Skip to main content
Log in

An overview on the processes and technologies for recycling cathodic active materials from spent lithium-ion batteries

  • SPECIAL FEATURE: REVIEW
  • The 7th International Conference on Waste Management and Technology (ICWMT) 2012
  • Published:
Journal of Material Cycles and Waste Management Aims and scope Submit manuscript

Abstract

This paper aims to make an overview on the current status and new tendency for recycling cathodic active materials from spent lithium-ion batteries. Firstly, it introduces several kinds of pretreatment technologies, followed by the summary of all kinds of single recycling processes mainly focusing on organic acid leaching and synergistic extraction. Then, several examples of typical combined processes and industrial recycling processes are presented in detail. Meanwhile, the advantages, disadvantages and prospect of each single process, combined process, as well as industrial recycling processes, are discussed. Finally, based on a novel acidic organic solvent, the authors briefly introduce an environmental friendly process to directly recycle and resynthesize cathodic active material LiNi1/3Co1/3Mn1/3O2 from spent lithium-ion batteries. The preliminary experimental results demonstrated the advantages of low reaction temperature, high separation efficiency and organic solvent cycling and preventing secondary pollution to the environment. This process may be used for large-scale recycling of spent lithium-ion batteries after further study.

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

Access this article

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

Instant access to the full article PDF.

Fig. 1
Fig. 2

Similar content being viewed by others

References

  1. Etacheri V, Marom R, Elazari R, Salitra G, Aurbach D (2011) Challenges in the development of advanced Li-ion batteries: a review. Energy Environ Sci 4:3243–3262

    Article  Google Scholar 

  2. Bruno Scrosati B, Hassoun J, Sun YK (2011) Lithium-ion batteries. A look into the future. Energy Environ Sci 4:3287–3295

    Article  Google Scholar 

  3. Ra DI, Han KS (2006) Used lithium ion rechargeable battery recycling using Etoile-Rebatt technology. J Power Sources 163:284–288

    Article  Google Scholar 

  4. Nan J, Han D, Zuo X (2005) Recovery of metal values from spent lithium-ion batteries with chemical deposition and solvent extraction. J Power Sources 152:278–284

    Article  Google Scholar 

  5. http://www.meti.go.jp/english/statistics/index.html. Accessed 28 Dec 2011

  6. http://www.chinabattery.org/index.php/archives/14608. Accessed 1 Oct 2012

  7. Suzuki T, Nakamura T, Inoue Y, Niinae M, Shibata J (2012) A hydrometallurgical process for the separation of aluminum, cobalt, copper and lithium in acidic sulfate media. Sep Purif Technol 98:396–401

    Article  Google Scholar 

  8. Contestabile M, Panero S, Scrosati B (2001) A laboratory-scale lithium-ion battery recycling process. J Power Sources 92:65–69

    Article  Google Scholar 

  9. http://www.miit.gov.cn/n11293472/n11293832/n11294132/n12858447/14536179.html. Accessed 30 Mar 2012

  10. Lee CK, Rhee KI (2003) Reductive leaching of cathodic active materials from lithium ion battery wastes. Hydrometallurgy 68:5–10

    Article  Google Scholar 

  11. Bernardes AM, Espinosa DCR, Tenório JAS (2004) Recycling of batteries: a review of current processes and technologies. J Power Sources 130:291–298

    Article  Google Scholar 

  12. Wu Q, Lu W, Prakash J (2000) Characterization of a commercial size cylindrical Li-ion cell with a reference electrode. J Power Sources 88:237–242

    Article  Google Scholar 

  13. Iwakura C, Fukumoto Y, Inoue H, Ohashi S, Kobayashi S, Tada H, Abe M (1997) Electrochemical characterization of various metal foils as a current collector of positive electrode for rechargeable lithium batteries. J Power Sources 68:301–303

    Article  Google Scholar 

  14. Chen JM, Yao CY, Sheu SP, Chiou YC, Shih HC (1997) The study of carbon half-cell voltage in lithium-ion secondary batteries. J Power Sources 68:242–244

    Article  Google Scholar 

  15. Shin SM, Kim NH, Sohn JS, Yang DH, Kim YH (2005) Development of a metal recovery process from Li-ion battery wastes. Hydrometallurgy 79:172–181

    Article  Google Scholar 

  16. Dorella G, Mansur MB (2007) A study of the separation of cobalt from spent Li-ion battery residues. J Power Sources 170:210–215

