Isocyanate-terminated urethane-based methacrylate for in situ collagen scaffold modification

When damaged or fractured collagen-rich hard tissues are repaired by resin material, the collagen matrix may be used as a scaffold, after removal of the natural minerals, for resin monomers to penetrate and polymerize in-situ. Formation of a collagen-polymer hybrid biocomposite via mechanical hybridization provides a stable and strong link between endogenous tissue and the prosthesis for successful clinical integration. However, the heterogeneity between hydrophobic resin polymers and hydrophilic collagen presents a challenge to the quality of hybrid biocomposite. The objective of the present study was to evaluate the potential benefits of a collagen-reactive monomer (CRM, an isocyanate-terminated urethane-based methacrylate) with covalent affinity to collagen as "chemical link" to enhance in-situ resin hybridization within a collagen scaffold. Here, the CRM ligand with active isocyanate group may be chemically grafted onto the collagen receptor via covalent and hydrogen bonds. Dentin-derived collagen chemical modified by CRM shows improved mechanical property, thermostability and enzymatic stability. Moreover, CRM inhibited both exogenous and endogenous collagenase activities. The modification of collagen by chemical grafting of resin monomers improved its mechanical and physicochemical properties and demonstrated the potential of CRM for use in promoting chemical adhesion and creating a much stronger and durable bonding interface. Formation of a chemical bond between polymer and collagen scaffold in-situ improves the mechanical performance of collagen and may create a much stronger and durable collagen-polymer hybrid material. Addition of CRM into adhesives might effectively prolong the longevity of clinical resin-bonded restorations.