Recycle of graphite and recovery of valuable metals from industrial-grade black mass of spent lithium-ion battery

doi:10.1016/j.cjche.2025.05.046

中国化学工程学报 ›› 2025, Vol. 88 ›› Issue (12): 335-347.DOI: 10.1016/j.cjche.2025.05.046

Recycle of graphite and recovery of valuable metals from industrial-grade black mass of spent lithium-ion battery

Shang Liu¹, Kai Wang¹, Linlin Chen¹, Yaoguo Huang¹, Xianfu Sun², Qingyan Chu¹, Yali Zhang¹

1. School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, China;
2. Haidi Power Technology Co., Ltd., Zaozhuang 277400, China

收稿日期:2025-03-10 修回日期:2025-04-18 接受日期:2025-05-28 出版日期:2026-02-09 发布日期:2025-09-18
通讯作者: Qingyan Chu,E-mail:chuqy@sdut.edu.cn;Yali Zhang,E-mail:zhangyali@sdut.edu.cn
基金资助:
The authors would like to thank the Shandong Provincial Natural Science Foundation, China (ZR2022MB129) for the financial support.

Recycle of graphite and recovery of valuable metals from industrial-grade black mass of spent lithium-ion battery

Shang Liu¹, Kai Wang¹, Linlin Chen¹, Yaoguo Huang¹, Xianfu Sun², Qingyan Chu¹, Yali Zhang¹

1. School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, China;
2. Haidi Power Technology Co., Ltd., Zaozhuang 277400, China

Received:2025-03-10 Revised:2025-04-18 Accepted:2025-05-28 Online:2026-02-09 Published:2025-09-18
Contact: Qingyan Chu,E-mail:chuqy@sdut.edu.cn;Yali Zhang,E-mail:zhangyali@sdut.edu.cn
Supported by:
The authors would like to thank the Shandong Provincial Natural Science Foundation, China (ZR2022MB129) for the financial support.

摘要/Abstract

摘要： The industrial-grade black mass of LiFePO₄/LiNi_xMn_yO₄/C from spent lithium-ion battery is difficult to be recovered because of its complex composition. In this study, a recycling of graphite and comprehensive recovery of valuable metals from industrial-grade black mass of spent lithium-ion battery was proposed. Acid leaching can separate graphite and cathode materials well. The separated graphite was purified by roasting, and its electrochemical properties were tested. The specific discharge capacity of graphite purified at 600° are the best, which reach 342.46 mA·h·g^-1 at 0.1 C. After 50 cycles at 0.1 C, the capacity retention rate was 98.26%. The charge-discharge cycle stability was improved at high rates. Nearly 100% of copper can be recovered from leaching solution by electrodeposition. FePO₄·2H₂O is recovered by adjusting the pH of the solution to 2, and α-FePO₄ is obtained by roasting. Ni, Mn and Li can be recovered by precipitation separation. The optimum conditions for the recovery process was determined, and the mechanisms of the leaching and electrodeposition process were characterized by XRD, XPS, SEM-EDS.

关键词: Spent lithium-ion batteries, Graphite, Electrodeposition, Valuable metal recovery

Abstract: The industrial-grade black mass of LiFePO₄/LiNi_xMn_yO₄/C from spent lithium-ion battery is difficult to be recovered because of its complex composition. In this study, a recycling of graphite and comprehensive recovery of valuable metals from industrial-grade black mass of spent lithium-ion battery was proposed. Acid leaching can separate graphite and cathode materials well. The separated graphite was purified by roasting, and its electrochemical properties were tested. The specific discharge capacity of graphite purified at 600° are the best, which reach 342.46 mA·h·g^-1 at 0.1 C. After 50 cycles at 0.1 C, the capacity retention rate was 98.26%. The charge-discharge cycle stability was improved at high rates. Nearly 100% of copper can be recovered from leaching solution by electrodeposition. FePO₄·2H₂O is recovered by adjusting the pH of the solution to 2, and α-FePO₄ is obtained by roasting. Ni, Mn and Li can be recovered by precipitation separation. The optimum conditions for the recovery process was determined, and the mechanisms of the leaching and electrodeposition process were characterized by XRD, XPS, SEM-EDS.

Key words: Spent lithium-ion batteries, Graphite, Electrodeposition, Valuable metal recovery

Shang Liu, Kai Wang, Linlin Chen, Yaoguo Huang, Xianfu Sun, Qingyan Chu, Yali Zhang. Recycle of graphite and recovery of valuable metals from industrial-grade black mass of spent lithium-ion battery[J]. 中国化学工程学报, 2025, 88(12): 335-347.

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Recycle of graphite and recovery of valuable metals from industrial-grade black mass of spent lithium-ion battery

Recycle of graphite and recovery of valuable metals from industrial-grade black mass of spent lithium-ion battery

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