Professional Documents
Culture Documents
www.elsevier.com/locate/jes
90110, Thailand
a r t i c l e i n f o a b s t r a c t
Article history: Distribution of PM0.1 , PM1 and PM2.5 particle- and gas-polycyclic aromatic hydrocarbons
Received 28 June 2021 (PAHs) during the 2019 normal, partial and strong haze periods at a background location in
Revised 9 October 2021 southern Thailand were investigated to understand the behaviors and carcinogenic risks.
Accepted 2 November 2021 PM1 was the predominant component, during partial and strong haze periods, accounting
for 45.1% and 52.9% of total suspended particulate matter, respectively, while during nor-
mal period the contribution was only 34.0%. PM0.1 concentrations, during the strong haze
Keywords: period, were approximately 2 times higher than those during the normal period. Substan-
Particle-PAH tially increased levels of particle-PAHs for PM0.1 , PM1 and PM2.5 were observed during strong
Gas-PAH haze period, about 3, 5 and 6 times higher than those during normal period. Gas-PAH con-
Ultrafine particle centrations were 10 to 36 times higher than those of particle-PAHs for PM2.5 . Average total
Health risk Benzo[a]Pyrene Toxic Equivalency Quotients (BaP-TEQ) in PM0.1 , PM1 and PM2.5 during haze
Source identification periods were about 2–6 times higher than in the normal period. The total accumulated Incre-
mental Lifetime Cancer Risks (ILCRs) in PM0.1 , PM1 and PM2.5 for all the age-specific groups
∗
Corresponding author.
E-mail: racha.d@psu.ac.th (R. Dejchanchaiwong).
https://doi.org/10.1016/j.jes.2021.11.005
1001-0742/© 2022 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.
254 journal of environmental sciences 124 (2023) 253–267
during the haze effected scenario were approximately 1.5 times higher than those in non-
haze scenario, indicating a higher potential carcinogenic risk. These observations suggest
PM0.1 , PM1 and PM2.5 were the significant sources of carcinogenic aerosols and were signifi-
cantly affected by transboundary haze from peatland fires. This leads to an increase in the
volume of smoke aerosol, exerting a significant impact on air quality in southern Thailand,
as well as many other countries in lower southeast Asia.
© 2022 The Research Center for Eco-Environmental Sciences, Chinese Academy of
Sciences. Published by Elsevier B.V.
(Chomanee et al., 2020) and no effort has been made to an inertial filter was used to collect particles in the 0.1–0.5 μm
distinguish the cause of health risks from peatland fires from (PM0.1-0.5 ) range. PM0.1 represents the sample collected from
clean background. the last stage, PM1 is a combination of the last 3 stages, and
The key contributions of this paper are investigations of PM2.5 is the sum of PM1 and another stage upstream. A 55-
the transboundary ultrafine particles affecting southern Thai- mm quartz fiber filter (2500QAT- UP, Pallflex, USA) was used
land atmosphere and the health risks for the population. The for collection in each stage. The stage with an inertial filter (IF)
current research aims to distinguish the fine (< 1 μm) and ul- used a stainless-steel filter pack (SUS304, fiber diameter = 9.8
trafine (<100 nm) particles- and gas-PAH effects to southern μm) to collect PM0.1-0.5 . The filter samples were treated (dried)
Thailand as a result of transboundary haze from peatland fires in a controlled desiccator (50±5% RH and 25±2°C for 72 hr).
in Indonesia. Samples were collected at the Songkhla Com- The temperature was far below the lowest boiling point of the
munity College site, Songkhla Province, Thailand (6°49 35.3 N PAHs (napthalene, 80°C). It was then weighed on an analyt-
100°57 59.3 E), where the haze was expected to have strong ical balance (CP225D, Sartorius, Germany, resolution 0.01mg)
influence on an otherwise a relatively clean air background. located in the room kept at 25 ± 2°C. The samples were kept in
Samples were taken in three periods: (a) strong haze (Sep a plastic bag wrapped by aluminium foil before analysis. This
2019), (b) partial haze (Jun-Aug 2019) and (c) normal (Jan-May, is an accepted procedure (Tan et al., 2005 and Furuuchi et al.,
Oct-Dec 2019). The PAHs in particles and gas phases were an- 2007) and the degradation of PAHs was minimized. Amber-
alyzed. We wanted to determine the chemical components lite resin XAD-2 (21130-U, Supelco, USA), a gas sampler based
and assess elevated risk of human exposure to fine and ultra- on the adsorption principle, was used to collect the non-polar
fine particles bound PAHs during the haze period in southern gas-phase PAHs from the air at the same site. The XAD-2 resin
part of Thailand. Human exposure risk assessments were es- adsorbent was contained in a tube cartridge, with inlet and
timated by using BaP-TEQ and ILCR of fine and ultrafine par- outlets are closed with polyurethane foam. The operating air
ticle bound PAHs via inhalation. Source identification by di- flow rate was 2 L/min and sampling time was 7 hr. In a pre-
agnostic particle-PAHs, chemical mass balance (CMB) model liminary test, a suitable time for XAD-2 collection to obtain
and air mass backward trajectory were used to confirm the PM sufficient PAHs for analysis was 7 hr, with a 2 L/min air flow.
