Sustainable upcycling of mixed spent cathodes to a high-voltage polyanionic cathode material

Guanjun Ji, Di Tang, Junxiong Wang (), Zheng Liang, Haocheng Ji, Jun Ma, Zhaofeng Zhuang, Song Liu, Guangmin Zhou () and Hui-Ming Cheng ()
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Guanjun Ji: Tsinghua University
Di Tang: Tsinghua University
Junxiong Wang: Tsinghua University
Zheng Liang: Shanghai Jiao Tong University
Haocheng Ji: Tsinghua University
Jun Ma: Tsinghua University
Zhaofeng Zhuang: Tsinghua University
Song Liu: Tsinghua University
Guangmin Zhou: Tsinghua University
Hui-Ming Cheng: Chinese Academy of Science

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Sustainable battery recycling is essential for achieving resource conservation and alleviating environmental issues. Many open/closed-loop strategies for critical metal recycling or direct recovery aim at a single component, and the reuse of mixed cathode materials is a significant challenge. To address this barrier, here we propose an upcycling strategy for spent LiFePO4 and Mn-rich cathodes by structural design and transition metal replacement, for which uses a green deep eutectic solvent to regenerate a high-voltage polyanionic cathode material. This process ensures the complete recycling of all the elements in mixed cathodes and the deep eutectic solvent can be reused. The regenerated LiFe0.5Mn0.5PO4 has an increased mean voltage (3.68 V versus Li/Li+) and energy density (559 Wh kg–1) compared with a commercial LiFePO4 (3.38 V and 524 Wh kg–1). The proposed upcycling strategy can expand at a gram-grade scale and was also applicable for LiFe0.5Mn0.5PO4 recovery, thus achieving a closed-loop recycling between the mixed spent cathodes and the next generation cathode materials. Techno-economic analysis shows that this strategy has potentially high environmental and economic benefits, while providing a sustainable approach for the value-added utilization of waste battery materials.

Date: 2024
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DOI: 10.1038/s41467-024-48181-9

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