Gelatin Hydrogels Reinforced by Absorbable Nanoparticles and Fibrils Cured In Situ by Visible Light for Tissue Adhesive Applications

Most gelatin hydrogels used in regenerative medicine applications today are fabricated by photocrosslinking due to the convenience and speed of this method. However, in most cases photoinitiators are used, which require UV light, which, in turn, can cause cell and tissue damage, or using functionalized gelatin. Recently, ruthenium (II) tris-bipyridyl chloride has been studied as an initiator that can induce dityrosine bond formation using visible light. In addition, continuous fibrils and small particles are often used to reinforce composite materials. Therefore, this study investigated the visible-light-induced photocrosslinking of native gelatin molecules via dityrosine bonds formation as well as gel reinforcement by collagen fibrils and mesoporous bioactive glass (MBG) particles. The results show that collagen and MBG exerted a synergistic effect on maintaining gel integrity with a dental LED curing light when the irradiation time was shortened to 30 s. Without the two reinforcing components, the gel could not form a geometric shape stable gel even when the exposure time was 120 s. The shear strength increased by 62% with the collagen and MBG compared with the blank control. Furthermore, our results demonstrate that the addition of collagen and MBG enhanced gel stability in an artificial saliva solution. These results demonstrate the considerable advantages of using tyrosine-containing biomolecules, and using a dental LED curing light for the crosslinking of hydrogels in terms of their suitability and feasibility for use as bioadhesives in confined clinical working space, such as the oral cavity, and in application as in situ-crosslinked injectable hydrogels.