Na2SO4–NaCl binary eutectic salt roasting to enhance extraction of lithium from pyrometallurgical slag of spent lithium-ion batteries

doi:10.1016/j.cjche.2021.09.008

Chinese Journal of Chemical Engineering ›› 2022, Vol. 41 ›› Issue (1): 294-300.DOI: 10.1016/j.cjche.2021.09.008

• Separation Science and Engineering • Previous Articles Next Articles

Na₂SO₄–NaCl binary eutectic salt roasting to enhance extraction of lithium from pyrometallurgical slag of spent lithium-ion batteries

Hui Dang¹, Zhidong Chang¹, Xue Wu², Sihang Ma¹, Yifei Zhan¹, Na Li¹, Wenbo Liu¹, Wenjun Li¹, Hualei Zhou¹, Changyan Sun¹

1 Department of Chemistry and Chemical Engineering, School of Chemistry and Biological Engineering, University of Science and Technology Beijing, Beijing 100083, China;
2 Institute of Biophysics, Chinese Academy of Sciences, Beijing 100101, China

Received:2021-06-02 Revised:2021-09-08 Online:2022-02-25 Published:2022-01-28
Contact: Zhidong Chang,E-mail address:zdchang@ustb.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (21276022).

Na₂SO₄–NaCl binary eutectic salt roasting to enhance extraction of lithium from pyrometallurgical slag of spent lithium-ion batteries

Hui Dang¹, Zhidong Chang¹, Xue Wu², Sihang Ma¹, Yifei Zhan¹, Na Li¹, Wenbo Liu¹, Wenjun Li¹, Hualei Zhou¹, Changyan Sun¹

1 Department of Chemistry and Chemical Engineering, School of Chemistry and Biological Engineering, University of Science and Technology Beijing, Beijing 100083, China;
2 Institute of Biophysics, Chinese Academy of Sciences, Beijing 100101, China

通讯作者: Zhidong Chang,E-mail address:zdchang@ustb.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (21276022).

Abstract

Abstract: Effectively extracting lithium at a relatively low temperature from the slag produced by the pyrometallurgical treatment of spent lithium-ion batteries remains a great challenge, which limits the acquirement of lithium. Herein, we proposed a eutectic system to roast slag at a lower temperature based on sodium sulfate–sodium chloride (Na₂SO₄–NaCl) binary eutectic salts. The optimal roasting conditions are as follows: the slag was roasted at 750 ℃ with a (SO₄^2–+Cl^–)/Li⁺ molar ratio of 5:1 for 120 min. Followed by aqueous leaching 5 min at room temperature with a water/roasted samples mass ratio of 30:1, it can get 97.07% lithium extraction efficiency.

Key words: Spent lithium–ion battery, Lithium recovery, Silicate structure, Binary eutectic salt roasting

摘要： Effectively extracting lithium at a relatively low temperature from the slag produced by the pyrometallurgical treatment of spent lithium-ion batteries remains a great challenge, which limits the acquirement of lithium. Herein, we proposed a eutectic system to roast slag at a lower temperature based on sodium sulfate–sodium chloride (Na₂SO₄–NaCl) binary eutectic salts. The optimal roasting conditions are as follows: the slag was roasted at 750 ℃ with a (SO₄^2–+Cl^–)/Li⁺ molar ratio of 5:1 for 120 min. Followed by aqueous leaching 5 min at room temperature with a water/roasted samples mass ratio of 30:1, it can get 97.07% lithium extraction efficiency.

关键词: Spent lithium–ion battery, Lithium recovery, Silicate structure, Binary eutectic salt roasting

Hui Dang, Zhidong Chang, Xue Wu, Sihang Ma, Yifei Zhan, Na Li, Wenbo Liu, Wenjun Li, Hualei Zhou, Changyan Sun. Na₂SO₄–NaCl binary eutectic salt roasting to enhance extraction of lithium from pyrometallurgical slag of spent lithium-ion batteries[J]. Chinese Journal of Chemical Engineering, 2022, 41(1): 294-300.

