Poly(β-hydroxyl amine)s: Valuable Building Blocks for Supramolecular Elastomers with Tunable Mechanical Performance and Superior Healing Capacity.

Supramolecular elastomers integrated with high mechanical toughness and excellent self-healing ability offer attractive applications in various fields such as biomedical materials and wearable electronics. However, the multistep preparation process for creating functional polymer precursors and the expensive stock materials required are two factors that limit the widespread use of supramolecular elastomers. Herein, for the first time, poly(β-hydroxyl amine)s generated by amine-epoxy polymerization were used in the development of supramolecular polymer materials. Based on the novel silicon-containing poly(β-hydroxyl amine)s synthesized by the polymerization between 1,3-bis(3-glycidyloxypropyl)tetramethyldisiloxane and 3-amino-1,2-propanediol, dually cross-linked supramolecular elastomers with both hydrogen bonding and metal coordination were achieved, displaying adjustable mechanical properties with the tensile strength varying from 0.70 MPa to 2.52 MPa, respectively. Thanks to the dynamic nature of the supramolecular interactions, these elastomers exhibited favorable hot-pressing reprocessability and excellent self-healing performance, with the healing efficiency reaching up to 98% at 60 °C for 48 h. Potential applications for photoluminescent materials and flexible electronic devices were demonstrated. We believe that its simplicity of synthesis, adjustable mechanical properties, and robust self-healing capacities bode well for future applications of this new supramolecular elastomer.