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Environmental Pollution
journal homepage: www.elsevier.com/locate/envpol
Department of Environmental Science and Engineering, Gwangju Institute of Science and Technology (GIST), Republic of Korea
International Environment Research Center (IERC), Gwangju Institute of Science and Technology (GIST), Republic of Korea
c
Soil Science & Land Management Department, College of Agriculture, Cantho University, Viet Nam
b
Detailed classication of the study area; indicators for elevated As levels in groundwater; inverse relationship between As and Mn levels,
characterization of As in groundwater and sediment.
a r t i c l e i n f o
a b s t r a c t
Article history:
Received 4 June 2009
Received in revised form
20 April 2010
Accepted 1 May 2010
A study of groundwater and sediment during 2007e2008 in the Mekong River delta in Vietnam (MDVN)
revealed that 26%, 74%, and 50% of groundwater samples were above the US EPA drinking water
guidelines for As (10 mg/L), Mn (0.05 mg/L), and Fe (0.3 mg/L). The range of As, Fe, and Mn concentrations
in the MDVN were <0.1e1351 mg/L, <0.01e38 mg/L, and <0.0114 mg/L, respectively. Elevated levels of
As were found in groundwater at sampling sites close to the Mekong River and in wells less than 60
70 m deep. An inverse relationship was found between As and Mn concentrations in groundwater.
Sediment samples from An Giang and Dong Thap had the highest As concentrations (18 mg/kg and
38 mg/kg, respectively). Arsenic sediment occurred mainly in the poorly crystalline Fe oxide phases.
Reductive dissolution of the Fe oxide phase is not necessarily the dominant mechanism of As release to
groundwater.
2010 Elsevier Ltd. All rights reserved.
Keywords:
Arsenic
Iron
Manganese
Groundwater
Core sample
Mekong river delta
Vietnam
1. Introduction
Arsenic (As) occurs in a variety of environmental media
including minerals, rocks, sedimentary deposits, soil, water, and
plants, but usually co-occurs with sulde minerals. The International Agency for Research on Cancer (IARC) evaluated As and As
compounds and classied them into Group 1, which includes
chemicals causally associated with cancer in humans.
Arsenic has caused signicant contamination of soil and
groundwater in many regions of the world including China,
Mongolia, Japan, Nepal, and the United States (Smedley and
Kinniburgh, 2002). Bangladesh and West Bengal have been identied as the countries with the most seriously As-contaminated
aquifers (Anawar et al., 2002; Chowdhury et al., 2000; Mudur,
2000; Smith et al., 2001; Tchounwou et al., 1999). Groundwater
in the Red River delta (Vietnam) has also been reported to be highly
contaminated with As (Berg et al., 2001, 2007, 2008; Buschmann
et al., 2007, 2008; Nguyen et al., 2009).
The geochemical behavior, release mechanism, and distribution
of As in aquifers have been well studied in the Ganges Plain (Harvey
* Corresponding authors.
E-mail addresses: sbang@gist.ac.kr (S. Bang), kwkim@gist.ac.kr (K.-W. Kim).
0269-7491/$ e see front matter 2010 Elsevier Ltd. All rights reserved.
doi:10.1016/j.envpol.2010.05.001
2649
Table 1
Analytical results for SRM 1640.
SRM 1640
As
Fe
Mn
26.67 0.4
26.73 1.8
34.3 1.6
35.2 1.4
121.5 1.1
122.3 3.6
Fig. 1. Arsenic in groundwater of the MDVN. (1) Kien Giang, (2) An Giang, (3) Dong
Thap, (4) Long An.
Table 2
Sequential extraction procedure modied from Silveira et al. (2006) (0.5 g soil).
Phase
Extraction Chemical
Detail
Soluble-Exchangeable
Surface adsorbed
Organic matter
Mn oxides
Poor crystalline
Fe oxides
Crystalline Fe oxides
Residual
2 h, room temperature
5 h, room temperature
30 min, 95 C
30 min
2 h, dark
24 h, room temperature
3 h, 85 C
2650
Table 3
Classication of sampling areas (AG1: Cho Moi; AG2: Phu Tan; AG3: Chau Thanh; AG4: Tan Chau; AG5: An Phu; DT1: Cao Lanh; DT2: Thanh Binh and Hong Ngu; DT3: Tan Hong
and Lai Vung; DT4: Tam Nong, Lap Vo and Thap Muoi; LA1: Can Giuoc, Ben Luc, Can Duoc and Tan Tru; LA2: Chau Thanh and Thu Thua; KG1: Hon Dat and Go Quao; KG2: Rach
Gia, Kien Luong, Tan Hiep and Chau Thanh; KG3: Ha Tien).
