Aerosol and Air Quality Research, 20: 2805–2825, 2020

ISSN: 1680-8584 print / 2071-1409 online

Publisher: Taiwan Association for Aerosol Research
https://doi.org/10.4209/aaqr.2020.04.0182

Spatio-seasonal Concentrations, Source Apportionment and Assessment of

Associated Human Health Risks of PM2.5-bound Polycyclic Aromatic
Hydrocarbons in Delhi, India

Anurag Yadav1,2, Sailesh N. Behera2,3*, Pavan K. Nagar1, Mukesh Sharma1

1
Department of Civil Engineering, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh, PIN: 208016, India
2
Department of Civil Engineering, Shiv Nadar University, Greater Noida, Gautam Buddha Nagar, Uttar Pradesh, PIN:
201314, India
3
Centre for Environmental Sciences and Engineering, Shiv Nadar University, Greater Noida, Gautam Buddha Nagar,
Uttar Pradesh, PIN: 201314, India

ABSTRACT

To characterize the polycyclic aromatic hydrocarbons (PAHs) in PM2.5 (particles with an aerodynamic diameter ≤ 2.5 µm)
in Delhi, the national capital of India and one of the most polluted megacities in the world, we conducted a comprehensive
field campaign at six sampling sites in different areas during winter and summer. Both the PM2.5 and PAH concentrations
exhibited seasonal variations, with higher values during winter (356 ± 136 µg m–3 and 75.1 ± 50.2 ng m–3 for the PM2.5 and
PAHs, respectively) than summer (268 ± 94 µg m–3 and 10.4 ± 8.5 ng m–3, respectively). Additionally, the maximum winter
concentrations were found in the urban industrial-cum-residential area (430 ± 104 µg m–3 and 124.5 ± 70.7 ng m–3 for the
PM2.5 and PAHs, respectively). Among the PAHs, benzo[ghi]perylene displayed the highest ambient concentration (14.3 ±
7.4 ng m–3 during winter), followed by indeno[1,2,3-cd]pyrene (13.1 ± 7.3 ng m–3 during winter), at the majority of the sampling
sites. Additionally, based on the benzo[a]pyrene-equivalent concentrations at the six sites, we estimated the PAH-associated
incremental lifetime cancer risk (ILCR) in the entire study area to be 423 per 1 million persons, which exceeds the World
Health Organization (WHO) limit. Source apportionment performed with the Chemical Mass Balance Model version 8.2
(CMB8.2) revealed that emissions from vehicles, municipal waste burning and biomass burning contributed 62%, 15% and
11% to the total PAH mass, respectively. Our results indicate that PM2.5-bound PAHs in Delhi will continue to pose serious
health risks without collective initiatives for pollution control from scientific, policy-making and regulatory bodies.

Keywords: Total benzo[a]pyrene-equivalent concentration; Incremental lifetime cancer risk (ILCR); Chemical Mass
Balance Model version 8.2 (CMB8.2); Biomass burning; Municipal solid waste burning.

INTRODUCTION examining the possible alleviation measures to reduce

pollution levels (Chowdhury et al., 2007; Kiesewetter et al.,
Delhi, the national capital of India and world’s second 2017). Specifically, the rise in atmospheric levels of PM2.5
most populous city has already been home to more than and its chemical constituents in Delhi is a matter of concern,
26 million inhabitants, and is rapidly growing in terms of as these are directly associated with increase in number of
population and industrialization along with its large vehicular hazy days in a year, and human health implications (Goel et
fleet of around 10 million registered vehicles in 2015 (Solanki al., 2015; Saraswat et al., 2016). For example, the health
et al., 2016; Economic Survey of Delhi Report, 2017). Because impact estimate reported by Guttikunda and Goel (2013)
of recurrence of severe air pollution episodes, the deteriorated assessed that 7,350–16,200 premature deaths, and 6.0
air quality in Delhi has drawn regional and global attentions million asthma effects happened in Delhi due to exposure to
from all sections of research and policy-making bodies in existing PM levels. Delhi’s 32.1% school children suffered
from respiratory problems which are directly associated
with concentration levels of respirable atmospheric particles
(Swaminathan et al., 2006; Siddique et al., 2011).
*
Corresponding author. The responsible sources of air pollution in Delhi are
Tel.: +91-120-3819100 ext. 745; Fax: +91-120-3001580 vehicles, industries (point and area sources), domestic heating
E-mail address: [email protected]; for cooking, open burning that includes municipal solid
[email protected] waste (MSW) burning and biomass (BM) burning, suspended

Copyright The Author(s). This is an open access article distributed under the terms of the Creative Commons Attribution License (CC BY 4.0), which permits
unrestricted use, distribution, and reproduction in any medium, provided the original author and source are cited.
2806 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020

coal and fly ash, suspended road dust, construction dust and exposure to PAHs in this rapidly growing Indian urban
many fugitive sources including roadside heating of region. The source apportionment studies of PAHs conducted
charcoal by small vendors (Chowdhury et al., 2007; Goel et during last two decades using characteristic ratios and
al., 2015; Nagar et al., 2017; Tyagi et al., 2017). The report principal component analysis (PCA) have revealed that
of World Health Organization (WHO) and observations vehicular emission was observed to be the largest source of
from other studies also established that inhabitants staying PAHs with contribution up to 85% during all seasons in
in Delhi are at higher risk of mortality and morbidity due to Delhi (Sharma et al., 2007; Ravindra et al., 2008). In addition,
exposure to air pollutants (WHO, 2005; Kantipudi et al., season-specific studies conducted in Delhi showed difference
2016). This is also a fact that despite several measures in levels and trends on contributions of sources to ambient
developed and implemented by concerned regulatory PAHs (Jyethi et al., 2014; Singh et al., 2011). Some studies
authorities such as relocation of highly polluting industries were also conducted at multi-sampling sites in Delhi in
like cement manufacturing, wood industries and brick kilns different seasons of a year (Gupta et al., 2011; Sarkar and
outside of Delhi’s boundary and conversion of public transport Khillare, 2013). However, the source contribution from
fleet for transport buses and 3-wheeler motor rickshaw from significant sources like open burning (municipal waste and
diesel to compressed natural gas (CNG) during 2002, the agricultural residue burning) to TPAHs has not been examined
annual average concentration of PM2.5 in Delhi was observed in detail so far. Hence, chances for increase in concentration
as 8–10 times higher than the annual average of WHO air levels of TPAHs during winter due to rise in activities of
quality standards of PM2.5 (10 µg m–3) during recent years biomass burning are higher in Delhi. In addition to studies of
(Chowdhury et al., 2007; Tiwari et al., 2014; Saxena et al., PAHs in Delhi as cited above, several other studies examined
2017). trends in concentration levels of PAHs at other Indian cities
Among various categories of particulate organic constituents, including Agra (Rajput and Lakhani, 2012; Masih et al.,
the ambient concentration levels of trace chemical compounds 2010), Amritsar (Kaur et al., 2013), Kanpur (Singh et al.,
of polycyclic aromatic hydrocarbons (PAHs) is a matter of 2015), Mumbai (Sahu et al., 2008; Abba et al., 2012), Chennai
concern for human health due to their highly persistent nature (Mohanraj et al., 2011), and Tiruchirappalli (Mohanraj et al.,
causing carcinogenic, mutagenic and teratogenic diseases 2011).
on a long-term basis (Kim et al., 2013; Kamiya et al., 2016; The Indian studies cited above lack in establishing source–
Yang et al., 2017). Normally, PAHs in the atmosphere are receptor linkage through a robust approach using more reliable
emitted from combustion of organic matter used for different quantitative method like chemical mass balance model. The
industrial processes and energy production, vehicular traffic, study to conduct present concentration levels of PAHs in
incineration of refuse burning, biomass burning and residential diversified ways with spatial and seasonal distributions at
heating (Ravindra et al., 2006; Liu et al., 2016; Lai et al., more number of sampling sites in Delhi should be
2017). PAHs with 2–3 rings (low molecular weight [LMW]) encouraged to get more insights. To fill the knowledge gaps
are generally present in the gas phase under normal in literature and establish the source-receptor linkage, this
atmospheric conditions, whereas PAHs with 4–7 rings (high comprehensive field campaign is first of its kind to present
molecular weight [HMW]) are mostly adsorbed on particle concentration levels PAHs at six different sampling sites
surfaces due to their low vapor pressure in particulate phase, during both winter and summer seasons in Delhi (Fig. 1).
especially in cold seasons (Tsapakis and Stephanou, 2005; This study used USEPA’s Chemical Mass Balance Model
Chen et al., 2016; Amarillo et al., 2017). The chemical version 8.2 (CMB8.2) to apportion contributions from
reactivity, solubility and vapor pressure of PAHs decrease significant sources to ambient concentration levels of PAHs
with increase in number of aromatic rings; as a result, HMW at different sites during both these seasons. In addition, we
PAHs bio-accumulate in human bodies with more intensity conducted human health risk assessments for occurrence of
causing severe health damages than that of LMW PAHs cancer diseases for adults due to exposure to ambient
(Ravindra et al., 2006; Amarillo et al., 2017). concentration levels of PM2.5-bound PAHs by considering
The Central Pollution Control Board (CPCB), the regulatory benzo[a]pyrene equivalents at different sites.
body of India, realized the incidence and long-term health
effects from the toxicity of PAHs, which are associated with MATERIALS AND METHODS
inhalable fraction of particulate matter (CPCB, 2012; Kaur
et al., 2013). As a result, India has adopted a maximum 24-h Characteristics of Study Area
average standard limit of 1 ng m–3 for benzo[a]pyrene (the The study area Delhi (28°38ʹN and 77°13ʹE; Fig. 1) is the
most common carcinogen in air with proven carcinogenicity national capital of India, and has 1,483 km2 area, with the
in animal and human bodies) as a surrogate of other PAHs largest spread and most densely populated (11,297 persons
to regulate atmospheric levels of PAHs. The ambient km–2) urban region in the Indo-Gangetic Plain (IGP) region.
concentration levels of total PAHs (TPAHs) measured in This IGP region is the largest river basin area in India,
Delhi were observed to be at least an order of higher located at latitudes from 22°30ʹN to 31°30ʹN, and longitudes
magnitude than that of European and U.S. cities, raising the from 73°30ʹE to 89°30ʹE that supports more than 40% of
concern over such higher levels in Delhi (Sarkar and Khillare, India’s population and 26% of Indian landmass (Behera and
2013; Jyethi et al., 2014; Manoli et al., 2015; Ramirez et al., Sharma, 2010; Behera et al., 2015). Three distinct seasons are
2016). Therefore, it is essential to monitor and examine levels being felt in the study area with summer, monsoon and winter.
of PAHs and conduct human health risk assessment with Calm atmospheric conditions and temperature inversions
 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020 2807

