Ecotoxicology and Environmental Safety 211 (2021) 111959

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Ecotoxicology and Environmental Safety

journal homepage: www.elsevier.com/locate/ecoenv

Research paper

Inhalation exposure to size-segregated fine particles and particulate PAHs

for the population burning biomass fuels in the Eastern Tibetan
Plateau area
Ye Huang a, b, Jinze Wang a, Nan Fu c, Shanshan Zhang a, Wei Du a, b, *, YuanChen Chen d,
Zhenglu Wang e, Meng Qi b, Wei Wang b, Qirui Zhong b, Yonghong Duan f, Guofeng Shen b,
Shu Tao b
a
Key Laboratory of Geographic Information Science of the Ministry of Education, School of Geographic Sciences, East China Normal University, Shanghai 200241, China
b
Laboratory of Earth Surface Processes, College of Urban and Environmental Sciences, Peking University, Beijing 100871, China
c
School of Energy and Power Engineering, Nanjing University of Science & Technology, Nanjing 210094, China
d
College of Environment, Research Centre of Environmental Science, Zhejiang University of Technology, Hangzhou 310032, China
e
College of Oceanography, Hohai University, Nanjing, Jiangsu, China
f
College of Resources and Environment, Shanxi Agricultural University, Taigu, Shanxi, 030801, China

A R T I C L E I N F O A B S T R A C T

Edited by: Dr G Liu Indoor biomass burning produces large amounts of small particles and hazardous contaminants leading to severe
air pollution and potentially high health risks associated with inhalation exposure. Personal samplers provide
Keywords: more accurate estimates of inhalation exposure. In this study, inhalation exposure to size-segregated particles
Personal exposure and particulate polycyclic aromatic hydrocarbons (PAHs) for the biomass user was studied by deploying personal
Particulate matter
samplers. The study found that daily PM2.5 inhalation exposure level was as high as 121 ± 96 μg/m3, and over
PAHs
84% was finer PM1.0. For PAHs, the exposure level was 113 ± 188 ng/m3, with over 77% in PM1.0. High mo­
Biomass use
Size distribution lecular weight PAHs with larger toxic potentials enriched in smaller particles resulting in much high risks
associated with PAHs inhalation exposure. Indoor exposure contributed to ~80% of the total inhalation exposure
as a result of high indoor air pollution and longer residence spent indoor. The highest exposure risk was found for
the male smoker who conducted cooking activities at home.

1. Introduction
Although cleaner fuels such as electricity and liquefied petroleum
gas (LPG) are becoming popular in China, a large proportion of rural
population still rely on solid fuels for cooking and space heating (Tao
et al., 2018; Du et al., 2018a). Inefficient burning of solid fuels in resi­
dential stoves produces large amounts of air pollutants like particulate
matter (PM), carbon monoxide, organic carbon, and polycyclic aromatic
hydrocarbons (PAHs), leading to higher personal exposure for those
people using solid fuels. It was reported that personal PM2.5 exposure for
people using biomass could be 2.5 times of that for people using LPG and
electricity (Huang et al., 2017). Exposure to these toxic air pollutants is
closely associated with many cardiovascular and respiratory diseases
and lung cancer (Burnett et al., 2014; Carl-Elis et al., 2002). It is
estimated that in 2019, nearly 2.31 (1.63–3.12 as range) million pre­
mature deaths were attributable to household air pollution (HAP),
accounted for nearly 34.6% of the PM2.5-related premature deaths in the
world (GBD, 2020). In China, severe household air pollution (HAP) due
to indoor solid fuel uses have been recognized in some past studies
(Huang et al., 2014; Shen et al., 2013a; Zhang and Smith, 2007; Wang
et al., 2017; Du et al., 2018b; He et al., 2020). The PM2.5-related pre­
mature deaths caused by HAP in rural area was estimated at about 0.52
million, contributing 43% to the total in 2015 (Zhao et al., 2018).
Exposure level is a critical factor in assessing health risks of inhala­
tion exposure. While time-weighted average concentrations from sta­
tionary monitoring at different microenvironments had been used in
some studies (Baumgartner et al., 2011; Hu et al., 2014; Downward
et al., 2014; Chen et al., 2016; Huang et al., 2017), it is believed that this

* Corresponding author at: Key Laboratory of Geographic Information Science of the Ministry of Education, School of Geographic Sciences, East China Normal
University, Shanghai 200241, China.
E-mail address: wdu@geo.ecnu.edu.cn (W. Du).