    Article  Google Scholar 

  17. Bernardes AM, Espinosa DCR, Tenório JAS (2003) Collection and recycling of portable batteries: a worldwide overview compared to the Brazilian situation. J Power Sources 124:586–592

    Article  Google Scholar 

  18. Espinosa DCR, Bernardes AM, Tenório JAS (2004) An overview on the current processes for the recycling of batteries. J Power Sources 135:311–319

    Article  Google Scholar 

  19. Xu J, Thomas HR, Francis RW, Lum KR, Wang J, Liang B (2008) A review of processes and technologies for the recycling of lithium-ion secondary batteries. J Power Sources 177:512–527

    Article  Google Scholar 

  20. Contestabile M, Panero S, Scrosati B (1999) A laboratory-scale lithium battery recycling process. J Power Sources 83:75–78

    Article  Google Scholar 

  21. Li J, Shi P, Wang Z, Chen Y, Chang CC (2009) A combined recovery process of metals in spent lithium-ion batteries. Chemosphere 77:1132–1136

    Article  Google Scholar 

  22. Li L, Chen R, Sun F, Wu F, Liu J (2011) Preparation of LiCoO2 films from spent lithium-ion batteries by a combined recycling process. Hydrometallurgy 108:220–225

    Article  Google Scholar 

  23. Li L, Lu J, Ren Y, Zhang XX, Chen RJ, Wu F, Amine K (2012) Ascorbic-acid assisted recovery of cobalt and lithium from spent Li-ion batteries. J Power Sources 218:21–27

    Article  Google Scholar 

  24. Li L, Ge J, Wu F, Chen R, Chen S, Wu B (2010) Recovery of cobalt and lithium from spent lithium ion batteries using organic citric acid as leachant. J Hazard Mater 176:288–293

    Article  Google Scholar 

  25. Li L, Ge J, Chen R, Wu F, Chen S, Zhang X (2010) Environmental friendly leaching reagent for cobalt and lithium recovery from spent lithium-ion batteries. Waste Manag 30:2615–2621

    Article  Google Scholar 

  26. Chen L, Tang X, Zhang Y, Li L, Zeng Z, Zhang Y (2011) Process for the recovery of cobalt oxalate from spent lithium-ion batteries. Hydrometallurgy 108:80–86

    Article  Google Scholar 

  27. Ferreira DA, Prados LMZ, Majuste D, Mansur MB (2009) Hydrometallurgical separation of aluminium, cobalt, copper and lithium from spent Li-ion batteries. J Power Sources 187:238–246

    Article  Google Scholar 

  28. Nan J, Han D, Yang M, Cui M, Hou X (2006) Recovery of metal values from a mixture of spent lithium-ion batteries and nickel-metal hydride batteries. Hydrometallurgy 84:75–80

    Article  Google Scholar 

  29. Lee CK, Rhee KI (2002) Preparation of LiCoO2 from spent lithium-ion batteries. J Power Sources 109:17–21

    Article  Google Scholar 

  30. Sun L, Qiu K (2012) Organic oxalate as leachant and precipitant for the recovery of valuable metals from spent lithium-ion batteries. Waste Manag 32:1575–1582

    Article  MathSciNet  Google Scholar 

  31. Sun L, Qiu K (2011) Vacuum pyrolysis and hydrometallurgical process for the recovery of valuable metals from spent lithium-ion batteries. J Hazard Mater 194:378–384

    Article  Google Scholar 

  32. Paulino JF, Busnardo NG, Afonso JC (2008) Recovery of valuable elements from spent Li-batteries. J Hazard Mater 150:843–849

    Article  Google Scholar 

  33. Mishra D, Kim D, Ralph DE, Ahn J, Rhee Y (2008) Bioleaching of metals from spent lithium ion secondary batteries using Acidithiobacillus ferrooxidans. Waste Manag 28:333–338

    Article  Google Scholar 

  34. Zeng G, Deng X, Luo S, Luo X, Zou J (2012) A copper-catalyzed bioleaching process for enhancement of cobalt dissolution from spent lithium-ion batteries. J Hazard Mater 199–200:164–169

    Article  Google Scholar 

  35. Xin B, Zhang D, Zhang X, Xia Y, Wu F, Chen S, Li L (2009) Bioleaching mechanism of Co and Li from spent lithium-ion battery by the mixed culture of acidophilic sulfur-oxidizing and iron-oxidizing bacteria. Bioresource Technol 100:6163–6169

