Science of the Total Environment 609 (2017) 682–693

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Science of the Total Environment

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

Review

Review on characteristics of PAHs in atmosphere, anthropogenic sources

and control technologies
Nguyen-Duy Dat, Moo Been Chang ⁎
Graduate Institute of Environmental Engineering, National Central University, Chungli 320, Taiwan

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Characteristics of ambient PAHs depend

on source and meteorological condi-
tions.
• Characteristics of PAHs emission vary
with burned material and combustion
condition.
• Synergistic effects of PAHs and fine par-
ticles on human health should be ad-
dressed.
• Studies on removal technologies and
operating parameters should be
strengthened.

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

Article history: Polycyclic aromatic hydrocarbons (PAHs) are a group of organic compounds composed of multiple aromatic
Received 28 April 2017 rings. PAHs are ubiquitous atmospheric pollutants which are well-recognized as carcinogenic, teratogenic and
Received in revised form 21 July 2017 genotoxic compounds. PAHs are released from incomplete combustion or pyrolysis of materials containing car-
Accepted 23 July 2017
bon and hydrogen, such as coal, oil, wood and petroleum products. Understanding the characteristics of PAHs in
Available online xxxx
atmosphere, source profiles and technologies available for controlling PAHs emission is essential to reduce the
Editor: D. Barcelo impacts of PAHs. This paper offers an overview on concentration and distribution of atmospheric PAHs, emission
factors and distribution of PAHs in different sources, and available control technologies. Characteristics of atmo-
Keywords: spheric PAHs vary with meteorological conditions and emission sources, while characteristics of PAHs emission
PAHs depend on burned material and combustion condition. Combination of some technologies may be necessary for
Characteristics effective removal of both low-ring and high-ring PAHs.
Ambient air © 2017 Elsevier B.V. All rights reserved.
Sources
Control technologies

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 683
2. Atmospheric PAH . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 684
2.1. Atmospheric PAH concentration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 684
2.2. Gas/particle distribution and partitioning of PAHs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 685

⁎ Corresponding author.
E-mail address: mbchang@ncuen.ncu.edu.tw (M.B. Chang).

http://dx.doi.org/10.1016/j.scitotenv.2017.07.204
0048-9697/© 2017 Elsevier B.V. All rights reserved.
 N.-D. Dat, M.B. Chang / Science of the Total Environment 609 (2017) 682–693 683

2.3. Particulate-bound PAHs. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 686

3. Characteristics of PAHs in source emission . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 687
3.1. Emission factor (EF) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 687
3.2. Distribution of PAHs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 689
4. Technologies for PAH removal . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 689
5. Conclusions and suggestions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 691
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 691
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 691

1. Introduction 1999). Significant anthropogenic sources include stationary combustion

Polycyclic aromatic hydrocarbons (PAHs) are a group of chemically
related compounds which are environmentally persistent with various
structures and varied toxicity (Nisbet and LaGoy, 1992). They are of con-
siderable concern primarily due to their ubiquitous presence in the en-
vironment and well-recognized carcinogenicity, teratogenicity and
genotoxicity (Yang et al., 2010a). PAHs are released into environment
from both natural and anthropogenic sources (Howsam and Jones,
1998). Volcano eruption and forest and prairie fire are considered as
major natural sources of atmospheric PAHs (Manoli and Samara,
sources and mobile sources. The most important sources of atmospheric
PAHs are incomplete combustion and pyrolysis of materials containing
carbon and hydrogen, such as coal, oil, wood and petroleum products
(Ravindra et al., 2008). PAHs are mostly formed from saturated hydro-
carbon under oxygen-deficient condition. Pyrosynthesis and pyrolysis
are two major mechanisms leading to PAH formation. The U.S. Environ-
mental Protection Agency (EPA) specified 16 PAHs as priority com-
pounds, with relevant information being summarized in Table 1.
A few review articles focusing on PAH sources, emission factors
and regulation (Ravindra et al., 2008), fate and concentration in

Table 1
Priority PAHs classified by USEPA and their primary information.

PAH compound Abbreviation No. of rings Vapor pressurea (Pa, 25 °C) TEFb Structure

Naphthalene NAP 2 11.14 0.001

Acenaphthylene ACY 3 3.87 0.001

Acenaphthene ACE 3 3.07 0.001

Fluorene FLU 3 1.66 0.001

−1
Phenanthrene PHE 3 1.06 × 10 0.001

Anthracene ANT 3 8.6 × 10−4 0.01

−4
Fluoranthene FLT 4 8.61 × 10 0.001

Pyrene PYR 4 5.0 × 10−5 0.001

Benzo[a]anthracene BaA 4 5.43 × 10−4 0.1

Chrysene CHR 4 4.0 × 10−6 0.01

Benzo[b]fluoranthene BbF 5 5.0 × 10−7 0.1

Benzo[k]fluoranthene BkF 5 5.2 × 10−8 0.1

Benzo[a]pyrene BaP 5 6.0 × 10−8 1

Dibenzo[ah]anthracene DahA 5 1.33 × 10−8 1

Indeno[123-cd]pyrene IcdP 6 1.27 × 10−7 0.01

Benzo[ghi]perylene BghiP 6 1.38 × 10−8 0.1

a: Vapor pressure: Mackay et al. (1997), Odabasi et al. (2006).

b: TEF refers to toxic equivalent factor, Nisbet and LaGoy (1992).
684 N.-D. Dat, M.B. Chang / Science of the Total Environment 609 (2017) 682–693