sources. Moreover, these data are important for understand- The cartridges were closed on both ends and wrapped in alu-
ing the behavior of background fine and ultrafine particles and minum foil to avoid photodegradation after sampling. Sam-
associated chemical species. They are also valuable in future ples were collected from January-December 2019: six samples,
planning and actions to control PAH sources to improve air during the normal period (Jan-May, Oct–Dec 2019), three, dur-
quality in lower SEA. ing the partial haze period (Jun-Aug 2019), and one, during
the strong haze period (Sep 2019), were collected using the
nanosampler for PM sampling and the XAD-2 resin for gas
1. Methodology sampling at the SKTP site. The number of months of each pe-
riod was estimated from the PM2.5 concentration in a nearby
1.1. Sampling site and physical analysis city, Hat Yai, measured by the Pollution Control Department
(PCD, 2021). Details are summarized in Table S1. In the follow-
Samples were collected at Songkhla Community College ing text, ‘normal period’ refers to the reference, normal peri-
(SKTP site), Thepha District, Songkhla Province, Thailand ods in Jan-May 2019 and Oct-Dec 2019 and ‘partial haze period’
(6°49 35.3 N 100°57 59.3 E), see Fig. 1. Thepha District is ∼80 km and ‘strong haze period’refer to periods defined in Table S1.
southeast of Hat Yai, Songkhla Province, which is the major
city in lower southern Thailand. It is a small city, where back- 1.2. PAH analysis
ground air is generally clean, and industrial, traffic and house-
hold emissions are considered low. There is only one small The 16 PAH compounds, classified by the United States En-
9.9 MW biomass power plant, located about 5 km northwest vironmental Protection Agency (U.S. EPA) as priority pollu-
of the sampling point. It does not significantly influence the tants, because of their potential toxicity in humans and other
background air, especially during the haze period, when the organisms and their prevalence and persistence in the en-
wind blows from the southwest. Weather in southern Thai- vironment (Hussar et al., 2012), were analyzed. The filter
land receives influence from the southwest monsoon, during and XAD-2 resin samples were extracted twice in 20 mL
May-October, and the northeast monsoon, during November- dichloromethane using an ultrasonic bath at a controlled tem-
January. These two seasons are separated by two relatively perature (∼5°C). 50 μL dimethyl sulfoxide was added to the
short inter-monsoon periods where wind directions vary con- extract and then dried in a rotary evaporator until nearly dry
siderably. Samples were collected on the top floor of a PM (∼50 μL). The residue was dissolved in 450 μL acetonitrile, fol-
monitoring station, ∼3 m above ground (U.S.EPA, 2011). lowing Phoungthong et al. (2013). The 16 priority PAHs were
A PM0.1 sampler or nanosampler, capable of segregating determined using a high-performance liquid chromatograph
particle size to 100 nm, was used to collect samples (Furuuchi (HPLC, Model-1100, Agilent, USA) with coupled diode array and
et al., 2010). Operating air flow rate was 40 L/min and sampling fluorescence detectors (HLPC-DAD/FLD). The portion of the ex-
time was 144 h during normal, partial and strong haze periods. tracted (20 μL) was injected into an Inersil ODS-PC-18 reversed
Particles were separated into six size ranges: <0.1 μm (PM<0.1 ), phase column, connected to a 5 μm guard column (particle
0.1–0.5 μm (PM0.1-0.5 ), 0.5–1.0 μm (PM0.5-1 ), 1.0–2.5 μm (PM1-2.5 ), size 5 μm, 4.6 mm diameter, 250 mm length).
2.5–10 μm (PM2.5-10 ) and >10 μm (PM>10 ). Particle size classifi- Extensive quality (QA/QC) controls were used. All field
cation on each stage used an impaction mechanism, whereas and laboratory blank filters were analyzed. The recovery of
256 journal of environmental sciences 124 (2023) 253–267
individual PAHs in the spiked samples ranged from 71.0% to it can quantitatively identify sources. The CMB model uses
108.4%. The limit of detection was determined from the con- the chemical composition of aerosols to estimate the contri-
centration of PAHs required to give a signal to noise ratio butions of different sources to the concentrations at the re-
≥ 3. Detection limits of the analytical procedure were 1.9– ceptor. In the present study, CMB analysis, using the CMB8.2
40.8 ng/mL for individual PAHs. The detection limits and per- software obtained from the U.S. EPA website, was used to iden-
cent recovery of 16 PAHs in the present study are shown in tify sources (U.S. EPA, 2005). The CMB outputs are acceptable
Table S2. Similar to the filter treatment and PAHs analysis, the when the performance indices are all within the target ranges;
spiked filters were treated in the desiccator for 72 h and then R2 ∈ (0.8, 1.0), χ 2 ∈ (0.0, 4.0), percent mass (% mass): 100% ± 20%
extracted and analyzed. The chemical component concentra- (U.S. EPA, 2004a). The CMB receptor model can be expressed as
tion in the blank filters (n = 3) was subtracted from the sam- (U.S.EPA, 2004b):
ples. To calibrate our system, stock solutions of the 16 PAHs
p
in acetonitrile were prepared by weighing and then diluted
to give concentrations ranging from 0.01 to 20 μg/ml. For all xi j = gik fk j + ei j (1)
k=1
16 compounds, a linear correlation between known solution
concentrations and peak areas was found with R2 > 0.99.
where xi j is the ambient concentration of chemical species
( j) measured in sample (i), gik is the concentration contributed
1.3. Source identification by source (k) to sample (i), fk j is the fractional concentration
of chemical species ( j) in the emission from source (k) and ei j
1.3.1. PAHs diagnostic ratio is the residual concentration of chemical species ( j) measured
The pair - Flu/(Flu+Pyr) and IDP/(IDP+BghiPe) - is com- in sample (i).
