Double-network acrylamide hydrogel compositions adapted to achieve cartilage-like dynamic stiffness

Since articular cartilage has a limited potential for spontaneous healing, various techniques are employed to repair cartilage lesions. Acrylate-based double-network (DN) hydrogels containing ~90% water have shown promising properties as repair materials for skeletal system soft tissues. Although their mechanical properties approach those of native cartilage, the critical factor—stiffness—of DN-gels does not equal the stiffness of articular cartilage. This study investigated whether revised PAMPS/PAAm compositions with lower water content result in stiffness parameters closer to cartilage. DN-gels containing 61, 86 and 90% water were evaluated using two non-destructive, mm-scale indentation test modes: fast-impact (FI) and slow-sinusoidal (SS) deformation. Deformation resistance (dynamic modulus) and energy handling (loss angle) were determined. The dynamic modulus increased with decreasing water content in both testing modes. In the 61% water DN-gel, the modulus resembled that of cartilage (FI-mode: DN-gel = 12, cartilage = 17; SS-mode: DN-gel = 4, cartilage = 1.7 MPa). Loss angle increased with decreasing water content in fast-impact, but not in slow-sinusoidal deformation. However, loss angle was still much lower than cartilage (FI: DN-gel = 5, cartilage = 11; SS: DN-gel = 10, cartilage = 32°), indicating somewhat less ability to dissipate energy. Overall, results show that it is possible to adapt DN-gel composition to produce dynamic stiffness properties close to normal articular cartilage.