Journal of Contaminant Hydrology 99 (2008) 137149

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Journal of Contaminant Hydrology

j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / j c o n h yd

Geochemical characterisation of shallow aquifer sediments of Matlab

Upazila, Southeastern Bangladesh Implications for targeting
low-As aquifers
Mattias von Brmssen a,h,, Sara Hller Larsson a, Prosun Bhattacharya a, M. Aziz Hasan a,b,
Kazi Matin Ahmed b, M. Jakariya c, Mohiuddin A. Sikder d, Ondra Sracek e, Annelie Bivn a,
Barbora Douov f, Claudio Patriarca g, Roger Thunvik a, Gunnar Jacks a
a
KTH-International Groundwater Arsenic Research Group, Department of Land and Water Resources Engineering,
Royal Institute of Technology (KTH), Teknikringen 76, SE-100 44 Stockholm, Sweden
b
Department of Geology, University of Dhaka, Curzon Hall Campus, Dhaka, 1000, Bangladesh
c
NGO Forum for Drinking Water Supply and Sanitation, 4/6 Block E, Lalmatia, Dhaka-1206, Bangladesh
d
Department of Environmental Sciences, Stamford University, Dhanmondi, Dhaka-1209, Bangladesh
e
Institute of Geological Sciences, Faculty of Science, Masaryk University, Kotlsk 2, 611 37 Brno, Czech Republic
f
Department of Solid State Chemistry, Institute of Chemical Technology in Prague, Technicka 5, 166 28 Prague 6, Czech Republic
g
Sapienza universit di Roma, Dipartimento Scienze della Terra, P.le A.Moro 5, 00185 Roma, Italy
h
Department of Soil and Water Environment, Rambll Sweden AB, Box 4205, SE-102 65 Stockholm, Sweden

a r t i c l e

i n f o

Article history:
Received 18 March 2008
Received in revised form 12 May 2008
Accepted 14 May 2008
Available online 24 May 2008
Keywords:
Arsenic
Groundwater
Bangladesh
Redox
Hydrogeochemistry
Shallow sedimentary aquifer

a b s t r a c t
High arsenic (As) concentrations in groundwater pose a serious threat to the health of millions of
people in Bangladesh. Reductive dissolution of Fe(III)-oxyhydroxides and release of its adsorbed As is
considered to be the principal mechanism responsible for mobilisation of As. The distribution of As is
extremely heterogeneous both laterally and vertically. Groundwater abstracted from oxidised
reddish sediments, in contrast to greyish reducing sediments, contains signicantly lower amount of
dissolved arsenic and can be a source of safe water. In order to study the sustainability of that
mitigation option, this study describes the lithofacies and genesis of the sediments within 60 m
depth and establishes a relationship between aqueous and solid phase geochemistry. Oxalate
extractable Fe and Mn contents are higher in the reduced unit than in the oxidised unit, where Fe and
Mn are present in more crystalline mineral phases. Equilibrium modelling of saturation indices
suggest that the concentrations of dissolved Fe, Mn and PO3
4 -tot in groundwater is inuenced by
secondary mineral phases in addition to redox processes. Simulating AsIII adsorption on hydroferric
oxides using the Diffuse Layer Model and analytical data gave realistic concentrations of dissolved
and adsorbed AsIII for the reducing aquifer and we speculate that the presence of high PO3
4 -tot in
combination with reductive dissolution results in the high-As groundwater. The study conrms high
mobility of As in reducing aquifers with typically dark colour of sediments found in previous studies
and thus validates the approach for location of wells used by local drillers based on sediment colour.
A more systematic and standardised colour description and similar studies at more locations are
necessary for wider application of the approach.
2008 Elsevier B.V. All rights reserved.

Corresponding author. Department of Soil and Water Environment,

Rambll Sweden AB, Box 4205, SE-102 65 Stockholm, Sweden.
E-mail addresses: mattias.bromssen@ramboll.se (M. von Brmssen),
prosun@kth.se (P. Bhattacharya), kmahmed@univdhaka.edu (K.M. Ahmed),
jakariya@ngof.org (M. Jakariya), am_sikder@hotmail.com (M.A. Sikder),
srondra@yahoo.com (O. Sracek), Barbora.Dousova@vscht.cz (B. Douov),
claudio.patriarca@gmail.com (C. Patriarca).
0169-7722/$ see front matter 2008 Elsevier B.V. All rights reserved.
doi:10.1016/j.jconhyd.2008.05.005

1. Introduction
Groundwater from shallow, Holocene alluvial aquifers of
Bangladesh contains elevated levels of geogenic arsenic (As)
(BGS and DPHE, 2001; Bhattacharya et al., 2002a,b; Ahmed
et al., 2004; Bhattacharya et al., 2006a,b, 2007). Several