Sampling Area
As
Mn
Safe-Slightly
contaminated
(50 ppb)
Moderately
contaminated
(50-100 ppb)
Seriously
contaminated
(> 100 ppb)
Fe
Safe-Slightly
contaminated
(0.5 ppm)
Moderately
contaminated
(0.5e3 ppm)
AG 1
AG 2
AG 3
AG 4
AG 5
DT 1
DT 2
DT 3
DT 4
LA 1
LA 2
KG 1
KG 2
KG 3
Seriously
contaminated
(>3 ppm)
Safe
(0.3 ppm)
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
C
3. Results
3.1. Groundwater quality
For all analyzed elements except As, Fe, and Mn, groundwater
concentrations in samples collected during the rainy season in
2007 from four provinces in the MDVN were well below drinking
water guidelines (Table 4 and Table S3). Excessive concentrations of
As were found principally in groundwater of An Giang and Dong
Thap provinces, whereas very high concentrations of Fe were found
in the groundwater of Dong Thap, Kien Giang, and Long An (Fig. 2).
Unlike the other provinces, approximately half of groundwater
samples collected from An Giang and Dong Thap had As
Seriously
contaminated
(>3 ppm)
C
C
C
C
C
C
C
Slightly
contaminated
(0.3e3 ppm)
Table 4
Average and median values, and ranges for groundwater parameters.
Parameter
Well depth
pH
As
Al
Ba
Cu
Pb
Zn
Co
Ni
Cr
Cd
Mn
Fe
Ca
Mg
Na
K
Si
TOC
Unit
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
mg/L
An Giang
Dong Thap
Kien Giang
(n 107)
(n 86)
(n 123)
Long An
(n 89)
Mean
Median
Range
Mean
Median
Range
Mean
Median
Range
Mean
Median
Range
70
7.75
110
26
361
57
0.5
32
1.8
1.6
0.6
0.4
1595
225
67
42
252
12.5
13.7
3
45
7.84
4
15
257
34
0.4
19
0.9
1
0.5
0.3
634
37
58
29
163
10.8
14.2
1.2
12e128
5.76e8.4
NDe1351
4e343
22e1272
8e722
<0.1e3
8e647
<0.1e12
0.2e15
<0.1e3
<0.1e2
<1e13,988
<1e4755
<0.1e200
2e149
21e1030
2.5e35
2e40
NDe5.8
230
7.4
57
20
366
27
0.7
32
2
3
0.6
0.6
1069
1983
70
51
187
11
21
4
50
7.43
9
13
156
9.5
0.6
132
0.8
1.2
<0.1
0.4
139
339
51
28
109
6
19
1
12e450
5.63e8.12
NDe666
2e253
4e4447
1e519
<0.1e3
3e508
<0.1e29
<0.1e26
<0.1e2
<0.1e6
4e11,038
5e36,277
2e467
2e357
13e1680
2e211
2e47
0.33e8.2
57
7.32
1.74
89
195
25
1.44
83.96
2.75
3.98
2.26
0.57
580
2527
63
68
236
11
29
5.3
50
7.4
0.7
16
122
7
0.5
16
0.5
1.4
<0.1
0.3
119
363
48
50
209
9
30
3.6
3e123
4.09e8.03
NDe16
3e7880
7e1393
<1e479
<0.1e29
5e5101
NDe95
0.2e197
<0.1e13
<0.1e8
1e9569
3e37,861
3e312
1e379
12e1200
2e124
3e66
0.5e18
223
6.67
4.4
273
19
10
0.4
17
1.4
2
0.4
0.13
670
2898
50
32
92
24
21
4.7
215
6.67
2
230
7
2
0.3
11
0.5
1
0.3
<0.1
491
826
41
24
61
22
19
4.1
100e350
3.52e7.86
NDe25
67e1034
<1e435
<1e513
<0.1e6.4
2e231
<0.1e9
<0.1e12
<0.1e2
<0.1e0.3
<1e9088
28e30,669
7e307
5e131
15e323
7e50
12e34
0.2e23
2651
Fig. 2. Ranges of a) pH, b) arsenic, c) iron, and d) manganese in groundwater of the MDVN (AG: An Giang; DT: Dong Thap; KG: Kien Giang; LA: Long An).
