IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-52499-9.html
   My bibliography  Save this article

Exploring dynamic solvation kinetics at electrocatalyst surfaces

Author

Listed:
  • Francisco Sarabia

    (Fritz-Haber Institute of the Max Planck Society)

  • Carlos Gomez Rodellar

    (Fritz-Haber Institute of the Max Planck Society)

  • Beatriz Roldan Cuenya

    (Fritz-Haber Institute of the Max Planck Society)

  • Sebastian Z. Oener

    (Fritz-Haber Institute of the Max Planck Society)

Abstract

The interface between electrocatalyst and electrolyte is highly dynamic. Even in absence of major structural changes, the intermediate coverage and interfacial solvent are bias and time dependent. This is not accounted for in current kinetic models. Here, we study the kinetics of the hydrogen evolution, ammonia oxidation and oxygen reduction reactions on polycrystalline Pt with distinct intrinsic rates and intermediates (e.g. *H, *OH, *NH2, *N). Despite these differences, we discover shared relationships between the pre-exponential factor and the activation energy that we link to solvation kinetics in the presence of electronic excess charge and charged intermediates. Further, we study dynamic changes of these kinetic parameters with a millisecond time resolution during electrosorption and double layer charging and dynamic *N and *NO poisoning. Finally, we discover a pH-dependent activation entropy that explains non-Nernstian overpotential shifts with pH. In sum, our results demonstrate the importance of accounting for a bias and time-dependent interfacial solvent and catalyst surface.

