Subtractive transformation of cathode materials in spent Li-ion batteries to a low-cobalt 5 V-class cathode material

Jun Ma; Junxiong Wang; Kai Jia; Zheng Liang; Guanjun Ji; Haocheng Ji; Yanfei Zhu; Wen Chen; Hui-Ming Cheng; Guangmin Zhou

doi:10.1038/s41467-024-45091-8

Subtractive transformation of cathode materials in spent Li-ion batteries to a low-cobalt 5 V-class cathode material

Nat Commun. 2024 Feb 5;15(1):1046. doi: 10.1038/s41467-024-45091-8.

Authors

Jun Ma¹, Junxiong Wang^{2

3}, Kai Jia^{1

4}, Zheng Liang⁴, Guanjun Ji^{1

4}, Haocheng Ji¹, Yanfei Zhu¹, Wen Chen¹, Hui-Ming Cheng^{5

6}, Guangmin Zhou⁷

Affiliations

¹ Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China.
² Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China. wjx1992@sjtu.edu.cn.
³ Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China. wjx1992@sjtu.edu.cn.
⁴ Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.
⁵ Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Science, Shenzhen, 518055, China. hm.cheng@siat.ac.cn.
⁶ Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Science, Shenyang, 110016, China. hm.cheng@siat.ac.cn.
⁷ Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China. guangminzhou@sz.tsinghua.edu.cn.

Abstract

Adding extra raw materials for direct recycling or upcycling is prospective for battery recycling, but overlooks subtracting specific components beforehand can facilitate the recycling to a self-sufficient mode of sustainable production. Here, a subtractive transformation strategy of degraded LiNi_0.5Co_0.2Mn_0.3O₂ and LiMn₂O₄ to a 5 V-class disordered spinel LiNi_0.5Mn_1.5O₄-like cathode material is proposed. Equal amounts of Co and Ni from degraded materials are selectively extracted, and the remaining transition metals are directly converted into Ni_0.4Co_0.1Mn_1.5(CO₃)₂ precursor for preparing cathode material with in-situ Co doping. The cathode material with improved conductivity and bond strength delivers high-rate (10 C and 20 C) and high-temperature (60 °C) cycling stability. This strategy with no extra precursor input can be generalized to practical degraded black mass and reduces the dependence of current cathode production on rare elements, showing the potential of upcycling from the spent to a next-generation 5 V-class cathode material for the sustainable Li-ion battery industry.

Grants and funding

U21A20174/National Science Foundation of China | NSAF Joint Fund