https://doi.org/10.1016/j.ecoenv.2021.111959
Received 23 October 2020; Received in revised form 10 January 2021; Accepted 17 January 2021
Available online 25 January 2021
0147-6513/© 2021 The Authors. Published by Elsevier Inc. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Y. Huang et al.
approach may hardly reflect the real exposure level as there are high
variations and many distinct microenvironments where a people may
stay in one day. For example, Du et al. (2017) found a notable over­
estimation when calculating the exposure by the stationary concentra­
tions and corresponding time the local residents spent in the
microenvironments compared to the directly measured exposure to
PM2.5. Thus, personal samplers are better choice for inhalation exposure
and risk assessment. However, this approach is challenged due to high
requirements and hard work in field conditions, and high costs. In this
study, inhalation exposure levels of PMs and PAHs for the rural popu­
lation burning biomass fuels from the southwest China were evaluated
by using personal samplers. The site was located in the eastern Tibetan
Plateau (TP) where there are high consumptions of biomass fuels due to
abundant resources and availability, and unaffordable to clean energies
in the rural area. Pollutants emission from biomass combustion in the TP
have significant impacts on ecosystem and human health (Downward
et al., 2014; Gao et al., 2009; Xiao et al., 2015; Huang et al., 2018;
Menon et al., 2002; Shen et al., 2019), but in comparison with the
adverse impacts from coal combustion, problems from the indoor
biomass burning are, to some extent, overlooked (Du et al., 2018b; Meng
et al., 2019) Besides the total exposure level, the study specifically
looked into detailed size distributions of PMs and PAHs in the inhaled
air. It is widely recognized that adverse health impacts associated with
particle exposure are related to not only particle mass but also its
chemical components and size (Oberdörster et al., 2005; Shiraiwa et al.,
2017; Du et al., 2020), thus calling for more attention. The main ob­
jectives of this study are: 1) to characterize the exposure level to PMs
and PAHs for the rural population burning biomass in eastern Tibetan
area; 2) to study the size distributions of PMs and PAHs in inhaled air;
and 3) to assess potential health risks associated with inhalation expo­
sure to PM and PAHs.
2. Material and method
2.1. Field site
This field study was conducted in rural Nanchong, Sichuan Province
in January, 2016. The field site was in Eastern Tibetan Plateau area.
Biomass fuels, mainly fuel wood and crop residues, are the most popular
cooking fuels in the studied area, and space heating in winter was not
very common in most homes. The typical stove used in this area was a
built-in-place brick stove with an outdoor chimney. In the study area,
most residents were old because young people usually chose to work in
cities, the mean ages for both men and women volunteers were 59. Most
households owe a small family size (~ 2 residents). The structure of most
local households was similar, with one kitchen, one living room and 1–2
bedrooms. Most exterior windows had only wood lattice without any
covering in these households and the photo of a typical households was
provided in Fig. S1. The detailed information about the sampling site
could be also found in Qi et al. (2019).
2.2. Personal exposure measurement
The Personal daily exposure to particulate matter and PAHs were
measured using personal samplers with written informed consent ob­
tained individually. Residents were selected randomly to participate in
this study. To collect particulate matter with diameter < 0.25, 0.25–1.0,
1.0–2.5, and >2.5 µm, the pump (the Sioutas four stage cascade im­
pactors, SKC, Eighty Four, PA, USA) with pre-weighed glass fiber filters
at a flow rate of 8.2 L/min were used. Participants were asked to carry
samplers for about 24 h, and only when sleeping and using the restroom,
they could place the samplers nearby within 1.0 m. Information
including gender, age, fuel types used for cooking, whether they smoke,
cook and go out for farm working or not were recorded. The sampling
flow was calibrated before and after each sampling cycle using a primary
flow calibrator (Bios Defender 510, USA). The pump automatically
2
Ecotoxicology and Environmental Safety 211 (2021) 111959
recorded sampling volume was double checked with recorded start and
end time. The samples were considered validly when the pump was
running when the research team returned the home in the next day. In a
recent study by Lee et al. (2021), pedometer was used to monitor
compliance in wearing personal samplers, which was great and could be
considered in the future study. In this study, 64 households were
approached for sampling, while 4 samples were discarded due to un­
expected pump stop. Finally, 60 valid samples were collected in this
study, detailed information about the sampling was listed in Table S1.
For quality control, we collected ~ 8% field blanks (5 Samples). The
filters were placed in the same samplers and the pump did not started,
thus the blanks were placed under the same field conditions as personal
samples.
