Renovation of LiCoO₂ with outstanding cycling stability by thermal treatment with Li₂CO₃ from spent Li-ion batteries

It is quite necessary for us to pay close attention to the recycling of the spent Li-ion batteries as the worldwide consumption of Li-ion batteries grows year-on-year, and the recycling process today is relatively complex and environmental harmful. So a simple and green recycling process is needed. An acid-free recycling process is proposed and used to recycle spent 18650-type LiCoO₂ batteries, and the recycled cathode material has been renovated by thermal treatment with Li₂CO₃. After dismantling, detachment of an 18650 cell and renovation of pristine cathode material, we recovered plastic, stainless steel, separator, Cu foil, Al foil and renovated cathode material. The total recovery weight ratio could reach 95.78%. X-ray diffraction patterns and Raman spectroscopy show that the compositions of the pristine cathode material are LiCoO₂ and Co₃O₄. X-ray photoelectric spectroscopy shows that Co₃O₄ decreased during the renovation process. The mole ratio of Li/Co has been adjusted in the process of renovation to obtain the optimal properties. The initial discharge capacity of the renovated cathode material is 150.3 mA h/g and delivers a discharge capacity of 140.1 mA h/g after 100 cycles with outstanding cycling stability. The effect of impurities of Al and Cu elements has been evaluated on the electrochemical properties for the renovated cathode material. The results demonstrate that the impact of both elements is in acceptable range. This renovated cathode material by as-proposed method has good electrochemical characteristics for Li-ion batteries, which can possibly meet the commercial requirements for reuse.