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Sustainable Cities and Society 80 (2022) 103796

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Sustainable Cities and Society


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

Assessment of heavy metal contamination levels and health risks in


environmental media in the northeast region
Yongbo Cui , Li Bai *, Chunhui Li , Zijian He , Xinru Liu
School of Municipal and Environmental Engineering, Jilin Jianzhu University, Changchun, 130118, China

A R T I C L E I N F O A B S T R A C T

Keywords: Rapid development in Northeast China has brought serious heavy metal pollution to the environmental media
Northeast China (soil, surface water and air). This paper presents a study on the spatial and temporal distribution, source analysis,
Heavy metals potential ecological risk and human health risk assessment of heavy metals in environmental media in Northeast
Temporal and spatial distribution
China, aiming to provide a theoretical foundation for controlling and reducing heavy metal pollution. The study
Source analysis
Risk assessment
shows the following results:1. Developed cities in Jilin Province (Changchun and Jilin) have the most serious
heavy metal pollution. 2. The main sources of heavy metals in soil are metallurgical production and agricultural
production. The main sources of heavy metals in surface water are industrial production, domestic waste, and
sewage. The main sources of heavy metals in the air are vehicle emissions, biomass combustion and coal burning
for winter heating. The sources of heavy metals are listed in order of decreasing significance in all three cases
above. 3. Soil, surface water and air heavy metal concentrations all have a significant impact on human health. 4.
Heavy metals in soil, surface water and air are an ecological risk and already pose a carcinogenic risk to humans.

1. Introduction air are receiving special attention, because they enter the body through
inhalation by adhering to particulate matters and depositing in the fine
Heavy metal contaminants are biologically resistant and insidious bronchi and alveoli, thus inducing diseases (Buczyńska et al., 2014; Lu
(Fang, Yang & Xu, 2013) and had not received sufficient research et al., 2019). Therefore, reducing the concentration of heavy metals in
attention until the publication of the National Land Pollution Bulletin in environmental media is of broad and current interest.
2014, which revealed the seriousness of heavy metal pollution in China. Many scholars at home and abroad have carried out research on
Medical studies have also shown that heavy metals are directly related to heavy metal levels in human body. Zhu et al. (2021) found that the
mortality and carcinogenicity in the population, so research interest in combined exposure of Al, Co and V was a risk factor for dyslipidemia by
heavy metal pollution in environmental media has risen gradually. determining the relationship between the levels of six heavy metals in
Heavy metals in soils are inaccessible to microorganisms due to their blood and dyslipidemia and the combined exposure of Cd, Sr and Pb.
insidious and persistent nature, and can enter the human body through Wu et al. (2017) determined the possible relationship between urinary
dermal contact and food chain intake, thereby endangering human heavy metal exposure level and neurotransmitter metabolism, indi­
health (Li, Bai, He, Liu & Xu, 2021; Li, Wei, Dai, He & Liu, 2021; Li, cating that urinary Cr level was significantly correlated with the
Kong, Han, Zhao & Chen, 2018). Studies have shown that almost 80% of decrease of serotonin level, and Cd was positively correlated with
China’s water environment suffers from different degrees of heavy metal norepinephrine and epinephrine. In addition, arsenic was found to be
pollution (Li & Wen, 2020; Zhao et al., 2012), which is difficult to be positively correlated with tryptophan, serotonin, dopamine and
degraded by microorganisms in water. Over a long period of time (Li & norepinephrine. Zhang et al. (2011) analyzed the metal elements in
Wen, 2020), heavy metal pollution leads to changes in the chemical breast milk of pregnant women in Xiamen and Baoding, and concluded
composition of the therefore posing a threat to the human body through that milk Pb level was related to eggs and saltwater fish consumptions
ingestion and dermal exposure. Air pollution has been an issue of and short stature during pregnancy, milk Cd level was related to salt­
continuous discussion among scholars since the London smog incident. water fish consumption, milk Hg level was related to eating saltwater
Recently, with the COVID-19 pandemic, heavy metal pollutants in the fish and crabs consumption. The above studies analyzed heavy metal

* Corresponding author.
E-mail address: baili@jlju.edu.cn (L. Bai).

https://doi.org/10.1016/j.scs.2022.103796
Received 10 November 2021; Received in revised form 18 January 2022; Accepted 17 February 2022
Available online 19 February 2022
2210-6707/© 2022 Elsevier Ltd. All rights reserved.
Y. Cui et al. Sustainable Cities and Society 80 (2022) 103796

