Environment Endurable, Self‐Healing, Super‐Adhesive, and Mechanically Strong Ionogels for Reliable Sensing

Abstract Ionogels possess high conductivity, stretchability, and adhesion, making them promising as flexible sensors. However, it remains challenging to fabricate an ionogel which integrates excellent environment endurance, superior mechanical strength, high self‐healing efficiency, and super adhesion. Herein, a supramolecular ionic liquid is synthesized using calcium chloride and 1‐butyl‐3‐methylimidazolium chloride. An advanced ionogel based on this supramolecular ionic liquid is conveniently constructed by a one‐pot method with acrylamide and acrylic acid as monomers. The supramolecular cross‐linking network, formed by affluent coordination interactions, hydrogen bonds, and electrostatic interactions, provides the ionogel with ideal mechanical strength (tensile strength up to 1.7 MPa), high self‐healing efficiency (up to 149%), super adhesion (up to 358 kPa on aluminum), excellent solvent tolerance (less than 10% weight increase, high mechanical and sensing performance retention after being soaked in organic solvents), and low‐temperature endurance (breaking elongation can reach 87% at −30 °C). The supramolecular ionogels can function as multi‐mode sensors, capable of monitoring strain and different amplitudes of human movements in real‐time. Moreover, the sensing performance of ionogels remains unaffected even after being self‐healed or exposure to organic solvents. It is expected that this study could offer valuable design ideas to construct advanced gel materials applicable in complicated environment.