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M. von Brmssen et al. / Journal of Contaminant Hydrology 99 (2008) 137149

million tubewells have been installed in these aquifers during

the last decades, in order to provide safe water to the vast
number of people exposed to waterborne diseases derived
from the use of bacterial contaminated surface water. Today,
shallow hand tubewells are the principal source of drinking
water in rural Bangladesh, and a population within a range
from 35 to 77 million is at risk of drinking groundwater with
elevated As concentrations (Smith et al., 2000; Chakraborti et
al., 2004; Kapaj et al., 2006). Most of the tubewells (~90%)
have been installed on private initiatives by local drillers or
masons, presumably by the simple hand percussion drilling
method, a low cost technique for well installation in the soft
unconsolidated alluvial sediments of Bangladesh.
Reductive dissolution of Fe(III)-oxyhydroxides under
strongly reducing conditions in the young sediments seems
to be the prime cause of As mobilization (Bhattacharya et al.,
1997; Nickson et al., 1998; BGS and DPHE, 2001; Harvey et al.,
2002; Stuben et al., 2003; Ahmed et al., 2004; McArthur et al.,
2004; Swartz et al., 2004). The distribution of As is extremely
heterogeneous, both laterally and vertically, and consequently, the patchy distribution has often been explained
in the terms of local variations in sedimentary characteristics, hydrogeological and hydrogeochemical conditions
(BGS and DPHE, 2001; Ravenscroft, 2001; Bhattacharya
et al., 2002a,b; McArthur et al., 2004; Bhattacharya et al.,
2006a,b; Bhattacharya et al., 2008). Targeting shallow
and low-As aquifers in Bangladesh has been difcult. Nickson

et al. (2000) argued that identication of the mechanism of As

release to groundwater may provide a framework to guide the
placement of new wells for abstracting groundwater with
acceptable concentrations of As following the drinking water
standards of Bangladesh (50 g/L) and more specically to
comply with the WHO drinking water guideline (10 g/L;
WHO, 2004). Because of the extremely heterogeneous
distribution of As, BGS and DPHE (2001) reported that
detailed mapping and investigation of As concentrations in
tubewells, as an option for the placement of As-safe tubewells,
would be too difcult. Nonetheless, switching to arsenic safe
tubewells that have been tested As safe and reinstallation of
shallow tubewells to alternate depths have emerged from
peoples own initiative (Jakariya et al., 2007). These so called
well-switching schemes have been encouraged by various
researchers, including van Geen et al. (2002).
In recent studies (van Geen et al., 2004; von Brmssen
et al., 2005; von Brmssen et al., 2007; Stollenwerk et al.,
2007; Hasan et al., in press; Pal and Mukherjee, in press) it
is argued that groundwater from red (or orange/brown)
sediments, within shallower depth (b150 m), are As safe.
These sediments were deposited in alluvial settings under
reducing conditions and were subsequently exposed to
weathering and oxidation during the last glacial maximum
(Umitsu, 1987; Umitsu, 1993). At that time, the surface
sediments were eroded and weathered and then ushed
(Goodbred et al., 2003). Von Brmssen et al. (2005, 2007)

Fig. 1. Location of Matlab Upazila (demarcated by embossed line) in southeastern Bangladesh (inset) and regional surface geology.

M. von Brmssen et al. / Journal of Contaminant Hydrology 99 (2008) 137149

demonstrated a distinct correlation between the colour of the

aquifer sands, groundwater redox-conditions and the relative
risk for mobilization of geogenic As. It was suggested that the
colours of the sediments could be used as a simple tool by the
local drillers to target As-safe aquifers. This study indicated
that it is possible to assess the relative risk of elevated
concentrations of As in aquifers if the colour characteristics of
the sediments are known which would help the local drillers
to target safe aquifers for the placement of new tubewells.
Thus following a simplied use of this sediment colour concept, a sustainable mitigation approach can be established in
Matlab Upazila, and other areas in Bangladesh with similar
geological settings, as well as elsewhere in the world, for
improving the safe water coverage based on the initiatives of
the local drillers. On the other hand, if the sustainability
cannot be proved, such initiatives and the current practice of
the local drillers needs to be stopped immediately before a
large investment is made for installation of new wells.
The objective of this study was to characterise the
different sediments from shallow aquifers of Matlab Upazila,
describe the lithofacies and genesis of sediments and to
establish the relationship between aqueous and solid phase
geochemistry and colour of sediments which is a prerequisite
for further studies on the sustainability of the oxidised low-As
aquifers for drinking water supplies.
2. The study area
Matlab Upazila is located approximately 60 km south-east
of Dhaka to the east of the conuence of the rivers of Ganges
(Padma), Brahmaputra (Jamuna) and Meghna (Fig. 1). Bangla-

