Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 20, Issue 16, Pages 4646-4652Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201304837
Keywords
alloys; gold; mixed sites; oxidative coupling; silver
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Funding
- U.S. Department of Energy, Basic Energy Sciences [FG02-84-ER13289]
- National Science Foundation, Division of Chemistry, Analytical and Surface Science [CHE-0952790]
- Harvard University Center for the Environment through the Graduate Consortium in Energy and the Environment
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Nanoporous gold, a dilute alloy of Ag in Au, activates molecular oxygen and promotes the oxygen-assisted catalytic coupling of methanol. Because this trace amount of Ag inherent to nanoporous gold has been proposed as the source of oxygen activation, a thin film Ag/Au alloy surface was studied as a model system for probing the origin of this reactivity. Thin alloy layers of AgxAu1-x, with 0.15x0.40, were examined for dioxygen activation and methanol self-coupling. These alloy surfaces recombine atomic oxygen at different temperatures depending on the alloy composition. Total conversion of methanol to selective oxidation products, that is, formaldehyde and methyl formate, was achieved at low initial oxygen coverage and at low temperature. Reaction channels for methyl formate formation occurred on both Au and Au/Ag mixed sites with a ratio, as was predicted from the local 2-dimensional composition.
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