Efficient Direct Regeneration Strategy for Spent NCM111 Cathode Materials via EG‐Based Solvent Separation

Abstract The sustainable development of lithium‐ion batteries (LIBs) depends on efficient recycling methods, with direct regeneration enabling material reuse. However, the effective separation of electrode materials remains a critical challenge. Traditional methods often rely on strong acids, bases, or high‐temperature treatments, which are energy intensive, environmentally harmful, and may damage the material structure, thus affecting regeneration quality. To address this, an ethylene glycol (EG) based separation method is proposed. Using LiNi _1/3 Co _1/3 Mn _1/3 O ₂ (NCM111) as a representative cathode material, EG effectively dissolves the polyvinylidene fluoride (PVDF) binder at 160 °C, while its ─OH groups replace the hydrogen bonds between PVDF and the Al foil, thereby promoting the separation of the cathode material. The recovered Al foil remains intact without corrosion, enhancing its economic value. Finally, a eutectic salt method (LiOH and Li ₂ CO ₃ , molar ratio 5.25:1) is employed to repair the structural degradation of the cathode material caused by Li ⁺ loss, with its recovery assessed through characterization and electrochemical testing. The EG‐based regeneration method enables efficient and sustainable recycling of LIBs cathode materials, contributing to the development of environmentally friendly battery recycling technologies.