SPECTROSCOPIC EVIDENCE FOR METHYL SPILLOVER ON SILICA-SUPPORTED COPPER-CATALYSTS

被引:4
作者
DRIESSEN, MD [1 ]
GRASSIAN, VH [1 ]
机构
[1] UNIV IOWA, DEPT CHEM, IOWA CITY, IA 52242 USA
关键词
D O I
10.1021/la00011a009
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Fourier transform infrared spectroscopy has been used to investigate the bonding and chemistry of methyl groups, from the dissociative adsorption of methyl iodide, adsorbed on silica-supported copper catalysts. After reaction of methyl iodide on Cu/SiO2 at room temperature, the infrared data show the presence of at least two different types of adsorbed methyl groups that differ in their thermal stability. The data suggest that methyl iodide initially dissociates on the Cu surface to form methyl groups and iodine atoms. Some of the methyl groups remain adsorbed on the copper particles whereas others migrate, or spillover, on to the nearby support where they react with SiOH to form SiOCH3. This is the first study to provide spectroscopic evidence for alkyl group spillover on an oxide-supported metal catalyst. Spillover of alkyl fragments has important implications for hydrocarbon catalysis.
引用
收藏
页码:4213 / 4216
页数:4
相关论文
共 28 条
[11]  
Inui T., 1993, STUDIES SURFACE SCI, V77
[12]   KINETICS AND ENERGETICS OF BETA-HYDRIDE ELIMINATION ON CU(100) - DETERMINING THE COPPER-ALKYL BOND-ENERGY [J].
JENKS, CJ ;
XI, M ;
YANG, MX ;
BENT, BE .
JOURNAL OF PHYSICAL CHEMISTRY, 1994, 98 (08) :2152-2157
[13]   FORMATION OF METHYL RADICALS DURING THE OXIDATIVE ADDITION OF IODOMETHANE TO A SINGLE-CRYSTAL COPPER SURFACE [J].
LIN, JL ;
BENT, BE .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1993, 115 (07) :2849-2853
[14]   IODOMETHANE DISSOCIATION ON CU(111) - BONDING AND CHEMISTRY OF ADSORBED METHYL-GROUPS [J].
LIN, JL ;
BENT, BE .
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A, 1992, 10 (04) :2202-2209
[15]   C-H VIBRATIONAL MODE-SOFTENING IN ALKYL-GROUPS BOUND TO CU(111) [J].
LIN, JL ;
BENT, BE .
CHEMICAL PHYSICS LETTERS, 1992, 194 (03) :208-212
[16]  
LIN JL, 1994, J CATAL, V146, P1
[17]  
MCGEE KC, UNPUB J CATAL
[18]   INFRARED STUDY OF THE ADSORPTION OF METHANOL ON OXIDIZED AND REDUCED CU/SIO2 CATALYSTS [J].
MILLAR, GJ ;
ROCHESTER, CH ;
WAUGH, KC .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1991, 87 (17) :2795-2804
[19]   INFRARED STUDIES OF REACTIONS ON OXIDE SURFACES .2. METHANOL ON SILICA [J].
MORROW, BA .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1974, 70 (08) :1527-1545
[20]   INFRARED SPECTROSCOPIC STUDY OF THE INTERACTION BETWEEN CARBON-MONOXIDE AND HYDROGEN ON SUPPORTED PALLADIUM [J].
PALAZOV, A ;
KADINOV, G ;
BONEV, C ;
SHOPOV, D .
JOURNAL OF CATALYSIS, 1982, 74 (01) :44-54