ACS Publications. Most Trusted. Most Cited. Most Read

OR SEARCH CITATIONS

My Activity
Publications
CONTENT TYPES

Figure 1Loading Img
Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Sustainable Chem. Eng. 2021, 9, 17, 6048-6055
RETURN TO ISSUEPREVResearch ArticleNEXT

Recovery of Cathode Materials and Aluminum Foil Using a Green Solvent

  • Yaocai Bai*
    Yaocai Bai
    Electrification and Energy Infrastructures Division, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, Tennessee 37830, United States
    *Email: [email protected]
    More by Yaocai Bai
    Orcidhttp://orcid.org/0000-0003-3700-2520
  • , 
  • Rachid Essehli
    Rachid Essehli
    Electrification and Energy Infrastructures Division, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, Tennessee 37830, United States
    More by Rachid Essehli
  • , 
  • Charl J. Jafta
    Charl J. Jafta
    Electrification and Energy Infrastructures Division, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, Tennessee 37830, United States
    More by Charl J. Jafta
    Orcidhttp://orcid.org/0000-0002-9773-6799
  • , 
  • Kelsey M. Livingston
    Kelsey M. Livingston
    Electrification and Energy Infrastructures Division, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, Tennessee 37830, United States
    More by Kelsey M. Livingston
  • , and 
  • Ilias Belharouak*
    Ilias Belharouak
    Electrification and Energy Infrastructures Division, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, Tennessee 37830, United States
    Bredesen Center for Interdisciplinary Research and Graduate Education, The University of Tennessee, 821 Volunteer Blvd., Knoxville, Tennessee 37996, United States
    *Email: [email protected]
    More by Ilias Belharouak
    Orcidhttp://orcid.org/0000-0002-3985-0278
Cite this: ACS Sustainable Chem. Eng. 2021, 9, 17, 6048–6055
Publication Date (Web):April 20, 2021
https://doi.org/10.1021/acssuschemeng.1c01293
Copyright © 2021 American Chemical Society
Request reuse permissions

    Article Views

    2624

    Altmetric

    -

    Citations

    34
    LEARN ABOUT THESE METRICS
    Read OnlinePDF (10 MB)
    Get e-Alerts
    Supporting Info (1)»
    SUBJECTS:

    Abstract

    Abstract Image

    Effective separation of cathode materials and current collectors is one of the most enabling steps, yet a very challenging step, in recycling electrode scraps and spent Li-ion cells. Here, a green solvent, triethyl phosphate, was used to recover invaluable cobalt-containing cathodes, such as NMC622, by dissolving the polymeric binder of poly(vinylidene fluoride). Electrochemically active materials were separated from cathode scraps collected at the manufacturing step of electrodes through a solvent-based separation method without jeopardizing their physical characteristics, crystalline structure, and electrochemical performance. We found that the recovered aluminum foils were clean without any sign of corrosion and that the polymeric binder could be recovered via a non-solvent-induced phase separation. Additionally, recovery of cathode materials from spent cells was achieved using refined separation parameters based on the recycling of cathode scraps. It is anticipated that this green solvent-based separation for cathode recovery will attract significant interest by the lithium-ion battery manufacturing and recycling communities.

    KEYWORDS:

    Supporting Information

    ARTICLE SECTIONS
    Jump To

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acssuschemeng.1c01293.

    • Electrochemical history of the pouch cell; photos of the recycled cathode powder on a large scale; photos of recovered materials from the spent cathode under different separation conditions; and XRD patterns of the spent cathode of NMC622 and the recovered NMC622 powder (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 34 publications.

