Pathway complexity in fibre assembly: from liquid crystals to hyper-helical gelmorphs.
Pathway complexity in fibre assembly: from liquid crystals to hyper-helical gelmorphs.
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DOI：
10.1039/d3sc03841f
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发表时间：
2023-10-25
期刊：
影响因子：
8.4
通讯作者：
Steed, Jonathan W.
中科院分区：
文献类型：
--
作者：
Contreras-Montoya, Rafael;Smith, James P.;Boothroyd, Stephen C.;Aguilar, Juan A.;Mirzamani, Marzieh;Screen, Martin A.;Yufit, Dmitry S.;Robertson, Mark;He, Lilin;Qian, Shuo;Kumari, Harshita;Steed, Jonathan W.
路径复杂性导致相同组件根据装配条件产生独特的材料。在这里，手性酰基氨基脲凝胶根据组装途径形成三种不同纤维形态的凝胶（称为“凝胶”）以及溶性液晶液滴。凝胶具有超螺旋（HH-Gel），带纤维（TF-Gel）或来自液晶相的薄纤维（lc - gel）的形态，并表现出非常不同的流变性能。凝胶在溶液中以三个缓慢相互转换的构象存在。这三种凝胶都由不对称的分子内氢键构象组成。动力学表明，显著的hh -凝胶的形成是协同的，并且假定涉及生长的纤维与非胶凝构象的结合。这个单分子动态构象库显示了在组装过程中由于紧急相互作用而产生的通路复杂性如何产生具有不同形态的非常不同的材料，从而产生非常不同的材料特性。路径复杂性导致相同组件根据装配条件产生独特的材料。
Pathway complexity results in unique materials from the same components according to the assembly conditions. Here a chiral acyl-semicarbazide gelator forms three different gels of contrasting fibre morphology (termed ‘gelmorphs’) as well as lyotropic liquid crystalline droplets depending on the assembly pathway. The gels have morphologies that are either hyperhelical (HH-Gel), tape-fibre (TF-Gel) or thin fibril derived from the liquid crystalline phase (LC-Gels) and exhibit very different rheological properties. The gelator exists as three slowly interconverting conformers in solution. All three gels are comprised of an unsymmetrical, intramolecular hydrogen bonded conformer. The kinetics show that formation of the remarkable HH-Gel is cooperative and is postulated to involve association of the growing fibril with a non-gelling conformer. This single molecule dynamic conformational library shows how very different materials with different morphology and hence very contrasting materials properties can arise from pathway complexity as a result of emergent interactions during the assembly process. Pathway complexity results in unique materials from the same components according to the assembly conditions.
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