Recovery of Cobalt from Used Lithium-Ion Batteries and its Leaching Kinetics

Alfred Obaje¹ , Douglas Onyancha² , Samuel Mirie³

1. Department of Chemistry, Dedan Kimathi University of Technology, Private Bag - 10143, Dedan Kimathi, Nyeri Kenya.
2. Department of Chemistry, Dedan Kimathi University of Technology, Private Bag - 10143, Dedan Kimathi, Nyeri Kenya.
3. Department of Chemistry, Dedan Kimathi University of Technology, Private Bag - 10143, Dedan Kimathi, Nyeri Kenya.

Section:Research Paper, Product Type: Journal-Paper
Vol.10 , Issue.3 , pp.1-12, Jun-2023

Online published on Jun 30, 2023

Copyright © Alfred Obaje, Douglas Onyancha, Samuel Mirie . This is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
 

View this paper at   Google Scholar | DPI Digital Library

XML View     PDF Download

How to Cite this Paper

109 Views    268 Downloads    31 Downloads

Abstract :
Lithium-ion batteries are frequently employed as rechargeable batteries, driving most of electronics and electric cars, significantly increased the quantity of utilized LIBs. Hence, ecosystems may be threatened by these used LIBs, due to the presence of heavy metals and poisonous electrolytes. Hence, for sound protection and financial considerations, it is highly essential to develop an efficient method to recycle used LIBs with an aim of preventing hazardous compounds entering ecosystem and endangering people’s health and recover valuable metal. The study concentrated on cobalt recovery using hydrometallurgical and thermal treatment techniques that enhanced a high rate of recovery, low energy use, and less waste production. Used LIBs of mobile phones, were collected from phone repairing shops in Nyeri town, Kenya. Hydrometallurgical process which involves acid leaching using mineral acids and organic acids was applied by using H2O2 as a reductant. Leaching process was optimized by varying parameters (type of acid, acid concentration, reductant dosage, time, and temperature). Cobalt ion concentration level in liquor, was analysed via ICP - OES, and finally cobalt was extracted from the leachate liquor via precipitation. XRF analysis showed that cathode active material has highest composition of 61.72 % cobalt and other valuable metals like 12.11 % Ni and 9.64 % Mn, hence need of recycling the cathode active material to recover the valuable metals and minimize chances of heavy metals release into the environment. Optimum conditions for leaching cobalt from cathode material were as follows: 80 ?, 120 minutes, 1.5 % v/v of H2O2, for both 3M H2SO4 and 2M C6H8O7. The cobalt leaching followed chemical reaction model, with best satisfactory regression coefficient fitting values above 0.98 and activation energy as 21.84 and 7.89 kJ/mol, and percentage recovery of 82.75 % and 67.47 % while using 3M H2SO4 and 2M C6H8O7 respectively.

Key-Words / Index Term :
Lithium-ion batteries (LIBs), Lithium cobalt oxide (LiCoO2), Polyvinylidene fluoride (PVDF), Leaching Kinetics

