Achieving low-temperature hydrothermal relithiation by redox mediation for direct recycling of spent lithium-ion battery cathodes

Yu, Xiaolu; Yu, Sicen; Yang, Zhenzhen; Gao, Hongpeng; Xu, Panpan; Cai, Guorui; Rose, Satchit; Brooks, Christopher; Liu, Ping; Chen, Zheng

doi:10.1016/j.ensm.2022.06.017

Achieving low-temperature hydrothermal relithiation by redox mediation for direct recycling of spent lithium-ion battery cathodes

Journal Article · Mon Jun 13 00:00:00 EDT 2022 · Energy Storage Materials

DOI:https://doi.org/10.1016/j.ensm.2022.06.017· OSTI ID:1875810

Yu, Xiaolu ^[1]; Yu, Sicen ^[1]; ^[2]; Gao, Hongpeng ^[1]; Xu, Panpan ^[1]; ^[1]; Rose, Satchit ^[1]; ^[3]; ^[1]; ^[1]

Univ. of California, San Diego, CA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Honda Development & Manufacturing of America, Raymond, OH (United States)

Lithium-ion battery (LIB) recycling is an urgent need to address the massive generation of spent LIBs from portable devices and electrical vehicles. However, the large-scale recycling is hampered by economic and safety issues associated with today's recycling processes. In this study, we demonstrate a safe and energy efficient direct regeneration process based on low-temperature hydrothermal relithiation (LTHR) at low pressure for spent LiNi_xCo_yMn_zO₂ (0 < x,y,z <1, x + y + z = 1, or NCM) cathode materials. A low concentration of low-cost redox mediator is employed to improve the relithiation kinetics of spent NCM materials, enabling full relithiation temperature to be reduced from 220 °C to 100 °C or below. Correspondingly, the pressure incurred in the relithiation process can be reduced from ~25 bar to 1 bar, offering significantly improved operation safety. Specifically, three NCM materials, including chemically delithiated NCM111, cycled (degraded) NCM111, and cycled NCM622, were successfully regenerated with complete recovery of composition, crystal structure, and electrochemical performance, achieving the same effectiveness as that achieved at high temperature process. Meanwhile, the total energy consumption of spent cell recycling and the greenhouse gas emission is also reduced. This work provides a facile and scalable way to more sustainable LIB recycling with high economic return, high operation safety and low cost.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Honda R&D Americas, Inc.; USDOE; University of California (UCSD)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1875810

Journal Information:: Energy Storage Materials, Journal Name: Energy Storage Materials Vol. 51; ISSN 2405-8297

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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