International Joint Research Laboratory of Nano-Micro Architecture Chemistry, College of Chemistry, Jilin University, 2699 Qianjin Street, Changchun 130012, People's Republic of China.
Key Laboratory of Automobile Materials of Ministry of Education and School of Materials Science and Engineering, Jilin University, 5988 Renmin Street, Changchun 130025, People's Republic of China.
J Am Chem Soc. 2021 Dec 8;143(48):20395-20402. doi: 10.1021/jacs.1c10139. Epub 2021 Nov 24.
The manipulation of molecular motions to construct highly ordered supramolecular architectures from chaos in the solid state is considered to be far more complex and challenging in comparison to that in solution. In this work, a bottom-up molecular assembly approach based on a newly designed skeleton-trimmed pillar[5]arene analogue, namely the permethylated leggero pillar[5]arene , is developed in the solid state. An amorphous powder of can take up certain guest vapors to form various ordered linker-containing solid-state molecular assemblies, which can be further used to construct a thermodynamically favored linker-free superstructure upon heating. These approaches are driven by vapor-induced solid-state molecular motions followed by a thermally triggered phase-to-phase transformation. The intermolecular interactions play a crucial role in controlling the molecular arrangements in the resulting assemblies. This research will open new insights into exploring controllable molecular motions and assemblies in the solid state, providing new perspectives in supramolecular chemistry and materials.
从混沌到高度有序的超分子结构的分子运动操控被认为在固态下比在溶液中要复杂和具有挑战性得多。在这项工作中，我们开发了一种基于新设计的骨架修剪的柱[5]芳烃类似物，即全甲基化的 Leggero 柱[5]芳烃的自下而上的分子组装方法。可以将无定形粉末吸收某些客体蒸气以形成各种具有有序连接体的固态分子组装体，这些组装体在加热时可以进一步用于构建热力学有利的无连接体超结构。这些方法是由蒸气诱导的固态分子运动驱动的，然后是热触发的相到相转变。分子间相互作用在控制所得组装体中的分子排列中起着至关重要的作用。这项研究将为探索固态中可控的分子运动和组装提供新的见解，为超分子化学和材料学提供新的视角。
