“Soggy‐Sand” Chemistry for High‐Voltage Aqueous Zinc‐Ion Batteries

• Published in: Advanced materials (Weinheim) 2024-03, Vol.36 (11), p.e2311153-n/a
• Main Authors: Deng, Rongyu, Chen, Jieshuangyang, Chu, Fulu, Qian, Mingzhi, He, Zhenjiang, Robertson, Alex W., Maier, Joachim, Wu, Feixiang
• Format: Article
• Language: English
• Subjects: Aluminum oxide; aqueous electrolyte; Aqueous electrolytes; Batteries; Chemical reactions; Electrochemical analysis; Electrolytes; Electrolytic cells; High voltages; Hydrogen bonds; Manganese dioxide; Molten salt electrolytes; oxides; Sand; soggy‐sand; Solid electrolytes; Solvation; Space charge; space charge layer; Zinc; zinc‐ion batteries
• ISSN: 0935-9648; 1521-4095
• DOI: 10.1002/adma.202311153

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.