Oxidation of CO in hydrogen-rich gas using a novel membrane combined with a microporous SiO2 layer and a metal-loaded γ-Al2O3 layer

被引:21
作者
Hasegawa, Y [1 ]
Ueda, A [1 ]
Kusakabe, K [1 ]
Morooka, S [1 ]
机构
[1] Kyushu Univ, Grad Sch Engn, Dept Appl Chem, Higashi Ku, Fukuoka 8128581, Japan
基金
日本学术振兴会;
关键词
reformed hydrogen fuel; CO oxidation; gamma-Al2O3; microporous silica; inorganic membrane; PEM fuel cell;
D O I
10.1016/S0926-860X(01)00854-7
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
In order to prepare metal-loaded catalyst membranes for CO oxidation, gamma-Al2O3 layers were formed on porous alpha-Al2O3 support tubes (1.7 mm i.d., 2.1 mm o.d.) using a sol-gel technique. The layers were then impregnated with Pt, Ru, Ni, Cc and Rh, using aqueous solutions of H2PtCl6, RUCl3, Ni (NO3)(2), CO(NO3)(2) and RhCl3, respectively, and calcined in air at 573 K. A gaseous mixture of H-2, CO and O-2 was permeated through these membranes, and their activities were determined with respect to CO oxidation at 423-523 K. The CO oxidation activity was the highest for the Rh/-gamma-Al2O3 membrane. Based on the report that the CO oxidation activity was much reduced for higher concentrations of CO than the threshold value, a membrane was developed by forming a microporous silica layer on the Rh/gamma-Al2O3 membrane. By the selective permeation with no feed of O-2, the CO concentration of 50,000 ppm on the feed side could be decreased to 610-2700 ppm. When O-2 was added to the feed, the CO concentration was further decreased. Thus, the composite membrane, which was developed in the present study, can play dual roles: H-2-selective permeation with a high H-2/CO separation factor, and catalytic oxidation of CO which leaked through the microporous silica layer. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:109 / 115
页数:7
相关论文
共 14 条
[1]   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
[2]   Improvement of CO tolerance of proton exchange membrane (PEM) fuel cells by a pulsing technique [J].
Carrette, LPL ;
Friedrich, KA ;
Huber, M ;
Stimming, U .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2001, 3 (03) :320-324
[3]   A compact CO selective oxidation reactor for solid polymer fuel cell powered vehicle application [J].
Dudfield, CD ;
Chen, R ;
Adcock, PL .
JOURNAL OF POWER SOURCES, 2000, 86 (1-2) :214-222
[4]  
Han J., 2000, J POWER SOURCES, V86, P223
[5]   Selective oxidation of carbon monoxide in hydrogen-rich mixtures by permeation through a platinum-loaded Y-type zeolite membrane [J].
Hasegawa, Y ;
Kusakabe, K ;
Morooka, S .
JOURNAL OF MEMBRANE SCIENCE, 2001, 190 (01) :1-8
[6]   Removal of carbon monoxide from hydrogen-rich fuels by selective oxidation over platinum catalyst supported on zeolite [J].
Igarashi, H ;
Uchida, H ;
Suzuki, M ;
Sasaki, Y ;
Watanabe, M .
APPLIED CATALYSIS A-GENERAL, 1997, 159 (1-2) :159-169
[7]   HYDROGEN ELECTROOXIDATION ON PLATINUM CATALYSTS IN THE PRESENCE OF TRACE CARBON-MONOXIDE [J].
IGARASHI, H ;
FUJINO, T ;
WATANABE, M .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1995, 391 (1-2) :119-123
[8]   Preparation of microporous silica membranes for gas separation [J].
Kim, YS ;
Kusakabe, K ;
Morooka, S ;
Yang, SM .
KOREAN JOURNAL OF CHEMICAL ENGINEERING, 2001, 18 (01) :106-112
[9]   Selective catalytic oxidation of CO in H2:: Fuel cell applications [J].
Korotkikh, O ;
Farrauto, R .
CATALYSIS TODAY, 2000, 62 (2-3) :249-254
[10]   Pore structure of silica membranes formed by a sol-gel technique using tetraethoxysilane and alkyltriethoxysilanes [J].
Kusakabe, K ;
Sakamoto, S ;
Saie, T ;
Morooka, S .
SEPARATION AND PURIFICATION TECHNOLOGY, 1999, 16 (02) :139-146