Applied Geochemistry 23 (2008) 3019–3028

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Applied Geochemistry
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Hydrogeological survey assessing arsenic and other groundwater

contaminants in the lowlands of Sumatra, Indonesia
Lenny Winkel, Michael Berg *, Caroline Stengel, Thomas Rosenberg
Eawag, Swiss Federal Institute of Aquatic Science and Technology, 8600 Dübendorf, Switzerland

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

Article history: Groundwater conditions in the lowlands of Sumatra, where peat swamps are the dominant
Available online 8 July 2008 landscape, were investigated. Based on topography, soil and geological surface properties,
this large area (about 100,000 km2) is vulnerable to groundwater As enrichment under
reducing aquifer conditions. The reconnaissance groundwater survey was conducted in
the province of South Sumatra, covering both presumed low- and high-risk areas of As
enrichment. Five distinct types of groundwater were recognized, reflecting a variety of geo-
logical sources and chemical conditions which are understood to be typical for the whole
east coast of Sumatra. Groundwater collected from tubewells in the youngest (Holocene)
swamp deposits had elevated As concentrations (>10 lg L1) with a maximum of
65 lg L1. Other elements exceeding the WHO drinking water guideline values include B,
Mn, and Se. In contrast to large deltas of continental South and SE Asia, significantly lower
sediment loads are transported by the rivers of Sumatra. The organic-rich Holocene sedi-
ments are hence relatively thin. Tubewells tapping the oldest geological formations of
the study area (middle Miocene to Pliocene) have a broad range of redox conditions reflect-
ing variations in aquifer geochemistry. This group is generally characterized by alkaline pH
conditions and high contents of Na, B, Se, and Sr. Oxic groundwaters were found in regions
elevated above 20 m a.s.l. and are characterized by low concentrations of dissolved solids
and acidic pH values (average 5.1). To date, groundwater data for the increasingly popu-
lated island of Sumatra are non-existent in the international literature and this study thus
provides a basis for future in-depth groundwater studies. The complete georeferenced
database of groundwater analysis is provided as supplementary material.
Ó 2008 Elsevier Ltd. All rights reserved.

1. Introduction environments of the Ganges–Brahmaputra delta, Cambo-

Numerous reports have been published on drinking
water enriched with As derived from natural geological
sources (e.g. McArthur et al., 2001; Berg et al., 2001; Smed-
ley and Kinniburgh, 2002; Buschmann et al., 2008). The
WHO guideline value for As in drinking water is 10 lg L1
but especially in SE Asia, groundwater As concentrations
can exceed 200 lg L1 (Berg et al., 2007; Polya et al.,
2005; Buschmann et al., 2007; Postma et al., 2007; Eiche
et al., 2008; Norrman et al., 2008; Rodriguez-Lado et al.,
2008; van Geen et al., 2008). The densely populated deltaic
* Corresponding author. Tel.: +41 44 823 50 78; fax: +41 44 823 50 28.
E-mail address: michael.berg@eawag.ch (M. Berg).
dia, and Vietnam (Red river delta and Mekong delta) are
undoubtedly among the most severely affected areas.
These regions of SE Asia have a number of characteristics
in common: (i) flat topography, (ii) rapid Holocene sedi-
mentation fed by large rivers, and (iii) abundance of
degradable organic material.
Microbially-mediated reductive dissolution of Fe oxides
is proposed to be the main mechanism for large-scale As-
release to the groundwater. Arsenic is to a large extent
adsorbed to Fe oxides such as ferrihydrate and goethite
especially at acidic pH. Arsenic mobilization by reductive
dissolution of Fe oxides requires a source of degradable
organic C (McArthur et al., 2001) which can be (sub)surface
organic material (Harvey et al., 2002; Islam et al., 2004) or