elements in the environment through blood, urine and breast milk, and pollution. As a pillar industry of Jilin Province, the automobile
there were certain flaws in sample collection and pretreatment, such as manufacturing industry has registered more than 4 million vehicles in
accuracy and feasibility issues. Human hair has been recommended by the province, and both the exhaust and the manufacturing process will
the World Health Organization (WHO), the U.S. National Environmental affect the soil, surface water and air to some extent. Jilin Province also
Protection Agency (EPA) and the International Atomic Energy Agency has an important pharmaceutical city in China, with sales value
(IAEA) as an important biomaterial for environmental monitoring exceeding 200 billion yuan per year for five consecutive years. The
worldwide due to its low cost, stable nature, strong operability and "three wastes" generated by biopharmaceuticals contaminate the soil as
convenient storage and transportation (Passwater et al., 1983; Ryabu­ well as causing environmental problems in water bodies. In summary,
khim, 1978; Samanta, Sharma, Roychowdhury & Chakraborti, 2004). various environmental media in Jilin Province are relatively more
Analyzing heavy metal pollution level in human body through analyzing seriously polluted by heavy metals, so analyzing the level of heavy metal
human hair has been increasingly widely used. Wu, Yang, Ma, Yu and pollution in Jilin Province from the perspective of different environ­
Wang (2007) have analyzed the distribution of heavy metal content in mental media yields more representative results. Therefore, this paper
the human body of residents of Liaohe River Basin through human hair, selects nine cities in Jilin Province in Northeast China as the research
and concluded that the level of heavy metal pollution of urban residents subject, uses the correlation between the concentration of heavy metals
is higher than that of rural residents. He, Li, Wang, Zhao and Yang in soil, surface water and air and the content of heavy metals in human
(2017) analyzed the levels of five heavy metals in human hair in the body as a starting point, and develops a series of studies that are of great
main city and suburbs of Chongqing, and pointed out that in the main scientific significance. Contamination characteristics and trends of
city, Cu, Ni and Pb in human hair had similar sources, while in the spatial and temporal patterns of heavy metals are studied using the
suburbs, Cd, Ni and Pb in human hair had similar sources. Wang, Wang, Kriging approach. The sources of heavy metal pollution are investigated
Qiu and Qian (2017) analyzed the spatial distribution characteristics of by principal component analysis. In addition, many preventive measures
heavy metal content in human hair in Shanghai, and obtained the spatial are proposed to control the source of pollution, which can not only
distribution rules of four heavy metal contents in Shanghai residents’ greatly reduce the pollution of heavy metals, but also propel sustainable
hair. In particular, the content of hair Cd and hair Pb showed a development. The linear correlation between the content of heavy
decreasing trend from urban to suburban. In summary, hair has been metals in human body and various environmental media is obtained by
widely used for the detection of heavy metal indicators in humans. multiple linear regression, the potential ecological hazard index (RI) of
Studies have shown that heavy metal pollutants enter the soil, sur­ metals and the degree of metal pollution are calculated to obtain the
face water and air, and subsequently enter the human body through skin ecological risk of metals and to assess the health risks of heavy metals in
contact, respiration and hand-to-mouth, and accumulate in the human the environment to the population, which provides theoretical basis for
body over time (Bai, Sun, Li, Kang & Ni, 2019). As the concentration of achieving sustainable development of the environment.
heavy metals in the body increases, heavy metals can interfere with
normal physiological functions and disrupt normal biochemical re­ 2. Method
actions for an extended period of time, harming human health. Studies
have shown that Cr(VI) accumulates in the body and causes skin ulcers 2.1. Study area
and eczema, liver damage, respiratory cancers, glomerular necrosis and
pneumonia (Xie, 2016; Yang et al., 2020). Ni has the greatest effect on The sample was collected in Jilin Province in Northeast China (lon­
the skin, causing pimples, herpes and erythema, followed by cancer, gitude:121◦ 38′ ~131◦ 19′ , latitude:40◦ 52′ ~46◦ 18′ ). As a national in­
neurological disorders, systemic disorders and reduced fertility (Huang, dustrial base, Jilin Province has serious environmental pollution
Wei & Su, 2008). Cu red-brown metal, can lead to chronic toxicity problems caused by industrial production, coal burning for winter
manifested by neurological weakness, metabolic disorders, cell carci­ heating, ore mining, the automobile industry and agricultural produc­
nogenesis and brain tissue lesions (Yang et al., 2020). Pb is widely tion. For the purposes of this study, human hair, soil, water and air were
distributed in nature and has clinical manifestations such as disorders of collected from nine cities in Jilin Province from March 2019 to March
metabolism, reduced hematopoiesis, central nervous system weakness 2020 (Fig. 1). Two sampling points are set in each city, and a total of
and infertility (Liu et al., 2018; Qin, 1994). Zn is a trace element in the 2450 effective samples are collected. The heavy metal elements in the
human body, and both high and low levels can cause related diseases samples were determined by inductively coupled plasma emission
(Bai et al., 2020). Zn deficiency can cause skin lesions, neurological spectrometry . The research framework is shown in Fig. 2.
disorders, lowered immunity, etc. Zn excess can lead to zinc poisoning
and symptoms such as vomiting and diarrhea (Zhang & Liu, 2019). 2.2. Sample collection
Therefore, it is very important to study the influence of different envi­
ronmental media on the content of heavy metals in the human body. 2.2.1. Soil
In the past ten years, experts at home and abroad have conducted According to Specification of land quality geochemical assessment
extensive research on heavy metal contamination and its control in (DZ/T 0295–2016) (Chinese Ministry od Natural Resources, 2016) and
environmental media (Abdullah et al., 2015; Bai, He, Chen & Wang, Technical Specification for soil Environmental monitoring (HJ/T
2019; Balachandran, Meena & Khillare, 2000; Maenhaut, Schwarz, 166–2004) (Chinese Ministry of Environmental Protection, 2004), soil
Cafmeyer & Chi, 2002). However, studies on the level of heavy metal samples were collected from 0 to 20 cm soil layer with stainless steel
pollution in Jilin Province are confined to a single environmental me­ spoon (Tang, Lu, Fan, Wu & Bao, 2020). The effective sample size 180.
dium (Bai, Chen, He, Sun & Qin, 2019; Fromme et al., 2008; C. H. Li After drying the soil samples, root and debris were removed. The sam­
et al., 2021; Q. Y. Li et al., 2021), and there are few reports on the ples were then dried through a nylon screen and then sealed and stored
correlation between the concentration of heavy metals in various in polyethylene bags.
environmental media and the content of heavy metals in human body.
Jilin Province is an important grain production base in China (Bai, Li, He 2.2.2. Water
& Chen, 2019), with an annual grain output of about 50 billion kg. According to the International Standards for Water and Atmospheric
Therefore, the increase in the application of chemical fertilizers and Quality Analysis Methods (International Organization for Standardiza­
pesticides will bring serious soil pollution problems. Due to coal burning tion Convergence, 1990), water samples from nine cities were collected
for heating in the winter (Bai, Li, Yu & He, 2021), Jilin province con­ in pre cleaned 1 L plastic containers. The effective sample size 180.
sumes about 71.321 million tons of energy every year, of which only Concentrated HNO3 was added to the water sample for acidification and
10.1% is clean energy. Therefore, heating in the winter causes serious air preservation. Then the samples were passed through 0.45 μm

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Y. Cui et al. Sustainable Cities and Society 80 (2022) 103796

Fig. 1. Sampling collection location.

Fig. 2. Framework for analysis the metal elements.

