Quantitative assessment of human health risks induced by vehicle exhaust

polycyclic aromatic hydrocarbons at Zhengzhou via multimedia fugacity

models with cancer risk assessment

Qian Li1, Minjeong Kim1, 2, Ying Liu3, ChangKyoo Yoo1*

Supporting Information

Number of pages: 21

Number of tables: 12

Number of figures: 6

Table of Contents
1. Theory ...................................................................................................................................................... 3
1.1 Calculation of the VEPAHs emission rate ...................................................................................... 3
1.2 Multimedia fugacity model .............................................................................................................. 3
Table S1. Four types of fugacity models. ............................................................................................. 3
1.3 Incremental lifetime cancer risk model (ILCR) ............................................................................. 4
1.4 Model calibration of multimedia fugacity Level III model ........................................................... 5
1.4.1 Sensitivity analysis ..................................................................................................................... 5
Table S2. The distribution information of each parameter in BaP Level III model.............................. 6
1.4.2 Genetic algorithm....................................................................................................................... 7
Table S3. The updated value of degradation half-life time (hfa) and depth of air (dep_a) of VEPAHs.
.............................................................................................................................................................. 7
Table S4. The standard and modeled VEPAHs concentration in air phase. ......................................... 8
2. Model input.............................................................................................................................................. 9
2.1 Model input for motor vehicles properties ..................................................................................... 9
Table S5. The motor vehicles populations during 1999 to 2015 of Zhengzhou city and the annual
mileage of different type of vehicles (Zhengzhou Statistic Yearbooks). .............................................. 9
Table S6. On-road emission factors of particle-phase PAHs with different types of vehicles [Ho et
al., 2009] ............................................................................................................................................. 10
 Figure S1 The reported data and fitted curve of time-trend BAP emission rate based on fourth order
polynomial function. ........................................................................................................................... 11
2.2 Model input for chemical properties ............................................................................................. 11
Table S7. Physical-chemical properties and half-lives of VEPAHs. .................................................. 11
2.3 Model input for ILCR model ......................................................................................................... 12
Table S8. The parameters of ILCR model [3]..................................................................................... 12
Table S9. Toxic equivalency factors (TEFs) of VEPAHs [21]. .......................................................... 12
2.4 Model input for sensitivity analysis ............................................................................................... 13
Table S10. Specific parameters of chemical BAP. ............................................................................. 13
2.5 Model input for environmental properties ................................................................................... 14
Table S11. Environmental compartment parameters of Zhengzhou downtown area. ........................ 14
2.6 Model input for measured mortality rate of pulmonary diseases .............................................. 14
Table S12. The mortality rate of respiratory diseases and lung cancer............................................... 14
Figure S2. (a) Satellite-derived annual average surface-level PM2.5 concentration (μg/m3) of China
in 2008 (NASA); (b) vehicle population per unit area (/km2) of china in 2008 (Chinese Statistic
Yearbook, 2009); and (c) estimated lung cancer mortality rate (per 100,000) base on province in
China 2008 [24]. ................................................................................................................................. 16
3. Results .................................................................................................................................................... 17
Figure S3. BaP concentration attributions in each compartment of air, water, soil and sediment (bar
chart) with the VEPs concentration proportion (pie graphs)............................................................... 17
Figure S4. Sensitivity results of BaP posed health risk against the input parameters through different
exposure routes, including (a) total risk (b) dermal contact (c) inhalation and (d) ingestion. ............ 18
Figure S5. (a) Total BaP equivalent concentration and (b) the estimated ILCR of the VEPAHs in
Zhengzhou city during 17 years. ......................................................................................................... 19
Figure S6. The respiratory diseases and lung cancer mortality rate and the estimated air phase
VEPAHs concentration from 1999 to 2015. ....................................................................................... 20
Reference ................................................................................................................................................... 21
1. Theory
1.1 Calculation of the VEPAHs emission rate
The emission rate can be calculated using Eq. S1 [1].
ERw =  Pj  M j  EFwj (S1)

where ER [μg/year] is the emission rate of VEPAHs per year, P is the motor vehicle population,
M [km/year] is the corresponding average mileage, EF [μg/km] is the emission factor of VEPAHs
discharged from different categories of vehicle exhaust, diesel vehicles and gasoline vehicles.

