Abstract

Rechargeable aqueous zinc-manganese dioxide (Zn-MnO2) batteries have gained significant attention in the field of energy storage systems owing to their cost-effectiveness, environmental friendliness, power, and ability to mitigate thermal propagation. However, Zn- MnO2 batteries encounter challenges and limitations, including capacity degradation and voltage hysteresis by the dissolution of Mn ions in the bulk electrolyte. In this study, interfacial stabilization is improved by promoting the decomposition of the 1,3-propane sultone (PS) electrolyte additive, which occurs close to the oxidation decomposition at 1.5 V. This facilitates the formation of a stable cathode–electrolyte interphase (CEI) and effectively suppresses Mn-ion dissolution. Density functional theory (DFT) simulations provide insights into the formation of a CEI layer product structure during cell operation, resulting in the thermodynamically reduced dissolution of Mn (Mn2+) into the electrolyte when a sulfur-based decomposed layer covers MnO2. Consequently, the cathode protection layer ensures high cycle retention, Coulombic efficiency, and high C-rate cell operating conditions for the Zn-MnO2 battery cell. This work presents a promising strategy for designing electrolytes to develop high-performance aqueous zinc-ion batteries.

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