Abstract

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.

Highlights

  • 2.52 MPa, respectivelyThanks 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

  • Introduction published maps and institutional affilSupramolecular elastomers [1] are elastic networks cross-linked by non-covalent bonds such as hydrogen bonds [2,3], metal–ligand interactions [4,5], host–guest interactions [6,7], and π-π stacking [8–10]

  • As shown in Scheme 1A, this functional polymer is readily prepared via the click polymerization of amine and epoxy monomers at ambient conditions

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Summary

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. Dually associated supramolecular polymers containing both hydrogen bonding and metal coordination was demonstrated with enhanced fracture energy and exhibiting multiple shape-memory and self-healing properties [15] Due to their rich chemical structures, adjustable mechanical properties, and self-healing capacities, supramolecular elastomers can potentially be used in the field of wearable electronics, electronic skins, motion tracking, and health monitoring [16–18]. Repetitive nitrogen atoms in the polymeric backbone can provide lone pairs of electrons for coordination with electron-deficient metal ions Both features make poly(β-hydroxyl amine)s promising candidates for the preparation of supramolecular polymer materials. This research provides a feasible method for designing mechanically tough, self-healing, reprocessable materials that demonstrate promising applications for use in photoluminescent materials and flexible electronics To our knowledge, this is the first attempt to use poly(β-hydroxyl amine) generated via the amine-epoxy polymerization for supramolecular materials

Materials
Characterization and Measurements
Synthesis of Polymer P1 via the Amine-Epoxy Polymerization
Preparation of Dually Supramolecular Elastomers (P1-Cu-x/1)
Self-Healing Tests of the Supramolecular Elastomers
Preparation of the Photoluminescent Supramolecular Elastomer P1-Eu-x
Preparation of the Conductive Supramolecular Elastomer P1-MWCNT
Results
H NMR spectra of monomer
Dynamic
Applications
Conclusions
Full Text
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