Ecotoxicology and Environmental Safety 171 (2019) 737–745

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Ecotoxicology and Environmental Safety

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

Health risk assessment of potentially harmful elements in subsidence water T

bodies using a Monte Carlo approach: An example from the Huainan coal
mining area, China
⁎ ⁎⁎
Guangzhou Chena,b, , Xingming Wangc, Ruwei Wangd, Guijian Liud,
a
Anhui Province Key Laboratory of Water Pollution Control and Wastewater Reuse, Anhui Jianzhu University, Hefei 230601, China
b
School of Environment and Energy Engineering, Anhui Jianzhu University, Hefei 230601, China
c
School of Earth and Environment, Anhui University of Science and Technology, Huainan 232001, China
d
CAS Key Laboratory of Crust-Mantle Materials and Environment, School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026,
China

A R T I C LE I N FO A B S T R A C T

Keywords: Enrichment of potentially harmful elements in surface water results in ecological risk to the surrounding en-
Potentially harmful elements vironment. Assessing the environmental risk of these elements is of great importance. In this study, surface water
Health risk assessment samples from 6 different subsidence water bodies in the Huainan coal mining area were collected. The con-
Monte Carlo simulation centrations of Cu, Ni, Pb, Cd, Co, Cr, V, Fe, Mn and Zn were measured by atomic absorption spectrophotometry,
Subsidence water bodies
and those of As and Hg were analyzed by atomic fluorescence spectrometry. Then, human health risks through
Coal mining area
the ingestion and dermal contact pathways were assessed and analyzed on the basis of a Monte Carlo simulation.
The mean and 95th percentile risks were reported. The results showed that the total carcinogenic risk values in
every subsidence water body summed for Cr, Ni and As via two exposure pathways were greater than the
maximum acceptable level (1 × 10−4), and Xinji’er water body had the highest carcinogenic risk. Among three
elements, Ni was the highest contributor to carcinogenic risk. All non-carcinogenic health risk (hazard quotients)
values except for one water area of Co (Xinji’er) were less than 1; however, the total non-carcinogenic health
risks of two water bodies (Xinji’er, Xinjiyi) summed for all the elements based on mean concentrations were
higher than 1. Xinji’er had the highest hazard index. The extent of the impacts of the total hazard quotients
followed the order of Co > As > Cd > Hg > Pb > V > Fe > Ni > Mn > Zn > Cr. Furthermore, the total hazard
quotients of Co and As via ingestion pathway summed for the six subsidence water areas were greater than 1,
which should be a concern.

1. Introduction
As an important industrial resource and the primary energy source,
coal plays an important role in economic development in China. At
present, China is the largest coal consumer and producer (Cao et al.,
2014; Dai et al., 2012). Coal contains many types of potentially harmful
elements and metalloids, which are discharged into the environment in
large amounts during the production, washing and other processes (Dai
et al., 2012; Wang et al., 2010). In addition, the exploration of coal
causes changes to ecological factors such as surface morphology, hy-
drology, climate, biology, and especially ground subsidence (Lian and
Wang, 2011; Xu et al., 2012). Gradually, water bodies are formed in the
areas of some ground subsidence, which become specific surface water
bodies. As a result of low terrain, leaching water from coal gangue piles,
domestic sewage and farmland drainage more easily flow into the water
bodies (Ouyang et al., 2018). Given the large areas of subsidence wa-
ters, the idea of building a plain reservoir has been proposed. Therefore,
an investigation of the water quality in the subsidence areas is of sig-
nificant importance for the development and utilization (such as
aquaculture industry).
In general, potentially harmful elements are poisonous and difficult
to biodegrade. They are easily released to many environmental media
and may enter the human body through the following three pathways:
inhalation exposure, dermal contact and ingestion (Cao et al., 2014). It
has been considered that potentially harmful elements may still be
harmful at detected levels (Clarke and Cummins, 2014). Increasingly,

⁎
Corresponding author at: Anhui Province Key Laboratory of Water Pollution Control and Wastewater Reuse, Anhui Jianzhu University, Hefei 230601, China.
⁎⁎
Corresponding author.
E-mail addresses: chgzh@ahjzu.edu.cn (G. Chen), lgj@ustc.edu.cn (G. Liu).

https://doi.org/10.1016/j.ecoenv.2018.12.101
Received 19 April 2018; Received in revised form 15 December 2018; Accepted 29 December 2018
0147-6513/ © 2019 Elsevier Inc. All rights reserved.
G. Chen et al. Ecotoxicology and Environmental Safety 171 (2019) 737–745