0883-2927/$ - see front matter Ó 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.apgeochem.2008.06.021
3020 L. Winkel et al. / Applied Geochemistry 23 (2008) 3019–3028
sedimentary organic matter (e.g. peat) (Ravenscroft et al.,
2001; McArthur et al., 2004; Meharg et al., 2006; Berg
et al., 2008). Once Fe-reducing conditions are established
in the aquifer, As is either desorbed from the surface of
the dissolving Fe oxide, or it is released from the mineral
structure itself (McArthur et al., 2001; Harvey et al.,
2002; Swartz et al., 2004). This process is commonly re-
ferred to as reductive dissolution. Other factors leading to
desorption of As from the surface of Fe oxides are alkaline
conditions (Fuller et al., 1993; Dzombak and Morel, 1990),
the reduction from adsorbed arsenate to arsenite (Smedley
and Kinniburgh, 2002; Bose and Sharma, 2002), the pres-
ence of competing ions such as phosphate (Appelo et al.,
2002), and recrystallization of more reactive Fe oxides into
more crystalline phases (Pedersen et al., 2006).
Several islands in the Indonesian archipelago, notably
Sumatra and Kalimantan, have characteristics in common
with the known major contaminated areas: low topo-
graphic gradients and environments rich in organic C, e.g.
tropical peat swamps. However, to the best of the authors’
knowledge, no data are available reporting groundwater As
enrichment in Indonesia. Nevertheless, new prediction
maps for As in groundwater at concentrations exceeding
10 lg L1 indicate a high risk (probabilities >0.4) for As
enrichment along Sumatra’s SE coast (Winkel et al.,
2008a). The present study aims to quantify the enrichment
of groundwaters with As and other potentially hazardous
elements in the lowlands of Sumatra. For this purpose,
102 groundwater samples were collected (5 dug wells, 97
tubewells) in the surroundings of the city of Palembang
(South Sumatra). The studied domain (some 5000 km2)
stretches across areas of high and low probabilities of
Fig. 1. (a) Map of Sumatra and (b) the study area, indicating high risk areas (probability >0.4) and low risk areas (probability <0.4) for groundwater with As
concentrations exceeding 10 lg L1 (maps modified from Winkel et al., 2008a).
groundwater being enriched in As (see Fig. 1). The goals
were (i) to assess the magnitude of As and other geogenic
potentially hazardous elements in the groundwater, (ii) to
chemically and geologically characterize the aquifers, and
(iii) to gain understanding on the mechanisms of As-re-
lease to the groundwater.
2. Geography and drinking water resources
South Sumatra is the largest of the island’s eight prov-
inces, with swamplands being the dominant landscape. It
is low-lying with an average elevation of less than 50 m
above sea level (a.s.l.) and dissected by nine rivers. The pro-
vincial population totals 6.9 million, but has a low popula-
tion density outside the capital Palembang. South Sumatra
is rich in natural resources such as oil, gas, and coal, and
harvests agricultural products like rubber, pepper, and
palm oil (Morris et al., 2002). Being located astride the
equator, the island of Sumatra has a humid tropical climate
with average daytime temperature of 28 °C. The dry season
runs from May through September and the rainy season
starts in November and peaks in February with average an-
nual rainfall over 2500 mm. Peat swamps are the typical
biotope of this province, which serve as a natural buffer be-
tween salt and fresh water and as a filter for potentially
harmful metals and hydrocarbons (Phillips, 1998). How-
ever, pristine peat swamp forests are continuously de-
stroyed by large-scale fires which pose an increasing
problem to Indonesia and surrounding countries (Dennis
et al., 2000). In coastal areas, wetland and peat soils are
found on top of the sediments. Mineral (sub)soils consist
of clays and along the coast potential acid sulfate soils are
 L. Winkel et al. / Applied Geochemistry 23 (2008) 3019–3028
present (Wösten et al., 2006). Inland areas (>20 m a.s.l.) are
better drained and mainly covered by laterite soils. Soil-
minerals are quartz, volcanic glass, labradorite (Ca–Na–Al
silicate), sanidine (K–Al silicate), and lithic fragments. Sec-
ondary minerals resulting from chemical weathering are
clay minerals (kaolinite, smectite, and illite) (Subandiono
and Badayos, 2005). In the district (Kabupaten) of Palem-
bang, drinking water is delivered by pipes from a river
water treatment plant. In the rural areas, drinking water
is mostly supplied from dug wells and tubewells although
many households in more secluded villages still rely on sur-
face water supply from rivers or marshes.
The population of South Sumatra has rapidly increased
over the last decades due to large-scale transmigration
programs involving government-financed movement of
landless people from the crowded inner islands of Java,
Bali, and Lombok to agricultural-based settlements in
Sumatra (Leinbach et al., 1992). Health problems related
to the consumption of contaminated groundwaters in
South Sumatra have not been reported so far. Where
groundwater is the main drinking water resource and lev-
els of dissolved Fe are high, the people frequently use
household filters to reduce Fe, applying sand, charcoal or
coconut skin as filter media. However, the effectiveness
in producing contaminant-free water remains unknown.
3. Regional geology
The study area geologically belongs to the South Suma-
tra basin that evolved from a marine to a deltaic deposi-
tional environment at the beginning of Tertiary times.
The youngest geological deposits are the Palembang for-
mation, which is the ‘‘regressive” stage of the South Suma-
tra basin fill, the Holocene swamp, and alluvial deposits
(Darman and Sidi, 2000). The Palembang formation is sub-
divided into three members: (i) Lower Palembang forma-
tion (Air Benekat formation), (ii) Middle Palembang
formation (Maura Enim formation), and (iii) Upper Palem-
bang formation (Kasai formation).
The lower Palembang formation is present in the NE of
the study area forming an eroded core of a gently dipping
anticline. It was deposited in the middle Miocene during a
period of marine regression when the depositional envi-
ronment changed from deep to shallow marine (Bishop,
2001). Sediments mainly consist of Glauconitic sands and
clays. The thickness of the formation ranges from 100 to
1000 m (Darman and Sidi, 2000). Recoverable reserves of
oil and gas are present in the sandstone reservoirs of this
formation and are currently exploited by Pertamina, a
state-owned oil company (Bishop, 2001).
The lower and upper contacts of the Middle Palembang
formation are marked by thick coal beds. This formation
