Role of support in CO2 reforming of CH4 over a Ni/γ-Al2O3 catalyst

被引:73
作者
Cheng, ZX [1 ]
Zhao, XG [1 ]
Li, JL [1 ]
Zhu, QM [1 ]
机构
[1] Tsinghua Univ, Dept Chem, State Key Lab C1 Chem Technol, Beijing 100084, Peoples R China
关键词
carbon dioxide; methane; reforming; nickel catalyst; hydrogen spillover; mechanism;
D O I
10.1016/S0926-860X(00)00560-3
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
A catalyst of 10% Ni/gamma -Al2O3 for CO2/CH4 reforming was prepared and characterized by TPR. TPD. XPS, XRD and activity measurements. XPS and TPR showed that Ni mainly exists in the form of NiAl2O4 in the calcined catalyst and is hard to reduce below 650 degreesC, indicating a strong interaction between metal and support. Reduction of the calcined catalyst results in fine particles of Ni-0. with an average diameter of about 20 nm as determined by XRD. The uptake of H on the reduced catalyst measured by H-2-TPD is 4.2-4.6 mole per mole of Ni species and does not depend on the reduction degree of Ni species. This provides a convincing piece of evidence for the occurrence of hydrogen spillover in the reduced catalyst. Only reduced catalysts present good activity, but the degree of nickel reduction has almost no effect on the reforming activity. This seems to suggest that Ni-0 is vital for the reforming activity, but gamma -Al2O3 is also involved in CO2/CH4 reforming and contributes even more. Based on the mechanism proposed by Bradford et al. and on our observations, a mechanistic model has been proposed to elucidate the role of gamma -Al2O3 in CO2/CH4 reforming. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:31 / 36
页数:6
相关论文
共 31 条
[2]   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
[3]   HYDROGENATION OF ETHYLENE ON ALUMINA AFTER HYDROGEN SPILLOVER [J].
BIANCHI, D ;
GARDES, GEE ;
PAJONK, GM ;
TEICHNER, SJ .
JOURNAL OF CATALYSIS, 1975, 38 (1-3) :135-146
[4]   CO2 reforming of CH4 [J].
Bradford, MCJ ;
Vannice, MA .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1999, 41 (01) :1-42
[5]  
Cevallos-Candau J.F., 1987, J CATAL, V106, p[378, 90249]
[6]   HYDROGENATION OF ORGANIC OXYGENATES ON NI/AL2O3 AND NI/SIO2 CATALYSTS [J].
CHEN, BS ;
FALCONER, JL .
JOURNAL OF CATALYSIS, 1994, 147 (01) :72-81
[7]  
CHIARANUSSATI P, 1993, CHEM ENG RES DES, V71, P267
[8]  
CONNER WC, 1986, ADV CATAL, V34, P1
[9]   SPILLOVER IN HETEROGENEOUS CATALYSIS [J].
CONNER, WC ;
FALCONER, JL .
CHEMICAL REVIEWS, 1995, 95 (03) :759-788
[10]  
DELMON B, 1992, APPL CATAL B-ENVIRON, V1, P1395