environment and human health effects (Kim et al., 2013), emission from
energy generation (Mastral and Callén, 2000), PAHs in Asia region
(Chang et al., 2006), source, environment impact, effect on human
health and remediation (Abdel-Shafy and Mansour, 2016) and PAH di-
agnostic ratios (Tobiszewski and Namiesnik, 2012) have been pub-
lished. However, the characteristics of each emission source, congener
distribution in gas/particle phase, especially, control technologies avail-
able for PAHs removal have not been discussed. In this work, the con-
centration, distribution, gas/particle partitioning of 16 priority PAHs in
ambient air and major PAH sources are summarized and discussed. Con-
trol technologies applied for PAHs removal of some industries are also
evaluated.
2. Atmospheric PAH
2.1. Atmospheric PAH concentration
Concentrations of PAHs measured in ambient air worldwide are
summarized in Table 2. Concentrations of PAHs in ambient air vary in
a wide range from lower than 50 pg m− 3 to higher than 1.7 μg m− 3
(up to 35.02 ng BaP-TEQ m−3), depending on where and when the sam-
ples were collected. In general, atmospheric PAH concentrations are
higher in industrial, urban or residential areas if compared with those
measured in remote or rural sites (Callen et al., 2011; Anastasopoulos
et al., 2012; Brown and Brown, 2012; Xia et al., 2013; Liu et al., 2014a;
Garrido et al., 2014). For instance, concentrations of atmospheric PAHs
in two urban sites of USA (Chicago and Cleveland) were greater than
those measured at other sites by 5 to 170 (average 20) times (Liu
et al., 2014a). Callen et al. (2011) indicated that particle-bound PAH
concentrations were 5 and 10 times higher in industrial and urban
areas, respectively, in comparison with those measured in rural areas.
Concentration of particle-associated PAHs in sugarcane-burning period
is 9.7 times higher than that in non-sugarcane burning period (Cristale
et al., 2012). Obviously, PAH concentration in atmosphere is strongly
dependent on sources of PAH nearby. Furthermore, ambient PAH con-
centration also depends on wind direction, weather event (non-haze
and haze or monsoon episodes (Tan et al., 2011; Mohanraj et al.,
2011). Significant correlation between population density and atmo-
spheric PAH concentration was observed by Hafner et al. (2005).
Wang et al. (2011) also indicate that total airborne PAH concentration
in Donghe was higher than that of Gubeikou due to 3 times more pop-
ulation and 8 times higher GDP in Donghe compared with Gubeiku.
In atmosphere, PAHs are found in both gas phase and particulate
phase in which the PAHs are associated with particles. In general, signif-
icantly higher gas-phase PAH concentrations compared with solid-
phase PAH concentrations are reported by various studies (Akyüz and
Çabuk, 2010; Yang et al., 2010b; Gregoris et al., 2014, Wu et al., 2014;
Lai et al., 2017). Van Drooge et al. (2010) indicated that particulate-
PAH accounts for 5% to 28% of total PAHs. It was observed that gas to
particulate (G/P) ratios of PAH vary in a relatively wide range, from ~2
(Liu et al., 2008) to N10 (Li et al., 2006).
In general, concentrations of PAH were reported greater in winter-
time compared to those measured in other seasons (Cincinelli et al.,
2007; Liu et al., 2008; Van Drooge et al., 2010; Wang et al., 2011;
Dvorská et al., 2012; Masih et al., 2012; Xia et al., 2013; Lv et al., 2016;
Tomaz et al., 2016; Wang et al., 2016b). Total PAH concentration was
about 5 times higher in winter than those measured in summer and au-
tumn as reported by Van Drooge et al. (2010). Liu et al. (2008) indicated
that PAH concentrations were 1.5 and 8 times higher in winter com-
pared to summer in gas and particulate phases, respectively. A higher
solid-phase PAH concentration in rainy season compared to dry season
was also observed by Hien et al. (2007) and sunshine duration was an
important meteorological parameter affecting seasonal variations of
PAHs in Ho Chi Minh City, Viet Nam. Overall, concentrations of all PAH
congeners were significantly higher in cold or rainy periods compared
to other seasons as a consequence of several reasons such as (Liu
et al., 2008; Kong et al., 2010; Masih et al., 2012; Lv et al., 2016;
Tomaz et al., 2016): (1) reduced photo-, thermo- and chemical-
oxidations in atmosphere due to reduced solar radiation during winter
and rainy seasons, (2) enhanced PAH emission due to domestic heating
demand (Birgul and Tasdemir, 2015) and lower combustion efficiency
of vehicle engines in winter (Arhami et al., 2010), (3) a thinner

Table 2
Total PAH concentrations reported worldwide.

