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Journal of Hazardous Materials 262 (2013) 10561063

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Journal of Hazardous Materials


journal homepage: www.elsevier.com/locate/jhazmat

Consumption of arsenic and other elements from vegetables and drinking water
from an arsenic-contaminated area of Bangladesh
Mohammad Mahmudur Rahman a,b , Md. Asaduzzaman a,b , Ravi Naidu a,b,
a
b

Centre for Environmental Risk Assessment and Remediation (CERAR), University of South Australia, Mawson Lakes Campus, Mawson Lakes, South Australia, SA 5095, Australia
Cooperative Research Centre for Contamination Assessment and Remediation of the Environment (CRC-CARE), P.O. Box 486, Salisbury South, SA 5106, Australia

h i g h l i g h t s






Concentrations of As and other elements in vegetables and drinking water.


Concentrations of As and other elements in garden soils.
Daily dietary intake of As and other elements for adults from vegetables and water.
Potential health risk was estimated comparing with the FAO/WHO values of metals.
Vegetables alone contribute the elemental intake below the PMTDI values.

a r t i c l e

i n f o

Article history:
Received 22 December 2011
Received in revised form 17 June 2012
Accepted 25 June 2012
Available online 30 June 2012
Keywords:
Arsenic
Groundwater
Garden soil
Vegetables
Health risk

a b s t r a c t
The study assesses the daily consumption by adults of arsenic (As) and other elements in drinking water
and home-grown vegetables in a severely As-contaminated area of Bangladesh. Most of the examined
elements in drinking water were below the World Health Organization (WHO) guideline values except
As. The median concentrations of As, cadmium (Cd), chromium (Cr), cobalt (Co), copper (Cu), lead (Pb),
Mn, nickel (Ni), and zinc (Zn) in vegetables were 90 g kg1 , 111 g kg1 , 0.80 mg kg1 , 168 g kg1 ,
13 mg kg1 , 2.1 mg kg1 , 65 mg kg1 , 1.7 mg kg1 , and 50 mg kg1 , respectively. Daily intakes of As, Cd,
Cr, Co, Cu, Pb, manganese (Mn), Ni, and Zn from vegetables and drinking water for adults were 839 g,
2.9 g, 20.8 g, 5.5 g, 0.35 mg, 56.4 g, 2.0 mg, 49.1 g, and 1.3 mg, respectively. The health risks from
consuming vegetables were estimated by comparing these gures with the WHO/FAO provisional tolerable weekly or daily intake (PTWI or PTDI). Vegetables alone contribute 0.05 g of As and 0.008 mg of Cu
per kg of body weight (bw) daily; 0.42 g of Cd, 8.77 mg of Pb, and 0.03 mg of Zn per kg bw weekly. Other
food sources and particularly dietary staple rice need to be evaluated to determine the exact health risks
from such foods.
2012 Elsevier B.V. All rights reserved.

1. Introduction
Geogenic As contamination of groundwater has been reported
in various regions worldwide, particularly in south-east Asia.
Countries such as Bangladesh, India (in several states), Nepal,
Myanmar, Pakistan, Vietnam, Lao Peoples Democratic Republic
(PDR), Cambodia, China (in several provinces), and the lowlands
of Sumatra in Indonesia are contaminated with As in groundwater [1]. Bangladesh and the state of West Bengal in India are the
two worst As-contaminated areas, where more than 100 million

Corresponding author at: Centre for Environmental Risk Assessment and Remediation (CERAR), University of South Australia, Mawson Lakes Campus, Mawson
Lakes, South Australia, SA 5095, Australia. Tel.: +61 8 8302 5041;
fax: +61 8 8302 3057.
E-mail address: ravi.naidu@crccare.com (R. Naidu).
0304-3894/$ see front matter 2012 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.jhazmat.2012.06.045

people are potentially at risk from groundwater As contamination


[1]. The British Geological Survey (BGS) estimated that 35 million
people are exposed to As levels above 50 g L1 while 57 million
are exposed to As levels above 10 g L1 . These gures are based
on the BGS analysis of 3534 tubewells in 61 of the 64 districts of
Bangladesh alone [2].
Besides As, concentrations of other elements such as Mn, Cr,
Pb, Ni, and U also exceeded the World Health Organization (WHO)
health-based drinking water guideline values in the groundwater of Western Bangladesh [3]. The accumulation of As in food
crops especially rice and vegetables grown in areas of Bangladesh
irrigated with As-contaminated groundwater is now well documented [412]. While a number of studies focused on total and
speciated As in Bangladeshi rice and vegetables [412], to date
studies on other elements present in vegetables are very limited
[4,11]. The concentrations of Cu, Zn, Cd, and Pb were reported in a
severely As-contaminated village (Samta) of Bangladesh [4]. Some

