Spin‐State Reconfiguration and Lattice Oxygen Activation Co‐Mediated Oxygen Evolution Catalysis Pathway via Artificial Hetero‐Sites for Rechargeable Zn–Air Batteries

Abstract It is desirable but challenging to develop low‐cost and high‐performance electrocatalysts for the oxygen evolution reaction (OER) in zinc–air batteries (ZABs) applications. In this work, a series of cerium oxide‐coated cobalt vanadium oxide nanoplates (denoted as CVO@CeO 2 ) are prepared using different CeO 2 loadings through a facile two‐step method. Compared to bare CVO, CeO 2, and commercial RuO 2 , the CVO@CeO 2 ‐0.20 catalyst presents much higher activity toward OER in alkaline solutions. Moreover, the CVO@CeO 2 ‐0.20 also exhibits superior open‐circuit voltage and durability when utilized as the cathode in ZABs. Both theoretical calculations and experimental results disclose that the decoration of CeO 2 on CVO not only regulates the formation of high‐spin state Co 3+ , optimizing the absorbate evolution mechanism (AEM) pathway, but also activates lattice oxygen, enhancing the lattice oxide oxidation mechanism (LOM) pathway. This research presents the CVO@CeO 2 heterojunction as an excellent catalyst for the OER and proposes a promising interface‐regulated strategy for developing catalysts based on the reinforcement of AEM and LOM mechanisms.