Thermo-Electro-Mechanical Modeling and Experimental Validation of Thickness Change of a Lithium-Ion Pouch Cell with Blend Positive Electrode

Abstract

Lithium-ion battery cells exhibit a complex and nonlinear coupling of thermal, electrochemical, and mechanical behavior. In order to increase insight into these processes, we report the development of a pseudo-three-dimensional (P3D) thermo-electro-mechanical model of a commercial lithium-ion pouch cell with graphite negative electrode and lithium nickel cobalt aluminum oxide/lithium cobalt oxide blend positive electrode. Nonlinear molar volumes of the active materials as function of lithium stoichiometry are taken from literature and implemented into the open-source software Cantera for convenient coupling to battery simulation codes. The model is parameterized and validated using electrical, thermal and thickness measurements over a wide range of C-rates from 0.05 C to 10 C. The combined experimental and simulated analyses show that thickness change during cycling is dominated by intercalation-induced swelling of graphite, while swelling of the two blend components partially cancel each other. At C-rates above 2 C, electrochemistry-induced temperature increase significantly contributes to cell swelling due to thermal expansion. The thickness changes are nonlinearly distributed over the thickness of the electrode pair due to gradients in the local lithiation, which may accelerate local degradation. Remaining discrepancies between simulation and experiment at high C-rates might be attributed to lithium plating, which is not considered in the model at present.