Aqueous zinc batteries are attracting interest because of their potential for cost-effective and safe electricity storage. However, metallic zinc exhibits only moderate reversibility in aqueous electrolytes. To circumvent this issue, we study aqueous Zn batteries able to form nanometric interphases at the Zn metal/liquid electrolyte interface, composed of an ion-oligomer complex. In Zn||Zn symmetric cell studies, we report highly reversible cycling at high current densities and capacities (e.g., 160 mA cm-2; 2.6 mAh cm-2). By means of quartz-crystal microbalance, nuclear magnetic resonance, and voltammetry measurements we show that the interphase film exists in a dynamic equilibrium with oligomers dissolved in the electrolyte. The interphase strategy is applied to aqueous Zn||I2 and Zn||MnO2 cells that are charged/discharged for 12,000 cycles and 1000 cycles, respectively, at a current density of 160 mA cm-2 and capacity of approximately 0.85 mAh cm-2. Finally, we demonstrate that Zn||I2-carbon pouch cells (9 cm2 area) cycle stably and deliver a specific energy of 151 Wh/kg (based on the total mass of active materials in the electrode) at a charge current density of 56 mA cm-2.
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