Citation: Zhao-Cheng WANG, Yi-Gang WANG, Chuan-Chao SHENG, Ping HE, Hao-Shen ZHOU. Manganese ion oxidation precipitation method for the recycling and reusing of LiNi0.8Co0.05Mn0.15O2 materials for lithium-ion batteries[J]. Chinese Journal of Inorganic Chemistry, ;2023, 39(9): 1661-1672. doi: 10.11862/CJIC.2023.130 shu

Manganese ion oxidation precipitation method for the recycling and reusing of LiNi0.8Co0.05Mn0.15O2 materials for lithium-ion batteries

  • Corresponding author: Ping HE, pinghe@nju.edu.cn
  • Received Date: 22 April 2023
    Revised Date: 11 June 2023

Figures(8)

  • This paper proposes a scheme of recycling spent batteries, using concentrated hydrochloric acid as leaching agent, NaOH and NH4HCO3 as precipitating agents. The oxidation reaction of Mn2+ under alkaline conditions was included to change the precipitation order of ions, thus recovered ions in steps. The optimal conditions for acid leaching of concentrated hydrochloric acid to treat the ternary cathode material LiNi0.8Co0.05Mn0.15O2 were studied. In the stepwise precipitation process, Mn2+ was oxidized to MnO(OH)2, which is insoluble in non-reducing acids, and then Mn was recovered under acidic conditions. While Ni and Co were recovered under alkaline conditions by using NaOH. Li was recovered by using NH4HCO3. Using this method, the recovery of Mn reached 85.1% and the product purity reached 98.6%; the recovery of Li reached 95.0% and the product purity reached 99.3%. The pouch cell assembled with the re-synthesized ternary cathode using the recovered material reached a discharge specific capacity of 175 mAh·g-1 in the first cycle. It could stably cycle for 50 cycles with Coulombic efficiency of over 99.5%.
  • 加载中
    1. [1]

      WANG J Y, WANG R, WANG S Q, WANG L F, ZHAN C. Facile one-step solid-state synthesis of Ni-rich layered oxide cathodes for lithiumion batteries[J]. Journal of Electrochemistry, 2022,28(8)2112131. doi: 10.13208/j.electrochem.211213

    2. [2]

      MA H Y, YAO X H, MIAO M Y, YI Y, WU S Z, ZHOU J. Degradation mechanism of LiNi0.83Co0.12Mn0.05O2 cycled at 45℃[J]. Journal of Electrochemistry, 2020,26(3):431-440.  

    3. [3]

      Harper G, Sommerville R, Kendrick E, Driscoll L, Slater P, Stolkin R, Walton A, Christensen P, Heidrich O, Lambert S, Abbott A, Ryder K, Gaines L, Anderson P. Recycling lithium-ion batteries from electric vehicles[J]. Nature, 2019,575(7781):75-86. doi: 10.1038/s41586-019-1682-5

    4. [4]

      Xing C X, Da H, Yang P, Huang J W, Gan M, Zhou J, Li Y, Zhang H T, Ge B H, Fei L F. Aluminum impurity from current collectors reactivates degraded NCM cathode materials toward superior electrochemical performance[J]. ACS Nano, 2023,17(3):3194-3203. doi: 10.1021/acsnano.3c00270

    5. [5]

      Zheng X H, Zhu Z W, Lin X, Zhang Y, He Y, Cao H B, Sun Z. A minireview on metal recycling from spent lithium ion batteries[J]. Engineering, 2018,4(3):361-370. doi: 10.1016/j.eng.2018.05.018

    6. [6]

      Zhang N, He Y C, Yi X, Yan Y N, Xu W L. Rapid start-up of autotrophic shortcut nitrification system in SBR and microbial community analysis[J]. Environ. Technol., 2022,43(27):4363-4375. doi: 10.1080/09593330.2021.1950213

    7. [7]

      Pan F, Yu Y, Xu A H, Xia D S, Sun Y M, Cai Z Q, Liu W, Fu J. Application of magnetic OMS-2 in sequencing batch reactor for treating dye wastewater as a modulator of microbial community[J]. J. Hazard. Mater., 2017,340:36-46. doi: 10.1016/j.jhazmat.2017.06.062

