Separation of lithium and nickel using ionic liquids and tributyl phosphate

doi:10.1016/j.cjche.2023.04.023

摘要/Abstract

摘要： With the vigorous development of the electronics industry, the consumption of lithium continues to increase, and more lithium needs to be mined to meet the development of the industry. The content of lithium in the solution is much higher than that of minerals, but the interference of impurity ions increases the difficulty of extracting lithium ions. Therefore, we prepared an imidazole-based ionic liquid (1-butyl-3-methylImidazolium bis(trifluoromethyl sulfonyl)imide) (IL) for efficient lithium extraction from aqueous solutions by solvent extraction. Using an extraction consisting of 10% IL, 85% tributyl phosphate (TBP), and 5% dichloroethane and an organic to aqueous phase ratio (O/A) of 2/1, over 64.23% of Li were extracted, and the extraction rate after five-stage extraction could reach more than 96%. The addition of ammonium ions to the solution inhibited the extraction of Ni, and the separation coefficient between lithium and nickel approached infinity, showing a very perfect separation effect. Fourier-transform infrared spectroscopy and slope methods were used to analyze the changes that occurred during extraction, revealing possible extraction mechanisms. In addition, the LiCl solution generated during the preparation of ionic liquids was mixed with the stripping solution, and the battery-grade lithium carbonate was prepared by Na₂CO₃ precipitation, with a purity of 99.74%. This study provides an efficient and sustainable strategy for recovering lithium from the solution.

关键词: Ionic liquids, Selective separation, Solvent extraction, Lithium

Abstract: With the vigorous development of the electronics industry, the consumption of lithium continues to increase, and more lithium needs to be mined to meet the development of the industry. The content of lithium in the solution is much higher than that of minerals, but the interference of impurity ions increases the difficulty of extracting lithium ions. Therefore, we prepared an imidazole-based ionic liquid (1-butyl-3-methylImidazolium bis(trifluoromethyl sulfonyl)imide) (IL) for efficient lithium extraction from aqueous solutions by solvent extraction. Using an extraction consisting of 10% IL, 85% tributyl phosphate (TBP), and 5% dichloroethane and an organic to aqueous phase ratio (O/A) of 2/1, over 64.23% of Li were extracted, and the extraction rate after five-stage extraction could reach more than 96%. The addition of ammonium ions to the solution inhibited the extraction of Ni, and the separation coefficient between lithium and nickel approached infinity, showing a very perfect separation effect. Fourier-transform infrared spectroscopy and slope methods were used to analyze the changes that occurred during extraction, revealing possible extraction mechanisms. In addition, the LiCl solution generated during the preparation of ionic liquids was mixed with the stripping solution, and the battery-grade lithium carbonate was prepared by Na₂CO₃ precipitation, with a purity of 99.74%. This study provides an efficient and sustainable strategy for recovering lithium from the solution.

Key words: Ionic liquids, Selective separation, Solvent extraction, Lithium

Kun Wang, Guoquan Zhang, Linye Li, Yuzhang Li, Xiangxin Liao, Pu Cheng, Mingzhi Luo. Separation of lithium and nickel using ionic liquids and tributyl phosphate[J]. 中国化学工程学报, 2023, 63(11): 63-70.

Kun Wang, Guoquan Zhang, Linye Li, Yuzhang Li, Xiangxin Liao, Pu Cheng, Mingzhi Luo. Separation of lithium and nickel using ionic liquids and tributyl phosphate[J]. Chinese Journal of Chemical Engineering, 2023, 63(11): 63-70.

