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Cooperative Allosteric Transitions

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Aromatic copolyimides with varying ether-ketone and ether-sulfone linkages exhibit distinct binding affinities for pyrene-based tweezer-molecules. These differences stem from conformational variations influencing secondary π-π-stacking interactions.

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Area of Science:

  • Polymer Chemistry
  • Supramolecular Chemistry
  • Materials Science

Background:

  • High molecular weight aromatic copolyimides feature pyromellitimide units.
  • These units are flanked by ether-ketone (K) or ether-sulfone (S) residues, forming triplet sequences like KIK, KIS, and SIS.
  • Pyrene-based tweezer-molecules bind to these polymers via π-π-stacking and hydrogen bonding.

Purpose of the Study:

  • To investigate the varying binding strengths of pyrene-based tweezer-molecules to different aromatic copolyimide triplet sequences.
  • To elucidate the molecular mechanisms governing these binding affinities.
  • To correlate structural features of the copolyimides with their binding capabilities.

Main Methods:

  • Nuclear Magnetic Resonance (NMR) spectroscopy to measure complexation shifts.
  • Determination of tweezer-polymer binding constants.
  • Computational modeling of tweezer-polymer interactions.
  • Single-crystal X-ray diffraction analysis of tweezer-complexes.

Main Results:

  • The binding strength follows the order: SIS > KIS > KIK.
  • (1)H NMR complexation shifts and binding constants quantify these differences.
  • Computational models and X-ray crystallography reveal that conformational preferences at diarylketone and diarylsulfone linkages are key.
  • These preferences dictate the occurrence of chain-folding and secondary π-π-stacking.

Conclusions:

  • The conformational flexibility of aromatic rings in ether-ketone and ether-sulfone linkages significantly impacts tweezer-molecule binding.
  • Secondary π-π-stacking interactions play a crucial role in the observed binding strength variations.
  • Understanding these structure-property relationships enables the design of advanced supramolecular materials.