Flux upcycling of spent NMC 111 to nickel-rich NMC cathodes in reciprocal ternary molten salts

Tao Wang; Huimin Luo; Juntian Fan; Bishnu P. Thapaliya; Yaocai Bai; Ilias Belharouak; Sheng Dai

doi:10.1016/j.isci.2022.103801

Flux upcycling of spent NMC 111 to nickel-rich NMC cathodes in reciprocal ternary molten salts

Tao Wang, Huimin Luo, Juntian Fan, Bishnu P. Thapaliya, Yaocai Bai, Ilias Belharouak, Sheng Dai

Research output: Contribution to journal › Article › peer-review

40 Scopus citations

Abstract

The proper handling of end-of-life (EOL) lithium-ion batteries (LIBs) has become an urgent and challenging issue with the surging use of LIBs, in which recovering high-value cathodes not only relieves the pressure on the raw material supply chain but also minimizes environmental pollution. Beyond direct recycling of spent cathodes to their pristine states, the direct upcycling of spent cathodes to the next-generation cathodes is of great significance to maximize the value of spent materials and to sustain the fast development of LIBs. Herein, a “reciprocal ternary molten salts” (RTMS) system was developed to directly upcycle spent NMC 111 to Ni-rich NMCs by simultaneously realizing the addition of Ni and the relithiation of Li in spent NMC 111. After RTMS flux upcycling, the obtained Ni-rich NMCs exhibited an α-NaFeO₂-type layered structure, restored Li content, and excellent performance, which is very similar to that of the pristine NMC 622.

Original language	English
Article number	103801
Journal	iScience
Volume	25
Issue number	2
DOIs	https://doi.org/10.1016/j.isci.2022.103801
State	Published - Feb 18 2022

Funding

This research was performed through the Re-Cell Center, which gratefully acknowledges support from the U. S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy , and the Vehicle Technologies Office . The authors thank Dr. Kris Pupek, Dr. Erik Dahl, and Dr. Bryant Polzin from Argonne National Laboratory for providing pristine and delithiated NMC 111. This manuscript was authored by UT-Battelle, LLC under Contract No. DEAC05-00OR22725 with the U.S. Department of Energy. This article has been contributed to by US Government employees and their work is in the public domain in the USA. The Department of Energy will provide public access to these results of federally sponsored research by the DOE Public Access Plan. This research was performed through the Re-Cell Center, which gratefully acknowledges support from the U. S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, and the Vehicle Technologies Office. The authors thank Dr. Kris Pupek, Dr. Erik Dahl, and Dr. Bryant Polzin from Argonne National Laboratory for providing pristine and delithiated NMC 111. This manuscript was authored by UT-Battelle, LLC under Contract No. DEAC05-00OR22725 with the U.S. Department of Energy. This article has been contributed to by US Government employees and their work is in the public domain in the USA. The Department of Energy will provide public access to these results of federally sponsored research by the DOE Public Access Plan. Conceptualization, SD; Methodology, T.W.; Investigation, T.W.; Writing – Original Draft, T.W.; Writing – Review & Editing, T.W. H. L. and SD; Funding Acquisition, H.L. and SD; Resources, B.P.T. Y.B. J.F. I. B. and H.L.; Supervision, SD, The authors declare no competing interests.

Funders	Funder number
U.S. Department of Energy
Office of Energy Efficiency and Renewable Energy	DEAC05-00OR22725
Argonne National Laboratory

Keywords

Electrochemical energy storage
Energy materials
Materials application
Mechanical engineering

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.isci.2022.103801

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title = "Flux upcycling of spent NMC 111 to nickel-rich NMC cathodes in reciprocal ternary molten salts",

abstract = "The proper handling of end-of-life (EOL) lithium-ion batteries (LIBs) has become an urgent and challenging issue with the surging use of LIBs, in which recovering high-value cathodes not only relieves the pressure on the raw material supply chain but also minimizes environmental pollution. Beyond direct recycling of spent cathodes to their pristine states, the direct upcycling of spent cathodes to the next-generation cathodes is of great significance to maximize the value of spent materials and to sustain the fast development of LIBs. Herein, a “reciprocal ternary molten salts” (RTMS) system was developed to directly upcycle spent NMC 111 to Ni-rich NMCs by simultaneously realizing the addition of Ni and the relithiation of Li in spent NMC 111. After RTMS flux upcycling, the obtained Ni-rich NMCs exhibited an α-NaFeO2-type layered structure, restored Li content, and excellent performance, which is very similar to that of the pristine NMC 622.",

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AU - Bai, Yaocai

AU - Belharouak, Ilias

AU - Dai, Sheng

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N2 - The proper handling of end-of-life (EOL) lithium-ion batteries (LIBs) has become an urgent and challenging issue with the surging use of LIBs, in which recovering high-value cathodes not only relieves the pressure on the raw material supply chain but also minimizes environmental pollution. Beyond direct recycling of spent cathodes to their pristine states, the direct upcycling of spent cathodes to the next-generation cathodes is of great significance to maximize the value of spent materials and to sustain the fast development of LIBs. Herein, a “reciprocal ternary molten salts” (RTMS) system was developed to directly upcycle spent NMC 111 to Ni-rich NMCs by simultaneously realizing the addition of Ni and the relithiation of Li in spent NMC 111. After RTMS flux upcycling, the obtained Ni-rich NMCs exhibited an α-NaFeO2-type layered structure, restored Li content, and excellent performance, which is very similar to that of the pristine NMC 622.

AB - The proper handling of end-of-life (EOL) lithium-ion batteries (LIBs) has become an urgent and challenging issue with the surging use of LIBs, in which recovering high-value cathodes not only relieves the pressure on the raw material supply chain but also minimizes environmental pollution. Beyond direct recycling of spent cathodes to their pristine states, the direct upcycling of spent cathodes to the next-generation cathodes is of great significance to maximize the value of spent materials and to sustain the fast development of LIBs. Herein, a “reciprocal ternary molten salts” (RTMS) system was developed to directly upcycle spent NMC 111 to Ni-rich NMCs by simultaneously realizing the addition of Ni and the relithiation of Li in spent NMC 111. After RTMS flux upcycling, the obtained Ni-rich NMCs exhibited an α-NaFeO2-type layered structure, restored Li content, and excellent performance, which is very similar to that of the pristine NMC 622.

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Flux upcycling of spent NMC 111 to nickel-rich NMC cathodes in reciprocal ternary molten salts

Abstract

Funding

Keywords

UN SDGs

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