1.2 Multimedia fugacity model

Multimedia fugacity models consist of four-level systems to evaluate the partitioning, diffusion,
and transformation of chemicals.

Table S1. Four types of fugacity models.

Type Description
Level I Closed and equilibrium system
Level II Opened and equilibrium system
Level III Opened and non-equilibrium system
Level IV Opened, non-equilibrium and unsteady state system

The mass-balance equations of the level III and IV models assume that the total input amount
of chemicals is equal to the sum of the total output amount and the accumulated amount, as follows:
E + DAdi f B + ( D ji f j ) − fi ( Dij + DAdi + DRi ) =  (S2)

where E [kg/h] is the emission rate, D [mol/Pa∙h] is the transport parameter, f [Pa] is the
fugacity of chemicals, the subscript B represents the background or initial value, Ad is the
adventive, R is the reaction, and i and j represent the environmental phase numbers. In Eq. S2, a
formula that product of D-values and fugacity is used to express the transport rate of the chemical.
The level III model assumes that the chemicals are in open system in steady state; thus, the term α
on the right side of Eq. S2 is considered to be zero. Alternatively, the Level IV model assumes that
the chemicals are in open system in non-steady state; thus, the term α is considered to be the time-
response fugacity: df / dt [2].
 The D-value used to explain the adventive term ( DAd ) is only considered in the air and water

phases and is obtained by Eq. S3:

DAdi = GZ = VZ /  A (S3)

where G [m3/h] is the flow rate, Z [mol/m3∙Pa] is the fugacity capacity, V [m3] is the volume of the
air or water phase, and  A [h] is the advection time. The D-value that describes the chemical

reaction ( DR ) is assumed to be a first-order reaction, as shown in Eq. S4.

DRi = VZ 1 2 R (S4)

where  1/2R [h] is half time of chemicals decomposition. The D-values of the diffusive process are

calculated based on Eq. S5.

Dij = KAij Z i (S5)

Where K [m/h] is the mass transfer coefficient, which can be treated as the net diffusion
velocity, and A [m2] is the interface area between two phases that are in contact [2]. The modified
part of the fugacity models is adding an additional mass transport process that corresponds to the
amount of pollutants in the air phase droplets in the build-up area that are deposited by rain; this
is calculated by Eq. S6.
Daero −build = K aero Abuild Z aero (S6)

where Drain −build [mol/Pa∙h] is the D-value of rain deposition, K rain [m/h] is the rain rate, Abuild [m2]

is the build-up area, and Z w [mol/m3∙Pa] is the fugacity capacity of water.

1.3 Incremental lifetime cancer risk model (ILCR)

The incremental lifetime cancer risk can be determined by Eq. S7.
Ri = SFi  ADI i (S7)

where SF [(mg/kg/day) –1] is the cancer slope factor of each VEPAH, and ADI [mg/kg/day] is
the average daily exposure dose, which is calculated by Eq. S8:
Ci   j IRij  EF  ED
ADI i = (S8)
BW  AT
where Ci [mg/m3] is the exposure concentration of VEPAHs in the i phase, IR [m3/day] is the

intake rate of VEPAHs per day, EF [days/year] is the exposure frequency in one year, ED [years]
is the exposure duration, BW [kg] is body weight, and AT [days] is the average exposure time
[3].
The VEPAHs in the air, water, and soil phases enter into the human body through dermal
contact. Eqs. S9- S11 express the intake rate of VEPAHs from these exposure sources through the
dermal contact route:
IRD − a = At  K p  ta (S9)

IRD − w = At  K p  t (S10)

IRD − s = As  ADF  ABF (S11)

where At [m2] the total skin surface area that contacts the polluted air and tap water when taking

a shower, K p [cm/h] is the dermal permeability coefficient of VEPAHs, t a [h/day] is the time that

skin is in contact with the air, t [min/day] is the shower time, As [cm2] is the skin surface area that

contacts the soil, ADF [mg/cm2/day] is the adherence factor of soil to skin, and ABF is the
dermal adsorption fraction [3, 4].
The VEPAHs in water, soil, and food are assumed to cause cancer risks to humans via ingestion.
Additionally, the VEPAHs in air can also cause cancer risks to humans through inhalation.

