期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 21, 期 43, 页码 15158-15162出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201502900
关键词
photocatalysis; solar fuels; transient X-ray absorption; XANES; X-ray absorption spectroscopy
资金
- Swiss National Science Foundation [200021-135226]
- European Commission [290605]
- ERC [306398]
- French National Research Agency (Labex program, ARCANE) [ANR-11-LABX-0003-01]
- Russian Foundation for Basic Research [14-02-31555]
- Ministry of Education and Science of Russia [RFMEFI58714X0002]
- Swiss National Science Foundation (SNF) [200021_135226] Funding Source: Swiss National Science Foundation (SNF)
- European Research Council (ERC) [306398] Funding Source: European Research Council (ERC)
Rational development of efficient photocatalytic systems for hydrogen production requires understanding the catalytic mechanism and detailed information about the structure of intermediates in the catalytic cycle. We demonstrate how time-resolved X-ray absorption spectroscopy in the microsecond time range can be used to identify such intermediates and to determine their local geometric structure. This method was used to obtain the solution structure of the Co-I intermediate of cobaloxime, which is a non-noble metal catalyst for solar hydrogen production from water. Distances between cobalt and the nearest ligands including two solvent molecules and displacement of the cobalt atom out of plane formed by the planar ligands have been determined. Combining in situ X-ray absorption and UV/Vis data, we demonstrate how slight modification of the catalyst structure can lead to the formation of a catalytically inactive Co-I state under similar conditions. Possible deactivation mechanisms are discussed.
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