Environ Sci Pollut Res (2017) 24:9387–9398
DOI 10.1007/s11356-017-8548-x
RESEARCH ARTICLE
Comparison of soil heavy metal pollution caused by e-waste
recycling activities and traditional industrial operations
Kailing He 1,2 & Zehang Sun 1,2 & Yuanan Hu 3 & Xiangying Zeng 1 & Zhiqiang Yu 1 &
Hefa Cheng 4
Received: 30 June 2016 / Accepted: 1 February 2017 / Published online: 23 February 2017
# Springer-Verlag Berlin Heidelberg 2017
Abstract The traditional industrial operations are well recog-
nized as an important source of heavy metal pollution, while
that caused by the e-waste recycling activities, which have
sprouted in some developing countries, is often overlooked.
This study was carried out to compare the status of soil heavy
metal pollution caused by the traditional industrial operations
and the e-waste recycling activities in the Pearl River Delta,
and assess whether greater attention should be paid to control
the pollution arising from e-waste recycling activities. Both
the total contents and the chemical fractionation of major
heavy metals (As, Cr, Cd, Ni, Pb, Cu, and Zn) in 50 surface
soil samples collected from the e-waste recycling areas and 20
soil samples from the traditional industrial zones were deter-
mined. The results show that the soils in the e-waste recycling
areas were mainly polluted by Cu, Zn, As, and Cd, while Cu,
Zn, As, Cd, and Pb were the major heavy metals in the soils
from the traditional industrial zones. Statistical analyses
Responsible editor: Philippe Garrigues
Electronic supplementary material The online version of this article
(doi:10.1007/s11356-017-8548-x) contains supplementary material,
which is available to authorized users.
* Hefa Cheng
hefac@umich.edu
1
State Key Laboratory of Organic Geochemistry, Guangzhou Institute
of Geochemistry, Chinese Academy of Sciences,
Guangzhou 510640, China
2
University of Chinese Academy of Sciences, Beijing 100049, China
3
MOE Laboratory of Groundwater Circulation and Evolution, School
of Water Resources and Environment, China University of
Geosciences (Beijing), Beijing 100083, China
4
MOE Laboratory for Earth Surface Processes, College of Urban and
Environmental Sciences, Peking University, Beijing 100871, China
consistently show that Cu, Cd, Pb, and Zn in the surface soils
from both types of sites were contributed mostly by human
activities, while As, Cr, and Ni in the soils were dominated by
natural background. No clear distinction was found on the
pollution characteristic of heavy metals in the surface soils
between the e-waste recycling areas and traditional industrial
zones. The potential ecological risk posed by heavy metals in
the surface soils from both types of sites, which was dominat-
ed by that from Cd, ranged from low to moderate. Given the
much shorter development history of e-waste recycling and its
largely unregulated nature, significant efforts should be made
to crack down on illegal e-waste recycling and strengthen
pollution control for related activities.
Keywords Soil pollution . Heavy metals . E-waste recycling .
Traditional industrial operations . Sequential extraction .
Potential ecological risk
Introduction
The quality of soils is closely related to agricultural produc-
tion, human health, and ecological security (Burges et al.
2015; Chen et al. 2014). Among all the pollutants in soils,
heavy metals are of significant concerns due to their inherent
toxicity, bioaccumulation, persistence, and non-degradability
(Liu et al. 2013). Heavy metals are considered as Bcontami-
nants^ when their occurrences are unwanted, or in forms or
concentrations resulting in detrimental effects to human or the
ecosystem. Although heavy metals rarely occur at toxic levels
naturally, intensive anthropogenic activities can drastically al-
ter the natural biogeochemical cycling and balances of some
heavy metals (Alloway 1995). The major anthropogenic
sources of heavy metals include industrial point sources, such
as mines, foundries, and smelters, as well as diffuse sources,
9388
e.g., vehicular emissions and urban and agricultural run-off
(Nriagu and Pacyna 1988). Irrespective of their sources in the
soil, accumulation of heavy metals can degrade soil quality, re-
duce the crop yield and the quality of agricultural products, and
thus negatively impacts the health of human, animals, and the
ecosystem (Nagajyoti et al. 2010).
The Pearl River Delta (PRD) in Guangdong Province,
which is a densely populated region of over 40,000 km2 with
a population over 40 million, is a major manufacturing base in
China. There used to be few industrial activities in the PRD
before the launch of economic reform in the late 1970s (Hu
et al. 2013). Cities, including Dongguan, Zhuhai, and
Zhongshan, have been transformed from agricultural lands
to major manufacturing hubs over the past three and a half
decades. Remarkable heavy metal pollution has resulted from
the manufacturing operations and the associated disposal of
industrial wastes (Hu et al. 2013). Along with the rapid indus-
trial and urban development, numerous cases of water, sedi-
ment, and soil pollution have occurred in the PRD
(Guangdong Environmental Protection Bureau 1996).
Previous studies have documented widespread pollution of
surface soils in the PRD (Hu and Cheng 2016; Hu et al.
2013; Qiu et al. 2015, 2016; Wang et al. 2015; Wong et al.
2002; Xiao et al. 2012). In particular, land use type has been
found as a major factor influencing the occurrence of soil
metal pollution (Hu and Cheng 2013, 2016). Surface soils
from industrial lands and related waste disposal/treatment sites
were typically more heavily polluted than those from the other
types of land uses, including forestry lands, drinking water
source protection areas, urban areas, and agricultural lands
(Hu and Cheng 2013, 2016).
In addition to the traditional industrial operations, an im-