monly used to characterize PAH sources. Flu/(Flu+Pyr) and
IDP/(IDP+BghiPe) ratios > 0.5 indicate strong biomass burn- 1.3.3. Backward trajectory
ing, whereas the ratios < 0.5 indicate strong combustion fuel 72-h backward trajectories (BT) of air and aerosol particles
as a source (Wiriya et al., 2013). Here, the ratios were used to from possible external sources was simulated using the
identify PAH sources of PM0.1 , PM1 and PM2.5 in southern Thai- Hybrid Single-Particle Lagrangian Trajectory (HYSPLIT) model
land. (Air Resources Laboratory, 2021). Backward trajectory simula-
tion of wind direction at 1000 m altitude (AGL) was overlaid
1.3.2. CMB model with hotspots in lower southeast Asia, obtained from the
The chemical mass balance (CMB) receptor model, developed NASA VIIRS 375 m active fire data (Earthdata, 2021). More
by the U.S. EPA, was also used in the present study, because details of the analytical methods for BT can be found
journal of environmental sciences 124 (2023) 253–267 257
Fig. 2 – PM concentrations and PM mass fraction at SKTP site during three periods in the present study.
ular weight (HMW-PAHs, 4–6 rings) groups, during normal, par- 83.8% to PM0.1 , 70.5–81.4% to PM1 and 68.9–79.7% to PM2.5 .
tial and strong haze periods, are shown in Fig. 3. The aver- Moreover, HMW-PAH concentrations, in both PM2.5 and PM1,
age total PAH concentrations during the strong haze period during partial and strong haze periods were approximately
were - PM0.1 0.28 ± 0.02 ng/m3 , PM1 1.75 ± 0.13 ng/m3 , and 2 and 5 times higher than those during the normal period,
PM2.5 2.52 ± 0.19 ng/m3 , while during partial haze and nor- respectively. However, HMW-PAH concentrations in PM0.1 in-
mal periods, they were 0.15 ± 0.03 and 0.11 ± 0.01 ng/m3 for creased only slightly during partial and strong haze periods
PM0.1 , 0.70 ± 0.05 and 0.34 ± 0.03 ng/m3 for PM1 , 0.90 ± 0.06 versus the normal period. This indicated that fine and ul-
and 0.43 ± 0.04 ng/m3 for PM2.5 , respectively. The total PAH trafine particles were the significant source of carcinogenic
concentrations in PM1 during partial and strong haze peri- aerosols, especially, during haze periods. Conversely, the to-
ods were 5 times higher than those during normal period. tal gas-PAH concentrations were dominated by LMW-PAHs,
The PAH concentrations in PM1 in these periods were 69.4– accounting for 94.4%–98.8%. This is because LMW-PAHs have
77.9% of PAH concentrations in PM2.5 , revealing that PAHs low boiling points and can be easily present in the gas phase
were mainly in <1 μm particles. This was consistent with (Ho et al., 2009). The predominant compounds were two-ring
Dejchanchaiwong et al. (2020), who found that the highest PAH (Nap) PAHs (46.6–64.2%) and three-ring ones (Act, Ace+Fle,
concentrations, in Bangkok during 2018–2019 haze period, af- Phe and Ant) (34.7%–48.5%) of gas PAHs in three periods. This
fected by biomass burning, were in the PM0.5–1.0 range. The agrees with Ho et al. (2009), who reported that LMW-PAHs
PAHs in PM0.1 during strong haze period were 3 times as high were the most abundant gas-PAHs and HMW-PAHs were most
as those in a normal period. abundant particle-PAHs.
Gas-PAHs in samples contained only 7 PAHs: Nap, Act,
Ace+Fle, Phe and Ant (LMW-PAHs) and Flu and Pyr (HMW- 2.2.2. Profiles of PAHs in the particle and gas phases
PAHs). Average gas-PAH concentrations were during normal Individual concentrations of particle- and gas-PAHs are listed
15.4 ± 2.6 ng/m3 , partial 10.8 ± 2.6 and strong 26.0 ± 5.2 haze in Fig. 4. Nap, Act, and Phe were dominant for LMW particle-
periods. The gas-PAH concentrations during the strong haze PAHs (2-3 ring), while BbF, BkF, and DBA were the most abun-
period increased by 69.4% compared to the normal period. In dant for HMW particle-PAHs (4-6 ring) in every period. More-
contrast, a decrease of 29.3% partial vs normal periods was over, BaP and IDP also dominated in the HMW particle-PAHs,
observed. In our observations, gas-PAH concentrations were during partial and strong haze periods. Benzo[a]pyrene (BaP)
10 to 36 times higher than PM2.5 particle-PAHs. HMW-PAHs (4- is a significant carcinogen and mainly present in the par-
6 rings) in particles, over the entire period, contributed 66.9– ticle phase, consistent with the study of Jiang et al. (2014).
journal of environmental sciences 124 (2023) 253–267 259
Fig. 3 – Particle- and gas-PAH concentrations during normal, partial and strong haze periods.
The average BaP (particle phase) concentrations during par- (0.04 ± 0.01 ng/m3 ), partial (0.08 ± 0.05 ng/m3 ) and strong haze
tial and strong haze periods were 0.052 and 0.095 ng/m3 periods (0.25 ng/m3 ). It is important to note, that fine and ul-
in PM2.5 , or 6 and 11 times higher than in the normal pe- trafine particles are a more significant source of carcinogens
riod (0.009 ng/m3 ), indicating more damage to human health. and cause more health effects, than larger particles, due to
BaP in PM1 contributed to 74.0–91.1% of BaP-PM2.5 . For gas- their higher surface areas.
