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Simultaneous removal of sulfur dioxide and polycyclic

aromatic hydrocarbons from incineration flue gas using
activated carbon fibers
a a a
Zhen-Shu Liu , Wen-Kai Li & Ming-Jui Hung
a
Department of Safety, Health and Environmental Engineering, Ming Chi University of
Technology, New Taipei City, Taiwan, Republic of China
Published online: 13 Aug 2014.

To cite this article: Zhen-Shu Liu, Wen-Kai Li & Ming-Jui Hung (2014) Simultaneous removal of sulfur dioxide and polycyclic
aromatic hydrocarbons from incineration flue gas using activated carbon fibers, Journal of the Air & Waste Management
Association, 64:9, 1038-1044, DOI: 10.1080/10962247.2014.922519

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 TECHNICAL PAPER

Simultaneous removal of sulfur dioxide and polycyclic aromatic

hydrocarbons from incineration flue gas using activated carbon
fibers
Zhen-Shu Liu,⁄ Wen-Kai Li, and Ming-Jui Hung
Department of Safety, Health and Environmental Engineering, Ming Chi University of Technology, New Taipei City, Taiwan, Republic of China
⁄Please address correspondence to: Zhen-Shu Liu, Department of Safety, Health and Environmental Engineering, Ming Chi University of
Technology, Taishan District, New Taipei City 24301, Taiwan, Republic of China; e-mail: zsliu@mail.mcut.edu.tw
Downloaded by [Northeastern University] at 14:38 25 November 2014

Incineration flue gas contains polycyclic aromatic hydrocarbons (PAHs) and sulfur dioxide (SO2). The effects of SO2
concentration (0, 350, 750, and 1000 ppm), reaction temperature (160, 200, and 280
C), and the type of activated carbon fibers
(ACFs) on the removal of SO2 and PAHs by ACFs were examined in this study. A fluidized bed incinerator was used to simulate
practical incineration flue gas. It was found that the presence of SO2 in the incineration flue gas could drastically decrease removal of
PAHs because of competitive adsorption. The effect of rise in the reaction temperature from 160 to 280
C on removal of PAHs was
greater than that on SO2 removal at an SO2 concentration of 750 ppm. Among the three ACFs studied, ACF-B, with the highest
microporous volume, highest O content, and the tightest structure, was the best adsorbent for removing SO2 and PAHs when these
gases coexisted in the incineration flue gas.

Implications: Simultaneous adsorption of sulfur dioxide (SO2) and polycyclic aromatic hydrocarbons (PAHs) emitted from
incineration flue gas onto activated carbon fibers (ACFs) meant to devise a new technique showed that the presence of SO2 in the
incineration flue gas leads to a drastic decrease in removal of PAHs because of competitive adsorption. Reaction temperature had a
greater influence on PAHs removal than on SO2 removal. ACF-B, with the highest microporous volume, highest O content, and
tightest structure among the three studied ACFs, was found to be the best adsorbent for removing SO2 and PAHs.