139

desh has a tropical climate with a mild winter season between

October and March, a hot humid summer from March to June and
a warm and humid monsoon season from June to October when
most of the precipitation occurs. The study area is situated within
the Meghna ood plain and is characterised by meander channels
and scrolls, natural levees and back swamps formed by the river
system. The low-lying landscape is naturally ooded each year
during the monsoon and the surface sediments are represented
by Holocene alluvial silt. The shallow Holocene aquifers of Matlab
Upazila are heavily affected by geogenic As that is very
heterogeneously distributed over the Upazila (Jakariya and
Bhattacharya, 2007). At the study site a thick layer of black to
grey sediments, down to approximately 40 m, overlies an
oxidised unit of yellowish-grey to reddish-brown sediments
(von Brmssen et al., 2007). The groundwater level is within a
depth of 5 m below ground surface and uctuates 34 m annually
in response to rechargedischarge conditions (Bangladesh Water
Development Board, unpublished data).
3. Materials and methods
3.1. Groundwater and sediment sampling
Groundwater samples were collected from hand tubewells
(n = 40) in two villages, Dighaldi and Mubarakdi of Matlab.
The depth of the tubewells and colour of the sediments (as
described by the drillers) at the screened depth were recorded
by interviewing the drillers who installed the wells. Subsequently, the groundwater composition was linked to the colour characteristics of the sediments. Four colours were used to
describe washed sediments characteristic in the area: black,

Fig. 2. Photographs of the 10 sediment core samples that were used for extraction tests and mineralogical studies, the numbers on top of the cores represent the
depth (in meter), these numbers are used to name the samples. The colour descriptions correspond to the colours described in von Brmssen et al. (2007) followed
by local drillers in Matlab Upazila.

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M. von Brmssen et al. / Journal of Contaminant Hydrology 99 (2008) 137149

described by von Brmssen et al. (2007), i.e. black, white, offwhite and red sediments (Fig. 2) were used for the mineralogical and geochemical investigations.
3.2. Analytical work

Fig. 3. A close-up photograph of the bioturbated shale at the depth of 36 m

(118 ft), the circle mark the vegetation material sampled for 14C-dating. The
diameter () of the core is 5 cm.

white, off-white (buff), and red (orange/brown). Sampling,

colour classication, analysis of tubewell water and evaluation
of the respective hydrogeochemical characteristics for the
different aquifer sediments were carried out during 2004 as
described in von Brmssen et al. (2007). During January
February 2005, a new set of samples were collected from the
same tubewells. The samples from the tubewells represent
typical ground water chemistry from both oxidised and reduced
units, as conrmed by previous investigation at the site (von
Brmssen et al. 2007).
One undisturbed core drilling was conducted at Mubarakdi village and samples were collected by a modied split
spoon method down to the depth of 60 m; 0.3 m core samples
were collected in 5 cm diameter plastic tubes. The drilling was
performed with a combination of a hammer technique and a
donkey pump. Core samples were taken every 1.5 m down to
the depth of 30 m and between 30 and 60 m at 0.6 m interval.
The core samples were sealed at both ends with wax
immediately after recovery in the eld to avoid any oxidation.
Later, the core samples were split for lithological studies
(Fig. 2), one half was preserved for lithological studies and the
other half was used for sequential extraction and mineralogical studies. When the core samples were split, a coal-like
vegetation remains (presumably from a root) was found in the
bioturbated shale unit at the depth of 36 m (Fig. 3). The
vegetation material was picked with clean inorganic tools and
wrapped in aluminium foil for 14C-dating. Ten sediment
samples representing the whole depth and colour spectra

3.2.1. Groundwater analyses

Alkalinity (HCO3) was determined according to the standard
method SS-EN ISO 9963-2 (SIS, 1996) by titrating the ltered
unacidied samples with 0.02 M HCl to pH 4.5. Other major
anions, F, Cl, and SO2
4 were analysed using the ltered
unacidied water samples, with a Dionex DX-120 ion chroma+
tograph with an IonPac As14 column. NO3, PO3
4 -tot and NH4
was analysed spectrophotometrically with a Tecator Aquatec
5400. The major cations (Ca, Mg, Na and K) and minor and trace
elements (Fe, Mn, As) were analyzed analysed by inductively
coupled plasma emission spectrometry (ICP-OES) at the
Department of Geology, Stockholm University. Dissolved
organic carbon (DOC) in the water samples was determined
on a Shimadzu 5000 TOC analyser (0.5 mg/L detection limit
with a precision of 10%). The 14C analysis was performed at the
Radiocarbon Dating Laboratory in Lund using Single Stage
Accelerator Mass Spectrometry (SSAMS).
3.2.2. Mineralogical investigations
Selected sediment samples were analysed under the
stereomicroscope in order to study the bulk minerals responsible for the colours of the sediments. X-ray uorescence (XRF)
and X-ray diffraction (XRD) analyses were carried out at the
Institute of Chemical Technology in Prague, Czech Republic.
3.2.3. Sequential extractions
Sequential extraction was carried out to quantify the
amount of reactive components such as Fe and Mn in the
sediments and their relationship with As. Ten selected core
sediment samples were sequentially leached using i) deionized water (DIW) for quantication of the water soluble
fraction of As and other trace elements; ii) 0.01 M NaHCO3 for
the release of elements under high pH conditions; iii) 1 M Naacetate (C2H3NaO2, NaAc) for elements bound to carbonates
and phosphates phases (Dodd et al., 2000; Ahmed et al.,
2004); iv) 0.2 M oxalate (NH4C2O4, Oxalate) for quantication
of Fe, Al, and Mn bound to amorphous oxides and hydroxides
in the sediments; v) 0.2 M oxalate (NH4C2O4) +0.1 M ascorbic
acid (Oxalate+AA) for residual amount of Fe, Al and Mn bound
to oxides and hydroxides including crystalline phases; and vi)
7 M HNO3 for determining As and other elements associated
with the non-silicate minerals (Table 1). The scheme followed

