Transport coefficients for ion and solvent coupling. The case of the lithium-ion battery electrolyte

S Kjelstrup and AF Gunnarshaug and O Gullbrekken and SK Schnell and A Lervik, JOURNAL OF CHEMICAL PHYSICS, 159, 034104 (2023).

DOI: 10.1063/5.0158623

Transport properties are essential for the understanding and modeling of electrochemical cells, in particular complex systems like lithium-ion batteries. In this study, we demonstrate how a certain degree of freedom in the choice of variables allows us to efficiently determine a complete set of transport properties. We apply the entropy production invariance condition to different sets of electrolyte variables and obtain a general set of formulas. We demonstrate the application of these formulas to an electrolyte typical for lithium-ion batteries, 1M lithium hexafluoro-phosphate in a 1:1 wt. % mixture of ethylene and diethyl carbonates. While simplifications can be introduced, they provide inadequate predictions of conductivity and transport numbers, and we argue that a full matrix of Onsager coefficients is needed for adequate property predictions. Our findings highlight the importance of a complete set of transport coefficients for accurate modeling of complex electrochemical systems and the need for careful consideration of the choice of variables used to determine these properties.

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