PAHs, Nap (7.1 ± 4.8 ng/m3 ), Act (4.4 ± 2.5 ng/m3 ) and Phe
(1.9 ± 1.5 ng/m3 ) were dominant, during normal period,
whereas in partial and strong haze periods, they were: Nap
2.3.2. ILCR Values of PAHs in PM0.1 , PM1 and PM2.5
The ILCR of inhalation by exposure to PM-bound PAHs ob-
(7.0 ± 2.0 and 14.7 ng/m3 ), Act (2.9 ± 2.3 and 5.6 ng/m3 ) and
tained from Eq. (3) and total accumulated ILCR risks for PM0.1 ,
Ace+Fle (0.7 ± 0.7 and 3.2 ng/m3 ), i.e. higher by two orders
PM1 , and PM2.5 during the haze effected and non-haze scenar-
of magnitude than in the particle phase, similar to reports by
ios are shown in Fig S1. An ILCR ≤ 10−6 is considered safe, ILCR
Ho et al. (2009).
from 10−6 to 10−4 indicates a potential risk, and ILCR ≥ 10−4 is
considered high risk (Fang et al., 2020). ILCR values increased
2.3. Health risk assessment with age from infant (0–1 year old) to adult (30–70 years old)
for both haze affected and non-haze scenarios, except for the
2.3.1. BaP-TEQ size distribution of PAHs in particles toddler age group (1–6 years). This was mainly attributed to
The BaP-TEQ concentrations for each particle size range dur- the relatively shorter exposure duration (5 years) and lower
ing all periods calculated by Eq. (2) are shown in Fig. 5. Average body mass for the toddler group. This suggested that toxic
BaP-TEQ concentrations during partial and strong haze peri- PAHs can accumulate in the human body. The highest ILCRs
ods were 0.03 ± 0.02 and 0.07 μg/m3 for PM0.1 , 0.15 ± 0.11 and were 6.7 × 10−8 (haze affected scenario) and 4.3 × 10−8 (non-
0.43 μg/m3 for PM1 and 0.16 ± 0.11 and 0.62 μg/m3 for PM2.5 , haze scenario) in the adult group (30–70 years) for PM2.5 , sug-
while during normal period, the values were 0.03 ± 0.02 μg/m3 gesting that adults over 30 years old may be at higher risk of
for PM0.1 , 0.09 ± 0.03 μg/m3 for PM1 and 0.10 ± 0.04 μg/m3 for developing cancer in haze affected than non-haze scenarios
PM2.5 . A large increase of BaP-TEQ concentrations in PM1 and (Chen and Liao, 2006).
PM2.5 , during the strong haze period, was found - 5 and 6 times The total accumulated ILCRs for all the age-specific groups
higher than the normal period. Also, the average BaP-TEQ con- during the haze effected and non-haze scenarios are shown
centrations in PM0.1 during partial and strong periods were in Table 2. The risks during the haze effected scenario were
slightly higher than those in normal period. The BaP-TEQ con- approximately 1.5 times higher than those for non-haze
centrations in PM1 occupied from 68.7- to 91.3%, while PM0.1 scenario. This was consistent with previous studies which
contributed to 10.5- to 28.9% of BaP-TEQ in PM2.5 . Moreover, showed that total ILCRs under the biomass burning conditions
while the BaP-TEQ PM0.1 concentration was 10.5% to 28.9%, were higher than those under clean conditions (Lu et al., 2016;
the mass fraction was only 6.0–6.9%. This clearly indicated Zhang et al., 2019). Contribution of PM0.1 in total ILCRs was
that the health risk caused by exposure to fine (< 1 μm) and 28.9% of the PM2.5 in haze effected scenario compared to 20.8%
ultrafine (<100 nm) was significantly elevated, when haze oc- in non-haze scenario. The influence of PM1 was 83.0% in haze
curred for a prolonged period. Moreover, the highest BaP-TEQ effected scenario compared to 80.5% in non-haze scenario. It
contributions were found in PM0.5-1.0 particles during normal is clear that PM1 plays an essential role in cancer risks from
260 journal of environmental sciences 124 (2023) 253–267
Fig. 4 – Individual particle- and gas-PAH concentrations during the 2019 normal, partial and strong haze periods.
Table 2 – Total accumulated ILCRs for all the age-specific groups during the haze effected and non-haze scenarios.
Particle size
Scenarios
PM0.1 PM1 PM2.5
Fig. 5 – BaP-TEQ concentrations for PM0.1, PM1 and PM2.5 during three periods in the present study.
PM2.5 , but the effect of PM0.1 is also significant. An increment higher than those during 2017 normal period (1.29-2.31 μg/m3
of total ILCR in PM0.1 , PM1 and PM2.5 for all the age-specific and 0.3–0.4 ng/m3 ). In this study, total PAH concentrations
groups during the haze periods indicated the higher potential in PM2.5 , during the haze period, were 2.5 ± 0.19 ng/m3
cancer risks. This suggests that the accumulated ILCR risks (strong haze) and 0.9 ± 0.06 ng/m3 (partial haze), similar
during the haze episode had more detrimental health effects to those measured by Dejchanchaiwong et al. (2020), during
than the normal period, as a result of higher PM and PAH con- the haze period in Bangkok, Thailand (1.3 ± 0.2-2.4 ± 0.9
centrations. However, they were still in the ‘safe band’, but the ng/m3 ), and Sulong et al. (2019) in Kuala Lumpur, Malaysia
haze affected period was only short. We note that our conclu- (2.51 ± 0.93-3.40 ± 0.68 ng/m3 ). For PM0.1 , the total PAH
sion may be limited to conditions in the current work and a concentration during partial (0.2 ± 0.01 ng/m3 ) and strong
specific location. However, it suggests that stronger and longer (0.3 ± 0.02 ng/m3 ) haze periods were much lower than those
haze periods could be detrimental to health and it is impor- reported earlier by Chomanee et al. (2020) in Hat Yai, Thai-
tant to control or limit the sources of haze, so that the effects land (1.1–4.8 ng/m3 for haze period), but following a simi-
