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Evaluation of gamma activities of naturally occurring radioactive materials in uncontaminated surface soils of Jamaica Maurice Miller Mitko Voutchkov Received: 28 September 2013 Ó Akade ´miai Kiado ´, Budapest, Hungary 2014 Abstract In this study a geological, lithological or ped- ogenesis analysis is used to explain the values and distri- bution of the primordial specific gamma activities in the Jamaican soil environment. A random systematic sampling method resulted in Jamaica being divided into 50 square grids with a maximum sampling density of 225 square meters per sample. The resulting sixty-eight (68) samples were measured on a Canberra HPGe detector for 24 h and the photopeaks for the primordial gammas of 238 U, 232 Th and 40 K analyzed. Spearman’s correlation was used to investigate the relationships between the primordial spe- cific activities and the geological features of the soil samples collected and the geographic information system, ArcGIS v10.1 used to graphically depict the gamma profile of the primordials across the island. The Kruskal–Wallis test indicated that in general the variations of the primor- dial gamma specific activities over the underlying soil geologies were statistically significant. However, the pair- wise Post-Hoc test results did not suggest a significant variation in mean specific for any of the primordial with all the underlying geology even when the unadjusted p value was used. This result along with the Spearman’s coefficient correlation values suggested a moderate to weak relation- ship between the gamma profile of the top soil and its underlying geology. With the exception of a weak corre- lation with 232 Th (-0.295) no other primordial radionu- clide correlated with the UNESCO/FAO soil categories for the island. The most significant correlations for soil char- acteristics and gamma activities were organic matters which were positive for 232 Th (0.518), 238 U (0.481) but negative for 40 K(-0.284). Keywords Primordial radionuclides Soil Geology Introduction Objective of the research This research has two main objectives. The first is to investigate the hypothesis that the characteristics of the soil location in Jamaica impact the gamma signature of natu- rally occurring radioactive material (NORM) in uncon- taminated soils. The characteristic of the soil location was restricted to the following parameters; organic matter, bauxicity, pH, geology, elevation, latitude, and longitude. Areas where the soil environment may be affected by anthropogenic activities are excluded from this investiga- tion. The second objective is to establish a baseline data for primordial activities in Jamaica in order to quantify the impact of any nuclear accident worldwide, on the terrestrial environment; in this exercise the distribution of the pri- mordial will be characterized. This study assumed that the soil and its underlying geology are related. Review of related studies Numerous studies have been done all over the world on the analysis of primordial radionuclides in both contaminated and uncontaminated soils. The main purposes of these studies are usually (a) to determine the activity of these primordial sources and quantify the health/exposure radio- logical indices that indicate the levels of risk faced by the populations in these areas, (b) establish a baseline data for M. Miller (&) M. Voutchkov Department of Physics, Faculty of Science and Technology, University of the West Indies, Mona Campus, Kingston 6, Jamaica e-mail: [email protected] 123 J Radioanal Nucl Chem DOI 10.1007/s10967-014-3000-x
Transcript

Evaluation of gamma activities of naturally occurring radioactivematerials in uncontaminated surface soils of Jamaica

Maurice Miller • Mitko Voutchkov

Received: 28 September 2013

� Akademiai Kiado, Budapest, Hungary 2014

Abstract In this study a geological, lithological or ped-

ogenesis analysis is used to explain the values and distri-

bution of the primordial specific gamma activities in the

Jamaican soil environment. A random systematic sampling

method resulted in Jamaica being divided into 50 square

grids with a maximum sampling density of 225 square

meters per sample. The resulting sixty-eight (68) samples

were measured on a Canberra HPGe detector for 24 h and

the photopeaks for the primordial gammas of 238U, 232Th

and 40K analyzed. Spearman’s correlation was used to

investigate the relationships between the primordial spe-

cific activities and the geological features of the soil

samples collected and the geographic information system,

ArcGIS v10.1 used to graphically depict the gamma profile

of the primordials across the island. The Kruskal–Wallis

test indicated that in general the variations of the primor-

dial gamma specific activities over the underlying soil

geologies were statistically significant. However, the pair-

wise Post-Hoc test results did not suggest a significant

variation in mean specific for any of the primordial with all

the underlying geology even when the unadjusted p value

was used. This result along with the Spearman’s coefficient

correlation values suggested a moderate to weak relation-

ship between the gamma profile of the top soil and its

underlying geology. With the exception of a weak corre-

lation with 232Th (-0.295) no other primordial radionu-

clide correlated with the UNESCO/FAO soil categories for

the island. The most significant correlations for soil char-

acteristics and gamma activities were organic matters

which were positive for 232Th (0.518), 238U (0.481) but

negative for 40K (-0.284).

