Fuel cell grade hydrogen from methanol on a commercial Cu/ZnO/Al2O3 catalyst

被引:175
作者
Choi, Y [1 ]
Stenger, HG [1 ]
机构
[1] Lehigh Univ, Dept Chem Engn, Bethlehem, PA 18015 USA
关键词
methanol decomposition; copper catalyst; methanol-steam reforming; reformer; fuel cell; hydrogen;
D O I
10.1016/S0926-3373(02)00054-1
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
This paper presents the results of experiments of the methanol decomposition reaction catalyzed by a commercial Cu/ZnO/Al2O3 in the absence and presence of water. Methanol decomposition of 100% in the absence of water was obtained at 290 degreesC and a space velocity of 2 cm(3)/h g cat. At these conditions, the hydrogen yield was 1.9-2.0. Water addition to the feed increased the yield of hydrogen and reduced the formation of: dimethyl ether; methyl formate and methane. The variation of the catalyst's activity and selectivity with time, temperature and feed composition was consistent with previous studies of methanol-steam reforming and water-gas shift reaction, however, this appears to be the first study over the same catalyst of methanol decomposition and methanol-steam reforming. XPS analysis of used catalyst samples and time on-stream data showed that the Cu2+ oxidation state of copper favors methanol decomposition, and we propose that the deactivation of the catalyst is mainly caused by the change in the oxidation state of copper. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:259 / 269
页数:11
相关论文
共 14 条
[1]   HYDROGEN-PRODUCTION BY THE CATALYTIC STEAM REFORMING OF METHANOL .1. THE THERMODYNAMICS [J].
AMPHLETT, JC ;
EVANS, MJ ;
JONES, RA ;
MANN, RF ;
WEIR, RD .
CANADIAN JOURNAL OF CHEMICAL ENGINEERING, 1981, 59 (06) :720-727
[2]  
Bart J. C., 1987, CATAL TODAY, V2, P1
[3]   REACTION AND XRD STUDIES ON CU BASED METHANOL DECOMPOSITION CATALYSTS - ROLE OF CONSTITUENTS AND DEVELOPMENT OF HIGH-ACTIVITY MULTICOMPONENT CATALYSTS [J].
CHENG, WH .
APPLIED CATALYSIS A-GENERAL, 1995, 130 (01) :13-30
[4]   Development of methanol decomposition catalysts for production of H2 and CO [J].
Cheng, WH .
ACCOUNTS OF CHEMICAL RESEARCH, 1999, 32 (08) :685-691
[5]   SYNTHESIS OF METHANOL .1. CATALYSTS AND KINETICS [J].
CHINCHEN, GC ;
DENNY, PJ ;
JENNINGS, JR ;
SPENCER, MS ;
WAUGH, KC .
APPLIED CATALYSIS, 1988, 36 (1-2) :1-65
[6]   A mechanistic study of methanol decomposition over Cu/SiO2, ZrO2/SiO2, and Cu/ZrO2/SiO2 [J].
Fisher, IA ;
Bell, AT .
JOURNAL OF CATALYSIS, 1999, 184 (02) :357-376
[7]   Kinetic modeling of the production of hydrogen from the methanol-steam reforming process over Mn-promoted coprecipitated Cu-Al catalyst [J].
Idem, RO ;
Bakhshi, NN .
CHEMICAL ENGINEERING SCIENCE, 1996, 51 (14) :3697-3708
[8]   KINETIC-STUDY OF STEAM REFORMING OF METHANOL OVER COPPER-BASED CATALYSTS [J].
JIANG, CJ ;
TRIMM, DL ;
WAINWRIGHT, MS ;
CANT, NW .
APPLIED CATALYSIS A-GENERAL, 1993, 93 (02) :245-255
[9]   CATALYTIC SYNTHESIS OF METHANOL FROM CO/H2 .4. THE EFFECTS OF CARBON-DIOXIDE [J].
KLIER, K ;
CHATIKAVANIJ, V ;
HERMAN, RG ;
SIMMONS, GW .
JOURNAL OF CATALYSIS, 1982, 74 (02) :343-360
[10]   METHANOL SYNTHESIS [J].
KLIER, K .
ADVANCES IN CATALYSIS, 1982, 31 :243-313