Active Interfacial Solvation Architecture for Highly Reversible Zinc Metal Anodes

Abstract The practical deployment of aqueous zinc-ion batteries (AZIBs) is fundamentally constrained by the uncontrolled activity of interfacial water, which triggers dendritic growth, hydrogen evolution, and corrosion. Addressing the challenge, this study presents a molecular-level strategy to actively reconstruct the interfacial hydrogen-bond network via the chemical confinement of molecular regulators within a polymer framework. Utilizing β-cyclodextrin (β-CD) and a polydopamine (PDA) framework as a model system, we demonstrate that this hybrid interface acts as a molecular sieve that reorganizes the solvation structure and disrupts continuous hydrogen-bond networks, thereby reducing local free water activity. This active solvation architecture suppresses parasitic reactions and facilitates Zn2+ desolvation, steering Zn deposition toward the thermodynamically favored (002) basal plane. The resulting anode exhibits exceptional electrochemical stability, sustaining reversible plating/stripping for over 5000 h at 1 mA cm−2. This work defines a new paradigm in interfacial engineering, shifting from passive physical protection to dynamic solvation regulation for next-generation energy storage.