Prediction of Lithium-Ion Battery Aging Due to SEI Growth and Lithium Plating Using 3D Microstructure-Based Modeling Method
Authors: Teel Hunter , Garrick Taylor R. , Lopata Joseph Steven , Wang Fengkun , Zeng Yangbing , Shimpalee Sirivatch 
Published: December 2024

It is well known that batteries age over time. Many aging processes that result in battery cell degradation over life are electrochemical in nature and linked to the side reactions present in the battery cell during operation or during rest. Batteries are electrochemical devices, and as such, the overpotential that occurs when driving electrochemical processes inside the battery results in deterioration of the active material and interfaces, result in a reduced usefulness for the targeted application. Different aging mechanisms occur simultaneously in batteries, and an interplay between environmental conditions and operating strategy impact the prevalence of each mechanism. Growth of the Solid Electrolyte Interphase (SEI) is the primary cause of aging in lithium-ion batteries at early stages of life. The electrolyte chemistry and mechanical stress of active materials due to volume change during operation1–5 have a major impact on the thickening of the SEI over time6. Usually, the SEI forms on the anode, which is primarily composed of graphite and occasionally combined with silicon or other higher energy density materials. The ions find it more difficult to pass through thicker SEIs due to the transport resistance present in the layer. The SEI expands as the battery ages, contributing to an internal resistance rise7. Furthermore, aging can be further accelerated by lithium plating when the anode electrochemical potential is equal to or less than that of metallic lithium8, or when other thermodynamically favorable conditions are met.
In this work, our three-dimensional microstructure based (3DMS) model is modified to capture aging phenomena of Li-ion battery9. The mechanisms of SEI growth and lithium plating are the primary focus. All equations that explain the growth of SEI and how the lithium is deposited on the surface were modified from Liu and Lu10 and Pannala7. The predictions of local thickness growth of SEI and plating on the anode active material and others electrochemical variables versus times will be reported. The experimental data of aging profiles at different C-rate, capacity fades as function of the cycle number, and the overall electrode capacity fade test11,12 will be used for model validation. These simulations can be extended to battery cell level simulations and system level simulations to drive virtual design and analysis of the battery cell, and determine if design changes need to be made in order to increase the likelihood of the battery meeting the end of life requirements.13

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