Addressing Inherent Challenges to Chemical Relithiation of Cycled End‐of‐Life Cathode Materials

Kirwa, Cyrus; Wang, Evelyna; Son, Seoung‐Bum; Preimesberger, Juliane; Key, Fulya Dogan; Bai, Yaocai; Pupek, Krzysztof; Luo, Hongmei; Keyser, Matthew; Coyle, Jaclyn

doi:10.1002/aenm.202501809

Addressing Inherent Challenges to Chemical Relithiation of Cycled End‐of‐Life Cathode Materials

Journal Article · Tue Jun 24 00:00:00 EDT 2025 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202501809· OSTI ID:2574457

Kirwa, Cyrus ^[1]; Wang, Evelyna ^[2]; Son, Seoung‐Bum ^[2]; Preimesberger, Juliane ^[3]; Key, Fulya Dogan ^[2]; ^[4]; Pupek, Krzysztof ^[2]; Luo, Hongmei ^[5]; Keyser, Matthew ^[3]; ^[3]

National Renewable Energy Laboratory (NREL), Golden, CO (United States); New Mexico State Univ., Las Cruces, NM (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
New Mexico State Univ., Las Cruces, NM (United States)

Recycling end‐of‐life (EOL) lithium‐ion batteries (LIBs) is important to retain valuable resources from critical materials present in EOL battery waste. Direct recycling methods offer an opportunity to recover intact valuable cathode materials with minimal re‐processing. An important step of the direct recycling process is relithiation which is used to restore lithium content to EOL cathode materials. However, little has been done to study how preprocessing steps such as washing or binder removal may affect relithiation methods in the direct recycling process. Here, the evolution of fluorine byproducts left over from preprocessing steps during a low‐temperature chemical redox mediator relithiation process is tracked. A facile washing step is presented as a solution for mediating adverse effects of surface contamination on the chemical relithiation performance. The structure, lithium content, and electrochemical performance of relithiated EOL NMC 622 material that underwent a pre‐relithiation washing step to remove fluorine byproducts is shown to match that of pristine NMC 622. In this work, it is showed that redox mediator relithiation as a part of a direct recycling process is a promising low energy method that can be applied to EOL material with inherent surface impurities if the proper pre‐relithiation processing steps are implemented.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 2574457

Alternate ID(s):: OSTI ID: 2574728

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials; ISSN 1614-6840; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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