portant and unique source of heavy metal pollution in the PRD
is e-waste recycling activities, which are largely illegal (Duan
et al. 2016). Driven by the profits from recycling the non-
ferrous metals in waste electronic products and reusable com-
ponents, e-waste recycling has started and developed quickly
in Guiyu and Qingyuan since the late 1980s, transforming
them into major e-waste recycling centers in China (Sun
et al. 2016; Wong et al. 2007a, b). Over 60,000 local residents
and 20,000 migrant workers are engaged in e-waste recycling
activities in Guiyu alone. It was estimated that over 150,000 t
of plastics and 200,000 t of metals had been processed in the
simple and primitive methods between 1995 and 2003 in
Guiyu alone (Guo et al. 2009). Similarly, a major portion of
e-waste is recycled in Qingyuan by the informal sector using
rudimentary techniques. The majority of the e-waste disman-
tled in these areas was shipped from the developed countries
(Ni and Zeng 2009; Pradhan and Kumar 2014; Robinson
2009), and the metal components were often handpicked after
heating and burning of the e-waste, while the waste residues
were typically dumped on the open ground (Sun et al. 2016).
As a result of such primitive and outdated recycling methods,
Environ Sci Pollut Res (2017) 24:9387–9398
large amounts of pollutants, including heavy metals, had been
released into the air, water, and soils in the surrounding areas
(Awasthi et al. 2016a; Huo et al. 2014), which caused envi-
ronmental pollution and posed a health risk to local residents
(Song and Li 2015; Wong et al. 2007a, b; Zeng et al. 2016).
Despite their rather different nature and production modes,
both traditional industrial operations and e-waste recycling
activities can cause pollution of surface soils by heavy metals
(Liu et al. 2011; Yekeen et al. 2016). Although pollution con-
trol and prevention regulations have been well established for
various types of traditional industrial operations, e-waste
recycling industry is rather unique and has not received
enough attention in the past. There is a pressing need for
assessing the soil pollution by heavy metals in the e-waste
recycling areas in comparison with that brought by traditional
industrial operations, while no previous study has attempted
such comparison. The present study was carried out to evalu-
ate and compare the soil heavy metal pollution in the e-waste
recycling areas and the traditional industrial zones of the PRD.
The results can help better understand the risk of soil heavy
metal pollution brought by e-waste recycling activities and
traditional industrial operations to the ecosystems and support
the development of environmental policy on e-waste
recycling.
Materials and methods
Sampling areas
A total of 70 surface soil samples were collected from three
traditional industrial zones (Dongguan, Zhuhai, and
Zhongshan) and two major e-waste recycling areas
(Qingyuan and Guiyu) in the central part of PRD. The loca-
tions where soil samples were collected in these five cities/
towns are depicted in Fig. 1. To avoid the direct impact of
point pollution sources, the soil samples were collected from
the surface layer (down to 10 cm below ground) in the forestry
and agricultural lands with no nearby pollution sources. All
the collected samples were stored in brown glass bottles and
brought back to the laboratory after removal of the pebbles,
weeds, and sticks.
Sample processing and chemical analysis
All soil samples were air-dried, ground into fine particles,
sieved through a 100 mesh nylon sieve, and oven dried at
105 °C prior to further processing. The total contents of heavy
metals in these soil samples were analyzed following Method
3052 of the U.S. Environmental Protection Agency (USEPA)
(USEPA 1996). In brief, approximately 0.2 g of soil samples
was digested in Teflon digestion vessels using trace metal grade
acids [9.0 mL concentrated nitric acid and 3.0 mL 40% (v/v)
Environ Sci Pollut Res (2017) 24:9387–9398
Fig. 1 Sampling sites of this study, where Qingyuan and Guiyu are major e-waste recycling areas in the PRD of south China, while Dongguan,
Zhongshan, and Zhuhai have well-developed traditional industrial operations
hydrofluoric acid] in a CEM Mars microwave system. The
digestion solutions obtained were then heated on an electric
heating plate to near dryness. The residues were re-dissolved
in dilute nitric acid and their contents of heavy metals (diluted
by 10 to 100 times when necessary) were determined on an
Agilent 7700X Inductively Coupled Plasma-Mass
Spectrometer. For the purpose of quality assurance and quality
control (QA/QC), four standard reference materials (SRM
1646A, GSS6, GSS7, and GSS16), blank sample, and dupli-
cates of 10% of the sample load were digested along with the
samples. The differences between the measured values and cer-
tified values for the reference materials were in the range of 79–
119% for the metals reported.
Chemical fractionation, which reveals the chemical forms in
which heavy metals occur in soils, can provide important in-
sights on their mobility, bioavailability, and eco-toxicity (Hu
and Cheng 2016; Rinklebe and Shaheen 2014; Shaheen and
Rinklebe 2014; Zhang et al. 2012b). Chemical fractionation
9389
of the heavy metals in all the soil samples (approximately
1.0 g) was determined using the modified BCR three-step se-
quential extraction procedure (Pueyo et al. 2001; Rauret et al.
1999). Specifically, heavy metals in the soil samples were ex-
tracted into the acid soluble (step 1—CH3COOH), reducible
(step 2—NH 2 OH·HCl), oxidizable (step 3—H 2 O 2 /
CH3COONH4), and residual fractions under appropriate condi-
tions (Hu and Cheng 2016). The contents of heavy metals in the
residual fraction were determined based on the difference be-
tween their total contents and those removed in the three sequen-
tial extraction steps in the soil samples. Various studies have
