吉林大学杨英威团队报道了通过客体诱导的分子间相互作用进行自底向上的固态分子组装。相关研究成果于2021年11月24日发表在国际顶尖学术期刊《美国化学会杂志》。

与溶液中相比，在固态中操纵分子运动从混沌中构建高度有序的超分子结构被认为是更复杂和更具挑战性的。

该文中，研究人员基于新设计的骨架修饰柱[5]芳烃类似物，即二甲基化leggero柱[5]芳烃MeP[5]L，开发了一种固态下的自底向上的分子组装方法。MeP[5]L的无定形粉末可吸收某些客体蒸汽以形成各种含有固态分子组装体的有序连接体，其可进一步用于在加热时构建热力学上有利的无连接体上部结构。

该方法由蒸汽诱导的固态分子运动驱动，随后是热触发的相-相转变。分子间的相互作用在控制最终组装体中的分子排列方面起着至关重要的作用。该研究将为探索固态可控分子运动和组装开辟新的视角，为超分子化学和材料提供新的视角。

附：英文原文

Title: Bottom-Up Solid-State Molecular Assembly via Guest-Induced Intermolecular Interactions

Author: Jia-Rui Wu, Zhi Cai, Gengxin Wu, Dihua Dai, Yu-Qing Liu, Ying-Wei Yang

Issue&Volume: November 24, 2021

Abstract: 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 MeP[5]L, is developed in the solid state. An amorphous powder of MeP[5]L 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.

DOI: 10.1021/jacs.1c10139

Source: https://pubs.acs.org/doi/10.1021/jacs.1c10139