Journal of Hazardous Materials 438 (2022) 129468

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Journal of Hazardous Materials

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

Research Paper

Apportionment and location of heavy metal(loid)s pollution sources for soil

and dust using the combination of principal component analysis,
Geodetector, and multiple linear regression of distance
Weibin Zeng a, b, Xiaoming Wan a, b, *, Lingqing Wang a, b, Mei Lei a, b, Tongbin Chen a, b,
Gaoquan Gu a, b
a
Institute of Geographic Sciences and Natural Resources Research, Chinese Academy of Sciences, Beijing 100101, China
b
University of Chinese Academy of Sciences, Beijing 100049, China

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• PCA- Geodetector-MLRD was used to

determine the location of the sources,
not just the type of source.
• The river, main road, mining area, metal
plant, and community can significantly
explain the PCA factors.
• A distance-based prediction model for
heavy metal concentration was estab­
lished and its effectiveness was verified.

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

Editor: Jörg Rinklebe The accurate identification of sources for soil heavy metal(loid) is difficult, especially for multi-functional parks,
which include multiple pollution sources. Aiming to identify the apportionment and location of heavy metal
Keywords: (loid)s pollution sources, this study established a method combining principal component analysis (PCA),
Dust Geodetector, and multiple linear regression of distance (MLRD) in soil and dust, taking a multi-functional in­
Ecological risk
dustrial park in Anhui Province, China, as an example. PCA and Geodetector were used to determine the type and
Heavy metal(loid)
possible location of the source. Source apportionment of individual elements is achieved by MLRD. The detection
Soil
Source identification results quantified the spatial explanatory power (0.21 ≤ q ≤ 0.51) of the potential source targets (e.g., river and
mining area) for the PCA factors. A comparative analysis of the regression equation (Model 1 and Model 3)
indicated that the river (0.50 ≤ R2 ≤0.78), main road (0.47 ≤ R2 ≤ 0.81), and mine (0.14 ≤ R2 ≤ 0.92) (p < 0.01)
were the main sources. Different from the traditional source apportionment methods, the current method could
obtain the exact contributing sources, not just the type of source (e.g., industrial activities), which could be useful
for pollution control in areas with multiple sources.

* Corresponding author at: Institute of Geographic Sciences and Natural Resources Research, Chinese Academy of Sciences, Beijing 100101, China.
E-mail address: wanxm.06s@igsnrr.ac.cn (X. Wan).