Nation Concentration Type of area Note Dominant Time of sampling Reference

congeners

UK 0.029–0.13 Rural ng BaP-TEQ m−3 – 2008–2010 Brown and Brown,

0.12–2 Urban – 2012
0.25–1.4 Suburban –
US 1.4–2.4 ng m−3 – 4 major contributor PAHs – 2013 Liu et al., 2014a
Europe 0.033–1.5 ng m−3 –
Canada 10.2–83.7 ng m−3 Urban ∑16 PAHs (0.678–0.945 ng BaP-TEQ m −3
) – Summer, 2009 Anastasopoulos et al.,
8.31–52.1 ng m−3 Winter, 2009 2012
Europe and Atlantic 53–4443 pg m−3 Remote ∑16 PAHs (0.005–0.112 ng BaP-TEQ m−3) PHE, FLU 2001–2002 Van Drooge et al.,
Ocean background 2010
Europe 2.243 ± 1.772 ng Urban, background ∑15 PAHs PHE, FLU, FLT, 1994–2010 Garrido et al., 2014
m−3 PYR
Spain 2.71–366.9 ng Chemical and ∑18 PAHs PHE, NAP 2008 Ramirez et al., 2011
m−3 industrial
Saudi Arabia 0.13–515.76 ng Urban ∑16PAHs (Particle-phase only) PYR, FLT 2011–2012 Bian et al., 2016
m−3
North China Plain 19.7–89.1 ng m−3 Background ∑15 PAHs (0.061–35.02 ng BaP-TEQ m−3) PHE, FLO October 2007 to August Wang et al., 2011
89.8–1616.5 ng Rural 2008
m−3
131–979.2 ng Urban
m−3
Korea 78.8 ± 38.2 ng Urban ∑16 PAHs 2–3 ring Oct. 2014 Kim and Kim, 2015
m−3
Turkey 30–198 ng m−3 Urban ∑12 PAHs PHE, FLT 2008–2009 Birgul and Tasdemir,
2015
−3 −3
Gemany 0.4–121.4 ng m Residential ∑21 PAHs (2.6 ng BaP-TEQ m , PYR, FLT Winter (2005 and Bari et al., 2010
Particle-phase only) 2006)
−3
Taiwan 69.3–325 ng m Industrial ∑16 PAHs (0.180–0.811 ng BaP-TEQ m−3) NAP, PHE, FLU Spring and summer Lai et al., 2017
(2012)
 N.-D. Dat, M.B. Chang / Science of the Total Environment 609 (2017) 682–693
planetary boundary layer and frequent thermal inversions may trap
pollutants in the lower troposphere and prevent their dispersion, (4) in-
creasing PAH volatilization from particle to gas phase and better dilu-
tion and dispersion of atmospheric PAH in summer (Kong et al., 2010).
Higher wind speed could reduce PAH level by increasing dilution
and dispersion of air mass and a negative correlation between PAHs
and wind speed was observed (Tan et al., 2006; Sharma et al., 2007).
Masih et al. (2012) found that PAH concentrations decrease with the in-
crease of temperature, and wind speed. Elorduy et al., 2016 also indicat-
ed that wind speed, temperature, and atmospheric pressure are the
significant meteorological parameters affecting PAHs concentration.
On the other hand, relatively low correlation between PAH concentra-
tion and humidity was found. Hence, temperature and wind speed
might be the major meteorological factors affecting the concentration
of atmospheric PAHs.
The level of atmospheric PAHs in ambient air quality standard was
established in some countries, whereas, regulation regarding the emis-
sions of PAHs from stationary sources has not been established yet. As
the most carcinogenic compound among 16 parent PAHs, BaP has
been used as a reference to set up the regulation or guideline for the
presence of PAHs in the atmosphere (Garrido et al., 2014). Limit concen-
tration of PAHs in ambient air quality standard is expressed as nano
gram BaP toxic equivalent per cubic meter (ng BaP-TEQ m−3), calculat-
ed by the sum of the mass concentration of individual congeners multi-
plied by their TEF values. European Commission established a target
value of 1 ng BaP-TEQ m−3 for the annual mean presence of ambient
PAHs in 2005 (European Commission, 2005), and this value entered
into force on 31 Dec. 2012 (European Commission, Air Quality Stan-
dard). This limit is taken as the ambient air standard not only in coun-
tries belong to European Commission but also in India and China (Air
Quality Standard in India and Air Quality Standard in China, 2012).
China government also set up the limit of 2.5 ng BaP-TEQ m−3 for 24-
h average exposure (Air Quality Standard in China, 2012). France set
up a limit of 0.9 ng BaP-TEQ m−3 for annual exposure, however, this
limit applies to 41 parent PAHs and their derivatives (Atmospheric
Quality Standards and Criteria in France).
2.2. Gas/particle distribution and partitioning of PAHs
In general, light molecular weight (LMW) PAHs (2- to 3-ring) with
higher vapor pressures are dominant in gas phase and high molecular
weight (HMW) PAHs (5, 6-ring) with low vapor pressures are main
contributors in particle phase while medium molecular weight
(MMW) PAHs (4-ring) are distributed in both gas and particulate
phases (Fig. 1). Phase distribution of atmospheric PAHs depends on
the vapor pressure of the compound and the predominance of gas-
Fig. 1. PAH distributions in gas phase (G) and particulate phase (P) in different observations: (1) Li et al., 2006; (2) Liu et al., 2015; (3) Lai et al., 2017; (4) Wang et al., 2011; (5) Gregoris
et al., 2014.
685
phase PAHs compared to particulate phase was also observed in many
studies such as Li et al. (2006), Cincinelli et al. (2007), Van Drooge
et al. (2010), Ramirez et al. (2011), Hassan and Khoder,
2012Anastasopoulos et al. (2012), Masih et al. (2012), Birgul and
Tasdemir (2015) and Liu et al. (2015).
Fig. 1 compares the distributions of PAHs in gas phase and particu-
late phase in ambient air from 5 different dataset with different charac-
teristics. Five dataset are collected from various locations, including an
urban site in Guangzhou (Li et al., 2006), a tunnel in Shanghai (Liu
et al., 2015), background, urban, rural sites in China (Wang et al.,
2011), background sites in Venice (Gregoris et al., 2014) and industrial
regions in Kaohsiung (Lai et al., 2017), respectively. Three first authors
reported 16 priority PAHs while others just reported 15 PAHs (except
for NAP). Distributions of PAHs in gas phase of 5 reports are quite differ-
ent with the dominance of PHE, NAP, NAP, FL and PHE, PHE and FLT, re-
spectively. Contribution of PAH congeners in particle phase reported by
Li et al. (2006) and Wang et al. (2011) are similar, with the dominance
of HMW congeners, while the particulate phase of sample collected in
tunnel (Liu et al., 2015) and Venice (Gregoris et al., 2014) are dominated
by LMW PAHs (NAP) and MMW PAHs (FLT and PYR), respectively. The
proportions of HMW PAHs in particle phase of sample collected from in-
dustrial sites (Lai et al., 2017) are relatively high, however, the domi-
nant congener is NAP. Distribution in gas and particle phase depends
on local PAH emission source. Dominance of 2-ring and 3-ring PAHs in
tunnel ambient air may be attributed to the gasoline-powered medium
and light duty vehicles (Liu et al., 2015). This observation is consistent
with the dominance of LMW PAHs in the samples collected at regions
where vehicle is the most important source (Lee et al., 1995; Hanedar
et al., 2011; Oliveira et al., 2011; Hassan and Khoder, 2012; Lai et al.,
2017; Krugly et al., 2014; Souza and Corrêa, 2016; Cao et al., 2017).
Moreover, previous studies indicate that PHE is dominant in the sam-
ples collected with pyrogenic and coal-burning as major sources (Ma
et al., 2011; Huang et al., 2013; Liu et al., 2015). It indicates that distribu-
tion of PAH in gas and particulate phases may be different, depending
on emission source.
In term of TEQ distribution, generally, particulate phase dominates
due to the strong association of HMW-PAHs which are of high toxic
equivalent factors. Significantly high contribution of particle phase to
total TEQ concentration was shown in many studies such as Chen
et al., 2011 (up to 94%); Wang et al., 2011 (98%); Akyüz and Çabuk,
2010 (up to 86%). However, an opposite trend was observed for the am-
bient air samples collected in the summer time at industry sites (Lai
et al., 2017) and background site (Wang et al., 2011), which implies
that PAHs evaporate from particles and contribute more to gas-phase
toxicity in the high-temperature condition. Furthermore, low concen-
tration of TSP in summer time might be also a reason for low toxicity
686 N.-D. Dat, M.B. Chang / Science of the Total Environment 609 (2017) 682–693
contribution of particulate phase. Among LMW- and MMW-PAHs,
LMW-PAHs contribute more to total TEQ concentration due to the high-
ly dominant mass concentrations. On average, the MMW-PAHs contrib-
ute 3.5–11% of total TEQ concentration (Akyüz and Çabuk, 2010; Chen
et al., 2011; Wang et al., 2011; Lai et al., 2017). The contributions of
LMW-PAHs to total TEQ in background sites are higher than those in
rural villages and urban sites, which are observed in all 4 seasons by
Wang et al. (2011). The dominant contribution of LMW-PAHs was
also reported by Lai et al. (2017) for the samples collected at industrial
sites in the summer time. These results indicate that the distributions of
PAHs to TEQ concentration depend on meteorological conditions and
the gas/particle partitioning of PAHs.
The gas–particulate ratios of PAHs at background sites (~ 4) were
lower than those at urban sites (~10) in Eordea basin, western Greece
(Terzi and Samara, 2004), indicating the influences of long-range trans-
port at the background site. Atmospheric lifetimes of particle-associated
PAHs are much longer than those of the gas-phase PAHs (Vione et al.,
2004). However, phase partitioning of PAHs in ambient air depends
on various factors including property of the compounds, ambient tem-
perature, concentration and property of atmospheric suspended parti-
cles (Baek et al., 1991; Wu et al., 2014). The gas/particle partitioning
of PAHs in ambient air is a function of both ambient temperature and
PAH volatility in question (Kim et al., 2013). The temperature-
dependence of gas/particle partitioning, the regression between logKp
and temperature was performed firstly by Yamasaki et al. (1982):
logKp ¼ mð1=TÞ þ b ð1Þ