reported good agreement (85–107%) for the contents of heavy
metals in soil samples determined using the methods of sequen-
tial extraction and total acid digestion (Gao et al. 2010; Martin
et al. 1998; Yuan et al. 2004). In general, heavy metals in the acid
soluble fraction are readily mobile and bioavailable, those in the
reducible and oxidizable fractions are potentially mobile and
bioavailable, while heavy metals present in the residual fraction
9390
are considered as stable and non-bioavailable (Hu and Cheng
2016; Tessier and Campbell 1987).
In all experiments, laboratory-produced triple-distilled wa-
ter was used. The extraction liquids were prepared from re-
agents of analytical grade or better and were checked for pos-
sible trace metal contamination. All the plastic vessels used
were pre-soaked in dilute nitric acid solution (10%, v/v) for
24 h and rinsed with triple-distilled water.
Data analysis
T test and Wilcoxon rank-sum test were conducted for the
heavy metal contents in all soil samples (n = 70) to evaluate
whether e-waste recycling activities have caused more severe
heavy metal pollution compared to traditional industrial oper-
ations in the PRD. Principal component analysis (PCA) was
used to determine the distribution patterns of heavy metals in
the surface soils from the traditional industry regions and the
e-waste recycling areas, and identify their probable sources.
Pearson correlation was performed to analyze the relationship
between the gross domestic product (GDP) and potential eco-
logical risk of soil heavy metal pollution in both the e-waste
recycling areas and the traditional industrial zones. All statis-
tical analyses were conducted using SPSS (version 18.0) soft-
ware package for Windows.
The contamination level for each heavy metal species in the
surface soils was evaluated with the pollution index (PI),
which is calculated as
Ci
PI ¼ ð1Þ
Si
where Ci is the measured concentration (mg/kg) of the metal
and Si is the corresponding local background level (mg/kg). The
background levels of As, Cd, Cr, Cu, Ni, Pb, and Zn in the
surface soils of Guangdong Province are 8.9, 0.056, 50.5, 17.0,
14.4, 36.0, and 47.3 mg/kg, respectively (Zhang et al. 2012a).
Based on the PI values, the level of heavy metal pollution can be
classified as low (PI ≤ 1), moderate (1 < PI ≤ 3), or high (PI > 3)
(Chen et al. 2005; Wei and Yang 2010).
The potential ecological risk of heavy metals in the surface
soils of the PRD was evaluated with the comprehensive eco-
logical risk index (RI), which is defined as
RI ¼ ∑E i ð2Þ
Ei is the potential ecological risk index of the individual
metal species and can be calculated from the measured content
of the metal in the soil (Ci) and its background level (Si) as
Ci
Ei ¼ T i ð3Þ
Si
where Ti is the toxicity factor of the heavy metal and the values
for Cr, Ni, Cu, Zn, As, Cd, and Pb are 2, 5, 5, 1, 10, 30, and 5,
Environ Sci Pollut Res (2017) 24:9387–9398
respectively (Hakanson 1980). The threshold values for clas-
sification of the potential ecological risk of heavy metals in the
soils based on Ei and RI values are summarized in Table S1.
Results and discussion
Heavy metal contents of the surface soils
Table 1 summarizes the total contents of Cr, Ni, Cu, Zn, As,
Cd, and Pb in the surface soils of the e-waste recycling areas
(Qingyuan and Guiyu) and the traditional industrial zones
(Dongguan, Zhuhai, and Zhongshan) of the PRD, together
with their soil background values. The mean contents of Cu,
Zn, As, and Cd in the surface soils of Qingyuan were 33.8,
141.4, 20.6, and 0.5 mg/kg, which are 2.0, 3.0, 2.3, and 9.0
times higher than the corresponding soil background values,
respectively. Luo et al. (2008) found that the concentrations of
Pb, Cu, and Cd in the soils surrounding e-waste open burning
sites in Longtang Town of Qingyuan were up to 1267-, 178-,
and 100-fold higher than those in the control site, respectively.
As the surface soil samples were collected in the forestry and
agricultural lands with the intention of avoiding direct source
inputs in this study, the enrichment of heavy metals was much
less significant compared to that reported in Luo et al. (2008).
Nonetheless, these results could be more representative of the
overall heavy metal pollution in the e-waste recycling areas.
The coefficient of variation (CV) can reflect the degree of
variability in the contents of heavy metals in the soils (low,
CV < 20%; moderate, 20% ≤ CV ≤ 50%; high, CV > 50%;
exceptionally high, CV > 100%) (Xiao et al. 2015). It has been
reported that heavy metals with CV values less than 20% are
dominated by natural sources, while those with CV values
above 50% are mainly affected by anthropogenic sources
(Guo et al. 2012). The CV values for the contents of Cu, As,
and Cd in the soils of Qingyuan were all greater than 50%.
That is, the contents of these metals varied largely among
different sites and they were contributed significantly by an-
thropogenic sources, presumably the prevalent e-waste
recycling activities. In the soils from Guiyu, the CV values
of Cd, Cu, Cr, and Ni were 104, 85, 60, and 58%, respectively,
which also suggests that human activities had contributed sig-
nificantly to these metals.
The above results indicate that e-waste recycling activities,
which often involve dismantling of circuit boards and cables
by burning, heating, and acid pickling, could cause contami-
nation of surface soils by heavy metals. In addition, the PI
values (Table 1) show that the soils in Qingyuan were highly
contaminated by Cd and moderately contaminated by Cu, As,
and Zn, while the soils in Guiyu were moderately contaminat-
ed by Cu, Cd, and Zn. Such difference probably resulted from
different types of e-waste products dismantled in Qingyuan
and Guiyu. Quan et al. (2015) observed that uncontrolled e-
Environ Sci Pollut Res (2017) 24:9387–9398 9391