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Y. Cui et al. Sustainable Cities and Society 80 (2022) 103796

microporous membrane filtrations and stored in polyethylene plastic



n
bottles. Z ∗ (S0 ) = λi (S0 )Z(S0i ) (1)
i=1

2.2.3. Air
Sampling shall be carried out in strict accordance with the relevant where Z (S0i) is the value at point S0i, which is a sample at location i.
provisions of Indoor air quality standard (GB/T18883–2002) (Chinese Here λi (S0) are the ordinary kriging weights, and Z*(S0) is the estimated
Ministry of Health, 2002). The sampling point was arranged 1 m away value. In this study, ArcGIS10.6 software was used to draw the spatial
from the window and 0.6 m away from the ground. The monitoring time distribution map of heavy metal concentration in all urban environ­
was 24 h/d. Each 50-minute sampling time was followed by a 10-minute ments of Jilin Province.
break, and the filter membrane WAS replaced every 5 days. A total of
180 effective samples were collected. The samples were sealed in clean 2.5.2. Multivariate linear fitting analysis
polyethylene plastic bags, numbered, and stored in environment with Multiple linear regression is a kind of regression analysis to model
stable conditions for use in subsequent experiments. the relationship between multiple independent variables and dependent
variables. linear regression is a statistical method whose main purpose is
2.2.4. Hair to predict, explain, and determine the quantitative relationship and
Based on IAEA recommendations (Ryabukhim, 1978), hair was degree of interdependence between more than two variables (Bas, Ortiz,
collected from residents who had lived in the city for over 20 years. The Ballesteros & Martorell, 2017). The formula is shown in Eq. (2), and
effective sample size was 1910 (the recovery rate was 95.5%). At the notations are summarized in Table 1.
residents’ home, stainless steel scissors were used to collect 5 g of hair Yt = Xt β + εt (2)
starting from 3 to 5 cm from the scalp in the back of residents’ head. The
hair was then sealed and stored in numbered clean polyethylene plastic Usually, the goodness-of-fit of multiple linear regression is measured
bags. Age and gender information was also recorded. by R2. An R2 value closer to 1 indicates almost all variations in the
dependent variables can be explained by the linear regression model.

2.3. Elemental analysis 2.5.3. Ecological risk assessment


According to the properties and environmental behavior of heavy
Elemental analysis were performed on all processed samples. The metals, Hakanson proposed the potential ecological hazard index
samples were put into a 50 ml Teflon beaker and dried to constant method from the perspective of sedimentology. The method has been
weight for use. Electronic balance was used to weigh about 0.5 g of widely used because it comprehensively considers the content of heavy
sample, which was then placed in beaker. Then 40 ml of HCL-HNO3 metals, the synergy between elements, the degree of toxicity, pollution
digestion solution (volume ratio: 3:1) were added. The solution in the concentration and pollution sensitivity (Islam, Ahmed, Mamun &
beaker was heated and refluxed on the microwave digestion instrument Masunaga, 2014). Please see formulas 3–5 for calculation of potential
(Topwave, Analytic Jena) for 2 h until the total volume was reduced to ecological hazard index method. The classification of potential ecolog­
25 ml. After cooling to room temperature, the ultrapure water was ical risk assessment indicators is shown in Table 2.
added to a 25 ml volumetric flask. The metal elements in all samples
Ci
were analyzed by inductively coupled plasma atomic emission spec­ Cfi = (3)
trometry (ICP-OES leeman, Prodigy XP-High Dispersion, USA). Cni

Eri = Tri × Cfi (4)


2.4. Quality control

m
RI = Eri (5)
In order to ensure the accuracy of the test results, the instrument i
components were cleaned and debugged before the test, and 2 ~ 3
spectral lines were selected for each element. The intensity, spectral line 2.5.4. Health risk assessment
and interference of each spectral line were analyzed and compared, and The health risk assessment model recommended by the U.S. Envi­
the best analytical spectrum of each element was finally selected, and ronmental Protection Agency (EPA) was used to calculate the level of
the detection limits of different heavy metal elements were obtained. heavy metal contamination in different environmental media (U.S.
Based on the concentration of the standard solution and the solution to Environment Protection Agency, 1996, 2002), the amounts of heavy
be tested, the error of the instrument was taken to be three times the metals entering the human body through different routes are shown in
detection limit. One quality control sample was added for every 10 formulas 6, 7 and 8. Significance and value of various parameters
samples, and the recovery rate of heavy metals in quality control sam­ (Duan, 2014; Ferreira-Baptista & Miguel, 2005; Van den Berg, 1994;
ples was 88% ~ 107%. Wang et al., 2009; Wang, Liu, Chen & Lin, 2008) are shown in Table 3.
C × IRing × EF × ED × CF
Handandmouthintake : ADDing = (6)
2.5. Statistical analysis BW × AT

2.5.1. Approach Respireintake : ADDinh =


C × IRinh × EF × ED × ET
(7)
Kriging approach is a geostatistical approach for spatial interpola­ PEF × BW × AT
tion. Under suitable assumptions on covariances, it gives the best linear
unbiased estimator of values at unsampled finite locations based on
variogram model (Xu, Zhang, Zhang, Li & Yu, 2018), derived from the Table 1
Parameter meaning.
spatial structure and the semivariance of the original data. The Kriging
method estimates the value at a location by computing a weighted Symbol Meanings
average of observed samples in the neighborhood of the point based on Yt Predicted value at the time
the relative spatial structure of the point with respect to all samples. The Xt A vector of explanatory variables at the time
weights are calculated from the variogram, and then the estimator is ß The vector of coefficient
A random error term at time
given by Formula 1:
Ɛt

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Table 2 HQ and HI values of at most 1 indicate the risk is negligible. HQ and


Classification of potential ecological risk assessment indicators. HI values strictly greater than 1, indicate a non-carcinogenic risk. An
Eri Single-factor ecological RI Multi-factor ecological element with ILCR<10− 6, has negligible carcinogenic risk. An element
hazard degree hazard degree with 10− 6<ILCR<10− 4 is at risk of carcinogenesis, while having
<40 Slight <150 Slight ILCR>10− 4 indicates high risk of cancer. According to relevant data
40~80 Medium 150~300 Medium (Duan et al., 2011; Li, 2018; Naeher, Smith, Leaderer & Neufeld, 2001),
80~160 Relationly strong 300~600 Strong the reference dose and slope coefficient of various heavy metal exposure
160~320 Strong >600 Very strong routes are shown in Table 4.
>320 Very strong

