Silk self-assembly mechanisms and control from thermodynamics to kinetics.
Silk self-assembly mechanisms and control from thermodynamics to kinetics.
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DOI：
10.1021/bm201731e
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发表时间：
2012-03-12
影响因子：
6.2
通讯作者：
Kaplan, David L.
中科院分区：
文献类型：
--
作者：
Lu, Qiang;Zhu, Hesun;Zhang, Cencen;Zhang, Feng;Zhang, Bing;Kaplan, David L.
蚕和蜘蛛产生的纤维具有很高的强度和延展性。涉及将丝蛋白加工成纤维形式的潜在机制仍不完全清楚，导致未能完全概括体外再生丝溶液中天然纤维的显着特性。本研究通过模拟天然纺丝工艺，使再生丝具有良好的延伸性和高强度。胶束内的构象转变，随后由胶束的聚集和它们的稳定，因为它们涉及到丝的亚稳结构进行了描述。随后，阐明了控制纳米纤维结构形成的机制。结果表明，丝在水溶液中的自组装是一个动力学驱动的过程，动力学也起着关键作用。四个关键因素，分子的流动性，电荷，亲水相互作用和浓度的基础上的过程。调整这些因素可以平衡纳米结构和构象组成，并用于获得具有与天然纤维相当的性质的丝基材料。这些机制为设计丝基多功能材料提供了新的方向。
Silkworms and spiders generate fibres that exhibit high strength and extensibility. The underlying mechanisms involved in processing silk proteins into fiber form remain incompletely understood, resulting in the failure to fully recapitulate the remarkable properties of native fibers in vitro from regenerated silk solutions. In the present study, the extensibility and high strength of regenerated silks were achieved by mimicking the natural spinning process. Conformational transitions inside micelles, followed by aggregation of micelles and their stabilization as they relate to the metastable structure of silk are described. Subsequently, the mechanisms to control the formation of nanofibrous structures were elucidated. The results clarify that the self-assembly of silk in aqueous solution is a thermodynamically driven process where kinetics also play a key role. Four key factors, molecular mobility, charge, hydrophilic interactions and concentration underlie the process. Adjusting these factors can balance nanostructure and conformational composition, and be used to achieve silk-based materials with properties comparable to native fibers. These mechanisms suggest new directions to design silk-based multifunctional materials.
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