Process Safety and Environmental Protection 171 (2023) 109–118

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Process Safety and Environmental Protection

journal homepage: www.journals.elsevier.com/process-safety-and-environmental-protection

Risk assessment and source apportionment of heavy metalloids from typical

farmlands provinces in China
Mabinty Sarah Tholley a, Lartey Young George b, Gehui Wang a, Sajid Ullah a, Zhihua Qiao a,
Siyuan Ling a, Jinhong Wu c, *, Cheng Peng a, Wei Zhang a, **
a
State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, School of Resource and Environmental Engineering,
East China University of Science and Technology, Shanghai 200237, PR China
b
State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering of Tongji University, Shanghai 200092, PR China
c
Shanghai Yaxin Urban Construction Co., Ltd., Shanghai 200436, PR China

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

Keywords: Potentially toxic metals in farmland soil have recently become a significant environmental concern in China. In
Farmland soils this study, the occurrence and distribution of eight (8) heavy metals (HMs) were investigated from 54 topsoil
Heavy metals samples obtained across 18 provinces. Human health and ecological hazards associated with HMs were assessed
Multivariate analysis
through different risk characterization indices and their sources predicted. The statistically mean concentrations
Risk assessment
Source apportionment
of HMs ranged from 0.08 to 70.05 mg kg− 1, which were below the determined threshold values for agricultural
lands according to the Chinese National Standard (GB 15618–2018). The respective ecological risk index (Eir ) of
HMs revealed that they posed a lower risk (Eir < 40) but their potential cumulative ecological risk (RI) was
determined as a considerable risk (300 ≤ RI < 600). Spatial distribution and heterogeneities of HMs were found
to be highly concentrated in the southern parts (e.g., Yunnan, Guangdong) of China, particularly for Arsenic (As),
Zinc (Zn), and Chromium (Cr). PMF model was found capable of efficiently elucidating respective sources of HMs
across the studied provinces as most were impacted by geological/pedogenic and anthropogenic activities (e.g.,
agricultural, industrial discharge fallouts). Probabilistic health risk assessment indicated that the non-
carcinogenic risk (NCR) and total carcinogenic risk (TCR) of HMs in both adults and children were low and
acceptable.

1. Introduction
Heavy metals (HMs) are a category of metalloids whose densities are
> 5 g cm− 3 on the periodic table (Oves et al., 2012). They are either of
natural origin over a long period of geological and lithological formation
or generated by human activities in different environmental matrices
(Chen et al., 2014). When their concentrations exceed, the tolerant loads
of the media in which they occur, HMs become classified as pollutants
decreasing the quality of soil and water resources (Wei et al., 2016).
Heavy metals (HMs) contamination in farmland soils has become an
important research avenue globally and mostly in China due to intensive
industrialization near agricultural establishments (Cai et al., 2019b; Dai
et al., 2018; Sun et al., 2013). Approximately 82.4% of polluted soils in
China are associated with HMs with the remaining 17.6% caused by
organic pollutants (Shifaw, 2018). According to China’s National Soil
Pollution Survey (2014), the general soil atmosphere is not conducive to
good health, with approximately 19.4% of farmland soils falling below
compliance limits of the Chinese Environmental Quality Standard for
Soils (Deng et al., 2016). According to the report, China’s soil has been
deteriorating and with the long-term cumulative conversion of rural
arable land to industrial activities, which could potentially become se­
vere. These have resulted in HMs pollution in farmlands soils that have
impacted crop yield (Deng et al., 2016). For instance, there have been
reported incidences of high Cd and Ni pollution rates of 7.2% and
3.04%, respectively, as well as a 2% Cu and Hg pollution rate (Teng
et al., 2014). Similarly, high levels of Cd (1.4 mg kg− 1), As
(39 mg kg− 1), Hg (1.4 mg kg− 1), and Pb (140 mg kg− 1) were found to
have been naturally generated in soils over time without any human
impacts in a study conducted (Yang et al., 2013). These naturally high
cumulative concentrations of HMs and their ecotoxicological effects on

* Corresponding author.
** Correspondence to: Box 563, 130 Meilong Road, Shanghai, China.
E-mail addresses: wu20092310222@126.com (J. Wu), wzhang@ecust.edu.cn (W. Zhang).