Fig. 1. Study area and sampling points in the study area.

there is evidence to show the negative health effects of cumulative, and non-carcinogenic health risks via the ingestion pathway and dermal
lower-level exposures to some metals (Tchounwou et al., 2012). contact pathway based on a Monte Carlo simulation; and 3) to analyze
Therefore, the presence of potentially harmful elements in Surface the uncertainty in the health risk assessment.
water, Groundwater and Top water (Cao et al., 2017; Clarke et al.,
2016; Haque et al., 2016; Khan et al., 2016; Nawab et al., 2016;
2. Materials and methods
Rupakheti et al., 2017; Wu et al., 2009); Soils (Chen et al., 2015;
Guagliardi et al., 2018; Guney et al., 2010; Li et al., 2014; Miguel et al.,
2.1. Study area and locations of the samples
2007; Tepanosyan et al., 2017); Sediments (Q.Q. Cao et al., 2015a;
Zuzolo et al., 2017); Fish (Gilbert et al., 2017; Li et al., 2015; Wang
The Huainan coalfield, located in the mid-northern part of the
et al., 2015); Cultivated topsoil and Grain (Zhao et al., 2014); Urban
Anhui Province, is one of thirteen billion-ton coal bases in China, and
topsoil (Buttafuoco et al., 2017); Size-fractionated particle-bound
covers approximately 3200 km2. In addition, Huainan, a city built re-
(Huang et al., 2016) and Multiple media (Cao et al., 2014, 2015b; Doabi
lying on the coal mine, is a large-scale base with coal, power and
et al., 2018) has gained the attention of many scholars.
chemical industries. The climate is warm and semi-humid. The annual
Focused on the Huainan mining area, some previous studies in-
mean precipitation and temperature are 922.6–926.3 mm and 15.2 °C,
vestigated the occurrence of As, Se, Hg, Cd, Co, Cr, Cu, Fe, Mn, Pb and
respectively (Fang et al., 2015). Mining activities have occurred in the
Zn in the subsidence pools (Liu et al., 2009; Yao and Gui, 2008); and
area for over 100 years, and more than 10 coal mines are presently in
Cd, Hg, Cu, Pb, As in soil (Yao et al., 2010). In recent years, the con-
production. In 2016, raw coal production was 77.354 million tons. The
centrations of Pb, Cd, As, Zn and Cu in water samples from the sub-
long duration of mining activities over the years led to the formation of
sidence pools around the coal waste rock piles (Panyi, Guqiao mine
many deep and large subsidence waters. By the end of 2013, the total
area) were measured, and the health risk was evaluated (Wang et al.,
subsidence area was approximately 220 km2 (Wei et al., 2016). By the
2012). After that, Cu, Pb, Cd and Zn in the water of subsidence pools
end of 2015, the area had reached to approximately 245 km2 (Ouyang
and different fish tissues were tested (Wang et al., 2015). Aimed at the
et al., 2018). With the continuation of coal mining activities, the sub-
changes of water quality between months, water samples from the
sidence area is also growing. To determine the risk of potentially
Guqiao, Panyi and Xinzhuangzi mining areas in April, June, August and
harmful elements of the subsidence water bodies, six subsidence water
October were tested (Wei et al., 2016).
bodies were selected, which included two new subsidence areas (near
The above studies for the Huainan coal mining area carried out a
the Zhuji and Pandong mine), two middle subsidence areas (near the
determination of concentrations and risk evaluation of potentially
Xinji’er and Zhangji mine), and two old subsidence areas (near the
harmful elements. While some achievements were obtained, relatively
Panyi and Xinjiyi mine). It was relatively divided into three categories
few types of the potentially harmful elements were tested, and they
in this study according to the formation time: new water body(less than
involved few sampling water areas. Moreover, to assess risk, they em-
10 years), medium water body (10–20 years), old water body (greater
ployed the deterministic risk assessment method, which produced
than 20 year). Their brief information is seen in Table S1.
single risk values used to assess the health risks (Giri and Singh, 2015;
Li and Zhang, 2010; Zeng et al., 2009). And again, the uncertainties of
the health risk assessment were not quantitatively considered; however, 2.2. Collection of water samples and test
there is an inherent link between risk assessment and uncertainty (Li
et al., 2006; Mesa-Frias et al., 2012). Therefore, to more definitively The surface water samples were collected using polyethylene plastic
determine their further harm on human health risk, a comprehensive buckets by vertical water sampler or sampling pump under the pressure
health risk assessment is needed. of manpower. At every subsidence water body, three water samples
The objectives of this study are 1) to investigate the magnitudes of were collected every certain distance along the shore of the water body.
twelve potentially harmful elements contaminants (Hg, Cr, Co, Pb, As, There are six different subsidence water bodies selected, totally eigh-
Mn, Cd, Cu, Zn, Ni, V and Fe) from three different subsidence periods teen surface water samples were sampled. The distribution of sampling
(new, medium and old), which reflect the length of formation time for points is shown in Fig. 1.
the subsidence water bodies; 2) to evaluate the potential carcinogenic Samples collected at the end of November, 2016, were analyzed for
Cd, Cr, Pb, Mn, Cu, Zn, Ni, Co, V and Fe. To make up for the first

