College of Chemistry and Molecular Sciences, Hubei Engineering Center of Natural Polymer-based Medical Materials, Wuhan University, Wuhan 430072, China.
College of Food Science and Engineering/Hubei Key Laboratory for Processing and Transformation of Agricultural Products, Wuhan Polytechnic University, Wuhan 430023, China.
ACS Appl Mater Interfaces. 2023 May 3;15(17):20761-20773. doi: 10.1021/acsami.3c02108. Epub 2023 Apr 19.
Trade-off of high-strength and dynamic crosslinking of hydrogels remains an enormous challenge. Motivated by the self-healing property of biological tissues, the strategy of combining multiple dynamic bond mechanisms and a polysaccharide network is proposed to fabricate biomimetic hydrogels with sufficient mechanical strength, injectability, biodegradability, and self-healing property for bone reconstruction engineering. Stable acylhydrazone bonds endowed hydrogels with robust mechanical strength (>10 kPa). The integration of dynamic imine bonds and acylhydrazone bonds optimized the reversible characteristic to protect the cell during the injection and mimicked ECM microenvironment for cell differentiation as well as rapid adapting bone defect area. Furthermore, due to the slow enzymatic hydrolysis kinetics of chitosan and the self-healing properties of resulting networks, hydrogels exhibited a satisfactory biodegradation period (>8 weeks) that highly matches with bone regeneration. Additionally, rBMSC-laden hydrogels exhibited splendid osteogenic induction and bone reconstruction without prefabrication scaffolds and incubation, demonstrating tremendous potential for clinical application. This work proposes an efficient strategy for the construction of a low-cost multifunctional hydrogel, making polysaccharide-based hydrogels as the optimal carrier for enabling cellular functions in bone repair.
水凝胶的高强度和动态交联之间的权衡仍然是一个巨大的挑战。受生物组织自修复特性的启发，提出了结合多种动态键合机制和多糖网络的策略，以制备具有足够机械强度、可注射性、生物可降解性和自修复特性的仿生水凝胶，用于骨重建工程。稳定的酰腙键赋予水凝胶强大的机械强度（>10 kPa）。动态亚胺键和酰腙键的结合优化了可逆特性，以在注射过程中保护细胞，并模拟 ECM 微环境以促进细胞分化和快速适应骨缺损区域。此外，由于壳聚糖的酶解动力学较慢以及由此产生的网络的自修复特性，水凝胶表现出令人满意的生物降解期（>8 周），与骨再生高度匹配。此外，负载 rBMSC 的水凝胶无需预制支架和孵育即可表现出出色的成骨诱导和骨重建能力，展示了巨大的临床应用潜力。这项工作提出了一种构建低成本多功能水凝胶的有效策略，使多糖基水凝胶成为实现骨修复中细胞功能的最佳载体。
