ISBN 979-3234-11-5

Arsenic pollution of groundwater in Bangladesh based on the analytical

results of groundwater and soils in Samta and Marua villages,
Jessore district
Kimiko Tanabe
Lecturer, Miyazaki University,
Gakuen Kibanadai, Miyazaki, 880-2192, Japan
m00002u@cc.miyazaki-u.ac.jp
YuKo Toguchida1, Kazuto Kudo1, Kazuhiro Hamabe1,
Hiroshi Yokota1, AAN2, and RGAG3
1. Miyazaki University, 2 Asia Arsenic Network, Miyazaki, Japan
3 Research Group for Applied Geology, Sub-group for Arsenic Contamination, Japan

ABSTRACT
In Bangladesh, where most people are supplied from the groundwater for drinking,
about 40 million people are currently exposed to the risk of arsenic poisoning. We have
carried out the investigation for elucidation of arsenic elution mechanism in the
groundwater at the two model villages, namely Samta and Marua, in Bangladesh at 9 times
since March 1997. Here, we compare the characteristics of arsenic pollution between the
two villages on the arsenic elution mechanism to the groundwater.
These results show that (1) the arsenic is mainly included in the organic substance of
soil, (2) the arsenic concentration in groundwater is closely related to the muddy layers
distribution, and (3) arsenic elution to groundwater is caused in the reduced state.

Key word : Bangladesh, arsenic pollution, elution mechanism , reduced state, water quality

1. INTRODUCTION
Arsenic pollution of the groundwater in Bangladesh is confirmed at 61 in 64 districts
(British Geology Survey, 2001) and this fact is widely known. But, the actual condition has not
been proven yet. Arsenic exists mainly with the iron mineral metallurgy and genus arsenate
in colliery and mine. In Bangladesh, from the size of extent of the pollution, the arsenic
origin seems to be the sediment carried by Ganges and Brahmaputra rivers. On the basis of
the investigation of the Ganges basin,
Chakraborty et al reported that arsenic elution
occur in oxidation state (Das, D., 1996 and
Chakraborti.D.,2000), meanwhile Nickson et
al.(2000) reported with that it occur in the
reduced state. However, arsenic elution
mechanism to the groundwater has not been
elucidated in the Ganges basin. Therefore, we
examined the arsenic elution to the
groundwater from the viewpoint of the water
quality survey in the two villages, Samta and Fig.1. Location of Samta village and
Marua villages, located at Jessor district, Marua village in Jessore, Bangladesh.
Bangladesh, where the arsenic pollution has
caused serious problems.

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2. RESEARCH AREAS AND METHOD OF ANALYSIS

2.1 Research areas

Research was carried out in Samta village from March, 1997 to January, 2003 at 9 times
and in Marua village in January, 2002 and January, 2003 as shown Fig.1.

2.2 Analysis (m )

Values of pH (Horiba U-10) and N

oxidation -reduction potential
(ORP, Toa Denpa PHL-10) were
determined by glass electrode 0 .0 2

method. Electron conductivity 0 .0 6

(EC) were determined by water 0 .0 1

quality checker (Horiba U-10).

As (mg/l)
As 0.01
%
3.5
0 .0 3
0 .0 2

Arsenic concentration was 0.01 As<0.05 4.6

0.05 As<0.1 18.1
quantified by atomic absorption 0.1 As<0.3 36.5
spectrometry (Shimadzu AA-
0 .2 5
R i c e F i e ld 0.3 As<0.5. 21.6 m g /l
05 As 15.7 D e e p T u b e w e l l fo r I r r i g a t i o n

6650) with arsenic speciation D e e p T u b e w e ll f o r D r in k in g

Fig.2. Distribution of arsenic concentration in

pretreatment system
(m )

groundwater in Samta village on March 1997.

(Shimadzu ASA-2SP) and
HPLC (Shimadzu LC 10AD ) - ICP/MS (Hull Packard HP 4500). Total iron and Fe2+ were
quantified by phenanthroline absorption spectrophotometry (Beckmann DU-650). HCO 3-
was quantified by separation titration method. Ca 2+ and Mg2+ were quantified by flame
atomic absorption spectrometry (Hitachi Z-800). Ion chromatography (Dionex DX-120)
was used for NH4+ and SO42-. PO43- was quantified by amino acid method. Arseniccontent
in drilling core Sample was analyzed by the method prescribed by the Japanese
Government Environmental Agency.