https://doi.org/10.1016/j.jhazmat.2022.129468
Received 5 May 2022; Received in revised form 10 June 2022; Accepted 24 June 2022
Available online 27 June 2022
0304-3894/© 2022 Elsevier B.V. All rights reserved.
W. Zeng et al.
1. Introduction
Heavy metal(loid)s are among the main pollutants of sites (Safari and
Delavar, 2019; Zhao et al., 2015; Wu et al., 2021). The land used by
industrial enterprises presents environmental problems, such as soil and
waste pollution (Pyatt et al., 2002; Z. Zhang et al., 2012a; Zhang et al.,
2012b; Jia et al., 2019; Dhaliwal et al., 2020). Thus, risk control stra­
tegies should be applied to these areas (Liu et al., 2020). The identifi­
cation of potential pollution sources is the basis of risk control, and the
source analysis of heavy metal(loid)s in soil has been one of the most
important topics in recent years (Yang et al., 2017, 2020; Hu et al.,
2020).
Principal component analysis (PCA), geostatistics, absolute principal
component score-multiple linear regression (APCS-MLR) analysis, the
positive matrix factorization (PMF) model, and the isotope method are
commonly used in source analysis (Wang et al., 2021a; Yang et al.,
2021a; Parra et al., 2014; Lv, 2019; Deng et al., 2020), including the
source apportionment of heavy metals or organic matter in sediments
(Pekey and Doğan, 2013), agricultural soils (Guan et al., 2018), and
urban topsoils (Chen and Lu, 2018; Qiao et al., 2021; Paatero and
Tapper, 1994). In recent years, APCS-MLR has been carried out often
with the PMF model to obtain sources of contamination (Lv, 2019; Wu
et al., 2020; Zhang et al., 2020; Li et al., 2021). One of the advantages of
the PMF and APCS/MLR methods is that they do not rely on the chemical
composition spectrum analysis of the source, which is highly convenient
and efficient (Lv, 2019). But most of the results obtained by the PMF or
APCS/MLR methods pertain to the source type, and few pertain to the
source location (Guan et al., 2018; Chen and Lu, 2018; Qiao et al., 2021;
Zhang et al., 2020; Li et al., 2021). For the risk control of a region, the
type and location of the source are very important, especially when
multiple sources belong to the same type (Yang et al., 2021a). Therefore,
how to achieve a more operational and intuitive source apportionment
should be emphasized.
Considering these, a modified model (the MLR model of distance
from sampling sites to sources [PCA-MLRD]) was proposed (Huang
et al., 2018). PCA was a widely used method to determine source type.
The regression equation obtained by the combination of PCA and MLRD
directly reflects the explanatory power of a certain source (Huang et al.,
2018). This differed from the PMF approach where the degree of match
between qualitative sources and factors was still need to be assessed
quantitatively. To obtain a better fitting model, Wang et al. (2020a)
conducted data conversion using the work of Huang et al. (2018) as a
reference and obtained a regression model with a higher degree of fit
than APCS-MLR and PMF. It can be found that the PCA-MLRD method
provides a new attempt to locate the source, but this method currently
has few applications. And it was unclear which type of regression model
should be used. These existing studies mainly rely on the comparison of
different models to verify results, while other verification and quanti­
fication methods are rarely used.
Thus, a quantitative approach, that is, the use of Geodetector, can be
combined with source identification models, such as PCA (Fei et al.,
2020; Tao et al., 2020; Wu et al., 2021). The factor detection in Geo­
detector can quantify the interpretation of factors from the perspective
of spatial heterogeneity (Wang et al., 2016; Wang and Xu, 2017). With
the help of the geo-detection results, the factors identified by the re­
ceptor model can be further clarified. The PCA-MLRD model can
quantify the contribution of potential pollution sources in the regression
equation. However, the combination of Geodetector and PCA-MLRD
models has been rarely studied.
In this study, a multi-functional industrial park in Central Anhui
Province, China, was selected as an example to locate the sources of
pollutants by combining Geodetector and PCA-MLRD. In this method,
the relationship between the specific pollution source and the pollutant
concentration was expressed in an equation. Geodetector was intro­
duced in the screening of the potential sources of pollution to quantify
the possibilities, reducing the subjectivity of relying on PCA alone.
2
Journal of Hazardous Materials 438 (2022) 129468
Therefore, this research has the following objectives: 1) to establish a
source analysis process from the screening of potential source ranges to
the identification of specific source factors, 2) to identify potential
sources using quantitative methods, and 3) to directly identify the
location of pollution sources via the use of regression equations.
2. Method and material
2.1. Overview of the research area
The study area was located in a prefecture-level city in the middle of
Anhui Province on the lower reaches of Yangtze River (Fig. 1). This
location has a subtropical humid monsoon climate, with a multiyear
average temperature and precipitation of 16.4 ◦ C and of 1400 mm,
respectively (Li et al., 2012; Wang et al., 2019). The area was rich in
mineral resources and has a long mining history of pyrite, copper, and
other minerals. This industrial park was established in the beginning of
the 21st century. After years of construction and development, a leading
industry focusing on copper processing and utilization and the me­
chanical manufacturing of electronic components was formed. In the
west, the park was bounded by rivers, which flow from south to
northwest. A mining area was situated on the upper reaches of this river.
The river water was used for irrigation of agricultural land in the area in
the early years. Subsequently, the farmland was transformed into con­
struction land and became part of the park. The industrial park has
various functional zoning. In addition to industrial land, the area has
residential and school lands.
2.2. Sampling and analysis
Soil and dust are interconnected and may be sources of heavy metals
to each other (Chang et al., 2009; Gabarrón et al., 2017a; 2017b; Han
et al., 2021). Comparing the two with each other can be used to syn­
thesize the source results. In this study, 68 sampling points were set up.
Soil and dust were simultaneously collected from most of the points,
while only soil or dust was collected in the other points, that was, soil
from 51 points and dust from 48 points. The sampling points basically
covered the study area. In some areas, because the land has not been
developed, the number of sample points is relatively small. For sensitive
receptors and enterprises with pollution potential, more sampling points
were set. The expected setting of dust and soil has a one-to-one corre­
spondence. In the actual sampling process, the ground was covered by
cements for a few points, and the soil near the dust points was selected.
Soil samples were collected from 0 to 30 cm layers with a stainless-steel
shovel. Dust samples were collected from roads or other ground covered
by cements with clean plastic brooms and dustpans (Gabarrón et al.,
2017a, b).
Approximately 0.100 g of each homogenized sample was weighed
and then digested in a mixture of HF-HNO3-HClO4 on a hot plate. The
concentrations of heavy metal(loid)s (Cr, Ni, Cu, Zn, As, Cd, Pb, Sb, and
Mn) in digested solution were detected using inductively coupled
plasma-mass spectrometry (ICP-MS, Thermo Scientific, Waltham, MA,
USA). The Hg content was determined using a DMA-80 mercury meter
(Wu et al., 2021; Zhang et al., 2021b). All of the vessels were soaked in
30 % HNO3 for 24 h before digestion and rinsed cleanly with ultra-pure
water.
The field survey and chemical analysis of soil and dust samples
strictly followed the field and indoor work specifications (GB/T
36197–2018) (SAC, 2018). The reference materials (GSS-1 and GSS-5)
from the Center of National Standard Reference Material of China,
blank samples, and three duplicates were used to ensure the reliability of
the analysis. The analysis errors of each element were less than ± 10 %.
The recovery percentages were within ± 10 %. And the correlation co­
efficient of the standard curve is greater than 0.999. Milli-Q deionized
water (18 MΩ⋅cm− 1) from Merck Millipore, USA, was used for complete
analytical and cleaning purposes.
