Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv
Review article
Department of Chemical Engineering, King Fahd University of Petroleum & Minerals, Dhahran 31261, Saudi Arabia
Center for Integrative Petroleum Research, King Fahd University of Petroleum & Minerals, Dhahran 31261, Saudi Arabia
h i g h l i g h t s
Common VOCs, their sources and impacts.
Alternative techniques for VOCs destruction/separation.
Catalytic oxidation of VOCs.
Mechanism of catalytic oxidation of VOCs.
Recent development of VOCs oxidation catalysts.
a r t i c l e i n f o
a b s t r a c t
Article history:
Received 22 January 2016
Received in revised form
27 April 2016
Accepted 17 May 2016
Available online 18 May 2016
Emission of volatile organic compounds (VOCs) is one of the major contributors to air pollution. The main
sources of VOCs are petroleum reneries, fuel combustions, chemical industries, decomposition in the
biosphere and biomass, pharmaceutical plants, automobile industries, textile manufacturers, solvents
processes, cleaning products, printing presses, insulating materials, ofce supplies, printers etc. The most
common VOCs are halogenated compounds, aldehydes, alcohols, ketones, aromatic compounds, and
ethers. High concentrations of these VOCs can cause irritations, nausea, dizziness, and headaches. Some
VOCs are also carcinogenic for both humans and animals. Therefore, it is crucial to minimize the emission
of VOCs. Among the available technologies, the catalytic oxidation of VOCs is the most popular because of
its versatility of handling a range of organic emissions under mild operating conditions. Due to that fact,
there are numerous research initiatives focused on developing advanced technologies for the catalytic
destruction of VOCs. This review discusses recent developments in catalytic systems for the destruction
of VOCs. Review also describes various VOCs and their sources of emission, mechanisms of catalytic
destruction, the causes of catalyst deactivation, and catalyst regeneration methods.
2016 Elsevier Ltd. All rights reserved.
Keywords:
VOCs
Oxidation
Oxidation process
Catalysts
Multicomponent catalysts
Mechanism
Kinetics
1. Introduction
Volatile organic compounds (VOCs) are those organic compounds with a Reid vapor pressure of over 10.3 Pa at normal temperature (293.15 K) and pressure (101.325 kPa). The VOCs are a
large group of carbon-based chemicals that easily evaporate at
room temperature (Li et al., 2009; Ojala et al., 2011; Olsen and
Nielsen, 2001). Table 1 lists the physicochemical and thermodynamic properties of common VOCs (Ihsan, 1995). VOCs are classied as major contributors to air pollution. They contribute both
indirectly as ozone/smog precursors and directly as substances
toxic to the environment (Amann and Lutz, 2000; Finlayson-Pitts
* Corresponding author.
E-mail address: mhossain@kfupm.edu.sa (M.M. Hossain).
http://dx.doi.org/10.1016/j.atmosenv.2016.05.031
1352-2310/ 2016 Elsevier Ltd. All rights reserved.
118
Table 1
Physical, chemical, and thermodynamic properties of common VOCs (Ihsan, 1995).
Compound
Formula
Cp (J/mol C)
B.P. ( C)
DGf (kJ/mol)
DHf (kJ/mol)
DHc (kJ/mol) @ 25 C
Toluene
Propane
Benzene
Ethylbenzene
o-Xylene
Acetylene
Acetone
Formaldehyde
n-Hexane
Dicholoromethane
Tricholoromethane
Tetracholoromethane
Tricholoroethylene
Tetracholoroethylene
Acetaldehyde
Ethylene
C7H8
C3H8
C6H6
C8H10
C8H10
C2H2
C3H6O
CH2O
C6H14
CH2Cl2
CHCl3
CCl4
C2HCl3
C2Cl4
C2 H4 O
C2 H4
166.0
73.8
136.1
185.9
188.8
44.1
125.0
35.4
195.0
50.8
65.8
133.9
80.02
95.6
53.7
42.9
110.6
42
80.1
136
144
84
56
19
68
39.6
61.2
76.72
87.2
121.1
20.2
103.7
114.09
23.4
124.5
120.0
110.8
209.2
155.3
109.9
4.0
68.9
68.5
62.5
6.7
20.6
133.2
68.4
12.0
103.8
49.0
12.5
24.4
226.7
248.1
115.9
198.8
95.5
101.3
132.8
19.1
14.2
166.4
52.5
3909.8
2220.0
3267.6
4564.7
4552.8
1299.6
1789.9
563.4
4163.1
583.8
435.2
260.7
910.8
772.8
1192.3
1411.1
aldehydes, aromatics, alkanes, ketones, olens, ethers, esters, parafns, and sulfur containing compounds (Carpentier et al., 2002;
Doggali et al., 2012; Khan and Kr Ghoshal, 2000; Miranda-Trevino
and Coles, 2003; Ozturk and Yilmaz, 2006; Soylu et al., 2010;
Yose et al., 2015).