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leakage test of Hg and As, the samples collected in May 2017 were
analyzed for Hg and As. Water samples were stored in a large plastic
box, which was protected from light. Then, they were sent to the lab
and stored in the dark. Subsequently, the water samples were sent to
the Experimental Center Laboratory of Anhui Hydrological Engineering
Investigation and Research Institute and tested as soon as possible.
All tests were carried out in strict accordance with Chinese national
standard test methods (GB/T 5750.6-2006, GB/T8538-2008). The ele-
ments of Cu, Ni, Pb, Cd, Co, Cr and V were measured by graphite fur-
nace atomic absorption spectrometry (A3AFG, China); Fe, Mn and Zn
were measured by atomic absorption spectrophotometry (TAS990F,
China); As and Hg were analyzed by atomic fluorescence spectrometry
(AFS9700, China). Quality assurance and control measures were
adopted. The measures are as follows: (1) Parallel double sample
method: 10% of the samples are randomly selected to carry out a
comparison test of parallel double samples for each batch, and the re-
lative deviation should be within the allowable value (3%); (2) A
standard reference solution (quality control sample) is compared and
analyzed; standard reference solutions with a known concentration of
the analyzed metals and samples were tested synchronously, and the
deviation value should be within the required range (5%).
2.3. Statistical analysis methods
The descriptive statistical characteristics of the concentration vari-
ables were expressed as the mean, minimum, maximum, standard de-
viation (S.D.), skewness, kurtosis and coefficient of variation (CV%). A
correlation matrix was used to highlight the strength of the inter-
relationship between two potentially harmful elements for the eighteen
water samples. The correlation was tested by a Pearson correlation
analysis. To analyze the concentration differences between the six
subsidence water bodies, a one-way analysis of variance (ANOVA) was
employed. In addition, the concentration differences from the different
subsidence time were analyzed based on the ANOVA method. The
statistical tests were done by SPSS 22.0. The level of p < 0.05 was
selected as statistically significant.
2.4. Exposure and health risk assessment
Potentially harmful elements may enter the body via three main
pathways: inhalation, ingestion and dermal absorption. As far as metals
in a water environment are concerned, direct water ingestion and
dermal contact are predominant (Kim et al., 2004; Saha et al., 2017; US
EPA (2004); Wu et al., 2010). Therefore, in this study, the pathways of
ingestion and dermal contact were considered.
2.4.1. Chronic daily intake (CDI)
The chronic daily intake (CDI, mg kg−1day−1) of an element in
water via the ingestion pathways and dermal contact exposure can be
computed by employing Eqs. (1) and (2), respectively (Cao et al., 2017;
Saha et al., 2017; Zheng et al., 2013).
C × IR × EF × ED
CDIingestion =
BW × AT (1)
C × SA × Kp × ET × EF × ED ×10
CDIdermal =
BW × AT (2)
where C represents the concentration of the potentially harmful ele-
ments in the subsidence water sample, in mgL−1; IR is the daily inges-
tion rate in Ld−1; EF is the exposure frequency in days year−1; ED is the
exposure duration, where 70 years is used for a carcinogen and 30 years
is used for a non-carcinogen; BW means the body weight in kg; AT
represents the average exposure time (AT = 365 × ED) in days; SA
means the surface area of the skin in m2, which is exposed to pollutants;
Kp represents the permeability coefficient through the skin under water
exposure (cm h−1); and ET represents the exposure time (h day−1).
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Ecotoxicology and Environmental Safety 171 (2019) 737–745
2.4.2. Carcinogenic risk
The incremental lifetime cancer risk can be computed as the in-
cremental probability of an individual, who develops cancer over a
lifetime due to exposure to a potential carcinogen. The incremental
lifetime cancer risk is defined to be (USEPA, 2011):
ILCR = CDI × SF (3)
−1 −1 −1
where SF expresses the cancer slope factor ((mg kg day ) ).
According to USEPA, as far as cancer risk is concerned, there is a range
of acceptable risk levels. If the value of the carcinogenic risk is low than
or equal to 10−6,then it is considered to be negligible; if the value is
larger than 10−4, then it is considered to be unacceptable; if the value is
between 1 × 10−6 and 1 × 10−4,then it should be discussed in the
light of the circumstances.
Assuming they have additive effects, the cancer risks of multiple
carcinogenic contaminants from all carcinogens and exposure routes
are added. In particular, aimed at the carcinogenic risk from a single
element, the allowable risk limit is set to 1 × 10−6, while the allowable