Fig. 1. Details of sampling campaign depicting site locations, pollution characteristics and sampling periods of all sampling
sites.

during winter due to low temperature (average: 12–13°C) residential Site, Urban Industrial Site II, and Semi-urban
are the reasons for lower atmospheric boundary layer, which Site. The basis of classification was based on the influence
restricts dispersion of pollutants (Hoque et al., 2008; Saxena of various sources on ambient levels of PM in that particular
et al., 2017). Thus, this atmospheric phenomenon shoots up region. The detailed descriptions of sampling sites with
concentration levels of air pollutants during winter, resulting location (coordinates), emission source characteristics and
in hazy condition that reduces atmospheric visibility (Saraswat sampling duration are presented in Fig. 1.
et al., 2016). For collection of PM samples at each sampling site, a
Partisol™ 2300 4-channel speciation sampler (Thermo Fisher
Particulate Sampling Campaign Scientific Inc., USA) was used at a flow rate of 16.7 L min–1
Atmospheric PM2.5 sampling campaign meant for analysis with an inlet that removed particles of aerodynamic diameter
of PAHs were conducted at six different sampling sites with greater than 2.5 µm. The remaining particles (PM2.5) were
diverse pollution activities during two distinct seasons, i.e., collected on 47 mm diameter quartz fiber filter (Grade QM-
winter (23 November 2013–22 February 2014) and summer A; Whatman). Each set of sampling meant for measurement
(4 April–16 July 2014). The sampling sites were classified of PAHs was conducted for 48 h. Quartz filters required for
into Urban Industrial-cum-residential Site, Urban Industrial sampling were first heated at 600°C for 12 h to remove
Site I, Urban Residential Site, Urban Commercial-cum- background organic matter. As a standard protocol, the
2808 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020

filters meant for sampling were pre-conditioned and post- evaporator (RV 10; IKA®, Germany) at 40°C and 500 mm
conditioned at temperature ~20°C, and RH ~40% in controlled Hg vacuum. 4 mL of n-hexane was used to re-dissolve the
desiccator for 24 h. A total number of 125 particulate field extract and was transferred to a sample bottle. The purified
samples (64 samples during winter and 61 during summer) extracted sample from rotary evaporator was subjected to a
were collected at six sampling sites for further sample concentrated volume of about 1 mL by gentle streaming of
preparation and chemical analysis of PAHs. The number of nitrogen (TurboVap; Caliper Life Sciences, USA). This
samples at each sampling site during every season was 10 extracted sample was finally transferred to a 2 mL capacity
or 11. Substantial quantity of field and laboratory blank sample vial before injecting it into gas chromatography-
filters (20%) were kept for assessment of quality assurance mass spectrometry (GC-MS).
and quality control (QA/QC) checks during chemical analysis. 16 USEPA priority PAHs analyzed and quantified in this
These blank filter samples were prepared and analyzed for study were: naphthalene (Naph), acenaphthylene (Acy),
individual PAHs (Table S1), and the final reported result of acenaphthene (Ace), anthracene (Ant), fluorene (Flu),
any field sample was measured concentration subtracted phenanthrene (Phe), pyrene (Pyr), fluoranthene (Flan),
with average of blank concentration. The gravimetric method benzo[a]anthracene (BaA), chrysene (Chr),
was used to determine concentrations of PM2.5 through benzo[b]fluoranthene (BbF), benzo[k]fluoranthene (BkF),
weighing quartz filters of pre- and post-sampling conditions benzo[a]pyrene (BaP), indeno[1,2,3-cd]pyrene (InP),
using a digital microbalance (MX5; Mettler-Toledo, USA) dibenzo[a,h]anthracene (DahA), benzo[ghi]perylene (BghiP).
with a sensitivity of 0.001 mg. As a standard protocol, regular The PAHs were analyzed using a GC–MS (Clarus 600 MS;
calibrations of balance for weighing and sampler for flow PerkinElmer, USA) with a PerkinElmer capillary column
rate were conducted for validation of PM mass measurements (30 m × 0.25 mm × 0.25 µm; Elite-5MS). During sample
throughout the sampling period. The filters were stored in analysis, injections were performed in split mode, with a
Petri dishes (lined with aluminum foil), sealed with Teflon high-purity helium flow rate of 1.0 mL min–1 and injector
tape during pre- and post-sampling periods. PM2.5 mass temperature at 280°C. The GC time–temperature was
concentrations (µg m–3) were calculated through gravimetric programmed as follows: Heat to 70°C, hold for 2 min,
analysis based on approach of our previous studies (Behera increasing 10°C min–1 until 180°C then heat to 230°C at 6°C
and Sharma, 2010, 2015; Nagar et al., 2017). After estimation min–1 without hold and heat to 275°C at 2°C min–1 followed
of PM2.5 mass, the filter samples were kept refrigerated at by hold for 5 min. The single ion monitoring mode (SIM)
4°C until further sample preparations. was performed for mass detection in the spectrometer
instrumentation. The GC–MS was calibrated for all targeted
Sample Preparation and Chemical Analysis PAHs using aforementioned mix standard and an internal
Glassware and apparatus required for sample preparation standard pyrene-d10. Table S1 presents summary of chemical
were washed with high-purity deionized water (18.2 MΩ cm–1) analytical parameters during quantification of PAHs.
taken from the Milli-Q system (Millipore, USA), followed After analytical results were produced from GC–MS, it
by rinsing with high-performance liquid chromatography was observed that the concentrations of Naph, Acy, Ace and
(HPLC) grade acetone and n-hexane prior to their uses. All Flan levels were below method detection limit (MDL). The
solvents, dichloromethane (DCM) and n-hexane used for reasons for such trends might be due to the facts that the low
sample preparation were of HPLC grade and procured from molecular weight, high volatility and use of high-volume
Merck (India) Ltd. For instrument calibration and sampling might impose uncertainties in the measured
standardization, a standard mixture containing 16 PAHs (16 concentrations of these PAHs. In addition, a study (Singh et
compounds specified in USEPA Method 610) and pyrene- al., 2012) conducted at Delhi also reported particulate
d10, procured from Supelco (Bellefonte, PA, USA) were portion of these PAHs were not detectable or of negligible
used as external and internal standards, respectively. Prior concentrations. In further interpretation of results for trends
to extraction process, all filter samples were spiked with in ambient levels, source apportionment and risk assessment,
known concentrations of PAHs and pyrene-d10 solution to these compounds were excluded in the data analysis. Hence,
assess the analytical recovery efficiencies during instrumental 12 PAHs considered for further analysis were Ant, Flu, Phe,
analysis. After spiking, each filter sample was ultra-sonicated Pyr, BaA, Chr, BbF, BkF, BaP, InP, DahA and BghiP.
in a mixture of n-hexane and DCM (1:1 v/v) with total of
10 mL volume for 30 min, followed by second sonication Characteristic Ratios of PAHs
for 30 min with additional 10 mL volume of same mixture Emission sources on a broader sense at six sampling sites
(Chang et al., 2006; Szulejko et al., 2014). After second during winter and summer were identified using
sonication, the suspension was decanted, followed by third concentration ratios of individual PAHs or group of PAHs,
sonication with 10 mL volume of same mixture and filtered assuming that source signature of a particular molecular
using a 0.22 µm Millex Syringe filter (Millipore, USA) into marker remains constant in the ambient air after emitted
a reagent bottle. The decanted samples were passed through from that source. In other words, PAHs used as tracers to
silica gel column clean-up (Loba Chemie, Mumbai) using identify any responsible sources should be considerably less
our established protocol reported earlier (Aatmeeyata and reactive when exposed to sunlight and atmospheric oxidants
Sharma, 2010). To elute PAHs from silica gel column, 30 mL (Zhao et al., 2011; Wu et al., 2014). The characteristic ratios
of a 3:1 v/v mixture of n-hexane and DCM was used. The of PAH molecular markers have been used to distinguish
sample extract was concentrated to dryness using a rotary among various possible sources including coal combustion,
 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020 2809