Introduction
Incineration is the main technique for treating municipal solid
waste in Taiwan. Some pollutants, including organic com-
pounds, sulfur dioxide (SO2), heavy metals, and fly ash, may
be emitted during incineration. To meet the stringent emission
standards for various contaminants in Taiwan, a spray dryer
integrated with a bag filter is used conventionally as an air
pollution control device (APCD) for incinerators, and powdered
activated carbon is injected into flue gas before it enters the bag
filter in order to remove the organic compounds. However, the
spray dryer suffers from some disadvantages, such as blockage
of the spray nozzle and production of sludge. Therefore, it is
important to devise a new technique to replace the conventional
APCD for incinerators.
Adsorption techniques are widely used to remove organic
compounds from industrial waste gas streams, and powdered
activated carbon, activated carbon fibers (ACFs), aluminum
oxide, silica gel, and zeolite are commonly used adsorbents.
Among these adsorbents, ACFs offer many advantages, includ-
ing higher adsorption and desorption rates, much higher surface
areas, a uniform micropore structure, and a lower pressure drop
(Fuertes et al., 2003; Huang et al., 2003; Lillo-Ródenas et al.,
2005; Muñiz et al., 2000; Park and Kim, 2001; Yang et al., 2011).
The use of ACFs for removing organic compounds from waste
gas streams has been extensively studied, indicating that the
removal efficiencies of organic compounds are affected by the
specific surface area, pore size distribution, pore volume, and
surface functional groups of the ACFs and by vapor pressure,
molecular size, and molecular weight of organic compounds
(Das et al., 2004; Gaur et al., 2006; Lin et al., 2013; Liu, 2006;
Liu et al., 2012; Mangun et al., 2001; Yi et al., 2009).
However, most species of the organic compounds explored in
previous studies are volatile organic compounds (VOCs), such as
benzene, toluene, and xylene (Das et al., 2004; Gaur et al., 2006;
Huang et al., 2003; Lin et al., 2013; Liu et al., 2012; Yi et al.,
2009). The 16 species of polycyclic aromatic hydrocarbons
(PAHs) listed by the U.S. Environmental Protection Agency
(EPA) as priority pollutants are rarely discussed in research of
ACFs (Liu, 2006). In this study, a fluidized bed incinerator was
used to simulate practical incineration flue gas.
Incineration flue gas contains PAHs and SO2. The presence of
SO2 in the incineration flue gas could affect the removal effi-
ciency and adsorption capacity of PAHs. Liu (2006) previously
determined that the removal efficiency of PAHs from incinera-
tion flue gas using ACFs exceeded 90%. Previous research has

1038
Journal of the Air & Waste Management Association, 64(9):1038–1044, 2014. Copyright © 2014 A&WMA. ISSN: 1096-2247 print
DOI: 10.1080/10962247.2014.922519 Submitted February 10, 2014; final version submitted April 22, 2014; accepted May 2, 2014.
 Liu et al. / Journal of the Air & Waste Management Association 64 (2014) 1038–1044 1039

shown that SO2 could be effectively removed by ACFs (Daley

et al., 1997; Ling et al., 1999; Liu, 2008). For example, Liu et al.
(2012) investigated the simultaneous removal of toluene and
SO2, and reported that SO2 inhibited the adsorption of toluene
on ACFs and the removal of toluene decreased with an increase
in the concentration of SO2. In this study, the simultaneous
removal of PAHs and SO2 from incineration flue gas and the
effect of SO2 on the removal of PAHs were examined at different
SO2 concentrations (0, 350, 750, and 1000 ppm), reaction tem-
peratures (160, 200, and 280
C), and for three types of ACFs.
Three adsorption temperatures, 160, 200, and 280
C, were
investigated because the temperature of flue gas in the APCD
is 200
C (Chi et al., 2006).

Experimental
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Experimental procedure
The three commercial ACFs used in this experiment were
provided by Taiwan Carbon Technology Co., Ltd., in Taiwan.
Polyacrylonitrile (PAN) was used as a precursor in the produc-
tion of these three ACFs. The thicknesses of ACF-A, ACF-B,
and ACF-C were 0.4, 1.2, and 0.4 mm, respectively. The densi-
ties of ACF-A, ACF-B, and ACF-C were 0.22, 0.07, and 0.29
gcm3, respectively. The ACFs were cleaned using deionized
water and then dried in an oven at 105
C for 24 hr before the
experiment was conducted. Thereafter, they were loaded into the
ACF adsorber. The height and inner diameter of the ACF adsor-
ber were 150 and 80 mm, respectively.
The laboratory-scale fluidized bed incinerator integrated with
an ACF adsorber used in this study is shown in Figure 1. The
combustion chamber was heated to the desired temperature,
800
C, by electrical heaters, and air entered the incinerator at
a flow rate of 60 Lmin1. When the temperature reached a
steady state, polypropylene (PP) granules and sulfur enclosed
in a small polyethylene (PE) bag was thrown into the incinerator
at the rate of one sample per 15 sec to simulate the flue gas.
Subsequently, the ACF adsorber was turned on and sampling was
initiated as described in the next paragraph. Detailed
Figure 1. Experimental system of fluidized-bed incinerator and activated carbon
fibers (ACFs) adsorber: (1) air compressor; (2) flowmeter; (3) combustion
chamber; (4) electrical heater; (5) thermal feedback controller; (6)
thermocouple; (7) feeder; (8) ACF adsorber; (9) sampling; (10) induced fan.
compositions of feedstock and operating parameters can be
seen in Table 1.
Sampling and analytical methods
To estimate the removal efficiency of PAHs and SO2, the flue
gas was sampled before entering and after exiting the ACF
adsorber. The sampling time periods for SO2 after and before
the passage of the flue gas through the ACF adsorber were 2–5
and 6–9 min, respectively. A flue gas analyzer (model 2800P;
IMR Environmental Equipment Inc., Florida, USA) was used to
determine the concentration of SO2. Before the experiments, the
analyzer was calibrated with standard gases. The accuracy and
resolution of the SO2 analyzer were 5% and 1 ppm, respectively.
The concentration range for the SO2 monitor was 0–4000 ppm
(Liu, 2008).

