期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 19, 期 23, 页码 7480-7486出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201300579
关键词
artificial photosynthesis; photooxidation; photosynthesis; semiconductors; tantalum
资金
- Ministry of Education, Culture, Sports, Science, and Technology (MEXT) of Japan [23000009]
- Advanced Low Carbon Technology Research and Development Program (ALCA) of the Japan Science and Technology Agency (JST)
- Global Center of Excellence (GCOE) Program for Chemistry Innovation through Cooperation of Science and Engineering
- A3 Foresight Program of the Japan Society for the Promotion of Science (JSPS)
- PRESTO/JST Program
- Nippon Sheet Glass Foundation for Materials Science and Engineering
- Grants-in-Aid for Scientific Research [23000009] Funding Source: KAKEN
Tantalum nitride (Ta3N5) modified with various O2-evolution cocatalysts was employed as a photocatalyst for water oxidation under visible light (>420nm) in an attempt to construct a redox-mediator-free Z-scheme water-splitting system. Ta3N5 was prepared by nitriding Ta2O5 powder under a flow of NH3 at 10231223K. The activity of Ta3N5 for water oxidation from an aqueous AgNO3 solution as an electron acceptor without cocatalyst was dependent on the generation of a well-crystallized Ta3N5 phase with a low density of anionic defects. Modification of Ta3N5 with nanoparticulate metal oxides as cocatalysts for O2 evolution improved water-oxidation activity. Of the cocatalysts examined, cobalt oxide (CoOx) was found to be the most effective, improving the water-oxidation efficiency of Ta3N5 by six to seven times. Further modification of CoOx/Ta3N5 with metallic Ir as an electron sink allowed one to achieve Z-scheme water splitting under simulated sunlight through interparticle electron transfer without the need for a shuttle redox mediator in combination with Ru-loaded SrTiO3 doped with Rh as a H2-evolution photocatalyst.
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