limits for the carcinogenic risk from multiple elements are < 1 × 10−4
(RAIS, 2017).
2.4.3. Non-carcinogenic risk
The non-carcinogenic risk is defined as:
HQ = CDI /RfD (4)
where HQ is the hazard quotient (unitless), and RfD represents the
reference dose for the corresponding element (mg kg−1 d−1). If the HQ
exceeds unity, there may be concern for this element. To compute the
total potential value for non-carcinogenic risks caused by a variety of
hazardous substances, the hazard index (HI) was computed as:
n
HI = ∑i =1 HQi (5)
where i shows the different elements. An HI < 1 indicates no sig-
nificant risk of negative health effects for the certain exposure pathway,
while an HI > 1 denotes a possibility of adverse health effects. The
total exposure hazard index was employed to express the non-cancer
risks from the diverse exposure pathways and computed by the fol-
lowing expression (USEPA, 2011):
n
HIt = ∑ j=1 HIj
(6)
where j represents the different exposure pathways.
2.5. Monte Carlo simulation and uncertainty analysis
2.5.1. Monte Carlo simulation
By employing statistical sampling techniques, a Monte Carlo simu-
lation (MCS) can obtain a probabilistic approximation of the solution
(Firestone et al., 1997; Thompson et al., 1992). That is, it is a prob-
ability density function for the output, which is contrasted with de-
terministic methods. Compared to the deterministic method, interval
estimation based on MCS can enhance the understanding of the en-
vironmental behaviors of contaminants and show the uncertainties
(Cao et al., 2017; Koupaie and Eskicioglu, 2015; Mari et al., 2009; Saha
et al., 2017). Therefore, MCS has recently become increasingly common
in environmental health and safety risk assessments (Jokic et al., 2013).
The main steps are as following: (1) Define the distribution functions of
the variables; (2) Sample randomly from the above distribution of the
variables; and (3) Carry out repeated simulations using the parameter
series selected randomly and output the probability distribution of si-
mulation results.
Health risks (carcinogenic and non-carcinogenic) in this study were
computed using a MCS, which was performed by the aid of Crystal Ball
software in this paper. The software is a preferable Monte Carlo mod-
eling tool that is widely used. Log-normal and triangular probability
distribution functions for the variables were employed. The number of
G. Chen et al.
Table 1
Monte Carlo parameter distributions and values used in the health risk assessment via ingestion and the dermal contact.
Parameters Distribution (Saha et al., 2017)
IR(the daily ingestion rate) Log-normal
BW(body weight) Log-normal
SA(surface area of the skin) Log-normal
EF(exposure frequency) Triangular
ET(exposure duration) Triangular
Note: C, ED, AT, Kp and RfDi are constant in the computing of Monte Carlo. Kp of Cd, Cr, As, Fe, Mn, Co, V and Hg were 1 × 10−3 cm h−1; Kp of Pb is 1 × 10−4
cm h−1; Kp of Zn is 6 × 10−4 cm h−1; Kp of Ni is 2 × 10−4 cm h−1, these data come from the Exposure Factors Handbook (USEPA).
iterations for every run was set to 10,000. Considering the actual
change range of the variables, the uncertainty range was set based on
the types of parameter distributions. The detailed information is sum-
marized in Table 1.
The mean, standard deviation and the 95th percentile risk results
were obtained. The histogram and cumulative probability distribution
curve of the risk assessment result were then obtained from the outputs.
2.5.2. Sensitivity and uncertainty analysis
A sensitivity analysis that is based on the rank order of the corre-
lation or contributions is employed to judge the significance of the
input variables to the risk estimation. Based on the results of the MCS, a
sensitivity analysis can be conducted.
An uncertainty analysis is utilized to assess the reliability of the risk
evaluation results. Model and parameter uncertainties are the two main
sources of uncertainty, which affect the accuracy of the evaluation re-
sults (Abdo et al., 2017). The causes of uncertainty have the following
sources: their stochastic nature, measurement errors, and lack of in-
formation and data (Lek, 2007; Neshat et al., 2015; Saeedi et al., 2008).
The evaluation methods for uncertainty include a Monte Carlo analysis,
the Taylor method, a probability tree, a sensitivity analysis and a
confidence interval (Xue and Li, 2012). A detailed summary was pre-
sented in the paper about the human health risk assessments (Dong
et al., 2015).
MCS is a common method that is used to assess uncertainty by
means of probability distribution functions. In this research, the models
of potentially harmful elements through ingestion and dermal contact
pathways were selected and used; therefore, only the uncertainties of
the input parameters of the model were considered.
