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Currently, composite and class I hybrid biomaterials are used for tissue regeneration applications. To improve and better control biomaterial properties, we synthesized class II organic/inorganic (O/I) hybrids, in which organic polymers and inorganic tertiary bioactive glass (TBG) were covalently cross-linked. To tailor their microstructure, bioactivity, degradation, and mechanical properties, we altered the degree of cross-linking by varying the amount of functional groups in the polymer that mediate covalent bonding to the TBG. We synthesized class II hybrids in a two-step process: first, vinylpyrrolidone (VP) and triethoxyvinylsilane (TEVS) were copolymerized at various molar ratios to obtain different amounts of silane functional groups in the copolymer; second, TBG and the copolymer were mixed and allowed to undergo hydrolysis and polycondensation forming Si-O-Si- and Si-O-P-bridging networks between the organic and inorganic phases. Higher amounts of functional groups increased copolymer-TBG covalent bonding and decreased degradation and the release of TBG dissolution products. Incubation in simulated body fluid led to biomimetic apatite deposition on the hybrid biomaterial surfaces, which was primarily dependent on O/I weight ratios. A higher TBG content improved apatite deposition and biocompatibility. Porous and interconnected three-dimensional scaffolds, fabricated by indirect 3D printing using polycaprolactone as a sacrificial template, had intriguing yield and compressive strengths, compressive moduli, and toughness. These studies demonstrate, for the first time, that the functionality of our synthesized copolymers greatly affects the nature of O/I matrix formation and degradation behavior of the class II hybrid biomaterials, creating possibilities for tailoring the physical, biochemical, and mechanical properties of scaffold biomaterials for tissue regeneration and related applications. |
