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Discrepancies in transference number measurements for LiFSI electrolytes indicate significant ion clustering. Newman

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Physical Chemistry

Background:

  • Binary electrolyte performance relies on conductivity, salt diffusion, and transference numbers.
  • Established methods for conductivity and diffusion exist, but transference number measurements often assume ideal conditions.
  • Ideal conditions imply complete salt dissociation, which may not hold true in concentrated electrolytes.

Purpose of the Study:

  • To determine a complete set of ion transport properties for LiFSI in a functionalized perfluoroether solvent.
  • To investigate the validity of ideal and NMR-based transference number measurements in concentrated solutions.
  • To resolve discrepancies in transference number measurements using concentrated solution theory.

Main Methods:

  • Utilized Newman's concentrated solution theory to analyze experimental data.
  • Measured ion transport properties including conductivity, salt diffusion coefficient, and transference numbers.
  • Compared transference numbers derived from concentrated solution theory (t), ideal methods (t+,id), and pulsed field gradient NMR (t+,NMR).

Main Results:

  • Concentrated solution theory-based transference number (t) is negative and increases with salt concentration.
  • Ideal transference number (t+,id) is positive and decreases with salt concentration.
  • NMR-based transference number (t+,NMR) is approximately 0.5, independent of concentration, highlighting ion clustering.

Conclusions:

  • Disparities between the three transference number measurements reveal significant ion clustering in LiFSI electrolytes.
  • Newman's concentrated solution theory successfully resolves these discrepancies, providing a more accurate picture of ion transport.
  • The study emphasizes the limitations of ideal and NMR methods for non-ideal, concentrated electrolyte systems.