Engineering Robust Electrode‐Electrolyte Interface by Adhesive Gel Polymer Electrolytes for CO ₂ ‐Tolerant Flexible Zinc‐Air Batteries

ABSTRACT As an emerging energy storage device, flexible zinc‐air batteries (FZABs) have garnered significant attention due to their high energy density, low cost, and environmental friendliness. However, FZABs, being a special type of semi‐open system, suffer from CO ₂ corrosion in strongly alkaline electrolyte environments, which leads to rapid degradation of battery performance and severely hinders the widespread application of FZABs. Herein, a novel polycationic backbone was constructed via free radical copolymerization of acrylamide (AM) and 3‐(methacryloylamino)propyltrimethylammonium chloride (MAPTAC). By incorporating gelatin, a highly viscous and strongly adhesive MPTA‐G gel polymer electrolyte (GPEs) was developed. The optimal MPTA‐G0.15 GPE achieves an ionic conductivity as high as 282 mS cm ⁻¹ and can effectively inhibit the growth of zinc dendrites. Moreover, the FZAB based on the MPTA‐G0.15 GPE shows excellent electrochemical performance and favorable tolerance to CO ₂ . Consequently, the synthesis of highly viscous and adhesive GPEs based on a gelatin‐reinforced strategy paves the way for developing FZABs with superior interfacial stability and CO ₂ resistance in strongly alkaline electrolytes.