https://doi.org/10.1016/j.psep.2022.12.092
Received 14 November 2022; Received in revised form 23 December 2022; Accepted 31 December 2022
Available online 2 January 2023
0957-5820/© 2023 Institution of Chemical Engineers. Published by Elsevier Ltd. All rights reserved.
M.S. Tholley et al.
plants in farming soils have been of critical concern to researchers (Rai
et al., 2019).
The release of different ranges of HMs into different soil types and
land uses across China has been recognized (Li et al., 2015). A major
source of HMs introduction into arable soils is via fertilizers which have
piqued attention due to their possible environmental hazard. Chemical
fertilizers, such as phosphate fertilizers, are the primary source of trace
metals among all inorganic fertilizers (Ahemad and Kibret, 2014;
Toader-Williams and Golubkina, 2009), while considerable emphasis
has been paid to the concentration of Cd in phosphate fertilizers. Since
clean-up and implementation of remediation programs for
HMs-contaminated sites are technically challenging, the health risks of
HMs from soils to different ranges of Chinese populations are dire. In the
European Union (EU) alone, it is estimated that approximately €17.3
billion would be needed annually to remediate sites contaminated by
HMs which underlines the critical extent of the problem in the continent
(Chen et al., 2018; Montanarella and Panagos, 2021; Tóth et al., 2016).
Therefore, options for the identification and management of
HMs-contaminated sources to control the risks of exposure become
paramount (Su et al., 2014).
HMs can affect human health, especially through children’s body
contact and unintentional ingestion of different items orally at play­
grounds and streets which are exposed to contamination (Saeedi et al.,
2012). They can also bind to soil particles and become suspended in the
atmosphere making it easy to inhalation. HMs contamination can also
disrupt the ecological functioning of water quality and damage the
health of green plants (Lu et al., 2007). Although some studies have
looked into heavy metal infusion in agricultural areas, where oral
ingestion has been considered the main route for human contact with
soils (Gao et al., 2021), further research is needed to provide a theo­
retical basis for more effective pollution management on farmland soils.
Researchers have adopted the potential ecological risk index (PERI) to
determine the pollution level of HMs in soils (Li et al., 2017; Wang et al.,
2015) based on their concentrations, speciation, and distribution. Sto­
chastic models and receptor models are efficient means to predict HM
identification in soil. Such stochastic models are essential approaches
based on the statistical analysis of sampled data along with corre­
sponding environmental parameters for source identification. None­
theless, these stochastic models are highly dependent on prior
knowledge of the source profiles and such knowledge could lead to an
underestimation of results. Different tools have been applied as single or
combined to efficiently quantify the contributing sources of HMs in soils.
These include multivariate statistics i.e., principal component analysis
(PCA), factor analysis, cluster analysis, geostatistics, and isotope tracer
analysis. Although these methods have been confirmed to be successful,
they tend to present some drawbacks in terms of quantifying the source
contribution of HMs. For instance, the multivariate analysis relies on the
elements of good correlations which are extracted into the same classi­
fication (Zhang et al., 2018). Isotope tracer analysis tends to rely on the
specific isotope composition of different sources to determine the main
sources of HMs pollution and hence heavily dwells on accurate results of
HMs isotopic composition (Cheng and Hu, 2010). Geographical distri­
bution approaches using spatial interpolation techniques have also been
used. However, spatial representation depends on sampling locations
and quantity (Wang et al., 2010). USEPA UNMIX is a non-negative
constraint factor analysis method developed using the self-modeling
curve resolution (SCMR) technique. It has been often used to deter­
mine the source distribution of HMs in sediments. The PMF is a matrix
decomposition method using non-negative constraint conditions, which
can manipulate missing and inexact data. As such, it is a simple and
feasible source analysis method (Lv, 2019).
In this study, we explored the pollution levels of the targeted HMs,
copper (Cu), zinc (Zn), cadmium (Cd), nickel (Ni), lead (Pb), chromium
(Cr), mercury (Hg), and arsenic (As) based on previous knowledge that
their contamination in the soil can be deleterious to humans and the
ecosystem and provided current datasets on their contamination levels
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Process Safety and Environmental Protection 171 (2023) 109–118
(Yang et al., 2018; Yuan et al., 2021). We comprehensively evaluated
their concentrations and spatial distributions, the correlation between
these pollutants and soil properties (soil pH, organic matter, electrical
capacity and cation exchange capacity), and then assessed their human
and ecological hazards and determined their source apportionment.
2. Materials and methods
2.1. Study areas
The study areas involved 18 provinces selected across China in Fig. 1.
Random selection and identification of farmlands in the respective
provinces were targeted to provide the needed current datasets on HMs.
The provinces included; Xinjiang, Ningxia, and Shaanxi provinces
located in northwest China; Yunnan and Chongqing provinces in
southwest China; Guangdong and Hainan provinces in the south of
China; Zhejiang, Jiangxi, and Anhui provinces in eastern China; Henan,
Hunan, and Hubei provinces in central of China; Beijing, Hebei, and
Shanxi provinces in northern China; Jilin and Heilongjiang provinces in
northeastern China. The abbreviation of provinces as indicated in Fig. 1
is shown in Table S1.
2.2. Soil sampling
54 topsoil samples (0–10 cm), 3 samples from each province were
collected from all hydrodynamic farmlands in the respective study areas.
The geographical coordinates of each sample source were recorded.
Each fine soil sample of 0.4–1.0 kg was separated into 4–6 sub-samples
and kept in polythene resealable bags, labeled by description and sent to
a laboratory for analysis. The soil samples were dried at room temper­
ature (≈25 ◦ C), pulverized, and sieved with 2 mm nylon to remove the
roots, stones, and other larger debris.
2.3. Experimental reagents, materials and quality control
For heavy metal detection, experimental reagents used were mixed
Ion Reference Standard for Plasma Emission Spectroscopy [GBW (E)
060668) 100 mL. 1 mg L− 1 of heavy metal (Cu, Zn, Pb, Ni, Cr, Hg, Cd, &
As) solutions were supplied by Shanghai Metrology and Testing Tech­
nology Institute (Shanghai, China P.R.). Concentrated nitric acid (pro­
cess ultra-pure, 65%), concentrated hydrochloric acid (excellent grade
pure), perchloric acid (analytical peroxide pure), and hydrogen (excel­
lent grade pure) were obtained from Sinopharm Chemical Reagent Co.,
Ltd. (Shanghai, China P.R). Before and after usage, the glass instruments
were soaked in 10% dilute nitric acid for 48 h, cleaned three times with
deionized water (Milli-Q system) and ultrapure water, and dried at
temperature 105 ◦ C.
2.4. Sample extraction and analysis
The pre-treatment approach was used to prepare and extract sam­
ples. 0.1 g of soil was placed in a closed Teflon digestion canister with
6 mL of aqua regia. The samples were digested according to the refer­
ence microwave digestion procedure (Bettinelli et al., 2000), with set
conditions of 10 min at room temperature to 120 ◦ C for 10 min, 5 min at
150 ◦ C for 20 min, 5 min at 160 ◦ C for 20 min. The extract was
collected, placed in an acid catcher, cooled and analyzed by ICP-MS
analysis (Mao et al., 2017). To guarantee the accuracy and reliability
of the test, the limits of detection (LODs) for 8 heavy metals varied in a
range of 0.02–1.00 ug L− 1, and the limits of quantification (LODs) were
defined as three times the LOD values ranging from 0.006 to
3.00 ug L− 1. Recovery values for all analytical elements were calculated
between 76.3% and 117.2% and the relative standard deviation (RSDs,
n = 6) was lower than 10%.
Soil pH was determined by the methods described in a previous study
(Kicińska et al., 2022). Organic matter content was determined per
M.S. Tholley et al. Process Safety and Environmental Protection 171 (2023) 109–118