M.M. Rahman et al. / Journal of Hazardous Materials 262 (2013) 10561063

vegetables such as bottle ground leaf (lau shak), ghotkol, taro (kachur
lati), eddoe (Mukhi kachu) and elephant foot (ol kachu) had much
higher concentrations of Pb compared to Cd, and other leafy and
root vegetables contained higher concentrations of Zn and Cu [4].
It is therefore important to determine: rstly, the content of As
and other elements in home-grown vegetables in As-contaminated
areas of Bangladesh; and secondly, the associated risks from consuming contaminated vegetables.
Chronic As exposure from drinking contaminated water causes
skin manifestations such as pigmentation, where depigmentation affects the trunk and limbs while keratosis affects the hands
and feet [13]. Exposure to As has also been associated with
an increased risk of diabetes mellitus, peripheral neuropathy,
hepatomegaly, peripheral vascular disease, cardiovascular effects,
pregnancy problems, cerebrovascular disease, non-pitting oedema
of hands, feet, or legs, and cancer of the lungs, kidney, bladder,
and skin [13]. Copper is an essential nutrient for human health
but it is also a drinking water pollutant; food and water are the
two major sources of Cu exposure in developed countries [14].
Long-term exposure to elevated levels of Cu can cause irritation
of the nose, mouth, and eyes as well as headaches, stomach aches,
dizziness, and acute gastrointestinal effects such as vomiting and
diarrhoea [15]. Long-term exposure to Cu levels above 1000 g L1
in drinking water has been found to cause kidney and liver damage
in infants [16].
Inhaled Ni compounds are carcinogenic to humans although
there is a lack of evidence of a carcinogenic risk from oral exposure
to Ni [14]. Food is the main source of Ni exposure in the nonsmoking, non-occupationally exposed population [14]. Manganese
is an essential nutrient and excessive exposure to Mn has been associated with adverse health effects including neurotoxicity [17]. A
relationship was observed between Mn in water and child intellectual function in the absence of estimates for levels of food and air
in Araihazar, located in Bangladesh [17]. Food is the main source
of daily exposure to Cd, an element which causes increased risk
of tubular dysfunction when exposure occurs at the current PTWI
[14]. Lead in drinking water can cause a variety of health problems.
A prolonged period of Pb exposure causes kidney issues or high
blood pressure in adults and delays in physical and mental development in children [18]. Zinc is essential for all living organisms
[3].
Drinking water, pond water used to irrigate home gardens, garden soils, and various types of home-garden vegetables (leafy and
non-leafy) were sampled from Noakhali to assess the concentrations of As and other elements such as Cr, Mn, Ni, Co, Cu, Zn, Cd,
and Pb. Noakhali is one of the most highly As-contaminated districts
in Bangladesh; 99% and 95% of 843 hand tubewell water samples
had As levels above 10 g L1 and 50 g L1 , respectively [19]. We
recently reported the level of As in drinking water, cooking water
and rice from the same area and the daily consumption of total and
inorganic As from those sources [20]. The main objectives of this
study were to determine the quantity of As and other elements
ingested from vegetables and drinking water by adult members
of the families surveyed in two villages of the Noakhali district of
Bangladesh.

2. Materials and methods


2.1. Sample collection and preparation
Drinking water (n = 14), garden top soils (n = 17), and a total of 87
home-garden leafy (n = 62) and non-leafy (n = 25) vegetables which
were commonly consumed collected from 14 households in two
adjacent villages (Chiladi and Basantapur) situated in the Noakhali
district in Bangladesh during December 2008. Due to the mitigation

