Single (002)-Textured Zinc Anode via Nonepitaxial Electrodeposition with <i>In Situ</i> Texture Maintenance for Stable Aqueous Zinc Batteries

Crystallography regulation of a zinc (Zn) metal substrate to expose more (002) textures holds great promise for stabilizing Zn anodes. However, significant challenges remain in directly constructing a single (002)-plane-textured Zn metal anode (S-(002)-Zn) and realizing a sustainable (002)-texture exposure in working batteries. Herein, we report an anion and cation coregulated nonepitaxial electrodeposition to fabricate S-(002)-Zn by introducing 1-ethyl-3-methylimidazolium iodide (EmimI) additives in low-cost ZnSO₄ aqueous electrolyte (ZS). Mechanistic studies reveal that the cooperation of Emim⁺ and I^- with oriented adsorption behaviors on Zn can synergistically boost the (100) plane growth, depress the (002) plane growth, and suppress H₂ evolution, thus enabling compact S-(002)-Zn electrodeposition. Moreover, other similar organic iodides (e.g., dimethyl-imidazolium iodide and 1-propyl-3-methylimidazolium iodide) are applicable to this scalable electrodeposition. On the other hand, the as-designed ZS-EmimI electrolyte can be directly applied in working Zn batteries, thus effectively sustaining the smooth (002) texture of S-(002)-Zn and inhibiting HER during cycling. Consequently, the combination of single-(002)-texture and ZS-EmimI electrolyte endows the S-(002)-Zn anode with an ultralong lifespan over 10,100 h (>14 months) at 1 mAh cm^-2 and superior deep-cycling stability under 88.0% utilization (25 mAh cm^-2) over 500 h and assures the stable operation of full Zn batteries.