Theory of Impedance Spectroscopy for Lithium Batteries
Authors: Fabian Single, Birger Horstmann, Arnulf Latz
AI-generated Key Points
- Authors Fabian Single, Birger Horstmann, and Arnulf Latz present a physics-based model for impedance spectroscopy in lithium batteries
- Model focuses on electrochemical cells with planar electrodes and includes the solid-electrolyte interphase (SEI) as a porous surface film
- Two key improvements: consistent description of lithium transport through electrolyte and SEI, analytical solution to show impedance signals' dependence on transport parameters
- Model offers an analytic expression for cell impedance covering both bulk and surface processes
- Importance of electrolyte convection in concentrated electrolytes highlighted through concentration polarization signals analysis
- Complex impedance expression simplified and compared to common equivalent circuit models within specific parameter ranges to demonstrate effectiveness
- Experimental comparisons with lithium metal electrodes reveal large transference numbers for lithium ions, suggesting similarities between lithium-ion transport through SEI and solid electrolytes
- Study published in The Journal of Physical Chemistry C provides valuable insights into impedance spectroscopy for lithium batteries and advances understanding of battery technology
Abstract: In this article, we derive and discuss a physics-based model for impedance spectroscopy of lithium batteries. Our model for electrochemical cells with planar electrodes takes into account the solid-electrolyte interphase (SEI) as porous surface film. We present two improvements over standard impedance models. Firstly, our model is based on a consistent description of lithium transport through electrolyte and SEI. We use well-defined transport parameters, e.g., transference numbers, and consider convection of the center-of-mass. Secondly, we solve our model equations analytically and state the full transport parameter dependence of the impedance signals. Our consistent model results in an analytic expression for the cell impedance including bulk and surface processes. The impedance signals due to concentration polarizations highlight the importance of electrolyte convection in concentrated electrolytes. We simplify our expression for the complex impedance and compare it to common equivalent circuit models. Such simplified models are good approximations in concise parameter ranges. Finally, we compare our model with experiments of lithium metal electrodes and find large transference numbers for lithium ions. This analysis reveals that lithium-ion transport through the SEI has solid electrolyte character.
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