Upgrading Polycrystalline Battery Cathodes to Single-Crystal NMC622 via Morphology-Controlled Recycling

Journal Article · Tue Oct 28 00:00:00 EDT 2025 · Cell Reports Sustainablity

DOI:https://doi.org/10.1016/j.crsus.2025.100552· OSTI ID:3014840

Yu, Lu ^[1]; Bai, Yaocai ^[1]; Allen, Eva ^[2]; Liu, Jue ^[1]; Fink, Kae ^[3]; Mangum, John ^[3]; Belharouak, Ilias ^[1]

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1. Oak Ridge National Laboratory
2. Argonne National Laboratory
3. National Laboratory of the Rockies, Golden, CO (United States)

The importance of recycling lithium-ion batteries is growing within the battery supply chain as a promising answer to economic and environmental challenges. Many initiatives are in progress to improve battery recycling technologies, as existing methods encounter major obstacles. Here, we report a polyol-metallurgical recycling process to upgrade polycrystalline cathodes to single-crystal cathodes, while detailing the coprecipitation and cathode resynthesis steps. Using citric acid and ethylene glycol enables effective leaching, simple separation, and controlled coprecipitation. Leveraging the distinct poly-esterification reactions in the precipitation phase, we achieve precise control over morphology and particle sizes. Using the coprecipitates, we have successfully resynthesized a LiNi0.6Co0.2Mn0.2O2 cathode with a similar elemental composition compared to the pristine cathode, free of impurities, and exhibiting a single-crystal morphology featuring grain sizes in the range of 10 ..mu..m. The study showcases the potential of polyol metallurgy as a novel and efficient method for recycling lithium-ion batteries and synthesizing advanced cathode materials.

• Research Organization: National Laboratory of the Rockies (NLR), Golden, CO (United States)
• Sponsoring Organization: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
• DOE Contract Number: AC36-08GO28308
• OSTI ID: 3014840
• Report Number(s): NLR/JA-5K00-92658
• Journal Information: Cell Reports Sustainablity, Journal Name: Cell Reports Sustainablity
• Country of Publication: United States
• Language: English

Related Subjects

25 ENERGY STORAGE
54 ENVIRONMENTAL SCIENCES
lithium-ion batteries recycling
morphology upgradation
polyol-metallurgy
single-crystal cathode