    Article  Google Scholar 

  36. Huang K, Li J, Xu ZM (2009) A novel process for recovering valuable metals from waste nickel-cadmium batteries. Environ Sci Technol 43:8974–8978

    Article  Google Scholar 

  37. Pietrelli L, Bellomo B, Fontana D, Montereali M (2005) Characterization and leaching of NiCd and NiMH spent batteries for the recovery of metals. Waste Manag 25:221–226

    Article  Google Scholar 

  38. Zhang P, Yokoyama T, Itabashi O, Suzuki TM, Inoue K (1998) Hydrometallurgical process for recovery of metal values from spent lithium-ion secondary batteries. Hydrometallurgy 47:259–271

    Article  Google Scholar 

  39. Castillo S, Ansart F, Laberty-Robert C, Portal J (2002) Advances in the recovering of spent lithium battery compounds. J Power Sources 112:247–254

    Article  Google Scholar 

  40. Aktas S, Fray DJ, Burheim O, Fenstad J, Acma E (2006) Recovery of metallic values from spent Li ion secondary batteries. Miner Process Extr M (Trans Inst Min Metall C) 115:95–100

    Article  Google Scholar 

  41. Wang RC, Lin YC, Wu SH (2009) A novel recovery process of metal values from the cathode active materials of the lithium-ion secondary batteries. Hydrometallurgy 99:194–201

    Article  Google Scholar 

  42. Li J, Li X, Hu Q, Wang Z, Zheng J, Wu L, Zhang L (2009) Study of extraction and purification of Ni, Co and Mn from spent battery material. Hydrometallurgy 99:7–12

    Article  Google Scholar 

  43. Li J, Li X, Zhang Y, Hu Q, Wang Z, Zhou Y (2009) Study of spent battery material leaching process. Trans Nonferrous Met Soc China 19:751–755

    Article  Google Scholar 

  44. Kang J, Senanayake G, Sohn J, Shin SM (2010) Recovery of cobalt sulfate from spent lithium ion batteries by reductive leaching and solvent extraction with Cyanex 272. Hydrometallurgy 100:168–171

    Article  Google Scholar 

  45. Kang J, Sohn J, Chang H, Senanayake G, Shin SM (2010) Preparation of cobalt oxide from concentrated cathode material of spent lithium ion batteries by hydrometallurgical method. Adv Powder Technol 21:175–179

    Article  Google Scholar 

  46. Lupi C, Pasquali M (2003) Electrolytic nickel recovery from lithium-ion batteries. Miner Eng 16:537–542

    Article  Google Scholar 

  47. Wang F, He F, Zhao J, Sui N, Xu L, Liu H (2012) Extraction and separation of cobalt(II), copper(II) and manganese(II) by Cyanex 272, PC-88A and their mixtures. Sep Purif Technol 93:8–14

    Article  Google Scholar 

  48. Zhao JM, Shen XY, Deng FL, Wang FC, Wu Y, Liu HZ (2011) Synergistic extraction and separation of valuable metals from waste cathodic material of lithium ion batteries using Cyanex 272 and PC-88A. Sep Purif Technol 78:345–351

    Article  Google Scholar 

  49. Cerpa A, Alguacil FJ (2004) Separation of cobalt and nickel from acidic sulfate solutions using mixtures of di(2-ethylhexyl)phosphoric acid (DP-8R) and hydroxyoxime (ACORGA M5640). J Chen Technol Biot 79:455–460

    Article  Google Scholar 

  50. Cheng CY (2006) Solvent extraction of nickel and cobalt with synergistic systems consisting of carboxylic acid and aliphatic hydroxyoxime. Hydrometallurgy 84:109–117

    Article  Google Scholar 

  51. du Preez AC, Preston JS (2004) Separation of nickel and cobalt from calcium, magnesium and manganese by solvent extraction with synergistic mixtures of carboxylic acids. J S Afr Inst Min Metall 104:333–338

    Google Scholar 

  52. Cheng CY, Zhang WS, Pranolo Y (2010) Separation of cobalt and zinc from manganese, magnesium, and calcium using a synergistic solvent extraction system consisting of Versatic 10 and LIX 63. Solvent Extr Ion Exch 28:608–624

