INFLUENCE OF ALKALI PROMOTERS IN THE SELECTIVE HYDROGENATION OF 3-METHYL-2-BUTENAL OVER RU/SIO2 CATALYSTS

被引:41
作者
WAGHRAY, A [1 ]
WANG, J [1 ]
OUKACI, R [1 ]
BLACKMOND, DG [1 ]
机构
[1] UNIV PITTSBURGH,DEPT CHEM & PETR ENGN,PITTSBURGH,PA 15261
关键词
D O I
10.1021/j100193a056
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 addition of potassium as a promoter to a Ru/SiO2 catalyst resulted in a striking shift in product selectivity in the hydrogenation of 3-methyl-2-butenal. The rate of hydrogenation at the C=O bond to produce the unsaturated alcohol increased concomitant with a decrease in the rate of C=C hydrogenation. IR spectroscopy showed a strong perturbation of the C=O bond for the alkali-promoted catalyst, and volumetric chemisorption and TPD results suggested that the alkali species blocked adsorption at low-coordination Ru sites. These adsorption and reaction studies suggest that polarization of the adsorbed substrate at the C=O bond is responsible for the significant shift in product selectivity upon alkali promotion. This work combines spectroscopic tools with the use of the catalytic reaction itself as a probe of catalyst surface chemistry.
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收藏
页码:5954 / 5959
页数:6
相关论文
共 45 条
[1]   RHODIUM CARBON-MONOXIDE SURFACE-CHEMISTRY - THE INVOLVEMENT OF SURFACE HYDROXYL-GROUPS ON AL2O3 AND SIO2 SUPPORTS [J].
BASU, P ;
PANAYOTOV, D ;
YATES, JT .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1988, 110 (07) :2074-2081
[2]   CROTONALDEHYDE AND METHYLCROTONALDEHYDE HYDROGENATION OVER PT(111) AND PT80FE20(111) SINGLE-CRYSTALS [J].
BECCAT, P ;
BERTOLINI, JC ;
GAUTHIER, Y ;
MASSARDIER, J ;
RUIZ, P .
JOURNAL OF CATALYSIS, 1990, 126 (02) :451-456
[3]   CO-INDUCED DISINTEGRATION OF RHODIUM AGGREGATES SUPPORTED IN ZEOLITES - INSITU SYNTHESIS OF RHODIUM CARBONYL CLUSTERS [J].
BERGERET, G ;
GALLEZOT, P ;
GELIN, P ;
BENTAARIT, Y ;
LEFEBVRE, F ;
NACCACHE, C ;
SHANNON, RD .
JOURNAL OF CATALYSIS, 1987, 104 (02) :279-287
[4]  
Betta R. A. D., 1975, J PHYS CHEM-US, V79, P2519
[5]   GEOMETRIC AND ELECTRONIC EFFECTS IN THE SELECTIVE HYDROGENATION OF ALPHA,BETA-UNSATURATED ALDEHYDES OVER ZEOLITE-SUPPORTED METALS [J].
BLACKMOND, DG ;
OUKACI, R ;
BLANC, B ;
GALLEZOT, P .
JOURNAL OF CATALYSIS, 1991, 131 (02) :401-411
[6]   RH/AIPO4 CATALYSTS .9. LIQUID-PHASE HYDROGENATION AND ISOMERIZATION OF ALPHA,BETA-UNSATURATED ALCOHOLS [J].
CAMPELO, JM ;
GARCIA, A ;
LUNA, D ;
MARINAS, JM .
JOURNAL OF CATALYSIS, 1988, 113 (01) :172-184
[7]   INSITU CHEMICAL TRAPPING OF CO/H-2 SURFACE SPECIES [J].
CAVALCANTI, FAP ;
BLACKMOND, DG ;
OUKACI, R ;
SAYARI, A ;
ERDEM-SENATALAR, A ;
WENDER, I .
JOURNAL OF CATALYSIS, 1988, 113 (01) :1-12
[8]  
CORDIER G, 1988, Patent No. 882919
[9]   INFRARED-SPECTRA FOR CO ISOTOPES CHEMISORBED ON PT[111] - EVIDENCE FOR STRONG ABSORBATE COUPLING INTERACTIONS [J].
CROSSLEY, A ;
KING, DA .
SURFACE SCIENCE, 1977, 68 (01) :528-538
[10]   POTASSIUM PROMOTED C-O BOND WEAKENING ON RU(001) .1. THROUGH-METAL INTERACTION AT LOW POTASSIUM PRECOVERAGE [J].
DEPAOLA, RA ;
HRBEK, J ;
HOFFMANN, FM .
JOURNAL OF CHEMICAL PHYSICS, 1985, 82 (05) :2484-2498