Green and efficient recycling method for spent Ni–Co–Mn lithium batteries utilizing multifunctional deep eutectic solvents

Abstract

Given the growing volume of discarded lithium-ion batteries (LIBs), the extraction and recovery of valuable metals through environmentally-friendly solvent processes have become crucial, but they remain challenging tasks. Deep eutectic solvent (DES), an innovative and green solvents, have demonstrated significant promise in the extraction of valued metal elements from spent LIBs. This work employed a multifunctional DES based on natural molecules dimethyl-beta-propiothetin (DMPT) and ethylene glycol (EG) for the efficient leaching of transition metal ions. Under the reduction effect of EG and the action of carboxyl groups and chloride ions in DMPT, the leaching rate of Li, Ni, Co, and Mn can reach 99.59%, 99.28%, 99.04%, and 99.45%, respectively. Furthermore, DFT calculations were employed to explore the microstructure of DES and its interactions with metal ions. The main active site in the DES molecule is near the chloride ion, and DES binds most strongly to Mn, followed by Co, and weakest to Ni. This work avoids the use of volatile acids and demonstrates great potential in extracting valuable metals, providing a sustainable and environment-friendly alternative for the efficient recycling of waste LIBs.