1.4 Model calibration of multimedia fugacity Level III model

The model calibration need to carry out before applying multimedia fugacity model to predict
the chemical behavior. The measured PAHs concentration in air is only available of year 2012 [5]
and the vehicle exhaust contribute to 27% of total emission sources of Zhengzhou in 2012 [6]. The
measured VEPAHs concentrations are listed in Table S4 and based on these standard concentration
the calibration method is implemented in Level III model. Firstly, the sensitivity analysis is carried
out to find the most influential parameters to the air phase VEPAHs concentration. Then the
genetic algorithm (GA) is used to optimize the model parameters via minimize the difference
between the modeled and the standard VEPAHs concentration.

1.4.1 Sensitivity analysis

For natural transport process, the input parameters in the sensitivity analysis follow a log-
normal distribution, which can be parameterized by the mean value ( m ) and confidence factor
( k ), where the confidence factor implies that 95% of all values are within a specific interval that
contains the mean value (the lower-limit is m / k , and the upper-limit is determined by m  k ) [7-
9]. The given variability of the input parameters were implemented with the Crystal Ball software
using Monte Carlo simulation methods with 10,000 trials (10,000 repeated random samplings).

For finding the effective parameters against the air phase concentration, 34 model parameters
were analyzed and the model default parameters for BaP chemical and the correlated confidence
factors of these parameters are listed in Table S2. After implementing the sensitivity analysis, the
degradation half-life time in air (hfa) and depth of air (dep_a) are found as the most influential
parameters of each VEPAHs for the air phase concentration.

Table S2. The distribution information of each parameter in BaP Level III model.
Assumed
Default
Variables Definitions confidence Lower limit Upper limit
value (m)
factor (k)
1 T Temperature 15.6 a 1.1 f 14.18 17.16

2 logKow Partition coefficients 6.04 b 2g 3.02 12.08

3 S Solubility in Water 0.0038 b 1.5 f 0.0025 0.0057

4 Pv Vapor Pressure 7.00×10-7 b 1.5 f 4.67 1.05×10-6

Degradation half-life time
5 hfa 5c 3g 1. 67 15
in air
Degradation half-life time
6 hfw 1440 c 3g 480 4320
in water
Degradation half-life time
7 hfs 2880 c 3g 960 8640
in soil
Degradation half-life time
8 hfse 13000 c 3g 4333 39000
in sediment
9 dep_a Depth of air 500 b – 10 b 1000 b

10 dep_w Depth of water 20 d 1.5 f 13.3 30

11 dep_s Depth of soil 0.2 d 1.5 f 0.13 0.3

12 dep_ase Depth of sediment 0.05 d 2f 0.025 0.1

13 fra_pa Fraction of particulate in air 3.7×10-10 e 3f 1.23×10-10 1.11×10-9

Fraction of particulate in
14 fra_pw 0.0027 e 3f 0.0009 0.0081
water
15 fra_fw Fraction of fish in water 1.00×10-6 d 3f 3.33×10-7 3×10-6

16 fra_as Fraction of air in soil 0.2 d 1.1 f 0.18 0.22

17 fra_wa Fraction of water in soil 0.3 d 1.1 f 0.27 0.33

Fraction of water in
18 fra_wse 0.8 d 1.1 f 0.72 0.88
sediment
19 foc1 OC content in soil solids 0.02 d 1.58 f 0.013 0.032
 OC content in sediment
20 foc2 0.04 d 1.5 f 0.027 0.06
solids
OC content in suspended
21 foc3 0.2 d 1.5 f 0.13 0.3
sediment
OC content in fish lipid
22 foc4 0.05 d 1.5 f 0.033 0.075
content
Air side air-water mass
23 mtc1 5d 3f 1.67 15
transfer coefficients
Water side air-water mass
24 mtc2 0.05 d 3f 0.0167 0.15
transfer coefficients
25 mtc3 Rain rate 4.37×10-4 a 3f 0.00015 0.0013

