Cu- and Ag-modified cerium oxide catalysts for methane oxidation

被引:256
作者
Kundakovic, L [1 ]
Flytzani-Stephanopoulos, M [1 ]
机构
[1] Tufts Univ, Dept Chem Engn, Medford, MA 02155 USA
关键词
cerium oxide; crystal size; reducibility; methane oxidation; silver; copper oxide;
D O I
10.1006/jcat.1998.2213
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
The catalytic activity of nanocrystalline doped ceria and Cu- and Ag-modified ceria for the complete oxidation of methane was studied in this work. The catalyst structure was studied by X-ray diffraction (XRD) and related to the availability of low-temperature oxygen species. Selected samples were also analyzed by STEM/EDX, HRTEM, and XPS. Temperature-programmed reduction (TPR) by H(2) and CH(4), as well as oxygen chemisorption, measurements were used to characterize the different oxygen species present on the catalyst. La and Zr were used as dopants to modify the crystal size and reduction properties of ceria. Enhanced activity for the complete oxidation of methane is discussed in terms of ceria reducibility, crystal size, and formation of oxygen defects at the surface (extrinsic oxygen vacancies). Addition of transition metal oxides (CuO) or transition metals (Ag) improves the low-temperature oxidation activity of cerium oxide. The interaction of ceria with Ag and CuO is a strong function of the crystal size of ceria. In the presence of the transition metal or metal oxide, a small crystal size of ceria favors the formation of highly reducible oxygen species and enhances the methane oxidation activity. (C) 1998 Academic Press.
引用
收藏
页码:203 / 221
页数:19
相关论文
共 72 条
[1]   MICROWAVE FREQUENCY BEHAVIOR OF THE EPR COPPER(II) ION-PAIRS SPECTRUM FORMED IN CUCE OXIDE [J].
ABOUKAIS, A ;
BENNANI, A ;
AISSI, CF ;
GUELTON, M ;
VEDRINE, JC .
CHEMISTRY OF MATERIALS, 1992, 4 (05) :977-979
[2]  
AMENOMIYA Y, 1988, P 9 INT C CAT CHEM I, P634
[3]   CATALYTIC OXIDATION OF METHANE [J].
ANDERSON, RB ;
STEIN, KC ;
FEENAN, JJ ;
HOFER, LJE .
INDUSTRIAL AND ENGINEERING CHEMISTRY, 1961, 53 (10) :809-812
[4]   CATALYTIC COMBUSTION OF METHANE OVER VARIOUS PEROVSKITE-TYPE OXIDES [J].
ARAI, H ;
YAMADA, T ;
EGUCHI, K ;
SEIYAMA, T .
APPLIED CATALYSIS, 1986, 26 (1-2) :265-276
[5]   AN UNUSUAL PROMOTION OF THE REDOX BEHAVIOR OF CEO2-ZRO2 SOLID-SOLUTIONS UPON SINTERING AT HIGH-TEMPERATURES [J].
BALDUCCI, G ;
FORNASIERO, P ;
DIMONTE, R ;
KASPAR, J ;
MERIANI, S ;
GRAZIANI, M .
CATALYSIS LETTERS, 1995, 33 (1-2) :193-200
[6]   CATALYTIC COMBUSTION OF METHANE OVER SUPPORTED PALLADIUM CATALYSTS .2. SUPPORT AND POSSIBLE MORPHOLOGICAL EFFECTS [J].
BALDWIN, TR ;
BURCH, R .
APPLIED CATALYSIS, 1990, 66 (02) :359-381
[7]   CATALYTIC COMBUSTION OF METHANE OVER SUPPORTED PALLADIUM CATALYSTS .1. ALUMINA SUPPORTED CATALYSTS [J].
BALDWIN, TR ;
BURCH, R .
APPLIED CATALYSIS, 1990, 66 (02) :337-358
[8]   MICROSTRUCTURAL AND CHEMICAL-PROPERTIES OF CERIA-SUPPORTED RHODIUM CATALYSTS REDUCED AT 773-K [J].
BERNAL, S ;
BOTANA, FJ ;
CALVINO, JJ ;
CAUQUI, MA ;
CIFREDO, GA ;
JOBACHO, A ;
PINTADO, JM ;
RODRIGUEZIZQUIERDO, JM .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (16) :4118-4123
[9]   HYDROGEN CHEMISORPTION ON CERIA - INFLUENCE OF THE OXIDE SURFACE-AREA AND DEGREE OF REDUCTION [J].
BERNAL, S ;
CALVINO, JJ ;
CIFREDO, GA ;
GATICA, JM ;
OMIL, JAP ;
PINTADO, JM .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1993, 89 (18) :3499-3505
[10]   A SPECTROSCOPIC CHARACTERIZATION OF THE REDUCTION OF CERIA FROM ELECTRONIC-TRANSITIONS OF INTRINSIC POINT-DEFECTS [J].
BINET, C ;
BADRI, A ;
LAVALLEY, JC .
JOURNAL OF PHYSICAL CHEMISTRY, 1994, 98 (25) :6392-6398