg 5ndash10 cm 2010ndash2015 Control 024 064 minus027ndash133Ctot gkg 5ndash10 cm 2010ndash2015 Limed 019 023 minus003ndash054Ctot gkg 10ndash30 cm 2003ndash2010 Control 017 04 minus028ndash08Ctot gkg 10ndash30 cm 2003ndash2010 Limed 011 026 minus023ndash034Ctot gkg 10ndash30 cm 2010ndash2015 Control minus001 022 minus021ndash03Ctot gkg 10ndash30 cm 2010ndash2015 Limed 007 037 minus033ndash067Ctot gkg 30ndash60 cm 2003ndash2010 Control 028 043 minus013ndash097Ctot gkg 30ndash60 cm 2003ndash2010 Limed 023 064 minus027ndash134Ctot gkg 30ndash60 cm 2010ndash2015 Control minus008 027 minus046ndash024Ctot gkg 30ndash60 cm 2010ndash2015 Limed 006 04 minus034ndash063Fe gkg O-layer 2003ndash2010 Control 053 085 minus02ndash181Fe gkg O-layer 2003ndash2010 Limed 017 067 minus066ndash084Fe gkg O-layer 2010ndash2015 Control 039 065 minus006ndash15Fe gkg O-layer 2010ndash2015 Limed minus02 028 minus039ndash029

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 079 092 minus001ndash192Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus026 052 minus088ndash03Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control 038 184 minus06ndash367Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus044 06 minus087ndash059Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 406 422 minus018ndash936Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 147 236 minus036ndash551Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 039 minus061ndash033Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus049 061 minus085ndash058Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 571 1038 minus034ndash2398Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 166 151 minus001ndash393

Soil Syst 2020 4 38 26 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus042 013 minus052ndashminus026Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus041 059 minus091ndash059Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 2111 2742 minus026ndash6757Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1786 1304 153ndash3778Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus066 028 minus095ndashminus026Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus056 049 minus093ndash028H+ micromolcg 0ndash5 cm 2003ndash2010 Control 054 061 minus005ndash144H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus064 035 minus1ndashminus013H+ micromolcg 0ndash5 cm 2010ndash2015 Control 007 033 minus039ndash051H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 61 1451 minus09ndash3204H+ micromolcg 5ndash10 cm 2003ndash2010 Control 023 058 minus04ndash105H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus015 055 minus062ndash08H+ micromolcg 5ndash10 cm 2010ndash2015 Control 034 068 minus026ndash15H+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus005 079 minus075ndash114H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus028 063 minus093ndash038H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus027 05 minus075ndash049H+ micromolcg 10ndash30 cm 2010ndash2015 Control 241 363 minus042ndash815H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 124 263 minus035ndash591H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus05 04 minus096ndashminus005H+ micromolcg 30ndash60 cm 2003ndash2010 Limed 116 369 minus073ndash775H+ micromolcg 30ndash60 cm 2010ndash2015 Control 276 544 minus037ndash124H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 057 068 minus05ndash107K gkg O-layer 2003ndash2010 Control 022 038 minus01ndash086K gkg O-layer 2003ndash2010 Limed 013 023 minus008ndash048K gkg O-layer 2010ndash2015 Control 007 021 minus016ndash034K gkg O-layer 2010ndash2015 Limed minus004 024 minus025ndash034

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 015 066 minus04ndash118K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 069 098 minus019ndash195K+ micromolcg 0ndash5 cm 2010ndash2015 Control 046 034 minus002ndash082K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 0 025 minus036ndash029K+ micromolcg 5ndash10 cm 2003ndash2010 Control 007 039 minus031ndash068K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 027 045 minus015ndash089K+ micromolcg 5ndash10 cm 2010ndash2015 Control 026 044 minus012ndash102K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus003 023 minus024ndash034K+ micromolcg 10ndash30 cm 2003ndash2010 Control 039 069 minus033ndash11K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 01 041 minus034ndash077K+ micromolcg 10ndash30 cm 2010ndash2015 Control 01 027 minus017ndash045K+ micromolcg 10ndash30 cm 2010ndash2015 Limed 004 014 minus02ndash015K+ micromolcg 30ndash60 cm 2003ndash2010 Control 053 095 minus038ndash157K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 025 053 minus033ndash093K+ micromolcg 30ndash60 cm 2010ndash2015 Control 008 024 minus027ndash032K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus012 016 minus02ndash016Mn gkg O-layer 2003ndash2010 Control 05 103 minus02ndash226Mn gkg O-layer 2003ndash2010 Limed 125 056 041ndash185Mn gkg O-layer 2010ndash2015 Control 062 056 minus001ndash145Mn gkg O-layer 2010ndash2015 Limed 001 056 minus037ndash1

