Abstract Aqueous zinc‐ion batteries (AZIBs) hold great potential in grid energy storage systems, whereas the non‐uniform Zn 2+ transport within traditional expensive glass fiber separator induces severe Zn dendrite and side reactions. Herein, the molecular aggregation state is regulated by the intermolecular hydrogen bond loosening effect to prepare a robust cellulose separator for addressing the above‐mentioned challenges. By choosing ethanol as a weakly protic regenerant, the solvent regeneration process suppresses hydrogen bond reformation and guides the supramolecular aggregation of cellulose chains into a loosely packed structure. Chromogenic experiments and molecular dynamics simulations demonstrate that the separator with aggregation state regulation facilitates the uniform Zn 2+ transport and accelerates the desolvation process. This leads to a comprehensive enhancement of Zn 2 ⁺ transference number (0.61), Zn 2 ⁺ conductivity (2.87 mS cm −1 ), Zn 2 ⁺ deposition kinetics, and suppression of Zn dendrite and side reactions. Consequently, Zn||I 2 battery demonstrates a remarkable long‐term stability (exceeding 68 000 cycles) and anti‐self‐discharge performance (96.37% capacity retention after resting for 100 h). This separator also functions well in the Zn||MnO 2 battery system under high‐loading of 10 mg cm −2 . This work presents the aggregation state regulation and scalable production of low‐cost cellulose separator to facilitate the application of AZIBs.
Li et al. (2025) studied this question.