参考文献

[1] A.N. Arias, A.Y. Tesio, V. Flexer, Review—non-carbonaceous materials as cathodes for lithium-sulfur batteries, J. Electrochem. Soc. 165 (1) (2018) A6119–A6135.
[2] X.C. Zhang, J. Wang, Z.Y. Ji, P.Y. Ji, J.E. Liu, Y.Y. Zhao, F. Li, J.S. Yuan, Preparation of Li₂CO₃ from high Mg²⁺/Li+ brines based on selective-electrodialysis with feed and bleed mode, J. Environ. Chem. Eng. 9 (6) (2021) 106635.
[3] A. Opitz, P. Badami, L. Shen, K. Vignarooban, A.M. Kannan, Can Li-ion batteries be the panacea for automotive applications? Renew. Sustain. Energy Rev. 68 (2017) 685–692.
[4] B. Swain, Separation and purification of lithium by solvent extraction and supported liquid membrane, analysis of their mechanism: A review, J. Chem. Technol. Biotechnol. 91 (10) (2016) 2549–2562.
[5] J.T. Hu, J.L. Zhang, H.X. Li, Y.Q. Chen, C.Y. Wang, A promising approach for the recovery of high value-added metals from spent lithium-ion batteries, J. Power Sources 351 (2017) 192–199.
[6] Y.F. Song, L.H. He, Z.W. Zhao, X.H. Liu, Separation and recovery of lithium from Li₃PO₄ leaching liquor using solvent extraction with saponified D2EHPA, Sep. Purif. Technol. 229 (2019) 115823.
[7] Y.X. Yang, X.H. Zheng, H.B. Cao, C.L. Zhao, X.A. Lin, P.G. Ning, Y. Zhang, W. Jin, Z. Sun, A closed-loop process for selective metal recovery from spent lithium iron phosphate batteries through mechanochemical activation, ACS Sustainable Chem. Eng. 5 (11) (2017) 9972–9980.
[8] B. Swain, Recovery and recycling of lithium: A review, Sep. Purif. Technol. 172 (2017) 388–403.
[9] X. Zhao, H.H. Wu, M.S. Duan, X.C. Hao, Q.W. Yang, Q. Zhang, X.P. Huang, Liquid-liquid extraction of lithium from aqueous solution using novel ionic liquid extractants via COSMO-RS and experiments, Fluid Phase Equilib. 459 (2018) 129–137.
[10] X.Y. Nie, S.Y. Sun, Z. Sun, X.F. Song, J.G. Yu, Ion-fractionation of lithium ions from magnesium ions by electrodialysis using monovalent selective ion-exchange membranes, Desalination 403 (2017) 128–135.
[11] A. Somrani, A.H. Hamzaoui, M. Pontie, Study on lithium separation from salt lake brines by nanofiltration (NF) and low pressure reverse osmosis (LPRO), Desalination 317 (2013) 184-192.
[12] H. Su, Z. Li, J.A. Zhang, W.S. Liu, Z.W. Zhu, L.N. Wang, T. Qi, Combining selective extraction and easy stripping of lithium using a ternary synergistic solvent extraction system through regulation of Fe³⁺ coordination, ACS Sustainable Chem. Eng. 8 (4) (2020) 1971–1979.
[13] C.L. Shi, H.X. Li, B. Liu, Y.R. Qin, G.X. Song, Solvent extraction of lithium from aqueous solution using an ammonium ionic liquid, J. Mol. Liq. 304 (2020) 112756.
[14] B. Liu, S. Wang, Y.Z. Jia, W.B. Zhu, Q.Y. Zhang, X.Q. Wang, Y. Yao, Y. Jing, Lithium isotope separation by crown ethers of different nitrogen-containing derivatives in the ionic liquid-anisole system, J. Mol. Liq. 272 (2018) 548–553.
[15] Á.S. Lima, C.M.F. Soares, R. Paltram, H. Halbwirth, K. Bica, Extraction and consecutive purification of anthocyanins from grape pomace using ionic liquid solutions, Fluid Phase Equilib. 451 (2017) 68–78.
[16] S.S. Swain, B. Nayak, N. Devi, S. Das, N. Swain, Liquid-liquid extraction of cadmium(II) from sulfate medium using phosphonium and ammonium based ionic liquids diluted in kerosene, Hydrometallurgy 162 (2016) 63–70.
