Zhang Hong-Tao, Guo Yu-Hua, Xiao Yao, Du Hao-Yi, Zhang Ming-Tian
Center of Basic Molecular Science (CBMS), Department of Chemistry, Tsinghua University, Beijing, 100084, China.
Institute of New Energy Technology, CHN Energy, Beijing, 102209, China.
Angew Chem Int Ed Engl. 2023 Apr 24;62(18):e202218859. doi: 10.1002/anie.202218859. Epub 2023 Mar 24.
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 (μ-O)Fe =O is the key intermediate and O-O bond was formed via intramolecular oxyl-oxo coupling between bridged O radical and terminal Fe =O moiety.
我们在此报告了用于理解水氧化催化中镍铁协同效应的异双核镍铁分子平台的开发。与同核双金属化合物（镍镍和铁铁）相比，镍铁配合物具有更显著的催化水氧化性能。机理研究表明，这种显著差异归因于镍铁协同作用可有效促进氧-氧键的形成。生成的Ni(μ-O)Fe=O是关键中间体，氧-氧键是通过桥连氧自由基与末端Fe=O部分之间的分子内氧-氧偶联形成的。
