Room-temperature self-healing polyurethane–cellulose nanocrystal composites with strong strength and toughness based on dynamic bonds

Self-healing materials suffer from a trade-off relationship between their self-healing ability and mechanical strength, which limits their applications. Therefore, we developed a room-temperature self-healing supramolecular composite based on polyurethane (PU) elastomer, cellulose nanocrystals (CNCs), and multiple dynamic bonds. In this system, the abundant hydroxyl groups on the surfaces of the CNCs form multiple hydrogen bonds with the PU elastomer, yielding a dynamic physical cross-linking network. This dynamic network enables self-healing without degrading the mechanical properties. As a result, the obtained supramolecular composites exhibited high tensile strength (24.5 ± 2.3 MPa), good elongation at break (1484.8 ± 74.9 %), favourable toughness (156.4 ± 31.1 MJ m-3, which is equivalent to that of spider silk and 5.1-times higher than that of aluminium), and excellent self-healing efficiency (95 ± 1.9 %). Notably, the mechanical properties of the supramolecular composites were almost completely retained after reprocessing three times. Further, using these composites, flexible electronic sensors were prepared and tested. In summary, we have reported a method for preparing supramolecular materials having high toughness and room temperature self-healing ability that have applications in flexible electronics.