Fig. 1. Study areas and sampling locations.

potassium dichromate oxidation-external heating method (Xiang et al., sample source, (mg kg− 1);Cin refers to the background value (mg kg− 1).
2020) after soil samples were calcined for 4 h in a muffle furnace at Tir values correspond to Cd = 30, Cr = 2, Zn = 1, Pb = Cu = 5, Hg = 40,
450 ◦ C. Electrical Conductivity (EC) was measured by HJ 802–2016 and As = 10 (Huang et al., 2015). Table S2 illustrates the adopted Igeo
(Chinese Industry Standard). Suspensions of 1:5 soil-water ratio were classification system.
centrifuged at 4000 r min− 1 for 10 min, and the retrieved supernatants
were used to test for EC. Cation exchange capacity (CEC) was measured 2.5.2. Ecological risk
by the EDTA-ammonium salt quick technique (Begheyn, 1987). Physical Ecological risks for heavy metals across the study areas were eval­
parameters including soil texture and particle compositions were also uated using the two ecological risk indices i.e., the Improved Nemerow
studied. In addition, to obtain the different soil particle sizes, the soil Index (INI) and Total Potential Ecological Risk Index (RI) following (Eqs.
samples were first passed through a < 0.002 mm sieve, then a (3) and (4)) (Hakanson, 1980).
0.002–0.05 mm and 0.05–2.00 mm sieve respectively. √̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
Igeo2 max + Igeo2 avg
INI = (3)
2
2.5. Assessment approach
∑
m

