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Enhancing Mechanical Resilience in Li-Ion Battery Cathodes with Nanoscale Elastic Framework Coatings

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    Enhancing Mechanical Resilience in Li-Ion Battery Cathodes with Nanoscale Elastic Framework Coatings
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    • Jong-Heon Lim
      Jong-Heon Lim
      Graduate Institute of Ferrous & Eco Materials Technology (GIFT), Pohang University of Science and Technology University, Pohang 37666, Republic of Korea
      More by Jong-Heon Lim
    • Jaehyun Kim
      Jaehyun Kim
      Department of Energy Systems Engineering, Chung-Ang University, Seoul 06974, Republic of Korea
      More by Jaehyun Kim
    • Jiwoong Oh
      Jiwoong Oh
      Graduate Institute of Ferrous & Eco Materials Technology (GIFT), Pohang University of Science and Technology University, Pohang 37666, Republic of Korea
      More by Jiwoong Oh
    • Jaesub Kwon
      Jaesub Kwon
      Department of Materials Science and Engineering (MSE), Pohang University of Science and Technology University, Pohang 37673, Republic of Korea
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    • Kyoung Eun Lee
      Kyoung Eun Lee
      Graduate Institute of Ferrous & Eco Materials Technology (GIFT), Pohang University of Science and Technology University, Pohang 37666, Republic of Korea
      More by Kyoung Eun Lee
      Orcidhttps://orcid.org/0000-0003-1110-8933
    • Youngsu Lee
      Youngsu Lee
      Graduate Institute of Ferrous & Eco Materials Technology (GIFT), Pohang University of Science and Technology University, Pohang 37666, Republic of Korea
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    • Seongeun Park
      Seongeun Park
      Graduate Institute of Ferrous & Eco Materials Technology (GIFT), Pohang University of Science and Technology University, Pohang 37666, Republic of Korea
      More by Seongeun Park
    • Jun Lim
      Jun Lim
      Pohang Accelerator Laboratory (PAL), Pohang University of Science and Technology, Pohang 37673, Republic of Korea
      More by Jun Lim
    • Dongwook Shin
      Dongwook Shin
      Materials Development Group, Samsung SDI, Samsung Future Technology Campus, 130 Samsung-ro, Yeongtong-gu, Suwon, Gyeonggi 16678, Republic of Korea
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      Orcidhttps://orcid.org/0000-0002-5660-3789
    • Changshin Jo
      Changshin Jo
      Graduate Institute of Ferrous & Eco Materials Technology (GIFT), Pohang University of Science and Technology University, Pohang 37666, Republic of Korea
      Department of Chemical Engineering, Pohang University of Science and Technology University, Pohang 37673, Republic of Korea
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    • Yong-Tae Kim
      Yong-Tae Kim
      Department of Materials Science and Engineering (MSE), Pohang University of Science and Technology University, Pohang 37673, Republic of Korea
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      Orcidhttps://orcid.org/0000-0001-9232-6558
    • Janghyuk Moon*
      Janghyuk Moon
      Department of Energy Systems Engineering, Chung-Ang University, Seoul 06974, Republic of Korea
      *E-mail: [email protected]
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      Orcidhttps://orcid.org/0000-0002-8965-1971
    • Mark C. Hersam*
      Mark C. Hersam
      Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States
      Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
      Department of Electrical and Computer Engineering, Northwestern University, Evanston, Illinois 60208, United States
      *E-mail: [email protected]
      More by Mark C. Hersam
      Orcidhttps://orcid.org/0000-0003-4120-1426
    • Kyu-Young Park*
      Kyu-Young Park
      Graduate Institute of Ferrous & Eco Materials Technology (GIFT), Pohang University of Science and Technology University, Pohang 37666, Republic of Korea
      Department of Materials Science and Engineering (MSE), Pohang University of Science and Technology University, Pohang 37673, Republic of Korea
      *E-mail: [email protected]
      More by Kyu-Young Park
      Orcidhttps://orcid.org/0000-0001-9560-8526
    Other Access OptionsSupporting Information (3)

    ACS Nano

    Cite this: ACS Nano 2025, 19, 1, 1588–1599
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c14980
    Published January 3, 2025
    Copyright © 2025 The Authors. Published by American Chemical Society
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    Abstract

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    Lattice volume changes in Li-ion batteries active materials are unavoidable during electrochemical cycling, posing significant engineering challenges from the particle to the electrode level. In this study, we present an elastic framework coating designed to absorb and reversibly release strain energy associated with particle volume changes, thereby enhancing mechanical resilience at both the particle and electrode levels. This framework, composed of multiwalled carbon nanotubes (MWCNTs), is applied to nickel-rich LiNi0.9Co0.05Mn0.05O2 (NCM9055) cathodes at a low loading of 0.5 wt %, effectively mitigating critical issues such as particle cracking, volume changes, and electrode thickness variations during cycling. Leveraging these advantages, an energy-dense electrode is achieved with a high active material loading of 20 mg cm–2, without the need for additional carbon additives. Demonstrated in a pouch cell format, this electrode achieves an exceptional capacity retention of 77.7% after 1000 cycles. This approach provides a comprehensive solution for designing Li-ion batteries capable of withstanding lattice volume variations, offering valuable insights for next-generation batteries technologies.

    Copyright © 2025 The Authors. Published by American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.4c14980.

    • Schematic illustration of supporting materials for proving the resilience effect of elastic framework; SEM images; GCD; TGA; Raman; TEM; HRPD; In situ XRD; statistical volume tracking result; simulated geometry of cathode particles; GITT; lattice parameters contracted from HRPD; simulated parameters; particle cross section images; Statistical analysis of internal microcrack, simulated result of finite element method, battery cycle life test; XANES and EXAFS; rate properties test; nano indenter test; in situ dilatometry test; XPS analysis; table of pouch cell design and cycle life (PDF)

    • Nano CT movie of bare NCM cathode after 200 cycles (MP4)

    • Nano CT movie of EF-NCM cathode after 200 cycles (MP4)

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    This article is cited by 2 publications.

    1. Sugeun Jo, Sangwoo Kim, Jun Lim. TXM-Pal : a companion software for advanced data processing in spectroscopic X-ray microscopy. Journal of Synchrotron Radiation 2025, 32 (3) , 815-822. https://doi.org/10.1107/S1600577525002036
    2. Seongeun Park, Jong-Heon Lim, Kyoung Eun Lee, Dongwook Shin, Kyu-Young Park. Water-based Pickering emulsion for concurrent washing and CNT coating of high-nickel layered lithium-ion cathodes. Chemical Engineering Journal 2025, 505 , 159376. https://doi.org/10.1016/j.cej.2025.159376
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    ACS Nano

    Cite this: ACS Nano 2025, 19, 1, 1588–1599
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c14980
    Published January 3, 2025
    Copyright © 2025 The Authors. Published by American Chemical Society
    Request reuse permissions

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