Journal of Natural Gas Chemistry 19(2010)369–374

Effect of O2 and H2O on the tri-reforming of the simulated

biogas to syngas over Ni-based SBA-15 catalysts
Daoan Sun1 , Xiujin Li2 , Shengfu Ji1∗ , Lingyan Cao1
1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
2. Department of Environmental Engineering, Beijing University of Chemical Technology, Beijing 100029, China
[ Manuscript received January 21, 2010; revised March 5, 2010 ]

Abstract
A series of Ni/SBA-15 catalysts with Ni contents from 7.5 wt% to 15 wt% were prepared by impregnation method. The effect of O2 and H2 O
on the combined reforming of the simulated biogas to syngas was investigated in a continuous flow fixed-bed micro-reactor. The stability of the
catalyst was tested at 800 ◦ C. The results indicated that 10wt%Ni/SBA-15 catalyst exhibited the highest catalytic activities for the combined
reforming of the simulated biogas to syngas. Under the reaction conditions of the feed gas molar ratios CH4 /CO2 /O2 /H2 O = 2/1/0.6/0.6,
GHSV = 24000 ml·g−1 cat ·h
−1 and the reaction temperature T = 800 ◦ C, the conversions of CH and CO were 92.8% and 76.3%, respectively,
4 2
and the yields of CO and H2 were 99.0% and 82.0%, respectively. The catalytic activities of the catalyst did not decrease obviously after 100 h
reaction time on stream.
Key words
biogas; reforming; syngas; oxygen; steam; Ni-based catalyst; SBA-15

1. Introduction syngas has been reported by many researchers. Liu et al.

[3] reported that the complex nano-catalysts could be suc-
Biogas which is composed of CH4 and CO2 with the vol- cessfully applied to the carbon dioxide reforming of methane
ume ratio of 2 could be produced by anaerobic fermentation of and the CH4 conversion of 85% could be reached at 700 ◦ C
agriculture wastes [1]. As the fossil energy resource reduces with the feed composition of CH4 : CO2 = 1 : 1 (molar ra-
sharply and the pollution of the environment becomes more tio). Chen et al. [4] studied the carbon dioxide reforming of
serious, people are searching for new energy for future. Bio- methane on Ni/Ce/MgO catalyst and found that the CH4 con-
gas is becoming more generally preferred. Further more, both version of 96% and CO2 conversion of 96% could be achieved
CH4 and CO2 are regarded as the main kinds of greenhouse at 850 ◦ C with the feed composition of CH4 : CO2 = 1 : 1.
gases, which pose a grave threat to global climate and envi- Wan et al. [5] investigated the steam reforming of methane
ronment. So if we could make use of the biogas effectively, over Ni/SBA-15 catalyst and reported that CO selectivity of
it would result in considerable economic and environmental 76% could be reached with CH4 conversion of 99.6% un-
benefits [2]. On the basis of the gas composition of biogas, der the reaction temperature of 800 ◦ C and the molar ratio
biogas was used as a raw material and an appropriate amount of CH4 : H2 O of 0.5. Hu et al. [6] reported the steam re-
of oxygen and/or steam was added for autothermal reforming forming of methane on Ni/ZrO2 catalyst, and found that the
and/or for the combined reforming to produce synthesis gas. CH4 conversion and the CO selectivity could reach 85% and
In this way, the syngas and basic chemical materials could be 70%, respectively, at 650 ◦ C with the feed composition of
produced via biomass and such a non-fossil route should pos- H2 O : CH4 : N2 = 2 : 1 : 2.67. Fabien et al. [7] discovered that
sess attractive prospects. the CH4 conversion was nearly 96.5% and the selectivity of
It is well recognized that the reforming of CH4 to syn- H2 and CO was 93.5% and 97.8%, respectively, in the partial
gas plays a crucial role in the combined reforming of the oxidation of methane to syngas on the Ni/SBA-15 catalyst at
simulated biogas. In recent years, the reforming of CH4 to 850 ◦ C when the feed composition of CH4 : O2 was 1.9. Song
∗ Corresponding author. Tel: +86-10-64419619; Fax: +86-10-64419619; E-mail: jisf@mail.buct.edu.cn
This work was supported by the National Basic Research Program of China (Project No. 2005CB221405), the National “863” Project of China (No.
2006AA10Z425) and the Beijing Natural Science Foundation (Project No: 8062023).

