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Quantifying selective solvent transport under an electric field in mixed-solvent electrolytes
Chao Fang1,2, David M Halat1,2, Aashutosh Mistry3
1Department of Chemical and Biomolecular Engineering, University of California Berkeley California 94720 USA ruiwang325@berkeley.edu.
Chemical Science
|May 26, 2023
Summary
This study shows that in lithium-ion battery electrolytes, ethylene carbonate (EC) and ethyl methyl carbonate (EMC) solvents move differently. Understanding these distinct solvent transports is key for better battery performance.
Area of Science:
- Electrochemistry
- Materials Science
- Physical Chemistry
Background:
- Lithium-ion battery electrolytes typically use solvent mixtures.
- Current ion transport analysis often simplifies these mixtures as single entities.
- Understanding solvent dynamics is crucial for optimizing battery performance.
Purpose of the Study:
- To quantify electric-field-induced transport in concentrated LiPF6 electrolytes using EC/EMC mixtures.
- To investigate the selective transport of ethylene carbonate (EC) relative to ethyl methyl carbonate (EMC).
- To highlight the necessity of considering multiple solvent species in electrolyte analysis.
Main Methods:
- Electrophoretic Nuclear Magnetic Resonance (eNMR) measurements.
- Molecular Dynamics (MD) simulations.
- Calculation of transference numbers for individual solvent species.
Main Results:
- Demonstrated selective transport of EC over EMC in the electrolyte mixture.
- Observed preferential solvation of cations by EC, influencing solvent dynamics.
- Simulations revealed diverse, transient solvent clusters migrating at varying velocities.
Conclusions:
- Acknowledging the presence and distinct behavior of all four species (Li+, PF6-, EC, EMC) is essential for accurate electrolyte modeling.
- The difference in transference numbers reflects preferential solvation and dynamic consequences.
- This research emphasizes the need for a multi-species approach in mixed-solvent electrolyte analysis.
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