Interfaces engineering of heterostructured NiCoP/NiFe LDH@CC for attaining high catalytic activity in long‐lasting rechargeable Zn–air batteries

Abstract Zinc–air batteries (ZABs) offer tremendous potential in various industries and daily life due to their excellent energy density, safety and affordability. However, the practical application of ZABs has been severely hindered by challenges such as high low round‐trip efficiencies and overpotential, primarily attributed to the inherent sluggish kinetics in the oxygen evolution reaction (OER) of air electrocatalysts. To address these issues effectively and economically, heterojunction engineering accompanied by interfacial chemistry emerges as an ideal approach to designing efficient OER electrocatalysts. Herein, a novel heterogeneous interfacial chemical structure, namely NiCoP/NiFe LDH (layered double hydroxide), needle‐like NiCoP and NiFe LDH nanosheets were assembled from cores and shells, respectively. Remarkably, the NiCoP/NiFe LDH‐based ZABs have an exceptionally long cycle life of 238 h, far superior to Pt/C + Ir/C batteries (~ 97 h). Theoretical calculations and experimental results demonstrate that NiCoP/NiFe LDH possesses tunable interfacial chemistry, demonstrating significant electronic, coordination, geometric and synergistic effects. These enhancements dramatically improve the active site density, intrinsic activity and electrochemical durability of the catalyst. In summary, this work provides a solid foundation for the development of cost‐effective OER electrocatalysts for electrochemical energy devices.