Table 1. Composition of feedstocks and operating conditions

Composition of Artificial Feedstocks

(g/sample)

Test Polypropylene Sulfur PE Bag ACF Type SO2 Concentration (ppm) Adsorption Temperature (
C)
Run 1 — ACF-A 0 200
Run 2 0.02 ACF-A 350 200
Run 3 0.03 ACF-A 750 200
Run 4 0.04 ACF-A 1000 200
Run 5 0.60 0.03 0.22 ACF-A 750 280
Run 6 0.03 ACF-A 750 160
Run 7 0.03 ACF-B 750 200
Run 8 0.03 ACF-C 750 200
Notes: PE ¼ polyethylene; ACFs ¼ activated carbon fibers.
 1040 Liu et al. / Journal of the Air & Waste Management Association 64 (2014) 1038–1044

extracted using dichloromethane over 20 hr through the Soxhlet

extraction process. The extraction solution was concentrated to 1
mL using a K-D evaporator concentrator (Chenghong Co.,
Kaohsiung, Taiwan), and these samples were analyzed using a
gas chromatograph with a flame ionization detector (Shimadzu
GC-2014; Kyoto, Japan) (Liu, 2006). The R2 of all calibration
curves are above 0.99.

Characterization of ACFs
The Brunauer-Emmett-Teller (BET) surface area and poros-
ities of various ACFs were determined using an ASAP 2020
vacuum volumetric sorption instrument (Micromeritics
Instrument Co., Georgia, USA) from the N2 adsorption-
desorption isotherms at 77 K. Before N2 sorption analysis, the
samples were preheated at 473 K for degassing and cooled at
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room temperature under vacuum conditions (Lin et al., 2013).

Figure 2. Sampling train for PAHs: (1) sampling probe; (2) heated filter and
heating hose; (3) thermometer; (4) cooling tube and XAD-4 adsorption tube; (5)
200 mL distilled water; (6) silica gel; (7) flow meter; (8) connect to vacuum pump.
PAHs were sampled using the EPA Modified Method 5. The
sampling time periods for PAHs after and before the passage of
the flue gas through the ACF adsorber were 10–15 and 15–20
min, respectively. The sampling flow rate for PAHs was 10
Lmin1. The removal efficiency of PAHs was defined as
follows:
%PAHs ¼ ½ðPAHsinlet  PAHsoutlet Þ:100=PAHsinlet
PAHsinlet and PAHsoutlet represent the total concentration of 16
PAHs before entering and after exiting the ACF adsorber, respec-
tively. Figure 2 shows the sampling train for PAHs. The gas
passed through a heated filter packed with fiberglass to collect
particles, and then through a cooling tube to capture the gaseous
PAHs onto a XAD-4 adsorbent (Sigma-Aldrich Co., Missouri,
USA). Next, the particles and XAD-4 containing PAHs were
The volume of the micropores (pores of size <2 nm) was calcu-
lated using the t-plot method. The mesopore volumes (pores of
size 2–50 nm) were calculated by subtracting the micropore
volumes from the total pore volume at P/P0 ¼ 0.98. The surface
functional groups of the ACFs were identified using a Fourier-
transform infrared (FTIR) spectrometer (Digilab FTX350;
American Digilab, Massachusetts, USA). The detailed FTIR
analysis procedure is described in Liu (2008). Additionally, the
contents of C, N, O, and H on the ACFs were determined using
an elemental analyzer (EA) (Elementar vario EL III; Hanau,
Germany). A Zeiss Axioplan 2 microscope (Jena, Germany)
equipped with an AxioCam HR color charge-coupled device
camera (Jena, Germany) was used to analyze the photomicro-
graphs of the ACFs.
Results and Discussion
Characterization of ACFs
(1) The detailed specific surface area and porosity of the three
ACFs, determined through N2 sorption analysis, can be viewed
in Table 2. The three ACFs have similar specific surface area and
total pore volume. Whereas the micropore and mesopore
volumes of ACF-A and ACF-C are similar, the micropore and
mesopore volumes of ACF-B are higher and lower, respectively,
than the similar corresponding volumes of ACF-A and ACF-C.
The FTIR spectra of the three ACFs can be viewed in
Figure 3. The spectra show peaks in the range 900–1300 cm1,