3. Results and discussion
3.1. Concentrations of potentially harmful elements
The concentrations of potentially harmful elements in the sub-
sidence water bodies are shown in Table S2. Seen from the Table S2, Fe,
Zn and Mn presented the relatively higher mean levels, while Cu was
only detected in one sample. One reason is relatively higher soil
background values in Huainan, and the other comes from the Human
activities (agricultural and mining activities). The mean concentrations
of the different elements followed a decreasing order: Fe > Zn >
Mn > V > Ni > Co > As > Pb > Cr > Cd > Hg.
Considering water quality standards (environmental quality stan-
dard of surface water, GB3838-2002, China), the concentrations of Hg
from four water bodies exceeded the standard identified for grade III
waters, and this result agreed with a previous study, where the con-
tamination of Hg was found to be notable (Liu et al., 2009). The con-
centrations of Fe from three water bodies exceeded the standards of
additional items for centralized drinking water sources; and those of Ni
from two water bodies exceeded the standard of specific indicators for
centralized drinking water sources.
The concentrations were shown in Fig. 2 by using the boxplots
(OriginPro 2017). Fig. 2 indicated the distribution characteristics of the
concentrations, and the fitting effects where the normal distribution
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Ecotoxicology and Environmental Safety 171 (2019) 737–745
Mean SD Units Uncertainty range
2.2 0.34 L −30% to 10%
70 10.71 kg −30% to 20%
1.8 0.092 m2 −10% to 10%
– – day 350(180–365)
– – h 0.58(0.4–0.7)
was employed. As seen in Fig. 2, the distribution of V was close to the
normal distribution, while the other potentially harmful elements
showed the characteristics of a non-normal distribution.
3.2. Results of statistical analysis
The coefficient of variance (CV) indicates the degree of variability
within the concentrations in the different water samples. As seen in
Supplementary Table 2, Pb, Ni, Cd, As, Fe, V, Co, Zn and Cr had a high
variability (Doabi et al., 2018), which is probably related to human
activities. The Pearson correlation analysis showed that Cd was posi-
tively related to Pb and Co at the 0.01 level; Pb was positively related to
Co at the 0.01 level; Fe was positively related to Cd, Pb and Co at the
0.05 level (Table S3). Therefore, Cd, Pb, Co and Fe might have the same
origin.
A one-way ANOVA from the different subsidence water bodies
showed that the concentrations of Cd, Cr, Pb, Ni, Fe, Co, V and As were
different in the different subsidence water bodies (Table S4(1)). This
result was consistent with the result of the coefficient of variation.
As for the different subsidence periods, the concentrations of Fe, Ni,
Pb and V showed the significant difference (Table S4(2)); Ni and Fe
showed the higher concentrations in middle subsidence water bodies of
mining. Cr showed the lower concentrations in old subsidence water
bodies of mining, while its significant test was not passed. The possible
reasons are:(1) the background values of surrounding soil; (2) the ele-
ment composition and release rule of coal gangue;(3) exchange be-
tween different media. About the change of different months, previous
study suggested that the concentrations of As, Cd, Pb and Cu were high
in April and June; those of Cr, Ni and Mn were high in August and
October; and those of V and Zn were basically not changed (Wei et al.,
2016).
3.3. Carcinogenic health risk
Five elements (Cr, Cd, As, Ni and Co) are classified as possible
carcinogens by the International Agency for Research on Cancer (IARC,
2013). The RfD and SF employed in this study are listed in Table S5
(Cao et al., 2014; Gilbert et al., 2017;Li and Zhang, 2010; Miguel et al.,
2007; Tepanosyan et al., 2017). Because of no SF of Cd and Co, two
ways of ingestion and dermal contact for Cr, As and Ni were considered
to assess human exposure. By comparison, it could be known that which
kind of exposure path was more harmful.
3.3.1. Assessment results of the two pathways
The evaluation results of the carcinogenic risk from six subsidence
water bodies via two pathways are showed in Table S6. As seen in Table
S6, the ranges of the mean carcinogenic risk via the ingestion pathway
caused by Cr, As and Ni were 2.16 × 10−5–2.63 × 10−5,
4.85 × 10−5–3.86 × 10−4, and 6.29 × 10−5–1.31 × 10−3, respec-
tively, and the ranges of the 95th percentile were
2.80 × 10−5–3.40 × 10−5, 6.28 × 10−5–4.98 × 10−4, and
8.10 × 10−5 – 1.69 × 10−3, respectively. Similarly, the ranges of the
mean carcinogenic risk via the dermal contact pathway caused by Cr,
As and Ni were 3.44 × 10−6–4.18 × 10−6, 4.73 × 10−7–3.77 × 10−6,
G. Chen et al. Ecotoxicology and Environmental Safety 171 (2019) 737–745

