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Pyrrolidinium-based ionic liquids doped with lithium salts: how does Li(+) coordination affect its diffusivity?

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This study characterizes LiX-doped room-temperature ionic liquids, revealing [Li(X)2](-) species and tetrahedral Li-ion coordination. Calculated activation barriers for Li+ diffusion align with experimental data, offering insights into ionic liquid behavior.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Physical Chemistry

Background:

  • Room-temperature ionic liquids (ILs) are promising electrolytes.
  • Understanding Li+ ion coordination and transport is crucial for battery technology.
  • N-butyl-N-methyl pyrrolidinium (PYR14) cation-based ILs with fluorinated anions are of interest.

Purpose of the Study:

  • To characterize LiX-doped PYR14-based ionic liquids with IM14 and BETI anions.
  • To investigate the local and long-range organization of ions using NMR NOE.
  • To measure ionic conductivity, viscosity, and self-diffusion coefficients and compare them with theoretical calculations.

Main Methods:

  • Nuclear Magnetic Resonance (NMR) Nuclear Overhauser Effect (NOE) experiments ({1H-19F} and {1H-7Li}).
  • Measurement of ionic conductivity, viscosity, and self-diffusion coefficients.
  • Density Functional Theory (DFT) calculations for Li-ion coordination complexes.

Main Results:

  • Confirmation of [Li(X)2](-) coordinated species in all LiX-doped ILs.
  • Detection of long-range intermolecular NOEs, providing insights into ion organization.
  • Experimental and DFT calculation results show tetrahedral coordination of Li-ion by oxygen atoms, with activation barriers around 46 kJ/mol for Li+ diffusion.

Conclusions:

  • LiX-doped PYR14-based ILs exhibit stable [Li(X)2](-) species and tetrahedral Li-ion coordination.
  • The study provides a comprehensive understanding of ion organization and transport mechanisms in these ILs.
  • Calculated Li+ diffusion activation barriers correlate well with experimental data, validating the proposed diffusion model.