IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-47409-y.html
   My bibliography  Save this article

Surface oxidation/spin state determines oxygen evolution reaction activity of cobalt-based catalysts in acidic environment

Author

Listed:
  • Jinzhen Huang

    (Paul Scherrer Institute)

  • Camelia Nicoleta Borca

    (Paul Scherrer Institute)

  • Thomas Huthwelker

    (Paul Scherrer Institute)

  • Nur Sena Yüzbasi

    (Empa - Swiss Federal Laboratories for Materials Science and Technology)

  • Dominika Baster

    (Paul Scherrer Institute)

  • Mario El Kazzi

    (Paul Scherrer Institute)

  • Christof W. Schneider

    (Paul Scherrer Institute)

  • Thomas J. Schmidt

    (Paul Scherrer Institute
    ETH Zurich)

  • Emiliana Fabbri

    (Paul Scherrer Institute)

Abstract

Co-based catalysts are promising candidates to replace Ir/Ru-based oxides for oxygen evolution reaction (OER) catalysis in an acidic environment. However, both the reaction mechanism and the active species under acidic conditions remain unclear. In this study, by combining surface-sensitive soft X-ray absorption spectroscopy characterization with electrochemical analysis, we discover that the acidic OER activity of Co-based catalysts are determined by their surface oxidation/spin state. Surfaces composed of only high-spin CoII are found to be not active due to their unfavorable water dissociation to form CoIII-OH species. By contrast, the presence of low-spin CoIII is essential, as it promotes surface reconstruction of Co oxides and, hence, OER catalysis. The correlation between OER activity and Co oxidation/spin state signifies a breakthrough in defining the structure-activity relationship of Co-based catalysts for acidic OER, though, interestingly, such a relationship does not hold in alkaline and neutral environments. These findings not only help to design efficient acidic OER catalysts, but also deepen the understanding of the reaction mechanism.

Suggested Citation

  • Jinzhen Huang & Camelia Nicoleta Borca & Thomas Huthwelker & Nur Sena Yüzbasi & Dominika Baster & Mario El Kazzi & Christof W. Schneider & Thomas J. Schmidt & Emiliana Fabbri, 2024. "Surface oxidation/spin state determines oxygen evolution reaction activity of cobalt-based catalysts in acidic environment," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47409-y
    DOI: 10.1038/s41467-024-47409-y
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-47409-y
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-47409-y?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Jinzhen Huang & Hongyuan Sheng & R. Dominic Ross & Jiecai Han & Xianjie Wang & Bo Song & Song Jin, 2021. "Modifying redox properties and local bonding of Co3O4 by CeO2 enhances oxygen evolution catalysis in acid," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Hongnan Jia & Na Yao & Yiming Jin & Liqing Wu & Juan Zhu & Wei Luo, 2024. "Stabilizing atomic Ru species in conjugated sp2 carbon-linked covalent organic framework for acidic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Pengcheng Ye & Keqing Fang & Haiyan Wang & Yahao Wang & Hao Huang & Chenbin Mo & Jiqiang Ning & Yong Hu, 2024. "Lattice oxygen activation and local electric field enhancement by co-doping Fe and F in CoO nanoneedle arrays for industrial electrocatalytic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    3. Gang Zhou & Peifang Wang & Bin Hu & Xinyue Shen & Chongchong Liu & Weixiang Tao & Peilin Huang & Lizhe Liu, 2022. "Spin-related symmetry breaking induced by half-disordered hybridization in BixEr2-xRu2O7 pyrochlores for acidic oxygen evolution," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    4. Shouwei Zuo & Zhi-Peng Wu & Deting Xu & Rafia Ahmad & Lirong Zheng & Jing Zhang & Lina Zhao & Wenhuan Huang & Hassan Al Qahtani & Yu Han & Luigi Cavallo & Huabin Zhang, 2024. "Local compressive strain-induced anti-corrosion over isolated Ru-decorated Co3O4 for efficient acidic oxygen evolution," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    5. Shiyi Chen & Shishi Zhang & Lei Guo & Lun Pan & Chengxiang Shi & Xiangwen Zhang & Zhen-Feng Huang & Guidong Yang & Ji-Jun Zou, 2023. "Reconstructed Ir‒O‒Mo species with strong Brønsted acidity for acidic water oxidation," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    6. Pei Xiong & Zhihang Xu & Tai-Sing Wu & Tong Yang & Qiong Lei & Jiangtong Li & Guangchao Li & Ming Yang & Yun-Liang Soo & Robert David Bennett & Shu Ping Lau & Shik Chi Edman Tsang & Ye Zhu & Molly Men, 2024. "Synthesis of core@shell catalysts guided by Tammann temperature," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    7. Qiang Fu & Lok Wing Wong & Fangyuan Zheng & Xiaodong Zheng & Chi Shing Tsang & Ka Hei Lai & Wenqian Shen & Thuc Hue Ly & Qingming Deng & Jiong Zhao, 2023. "Unraveling and leveraging in situ surface amorphization for enhanced hydrogen evolution reaction in alkaline media," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    8. Fanpeng Cheng & Xianyun Peng & Lingzi Hu & Bin Yang & Zhongjian Li & Chung-Li Dong & Jeng-Lung Chen & Liang-Ching Hsu & Lecheng Lei & Qiang Zheng & Ming Qiu & Liming Dai & Yang Hou, 2022. "Accelerated water activation and stabilized metal-organic framework via constructing triangular active-regions for ampere-level current density hydrogen production," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47409-y. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.