3. RESULTS AND DISCUSSION

3.1 Samta village

We analyzed the arsenic concentration in all tubewells (n=282) for drinking in
Samta village in March
1997. The result is shown in Fig.2.
sN`Kv
QuickTime
Graphics LvO TheB figure shows that tubewells
-1
with arsenic concentration of less than 0.01mgl (the guideline set by the World Health
1.8 J
B 26A11 28A11
1.6
Arsenic concentration (mg/l)

J 27A16 28B28
1.4 Flood
1.2 H 27B 1 29B 9 S ep.,2000
1 F 27B34 30A19 F
J
0.8 3 28A 5 3
J

0.6 B 3
JB
H
B
F
3


J J
H F

B
H



0.4 H

F F


J


0.2 B
H
3
B
F B
H

F
H
B
H
F


H
3

F
3

0 3
Mar.97 Oct.97 May.98 May.99 Nov.99 May.00 Mar.01 Jan.02 Jan.03
Fig.3. Time course plot of arsenic concentration of groundwater in Samta.

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As(mg/kg)
As(mg/kg) As(mg/kg) As(mg/kg)
0 0.1 1
10 1020 100 30 0 10 20 30
0 10 20 30

Organization) were only 3.5% of the 0 0

total and those within the limit (0.05

mgl-1) in Bangladesh were 5 5
approximately 8%. Moreover 15% of
the tubewells contained arsenic does
10 10
greater than 0.5 mgl-1 and the highest
value was as 1.4 mgl-1. High
concentration of arsenic found in the 15 15

south part of the village, and the

concentration tended to be lower 20 20

towards the north. Fig.3 shows the

change of arsenic concentration in 25 25
Samta village with the passage of time.
The background of gray shows rainy
season (October 1997 and November 30 30

1999), and the others show dry season.

From this figure, arsenic concentration 35 35

tend to increase and it varied among

seasons. But after the flood occurred 40 40
(September, 2000), the arsenic
concentration in tubewell water was 44 44
lowered. We suggest that the result 0 10 20 0 10 20
shows relation on the arsenic As (mg/kg) As (mg/kg)
concentration in the groundwater with a : Samta b : Marua
the subterranean stream. It was proven Fig.4. The geological histogram and arsenic
content of boringcore. a: OBS-5 point
that the groundwater level in Samta inSamta village, b: M-7 point in Marua village
changed within 3-6 m between the dry
and rainy seasons (Kosaka,A., 1999). : Upper muddy Layer
From an analytic result of drilling cores : Sand Layer
: Muddy Layer
showed in Fig.4.a, it was known that the
top stratum in Samta consists of the clay layer about 10 m deepth following the sand layer
and that the peat in the clay layer contains rich arsenic (Ishiga,H., 2002). It is possible to
assume that arsenic concentrations in groundwater in the rainy season become higher than
in the dry season due to the arsenic in the clay layer easily leaches out in the rainy season in
which the water table rised. Moreover, it denotes that the flow of groundwater become
stronger at some areas (Bando,K., 1998), and it is highly conceivable that arsenic is
transported by the flow of groundwater. From Fig. 3, it is also noted that arsenic
concentrations of groundwater tend to increase with the passage of time.
The results of the quality of tubewell water conducted in May 1998 are shown in Table
1. The pH was from 7.1 to 7.6, showing weak alkalescence, and the ORP values were
almost negative, showing a reduced state. The concentration of HCO 3- and iron were 179-
432 mgl-1 and 3.9-10.5 mgl-1 respectively, much higher than those of normal groundwater,
and whereas the concentration of SO42- were within the range 0-7.9 mgl-1, with most of the
samples were below 2.0 mgl-1, which can be estimated very low.
The arsenic can be at trivalent or pentavalent in the water. Fig.5 shows arsenic
concentration and proportion of As3+ and As5+ in groundwater of Samta. As5+ concentration
in groundwater was higher than that of As3+ in north of Samta. But in the south, As 3+