26 mtc4 Aerosol deposition velocity 6×10-10 d 3f 2×10-10 1.8×10-9

Soil air phase diffusion
27 mtc5 0.02 d 3f 0.0067 0.06
mass transfer coefficients
Soil water phase diffusion
28 mtc6 1.00×10-5 d 3f 3.33×10-6 3×10-5
mass transfer coefficients
Soil air boundary layer
29 mtc7 5d 3f 1.67 15
mass transfer coefficients
Soil air boundary layer
30 mtc8 1.00×10-4 d 3f 3.33×10-5 3×10-4
mass transfer coefficients
Sediment deposition
31 mtc9 5.00×10-7 d 3f 1.67×10-7 1.5×10-6
velocity
Sediment deposition
32 mtc10 2.00×10-7 d 3f 6.67×10-8 6E-7
velocity
33 mtc11 Soil water runoff rate 5.00×10-5 d 3f 1.67×10-5 1.5×10-4

34 mtc12 Soil solids runoff rate 1.00×10-8 d 3f 3.33×10-9 3×10-8

a
Refer from http://szb.zhengzhou.gov.cn/html/2012/zzgl_1219/57.html (Chinese); b Reference [2];
c
Reference [10]; d Reference [11]; e Reference [12]; f Reference [13]; g Reference [8];
1.4.2 Genetic algorithm
The genetic algorithm (GA) method is a popular tool to solve optimization problem based on
the concept of natural selection and genetics [14]. Many researchers already applied this method
to calibrate the model from a particular criterion [15, 16].
The updated parameters are list in Table S3. Then these calibrated parameters are applied in
the Level III model again to predicted the modeled VEPAHs concentration, which shown in Table
S4. The model results show better performance after calibrated and these updated parameters will
be adopted to use in multimedia fugacity models to predict the VEPAHs concentrations in each
compartment.

Table S3. The updated value of degradation half-life time (hfa) and depth of air (dep_a) of
VEPAHs.
VEPAHs hfa dep_a
Lower Upper Lower Upper
Default Updated Default Updated
limit limit limit limit
FLU 19.7 6.5 59.1 11.02 500 10 1000 869.8
PHE 20 6.7 60 6.67 500 10 1000 942.8
ANT 6 2 18 2.40 500 10 1000 855.3
FLA 23.3 7.8 69.9 10.61 500 10 1000 790.5
PYR 5 1.7 15 12.26 500 10 1000 290.8
BAA 5.1 1.7 15.3 6.92 500 10 1000 940.3
CHR 5 1.7 15 14.19 500 10 1000 387.3
BBF 14 4.7 42 7.51 500 10 1000 897.7
BKF 4.8 1.7 14.4 12.14 500 10 1000 104.3
B[a]P 5 1.7 15 3.81 500 10 1000 748.4
IcdP 4 1.3 12 12 500 10 1000 301.4
DBA 5.1 1.7 15.3 1.7 500 10 1000 982.2
BghiP 3 1 9 9 500 10 1000 104.4

Table S4. The standard and modeled VEPAHs concentration in air phase.

VEPAHs Standard Model 1 (default parameters) Model 2 (calibrated parameters)

FLU 1.31 2.31 1.31
PHE 9.48 6.81 9.49
ANT 0.46 3.72 0.62
FLA 3.11 7.61 3.11
PYR 1.45 0.78 1.45
BAA 2.53 3.99 2.53
CHR 0.49 0.58 0.49
BBF 0.42 0.50 0.42
BKF 0.42 0.07 0.42
B[a]P 0.58 1.10 0.58
IcdP 1.72 0.35 1.72
 DBA 0.20 1.24 0.21
BghiP 0.89 0.09 0.89

2. Model input
2.1 Model input for motor vehicles properties
The population of motor vehicles from 1999 to 2015 is listed in Table S5 (Zhengzhou
Statistical Yearbook, 1999-2015), as is the annual mileage of the different types of vehicles. Table
S6 shows the emission factors of VEPAHs discharged from different fuel-driven vehicles types –
diesel and gasoline vehicles [17]. There are approximately 90% of heavy duty vehicles (HDVs)
and 5% of light duty vehicles (LDVs) are diesel-driven and the remaining are gasoline vehicles
[18-20].