Keywords Primordial radionuclides � Soil � Geology

Introduction

Objective of the research

This research has two main objectives. The first is to

investigate the hypothesis that the characteristics of the soil

location in Jamaica impact the gamma signature of natu-

rally occurring radioactive material (NORM) in uncon-

taminated soils. The characteristic of the soil location was

restricted to the following parameters; organic matter,

bauxicity, pH, geology, elevation, latitude, and longitude.

Areas where the soil environment may be affected by

anthropogenic activities are excluded from this investiga-

tion. The second objective is to establish a baseline data for

primordial activities in Jamaica in order to quantify the

impact of any nuclear accident worldwide, on the terrestrial

environment; in this exercise the distribution of the pri-

mordial will be characterized. This study assumed that the

soil and its underlying geology are related.

Review of related studies

Numerous studies have been done all over the world on the

analysis of primordial radionuclides in both contaminated

and uncontaminated soils. The main purposes of these

studies are usually (a) to determine the activity of these

primordial sources and quantify the health/exposure radio-

logical indices that indicate the levels of risk faced by the

populations in these areas, (b) establish a baseline data for

M. Miller (&) � M. Voutchkov

Department of Physics, Faculty of Science and Technology,

University of the West Indies, Mona Campus, Kingston 6,

Jamaica

e-mail: [email protected]

123

J Radioanal Nucl Chem

DOI 10.1007/s10967-014-3000-x

the level of normal background radiation levels, (c) deter-

mine the variability of particular radionuclide concentration

across the area, (d) quantify the impact of industrial oper-

ations such as cement manufacturing, bauxite, and petro-

leum and electricity generation on the normally occurring

radioactivity materials in the environment, and (e) deter-

mine the levels of specific artificial radionuclides, espe-

cially those produced in nuclear reactors [1–16]. The

NORM of interest in soil varies between countries and

between radionuclides; in almost all cases examined the

activity of 40K outpaces by sometimes a factor of ten the

activities of 238U, 226Ra, and 232Th. The carcinogenic

impact of primordial radiation is of particular interest

worldwide and has been examined in a number of publi-

cations. The excess lifetime risks of cancer, and the annual

effective gamma doses in western Mazandaran Province of

Iran, were found higher than the global average when

gamma analysis of 54 soil samples were performed [1]. In

Nigeria, incidence of cancer from soil radioactivity found

that cancer cases attributable to radiation exposure due to

soil radioactivity was low, constituting between 1.3 and

9.2 % of the total reported cases [17]. In Kirklareli, Turkey,

the excess lifetime cancer risks and outdoor gamma dose

rates were determined from 230 sampling stations and soil

samples taken from 177 locations. The annual effective

gamma dose of Kirklareli was 144 [mu]Sv and the excess

lifetime cancer risk of 5.0 9 10-4 [18].

Geological and soil characterization of Jamaica

The island of Jamaica is located at coordinates 18�150N77�300W with an area of 10,911 square kilometers. The

geology of Jamaica may be classified by rock types

belonging to the groups Cretaceous, Wagwater and John

Crow Rift deposits, Limestone (yellow and white), Coastal

Groups and Alluvium as shown in Fig. 1. The yellow lime-

stone group in Jamaica overlay tectonically stable blocks

during the mid-Eocene period and along with the white

limestone, these Cenozoic limestone constitute 70 % of the

island and dominate the central regions of Jamaica [19]. This

central section of the island has a blanket of terra rossa and

bauxite covering the Cenozoic limestone and the large

majority of bauxite plants and productions occur here. The

soils in Jamaica have a wide range in classification mainly

due to the variability in the parent material, topography and

rainfall. These soils cover two major regions; a highland

interior and an almost flat coastal region in Jamaica. The red

limestone occurs mainly in St. Ann, Manchester and St.

Elizabeth and constitutes the bauxitic soils with red color due

to oxidation of iron. The black limestone, exposed over

yellow limestone rock, do not exhibit the red bauxite color

due to their high calcium and water component which

inhibits ferric oxidation.

