Carcinogenic and non-carcinogenic risks from PM10-and PM2.5-Bound metals in a critically polluted coal mining area

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Carcinogenic and non-carcinogenic risks from PM10-and PM2.5-Bound metals in a critically polluted coal mining area

T

Debananda Roya, Gurdeep Singhb, Yong-Chil Seoa,∗ a b

Department of Environmental Engineering, Yonsei University, Wonju, Republic of Korea Department of Environmental Science and Engineering, Indian Institute of Technology (ISM), Dhanbad, India

A R T I C LE I N FO

A B S T R A C T

Keywords: Particulate matter Trace metals Non-cancer risk Cancer risks Coal mining

This study analyzed the carcinogenic and non-carcinogenic risks of PM10-and PM2.5-bound trace metals, using exposure pathways, in a critically polluted coal mining area, the Jharia coalfield (JCF), India. The human health risks were calculated via ingestion (ing), inhalation (inh), and dermal (derm) absorption in adults and children. The cancer risks (CR) were evaluated as Total CR, CRinh, CRing, and CRderm, and the non-cancer risks as the hazard quotient (HQ) and hazard index (HI). The obtained CR levels were verified using the incremental lifetime cancer risk for inhalation exposure and Monte Carlo simulations for all exposure pathways. The HQinh and HI were found to be significant (> 1) for both PM10 and PM2.5 at all 18 monitoring stations that were selected for this study. The Total CR for PM10 was estimated to be maximum in the city near the mine-fire area (3.67 × 10−2), followed by the mine-fire area (2.26 × 10−2), while that for PM2.5 was highest at the core mining area (1.06 × 10−2), followed by the city adjacent to the mine-fire area (8.85 × 10−3). The Total CR and CR for all individual exposures were not only found to be significant (> 10−6), but also exceeded the acceptable CR levels (1.00 × 10−6- 1.00 × 10−4). Consequently, the study area fell in the high (10−3≤ to < 10−1) and moderate (10−4≤ to < 10−3) risk categories for PM10 and PM2.5, respectively. Finally, Cd, Cr(VI), and Pb, which are signature elements of coal and oil combustions, were identified as significant contributors to the CR levels in JCF.

1. Introduction Atmospheric pollution levels with respect to (w.r.t) particulatebound trace elements is an important aspect of global health issues, given their toxicity and adverse health impacts (Chithra and Nagendra, 2013; IARC, 1982; Landrigan et al., 2017; WHO, 2016). High exposure to particulate matter (PM) is known to cause several diseases, such as abnormal heartbeat, pulse rate, and pulmonary lung functions, lung capacity reduction, chronic and acute respiratory illnesses, chronic obstructive pulmonary diseases, lung cancer, and cardiovascular diseases (Dockery and Pope, 1994; Mate et al., 2010; Pope et al., 2002; Ranjan et al., 2016; Roy et al., 2019; Wallenborn et al., 2009; WHO, 2003). Globally, exposure of ambient PM2.5 accounted for 2.9 million deaths (State of Global air, 2019). Straif et al. (2013) reported that worldwide, approximately 223,000 deaths have occurred due to air pollution related lung cancer. Hence, The International Agency for Research on Cancer (IARC) classified atmospheric pollutants as major carcinogens (IARC, 2013).

In India, the Jharia coalfield (JCF) is one of the prominent coking coal producing areas. Open cast coal mining and its associated activities are primary contributors of particulate pollution in coal mining complexes (Ghose, 2002; Roy et al., 2015, 2016). A PM10 source apportionment study reported that apart from coal mining activities the other multiple pollution sources such as vehicle exhaust emissions, open coalburning and mine fires, garbage burning, and diesel generator (DG) set emissions sources made Jharia and Dhanbad city more critical polluted area in the country (Roy et al., 2016). The adverse health impacts from exposure to PM in this critically polluted area have eventually become a matter of great concern. Roy et al. (2017) indicated significant inhalation cancer risk due to the presence of PM10-bound polycyclic aromatic hydrocarbons (PAHs). Similarly, Jana and Singh (2017) reported higher cancer risk (CR) levels from inhalation exposure to PM10bound trace metals, while Tarafdar et al. (2018) reported significant carcinogenicity associated with roadside soil-bound PAHs in Indian mining areas. However, to date, there is a complete lack of significantly detailed reports on cancer and non-cancer risks from PM2.5-bound

Peer review under responsibility of Turkish National Committee for Air Pollution Research and Control. ∗ Corresponding author. Dept. of Environmental Engineering, Yonsei University, Wonju, 220-710, Republic of Korea. E-mail address: [email protected] (Y.-C. Seo). https://doi.org/10.1016/j.apr.2019.09.002 Received 20 May 2019; Received in revised form 23 August 2019; Accepted 4 September 2019 Available online 09 September 2019 1309-1042/ © 2019 Turkish National Committee for Air Pollution Research and Control. Production and hosting by Elsevier B.V. All rights reserved.

Atmospheric Pollution Research 10 (2019) 1964–1975

D. Roy, et al.

papers. The concentrations of selected trace metals were determined using inductively coupled plasma optical emission spectrometry (PerkinElmer® Optima™ 7300 DV ICP-OES equipped with WinLab 32™ for ICP Version 4.0 software for simultaneous measurement of all wavelengths of interest). Calibration of the instrument was carried out using ICP-OES standard solution from E-Merck (Germany). The detailed ambient air monitoring, extraction methods, chemical species analysis, instrumental conditions, and QA/QC have been provided in supplementary information part 3 and in the previous study (Roy et al., 2016; Jena and Singh, 2017).

metals in a critically polluted coalmining complex. The current study is the first attempt to simulate, compare, and verify the non-cancer and cancer risks for both PM10-and PM2.5-bound trace metals in one such Indian coalmining complex, the JCF. Hence, this study, 1) assessed the air quality in JCF for PM10 and PM2.5, 2) investigated the particulatebound trace metals for non-cancer and cancer risks through exposure pathways, 3) estimated the human health risk levels in different zones (mining area near the thermal power station, core mining area, mine fire-affected and mining area, and the urban area) and within different age groups, 4) the CR levels were verified the by ILCR and Monte Carlo analysis.

2.4. Health risk assessment 2. Materials and methods The human health risks of PM-bound trace metals were calculated using exposure pathway models (Jena and Singh, 2017; Wu et al., 2011). The United States Environmental Protection Agency (USEPA) developed the tool for carcinogenic and non-carcinogenic risks of toxic substances present in the environment. This study adopted the following assumptions: 1) the residents of the sampling locations were potentially exposed; 2) the target population comprised of children (aged 12 years) and adults (aged 70 years); 3) three possible human exposure pathways - dermal absorption, inhalation, and ingestion; and 4) CR calculated as 24 h/day atmospheric exposure for 350 days/year (Hoseini et al., 2015; Jana and Singh, 2017; Megido et al., 2017). The concentration of Cr(VI) was calculated as oneseventh of the concentration of the total Cr according to the USEPA model (Izhar et al., 2016; Massey et al., 2013).

2.1. Study area The JCF, located in the state of Jharkhand, is one of India's chief coalfields, containing significant reserves of coking coal (CMPDIL, 1988). Situated in the center of Damodar valley between 23°38′and 23°48′N and 86°11′, 86°27′E, it covers an area of over 460 km2. Eighteen monitoring stations (A1–A18) in Dhanbad and JCF were considered for this study, which were then subdivided into four zones to acquire a better understanding of the most probable pollution sources and their impacts. Zone ZMP (ZMP: A1–A4) represented the mining area near the thermal power station, Zone ZM (ZM: A5, A7–A10, and A17) the core mining area, Zone ZMF (ZMF: A6, A11, and A12) the mining and mine fire-affected area, and Zone ZC (ZC: A13–A16) represented the urban area. A18 was used as a reference station (R). Details about the monitoring stations and sources were provided in a previous study by Roy et al. (2016). The study area location is shown in Supplementary Figure SF1.

2.4.1. Human exposure pathways The daily intake in terms of ingestion (CDIing), dermal absorption dose (DADderm), and exposure through inhalation (ECinh) were calculated for each PM-bound trace metal using the following equations (USEPA, 1989, 2004, 2009).

