Dendrite‐Free Zn Anodes via Synergistic Cosolvent‐Mediated Solvation Regulation and Polyhydroxy‐Induced Interface Stabilization

ABSTRACT Aqueous zinc‐ion batteries (AZIBs), well known for their inherent safety, resource abundance, and low cost, hold broad application prospects in the energy storage field. However, issues such as zinc dendrite growth, severe hydrogen evolution reactions, and corrosion by‐products impede their extensive application and commercialization. Herein, we propose a “dual regulation” electrolyte strategy employing a green co‐solvent and a low‐cost additive to construct a stable zinc anode. Specifically, 1,2‐propanediol (PG) is introduced as a co‐solvent to reconstruct the Zn 2 + solvation structure. It could effectively break the original hydrogen‐bond network of water molecules, thereby fundamentally suppressing hydrogen evolution and enhancing the anti‐freezing performance of the electrolyte. Furthermore, the addition of D‐sorbitol (DS) as an additive induces the preferential deposition of Zn 2 + on the (002) crystal plane, which improves the interfacial stability of the zinc electrode. As a result, the Zn//Zn symmetric cell demonstrates exceptional 3300 h long‐term cycling stability, and the Zn//Cu half cell exhibits a high Coulombic efficiency of 99.74% over 1400 cycles. Notably, even at −20°C and under a current density of 1 A g −1 , the capacity retention rate of Zn//PANI full cell achieved 81.5% after 1500 cycles. This study presents a “two‐pronged” strategy, providing a promising approach for designing water‐based high‐performance electrolytes and advancing the development of safe, low‐cost, and durable AZIBs.