Citation: Liang Lou, Xuncheng Liu, Yuanyu Wang, Tao Hu, Zhongjie Wang, Houqiang Shi, Junkai Xiong, Siqi Jing, Liankang Ye, Qihui Guo, Xiang Ge. Achieving reusability of leachate for multi-element recovery of the discarded LiNi_xCo_yMn_1-x-yO₂ cathode by regulating the co-precipitation coefficient[J]. Chinese Chemical Letters, ;2025, 36(5): 109726. doi: 10.1016/j.cclet.2024.109726 shu

Achieving reusability of leachate for multi-element recovery of the discarded LiNi_xCo_yMn_1-x-yO₂ cathode by regulating the co-precipitation coefficient

Department of Materials and Metallurgy, Guizhou University, Guiyang 550025, China

xge@gzu.edu.cn

Received Date: 26 December 2023
Revised Date: 18 February 2024
Accepted Date: 1 March 2024
Available Online: 6 March 2024

Figures(5)

Conventional hydrometallurgy recycling process for treating wasted lithium-ion batteries (LIBs) typically results in the consumption of large amounts of corrosive leachates. Recent research on reusable leachate is expected to significantly improve the economic and environmental benefits, but is usually limited to specific and unique chemical reactions which could only apply to one type of metal elements. Herein, we report the co-extraction of multiple metal elements can be extracted without adding precipitates by mixed crystal co-precipitation, which enables the reusability of the leachate. We show that an oxalic acid (OA): choline chloride (ChCl): ethylene glycol (EG) type DES leachate system can leach transition metals from wasted LiNi_xCo_yMn_1-x-yO₂ (NCM) cathode materials with satisfactory efficiency (The time required for complete leaching at 120 ℃ is 1.5 h). The transition metals were then efficiently extracted (with a recovery efficiency of over 96% for all elements) by directly adding water without precipitants. Noteworthy, the leachate can be efficiently recovered by directly evaporating the added water. The successful realization of reusability of leachate for the synergistic extraction of multiple elements relies on the regulation of the mixed crystal co-precipitation coefficient, which is realized by rationally design the reaction condition (composition of leachate, temperature and time) and induces the extraction of originally soluble manganese element. Our strategy is expected to be generally applicable and highly competent for industrial applications.
- Lithium-ion batteries recycle,
- Reusable leachate,
- Deep eutectic solvent,
- Mixed crystal co-precipitation,
- Co-extraction
1. [1]
  G. Harper, R. Sommerville, E. Kendrick, et al., Nature 575 (2019) 75–86. doi: 10.1038/s41586-019-1682-5
2. [2]
  H.J. Peng, J.Q. Huang, X.B. Cheng, et al., Adv. Energy Mater. 7 (2017) 1700260.
3. [3]
  D.M. Li, B. Zhang, X. Ou, et al., Chin. Chem. Lett. 32 (2021) 2333–2337.
4. [4]
  M. Du, J.Z. Guo, S.H. Zheng, et al., Chin. Chem. Lett. 34 (2023) 107706.
5. [5]
  X. Yan, T. Li, Y. Xiong, et al., Energy Storage Mater. 36 (2021) 213–221.
6. [6]
