期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 53, 期 30, 页码 7887-7891出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201404259
关键词
electron transfer; photoelectrochemistry; solar energy conversion; surface plasmon resonance; water splitting
资金
- NSF [CHE-1038015]
- CCI Center for Nanostructured Electronic Materials
- ORAU
- Sigma Xi
- University of Florida
- U.S. Department of Energy, Office of Basic Energy Sciences [BNL-CFN-31913, DE-AC01-98CH10886]
Ideal solar-to-fuel photocatalysts must effectively harvest sunlight to generate significant quantities of long-lived charge carriers necessary for chemical reactions. Here we demonstrate the merits of augmenting traditional photoelectrochemical cells with plasmonic nanoparticles to satisfy these daunting photocatalytic requirements. Electrochemical techniques were employed to elucidate the mechanics of plasmon-mediated electron transfer within Au/TiO2 heterostructures under visible-light (lambda > 515 nm) irradiation in solution. Significantly, we discovered that these transferred electrons displayed excited-state lifetimes two orders of magnitude longer than those of electrons photogenerated directly within TiO2 via UV excitation. These long-lived electrons further enable visible-light-driven H-2 evolution from water, heralding a new photocatalytic paradigm for solar energy conversion.
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