Enhancing Zinc Anode Stability via Self‐Assembled Organic/Inorganic Hybrid Electrolyte Interfaces

Abstract Aqueous zinc‐ion batteries (ZIBs) are emerging as promising candidates for next‐generation energy storage systems due to their numerous advantages. However, their practical application is hindered by zinc electrode corrosion and side reactions in neutral and weakly acidic electrolytes. This study leverages the facile reductive decomposition of 2,5‐pyrroledione (Py) to in situ construct an organic/inorganic hybrid solid electrolyte interface (SEI) on the Zn anode. Characterization reveals that the Py‐interface comprises self‐assembled ZnCO 3 , Zn 4 SO 4 (OH) 6 ·H 2 O, ZnS, and polyacrylamide. This hybrid SEI exhibits strong mechanical properties, suppressing Zn dendrite formation, inhibiting Zn 4 SO 4 (OH) 6 ·H 2 O precipitation, and promoting uniform Zn 2 ⁺ deposition. Benefiting from these improvements, the Py@Zn symmetric battery demonstrates impressive cycling performance, achieving lifetimes of 2850 and 2000 h at 1 and 10 mA cm −2 , respectively. Additionally, the Py@Zn‐Cu battery exhibits enhanced cycling stability, maintaining a Coulombic efficiency of 99.7% over 2000 cycles. The Zn‐NVO battery also shows improved cycling stability due to the in situ SEI, underscoring the additive's potential in advancing Zn electrode stability and guiding future ZIB developments.