In situ UV-Vis diffuse reflectance spectroscopy -: on line activity measurements of supported chromium oxide catalysts:: relating isobutane dehydrogenation activity with Cr-speciation via experimental design

被引:81
作者
Weckhuysen, BM
Verberckmoes, AA
Debaere, J
Ooms, K
Langhans, I
Schoonheydt, RA
机构
[1] Katholieke Univ Leuven, Dept Interfasechem, Ctr Oppervlaktechem Katalyse, B-3001 Heverlee, Belgium
[2] Katholieke Univ Leuven, CQ Consultancy, B-3001 Heverlee, Belgium
关键词
in situ spectroscopy; diffuse reflectance spectroscopy; supported chromium oxide catalysts; experimental design; chemometrics;
D O I
10.1016/S1381-1169(99)00259-9
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 dehydrogenation of isobutane over supported chromium oxide catalysts was studied by a combination of in situ UV-Vis diffuse reflectance spectroscopy and on line GC analysis. A well-defined set of experiments, based on an experimental design, was carried out to develop mathematical models, which quantitatively relate Cr-speciation and dehydrogenation activity with reaction temperature and time, support composition, gas composition and Cr loading. It will be shown that: (1) the dehydrogenation activity is proportional with the amount of in situ measured surface Cr2+/3+, and maximum for a 7.5 wt.% Cr/Al2O3 catalyst operating at 500 degrees C in 2% isobutane in N-2; and (2) Cr3+-sites are more active in alkane dehydrogenation than Cr2+-sites. This paper is the first example of the use of experimental design for deriving structure-activity relationships in the field of heterogeneous catalysis. (C) 2000 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:115 / 131
页数:17
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