1996; Vione et al., 2004; Fang et al., 2006; Kong et al., 2010; Martellini
Kp ¼ Cp =TSP =Cg ð2Þ
where Kp (m3 μg−1) is the gas/particle partitioning coefficient defined
by Eq. (2) (Pankow, 1987), Cp and Cg are the particulate and gaseous
PAH concentrations (ng m−3), respectively, and TSP is the total
suspended particulate concentration (μg m−3), m and b are empirical
constants related to heat of the PAH phase change and the properties
of the individual PAH and the particulate matter. As defined in Eqs.
(1) and (2), a compound with larger Kp value reveals its higher tenden-
cy to sorb to particulate matter and the equilibrium shifts towards PAHs
in the particle phase when ambient temperature decreases. Therefore,
many authors report that higher logKp values are measured in the win-
ter than those in the summer and high molecular weight PAHs have
high logKp values (Terzi and Samara, 2004; Akyüz and Çabuk, 2010;
Yang et al., 2010b; Wang et al., 2011, Yu and Yu, 2012; Carreras et al.,
2013; Zhu et al., 2014). Furthermore, the decreases of logKp values
were observed for all of 16 PAHs when the sizes of particles were in-
creased from nuclei mode (0.04 μm) to coarse mode (4 μm) (Yu and
Yu, 2012), indicating that PAHs have higher tendency to associate
with fine particles rather than coarse particles.
0
logKp ¼ mr logP L þ br ð3Þ
Gas/particle partitioning coefficient provides the information re-
garding to the tendency of PAHs being associated with particles, howev-
er, Kp, by itself, does not indicate the nature of partitioning process, for
instance, whether the mechanism governing gas/particle partitioning
is adsorption onto particle surface, absorption into organic matter or
combination between adsorption and absorption (Pankow, 1994).
Pankow and Bidleman (1992) reported that the observed logKp vs
logP0L (a temperature-dependent value, is the log of the PAH sub-
cooled liquid vapor pressure) data are well correlated according to Eq.
(3) and the slope values are usually close to − 1, which is consistent
with adsorption mechanism. Pankow (1994) indicated that Eq. (3) is
also linearly correlated if absorption is dominant mechanism, which re-
veals that regardless of the importance of adsorbent or absorbent in gas/
particle partitioning, the plot of logKp vs logP0L will be correlated with
the slope close to − 1. Goss and Schwarzenbach (1998) reviewed on
slope mr for field data of gas/particle partitioning from literature and in-
dicated that under equilibrium conditions, the slope mr should be equal
to −1 if either adsorption or absorption mechanism explain gas/particle
PAH partitioning. The slope significantly steeper than −1 indicates ad-
sorption on a rather strong adsorbent and slope shallower than − 0.6
suggests absorption into an absorbent with high cohesive energy. On
the other hand, the slope in the range of −0.6 to −1 occurs when either
absorption or adsorption is involved. Nowadays, this result is used as
the most popular criterion to evaluate mechanism governing gas/parti-
cle partitioning of PAH, which implies that the slope higher than −1 in-
dicates the non-equilibrium conditions or sampling artifacts; the slope
close to −1 denotes that compounds underwent long-range transport
to sampling site, and the slope far from −1 reveals the contribution of
local sources (Akyüz and Çabuk, 2010). Generally, steeper slope (closer
to −1) was observed in the cold event while shallower slope was found
in the hot season (Lohmann et al., 2000; Yang et al., 2010b). The slope
closer to −1 was found in background and rural areas compared with
industrial and urban sites (Wang et al., 2011).
2.3. Particulate-bound PAHs
Particulate-phase PAHs have received more public concern than gas-
phase PAHs due to predominance of HMW PAHs which are more toxic
to human beings. Particulate-phase PAHs also affect the transport, de-
position and degradation of PAHs (Baek et al., 1991; Lv et al., 2016).
There are several studies focusing on particulate-bound PAHs to further
understand the human health effect and PM-bound PAHs (Allen et al.,
et al., 2012; Carreras et al., 2013; Zhu et al., 2014; Tomaz et al., 2016;
Bian et al., 2016).
In ambient air, PAH content in fine particles is significantly higher
than that in coarse particles (Manoli et al., 2002; Sanderson and
Farant, 2005; Fang et al., 2006; Oliveira et al., 2011; Sarti et al., 2017).
90% of the total particle-bound PAHs were found in PM2.5 (Kong et al.,
2010), 95–99% of particulate PAHs (13 PAHs) was found in fine particles
(b 3 μm) (Manoli et al., 2002). These observations are consistent with
the distribution of PAHs in different particle sizes of fresh emission
from residential coal combustion. N 69 ± 6% particulate-PAH is associat-
ed with PM2.5 (Shen et al., 2010), similar observation was also reported
by Wang et al. (2016a), who indicated that fraction of PAHs increased
significantly in PM1 (46.6–49.6%) and PM1–2.5 (30.0–33.0%) compared
with those of PM2.5–10 (19.6–22.4%). Similar results were also reported
by Shen et al. (2011), indicating that 54 ± 11% of particulate-bound
PAHs from indoor crop burning were found with the particle sizes be-
tween 0.7 and 2.1 μm and over 80 ± 6% were associated with PM2.5. Par-
ticles emitted from motorcycles (Yang et al., 2005a; Chien and Huang,
2010), and different stationary sources (Kong et al., 2010) also reveal
similar PAH-particle size distribution.
Seasonal variation of PAHs distribution in particles was reported by
Kong et al., 2010and Anastasopoulos et al., (2012). PAHs in PM2.5 had
a winter to summer ratio varying from 6.5 to 125.8 while PAHs in
PM2.5–10 had a ratio ranging from 1.7 to 37.6. (Kong et al., 2010). Similar
observation was reported by Allen et al. (1996) for PAH distribution in
summer time, furthermore, difference between PAH distribution in
urban and rural sites indicated that LMW- and HMW-PAHs are associat-
ed with both fine and coarse particles in rural samples, while LMW-
PAHs are distributed between fine and coarse particles and HMW-
PAHs are associated with fine particle in urban samples. The result indi-
cates that PAHs, especially HMW-PAHs, do not reach equilibrium in
urban aerosols.
The higher the molecular weight the stronger the association with
fine particles was reported for PAH emission from indoor crop residue
burning by Shen et al. (2011), who indicated that almost 60% of NAP
was associated with particles larger than 2.1 μm, while 81–90% of 4–6
ring PAHs from PYR to BghiP bound to particles smaller than 2.1 μm.
Similar trend of PAH distribution in ambient air is also reported by
 N.-D. Dat, M.B. Chang / Science of the Total Environment 609 (2017) 682–693
various authors (Allen et al., 1996; Kong et al., 2010; Yu and Yu, 2012;
Zhu et al., 2014; Lv et al., 2016; Zhai et al., 2016). Zhu et al. (2014)
shows that 3-ring PAHs associate with particles in both fine (1.0–1.8
μm) and coarse modes (3.2–5.6 μm), while 4–6 ring PAHs mainly asso-
ciate with particles in accumulation mode. The coarse fraction decreases
with the increase of PAH ring and relatively disappears for 5- and 6- ring
PAHs. As a consequence of high association of HMW PAHs which are of
high toxic potential in fine particles, BaP toxic equivalent (BaP-TEQ)
concentration of particulate PAH is dominated by fine particles. Zhu
et al. (2014) indicated that proportion of BaP-TEQ in fine particles (dp
b 1.8 μm) ranges from 45.8% (spring) to 79.3% (winter). This is in agree-
ment with the observation reported elsewhere (Baek et al., 1991;
Oliveira et al., 2011).
Although most PAHs are emitted from combustion sources in gas
phase or with fine particles, PAHs can associate with course particles
by either growth of fine combustion particles or volatilization from
