Selective Lithium Plating on Graphite–Silicon Composite Anodes During Fast Charging in Rechargeable Lithium Batteries

In this study, we systematically analyzed selective lithium plating on graphite (Gr)–silicon (Si) composite anodes for lithium-ion batteries during fast charging, using electrochemical techniques. To achieve this, half-cells were first constructed with single Gr and Si electrodes, and lithium plating on each electrode was examined at different charging rates. It was observed that lithium plating on both electrodes began at a lower state of charge (SoC) as the charge rate increased. Furthermore, at a given charge rate, lithium plating occurred on the Si electrode at a lower SoC than on the Gr electrode. Based on the experimental findings, the lithium plating behavior of Gr and Si as a function of the charge rate was formulated to investigate the plating behavior of hypothetical composite electrodes with varying Gr–Si ratios. The lithium plating behavior observed on the actual composite electrode was consistent with that predicted from the hypothetical composite electrode, which was simulated using the same Gr–Si ratio based on the behaviors of the individual electrodes. By comparing the results from the single and composite electrodes, it is proposed that lithium plating occurs first on Si and then on Gr at low charge rates, whereas, at high charge rates, it proceeds first on Gr and then on Si. We discuss how to extrapolate the preferential plating signals—namely, plating onto Si at low charge rates and onto Gr at high charge rates—that are not directly evident in the signal from the actual composite electrode.