Copyright©2010, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. All rights reserved.
doi:10.1016/S1003-9953(09)60096-7
370 Daoan Sun et al./ Journal of Natural Gas Chemistry Vol. 19 No. 4 2010

et al. [8] successfully applied Ni/ZrO2 catalyst to partial water and 4 mol/L hydrochloric acid of 60 g. The solution
oxidation of methane (POM) reaction and observed that the was stirred at 40 ◦ C for 2 h, and 8.5 g of tetraethyl orthosili-
H2 selectivity of 93% and the CO selectivity of 92.5% could cate (TEOS) was then slowly added to the mixture with vigor-
be reached, respectively, at a CH4 conversion of 86.7% under ous stirring at 40 ◦ C for 22 h. The gel mixture was transferred
700 ◦ C when the feed composition CH4 : O2 = 2. into a Teflon bottle and was heated at 100 ◦ C for 24 h under
More recently, some preliminary research work has been static conditions. The solid product was filtered, washed with
conducted in our research group on the reforming of the sim- deionized water for five times, then dried at room temperature
ulated biogas to syngas. Huang et al. [9] reported the re- and finally calcined at 550 ◦ C for 6 h in air in order to remove
forming of the simulated biogas with steam to syngas on the the organic template of triblock copolymer.
MgO/Ni/SBA-15 catalysts and found that the CH4 conver- Ni-based catalysts, with the nickel contents from 7.5 wt%
sion of 98% and CO2 conversion of 92% could be achieved to 15 wt%, were prepared by the impregnation method.
at 850 ◦ C when the feed composition CH4 : CO2 : H2 O was Firstly, SBA-15 was impregnated with a Ni(NO3 )2 solution,
2 : 1 : 1.5. Lang et al. [10] studied the combined reforming then dried at 100 ◦ C for 24 h and calcined at 550 ◦ C for 6 h in
of the simulated biogas to syngas with oxygen to syngas on muffle furnace.
the La/Ni/SBA-15 catalysts and found that CH4 conversion
of 97.7% and CO2 conversion of 93.8% could be achieved at 2.2. Catalyst activity test
850 ◦ C with the feed ratios of CH4 : CO2 : O2 = 2 : 1: 0.57.
However, these research works were mainly based on the
Figure 1 shows a schematic diagram of the fixed-bed
modification of the reforming catalysts and the reforming re-
continuous-flow quartz reactor (i.d. 6 mm) for the combined
action of the simulated biogas was conducted by solely using
reforming of the simulated biogas to syngas. The reactant gas
either H2 O or O2 . However, few attentions had been paid to
stream consisted of CH4 , CO2 , O2 and H2 O with different
the effect of both O2 and H2 O on the combined reforming
molar ratios. The flow rates of the gas components were con-
reaction. Moreover, compared to the reforming of methane
trolled by a mass flow controller (Beijing Seven Star Electron-
by solely using O2 or H2 O to syngas, the tri-reforming [11]
ics CO. LTD., D08-1A/ZM) while water was fed with a sy-
of methane clearly showed some advantages, such as energy
ringe pump (Beijing Satellite Manufacturing Factory, SZB-2)
saving, easy adjustment of H2 /CO molar ratios, and so on
into an evaporator installed at the inlet of the reactor and then
[12−14]. In addition, the tri-reforming of methane was es-
mingled with other feed gases. At last, they entered the reac-
pecially suitable for the system that two or three kinds of gas
tor together through a heating belt. The mass of the catalyst
coexisted, such as power plant flue gas, coal bed gas, liquefied
used was 0.2 g.
natural gas, and others [15]. Consequently, the tri-reforming
Prior to reaction, the catalyst was reduced in a stream of
of the biogas using both H2 O and O2 to syngas is very
hydrogen (10 ml/min) at 750 ◦ C for 3 h and cooled to 700 ◦ C
important.
by Ar. The reaction was carried out at temperature varying
SBA-15, a new kind of molecular sieve, which possesses from 700 to 850 ◦ C and the gas products were treated by a
larger pores, thicker walls and higher thermal stability, has cool trap in order to remove water before they entered the
been used as a catalyst support in several catalytic reactions analytical phase. Along with the reaction, the gas products
[16−18]. Ni-based SBA-15 catalysts have been applied to the were collected and analyzed by an on line Gas Chromatograph
reforming of CH4 with steam or CO2 and the results showed (Beijing East & West Electronics Institute, GC-4000 A) with
that it was a promising catalyst support [19,20]. The main a TDX-01 column and a thermal conductivity detector. After
goal of this research is to provide some useful information for reaction, the catalyst was cooled to room temperature under
the reforming biogas to syngas. In present study, a series of N2 protection.
Ni-based catalysts were prepared. The effect of Ni contents
In this work, the catalytic performances of the combined
of the catalysts, addition amount of O2 and H2 O in the sim-
reforming over the catalysts such as CH4 conversion, CO2
ulated biogas, and the catalyst stability for the tri-reforming
conversion, H2 yield and CO yield were calculated as follows:
was investigated.
FCH4 ,in − FCH4 ,out
XCH4 = × 100% (1)
2. Experimental FCH4 ,in
FCO2 ,in − FCO2 ,out
2.1. Catalyst preparation XCO2 = × 100% (2)
FCO2 ,in
FCO,out
Before preparation of the catalysts, SBA-15 support was YCO = × 100% (3)
prepared according to the method described extensively in FCH4 ,in + FCO2 ,in
previously published articles [7]. Typically, it was synthe- FH2 ,out
sized from sodium silicate with a triblock copolymer (P123), YH2 = × 100% (4)
2FCH4 ,in + FH2 O,in
which was used as a precursor agent. In a typical synthesis,
4.0 g of triblock copolymer P123 (Aldrich, EO20 PO70 EO20 , where, FCH4 ,in , FCO2 ,in and FH2 O,in are inlet flow rates and
M = 5800) was dissolved in a solution with 90 g deionized FCH4 ,out , FCO2 ,out and FH2 ,out are outlet gas flow rates.
 Journal of Natural Gas Chemistry Vol. 19 No. 4 2010 371