2.2. Sampling protocols, sample collection, and estimation of particulate matters

CDIing = Air quality monitoring w.r.t. PM10 and PM2.5 were performed twice a week, at the 18 stations throughout the study area over a period of one year (March 2011 to February 2012). The total 104 samples for each PM10 and PM2.5 were collected using a respirable dust sampler (RDS) (Envirotech APM 460) and a fine dust sampler (Envirotech APM 550 MFC), respectively. Sampling for both types of PM was conducted for 24 h for all monitoring stations. The RDSs were operated at an average flow rate of 1.1–1.2 m3/min according to IS: 5182 PART 4 (Bureau of Indian Standards, 1999), and the fine dust samplers at an average flow rate of 1.67 L/min. The PM10 and PM2.5 concentrations were computed using standard methods after weighing the EPM 2000 and polytetrafluoroethylene (PTFE) filter papers, respectively. Each filter paper was weighed gravimetrically pre- and post-sampling using an electronic balance (Denver Instruments Model TB-215D) to measure their weight differences. Detailed descriptions of the sampling protocols, sample collection, and estimation of particulate matters have been reported in a previous study (Roy et al., 2015, 2016, 2017).

C × IngR EF × ED × × CF BW AT

DADderm =

C × SA × AF × ABS × EF × ED × CF BW × AT

ECinh = C × ET ×

EF × ED AT

(1) (2) (3)

where C is the 95% upper confidence limit (UCL) of the mean metals in PM10 and PM2.5 at exposure point concentration; IngR, ingestion rate (Hu et al., 2012; Keshavarzi et al., 2015; Shi et al., 2011; Sun et al., 2014; USEPA, 1989); BW, average body weight; ED, exposure duration; EF, exposure frequency; AT, averaging time; CF, conversion factor; SA, surface area of the skin in contact with air (Izhar et al., 2016; Keshavarzi et al., 2015); AF, skin adherence factor for air-borne particulates (USEPA, 2004); ABS, dermal absorption factor (ABS values of 0.03, 0.001, and 0.01 were used for As, Cd, and other trace metals, respectively (USEPA, 2016)); and ET, exposure time. The model parameter values were adopted from the Risk Assessment Guidance of the USEPA (1989) to characterize the cancer and non-cancer risks for children and adults in the study area (see Supplementary Table ST1) (Chen et al., 2012; Chen and Liao, 2006; Islam et al., 2018; Jang et al., 2007; USEPA, 1997, 2002, 2004, 2011).

2.3. Determination of trace metal fractions The PM10 and PM2.5 samples were analyzed for their trace elements characteristics using a chemical method. The EPM 2000 and PTFE filters were cut into four pieces after their gravimetric analysis; one-fourth of the filter paper was used to determine the trace elements. This piece was digested in a mixture of nitric acid (65% GR grade, Merck) and perchloric acid (70% GR grade, Merck) (20:2, v/v), over hot plate heating (at approximately 150 °C) to evaporate the nitric acid solution to 5 ml (method IO-3.1; USEPA, 1999). The digested solution was then filtered through a Whatman 42 filter paper, diluted to 50 ml with double distilled water, and refrigerated in a clean polypropylene bottle for further analysis. The same procedure was repeated for blank filter

2.4.2. Risk characterization 2.4.2.1. Non-cancer risks. The non-cancer risks for PM-bound trace metals were evaluated using the hazard quotient (HQ) and hazard index (HI) (USEPA, 1989, 2004, 2009). As HQ and HI value greater than one indicates probable non-cancer risks. The higher level of noncancer risks depends on the HQ and HI values (USEPA, 1989). In addition, the sums of all HQ and HI were calculated to estimate the total health risks due to exposure to multiple elements (USEPA, 2009). The non-cancer risks due to ingestion, dermal contact, and inhalation were 1965

1966

A1 A2 A3 A4

A5 A7 A8 A9 A10 A17

A6 A11 A12

A13 A14 A15 A16

A18

Location Code

A1 A2 A3 A4

A5 A7 A8 A9 A10 A17

A6 A11 A12

A13 A14 A15 A16

A18

ZMP

ZM

ZMF

ZC

R

Zone

ZMP

ZM

ZMF

ZC

R

± ± ± ± ± ±

0.240 0.003 0.160 0.002 0.060 0.002

0.002 0.003 0.004 0.230

± ± ± ±

0.020 0.310 0.260 0.110

± ± ± ± ± ±

± ± ± ± 0.005 0.047 0.001 0.029 0.001 0.029

0.002 0.002 0.004 0.003

± ± ± ±

0.020 0.040 0.002 0.010

± ± ± ± ± ±

0.014 0.003 0.016 0.002 0.006 0.002

0.002 0.003 0.004 0.002

± ± ± ±

0.020 0.003 0.003 0.011

0.018 ± 0.003

0.158 0.027 0.035 0.274

0.034 ± 0.002 0.240 ± 0.011 0.035 ± 0.003

0.040 0.018 0.096 0.047 0.044 0.124

± ± ± ± ± ± ± ± ± ±

± ± ± ± 0.005 0.005 0.001 0.029 0.001 0.009

0.002 0.002 0.004 0.003

± ± ± ±

0.020 0.004 0.002 0.010

0.014 ± 0.001

0.043 0.035 0.036 0.043

0.058 ± 0.010 0.045 ± 0.002 0.026 ± 0.002

0.064 0.015 0.065 0.062 0.044 0.033

0.057 0.059 0.064 0.035

Mean ± Stdev

Mean ± Stdev

0.030 0.110 0.052 0.047

Ni

0.023 ± 0.001

0.181 0.072 0.054 0.081

0.068 ± 0.103 0.085 ± 0.002 0.054 ± 0.002

0.094 0.056 0.083 0.077 0.078 0.077

0.064 0.064 0.077 0.092

Pb

0.026 ± 0.310

0.680 0.890 0.722 0.791

0.166 ± 0.002 0.860 ± 0.110 0.193 ± 0.030

0.622 0.125 0.509 0.466 0.400 0.766

± ± ± ±

Mean ± Stdev

Mean ± Stdev

0.056 0.325 0.329 0.621

Ni

Pb

± ± ± ± ± ±

0.28 0.25 0.06 0.15 0.12 0.15

± ± ± ±

0.23 0.31 0.22 0.17

± ± ± ± ± ±

± ± ± ± 0.028 0.015 0.020 0.015 0.012 0.145

0.015 0.025 0.087 0.040

± ± ± ±

0.230 0.310 0.020 0.170

0.043 ± 0.021

0.869 0.702 0.366 1.113

0.081 ± 0.015 0.363 ± 0.020 0.062 ± 0.027

0.110 0.051 0.091 0.175 0.056 0.515

0.080 0.173 0.122 0.089

Mean ± Stdev

Cu

0.580 ± 0.210

2.22 2.22 2.36 6.32

2.98 ± 0.15 3.11 ± 0.02 1.58 ± 0.27

2.98 1.54 1.68 1.97 1.96 2.97

0.967 ± 0.145 1.24 ± 0.25 0.685 ± 0.868 0.992 ± 0.040

Mean ± Stdev

Cu

± ± ± ± ± ±

± ± ± ± 0.023 0.004 0.050 0.030 0.010 0.030

0.008 0.002 0.002 0.011

± ± ± ±

0.030 0.030 0.005 0.040 0.043 ± 0.070

0.204 0.081 0.039 0.086

0.121 ± 0.006 0.637 ± 0.260 0.043 ± 0.010

0.281 0.031 0.417 0.170 0.091 0.075

0.121 0.193 0.193 0.141

Mean ± Stdev

Mn

0.234 ± 0.070

0.213 ± 0.030 0.223 ± 0.003 1.21 ± 0.05 1.49 ± 0.04

0.590 ± 0.006 1.64 ± 0.26 0.255 ± 0.010

1.29 ± 0.23 0.083 ± 0.004 0.770 ± 0.050 0.856 ± 0.298 0.219 ± 0.080 1.36 ± 0.30

0.260 ± 0.008 0.550 ± 0.002 0.394 ± 0.002 1.61 ± 0.11

Mean ± Stdev

Mn

± ± ± ± ± ±

± ± ± ± 0.1 0.1 0.3 0.01 0.25 0.1

0.01 0.1 0.1 0.1

± ± ± ±

0.32 0.34 0.21 0.5

± ± ± ± ± ±

± ± ± ± 0.11 0.01 0.27 0.01 0.25 0.01

0.01 0.01 0.1 0.11

1.18 ± 0.09

4.61 ± 0.32 3.31 ± 0.34 3.80 ± 0.21 11.25 ± 0.45

2.19 ± 0.01 3.10 ± 0.25 3.80 ± 0.23

9.67 1.17 7.13 1.09 2.91 4.02

2.19 7.83 10.1 3.35

Mean ± Stdev

Fe

4.66 ± 0.09

5.78 5.67 5.69 32.5

2.35 ± 0.01 28.4 ± 0.3 8.34 ± 0.23

16.2 11.7 21.7 4.35 6.45 10.4

3.37 14.8 15.5 17.5

Mean ± Stdev

Fe

Note: N* = Number of samples exceed the limit for National Ambient Air Quality Standard (NAAQS), India.

