Chemosphere 139 (2015) 5464

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Chemosphere
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Concentrations of arsenic and other elements in groundwater of

Bangladesh and West Bengal, India: Potential cancer risk
Mohammad Mahmudur Rahman, Zhaomin Dong, Ravi Naidu
Centre for Environmental Risk Assessment and Remediation (CERAR), University of South Australia, Mawson Lakes Campus, SA 5095, Australia
Cooperative Research Centre for Contamination Assessment and Remediation of the Environment (CRC-CARE), PO Box 486, Salisbury South, SA 5106, Australia

h i g h l i g h t s

 Data on arsenic and other elements from arsenic-endemic areas of Bengal delta.
 Arsenic contaminated groundwater also had unsafe levels of Mn, Se and U.
 Data were compared with previously published data from Southeast Asian regions.
 Correlations between arsenic and other elements.
 Estimation of potential cancer risk.

a r t i c l e i n f o a b s t r a c t

Article history: We investigated the concentrations of 23 elements in groundwater from arsenic (As) contaminated areas
Received 25 July 2014 of Bangladesh and West Bengal, India to determine the potential human exposure to metals and metal-
Received in revised form 14 May 2015 loids. Elevated concentrations of As was found in all ve study areas that exceeded the World Health
Accepted 17 May 2015
Organization (WHO) guideline value of 10 lg/L. The mean As concentrations in groundwater of
Noakhali, Jalangi and Domkal, Dasdia Nonaghata, Deganga and Baruipur were 297 lg/L, 262 lg/L,
115 lg/L, 161 lg/L and 349 lg/L, respectively. Elevated concentrations of Mn were also detected in all
Keywords:
areas with mean concentrations were 139 lg/L, 807 lg/L, 341 lg/L, 579 lg/L and 584 lg/L for
Arsenic
Groundwater
Noakhali, Jalangi and Domkal, Dasdia Nonaghata, Deganga and Baruipur, respectively. Daily As intakes
Tubewell from drinking water for adults and the potential cancer risk for all areas was also estimated. Results sug-
Manganese gest that mitigation activities such as water treatment should not only be focused on As but must also
Cancer risk consider other elements including Mn, B and Ba. The groundwater used for public drinking purposes
needs to be tested periodically for As and other elements to ensure the quality of drinking water is within
the prescribed national guidelines.
2015 Published by Elsevier Ltd.

1. Introduction these regions is still unknown. In 2008 UNICEF estimated that

To prevent water-borne diseases such as diarrhoea, cholera, and
typhoid, and to reduce the childhood mortality, millions of tube-
wells were installed to provide safe drinking water supplies to
the inhabitants of Bangladesh, India and other Asian countries
(Smith et al., 2000; Harvey et al., 2002; UNICEF, 2003; Escamilla
et al., 2011). Groundwater is the primary source of potable water
in the Bengal deltaic plain of Bangladesh and West Bengal state
of India (Rahman et al., 2003). The exact number of tubewells in
Corresponding author at: Centre for Environmental Risk Assessment and
Remediation (CERAR), University of South Australia, Mawson Lakes Campus, SA
5095, Australia.
E-mail address: ravi.naidu@crccare.com (R. Naidu).
the number of tubewells in Bangladesh alone was 8.6 million,
based on an arsenic (As) mitigation project (http://www.unicef.
org/bangladesh/Arsenic.pdf). Although these tubewells reduced
deaths from water-borne diseases, millions of people are currently
exposed to As through consumption of contaminated groundwater.
Arsenic contamination of the groundwater of West Bengal was rst
recognized in 1982 and it came into the limelight during the
International Conference on As in 1995 in Calcutta (International
Conference on Arsenic, 1995). Detailed investigations by
Chakraborti et al. (2009) showed that 3417 villages in 107 blocks
(precinct) from nine districts in West Bengal contained elevated
concentrations of As in groundwater. This study also reported that
48.1% of the tubewells had As concentrations in groundwater
>10 lg/L (the WHO guideline value for drinking water) and 23.8%