and thus the apparent conversion of CO2 was suppressed.

As we can see from Figure 2, when the oxygen did not
add to the feed gas, the H2 /CO molar ratio of the product was
0.95 and it increased markedly from 0.95 to 1.26 when added
oxygen was amounted to 0.4. However, only a slight increase
from 1.26 to 1.30 in the H2 /CO molar ratio could be observed
with further increasing the added oxygen from 0.4 to 1.0 mo-
lar ratio. It is reasonable that with the addition of oxygen the
partial oxidation of methane which exists in the autothermal
reforming will be prevailed, leading to the increase of H2 /CO
molar ratio. Jing et al. [22] also reported that the H2 /CO mo-
lar ratio increased obviously from 0.95 to 1.86 when O2 /CH4
molar ratio moved up from 0 to 2. It indicated that the H2 /CO
molar ratio could be flexibly adjusted by the added amount
of oxygen in order to meet the requirements of downstream
processes.
Figure 1. Schematic diagram of the experiment. 1—Plunger pump, 2— Briefly, 10wt%Ni/SBA-15 catalyst exhibited a high cat-
Mass flow meter, 3—Valve, 4—Evaporator, 5—Heating belt, 6—Furnace, alytic activity for reforming of the simulated biogas when the
7—Catalyst bed, 8—Quartz reactor, 9—Cold trap, 10—GC
CH4 : CO2 : O2 molar ratio of the feed gas was 2 : 1 : 0.6. In
this case, the conversion of CH4 and CO2 can reach 90.8%
and 86.0%, respectively.
3. Results and discussion

3.1. The ef fect of added amount of oxygen on the catalytic

performances

Reforming of the simulated biogas alone was in essence

the carbon dioxide reforming of methane, which was a highly
endothermic reaction. In addition, methane was in excess
stoi-chiometrically. As a result, different amount of oxy-
gen was added into the simulated biogas for reforming.
The effect of oxygen amount on the catalytic performances
of 10wt%Ni/SBA-15 was investigated, and the results were
shown in Figure 2.
As shown in Figure 2, before adding oxygen, the conver-
sion of CH4 was 65.1% and the conversion of CO2 was 87.1%,
and H2 /CO molar ratio was 0.95 or so. When 0.4 molar ratio Figure 2. The effect of different added amount of oxygen on the catalytic per-
(based on CO2 ) oxygen was added, CH4 conversion increased formances of combined reforming on 10wt%Ni/SBA-15 catalyst. Reaction
rapidly from 65.1% to 86.3%. CH4 conversion increased with conditions: GHSV = 24000 ml·g−1 −1 ◦
cat ·h ; T = 800 C; CH4 : CO2 : O2 = 2 : 1:
increasing the amount of oxygen and reached 99.1% when the X; catalyst 0.2 g
molar ratio of oxygen added was 1.0. Different from CH4
conversion, CO2 conversion had no obvious change when the
molar ratio of oxygen added was smaller than 0.6. However, 3.2. The ef fect of the added dif ferent amount of steam on the
when the molar ratio of oxygen added was higher than 0.6, it catalytic performances
decreased rapidly. When the molar ratio of oxygen added was
1.0, CO2 conversion dropped from 87.1% to 66.0%, suggest- The effect of the added amount of steam on the catalytic
ing that added oxygen could promote the conversion of CH4 , performances of combined reforming on 10wt%Ni/SBA-15
but had a contrary effect on the conversion of CO2 . catalyst with the molar ratio of CH4 : CO2 : O2 = 2 : 1 : 0.6 in
Guo et al. [21] reported the combined carbon dioxide and the feed gas was also investigated. Figure 3 shows that CH4
oxygen reforming of methane on the Ni/SiO2 catalyst. They conversion increased slowly from 90.8% to 97.4% with the in-
found that the CH4 conversion increased and CO2 conversion creasing of added steam, however, CO2 conversion decreased
decreased with the increasing of O2 /CH4 molar ratio under the sharply from 86% to 57.3% and the trend became more ob-
C/O atomic ratio of 1. Molecular O2 possesses strong oxidiz- vious with the further increasing of added steam. Huang et
ing property and will facilitate the dissociation of CH4 , result- al. [9] found that CH4 conversion increased very slowly from
ing in the increase in CH4 conversion. Meanwhile, CH4 could 97.7% to 98.9% and CO2 conversion dropped from 94.1%
be deeply oxidized to CO2 easily and the product CO could to 84% with the proportion of the added steam in the feed
also be oxidized to CO2 when there was much more oxygen, moving up from 1/9 to 4/9 while the CH4 /(CO2 +H2 O) mo-
372 Daoan Sun et al./ Journal of Natural Gas Chemistry Vol. 19 No. 4 2010

