Three-dimensional electrochemical-thermodynamic modeling reveals manufacturing defect mechanisms governing lithium plating in lithium-ion batteries

Lithium plating on anodes severely limits fast-charging performance and reduces battery safety in lithium-ion batteries, creating a fundamental barrier to widespread electric vehicle adoption. However, the quantitative mechanisms by which manufacturing defects in electrodes trigger lithium plating remain poorly characterized, limiting advances in battery manufacturing optimization. This study extends the classical Newman model to incorporate multiple anode reactions: lithium intercalation, plating, and stripping, within a comprehensive three-dimensional electrochemical-thermodynamic framework. The modeling approach systematically characterizes two critical manufacturing defects: active material detachment at electrode edges and non-uniform calendering density distribution. Experimental validation across wide temperature ranges (−5 °C to 45 °C) and multiple charging rates demonstrates exceptional model accuracy, with terminal voltage errors consistently below 21.27 mV. This validated framework enables quantitative analysis of defect-induced lithium plating mechanisms previously inaccessible to experimental characterization alone. Results reveal fundamentally different but interconnected pathways: active material detachment creates localized current density concentrations that preferentially trigger lithium plating, while non-uniform calendering disrupts ion transport pathways and compromises electrical network integrity. Parameter sensitivity analysis uncovers pronounced nonlinear interactions between defect severity and charging protocols, with heterogeneity effects becoming dominant under high-rate conditions. These mechanistic insights enable development of an optimized anode overhang design strategy that achieves lithium plating reduction of up to 29.3 % across diverse defect scenarios, as validated through computational predictions. The established quantitative framework bridges the critical knowledge gap between manufacturing process variations and electrochemical performance. These findings advance fundamental understanding of defect-induced failure mechanisms while offering practical pathways to enhance electric vehicle battery safety, charging speed, and operational longevity.