  X. Yan, Q. Guo, W. Huang, et al., Carbon Neutralization 2 (2023) 300–309. doi: 10.1002/cnl2.55
7. [7]
  S. Jing, X. Yan, Y. Xiong, et al., J. Energy Chem. 84 (2023) 34–40.
8. [8]
  X. Ge, S.K. Cao, Z.S. Lv, et al., Adv. Mater. 34 (2022) 2206797.
9. [9]
  J.W. Liu, M. Yue, S.Q. Wang, et al., Adv. Funct. Mater. 33 (2023) 2214432.
10. [10]
  V. Srivastava, V. Rantala, P. Mehdipour, et al., Chem. Eng. J. 474 (2023) 145822.
11. [11]
  J.F. Zhang, J.T. Zou, D. He, et al., Green Chem. 25 (2023) 6057–6066. doi: 10.1039/d3gc00116d
12. [12]
  M. Du, K.D. Du, J.Z. Guo, et al., Rare Met. 42 (2023) 1603–1613. doi: 10.1007/s12598-022-02230-8
13. [13]
  Y.F. Meng, H.J. Liang, C.D. Zhao, et al., J. Energy Chem. 64 (2022) 166–171.
14. [14]
  X.X. Zhao, X.T. Wang, J.Z. Guo, et al., Adv. Mater. 36 (2024) 2308927.
15. [15]
  X. Liu, R. Wang, S. Liu, et al., Adv. Energy Mater. 13 (2023) 2302987.
16. [16]
  R. Kumar, S. Chakrabortty, P. Chakrabortty, et al., Chem. Eng. J. 470 (2023) 144169.
17. [17]
  G. Liang, J. Zhang, H. Liu, et al., ACS Sustain. Chem. Eng. 11 (2023) 12484–12493. doi: 10.1021/acssuschemeng.3c00343
18. [18]
  M. Wang, Z. Xu, S. Dutta, et al., One Earth 6 (2023) 1400–1413.
19. [19]
  M. Gutsch, J. Leker, Appl. Energy 353 (2024) 122132.
20. [20]
  Y.E. Milian, N. Jamett, C. Cruz, et al., Sci. Total Environ. 910 (2023) 168543.
21. [21]
  A. Porvali, M. Aaltonen, S. Ojanen, et al., Resour. Conserv. Recycl. 142 (2019) 257–266.
22. [22]
  X. Chang, M. Fan, C.F. Gu, et al., Angew. Chem. Int. Ed. 61 (2022) e202202558.
23. [23]
  W. Mrozik, M.A. Rajaeifar, O. Heidrich, et al., Energy Environ. Sci. 14 (2021) 6099–6121. doi: 10.1039/d1ee00691f
24. [24]
  X. Zheng, Z. Zhu, X. Lin, et al., Engineering 4 (2018) 361–370.
25. [25]
  D.J. Garole, R. Hossain, V.J. Garole, et al., ChemSusChem 13 (2020) 3079–3100. doi: 10.1002/cssc.201903213
26. [26]
  C. Ma, M. Svärd, K. Forsberg, Resour. Conserv. Recycl. 186 (2022) 106579.
27. [27]
  A. Zhu, X. Bian, W. Han, et al., Resour. Conserv. Recycl. 188 (2023) 106690.
28. [28]
  P.G. Schiavi, P. Altimari, M. Branchi, et al., Chem. Eng. J. 417 (2021) 129249.
29. [29]
  P.G. Schiavi, P. Altimari, E. Sturabotti, et al., ChemSusChem 15 (2022) e202200966.
30. [30]
  X. Zeng, J. Li, B. Shen, J. Hazard. Mater. 295 (2015) 112–118.
31. [31]
  X. Chen, H. Ma, C. Luo, et al., J. Hazard. Mater. 326 (2017) 77–86.
32. [32]
  R. Golmohammadzadeh, F. Faraji, F. Rashchi, Resour. Conserv. Recycl. 136 (2018) 418–435.
33. [33]
  S. Barik, G. Prabaharan, L. Kumar, J. Cleaner Prod. 147 (2017) 37–43.
34. [34]
  Y. Guo, F. Li, H. Zhu, et al., Waste Manage. 51 (2016) 227–233.
35. [35]
  T. Li, Y. Xiong, X. Yan, et al., J. Energy Chem. 72 (2022) 532–538.
36. [36]
  C. Liu, P. Liu, H. Xu, et al., Resour. Conserv. Recycl. 190 (2023) 106782.
37. [37]
  A. Verma, G.H. Johnson, D.R. Corbin, et al., ACS Sustain. Chem. Eng. 8 (2020) 6100–6108. doi: 10.1021/acssuschemeng.0c01128
38. [38]
