Journal
CHEMICAL SOCIETY REVIEWS
Volume 43, Issue 22, Pages 7664-7680Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3cs60445d
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Funding
- U.S. Department of Energy Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences
- U.S. DOE by Battelle Memorial Institute [DE-AC06-76RLO 1830]
- Robert Ramsay Endowment of The University of Alabama
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Supported early transition metal oxides have important applications in numerous catalytic reactions. In this article, we review the synthesis and activity of well-defined model WO3 and MoO3 catalysts that are prepared via deposition of cyclic gas-phase (WO3)(3) and (MoO3)(3) clusters generated by sublimation of WO3 and MoO3 powders. Conversion of small aliphatic alcohols to alkenes, aldehydes/ketones, and ethers is employed to probe the structure-activity relationships on model catalysts ranging from unsupported (WO3)(3) and (MoO3)(3) clusters embedded in alcohol matrices, to (WO3)(3) clusters supported on surfaces of other oxides, and epitaxial and nanoporous WO3 films. Detailed theoretical calculations reveal the underlying reaction mechanisms and provide insight into the origin of the differences in the WO3 and MoO3 reactivity. The catalytic activity for a range of interrogated (WO3)(3) motifs (from unsupported clusters to nanoporous films) further sheds light onto the role structure and binding of (WO3)(3) clusters with the support play in determining their catalytic activity.
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