当前位置: X-MOL 学术J. Am. Chem. Soc. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Assembling a natural small molecule into a supramolecular network with high structural order and dynamic functions
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2019-07-26 , DOI: 10.1021/jacs.9b05740
Qi Zhang 1 , Yuan-Xin Deng 1 , Hong-Xi Luo 2 , Chen-Yu Shi 1 , Geoffrey M Geise 2 , Ben L Feringa 1, 3 , He Tian 1 , Da-Hui Qu 1
Affiliation  

Programming the hierarchical self-assembly of small molecules has been a fundamental topic of great significance in biological systems and artificial supramolecular systems. Precise and highly programmed self-assembly can produce supramolecular architectures with distinct structural features. However, it still remains a challenge how to precisely control the self-assembly pathway in a desirable way by introducing abundant structural information into a limited molecular backbone. Here we disclose a strategy that directs the hierarchical self-assembly of sodium thioctate, a small molecule of biological origin, into a highly ordered supramolecular layered network. By combining the unique dynamic covalent ring-opening-polymerization of sodium thioctate and an evaporation-induced interfacial confinement effect, we precisely direct the dynamic supramolecular self-assembly of this simple small molecule in a scheduled hierarchical pathway, resulting in a layered structure with long-range order at both macroscopic and molecular scales, which is revealed by small-angle and wide-angle X-ray scattering technologies. The resulting supramolecular layers are found to be able to bind water molecules as structural water, which works as an interlayer lubricant to modulate the material properties, such as mechanical performance, self-healing capability, and actuating function. Analogous to many reversibly self-assembled biological systems, the highly dynamic polymeric network can be degraded into monomers and reformed by a water-mediated route, exhibiting full recyclability in a facile, mild, and environmentally friendly way. This approach for assembling commercial small molecules into structurally complex materials paves the way for low-cost functional supramolecular materials based on synthetically simple procedures.

中文翻译:

将天然小分子组装成具有高度结构有序和动态功能的超分子网络

对小分子的分层自组装进行编程一直是生物系统和人工超分子系统中具有重要意义的基础课题。精确且高度程序化的自组装可以产生具有独特结构特征的超分子结构。然而,如何通过将丰富的结构信息引入有限的分子骨架,以理想的方式精确控制自组装途径仍然是一个挑战。在这里,我们公开了一种策略,将硫辛酸钠(一种生物来源的小分子)的分层自组装引导到高度有序的超分子层状网络中。通过结合硫辛酸钠独特的动态共价开环聚合和蒸发诱导的界面限制效应,我们精确地将这种简单小分子的动态超分子自组装引导到预定的分层路径中,从而在宏观和分子尺度上形成具有长程有序的分层结构,小角度和广角 X-射线散射技术。发现由此产生的超分子层能够将水分子结合为结构水,作为层间润滑剂来调节材料性能,如机械性能、自愈能力和驱动功能。类似于许多可逆自组装生物系统,高动态聚合物网络可以降解为单体并通过水介导的途径进行改造,以一种简便、温和且环保的方式表现出完全的可回收性。
更新日期:2019-07-26
down
wechat
bug