journal article·2025-09-14Open access

Sustainable Recovery of Critical Metals from Spent Lithium-Ion Batteries Using Deep Eutectic Solvents

Jafar Goudarzi, Zhi Chen, Gaixia Zhang, Jinguang Hu, Karim Zaghib, Sixu Deng, Afzal Ahmed Dar, Xiaolei Wang, Fariborz Haghighat, Catherine N. Mulligan, Chunjiang An, Antonio Avalos Ramirez

Batteries· Volume 11· Issue 9

Abstract

The surging demand for lithium-ion batteries (LIBs) has intensified the need for sustainable recovery of critical metals such as lithium, manganese, cobalt, and nickel from spent cathodes. While conventional hydrometallurgical and pyrometallurgical methods are widely used, they involve high energy consumption, hazardous waste generation, and complex processing steps, underscoring the urgency of developing eco-friendly alternatives. This study presents a novel, water-enhanced deep eutectic solvent (DES) system composed of choline chloride and D-glucose for the efficient leaching of valuable metals from spent LiMn-based battery cathodes. The DES was synthesized under mild conditions and applied to dissolve cathode powder, with leaching performance optimized by varying temperature and duration. Under optimal conditions (100 °C, 24 h), exceptional recovery efficiencies were achieved: 98.9% for lithium, 98.4% for manganese, and 71.7% for nickel. Material characterization using X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), differential scanning calorimetry (DSC), and inductively coupled plasma mass spectrometer (ICP-MS) confirm effective phase dissolution and metal release. Although this DES system requires relatively higher temperature and longer reaction time compared to traditional acid leaching, it offers clear advantages in terms of non-toxicity, biodegradability, and elimination of strong oxidizing agents. These results demonstrate the potential of water-enhanced choline chloride–glucose DES as a green alternative for future development in sustainable battery recycling, supporting circular economy objectives.
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Research context

OpenAlex topics: Extraction and Separation Processes · Advancements in Battery Materials · Ionic liquids properties and applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Building, Civil, and Environmental Engineering, Concordia University, 1455 de Maisonneuve Blvd. W., Montreal, QC H3G 1M8, Canada

Concordia Institute of Water, Energy and Sustainable Systems, Concordia University, Montreal, QC H3G 1M8, Canada

Department of Electrical Engineering, École de Technologie Supérieure (ÉTS), Montreal, QC H3C 1K3, Canada

Department of Chemical and Petroleum Engineering, University of Calgary, 2500 University Drive, NW, Calgary, AB T2N 1N4, Canada

Department of Chemical and Materials Engineering, Concordia University, 1455 de Maisonneuve Blvd. W., Montreal, QC H3G 1M8, Canada

Department of Chemical and Materials Engineering, University of Alberta, 12-241 Donadeo Innovation Centre for Engineering, 9211-116 Street NW, Edmonton, AB T6G 1H9, Canada

Centre National en Électrochimie et en Technologies Environnementales, 2263 Av. du Collège, Shawinigan, QC G9N 6V8, Canada

Funding

Concordia University

References (62)