Location Code

Zone

± ± ± ±

0.262 0.188 0.205 0.110

± ± ± ± ± ±

± ± ± ±

0.230 0.035 0.030 0.062 0.050 0.062

0.062 0.088 0.052 0.011

± ± ± ±

0.040 0.030 0.030 0.040 0.185 ± 0.030

0.531 0.225 0.242 0.630

0.309 ± 0.062 0.186 ± 0.010 0.615 ± 0.040

0.420 0.382 0.588 0.435 0.405 0.497

0.308 0.528 0.303 0.241

Mean ± Stdev

Zn

0.319 ± 0.030

0.890 ± 0.040 0.512 ± 0.030 0.659 ± 0.030 1.40 ± 0.04

0.745 ± 0.162 1.16 ± 0.01 0.849 ± 0.040

0.660 ± 0.230 0.825 ± 0.934 1.67 ± 0.03 1.45 ± 1.62 0.954 ± 0.050 1.15 ± 1.62

0.781 0.836 0.603 0.611

Mean ± Stdev

Zn

± ± ± ± ± ±

± ± ± ± 0.1 0.5 0.4 0.2 0.30 2.4

0.1 0.20 0.2 0.30

± ± ± ±

0.20 0.30 0.10 2.4

± ± ± ± ± ±

± ± ± ±

0.10 0.50 0.40 0.21 0.30 0.39

0.11 0.20 0.20 0.30

± ± ± ±

0.20 0.31 0.10 2.39 0.758 ± 0.010

3.66 3.16 3.52 3.28

3.17 ± 0.16 2.60 ± 0.20 3.60 ± 0.10

4.96 2.17 4.58 4.79 2.66 2.46

2.17 7.16 3.84 3.26

Mean ± Stdev

Al

4.10 ± 2.01

6.33 4.12 6.33 18.8

14.7 ± 0.2 10.2 ± 0.2 6.74 ± 0.10

15.6 15.7 12.2 14.5 5.36 16.8

12.7 8.53 10.2 8.83

Mean ± Stdev

Al

Table 1 Results of PM10 and PM2.5-bound elemental concentration levels (μg/m3) throughout the study area (number of samples n = 104).

± ± ± ±

0.010 0.010 0.010 0.050

± ± ± ±

0.01 0.01 0.01 0.1

± ± ± ± ± ±

± ± ± ±

0.006 0.004 0.005 0.004 0.006 0.006

0.001 0.010 0.001 0.005

± ± ± ±

0.010 0.003 0.010 0.010 0.013 ± 0.001

0.039 0.013 0.065 0.401

0.014 ± 0.001 0.015 ± 0.001 0.013 ± 0.001

0.065 0.026 0.065 0.026 0.014 0.055

0.013 0.078 0.026 0.023

Mean ± Stdev

Cd

0.022 ± 0.010

1.10 3.05 1.40 13.4

0.456 ± 0.010 6.049 ± 0.010 0.078 ± 0.010

0.608 ± 0.060 0.649 ± 0.040 0.304 ± 0.050 0.488 ± 0.040 0.206 ± 0.060 6.75 ± 1.62

0.078 0.731 0.361 0.063

Mean ± Stdev

Cd

± ± ± ± ± ±

± ± ± ± 0.002 0.040 0.060 0.040 0.003 0.040

0.040 0.040 0.040 0.090

± ± ± ±

0.001 0.003 0.005 0.001

± ± ± ±

0.004 0.040 0.040 0.090

± ± ± ±

0.000 0.003 0.005 0.001 0.019 ± 0.001

0.044 0.102 0.017 0.099

0.036 ± 0.004 0.122 ± 0.040 0.022 ± 0.003

0.248 ± 0.002 0.018 ± 0.004 0.276 ± 0.060 1.03 ± 0.04 0.096 ± 0.003 0.096 ± 0.040

0.036 0.093 0.384 0.109

Mean ± Stdev

Cr

0.125 ± 0.001

0.239 0.218 0.226 0.213

0.301 ± 0.040 0.399 ± 0.040 0.395 ± 0.003

0.376 0.314 0.376 0.309 0.320 0.315

0.299 0.319 0.284 0.394

Mean ± Stdev

Cr

164 ± 14 80.0 ± 12.2 140 ± 14 90.0 ± 9.1 189 ± 19 121 ± 18 126 ± 15 150 ± 17 118 ± 12 110 119 198 191

41.0 ± 9.6

– – – – – – – – – – – – – –

8 17 19 23

166 ± 12 133 ± 14 192 ± 18 93.0 ± 9.8

– – – –

± ± ± ±

Mean ± Stdev

PM2.5 Mean

As

76.6 ± 8.5

17 21 32 26 –

± ± ± ±

165 355 440 441

0.001 – – –

366 ± 16 353 ± 17 355 ± 16

21 14 17 11 26 20 – – –

± ± ± ± ± ±

480 175 362 203 452 358

0.001 0.001 0.001 – 0.001 –

11 15 20 13

383 243 530 269

– 0.001 – 0.001 ± ± ± ±

Mean ± Stdev

PM10

Mean

As

31

100 100 100 100

100 100 100

100 96 100 100 100 100

100 100 100 100

In %

N*

81

95 100 100 100

100 100 100

100 94 100 100 100 100

100 100 100 100

in %

N*

D. Roy, et al.

Atmospheric Pollution Research 10 (2019) 1964–1975

Atmospheric Pollution Research 10 (2019) 1964–1975

D. Roy, et al.

Table 2 Results of non-cancer risks as hazard quotient (HQ) and hazard index (HI) for PM10 and PM2.5-bound elements via inhalation (inh), ingestion (ing), and dermal absorption (derm) for children and adults in the study. Zones

Locations

ZMP

A1 A2 A3 A4

ZM

A5 A7 A8 A9 A10 A17

ZMF

A6 A11 A12

ZC

A13 A14 A15 A16

R

A18

PM10

PM2.5

Age Groups

HQinh

HQing

HQderm

HI

HQinh

HQing

HQderm

HI

Children Adult Children Adult Children Adult Children Adult

5.23 × 100 5.26 × 100 1.15 × 10+1 1.15 × 10+1 8.13 × 100 8.15 × 100 3.17 × 100 3.17 × 10+1

1.10 × 100 2.54 × 10−1 1.23 × 10+1 2.47 × 100 3.19 × 100 6.44 × 10−1 3.94 × 100 8.21 × 10−1

2.62 × 10−1 1.41 × 10−1 1.15 × 100 6.11 × 10−1 3.32 × 10−1 1.77 × 10−1 5.09 × 10−1 2.73 × 10−1

6.60 × 100 5.65 × 100 2.49 × 10+1 1.46 × 10+1 1.17 × 10+1 8.97 × 100 3.62 × 10+1 3.28 × 10+1

2.42 × 100 2.42 × 100 3.87 × 100 3.87 × 100 3.90 × 100 3.91 × 100 2.84 × 100 2.84 × 100

6.56 × 10−1 1.35 × 10−1 3.20 × 100 6.41 × 10−01 1.19 × 100 2.42 × 10−1 1.76 × 100 3.58 × 10−1

1.84 × 10−1 9.78 × 10−2 3.84 × 10−1 2.05 × 10−1 5.47 × 10−1 2.91 × 10−1 4.27 × 10−1 2.27 × 10−1

