Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 131, Issue 20, Pages 7086-7093Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja810045y
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Funding
- MEXT [18064017]
- CREST program
- Japan Society for the Promotion of Science for Young Scientists
- Grants-in-Aid for Scientific Research [18064017] Funding Source: KAKEN
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Au clusters smaller than 1.5 nm and stabilized by poly(N-vinyl-2-pyrrolidone) (PVP) showed higher activity for aerobic oxidation of alcohol than those of larger size or stabilized by poly(allylamine) (PAA). X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy of adsorbed CO, and X-ray absorption near edge structure measurements revealed that the catalytically active Au clusters are negatively charged by electron donation from PVP, and the catalytic activity is enhanced with increasing electron density on the Au core. Based on similar observations of Au cluster anions in the gas phase, we propose that electron transfer from the anionic Au cores of Au:PVP into the LUMO (pi*) of O-2 generates superoxoor peroxo-like species, which plays a key role in the oxidation of alcohol. On the basis of these results, a simple principle is presented for the synthesis of Au oxidation catalysts stabilized by organic molecules.
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