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This article appeared in a journal published by Elsevier. The attachedcopy is furnished to the author for internal non-commercial researchand education use, including for instruction at the authors institution
and sharing with colleagues.
Other uses, including reproduction and distribution, or selling orlicensing copies, or posting to personal, institutional or third party
websites are prohibited.
In most cases authors are permitted to post their version of thearticle (e.g. in Word or Tex form) to their personal website orinstitutional repository. Authors requiring further information
regarding Elsevier’s archiving and manuscript policies areencouraged to visit:
Impact of Santiago de Chile urban atmospheric pollution on anthropogenic traceelements enrichment in snow precipitation at Cerro Colorado, Central Andes
F. Cereceda-Balic a, M.R. Palomo-Marín b, E. Bernalte b, V. Vidal a, J. Christie a, X. Fadic a, J.L. Guevara a,1,C. Miro c, E. Pinilla Gil b,*aCentro de Tecnologías Ambientales, Universidad Técnica Federico Santa María, Av. de España, Valparaíso, ChilebDepartamento de Química Analítica, Facultad de Ciencias, Universidad de Extremadura, Av. de Elvas, s/n. 06006 Badajoz, SpaincDepartamento de Física Aplicada, Universidad de Extremadura, Campus Universitario, Cáceres, Spain
Winter snow precipitation in the Central Andes mountain range reflects urban atmospheric emissions of Santiago de Chile by significantenrichment of anthropogenic elements. The preliminary results obtained in this study are promising for assignment and tracking of pollutionsources by exploiting chemical information collected in the snow.
a r t i c l e i n f o
Article history:Received 5 July 2011Received in revised form2 November 2011Accepted 16 November 2011
Keywords:Trace elementsAtmospheric pollutionSnowSantiago de ChileCentral Andes
a b s t r a c t
Seasonal snow precipitation in the Andes mountain range is evaluated as an environmental indicator ofthe composition of atmospheric emissions in Santiago de Chile metropolitan area, by measuring a set ofrepresentative trace elements in snow samples by ICP-MS. Three late winter sampling campaigns (2003,2008 and 2009) were conducted in three sampling areas around Cerro Colorado, a Central Andesmountain range sector NE of Santiago (36 km). Nevados de Chillán, a sector in The Andes located about500 km south from the metropolitan area, was selected as a reference area. The experimental results atCerro Colorado and Nevados de Chillán were compared with previously published data of fresh snowfrom remote and urban background sites. High snow concentrations of a range of anthropogenic markerelements were found at Cerro Colorado, probably derived from Santiago urban aerosol transport anddeposition combined with the effect of mining and smelting activities in the area, whereas Nevados deChillán levels roughly correspond to urban background areas. Enhanced concentrations in surface snowrespect to deeper samples are discussed. Significant differences found between the 2003, 2008 and 2009anthropogenic source markers profiles at Cerro Colorado sampling points were correlated with changesin emission sources at the city. The preliminary results obtained in this study, the first of this kind in thesouthern hemisphere, show promising use of snow precipitation in the Central Andes as a suitablematrix for receptor model studies aimed at identifying and quantifying pollution sources in Santiagode Chile.
� 2011 Elsevier Ltd. All rights reserved.
1. Introduction
Trace elemental profiles are key data sets for the assessment ofpotential aerosol toxicity and also for pollution sources identificationand quantification (Watson et al., 2002; Viana et al., 2008, andreferences therein). Urban aerosol elemental profiles are usuallyevaluated on aerosol samples obtained at particular city locations orclosely around, but these samples can be potentially affected byanalytical noise due to rapid temporal changes of pollution sources,and also by the intrinsic heterogeneity of the urban areas. In contrast,remote sampling may provide clearer information, aside of data
aboutmedium and long range transportation of atmospheric aerosol(Walker et al., 2003; Caritat et al., 2005).
