IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-41359-7.html
   My bibliography  Save this article

Synergistic effects of mixing and strain in high entropy spinel oxides for oxygen evolution reaction

Author

Listed:
  • Jihyun Baek

    (Stanford University)

  • Md Delowar Hossain

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Pinaki Mukherjee

    (Stanford University)

  • Junghwa Lee

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Kirsten T. Winther

    (SLAC National Accelerator Laboratory)

  • Juyoung Leem

    (Stanford University)

  • Yue Jiang

    (Stanford University)

  • William C. Chueh

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Michal Bajdich

    (SLAC National Accelerator Laboratory)

  • Xiaolin Zheng

    (Stanford University)

Abstract

Developing stable and efficient electrocatalysts is vital for boosting oxygen evolution reaction (OER) rates in sustainable hydrogen production. High-entropy oxides (HEOs) consist of five or more metal cations, providing opportunities to tune their catalytic properties toward high OER efficiency. This work combines theoretical and experimental studies to scrutinize the OER activity and stability for spinel-type HEOs. Density functional theory confirms that randomly mixed metal sites show thermodynamic stability, with intermediate adsorption energies displaying wider distributions due to mixing-induced equatorial strain in active metal-oxygen bonds. The rapid sol-flame method is employed to synthesize HEO, comprising five 3d-transition metal cations, which exhibits superior OER activity and durability under alkaline conditions, outperforming lower-entropy oxides, even with partial surface oxidations. The study highlights that the enhanced activity of HEO is primarily attributed to the mixing of multiple elements, leading to strain effects near the active site, as well as surface composition and coverage.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41359-7
    DOI: 10.1038/s41467-023-41359-7
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-41359-7
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-023-41359-7?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. 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.
    2. Haotian Wang & Hyun-Wook Lee & Yong Deng & Zhiyi Lu & Po-Chun Hsu & Yayuan Liu & Dingchang Lin & Yi Cui, 2015. "Bifunctional non-noble metal oxide nanoparticle electrocatalysts through lithium-induced conversion for overall water splitting," Nature Communications, Nature, vol. 6(1), pages 1-8, November.
    3. Abhishek Sarkar & Leonardo Velasco & Di Wang & Qingsong Wang & Gopichand Talasila & Lea de Biasi & Christian Kübel & Torsten Brezesinski & Subramshu S. Bhattacharya & Horst Hahn & Ben Breitung, 2018. "High entropy oxides for reversible energy storage," Nature Communications, Nature, vol. 9(1), pages 1-9, 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. 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. 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.
    3. 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.
    4. Adánez-Rubio, Iñaki & Izquierdo, María T. & Brorsson, Joakim & Mei, Daofeng & Mattisson, Tobias & Adánez, Juan, 2024. "Use of a high-entropy oxide as an oxygen carrier for chemical looping," Energy, Elsevier, vol. 298(C).
    5. 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.
    6. Bin Ouyang & Yan Zeng, 2024. "The rise of high-entropy battery materials," Nature Communications, Nature, vol. 15(1), pages 1-5, December.
    7. 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.
    8. Sishuang Tang & Minghao Xie & Saerom Yu & Xun Zhan & Ruilin Wei & Maoyu Wang & Weixin Guan & Bowen Zhang & Yuyang Wang & Hua Zhou & Gengfeng Zheng & Yuanyue Liu & Jamie H. Warner & Guihua Yu, 2024. "General synthesis of high-entropy single-atom nanocages for electrosynthesis of ammonia from nitrate," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    9. 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.
    10. Siyang Nie & Liang Wu & Qinghua Zhang & Yunwei Huang & Qingda Liu & Xun Wang, 2024. "High-entropy-perovskite subnanowires for photoelectrocatalytic coupling of methane to acetic acid," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    11. Mengyuan Zhang & Ying Gao & Chengmin Xie & Xiaolan Duan & Xiaoyan Lu & Kongliang Luo & Jian Ye & Xiaopeng Wang & Xinhua Gao & Qiang Niu & Pengfei Zhang & Sheng Dai, 2024. "Designing water resistant high entropy oxide materials," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    12. 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.
    13. Jose Antonio Garrido Torres & Vahe Gharakhanyan & Nongnuch Artrith & Tobias Hoffmann Eegholm & Alexander Urban, 2021. "Augmenting zero-Kelvin quantum mechanics with machine learning for the prediction of chemical reactions at high temperatures," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    14. Yanzhi Wang & Hangjuan He & Hao Lv & Fengrui Jia & Ben Liu, 2024. "Two-dimensional single-crystalline mesoporous high-entropy oxide nanoplates for efficient electrochemical biomass upgrading," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    15. Mengyun Hou & Lirong Zheng & Di Zhao & Xin Tan & Wuyi Feng & Jiantao Fu & Tianxin Wei & Minhua Cao & Jiatao Zhang & Chen Chen, 2024. "Microenvironment reconstitution of highly active Ni single atoms on oxygen-incorporated Mo2C for water splitting," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    16. Wei Chen & Antoine Hilhorst & Georgios Bokas & Stéphane Gorsse & Pascal J. Jacques & Geoffroy Hautier, 2023. "A map of single-phase high-entropy alloys," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    17. 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.
    18. Lei Su & Huaixun Huyan & Abhishek Sarkar & Wenpei Gao & Xingxu Yan & Christopher Addiego & Robert Kruk & Horst Hahn & Xiaoqing Pan, 2022. "Direct observation of elemental fluctuation and oxygen octahedral distortion-dependent charge distribution in high entropy oxides," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    19. 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.
    20. Yixiu Luo & Luchao Sun & Jiemin Wang & Tiefeng Du & Cui Zhou & Jie Zhang & Jingyang Wang, 2023. "Phase formation capability and compositional design of β-phase multiple rare-earth principal component disilicates," Nature Communications, Nature, vol. 14(1), pages 1-13, 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:14:y:2023:i:1:d:10.1038_s41467-023-41359-7. 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.