Extremely Stretchable, Self-Healable Elastomers with Tunable Mechanical Properties: Synthesis and Applications

Stretchable and autonomously self-healable elastomers with wide-ranging tunable mechanical properties have attracted increasing attention in various industries. To date, it continues to be a huge challenge to synthesize self-healing elastomers integrating extreme stretchability, relatively high mechanical modulus, and autonomous and rapid self-healing capability. Herein, we propose a novel covalent/supramolecular hybrid construction strategy, in which the covalent cross-links are responsible for providing high modulus and elasticity, while supramolecular cross-links realize extreme stretchability and rapid self-healing under room temperature depending on the ultrafast exchange kinetics of metal–ligand motifs and multicoordination modes. The representative polyurea hybrid elastomer, CSH-PPG-Zn-0.25, can be stretched more than 180× its original length with the highest Young’s modulus (1.78 ± 0.08 MPa) among reported ultrastretchable materials. CSH-PPG-Zn-0.25 can fully restore mechanical properties of compl...