was deposited in the late Miocene to Pliocene as shallow
marine to continental sands, tuffaceous muds, and coals.
Sands may be glauconitic and contain volcanic debris of
acid to intermediate composition (Darman and Sidi,
2000). The formation thins to the north from a maximum
of 750 m in the south (Hutchison, 1996). Sediment sources
are erosional products of the Barisan mountains (western
Sumatra).
3021
The Upper Palembang formation contains continental
tuffaceous sands, clays, gravels, and thin coal beds. This
formation is found in valleys and synclines formed during
deformation of the Barisan Mountains (Bishop, 2001). Its
contact with the Middle Palembang formation is character-
ized by brownish-red to gray Fe oxide gravel. Sediments of
this formation are derived primarily from the Barisan
mountains. Intercalations of ash layers are frequent
(Hutchison, 1996). The formation is 100–500 m thick and
most surface sediments in the South Sumatra basin belong
to this unit.
The youngest sediments (late Pleistocene and Holo-
cene) unconformably overly the older sediments and are
mainly deposited in peat swamp forests or along modern
rivers, where local sediment thicknesses exceed 100 m.
Nevertheless, the Holocene swamp formation has a highly
irregular thickness since it mainly fills depressions in older
formations. Groundwater generally flows from west to east
(i.e. from the mountains to the swampy lowlands), but lo-
cal alterations along the courses of rivers and geological
intersections are likely.
4. Sampling and analysis
The groundwater survey was conducted in the province
of South Sumatra (Sumatera Selatan). The dimensions of
the study area are 85 km (west to east) by 65 km (north
to south), situated between 2.8717S–3.91043S and
103.9493E–104.9932E (WGS84 system) (see map in
Fig. 1). Accessible groundwater wells were randomly se-
lected at an average sampling density of one sample per
50 km2, with 102 samples (5 dug wells and 97 tubewells)
being collected in January 2007. Each location was geo-ref-
erenced with a hand-held global positioning system (GPS)
unit.
Procedures of sampling were carried out as described in
Buschmann et al. (2007). Groundwater was pumped with
the hand- or electrical pumps permanently mounted to
the privately owned tubewells. Redox potential (against
SHE), pH, temperature, O2, and conductivity were recorded
on-site by a portable system YSI 556 and a WTW Multi
340i (John Morris Scientific Pty Ltd). Prior to sampling, at
least two tubewell volumes of groundwater were pumped
(e.g., at least 160 L from a 40 m deep well, tube i.d. 5 cm
(2 in.)). Samples were then taken once the O2 and redox
readings in the water reached stable values. An aliquot
(60 mL) for the analysis of metals, NH4+ and PO43 was fil-
tered (0.45 lm cellulose nitrate filter, Schleicher & Schuell,
Germany) and acidified with approximately 1 mL of con-
centrated HNO3 (65%, Fluka, Switzerland) to a pH < 2. An-
ions, alkalinity, and DOC were determined in non-
acidified and non-filtered water (120 mL). The samples
were shipped to Switzerland by airplain and stored at
4 °C in the dark until analysis.
The chemical constituents in the groundwater samples
were quantified from triplicate analyses. Arsenic, Al, B,
Cu, Pb, Se, Zn, and U concentrations were measured by high
resolution inductively-coupled-plasma mass spectrometry
(HR ICP-MS, Element 2, Thermo Fisher, Bremen, Germany).
Iron, Mn, Na, K, Ca, Mg, Sr, and Ba concentrations were
3022 L. Winkel et al. / Applied Geochemistry 23 (2008) 3019–3028
measured by inductively-coupled-plasma optical emission
spectroscopy (ICP-OES, Spectro Ciros CCD, Kleve, Ger-
2
many); NH4+ and PO43 by photometry; NO 3 , SO4 , and
Cl by ion chromatography (Dionex, Switzerland); alkalin-
ity by titration; and dissolved organic C (DOC) with a TOC
5000A analyzer (Shimadzu, Switzerland). Analytical uncer-
tainties of the measured parameters were <20%. More de-
tails on the applied analyses as well as on quality
assurance measures are given in Berg et al. (2008). The
complete georeferenced database of groundwater analysis
is provided as Supplementary material.
5. Results and discussion
5.1. Arsenic concentrations in groundwater
Arsenic concentrations showed a heterogeneous distri-
bution over the study area, with 12 out of 97 samples from
the tubewells exceeding the WHO guideline value for
drinking water (10 lg L1) (see Fig. 2). Elevated As levels
were mostly present in groundwater of tubewells located
in Holocene deposits, but were not related to geographical
features (e.g. population density). To gain insight into the
mechanism of As-release to the groundwater, it is impor-
tant to consider Eh and pH values as they are key parame-
ters in the mobilization processes (Cullen and Reimer,
1989: Smedley and Kinniburgh, 2002). Fig. 3 shows that
Fig. 2. Arsenic concentrations measured in groundwater collected ran-
domly at accessible wells in the Palembang area (Sumatra) in January
2007. Arsenic concentrations exceeding 10 lg L1 are mainly found in
low-lying areas (<10 m a.s.l.) and in the vicinity of rivers.
Fig. 3. Log As concentration versus pH in groundwaters of Sumatra.
As concentrations >10 lg L1 were present at pH values
between 6 and 7.5. Fig. 4 depicts concentration trends of
Fe, Mn, As, PO4, and SO4, plotted against Eh measured in
the field. At high Eh values, SO4 is present as the dominant
species and Fe, Mn, As, and PO4 concentrations are low.
With decreasing Eh values, the first species that appears
in the groundwater is Mn, presumably by reduction of
MnO2. The second element to appear in solution as Eh val-
ues continue to decrease is Fe, due to the dissolution of Fe
oxides as is discussed previously. At an Eh value of below
180 mV, PO4 levels gradually increase. As soon as condi-
tions change from oxidizing to reducing, concentrations
of As and PO4 increase rapidly (from 10 mV downwards),
accompanied by a sharp decrease in SO4 presumably be-
cause it being reduced to sulfide. Similar enrichment
trends of PO4 and As can be explained by ion competition.
Since PO4 and arsenate are structurally similar (Hiemstra
and van Riemsdijk, 1999), there is strong competition be-
Fig. 4. Concentration trends of As, Fe, Mn, PO4 and SO4 plotted against
measured redox potentials (Eh). To normalize the abundance of the
species, percentages relative to the highest measured value were used as
Y-axis. These percentages are plotted as trend lines, which were
smoothed using a Moving Average filter (using Excels Chart Add
Trendline) with a period of 20 (the first point of the trend line is the
average of the first 20 values).
 L. Winkel et al. / Applied Geochemistry 23 (2008) 3019–3028 3023