    1. Shuai Yan, Haomiao Li, Wenxin Chen, Hao Zhou, Xianbo Zhou, Weixin Zhang, Zehang Li, Yaling He, Kangli Wang, Kai Jiang. Full-Lifetime Recycling and Reutilization of Key Materials of Low-Cost and Sustainable Liquid Metal Batteries. ACS Sustainable Chemistry & Engineering 2023, Article ASAP.
    2. Md. Sajibul Alam Bhuyan, Hosop Shin. Green Recovery of Cathode Active Materials from Li-Ion Battery Electrode Scraps Using Propylene Carbonate: A Novel Approach for Direct Recycling. ACS Sustainable Chemistry & Engineering 2023, 11 (29) , 10677-10687. https://doi.org/10.1021/acssuschemeng.3c01278
    3. Anthony T. Montoya, Zhenzhen Yang, Erik U. Dahl, Krzysztof Z. Pupek, Bryant Polzin, Alison Dunlop, J. T. Vaughey. Direct Recycling of Lithium-Ion Battery Cathodes: A Multi-Stage Annealing Process to Recover the Pristine Structure and Performance. ACS Sustainable Chemistry & Engineering 2022, 10 (40) , 13319-13324. https://doi.org/10.1021/acssuschemeng.2c02643
    4. Yaocai Bai Nitin Muralidharan Jagjit Nanda Ilias Belharouak . Enabling Sustainable Lithium-Ion Battery Manufacturing via Recycling. , 551-565. https://doi.org/10.1021/bk-2022-1412.ch013
    5. Jianlin Li, James Fleetwood, W. Blake Hawley, William Kays. From Materials to Cell: State-of-the-Art and Prospective Technologies for Lithium-Ion Battery Electrode Processing. Chemical Reviews 2022, 122 (1) , 903-956. https://doi.org/10.1021/acs.chemrev.1c00565
    6. Zhang Xu, Liang Zhiyuan, Ma Wenjun, Zhao Qinxin. Pretreatment options for the recycling of spent lithium-ion batteries: A comprehensive review. Journal of Energy Storage 2023, 72 , 108691. https://doi.org/10.1016/j.est.2023.108691
    7. Tushar Maske, Ravi Methekar. Usage of Recycled Alkali Waste for Delamination of Cathode Electrodes: Systematic Selection and Optimization of Hydrometallurgical Approach. JOM 2023, 75 (9) , 3674-3686. https://doi.org/10.1007/s11837-023-05916-1
    8. Yudie Ou, Shuxuan Yan, Lu Yuan, Xiangping Chen, Tao Zhou. Novel strategy towards in-situ recycling of valuable metals from spent lithium-ion batteries through endogenous advanced oxidation process. Journal of Hazardous Materials 2023, 457 , 131818. https://doi.org/10.1016/j.jhazmat.2023.131818
    9. Chenyu Zhang, Xueshuai Zhu, Yizi Xie, Jingying Wu, Xue Huang, Huiyuan Xu, Ping Feng. Shearing-enhanced mechanical exfoliation with mild-temperature pretreatment for cathode active material recovery from spent LIBs. Journal of Hazardous Materials 2023, 458 , 131959. https://doi.org/10.1016/j.jhazmat.2023.131959
    10. Madhushri Bhar, Shuvajit Ghosh, Satheesh Krishnamurthy, Y. Kaliprasad, Surendra K. Martha. A review on spent lithium-ion battery recycling: from collection to black mass recovery. RSC Sustainability 2023, 1 (5) , 1150-1167. https://doi.org/10.1039/D3SU00086A
    11. Tushar Maske, Sandeep Anwani, Ravi Methekar. Development of environmentally and economically sustainable delamination process for spent lithium-ion batteries. Energy Sources, Part A: Recovery, Utilization, and Environmental Effects 2023, 45 (1) , 2572-2586. https://doi.org/10.1080/15567036.2023.2187899
