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A Universal Molten Salt Method for Direct Upcycling of Spent Ni-rich Cathode towards Single-crystalline Li-rich Cathode
Authors:Zuoyu Qin  Dr Ying Zhang  Wuqing Luo  Tao Zhang  Tao Wang  Lianshan Ni  Haoji Wang  Prof Ning Zhang  Prof Xiaohe Liu  Jiang Zhou  Prof Gen Chen
Institution:1. School of Materials Science and Engineering, Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials, Central South University, 410083 Changsha, Hunan, P. R. China

Contribution: Conceptualization (equal), Data curation (lead), Formal analysis (lead), ​Investigation (equal), Writing - original draft (lead);2. Zhongyuan Critical Metals Laboratory and School of Chemical Engineering, Zhengzhou University, 450001 Zhengzhou, Henan, P. R. China

Contribution: ​Investigation (supporting), Visualization (lead), Writing - review & editing (equal);3. School of Materials Science and Engineering, Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials, Central South University, 410083 Changsha, Hunan, P. R. China

Contribution: Validation (lead);4. School of Materials Science and Engineering, Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials, Central South University, 410083 Changsha, Hunan, P. R. China

Contribution: ​Investigation (supporting), Resources (lead), Visualization (supporting);5. School of Metallurgy and Environment, Central South University, 410083 Changsha, Hunan, P. R. China

Contribution: ​Investigation (supporting), Writing - review & editing (supporting);6. College of Chemistry and Chemical Engineering, Central South University, 410083 Changsha, Hunan, P. R. China

Contribution: Formal analysis (supporting), ​Investigation (supporting);7. College of Chemistry and Chemical Engineering, Central South University, 410083 Changsha, Hunan, P. R. China

Contribution: Validation (supporting), Writing - review & editing (supporting);8. School of Materials Science and Engineering, Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials, Central South University, 410083 Changsha, Hunan, P. R. China

Contribution: Methodology (supporting), Writing - review & editing (supporting);9. Zhongyuan Critical Metals Laboratory and School of Chemical Engineering, Zhengzhou University, 450001 Zhengzhou, Henan, P. R. China

Contribution: Project administration (supporting), Writing - review & editing (supporting);10. School of Materials Science and Engineering, Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials, Central South University, 410083 Changsha, Hunan, P. R. China

Abstract:With ever-increasing pursuit for high-value output in recycling spent lithium-ion batteries (LIBs), traditional recycling methods of cathodes tend to be obsolete because of the complicated procedures. Herein, we first upcycle spent polycrystal LiNi0.88Co0.095Al0.025O2 (S-NCA) to high value-added single-crystalline and Li-rich cathode materials through a simple but feasible LiOH-Na2SO4 eutectic molten salt strategy. The in situ X-ray diffraction technique and a series of paratactic experiments record the evolution process of upcycling and prove that excessive Li occupies the transition metal (TM) layers. Beneficial from the single-crystalline and Li-rich nature, the regenerated NCA (R-NCA) exhibits remarkably enhanced electrochemical performances in terms of long-term cyclability, high-rate performance and low polarization. This approach can also be successfully extended to other cathode materials e.g., LiNixCoyMnzO2 (NCM) and mixed spent NCAs with varied degree of Li loss.
Keywords:Li-Rich Cathode  Single-Crystalline  Spent LiNi0  88Co0  095Al0  025O2  Upcycling
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