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DOI 10.1007/s12665-011-1126-5
ORIGINAL ARTICLE
Received: 18 December 2009 / Accepted: 13 May 2011 / Published online: 15 June 2011
Ó Springer-Verlag 2011
Abstract Groundwater contaminated with arsenic (As), 50–690 lg/L; mean 321 lg/L) in groundwater has excee-
when extensively used for irrigation, causes potentially ded both WHO recommended guideline values (10 lg/L)
long-term detrimental effects to surface soils. Such con- and the National safe drinking water limit (50 lg/L).
tamination can also directly affect human health when Regression analyses demonstrate that the bioavailability of
irrigated crops, such as rice, vegetable and fruits, are used As in the soil horizon is mainly controlled by the compo-
for human consumption. Therefore, an understanding of the sition of free Fe2O3 and CaCO3 content of the soils. How-
leaching behavior of As in surface soils is of high impor- ever, application of P could increase bioavailability of As
tance, because such behavior may increase the bioavail- in the soil horizon and become available to plants for
ability of As in the soil horizon. In this study, we have uptake.
investigated the role of phosphate ions in leaching and
bioavailability of As in the soil horizon, where drinking Keywords Arsenic Bioavailability Bicarbonate Iron
groundwater contains elevated levels of As (C50 lg/L). oxyhydroxide Phosphate Soil properties
Soil and groundwater samples were characterized in the
laboratory and measured for physical and chemical con-
stituents. The soils are generally neutral to slightly alkaline Introduction
in character (pH range 7.5–8.1) with low to moderate levels
of free Fe2O3, Al2O3, CaCO3, organic carbon, and clay Arsenic (As) is a toxic and ubiquitous element in nature,
content. The measured electrical conductivity (mean which poses a potential threat to human health and the
599 lS/cm) of the soils demonstrates their non-saline environment. Arsenic is widely distributed in nature
nature. The Eh values (range -37 to -151 mV) of the (especially in soils) with concentrations ranging from 1 to
groundwater indicate anoxic condition with low to moder- 40 mg/kg (Eckel and Langley 1988; Yan-Chu 1994).
ate levels of bicarbonate (range 100–630 mg/L) and phos- Arsenic can be mobilized from the soils to groundwater
phate (range 0.002–4.0 mg/L). The arsenic content (range under favorable geochemical conditions (e.g., Smedley and
Kinniburgh 2002; Nath et al. 2009). Recently, naturally
occurring high As concentration was observed in ground-
S. J. Sahu S. Roy D. Chatterjee (&)
Department of Chemistry, University of Kalyani, water in Bengal Delta Plain (BDP). Such high As occur-
Kalyani 741 235, West Bengal, India rences in groundwater had received significant
e-mail: dbchat2001@rediffmail.com international attention due to widespread exposure to
human health and the environment (e.g., Smith et al. 2000;
B. Nath
School of Geosciences, University of Sydney, Guha Mazumder et al. 2000).
Sydney, NSW 2006, Australia The bioavailability of As in soil is strongly controlled by
the adsorption and desorption processes (Quaghebeur et al.
B. Mandal
2005; Naidu et al. 2009a). The use of arsenical pesticides
Department of Agricultural Chemistry and Soil Science,
Bidhan Chandra Krishi Viswavidyalaya, Kalyani 741 235, and/or fertilizers during irrigation, farming practice
West Bengal, India enhances As accumulation in soils (Sandberg and Allen
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814 Environ Earth Sci (2012) 65:813–821
123
Environ Earth Sci (2012) 65:813–821 815
multimeter (WTW, Germany). Free iron oxides (Fe2O3) as HCO3) was also measured in the field using the titri-
were extracted by citrate–bicarbonate–dithionite solution metric method described by Bhattacharyya et al. (2003).