small. In the light of those results, the different peaks for

As and Fe concentrations may indicate that the release of
As is limited by the adsorption capacities of Fe oxides.

5.2. General water chemistry

Chemical compositions and field parameters of the indi-

Fig. 5. Iron and NHþ
4 concentrations as a function of As concentration.
tween both ions for adsorption sites (Acharyya et al.,
1999).
The prevailing hypothesis for As mobilization is that it
is released simultaneously with Fe(II) from sediments dur-
ing the microbially-mediated reduction of Fe oxides
(Smedley and Kinniburgh, 2002). The data plotted in
Fig. 5 show a weak but positive correlation between As
2
and NHþ 4 (R = 0.24). There is no correlation of dissolved
Fe with As (R2 = 0.01), nor do the maxima in Fe and As con-
centrations occur at the same Eh values. Results from a re-
cent study (Pedersen et al., 2006) show that the congruent
release of As and Fe during reductive dissolution of certain
Fe oxides cannot be expected because arsenate remains ab-
sorbed to the surface until the surface area becomes too
vidual tube and dug well samples are listed in Table SD 1
(Supplementary material). The investigated dug wells are
located in the swampy lowlands close to Palembang and
are very shallow, between 2 and 8 m depth. Dug well
waters are characterized by acidic pH (4.0–6.3; median
5.4), high DOC concentrations and low levels of dissolved
O2 and low concentrations of inorganic ions, which is typ-
ical of groundwater derived from recent peat deposits
(Phillips, 1998). Eh values ranged from 59 to 374 mV (med-
ian 244), indicating rather oxic conditions. The amount of
total dissolved solids (TDS) was low (22.9–133 mg L1;
median 106 mg L1) reflecting limited mineral reaction
and a lack of sea salt in the recharge.
Chemical analyses of the tubewell samples revealed a
broad range in the composition of groundwater constitu-
ents reflecting different water bodies and solutes as well
as different redox conditions. A summary of data is pre-
sented in Table 1. Based on Fe and NO3 concentrations,
four characteristic groups of groundwaters were identified
(see Fig. 6). These groups are: group A (13 wells) with NO3
and Fe concentrations below limit of quantification (LOQ);
group B (27 wells) with high NO3 concentrations and Fe
below LOQ; group C (11 wells) with NO3 concentrations
below LOQ and high Fe concentrations (>11.2 mg L1);