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 156 181 minus021ndash442Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 13 184 minus061ndash432Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 757 1579 minus056ndash3576Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 279 569 minus021ndash1295Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 619 918 minus064ndash2046Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 046 083 minus056ndash118Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control 115 301 minus052ndash652Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed 084 181 minus064ndash398Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 4957 1060 minus015ndash23918

Soil Syst 2020 4 38 27 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 054 031 014ndash087Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus029 047 minus06ndash055Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 051 minus051ndash079Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 607 87 minus017ndash2137Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 179 173 036ndash392Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus044 015 minus055ndashminus022Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus013 046 minus068ndash042

Na gkg O-layer 2003ndash2010 Control 068 056 027ndash165Na gkg O-layer 2003ndash2010 Limed 065 054 minus006ndash133Na gkg O-layer 2010ndash2015 Control minus016 031 minus055ndash017Na gkg O-layer 2010ndash2015 Limed minus005 068 minus066ndash078

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 242 145 1ndash435Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 293 418 minus006ndash1004Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 052 09 minus008ndash209Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 086 046 021ndash121Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 166 055 11ndash25Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 258 24 042ndash653Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 025 048 minus031ndash097Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 052 049 minus003ndash121Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 339 33 minus005ndash756Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 271 408 041ndash995Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 014 042 minus027ndash072Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 094 177 minus021ndash408Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 129 246 minus038ndash564Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 427 505 003ndash1248Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 024 063 minus033ndash124Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 002 061 minus042ndash108Ntot gkg O-layer 2003ndash2010 Control 007 024 minus016ndash034Ntot gkg O-layer 2003ndash2010 Limed 018 062 minus033ndash103Ntot gkg O-layer 2010ndash2015 Control minus012 007 minus023ndashminus007Ntot gkg O-layer 2010ndash2015 Limed 003 021 minus025ndash028Ntot gkg 0ndash5 cm 2003ndash2010 Control 027 044 minus029ndash089Ntot gkg 0ndash5 cm 2003ndash2010 Limed 065 053 011ndash123Ntot gkg 0ndash5 cm 2010ndash2015 Control 026 033 minus014ndash06Ntot gkg 0ndash5 cm 2010ndash2015 Limed 016 031 minus01ndash066Ntot gkg 5ndash10 cm 2003ndash2010 Control 017 038 minus014ndash08Ntot gkg 5ndash10 cm 2003ndash2010 Limed 017 02 minus005ndash035Ntot gkg 5ndash10 cm 2010ndash2015 Control 022 044 minus021ndash095Ntot gkg 5ndash10 cm 2010ndash2015 Limed 024 025 minus003ndash062Ntot gkg 10ndash30 cm 2003ndash2010 Control 035 071 minus011ndash161Ntot gkg 10ndash30 cm 2003ndash2010 Limed 0 018 minus029ndash016Ntot gkg 10ndash30 cm 2010ndash2015 Control minus001 016 minus012ndash025Ntot gkg 10ndash30 cm 2010ndash2015 Limed 009 022 minus02ndash039Ntot gkg 30ndash60 cm 2003ndash2010 Control 076 127 minus006ndash289Ntot gkg 30ndash60 cm 2003ndash2010 Limed minus001 027 minus039ndash031Ntot gkg 30ndash60 cm 2010ndash2015 Control minus005 012 minus018ndash013Ntot gkg 30ndash60 cm 2010ndash2015 Limed 013 023 minus013ndash045

pH-KCl O-layer 2003ndash2010 Control 003 025 minus031ndash031pH-KCl O-layer 2003ndash2010 Limed 246 053 154ndash285pH-KCl O-layer 2010ndash2015 Control 029 022 008ndash065pH-KCl O-layer 2010ndash2015 Limed minus109 059 minus167ndashminus011pH-KCl 0ndash5 cm 2003ndash2010 Control 008 013 minus015ndash019pH-KCl 0ndash5 cm 2003ndash2010 Limed 111 073 057ndash225pH-KCl 0ndash5 cm 2010ndash2015 Control minus001 016 minus018ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed minus01 074 minus106ndash099pH-KCl 5ndash10 cm 2003ndash2010 Control 009 013 minus013ndash022