W. Zeng et al.
2.3. Potential ecological risk evaluation
A new potential ecological risk assessment method called the NIRI
was developed by Men et al. (2020) based on the nemerow integrated
pollution index (NIPI) and potential ecological risk index (RI) (Hakan­
son, 1980; Huang et al., 2021; Roy et al., 2019; Luo et al., 2022).
The advantage of this method over NIPI and RI was that it takes into
account the effects of both the toxicity factor and the number of ele­
ments. In this study, NIRI was used to assess the ecological risk of ten
elements. The calculation equations are as follows:
ci
Eir = T ir × , (1)
cib
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
)2 ( )2 /
NIRI =
(
[ Eir max + Eir average ] 2 ,
where NIRI: Comprehensive ecological risk index of various heavy metal
(loid)s in soil or dust.
Eir : Potential ecological risk coefficient of the heavy metal(loid)s
element i in soil or dust.
T ir : Toxicity coefficient of heavy metal(loid)s element i.
ci : Heavy metal(loid) element i content.
cib : Calculated required reference values (select local soil background
values for comparison) of heavy metal(loid)s element i.
NIRI: Comprehensive ecological risk index of various heavy metal
(loid)s in soil or dust.
The toxicity coefficients of Cr, Ni, Cu, Zn, Hg, As, Pb, Cd, Mn, and Sb
are 2, 5, 5, 1, 40, 10, 5, 30, 1, and 10, respectively (Hakanson, 1980;
Zhang et al., 2019; Huang et al., 2021). For the local background soil, we
referred to the study of Li et al. (2012) and Wang et al. (2019). The
background values of Cr, Ni, Cu, Zn, Hg, As, Pb, Cd, Mn, and Sb are 80.0,
34.0, 34.0, 79.0, 0.06, 13.8, 29.0 0.23, 598, and 1.00 mg/kg, respec­
tively. According to Men et al. (2020), the evaluation criteria for the risk
level were shown in Table S1.
Fig. 1. Study area and location of sampling points.
Journal of Hazardous Materials 438 (2022) 129468
2.4. PCA-Geodetector-MLRD
2.4.1. Principal component analysis (PCA)
The element content was analyzed using the PCA method, and the
principal component factor scores and factor loadings of soil and dust
were obtained. The maximal rotation of variance method was used in
this work. The concentration of the element was used as the initial value
for PCA, and factor extraction with eigenvalues > 1 after varimax
rotation was used for source identification. Factor loading was adopted
to determine the type and range of potential sources. The factor score
was used to determine the principal component factor with the factor
detection in Geodetector. In this study, the spatial distribution of factor
scores was obtained in conjunction with geographic information science
(GIS). The scores were divided into five levels (Zones 1–5) on the map.
(2) Zones 4 and 5 are the high-scoring zones, and the main source targets
were screened within these two zones.
2.4.2. Geodetector modeling
A common submodule, namely, the factor detector, was used in this
study (Wang et al., 2010, 2016). The factor detector uses the q value to
measure the degree of influence of a certain factor (X) on dependent
variable Y. Here, factors X1, …, Xn represented the distance from the
sampling point to the potential source (e.g., river).
∑L 2
h=1 Nh σ h
qx = 1 − , (3)
N σ2
where qx is an index value used to measure the spatial association
between X and Y; h = 1, 2, 3,., L, where L is the number of strata
(subregions or subclasses) of factor X; and N and Nh are the number of
samples in the study area and in each stratum h, respectively. Symbols σ2
and σ2h represent the variances of Y in the entire region and in each
stratum (h), respectively. The value of qx∈[0,1] indicates how much Y is
influenced by X. The larger the value of qx is, the stronger the spatial
association between X and Y is (Tao et al., 2020).
In the factor detection of this research, Y is the score of each factor
obtained by the PCA of soil and dust, and X is the distance of the po­
tential sources determined initially. The type and location of potential
sources were determined (Section 2.4.1) based on the spatial distribu­
tion of factor scores. Geodetector was obtained from the website htt
3
W. Zeng et al.
p://geodetector.cn/.
2.4.3. Multiple linear regression of distance (MLRD)
Using PCA to identify potential sources, the source contribution can
be calculated based on the heavy metal(loid) content and the MLR of the
distance from the source. The content of heavy metal(loid)s theoretically
decreases with increasing distance from the source. Considering this, the
distance from the sampling point to the emission source can be used to
quantify their contribution. Here we propose three possible regression
models. These three models are common functional forms. At the same
time, it refers to the data transformation attempts proposed in the
existing source resolution research (Huang et al., 2018; Yang et al.,
2020). As the independent variable increases, the dependent variable
gradually decreases. Since the specific relationship between the source
and heavy metals was not very clear. The final source apportionment
model will be determined based on the validation results. The following
three regression models were used in this study:
∑p
1
Cik = Bin , (4)
n=1 Dnk
∑p
Model2 : Cik = Bin exp( − Dnk ), (5)
n=1
∑p
Model3 : Cik = n=1
Bin 0.5Dnk , (6)
where Cik is the content of element i in sampling site k, Dnk is the distance
from sampling site k to source n, Bin is the regression coefficient matrix
of distance Dnk , and n is the number of sources, p is the number of
pollution sources by the regression.
MLR uses a stepwise regression method to avoid collinearity, 80 % of
the data was used as the training set for the construction of three models,
and 20 % of the data was used as the validation set. The R2 and the RMSE
were used as the metrics to evaluate the models. The evaluation results
served as the basis for selecting the best models for soil and dust. Ac­
cording to Huang et al. (2018) and Wang et al. (2020a), R2 > 0.5 and
p ≤ 0.01 were used to filter all element models. Then, the source results
were compared with the results of the PMF model. A detailed flow chart
can be seen in Fig. 2.
Fig. 2. Flowchart of PCA-Geodetector-MLRD model.
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Journal of Hazardous Materials 438 (2022) 129468
2.5. Data analysis
Source apportionment and the corresponding uncertainty analysis
were also performed using the PMF model (Version 5.0) (USEPA, 2014).
The calculation method of the PMF model can be seen in the supple­
mentary material. The data processing in this study was completed on
Excel 2016 and SPSS 24. Graphs were created in Origin 2021 and ArcGIS
10.6. The shortest distance between the sampling point and the source
used for analysis in Geodetector and MLRD was calculated by the
analysis tools of ArcGIS 10.6 (Huang et al., 2018).
3. Results and discussion
3.1. Descriptive statistics of heavy metal(loid)s in soil and dust
Table 1 presented the descriptive statistical results of the heavy
metal(loid) content of soil and dust. The contents of 10 heavy metal
(loid)s varied greatly. The maximum concentration can be 100 times the
minimum value, whereas the average heavy metal(loid)s content was
higher than the local background value. The As content exceeded the
screening value (MEE, 2018).
The variation coefficients of the soil’s Cd, Zn, Cu, Mn, As, and Pb
were 1.84, 1.69, 1.55, 1.46, 1.27, and 1.04, respectively, indicating that
these elements fluctuated within a wide range and exhibited a strong
spatial heterogeneity. The fluctuation range of most of the dust metal
(loid)s in this region, such as Ni, As, and Pb, was near that in soil. The
metal(loid) elements in the dust with a strong spatial heterogeneity were
Hg, Cu, As, and Cr.
The results of other studies near the same area (industrial park) were
compared with those of the current study. The maximum Cu, Zn, and Cd
contents in this study were higher than those (340.43, 859.25, and
10.20 mg/kg, respectively) obtained by Wang et al. (2019). The Hg
content in this study (0.01–0.13 mg/kg) was similar to that obtained by
Wang et al. (2019) (0.03–0.17 mg/kg). The differences may be related to
the dispersed sampling sites of Wang et al. (2019). In their study, 29 soil
sampling sites covered most of the entire city, with approximately six
sampling sites near the mining area. By contrast, all the soil samples in
this study were obtained adjacent to the industrial park. Shen et al.
W. Zeng et al. Journal of Hazardous Materials 438 (2022) 129468

