Multi-methods approach for characterizing lithium-ion batteries aged to induce lithium plating

A comprehensive understanding of aging phenomena in lithiumion batteries requires advanced analytical tools. This study applies a multi-method post-mortem approach to characterize structural and chemical changes in graphite anodes from cells cycled under conditions designed to induce lithium plating. The work is part of the SUSTAIN project, which supports the development of a catalog of battery damages to enable reliable diagnostics for second-life and recycling applications. Samples from aged and reference 18650-type cells were analyzed using scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), Raman spectroscopy, time-of-flight secondary ion mass spectrometry (ToF-SIMS), X-ray photoelectron spectroscopy (XPS), and laser-induced breakdown spectroscopy (LIBS). This combination enabled cross-validation of findings and a deeper insight into surface morphology, elemental composition, chemical bonding, and lithium distribution. The analysis revealed two distinct degradation features on the aged anodes—a porous carbon-rich surface and a localized mossy structure—each with unique signatures across the applied methods. The results highlight how different techniques complement each other in identifying electrolyte breakdown products, structural disorders, and lithium-related changes. This study demonstrates the value of a multi-method strategy for building a structured catalog of degradation modes, supporting condition diagnostics, and sustainable battery use.