Show source-provided references
1. Deep eutectic solvents for cathode recycling of Li-ion batteries10.1038/s41560-019-0368-4 ↗
2. Recycle, Recover and Repurpose Strategy of Spent Li-ion Batteries and Catalysts: Current Status and Future Opportunities10.1002/cssc.201903213 ↗
3. Progress, challenges, and prospects of spent lithium-ion batteries recycling: A review10.1016/j.jechem.2023.10.012 ↗
4. Non–closed–loop recycling strategies for spent lithium–ion batteries: Current status and future prospects10.1016/j.ensm.2024.103288 ↗
5. A comprehensive review of emerging technologies for recycling spent lithium-ion batteries10.1016/j.scitotenv.2023.168543 ↗
6. End-of-life automotive lithium-ion batteries (LIBs) in Brazil: Prediction of flows and revenues by 203010.1016/j.resconrec.2021.105522 ↗
7. Recovery of metals from sulfate leach solutions of spent ternary lithium-ion batteries by precipitation with phosphate and solvent extraction with P50710.1016/j.hydromet.2022.105861 ↗
8. Pyrometallurgical options for recycling spent lithium-ion batteries: A comprehensive review10.1016/j.jpowsour.2021.229622 ↗
9. Sustainable recycling of spent ternary lithium-ion batteries via an environmentally friendly process: Selective recovery of lithium and non-hazardous upcycling of residue10.1016/j.cej.2024.148516 ↗
10. Rehman, S., Al-Greer, M., Burn, A.S., Short, M., and Cui, X. (2025). High-Volume Battery Recycling: Technical Review of Challenges and Future Directions. Batteries, 11.10.20944/preprints202501.1483.v1 ↗
11. Chemical Transformations in Li-Ion Battery Electrode Materials by Carbothermic Reduction10.1021/acssuschemeng.8b06540 ↗
12. Bioprocessing of spent lithium-ion batteries for critical metals recovery—A review10.1016/j.resconrec.2020.105225 ↗
13. Novel targetedly extracting lithium: An environmental-friendly controlled chlorinating technology and mechanism of spent lithium-ion batteries recovery10.1016/j.jhazmat.2020.123947 ↗
14. Development and challenges of deep eutectic solvents for cathode recycling of end-of-life lithium-ion batteries10.1016/j.cej.2023.142278 ↗
15. Issues and challenges facing rechargeable lithium batteries10.1038/35104644 ↗
16. The Li-Ion Rechargeable Battery: A Perspective10.1021/ja3091438 ↗
17. Solvometallurgical recycling of spent LiNixCoyMnzO2 (NCM) cathode material using ternary choline chloride-ethylene glycol-p-toluenesulfonic acid deep eutectic solvent10.1016/j.hydromet.2023.106184 ↗
18. Advanced cathode materials and efficient electrolytes for rechargeable batteries: Practical challenges and future perspectives10.1039/C9TA00581A ↗
19. Thermochemically driven layer structure collapse via sulfate roasting toward the selective extraction of lithium and cobalt from spent LiCoO2 batteries10.1016/j.jpowsour.2023.233094 ↗
20. Lithium-ion battery recycling: A source of per- and polyfluoroalkyl substances (PFAS) to the environment?10.1039/D2EM00511E ↗
21. Lithium-ion battery recycling processes: Research towards a sustainable course
22. Combined pyro-hydrometallurgical technology for recovering valuable metal elements from spent lithium-ion batteries: A review of recent developments10.1039/D3GC01077E ↗
23. Safety Concerns for the Management of End-of-Life Lithium-Ion Batteries
24. Recent progress in pyrometallurgy for the recovery of spent lithium-ion batteries: A review of state-of-the-art developments10.1016/j.cogsc.2024.100881 ↗
25. Pyrometallurgical recycling of different lithium-ion battery cell systems: Economic and technical analysis10.1016/j.jclepro.2023.137834 ↗
26. A Review on Environmental, Economic and Hydrometallurgical Processes of Recycling Spent Lithium-ion Batteries10.1080/08827508.2020.1781628 ↗
27. Ultra-low viscosity betaine hydrochloride-formic acid deep eutectic solvent for leaching critical metals from spent NCM lithium-ion batteries10.1016/j.jece.2024.112586 ↗
28. Sulfuric acid leaching of metals from waste Li-ion batteries without using reducing agent10.1016/j.mineng.2022.107597 ↗
29. Complete and selective recovery of lithium from EV lithium-ion batteries: Modeling and optimization using oxalic acid as a leaching agent10.1016/j.seppur.2023.124143 ↗
30. Recovery of Li, Ni, Co and Mn from spent lithium-ion batteries assisted by organic acids: Process optimization and leaching mechanism10.1007/s12613-023-2735-1 ↗