fine particles followed by condensation/absorption/adsorption onto
coarse particles (Allen et al., 1996). If the growth of combustion-
generated fine particles is the dominant mechanism for PAH association
with coarse particles, the mixture of PAHs in fine and coarse particles
would be similar. However, this trend was not observed (Allen et al.,
1996; Lv et al., 2016), instead, the HMW-PAHs are associated more
with fine particles and LMW-PAHs are more related with coarse parti-
cles. A possible explanation for these results is that higher ring PAHs
having lower vapor pressures and Henry constants which require
much longer time to evaporate from fine particles and associate with
coarse particles, thus, would more likely associate with fine particles
(Allen et al., 1996; Zhu et al., 2014). On the other hand, lower ring
PAHs volatile more quickly from fine particles compared with non-
volatile PAHs sorbed onto coarse particles (Zhu et al., 2014). When
PAHs and particles are emitted into the air, they can be involved in the
particle aging process due to absorption or adsorption of PAHs on
preexisting particles via either self-nucleation or gas-particle portion-
ing, leading to an increase of PAH content in fine particles (Lv et al.,
2016). Currently, the mechanisms proposed for controlling PAH distri-
bution between different size particles include adsorption to nucleus
particles, adsorption and absorption to accumulation particles, and mul-
tilayer adsorption on coarse particles (Venkataraman et al., 1999). Lv
et al. (2016) have proven that multiple mechanisms govern the distri-
bution of PAHs among different size particles such as adsorption and ab-
sorption and adsorption plays a stronger role in distribution process of
higher ring PAHs than low ring PAHs due to the relatively lower volatil-
ity of higher ring PAHs. Wang et al. (2015) also indicated that two
mechanisms including absorption by organic matter and adsorption
on element carbon of soot particles occur simultaneously. Yu and Yu
(2012) and Wang et al. (2013) report that soot played an important
role in the partitioning of PAHs to aerosols and adsorption on elemental
carbon is more important than absorption by organic matter.
3. Characteristics of PAHs in source emission
3.1. Emission factor (EF)
Due to some similar characteristics of residential and biomass burn-
ing such as no air pollution control device equipped, no control of com-
bustion condition, and similar burned materials, these stationary PAH
sources are considered together. As a result of no air pollution control
device and no combustion condition control, PAH emission factors
from these sources are significantly higher than others (Table 3). Tradi-
tional materials for residential burning are firewood, biomass and coals
including anthracite, bituminous and honeycomb briquette. The yield of
total PAHs varies with a wide range, depending on burning conditions
and fuel types (Jenkins et al., 1996). Among these coals, the highest
PAH emission factor was found in bituminous coal combustion (Liu
et al., 2009; Shen et al., 2010; Shen et al., 2013). According to Singh
et al. (2013), combustion of sugar cane and dung cake also results in a
687
high PAH emission factor which is comparable with fuel wood. PAH
emission factors of residential burned materials are compared in
Fig. 2. Different emission factors of the same type of a material are also
presented, demonstrating that the PAH emission factor of a certain ma-
terial is not constant. For instance, as the same crop residue as wheat
straw was burned, emission factors are significantly different between
experiment stove (Zhang et al., 2011) and real cooking stove (Shen
et al., 2011). Shen et al. (2011) stated that emission factors of biomass
burned in stove are higher than those burned in chamber due to oxygen
deficiency and less turbulence in real cooking stove compared to cham-
ber. Furthermore, the higher temperature in stove may be an additional
reason for a higher PAH emission factor. Similar trends were observed
when rice and bean straw were burned within the temperature ranging
from 200 to 700 °C (Lu et al., 2009).
Devos et al. (2006) indicated that PAH emission factors of gasoline
vehicle were higher than those of diesel vehicle, however, Eiguren-
Fernandez and Miguel (2012) and Wei et al. (2015) reported that PAH
emission factor of diesel vehicle is higher than that of gasoline vehicle
(with some of exceptions). Several factors affect the PAH emission fac-
tor of vehicles including engine type, engine temperature, service age,
mileage, and maintenance (Cheruiyot et al., 2015). Elghawi et al.
(2010) stated that two possible mechanisms of PAH formation in the
gasoline engines are survival and pyrosynthesis. Souza and Corrêa
(2016) reported that the patterns of PAHs in diesel and exhaust emis-
sion are similar, furthermore, 95–99% of PAHs in diesel were destroyed,
indicating that the survival should be the main mechanism of PAH pres-
ence in exhaust gas. However, significant enrichment of FLU, PHE was
found in exhaust gases of non-catalyst and catalyst vehicles compared
with gasoline burned (Schauer et al., 2002). Comparison of diesel and
biodiesel fuels (Table 3) indicates that biodiesel has a lower PAH emis-
sion factor than diesel. The results can be explained by the absence of
PAHs contents in biodiesel and the improved combustion rendered by
oxygen content in biodiesel (Lin et al., 2006; He et al., 2010). Further-
more, emission of PAHs can be reduced by using n-butanol-diesel
blended with water (Lin et al., 2012) or gasoline blended with ethanol
(Cheruiyot et al., 2015).
Comparison between industrial processes and waste incinerators in-
dicates that except for magnesium metallurgy, emission factors of PAHs
from industrial processes are significantly higher than that of waste in-
cinerators. Survey of PAH emissions from various industrial processes
was conducted by Yang et al. (1998) and indicated that the highest
PAH emission factor was found in heavy oil plant, followed by coal-
fired power plant and basic oxygen furnace (Table 3). However, this
study was conducted about 20 years ago, when production techniques
were old, and single or simple technique was applied to remove pollut-
ants (compared to nowadays). PAHs emission factors of coal-related
processes are likely higher than those of others. Recently, Peng et al.
(2016) compared the emission factors of coal, MSW incineration and
coal/MSW co-combustion, and the results showed that emission factor
of MSW incineration was significantly higher than that of coal and
coal/MSW co-combustion. Similar result was also reported by Hsu
et al. (2016), indicating that the property of burned materials affects
PAH emission factor. Suksankraisorn et al. (2010) indicate that inciner-
ation of MSW with a high moisture content (60%) has a higher PAH
emission factor due to incomplete combustion compared to MSW
with a lower moisture content (35%). Lu et al. (2009) also indicated a
negative correlation between moisture content in straw and PAH for-
mation at 700 °C. In some case, emission factor of PAHs increases with
the increment of combustion temperature. Peng et al. (2016) indicated
that the yields of PAH increase with the elevation of temperature (from
500 to 900 °C) for coal combustion, MSW incineration and MSW/coal
co-combustion. Similar observation was reported by Lu et al. (2009)
who conducted the experiment of rice and bean straw combustion in
the temperature range of 200-700 °C.
Variations of emission factors with different combustion phases are
reported by some studies. Kaivosoja et al. (2012) indicated that
688 N.-D. Dat, M.B. Chang / Science of the Total Environment 609 (2017) 682–693

