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 on cell geometry and can vary widely within a large cell. The resulting uneven degradation is challenging to study at the full cell level but can be revealed upon disassembly and post mortem analysis. In this work, we report localized lithium plating in automotive-grade, prismatic lithium-ion cells, also under cycling conditions generally considered to be mild (e.g., 5–65 %SOC, 23 °C, 0.5C cycle rate). Dead lithium content is quantified using 7Li nuclear magnetic resonance 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 both the separators and negative electrodes are ultimately deactivated. High pressure arises during cycling, and we propose 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 under mild cycling conditions. Notably, components harvested from regions with no detected lithium plating maintained adequate electrochemical performance. [Display omitted] •Detection of lithium plating at ambient temperature and low charge rate.•Quantitative mapping of lithium plating using 7Li NMR spectroscopy.•Parallel cycling of harvested material segments to reconstruct full cell current distribution.•Mechanism of pore closure and deactivation of electrode and separator.•Model of lithium plating propagation in deactivated regions.