Snow is considered to be an ideal matrix to observe depositionfrom the atmosphere. Atmospheric deposition events can be easilyand cheaply sampled inwell defined increments. Compared to othersedimentary records, atmospheric particulates in snow are dilutedby pure water rather than other earth materials so the compositionof atmospheric deposition may be unambiguously measured downto very low concentrations. Snowflakes accumulate more pollutantsfrom the atmosphere than raindrops because of their larger surfacearea and slower fall velocity (Telmer et al., 2004).
A number of studies have dealt with the use of snow as envi-ronmental receptor of trace elements, for the identification andquantification of precipitation sources at remote locations. Local,regional and long range transports have been identified in the French
1 Present address: Departamento de Biología y Química, Facultad de CienciasBásicas, Universidad Católica del Maule. Avenida San Miguel, 3605. Talca, Chile.
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Alps (Veysseyre et al., 2001), north eastern European Russia (Walkeret al., 2003), rural locations around a smelter in Quebec (Telmer et al.,2004), Mt. Everest at Central Himalayas (Kang et al., 2007; Lee et al.,2008); Italian Dolomites (Gabrielli et al., 2008), or the Pyrenees(Veschambre, 2006; Bacardit and Camarero, 2010). Less informationis found in the literature about the use of trace elements in snow asa matrix for the investigation of short range urban pollution.Anthropogenic enrichment of heavy metals in snow samples aroundLulea, Sweden, has been described (Viklander, 1998,1999). The samegroup has studied the differences among snow samples obtained atdifferent cities in Sweden (Reinosdotter and Viklander, 2005). Glennand Sansalone (2002), measured the Cu, Zn, Pb and Cd levels in snowsamples taken from urban background areas around Cincinnati, OH,USA. Engelhard et al. (2007) studied the impact of urban pollution onthe composition of seasonal snow at Innsbruck, Austria. No studiesabout snow as environmental receptor of trace elements at locationsin the southern hemisphere are reported in the literature.
Santiago de Chile (pop. almost 6 million), is located in a rela-tively flat valley at an altitude of 500 m. The Andes mountain rangeis located close to the east, with hills up to 4500 m. A smallercoastal mountain range is located in the west, with hills up to2000 m. Due to its subtropical latitude; the vertical exchange of airduring most of the year is controlled by permanent subsidence andthe formation of a thermal inversion layer, caused by the South
Pacific sub-tropical anticyclone (Morata et al., 2008). This results ina semiarid climate with temperatures ranging between �2 and35 �C (average values around 14 �C) and an average rainfall of350 mm per year with large interannual variability (Ruthlant andGarreaud, 1995). The thermal inversion subsidence layer lies atabout 400 m above the ground during the winter and the autumnand at 1000 m during the spring and the summer. During thesethermal inversion periods, the vertical ventilation is highlyrestricted and air pollution increases with potential effects on thenearby mountains. The urban area of Santiago is showing a rapidgrowth, concentrating most of the new services, housing andindustries as compared to the rest of the country (Romero et al.,1999), thus reinforcing the magnitude of this pollution problem.Intense episodes of air pollution are frequent from April to August(Ruthlant and Garreaud, 1995), with significant impact on partic-ulate matter and anthropogenic element contents in the city(Romo-Kröger, 1990; Gramsch et al., 2006; Sax et al., 2007; Morataet al., 2008). Particlemass concentration (PM10) 24-h averages near300 mgm�3 are frequent in the western part of Santiago (Pudahuel,Cerrillos). Some isolated events of 500 mgm�3 or more occurseveral times during winter (Jorquera et al., 1998; Perez et al., 2000;Artaxo et al., 1999). Some active copper mines and smelters arepresent in the proximity of Santiago, including the world classEl Teniente Mine and the associated Caletones smelter. SO2 and
Fig. 1. Map of Central Chile showing the Cerro Colorado (CC) sampling area close to Santiago de Chile and the Nevados de Chillán (NCH) reference sampling area.
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other gaseous pollutants concentrations have increased from 2004to 2009 due to the operation of additional coal fired power plants incentral Chile as a result of the expansion of the copper industrywith a corresponding increase of energy demand.
