Modélisation multi-physique de l'électrode de graphite au sein d'une batterie lithium-ion : Etude des hétérogénéités et des mécanismes de vieillissement

Abstract : Negative electrodes of lithium-ion batteries are mainly based on graphite, because of their good electrochemical properties. Unfortunately, intercalation kinetics, aging phenomena and lithium transport through active material and electrode porosity decay the optimal and homogeneous operations of this electrode. Origins of these limits are investigated in this work thanks to a porous electrode model.A sensitivity study indicates that preponderant model parameters are related to the kinetics and lithium transport in solid and liquid phases. The model is experimentally validated at a cell scale and predicts the appearances of lithium heterogeneities during the graphite lithiation. They are correlated to the staged shape of the graphite equilibrium potential. Modeling additional inhomogeneity sources, especially particle distribution, amplifies these heterogeneities and decrease drastically cell performance. In a first approach, an operando measure of the local lithiation state confirms this heterogeneity aspect during operations.In a second part, data of cycled and calendar aged graphite-NMC cell validates different aging models. The growth of the passive layer on the graphite surface (SEI) explains the cyclable lithium loss on its own. SEI heterogeneities are negligible in the porous model as opposition to experimental finding. Capacity recoveries and sudden loss are explained respectively via a SEI dissolution mechanism and lithium-plating correlated to the degradation of the electrode transport properties.
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Nicolas Dufour. Modélisation multi-physique de l'électrode de graphite au sein d'une batterie lithium-ion : Etude des hétérogénéités et des mécanismes de vieillissement. Mécanique des matériaux [physics.class-ph]. Université Grenoble Alpes, 2019. Français. ⟨NNT : 2019GREAI007⟩. ⟨tel-02148211⟩

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