The Alluvial Plain and Valley soils, deposited by rivers,

are mostly found on the southern and eastern end of the

island and in small areas in the central regions. They are

known to consist of loam, sand and gravel and gave rise to

good agricultural lands. The soil environment is described

by a 1984 study which developed 206 Jamaican soil names

which characterized the soils in Jamaica according to

features such as the texture, slope, root limiting layer,

internal drainage, moisture supplying capacity, erosion

hazard, and the levels of pH, potassium, phosphorus, and

nitrogen. The soil names were developed from the areas

where they were first found and is appended by the soil

texture; the same name was then applied anywhere else the

soil was found. Except for the St. Ann clay loam which

constitutes 5.3 % of the island, all the other soils are less

that 5 % in island wide distribution {Rural Physical Plan-

ning Department-Ministry of Agriculture, 1982 #2581}. A

more international naming convention of the soil environ-

ment in Jamaica is based on the United Nations Economic,

Scientific and Cultural Organization/Food and Agricultural

Organization (UNESCO/FAO) soil type published in the

World Harmonized Soil Database. The soils types in

Jamaica are listed as Ferralsols, Leptosols, Cambisols, and

Vertisols. The Jamaican soil has a Soil Mapping Unit ID of

17312. Other studies have been done examining terrestrial

gamma rays in the geological environment. Ramli et al.

[20] reported a valid statistical relationship between pre-

dicted terrestrial gamma dose rate based on geological

features and soil types in Kota Tinggi district, Malaysia. A

study in the Levos island of Greece using gamma-ray

scintillation spectrometry attempted to correlate radioac-

tive isotopes levels among various igneous rock types

formations exposed on the island. They noted high levels of40K, 232Th and 238U in several geological formations [21].

A study done in Jamaica resulted in a publication ‘‘A

Geochemical Atlas of Jamaica’’ detailing soils and heavy

metal analysis [22].

The soil metadata

The soil samples were distributed as follows: (a) underly-

ing geology—alluvium deposits (25.8 %), coastal group

(15.2 %), cretaceous (15.2 %),Wagwater (4.5 %), White

Limestone (36.4 %), and yellow limestone (3 %) (b) FAO

soil category—Canbisols (13.6 %), Ferralsols (66.7 %),

Leptosols (12.1 %), and Vertisols (7.6 %) (c) pH level—

acidic (15.2 %), alkaline (57.6 %), neutral (6.1 %), slightly

acidic (18.2 %), and unreported (3.0 %) (d) Soil texture—

clay (12.1 %), clay loam (10.6 %), gravelly loam (3 %),

gravelly sandy loam (3 %), loam (6.1 %), sand (3 %),

sandy loam (1.5 %), stony loam (59.1 %), and swamp

(1.5 %) (e) elevation levels—range 5–1,237 m with

50th percentile of 110 m (f) organic matter—range

J Radioanal Nucl Chem

123

2.65–28.30 % with 50th percentile of 11.8 %. The soil

environment is dominated by soils categorized by the FAO

as Ferralsols (66.7 %) with a dominant texture of stony

loam (59.1 %). These factors are analyzed further to see if

they impact the gamma profile of the terrestrial environ-

ment in Jamaica.

Materials and methods

Sample collection

The application of a random systematic sampling technique

resulted in Jamaica being divided into 50 square grids with

a maximum sampling density of 225 square meters per

sample. A location within the grid was selected using a

random generator which generated two numbers corre-

sponding to a location within the grid. At least one repre-

sentative soil sample (of minimum five sub-samples taken

from an area 20 9 20 m) was then collected from each

location resulting in a total of sixty-eight (68) soil samples.

The samples taken were restricted to the 0–10 cm section

of the soil after all living vegetation was removed. The

collected soils samples were sieved using a 2 mm sieve,

dried at 60 degrees for approximately 18 h and stored in a

sealed cylindrical container in a cool dark area for a min-

imum of thirty days prior to gamma measurement to ensure

secular equilibrium between 238U and its progenies.

Spectrometry

The detector used in this research was a Canberra 3825

HPGe detector (absolute efficiency = 27.61 %, measured

and 28.15 %, ISOCS value. This detector has an active area

of 38 cm2 and active diameter of 71 mm, [100] and was

cryogenically cooled by liquid nitrogen in a vertical dip-

stick type 7500SL 30 litre Dewar throughout the mea-

surement process. The detector and samples were enclosed

in a 950-kg Model 747E 10-cm thick lead shield with

graded 1 mm tin and 1.6 mm copper liner to reduce

interference from lead x-rays, cosmic and background

radiation during counting, reduce counting time and

improve the lower levels of detection. The floor of the

shield had a 12.1 cm hole to facilitate the cryostat and the

shield itself had a 9.5 mm thick low carbon steel. Soil and

background samples were counted in lead enclosure for

approximately 24 h using Genie 2000 software for spec-

trum acquisition. The entire detector and samples were

enclosed in a lead shield to reduce the background radia-

tion. Soil and background samples were counted in lead

enclosure for approximately 24 h using Genie 2000 soft-

ware for spectrum acquisition. The data for each sample

were entered into a Microsoft Excel spreadsheet for further

analysis. SPECTRW software was used for gamma ana-

lysis of the spectrum for each sample. For counting and

activity analysis the following photopeaks were used

(a) 40K, peak at 1,460.83 keV, (b) 235U, weighted average

of photopeak at 143.76 and 185.71 keV after correcting for

interference from 226Ra at 186.21 keV. (c) 238U, from the

weighted average of the daughters 214Pb (351.9 keV), 214Bi

(609.32 keV), and (d) 232Th, the weighted average of the

daughters 208Tl (583.19 keV), 228Ac (911.16), and 212Pb

(238.63 keV).

