Direct NCA Cathode Active Materials Recycling from Spent Li-Ion Batteries: Solvent-Free Recovery and Healing by Heat Treatment

Oubaha, Hamid; Fkhar, Lahcen; Cloots, Rudi; Boschini, Frédéric; Mahmoud, Abdelfattah

doi:10.1021/acssusresmgt.4c00133

Article (Scientific journals)

Direct NCA Cathode Active Materials Recycling from Spent Li-Ion Batteries: Solvent-Free Recovery and Healing by Heat Treatment

Oubaha, Hamid; Fkhar, Lahcen; Cloots, Rudi et al.

2024 • In ACS Sustainable Resource Management, 1 (8), p. 1791–1801

Peer reviewed

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https://hdl.handle.net/2268/321375

DOI
10.1021/acssusresmgt.4c00133

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Keywords :

Direct recycling; Cathode active materials; Lithium-ion batteries; Lithium nickel cobalt aluminum oxides; NCA; Regeneration

Abstract :

[en] The steadily growing lithium-ion batteries (LIBs) market brings the critical question of the future treatment of tremendous waste from end-of-life (EoL) LIBs. Therefore, recycling of EoL LIBs has become an urgent need to overcome the foreseen environmental and economic challenges. Herein, we propose a direct recycling process to regenerate NCA cathode active material (CAM) from spent LIBs. A gentle heat pretreatment at a low temperature is applied to facilitate the recovery of the CAMs. The cathode strips from EoL LIBs were subjected to two temperatures (150 or 250 °C) during a short time (2 h) to deactivate the strong bonding between the polyvinylidene difluoride binder and the Al current collector surface. Thus, the CAM is easily and fully reclaimed from the Al foil. Moreover, the developed procedure preserves the integrity of the NCA structure without any morphological changes. The full restoration of NCA-based CAM powder is successfully achieved through Li-replenishing using Li2CO3 under O2 atmosphere at different sintering temperatures (750 or 900 °C). The healed NCA CAMs demonstrate decent electrochemical performance including good cyclability and rate performance in NCA//Li half-cell and NCA//LTO full-cell configurations.

Disciplines :

Chemistry

Author, co-author :

Oubaha, Hamid ; Université de Liège - ULiège > Département de chimie (sciences) > GREEnMat

Fkhar, Lahcen ; Université de Liège - ULiège > Complex and Entangled Systems from Atoms to Materials (CESAM)

Cloots, Rudi ; Université de Liège - ULiège > Département de chimie (sciences) > GREEnMat

Boschini, Frédéric ; Université de Liège - ULiège > Département de chimie (sciences) > GREEnMat

Mahmoud, Abdelfattah ; Université de Liège - ULiège > Département de chimie (sciences) > GREEnMat

Language :

English

Title :

Direct NCA Cathode Active Materials Recycling from Spent Li-Ion Batteries: Solvent-Free Recovery and Healing by Heat Treatment

Publication date :

30 July 2024

Journal title :

ACS Sustainable Resource Management

ISSN :

2837-1445

eISSN :

2837-1445

Publisher :

American Chemical Society (ACS)

Volume :

Issue :

Pages :

1791–1801

Peer reviewed :

Peer reviewed

Additional URL :

https://pubs.acs.org/doi/pdf/10.1021/acssusresmgt.4c00133

Name of the research project :

CISTEMEEC project - PNRR convention n° 8677

Funders :

EU - European Union
Walloon region

Available on ORBi :