remain within acceptable levels. lar trend to Dejchanchaiwong et al. (2020) in Bangkok, Thai-
land (0.3 ± 0.1 ng/m3 and 0.5 ± 0.2 ng/m3 ). This was because
2.4. Comparison of particle-PAHs in lower southeast Asia southern Thailand was more severely hit by the transbound-
ary haze in 2015 than the 2019 counterpart. Human expo-
The PM, PAHs and BaP-TEQ concentrations in this and previ- sure to PM-bound PAHs during haze periods showed higher
ous studies in lower SEA are shown in Table 3. In Malaysia, carcinogenic risks and was similar to those found in central
PM10 and PAH concentrations during 2010-2011 in Kuala Thailand (Dejchanchaiwong et al., 2020), southern Thailand
Lumpur, Petaling Jaya, and Bangi increased during dry seasons (Chomanee et al., 2020), Malaysia (Jamhari et al., 2014) and
(Jamhari et al., 2014). PM2.5 concentration in Kuala Lumpur Singapore (Urbancok et al., 2017). The PM0.1 and PAH concen-
during the year 2015 was enhanced by biomass burning in tration during the normal period in this study were approxi-
Sumatra, Indonesia (Sulong et al., 2019). PAH concentrations mately 3-10 times lower than the previous studies in Hat Yai
during the 2015 haze period was 3.40 ± 0.68 ng/m3 , ap- (Chomanee et al., 2020) and Bangkok (Dejchanchaiwong et al.,
proximately 2 times higher than those during normal period 2020). This confirmed that the atmosphere in the sampling
(1.37 ± 0.09 ng/m3 ). During the 2006 haze period in Singa- site in this study was generally ‘clean’, i.e. industrial, traf-
pore, TSP concentration was 94.1 ± 33.4 μg/m3 compared to fic and household emissions were considered low. Hence, the
24.0 ± 5.2 μg/m3 , during the non-haze period (Engling et al., high values of PM and PAH concentrations during haze peri-
2014). PAH concentrations increased from 2.1 ± 1.3 ng/m3 ods can be attributed mainly to transboundary air pollutants
during the non-haze period to 6.9 ± 2.4 ng/m3 during the from Sumatra, Indonesia.
haze period, a threefold rise. In the recent and severe haze
episode of 2015, PAH concentrations on PM10 ranged from 2.5. Effect of transboundary haze on air quality in
1.07 to 5.97 ng/m3 compared to 0.68 to 3.07 ng/m3 during the southern Thailand
non-haze period (Urbancok et al., 2017). In southern Thai-
land, concentrations in Hat Yai during the 2013 haze period 2.5.1. PAH diagnostic ratios
were as high as 46.0-112.7 μg/m3 for TSP and 11.8–26.6 ng/m3 The PAHs diagnostic ratios are commonly used as chemical
for PAHs, and very high during the 2015 haze period (322.5 trackers to identify sources of PAHs. Here, the PAH ratios of
μg/m3 for PM10 and 4.3-35.6 ng/m3 for PAHs) (Chomanee et al., Flu/(Flu+Pyr) and IDP/(IDP+BghiPe) were used to identify the
2020). PM0.1 and PAH concentrations during the 2015 haze pe- potential PAH sources of PM0.1 , PM1 and PM2.5 in southern
riod were from 3.7 to 23.6 μg/m3 and 1.1–4.8 ng/m3 , much Thailand, as shown in Fig. S2. The values during the partial
262
Table 3 – PM, PAHs and BaP-TEQs concentrations reported in this and previous studies in lower SEA
Site Site classification Periods Particle size PM (μg/m3 ) PAHs (ng/m3 ) BaP-TEQ (ng/m3 ) References
Thepa, Songkhla Sub-urban Normal PM0.1 1.4 ± 0.9 0.1 ± 0.01 0.03 ± 0.02 This study
PM1 7.8 ± 2.2 0.3 ± 0.03 0.09 ± 0.03
PM2.5 10.7 ± 3.5 0.4 ± 0.04 0.10 ± 0.04
Partial haze PM0.1 2.0 ± 1.0 0.2 ± 0.03 0.03 ± 0.02
PM1 15.9 ± 2.3 0.7 ± 0.05 0.15 ± 0.11
PM2.5 21.6 ± 2.4 0.9 ± 0.06 0.16 ± 0.11
Fig. 6 – CMB results during strong haze, partial haze and normal periods for (a) PM2.5 , (b) PM1 and (c) PM0.1 .
haze and normal periods were in the lower and upper right industries in the southern part of Thailand were mainly
quadrant, whereas during the strong haze period, they were connected to agriculture, especially natural rubber plants
in the upper right quadrant. Hence, the ratios indicated that (Tekasakul et al., 2008; Dejchanchaiwong et al., 2017, 2019).
the major sources of PM during strong haze period were dom- The residues from rubber plants were used as the main fuel in
inantly from biomass burning. It indicated a clear influence many industries in this area as well as agricultural activities
of peatland fire emission for PM0.1 , PM1 and PM2.5 , though the which releases environmental pollutants, especially PM and
PM2.5 influence on was strongest, similar to trends in previ- PAHs (Chomanee et al., 2018; Phairuang et al., 2019).
ous studies (Chomanee et al., 2020; Phairuang et al., 2020).
This agrees with Phairuang et al. (2020) - those sources of 2.5.2. CMB analysis
PM0.1 were a mix of vehicle combustion and biomass burn- The CMB model using Eq. (1) was applied to determine the pri-
ing, even when biomass burning dominated. The petroleum mary source contributions to PAH components in PM. Here,
and biomass combustions were the leading sources of PM the primary categories of local sources were bituminous,
during partial haze and normal periods. This is because the palm fiber, palm kernel, rubber wood, biomass burning, diesel
264 journal of environmental sciences 124 (2023) 253–267
during the strong haze period were approximately 2 times Chen, S.-C., Liao, C.-M., 2006. Health risk assessment on human
higher than those during the normal period. Levels of PAHs exposed to environmental polycyclic aromatic hydrocarbons
during the strong haze period for fine and ultrafine particles pollution sources. Sci. Total Environ. 366 (1), 112–123.
