期刊
NATURE CHEMISTRY
卷 10, 期 7, 页码 763-769出版社
NATURE PORTFOLIO
DOI: 10.1038/s41557-018-0054-3
关键词
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资金
- Arnold and Mabel Beckman Foundation Young Investigator Award
- CAREER award from the National Science Foundation [NSF CHE-1455011]
- Division Of Chemistry [1455011] Funding Source: National Science Foundation
Multi-electron redox reactions, although central to artificial photosynthesis, are kinetically sluggish. Amidst the search for synthetic catalysts for such processes, plasmonic nanoparticles have been found to catalyse multi-electron reduction of CO2 under visible light. This example motivates the need for a general, insight-driven framework for plasmonic catalysis of such multielectron chemistry. Here, we elucidate the principles underlying the extraction of multiple redox equivalents from a plasmonic photocatalyst. We measure the kinetics of electron harvesting from a gold nanoparticle photocatalyst as a function of photon flux. Our measurements, supported by theoretical modelling, reveal a regime where two-electron transfer from the excited gold nanoparticle becomes prevalent. Multiple electron harvesting becomes possible under continuous-wave, visible-light excitation of moderate intensity due to strong interband transitions in gold and electron-hole separation accomplished using a hole scavenger. These insights will help expand the utility of plasmonic photocatalysis beyond CO2 reduction to other challenging multi-electron, multi-proton transformations such as N-2 fixation.
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