Bioactive and biomimetic 3D scaffolds for bone tissue engineering using graphitic carbon nitride as a sustainable visible light photoinitiator

Graphitic carbon nitride (g-C₃N₄) is explored as a novel sustainable visible light photoinitiator for the preparation of biomimetic 3D hydrogel scaffolds comprising gelatin methacrylamide (GelMA) and dopamine methacrylamide for use in tissue engineering. The initiator efficiency was assessed by comparing the swelling behavior and the stability of photopolymerized hydrogels prepared with GelMA of different degrees of functionalization and different comonomer compositions. Bioactive composite hydrogels with a 50 wt% nanohydroxyapatite (nHAp) content, to closely mimic the actual bone composition, were successfully obtained by the introduction of nHAp in the prepolymer solutions followed by photopolymerization. The composite hydrogels demonstrated enhanced mechanical properties and excellent stability in PBS verifying the preparation of robust 3D scaffolds for use in cancellous or pre-calcified bone tissue engineering applications. The in vitro cell response of the composite scaffolds exhibited high cell viability and enhanced differentiation of pre-osteoblasts to mature osteoblasts, demonstrating their osteogenic potential. This work establishes, for the first time, the excellent properties of g-C₃N₄ as a sustainable, visible light initiator, fully satisfying the principles of green chemistry, for the preparation of robust and biologically relevant hydrogels, and proposes a new approach to overcome the main challenges of conventional photoinitiators in cell scaffold fabrication, such as photobleaching, high cost and non-scalable synthesis employing toxic organic precursors and solvents.