Stabilizing Interface pH by Mixing Electrolytes for High‐Performance Aqueous Zn Metal Batteries

Abstract Aqueous zinc metal batteries with mild acidic electrolytes are considered promising candidates for large‐scale energy storage. However, the Zn anode suffers from severe Zn dendrite growth and side reactions due to the unstable interfacial pH and the absence of a solid electrolyte interphase (SEI) protective layer. Herein, a novel and simple mixed electrolyte strategy is proposed to address these problems. The mixed electrolytes of 2 M ZnSO 4 and 2 M Zn (CF 3 SO 3 ) 2 can efficiently buffer the interfacial pH and induce the in situ formation of the organic‐inorganic SEI layer, which eliminates dendrite growth and prevents side reactions. As a result, Zn anodes in mixed electrolyte exhibit a lifespan enhancement over 400 times, endure stable cycling over 270 h at a high DOD of 62% and achieve high Zn plating/stripping reversibility with an average CE of 99.5% for 1000 cycles at 1 mA cm −2 . The findings pave the way for developing practical electrolyte systems for Zn batteries.