MICROKINETIC ANALYSIS OF DIVERSE EXPERIMENTAL-DATA FOR ETHYLENE HYDROGENATION ON PLATINUM

被引:111
作者
REKOSKE, JE [1 ]
CORTRIGHT, RD [1 ]
GODDARD, SA [1 ]
SHARMA, SB [1 ]
DUMESIC, JA [1 ]
机构
[1] UNIV WISCONSIN,DEPT CHEM ENGN,MADISON,WI 53706
关键词
D O I
10.1021/j100183a067
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
Kinetic analysis employing a mechanism that captures the essential surface chemistry of the reaction allows quantitative interpretation of diverse experimental data. This approach is used with a Horiuti-Polanyi mechanism, modified by hydrogen activation steps, to describe the surface chemistry for ethylene hydrogenation over platinum catalysts. In this investigation, kinetic analysis provides a quantitative means of comparing, contrasting, and consolidating results from steady-state kinetic studies, deuterium tracing measurements, vibrational spectroscopy, and temperature programmed desorption. A noncompetitive pathway is dominant at low temperatures, involving sites for hydrogen adsorption that are not blocked by carbonaceous species. At higher temperatures and lower ethylene pressures, more surface sites become available for hydrogen adsorption, and the reaction shifts to a pathway involving competitive hydrogen and ethylene adsorption.
引用
收藏
页码:1880 / 1888
页数:9
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