Localized lithium plating under mild cycling conditions in high-energy lithium-ion batteries

Conditions such as the temperature and pressure experienced by lithium-ion battery components are dependent oncell geometry and can vary widely within a large cell. The resulting uneven degradation is challenging to study at thefull cell level but can be revealed upon disassembly and post mortem analysis. In this work, we report localizedlithium plating in automotive-grade, prismatic lithium-ion cells, also under cycling conditions generally consideredto be mild (e.g., 5–65 %SOC, 23 ◦C, 0.5C cycle rate). Dead lithium content is quantified using 7Li nuclear magneticresonance spectroscopy in both electrode and separator samples, corresponding to substantial capacity fade(26–46%) of the full cells. Severe lithium plating is typically initiated in regions near the positive tab, in which boththe separators and negative electrodes are ultimately deactivated. High pressure arises during cycling, and wepropose a deactivation mechanism based on high local stress due to electrode expansion and external constraint.Further, we develop a model to demonstrate that component deactivation can result in lithium plating even undermild cycling conditions. Notably, components harvested from regions with no detected lithium plating maintainedadequate electrochemical performance. QC 20230522