References

[1] R. Wang, W. Cui, F. Chu, F. Wu, Lithium metal anodes:Present and future, J. Energy Chem. 48(2020)145-159.
[2] F. Wu, G. Yushin, Conversion cathodes for rechargeable lithium and lithiumion batteries, Energy Environ. Sci. 10(2)(2017)435-459.
[3] A. Manthiram, A reflection on lithium-ion battery cathode chemistry, Nat. Commun. 11(1)(2020)1550.
[4] G. Harper, R. Sommerville, E. Kendrick, L. Driscoll, P. Slater, R. Stolkin, A. Walton, P. Christensen, O. Heidrich, S. Lambert, A. Abbott, K. Ryder, L. Gaines, P. Anderson, Recycling lithium-ion batteries from electric vehicles, Nature 575(7781)(2019)75-86.
[5] C. Liu, J. Lin, H. Cao, Y.i. Zhang, Z. Sun, Recycling of spent lithium-ion batteries in view of lithium recovery:A critical review, J. Clean. Prod. 228(2019)801-813.
[6] J. Xiao, J. Li, Z. Xu, Challenges to future development of spent lithium ion batteries recovery from environmental and technological perspectives, Environ. Sci. Technol. 54(1)(2020)9-25.
[7] J. Xiao, B.o. Niu, Q. Song, L.u. Zhan, Z. Xu, Novel targetedly extracting lithium: An environmental-friendly controlled chlorinating technology and mechanism of spent lithium ion batteries recovery, J. Hazard. Mater. 404(2021)123947.
[8] Y.Q. Tang, B.L. Zhang, H.W. Xie, X. Qu, P.F. Xing, H.Y. Yin, Recovery and regeneration of lithium cobalt oxide from spent lithium-ion batteries through a low-temperature ammonium sulfate roasting approach, J. Power Sources 474(2020)228596.
[9] T. Georgi-Maschler, B. Friedrich, R. Weyhe, H. Heegn, M. Rutz, Development of a recycling process for Li-ion batteries, J. Power Sources. 207(2012)173-182.
[10] F. Wang, T. Zhang, Y. He, Y. Zhao, S. Wang, G. Zhang, Y.u. Zhang, Y.i. Feng, Recovery of valuable materials from spent lithium-ion batteries by mechanical separation and thermal treatment, J. Clean. Prod. 185(2018)646-652.
[11] H. Dang, B. Wang, Z. Chang, X. Wu, J. Feng, H. Zhou, W. Li, C. Sun, Recycled lithium from simulated pyrometallurgical slag by chlorination roasting, ACS Sustainable Chem. Eng. 6(10)(2018)13160-13167.
[12] L.C. Zhang, L.J. Li, H.M. Rui, D. Shi, X.W. Peng, L.M. Ji, X.X. Song, Lithium recovery from effluent of spent lithium battery recycling process using solvent extraction, J. Hazard. Mater. 398(2020)122840.
[13] P. Yadav, C.J. Jie, S. Tan, M. Srinivasan, Recycling of cathode from spent lithium iron phosphate batteries, J. Hazard. Mater. 399(2020)123068.
[14] X.P. Chen, D.Z. Kang, J.Z. Li, T. Zhou, H.R. Ma, Gradient and facile extraction of valuable metals from spent lithium ion batteries for new cathode materials refabrication, J. Hazard. Mater. 389(2020)121887.
[15] S.Y. Lei, Y. Cao, X.F. Cao, W. Sun, Y.Q. Weng, Y. Yang, Separation of lithium and transition metals from leachate of spent lithium-ion batteries by solvent extraction method with Versatic 10, Sep. Purif. Technol. 250(2020)117258.
[16] D. Cheret, S. Santen, Battery recycling, U.S. Pat., 7169206(2007).
[17] J. Heulens, D. Horebeek, M. Quix, S. Brouwer, Process for smelting lithium-ion batteries, U.S. Pat., 20170229744A1(2017).
[18] H. Dang, N. Li, Z.D. Chang, B.F. Wang, Y.F. Zhan, X. Wu, W.B. Liu, S. Ali, H.D. Li, J. H. Guo, W.J. Li, H.L. Zhou, C.Y. Sun, Lithium leaching via calcium chloride roasting from simulated pyrometallurgical slag of spent lithium ion battery, Sep. Purif. Technol. 233(2020)116025.
[19] Q.-X. YAN, X.-H. LI, Z.-X. WANG, J.-x. WANG, H.-J. GUO, Q.-Y. HU, W.-J. PENG, X.-F. WU, Extraction of lithium from lepidolite using chlorination roastingwater leaching process, Trans. Nonferrous. Met. Soc. China 22(7)(2012)1753-1759.
[20] X.F. Zhang, T. Aldahri, X.M. Tan, W.Z. Liu, L.Z. Zhang, S.W. Tang, Efficient coextraction of lithium, rubidium, cesium and potassium from lepidolite by process intensification of chlorination roasting, Chem. Eng. Process.-Process Intensif. 147(2020)107777.
[21] L.I. Barbosa, J.A. González, M.D.C. Ruiz, Extraction of lithium from bspodumene using chlorination roasting with calcium chloride, Thermochim. Acta 605(2015)63-67.
