Journal of Hazardous Materials 388 (2020) 121763

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Journal of Hazardous Materials

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Source-specific ecological risk analysis and critical source identification of T

heavy metals in road dust in Beijing, China
Cong Mena, Ruimin Liua,*, Libing Xub, Qingrui Wanga, Lijia Guoa, Yuexi Miaoa, Zhenyao Shena
a
State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, No. 19, Xinjiekouwai Street, Beijing, 100875, China
b
College of Agronomy, Nanjing Agricultural University, Nanjing, 210095, China

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

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

Editor: OK Yong Sik To explore the spatial variation of source-specific ecological risks and identify critical sources of heavy metals in
Keywords: road dust, 36 road dust samples collected in Beijing in March 2017 were analyzed for heavy metals. A new
Heavy metals method that takes into consideration the heavy-metal toxic response and is flexible to changes in the number of
Road dust calculated heavy metals, called the Nemerow integrated risk index (NIRI), was developed for ecological risk
Integrated ecological risk assessment. The NIRI indicated that heavy metals posed considerable to high risks at the majority of sites, and 22
Source-specific risk apportionment % of the sites suffered extreme risk in spring (NIRI > 320). Four main sources were identified based on positive
Critical source matrix factorization (PMF): traffic exhaust, fuel combustion, construction, and use of pesticides and fertilizers.
Owing to the lower toxic response factors of representative heavy metals of fuel combustion than those of other
sources, although fuel combustion had the highest contribution (34.21 %) to heavy metals in spring, it only
contributed 5.57 % to ecological risks. Critical sources and critical source areas were determined by considering
the contributions to both heavy metals and ecological risks. The use of pesticide and fertilizer and traffic-related
exhaust were identified as critical sources of heavy metals in spring. Source-specific ecological risks and critical
sources of heavy metals changed with the changing seasons, which suggests that different strategies should be
adopted in different seasons.

⁎
Corresponding author.
E-mail address: liurm@bnu.edu.cn (R. Liu).