Table 3
PAH emission factors of various sources and relevant information.

Emission Concentration Emission factor Note APCD Ref.

sources

Residential/biomass burning
Anthracite 6.25 ± 1.16 mg kg−1 A commonly used stove in rural China; No APCD Shen et al., 2010
Bituminous 253 ± 170 mg kg−1 16 PAHs
Bituminous coal 880 mg kg−1 Daily-used coal stoves; 15 PAHs No APCD Liu et al., 2009
Anthracite coal 67.6 mg kg−1
Honeycomb 350.6 mg kg−1
briquette
Honeycomb 6.898 ± 7.893 mg kg−1 Typical coal stoves, 16 PAHs No APCD Chen et al., 2015
Briquette
Coal chunks 2.27 ± 1.607 mg kg−1
Rice straw 5.26 mg kg−1 Self-designed combustion stove; 16 No APCD Zhang et al., 2011
Corn straw 1.74 mg kg−1 PAHs
Wheat straw 1.36 mg kg−1
Fuel wood 21.1–66.7 mg kg−1 13 fuel wood, India; 16 PAHs No APCD Singh et al., 2013
Residual crop 13.9–49.4 mg kg−1 11 residual crops, India; 16 PAHs
Residual crop 27 (cotton stalk) – 142 mg 9 residual crops, China; cooking stove; No APCD Shen et al., 2011
kg−1 (wheat straw) 16 PAHs
Vehicle
Gasoline 35.69 μg m−3 Nanjing Iveco/A40 Original configuration of the vehicle's Wei et al., 2015
passenger car, 16 PAHs exhaust system, Velocity = 50 km h−1
Diesel 86.53 μg m−3 Chang'an/SC6372A minibus, 16 PAHs
Gasoline 10.4 (summer) – 19.4 Light-duty vehicles with spark ignition Real APCDs equipped for vehicles Eiguren-Fernandez
(winter) μg kg−1 (9 PAHs) and Miguel, 2012
Diesel 140 (summer) – 294 Heavy-duty diesels with compression
(winter) μg kg−1 ignition (9 PAHs)
Diesel 18.8–54.9 μg 62.7–731.3 μg kWh−1 EURO II diesel engine; 16 PAHs Real APCDs equipped for vehicles He et al., 2010
m−3
Biodiesel 13.2–43.2 μg 72.5–499.6 μg kWh−1
(B100) m−3
Diesel 82,229.11 ± 41,906.06 μg Light-duty diesel trucks; 16 PAHs Cao et al., 2017
km−1
52,867.43 ± 18,946.47 μg Medium-duty diesel trucks; 16 PAHs
km−1
93,837.35 ± 32,193.14 μg Heavy-duty diesel trucks; 16 PAHs
km−1
Industrial processes (16 PAHs)
Coal 179.57–3616.96 mg kg−1 China Bituminous coal No APCD Peng et al., 2016
combustion
Co-combustion 120.49–2402.17 mg kg−1 Bituminous coal + modified MSW
coal + MSW
Coal-fired 1130 ng Nm−3 1.56 μg kg −1
Indonesian and Australia coals SCR + ESP + FGD Hsu et al., 2016
power plant
Coal-fired 8.84–22.58 China bituminous coal ESP (+ WFGD) Wang et al., 2015
power plant μg Nm−3
Magnesium metallurgy Nie et al., 2014
Oxidation stage 4.1 ± 2,1 μg 145 μg ton−1 Coal and dolomite ore ESP (+BF)
Nm−3
Reduction 5.7 ± 1.5 μg 21 μg ton−1 BF
stage Nm−3
Blast furnace 75.6 μg kg−1 Coke + liquid steel + sinter Bag house Yang et al., 1998
Basic oxygen 512.9 μg kg−1 Liquid steel Bag house
furnace
Coke oven 232.7 μg kg−1 Coal Bag house
Electric arc 160.2 μg kg−1 Waste steel + heavy oil + charcoal Bag house
furnace
Heavy oil plant 3507 μg kg−1 Fuel oil No APCD
Power plant 560.2 μg kg−1 Bituminous ESP
Cement plant 124.8 μg kg−1 Cement raw material ESP
174 μg kg−1 Kiln feed ESP
8.97–15.31 μg Petroleum coke + solid waste Cyclone + BF Conesa et al., 2016
Nm−3
Coke plant 10.98–146.98 Coal BF Mu et al., 2014
μg Nm−3
45.776–414.874 93.173–346.132 μg kg−1 Coal BF Mu et al., 2013
μg Nm−3
Waste incineration (16 PAHs)
MSWI 111.28–10,047.22 μg kg−1 Modified MSW No APCD Peng et al., 2016
MWI 268 ng Nm−3 8.05 μg kg−1 Municipal solid waste SDA + ACI + BF Hsu et al., 2016
IWI 7.46 μg Nm−3 3.64 μg kg−1 Sludge of WWTP, refuse derived fuel, ESP + SDS + BF + WS Caneghem and
automotive shredder residue Vandecasteele, 2014
SSI 1.153–189.449 Sewage sludge or SS + MSW SDA (MC) + ESP (BF) + WS Park et al., 2009
μg m−3