    12. Yaqing Guo, Chi Guo, Pengjie Huang, Qigao Han, Fuhe Wang, Hao Zhang, Honghao Liu, Yuan-Cheng Cao, Yonggang Yao, Yunhui Huang. Rejuvenating LiNi0.5Co0.2Mn0.3O2 cathode directly from battery scraps. eScience 2023, 3 (2) , 100091. https://doi.org/10.1016/j.esci.2023.100091
    13. V.M. Leal, J.S. Ribeiro, E.L.D. Coelho, M.B.J.G. Freitas. Recycling of spent lithium-ion batteries as a sustainable solution to obtain raw materials for different applications. Journal of Energy Chemistry 2023, 79 , 118-134. https://doi.org/10.1016/j.jechem.2022.08.005
    14. Xin Wang, Xiaoming Zhang, Chunmeng Zhang, Long Zhang, Jiawei Wen, Chunxia Wang, Guoyong Huang. Synthesis of high-nickel and high-performance ternary cathode materials through spent lithium-ion batteries recycling system. Sustainable Chemistry and Pharmacy 2023, 31 , 100959. https://doi.org/10.1016/j.scp.2022.100959
    15. Yaocai Bai, Mengya Li, Charl J. Jafta, Qiang Dai, Rachid Essehli, Bryant J. Polzin, Ilias Belharouak. Direct recycling and remanufacturing of anode scraps. Sustainable Materials and Technologies 2023, 35 , e00542. https://doi.org/10.1016/j.susmat.2022.e00542
    16. Jiao Lin, Xiaodong Zhang, Ersha Fan, Renjie Chen, Feng Wu, Li Li. Carbon neutrality strategies for sustainable batteries: from structure, recycling, and properties to applications. Energy & Environmental Science 2023, 16 (3) , 745-791. https://doi.org/10.1039/D2EE03257K
    17. Mengmeng Wang, Kang Liu, Jiadong Yu, Qiaozhi Zhang, Yuying Zhang, Marjorie Valix, Daniel C.W. Tsang. Challenges in Recycling Spent Lithium‐Ion Batteries: Spotlight on Polyvinylidene Fluoride Removal. Global Challenges 2023, 7 (3) https://doi.org/10.1002/gch2.202200237
    18. Changlong Chen, Vignyatha Reddy Tatagari, Hao Lin, Leon Shaw. Investigating TEP as a greener alternative to NMP in Ni-rich cathode fabrication. Journal of Energy Chemistry 2023, 78 , 240-245. https://doi.org/10.1016/j.jechem.2022.12.006
    19. Anjali Banger, Anamika Srivastava, Anjali Yadav, Ruchika Sharma, Manish Srivastava. Application of Green Solvent in Green Chemistry: An overview. Green Chemistry & Technology Letters 2023, 9 (1) , 01-14. https://doi.org/10.18510/gctl.2023.911
    20. Zheng Fang, Qiangling Duan, Qingkui Peng, Zesen Wei, Lihua Jiang, Jinhua Sun, Qingsong Wang. A sustainable delamination method to completely separate spent cathode foils via biomass-derived γ-valerolactone. Green Chemistry 2023, 25 (4) , 1546-1558. https://doi.org/10.1039/D2GC04436F
    21. Varun Gupta, Xiaolu Yu, Hongpeng Gao, Christopher Brooks, Weikang Li, Zheng Chen. Scalable Direct Recycling of Cathode Black Mass from Spent Lithium‐Ion Batteries. Advanced Energy Materials 2023, 13 (6) https://doi.org/10.1002/aenm.202203093
    22. Xuehu Zhong, Xiaohui Mao, Wenqing Qin, Hongbo Zeng, Guangjin Zhao, Junwei Han. Facile separation and regeneration of LiFePO4 from spent lithium-ion batteries via effective pyrolysis and flotation: An economical and eco-friendly approach. Waste Management 2023, 156 , 236-246. https://doi.org/10.1016/j.wasman.2022.11.045
    23. Tendai Tawonezvi, Myalelo Nomnqa, Leslie Petrik, Bernard Jan Bladergroen. Recovery and Recycling of Valuable Metals from Spent Lithium-Ion Batteries: A Comprehensive Review and Analysis. Energies 2023, 16 (3) , 1365. https://doi.org/10.3390/en16031365
