Journal
CHEMICAL SOCIETY REVIEWS
Volume 43, Issue 22, Pages 7536-7547Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3cs60420a
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- U.S. Department of Energy, Office of Basic Energy Sciences, Catalysis Science Division [DE-FG02-03ER15478]
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Advances in the fundamental understanding of alkane activation on oxide surfaces are essential for developing new catalysts that efficiently and selectively promote chemical transformations of alkanes. In this tutorial review, we discuss the current understanding of alkane activation on crystalline metal oxide surfaces, and focus mainly on summarizing our findings on alkane adsorption and C-H bond cleavage on the PdO(101) surface as determined from model ultrahigh vacuum experiments and theoretical calculations. These studies show that alkanes form strongly-bound sigma-complexes on PdO(101) by datively bonding with coordinatively-unsaturated Pd atoms and that these molecularly adsorbed species serve as precursors for C-H bond activation on the oxide surface. In addition to discussing the binding and properties of alkane sigma-complexes on PdO(101), we also summarize recent advances in kinetic models to predict alkane dissociation rates on solid surfaces. Lastly, we highlight computations which predict that the formation and facile C-H bond activation of alkane sigma-complexes also occurs on RuO2 and IrO2 surfaces.
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