文献类型：期刊文献

英文题名：Assembling a Natural Small Molecule into a Supramolecular Network with High Structural Order and Dynamic Functions

作者：Zhang, Qi[1,2];Deng, Yuan-Xin[1,2];Luo, Hong-Xi[3];Shi, Chen-Yu[1,2];Geise, Geoffrey M.[3];Feringa, Ben L.[1,2,4,5];Tian, He[1,2];Qu, Da-Hui[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Feringa Nobel Prize Scientist Joint Res Ctr, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Feringa Nobel Prize Scientist Joint Res Ctr, Joint Int Res Lab Precis Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Univ Virginia, Dept Chem Engn, 102 Engineers Way,POB 400741, Charlottesville, VA 22904 USA;[4]Univ Groningen, Fac Math & Nat Sci, Stratingh Inst Chem, Ctr Syst Chem, Nijenborgh 4, NL-9747 AG Groningen, Netherlands;[5]Univ Groningen, Fac Math & Nat Sci, Zernike Inst Adv Mat, Nijenborgh 4, NL-9747 AG Groningen, Netherlands

年份：2019

卷号：141

期号：32

起止页码：12804

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20193407324683);WOS:【SCI-EXPANDED(收录号:WOS:000481563500048)】；

基金：This work was supported by National Natural Science Foundation of China (Grants 21788102, 21790361, 21871084, 21672060, and 21421004), Shanghai Municipal Science and Technology Major Project (Grant 2018SHZDZX03), the Fundamental Research Funds for the Central Universities, the Programme of Introducing Talents of Discipline to Universities (Grant B16017), Program of Shanghai Academic/Technology Research Leader (19XD1421100), and the Shanghai Science and Technology Committee (Grant 17520750100). Geoffrey M. Geise appreciates the support of National Science Foundation under Grant CBET-1752048. Ben L. Feringa acknowledges financial support of The Netherlands Ministry of Education, Culture, and Science (Gravitation program 024.601035). We appreciate Dr. Na Li (BL19U2 beamline of Shanghai Synchrotron Radiation Facility) for her kind help in synchrotron SAXS test and Miss Qi Wei and Prof. Zhijun Ning (ShanghaiTech University) for their kind help in GIWAXS experiments. We thank the Research Center of Analysis and Test of East China University of Science and Technology for help on the material characterization.

语种：英文

外文关键词：Biological systems - Molecules - Costs - Network layers - Hierarchical systems - Ring opening polymerization - X ray scattering

摘要：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.