Heterobimetallic NiFe Cooperative Molecular Water Oxidation Catalyst

Abstract 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 ( μ ‐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.