Electron Redistribution via LDH-to-DACs Coupling Enhances d-Band Regulation and Stability for Zinc-Air Battery Electrocatalysis

The limited activity and poor long-term stability of oxygen electrocatalysts remain major obstacles to the practical deployment of zinc-air batteries (ZABs). Herein, a heterostructure catalyst, FeNi-LDH@DACs, was constructed by anchoring ultrasmall FeNi layered double hydroxide (LDH) nanodots onto polyhedral FeNi dual-atomic catalysts (DACs), forming a "sesame-ball-like" architecture. This spatial arrangement enables interfacial coupling, where electron transfer from LDH to DACs modulates the d-band center of the FeNi atomic sites and adjusts the adsorption energies of oxygen intermediates. The porous carbon framework of DACs also enhances conductivity, facilitating charge transport during the oxygen evolution reaction. FeNi-LDH@DACs delivers a peak power density of 211.6 mW cm–2 and maintains cycling stability for 500 h at 10 mA cm–2 in ZABs tests. These results demonstrate that engineering heterointerfaces via electronic structure modulation can be an effective approach for improving the performance and durability of bifunctional electrocatalysts for ZABs applications.