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

doi:10.1007/s40242-019-0010-9

高等学校化学研究 ›› 2020, Vol. 36 ›› Issue (5): 908-914.doi: 10.1007/s40242-019-0010-9

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. 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

收稿日期:2019-10-18 修回日期:2019-11-29 出版日期:2020-10-01 发布日期:2020-10-01
通讯作者: WANG Dahui E-mail:wangdh@lut.edu.cn
基金资助:
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).

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. 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).

摘要/Abstract

摘要： 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→Li_1-xCoO₂, LiNaSO₄, Na₂S₂O₇, Na₂SO₄→Li_1-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.

关键词: LiCoO₂, Chemical evolution, Roasting, In situ XRD

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→Li_1-xCoO₂, LiNaSO₄, Na₂S₂O₇, Na₂SO₄→Li_1-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

YU Yueshan, WANG Dahui, CHEN Huaijing, ZHANG Xiaodong, XU Li, YANG Lixin. Mechanism of Lithium and Cobalt Recovery from Spent Lithium-ion Batteries by Sulfation Roasting Process[J]. 高等学校化学研究, 2020, 36(5): 908-914.

参考文献 32

[1]	Jiang X., Shi N. N., Zhang Y., Cheng K., Ye K., Wang G. L., Cao D. X., Chem. J. Chinese Universities, 2015, 36(4), 739
[2]	Feng J. J., Xu R. Q., Tang Z. Y., Ai H. Q., Chem. J. Chinese Universities, 2007, 28(8), 1532
[3]	Yang Y., Xu S. M., He Y. G., Waste Manag., 2017, 64, 219
[4]	Wang Y. H., Ma L. W., Xi X. L., Nie Z. R., Zhang Y. H., Wen X., Waste Manag., 2019, 95, 192
[5]	Zheng R. J., Wang W. H., Dai Y. K., Ma Q. X., Liu Y. L., Mu D. Y., Li R. H., Ren J., Dai C. S., Green Energy & Environment, 2017, 2(1), 42
[6]	Liu C. W., Lin J., Cao H. B., Zhang Y., Sun Z., J. Clean Prod., 2019, 228, 801
[7]	Shi Y., Chen G., Chen Z., Green Chem., 2018, 20(4), 851
[8]	Zhu S. G., He W. Z., Li G. M., Zhou X., Zhang X. J., Huang J. W., Transactions of Nonferrous Metals Society of China, 2012, 22(9), 2274
[9]	Guo Y., Li F., Zhu H. C., Li G. M., Huang J. W., He W. Z., Waste Manag., 2016, 51, 227
[10]	Chen X. P., Ma H. R., Luo C. B., Zhou T., J. Hazard Mater., 2017, 326, 77
[11]	Lee C. K., Rhee k. I., Hydrometallurgy, 2003, 68(1-3), 5
[12]	Li L., Ge J., Chen R. J., Wu F., Chen S., Zhang X. X., Waste Manag., 2010, 30(12), 2615
[13]	Li L., Ge J., Wu F., Chen R. J., Chen S., Wu B. R., J. Hazard Mater., 2010, 176(1-3), 288
[14]	Li L., Lu J., Ren Y., Zhang X. X., Chen R. J., Wu F., Amine K., J. Power Sources, 2012, 218, 21
[15]	Li L., Dunn J. B., Zhang X. X., Gaines L., Chen R. J., Wu F., Amine K., J. Power Sources, 2013, 233, 180
[16]	Zeng X. L., Li J. H., Shen B. Y., J. Hazard Mater., 2015, 295, 112
[17]	Li D. F., Wang C. Y., Yin F., Chen Y. Q., Yang Y. Q., Jie X. W., Nonferrous Metals, 2009, 61(3), 83
[18]	Liu P. C., Xiao L., Tang Y. W., Chen Y. F., Ye L. G., Zhu Y. R., J. Theam. Anal. Calorim., 2018, 136(3), 1323
[19]	Ren G. X., Xiao S. W., Xie M. Q., Pan S., Fan Y. Q., Wang F. G., Xia X., J. Sustainable Metallurgy, 2017, 3(4), 703
[20]	Zheng X. H., Gao W. F., Zhang X. H., He M. M., Lin X., Cao H. B., Zhang Y., Sun Z., Waste Manag., 2016, 60, 680
[21]	Mishra D., Kim D. J., Ralph D. E., Ahn J. G., Rhee Y. H., Waste Manag., 2008, 28(2), 333
[22]	Horeh N. B., Mousavi S. M., Shojaosadati S. A., J. Power Sources, 2016, 320, 257
[23]	Wang D. H., Wen H., Chen H. J., Yang Y. J., Liang H. Y., Chem. Res. Chinese Universities, 2016, 32(4), 674
[24]	Wang D. H., Zhang X. D., Chen H. J., Sun J. Y., Minerals Enginee-ring, 2018, 126, 28
[25]	Hayashi T., Okada J., Toda E., Kuzuo R., Matsuda Y., Kuwata N., Kawamura J., J. Power Sources, 2015, 285, 559
[26]	Han S. J., Xia Y. G., Wei Z., Qiu B., Pan L. C., Gu Q. W., Liu Z. Y., Guo Z. Y., J. Mater. Chem. A, 2015, 3(22), 11930
[27]	Lindberg B. J., Hamrin L. K., Johansson G., Gelius U., Fahlman A., Nordling C., Siegbahn K., Physica Scripta, 1970, 1(5/6), 286
[28]	Zheng Y. C., Li Z. Q., Xu J., Wang T. L., Liu X., Duan X. H., Ma Y. J., Zhou Y., Pei C. H., Nano Energy, 2016, 20, 94
[29]	Kosova N., Devyatkina E., Slobodyuk A., Kaichev V., Solid State Ionics, 2008, 179(27-32), 1745
[30]	Miran H. A,. Rahman M. M., Jiang Z. T., Altarawneh M., Chuah L. S., Lee H. L., Mohammedpur E., Amri A., Mondinos N., Dlugogorski B. Z., J. Alloy Compd., 2017, 701, 222
[31]	Shatilo Y. V., Makhonina E. V., Pervov V. S., Dubasova V. S., Nikolenko A. F., Dobrokhotova Z. V., Kedrinskii I. A., Inorg Mater., 2006, 42(7), 782
[32]	Zhang Y. Q., Li L., Shi S. J., Xiong Q. Q., Zhao X. Y., Wang X. L., Gu C. D., Tu J. P., J. Power Sources, 2014, 256, 200

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

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

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