Upgrading polycrystalline battery cathodes to single-crystal NMC622 via morphology-controlled recycling

Lu Yu; Yaocai Bai; Eva Allen; Jue Liu; Kae Fink; John Mangum; Ilias Belharouak

doi:10.1016/j.crsus.2025.100552

Upgrading polycrystalline battery cathodes to single-crystal NMC622 via morphology-controlled recycling

Lu Yu
, Yaocai Bai
, Eva Allen
, Jue Liu
, Kae Fink
, John Mangum
, Ilias Belharouak

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

Abstract

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 LiNi_0.6Co_0.2Mn_0.2O₂ 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 μm. The study showcases the potential of polyol metallurgy as a novel and efficient method for recycling lithium-ion batteries and synthesizing advanced cathode materials.

Original language	English
Article number	100552
Journal	Cell Reports Sustainability
Volume	3
Issue number	1
DOIs	https://doi.org/10.1016/j.crsus.2025.100552
State	Published - Jan 23 2026

Funding

Notice: This manuscript has been authored by UT-Battelle, LLC , under contract no. DE-AC05-00OR22725 with the US DOE . The US government retains, and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). This work was sponsored by the Office of Energy Efficiency and Renewable Energy's Vehicle Technologies Office through the ReCell Center for Advanced Battery Recycling, DOE-VTO program managers (Tina Chen and Stephanie Spence). Research was conducted at the Oak Ridge National Laboratory (ORNL), managed by UT Battelle, LLC, for the US Department of Energy under contract no. DE-AC05-00OR22725. This research used resources 18ID FXI of the National Synchrotron Light Source II, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. The neutron diffraction characterization was conducted at the NOMAD beamlines at ORNL's Spallation Neutron Source, which was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, US Department of Energy. EBSD characterization was conducted at the National Renewable Energy Laboratory (NREL), which is managed and operated by the Alliance for Sustainable Energy, LLC under contract no. DE-AC36-08GO28308.Notice: This manuscript has been authored by UT-Battelle, LLC, under contract no. DE-AC05-00OR22725 with the US DOE. The US government retains, and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This work was sponsored by the Office of Energy Efficiency and Renewable Energy’s Vehicle Technologies Office through the ReCell Center for Advanced Battery Recycling , DOE-VTO program managers (Tina Chen and Stephanie Spence). Research was conducted at the Oak Ridge National Laboratory (ORNL), managed by UT Battelle, LLC, for the US Department of Energy under contract no. DE-AC05-00OR22725 . This research used resources 18ID FXI of the National Synchrotron Light Source II, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704 . The neutron diffraction characterization was conducted at the NOMAD beamlines at ORNL’s Spallation Neutron Source, which was sponsored by the Scientific User Facilities Division, Office of Basic Sciences , US Department of Energy . EBSD characterization was conducted at the National Renewable Energy Laboratory (NREL) , which is managed and operated by the Alliance for Sustainable Energy, LLC under contract no. DE-AC36-08GO28308 .

Keywords

critical materials
lithium-ion batteries
morphology upgrade
polyol-metallurgy
recycling
single-crystal cathode
supply chain

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10.1016/j.crsus.2025.100552

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title = "Upgrading polycrystalline battery cathodes to single-crystal NMC622 via morphology-controlled recycling",

abstract = "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 μm. The study showcases the potential of polyol metallurgy as a novel and efficient method for recycling lithium-ion batteries and synthesizing advanced cathode materials.",

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AU - Bai, Yaocai

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AU - Liu, Jue

AU - Fink, Kae

AU - Mangum, John

AU - Belharouak, Ilias

PY - 2026/1/23

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N2 - 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 μm. The study showcases the potential of polyol metallurgy as a novel and efficient method for recycling lithium-ion batteries and synthesizing advanced cathode materials.

AB - 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 μm. The study showcases the potential of polyol metallurgy as a novel and efficient method for recycling lithium-ion batteries and synthesizing advanced cathode materials.

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Upgrading polycrystalline battery cathodes to single-crystal NMC622 via morphology-controlled recycling

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Keywords

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