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Modulating Supramolecular Charge-Transfer Interactions in the Solid State using Compressible Macrocyclic Hosts.

Jia-Rui Wu1,2, Dongxia Li1, Gengxin Wu1

  • 1International Joint Research Laboratory of Nano-Micro Architecture Chemistry, College of Chemistry, Jilin University, 2699 Qianjin Street, Changchun, 130012, P. R. China.

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|September 8, 2022
PubMed
Summary
This summary is machine-generated.

Researchers enhanced solid-state intermolecular charge-transfer (ICT) interactions by compressing a macrocyclic host

Keywords:
Co-CrystalsHost-Guest ChemistryIntermolecular Charge-TransferMacrocyclesSuperstructures

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Area of Science:

  • Supramolecular Chemistry
  • Materials Science
  • Crystal Engineering

Background:

  • Modulating intermolecular charge-transfer (ICT) interactions in host-guest systems is crucial for supramolecular chemistry and materials science.
  • Achieving controlled ICT in the solid state presents significant challenges.
  • Macrocyclic hosts offer a platform for designing specific host-guest interactions.

Purpose of the Study:

  • To develop a strategy for modulating supramolecular ICT interactions in the solid state.
  • To enhance the ICT affinities of a macrocyclic host towards electron-deficient guests.
  • To investigate the structural basis for improved host-guest interactions.

Main Methods:

  • Synthesis and characterization of perethylated leaning pillar[6]arene (p-EtLP6) and its isomeric form (m-EtLP6).
  • Investigation of solid-state ICT affinities using various electron-deficient planar guests.
  • X-ray single-crystal structural analyses.
  • Theoretical calculations to understand host-guest interactions.

Main Results:

  • A novel strategy was developed to modulate solid-state ICT interactions by compressing the host's binding cavity.
  • The isomeric form (m-EtLP6) demonstrated significantly enhanced ICT affinities compared to the parent host (p-EtLP6).
  • Structural analysis revealed that a compressed binding cavity in m-EtLP6 leads to superior host-guest size fit.
  • Theoretical calculations corroborated the experimental findings regarding enhanced ICT affinities.

Conclusions:

  • Transforming the macrocyclic backbone of pillararenes can effectively modulate solid-state ICT affinities.
  • Enhanced host-guest size fit, resulting from a compressed binding cavity, is key to improving ICT interactions.
  • This work provides a new approach for designing advanced supramolecular materials with tailored ICT properties.