Reactivity of the gold/water interface during selective oxidation catalysis

Bhushan N. Zope, David D. Hibbitts, Matthew Neurock, Robert J. Davis

Research output: Contribution to journalArticlepeer-review

655 Scopus citations

Abstract

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 18O2 and H218O 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.

Original languageEnglish (US)
Pages (from-to)74-78
Number of pages5
JournalScience
Volume330
Issue number6000
DOIs
StatePublished - Oct 1 2010

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