Study on Printability Evaluation of Alginate/Silk Fibroin/Collagen Double-Cross-Linked Inks and the Properties of 3D Printed Constructs

In recent years, biological 3D printing has garnered increasing attention for tissue and organ repair. The challenge with 3D-printing inks is to combine mechanical properties as well as biocompatibility. Proteins serve as vital structural components in living systems, and utilizing protein-based inks can ensure that the materials maintain the necessary biological activity. In this study, we incorporated two natural biomaterials, silk fibroin (SF) and collagen (COL), into a low-concentration sodium alginate (SA) solution to create novel composite inks. SF and COL were modified with glycidyl methacrylate (GMA) to impart photo-cross-linking properties. The UV light test and 1 H NMR results demonstrated successful curing of silk fibroin (SF) and collagen (COL) after modification and grafting. Subsequently, the printability of modified silk fibroin (RSFMA)/SA with varying concentration gradients was assessed using a set of three consecutive printing models, and the material’s properties were tested. The research results prove that the addition of RSFMA and ColMA enhances the printability of low-concentration SA solutions, with the Pr values increasing from 0.85 ± 0.02 to 0.90 ± 0.03 and 0.92 ± 0.02, respectively, and the mechanical strength increasing from 0.19 ± 0.01 to 0.28 ± 0.01 and 0.38 ± 0.01 MPa; cytocompatibility has also been improved. Furthermore, rheological tests indicated that all of the inks exhibited shear thinning properties. CCK-8 experiments demonstrated that the addition of ColMA increased the cytocompatibility of the ink system. Overall, the utilization of SF and COL-modified SA materials as inks represents a promising advancement in 3D-printed ink technology.