16 8
3.5
4
14

3.0 6
12
3
2.5 10

Concentration (μg/L)

Concentration (μg/L)

Concentration (μg/L)
Concentration (μg/L)

4
8
2 2.0
6
2
1.5
4
1

1.0 2
0

0
0
0.5

-2 -2
Cd Cr As Pb

1800 120

400 40
1600 110

1400 100
300 30
1200
90
Concentration (μg/L)

Concentration (μg/L)

Concentration (μg/L)
Concentration (μg/L)

1000
80
200 20
800
70
600
60
100 10
400
50
200

0 0 40
0

-200 30
Zn Ni Fe Mn

18 0.9
30
16 0.8

14 25 0.7

12
0.6
20
Concentration (μg/L)
Concentration (μg/L)
Concentration (μg/L)

10
0.5

8 15
0.4
6
10 0.3
4
0.2
5
2

0.1
0
0
0.0
-2
Hg
Co V

Fig. 2. Boxplots of potentially harmful elements (squares and solid black lines represent the mean and median, respectively.

and 1.25 × 10−6–2.60 × 10−5, respectively, and the ranges of 95th the pathways, the carcinogenic risk of the dermal pathway was approxi-
percentile were 4.78 × 10−6–5.77 × 10−6, 6.58 × 10−7 –5.24 × 10−6 mately 1–2 orders of magnitude lower than that of the ingestion
and 1.75 × 10−6–3.63 × 10−5, respectively. In terms of the two pathway. Among the three potentially harmful elements, the

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G. Chen et al. Ecotoxicology and Environmental Safety 171 (2019) 737–745

Fig. 3. Carcinogenic risk values via ingestion (a) and dermal contact (b) based on the mean risk.

carcinogenic risk of Ni was relatively high.

Carcinogenic risk by the ingestion pathway is shown in Fig. 3(a) and
carcinogenic risk by dermal contact is shown in Fig. 3(b). As seen in
Fig. 3(a), the mean carcinogenic risk values via the ingestion pathway
are relatively high, and the most values of Ni and As are greater than
1.0 × 10−4. Fig. 3(b) shows that the mean carcinogenic risk values via
the dermal contact pathway are below 1.0 × 10−4; however, some
values are greater than 1.0 × 10−6.
For the subsidence water bodies of different periods, the order of the
total carcinogenic risk from high to low was Xinji’er (middle) > Zhangji
(middle) > Xinjiyi (old) > Panyi (old) > Pandong (new) > Zhuji
(new). Among them, Zhangji had the highest carcinogenic risk of Cr for
the two pathways, Xinjiyi had the highest carcinogenic risk of As, and
Xinji’er had the highest carcinogenic risk of Ni. Moreover, the six total
carcinogenic risk values from the six subsidence water bodies were all
above 1.0 × 10−4, which was generally the acceptable upper limit of
the interval, and these values were considered to be unacceptable.
The total carcinogenic health risk from three potentially harmful
elements via the ingestion pathway decreased in the order of
Ni > As > Cr. The order of the total carcinogenic health risk via the
dermal contact pathway was Ni > Cr > As. Therefore, Ni should be the Health risks
primary concern. In a previous study, As was considered to be a po- Fig. 4. Histogram of risk assessment for Ni via the ingestion pathway in the
tential carcinogenic risk (Wang et al., 2012). By comparison, the result Xinji’er water area.
in this study was consistent with that of the above literature. The dif-
ference is that a greater health risk of Ni was found in this study. A
possible explanation is that its concentration in the coal is relatively
higher. A previous study suggested that Huainan coal was higher in Cr,
Co, Ni, and Se than the average coals in China and the world, and their
potential environmental hazard and adverse health effects should be of
concern (Chen et al., 2011).
From the view of formation time, the descending order for carci-
nogenic health risk was mid-term subsidence water areas > old sub-
sidence water areas > new subsidence water areas.