Minimum detection limits

Genie 2000 Nuclide MDA Report was run to generate the

minimum detectable activity for the radionuclides under

investigation in this study. This report was found to be

quite useful as it showed nuclides identified during the

nuclide identification process, the energy at which it was

found in the spectrum, nuclides that required/did not

required coincidence correction, and nuclides whose

energy were not found in the spectrum. The MDA (in

brackets in Bq/kg), for the radionuclides of interest were as

follows: 40K (6.24), 208Tl (0.889), 212Bi (7.20), 214Bi

(1.59), 214Pb (1.49), 226Ra (1.16), 234Pa (2.4), 234Th (5.8),

and 235U (0.706).

Nuclear analytical technique

A special gamma analytical method was used throughout

the research to ensure that the reported values were as

accurate as possible. This method involved the use of

several software applications including Canberra’s Lab-

SOCs and Genie 2000 for absolute efficiency measure-

ments and spectra counting respectively, SPECTRW

(courtesy of Costas Kalfas, Greece, for gamma analysis),

EFTRAN (courtesy of Tim Vidmar, Belgium, for cascade

summing correction), and Sigma Plot 10.0 (curve fitting

algorithm and generation of fitting parameters). In ana-

lyzing the photopeaks at 241 keV, the analysis program

used in this study firstly assigned the counts to both 224Ra

and 214Pb, since the corresponding peaks at 241.00 and

241.92 respectively cannot be separately resolved since as

it falls outside the resolution capability of the detector. The

observed peak is the sum of the two individual radionuc-

lides and is then apportioned by examining the activity of214Pb at 351 keV to determine the counts at 241 keV which

would give this activity. Since 214Pb has peaks (at

295 keV, BR = 18.5 %, and 351 keV with BR = 35.8 %),

an average activity can be assigned to this isotope based on

these intense peaks. A similar case, but a different

approach, was adopted for the 186 keV spectral line with

the unresolved composite of the 185.715 keV (235U) and

186.21 keV (226Ra).

J Radioanal Nucl Chem

123

Quality assurance

The method suggested by the equipment manufacturer

(Canberra) was adopted for Quality Assurance during the

counting process. Specific counting parameters were

monitored and documented following the analysis of the

radioactive source Model EU-NA-S installed in the Model

ISOXSRCE Check Source Fixture which ensured a con-

sistent geometry. This source contains 155Eu (86.5 and

105.3 keV), 22Na (511 and 1,275 keV); each nuclide has a

1 microcurie initial activity. On the front and side orien-

tation position, the source is located at 10 cm above and

beside the detector’s end-cap. Because it was deemed

impractical to move the detector from the lead shield each

time the QA measurements were being done, the 86.5 keV155Eu peak was discarded from the analysis due to possible

interference from lead X-rays at 87.15 keV. A counting

time of 5 min was employed to ensure a 1–2 % relative

precision in the 1,275 keV energy peak [23].

Other analytical technique

The soil type, pH, geographic information systems (GIS)

shapefiles, geological parameters, and the underlying geo-

logical formation related to the soil sampling locations in

Jamaica were obtained from both the Rural Physical Plan-

ning Division of the Ministry of Agriculture and Fisheries,

and the Department of Geology and Geography at the Uni-

versity of the West Indies in Jamaica. The GIS shapefiles

were analyzed using ArcGIS 10.1 state-of-the-art geo-

graphic information systems software to develop an under-

standing of the geographic distribution of the general soil

texture characteristics and the levels of calcium, potassium,

and nitrogen from which the samples originated. Additional

soil geological properties related to aluminum and pH were

obtained from the publication ‘‘A Geochemical Atlas of

Jamaica’’. The bauxiticy levels of the soils were inferred

from the levels of aluminum (Al) reported for the sample

locations. The adopted convention used was that soils with

less than 10 % concentration of aluminum are considered

non-bauxitic. The underlying geological formation was

provided by maps supplied by the Geology and Geography

Department of the University of the West Indies and the

1:250,000 geological map of Jamaica published by the Mines

and Geology Department of the Ministry of Energy and

Mining. Another useful source of information was the 1984

Comprehensive Resource Inventory and Evaluation System

Report that characterized the soil environment in Jamaica.

