Adhesive Gelatin-Catechol Complex Reinforced Poly(Acrylic Acid) Hydrogel with Enhanced Toughness and Cell Affinity for Cartilage Regeneration

The repair of cartilage damage caused by trauma, wear, or degenerative deformation remains a major challenge in modern medicine. Therefore, it is essential to develop a mechanically compatible and bioactive scaffold for cartilage tissue regeneration. In this study, a mussel-inspired, tough, adhesive polydopamine/gelatin-poly(acrylic acid) (PDA/Gel-PAA) composite hydrogel was developed for cartilage regeneration. The hydrogel achieved a high compressive strength of up to 0.67 MPa and a toughness of 420 J/m2 because of the unique chemical-physical cross-linking structure by introducing the PDA/Gel complex into the PAA network. PAA chains with rich carboxyl groups mimic the negatively charged glycosaminoglycans (GAGs) in the natural cartilage extracellular matrix (ECM), leading to strong water retention in the hydrogel. The incorporation of the PDA/Gel complex with catechol groups on PDA and arginine-glycine-aspartic acid (RGD) sequences on gelatin chains provided abundant adhesive motifs to improve the cell affinity and tissue adhesiveness of PAA, thereby facilitating the adhesion and proliferation of bone marrow stromal cells (BMSCs). In addition, transforming growth factor-β3 (TGFβ3) was stably immobilized and released from the PDA/Gel-PAA hydrogel. Thus, adhesive hydrogels can provide a suitable microenvironment to promote cell migration in the defect area and induce chronogenesis for cartilage regeneration.