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Guest-dependent isomer convergence of a permanently fluxional coordination cage

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dc.contributor.authorBirve, A.
dc.contributor.authorPatel, H.D.
dc.contributor.authorPrice, J.R.
dc.contributor.authorBloch, W.M.
dc.contributor.authorFallon, T.
dc.date.issued2022
dc.descriptionFirst published: 01 December 2021
dc.description.abstractA fluxional bis-monodentate ligand, based on the archetypal shape-shifting molecule bullvalene, self-assembles with M2+ (M = Pd2+ or Pt2+) to produce a highly complex ensemble of permanently fluxional coordination cages. Metal-mediated self-assembly selects for an M2L4 architecture while maintaining shape-shifting ligand complexity. A second level of simplification is achieved with guest-exchange; the binding of halides within the M2L4 cage mixture results in a convergence to a cage species with all four ligands present as the "B isomer". Within this confine, the reaction graph of the bullvalene is greatly restricted, but gives rise to a mixture of 38 possible diastereoisomers in rapid exchange. X-ray crystallography reveals a preference for an achiral form consisting of both ligand enantiomers. Through a combination of NMR spectroscopy and DFT calculations, we elucidate the restricted isomerisation pathway of the permanently fluxional M2L4 assembly.
dc.description.statementofresponsibilityAndré P. Birvé, Harshal D. Patel, Jason R. Price, Witold M. Bloch, Thomas Fallon
dc.identifier.citationAngewandte Chemie International Edition, 2022; 61(9):e202115468-1-e202115468-6
dc.identifier.doi10.1002/anie.202115468
dc.identifier.issn1433-7851
dc.identifier.issn1521-3773
dc.identifier.orcidPatel, H.D. [0000-0003-1900-0505]
dc.identifier.orcidBloch, W.M. [0000-0003-1084-1287]
dc.identifier.orcidFallon, T. [0000-0002-6495-5282]
dc.identifier.urihttps://hdl.handle.net/2440/134230
dc.language.isoen
dc.publisherWiley
dc.relation.granthttp://purl.org/au-research/grants/arc/DE190100327
dc.rights© 2021The Authors.Angewandte Chemie International Edition published by Wiley-VCHGmbH.This is an open access article under the terms of the Creative Commons Attribution Non-Commercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes
dc.source.urihttps://doi.org/10.1002/anie.202115468
dc.subjectconvergence * coordination cage * fluxional molecule * host-guest chemistry * self-assembly
dc.titleGuest-dependent isomer convergence of a permanently fluxional coordination cage
dc.typeJournal article
pubs.publication-statusPublished

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