Table 1
Average concentrations and ranges for the five groups of tubewells

Unit WHO guideline Group A (n = 13) Group B (n = 27) Group C (n = 11) Group D1 (n = 20) Group D2 (n = 26)
avg. (range) avg. (range) avg. (range) avg. (range) avg. (range)
Fe mgL1 0.1 (<0.10.6) 0.1 (<0.11.5) 23.3 (11.452.5) 3.6 (1.08.8) 5.3 (1.511.1)
NO3-N mgL1 <0.25 (<0.25) 5.6 (0.328) <0.25 (<0.25) <0.25 (<0.250.8) <0.25 (<0.250.7)
As lgL1 10 5.8 (<0.134) 0.5 (<0.13.8) 7.2 (<0.135) 9.8 (0.265) 2.6 (<0.122)
B lgL1 300 1030 (1.03700) 88 (<12000) 110 (12230) 340 (161300) 25 (<1120)
Cu lgL1 2000 1.4 (0.15.2) 4.6 (<0.310) 0.4 (0.11.3) 0.9 (0.16.8) 0.7 (0.22.3)
Mn lgL1 300 30 (<10120) 140 (<101430) 1170 (804720) 200 (<10630) 280 (50760)
Pb lgL1 10 0.23 (0.041.3)) 1.6 (0.068.1) 0.08 (0.020.14) 0.12 (0.100.55) 0.09 (0.030.38)
Se lgL1 10 16 (<0.156) 0.7 (<0.114) 15 (<0.148) 8.3 (<0.179) 0.6 (<0.110)
Zn lgL1 5000 24 (1.346) 38 (3.2110) 30 (3.192) 33 (1.4240) 27 (2.4210)
Na mgL1 – 220 (1.4650) 24 (1.1160) 130 (15340) 150 (16660) 27 (2.788)
Ca mgL1 – 19 (0.377) 9.3 (<0.339) 28 (8.564) 24 (3.5160) 6.2 (0.818)
Mg mgL1 – 13 (0.169) 2.1 (0.039.4) 25 (3.968) 23 (1.2111) 2.0 (0.37.4)
Sr lgL1 – 380 (<21810) 63 (<2320) 330 (85720) 310 (322600) 64 (10190)
DOC mgL1 – 4.1 (<0.514.7) 1.6 (<0.57.3) 5.2 (<0.513.8) 9.5 (2.535.0) 1.0 (<0.53.3)
HCO3 mgL1 – 340 (<12770) 43 (<12450) 160 (<12410) 330 (19910) 82 (22190)
NH4-N mgL1 – 1.6 (0.054.7) 0.28 (0.050.86) 5.3 (0.2222) 4.0 (0.2913) 0.35 (0.080.83)
PO4-P mgL1 – 0.17 (<0.031.31) 0.12 (<0.031.33) 1.0 (<0.033.35) 1.4 (<0.035.21) 0.22 (<0.031.45)
SO2
4 mgL1 – <5 (<5) 7 (<524) <5 (<511) 13 (<5118) <5 (<5)
Eh mV – 38 (274341) 220 (167392) 85 (13625) 89 (260180) 55 (18968)
pH  – 7.1 (4.78.6) 5.1 (4.17.8) 6.3 (5.96.8) 6.6 (5.17.4) 6.4 (6.06.8)
DO mgL1 – 1.4 (0.18.5) 2.5 (0.17.8) 0.7 (0.11.6) 0.8 (0.13.1) 0.9 (<0.13.9)
Ec lscm1 – 1100 (163400) 210 (19817) 1140 (3032810) 1080 (1615140) 210 (49724)
TDS mgL1 – 440 (41260) 68 (2231) 400 (861210) 350 (272110) 54 (7253)
Depth m – 74 (21200) 43 (20135) 39 (2481) 31 (1470) 50 (1290)

Contents of total dissolved solids (TDS) were obtained by summation of concentrations of Na, K, Ca, Mg, Sr, Ba, B, Cl, SO4, and NO3. The full database of
parameters analyzed is provided as Supplementary data (Table SD 1).
3024 L. Winkel et al. / Applied Geochemistry 23 (2008) 3019–3028

Fig. 6. NO
3 concentration as a function of Fe concentration.

and group D (46 wells) with low NO3 concentrations

(<0.8 mg L1) and medium Fe concentrations (1.0 < Fe <
11.2 mg L1). Group D was further subdivided based on
DOC contents into group D1 (20 wells) with DOC > 2
mg L1, and D2 (26 wells) with DOC < 2 mg L1. Examining
the association of Fe, NO
3 , and DOC is useful to explain re-
dox conditions in the groundwater, as was previously
shown by clustering of chemical variables using principal
component or factor analysis (Stüben et al., 2003; Busch-
mann et al., 2007; Berg et al., 2008). Locations of all tube-
wells of the five groups are projected on the geological
map shown in Fig. 7. Typical chemical and geological char-
acteristics of each group are discussed below.