lar ratio was 2 : 2.5. The effect of added steam on the cat- tent when Ni content was lower than 10wt%, but it decreased
alytic performances was investigated by Xu et al. [12] at at- rapidly when Ni content was higher than 10wt%.
mospheric pressure when the feed composition molar ratio
of CH4 : CO2 : Air was 1.0 : 0.2 : 1.9. It was observed that
CH4 conversion increased and CO2 conversion obviously de-
creased when a few steam was added. It is reasonable since
the added steam would favor the steam reforming of methane
and unfavor the conversion of CO2 . From the point of view of
thermodynamics, CH4 can react with H2 O prior to with CO2
[23]. It indicated that the carbon dioxide reforming would be
depressed by the increasing steam. Besides, the added steam
would facilitate the water gas shift reaction, leading to the in-
crease in H2 /CO molar ratio.

Figure 3. The effect of added amount of steam on the cat-

alytic performances of combined reforming on 10wt%Ni/SBA-15 cat-
alyst. Reaction conditions: GHSV = 24000 ml·g−1 −1 ◦
cat ·h ; T = 800 C;
CH4 : CO2 : O2 : H2 O = 2 : 1 : 0.6 : Y ; catalyst 0.2 g
Figure 4. The effect of Ni contents and reaction temperature on the catalytic
performances of Ni/SBA-15 catalysts. Reaction conditions: GHSV = 24000
In conclusion, 10wt%Ni/SBA-15 catalyst shows the best ml·g−1 −1
cat ·h ; CH4 : CO2 : O2 : H2 O = 2 : 1 : 0.6 : 0.6; catalyst 0.2 g
catalytic performance for the combined reforming of the sim-
ulated biogas when the molar ratio of CH4 : CO2 : O2 : H2 O Between Figure 4(a) and 4(b), it was found that CO2 con-
in feed gas was 2 : 1 : 0.6 : 0.6 and the conversions of CH4 version was more sensitive to the change of Ni content. The
and CO2 reach 92.8% and 76.3%, respectively, as well as the conversion of CO2 was obviously lower than that of CH4 ,
H2 /CO molar ratio was about 1.35. which could be explained by the fact that Ni promoted the
dissociation of CH4 more easily than CO2 . In short, the op-
3.3. The ef fect of nickel content on the reaction performances timal Ni content was 10wt% for this reaction. As to reaction
temperature, it could be found that both CH4 and CO2 conver-
Many researchers have proven that there was an optimal sions went up rapidly with the increase of temperature ranging
threshold of active component content, which would vary by from 700 ◦ C to 800 ◦ C, but the conversion increased slowly at
a small scale with different catalyst carrier and reaction. The higher temperature.
Ni-based catalysts were a good candidate for methane reform-
ing reactions due to its low cost, rich reserves and high activity 3.4. The ef fect of space velocity on the reaction performances
[24−27].
The effect of different Ni contents in Ni-based catalyst on Figure 5 shows the effect of GVSH on the reaction per-
the catalytic performances is shown in Figure 4. According to formances during the combined reforming of the simulated
Figure 4(a), when the Ni content was lower than 10wt%, CH4 biogas to syngas. It was observed that both the CH4 and
conversion increased slightly with the increasing in Ni con- CO2 conversions declined, and the H2 /CO molar ratio of the
tent. However, there was no obvious change in CH4 conver- product increased with the increase of GHSV. CH4 conver-
sion when Ni content was higher than 10wt% and even some- sion decreased from 94.3% to 90.0% and CO2 conversion de-
what lower than the catalytic activity of 10wt%Ni/SBA-15 creased from 82.4% to 71.4% when the GHSV increased from
catalyst. Different from CH4 conversion, as is shown in Fig- 16000 ml/(g·h) to 32000 ml/(g·h). In addition, the H2 /CO mo-
ure 4(b), CO2 conversion increased with increasing in Ni con- lar ratio increased from 1.27 to 1.47. When the GHSV ex-
 Journal of Natural Gas Chemistry Vol. 19 No. 4 2010 373