Abbreviation: APCD-air pollution control device, SCR-selective catalytic reduction, ESP-electrostatic precipitation, FGD-fuel gas desulfurization, WFDS- wet fuel gas desulfurization, SDA-
semidry absorber, ACI-activated carbon injection, BF-bag filter, SDS- semidry scrubber, WS- wet scrubber, MSW- municipal solid waste incinerator, MWI- municipal waste incinerator,
IWI- industrial waste incinerator, WWTP-wastewater treatment plant, SSI- sewage sludge incinerator.
 N.-D. Dat, M.B. Chang / Science of the Total Environment 609 (2017) 682–693
among three phases of residential wood combustion including ignition,
pyrolysis, and burnout, concentration of PAHs in pyrolysis phase was
the highest (69 mg Nm−3) due to insufficient air supply or poor mixing
condition. On the other hand, the emission factors of PAHs during igni-
tion phase and burnout phase are 4.3 and 1.9 mg Nm−3, respectively.
Shen et al. (2011) found that emission factors of both gas-phase and
particulate-phase PAHs in flaming phase were higher than that of smol-
dering phase when 9 commonly used crop residues were test for deter-
mining PAH emission factors. Emission factors of total PAHs in the
flaming and smoldering phases were 99 ± 60 and 58 ± 32 mg kg−1, re-
spectively. Jenkins et al. (1996) indicated that PAH emission factor de-
creases with the increase of combustion efficiency, furthermore, weak
flaming and smoldering contribute an additional 70% to the total PAH
load from Ponderosa pine.
PAH emission depends on various factors such as type of fuel, com-
bustion conditions including resident time, temperature, turbulence,
moisture content, kind of combustor and type of air pollution control
devices equipped.
3.2. Distribution of PAHs
Distributions of PAH congeners in exhaust gas emitted from various
combustion processes are presented in Fig. 3. It indicates that heavy
molecule weight PAH (DahA) predominates in emission from biomass
burning, while light molecule weight and medium molecule weight
PAHs (NAP and PHE) are dominant congeners in emission of vehicle en-
gine, waste incinerator, coke plant and steel iron plant. Profile of PAHs
emission from various industries in Taiwan as investigated by Yang
et al. (1998) also indicated that LMW PAHs dominate, with average con-
tribution of 75.9%, and NAP is the most abundant congener. Khalili et al.
(1995) also evaluated PAH profile of major PAH sources in Chicago and
indicated that 2- and 3-ring PAHs accounted for 98, 76, 92, 73 and 80% of
total 20 PAHs measured for coke ovens, diesel engines, highway tunnels,
gasoline engines and wood combustion samples, respectively. Similar
trends were also reported by Hsu et al. (2016); Park et al. (2009);
Caneghem and Vandecasteele (2014), Zhou et al. (2005) and Conesa
et al. (2016) for PAH emissions from coal combustion, MSW incinera-
tion, sewage sludge incineration and cement plant.
PAH congener distributions between gas phase and particle phase
emitted from some burning processes are summarized and compared
in Fig. 4. Generally, among all kinds of burning material, proportion of
light PAHs in gas phase and contribution of heavy PAHs in particulate
phase are relatively high. However, distribution of PAH congeners in
gas phase and particle phase depends on emission characteristics. For
Fig. 2. Emission factors of PAHs from various biomass and residential burned materials (a, b, c, d represent ref. Shen et al., 2013; Zhang et al., 2011; Singh et al., 2013 and Shen et al., 2011).
689
instance, DahA is a strongly dominant congener of biomass burning
emission, therefore, it is the main contributor in both gas and particle
phases (see Fig. 4). On the other hand, NAP is dominant in gas phase,
and heavier PAH (PHE) is dominant in particle phase of vehicle (diesel
and biodiesel) emission (Yang et al., 2005b; He et al., 2010).
Distributions of PAH in gas phase and particle phase vary case by
case, Zhang et al. (2011) indicated that HMW (DahA) is dominant in
both gas and solid phases (about 50%) when crop residues (rice, corn
and wheat) are burned in a self-designed stove. However, according
to Shen et al. (2011), congener profiles of PAH emissions from 9 residual
crops (rice, wheat, corn, soybean, peanut, cotton, sesame, horse bean,
and rape residue) show that 2–3 ring PAHs (from NAP to ANT) are
main contributors, accounting for about 78% of total PAH emission.
NAP is the most contributor of gas-phase PAH (76 ± 5%), followed by
ACY (15 ± 4%). Particulate-bound PAHs include PHE (20 ± 12%), FLT
(11 ± 7%), FLU (11 ± 7%), and PYR (10 ± 7%). The results indicate
that even for the same burned material, PAH emission profiles might
be significantly different depending on combustion conditions.
Distributions of PAH congener vary with different operating temper-
atures. Peng et al. (2016) indicated that distributions of PAH congeners
varied with temperatures and the materials burned. For coal combus-
tion, 3-ring PAHs were dominant at all temperatures examined, howev-
er, the congeners which dominated at a specific temperature were
different. For municipal solid waste incineration, 3-ring PAHs were
main contributors (42.75%–68.17%) at temperatures ranging from 500
°C to 800 °C and 4-ring PAHs were dominant at 900 °C. For MSW/coal
co-combustion, ANT, PHE and NAP were dominant PAHs at the temper-
ature range of 500 °C–800 °C, while at 900 °C, the most abundant spe-
cies was PHE, followed by PYR and FLU.
NAP is the main contributor in both raw gas and stack gas of coal-
fired power plant and MWI (Hsu et al., 2016). Considering the PAH dis-
tribution between inlet and outlet of APCDs, a similar congener distribu-
tion was observed in coal-fired power plant with the major contributors
of NAP, PHE, FLT and PYR.
4. Technologies for PAH removal
Although many studies on the presence of PAH in environment and
emission characteristics have been published, studies on techniques for
PAH removal are rather limited. Liu et al. (2002) reported that a conven-
tional APCD consisting of spray dryer coupled with a fabric filter can
only remove 40% of PAHs. Zhou et al. (2005) conducted the experiment
using in-duct activated carbon injection (ACI) to remove PAHs in flue
gas emitted from MSW incinerator. Results showed that ACI could
690 N.-D. Dat, M.B. Chang / Science of the Total Environment 609 (2017) 682–693

Fig. 3. Congener distributions of PAHs in exhaust gases of some combustion processes [(1) Zhang et al., 2011; (2) Li et al., 2016; (3) Caneghem and Vandecasteele, 2014; (4) Chen et al.,
2013; (5) Mu et al., 2014; (6) Yang et al., 2002; (7) He et al., 2010; (8) Wei et al., 2015].