3.3.2. Uncertainty analysis

Taking Ni as an example, the risk assessment histogram for the in-
gestion pathway in the Xinji’er subsidence water area is presented in
Fig. 4, which reflects the probability distribution characteristics, as well
as the 5% and 95% percentile risk values. A cumulative distribution
plot can be generated with the data from the MCS. Fig. 5 shows the
cumulative distribution of the carcinogenic risk of Ni from the six water
areas via the ingestion pathway, and Xinji’er has the highest risk. The
advantage of presenting the data in this format is that the associated Fig. 5. Cumulative probability distribution curve of risk assessment for Ni via
risks are more obvious (Pask et al., 2017). the ingestion pathway.
In addition, according to the results of the Monte Carlo simulation,

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G. Chen et al.
Fig. 6. Hazard quotients of heavy metals via two exposure pathways in six
water areas based on mean value (Suffix 1 represents the ingestion pathway,
Suffix 2 represents the dermal contact pathway).
as far as the ingestion pathway is concerned, the sensitivity analysis
showed that IR presented a positive effect and BW presented a negative
effect. For the dermal contact pathway, EF presented the strongest
positive effect, followed by ET and IR, and BW presented a negative
effect; the detailed sensitivity information is shown in Fig. S1.
3.4. Non-carcinogenic health risk
3.4.1. Base parameters and results
The reference dose (RfD) values for the non-carcinogenic health
risks employed in this study are shown in Table S5. The assessment
results of the non-carcinogenic health risks of potentially harmful ele-
ments by the two pathways are summarized in Table S7. The hazard
quotients of the potentially harmful elements via the two exposure
pathways are shown in Fig. 6.
3.4.2. Results analysis
Table S7 showed that the hazard quotient of Co in the Xinji’er water
area is 1.42, which is above 1, meaning the possibility of adverse health
effects. However, the values for the other metals are below 1. For the six
subsidence water areas, in light of the ingestion pathway, (1) Xinjiyi
had the highest hazard quotients for As and Mn, Panyi had the highest
hazard quotient for V; (2) Xinji’er had the highest hazard quotients for
Cd, Pb, Ni, Fe, Co and Hg; Zhangji had the highest hazard quotient for
Cr; (3) Zhuji had the highest hazard quotient for Zn. The non-carcino-
genic risk results of the dermal contact pathway were basically in ac-
cordance with that of the ingestion pathway. Furthermore, the non-
carcinogenic risk of the dermal pathway was approximately 1–3 orders
of magnitude lower than that of the ingestion pathway.
As seen from Table S7, the order of the extent of impact for HIt
caused by the potentially harmful elements from the two exposure
pathways was Co > As > Cd > V > Hg > Pb > Fe > Ni > Mn > Zn >
Cr. In addition, the summing hazard quotients of Co and As for the six
subsidence water areas via the ingestion pathway were greater than 1,
which should be a concern. In terms of the mean risk, there were two
subsidence water areas (Xinji’er, Xinjiyi) with total exposure hazard
indexes (HI) above 1. Among them, Xinji’er had the highest hazard
index, followed by Xinjiyi. This result showed that the non-carcinogenic
health risks caused by potentially harmful elements should be of con-
cern in Xinji’er and Xinjiyi. If the 95th percentile is evaluated, then
there are four water areas with total exposure hazard indexes (HI)
above 1, which are shown in Fig. 7.
In a previous study (Wang et al., 2012), the HQs of As, Zn, Pb and
Cd in the subsidence water bodies were less than 1, and the results in
this study were consistent with that result. In another study (Wang
743
Ecotoxicology and Environmental Safety 171 (2019) 737–745
Fig. 7. Hazard indexes of the mean and 95th percentile in the six mining water
areas.
et al., 2015), it was concluded that the aquatic ecosystem was not
contaminated by Zn, Pb, Cd, and Cu. Similarly, the results of this study
showed that the hazard quotients of Cd, Cu, Pb, and Zn were relatively
low. Unlike previous studies, Co was tested in this study and was found
to have the highest hazard quotient. The possible explanation was that
the content in the coal were relatively high (Chen et al., 2011).