2.3. Laboratory analysis and quality control
Filters were weighed using a high precision digital balance (0.01 mg,
XS105, Mettler-Toledo). Before the gravimetrical measurement, the fil­
ters were placed in a desiccator for ≥24 h in a room with an ambient
temperature of 25–30 ◦ C and a relative humidity of 45%− 55%.
Laboratory PAHs analysis followed the mature procedure in previous
works (Zhuo et al., 2017; Du et al., 2018c). The detailed analysis pro­
cesses and target PAHs including 15 U.S. EPA priority PAHs (without
NAP) and 12 non-priority parent PAHs were provided in Supporting
materials.
Recoveries of targeted PAHs spiked on blank filters were in the range
of 71–120%. In each analysis batch, two surrogates (2-fluoro-1,1′ -
biphenyl and p-terphenyl-d14, Accustandard Inc., via J&W Scientific,
USA) were added randomly in at least 20% samples as a quality control.
The surrogate recoveries were 80–131% and 72–110%, respectively.
Procedure and reagent blanks were measured, and the values of the
blanks were subtracted from the sample results.
2.4. Data analysis and risk assessment
The PM2.5 mass was the sum of the fractions of PM1.0–2.5, PM0.25–1.0,
and PM0.25. PM1.0 mass was the sum of the fractions of PM0.25–1.0 and
PM0.25.
The relative contribution (RC) of indoor and outdoor PM2.5 and PAHs
were estimated using the following equation:
/ /
RCout = {Cout × tout 1440} Cexposure
RCin = 1 − RCout
Where RCin and RCout are the relative contribution of indoor and out­
door PM2.5 or PAHs, respectively; Cout is the concentration of PM2.5 or
PAHs in outdoor air; Cexposure is the exposure level of PM2.5 or PAHs; tout is
the time the local residents spent in outdoor, minutes. 1440 is the total
minutes of one day. In rural Sichuan, the time rural residents spent in
outdoor was 208 min (MEP, 2013). The outdoor PM2.5 and PAHs con­
centrations were 91 ± 39 μg/m3 and 76 ± 35 ng/m3, respectively,
based on the data from field studies conducted in the same site and
sampling periods (Qi et al., 2019; Fu et al., 2020). A Monte Carlo
simulation with variations for PM2.5 and PAHs concentrations and time
spent indoor and outdoor considered was conducted to estimate the
uncertainties of indoor and outdoor contribution. For PM2.5 and PAHs
concentrations, log-normally distribution was applied based on our
first-hand data. For the time spent in outdoor, uniform distribution with
a range of 0–516 was applied and then the time spent in outdoor could
be calculated.
Burnett et al. (2014) developed series of Integrated
Exposure-Response (IER) models to estimate relative risks (RR) for the
mortality associated with ischemic heart disease (IHD), cerebrovascular
disease (stroke), chronic obstructive pulmonary disease (COPD), lung
cancer (LC), and incidence of acute respiratory infection (ALRI) due to
Y. Huang et al.
exposure to PM2.5. The IER model could be described by:
for z < zcf, RRIER(z) = 1, and
for z ≥ zcf, RRIER(z) = 1 + α{1–exp[− γ(z − zcf)δ]},
Where z represents exposure level to PM2.5 in μg/m3 and zcf repre­
sents the counterfactual concentration below which no additional risk is
assumed. Based on available RR information originated from studies of
ambient air pollution, second hand tobacco smoke household solid
cooking fuel and active smoking, 1000 sets of α, γ, δ and zcf were ac­
quired by fitting IER model to account for the uncertainty of RR for
target health outcome. The best estimate and 95% confidence interval of
RR for each health outcome under given exposure were then acquired.
The population attributable fraction (PAF, referenced as the reduction in
the proportion of certain morbidities or mortalities among the definite
population if the risk factor was removed) due to exposure to PM2.5
could be qualified as 1–1/RR (Burnett et al., 2014).
PAH15 and PAH27 represented the total mass concentrations of the
15 U.S. EPA priority PAHs (without NAP) and the total 27 PAHs
measured in this study, respectively. BaPeq (Bap equivalent concentra­
tion) was calculated by:
∑
i=n
BaPeq = (Ci × TEF i )
i=1
where Ci is the concentration of PAH congener i; TEFi is the toxicity
equivalency factor (TEF) of PAH congener i (Table S2). The risk of PAHs
inhalation exposure was evaluated by calculating incremental lifetime
cancer risk (ILCR) for different population groups following:
ILCR = BaPeq × URBaP
Where URBaP is the cancer Unit Risk factor of BaP. The value recom­
mended by CalEPA, 1.1 × 10− 6 per ng/m3 (OEHHA, 2003, 2005), was
adopted in the present analysis, as done in many past studies (Duan
et al., 2014; Shen et al., 2014; Zhang et al., 2019).