Chen, Y.C., Chiang, H.C., Hsu, C.Y., Yang, T.T., Lin, T.Y., Chen, M.J.,
were significantly higher than those during the normal period.
et al., 2016. Ambient PM 2.5-bound polycyclic aromatic
Gas-PAHs were dominant by LMW-PAHs (2–3 rings), whereas
hydrocar-bons (PAHs) in Changhua County, central Taiwan:
HMW-PAHs (4–6 rings) were mainly associated with particles, Seasonal variation, source apportionment and cancer risk
indicating that carcinogenic PAHs were mainly found in the assessment. Environ. Pollut. 218, 372–382.
particle phase. PM1 played a major role in toxicity in PM2.5 , Chomanee, J., Tekasakul, S., Tekasakul, P., Furuuchi, M., 2018.
measured by BaP-TEQ concentrations, accounting for 68.7%– Effect of irradiation energy and residence time on
91.3%, whereas PM0.1 contributed to 10.5%–28.9% of the BaP- decomposition efficiency of polycyclic aromatic hydrocarbons
(PAHs) from rubber wood combustion emission using soft
TEQ in PM2.5 . This indicated that smaller particles, <1 μm,
X-rays. Chemosphere 210, 417–423.
were a more significant source of carcinogenic aerosols and Chomanee, J., Thongboon, K., Tekasakul, S., Furuuchi, M.,
caused more health detriments than larger particles. The total Dejchanchaiwong, R., Tekasakul, P., 2020. Physicochemical and
accumulated ILCRs for PM0.1 , PM1 and PM2.5 , during the haze toxicological characteristics of nanoparticles in aerosols in
scenario had more health effects than in the non-haze sce- southern Thailand during recent haze episodes in lower
nario, but they were still in the safety band. The haze affected Southeast Asia. J. Environ. Sci. 94, 72–80.
ChooChuay, C., Pongpiachan, S., Tipmanee, D., Deelaman, W.,
period in 2019 at the sampling location was fortunately not
Suttinun, O., Wang, Q., et al., 2020. Long-range transboundary
long. A stronger and longer period of haze could be severely
atmospheric transport of polycyclic aromatic hydrocarbons,
detrimental. The PAH diagnostic ratios and CMB analysis for carbonaceous compositions, and water-soluble ionic species
PM0.1 , PM1 and PM2.5 during partial haze and normal peri- in southern Thailand. Aerosol Air Qual. Res. 20, 1591–1606.
ods indicated mixed sources of petroleum combustion and Dejchanchaiwong, R., Tirawanichakul, Y., Tirawanichakul, S.,
biomass burning, whereas the major source was peatland fires Kumar, A., Tekasakul, P., 2017. Techno-economic assessment
during the strong haze period. The contribution from local of forced-convection rubber smoking room for rubber
cooperatives. Energy 137, 152–159.
biomass burning was significant in PM2.5 and PM1 during the
Dejchanchaiwong, R., Kumar, A., Tekasakul, P., 2019. Performance
normal period, whereas diesel exhaust completely dominated
and economic analysis of natural convection based rubber
PM0.1 . The identification of the transboundary source as peat- smoking room for rubber cooperatives in Thailand. Renew.
land fires in Sumatra Island, Indonesia, was supported by the Energy 132, 233–242.
air mass backward trajectories. Dejchanchaiwong, R., Tekasakul, P., Tekasakul, S., Phairuang, W.,
This study provides crucial information for policy makers Nim, N., Thongboon, K., et al., 2020. Impact of transport of fine
to set an achievable and reasonable goal for PM1 and PM0.1 and ultrafine particles from open biomass burning on air
quality during 2019 Bangkok haze episode. J. Environ. Sci. 97,
reduction. Comprehensive health risk assessment could give
149–161.
a better and clearer understanding of the toxicity of fine and Dejchanchaiwong, R., Tekasakul, P., 2021. Effects of coronavirus
ultrafine particles and hence lead to the enhancement of the induced city lockdown on PM2.5 and gaseous pollutant
quality of health in lower SEA. concentrations in Bangkok. Aerosol Air Qual. Res. 21, 200418.
Engling, G., He, J., Betha, R., Balasubramanian, R., 2014. Assessing
the regional impact of indonesian biomass burning emissions
Acknowledgements based on organic molecular tracers and chemical mass
balance modeling. Atmos. Chem. Phys. 14, 8043–8054.
This research was financially supported by Thailand Science Fang, B., Zhang, L., Zeng, H., Liu, J., Yang, Z., Wang, H., et al., 2020.
PM2.5 -bound polycyclic aromatic hydrocarbons: sources and
Research and Innovation (TSRI) and Electricity Generating Au-
health risk during non-heating and heating periods
thority of Thailand (EGAT) under grant number RDG60D0002.
(Tangshan, China). Int. J. Environ. Res. Public Health 17 (2), 483.
This work was also supported by the Interdisciplinary Grad- Fujii, Y., Iriana, W., Oda, W., Puriwigati, A., Tohno, S., Lestari, P.,
uate School of Energy Systems, Prince of Songkla University et al., 2014. Characteristics of carbonaceous aerosols emitted
via student scholarships under grant number IGS-Energy 1- from peatland fire in Riau, Sumatra, Indonesia. Atmos.
2018/09. Equipment support from the East Asia Nanoparticle Environ. 87, 164–169.
Monitoring Network (EA-NanoNet) is acknowledged. We are Furuuchi, M., Murase, T., Tsukawaki, S., Hang, P., Sieng, S.,
Hata, M., 2007. Characteristics of ambient particle-bound
also thankful to John Morris for his great English language
polycyclic aromatic hydrocarbons in the Angkor monument
editing. area of Cambodia. Aerosol Air Qual. Res. 7, 221–238.