Table 5
Percentage of samples from four provinces exceeding the guidelines for drinking
water.
Parameter
(guidelines)
Dong Thap
(N 86)
Kien Giang
(N 122)
Long An
(N 89)
As (10 ppb)
Mn (0.05 ppm)
Fe (0.3 ppm)
43
87
13
38
69
54
2.4
66
55
12
81
71
2652
Table 6
Sampling areas contaminated by arsenic, iron and manganese.
Parameter
(guidelines)
As (10 ppb)
25
Mn (0.05 ppm) 100
Fe (0.3 ppm)
17
AG 2
(n 12)
AG 3
(n 17)
AG 4
(n 41)
AG 5
(n 25)
DT 1
(n 17)
DT 2
(n 23)
DT 3
(n 27)
DT 4
(n 19)
LA 1
LA 2
(n 64) (n 25)
KG 1
(n 60)
KG 2
(n 53)
KG 3
(n 10)
50
92
17
0
100
0
44
90
2.4
72
64
36
41
82
41
83
83
83
15
59
63
16
53
16
0
96
88
1.7
73
54
1.9
64
59
10
40
40
44
40
28
Fig. 3. Interactions of arsenic and target parameters measured in groundwater of An Giang and Dong Thap.
2653
Table 7
Mean arsenic levels (mg/L) among sample groups from An Giang and Dong Thap.
Grouping factors
Distance
Well depth
pH
TOC
Mn
Fe
An Giang (N 107)
Groups
Mean (ppb)
Median (ppb)
Range
Groups
Mean (ppb)
Median (ppb)
Range
2 km
>2 km
N.A
60 m
>60 m
99
7
1
100
7
118
12
0.7
115
19
6
0.9
ND-1351
0.4e66
10
2
NDe666
0.2e16
8
>8
1 ppm
>1 ppm
3 ppm
>3 ppm
0.3 ppm
>0.3 ppm
83
24
43
64
89
18
95
12
132
32
5
180
127
4
105
194
6
1.5
0.8
55
15
3.7
2
111
0.2e1351
ND-275
NDe110
0.4e1351
NDe1351
0.2e32
NDe1351
0.8e543
57
14
21
63
3
4
56
4
6
104
56
2
7
90
NDe666
NDe42
0.2e1351
ND-110
74
9
3
69
15
2
79
7
46
40
78
8
40
46
3
7
6
0.9
15 km
>15 km
N.A
70 m
>70 m
N.A
8
>8
1 ppm
>1 ppm
3 ppm
>3 ppm
0.3 ppm
>0.3 ppm
6
4
1.5
40
6
0.4
1
21
ND-666
ND e8
NDe55
NDe666
NDe666
NDe10
NDe103
NDe666
Distance
Well depth
pH
TOC
Mn
Fe
Ba
Ca
Mg
Na
Si
Co
Ni
Correlation with As
An Giang
Dong Thap
n.s
(0.244; 0.011)
(0.339; 0.000)
(0.390; 0.000)
(0.269; 0.005)
n.s
(0.209; 0.031)
(0.210; 0.030)
(0.294; 0.002)
(0.270; 0.005)
(0.293; 0.002)
(0.245; 0.011)
(0.226; 0.019)
(0.252; 0.025)
n.s
(0.394; 0.000)
(0.367; 0.001)
n.s
(0.243; 0.026)
(0.464; 0.000)
n.s
n.s
n.s
(0.234; 0.030)
n.s
n.s
Values in the parameter are the correlation and signicance, respectively. n.s:
correlation is not signicant.
2654
Table 9
Correlations between As and parameters in groundwater of An Giang and Dong Thap.
Province
An Giang
Dong Thap
Distance
Well depth
pH
TOC
Mn
Fe
Cor.
Inf.
Cor.
Inf.
Cor.
Inf.
Cor.
Inf.
Cor.
Inf.
Cor.
Inf.
O ()
O ()
O
O
O ()
O ()
O
O ()
O ()
O
O
O ()
O
O ()
O
Cor. e correlation between the parameter and As. Inf. inuence of the parameter on As concentration examined by independent sample t-test. correlation or
inuence is not signicant. O - correlation or inuence is signicant.
Fig. 4. Depth prole of arsenic, iron and manganese in core samples from a) Cho Vam-An Giang and b) Thanh Binh-Dong Thap.
2655
Fig. 5. Operationally-dened phases of As in core samples from a) Cho Vam-An Giang and b) Thanh Binh-Dong Thap.
