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Self-assembled hydrogel fiber bundles from oppositely charged polyelectrolytes mimic micro-/nanoscale hierarchy of collagen

机译：来自带相反电荷的聚电解质的自组装水凝胶纤维束模拟胶原的微米/纳米尺度层次

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摘要

Fiber bundles are present in many tissues throughout the body. In most cases,collagen subunits spontaneously self-assemble into a fibrilar structure thatprovides ductility to bone and constitutes the basis of muscle contraction.Translating these natural architectural features into a biomimetic scaffold stillremains a great challenge. Here, a simple strategy is proposed to engineerbiomimetic fiber bundles that replicate the self-assembly and hierarchy ofnatural collagen fibers. The electrostatic interaction of methacrylated gellangum with a countercharged chitosan polymer leads to the complexation of thepolyelectrolytes. When directed through a polydimethylsiloxane channel, thepolyelectrolytes form a hierarchical fibrous hydrogel demonstrating nanoscaleperiodic light/dark bands similar to D-periodic bands in native collagen andalign parallel fibrils at microscale. Importantly, collagen-mimicking hydrogelfibers exhibit robust mechanical properties (MPa scale) at a single fiber bundlelevel and enable encapsulation of cells inside the fibers under cell-friendly mildconditions. Presence of carboxyl- (in gellan gum) or amino- (in chitosan) functionalitiesfurther enables controlled peptide functionalization such as Arginylglycylasparticacid (RGD) for biochemical mimicry (cell adhesion sites) of nativecollagen. This biomimetic-aligned fibrous hydrogel system can potentially beused as a scaffold for tissue engineering as well as a drug/gene delivery vehicle.
机译：纤维束存在于全身的许多组织中。在大多数情况下，胶原蛋白亚基自发自组装成纤维状结构，可提供骨骼的延展性并构成肌肉收缩的基础。将这些天然建筑特征转化为仿生支架仍然是一个巨大的挑战。在这里，提出了一种简单的策略来模拟仿生纤维束，该纤维束可以复制天然胶原纤维的自组装和层次结构。甲基丙烯酸酯的胶球与带相反电荷的壳聚糖聚合物的静电相互作用导致聚电解质的络合。当被引导通过聚二甲基硅氧烷通道时，聚电解质形成分层的纤维水凝胶，其显示出类似于天然胶原中的D-周期性带的纳米级周期性的亮/暗带，并且在微观上对准平行的原纤维。重要的是，模仿胶原蛋白的水凝胶纤维在单纤维束水平上表现出强大的机械性能（MPa级），并且能够在对细胞友好的温和条件下将细胞包裹在纤维内。羧基（在吉兰糖胶中）或氨基（在壳聚糖中）的功能性的存在还使得受控的肽功能化，例如精氨酸的糖基糖基天冬氨酸（RGD）可以用于天然胶原蛋白的生物化学模拟（细胞粘附位点）。这种仿生排列的纤维水凝胶系统可以潜在地用作组织工程的支架以及药物/基因递送载体。

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