SPSS 23.0 (IBM Corporation, Armonk, NY, USA) was used, and non-
parameter Spearman correlation and Kolmogorov-Smirnov methods
were applied for statistical analysis with a significance level of 0.05.
3. Results and discussion
3.1. Personal exposure to PMs and PAHs
3.1.1. PMs exposure
The personal daily inhalation exposure levels measured by personal
samplers were 144 ± 107 (36–576 as range), 121 ± 96 (31− 508),
101 ± 78 (27− 393) and 52 ± 48 (16− 254) μg/m3 for TSP, PM2.5, PM1.0,
and PM0.25, respectively. The coefficients of variation (COVs) of PMs
was around 76%− 94%, indicating relatively large variations of per­
sonal exposure in this area. The mass fractions of PM2.5, PM1.0 and
PM0.25 in TSP were 83.5 ± 9.1%, 70.7 ± 10.3%, and 34.9 ± 9.5%,
respectively. The mass percent of PM1.0 in PM2.5 was 84.3 ± 5.8%. High
fractions of fine particles were thought to be associated with the burning
of biomass fuels in which past emission studies found high fractions of
fine and ultrafine particles (Chen et al., 2005; Shen et al., 2012, 2017).
The PM2.5 exposure level exceeded the national daily ambient PM2.5
standard of 75 μg/m3 by a factor of 1.6 on average, with nearly 73%
population exposing to pollutions exceeding this standard. Even for
PM1.0 that might be more harmful as submicron particles could pene­
trate deep into lung areas (Meng et al., 2013; Dong et al., 2018; Du et al.,
2020), the exposure level exceeded the standard of 75 μg/m3 by a factor
of 1.3 time on average. In comparison with the World Health Organi­
zation (WHO) guideline of 25 μg/m3 for 24-hour mean PM2.5, the
exposure levels for the studied population were much higher, suggesting
high harmful health outcomes associated with particle exposure.
Till now, there were limited studies focused on personal exposure to
PM2.5, especially using personal samplers (Du et al., 2018b). Table S3
3
Ecotoxicology and Environmental Safety 211 (2021) 111959
summarized personal exposure to fine PMs from previous studies. The
exposure levels measured in this study was close to the literature studies
in winter in southern areas, but significantly lower than that in northern
areas. It is believed that in winter, air pollution as well as PM2.5 exposure
in northern area were higher than that in southern areas, mainly due to
the stronger internal emission from space heating in northern areas.
3.1.2. PAHs exposure
The personal daily inhalation exposure levels of PAH27 bounded to
TSP, PM2.5, PM1.0 and PM0.25 were 113 ± 189, 103 ± 185, 91 ± 177,
and 46 ± 81 ng/m3, respectively. Similar to particles, there were higher
mass fractions of PAHs in smaller particles. The mass fractions of PAHs
bounded to PM2.5, PM1.0 and PM0.25 were 89.3 ± 9.5%, 77.4 ± 15.8%,
and 41.9 ± 11.9% of total PAHs, respectively. The mass percent of PAHs
bounded to PM1.0 accounted for 86.0 ± 11.3% of PAHs bounded to
PM2.5. The high fraction of PAHs bounded to fine particles also could be
explained by indoor biomass burning as a previous study found that
PAHs in PM2.5 could comprise up to 87% to the total PAHs emitted from
biomass burning in residential stoves (Shen et al., 2013b).
The variation in exposed PAHs levels was much larger than the
variation in particle. The lowest exposure level was found for a female
without cooking and smoking activities, while the highest exposure level
was found for a male smoker who also used solid fuel for cooking. Some
non-priority high molecular weight (HMW) PAHs were reported to have
high toxic potentials, even compared to some priority PAH species
(Delistraty, 1997; Zhuo et al., 2017; Du et al., 2020). In this study, the
PAH15 accounted for about 79% to the PAH27 mass, while the BaPeq
calculated based on the 15 priority PAHs comprised to only 62% to the
total BaPeq. Instead of regulations on many PAHs species, BaP is the
most widely concerned and regulated in ambient or indoor air standards
due to its high toxicity. In China, the national standards of BaP in
ambient air and indoor air for 24-hour mean are 2.5 ng/m3 and
1.0 ng/m3, respectively (Ministry of Environmental Protection of China,
2002, 2012). The BaP exposure level for the studied population excee­
ded the standard significantly, in comparison to ambient and indoor air
standards by about 2.6 and 6.5 times, respectively.
