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Z-bonds, a novel interaction, are key in deep eutectic solvents (DES). This study reveals Z-bonds drive choline cation solvation, influencing DES microstructure and transport properties.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Supramolecular Chemistry

Background:

  • Z-bonds, a weak interaction combining H-bonds and electrostatics, are crucial for ionic liquid and deep eutectic solvent (DES) formation.
  • Direct experimental evidence for Z-bonds remains scarce, limiting understanding of their role in DES microstructure.

Purpose of the Study:

  • To experimentally elucidate the microstructure of choline chloride (ChCl)/3H2O DES.
  • To investigate the specific roles of Z-bonds and H-bonds in DES formation and ion solvation.
  • To correlate structural insights with observed transport properties.

Main Methods:

  • Utilized X-ray scattering (XRS) and isotope-substituted neutron scattering (ISNS) for multi-data reverse-driven all-atom modeling.
  • Employed empirical potential structure refinement (EPSR) to analyze DES microstructure.
  • Performed density functional theory (DFT) calculations to confirm and quantify bond strengths.

Main Results:

  • Z-bonds were identified as the primary driving force for choline cation (Ch+) solvation.
  • Hydrogen bonds (H-bonds) were found to directly drive chloride anion (Cl-) solvation.
  • Z-bonds favor medium-length chains and smaller rings, while H-bonds promote longer chains and larger rings.
  • DFT calculations confirmed Z-bonds and H-bonds, quantifying their respective strengths.

Conclusions:

  • Z-bonds significantly influence DES microstructure by forming specific chain and ring structures.
  • The distinct structural roles of Z-bonds and H-bonds lead to differential solvation and transport properties.
  • Z-bonds are crucial for modulating the transport properties of DES, as evidenced by the lower diffusion coefficient of Ch+ compared to Cl-.