3.26 × 100 2.66 × 100 7.45 × 100 4.72 × 100 5.64 × 100 4.44 × 100 5.03 × 100 3.42 × 100

Children Adult Children Adult Children Adult Children Adult Children Adult Children Adult

2.60 × 10+1 2.60 × 10+1 1.70 × 100 1.74 × 100 1.53 × 10+1 1.53 × 10+1 1.83 × 10+1 1.83 × 10+1 4.96 × 100 5.00 × 100 3.42 × 10+1 3.43 × 10+1

3.22 × 100 7.22 × 10−1 2.24 × 100 5.74 × 10−1 3.65 × 100 7.80 × 10−1 1.14 × 10+1 2.37 × 100 2.81 × 100 6.13 × 10−1 7.14 × 10+1 1.40 × 10+1

5.04 × 10−1 2.72 × 10−1 1.89 × 10−1 1.07 × 10−1 6.52 × 10−1 3.49 × 10−1 1.08 × 100 5.80 × 10−1 3.24 × 10−1 1.75 × 10−1 5.37 × 100 2.85 × 100

2.97 × 10+1 2.70 × 10+1 4.14 × 100 2.42 × 100 1.96 × 10+1 1.65 × 10+1 3.08 × 10+1 2.12 × 10+1 8.09 × 100 5.79 × 100 1.11 × 10+1 5.11 × 10+1

5.65 × 100 5.65 × 100 6.54 × 10−1 6.55 × 10−1 8.38 × 100 8.39 × 100 3.78 × 100 3.78 × 100 1.86 × 100 1.86 × 100 1.68 × 100 1.69 × 100

2.06 × 100 4.11 × 10−1 1.54 × 100 3.09 × 10−1 2.89 × 100 5.70 × 10−1 3.71 × 100 7.49 × 10−1 6.73 × 10−1 1.35 × 10−1 2.89 × 100 6.28 × 10−1

4.98 × 10−1 2.64 × 10−1 1.62 × 10−1 8.66 × 10−2 6.56 × 10−1 3.48 × 10−1 2.86 × 100 1.52 × 100 1.64 × 10−1 8.73 × 10−2 3.59 × 10−1 1.94 × 10−1

8.21 × 100 6.33 × 100 2.36 × 100 1.05 × 100 1.19 × 10+1 9.31 × 100 1.03 × 10+1 6.05 × 100 2.70 × 100 2.08 × 100 4.92 × 100 2.51 × 100

Children Adult Children Adult Children Adult

1.20 × 10+1 1.20 × 10+1 3.86 × 10+1 3.87 × 10+1 5.22 × 100 5.25 × 100

5.16 × 100 1.13 × 100 6.30 × 10+1 1.24 × 10+1 1.64 × 100 3.90 × 10−1

5.55 × 10−1 3.01 × 10−1 4.78 × 100 2.54 × 100 3.47 × 10−1 1.88 × 10−1

1.77 × 10+1 1.35 × 10+1 1.06 × 10+2 5.36 × 10+1 7.21 × 100 5.83 × 100

2.40 × 100 2.40 × 100 1.33 × 10+1 1.33 × 10+1 9.00 × 10−1 9.02 × 10−1

8.49 × 10−1 1.75 × 10−1 2.28 × 100 4.80 × 10−1 8.31 × 10−1 1.70 × 10−1

1.41 × 10−1 7.54 × 10−2 2.85 × 10−1 1.53 × 10−1 9.87 × 10−2 5.28 × 10−2

3.39 × 100 2.65 × 100 1.59 × 10+1 1.40 × 10+1 1.83 × 100 1.12 × 100

Children Adult Children Adult Children Adult Children Adult

5.58 × 100 5.63 × 100 7.68 × 100 7.73 × 100 2.51 × 10+1 2.52 × 10+1 4.19 × 10+1 4.20 × 10+1

2.79 × 10+1 5.62 × 100 3.29 × 10+1 6.48 × 100 1.31 × 10+1 2.62 × 100 1.08 × 10+2 2.12 × 10+1

2.22 × 100 1.19 × 100 2.43 × 100 1.30 × 100 9.88 × 10−1 5.28 × 10−1 8.01 × 100 4.26 × 100

3.57 × 10+1 1.24 × 10+1 4.30 × 10+1 1.55 × 10+1 3.92 × 10+1 2.83 × 10+1 1.58 × 10+2 6.75 × 10+1

4.15 × 100 4.17 × 100 1.74 × 100 1.75 × 100 8.67 × 10−1 8.75 × 10−1 2.31 × 100 2.33 × 100

3.07 × 100 7.23 × 10−1 9.04 × 10−1 2.73 × 10−1 1.44 × 100 3.08 × 10−1 8.93 × 100 1.82 × 100

2.55 × 10−1 1.42 × 10−1 2.59 × 10−1 1.42 × 10−1 1.27 × 10−1 6.88 × 10−1 7.06 × 10−1 3.79 × 10−1

7.47 × 100 5.03 × 100 2.90 × 100 2.17 × 100 2.43 × 100 1.25 × 100 1.19 × 100 4.53 × 100

Children Adult

4.84 × 100 4.86 × 100

2.70 × 100 6.47 × 10−1

5.11 × 10−1 2.77 × 10−1

8.05 × 100 5.78 × 100

1.11 × 100 1.11 × 100

1.75 × 100 3.57 × 10−1

2.22 × 10−1 1.18 × 10−1

3.08 × 100 1.59 × 100

Note: Significant (> 1) level of non-cancer risk is presented in Bold.

2.4.2.2. Cancer risks via exposure pathway. The cancer risks of PM10 and PM2.5 based on human exposure pathways were calculated for ingestion (CRing), dermal contact (CRderm), and inhalation (CRinh) using the following equations (USEPA, 1989, 2004, 2009).

estimated by the following equations (USEPA, 1989, 2004, 2009).

HQing =

CDIing RfD

HQderm =

DADderm RfD × GIABS

(4)

CRing = CDIing × SFo (5)

CRderm = HQinh =

ECinh RfCi × 1000μg / mg

(6)

where HQing, HQderm, and HQinh are the hazard quotients due to ingestion, dermal contact, and inhalation respectively; RfD, reference dose; RfCi, inhalation reference concentration; and GIABS, gastrointestinal absorption factor. The RfD and RfCi values for all metals were obtained from Megido et al. (2017) and USEPA (2016). Furthermore, HQs of all individual metals were added to calculate the HI. The HI indicates the mixed exposure to multiple elements, as determined by equation (7).

∑ HQ1 + HQ2 + ..... + HQi i=1

(9)

CRinh = IUR × ECinh

(10)

TotalCR = CRing + CRderm + CRinh

(11)

where SFo is the oral slope factor, and IUR, inhalation unit risk. The probable values of SFo, GIABS, and IUR for carcinogenic elements such as Pb, Ni, Cd, Cr(VI), and As were obtained from Hu et al. (2012), Megido et al. (2017), and USEPA (2016) as presented in Supplementary Table ST2. The lifetime cancer risks have been categorized as very low (≤10−6), low (10−6≤ to < 10−4), moderate (10−4≤ to < 10−3), high (10−3≤ to < 10−1), and very high (≥10−1) by the New York State Department of Health (NYS DOH, 2012).

n

HI =

DADderm × SFo GIABS

(8)

(7)

2.4.2.3. Incremental lifetime cancer risk. The incremental lifetime cancer risk (ILCR) was calculated using equation (12) for PM2.5- and PM10bound Cr(VI), Ni, and Pb (Sarkar and Khillare, 2011; USEPA, 2011;

where HI > 1 indicates a significant risk level (Guney et al., 2010; USEPA, 1989; Zheng et al., 2010). 1967

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Fig. 1. Comparisons between cancer risk via inhalation (CRinh) and incremental lifetime cancer risk (ILCR) at different zones including the reference station (A18: R) for children and adult groups, for PM10 and PM2.5.

this technique is used to calculate the potential health effects of multiple polluting agents (Wu et al., 2011).

Widziewicz et al., 2018).

