Tailoring viscoelastic properties of dynamic supramolecular poly(butadiene)-based elastomers

• Published in: Materials today chemistry Vol. 26; p. 101008
• Main Authors: Hyder, M., O'Donnell, A.D., Chippindale, A.M., German, I.M., Harries, J.L., Shebanova, O., Hamley, I.W., Hayes, W.
• Format: Journal Article
• Language: English
• Published: Elsevier Ltd 01.12.2022
• Subjects: Adhesive; End-group control; Healable; Supramolecular materials; End-group control; Supramolecular materials; Healable; Adhesive
• ISSN: 2468-5194; 2468-5194
• DOI: 10.1016/j.mtchem.2022.101008

The discovery and development of new adhesive materials is critical for real-world applications of polymeric composite materials. Herein, we report the design and synthesis of a library of structurally related phase-separated supramolecular polyurethanes whose mechanical properties and adhesive characteristics can be enhanced through minor structural modifications of the polymer end-group. The interplay between phase separation of the hard domain polar end-groups and soft polybutadiene domains, coupled with tuneable self-assembly afforded by the polar end-groups, gives rise to a class of materials with tuneable mechanical properties. Exceptionally strong supramolecular adhesives and mechanically robust self-healing elastomers were identified. The mechanical properties were investigated through tensile testing. Finally, rheological analysis of the supramolecular materials was used to identify suitable healing and adhesive temperatures in addition to elucidate the supramolecular polyurethanes' thermal-responsive nature. [Display omitted] •Tune supramolecular assembly by structural variation of the polymer end-group.•The competitive composition of the end-group determines viscoelastic properties.•Access to strong, tough supramolecular elastomeric and healable adhesives.