5.2.1. Group A
Tubewells of group A are mainly located in areas where
older sediments (Lower and Middle Palembang forma-
tions) crop out at the surface (Fig. 7). These wells are on
average deeper than in other groups (median 64 m). Tube-
wells in the Lower Palembang formation in the NE of
Palembang are scarce since the aquifers are particularly
deep in this unit (>100 m). Concentrations of HCO3 are
generally high and mainly correlated to Na (R2 = 0.80). No
significant correlation of the rock-forming elements Ca
(R2 = 0.01) and Mg (R2 = 0.04) was found (see Fig. 8a). Ele-
vated concentrations of Na, as well as of B (see Table 1),
could partly be explained by ‘‘old” seawater pockets,
formed during the marine to transitional history of sedi-
ments. However, after correcting for Na with Cl from sea-
water input, it becomes obvious that Na is in excess and
there must be another explanation for elevated Na concen-
trations. Groundwaters with similar chemical characteris-
tics, i.e. Na-rich, Ca-low, have been reported in
Norwegian crystalline bedrock aquifers (Banks and Frengs-
tad, 2006). The evolution of those groundwaters was ex-
plained by progressive silicate weathering, such as the
hydrolysis of plagioclase (e.g. labradorite) (Garrels, 1967;
Banks and Frengstad, 2006):
2NaCaAl3 Si5 O16 þ 4CO2 þ 7H2 O
! 2CaCO3 þ 2Naþ þ 2HCO3 þ 4SiO2 þ 3Al2 Si5 O5 ðOHÞ4
Since Ca reacts to calcite (CaCO3), Ca in solution is sub-
sequently depleted. On the other hand, Na dissolution con-
currently increases with alkalinity while consumption of
Fig. 7. Geological map of the study area with the locations of sampled
dug wells and tubewells, classified in five groups. The geological cross-
section corresponding to the indicated transect A–B is shown in Fig. 10.
This map is based on the geological map of Indonesia 1:1,000,000, US
Agency for International Development (USAID); quadrangle X,
Palembang.
protons leads to a rise in pH. Sediments of the Middle
Palembang formation are composed of shallow marine
clays and sands containing acid volcanic debris (tuff), par-
ticularly in the upper part. Acid to intermediate tuffs con-
tain a large fraction of Na-rich feldspars and therefore
plagioclase hydrolysis may play an important role in ele-
vated Na concentrations. Levels of B and Se are also partic-
ularly elevated in this group: 54% of the samples were
found to exceed the WHO drinking water guideline value
for B (0.3 mg L1) and 46% for Se (10 lg L1). Ravenscroft
and McArthur (2004) observed elevated B levels in late
Pleistocene-early Holocene aquifers of Bangladesh. They
explained this by B desorption from mineral surfaces as
freshwater flushing displaces older saline waters from
 L. Winkel et al. / Applied Geochemistry 23 (2008) 3019–3028
Fig. 8. Variations in group A of (a) Na, Ca, and Mg with alkalinity, and (b)
Na, Ca, Se, Sr, and B with pH.
the aquifer. Enrichment of B and Se in groundwater can
also be caused by irrigation, but the study area receives en-
ough rain to sustain agriculture. Selenium in groundwater
is usually present as the oxyanion selenate which tends to
sorb to Fe oxides, clay minerals, and organic matter (Niedz-
ielski and Siepak, 2005). Since adsorption/desorption is
influenced by pH (see Fig. 8b), the Se content in this group
is presumably caused by desorption from mineral surfaces
under more alkaline conditions.
5.2.2. Group B
These groundwaters are typically oxic with a median
dissolved O2 level of 2.1 mg L1. As can be seen in Fig. 7,
the majority of the wells in this group are located on
slightly elevated terrain (20–50 m a.s.l.) in the outcrops
of the Upper Palembang formation. Low TDS levels (Table
1) suggest little mineral dissolution and a lack of seawater
intrusion (Smedley et al., 2007). Wells in this group are fur-
thest away from the coastline and draw water from non-
marine sediments. Elevated Cu, Pb, and Zn concentrations
are indicators for the weathering of primary iron sulfides,
which typically contain trace amounts of transition metals
either incorporated in a solid solution or present as associ-
ated minerals (CuFeS2, PbS, and ZnS) (Winkel et al., 2008b).
Since the sediments from the Upper Palembang formation
are mainly derived from the nearby volcanic mountain
chain (Barisan mountains), the presence of primary sul-
fides in the sediments is feasible. Seawater as a source of
S can be ruled out based on low TDS values and a terrestrial
source of sediments. Furthermore, at the low pH value of
3025
Fig. 9. (a) Variation of Fe and Mn with redox potential (Eh) in tubewells
of group C, and (b) variation of Fe with phosphate in tubewells of groups C
and D1.
this group (median: 5.0), the concentrations of dissolved
Cu and Pb are generally higher than in the other groups,
pointing to enhanced dissolution of these elements from
sedimentary sulfides.
5.2.3. Group C
Most of the wells belonging to this group are located in
the vicinity of a river draining Holocene swamp deposits
(Fig. 7). Geological profiles printed on the geological map
of Indonesia (1:1,000,000, US Agency for International
Development (USAID); quadrangle Palembang) indicate a
