β‐Cyclodextrin modified deep eutectic solvent for recovering valuable metals from retired lithium batteries

Abstract An eco‐friendly supramolecular deep eutectic solvent (SUPRADES) is introduced to selectively extract valuable metals from retired lithium‐ion batteries (LIBs). Under optimized conditions (25°C, pH = 5), SUPRADES (β‐CD + [TOP][Lid]) achieved extraction efficiencies of 99.03% for Co 2+ and 92.97% for Ni 2+ in a three‐stage process. In contrast, SUPRADES (β‐CD + [TBP][Lid]) yielded 98.63% for Co 2+ and 90.98% for Ni 2+ , significantly outperforming pre‐modified solvents. Lithium ions were effectively concentrated in the extract. The system enabled successful metal recovery and solvent regeneration via reverse extraction. Molecular simulations indicated that electrostatic and coordination interactions are the main mechanisms driving extraction. This work provides an efficient, sustainable strategy for metal recycling from spent LIBs and offers theoretical insights into supramolecular macrocycle‐based recovery systems.