  J. Tan, Q. Wang, S. Chen, et al., Energy Storage Mater. 41 (2021) 380–394. doi: 10.3390/rel12060380
39. [39]
  S. Refly, O. Floweri, T.R. Mayangsari, et al., ACS Sustain. Chem. Eng. 8 (2020) 16104–16114. doi: 10.1021/acssuschemeng.0c01006
40. [40]
  L. Yu, X. Liu, S. Feng, et al., Chem. Eng. J. 476 (2023) 146733.
41. [41]
  A.R. Carreira, A. Nogueira, A.P. Crema, et al., Chem. Eng. J. 475 (2023) 146374.
42. [42]
  M. Fan, X. Chang, Q. Meng, et al., SusMat 1 (2021) 241–254. doi: 10.1002/sus2.16
43. [43]
  I. Kolthoff, J. Chem. Phys. 36 (2002) 860–881.
44. [44]
  M.K. Tran, M.T.F. Rodrigues, K. Kato, et al., Nat. Energy 4 (2019) 339–345. doi: 10.1038/s41560-019-0368-4
45. [45]
  Y. Fan, Y. Kong, P. Jiang, et al., Chem. Eng. J. 463 (2023) 142278.
46. [46]
  Y. Hua, Y. Sun, F. Yan, et al., Chem. Eng. J. 436 (2022) 133200.
47. [47]
  F. Huang, T. Li, X. Yan, et al., ACS Omega 7 (2022) 11452–11459. doi: 10.1021/acsomega.2c00742
48. [48]
  Z. Wang, S. Li, T. Li, et al., Min. Metall. Explor. 39 (2022) 2149–2165. doi: 10.1007/s42461-022-00660-7
49. [49]
  Y. Chen, Y. Wang, Y. Bai, et al., ACS Sustain. Chem. Eng. 9 (2021) 12940–12948. doi: 10.1021/acssuschemeng.1c04220
50. [50]
  X. Ge, C. Gu, X. Wang, et al., J. Mater. Chem. A 5 (2017) 8209–8229.
51. [51]
  N.R. Rodriguez, A. van den Bruinhorst, L.J. Kollau, et al., ACS Sustain. Chem. Eng. 7 (2019) 11521–11528.
52. [52]
  L. Li, Y. Bian, X. Zhang, et al., Waste Manage. 71 (2018) 362–371. doi: 10.13110/marvelstales.32.2.0362
53. [53]
  H.A. Doerner, W.M. Hoskins, J. Am. Chem. Soc. 47 (1925) 662–675. doi: 10.1021/ja01680a010
54. [54]
  H. Dong, G.M. Koenig, CrystEngComm 22 (2020) 1514–1530. doi: 10.1039/c9ce00679f
55. [55]
  Y. Luo, L. Ou, C. Yin, Sci. Total Environ. 875 (2023) 162567.
56. [56]
  T. Hu, T. Li, X. Liu, et al., Green Chem. 26 (2024) 2653–2660. doi: 10.1039/d3gc04166b
57. [57]
  J. You, Z. Qin, G. Wang, et al., J. Clean. Prod. 428 (2023) 139488.
58. [58]
  Y. Lan, X. Li, G. Zhou, et al., Adv. Sci. 11 (2024) e2304425.
59. [59]
  Y. Tao, C.D. Rahn, L.A. Archer, et al., Sci. Adv. 7 (2021) eabi7633.
60. [60]
  K. Du, E.H. Ang, X. Wu, et al., Energy Environ. Mater. 5 (2022) 1012–1036. doi: 10.1002/eem2.12271
61. [61]
  D. Song, J. Yu, M. Wang, et al., Energy Storage Mater. 61 (2023) 102870.
62. [62]
  J.B. Dunn, L. Gaines, J.C. Kelly, et al., Energy Environ. Sci. 8 (2015) 158–168.
63. [63]
  C.M. Costa, J.C. Barbosa, R. Gonçalves, et al., Energy Storage Mater. 37 (2021) 433–465.
64. [64]
  Z. Chen, R. Feng, W. Wang, et al., Nat. Commun. 14 (2023) 4648.
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沈阳化工大学材料科学与工程学院沈阳 110142

Achieving reusability of leachate for multi-element recovery of the discarded LiNixCoyMn1-x-yO2 cathode by regulating the co-precipitation coefficient

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通讯作者: 陈斌, bchen63@163.com

Achieving reusability of leachate for multi-element recovery of the discarded LiNi_xCo_yMn_1-x-yO₂ cathode by regulating the co-precipitation coefficient