1057

activities, all surveyed families were aware of As contamination in


groundwater and revealed that pond water was currently used to
irrigate their garden vegetables. We also collected and analysed
water from 14 ponds used by the selected households for agricultural irrigation of their home gardens. During the eld sampling,
interviews were undertaken with all surveyed families to establish
the rate of daily intake of vegetables and water by each individual.
A few samples of cooked vegetables (n = 5) were also collected. All
food samples except cooked vegetables were washed three times
with tap water followed by de-ionized water (twice). Vegetables
were dried in an oven at 65 C and homogenized by grinding them
with a stainless steel grinder. Concentrated nitric acid was used for
the digestion of vegetables; this digestion procedure was reported
elsewhere [21]. Elemental concentrations in vegetables were determined on a dry weight basis. A microwave digestion system (model:
MARS 5, CEM) was used for the digestion of soil using the USEPA
3051 method.
2.2. Sample analysis
An Agilent 7500c (Agilent Technologies, Tokyo, Japan) inductively coupled plasma mass spectrometer (ICP-MS) was used to
determine the amount of As and other elements in vegetables,
water, and soil.
2.3. Analysis of standard reference materials (SRMs)
Standard reference materials (SRMs) from the National Institute
of Standards and Technology (NIST) such as 1640 (trace elements
in natural water), 2711 (Montana soil), and 1573a (tomato leaves)
were used to verify the results for As and other elements in water,
soil, and vegetables, respectively. Montana soil and tomato leaves
were digested after utilizing the same procedure as that used for
soil and vegetable samples. The analytical results of As and other
metals in trace elements in natural water, Montana soil, and tomato
leaves indicate that the observed values are very close to the certied values (Tables 13).
2.4. Consumption of As and other elements by adults
The daily consumption of As and other elements from vegetables
and drinking water by adults in this study is calculated by using the
following equation:
DCE = CRV CEV + CRD CED
where DCE, daily consumption of elements; CRV , median consumption rate of vegetables; CEV , median concentrations of elements
observed in vegetables; CRD , median consumption rate of drinking water; CED , median concentrations of elements observed in
drinking water.
3. Results and discussion
3.1. Contents of As and other elements in drinking water
Table 1 summarises the results for the analysis of As and other
elements present in drinking water. It appears that all drinking
water samples exceeded the recommended level of As for drinking
water set by the WHO (10 g L1 ). The average As concentration in
tubewell water samples was almost 33 times greater than the WHO
recommended level. Only one sample was below the Bangladesh
standard for As (50 g L1 ). With the exception of As, the levels of
other elements were below the WHO guideline values. Currently
there is no WHO guideline value for Mn in drinking water [22],
only one sample exceeded the previous WHO guideline value for

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M.M. Rahman et al. / Journal of Hazardous Materials 262 (2013) 10561063

Table 1
Concentrations of As and other elements in groundwater used for drinking and pond water used for agricultural irrigation of home gardens collected from Noakhali district
of Bangladesh.
Parameter

As
Cd
Co
Cr
Cu
Mn
Ni
Pb
Zn
a

Drinking water (n = 14)


Mean
(g L1 )

Median
(g L1 )

328
<0.05
0.57
0.81
4.64
192
1.24
0.17
23.23

279
<0.05
0.36
0.62
2.33
112
1.03
0.15
7.71

Range
(g L1 )
14772

0.161.31
0.263.17
0.3419.37
21459
0.682.57
0.100.38
0.1389.85

NIST SRM water 1640

Pond water (n = 14)

WHOs guideline
values (g L1 )

No. of samples
exceeding WHO
guideline value (%)

Certied values

Mean
(g L1 )

10
3

50
2000

70
10

14 (100)

26.67
22.79
20.28
38.6
85.2
121.5
27.4
27.89
53.2

Observed
values (n = 3)

0.41
0.96
0.31
1.6
1.2a
1.1
0.8a
0.14
1.1a

26.31
21.85
19.62
35.4
86.2
114.5
26.02
26.97
49.9

0.28
0.67
0.19
0.7
0.8
1.1
0.3
0.10
1.1

2.5
<0.05
0.4
0.8
0.9
153
1.8
0.8
3.9

Reference values.

Table 2
Concentrations of As and other elements (g g1 ) in home garden soils (n = 17) collected from Noakhali district of Bangladesh.
Parameter

As

Cd

Co

Cr

Cu

Mn

Ni

Pb

Zn

Mean
Median
Range
Montana soil Certied/
non-certied values
Montana soil observed values

3.3
2.9
1.59.2
105 8

0.07
0.05
0.030.2
41.7 0.25

10
10
614
10a

29
27
1846
47a

22
21
1363
114 2

303
305
192496
638 28

64
63
3793
20.6 1.1

13
12
822
1162 31

75
71
50116
350.4 4.8

99 4

42.1 0.30

83

41.3 2.8

99 2

589 36

19.1 2.3

1170 32

335.1 4.9

Non-certied values.

