Comprehensive H2O Molecules Regulation via Deep Eutectic Solvents for Ultra‐Stable Zinc Metal Anode

Abstract: The corrosion, parasitic reactions, and aggravated dendrite growth severely restrict development of aqueous Zn-ion batteries. Here, we report a novel strategy to break the hydrogen bond network between water molecules and construct the sulfolane−H2O deep eutectic solvents. This strategy cuts off the transfer of protons/hydroxides and inhibits the activity of H2O, as reflected in a much lower freezing point (< −80 °C), a significantly larger electrochemical stable window (> 3 V), and suppressed evaporative water from electrolytes. Stable Zn plating/stripping for over 9600 h was obtained. Based on experimental characterizations and theoretical simulations, it has been proved that sulfolane can effectively regulate solvation shell and simultaneously build the multifunctional Zn−electrolyte interface. Moreover, the multi-layer homemade modular cell and 1.32 Ah pouch cell further confirm its prospect for practical application.