Table 1
Descriptive statistics of heavy metal(loid)s in soil and dust.
Cr Ni Cu Zn Hg As Pb Cd Mn Sb

Soil Minimum (mg/kg) 47.86 13.24 43.70 70.93 0.01 12.21 20.95 0.09 105.40 0.01
Maximum(mg/kg) 200.32 61.28 1371.53 2785.99 0.13 228.11 363.59 23.20 12,520.00 11.88
Mean(mg/kg) 88.92 31.28 249.70 431.86 0.04 45.49 97.35 3.09 1707.14 3.08
SDa 27.27 12.63 385.89 730.81 0.03 57.81 100.97 5.70 2487.80 2.66
CVb 0.31 0.40 1.55 1.69 0.76 1.27 1.04 1.84 1.46 0.86
Skewness 1.90 0.46 2.03 2.27 1.30 2.06 1.49 2.07 2.79 1.18
Kurtosis 4.96 -0.31 2.55 3.81 0.55 2.86 1.04 3.24 8.14 1.38
Dust Minimum (mg/kg) 35.62 13.24 51.70 83.12 0.02 4.35 23.90 0.09 585.74 0.72
Maximum (mg/kg) 955.92 72.09 1822.38 895.62 3.41 279.39 279.79 3.82 2348.77 21.00
Mean (mg/kg) 138.60 33.41 228.50 350.63 0.27 63.18 72.93 1.21 1258.74 5.70
SD 133.35 14.16 263.66 200.06 0.60 63.41 40.40 0.93 411.21 4.43
CV 0.96 0.42 1.15 0.57 2.23 1.00 0.55 0.77 0.33 0.78
Skewness 5.14 0.61 4.97 0.79 4.57 2.12 2.95 0.83 0.82 2.13
Kurtosis 31.03 -0.33 29.31 0.18 21.16 4.43 14.00 -0.02 0.32 5.00
Risk screening value (mg/kg) 200.00 900.00 18,000.00 – 38.00 60.00 800.00 65.00 180
Soil background value(mg/kg) 80.00 34.00 34.00 79.00 0.06 13.80 29.00 0.23 598.00 1.00

Risk screening value refer to MEE (2018); soil background value refer Li et al. (2012) and Zhang, . et al. (2019)
a
SD means standard deviation
b
CV means coefficient of variation

(2019) studied the heavy metal(loid)s in the farmland around a mining
area and found that the average concentration of Cd in more than 82 %
of the soil samples exceeded the screening value (0.3 mg⋅kg− 1) in Chi­
nese Environmental Quality Standard for Soils (SAC, 2018). And the
concentrations of all heavy metal(loid)s in the topsoils were higher than
those of the subsoils.
the soil sampling site) were higher than those in soil. They found that the
difference was mainly caused by the transportation and sedimentation
of dust. The differences in ecological risks between soil and dust indi­
cated the requirement for accurate source identification.
3.3. Identification of the potential sources of pollution

3.2. Characteristic of ecological risks 3.3.1. Identification of principal components by PCA

For Cu and Cd, some samples showed a high or very -high risk
ecological index (Fig. 3(a), Table S1), while for other elements, the
potential ecological risk index (Eir ) was generally low (Fig. 3a). Cd was a
high-risk pollutant in several regions of China (Wu et al., 2022).
Smelting activities and inappropriate agricultural measures were the
major sources of Cd pollution (Zhang et al., 2012a; 2012b; Han et al.,
2021; Wu et al., 2022). The reference value of Cd in the study area was
0.23 mg/kg (Li et al., 2012), while the Cd content in the soil was up to
23.20 mg/kg. This directly leaded to the higher ecological risk of Cd.
And the high content of Cd was speculated to be highly related to local
copper mining and smelting activities (Wang et al., 2004). The risk
levels of most heavy metal(loid)s in the dust samples were higher than in
the soil (Fig. 3b). This trend was obvious for Hg, showing a significantly
higher risk in the dust samples than in the soil samples. The numbers of
sampling points with As in the low- and medium-risk range were rela­
tively large. The comprehensive potential ecological risk index (NIRI)
showed the overall characteristics of the soil and dust elements content
(Fig. 3c). The NIRI of 1/3 of the points of the soil was above the medium
risk (Table S1). A few points have a high NIRI, reaching 2155.21. The
proportion of the dust points above the medium risk was high, reaching
1/2, but the highest NIRI was lower than that of soil, which was
1618.80. Few points have a high dust NIRI.
Several heavy metal(loid)s exhibited high-risk levels in the dust
(represented by Hg) and soil (represented by Cd). The apparent differ­
ence between the risks exhibited by soil and dust indicated that the
sources of heavy metal(loid)s in dust and soil might be different.
Gabarrón et al. (2017b; 2017a) conducted several detailed studies on the
heavy metals in soil and road dust. They found that heavy metals in road
dust have a higher health risk than those in soil. The sources of heavy
metals included the leather industry, smelters, and fertilizer industries.
Chang et al. (2009) found that soil and road dust have different sources
of heavy metal(loid)s, and the content of heavy metal(loid)s in the dust
was higher than that in soil. Another study (Long et al., 2021) from a city
in Southwestern China showed that the heavy metal(loid)s in dust (the
dust from road guardrails, air conditioners, and residents’ balconies near
Based on the 10 heavy metal(loid)s, two principal component factors
were screened for soil, and three principal component factors were
screened for dust (Table 2). In the soil, Factor 1 explained the majority of
the nine heavy metal(loid)s, namely, Cr, Cu, Zn, Hg, As, Pb, Cd, Mn, and
Sb, with coefficients of 0.82, 0.96, 0.97, 0.87, 0.97, 0.92, 0.96, 0.94, and
0.79, respectively. However, among them, the coefficients of Cr, Hg, and
Sb were slightly lower than those of other elements. Taking Cr as an
example, its factor 2 coefficient was 0.43. This shows that factor 2 also
has a certain explanatory effect on Cr. The results for Hg and Sb were
similar to those for Cr. This result indicated that the heavy metal(loid)
elements in the soil were mainly from one source (Factor 1), but some of
them also were influenced by Factor 2.
Section 3.1 showed that the background values of soil heavy metal
(loid)s in the study area were not high. And the main local industry was
copper mining and processing. This industry may contribute to the
diffusion and pollution of heavy metal(loid)s from atmospheric depo­
sition, transport vehicles, and rivers (Xu et al., 2013; Shen et al., 2019).
Therefore, Factor 1 was presumed to be an anthropogenic source,
associated with smelting activities. And the exact type of it needed to be
determined in the next step. As seen in Table 2, Factor 2 explained the
source of Ni (0.94). Several studies concluded that the Ni in soil mainly
originated from the soil parent material (Guan et al., 2019; Wang et al.,
2020b; Liu et al., 2021). Here, factor 2 may represent natural sources.
Combined with GIS technology, the spatial distribution map of soil
element principal component factors 1 and 2 was obtained (Fig. 4(a) and
(b)). Based on the factor scores, the interpolation area could be divided
into five zones. In Fig. 4(a), the sources related to factor 1 were most
likely to be distributed in Zones 4 and 5 (high scores). A comparison of
the site survey results showed that the area was near the river, and no
other obvious source of pollution was identified. Sun (2013) and Kuang
et al. (2018) have found that the heavy metal(loid)s in the river water
were obviously high and the highest concentrations of Cu, Zn, Cd, and As
can reach 5204.30, 2368.90, 222.50, and 310.20 μg/L. Hence, the river
was first included as potential sources of soil pollution.
The study area was an industrial park, mainly for copper processing,
and the mines outside the park were mainly for copper production