Table 1 Summary of heavy

metal contents (mg/kg) in the Location Items Mean Minimum Maximum SD CV (%) PI Si
surface soil samples collected
from the e-waste recycling areas Qingyuan (n = 27) Cr 27.92 3.46 91.13 18.68 67 0.55 50.50
(Qingyuan and Guiyu) and the Ni 13.06 1.51 51.35 10.87 83 0.91 14.40
traditional industrial zones Cu 33.77 3.05 158.25 43.47 129 1.99 17.00
(Dongguan, Zhuhai, and
Zhongshan) of the PRD Zn 141.42 14.00 258.50 64.68 46 2.99 47.30
As 20.55 4.56 55.91 15.97 78 2.31 8.90
Cd 0.50 0.01 2.54 0.70 138 9.00 0.06
Pb 34.39 5.64 70.35 19.21 56 0.96 36.00
Guiyu (n = 23) Cr 20.99 4.70 41.74 12.69 60 0.42 50.50
Ni 8.34 2.70 17.46 4.81 58 0.58 14.40
Cu 17.34 1.20 48.10 14.81 85 1.02 17.00
Zn 127.94 34.79 224.33 49.40 39 2.70 47.30
As 6.65 1.88 13.65 3.04 46 0.75 8.90
Cd 0.13 <0.001 0.44 0.14 104 2.35 0.06
Pb 34.47 5.40 66.25 16.10 47 0.96 36.00
Dongguan (n = 6) Cr 33.06 17.63 42.31 8.80 27 0.65 50.50
Ni 13.34 7.20 16.71 3.40 26 0.93 14.40
Cu 31.70 13.93 99.75 33.73 106 1.86 17.00
Zn 119.66 81.75 159.30 33.88 28 2.53 47.30
As 21.85 11.13 28.41 6.73 31 2.46 8.90
Cd 0.14 0.10 0.26 0.06 45 2.52 0.06
Pb 38.90 25.28 52.79 9.66 25 1.08 36.00
Zhuhai (n = 5) Cr 18.35 6.17 34.81 11.59 63 0.36 50.50
Ni 7.57 4.13 17.84 5.86 77 0.53 14.40
Cu 14.12 2.92 30.41 13.84 98 0.83 17.00
Zn 203.81 124.31 284.88 75.81 37 4.31 47.30
As 6.03 3.84 7.24 1.53 25 0.68 8.90
Cd 0.37 0.06 0.75 0.30 81 6.58 0.06
Pb 83.62 42.40 130.72 31.68 38 2.32 36.00
Zhongshan (n = 9) Cr 27.34 8.40 87.15 31.12 114 0.54 50.50
Ni 27.72 2.66 134.05 42.25 152 1.92 14.40
Cu 18.78 1.88 60.31 23.08 123 1.10 17.00
Zn 157.28 63.35 312.03 84.99 54 3.33 47.30
As 11.76 4.05 32.54 9.87 84 1.32 8.90
Cd 0.23 0.01 0.67 0.24 101 4.17 0.06
Pb 25.44 3.14 63.52 17.85 70 0.71 36.00

SD standard deviation, CV coefficient of variation, PI pollution index, Si regional soil background