following the method of Mehra and Jackson (1960). The The samples were filtered on-site using Sartorious filter
clay and organic carbon contents of the soils were mea- paper (0.45 lm) and separated into two groups: (1) filtered
sured following the method described in Jackson (1973). un-acidified for anion (e.g., NO3, PO4 and SO4) and (2)
CaCO3 contents were extracted with 0.5 N HCl following filtered acidified (with a few drops of HNO3, pH *2) for
the procedure described in Black (1965). The Al2O3 con- total As and Fe analysis. The anion concentrations were
tent was extracted with 0.5 N NaOH following the proce- measured by ion chromatography (Dionex, CA, USA)
dure detailed in Jackson (1973). The soil As content (easily using external calibration (accuracy ±6% and precision
labile and/or surface adsorbed fractions) was determined ±5%). Arsenic and iron concentrations were measured
by extraction with 0.1 M NaHCO3 at a pH of 8.5. The using a HG-AAS (accuracy and precision ±5%).
detailed soil As extraction procedure was described in
McLaren et al. (1998). The extractant was measured for As Column experiments
concentrations using a hydride generation atomic absorp-
tion spectrophotometer (HG-AAS). Undisturbed soil cores (in a polyvinyl chloride hollow pipe,
Groundwater pH, Eh, and EC were measured in the field length 60 cm, inner diameter 10 cm) were collected from
using WTW multimeters (Germany). Alkalinity (reported two sites (areas of low and high As concentrations in
Table 1 Chemical characteristics of the soil samples collected from the guava orchards of the study area
Location ID Latitude Longitude As pH EC Al2O3 CaCO3 Fe2O3 Organic carbon Clay
(mg/kg) (lS/cm) (g/kg) (g/kg) (g/kg) (g/kg) (g/kg)
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816 Environ Earth Sci (2012) 65:813–821
groundwater) to examine the influence of phosphate ions electrical conductivity of the soils ranged between 75 and
on the bioavailability of As in the soil horizon. Each soil 1,170 lS/cm (mean 599 lS/cm), indicating non-saline
profile was divided into two columns. The first column was nature (Table 1).
used as a control, while 10 ppm As was applied (from the Alkali bicarbonate salt (0.1 M NaHCO3) was used to
top) to the second column. After amending with As, the extract As (easily labile and/or surface adsorbed fractions)
soil columns were left for aging (15 days). On the com- from different soil horizons. The extracted As content of
pletion of the aging period, three levels of phosphorous (1) the soils ranged between 2.5 and 11 mg/kg, with a mean
distilled water with no phosphorous (as a control), (2) concentration of 6.5 mg/kg. The result showed variable
50 mg/kg of phosphorous, and (3) 100 mg/kg of phos- amount of As extracted from different soil layers (Fig. 2).
phorous solution was applied to both groups of soil and left The depth variation showed a decreasing trend in all but
for aging (18 months). During the aging period, the col- one soil column, suggesting that most of the As imported
umns were kept under moist condition by adding distilled during irrigation drawdown is being adsorbed at shallow
water to maintain the site condition. After 18 months, each depth in the soil profile (0–15 cm). At pH 8.5, bicar-
soil column was cut into four equal pieces and the samples bonate ion was used to displace loosely bound As from
were collected from each parts (0, 15, 30 and 60 cm). The the surface sites of Fe-oxyhydroxides and thereby
collected soil samples were dried, ground, and sieved increasing bioavailability of As in the soil horizon
(\2 mm), and finally extracted for As (easily labile and/or (Anawar et al. 2004). However, downward leaching of As
surface adsorbed fractions) with 0.1 M NaHCO3 at a pH of may be controlled by the permeability of the soils, which
8.5. The extracted As was measured with HG-AAS. might have partly controlled the distribution of As in the
shallow groundwater and/or uptake by the plants (Nath
et al. 2008).