Soil Syst 2020 4 38 28 of 33

Table A3 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

pH-KCl 5ndash10 cm 2003ndash2010 Limed 028 024 minus006ndash059pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 016 minus034ndash006pH-KCl 5ndash10 cm 2010ndash2015 Limed 017 04 minus032ndash065pH-KCl 10ndash30 cm 2003ndash2010 Control 016 013 minus001ndash029pH-KCl 10ndash30 cm 2003ndash2010 Limed 015 011 minus001ndash025pH-KCl 10ndash30 cm 2010ndash2015 Control minus004 017 minus023ndash019pH-KCl 10ndash30 cm 2010ndash2015 Limed minus007 017 minus034ndash01pH-KCl 30ndash60 cm 2003ndash2010 Control 015 02 minus002ndash049pH-KCl 30ndash60 cm 2003ndash2010 Limed 007 017 minus022ndash024pH-KCl 30ndash60 cm 2010ndash2015 Control minus007 02 minus03ndash014pH-KCl 30ndash60 cm 2010ndash2015 Limed minus001 009 minus007ndash015

Table A4 G2 study site parameter pH-KCl Mg K Na Fe Mn H C and N response ratios (RR) totime in 2003ndash2015

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

CN O-layer 2003ndash2010 Control minus013 153 minus204ndash186CN O-layer 2003ndash2010 Limed minus25 354 minus71ndash202CN O-layer 2010ndash2015 Control minus125 102 minus244ndash034CN O-layer 2010ndash2015 Limed 007 17 minus251ndash22CN 0ndash5 cm 2003ndash2010 Control 03 163 minus103ndash298CN 0ndash5 cm 2003ndash2010 Limed minus03 224 minus27ndash338CN 0ndash5 cm 2010ndash2015 Control minus168 339 minus688ndash245CN 0ndash5 cm 2010ndash2015 Limed minus009 199 minus311ndash232CN 5ndash10 cm 2003ndash2010 Control minus008 121 minus105ndash185CN 5ndash10 cm 2003ndash2010 Limed minus063 228 minus367ndash193CN 5ndash10 cm 2010ndash2015 Control minus102 292 minus569ndash23CN 5ndash10 cm 2010ndash2015 Limed 006 18 minus162ndash278CN 10ndash30 cm 2003ndash2010 Control minus089 191 minus328ndash188CN 10ndash30 cm 2003ndash2010 Limed minus01 212 minus298ndash197CN 10ndash30 cm 2010ndash2015 Control minus053 185 minus368ndash113CN 10ndash30 cm 2010ndash2015 Limed minus024 054 minus091ndash048CN 30ndash60 cm 2003ndash2010 Control minus129 297 minus517ndash178CN 30ndash60 cm 2003ndash2010 Limed minus048 164 minus29ndash097CN 30ndash60 cm 2010ndash2015 Control 051 155 minus133ndash217CN 30ndash60 cm 2010ndash2015 Limed minus023 112 minus209ndash082Ctot gkg O-layer 2003ndash2010 Control minus01 011 minus028ndash0Ctot gkg O-layer 2003ndash2010 Limed minus016 025 minus042ndash021Ctot gkg O-layer 2010ndash2015 Control minus004 028 minus033ndash041Ctot gkg O-layer 2010ndash2015 Limed minus001 02 minus025ndash029Ctot gkg 0ndash5 cm 2003ndash2010 Control 011 027 minus019ndash047Ctot gkg 0ndash5 cm 2003ndash2010 Limed minus034 024 minus071ndashminus004Ctot gkg 0ndash5 cm 2010ndash2015 Control 03 066 minus021ndash142Ctot gkg 0ndash5 cm 2010ndash2015 Limed 031 02 minus001ndash05Ctot gkg 5ndash10 cm 2003ndash2010 Control 0 015 minus018ndash024Ctot gkg 5ndash10 cm 2003ndash2010 Limed minus004 034 minus041ndash044Ctot gkg 5ndash10 cm 2010ndash2015 Control 02 037 minus018ndash074Ctot gkg 5ndash10 cm 2010ndash2015 Limed 008 017 minus008ndash034Ctot gkg 10ndash30 cm 2003ndash2010 Control minus012 027 minus042ndash019Ctot gkg 10ndash30 cm 2003ndash2010 Limed 013 04 minus024ndash076Ctot gkg 10ndash30 cm 2010ndash2015 Control 02 024 minus005ndash06Ctot gkg 10ndash30 cm 2010ndash2015 Limed 0 025 minus035ndash026Ctot gkg 30ndash60 cm 2003ndash2010 Control minus001 039 minus054ndash054Ctot gkg 30ndash60 cm 2003ndash2010 Limed 0 027 minus039ndash029Ctot gkg 30ndash60 cm 2010ndash2015 Control 031 049 minus007ndash116Ctot gkg 30ndash60 cm 2010ndash2015 Limed 003 024 minus036ndash02