5
W. Zeng et al. Journal of Hazardous Materials 438 (2022) 129468

Table 2
Rotating component matrix obtained by PCA.
Component of soil Component of dust

Factor 1 Factor 2 Factor 1 Factor 2 Factor 3

Cr 0.828 0.43 0.188 0.79 -0.015

Ni -0.152 0.938 -0.183 0.741 0.125
Cu 0.96 -0.197 0.285 0.006 0.895
Zn 0.969 -0.073 0.848 0.116 0.363
Hg 0.873 -0.288 -0.213 0.016 0.911
As 0.969 -0.164 0.617 0.646 -0.016
Pb 0.918 -0.253 0.836 0.008 -0.046
Cd 0.956 -0.162 0.828 0.075 -0.043
Mn 0.935 0.16 0.682 0.393 -0.046
Sb 0.783 -0.318 0.44 0.686 -0.104

Elements As and Sb were explained by Factors 1 and 2. The sources of As

and Sb were also closely related to human activities (Lv, 2019).
Fig. 4(c), (d), and (e) were the interpolation results of the principal
component factors of the dust elements. The zones with a high Factor 1
score were scattered and distributed in the south, southwest, and north
of the study region. Within these high-scoring areas, two targets were
identified: mining (southwest) and community (south). However, no
more obvious targets were found in the high-scoring area in the north.
The interpolation results of Factor 2 show that the high-scoring areas
(Zones 4 and 5) were located near the main roads. Fig. 4(e) showed an
obvious target, that was, the metal plant, in the high score area (Zone 4).
Therefore, combining the soil and dust results, the PCA approach
helped obtain the potential source range, including five targets, namely,
river, mining area, community, main road, and metal plant.
The possibility of the above sources was determined through existing
research and professional knowledge, which might be subjective. Ac­
curate judgement was difficult when multiple factors have strong in­
terpretations. Therefore, a quantitative method (Geodetector) was
further introduced to reveal the explanatory power of specific sources.
On the basis of the above discussion, five specific targets were summa­
rized as the next source identification, namely, metal plant, river, main
road, mining area, and community. The shortest distances from the five
targets to the sampling points were set to X, and the PCA factor scores
were set to Y.

3.3.2. Spatial detection of pollution sources by Geodetector

Fig. 3. Ecological risks of heavy metals in soil and dust.
(Wang et al., 2019; Wu et al., 2021). The explanatory factors corre­
sponding to the 10 heavy metal(loid)s in dust were more scattered than
those in soil. Cr and Ni were mainly explained by factor 2 (the co­
efficients were 0.79 and 0.74, respectively). Cu (0.89) and Hg (0.91)
were mainly explained by Factor 3. The source of Cu may be highly
related to local copper mining and processing.
Factor 1 of the dust elements explains most of the sources of Zn, Pb,
Cd, and Mn (Table 2). Pb was considered to be an important indicator of
the transportation source because the lead in gasoline was one of the
main sources of the lead in soil (Cui et al., 2018; Zhang et al., 2021a).
The factor detection in Geodetector matched the above potential
source range and principal component factors from the perspective of
spatial heterogeneity, verifying the accuracy of the principal component
analysis results. Fig. 5 presented the result of factor detection. In the
matching results of soil Factor 1, river, metal plant, and community have
a significant (p < 0.05) explanatory power. That was, the spatial dis­
tribution of the three was similar to soil Factor 1. According to the
distribution map of the principal component factors (Fig. 4), when the
point was near the river, the factor score showed an increasing trend, but
when the point was near the metal plant and the community, the factor
score was low. This meant that the river matched the actual meaning of
the source of Factor 1. Soil Factor 2 was previously judged to be a nat­
ural source, and the factor detection results showed that only the mining
area and soil Factor 2 had a certain matching relationship among the
five targets.
The spatial distribution of dust Factor 1 was scattered, and the target
of the main road has a certain explanatory effect on dust Factor 1 (q =
0.23, p < 0.05). This finding was consistent with the principal compo­
nent results in Section 3.3.1. The detection results of dust Factor 2
showed that many targets have a similar spatial distribution with dust
Factor 2. In addition to the main road, metal plant, community, and
river have a significant explanatory power (p < 0.05). The geographical
location of the first three overlapped with the high score of dust Factor 2,
but the river was located in the low score of dust Factor 2. The reason
why rivers have a certain explanatory role was similar to soil Factor 2

