Abstract

The article presents a statistical physics-based model for the growth of the solid electrolyte interphase (SEI) in the negative electrode of lithium ion batteries. During battery operation, the SEI thickness grows by the reaction between lithium ions, electrons and solvent species on the surface of active particles at the negative electrode. The growth of the SEI layer causes a loss of lithium ions that induces capacity fade. In addition, it increases the ion transport resistance and decreases the total porosity. Our model employs a population balance formalism based on the Fokker-Planck Equation to describe the propagation of the particle density distribution function in the electrode. Structure-transforming processes at the level of individual particles are accounted for by using a set of kinetic and transport equations. These processes alter the particle density distribution function, and cause changes in battery performance. A parametric study of the model singles out the first moment of the initial SEI thickness distribution as the determining factor in predicting the capacity fade. The model-based treatment of experimental data allows analyzing processes that control SEI growth and extracting their controlling parameters.

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