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Water significantly alters molecular motion and interactions in choline chloride based deep eutectic solvents (DESs). Pulsed field gradient NMR reveals complex behaviors, with some DESs forming inhomogeneous mixtures even with added water.

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Area of Science:

  • Physical Chemistry
  • Supramolecular Chemistry
  • Materials Science

Background:

  • Deep eutectic solvents (DESs) are tunable solvents with applications in various chemical processes.
  • Understanding the behavior of aqueous DES mixtures is crucial for optimizing their use.
  • Choline chloride (ChCl) based DESs are widely studied due to their unique properties.

Purpose of the Study:

  • To investigate the effect of water on molecular dynamics and inter-molecular interactions in ChCl-based DESs.
  • To elucidate the behavior of choline cations (Ch(+)) and hydrogen bond donors (HBDs) in aqueous DES mixtures.
  • To explore the micro-heterogeneity of aqueous DES systems using advanced NMR techniques.

Main Methods:

  • Pulsed field gradient nuclear magnetic resonance (PFG NMR) spectroscopy was employed.
  • Self-diffusion coefficients of molecular and ionic species were measured.
  • The study focused on aqueous mixtures of Ethaline, Glyceline, and Reline.

Main Results:

  • Water addition significantly altered the diffusion coefficients of hydroxyl protons in Ch(+) and HBDs, indicating changed inter-molecular interactions.
  • Aqueous Ethaline showed stronger interactions between Ch(+), HBD, and water upon water addition.
  • Aqueous Reline and Glyceline exhibited unexpectedly high water self-diffusion, suggesting microscopic inhomogeneity.
  • In Reline, water may facilitate the formation of ammonium hydroxide.

Conclusions:

  • PFG NMR is a powerful technique for studying molecular dynamics and interactions in complex liquid mixtures like aqueous DESs.
  • The addition of water can lead to significant changes in the structure and dynamics of DESs, including micro-heterogeneity.
  • The behavior of aqueous DESs is highly dependent on the specific components and their interactions with water.