Interface-Induced Crystallographic Orientation of Zinc Deposition Enabled by a Zwitterionic Dynamic Buffering Interface for Ultralong-Life Aqueous Zinc Batteries

Abstract The development of aqueous zinc batteries is critically constrained by the electrode–electrolyte interfacial instability at the Zn anode. Herein, a zwitterionic dynamic buffering interface (ZDBI) is constructed by using trace glufosinate ammonium (GA). The dissociated GA– anchors onto the Zn(101) surface via its phosphinate and carboxylate groups with its protonated amino group (−NH3+) extending into the electrolyte to dynamically respond to interfacial electric fields. Meanwhile, free NH4+ cations can form an electrostatic shielding layer under an electric field. This synergistic chemisorbed-mobile-ion buffering network thickens the electric double layer, inhibits water-splitting parasitic reactions, and induces (101)-oriented deposition. Consequently, Zn||Zn symmetric cells sustain stable cycling for over 7800 h with a cumulative capacity of 3.9 Ah cm–2, while Zn||Cu half-cells achieve an average Coulombic efficiency of 99.3%, and Zn||V2O5 full cells retain 88% capacity after 1000 cycles at 5 A g–1. This work offers an efficient strategy for addressing electrode–electrolyte interfacial issues.