The effect of VOCs on the atmosphere depends on the nature of
VOCs, their concentration, and emission sources. However, they
have been identied as been responsible for stratospheric ozone
depletion, tropospheric ozone formation, ground level smog formation, climate change, sick building syndrome, decay of plants,
toxicity of the atmosphere, and carcinogenic effects in humans
(Carabineiro and Thompson, 2007; Masui et al., 2010; Ozturk and
Yilmaz, 2006). As most of the countries have imposed strict conditions to limit VOCs in the environment, there are numerous
research initiatives around the world developing efcient technologies to meet the stringent environment regulations.
The emission of VOCs can be controlled using methods based on
recovery and destruction. The techniques based on recovery
include absorption, adsorption, membrane separation, and
condensation. High concentrations of VOCs, especially watersoluble compounds can be removed from ue gas streams by absorption using a suitable solvent. The disposal of VOCs and the
spent solvent from an absorber are the common problems faced by
the absorption processes. Physical and/or chemical adsorption is
another technique in which a suitable adsorbent (activated carbon,
zeolite, polymeric adsorbents etc.) is employed to selectively
adsorb the VOCs. Adsorption approach is economical only in situations where VOCs are highly diluted in a ue gas stream. The high
cost of the adsorbents and the necessity of frequent regeneration of
the adsorbent are the major limitations of adsorption processes
(Kujawa et al., 2015). The VOCs can be removed using condensation
induced by increasing the system pressure at a given temperature
or lowering the temperature at a given pressure. One of the limitations of the condensation processes is the disposal of the spent
coolants. Due to the energy intensive nature of the process,
condensation is limited to only evaporative solvents (Shah et al.,
2000). Membrane separation is another possible alternative for
the removal of VOCs. Silicon rubber membranes are the most
commonly used membrane for the separation of VOCs. In the bioltration process, VOCs in the air is removed biologically in a solid
phase reactor (Leson and Winer, 1991). In this approach, the
contaminated wet-gas is fed at the bottom of the lter and the
contaminants in air diffuse into a wet, biologically active layer (i.e.,
biolm) on the surface of the lter particles. The biolm with aerobic bacteria degrades the target pollutant(s) and produces CO2,
water, and microbial biomass. Both the membranes and
119
Aromatic compounds such as benzene, toluene, and ethylbenzene occur naturally in petroleum products, including gasoline
and other fuels produced from crude oil. Consequently, the
incomplete combustion of liquid fuels in automobiles releases
signicant amounts of aromatic compounds into the atmosphere.
These compounds are also used in various products and formulations such as petrochemicals, paint, medicine, and detergents
(Ozelik
et al., 2009). Aromatic compounds are not only toxic and
carcinogenic, but also cause severe damage to the ozone layer,
produce photochemical smog, and pose mutagenic hazards (Kim
and Shim, 2010). The aromatic solvents commonly used in paints,
thinners, gums, adhesives, lacquers, and printing inks, are classied
as priority pollutants (Shahna et al., 2010). At low-level exposure,
aromatic VOCs can cause weakness, confusion, nausea, loss of
appetite and memory, tiredness, and loss of sight. Inhalation of a
high level of aromatic compounds can cause unconsciousness,
dizziness, and even death (Kim, 2002; Suib, 2013). The maximum
safe limit of aromatic compounds is 1 mg/L in drinking water and
200 ppm in air (Alifanti et al., 2007; Blanco et al., 2007; Chen et al.,
2008a; de Rivas et al., 2006; Delimaris and Ioannides, 2008b;
Huang et al., 2008a; Luo et al., 2007; Musialik-Piotrowska and
et al., 2001b; Scire
Landmesser, 2008; Palacio et al., 2008; Scire
et al., 2003; Tidahy et al., 2007, 2008; Wang et al., 2008; Wu et al.,
2000; Zhang et al., 2008; Li et al., 2015).
