Design of Bridging‐Oxygen‐Modulated Fe–Ni Dual‐Atom Sites With Multifaceted Stabilization for Durable Cathode Catalysis in Rechargeable Zinc–Air Batteries

ABSTRACT Rechargeable zinc–air batteries (RZABs) require durable bifunctional oxygen electrocatalysts. However, the long‐term stability of metal‐nitrogen‐carbon atomic‐site catalysts (M–N–Cs) remains challenged by electrochemical corrosion and reactive oxygen species (ROS)‐induced damage arising from multiple degradation pathways, which collectively demand comprehensive solutions due to the “buckets effect” of instabilities. Herein, we develop a robust FeNi–N–C dual‐atom catalyst (DAC) featuring a bridging µ 2 ‐O electron modulator for long‐life RZAB catalysis, retaining 80% of its initial energy efficiency after 2800 h. Theoretical simulations and experimental evidence support multifaceted stabilization of the N/O‐coordinated vicinal Fe–Ni configuration. The µ 2 ‐O bridge improves intrinsic structural stability, decreases electron density on adjacent metal and N atoms to mitigate N‐site protonation and intermediate‐induced metal stripping, and promotes an O─O cleavage pathway that suppresses H 2 O 2 /ROS accumulation. These findings provide a coordination‐engineering strategy for designing durable M–N–C catalysts for long‐life RZABs.