Table 2. Specific surface area and porosity of activated carbon fibers (ACFs) by N2 isotherms

t-Plot Method
Sample SBETa (m2/g) VTb (cm3/g) Smicroc (<2 nm) (m2/g) Vmicrod (<2 nm) (cm3/g) Vmesoe (2–50 nm) (cm3/g)
ACF-A 1175 0.57 534 0.23 0.34
ACF-B 1142 0.51 914 0.41 0.10
ACF-C 1204 0.58 579 0.25 0.34
Notes: aSpecific surface area by the Brunauer-Emmett-Teller (BET) method. bTotal pore volume at P/P0 ¼ 0.98. cMicropore surface area. dMicropore volume.
e
Mesopore volume.
 Liu et al. / Journal of the Air & Waste Management Association 64 (2014) 1038–1044
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Figure 3. FTIR spectrum for different activated carbon fibers (ACFs).
which correspond to both –C–O stretching and –O–H bending
modes, and at ~1600 cm1, which corresponds to the –C¼O
groups (Fanning and Vannice, 1993; Gaur et al., 2006; Lin et al.,
2013). Bands at ~2380 cm1 and at ~3800 cm1 in the FTIR
spectrum of ACF-A are assigned to the ketene group (¼C¼O)
and the nitrogen species, respectively (Gaur et al., 2006; Tsuji
and Shiraishi, 1997). Table 3 lists the elemental analysis of the
three ACFs and indicates that the O content of the three ACFs
follows the order of ACF-B > ACF-C > ACF-A.
It is clear from Figure 4 that the knitted structure of ACF-B is
tighter than that of ACF-A and ACF-C, which might affect its
efficiency in removing SO2 and PAHs. SO2 and PAHs can be
absorbed onto fly ash, and ACFs with tighter structures are very
efficient at removing fly ash. In addition to the tightness of ACF
knitted structures, the pore volume and surface functional groups
of ACFs may affect the adsorption capacities and mechanisms of
SO2 and PAHs on ACFs. Other than type of ACFs, the presence
Table 3. Element content of the three activated carbon fibers (ACFs) by an elemental analyzer
Element Content (wt. %)
Sample C N
ACF-A 65.19 2.62
ACF-B 52.15 2.58
ACF-C 59.14 2.22
1041
of SO2 in the incineration flue gas can decrease PAH removal
drastically because of competitive adsorption. Additionally,
reaction temperature may also affect the adsorption capacities
and mechanisms of SO2 and PAHs on ACFs. Additional detail
regarding the effects of SO2 concentration, reaction temperature,
and the type of ACFs on the simultaneous removal of SO2 and
PAHs will be provided below.
Effect of SO2 concentration on PAH removal
The effects of SO2 concentration on the removal efficiencies
of SO2 and PAHs are apparent in Figure 5. The results indicate
that the removal efficiency of PAHs is 90% in the absence of
SO2. When the concentration of SO2 is 350 ppm, the removal
efficiencies of SO2 and PAHs are 92% and 33%, respectively.
The presence of SO2 in the incineration flue gas leads to a drastic
decrease in removal of PAHs because of competitive adsorption.
These results are in agreement with those of Liu et al. (2012),
which reported that the presence of SO2 decreased the removal of
toluene because the polarity and the dipole moment of SO2 were
stronger than those of toluene. Hence, SO2 first adsorbs onto a
polar or basic adsorption site and then oxidizes to SO3 in the
presence of O2, which prevents the PAH removal efficiency from
increasing.
Figure 5 shows that the removal efficiency of SO2 decreases
markedly when the concentration of SO2 increases to 750 ppm,
and beyond this concentration no changes are apparent in
removal of PAHs with increasing SO2 concentration. This may
occur because SO2 was first adsorbed by ACFs when SO2 and
PAHs coexisted in the incineration flue gas and the effect of SO2
concentration on SO2 removal was greater than that on PAH
