Selective leaching of lithium from spent lithium-ion batteries using sulfuric acid and oxalic acid
Haijun Yu , Dongxing Wang , Shuai Rao , Lijuan Duan , Cairu Shao , Xiaohui Tu , Zhiyuan Ma , Hongyang Cao , Zhiqiang Liu
International Journal of Minerals, Metallurgy, and Materials ›› 2024, Vol. 31 ›› Issue (4) : 688 -696.
Selective leaching of lithium from spent lithium-ion batteries using sulfuric acid and oxalic acid
Traditional hydrometallurgical methods for recovering spent lithium-ion batteries (LIBs) involve acid leaching to simultaneously extract all valuable metals into the leachate. These methods usually are followed by a series of separation steps such as precipitation, extraction, and stripping to separate the individual valuable metals. In this study, we present a process for selectively leaching lithium through the synergistic effect of sulfuric and oxalic acids. Under optimal leaching conditions (leaching time of 1.5 h, leaching temperature of 70°C, liquid-solid ratio of 4 mL/g, oxalic acid ratio of 1.3, and sulfuric acid ratio of 1.3), the lithium leaching efficiency reached 89.6%, and the leaching efficiencies of Ni, Co, and Mn were 12.8%, 6.5%, and 21.7%. X-ray diffraction (XRD) and inductively coupled plasma optical emission spectrometer (ICP-OES) analyses showed that most of the Ni, Co, and Mn in the raw material remained as solid residue oxides and oxalates. This study offers a new approach to enriching the relevant theory for selectively recovering lithium from spent LIBs.
selective leaching / oxalic acid / sulfuric acid / spent lithium-ion batteries
| [1] |
X.W. Duan, W.K. Zhu, Z.K. Ruan, M. Xie, J. Chen, and X.H. Ren, Recycling of lithium batteries—A review, Energies, 15(2022), No. 5, art. No. 1611. |
| [2] |
|
| [3] |
|
| [4] |
S. Natarajan and V. Aravindan, Burgeoning prospects of spent lithium-ion batteries in multifarious applications, Adv. Energy Mater., 8(2018), No. 33, art. No. 1802303. |
| [5] |
|
| [6] |
|
| [7] |
|
| [8] |
|
| [9] |
|
| [10] |
|
| [11] |
|
| [12] |
B. Makuza, Q.H. Tian, X.Y. Guo, K. Chattopadhyay, and D.W. Yu, Pyrometallurgical options for recycling spent lithium-ion batteries: A comprehensive review, J. Power Sources, 491(2021), art. No. 229622. |
| [13] |
S. Windisch-Kern, A. Holzer, C. Ponak, and H. Raupenstrauch, Pyrometallurgical lithium-ion-battery recycling: Approach to limiting lithium slagging with the InduRed reactor concept, Processes, 9(2021), No. 1, art. No. 84. |
| [14] |
|
| [15] |
|
| [16] |
|
| [17] |
D.X. Wang, W. Li, S. Rao, et al., Oxygen-free calcination for enhanced leaching of valuable metals from spent lithium-ion batteries without a reductant, Sep. Purif. Technol., 259(2021), art. No. 118212. |
| [18] |
D.D. Chen, S. Rao, D.X. Wang, H.Y. Cao, W.M. Xie, and Z.Q. Liu, Synergistic leaching of valuable metals from spent Li-ion batteries using sulfuric acid-L-ascorbic acid system, Chem. Eng. J., 388(2020), art. No. 124321. |
| [19] |
S. Gu, L. Zhang, B.T. Fu, X.P. Wang, and J.W. Ahn, Feasible route for the recovery of strategic metals from mixed lithiumion batteries cathode materials by precipitation and carbonation, Chem. Eng. J., 420(2021), art. No. 127561. |
| [20] |
L.C. Zhang, L.J. Li, H.M. Rui, et al., Lithium recovery from effluent of spent lithium battery recycling process using solvent extraction, J. Hazard. Mater., 398(2020), art. No. 122840. |
| [21] |
|
| [22] |
|
| [23] |
Yuliusman, R. Fajaryanto, A. Nurqomariah, and Silvia, Acid leaching and kinetics study of cobalt recovery from spent lithium-ion batteries with nitric acid, E3S Web Conf., 67(2018), art. No. 03025. |
| [24] |
|
| [25] |
|
| [26] |
B. Wang, X.Y. Lin, Y.Y. Tang, Q. Wang, M.K.H. Leung, and X.Y. Lu, Recycling LiCoO2 with methanesulfonic acid for regeneration of lithium-ion battery electrode materials, J. Power Sources, 436(2019), art. No. 226828. |
| [27] |
|
| [28] |
|
| [29] |
Yuliusman, Silvia, A. Nurqomariah, and R. Fajaryanto, Recovery of cobalt and nickel from spent lithium ion batteries with citric acid using leaching process: Kinetics study, E3S Web Conf., 67(2018), art. No. 03008. |
| [30] |
S.X. Yan, C.H. Sun, T. Zhou, R.C. Gao, and H.S. Xie, Ultrasonic-assisted leaching of valuable metals from spent lithium-ion batteries using organic additives, Sep. Purif. Technol., 257(2021), art. No. 117930. |
| [31] |
|
| [32] |
|
| [33] |
O.K. Park, Y. Cho, S.H. Lee, H.C. Yoo, H.K. Song, and J. Cho, Who will drive electric vehicles, olivine or spinel?, Energy Environ. Sci., 4(2011), No. 5, art. No. 1621. |
| [34] |
|
| [35] |
|
| [36] |
|
| [37] |
|
| [38] |
C.Y. Yang, J.W. Wang, P. Yang, et al., Recovery of valuable metals from spent LiNi0.8Co0.1Mn0.1O2 cathode materials using compound leaching agents of sulfuric acid and oxalic acid, Sustainability, 14(2022), No. 21, art. No. 14169. |
| [39] |
J. Chen, T.C. Liu, H.L. Li, et al., A Kind of Ternary Lithium Battery Cathode Material Recycling Method, Chinese Patent, CN112063847A, 2020. |
| [40] |
|
| [41] |
|
| [42] |
|
| [43] |
|
| [44] |
Y.Y. Wang, T.Y. Wang, L.J. Wu, et al., Recovery of valuable metals from spent ternary Li-ion batteries: Dissolution with amidosulfonic acid and D, Hydrometallurgy, 190(2019), art. No. 105162. |
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