Elevating Li-ion battery paradigms: Sophisticated ionic architectures in lithium-excess layered oxides for unprecedented electrochemical performance
In exploring the frontier of high-energy-density cathode materials for lithium-ion batteries, substantial progress has been made by fine-tuning the composition of Ni-rich cathodes tailored for high-capacity operation. Equally promising are Li-rich cathode materials, which leverage the novel mechanis...
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KeAi Communications Co. Ltd.
2025-07-01
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| Series: | eScience |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2667141725000060 |
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| author | Jun Ho Yu Konstantin Köster Natalia Voronina Sungkyu Kim Hyeon-Ji Shin Kyung Sun Kim Kyuwook Ihm Hyungsub Kim Hun-Gi Jung Koji Yazawa Olivier Guillon Pierluigi Gargiani Laura Simonelli Payam Kaghazchi Seung-Taek Myung |
| author_facet | Jun Ho Yu Konstantin Köster Natalia Voronina Sungkyu Kim Hyeon-Ji Shin Kyung Sun Kim Kyuwook Ihm Hyungsub Kim Hun-Gi Jung Koji Yazawa Olivier Guillon Pierluigi Gargiani Laura Simonelli Payam Kaghazchi Seung-Taek Myung |
| author_sort | Jun Ho Yu |
| collection | DOAJ |
| description | In exploring the frontier of high-energy-density cathode materials for lithium-ion batteries, substantial progress has been made by fine-tuning the composition of Ni-rich cathodes tailored for high-capacity operation. Equally promising are Li-rich cathode materials, which leverage the novel mechanism of oxygen-redox chemistry to achieve enhanced capacities. Nonetheless, the practical realization of these capacities remains elusive, falling short of the desired benchmarks. In this work, we pioneer a Mn-based, Co-free, reduced-nickel, high-capacity cathode material: Li0.75[Li0.15Ni0.15Mn0.7]O2 ionic exchanged from Na0.75[Li0.15Ni0.15Mn0.7]O2. This material is an O2-type layered structure, distinguished by honeycomb ordering within the transition-metal layer, as confirmed by comprehensive neutron and X-ray studies and extensive electrostatic screening. The material's unique structural integrity facilitates the delivery of an exceptional quantity of Li+ ions via O2−/O2n− redox, circumventing oxygen release and phase transition. The de/lithiation process enables the delivery of a substantial reversible capacity of ∼284 mAh (g-oxide)−1 (956 Wh (kg-oxide)−1). Moreover, this structural and chemical stability contributes to an acceptable cycling stability for 500 cycles in full cells, providing improved thermal stability with lower exothermic heat generation and thus highlighting the feasibility of a Mn-based, Co-free, reduced-nickel composition. This investigation marks a pivotal advancement in layered lithium cathode materials. |
| format | Article |
| id | doaj-art-a61e89ec4c664e66a7fcf890bd7b3a9d |
| institution | DOAJ |
| issn | 2667-1417 |
| language | English |
| publishDate | 2025-07-01 |
| publisher | KeAi Communications Co. Ltd. |
| record_format | Article |
| series | eScience |
| spelling | doaj-art-a61e89ec4c664e66a7fcf890bd7b3a9d2025-08-20T02:39:59ZengKeAi Communications Co. Ltd.eScience2667-14172025-07-015410037610.1016/j.esci.2025.100376Elevating Li-ion battery paradigms: Sophisticated ionic architectures in lithium-excess layered oxides for unprecedented electrochemical performanceJun Ho Yu0Konstantin Köster1Natalia Voronina2Sungkyu Kim3Hyeon-Ji Shin4Kyung Sun Kim5Kyuwook Ihm6Hyungsub Kim7Hun-Gi Jung8Koji Yazawa9Olivier Guillon10Pierluigi Gargiani11Laura Simonelli12Payam Kaghazchi13Seung-Taek Myung14Hybrid Materials Research Center, Department of Nanotechnology and Advanced Materials Engineering & Sejong Battery Institute, Sejong University, 98 Gunja-dong, Gwangjin-gu, Seoul, 05006, South KoreaInstitute of Energy Materials and Devices - Materials Synthesis and Processing (IMD-2), Forschungszentrum Jülich GmbH, 52425, Jülich, Germany; MESA+ Institute for Nanotechnology, University of Twente, 7500 AE, Enschede, the NetherlandsHybrid Materials Research Center, Department of Nanotechnology and Advanced Materials Engineering & Sejong Battery Institute, Sejong University, 98 Gunja-dong, Gwangjin-gu, Seoul, 05006, South KoreaHybrid Materials Research Center, Department of Nanotechnology and Advanced Materials Engineering & Sejong Battery Institute, Sejong University, 98 Gunja-dong, Gwangjin-gu, Seoul, 05006, South KoreaCenter for Energy Storage Research, Korea Institute of Science and Technology, Seoul, 02792, South KoreaNeutron Science Division, Korea