    Article  Google Scholar 

  53. Kim DS, Sohn JS, Lee CK, Lee JH, Han KS, Lee YI (2004) Simultaneous separation and renovation of lithium cobalt oxide from the cathode of spent lithium ion rechargeable batteries. J Power Sources 132:145–149

    Article  Google Scholar 

  54. Yoshimura M, Han KS, Tsurimoto S (1998) Direct fabrication of thin-film LiNiO2 electrodes in LiOH solution by electrochemical-hydrothermal method. Solid State Ionics 106:39–44

    Article  Google Scholar 

  55. Han KS, Song SW, Fujita H, Yoshimura M (2000) Single-step fabrication of Li1−x Ni1+x O2 and LiCoO2 films by soft solution-processing at 20–200°C. Solid State Ionics 135:273–276

    Article  Google Scholar 

  56. Han KS, Tsurimoto S, Yoshimura M (1999) Fabrication temperature and applied current density effects on the direct fabrication of lithium nickel oxide thin-film electrodes in LiOH solution by the electrochemical-hydrothermal method. Solid State Ionics 121:229–233

    Article  Google Scholar 

  57. Song SW, Han KS, Sasagawa I, Watanabe T, Yoshimura M (2000) Effect of LiOH concentration change on simultaneous preparation of LiCoO2 film and powder by hydrothermal method. Solid State Ionics 135:277–281

    Article  Google Scholar 

  58. Watanabe T, Uono H, Song SW, Han KS, Yoshimura M (2001) Direct fabrication of lithium cobalt oxide films on various substrates in flowing aqueous solutions at 150°C. J Solid State Chem 162:364–370

    Article  Google Scholar 

  59. Han KS, Song SW, Tsurimoto S, Fujita H, Sasagawa I, Choi KH, Kang HK, Yoshimura M (2002) Soft solution processing for direct fabrication of LiMO2 (M=Ni and Co) film. Solid State Ionics 151:11–18

    Article  Google Scholar 

  60. U.S. Geological Survey (2011) Mineral commodity summaries 2011. U.S. Geological Survey, Reston, Virginia

  61. Rentz O, Engels B, Schultmann F (2001) Environmental research plan of the German Federal Ministry for the Environment, nature conservation and nuclear safety. Research Project 299 35 330. French-German Institute for Environmental Research, Universität Karlsruhe (TH)

  62. Bau-, Verkehrs- und Energiedirektion des Kantons Bern, GSA – Amt für Gewässerschutz und Abfallwirtschaft (Ed.) (2003) Altbatterien gehören nicht in den Kehrrichtsack, Abfallsplitter, Waste Information Canton Bern

  63. Pistoia G, Wiaux JP, Wolsky SP (2001) Used battery collection and recycling. Elsevier Science, Amsterdam

    Google Scholar 

  64. Henrion P (2004) ICBR—international congress for battery recycling, Como

  65. Henrion P (2008) EBR—electronics & battery recycling, Toronto

  66. Henrion P (2008) ICBR—international congress for battery recycling, Düsseldorf

  67. Tollinsky N (2008) Xstrata boosts recycling capacity. Sudbury Min Solut J 5:1–36

    Google Scholar 

  68. Chéret D (2004) ICBR—international congress for battery recycling, Como

  69. Chéret D (2006) ICBR—international congress for battery recycling, Interlaken

  70. Meskers CEM, Hagelüken C, Van Damme G (2009) Greeen recycling of EEE: special and precious metal recovery from EEE. In: Stanley M, Howard (eds) Proceedings of sessions and symposia sponsored by the extraction & processing division (EPD) of the minerals, metals & materials society (TMS), San Franscisco, California, pp 1131–1136

  71. Siret C (2008) ICBR—international congress for battery recycling, Düsseldorf

  72. Siret C, Van Damme G (2008) EBR—electronics & battery recycling, Toronto

Download references

Acknowledgments

This study was supported by the Chinese Academy of Sciences (No. 2011YDHZ-JSC02), Guangdong Province (No. 2011A032302001) and the China Postdoctoral Science Foundation (No. 2012M510553).

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Hongbin Cao.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Zhang, X., Xie, Y., Lin, X. et al. An overview on the processes and technologies for recycling cathodic active materials from spent lithium-ion batteries. J Mater Cycles Waste Manag 15, 420–430 (2013). https://doi.org/10.1007/s10163-013-0140-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10163-013-0140-y

Keywords

Navigation