6
W. Zeng et al.
Fig. 4. Spatial distribution of principal component factors of soil (a and b) and dust elements (c, d, and e).
above. The detection results of dust Factor 3 did not show an obvious
target, and the only target with a significant explanatory power
(p < 0.05), the river, was supposed to explain the region with a low dust
Factor 3, which does not belong to the source range. The detection re­
sults of dust Factor 3 must be further revealed. In general, the factor
detection in Geodetector basically verified the judgment results of the
principal component analysis in Section 3.3.1. That was, the potential
source range composed of five targets (metal plant, river, main road,
mining area, and community) has significant explanatory power. This
7
Journal of Hazardous Materials 438 (2022) 129468
result will also provide a basis for the next step of model building.
3.4. Sources apportionment by the establishment of the regression model
based on distance
3.4.1. Comparison and screening of model performance
Three regression methods were used for the source apportionment of
soil and dust elements. The regression coefficient (R2) of the 10 elements
in the soil and dust training sets was shown in Fig. 6. The fitting result of
W. Zeng et al. Journal of Hazardous Materials 438 (2022) 129468

Fig. 5. Detection results (q value) of principal component factors types using Geodetector. The shortest distances from the five targets (metal plant, river, main road,
mining area, and community) to the sampling points are set to X, and the PCA factor scores are set to Y.

the three regression methods was different among different elements. respectively, and the fitting coefficient of Model 3 was slightly higher
For example, the fitting effect of Model 2 of Zn (R2 =0.622) was higher than those of the other two models. Overall, most elements have an R2
than that of Models 1 and 2 (R2 =0.614, 0.581). However, the R2 of the greater than 0.5. Similarly, the training set regression coefficient R2 of
three Hg models (Models 1, 2, and 3) were 0.751, 0.763, and 0.778, Pb, Zn, and Cu in dust exceeds 0.6. The R2 of Mn was higher than those

Fig. 6. Comparison of three models for training set of soil (a) and dust (b) elements.

8
W. Zeng et al. Journal of Hazardous Materials 438 (2022) 129468

of the other elements. In terms of soil and dust, although the three can explain the source of most elements (Huang et al., 2018; Wang et al.,
regression methods were different, one model shows no absolute 2020a), and the highest was 0.791 (Pb).
advantage over the other two. The model to be selected for subsequent Regression equations were also developed for the 10 heavy metal
source apportionment should also be evaluated by the validation results. (loid)s in the dust. Droad, Dmine, Dmetal, and Dcommunity represent the
Table 3 shows the validation results of soil and dust. R2 and RMSE distance from the sampling site to the main road, the mine, the metal
were used to measure the regression effects of the three methods. For plant, and the community, respectively. An obvious feature was that the
soil, the R2 values of Cu, Zn, Hg, As, Pb, Cd, Mn, and Sb obtained by sources of most elements in dust were different from those in soil, and
Model 1 were higher than those obtained by Models 2 and 3. The RMSE the source amount was higher. The main road, community, and mine
values of these elements were lower than those of the other two models. were the primary sources of heavy metal(loid)s in dust, with the main
For example, the R2 of As Model 1 was 0.80, which was higher than road acting as the main source of eight heavy metal(loid)s, including Cu,
those of Models 2 (0.71) and 3 (0.57). The results show that the fitting Zn, As, Pb, Cd, Sb, and As. Community plays an important role in
method of model 1 has more advantages than those of Models 2 and 3. explaining the source of Cr, As, and Mn in the dust (Table S5).
The fitting effect of the Cr and Ni validation set differed greatly from that The results of the heavy metal(loid)s source analysis for soil and dust
of the training set, indicating that the two elements may be over-fitting reveal that dust was a different and more diverse source of heavy metal
to a certain extent. In Table 3, the R2 of soil Cr and Ni was lower than (loid)s than soil. The community represents the living behavior of the
that of other elements. The most important reason may be that their inhabitants of the study area, suggesting that heavy metal(loid)s affect
sources were from natural sources. The results of the PCA (Table 2) human health in such a multifunctional park and human living behavior
indicated that the natural source (soil factor 2) explained most of the Ni may contribute to the heavy metal(loid)s in soil and dust.
and part of the Cr sources. This was consistent with the results of several In addition, the metal plant was not identified as a major source of
existing studies that elements grouped with Cr and Ni were often soil heavy metals in the regression model. This differed from previous
considered to be associated with natural sources (Cai et al., 2019; Wang studies in which metal plants caused serious contamination in the sur­
et al., 2020b; Liu et al., 2021). rounding area (Roels et al., 1978; Izydorczyk et al., 2021). A major
For dust, the R2 of Ni, Cu, Zn, Mn, and Sb of Model 3 was higher than reason is that this plant is mainly engaged in metal-processing instead of
those of Models 1 and 2. The R2 of Model 1 was high in Hg and Cd, and metal-smelting. The mining and smelting of copper ore in the study area
the R2 of Model 2 was high in Cr, As, and Pb. Accordingly, the regression was carried out in the mine area while the metal plant in the park mainly
equation (RMSE) value of the dust element also presented a similar performs post-processing. Compared to mining and smelting,
trend. Therefore, based on the validation results, the soil Model 1 metal-processing plant usually presented a lower, heavy metal pollution
method was selected, while the dust Model 3 method was selected for and risk (Hutter et al., 2016b; Klasson et al., 2016).
subsequent source analysis. Also, in this study, the shortest distances were chosen in both the
Geodetector and MLRD. Considering that the line source of the road
3.4.2. Sources of elements identified by the regression models affects the heavy metal content through atmospheric deposition, this
The capability to quantitatively identify pollution sources was one of process was affected by the wind direction (Lv, 2019; Zhang et al.,
the most important features of distance-based regression models 2019). And when calculating the distance between the road and the
compared with the PMF model. Fig. 7 showed the regression model for receiving point, the distance was not calculated according to the wind
heavy metal(loid)s in soil and dust (Table S4-5). direction. This may add uncertainty to the results.
Fig. 7 showed the sources of soil and dust elements obtained by PCA-
Geodetector-MLRD. The river and mining areas were the main factors 3.5. Comparison of the established PCA-Geodetector-MLRD with the
that explain the source of heavy metal(loid)s in soil. The river was the commonly used PMF in terms of source identification
most likely sources of pollution by Cu, Zn, Hg, As, Pb, Cd, and Mn. The
mining area was the most important source of Sb and explains part of the 3.5.1. PMF model results
sources of Cr, Ni, and Mn. R2 was used to measure the degree of Fig. 8 showed the results of the PMF model. Fig. 8(a) showed the
explanation of the variables using the regression equation. The R2 values analytical results of soil. The explanatory power of Factor 1 on Cr, Ni,
of Cu, Zn, Hg, As, Pb, Mn, and Sb exceed 0.5, implying that the model Hg, and Mn was evidently stronger than that on the other elements. The
Cr and Ni in soil mainly originated from parent materials (Jiang et al.,
Table 3 2017; Liu et al., 2021). Factor 1 was regarded as the parent material of
Validation results of soil and dust elements regression models. soil formation. Factor 2 has a certain explanatory effect on all metals,
except Sb (Zhuo et al., 2019). Zhang et al. (2019) believed that Sb was
R2 RMSE
more likely to come from industrial activities. Here, Factor 2 was also
model 1 model 2 model 3 model 1 model 2 model 3 speculated to be an industrial source. Moreover, the specific source
Soil Cr 0.02 0.14 0.16 17.177 20.894 18.234 categories should be further studied. Factor 3 has a similar contribution
Ni 0.06 0.05 0.07 15.271 15.717 14.231 to Cr, Ni, Cu, and As, that was, approximately 40 %. The Cr and Ni in soil
Cu 0.78 0.63 0.50 194.409 226.523 241.881
were considered to be mainly from natural sources (Jiang et al., 2017;
Zn 0.78 0.65 0.46 143.902 285.916 208.427
Hg 0.69 0.18 0.17 0.014 0.023 0.022 Liu et al., 2021). Meanwhile, Cu and As were considered to be from
As 0.80 0.71 0.57 13.041 22.318 20.609 anthropogenic sources (Fei et al., 2020). The type of Factor 3 was un­
Pb 0.75 0.63 0.55 41.817 49.557 55.277 clear. Factor 4 strongly explained Cu, Zn, As, Pb, Cd, and Mn (62.1 %,
Cd 0.76 0.53 0.44 2.670 2.956 3.180 53.9 %, 37.4 %, 54.3 %, 72.2 %, and 35.4 %, respectively). Agricultural
Mn 0.71 0.19 0.48 538.040 752.680 640.201
Sb 0.25 0.01 0.21 1.755 2.195 2.642
activities, such as phosphate fertilizers, pesticides, organic fertilizers,
Dust Cr 0.04 0.40 0.17 64.838 42.472 58.724 and sewage irrigation, usually provided large amounts of Cd (Shao et al.,
Ni 0.33 0.61 0.68 11.740 10.393 9.155 2016; Fei et al., 2020). Multiple studies using the PMF model for heavy
Cu 0.57 0.69 0.70 126.601 138.350 124.671 metal(loid) source analysis showed that the factors with a strong
Zn 0.33 0.77 0.75 71.073 54.293 43.169
explanatory effect on Cd, Cu, and As elements were likely to originate
Hg 0.58 0.51 0.50 0.007 0.041 0.027
As 0.36 0.58 0.57 9.857 13.445 11.828 from agricultural activities (Fei et al., 2020; Liu et al., 2021). In this
Pb 0.50 0.77 0.74 6.087 15.027 9.081 study, the industrial park used to be an agricultural land in the early
Cd 0.46 0.22 0.21 0.147 0.315 0.235 stage. Therefore, Factor 4 may represent agricultural activities.
Mn 0.77 0.68 0.86 182.800 254.455 140.290 Fig. 8(b) shows the analytical results of heavy metal(loid)s sources in
Sb 0.59 0.53 0.74 0.751 1.135 0.747
the dust. Factor 1 explains some of the sources of Ni, Mn, and Sb.