Soil Syst 2020 4 38 29 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Fe gkg O-layer 2003ndash2010 Control 037 025 007ndash064Fe gkg O-layer 2003ndash2010 Limed 073 103 minus059ndash204Fe gkg O-layer 2010ndash2015 Control 02 062 minus054ndash106Fe gkg O-layer 2010ndash2015 Limed 017 052 minus032ndash1

Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Control 088 149 minus023ndash349Fe3+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus036 033 minus092ndashminus011Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Control minus018 056 minus061ndash078Fe3+ micromolcg 0ndash5 cm 2010ndash2015 Limed minus05 03 minus072ndash001Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 389 minus064ndash905Fe3+ micromolcg 5ndash10 cm 2003ndash2010 Limed 116 259 minus077ndash49Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Control minus001 097 minus087ndash153Fe3+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus062 016 minus082ndashminus045Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Control 543 777 minus038ndash163Fe3+ micromolcg 10ndash30 cm 2003ndash2010 Limed 531 767 019ndash187Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Control minus038 046 minus08ndash038Fe3+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus067 021 minus086ndashminus033Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Control 869 522 155ndash156Fe3+ micromolcg 30ndash60 cm 2003ndash2010 Limed 1246 1142 306ndash3127Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Control minus073 012 minus091ndashminus061Fe3+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus076 013 minus093ndashminus061H+ micromolcg 0ndash5 cm 2003ndash2010 Control 031 046 minus017ndash105H+ micromolcg 0ndash5 cm 2003ndash2010 Limed minus065 026 minus094ndashminus036H+ micromolcg 0ndash5 cm 2010ndash2015 Control 024 062 minus034ndash123H+ micromolcg 0ndash5 cm 2010ndash2015 Limed 033 095 minus044ndash162H+ micromolcg 5ndash10 cm 2003ndash2010 Control minus01 055 minus054ndash085H+ micromolcg 5ndash10 cm 2003ndash2010 Limed minus045 04 minus083ndash01H+ micromolcg 5ndash10 cm 2010ndash2015 Control 044 072 minus033ndash154H+ micromolcg 5ndash10 cm 2010ndash2015 Limed 006 02 minus009ndash041H+ micromolcg 10ndash30 cm 2003ndash2010 Control minus051 023 minus072ndashminus026H+ micromolcg 10ndash30 cm 2003ndash2010 Limed minus04 014 minus055ndashminus019H+ micromolcg 10ndash30 cm 2010ndash2015 Control 048 034 minus006ndash077H+ micromolcg 10ndash30 cm 2010ndash2015 Limed 022 043 minus039ndash071H+ micromolcg 30ndash60 cm 2003ndash2010 Control minus027 038 minus062ndash037H+ micromolcg 30ndash60 cm 2003ndash2010 Limed minus024 037 minus06ndash035H+ micromolcg 30ndash60 cm 2010ndash2015 Control minus001 057 minus087ndash053H+ micromolcg 30ndash60 cm 2010ndash2015 Limed 009 06 minus047ndash096K gkg O-layer 2003ndash2010 Control 022 021 minus006ndash047K gkg O-layer 2003ndash2010 Limed 019 025 minus025ndash037K gkg O-layer 2010ndash2015 Control minus015 02 minus044ndash012K gkg O-layer 2010ndash2015 Limed minus016 019 minus032ndash016

K+ micromolcg 0ndash5 cm 2003ndash2010 Control 048 055 minus041ndash109K+ micromolcg 0ndash5 cm 2003ndash2010 Limed 004 021 minus016ndash037K+ micromolcg 0ndash5 cm 2010ndash2015 Control 033 048 minus018ndash108K+ micromolcg 0ndash5 cm 2010ndash2015 Limed 029 063 minus021ndash128K+ micromolcg 5ndash10 cm 2003ndash2010 Control 015 05 minus032ndash092K+ micromolcg 5ndash10 cm 2003ndash2010 Limed 033 021 01ndash053K+ micromolcg 5ndash10 cm 2010ndash2015 Control 022 027 minus004ndash067K+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus004 028 minus04ndash024K+ micromolcg 10ndash30 cm 2003ndash2010 Control 027 026 minus001ndash068K+ micromolcg 10ndash30 cm 2003ndash2010 Limed 035 031 011ndash085K+ micromolcg 10ndash30 cm 2010ndash2015 Control 001 009 minus011ndash013K+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus005 013 minus025ndash006K+ micromolcg 30ndash60 cm 2003ndash2010 Control 018 022 minus011ndash038K+ micromolcg 30ndash60 cm 2003ndash2010 Limed 039 044 minus001ndash111K+ micromolcg 30ndash60 cm 2010ndash2015 Control minus017 013 minus034ndashminus001K+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus015 018 minus046ndashminus002

