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Heteromeric Completive Self-Sorting in Coordination Cage Systems.

Elie Benchimol1, Irene Regeni1, Bo Zhang1

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Area of Science:

  • Coordination chemistry
  • Supramolecular chemistry
  • Materials science

Background:

  • Heteroleptic coordination cages are assembled from multiple ligand types.
  • Existing methods include statistical mixing or cage-to-cage transformations.
  • Control over heteroleptic cage formation remains a challenge.

Purpose of the Study:

  • To introduce and demonstrate 'heteromeric completive self-sorting' in coordination cage systems.
  • To explore the controllable coexistence of distinct heteroleptic cages.
  • To investigate the role of ligand ratios and enthalpic factors in self-sorting outcomes.

Main Methods:

  • Utilizing cage-to-cage transformations from homoleptic precursors.
  • Employing a systems chemistry approach with varying ligand ratios.
  • Characterization via Nuclear Magnetic Resonance (NMR) and Mass Spectrometry (MS).
  • Structural elucidation using single-crystal X-ray diffraction.

Main Results:

  • Demonstrated coexistence of two distinct heteroleptic cages (Pd2A2B2 and Pd2A2C2) through heteromeric completive self-sorting.
  • Showed control over self-sorting outcome by varying ligand ratios, transitioning from integrative to completive self-sorting.
  • Obtained crystal structures revealing diverse ligand arrangements (trans-figure-of-eight, cis-edges, single edge) dictated by cage composition.

Conclusions:

  • Heteromeric completive self-sorting offers a new level of control over heteroleptic cage populations.
  • Enthalpic factors are crucial but controllable determinants of self-sorting.
  • This work enables future applications in information processing, adaptive selectivity, and responsive catalysis.