https://doi.org/10.1016/j.jhazmat.2019.121763
Received 12 September 2019; Received in revised form 24 November 2019; Accepted 25 November 2019
Available online 27 November 2019
0304-3894/ © 2019 Elsevier B.V. All rights reserved.
C. Men, et al.
1. Introduction
Cities have high population densities and intensive human activities
(Nian et al., 2018; Amjadian et al., 2016). Heavy metals are discharged
from various human activities in cities, such as coal combustion for
heating and industry, traffic exhaust, and discharge of raw sewage
(Huang et al., 2018a,b). Road dust act as the source and sink of heavy
metals and receives heavy metals from the air and soil (Duzgoren-Aydin
et al., 2006). The self-regulating ability of ecosystems in cities is weaker
than that of natural ecosystems, which results in higher concentrations
of heavy metals than background values in many cities (Zhao et al.,
2015a). Heavy metals (i.e., As, Cd, Cr, Cu, Mn, Ni, and Pb) have a
strong tendency to accumulate and a weak tendency to degrade, and
can be transferred through the food chain (Zhuang et al., 2009). Heavy
metals, such as Cd, Pb, Zn, Mn, Cu, Hg, and Ni, have potential toxicity
that can result in cell injury and inflammation (Safiur Rahman et al.,
2019). These potentially toxic heavy metals can decrease the survival
rate of living organisms (Luo et al., 2014; Mohamad et al., 2018). In
particular, some heavy metals, such as As, Cd, Cr, and Ni, are classified
as class-I carcinogenic contaminants that can cause poisoning, anemia,
neurotoxicity, lung cell damage and other breathing problems (Liu and
Ren, 2019). Although Pb inorganics are classified as class-II carcino-
genic contaminants, high levels of Pb can affect nervous systems and
tissues of the brain, and Pb can even result in spontaneous abortion. In
many cities, heavy metals in road dust have resulted in ecological risk
(Amjadian et al., 2018).
Risks associated with heavy metals are influenced by various fac-
tors, such as concentration, toxicity, and the integrative actions of
multiple types of heavy metals (Wiesner et al., 2009). To assess the risks
and contamination caused by heavy metals, a variety of methods have
been applied, such as the use of the Nemerow integrated pollution
index (NIPI), geo-accumulation index (Igeo), potential ecological risk
index (RI), and enrichment factor (EF) (Liu et al., 2016; Men et al.,
2018a). These methods are used to evaluate risks of various aspects.
The NIPI and RI have been widely used among these methods (Soltani
et al., 2015; Sawut et al., 2018). However, the NIPI neglects the dif-
ferences in toxic response factors, which differ dozens of time between
some heavy metals (Liu et al., 2016; Zhao and Li, 2013). However, the
RI takes into consideration the toxic response factors, but the obtained
result may be exaggerated owing to the increased numbers of assessed
heavy metals for a certain sample (Wang et al., 2018a). For the risk
assessment, a new method is required to be developed that takes into
consideration the toxic response factor and eliminates the influence of
the number of assessed heavy metals.
Quantitative risk apportionment of heavy metals in road dust is
beneficial to the effective control of ecological risks (Praipipat et al.,
2017). A risk apportionment method was developed based on source
apportionment and risk assessment methods (Taghvaee et al., 2018).
Positive matrix factorization (PMF) is a receptor model that has been
widely applied in source apportionment (Praipipat et al., 2017; Liu
et al., 2019). With increasing attention on the pollution in road dust,
this method has been used in the source apportionment of heavy metals
in road dust in many cities (Zhang et al., 2019a; Men et al., 2018b).
Although the ecological risks of heavy metals have been studied in
many cities, research on the risk apportionment has just begun and is
now attracting increasing attention (Huang et al., 2018b; Shi et al.,
2019). Heavy-metal sources vary spatially because of the spatial var-
iation of human activities (Wang et al., 2018a; Hu et al., 2019; Park
et al., 2017; Wang et al., 2019a). A comprehensive understanding of the
risk apportionment and its spatial variation can contribute to the con-
trol of heavy metals in road dust.
A variety of sources caused heavy metal pollution, and the con-
tributions of these sources to risks vary greatly (Huang et al., 2018b).
The management of these sources usually requires considerable re-
sources, including manpower and material resources (Wang et al.,
2018b; Pu et al., 2019). Owing to limitation in the availability of time
2
Journal of Hazardous Materials 388 (2020) 121763
and resources, not all heavy-metal sources can be controlled at the same
time, and a stepwise management of the sources is more feasible (Chao
et al., 2019). Therefore, the determination of prior controlled sources is
the basis for pollution prevention and management (Cramer et al.,
2019). The concept of the critical source was introduced for the tar-
geted reduction of contamination and risks in road dust. Both the
amount of heavy metals (source apportionment) and ecological risks
(risk apportionment) contributed by sources should be considered in
the determination of the critical source (Wang et al., 2018c). Multiple
attribute decision making (MADM) methods can be used to determine
the weight of multiple factors, and the most suitable decision can be
selected from all alternatives (Escolar et al., 2019; Kalbar et al., 2017).
The use of MADM methods to determine the critical source would im-
prove pollution prevention and management.
In this study, using 36 road dust samples from Beijing in spring,
characteristics of source-specific ecological risks and critical sources of
heavy metals were explored using multiple methods, including PMF, a
newly developed risk assessment method (NIRI), and MADM methods.
The main objectives in this study were to: 1) establish a new assessment
method to improve the existing risk assessment methods and assess the
ecological risks posed by heavy metals; 2) evaluate the ecological risk
from each source and reveal their spatial characteristics; 3) determine
critical sources and critical source areas by considering both source
apportionment of heavy metals and source-specific risk apportionment.
2. Materials and methods
2.1. Study area
Beijing (115.7°–117.4 °E, 39.4°–41.6 °N) is the political and cultural
center of China (Fig. 1) (Men et al., 2018b). Beijing has an area of
approximately 16,410 km2 and is located in the northwest area of the
North China Plain. The climate in Beijing is distinct in its four seasons.
The weather in spring (March to May) is windy and dry. Beijing is a
typical representative city of rapid urbanization (Zhang et al., 2019b).
The permanent resident population in Beijing in 2017 was 21.7 million,
and the population density was 1323 persons/km2 (Beijing-Statistics-
Bureau, 2018). This large population has imposed considerable burdens
on the traffic, energy, and environment. The crowded traffic, high en-
ergy consumption, and other human activities have placed heavy bur-
dens on the environment, which has resulted in the contamination of
the soil, air, and road dust (Liu et al., 2018a; Meng et al., 2019; Wei
et al., 2015). Road dust poses potential ecological risks and health risks
(Tang et al., 2013; Yu et al., 2015).
2.2. Sampling
Samples were collected at 36 sites in urban Beijing in March 2017
(Fig. 1). These sampling sites were evenly distributed and covered the
entire study area, which were under the effect of various human ac-
tivities. Each sample composed five sub-samples. The sampling was
performed after the ground had been dry for over seven days. Plastic
brushes and dustpans were used on hardened ground to collect more
than 100 g of road dust at each site. The samples were stored in self-
sealing polyethylene bags. After the samples were air-dried for 15 days,
they were sieved with a 1,000-μm nylon sieve. Except for the sampling
time, the sampling procedures and determination of heavy metals in
road dust in this study was the same as that in our previous study re-
ferenced as (Men et al. (2018b)).
After referencing some related studies (Kefeni and Okonkwo, 2013;
Coufalík et al., 2014): arsenic (As), cadmium (Cd), chromium (Cr),
copper (Cu), mercury (Hg), manganese (Mn), nickel (Ni), lead (Pb), zinc
(Zn), and iron (Fe). Detailed information regarding the concentrations
of the heavy metals in each sample is available in the Supplemental
information. The experiments were performed under strict quality
control. The reference materials, blank samples, and three duplicates
C. Men, et al. Journal of Hazardous Materials 388 (2020) 121763