petroleum sources and wood burning (representative of BM sources into fuel type and industrial combustion process
burning) of PAHs (Yunker et al., 2002; Ravindra et al., type. For example, combustion of coal occurs in several
2006; Hu et al., 2011; Mishra et al., 2016; Yang et al., 2017). activities such as solid fuel in boilers in power plants, coke
This has been observed that lower molecular weight of 2–3 ovens, residential cooking in lower socio-economic areas,
ring PAHs are occurred mostly in gaseous phase and higher and restaurant usage for grilling and baking of food. The
molecular weight of 4–6 ring PAHs are occurred mostly in emission source profiles of PAHs for various identified
particulate phase (Singh et al., 2012). The characteristic sources were adopted from relevant literature (Raiyani et al.,
ratios should be chosen in such a way that they should be 1993; Khalili et al., 1995; Lee and Kim, 2007; Bi et al.,
more conservative than other ratios during transportation in 2008; Kong et al., 2013; Park et al., 2013; USEPA, 2016;
the air medium (Tobiszewski and Namieśnik, 2012; Wu et Lai et al., 2017). We considered an uncertainty of 20% for
al., 2012). As a result, the characteristic ratios can stay the all ambient concentrations and source profiles of individual
same among gas-phase, particle-phase and total (gas-phase PAH compounds during simulation on the platform of
+ particle-phase) PAHs (Tobiszewski and Namieśnik, 2012; CMB8.2 (Lai et al., 2017). Looking at the past trends of
Wu et al., 2010, 2012). A couple of past studies (Ströher et research reported in the literature, several studies in
al., 2007; Zhao et al., 2011) suggested to use the concentration developing countries have used the source profiles of both
of both gas and particle phases of each marker together to developed and developing countries (Hanedar et al., 2011;
estimate the characteristic ratios. Several studies (e.g., Zhou Bortey-Sam et al., 2015; Teixeira et al., 2015). The vehicular
et al., 2005; Wang et al., 2006) showed that characteristic emission technologies and some of the other sources in
ratios of PAH markers do not change with particle size, e.g., India are mostly similar to developed countries.
PM2.5 (fine particle) or PM2.5-10 (coarse particle). The source elimination option of CMB8.2 software was
With aforementioned concepts and based on supportive adopted in this study to remove negative source contribution
literature, we used different characteristic ratios to assess estimates from the CMB results. After simulations, specific
qualitative attributions of various emission sources responsible outputs were considered as calculation of SCEs for further
for concentration levels of PAHs (Caricchia et al., 1999; interpretation in source apportionment with values of standard
Dickhut et al., 2000; Wang et al., 2007; Wilcke, 2007). performance indices as follows: reduced chi-square (χ2) ≤
Although source apportionment modeling using CMB8.2 4.0, correlation coefficient (R2) ≥ 0.8, 80 < percent mass
was conducted in this study (described subsequently); (PCmass) ≤ 120, t-statistic (t-test) ≥ 2.0, the degrees of
however, the attempt of using characteristic ratios to freedom (DF) > 5, and –2 < ratio of residual to its uncertainty
identify the possible combustion sources would strengthen (R/U) < 2 (Watson et al., 2004). Table S3 presents the
the simulation results of CMB8.2. Table S2 presents the source profiles of 12 PAHs used for CMB8.2 modeling in
details of characteristic ratios used in this study to identify this study.
different responsible sources in the aspect of spatio-seasonal The advantage of the CMB Model over positive matrix
variations. The characteristic ratios used in this study were factorization (PMF) model is with the fact that CMB does
defined as follows: (1) LMW/HMW, (2) BaA/(BaA + Chr), not overestimate emissions or misallocate residual mass
(3) InP/BghiP, and (4) BaP/BghiP. (Teixeira et al., 2015; Bullock et al., 2008). Other advantage
includes the model precision through the use of their
Source Apportionment Through CMB Modeling statistical parameters as mentioned in the last paragraph. In
The source contribution estimates (SCEs) of 12 measured the past, several studies from various countries have
PM2.5-bound PAHs were predicted using the platform of the conducted source apportionment of particulate PAHs using
USEPA-developed CMB8.2. In brief, CMB8.2 finds a CMB Model (Hanedar et al., 2011; Bortey-Sam et al., 2015;
statistical solution to the set of linear equations that expresses Afshar-Mohajera et al., 2016; Manoli et al., 2016).
concentrations of predictor compounds as a sum of the
products of source profile abundances multiplied by the source Exposure Risk Assessment for Human Bodies
contributions, and assuming that no chemical transformation During human health risk assessment due to exposure of
of compounds in the atmosphere takes place after emitted toxic compounds, cancer risk has been considered as a
from sources. For detailed description of approach in making stochastic response, indicating that a rise in the dose of
input files, procedure of simulation process on application chemical does not essentially result in an increase in severity
of this model, and compilation of outputs from simulations, of the response, but the occurrence of probability (Mateos
CMB8.2 User Manual can be referred (Coulter, 2004, and et al., 2018). However, non-cancer risk assessment is
references therein). We identified possible significant sources treated as deterministic, i.e., when increasing the dose, a
of PAHs in the study area as follows: vehicles (petrol, diesel more severe response is expected (Evans, 2003; Mateos et
and CNG engines), industries (thermal power plant, diesel al., 2018). In this study, inhalation exposure pathway of air
generator [DG] sets, coke oven and smelters), domestic particles contaminated with PAHs that can cause cancer was
cooking (liquefied petroleum gas [LPG], coal and wood), considered for assessment of human health risk. We used
MSW burning (plastic, wood and leaves), and BM burning the classification of International Agency for Research on
(wood, crop residue and leaves). Cancer (IARC) of WHO, and identified 7 PAHs, classified
The best suitable source profiles were adopted for as carcinogenic (Group 1; BaP), probably carcinogenic
simulation exercise in CMB modeling based on previous (Group 2A; DahA), and possibly carcinogenic (Group 2B;
reported results. For CMB modeling, we categorized emission BaA, Chr, BbF, BkF, and InP) to humans. Although PAHs
2810 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020

