Carbon deposition and catalytic deactivation during CO2 reforming of CH4 over Co/γ-Al2O3 catalysts

被引:278
作者
Ruckenstein, E [1 ]
Wang, HY [1 ]
机构
[1] SUNY Buffalo, Dept Chem Engn, Amherst, NY 14260 USA
关键词
carbon dioxide reforming of methane; synthesis gas; Co catalyst; deactivation;
D O I
10.1006/jcat.2001.3458
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The reaction behavior and carbon deposition during the CO2/CH4 reforming reaction have been investigated over the gamma-Al2O3-supported Co catalysts as a function of Co loading (between 2 and 20 wt%) and calcination temperature (T-c = 500 or 1000degreesC). It was found that the stability of Co/gamma-Al2O3 catalysts was strongly dependent on the Co loading and calcination temperature. For some loadings (6 wt% for T-c = 500degreesC and 9 wt% for T-c = 1000degreesC), stable activities have been achieved. However, over the catalysts with high Co loadings (>12 wt%), notable amounts of carbon were accumulated during reforming, and deactivation was observed. Moreover, severe deactivation was also noted over the 2 wt% catalysts, both when carbon deposition occurred (T-c = 500degreesC) or was absent (T-c = 1000degreesC). In the latter case, the oxidation of the metallic sites was responsible for the deactivation. Hence, there are two different deactivation mechanisms, namely, carbon deposition and oxidation of metallic sites. The activities were stable when a balance between carbon formation and its oxidation could be achieved. (C) 2002 Elsevier Science.
引用
收藏
页码:289 / 293
页数:5
相关论文
共 39 条
[1]   PARTIAL OXIDATION OF METHANE TO SYNTHESIS GAS-USING CARBON-DIOXIDE [J].
ASHCROFT, AT ;
CHEETHAM, AK ;
GREEN, MLH ;
VERNON, PDF .
NATURE, 1991, 352 (6332) :225-226
[2]   Potential of zeolite supported rhodium catalysts for the CO2 reforming of CH4 [J].
Bhat, RN ;
Sachtler, WMH .
APPLIED CATALYSIS A-GENERAL, 1997, 150 (02) :279-296
[3]   Mono and bifunctional pathways of CO2/CH4 reforming over Pt and Rh based catalysts [J].
Bitter, JH ;
Seshan, K ;
Lercher, JA .
JOURNAL OF CATALYSIS, 1998, 176 (01) :93-101
[4]   Deactivation and coke accumulation during CO2/CH4 reforming over Pt catalysts [J].
Bitter, JH ;
Seshan, K ;
Lercher, JA .
JOURNAL OF CATALYSIS, 1999, 183 (02) :336-343
[5]   Promoting effect of Pt, Pd and Rh noble metals to the Ni0.03Mg0.97O solid solution catalysts for the reforming of CH4 with CO2 [J].
Chen, YG ;
Tomishige, K ;
Yokoyama, K ;
Fujimoto, K .
APPLIED CATALYSIS A-GENERAL, 1997, 165 (1-2) :335-347
[6]   Catalytic performance and catalyst structure of nickel-magnesia catalysts for CO2 reforming of methane [J].
Chen, YG ;
Tomishige, K ;
Yokoyama, K ;
Fujimoto, K .
JOURNAL OF CATALYSIS, 1999, 184 (02) :479-490
[7]   ACTIVATION OF CH4 AND ITS REACTION WITH CO2 OVER SUPPORTED RH CATALYSTS [J].
ERDOHELYI, A ;
CSERENYI, J ;
SOLYMOSI, F .
JOURNAL OF CATALYSIS, 1993, 141 (01) :287-299
[8]   THE ROLE OF CATALYST SUPPORT ON THE ACTIVITY OF NICKEL FOR REFORMING METHANE WITH CO2 [J].
GADALLA, AM ;
BOWER, B .
CHEMICAL ENGINEERING SCIENCE, 1988, 43 (11) :3049-3062
[9]   Isotopic study of the reaction of methane with the lattice oxygen of a NiO/MgO solid solution [J].
Hu, YH ;
Ruckenstein, E .
CATALYSIS LETTERS, 1999, 57 (04) :167-169
[10]   An optimum NiO content in the CO2 reforming of CH4 with NiO/MgO solid solution catalysts [J].
Hu, YH ;
Ruckenstein, E .
CATALYSIS LETTERS, 1996, 36 (3-4) :145-149