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Özge Yazıcı_edited.jpg

Özge Yazıcı, BSc. Student 

Metallurgical and Materials Engineering

Yıldız Technical Universityözgeyazıcı

Li-Ion Recycling-based Sustainable Production of Glass-Ceramic Raw Materials

Supervisors: Kumru Karaman, Yasin Bozkurt Yılmaz, Assoc Prof. Dr. Buğra Çiçek

Global demand for lithium-ion batteries is roughly doubling every year and the primary market switches from portable devices to electric vehicles.[1] This growing demand causes more used batteries than ever since the current primary market requires more energy.[1] Besides environmental concerns, if growth continues at this rate, lithium can be in a critical situation to use in other industries such as ceramics and glass manufacturing.[1][2] Therefore, the recycling of lithium-ion batteries is becoming more necessary nowadays. The recycling processes of batteries are divided into two groups, physical processes and chemical processes. Physical processes are pretreatments that are dismantling, crushing, screening, magnetic separation, washing, and thermal pretreatment while chemical processes are pyrometallurgical processes and hydrometallurgical processes. Pyrometallurgical processes are mainly used for the recovery of cobalt, however, copper and nickel can be also recovered.[3][4] To recover lithium with pyrometallurgy, slag should be processed.[3] Hydrometallurgical processes were initially made only for lithium recovery; however, they can recover many components today.[5][6] Hydrometallurgical processes involve leaching and recovery steps, and they offer higher recovery efficiency in general.[5][6] The initial aim of this project was to recover the cathode materials of lithium-ion batteries because the cathode content contains valuable components such as cobalt. Pyrolytic methods were tried to remove the anode material, which is graphite, and binders. However, it leads to some disadvantages such as undesirable phase transitions, high heat consumption, and emission of carbon dioxide or carbon monoxide. Therefore, it is decided to recycle the graphite and further strategies are searched to serve the purpose. It is desirable to separate the anode and cathode at the beginning of the recycling process with low-cost and sustainable methods. From this point of view, the initial process flow sheet is updated by adding new steps to recover graphite. The major process is flotation. However, direct flotation is not efficient because of similar surface properties of electrode materials due to being covered with binders and other functional groups.[7][8][9] The materials should be prepared for the flotation process in the initial steps such as grinding, pyrolysis, and ultrasonic pretreatment.[11][12][13] This project aims to recover at as high as possible recovery rate with the anode, which is graphite, and cathode materials. Recovered cathode materials will be used as glass-ceramic enamel.
[1] Zubi, Ghassan & Dufo-López, Rodolfo & Carvalho, Monica & Pasaoglu, Guzay, 2018. "The lithium-ion battery: State of the art and future perspectives," Renewable and Sustainable Energy Reviews, Elsevier, vol. 89(C), pages 292-308, doi: 10.1016/j.rser.2018.03.002.
[2] Schulz, K.J., DeYoung, J.H., Jr., Bradley, D.C., and Seal, R.R., II, 2017, Critical mineral resources of the United States—An introduction, chap. A of Schulz, K.J., DeYoung, J.H., Jr., Seal, R.R., II, and Bradley, D.C., eds., Critical mineral resources of the United States—Economic and environmental geology and prospects for future supply: U.S. Geological Survey Professional Paper 1802,
[3] S. Doose, J. K. Mayer, P. Michalowski, and A. Kwade, “Challenges in ecofriendly battery recycling and closed material cycles: A perspective on future lithium battery generations,” Metals (Basel)., vol. 11, no. 2, pp. 1–17, 2021, doi: 10.3390/met11020291.
[4] Bruckner L, Frank J, Elwert T. Industrial recycling of lithium-ion batteries – acritical review of metallurgical process routes. Metals-Basel. 2020;10:1107.
[5] H. Bae, Y. Kim; «Technologies of lithium recycling from waste lithium ion batteries: a review»; 2021. DOI: 10.1039/d1ma00216c
[6] B. Huang, Z. Pan, X. Su, and L. An, “Recycling of lithium-ion batteries: Recent advances and perspectives,” J. Power Sources, vol. 399, no. July, pp. 274–286, 2018, doi: 10.1016/j.jpowsour.2018.07.116.
[7] Zhang, G.; He, Y.; Wang, H.; Feng, Y.; Xie, W.; Zhu, X. Application of mechanical crushing combined with pyrolysis-enhancedflotation technology to recover graphite and LiCoO2 from spent lithium-ion batteries. J. Clean. Prod. 2019, 231, 1418–1427
[8] C. Hanisch, T. Loellhoeffel, J. Diekmann, K. J. Markley, W. Haselrieder, A. Kwade, Journal of Cleaner Production 2015, 108, 301-311.
[9] A. S. Rothermel et al., “Title : Graphite recycling from Spent Lithium Ion Batteries Graphite Recycling from Spent Lithium Ion Batteries.”
[10] S. Editors, C. Herrmann, and S. Kara, Recycling of Lithium-Ion Batteries.
[11] J. Yu, Y. He, Z. Ge, H. Li, W. Xie, and S. Wang, “A promising physical method for recovery of LiCoO2 and graphite from spent lithium-ion batteries: Grinding flotation,” Sep. Purif. Technol., vol. 190, no. August 2017, pp. 45–52, 2018, doi: 10.1016/j.seppur.2017.08.049.
[12] G. Zhang, Y. He, H. Wang, Y. Feng, W. Xie, and X. Zhu, “Application of mechanical crushing combined with pyrolysis-enhanced flotation technology to recover graphite and LiCoO2 from spent lithium-ion batteries,” J. Clean. Prod., vol. 231, pp. 1418–1427, 2019, doi: 10.1016/j.jclepro.2019.04.279.
[13] G. Zhang, Y. He, Y. Feng, H. Wang, and X. Zhu, “Pyrolysis-Ultrasonic-Assisted Flotation Technology for Recovering Graphite and LiCoO2 from Spent Lithium-Ion

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