other than these 7 PAHs possess limited carcinogenicity, occurrence of 1 cancer case over 1 million people) was
those PAHs can increase the overall exposure when present considered as significant risk, and cancer risk of more than
in PAH mixtures (Nisbet and Lagoy, 1992; Li et al., 2016; or equal to 1 × 10–4 was considered as unacceptable risk
Pongpiachan, 2016). (U.S. EPA, 2005; Amarillo et al., 2014).
The carcinogenicity potential of each PAH congener
concentration was estimated in terms of BaP-equivalent RESULTS AND DISCUSSION
(BaPeq) concentration to exposure of a mixture of PAHs.
Hence, in estimate of BaP-equivalent concentration of Overall Results with Spatio-seasonal Concentrations of
individual PAH congener, the toxic equivalency factors PM2.5
(TEFs) of 12 PAHs with respect to BaP proposed by Nisbet Considering all individual samples (number of data points
and Lagoy (1992) were used to conduct further carcinogenic [N] = 125) during sampling campaign, the annual average
health risk assessment (Table S4). This is to be noted that concentration of PM2.5 measured in Delhi (313 ± 122 µg m–3)
the same approach has been adopted by several other previous exceeded Indian annual PM2.5 standard of 40 µg m–3 and
studies (Kaur et al., 2013; Pongpiachan, 2016; Majewski et WHO annual PM2.5 standard of 10 µg m–3 by factors of 8
al., 2018). We estimated BaPeq for individual PAH congener, and 31, respectively. The PM2.5 concentration of individual
and then considered the sum of all 12 PAHs for getting the samples ranged from 117 µg m–3 at Semi-urban Site during
BaPeq concentration for each sampling observation at summer to 706 µg m–3 at Urban Industrial Site II during
various sites, as expressed as Eq. (1): winter. From the experimental results, it was observed that
ambient concentrations of PM2.5 at all six sampling sites
n during two seasons (winter and summer) exceeded by 100%
BaP
= eq ∑ C × TEF
i =1
i i (1) time with 24-h Indian air quality standard of 60 µg m–3
(http://www.cpcb.nic.in). With all individual data points
during respective seasons, higher concentrations of PM2.5
where, BaPeq is the BaP-equivalent concentration of all
were observed during winter at 356 ± 131 µg m–3 (N = 64)
PAHs; Ci is the ambient concentration of individual PAH
compared to that of summer at 268 ± 94 µg m–3 (N = 64).
congener i; TEFi is the toxicity equivalency factor of
The seasonal difference of PM2.5 concentration between
individual PAH congener i.
winter and summer was assessed using a paired t-test with
After estimate of BaPeq on each sampling day, the ILCR
unequal variance with the statistical platform of SigmaPlot
(incremental lifetime cancer risk) representing carcinogenic
14.0. The statistical results revealed that PM2.5 concentration
health risk of PAHs was estimated using following numerical
during winter increased significantly compared to that of
equations, expressed as:
summer at 95% level of confidence.
Fig. 2 shows concentration levels of PM2.5 at six sampling
ILCR = [CDI] × [SF] (2)
sites during winter and summer. The average concentration
of PM2.5 during winter at individual sites varied from
  IR × ET × EF × ED × ADAF   281 µg m–3 at Semi-urban Site to 451 µg m–3 at Urban
=  ( Ca ) ×  a
ILCR 
  BW × AT  Industrial-cum-residential Site. Similarly, the values during
(3)
 IUR × BW  summer varied from 240 µg m–3 at Urban Residential Site
×  to 410 µg m–3 at Urban Industrial Site-I. Such trend of higher
 IRb  PM2.5 concentration during winter indicated the prevalence of
calmer atmospheric conditions resulting in lower atmospheric
where CDI, the chronic daily intake, is the life-averaged boundary layer height and dispersion of pollutants (Hoque
daily dose, expressed in ng (kg day)–1; SF, the slope factor, et al., 2008; Saxena et al., 2017). In addition, increase in
is an estimate of the upper-bound probability of a person to levels of fine particles during winter could be associated
develop a cancer as a result of the lifetime exposure to with rise in emission activities, specifically additional energy
certain level of potential carcinogen in ng–1 (kg day); Ca is requirement in thermal power plants, domestic heating and
the BaPeq ambient concentration of PAHs in ng m–3; IRa is burning of wood, coal and charcoal to get rid of severe cold
the breathing/inhalation rate in m3 h–1; ET, the exposure (Nagar et al., 2017; Tyagi et al., 2017). Although concentration
time, is the number of hours per exposure, i.e., h day–1; EF, of PM2.5 during winter at Semi-urban Site were observed to
the exposure frequency, is the number of exposures per year, be only 10% higher than that during summer, the seasonal
i.e., days year–1; ED, the exposure duration, is the duration variation was not significant at 95% level of confidence.
of exposure in years; ADAF is the age-dependent adjustment The trend at this particular site was contrary to other five
factor used in estimate of risk; BW is the body weight of the sites which showed significant seasonal variations. This
receptor in kg; AT, the average time, is average exposure could be due to the fact that resuspension of road dust, fly
extent over a lifetime (days) = average life span (years) × ash and soil-borne particles under higher wind speed had
365; IUR is the inhalation unit risk in (ng m–3)–1; and IRb is significant influence on PM2.5 mass concentrations during
the breathing/inhalation rate in m3 day–1. summer at this semi-urban site. Insignificant concentration
The parameters considered in human health risk assessment difference of PM10 levels between winter and summer at
are presented in Table S5. To designate the results of health some localities in the study area have also been reported by
effects, cancer risk of more than or equal to 1 × 10–6 (i.e., a previous study (Jyethi et al., 2014).
 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020 2811

Fig. 2. Ambient concentration of PM2.5 at six sampling sites during winter and summer. The error bars in PM2.5
concentrations are standard deviations of respective data sets.

On annual average basis, the highest PM2.5 concentration biomass burning those would be more responsible for existing
was observed at Urban Industrial Site I (398 ± 95 µg m–3), levels of PAHs in Delhi. The concentrations of TPAHs of
followed by Urban Industrial-cum-residential Site (366 ± individual samples (N = 125) at six sampling sites ranged
124 µg m–3), and the minimum at Semi-urban Site (242 ± from 1.3 ng m–3 during summer at Urban Residential Site to
73 µg m–3). The trends with such spatial variations confirmed 279.6 ng m–3 during winter at Urban Industrial-cum-
the role of pollution activities such as industries, commercial residential Site.
activities and vehicles in contributing larger mass to ambient With all individual data points during respective seasons,
concentrations of PM2.5. In the perspectives of seasonal higher concentrations of TPAHs were observed during winter
variations, the order of particulate pollution levels at six at 75.1 ± 50.2 ng m–3 (N = 64) compared to that of summer
sampling sites were different during two seasons. The change at 10.4 ± 8.5 ng m–3 (N = 61). Through aforementioned
in order during these two seasons indicated multiple source statistical method, the seasonal difference in concentration
of origins with variations in contributions to overall particulate of TPAHs between winter and summer was assessed using
pollution in Delhi; this fact has also been evidenced in other a paired t-test with unequal variance. The statistical results
studies conducted in Indian cities (Masih et al., 2010; Kaur revealed that concentration of TPAHs during winter increased
et al., 2013; Sarkar and Khillare, 2013). significantly compared to that of summer at 95% level of
confidence. In a similar way, the concentration of individual
Overall Results with Spatio-seasonal Concentrations of marker BaP showed significant seasonal variations at city
PAHs level with higher concentrations during winter than summer.
Considering all individual data points (N = 125) at six Fig. 3 shows concentration levels of TPAHs and BaP at
sampling sites for total polycyclic aromatic hydrocarbons six sampling sites during winter and summer. Seasonal
(sum of 12 measured PAHs), the annual average concentration variations of concentrations of TPAHs and BaP at city level
of TPAHs quantified in Delhi was observed as 44 ± 43 ng m–3. and individual sites were observed with higher concentrations
This average concentration level seemed to be several times during winter than summer at 95% level of confidence. The
higher than that of European cities (refer Table 1 that seasonal variations of concentrations of TPAHs at all sampling
presents relevant results of limited cities across the world). sites confirmed that winter season was more critical for
Many initiative measures including conversion of all public residents in getting exposed to such noxious emerging
transport fleet (transport buses, 3-wheeler motor rickshaw) organic contaminants in Delhi. The concentration ratio of
from diesel to CNG were implemented during 2002 by winter/summer TPAHs varied from 4.1 at Semi-urban Site
governments of Delhi and India to reduce levels of PM and to 18.3 at Urban Residential Site, showing additional sources
its constituents. However, studies reported by some other such as wood, coal and biomass (cow dung, crop residue)
research groups (Sharma et al., 2007; Sarkar and Khillare, burning for space heating in cold nights and meteorological
2013; Jyethi et al., 2014) could not find any strong linkage conditions were responsible for rise in concentrations of
between conversion of diesel-driven vehicles into CNG-driven TPAHs during winter compared to summer. The annual
public vehicles and ambient concentration of PAHs in Delhi. average concentration of BaP was observed as 4.6 ±
Hence, such trends indicated at other emission activities 2.6 ng m–3. With all individual data points during winter and
including increase in diesel- and petrol-driven vehicles, and summer, the percentage of exceedance of 24-h Indian standard
2812 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020

Fig. 3. Ambient concentration of TPAHs and BaP at six sampling sites during winter and summer. The error bars are standard
deviations of respective data sets.

