As the demand for lithium-ion batteries for electric vehicles is increasing, it is important to recover valuable metals from waste lithium-ion batteries. In this study, the effects of gas flow rate and hydrogen partial pressure on hydrogen reduction of NCM-based lithium-ion battery cathode materials were investigated. As the gas flow rate and hydrogen partial pressure increased, the weight loss rate increased significantly from the beginning of the reaction due to the reduction of NiO and CoO by hydrogen. At 700 °C and hydrogen partial pressure above 0.5 atm, Ni and Li2O were produced by hydrogen reduction. From the reduction product and Li recovery rate, the hydrogen reduction of NCM-based cathode materials was significantly affected by hydrogen partial pressure. The Li compounds recovered from the solution after water leaching of the reduction products were LiOH, LiOH·H2O, and Li2CO3, with about 0.02 wt% Al as an impurity.

In this study, an experiment is performed to recover the Li in Li2CO3 phase from the cathode active material NMC (LiNiCoMnO2) in waste lithium ion batteries. Firstly, carbonation is performed to convert the LiNiO, LiCoO, and Li2MnO3 phases within the powder to Li2CO3 and NiO, CoO, and MnO. The carbonation for phase separation proceeds at a temperature range of 600oC~800oC in a CO2 gas (300 cc/min) atmosphere. At 600~700oC, Li2CO3 and NiO, CoO, and MnO are not completely separated, while Li and other metallic compounds remain. At 800 oC, we can confirm that LiNiO, LiCoO, and Li2MnO3 phases are separated into Li2CO3 and NiO, CoO, and MnO phases. After completing the phase separation, by using the solubility difference of Li2CO3 and NiO, CoO, and MnO, we set the ratio of solution (distilled water) to powder after carbonation as 30:1. Subsequently, water leaching is carried out. Then, the Li2CO3 within the solution melts and concentrates, while NiO, MnO, and CoO phases remain after filtering. Thus, Li2CO3 can be recovered.

The electrochemical properties of cells assembled with the LiNiO2 (LNO) recycled from cathode materialsof waste lithium secondary batteries (Li[Ni,Co,Mn]O2), were evaluated in this study. The leaching, neutralization andsolvent extraction process were applied to produce high-purity NiSO4 solution from waste lithium secondary batteries.High-purity NiO powder was then fabricated by the heat-treatment and mixing of the NiSO4 solution and H2C2O4.Finally, LiNiO2 as a cathode material for lithium ion secondary batteries was synthesized by heat treatment and mixingof the NiO and Li2CO3 powders. We assembled the cells using the LiNiO2 powders and evaluated the electrochemicalproperties. Subsequently, we evaluated the recycling possibility of the cathode materials for waste lithium secondary bat-tery using the processes applied in this work.