Interplay of Lithium Plating Quantification on Thermal Safety Characteristics of Lithium-Ion Batteries

Abstract

Adverse lithium plating is a significant side reaction during the fast charging of lithium-ion (Li-ion) batteries when the Li-ion flux exceeds the intercalation or diffusion limits of graphite electrodes. Accurate quantification of lithium plating has always been a tough challenge given the severe defects of online detection methods such as coulombic efficiency and voltage relaxation plateau, making the mathematical correlation between cell-level thermal safety hazards and quantitative lithium plating events still a bottleneck problem. In this study, we apply a three-electrode (3E) Li-ion cell configuration and the accelerating rate calorimeter (ARC) to comprehensively investigate the interplay of unfavorable lithium plating on thermal runaway characteristics of Li-ion batteries. Lithium plating is introduced by cycling 3E Li-ion cells at low temperatures and quantified by analyzing potential-based plating energy, coulombic inefficiency, internal resistance, and voltage relaxation plateau. Surface microscopic characterization is carried out on graphite electrodes to reveal the morphologies and chemical states of lithium deposition. ARC experiments are implemented at full-cell and partial-cell scales to fundamentally understand the effects and contributions of thermally unstable lithium plating to the overall safety performance of Li-ion cell chemistries.