Gelation of silk fibroin solution via β-sheet formation promoted by riboflavin-mediated photo-crosslinking

Di-tyrosine photo-crosslinking of silk fibroin (SF) is recently highlighted as a biocompatible hydrogel fabrication process, because this method does not need potentially harmful chemical species. However, the resulting crosslinking density is often insufficient to obtain a mechanically stiff hydrogel unless additional oxygen is provided during the reaction. In this study, we proposed a combinational crosslinking method to form an SF hydrogel via the di-tyrosine photo-crosslinking with riboflavin (photoinitiator) and physical interaction of SF chains. In the UV light-irradiated SF solution, small particles formed and these particles promoted β-sheet formation of SF molecules, resulting in quick gelation. The di-tyrosine photo-crosslinking produced nuclei that might trigger regular assembly of SF molecules in high temperature condition. Conclusively, this process would contribute to a development of biocompatible hydrogel fabrication for biomedical uses of SF hydrogels.