3. Results

Table 3 3.1. Temporal and spatial distribution of heavy metals in environmental


Parameter meaning and value. media
Symbol Unit Meanings Child Adult

ADDing (kg⋅d)/ the amount of exposure by hand and – The spatial and temporal distributions of heavy metals in soil, water
mg mouth and air in Jilin Province are shown in Figs.. 3, 4 and 5 respectively. In
ADDinh (kg⋅d)/ the amount of exposure by respiratory – soil, Cr(VI) concentration in Jilin Province are 1.21 times higher than
mg intake
the local background value (Du & Feng, 1983), Cu concentration is 1.09
ADDder (kg⋅d)/ the amount of exposure by respiratory –
mg intake times higher than the local background value in Baicheng City and
EF d/a Exposure frequency 365 Songyuan City, Ni concentration decreases from south to north, Pb
ED a Exposure duration 6 24 concentration is only 1.5 times higher than the background value in the
AT d Average exposure time 8760(non- border area between China and North Korea in Yanji City in Jilin
carcinogenic)/
Province, and Zn concentration gradually increases from west to east.
25,550
(carcinogenic) In surface water, Cr(VI) concentration in Jilin Province is higher than
IRing mg/d the intake of hand and mouth 200 100 the local background values in Baicheng, Songyuan, Changchun, Siping
IRinh m3/d the intake of breath 5 20 and Jilin cities, Cu concentration shows a decreasing trend from east to
BW kg Body weight 16 62
west, Ni and Zn concentrations are higher than the local background
PEF m3/kg Particle emission factor 1.32 × 109
SA cm2 Dermal exposure area 1600 4350
values, and Pb concentration is higher than the local background values
ET h/d exposure time 20 in Yanji city only.
PC cm/h Dermal adsorption fraction 2 × 10− 3(Cr In air, Cr(VI) concentration in Jilin Province decreases from south to
(VI)) 6 × north, Cu concentration decreases from Changchun to the surrounding
10− 4(Cu) 1 ×
cities, Ni concentration is 1.16 times higher than the local background
10− 4(Ni) 4 ×
10− 6 (Pb) 6 × value, Pb concentration is 4.24 times higher than the local background
10− 4(Zn) value in Yanji, and Zn concentration gradually increases from east to
west. In addition, heavy metal pollution in different environmental
media in Jilin Province concentrates in Changchun and Jilin cities, with
C × SA × PC × CF × EF × ED generally high levels of concentration for the five heavy metals.
Skinintake : ADDder = (8)
BW × AT
The characterization of heavy metals on human health risk is divided 3.2. Source analysis of heavy metals in environmental media
into non-carcinogenic risk and carcinogenic risk. Generally, the non-
carcinogenic risk is expressed by HQ and the carcinogenic risk is The sources of the five heavy metals in the environmental media
expressed by ILCR. The calculation formula is as follows: were analyzed using principal component Table 5. shows that the main
sources of heavy metal pollution in soil are metallurgical production and
HQ =
ADD
(9) agricultural production processes, in surface water are industrial pro­
RfD duction, domestic waste and sewage, and in air are coal combustion for
∑ winter heating, mixed sources biomass combustion and vehicle exhaust
HI = HQi (10) emissions. In addition, the cumulative contribution of heavy metal
pollution in soil, surface water and air was found to be 74.35%, 82.572%
ILCR = ADD × SF (11) and 88.543% respectively through principal component analysis.
The correlation analysis results (Fig. 6) show that the correlation
where, HQ denotes the non-carcinogenic risk of a single heavy metal, HI
coefficients of Cr(VI)-Cu and Cr(VI)-Pb in soil are 0.650 and 0.617, the
denotes the integrated non-carcinogenic of a single heavy metal, ADD
correlation coefficients of Cr(VI)-Cu, Cr(VI)-Ni and Cr(VI)-Pb in surface
denotes non-carcinogenic daily average exposure in mg/(kg⋅d), RfD is
water are 0.791, 0.812 and 0.651, and the correlation coefficients of Cr
the reference dose of exposure route in mg/(kg⋅d), SF is the slope co­
(VI)-Cu, Cr(VI)-Ni and Cr(VI)-Pb in air are 0.822, 0.781 and 0.773. In
efficient, and ILCR is the carcinogenic risk of single heavy metals.
conclusion, Cr(VI)-Cu and Cr(VI)-Pb in environmental media have
strong correlations.
Table 4
Reference dose and slope coefficient of heavy metal exposure pathway. 3.3. Study on the correlation between the concentration of heavy metals
in environmental media and the content of heavy metals in the human
Element RfDing[mg/ RfDinh[mg/ RfDder[mg/ SF
(kg⋅d)] (kg⋅d)] (kg⋅d)] body
3 5 5
Cr(VI) 3.00 × 10− 2.86 × 10− 6.00 × 10− 9.80
Cu 4.00 × 10− 2
4.00 × 10− 2
1.20 × 10− 2
– The linear fit analysis of heavy metals in different environmental
Ni 2.00 × 10− 2
2.00 × 10− 2
5.40 × 10− 3
8.40 × media to human heavy metal concentrations is shown in Fig. 7. The
10− 1 coefficients of determination, R2 values, of the fitted curves are above
3 3 4
Pb 3.52 × 10− 3.52 × 10− 5.25 × 10− – 0.9, indicating that over 90% of variations in heavy metal concentration
1 1 2
Zn 3.00 × 10− 3.00 × 10− 6.00 × 10−
in human body can be explained by variations in heavy metal

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Fig. 3. Spatial distribution characteristics of heavy metals in the soil of Jilin Province.

concentration in environmental media. Soil, surface water and air heavy ranked as Pb > Cu > Ni > Cr(VI) > Zn. The potential ecological risk
metals are significantly correlated with human heavy metal concentra­ index for all five heavy metals in surface water is less than 40, which is a
tions. The graphs show that air is the most important factor affecting low ecological risk. The hazard index of heavy metals in air is ranked as
human heavy metal concentrations, followed by soil and surface water. Pb > Cu > Ni > Cr(VI) > Zn. Potential ecological index of Cr(VI), Cu, Ni
The five heavy metals, Pb and Zn show linear correlation coefficients of and Zn in air less than 40, also indicating low ecological risk. Of the five
0.98 and close to 1, indicating that Pb and Zn levels in humans are monitored heavy metals, only Pb has anecological risk index of >40,
strongly correlated with corresponding levels in various environmental posing a moderate ecological risk. The above analysis reveals that
media. although the heavy metal concentrations in the environmental media
are higher than the local background values, only Pb presents an
ecological risk, and therefore we should focus our subsequent studies on
3.4. Potential ecological risks of heavy metals in environmental media Pb contamination.

