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Introduction Significant efforts have concentrated on creating various synthetic and natural biomaterials that mimic the native bone extracellular matrix, promote osteogenic differentiation, and improve effective bone regeneration. 3D printing has become a widely used fabrication method for scaffolds, facilitating the accurate mapping of the 3D structure of bone defects [1]. In this research, we aim to develop a multifunctional ink for 3D printing by combining the biological support of methacrylated gelatin (GelMA), the printability and structural reinforcement of κ-carrageenan, and the bioactive enhancements of polyhedral oligomeric silsesquioxane (POSS) and polydopamine (PDA), creating a composite system that integrates mechanical strength, osteoinductivity, and cellular compatibility [2] [3] [4].
Methods: Hydrogels composed of GelMA or dopamine-grafted GelMA (GelMA-Dopa), κ-carrageenan, POSS, and PDA were initially synthesized to evaluate their physicochemical characteristics, with the most promising formulation selected for subsequent 3D printing. The resulting freeze-dried scaffolds were structurally characterized using FTIR Spectroscopy, their rehydration capacity was assessed, and their morphology was examined via SEM. Additionally, compressive strength tests were performed, and biocompatibility was evaluated to determine their suitability for bone tissue engineering applications.
Results: FTIR Spectroscopy and 1H-NMR analyses confirmed the successful synthesis of GelMA-Dopa, while the formation of PDA was verified by FTIR. Furthermore, AFM and DLS analyses provided insights into the morphology and size distribution of the PDA particles. The incorporation of POSS and PDA significantly influenced the scaffold properties, leading to a reduced swelling degree and enhanced compressive strength. 3D printing experiments demonstrated favorable printability and high shape fidelity, highlighting the potential of these formulations for bone tissue engineering applications.
Conclusion: This research illustrates a multifunctional ink designed for bone tissue engineering, using GelMA, κ-carrageenan, POSS, and PDA to attain an equilibrium among biocompatibility, mechanical strength, and printability. The synthesis and characterization of the hydrogel components validated the structural integrity and functionalization of the materials, whereas the integration of POSS and PDA significantly improved scaffold performance by enhancing compressive resistance and diminishing swelling behavior. Furthermore, 3D printing evaluations validated the materials’ capacity to generate constructions with exceptional print quality and structural integrity.
Acknowledgements: A. Dinu acknowledges the funding received from Romanian Ministry of Education and Research and National University of Science and Technology Politehnica Bucharest.
References:
[1] Z. Li, Q. Wang, and G. Liu, “A Review of 3D Printed Bone Implants,” Apr. 01, 2022, MDPI. doi: 10.3390/mi13040528.
[2] L. Tytgat et al., “Extrusion-based 3D printing of photo-crosslinkable gelatin and κ-carrageenan hydrogel blends for adipose tissue regeneration,” Int J Biol Macromol, vol. 140, pp. 929–938, Nov. 2019, doi: 10.1016/j.ijbiomac.2019.08.124.
[3] M. Chen et al., “Long-Term Bone Regeneration Enabled by a Polyhedral Oligomeric Silsesquioxane (POSS)-Enhanced Biodegradable Hydrogel,” ACS Biomater Sci Eng, vol. 5, no. 9, pp. 4612–4623, 2019, doi: 10.1021/acsbiomaterials.9b00642.
[4] Y. Xu et al., “Bioinspired polydopamine hydrogels: Strategies and applications,” Nov. 01, 2023, Elsevier Ltd. doi: 10.1016/j.progpolymsci.2023.101740.
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