Fabrication of anti-freezing and self-healing nanocomposite hydrogels based on phytic acid and cellulose nanocrystals for high strain sensing applications

For hydrogel-based flexible sensors, it is a challenge to enhance the stability at sub-zero temperatures while maintaining good self-healing properties. Herein, an anti-freezing nanocomposite hydrogel with self-healing properties and conductivity was designed by introducing cellulose nanocrystals (CNCs) and phytic acid (PA). The CNCs were grafted with polypyrrole (PPy) by chemical oxidation, which were used as the nanoparticle reinforcement phase to reinforce the mechanical strength of hydrogels (851.8%). PA as a biomass material could form strong hydrogen bond interactions with H₂O molecules, endowing hydrogels with prominent anti-freezing properties. Based on the non-covalent interactions, the self-healing rate of the hydrogels reached 92.9% at -15 °C as the content of PA was 40.0 wt%. Hydrogel-based strain sensors displayed high sensitivity (GF = 0.75), rapid response time (350 ms), good conductivity (3.1 S m^-1) and stability at -15 °C. Various human movements could be detected by using them, including small (smile and frown) and large changes (elbow and knee bending). This work provides a promising method for the development of flexible wearable sensors that work stably in frigid environments.