Fast Reaction Kinetics and Commendable Low‐Temperature Adaptability of Zinc Batteries Enabled by Aprotic Water‐Acetamide Symbiotic Solvation Sheath

Abstract Although rechargeable aqueous zinc batteries are cost effectiveness, intrinsicly safe, and high activity, they are also known for bringing rampant hydrogen evolution reaction and corrosion. While eutectic electrolytes can effectively eliminate these issues, its high viscosity severely reduces the mobility of Zn 2+ ions and exhibits poor temperature adaptability. Here, we infuse acetamide molecules with Lewis base and hydrogen bond donors into a solvated shell of Zn(H 2 O) 6 2+ to create Zn(H 2 O) 3 (ace)(BF 4 ) 2 . The viscosity of 1ace‐1H 2 O is 0.032 Pa s, significantly lower than that of 1ace‐0H 2 O (995.6 Pa s), which improves ionic conductivity (9.56 mS cm −1 ) and shows lower freezing point of −45 °C, as opposed to 1ace‐0H 2 O of 4.04 mS cm −1 and 12 °C, respectively. The acidity of 1ace‐1H 2 O is ≈2.8, higher than 0ace‐1H 2 O at ≈0.76, making side reactions less likely. Furthermore, benefiting from the ZnCO 3 /ZnF 2 ‐rich organic/inorganic solid electrolyte interface, the Zn || Zn cells cycle more than 1300 hours at 1 mA cm −2 , and the Zn || Cu operated over 1800 cycles with an average Coulomb efficiency of ≈99.8 %. The Zn || PANI cell cycled over 8500 cycles, with a specific capacity of 99.8 mAh g −1 at 5 A g −1 at room temperature, and operated at −40 °C with a capacity of 66.8 mAh g −1 .