Efficient Ionic Liquid-Based Leaching and Extraction of Metals from NMC Cathodes

The increasing demand for lithium-ion batteries (LIBs) and their limited lifespan emphasize the urgent need for sustainable recycling strategies. This study investigates the application of tetrabutylphosphonium-based ionic liquids (ILs) as alternative leaching agents for recovering critical metals, Li(I), Co(II), Ni(II), and Mn(II), from spent NMC cathode materials. Initial screening experiments evaluated the leaching efficiencies of nine tetrabutylphosphonium-based ILs for Co(II), Ni(II), Mn(II), and Li(I), revealing distinct metal dissolution behaviors. Three ILs containing HSO4−, EDTA2−, and DTPA3− anions exhibited the highest leaching performance and were selected for further optimization. Key leaching parameters, including IL and acid concentrations, temperature, time, and solid-to-liquid ratio, were systematically adjusted, achieving leaching efficiencies exceeding 90%. Among the tested systems, [TBP][HSO4] enabled near-complete metal dissolution (~100%) even at room temperature. Furthermore, an aqueous biphasic system (ABS) was investigated utilizing [TBP][HSO4] in combination with ammonium sulfate, enabling the complete extraction of all metals into the salt-rich phase while leaving the IL phase metal-free and potentially suitable for reuse, indicating the feasibility of integrating leaching and extraction into a continuous, interconnected process. This approach represents a promising step forward in LIB recycling, highlighting the potential for sustainable and efficient integration of leaching and extraction within established hydrometallurgical frameworks.