Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

A contact-electro-catalytic cathode recycling method for spent lithium-ion batteries

Nature Energy volume 8, pages 1137–1144 (2023)Cite this article

Subjects

Abstract

With the global trend towards carbon neutrality, the demand for lithium-ion batteries (LIBs) is continuously increasing. However, current recycling methods for spent LIBs need urgent improvement in terms of eco-friendliness, cost and efficiency. Here we propose a mechano-catalytic method, dubbed contact-electro-catalysis, utilizing radicals generated by contact electrification to promote the metal leaching under the ultrasonic wave. We also use SiO2 as a recyclable catalyst in the process. For lithium cobalt (III) oxide batteries, the leaching efficiency reached 100% for lithium and 92.19% for cobalt at 90 °C within 6 hours. For ternary lithium batteries, the leaching efficiencies of lithium, nickel, manganese and cobalt reached 94.56%, 96.62%, 96.54% and 98.39% at 70 °C, respectively, within 6 hours. We anticipate that this method can provide a green, high efficiency and economic approach for LIB recycling, meeting the exponentially growing demand for LIB productions.

This is a preview of subscription content, access via your institution

Access options

Buy this article

  • Purchase on SpringerLink
  • Instant access to full article PDF
Buy now

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Flow chart of lithium battery recovery by CEC leaching.
Fig. 2: Metal extraction by CEC leaching.
Fig. 3: Investigations on the CEC-generated radicals for recycling.
Fig. 4: Characterization of precipitate from leaching solution after CEC treatment.
Fig. 5: Recyclability demonstration of SiO2 for CEC leaching.

Similar content being viewed by others

Data availability

The data supporting the findings of this study are available within the paper and its Supplementary Information files. Source data are provided with this paper.

References

  1. Lv, H. et al. Electric field driven de-lithiation: a strategy towards comprehensive and efficient recycling of electrode materials from spent lithium ion batteries. Applied Catal. B 283, 119634 (2021).

    Article  Google Scholar 

  2. Kang, D. H., Chen, M. & Ogunseitan, O. A. Potential environmental and human health impacts of rechargeable lithium batteries in electronic waste. Environ. Sci. Technol. 47, 5495–5503 (2013).

    Article  Google Scholar 

  3. Ciez, R. E. & Whitacre, J. F. Examining different recycling processes for lithium-ion batteries. Nat. Sustain. 2, 148–156 (2019).

    Article  Google Scholar 

  4. Global Supply Chains of EV Batteries (IEA, 2022); https://www.iea.org/reports/global-supply-chains-of-ev-batteries

  5. Chernyaev, A. et al. The efficiency of scrap Cu and Al current collector materials as reductants in LIB waste leaching. Hydrometallurgy 203, 105608 (2021).

    Article  Google Scholar 

  6. Wang, S., Zhang, Z., Lu, Z. & Xu, Z. A novel method for screening deep eutectic solvent to recycle the cathode of Li-ion batteries. Green Chem. 22, 4473–4482 (2020).

    Article  Google Scholar 

  7. Yang, Y. et al. Selective recovery of lithium from spent lithium iron phosphate batteries: a sustainable process. Green Chem. 20, 3121–3133 (2018).

    Article  Google Scholar 

  8. Zeng, A. et al. Battery technology and recycling alone will not save the electric mobility transition from future cobalt shortages. Nat. Commun. 13, 1341 (2022).

    Article  Google Scholar 

  9. Or, T., Gourley, S. W. D., Kaliyappan, K., Yu, A. & Chen, Z. Recycling of mixed cathode lithium‐ion batteries for electric vehicles: current status and future outlook. Carbon Energy 2, 6–43 (2020).

    Article  Google Scholar 

  10. Wang, Y. et al. Recent progress on the recycling technology of Li-ion batteries. J. Energy Chem. 55, 391–419 (2021).

    Article  Google Scholar 

  11. Raj, T. et al. Recycling of cathode material from spent lithium-ion batteries: challenges and future perspectives. J. Hazard. Mater. 429, 128312 (2022).

    Article  Google Scholar 

  12. Baum, Z. J., Bird, R. E., Yu, X. & Ma, J. Lithium-ion battery recycling─overview of techniques and trends. ACS Energy Lett. 7, 712–719 (2022).

    Article  Google Scholar 

  13. Garole, D. J. et al. Recycle, recover and repurpose strategy of spent Li-ion batteries and catalysts: current status and future opportunities. ChemSusChem 13, 3079–3100 (2020).

    Article  Google Scholar 

  14. Barik, S. P., Prabaharan, G. & Kumar, L. Leaching and separation of Co and Mn from electrode materials of spent lithium-ion batteries using hydrochloric acid: laboratory and pilot-scale study. J. Clean. Prod. 147, 37–43 (2017).

