Mechanically Robust, Self-Healing Adaptive Ionic Conductors Enabled by Cellulose-Mediated Dynamic Covalent–Noncovalent Networks for Environmentally Adaptable Electronics

Abstract Ionic conductors have garnered significant attention in wearable sensors owing to their excellent weather resistance. However, their unsatisfactory mechanical properties and lack of self-healing capabilities hinder their practical application. Herein, an adaptive ionic conductor (AIC) with excellent mechanical properties, self-healing ability, and anti-freezing performance was developed by constructing dynamic covalent–noncovalent adaptive networks. In this AIC, amino cellulose (AC) is employed as a macromolecular crosslinker and in situ crosslinked with the aldehyde groups of vanillin monomer in a choline chloride/acrylic acid/vanillin monomer-derived polymerizable deep eutectic solvent to construct the dynamic covalent–noncovalent adaptive network through Schiff base chemistry and multiple hydrogen-bonding interactions. The synergistic effects of cellulose reinforcement and the formation of covalent–noncovalent adaptive networks endow the AIC with high mechanical strength (1.11 MPa), remarkable toughness (3.31 MJ/m3), and excellent anti-freezing capability. Meanwhile, the dynamic reversibility of the adaptive network imparts the AIC with outstanding self-healing performance, achieving a stress self-healing efficiency exceeding 90%. Notably, the AIC was successfully applied in environmentally adaptable multifunctional sensors and triboelectric nanogenerators for monitoring human motion and harvesting mechanical energy under extreme conditions. This work provides a promising strategy for the development of multifunctional adaptive ionic conductors for durable wearable sensors in harsh environments.