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Post‐Synthetic Modification Unlocks a 2D‐to‐3D Switch in MOF Breathing Response: A Single‐Crystal‐Diffraction Mapping Study

Elliot J. Carrington, Stephen F. Dodsworth, Sandra van Meurs, Mark R. Warren, Lee Brammer

2021Angewandte Chemie International Edition24 citationsDOIOpen Access PDF

Abstract

Abstract Post‐synthetic modification (PSM) of the interpenetrated diamondoid metal–organic framework (Me 2 NH 2 )[In(BDC‐NH 2 ) 2 ] (BDC‐NH 2 =aminobenzenedicarboxylate) SHF‐61 proceeds quantitatively in a single‐crystal‐to‐single‐crystal manner to yield the acetamide derivative (Me 2 NH 2 )[In(BDC‐NHC(O)Me) 2 ] SHF‐62 . Continuous breathing behaviour during activation/desolvation is retained upon PSM, but pore closing now leads to ring‐flipping to avert steric clash of amide methyl groups of the modified ligands. This triggers a reduction in the amplitude of the breathing deformation in the two dimensions associated with pore diameter, but a large increase in the third dimension associated with pore length. The MOF is thereby converted from predominantly 2D breathing (in SHF‐61 ) to a distinctly 3D breathing motion (in SHF‐62 ) indicating a decoupling of the pore‐width and pore‐length breathing motions. These breathing motions have been mapped by a series of single‐crystal diffraction studies.

Topics & Concepts

DiamondoidBreathingSingle crystalMaterials scienceCrystallographySteric effectsChemistryStereochemistryMoleculeOrganic chemistryAnatomyMedicineMetal-Organic Frameworks: Synthesis and ApplicationsCovalent Organic Framework ApplicationsMagnetism in coordination complexes
Post‐Synthetic Modification Unlocks a 2D‐to‐3D Switch in MOF Breathing Response: A Single‐Crystal‐Diffraction Mapping Study | Litcius