Fig. 1. Locations of the study area (Men et al., 2018b).

were used to ensure the reliability of the analysis. The recoveries Table 1
ranged from 88 % to 111 %. Blank samples showed no detectable The classification of Indexes.
metals, and repeat samples indicated that all the samples qualified Index Category Description References
under the quality control criteria.
NIPI NIPI ≤ 0.7; PI≤1 unpolluted (Yang et al.,
2.3. New risk assessment method: NIRI 0.7 < NIPI ≤ 1 Warning limit of 2011)
pollution
1 < NIPI ≤ 2; 1 < PI≤2 Low polluted
In this study, a new method called the NIRI was developed for as- 2 < NIPI ≤ 3; 2 < PI ≤3 Moderately polluted
sessing the integrated ecological risk of heavy metals based on the NIPI NIPI > 3; PI > 3 Strongly polluted
and potential ecological risk index (RI). RI RI≤150; Eri ≤40 Low risk (Zhao et al.,
150 < RI ≤ 300; Moderate risk 2015b)
Among the existing risk assessment methods, the NIPI and RI are
40 < Eri≤80
two that are widely used (Wang et al., 2017). The NIPI can be calcu- 300 < RI ≤ 600; Considerable risk
lated using the following formula (Yang et al., 2011; Fang et al., 2019): 80 < Eri≤160
RI > 600; 160 < Eri≤320 High risk
2 2
NIPI = (PIave + PImax ) 2 (1) Eri > 320 Extreme risk
NIRI NIRI ≤40; Eri≤40 Low risk Specified in this
PI = Ci Si (2) 40 < NIRI ≤ 80; Moderate risk study
40 < Eri≤80
where Ci is the concentration of heavy metal i and Si is the reference 80 < NIRI ≤ 160; Considerable risk
level of heavy metal i; Ci and Si have the same concentration units. PI is 80 < Eri≤160
the pollution index of each heavy metal; PIave and PImax are the mean 160 < NIRI ≤ 320; High risk
160 < Eri≤320
value and maximum value of PI of all the heavy metals studied. NIRI > 320; Eri > 320 Extreme risk
The formulas of RI are as follows (Li et al., 2017a; Zhao et al.,
2015b):
n the influence of the number of heavy metals on the value of the RI and
RI = ∑ Eri the lack of consideration of the difference in toxic response factors of
i=1 (3) heavy metals in the evaluation of the NIPI (Wang et al., 2008, 2018d).
Eri = Tri × Ci Si The NIRI can provide a more accurate evaluation of the integrated ef-
(4)
fect of multiple types of heavy metals. It also introduces the toxic re-
where Eri is the potential ecological risk factor of heavy metal i, r is the sponse factor to differentiate the effects of heavy metals. The NIRI can
abbreviation of risk and is not a variable; Tri is the toxic response factor be calculated using the following formula:
of heavy metal i, and Ci and Si were the same as those in Formula (2).
Classifications of the NIPI and RI are listed in Table 1.
NIRI = (Eri2max + Eraverage
i2
) 2 (5)
The NIRI overcomes the defects of the NIPI and RI, which include