Table 3
Concentrations of As and other elements in all vegetables.
Elements

Mean

Median

As (g kg1 )
Cd (g kg1 )
Co (g kg1 )
Cr (mg kg1 )
Cu (mg kg1 )
Mn (mg kg1 )
Ni (mg kg1 )
Pb (mg kg1 )
Zn (mg kg1 )

113
134
216
0.98
18
124
2.1
3.1
55

90
111
168
0.80
13
65
1.78
2.18
50

Mn (400 g L1 ); this samples value was 459 g L1 . Thus out of


14 samples only one was detected where levels of As and Mn were
above 10 g L1 and above 400 g L1 , although the total sample
size was low. Consequently the drinking water sources of the other
13 families were found to be safe with respect to other elements
such as Cr, Mn, Ni, Co, Cu, Zn, Cd, and Pb.

Range

11464
6428
16974
0.184.48
286
4881
0.325.68
0.6716.5
17183

NIST SRM 1573a


Certied values

Observed values

112
1520
570
1.99
4.70
246
1.59

30.9

119
1460
610
1.85
5.01
235
1.68
1.46
32.2

0.004
40
20
0.06
0.14
8
0.07
0.7

3
60
40
0.08
0.19
6
0.08
0.06
0.9

and median As concentrations of agricultural lands in West Bengal, India, were 10.7 mg kg1 and 7.3 mg kg1 , with a range of
3.331.6 mg kg1 [25]. The mean and median As content in this
study was much lower compared to what previous studies have
reported from Bangladesh and West Bengal because As-safe pond
water was used to irrigate home-grown vegetables at the time of
this study. Fig. 1 presents a bar diagram of mean concentrations

3.2. Contents of As and other elements in pond water


The mean concentrations of As and other elements in pond
water used for the irrigation of home-garden vegetables were found
to be safe according to the WHO recommended levels (Table 1).
3.3. Contents of As and other elements in garden soils
The concentrations (mean, median, and range) of As and other
elements in soils are presented in Table 2. Arsenic levels in 71
paddy soils (depth 015 cm) varied from 3.1 and 42.5 g g1 (average: 15.2 g g1 and median: 12.8 g g1 ) in a study reported from
Bangladesh [23]. Another study found that As levels in 25 soils
(depth 015 cm) ranged from an undetectable level to 31.8 g g1
(average: 11.9 g g1 and median: 8.9 g g1 ) [24]. These investigators also reported that As content in soils was positively
correlated with As content in irrigation water [24]. The mean

Fig. 1. Bar diagram of mean concentrations of As and other elements in soils compared with the data reported from As-affected areas of Bangladesh and West Bengal.

M.M. Rahman et al. / Journal of Hazardous Materials 262 (2013) 10561063

of As and other elements in soils compared to the data reported


in previous studies from As-affected areas of Bangladesh and West
Bengal. The mean concentrations of Cr, Cu, Mn and Pb in the examined soils were comparable with the results of the study conducted
in West Bengal [25]. Levels of most of the elements in this study
except Cd and Ni were much lower in the examined soils compared
to the study conducted in Faridpur district of Bangladesh [26].
3.4. Daily consumption of vegetables
The daily vegetable consumption rate for adult males and
females (n = 71, age range 1280 years) was an average of 205 g
(median: 200 g, fresh weight), which is equivalent to 26 g (dry
weight), considering there was on average 87% moisture content
in the vegetables. The vegetable intake rate is much higher than
in the village of Samta, where the average per capita consumption of leafy and non-leafy vegetables is 130 g per person daily
for adults of all ages [4]. The vegetable intake varied from 126
to 169 g daily amongst Bangladeshi adults according to a recent
study in Bangladesh [27]. The villagers in this study area are
socio-economically rich and this could be one reason why vegetable intake was higher compared to other studies conducted in
Bangladesh. The median intake of drinking water among adults was
3 L per day.
3.5. Contents of As and other elements in different types of
home-grown vegetables and compared to other studies
The mean, median, and range of As and other elements in all
vegetables are presented in Table 3. Figs. 24 show concentrations
of Co, As, Cd, Cr, Ni, Pb, Mn, Cu, and Zn in different types of garden
vegetables.
3.5.1. Arsenic
The vegetables with the highest mean As levels were
arum leaf > pumpkin leaf > coriander leaf > radish leaf > gourd
amaranth > arum
stem > Indian
leaf > radish > spinach > red
spinach > arum tuber > bean > papaya > green chilli > eggplant.
Individual vegetable gourd leaves showed the highest As concentration whereas bean exhibited the lowest As content. The
range of As levels in home-grown vegetables from Samta village
in Bangladesh was 19489 g kg1 [4]. The range of As levels
was 703990 g kg1 in vegetables from Chandpur and Jamalpur
districts [6] and <401930 g kg1 in vegetables from Sathkhira,
Rajshahi, and Comilla districts [7]. The range of As levels in this
study was comparable with the results from Samta [4] but much
lower than in another two studies [6,7]. In a recent study, the
range of As levels in 45 vegetable samples collected from Matlab of
Bangladesh was 0.526 g kg1 [12]. A study assessed As and other
heavy metals in vegetables from Jalangi and Domkal blocks of
West Bengal in India and reported that the mean As levels in vegetables were 20.9 g kg1 (<0.04138 g kg1 ) and 21.2 g kg1
(0.04212 g kg1 ) in Jalangi and Domkal, respectively [28].
Both studies [12,28] found very low mean As concentrations in
vegetables compared to other studies undertaken in Bangladesh
and West Bengal.
In the case of leafy vegetables, the mean and median As concentrations were 141 g kg1 and 110 g kg1 , respectively (range:
41464 g kg1 ). The range of As levels in leafy vegetables from
Sathkhira, Rajshahi, and Comilla districts was 100790 g kg1
[7]. On the other hand, the mean and median As concentrations
of non-leafy vegetables were 45 g kg1 and 30 g kg1 (range:
11145 g kg1 ). The range of As levels in non-leafy vegetables
(fruit, root, and tuber) from Sathkhira, Rajshahi, and Comilla districts was <401930 g kg1 [7]. Arsenic levels were much lower
in both leafy and non-leafy vegetables in our study compared to

