期刊
INORGANIC CHEMISTRY
卷 57, 期 1, 页码 486-494出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.7b02758
关键词
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资金
- UNC EFRC: Center for Solar Fuels, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0001011]
- Grants-in-Aid for Scientific Research [16K17891] Funding Source: KAKEN
Described herein is a photochemical approach to the generation of a high-valent metal-oxo species that utilizes a chromophore or sensitizer, a semiconducting electron acceptor, and a redox buffer that poises a catalyst's initial protonation and oxidation state. The photoexcited sensitizer injects an electron into the semiconductor and then oxidizes the catalyst whose reactivity occurs in kinetic competition with back electron transfer. Core shell SnO2/TiO2 semiconductor nanocrystallites inhibited charge recombination relative to TiO2 acceptors. With low sensitizer catalyst surface coverages, a novel trapping process is exploited that enables catalysis reactivity to be quantified on time scales ranging from nanoseconds to minutes. A proof-of-principle example provides the demonstration of a light-initiated, (1e(-), 2H(+))-transfer reaction, with an inverse Ru(IV) oxo species.
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