The potential ecological risk of heavy metals in environmental media


in Jilin Province was calculated using Eqs. (3)-(5), and the results are 3.5. Health risk assessment of heavy metals in environmental media
shown in Table 6. The hazard index of heavy metals in soils is ranked as
Pb > Cu > Cr(VI) > Ni > Zn. The potential ecological risk index of five The risk values of heavy metals in different environmental media in
heavy metals in soil is less than 40, and the ecological risk is relatively Jilin Province are calculated by formulas 6–11. The non-carcinogenic
low. The hazard index of heavy metal elements in surface water is risks of heavy metal elements in soil are shown in Table 7. The non-

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Y. Cui et al. Sustainable Cities and Society 80 (2022) 103796

Fig. 4. Spatial distribution characteristics of heavy metals in surface water of Jilin Provinc.

carcinogenic risk of Cr(VI) is significantly higher than that of the other has a strong carcinogenic risk while Ni has a moderate one, with values
elements. The non-carcinogenic risk levels of heavy metals are ranked Cr 10− 6<Ni<10− 4<Cr(VI). In water, for adults, carcinogenic risk values of
(VI) > Pb > Ni > Cu > Zn. The non-carcinogenic risk through hand oral heavy metals satisfy 10− 6<Ni<Cr(VI)<10− 4, while in children we have
intake, inhalation and skin contact for children is significantly higher 10− 6<Ni<10− 4<Cr(VI). This shows that the carcinogenic risk value of
than for adults. The non-carcinogenic risk levels of heavy metal ele­ heavy metals in water is significantly higher for children than for adults.
ments in water are shown in Table 7. The non-carcinogenic risk levels of In air, for both adults and children, the carcinogenic risk values of heavy
heavy metal elements are ranked Cr(VI) > Pb > Ni > Cu > Zn. The non- are 10–6<Ni<10–4<Cr(VI), which shows that Cr(VI) and Ni elements
carcinogenic risk for children through ingestion and skin contact is present serious carcinogenic risks to the human body.
higher than for adults, while the non-carcinogenic risk through inhala­
tion is lower for children. The non-carcinogenic risk levels of heavy 4. Discussions
metal elements in the air are shown in Table 7. The non-carcinogenic
risks through ingestion are higher in children, while the non- This section further discusses the temporal and spatial distribution,
carcinogenic risks through inhalation are lower in children. In addi­ source analysis, linear regression analysis, potential ecological risk and
tion, the total non-carcinogenic risk of heavy metals in different envi­ human health risk assessment of heavy metals in different environ­
ronmental media is smaller than 1 and negligible. mental media in Jilin Province in Northeast China.
The carcinogenicities of heavy metals in different environmental In this study, soil heavy metal contamination was ranked as Zn > Cr
media areshown in Table 8, In soil, for both adults and children, Cr(VI) (VI) > Ni > Pb > Cu. Average soil concentrations of Zn and Cr(VI) were

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Fig. 5. Spatial distribution characteristics of heavy metals in the air of Jilin Province.

117% and 121% times higher than the local background values,
Table 5 respectively. Compared with other regions (Table 9), those concentra­
Principal component analysis.
tions in the area of interest of this paper are significantly higher than
Element Soil Water Air those in regions, One possible explanation is that Jilin Province is a
Factor Factor Factor Factor Factor Factor major agricultural province, with an annual grain production of about
1 2 1 2 1 2 50 billion kg. The amount of chemical fertilizers used in Jilin Province in
Cr(VI) 0.818 − 0.123 0.913 0.092 0.884 − 0.400 2020 reached 4 million tons based on survey in the area. The use of
Cu 0.756 − 0.362 0.845 − 0.149 0.853 − 0.326 mulch and the application of large amounts of phosphorus and waste
Ni 0.382 0.895 0.935 − 0.070 0.952 0.080 fertilizers lead to a large amount of Cr(VI) and Zn elements in soil,
Pb 0.894 0.301 0.754 0.581 0.882 0.090
resulting in an increase in the heavy metal contents in soil causing
Zn 0.561 − 0.423 0.757 − 0.437 0.511 0.769
Variance 50.011 24.339 71.278 11.294 73.972 14.572 serious pollution. The levels of heavy metal pollution in surface water
contribution are ranked as Zn > Cr(VI) > Ni > Pb > Cu, consistent with the ranking in
rate/% soil. This is because various ions of heavy metal elements in water form
Cumulative 50.011 74.350 71.278 82.572 73.972 88.543 insoluble salts, which are transported to the soil through deposition or
contribution
rate/%
adsorption by sediment and microorganisms in water. This is consistent
with Chen Mingjun’ research results (Fu, Chen & Qi, 2008). The con­
centration of heavy metals in the air is ranked Pb > Zn > Cr(VI) > Ni >
Cu. The Pb concentration in the air is 424% times higher than the local

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Y. Cui et al. Sustainable Cities and Society 80 (2022) 103796

Fig. 6. Relevance analysis results.