http://dx.doi.org/10.1016/j.chemosphere.2015.05.051
0045-6535/ 2015 Published by Elsevier Ltd.
 M.M. Rahman et al. / Chemosphere 139 (2015) 5464
had As concentrations >50 lg/L (guideline value for many develop-
ing countries including India and Bangladesh), based on analyses of
140,150 water samples from tubewells in all 19 districts of West
Bengal.
Arsenic contamination of groundwater in Bangladesh was rst
reported in 1992 (Dhar et al., 1997). Based on an analysis of
52,202 tubewell water samples from all 64 districts of the country,
As concentrations exceeding 10 lg/L and 50 lg/L were found in 59
districts and 50 districts, respectively; 27.2% and 42.1% of all ana-
lyzed tubewells had As > 50 lg/L and 10 lg/L, respectively
(Chakraborti et al., 2010). The British Geological Survey (BGS)
and the Department of Public Health Engineering (DPHE) reported
that 46% and 27% of the 3534 tubewells water analysis from all
over Bangladesh, excluding the Chittagong Hill tract, exceeded
10 lg/L and 50 lg/L of As, respectively (BGS-DPHE, 2001). It was
also reported that 57 million and 35 million people could be drink-
ing water contaminated by As at concentrations >10 lg/L and
>50 lg/L, respectively, in Bangladesh (BGS-DPHE, 2001).
Arsenic occurs in nature as a component of more than 245 min-
erals, usually ores containing sulde, along with metals including
copper, nickel, lead, cobalt, etc. (Mandal and Suzuki, 2002). The
weathering of rocks and minerals appears to be the main source
of As in the soils, rocks, natural waters and organisms; mobilized
through a combination of natural processes such as weathering
reactions, biological activity, transport, precipitation, volcanic
emissions as well as through a number of anthropogenic activities
(Smedley and Kinniburgh, 2002). Several theories such as oxida-
tion, reduction, and recent inow of carbon have been proposed
to explain the mechanism of As release in groundwater of the
Bengal delta (Bhattacharya et al., 1997; Nickson et al., 1998;
Chowdhury et al., 1999; Harvey et al., 2002; Ahmed et al., 2004).
A study from West Bengal reported that metal-reducing bacteria
play a crucial role in the As release from sediments (Islam et al.,
2004). A study from Bangladesh reported that microbially or geo-
chemically mediated reductive dissolution of As associated with
Fe oxyhydroxides is the main mechanism for As release, and that
the reducing conditions are caused by decomposition of organic
matter (Anawar et al., 2011).
Previous and current research activities in Bangladesh and West
Bengal are primarily focused on the extent and severity of As con-
tamination, sources and mobilization of As, human health effects,
entry of As into the food chain, social and socioeconomic aspects
of arsenicosis-affected patients, and mitigation options
(Chakraborti et al., 2010 and references therein). Most of the previ-
ous studies focus on risk posed by exposure to As. Less attention
has been paid to other elements present in groundwater from
these regions, especially in the Bengal delta plain. A few articles
have addressed the concentrations of As and other toxic elements
in groundwater from several countries in Southeast Asia, mainly
from Cambodia and Vietnam, based on limited numbers of samples
(Agusa et al., 2006; Buschmann et al., 2007,2008; Frisbie et al.,
2002,2009; Islam et al., 2000; Luu et al., 2009; Nguyen et al.,
2009; Roychowdhury et al., 2003; Shinkai et al., 2007; Winkel
et al., 2008). Besides As, other elements such as Mn, Ba, B, Se, U,
Ni, Pb, Cd, Fe, and Cr in groundwater exceeded the WHO drinking
water guideline values. Only a few articles reported the presence of
other elements in the groundwater of Bangladesh and West Bengal
(Frisbie et al., 2002, 2009; Islam et al., 2000; Ohno et al., 2005;
Roychowdhury et al., 2003; Nath et al., 2008,2011). In 2009,
UNICEF conducted analysis of groundwater in Bangladesh for met-
als and metalloids as a part of national drinking water quality sur-
vey and reported that 65% of the water samples met the previous
WHO guideline value for Mn (400 lg/L) (UNICEF, 2011).
Recently WHO (2011) revised the drinking water quality guide-
lines for several elements such as B, Se, Mn and U. The previous
WHO guideline values for B, Se, Mn and U were 500 lg/L,
55
10 lg/L, 400 lg/L and 15 lg/L, respectively, which were recently
revised and increased to 2400 lg/L, 40 lg/L and 30 lg/L for B, Se
and U, respectively. Currently there is no guideline value for Mn
in drinking water (WHO, 2011). A study showed that 35% of the
groundwater samples exceeded the previous WHO guideline value
(400 lg/L) for Mn and 5.3% of the samples exceeded the previous
WHO guideline value (500 lg/L) for B, based on a nationwide sur-
vey in Bangladesh (BGS-DPHE, 2001). The risk and implications of
exposure to elevated levels of other elements in combination with
As to human health from mixed contaminants in potable water is
yet to be established. WHO (2005) developed a comprehensive
publication for enacting a water safety plan (WSP) which is of
utmost importance as far as the drinking water quality of ground-
water for public consumption is concerned. Unfortunately, this
approach has been largely overshadowed in the past few years
by the As calamity in the Bengal delta plain. Ongoing activities of
classifying safe drinking water sources by testing tubewells for
As only will not assure safe levels of Mn, U, Pb, Ni, Cr, and probably
other elements (Frisbie et al., 2009). Although As is of major con-
cern in the Bengal deltaic plain, policy makers are not yet cog-
nizant of the potential health hazards of the presence of other
trace elements in groundwater. Therefore, it is important to con-
duct a study on As and other elements present in groundwater
from As-contaminated areas in Bengal delta regions of
Bangladesh and West Bengal.
The present study reports the concentrations of As and an addi-
tional twenty two potentially toxic elements including Be, B, Na,
Mg, K, Ca, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Se, Mo, Cd, Sn, Sb, Ba, Pb,
and U in groundwater from an As-affected area in Bangladesh
and four areas of West Bengal where groundwater contains As
levels greater than 50 lg/L to determine the magnitude of ground-
water contamination by a wide range of elements. We applied the
results to determine the daily intakes of As and other elements
from drinking water by adults.
2. Materials and methods
2.1. Groundwater sampling and analysis
Groundwater from tubewells was sampled from randomly
selected tubewells from two neighboring villages (Chiladi and
Basantapur) in the Noakhali district of Bangladesh during
December 2008 and four As-contaminated areas (Domkal and
Jalangi blocks in Murshidabad, Dasdia Nonaghata villages in Nadia,
Deganga block in North 24 Parganas district, and Baruipur block in
South 24 Parganas district) of West Bengal in December 2009.
The Bengal deltaic plain consists of sediments deposited by the
Ganges, Brahmaputra, and Meghna rivers and their tributaries and
distributaries (Bhattacharya et al., 1997). Arsenic in groundwater is
hosted by the sediments deposited by the meandering river chan-
nels during the late Quaternary or the Holocene age (Mukherjee
and Bhattacharya, 2001).
The Bengal delta of West Bengal can be divided into two
regions: (1) the upper deltaic plain of meander belts of the
PadmaBhagirathi Rivers in the north and (2) the lower deltaic
plain with several tidal creeks in the south (Das et al., 1996).
Arsenic affected areas of West Bengal are all located in the upper
deltaic plain and mostly in the abandoned meander belts (Das
et al., 1996). Districts such as Murshidabad, Nadia and North 24
Pargana are in the upper deltaic plain of the meander belt whereas
South 24 Pargana is in lower deltaic plain of the Gangetic plain in
West Bengal (Bhattacharya et al., 1997). Groundwater occurs
under unconned conditions particularly in the Nadia and
Murshidabad and under semi-conned conditions in the North
and South 24-Parganas districts (Bhattacharya et al., 1997).
56 M.M. Rahman et al. / Chemosphere 139 (2015) 5464