Table S5. The motor vehicles populations during 1999 to 2015 of Zhengzhou city and the annual
mileage of different type of vehicles (Zhengzhou Statistic Yearbooks).
Classification Light duty Heavy duty
Private Commercial Freight Coach/ Freight
Year\Type Total
cars cars cars bus cars
1999 76,808 10,737 15,331 4,283 30,514 137,673

2000 93,720 10,671 16956 4,548 31,918 157,813

2001 106,826 a 10,660 18,246 a 5,006 a 34,624 a 175,362

2002 119,931 10,764 19,536 5,463 37,330 193,024

2003 113,612 10,757 49,019 14,140 39,549 227,077

2004 132,900 10,757 49,882 15,151 40,881 249,571

2005 171,026 10,757 40,588 12,885 30,252 265,508

2006 200,770 10,851 40,697 14,798 31,973 299,089

2007 259,979 10,865 45,682 16,456 33,939 366,921

2008 331,239 10,862 44,558 18,006 36,819 441,484

2009 415,819 10,859 45,626 19,892 40,390 532,586

2010 545,791 10,607 53,785 21,113 47,347 678,643

2011 726,138 10,607 62,912 22,705 55,097 877,459

 2012 939,235 10,607 93,764 26,272 62,725 1,132,603
2013 1,181,393 10,607 105,000 29,000 69,000 1,395,000

2014 1,474,455 10,608 117,579 30,920 72,595 1,706,157

2015 1,851,756 10,608 125,028 32,711 67,709 2,087,812

Annual mileage
33,700 90,900 379,00 65,000 75,000 \
(km)
a
The data is estimated by the average value of vehicle population in 2000 and 2002.

Table S6. On-road emission factors of particle-phase PAHs with different types of vehicles [Ho
et al., 2009]

Emission factor (μg/km)

VEPAHs Abbr.
Diesel vehicles Gasoline vehicles
Naphthalene NAP 613.4 261.0
Acenaphthylene ACY 584.2 46.3
Acenaphthene ACE 1479.1 196.7
Fluorene FLU 105.3 16.4
Phenanthrene PHE 153.2 6.3
Anthracene ANT 22.5 1.9
Fluoranthene FLA 50.7 2.1
Pyrene PYR 60.5 2
Benz[a]anthracene BAA 10.8 1.3
Chrysene CHR 18.3 1.6
Benzo[b]fluoranthene BBF 0.7 5.9
Benzo[k]fluoranthene BKF 0.3 2.4
Benzo[a]pyrene BAP 2.9 1.4
Indeno[1,2,3-cd]pyrene IcdP 1 1
Dibenzo[a,h]anthracene DBA 0.4 0.4
Benzo[g,h,i]perylene BghiP 1.1 6.3
 0.12

0.11 Data
Fitted model
0.1

0.09

Emission rate (kg/h)

0.08

0.07

0.06

0.05

0.04

0.03

0.02
0 5 10 15
t (h) 4
x 10

Figure S1 The reported data and fitted curve of time-trend BAP emission rate based on fourth
order polynomial function.