background value. When comparing with other countries, the air Pb production is the primary one, accounting for 50.011% of all sources.
concentration in this study is significantly higher than that of old in­ Waste gas, waste water and waste residue enter the environment (Wang
dustrial powers such as Germany (Zereini et al., 2005) and Spain Campa et al., 2018) due to metallurgical production. Therefore, reducing the
et al., (2010) in the 21st century. Since the 19th century, western production of "three wastes" and effectively recycling them to meet the
developed countries have been committed to air pollution control and emission standards of waste gasses in China (He & Cai, 2021) is of
pollution source control of industrial enterprises (Lu, Xiao, Zhang, Chen crucial importance. In addition, the government should impose stricter
& Liu, 2018). However, the area of interest in this study is in a period of panelties for exceeding the standard, and enterprises should establish a
rapid urban development, and lead pollution is more serious due to the comprehensive enterprise emission permit system, strictly control the
impact of industrial production (Xiao, 2017). The pollution of different flow of waste, and form a control waste emission list, because the
environmental media is ranked as air > soil > surface water. One implementation of a systematic and comprehensive tracking manage­
explanation is that in recent years, there is a large straw surplus in the ment (Chen, 2020; Zhai, Cheng, Ai & Shang, 2020) can greatly reduce
three northeastern provinces, and biomass fuel is still widely used for the pollution caused by heavy metals to the soil. The second source is the
cooking and heating in Northeast China (Zhang, Tao, Cao & Covency, agricultural production process, accounting for 24.339% of all sources.
2007). Secondly, the number of cars in Jilin Province is high, and the Relevant studies have found that agricultural production process has
harmful gasses and dust containing heavy metals emitted by automo­ become one of the most important sources of heavy metals in the
bilesand tire wear also contribute considerably to air heavy metal environment (Van den Berg, 1994). The use of a large number of
pollution (Li, Lin, Zhang, Xu & Yu, 2005). The figure shows that the Pb chemical fertilizers and pesticides in the process of agricultural pro­
pollution in Yanji city is high, resulting from large emission of the heavy duction leads to the increase of soil heavy metal concentration (Qu et al.,
metal lead in the city, accounting for 80.8% of the whole province (Liu, 2016), which poses a great threat to human health. Studies show that
Bao, Wu & Li, 2011), because a large number of lead elements are balanced cultivation techniques (Pataczek et al., 2018) biodegradable
emitted in the city. Therefore, the concentrations of heavy metals in soil, mulch (Boularbah, Schwartz, Bitton & Morel, 2006) and organic fertil­
surface water and air are high in Yanji City. Changchun and Jilin are the izers can balance the soil ecosystem, provide comprehensive nutrition
main areas of heavy metal pollution, while Tonghua and Baishan have a for plants, and improve the physical and chemical properties of soil.
better overall environmental level. One possible reason is that Chang­ Therefore, balanced cultivation techniques, biodegradable mulch and
chun is the capital city of Jilin province and Jilin is the second largestcity organic fertilizers should be widely popularized in the process of agri­
in Jilin province, with a large population and rapid economic develop­ cultural production, so as to reduce the health risk of agricultural pro­
ment. In addition, Changchun produces at least 13 million tons of straws duction to human body.
every year, and the burning of which bring serious pollution to the city The analysis of the five heavy metals in surface water shows that
and the surrounding cities. Therefore, heavy metal pollution in Jilin there are two main sources, with the primary source being industrial
Province is mainly concentrates in Changchun and Jilin. Through the production, which accounts for 71.278% of the sources of water pol­
analysis of the sources of heavy metal pollutants in different environ­ lutants. Studies have shown that industrial production can result in large
mental media using principal component analysis, source control can be numbers of heavy metals entering the water body (Kurt-Karakus, 2012).
achieved to reduce the degree of heavy metal pollution. The area of interest in this paper is a famous industrial base and phar­
The analysis of heavy metals in the soil reveals two main sources. As maceutical production base in China. Therefore, establishing a sewage
in the paper by Hao, Guo, Yang, Fang and Feng (2007) metallurgical control system, dynamically monitoring the operating status of the

9
Y. Cui et al. Sustainable Cities and Society 80 (2022) 103796

Fig. 7. Linear regression analysis of heavy metal concentration in environmental factors and human heavy metal concentration.

sewage treatment system to ensure the standards of the quality of the identification of waste characteristics, and the mixed composting
effluent check items are met, and efficiently improving the quality of (Huang et al., 2017) of certain waste such as straw, livestock manure and
sewage treatment, will greatly reduce the pollution of heavy metals woodland waste, can not only achieve the integrated use of energy, but
(Yang, Yang & Li, 2021). The second major source is domestic waste and also serve as an important measure to reduce heavy metal pollution.
sewage, accounting for 11.294% of all sources. The impervious burial of The five heavy metals in the air come from two sources. The primary
domestic garbage and the improper discharge of domestic sewage can sources are coal and biomass combustion in the winter, accounting for
pollute and impair the water body (Wang, Wang, Gao, Han & Wu, 2014). 73.972% of all sources. Studies have shown that coal and biomass
Therefore, the establishment of a suitable waste treatment plant, the combustion in the winter releases a large number of heavy metals into

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Y. Cui et al. Sustainable Cities and Society 80 (2022) 103796

Table 6
Potential ecological risks of heavy metals in soil, surface water and air.
Category Element Toxicity coefficient Potential ecological risk coefficient Eri Potential ecological risk Comprehensive ecological risk

Soil Cr(VI) 2 5 Slight Slight (25.4)


Cu 5 5.5 Slight
Ni 5 5 Slight
Pb 5 7.5 Slight
Zn 1 2.4 Slight
Surface water Cr(VI) 2 0.6 Slight Slight (11.8)
Cu 5 4.3 Slight
Ni 5 2.4 Slight
Pb 5 4 Slight
Zn 1 0.5 Slight
Air Cr(VI) 2 3.2 Slight Slight (79.67)
Cu 5 12 Slight
Ni 5 5.8 Slight
Pb 5 57.27 Medium
Zn 1 1.4 Slight