ILCR =

∑i

Ei × EF × ED × IR × CSFi × cf BW × AT

(12) 3. Results and discussion

where EF is the exposure frequency; Ei, concentration of the ith element (μg/m3) in PM10 (at 95% UCL); CSFi, cancer slope factor for the ith element; ED, exposure duration; cf, conversion factor (10−3) (μg/mg); BW, body weight; AT, average time; and IR, inhalation rate. The EF, ED, AT, IR, and BW values are provided in Supplementary Table ST1. The CSFi values for Cr(VI), Ni, Cd, and Pb are given in Supplementary Table ST2 according to the Risk Assessment Information System (RAIS) (https://rais.ornl.gov/tox/profiles/chromium.html), Widziewicz et al. (2018), and the California Environmental Protection Agency and USEPA (CEPA, 2004; USEPA, 2000).

3.1. PM2.5 and PM10 levels Table 1 lists the mean PM10 and PM2.5 concentrations recorded at the 18 monitoring stations. The average PM10 and PM2.5 concentrations appeared in the sequence of ZMF > ZMP > ZC > ZM and ZC > ZMP > ZMF > ZM, respectively. Among the four zones, mean value of PM10 were observed maximum at ZMP (A3:531 μg/m3), followed by ZM (A5:480 μg/m3; A10: 452 μg/m3) and ZC (A16:441 μg/m3). The reference station, A18, had lower PM levels than the others locations. The stations located in the city were more polluted w.r.t fine PM (PM2.5). Roy et al. (2016) had observed that the primary factors responsible for PM2.5 pollution in this area were paved/non-paved dust and vehicular combustion. The monitoring stations located in ZMF were more polluted w.r.t PM10, while ZMP was the second highest polluted zone w.r.t. both PM10 and PM2.5. The lowest pollution level was recorded at ZM. Roy et al. (2016) had concluded that ZM was affected by industrial, vehicular, and paved/non-paved dust sources, accounting for 45%, 25%, and 15% of the PM in the zone, respectively. In India, the upper permissible limit for PM10 and PM2.5 is 60 μg/m3 and 40 μg/m3, respectively for industrial, residential, rural, and other areas, as per the national ambient air quality standard (NAAQS) (CPCB, 2009). Hence, concentration levels of all PMs exceed the NAAQ limit by 100% per each station in each zone except three stations (A7: 94%;

2.4.2.4. Monte Carlo statistical analysis. The 95% confidence levels of cancer risk were analyzed for each exposure pathway using a Monte Carlo simulation to verify the cancer risk levels. The Crystal Ball (11.1.2.4.600) software (Oracle) was used to evaluate the cancer risk level. The simulation ran for 50,000 iterations. A probability density function is assigned to each input parameter using the probabilistic uncertainty analysis technique. Selecting of random values from each of the distributions and using these selected values in the exposure equations are integral parts of the simulation. The distribution of predicted values and the sensitivity of the significant input parameters are determined through the simulation. Monte Carlo and sensitivity analysis are probabilistic approaches to estimate the stochastic properties of human exposure and uncertainty. Globally, 1968

1969

R

ZMC

ZMF

ZM

A1

ZMP

A18

A16

A15

A14

A13

A12

A11

A6

A17

A10

A9

A8

A7

A5

A4

A3

A2

Locations

Zones

C A

C A C A C A C A

C A C A C A

C A C A C A C A C A C A

C A C A C A C A

Age Groups

1.22 × 10−4 5.30 × 10−4 4.38 × 10−5 1.90 × 10−4 1.33 × 10−4 5.75 × 10−4 2.68 × 10−4 1.16 × 10−3 1.86 × 10−4 8.08 × 10−4 2.21 × 10−3 9.59 × 10−3 2.54 × 10−4 1.10 × 10−3 1.94 × 10−3 8.40 × 10−3 1.65 × 10−4 7.16 × 10−4 4.31 × 10−4 1.87 × 10−3 9.97 × 10−4 4.32 × 10−3 5.11 × 10−4 2.21 × 10−3 4.06 × 10−3 1.76 × 10−2 7.09 × 10−5 3.07 × 10−4

1.81 × 10−3 2.83 × 10−3 9.90 × 10−3 1.55 × 10−2 1.61 × 10−3 2.53 × 10−3

2.45 × 10−3 3.84 × 10−3 5.05 × 10−3 7.93 × 10−3 2.80 × 10−3 4.40 × 10−3 1.93 × 10−2 3.03 × 10−2

5.08 × 10−4 7.97 × 10−4

1.13 × 10 4.89 × 10−4 3.40 × 10−4 1.47 × 10−3 2.21 × 10−4 9.57 × 10−4 1.70 × 10−4 7.37 × 10−4

2.29 × 10−3 3.59 × 10−3 2.13 × 10−3 3.34 × 10−3 1.91 × 10−3 2.99 × 10−3 1.89 × 10−3 2.96 × 10−3 1.52 × 10−3 2.38 × 10−3 1.10 × 10−2 1.72 × 10−2

1.27 × 10 2.00 × 10−3 2.25 × 10−3 3.53 × 10−3 1.61 × 10−3 2.53 × 10−3 1.66 × 10−3 2.61 × 10−3

−4

−4

2.27 × 10−3 1.91 × 10−3

5.19 × 10−3 4.36 × 10−3 5.67 × 10−3 4.76 × 10−3 3.43 × 10−3 2.89 × 10−3 1.39 × 10−2 1.16 × 10−2

2.49 × 10−3 2.09 × 10−3 8.96 × 10−3 7.53 × 10−3 2.13 × 10−3 1.79 × 10−3

2.35 × 10−3 1.98 × 10−3 2.16 × 10−3 1.81 × 10−3 2.42 × 10−3 2.03 × 10−3 3.29 × 10−3 2.76 × 10−3 2.27 × 10−3 1.90 × 10−3 9.86 × 10−3 8.28 × 10−3

1.40 × 10 1.17 × 10−4 3.34 × 10−3 2.80 × 10−3 2.29 × 10−3 1.92 × 10−3 2.48 × 10−3 2.09 × 10−3

CRing −5

2.45 × 10−3 5.63 × 10−3

2.63 × 10−3 6.04 × 10−3 2.63 × 10−3 6.04 × 10−3 2.47 × 10−3 5.67 × 10−3 3.24 × 10−3 7.44 × 10−3

2.43 × 10−3 5.58 × 10−3 2.91 × 10−3 6.68 × 10−3 2.42 × 10−3 5.55 × 10−3

2.45 × 10−3 5.63 × 10−3 2.37 × 10−3 5.44 × 10−3 2.48 × 10−3 5.71 × 10−3 2.51 × 10−3 5.77 × 10−3 2.40 × 10−3 5.52 × 10−3 2.96 × 10−3 6.80 × 10−3

5.53 × 10 1.27 × 10−4 2.51 × 10−3 5.77 × 10−3 2.40 × 10−3 5.51 × 10−3 2.45 × 10−3 5.63 × 10−3

CRderm −4

4.79 × 10−3 7.85 × 10−3

8.26 × 10−3 1.23 × 10−2 9.29 × 10−3 1.51 × 10−2 6.41 × 10−3 1.08 × 10−2 2.12 × 10−2 3.67 × 10−2

5.18 × 10−3 8.78 × 10−3 1.38 × 10−2 2.26 × 10−2 4.71 × 10−3 8.06 × 10−3

4.92 × 10−3 8.13 × 10−3 4.57 × 10−3 7.44 × 10−3 5.03 × 10−3 8.31 × 10−3 6.07 × 10−3 9.69 × 10−3 4.85 × 10−3 8.23 × 10−3 1.50 × 10−2 2.47 × 10−2

3.08 × 10 7.34 × 10−4 6.19 × 10−3 1.00 × 10−2 4.91 × 10−3 8.39 × 10−3 5.10 × 10−3 8.45 × 10−3

Total CR −5

2.96 × 10−5 4.64 × 10−5

8.50 × 10−5 1.33 × 10−4 7.72 × 10−5 1.21 × 10−4 1.06 × 10−4 1.66 × 10−4 6.15 × 10−4 9.65 × 10−4