3
C. Men, et al. Journal of Hazardous Materials 388 (2020) 121763

i
where Eri max and Eraverage are the maximum and average value of Eri , where n is the number of samples (36 in this study); and uji is the un-
respectively. certainty of heavy metal i in sample j, which is calculated as follows:
In this study, the value of the NIRI of As, Cd, Cr, Cu, Hg, Mn, Ni, Pb,
⎧ 5
and Zn were evaluated. The ecological risk of Fe in urban cities was × MDL, x ji ≤ MDL
generally ignored because of its low toxic response and comparable uji = 6
⎨
concentration with the background value (Bourliva et al., 2018; (σi × x ji )2 + (MDL)2 , x ji > MDL (11)
⎩
Ghanavati et al., 2019; Karimian Torghabeh et al., 2019; Li et al.,
2018a, b; Paul et al., 2019). Referenced from Tri in RI, Tri of As, Cd, Cr, where σi is the relative standard deviation of the concentration of heavy
Cu, Hg, Mn, Ni, Pb, and Zn in NIRI was 10, 30, 2, 5, 40, 1, 5, 5, and 1, metal i.
respectively (Fang et al., 2019; Hakanson, 1980). Si was the background In the PMF-based source apportionment, sources were determined
reference concentration of each heavy metal in the soils, and its value of based on both representative heavy metals and the information col-
As, Cd, Cr, Cu, Hg, Mn, Ni, Pb, and Zn was 9.6 μg/g, 0.079 μg/g, lected in the study area.
57.3 μg/g, 20.7 μg/g, 0.038 μg/g, 540 μg/g, 24.9 μg/g, 23.5 μg/g, and
68.0 μg/g, respectively (Wei et al. (1991)). 2.5. Critical source identification method
In the development of the NIRI in Formula (5), mean value and
maximum value of Eri of heavy metals were used. The structure of the In this study, the concept of the critical source, which integrates the
NIRI in Formula (5) was similar to the structure of NIPI in Formula (1). contributions of sources to heavy metals and proportions of sources to
As the classification of the NIPI is referenced from that of the PI, the risks, was introduced for targeted reduction of contamination and risks
classification of the NIRI could be referenced from that of Eri. The in road dust. Critical source identification is used in MADM problems,
classification of all the indexes referred to above are listed in Table 1. which can be analyzed via the combined use of the information entropy
method (IEM) and weighted method of simple additivity (SAW). The
2.4. Source-specific risk apportionment method IEM is a method used for objective weighting in multiple attribute
decision-making problems, which are widely encountered in various
Referencing the toxicity apportionment (Zhang et al., 2012), a fields, such as soft computing (Li et al., 2017a), laser physics (Garnaeva
method for risk apportionment based on various factors has been es- et al., 2018), and environmental science (Li et al., 2018b). The formula
tablished. The contributions of each source to the risk can be evaluated of the IEM is as follows:
through risk apportionment. In risk apportionment, the new risk as- A1 a11 ⋯ a1w
⎡ ⎤
sessment method of the NIRI and source apportionment by PMF were M= ⋮ ⎢⋮ ⋮ ⎥
combined. Types and contributions to the concentrations of heavy Ak ⎣ ak1 ⋯ akw ⎦ (12)
metals were imported into the formula of the NIRI. This can be ex-
apv
pressed as follows: Ppv = k
∑p = 1 apv (13)
RAp = (RAip2 max + RAipaverage
2
)
2 (6) k
B v = −K ∑ Ppv ln(Ppv )
RAip = Tri × Cip Si (7) p=1 (14)
where p and i represent different factors and heavy metals; m is the d v = 1 − Bv (15)
number of heavy metals; RAp is the value of the risk from factor p, and
the categories of RAp are the same as those of the NIRI in Table 1; RAip dv
Wv = w
is the risk of heavy metal i contributed by source p; Cip is the con- ∑v = 1 d v (16)
centration of the heavy metal i contributed by factor p. The values of Cip
were calculated and modelled in the source apportionment by using where M is the multiple attribute decision matrix of the critical sources;
PMF. Ak (p = 1 to k) is the kth source; v (v = 1 to w, and w = 2 in this study)
In the source apportionment via PMF, non-negativity constraints are represents the proportion to concentration of heavy metals (v = 1) and
implemented to more accurately reflect reality (Frie et al., 2017). A proportions to ecological risks (v = 2); apv represents the proportions of
matrix of concentrations of heavy metals could be decomposed into a each source to heavy metals or ecological risks; Ppv is the contribution of
source profile matrix (F ) and a source contribution matrix (G ) obtained the vth attribute of each source; B v is the total contribution of all
using PMF. The principles of the PMF model are as follows: sources; K is a constant, K = 1 ln k ; Wv is the weight of the vth attribute;
and d v is the uniformity of the vth attribute among different sources.
k
The vth attribute can be ignored when d v is zero.
x ji = ∑ gjp fpi + eji
Based on the results of the IEM, the critical sources are determined
p=1 (8)
using SAW:
m w
fp = ∑ fip m Zp = ∑ Ppv×Wv
i=1 (9) v=1 (17)
where x ji is the concentration of heavy metal i in sample j; gjp is the where Zp is the weight of each source. The identification of critical
proportion of source p in sample j; fpi is the proportion of source p in sources was based on the comparison of Zp among the different sources.
heavy metal i; fp is the proportion of source p to heavy metals; eji is the Sources with a higher Zp value than other sources should be identified
modeling error in the concentration of heavy metal i in sample j; and k as critical sources.
is the number of factors.
Q is the objection function that reflects the goodness of modeling. 3. Results and discussion
Factor contributions and profiles are derived using the PMF model by
minimizing the objective function Q . The formula of Q is as follows: 3.1. General characteristics of heavy metals in road dust
n m 2
⎡ eji ⎤
Q= ∑∑ ⎢ uji ⎥ The mean and median values of the concentrations of the majority
j=1 i=1 ⎣ ⎦ (10) of heavy metals exceeded their background values (Table 2) (Wei et al.,