waste processing caused contamination of surface soils by Ni,
Cu, Zn, Cd, Pb, Sn, and Sb in Guiyu, and the contamination
was particularly heavy for the surface soils in acid-leaching
areas. Overall, the enrichment of heavy metals in the surface
soils in the e-waste recycling areas in the PRD is similar to that
observed in the e-waste processing areas in Zhejiang province
of southeastern China. For example, Fu et al. (2008) found
that the soils from e-waste recycling areas in Taizhou were
primarily contaminated by Cd, followed by Cu, whereas the
contamination of Pb, Ni, Cr, and Hg was not serious. Fu et al.
(2013) reported that the concentrations of Cd, Cu, and Pb in
the soils from the e-waste dismantling areas in Taizhou were
remarkably higher than those in the control areas without e-
waste dismantling, and the soil contents of Pb, Cu, and Cd
were closely correlated with e-waste recycling activities. Zhao
et al. (2016) reported that the concentrations of Cd, Cu, Zn,
Pb, and Ni in the surface soils of e-waste recycling areas in
Wenling were above the background levels, with the contents
of Cd and Pb exhibiting exceptionally high variability and
those of Cu, Zn, and Ni having moderate variability.
Pollution of surface soils was also observed in the tradi-
tional industrial zones of the PRD. The contents of Zn, As, and
Cd in all the soil samples from Dongguan were higher than the
values of soil background in Guangdong province. The PI
9392
values of Cu and Pb were in the range of 1.0 to 2.0, which are
indicative of moderate contamination. In contrast, with PI
values greater than 2.0, the contamination level of Zn, As,
and Cd was high, which suggests that anthropogenic activi-
ties, primarily manufacturing of electronics and hardware, had
caused significant enrichment of these metals in the surface
soils. Similarly, the surface soils from Zhuhai were highly
contaminated by Zn and Pb, and severely polluted by Cd,
while the soils from Zhongshan were seriously polluted by
Zn and Cd. This is not surprising as these cities are major
production bases of electronic and information technology
products, machinery and equipment, hardware, and home ap-
pliances in China. In general, the CV values of all the mea-
sured heavy metals in the surface soils from Dongguan,
Zhuhai, and Zhongshan were higher than 20%, indicating
moderate variability, except for Cu, which exhibited excep-
tionally high CV values. These results indicate that heavy
metals in the surface soils of Dongguan, Zhuhai, and
Zhongshan had been significantly influenced by anthropogen-
ic sources, mainly the traditional industrial operations. Soil
pollution by heavy metals in the PRD has been shown to be
strongly affected by the types of land use, with much heavier
pollution occurring in the industrial lands compared to the
agricultural and forestry lands (Hu and Cheng 2013, 2016).
Mahmoudabadi et al. (2015) also showed that the distribution
of heavy metals in the surface soils of an industrial zone in the
west of Tehran City, Iran, was primarily affected by industrial
activities and road traffic. Together, the above results show
that the contents of heavy metals in the surface soils from
the e-waste recycling areas were in ranges comparable to those
occurring in the surface soils from the traditional industrial
zones, and significant portions of the heavy metals in the
surface soils of these areas were contributed by human
activities.
Chemical fractionation of heavy metals in the surface soils
Figure 2 depicts the overall partitioning of heavy metals
among the acid soluble, reducible, oxidizable, and residual
fractions of the surface soils in the e-waste recycling areas
and the traditional industrial zones of the PRD. Most of Cd
resided in the acid soluble fraction (63.6%) and the reducible
fraction (20.6%) in the soils from Qingyuan (Fig. 2a), thus Cd
could pose significant ready and potential risk to the environ-
ment and ecosystem (Hu et al. 2016). Significant portions
(>20%) of Zn, Ni, and Cu were also present in the acid soluble
faction. These results indicate that Cd, Zn, Ni, and Cu in the
surface soils were sensitive to the variation of environmental
conditions (e.g., pH) and could easily become mobile and
bioavailable (Hu and Cheng 2016; Huang et al. 2013). Cu
(39.4%) and Pb (45.5%) partitioned mainly in the reducible
fraction, indicating they were potentially mobile and bioavail-
able in the soils. In contrast, Cr (84.6%), As (76.6%), Ni
Environ Sci Pollut Res (2017) 24:9387–9398
(64.7%), and Zn (63.4%) were primarily present in the resid-
ual fraction, which is not available for biogeochemical cy-
cling. Despite the relatively high contents of these metals in
the surface soils, they could pose a relatively low risk to the
environment and ecosystem. Overall, more than half of the
Cd, Cu, and Pb were partitioned in the non-residual fraction
in the soils from Qingyuan. Zhang et al. (2015b) have also
previously shown that on the average, 61.3% of Pb, 65.3% of
Cu, and 80.7% of Cd were present in the readily and poten-
tially bioavailable fractions in the farmland soils polluted by e-
waste recycling activities in Qingyuan. In general, the chem-
ical fractionation of heavy metals in the surface soils from
Guiyu is comparable to that observed in the surface soils from
Qingyuan. On average, 60.1% of Cd was present in the acid
soluble fraction, while most of Cr (85.1%), Zn (72.7%), Ni
(65.0%), As (49.6%), and Cu (38.9%) were partitioned in the
residual fraction (Fig. 2b). Pb (59.7%), As (34.8), and Cu
(30.2%) had significant portions distributed in the reducible
fraction, indicating high potential mobility and bioavailability.
Overall, these findings are comparable to those reported in the
study by Luo et al. (2011), which found that Cd had much
higher mobility and bioavailability compared to the other
heavy metals (Cu, Cr, Pb, Ni, and Zn) in the surface soils
impacted by e-waste recycling activities in Qingyuan.
Cd (66.5%) and Cu (52.1%) in the surface soils from
Dongguan were mainly present in the acid soluble fraction
(Fig. 2c), while they also had considerable portions (26.1
and 24.4%, respectively) partitioned in the reducible fraction.
Pb was predominantly partitioned in the reducible fraction
(77.0%), indicating most of Pb in the soils is potentially mo-
bile and bioavailable. In contrast, Cr (83.3%), Ni (72.5%), As
(72.3%), and Zn (67.3%) resided mostly in the residual frac-
tion that is not bioavailable. In the surface soils from Zhuhai
(Fig. 2d), Cu (33.9%), As (37.7%), and Pb (51.2%) were
primarily bound in the reducible fraction, implying they could
pose potential risk to the ecosystem, while Cr (80.6%), Ni
(61.5%), and Zn (56.5%) were present predominantly in the
residual fraction. Cd in the soils from Zhuhai could pose a
significant risk due to its high contents (mean = 0.37 mg/kg)
and high percentage partitioned in the acid soluble fraction
(mean = 61.7%). Similarly, most of the Cd (53.6%) in the
surface soils from Zhongshan was also present in the acid
soluble fraction (Fig. 2e). Pb resided primarily in the reducible
fraction (51.0%), while Cr (81.2%), Ni (73.6%), Cu (41.3%),
Zn (62.4%), and As (84.8%) were mostly partitioned in the
residual fraction, suggesting they were biogeochemically sta-
ble and posed a relatively low risk. Dongguan, Zhuhai, and
Zhongshan are among the largest electronic manufacturing
centers in the world, and they also host many heavily polluting
industries, such as chemical, paper-making, dying, smelting,
and electroplating. Qiu et al. (2015) found that the concentra-
tions of Cd and Zn in agricultural soils of Dongguan increased
by 54.7 and 20.8%, respectively, while those of Cr, As, Cu,
Environ Sci Pollut Res (2017) 24:9387–9398 9393

