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  1. Abstract

    The enhanced safety, superior energy, and power density of rechargeable metal‐air batteries make them ideal energy storage systems for application in energy grids and electric vehicles. However, the absence of a cost‐effective and stable bifunctional catalyst that can replace expensive platinum (Pt)‐based catalyst to promote oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) at the air cathode hinders their broader adaptation. Here, it is demonstrated that Tin (Sn) doped β‐gallium oxide (β‐Ga2O3) in the bulk form can efficiently catalyze ORR and OER and, hence, be applied as the cathode in Zn‐air batteries. The Sn‐doped β‐Ga2O3sample with 15% Sn (Snx=0.15‐Ga2O3) displayed exceptional catalytic activity for a bulk, non‐noble metal‐based catalyst. When used as a cathode, the excellent electrocatalytic bifunctional activity of Snx=0.15‐Ga2O3leads to a prototype Zn‐air battery with a high‐power density of 138 mW cm−2and improved cycling stability compared to devices with benchmark Pt‐based cathode. The combined experimental and theoretical exploration revealed that the Lewis acid sites in β‐Ga2O3aid in regulating the electron density distribution on the Sn‐doped sites, optimize the adsorption energies of reaction intermediates, and facilitate the formation of critical reaction intermediate (O*), leading to enhanced electrocatalytic activity.

     
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