Solvation-interface coupling directs Zn(002)-oriented deposition for highly reversible zinc batteries.

Aqueous zinc batteries are promising candidates for large-scale energy storage owing to their intrinsic safety and low cost, yet their practical deployment remains hindered by parasitic interfacial reactions, unstable Zn deposition, and dendrite growth. Herein, we report a molecular-mediated elecAtrolyte strategy employing propionamide (PA) to stabilize Zn metal anodes through solvation-interface coupling regulation. PA partially replaces coordinated H2O molecules in the Zn2+ solvation sheath and simultaneously reorganizes the hydrogen-bond network, thereby reducing H2O activity and mitigating water-induced parasitic reactions. Meanwhile, PA exhibits a strong affinity toward Zn surfaces, forming a stable adsorption environment that modulates interfacial reaction kinetics. Theory calculations reveal preferential adsorption of PA on Zn facets, which promotes thermodynamically favored Zn(002)-oriented growth. Consequently, Zn deposition evolves into dense and smooth layers with a highly textured crystallographic orientation and effectively suppressed dendrite formation. Owing to this solvation-interface coupled regulation, Zn||Zn symmetric cells achieve stable cycling for over 3800 h at 1 mA cm-2 and 1 mAh cm-2, while Zn||VO2 full cells maintain highly reversible operation for more than 10,000 cycles. This work establishes solvation-interface coupling regulation as an effective electrolyte-design principle for directing Zn crystallization and stabilizing aqueous zinc batteries.