期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 62, 期 18, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202218859
关键词
Artificial Photosynthesis; Heterobimetallic Cooperation; Nickel-Iron Molecular Catalyst; O-O Bond Formation; Water Oxidation
We reported here the development of a heterobimetallic NiFe molecular platform to investigate the synergistic effect of NiFe in water oxidation catalysis. Compared to homonuclear bimetallic compounds (NiNi and FeFe), the NiFe complex exhibited significant catalytic activity in water oxidation. Mechanistic studies showed that this enhanced activity is attributed to the effective promotion of O-O bond formation by NiFe synergy. The formation of Ni-III(mu-O)Fe-IV=O intermediate is the key step for O-O bond formation through intramolecular oxyl-oxo coupling between bridged O radical and terminal Fe-IV=O moiety.
We reported herein the development of heterobimetallic NiFe molecular platform to understand NiFe synergistic effect in water oxidation catalysis. Compared to homonuclear bimetallic compounds (NiNi and FeFe), NiFe complex possesses more remarkable catalytic water oxidation performance. Mechanistic studies suggest that this remarkable difference is attributed to the fact that NiFe synergy can effectively promote O-O bond formation. The generated Ni-III(mu-O)Fe-IV=O is the key intermediate and O-O bond was formed via intramolecular oxyl-oxo coupling between bridged O radical and terminal Fe-IV=O moiety.
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