removal. Further, when the concentration of SO2 became very
high, the molecules of SO2 collided with each other, thereby
reducing the number of opportunities for SO2 not only to diffuse
from the surface of the ACFs into the pores in the ACFs, but also
to be adsorbed onto the ACFs (Liu, 2008). As a result, the
removal efficiency of SO2 decreased with increasing SO2
concentration.
Effect of reaction temperature on SO2 and PAH
removal
The effects of reaction temperature on the removal efficien-
cies of SO2 and PAHs are shown in Figure 6. SO2 removal is
unaffected by an increase in temperature from 160 to 280
C at
an SO2 concentration of 750 ppm. Liu (2008) previously
reported that an increase in reaction temperature from 150 to
O H O/C
27.66 3.82 0.42
40.02 4.49 0.77
30.42 4.02 0.51
 1042 Liu et al. / Journal of the Air & Waste Management Association 64 (2014) 1038–1044
Figure 4. The knitted structure of a piece of activated carbon fibers (ACFs): (a) ACF-A; (b) ACF-B; (c) ACF-C (25).
Downloaded by [Northeastern University] at 14:38 25 November 2014
Figure 5. Effects of SO2 concentration on the removal efficiencies of SO2 and
PAHs (reaction condition: reaction temperature ¼ 200
C, ACF type: ACF-A).
Figure 6. Effects of reaction temperature on the removal efficiencies of SO2 and
PAHs (reaction condition: SO2 concentration ¼ 750 ppm, ACF type: ACF-A).
260
C had a considerable effect on SO2 removal using ACFs
modified with HNO3 at an SO2 concentration of 200 ppm, with
the highest SO2 removal efficiency observed of 80% at
200
C. In this study, changes in the reaction temperature had
less of an influence on SO2 removal at a high SO2 concentration
(750 ppm) than at a low SO2 concentration (200 ppm). This may
be so because the removal efficiency of SO2 at a high SO2
concentration of 750 ppm (<30%) was too low to be affected
by the reaction temperature.
The results also show that the removal efficiency of PAHs
follows the order of 280
C > 160
C > 200
C. The concentra-
tion of two-ring PAHs (naphthalene) is much higher than the
concentrations of other PAH species in incineration flue gas. The
boiling point of naphthalene is 218
C, which is close to 200
C
(Liu, 2006). Thus, the naphthalene is removed by ACFs by
condensation at 160
C. However, the condensation of naphtha-
lene on the ACF surface would block the pores on the ACF
surface, thus decreasing the PAH removal. Further, because of
the blocking of the pores on the ACF surface, the micropores
inside the ACFs cannot be completely utilized during the adsorp-
tion process. Therefore, 280
C was the optimum temperature for
the adsorption of PAHs on ACF-A in this study. Reaction tem-
perature had a greater influence on PAH removal than on SO2
removal when SO2 and PAHs coexisted in the incineration flue
gas. Liu (2006) previously confirmed that the adsorption of
PAHs on ACFs is attributed to condensation and physical
adsorption, whereas the adsorption process between PAHs and
fly ash is attributed to chemical adsorption.
Effect of type of ACFs on SO2 and PAH removal
Figure 7 shows the effects of different types of ACFs on the
removal efficiencies of SO2 and PAHs at 200
C, because in
practice the temperature of flue gas entered into the APCD of
incinerators is 200
C. Removal efficiencies of SO2 and PAHs
when ACF-A was used as the adsorbent were similar to the
corresponding values when ACF-C was used. When ACF-B
was used as the adsorbent, the removal efficiencies of SO2 and
PAHs increased to 54% and 89%, respectively. Removal
Figure 7. Effects of different ACF types on the removal efficiencies of SO2 and
