IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v11y2020i1d10.1038_s41467-020-16237-1.html
   My bibliography  Save this article

In-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution

Author

Listed:
  • Fabio Dionigi

    (Technical University Berlin)

  • Zhenhua Zeng

    (Purdue University)

  • Ilya Sinev

    (Ruhr-University Bochum
    Fritz-Haber-Institut der Max-Planck-Gesellschaft)

  • Thomas Merzdorf

    (Technical University Berlin)

  • Siddharth Deshpande

    (Purdue University)

  • Miguel Bernal Lopez

    (Ruhr-University Bochum
    Fritz-Haber-Institut der Max-Planck-Gesellschaft)

  • Sebastian Kunze

    (Ruhr-University Bochum
    Fritz-Haber-Institut der Max-Planck-Gesellschaft)

  • Ioannis Zegkinoglou

    (Ruhr-University Bochum
    Fritz-Haber-Institut der Max-Planck-Gesellschaft)

  • Hannes Sarodnik

    (Technical University Berlin)

  • Dingxin Fan

    (Purdue University)

  • Arno Bergmann

    (Technical University Berlin
    Fritz-Haber-Institut der Max-Planck-Gesellschaft)

  • Jakub Drnec

    (European Synchrotron Radiation Facility)

  • Jorge Ferreira de Araujo

    (Technical University Berlin)

  • Manuel Gliech

    (Technical University Berlin)

  • Detre Teschner

    (Fritz-Haber-Institut der Max-Planck-Gesellschaft
    Max Planck Institute for Chemical Energy Conversion)

  • Jing Zhu

    (School of Chemistry and Materials Science, University of Science and Technology of China)

  • Wei-Xue Li

    (School of Chemistry and Materials Science, University of Science and Technology of China)

  • Jeffrey Greeley

    (Purdue University)

  • Beatriz Roldan Cuenya

    (Fritz-Haber-Institut der Max-Planck-Gesellschaft)

  • Peter Strasser

    (Technical University Berlin)

Abstract

NiFe and CoFe (MFe) layered double hydroxides (LDHs) are among the most active electrocatalysts for the alkaline oxygen evolution reaction (OER). Herein, we combine electrochemical measurements, operando X-ray scattering and absorption spectroscopy, and density functional theory (DFT) calculations to elucidate the catalytically active phase, reaction center and the OER mechanism. We provide the first direct atomic-scale evidence that, under applied anodic potentials, MFe LDHs oxidize from as-prepared α-phases to activated γ-phases. The OER-active γ-phases are characterized by about 8% contraction of the lattice spacing and switching of the intercalated ions. DFT calculations reveal that the OER proceeds via a Mars van Krevelen mechanism. The flexible electronic structure of the surface Fe sites, and their synergy with nearest-neighbor M sites through formation of O-bridged Fe-M reaction centers, stabilize OER intermediates that are unfavorable on pure M-M centers and single Fe sites, fundamentally accounting for the high catalytic activity of MFe LDHs.

Suggested Citation

  • Fabio Dionigi & Zhenhua Zeng & Ilya Sinev & Thomas Merzdorf & Siddharth Deshpande & Miguel Bernal Lopez & Sebastian Kunze & Ioannis Zegkinoglou & Hannes Sarodnik & Dingxin Fan & Arno Bergmann & Jakub , 2020. "In-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-16237-1
    DOI: 10.1038/s41467-020-16237-1
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-020-16237-1
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-020-16237-1?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
    ---><---