2.5.1. Assessment of pollution indices RI = Eir (4)

i=1
To assess the pollution levels of heavy metals in farmland soils across
the study areas, the two geochemical pollution indices i.e., Geo- where Igeomax and Igeoavg refer to the maximum and mean of Igeo of heavy
accumulation Index (Igeo) and Ecological Risk Index (Eir )were applied metals. The classification levels of RI and INI were described by Yuanan
(Eqs. (1) and (2)) (Huang et al., 2021). et al. (2020) and illustrated in Table S3.
( )
Cis
Igeo = log2 (1) 2.5.3. Source apportionment
1.5 x Cin
Positive Matrix Factorization (PMF) model with multivariate prin­
cipal component analysis (PCA) was used to quantitatively estimate the
T ir x Cis
Eir = T ir Cir = (2) degree to which various heavy metals contributed to the pollution load
Cin across the study area. The PMF model estimation is based on the
reduction of the objective function, and Q is based on the equation (Eqs.
where i is the heavy metal element content; r is the sampling point; Tir is
(5)–(8)).
the toxic reaction factor (unitless); Cir is the single pollution coefficient
(unitless); Cis is the calculated heavy metal concentration from the

111
M.S. Tholley et al. Process Safety and Environmental Protection 171 (2023) 109–118

p
∑ threshold (RfD, mg kg− 1 d− 1) and slope factors (SF, mg kg− 1
d− 1) values
Cij = gik fkj + eij (5) are presented in Table S5.
k=1

⎛ p
∑ ⎞2
m ⎜xij − gik fkj 2.6. Software and data analysis
∑
n ∑ ⎟
Q= ⎜
⎝
k=1 ⎟
⎠ (6)
i− 1 j=1
Uij All statistical computations were performed in Microsoft Excel 2019
and OriginPro 2021b (OriginLab Corporation, Northampton, USA). All
spatial maps were generated in ArcGIS 10.7 (ESRI Inc, Redlands, CA).
5
forc ≤ MDL, uij = MDL (7) Pearson correlation analysis was used to determine the association be­
6
tween heavy metals and heavy metals and soil properties. PMF model
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
( )2̅ was built using approved USEPA PMF v5.0 (USEPA, USA). Spatial
MDL
uij = (Errorfractionxc) + 2
(8) interpolation by kriging was adopted to determine the spatial extent and
2
distribution of heavy metals and confirm PMF outputs. Probabilistic
human health risk analysis was performed by Monte Carlo Simulation
where i, j, and k signify the number of samples, elements, and different
over 10,000 runs in Oracle Crystal Ball (v11.1.2.3), a Microsoft Excel
sources, respectively; Cij means the element content; g means the source
Add-in. The model data distributions and set-up are illustrated in
contribution; fkj denotes the element amount of source; eik means the
Table S3.
residual; uij refers to the element uncertainty; MDL stands for the spe­
cies-specific method detection limit, and Error fraction suggests the
3. Results and discussions
percentage for measurement uncertainty.