4
C. Men, et al.
Table 2
Concentrations of heavy metals in the study area (μg/g).
As Cd Cr Cu
Background 9.7 0.074 68.1 23.6
Mean 4.08 0.51 99.50 97.37
Median 4.07 0.44 91.46 86.77
Min 1.87 0.13 50.01 20.57
Max 7.14 1.93 217.98 480.82
1991). However, only their mean concentrations of As, Mn, and Fe were
lower than their background values. The mean concentrations of Cu,
Hg, Ni, and Zn were also over two times their background values. The
mean concentration of Cd was 6.89 times its background value. This
may indicate that road dust is significantly influenced by human ac-
tivities (Tian et al., 2019).
For the majority of heavy metals, the concentrations in the central
area were higher than those in the surrounding areas (especially outside
the fourth ring road) (Fig. 2). The concentrations of the majority of the
heavy metals in the western and eastern areas were lower than those in
other areas, and only the concentrations of Cu and Zn reached their
highest value in the eastern and western area, respectively. The con-
centrations of As, Cd, Ni, and Fe in the northern areas were also higher
than those in other areas. The densities of the population and impact of
human activities in the central and northern areas may be greater than
those in other areas (Beijing-Statistics-Bureau, 2018).
3.2. Integrated ecological risk assessment
The values of the NIRI for the majority of the sites were higher than
40 in spring, which indicates no less than moderate risk at the majority
of the sites (Fig. 3a). Only one out of 36 sites was at low risk (NIRI was
34.40). The first and third quartiles of the NIRI were 83.94 and 276.35,
respectively, which indicates that the majority of the sites suffered
considerable risk to high risk. The NIRI at some sites (22 %) was even
higher than 320, which indicates extreme risk. The values of Eri differed
among heavy metals (Fig. S1). The values of Eri of Hg were the highest
among those of all heavy metals at 50 % of the sites, and the values of
Eri of Cd were the highest at 44 % of the sites. According to Formula (5),
the values of the NIRI were largely influenced by the Eri values of Hg
and Cd. Spatially, the NIRI was higher in the central part of the study
area, and the NIRI levels were similar from north to south (Fig. 3b). The
NIRI in the west and east was lower than those in other areas. The
values of the NIRI differed greatly between areas divided by different
ring roads. The mean value of the NIRI within different ring roads de-
creased in the order of second ring road (367.84) > second to third ring
road (324.51) > third to fourth ring road (262.94) > fourth ring road
to fifth ring road (204.70) > outside of the fifth ring road (155.33). The
standard deviation of the NIRI within different ring roads increased
from areas within the second ring road to areas outside of the fifth ring
road, which indicates a larger difference of the NIRI in the surrounding
areas. The spatial pattern of the risks was closely related to the spatial
intensities of the sources (Xu et al., 2019).
The difference in the NIRI levels and NIPI/RI levels at all the sites
was significant. The significance for the difference of levels of the NIRI
and NIPI was 1.4 %, and that of the NIRI and RI was less than 0.0 %.
The levels indicated by the NIPI were more severe that those of the
NIRI. The first quartile (3.85) of the NIPI at all the sites was larger than
the highest criterion (NIPI was 3), and the third quartile (10.17) of the
NIPI was over three times the highest criterion. In contrast to the values
of Eri max , the values of PImax at the majority of the sites (72 %) were the
values of the PI of Cd (Fig. S1). Only at 11 % of the sites, the values of
the PI of Hg were the highest among all the heavy metals. The differ-
ence in levels between the NIPI and NIRI (between PImax and Eri max )
verified the strong impact of the toxicity of heavy metals on the level of
risk. The toxicities of different heavy metals vary greatly, thus
Journal of Hazardous Materials 388 (2020) 121763
Hg Mn Ni Pb Zn Fe
0.069 705 29 25.4 102.6 29,700
0.26 536.29 40.76 62.29 255.90 28,697
0.16 527.60 27.03 56.72 235.73 27,858.08
0.03 408.82 17.40 18.85 64.80 22,858.81
1.26 697.08 402.35 137.02 480.18 44,463.99
influencing the levels of risk of heavy metals (Shi et al., 2018; Gao et al.,
2018). The toxic response factor should be introduced to reflect the
differences in the characteristics of heavy metals, which are neglected
by indices such as the NIPI (Brady et al., 2014; Cheng et al., 2015). As
compared with the NIPI, the NIRI not only considers the concentrations
of heavy metals but also the differences in the toxic response factors
among heavy metals.
The road dust was affected by multiple types of heavy metals (Men
et al., 2018a). Many studies have been conducted to assess the risks of
heavy metals, while the number of calculated heavy metal varied from
three to a dozen (Liu et al., 2016; Wang et al., 2012). Indices such as the
RI simply add the risks of different heavy metals to calculate the in-
tegrated risk (Sun et al., 2010). However, integrated risk is significantly
influenced by the number of calculated heavy metals, and this risk
would be higher in case of a larger number of heavy metals (Gao and
Wang, 2018; Sta et al., 2017). The impact of the number of heavy
metals calculated should be eliminated in risk assessments (Aldenberg
and Jaworska, 2000). The NIRI revised the undulation of the RI caused
by the number of heavy metals, and increases flexibility of the NIRI in
terms of changes in the number of calculated heavy metals.
3.3. Source-specific ecological risk analysis
Four sources contributed to the heavy metals in the road dust
(Fig. 4a). Source 1 was characterized by Cd (59.29 %), Pb (67.02 %),
and Zn (56.37 %). Cd, Pb, and Zn are contained in brakes, tires, lu-
bricating oil, roads, and pavements, and these heavy metals could be
released into the environment and then deposited and adsorbed into
