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REVIEW
factors that will control changes in the distri-
bution of As over time.
“T
he largest poisoning of a population ments has shown that the fine-grained,
in history” is how Smith et al. (1) high–surface area fraction (<10 mm)
described the health impact of el- contains five times as much As as bulk
evated groundwater arsenic (As) concentrations sediments or mica separates (9, 19–21).
in many parts of Bangladesh. Estimates of the Destabilizing As on these Fe oxides is
rural population exposed to unsafe As levels now recognized as a key step in the
by drinking untreated groundwater in India, widespread contamination of ground-
China, Myanmar, Pakistan, Vietnam, Nepal, and water, with other phases possibly
Cambodia have grown to over 100 million (2). playing a subordinate role (14, 22, 23).
Widespread symptoms of disease in people drinking Arsenic is released from Fe oxides
groundwater high in As in some of these countries into groundwater as a result of two
and epidemiological studies conducted elsewhere potentially concurrent processes un-
lead to predictions of a doubling of the lifetime der the anoxic conditions that pre-
mortality risk caused by cancers of the liver, blad- vail in the subsurface. First, field and
der, and lung (3, 4). Groundwater containing As laboratory evidence suggest that mi-
also causes cardiovascular disease and inhibits the crobial reduction of Fe(III) oxides
mental development of children (5, 6). liberates As into the dissolved phase
The affected areas of South and Southeast (23, 24). Reduction of As(V) to more
Asia are low-lying, topographically flat floodplains labile As(III) probably contributes to
of rivers that drain the Himalayas (Fig. 1A) (7). this release but is hard to distinguish
Unconsolidated sands underlying these floodplains India, tubewells extend to depths of ~350 m com- from the reduction of Fe oxides under natural
host increasing numbers of inexpensive wells pared to a maximum of ~100 m in Nepal, Cam- conditions given the rates of groundwater flow.
made of polyvinyl chloride pipe with a cast-iron bodia, and Vietnam, owing to difference in the Second, dissolution of Fe oxides is accompanied
handpump mounted on top (tubewells) that are thickness of unconsolidated sand deposits (8). by the release of other ligands such as phosphate
installed to avoid drinking surface water con- More than half the wells in at least one depth that compete with As for adsorption on the
taminated with microbial pathogens. Extensive, al- interval in each of the five affected countries do remaining Fe oxide surface sites (9).
though by no means sufficient, testing of tubewell not meet the World Health Organization (WHO) The restriction of high dissolved As concen-
water for As has been carried out in most of the guideline of 10 mg/liter As in drinking water trations to aquifers composed of gray-colored sands,
countries that are at risk, with Myanmar the glaring (Fig. 1B). There are also numerous wells con- indicative of coatings of reduced or mixed-valence
exception. taining <10 mg/liter As at all depths. The ex- Fe(II+III) oxides, and the absence of elevated con-
Within the arsenic-affected areas of South and tensive spatial variability of As concentrations at centrations from aquifers containing orange sands
Southeast Asia there is extensive variation in the shallow depths (9–11), even within a single village, coated with Fe(III) oxides (Box 1) suggest that Fe
depth distribution of wells (Fig. 1B). In Bangla- hinders comparisons among field sites and the rec- (III) reduction is a primary factor contributing to
desh and the bordering state of West Bengal, ognition of presumably common biogeochemical- high As concentrations in groundwater (9, 24–28).
hydrological processes that regulate As levels in A systematic analysis of the composition of hun-
groundwater. The source of As is not a mystery, dreds of groundwater samples from the Bengal,
1
Department of Earth System Sciences, Stanford University, however; what is less clear is how the current dis- Mekong, and Red River basins has shown that
CREDIT: SCOTT FENDORF
Stanford, CA 94305, USA. 2Department of Geological Sciences, tribution of dissolved As in the subsurface reached high concentrations of As in groundwater prevail
University of Delaware, Newark, DE 19716, USA. 3Lamont-Doherty its current state. This review focuses on what has under advanced stages of reduction rather than
Earth Observatory of Columbia University, Palisades, NY 10964,
USA. been learned from a decade of field research the onset of Fe oxide reduction (29).