4.47 × 10−5 7.01 × 10−5 9.57 × 10−5 1.50 × 10−4 3.29 × 10−5 5.16 × 10−5

2.31 × 10−4 3.62 × 10−4 4.92 × 10−5 7.73 × 10−5 2.52 × 10−4 3.96 × 10−4 6.03 × 10−4 9.46 × 10−4 7.66 × 10−5 1.20 × 10−4 1.36 × 10−4 2.14 × 10−4

4.30 × 10 6.74 × 10−5 1.70 × 10−4 2.67 × 10−4 2.53 × 10−4 3.97 × 10−4 1.05 × 10−4 1.64 × 10−4

ILCR

CRinh

ILCR −3

PM2.5

PM10

−5

3.72 × 10−5 1.61 × 10−4

5.43 × 10−5 2.35 × 10−4 6.19 × 10−5 2.68 × 10−4 5.40 × 10−5 2.34 × 10−4 1.77 × 10−4 7.67 × 10−4

4.46 × 10−5 1.93 × 10−4 7.09 × 10−5 3.07 × 10−4 3.89 × 10−5 1.69 × 10−4

1.20 × 10−4 5.19 × 10−4 4.15 × 10−5 1.80 × 10−4 1.31 × 10−4 5.68 × 10−4 3.31 × 10−4 1.43 × 10−3 6.11 × 10−5 2.65 × 10−4 7.48 × 10−5 3.24 × 10−4

3.24 × 10 1.41 × 10−4 8.22 × 10−5 3.56 × 10−4 1.48 × 10−4 6.43 × 10−4 7.18 × 10−5 3.11 × 10−4

CRinh −5

2.11 × 10−3 1.77 × 10−3

2.30 × 10−3 1.94 × 10−3 2.02 × 10−3 1.69 × 10−3 2.06 × 10−3 1.73 × 10−3 2.96 × 10−3 2.49 × 10−3

2.00 × 10−3 1.68 × 10−3 2.24 × 10−3 1.88 × 10−3 2.00 × 10−3 1.68 × 10−3

2.16 × 10−3 1.82 × 10−3 2.08 × 10−3 1.74 × 10−3 2.28 × 10−3 1.92 × 10−3 2.59 × 10−3 2.18 × 10−3 1.99 × 10−3 1.67 × 10−3 2.28 × 10−3 1.91 × 10−3

8.48 × 10 7.12 × 10−5 2.30 × 10−3 1.93 × 10−3 2.08 × 10−3 1.75 × 10−3 2.14 × 10−3 1.80 × 10−3

CRing

−5

2.38 × 10−3 5.46 × 10−3

2.38 × 10−3 5.47 × 10−3 2.40 × 10−3 5.51 × 10−3 2.36 × 10−3 5.41 × 10−3 2.44 × 10−3 5.60 × 10−3

2.36 × 10−3 5.43 × 10−3 2.40 × 10−3 5.52 × 10−3 2.36 × 10−3 5.42 × 10−3

2.44 × 10−3 5.62 × 10−3 2.37 × 10−3 5.44 × 10−3 2.48 × 10−3 5.70 × 10−3 3.05 × 10−3 7.00 × 10−3 2.38 × 10−3 5.46 × 10−3 2.41 × 10−3 5.53 × 10−3

3.66 × 10 8.40 × 10−5 2.41 × 10−3 5.53 × 10−3 2.47 × 10−3 5.67 × 10−3 2.43 × 10−3 5.59 × 10−3

CRderm

4.53 × 10−3 7.40 × 10−3

4.74 × 10−3 7.64 × 10−3 4.48 × 10−3 7.47 × 10−3 4.47 × 10−3 7.38 × 10−3 5.57 × 10−3 8.85 × 10−3

4.41 × 10−3 7.30 × 10−3 4.71 × 10−3 7.71 × 10−3 4.40 × 10−3 7.26 × 10−3

4.73 × 10−3 7.95 × 10−3 4.48 × 10−3 7.36 × 10−3 4.90 × 10−3 8.19 × 10−3 5.97 × 10−3 1.06 × 10−3 4.43 × 10−3 7.39 × 10−3 4.76 × 10−3 7.77 × 10−3

1.54 × 10−4 2.96 × 10−4 4.79 × 10−3 7.82 × 10−3 4.70 × 10−3 8.07 × 10−3 4.64 × 10−3 7.70 × 10−3

Total CR

Table 3 Results of cancer risks as CR (via inhalation (inh), ingestion (ing), and dermal absorption (derm)) and incremental life time cancer risk (ILCR) for PM10 and PM2.5-bound elements throughout the study area for children (C) and adults (A).

D. Roy, et al.

Atmospheric Pollution Research 10 (2019) 1964–1975

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Fig. 2. Probability density functions of predicted Total CR at the main city area (A16) for adult and children groups for PM10.

(ZM), A16 (ZC), and A11 (ZMF), respectively. Total PM10-bound carcinogenic elements (PB, Ni, Cr, and Cd) estimated maximum at ZC (A16: 14.51 μg/m3), followed by ZM (A17: 8.23 μg/m3) and ZMF (A11: 7.42 μg/m3). Among the all carcinogenic trace metals contribution of Cd was found to be higher with 92%, followed by Pb (6%) and Ni (1%) at A16 location. The excessive contribution of Cd in PM10 levels indicates that the mine fire activities and other local pollution sources could be the possible pollution sources of PM levels at city nearby mine fire area (A16) (ATSDR, 2012; Roy et al., 2016). Hence, the reference station (A18) is established nearby city area and far away from the mining area. A18 had lowest total trace metals (2–7 times) and carcinogenic trace metals (3–56 times) levels throughout the study area. Moreover, the trace metals found in the order of ZC (A16: 17.8 μg/ m3) > ZMP (A2: 16.3 μg/m3) > ZM (A5: 16 μg/m3) with the contribution of 12%, 10%, and 9%, respectively for total PM2.5 levels. Hence, PM2.5–bound carcinogenic trace metals estimated as 1.29% (1.18 μg/ m3) and 0.42% (0.82 μg/m3) at A9 (ZM) and A16 (ZC), correspondingly. Among the all trace metals carcinogenic metals were found 15%, 6%, and 5% at A9 (ZM), A11 (ZMF), and A16 (ZC) with the significant contributions of Cr, Pb, and Cd. The center of Dhanbad city, A16, had the highest concentrations of Pb and Cd. Roy et al. (2016) reported the vehicular exhaust emissions (20%) and open coal burning at hotels and restaurants (21%, kerosene and coal being the dominant fuels) were the major contributors of PM at A16. The highest concentrations of Cr, Ni, As, Al, and Mn were found at A9, A8, A2, and A11, respectively. In

A13: 95%; and A18: 81%) for PM10 and two stations (A7: 96% and A18: 31%) for PM2.5 (Table 1). However, in coalmining areas, such as the JCF, the permissible limit for PM10 is 250 μg/m3, as per the Environment (Protection) Rules, 1986. There is no specific ambient air quality standard for PM2.5 in Indian mining areas. Accordingly, this study found the monitoring stations located in the mining area having PM10 levels that exceeded the permissible limit except for A2, A9, and A7. PM10 and PM2.5 levels were also found to far exceed the permissible limits of the NAAQS across all monitoring stations. Zheng et al. (2019) reported similar high PM10 levels, as those of JCF, in the coal mining cities of China. The PM10 levels in JCF were also found to be significantly higher than that in the USA, Taiwan, and Spain (Jena and Singh, 2017). In 2009, the Central Pollution Control Board (CPCB) of India identified Dhanbad (Jharkhand) as a critically polluted industrial cluster/area with a CEPI score of 78.6 (CPCB, 2014). 3.2. Trace metal analysis Table 1 details the mean concentrations of trace metals in the PM10 and PM2.5 samples, wherein the level of Fe in both types of PM, throughout the study area, was found to be the highest, followed by Al and Cu. Across the 18 monitoring stations, the PM10-bound total trace metals estimated in the order of ZM (A17: 41.67 μg/m3) < ZMF (A11: 52.09 μg/m3) < ZC (A16: 75.52 μg/m3). The contribution of trace metals on total PM10 levels were quantify 19%, 17%, and 15% at A7 1970

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Fig. 3. Percentage contributions of carcinogenic elements in Total CR via inhalation, ingestion, and dermal absorption for both children and adult groups at A6, A11, A12 stations in ZMF and the reference location (A18/R) for PM10 and PM2.5.

