Multi-Modal Mechanical Response of Self-Healing Double-Network Hydrogel Coatings Based on Schiff Base Bond

Ti6Al4V alloy is one of the most widely used orthopedic implants due to its low density, high strength and good biocompatibility, but surface tribology limits its service life and performance. In this paper, a layer of dynamic double-network hydrogel based on a Schiff base bond and a hydrogen bond was grafted on the surface of Ti6Al4V alloy by the mussel chemical self-assembly method. The -NH2 of acrylamide (AM) and -CHO of vanillin (VA) formed Schiff base bonds to form the first layer of a cross-linked network, a large number of hydrogen bonds were formed between the -OH of vanillin and the -OH of sodium alginate (SA) to provide the second layer of the cross-linked network and the network was properly regulated by introducing core–shell polymer nanoparticles (PDCS). Dynamic self-healing bonds, Schiff base bonds and hydrogen bonds endow qPDCS/SA/VA/AM hydrogels with self-healing ability, and the network structure destroyed under high strain (250%) can be rebuilt under low strain (1%). In the second cycle, G’ and G can recover almost the same value. PDCS/SA/VA/AM hydrogel coating can achieve dynamic repair through reversible Schiff base bond dissociation–recombination during friction, while 1000ppmPDCS/SA/VA/AM hydrogel coating can achieve stable friction reduction and low wear under multiple loads. Under 0.5 N load, the average friction coefficient of 1000ppmPDCS/SA/VA/AM hydrogel coating is as low as 0.157, which is 67.74% lower than the uncoated Ti6Al4V surface under the same load. Under 2 N load, 1000ppmPDCS/SA/VA/AM hydrogel coating remains stable and low-friction, and the average coefficient of friction (ACOF) can reach 0.130, which is 59.27% lower than the uncoated Ti6Al4V surface under the same load. The design idea of the hydrogel network regulated by core–shell polymer nanoparticles (PDCS) to achieve low friction and low wear provides a new strategy for biolubricating materials.