31. Fundamentals, status and challenges of direct recycling technologies for lithium-ion batteries10.1039/D3CS00254C ↗
32. Challenges in Recycling Spent Lithium-Ion Batteries: Spotlight on Polyvinylidene Fluoride Removal10.1002/gch2.202200237 ↗
33. Deep Eutectic Solvents formed between choline chloride and carboxylic acids: Versatile alternatives to ionic liquids10.1021/ja048266j ↗
34. Solvometallurgical recovery of cobalt from lithium-ion battery cathode materials using deep-eutectic solvents10.1039/D0GC00940G ↗
35. Status and advances of deep eutectic solvents for metal separation and recovery10.1039/D1GC03851F ↗
36. Solubility of metal oxides in deep eutectic solvents based on choline chloride10.1021/je060038c ↗
37. A Review of Processes and Technologies for the Recycling of Spent Lithium-ion Batteries10.1088/1757-899X/782/2/022025 ↗
38. The Le Chatelier’s principle enables closed loop regenerating ternary cathode materials for spent lithium-ion batteries10.1016/j.ensm.2024.103250 ↗
39. Acid-free extraction of valuable metal elements from spent lithium-ion batteries using waste copperas10.1016/j.wasman.2023.01.013 ↗
40. A novel method for screening deep eutectic solvent to recycle the cathode of Li-ion batteries10.1039/D0GC00701C ↗
41. The application of deep eutectic solvents in lithium-ion battery recycling: A comprehensive review10.1016/j.resconrec.2022.106690 ↗
42. A comprehensive review of the reclamation of resources from spent lithium-ion batteries10.1016/j.cej.2023.145822 ↗
43. Selective recovery of cobalt from mixed lithium-ion battery wastes using deep eutectic solvent10.1016/j.cej.2021.129249 ↗
44. Strategies for overcoming challenges in using deep eutectic solvents for the selective extraction of valuable metals from spent lithium-ion batteries: A review10.1016/j.jece.2024.113200 ↗
45. A study of the separation of cobalt from spent Li-ion battery residues10.1016/j.jpowsour.2007.04.025 ↗
46. Molecular dynamic (MD) simulation and density function theory (DFT) calculation relevant to green leaching of metals from spent lithium-ion battery cathode materials using glucose-based deep eutectic solvent (DES)10.1016/j.hydromet.2023.106223 ↗
47. Recovery of lithium and cobalt from spent lithium-ion batteries using organic acids: Process optimization and kinetic aspects10.1016/j.wasman.2017.03.037 ↗
48. Density, Viscosity, and Refractive Index of a Choline Chloride + d -(-)-Fructose Deep Eutectic Solvent + Water Mixture at Different Temperatures: An Experimental Study and Thermodynamic Modeling10.1021/acs.jced.2c00440 ↗
49. Deep Eutectic Solvents (DESs) and Their Applications10.1021/cr300162p ↗
50. Effect of water addition on choline chloride/glycol deep eutectic solvents: Characterization of their structural and physicochemical properties10.1016/j.molliq.2019.111301 ↗
51. Effect of water and hydrogen bond acceptor on the density and viscosity of glycol-based eutectic solvents10.1016/j.molliq.2023.122856 ↗
52. Effect of Water on a Hydrophobic Deep Eutectic Solvent10.1021/acs.jpcb.1c08170 ↗
53. Physico-chemical characterisation of glycerol- and ethylene glycol-based deep eutectic solvents10.1016/j.molliq.2023.123777 ↗
54. Insights on the water effect on deep eutectic solvents properties and structuring: The archetypical case of choline chloride + ethylene glycol10.1016/j.molliq.2021.117717 ↗
55. Modeling the Viscosity of ChCl-Based Deep Eutectic Solvents and Their Mixtures with Water10.1021/acs.iecr.3c03652 ↗
56. Deep eutectic solvents as an emerging green platform for the synthesis of functional materials10.1039/D3GC04289H ↗
57. Efficient and Selective Dissolution of Li from Lithium-Ion Battery LiFePO4 Cathode by Natural Deep Eutectic Solvents10.1021/acs.energyfuels.4c00080 ↗
58. Green recycling of spent Li-ion battery cathodes via deep-eutectic solvents10.1039/D3EE02978F ↗
59. Deep Eutectic Solvents: Green Approach for Cathode Recycling of Li-Ion Batteries10.1002/aesr.202100133 ↗
60. Neoteric deep eutectic solvents: History, recent developments, and catalytic applications10.1039/D1SM01797G ↗
61. Recent advances in pretreating technology for recycling valuable metals from spent lithium-ion batteries10.1016/j.jhazmat.2020.124332 ↗
62. Selective extraction of transition metals from spent LiNixCoγMn1−x−γO2 cathode via regulation of coordination environment10.1002/anie.202202558 ↗