road dust (Hou et al., 2019). Cd, Pb, and Zn were regarded as trace
elements of traffic exhaust (Wang et al., 2019b). Therefore, Source 1
was probably traffic exhaust. Source 2 contributed more (50.10–76.15
%) to As, Cr, Mn, Ni, and Fe. As and Ni were considered to be tracers of
fuel combustion (Turap et al., 2019; Zhang et al., 2018). Cr, Mn, and Fe
are also contained in fuels and could be released into the environment
in the form of fly ash and then deposited into road dust (Bozkurt et al.,
2018; Zhou et al., 2018). Therefore, Source 2 probably represented fuel
combustion. Source 3 was mainly represented by Cu (73.09 %). Cu is an
important element used in industrial activities such as constructions
(Wang et al., 2019b, e). Fine particles could be released into the en-
vironment under the effect of wind and accumulate in road dust. Source
3 probably represented constructions. Hg (89.69 %) was mainly con-
tributed by Source 4. Hg is an important element contained in pesti-
cides and fertilizers (Guo et al., 2019). In the afforestation of the city
and in agriculture, pesticides and fertilizers are widely used and over-
used in many situations (Onakpa et al., 2018). Hg could be released into
the environment during the use of pesticides and fertilizers, and the
excess pesticides and fertilizers could also migrate in the environment
and become concentrated in road dust (Liu et al., 2015). Source 4
probably represented the use of pesticides and fertilizers. Therefore,
traffic exhaust, fuel combustion, construction, and the use of pesticides
and fertilizers were the four sources that contributed to the presence of
heavy metals in road dust. Proportions of each source to heavy metals
were calculated using Formula (9). Among these sources, fuel com-
bustion had the greatest contribution of heavy metals, and its propor-
tion was 34.21 % (Fig. 4b). The contributions of traffic exhaust and use
of pesticides and fertilizers were similar at approximately 25 %.
5
C. Men, et al.
Fig. 2. Spatial patterns of concentrations of heavy metals in road dust.
Construction only contributed 15.81 % to heavy metals, which was the
smallest contribution.
Based on the source apportionment of heavy metals, source-specific
ecological risks were calculated using Formula (6) (Fig. 5). The ob-
tained results showed that risks from different sources varied. Traffic
exhaust contributed 41.34 % to the total risk of heavy metals in road
dust and resulted in no less than moderate risk. Construction only
6
Journal of Hazardous Materials 388 (2020) 121763
contributed 3.32 % to the total risk, and only posed low risks. Although
fuel combustion contributed more significantly to the presence of heavy
metals in road dust (34.21 %), it contributed a smaller proportion to the
risks (5.57 %) than other sources. In contrast, the use of pesticides and
fertilizers contributed less to heavy metals (25.73 %) than fuel com-
bustion, while it contributed the highest risk (49.75 %) among all
sources. Hg was mainly contributed by the use of pesticides and
C. Men, et al.
Fig. 3. Risks posed by heavy metals at different sites in spring: (a) Values of risks in different indexes; (b) Spatial pattern of NIRI.
fertilizers, of which the toxic response factor was 40, whereas the toxic
response factor of the main heavy metals contributed by fuel combus-
tion was less than 10. The toxic response factors differed greatly among
the heavy metals. The toxic response factor of Hg was the highest (40)
among all the heavy metals and is followed by that of Cd (30). They
were 40 and 30 times of that of Mn and Zn, respectively. The main
sources of heavy metals with a high toxicity (i.e., Hg and Cd) were more
likely to cause ecological risks than those with low toxicity (i. e., Mn
and Zn).Owing to the different toxic response factors of the heavy
metals, the levels of the proportions of sources may not be consistent
with the levels of the risks (Liu et al., 2018b).
Based on spatial pattern of contributions of each source to heavy
metals (Fig. S2), the spatial intensities of risks from each source were
analyzed (Fig. 6). The risks caused by traffic exhaust in the central area
were higher than other areas, whereas those in the western and eastern
areas were lower than those of other areas in the study area. The
densities of vehicles in the central area were higher than those in other
areas (Fig. S3), and the high-traffic conditions enhanced the release of
heavy metals (Sahu and Elumalai, 2017). The influence of traffic ex-
haust declined as the distance from traffic increased, which resulted in
weaker impacts on the surrounding areas (Sezgin et al., 2004). The
7
Journal of Hazardous Materials 388 (2020) 121763
higher risk caused by fuel combustion in the southern area was similar
to that in the northern area. This spatial similarity was partly because of
the wind blowing from north to south in the study area (Liu et al.,
2010). The migration of heavy metals from fuel combustion was in-
fluenced by multiple conditions, such as chimney height, speed and
direction of wind, and landscapes (Wang et al., 2016). The spatial
patterns of the risks from construction were opposite to those from
traffic exhaust. Risks from construction were higher in the surrounding
areas, but lower in the central areas. This type of pattern was probably
influenced by the spatial distribution of plants (Setyan et al., 2019). In
the central, northern, and southern parts of the study area, the risks
from use of pesticides and fertilizers were higher. The use of pesticides
and fertilizers in urban landscaping in the central area and agriculture
in the southern area may contribute to a higher risk in the central and
southern areas (Beijing-Statistics-Bureau, 2016; Arenas-Sánchez et al.,
2019).
3.4. Critical sources identification
The contributions of sources to heavy metals varied among the
sources, and the risks sources posed were also different (Huang et al.,
C. Men, et al. Journal of Hazardous Materials 388 (2020) 121763