The PAHs exposure measured by personal samplers was also limited
to date. And, available studies measured either gaseous or particulate
phases, or both, making it inappropriate to simply compare the reported
total level with one another. BaP (mainly in particle phase) could be a
better choice for comparison across different studies (Zhuo et al., 2017).
Personal BaP exposure from previous studies were summarized in
Table S4. The average BaP exposure in rural China was about 39 ng/m3
(range from 0.1 to 190 ng/m3). The average of BaP exposure in the
present study was 6.5 ng/m3, that was higher than the summertime
studies in northern China (Ding et al., 2012; Chen et al., 2015; Zhang
et al., 2019), but lower than wintertime studies in northern China (Duan
et al., 2014; Du et al., 2018c). The BaP exposure in this study was also
lower than past studies in rural southern area in winter (Lin et al., 2016;
Downward et al., 2014).
3.1.3. Exposure difference across different groups
Personal exposure could be influenced by mass of factors such as fuel
type, cooking and smoking activities, household conditions, etc., (Clark
et al., 2013; Du et al., 2020). In this study, only biomass fuels were used
for daily cooking. And the participants were all rural farmers living in
homes with very similar structure influenced partly by the local culture.
Therefore, here the influence of cooking and smoking activities was
specifically discussed.
In this study, the exposure levels of PM2.5 and PM1.0 were 134 ± 112
and 111 ± 91 μg/m3 for the cooker, and 94 ± 39 and 79 ± 33 μg/m3 for
the non-cooker, respectively. The difference was statistically not sig­
nificant (p > 0.05). The exposure of PM2.5 and PM1.0 were 170 ± 137
and 138 ± 111 μg/m3 for smoker, and 100 ± 63 and 85 ± 53 μg/m3 for
non-smoker. Again, no statistically significant difference was found.
Similar results were in PAHs exposure, in which the exposure levels were
Y. Huang et al.
higher for the cooker compared to the non-cooker, and higher for the
smoker than the non-smoker, but the difference was statistically not
significant (p > 0.05). Though cooking and smoking are considered as
major factors affecting personal exposure, significant differences be­
tween the cooker and non-cooker, and between the smoker and non-
smoker groups could be hardly be revealed by a simple controlled
analysis as various factors may interact with each other. This result was
consistent with several previous studies, such as Zhang et al. (2019) in
Shandong, Du et al. (2017) in Shanxi and Guizhou and Shen et al. (2016)
in Hubei. A study conducted in multiple provinces focused on personal
exposure to PM1.0 and PM1.0-PAHs in rural areas also found the fuel type
was the only significant factor that affected the personal exposure, while
the cooking and smoking activities not (Du et al., 2020). Fig. 1 showed
the exposure level of PMs and PAHs among four subgroups NC&NS (not
cooking, not smoking), C&NS (cooking, not smoking), NC&S (not
cooking, smoking), and C&S (cooking, smoking). A trend that
NC&NS < C&NS< NC&S < C&S could be observed for PMs and PAHs
exposure, but only the difference between C&S and NC&NS was statis­
tically significant (p < 0.05). That the exposure for C&NS is lower than
those for NC&S suggested dominate influence of smoking over cooking
on personal exposure, this was consistent with the larger difference
between smoker and non-smoker than between cooker and non-cooker
revealed in this study, and also consistent the study conducted in
Rural Shanxi (Huang et al., 2017). Both cooking and smoking would
make people be closer to the emission source and elevated the exposure
of cooker and smoker. However, because non-cooker usually stays in the
kitchen during cooking time in the winter for heating purpose in rural
household, the difference between NC and C was minimized, making
cooking be a minor factor affecting personal exposure compared
smoking. Cigarette burning could emit high levels of PM2.5 (Lee et al.,
2021) and largely elevated the exposures of smoker. By applying a linear
model assuming that personal exposures to PMs due to smoking would
linearly increase with the number of cigarettes smoked, increase of
personal exposures by 1.47 ± 1.14, 0.62 ± 0.62 and 1.20 ± 0.69 μg/m3
for PM0.25–1, PM1–2.5 and PM>2.5, respectively, was revealed (Fig. S2).