There are four main geo-morphological regions in Bangladesh
namely (a) Hill Tract, (b) Table Land (Pleistocene Plain and
Pleistocene Upland), (c) Flood Plain and (d) Deltaic Region (includ-
ing Coastal regions) (Chakraborti et al., 2010). Most groundwater
from the shallow alluvial aquifers (<150 m), particularly in the
Holocene plain lands, are susceptible to elevated As concentrations
(Ahmed et al., 2004). The deltaic plain and ood plains of the
GangaBrahmaputra river system are the most As-contaminated
areas in Bangladesh (Ahmed et al., 2004; Chakraborti et al.,
2010). The study area Noakhali is situated in ood plain region of
Bangladesh.
The tubewells were purged for 5 min before sample collection.
All groundwater samples were stored in plastic tubes and pre-
served in nitric acid (7 M). All samples were stored in a cool ice
box and then transported to the CERAR laboratory for
multi-elemental analysis.
An Agilent (7500ce) inductively coupled plasma mass spec-
trometer (ICP-MS) with an octopole reaction system (ORS) was
used for multi-elemental analysis.
2.2. Quality control and quality assurance issues
Standard Reference Material (NIST 1640a trace elements in
natural water and NIST 1643e trace elements in water) from
the National Institute of Standards and Technology (NIST) were
used to check the results of the analyses of As and other elements.
The certied and observed values of NIST water standards for all
examined elements are presented in Table 1. The observed values
show good agreement with certied values for all elements.
2.3. Statistical analysis
The Pearson correlation coefcient was used to determine the
strength of the relationships between As and other elements. A p
value of <0.01 was considered to indicate statistical signicance.
Multiple correlation coefcient of As in groundwater samples were
also estimated. As we examined 23 analytes for this study, so there
were potentially 22 variables that could be used in a multiple
correlation.
2.4. Distribution of elements and their speciation and mineral
saturation index
The distribution of elements and their speciation and saturation
indices (SI) of major mineral phases in groundwater were deter-
mined using the aqueous geochemical modeling program
PHREEQC to understand aqueous speciation of these trace ele-
ments (http://www.ndsu.edu/pubweb/webphreeq/webphreeq-2.
0/).
3. Results and discussion
3.1. Arsenic concentrations in groundwater of Bangladesh and West
Bengal
Table 2 presents the concentrations of As and other elements in
groundwater of the Noakhali in Bangladesh. About 98.6% of the
samples had As concentrations greater than the WHO guideline
value for drinking water (10 lg/L), and 97% of the samples had
As concentrations greater than the Bangladeshi standard
(50 lg/L). The mean As concentration was almost 30 times greater
than the WHO guideline value and almost six times higher than the
Bangladeshi standard. A study reported that 72 out of 73 tubewells
sampled in Chiladi village before 2002 contained As concentrations
exceeding 100 lg/L (Chakraborti et al., 2010). It was also found
that 21 tubewells from this village had As concentrations
>1000 lg/L (Chakraborti et al., 2010). Due to the mitigation activ-
ities many contaminated tubewells were sealed or rebored and it
can be expected that As concentrations in this study would differ
from those in Chiladi reported earlier.
The concentrations of As and other elements in groundwater
from four areas of West Bengal are presented in Table 3. About
98.4% of the tubewells analyzed in Jalangi and Domkal, 95% in
Deganga, and 100% in Baruipur had As concentrations greater than
10 lg/L whereas 53% of the samples from Dasdia Nonaghata had As
concentrations greater than 10 lg/L. The percentages of samples
that exceeded 50 lg/L were 92%, 88%, 100%, and 41% in Jalangi
and Domkal, Deganga, Baruipur, and Dasdia Nonaghata, respec-
tively. The highest concentration found in a tubewell water sample
was 1219 lg/L in Jalangi and Domkal. A study reported that 57%

Table 1
Arsenic and other elements in NIST SRMs.

Elements NIST 1640a (n = 12) NIST 1643e (n = 12)

Certied values Observed values Percentage of recovery Certied values Observed values Percentage of recovery
As (lg/L) 26.67 0.41 25.35 1.71 95.1 60.45 0.72 54.67 2.91 90.4
Be (lg/L) 34.94 0.41 35.08 1.52 100.4 13.98 0.17 14.08 1.17 100.7
B (lg/L) 301.1 6.1 283.6 12.75 94.2 157.9 3.9 168.5 9.5 106.6
Na (mg/L) 29.35 0.31 30.93 2.13 105.3 20.740 0.260 19.061 0.953 91.9
Mg (mg/L) 5.8 0.056 5.4 0.137 93.8 8.037 0.098 7.845 0.549 97.6
K (mg/L) 994 27 993 95 99.9 2.034 0.029 1.917 0.106 94.2
Ca (mg/L) 7.045 0.089 7.596 1.025 107.8 32.3 1.1 24.7 1.7 76.5
V (lg/L) 12.99 0.37 12.64 0.33 97.3 37.86 0.59 35.63 3.15 94.1
Cr (lg/L) 38.6 1.6 35.7 1.14 92.5 20.4 0.24 19.7 1.99 96.9
Mn (lg/L) 121.5 1.1 115.3 4.06 94.9 38.97 0.45 37.90 3.42 97.3
Fe (mg/L) 34.3 1.6 35.2 1.62 102.6 98.1 1.4 103.0 12.66 104.9
Co (lg/L) 20.28 0.31 19.64 0.72 96.8 27.06 0.32 25.93 2.53 95.8
Ni (lg/L) 27.4 0.8 26.0 0.92 95.3 62.41 0.69 58.68 5.73 94.0
Cu (lg/L) 85.2 1.2 87.2 3.05 102.3 22.76 0.31 20.62 2.06 90.6
Zn (lg/L) 53.2 1.1 51.6 3.72 96.9 78.5 2.2 69.8 4.09 88.9
Se (lg/L) 21.96 0.51 22.10 3.54 100.6 11.97 0.14 11.16 1.08 93.2
Mo (lg/L) 46.75 0.26 45.86 0.57 98.1 121.4 1.3 121.5 1.82 100.0
Cd (lg/L) 22.79 0.96 19.69 1.37 86.4 6.568 0.073 6.30 0.10 95.9
Sn (lg/L)
Sb (lg/L) 13.79 0.42 13.72 1.80 99.5 58.3 0.61 55.5 5.34 95.1
Ba (lg/L) 148 2.2 130 4.62 88.2 544.2 5.8 509.7 43.1 93.6
Pb (lg/L) 27.89 0.14 27.22 1.01 97.6 19.63 0.21 18.81 1.63 95.8
U (lg/L)
 M.M. Rahman et al. / Chemosphere 139 (2015) 5464 57

Table 2
Arsenic and other elements in the groundwater (n = 70) of Noakhali district of Bangladesh.

