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Concentration of arsenic in groundwater,

vegetables, human hair and nails in mining site
in the Northern Thai Nguyen province, Vietnam:
human exposure and risks assessment

Thi Phuong Mai Nguyen, Thi Phuong Thao Nguyen, Thi Hieu Bui & Thi Hue
Nguyen

To cite this article: Thi Phuong Mai Nguyen, Thi Phuong Thao Nguyen, Thi Hieu Bui & Thi
Hue Nguyen (2018): Concentration of arsenic in groundwater, vegetables, human hair and
nails in mining site in the Northern Thai Nguyen province, Vietnam: human exposure and
risks assessment, Human and Ecological Risk Assessment: An International Journal, DOI:
10.1080/10807039.2018.1483189

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HUMAN AND ECOLOGICAL RISK ASSESSMENT
https://doi.org/10.1080/10807039.2018.1483189

Concentration of arsenic in groundwater, vegetables,

human hair and nails in mining site in the Northern Thai
Nguyen province, Vietnam: human exposure and
risks assessment
Thi Phuong Mai Nguyena , Thi Phuong Thao Nguyena, Thi Hieu Buib, and
Thi Hue Nguyena
a
Institute of Environmental Technology, Vietnam Academy of Science and Technology, Cau Giay, Hanoi,
Vietnam; bNational University of Civil Engineering, Hanoi, Vietnam

ABSTRACT ARTICLE HISTORY

This study was aimed to examine the risk of chronic arsenic (As) Received 26 March 2018
exposure for the residents living in Nui Phao, Thai Nguyen in the Revised manuscript
northern Vietnam. Groundwater, vegetables, human hair, and nail accepted 4 July 2018
samples were collected from volunteers living in Nui Phao. The
KEYWORDS
results revealed that 75% of the groundwater samples had As arsenic; hair-nail; water-
exceeding the World Health Organization (WHO) drinking water vegetables; health
guideline of 10 mg L
1. The result of As concentration for most of risk; mining
the vegetable samples was greater than the WHO/FAO safe
(0.1 mg kg
1). The result of hair and nail samples in this study
showed that 3.5 and 20% of the samples had As concentration
exceeding the level of As toxicity in hair and nails, respectively. The
result of health risks indicated that the potential health risk of As
contamination is greater for groundwater than vegetables. The total
hazard quotient (HQ) value through vegetables ingestion and drink-
ing water exceeded 1.0 suggesting potential health risk for local resi-
dents. The calculation of potential carcinogenic risk through both
consumption of vegetables and drinking water was low cancer risk
in adults. Other food sources and the exposure pathways are needed
to exactly assess health risks in this area.

Introduction
Arsenic (As) is known as a human carcinogen and has been associated with cancer
of the bladder, lungs, skin, and pregnancy-related problems (International Agency
for Research on Cancer [IARC] 2001; United States Department of Health and
Human Services 2003). The consumption of water source or which contaminated As
cause human health problems (Santra et al. 2013; Rasool et al. 2016). High-contami-
nated As in groundwater in West Bengal, India (Das et al. 1995; Samanta et al.
2004; Ahamed et al. 2006) and in Bangladesh (Samanta et al. 1999; Alam et al.
2003; Das et al. 2004; Rahman et al. 2013), in Vietnam (Agusa et al. 2006; Nguyen

CONTACT Thi Phuong Mai Nguyen npmai82@gmail.com Institute of Environmental Technology, Vietnam
Academy of Science and Technology, 18 Hoang Quoc Viet, Cau Giay, Hanoi, Vietnam.
ß 2018 Taylor & Francis Group, LLC
2 T. P. M. MGUYEN ET AL.