*To whom correspondence should be addressed. E-mail:
conducted in South and Southeast Asia about Microbial Fe(III) and As(V) reduction both
fendorf@stanford.edu (S.F); hmichael@udel.edu (H.A.M.); the processes that resulted in the current dis- require a supply of labile organic carbon. When
avangeen@ldeo.columbia.edu (A.v.G.) tribution of As in groundwater and the key the biological oxygen demand from the decom-
us
Ind utra
h map
Gan
ges Bra
na y
dd
gh
Me
wa
R
Irra
ed
Me
ko
ng
0 400 800 km
B
Nepal India (West Bengal) Bangladesh Cambodia Vietnam
100
Depth (m)
200
300 Ganges
Brahmaputra Red
Ganges Ganges Meghna Mekong Mekong
400
0.0 0.3 0.6 0.9 0.0 0.3 0.6 0.9 0.0 0.3 0.6 0.9 0.0 0.3 0.6 0.9 0.0 0.3 0.6 0.9
Fraction of wells with >10 g/liter per depth quartile
Fig. 1. Distribution of arsenic in groundwater of South and Southeast Asia. (A) are shown on a logarithmic scale. Symbols are color-coded according to the major
Map of four major river basins draining the Himalayas. (B) Depth distribution of river basins shown in (A). The pink line depicts the fraction of wells that exceed
As in groundwater determined for five affected countries. Concentrations of As the WHO As guideline of 10 mg/liter for each depth quartile of the available data (54).
Extractable Fe (g/kg)
15
continued reduction of Fe oxides. from the local (tens of meters) to
Such a situation has been docu- the regional (hundreds of kilo-
mented for deeper aquifers of Bang- meters). Studies of local-scale flow
ladesh where dissolved As levels are 10 systems (39–42), which are most
low despite elevated Fe(II) concen- relevant to the distribution of As in
trations in groundwater (16). In other shallow aquifers, illustrate the com-
situations, the available pool of labile plex, site-specific, and transient na-
organic carbon has been depleted al- Bangladesh ture of natural patterns of recharge
5
though some labile As is still bound Cambodia and discharge (Fig. 3B). Further,
to sediment particles. Sediments de- Vietnam (18) abundant surface water bodies such
posited prior to about 20,000 years Vietnam (50) as rivers, ponds, and wetlands inter-
ago and that were well drained be- 0 act with the groundwater systems.
cause of incision during the last glacial 0 2 4 6 8 10 Monsoonal rains and dry-season
A Groundwater (years)
10-1 10 0 101 102 103 104 105
0
100 B
Depth (m)
NORTH
200
Transfer of As from
sulfide to Fe oxide
by weathering
Release of As
300 from Fe oxides
As sorbs more strongly to groundwater
to orange Fe(III) oxides by reduction
As (μg/liter) than to gray sediments SOUTH
Trapping of As
400 Flushing decreases at oxic interface
<10 >10
14 mobilizable during discharge Wet season
C As pool flooding
3
Local
H - 3He groundwater
flow Potentially sustainable
low-As tubewell Dry season
Fe(III) + As(V) water table
Fe(II) + As(III)
SO42- S2
Fe(II) + As(III)
Fig. 3. (A) Depth distribution of groundwater ages in Bangladesh de- light blue circles but are likely to be low; the age of samples shown as gray
termined by either the 3H-3He method (red symbols) or radiocarbon in those circles is uncertain owing to their low 3He content. (B) Conceptual diagram
cases where 3H was measured and not detected (blue symbols) (54). modified from (9) showing the key processes affecting the distribution of As in
Concentrations of As were not reported for three deep samples shown as groundwater.