3.1. Statistical analysis and general behavior of heavy metals

2.5.4. Human health hazard analysis
To estimate the human health risk of heavy metals in farming soils,
A statistical overview of HMs concentrations is presented in Table S6.
this study employed the exposure model approach recommended by the
Mean concentrations (mg kg− 1) of investigated heavy metals were Cr
USEPA in ‘’Risk Assessment Guidance for Superfund, Vol. I: Human
(60), Ni (36.87), Cu (27.82), Zn (70.05), Cd (0.28), Pb (26.60), Hg (0.08)
Health Evaluation Manual’’. Inhalation of suspended air particles
and As (7.57). Ni, Zn, Cu and Cr showed high accumulation, indicating
through the nose and mouth (Minh-s), direct ingestion of substrate par­
that they were most likely generated by human activities (Luo et al.,
ticles (Ming-s), and absorption of elements in particles adhering to
2009). The statistical mean concentrations of HMs were generally below
exposed skin are the three main mechanisms by which pollutants in the
the threshold values of GB 15618–2018. Soil pH is an important
soil reach the body (Mder-s) (Zupančič et al., 2021). This study used a
chemical feature since it regulates a variety of other soil physicochem­
specialized approach for human soil exposure when conducting expo­
ical properties. Soil pH varied from 4.91 to 8.89, with a mean of 6.96 and
sure analysis, with a special focus on children’s noncarcinogen expo­
approximately 60% being acidic with pH < 7. The acidic nature of the
sure. The elemental dosage (M, mg kg− 1 d− 1) intake by adults and
soil could be attributed to the high application of nitrogen-based fer­
children through each of these pathways is determined using the
tilizers (Guo et al., 2010; Xun et al., 2017). The mean values of organic
following equation (Eqs. (9)–(13)):
matter (OM) ranged from 3.31 to 54.71 g kg− 1 which could infer the
( )
Oral dose Ming− s : Ming− s =
Cs × IngR × EF × ED × CF
(9) soils across the study areas were productive (OM > 1%). Soil EC on
BW × AT average was 0.30 ms cm− 1 across all samples while CEC was 15.06 cmol
kg− 1. A higher CEC implies that the soils could bind and hold nutrients
Cs × InhR × EF × ED
Inhalation(Minh− s ) : Minh− s = (10) maintaining their productivity over time. The average particle compo­
BW × AT × PEF
sition of soils was 25.20% 0.002 mm, 49.69% 0.002–0.05 mm and
Cs × SA × SL × ABS × EF × ED × CF 25.10% 0.05–2.00 mm, respectively. Comparative evaluation in Fig. 2,
Dermal dose(Mder− s ) : Mder =
BW × AT of the mean concentrations in this study to other reported results,
(11)

∑ ∑ADI ij
HI = HQi = (12)
RfDij
∑ ∑
TCR = CRi = ADI ij xSF ij (13)

where Cs is the concentration of pollutants in soil (mg kg− 1), EF is the

exposure frequency (days year− 1), ED is the exposure duration (years),
PEF is the soil-to-air particulate emission factor (m3 kg− 1), IngR is the
receptor soil ingestion rate (mg d− 1), InhR is the receptor soil inhalation
rate (m3 d− 1), SA is the skin surface area available for exposure (cm2), SL
is the soil-to-skin adherence factor (mg cm− 2 event− 1), ABS is the dermal
dimensionless factor, BW is the time-averaged body weight (kg), and AT
is the average time of noncarcinogenic and carcinogenic risks (days).
Specific parameters for the estimation of non-carcinogenic risk are
provided in Table S3.
For non-carcinogenic risk (NCR), HI refers to all sum of HQ (Hazard
Quotients) in heavy metals. HI > 1 represents the potential adverse ef­
fect on human health. For Total Carcinogenic Risk (TCR) and Carcino­
genic Risk (CR), the values TCR & CR < 10− 6, 10− 6 < TCR & CR < 10− 4,
and TCR and 10− 4 represent no health risk, no significant health risk and
high health risk, respectively (Zhang et al., 2020). The specific toxicity Fig. 2. Comparison of heavy metals in farmlands in China and other studies.