Soil Syst 2020 4 38 30 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Mn gkg O-layer 2003ndash2010 Control 099 136 006ndash325Mn gkg O-layer 2003ndash2010 Limed 2 379 minus02ndash875Mn gkg O-layer 2010ndash2015 Control minus001 033 minus035ndash038Mn gkg O-layer 2010ndash2015 Limed 006 032 minus033ndash041

Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Control 259 564 minus056ndash1262Mn2+ micromolcg 0ndash5 cm 2003ndash2010 Limed 339 78 minus054ndash1732Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Control 014 078 minus043ndash149Mn2+ micromolcg 0ndash5 cm 2010ndash2015 Limed 037 038 minus016ndash077Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Control 207 477 minus04ndash1059Mn2+ micromolcg 5ndash10 cm 2003ndash2010 Limed 053 06 minus051ndash094Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Control minus035 006 minus043ndashminus028Mn2+ micromolcg 5ndash10 cm 2010ndash2015 Limed minus016 023 minus047ndash013Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Control 073 17 minus058ndash367Mn2+ micromolcg 10ndash30 cm 2003ndash2010 Limed 048 079 minus03ndash171Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Control minus028 025 minus047ndash015Mn2+ micromolcg 10ndash30 cm 2010ndash2015 Limed minus023 022 minus05ndash011Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Control 102 149 minus052ndash339Mn2+ micromolcg 30ndash60 cm 2003ndash2010 Limed 197 255 minus03ndash617Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Control minus012 049 minus056ndash072Mn2+ micromolcg 30ndash60 cm 2010ndash2015 Limed minus038 018 minus068ndashminus018

Na gkg O-layer 2003ndash2010 Control 271 562 minus044ndash1269Na gkg O-layer 2003ndash2010 Limed 114 092 minus038ndash208Na gkg O-layer 2010ndash2015 Control 006 031 minus041ndash035Na gkg O-layer 2010ndash2015 Limed minus018 035 minus059ndash033

Na+ micromolcg 0ndash5 cm 2003ndash2010 Control 302 585 minus012ndash1345Na+ micromolcg 0ndash5 cm 2003ndash2010 Limed 113 127 minus026ndash294Na+ micromolcg 0ndash5 cm 2010ndash2015 Control 059 073 minus031ndash156Na+ micromolcg 0ndash5 cm 2010ndash2015 Limed 054 05 002ndash123Na+ micromolcg 5ndash10 cm 2003ndash2010 Control 222 363 minus03ndash851Na+ micromolcg 5ndash10 cm 2003ndash2010 Limed 125 162 minus038ndash354Na+ micromolcg 5ndash10 cm 2010ndash2015 Control 041 061 minus024ndash118Na+ micromolcg 5ndash10 cm 2010ndash2015 Limed 051 052 minus005ndash118Na+ micromolcg 10ndash30 cm 2003ndash2010 Control 034 104 minus044ndash21Na+ micromolcg 10ndash30 cm 2003ndash2010 Limed 113 147 008ndash324Na+ micromolcg 10ndash30 cm 2010ndash2015 Control 088 137 minus004ndash33Na+ micromolcg 10ndash30 cm 2010ndash2015 Limed 054 099 minus049ndash212Na+ micromolcg 30ndash60 cm 2003ndash2010 Control 015 041 minus032ndash07Na+ micromolcg 30ndash60 cm 2003ndash2010 Limed 211 237 minus038ndash57Na+ micromolcg 30ndash60 cm 2010ndash2015 Control 0 067 minus055ndash114Na+ micromolcg 30ndash60 cm 2010ndash2015 Limed 021 073 minus048ndash131Ntot gkg O-layer 2003ndash2010 Control minus009 015 minus033ndash005Ntot gkg O-layer 2003ndash2010 Limed minus009 019 minus025ndash022Ntot gkg O-layer 2010ndash2015 Control 0 027 minus027ndash046Ntot gkg O-layer 2010ndash2015 Limed minus001 014 minus016ndash018Ntot gkg 0ndash5 cm 2003ndash2010 Control 008 024 minus016ndash041Ntot gkg 0ndash5 cm 2003ndash2010 Limed minus032 026 minus069ndash001Ntot gkg 0ndash5 cm 2010ndash2015 Control 034 044 minus014ndash102Ntot gkg 0ndash5 cm 2010ndash2015 Limed 032 026 003ndash069Ntot gkg 5ndash10 cm 2003ndash2010 Control 0 012 minus013ndash019Ntot gkg 5ndash10 cm 2003ndash2010 Limed minus002 032 minus038ndash033Ntot gkg 5ndash10 cm 2010ndash2015 Control 024 028 minus017ndash05Ntot gkg 5ndash10 cm 2010ndash2015 Limed 009 023 minus022ndash034Ntot gkg 10ndash30 cm 2003ndash2010 Control minus007 024 minus031ndash02Ntot gkg 10ndash30 cm 2003ndash2010 Limed 01 033 minus023ndash064Ntot gkg 10ndash30 cm 2010ndash2015 Control 023 02 minus002ndash049