Fig. 2 The overall partitioning of As, Cd, Cr, Cu, Ni, Pb, and Zn among the acid soluble, reducible, oxidizable, and residual fractions of the surface soils
from a Qingyuan, b Guiyu, c Dongguan, d Zhuhai, and e Zhongshan based on the mean measured contents

and Ni changed little between 2002 and 2012. Heavy metals Overall, the results of sequential extraction show that Cu,
introduced into surface soils by human activities would be Cd, and Pb were primarily present in the non-residual fraction
present primarily in the non-residual fractions and thus had in the soils from both the e-waste recycling areas and the
high mobility and bioavailability (Hu and Cheng 2016). traditional industrial zones, which is indicative of significant
9394 Environ Sci Pollut Res (2017) 24:9387–9398

anthropogenic contribution (Hu and Cheng 2016). These metals Cu (85%), Zn (80%), As (95%), Cd (92%), and Pb (90%)
are readily and potentially mobile and bioavailable, and could suggest that these five principal components could represent
pose a significant potential risk when occurring at high levels in the heavy metals well. Factor loadings are considered to be
the surface soils as the red soils in the PRD are typically highly excellent with the values higher than 0.71 and poor in cases
weathered and acidic (Hu et al. 2016; Wilson et al. 2004). In of values lower than 0.32 (Garcia et al. 2004). PC1 explained
contrast, most of the Cr, Ni, and Zn were partitioned in the 21.95% of the total variance and was dominated by Cu and Cd
residual fraction, posing a relatively low risk to the ecosystem. with loading coefficients of 0.75 and 0.91, respectively. Pb and
As was primarily partitioned in the residual fraction in the surface Zn exhibited high factor loading values in PC2, which
soils from Qingyuan, Dongguan, and Zhongshan, about half of accounted for 21.24% of the total variance. These results indi-
the As in the surface soils from Guiyu was presented in the cate that Cu, Cd, Pb, and Zn in the surface soils were probably
residual fraction. Relatively high mobility and bioavailability contributed primarily by the anthropogenic sources. As, Cr, and
were observed for As only in the surface soils of Zhuhai. Ni had the highest factor loading values in PC3, PC4, and PC5,
Apparently, there is no significant difference in the chemical respectively, and they originated mostly from soil parent mate-
fractionation of heavy metals in the surface soils between the rials, which is consistent with the findings of source apportion-
traditional industrial zones and the e-waste recycling areas of ment studies for heavy metals in the surface soils of the PRD
the PRD. (Hu and Cheng 2013, 2016). Each of the investigated heavy
metals had one factor loading value greater than 0.7 in these
Occurrence patterns of heavy metals in the surface soils five principal components. It should be noted that Cu and Zn
exhibited quasi-independent behavior in the group, as they also
The heavy metals in the surface soils from the e-waste recycling had factor loading values (0.52 and 0.41, respectively) between
areas and the traditionally industrial zones could come from 0.32 and 0.7 in other principal components (Hu et al. 2013).
both natural and anthropogenic sources (Cheng and Hu 2010; Heavy metal pollution in the surface soils from different
Hu and Cheng 2013, 2016). Due to the relatively large numbers sites was further examined with the score plots of PCA.
of soil samples and multiple heavy metal species measured for Figure 3a to c depicts the distribution patterns of heavy metals
each sample, it is necessary to reduce the multi-dimensional in the surface soils collected from two e-waste recycling areas
data sets to lower dimensions. PCA has been commonly and three traditional industrial zones. Table 2 indicates that the
employed to identify the heavy metals or heavy metal clusters variance explained by PC1 and PC2 is very close, while PC3,
in the soils that account for the majority of the variation and PC4, and PCA5 also explain comparable percentages of the
infer their sources (Hu et al. 2013; Liu et al. 2015; Zhang et al. total variance. Thus, all five principal components are shown
2012b). PCA with Varimax rotation was used in the present on the PCA score plots. Overall, no apparent spatial clustering
study to examine the association of heavy metals in the surface of the sampling sites was observed. With the exception of
soils from the e-waste recycling areas and the traditional indus- several samples with extreme values from Qingyuan, the soils
trial zones based on the measured metal contents of all samples. collected from e-waste recycling areas were well mixed with
Five principal components (PC1–PC5), which could explain those collected from the traditional industry zones. That is,
more than 90% the cumulative variance, were retained for anal- there was no distinction in the pollution characteristic of heavy
ysis (Table 2). The communality values of Cr (97%), Ni (98%), metals in the surface soils between the e-waste recycling areas
and the traditional industrial zones. It is noted that PC5 and
PC4, which were dominated by Cr and Ni, respectively, ex-
Table 2 The rotated component matrix of heavy metal contents in the hibit significant linear correlation (Fig. 3c). This was due to
surface soil samples obtained from PCA with Varimax normalized
rotation the fact that these metals were contributed primarily by the soil
parent materials (Hu and Cheng 2013, 2016).
Metal PC1 PC2 PC3 PC4 PC5 The T test and the Wilcoxon rank-sum test were conducted
to further investigate whether the mean concentrations of
Cr 0.16 0.16 0.19 0.92 0.15
heavy metals in the surface soils collected from the e-waste
Ni 0.09 0.07 0.11 0.15 0.97
recycling areas and the traditional industrial zones had com-
Cu 0.75 0.09 0.52 0.13 0.02
parable occurrence patterns. Table 3 shows that the p values of
Zn 0.21 0.71 0.06 0.41 0.27
T test vary between 0.10 for Ni and 0.81 for As, while the
As 0.22 0.13 0.91 0.18 0.14
Wilcoxon test yields p values ranging from 0.33 for Pb to 0.94
Cd 0.91 0.22 0.08 0.14 0.11
for Cr. The p values were all higher than 0.05, indicating none
Pb 0.13 0.93 0.12 0.02 −0.04
of these tests detect any significant statistical difference in the
Variance explained (%) 21.95 21.24 16.80 15.92 15.20
occurrence of heavy metals in the surface soils between the e-
Factor loadings greater than 0.32, which could account for significant waste recycling areas and the traditional industrial zones.
portion of the overall variance, are marked with boldface These results consistently indicate that the heavy metal
Environ Sci Pollut Res (2017) 24:9387–9398 9395