for BaP (1 ng m–3) was estimated. It was found that 95% of and (d) the Terra MODIS true color composite images on
data points during winter and 31% of data points during 26 October 2017 over Punjab state, India. This is to be noted
summer exceeded the Indian 24-h standard of BaP. This is that CRB is a common practice of agricultural waste
to be noted total BaPeq calculated using Eq. (1) considering burning in neighboring states of Delhi (Punjab and Haryana)
all markers of PAHs at individual data points during both during mid-October to mid-November of every year before
the seasons exceeded 1 ng m–3 most of the times (more sowing next slots of crop on agricultural field (Sharma et al.,
explanations are provided in later section). 2010; Thumaty et al., 2015). Moreover, Punjab and Haryana
Semi-urban Site had experienced the lowest concentration regions along with western Uttar Pradesh in the IGP region
of TPAHs (26.1 ± 16.3 ng m–3) and BaP (2.1 ± 1.8 ng m–3), are considered as the rice and wheat bowl of India with
which was about one-third of TPAH levels at remaining five ~12 million hectares of land accounted for rice/wheat crop
sites throughout the sampling campaign during winter. This cultivation. Almost 80% of the rice straw residue (due to its
observation trend was because of the location of Semi-urban inferior quality as a cattle feed) are subjected to open
Site near to a large reserve forest (Central Ridge, Delhi), and burning from mid-October to mid-November every year in
moreover, this site was not severely affected by large traffic more than 60% of agricultural land (Sharma et al., 2010;
and combustion sources. As explained in Fig. 1, some Thumaty et al., 2015).
concurrent measurements were conducted at couple of sites Urban Industrial-cum-residential Site was closer to these
during this sampling campaign. So, we examined the two neighboring states (Punjab and Haryana) compared to
temporal variations of limited data points, where the Urban Industrial Site I. Therefore, samples captured during
concentrations were observed as abnormal compared to third week of November at Urban Industrial-cum-residential
other individual data points. The measurement conducted Site had shown more enhancement in levels of TPAHs
during third week of November 2013 at two sampling sites compared to Urban Industrial Site I. The characteristics of
(Urban Industrial-cum-residential Site and Urban Industrial PAHs are such that those are largely emitted as vapors, and
Site I) generated larger increase in concentrations of TPAHs get quickly adsorbed on condensing carrier particles such as
compared to other four sampling sites. Specifically, sharp soot and fly ash located close to emission site. During winter
increase in concentration of TPAHs was observed for the season, major photodecomposition transformation of PAHs
samples captured on dates of 15, 19, 21, and 23 November cannot happen due to less solar radiation, and hence, PAHs
2013 at Urban Industrial-cum-residential Site, and on dates adsorb on 1 µm particles (Singh et al., 2017). From the
of 15, 19, and 21 November 2013 at Urban Industrial Site I. trends in variations of TPAHs during month of November
To find the reasons for such trend, outside sources were 2013, it was confirmed that transboundary transport of
considered for examination, and maps representing PAHs from CRB hotspots of Punjab and Haryana to Delhi
locations of crop residue burning (CRB) in northern India was possible because of least photochemical degradation of
were used from Terra and Aqua MODIS satellite images TPAHs into their by-products under lower temperature,
(https://visibleearth.nasa.gov/view.php?id=91185). higher relative humidity and lower solar radiation coupled
Fig. S1 shows respective information as follows: (a) fire with prevailing wind direction (NW).
map marked with red dots for crop residue burning in IGP
region for period 3–23 November 2013; (b, c) image from Comparison of Measurement Results with Other Studies
Terra and Aqua MODIS true color composite images on 12 Although comparison of results from this study with
November 2013 of smoke plume over entire IGP region; other studies conducted in the same study area and other
 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020 2813

geographical locations in the world should not be done sources. However, in case of Delhi, the levels of TPAHs
directly, such interpretations sometimes help in understanding were more than levels of TPAHs in Shanghai by 2–4 times.
the trends in ambient concentration levels of PM and Hence, the policy makers and scientific bodies in India
TPAHs. Table 1 presents compiled data of relevant parameters should look into more time-bound action plans for reduction
of observed levels of PM mass and TPAHs at important of TPAH levels in Delhi.
cities across the globe. In the aspects of atmospheric levels
of TPAHs in Delhi, no consistent trend was observed with Variations of Concentrations of Individual PAHs
year of measurement. The studies conducted during 2008– Fig. 4 shows measured mass concentration of individual
2010 for TPAHs in PM10 (Sarkar and Khillare, 2013; Jyethi PAHs at six sampling sites during winter and summer. For
et al., 2014) reported concentration levels with similar clarity in presentation of data, we divided 12 PAHs into two
quantities more than 100 ng m–3. Study done by Singh et al. groups based on their ambient concentrations and plotted
(2012) during 2007–2008 reported TPAHs in PM10 as more them separately. The top 6 PAHs (Phe, Chr, BbF, BaP, InP
than 40 ng m–3. The results from this study was similar to and BghiP) with higher concentrations were plotted
observations by Sonwani (2016) conducted during the same differently from PAHs with lower concentrations (Flu, Ant,
study period. The studies selected for comparison of TPAHs Pyr, BaA, BkF and DahA). The ambient concentrations of
in Delhi have revealed that the atmospheric levels of TPAHs all individual 12 PAHs during winter exceeded significantly
depend on sampling locations, sampling duration, sampling at 95% level of confidence compared to those concentrations
frequency, season of sampling and many other factors. during summer (paired t-test with unequal variance was
The levels of TPAHs observed in Delhi were comparable conducted). Based on all individual samples during sampling
with TPAH levels in other Indian cities such as Amritsar campaign, the ratio of ambient concentration during winter
(154 ± 42 ng m–3; Kaur et al., 2013) and Mumbai (86.2 ± to summer varied from 1.6 (for Ant) to 21.5 (for BkF), with
4.6 ng m–3; Abba et al., 2011). However, the levels of an average of 8.8 for all markers of PAHs.
TPAHs observed in Agra (269 ± 121 ng m–3; Masih et al., Considering all sampling sites for individual markers, the
2010; Rajput and Lakhani, 2012) and Chennai (517.1 ng m–3; highest average concentration level was observed as BghiP
Mohanraj et al., 2011) were much higher than that of Delhi. (14.3 ± 7.4 ng m–3 during winter and 2.5 ± 1.8 ng m–3 during
The levels of TPAHs of Delhi was comparable with Yangtze summer), followed by InP during winter (13.1 ± 7.3 ng m–3)
River Delta, China (51.1 ± 29.8 ng m–3; Zhuo et al., 2017); and BbF during summer (2.1 ± 1.4 ng m–3). As the
Nanjing, China (58.2 ng m–3; He et al., 2014); Istanbul, concentration levels of BghiP and InP during winter at all
Turkey (73.5 ± 40.4 ng m–3; Hanedar et al., 2014); Tehran, sampling sites were higher compared to concentration levels
Iran (115.7 ± 58.2 ng m–3; Hoseini et al., 2016), and Alexandria, of remaining markers, large contribution from vehicular
Egypt (133.5 ± 89.5 ng m–3; Khairy and Lohmann, 2013), sources (gasoline and diesel) to ambient levels of PAHs
indicating similar source problems of PAH contamination were indicated in Delhi (Ravindra et al., 2008; Chen et al.,
are being faced by these cities. The ambient air in Seoul, 2016; Fan et al., 2016). In addition to the above observation
South Korea (11.6 ± 11.5 ng m–3; Choi et al., 2016); Riyadh, on higher concentrations of BghiP, InP and BbF, it was also
Saudi Arabia (18.4 ± 61.1 ng m–3; Bian et al., 2016); assessed that Phe (9.7 ± 6.2 ng m–3) followed by BaP (8.3 ±
Brisbane, Australia (19.6 ± 2.9 ng m–3; Mishra et al., 2016), 4.3 ng m–3) and Chr (6.9 ± 3.6 ng m–3) were also recorded
and Shanghai, China (21.2 ± 17.1 ng m–3; Liu et al., 2016) as next three higher concentrations during winter, indicating
contain less levels of TPAHs than cities in India, Iran, Egypt that emissions from both traffic and domestic combustion
and Turkey. of organic materials (biomass burning) such as wood, cow
Examining TPAH levels of European cities in Greece, Spain, dung and crop residue occurred in the study area (Fan et al.,
Portugal and Italy, North American city (Atlanta, USA), 2016; Yang et al., 2017). The decrease in concentrations of
South American city (Cordoba, Argentina), it was assessed markers of PAHs during summer could be attributed to
that these cities had less ambient concentrations of TPAHs usage of less residential fuel combustion for heating, and
by several orders compared to Asian or African cities. The greater photolytic and thermal decomposition of PAHs due
levels of TPAHs of urban areas in Japan (2.5 ± 1.3 ng m–3; to prevailing meteorological conditions during warmer months
Tham et al., 2008), Malaysia (2.7 ± 1.4 ng m–3; Jamhari et (Vasilakos et al., 2007; Liu et al., 2016). Concentrations of
al., 2014), Taiwan (2.9 ± 1.4 ng m–3; Chen et al., 2016) and markers of PAH can be affected by photochemical oxidations
Hong Kong, China (3.5 ± 0.9 ng m–3; Fan et al., 2017), were prompted by solar radiation and carried out by a number of
less polluted by several orders compared to other cities of atmospheric oxidants such as ozone, NO, NO2 and hydroxyl
Asian countries. Thus, this trend of ambient concentration radicals, which decompose PAHs during the warmest seasons
of TPAHs in these Asian cities confirmed that these cities (Manoli et al., 2016; Vasilakos et al., 2007). In addition, the
were cleaner cities and better air quality were maintained semi-volatile nature of PAHs can cause more adsorption of
similar to European and North American cities. In similar HMW-PAHs on particle surfaces due to lower temperature
Asian cities, Delhi and Shanghai had common air pollution and higher relative humidity those increased levels of PAHs
problems with more severity causing occurrence of hazier during winter compared to summer (Manoli et al., 2016).
days in these two large urban areas. The levels of TPAHs in Similar seasonal pattern for concentrations of markers of
Shanghai indicated that regulating the levels of TPAHs PAH has also been reported in other past studies (Mantis et
through effective implementation of stringent laws by al., 2005; Chrysikou and Samara, 2009; Pietrogrande et al.,
policy-making bodies to reduce activities at polluting 2011; Yang et al., 2017).
 2814
Table 1. Comparison of results of PM and TPAHs with other studies conducted in different urban areas of the world (mean ± standard deviation, and range).
Particle PM mass (µg m–3) TPAHs (ng m–3)
Study area Study period Reference
size (Mean ± SD) Range (Min–Max) Mean ± SD
Delhi 2013–2014 PM2.5 313 ± 122 1.3–279.6 43.8 ± 42.8 Present study
Delhia 2013–2014 PM10 193 ± 90 15.0–161.0 48.2 ± 33.9 Sonwani (2016)
Delhib 2009–2010 PM10 222 ± 30 38.4–213.7 103.4 ± 51.2 Jyethi et al. (2014)
Delhic 2008–2009 PM10 178 ± 63 43.2–219.4 105.3 ± 84.9 Sarkar and Khillare (2013)
Delhid 2007–2008 PM10 147 11.0–105.3 46.9 ± 12.0 Singh et al. (2012)
Amritsar* 2011 PM10 NA 37.0–274.0 154 ± 42 Kaur et al. (2013)
Agra 2006 TSPM 400 ± 129 150.0–480.0 269 ± 121 Rajput and Lakhani (2012)
Mumbai† 2007–2008 PM2.5 84 ± 31 NA 86.2 ± 4.6 Abba et al. (2011)
Chennai% 2009–2010 PM2.5 92 121.1 ̶ 1,371.5 517.1 Mohanraj et al. (2011)
Lumbini, Nepal%% 2013–2014 TSP 209 ± 123 16.8–193 95 ± 55 Chen et al. (2016a)
Kathmandu, Nepal%%% 2013–2014 TSP 199 ± 124 18.1–453 155 ± 130 Chen et al. (2015)
Tehran, Iran$ 2013–2014 PM10 83 ± 14 49.4–204.6 115.7 ± 58.2 Hoseini et al. (2016)
Riyadh, Saudi Arabia 2011–2012 PM10 NA 0.1–515.8 18.4 ± 61.1 Bian et al. (2016)
Istanbul, Turkey$$ 2006–2007 TSP 71 ± 57 7.1–283.3 73.5 ± 40.4 Hanedar et al. (2014)
Hong Kong, China 2014 PM2.5 34 ± 10 NA 3.5 ± 0.9 Fan et al. (2017)
Shanghai, China¥ 2012–2013 PM2.5 NA NA 21.2 ± 17.1 Liu et al. (2016)
Yangtze River Delta, China# 2014–2015 PM10 NA NA 51.1 ± 29.8 Zhuo et al. (2017)
Nanjing, China## 2009–2010 PM2.1 NA NA 58.2 He et al. (2014)
Changhua County, Taiwanψ 2014–2015 PM2.5 32 ± 20 2.9–3.0 2.9 ± 1.4 Chen et al. (2016b)
Malaysia$$$ 2010–2011 PM10 39 ± 8 1.3–4.8 2.7 ± 1.4 Jamhari et al. (2014)
Higashi Hiroshima, Japan¥¥ 2006–2007 PM10 NA NA 2.5 ± 1.3 Tham et al. (2008)
Seoul, South Korea 2010–2011 PM10 NA 0.5–59.3 11.6 ± 11.5 Choi et al. (2016)
Alexandria, Egypt†† 2010–2011 SPM NA 14.0–420.0 133.5 ± 89.5 Khairy and Lohmann (2013)
Cordoba, Argentina††† 2011–2013 PM10 98 ± 72 0.1–37.7 4.5 ± 4.3 Amarillio et al. (2017)
Spain### 2013 PM10 NA 1.2–9.8 3.2 ± 3.1 Elorduy et al. (2016)
Thessaloniki, Greece€ 2011–2012 PM2.5 42 ± 14 0.1–36.0 6.5 ± 4.3 Manoli et al. (2016)
Oporto, Portugal*** 2007–2008 PM2.5 NA 0.4–21.3 4.7 Slezakova et al. (2013)
Rome, Italyψψ 2011–2012 PM2.5 22 ± 5 0.3–14.3 3.9 ± 1.6 Romagnoli et al. (2017)
Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020