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concentration was higher than that of As5+, and Table 1 Water quality of groundwater in
arsenic concentration was high there. Fig.6 Samta Village on May 1998
Drinking Irrigation Drinking
shows the relationship between groundwater Items
(30-50m) (100m) (200m)
3+
quality and proportion of As for total As pH 7.1-7.6 7.2-7.3 7.5-7.6
(As3+ + As5+). There was a tendency that the EC (s/cm) 574-1192 806-1228 968-1373
point with a high proportion of As3+ have ORP (mv) -88 - -6 -52 - -3 -50 - 3
2+
higher concentration of arsenic, SiO2, Fe and As 3+,5+
(mgl -1
) 0.03-1.2 0.03-0.2 0.05-0.08
2+ -1
HCO3- and also higher EC and ORP values. Fe 3+ (mgl-1 ) 3.9-10.5 4.2-6.3 1.1-1.4
On the contrary, the place with high proportion Fe (mgl -
)
-1
0-1.0 0+0.6 0
HCO (mgl ) 179-432 340-358 381-392
of As5+ showed high concentration of NH4+ NH 3+(mgl-1) 0.1-8.4 3.0-8.1 0.5-2.0
4
and SO42- and high value of pH. On this fact, it K+(mgl-1) 2.1-14.7 3.1-10.9 5.1-15.8
is proposed that the groundwater is an Mg2+(mgl-1) 13-48 27-34 36-47
oxidation state, because fertilizer and oxygen Ca2+(mgl-1) 51-100 49-57 40-43
- -1
from the ground to the underground are taken F (mgl ) 0-4.4 0-1.3 1.0-2.4
in north in the village. The contour lines in Cl-(mgl-1) 0-58.3 4.0-14.3 26.5-48.4
Br-(mgl-1) 0-0.10 0-0.02 0.05-0.15
Fig.5 are distribution of thickness of the upper
NO3-(mgl-1) 0-0.40 0.01-0.08 0.03-0.05
muddy layer in the village. The thickness is SO42-(mgl-1) 0-7.9 0.1-0.3 0.2-0.5
variable among the places, for example,
thickness in the rice field in the northern area
(arsenic concentration of adjacent tubewells was 0-0.02 mgl-1) is 0 - 1 m, in northern part
( area with low arsenic concentration) is 1-3 m, in the middle area (arsenic concentration of
adjacent tubewells 0.3 mgl-1) is 6-12 m, in the southern area (where has high arsenic
concentration) is 4-6m and in the southern rice field is 3-4 m. We think that the thickness of
upper muddy layer is strongly related to the arsenic concentration in groundwater, because
the distribution of the upper muddy layer resembles the distribution of the arsenic
concentration.
It has been proven that the arsenic is included mainly the peat in upper muddy layer.
We have clarified that geology stratigraphy (Bando, K. 1998) of the Samta village consist
of most upper sand layer, upper muddy layer, upper sand layer (first aquifer), lower muddy
layer and lower sand layer
0m 0m
(second aquifer) . The water of

N

tubewells in Samta for

3m
drinking is taken from first 6m
aquifer. 8m 3+ 5+
As /As ratio(%)
13/87
100/0 0/0100 5/95
3.2 Marua village 100/0
100/0 100/0 3m

In January, 2002, we 99/1

analyzed the water taken from 100/0 6m
98/2
all tubewells (273), which is 100/0 3m As (mg/l)
used for drinking in Marua As 0.01
village (Fig.7). The figure 0.01 As<0.05.
shows that tubewells with 0.05 As<0.3
arsenic concentration of less 0 500 1 0 0 0 (m ) 0.3 As<0.5.
than 0.05mgl-1 were 36% of 05 As
the total and 6% of the
Fig.5 Distribution of upper muddy layer and arsenic
tubewells contained more than
concentration and propotion of As3+ and As5+ in groundwater in
0.5 mgl-1. Average arsenic Samta.