the environment (Fytianos & Tsaniklidi, 1998; Xu, 2020). In the area of there is an upward trend of heavy metal ecological risks, which calls for
interest of this paper, coal and biomass combustion is commonly used great effort to track and monitor the pollution levels to avoid wider and
for cooking and heating, with low combustion efficiency. Therefore, more serious pollution. Through the calculations in formulas 6–11, it is
efficient combustion technologies should be studied so as to facilitate found that the non-carcinogenic risk HI of soil, surface water and air to
the establishment of a biomass fuel collection, pretreatment and distri­ adults and children is less than 1, indicating that there is no non-
bution system and a suitable biomass power generation system. This will carcinogenic risk. Cr(VI) and Ni in soil, water and air have serious
not only result in near-zero CO2 and particulate matter emission, cancer risks, with ILCRAir>ILCRSoil>ILCRWater. As analyzed above, Cr
meeting carbon peaking and carbon neutral targets, but also reduce (VI) and Ni mainly come from industrial production, coal combustion
heavy metal emissions (Jagustyn, Kmieć, Smędowski & Sajdak, 2016; and transportation sources. Therefore, we should target the Cr(VI) and
Xue et al., 2022). The second source is automobile exhaust emission, and Ni sources to control the health risks caused by heavy metal pollution.
zinc is a landmark element of automobile exhaust emission (Taiwo, The risk of hand and mouth exposure under different environmental
Harrison & Shi, 2014). Studies show that vehicle emission has become media is significantly higher than inhalation and skin contact. The risk
one of the most important sources of heavy metals in the environment of cancer caused by metal elements in adults is significantly lower than
(Bai et al., 2020). Automobile exhaust contains a large number of that in children, who have more exposure due to outdoor activities. This
harmful substances such as suspended solids and heavy metals, resulting result is the same as the trend of heavy metal exposure for residents in
in changes of heavy metal concentration in the air (Odoh, Udegbunam & Chongqing (He et al., 2017). Under different environmental media, the
Etim, 2013), and thus endangering human health. We should encourage carcinogenic risk of Cr(VI) is significantly higher than that of Ni, indi­
urban and rural residents to choose eco-friendly transportation methods, cating that the potential harm of Cr(VI) is much greater than that of Ni.
and promote new energy vehicles and electric vehicles, which will not Therefore, isolation measures should be taken in metallurgical produc­
only reduce emission pollution and improve air quality (Zhang, 2019), tion to protect the surrounding residents.
but also reduce the content of heavy metals in the air.
This study analyzes the correlation between metal concentration 5. Conclusions
levels in the human body and in different environmental media,
concluding that the concentrations of heavy metals in different envi­ The spatial and temporal distribution of heavy metals in soil, water
ronmental media have a significant impact on the concentrations in and air, linear regression analysis, potential ecological risks and human
human body. Wang et al. (2003) also showed that serious heavy metal health risk assessment were analyzed through monitoring heavy metals
pollution can occur in soil, surface water and air will produce serious in different environmental media in northeast China, with Jilin Province
heavy metal pollution. Relevant studies show that heavy metals in soil as the focus. The following conclusions were drawn:
are absorbed by plants, not only increasing the concentration of heavy
metal in plants themselves, but also finding their way into the human 1 Heavy metal concentrations in soil, surface water and air were
body through the plants (Zeng et al., 2011). Heavy metals in surface ranked as Zn>Cr(VI)>Ni>Pb>Cu; Zn>Cr(VI)>Ni>Pb>Cu;
water accumulate easily in aquatic organisms and are bioaccumulative Pb>Zn>Cr(VI)>Ni>Cu, and heavy metal concentrations in envi­
in the food chain, posing a serious threat to human health (Shue, Chen, ronmental media were ranked as air>soil>surface water, with
Tseng & Lai, 2012). Gupta, Rai, Pandey and Sharma (2009) have shown Changchun and Jilin cities having the most prominent heavy metal
that the trend of heavy metal concentrations in water aligns with that in pollution.
fish. As a major grain producer of China, Jilin Province has a large 2 The main sources of heavy metal pollution in soil are metallurgical
number of biomass retention and biomass combustion every year. In production and agricultural processes, in surface water pollution are
addition, heating in the winter, coal combustion and automobile exhaust industrial production and domestic waste and sewage, and in air
all emit considerable pollution into the air, which thenenters the human pollution are biomass burning, coal combustion and vehicle
body through breathing. Bai et al. (2021) have shown that the sources of emissions.
air pollution in Jilin Province are coal combustion and automobile 3 Heavy metals in soil, surface water and air enter the human body in
exhaust. many ways and have a significant impact on human health.
Next, we further explore the potential ecological risks caused by 4 The concentrations of heavy metals in soil, surface water and air
heavy metals in different environmental media and the carcinogenic constitute ecological risk, and Pb in air has moderate ecological risk.
risks to children and adults. Through evaluating the synergistic effect, 5 The non-carcinogenic risk HI of soil, surface water and air to adults
toxicity level, pollution degree and sensitivity of heavy metals, it is and children is less than 1, indicating that there is no non-
found that there are ecological risks in soil, surface water and air, in carcinogenic risk. Cr(VI) and Ni in soil, water and air have serious
particular, Pb in the air. In terms of the degree of heavy metal pollution, carcinogenic risk, with ILCRAir>ILCRSoil>ILCRWater. The risk of

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Y. Cui et al. Sustainable Cities and Society 80 (2022) 103796

Table 7 Table 8
Non-carcinogenic risk assessment of heavy metals in soil, surface water and air. Carcinogenic risk assessment of heavy metals in soil, water and air.
Media Group Element HQing HQinh HQder HI Media Group Element ILCRing ILCRinh ILCRder ILCR

Soil Adult Cr(VI) 3.10 × 9.92 × 1.36 × 1.49 × Soil Adult Cr(VI) 3.16 × 9.53 × 2.74 × 3.43 ×
10− 3 10− 3 10− 1 10− 1 10− 4 10− 7 10− 5 10− 4
Cu 7.40 × 2.24 × 6.44 × 8.06 × Ni 1.40 × 4.24 × 6.09 × 1.41 ×
10− 4 10− 6 10− 4 10− 4 10− 5 10− 8 10− 8 10− 5
Ni 2.43 × 7.36 × 3.92 × 2.48 × Child Cr(VI) 6.88 × 2.61 × 4.40 × 7.32 ×
10− 3 10− 6 10− 5 10− 3 10− 4 10− 7 10− 5 10− 4
Pb 1.17 × 3.53 × 1.37 × 1.18 × Ni 3.06 × 1.16 × 9.80 × 3.07 ×
10− 2 10− 5 10− 6 10− 2 10− 5 10− 8 10− 8 10− 5
Zn 3.35 × 1.02 × 4.38 × 3.80 × Surface Adult Cr(VI) 8.07 × 2.45 × 7.03 × 8.80 ×
10− 4 10− 6 10− 5 10− 4 water 10− 5 10− 7 10− 6 10− 5

1.83 × 9.97 × 1.38 × 1.66 × Ni 6.73 × 2.04 × 2.93 × 6.78 ×
10− 2 10− 3 10− 1 10− 1 10− 6 10− 8 10− 8 10− 6
Child Cr(VI) 6.83 × 2.71 × 2.19 × 2.28 × Child Cr(VI) 4.57 × 1.39 × 3.98 × 4.98 ×
10− 3 10− 3 10− 1 10− 1 10− 4 10− 6 10− 5 10− 4
Cu 1.62 × 6.13 × 1.04 × 1.72 × Ni 1.47 × 5.58 × 4.71 × 1.48 ×
10− 3 10− 7 10− 4 10− 3 10− 5 10− 9 10− 8 10− 5
Ni 5.32 × 4.86 × 6.30 × 5.83 × Air Adult Cr(VI) 4.18 × 1.27 × 3.64 × 4.56 ×
10− 3 10− 6 10− 5 10− 3 10− 4 10− 6 10− 5 10− 4
Pb 2.55 × 9.66 × 2.21 × 2.55 × Ni 1.62 × 4.91 × 7.05 × 1.63 ×
10− 2 10− 5 10− 6 10− 2 10− 5 10− 8 10− 8 10− 5
Zn 7.34 × 2.78 × 7.05 × 8.05 × Child Cr(VI) 9.16 × 3.47 × 5.86 × 9.75 ×
10− 4 10− 7 10− 5 10− 4 10− 4 10− 7 10− 5 10− 4