1059

the previous study [7]. The uptake of metals in vegetables from soil
varies from area to area depending on the concentrations of metals
in soils and irrigation water.
The mean and median As concentrations detected in cooked
vegetables were 356 g kg1 and 288 g kg1 , respectively, with
a range of 98754 g kg1 . Based on 39 cooked vegetable samples
from Munshiganj and Monohordi of Bangladesh, the reported mean
and range of As were 333 g kg1 and 192334 g kg1 , respectively [8]. Although the mean As concentration in cooked vegetables
of this study is comparable to that found in a previous study [8],
the maximum level of As was much lower. This is because all the
families in this study used As-safe pond water for cooking [20].
3.5.2. Cadmium
The vegetables with the highest mean Cd levels were
spinach > coriander leaf > radish leaf > Indian spinach > red amaranth. The Cd concentrations in all vegetables in Samta village
varied between 12 g kg1 and 216 g kg1 [4]. The mean Cd concentration of vegetables from Matlab in Bangladesh was 27 g kg1
[12], which was much lower than that found in our study. Previous study shows that the mean Cd levels in amaranth, bitter
gourd, and eggplant were 33 g kg1 , 21.1 g kg1 , and 27 g kg1 ,
respectively [12]. In our study, the mean concentration of eggplant
was almost 2.8 times higher than that found in a previous study
from Bangladesh [12]. The mean and median Cd concentrations of
leafy vegetables were 163 g kg1 and 144 g kg1 , respectively
(range: 16428 g kg1 ). The mean and median Cd concentrations
of non-leafy vegetables were 58 g kg1 and 24 g kg1 (range:
6265 g kg1 ). The mean and median Cd concentrations in cooked
vegetables were 147 g kg1 and 183 g kg1 , respectively, ranging from 42211 g kg1 . The mean concentrations of Cd in raw
and cooked vegetables are almost the same.
3.5.3. Chromium
The vegetables with the highest mean Cr levels were coriander
leaf > radish leaf > red amaranth > pumpkin leaf > spinach > arum
leaf > gourd leaf. The mean and median Cr concentrations in
leafy vegetables were 1.12 mg kg1 and 0.89 mg kg1 , respectively
(range: 0.354.48 mg kg1 ). The mean and median Cr concentrations of non-leafy vegetables were 0.64 mg kg1 and 0.45 mg kg1
(range: 0.181.91 mg kg1 ). The mean Cr concentration in vegetables of this study was considerably lower than the mean
Cr concentrations detected in vegetables from ve Upazilas
in Feni district of Bangladesh [Dagon Bhuyia (33.84 mg kg1 ),
Feni Sadar (27.37 mg kg1 ), Sonagazi (25.89 mg kg1 ), Pulgazi
(25.28 mg kg1 ), and Parsuram (23.31 mg kg1 )] [11]. The mean and
median Cr concentrations in cooked vegetables were 1.2 mg kg1
and 1.4 mg kg1 , respectively, with a range of 0.581.9 mg kg1 . The
mean Cr level in cooked vegetables was slightly higher than in raw
vegetables.
3.5.4. Cobalt
The vegetables with the highest mean Co levels
arum
tuber > red
amaranth > arum
leaf > coriander
were
leaf > spinach > pumpkin > radish leaf. The mean and median
Co concentrations in leafy vegetables were 252 g kg1 and
228 g kg1 respectively (range: 48644 g kg1 ). The mean
and median Co concentrations of non-leafy vegetables were
127 g kg1 and 58 g kg1 (range: 16974 g kg1 ). Regarding
cooked vegetables, the mean and median Co concentrations
were 147 g kg1 and 85 g kg1 , respectively, with a range of
63227 g kg1 , which is lower than in raw vegetables.
3.5.5. Copper
The vegetables with the highest mean Cu levels were arum
tuber > bean > gourd leaf > arum leaf > Indian spinach > coriander

