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Abstract Cellulose separators for aqueous zinc‐ion batteries face challenges at high‐rate conditions owing to the inherent limitations of slow Zn 2 ⁺ diffusion due to extensive intermolecular hydrogen bonding, and interfacial instability from excessive water activity. Herein, an interface‐engineered tandem chemistry is proposed by integrating chitosan‐trimesoyl chloride (CS‐TMC) layer on a bacterial cellulose separator. The inner CS cross‐linked with cellulose, rich in zincophilic ─OH groups, enhances the wettability, electrolyte uptake rate, and rapid transportation of Zn 2+ through the bulk separator. Simultaneously, the outer grafted TMC with hydrophobic groups such as benzene rings and acyl chlorides can assist to facilitate desolvation of hydrated Zn 2+ and suppress the interfacial side reactions by reducing the amount of active water. Consequently, Zn||Zn symmetrical cells with CS‐TMC separator deliver long lifespan over 4500 cycles at a high current density of 40 mA cm −2 , surpassing most reported cellulose‐based separators. Moreover, the CS‐TMC separator can also protect vanadium oxide cathode from dissolution, which can render 270 mAh g −1 at 10 A g −1 with 98.2% capacity retention after 10 000 cycles, highlighting the promising potential of the tandem chemistry design for cellulose separator in practical applications.
Miao et al. (Thu,) studied this question.