Self-assembly of metal-organic polyhedra into supramolecular polymers with intrinsic microporosity

Nature Communications
Arnau Carné-SánchezShuhei Furukawa

Abstract

Designed porosity in coordination materials often relies on highly ordered crystalline networks, which provide stability upon solvent removal. However, the requirement for crystallinity often impedes control of higher degrees of morphological versatility, or materials processing. Herein, we describe a supramolecular approach to the synthesis of amorphous polymer materials with controlled microporosity. The strategy entails the use of robust metal-organic polyhedra (MOPs) as porous monomers in the supramolecular polymerization reaction. Detailed analysis of the reaction mechanism of the MOPs with imidazole-based linkers revealed the polymerization to consist of three separate stages: nucleation, elongation, and cross-linking. By controlling the self-assembly pathways, we successfully tuned the resulting macroscopic form of the polymers, from spherical colloidal particles to colloidal gels with hierarchical porosity. The resulting materials display distinct microporous properties arising from the internal cavity of the MOPs. This synthetic approach could lead to the fabrication of soft, flexible materials with permanent porosity.

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Jul 31, 2019·Chemical Society Reviews·Liang FengHong-Cai Zhou
Nov 7, 2019·Chemistry : a European Journal·Miguel A AndrésIgnacio Gascón
Mar 14, 2020·Chemical Communications : Chem Comm·Jun ZhaoXuzhou Yan
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Nov 12, 2020·Chemical Communications : Chem Comm·Zhuxiu ZhangXu Qiao
Jan 14, 2021·Chemical Communications : Chem Comm·Yufeng HuoZhanhu Guo
Feb 23, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Meaghan M Deegan, Eric D Bloch
Mar 2, 2021·Journal of the American Chemical Society·Alexandre LegrandShuhei Furukawa
Mar 21, 2021·Chemistry, an Asian Journal·Chao LiuQi An
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Mar 17, 2021·Angewandte Chemie·Jesús Á Martín-IllánFélix Zamora
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Jun 11, 2020·Chemical Reviews·Aeri J GosselinEric D Bloch

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Methods Mentioned

BETA
nuclear magnetic resonance
scanning electron microscopy
X-ray

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