since 22 August 2024

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Bibliography

Manthiram, A. An Outlook on Lithium Ion Battery Technology. ACS Cent. Sci. 2017, 3 (10), 1063–1069, 10.1021/acscentsci.7b00288
Mrozik, W.; Rajaeifar, M. A.; Heidrich, O.; Christensen, P. Environmental impacts, pollution sources and pathways of spent lithium-ion batteries. Energy Environ. Sci. 2021, 14 (12), 6099–6121, 10.1039/D1EE00691F
Bird, R.; Baum, Z. J.; Yu, X.; Ma, J. The Regulatory Environment for Lithium-Ion Battery Recycling. ACS Energy Lett. 2022, 7 (2), 736–740, 10.1021/acsenergylett.1c02724
Xu, C.; Dai, Q.; Gaines, L.; Hu, M.; Tukker, A.; Steubing, B. Future material demand for automotive lithium-based batteries. Commun. Mater. 2020, 1 (1), 99, 10.1038/s43246-020-00095-x
Qi, L.; Wang, Y.; Kong, L.; Yi, M.; Song, J.; Hao, D.; Zhou, X.; Zhang, Z.; Yan, J. Manufacturing processes and recycling technology of automotive lithium-ion battery: A review. J. Energy Storage 2023, 67, 107533, 10.1016/j.est.2023.107533
Narins, T. P. The battery business: Lithium availability and the growth of the global electric car industry. Extr. Ind. Soc. 2017, 4 (2), 321–328, 10.1016/j.exis.2017.01.013
Maisel, F.; Neef, C.; Marscheider-Weidemann, F.; Nissen, N. F. A forecast on future raw material demand and recycling potential of lithium-ion batteries in electric vehicles. Resour., Conserv. Recycl. 2023, 192, 106920, 10.1016/j.resconrec.2023.106920
Schmuch, R.; Wagner, R.; Hörpel, G.; Placke, T.; Winter, M. Performance and cost of materials for lithium-based rechargeable automotive batteries. Nat. Energy 2018, 3 (4), 267–278, 10.1038/s41560-018-0107-2
Commission, E. European Critical Raw Materials Act; European Commission, 2023. https://commission.europa.eu/strategy-and-policy/priorities-2019-2024/european-green-deal/green-deal-industrial-plan/european-critical-raw-materials-act_en (accessed 02-17-2024).
Wang, Y.; Goikolea, E.; de Larramendi, I. R.; Lanceros-Méndez, S.; Zhang, Q. Recycling methods for different cathode chemistries - A critical review. J. Energy Storage 2022, 56, 106053, 10.1016/j.est.2022.106053
Neumann, J.; Petranikova, M.; Meeus, M.; Gamarra, J. D.; Younesi, R.; Winter, M.; Nowak, S. Recycling of Lithium-Ion Batteries─Current State of the Art, Circular Economy, and Next Generation Recycling. Adv. Energy Mater. 2022, 12 (17), 2102917, 10.1002/aenm.202102917
Ciez, R. E.; Whitacre, J. F. Examining different recycling processes for lithium-ion batteries. Nat. Sustainability 2019, 2 (2), 148–156, 10.1038/s41893-019-0222-5
Elmaataouy, E.; Kouchi, K.; El bendali, A.; Chari, A.; Alami, J.; Dahbi, M. Recycling of NCA cathode material from end–of–life LiBs via Glycerol–triacetate solvent–based separation. J. Power Sources 2023, 587, 233702, 10.1016/j.jpowsour.2023.233702
Brückner, L.; Frank, J.; Elwert, T. Industrial Recycling of Lithium-Ion Batteries─A Critical Review of Metallurgical Process Routes. Metals 2020, 10 (8), 1107, 10.3390/met10081107
Gaines, L.; Dai, Q.; Vaughey, J. T.; Gillard, S. Direct Recycling R&D at the ReCell Center. Recycling 2021, 6 (2), 31, 10.3390/recycling6020031
Meshram, P.; Pandey, B. D.; Mankhand, T. R. Extraction of lithium from primary and secondary sources by pre-treatment, leaching and separation: A comprehensive review. Hydrometallurgy 2014, 150, 192–208, 10.1016/j.hydromet.2014.10.012