References :
[1]. W. S. Chen and H. J. Ho, “Recovery of valuable metals from lithium-ion batteries NMC cathode waste materials by hydrometallurgical methods,” Metals (Basel), vol. 8, no. 5, May 2018, : 10.3390/met8050321.
[2]. Zheng X, Zhu Z, Lin Z, “A Mini-Review on Metal Recycling from Spent Lithium-Ion Batteries,” Engineering, vol. 4, no. 3. Elsevier Ltd, pp. 361–370, Jun. 01, 2018. doi: 10.1016/j.eng.2018.05.018.
[3]. E. Asadi Dalini, G. Karimi, S. Zandevakili, and M. Goodarzi, “A Review on Environmental, Economic and Hydrometallurgical Processes of Recycling Spent Lithium-ion Batteries,” Mineral Processing and Extractive Metallurgy Review. Taylor and Francis Inc., pp. 1–22, 2020. doi: 10.1080/08827508.2020.1781628.
[4]. Wang F, Zhang T, He Y, “Recovery of valuable materials from spent lithium-ion batteries by mechanical separation and thermal treatment,” J Clean Prod, vol. 185, pp. 646–652, Jun. 2018, doi: 10.1016/j.jclepro.2018.03.069.
[5]. Raj T, Chandrasekhar, “Recycling of cathode material from spent lithium-ion batteries: Challenges and future perspectives,” J Hazard Mater, vol. 429, May 2022, doi: 10.1016/j.jhazmat.2022.128312.
[6]. R. Golmohammadzadeh, F. Rashchi, and E. Vahidi, “Recovery of lithium and cobalt from spent lithium-ion batteries using organic acids: Process optimization and kinetic aspects,” Waste Management, vol. 64, pp. 244–254, Jun. 2017, doi: 10.1016/j.wasman.2017.03.037.
[7]. S. Yan, C. Sun, T. Zhou, R. Gao, and H. Xie, “Ultrasonic-assisted leaching of valuable metals from spent lithium-ion batteries using organic additives,” Sep Purif Technol, vol. 257, Feb. 2021, doi: 10.1016/j.seppur.2020.117930.
[8]. R. Sattar, S. Ilyas, H. N. Bhatti, and A. Ghaffar, “Resource recovery of critically-rare metals by hydrometallurgical recycling of spent lithium-ion batteries,” Sep Purif Technol, vol. 209, pp. 725–733, Jan. 2019, doi: 10.1016/j.seppur.2018.09.019.
[9]. Yuliusman, Silvia, A. Nurqomariah, and R. Fajaryanto, “Recovery of cobalt and nickel from spent lithium-ion batteries with citric acid using leaching process: Kinetics study,” in E3S Web of Conferences, EDP Sciences, Nov. 2018. doi: 10.1051/e3sconf/20186703008.
[10]. Wang S, Tian Y, Zhang, “A Review of Processes and Technologies for the Recycling of Spent Lithium-ion Batteries,” in IOP Conference Series: Materials Science and Engineering, Institute of Physics Publishing, Apr. 2020. doi: 10.1088/1757-899X/782/2/022025.
[11]. M. K. Jha, A. Kumari, A. K. Jha, V. Kumar, J. Hait, and B. D. Pandey, “Recovery of lithium and cobalt from waste lithium-ion batteries of mobile phone,” Waste Management, vol. 33, no. 9, pp. 1890–1897, Sep. 2013, doi: 10.1016/j.wasman.2013.05.008.
[12]. X. Chen, L. Cao, D. Kang, J. Li, T. Zhou, and H. Ma, “Recovery of valuable metals from mixed types of spent lithium-ion batteries. Part II: Selective extraction of lithium,” Waste Management, vol. 80, pp. 198–210, Oct. 2018, doi: 10.1016/j.wasman.2018.09.013.
[13]. J. Lie and J. C. Liu, “Closed-vessel microwave leaching of valuable metals from spent lithium-ion batteries (LIBs) using dual-function leaching agent: Ascorbic acid,” Sep Purif Technol, vol. 266, Jul. 2021, doi: 10.1016/j.seppur.2021.118458.
[14]. M. M. Torabian, M. Jafari, and A. Bazargan, “Discharge of lithium-ion batteries in salt solutions for safer storage, transport, and resource recovery,” Waste Management and Research, 2021, doi: 10.1177/0734242X211022658.
[15]. Santos M, Garde I, Ro, “A technology for recycling lithium-ion batteries promoting the circular economy: The RecycLib,” Resour Conserv Recycl, vol. 175, Dec. 2021, doi: 10.1016/j.resconrec.2021.105863.
[16]. M. Yu, Z. Zhang, F. Xue, B. Yang, G. Guo, and J. Qiu, “A more simple and efficient process for recovery of cobalt and lithium from spent lithium-ion batteries with citric acid,” Sep Purif Technol, vol. 215, pp. 398–402, May 2019, doi: 10.1016/j.seppur.2019.01.027.
[17]. W. Lv, Z. Wang, H. Cao, Y. Sun, Y. Zhang, and Z. Sun, “A Critical Review and Analysis on the Recycling of Spent Lithium-Ion Batteries,” ACS Sustainable Chemistry and Engineering, vol. 6, no. 2. American Chemical Society, pp. 1504–1521, Feb. 05, 2018. doi: 10.1021/acssuschemeng.7b03811.
