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Research Article

Converting intercalation-type cathode in spent lithium-ion batteries into conversion-type cathode

Dingding Zhu1,§, Yong Su1,§, Jingzhao Chen2,§, Xiangze Ou1, Xuedong Zhang1, Wen Xie1, Yuyan Zhou1, Yunna Guo2, Qiushi Dai2, Peng Jia2, Jitong Yan2, Lin Geng2, Baiyu Guo2, Liqiang Zhang2, Yongfu Tang2, Qiao Huang1( ), Jianyu Huang1,2( )
School of Materials Science and Engineering, Xiangtan University, Xiangtan 411105, China
Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066000, China

§ Dingding Zhu, Yong Su, and Jingzhao Chen contributed equally to this work.

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Graphical Abstract

Our studies provide a versatile strategy to recycle spent lithium-ion batteries (LIBs) and convert the intercalation-cathodes into high energy density metal fluorides by a fluorination technique, which offers a new avenue to recycle spent LIBs and substantially increase the energy densities of next generation LIBs.

Abstract

The widespread applications of lithium-ion batteries (LIBs) generate tons of spent LIBs. Therefore, recycling LIBs is of paramount importance in protecting the environment and saving the resources. Current commercialized LIBs mostly adopt layered oxides such as LiCoO2 (LCO) or LiNixCoyMn1−x−yO2 (NMC) as the cathode materials. Converting the intercalation-type spent oxides into conversion-type cathodes (such as metal fluorides (MFs)) offers a valid recycling strategy and provides substantially improved energy densities for LIBs. Herein, two typical Co-based cathodes, LCO and LiNi0.6Co0.2Mn0.2O2 (NMC622), in spent LIBs were successfully converted to CoF2 and (NixCoyMnz)F2 cathodes by a reduction and fluorination technique. The as converted CoF2 and (NixCoyMnz)F2 delivered cell energy densities of 650 and 700 Wh/kg, respectively. Advanced atomic-level electron microscopy revealed that the used LCO and NMC622 were converted to highly phase pure Co metal and Ni0.6Co0.2Mn0.2 alloys in the used graphite-assisted reduction roasting, simultaneously producing the important product of Li2CO3 using only environment friendly solvent. Our study provided a versatile strategy to convert the intercalation-type Co-based cathode in the spent LIBs into conversion-type MFs cathodes, which offers a new avenue to recycle the spent LIBs and substantially increase the energy densities of next generation LIBs.

Keywords

spent lithium-ion batteriesrecyclingenergy densitiesconversion-type cathode

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Nano Research
Volume 17 Issue 5,
May 2024
Pages 4602-4609
DOI: 10.1007/s12274-023-6289-3
Cite this article:
Zhu D, Su Y, Chen J, et al. Converting intercalation-type cathode in spent lithium-ion batteries into conversion-type cathode. Nano Research, 2024, 17(5): 4602-4609. https://doi.org/10.1007/s12274-023-6289-3
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Received: 09 September 2023
Revised: 17 October 2023
Accepted: 25 October 2023
Published: 21 November 2023
© Tsinghua University Press 2023
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