No reference has been found about the impact of Santiago deChile atmospheric emissions on seasonal snow precipitation at theclose Andes heights, so we have conducted a preliminary study toevaluate this impact by measuring the levels of selected anthro-pogenic elements in the snow. Aside to the evaluation of potentialusefulness of snow precipitation at Central Andes as a suitablematrix for receptor model studies (aimed to identify and quantifypollution sources in Santiago de Chile), this study can also serve asa starting point to estimate the potential impact of snow pollutantson receiving water bodies as the winter snow deposits begin tomelt, especially in case of rain-on-snow events, causing rapidreleasing of pollutants from snow piles. This is the first study of thistype in the southern hemisphere.
2. Materials and methods
2.1. Sampling sites
Snow sampling was conducted in the Cerro Colorado area (33�
200 S, 70� 170 W) and in the Nevados de Chillán area (36� 540 S, 71�
240 W), as depicted in Fig. 1. Cerro Colorado is 36 km NE of Santiagode Chile downtown, so it is considered to be at a suitable distancerange to test the influence of the urban atmosphere on theprecipitated snow, especially because of the prevailing SWwinds inthe area (Morata et al., 2008). Nevados de Chillán, selected asa reference area, is a relatively undisturbed sector of The Andesrange, 500 km south of Santiago de Chile. The most significanthuman agglomeration in the area is the city of Chillán (162,000inhabitants, 60 km NW of the sampling area). Both Cerro Coloradoand Nevados de Chillán are affected by sporting activities based onnearby skiing facilities and scarce urbanization. The samples werecollected from October 1 to 15 (2003, 2008 and 2009, singlecampaigns each year), after the major winter snowfall had occurredand before the snowpack had started to melt. Three samplingpoints were selected at Cerro Colorado, along a transect line from3000 to 3050 m.a.s.l. (Fig. 2a). Five sampling points were selected atNevados de Chillán (Fig. 2b) along the Diguillín Valley from twoaltitudes: 1570 (two points) and 1740 (three points) m.a.s.l. Fieldduplicates were collected at each sampling point.
2.2. Sampling procedure
The purity of snow makes it more prone to contamination andtherefore special handling protocols are required (Veysseyre et al.,2001). Sampling materials were previously acid cleaned and thenrinsed with ultra pure water obtained by coupling a reverseosmosis system (Wasserlab, Spain) with a four-column ionexchange system Milli-Q equipped with a 0.2 mm filter (Millipore,Bedford, MA). The HNO3 used were subboiled at a quartz distiller(Kürner, Germany). Samples were collected from a 1 square meterhand-dug shallow snow pit by operators wearing polyethylenegloves, using acid-cleaned plastic shovels. Approximately 2 kg ofsurface snow was then collected from the first 5 cm of snow, andthen 2 kg of deep snow was collected under 5 cm deep. Thesamples were immediately transferred to cleaned polyethylenebags (Ziploc), sealed and kept frozen at �20 �C until analysis.Appropriate precautions were taken to avoid contamination asfollows: Powderless polyethylene gloves were always used, and thetools were well cleaned between each use by rinsing with snowfrom the subsequent sample site. At each site, samplingwas done inundisturbed snow which was approached by walking into the
wind. The sampling sites were selected so that they were as far aspossible from local contamination sources such as ski trails, cablecar stations, trees or exposed rocks.
2.3. Analytical procedure
The samples were melted at room temperature under hoodextraction and acidified with subboiled nitric acid to make 5%solutions. A complete set of trace elements was determined byICP-MS using a PerkinElmer ELAN 9000 instrument placed in a cleanroom. Analytical determinationswere carried out in triplicate on rawaqueous sampleswithout any preconcentration or pretreatment stepto minimize contamination. Some elements were under the instru-ment detection limit and other gave no relevant environmentalinformation, so As, Pb, Cd, Ni, V, Cr, Mn, Co, Ba, Cu, Zn, Mo and Sbwere selected for discussion after screening the data base for rele-vant results. These elements are classified in the literature as tracersof diverse anthropogenic activities (Viana et al., 2008 and referencestherein). The precision ranged from 10 to 20% depending on theelements and the concentration levels. Detection limits were calcu-lated according to the IUPAC definition as three times the standard
Fig. 2. Map showing the location of the sampling sites Cerro Colorado (a) and Nevadosde Chillán (b).