[18]. P. Alves Dias, D. Blagoeva, C. C. Pavel, N. Arvanitidis, and Europa?ische Kommission Gemeinsame Forschungsstelle, Cobalt demand-supply balances in the transition to electric mobility. pp. 25–49, 2017.
[19]. Gao W, Liu C, Cao H, “Comprehensive evaluation on effective leaching of critical metals from spent lithium-ion batteries,” Waste Management, vol. 75, pp. 477–485, May 2018, doi: 10.1016/j.wasman.2018.02.023.
[20]. Quintero-Almanza D, G, “Recovery of cobalt from spent lithium-ion mobile phone batteries using liquid–liquid extraction,” Batteries, vol. 5, no. 2, Jun. 2019, doi: 10.3390/batteries5020044.
[21]. K. Chabhadiya, R. R. Srivastava, and P. Pathak, “Two-step leaching process and kinetics for an eco-friendly recycling of critical metals from spent Li-ion batteries,” J Environ Chem Eng, vol. 9, no. 3, Jun. 2021, doi: 10.1016/j.jece.2021.105232.
[22]. S. P. Barik, G. Prabaharan, and L. Kumar, “Leaching and separation of Co and Mn from electrode materials of spent lithium-ion batteries using hydrochloric acid: Laboratory and pilot scale study,” J Clean Prod, vol. 147, pp. 37–43, Mar. 2017, doi: 10.1016/j.jclepro.2017.01.095.
[23]. A. Pehkonen, “The possibilities of cobalt and lithium recovery from spent portable lithium accumulators in laboratory scale.” pp. 3–12, 2015.
[24]. S. Anwani, R. Methekar, and V. Ramadesigan, “Resynthesizing of lithium cobalt oxide from spent lithium-ion batteries using an environmentally benign and economically viable recycling process,” Hydrometallurgy, vol. 197, Nov. 2020, doi: 10.1016/j.hydromet.2020.105430.
[25]. M. Lu, X. Zheng, H. Zhang, B. Wang, and C. Dai, “The Re-Synthesis of LiCoO2 from Spent Lithium-Ion Batteries Separated by Vacuum-Assisted Heat-Treating Method Safety performance of lithium-ion battery View project The Re-Synthesis of LiCoO 2 from Spent Lithium-Ion Batteries Separated by Vacuum-Assisted Heat-Treating Method,” 2013. [Online]. Available: www.electrochemsci.org
[26]. X. Chen, D. Kang, L. Cao, J. Li, T. Zhou, and H. Ma, “Separation and recovery of valuable metals from spent lithium-ion batteries: Simultaneous recovery of Li and Co in a single step,” Sep Purif Technol, vol. 210, pp. 690–697, Feb. 2019, doi: 10.1016/j.seppur.2018.08.072.
[27]. Tang X, Tang W, Duan, “Recovery of valuable metals and modification of cathode materials from spent lithium-ion batteries,” J Alloys Compd, vol. 874, Sep. 2021, doi: 10.1016/j.jallcom.2021.159853.
[28]. A. A. Nayl, R. A. Elkhashab, S. M. Badawy, and M. A. El-Khateeb, “Acid leaching of mixed spent Li-ion batteries,” Arabian Journal of Chemistry, vol. 10, pp. S3632–S3639, May 2017, doi: 10.1016/j.arabjc.2014.04.001.
[29]. L. Yu, B. Shu, and S. Yao, “Recycling of Cobalt by Liquid Leaching from Waste 18650-Type Lithium-Ion Batteries,” Advances in Chemical Engineering and Science, vol. 05, no. 04, pp. 425–429, 2015, doi: 10.4236/aces.2015.54043.
[30]. F. Wang, R. Sun, J. Xu, Z. Chen, and M. Kang, “Recovery of cobalt from spent lithium-ion batteries using sulphuric acid leaching followed by solid-liquid separation and solvent extraction,” RSC Adv, vol. 6, no. 88, pp. 85303–85311, 2016, doi: 10.1039/c6ra16801a.
[31]. Gao W, Song J, Cao H, “Selective recovery of valuable metals from spent lithium-ion batteries – Process development and kinetics evaluation,” J Clean Prod, vol. 178, pp. 833–845, Mar. 2018, doi: 10.1016/j.jclepro.2018.01.040.
[32]. X. Chen, T. Zhou, J. Kong, H. Fang, and Y. Chen, “Separation and recovery of metal values from leach liquor of waste lithium nickel cobalt manganese oxide-based cathodes,” Sep Purif Technol, vol. 141, pp. 76–83, Feb. 2015, doi: 10.1016/j.seppur.2014.11.039.
[33]. D. Yu, Z. Huang, B. Makuza, X. Guo, and Q. Tian, “Pretreatment options for the recycling of spent lithium-ion batteries: A comprehensive review,” Minerals Engineering, vol. 173. Elsevier Ltd, Nov. 01, 2021. doi: 10.1016/j.mineng.2021.107218.
[34]. Shaw-Stewart J, Alvare, “Aqueous solution discharge of cylindrical lithium-ion cells,” Sustainable Materials and Technologies, vol. 22, Dec. 2019, doi: 10.1016/j.susmat.2019.e00110.