Atlanta, USAψψψ 2004 PM2.5 NA 0.4–6.9 2.2 Li et al. (2009)

Brisbane, Australia€€ 2010–2012 PM0.1 NA 0.4–43.4 19.6 ± 2.9 Mishra et al. (2016)
For reported data: Mean: average; SD: standard deviation; Min: minimum; and Max: maximum. NA: data not applicable/provided; TPAHs: sum of concentrations of all PAHs reported in
respective studies; PM10: particulate matter with aerodynamic diameter ≤ 10 µm; SPM: suspended particulate matter; TSPM: total suspended particulate matter.
a Average of two sites during two seasons for 10 PAHs. b Average of sampling for whole year for 10 PAHs. c Average of sampling for whole year (three seasons) for 16 PAHs. d Average of

sampling for whole year for particulate contents only for 12 PAHs. * Average of six sites during winter for 14 PAHs. † Average of four sites during post-monsoon for 16 PAHs. % Average
of four sites for 11 PAHs. %% Annual average for 15 PAHs. %%% Annual average for 15 PAHs. $ Average of ten sites for 16 PAHs. $$ Average of three sites for 16 PAHs. ¥ Average of four
seasons for 16 PAHs. # Average of four seasons for 16 PAHs, and data of both gas and particles. ## Average of four seasons at all sites for 16 PAHs. ψ Average of two sites for 22 PAHs. $$$
Average of three sites during four seasons for 16 PAHs. ¥¥ Average of four seasons for 13 PAHs. †† Average of two seasons for particulate contents only for 22 PAHs. ††† Average of three
seasons for 14 PAHs. ### Average of all durations for 13 PAHs. € Average of two sites during two seasons for 13 PAHs. *** Data of two sites for 17 PAHs. ψψ Data from urban background
site during two seasons for 8 PAHs. ψψψ Average of three sites for whole year for 28 PAHs. €€ Average during whole sampling period for 16 PAHs.
 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020 2815

Fig. 4. Measured mass concentration of individual PAHs at six sampling sites during winter and summer. The error bars are
standard deviations of respective data sets.

The total BaPeq concentration at each sampling site during 0.9 ng m–3, respectively. The markers, BaP, DahA, BbF and
every season was estimated as the sum of concentrations of InP were the major carcinogenic toxins among 12 PAHs,
individual PAH multiplied by their respective TEFs (refer comprising (annual average) of 60.1%, 15.9%, 9.6%, and 9.1%
Eq. (1) and Table S4 for estimation details). In other words, of total carcinogenic toxicity, respectively. Overall, the
the carcinogenic potency of total PAH mass concentrations descending order of carcinogenic toxicity on annual basis at
was represented as total BaPeq. The average total BaPeq the study area followed the sequence as: BaP > DahA > BbF
concentrations of 12 PAHs at six sampling sites during > InP > BaA > BkF > BghiP > Chr > Phe > Pyr > Flu > Ant.
winter and summer were 13.9 ± 8.9 ng m–3 and 1.4 ± On annual basis at city level, average contribution of
2816 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020

