Injectable hydrogels self-assembled from oligopeptide-poly(2-methacryloyloxyethyl phosphorylcholine) hybrid graft copolymers for cell scaffolds and controlled release applications
Injectable hydrogels self-assembled from oligopeptide-poly(2-methacryloyloxyethyl phosphorylcholine) hybrid graft copolymers for cell scaffolds and controlled release applications
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DOI：
10.1039/d1ma00347j
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发表时间：
2021-05-25
影响因子：
5
通讯作者：
Higashi, Nobuyuki
中科院分区：
文献类型：
--
作者：
Koga, Tomoyuki;Matsuoka, Tomoo;Higashi, Nobuyuki
在本文中，我们报告了可形成可注射水凝胶的新型肽基杂化接枝共聚物的合成和表征。这些杂化接枝共聚物由生物相容性聚（2-甲基丙烯酰氧基乙基磷酰胆碱）主链和自组装低聚丙氨酸-嵌段-聚乙二醇接枝物（接枝率（m）= 6、10、20、28、32和40%）组成，通过结合固相肽合成和常规自由基聚合方法，可以使用大分子单体轻松合成。在多种稀水溶液（pH 3-10 和 4-70 摄氏度）下进行的构象分析显示稳定的 β-折叠形成。随着溶液浓度的增加，由于肽接枝物的可逆自组装特性，除接枝率低（m = 6）的接枝共聚物外，接枝共聚物形成的水凝胶表现出剪切稀化和自修复行为。有趣的是，杂化接枝共聚物的机械性能强烈依赖于杂化共聚物的接枝密度。因此，观察到接枝率的增加增强了聚合物间网络。这些特征使得移植型杂化物能够用作 3D 细胞支架和控释应用的可注射水凝胶。
In this paper, we report the synthesis and characterization of novel peptide based hybrid graft copolymers that can form injectable hydrogels. These hybrid graft copolymers are composed of a biocompatible poly(2-methacryloyloxyethyl phosphorylcholine) main chain and self-assembling oligoalanine-block-poly(ethylene glycol) grafts (grafting ratio (m) = 6, 10, 20, 28, 32, and 40%), which are readily synthesized using a macromonomer by combining the solid phase peptide synthesis and conventional radical polymerization methods. Conformational analyses under a wide range of dilute aqueous solutions (pH 3-10 and 4-70 degrees C) revealed stable beta-sheet formation. With an increase in solution concentration, the graft copolymers, except those with a low grafting ratio of m = 6, formed hydrogels displaying shear-thinning and self-healing behaviors because of the reversible self-assembly property of peptide grafts. Interestingly, the mechanical properties of hybrid graft copolymers were strongly dependent on the grafting density of the hybrid copolymers. Thus, it was observed that an increase in grafting ratio strengthened the inter-polymer network. These features enabled the graft-type hybrids to be used as injectable hydrogels for 3D cell scaffolds and controlled-release applications.