2.4. Polycyclic aromatic hydrocarbons
Polycyclic aromatic hydrocarbons (PAH) are a family of VOCs,
and they are mainly released by combustion processes (VarelaGanda et al., 2013). These compounds contain several benzene
rings in their structure. Some typical examples of PAH are naphthalene (two rings), phenanthrene (three rings), and pyrene (four
rings). The main sources of PAH are incomplete fuel combustion,
asphalt transformation plants, and coal power plants (Diehl et al.,
2010; Puertolas et al., 2010). PAH have been identied as carcinogenic and therefore, it is extremely important to reduce their
emission (Kim et al., 2007b).
2.5. Alcohols and ketones
Alcohols and ketones are commonly used in cosmetics and
personal care products such as nail polish, nail polish removers,
colognes, perfumes, rubbing alcohol, and hair spray. Ketones are
used in aerosols, varnishes, window cleaners, paint thinners, and
adhesives (Makshina et al., 2008; Santos et al., 2011). Common
alcohol based VOCs include ethyl alcohol, isopropyl alcohol, benzyl
alcohol, while acetone, methacrylates (methyl or ethyl), ethyl acetate, and methyl ethyl ketone are ketone based VOCs.
120
1
y
Cx Hy x y O2 /xCO2 H2 O
4
2
rVOC
(2)
rVOC
rVOC
2
(3)
(4)
(1)
Fig. 1. Schematic of oxidation of VOCs (benzene) on MnO (Li et al., 2011).
rVOC
(5)
The validity of each mechanism strongly depends on the properties of the catalyst (active metal and the support) as well as on the
nature of the VOCs. Generally, one of the above models provides a
good t for the experimental data for the oxidation of the VOCs
over metal-oxide and noble-metal catalysts.
Table 2 summarizes the kinetics models and the estimated
activation energies for the oxidation of a range of VOCs reported in
the literature. The activation energy varies between 10 and 50 kcal/
mol. Choudhary and Deshmukh conducted a kinetic study of the
combustion of propane and methyl ethyl ketone (MEK) over Crdoped ZrO2 (Choudhary and Deshmukh, 2005). Although the
experimental data t both the power law and MVK model
reasonably well, the MVK model gave the best t. Activation energy
for the combustion of propane and MEK was determined to be
16.5 kcal mol1 and 13.2 kcal mol1, respectively. Ordonez et al.
showed that the kinetics of the oxidation of aromatic compounds
(benzene and toluene) over Pt/g-Al2O3 cab be expressed using the
MVK model. The estimated activation energy of benzene and
toluene are 24 and 25 kcal/mol, respectively (Ordonez et al., 2010).
Radic et al. studied the kinetics of the oxidation of n-hexane and
toluene over 0.12% Pt/Al2O3 (Radic et al., 2004). MVK type rate
expression was used to calculate the reaction rate constant. The
activation energy for the chemisorption decreases with increasing
Pt crystallite size. On the other hand, the activation energy for the
surface reaction is independent of the Pt crystallite size. Gangwal
et al. also applied the MVK mechanism to study the kinetics of the
oxidation of n-hexane (Gangwal et al., 1988). Pei et al. tted the
experimental data of the catalytic oxidation of formaldehyde over
copper manganese oxide to three models including rst order kinetics, LH, and the MVK models (Pei et al., 2015). They proposed the
following models and tted the experimental data to them: (i)
single-variable (surface concentration) kinetic model; (ii) twovariable kinetic model (surface concentration and water vapor
concentration); and three variable model (surface concentration,
water vapor concentration, and temperature). The best t of the
experimental data was obtained for the LH model that considers
two adsorbed reactants with competitive adsorption. The goodness
121
Table 2
Summary of the activation energy of the oxidation of some VOCs, and the catalysts and kinetics models used.