Table 1
Sequential extraction procedure adopted for the study
Fraction

Extractant

Extracting condition

SSR

Wash step

1 (DIW)
2 (NaHCO3)
3 (NaAc)

DIW
0.01 M NaHCO3 (pH 8.65)
1 M Na-acetate (C2H3NaO2)

1:25
1:25
1:50

25 mL DIW
25 mL DIW
25 mL DIW

4 (Oxalate)
5 (Oxalate+AA)

0.2 M oxalate (NH4C2O4)

0.2 M oxalate (NH4C2O4) + 0.1 M
ascorbic acid
7 M HNO3

2 h shaking, 20 C, pH adjusted to 6.95 with NaOH

2 h shaking, 20 C
2 h shaking, 20 C, pH adjusted to 5 with
acetic acid glacial (C2H4O2)
4 h shaking, 20 C, in the dark
30 min in water bath at 96 C 3 C in the light

1:25
1:25

2 h on sand bed, boiling.

1:15

25 mL DIW
25 mL 0.2 M oxalate (NH4C2O4),
10 min shaking in the dark
None

6 (HNO3)

M. von Brmssen et al. / Journal of Contaminant Hydrology 99 (2008) 137149

141

Table 2
Analytical data used for adsorption simulations using Visual MINTEQ v. 2.53 and diffusive layer model by Dzombak and Morel (1990)
Analytical data
FeOx
As
PO3
4
AsOx

Min

Max

Corresponding input data for simulation

mg/kg
g/L
mg/L
mg/kg

700
1
0.5
0.5

15 000
350
8
1.5

Hfo
As (dissolved)
PO3
4 (dissolved)
As (assumed to be adsorbed)

g/L
mg/L

5
0.5
6.3
25
2.1

100
8.0
7.1
25
7.77

Total amount (solid phase only)

Fixed dissolved concentration
Fixed
Fixed at 25
Total amount (adsorbed + dissolved)
Used for unit conversion for the model

Input data for simulation

Hfo
PO3
4
pH
T
As
L/S ratio aquifer

Boundary condition

C
mg/L
0.238

the methods described by Wenzel et al. (2001) and Bhattacharya et al. (2006a,b) and was performed on 1 g air-dried
homogenised sediment sample in a 50 mL centrifuge tube.
Between each step, the sediment was washed. The extracts
were preserved by acidication with 0.5 mL ultrapure 14 M
HNO3/100 mL. Blanks were used in each step so that
impurities could be subtracted from the extractants.
3.3. Geochemical modelling
Thermodynamic relationships between species in solution
and aquifer solid phases have been investigated through the
degree of saturation with respect to minerals dened as
saturation indices (SI):
SI log IAP=Ksp

where IAP is the ion activity product and Ksp is the solubility
product for a given temperature. When SI = 0 (IAP = Ksp) the
solution is at thermodynamic equilibrium with respect to a
specic mineral and when SI N 0 the water is supersaturated
with respect to a mineral and vice versa if SI b 0. Chemical
equilibrium modelling of SI was thus used to identify possible
sinks, sources and reactions in the aquifer system (Sracek
et al., 2004). Saturation indices calculations were performed
using PHREEQC version 2.14.2 (Parkhurst and Appelo, 1999)
with the WATEQ4F thermodynamic database. Eh values
measured in eld and corrected with respect to standard
hydrogen electrode (SHE) were used for speciation of redoxcouples. This means that the model calculates the activities of
the different species of each element and then uses these
activities for calculation of saturation indices. As redox potential (Eh) as a proxy for redox condition for modelling is
valid only under conditions when there is redox equilibrium,
a sensitivity analysis was done to evaluate the impact of Eh on
the resulting SI values by altering Eh in the model.
Adsorption of As for aquifer conditions was simulated as
surface complexation reactions on hydroferric oxides (Hfo)
with the Diffuse Layer Model (DLM) in Visual MINTEQ 2.53
(Dzombak and Morel, 1990; Allison et al., 1991). The system
hydroferric oxides, adsorbed and dissolved AsIII and PO3
4 were
simulated and compared with analytical data. Default parameter based on Dzombak and Morel (1990) was used for
specic surface (600 m2/g). The modelling approach was based
on the assumptions that As adsorption was controlled by pH,
Hfo content, species of As (AsIII or AsV) and presence of available