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deviation of concentrations estimated after ten repetitive measure-ment of the blank solution (5%HNO3 in ultrapurewater) are reportedin Table 1. The obtained values were low enough for measuring theexpected concentrations in the real samples. A certified referencematerial (SPS-SW2 “Reference material for measurements ofelements in surface waters”, Spectrapure Standards, Oslo, Norway)was used for quality control of the data. A good agreement betweenmeasured and certified values was observed for most elementsassayed (Table 1). Enrichment of elements in the real snow sampleswere calculated as mean element concentration at location 1/meanelement concentration at location 2.
3. Results and discussion
3.1. General overview and comparison with reference areas
Trace element concentrations measured in the surface snow atthe sampling locations Cerro Colorado (CC) and Nevados de Chillán(NCH) are given in Table 2, aside with literature data about previ-ously reported values of trace elements in fresh snow from locationsthat can be considered relatively remote in their regional context(Pyrenees, Alps, and Alaska). For each area, the quoted values are themedian values and the range (minimum and maximum) of thewhole set of samples obtained during the sampling campaigns. Mostanthropogenic elemental concentrations measured at CerroColorado are higher than corresponding literature values. The
differences were especially significant in the cases of As, Pb, Cd, Mn,Co, Ba, Cu, Zn and Mo, whereas Ni and V concentrations were onlyslightly higher. Cr and Sb concentrations in Cerro Colorado snowsamples were similar or lower than previously reported values inregional background areas. These results are in support of a signifi-cant impact of emission sources from Santiago de Chile in the area,but the data can also reflect the impact of miningesmelting activi-ties. The proximity of copper strip mining operations at Los Bronces(40 km NWof the Cerro Colorado sampling area) is probably relatedwith the high Cu values observed. The giant El Teniente (mine) eCaletones (smelter) copper complex (95 km SW), can be also relatedwith enhanced levels of some elements in the snow of Cerro Colo-rado as a result of particulate matter transport. Elevated levels of Cu,Zn and Asweremeasured by Romo-Kröger et al. (1994) in particulatematter around El Teniente e Caletones. Snow samples taken atNevados de Chillán presented similar concentration ranges foranthropogenic elements than literature values for most elements,except for somewhat elevated values of Pb, Cd, Cu, and Mo.WhereasNevados de Chillán has been selected as a regional reference in ourstudy, the experimental data shown that a significant degree ofanthropogenic impact is detected in the area. This can be due tonearby sporting activities, but transport from regional sources can beimplied, including emissions from Chillán (60 km NW) and Con-cepción (130 kmW). Also, altered composition of particulate matterin the regional scale, due to geological abnormalities and surfacecoverage mobilization by weathering and mining activities is typicalin Chile, and also the regional dispersion of smelting particulateemissions (Kavouras et al., 2001; De Gregori et al., 2002; Gidhagenet al., 2002). The regional air dynamics configuration contributes tothis phenomenon, with SWairmasses traveling from the coast to thehigh slope, west face mountainsides in The Andes.
Anthropogenic elements concentrations at Cerro Colorado andNevados de Chillán samples were then compared with previouslyreported values for Cu, Zn, Pb and Cd levels in snow sampled fromurban background areas around Cincinnati, OH, USA (Glenn andSansalone, 2002), Lulea and Sundsvall in Sweden (Reinosdotterand Viklander, 2005), and Innsbruck in Austria (Engelhard et al.,2007). The results are summarized in Table 3. The most notablefeature is probably the very high Cu levels measured at CerroColorado snow samples, with maximum values exceeding oneorder of magnitude Nevados de Chillán values and previouslypublished urban background data. Cu levels at Nevados de Chillánsamples were similar to those reported in the literature. Znconcentrations in snow samples from Cerro Colorado are in the
Table 2Element concentration rangesmeasured values in Cerro Colorado (CC) and Nevados de Chillán (NCH) and comparisonwith literature values about trace elements in fresh snowfrom regional background locations. Concentrations are given in median values and range in brackets. All data in mg kg�1.
