期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 137, 期 29, 页码 9324-9332出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b04062
关键词
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资金
- Ministry of Education, Culture, Sports, Science and Technology, Japan (MEXT) [26289296]
- Precursory Research for Embryonic Science and Technology (PRESTO) from Japan Science and Technology Agency (JST)
- Grants-in-Aid for Scientific Research [26289296] Funding Source: KAKEN
Aerobic oxidation on a heterogeneous catalyst driven by visible light (lambda >400 nm) at ambient temperature is a very important reaction for green organic synthesis. A metal particles/semiconductor system, driven by charge separation via an injection of hot electrons (e(hot)(-)) from photoactivated metal particles to semiconductor, is one of the promising systems. These systems, however, suffer from low quantum yields for the reaction (<5% at 550 nm) because the Schottky barrier created at the metal/semiconductor interface suppresses the e(hot)(-) injection. Some metal particle systems promote aerobic oxidation via a non-e(hot)(-)-injection mechanism, but require high reaction temperatures (>373 K). Here we report that Pt nanoparticles (similar to 5 nm diameter), when supported on semiconductor Ta2O5, promote the reaction without e(hot)(-) injection at room temperature with significantly high quantum yields (similar to 25%). Strong Pt-Ta2O5 interaction increases the electron density of the Pt particles and enhances interband transition of Pt electrons by absorbing visible light. A large number of photogenerated e(hot)(-) directly activate O-2 on the Pt surface and produce active oxygen species, thus promoting highly efficient aerobic oxidation at room temperature.
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