HMW-PAHs (sum of 4-, 5-, and 6-ring PAHs) was observed summer, indicating that petroleum sources were predominant
as 82.5% to total mass concentration of all 12 markers sources at that site; (ii) some data points of estimated
(TPAHs). The range of contribution of HMW-PAHs to BaA/(BaA + Chr) ratio at Urban Industrial-cum-residential
TPAHs varied from 67.2% to 94.3% during winter and from Site, Urban Industrial Site I and Urban Residential Site >
78.1% to 87.2% during summer at six sampling sites. Such 0.35 during winter, indicating that combustion sources were
higher percentage contributions of HMW-PAHs to TPAHs predominant sources on those days; (iii) most of the data
indicated occurrence of more human health implications in points of estimated BaA/(BaA + Chr) ratio at Urban Industrial
the study area, as HMW-PAHs represent all probable and Site II were in the range from 0.2 to 0.35, indicating that
possible carcinogenic species of PAHs. On the other hand, both petroleum and combustion sources were responsible
average contribution of LMW-PAHs (sum of 3-ring PAHs) for prevailed ambient concentrations of PAHs. For example:
was 17.5% to total mass concentration TPAHs. Such lower (i) average BaA/(BaA + Chr) ratio < 0.2 at Urban Commercial-
concentration of LMW-PAHs indicated PAHs in the study cum-residential Site during summer, indicating that petroleum
area were predominately in particulate phase and having sources were predominant sources at that site; (ii) some data
less semi-volatile components (Singh et al., 2012; Jeong et points of estimated BaA/(BaA + Chr) ratio at Urban Industrial-
al., 2017). Although LMW-PAHs have weaker carcinogenicity, cum-residential Site, Urban Industrial Site I and Urban
they react very actively with other pollutants in the air to Residential Site > 0.35 during winter, indicating that
form more toxic secondary species such as nitro-PAHs combustion sources were predominant sources on those days;
(Hanedar et al., 2011; Alegbeleye et al., 2017). Hence, from (iii) most of the data points of estimated BaA/(BaA + Chr)
regulation point of view, both HMW- and LMW-PAHs ratio at Urban Industrial Site II were in the range from 0.2
should be targeted for their possible control in the study area. to 0.35, indicating that both petroleum and combustion
sources were responsible for prevailed ambient concentrations
Characteristic Ratios of PAHs of PAHs.
Fig. 5 shows the estimated values of respective characteristic To segregate further between sources of gasoline and
ratios used in this study for identification of predominant diesel combustions, InP/BghiP ratio was estimated (Yassaa
sources at six sampling sites during winter and summer. et al., 2001; Jytehi et al., 2014). It was found that the average
Considering all individual data points at six sampling sites, of mean at six sampling site was 0.66 ± 0.32 (range: 0.2–
the ratio of LMW to HMW of PAHs ranged from 0.1 to 2.6, 1.1) during winter and 0.47 ± 0.26 (range: 0.2–0.7) during
suggested that both pyrolytic and petrogenic combustion summer. Such trends in individual data points of sampling
sources prevailed in the study area. Some single data points sites indicated that both gasoline and diesel combustions
with LMW/HMW ratio > 1.0 during winter sampling period were responsible for the prevailed ambient concentrations
indicated predominant contributions of BM burning to of PAHs. For finding the distinction of indicative sources
ambient concentrations of PAHs. In the meanwhile, with between vehicles and coal combustions, BaP/BghiP ratio
average of data points of six individual sampling sites, it was estimated for individual data points at six sampling sites
was revealed that mean of LMW/HMW ratio was 0.3 ± 0.7 during winter and summer. The BaP/BghiP ratio ranged
during winter and 0.3 ± 0.4 during summer. Such more from 0.31 to 0.96, suggested that depending on characteristics
variable data points of winter compared to summer confirmed of any specific sampling site, vehicles and/or coal combustion
that additional sources including crop residue, wood and sources were responsible for ambient concentrations of
MSW burning were among responsible contributors to PAHs in the study area. The estimated value of average
ambient concentrations of PAHs during winter. The high BaP/BghiP ratio at six sampling sites was 0.74 ± 0.27 and
percentage of PAHs with a high molecular weight (lower 0.42 ± 0.26 during winter and summer, respectively. Overall,
value of LMW/HMW ratio) indicated that the predominant it was observed that vehicles were the dominating source
PAH sources were involved with high-temperature followed by MSW burning, BM burning, coal combustion
processes, such as combustion of fuels in engines (Amarillo sources with significant contributors to PAHs in Delhi.
et al., 2014; Fan et al., 2017).
Based on past studies (Soclo et al., 2000; Yunker et al., Source Apportionment Results
2002; Mishra et al., 2016) conducted in other parts of the After successful simulation in the platform of CMB8.2,
world, it has been conceptualized that: (i) if estimated ratio, the output data fulfilling the norms set for standard
BaA/(BaA + Chr), is less than 0.20, the responsible sources performance indices (explained in Section 2.5) were
may be dominated by petrogenic (petroleum); (ii) if considered for calculation of SCEs of individual sources at
estimated BaA/(BaA + Chr) ratio ranges from 0.20 to 0.35, each of the sampling sites for both seasons. In the aspects of
the responsible sources may be either petroleum or combustion spatial and seasonal variations of SCEs of major sources,
sources; (iii) if BaA/(BaA + Chr) ratio > 0.35, the responsible the predicted ambient air concentrations of PAHs were
sources may be dominated by combustion sources (coal considered for quantitative source apportionment analysis.
combustion). Considering all individual data points at six Four major source groups identified by CMB8.2 were
sampling sites, BaA/(BaA + Chr) ratio ranged from 0.14 to vehicles, MSW burning, BM burning and coal burning.
0.41, suggested that petroleum and/or combustion sources Further analysis of apportioned major sources with success-
were responsible for ambient concentrations of PAHs in the based acceptable CMB8.2 outputs were performed to
study area. For example: (i) average BaA/(BaA + Chr) ratio examine the break-up of major sources. Hence, classification
< 0.2 at Urban Commercial-cum-residential Site during of major sources was done to estimate SCEs of those
 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020 2817

Fig. 5. Characteristic ratios of PAHs at six sampling sites during winter and summer. The error bars are standard deviations
of respective data sets.

sources as follows: (i) vehicles into petrol, diesel and CNG; Khillare, 2013). Findings from other megacities, such as
(ii) BM burning into CRB and wood; (iii) coal burning into Shanghai, China (38–43%; Liu et al., 2016); Brisbane,
power plant, and domestic cooking and heating; and (iv) Australia (56%; Mishra et al., 2015), and Kütahya, Turkey
others into LPG, DG sets and unidentified mass. (47.3%; Dumanoglu et al., 2017), also confirmed that our
Fig. 6 shows annual and seasonal results of source prediction of vehicles as dominant source of contribution to
apportionment with a break-up of major emission sources, PM2.5-bound TPAHs was rational. The annual sub-break-up
and their sub-break-ups with aforementioned classification. of SCE of the predominant source, vehicles, was calculated
The pie charts show average of SCEs of major predicted as 84%, 12%, and 4%, respectively, by gasoline-, diesel-,
sources in percentage (%), and the sub-break-up of major and CNG-driven vehicles. Delhi has a large fleet of vehicles
sources in percentage at six sampling sites. Annual average powered by gasoline fuel (~90% of total vehicular fleet)
SCE of every source was calculated considering predicted such as 2-wheeler motorbikes and scooters, passenger cars
values of both winter and summer concentrations. Bar chart and taxis (Economic Survey of Delhi, 2017). In comparing
shows spatial distribution of predicted mass (ng m–3) for such predicted results of SCEs with dominance by gasoline-
major sources (vehicles, BM burning, MSW burning, coal driven vehicles, we found that the emission factor profiles
burning and others). The average annual values of SCEs developed by U.S. EPA for on-road gasoline engines
from major emission sources predicted through CMB8.2 indicated that gasoline-fueled vehicles could emit 80–90%
were 62%, 15%, 11%, and 4%, respectively, by vehicles, of HMW-PAHs (USEPA, 2015). Hence, the values of SCEs
MSW burning, BM burning and coal burning. The annual from gasoline-driven vehicles during winter and summer
average value of SCE from source category of others was were identified as dominant source among all categories
predicted as 8% to TPAH mass, and this source category (gasoline, diesel and CNG) of major source, vehicles. In
was possibly expected by various minor sources such as specific, the range of spatial variations of SCEs from
LPG combustion, DG sets, resuspension of road dust and gasoline varied from 84% to 87%, followed by diesel (from
other fugitive emissions. 9% to 13%), and CNG (from 3% to 4%) to TPAHs emitted
A few studies conducted in the study area reported in the from vehicles.
past have observed similar trends in SCE values from vehicles Next to vehicles, it was observed that MSW burning was
(predominant source) to ambient concentration of TPAHs, the second largest source (annual average: 15%) in
e.g., 59.5% (Jyethi et al., 2014) and 62–83% (Sarkar and contribution to TPAHs. Such significant value of SCE from
2818 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020

Fig. 6. Source apportionment results with a break-up of specific emission sources. The error bars are standard deviations of
respective data sets. Abbreviations for sub-break-ups in pie charts: P: petrol; D: diesel; CNG: compressed natural gas; CRB:
crop residue burning; W: wood burning; PP: power plant; DC & H: domestic cooking and heating; LPG: liquefied natural
gas; DG: diesel generator sets; and UI: unidentified mass.

