An Efficient and Eco-Friendly Recycling Route of Valuable Metals from Spent Ternary Li-Ion Batteries: Kinetics Evaluation of Chlorination Processes and Regeneration of LiNiCoMnO Cathode Materials.

The recycling of spent Li-ion batteries is urgent, and the effective recovery of valuable metals from spent cathode material is an economic and eco-friendly approach. In this study, Ni, Cu, Co, and Mn were extracted synchronously from spent LiNiCoMnO by chlorination and the complexation reaction of ammonium chloride at low temperatures. The kinetics of the chlorination process was investigated by nonisothermal thermal analysis to determine the rate equation of metal conversion, and the apparent activation energies were calculated to be 99.96 kJ·mol for lithium and 146.70 kJ·mol for nickel, cobalt, and manganese, respectively. The separation of valuable metals from polymetallic leaching solution and the regeneration of cathode materials were further investigated to promote the industrialization of the process. The recoveries of Ni, Co, Mn, and Li can reach 97.75, 99.99, 99.99, and 92.23%, respectively. The prepared LiNiCoMnO precursor is a multilayer spherical particle formed by stacking primary hexagonal nanosheets along the (010) crystal axis, the formation mechanism of which was discussed. The effect of temperature, time, and mixed lithium ratio on the performance of single crystal LiNiCoMnO cathode in the synthesis process was investigated to determine the optimum conditions. Compared with commercial materials, the prepared single crystal LiNiCoMnO cathode has a more regular crystal structure and higher initial discharge capacity (215.9 mAh·g at 0.1 C).