Abstract
Spent lithium-ion batteries (LIBs) provide a valuable source of critical metals for cathode material production. However, the prevalent recycling technologies focus on processing only one type of spent cathode material, demanding high energy input and significant chemical consumption, which raises both environmental and economic concerns. Here, we propose a complementary redox-mediated recycling strategy for multiple types of spent cathode materials using a redox-targeting flow cell design. In this system, spent LiFePO4 and layered oxide cathode materials serve as the anodic and cathodic feedstocks, respectively. Coupled redox-mediated oxidative and reductive leaching simultaneously generates electricity (theoretically 246 MWh per annum for 10,000 tonnes of black mass) while driving lithium-ion migration into the catholyte. Leaching efficiencies of critical metals exceed 95% for both materials, accompanied by a calculated carbon dioxide capture rate of 1,066 tonnes per annum. By integrating hydrogen looping for base and acid regeneration, the system operates over a closed loop without net chemical consumption. This strategy shows potential greater environmental and economic benefits compared with the traditional hydrometallurgical method based on techno-economic analysis, potentially offering a sustainable approach to LIBs recycling.
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All the data generated in this study are provided in this paper and its Supplementary Information file. Source data are provided with this paper.
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Acknowledgements
This research is supported by the National Research Foundation, Singapore, under its Competitive Research Programme (Award No.: NRF-CRP26-2021-0003 (Q.W.)), and by A*STAR under its MTC Programmatic Fund (Award No.: M24N5b0037 (Q.W.)).
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Q.W., S.Q.H. and S.P.H. conceived the study. Q.W. supervised the work. S.Q.H. performed most of the experiments and data analysis. S.P.H. did preliminary tests. M.L. assisted with battery tests and granule synthesis. H.Z. conducted DFT calculations. X.W. advised on techno-economic analysis. M.S. conducted the NMR tests. S.Q.H. and Q.W. wrote the paper.
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Huang, S., Huang, S., Li, M. et al. Self-driven recycling of spent Li-ion battery materials with electricity generation. Nat Commun (2026). https://doi.org/10.1038/s41467-026-69868-1
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DOI: https://doi.org/10.1038/s41467-026-69868-1
