Building electrode/electrolyte interphases in aqueous zinc batteries via self-polymerization of electrolyte additives

Abstract Aqueous zinc batteries offer promising prospects for large-scale energy storage, yet their application is limited by undesired side reactions at the electrode-electrolyte interface. Here, we report a universal approach for in situ building an electrode/electrolyte interphase (EEI) layer on both the cathode and anode through the self-polymerization of electrolyte additives. In an exemplified Zn||V2O5·nH2O cell, we reveal that the glutamate additive undergoes radical-initiated electro-polymerization on the cathode and polycondensation on the anode, yielding polyglutamic acid-dominated EEI layers on both electrodes. These EEI layers effectively mitigate undesired interfacial side reactions while enhance reaction kinetics, enabling Zn||V2O5·nH2O cell to achieve a high capacity of 387 mAh g−1 at 0.2 A g−1 and maintain over 96.3% capacity retention after 1500 cycles at 1 A g−1. Moreover, this interphase-forming additive exhibits broad applicability to varied cathode materials, encompassing VS2, VS4, VO2, α-MnO2, β-MnO2, and δ-MnO2. The methodology of utilizing self-polymerizable electrolyte additives to construct robust EEI layers opens a novel pathway of interphase engineering for electrode stabilizing in aqueous batteries.