"Soggy-Sand" Chemistry for High-Voltage Aqueous Zinc-Ion Batteries

The narrow electrochemical stability window, deleterious side reactions, and zinc dendrites prevent the use of aqueous zinc-ion batteries. Here, aqueous "soggy-sand" electrolytes (synergistic electrolyte-insulator dispersions) are developed for achieving high-voltage Zn-ion batteries. How these electrolytes bring a unique combination of benefits, synergizing the advantages of solid and liquid electrolytes is revealed. The oxide additions adsorb water molecules and trap anions, causing a network of space charge layers with increased Zn2+ transference number and reduced interfacial resistance. They beneficially modify the hydrogen bond network and solvation structures, thereby influencing the mechanical and electrochemical properties, and causing the Mn2+ in the solution to be oxidized. As a result, the best performing Al2O3-based "soggy-sand" electrolyte exhibits a long life of 2500 h in Zn||Zn cells. Furthermore, it increases the charging cut-off voltage for Zn/MnO2 cells to 2 V, achieving higher specific capacities. Even with amass loading of 10 mgMnO2 cm-2, it yields a promising specific capacity of 189 mAh g-1 at 1 A g-1 after 500 cycles. The concept of "soggy-sand" chemistry provides a new approach to design powerful and universal electrolytes for aqueous batteries. 'Soggy-sand' electrolytes are designed for aqueous zinc-ion batteries. By acting to decrease the water molecules' reactivity, aiding in uniform zinc deposition, and capturing anions to hasten Zn2+ transport, 'soggy-sand' electrolytes address several of the core challenges faced by conventional electrolytes. This work provides a new concept for activating the electrochemical properties of aqueous rechargeable batteries.image