Gao, Y., Yang, L.X., Chen, J.M., Li, Y.Y., Jiang, P., Zhang, J.M., et al.,
2018. Nitro and oxy-PAHs bounded in PM2.5 and PM1.0 under
Supplementary materials different weather conditions at Mount Tai in Eastern China:
Sources, long-distance transport, and cancer risk assessment.
Supplementary material associated with this article can be Sci. Total Environ. 622–623, 1400–1407.
found, in the online version, at doi:10.1016/j.jes.2021.11.005. Ho, A.F.W., Zheng, H., Earnest, A., Cheong, K.H., Pek, P.P., Seok, J.Y.,
et al., 2019. Time-stratified case crossover study of the
references association of outdoor ambient air pollution with the risk of
acute myocardial infarction in the context of seasonal
exposure to the southeast asian haze problem. J. Am. Heart
Assoc. 8, 1–10.
Adam, M.G., Tran, P.T.M., Bolan, N., Balasubramanian, R., 2020. Ho, K.F., Ho, S.S.H., Lee, S.C., Cheng, Y., Chow, J.C., Watson, J.G.,
Biomass burning-derived airborne particulate matter in et al., 2009. Emissions of gas- and particle-phase polycyclic
Southeast Asia: a critical review. J. Hazard. Mater., 124760.
266 journal of environmental sciences 124 (2023) 253–267
aromatic hydrocarbons (PAHs) in the Shing Mun Tunnel, Hong forest fires in Thailand on the carbonaceous components in
Kong. Atmos. Environ. 43, 6343–6351. size-fractionated particles. Environ. Pollut. 247, 238–247.
Hussar, E., Richards, S., Lin, Z.Q., Dixon, R.P., Johnson, K.A., 2012. Phairuang, W., Inerb, M., Furuuchi, M., Hata, M., Tekasakul, S.,
Human health risk assessment of 16 priority polycyclic Tekasakul, P., 2020. Size-fractionated carbonaceous aerosols
aromatic hydrocarbons in soils of chattanooga, tennessee, down to PM0.1 in southern Thailand: Local and long-range
USA. Water Air Soil Pollut. 223 (9), 5535–5548. transport effects. Environ. Pollut. 260, 114031.
Jaafar, S.A., Latif, M.T., Razak, I.S., Wahid, N.B., Khan, A., M, F., Phoungthong, K., Tekasakul, S., Tekasakul, P., Hata, M., 2013.
Srithawirat, T., 2018. Composition of carbohydrates, Emissions of particulate matter and associated polycyclic
surfactants, major elements and anions in PM2.5 during the aromatic hydrocarbons from agricultural diesel engine fueled
2013 Southeast Asia high pollution episode in Malaysia. with degummed, deacidified mixed crude palm oil blends. J.
Particuology 37, 119–126. Environ. Sci. 25 (4), 751–757.
Jamhari, A.A., Sahani, M., Latif, M.T., Chan, K.M., Tan, H.S., Paoin, K., Ueda, K., Vathesatogki, P., Ingviya, T., Buya, S.,
Khan, M.F., et al., 2014. Concentration and source Dejchanchaiwong, R., et al., 2022. Long-term air pollution
identification of polycyclic aromatic hydrocarbons (PAHs) in exposure and decreased kidney function: A longitudinal
PM10 of urban, industrial and semi-urban areas in Malaysia. cohort study in Bangkok Metropolitan Region, Thailand from
Atmos. Environ. 86, 16–27. 2002 to 2012. Chemosphere 287, 132117.
Jiang, Y., Status, Hu, X., Yves, U.J., Zhan, H., Wu, Y., 2014. Status, Ravindra, K., Sokhi, R., Grieken, R.V., 2008. Atmospheric polycyclic
source and health risk assessment of polycyclic aromatic aromatic hydrocarbons: Source attribution, emission factors
hydrocarbons in street dust of an industrial city, NW China. and regulation. Atmos. Environ. 42 (13), 2895–2921.
Ecotoxicol. Environ. Saf. 106, 11–18. Samsuddin, N.A.C., Khan, M.F., Maulud, K.N.A., Hamid, A.H.,
Jin, T., Han, M., Han, K., Fu, X., Xu, L., Xu, X., 2018. Health risk of Munna, F.T., Rahim, M.A.A., et al., 2018. Local and
ambient PM10-bound PAHs at bus stops in spring and autumn transboundary factors’ impacts on trace gases and aerosol
in Tianjin, China. Aerosol Air Qual. Res. 18, 1828–1838. during haze episode in 2015 El Niño in Malaysia. Sci. Total
Kongpran, J., Kliengchuay, W., Niampradit, S., Sahanavin, N., Environ. 630, 1502–1514.
Siriratruengsuk, W., Tantrakarnapa, K., 2021. The health risks Sresawasd, C., Chetiyanukornkul, T., Suriyawong, P., Tekasakul, S.,
of airborne polycyclic aromatic hydrocarbons (PAHs): upper Furuuchi, M., Hata, M., et al., 2021. Influence of meteorological
north Thailand. Geo Health 5, e2020GH000352. conditions and fire hotspots on PM0.1 in northern Thailand
Latif, M.T., Othman, M., Idris, N., Juneng, L., Abdullah, A.M., during strong haze episodes and carbonaceous aerosol
Hamzah, W.P., Jaafar, A.B., 2018. Impact of regional haze characterization. Aerosol Air Qual. Res. 21, 210069.
towards air quality in Malaysia: a review. Atmos. Environ. 177, Sulong, N.A., Latif, M.T., Sahani, M., Khan, M.F., Fadzil, M.F.,
28–44. Tahir, N.M., et al., 2019. Distribution, sources and potential
Lavigne, E., Lima, I., Hatzopoulou, M., Van Ryswyk, K., van health risks of polycyclic aromatic hydrocarbons (PAHs) in
Donkelaar, A., Martin, R. V., et al., 2020. Ambient ultrafine PM2.5 collected during different monsoon seasons and haze
particle concentrations and incidence of childhood cancers. episode in Kuala Lumpur. Chemosphere 219, 1–14.
