Investigation of solution chemistry to enable efficient lithium recovery from low-concentration lithium-containing wastewater

Abstract

In the production of lithium-ion batteries (LIBs) and recycling of spent LIBs, a large amount of low-concentration lithium-containing wastewater (LCW) is generated. The recovery of Li from this medium has attracted significant global attention from both the environmental and economic perspectives. To achieve effective Li recycling, the features of impurity removal and the interactions among different ions must be understood. However, it is generally difficult to ensure highly efficient removal of impurity ions while retaining Li in the solution for further recovery. In this study, the removal of typical impurity ions from LCW and the interactions between these species were systematically investigated from the thermodynamic and kinetics aspects. It was found that the main impurities (e.g., Fe³⁺, Al³⁺, Ca²⁺, and Mg²⁺) could be efficiently removed with high Li recovery by controlling the ionic strength of the solution. The mechanisms of Fe³⁺, Al³⁺, Ca²⁺, and Mg²⁺ removal were investigated to identify the controlling steps and reaction kinetics. It was found that the precipitates are formed by a zero-order reaction, and the activation energies tend to be low with a sequence of fast chemical reactions that reach equilibrium very quickly. Moreover, this study focused on Li loss during removal of the impurities, and the corresponding removal rates of Fe³⁺, Al³⁺, Ca²⁺, and Mg²⁺ were found to be 99.8%, 99.5%, 99%, and 99.7%, respectively. Consequently, high-purity Li₃PO₄ was obtained via one-step precipitation. Thus, this research demonstrates a potential route for the effective recovery of Li from low-concentration LCW and for the appropriate treatment of acidic LCW.

Graphical abstract

Keywords

lithium-containing wastewater / lithium phosphate / precipitation / impurity ion

References

[1] Chi S S, Liu Y, Song W L, Fan L Z, Zhang Q. Prestoring lithium into stable 3D nickel foam host as dendrite-free lithium metal anode. Advanced Functional Materials, 2017, 27(24): 1700348

[2] Etacheri V, Marom R, Elazari R, Salitra G, Aurbach D. Challenges in the development of advanced Li-ion batteries: A review. Energy & Environmental Science, 2011, 4(9): 3243–3262

[3] Lv W G, Wang Z H, Cao H B, Sun Y, Zhang Y, Sun Z. A critical review and analysis on the recycling of spent lithium-ion batteries. ACS Sustainable Chemistry & Engineering, 2018, 6(2): 1504–1521

[4] Zeng X L, Li J H, Shen B Y. Novel approach to recover cobalt and lithium from spent lithium-ion battery using oxalic acid. Journal of Hazardous Materials, 2015, 295: 112–118

[5] Li L, Qu W J, Zhang X X, Lu J, Chen R J, Wu F, Amine K. Succinic acid-based leaching system: A sustainable process for recovery of valuable metals from spent Li-ion batteries. Journal of Power Sources, 2015, 282: 544–551

[6] Zheng X H, Gao W F, Zhang X H, He M M, Lin X, Cao H B, Zhang Y, Sun Z. Spent lithium-ion battery recycling-Reductive ammonia leaching of metals from cathode scrap by sodium sulphite. Waste Management (New York, N.Y.), 2017, 60: 680–688

[7] Swain B. Recovery and recycling of lithium: A review. Separation and Purification Technology, 2017, 172: 388–403

[8] Yu L H, Miao J S, Jin Y, Lin Y S. A comparative study on polypropylene separators coated with different inorganic materials for lithium-ion batteries. Frontiers of Chemical Science and Engineering, 2017, 11(3): 346–352

[9] Wang S Q, Guo Y F, Zhang N, Bu L Z, Deng T L, Zheng M P. Caloric evaporation of the brine in Zangnan Salt Lake. Frontiers of Chemical Science and Engineering, 2011, 5(3): 343–348

[10] Vieceli N, Nogueira C A, Pereira M F C, Durão F O, Guimarães C, Margarido F. Recovery of lithium carbonate by acid digestion and hydrometallurgical processing from mechanically activated lepidolite. Hydrometallurgy, 2018, 175: 1–10

[11] Wang H Y, Zhong Y, Du B Q, Zhao Y J, Wang M. Recovery of both magnesium and lithium from high Mg/Li ratio brines using a novel process. Hydrometallurgy, 2018, 175: 102–108