remove PAHs with the efficiencies ranging from 76% to 91% for total
PAHs as AC concentration was controlled at 1–2 g Nm−3. The results
also indicated that higher ring-PAHs were removed more effectively,
for instance, 6-ring PAHs were removed with 100% at all AC feed rates.
The flue gas after treatment was dominated by 2-ring PAHs while 6-
ring PAHs were not detected. This may be attributed to the fact that
the HMW-PAHs have high boiling points and low vapor pressures,
which usually exist in the form of solid phase at low temperatures and
are easy to deposit or adsorb on fly ash and AC through nucleation, con-
densation and adsorption. The PAH removal efficiency of activated car-
bon filter (ACF) is reduced by the presence of competitively adsorbed
compounds such as SO2 (Liu et al., 2014b). In order to improve the
PAH removal efficiency of ACF, metal catalysts (Pt, Pd, Fe, Co, Ni, and
Cu) supported on ACFs were investigated (Lin et al., 2011; Tseng et al.,
2011). Pt was the most effective metal for reduction of PAHs and the
ACFs-supported metal catalyst were effective in the removal of HMW-
PAHs (Lin et al., 2011). The removal efficiencies of PAHs achieved with
AC-supported Fe, Co, Ni and Cu catalysts were 62%, 94%, 23%, and 55%,
respectively and 3-ring PAHs were removed more effectively (Tseng
et al., 2011). Liljelind et al. (2001) used titanium dioxide/vanadium
pentoxide as catalyst for PAHs and other POPs removal from solid
waste incinerator flue gas. The removal efficiency increases from 75%
to 98% as the temperature is increased from 100 °C to 230 °C. Both
adsorption and destruction are major mechanisms for PAHs removal
at 100 °C, however, PAHs are removed mainly by destruction at 150
and 230 °C.
Hsu et al. (2016) compared the characteristics of PAH emission from
coal-fired power plant and MSW incinerator equipped with different
APCDs (SCR + ESP + FGD and SDA + ACI + BF → SDA + catalyst filter,
respectively). The results showed that FGD is effective for PAH removal
and the removal efficiency achieved with catalytic filter (CF) increased
as operating temperature is increased. Efficiencies achieved with ACI
+ BF and CF are higher for higher ring PAHs, which are of higher BaP
TEF. Efficiency of CF was higher than that of ACI + BF for 2–3 ring
PAHs. Higher PAH content in BF dust compared to that of CF is attributed
to the different PAH removal mechanisms. ACI + BF just transfers PAHs
into fly ash while CF combines two mechanisms including effective de-
struction of gas-phase PAHs and filtration of particulate-phase PAHs.
Wang et al. (2015) indicated that WFGD was more effective in the
removal of PAHs compared to ESP in coal-fired power plant. 5 and 6-
ring PAHs were removed effectively at a coal-fired boiler equipped
with WFGD due to the adsorption with gypsum. Li et al. (2016) reported
that removal efficiency of WFGD was 17% while that of WESP was 83.5%.
The result also showed that 5 and 6-ring PAHs were removed more ef-
fectively than others in WFGD, which is consistent with the observation
reported by Wang et al. (2015). Furthermore, the removal efficiency of

Fig. 4. Congener distribution of PAHs in gas phase (G) and particulate phase (P) (Zhang et al., 2011; Li et al., 2016; He et al., 2010).
 N.-D. Dat, M.B. Chang / Science of the Total Environment 609 (2017) 682–693
PAHs achieved with WESP (83.5%) was significantly higher than that
achieved with ESP as reported by Hsu et al. (2016), especially, efficiency
of WESP for NAP removal in gas phase was 99%, which was higher than
that of ESP for removal of total NAP (30%). The combination of low tem-
perature and the presence of water in WESP might facilitate PAH re-
moval. This assumption is consistent with the higher water solubility
of NAP compared with other PAH congeners and NAP was observed as
dominant congener in water-phase of wet scrubber effluent (Chen
et al., 2007).
A remarkable point should be noted is the formation of PAHs in SCR
system under high-temperature and high particulate matter conditions
(Hsu et al., 2016). In this case, SCR is effective for NOx removal, but pro-
motes PAHs formation. It suggests that PM needs to be removed before
SCR system to reduce PAHs formation.
5. Conclusions and suggestions
Concentration and distribution of PAHs in atmosphere vary widely
and depend on various factors including source and meteorological con-
ditions. High level of PAHs is observed in urban areas or high population
regions in wintertime. Generally, concentration of ambient gas-phase
PAHs is significantly higher than that of particle phase PAHs. LMW-
PAHs dominate in gas phase, while MMW-PAHs are associated with
both gas and particulate phases and HMW-PAHs are mainly distributed
in particulate phase. Particulate-bound PAHs have received more public
concern due to the dominance of HMW PAHs which are of high toxic
congeners in particulate phase. The results of size-particle distributions
of PAHs indicate that low-ring PAHs are associated more with coarse
particles while high-ring PAHs dominate in fine particles (PM2.5). The
synergistic effect of high toxic PAHs associated with fine particle and
high impact of fine particle to human health should be addressed.
Emission characteristics of PAHs depend on many factors such as
burned material, type of combustor and combustion conditions (tem-
perature, residence time, moisture content, and oxygen supply). Resi-
dential combustion and biomass burning are important PAH sources
due to similar characteristics such as wide application, noncontinuous
operation, no air pollution control device equipped and no operating
condition control. Coal and biomass are the popular materials for resi-
dential and biomass burning. Comparison of the EFs between coals
and biomass combustion, EFs of coal combustion are significantly higher
than those of biomass burning, and bituminous coal is likely with the
highest PAH emission. Biodiesel has a lower EF than that of diesel due
to the absence of PAHs in biodiesel, which suggests that biodiesel
could be used as alternative fuel to reduce PAH emission. The emission
factor of PAHs also depends on kinds of stove burning, normally, com-
bustor with sufficient oxygen supply and turbulent condition has a
lower EF of PAHs. Positive correlation between temperature and EF is
observed, suggesting that combustion at low temperatures can restrict
the formation of PAHs. The moisture content is also an important pa-
rameter affecting EF. High moisture content material is reported to re-
lease less PAHs than low moisture content material by some authors
due to lower combustion temperature. However, some reports show
that moisture content can promote the formation of PAHs due to incom-
plete combustion. The contradictory findings need to be clarified.
Available data of EFs for industrial processes are still scare. More
studies on PAH emission characteristics are needed to figure out the
whole picture of PAHs emission. In term of the EFs of industrial process-
es and waste incineration, available data generally indicates that indus-
trial processes have higher EFs compared to waste incineration. PAH
distributions in sources, generally, are similar to the distribution of
PAH in ambient air. NAP and other LMW PAHs are commonly dominant
congeners in vehicle emission, industrial and incinerator stack gas. Dis-
tributions of PAHs in residential and biomass burning depend on char-
acteristics of combustion.
ACI is effective for PAH removal with a high removal efficiency for
high-ring PAHs. Catalytic filter also effectively removes PAHs and the
691
efficiency increases with increasing temperature. Higher ring PAHs are
removed with higher efficiencies by both ACI and CF. However, low-
ring PAH removal efficiency achieved with CF is higher than that of
ACI. WFGD has an obvious cobenefit of PAH abatement, especially for
HMW-PAHs due to the adsorption of gypsum. WESP is more effective
than ESP for PAH removal, especially, for NAP. High water solubility of
NAP at low temperatures in WESP may be the reason for its high remov-
al efficiency of NAP in WESP. In order to remove both low-ring and high-
ring PAHs effectively, the combination between some technologies is
necessary. Studies on the control technologies and the effect of relevant
operating parameters on PAH removal are still limited. More research
and appropriate regulation are deemed necessary for effective reduc-
tion of PAH emission.
Acknowledgements
The authors gratefully acknowledge the financial supports provided
by the Taiwan EPA (MOST-105-EPA-F-005-003) and the Ministry of Sci-
ence and Technology (MOST-105-2622-8-009-007-TE4).
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