    Article  Google Scholar 

  15. Chen, X., Ma, H., Luo, C. & Zhou, T. Recovery of valuable metals from waste cathode materials of spent lithium-ion batteries using mild phosphoric acid. J. Hazard. Mater. 326, 77–86 (2017).

    Article  Google Scholar 

  16. Zhou, S. et al. Recycling of LiCoO2 cathode material from spent lithium ion batteries by ultrasonic enhanced leaching and one-step regeneration. J. Environ. Manage. 277, 111426 (2021).

    Article  Google Scholar 

  17. Bai, Y. et al. Energy and environmental aspects in recycling lithium-ion batteries: concept of battery identity global passport. Mater. Today 41, 304–315 (2020).

    Article  Google Scholar 

  18. Li, L. et al. Succinic acid-based leaching system: a sustainable process for recovery of valuable metals from spent Li-ion batteries. J. Power Sources 282, 544–551 (2015).

    Article  Google Scholar 

  19. Gao, W. et al. Comprehensive evaluation on effective leaching of critical metals from spent lithium-ion batteries. Waste Manage. 75, 477–485 (2018).

    Article  Google Scholar 

  20. Li, L. et al. Recovery of metals from spent lithium-ion batteries with organic acids as leaching reagents and environmental assessment. J. Power Sources 233, 180–189 (2013).

    Article  Google Scholar 

  21. Fan, E. et al. Sustainable recycling technology for Li-ion batteries and beyond: challenges and future prospects. Chem. Rev. 120, 7020–7063 (2020).

    Article  Google Scholar 

  22. Tran, M. K., Rodrigues, M.-T. F., Kato, K., Babu, G. & Ajayan, P. M. Deep eutectic solvents for cathode recycling of Li-ion batteries. Nat. Energy 4, 339–345 (2019).

    Article  Google Scholar 

  23. Wang, Z. et al. Contact-electro-catalysis for the degradation of organic pollutants using pristine dielectric powders. Nat. Commun. 13, 130 (2022).

    Article  Google Scholar 

  24. Chen, B. et al. Water-solid contact electrification causes hydrogen peroxide production from hydroxyl radical recombination in sprayed microdroplets. Proc. Natl Acad. Sci. USA 119, e2209056119 (2022).

    Article  Google Scholar 

  25. Lin, S., Xu, L., Chi Wang, A. & Wang, Z. L. Quantifying electron-transfer in liquid–solid contact electrification and the formation of electric double-layer. Nat. Commun. 11, 399 (2020).

    Article  Google Scholar 

  26. Sun, M., Lu, Q., Wang, Z. L. & Huang, B. Understanding contact electrification at liquid–solid interfaces from surface electronic structure. Nat. Commun. 12, 1752 (2021).

    Article  Google Scholar 

  27. Lin, M.-F. et al. Imaging the short-lived hydroxyl-hydronium pair in ionized liquid water. Science 374, 92–95 (2021).

    Article  Google Scholar 

  28. Wang, J. et al. Sonocatalytic damage of bovine serum albumin (BSA) under ultrasonic irradiation by mixed TiO2/SiO2 powder. J. Chem. Technol. Biotechnol. 84, 538–546 (2009).

    Article  Google Scholar 

  29. Deveci, I. & Mercimek, B. Performance of SiO2/Ag core/shell particles in sonocatalalytic degradation of rhodamine B. Ultrason. Sonochem. 51, 197–205 (2019).

    Article  Google Scholar 

  30. Zhan, F. et al. Electron transfer as a liquid droplet contacting a polymer surface. ACS Nano. 14, 17565–17573 (2020).

    Article  Google Scholar 

  31. Behera, S. S. & Parhi, P. K. Leaching kinetics study of neodymium from the scrap magnet using acetic acid. Sep. Purif. Technol. 160, 59–66 (2016).

    Article  Google Scholar 

  32. Hu, W. et al. Photocatalytic reduction of Cr(VI) using a wurtzite/natural sphalerite heterostructure: synergistic effects of exposed active facets, vacancies and a heterophase junction. Appl. Surf. Sci. 550, 149267 (2021).

    Article  Google Scholar 

  33. Liang, H. et al. 3-D hierarchical Ag/ZnO@CF for synergistically removing phenol and Cr(VI): heterogeneous vs homogeneous photocatalysis. J. Colloid Interface Sci. 558, 85–94 (2020).

    Article  Google Scholar 

  34. Nosaka, Y. & Nosaka, A. Y. Generation and detection of reactive oxygen species in photocatalysis. Chem. Rev. 117, 11302–11336 (2017).

    Article  Google Scholar 

  35. Xiao, R. et al. In situ fabrication of 1D CdS nanorod/2D Ti3C2 MXene nanosheet Schottky heterojunction toward enhanced photocatalytic hydrogen evolution. Appl. Catal. B 268, 118382 (2020).

    Article  Google Scholar 

  36. Xu, C. et al. Raising the working temperature of a triboelectric nanogenerator by quenching down electron thermionic emission in contact-electrification. Adv. Mater. 30, e1803968 (2018).

