Mechanically Robust and Room Temperature Self‐Healing Ionogel Based on Ionic Liquid Inhibited Reversible Reaction of Disulfide Bonds

Although highly desired, it is difficult to develop mechanically robust and room temperature self‐healing ionic liquid‐based gels (ionogels), which are very promising for next‐generation stretchable electronic devices. Herein, it is discovered that the ionic liquid significantly reduces the reversible reaction rate of disulfide bonds without altering its thermodynamic equilibrium constant via small molecule model reaction and activation energy evolution of the dissociation of the dynamic network. This inhibitory effect would reduce the dissociated units in the dynamic polymeric network, beneficial for the strength of the ionogel. Furthermore, aromatic disulfide bonds with high reversibility are embedded in the polyurethane to endow the ionogel with superior room temperature self‐healing performance. Isocyanates with an asymmetric alicyclic structure are chosen to provide optimal exchange efficiencies for the embedded disulfide bonds relative to aromatic and linear aliphatic. Carbonyl‐rich poly(ethylene‐glycol‐adipate) diols are selected as soft segments to provide sufficient interaction sites for ionic liquids to endow the ionogel with high transparency, stretchability, and elasticity. Finally, a self‐healing ionogel with a tensile strength of 1.65 ± 0.08 MPa is successfully developed, which is significantly higher than all the reported transparent room temperature self‐healing ionogel and its application in a 3D printed stretchable numeric keyboard is exemplified.