Soil Syst 2020 4 38 31 of 33

Table A4 Cont

Parameter Unit Depth Period Treatment RR Mean RR SD RR Range

Ntot gkg 10ndash30 cm 2010ndash2015 Limed 002 026 minus034ndash032Ntot gkg 30ndash60 cm 2003ndash2010 Control 01 033 minus018ndash061Ntot gkg 30ndash60 cm 2003ndash2010 Limed 004 015 minus014ndash019Ntot gkg 30ndash60 cm 2010ndash2015 Control 014 028 minus011ndash058Ntot gkg 30ndash60 cm 2010ndash2015 Limed minus001 015 minus024ndash018

pH-KCl O-layer 2003ndash2010 Control 016 02 minus001ndash05pH-KCl O-layer 2003ndash2010 Limed 179 076 068ndash278pH-KCl O-layer 2010ndash2015 Control minus003 021 minus03ndash026pH-KCl O-layer 2010ndash2015 Limed minus032 078 minus111ndash084pH-KCl 0ndash5 cm 2003ndash2010 Control 011 014 minus006ndash024pH-KCl 0ndash5 cm 2003ndash2010 Limed 065 036 029ndash12pH-KCl 0ndash5 cm 2010ndash2015 Control minus004 015 minus022ndash017pH-KCl 0ndash5 cm 2010ndash2015 Limed 007 023 minus019ndash027pH-KCl 5ndash10 cm 2003ndash2010 Control 015 023 minus013ndash048pH-KCl 5ndash10 cm 2003ndash2010 Limed 035 029 004ndash067pH-KCl 5ndash10 cm 2010ndash2015 Control minus008 017 minus027ndash016pH-KCl 5ndash10 cm 2010ndash2015 Limed 003 004 minus003ndash007pH-KCl 10ndash30 cm 2003ndash2010 Control 018 014 minus002ndash031pH-KCl 10ndash30 cm 2003ndash2010 Limed 014 007 007ndash024pH-KCl 10ndash30 cm 2010ndash2015 Control minus007 01 minus017ndash006pH-KCl 10ndash30 cm 2010ndash2015 Limed 001 006 minus007ndash008pH-KCl 30ndash60 cm 2003ndash2010 Control 004 015 minus01ndash026pH-KCl 30ndash60 cm 2003ndash2010 Limed 012 014 minus008ndash027pH-KCl 30ndash60 cm 2010ndash2015 Control 007 017 minus008ndash035pH-KCl 30ndash60 cm 2010ndash2015 Limed 005 009 minus008ndash016

References

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2 Berger TW Tuumlrtscher S Berger P Lindebner L A slight recovery of soils from Acid Rain over the lastthree decades is not reflected in the macro nutrition of beech (Fagus sylvatica) at 97 forest stands of the ViennaWoods Environ Pollut 2016 216 624ndash635 [CrossRef] [PubMed]

3 Majdi H Viebke C-G Effects of fertilization with dolomite lime+ PK or wood ash on root distribution andmorphology in a Norway spruce stand in Southwest Sweden For Sci 2004 50 802ndash809 [CrossRef]

4 Cudlin P Kieliszewska-Rokicka B Rudawska M Grebenc T Alberton O Lehto T Bakker MRBoslashrja I Konocircpka B Leski T et al Fine roots and ectomycorrhizas as indicators of environmental changePlant Biosyst 2007 141 406ndash425 [CrossRef]