Fig. 4. Contributions from each source: (a) to each kind of heavy metal; (b) to all heavy metals.

2018b). Owing to difference in the toxicity response factors of the

heavy metals, higher proportions of sources may pose lower risks (i.e.,
fuel combustion), whereas sources that contributed less to heavy metals
may pose higher risks (i.e., use of pesticides and fertilizers). Therefore,
to control the sources of heavy metals, attention should be focused not
only on the proportions of sources but also on the risks from different
source (Prakash et al., 2018). The proportions and risks of four sources
were analyzed to identify the critical sources. In terms of the weight of
each source (Z), the use of pesticides and fertilizers and traffic exhaust
had the largest (0.12) and second largest weight (0.10), both being over
six times those of other sources (Fig. 7a). Traffic exhaust and the use of
pesticides and fertilizers were identified as the critical sources in spring.
This was because of the proportions of heavy metals and risks con-
tributed by these two sources. The proportions of heavy metals con-
tributed by traffic exhaust and the use of pesticides and fertilizers were
both approximately 25 %, which was the second largest value among
all the sources. Furthermore, representative heavy metals of traffic
exhaust and the use of pesticides and fertilizers had high toxicity re-
sponse factors (Cd, 30; Hg, 40). Traffic exhaust and use of pesticides
and fertilizers contributed 41.34 % and 49.57 % to the total risks, re-
spectively.
Fig. 5. NIRI contributed by each source for heavy metals in road dust.
The critical source areas were different between ring roads (Fig. 7b).
The values of S of the critical sources (traffic exhaust and the use of
pesticides and fertilizers) were larger in the central ring road and

