A simple green method for in-situ selective extraction of Li from spent LiFePO4 batteries by synergistic effect of deep-eutectic solvent and ozone

Efficient and clean extraction lithium (Li) from spent LiFePO4 batteries (LIBs) still remains a challenge. In this paper, a green deep eutectic solvent (DES) based on ethylene glycol (EG) and choline chloride (CC), combined with ozone (O3) from air source, realized highly selective leaching Li from LiFePO4 in situ for the first time. The influence of experimental parameters on Li and Fe leaching efficiencies (ηLi, ηFe) were studied by orthogonal and single-factor tests, and ηLi ≥ 92.2% while ηFe ≤ 1.6% were obtained under the optimal conditions (6 h, 20 g/L, 8EG:1CC, 40 °C). The impurity Fe in the filtrate was completely precipitated as amorphous FePO4·3H2O after heating (150 °C, 0.5 h), achieving a pure Li-solution. The leaching mechanism elucidated that the synergistic effect (acidification, replacement and oxidation reaction) between the DES and O3 determined the phase transition of Li and Fe, promoting the efficient selective extraction of Li and in-situ separation of Fe (FePO4). The average ηLi and ηFe were separately 85.4% and 2.0% after ten cycles of the 8EG:1CC, indicative of its' excellent reusability. Meanwhile, LiCl was recovered from the filtrate. This process avoided the use of strong acid/alkali and discharge of waste water, providing fresh perspectives on the green recovery of spent LiFePO4 batteries.