et al. 2009; Pham et al. 2017), in Pakistan (Rasool et al. 2016; Rehman et al. 2016),
and in Cambodia (Phan et al. 2010) suggests that human heath in those areas is
affected by As. When As enters the human body, the major portion is excreted in
urine, a small portion accumulates in hair and nail. Thus, hair, urine, and nails has
been used as a biomarker for monitoring the exposure to As in humans (Hunter
et al. 1990; Brima et al. 2006). Hair and nails, however, are considered a useful bio-
marker of chronic As exposure due to ease of collection, storage convenience, and
handling (Gault et al. 2008).
Several studies have revealed that nails and hair As concentration are well-correlated
with As-contaminated groundwater (Das et al. 1995; Yang et al. 2002; Samanta et al.
2004; Conesa et al. 2008; Gault et al. 2008) and indicated that human health was threat-
ened by As ingestion through drinking water. Human exposure to As is not only
through As-contaminated drinking water but also consumption of As-contaminated
vegetables. Some researchers reported that ingestion of As-contaminated vegetable for
long-term residents has a potential cancer risk (Das et al. 2004; Smith et al. 2006;
Rehman et al. 2016; Li et al. 2017). High As concentration in water or food chain is
released from both natural source (Nickson et al. 1998; Berg et al. 2001) and from
anthropogenic activities such as agricultural practices, pesticide, fertilizer application
(Smith et al. 1998; Huang et al. 2006; Zhu et al. 2008), and mining activities (Bui et al.
2016; Li et al. 2017; Long et al. 2018).
In recent years, several researches have been carried out to investigate
consumption of As from vegetables grown, drinking water and its risk assessment to
human health in various areas (Berg et al. 2001; Das et al. 2004; Agusa et al. 2006;
Ahamed et al. 2006; Huang et al. 2006; Gault et al. 2008; Nguyen et al. 2009;
Rahman et al. 2013; Rasool et al. 2016; Rehman et al. 2016; Rasheed et al. 2017).
These researches have been focused on As exposure assessment to human health in
As-contaminated areas by natural source, whereas the human health risks
from anthropogenic activities (e.g. mining activities) has been not assessed. Mining
activities have released heavy metal into the surrounding environment (Navarro
et al. 2008; Wang et al. 2017). Concentrations of As in vegetables and water near
mining areas are affected by mining activities and high concentration of As are
found around mining areas (Liu et al. 2010; Ha et al. 2011; Hajalilou et al. 2011;
Bui et al. 2016; Li et al. 2017). To date, few studied have evaluated accumulation of
As in hair, nail, groundwater, and vegetables in mining exploitation in Nui Phao,
Thai Nguyen. Nui Phao mine, one of the largest operating tungsten mines in
Vietnam, consists of primary wolframite, bismuth, copper, and other elements.
The mining has been explored since 1995 and operated since 2004. Surrounding
environment (e.g. soil, water, air) near mine site and the human health have been
affect by exploration and mining activities. Therefore, the present research will
focus on the As pollution in environment and its potential health risks to
local residents.
The aims of the present study were: (1) to determine the concentration of As in
groundwater, leafy vegetables around mining site; (2) to assess the potential human
health risks associated with vegetables consumption and drinking water through hair
and nails analysis from local people.
 HUMAN AND ECOLOGICAL RISK ASSESSMENT 3

Methods and materials

Study area
Environmental samples were collected in Ha Thuong commute (21 380 1700 B
105 410 2200 D- 21 380 1700 N 105 410 2200 E), near Nui Phao mining area in Thai
Nguyen province. Nui Phao mine is the biggest wolfram mine, which is located in the
Ha Thuong commute, Dai Tu District of the Thai Nguyen province in northern part of
Vietnam. Nui Phao mine is the multi-metal ore exploitation which contains mineral
deposit of tungsten, fluorspar, bismuth, copper, and traces of gold and cover an area of
9.21 km2. The study subject was 84 local people (25–50 years of age) who have lived at
least 5 years in the villages of Ha Thuong commute. They were local healthy farmers
with non-colored or non-treated hair. They do not have smoking habit and use ground-
water source for domestic purpose such as drinking, cooking, bathing, and washing
clothes. The hair and nails samples were collected from these 84 individuals. Hair, nails,
and groundwater samples were collected on the same day from those participants in
this area.

