A tandem approach for precipitant-free highly selective recovery of valuable metals from end-of-life lithium-ion batteries using a green deep eutectic solvent

Abstract

Recently, recycling lithium-ion batteries (LIBs) waste and the efficient recovery of valuable metals has become crucial for the circular economy. Deep eutectic solvents (DESs) have shown immense potential for metal extraction from end-of-life (EoL) LIBs. However, a complicated subsequent separation process is required due to the non-selectivity of the DES components for metal. Herein, we propose a tandem precipitant-free hydrometallurgical process for the selective recovery of Li and other valuable metals (Ni, Co, Mn) from EoL LIBs using a green DES. The process parameters, viz., reaction temperature (T), time (t), pulp density (S/L), and molar ratio (MR) of ethylene glycol to tartaric acid, were optimized via the statistical optimization technique of response surface methodology. The results revealed maximum extraction efficiencies of 99.2 ± 0.5%, 96.1 ± 1.4%, 95.2 ± 1.2%, and 97.8 ± 1.5% for Li, Ni, Co, and Mn, respectively, under the optimized process conditions of T = 118 °C, t = 17 min, S/L = 42 g/L, and MR = 3:1. The kinetic study showed that interfacial reaction governed the extraction process. A plausible mechanism depicting the role of DES constituents in synergistically facilitating the extraction reaction was elucidated. Moreover, Li and other metals (Ni, Co, and Mn) were selectively separated and recovered with an overall efficiency of ∼99%. The reusability of the recovered metal products and the DES were also assessed for a closed-loop recycling process. At the outset, the proposed process paves the way for a greener alternative for recycling valuable metals from EoL LIBs rather than conventional acid-based leaching processes.