Environmental Pollution 238 (2018) 431e439

Contents lists available at ScienceDirect

Environmental Pollution
journal homepage: www.elsevier.com/locate/envpol

Assessment of airborne polycyclic aromatic hydrocarbons in a

megacity of South China: Spatiotemporal variability, indoor-outdoor
interplay and potential human health risk*
Yuan-Jie Hu a, d, Lian-Jun Bao b, *, Chun-Li Huang b, Shao-Meng Li c, **, Peter Liu c,
Eddy Y. Zeng b
a
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, 510640, China
b
School of Environment and Guangdong Key Laboratory of Environmental Pollution and Health, Jinan University, Guangzhou, 511443, China
c
Air Quality Research Division, Environment and Climate Change Canada, 4905, Dufferin Street, Toronto, Ontario, M3H5T4, Canada
d
University of Chinese Academy of Sciences, Beijing, 100049, China

a r t i c l e i n f o a b s t r a c t

Article history: Although a number of studies have assessed the occurrence of atmospheric polycyclic aromatic hydro-
Received 21 December 2017 carbons (PAHs) in indoor environment, few studies have systemically examined the indoor-outdoor
Received in revised form interplay of size-dependent particulate PAHs and potential health risk based on daily lifestyles. In the
24 February 2018
present study, size-dependent particle and gaseous samples were collected both indoors and outdoors
Accepted 13 March 2018
within selected schools, offices and residences located in three districts of Guangzhou, China with
different urbanization levels during the dry and wet weather seasons. Results from measurements of
PAHs showed that higher total PAH concentrations occurred in residential areas than in other settings
Keywords:
Polycyclic aromatic hydrocarbons
and in indoor than in outdoor environments. Compositional profiles and size distribution patterns of
Size distribution particle-bound PAHs were similar indoors and outdoors, predominated by 4-and 5-ring PAHs and the
Indoor and outdoor exchange 0.56e1.0 mm particle fraction. Statistical analyses indicated that outdoor sources may have contributed to
Respiratory exposure 38e99% and 62e100% of the variations for indoor particle-bound and gaseous PAH concentrations,
Potential health risk respectively. Incremental life cancer risk (ILCR) from human exposure to indoor and outdoor PAHs based
on different lifestyles followed the order of adults > children > adolescents > seniors. All average ILCR
values for four age groups were below the lower limit of the Safe Acceptable Range (10
6). In addition,
the ILCR value for adults (average: 7.2  10
7; 95% CI: 5.4  10
8‒2.5  10
6), estimated from outdoor air
PAH levels with 24-h exposure time, was significantly higher than our assessment results (average:
5.9  10
7; 95% CI: 6.3  10
8‒1.9  10
6), suggesting the significance of assessing human inhalation
exposure risks of indoor and outdoor PAHs in urban air based on daily lifestyles.
© 2018 Elsevier Ltd. All rights reserved.

1. Introduction from human activities and related harmful effects in daily life
(Destaillats et al., 2008; Rivas et al., 2014; Williams et al., 2000). A
Environmental quality has been deteriorating during the last great example is air pollution within indoor settings, as the general
few decades, partly due to the manufacture and consumption of population spends approximately 90% of the time indoors and
increased amounts of chemicals and inappropriate disposal of therefore is more exposed to pollution indoors than outdoors
obsolete consumer products. Growing concerns have been raised (Klepeis et al., 2001). The situation is even worse for certain
about the levels of hazardous contaminants constantly emitted vulnerable groups such as the elderly, children and the sick.
Another issue is how much outdoor pollution contributes to indoor
loadings and vice versa, which has not been adequately addressed.
*
This paper has been recommended for acceptance by David Carpenter.
Although indoor pollutants are complex and diversified, poly-
* Corresponding author. cyclic aromatic hydrocarbons (PAHs) have remained the most
** Corresponding author. abundant and therefore are most relevant for human health effects
E-mail addresses: [email protected] (L.-J. Bao), [email protected] (Kim et al., 2013). They are mainly generated from incomplete
(S.-M. Li).

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432 Y.-J. Hu et al. / Environmental Pollution 238 (2018) 431e439

