Atomically Dispersed Fe Anchored on Nitrogen‐Doped Graphene as Advanced Bifunctional Electrocatalyst for Oxygen Electrode in Rechargeable Zn–Air Battery

Abstract Developing nonprecious metal oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) electrocatalysts with both high activity and stability remains a critical challenge for advanced metal–air battery. In this work, we develop a ball‐milling assisted pyrolysis strategy to fabricate atomically dispersed Fe anchored on nitrogen‐doped graphene (Fe–N–C/Gra), which precisely constructs Fe‐Nx active centers for efficient ORR/OER bifunctional catalysis. The fabricated Fe–N–C/Gra‐600 demonstrates ORR half‐wave potential of 0.862 V and OER overpotential of 1.743 V at 10 mA cm−2, surpassing commercial Pt/C benchmarks. Remarkably, under high electrolyte concentration conditions, catalyst exhibits reduced OER overpotentials due to increased electrochemical active surface area and optimized electron transfer resistance. Noteworthy, the Zn–air battery equipped with Fe–N–C/Gra‐600 as air electrode catalyst, delivers a remarkable peak power density of 430 mW cm−2, along with excellent charge–discharge cycling stability at 10 mA cm−2. The outstanding bifunctional performance originates from synergistic effects of Fe–N–C/Gra‐600, in which atomically dispersed Fe accelerates adsorption and activation of reactants due to formation of Fe–Nx species, synergistically with high conductive property of graphene substrate. This study not only demonstrates great potential of graphene‐supported Fe–N–C single‐atom catalysts for metal–air battery applications but also provides a new strategy for preparing high‐performance nonprecious metal electrocatalysts.