    Article  Google Scholar 

  37. Shen, F. et al. Influence of temperature difference on performance of solid–liquid triboelectric nanogenerators. Nano Energy 99, 107431 (2022).

    Article  Google Scholar 

  38. Huang, H. et al. Macroscopic polarization enhancement promoting photo- and piezoelectric-induced charge separation and molecular oxygen activation. Angew. Chem. Int. Ed. 56, 11860–11864 (2017).

    Article  Google Scholar 

  39. Geng, M. & Duan, Z. Prediction of oxygen solubility in pure water and brines up to high temperatures and pressures. Geochim. Cosmochim. Acta 74, 5631–5640 (2010).

    Article  Google Scholar 

  40. Rodrigues, C. et al. Emerging triboelectric nanogenerators for ocean wave energy harvesting: state of the art and future perspectives. Energy Environ. Sci. 13, 2657–2683 (2020).

    Article  Google Scholar 

  41. Lin, S., Chen, X. & Wang, Z. L. Contact electrification at the liquid–solid interface. Chem. Rev. 122, 5209–5232 (2022).

    Article  Google Scholar 

  42. Huang, Z. et al. Solution inheritance of CoC2O4·2H2O rods to nanoparticle-assembled Co3O4 rods. Colloids Surf. A 490, 307–317 (2016).

    Article  Google Scholar 

  43. Qiu, X. et al. Enabling the sustainable recycling of LiFePO4 from spent lithium-ion batteries. Green Chem. 24, 2506–2515 (2022).

    Article  Google Scholar 

  44. Cai, W., Chen, R., Yang, Y., Yi, M. & Xiang, L. Removal of SO42− from Li2CO3 by recrystallization in Na2CO3 solution. Crystals 8, 19 (2018).

    Article  Google Scholar 

  45. Chen, X., Kang, D., Li, J., Zhou, T. & Ma, H. Gradient and facile extraction of valuable metals from spent lithium ion batteries for new cathode materials re-fabrication. J. Hazard. Mater. 389, 121887 (2020).

    Article  Google Scholar 

  46. Wang, K. et al. Hexadecane-containing sandwich structure based triboelectric nanogenerator with remarkable performance enhancement. Nano Energy 87, 106198 (2021).

    Article  Google Scholar 

Download references

Acknowledgements

We appreciate C. Li, S. Shu and Y. Su for their assistance with collecting and organizing data. This research was supported by the National Key R&D Project from the Minister of Science and Technology (2021YFA1201601) and National Natural Science Foundation of China (grant number 52192610), Youth Innovation Promotion Association (W.T.) and CAS-TWAS President’s Fellowship (A.B.).

Author information

Authors and Affiliations

  1. CAS Center for Excellence in Nanoscience, Beijing Institute of Nanoenergy and Nanosystems, Chinese Academy of Sciences, Beijing, China

    Huifan Li, Andy Berbille, Xin Zhao, Ziming Wang, Wei Tang & Zhong Lin Wang

  2. Center on Nanoenergy Research, School of Physical Science and Technology, Guangxi University, Nanning, China

    Huifan Li

  3. School of Nanoscience and Technology, University of Chinese Academy of Sciences, Beijing, China

    Andy Berbille, Ziming Wang, Wei Tang & Zhong Lin Wang

  4. Yonsei Frontier Lab, Yonsei University, Seoul, Republic of Korea

    Zhong Lin Wang

Authors
  1. Huifan Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Andy Berbille
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Xin Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Ziming Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Wei Tang
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Zhong Lin Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

W.T. and Z.L.W. conceived the idea and supervised the experiment. H.L., A.B. and X.Z. performed the experiments, H.L. and W.T. analysed the data. Z.W. assisted in data measurements. H.L., A.B. and W.T. prepared the manuscript. Z.L.W. revised the manuscript.

Corresponding authors

Correspondence to Wei Tang or Zhong Lin Wang.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature Energy thanks Gavin Harper, Jia Li and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Figs. 1–8, Note 1 and Tables 1 and 2.

Supplementary Table 1

Statistical source data.

Supplementary Data

Statistical source data.

Supplementary Data

Statistical source data.

Supplementary Data

Statistical source data.

Supplementary Data

Statistical source data.

Supplementary Data

Statistical source data.

Supplementary Data

Statistical source data.

Supplementary Data

Statistical source d.ata

Source data

Source Data Fig. 2

Statistical source data.

Source Data Fig. 3

Statistical source data.

Source Data Fig. 4

Statistical source data.

Source Data Fig. 5

Statistical source data.

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Li, H., Berbille, A., Zhao, X. et al. A contact-electro-catalytic cathode recycling method for spent lithium-ion batteries. Nat Energy 8, 1137–1144 (2023). https://doi.org/10.1038/s41560-023-01348-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41560-023-01348-y

This article is cited by

Search

Advanced search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing