Covalent Capture of Aligned Self-Assembling Nanofibers.
Covalent Capture of Aligned Self-Assembling Nanofibers.
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DOI：
10.1021/jacs.7b04655
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发表时间：
2017-06-14
影响因子：
15
通讯作者：
Hartgerink JD
中科院分区：
文献类型：
--
作者：
Li IC;Hartgerink JD
大量的努力已经投入到自发组装成纳米纤维的系统的设计和表征。这些系统是有趣的基础超分子化学，也已被证明是有前途的材料，特别是在生物医学应用。多结构域肽就是这样一种组装器，在以前的工作中，我们已经证明了它们在温和和容易控制的条件下组装的可逆性，沿着它们在时间控制的药物递送、蛋白质递送、细胞包封和细胞递送应用中的效用。此外，它们高度兼容的序列选择标准允许它们被修改以并入蛋白酶敏感性和用于细胞粘附和血管生成的生物识别基序。然而，其组装的控制一直限于无序纳米纤维的形成。在这项工作中，我们扩大了我们的能力，操纵多结构域肽组装成平行排列的纤维束。尽管这种比对是通过注射器递送的剪切力实现的，但它也依赖于多结构域肽的氨基酸序列。氨基酸DOPA（3，4-二羟基苯丙氨酸）的掺入允许自组装纳米纤维在适度剪切应力下形成各向异性水凝胶串。水凝胶线显示出显著的双折射，并且在扫描电子显微镜中可以看到高度对齐的纳米纤维。此外，由DOPA氧化诱导的共价键允许共价捕获对齐的双折射束，增强其双折射和结构完整性。
A great deal of effort has been invested in the design and characterization of systems which spontaneously assemble into nanofibers. These systems are interesting for their fundamental supramolecular chemistry and have also been shown to be promising materials, particularly for biomedical applications. Multidomain peptides are one such assembler, and in previous work we have demonstrated the reversibility of their assembly under mild and easily controlled conditions, along with their utility for time-controlled drug delivery, protein delivery, cell encapsulation, and cell delivery applications. Additionally, their highly compliant criteria for sequence selection allows them to be modified to incorporate protease susceptibility and biological-recognition motifs for cell adhesion and angiogenesis. However, control of their assembly has been limited to the formation of disorganized nanofibers. In this work, we expand our ability to manipulate multidomain-peptide assembly into parallel-aligned fiber bundles. Albeit this alignment is achieved by the shearing forces of syringe delivery, it is also dependent on the amino acid sequence of the multidomain peptide. The incorporation of the amino acid DOPA (3,4-dihydroxyphenylalanine) allows the self-assembled nanofibers to form an anisotropic hydrogel string under modest shear stress. The hydrogel string shows remarkable birefringence, and highly aligned nanofibers are visible in scanning electronic microscopy. Furthermore, the covalent linkage induced by DOPA oxidation allows covalent capture of the aligned nanofiber bundles, enhancing their birefringence and structural integrity.