Element CC NCH Atlantic pyreneesa Central pyreneesb Chamonix alpsc Eastern alpsd NW Alaskae
a Veschambre (2006).b Bacardit and Camarero (2010).c Veysseyre et al. (2001).d Gabrielli et al. (2008).e Douglas and Sturm (2004).
Table 1Limits of detection (LOD) calculated from 3s of 10 replicates of blank solution andanalytical results of certified reference material SPS-SW2 “Reference material formeasurements of elements in surface waters”. All data in mg kg�1.
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range of previously published values in the urban reference areas ofCincinnati and Sundsvall, but lower than reference values fromLulea and Innsbruck. Zn levels in Nevados de Chillán samples gavevalues within the lower end range of Cincinnati and Sundsvallvalues. Concentration values for Cd at Cerro Colorado were lowerthan those found by Engelhard et al. (2007) in background areas ofInnsbruck, but higher than the values reported at Cincinnati byGlenn and Sansalone (2002). These latter values were similar to ourCd results in the samples taken at Nevados de Chillán. Relativelyelevated values of Pb concentration were observed in CerroColorado snow samples with respect to previously reported valuesin Cincinnati and Sundsvall, but similar to variability ranges in Luleaand Innsbruck. Nevados de Chillán Pb values are similar to thosefound in urban reference areas of Sundsvall by Reinosdotter andViklander (2005). These results are in support of the previousconclusion about the impact of Santiago de Chile urban emissionson snow precipitation at Cerro Colorado, probably combined withthe effect of mining-smelting activities in the area.
3.2. Comparison between Cerro Colorado and Nevados de Chillán
A detailed study of anthropogenic elements concentration in thesnow samples was then conducted to evaluate the relative impact
of pollution sources around Santiago de Chile with respect to theregional reference area at Nevados de Chillán. A detailed view ofCerro Colorado vs Nevados de Chillán data sets is provided in Fig. 3,showing the significant differences observed for most elementsbetween the two sampling sites. Table 4 summarizes anthropo-genic sources that can be assigned to elements assayed in atmo-spheric deposition according to published literature: traffic (Querolet al., 2001), smelting (Alastuey et al., 2006), biomass and coalburning (Andersen et al., 2007) and waste incineration (Harrisonet al., 1996). It also reflects experimental mean values in theassayed snow samples and calculated concentration ratios (meanelement concentration at CC/mean element concentration at NCH).Higher mean concentrations of anthropogenic elements werefound in Cerro Colorado compared with the Nevados de Chillánreference area, with concentration ratios ranging from 2.2 (Cd) to108.1 (V). Average concentration ratios were calculated for groupsof elements linked to specific sources, with highest average ratiofound for traffic sources (30.4), followed by biomass and coalburning (17.0), smelting sources (16.8), and waste incineration(6.3). These preliminary results confirm the dominant impact ofurban traffic emission sources on the composition of the snowcollected at Cerro Colorado, with a significant contribution ofsmelting and burning activities.
3.3. Variability of the elements in the snowpack
2008 and 2009 sampling campaigns at Cerro Colorado includedcollection of surface and deep samples, as described in themethodssection. The snow samples were taken one month after the lastsnowing event, to inspect the degree of anthropogenic elementsenrichment due to dry deposition of atmospheric particulates onthe snow. The results are shown in Fig. 4, depicting the ratiobetween element concentrations in surface and deep snow. Cr wasunder the detection limit in deep samples, so the results for thiselement were excluded. These preliminary results shown a highvariability within the snowpack, with significant enrichment for allthe elements assayed in surface samples. A more detailed study
Fig. 3. Box and whisker plots showing the distribution of selected anthropogenic elements concentrations in the snow from sampling areas at Cerro Colorado (CC) and Nevados deChillán (NCH).