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100
90
80
70
60
50
40
30
20
10
0
7.1 7.2 7.3 7.4 -70-60-50-40-30-20-10
7.5 600
0 800 1000 1200
15 16 17 18 19 20 21 22
S iO (mg/l)
pH ORP(mV) EC(S /cm) 2

100
90
80
70
60
50
40
30
20
10
0
3 4 5 6 7 8 9 10 0 1 2 3 4 5 6 7 8 09 0.4 0.8 1.2 200 1.6 250 300 350
2+
Fe (mg/l) +
NH4 (mg/l)
2
S O 4 (mg/l) HCO3-(mg/l)
Fig.6.. Relationship between groundwater quality and proportion of As to total As(As3+ + As5+).
3+

concentration of the village is 0.13 mgl-1, but the arsenic concentration in the eastern area
in the village (east pala) was low (average 0.04 mgl-1.) and western area (west pala) was
high (average 0.17 mgl-1.). The well depth is 72ft (22m) in east pala, and 106ft (32m) in
west pala. From the result of the geological survey, the upper muddy layer was not found in
the east pala, and the muddy layer and sand layer are overlapped multiply in west pala. As
the result, in the west pala, the well depth is much deeper, and it seems to take water from
the different aquifer.
Table 2 shows that the groundwater quality in Marua village(December, 2002). From
the result of the water analysis, the groundwater in the Marua village was almost neutrality,
and ORP showed the negative value, then the groundwater was reduced state. In
comparison with usual groundwater, EC, HCO3-, NH4+and total iron were higher. On the
other hand, NO3- and NO2- were not entirely detected. The relation between arsenic
concentration and other water quality item could not be found as in those from the Samta
village. For this reason, we think that the tubewells in Samta village are identical aquifer,
and Marua are different aquifer. Arsenic content in the boring core in Marua village was
high in muddy layer (Fig.4.b). This accorded with the results of Samta village.

3.3 Arsenic elution to groundwater

The causes of natural leaching out of arsenic to groundwater are indicated to be due to
oxidation or reduction states of the underground. The oxidation theory suggests that the
arsenic elution to groundwater is generated, when the minerals such as pyrite and
arsenopyrite including the arsenic is oxidized. The reduction theory is proposed that iron
oxyhydroxide (FeOOH) trapping arsenic is dissolved under reductive environment and

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Fig.. Distribution of arsenic concentration in groundwater in Marua village on

January 2002.

arsenic is then released in water when Fe3+ turn into Fe2+.

We discuss about the arsenic elution to groundwater using the survey result of Samta.
From Fig.5 and Fig.6, it demonstrate that the arsenic existed almost at trivalent with high
arsenic concentration area, where is also contains high concentration of iron (almost Fe 2+)
and HCO3-, and EC. In soil on the reduced state, HCO3- can be produced when carbon in
deposited organic matter is oxidized by microorganisms in the absence of oxygen or when
SO42- is reduced by organic matter. The reaction that carbon in organic matter is oxidized by
bacteria could be easier to occur than the production of HCO 3- due to oxidation of pyrite
(Nickson, 2000). For this reason, the high concentration of HCO 3- in groundwater in Samta
could be mostly produced under reduced state. HCO3- concentration in groundwater was
also high in Marua. Iron concentration was high and was almost Fe2+, in Samta and Marua.
And Fe2+ concentration in groundwater was high in the place where the arsenic
concentration was high in Samta. Arsenic was almost the trivalent in the groundwater on
the south in the village of which the arsenic concentration is high. However in the north,
pentavalent arsenic was higher than that of trivalent. It is considered that in Samta, the
groundwater in the north is in oxidation state and the groundwater in the south is in reduced
state. It has been reported that from the investigation of the groundwater level, the
groundwater in the Samta village flow from the north in the village to the south, and that
stays temporarily in the place, where the arsenic concentration is high, and then it is flowed
to the east. Generally, accumulating groundwater is a reduced state. The EC value of the
groundwater is high in this accumulated place. Therefore, many dissolved components
would accumulate in this place. And, from Fig. 5, it is specifies that the thickness of the
upper muddy layer with high contained arsenic is closely related to the arsenic
concentration in groundwater.
From the boring core of the Samta, though the framboidal pyrite with the arsenic was
found, it seemed too little for to explain the high concentration arsenic in the groundwater.

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From the result of water analysis and this fact, we think that the arsenic elution from the
oxidation state is difficult.
We cannot conclude the arsenic elution to groundwater by water quality in Marua village,
because the aquifer was not identical. The arsenic elution seems to have produced in the
reduced state, because the groundwater in Marua village is also in reduced state.

Table 2 Water quality analysis for the groundwater at Marua village on January 2003.