Elements Detection limit Mean Median Range WHOs guideline Samples exceeding WHO Bangladesh Samples exceeding
of ICP-MS values (lg/L)a guideline value (%) standard (lg/L) Bangladesh standard (%)
As (lg/L) 0.01 297.5 283.5 1.5587.6 10 69 (98.6) 50 68 (97)
Be (lg/L) 0.01 0.02 0.02 <0.010.03 NA NA NA NA
B (lg/L) 0.1 160.4 143.3 11.3388.9 2400 1000
Na (mg/L) 0.05 168.4 155.3 8.3398.8 NA NA 200 23 (32.8)
Mg (mg/L) 0.05 28.8 25.6 4.386.9 NA NA 35 20 (28.5)
K (mg/L) 0.05 10.8 11.1 3.419.7 NA NA 12 26 (37.1)
Ca (mg/L) 0.05 23.5 18.6 5.170.4 NA NA 75
V (lg/L) 0.05 6.5 5.9 1.912.9 NA NA NA NA
Cr (lg/L) 0.03 0.8 0.6 0.195.1 50 NA NA
Mn (lg/L) 0.01 139.6 97 18.9499.5 NA 100 34 (48.5)
Fe (mg/L) 0.01 3.3 2.9 0.059.0 NA NA 1000 68 (97)
Co (lg/L) 0.05 0.4 0.3 0.051.4 NA NA NA NA
Ni (lg/L) 0.1 1.0 0.7 0.31.0 70 100
Cu (lg/L) 0.02 4.5 1.9 <0.02114.2 2000 1000
Zn (lg/L) 0.01 37.4 8.3 <0.01359.5 NA NA 5000
Se (lg/L) 0.2 0.2 0.2 <0.20.25 40 10
Mo (lg/L) 0.05 2.4 2.0 <0.0511.0 NA NA NA
Cd (lg/L) 0.03 <0.03 < 0.03 3 NA NA
Sn (lg/L) 0.03 0.7 0.6 0.032.7 NA NA NA NA
Sb (lg/L) 0.05 0.23 0.09 <0.051.6 20 NA NA
Ba (lg/L) 0.05 6.2 3.9 <0.0528.7 700 NA NA
Pb (lg/L) 0.05 1.1 0.3 <0.057.9 10 NA NA
U (lg/L) 0.01 0.03 0.03 <0.010.07 30 NA NA
Depth (m) 17 16 1233
a
For elements that are of health signicance in drinking-water.

and 37% of 9949 water samples in Deganga had As concentrations
greater than 10 and 50 lg/L, respectively (Rahman et al., 2003). A
previous study also reported that 41% of 5282 water samples from
Jalangi and Domkal blocks had As concentrations greater than
50 lg/L (Rahman et al., 2005).
Fig. 1 shows a comparison of the mean As concentrations
observed in this study and those from other studies conducted in
Cambodia, Vietnam, Indonesia, Bangladesh, and West Bengal. It
appears that the mean As concentration in Noakhali district was
somewhat higher than that in Jalangi and Domkal, somewhat
lower than in Baruipur and much higher than in Dasdia
Nonaghata and Deganga. The mean As concentration in Noakhali
was also much higher than that found in two previous studies con-
ducted from Bangladesh (BGS-DPHE, 2001; Frisbie et al., 2009). The
mean As concentration of Noakhali was somewhat lower than that
of Vinh Tru and Hao Hau areas (depth range 1640 m), Vietnam
(Nguyen et al., 2009), and comparatively higher than in some areas
of Cambodia and Vietnam (depth range 965 m) (Berg et al., 2007;
Buschmann et al., 2007; Nguyen et al., 2009). Arsenic concentra-
tions in groundwater usually vary from region to region based on
regional geology.
3.2. Concentration of other elements in groundwater of Bangladesh
and West Bengal
Apart from As, all other elements measured in the present
study were below the WHO current guideline values in the
groundwater of Noakhali. Only one sample exceeded the previous
WHO guideline value (400 lg/L) for Mn, with a Mn concentration
of 499 lg/L (currently there is no guideline value for Mn). The
standard values of Mn, Fe, Na, K and Mg in drinking water for
Bangladesh are 100 lg/L, 1000 lg/L, 200 mg/L, 35 mg/L and
12 mg/L, respectively. This study shows that 49%, 97%, 33%, 28%
and 37% of the samples from Noakhali had Mn, Fe, Na, K and
Mg levels above the Bangladeshi guideline values, respectively
(Table 2). The concentrations of B, Ni, Cu, Zn and Se did not
exceed the Bangladeshi drinking water standards. Statistical box
plots of As and other elements showing median, 10th, 25th,
75th and 90th percentiles as vertical boxes with error bars from
all study areas are presented in Supplementary Information
(Figs. S15).
Frisbie et al. (2002) reported unsafe levels of Mn, Pb, Ni, and Cr
based on 112 tubewell water samples from Bangladesh. It was fur-
ther reported that the percentages of tubewells that had concen-
trations exceeding the WHO health-based drinking water
guidelines were 78% for Mn (based on the previous guideline
value), 48% for U (current guideline value is 30 lg/L), 1% for Pb,
1% for Ni, and 1% for Cr (Frisbie et al., 2009). Fig. 2 shows the com-
parative bar diagram of mean concentrations of As and other ele-
ments reported in this study and the previous studies (Frisbie
et al., 2009) conducted in Bangladesh. It appears that the mean
concentrations of Mn, Ba, Cr, Ni, Sb and U in the previous study
(Frisbie et al., 2009) of Bangladesh were higher than that in
Noakhali (Fig. 2). The major cation concentrations in a recent sur-
vey of national drinking water quality of Bangladesh (UNICEF,
2011) were lower than in this study. Concentrations of Mn and
Ba were considerably higher in the UNICEF study whereas the con-
centrations of B, Zn, Co were comparable. The concentrations of Mn
and Ba were also much lower in this study than those of Nath et al.
(2011) from the Manikganj district of Bangladesh.
About 81% of the groundwater samples exceeded the previous
WHO guideline value (400 lg/L) of Mn in Jalangi and Domkal,
36% in Dasdia Nonaghata, 81% in Deganga and 88% in Baruipur of
West Bengal. More than 23% of the samples from Baruipur had
Se concentrations greater than the previous WHO guideline value
of 10 lg/L. The groundwater of all studied areas had U levels below
the WHO current guideline value (30 lg/L). The Bureau of Indian
Standard (BIS) Acceptable Limits for Cr, Mn, Fe, Ni, Cu, Zn, Se,
Mo, Cd, Ba and Pb in drinking water are 50 lg/L, 100 lg/L,
300 lg/L, 20 lg/L, 50 lg/L, 5000 lg/L, 10 lg/L, 70 lg/L, 3 lg/L,
700 lg/L and 10 lg/L respectively (Table 3). This study shows that
98%, 90% and 6.5% of the samples from all areas of West Bengal had
Mn, Fe and Se concentrations above the BIS acceptable values,
respectively (Table 3).
Fig. 3 shows a bar diagram comparing the concentrations of As
and other elements observed in this study with the results of a
 58
Table 3
Arsenic and other elements in the groundwater of four As-contaminated districts of West Bengal in India.

