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Area of Science:

  • Physical Chemistry
  • Solution Thermodynamics
  • Ionic Liquids

Background:

  • Ionic liquids (ILs) exhibit sensitivity to water, impacting their properties even at low concentrations.
  • The structural thermodynamics of protic ionic liquid (PIL)-water systems at low water concentrations remain poorly understood.
  • Understanding these interactions is crucial for designing and utilizing ILs in various applications.

Purpose of the Study:

  • To elucidate the structural thermodynamics of protic ionic liquid (PIL)-water systems at low water concentrations.
  • To compare the water-IL interactions in protic and aprotic ionic liquids (AILs).
  • To investigate the effect of water on ion-ion and water-water interactions within these systems.

Main Methods:

  • Application of the rigorous Kirkwood-Buff theory of solutions.
  • Quantification of species interactions using solely thermodynamic data.
  • Analysis of IL-water systems at varying water concentrations.

Main Results:

  • Cholinium bis(trifluoromethanesulfonyl)imide ([Ch][NTf2]), an AIL, shows stronger water interactions at low concentrations compared to its analogous PIL, N,N-dimethylethanolammonium bis(trifluoromethanesulfonyl)imide ([DMEtA][NTf2]).
  • [DMEtA][NTf2] exhibits stronger water-ion interactions at higher water contents, with both systems showing weakening water-ion interactions as water content increases.
  • Water minimally affects ion-ion interactions in most ILs, except for [Ch][NTf2], where they strengthen with increasing water content.
  • Evidence of water self-association and large water aggregates in PIL-rich compositions was found, with water-water interactions in [DMEtA][NTf2] resembling those in dialkylimidazolium AILs.

Conclusions:

  • The study provides a detailed thermodynamic understanding of water interactions in PIL-water systems.
  • Differences in anion-water interactions significantly influence water self-association in PILs.
  • The findings offer insights into the behavior of ILs in the presence of water, crucial for their practical applications.