Constructing Atomically Dispersed Bimetallic Electrocatalyst by a Topologically Confined Pre‐Anchoring Strategy for Enhanced Oxygen Reduction Reaction and Zn‐Air Battery

The development of atomically dispersed multi‐metallic catalysts is imperative for tailoring catalytic performance and elucidating structure–activity relationships. However, synthesizing such precisely engineered architectures while maintaining atomic dispersion of distinct metal centers remains a formidable challenge due to thermodynamic instability and synthetic complexity. We herein propose a topological confinement pre‐anchoring strategy via pre‐anchoring spatially resolved Zn/Fe dual‐metal sources in a structurally engineered metal–organic framework precursor to synthesize atomically dispersed ZnFe bimetallic single‐atom catalysts. Extended X‐ray absorption fine structure measurements and X‐ray absorption near‐edge structure reveal that the atomically dispersed Zn/Fe metal sites and electronic redistribution in ZnFe bimetallic single‐atom catalysts. The ultrahigh surface area, hierarchical pore, and synergistic effect between Zn/Fe can greatly favor the exposure of the active site, mass transport, and improvement of intrinsic activity. Consequently, the ZnFe bimetallic single‐atom catalyst demonstrates superior oxygen reduction reaction performance, achieving a half‐wave potential of 0.86 V and delivering a kinetic current density of 10.1 mA cm −2 at 0.85 V versus RHE in 0.1 m KOH electrolyte. These metrics not only surpass those of commercial Pt/C, but also rival the highest‐performing catalysts reported to date. The Zn‐air battery built with ZnFe bimetallic single‐atom catalyst exhibits high power density (278.5 mW cm −2 ) and specific discharging capacities (657 mAh g −1 ). This work provides a new design pathway for constructing atomically dispersed multi‐metal electrocatalysts for high‐performance energy‐related applications.