Department of Chemistry, Indian Institution of Science Education and Research Bhopal, Bhopal, 462066, Madhya Pradesh, India.
Angew Chem Int Ed Engl. 2023 Jun 5;62(23):e202219083. doi: 10.1002/anie.202219083. Epub 2023 Apr 3.
Dynamic covalent chemistry (DCC) opens up a fascinating route for the construction of well-organized supramolecular architectures, starting from organic molecular cages to crystalline macromolecular covalent organic frameworks (COFs). Herein, for the first time, we have manifested a facile room-temperature DCC-directed transformation of discrete organic imine cage-to-COF film at the liquid-liquid interface. The unfolding of the cage leading to the generation of imine intermediates, followed by their interface-assisted preorganization and subsequent growth of the COF film, are elucidated through detailed spectroscopic and microscopic investigations. The interfacial cage-to-COF transformation provides a facile route for the faster fabrication of free-standing COF films with high porosity and crystallinity, demonstrating excellent performance towards molecular sieving and high solvent permeance. Thus, the current study opens up a new route for structural interconversion between two crystalline entities with diverse dimensionality employing DCC at the confined interface.
动态共价化学（DCC）为构建组织良好的超分子结构开辟了一条引人入胜的途径，从有机分子笼到结晶的高分子共价有机框架（COF）。在此，我们首次在液-液界面展示了一种简便的室温 DCC 导向的离散有机亚胺笼到 COF 薄膜的转化。通过详细的光谱和显微镜研究阐明了笼的展开导致亚胺中间体的生成，然后是它们在界面辅助下的预组织和随后 COF 薄膜的生长。界面笼到 COF 的转化为具有高孔隙率和结晶度的独立 COF 薄膜的更快制造提供了一种简便途径，在分子筛和高溶剂透过率方面表现出优异的性能。因此，当前的研究为在受限界面处使用 DCC 在具有不同维度的两个结晶实体之间进行结构互变开辟了新途径。
