A CuO-CeO2 mixed-oxide catalyst for CO clean-up by selective oxidation in hydrogen-rich mixtures

被引:134
作者
Kim, DH [1 ]
Cha, JE [1 ]
机构
[1] Kyungpook Natl Univ, Dept Chem Engn, Taegu 702701, South Korea
关键词
CO clean-up; copper-ceria catalyst; hydrogen production; CO oxidation;
D O I
10.1023/A:1022671327794
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 CuO-CeO2 mixed-oxide catalyst was shown experimentally to be highly active and selective for the oxidation of CO in hydrogen-rich mixtures, and an attractive alternative to the noble metal catalysts presently used for CO clean-up in hydrogen mixtures for proton-exchange membrane fuel cells (PEMFC). Although the presence of H2O and CO2 in the feed decreased the activity and increased the reaction temperature considerably to achieve a given CO conversion with a reactor, the selectivity profile with respect to the conversion remained virtually the same. The effect of H2O and CO2 on the reaction was found to increase the required energy for reduction of the active copper species in the redox cycles undergone during the reaction. The catalyst showed a slow, reversible deactivation, but the activity was restored on heating the catalyst at 300 degreesC, even under an inert flow. At space velocities above 42 g h m(-3), the catalyst reduced the CO content to less than 10 ppm in the temperature range 166-176 degreesC for a feed of 1% CO, 1% O-2, 50% H-2, 20% H2O, 13.5% CO2 and balance He. Hence, with this catalyst it is feasible to clean up the CO in a single-stage reactor with relatively small excess oxygen, which is in contrast to the typical multistage reactor systems using noble metal catalysts.
引用
收藏
页码:107 / 112
页数:6
相关论文
共 32 条
[1]   CuO-CeO2 mixed oxide catalysts for the selective oxidation of carbon monoxide in excess hydrogen [J].
Avgouropoulos, G ;
Ioannides, T ;
Matralis, HK ;
Batista, J ;
Hocevar, S .
CATALYSIS LETTERS, 2001, 73 (01) :33-40
[2]   A comparative study of Pt/γ-Al2O3, Au/α-Fe2O3 and CuO-CeO2 catalysts for the selective oxidation of carbon monoxide in excess hydrogen [J].
Avgouropoulos, G ;
Ioannides, T ;
Papadopoulou, C ;
Batista, J ;
Hocevar, S ;
Matralis, HK .
CATALYSIS TODAY, 2002, 75 (1-4) :157-167
[3]   Promoting effect of CeO2 in a Cu/CeO2 catalyst:: lowering of redox potentials of Cu species in the CeO2 matrix [J].
Bera, P ;
Mitra, S ;
Sampath, S ;
Hegde, MS .
CHEMICAL COMMUNICATIONS, 2001, (10) :927-928
[4]   ADSORPTION OF WATER ON POLYCRYSTALLINE COPPER - RELEVANCE TO THE WATER GAS SHIFT REACTION [J].
COLBOURN, E ;
HADDEN, RA ;
VANDERVELL, HD ;
WAUGH, KC ;
WEBB, G .
JOURNAL OF CATALYSIS, 1991, 130 (02) :514-527
[5]   A carbon monoxide PROX reactor for PEM fuel cell automotive application [J].
Dudfield, CD ;
Chen, R ;
Adcock, PL .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2001, 26 (07) :763-775
[6]   On-board hydrogen generation for transport applications:: the HotSpot™ methanol processor [J].
Edwards, N ;
Ellis, SR ;
Frost, JC ;
Golunski, SE ;
van Keulen, ANJ ;
Lindewald, NG ;
Reinkingh, JG .
JOURNAL OF POWER SOURCES, 1998, 71 (1-2) :123-128
[7]   A study of the activated decomposition of CO2 on the Cu component of a Cu/ZnO/Al2O3 catalyst [J].
Elliott, AJ ;
Watson, MJ ;
Tabatabaei, J ;
Zemichael, FW ;
Waugh, KC .
CATALYSIS LETTERS, 2002, 79 (1-4) :1-6
[8]  
Farrauto R.J., 1997, FUNDAMENTALS IND CAT
[9]   Study of the reducibility of copper in CuO-ZnO catalysts by temperature-programmed reduction [J].
Fierro, G ;
LoJacono, M ;
Inversi, M ;
Porta, P ;
Cioci, F ;
Lavecchia, R .
APPLIED CATALYSIS A-GENERAL, 1996, 137 (02) :327-348
[10]  
Fogler H.S., 1999, ELEMENTS CHEM REACTI