Abstract

Flexible zinc-ion batteries (ZIBs) assembled with hydrogel electrolyte are considered as promising flexible energy storage devices because of their inherent safety and versatility. However, the ionic conductivity and mechanical properties of most hydrogel electrolytes are not satisfactory, Furthermore, they will freeze at subzero temperature due to existing water. In this work, a freezing resistant polycarboxylic double network gel electrolyte (SIP-CS) with high ionic conductivity (14.36 mS cm⁻1 at −20 °C) and excellent mechanical property (fracture stress of 241.5 kPa and fracture strain of 1011 %) is prepared. Iminodiacetic acid (IDA) is applied to modify the alginate mainchains with many -COOH groups, which could provide channels for ion migration and endow hydrogel with high ionic conductivity. Additionally, sorbitol, containing lots of hydroxyl groups, is applied as a cryoprotectant to enhance the subzero performance of the electrolyte, because sorbitol could break the hydrogen bonds between water molecules, inhibit the formation of ice crystals, and reduce the freezing point of the gel electrolyte. The freezing point of SIP-CS is −37.0 °C, enabling the electrolyte to perform well at low temperatures. The flexible quasi solid Zn-MnO2 battery is assembled to evaluate the low-temperature electrochemical performance of SIP-CS. The assembled Zn-MnO2 battery shows good cycling and stable electrochemical performance, which proves the excellent antifreezing property of SIP-CS. This work provides a new strategy for preparing an electrolyte with good withstand low-temperature capability.

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