Chelation and Interfacial Engineering for Long‐Term Cycling and Self‐Healing Aqueous Zinc Batteries

Abstract Aqueous zinc‐ion batteries (AZIBs) are promising for grid‐scale energy storage but suffer from Zn anode instability caused by dendrite growth, hydrogen evolution, and corrosion. In this work, L‐carnosine (L‐C), a natural dipeptide, is introduced as an electrolyte additive to address these challenges, due to its dual ion‐chelating and Zn‐adsorbing capabilities. It is demonstrated that L‐C can regulate Zn ²⁺ solvation structures by displacing water molecules via strong coordination bonds. Simultaneously, L‐C can preferentially adsorb on Zn surfaces, guiding uniform Zn deposition along the (101) plane and forming a dynamic protective layer that dynamically repairs interfacial defects. This self‐healing capability enables short‐circuited Zn anodes to recover stable cycling for over 2000 h, while pre‐scratched surfaces are fully restored during cycling. These synergistic mechanisms enable Zn||Zn symmetric cells to achieve exceptional cycling stability (>5400 h at 1 mA cm ⁻² , 1 mAh cm ⁻² ) and high‐rate durability (>1100 h at 5 mA cm ⁻² , 5 mAh cm ⁻² ). Full cells, paired with NH ₄ V ₄ O ₁₀ (NHVO) cathodes, retain 82.26% capacity after 2000 cycles at 5 A g ⁻¹ , highlighting practical viability. The bioinspired solvation‐interfacial dual‐regulation strategy provides a universal approach for designing eco‐friendly, high‐performance AZIBs.