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Macroscopic hydrogel fibers are highly desirable for smart textiles, but the fabrication of self-healable and super-tough covalent/physical double-network hydrogels is rarely reported. Herein, copolymers containing ketone groups were synthesized and prepared into a dynamic covalent hydrogel via acylhydrazone chemistry. Double-network hydrogels were constructed via the dynamic covalent crosslinking of copolymers and the supramolecular interactions of iota-carrageenan. Tensile tests on double-network and parental hydrogels revealed the successful construction of strong and tough hydrogels. The double-network hydrogel precursor was wet spun to obtain macroscopic fibers with controlled drawing ratios. The resultant fibers reached a high strength of 1.35 MPa or a large toughness of 1.22 MJ/m3. Highly efficient self-healing performances were observed in hydrogel fibers and their bulk specimens. Through the simultaneous healing of covalent and supramolecular networks under acidic and heated conditions, fibers achieved rapid and near-complete healing with 96% efficiency. Such self-healable and super-tough hydrogel fibers were applied as shape memory fibers for repetitive actuating in response to water, indicating their potential in intelligent fabrics.

Self-Healable and Super-Tough Double-Network Hydrogel Fibers from Dynamic Acylhydrazone Bonding and Supramolecular Interactions