PAHs (reaction condition: SO2 concentration ¼ 750 ppm, reaction temperature ¼
200
C).
 Liu et al. / Journal of the Air & Waste Management Association 64 (2014) 1038–1044
efficiencies of SO2 and PAHs were the highest when ACF-B was
used, which is in accordance with the order of micropore volume
of the ACFs (see Table 2). Table 2 confirms that the three ACFs
have similar specific surface area and total pore volume. It can
therefore be concluded that the removal of SO2 and PAHs
depends mainly on the micropore volume of the ACFs reported
in this study.
Liu (2006) previously confirmed that micropore volume
plays an important role in determining the removal of gaseous
PAHs when the concentration of PAHs is low and the BET
surface area is sufficient for PAH removal. Kisamori and
Mochida (1994) previously demonstrated that a certain amount
of CO2 was released by the decomposition of O functional
groups at 200
C, thus reducing the amount of active sites but
increasing the mesopore volume and, in turn, increasing the
storage capacity of H2SO4 on the ACFs. As can be seen in
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Table 3, the O content of ACF-B was the highest among the
three ACFs.
It is possible to simultaneously remove fly ash and PAHs
from incinerator flue gas by using ACFs because PAHs can
be condensed or adsorbed on fly ash and ACFs are very
efficient in removing fly ash. Further, since ACF-B has the
tightest knitted structure among the three ACFs, fly ash can
be separated effectively by ACF-B. Thus, the removal of the
PAHs, which are adsorbed on fly ash, will improve because
of the tight structure of ACF-B. Thus, ACF-B, with the
highest microporous volume, highest O content, and tightest
structure among the three ACFs, was the best adsorbent for
removing SO 2 and PAHs when they coexisted in incineration
flue gas.
Conclusions
The simultaneous removal of PAHs and SO2 from incinera-
tion flue gas was examined in this study. The effect of SO2 on the
removal of PAHs and the effects of reaction temperature and type
of ACFs on removal of SO2 and PAHs were determined. The
results indicate that the removal efficiency of PAHs by using
ACF-A was 90% in the absence of SO2. When the concentration
of SO2 was 350 ppm, the removal efficiencies of SO2 and PAHs
by using ACF-A were 92% and 33%, respectively. The presence
of SO2 in the incineration flue gas can decrease the removal of
PAHs drastically because of competitive adsorption onto the
ACFs. However, removal of PAHs was insignificant when the
concentration of SO2 increased from 350 ppm to greater than
750 ppm (SO2 concentration up to 1000 ppm were examined).
Moreover, the variation in SO2 removal was insignificant at an
SO2 concentration of 750 ppm when the temperature increased
from 160 to 280
C, and the removal efficiency of PAHs fol-
lowed the order 280
C > 160
C > 200
C. ACF-B, with the
highest microporous volume, highest O content, and tightest
structure among the three studied ACFs, was found to be the
best adsorbent for removing SO2 and PAHs when these gases
coexisted in incineration flue gas.
1043
Funding
The authors thank the National Science Council of the
Republic of China (Taiwan) for financially supporting this
research under contract no. NSC 96-2211-E-131-019-MY3.
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About the Authors
Zhen-Shu Liu is an associate professor, Wen-Kai Li was a postgraduate student,
and Ming-Jui Hung is an assistant professor in the Department of Safety, Health
and Environmental Engineering at the Ming Chi University of Technology, New
Taipei City, Taiwan.