9
W. Zeng et al. Journal of Hazardous Materials 438 (2022) 129468

Fig. 7. R2 is determined by the coefficient of determination from the regression equation for each element.
(a) Sources of soil and dust elements obtained by PCA-Geodetector-MLRD. (b) (a): the sources of soil elements; (b): the sources of dust elements.

Previous studies (Filella et al., 2009; Mandal et al., 2021) pointed to
natural factors, such as rock weathering, and anthropogenic factors,
such as mining and smelting activities, vehicle emissions, and agricul­
tural fertilizers, as potential sources of Sb. The contribution of Factor 1
to other elements was also low, so Factor 1 may represent a natural
source. The explanatory power of Factor 2 was obviously stronger than
that of Factor 1, which plays a major role in explaining the sources of Zn,
Hg, Pb, Cd, Mn, and Sb. The contribution ratio reached 25 %, 53 %, 50
%, 45 %, 35 %, and 54 %. Hg was considered to be closely related to
atmospheric deposition (Zhang et al., 2019). Pb was often regarded as an
important indicator of traffic source (Lv, 2019). Therefore, Factor 2 was
likely to represent the atmospheric deposition caused by human activ­
ities. Factor 3 contributed another part of the source of Ni and Hg. Ni
was also considered to have a partial relationship with natural sources.
According to the above analysis, Hg may come from human activities.
Therefore, the type of Factor 3 was unclear. Factor 4 mainly explains the
sources of Cu and Zn. Local copper mining and smelting activities may
result in high levels of Cu in the dust. Factor 4 may be related to mineral
smelting activities. Factor 5 explains the main sources of Cr, As, and Cd
as well as Cu and Zn. As and Cd were important indicators used to judge
anthropogenic sources (Yoon et al., 2022). Agricultural activities, such
as the application of pesticides and sewage irrigation, often provide