112
M.S. Tholley et al.
revealed that HMs concentrations across the farmlands in the studied
provinces were on average lower than those in some European states
(Salminen et al., 1998), Canada (Saint-Laurent et al., 2010), USA
(Nahlik et al., 2019), Greece (Kelepertzis, 2014), and India (Adimalla
et al., 2019). Specifically, Cr, Ni, Cu, Zn, and As concentrations across
the studied provinces were higher than those in Europe and USA but
lower than those in India, Korea, Greece, and Canada while Cd was
lower than the reported concentrations in Greece, India, Canada and
USA, respectively. The variations in the concentrations could be due to
the differences in geological, agricultural, industrial, and human activ­
ities in research areas (Adimalla et al., 2019; Luo et al., 2009).
3.2. Environmental risk analysis of heavy metals
Igeo and Eir values were determined to evaluate the extent of
contamination by these HMs. Except for Cd and Hg which indicated Igeo
values (Igeo ≤ 0) i.e., uncontaminated, all other HMs were found to
contribute to overall cumulative contamination of soils with Igeo values
in the category of ‘extremely contaminated’ (Igeo ≥ 5). These could be
associated with high industrial emission influences, agricultural activ­
ities, and other anthropogenic sources e.g. HMs from unleaded fuel
emissions (Du et al., 2019). Determined INI values could classify the
soils in the study areas at ‘class 6, extremely contaminated’ (INI ≥ 5)
mostly contributed by Cr, Ni, Cd, Cu, Pb and As. These were visually
observed in Fig. 3, as HMs contamination spatially varied per location
with high-density concentrations in the southern parts of the study areas
based on the INI and RI-determined values. This could be attributed to
high agricultural and industrial activities in the areas mostly in the south
of China represented in this study by Guangdong (industrial), and
Yunnan (agricultural). The northwestern province is noted for high
agricultural activities. The ecological risk values for each HM are rep­
resented in Table S7.
3.3. Spatial association and source apportionment of heavy metals
As shown in Fig. S1, the spatial distribution of heavy metals can be
used to identify heavily polluted areas and deduce potential sources of
metal origins (Cai et al., 2019a). The provincial distributions of Pb, Cr,
Ni, Cu, As, and Zn could reveal comparable contamination trends, where
parental pedogenic processes and materials influenced the soils (Lv,
2019; Sun et al., 2019; Wang et al., 2019b). Provincial differences in
agricultural, anthropogenic activities manufacturing and industrial ac­
tivities were principally responsible for their spatial structure. The
highest concentration of Ni was found in the South. Vehicular emissions
and transport to nearby farmlands are a substantial contribution to Pb
accumulation (50–60%) (Wang et al., 2019a). Agricultural activities,
Fig. 3. Contamination evaluation for heavy metal of farmland with Improved Nemerow Index (INI) and potential ecological risk index (RI).
113
Process Safety and Environmental Protection 171 (2023) 109–118
such as the application of fertilizers (livestock dung and phosphate
fertilizers), were found to be the predominant source of Zn in another
study (Sun et al., 2013). Cd concentrations were low or absent in most
farmland soils but were slightly higher in Henan, Ningxia, and Shaanxi
in the Northwest, Beijing/Heilongjiang in the North/Northeast,
Anhui/Zhejiang in the East, and Hainan in the South, indicating that the
soils had been impacted by serious agricultural activities, particularly
the use of a large number of organic fertilizers. In the farming soils of
Henan, Ningxia, and Chongqing in the Northeast/Northwest, Anhui/Z­
hejiang in the East, and Hainan in the South, Hg was regionally
distributed. Hg concentration in soil could be associated with high
traffic density, industrial operations, and municipal waste dis­
charge/leakages to nearby farmlands (Davis et al., 2009; Rodríguez
Martín et al., 2006).
Pearson correlation analyses of heavy metals and heavy metals with
soil properties are presented in Fig. 4. Fig. 4a revealed significant pos­
itive and negative correlations within the different HMs. For example,
Pb displayed a positive association with Cr (r = 0.72) and Cd (r = 0.49),
while Cu and Zn positively correlated with Ni at r = 0.94 and 0.48
respectively. Meanwhile, there were some negative associations dis­
played by As and Ni (r = − 0.55) and Cu (r = − 0.53). Fig. 4b showed
that soil pH is the major influencing property of most physicochemical
parameters indicating a significant negative relationship with Ni
(r = − 0.61), and Cu (r = − 0.57). CEC also showed a positive weak
correlation with pH. In terms of soil particle size composition, there
were strong associations with the various heavy metal groups. The large
particle composition (PC1) showed a strong positive association with
soil pH (r = 0.65) but a negative association with Hg (r = − 0.47).
Similar negative correlations were observed with PC2 (medium) with Ni
(r = − 0.5) and Cu (r = − 0.48) and PC3 (large) at r = − 0.50.
Heavy metals sources analyses by PCA in Fig. 5a showed that the
three components comprising PC1 (39.4%), PC2 (30.8%), and PC3
(12.7%) could best display the spatial variation of heavy metals in the
