文献类型：期刊文献

英文题名：Controlled Hierarchical Self-Assembly of Catenated Cages

作者：Sun, Zhongwei[1];Li, Pan[1];Xu, Shijun[2];Li, Zi-Ying[2];Nomura, Yoshiaki[1];Li, Zimu[1];Liu, Xiaoyun[2];Zhang, Shaodong[1]

机构：[1]Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Frontiers Sci Ctr Transformat Mol, Shanghai Key Lab Elect Insulat & Thermal Aging, Shanghai 200240, Peoples R China;[2]East China Univ Sci & Technol, Key Lab Specially Funct Polymer Mat & Related Tec, Minist Educ, Shanghai 200237, Peoples R China

年份：2020

卷号：142

期号：24

起止页码：10833

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20202708887975);WOS:【SCI-EXPANDED(收录号:WOS:000542929600028)】；

基金：This work was supported by National Natural Science Foundation of China (key program 21890733), and the Shanghai Natural Science Foundation (18ZR1420800). We thank Dr. Hang Wang (MALDI-TOF MS) and Wanping Lu (Supercritical Fluid Chromatography) at the Instrumental Analysis Centre of SJTU and Rongrong Yu for his assistance in chiral HPLC characterization. We thank Dr. Shan Jiang from ShanghaiTech University for constructive discussion and suggestions.

语种：英文

外文关键词：Self assembly

摘要：Constructing hierarchical superstructures to achieve comparable complexity and functions to proteins with four-level hierarchy is challenging, which relies on the elaboration of novel building blocks with complex structures. We present a series of catenated cages with unique structural complexity and tailorability. The rational design was realized as such: A catenane of two symmetric cages (CSC), CSC-1, with all rigid imine panels was converted to a catenane of two dissymmetric cages (CDC), CDC-1, with two exterior flexible amine panels, and CDC-5 was tailored from CDC-1 by introducing an additional methyl group on each blade to increase lateral hindrance. CDC-1s with the most irregular and flexible configuration formed supramolecular dimers, which self-organized into 3D continuous wavelike plank with a three-level hierarchy, previously undiscovered by conventional building blocks. A drastically different 3D triclinic crystalline phase with a four-level hierarchy and trigonal phase with a three-level hierarchy were constructed of distorted CSC-1s and the most symmetric CDC-5s, respectively. The wavelike plank exhibited the lowest order, and the triclinic phase had a lower order than the trigonal phase which had the highest order. It correlates with the configuration of the primary structures, namely, the most disordered shape of CDC-1, the low-order configuration of CSC-1, and the most ordered geometry of CDC-5. The catenated cages with subtle structural differences therefore provide a promising platform for the search of emerging hierarchical superstructures that might be applied to proton conductivity, ferroelectricity, and catalysis.