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

The dehydrogenation of isobutane over supported chromium oxide catalysts wa s studied by a combination of in situ UV-Vis diffuse reflectance spectrosco py 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 react ion temperature and time, support composition, gas composition and Cr loadi ng. 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+-site s. This paper is the first example of the use of experimental design for de riving structure-activity relationships in the field of heterogeneous catal ysis. (C) 2000 Elsevier Science B.V. All rights reserved.