competing ions (Smedley and Kinniburgh, 2002; Sracek et al.,

2004; Gustafsson and Bhattacharya, 2007). Input data for the
modelling came from both this and previous studies (Table 2).
The amounts of Hfo and As were calculated based on oxalate
extractions data for Fe and As respectively (FeOx, AsOx) and the
L/S ratio of alluvial aquifer properties. Dissolved As concentration was added to AsOx amount giving total available As in the
system. Dissolved PO3
4 -tot concentration was xed assuming
dissolved PO3
4 -tot was controlled by secondary mineral phases,
and thus, only adsorbed amount was simulated. This assumption was based on the simulations of SI of mineral phases
including PO3
4 -tot (see below).
4. Results
4.1. Sequence of aquifer sediments
The colour of the sediments from the uppermost sequence
is black to greyish while the sediments from the lower
sequence are reddish, yellowish to whitish (Fig. 2). The major
units are separated by 5 m thick hard clayey shale (Figs. 3
and 4). The lithological log prepared from the core samples
with the diagnostic sedimentological characteristics of the
major units are presented in Fig. 4.
The uppermost sequence (Unit 1, Fig. 4) consist of a partly
oxidised topsoil of 2 m covering 5 m dark coloured clay and
28 m of sand, silt and clay in a ning upward sequence down
to a depth of 35 m below the surface. Cross beddings and
trough cross beddings identied in the core samples reveal
that the deposition of the sediments occurred in a tide inuenced ood plain environment. This uppermost sequence
is of Holocene age and has not undergone any extensive
weathering or oxidation and represents reducing aquifer
conditions. Biotite and other dark coloured ferromagnesian
and opaque minerals are responsible for the dark colours.
These minerals are found in bands and together with organic
matters at the depths of 1520 m.
The bioturbated hard shale (Unit 2A, Fig. 4) separating
the two major units is grey in colour and indicate shallow
marine depositional environment. The vegetation matter (root)
incorporated in the shale gave an age of approximately 8000 yr
BP from 14C-analysis and suggests that the marine transgression
took place around that time which is consistent with other
published studies (Goodbred et al., 2003). During 70009800 yr
BP bioturbated sediments were deposited in the Bengal basin.
An unconformity has been identied between the shale and the

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M. von Brmssen et al. / Journal of Contaminant Hydrology 99 (2008) 137149

Fig. 4. Lithological log with the diagnostic sedimentological characteristics of the sequence of sedimentary aquifers of the study area based on the recovered
sediment cores.

uppermost reduced sequence conrming that the underlying

sediments were eroded and exposed to weathering and
oxidation. Thus the two major units correspond to two
interglacial periods. However, no dating could be done for the
underlying sequence due to the lack of organic matter.

Investigations of the core samples derived from the lower

oxidised unit (Unit 2B, Fig. 4) show that these sediments were
also exposed to weathering and oxidation. They have lower
abundance of biotite. Fe(III)-oxyhydroxides coatings on
quartz, feldspars and other mineral grains are responsible

Table
Table 33
Mineralogical
composition of
of sediment
sediment samples
samples investigated
investigated from
from the
the sediment
sediment core
coreprole
prole
Mineralogical composition

* See Figure 4 for the position of the respective sediment samples in the sedimentary sequence
* See Figure 4 for the position of the respective sediment samples in the sedimentary sequence

M. von Brmssen et al. / Journal of Contaminant Hydrology 99 (2008) 137149

for the reddish colour of the sediments. This unit was also
deposited in a uvial and ood plain environment and is
represented by ning upward sequences of sand, silt and clay.
Clayballs incorporated in the sand (see Fig. 2, sample 54) indicate
that some of sediments were deposited in river channels.
4.2. Geochemical characterisation of the aquifers
4.2.1. Groundwater chemical composition
The groundwater samples are mostly of CaMgHCO3 and
CaNaHCO3 types, with HCO3 as the dominant anion.

Reducing conditions with low SO2

4 and NO3 coupled with
+
high NH4 and DOC typically characterise the aquifers
associated with high dissolved concentrations of As. The
groundwater from the reducing unit is characterised by high
+
2
concentrations of As, PO3
4 -tot, NH4, DOC, Fe and by low SO4
while the groundwater from the oxidised unit is characterised
by high Mn, low NH+4, DOC, Fe, PO3
4 -tot and As. For further
details of the groundwater chemical composition of the study
area, we refer to von Brmssen et al. (2007).