Fig. 3 PCA score plots grouping the surface soil samples from different sites on the planes of a PC1 and PC2, b PC3 and PC4, and c PC4 and PC5

pollution caused by e-waste recycling activities was compara-
ble to that brought by traditional industrial operations in the
PRD.
Ecological risk of heavy metal pollution
Table 4 summarizes the potential ecological risk index (Ei)
posed by individual metal species and the comprehensive po-
tential ecological risk index (RI) of heavy metal pollution in
the surface soils from the e-waste recycling areas and the
traditional industrial zones of the PRD. Apparently, Cd posed
a high risk in the surface soils of Qingyuan and moderate risk
in the surface soils of Guiyu, while the other heavy metals
posed low ecological risk based on their Ei values. In the
traditional industrial zones, Cd posed moderate, high, and
considerable risk in the surface soils of Dongguan,
Zhongshan, and Zhuhai, respectively, while the other metals
posed low ecological risk. The potential ecological risk of

Table 3 T test and Wilcoxon

rank-sum test of heavy metal Metal Samples from e-waste recycling areas and traditional industrial zones
contents in the surface soil sam-
ples collected from the e-waste T test Wilcoxon rank-sum test
recycling areas and the traditional
industrial zones of the PRD T value Prob F χ2 p

As 0.06 0.81 0.01 0.92

Cd 0.54 0.47 0.24 0.62
Cr 0.19 0.67 0.01 0.94
Cu 0.31 0.58 0.11 0.74
Ni 2.74 0.10 0.69 0.41
Pb 2.68 0.11 0.95 0.33
Zn 1.80 0.18 0.76 0.38
9396 Environ Sci Pollut Res (2017) 24:9387–9398

Table 4 The potential ecological

risk posed by individual metal Category Location Ei RI
species (Ei) and multiple metals
(RI) present in the surface soils Cr Ni Cu Zn As Cd Pb
from the e-waste recycling areas
and the traditional industrial E-waste recycling areas Qingyuan 1.11 4.53 9.93 2.99 23.09 269.91 4.78 316.34
zones of the PRD Guiyu 0.83 2.89 5.10 2.70 7.47 70.53 4.79 94.31
Traditional industrial Dongguan 1.31 4.63 9.32 2.53 24.55 75.67 5.40 123.43
zones Zhuhai 0.73 2.63 4.15 4.31 6.78 197.37 11.61 227.58
Zhongshan 1.08 5.92 7.16 3.33 13.21 125.08 3.53 159.31

