Customizable Low-Friction Tough Hydrogels for Potential Cartilage Tissue Engineering by a Rapid Orthogonal Photoreactive 3D-Printing Design

Hydrogels have demonstrated wide applications in tissue engineering, but it is still challenging to develop strong, customizable, low-friction artificial scaffolds. Here, we report a rapid orthogonal photoreactive 3D-printing (ROP3P) strategy to achieve the design of high-performance hydrogels in tens of minutes. The orthogonal ruthenium chemistry enables the formation of multinetworks in hydrogels via phenol-coupling reaction and traditional radical polymerization. Further Ca2+-cross-linking treatment greatly improves their mechanical properties (6.4 MPa at a critical strain of 300%) and toughness (10.85 MJ m–3). The tribological investigation reveals that the high elastic moduli of the as-prepared hydrogels improve their lubrication (∼0.02) and wear-resistance performances. These hydrogels are biocompatible and nontoxic and promote bone marrow mesenchymal stem cell adhesion and propagation. The introduction of 1-hydroxy-3-(acryloylamino)-1,1-propanediylbisphosphonic acid units can greatly enhance their antibacterial property to kill typical Escherichia coli and Staphylococcus aureus. Moreover, the rapid ROP3P can achieve hydrogel preparation in several seconds and is readily compatible with making artificial meniscus scaffolds. The printed meniscus-like materials are mechanically stable and can maintain their shape under long-term gliding tests. It is anticipated that these high-performance customizable low-friction tough hydrogels and the highly efficient ROP3P strategy could promote further development and practical applications of hydrogels in biomimetic tissue engineering, materials chemistry, bioelectronics, and so on.