Trace Triazole Enables Kinetic-Controlled Zn Deposition via Adsorptive Interface Regulation for Highly Reversible Zinc Metal Anodes

Despite the inherent advantages of aqueous zinc-ion batteries (AZIBs), such as low cost, facile assembly, and high safety enabled by aqueous electrolytes, the severe parasitic reactions induced by active water molecules at the Zn anode interface critically compromise the cycling stability and practical applications. Herein, the trace multifunctional additive 1H-1,2,3-Triazole (Trl) was introduced into the electrolyte to reconfigure the interfacial environment for highly reversible Zn anodes. Density functional theory (DFT) calculations and experimental analyses reveal that Trl exhibits a stronger adsorption preference on Zn anodes, forming an aqueous-depleted electric double layer (EDL) that effectively suppresses water-induced side reactions. Crucially, comparative analysis of Zn 2+ binding energies demonstrates that trace Trl cannot disrupt the [Zn(H 2 O) 6 ] 2+ solvation structure in bulk electrolytes, while within the Trl-regulated EDL, it accelerates Zn 2+ desolvation and diffusion relaxation, thereby promoting orderly Zn 2+ diffusion and uniform deposition. This multimodal regulation shifts the Zn deposition mechanism from diffusion-controlled to kinetic-controlled. Consequently, Zn||Zn symmetric cells achieve ultralong cycling stability for over 5000 h at 3 mA cm –2 and 1 mAh cm –2, and the Coulombic Efficiency is remarkably improved to 99.75%. Full cells paired with NH 4 V 4 O 10 cathodes also demonstrate enhanced electrochemical performance, significantly outperforming their additive-free counterparts.