Statistical analysis
Soil properties
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Environ Earth Sci (2012) 65:813–821 817
139–630 mg/L; mean 309 mg/L). The electrical conduc- sulfidic minerals, Fe-oxyhydroxides etc.) (Smedley and
tivity of groundwater ranges from 600 to 3,800 lS/cm Kinniburgh 2002). However, accumulation of As in soils
(mean 1,250 lS/cm). Groundwater contains low to mod- due to irrigation drawdown and subsequent increase in
erate levels of nitrate (range 0.01–0.43 mg/L; mean bioavailability to plants is governed by the combination of
0.12 mg/L), phosphate (range 0.01–4.0 mg/L; mean geochemical and anthropogenic processes. The correlation
0.49 mg/L), Fe (range 1.6–25 mg/L; mean 13 mg/L) and of As versus Fe in groundwater (Table 3) suggests that the
sulphate (range 0.28–88 mg/L; mean 14 mg/L). The Eh release of As at this site is controlled in part by the redox
values (-144 to -37 mV) of the groundwater demonstrate reaction involving the dissolution of Fe-oxides. This
reducing nature of the aquifer. The range of As content observation is in agreement with the previous studies from
(50–690 lg/L; mean 321 lg/L) in groundwater exceeded BDP (e.g., PHED 1993; BGS and DPHE 2001; McArthur
both the WHO recommended guideline value (10 lg/L) et al. 2001). Therefore, the impact of groundwater use for
and the National safe drinking water limit (50 lg/L). irrigation will be manifold (1) accumulation of As in sur-
The mobilization of As in groundwater is thought to be face soils, (2) increasing bioavailability of As for plant
controlled by the geochemical processes that involve uptake, and (3) downward leaching of As to the shallow
leaching of As from the source material (e.g., As-bearing aquifer.
Table 2 Chemical characteristics of the groundwater samples collected from the household domestic wells of the study area
Well Latitude Longitude Depth pH Eh EC As Fe NO3 PO4 SO4 Alkalinity
ID (m) (mV) (lS/cm) (lg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L)
SJ01 22.3490 88.4600 22 8.1 -110 850 50 25 0.01 0.12 3.2 139
SJ02 22.3425 88.4725 24 8.0 -101 1,000 610 21 0.16 0.34 0.28 335
SJ03 22.3257 88.4605 17 7.4 -63 700 220 23 0.01 0.12 2.7 189
SJ04 22.3167 88.4708 37 8.1 -40 1,100 630 20 0.43 0.32 5.2 255
SJ05 22.3250 88.4617 15 7.7 -136 750 100 3.4 0.11 4.0 4.6 602
SJ06 22.3292 88.4820 30 7.4 -60 1,600 690 24 0.01 0.16 1.9 630
SJ07 22.3142 88.4642 22 7.4 -42 650 652 20 0.41 0.08 3.3 349
SJ08 22.3350 88.4642 14 7.4 -61 800 200 21 0.08 0.52 2.1 352
SJ09 22.3200 88.4533 15 7.6 -48 800 170 20 0.01 0.08 5.1 156
SJ10 22.3258 88.4767 40 7.4 -41 1,000 553 17 0.05 1.0 5.3 449
SJ11 22.3085 88.4545 14 7.4 -40 1,200 600 19 0.41 0.34 3.7 284
SJ12 22.3092 88.4623 18 7.5 -44 1,200 510 17 0.40 0.56 5.2 290
SJ13 22.3615 88.4783 61 7.3 -51 600 440 16 0.15 0.03 3.3 260
SJ14 22.3275 88.4575 21 7.6 -53 850 110 17 0.01 0.01 13 153
SJ15 22.3615 88.4670 30 7.5 -125 700 510 17 0.40 0.99 16 167
SJ16 22.3400 88.5465 74 7.4 -89 2,800 480 18 0.01 0.01 32 175
SJ17 22.3357 88.4683 18 7.3 -44 1,700 406 13 0.01 1.7 11 480
SJ18 22.3152 88.4495 20 8.0 -58 800 210 11 0.01 0.16 3.3 182
SJ19 22.3188 88.4657 55 6.9 -58 800 271 7.4 0.11 0.36 5.3 240
SJ20 22.3358 88.4690 30 7.9 -37 1,100 271 9.1 0.01 2.1 13 416
