Amino‐Functionalized Interfacial Layer Enables an Ultra‐Uniform Amorphous Solid Electrolyte Interphase for High‐Performance Aqueous Zinc‐Based Batteries

Abstract Aqueous rechargeable zinc‐based batteries (ZBBs) are emerging as desirable energy storage systems because of their high capacity, low cost, and inherent safety. However, the further application of ZBBs still faces many challenges, such as the issues of uncontrolled dendrite growth and severe parasitic reactions occurring at the Zn anode. Herein, an amino‐grafted bacterial cellulose (NBC) film is prepared as artificial solid electrolyte interphase (SEI) for the Zn metal anodes, which can significantly reduce zinc nucleation overpotential and lead to the dendrite‐free deposition of Zn metal along the (002) crystal plane more easily without any external stimulus. More importantly, the chelation between the modified amino groups and zinc ions can promote the formation of an ultra‐even amorphous SEI upon cycling, reducing the activity of hydrate ions, and inhibiting the water‐induced side reactions. As a result, the Zn||Zn symmetric cell with NBC film exhibits lower overpotential and higher cyclic stability. When coupled with the V 2 O 5 cathode, the practical pouch cell achieves superior electrochemical performance over 1000 cycles.