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Self-Assembled Hydrogel Fiber Bundles from Oppositely Charged Polyelectrolytes Mimic Micro-/Nanoscale Hierarchy of Collagen

机译：来自相反电荷的聚电解质的自组装水凝胶纤维束模仿胶原蛋白的微观/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 that provides ductility to bone and constitutes the basis of muscle contraction. Translating these natural architectural features into a biomimetic scaffold still remains a great challenge. Here, a simple strategy is proposed to engineer biomimetic fiber bundles that replicate the self-assembly and hierarchy of natural collagen fibers. The electrostatic interaction of methacrylated gellan gum with a countercharged chitosan polymer leads to the complexation of the polyelectrolytes. When directed through a polydimethylsiloxane channel, the polyelectrolytes form a hierarchical fibrous hydrogel demonstrating nanoscale periodic light/dark bands similar to D-periodic bands in native collagen and align parallel fibrils at microscale. Importantly, collagen-mimicking hydrogel fibers exhibit robust mechanical properties (MPa scale) at a single fiber bundle level and enable encapsulation of cells inside the fibers under cell-friendly mild conditions. Presence of carboxyl-(in gellan gum) or amino-(in chitosan) functionalities further enables controlled peptide functionalization such as Arginylglycylaspartic acid (RGD) for biochemical mimicry (cell adhesion sites) of native collagen. This biomimetic-aligned fibrous hydrogel system can potentially be used 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，胶原蛋白亚基自发地自我组装成纤维状结构，为骨骼提供延展性并构成肌肉收缩的基础。将这些自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设计仿生纤维束，该束能够复制天然胶原纤维的自组装和层次结构。甲基丙烯酸酯的结冷胶与带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。当直接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，显示出类似于天然胶原蛋白中D周期带的纳米级周期性亮/暗带，并在微米级排列平行的原纤维。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）的功能性进一步使受控的肽功能化（例如精氨酰糖基天冬氨酸（RGD））可用于天然胶原的生物化学模拟（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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  • 来源
    《Advanced Functional Materials》 |2017年第36期|1606273.1-1606273.10|共10页
  • 作者

    Sant Shilpa; Coutinho Daniela F.; Gaharwar Akhilesh K.; Neves Nuno M.; Reis Rui L.; Gomes Manuela E.; Khademhosseini Ali;

  • 作者单位

    Harvard Med Sch, Ctr Biomed Engn, Dept Med, Brigham & Womens Hosp, Cambridge, MA 02139 USA|MIT, Harvard Mit Div Hlth Sci & Technol, Cambridge, MA 02139 USA|Harvard Univ, Wyss Inst Biol Inspired Engn, Boston, MA 02115 USA|Univ Pittsburgh, Sch Pharm, Dept Pharmaceut Sci, Pittsburgh, PA 15261 USA|Univ Pittsburgh, Dept Bioengn, Swanson Sch Engn, Pittsburgh, PA 15261 USA|Univ Pittsburgh, McGowan Inst Regenerat Med, Pittsburgh, PA 15261 USA;

    Harvard Med Sch, Ctr Biomed Engn, Dept Med, Brigham & Womens Hosp, Cambridge, MA 02139 USA|MIT, Harvard Mit Div Hlth Sci & Technol, Cambridge, MA 02139 USA|Univ Minho, Headquarters European Inst Excellence Tissue Engn, Dept Polymer Engn, Res Grp Biomat Biodegradables & Biomimet 3Bs, Ave Pk, P-4805017 Barco, Guimaraes, Portugal|ICVS 3Bs PT Govt Associate Lab, Braga, Portugal;

    Harvard Med Sch, Ctr Biomed Engn, Dept Med, Brigham & Womens Hosp, Cambridge, MA 02139 USA|MIT, Harvard Mit Div Hlth Sci & Technol, Cambridge, MA 02139 USA|Harvard Univ, Wyss Inst Biol Inspired Engn, Boston, MA 02115 USA|Texas A&M Univ, Dept Biomed Engn, College Stn, TX 77841 USA|Texas A&M Univ, Dept Mat Sci & Engn, College Stn, TX 77841 USA;

    Univ Minho, Headquarters European Inst Excellence Tissue Engn, Dept Polymer Engn, Res Grp Biomat Biodegradables & Biomimet 3Bs, Ave Pk, P-4805017 Barco, Guimaraes, Portugal|ICVS 3Bs PT Govt Associate Lab, Braga, Portugal;

    Univ Minho, Headquarters European Inst Excellence Tissue Engn, Dept Polymer Engn, Res Grp Biomat Biodegradables & Biomimet 3Bs, Ave Pk, P-4805017 Barco, Guimaraes, Portugal|ICVS 3Bs PT Govt Associate Lab, Braga, Portugal;

    Univ Minho, Headquarters European Inst Excellence Tissue Engn, Dept Polymer Engn, Res Grp Biomat Biodegradables & Biomimet 3Bs, Ave Pk, P-4805017 Barco, Guimaraes, Portugal|ICVS 3Bs PT Govt Associate Lab, Braga, Portugal;

    MIT, Harvard Mit Div Hlth Sci & Technol, Cambridge, MA 02139 USA|Harvard Univ, Wyss Inst Biol Inspired Engn, Boston, MA 02115 USA;

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  • 正文语种 eng
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  • 关键词

    bottom-up self-assembly; chitosan and gellan gum; collagen mimicking; hierarchical hydrogel fibers; polyelectrolyte complexes;

    机译：自下而上的自组装;壳聚糖和结冷胶;模拟胶原;分层水凝胶纤维;聚电解质配合物;

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