ceeded 32000 ml/(g·h), there was no obvious change in these of SBA-15, which avoided the aggregation of nickel particles
three parameters. Besides, H2 and CO yields kept invariant impregnated into the mesoporous SBA-15. 10wt%Ni/SBA-15
with the increase of GHSV, and H2 yield and CO yield main- exhibited a good stability for the combined reforming of the
tained at 81.0% and 99.0%, respectively. simulated biogas to syngas in the present case, which might
Zhou et al. [28] found that CH4 conversion decreased be ascribed to the same reason as Zhang suggested [19].
with the increase of GHSV during the steam reforming of
methane. It would be due to the residence time of reactants
which was shorten by the increase of GHSV. Moreover, Jing
et al. [29] also found that CH4 and CO2 conversions declined
when GHSV increased in combined partial oxidation and car-
bon dioxide reforming of methane. It indicated that contact
time between the reactants and catalyst reduced with the in-
crease of GHSV. So, the adsorption and activation of reactant
molecule decreased. Meanwhile, the real temperature of the
catalyst bed will be lowered since more reactants will enter the
reactor with a higher GHSV. This also leads to a decrease in
the CH4 and CO2 conversions. However, the decrease in real
temperature of the catalyst bed will favor for the water gas
shift reaction. It resulted in the increase of the H2 /CO molar
ratio.

Figure 5. The effect of GHSV on the reaction perfor-

mances of 10wt%Ni/SBA-15 catalyst. Reaction conditions:
CH4 : CO2 : O2 : H2 O = 2 : 1 : 0.6 : 0.6; T = 800 ◦ C; catalyst 0.2 g

Figure 6. The stability of 10wt%Ni/SBA-15 catalyst. Reaction conditions:

3.5. The stability of 10wt%Ni/SBA-15 catalyst T = 800 ◦ C; GHSV = 24000 ml·g−1 −1
cat ·h ; CH4 :CO2 :O2 :H2 O = 2:1:0.6:0.6;
catalyst 0.2 g
The stability of 10wt%Ni/SBA-15 catalyst for the com-
bined reforming of the simulated biogas to syngas was exam-
ined and the results are shown in Figure 6. At the initial re- 4. Conclusions
action stage, CH4 conversion reached 92.8%, CO2 conversion
was about 76.3% and the H2 /CO molar ratio was around 1.35. Ni-based SBA-15 catalysts were prepared by the impreg-
After reacting at 800 ◦ C for 100 h, both CH4 conversion and nation method and showed good catalytic performances for
CO2 conversion decreased only about 5%. However, no sig- the combined reforming of the simulated biogas to syngas.
nificant change could be observed for the H2 /CO molar ratio. Oxygen added in the feed could promote the conversion of
In addition, H2 and CO yields still kept above 82% and 91%, CH4 , but inhibit the conversion of CO2 . Besides, the H2 /CO
respectively. This indicated that the catalyst had an excellent molar ratio of the product increased markedly when oxygen
activity and stability at high temperature. Zhang et al. [19] was added, however, only a slight increase in the H2 /CO mo-
studied the activity and stability of Ni/SBA-15 catalyst for the lar ratio was found with a further increasing the amount of
carbon dioxide reforming of methane. It was reported that the added oxygen. The optimal molar ratio of oxygen added was
12.5wt%Ni/SBA-15 catalyst showed highly stable activity at 0.6, and the conversions of CH4 and CO2 could reach 90.8%
800 ◦ C for 600 h and it was ascribed to the porous structure and 86.0%, respectively. Moreover, CH4 conversion increased
374 Daoan Sun et al./ Journal of Natural Gas Chemistry Vol. 19 No. 4 2010

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