Table 3Comparison of literature values concentration level ranges of heavy metals in urbanbackground snow samples andmeasured values in Cerro Colorado (CC) and Nevadosde Chillán (NCH). All data in mg kg�1.
Sampling site Cu Zn Cd Pb Source
Cincinnati 2e10 5e35 0.2e0.35 0.5e10 Glenn and Sansalone,2002
Lulea 5e70 25e410 e 4e45 Reinosdotter andViklander, 2005
Sundsvall 1e10 5e70 e 8e17 Reinosdotter andViklander, 2005
Innsbruck 10e40 50e300 0.25e11.54 0.2e33 Engelhard et al., 2007CC 5e387 10e114 0.13e2.20 2.4e74.9 This workNCH 1e18 13e17 0.14e0.80 1.8e13.5 This work
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including sampling of individual snowing events would be neces-sary to fully characterize elements distribution in the snow duringthe winter season.
3.4. Temporal variability of the data at Cerro Colorado
Comparison of the concentration of anthropogenic elements inthe surface snow taken at Cerro Colorado during the 2003, 2008and 2009 sampling campaigns (Table 5) was conducted to inspectpossible correlations of seasonal snow compositionwith changes inthe urban atmosphere of Santiago de Chile. These are measured bya network of eight monitoring stations (Macam network) distrib-uted around the city and operated by the Ministry of Health, andtranslated to a set of air pollution indexes (Gramsch et al., 2006). Airpollution indexes related to particulate matter levels showeda steady decrease from 1997 to 2005, as a result of pollution controlstrategies developed after the Chilean “Environmental Base Law”
(Conama, 1994) and a specific plan for decontamination of Santiago(Conama, 1997). The decreasing trend of particulate matter indexeswas however reversed in the period 2005e2008 after the naturalgas supply shortage from Argentina caused significant changes inenergy consumption modes, with increased use of diesel, coal andbiomass burning in Chile (Comisión Nacional de Energía, 2011).Improved efforts directed to pollution control in Santiago de Chilemetropolitan area are currently in progress (PPDA, 2010). Ourresults for elemental concentrations in the snow presenta minimum in the year 2003 for As, Pb, Mo and Sb, while in 2008
the concentrations of As, Pb, Cd, V, Mn, Co, Cu, Mo and Sb weremaximum, probably reflecting the impact of significant changes inthe energy sources distribution at Santiago de Chile during thestudied period. Ni, Cr, Ba (no biomass or coal burning tracers) andZn showed a different trend with decreasing values from 2003 to2009. These preliminary results support the potential use of snowanalysis at Cerro Colorado for indicating changes in the urbanatmosphere of Santiago.
4. Conclusions
This work has demonstrated that anthropogenic trace elementlevels in snow precipitation at sampling locations in Cerro Colorado,Central Andes, about 40 km NE from the metropolitan area areaffected by urban atmospheric emissions from Santiago de Chile. Asimple methodological approach consisting in surface snowsampling and analysis by a standardized ICP-MS method (includingproper precautions to avoid sample contamination), provide infor-mation about spatial distribution and temporal evolution of theatmospheric precipitation at the selected sampling locations.
Significant enrichments for a variety of trace element markers,related to traffic, smelting and biomass burning were found inCerro Colorado, by comparison with relatively undisturbed loca-tions at Nevados de Chillán, 500 km S. Temporal evolution of traceelement levels at Cerro Colorado, between 2003 and 2009, werecorrelated with changes in Santiago de Chile urban atmosphericemissions in the same period.
Our preliminary results have shown that snow precipitation inthe Central Andes could be a suitable matrix for receptor modelstudies aimed at identifying and quantifying pollution sources atSantiago de Chile, as a simple and affordable methodology tocomplement the information of urban atmospheric surveillancenetworks.
Acknowledgements
This work was supported by Agencia Española de CooperaciónInternacional al Desarrollo (AECID), project D/031258/10. Addi-tional support from projects CONICYT: FONDEF D05-I-10054,FONDECYT 1070500; DGIP-USM N�13.09.57 and Junta de Extrem-adura (Spain) is also acknowledged.
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