2.2 Model input for chemical properties

Table S7. Physical-chemical properties and half-lives of VEPAHs.
Melting Water Vapor Log
VEPAHs Rings CAS# MW
point solubility pressure Kow
Degradation Half-lives (h)
(g/m) (℃) (g/m3) (Pa) Air Water Soil Sediment
NAP 2 91-20-3 128.2 80 2.65E+01 7.94E+00 3.36 11.9 900 1800 8100
ACY 3 208-96-8 152.2 93 1.47E+01 5.90E-01 4.01 1 360 720 3240
ACE 3 83-32-9 154.2 93 3.30E+00 1.89E-01 3.99 4.4 900 1800 8100
FLU 3 86-73-7 166.2 115 1.44E+00 4.97E-02 4.11 19.7 360 720 3240
PHE 3 85-01-8 178.2 99 1.00E+00 1.05E-02 4.53 20 1440 2880 13000
ANT 3 120-12-7 178.2 215 3.43E-02 5.68E-04 4.52 6 1440 2880 13000
FLA 4 206-44-0 202.3 108 2.23E-01 7.14E-04 5.23 23.3 1440 2880 13000
PYR 4 129-00-0 202.3 151 1.17E-01 3.50E-04 4.95 5 1440 2880 13000
BAA 4 56-55-3 228.3 84 7.89E-03 1.64E-05 5.86 5.1 1440 2880 13000
CHR 4 218-01-9 228.3 258 1.61E-03 4.71E-07 5.89 5 1440 2880 13000
BBF 5 205-99-2 252.3 168 1.22E-03 3.77E-05 5.88 14 1440 2880 13000
BKF 5 207-08-9 252.3 217 6.38E-04 7.28E-08 6.21 4.8 1440 2880 13000
a a a a
BAP 5 50-32-8 252.3 175 3.8E-03 7E-07 6.04 5 1440 2880 13000
IcdP 6 193-39-5 276.3 164 1.47E-04 9.13E-09 6.8 4 1440 2880 13000
DBA 5 53-70-3 278.4 270 7.98E-04 6.87E-08 6.64 5.1 1440 2880 13000
BghiP 6 191-24-2 276.3 278 2.26E-04 7.16E-09 6.73 3 1440 2880 13000
a
Reference [2]; Others refer from [10].
2.3 Model input for ILCR model
The parameters used to evaluate the human health risks of VEPAHs are listed in Table S8. The
cancer slope factors are only available for BaP; thus, toxic equivalency factors (TEFs) are used to
estimate the cancer slope factors of the other PAHs based on that of BaP [21] (shown in Table S9).

Table S8. The parameters of ILCR model [3].

Exposure routes Parameters Symbol Units Values

Inhalation Inhalation rate IRi m3/day 12.44
Cancer slope factor of inhalation SFi (mg/kg/day) –1 3.9
Ingestion Intake rate of water IRw mL/day 1366
Intake rate of fish IRf mg/day 61.25
Intake rate of soil IRs mg/day 25
BaP cancer slope factor of ingestion SFo (mg/kg/day) –1 7.3
Dermal contact Total skin surface area At m2 1.67
Dermal permeability coefficient Kp cm/h 0.7
Show time t min/day 10.4
Dermal exposure time ta hour 24
Exposed skin surface area As cm2 1530
Adherence factor of soil ADF mg/cm2-day 0.49
Absorption factor of dermal ABF \ 0.13
BaP cancer slope factor of dermal
SFd (mg/kg/day) –1 25
contact
Population
Body weight BW kg 58.7
characters
Average time AT days 25550
Exposure frequency EF days/year 345
Exposure duration ED years 70

Table S9. Toxic equivalency factors (TEFs) of VEPAHs [21].

VEPAHs TEFs VEPAHs TEFs

NAP 0.001 BAA 0.1
 ACY 0.001 CHR 0.01
ACE 0.001 BBF 0.1
FLU 0.001 BKF 0.1
PHE 0.001 B[a]P 1
ANT 0.001 IcdP 0.1
FLA 0.001 DBA 5
PYR 0.001 BghiP 0.01

2.4 Model input for sensitivity analysis

The sensitivity of the important chemical properties parameters (including Henry’s law
constant, the octanol-water partition coefficient, the chemical degradation half-life in the four
phases, and the cancer slope factors [8, 9, 22]) to the Level III–ILCR model are implemented in
this study, and the rank correlation coefficient is used to assess the uncertainty between the input
parameters and output results. The default value of input chemical properties parameters the
correlated dispersion factors of these parameters are listed in Tables S10.

Table S10. Specific parameters of chemical BAP.