Sampling
Groundwater samples were collected from the tube wells whose depths ranged from 16
to 30 m. Total of 64 groundwater samples were collected from tube well in 500 mL
polyethylene bottles. The samples were acidified with hydrochloric acid until the pH
was <2 and perseverated at 4  C for further analysis. Leafy vegetables (n ¼ 16) were col-
lected from local market in Ha Thuong commute. Leafy vegetables including cabbage,
lettuce, and brassica integrifolia grown in local village were the major food for resident
in this study. Vegetables were taken to local market for human ingestion. The samples
were gathered by hand and packed into ziplock bags, and perseverated at 4  C for fur-
ther analysis. Hair (n ¼ 84) and fingernail (n ¼ 79) samples were collected from 84 indi-
viduals who live in the villages of Ha Thuong near region of multi-metal ore
exploitation. Five nail samples were not collected because of less amount of nails. At
least 1 g of human hair samples was collected from the nape of the head using stainless
scissor. Finger nail samples were collected using stainless steel nail clippers. The hair
and nail samples were sealed separately in labeled polyethylene ziplock bags and stored
in darkness until analyses.

Sample preparation and analyses

Human hair samples were cut into small pieces (0.3 cm). Hair and nail samples were
washed three time with deionized water) and acetone (25 mL) recommended by
Ryabukhin et al. (1978) and Das et al. (1995). Firstly, the nail and hair samples were
treated sequentially with acetone (25 mL, 10 min sonication), then three times with
deionized water (25 mL, 10 min sonication each time) and finally acetone (25 mL,
10 min sonication). After washing, the hair and nail samples were dried at 50–60  C
overnight before to digestion. Hair and nail samples were digested by boiling in a nitric
acid and hydrogen peroxide. Approximately 0.2 g of dry washed hair and nail samples
4 T. P. M. MGUYEN ET AL.

were weighted into cleaned glass tubes of 10 mL, and 3 mL of HNO3 was added, then
1 mL of H2O2 was added, and the tubes were capped, and kept overnight. The glass
tubes were then placed in an Aqualytic (AL38, Dortmund, Germany) at 150  C for
2–3 h until clear solution was obtained. After cooling, the digested samples were trans-
ferred to Teflon cup and was heated at 115  C until the acid evaporated. The samples
digestion was reconstituted to 2 mL of HCl and adjusted to a final volume of 10 mL
with distilled water and transferred to plastic bottles for subsequent analysis. Vegetable
samples were digested in the same manner as the hair and nail samples. For quality
control, a reagent blank, a triplicated sample, and a spiked sample were analyzed in
order to reliability of the analysis results. Standard deviation of As was <5% and the
analytical error was estimated at <10%. The detection limit for As in water, vegetable,
hair, and toenails were 0.001 mg L
1, 0.010 mg kg
1, 0.025 mg kg
1, and 0.025 mg kg
1,
respectively.
Total As in the samples were analyzed by hydride vapor generator an atomic absorp-
tion spectrometer (HVG–AAS 6800; Shimadzu Corporation, Shimadzu, Japan). The
condition of analytical As in solution by HVG–AAS was followed Pham et al. (2017).

Health risk assessment

A health risk assessment is the method in order to give information about non-carcino-
gen and carcinogen effects to individuals who consume As by three ways: inhalation,
ingestion, and dermal contact (Jiang et al. 2015; Rehman et al. 2016). To assess the
human health risk index of As, it is necessary to calculate the average arsenic daily dose
(ADD) through drinking water or ingestion pathway and hazard quotient (HQ). The
average ADD through drinking water and vegetables pathway was given by the USEPA
(2012):
Ci  IRi  EF  ED
ADDig ¼
AT  BW
where ADDig is average daily dose (mg kg
1 day
1), Ci is As concentration in ground-
water and vegetables (mg L
1, mg kg
1), IR is the drinking water consumption
(L day
1) and vegetables ingestion rate (g day
1), EF is the exposure frequency
(day year
1), ED is the exposure duration (years), AT is the averaging time (day), and
BW is body weight (kg).
HQ was calculated flowing the equation below:
ADD
HQ ¼
RfD
RfD is reference dose (RfD ¼ 3  10
4 mg kg
1 day
1 consumption through water
and vegetables were recommended by United Stated Environmental Protection Agency
(USEPA 2012). If HQ is 1, it showed that the human health effect is considered to be
negligible, while HQ is >1, suggesting health effect should be concern.
X
HI ¼ HQ

Hazard index (HI) was the sum of HQ values of vegetables and drinking water. If HI
>1, there is no significant risk of non-carcinogenic effects.
 HUMAN AND ECOLOGICAL RISK ASSESSMENT 5

Table 1. Concentration of As in groundwater and vegetables.

