Different Impacts of Dissolved Transition Metals on the Graphite Anode in Lithium-Ion Batteries

Abstract The dissolution of transition metals (TM) from the cathode and their subsequent deposition on the anode represent significant degradation mechanisms in lithium-ion batteries, particularly as the industry seeks to transition towards more sustainable and cost-efficient materials. In this work, the impacts of Mn, Fe, Ni, and Co depositions on the lithiated graphite anode were investigated using pouch storage experiments to simulate the migration-deposition process and compare it to electrodes from real cells. The morphology, chemical distribution, and oxidation states of deposited TMs were investigated by scanning electron microscopy, X-ray absorption spectroscopy, and scanning transmission X‐ray microscopy. X-ray diffraction and half-cell studies for post-storage electrodes determined the lithium loss and impedance growth due to TM deposition. The impact of each TM on the lithiated graphite was found to be significantly different. Deposited Mn and Fe were fully metallic, preferred to accumulate on electrode surface, and caused severe delithiation of the graphite, while Ni and Co deposition were rather harmless. The results obtained from simulated TM-containing graphite electrodes closely corresponded with those extracted from cycled cells. This alignment enhances our understanding of the behavior of dissolved TM and paves the way for solutions aimed at mitigating capacity fade in commercial lithium-ion batteries.