Dual‐Function Electrolyte Additive via Molecular Spatial Shielding and Solvation Regulation Enables Highly Reversible Zn Anode

Abstract The practical application of aqueous Zn‐ion batteries (AZIBs) is limited by uncontrollable dendrite growth at the Zn anode interface and parasitic reactions induced by moisture. A novel molecular anchoring strategy is proposed, which involves incorporating N‐hydroxysuccinimide (NHS) as a multifunctional electrolyte additive to regulate Zn 2+ deposition and stabilize the electrode–electrolyte interface. The rigid five‐membered ring structure of NHS, together with its carbonyl (C═O) and N‐hydroxyl (N─OH) functional groups, enables strong and orderly adsorption on the Zn surface, creating a spatial shielding and solvation regulation. This effect not only homogenizes the electric field and ion current to achieve dendrite‐free zinc deposition but also effectively blocks water molecules from contacting the negative electrode, thereby suppressing hydrogen evolution and corrosion. The NHS‐containing electrolyte demonstrates exceptional performance, with a cycle life of 4200 h at 1 mA cm −2 /1 mAh cm −2 and a Coulombic efficiency of 99.83%. Furthermore, the fabricated Zn||NH 4 V 4 O 10 full cells exhibit excellent cycling stability, retaining 80% of their initial capacity after 1000 extended cycles at 5 A·g −1 . This work elucidates the synergistic mechanism through which NHS optimizes the electrolyte environment and regulates interfacial chemistry, thereby providing a scientific basis for the development of more efficient and stable AZIBs.