combustion of carbonaceous materials from natural and anthro- 2.2. Sample collection
pogenic sources, including industrial, traffic and residential emis-
sions (Kim et al., 2012; Liu et al., 2001). The amount of PAHs emitted Nine school, office and residence sites, located at the districts of
from China was 106 Gg in 2007, accounting for 21% of the total Tianhe, Luogang and Zengcheng representative of substantial,
global amount, of which 62% was from residential activities (Chen moderate and light urbanization, respectively, were selected for
et al., 2017; Shen et al., 2013). Atmospheric PAHs are often a com- sample collection. Detailed procedures about the sample collection
plex mixture distributed between the particle and gaseous phases are presented in Text S1 (“S” indicates texts, tables and figures in
and can cause bronchitis, asthma, lung cancer and atherosclerosis the Supplementary material afterwards). A total of 550 particles
in human through inhalation exposure (Farmer et al., 2014). samples (50 samples containing 11 size fractions) and 50 gaseous
Despite numerous efforts in evaluating indoor and outdoor samples, including duplicate samples, were collected with a Micro-
airborne PAHs and associated human health risks, there is a paucity Orifice Uniform Deposit Impactor (MOUDI; MSP Corporation,
of the systemic assessment with daily life scenarios in current Shoreview, MN, USA) connected to a stainless steel unit containing
datasets. We compiled 457 publications (data from Web of Science) polyurethane foam (PUF). Gaseous samples (PUFs) were sealed
on the occurrence of and human exposure to indoor atmospheric consecutively with plastic zipper closed bags and lightly vacuum
PAHs from 2007 to 2017, 20% of which focused on residential air plastic bags, and particle samples were kept in membrane cell
PAHs levels. Besides, only one study was conducted to determine holders immediately after sampling. All samples were cooled with
atmospheric PAH concentrations in multiple indoor microenvi- ice during transport to the laboratory and were stored at
20  C
ronments such as schools, homes, offices, hospitals, cars and buses until analysis.
(Romagnoli et al., 2014). As the event time duration in a specific
exposure scenario is a key input parameter, assessments based on a 2.3. Sample extraction and instrumental analysis
single indoor microenvironment may underestimate or over-
estimate the potential health risk. Although particle-bound PAHs Both glass fiber filters (47 mm diameter and 1.6 mm aperture)
are the major contributor to inhalation exposure to airborne PAHs and PUFs loaded with particulate and gaseous PAHs, respectively,
in indoor environment (Delgado-Saborit et al., 2011). Size- were spiked with the surrogate standards before extraction. Loaded
dependent exposure to particle-bound PAHs has not been well filters were sonicated three times with 20 mL of hexane,
characterized because total particles were often collected by high- dichloromethane and acetone mixture (2:2:1 in volume) and PUFs
volume air samplers (Ellickson et al., 2017; Guo et al., 2003; Shi were Soxhlet-extracted for 48 h with 200 mL of the same mixed
et al., 2003). To our best knowledge, only our previous study solvent. Each extract was concentrated, solvent-exchanged to
(Zhang et al., 2012a) has evaluated inhalation exposure to size- hexane and further concentrated with a Zymark TurboVap 500
fractionated particle-bound PAHs in indoor environments in (Hopkinton, MA, USA). The gaseous sample extracts were purified
Guangzhou, but the sampling size was limited. consecutively with a glass column (with an internal diameter at
Amid the above-mentioned knowledge gap, the present study 0.8 cm) packed with 5 cm neutral silica gel and 1 cm anhydrous
was conducted to simultaneously evaluate the occurrence of indoor sodium sulfate from bottom to top. The fraction containing target
and outdoor airborne PAHs and human health risk from inhalation PAHs was eluted with 15 mL of hexane, and the extract was
exposure to PAHs. Three typical types of urban settings (school, concentrated to 1 mL and spiked with the internal standards before
office and residence) within three districts with different urbani- instrumental analysis.
zation levels in Guangzhou of China were selected for field sam- All samples were analyzed with a Shimadzu gas chromatograph
pling. The spatial and temporal distribution of airborne PAHs, coupled to a mass spectrometer (GCMS-2010 Plus). An HP-5MS
infiltration of outdoor pollutants to indoor loadings, particle size capillary column (30 m  0.25 mm i.d. with a 0.25 mm film thick-
distribution patterns and human health risk from inhalation ness) was used for chromatographic separation. The column tem-
exposure to PAHs were examined. We also explored the influences perature was programmed from 60  C (initially held for 1 min),
of human activities, such as cooking and smoking, and haze con- elevated to 250  C at 20  C min
1 (held for 2 min), ramped to 280  C
ditions on the distribution patterns and levels of indoor PAHs. The at 5  C min
1 (held for 15 min) and further increased to 300  C at
results are expected to provide updated information for the public 20  C min
1 (held for 20 min). All samples were automatically
and regulatory agencies in implementing better measures to injected (1 mL each) in a programmed temperature vaporizer with
improve personal environments. an initial temperature of 60  C and then elevated to 300  C at 400  C
min
1 (held for 10 min). Ultrahigh-purity helium was used as car-
2. Materials and methods rier gas at a flow rate of 1 mL min
1. Mass spectra were acquired in
the full scan mode with an electron impact energy of 70 eV.
2.1. Materials
2.4. Quality assurance and quality control
A standard solution of 16 PAHs, including acenaphthene (Ace),
fluorene (Flo), phenanthrene (Phe), anthracene (Ant), fluoranthene One procedural blank and one field blank sample were analyzed
(Fla), pyrene (Pyr), benz[a]anthracene (B[a]A), chrysene (Chr), for every batch of 22 particle samples and 12 gaseous samples,
benzo[b]fluoranthene (B[b]F), benzo[k]fluoranthene (B[k]F), benzo respectively. The recoveries of the surrogate standards, i.e., ace-
[e]pyrene (B[e]P), benzo[a]pyrene (B[a]P), indeno[1,2,3-cd]pyrene naphthene-d10, phenanthrene-d10, chrysene-d12, perylene-d12,
(IcdP), dibenzo[a,h]anthracene (DahA), benzo[ghi]perylene (BghiP) benzo[ghi]perylene-d12 and coronene-d12, for various samples are
and coronene (Cor), was obtained from AccuStandard (New Haven, represented in Table S1. The recoveries of individual PAH com-
CT, USA). Acenaphthene-d10, phenanthrene-d10, chrysene-d12, per- pounds in the spiked samples ranged from 82% to 114%. Concen-
ylene-d12, benzo[ghi]perylene-d12 and coronene-d12 used as sur- trations of PAHs in all field samples were corrected by those
rogate standards were obtained from Dr. Ehrenstorfer GmbH detected in the corresponding procedural blanks within the same
(Augsburg, Germany). Fluorene-d10 and pyrene-d10 were purchased batch but not corrected for the surrogate standard recoveries. The
from AccuStandard (New Haven, CT, USA) and dibenzo[a,h] lowest calibration concentrations divided by the actual sample
anthracene-d14 was from Cambridge Isotope Laboratories (And- volumes were defined as the reporting limits for the target com-
over, MA, USA); they were used as internal standards. pounds. The reporting limits for particle-bound and gaseous PAHs
 Y.-J. Hu et al. / Environmental Pollution 238 (2018) 431e439 433