The geological related parameters of interest examined in

this research were the soil levels of potassium, phosphorus,

nitrogen, pH and bauxiticy. Sample point parameters col-

lected were the UNESCO/FAO soil type, elevation, latitude,

longitude, organic matter, soil texture and the underlying

geology. ArcMAP (a component of ArcGIS) was used to

overlay the various shapefiles and relate each sample point to

its geological characteristics. The Inverse Distance

Weighting interpolation technique was used to develop

various maps showing the distribution of the primordial ra-

dionuclides and gamma activity in Jamaica. The soil samples

were described by the following metadata (a) underlying

geology (b) FAO soil category (c) pH level (d) soil texture

(e) sample elevation levels, (f) organic matter (g) primordial

specific gamma activity, and (h) geographic location. A

number of statistical approaches,including the One-Sample

T-Tests, Kruskal–Wallis Test, Spearman’s Correlation,

Percentile Ranks, Box-and-Whisker plots, and parametric

and non-parametric Post-Hoc tests for variability of means

were used to analyze and report the data. For the Post-Hoc

analysis of the samples within the geologies for the specific

radionuclide, the adjusted p value was used as it gives a better

representation of the data set, incorporates all the processes

which contribute to the characteristics of the data, and is a

conservative method [24]. The statistical software SPSS

version 22.0 and GraphPad Prism version 6.00 for Windows

were used to perform the statistical analysis reported in this

paper.

Results and discussions

Minimizing uncertainty in the nuclear analytical

process

All analyzed samples were associated with an error from

which the mean activities were reported. The errors and

standard deviations in the mean specific activities of the

radionuclides in this study were detailed in the ‘‘Results

and discussion’’ section of this paper. The nuclear analysis

technique employed a dual efficiency curve for the cylin-

drical container in contact with the face of the Canberra

3825 HPGe detector; the expressions are shown in Eq. (1).

The resulting equations below (for the range before and

after 100 keV respectively) increased the accuracy of the

spectrometry results.

Equation (1)—Dual efficiency curve for the analytical

process.

ln Effð Þ ¼ �38:01 � þ22:38lnðE Þ � 4:642lnðEÞ2

þ 0:3185lnðEÞ3

¼ �110:8 � þ76:3lnðEÞ � 20:35lnðEÞ2

þ 2:56lnðEÞ3 � 0:15 ln Eð Þ4þ3:214 � 10�3lnðEÞ5

ð1Þ

Additional uncertainties were reduced by employing

coincidence correction to the photopeaks, interference

corrections (see ‘‘Nuclear analytical technique’’ section),

J Radioanal Nucl Chem

123

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J Radioanal Nucl Chem

123

the type of background shielding employed (see ‘‘Spec-

trometry’’ section), and the quality assurance employed

during the counting process (see ‘‘Quality assurance’’

section). Photopeaks below 100 keV were avoided to

eliminate interference from fluorescence x-rays in the

experimental setup, and reduce errors due to attenuation

and self-absorption of low energy gamma [25]. The 208Tl

photopeak at 510.7 keV was omitted from the weighted

activity for 232Th as it difficult to resolve from the 511 keV

annihilation peak. Errors due to disequilibrium in the post

radium nuclides of 238U, were reduced by keeping the

samples in a sealed container in a cool dark section of the

lab for a minimum of 30 days before counting. The door to

the lab was kept closed (as long as practical) to reduce

fluctuations in the background due to radon, and the entire

counting system was kept on a rubber mat to reduce

microphonics interference. Finally, the background used in

the peaked background correction process, was counted for

approximately three days.

Correlation data

The Spearman’s non-parametric statistic was used to

deduce the correlation among the variables investigated in

this report since the D’Agostino and Pearson Onibus

Normality tests indicated that with the exception of the

gamma total specific activity, all other variables were from

a non-Gaussian distribution. The correlation results are

shown in Table 1 and their implications are discussed in

the subsequent sections.

