Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 29, Pages 9073-9077Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201803214
Keywords
cocatalysts; hydrogen evolution; nanosheets; photocatalysis; water splitting
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Funding
- Japan Society for the Promotion of Science (JSPS) KAKENHI [15H01993, 16H06293, 17H05484]
- ENEOS Hydrogen Trust Fund
- International Institute for Carbon Neutral Energy Research
- World Premier International Research Center Initiative (WPI), MEXT, Japan
- U.S. National Science Foundation under PIRE Grant [1545907]
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The hydrogen evolution reaction using semiconductor photocatalysts has been significantly improved by cocatalyst loading. However, there are still many speculations regarding the actual role of the cocatalyst. Now a photocatalytic hydrogen evolution reaction pathway is reported on a cocatalyst site using TiO2 nanosheets doped with Rh at Ti sites as one-atom cocatalysts. A hydride species adsorbed on the one-atom Rh dopant cocatalyst site was confirmed experimentally as the intermediate state for hydrogen evolution, which was consistent with the results of density functional theory (DFT) calculations. In this system, the role of the cocatalyst in photocatalytic hydrogen evolution is related to the withdrawal of photo-excited electrons and stabilization of the hydride intermediate species; the presence of oxygen vacancies induced by Rh facilitate the withdrawal of electrons and stabilization of the hydride.
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