all monitoring stations except few locations for adult. Moreover, children group has found higher HQing, HQderm, and HI levels. The most probable reasons are, a) low AT (ED × 365), b) higher IngR (children: 100 and adult: 50), and c) skin adherence factor (children: 0.04 and adult: 0.02). The non-cancer risk has direct relation with the concentration levels of trace metals. At A16 (ZC) was found to be maximum non-cancer risks due to high concentration levels of PM10-and PM2.5bound trace metals. Amongst all the elements, the highest HQ levels were obtained for Mn and Cd. As example, for PM10, at A16, elements such as Mn (2.8 × 10+1 and 2.87 × 10+1), Cd (2.06 × 10+1 and 1.06 × 10+2), and Cd (4.16 and 7.84) were contributed maximum in the HQ levels via inhalation, ingestion, and dermal absorption, respectively, for adult and children. For HQinh, Cd also showed an important factor of non-cancer risk levels with the value of 1.29 × 10+1 for both age groups for PM10. Jena and Singh (2017) had reported similar non-cancer risks in the city, institute, and mining areas of Dhanbad/JCF. Similar significant non-cancer risks were reported for PM10-bound metals in Asturias, Spain (Megido et al., 2017), while adequate non-cancer risks of PM2.5-bound metals (in terms of HQinh and HI) were reported from the Shandong Province and Nanjing, China (Hu et al., 2012; Zhang et al., 2018).

these locations, industrial (30–40%), vehicular (21–22%), paved/nonpaved (11–15%), and coal combustion (13–25%) emissions were the major sources (Roy et al., 2016). In ZMP, the mean concentrations of Pb, Ni, Cd, and Cr, varied between 1.10 and 0.03 μg/m3, 0.064–0.035 μg/m3, 0.078–0.013 μg/m3, and 0.384–0.036 μg/m3, respectively; ZM, 0.096 ± 0.018 μg/m3, 0.065 ± 0.015 μg/m3, 3 0.065 ± 0.014 μg/m , and 0.276 ± 0.018 μg/m3, respectively; ZMF, 0.034–0.240 μg/m3, 0.044–0.058 μg/m3, 0.014–0.015 μg/m3, and 0.036–0.122 μg/m3, respectively; and ZC, 0.027–0.274 μg/m3, 0.400–0.026 μg/m3, 0.4–0.013 μg/m3, and 0.16–0.02 μg/m3, respectively. A18 had the lowest total trace metals (2–8 times) and carcinogenic trace metals (3–13 times) levels throughout the study area. Major sources of Fe could be mining, soil erosion, road dust re-suspension, construction activities etc. (Dubey et al., 2012), while fuel combustion, wind-blown soil, the metal industry etc., could be sources of secondary elements like Al (Roy et al., 2016). Cd, a signature element of fossil fuel combustion, was found to be high in both Z3 and Z4 (ATSDR, 2012). 3.3. Potential health risks 3.3.1. Non-cancer risks The HQ and HI values for PM10-and PM2.5-bound Pb, Ni, Cu, Mn, Fe, Zn, Cd, Cr, and As, are presented in Table 2, where insignificant HQing and HI was observed for children and adult groups throughout the study area. The non-cancer risks were higher in children than in adult w.r.t all exposure types. The overall HI values for PM10 and PM2.5 were in the ranges of 2.47–1.58 × 10+2 and 1.05–1.59 × 10+1, respectively. The maximum HI levels for PM10 in children were found in ZC (A16: 1.58 × 10+2), followed by ZM (A17: 1.11 × 10+2), and ZMF (A11: 1.06 × 10+2). Similarly, ZMF exhibited the maximum HI level for PM2.5 in children at 1.59 × 10+1 (A11), followed by ZC (A16: 1.19 × 10+1). The HQinh levels were found to be significant than the other exposures amongst all the locations and age groups, the highest being at ZC (A16: 4.19 × 10+1) and ZMF (A11: 1.33 × 10+1) for PM10 and PM2.5, respectively. Significant HQing values for PM10 occurred in

3.3.2. Cancer risks Fig. 1 and Table 3 presents the detailed output of CR associated with PM10-and PM2.5-bound trace elements (Pb, Cd, Cr(VI), and Ni), via inhalation (CRinh), ingestion (CRing), and dermal absorption (CRderm). Accordingly, A16 displayed the highest Total CR values for PM10, for both age groups (adult: 3.67 × 10−2; children: 2.12 × 10−2) in ZC, followed by A17 (adult: 2.47 × 10−2; children: 1.50 × 10−2) in ZM, and A11 (adult: 2.26 × 10−2; children: 1.38 × 10−2) in ZMF. A16 also exhibited the maximum CRinh (1.76 × 10−2 and 4.06 × 10−3), CRing (1.16 × 10−2 and 1.39E × 10−2), and CRderm (7.44 × 10−3 and 3.24 × 10−3) values for adult and children, respectively throughout the study area for the same PM. Moreover, amongst the two age groups, CR was found to be higher for adults than children. The values of the 1971

Atmospheric Pollution Research 10 (2019) 1964–1975

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Fig. 4. Probability density functions of predicted Total CR at the coal mining area (A9) for adult and children groups for PM2.5.

(mean: 1.2 × 10−4), and in an urban site (mean: 6.37 × 10−4) (Chen et al., 2008; Jia et al., 2011; Ramírez et al., 2011). The percentage contribution of each element to individual exposures revealed Cd, Cr, and Pb as more significant for raising the cancer risk levels in the study area (equally for adults and children). For example, Cd contributed 7020%, 98-20%, 95–17%, and 99–82% to the CRinh levels in all four zones: ZMP, ZM, ZMF, and ZC, respectively. Moreover, Cr(VI) and Cd were found to be the highest contributors to CRderm and CRing, respectively. However, in the background area, Cr(VI) contributed 80% and 90%, respectively to CRinh and CRderm levels. While, Cd is a signature element of fossil fuel combustion and can be transported over long distances in the atmosphere (ATSDR, 2012), Cr is a marker of high temperature oil combustion and road dust emissions (Roy et al., 2016). Hence, mining and mine-fire activities, along with local combustion/ road dust emissions could be the primary sources of PM10-bound carcinogenic trace metals in the four zones of the study area (Roy et al., 2016). For PM2.5, Total CR, CRinh, CRing, and CRderm levels ranged from 1.54 × 10−4 to 1.06 × 10−2, 3.24 × 10−5 to 1.43 × 10−3, 8.48 × 10−5 to 2.59 × 10−3, and 3.66 × 10−5 to 7.00 × 10−3, respectively, throughout the study area. The maximum Total CR (1.06 × 10−2), CRinh (1.43 × 10−3), and CRderm (7.00 × 10−3) values for adult were reported at A9 in Z2 (core mining area). The second

parameters considered in the CR analysis, such as ED (for inhalation, ingestion, and dermal absorption), IngR (for ingestion), and SA (for dermal absorption), was higher for adults than children (Supplementary Table ST1). Similar cancer risk levels were observed in the ILCR evaluation throughout the study area, as depicted in Fig. 1. Moreover, a Monte Carlo simulation with 50,000 iterations was used to assess the 95% confidence level of Total CR and the contribution of individual exposure routes at A16, to verify the CR levels, as shown in Fig. 2 and Supplementary Figures: SF2 to SF7. The results, thus obtained, showed the same CR values as calculated from the exposure pathways with 95% UCL for PM10-bound carcinogenic trace metals. The Total CR levels were not only found to be significant (> 1 × 10−6), but also far exceeded the regulatory level of acceptable CR (1.00 × 10−6 to 1.00 × 10−4) (Widziewicz et al., 2016). Consequently, the study area falls within the high-risk category (10−3≤ to < 10−1). The ILCR values varied within the same range as CR, estimated via exposure pathways for both age groups. The percentage contribution of each element of PM10 to the Total CR via three exposures is shown in Fig. 3 and Supplementary Figures: SF8 to SF10. Similar inhalation CRin mining areas have been reported by Jena and Singh (2017), Zhang et al. (2008), and Zheng et al. (2019) for adults and children in India and China. Apart from mining, substantial lung CR were reported for the manufacturing industry (mean: 1.64 × 10−2), the chemical industry

