COMPLETE OXIDATION OF CARBON-MONOXIDE AND METHANE OVER METAL-PROMOTED FLUORITE OXIDE CATALYSTS

被引:87
作者
LIU, W
SAROFIM, AF
FLYTZANI-STEPHANOPOULOS, M
机构
[1] TUFTS UNIV, DEPT CHEM ENGN, MEDFORD, MA 02155 USA
[2] MIT, DEPT CHEM ENGN, CAMBRIDGE, MA 02139 USA
关键词
D O I
10.1016/S0009-2509(05)80066-1
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Cu-Ce-O binary oxide catalysts were found to have high activity for the oxidation of CO and methane by oxygen to carbon dioxide and water as well as oxidation of CO by sulfur dioxide to carbon dioxide and elemental sulfur. The catalysts were characterized by X-ray powder diffraction, X-ray photoelectron spectroscopy (XPS), and scanning transmission electron microscopy. It was found that copper in the Cu-Ce-O system existed in the form of clusters dispersed in the cerium oxide matrix and in the form of segregated agglomerates (> 10 nm). The former are present in all catalyst compositions, while the latter increased with the copper content. The dispersed copper clusters may be stabilized by diffusion of copper ions into interstitial metal ion sites of the cerium oxide lattice forming Cu+1 species in the process. Cu+1 species were identified by XPS. A synergistic reaction model is proposed to explain the enhanced catalytic activity and stability. In the model, the Cu+1 species on the copper cluster provide surface sites for CO adsorption and the cerium oxide provides the oxygen source. The adsorbed CO reacts with oxygen at the interface of the two materials.
引用
收藏
页码:4871 / 4888
页数:18
相关论文
共 46 条
[1]   ACTIVITY AND STRUCTURAL-CHANGES OF ALUMINA-SUPPORTED CUO AND CUCR2O4 CATALYSTS DURING CARBON-MONOXIDE OXIDATION IN THE PRESENCE OF WATER [J].
AGUDO, AL ;
PALACIOS, JM ;
FIERRO, JLG ;
LAINE, J ;
SEVERINO, F .
APPLIED CATALYSIS A-GENERAL, 1992, 91 (01) :43-55
[2]  
BAKER RTK, 1986, STRONG METAL SUPPORT
[3]   PREPARATION AND CHARACTERIZATION OF COPPER-THORIUM OXIDE CATALYSTS .1. SOLID-SOLUTION OF COPPER(II) IN THORIA - AN ESR STUDY [J].
BECHARA, R ;
WROBEL, G ;
AISSI, CF ;
GUELTON, M ;
BONNELLE, JP ;
ABOUKAIS, A .
CHEMISTRY OF MATERIALS, 1990, 2 (05) :518-522
[4]   PREPARATION AND CHARACTERIZATION OF COPPER THORIUM-OXIDE CATALYSTS .2. ESR STUDY OF COPPER(II) ION-PAIRS AND CORRELATION WITH THE SELECTIVE HYDROGENATION OF ISOPRENE [J].
BECHARA, R ;
DHUYSSER, A ;
AISSI, CF ;
GUELTON, M ;
BONNELLE, JP ;
ABOUKAIS, A .
CHEMISTRY OF MATERIALS, 1990, 2 (05) :522-526
[5]  
BELL AT, 1987, CATALYST DESIGN PROG, P103
[6]  
BOULAHOUACHE A, 1990, APPL CATAL A-GEN, V9, P115
[7]   STRONG METAL-SUPPORT INTERACTIONS IN NICKEL/TITANIA CATALYSTS - THE IMPORTANCE OF INTERFACIAL PHENOMENA [J].
BURCH, R ;
FLAMBARD, AR .
JOURNAL OF CATALYSIS, 1982, 78 (02) :389-405
[8]   DOPANT ION RADIUS AND IONIC-CONDUCTIVITY IN CERIUM DIOXIDE [J].
BUTLER, V ;
CATLOW, CRA ;
FENDER, BEF ;
HARDING, JH .
SOLID STATE IONICS, 1983, 8 (02) :109-113
[9]   CO OXIDATION OVER PD AND CU CATALYSTS .4. PREREDUCED AL2O3-SUPPORTED COPPER [J].
CHOI, KI ;
VANNICE, MA .
JOURNAL OF CATALYSIS, 1991, 131 (01) :22-35
[10]   AN INFRARED STUDY OF THE INTERACTIONS OF CO AND CO2 WITH CU/SIO2 [J].
CLARKE, DB ;
SUZUKI, I ;
BELL, AT .
JOURNAL OF CATALYSIS, 1993, 142 (01) :27-36