Groundwatera (mg L
1) Vegetablesb (mg kg
1)
n 60 16
Mean ± standard error 0.021 ± 0.019 0.37 ± 0.27
Minimum 0.004 0.05
Maximum 0.082 1.06
a
The legal limit of arsenic in groundwater is 0.05 mg L
1 set by Vietnamese standard.
b
The legal limit of arsenic in vegetables is 0.1 mg kg
1 set by WHO.

Carcinogenic risk (ILCR) can be calculated as:

ILCR ¼ SF  ADD
where SF is the slope factor; slope factor of As is 1.5 mg kg
1 day
1 USEPA (2010).

Results and discussions

Arsenic in water and vegetable
Analytical results of groundwater samples show that As concentration of Nui Phao
range from 4 to 82 mg L
1 with the mean average total As concentration was 21 mg L
1
(Table 1). Six out of sixty samples in Nui Phao were detected at level that exceeded the
Vietnamese standard for As in groundwater (50 mg L
1). However, 75% of groundwater
samples had higher As concentration than WHO drinking water guidelines (10 mg L
1)
suggesting the occurrence of As contamination in this area. Average total As concentra-
tion was higher in present study compared to a study done in Hanoi, Vietnam where
the value is 11 ± 14 mg L
1 (Agusa et al. 2006). Concentrations of As in groundwater
were lower than that found in another study in Bangladesh (Rahman et al. 2013), in Ha
Nam province, Vietnam (Nguyen et al. 2009), and in Cambodia (Gault et al. 2008;
Phan et al. 2010). The results of average total As concentration in groundwater was
lower than the concentration of As in groundwater samples (43 mg L
1) from
Lianhuashan tungsten mining in China (Liu et al. 2010) possible because of the differ-
ence of the mining activities time.
The concentrations of As in 16 vegetables samples in the study area shown in Table
1. The mean As concentration was 0.37 ± 0.27 mg kg
1, all of which were lower than
the safe maximum allowable limit MAL (1 mg kg
1) established by Australia for agricul-
tural food crop, while 31% of the sample has As concentration higher than the Chinese
National Standards (0.5 mg kg
1) for As in vegetables (Li et al. 2017). Nevertheless, the
mean concentration of As in most of vegetable samples were exceeded the MAL
(0.1 mg kg
1) set by WHO/FAO. The results started that As levels in vegetables col-
lected from near mining area were lower than of leaf vegetables (with a mean of
0.59 mg kg
1) collected from Shihupu village near the East River of the Shizhuyuan
mining area in China (Li et al. 2017), and the vegetable (with an average of
0.63 mg kg
1) grown on Lianhuashan tungsten mining area (Liu et al. 2010), and the
vegetables (with an average 0.81 mg kg
1) grown near Bac Kan mining area, Vietnam
(Bui et al. 2016). The average As concentration in vegetables collected from near Nui
Phao mining area was greater than the As the vegetables (with a mean of 0.09 mg kg
1)
from As-contaminated area of Bangladesh observed by Rahman et al. (2013). The
6 T. P. M. MGUYEN ET AL.

Table 2. Summary of As in hair and nail.

Haira (mg kg
1) Nailb (mg kg
1)
N 86 79
Mean ± standard error (mg kg
1) 0.29 ± 0.19 0.67 ± 0.30
Mean 0.22 0.52
Minimum 0.12 0.36
Maximum 1.84 1.67
a
Normal amount of As in hair is about 0.08–0.25 mg kg
1, with 1.0 mg kg
1 being an indication of toxicity (Arnold
et al. 1990).
b
Normal As content in nails is 0.43–1.08 mg kg
1 (Ioanid et al. 1961).

results of leafy vegetables in the study were consistent with the finding of Alam
et al. (2003).