Elements Jalangi and Domkal, Murshidabad Haringhata, Nadia (n = 58) Deganga, North 24 Parganas (n = 60) Baruipur, South 24 Parganas (n = 51) BIS valuea B (All areas) n = 232
(n = 63)
Mean Median Range A Mean Median Range A Mean Median Range A Mean Median Range A
As (lg/L) 262.3 196.7 1.11219 98.4 115.8 16.2 0.1692.3 53.4 161.2 152.2 0.2542.8 95 348.9 339.7 51.8692.4 100 10 86.6
Be (lg/L) 0.01 0.01 <0.010.02 NA 0.02 0.02 <0.010.05 NA 0.01 0.02 <0.010.05 NA 0.01 0.01 <0.010.01 NA NA NA
B (lg/L) 28.2 24.0 6.770.5 34.2 26.3 10.7483.8 22.9 22.1 8.940.7 35.9 35.1 24.883.3 500

M.M. Rahman et al. / Chemosphere 139 (2015) 5464

Na (mg/L) 26.2 22.4 10.264.6 NA 29.9 25.4 2.929.2 NA 17.4 15485 7.564.0 NA 26.5 22.1 13.172.0 NA NA NA
Mg (mg/L) 33.2 30.8 12.872.5 NA 25.4 24.1 3.449.2 NA 22.4 22.1 9.936.4 NA 27.8 27.1 20.140.5 NA 30 28.4
K (mg/L) 6.4 4.9 2.936.9 NA 2.4 2.2 0.44.0 NA 3.2 3.1 2.05.0 NA 3.9 3.5 2.79.4 NA NA NA
Ca (mg/L) 121.4 114.3 60.8228.8 NA 95.6 86.4 12.5198.5 NA 100.4 95.5 62.8253.7 NA 112.5 110.5 83.8157.0 NA 75 95.6
V (lg/L) 0.5 0.1 <0.056.3 NA 0.9 0.7 <0.054.2 NA 0.1 0.1 0.050.65 NA 0.1 0.1 0.050.5 NA NA NA
Cr (lg/L) 0.4 0.4 0.11.0 0.4 0.3 <0.031.6 0.4 0.4 0.21.3 0.2 0.2 <0.030.9 50
Mn (lg/L) 807.9 871.0 87.11408 341.5 341.5 25.1814 579 524 881538 584 571 160860 100 97.4
Fe (mg/L) 3.9 1.9 0.0616.5 NA 3.4 1.6 0.0718.5 3.9 3.3 0.315.4 NA 4.2 2.6 0.415.0 NA 300 90.1
Co (lg/L) 0.3 0.2 <0.051.4 NA 0.3 0.3 <0.050.6 NA 0.3 0.2 <0.051.1 NA 0.4 0.4 0.11.6 NA NA NA
Ni (lg/L) 0.4 0.2 <0.11.6 0.6 0.6 <0.11.6 0.4 0.3 <0.11.2 0.7 0.7 0.41.2 20
Cu (lg/L) 2.7 0.7 <0.0237.8 0.9 0.5 <0.026.3 0.9 0.4 <0.025.6 3.6 1.5 <0.0214.3 50
Zn (lg/L) 33.5 5.6 <0.01488 NA 128.6 14.1 <0.012386 NA 109.8 37.0 2999 NA 16.1 5.3 0.5117.6 NA 5000
Se (lg/L) 1.5 1.0 <0.24.9 2.8 2.9 <0.27.0 1.9 1.8 <0.25.1 9.6 8.9 1.317.5 10 6.5
Mo (lg/L) 2.6 2.1 <0.059.4 1.1 0.9 <0.053.8 1.438 1.3 0.24.2 2.8 2.7 0.85.0 70
Cd (lg/L) <0.03 < 0.03 0.08 0.07 <0.030.2 0.1 0.1 <0.030.3 0.05 0.04 <0.030.08 3
Sn (lg/L) 0.26 0.1 <0.030.9 NA 0.3 0.3 <0.030.4 NA 0.2 0.1 <0.030.8 NA 0.1 0.1 <0.030.2 NA NA NA
Sb (lg/L) 0.07 0.07 <0.050.7 0.1 0.1 <0.050.6 0.1 0.1 <0.050.2 0.1 0.06 <0.050.3 NA NA
Ba (lg/L) 309.7 299.0 143.2523.7 206.8 183.6 51.4494.5 201.8 186.6 114.7343.6 225.1 221.3 152323 700
Pb (lg/L) 0.6 0.4 <0.052.7 0.9 0.7 0.17.2 0.2 0.1 0.051.8 0.2 0.1 0.051.2 10
U (lg/L) 1.5 0.3 <0.0113.9 1.5 1.1 <0.015.6 0.2 0.1 <0.010.8 0.2 0.2 <0.010.8 NA
Depth (m) 23 21 2361 40 42 1876 27 26 2045 28 26 1461 1476

A Percentage of samples exceeding the WHO guideline value.