VOCs
Catalyst
Model type
Reference
Cr-doped ZrO2
Cr-doped ZrO2
Pd
Pt/Al2O3
Pt/Al2O3
Pt,Ni/g-Al203
Pt,Ni/g-Al203
CuO/MnO2
Pd/activated- C
Cu1.5Mn1.5O4
MnO2
Cr2O3
Mn2O3/g-Al2O3
Cu0.13Ce0.87Oy
Pt/g-Al2O3
Pt/g-Al2O3
Pt/g-Al2O3
Mars-van Krevelen
Power law
Power law
Mars-van Krevelen
Mars-van Krevelen
Mars-van Krevelen
Mars-van Krevelen
Langmuir-Hinshelwood
Langmuir-Hinshelwood
Mars-van Krevelen
Power Law
Power Law
Power Law
Langmuir-Hinshelwood
Mars-van Krevelen
Mars-van Krevelen
Mars-van Krevelen
16.5
13.2
48.2
22.4
17.4
22.9
19.6
13.2
19.8
26.6
9.3
10.5
10.4
26.1
24.1
25.3
31.8
122
2011). Also they are less stable in the presence of chloride compounds (Everaert and Baeyens, 2004). Several investigations on
noble-metal catalysts on different supports have been reported
(Cant and Hall, 1970). Performance of these catalysts depends on
the method of preparation, precursor type, particle size, metal
loading, concentration of the VOCs, reactor type, and the overall gas
ow rate (Cant et al., 1998; Carballo and Wolf, 1978; Radic et al.,
2004). Larger the heat of formation of an oxide the lesser the activity of the catalyst. Use of noble-metal catalysts in propylene
oxidation indicates that the total reaction rate increases with the
oxygen pressure and decreases with the olen pressure. For Rh and
Ir the oxidation rate increases with the olen pressure and decreases with the oxygen concentration. On the contrary, Ru catalysts show higher oxidation rate with increased oxygen pressure
while the rate is independent of the olen pressure (Cant and Hall,
1970; Carballo and Wolf, 1978). Paulis et al. studied the effect of
chlorine, which is normally added as a catalyst precursor, on the
oxidation of toluene on the Pt/Al2O3 catalyst (Paulis et al., 2001).
Chlorinated precursors increase the surface acidity and decrease
the adsorption of carbonates and bicarbonates on the surface of the
support during CO oxidation. Moreover, using chlorinated precursors will result in platinum oxychloride species, which have a
higher reduction temperature.
Supported noble metals (Pt, Pd, Rh etc.) are attractive as catalysts due to their high efciency for the removal of VOCs at low
temperatures (Avgouropoulos et al., 2006; Liotta, 2010;
dar et al., 2004; Papaefthimiou et al., 1999; Tidahy
Maldonado-Ho
et al., 2007). The most common support materials for the noble
metal catalysts are ceramics or metallic material in monolithic or
honeycomb form. Table 3 summarizes some noble metal catalyst
systems reported recently. Noble-metal-based catalysts are
expensive and can be deactivated by sintering or poisoning (Liotta,
2010) and alone they are not normally selective enough (Ojala et al.,
Table 3
Reported Noble-metal catalyst systems for the oxidation of VOCs.
Catalyst
Support
VOCs
Temp (oC)
Conversion %
References
Pd
Au
Au
Pd
Pt
Pt
Pt
Pt
Au
Au
Au
Au
Au
Au
Au
Au
Au
Au
Au
Au
Au
Pt
Pt
Pt
Pt
Au
Pd
Pd
Nb2O5
CeO2-ZrO2-TiO2
CeO2/Fe2O3
Co3O4
Al2O3
CeO2
CeO2
Al2O3
CuO
Fe2O3
La2O3
MgO
NiO
CuO
Fe2O3
La2O3
MgO
NiO
Co3O4
Co3O4
Co3O4
Activated carbon
Activated carbon
Activated carbon
Activated carbon
Fe2O3
Co3O4
Al2O3
Toluene
Propane
Benzene
Xylene
Toluene
n-butanol
n-butanol
n-butanol
Ethyl acetate
Ethyl acetate
Ethyl acetate
Ethyl acetate
Ethyl acetate
Toluene
Toluene
Toluene
Toluene
Toluene
Benzene
Toluene
Xylene
Benzene
Toluene
Ethylbenzene
Xylene
Toluene
o-Xylene
o-Xylene
440
360
200
249
200
167
135
165
311
354
325
290
345
315
345
>400
387
320
189
138
162
112
109
106
104
260
254
145
90
50
100
90
95
90
90
90
100
100
100
100
100
100
100
100
100
100
90
90
90
100
100
100
100
90
90
90
preparation, size and shape of the gold nanoparticles, and con and Liotta, 2012).
centration of VOCs (Scire
Carabineiro et al. used Au catalysts supported on La2O3, MgO,
NiO, and Fe2O3 for the oxidation of toluene (Carabineiro et al.,
2015b). They showed that the reducibility and the crystal size are
major factors affecting the catalytic activity, while the oxidation
state of Au has no effect on the catalytic activity (Carabineiro et al.,
2015b).