143

represented by the white and off-white sediments. Maximum

contents of Fetotal and Mntotal were 32,800 and 300 mg/kg and
minimum contents were 1580 and 14 mg/kg, respectively.
Fetotal and Mntotal correlate very well (Fig. 7) and Fetotal/Mntotal
are almost constant (average 112, std 35) for all samples. Also
FeOx and MnOx correlate well for all sediments although FeOx/
MnOx is distinctively different between reducing (average 107,
std 24) and oxidised sediments (average 35, std 19). AsOx and
FeOx correlate (R = 0.95) for the reducing samples although the
number of samples (n = 4) is low. The FeOxAA/FeOx ratio for the
reducing unit is much lower (average ratio = 3) than for the
oxidised unit (average ratio = 26) and in the oxidised unit FeOx
is much lower than in the reducing unit, approximately 10 to
20 times. While performing the sequential extraction we
noted that the colour of the red sediments changed during the
OxAA extraction step from red to whitish.
The blank concentration for As relative to the extraction
concentration was 50% (std = 25) due to low amounts of As in
respective fraction. For Fe and Mn the blank concentration
relative to the extraction concentration was 2% and 1%
respectively (std = 6% and 1% respectively).

4.2.2. Mineralogical investigations

XRD analysis shows that the mineralogy of the sands is
dominated by quartz, K-feldspar (orthoclase) and plagioclase
(anorthite and albite) with a substantial content of biotite and
ferro-hornblende in the reducing Holocene sediments. Magnetite and rutile were also identied in this sequence
(Table 3). Biotite identied at the depth of 21 and 23 m
corresponds to the dark bands found in the core samples
(Fig. 4). The lower weathered and oxidised sediment
sequence contains relatively lower quantities of feldspars. In
this sequence neither biotite nor ferro-hornblende were
identied, however both rutile and magnetite were found.
Semi-quantitative analysis using XRF shows that the most
abundant metal is Al followed by Fe, Ti, and Mn, respectively
(Fig. 5). Iron content is approximately 65 times higher than Mn
content (average value) for both the reducing and oxidised
sediments. Relatively higher contents of Fe2O3 and MnO
coincide with the reducing sediments, particularly the dark
banded core samples at the depth of 21 m and 23 m, and the red
samples from the depth of 40 and 44 m. Low CaO, MgO and P2O5
coincide with the samples from the oxidised sequence. The very
red sample from 44 m depth is distinctively lower in Na2O, MgO
and CaO. The SiO2 content is relatively lower in the reducing
sequence, ranging from 63 to 82 wt.%.
4.2.3. Sequential extractions
The sequential extraction shows that Astotal contents are low,
maximum total content is 3500 g/kg and was found in the
reducing sequence at the depth of 23 m (Fig. 6). AsDIW
and AsNaHCO3 contents were all below detection limit (bdl:
b130 g/kg), AsNaAc contents ranged from bdl to 400 g/kg, AsOx
from bdl to 1060 g/kg. Highest AsNaAc as well as AsOx values
coincide with reducing sample from 23 m depth, but except that
sample AsNaAc and AsOx contents were of the same magnitude in
both sequences. The highest content of As (1900 g/kg) was
found in the OxAA-fraction of reducing sample 21 and AsoxAA
fraction holds most of the As in 50% of the samples.
The concentrations of extractable Fe and Mn in all
fractions were high in the reducing sequence. The corresponding concentrations were low for the oxidised sediments

Fig. 5. Major element composition (plotted as oxide wt.%) of the sediments

representing the two distinct sedimentary units based on the XRF analyses. a)
Fe, Mn, Al and Ti; b) Si, Ca, K, Na, Mg and P.

Fig. 6. Depth-wise distribution of a) As, b) Fe, and c) Mn, based on the results of the sequential extraction of the aquifer sediments. Please note that the DIW and NaHCO3 fractions are not shown as they were very low
compared to the other fraction.

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145

Fig. 7. Correlations between selected species and sequential extraction fractions, a) Mntotal vs Fetotal, b) MnOx vs FeOx, c) Astotal vs Fetotal, d) AsOx vs FeOx.

4.2.4. Geochemical modelling

The sensitivity analysis of the simulations of SI values shows
that mineral phases including Fe(III), e.g. Fe(III)-oxyhydroxides,
are sensitive to an alteration of Eh. The other mineral phases
discussed in this paper, e.g. siderite and vivianite are not sensitive to the alteration of Eh.
SI calculations indicate that groundwater in both reducing
(black samples) and oxidising aquifers (white, off-white and red
samples) is near saturation with respect to Fe(III)-oxyhydroxides. When performing the sensitivity analysis with lower Eh
values, ground water becomes unsaturated with respect to Fe
(III)-oxyhydroxides. Ground water in the reducing unit is
slightly supersaturated with respect to siderite (FeCO3) and
vivianite (Fe3(PO4)28(H2O)) (SImax ~ 1 and 3, respectively) but
undersaturated in the oxidised unit. SI values for siderite and
vivianite correlate well with concentration of dissolved Fe.
Groundwater in both aquifer units is near saturation with
respect to rhodochrosite (MnCO3) and supersaturated with
respect to MnHPO4. Groundwater from the reducing unit is near
saturation with respect to hydroxyapatite (Ca5(PO4)3(OH)), but
it is undersaturated with respect to the mineral phase in the
oxidised unit (Fig. 8).

