Direct Regeneration of Spent LiCoO2 Black Mass Based on Fluorenone‐Mediated Lithium Supplementation and Energy‐Saving Structural Restoration

Author:

Xu Mingli1,Wu Chen1,Ye Lang1,Zhang Yuanteng2,Zhang Chenyi3,Hu Jieming1,Tan Ran1,Gu Dong2,Wang Xuanze4,Fontaine Olivier45,Zhan Chun6,Zhuang Lin1,Ai Xinping1,Qian Jiangfeng1ORCID

Affiliation:

1. Hubei Key Laboratory of Electrochemical Power Sources College of Chemistry and Molecular Sciences Wuhan University Wuhan Hubei 430072 China

2. Institute of Technological Sciences Wuhan University Wuhan Hubei 430072 China

3. The Institute for Advanced Studies Wuhan University Wuhan Hubei 430072 China

4. School of Energy Science and Engineering Vidyasirimedhi Institute of Science and Technology (VISTEC) Rayong 21210 Thailand

5. Institut Universitaire de France 103 Boulevard Saint‐Michel Paris 75005 France

6. State Key Laboratory of Advanced Metallurgy School of Metallurgical and Ecological Engineering University of Science and Technology Beijing Beijing 100083 China

Abstract

AbstractDegraded LiCoO2 cathode from retired Li‐ion batteries is urgently required to be recycled in a greener way for economic and environmental considerations. The coarse metallurgy technologies for Li/Co extraction with massive CO2 emission and energy consumption cannot satisfy the requirements of carbon neutralization. Herein, it is proposed that direct regeneration of degraded LiCoO2 cathode could be realized via 9‐fluorenone‐mediated Li supplementation and follow‐up structural restoration. The 9‐fluorenone‐lithium reagent is elaborately selected to compensate for the missing Li+ into lattice with targeted stoichiometry owing to its compatible redox potential of 1.95 V versus Li+/Li, which is located just between the reversible intercalation (3.8 V) and irreversible conversion (1.2 V) potentials of LiCoO2 electrode. Then, thermal energy‐driven structure reorganization enables Li/Co atoms to occupy the right sites, accomplishing desirable structure healing within a short annealing time of 4 h. The regenerated LiCoO2 cathode exhibits comparable Li‐storage capability to commercial LiCoO2, benefiting from the non‐destructive direct regeneration technology. In addition, the regeneration route is regarded as environmentally (0.13 kg CO2 kg−1 cell) and economically (10.07 $ kg−1 cell) superior to conventional recycling routes based on life‐cycle analysis. The precise surgery on spent LiCoO2 cathode provides a promising solution for the forthcoming retirement rush of Li‐ion batteries.

Funder

National Natural Science Foundation of China

Fundamental Research Funds for the Central Universities

Natural Science Foundation of Hubei Province

Publisher

Wiley

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