Study on metal recovery process and kinetics of oxidative leaching from spent LiFePO4 Li-batteries

doi:10.1016/j.cjche.2023.12.022

Chinese Journal of Chemical Engineering ›› 2024, Vol. 68 ›› Issue (4): 94-102.DOI: 10.1016/j.cjche.2023.12.022

Study on metal recovery process and kinetics of oxidative leaching from spent LiFePO₄ Li-batteries

Xiaoming Zhang^1,2, Wen Xie³, Xiaolei Zhou³, Wenjie Zhang^1,2, Jiawei Wen^1,2, Xin Wang^1,2,4, Guoyong Huang^1,2, Shengming Xu^5,6

1. College of New Energy and Materials, China University of Petroleum, Beijing 102249, China;
2. State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum, Beijing 102249, China;
3. Beijing Spacecrafts, Beijing 100094, China;
4. Ganfeng Lithium Group Co., Ltd., Xinyu 338000, China;
5. Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China;
6. Beijing Key Laboratory of Fine Ceramics, Tsinghua University, Beijing 100084, China

Received:2023-09-28 Revised:2023-11-13 Online:2024-06-28 Published:2024-04-28
Contact: Xin Wang,E-mail address:WX841780383@163.com;Guoyong Huang,E-mail address:huanggy@cup.edu.cn
Supported by:
This project was supported by the National Natural Science Foundation of China (51834008, 52022109, 52274307, and 21804319), National Key Research and Development Program of China (2021YFC2901100), Science Foundation of China University of Petroleum, Beijing (2462022QZDX008, 2462021QNX2010, 2462020YXZZ019 and 2462020YXZZ016), State Key Laboratory of Heavy Oil Processing (HON-KFKT2022-10).

Study on metal recovery process and kinetics of oxidative leaching from spent LiFePO₄ Li-batteries

Xiaoming Zhang^1,2, Wen Xie³, Xiaolei Zhou³, Wenjie Zhang^1,2, Jiawei Wen^1,2, Xin Wang^1,2,4, Guoyong Huang^1,2, Shengming Xu^5,6

1. College of New Energy and Materials, China University of Petroleum, Beijing 102249, China;
2. State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum, Beijing 102249, China;
3. Beijing Spacecrafts, Beijing 100094, China;
4. Ganfeng Lithium Group Co., Ltd., Xinyu 338000, China;
5. Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China;
6. Beijing Key Laboratory of Fine Ceramics, Tsinghua University, Beijing 100084, China

通讯作者: Xin Wang,E-mail address:WX841780383@163.com;Guoyong Huang,E-mail address:huanggy@cup.edu.cn
基金资助:
This project was supported by the National Natural Science Foundation of China (51834008, 52022109, 52274307, and 21804319), National Key Research and Development Program of China (2021YFC2901100), Science Foundation of China University of Petroleum, Beijing (2462022QZDX008, 2462021QNX2010, 2462020YXZZ019 and 2462020YXZZ016), State Key Laboratory of Heavy Oil Processing (HON-KFKT2022-10).

Abstract

Abstract: A green environmental protection and enhanced leaching process was proposed to recover all elements from spent lithium iron phosphate (LiFePO₄) lithium batteries. In order to reduce the influence of Al impurity in the recovery process, NaOH was used to remove impurity. After impurity removal, the spent LiFePO₄ cathode material was used as raw material under the H₂SO₄ system, and the pressure oxidation leaching process was adopted to achieve the preferential leaching of lithium. The E-pH diagram of the Fe-P-Al-H₂O system can determine the stable region of each element in the recovery process of spent LiFePO₄ Li-batteries. Under the optimal conditions (500 r·min^-1, 15 h, 363.15 K, 0.4 MPa, the liquid-solid ratio was 4:1 ml·g^-1 and the acid-material ratio was 0.29), the leaching rate of Li was 99.24%, Fe, Al, and Ti were 0.10%, 2.07%, and 0.03%, respectively. The Fe and P were precipitated and recovered as FePO₄·2H₂O. The kinetic analysis shows that the process of high-pressure acid leaching of spent LiFePO₄ materials depends on the surface chemical reaction. Through the life cycle assessment (LCA) of the spent LiFePO₄ whole recovery process, eight midpoint impact categories were selected to assess the impact of recovery process. The results can provide basic environmental information on production process for recycling industry.

Key words: Spent LiFePO₄ Li-batteries, Oxidative leaching, Kinetic study, Life cycle assessment

摘要： A green environmental protection and enhanced leaching process was proposed to recover all elements from spent lithium iron phosphate (LiFePO₄) lithium batteries. In order to reduce the influence of Al impurity in the recovery process, NaOH was used to remove impurity. After impurity removal, the spent LiFePO₄ cathode material was used as raw material under the H₂SO₄ system, and the pressure oxidation leaching process was adopted to achieve the preferential leaching of lithium. The E-pH diagram of the Fe-P-Al-H₂O system can determine the stable region of each element in the recovery process of spent LiFePO₄ Li-batteries. Under the optimal conditions (500 r·min^-1, 15 h, 363.15 K, 0.4 MPa, the liquid-solid ratio was 4:1 ml·g^-1 and the acid-material ratio was 0.29), the leaching rate of Li was 99.24%, Fe, Al, and Ti were 0.10%, 2.07%, and 0.03%, respectively. The Fe and P were precipitated and recovered as FePO₄·2H₂O. The kinetic analysis shows that the process of high-pressure acid leaching of spent LiFePO₄ materials depends on the surface chemical reaction. Through the life cycle assessment (LCA) of the spent LiFePO₄ whole recovery process, eight midpoint impact categories were selected to assess the impact of recovery process. The results can provide basic environmental information on production process for recycling industry.

关键词: Spent LiFePO₄ Li-batteries, Oxidative leaching, Kinetic study, Life cycle assessment

Xiaoming Zhang, Wen Xie, Xiaolei Zhou, Wenjie Zhang, Jiawei Wen, Xin Wang, Guoyong Huang, Shengming Xu. Study on metal recovery process and kinetics of oxidative leaching from spent LiFePO₄ Li-batteries[J]. Chinese Journal of Chemical Engineering, 2024, 68(4): 94-102.

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Study on metal recovery process and kinetics of oxidative leaching from spent LiFePO₄ Li-batteries

Study on metal recovery process and kinetics of oxidative leaching from spent LiFePO₄ Li-batteries

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