Potassium-40 distribution characteristics in Jamaica

Figure 2 showed that the distribution of potassium-40 (K-

40) in Jamaica ranged from 19.67 to 654.25 Bq/kg with the

eastern section of the island showing higher in comparison

to the mid central regions. The One-Sample T-Test results

[t(67) = -17.636, p \ 0.01] indicated that the sample dis-

tribution (M = 200.7601 ± 21.50431, SD = 177.32912)

Bq/kg was statistically significantly lower than the world

mean of 640 Bq/kg. The Jamaican mean specific activity of

200 Bq/kg is the vicinity of values reported for Indonesia

(197 Bq/kg), Philippines (212 Bq/kg), and Mexico

(244 Bq/kg) [26].The percentile rank of the world mean

(0.97) suggested that 97 % of the island is below the world

mean for K-40; a similar test showed that 62 % of the

island was below the local mean value of 200 Bq/kg.The

most significant correlations were with thorium (-0.596)

and uranium (-0.704). The higher levels of potassium-40

activity in the eastern end of the island are indicative of

higher levels of potassium salts and potassium–feldspar

present in the soil. The lower levels of potassium (in the

bauxitic areas) are probably due to the process of frac-

tionation which dominates the process of accumulation of

Fig. 1 Simplified geology map of Jamaica: courtesy of the Department of geology and Geography, University of the West Indies

J Radioanal Nucl Chem

123

these radionuclides in the presence of thorium. Addition-

ally, the correlation relationship is probably indicative of

the differences in (a) how they were accumulated in rocks

during the formation period, the different chemical prop-

erties which provided different migration rates, and (b) the

formation patterns of the soils. This low level of correlation

between 40K and 232Th has been reported in a previous

study with value of 0.32 over metamorphic rocks [7].

Potassium moderately correlated with geology (-0.355)

and further investigation using the Independent Samples

Kruskal–Wallis Test indicated that the distribution of the

activity by geology (shown in Fig. 3) was significant,

H(5) = 15.782, p \ 0.05. The Post-Hoc pairwise compar-

ison test within the samples however, indicated that only

the difference (in mean rank) between the White Limestone

and the Cretaceous rocks was statistically significant at the

p = 0.5 level when the adjusted p value (= 0.017) was

used. When the unadjusted p value was used, other sig-

nificant differences in the mean ranks were White Lime-

stone–Alluvium (p = 0.010), White Limestone—Coastal

Group (p = 0.021), and White Limestone Wagwater

(0.036). The largest standard deviation in the specific

activity occurred over the cretaceous rocks (241.73 Bq/kg)

may be probably due to a wide variation in the density of

the potassium–feldspar in the soils or variation in the

chemical processes which gave rise to the rocks in these

areas.

238U and 232Th distribution characteristics in Jamaica

The analysis of uranium-238 (238U) and thorium-232

( 232Th) distribution, shown in Figs. 4 and 5 respectively, is

presented together because of certain similarities in their

distribution in the Jamaican environment. Both radionuc-

lides were closely correlated (0.86) with increased gamma

activity over the central bauxite mining areas of the island.

Their ranges in the Jamaican soil are similar with uranium-

238 ranging from 4 to 400 Bq/kg and thorium ranging from

4 to 172 Bq/kg. The One-Sample T-Test results for ura-

nium [t(67) = -3.687, p \ 0.01] indicated that the local

sample’s mean specific activity (M = 87.0156 ± 12.751,

SD = 105.139) Bq/kg was statistically significantly higher

than the world mean of 40 Bq/kg and by as much as 200 %

in some areas. The Jamaica mean activity of 87 Bq/kg is

similar to Hong Kong (84 Bq/kg) but lower than Thailand

(114 Bq/kg) [26]. The percentile rank of the world mean

(0.54) suggested that 46 % of the island is above the world

mean of 40 Bq/kg for uranium-238. However, for thorium,

the local mean specific activity of 42.92 ± 4.98 Bq/kg was

not statistically different from the world mean value of

40 Bq/kg although 40 % of the island showed elevated

levels of this radionuclide. Locations with similar mean

activity for thorium 232 include India (42 Bq/kg), Iran

(39 Bq/kg), and China (41 Bq/kg) [26]. The Independent

Samples Kruskal–Wallis tests rejected the null hypothesis

that the gamma activity distribution of 238U

[H(5) = 121.018] and 232Th [H(5) = 20.052] were the

same at the a = 0.5 level. The Post-Hoc pairwise com-

parison analysis using the adjusted p value suggested sig-

nificance in the mean rank between the Cretaceous and

White Limestone regions for 238U and between the Coastal

Fig. 2 Map of 40K specific

activity (Bq/kg) distribution

across Jamaica

Fig. 3 -Distribution of 40K specific gamma activity (Bq/kg) over

underlying geology in Jamaica. Post-Hoc pairwise comparison

indicates that only Cretaceous and White Limestone distributions

were statistically significant

J Radioanal Nucl Chem

123

Group and White Limestone regions for 232Th; the dis-

tributions are shown in Figs. 6 and 7.

