Chitosan-reinforced gelatin composite hydrogel as a tough, anti-freezing, and flame-retardant gel polymer electrolyte for flexible supercapacitors

Hydrogel-based electrolytes for flexible solid-state supercapacitors (SSCs) have received significant attention due to their mechanical robustness and stable electrochemical performance over a wide temperature range. However, achieving flame retardancy in such SSCs at subzero temperatures to increase their practical utility remains challenging. Furthermore, there is a need for sustainable and bio-friendly SSCs that use natural polymer-based hydrogel electrolytes. This study reports a novel approach for developing a chitosan-reinforced anti-freezing ionic conductive gelatin hydrogel to meet these demands. Immersion of chitosan-containing gelatin hydrogels in salt solutions caused chitosan precipitation, resulting in composite hydrogels. The precipitated chitosan contributes to the reinforcement of the gelatin hydrogel network, resulting in a high mechanical toughness of up to 3.81 MJ/m3, a fracture energy of 26 kJ/m2, anti-freezing properties (below -30 °C), and excellent flame retardancy without softening. Furthermore, the hydrogel exhibits excellent electrochemical performance, with an ionic conductivity ranging from 72 mS/cm at room temperature (26 °C) to 39 mS/cm at -30 °C. The proposed hydrogel exhibits potential for use in SSC as a gel polymer electrolyte. This study demonstrates a novel strategy for controlling the mechanical, thermal, and electrochemical characteristics of flexible supercapacitors using biological macromolecules.