Chemical Research in Chinese Universities ›› 2020, Vol. 36 ›› Issue (5): 908-914.doi: 10.1007/s40242-019-0010-9

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Mechanism of Lithium and Cobalt Recovery from Spent Lithium-ion Batteries by Sulfation Roasting Process

YU Yueshan1, WANG Dahui1, CHEN Huaijing2, ZHANG Xiaodong1, XU Li1, YANG Lixin1   

  1. 1. State Key Laboratory of Advance Processing and Recycling of Nonferrous Metals, Lanzhou University of Technology, Lanzhou 730050, P. R. China;
    2. College of Science, Lanzhou University of Technology, Lanzhou 730050, P. R. China
  • Received:2019-10-18 Revised:2019-11-29 Online:2020-10-01 Published:2020-10-01
  • Contact: WANG Dahui E-mail:wangdh@lut.edu.cn
  • Supported by:
    Supported by the National Natural Science Foundation of China(No.51864032) and the Joint Fund Between the Shenyang National Laboratory for Materials Science and the State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals, China(No.18LHZD002).

Abstract: Different from the traditional pyrometallurgical recovery process of Li and Co from spent lithium-ion batteries, a new recovery method for Li and Co was established by converting LiCoO2 into water-soluble metal sulfates by roasting a mixture of LiCoO2 and NaHSO4·H2O. The evolution law of the mixture with increased roasting temperature was investigated by thermogravimetry-differential scanning calorimetry(TG-DSC), in situ X-ray diffraction(XRD), XRD, and X-ray photoelectron spectroscopy(XPS). The results show that the phase transition of LiCoO2 mixed with NaHSO4·H2O with increased temperature proceeded as follows:LiCoO2, NaHSO4·H2O→LiCoO2, NaHSO4→Li1-xCoO2, LiNaSO4, Na2S2O7, Na2SO4→Li1-xCoO2, Co3O4, LiNaSO4, Na2SO4→Co3O4, LiNaSO4. The reaction mechanism of this roasting process may be as follows:LiCoO2+NaHSO4·H2O→1/2Li2SO4+ 1/2Na2SO4+1/3Co3O4+1/12O2+3/2H2O, Li2SO4+Na2SO4=2LiNaSO4.

Key words: LiCoO2, Chemical evolution, Roasting, In situ XRD