Journal
SCIENCE
Volume 330, Issue 6000, Pages 74-78Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1195055
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Funding
- NSF [CTS-0624608, OISE 0730277, EEC-0813570]
- U.S. Department of Energy (DOE) [DE-FG02-03ER15460]
- DOE's Office of Biological and Environmental Research at Pacific Northwest National Laboratory
- National Center for Computational Sciences at Oak Ridge National Laboratory
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The selective oxidation of alcohols in aqueous phase over supported metal catalysts is facilitated by high-pH conditions. We have studied the mechanism of ethanol and glycerol oxidation to acids over various supported gold and platinum catalysts. Labeling experiments with O-18(2) and (H2O)-O-18 demonstrate that oxygen atoms originating from hydroxide ions instead of molecular oxygen are incorporated into the alcohol during the oxidation reaction. Density functional theory calculations suggest that the reaction path involves both solution-mediated and metal-catalyzed elementary steps. Molecular oxygen is proposed to participate in the catalytic cycle not by dissociation to atomic oxygen but by regenerating hydroxide ions formed via the catalytic decomposition of a peroxide intermediate.
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