Environ. Int. 145, 106135. Tang, N., Hattori, T., Taga, R., Igarashi, K., Yang, X., Tamura, K.,
Li, Y., Chen, Q., Zhao, H., Wang, L., Tao, R., 2015. Variations in et al., 2005. Polycyclic aromatic hydrocarbons and
PM10, PM2.5 and PM1.0 in an urban area of the Sichuan Basin nitropolycyclic aromatic hydrocarbons in urban air
and their relation to meteorological factors. Atmosphere 6 (1), particulates and their relationship to emission sources in the
150–163. Pan-Japan Sea Countries. Atmos. Environ. 39, 5817–5826.
Lu, H., Wang, S., Wu, Z., Yao, S., Han, J., Tang, X., Jiang, B., 2017. Tekasakul, P., Furuuchi, M., Tekasakul, S., Chomanee, J., Otani, Y.,
Variations of polycyclic aromatic hydrocarbons in ambient air 2008. Characteristics of PAHs in particulates in the
during haze and non-haze episodes in warm seasons in atmospheric environment of Hat Yai City, Thailand, and
Hangzhou, China. Environ. Sci. Pollut. Res. 24, 135–145. relationship with rubber-wood burning in rubber sheet
Lu, W., Yang, L.X., Chen, J.M., Wang, X.F., Li, H., Zhu, Y.H., et al., production. Aerosol Air Qual. Res. 8 (3), 265–278.
2016. Identification of concentrations and sources of U.S.EPA, 2004a. Protocol for Applying and Validating the CMB
PM2.5-bound PAHs in North China during haze episodes in Model for PM2.5 and VOC Report No. EPA-451/R-04-001
2013. Air Qual. Atmos. Health 9, 823–833. Prepared by U.S. Environmental Protection Agency, Research
Maitre, A., Petit, P., Marques, M., Hervé, C., Montlevier, S., Triangle Park, NC.
Persoons, R., et al., 2018. Exporisq-HAP database: 20 years of U.S.EPA, 2004b. EPA-CMB8.2 User’s Manual Report No.
monitoring French occupational exposure to polycyclic EPA-452/R-04-011 prepared by U.S. Environmental Protection
aromatic hydrocarbon mixtures and identification of exposure Agency, Research Triangle Park, NC.
determinants. Int. J. Hyg. Environ. Health 221 (2), 334–346. U.S.EPA, 2005. EPA-CMB8.2 Model Code. Available https:
Mikuška, P., Čapka, L., Večeřa, Z., 2018. Aerosol sampler for //www.epa.gov/scram/chemical- mass- balance- cmb- model
analysis of fine and ultrafine aerosols. Anal. Chim. Acta 1020, Accessed: August 20, 2021.
123–133. U.S.EPA, 2011. Exposure Factors Handbook Report No.
Nisbet, I.C.T., LaGoy, P., 1992. Toxic equivalency factors (TEFs) for EPA/600/R-09/052F. prepared by U.S. Environmental Protection
polycyclic aromatic hydrocarbons (PAHs). Regul. Toxicol. Agency, Research Triangle Park, NC.
Pharmacol. 16 (3), 290–300. Unwin, J., Cocker, J., Scobbie, E., Chambers, H., 2006. An
Earthdata, 2021. NRT VIIRS 375 m Active Fire product VNP14IMGT. assessment of occupational exposure to polycyclic aromatic
Available: https://earthdata.nasa.gov/firms. Accessed July 15, hydrocarbons in the UK. Ann. Occup. Hyg. 50 (4), 395–403.
2021. Urbancok, D., Payne, A.J.R., Webster, R.D., 2017. Regional transport,
PCD, 2021. Air quality standards in the atmosphere in Thailand. source apportionment and health impact of PM10 bound
Available: polycyclic aromatic hydrocarbons in Singapore’s atmosphere.
http://air4thai.pcd.go.th/webV2/download.php?grpIndex=1. Environ. Pollut. 229, 984–993.
Accessed: August 18, 2021. WHO, 1987. Air quality guidelines for Europe WHO Regional
Phairuang, W., Suwattiga, P., Chetiyanukornkul, T., Hongtieab, S., Publications, 23. European Series.
Limpaseni, W., Ikemori, F., Hata, M., Furuuchi, M., 2019. The Wiriya, W., Chantara, S., Sillapapiromsuk, S., Lin, N.H., 2016.
influence of the open burning of agricultural biomass and Emission Profiles of PM10-bound polycyclic aromatic
journal of environmental sciences 124 (2023) 253–267 267
hydrocarbons from biomass burning determined in chamber Zhang, Y., Yang, L., Gao, Y., Chen, J., Li, Y., Jiang, P., et al., 2019.
for assessment of air pollutants from open burning. Aerosol Comparative study of PAHs in PM1 and PM2.5 at a background
Air Qual. Res. 16 (11), 2716–2727. site in the North China plain. Aerosol Air Qual. Res. 19 (10),
Wiriya, W., Prapamontol, T., Chantara, S., 2013. PM10-bound 2281–2293.
polycyclic aromatic hydrocarbons in Chiang Mai (Thailand): Air Resources Laboratory, 2021. HYSPLIT model. Available: https:
Seasonal variations, source identification, health risk //ready.arl.noaa.gov/hypub-bin/trajtype.pl?runtype=archive.
assessment and their relationship to air-mass movement. Accessed: July 31, 2021.
Atmos. Res. 124, 109–122.