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Coupling Lithium Plating with SEI Formation in a Pseudo-3D Model: A Comprehensive Approach to Describe Aging in Lithium-Ion Cells


 The lifetime of a battery is affected by various aging processes happening at the electrode scale and causing capacity and power fade over time. Two of the most critical mechanisms are the deposition of metallic lithium (plating) and the loss of lithium inventory to the SEI. These side reactions compete with reversible lithium intercalation at the anode. Here we present a comprehensive physicochemical pseudo-3D aging model for a lithium-ion battery cell, which includes electrochemical reactions for SEI formation on graphite anode, lithium plating, and SEI formation on plated lithium. The thermodynamics of the aging reactions are modeled depending on temperature and ion concentration, and the reactions kinetics are described with an Arrhenius-type rate law. The model includes also the positive feedback of plating on SEI growth, with the presence of plated lithium corresponding to a higher SEI formation compared to the values obtained in its absence at the same operating conditions. The model is thus able to describe cell aging and to quantify capacity loss due to cycling (here in % per year) as function of operating conditions. This allows the visualization of aging colormaps as function of both temperature and C-rate and the identification of critical operation conditions.