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. Panlong Zhai & Chen Wang & Yuanyuan Zhao & Yanxue Zhang & Junfeng Gao & Licheng Sun & Jungang Hou, 2023. "Regulating electronic states of nitride/hydroxide to accelerate kinetics for oxygen evolution at large current density," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Rishi Verma & Charvi Singhvi & Amrit Venkatesh & Vivek Polshettiwar, 2024. "Defects tune the acidic strength of amorphous aluminosilicates," Nature Communications, Nature, vol. 15(1), pages 1-16, December.
    3. Yingqing Ou & Liam P. Twight & Bipasa Samanta & Lu Liu & Santu Biswas & Jessica L. Fehrs & Nicole A. Sagui & Javier Villalobos & Joaquín Morales-Santelices & Denis Antipin & Marcel Risch & Maytal Casp, 2023. "Cooperative Fe sites on transition metal (oxy)hydroxides drive high oxygen evolution activity in base," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. Chun-Kuo Peng & Yu-Chang Lin & Chao‐Lung Chiang & Zhengxin Qian & Yu-Cheng Huang & Chung-Li Dong & Jian‐Feng Li & Chien-Te Chen & Zhiwei Hu & San-Yuan Chen & Yan-Gu Lin, 2023. "Zhang-Rice singlets state formed by two-step oxidation for triggering water oxidation under operando conditions," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    5. Qianbao Wu & Junwu Liang & Mengjun Xiao & Chang Long & Lei Li & Zhenhua Zeng & Andraž Mavrič & Xia Zheng & Jing Zhu & Hai-Wei Liang & Hongfei Liu & Matjaz Valant & Wei Wang & Zhengxing Lv & Jiong Li &, 2023. "Non-covalent ligand-oxide interaction promotes oxygen evolution," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    6. Botao Zhu & Bo Dong & Feng Wang & Qifeng Yang & Yunpeng He & Cunjin Zhang & Peng Jin & Lai Feng, 2023. "Unraveling a bifunctional mechanism for methanol-to-formate electro-oxidation on nickel-based hydroxides," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    7. Zeyu Wang & William A. Goddard & Hai Xiao, 2023. "Potential-dependent transition of reaction mechanisms for oxygen evolution on layered double hydroxides," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    8. Michael High & Clemens F. Patzschke & Liya Zheng & Dewang Zeng & Oriol Gavalda-Diaz & Nan Ding & Ka Ho Horace Chien & Zili Zhang & George E. Wilson & Andrey V. Berenov & Stephen J. Skinner & Kyra L. S, 2022. "Precursor engineering of hydrotalcite-derived redox sorbents for reversible and stable thermochemical oxygen storage," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    9. Haoliang Huang & Yu-Chung Chang & Yu-Cheng Huang & Lili Li & Alexander C. Komarek & Liu Hao Tjeng & Yuki Orikasa & Chih-Wen Pao & Ting-Shan Chan & Jin-Ming Chen & Shu-Chih Haw & Jing Zhou & Yifeng Wan, 2023. "Unusual double ligand holes as catalytic active sites in LiNiO2," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    10. Jihyun Baek & Md Delowar Hossain & Pinaki Mukherjee & Junghwa Lee & Kirsten T. Winther & Juyoung Leem & Yue Jiang & William C. Chueh & Michal Bajdich & Xiaolin Zheng, 2023. "Synergistic effects of mixing and strain in high entropy spinel oxides for oxygen evolution reaction," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    11. Pushkar G. Ghanekar & Siddharth Deshpande & Jeffrey Greeley, 2022. "Adsorbate chemical environment-based machine learning framework for heterogeneous catalysis," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    12. Jie Huang & Yuyang Kang & Jianan Liu & Tingting Yao & Jianhang Qiu & Peipei Du & Biaohong Huang & Weijin Hu & Yan Liang & Tengfeng Xie & Chunlin Chen & Li-Chang Yin & Lianzhou Wang & Hui-Ming Cheng & , 2023. "Gradient tungsten-doped Bi3TiNbO9 ferroelectric photocatalysts with additional built-in electric field for efficient overall water splitting," Nature Communications, Nature, vol. 14(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:11:y:2020:i:1:d:10.1038_s41467-020-16237-1. 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.

    We have no bibliographic references for this item. You can help adding them by using 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.