are represented in Table S2, calculated with the air volumes of often used to assess exposure risk via inhalation (Guo and Kannan,
30.0e169.2 m3 for both particle and gaseous samples. In addition, 2011; United States Environmental Protection Agency, 1991, 2009)
66 particle samples (six samples containing 11 size fractions) and
six gaseous samples were collected as duplicate samples. Duplicate C  IR  ET
DI ¼ (2)
samples with mean concentrations and standard deviations of BW
target PAHs are presented in Table S3.
C  IR  ET  ED  EF  CSF
ILCR ¼  10
6 (3)
2.5. Data analysis BW  AT

where C is the sum of deposition concentrations of size-

The free sampling approach used in the present study was able
fractionated particle-bound and gaseous PAHs with B[a]P equiva-
to capture the levels of atmospheric PAHs closely associated with
lent (B[a]Peq) concentration in the human respiratory system (ng
human daily life. The sampling scenarios were organized into four
m
3); IR is the rate of inhalation (m3 h
1); ET is the event time, i.e.,
types i.e., normal (without unexpected indoor and outdoor sources,
the time duration for a day with exposure (h d
1); BW is the
including the school sites in Tianhe, Luogang and Zengcheng dis-
average body weight (kg), ED is the lifetime exposure duration
tricts during the dry and wet weather seasons, the office site in
(year), EF is the exposure frequency (365 d year
1), AT is the average
Tianhe district during the wet weather season and the office sites in
time for carcinogenic effects set at 70 years  365 d yr
1 (day) and
Luogang and Zengcheng districts during the dry and wet weather
CSF is the cancer slope factor ((mg kg
1 bw day
1)
1). Because body
seasons), cooking (with indoor cooking emission, including the
weights and air inhalation rates vary by age, DI and ILCR of PAHs
residence sites in Tianhe and Luogang districts during the dry and
were calculated for four age groups, i.e., children (<6 years), ado-
wet weather seasons), smoking (with indoor smoking emission,
lescents (6e17 years), adults (18e60 years) and seniors (>60 years).
including the residence site in Zengcheng district during the dry
These are corresponding to four integrated scenarios, i.e., residence
weather season) and haze episode (with an outdoor haze episode,
and outdoors for children, school, residence and outdoors for ad-
including the office site in Tianhe district during the dry weather
olescents, office, residence and outdoors for adults and residence
season).
and outdoors for seniors (Table S4). It should be noted that ado-
All statistical analyses were performed with PASW Statistics 18
lescents are defined as 6e17 years old, because the school sampling
(Chicago, IL, USA). The independent-samples t-test was performed
sites in the present study are located in primary and middle
to identify any variability in concentrations of particle-bound and
schools. A Monte Carlo simulation was conducted to assess the
gaseous PAHs between the dry and wet weather seasons and
uncertainty in variability of daily inhalation intake and ILCR by
among different urban settings. The relationships between the in-
Crystal Ball software (version 2000.2, Decisioneering, Denver, CO,
door and outdoor PAH concentrations were examined using the
USA). Although the event time vary with age groups (Table S4), the
indoor-to-outdoor (I/O) ratio of individual PAHs. An I/O ratio
total indoor and outdoor exposure time is 24 h at the Monte Carlo
greater than 1 means positive contribution from indoor sources to
simulation. The uncertainty, sensitivity and 95% confidence interval
outdoor PAHs air concentrations and vice versa (Naumova et al.,
(CI) for all calculation were reported with 5000 iterations of
2002). Linear regression was conducted between indoor and out-
simulation.
door concentrations of total and individual PAHs for each sampling
Due to instrumental errors, some data were lost from individual
site without indoor source emission.
sampling sites, i.e., concentrations in both indoor and outdoor
Chrysene was used as a tracer to estimate the infiltration factor
samples at the residential site in Zengcheng during the wet
(Finf) for assessing the contributions of outdoor-generated PAHs to
weather season. Particles collected with MOUDI were divided into
indoor loadings (Choi and Spengler, 2014; Mohammed et al., 2016).
three diameter groups corresponding to larger than 1.8 mm, be-
In the absence of any significant indoor source (cooking and
tween 0.1 and 1.8 mm and smaller than 0.1 mm, which are defined as
smoking in the present study), Finf is calculated by standardizing
coarse, accumulation mode and ultrafine particles, respectively.
the I/O ratio of each target compound with the concentration of Chr
The sum of accumulation mode and ultrafine particles is defined as
as (Choi and Spengler, 2014)
fine particles.
PAHin Chrout
Finf ¼  (1)
Chrin PAHout 3. Results and discussion