Wang, J.; Ma, J.; Zhuang, Z.; Liang, Z.; Jia, K.; Ji, G.; Zhou, G.; Cheng, H.-M. Toward Direct Regeneration of Spent Lithium-Ion Batteries: A Next-Generation Recycling Method. Chem. Rev. 2024, 124 (5), 2839–2887, 10.1021/acs.chemrev.3c00884
Cao, Y.; Li, J.; Ji, H.; Wei, X.; Zhou, G.; Cheng, H.-M. A review of direct recycling methods for spent lithium-ion batteries. Energy Storage Mater. 2024, 70, 103475, 10.1016/j.ensm.2024.103475
Yu, X.; Li, W.; Gupta, V.; Gao, H.; Tran, D.; Sarwar, S.; Chen, Z. Current Challenges in Efficient Lithium-Ion Batteries’ Recycling: A Perspective. Global Challenges 2022, 6 (12), 2200099, 10.1002/gch2.202200099
Wang, X.-T.; Gu, Z.-Y.; Ang, E. H.; Zhao, X.-X.; Wu, X.-L.; Liu, Y. Prospects for managing end-of-life lithium-ion batteries: Present and future. Interdiscip. Mater. 2022, 1 (3), 417–433, 10.1002/idm2.12041
Harper, G.; Sommerville, R.; Kendrick, E.; Driscoll, L.; Slater, P.; Stolkin, R.; Walton, A.; Christensen, P.; Heidrich, O.; Lambert, S. et al. Recycling lithium-ion batteries from electric vehicles. Nature 2019, 575 (7781), 75–86, 10.1038/s41586-019-1682-5
Du, M.; Du, K.-D.; Guo, J.-Z.; Liu, Y.; Aravindan, V.; Yang, J.-L.; Zhang, K.-Y.; Gu, Z.-Y.; Wang, X.-T.; Wu, X.-L. Direct reuse of oxide scrap from retired lithium-ion batteries: advanced cathode materials for sodium-ion batteries. Rare Met. 2023, 42 (5), 1603–1613, 10.1007/s12598-022-02230-8
Wang, H.; Burke, S.; Yuan, R.; Whitacre, J. F. Effective direct recycling of inhomogeneously aged Li-ion battery cathode active materials. J. Energy Storage 2023, 60, 106616, 10.1016/j.est.2023.106616
Lan, Y.; Li, X.; Zhou, G.; Yao, W.; Cheng, H.-M.; Tang, Y. Direct Regenerating Cathode Materials from Spent Lithium-Ion Batteries. Adv. Sci. 2024, 11 (1), 2304425, 10.1002/advs.202304425
Sabisch, J. E. C.; Anapolsky, A.; Liu, G.; Minor, A. M. Evaluation of using pre-lithiated graphite from recycled Li-ion batteries for new LiB anodes. Resour., Conserv. Recycl. 2018, 129, 129–134, 10.1016/j.resconrec.2017.10.029
Abdollahifar, M.; Doose, S.; Cavers, H.; Kwade, A. Graphite Recycling from End-of-Life Lithium-Ion Batteries: Processes and Applications. Adv. Mater. Technol. 2023, 8 (2), 2200368, 10.1002/admt.202200368
Zhong, X.; Han, J.; Chen, L.; Liu, W.; Jiao, F.; Zhu, H.; Qin, W. Binding mechanisms of PVDF in lithium ion batteries. Appl. Surf. Sci. 2021, 553, 149564, 10.1016/j.apsusc.2021.149564
Fan, E.; Li, L.; Wang, Z.; Lin, J.; Huang, Y.; Yao, Y.; Chen, R.; Wu, F. Sustainable Recycling Technology for Li-Ion Batteries and Beyond: Challenges and Future Prospects. Chem. Rev. 2020, 120 (14), 7020–7063, 10.1021/acs.chemrev.9b00535
Natarajan, S.; Aravindan, V. Recycling Strategies for Spent Li-Ion Battery Mixed Cathodes. ACS Energy Lett. 2018, 3 (9), 2101–2103, 10.1021/acsenergylett.8b01233
Sloop, S.; Crandon, L.; Allen, M.; Koetje, K.; Reed, L.; Gaines, L.; Sirisaksoontorn, W.; Lerner, M. A direct recycling case study from a lithium-ion battery recall. Sustainable Mater. Technol. 2020, 25, e00152 10.1016/j.susmat.2020.e00152
Bai, Y.; Essehli, R.; Jafta, C. J.; Livingston, K. M.; Belharouak, I. Recovery of Cathode Materials and Aluminum Foil Using a Green Solvent. ACS Sustainable Chem. Eng. 2021, 9 (17), 6048–6055, 10.1021/acssuschemeng.1c01293
