A dual network hydrogel made up of polyvinylalcohol (PVA) crosslinked by borax and polyvinylpyrrolidone (PVP) was prepared by means of freezing-thawing circles. Here PVP was incorporated by linking with PVA to form a network structure, while the introduction of borax played the role of crosslinking PVA chains to accelerate the formation of a dual network structure in PVA/PVP composite hydrogel, thus endowing the hydrogel with high mechanical properties. The effects of both PVP and borax on the hydrogels were evaluated by comparing the two systems of PVA/PVP/borax and PVA/borax hydrogels. In the former system, adding 4.0% PVP not only increased the water content and the storage modulus but also enhanced the mechanical strength of the final hydrogel. But an overdose of PVP just as more than 4.0% tended to undermine the structure of hydrogels, and thus deteriorated hydrogels’ properties because of the weakened secondary interaction between PVP and PVA. Likewise, increasing borax could promote the gel crosslinking degree, thus making gels show a decrease in water content and swelling ratio, meanwhile shrinking the pores inside the hydrogels and finally enhancing the mechanical strength of hydrogels prominently. The developed hydrogel with high performances holds great potential for applications in biomedical and industrial fields.
The inability of damaged load-bearing cartilage to regenerate and self-repair remains a long-standing challenge in clinical settings. In the past, the use of PVA hydrogels as cartilage replacements has been explored; however, both pristine and annealed PVA are not ideal for load-bearing cartilage applications, and new materials with improved properties are highly desirable. In this work, we developed a novel hybrid hydrogel system consisting of glycerol-modified PVA hydrogel reinforced by a 3D printed PCL-graphene composite scaffold. The composition of the hydrogel within the hybrid material was optimized to achieve high water retention and enhanced stiffness. The hybrid hydrogel formed by reinforcement with a 3D printed PCL-graphene scaffold with optimized architecture demonstrated desirable mechanical properties (stiffness, toughness, and tribological properties) matching those of natural load-bearing cartilage. Our novel hydrogel system has also been designed to provide drug release and on-demand photothermal conversion functions and at the same time offers excellent biocompatibility with low cell adhesion. These promising properties may allow our unique hybrid hydrogel system to be used for potential applications, such as load-bearing cartilage repair/replacement, as well as targeting certain challenging clinical conditions, such as the treatment of severe arthritis.