期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 57, 期 12, 页码 3207-3211出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201712678
关键词
diiron complexes; iron; oxidation; photochemistry; reaction mechanisms
资金
- COST association action ECOSTBio (STSM) [CM1305, 38503]
- European Research Council [ERC 279549]
- Labex ARCANE [ANR-11-LABX-003]
- Serbian Ministry of Science [OI172035]
- Chinese Scholarship Council (CSC)
- Center for Information Technology of the University of Groningen
Non-heme (L)Fe-III and (L)Fe-III-O-Fe-III(L) complexes (L=1,1-di(pyridin-2-yl)-N,N-bis(pyridin-2-ylmethyl)-ethan-1-amine) underwent reduction under irradiation to the Fe-II state with concomitant oxidation of methanol to methanal, without the need for a secondary photosensitizer. Spectroscopic and DFT studies support a mechanism in which irradiation results in charge-transfer excitation of a Fe-III-mu-O-Fe-III complex to generate [(L)Fe-IV=O](2+) (observed transiently during irradiation in acetonitrile), and an equivalent of (L)Fe-II. Under aerobic conditions, irradiation accelerates reoxidation from the Fe-II to the Fe-III state with O-2, thus closing the cycle of methanol oxidation to methanal.
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