An Unprecedented Stimuli-Controlled Single-Crystal Reversible Phase Transition of a Metal-Organic Framework and Its Application to a Novel Method of Guest Encapsulation

Advanced Materials
Fangchang TanJosé Giner Planas

Abstract

The flexibility and unexpected dynamic behavior of a third-generation metal-organic framework are described for the first time. The synthetic strategy is based on the flexibility and spherical shape of dipyridyl-based carborane linkers that act as pillars between rigid Co/BTB (BTB: 1,3,5-benzenetricarboxylate) layers, providing a 3D porous structure (1). A phase transition of the solid can be induced to generate a new, nonporous 2D structure (2) without any loss of the carborane linkers. The structural transformation is visualized by snapshots of the multistep single-crystal-to-single-crystal transformation by single-crystal and powder X-ray diffraction. Poor hydrogen bond acceptors such as MeOH, CHCl3 or supercritical CO2 induce such a 3D to 2D transformation. Remarkably, the transformation is reversible and the 2D phase 2 is further converted back into 1 by heating in dimethylformamide. The energy requirements involved in such processes are investigated using periodic density functional theory calculations. As a proof of concept for potential applications, encapsulation of C60 is achieved by trapping this molecule during the reversible 2D to 3D phase transition, whereas no adsorption is observed by straight solvent diffusion ...Continue Reading

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Citations

Oct 9, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Elena OleshkevichClara Viñas
Sep 6, 2019·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Lei GanJosé G Planas
Sep 12, 2019·Advanced Science·Yuri A MezenovValentin A Milichko
Nov 8, 2019·Chemistry : a European Journal·Wen-Wen FanQiu-E Cao
Jul 2, 2020·Chemistry : a European Journal·Pablo Labra-VázquezRosario Núñez
Jan 14, 2021·Inorganic Chemistry·Nadine BönischStefan Kaskel
Dec 24, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Zhen LiJosé G Planas

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