B Percentage of samples exceeding the BIS acceptable values.
a
Bureau of Indian Standard (BIS 2009).
 M.M. Rahman et al. / Chemosphere 139 (2015) 5464 59

Fig. 1. Comparative mean As concentrations (lg/L) in groundwater observed in this study with other studies conducted from Cambodia, Vietnam, Indonesia, Bangladesh and
West Bengal of India.

Fig. 2. Comparative bar diagram of mean concentration of As and other elements (lg/L) in groundwater observed in this study with previous study (Frisbie et al., 2009)
conducted from Bangladesh.

previous study conducted in Jalangi and Domkal (Roychowdhury
et al., 2003). The mean As concentrations in Jalangi and Domkal
(262 lg/L) were much higher than those found in a previous study
conducted in Jalangi (133 lg/L) and Domkal (100 lg/L)
(Roychowdhury et al., 2003). The mean As concentrations in
Deganga (161 lg/L) and Baruipur (349 lg/L) were also higher
those found in the study of Jalangi and Domkal (Roychowdhury
et al., 2003) but comparable with Dasdia Nonaghata (116 lg/L).
The Mn concentrations groundwater samples from Deganga and
Baruipur were comparable with the results of the Jalangi study
(Roychowdhury et al., 2003). The mean Ni concentrations of all
four areas were much lower in this study compared to the previous
study in Jalangi and Domkal (Roychowdhury et al., 2003). The Cu
concentrations of Jalangi and Domkal groundwater were compara-
ble with those found in the previous study in Jalangi and Domkal
(Roychowdhury et al., 2003). The Se concentrations in Baruipur
and the Zn concentrations in Deganga and Dasdia Nonaghata were
much higher compared to other areas of West Bengal. The average
concentrations of major cations (Na, K, Mg and Ca), Mn, Ba, Co and
Mo were comparable with those of Nath et al. (2011).
60 M.M. Rahman et al. / Chemosphere 139 (2015) 5464
Concentrations of Fe and Zn were almost 2-fold higher in the study
of Nath et al. (2011).
About 67%, 80%, and 86% of groundwater samples from the
Kandal Province of Cambodia contained concentrations of Ba, Mn,
and Pb, respectively, that were higher than the WHO drinking
water guideline values (Luu et al., 2009). Fig. 4 illustrates the com-
parison between the mean concentrations of Mn, Pb, and Ba
observed in Bangladesh, West Bengal, Vietnam, and Cambodia,
and the results of this study. It appears that the mean Mn concen-
trations of groundwater from the Mekong Delta, Vietnam, and
Southern Vietnam were much higher than found in other studies.
The Pb concentration in groundwater from Vietnam was
non-detectable but a low concentration of Pb was detected in this
study. The Ba concentrations of most studies were below the WHO
guideline value except in three areas of Vietnam.
This study reveals that the distribution of major ions such as Ca
(5.1253 mg/L), Mg (3.387 mg/L), Na (3.1399 mg/L), and K (<1
37 mg/L) show signicant variations and this is similar to that
reported by Bhattacharya et al. (2002) who also reported signi-
cant variations.
The calculated SI of various mineral phases in groundwater of
all studied areas is presented in Table I of the Supplementary
Information. The values of SI (positive and negative) indicate the
thermodynamic potential for precipitation and dissolution, respec-
tively (Bhowmick et al., 2013). The SI calculations reveal that most
of the Fe-oxide/hydroxide (FeIII) minerals are saturated (i.e. posi-
tive values) in groundwater in all study areas. Similar observations
were also reported by Bhowmick et al. (2013) in groundwater of
West Bengal, India. The negative SI values indicate that the As min-
erals are under-saturated. Overall the SI values imply geochemical
condition suitable for the presence of As in solution.
3.3. Concentrations of other elements in tubewells with As greater than
10 lg/L
We found only one groundwater sample with an As concentra-
tion exceeding 10 lg/L in Noakhali where the Mn concentrations
also exceeded the previous WHO guideline value. The mean con-
centration of As in groundwater samples from Noakhali was
Fig. 3. Comparative bar diagram of mean concentration of As and other elements (lg/L) observed in groundwater from 4 districts of West Bengal in this study with previous
study (Roychowdhury et al., 2003) conducted from Murshidabad district of West Bengal.
301 lg/L. Of the 61 samples with As concentrations exceeding
10 lg/L from Jalangi and Domkal, 84% of the samples had Mn con-
centrations (mean: 818 lg/L), greater than the previous WHO
guideline value. In Dasdia Nonaghata village, 22.6% of the 31 sam-
ples with As concentrations greater than 10 lg/L had Mn (mean:
632 lg/L), and from Deganga the corresponding value was 86%
(mean Mn: 601 lg/L). About 88% and 25% of 51 samples from
Baruipur with As greater than 10 lg/L had Mn (mean: 584 lg/L)
and Se (mean: 10 lg/L) levels greater than the previous WHO
guideline values, respectively.
3.4. Concentrations of other elements in tubewells with As levels below
10 lg/L
We detected an As concentration below 10 lg/L in only one sam-
ple from both Noakhali and Jalangi and Domkal areas, and all other
elements of that sample were below the respective WHO guideline
values. The mean concentration of As in groundwater samples from
Dasdia Nonaghata with As concentrations below 10 lg/L was
0.79 lg/L (the detection limit of As in the ICPMS instrument was
0.01 lg/L). In Deganga, of 3 samples with As levels below 10 lg/L,
none of the elements exceeded the WHO guideline values. In
Dasdia Nonaghata, out of 27 samples with As levels below
10 lg/L, 52% of samples had Mn (mean: 455 lg/L) levels greater
than the previous WHO recommended value. This study suggests
that concentrations of other elements in groundwater with As levels
below 10 lg/L did not exceed the previous WHO guideline values,
although Mn concentrations were higher in groundwater of all stud-
ied areas, and exceeded the previous WHO guideline value
(400 lg/L). Therefore even if groundwater samples are safe with
respect to As they should be further checked for other elements
before they are recommended as safe for public drinking water.
3.5. Relationship between As and other elements
The relationships between As and other elements in all ground-
water samples analyzed from Bangladesh and West Bengal are pre-
sented in Table II of the Supplementary Information. Signicant
correlations (p < 0.01) were observed between As and Se, Mo, and
 M.M. Rahman et al. / Chemosphere 139 (2015) 5464
Fig. 4. Comparative mean concentrations (lg/L) of Mn, Pb, Ba observed in groundwater from Cambodia, Vietnam, Indonesia, Bangladesh and West Bengal.
Sn in the groundwater. We also observed signicant correlation
between As and Fe (0.21, p < 0.05). The correlation between As
and Mn in groundwater was poor. Previous study found correla-
tions between As and Fe from both Bangladesh (0.49) and West
Bengal (0.2), but no correlation was observed for As vs Mn
(Maity et al., 2011).
A backward elimination procedure was used to produce the
subset of predictors listed in Table III of the Supplementary
Information. Two of the predictors (Co and U) had 87 and 89 values
below detection and Mo had 3 values below detection. For that
model R2 = 0.489, multiple R = 0.699, with an adjusted R2 of 0.475
(adjusted multiple R = 0.689), the largest contribution was from
Mo this also had the highest Pearsons correlation (0.544) with
As. The relatively low R2 value indicates that the linear model
across the whole data set is not a good t.
3.6. Consumption of As and other elements from drinking water by
adults
The daily consumption of As and other elements from drinking
water by adults was calculated by using the following equation:
DCE CRD  CED
where DCE = Daily consumption of elements (lg), CRD = Mean con-
sumption rate of drinking water (L) and CED = Mean concentrations
of elements observed in drinking water (lg/L).
61
Our previous study shows that the mean and median water
intake rates for drinking were 2.9 L and 3.0 L per day, respectively,
for adults (n = 71) from Noakhali district of Bangladesh (Rahman
et al., 2011). The average water intake was 3.5 L for adults
(n = 640) from Natore district of Bangladesh (Milton et al., 2006),
which is higher than this study. Ahsan et al. (2006) reported that
the mean water intake rate was 3.0 L for adults (n = 11,746) from
a large population based study conducted from Araihazar Thana
of Bangladesh, which is similar to this study. Recently Hossain
et al. (2013) estimated the daily water intake from three
As-affected villages of West Bengal, and reported that the mean
daily water intake was 3.1 for adults (n = 423) and this value is
used to estimate As intake from water for all four areas of West
Bengal.
The daily intake of As and other elements from drinking water
in all study areas for adults is presented in Table 4. Besides As,
the daily consumption of B and Mn from drinking water were also
much higher for adults in Noakhali. The daily intake of Mn and Ba
in all four areas of West Bengal were signicantly higher than
Noakhali. The comparative daily total consumption of As, Mn, B
and Ba from drinking water for adults of all studied areas is pre-
sented in Fig. 5. It appears that adults consume considerable
amounts of As and Mn in the studied areas. It should be also noted
that many people are currently aware of the risk of drinking As
contaminated water and many of them are currently drinking
water from tubewells that are safe (As < 10 lg/L) due to the
62 M.M. Rahman et al. / Chemosphere 139 (2015) 5464

