Approaching Sustainable Lithium-Ion Batteries through Voltage-Responsive Smart Prelithiation Separator with Surface-Engineered Sacrificial Lithium Agents
Xin Chang
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
These authors contributed equally to this work.
Contribution: Investigation (lead), Writing - original draft (lead)
Search for more papers by this authorMin Fan
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
These authors contributed equally to this work.
Contribution: Investigation (equal)
Search for more papers by this authorBoheng Yuan
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
Contribution: Investigation (equal)
Search for more papers by this authorWei-Huan He
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
Contribution: Investigation (equal)
Search for more papers by this authorChao-Fan Gu
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
Contribution: Investigation (equal)
Search for more papers by this authorChen Li
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
Contribution: Investigation (equal)
Search for more papers by this authorCorresponding Author
Dr. Qinghai Meng
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Contribution: Funding acquisition (equal), Investigation (lead), Supervision (lead), Writing - review & editing (lead)
Search for more papers by this authorCorresponding Author
Prof. Yu-Guo Guo
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
Contribution: Funding acquisition (lead), Investigation (lead), Supervision (lead), Writing - review & editing (lead)
Search for more papers by this authorXin Chang
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
These authors contributed equally to this work.
Contribution: Investigation (lead), Writing - original draft (lead)
Search for more papers by this authorMin Fan
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
These authors contributed equally to this work.
Contribution: Investigation (equal)
Search for more papers by this authorBoheng Yuan
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
Contribution: Investigation (equal)
Search for more papers by this authorWei-Huan He
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
Contribution: Investigation (equal)
Search for more papers by this authorChao-Fan Gu
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
Contribution: Investigation (equal)
Search for more papers by this authorChen Li
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
Contribution: Investigation (equal)
Search for more papers by this authorCorresponding Author
Dr. Qinghai Meng
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Contribution: Funding acquisition (equal), Investigation (lead), Supervision (lead), Writing - review & editing (lead)
Search for more papers by this authorCorresponding Author
Prof. Yu-Guo Guo
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China
Contribution: Funding acquisition (lead), Investigation (lead), Supervision (lead), Writing - review & editing (lead)
Search for more papers by this authorGraphical Abstract
A smart lithium compensation strategy by introducing voltage-responsive prelithiation separator can staged release active lithium, regenerating spent lithium-ion batteries and extending their life. The separator's ability to absorb excess lithium below operating voltage protects the cathode from electrochemical failure or short circuit, enhancing safety and sustainability.
Abstract
The surge in lithium-ion batteries has heightened concerns regarding metal resource depletion and the environmental impact of spent batteries. Battery recycling has become paramount globally, but conventional techniques, while effective at extracting transition metals like cobalt and nickel from cathodes, often overlook widely used spent LiFePO4 due to its abundant and low-cost iron content. Direct regeneration, a promising approach for restoring deteriorated cathodes, is hindered by practicality and cost issues despite successful methods like solid-state sintering. Hence, a smart prelithiation separator based on surface-engineered sacrificial lithium agents is proposed. Benefiting from the synergistic anionic and cationic redox, the prelithiation separator can intelligently release or intake active lithium via voltage regulation. The staged lithium replenishment strategy was implemented, successfully restoring spent LiFePO4’s capacity to 163.7 mAh g−1 and a doubled life. Simultaneously, the separator can absorb excess active lithium up to approximately 600 mAh g−1 below 2.5 V to prevent over-lithiation of the cathode This innovative, straightforward, and cost-effective strategy paves the way for the direct regeneration of spent batteries, expanding the possibilities in the realm of lithium-ion battery recycling.
Conflict of interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
Supporting Information
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| anie202406557-sup-0001-misc_information.pdf2.7 MB | Supporting Information |
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