[22] T.T. Hien-Dinh, V.T. Luong, R. Gieré, T. Tran, Extraction of lithium from lepidolite via iron sulphide roasting and water leaching, Hydrometallurgy 153(2015)154-159.
[23] H. Su, J.Y. Ju, J. Zhang, A.F. Yi, Z. Lei, L.N. Wang, Z.W. Zhu, T. Qi, Lithium recovery from lepidolite roasted with potassium compounds, Miner. Eng. 145(2020) 106087.
[24] N.a. Li, J. Guo, Z. Chang, H. Dang, X. Zhao, S. Ali, W. Li, H. Zhou, C. Sun, Aqueous leaching of lithium from simulated pyrometallurgical slag by sodium sulfate roasting, RSC Adv. 9(41)(2019)23908-23915.
[25] L.L.D. Santos, R.M.D. Nascimento, S.B.C. Pergher, Beta-spodumene:Na₂CO₃: NaCl system calcination:A kinetic study of the conversion to lithium salt, Chem. Eng. Res. Des. 147(2019)338-345.
[26] B.i. Yang, J. Zhou, W. Wang, C. Liu, D. Zhou, L. Yang, Extraction and separation of tungsten and vanadium from spent V₂O₅-WO₃/TiO₂ SCR catalysts and recovery of TiO₂ and sodium titanate nanorods as adsorbent for heavy metal ions, Colloids Surf. A:Physicochem. Eng. Aspects 601(2020)124963.
[27] C. Song, D. Zhou, L. Yang, J. Zhou, C. Liu, Z.-G. Chen, Recovery TiO₂ and sodium titanate nanowires as Cd (II) adsorbent from waste V₂O₅-WO₃/TiO₂ selective catalytic reduction catalysts by Na₂CO₃-NaCl-KCl molten salt roasting method, J. Taiwan Inst. Chem. Eng. 88(2018)226-233.
[28] V.T. Luong, D.J. Kang, J.W. An, M.J. Kim, T. Tran, Factors affecting the extraction of lithium from lepidolite, Hydrometallurgy 134-135(2013)54-61.
[29] Y. Jiang, Y. Sun, R.D. Jacob, F. Bruno, S. Li, Novel Na₂SO₄-NaCl-ceramic composites as high temperature phase change materials for solar thermal power plants (Part I), Sol. Energy Mater. Sol. Cells 178(2018)74-83.
[30] K. Verscheure, M. Campforts, M. Camp, Process for the valorization of metals from Li-ion batteries, U.S. Pat. 8840702B2(2014).
[31] G.-X. REN, S.-W. XIAO, M.-Q. XIE, B. PAN, J. CHEN, F.-G. WANG, X. XIA, Recovery of valuable metals fromspent lithium ion batteries by smelting reduction process based on FeO-SiO₂-Al₂O₃ slag system, Trans. Nonferrous Met. Soc. China 27(2)(2017)450-456.
[32] M.R.B. Guerrero, J.M. Salinas Gutiérrez, M.J. Meléndez Zaragoza, A. López Ortiz, V. Collins-Martínez, Optimal slow pyrolysis of apple pomace reaction conditions for the generation of a feedstock gas for hydrogen production, Int. J. Hydrog. Energy 41(48)(2016)23232-23237.
[33] S. Olivotos, M. Economou-Eliopoulos, Gibbs free energy of formation for selected platinum group minerals (PGM), Geoscience 6(1)(2016)2.
[34] A. Roine, HSC, 6.0 Chemistry. Chemical reactions and equilibrium software with extensive thermochemical database and flowsheet simulation, Outokumpu Research Oy Information Center, Pori, 2006, p. 448.
[35] N. Marzari, D. Vanderbilt, M.C. Payne, Ensemble density-functional theory forab-initio molecular dynamics of metals and finite-temperature insulators, Phys. Rev. Lett. 79(7)(1997)1337.
[36] R.O. Jones, O. Gunnarsson, The density functional formalism, its applications and prospects, Rev. Mod. Phys. 61(3)(1989)689-746.
[37] W. Kohn, L.J. Sham, Self-consistent equations including exchange and correlation effects, Phys. Rev. 140(4A)(1965) A1133-A1138.
[38] John P. Perdew, Kieron Burke, Matthias Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77(18)(1996)3865-3868.
[39] Hendrik J. Monkhorst, James D. Pack, Special points for Brillouin-zone integrations, Phys. Rev. B 13(12)(1976)5188-5192.
[40] J.P. Perdew, J.A. Chevary, S.H. Vosko, K.A. Jackson, M.R. Pederson, D.J. Singh, C. Fiolhais, Atoms, molecules, solids, and surfaces:Applications of the generalized gradient approximation for exchange and correlation, Phys. Rev. B 46(1992)6671-6687.

Na₂SO₄–NaCl binary eutectic salt roasting to enhance extraction of lithium from pyrometallurgical slag of spent lithium-ion batteries

Na₂SO₄–NaCl binary eutectic salt roasting to enhance extraction of lithium from pyrometallurgical slag of spent lithium-ion batteries

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