The surface complexation modelling of AsIII adsorption in

the reducing aquifer unit suggests that AsIII adsorption is
mainly controlled by the amount of Hfo in solid phase. pH is
less important within the pH-interval found in the aquifer
units of the study area. Only if PO3
4 -tot is included as
a competing ion in the simulations they result in reasonable
concentrations of dissolved and adsorbed AsIII. If PO3
4 -tot is
excluded all AsIII would be adsorbed onto the Hfo. According
to the modelling results H2PO4 is the major P specie with an
3
activity 2 to 4 times higher than HPO2
4 . PO4 is a minor
species only. Fig. 9 shows the simulated dissolved concentrations of AsIII vs dissolved PO3
4 -tot concentrations. In the
diagrams actual groundwater samples are overlain (grey
dots) and a correlation between As and PO3
4 -tot is
observed for the reduced aquifer unit, the R2 value
is 0.4826.
5. Discussion
The lithofacies and genesis of the reddish oxidised
sediments in Matlab Upazila seems to correlate well with
sediments reported from other areas in Bangladesh and West-

146

M. von Brmssen et al. / Journal of Contaminant Hydrology 99 (2008) 137149

Fig. 8. a) Bivariate plots showing the dependency of the modelled SI values for a) Fe(OH)3(a) vs Fe, b) siderite vs Fe, c) vivianite vs Fe, d) hydroxyapatite vs PO3
4 ,
e) MnHPO4 vs Mn and f) rhodochrosite vs Mn.

Bengal India. Oxidised reddish (orange/brown) sediments

have been reported from various parts of West-Bengal, India
(Pal and Mukherjee, in press; McArthur et al., 2004) and
Bangladesh (Umitsu, 1993; Goodbred and Kuehl, 2000; van
Geen et al., 2004; Stollenwerk et al., 2007; Hasan et al., in
press). Further characterisation of these oxidised As-low
aquifers should be given high priority as this appears to be
a viable mitigation option. For drinking water management
purposes a common classication system of these shallow
aquifers should be established so that the different studies
can be systematically organized. Even though the reported
aquifer sequences appear to be very heterogeneous, similar
sediments have been found in nature elsewhere under
similar geological settings. This implies the knowledge of
the sedimentary sequences is important for the local drillers
for the identication of the safe sediments for the installation
of safe wells.
The elevated aqueous concentrations of Fe and Mn
are expected to be a product of reductive dissolution of Fe(III)-

oxyhydroxides and reduction of solid phase Mn(IV)-oxides as

expressed by the simplied equations (for a detailed evaluation of
these processes we refer to Mukherjee et al., 2008-this issue):
8Fe(OH)3(s) + CH3OO + 21H+ = 8Fe2+ + CO2 + 24H2O
2MnO2(s) + CH3OO + 5H+ = 2Mn2+ + 4H2O + CO2
As distinctively higher contents of amorphous Fe and Mn
(FeOx and MnOx) are found in the reduced unit and redoxstatus is sufciently low for iron-reduction, high dissolved
concentrations of both these elements would be expected in
groundwater from the reducing aquifer unit. However,
dissolved Fe concentration is relatively higher in groundwater
of the reduced unit while Mn concentration is relatively
higher in the oxidised unit. As both rhodochrosite and
MnHPO4 are near saturation and/or slightly supersaturated
in both units, these two minerals may exert an important role
for controlling dissolved Mn concentrations, in addition to
redox processes. The SI values for MnHPO4 are approximately
2 and, thus, these calculations may represent a crystalline

M. von Brmssen et al. / Journal of Contaminant Hydrology 99 (2008) 137149

147

Fig. 9. Simulation of adsorbed and dissolved AsIII for the system with hydroferric oxides (Hfo), AsIII and PO3
4 using the Diffuse Layer Model. Figure a) shows results
with maximum amount As found in the sediments and b) with minimum amount.

phase while a non- or semi-crystalline phase may be present

in the aquifer. For dissolved Fe, siderite, vivianite, and/or Fe
(III)-oxyhydroxides would be the minerals that are likely to
control dissolved Fe concentration in the reducing unit, in
addition to redox processes. In the oxidised unit Fe seems to
be more crystalline and less accessible to reductive dissolution. It appears that As is bound to more crystalline phases in
the oxidised zone as the fractions of amorphous phases of Fe
are low. Both oxalate and NaAc extractable fractions of Fe are
low for the oxidised samples.
As we found that both amorphous Fe-oxyhydroxides (FeOx)
and solid phase Mn(IV) oxides (MnOx) contents are higher
(approximately 10 to 20 times) in the reduced unit dissolved As
concentration should be lower here than in the oxidised unit
assuming i) that Fe-oxyhydroxides are the main sorbent, ii) the
same species of As are present, and that iii) pH, the available
amount of As and concentrations of competing ions are
comparable. The species of As were only known for the
dissolved phase in the reduced unit (98% was found to be in
the form of AsIII; von Brmssen et al. 2007) and thus AsIII was
assumed to be the adsorbed species as well. Modelling
adsorption of AsIII shows that competing ion(s) was needed to
explain the high dissolved AsIII concentrations or else all AsIII
was adsorbed onto the Hfo. Including xed dissolved concentration of PO3
4 -tot in the model gave reasonable activities

