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.