Solid-Electrolyte Interphase During Battery Cycling: Theory of Growth Regimes

Abstract

The capacity fade of modern lithium ion batteries is mainly caused by the formation and growth of the solid-electrolyte interphase (SEI). Numerous continuum models support its understanding and mitigation by studying SEI growth during battery storage. However, only a few electrochemical models discuss SEI growth during battery operation. In this article, we develop a continuum model, which consistently captures the influence of open circuit potential, current direction, current magnitude, and cycle number on the growth of the SEI. Our model is based on the formation and diffusion of neutral lithium atoms, which carry electrons through the SEI. Recent short- and long-term experiments provide validation for our model. We show that SEI growth is either reaction, diffusion, or migration limited. For the first time, we model the transition between these mechanisms and explain empirically derived capacity fade models of the form $\Delta Q\propto t^{\beta }$ with $0\le \beta \le 1$. Based on our model, we identify critical operation conditions accelerating SEI growth.

11 pages, 7 figures

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Cited by in corpus (10)

• Solid-Electrolyte Interphase During Battery Cycling: Theory of Growth Regimes
• Chemo-Mechanical Model of SEI Growth on Silicon Electrode Particles
• Growth of the Solid-Electrolyte Interphase: Electron Diffusion versus Solvent Diffusion
• Voltage Hysteresis of Silicon Nanoparticles: Chemo-Mechanical Particle-SEI Model
• Systematic Feature Design for Cycle Life Prediction of Lithium-Ion Batteries During Formation
• A four parameter model for the solid-electrolyte interphase to predict battery aging during operation
• Theory of layered-oxide cathode degradation in Li-ion batteries by oxidation-induced cation disorder
• Microstructure-Resolved Degradation Simulation of Lithium-Ion Batteries in Space Applications
• Transition between growth of dense and porous films: Theory of dual-layer SEI
• Effects of High-Temperature Preconditioning on Li Plating During Low-Temperature Cycling of the COTS LG Chem HG2 Cell