SJ21 22.3107 88.4607 40 7.1 -71 1,200 245 9.0 0.07 0.15 3.8 455
SJ22 22.3388 88.5053 243 7.4 -95 2,500 235 9.6 0.01 0.19 62 398
SJ23 22.3572 88.4672 11 7.5 -144 1,300 90 1.6 0.01 0.03 1.2 195
SJ24 22.3083 88.4620 15 7.4 -52 1,300 209 7.5 0.41 0.29 6.2 288
SJ25 22.3347 88.4487 27 7.5 -63 650 120 5.7 0.01 0.01 7.3 142
SJ26 22.3333 88.4633 14 7.4 -50 700 510 7.0 0.30 0.64 12 388
SJ27 22.3330 88.5167 243 7.8 -86 1,800 133 3.5 0.01 0.28 57 370
SJ28 22.3452 88.5448 107 7.5 -58 2,600 102 3.2 0.01 0.01 29 250
SJ29 22.3345 88.5315 259 7.4 -45 3,800 164 5.7 0.01 0.01 88 450
SJ30 22.3035 88.4692 37 7.3 -65 900 133 3.4 0.01 0.01 1.8 215
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818 Environ Earth Sci (2012) 65:813–821
Table 3 Correlation coefficient (Pearson r) of different chemical characteristics of the groundwater and soil samples collected from the study
area
Groundwater composition Soil composition
pH 1
Eh -0.20 1
EC -0.11 0.01 1
As -0.05 0.30 -0.10 1
Fe 0.21 0.19 -0.26 0.53 1
NO3 0.01 0.17 -0.28 0.59 0.22 1
PO4 0.15 -0.23 -0.17 -0.02 -0.20 0.04 1
SO4 -0.04 -0.03 0.83 -0.23 -0.35 -0.25 -0.13 1
Alkalinity -0.16 0.07 0.24 0.27 -0.12 -0.04 0.54 0.18 1
As -0.31 0.04 0.45 -0.43 -0.85 -0.21 -0.19 0.52 -0.04 1
pH 0.34 0.00 -0.44 0.47 0.81 0.29 0.24 -0.53 0.04 -0.97 1
EC -0.31 0.04 0.44 -0.43 -0.86 -0.22 -0.17 0.50 -0.04 1.00 -0.96 1
Al2O3 0.30 -0.04 -0.46 0.40 0.85 0.22 0.16 -0.54 0.02 -0.99 0.96 -0.99 1
CaCO3 0.28 -0.04 -0.44 0.41 0.86 0.19 0.17 -0.53 0.01 -0.99 0.96 -0.99 0.99 1
Fe2O3 -0.26 0.03 0.44 -0.38 -0.83 -0.18 -0.21 0.50 -0.07 0.98 -0.94 0.98 -0.98 -0.97 1
Org C -0.32 0.02 0.44 -0.42 -0.85 -0.20 -0.21 0.52 -0.04 0.99 -0.97 0.99 -0.99 -0.99 0.97 1
Clay 0.31 -0.02 -0.44 0.43 0.85 0.23 0.20 -0.50 0.03 -0.99 0.97 -0.99 0.99 0.99 -0.97 -0.99 1
Bioavailability of arsenic in the soil horizon Therefore, under such conditions, bicarbonate can easily
exchange arsenate from the adsorbed phases and thereby
Effect of soil properties increasing dissolved As concentrations (Appelo et al.
2002). Appelo et al. (2002) further reported that the sorp-
Regression analysis was performed to identify the inter- tion of carbonate ions at common soil and groundwater
relationships between different soil properties (e.g., pH, EC, concentrations reduces adsorption of As onto ferrihydrite
Al2O3, CaCO3, Fe2O3, organic carbon, and clay contents) resulting in release of As in groundwater. Moreover, the
and the bioavailability of As in soils. The result showed association between Fe2O3 and As further suggests that
positive correlation between the extracted soil As versus bioavailability of As can be controlled by the Fe-reduction
Fe2O3 (r = 0.99), and organic carbon (r = 0.99) (Table 3). processes (e.g., breakdown of organic matter under low
This suggests an association of As with free Fe2O3 and redox condition) in the shallow groundwater. This issue is
organic carbon. Under moist conditions (mainly during rainy currently being investigated at this site, and also supported
season) As might therefore release in the root zone of the soil by the positive correlation between the dissolved As and Fe
layers due to microbial oxidation of organic matter, thereby concentrations and low Eh values (Table 3).
