Synthesis of Ni-Rich Cathode from Li-Ion Battery Waste Using Environmentally Friendly Hydrometallurgy Process: Effect of Heat Treatment Atmosphere

Article Preview

Abstract:

This study investigated the recovery of nickel and other valuable metals from spent batteries, utilizing environmentally friendly hydrometallurgical techniques, i.e., organic acid leaching and oxalic acid co-precipitation, to recover the metal ions. The recovered metal ions in the form of oxalate precipitate served as a precursor for synthesizing nickel-rich cathodes, specifically nickel-cobalt-manganese (NCM) cathode with a composition of Ni:Co:Mn of 8:1:1. In this work, the effect of heat treatment atmosphere on the properties of the synthesized cathode materials was studied. The effect of heat treatment without and with oxygen flow was evaluated to determine its impact on the cathode’s structural integrity, electrochemical performance, and electrochemical stability. The results indicated that the choice of heat treatment atmosphere significantly influences the crystallinity, structure formation, particle morphology, and electrochemical properties of the cathode materials, e.g., specific capacity and cycling stability. The sample prepared by heat treating the precursors under oxygen flow demonstrated a higher initial specific discharge capacity of 181 mAh/g compared to that prepared without oxygen flow (87 mAh/g). This study demonstrated that synthesizing nickel-rich cathode materials from waste lithium-ion batteries can become a sustainable approach to ensure future battery production by reducing raw material demand and waste. Additionally, the findings on heat treatment atmosphere provided valuable insights for further study in optimizing the synthesis process of Ni-rich NCM cathode from waste battery cathode.

You might also be interested in these eBooks

Info:

Periodical:

Pages:

93-99

Citation:

Online since:

March 2025

Export:

Price:

Permissions CCC:

Permissions PLS:

Сopyright:

© 2025 Trans Tech Publications Ltd. All Rights Reserved

Share:

Citation:

* - Corresponding Author

[1] A. Manthiram, A reflection on lithium-ion battery cathode chemistry, Nature Communications 2020 11:1 11 (2020) 1–9.

DOI: 10.1038/s41467-020-15355-0

Google Scholar

[2] K.J. Park, H.G. Jung, L.Y. Kuo, P. Kaghazchi, C.S. Yoon, Y.K. Sun, Improved Cycling Stability of Li[Ni0.90Co0.05Mn0.05]O2 Through Microstructure Modification by Boron Doping for Li-Ion Batteries, Adv Energy Mater 8 (2018) 1801202.

DOI: 10.1002/aenm.201801202

Google Scholar

[3] J. Li, N. Zhang, H. Li, A. Liu, Y. Wang, S. Yin, H. Wu, J.R. Dahn, Impact of the Synthesis Conditions on the Performance of LiNixCoyAlzO2 with High Ni and Low Co Content, J Electrochem Soc 165 (2018) A3544–A3557.

DOI: 10.1149/2.0931814jes

Google Scholar

[4] P.N. Suryadi, J. Karunawan, O. Floweri, F. Iskandar, Toward high-rate capability of intercalation cathodes Li-ion batteries, potency for fast-charging application: A materials perspective, J Energy Storage 68 (2023) 107634.

DOI: 10.1016/j.est.2023.107634

Google Scholar

[5] Y. Hong Luo, H. Xin Wei, L. Bo Tang, Y. de Huang, Z. Yu Wang, Z. Jiang He, C. Yan, J. Mao, K. Dai, J. Chao Zheng, Nickel-rich and cobalt-free layered oxide cathode materials for lithium-ion batteries, Energy Storage Mater 50 (2022) 274–307.

DOI: 10.1016/j.ensm.2022.05.019

Google Scholar

[6] D. Castelvecchi, Electric cars and batteries: how will the world produce enough?, Nature 596 (2021) 336–339.

DOI: 10.1038/d41586-021-02222-1

Google Scholar

[7] M. Roshanfar, R. Golmohammadzadeh, F. Rashchi, An environmentally friendly method for recovery of lithium and cobalt from spent lithium-ion batteries using gluconic and lactic acids, J Environ Chem Eng 7 (2019) 102794.

