Influence of metallic contaminants on the electrochemical and thermal behavior of Li-ion electrodes

Emerging nondestructive (direct) recycling techniques for lithium-ion batteries may introduce metallic impurities into recycled electrodes. In the present work, the impact of such nonionic contaminants on the practical performance of both anode and cathode materials is evaluated using a synergistic combination of electrochemical and thermal analysis. The impurities under study have been selected through evaluation of industrially shredded batteries, and include Fe0, Al0, Mg0, Cu0, and Si0. The electrochemical behavior of materials containing each individual contaminant at either the anode or the cathode is evaluated in both half-cell and full-cell format. Further, the first-cycle thermal signatures of full cells are used to validate and complement electrochemical signatures, and the two techniques are used in conjunction to suggest distinct mechanisms of electrochemical reactivity for the various impurities. At the anode, metallic contaminants are found to disrupt performance through direct reaction with Li and may serve as weak catalysts to accelerate electrolyte degradation. At the cathode, metallic contaminants show evidence of crossover during formation cycling to disrupt SEI formation. We suggest that coupled electrochemical and thermal analysis may be used to both identify the presence of contaminants and to elucidate specific mechanisms of reactivity for metallic impurities under anodic and cathodic conditions. •Coupled thermal & electrochemical signatures of metallic contaminants are established.•Cathode contaminants are found to disrupt SEI formation through crossover reactions.•Anode contaminants adversely react with Li & accelerate electrolyte degradation.•Complementary characterization offers powerful tool to selectively identify impurities.