Windisch-Kern, S.; Holzer, A.; Wiszniewski, L.; Raupenstrauch, H. Investigation of Potential Recovery Rates of Nickel, Manganese, Cobalt, and Particularly Lithium from NMC-Type Cathode Materials (LiNixMnyCozO2) by Carbo-Thermal Reduction in an Inductively Heated Carbon Bed Reactor. Metals 2021, 11 (11), 1844, 10.3390/met11111844
Wang, T.; Luo, H.; Bai, Y.; Li, J.; Belharouak, I.; Dai, S. Direct Recycling of Spent NCM Cathodes through Ionothermal Lithiation. Adv. Energy Mater. 2020, 10 (30), 2001204, 10.1002/aenm.202001204
Qin, Z.; Li, J.; Zhang, T.; Wen, Z.; Zheng, Z.; Zhang, Y.; Zhang, N.; Jia, C.; Liu, X.; Chen, G. Effective separation of LiNi0.5Co0.2Mn0.3O2cathode material and Al foil via digestion of PVDF enabling a closed-loop recycle. J. Mater. Chem. A 2022, 10 (44), 23905–23914, 10.1039/D2TA06959H
Jiang, G.; Zhang, Y.; Meng, Q.; Zhang, Y.; Dong, P.; Zhang, M.; Yang, X. Direct Regeneration of LiNi0.5Co0.2Mn0.3O2Cathode from Spent Lithium-Ion Batteries by the Molten Salts Method. ACS Sustainable Chem. Eng. 2020, 8 (49), 18138–18147, 10.1021/acssuschemeng.0c06514
Du, M.; Guo, J.-Z.; Zheng, S.-H.; Liu, Y.; Yang, J.-L.; Zhang, K.-Y.; Gu, Z.-Y.; Wang, X.-T.; Wu, X.-L. Direct reuse of LiFePO4cathode materials from spent lithium-ion batteries: Extracting Li from brine. Chin. Chem. Lett. 2023, 34 (6), 107706, 10.1016/j.cclet.2022.07.049
Peng, D.; Wang, X.; Wang, S.; Zhang, B.; Lu, X.; Hu, W.; Zou, J.; Li, P.; Wen, Y.; Zhang, J. Efficient regeneration of retired LiFePO4cathode by combining spontaneous and electrically driven processes. Green Chem. 2022, 24 (11), 4544–4556, 10.1039/D2GC01007K
Song, X.; Hu, T.; Liang, C.; Long, H. L.; Zhou, L.; Song, W.; You, L.; Wu, Z. S.; Liu, J. W. Direct regeneration of cathode materials from spent lithium iron phosphate batteries using a solid phase sintering method. RSC Adv. 2017, 7 (8), 4783–4790, 10.1039/C6RA27210J
Ouaneche, T.; Courty, M.; Stievano, L.; Monconduit, L.; Guéry, C.; Sougrati, M. T.; Recham, N. Room temperature efficient regeneration of spent LiFePO4by direct chemical lithiation. J. Power Sources 2023, 579, 233248, 10.1016/j.jpowsour.2023.233248
Zhao, X.-X.; Wang, X.-T.; Guo, J.-Z.; Gu, Z.-Y.; Cao, J.-M.; Yang, J.-L.; Lu, F.-Q.; Zhang, J.-P.; Wu, X.-L. Dynamic Li+Capture through Ligand-Chain Interaction for the Regeneration of Depleted LiFePO4Cathode. Adv. Mater. 2024, 36 (14), 2308927, 10.1002/adma.202308927
Qin, Z.; Zhang, Y.; Luo, W.; Zhang, T.; Wang, T.; Ni, L.; Wang, H.; Zhang, N.; Liu, X.; Zhou, J. et al. A Universal Molten Salt Method for Direct Upcycling of Spent Ni-rich Cathode towards Single-crystalline Li-rich Cathode. Angew. Chem. Int. Ed. 2023, 62 (25), e202218672 10.1002/anie.202218672
Vadivel, S.; Phattharasupakun, N.; Wutthiprom, J.; duangdangchote, S.; Sawangphruk, M. High-Performance Li-Ion Batteries Using Nickel-Rich Lithium Nickel Cobalt Aluminium Oxide-Nanocarbon Core-Shell Cathode: In Operando X-ray Diffraction. ACS Appl. Mater. Interfaces 2019, 11 (34), 30719–30727, 10.1021/acsami.9b06553