DOI: 10.1016/j.jece.2018.11.039

Google Scholar

[8] S. Refly, O. Floweri, T.R. Mayangsari, A. Sumboja, S.P. Santosa, T. Ogi, F. Iskandar, Regeneration of LiNi1/3Co1/3Mn1/3O2 cathode active materials from end-of-life lithium-ion batteries through ascorbic acid leaching and oxalic acid co-precipitation processes, ACS Sustain Chem Eng 8 (2020).

DOI: 10.1021/acssuschemeng.0c01006.s001

Google Scholar

[9] A.L. Sidiq, O. Floweri, J. Karunawan, O.B. Abdillah, S.P. Santosa, F. Iskandar, NCM cathode active materials reproduced from end-of-life Li-ion batteries using a simple and green hydrometallurgical recycling process, Mater Res Bull 153 (2022).

DOI: 10.1016/j.materresbull.2022.111901

Google Scholar

[10] S. Refly, O. Floweri, T.R. Mayangsari, A.H. Aimon, F. Iskandar, Green recycle processing of cathode active material from LiNi1/3Co1/3Mn1/3O2 (NCM 111) battery waste through citric acid leaching and oxalate co-precipitation process, Mater Today Proc 44 (2020).

DOI: 10.1016/j.matpr.2020.11.664

Google Scholar

[11] D. Wang, I. Belharouak, G. Zhou, K. Amine, Synthesis of Lithium and Manganese-Rich Cathode Materials via an Oxalate Co-Precipitation Method, J Electrochem Soc 160 (2013) A3108–A3112.

DOI: 10.1149/2.016305jes

Google Scholar

[12] A.L. Sidiq, O. Floweri, A.H. Aimon, F. Iskandar, Transition metals recovery from organic acid leachate of spent lithium-ion battery cathode via oxalic acid co-precipitation, AIP Conf Proc 2652 (2022).

DOI: 10.1063/5.0106405

Google Scholar

[13] Y. Lei, J. Ai, S. Yang, H. Jiang, C. Lai, Q. Xu, Effect of flower-like Ni(OH)2 precursors on Li+/Ni2+ cation mixing and electrochemical performance of nickel-rich layered cathode, J Alloys Compd 797 (2019) 421–431.

DOI: 10.1016/j.jallcom.2019.05.065

Google Scholar

[14] L.P. He, S.Y. Sun, J.G. Yu, Performance of LiNi1/3Co1/3Mn1/3O2 prepared from spent lithium-ion batteries by a carbonate co-precipitation method, Ceram Int 44 (2018) 351–357.

DOI: 10.1016/j.ceramint.2017.09.180

Google Scholar

[15] P. Xiao, W. Li, S. Chen, G. Li, Z. Dai, M. Feng, X. Chen, W. Yang, Effects of Oxygen Pressurization on Li+/Ni2+ Cation Mixing and the Oxygen Vacancies of LiNi0.8Co0.15Al0.05O2 Cathode Materials, ACS Appl Mater Interfaces 14 (2022) 31851–31861.

DOI: 10.1021/acsami.2c05136

Google Scholar

[16] N. V. Kosova, E.T. Devyatkina, V. V. Kaichev, Optimization of Ni2+/Ni3+ ratio in layered Li(Ni,Mn,Co)O2 cathodes for better electrochemistry, J Power Sources 174 (2007) 965–969.

DOI: 10.1016/j.jpowsour.2007.06.051

Google Scholar

[17] 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 (Basel) 13 (2021) 1628.

DOI: 10.3390/sym13091628

Google Scholar

[18] Z. Huang, M. Chu, R. Wang, W. Zhu, W. Zhao, C. Wang, Y. Zhang, L. He, J. Chen, S. Deng, L. Mei, W.H. Kan, M. Avdeev, F. Pan, Y. Xiao, Optimizing the structure of layered cathode material for higher electrochemical performance by elucidating structural evolution during heat processing, Nano Energy 78 (2020) 105194.

DOI: 10.1016/j.nanoen.2020.105194

Google Scholar