Electrochemical properties of nickel manganese cobalt oxide cathode material obtained during battery recycling
Original scientific paper
DOI:
https://doi.org/10.5599/jese.3330Keywords:
Spent batteries, battery cathode recovery, ternary layered oxides, oxalic acid leaching, electrochemical testsAbstract
Recycling spent batteries, particularly lithium-ion batteries, is becoming a global priority. Among the various recycling approaches, hydrometallurgy is one of the most useful methods. Among the many chemical compositions of cathode materials, ternary layered oxides warrant particular attention in recycling technology, making them more suitable candidates than other cathode materials. During hydrometallurgical leaching, various carboxylic acids are employed as solvents; however, oxalic acid deserves special consideration due to its high selectivity for lithium extraction. Nickel, cobalt, and manganese oxalates are practically insoluble in water and exist as the corresponding crystal hydrates. When a solution of transition metal sulphates, derived from cathode powder, is treated with a mixture of oxalic acid, the lithium remains in solution as a mixture of lithium sulphate and oxalate, while the transition metals are converted into their corresponding oxalates. In this process, a significant increase in the mass of the precipitate is observed, corresponding to the formation of oxalates. Thus, oxalic acid enables selective extraction of lithium from the “black mass” of lithium-ion batteries based on layered transition metal oxides. Moreover, the resulting mixture of transition metal oxalates, after minor compositional adjustments, can be directly reused for the resynthesis of ternary layered oxides. This paper presents methods for the hydrometallurgical processing of NCM523 (lithium nickel-cobalt-manganese oxide with a 5:2:3 molar ratio of Ni:Co:Mn) cathode material and its subsequent re-synthesis using transition metal and lithium oxalates. The physicochemical characteristics and electrochemical properties of the regenerated NCM523 electrodes are evaluated from the perspective of their potential reuse in rechargeable power sources.
Downloads
References
[1] Y. Jin, X. Qu, L. Ju, Z. Zhou, W. Sun, L. Song, M. Zhang, Sustainable regeneration of a spent layered lithium nickel cobalt manganese oxide cathode from a scrapped lithium-ion battery, Journal of Materials Chemistry A 12 (2024) 32613-32637. https://doi.org/10.1039/D4TA05089D DOI: https://doi.org/10.1039/D4TA05089D
[2] J. Quan, S. Zhao, D. Song, T. Wang, W. He, G. Li, Comparative life cycle assessment of LFP and NCM batteries including the secondary use and different recycling technologies, Science of the Total Environment 819 (2022) 153105. https://doi.org/10.1016/j.scitotenv.2022.153105 DOI: https://doi.org/10.1016/j.scitotenv.2022.153105
[3] S. Natarajan, V. Aravindan, Recycling strategies for spent Li-ion battery mixed cathodes, ACS Energy Letters 3 (2018) 2101-2103. https://doi.org/10.1021/acsenergylett.8b01233 DOI: https://doi.org/10.1021/acsenergylett.8b01233
[4] M. Buchert, W. Jenseit, C. Merz, D. Schüler, Verbundprojekt: Entwicklung eines realisierbaren Recyclingkonzepts für die Hochleistungsbatterien zukünftiger Elektrofahrzeuge - LiBRi: Teilprojekt: LCA der Recyclingverfahren, Oeko-Institut, Darmstadt, Germany, 2011. https://www.oeko.de/oekodoc/1499/2011-068-de.pdf (in German)
[5] J. Li, J. Fleetwood, W. B. Hawley, W. Kays, From materials to cell: State-of-the-art and prospective technologies for lithium-ion battery electrode processing, Chemical Reviews 122 (2022) 903-956. https://doi.org/10.1021/acs.chemrev.1c00565 DOI: https://doi.org/10.1021/acs.chemrev.1c00565