Yeh, N.-H.; Wang, F.-M.; Khotimah, C.; Wang, X.-C.; Lin, Y.-W.; Chang, S.-C.; Hsu, C.-C.; Chang, Y.-J.; Tiong, L.; Liu, C.-H. et al. Controlling Ni2+from the Surface to the Bulk by a New Cathode Electrolyte Interphase Formation on a Ni-Rich Layered Cathode in High-Safe and High-Energy-Density Lithium-Ion Batteries. ACS Appl. Mater. Interfaces 2021, 13 (6), 7355–7369, 10.1021/acsami.0c22295
Sungjemmenla, V. S. K.; Soni, C. B.; Kumar, V.; Seh, Z. W. Understanding the Cathode-Electrolyte Interphase in Lithium-Ion Batteries. Energy Technology 2022, 10 (9), 2200421, 10.1002/ente.202200421
Guilmard, M.; Croguennec, L.; Denux, D.; Delmas, C. Thermal Stability of Lithium Nickel Oxide Derivatives. Part I: LixNi1.02O2and LixNi0.89Al0.16O2(x = 0.50 and 0.30). Chem. Mater. 2003, 15 (23), 4476–4483, 10.1021/cm030059f
Kim, T.; Ono, L. K.; Qi, Y. Understanding the active formation of a cathode-electrolyte interphase (CEI) layer with energy level band bending for lithium-ion batteries. J. Mater. Chem. A 2022, 11 (1), 221–231, 10.1039/D2TA07565B
Ross, B. J.; LeResche, M.; Liu, D.; Durham, J. L.; Dahl, E. U.; Lipson, A. L. Mitigating the Impact of Thermal Binder Removal for Direct Li-Ion Battery Recycling. ACS Sustainable Chem. Eng. 2020, 8 (33), 12511–12515, 10.1021/acssuschemeng.0c03424
Stenzel, Y. P.; Börner, M.; Preibisch, Y.; Winter, M.; Nowak, S. Thermal profiling of lithium ion battery electrodes at different states of charge and aging conditions. J. Power Sources 2019, 433, 226709, 10.1016/j.jpowsour.2019.226709
Le, A. V.; Wang, M.; Noelle, D. J.; Shi, Y.; Shirley Meng, Y.; Wu, D.; Fan, J.; Qiao, Y. Using high-HFP-content cathode binder for mitigation of heat generation of lithium-ion battery. Int. J. Energy Res. 2017, 41 (14), 2430–2438, 10.1002/er.3824
Leng, J.; Wang, J.; Peng, W.; Tang, Z.; Xu, S.; Liu, Y.; Wang, J. Highly-Dispersed Submicrometer Single-Crystal Nickel-Rich Layered Cathode: Spray Synthesis and Accelerated Lithium-Ion Transport. Small 2021, 17 (14), 2006869, 10.1002/smll.202006869
Ji, H.; Wang, J.; Ma, J.; Cheng, H.-M.; Zhou, G. Fundamentals, status and challenges of direct recycling technologies for lithium ion batteries. Chem. Soc. Rev. 2023, 52 (23), 8194–8244, 10.1039/D3CS00254C
Sim, S.-J.; Lee, S.-H.; Jin, B.-S.; Kim, H.-S. Use of carbon coating on LiNi0.8Co0.1Mn0.1O2cathode material for enhanced performances of lithium-ion batteries. Sci. Rep. 2020, 10 (1), 11114, 10.1038/s41598-020-67818-5
Zhong, S.; Lai, M.; Yao, W.; Li, Z. Synthesis and electrochemical properties of LiNi0.8CoxMn0.2-xO2positive-electrode material for lithium-ion batteries. Electrochim. Acta 2016, 212, 343–351, 10.1016/j.electacta.2016.07.040
Huang, B.; Li, X.; Wang, Z.; Guo, H.; Shen, L.; Wang, J. A comprehensive study on electrochemical performance of Mn-surface-modified LiNi0.8Co0.15Al0.05O2synthesized by an in situ oxidizing-coating method. J. Power Sources 2014, 252, 200–207, 10.1016/j.jpowsour.2013.11.092
Hestenes, J. C.; Marbella, L. E. Beyond Composition: Surface Reactivity and Structural Arrangement of the Cathode-Electrolyte Interphase. ACS Energy Lett. 2023, 8 (11), 4572–4596, 10.1021/acsenergylett.3c01529
Gauthier, M.; Carney, T. J.; Grimaud, A.; Giordano, L.; Pour, N.; Chang, H.-H.; Fenning, D. P.; Lux, S. F.; Paschos, O.; Bauer, C. et al. Electrode-Electrolyte Interface in Li-Ion Batteries: Current Understanding and New Insights. J. Phys. Chem. Lett. 2015, 6 (22), 4653–4672, 10.1021/acs.jpclett.5b01727