Shi Yadong, Wang Shuodong, Tao Wei, Guo Jingjing, Xie Sheng, Ding Yanglan, Xu Guoyong, Chen Cheng, Sun Xiaoyu, Zhang Zengming, He Zikai, Wei Peifa, Tang Ben Zhong
Institutes of Physical Science and Information Technology, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui Graphene Engineering Laboratory, Anhui University, Hefei, 230601, China.
State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China.
Nat Commun. 2022 Apr 6;13(1):1882. doi: 10.1038/s41467-022-29565-1.
The development of new strategies to construct on-demand porous lattice frameworks from simple motifs is desirable. However, mitigating complexity while combing multiplicity and reversibility in the porous architectures is a challenging task. Herein, based on the synergy of dynamic intermolecular interactions and flexible molecular conformation of a simple cyano-modified tetraphenylethylene tecton, eleven kinetic-stable hydrogen-bonded organic frameworks (HOFs) with various shapes and two thermo-stable non-porous structures with rare perpendicular conformation are obtained. Multimode reversible structural transformations along with visible fluorescence output between porous and non-porous or between different porous forms is realized under different external stimuli. Furthermore, the collaborative of flexible framework and soft long-chain guests facilitate the relaxation from intrinsic blue emission to yellow emission in the excited state, which represents a strategy for generating white-light emission. The dynamic intermolecular interactions, facilitated by flexible molecular conformation and soft guests, diversifies the strategies of construction of versatile smart molecular frameworks.
开发从简单结构单元构建按需多孔晶格框架的新策略是很有必要的。然而，在多孔结构中结合多样性和可逆性的同时减轻复杂性是一项具有挑战性的任务。在此，基于简单的氰基修饰四苯乙烯结构单元的动态分子间相互作用和灵活的分子构象协同作用，获得了十一种具有各种形状的动力学稳定氢键有机框架（HOF）和两种具有罕见垂直构象的热稳定无孔结构。在不同外部刺激下，实现了多孔与无孔之间或不同多孔形式之间的多模式可逆结构转变以及可见荧光输出。此外，柔性框架与软长链客体的协同作用促进了激发态下从固有蓝色发射到黄色发射的弛豫，这代表了一种产生白光发射的策略。由灵活的分子构象和软客体促进的动态分子间相互作用，使构建多功能智能分子框架的策略多样化。
