Microstructure Scale Lithium-Ion Battery Modeling: Part III. When and Where Lithium Plating Occurs and its Correlation with the Electrode Microstructure

Li-ion battery performance and degradation are closely related to the cell’s underlying electrode microstructure. Electrode microstructures are typically characterized with volume-averaged properties that neglect the impact of local heterogeneities. However, local heterogeneities create hot spots that can trigger degradation onset. Herein, a microstructure scale electrochemical model is used to investigate the impact of microstructure heterogeneity on lithium plating. The model predicts lithium plating is not uniform, even when considering a relatively small portion of the electrode (a cross-sectional area of 154×144 µm 2 ), preferring to plate on larger particles as compared to smaller particles. While local heterogeneities control where plating occurs, the model predicts that volume-averaged properties control when plating occurs. Additionally, the model predicts that the active material specific surface area has a linear relationship with the plating onset. However, the linear relationship between increased active material surface area and delayed plating response appears to be sensitive to the microstructure feature used to increase the active interface area. Here, a comparative case-study is explored where the specific surface area is increased by either reducing the active material particle diameter, adding open-porosity cracks, or increasing the active material surface roughness. The model predicts that increasing the specific surface area by reducing the active material particle diameter is the most effective strategy for delaying lithium plating. At 6C, reducing particle size is shown to be 3 and 20 times more effective than, respectively, adding open-porosity cracks and increasing surface roughness. A dual-layer electrode architecture combining gradations both for average properties and uniformities is eventually proposed to improve homogeneous material utilization and reduce degradation at high charge rates.