[12] Schneidera A, Schmidta H, Mevenb M, Brendlerc E, Kirchnerd J, Martine G, Bertaue M, Voigt W. Lithium extraction from the mineral zinnwaldite: Part I: Effect of thermal treatment on properties and structure of zinnwaldite. Minerals Engineering, 2017, 111: 55–67

[13] Jandová J P, Dvořák P, Vu H N. Processing of zinnwaldite waste to obtain Li₂CO₃. Hydrometallurgy, 2010, 103(1-4): 12–18

[14] Yang S X, Zhang F, Ding H P, He P, Zhou H S. Lithium metal extraction from seawater. Joule, 2018, 2(9): 1648–1651

[15] Kesler S E, Gruber P W, Medina P A, Keoleian G A, Everson M P, Wallington T J. Global lithium resources: Relative importance of pegmatite, brine and other deposits. Ore Geology Reviews, 2012, 48(5): 55–69

[16] Luo X B, Guo B, Luo J M, Deng F, Zhang S Y, Luo S L, Crittenden J. Recovery of lithium from wastewater using development of Li ion-imprinted polymers. ACS Sustainable Chemistry & Engineering, 2015, 3(3): 460–467

[17] Sun Z, Cao H B, Venkatesan P, Jin W, Xiao Y P, Sietsma J, Yang Y X. Electrochemistry during efficient copper recovery from complex electronic waste using ammonia based solutions. Frontiers of Chemical Science and Engineering, 2017, 11(3): 308–316

[18] Xu X, Chen Y M, Wang P Y, Gasem K, Wang K Y, He T, Adidharma H, Fan M H. Extraction of lithium with functionalized lithium ion sieves. Progress in Materials Science, 2016, 84: 276–313

[19] Zandevakili S, Ranjbar M, Ehteshamzadeh M. Recovery of lithium from Urmia Lake by a nanostructure MnO₂ ion sieve. Hydrometallurgy, 2014, 149: 148–152

[20] Yan Q X, Li X H, Wang Z X, Wu X F, Wang J X, Guo H J, Hu Q Y, Peng W J. Extraction of lithium from lepidolite by sulfation roasting and water leaching. International Journal of Mineral Processing, 2012, 110-111: 1–5

[21] Kong W B, Miao Q, Qing P Y, Baeyens J, Tan T W. Environmental and economic assessment of vegetable oil production using membrane separation and vapor recompression. Frontiers of Chemical Science and Engineering, 2017, 11(2): 166–176

[22] Somrani A, Hamzaoui A H, Pontie M. Study on lithium separation from salt lake brines by nanofiltration (NF) and low pressure reverse osmosis (LPRO). Desalination, 2013, 317: 184–192

[23] Fridman-Bishop N, Tankus K A, Freger V. Permeation mechanism and interplay between ions in nanofiltration. Journal of Membrane Science, 2018, 548: 449–458

[24] Chen Q B, Ji Z Y, Liu J, Zhao Y Y, Wang S Z, Yuan J S. Development of recovering lithium from brines by selective-electrodialysis: Effect of coexisting cations on the migration of lithium. Journal of Membrane Science, 2018, 548: 408–420

[25] Ji Z Y, Chen Q B, Yuan J S, Liu J, Zhao Y Y, Feng W X. Preliminary study on recovering lithium from high Mg²⁺/Li⁺ ratio brines by electrodialysis. Separation and Purification Technology, 2017, 172: 168–177

[26] Kim S, Kim J, Kim S, Lee J, Yoon J. Electrochemical lithium recovery and organic pollutant removal from industrial wastewater of a battery recycling plant. Environmental Science. Water Research & Technology, 2017, 4(2): 175–182

[27] Ooi K, Sonoda A, Makita Y, Chitrakar R, Tasaki-Handa Y, Nakazato T. Recovery of lithium from salt-brine eluates by direct crystallization as lithium sulfate. Hydrometallurgy, 2017, 174: 123–130

[28] Hong H J, Park I S, Ryu T, Ryu J, Kim B G, Chung K S. Granulation of Li_1.33Mn_1.67O₄ (LMO) through the use of cross-linked chitosan for the effective recovery of Li⁺ from seawater. Chemical Engineering Journal, 2013, 234: 16–22

[29] Zhu G R, Wang P, Qi P F, Gao C J. Adsorption and desorption properties of Li⁺ on PVC-H_1.6Mn_1.6O₄ lithium ion-sieve membrane. Chemical Engineering Journal, 2014, 235(1): 340–348

