Hydrophobic Shielding of Outer Surface: Enhancing the Chemical Stability of Metal–Organic Polyhedra

Metal–organic polyhedra (MOP) are a promising class of crystalline porous materials with multifarious potential applications. Although MOPs and metal–organic frameworks (MOFs) have similar potential in terms of their intrinsic porosities and physicochemical properties, the exploitation of carboxylat...

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Bibliographic Details
Published in:Angewandte Chemie 2019-01, Vol.131 (4), p.1053-1057
Main Authors: Mollick, Samraj, Mukherjee, Soumya, Kim, Dongwook, Qiao, Zhiwei, Desai, Aamod V., Saha, Rajat, More, Yogeshwar D., Jiang, Jianwen, Lah, Myoung Soo, Ghosh, Sujit K.
Format: Article
Language:English
Subjects:
Acidic oxides
Ambient temperature
Chemistry
Corrosion resistance
Exploitation
Fabrication
Hydrophobicity
Hydrophobie
Kupfer
Metal-organic frameworks
Metall-organische Polyeder
Metals
Molecular modelling
Mopping
Organic chemistry
Oxidation
Physicochemical properties
Polyhedra
Porous materials
Poröse Materialien
Shielding
Stability
Strukturaufklärung
Surface stability
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Summary:Metal–organic polyhedra (MOP) are a promising class of crystalline porous materials with multifarious potential applications. Although MOPs and metal–organic frameworks (MOFs) have similar potential in terms of their intrinsic porosities and physicochemical properties, the exploitation of carboxylate MOPs is still rudimentary because of the lack of systematic development addressing their chemical stability. Herein we describe the fabrication of chemically robust carboxylate MOPs via outer‐surface functionalization as an a priori methodology, to stabilize those MOPs system where metal–ligand bond is not so strong. Fine‐tuning of hydrophobic shielding is key to attaining chemical inertness with retention of the framework integrity over a wide range of pH values, in strong acidic conditions, and in oxidizing and reducing media. These results are further corroborated by molecular modelling studies. Owing to the unprecedented transition from instability to a chemically ultra‐stable regime using a rapid ambient‐temperature gram‐scale synthesis (within seconds), a prototype strategy towards chemically stable MOPs is reported. Systematische Stabilität: Es besteht ein Zusammenhang zwischen Hydrophobie und chemischer Beständigkeit für Metall‐organische Polyeder (MOPs). Für Käfige mit ähnlichem Kern folgt eine höhere chemische Beständigkeit aus der inkrementellen Hydrophobie der Oberfläche. Dies zeigt sich in strukturellen Charakterisierungen und Simulationsdaten.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.201811037