within the range of AsIII concentrations found in the reducing

aquifer unit demonstrating that high PO3
4 -tot may be responsible for mobilization of As, in addition to the reductive
dissolution of Fe(III)-oxyhydroxides. Fixed dissolved concentra3
tions of PO3
4 -tot could be used as a condition for PO4 -tot in the
3
model, assuming that PO4 -tot concentrations are regulated by
equilibriums with other secondary mineral phases such as
hydroxyapatite and vivianite. Furthermore, a correlation
between dissolved As and PO3
4 -tot was also found and, thus,
based on the surface complexation modelling results we
speculate that PO3
4 -tot and/or other competing ions are
responsible for the high dissolved As concentrations, in addition
to the reductive dissolution of Fe(III)-oxyhydroxides. Validation
of the results of surface complexation modelling has not been
done, however, we suggest that the role of PO3
4 -tot for
mobilizing As should be further studied.
6. Conclusions
The results presented here describe the lithofacies
and genesis of the sediments in the shallow aquifer and
establish the relationship between aqueous and solid phase
geochemistry.
The ndings from these investigations are consistent with
the results reported earlier from the region (von Brmssen

148

M. von Brmssen et al. / Journal of Contaminant Hydrology 99 (2008) 137149

et al. 2007). The ndings also validate the approach of

installation of new safe wells on the basis of sediment colour
as used by the local drillers. However, the colour description
needs to be standardised using scientically acceptable charts
improvising the colour codes following the Munsell Colour
Chart (Munsell Color, 2000). Locally adoptable colour charts
may be produced and provided to the drillers for use in the
eld.
Groundwater in the contaminated reducing aquifers is
+
characterised by high concentrations of PO3
4 -tot, NH4, DOC, Fe
,whereas
the
targeted
oxidised
low-As
aquifers
and low SO2
4
are characterised by high Mn, low NH+4, DOC, Fe, and PO3
4 -tot.
Sediment chemistry of the high-and low-As aquifers show
that Fetotal and Mntotal correlates well for both the high- and
the low-As unit. However, the FeOx/MnOx (oxalate extraction)
is distinctively higher for the reducing high-As unit indicating
that amorphous Fe oxides and hydroxides are more inclined to
weathering and oxidation than amorphous Mn oxides and
hydroxides. Geochemical modelling indicates that the concentrations of Fe, Mn and PO3
4 -tot in groundwater are also
inuenced by the formation of secondary minerals in addition
to redox processes. Simulation of AsIII adsorption within the
reducing aquifer unit system showed that AsIII was largely
inuenced by the amount of Hfo, pH and by competing ion(s).
In addition to reductive dissolution of Fe(III)-oxyhydroxides
we speculate that high PO3
4 -tot concentrations are responsible for mobilization of As as simulation using the Diffuse
Layer Model showed a good t with the observed groundwater
and adsorbed concentrations of AsIII. The study conrms high
mobility of dissolved As concentration in reducing aquifers
with typically dark colour of sediments found in previous
studies and, thus, validates the approach for location of wells
used by local drillers, which is based on sediment colour that
hold promise for future implementation as a sustainable
arsenic mitigation.
The ndings presented here have implications for targeting
low-As aquifers that prompt further studies of the sustainability
of As-low aquifers of Matlab Upazila, SE-Bangladesh. Further
characterisation of the oxidised As-low aquifers should be done
as this appears to be a viable mitigation option. For drinking
water management purposes a common classication system
for the aquifers and colour description of the sediments should
be established. Even though reported aquifer sequences are
heterogeneous, local drillers may target the As-low aquifer
units and thus they play a central part for implementation of the
proposed mitigation option.
Acknowledgements
The work was supported by the research grants from the
Swedish International Development Agency (Sida-SAREC)
dnr:SWE-2002-129, Swedish Research Council (VR-Sida)
dnr: 348-2003-4963 and the Strategic Environmental
Research Foundation (MISTRA) dnr: 2005-035-137. The
authors thank BRAC and NGO Forum for Drinking Water
Supply and Sanitation, Bangladesh for the facilities at Matlab
and to Karim and Alec for assistance during the eldwork. Ann
Fylkner, Magnus Mrth, Monica Lwn, Marianne Ahlbom
helped us with the analytical work. We acknowledge Sigrun
Santesson at the KTH-International Ofce for providing our
students (SLH and AB) with Minor Field Study (MFS) grant as

well as Giesela at Svalorna in Bangladesh for local hospitality

during the eldwork.
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