    24. Jiawei Wu, Mengting Zheng, Tiefeng Liu, Yao Wang, Yujing Liu, Jianwei Nai, Liang Zhang, Shanqing Zhang, Xinyong Tao. Direct recovery: A sustainable recycling technology for spent lithium-ion battery. Energy Storage Materials 2023, 54 , 120-134. https://doi.org/10.1016/j.ensm.2022.09.029
    25. Wenhao Yu, Yi Guo, Shengming Xu, Yue Yang, Yufeng Zhao, Jiujun Zhang. Comprehensive recycling of lithium-ion batteries: Fundamentals, pretreatment, and perspectives. Energy Storage Materials 2023, 54 , 172-220. https://doi.org/10.1016/j.ensm.2022.10.033
    26. Xuehu Zhong, Junwei Han, Xiaohui Mao, Lingling Chen, Mengjun Chen, Hailing Zhu, Hongbo Zeng, Wenqing Qin. Innovative methodology for green recycling of spent lithium-ion batteries: Effective pyrolysis with DMF. Journal of Cleaner Production 2022, 377 , 134503. https://doi.org/10.1016/j.jclepro.2022.134503
    27. Yunhui Hua, Zhenghe Xu, Baojun Zhao, Zuotai Zhang. Efficient separation of electrode active materials and current collector metal foils from spent lithium-ion batteries by a green deep eutectic solvent. Green Chemistry 2022, 24 (20) , 8131-8141. https://doi.org/10.1039/D2GC02844A
    28. Xiao‐Tong Wang, Zhen‐Yi Gu, Edison Huixiang Ang, Xin‐Xin Zhao, Xing‐Long Wu, Yichun Liu. Prospects for managing end‐of‐life lithium‐ion batteries: Present and future. Interdisciplinary Materials 2022, 1 (3) , 417-433. https://doi.org/10.1002/idm2.12041
    29. Subramanian Natarajan, Manohar Akshay, Vanchiappan Aravindan. Recycling/Reuse of Current Collectors from Spent Lithium‐Ion Batteries: Benefits and Issues. Advanced Sustainable Systems 2022, 6 (3) https://doi.org/10.1002/adsu.202100432
    30. Congrui Jin, Jianlin Li. Bio-inspired nanotechnology for easy-to-recycle lithium-ion batteries. 2022, 141-158. https://doi.org/10.1016/B978-0-323-91134-4.00001-7
    31. Xing-Long Wu, Hai-Yang Xu. Advances and Challenges on Recycling the Electrode and Electrolyte Materials in Spent Lithium-Ion Batteries. Materials Lab 2022, 1 https://doi.org/10.54227/mlab.20220036
    32. Jasmin Smajic, Amira Alazmi, Nimer Wehbe, Pedro M. F. J. Costa. Electrode–Electrolyte Interactions in an Aqueous Aluminum–Carbon Rechargeable Battery System. Nanomaterials 2021, 11 (12) , 3235. https://doi.org/10.3390/nano11123235
    33. Yukun Li, Weiguang Lv, Hanlin Huang, Wenyi Yan, Xiaokang Li, Pengge Ning, Hongbin Cao, Zhi Sun. Recycling of spent lithium-ion batteries in view of green chemistry. Green Chemistry 2021, 23 (17) , 6139-6171. https://doi.org/10.1039/D1GC01639C
    34. Onurcan Buken, Kayla Mancini, Amrita Sarkar. A sustainable approach to cathode delamination using a green solvent. RSC Advances 2021, 11 (44) , 27356-27368. https://doi.org/10.1039/D1RA04922D
    Download PDF

    Pair your accounts.

    Export articles to Mendeley

    Get article recommendations from ACS based on references in your Mendeley library.

    Pair your accounts.

    Export articles to Mendeley

    Get article recommendations from ACS based on references in your Mendeley library.

    You’ve supercharged your research process with ACS and Mendeley!

    STEP 1:
    Click to create an ACS ID

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    MENDELEY PAIRING EXPIRED
    Your Mendeley pairing has expired. Please reconnect