5 Wellbrock N Eickenscheidt N Gruumlneberg E Boumlgelein R Environmental settings and their changesin the last decades In Status and Dynamics of Forests in Germany Results of the National Forest MonitoringWellbrock N Bolte A Eds Springer Nature Cham Switzerland 2019 Volume 237 pp 29ndash54 [CrossRef]

6 Homan C Beier C McCay T Lawrence G Application of lime (CaCO3) to promote forest recoveryfrom severe acidification increases potential for earthworm invasion For Ecol Manag 2016 368 39ndash44[CrossRef]

7 Rizvi SH Gauquelin T Gers C Gueacuterold F Pagnout C Baldy V Calciumndashmagnesium liming ofacidified forested catchments Effects on humus morphology and functioning Appl Soil Ecol 2012 6281ndash87 [CrossRef]

8 Ulrich B Soil acidity and its relations to acid deposition In Effects of Accumulation of Air Pollutants in ForestEcosystems Ulrich B Pankrath J Eds Springer Dordrecht The Netherlands 1983 pp 127ndash146 [CrossRef]

9 Heisner U Wilpert K Hildebrand EE Vergleich aktueller Messungen zum Aziditaumltsstatussuumldwestdeutscher Waldboumlden mit historischen Messungen von 1927 Allg Forst Und Jagdztg 2003174 41ndash44

Soil Syst 2020 4 38 32 of 33

10 Draacutepelovaacute I Kulhavyacute J Comparison of soil and seepage water properties in the limed and not-limedspruce forest stands in the Beskydy Mts Beskydy 2012 5 55ndash64 [CrossRef]

11 Pavlu L Drabek O Stejskalova S Tejnecky V Hradilova M Nikodem A Boruvka L Distribution ofaluminium fractions in acid forest soils Influence of vegetation changes iForest 2018 11 721ndash727 [CrossRef]

12 Meesenburg H Riek W Ahrends B Eickenscheidt N Gruumlneberg E Evers J Fortmann H Koumlnig NLauer A Meiwes KJ et al Soil acidification in German forest soils In Status and Dynamics of Forests inGermany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer Nature ChamSwitzerland 2019 Volume 237 pp 93ndash121 [CrossRef]

13 Court M van der Heijden G Didier S Nys C Richter C Pousse N Saint-Andreacute L Legout ALong-term effects of forest liming on mineral soil organic layer and foliage chemistry Insights from multiplebeech experimental sites in Northern France For Ecol Manag 2018 409 872ndash889 [CrossRef]

14 UNECE Convention on Long-range Transboundary Air Pollution (CLRTAP) United Nations EconomicCommission for Europe Geneva Switzerland 1979

15 Jonard M Fuumlrst A Verstraeten A Thimonier A Timmermann V Potocic N Waldner P Benham SHansen K Merilauml P et al Tree mineral nutrition is deteriorating in Europe Glob Chang Biol 2015 21418ndash430 [CrossRef]

16 Li Y Cui S Chang SX Zhang Q Liming effects on soil pH and crop yield depend on lime material typeapplication method and rate and crop species A global meta-analysis J Soils Sediments 2018 19 1393ndash1406[CrossRef]

17 Reid C Watmough SA Evaluating the effects of liming and wood-ash treatment on forest ecosystemsthrough systematic meta-analysis Can J For Res 2014 44 867ndash885 [CrossRef]

18 Saarsalmi A Tamminen P Kukkola M Levula T Effects of liming on chemical properties of soil needlenutrients and growth of Scots pine transplants For Ecol Manag 2011 278ndash285 [CrossRef]

19 Šraacutemek V Fadrhonsovaacute V Vortelovaacute L Lomskyacute B Development of chemical soil properties in thewestern Ore Mts (Czech Republic) 10 years after liming J For Sci 2012 58 57ndash66 [CrossRef]

20 Ouimet R Moore J-D Effects of fertilization and liming on tree growth vitality and nutrient status inboreal balsam fir stands For Ecol Manag 2015 345 39ndash49 [CrossRef]

21 Fleck S Eickenscheidt N Ahrends B Evers J Gruumlneberg E Ziche D Houmlhle J Schmitz A Weis WSchmidt-Walter P et al Nitrogen status and dynamics in German forest soils In Status and Dynamics ofForests in Germany Results of the National Forest Monitoring Wellbrock N Bolte A Eds Springer NatureCham Switzerland 2019 Volume 237 pp 123ndash166 [CrossRef]