[17] S. Marsousi, J. Karimi-Sabet, M. Ali Moosavian, Y. Amini, Liquid-liquid extraction of calcium using ionic liquids in spiral microfluidics, Chem. Eng. J. 356 (2019) 492–505.
[18] Y. Zhang, Y. Deng, W.D. Guo, D.H. Liu, Y.G. Ding, Enhanced homogeneous liquid–liquid extraction for the selective recovery of Sc(III) by novel UCST-type ionic liquids, ACS Sustainable Chem. Eng. 9 (29) (2021) 9932–9940.
[19] G. Zante, D. Trébouet, M. Boltoeva, Solvent extraction of lithium from simulated shale gas produced water with a bifunctional ionic liquid, Appl. Geochem. 123 (2020) 104783.
[20] Y. Zhang, W. Sun, R. Xu, L. Wang, H.H. Tang, Lithium extraction from water lithium resources through green electrochemical-battery approaches: A comprehensive review, J. Clean. Prod. 285 (2021) 124905.
[21] X.A. Su, Z.Y. Zhao, X.Q. Sun, Phenoxy dicarboxylate-type functionalized ionic liquids for selective recovery of valuable metals, Ind. Eng. Chem. Res. 59 (31) (2020) 14075–14084.
[22] C.L. Shi, D.P. Duan, Y.Z. Jia, Y. Jing, A highly efficient solvent system containing ionic liquid in tributyl phosphate for lithium ion extraction, J. Mol. Liq. 200 (2014) 191–195.
[23] C.L. Shi, Y. Jing, J. Xiao, X.Q. Wang, Y. Yao, Y.Z. Jia, Solvent extraction of lithium from aqueous solution using non-fluorinated functionalized ionic liquids as extraction agents, Sep. Purif. Technol. 172 (2017) 473–479.
[24] A. Masmoudi, G. Zante, D. Trébouet, R. Barillon, M. Boltoeva, Solvent extraction of lithium ions using benzoyltrifluoroacetone in new solvents, Sep. Purif. Technol. 255 (2021) 117653.
[25] S.C. Yang, G.W. Liu, J.F. Wang, L. Cui, Y.M. Chen, Recovery of lithium from alkaline brine by solvent extraction with functionalized ionic liquid, Fluid Phase Equilib. 493 (2019) 129–136.
[26] H.S. Zheng, T. Dong, Y.F. Sha, D.F. Jiang, H.T. Zhang, S.J. Zhang, Selective extraction of lithium from spent lithium batteries by functional ionic liquid, ACS Sustainable Chem. Eng. 9 (20) (2021) 7022–7029.
[27] K. Wang, G.Q. Zhang, M.Z. Luo, M.A. Zeng, Separation of Co and Mn from acetic acid leaching solution of spent lithium-ion battery by Cyanex272, J. Environ. Chem. Eng. 10 (5) (2022) 108250.
[28] Z.F. Qin, G.Q. Zhang, Y.J. Xiong, D.M. Luo, C. Li, S.Y. Tang, H.R. Yue, B. Liang, Recovery of vanadium from leach solutions of vanadium slag using solvent extraction with N235, Hydrometallurgy 192 (2020) 105259.
[29] Z.F. Qin, G.Q. Zhang, D.M. Luo, C. Li, H.R. Yue, B. Liang, Separation of titanium from vanadium and iron in leach solutions of vanadium slag by solvent extraction with trioctyl tertiary amine (N235), Hydrometallurgy 188 (2019) 216-221.
[30] V. Mazan, M.Y. Boltoeva, E.E. Tereshatov, C.M. Folden, Mutual solubility of water and hydrophobic ionic liquids in the presence of hydrochloric acid, RSC Adv. 6 (61) (2016) 56260–56270.
[31] J.S. Hu, D. Zou, J. Chen, D.Q. Li, A novel synergistic extraction system for the recovery of scandium (III) by Cyanex272 and Cyanex923 in sulfuric acid medium, Sep. Purif. Technol. 233 (2020) 115977.
[32] C.L. Shi, Y. Jing, Y.Z. Jia, Solvent extraction of lithium ions by tri-n-butyl phosphate using a room temperature ionic liquid, J. Mol. Liq. 215 (2016) 640–646.
[33] A. Masmoudi, G. Zante, D. Trébouet, R. Barillon, M. Boltoeva, Understanding the mechanism of lithium ion extraction using tributyl phosphate in room temperature ionic liquid, Solvent Extr. Ion Exch. 38 (7) (2020) 777–799.