where PAHin and PAHout are the indoor and outdoor concentrations 3.1. Temporal and spatial variability of particle-bound and gaseous
of a PAH compound and Chrin and Chrout are the concentrations of target PAHs
indoor and outdoor Chr. The value of Finf greater than unity means a
higher indoor concentration of the target analyte than that from Of 16 PAHs, individual analytes not detected or with concen-
outdoor infiltration only (Choi and Spengler, 2014; Mohammed trations below the reporting limits in most samples will not be
et al., 2016). further discussed herein. The remaining analytes are designed as
P
The deposition fractions and concentrations of inhaled particle- p PAH (sum of particle-bound Ace, Flo, Phe, Fla, Pyr, B[a]A, Chr, B
P
bound PAHs in the human respiratory tract were calculated with [bþk]F, B[e]P, B[a]P, IcdP, DahA, BghiP and Cor), g PAH (sum of
P
the simplified equations from the International Commission on gaseous Ace, Flo, Phe, Ant, Fla, PYR, B[a]A and Chr) and (pþg) PAH
P P
Radiological Protection (ICRP) model (International Commission on (sum of p PAH and g PAH). Statistical data are summarized in
Radiological Protection, 1994). The model calculates the deposition Table 1.
fractions of inhaled particles in three main regions of the respira- The concentrations of particle-bound PAHs were significantly
tory tract, i.e., head airway (HA, which includes nose, mouth, higher in the dry weather season than in the wet weather season (t-
pharynx and larynx), tracheobronchial region (TB) and alveolar test and p < 0.05), while those of gaseous PAHs were only slightly
region (AR) (Hinds, 1982; International Commission on Radiological higher in the dry weather season than in the wet weather season (t-
Protection, 1994). More details about the model are provided in test and p > 0.05). Such variability may partially be explained by
Text S2. wet deposition, which would remove a much larger portion of
Daily intake (DI) and incremental lifetime cancer risk (ILCR) are particle-bound PAHs in the wet weather season than in the dry
434 Y.-J. Hu et al. / Environmental Pollution 238 (2018) 431e439

Table 1
Concentrations (Mean, Median, Minimum and Maximum; ng m
3) of airborne PAHs in Guangzhou, China.

Sp PAHa Sg PAHb S(pþg) PAHc

Mean ± SDd Median Min Max Mean ± SD Median Min Max Mean ± SD Median Min Max

Seasonality
Dry Weather Season 5.06 ± 2.50 4.79 2.35 11.9 383 ± 339 309 40.2 1280 388 ± 341 314 42.5 1290
Wet Weather Season 3.07 ± 0.96 3.16 1.71 5.30 268 ± 136 239 59.8 524 271 ± 136 244 63.8 527
District
Tianhe 3.90 ± 1.42 3.32 2.35 5.94 237 ± 155 213 40.2 524 241 ± 156 218 42.5 527
Luogang 3.41 ± 1.43 2.93 1.71 5.64 276 ± 120 313 59.8 419 279 ± 120 318 63.8 422
Zengcheng 5.55 ± 3.31 3.88 2.98 11.9 548 ± 424 400 167 1280 553 ± 427 403 171 1290
Urban Setting
School 3.50 ± 1.08 3.16 2.35 5.64 214 ± 156 171 40.2 530 217 ± 156 174 42.5 534
Office 3.76 ± 1.45 3.30 1.83 5.94 295 ± 119 316 74.8 420 299 ± 118 318 80.6 423
Residence 5.25 ± 3.23 4.61 1.71 11.9 501 ± 386 341 117 1280 506 ± 389 345 119 1290
Sampling Site
Indoors 3.78 ± 2.37 3.06 1.75 11.9 334 ± 274 318 40.2 1280 338 ± 276 322 42.5 1290
Outdoors 4.52 ± 1.89 4.13 1.71 9.50 323 ± 267 274 59.8 1140 327 ± 268 280 63.8 1150
a
Sp PAH is sum of particle-bound Ace, Flo, Phe, Fla, Pyr, B[a]A, Chr, B[bþk]F, B[e]P, B[a]P, IcdP, DahA, BghiP and Cor.
b
Sg PAH is sum of gaseous Ace, Flo, Phe, Ant, Fla, Pyr, B[a]A and Chr.
c
S(pþg) PAH is sum of Sp PAH and Sg PAH.
d
Standard deviation.