Arsenic contamination in hair and nail

Table 2 insulates the concentrations of total As in hair and nail. The normal concentra-
tion of As in hair for people living in a non-contaminated environment ranges from
0.08 to 0.25 mg kg
1. Hair As level in excess of 1 mg kg
1 normally indicates toxicity
recommended by WHO (2001), Hashim et al. (2013), and Arnold et al. (1990). Dart
(2004) suggested that hair As concentration for patients with chronic poisoning ranged
from 1 to 5 mg kg
1, but it is often exceeded the value of 10 mg kg
1. In this study, the
As concentration in hair ranged from 0.12 to 1.84 mg kg
1 with an average of
0.29 ± 0.19 mg kg
1, while 3.5% of the samples had As concentration exceeding the level
of As toxicity (1.00 mg kg
1) (Figure 1).
The normal As concentration in nails ranged from 0.43 to 1.08 mg kg
1,
1.08 mg kg
1 indicates toxicity (Ioanid et al. 1961; WHO 2001; Rahman et al. 2005).
The As concentration in nail ranged from 0.36 to 1.67 mg kg
1, with a median nail As
concentration of 0.67 ± 0.30 mg kg
1, while 20% of the samples had As concentration
above the normal As content in nails is 0.43–1.08 mg kg
1 (Figure 2). As levels in
human hair and nail in present study were much lower than those of the As-contami-
nated areas such as Bangladesh and West Bengal, India (Samanta et al. 1999) and the
As concentration in human hair (with a mean value of 1.41 mg kg
1) and nails (with a
mean value of 1.90 mg kg
1) in Kandal, Cambodia (Gault et al. 2008). The concentra-
tion in hair found in our study was comparable with that of the local people from As-
contaminated areas of in Thanh Tri and Gia Lam Districts, Hanoi with an average of
0.54 mg kg
1 (Agusa et al. 2006). The As concentrations found in the human hair sam-
ple were similar to the concentration of the hair samples in the contaminated area in
Hanam (from 0.12 to 1.09 mg kg
1) (Nguyen et al. 2009). The reason could be due to
the difference in As levels in groundwater, which would lead to different accumulated
As level. Indeed, As concentration in groundwater in the present study ranged from 21
to 82 lg L
1 while As-contaminated groundwater in Cambodia ranged from 0.21 to
943 lg L
1 (Gault et al. 2008) and the range of As in Hanoi was from <0.1 to
330 lg L
1 (Agusa et al. 2006).
As concentration in groundwater is significantly correlated (Spearman’s r ¼ 0.52,
p<.01) with As concentration in human hair (Figure 3). This result showed that con-
sumption of As contaminated in groundwater possibly resulted in high accumulated As
in human body. The correlation between As concentration in groundwater with nails
 HUMAN AND ECOLOGICAL RISK ASSESSMENT 7

Total As standard limit

1.4
Normal amount of As

As concentration in hair (mg Kg-1)

1.2 Normal amount of As

0.8

0.6

0.4

0.2

0
0 20 40 60 80 100

Figure 1. Concentration of As in human hair samples.

Normal amount of As
1.8
Normal amount of As
As concentration in nail (mg Kg-1)

1.6
1.4
1.2
1
0.8
0.6
0.4
0.2
0
0 20 40 60 80 100

Figure 2. Concentration of As in nail samples.

(r ¼ 0.26, p < .01) was lower than that with human hair because the local peoples often
has cut their nails. These results indicated that human hair is used as a good reflection
of long-term exposure compared with nails. The result suggested that groundwater pos-
sibly is one of the sources of As exposure to human health.

Arsenic risk assessment

Average daily dose and hazard quotient
In this study, Nui Phao mining has been exploited since 1995, therefore, assumed that
groundwater has been used as drinking water for 14 years (1995–2009). All parameters
were evaluated according to the biological factor of the Vietnamese people and local people
have used groundwater as the main source for drinking water. The values of principal fac-
tors that have been selected in the exposure assessment calculation were listed in Table 3.
The values of ADI and HQ for As via food ingestion and drinking water for resi-
dent’s Nui Phao showed in Table 4. The obtained results shown that the ADI values for
As through drinking water (2.90  10
4 mg kg
1 day
1) were higher than those inges-
tion vegetables (1.86  10
4 mg kg
1 day
1). The ADI values showed that the As intake
for local people through drinking water and vegetables feeding was lower than the RfD
8 T. P. M. MGUYEN ET AL.