Assumed Interval of 95% of all sample value
Parameters Mean confidence
factor, k Min (2.5%) Max (97.5%)
Vapor Pressure 7 10 −7 a 1.5 4.67 10 −7 1.05 10−6
Solubility 3.8 10−3 a 1.5 2.53 10−3 5.70 10−3
Log Kow 6.04 a
2 4.80 12.10
Half-life in air 3.8 b 3 2.16 19.40
Half-life in water 1440 b 3 480 4320
Half-life in soil 2880 b 3 960 8640
Half-life in sediment 13000 b 3 4333 39000
SF of inhalation 3.9 c 2 1.95 7.8
SF of ingestion 7.3 c 2 3.15 14.6
SF of dermal contact 25 c 2 12.5 50
a b c
Reference [2]; Reference [10]; Reference [3];
2.5 Model input for environmental properties
Table S11. Environmental compartment parameters of Zhengzhou downtown area.

Area (km2) a Depth (m) b Volume (m3)

Air 1010.3 1000 1.01×109
Water 11.4 20 2.28×108
Soil 662.8 0.2 132.52×108
Sediment 11.4 0.05 0.57×108
Build up area 336.1 \ \
a b
Reference [23]; Reference [2].

2.6 Model input for measured mortality rate of pulmonary diseases

Table S12. The mortality rate of respiratory diseases and lung cancer.
Estimated VEPAHs Respiratory diseases Lung cancer
Year Concentration in air mortality rate mortality rate
phase (ng/m3) (/100,000) (1/100,000)
1999 0.57 - 18.88[j, k]
2000 0.76 27.35 [a] 20.92[j, k]
2001 0.86 - 22.25[j, k]
2002 0.91 21.44[b] 21.55[j, k]
2003 0.93 25.97[c] 21.58[j, k]
2004 0.95 - 21.23[j, k]
2005 0.96 41.53[d] 22.70[j, k]
2006 1.00 - 23.30[j, k]
2007 1.08 48.25[e] 22.35[j, k]
2008 1.19 48.25[e] 22.88[j, k]
2009 1.34 48.25[e] 23.48[j, k]
2010 1.54 48.11[f] 25.18[j, k]
2011 1.78 41.65[g] 24.49[j, k]
2012 2.05 47.27[h] 24.68[l]
2013 2.34 - 23.78[l]
 2014 2.65 48.74[i] 24.10[l]
2015 2.96 -

[a]
Reference [26]; [b] Reference [27]; [c] Reference [28]; [d] Reference [29]; [e] Reference [30]; [f]
Reference [31]; [g] Reference [32]; [h] Reference [33]; [i] Reference [34]; [j] Reference [35]; [k]
Reference [30]; [l] Reference [36].
 (a)

(b) (c)

Figure S2. (a) Satellite-derived annual average surface-level PM2.5 concentration (μg/m3) of
China in 2008 (NASA); (b) vehicle population per unit area (/km2) of china in 2008 (Chinese
Statistic Yearbook, 2009); and (c) estimated lung cancer mortality rate (per 100,000) base on
province in China 2008 [24].
3. Results

Figure S3. BaP concentration attributions in each compartment of air, water, soil and sediment
(bar chart) with the VEPs concentration proportion (pie graphs).
 (a) (b)

(c) (d)

Figure S4. Sensitivity results of BaP posed health risk against the input parameters through
different exposure routes, including (a) total risk (b) dermal contact (c) inhalation and (d)
ingestion.
 6
10
Air
Water
5
10 Soil
Sediment

4
10
Concentration (ng/m3)

3
10

2
10

1
10

0
10

-1
10
1998 2000 2002 2004 2006 2008 2010 2012 2014 2016
t (year)

(a)

-5
10
Limit line
Total risk
Dermal contact
Inhalation
-6
10 Ingestion
Incremental lifetime cancer risk

-7
10

-8
10

-9
10
1998 2000 2002 2004 2006 2008 2010 2012
t (year)

(b)
Figure S5. (a) Total BaP equivalent concentration and (b) the estimated ILCR of the VEPAHs in
Zhengzhou city during 17 years.
Figure S6. The respiratory diseases and lung cancer mortality rate and the estimated air phase
VEPAHs concentration from 1999 to 2015.
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