weather season. were 1290 and 1150 ng m
3, 19 times higher than that
Both particulate and gaseous concentrations of PAHs were not (66.7 ng m
3) in another tobacco smoking scenario within resi-
consistent with the level of urbanization in the administrative dential indoor settings in Porto, Portugal (Castro et al., 2011). Such
districts under investigation, which follows the sequence of variation may be affected by different emission processes, or even
Tianhe > Luogang > Zengcheng, with population densities of by indoor ventilation efficiency.
15400, 1000 and 650 km
2 and GDP of 280, 190 and 90 billion RMB A short haze episode occurred from the evening of October 25 to
(Elivecity Laboratory, 2013; Guangzhou Statistics, 2013). In urban early morning of October 26, 2014 during one of the sampling
areas, PAHs are generally derived from incomplete combustion of events at the office site in Tianhe district. The outdoor particle-
fossil fuels (Zhang et al., 2007), especially traffic emissions (Nielsen, bound PAHs concentration in the sample collected during this
1996). Transport of atmospheric PAHs would result in spreading of event was 5.94 ng m
3, higher than the average value (4.24 ng m
3)
PAHs from urban centers to adjacent regions, i.e., rapid urbaniza- measured during the non-haze periods. A previous study suggested
tion can aggravate environmental pollution (Shao et al., 2006). that concentrations of particle-bound PAHs were considerably
Besides traffic emissions, human daily activities such as cooking enhanced under stagnant haze conditions, i.e., air masses were
and smoking may also add to the pre-existing contaminant loads, transported to Guangzhou from northeast on October 24, adding to
which is perhaps why total PAH concentrations varied widely at the local emissions as the main contributors to PAHs (Tan et al., 2011).
sampling sites, i.e., 42.5e527 ng m
3 in Tianhe, 63.8e422 ng m
3 in The concentration of indoor particle-bound PAHs also increased to
Luogang and 171e1290 ng m
3 in Zengcheng (Table 1). These re- 5.59 ng m
3 during the haze episode, higher than average value
sults were corroborated by the distribution of indoor PAH con- (3.10 ng m
3). Although the data during the haze episode is limited,
centrations (particle þ gas) among three urban settings, i.e., higher the derived result still indicated that indoor environment in
in residence (506 ng m
3) than in office (299 ng m
3) and school Guangzhou is incessantly affected by outdoor sources.
(217 ng m
3) (Table 1).
The average indoor and outdoor PAH concentrations were 3.2. Profiles of particle-bound and gaseous PAHs
258 ng m
3 (range: 42.5e404 ng m
3) and 268 ng m
3 (range:
63.8e534 ng m
3), respectively (Table S5). The I/O ratio of particle- The composition profiles of particle-bound and gaseous PAHs by
bound PAHs varied within 0.50e0.97 with an average of 0.73 ring size in indoor and outdoor settings varied with four sampling
(Fig. 1), suggesting that particle-bound PAHs are mainly derived scenarios. Physicochemical properties are an important factor in
from outdoor sources. On the other hand, the average I/O ratio of dictating the gas‒particle partitioning of PAHs (Kim et al., 2013),
gaseous PAHs was 1.38 (range: 0.30e6.08). Specifically, I/O ratios of e.g., concentrations of 2‒4-ring particle-bound and gaseous PAHs
low molecular weight (LMW) (2‒3-ring) gaseous PAHs were all were comparable, while 5‒7-ring PAHs occurred in the particulate
greater than 1 (Fig. 1), consistent with previously reported findings phase only (Bi et al., 2003). The profiles of particle-bound PAHs in
(Li and Ro, 2000; Naumova et al., 2002), i.e., LMW PAHs were both indoor and outdoor environments were dominated by 4- and
largely generated from indoor sources. Consumer products were 5-ring PAHs, accounting for 27e41% and 25e29% of total concen-
found to emit LMW PAHs (Zhang and Tao, 2009), e.g., heated plastic trations, respectively (Fig. 2). Gaseous PAH profiles were substan-
materials, chips and other computer components could emit Phe tially different from those of particle-bound PAHs, with 3-ring PAHs
(Destaillats et al., 2008). accounting for 81e84% of total levels (Fig. S1). The composition
Multiple studies have documented that levels of indoor PAHs profiles of particle-bound and gaseous PAHs were not significantly
are influenced by endogenous sources (Abdullahi et al., 2013; different between indoor and outdoor environments (t-test and
Romagnoli et al., 2014). In residence environment with cooking in p > 0.05). In contrast, the profiles of indoor LMW PAHs were
the present study, indoor and outdoor PAH concentrations different with and without indoor emissions. For example, 2‒4-ring
(particle þ gas) were 385 and 272 ng m
3 (Table S5), higher than PAHs accounted for 53% and 54% of indoor particle-bound PAHs
164 ng m
3 (indoors) and 36.7 ng m
3 (outdoors) from another under cooking and smoking scenarios, respectively, which is higher
cooking scenario (Pandit et al., 2001). In the indoor smoking sce- than those under normal scenario (43%) (Fig. 2). During the haze
nario, the indoor and outdoor PAH concentrations (particle þ gas) event, the contributions of 5‒7-ring PAHs to particle-bound
 Y.-J. Hu et al. / Environmental Pollution 238 (2018) 431e439 435

