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 Cr2qr3q, and maximum for a 7.5 wt.% CrrAl2O3 catalyst operating at 5008C in 2% isobutane in N2; and (2) Cr 3q-sites are more active in\ud alkane dehydrogenation than Cr2q-sites. This paper is the first example of the use of experimental design for deriving\ud structure–activity relationships in the field of heterogeneous catalysis
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