Delamination of Aluminium Current Collectors from Spent Lithium-Ion Battery Cathodes Using Room-Temperature Organic Acid-Assisted Ultrasonication

The strong adhesion between cathode materials and aluminium (Al) foil substrates presents a significant challenge in the recycling of spent lithium-ion batteries (LiBs). Conventionally, high temperatures and high concentrations of costly organic solvents such as N-methyl-2-pyrrolidone (NMP), dimethylacetamide (DMAC), dimethylformamide (DMF), and dimethyl sulfoxide (DMSO) are used to enhance ultrasonication-based delamination. In this study, a novel, eco-efficient approach was demonstrated for delaminating cathode materials from Al foil using a low-concentration organic citric-acid-assisted low-power ultrasonic treatment coupled with a gentle, low-power-per-volume mechanical mixing system at room temperature. The separation mechanism was attributed to the structure disruption, possibly swelling, of the polyvinylidene fluoride (PVDF) binder using low-concentration citric acid and the cavitation effects induced by ultrasound. Key parameters influencing the delamination efficiency included the solvent type, temperature, ultrasonic power, and treatment duration. Under optimised conditions, citric acid was used as the sonication reagent, with a process temperature of 20 °C, 60 W ultrasonic power, and 80 min of ultrasonication; a delamination efficiency of approximately 92% was achieved. The recovered cathode materials exhibited low agglomeration, favouring subsequent leaching processes. This work proposes an environmentally friendly and effective method for cathode and Al foil recovery from spent LiBs, integrating manual dismantling, ultrasonic treatment, and material separation.