10
W. Zeng et al.
Fig. 8. Source analysis results of soil (a) and dust (b) heavy metal(loid)s by the PMF model.
large amounts of Cd (Lv, 2019). As was associated with mining activ­
ities, the use of phosphate fertilizers, the herbicides and pesticides in
agricultural areas (Yoon et al., 2022). In this study, anthropogenic
sources that can discharge these substances included early agricultural
activities (such as sewage irrigation) and wastewater and exhaust
emissions from mining and smelting activities. Thus, Factor 5 may
represent agricultural activity. For the uncertainty of the result, Qtrue
and Qrobust are two sets of Q data used in the PMF model (Wang et al.,
2021b). The number of factors was determined by the lowest Qrobust. The
error estimate contributed by the PMF model source was determined by
the DISP and BS methods (Figs. S1–4). The errors from the base run were
all within the interquartile range (25th–75th) of the BS and DISP runs,
indicating that the fitting errors of the PMF base run were all within the
acceptable range (Paatero et al., 2003; Yang et al., 2021b).
3.5.2. Comparison of source identification results by the PCA-Geodetector-
MLRD and PMF model
The heavy metal(loid) sources identified by the PCA-Geodetector-
MLRD and PMF models were compared (Fig. 9). According to the re­
sults of the PCA-Geodetector-MLRD model, the river was the most
important pollution source of heavy metal(loid)s in soil, showing a
strong explanatory power for the sources of Cu, Zn, Hg, As, Pb, and Cd.
11
Journal of Hazardous Materials 438 (2022) 129468
The field investigations in this area showed that the soil in the industrial
park of the study area was used as agricultural land in the early stage,
and this area was near a river flowing upstream through the mining area
(Wang et al., 2019). Sun (2013) combined isotope and scanning electron
microscopy to test the heavy metals content in the river and found that
more than 55 % of the points were seriously polluted. Another local
study (Jiang et al., 2018) showed that the Cd in the soil was mainly from
mining and irrigation with contaminated water. Xu et al. (2013) and
Shen et al. (2019) found that local mining activities were the main
reason for the high content of heavy metals in soil and river. Therefore, it
is suggested that one of the pollution sources for the soil heavy metal
(loid)s pollution is irrigation by river water carrying heavy metal(loid)s.
Multiple factors were identified by the PMF method. Unlike PCA-
Geodetector-MLRD, these factors need to be further defined and speci­
fied (Fig. 9). For instance, Factor 4 of soil heavy metal(loid) identified by
the PMF model, which has a strong interpretation for Cu, Zn, As, Pb, and
Cd, has a high probability of being an anthropogenic source. According
to Shao et al. (2016) and Fei et al. (2020), agricultural activities may
provide large amounts of Cd. And multiple studies suggested that the
factors contributing to Cd, Cu, and As were mainly related to agricul­
tural activities (Fei et al., 2020; Liu et al., 2021). Combined with the
field survey results of the park, this source could be an agricultural
W. Zeng et al.
Fig. 9. Comparison of source identification results between PCA-Geodetector-MLRD and PMF model.
activity (Liu et al., 2021).
The comparison above showed that there were differences in the
sources obtained by the two methods. The main reason was that Geo­
detector and MLRD can express the potential targets and locations cor­
responding to the source types identified by PCA. Therefore, the PCA-
Geodetector-MLRD method was considered to have certain advantages
in source location identification over the PMF model.
While, the PCA-Geodetector-MLRD method also has shortcomings,
such as the inability to quantitatively analyze some nonpoint sources,
including the influence of soil parent materials and atmospheric depo­
sition. The study attempted to convert nonpoint sources to point source
treatment. A mining area and a metal plant were identified as targets to
represent partial atmospheric subsidence. Furthermore, the living
behavior of residents in the industrial park may also be a nonpoint
source. The distance to the community was selected to represent this
factor. The PCA results can indicate the influence of natural sources
(such as soil parent material), but the importance of this factor did not
receive attention in the subsequent research steps. This shortcoming of
PCA-Geodetector-MLRD should be addressed in future work.
In general, for the risk management of a certain area, the source
might be difficult to manage when only the type of the source was
known (the location was uncertain). Because some areas may have
several sources that belong to the same category. For example, the
mining area and metal plant in this study were all industrial activities.
The sources obtained by the PMF model were difficult to use for further
source location. But the PCA-Geodetector-MLRD method can be used
with distance to quantify whether a possible source (with known loca­
tion) was the main source factor. This approach has strong operability
and an important value in source analysis and risk management for soil
pollution in a complicated environment.
12
Journal of Hazardous Materials 438 (2022) 129468
4. Conclusion
In this study, the PCA-Geodetector-MLRD method was used for
source identification. The PCA-MLRD approach uses a quantitative
rather than just a qualitative approach to identify sources, and the
combination with Geodetector further reduces the subjectivity in
screening potential sources. The source identified by this method was
more specific than the PMF method. The combination of Geodetector
and PCA-MLRD was applied to the multifunctional industrial park,
enabling the source identification and localization of heavy metal(loid)
sources. The PCA-Geodetector-MLRD method used in this study can
provide new information for source analysis methods, which will also
provide a foundation for the subsequent development of more complete
and accurate source identification methods.
Further, the risk levels of soil differ at various levels. Most heavy
metal(loid)s, such as Hg and As, show a higher concentration in dust
than in soil. However, Cd and Pb show a higher concentration in soil
than in dust. The main sources were also different. The heavy metal
(loid)s in soil mainly come from the river, whereas the metal(loid)s in
dust were associated with the road and the mine. The difference between
soil and dust indicates that the heavy metal(loid) sources were complex
inside and outside the park. The current study can provide useful in­
formation for environmental management.
Environmental implication
The existing source analysis methods rely on subjective judgments
when concretizing the main factors. This study proposed a modified
method for the combined use of Geodetector and PCA-MLRD. Factor
detection provides quantitative tools for determining principal compo­
nent factors and screening potential pollution sources. The main
W. Zeng et al.
pollution sources of specific elements were further identified by
regression equation. And the combination of soil and dust indicated that
soil heavy metals are closely associated with rivers, whereas dust is more
associated with roads.
CRediT authorship contribution statement
Weibin Zeng: Methodology, Investigation, Writing – original draft,
Visualization. Xiaoming Wan: Conceptualization, Writing - review &
editing, Lingqing Wang: Investigation, Resources. Gaoquan Gu:
Writing – review & editing, Visualization. Mei Lei: Resources, Super­
vision. Tongbin Chen: Resources, Supervision.
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.
Data Availability
Data will be made available on request.
Acknowledgment
This work was supported by the National Key Research and Devel­
opment Program of China (Grant No. 2018YFC1800302) and the Inno­
vation Academy for Green Manufacture of the Chinese Academy of
Sciences (Grant No. IAGM-2019-A16-5).
Appendix A. Supporting information
Supplementary data associated with this article can be found in the
online version at doi:10.1016/j.jhazmat.2022.129468.
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