Name
of ORP EC As3+ As5+ T-As HPO43- HCO3- NH4+ Fe2+ T- Iron
Area pH
tube- (mV) (mS/cm) (mgl ) (mgl ) (mgl ) (mgl ) (mgl ) (mgl ) (mgl-1)
-1 -1 -1 -1 -1 -1
(mgl-1)
well
58 7.2 -123 0.757 0.22 0.002 0.222 5.15 476.0 3.49 7.86 10.01
218 7.3 -114 0.591 0.08 0.02 0.10 1.30 446.7 1.26 5.52 8.94
A A-14 7.1 -133 1.52 0.02 0.03 0.05 3.41 634.6 - 15.88 19.40
A-15 7.2 -133 0.851 0.02 0.02 0.04 3.15 491.8 1.447 8.56 12.42
A-2 6.9 -70 1.04 0.001 0.00 0.001 0.10 537.0 4.52 5.83 8.68
3 7.1 -132 0.794 0.07 0.03 0.10 5.82 510.1 4.699 11.24 13.30
33 7.2 -126 0.802 0.03 0.01 0.04 4.12 546.0 2.893 9.95 11.00
B
87 7.2 -125 0.678 0.03 0.03 0.06 2.30 476.0 0.99 5.89 9.46
B-10 7.1 -132 1.14 0.16 0.05 0.21 6.23 806.7 8.298 12.64 16.43
C-6 7.1 -123 0.978 0.14 0.05 0.19 4.04 573.6 5.462 9.28 12.51
C-8 7.1 -137 0.864 0.28 0.06 0.34 4.53 768.9 3.608 7.90 14.85
140 7.1 -136 1.1 0.34 0.04 0.38 4.65 671.2 5.995 11.63 16.57
C
157 7.2 -136 0.673 0.31 0.08 0.39 4.59 482.6 1.249 9.77 12.38
251 7.1 -140 0.822 0.14 0.19 0.33 7.40 698.0 5.154 7.94 10.59
262 7.3 -103 0.462 0.08 0.05 0.12 0.94 378.3 3.925 2.61 3.61
18 7.1 -118 0.534 0.02 0.03 0.05 4.18 418.0 0.502 7.50 9.45
100 7.1 -104 0.827 0.003 0.0004 0.0034 0.77 571.0 1.592 5.11 7.29
D
132 7.1 -74 0.829 0.002 0.0003 0.0023 0.10 537.0 4.48 3.61 3.95
E-15 7.1 -122 0.789 0.002 0.001 0.003 3.94 395.0 1.603 10.21 14.94
Area A, B and C are west pala. Area D is east pala. T-As shows As + As . T-Iron shows Fe + Fe3+.
3+ 5+ 2+

4. CONCLUSIONS
The results on the arsenic elution to groundwater in Samta are summarized as follows.
The environmental condition of the groundwater in the northern part of the village is in the
oxidation state. Where the arsenic concentration is low. There is no upper muddy layer
where arsenic is contained. The iron is existed in the form of trivalent. And in the
groundwater, ferric ion becomes iron oxyhydroxide, in which the arsenic is trapped. They
have precipitated in the groundwater. As the groundwater flows from the north to the south
in the village, the upper muddy layer was thickened, and the groundwater becomes a
reduced state. In the reduced state, iron oxyhydroxide changes to iron hydroxide. Then the
arsenic is released into the groundwater which causes arsenic concentration become high in
the groundwater.

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ACKNOWLEDGMENT This research was supported by a Grant-in-Aid for Scientific

Research from the Ministry of Education, Science, and Culture of Japan (No.13480159).
We deeply appreciate the National Institute of Preventive & Social Medicate of Bangladesh
for their support.

REFERENCES
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Groundwater in Asia, Miyazaki, Japan,35-38pp.
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Bangladesh, Vol1:Summary, February.
Chakraborti.D., Basu,G.K., Biswas,B.K., Chowdhury,U.K., Rahman,M.M., Paul.K,.
Chowdhury,T.R., Chanda,C.R..Lodh,D., and Ray,S.L.(2000). Proceeding of the
Forth International Conference on Arsenic, Exposure and Health Effects IV, Sam
Diego, California, 27-51pp.
Das, D., Samanta,G., Mandal, B.K., Chowdhury,T.R., Chanda, C.R., Chowdhury,P.P.,
Basu,G.K.,and Chakraborti,D. (1996). Arsenic in groundwater in six districts of West
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