considerable increase in thickness (up to 100 m) of Holo-
cene fluviatile/swamp deposits in this area. This suggests
that tubewells in group C tap younger sediments than
the wells of groups A and B. High concentrations of dis-
solved Fe and Mn and the presence of N as the reduced
NHþ 4 species (Table 1) demonstrate the presence of reduc-
ing groundwaters, confirmed by the entirely negative Eh
values (Buschmann et al., 2007). However, as can be seen
in Fig. 9a, concentrations of both Mn and Fe decrease with
further decreasing Eh (R2 = 0.35 and 0.60, respectively).
This can be interpreted as a shift in redox reactions from
Fe and Mn reducing conditions towards SO4 reducing con-
ditions, resulting in the precipitation of Mn and by incor-
poration in sulfide minerals (Stumm and Morgan, 1981).
5.2.4. Group D1
Groundwaters in this group have similar chemical
characteristics to group C, apart from the following
3026 L. Winkel et al. / Applied Geochemistry 23 (2008) 3019–3028
distinctions, i.e., median Fe concentrations are lower and
3
median concentrations of DOC, HCOþ 3 , and PO4 are higher.
All but three wells are situated in the Holocene swamp
deposits. In contrast to group C (that also tap the Holocene
deposits), group D1 wells are more centrally located within
the Holocene depositions (Fig. 7). The high DOC and HCO
levels point to aquifers with abundant and degradable or-
ganic matter, such as formed in peat swamps. The elemen-
tal composition and low Eh values point to overall strongly
reducing groundwater conditions. As was previously dis-
cussed for group C, lower Fe contents could be linked to
SO4 reducing or even methanogenic conditions. Although
CH4 was not measured in the samples, some of the samples
with lowest Eh values (<200 mV) were observed to contain
gas bubbles. In contrast to group C, showing a weak nega-
tive correlation between Fe and PO4 content (R2 = 0.38), Fe
in group D1 is not related to PO4 (R2 = 0.01). This becomes
evident from the data plotted in Fig. 9b. It is therefore con-
cluded that Fe is removed from solution to a higher extend
than is the case in group C, presumably by sulfide
precipitation.
5.2.5. Group D2
Low DOC, HCO þ
3 , and NH4 contents (Table 1) imply that
these aquifers are low in organic material. Sulfate and NO3
concentrations are also low and the small amount of N in
the groundwater is entirely present as the reduced NHþ 4 atively low sedimentation rates during the Cenozoic era
species. This indicates that these groundwaters are reduc-
ing in nature, as is also evident from the median Eh value
(46 mV). Nevertheless the quantity of degradable organic
material is probably insufficient to establish strongly
reducing conditions. Similar to group A, these wells are
mainly located on the outcrops of the Upper Palembang
formation, although at lower elevations (10–20 m a.s.l.).
Based on the chemical composition, this group can be
interpreted to lie at the boundary of a more elevated area
with oxic aquifers (group A) and a lower-lying, poorly
drained swamp area (groups C and D1).
5.3. Possible sinks of arsenic, iron, manganese, and phosphate
Highest concentrations of As and PO4 are reached at re-
dox potentials of 80 to 100 mV (see Fig. 4) but a further
decrease in Eh values leads to a decrease in their concen-
trations. Similarly, Mn concentrations reach a maximum
between 10 and 60 mV and then decrease again. The
value of –60 mV also marks the beginning of a decrease
in Fe concentrations. The ‘‘earlier” decrease of Fe concen-
trations compared to As concentrations may be explained
by the incongruent precipitation of Fe and As as sulfides
(Keimowitz et al., 2007). Eh–pH diagrams of As and Fe spe-
ciation show that at a constant pH value of 6.6 (median of
groups C and D1), a decrease in Eh values would first lead
to pyrite precipitation and thus to removal of Fe from solu-
tion. Only when Eh values decrease further, would As(III)
be removed from solution to form orpiment (As2S3). A
decrease in PO4, Fe, and Mn concentrations has also been
observed in reducing groundwaters being close to satura-
tion or supersaturated with respect to vivianite (Fe3(PO4)2
8(H2O)), siderite (FeCO3), and rhodochrosite (MnCO3)
(Postma, 1981; Ptacek, 1998), or can result from resorption
and/or incorporation (sequestration) to sediment phases
(Berg et al., 2008).
5.4. Magnitude of arsenic concentrations
3 Even though a substantial number of tubewells in the
study area had As concentrations exceeding 10 lg L1, in
comparison to the high concentrations (>200 lg L1) mea-
sured in the Bengal, Vietnam, and Cambodia deltas, the
concentrations are moderate. Possibly, these moderate
concentrations are related to the relatively low pH values
measured in the study area. Buschmann et al. (2007) ob-
served that high As concentrations are accompanied by
high pH values (>7.3). Lower As concentrations were found
in groundwaters with predominantly acidic pH values
(average values 6.4 and 6.8). Also the groundwaters in
the Holocene swamp deposits (groups C and D2) are
mainly acidic, which suggests a hindered desorption of