4.00 × 2.81 × 2.19 × 2.62 × Ni 3.55 × 1.32 × 1.13 × 3.56 ×
10− 2 10− 3 10− 1 10− 1 10− 5 10− 8 10− 7 10− 5
Surface Adult Cr(VI) 8.01 × 2.55 × 3.48 × 3.82 ×
water 10− 4 10− 3 10− 2 10− 2
Cu 5.75 × 1.74 × 5.01 × 6.27 ×
10− 4 10− 6 10− 5 10− 4 Table 9
Ni 1.17 × 3.54 × 1.88 × 1.19 × Comparison with Cr(VI) and Zn concentrations in different regions.
10− 3 10− 6 10− 5 10− 3
Location Region Element Concentrations References
Pb 6.18 × 1.87 × 7.36 × 6.20 ×
(μg/g)
10− 3 10− 5 10− 7 10− 3
Zn 1.24 × 3.75 × 1.61 × 1.40 × Isfahan Iran Cr(VI) 80.87 Mehr et al. (2017)
10− 4 10− 7 10− 5 10− 4 Zn 70.36

8.85 × 2.57 × 3.49 × 4.63 × Johannesburg South Cr(VI) 73.39 Olobatoke and
10− 3 10− 3 10− 2 10− 2 Africa Zn 49.00 Mathuthu (2016)
Child Cr(VI) 1.75 × 6.96 × 5.61 × 5.85 × Ibadan Nigeria Cr(VI) 64.40 Odewande and
10− 3 10− 4 10− 2 10− 2 Zn 20.20 Abimbola (2008)
Cu 1.26 × 4.77 × 8.05 × 1.34 × Cincinnati America Cr(VI) 35.14 Turer, Maynard and
10− 3 10− 7 10− 5 10− 3 Zn 101.00 Sansalone (2001)
Ni 2.56 × 2.26 × 3.03 × 2.59 × Cuenca Ecuador Cr(VI) – Hewitt and Candy
10− 3 10− 6 10− 5 10− 3 Zn 44.00 (1990)
Pb 1.35 × 5.12 × 1.19 × 1.35 × Rural England Cr(VI) 0.0006 Weekes et al. (2007)
10− 2 10− 6 10− 6 10− 2 Zn 2.8986
Zn 2.70 × 1.03 × 2.60 × 2.97 × Shandong China Cr(VI) 68.50 Liu et al. (2022)
10− 4 10− 7 10− 5 10− 4 Zn 64.20

1.93 × 7.04 × 5.62 × 7.62 × Zhejiang China Cr(VI) 38.14 Li et al. (2022)
10− 2 10− 4 10− 2 10− 2 Zn 76.91
Air Adult Cr(VI) 4.15 × 1.32 × 1.81 × 1.98 × Shanxi China Cr(VI) 54.76 Zhan, Hu, Zhen, &
10− 3 10− 2 10− 1 10− 1 Zn 33.80 Rong (2021)
Cu 1.61 × 4.89 × 1.40 × 1.76 × Yunnan China Cr(VI) 51.09 Wang et al. (2022)
10− 3 10− 6 10− 4 10− 3 Zn 381.79
Ni 2.81 × 8.53 × 4.53 × 2.88 × Henan China Cr(VI) 62.74 Wang, Qiao, Zhang,
10− 3 10− 6 10− 5 10− 3 Zn – Yang and Jiang
Pb 8.88 × 2.69 × 1.07 × 8.91 × (2018), Wang, Gui,
10− 2 10− 4 10− 5 10− 2 Cao, Liu and Song
Zn 3.86 × 1.17 × 5.04 × 4.37 × (2018)
10− 4 10− 6 10− 5 10− 4 This study China Cr(VI) 95.54

9.78 × 1.35 × 1.81 × 2.93 × Zn 80.44
10− 2 10− 2 10− 1 10− 1
Child Cr(VI) 9.09 × 3.61 × 2.91 × 3.03 ×
10− 3 10− 3 10− 1 10− 1 hand and mouth exposure under different environmental media was
Cu 3.53 × 1.34 × 2.26 × 3.75 ×
significantly greater than inhalation and skin contact, and the risk of
10− 3 10− 6 10− 4 10− 3
Ni 6.16 × 5.58 × 7.30 × 6.23 × cancer caused by metal elements in children was significantly higher
10− 3 10− 6 10− 5 10− 3 than that in adults.The spatial and temporal distribution of heavy
Pb 1.94 × 7.36 × 1.72 × 1.94 × metals in soil, water and air, linear regression analysis, potential
10− 1 10− 5 10− 5 10− 1 ecological risks and human health risk assessment were analyzed
Zn 8.44 × 3.27 × 8.11 × 9.26 ×
through monitoring heavy metals in different environmental media
10− 4 10− 7 10− 5 10− 4

2.13 × 3.69 × 2.91 × 5.04 × in northeast China, with Jilin Province as the focus. The following
10− 1 10− 3 10− 1 10− 1 conclusions were drawn:

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Y. Cui et al. Sustainable Cities and Society 80 (2022) 103796

6. Suggestions Declaration of Competing Interest

Xi, the general secretary, urges the acceleration in promoting the The authors declare that they have no known competing financial
new era of comprehensive revitalization of Jilin Province and Northeast interests or personal relationships that could have appeared to influence
China, the firm establishment of the concept that clean water and green the work reported in this paper.
mountain is the silver mountain, and the implementation of major
ecological projects, when visiting and inspecting locations including Acknowledgement
Jilin Lishu and Changchun FAW. This paper proposes to reduce heavy
metal pollution from the source, which not only effectively reduces the We greatly appreciate Dr. Mengnan Shen, Dr. Na Li and all who
health hazards of heavy metal pollutants to human beings, but also contributed to this study.
ensures rapid and sustainable development in the treatment, prevention,
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