Preparation, characterization, and catalytic activity of chromia supported on SBA-15 for the oxidative dehydrogenation of isobutane
Mesoporous SBA-15 and 1–12 wt% CrOx/SBA-15 have been prepared by triblock copolymer P123-templated hydrothermal synthesis and incipient wetness impregnation method, respectively. The materials were characterized by means of a number of analytical techniques and their catalytic activities were evaluated for the oxidative dehydrogenation (ODH) of isobutane. It is found that with rise of chromia loading, the morphology of SBA-15 changed from long interconnected chains to short banana-like rods, and finally changed to spheres with wormholes. The results of Raman and X-ray photoelectron spectroscopic investigations reveal that the surface Cr species are mainly Cr6+ in mono- and polychromate, with a minor amount of Cr3+ due to α-Cr2O3 formation. The H2 temperature-programmed reduction study demonstrates that the catalysts at chromia loading of 6–10 wt% are more reducible. The 10 wt% CrOx/SBA-15 catalyst exhibits the best activity, showing 79% C4-olefin selectivity and 11% C4-olefin yield at 540 °C. One monolayer CrOx coverage on SBA-15 occurs at Cr surface density = 1.05–1.43 Cr-atom/nm2. We conclude that factors such as (i) presence of active Cr6+ in mono- and polychromate, (ii) strong redox ability of Cr species, and (iii) good dispersion of CrOx on banana-like rods of well-ordered mesoporous SBA-15 are responsible for the good performance of the SBA-15-supported chromia in isobutane ODH.
Graphical abstractLoaded chromia exists in mono- and polychromate forms on SBA-15 surfaces. Isobutane interacts with the lattice oxygen of CrOx/SAB-15 to generate isobutanoxide adspecies that decompose to give isobutene, and the reduced catalyst is re-oxidized by gas-phase oxygen. The well-dispersed CrOx and its strong redox ability account for the excellent catalytic performance of the SBA-15-supported chromia.Figure optionsDownload full-size imageDownload as PowerPoint slide
Journal: Applied Catalysis A: General - Volume 355, Issues 1–2, 28 February 2009, Pages 192–201