Dimitroulopoulou et al. (2001) reported an elevated daily PM2.5 con­
centration of 1–1.5 μg/m3 in the living room and Klepeis et al. (2007)
found an increased inhaled PM3.5 concentration by 4 μg/m3 with just
one cigarette smoked. These results demonstrated the significant effect
of smoking on personal exposures.
In many countries, female usually take more responsibility to cook
the meals, resulting in higher potential exposure and catching more
attentions (Agrawal and Yamamoto, 2015; Huang et al., 2015). In the
present study, the personal exposures to PM2.5 and PM1.0 were
140 ± 116 and 115 ± 94 μg/m3 for the male (n = 30), whereas the
levels for the female (n = 30) were 95 ± 68 and 85 ± 58 μg/m3. The
Fig. 1. The personal exposures to PMs and PAHs with different diameters of subgroups of NC&NS, C&NS, NC&S, and C&S. Data shown was mean concentrations and
standard deviations.
4
Ecotoxicology and Environmental Safety 211 (2021) 111959
exposure for the male was higher than that for the female, though not
statistically significant (p > 0.05). In this study, 11 (37% of participated
males) males were recorded both cooking and smoking, 8 (27% of
participated males) males were recorded cooking but non-smoking, and
7 (23% of participated males) males were recorded non-cooking but
smoking, compared to 0, 21(70% of participated females), and 0 for the
female, respectively. It seems that higher proportion of male (87%) did
cooking or smoking than female (70%) was the major cause of higher
exposure for male than female as cook and/or smoking could increase
the exposure level to a certain extent (Huang et al., 2017). A study in
rural Shandong found very close exposure level after subdividing the
residents into cooking male and cooking female (Zhang et al., 2019).
The result here indicated that activities such as cooking and smoking
that mattered the personal exposure instead of gender.
3.2. PAHs composition profiles in inhaled air
Here we compared PM2.5-PAHs composition profiles of inhaled air
(this study) with emission source and indoor air. In the present study,
BbF, PHE, and PYR were the three most dominant species in inhaled air
and they contributed 30% to the total exposure of PAHs in PM2.5, fol­
lowed by CHR, CcdP, and FLA which contributed 25%. Fig. 2. compared
the PAHs composition files in PM2.5 of inhaled air with indoor air in
households using wood and PAHs emission from wood burning (Du
et al., 2018c; Shen et al., 2015). PYR, BbF, and CHR were the three most
dominant species which contributed 42% to the total PAHs in indoor air.
For emission source, PYR, PHE, and FLA were the three most dominant
species, contributing 63% to the total PAHs. PYR was the same dominant
species for inhaled air, indoor air and emission source. BbF was the same
dominant species for inhaled air and indoor air and PHE was the same
dominant species for inhaled air and emission source. It clearly showed
that the PM2.5-PAHs composition profiles of inhaled air was different
from emission source and indoor air, indicating the different environ­
mental fate of PAH species after being emitted to atmosphere from
biomass burning (Zhang et al., 2005a, 2005b).
3.3. The indoor/outdoor contribution to inhalation exposure
In previous studies, personal exposure was found well positively
correlated with indoor and outdoor pollutants concentration (Du et al.,
2017; Zhang et al., 2019), but limited studies estimated the relative
contribution of indoor and outdoor air to inhalation exposure. In this
study, Monte Carlo runs 10,000 times to estimate the contribution of
indoor and outdoor air and results were presented in Fig. 3. The esti­
mated contribution of outdoor PM2.5 and PAHs followed left-skewed
distributions with relatively narrow variation and the contribution of
Y. Huang et al. Ecotoxicology and Environmental Safety 211 (2021) 111959

Fig. 2. Comparison of PM2.5-PAHs composition profiles of inhaled air with emission source and indoor air.

Fig. 3. Relative contribution of indoor/outdoor PM2.5 and PAHs to the inhalation exposure.

indoor PM2.5 and PAHs followed right-skewed distributions. The indoor
PM2.5 contributed 88% (78–93% as interquartile range) to the inhala­
tion exposure, significantly higher than the contribution of outdoor
PM2.5 and similar result was found in PAHs. The expected result that
indoor air pollution contributed more than outdoor air to inhalation
exposure could be explained by severer indoor pollution associated with
strong internal emission and longer time spent in indoor environments
(Ministry of Environmental Protection (MEP), 2013; Du et al., 2018b).
This result indicated the inhalation exposure highly depended on indoor
air pollution, which was extremely severe in the study area due to
biomass burning.