Table 3. Parameters used for the calculation of ADD, HQ, and ILTCR.
Parameters Symbol Unit Values References
Total As in vegetables Cveg mg kg
1 Presented in Table 1 This study
Total As in groundwater Cw mg L
1 Presented in Table 1 This study
Ingestion rates of leafy vegetables IRveg g day
1 100.4 Jiang et al. (2015)
Ingestion rates drinking water IRw L day
1 2 Rasool et al. (2016)
Nguyen et al. (2009)
Exposure frequency EF days year
1 365 Nguyen et al. (2009)
Exposure duration ED year 14 This study
Body weight Bw kg 55 Nguyen et al. (2009)
Averaging time AT day 18,250 Nguyen et al. (2009)
As reference dose RfD mg kg day
1 0.0003 USEPA (2012)
Cancer slope factor SF kg day mg
1 1.5 for adult USEPA (2012)

1.4
Arsenic in human hair (mg kg-1)

1.2
1
0.8
0.6
0.4
0.2
0
0 0.02 0.04 0.06 0.08 0.1
Arsenic in groundwater (µg L-1)

Figure 3. Correlation between As concentration in human hair and groundwater.

limit (3.0  10
4 mg kg
1 day
1) set up USEPA (2012); however, the total ADI values
(4.76  10
4 mg kg
1 day
1) was exceeded the RfD limit.
The HQ was used to assess the potential health risk through consumption of As con-
tamination in drinking water and vegetables. In this study, the HQ values of As through
consumption of vegetables or drinking water are <1.0. The measured HQ value was 1.5
times higher for drinking water (9.67  10
1) than through ingestion of vegetable
(6.20  10
1), suggesting the potential health risk of As contamination is greater for
groundwater than vegetables. The HI (total HQ) value through vegetables ingestion and
drinking water exceeded 1.0 (Figure 4) indicating potential health risk for this resident.
These results stated that vegetable ingestion and drinking water may have caused high
As accumulation in nail and hair in this area. The HI value through ingestion of vegeta-
bles and groundwater in this study was higher than Pakistan. The HI value was much
lower in this study compared with previous study in the Shizhuyuan mining area,
China (Li et al. 2017). The HI value in this study was similar to the result observed in
Cho Don mining area in Vietnam (Bui et al. 2016).
The ILCR values revealed that the cancer risk was 4.3 extra individuals per 10,000 for
adults through drinking groundwater in the study area, while the values was 2.9 individ-
uals per 10,000 via ingestion of vegetables. According to USEPA (2012), the ratio 1 in
1,000,000 is considered to be safe standard for carcinogenic risk. In the present study,
the overall potential carcinogenic risk through consumption of vegetables and drinking
water was about seven individuals per 10,000 suggesting there is low cancer risk in
adults. The ILCR data of As through vegetables ingestion in this area were lower than
those vegetables from Southern Pakistan (Rehman et al. 2016).
 HUMAN AND ECOLOGICAL RISK ASSESSMENT 9

2
Vegetables
Groundwater
1.5

Total HQ value
1

0.5

0
Risk index of adult

Figure 4. Total HQ values of As due to consumption of vegetables and groundwater.

Conclusion
As concentrations in groundwater samples of the mining area showed that 75% of
the studied groundwater exceeded the WHO (0.01 mg L
1) suggesting As removal
from groundwater before using as drinking water. The result of As concentration for
most of the vegetable samples was greater than the WHO/FAO safe (0.1 mg kg
1).
The result of hair and nail samples in this study showed that 3.5 and 20% of the
samples had As concentration exceeding the level of As toxicity in hair and nails,
respectively. These results indicated that As accumulation in hair and nail samples
was possibly related to As contamination in groundwater and vegetable samples in
this study, demonstrating that the residents have been exposed to As through drink-
ing water and consumption vegetables from As-contaminated area of Nui Phao, Thai
Nguyen. The result indicated that the potential health risk of As contamination is
greater for groundwater than vegetables. The total HQ value through vegetables
ingestion and drinking water exceeded 1.0 suggesting potential health risk for this
resident. The calculation of potential carcinogenic risk through both consumption of
vegetables and drinking water was 7.14  10
4 suggesting there is low cancer risk in
adults recommended by USEPA (2012) in this study. However, vegetable samples
were small and not representative of all vegetables in this study. Further research
study to investigate the concentration of As in other foods, soil and contact path-
ways to assess exposure to human is needed.

Disclosure statement
No potential conflict of interest was reported by the authors.

ORCID
Thi Phuong Mai Nguyen http://orcid.org/0000-0003-3074-6535

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