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Unveiling molecular interactions in glycerol-based deep eutectic solvents.

Letícia A Souza1, Beatriz R de Moraes1, Rafael M de Souza1

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The anion significantly impacts deep eutectic solvents (DES) structure and dynamics. Stronger glycerol-anion interactions, especially with chloride, influence local liquid dynamics and overall solvent properties.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Supramolecular Chemistry

Background:

  • Deep eutectic solvents (DES) are tunable materials with unique properties.
  • Understanding the liquid structure of DES is key to their application.
  • The role of specific anions in DES structure and dynamics requires further investigation.

Purpose of the Study:

  • To investigate the impact of anions (chloride vs. bromide) on the liquid structure and local interactions in DES.
  • To explore the phase behavior and hydrogen bonding in tetrabutylammonium salt-glycerol mixtures.
  • To elucidate the influence of anion-glycerol interactions on DES dynamics.

Main Methods:

  • Differential scanning calorimetry (DSC) for phase behavior analysis.
  • Infrared (IR) and Far-infrared (FIR) spectroscopy for probing hydrogen bonding and dynamics.
  • Quantum chemical calculations and Molecular Dynamics (MD) simulations for structural and dynamic insights.

Main Results:

  • Mixtures of tetrabutylammonium chloride/bromide with glycerol form stable liquids at room temperature and specific salt compositions (x_salt = 0.25).
  • Stronger hydrogen bonding between glycerol and the anion was observed for chloride compared to bromide.
  • MD simulations confirmed persistent glycerol-glycerol hydrogen bonds and revealed anion-induced changes in local dynamics due to confinement effects.

Conclusions:

  • The anion plays a critical role in dictating the liquid structure and local interactions within DES.
  • Anion-glycerol interactions significantly influence the solvent's properties and dynamics.
  • This study provides fundamental insights into DES structure-property relationships, crucial for designing new materials.