Skip to main content
SpringerLink
Log in

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

  • Research Article
  • Published:
Frontiers of Chemical Science and Engineering Aims and scope Submit manuscript

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.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Similar content being viewed by others

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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  PubMed  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  CAS  Google Scholar 

  28. Hong H J, Park I S, Ryu T, Ryu J, Kim B G, Chung K S. Granulation of Li1.33Mn1.67O4 (LMO) through the use of cross-linked chitosan for the effective recovery of Li+ from seawater. Chemical Engineering Journal, 2013, 234: 16–22

    Article  CAS  Google Scholar 

  29. Zhu G R, Wang P, Qi P F, Gao C J. Adsorption and desorption properties of Li+ on PVC-H1.6Mn1.6O4 lithium ion-sieve membrane. Chemical Engineering Journal, 2014, 235(1): 340–348

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

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

    Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

  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

    Article  CAS  Google Scholar 

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

    Google Scholar 

Download references

Acknowledgements

The authors acknowledge financial support for this research from the National Key Research and Development Program of China (No. 2017YFB0403300 and 2017YFB0403305), the National Natural Science Foundation of China (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).

Author information

Authors and Affiliations

  1. State Key Laboratory of Advanced Metallurgy, University of Science and Technology Beijing, Beijing, 100083, China

    Chunlong Zhao & Yanling Zhang

  2. Beijing Engineering Research Center of Process Pollution Control, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, China

    Chunlong Zhao, Mingming He, Hongbin Cao, Xiaohong Zheng, Wenfang Gao, He Zhao & Zhi Sun

  3. University of Nottingham Ningbo China, Ningbo, 315100, China

    Yong Sun

  4. Henan Bingsheng Biotechnology Company Limited, Kaifeng, 475103, China

    Dalong Liu

Authors
  1. Chunlong Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Mingming He
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Hongbin Cao
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Xiaohong Zheng
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Wenfang Gao
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Yong Sun
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. He Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Dalong Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Yanling Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Zhi Sun
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Zhi Sun.

Electronic supplementary material

11705_2019_1806_MOESM1_ESM.pdf

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

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhao, C., He, M., Cao, H. et al. Investigation of solution chemistry to enable efficient lithium recovery from low-concentration lithium-containing wastewater. Front. Chem. Sci. Eng. 14, 639–650 (2020). https://doi.org/10.1007/s11705-019-1806-3

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11705-019-1806-3

Keywords

Search

Navigation