[6] R. Tao, Y. Gu, Z. Du, X. Lyu, J. Li. Advanced electrode processing for lithium-ion battery manufacturing, Nature Reviews Clean Technology 1 (2025) 116-131. https://doi.org/10.1038/s44359-024-00018-w DOI: https://doi.org/10.1038/s44359-024-00018-w
[7] N. Hayagan, I. Gaalich, P. Loubet, L. Croguennec, C. Aymonier, G. Philippot, J. Olchowka, Chal¬len¬ges and perspectives for direct recycling of electrode scraps and end-of-life lithium-ion batteries, Batteries and Supercaps 7 (2024) e202400120. https://doi.org/10.1002/batt.202400120 DOI: https://doi.org/10.1002/batt.202400120
[8] H. Ji, J. Wang, J. Ma, H. M. Cheng, G. Zhou, Fundamentals, status and challenges of direct recycling technologies for lithium ion batteries, Chemical Society Reviews 52 (2023) 8194-8244. https://doi.org/10.1039/D3CS00254C DOI: https://doi.org/10.1039/D3CS00254C
[9] S. O. Oriekhov, O. V. Potapenko, V. A. Sirosh. Extraction of elements from the cathode mass of a lithium-nickel-cobalt-manganese oxide-based battery. Ukrainian Conference with Inter-national Participation “Chemistry, physics and technology of surface” dedicated to the 95-th birthday of Academician Oleksii Chuiko, Kyiv, Ukraine, 2025, p. 169. ISBN 978-617-95367-2-4
[10] B. Halyuk, A. Mishuk, R. Derkach, V. Barsukov. Recycling of spent lithium-ion battery cathodes using electrolysis. Promising Materials and Processes in Applied Electrochemistry, Kyiv, Ukraine, 2024, p. 47-52. ISBN 978-617-7763-42-9
[11] A. Zanoletti, A. Mannu, A. Cornelio, Solvometallurgy as alternative to pyro- and hydrometallurgy for lithium, cobalt, nickel, and manganese extraction from black mass processing: State of the art, Materials 18 (2025) 2761. https://doi.org/10.3390/ma18122761 DOI: https://doi.org/10.3390/ma18122761
[12] A. B. Shrestha, A. S. Amarasekara, The sustainable and green management of spent lithium-ion batteries through hydroxy acid Recycling and direct regeneration of active positive electrode material: A Review, Batteries 11 (2025) 68-90. https://doi.org/10.3390/batteries11020068 DOI: https://doi.org/10.3390/batteries11020068
[13] O. V. Potapenko, O. I. V’yunov, H. V. Potapenko, K. I. Vavilon, O. A. Vyshnevskyi, V. A. Sirosh, V. O. Oliinyk, Efficient Hydrometallurgical Recycling of Lithium iron-phosphate batteries using the acetic acid, Chemistry, Physics and Technology of Surface 16 (2025) 463-473. https://doi.org/10.15407/hftp16.04.463 DOI: https://doi.org/10.15407/hftp16.04.463
[14] Z. J. Baum, R. E. Bird, X. Yu, J. Ma, Lithium-Ion Battery Recycling Overview of Techniques and Trends, ACS Energy Letters 7 (2022) 712-719. https://doi.org/10.1021/acsenergylett.1c02602 DOI: https://doi.org/10.1021/acsenergylett.1c02602
[15] F. Larouche, F. Tedjar, K. Amouzegar, G. Houlachi, P. Bouchard et al. Progress and Status of Hydrometallurgical and Direct Recycling of Li-Ion Batteries and Beyond. Materials 13 (2020) 801. https://doi.org/10.3390/ma13030801 DOI: https://doi.org/10.3390/ma13030801
[16] Q. Guo, J. Huang, Z. Liang, H. Potapenko, M. Zhou, X. Tang, S. Zhong, The use of a single-crystal nickel-rich layered NCM cathode for excellent cycle performance of lithium-ion batteries. New Journal of Chemistry 45 (2021) 3652-3659. https://doi.org/10.1039/D0NJ05914E DOI: https://doi.org/10.1039/D0NJ05914E
[17] J. Wang, J. Li, S. Li, W. Du, Y. Xu, K. Wang, An oxide precursor route for manufacturing nickel-rich NCM cathode materials through the flame synthesis approach, Progress in Natural Science: Materials International 35 (2025) 485-491. https://doi.org/10.1016/j.pnsc.2025.04.001 DOI: https://doi.org/10.1016/j.pnsc.2025.04.001
