College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu 610065, China.
State Key Laboratory of Oral Diseases, West China Hospital of Stomatology, Sichuan University, Chengdu, 610041, China.
J Mater Chem B. 2022 Jun 15;10(23):4386-4394. doi: 10.1039/d2tb00545j.
As an ideal biomaterial, the injectable dual crosslinking hydrogel can fill irregular shaped defects for treating bone defects. Despite advances in the fabrication of injectable dual crosslinking hydrogels, current methods pose several limitations in the gelation process, such as unadjustable injectability, materials loss after injection and the employment of nonphysiological environments. A more rational designed hydrogel should be shear-thinning and self-healing quickly after injection, which requires a reversible noncovalent or dynamic covalent interaction. Besides, the improved mechanical properties and stability can be achieved . In this present research study, inspired by a high Ca concentration in the bone defect sites, a strategy combining hydrogen bonds and ion coordination to construct dual crosslinking hydrogels is developed. The prefabricated gel precursors based on hydrogen bonds of synthetic triblock poly(aspartic acid)-poly(ethylene glycol)-poly(aspartic acid) copolymers and tannic acid can be injected smoothly and recover rapidly to the initial state after injection. In addition, the hydrogel network can be crosslinked more tightly through the -COOH-Ca chelation, which results in reinforced mechanical properties and stability. The developed injectable dual crosslinking hydrogels will provide a design idea for the secondary crosslinking of injectable hydrogels , especially in the bone repair sites.
作为一种理想的生物材料,可注射双交联水凝胶可以填充不规则形状的缺陷来治疗骨缺损。尽管在可注射双交联水凝胶的制备方面取得了进展,但目前的方法在凝胶化过程中存在一些局限性,例如不可调节的可注射性、注射后材料损失以及使用非生理环境。更合理设计的水凝胶应该在注射后具有剪切稀化和快速自修复的特性,这需要可逆的非共价或动态共价相互作用。此外,还可以提高机械性能和稳定性。在本研究中,受骨缺损部位高钙离子浓度的启发,开发了一种结合氢键和离子配位构建双交联水凝胶的策略。基于合成三嵌段聚(天冬氨酸)-聚(乙二醇)-聚(天冬氨酸)共聚物氢键的预制凝胶前体和单宁酸可以顺利注射,并在注射后迅速恢复到初始状态。此外,通过-COOH-Ca 螯合作用可以使水凝胶网络交联得更紧密,从而增强机械性能和稳定性。所开发的可注射双交联水凝胶为可注射水凝胶的二次交联提供了设计思路,特别是在骨修复部位。