From the view of formation time, except for Zhangji, the descending
order for non-carcinogenic health risk was mid-term subsidence water
areas (Xinji’er) > old subsidence water areas (Xinjiyi, Panyi) > new
subsidence water areas (Zhuji, Pandong). The order of health risk is
basically consistent with carcinogenic health risk.
3.4.3. Uncertainty analysis
Taking Co as an example, the histogram of the hazard quotient via
the ingestion pathway in the Xinji’er water area is presented in Fig. S2,
where shows the probability distribution characteristics and values of
the 5th and 95th percentiles.
For the uncertainties of the input parameters for the ingestion
pathway, according to the results of the Monte Carlo simulation, IR
presented a positive effect and BW presented a negative effect. For the
dermal contact pathway, EF presented the strongest positive effect,
followed by ET and IR, and BW presented a negative effect; detailed
information is shown in Fig. S3.
In regard to the different exposure routes of water, the carcinogenic
risk and non -carcinogenic risk of the dermal pathway were approxi-
mately 1–3 orders of magnitude lower than that of the ingestion
pathway. The above result shows that the ingestion path played the
dominant role for the most metals and indicated that human exposure
to potentially harmful elements through dermal contact of water was
approximately negligible. This result was identical to the results re-
ported by many other studies (Alves et al., 2014; Doabi et al., 2018;
Saha et al., 2017).
Overall, in terms of the calculation method, which was different
from traditional deterministic methods, valuable information based on
a Monte Carlo simulation was obtained in this study, such as the
probability density function of risk and confidence intervals. Moreover,
a sensitivity analysis was also conducted to reveal the importance of the
input variables. Therefore, the method based on the Monte Carlo si-
mulation had many advantages.
Notwithstanding, given the relatively low number of analyzed water
samples and single measurement, the results of the current investiga-
tion should be considered as preliminary.
4. Conclusion
In this study, the concentrations of Cd, Cr, As, Hg, Fe, Cu, Pb, Zn, Ni,
Mn, V and Co from six subsidence water bodies with different sub-
sidence periods in the Huainan coal mining area were investigated, and
G. Chen et al.
their carcinogenic and non-carcinogenic health risks were analyzed.
The mean concentrations of potentially harmful elements for six sub-
sidence water bodies followed a decreasing order:
Fe > Zn > Mn > V > Ni > Co > As > Pb > Cr > Cd > Hg. The ana-
lysis showed that Ni had the highest carcinogenic risk value in the
Xinji’er water area, and the total carcinogenic risks of the three po-
tentially harmful elements(Ni, As and Cr) for the six water areas were
all greater than 1 × 10−4, which was considered to be unacceptable.
The order of the total carcinogenic risk from high to low was
Xinji’er > Zhangji > Xinjiyi > Panyi > Pandong > Zhuji. The hazard
quotients for all samples except for Co in one sample in the Xinji’er
mining area were less than 1. Based on the mean risk, the total non-
carcinogenic health risk values for two water areas (Xinji’er, Xinjiyi)
were greater than 1. In addition, Co had the highest hazard quotient in
the Xinji’er water area, and the Xinji’er water area had the highest
hazard index. Regardless of cancer risk or non-carcinogenic risk,
Xinji’er water body had the highest health risk, so it should be a pri-
mary concern. The results provide a preliminary understanding for
health risks of the subsidence water bodies.
Acknowledgments
The work was supported by National Natural Science Foundation of
China (Grant nos. 41471422 and 51878004); Natural Science
Foundation of Anhui Provine (Grant no. 1508085 MD67); Key Project
of Excellent Young Talents of Universities in Anhui Province (Grant no.
gxyqZD2016148). We would like to thank three anonymous reviewers
for their supportive remarks on this manuscript. And also thank the
graduate students for their hard sampling work.
Appendix A. Supporting information
Supplementary data associated with this article can be found in the
online version at doi:10.1016/j.ecoenv.2018.12.101.
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