MSW burning was due to open burning of 2–3% of total subjected to smoldering that can contribute significantly to
generated MSW in Delhi due to lack of disposable concentration of PAHs in Delhi. Higher average value of
infrastructure and public awareness (Nagpure et al., 2015). SCE from MSW burning was observed during winter (16%)
At present, half of total MSW (4,611 tons day–1) are disposed than summer (11%). The reason for such higher contribution
into three large solid waste disposal sites, i.e., Bhalswa, from MSW burning to ambient concentrations of TPAHs
Ghazipur and Okhla in Delhi, which have exceeded their could be due to enhanced burning of combustibles such as
capacities way back in 2008. As a result, solid wastes are paper, plastics and tires for space heating in lower socio-
overflowing and most of the wastes are generally disposed economic areas during winter (Jyethi et al., 2014; Nagpure
without any pre-treatment which can often be seen as et al., 2015). Despite large emissions of LMW-PAHs like
 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020 2819

Flu and Phe from MSW combustion (weaker carcinogenicity), SCE from others was predicted as 8% to ambient
significant levels of HMW-PAHs (more carcinogenicity) concentrations of TPAHs, and the sub-break-up sources
such as BaA, InP and BaP are also emitted especially from were identified as LPG, DG sets and unidentified.
plastic burning (Park et al., 2013). Hence, MSW burning is
a matter for concern for the scientific and policy-making Human Exposure Health Risk Assessment
bodies to find the control ways in regulating occurrence of To conduct human health risk assessment, we assumed
MSW burning in Delhi. the ambient concentrations of PAHs during the whole year
Unlike the seasonal trends in values of SCEs from as follows: (i) The mean concentrations of PAHs during
vehicles and MSW burning, it was found that contribution winter at each of the sites were the same for a duration of
of BM burning to TPAHs was mostly observed during winter. 150 days to account for all winter days during October–
The annual average value of SCE from BM burning (CRB February; (ii) the mean concentrations of PAHs during
and wood) was predicted as 11% to TPAHs, with sub-break- summer at each of the sites were the same for a duration of
up as CRB, 44%, and wood burning, 56%. Higher contribution 120 days to account for summer days during March–June;
of BM burning was observed at Urban Industrial-cum- and (iii) the mean concentrations of PAHs during monsoon
residential Site (34.6%) compared to other sampling sites at each of sites were 30% of mean concentration of summer
(7.1–18.5%). The reason was due to addition of pollutants for a duration of 95 days to account for monsoon days
through medium- to long-range transport of air coming from during July–September. The WHO has estimated inhalation
crop residue burning (mid-October to mid-November) in unit risk of BaP at 8.7 × 10–5 (ng m–3)–1 based on an
upwind states of Punjab and Haryana, and in surrounding epidemiology study on coke oven workers in Pennsylvania
areas of NW Delhi. The predicted contribution from wood (WHO, 2000). The IUR value from WHO was used for
burning was more than CRB to total BM burning emissions estimate of excess PAH-induced incremental lifetime cancer
in winter in Delhi. The values of SCEs from BM burning at risk (ILCR), and the final estimate values was abbreviated
other sampling sites during December–February months as ILCR.
was observed in the decreasing order as Urban Residential Site Fig. 7 shows the results from ILCR assessment for human
(18.5%) > Urban Commercial-cum-residential Site (15.6%) > exposure to particulate PAHs of adults staying near to six
Urban Industrial Site II (10.0%) > Semi-urban Site (7.1%), sampling sites. Our estimate of ILCR for adults varied in
which indicated that BM burning gradually decreased as the range from 102 (at Semi-urban Site) to 788 (at Urban
winter approached its end during February. Industrial-cum-residential Site) in 1 million. We compared
Coal burning was identified as a minor contributor our results with previous reported studies. Sarkar and
(annual average SCE as 4%) to TPAHs in Delhi. Out of two Khillare (2013) reported a cancer risk ranging between 30
practice of coal burning (thermal power plant, and remaining and 2,340 in 1 million in Delhi. Hong et al. (2016) reported
under domestic cooking and heating sub-category), coal that lifetime cancer risk varied from 9.1 to 720 in 1 million
burning was identified as a major fuel used in domestic in Indian cities. Liu et al. (2007) reported PAH-induced
cooking and heating, hotels and restaurants in tandoors inhalation cancer risk of 583 per 1 million people for Beijing
(cylindrical clay oven) for baking bread (chapati), and traffic police and 416 per 1 million people. Ramirez et al.
roasting/grilling meat in Delhi. The value of annual average (2009) estimated ILCR of 120 in 1 million in southern Europe.

Fig. 7. Results for cancer health risk assessment of humans staying near six sampling sites.
2820 Yadav et al., Aerosol and Air Quality Research, 20: 2805–2825, 2020

and Mediterranean area due to exposure to particulate PAHs contributed 62% of the average annual PAH
Most of the regulatory bodies cite an ILCR between 10–6 concentrations, whereas MSW, BM and coal combustion
(1 in 1 million) and 10–4 (100 in 1 million) for potential risk, contributed 15%, 11% and 4%, respectively. BM burning,
whereas ILCR greater than 10–4 (100 in 1 million) indicates which increased the ambient PAH concentrations, was
higher potential health risk. Hence, it was inferred that mainly observed during winter (November–February).
inhabitants staying in the study area were at higher risk of ● The ILCR for adults (between 16 and < 70 years of age)
potential health implications of getting cancer during their averaged 423 per 1 million persons across the total study
life span. area during the sampling period. However, the individual
The estimated ILCR was the highest at Urban Industrial- sites displayed ILCR values ranging from 102 (at the
cum-residential Site (7.88 × 10–4) followed by Urban semi-urban site) to 788 (at the urban industrial-cum-
Industrial Site I (6.19 × 10–4) with minimum at Semi-urban residential site) per 1 million persons, indicating that
Site (1.02 × 10–4). Such trends in spatial variations of ILCR proximity to roads and industry exacerbates the risk
in the study area indicated that people staying in the areas through increased exposure to PM2.5-bound PAHs.
with higher vehicular and industrial activities would be more
prone to occurrence of cancer through exposure to particulate ACKNOWLEDGEMENTS
PAHs. The BaP and DahA were found to be contributing
the highest to ILCR compared to all other markers of PAHs The measurements of mass concentration levels of PM2.5
at all sampling sites ranging between 10–5 and 10–3. Although and PM2.5-bound PAHs were part of the project supported
Phe, BbF, InP and BghiP had the higher contribution to total by regulatory bodies of Delhi. The authors gratefully
PAHs concentration at all sites during winter, the ILCR acknowledge the Government of National Capital Territory
posed by them varied in the range of 10–9 to 10–5 due to their of Delhi (NCTD) and Delhi Pollution Control Committee
low carcinogenic potential compared to BaP and DahA (DPCC), Delhi, for their financial support. The data analysis,
(Ramirez et al., 2011). Hence, MSW burning which computational modeling, and human health risk assessment
contributes large amount of Phe and Pyr to the ambient air, were conducted in research collaboration between teams of
was a lower threat to the public health risk than vehicles and Indian Institute of Technology Kanpur (IITK), and Shiv
biomass burning. Nadar University (SNU), Greater Noida.

CONCLUSIONS AUTHOR CONTRIBUTIONS

This comprehensive field campaign, which was conducted The chemical analysis, data generation, and modeling
at six sampling sites in Delhi during winter and summer, were done by A. Yadav. Data processing, interpretation,
analyzed 12 priority PAHs and evaluated their spatio- modeling and manuscript development were done by S.N.
temporal and seasonal variation, sources and health risks. Behera. Chemical analysis and modeling were supported by
Our conclusions are summarized as follows: P.K. Nagar. The sampling campaign and analytical facilities,
● The average annual PM2.5 concentration measured in overall design and supervision were provided by M. Sharma.
Delhi (313 ± 122 µg m–3) exceeded the Indian standard All authors read and agreed for the final submission of this
(40 µg m–3) and the WHO standard (10 µg m–3) by manuscript to Journal, Aerosol and Air Quality Research.
factors of 8 and 31, respectively. The concentration
ranged from 117 µg m–3 at the semi-urban site during COMPETING INTERESTS
summer to 706 µg m–3 at one of the urban industrial sites
during winter, confirming a relationship between The authors declare no competing interests exist.
vehicular and industrial activity and ambient PM2.5.
● The TPAH concentration ranged from 1.3 ng m–3 at the SUPPLEMENTARY MATERIAL
urban residential site during summer to 279.6 ng m–3 at
the urban industrial-cum-residential site during winter. Supplementary data associated with this article can be
The ratio for the winter/summer concentrations varied found in the online version at https://doi.org/10.4209/aaqr.2
from 4.1 at the semi-urban site to 18.3 at the urban 020.04.0182
residential site, suggesting that wood, coal and biomass
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