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Nanoscale Spatial Heterogeneity in Deep Eutectic Solvents.

Supreet Kaur1, Aditya Gupta1, Hemant K Kashyap1

  • 1Department of Chemistry, Indian Institute of Technology Delhi , Hauz Khas, New Delhi 110016, India.

The Journal of Physical Chemistry. B
|June 18, 2016
PubMed
Summary
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Deep eutectic solvents (DESs) exhibit nanoscale spatial heterogeneity, revealed by molecular dynamics simulations of X-ray and neutron scattering. Longer alkylamide chains in DESs enhance nanoscale morphology and ion pairing.

Area of Science:

  • Physical Chemistry
  • Materials Science
  • Computational Chemistry

Background:

  • Deep eutectic solvents (DESs) are emerging as versatile materials with tunable properties.
  • Understanding the nanoscale structure of DESs is crucial for their application in various fields.
  • Previous studies have suggested structural complexity in DESs, but direct molecular-level insights are often limited.

Purpose of the Study:

  • To investigate the nanoscale spatial heterogeneity of deep eutectic solvents (DESs) using molecular dynamics simulations.
  • To analyze the X-ray and neutron scattering structure functions (S(q)s) of DESs composed of alkylamide and Li(+)/ClO4(-).
  • To correlate observed scattering features with molecular-level structural organization and ion pairing.

Main Methods:

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  • Molecular dynamics (MD) simulations were employed to model DESs.
  • X-ray and neutron scattering structure functions (S(q)s) were simulated from MD trajectories.
  • Analysis focused on identifying peaks and prepeaks in S(q)s to infer nanoscale heterogeneity.

    • Main Results:

    • Simulated S(q)s for alkylamide + Li(+)/ClO4(-) DESs showed distinct intermolecular peaks.
    • A prepeak at 0.1 < q/Å(-1) < 0.4 indicated nanoscale structural organization/heterogeneity.
    • The principal peak around 1.2 < q/Å(-1) < 2 resulted from short-distance inter- and intraspecies correlations.
    • Nanoscale spatial heterogeneity was attributed to segregated domains of the constituent electrolyte.

    Conclusions:

    • Deep eutectic solvents studied exhibit significant nanoscale spatial heterogeneity.
    • The principal peak in scattering functions is linked to close-contact correlations within segregated domains.
    • Longer alkylamide chains in DESs lead to enhanced nanoscale morphology and stronger ion pairing.