heavy metals in the surface soils from Qingyuan was merely
in the category of high (RI = 316.3), which was contributed
predominantly by Cd, while the heavy metals in the surface
soils of Guiyu posed a low risk. In comparison, the potential
ecological risk posed by heavy metals present in the soils from
the traditional industrial zones ranged from low to moderate,
which was also dominated by that from Cd. Together, these
results indicated that the ecological risk of heavy metals in the
soils from the e-waste recycling areas and that from the tradi-
tional industrial zones was comparable.
Massive industrialization of the previously rural lands has
occurred gradually in the PRD, spanning for over three and a
half decades (Hu et al. 2013). In contrast, e-waste recycling
activities started in Guiyu and Qingyuan less than two decades
ago (Sun et al. 2016), but they already caused soil heavy metal
pollution comparable to that brought by the traditional indus-
trial operations. Table S2 summarizes the average GDP of
Qingyuan, Chaoyang District of Shantou (where Guiyu is
located), Dongguan, Zhuhai, and Zhongshan over the period
of 2005 to 2009. A statistically significant correlation was
found between the RI of heavy metals and the average GDP
in Qingyuan and Chaoyang District of Shantou, while the RI
values of heavy metals in the traditional industrial zones were
not correlated with the local GPD values (Tables S3–S4).
These results suggest that contamination of surface soils by
heavy metals in Qingyuan and Guiyu resulted primarily from
the e-waste recycling activities, which also contributed to ma-
jor portion of GDP in these areas. In contrast, heavy metal
contamination of surface soils in Dongguan, Zhuhai, and
Zhongshan was not correlated with local GDP. One possible
reason for this is that pollution prevention and control mea-
sures were implemented during the development of traditional
industrial operations, while pollutant releases to the environ-
ment in e-waste recycling areas were proportional to the
amount of e-waste processed due to the lack of effective pol-
lution control.
E-waste recycling activities are largely illegal and unregu-
lated in China. Dismantling of the e-waste using simple and
primitive methods and dumping of the waste residues in open
air have been well documented to release a range of pollutants,
including dusts that bear heavy metals and organic pollutants
(Cui and Forssberg 2003; Leung et al. 2006). As an industry,
e-waste recycling could contribute to local economic growth
and create employment opportunities, but it is much less ef-
fective compared to the traditional industrial operations.
Furthermore, e-waste recycling is highly damaging to the en-
vironment because of the primitive activities and the lack of
supervision. It has been estimated that e-waste recycling gen-
erated over 100 billion Yuan GDP per year in Guangdong.
Assuming that all the e-waste recycling activities occurred in
Qingyuan and Guiyu, the per capita GDP is only about 25,000
Yuan. In comparison, the per capita GDP in Dongguan was
estimated to be over 67,309 Yuan GDP in 2014 (Zhang and
Chen 2015a). Therefore, e-waste recycling has rather limited
contribution to economic growth, but bears high costs of en-
vironmental pollution, particularly with respect to heavy
metals. Therefore, the local governments of Qingyuan and
Guiyu need to take significant efforts on cracking down on
the illegal e-waste recycling activities. To minimize the pollu-
tion caused by e-waste recycling, the governments should also
guide the establishment of centralized facilities with proper
pollution control, while development of other types of indus-
tries, including the traditional industrial operations, can help
accelerate local economic growth. It is worth noting that the
pollution problem of e-waste recycling occurs not only in
China but also in some other developing countries in Asia
and Africa as well (Awasthi et al. 2016b; Fujimori et al.
2016; Iqbal et al. 2015). Thus, the findings of this study may
also provide valuable insights to these countries in term of
developing local economy and managing the e-waste
recycling activities.
Conclusion
The total contents and chemical fractionation of Cr, Cu, Zn,
Ni, As, Pb, and Cd in 70 surface soil samples collected from
representative e-waste recycling areas and traditional industri-
al zones in the PRD were analyzed. The concentrations of
heavy metals were elevated compared to the regional soil
background, and the CV values of some heavy metals were
over 30%, which is indicative of significant contribution from
anthropogenic sources. The soils in the e-waste recycling
areas were mainly polluted by Cu, Zn, As, and Cd, while those
Environ Sci Pollut Res (2017) 24:9387–9398
from the traditional industrial zones were primarily polluted
by Cu, Zn, As, Cd, and Pb. Results of PCA analysis suggest
that Cu, Cd, Pb, and Zn in the surface soils from both types of
sites were probably contributed mainly by anthropogenic
sources, while As, Cr, and Ni originated primarily from the
soil parent materials. Statistical analyses also show that the
pollution characteristic of heavy metals in the surface soils
from the e-waste recycling areas and the traditional industrial
zones was comparable. The potential ecological risk posed by
heavy metals in the surface soils from the traditional industrial
zones ranged from low to moderate and was dominated by
that from Cd, while that in the surface soils from the e-waste
recycling areas was comparable. Overall, the results consis-
tently suggest that e-waste recycling activities had not caused
more severe heavy metal pollution in the PRD compared to
the traditional industrial operations. However, the e-waste
recycling activities brought more intense heavy metal pollu-
tion and contributed less to economic growth compared to
traditional industrial operations. Therefore, significant efforts
should be made to control illegal e-waste recycling activities
and reduce the associated emissions of heavy metals to the
surrounding areas. The findings of this study can also help
guide the economic and environmental planning processes
in other e-waste recycling sites around the world.
Acknowledgements The constructive comments of the anonymous re-
viewers on an earlier version of this manuscript are greatly appreciated.
This study was supported in part by the National Key Research and
Development Program of China (2016YFD0800302), the Natural
Science Foundation of China (Grant Nos. 41673089 and 41472324),
the Fundamental Research Funds for the Central Universities (No.
2652015141), and the National Program for Support of Top-notch
Young Professionals.
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