mitigation activities carried out by both government and other aid
agencies in both Bangladesh and West Bengal.
3.7. Risk
As shown in Tables 2 and 3, while the measured concentrations
for most elements are below than the WHO guideline value, the
concentrations for As value are even 20 times than the suggested
value. Considered the potential cancer risk to using groundwater
as drinking water in the objective area, the cancer probability for
As is calculated as per the equation below (Ma et al., 2012).
X
5000
Ri 1=5000  C ij  kj
j1
where the subscript i represents the sampling regions, C * j is the
average concentration of As in groundwater that was estimated
by the bootstrap method (Matlab, 2012), j is the sampling times
in the bootstrap method, and kj is the random number that sam-
pling from the distribution for cancer slope of Arsenic for drinking
water. The cancer slope (5E05 per lg/L, with the range of 3E05
per lg/L to 7E05 per lg/L) was recommended by U.S. EPA were
used in this study (IRIS, 2007). In this study, a normal distribution
was assumed for the cancer slope, and 95% CI was estimated as
the same range provided by U.S. EPA (U.S. EPA, 1988). Thus, the
mean and standard deviation was estimated to be 5E105 per
lg/L and 1.03E105 per lg/L, respectively. The C and K represent
the variability and uncertainty in this study, respectively. The aim
of these treatments was to integrate both the variability and uncer-
tainty (Bogen and Spear, 1987; Siirila et al., 2012). Considering the
variability for the exposure population (Fig. 6), the estimated cancer
risks for Noakhali, Murshidabad, Nadia, Degenga, Baruipur were
1.49% (95% condential interval (CI): 1.351.63%), 1.31% (95% CI:
1.051.62%), 0.58% (95% CI: 0.350.83%), 0.81% (95% CI: 0.67
0.96%), 1.74% (95% CI: 1.551.94%), respectively. The mean risk
was 5801740 times higher than a cancer risk of 105, which is
the default acceptable level (Benner, 2004). When plus the uncer-
tainties, the 95% CI for the ve regions were estimated to be
0.902.10%, 0.741.94%, 0.290.96%, 0.451.19%, and 1.032.49%.
The estimated risk presented here indicated a terrible high cancer
risk due to the As exposure in this region, and the standard devia-
tions ratio between variability and uncertainty were estimated to
be 0.231.17.
In this study, the non-carcinogenic risk was also estimated. The
value of 3E4 mg/kg was recommended as reference dose (IRIS,
2007). Using the re-sampling method as described in the estima-
tion for carcinogenic risk, the hazard quotients were estimated to
be 28.38 (95% CI: 25.7131.05), 24.95 (95% CI: 20.0030.85),
11.05 (95% CI: 6.6715.81), 15.43 (95% CI: 12.7618.29), 33.14
(95% CI: 29.5336.95) for Noakhali, Murshidabad, Nadia,
Degenga, Baruipur, respectively (water consumption of 2 L and
body weight of 70 kg were assumed for adult). All the hazard quo-
tients were much higher than 1, which mean all the exposure were
higher than the reference dose.
4. Conclusions and recommendations
This study demonstrates that none of the examined elements
except As exceeded the current WHO guideline values, although
the concentrations of Mn and Fe in drinking water of Bangladesh
and West Bengal exceed both Bangladeshi and Indian BIS values.
Many elements do not have guideline values set by WHO and other
national agencies. People ingesting groundwater, whether for
drinking or for cooking are also exposed to high concentrations
of Mn, Ba and B in Bangladesh and West Bengal. The concentra-
tions of Se and Sb are generally low in groundwater samples ana-
lyzed in this study from both Bangladesh and West Bengal,
although 6.5% samples in West Bengal exceed the BIS value.
Recently 19%, 6% and 31% of the groundwater samples from
Bongaon of West Bengal were detected with signicant concentra-
tions of Mn, B and Th, respectively (Bacquart et al., 2012).
Hexavalent chromium (Cr[VI]) (927,400 lg/L), and cyanide

Table 4
Daily intake of As and other elements from drinking water.

