Dual-descriptor-guided electrolyte additive screening strategy for achieving highly reversible aqueous zinc-ion batteries

Organic solvent additives are widely employed in aqueous zinc-ion batteries (AZIBs) to achieve high coulombic efficiency (CE), regulate oriented zinc deposition, and stabilize interfacial chemistry. However, conventional screening strategies rely primarily on bulk molecular electronic behavior, often overlooking the interfacial energetics that govern additive-electrode interactions. Herein, using density functional theory calculations, we introduce a dual-descriptor framework based on the molecular electrostatic potential minimum (ESP min ) and the molecule-electrode surface free energy ( γ ). This approach effectively incorporates solvent behavior and interfacial structural stability, establishing clear screening criteria for high-CE electrolytes. By analyzing 319 literature-reported organic solvents, including 29 additives with established experimental CE, we demonstrate that the high-CE region (> 99.5%) falls into a specific energetic window of ESP min > –2.0 eV and γ < –0.015 eV·Å –2 . Furthermore, molecular dynamics (MD) simulations reveal that candidates matching these criteria, such as the experimentally validated chloroacetamide (CTA) and 1,4-butanediol (BDO), reconfigure the Zn 2+ primary solvation sheath to deplete active water at the electrode interface, thereby enabling highly reversible and uniform zinc plating. Ultimately, this work establishes a direct correlation between intrinsic molecular properties and interfacial characteristics, offering a screening methodology that can be readily extended to other advanced battery systems.