A published survey of soils in Jamaica, indicated that238U correlated with aluminum (0.72), chromium (0.71),

iron (0.61) and the rare earth elements (0.60–0.76) [22].

The results of this study validates the conclusion of a

previous local study which found higher uranium gamma

levels in bauxite areas of Jamaica [22]. 232Th mobility

during high-grade metamorphism or retrogression has been

suggested as the reason for its variation in metamorphic

rocks, with the highest concentration found in shales due to

absorption into clays. The higher levels of thorium found in

the St. Elizabeth and Trelawny areas of Jamaica were

consistent with previous studies [22]. A previous study

confirms this observation by noting that thorium correlates

well with Al (0.90) in Jamaican soil [22]. Other significant

correlations have been found with Cr (0.86), Sc (0.80), Fe

(0.75), and the rare earth elements (0.72–0.94) [22].The

observation from this study may be useful in using the

activity of Tl-208 to identify areas where bauxite produc-

tion may be useful, as well as areas where the correlated

heavy metals may be found. The negative correlation

Fig. 4 Map of 238U specific

activity (Bq/kg) distribution

across Jamaica

Fig. 5 Map of 232Th specific

activity (Bq/kg) distribution

across Jamaica

Fig. 6 Distribution of 232Th specific gamma activity (Bq/kg) over

underlying geology in Jamaica. Post-Hoc pairwise comparison

indicates that only Coastal Group and White Limestone distributions

were statistically significant

Fig. 7 Distribution of 238U specific gamma activity (Bq/kg) over

underlying geology in Jamaica Post-Hoc pairwise comparison

indicates that only Cretaceous and White Limestone distributions

were statistically significant

J Radioanal Nucl Chem

123

between 232Th and 40K (-0.596) suggested that the

geochemical processes that gives rise to these soils, favors

fractionation over accumulation. The lowest activity of

thorium was noted as occurring over the Wagwater

deposits and Cretaceous rocks in Jamaica.

Total gamma from primordial sources

Figures 8 shows the two main hotspots for primordial

gamma radiation in Jamaican soils. Hot Spot A occur in

soils overlaying the Cretaceous and Wag Water geological

formation in the eastern end of the island, and Hot Spot B

is in the bauxitic soils overlaying predominantly White

Limestone in the central portion of the island. The radiation

map shows that the highest levels of radiation in Jamaica

occur over the non-bauxitic soil regions of the eastern end

of the island with the main contributor here being 40K.

This area is mainly in the St. Thomas and southern Port-

land region where the Wagwater and John Crow Rift

deposits occur in the island. In the analysis (shown in

Table 1), total gamma correlated moderately with 40K

(0.489). The total gamma specific activity was Gaussian in

distribution as shown in Fig. 9.

A One-Way Analysis of Variance Test (ANOVA)

however indicated that the variability in the means (of the

total specific gamma activity) over the geologies was not

statistically significant [H (5) = 1.753, p [ 0.05]. The

study therefore concludes that there is no relationship

between total gamma specific activities from primordial

sources and the underlying soil geologies in Jamaica.

The impact of soil characteristics

The general observations from Table 1 indicated that the

gamma activities of the primordials in Jamaica exhibited

weak to moderate correlation with the chemistry, location,

texture or FAO classification of the soil environment. The

correlation between soil texture and 232Th (0.44) and 238U

(0.50) were moderate but weak for 40K (-0.275). With the

exception of a weak correlation with 232Th (-0.295) no

other primordial radionuclide correlated with the UNE-

SCO/FAO soil categories for the island. The lack of cor-

relation between FAO/UNESCO soil type and primordial

gamma was initially expected, but is perhaps due to the

extensive underlying limestone geology which has varying

levels of primordial concentration. The most significant

correlations for soil characteristics and gamma activities

were organic matters which were positive for 232Th

(0.518), 238U (0.481) but negative for 40K (-0.284). A

possible explanation for this correlation result is that while238U and 232Th accumulate to reasonable concentrations in

soils with high organic matter constituent unlike 40K.The

accumulation of uranium in anaerobic soils and peats has

been noted by other researchers [27, 28]. Ashing of soil

samples could therefore assists in the analysis of 40K.

Ashing is recommended for samples originating from the

biosphere but generally not required for samples originat-

ing from the lithosphere [29].