    8. [8]

      Sun L, Qiu K Q. Vacuum pyrolysis and hydrometallurgical process for the recovery of valuable metals from spent lithium-ion batteries[J]. J. Hazard. Mater., 2011,194:378-84. doi: 10.1016/j.jhazmat.2011.07.114

    9. [9]

      Xiao J F, Li J, Xu Z M. Recycling metals from lithium ion battery by mechanical separation and vacuum metallurgy[J]. J. Hazard. Mater., 2017,338:124-131. doi: 10.1016/j.jhazmat.2017.05.024

    10. [10]

      Li J H, Zhong S W, Xiong D L, Chen H. Synthesis and electrochemical performances of LiCoO2 recycled from the incisors bound of Liion batteries[J]. Rare Metals, 2009,28(4):328-332. doi: 10.1007/s12598-009-0064-9

    11. [11]

      Choubey P K, Kim M S, Srivastava R R, Lee J C, Lee J Y. Advance review on the exploitation of the prominent energy-storage element: lithium. Part Ⅰ: From mineral and brine resources[J]. Miner. Eng., 2016,89:119-137. doi: 10.1016/j.mineng.2016.01.010

    12. [12]

      Choubey P K, Chung K S, Kim M S, Lee J C, Srivastava R R. Advance review on the exploitation of the prominent energy-storage element lithium. Part Ⅱ: From sea water and spent lithium ion batteries (LIBs)[J]. Miner. Eng., 2017,110:104-121. doi: 10.1016/j.mineng.2017.04.008

    13. [13]

      Rao Z H, Wang S F. A review of power battery thermal energy management[J]. Renew. Sust. Energ. Rev., 2011,15(9):4554-4571. doi: 10.1016/j.rser.2011.07.096

    14. [14]

      Li L, Fan E S, Guan Y B A, Zhang X X, Xue Q, Wei L, Wu F, Chen R J. Sustainable recovery of cathode materials from spent lithium-ion batteries using lactic acid leaching system[J]. ACS Sustain. Chem. Eng., 2017,5(6):5224-5233. doi: 10.1021/acssuschemeng.7b00571

    15. [15]

      Li M T, Zhang B L, Qu X, Cai M Y, Liu D X, Zhou F Y, Xie H W, Gao S B, Yin H Y. A SiCl4-assisted roasting approach for recovering spent LiCoO2 cathode[J]. ACS Sustain. Chem. Eng., 2022,10(26):8305-8313. doi: 10.1021/acssuschemeng.2c00814

    16. [16]

      Zhang J F, Hu W Y, Zou J T, Wang X W, Li P F, Peng D Z, Li Y, Zhao R R, He D. Directional high-value regeneration of lithium, iron, and phosphorus from spent lithium iron phosphatebatteries[J]. ACS Sustain. Chem. Eng., 2022,10(40):13424-13434. doi: 10.1021/acssuschemeng.2c03997

    17. [17]

      Chen D D, Rao S, Wang D X, Cao H Y, Xie W M, Liu Z Q. Synergistic leaching of valuable metals from spent Li-ion batteries using sulfuric acid-l-ascorbic acid system[J]. Chem. Eng. J., 2020,388124321. doi: 10.1016/j.cej.2020.124321

    18. [18]

      Fang J H, Ding Z P, Ling Y, Li J P, Zhuge X Q, Luo Z H, Ren Y R, Luo K. Green recycling and regeneration of LiNi0.5Co0.2Mn0.3O2 from spent lithium-ion batteries assisted by sodium sulfate electrolysis[J]. Chem. Eng. J., 2022,440135880. doi: 10.1016/j.cej.2022.135880

    19. [19]

      Lee J, Kitchaev D A, Kwon D H, Lee C W, Papp J K, Liu Y S, Lun Z, Clement R J, Shi T, McCloskey B D, Guo J, Balasubramanian M, Ceder G. Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials[J]. Nature, 2018,556(7700):185-190. doi: 10.1038/s41586-018-0015-4

