Production of hydrogen from methanol over Cu/ZnO catalysts promoted by ZrO2 and Al2O3

被引:388
作者
Agrell, J [1 ]
Birgersson, H
Boutonnet, M
Melián-Cabrera, I
Navarro, RM
Fierro, JLG
机构
[1] KTH, Royal Inst Technol, SE-10044 Stockholm, Sweden
[2] CSIC, Inst Catalisis & Petroleoquim, E-28049 Madrid, Spain
关键词
fuel cell; methanol steam reforming; methanol oxidation (partial); Cu/ZnO/ZrO2/Al2O3; catalyst; characterization; N2O chemsorption; TPR/TPC; XPS;
D O I
10.1016/s0021-9517(03)00221-5
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
Production of H-2 from methanol by steam reforming, partial oxidation, or a combination thereof was studied over Cu/ZnO-based catalysts. The catalysts were characterized by a variety of techniques, including N2O chemisorption, X-ray photoelectron spectroscopy, X-ray diffraction, and temperature-programmed reduction/oxidation. The influence of feed composition, reaction temperature, and catalyst formulation on H-2 production rate, product distribution, and catalyst lifetime was investigated. Distinct differences between the processes were observed with respect to catalyst behavior. ZrO2-containing catalysts, especially Cu/ZnO/ZrO2/Al2O3, exhibit the best performance in the steam reforming reaction. During partial oxidation, however, a binary Cu/ZnO catalyst exhibits the lowest light-off temperature and the lowest level of CO by-product. The redox properties of the catalyst appear to play a key role in determining the pathway for H-2 production. In particular. the extent of methanol and/or H-2 combustion at differential O-2 conversion is strongly dependent on the ease of copper oxidation in the catalyst. (C) 2003 Elsevier Inc. All rights reserved.
引用
收藏
页码:389 / 403
页数:15
相关论文
共 60 条
[1]   Steam reforming of methanol over a Cu/ZnO/Al2O3 catalyst:: a kinetic analysis and strategies for suppression of CO formation [J].
Agrell, J ;
Birgersson, H ;
Boutonnet, M .
JOURNAL OF POWER SOURCES, 2002, 106 (1-2) :249-257
[2]   Production of hydrogen by partial oxidation of methanol over Cu/ZnO catalysts prepared by microemulsion technique [J].
Agrell, J ;
Hasselbo, K ;
Jansson, K ;
Järås, SG ;
Boutonnet, M .
APPLIED CATALYSIS A-GENERAL, 2001, 211 (02) :239-250
[3]  
AGRELL J, 2002, CATALYSIS SPECIALIST, V16, P67
[4]   Partial oxidation of methanol to produce hydrogen over Cu-Zn-based catalysts [J].
Alejo, L ;
Lago, R ;
Pena, MA ;
Fierro, JLG .
APPLIED CATALYSIS A-GENERAL, 1997, 162 (1-2) :281-297
[5]   HYDROGEN-PRODUCTION BY STEAM REFORMING OF METHANOL FOR POLYMER ELECTROLYTE FUEL-CELLS [J].
AMPHLETT, JC ;
CREBER, KAM ;
DAVIS, JM ;
MANN, RF ;
PEPPLEY, BA ;
STOKES, DM .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 1994, 19 (02) :131-137
[6]   On board hydrogen purification for steam reformation PEM fuel cell vehicle power plants [J].
Amphlett, JC ;
Mann, RF ;
Peppley, BA .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 1996, 21 (08) :673-678
[7]   HYDROGEN-PRODUCTION BY THE CATALYTIC STEAM REFORMING OF METHANOL .2. KINETICS OF METHANOL DECOMPOSITION USING GIRDLER G66B CATALYST [J].
AMPHLETT, JC ;
EVANS, MJ ;
MANN, RF ;
WEIR, RD .
CANADIAN JOURNAL OF CHEMICAL ENGINEERING, 1985, 63 (04) :605-611
[8]  
Appleby A.J., 1989, FUEL CELL HDB
[9]   KINETICS OF CATALYTIC CONVERSION OF METHANOL AT HIGHER PRESSURES [J].
BARTON, J ;
POUR, V .
COLLECTION OF CZECHOSLOVAK CHEMICAL COMMUNICATIONS, 1980, 45 (12) :3402-3407
[10]   Methanol reforming for fuel-cell applications: development of zirconia-containing Cu-Zn-Al catalysts [J].
Breen, JP ;
Ross, JRH .
CATALYSIS TODAY, 1999, 51 (3-4) :521-533