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Deep Eutectic Solvents (DESs) for Green Recycling of Wasted Lithium-Ion Batteries (LIBs): Progress on Pushing the Overall Efficiency

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Abstract

As one of the main power sources, lithium-ion batteries (LIBs) will continue to be applied on a large scale in the future market. Commercialized LIBs cathode materials contain various valuable metal elements including Li, Co, and Ni. The development of green and efficient recycling technology is essential. Deep eutectic solvents (DESs) have recently emerged as a new class of green solvents that could potentially be applied for the LIBs recycling industry due to their capability to leach the active materials without the introduction of environmentally hazardous reagents as used in conventional hydrometallurgy process. Considering the rapid progress, a critical review focusing on the progress and fundamentals about the overall efficiency has practical significance for the further advancement of this field. Herein, we briefly introduce the overall process of using DESs for LIBs recycling and specifically focus on the efficiency of each step. Current fundamental understandings and new experimental approaches to enhance the efficiency of the leaching process, the extraction process, and reusability are summarized. We expect this review article to inspire scientists to use DESs as powerful tools for advancing the frontiers of LIBs recycling.

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Fig. 1
Fig. 2

Copyright 2022, ACS Publications

Fig. 3
Fig. 4

Copyright 2006, ACS Publications. c Solubility of metal oxides in ptsa-ChCl type DES with different ratios. Reproduced with permission [93]. Copyright 2019, ACS Publications

Fig. 5

Copyright 2019, Nature Publishing Group. d Possible delamination mechanism based on competitive inhibition of binding via hydrogen bonding. Reproduced with permission [95]. Copyright 2020, ChemSusChem

Fig. 6

Copyright 2021, Green Chemistry. b The selection of DES with reductive property by calculating the atomic charges based on the Fukui function. Reproduced with permission [103]. Copyright 2020, Green Chemistry. c Evaluate the difficulty of capturing electrons based on IP calculation [104]. d The organic acid with a lower potential for its first oxidation was screened based on IP calculation. The DESs composed of ChCl as the HBA and various organic acid species as the HBD could be used to compare the leaching efficiency of NMC cathode material. Reproduced with permission [104]. Copyright 2021, Chemical Engineering Journal

Fig. 7

Copyright 2021, Journal of Kunming University of Science and Technology (Natural Science Edition). b The influence of the alcohol chain length for HBD on the viscosity. Reproduced with permission [119]. Copyright 2021, Elsevier. c The influence of the additional water content on the leaching process of Co and Li in ChCl-LAA DES. Reproduced with permission [104]. Copyright 2021, Chemical Engineering Journal. d GC–MS analysis of ChCl-EG DES heated at 180 °C for 24 h [121]. e Evolution of the XPS data for the metal oxide during the leaching process. The O1s spectra of the original electrode powder and the residual powder after leaching at 180 °C for 24 h show that the surface hydroxyl oxygen increases after leaching [121]. f UV–Vis spectrum shows the effect of N2 addition on the Co complexing ability [121]. g Comparison of the metal extraction yields of fresh and reused DESs. Reproduced with permission [121]. Copyright 2021, Chemical Engineering Journal

Fig. 8

Copyright 2020, Green Chemistry. g–i shows the SEM images of the Ni-Co nuclei obtained on the GCE surface using electrodeposition by applying a constant potential of − 0.78 V νs. Ag QRE, during 300 s at different magnifications: g: 2500 × ; h: 10,000 × ; i: 50,000 × . Reproduced with permission [128]. Copyright 2020, Journal of Alloys and Compounds

Fig. 9

Copyright 2022, Journal of Energy Chemistry. Comparison of the rate performances between b recycled and c commercial LNCO cathodes at different C rates. Reproduced with permission [50]. Copyright 2022, ChemSusChem

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Acknowledgements

This work was supported by the Natural Science Foundation of Guizhou Science and Technology Department (QKHJC-ZK[2021]-YB257) and the Talent program of Guizhou University (702759203301).

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Authors and Affiliations

  1. School of Materials and Metallurgy, Guizhou University, Guiyang, Guizhou, China

    Zhongjie Wang, Shuie Li, Taibai Li, Tao Hu & Xiang Ge

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  1. Zhongjie Wang
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  2. Shuie Li
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  3. Taibai Li
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  4. Tao Hu
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  5. Xiang Ge
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Correspondence to Shuie Li or Xiang Ge.

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Wang, Z., Li, S., Li, T. et al. Deep Eutectic Solvents (DESs) for Green Recycling of Wasted Lithium-Ion Batteries (LIBs): Progress on Pushing the Overall Efficiency. Mining, Metallurgy & Exploration 39, 2149–2165 (2022). https://doi.org/10.1007/s42461-022-00660-7

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