3
Particle-bound PAHs Infiltration Factors (Finf)
Indoor/Outdoor (I/O) Ratios
Indoor/Outdoor (I/O) Ratios = 1
2

Values
1

0
Ace Flo Phe Flu Pyr B[a]A Chr B[b+k]F B[e]P B[a]P IcdP DahA BghiP Cor

9
Gaseous PAHs

6
Values

-3

Ace Flo Phe Ant Fla Pyr B[a]A Chr

Fig. 1. Estimated infiltration factors (Finf) and indoor/outdoor (I/O) values of particle-bound and gaseous PAHs.

concentrations (indoor: 50%; outdoor: 48%) were greater than et al. (2014) showed that almost all PAHs were concentrated in
those in indoor emission scenarios with cooking and smoking. Tan particles with diameters < 0.43 mm, regardless of food types.
et al. (2011) also revealed that a haze episode with air masses from Kleeman et al. (2008) reported the greater concentration of PAHs in
north and south of Guangzhou contributed abundant 5‒6-ring ultrafine particles (size < 100 nm) than coarse particles from char
PAHs (55e75%) to particle-bound PAHs. grilling. Moreover, the particle-bound PAHs emitting from different
types of incense smokes exhibited bimodal distributions at < 0.18
3.3. Particle size distribution of PAHs with four sampling scenarios and 0.32e0.56 mm (Yang et al., 2007). Different from the previous
study, the present results may point to the tendency of PAHs to
The particle size distributions (dC/C dlog Dp versus Dp) of indi- migrate towards large particles in ambient environment. In
vidual and total PAHs in both indoor and outdoor settings for four particular, it may take longer for indoor particles within closed
sampling scenarios (normal, cooking, smoking and haze episode) environments to undergo aging process than fresh particle-bound
were unimodal, with a sharp peak in the 0.56e1.0 mm fraction PAHs emitted from combustion sources (Venkataraman et al.,
(Figs. S2‒S5), except for outdoor samples collected during the haze 1994). The similar size-dependent distributions of particle-bound
episode (0.32e1.8 mm). While the predominance of PAHs in fine PAHs in indoor and outdoor environments suggested an efficient
particles has been widely observed in previous studies (Kawanaka air exchange that should not be neglected in assessing air quality in
et al., 2009; Zhang et al., 2012a, 2012b), the size distribution pat- indoor environments.
terns in the present study were different from a previous finding During the haze episode, the size distributions of PAHs
where total PAHs peaked at 0.32e0.56 mm in summer of Guangz- remained unimodal, but the peak spread to larger size
hou (Zhang et al., 2012a). The peak shift toward larger size fraction (0.32e1.8 mm) for 3‒4-ring PAHs both indoors and outdoors
in the present study may have resulted from prolonged aging (Fig. S5). For 5‒7-ring PAHs, a major peak occurred around
processes for accumulation mode PAHs, as discussed by Vaeck and 0.32e1.0 mm indoors and a sharp peak at 0.56e1.0 mm outdoors.
Cauwenberghe (1985). The outdoor particle-bound PAHs peak at 1.0e1.8 mm was more
No obvious peaks were observed for 2-ring PAHs in both indoor prominent than the indoor peak (Fig. S5). During the haze episode,
and outdoor samples (Figs. S2‒S5). The size distributions of 3‒7- some coarse particles were generated from the transformation of
ring PAHs were essentially unimodal peaking at 0.56e1.0 mm size. accumulation mode aerosols with prolonged suspension,
In particular, the size profiles of 5‒7-ring PAHs were unimodal with enhancing the affiliation of PAHs with large particles (Tan et al.,
a sharp peak at 0.56e1.0 mm (Figs. S3‒S4) with indoor cooking and 2011), which was probably due to weak infiltration of PAHs affili-
smoking. Several previous studies indicated that particle-bound ated with outdoor large particles into indoor settings.
PAHs emitted freshly from combustion are dominantly distrib-
uted in the ultrafine fractions (Miguel et al., 1998; Phuleria et al., 3.4. Relationship between indoor and outdoor PAH concentrations
2006), but unimodal size distributions of PAHs peaking at larger
particle sizes have been observed from cooking and smoking in the Simultaneous measurements of indoor and outdoor PAHs allows
present study than those in previous studies. For example, Saito the estimation of the infiltration of outdoor-generated PAHs into
436 Y.-J. Hu et al. / Environmental Pollution 238 (2018) 431e439

Fig. 2. Composition profiles of particle-bound PAHs under four sampling scenarios (normal, cooking, smoking and haze) indoors and outdoors in Guangzhou, China.

indoor settings (Mohammed et al., 2016). All paired indoor and determination, r2, for all groups with significant correlations
outdoor samples were organized into 17 groups. The indoor (Cin- ranged from 0.38 to 0.99 (average r2 ¼ 0.77) for particle-bound
door) and outdoor (Coutdoor) concentrations of particle-bound and PAHs and 0.62 to 1.0 (average r2 ¼ 0.97) for gaseous PAHs. This
gaseous PAHs for each group were linearly regressed by implied that 38e99% (or 77% on average) and 62e100% (or 97% on
average) of the variations for the indoor concentrations of particle-
Cindoor ¼ a Coutdoor þ b (4) bound and gaseous PAHs were explained by the outdoor concen-
trations. This was particularly true for 5‒7-ring particle-bound
where a and b are the fitting parameters. Significant correlation PAHs which exhibited a highly significant correlation (p < 0.01). A
between Cindoor and Coutdoor was found for total PAHs both in previous study also obtained r2 values of 0.64e0.99 for 5‒7-ring
particle-bound and gaseous samples (Table S6). The coefficients of PAHs, attributed to the predominance of outdoor sources over
 Y.-J. Hu et al. / Environmental Pollution 238 (2018) 431e439 437

indoor respirable 5‒7-ring PAHs (Naumova et al., 2002).