As from e.g. Fe oxides (Dixit and Hering, 2003).
Another hypothesis for moderate As concentrations is
that the aquifer sediments have sufficiently matured and
that Fe oxides have recrystallized in more orderly struc-
tures. This would result in an overall decrease of As in solu-
tion, either because it is more firmly bound to the
recrystallized phase (Pedersen et al., 2006) or because it
has been flushed away. This hypothesis is supported by rel-
(Métivier et al., 1999) leaving more time for maturation
of sediments. Most of the tubewells with As concentrations
exceeding 10 lg L1 are indeed present in recent alluvial
deposits at close distance to rivers (<5 km; group C) (see
Fig. 2). Therefore As-bearing aquifers appear to be more
abundant where river channels have cut through the older
sediments and where sedimentation rates have been fast
enough to ensure a rapid burial of a thick Holocene sedi-
mentary sequence.
6. Summary and conclusions
Five distinct groups of groundwater composition were
recognized that reflect a variety of geological sources
and/or chemical conditions (pH and redox). A geological
cross-section and exemplified wells of each group are gi-
ven in Fig. 10. The geological units illustrated in this
cross-section are representative for the whole east coast
of Sumatra where similar groundwater conditions are ex-
pected to be present. Arsenic concentrations show a heter-
ogeneous distribution, with the lowest concentrations
measured in group B (oxidizing conditions) and the highest
values in areas with Holocene swamp and alluvial sedi-
mentation (groups C and D1). In 12 of 97 tubewells, As
concentrations exceeded the WHO guideline value for
drinking water (10 lg L1).
The most oxic groundwaters (group B) were found in
the elevated regions (2050 m a.s.l.), which are character-
ized by well-drained sandy soils and terrestrial sediments,
while most reducing groundwaters (group C and D1) were
present in the low-lying, poorly drained, swamp deposits
(<5 m). Group D2 wells form a corridor between oxic and
reducing conditions (Fig. 7). Reducing aquifer conditions
 L. Winkel et al. / Applied Geochemistry 23 (2008) 3019–3028
Fig. 10. Schematic geological cross-section along the transect A–B indicated in Fig. 7. Exemplified tubewells tapping water from the distinct groundwater
groups A–D2 (see Section 5.2) are indicated. The cross-section is based on sediment profiles of the Palembang sheet (X) of the geological map of Indonesia
(1:1,000,000, US Agency for International Development (USAID); quadrangle X, Palembang), of the Geological Research and Development Center, Bandung
(1975–1996), and sheets 1012, 1013, and 1112 of the geological quadrangle map of Indonesia 1:250,000 (Ministry of Mines and Energy. Geological Survey
of Indonesia, Bandung, 1973).
may be related to the proximity of D2 wells to Holocene
swamp deposits. Most of these wells presumably tap aqui-
fers of the Upper Palembang formation (similar to group B
wells; see Fig. 10). The Upper Palembang formation itself
seems to be rather low in organic material, but organic-
rich Holocene swamp deposits overlying this older sedi-
ments may have triggered reducing aquifer conditions by
leaching of organic matter (Berg et al., 2008). Wells posi-
tioned in, and presumably also tapping Holocene swamp
deposits, indicate more substantial mobilization of Fe, As
and PO4. Nevertheless, the lightly acidic conditions prevail-
ing in aquifers of the Holocene swamp deposits could hin-
der a large-scale As-release by desorption from mineral
surfaces.
Tubewells present in the oldest geological formations of
the study area (group A; Fig. 10) have a large range of re-
dox conditions reflecting variations in aquifer chemical
and mineralogical compositions. In general, pH conditions
are lightly alkaline and thus favour the release of species
adsorbed to mineral surfaces (e.g. Se). The three wells of
this group having As concentrations >10 lg L1 are charac-
terized by alkaline pH values and reducing conditions.
Health problems related to the consumption of geogen-
ically enriched groundwaters in the province of South
Sumatra have not been reported so far. Nevertheless, to en-
sure compliance with drinking water standards, testing of
groundwater quality will remain an important activity,
particularly since groundwater progressively gains in
importance as a source of drinking water in Sumatra. Be-
sides As, the elements exceeding the WHO drinking water
guideline include B, Mn and Se.
Acknowledgments
We thank Rudi Febriamansyah, M.A. Hayatuddin and
Erwin Nofyan for support during sampling. We are grateful
to T. Rüttimann and the AuA laboratory for elemental anal-
yses, J. Buschmann for manuscript feedback and A. Johnson
3027
for support within the WRQ project at Eawag. This manu-
script benefited from detailed peer review comments of J.
Klausen, C.J. Sparrenbom and two anonymous reviewers.
Appendix A. Supplementary material
Supplementary data associated with this article can be
found, in the online version, at doi:10.1016/j.apgeochem.
2008.06.021.
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