3.4. Size distribution
There are few studies on the size distributions of PMs and PAHs in
inhaled air so far. Fig. 4 showed the size distribution of PMs, PAH27, and
BaPeq in inhaled air of the rural populations in the Eastern Tibetan
Plateau. The size distributions were similar among PMs, PAH27, and
BaPeq. The 0.25–1.0 and <0.25 µm fractions were the dominant frac­
tions, which could be explained by the fact that particles from com­
bustion sources were usually very small (Shen et al., 2012, 2013c). The
fraction of BaPeq in PM0.25 was 0.52, higher than the fraction of PAH27
in PM0.25 (0.42), indicating the PM0.25 not only has high PAHs level, but
also high potential risk.

5
Y. Huang et al.
Fig. 4. Size distribution of PMs (A), PAH27 (B), and BaPeq(C) in inhaled air of rural populations in the Eastern Tibetan Plateau.
Fig. 5 showed the relative mass fraction of PAHs with different rings
in PMs with different diameters, the mass fraction of PAHs with 5–6
rings increased when the PM diameter decreased, opposite to the trend
of PAHs with 2–3 rings. Given the PAHs with higher molecular weight
(more rings) were more toxic (Delistraty, 1997), and along with high
mass concentration in finer particles such as PM0.25, the finer particles
could result in severer health outcome compared to the coarse ones.
3.5. Risk assessment
The estimated values of RR and PAF for the morbidity of acute lower
respiratory infections (ALRI) and mortality caused by chronic obstruc­
tive pulmonary diseases (COPD), lung cancer (LC), and ischemic heart
disease (IHD) and stroke associated to personal PM2.5 exposure were
listed in Table S5. In the studied area, the PM exposure contributed to
54% of morbidity of ALRI and 30%, 38%, 30, 53% of mortality caused
by COPD, LC, IHD and stroke, respectively. The RR and PAF for the male
were higher than those for the female. Similar to the result of PM2.5
exposure, the C&S group had the highest exposure risk associated with
PM2.5 exposure, followed by NC&S, C&NS, and NC&NS group. The RR
and PAF for population in this study were higher than China national
average reported by previous studies (Cohen et al., 2017; Yun et al.,
2020), mainly due to higher exposure levels here with the inclusion of
severe indoor air pollution caused by use solid biomass. However, the
RR and PAF for the people in the studied areas were lower than those for
the people using solid biomass in a rural village in north of China (Huang
et al., 2017), because of higher heating demand due to lower tempera­
ture in northern China. Indoor air, especially in rural households using
solid fuels, is heavily polluted, and residents usually stay longer in
Fig. 5. The relative fraction of PAHs with different rings in PMs with
different diameters.
6
Ecotoxicology and Environmental Safety 211 (2021) 111959
indoor, resulting in high exposure levels. Some recent studies taking
both the indoor and ambient air pollution exposure into account pur­
posed integrated population-weighted exposure (IPWE) when esti­
mating personal exposure from stationary sampling results (Zhao et al.,
2018; Chen et al., 2018). The IPWE was believed to closer to real
exposure levels if an indirect estimation method was adopted, instead of
using direct personal exposure measurement.
The geomean of incremental lifetime cancer risk (ILCR) associated
with PAHs exposure estimated for rural residents in this study was
1.2 × 10− 5, lower than 3.3 × 10− 5 for rural residents in Taiyuan due to
larger heating demand in this area (Duan et al., 2014). And for the male
and the female, the ILCR values were 1.3 × 10− 5 and 1.0 × 10− 5,
respectively. The estimated ILCR followed a decreased trend of C&S,
NC&S, C&NS, and NC&NS group. Although the ILCR estimated in this
study was lower than the serious level 10− 4, but still higher than the
acceptable risk level of 10− 6 (Asante-Duah, 2002). It should be noted
that such estimation might overestimated the risk due to respiratory
exposure of PAHs, as the exposure concentration was only based on the
wintertime study. Given lower pollution levels in summer (Du et al.,
2018b), the lifetime exposure could be lower, resulting in lower risks
associated with PAHs exposure in this area.
3.6. Implications and limitations
High exposure to PMs and PAHs associated with solid fuel use is
associated with foreseeable health risk, however, this problem has been
overlooked in a long time (Zhao et al., 2018). In the last few years, clean
fuel was becoming popular in some areas (Tao et al., 2018), but in many
remote villages they still rely on traditional solid fuels including raw
coal and biomass fuels, resulting in severe inhalation exposure (Shen
et al., 2019). For a better understanding on harmful health impacts
associated with HAP exposure, it is necessary to accurately evaluate
personal exposure to products of incomplete combustion by using more
reliable and accurate measurement technologies.