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M.M. Rahman et al. / Journal of Hazardous Materials 262 (2013) 10561063

Fig. 2. Concentrations of Co, As, and Cd in vegetables.

leaf. The mean and median Cu concentrations in leafy vegetables were 17.3 mg kg1 and 13.7 mg kg1 respectively (range:
4.584.2 mg kg1 ). The mean and median Cu concentrations of
non-leafy vegetables were 20.6 mg kg1 and 11.9 mg kg1 (range:
2.186.3 mg kg1 ). The average Cu concentrations in leafy and
non-leafy vegetables from Samta were 15.5 and 8.51 mg kg1 ,
respectively [4]. The mean Cu level in leafy vegetables of
this study was comparable to that in Samta but the value
was considerably higher for non-leafy vegetables. The mean
Cu level in all vegetables was signicantly higher than the
West Bengal study [28], where the mean Cu levels in vegetables were 1.59 mg kg1 (0.0324.02 mg kg1 ) and 1.58 mg kg1
(0.334.21 mg kg1 ) in Jalangi and Domkal blocks, respectively.
The mean and median Cu concentrations in cooked vegetables were 2.9 mg kg1 and 1.3 mg kg1 , respectively, with a
range of 1.19.3 mg kg1 , which is much lower than in raw
vegetables.

3.5.6. Lead
The vegetables with the highest mean Pb levels were
bean > papaya > arum tuber > arum leaf > coriander leaf. The range
of Pb levels in all vegetables (Table 3) was appreciably higher than
in Samta, where the range of Pb concentrations in all vegetables was
0.1431.689 mg kg1 [4]. The mean and median Pb concentrations
in leafy vegetables were 2.8 mg kg1 and 2.2 mg kg1 respectively
(range: 0.8513.8 mg kg1 ). The mean and median Pb concentrations of non-leafy vegetables were 3.7 mg kg1 and 1.9 mg kg1 ,
respectively (range: 0.6716.5 mg kg1 ). The mean and median
Pb concentrations in cooked vegetables were 6.9 mg kg1 and
3.0 mg kg1 , respectively, with a range of 1.19.3 mg kg1 , which
is almost three times higher than in raw vegetables.
3.5.7. Manganese
The vegetables with the highest mean Mn levels were arum
leaf > pumpkin leaf > gourd leaf > spinach > arum stem > red ama-

Fig. 3. Concentrations of Cr, Ni, and Pb in vegetables.

M.M. Rahman et al. / Journal of Hazardous Materials 262 (2013) 10561063

1061

Fig. 4. Concentrations of Mn, Cu, and Zn in vegetables.

