Eco-Friendly Leaching of Spent Lithium-Ion Battery Black Mass Using a Ternary Deep Eutectic Solvent System Based on Choline Chloride, Glycolic Acid, and Ascorbic Acid

Abstract

Lithium-ion batteries (LiBs) are utilized in numerous applications due to advancements in technology, and the recovery of end-of-life (EoL) LiBs is imperative for environmental and economic reasons. Pyrometallurgical and hydrometallurgical methods have been used in the recovery of metals such as Li, Co, and Ni in the EoL LiBs. Hydrometallurgical methods, which have been demonstrated to exhibit higher recovery efficiency and reduced energy consumption, have garnered increased attention in recent research. Inorganic acids, including HCl, HNO3, and H2SO4, as well as organic acids such as acetic acid and citric acid, are employed in the hydrometallurgical recovery of these metals. It is imperative to acknowledge the environmental hazards posed by these acids. Consequently, solvometallurgical processes, which involve the use of organic solvents with minimal or no water, are gaining increasing attention as alternative or complementary techniques to conventional hydrometallurgical processes. In the context of solvent systems that have been examined for a range of solvometallurgical methods, deep eutectic solvents (DESs) have garnered particular interest due to their low toxicity, biodegradable nature, tunable properties, and efficient metal recovery potential. In this study, the leaching process of black mass containing graphite, LCO, NMC, and LMO was carried out in a short time using the ternary DES system. The ternary DES system consists of choline chloride (ChCl), glycolic acid (GLY), and ascorbic acid (AA). As a result of the leaching process of cathode powders in the black mass without any pre-enrichment process, Li, Co, Ni, and Mn elements passed into solution with an efficiency of over 95% at 60 °C and within 1 h. Moreover, the kinetics of the leaching process was investigated, and Density Functional Theory (DFT) calculations were used to explain the leaching mechanism.