2656
groundwater) may control As leaching from sediment to groundwater. Prerequisites for As release to groundwater may differ
among locations.
4.3. Relationship between arsenic and manganese levels in
groundwater
The relationship between As and Fe in groundwater has been
considered in many studies, including those cited above. However,
it is only recently that concerns about Mn in groundwater have
been raised because of increasing evidence of Mn-caused oral
neurotoxicity, especially in infants (Wasserman et al., 2006).
We observed an inverse relationship between As and Mn
concentrations during our study of more than 400 wells (Fig. 7),
and a high proportion of samples did not meet drinking water
guidelines for these two elements. Table 2 shows that 49% and 88%
of groundwater samples from An Giang exceeded guidelines for As
and Mn, respectively. Up to 93% of groundwater samples from An
Giang were found to have unsafe levels of As and/or Mn. In Dong
Thap, 76% of groundwater samples were contaminated with As
and/or Mn, and only 48% and 37% of groundwater samples had
elevated levels of either of As or Mn (thus not both), respectively.
Only 35% of groundwater samples in the study area had safe levels
of both As and Mn. A similar trend has been reported for groundwater in the Mekong River delta oodplain of Cambodia
(Buschmann et al., 2007).
Manganese is an essential trace element for plants, animals, and
many microorganisms. Mn has been regarded as one of the least
toxic metals when taken orally because homeostasis limits
gastrointestinal absorption. The presence of Mn and Fe in a water
source has been considered problematic because of undesirable
odor and taste. Elevated Mn concentrations may have effects on
plants and humans, especially infants. In 1995, the British Columbia
Ministry of Environment, Lands and Parks established a recommended maximum level of Mn for fresh water aquatic life of
0.1e1 mg/L. In 1987, the Canadian Council of Ministers of the
Environment set an irrigation water guideline of 0.2 mg/L for
continuous watering of any soil types, specically to protect against
the possible toxic effects on plants growing in acidic soils. An irrigation water guideline of 10 mg/L was recommended for continuous watering of up to 20 years on neutral and alkaline soils. A
guideline of 0.05 mg/L for Mn in drinking water recommended by
the US EPA was not toxicologically based, but was rather established to address aesthetic considerations including staining of
plumbing and laundry, and an undesirable taste. From 1958 to
2006, the World Health Organization modied the drinking water
guideline for Mn several times: 500 mg/L (1958), 100 mg/L (1983),
500 mg/L (1993), and 400 mg/L (2006). The Vietnamese guideline for
Mn in drinking water is 0.5 mg/L (TCVN 6002-1995). However,
a level of 0.01 mg/L was recommended for Mn based on a study of
Mn deposition in a drinking water distribution system (Sly et al.,
1990). In our study region, the occurrence of Mn in the water
supply is a serious issue that should be addressed, particularly in
view of the inverse relationship between Mn and As.
5. Conclusion
In a study of 460 wells in the MDVN, we found that 26% and 50%
of groundwater samples exceeded WHO guidelines for As and Fe,
respectively, and 74% of groundwater samples exceeded the US EPA
guideline for Mn. Groundwater in the AG2, AG5, and DT2 areas was
seriously contaminated by As. Convincing evidence was found for
the dependence of groundwater As concentrations on spatial
parameters (distance to the Mekong River and well depth) and
hydrogeochemical variables (pH, TOC, and Mn and Fe concentrations). Indicators of elevated As concentration in groundwater
included well location within 2 km of the Mekong River bank, and
well depths less than 6070 m. An inverse relationship found
between As and Mn, that negatively affected groundwater quality.
The maximum concentrations of As in the CV and TB cores were
found at depths of 46 m and 34.5e34.9 m, respectively. The largest
proportion of sedimentary As was associated with poorly crystalline Fe oxides, whereas As was almost absent in carbonate and Mn
oxide phases. Local hydrobiogeochemical conditions in the aquifer,
including presence of sedimentary organic matter (or other electron donors), indigenous microorganisms, groundwater ORP, pH,
and the combined effects of ions in groundwater, may control As
leaching from sediment to groundwater.
Acknowledgement
This study was supported by the UNU & GIST Joint Programme
on Science and Technology for Sustainability, and also by the
Vietnamese Ministry of Education and Training (MOET) through
the HUS-GIST Joint PhD Programme.
Appendix. Supporting information
Supplementary information associated with this paper can be
found, in the online version, at doi:10.1016/j.envpol.2010.05.001
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