Tracking Structural Evolution in Lithium-ion Batteries via In-Operando Scanning Electron Microscopy

This study presents a novel operando SEM workflow for real-time analysis of structural and morphological changes in Li-ion battery electrodes during cycling. The methodology combines broad ion beam (BIB) polishing and an inert gas transfer system to enable high-resolution cross-sectional imaging without sample degradation. The workflow is demonstrated on NMC–LTO and graphite–Li metal systems, revealing insights into electrode expansion, particle cracking, and degradation mechanisms. Automated image processing is used to correlate SEM images with electrochemical data, enabling quantitative evaluation of NMC particle size changes and electrode thickness evolution during cycling. This technique offers a powerful diagnostic tool for both fundamental research and industrial quality control in battery development