ranth. The mean concentration of Mn in all vegetables was substantially higher than in Jalangi and Domkal, where the mean Mn levels
in vegetables were 3.3 mg kg1 (0.79.49 mg kg1 ) and 4.2 mg kg1
(0.2215.4 mg kg1 ), respectively [28]. The mean and median
Mn concentrations in leafy vegetables were 160.3 mg kg1 and
91.1 mg kg1 , respectively (range: 33.7881.3 mg kg1 ). For nonleafy vegetables, the mean and median Mn concentrations were
34.5 mg kg1 and 27.4 mg kg1 (range: 4.0176.8 mg kg1 ). The
mean and median Mn concentrations in cooked vegetables were
46.1 mg kg1 and 17.2 mg kg1 , respectively, with a range of
13.4113.1 mg kg1 , which is much lower than in raw vegetables.
3.5.8. Nickel
The vegetables with the highest mean Ni levels were
coriander leaf > red amaranth > pumpkin leaf > radish leaf > arum
leaf > spinach. The mean concentration of Ni in all vegetables
was noticeably higher than that reported in the previous study
from West Bengal [28], where the mean Ni levels in vegetables were 0.36 mg kg1 (<0.00021.04 mg kg1 ) and 0.16 mg kg1
(<0.00020.53 mg kg1 ) in Jalangi and Domkal, respectively.
The mean and median Ni concentrations in leafy vegetables were 2.47 mg kg1 and 2.26 mg kg1 , respectively (range:
0.8175.684 mg kg1 ). The mean and median Ni concentrations
in non-leafy vegetables were 1.439 mg kg1 and 1.264 mg kg1
(range: 0.3214.696 mg kg1 ). The mean and median Ni concentrations in cooked vegetables were 1.9 mg kg1 and 1.3 mg kg1 ,
respectively, with a range of 1.013.6 mg kg1 , which is slightly
lower than in raw vegetables.
3.5.9. Zinc
The vegetables with the highest mean Zn levels were red amaranth > arum tuber > pumpkin leaf > spinach > coriander leaf > arum
stem. The average Zn level among all categories of vegetables
was found to be 95.6 mg kg1 (range: 7304 mg kg1 ) [11], which
was greatly higher than in this study. The mean Zn levels in
vegetables were 5.33 mg kg1 (2.019.52 mg kg1 ) and 5 mg kg1
(0.8412.8 mg kg1 ) in Jalangi and Domkal, respectively [28],
which was much lower than in this study. In leafy vegetables,
the mean and median Zn concentrations were 59.6 mg kg1 and
52.2 mg kg1 , respectively (range: 21.4182.9 mg kg1 ), while the
mean and median Zn concentrations of non-leafy vegetables

were 44.3 mg kg1 and 42.7 mg kg1 (range: 17.2122.3 mg kg1 ).


The mean and median Zn concentrations in cooked vegetables
were 38.8 mg kg and 38.9 mg kg1 , respectively, with a range of
24.554.1 mg kg1 , which is lower than in raw vegetables.
The Pearson product-moment correlation co-efcient was used
to discover whether there is any correlation between As and
any other elements. A strong positive correlation (r = 0.74) was
observed between As and Mn in vegetables. The concentrations
of As, Cr, and Pb were higher in raw vegetables compared to the
cooked vegetables and Co, Cu, Mn, Ni, and Zn concentrations were
higher in cooked vegetables than in raw vegetables. Cooking water
may play an important role in this variation. Although two studies
[4,28] were conducted in severely As-affected areas (Samta, Jalangi,
and Domkal) of Bangladesh and West Bengal, respectively, the levels of other metals in vegetables were comparatively lower than
those observed in this study.
3.5.10. Consumption of As and other elements from vegetables
and drinking water
The daily total consumption of As and other elements from vegetables and drinking water for adults is presented in Table 4. The
estimated daily average intake of total As from leafy and non-leafy
vegetables of Samta was 27.8 g day1 [4]. Daily As intake from
vegetables was much lower in this study compared to the previous study [11] where the average estimated As intake of Feni,
Bangladesh, was 105 g day1 . The estimated average daily dietary
intakes of As from vegetables by adults were 10.4 g and 10.6 g
in the Jalangi and Domkal blocks, respectively [28]. The daily As
consumption from vegetables in this study was much lower than
Samta and Jalangi and Domkal blocks. Calculated daily median As
intake from drinking water by adults was 837 g. Adults consume
839 g of As from both drinking water and vegetables. Thus drinking water contributes considerable As to the daily exposure. The
daily As contribution from rice, vegetables and drinking water is
presented in Fig. 5.
In a recent evaluation conducted by the Joint FAO/WHO Expert
Committee on Food Additives (JECFA), the PTDI of As (2.1 g kg1
bw) has been withdrawn and is no longer valid as the inorganic
As lower limit of the benchmark dose for a 0.5% increased the
incidence of lung cancer (BMDL0.5). This was determined from
epidemiological studies to be 3.0 g kg1 bw per day (27 g kg1

1062

M.M. Rahman et al. / Journal of Hazardous Materials 262 (2013) 10561063

Table 4
Daily intake of As and other elements from vegetables and drinking water.
Elements

As
Cd
Co
Cr
Cu
Mn
Ni
Pb
Zn
a
b

Median intake of
vegetables (g) per
day for adults

26

Median
concentration in
vegetables (g kg1 )
90
111
168
800
13a
65a
1700
2100
50a

Intake from
vegetables (g
or mg)
2.3
2.9
4.4
20.8
0.34b
1.7b
46
56
1.3b

Median intake
of water (L) per
day for adults

Median concentration
in drinking water
(g L1 )

Intake from
drinking water
(g)

Total intake from


vegetables and water
(g or mg)

279

0.36
0.62
2.33
112
1.03
0.15
7.71

837

1.1
1.9
7.0
336
3.1
0.4
23.1

839.3
2.9
5.5
22.7
0.35b
2.0b
49.1
56.4
1.3b

Units expressed in mg kg1 .