Summary of major findings

(a) K-40 specific activity values falls below the world

mean (of 640 Bq/kg) in approximately 97 % of the

High : 702.033

Low : 82.8502

Hot Spot A –mainly due to 40K

Hot Spot B –mainly due to 238U

Fig. 8 Map of total gamma

from primordial sources in Bq/

kg in Jamaica showing the two

major radiation hotspots and

their main radionuclide

contributors

Fig. 9 Distribution of total gamma in the data set

J Radioanal Nucl Chem

123

island with the bauxite soil exhibiting lower activity

than the local mean value of 200 Bq/kg. The highest

levels occur in soils overlaying the Cretaceous and

Wag Water geological formation in the eastern end of

the island. The most significant correlations were with

thorium (-0.596) and uranium (-0.704).

(b) 238U and 232Th exhibit certain similarities in their

distribution in the Jamaican environment. Both radio-

nuclides were closely correlated (0.86) with increased

gamma activity over the central bauxite mining areas

of the island. Their ranges in the Jamaican soil are

similar with Uranium 238 ranging from 4 to 400 Bq/

kg and Thorium ranging from 4 to 172 Bq/kg.

(c) Two major radiation hotspots were identified. Hot

Spot A occur in soils overlaying the Cretaceous and

Wag Water geological formation in the eastern end of

the island, and Hot Spot B is in the bauxitic soils

overlaying predominantly White Limestone in the

central portion of the island.

(d) The radiation map shows that the highest levels of

radiation in Jamaica occur over the non-bauxitic soil

regions of the eastern end of the island with the main

contributor here being potassium-40.

(e) While the rank of the mean of specific primordial

activities were significant over the various geological

formations in Jamaica, Post-Hoc non parametric tests

showed that, with the exception of the White Lime-

stones, no other geology could be characterized by all

of the primordial radionuclides specific activities in

the soils in Jamaica. A conservative approach was

adopted to use the adjusted p value instead of the

usual unadjusted p value. This approach showed that

in general, the geology cannot be completely charac-

terized from the radiation signature of the surface

soils.

(f) The organic matter distribution of the Jamaican soil

environment was similar in distribution to 232Th and238U, indicating that bauxitic soils in Jamaica exhibit a

tendency for higher organic matter composition.

(g) The study therefore concludes that there is no

relationship between total gamma specific activities

from primordial sources and the underlying soil

geologies in Jamaica.

Application of research results

(a) The low values recorded for thorium over the Creta-

ceous inliers is typical due to the low bedrock con-

centration inherent in this lithology. Gamma

spectrometry of thorium activity may prove useful in

identifying and classifying lands for agricultural use

based on low or high concentrations of bedrocks

which may accommodate specific plant growth based

on root requirements.

(b) In the Jamaican environment, the gamma profile of

thorium is a minimum distribution over Wagwater

deposits and cretaceous rocks, and a maximum over the

limestone regions of Jamaica. This study suggest that

the wide variation over the limestone regions of

Jamaica is probably due to the existence of metamor-

phic rocks originating from the transformation of

various rock types and now containing various chem-

ical compositions from its prolith. From a geological

perspective, this information may be useful in classi-

fying metamorphic rocks characteristics in Jamaica by

measuring the activity of thallium-208 (208Tl) at

583 keV. Perhaps the gamma activity of the locations

that are similar, may be classified as either originating

in the same era or from the same prolith rocks.

(c) Geostatistical analysis suggested where 232Th spe-

cific activity exceeds approximately 45 Bq/kg, coin-

cided with the areas where the soil is mined for

bauxite and aluminum.

Conclusion

(a) This study recommends the development of a national

environmental specimen banking approach to aid in

the nuclear contamination monitoring by real-time

and retrospective analysis. These contaminants are

more likely to originate from local anthropogenic

sources such as in the manufacturing of cement and

bauxite and the production of electricity, the latter

which is still based on fossil fuels in Jamaica. A good

reference for prototyping a specimen bank has been

published [30]. Since the lungs, kidneys and bone in

humans receive the highest annual doses from ura-

nium [31], additional study in required to further

enhance our understanding of the impact of elevated

levels of soil-resident uranium and their impact on

cancers and related health issues in Jamaica.

(b) The main agricultural produce should be measured to

ascertain the transfer ratio of uranium since thorium is

relatively insoluble with low specific activity making

it available in biological materials in insignificant

amounts [31]. Also, since the human body does not

store excess potassium because of matters related to

homeostatic control and the relative low level of 40K

found in Jamaican soils, 40K radiation is not

considered critical.

Acknowledgments The authors wish to acknowledge the kind

cooperation of the following organizations: The Rural Physical

J Radioanal Nucl Chem

123

Planning Authority, Ministry of Agriculture, Jamaica, The Depart-

ment of Geology and Geography, the University of the West Indies,

Mona Campus, and The Mona Geoinformatics Institute.

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