The focus of the thesis is the fast-charging process of lithium-ion batteries and, more specifically, the phenomenon of lithium plating, which will be studied using operando NMR. The target application is electric mobility. The objective of the thesis is to study the dynamics of lithium insertion and lithium metal deposition at the graphite or graphite/silicon-based negative electrode in order to understand the mechanisms leading to plating formation.
Operando NMR is an ideal technique for this study because it offers the unique possibility of simultaneously tracking the signals of the lithiated graphite phases and of deposited lithium during the electrochemical processes. The coupling of electrochemistry and operando NMR will allow us to determine the onset of plating, i.e. the potential of the negative electrode at which deposition begins, and the kinetics of lithium metal deposition and reinsertion at different temperatures and different charging current regimes. We will study Li-ion batteries with a pure graphite negative electrode, but also with graphite-silicon electrodes, in order to investigate the impact of silicon on this phenomenon. The data obtained on the onset mechanisms and the kinetics of lithium metal deposition and reinsertion will be used in a multiphysics model that has already been developed in the laboratory to improve the prediction of plating onset. We will then be able to evaluate the chargeability gains on an NMC 811 // Gr+Si system incorporating optimized electrodes and propose innovative charging protocols.