study areas contributed by the first 3 PCs with eigenvalues (>1). While
PC1 indicated the largest source of variation, PC2 showed an inverse
association between Hg and Cr, Pb, As, Cd, and Zn which could infer that
it could be generated from a different source. On the contrary, Cr, Pb and
As increased proportionally, but Cr exhibited an inverse association with
Cd and Zn which could infer their potentially different generating
sources. A similar proportional relationship between Ni and Cu was
observed along the PC3 axes. In summary, these findings suggested that
heavy metals had some unique associations and a high likelihood of
forming synergies, potentially leading to chemical contamination
(Covelo et al., 2007). Further spatial apportionment to predict the high
efficiency of heavy metals source generation with PMF could reveal
several factors’ contributions as shown in Fig. 5b. Factor 1 as
M.S. Tholley et al.
Fig. 4. Pearson correlation plot of the association between (a) heavy metals and (b) heavy metals and soil properties.
Fig. 5. Source apportionment for heavy metals (HMs) of farmland in the study areas. (a) Factor profiles of HMs in farmland derived from the positive matrix
factorization (PMF) model. (b) Principal component analysis (PCA) 3D biplot of HMs.
recommended by PMF was heavily loaded on Pb > Zn > As > Cu > Hg.
The elements could be associated with lithogenic and industrial
discharge sources. Pb, Zn and Cu are typical industrial pollutants
derived from wastewater and leaded gasoline (Jing et al., 2018) and
hence could be originated from similar sources while As is typically
derived from pedogenic and geodetic processes (Meharg and Meharg,
2021). The observation was similar to the spatial trends depicted. Factor
2 was heavily loaded on Cd > Ni > As > Hg > Pb > Cr. The spatial
distribution could reveal a distinction in the sources’ generation of the
elements as their distribution varied significantly. This could infer
different industrial, natural and anthropogenic factors contributing to
their generation. Majorly, it is reported that the historical application of
As, Hg, and Pb-based fertilizers and the application of feed additives
containing Cd and Pb in large-scale agriculture could impact farmland
soils (Liu et al., 2021; Xu et al., 2021) and hence in this case Factors
could be associated with agricultural activities. Factor 3 was heavily
loaded on Ni > Cr > Cu > Zn > Cd. The ranges of elements exhibited are
of typical industrial ranges and components of major electrical products
and hence could be associated with their source (Meng et al., 2021). This
was in association with the spatial distributions, as high concentrations
of the elements were displayed in southwestern parts of the study areas
where there are high industrial operations. Factor 4 had a high loading
on Cr > Zn > As > Pb > Cu. The spatial distributions of the elements
were quite similar with sparingly low concentrations in the north and
high concentrations in the southern part of the study areas. The
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Process Safety and Environmental Protection 171 (2023) 109–118
contribution sources in the northern parts could be associated with
agricultural and anthropogenic activities while the southern part is
dominated by industrial emissions hence Factor 4 could be assigned as
potentially a mixed source. Similar observations were reported in a
previous study (Zeng et al., 2022). Factor 5 displayed high loading ac­
cording to Hg > Cu > Cd > Zn. Although Hg could exist naturally, its
spatial distribution in the study areas was heavily concentrated in the
central partition of southern China which is highly noted for industrial
operations. This was similar to other elements in the group which could
confirm assigning Factor 5 as a major industrial source (Ma et al., 2016).
3.4. Probabilistic health risk assessment
The non-carcinogenic (NCR) and carcinogenic (CR) health risks of
heavy metals to adults and children were predicted and the results are
illustrated in Figs. 6 and 7. NCR values were examined along the three
exposure pathways including ingestion (HQing), inhalation (HQinh), and
dermal (HQder). The average adult mean NCR hazard quotient (HQ) for
HMs were 1.42 × 10− 2, 9.3 × 10− 4, and 1.52 × 10− 3, respectively, for
oral dosage, inhalation, and dermal exposure pathways shown in
Table S8. Cu had the lowest mean HQ value of 1.8 × 10− 3, indicating
that it has a lower danger than the others. However, Cd and Hg had the
highest mean HQ values of 6.34 × 10− 4 and 6.31 × 10− 3, respectively,
indicating that they could pose a greater risk to adults than the other
heavy metals. Cd also had the highest HQinh of 7.53, indicating that it
M.S. Tholley et al.
Fig. 6. Probability distribution plots of heavy metals non-carcinogenic hazard quotient.
can cause more health impacts through inhalation (nose) than through
oral dose (mouth) or dermal (skin) exposure. Mean values for NCR
hazards in children were 9.30 × 10− 2, 9.34 × 10− 5, and 2.70 × 10− 3,
respectively. Individual mean HQ values varied from 2.04 × 10− 2 to
7.7 × 10− 3 with Cu having the highest HQing of 7.7 × 10− 3 indicating
that children are the most likely to be exposed to Cu through oral dose