Units expressed in mg.

bw per day based on the range of estimated total dietary exposure)


using a range of assumptions to estimate total dietary exposure
to inorganic As from drinking water and food [29]. Based on the
average bw of a Bangladeshi adult (45 kg) from Madaripur thana of
Bangladesh [30], vegetables alone contribute 0.05 g of As per kg
bw daily. Both vegetables and drinking water contribute 18.6 g
of As per kg bw daily. The value would be 20 g of As per kg bw
daily, when we combine As contribution from rice (data derived
from [20]), vegetables and drinking water.
The Cu intake from vegetables in this study was half that of the
previous study done in West Bengal [4]. The Provisional Maximum
Tolerable Daily Intake (PMTDI) of Cu is 0.050.5 mg kg1 bw [31].
Both vegetables and drinking water contribute 0.008 mg of Cu per
kg bw daily, which is much lower than the PMTDI value. The estimated average daily dietary intakes of Ni from vegetables for adults
were 180 g and 80 g in the Jalangi and Domkal blocks, respectively [28]. In this study, the Ni intake from both vegetables and
drinking water was much lower than both in Jalangi and Domkal
blocks.
The calculated Mn intake from vegetables for adults in this study
was comparable with the Jalangi and Domkal study [28]. The daily
intake of Mn from vegetables was almost half in this study compared to a study undertaken in Bangladesh, where the value was
3.53 mg [11]. The PTWI of Cd is 7 g kg1 bw [32]. The average daily
intake of Cd from vegetables in Samta village (9.45 g) was much
higher than that observed in our study (2.9 g). Thus, vegetables
contribute only 0.06 g of Cd per kg bw per day, which is equivalent to 0.42 g weekly. As the Cd level in drinking water could not
be detected in this study, drinking water does not add further Cd
to the daily exposure.

The PTWI of Pb is 0.025 mg kg1 bw [33]. The median daily intake


of Pb from vegetables was much lower than in Samta, where the
value was 0.523 mg per week. Thus, vegetables contribute only
1.25 g of Pb per kg bw per day, which is equivalent to 8.77 g
per kg bw per week. So, vegetables alone contribute one-third of
the recommended PTWI of Pb in this study. Drinking water does
not add further Pb to the daily exposure as the Pb level in drinking
water was very low. The PMTDI of Zn is 0.31 mg kg1 bw [34]. The
estimated daily intake of Zn in this study was much lower than that
found in another study in Bangladesh where the value was 87 mg
[11]. The daily intake was three times lower than in Samta village
(3.5 mg) [4]. Zinc intake was lower compared to the Jalangi and
Domkal blocks, where the average daily dietary intakes of Zn from
vegetables by adults were 2.6 g and 2.5 mg, respectively [28]. It
can be stated that vegetables and drinking water contribute 0.03 mg
of Zn per kg bw per day.
4. Conclusions
The concentrations of metals varied extensively among the
different types of vegetables. Leafy vegetables contained higher
concentrations of As, Cd, Cr, Mn, Ni, and Zn than non-leafy vegetables. Vegetables alone contributed an intake of As and other
elements that was below the PMTDI values. The daily intakes of
other elements from other food sources such as rice need to be
evaluated to determine the total exposure to other elements from
the main Bangladeshi foods. Although we collected various types
of commonly consumed vegetables from the study area, they are
not representative of all vegetables consumed by the populations
in other areas of Bangladesh. Food surveys should not be restricted
to As alone; other elements also need to be monitored regularly.
Acknowledgements
The authors thank CERAR, University of South Australia, for
laboratory support. Financial support from CRC-CARE is gratefully
acknowledged. Md. Asaduzzman is grateful to the ATSE Crawford
Fund, Australia, for the fellowship during his training at the CERAR.
The authors are grateful to Dhaka Community Hospital, Dhaka,
Bangladesh for the laboratory support for processing the vegetable
samples.
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Fig. 5. Daily As (g) contribution from rice [20], vegetables and drinking water for
adults.

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