The indoor/outdoor relationships for individual PAHs were quite
different. Largest variability in I/O ratios (0.11e14) and Finf
(0.17e9.3) occurred with 2‒4-ring PAHs predominantly present in
the gas phase (Table S6). Apparently higher volatile PAHs were
more likely affected by indoor sources than outdoors. On the other
hand, in the absence of indoor emission sources, good correlation
between the indoor and outdoor concentrations of particle-bound
5‒7-ring PAHs and their high Finf values (1.2e1.5 greater than 1;
Fig. 1) indicated that they were mainly from outdoor-to-indoor
exchange. Obviously, atmospheric PAHs exchange between indoor
and outdoor environments was efficient and synergistically influ-
enced human inhalation exposure to atmospheric PAHs in ambient
environment.

3.5. Regional deposition and size dependence of particle-bound

PAHs in human respiratory tract

The inhalable, thoracic and respirable fractions are defined by

the International Standards Organization and American Conference
of Governmental Industrial Hygienists (Hinds, 1982). The calculated
inhalable, thoracic and respirable fractions of PAH concentrations
were 91e98%, 80e98% and 68e97% indoors and 89e97%, 78e98%
and 63e97% outdoors (Table S7). By comparison, only 30e55% and
32e54% of PAHs indoors and outdoors could deposit in the human
respiratory tract as determined from the ICRP model.
The deposition concentrations of particle-bound PAHs were
0.62e4.4 ng m
3 indoors and 0.71e3.2 ng m
3 outdoors among all
sampling sites (Table S8), with the combined mean values
(indoors þ outdoors) following the sequence of residence
(4.1 ng m
3) > office (2.8 ng m
3) > school (2.5 ng m
3). The HA
received the most abundant fraction of PAHs, followed by the AR
and TB. The regional deposition efficiencies of individual inhaled
PAHs in HA, TB and AR were 19e43%, 1.8e2.8% and 8.1e10% indoors
and 21e44%, 1.9e2.8% and 7.7e9.9% outdoors, respectively.
Apparently, the deposition efficiencies of indoor and outdoor
particle-bound PAHs in human respiratory tract were similar,
although their deposition concentrations were slightly different.
The deposition concentrations of particle-bound PAHs in
different respiratory tract regions were size-dependent (Fig. 3).
Coarse particles-affiliated PAHs predominantly deposited in the HA
(38e47%), while PAHs in fine particles mostly occurred in the AR
(68e75%) and TB (87e90%) (Table S9). The size-dependent depo-
sition fractions of particle-bound PAHs were different among all
sampling sites (Table S9), and also from other previous studies. For
example, Zhang et al. (2012a) reported the efficiencies of
Fig. 3. Concentrations of particle size-fractionated PAHs deposited in different regions
87.1e96.3%, 26.4e35.1% and 27.0% for PAHs in coarse, accumulation of the human respiratory tract both indoors and outdoors at school, office, and
and ultrafine particles to deposit in the respiratory tract in residence.
Guangzhou urban environment. In a study conducted at an e-waste
recycling zone (Qingyuan) and urban Guangzhou, PAHs in coarse
particles were found to prevalently deposit in the HA (69e91%), scenarios should be carefully considered in risk assessment of hu-
while PAHs in fine particles were dominant in the AR (62e80%) and man inhalation exposure to airborne PAHs. Estimated average daily
TB (44e68%) (Luo et al., 2015). inhalation intake of airborne PAHs for four age groups based on B[a]
Peq deposition concentration followed the sequence of children
3.6. Risk assessment of human inhalation exposure to airborne (1.1 ng kg
1 bw d
1) > adolescents (0.51 ng kg
1 bw d
1) > adults
PAHs (0.33 ng kg
1 bw d
1) > seniors (0.19 ng kg
1 bw d
1) (Table 2). For
all four age groups, daily inhalation intake through indoor air
Based on the relative Potency Factor Approach (Flowers et al., exposure to PAHs was 3e9 times greater than that through outdoor
2002), the average values of the total carcinogenic potency B[a] exposure (Table 2), suggesting higher health risk in indoor envi-
Peq concentrations of particle-bound and gaseous PAHs were ronments than in outdoor environments for general population
1.2 ± 0.6, 1.4 ± 0.6 and 1.5 ± 0.6 ng m
3 indoors at school, office and except outdoor workers in urbanized megacities of China such as
residence, respectively, which are slightly higher than the European Guangzhou.
Union's annual average B[a]Peq standard (1 ng m
3) (European Inhalation ILCRs from exposure to indoor and outdoor airborne
Union, 2012). Amid the spatial variability of PAHs in indoor set- PAHs for all four age groups ranged from 8.8  10
8 (95% CI:
tings, different age groups with different prevailing exposure 4.9  10
9‒3.3  10
7) for seniors to 5.9  10
7 (95% CI: 6.3  10
8‒
438 Y.-J. Hu et al. / Environmental Pollution 238 (2018) 431e439

Table 2
Daily inhalation intakes (DI; ng kg
1 bw d
1, B[a]P equivalent (B[a]Peq)) and incremental lifetime cancer risk (ILCR, 10
6) upon exposure to PAHs for children, adolescents,
adults and seniors in indoor and outdoor settings.