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highest CR levels were estimated at A16 (Total CR: 8.85 × 10−3 and 5.57 × 10−3, CRinh: 7.67 × 10−4 and 1.77 × 10−4, CRing: 2.49 × 10−3 and 2.96 × 10−3, and CRderm: 5.60 × 10−3 and 2.44 × 10−3 for adult and children, respectively) in ZC (city nearby mine-fire area). Once again, higher CR levels were estimated for adults than children, because of the influence of IngR, ED, and SA upon the age specific risk levels. The mining area and the city nearby the mine fire area exhibited higher CR levels compared to the other zones. The Total CR fell in the moderate risk category (10−4≤ to < 10−3) throughout the study area, as per the NYS DOH (2012), while CRinh, CRing, and CRderm were found in the low (10−6≤ to < 10−4) and moderate (10−4≤ to < 10−3) categories. Moreover, the Total CR levels were not only significant (> 10−6), but also exceeded the regulatory levels of acceptable CR (1.00 × 10−6 to 1.00 × 10−4) (Widziewicz et al., 2016), while the ILCR values (4.30 × 10−5 to 9.65 × 10−4) were found to be slightly lower than the total CRinh values for PM2.5. However, both risk levels remained in the low and moderate categories throughout the study area for adults and children. Similar levels of Total CR, CRinh, CRing, and CRderm were estimated through Monte Carlo simulation as shown in Fig. 4 and Supplementary Figures: SF11 to SF16. Comparably significant and high-risk levels for PM2.5-bound metals have been reported in Velenje, Solvenia (in the mining area) (Moreno et al., 2019); in Shandong province, China (with CR levels of 4.00 × 10−3 to 5.40 × 10−4) (Zhang et al., 2018); and in Kolkata, India (1.40 × 10−2) (Das et al., 2015). Furthermore, significant CR level was found in Beijing (1.80 × 10−4) and north-east (1.00 × 10−6), and Nanjing (2.00 × 10−5) in China, and Canadian oil sands communities (1.00 × 10−5) for PM2.5-bound trace metals (Bari and Kindzierski, 2017; Gao et al., 2017; Gao and Ji, 2018; Hu et al., 2012). For all exposures, the impact of Cr(VI) and Cd (PM2.5-bound) upon the CR levels were identified to be more significant than other metals, equally for adults and children. The contribution of Cr(VI) to total CRinh varied between 92 and 52% (ZMP), 98-40% (ZM), 85-55% (ZMF), and 85-20% (ZC) as shown in Fig. 3 and Supplementary Figure (SF8-SF10). It was found that Cr(VI) was also the maximum contributor to CRinh (55%) and CRderm (73%) at the reference station. For CRing and CRderm, along with Cr(VI), Pb was the highest contributor in ZMP, ZM, and ZMF. In ZC, Cd was found as the major contributor (CRinh: 7910%; CRing: 78-37%; and CRderm: 62-25%). Moreover, Cr and Cd are the marker elements of high-temperature oil, coal, and refuse combustion, among others (Roy et al., 2016; Uberoi and Shadman, 1991). In Kolkata, India, PM2.5-bound Cr was assessed to be the highest CR element (1.20 × 10−2) (Das et al., 2015). Similarly, in Beijing and Nanjing (China), the primary element of CR levels was identified as PM2.5bound Cr (Gao and Ji, 2018; Hu et al., 2012). Therefore, it can be concluded that local combustion/road dust emissions, mining, and mine fire sources could be the major contributors of PM2.5-bound carcinogenic trace metals in the study area (ZMP, ZM, ZMF, and ZC) for adults and children alike (Roy et al., 2016).The fine PM such as PM2.5 is an integral part of PM10. The average CR levels for PM2.5 were highest at ZC (48%), followed by ZMF (29%), ZMP (22%), and ZM (13%), compared to the Total CR values calculated for PM10. The CR associated with fine PM-bound trace metals was found to be higher in the city (A16: 74%) and mine-fire (A11: 66%) areas. Pollution due to PM2.5 is serious since it can penetrate and deposit at the lower part (Tracheobronchial and Pulmonary region) of the human respiratory tract (de Winter-Sorkina and Cassee, 2002; Sarigiannis et al., 2015). Hence, CR values calculated for PM2.5-bound trace metals were more significant for the people living in the study area.

73.2%, children: 64.1%) and AF (adult: 25.9%, children: 28.5%) were identified as the leading factors, followed by the SA (adult: 0.5%, children: 6.0%) for PM2.5. Conversely, at A16, ED (adult: 78.7%, children: 93.4%) was recognized as the predominant factor for PM10. Both ED and AF have consistently been identified as important factors by previous studies (Chen and Liao, 2006; Tarafdar and Sinha, 2017; Wu et al., 2013). Moreover, the negative values of BW indicates an inverse correlation with CRinh both age groups, for PM10 and PM2.5. Amongst all the carcinogenic elements, PM10-bound Cd was found to be most significant at A16 (adult: 19.9%, children: 4.0%). Roy et al. (2016) suggested the coal combustion activities like coal mine-fire, adjacent to the location, as the possible sources of Cd. Hence, assessing the contribution of non-anthropogenic factors such as coal mine-fires in the nearby city area along with the detailed health risk analysis considering different age groups of adults and teen could be the future scope of the present study. 3.5. Uncertainty of the assessment The inappropriate use of input parameters can cause uncertainty in the assessment of health risks. Therefore, this study applied the Monte Carlo simulation technique, with 50,000 iterations, to minimize the level of uncertainty. The CR calculated from the 95% UCL values of PMbound carcinogenic trace metals were verified by the 95% cancer risk levels calculated through the Monte Carlo probabilistic analysis. However, uncertainty in this study could possibly generate from the exposure parameters, such as SA, IR, and AF, which were as per the USEPA recommended values. The same values might not apply to the Indian scenario. Moreover, there are no significant studies were reported on the health risk parameters (ET and EF) for the people living in mining area. These values were considered (ET: 24hrs/day and EF: 350 days/year) as per the previous study conducted in the same mining area (Jena and Singh, 2017), suburban (Megido et al., 2017) and urban (Hoseini et al., 2015) area as per USEPA, 2016. People are living nearby the mining area spends their maximum time at outdoor. Even they sleep outside the room at night in all days except strong winter and rain. Detailed investigation on ET and EF values for the people living in mining area could be the future scope of this study. 4. Conclusions Particulate matter pollution is responsible for serious and adverse health effects in critically polluted mining sectors, such as the JCF in India. This study found the concentration levels of PM10 and PM2.5 to be considerably higher than their permissible limits for residential and coal mining areas in India. Human health risks of PM10 and PM2.5, in terms of non-cancer risks (as HQ and HI) were estimated to be adequate throughout the study area. The CRinh, CRing, and CRderm were also estimated to be significant for adults and children. For PM10, the Total CR levels were significant, as well as far exceeded the acceptable regulatory levels. Consequently, the study area falls in the high-risk category. The ILCR values were in the same range as CR for both age groups, as estimated via exposure pathways. In case of PM2.5, the Total CR remained in the moderate risk category, while CRinh, CRing, and CRderm levels were low and moderate. The ILCR values were slightly different from the total CRinh for PM2.5, although both risk levels were in the same category (low and moderate) for both adults and children. Comparable levels of Total CR, CRinh, CRing, and CRderm were obtained through Monte Carlo simulation for PM10 and PM2.5. Cd, Cr, and Pb were significant contributors to the CR levels of the study area, equally for adults and children. Moreover, the effect of Cd emerged to be most pronounced amongst all other elements in the city area adjacent to the mine-fire area. The local combustion/road dust emissions, mining, and mine-fires could be the major sources of PM10 and PM2.5bound carcinogenic trace metals in the study area. Thus, this study concludes that the Jharia coalfield is not only critically polluted with

3.4. Sensitivity analysis The most important factors of CR outcomes were identified through sensitivity analysis using tornado plots, as shown in Figs. 2 and 4 for PM10 and PM2.5, respectively. The A9 and A16 locations showed the highest CR levels for PM2.5 and PM10, respectively. At A9, ED (adult: 1973

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respect to particulate matter pollution levels, but is also a potential health risk zone.

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