Atomic Energy Research Institute (KAERI), 111 Daedeok-daero 989 Beon-Gil, Yuseong-gu, Daejeon, 34057, South KoreaPohang Accelerator Laboratory, 80 Jigokro-127-beongil, Nam-gu, Pohang, Gyeongbuk, 37673, South KoreaNeutron Science Division, Korea Atomic Energy Research Institute (KAERI), 111 Daedeok-daero 989 Beon-Gil, Yuseong-gu, Daejeon, 34057, South KoreaCenter for Energy Storage Research, Korea Institute of Science and Technology, Seoul, 02792, South KoreaJeol Resonance Inc, 3-1-1 Musashino, Akishima, Tokyo, 196-8558, JapanInstitute of Energy Materials and Devices - Materials Synthesis and Processing (IMD-2), Forschungszentrum Jülich GmbH, 52425, Jülich, GermanyCELLS-ALBA Synchrotron, Cerdanyola del Valles, Barcelona, E-08290, SpainCELLS-ALBA Synchrotron, Cerdanyola del Valles, Barcelona, E-08290, Spain; Corresponding authors.Institute of Energy Materials and Devices - Materials Synthesis and Processing (IMD-2), Forschungszentrum Jülich GmbH, 52425, Jülich, Germany; MESA+ Institute for Nanotechnology, University of Twente, 7500 AE, Enschede, the Netherlands; Corresponding authors.Hybrid Materials Research Center, Department of Nanotechnology and Advanced Materials Engineering & Sejong Battery Institute, Sejong University, 98 Gunja-dong, Gwangjin-gu, Seoul, 05006, South Korea; Corresponding authors.In exploring the frontier of high-energy-density cathode materials for lithium-ion batteries, substantial progress has been made by fine-tuning the composition of Ni-rich cathodes tailored for high-capacity operation. Equally promising are Li-rich cathode materials, which leverage the novel mechanism of oxygen-redox chemistry to achieve enhanced capacities. Nonetheless, the practical realization of these capacities remains elusive, falling short of the desired benchmarks. In this work, we pioneer a Mn-based, Co-free, reduced-nickel, high-capacity cathode material: Li0.75[Li0.15Ni0.15Mn0.7]O2 ionic exchanged from Na0.75[Li0.15Ni0.15Mn0.7]O2. This material is an O2-type layered structure, distinguished by honeycomb ordering within the transition-metal layer, as confirmed by comprehensive neutron and X-ray studies and extensive electrostatic screening. The material's unique structural integrity facilitates the delivery of an exceptional quantity of Li+ ions via O2−/O2n− redox, circumventing oxygen release and phase transition. The de/lithiation process enables the delivery of a substantial reversible capacity of ∼284 mAh (g-oxide)−1 (956 Wh (kg-oxide)−1). Moreover, this structural and chemical stability contributes to an acceptable cycling stability for 500 cycles in full cells, providing improved thermal stability with lower exothermic heat generation and thus highlighting the feasibility of a Mn-based, Co-free, reduced-nickel composition. This investigation marks a pivotal advancement in layered lithium cathode materials.http://www.sciencedirect.com/science/article/pii/S2667141725000060Li excessLayerCathodeLithiumBattery |
| spellingShingle | Jun Ho Yu Konstantin Köster Natalia Voronina Sungkyu Kim Hyeon-Ji Shin Kyung Sun Kim Kyuwook Ihm Hyungsub Kim Hun-Gi Jung Koji Yazawa Olivier Guillon Pierluigi Gargiani Laura Simonelli Payam Kaghazchi Seung-Taek Myung Elevating Li-ion battery paradigms: Sophisticated ionic architectures in lithium-excess layered oxides for unprecedented electrochemical performance eScience Li excess Layer Cathode Lithium Battery |
| title | Elevating Li-ion battery paradigms: Sophisticated ionic architectures in lithium-excess layered oxides for unprecedented electrochemical performance |
| title_full | Elevating Li-ion battery paradigms: Sophisticated ionic architectures in lithium-excess layered oxides for unprecedented electrochemical performance |
| title_fullStr | Elevating Li-ion battery paradigms: Sophisticated ionic architectures in lithium-excess layered oxides for unprecedented electrochemical performance |
| title_full_unstemmed | Elevating Li-ion battery paradigms: Sophisticated ionic architectures in lithium-excess layered oxides for unprecedented electrochemical performance |
| title_short | Elevating Li-ion battery paradigms: Sophisticated ionic architectures in lithium-excess layered oxides for unprecedented electrochemical performance |
| title_sort | elevating li ion battery paradigms sophisticated ionic architectures in lithium excess layered oxides for unprecedented electrochemical performance |
| topic | Li excess Layer Cathode Lithium Battery |
| url | http://www.sciencedirect.com/science/article/pii/S2667141725000060 |
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