(mouth) than through other routes. Furthermore, the high Zn values in
HQinh and HQder than other heavy metals. Zn, on the other hand, could
cause more health problems in children through inhalation (through the
nose) and dermal (skin contact) exposure than all other heavy metals.
However, comparing the carcinogenic risks (CR) of adults to children
revealed that Cr, Ni, Cd, Pb, and As could result in more health effects on
children than adults as shown in Table S9. The mean CR values for adults
were from 7.7 × 10− 6, 1.36 × 10− 7, and 7.07 × 10− 7 for ingestion,
inhalation and dermal pathways. Inhalation could therefore be the
highest exposure risk route for adults. Individually, Cd had the highest
CR value at 9.46 × 10− 7. For children, the mean CR values for ingestion
(1.27 ×10− 5), inhalation (6.61 ×10− 8) and dermal (8.79 ×10− 7) indi­
cate that oral exposure could be the most likely severe threat to children.
This is because children are susceptible receptors, and some preventive
measures should be taken, such as prohibiting the presence of children
near or around farming areas, etc., which is consistent with previous
115
Process Safety and Environmental Protection 171 (2023) 109–118
studies both in China (Huang et al., 2015), and other parts of the world
(Alsafran et al., 2021). Following the probability distribution in Fig. 6,
the predicted NCR from all heavy metals seemed to follow a similar
pattern with no exceedance of the threshold limits in adults or children
for the heavy metals studied. The predicted mean values ranged from
1 × 10− 5 to 4.3 × 10 in adults while for children, the means ranged
from 3.3 × 10− 5 to 1.3 × 10− 3. The carcinogenic risks of three metal­
loids, Cr, Cd and As are illustrated in Fig. 7. The CR values were in the
range of 3.2 × 10− 7 to 1.7 × 10− 3. Similar observations of predicted
heavy metals exceedance were reported by (Zeng et al., 2019) who
found that As in farmland soils of China could reach up to 6.03 × 10− 8 to
5.24 × 10− 3. The results are indicative that future monitoring of the
health risks of heavy metals in farmlands is critical and remediation
measures must be implemented.
4. Conclusions
This study presents current results on the distribution and charac­
teristics of heavy metals as pollutants in farmland soils across 18 prov­
inces in China. The soil samples contained more than 1% organic matter,
ranging from 3.31 to 54.71 g kg− 1, which implied that the soils in this
study were productive. Overall, the HMs values were below the
M.S. Tholley et al.
Fig. 7. Probability distribution plots of heavy metals carcinogenic risk index. (a) Cr, (b) Cd, (c) As, (d) Pb, (e) Ni.
determined threshold limits with the maximum mean recorded by Zn
(70.05 mg kg− 1). Most of the metal species studied indicated a strong
positive correlation within the sample groups. According to the spatial
distribution results, heavy metals pollution exhibited different regional
distributions, with the Southeast having higher levels of pollution and
was more prevalent in the South, Southeast, North, and East, while it
was less prevalent in the West. A further prediction of the HMs sources
with PMF and PCA tended to provide a high efficiency of prediction.
However, due to different provincial pollution sources, source analyses
of HMs must be based on the local setting description. Meanwhile, we
found the industrial and agricultural inputs sources as the main
contributing factors. Also, the comparison of the mean concentrations of
116
Process Safety and Environmental Protection 171 (2023) 109–118
heavy metals pollutants in soils in this study (China) to similar studies
conducted in other countries outcome was, that Hg concentration in soil
in Europe was less than in China (this study) with mean values of 0.03
and 0.07 mg kg− 1 respectively. The probabilistic risks of HMs deter­
mined by NCR and TCR were both acceptable. Nonetheless, to provide
more scientific evidence to facilitate the remediation of HMs-
contaminated soils, further research should be conducted across the
provinces to provide deeper insights into the correlation between soil
properties and HMs.
M.S. Tholley et al.
CRediT authorship contribution statement
Mabinty Sarah Tholley: Investigation, Data curation, Writing −
original draft preparation. Lartey-Young George: Statistical/spatial
analysis, visualization, Writing − review & editing. Gehui Wang, Sajid
Ullah, Zhihua Qiao, Siyuan Ling: Investigation, visualization, Writing
− review & editing. Jinhong Wu: Validation, Funding, Project admin­
istration, Resources. Cheng Peng: Writing − review & editing. Wei
Zhang: Conceptualization, Project administration, Supervision, Re­
sources, Validation, Funding, Writing − review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgment
This research was supported by the projects of the National Key
Research and Development Program of China (2022YFC3902503), the
Special Fund of the State Environmental Protection Engineering Center
for Urban Soil Contamination Control and Remediation (USCR-202206),
and the National Natural Science Foundation of China (41877124,
21737005, 42177395).
Appendix A. Supporting information
Supplementary data associated with this article can be found in the
online version at doi:10.1016/j.psep.2022.12.092.
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