The present study found high exposure levels, but also high fractions
of finer particles in inhaled air, the PM1.0 contributed more than 70% to
the total PM exposure. The outdoor PM2.5 contributed only 17% to the
total exposure, compared to 83% of the indoor PM2.5 contribution,
indicating the personal exposure was highly depended on indoor air
pollution. PAHs, especially those with higher molecular weight, were
likely to distribute on fine particles, indicating that the household air
pollution and inhalation exposure for rural residents burning solid fuels
should be paid more attention to and clean intervention was in urgent
need.
It is recognized that the sample size was still considerably small, even
though much high costs and field working labor intensity are required in
such field campaigns, especially in filter-based personal sampling
Y. Huang et al.
technologies. The present study did not sample household air simulta­
neously, which made it difficult to compare indoor and outdoor expo­
sure. The relative contributions of household air pollution to the total
exposure here estimated by Monte Carlo and results from previous
studies might cause uncertainties. However, it is believed that indoor
exposure could contribute largely to the overall exposure as a result of
high indoor pollution levels and long indoor residue time. And, the
present results are from one season, thus the exposure concentration can
be hardly to representative the yearly or lifetime average exposure. This
results in relatively high biases in exposure risk assessment. Most
experimental studies so far can hardly afford a long-term follow-up
observation and measurements. These should be paid more attention
when generalizing the results, and it is also expected that future studies
can be improved in some aspects to overcome these limitations.
4. Conclusion
Household air pollution has been recognized as one top environ­
mental risk factor in rural China, however, field investigations on per­
sonal inhalation exposure using personal samplers were still very
limited, especially scarce on the information of size segregated particles
and components such as toxic PAHs. The present field study conducted
in Eastern Tibetan Plateau found that personal daily exposure to PM2.5
and PM1.0 was 121 ± 96 and 101 ± 78 μg/m3 respectively, and
103 ± 185 and 91 ± 177 ng/m3 for PAH27 bounded to PM2.5 and PM1.0.
Inhaled particles are very small with high mass fractions of 0.25–1.0 and
< 0.25 µm due to biomass burning. The size distribution result indicated
ultrafine particles were not only associated with high concentration of
PAHs, but also with high toxic PAH species, which might cause severe
health outcome on local residents. The indoor PM2.5 pollution contrib­
uted more than 80% to the total exposure, indicating the indoor air
pollution associated with biomass burning is strongly responsible for the
severe personal exposure in this area. PAHs composition profiles of
inhaled air was different from emission source and indoor air, indicating
the different environmental fate of PAH species after being emitted to
atmosphere from biomass burning. Given the high health risk associated
with PMs and PAHs exposure, clean intervention was in urgent need to
improve the household air quality to protect rural residents’ health.
CRediT authorship contribution statement
Ye Huang: Formal analysis, Funding acquisition, Visualization,
Writing - original draft. Jinze Wang: Investigation, Writing - review &
editing. Nan Fu: Investigation, Writing - review & editing. Shanshan
Zhang: Investigation, Writing - review & editing. Wei Du: Conceptu­
alization, Formal analysis, Funding acquisition, Methodology, Visuali­
zation, Validation, Writing - original draft, Writing - review & editing.
YuanChen Chen: Funding acquisition, Writing - review & editing.
Zhenglu Wang: Investigation, Writing - review & editing. Meng Qi:
Investigation, Writing - review & editing. Wei Wang: Investigation,
Writing - review & editing. Qirui Zhong: Formal analysis, Writing -
review & editing. Yonghong Duan: Investigation, Writing - review &
editing. Guofeng Shen: Conceptualization, Funding acquisition, Meth­
odology, Writing - original draft. Shu Tao: Conceptualization, Funding
acquisition, Methodology, Writing - review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgement
We sincerely thank all the volunteers and rural residents partici­
pating in this field campaign. This work was supported by the National
7
Ecotoxicology and Environmental Safety 211 (2021) 111959
Natural Science Foundation of China (41922057, 41830641, 42077328,
41907313, 41730646, 41701584), Ministry of Science and Technology,
People’s Republic of China (2019QZKK0605), Science and Technology
Commission of Shanghai Municipality (19ZR1415100), the Chinese
Academy of Sciences (XDA23010100), and China Postdoctoral Science
Foundation (2019M661425).
Appendix A. Supporting information
Supplementary data associated with this article can be found in the
online version at doi:10.1016/j.ecoenv.2021.111959.
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