Bendable quasi-solid-state aqueous sodium-ion batteries operated at -30 °C

Aqueous sodium-ion batteries (ASIBs) have garnered considerable attention for large-scale energy storage because of inherent safety and the Na abundance. Nonetheless, the solidification of aqueous electrolytes under sub-zero conditions results in diminished ionic conductivity and increased viscosity, hindering the electrochemical performance and versatility of ASIBs. Herein, we introduce a novel freeze-tolerant ASIB using antifreezing ethylene glycol-polyacrylamide-sodium perchlorate hydrogel electrolyte, paired with new couple of Na₃MnTi(PO₄)₃ cathode and Fe-based anode. The addition of ethylene glycol in the electrolyte enhances ionic conductivity at cold temperatures and optimizes electrode capacity by reduced hydrogen bonding within the water molecules and a decline in free water activity. The pronounced interaction between ethylene glycol and water, combined with the cooperative effect of the crosslinked polyacrylamide network, enables the hydrogel electrolyte to effectively suppress water solidification and maintain better water-retaining capability, achieving remarkable mechanical extensibility and good ionic conductivity (2.5 mS cm^-1) at - 40 °C. Consequently, the ASIB equipped with hydrogel electrolyte delivers high energy density of 43.6 Wh kg^-1 and retains 64 % at - 30 °C. Furthermore, the flexible ASIB demonstrates robust mechanical durability when bent or compressed, efficiently powering electronic devices even at - 30 °C. Our findings will pave the way for advancing low-temperature ASIBs with hydrogel-based electrolytes.