Nanocomposite Hydrogels Enhanced by Cellulose Nanocrystals Stabilized Pickering Emulsions with Self-Healing Performance in Subzero Environment

Nowadays, hydrogels as flexible materials have attracted considerable attention in frontier fields such as wearable electronic devices, soft actuators and robotics. However, water-based hydrogels inevitably freeze at subzero temperatures and suffer damage from contact with objects, which greatly reduce their service life and practical value. Herein, nanocomposite hydrogels with self-healing performance at subzero temperatures were proposed by introducing binary water-glycerol continuous phase and dual self-healing interactions. The binary solvents were emphasized in preventing the formation of ice crystals, enhancing flexible and self-healing abilities of hydrogels in subzero environment. Linseed oil as healing agent was effectively loaded in Pickering droplets by cellulose nanocrystals. Owing to non-covalent bonding and external healing agent, the obtained hydrogels showed improved mechanical properties and self-healing abilities. Particularly, after incorporating Pickering droplets, the rupture stress of nanocomposite hydrogels was 0.24 MPa, the rupture strain was 1900% and the healing efficiency could be up to 80.1% for 12 h at − 20 °C. Therefore, the obtained hydrogels with frost resistance, stretchability and self-healing properties should have broader potential applications, especially in subzero environment.