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Unraveling relationship between complex lifetimes and microscopic diffusion in deep eutectic solvents.

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Water influences deep eutectic solvents (DESs) by altering microscopic dynamics and transport properties. This study reveals how bond kinetics and diffusion mechanisms are interconnected, crucial for understanding DES behavior.

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Area of Science:

  • Physical Chemistry
  • Materials Science

Background:

  • Aqueous mixtures of deep eutectic solvents (DESs) exhibit tunable physicochemical properties.
  • Understanding water's impact on DES microscopic dynamics and transport is crucial but limited.
  • DES diffusion mechanisms are complex, influenced by hydrogen bond and complex formation/dissociation kinetics.

Purpose of the Study:

  • To investigate the relationship between bond kinetics, diffusion mechanisms, and dynamical heterogeneity in DESs.
  • To explore the influence of varying water concentrations on relaxation phenomena in acetamide-lithium perchlorate DES.
  • To elucidate how water addition modulates molecular dynamics and transport properties in DES.

Main Methods:

  • Studied relaxation phenomena in acetamide-lithium perchlorate DES with varying water concentrations.
  • Analyzed diffusion mechanisms, including Fickian and non-Gaussian behavior.
  • Quantified relationships between bond lifetimes (acetamide-water, acetamide-lithium) and diffusive timescales.

Main Results:

  • Acetamide exhibited Fickian yet non-Gaussian diffusion across all water concentrations.
  • A power-law relationship (τg∝τfγ, γ ∼ 1.4) was observed between Fickian and Gaussian timescales.
  • A transition in diffusion mechanism from vehicular to structural was identified at 20 wt.% water, linked to acetamide-lithium complex lifetimes.

Conclusions:

  • Bond dynamics in DESs are critical regulators of molecular diffusion processes.
  • Water concentration significantly impacts the interplay between bond kinetics and diffusion in DESs.
  • The findings highlight the importance of considering specific interactions (e.g., hydrogen bonds, complex formation) for predicting DES behavior.