DI ILCR

Indoor Outdoor Total Indoor Outdoor Total

a
Children (<6 yr) 0.84 (0.13e2.5) 0.25 (0.02e0.88) 1.1 (0.17e3.2) 0.24 (0.02e0.79) 0.07 (0.003e0.27) 0.30 (0.03e1.0)
Adolescents (6e17 yr) 0.36 (0.07e1.0) 0.13 (0.01e0.46) 0.51 (0.10e1.4) 0.19 (0.03e0.59) 0.06 (0.004e0.23) 0.26 (0.04e0.77)
Adults (18e60 yr) 0.28 (0.03e0.90) 0.03 (0.002e0.12) 0.33 (0.04e1.0) 0.53 (0.06e1.8) 0.06 (0.03e0.23) 0.59 (0.06e1.9)
Seniors (>60 yr) 0.14 (0.01e0.54) 0.04 (0.002e0.16) 0.19 (0.01e0.67) 0.07 (0.003e0.24) 0.02 (0.001e0.06) 0.09 (0.005e0.33)
a
A (B
C) represents the median A and a 95% confidence interval.

Fig. 4. Incremental lifetime cancer risk induced by inhalation exposure to indoor and outdoor PAHs for adults under different exposure scenarios. Results for the indoor envi-
ronment were obtained based on the concentrations of PAHs for the residence only.

1.9  10
6) for adults (Table 2). All average ILCR values for residents assessment should be conducted with specific details, e.g., both
were lower than the risk threshold (1.0  10
6; Table 2) (United indoor and outdoor environments within different sampling sce-
States Environmental Protection Agency, 1989), suggesting lower narios to better reflect human daily life.
cancer risk for exposure to indoor and outdoor air PAHs in
Guangzhou. The calculated values are generally lower than and
4. Conclusions
comparable to the ILCR values obtained in other urban areas of
China. For example, the median ILCR of PAHs for urban citizens in
Tianjin was 2.2  10
4 (Bai et al., 2009). The geometric mean The present study has demonstrated that the concentrations of
indoor airborne PAHs were elevated by common contributions
inhalation ILCRs for children and adults in Taiyuan were 1.76  10
6
and 7.95  10
6, respectively (Xia et al., 2013). Zhang et al. (2009) from indoor source emission and outdoor infiltration with outdoor-
to-indoor exchange. The profiles and size distributions of particle-
reported the arithmetic mean for general residents in 2003 as
1.79  10
4 in Shanxi Province of China and 6.5  10
6 for all of bound PAHs were related to various lifestyles, such as cooking
and smoking. Particle-bound PAHs with accumulation mode
China. In addition, the indoor inhalation ILCRs for general popula-
tion from exposure to PAHs (0.02  10
6e2.7  10
6) were higher contributed the majority of PAHs that may deposit in the human
respiratory system. All average ILCR values for four age groups were
than outdoor ones (0.008  10
6e1.0  10
6; Table 2), further
suggesting the urgency to minimize indoor exposure to airborne below the lower limit of the Safe Acceptable Range (10
6). Collec-
tively, the health risks of exposure to indoor and outdoor PAHs via
PAHs. Furthermore, it is noteworthy that the ILCR value for adults
(average: 6.2  10
7; 95% CI: 4.9  10
8‒2.1  10
6), estimated inhalation were low for residents with different age groups in
Guangzhou, China.
from indoor air PAH levels only in residence with 24-h exposure
time, was comparable to our assessment results (average:
5.9  10
7; 95% CI: 6.3  10
8‒1.9  10
6), while the risk value Acknowledgments
derived from outdoor concentrations (average: 7.3  10
7; 95% CI:
5.2  10
8‒2.6  10
6) with 24-h exposure time was significantly The present study was financially supported by the National
(t-test; p < 0.01) higher than our estimation (Fig. 4). This was Natural Science Foundation of China (Nos. 41329002, 413290240
obviously attributed to the higher B[a]Peq concentrations of and 21637001). This is contribution No. IS-2518 from GIGCAS.
particle-bound 5‒6-ring PAHs outdoors than indoors (Table S8).
Apparently, the extent of overestimation for exposure risk could
become greater if the total concentration of particle-bound PAHs Appendix A. Supplementary data
other than the deposition concentration was included in the
assessment. The findings also suggested that the respiratory risk Supplementary data related to this article can be found at
https://doi.org/10.1016/j.envpol.2018.03.040.
 Y.-J. Hu et al. / Environmental Pollution 238 (2018) 431e439 439

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