22 Littek T Zum Stand der Praxis-Duumlngeversuche in Baden-Wuumlrttemberg In Versuche zur Minderung derWalderkrankung Littek T Adam K Eds Mitteilungen der Forstlichen Versuchs- und ForschungsanstaltBaden-Wuumlrttemberg Freiburg Germany 1985 Volume 119 pp 1ndash25

23 Wilpert K Hildebrand EE Huth T Ergebnisse des Praxis-Groszligduumlngeversuches Abschluszligbericht uumlber dieAnfangsaufnahmen (198586) und die Endaufnahmen (198990) Mitteilungen der Forstlichen Versuchs- undForschungsanstalt Baden-Wuumlrttemberg Freiburg Germany 1993 Volume 171

24 FAO Guidelines for Soil Description 4th ed Food and Agriculture Organization of the United Nations RomeItaly 2006 pp 25ndash29

25 Ad-hoc-Arbeitsgruppe Boden Bodenkundliche Kartieranleitung 5th ed Bundesanstalt fuumlr Geowissenschaftenund Rohstoffe in Zusammenarbeit mit den Staatlichen Geologischen Diensten Hannover Germany 2005pp 303ndash310

26 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk des Gutachterausschuss Forstliche Analytik (GAFA)Federal Ministry of Food Agriculture and Consumer Protection Northwest German Forest Research InstituteBonn Germany 2005

27 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash4 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2008

28 GAFA (Ed) Handbuch Forstliche Analytik (HFA) Grundwerk und 1ndash5 Ergaumlnzung des GutachterausschussForstliche Analytik (GAFA) Federal Ministry of Food Agriculture and Consumer Protection NorthwestGerman Forest Research Institute Bonn Germany 2014

29 Hedges LV Gurevitch J Curtis PS The meta-analysis of response ratios in experimental ecology Ecology1999 80 1150ndash1156 [CrossRef]

Soil Syst 2020 4 38 33 of 33

30 Schoumlpp W Posch M Mylona S Johannsson M Long-term development of acid deposition (1880-2030) insensitive freschwater regions in Europe Hydrol Earth Syst Sci 2003 7 436ndash446 [CrossRef]

31 Kretzschmar R Chemische Eigenschaften und Prozesse In SchefferSchachtschabel Lehrbuch der Bodenkunde17th ed Amelung W Blume H-P Fleige H Horn R Kandeler E Koumlgel-Knabner I Kretzschmar RStahr K Wilke B-M Eds Springer Spektrum Berlin Germany 2018 pp 151ndash211 [CrossRef]

32 Pabian SE Rummel SM Sharpe WE Brittingham MC Terrestrial liming as a restoration technique foracidified forest ecosystems Int J For Res 2012 2012 1ndash10 [CrossRef]

33 Huber C Baier R Goumlttlein A Weis W Changes in soil seepage water and needle chemistry between 1984and 2004 after liming an N-saturated Norway spruce stand at the Houmlglwald Germany For Ecol Manag2006 233 11ndash20 [CrossRef]

34 Guckland A Ahrends B Paar U Dammann I Evers J Meiwes KJ Schoumlnfelder E Ullrich TMindrup M Koumlnig N et al Predicting depth translocation of base cations after forest liming Results fromlong-term experiments Eur J For Res 2012 131 1869ndash1887 [CrossRef]

35 Loumlfgren S Cory N Zetterberg T Larsson PE Kronnaumls V The long-term effects of catchment liming andreduced sulphur deposition on forest soils and runoff chemistry in southwest Sweden For Ecol Manag2009 258 567ndash578 [CrossRef]

36 Cools N Vesterdal L de Vos B Vanguelova E Hansen K Tree species is the major factor explaining CNratios in European forest soils For Ecol Manag 2014 311 3ndash16 [CrossRef]

copy 2020 by the authors Licensee MDPI Basel Switzerland This article is an open accessarticle distributed under the terms and conditions of the Creative Commons Attribution(CC BY) license (httpcreativecommonsorglicensesby40)

  • Introduction
  • Materials and Methods
    • Site Description
    • Soil Sampling and Laboratory Methods
    • Statistical Analysis
      • Results
        • Liming Effects in 2003
        • Soil Acidity Status Development between 2003 and 2015
          • pH Values
          • Base Saturation
          • Cation Exchange Capacities
            • O-layer Stocks Carbon and Nitrogen
              • Discussion
                • Discussion on Methods and Boundary Conditions of the Study
                • Natural Recovery of Acidified Soils
                • Effects of Liming
                  • Conclusions
                  • References
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