[18] X. Xu, H. Huo, J. Jian, L. Wang, H. Zhu, S. Xu, X. He, G. Yin, C. Du, X. Sun, Radially oriented single-crystal primary nanosheets enable ultrahigh rate and cycling properties of LiNi0.8Co0.1Mn0.1O2 cathode material for lithium-ion batteries, Advanced Energy Materials 9 (2019) 1803963. https://doi.org/10.1002/aenm.201803963 DOI: https://doi.org/10.1002/aenm.201803963
[19] A. K. Nikumbh, A. E. Athare, V. B. Raut, А study of the thermal decomposition of cobalt (II) and nickel (II) oxalate dihydrate using direct current electrical conductivity measurements, Thermochimica Acta 186 (1991) 217-233. https://doi.org/10.1016/0040-6031(91)87038-X DOI: https://doi.org/10.1016/0040-6031(91)87038-X
[20] F. Wu, J. Tian, Y. Su, J. Wang, C. Zhang, L. Bao, T. He, J. Li, S. Chen, Effect of Ni2+ content on lithium/nickel disorder for Ni-Rich cathode materials, ACS Applied Materials & Interfaces 7 (2015) 7702-7708. https://doi.org/10.1021/acsami.5b00645 DOI: https://doi.org/10.1021/acsami.5b00645
[21] S. Bhanuchandar, G. Vinothkumar, P. Arunkumar, M. Sribalaji, A. K. Keshri, K. S. Babu,. Unravelling the role of cationic Ni2+ vacancies and Ni3+ ions in non-stoichiometric NiO: breakdown of anti-ferromagnetic ordering and large exchange bias, Journal of Materials Science 58 (2023) 13136-13153. https://doi.org/10.1007/s10853-023-08853-1 DOI: https://doi.org/10.1007/s10853-023-08853-1
[22] Z. Fu, J. Hu, W. Hu, S. Yang, Y. Luo, Quantitative analysis of Ni2+/Ni3+ in Li[NixMnyCoz]O2 cathode materials: Non-linear least-squares fitting of XPS spectra, Applied Surface Science 441 (2018) 1048-1056. https://doi.org/10.1016/j.apsusc.2018.02.114 DOI: https://doi.org/10.1016/j.apsusc.2018.02.114
[23] S. O. Ajayi, C. O. Ehi-Eromosele, X. Liu, M. K. Mathe, Improving cycling performance and high rate capability of LiNi0.5Mn0.3Co0.2O2 cathode materials by sol-gel combustion synthesis, Journal of Physics and Chemistry of Solids 196 (2025) 112352. https://doi.org/10.1016/j.jpcs.2024.112352 DOI: https://doi.org/10.1016/j.jpcs.2024.112352
[24] J. Xu, J. Yang, S. Wang, J. Jiang, Q. Zhuang, X. Qiu, K. Wu, H. Zheng, Ion transport and electrochemical reaction in LiNi0.5Co0.2Mn0.3O2-based high energy/power lithium-ion batteries, Nanomaterials 13 (2023) 856-870. https://doi.org/10.3390/nano13050856 DOI: https://doi.org/10.3390/nano13050856
[25] E. D. Orlova, A. A. Savina, S. A. Abakumov, A. V. Morozov, A. M. Abakumov, Comprehensive study of Li+/Ni2+ disorder in Ni-rich NMCs cathodes for Li-ion batteries, Symmetry 13 (2021) 1628-1642. https://doi.org/10.3390/sym13091628 DOI: https://doi.org/10.3390/sym13091628
[26] J. Li, G. Liang, W. Z. Zhang, S. Zhang, K. Davey, W. K. Pang, Z. Guo, Addressing cation mixing in layered structured cathodes for lithium-ion batteries: A critical review, Nano Materials Science 5 (2023) 404-420. https://doi.org/10.1016/j.nanoms.2022.09.001 DOI: https://doi.org/10.1016/j.nanoms.2022.09.001
[27] X. Li, B. Su, W. Xue, J. Zhang, Synthesis and electrochemical characterization of LiNi0.5Co0.2Mn0.3O2 cathode material by solid-phase reaction, Materials 15 (2022) 3931-3940. https://doi.org/10.3390/ma15113931 DOI: https://doi.org/10.3390/ma15113931
[28] J. Zheng, Y. Ye, T. Liu, Y. Xiao, C. Wang, F. Wang, F. Pan. Ni/Li disordering in layered transition metal oxide: Electrochemical impact, origin, and control, Accounts of Chemical Research 52 (2019) 2201-2209. https://doi.org/10.1021/acs.accounts.9b00033 DOI: https://doi.org/10.1021/acs.accounts.9b00033
Downloads
Published
Issue
Section
License
Copyright (c) 2026 Hanna Potapenko, Oleksandr Potapenko, Vitalii Sirosh, Zhou Chang Ji, Hui Zhou , Borys Haliuk, Chee Sien Wong, Viacheslav Barsukov

This work is licensed under a Creative Commons Attribution 4.0 International License.
How to Cite
Funding data
-
National Academy of Sciences of Ukraine
Grant numbers 0123U101087