8
C. Men, et al.
Fig. 6. Spatial pattern of risks posed by each source.
decreased as the number of ring road increased, which indicates that
the critical source areas of the critical sources were all in the central
area. The Z value of traffic exhaust in the area within the third ring road
was 36%–38% higher than that outside the fifth ring road. The Z value
of use of pesticides and fertilizers in spring in the area within the third
ring road was 122%–241% higher than that in the area outside the fifth
ring road. Greater numbers of vehicles and high traffic conditions were
probably the reasons for the more significant influence of traffic ex-
haust, especially in the central area of the city (Zhang et al., 2019c).
Under the afforestation project (66,700 ha) launched in Beijing, the
afforested area is increasing in the central areas within the third ring
road, consumption of more pesticides and fertilizers (Tong et al., 2018;
Huang et al., 2017).
3.5. Temporal variation of ecological risks
Based on our previous works, the source-specific ecological risks of
heavy metals in road dust in summer, autumn, and winter were also
evaluated (Men et al., 2018a, b; Men et al., 2019). The levels of eco-
logical risk in different seasons were similar, whereas the interquartile
ranges of risks (NIRI) at different sites in other seasons were smaller
than that in spring (Fig. S4). This may be related to the migration
process of the main sources in different seasons. Traffic exhaust, con-
struction, and fuel combustion were the major contributors in summer,
autumn, and winter. As compared with heavy metals from the use of
pesticides and fertilizers, those from other sources could easily migrate
and become diffused in the study area, which resulted in smaller spatial
differences in these seasons (Chen and Poon, 2009; Hang et al., 2009;
Zhang et al., 2017). Both the mean value and interquartile range of
ecological risks at different sites in autumn were the lowest among all
the seasons. This was mainly because that the risk of each sources in
autumn were the lowest or the second lowest among all seasons.
Source-specific risks changes in seasons (Fig. S5). In summer, the
risk from traffic exhaust was the highest (close to 80) and reached a
considerable risk. As compared with other seasons, the higher tem-
perature in summer can accelerate tire wear, brake wear, and road
erosion (Kucbel et al., 2017). The increased number of tourists in
summer may also aggravate the adverse effects of traffic (Beijing-
Statistics-Bureau, 2018). In contrast to the moderate risk contributed by
9
Journal of Hazardous Materials 388 (2020) 121763
fuel combustion in winter, fuel combustion only contributed a low risk
in the majority of the seasons. This may be due to the increased heating
demand in winter (Rosser et al., 2016). The risk from the use of pes-
ticides and fertilizers reached its peak in spring, and the value of the
NIRI in spring was nearly twice that in other seasons. In contrast to the
other sources, the risks from construction were low in all the seasons.
The highest value of the NIRI from construction during all seasons was
only approximately 30.
The critical sources varied during different seasons, and the use of
pesticides and fertilizers was only critical in spring (Fig. S6). In addition
to spring, traffic exhaust was also a critical source in other seasons.
Although the proportions of traffic exhaust to heavy metals fluctuated
with the season, their values were the largest or second largest in each
season. The toxic response factor of Cd (a representative element of
traffic exhaust) was also higher than those of the majority of the heavy
metals, which resulted in higher ecological risks. In addition to traffic
exhaust, fuel combustion was another critical source in winter.
Although the toxic response factors of the main heavy metals (As, Cr,
Mn, and Ni) contributed by fuel combustion were all low (less than 10),
the proportion of fuel combustion to heavy metals was the largest
(32.40 %) in winter. Different strategies targeting critical sources
should be adopted in different seasons to reduce the ecological risks in
road dust.
Critical sources serve as a reference in the control of heavy-metal
contamination Wang et al. (2018c); Heathwaite et al. (2005). Effective
strategies targeted at critical sources should be adopted in different
seasons to reduce risks from heavy metals, and the focus should be on
critical source area (central area in the city) should be controlled. To
reduce the adverse effects of heavy metals from traffic exhaust in every
season, a limitation on the number of cars in use would be beneficial.
Efficient traffic management could also reduce the exhaust of heavy
metals in the case of a certain numbers of cars (Limo et al., 2018). In
winter, in addition to traffic exhaust, the control of fuel combustion is
also critical. New energy sources that generate fewer pollutants should
be explored and applied to replace fuel combustion (Michalski et al.,
2019; Nadaleti et al., 2019). To meet the demand of energy with the use
of fewer energy sources, their utilization efficiency should be monitored
and improved by using better facilities in factories and power stations
(Sedighizadeh et al., 2019; Sodiq et al., 2019). Pollutants generated in
C. Men, et al.
Fig. 7. Values of S for different sources in the identification of critical sources
(a) and critical source areas (b).
the combustion should be collected and controlled to prevent their
diffusion into the environment (Li et al., 2019). Reducing the heavy
metals emitted from the use of pesticides and fertilizers during spring is
also helpful and important. The use efficiency of pesticide and fertili-
zers should be improved to decrease the amounts used (Sun et al., 2010;
Iorns Magallanes, 2018). New types of pesticides and fertilizers that are
less of a hazard to the environment should be researched and developed
(Matzrafi, 2019).
4. Conclusions
A new method called the NIRI was developed for the risk assessment
of heavy metals. The obtained values of the NIRI showed that all the
sites were under no less than a low to moderate risk during spring, and
22 % of all the sites even suffered extreme risk. The NIRI decreased
from the central area and surrounding areas. The NIRI took into con-
sideration variations in the toxic response factors of different heavy
metals, and it was flexible to changes in terms of the number of cal-
culated heavy metals.
Four sources contributed heavy metals and ecological risks. They
were traffic exhaust, fuel combustion, construction, and the use of
10
Journal of Hazardous Materials 388 (2020) 121763
pesticides and fertilizers. Fuel combustion exhibited the largest con-
tributions to heavy metals (34.21 %) in spring, followed by traffic re-
lated exhaust and the use of pesticides, fertilizers and medical devices.
However, the source-specific ecological risks showed that fuel com-
bustion only contributed 5.57 % to the risks of heavy metals in road
dust. Ecological risks were predominantly contributed by traffic ex-
haust (41.34 %) and the use of pesticides and fertilizers (49.75 %); each
of these resulted in no less than moderate risks. In terms of the spatial
patterns of risks, the majority of the sources posed higher risks in the
central area, while higher risks from construction were mainly observed
in the surrounding areas.
Critical sources and critical-source areas were identified while
considering both proportions of sources and risks of sources. Traffic
exhaust and the use of pesticides and fertilizers were identified as the
critical sources in spring, which was indicated by their larger weights
(0.10 and 0.12, respectively). The impact of the critical sources varied
among the different ring roads, and the critical source areas were in the
central area.
Furthermore, the source-specific ecological risks and critical sources
of heavy metals changed with changes in the seasons. Different stra-
tegies targeted at critical sources and critical source areas should be
adopted in different seasons to reduce the risks from heavy metals in
road dust.
CRediT authorship contribution statement
Cong Men: Conceptualization, Methodology, Software, Writing -
original draft. Ruimin Liu: Conceptualization, Writing - review &
editing, Funding acquisition. Libing Xu: Data curation, Formal ana-
lysis. Qingrui Wang: Visualization, Investigation. Lijia Guo:
Validation, Resources. Yuexi Miao: Software, Resources. Zhenyao
Shen: Supervision, Funding acquisition.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgements
The research was funded by the Key Program of National Natural
Science Foundation of China (41530635), the National Key Research
and Development Plan (2016YFC0503005), the National Natural
Science Foundation of China (41571486) and the Interdiscipline
Research Funds of Beijing Normal University. The authors would like to
thank the editors and the anonymous reviewers for their valuable
comments and suggestions on this paper.
Appendix A. Supplementary data
Supplementary material related to this article can be found, in the
online version, at doi:https://doi.org/10.1016/j.jhazmat.2019.121763.
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