[30] Wang S L, Zheng S L, Wang Z M, Cui W W, Zhang H L, Yang L R, Zhang Y, Li P. Superior lithium adsorption and required magnetic separation behavior of iron-doped lithium ion-sieves. Chemical Engineering Journal, 2018, 332: 160–168

[31] Zhang L Y, Zhou D L, Yao Q Q, Zhou J B. Preparation of H₂TiO₃-lithium adsorbent by the sol–gel process and its adsorption performance. Applied Surface Science, 2016, 368: 82–87

[32] Paranthaman M P, Li L, Luo J Q, Hoke T, Ucar H, Moyer B A, Harrison S. Recovery of lithium from geothermal brine with lithium-aluminum layered double hydroxide chloride sorbents. Environmental Science & Technology, 2017, 51(22): 13481–13486

[33] Mishra B, Costu S. Materials sustainability for environment: Red-mud treatment. Frontiers of Chemical Science and Engineering, 2017, 11(3): 483–496

[34] Luo X B, Zhang K, Luo J M, Luo S L, Crittenden J. Capturing lithium from wastewater using a fixed bed packed with 3-D MnO₂ ion cages. Environmental Science & Technology, 2016, 50(23): 13002–13012

[35] Pranolo Y, Zhu Z W, Cheng C Y. Separation of lithium from sodium in chloride solutions using SSX systems with LIX 54 and Cyanex 923. Hydrometallurgy, 2015, 154: 33–39

[36] Li X H, Zhang C J, Zhang S N, Li J X, He B Q, Cui Z Y. Preparation and characterization of positively charged polyamide composite nanofiltration hollow fiber membrane for lithium and magnesium separation. Desalination, 2015, 369: 26–36

[37] Nie X Y, Sun S Y, Sun Z, Song X F, Yu J G. Ion-fractionation of lithium ions from magnesium ions by electrodialysis using monovalent selective ion-exchange membranes. Desalination, 2017, 403: 128–135

[38] Gao W F, Zhang X H, Zheng X H, Lin X, Cao H B, Zhang Y, Sun Z. Lithium carbonate recovery from cathode scrap of spent lithium-ion battery: A closed-loop process. Environmental Science & Technology, 2017, 51(3): 1662–1669

[39] Yang Y X, Zheng X H, Cao H B, Zhao C L, Lin X, Ning P G, Zhang Y, Jin W, Sun Z. A closed-loop process for selective metal recovery from spent lithium iron phosphate batteries through mechanochemical activation. ACS Sustainable Chemistry & Engineering, 2017, 5(11): 9972–9980

[40] Song Y F, Zhao Z W. Recovery of lithium from spent lithium-ion batteries using precipitation and electrodialysis techniques. Separation and Purification Technology, 2018, 206: 335–342

[41] Liang Y J. Practical Inorganic Thermodynamic Data Sheet. Shenyang: Northeastern University Press, 1993, 614–620

[42] Pesterfield L L, Maddox J B, Crocker M S, Schweitzer G K. Pourbaix (E-pH-M) diagrams in three dimensions. Journal of Chemical Education, 2012, 89(7): 891–899

[43] Sun Z, Cao H B, Xiao Y P, Sietsma S, Jin W, Agterhuis H, Yang Y X. Toward sustainability for recovery of critical metals from electronic waste: The hydrochemistry processes. ACS Sustainable Chemistry & Engineering, 2017, 5(1): 21–40

[44] Tan X T, Chang P P, Fan Q H, Zhou X, Yu S M, Wu M W, Wang X K. Sorption of Pb(II) on Na-rectorite: Effects of pH, ionic strength, temperature, soil humic acid and fulvic acid. Colloids and Surfaces. A, Physicochemical and Engineering Aspects, 2008, 328(1-3): 8–14

[45] Li H G. Metallurgical Principle. Beijing: Science Press, 2017, 291–316

Acknowledgements

The authors acknowledge financial support for this research from the National Key Research and Development Program of China (No. 2017YFB0403300/2017YFB0403305), the National Natural Science Foundation of China and (Grant Nos. 51425405, 51674022, and L1624051), Key Program of Chinese Academy of Sciences KFZD-SW-315, and 1000 Talents Program of China (Z.S.), as well as the Shanxi Provincial Science and Technology Major Projects (MC2016-05).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-019-1806-3 and is accessible for authorized users.

RIGHTS & PERMISSIONS

2020 Higher Education Press