    20. [20]

      Andrew P A, Glen C, David L D, Katy J M, Stephen U O. Solubility of metal oxides in deep eutectic solvents based on choline chloride[J]. J. Chem. Eng. Data, 2006,51:1280-1282. doi: 10.1021/je060038c

    21. [21]

      Tran M K, Rodrigues M T F, Kato K, Babu G, Ajayan P M. Deep eutectic solvents for cathode recycling of Li-ion batteries[J]. Nat. Energy, 2019,4(4):339-345. doi: 10.1038/s41560-019-0368-4

    22. [22]

      Lin J, Liu C W, Cao H B, Chen R J, Yang Y X, Li L, Sun Z. Environmentally benign process for selective recovery of valuable metals from spent lithium-ion batteries by using conventional sulfation roasting[J]. Green Chem., 2019,21(21):5904-5913. doi: 10.1039/C9GC01350D

    23. [23]

      Chang X, Fan M, Gu C F, He W H, Meng Q, Wan L J, Guo Y G. Selective extraction of transition metals from spent LiNixCoyMn1-x-yO2 cathode via regulation of coordination environment[J]. Angew. Chem. Int. Ed., 2022,61(24)e202202558. doi: 10.1002/anie.202202558

    24. [24]

      Dong L, Zhang L, Jia Y, Shao B, Lü W, Zhao S, You H. Site occupation and luminescence of novel orange-red Ca3M2Ge3O12: Mn2+, Mn4+(M=Al, Ga) phosphors[J]. ACS Sustain. Chem. Eng., 2020,8(8):3357-3366. doi: 10.1021/acssuschemeng.9b07281

    25. [25]

      Chen Y T, Gu S, Wu S L, Ma X X, Hussain I, Sun Z P, Lu Z G, Zhang K L. Copper activated near-full two-electron Mn4+/Mn2+ redox for mild aqueous Zn/MnO2 battery[J]. Chem. Eng. J., 2022,450(21):306-310.

    26. [26]

      Dong L P, Zhang L, Jia Y H, Xu Y W, Yin S P, You H. ZnGa2-yAlyO4: Mn2+, Mn4+ thermochromic phosphors: Valence state control and optical temperature sensing[J]. Inorg. Chem., 2020,59(21):15969-15976. doi: 10.1021/acs.inorgchem.0c02474

    27. [27]

      Zhu B X, Wang L, Shi Q F, Guo H J, Qiao J W, Cui C, Huang P. MgGa2O4: Mn2+, Mn4+: A dual-emitting phosphors with unique optical temperature sensing[J]. J. Alloy. Compd., 2023,948169717. doi: 10.1016/j.jallcom.2023.169717

    28. [28]

      Shi L Y, Zhao D, Zhang R J, Yao Q X, Liu W. A new optical temperature sensor based on the fluorescence intensity ratio of Mn2+ and Mn4+[J]. J. Am. Ceram. Soc., 2022,105(12):7479-7491. doi: 10.1111/jace.18698

    29. [29]

      GUO R, SHI P F, CHEN X Q, LI J. Synthesis and characterization of LiNi1/3Mn1/3Co1/3O2 by high temperature solid-state method[J]. Chinese J. Inorg. Chem., 2007,23(8):1387-1392. doi: 10.3321/j.issn:1001-4861.2007.08.013

    30. [30]

      ZHENG Z, HUA W B, WU Z G, XIANG W, ZHONG B H, GUO X D. Controllable preparation of ultra-high rate LiNi1/3Co1/3Mn1/3O2 cathode through carbonate Co-precipitation method for Li-ion batteries[J]. Chinese J. Inorg. Chem., 2017,33(2):307-314.  

    31. [31]

      Pi H, Xiong Y, Guo S Y. The kinetic studies of elimination of HCl during thermal decomposition of PVC in the presence of transition metal oxides[J]. Polym.-Plast. Technol. Eng., 2005,44(2):275-288. doi: 10.1081/PTE-200048727

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