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Steric Hindrance in Metal Coordination Drives the Separation of Pyridine Regioisomers Using Rhodium(II)‐Based Metal–Organic Polyhedra

Laura Hernández‐López, Jordi Martínez‐Esaín, Arnau Carné‐Sánchez, Thais Grancha, Jordi Faraudo, Daniel Maspoch

2021Angewandte Chemie International Edition28 citationsDOIOpen Access PDF

Abstract

Abstract The physicochemical similarity of isomers makes their chemical separation through conventional techniques energy intensive. Herein, we report that, instead of using traditional encapsulation‐driven processes, steric hindrance in metal coordination on the outer surface of Rh II ‐based metal–organic polyhedra (Rh‐MOPs) can be used to separate pyridine‐based regioisomers via liquid–liquid extraction. Through molecular dynamics simulations and wet experiments, we discovered that the capacity of pyridines to coordinatively bind to Rh‐MOPs is determined by the positions of the pyridine substituents relative to the pyridine nitrogen and is influenced by steric hindrance. Thus, we exploited the differential solubility of bound and non‐bound pyridine regioisomers to engineer liquid–liquid self‐sorting systems. As a proof of concept, we separated four different equimolecular mixtures of regioisomers, including a mixture of the industrially relevant compounds 2‐chloropyridine and 3‐chloropyridine, isolating highly pure compounds in all cases.

Topics & Concepts

Structural isomerSteric effectsChemistryPyridineMetalSolubilityRhodiumOrganic chemistryComputational chemistryCatalysisMetal-Organic Frameworks: Synthesis and ApplicationsMagnetism in coordination complexesSupramolecular Chemistry and Complexes
Steric Hindrance in Metal Coordination Drives the Separation of Pyridine Regioisomers Using Rhodium(II)‐Based Metal–Organic Polyhedra | Litcius