期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 9, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202115468
关键词
Convergence; Coordination cage; Fluxional molecule; Host-guest chemistry; Self-assembly
资金
- Australian Research Council [DE190100327]
- New Zealand Marsden Fund (Fast Start Grant) [15-MAU-154]
- AINSE Honours Scholarship
- Australian Research Council [DE190100327] Funding Source: Australian Research Council
A fluxional bis-monodentate ligand, based on the bullvalene molecule, self-assembles with M2+ to produce complex coordination cages. Guest-exchange simplifies the system, leading to a mixture of 38 diastereoisomers. NMR spectroscopy and DFT calculations elucidate the isomerization pathway.
A 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.
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