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
[1]   THEORETICAL-STUDY OF THE THERMOCHEMISTRY OF MOLECULES IN THE SI-C-H SYSTEM [J].
ALLENDORF, MD ;
MELIUS, CF .
JOURNAL OF PHYSICAL CHEMISTRY, 1992, 96 (01) :428-437
[2]   WIDE TEMPERATURE-RANGE IR SPECTROSCOPY CELL FOR STUDIES OF ADSORPTION AND DESORPTION ON HIGH AREA SOLIDS [J].
BASU, P ;
BALLINGER, TH ;
YATES, JT .
REVIEW OF SCIENTIFIC INSTRUMENTS, 1988, 59 (08) :1321-1327
[3]   HYDROGEN SPILLOVER ON ALUMINA - A STUDY BY INFRARED-SPECTROSCOPY [J].
CAVANAGH, RR ;
YATES, JT .
JOURNAL OF CATALYSIS, 1981, 68 (01) :22-26
[4]   INFRARED STUDIES OF THE MECHANISM OF METHANOL DECOMPOSITION ON CU/SIO2 [J].
CLARKE, DB ;
LEE, DK ;
SANDOVAL, MJ ;
BELL, AT .
JOURNAL OF CATALYSIS, 1994, 150 (01) :81-93
[5]  
CONNER WC, 1986, ADV CATAL, V34, P1
[6]   AN INFRARED SPECTROSCOPIC STUDY OF THE ADSORPTION OF CARBON-MONOXIDE ON SILICA-SUPPORTED COPPER PARTICLES [J].
DEJONG, KP ;
GEUS, JW ;
JOZIASSE, J .
APPLIED SURFACE SCIENCE, 1980, 6 (3-4) :273-287
[7]  
DRIESSEN MD, IN PRESS J PHYS CHEM
[8]   INFRARED STUDY OF THE OXIDATION OF HEXAFLUOROPROPENE ON TIO2 [J].
FAN, JF ;
YATES, JT .
JOURNAL OF PHYSICAL CHEMISTRY, 1994, 98 (41) :10621-10627
[9]   SURFACE NITRIDE FORMATION ON SUPPORTED COPPER-CATALYSTS AND ITS INTERACTION WITH CO [J].
HIGGS, V ;
PRITCHARD, J .
APPLIED CATALYSIS, 1986, 25 (1-2) :149-156
[10]   THEORETICAL-STUDY OF THE THERMOCHEMISTRY OF MOLECULES IN THE SI-O-H-C SYSTEM [J].
HO, P ;
MELIUS, CF .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (07) :2166-2176