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Abstract

During the normal charging process of lithium-ion batteries (LIBs), lithium ions are extracted from the cathode, transported through the electrolyte, and finally intercalated into the anode. However, abusive conditions such as overcharging, fast charging, and low-temperature charging can lead to the occurrence of lithium plating on the anode, which facilitates capacity fade, lithium dendrite growth, and even an internal short circuit in LIBs. Therefore, detecting the onset of lithium plating, understanding its mechanism, and avoiding this unwanted side reaction is significant for the safe design of LIBs.Firstly, detecting the initiation of lithium plating on graphite electrodes is of paramount importance in ensuring battery safety. To achieve this, Graphite/Li cells with consistent and reliable electrochemical performance are manufactured and selected. Discharging tests with various capacities are conducted on these cells to intentionally induce lithium plating on the graphite electrode. By comparing the voltage analysis and morphology analysis results of Graphite/Li coin cells with different discharging capacities, the localization of the lithium plating onset is detected within a narrow discharge capacity range. An electrochemical model applied to the experimental Graphite/Li coin cells is proposed to further determine the precise onset of lithium plating and provide a deep understanding of its mechanism. The model incorporating a concentration criterion can precisely predict the onset of lithium plating on graphite and elucidate the underlying mechanisms governing its occurrence. Moreover, comparative analysis reveals that the model incorporating a concentration criterion is more suitable for predicting the onset of lithium plating than a model relying on a potential criterion, particularly under high C-rate conditions. Based on the concentration criterion model, a parametric study is conducted to obtain an optimized discharging protocol with high discharging efficiency but no occurrence of lithium plating. Furthermore, a 2D physics-based model considering the actual winding structure of the battery is established to investigate the distribution of lithium plating among the winding structure in a cell. The model is validated based on the voltage-time curves of charging tests with different C-rates. By analyzing the lithium plating current density and lithium plating overpotential at different layers, it is shown that lithium plating tends to occur in the inner layers of the battery. Based on this validated model, a parametric study is conducted to clarify the influence of governing factors, including the electrochemical properties of the materials, tab arrangement, and charge protocols. According to the results, appropriate designs and use of the battery are proposed to reduce the risk of lithium plating. This study comprehensively investigates the behavior of lithium plating, including its onset, mechanism, and mitigation strategies. The results provide powerful tools for designing the next generation of long cycle-life batteries.

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