Competitive oxidation and reduction of aliphatic alcohols over (wo3)3 clusters
Journal of Physical Chemistry C, ISSN: 1932-7447, Vol: 113, Issue: 22, Page: 9721-9730
2009
- 47Citations
- 18Captures
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Article Description
The reactions of C1-C4 aliphatic alcohols over (WO ) clusters were studied experimentally and theoretically using temperature-programmed desorption, infrared reflection-absorption spectroscopy, and density functional theory. The results reveal that all C1-C4 aliphatic alcohols readily react with (WO ) clusters by heterolytic cleavage of the RO-H bond to give alkoxy (RO-) bound to W(VI) centers and a proton (H ) attached to the terminal oxygen atom of a tungstyl group (WdO). Two protons adsorbed onto the cluster readily react with the doubly bonded oxygen to from a water molecule that desorbs at 200-300 K and the alkoxy that undergoes decomposition at higher temperatures into the corresponding alkene, aldehyde, and/or ether. Our theory predicts that all three channels proceed over the W(VI) Lewis acid sites with energy barriers of 30-40 kcal/mol, where dehydration is favored over the others. We also present further analysis of the yield and reaction temperature as a function of the alkyl substituents and discuss the origin of the reaction selectivity among the three reaction channels. © 2009 American Chemical Society.
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