[35]. Zheng X, Zhu Z, Lin X, “A Mini-Review on Metal Recycling from Spent Lithium-Ion Batteries,” Engineering, vol. 4, no. 3. Elsevier Ltd, pp. 361–370, Jun. 01, 2018. doi: 10.1016/j.eng.2018.05.018.A
36]. B. Musariri, G. Akdogan, C. Dorfling, and S. Bradshaw, “Evaluating organic acids as alternative leaching reagents for metal recovery from lithium-ion batteries,” Miner Eng, vol. 137, pp. 108–117, Jun. 2019, doi: 10.1016/j.mineng.2019.03.027.
[37]. Y. Zhang, Q. Meng, P. Dong, J. Duan, and Y. Lin, “Use of grape seed as reductant for leaching of cobalt from spent lithium-ion batteries,” Journal of Industrial and Engineering Chemistry, vol. 66, pp. 86–93, Oct. 2018, doi: 10.1016/j.jiec.2018.05.004.
[38]. Q. Li, B. Zhang, X. B. Min, and W. Q. Shen, “Acid leaching kinetics of zinc plant purification residue,” Transactions of Nonferrous Metals Society of China (English Edition), vol. 23, no. 9, pp. 2786–2791, 2013, doi: 10.1016/S1003-6326(13)62798-3.
[39]. F. Faraji, A. Alizadeh, F. Rashchi, and N. Mostoufi, “Kinetics of leaching: A review,” Reviews in Chemical Engineering, vol. 38, no. 2. De Gruyter Open Ltd, pp. 113–148, Feb. 01, 2022. doi: 10.1515/revce-2019-0073.
[40]. D. Aurbach, B. Markovsky, A. Rodkin, M. Cojocaru, E. Levi, and H.-J. Kim, “An analysis of rechargeable lithium-ion batteries after prolonged cycling.” [Online]. Available: www.elsevier.com/locate/electacta
[41]. Ajiboye E, Panda P, “Leaching kinetics of Cu, Ni and Zn from waste silica rich integrated circuits using mild nitric acid,” Hydrometallurgy, vol. 188, pp. 161–168, Sep. 2019, doi: 10.1016/j.hydromet.2019.06.016.
[42]. S. S. Behera and P. K. Parhi, “Leaching kinetics study of neodymium from the scrap magnet using acetic acid,” Sep Purif Technol, vol. 160, pp. 59–66, Feb. 2016, doi: 10.1016/j.seppur.2016.01.014.
[43]. Li L, Qu W, Zhang X, L, “Succinic acid-based leaching system: A sustainable process for recovery of valuable metals from spent Li-ion batteries,” J Power Sources, vol. 282, pp. 544–551, May 2015, doi: 10.1016/j.jpowsour.2015.02.073.
[44]. X. Chen, D. Kang, L. Cao, J. Li, T. Zhou, and H. Ma, “Separation and recovery of valuable metals from spent lithium-ion batteries: Simultaneous recovery of Li and Co in a single step,” Sep Purif Technol, vol. 210, pp. 690–697, Feb. 2019, doi: 10.1016/j.seppur.2018.08.072.
[45]. Chen X, Guo C, Ma H, “Organic reductants-based leaching: A sustainable process for the recovery of valuable metals from spent lithium-ion batteries,” Waste Management, vol. 75, pp. 459–468, May 2018, doi: 10.1016/j.wasman.2018.01.021.
[46]. V. Agarwal, M. K. Khalid, A. Porvali, B. P. Wilson, and M. Lundström, “Recycling of spent NiMH batteries: Integration of battery leach solution into primary Ni production using solvent extraction,” Sustainable Materials and Technologies, vol. 22, Dec. 2019, doi: 10.1016/j.susmat.2019.e00121.
[47]. A. H. Shuva, A. S. W. Kurny, and A. I. Journal, “Characterization of spent lithium-ion batteries in the process of recovery of value metals Materials Science.” pp. 5–11, 2017
[48]. A. Obaje, D. Onyancha, and S. Mirie, “Pre-Treatment and Characterization of Cathode Active Material from Spent Lithium-Ion Batteries,” International Journal of Scientific Research in Chemical Sciences, vol. 10, no. 1, pp. 8–15, 2023, doi: 10.26438/ijsrcs/v10i1.815.
[49]. R. Golmohammadzadeh, F. Faraji, and F. Rashchi, “Recovery of lithium and cobalt from spent lithium-ion batteries (LIBs) using organic acids as leaching reagents: A review,” Resources, Conservation and Recycling, vol. 136. Elsevier B.V., pp. 418–435, Sep. 01, 2018. doi: 10.1016/j.resconrec.2018.04.024.
[50]. M. B. Mansur, A. S. Guimarães, and M. Petraniková, “An Overview on the Recovery of Cobalt from End-of-life Lithium-Ion Batteries,” Mineral Processing and Extractive Metallurgy Review, vol. 43, no. 4. Taylor and Francis Ltd., pp. 489–509, 2022. doi: 10.1080/08827508.2021.1883014.
[51]. Nayaka G, Zhang Y, He Y, “An environmentally friendly attempt to recycle the spent Li-ion battery cathode through organic acid leaching,” J Environ Chem Eng, vol. 7, no. 1, Feb. 2019, doi: 10.1016/j.jece.2018.102854.