Au/Co3O4 system has been reported as the most active system
for the combustion of light alkanes (Haruta, 1997a; Waters et al.,
1994). Au/CeO2 and Au/MnOx have been used to oxidize different
VOCs such as toluene and ethyl acetate (Bastos et al., 2012). At
250 C, both Au/CeO2 and Au/MnOx oxidize ethyl acetate into CO2.
Au/Mn5O10 catalyst system completely oxidizes ethanol at 230 C.
Toluene oxidation is the toughest and it has been achieved at
300 C with Au/Mn3O4. Gold catalysts supported on ceria have been
used for the oxidation of benzene, toluene, propanol, propene, and
formaldehyde (Lakshmanan et al., 2010; Pinna, 1998; Scire et al.,
2003; Shen et al., 2008).
Solsona et al. investigated a catalyst based on gold supported on
nickel-cerium oxide for the oxidation of propane (Solsona et al.,
2011). These catalysts showed good activity, which is due to the
high surface area of the catalyst, low bond strength (Ni-O), and the
high reducibility of the nickel sites (Solsona et al., 2011). Shen et al.
studied several Au/CeO2 catalysts with a gold content of less than
0.85%, prepared by different routes for formaldehyde oxidation
(Shen et al., 2008). The results indicate that gold catalysts with a
high dispersion are more active in the oxidation of formaldehyde,
while the formation of larger crystals decreases the activity of the
catalyst.
4.1.2. Palladium catalysts
Palladium catalysts have a higher thermal and hydrothermal
resistance compared to other noble metal catalysts (Huang et al.,
2008b). There are different views on the contribution of the
metallic state and oxidized state of Pd to the oxidation reactions of
VOCs. Some authors believe that the oxidized state is more
lin and Primet, 2002), while others
important (Burch et al., 1996; Ge
consider that the metallic state is more important in oxidation
ge
et al., 2000; Huang et al., 2008b; Ihm et al., 2004).
reactions (De
Some results suggest that both states are equally important
(Yazawa et al., 1998). The support plays an important role in the
activity of Pd-based catalysts. Normally the porous supports increase the activity of Pd catalysts due to the stabilization of active
Pd species on porous structures (Centi, 2001; Wang et al., 2013b).
Acid-base properties of the supports are known to inuence the
activity of Pd catalysts. Weakly acidic supports provide high catalytic activity (Okumura et al., 2003). Pd-based catalysts are more
efcient than noble-metal catalysts and metal-oxide catalysts in
removing benzene, toluene, xylene, and methane (Centi, 2001;
Huang et al., 2008b; Kim and Shim, 2009).
Wang et al. showed that Pd/Co3O4 catalysts possess high efciency for the oxidation of xylene. Efciency depends on the particle size, oxidized Pd species, and the oxygen vacancies on the
support (Wang et al., 2013b). The comparison of two Pd/Co3O4
catalysts synthesized by in situ nanocasting and post-impregnation
methods indicates that the catalyst synthesized by in situ nanocasting has a high catalytic activity. The high activity is due to the
more ordered structure of the catalyst and the well dispersed PdO
species. Huang et al. found that the catalytic activity of the Pd/Al2O3
catalysts increased with the increasing Pd loading (Huang et al.,
2008b). Ihm et al. showed that the pre-treatment methods
strongly affect the activity of the Pd/Al2O3 catalysts [140]. Catalysts
treated in hydrogen showed higher activity compared to the catalyst treated in air.
123
124
Table 4
Some reported metal-oxide catalysts for the oxidation of VOCs.