increasing the bioavailability of As in the soil horizon
and thereby increasing plant uptake. Previous studies (De Effect of phosphate ion
Brouwere et al. 2004; Violante and Pigna 2002) also dem-
onstrated the same, where Fe-oxides appear to be the most The column tests indicated that the addition of P did not
important solid phase that adsorbs and retains As(V). increase the bioavailability of As in the soils collected from
A stepwise regression model (soil As = 1.6 - 0.06 the areas of low As concentrations in groundwater
CaCO3** ? 0.61 Fe2O3**; R2 = 0.99; **significant at (Fig. 3a). However, *70% of the adsorbed As was able to
p \ 0.01) has indicated that Fe2O3 and CaCO3 are the two be extracted from the soils collected from areas of high As
important mineral phases that control the bioavailability of concentrations in groundwater (Fig. 4a). This suggests that
As in the soil horizon. In alkaline condition, As is less competitive phosphate–arsenate exchange might be an
strongly bound to Fe-oxyhydroxides than at neutral or low important mechanism for increasing the bioavailability of
pH condition (Smedley et al. 2002). Calcium carbonate As in the soil horizon. Generally, phosphate enhances the
generally reacts with H? ions, causing increase in the bioavailability of As in the soil environment by displacing
bicarbonate concentration and pH of the solution. arsenate from the sorption sites and increasing soil P
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Environ Earth Sci (2012) 65:813–821 819
Fig. 3 Leaching of As in control and phosphate amended (50 and Fig. 4 Leaching of As in control and phosphate amended (50 and
100 mg/kg) soils collected from areas where low As concentrations in 100 mg/kg) soils collected from areas where high As concentrations
groundwater were observed: a native soil, and b As amended in groundwater were observed: a native soil, and b As amended
(10 ppm) soil (10 ppm) soil
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820 Environ Earth Sci (2012) 65:813–821
soils, where As containing herbicides and/or insecticides De Brouwere K, Smolders E, Merckx R (2004) Soil properties
are used (Woolson 1973). Increases in As bioavailability affecting solid–liquid distribution of As (V) in soils. Eur J Soil
Sci 55:165–173
may induce the accumulation of As in the plants as well as Eckel WP, Langley WD (1988) A background-based ranking
in the fruits. There are many reports available in the lit- technique for assessment of elemental enrichment in soils at
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detrimental to human health. Conference, Nov 28–30, Washington DC, Silver Spring, MD.
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Jackson ML (1973) Soil Chemical analysis, 2nd edn. Prentice Hall of
This study indicates that application of P to As-contami- India Pvt. Ltd., New Delhi, p 498
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As in the soil horizon, thereby increasing the risk associ- corn. Commun Soil Sci Plant Anal 1:85–93
ated with As uptake by plants in orchards. Bicarbonate ion Johnston SE, Barnard WM (1979) Comparative effectiveness of 14
solutions for extracting arsenic from 4 western New York soils.
was also shown to influence As leaching at this site. The Soil Sci Soc Am J 43:304–308
magnitude of this behavior is varied between the soils, McArthur JM, Ravencroft P, Safiullah S, Thirlwall MF (2001)
which are influenced by the As loading, physical and Arsenic in groundwater: testing pollution mechanism for sedi-
chemical properties of the soil, the amount of bicarbonate mentary aquifers in Bangladesh. Water Resour Res 37:109–117
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Acknowledgments The principal author (DC) acknowledges the Mehra OP, Jackson ML (1960) Iron oxide removal from soils and
support of Late Prof. Nityananda Saha (Ex-Vice Chancellor, Uni- clays by a dithionite- Citrate system buffered with sodium
versity of Kalyani) to carry out this research work. The authors would bicarbonate. Clay miner 7:317–327
also like to acknowledge the Swedish Research Council (VR), Sida- Melamed R, Jurinak JJ, Dudley LM (1995) Effect of adsorbed
SAREC and Rajiv Gandhi National Drinking Water Mission phosphate on transport of arsenate through an oxisol. Soil Sci
(RGNDWM), Department of Drinking Water Supply, Govt. of India Am J 59:1289–1294
for supporting the research on high arsenic groundwater of West Naidu R, Bhattacharya P (2009) Arsenic in the environment—risks
Bengal, India. and management strategies. Environ Geochem Health 31:1–18
Naidu R, Smith E, Imamul Huq SM, Owens G (2009) Sorption and
bioavailability of arsenic in selected Bangladesh soils. Environ
Geochem Health 31:61–68
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