Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, State Key Laboratory of Molecular Engineering of Polymers, Department of Chemistry, Fudan University, Shanghai 200433, P.R. China.
State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, Shanghai 200032 P.R. China.
J Am Chem Soc. 2021 Jan 20;143(2):1119-1125. doi: 10.1021/jacs.0c11925. Epub 2020 Dec 31.
Two molecular metalla-knots containing over 500 non-hydrogen atoms (especially 16 Rh ions) and one molecular Borromean ring were obtained in high yields facilitated by multiple intermolecular interactions between their components. The syntheses rely on the strategic selection of the nonlinear dipyridyl ligand 2,7-di(pyridin-4-yl)-9-fluorene () as precursor, and the structures of the assemblies were confirmed by detailed X-ray crystallographic analysis. Subsequently, replacing with the bulkier ligand 4,4'-(9,9-dimethyl-9-fluorene-2,7-diyl)dipyridine () led to the formation of three tetranuclear metallocycles in high yields on account of the weakened π-π stacking interactions between the naphthacene/anthracene and fluorene moieties, which in turn confirmed the significance of stacking interactions in the construction of the molecular 8 metalla-knots and the molecular Borromean ring.
两个含有超过 500 个非氢原子（特别是 16 个 Rh 离子）的分子金属纽结和一个分子博洛米安环在多种分子间相互作用的促进下以高产率得到。这些合成依赖于非线性二吡啶配体 2,7-二（吡啶-4-基）-9-芴（）作为前体的战略选择，并且通过详细的 X 射线晶体学分析证实了组装体的结构。随后，用更大体积的配体 4,4'-(9,9-二甲基-9-芴-2,7-二基)二吡啶（）取代，由于萘/蒽和芴部分之间的 π-π 堆积相互作用减弱，从而以高产率形成了三个四核金属环，这反过来又证实了堆积相互作用在分子 8 金属纽结和分子博洛米安环的构建中的重要性。
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