Catalyst
Support
VOCs
Temp
Conversion %
References
Co3O4
Co3O4
Co3O4
Co3O4
CuO
Co3O4
CeO2
Nb2O5
Clay
Clay
e
e
e
e
Aluminosilicate
e
Acetylene
Propylene
1,2-Dichloroethane
Ethyl acetate
Ethyl acetate
Propane
Acetone
Toluene
360
460
350
245
280
250
200
400
100
100
100
100
e
99
85
90
125
126
Table 5
Some reported mixed-oxide catalysts for the oxidation of VOCs.
Catalyst
VOC
Temp ( C)
Conversion (%)
References
Ce-Co
La-Co
Mn-Ce
Mn-Ce
Mn-Ce
Mn0.5Ce0.5-O2
Cu-Ce
Cu0.3Ce0.7Ox
Cu0.3Ce0.7Ox
Mn-Co
Mn-Co
Mn-Co
Mn-Co
Mn-Co
MnOx-TiO2
MnOx-TiO2-SnOx
Ce-Zr
Cu-Co
Toluene
Toluene
Benzene
Toluene
Ethyl acetate
Formaldehyde
Chlorobenzene
Toluene
Propanol
Toluene
Ethylbenzene
Ethyl acetate
n-hexane
Toluene
Chlorobenzene
Chlorobenzene
1-2 Dichloroethane
Benzene
250
300
260
245
180
270
328
212
192
250
250
194
210
250
177
177
120
290
100
100
90
90
90
100
99
90
90
98.7
90
90
90
100
90
90
90
90
release from the catalyst matrix (Yose et al., 2015). For example,
CeO2 catalysts achieved 90% conversion of trichloroethylene, but is
not thermally stable and deactivates within a few hours due to
adsorption of HCl and Cl2 (Dai et al., 2008). However, modifying
CeO2 with other metals can improve the oxygen storage capacity,
thermal resistance, and enhance its activity (Gluhoi et al., 2005;
Trovarelli et al., 1999).
CuO-CeO2 mixed-metal catalysts have been investigated in the
combustion reactions of CO and CH4, the reduction of NO, and the
wet oxidation of phenol (Avgouropoulos and Ioannides, 2003; Liu
and Flytzanistephanopoulos, 1995; Liu et al., 1994). The high efciency is attributed to the promoting effect of ceria due to the high
oxygen storage capacity. Cu-Ce oxides have been studied for the
oxidation of the following VOCs: ethyl acetate, ethanol (Larsson and
Andersson, 1998), benzene (Hu et al., 2008), and toluene (Delimaris
and Ioannides, 2009). This catalyst system has been synthesized
using combustion (Rao et al., 2003), thermal decomposition
(Xiaoyuan et al., 2001), impregnation, co-precipitation, and sol-gel
method (Zheng et al., 2005). He et al. synthesized Cu-Ce mixedoxide catalysts using the self-precipitation approach and investigated their efciency for toluene and propanol oxidation (He et al.,
2014). Cu and Ce have a synergistic effect on the reducibility of the
mixed-oxide catalyst. Low temperature reducibility is the highest
for Cu0.3Ce0.7Ox followed by Cu0.15Ce0.85Ox, Cu0.4Ce0.6Ox, and
CuCeOx.
In the oxidation of ethyl acetate, ethanol, and toluene the mixed
catalyst system has a lower activity compared to the individual
metal oxides due to the suppression of the intrinsic activity by
combining the two metal oxides (Delimaris and Ioannides, 2009).
MnOx-CeO2 catalyst system has been investigated for the abatement of different types of VOCs, such as ethanol (Rao et al., 2007),
formaldehyde (Tang et al., 2006), hexane (Picasso et al., 2007),
phenol (Chen et al., 2001), ethyl acetate (Delimaris and Ioannides,
2008a), and toluene (Delimaris and Ioannides, 2008a). These catalysts are mainly prepared by the sol-gel method (Rao et al., 2007;
Tang et al., 2006), co-precipitation (Chen et al., 2001; Picasso et al.,
2007; Qi et al., 2004; Silva et al., 2004; Tang et al., 2006), and
combustion (Delimaris and Ioannides, 2008a).
CeO2-CrOx mixed catalysts show excellent performance in the
removal of various halogenated VOCs (Yang et al., 2015b). Yang et al.
(2015a) showed that the formation of Cr6 species with its strong
oxidizing ability and the oxygen defects are enhanced due to the
good synergism between CeO2 and CrOx. All the mixed catalysts
prepared under different conditions show better performance
127
128
129
130
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