Leaching of valuable metals from cathode active materials in spent lithium-ion batteries by levulinic acid and biological approaches

Recycling of valuable metals from spent lithium-ion batteries (LIBs) is of paramount importance for the sustainable development of consumer electronics and electric vehicles. This study comparatively investigated two eco-friendly leaching methods for recovering Li, Ni, Co, and Mn from waste NCM523 (LiNi_0.5Co_0.2Mn_0.3O₂) cathode materials in spent LIBs, i.e., chemical leaching by a green organic solvent, levulinic acid (LA) and bioleaching by an enriched microbial consortium. In chemical leaching, mathematical models predicting leaching efficiency from liquid-to-solid ratio (L/S; L/kg), temperature (°C), and duration (h) were established and validated. Results revealed that LA of 6.86 M was able to achieve complete leaching of all target metals in the absence of reductants at the optimal conditions (10 L/kg, 90 °C, and 48 h) identified by the models. The evaluation of direct one- and two-step and indirect bioleaching indicated that the latter was more feasible for metal extraction from waste NCM523. L/S was found to impact the indirect bioleaching most significantly among the three operating variables. Pretreatment of waste NCM523 by washing with 1 vol% methanesulfonic acid significantly improved indirect bioleaching. The side-by-side comparison of these two leaching approaches on the same cathode active material (CAM) thus provided the technical details for further comparison with respect to cost and environmental impact.