Elements Average Average Daily Average Average Daily Average Daily Average Daily Average Daily
water intake conc. intake water intake conc. intake conc. intake conc. intake conc. intake
(L) (lg/L) (lg) (L) (lg/L) (lg) (lg/L) (lg) (lg/L) (lg) (lg/L) (lg)
Bangladesh West Bengal
Noakhali Jalangi and Domkal Haringhata Deganga Baruipur
As 2.9 297.5 862.7 3.1 262.3 813.1 115.8 358.9 161.2 499.7 348.9 1081
Be 0.02 0.06 0.01 0.03 0.02 0.06 0.01 0.03 0.01 0.03
B 160.4 465.1 28.2 87.42 34.2 106.0 22.9 70.99 35.9 111.2
Naa 168.4 488.3 26.2 81.22 29.9 92.69 17.4 53.94 26.5 82.15
Mga 28.8 83.52 33.2 102.9 25.4 78.74 22.4 69.44 27.8 86.18
Ka 10.8 31.32 6.4 19.84 2.4 7.44 3.2 9.92 3.9 12.09
Caa 23.5 68.15 121.4 376.3 95.6 296.3 100.4 311.2 112.5 348.7
V 6.5 18.85 0.5 1.55 0.9 2.79 0.1 0.31 0.1 0.31
Cr 0.8 2.32 0.4 1.24 0.4 1.24 0.4 1.24 0.2 0.62
Mn 139.6 404.8 807.9 2504 341.5 1058 579 1794 584 1810
Fea 3.3 9.57 3.9 12.09 3.4 10.54 3.9 12.09 4.2 13.02
Co 0.4 1.16 0.3 0.93 0.3 0.93 0.3 0.93 0.4 1.24
Ni 1.0 2.90 0.4 1.24 0.6 1.86 0.4 1.24 0.7 2.17
Cu 4.5 13.05 2.7 8.37 0.9 2.79 0.9 2.79 3.6 11.16
Zn 37.4 108.4 33.5 103.8 128.6 398.6 109.8 340.3 16.1 49.91
Se 0.2 0.58 1.5 4.65 2.8 8.68 1.9 5.89 9.6 29.76
Mo 2.4 6.96 2.6 8.06 1.1 3.41 1.438 4.46 2.8 8.68
Cd 0.00 0.08 0.25 0.1 0.31 0.05 0.16
Sn 0.7 2.03 0.26 0.81 0.3 0.93 0.2 0.62 0.1 0.31
Sb 0.23 0.67 0.07 0.22 0.1 0.31 0.1 0.31 0.1 0.31
Ba 6.2 17.98 309.7 960.1 206.8 641.1 201.8 625.5 225.1 697.8
Pb 1.1 3.19 0.6 1.86 0.9 2.79 0.2 0.62 0.2 0.62
U 0.03 0.09 1.5 4.65 1.5 4.65 0.2 0.62 0.2 0.62
a
Concentration unit expressed as mg/L and intake expressed as mg.
 M.M. Rahman et al. / Chemosphere 139 (2015) 5464
Fig. 5. Comparative daily total consumption of As, Mn, B and Ba from drinking water for adults of all studied areas of Bangladesh and West Bengal.
(310,000 lg/L) were found in groundwater of the industrial city of
Ludhiana, Punjab (Chaudhary et al., 2001). Ghosh et al. (2004)
reported that carcinogenic alpha (4He2+) emitting radionuclides
have been found in the range of 39220 Bq/L (global average,
10 Bq/L) in As-contaminated tubewell water from two districts of
West Bengal.
Although none of the elements except As exceeded the WHO
guideline values, the maximum concentrations (worst case scenar-
io) is always an issue, which needs proper attention. The ground-
water of other contaminated districts of Bangladesh and West
Bengal need to be tested to get a clear picture of elements present
in the groundwater. Besides As, elements such as Mn, U, Se, Pb, Ni,
Ba, B and Cr need to be tested before using the groundwater for
drinking and cooking purposes. Mitigation options should not be
limited to As alone; the health risks from other elements present
in groundwater also need to be considered, although the major
health concern is currently due to As in drinking water. Water
treatment plants to purify drinking water should be designed to
remove not only As but also other elements to achieve satisfactory
drinking water quality. The huge amount of available surface water
and rainwater harvested should be used for drinking purposes after
proper treatment to avoid possible hazards from As and other ele-
ments present in groundwater.
Fig. 6. The estimated cancer risk for As exposure in different regions. On each box,
the central mark is the median, the edges of the box are the 25th and 75th
percentiles, the whiskers extend to the most extreme data points not considered
outliers, and outliers are not plotted.
63
Acknowledgements
We extend our sincere thanks to Dr. Dipankar Chakraborti,
School of Environmental Studies (SOES), Jadavpur University,
Kolkata, India for providing us with groundwater samples from
West Bengal. The authors also thank CERAR for laboratory support.
We also thank Mr. Md. Asaduzzman for his help during sampling in
Noakhali. M.M. Rahman is grateful to the University of South
Australia for the nancial support under the Early Career
Researcher (ECR) Travel Grant Scheme to travel to Kolkata, India,
to carry out academic research in SOES, Jadavpur University, for a
month. We would like to extend our heartfelt thanks to Dr. Ray
Correll of CERAR for supporting with statistical analysis.
Appendix A. Supplementary material
Supplementary data associated with this article can be found, in
the online version, at http://dx.doi.org/10.1016/j.chemosphere.
2015.05.051.
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