Suggested Citation

  • Francisco Sarabia & Carlos Gomez Rodellar & Beatriz Roldan Cuenya & Sebastian Z. Oener, 2024. "Exploring dynamic solvation kinetics at electrocatalyst surfaces," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-52499-9
    DOI: 10.1038/s41467-024-52499-9
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-52499-9
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-024-52499-9?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. Carlos G. Rodellar & José M. Gisbert-Gonzalez & Francisco Sarabia & Beatriz Roldan Cuenya & Sebastian Z. Oener, 2024. "Ion solvation kinetics in bipolar membranes and at electrolyte–metal interfaces," Nature Energy, Nature, vol. 9(5), pages 548-558, May.
    2. Hong Nhan Nong & Lorenz J. Falling & Arno Bergmann & Malte Klingenhof & Hoang Phi Tran & Camillo Spöri & Rik Mom & Janis Timoshenko & Guido Zichittella & Axel Knop-Gericke & Simone Piccinin & Javier P, 2020. "Key role of chemistry versus bias in electrocatalytic oxygen evolution," Nature, Nature, vol. 587(7834), pages 408-413, November.
    3. Isis Ledezma-Yanez & W. David Z. Wallace & Paula Sebastián-Pascual & Victor Climent & Juan M. Feliu & Marc T. M. Koper, 2017. "Interfacial water reorganization as a pH-dependent descriptor of the hydrogen evolution rate on platinum electrodes," Nature Energy, Nature, vol. 2(4), pages 1-7, April.
    4. Felix T. Haase & Arno Bergmann & Travis E. Jones & Janis Timoshenko & Antonia Herzog & Hyo Sang Jeon & Clara Rettenmaier & Beatriz Roldan Cuenya, 2022. "Size effects and active state formation of cobalt oxide nanoparticles during the oxygen evolution reaction," Nature Energy, Nature, vol. 7(8), pages 765-773, August.
    5. Aleksandar R. Zeradjanin, 2024. "Understanding entropic barriers," Nature Energy, Nature, vol. 9(5), pages 514-515, May.
    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. Carlos G. Rodellar & José M. Gisbert-Gonzalez & Francisco Sarabia & Beatriz Roldan Cuenya & Sebastian Z. Oener, 2024. "Ion solvation kinetics in bipolar membranes and at electrolyte–metal interfaces," Nature Energy, Nature, vol. 9(5), pages 548-558, May.
    2. Xin Zhang & Haoyin Zhong & Qi Zhang & Qihan Zhang & Chao Wu & Junchen Yu & Yifan Ma & Hang An & Hao Wang & Yiming Zou & Caozheng Diao & Jingsheng Chen & Zhi Gen Yu & Shibo Xi & Xiaopeng Wang & Junmin , 2024. "High-spin Co3+ in cobalt oxyhydroxide for efficient water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. Yixin Hao & Sung-Fu Hung & Luqi Wang & Liming Deng & Wen-Jing Zeng & Chenchen Zhang & Zih-Yi Lin & Chun-Han Kuo & Ye Wang & Ying Zhang & Han-Yi Chen & Feng Hu & Linlin Li & Shengjie Peng, 2024. "Designing neighboring-site activation of single atom via tunnel ions for boosting acidic oxygen evolution," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    4. Earl Matthew Davis & Arno Bergmann & Chao Zhan & Helmut Kuhlenbeck & Beatriz Roldan Cuenya, 2023. "Comparative study of Co3O4(111), CoFe2O4(111), and Fe3O4(111) thin film electrocatalysts for the oxygen evolution reaction," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Kai Liu & Hao Yang & Yilan Jiang & Zhaojun Liu & Shumeng Zhang & Zhixue Zhang & Zhun Qiao & Yiming Lu & Tao Cheng & Osamu Terasaki & Qing Zhang & Chuanbo Gao, 2023. "Coherent hexagonal platinum skin on nickel nanocrystals for enhanced hydrogen evolution activity," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    6. Haoyin Zhong & Qi Zhang & Junchen Yu & Xin Zhang & Chao Wu & Hang An & Yifan Ma & Hao Wang & Jun Zhang & Yong-Wei Zhang & Caozheng Diao & Zhi Gen Yu & Shibo Xi & Xiaopeng Wang & Junmin Xue, 2023. "Key role of eg* band broadening in nickel-based oxyhydroxides on coupled oxygen evolution mechanism," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    7. Felix T. Haase & Arno Bergmann & Travis E. Jones & Janis Timoshenko & Antonia Herzog & Hyo Sang Jeon & Clara Rettenmaier & Beatriz Roldan Cuenya, 2022. "Size effects and active state formation of cobalt oxide nanoparticles during the oxygen evolution reaction," Nature Energy, Nature, vol. 7(8), pages 765-773, August.
    8. Raj Pandya & Florian Dorchies & Davide Romanin & Jean-François Lemineur & Frédéric Kanoufi & Sylvain Gigan & Alex W. Chin & Hilton B. Aguiar & Alexis Grimaud, 2024. "Concurrent oxygen evolution reaction pathways revealed by high-speed compressive Raman imaging," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    9. Zhenhua Li & Xiaofan Li & Hua Zhou & Yan Xu & Si-Min Xu & Yue Ren & Yifan Yan & Jiangrong Yang & Kaiyue Ji & Li Li & Ming Xu & Mingfei Shao & Xianggui Kong & Xiaoming Sun & Haohong Duan, 2022. "Electrocatalytic synthesis of adipic acid coupled with H2 production enhanced by a ligand modification strategy," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    10. Jiaxi Zhang & Longhai Zhang & Jiamin Liu & Chengzhi Zhong & Yuanhua Tu & Peng Li & Li Du & Shengli Chen & Zhiming Cui, 2022. "OH spectator at IrMo intermetallic narrowing activity gap between alkaline and acidic hydrogen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    11. 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.
    12. Yanyan Fang & Cong Wei & Zenan Bian & Xuanwei Yin & Bo Liu & Zhaohui Liu & Peng Chi & Junxin Xiao & Wanjie Song & Shuwen Niu & Chongyang Tang & Jun Liu & Xiaolin Ge & Tongwen Xu & Gongming Wang, 2024. "Unveiling the nature of Pt-induced anti-deactivation of Ru for alkaline hydrogen oxidation reaction," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    13. Hao Tan & Bing Tang & Ying Lu & Qianqian Ji & Liyang Lv & Hengli Duan & Na Li & Yao Wang & Sihua Feng & Zhi Li & Chao Wang & Fengchun Hu & Zhihu Sun & Wensheng Yan, 2022. "Engineering a local acid-like environment in alkaline medium for efficient hydrogen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    14. Ye Tian & Botao Huang & Yizhi Song & Yirui Zhang & Dong Guan & Jiani Hong & Duanyun Cao & Enge Wang & Limei Xu & Yang Shao-Horn & Ying Jiang, 2024. "Effect of ion-specific water structures at metal surfaces on hydrogen production," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    15. Zhirong Zhang & Chuanyi Jia & Peiyu Ma & Chen Feng & Jin Yang & Junming Huang & Jiana Zheng & Ming Zuo & Mingkai Liu & Shiming Zhou & Jie Zeng, 2024. "Distance effect of single atoms on stability of cobalt oxide catalysts for acidic oxygen evolution," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    16. Sheng Zhao & Sung-Fu Hung & Liming Deng & Wen-Jing Zeng & Tian Xiao & Shaoxiong Li & Chun-Han Kuo & Han-Yi Chen & Feng Hu & Shengjie Peng, 2024. "Constructing regulable supports via non-stoichiometric engineering to stabilize ruthenium nanoparticles for enhanced pH-universal water splitting," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    17. Kui Fan & Wenfu Xie & Jinze Li & Yining Sun & Pengcheng Xu & Yang Tang & Zhenhua Li & Mingfei Shao, 2022. "Active hydrogen boosts electrochemical nitrate reduction to ammonia," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    18. Chao-Yu Li & Ming Chen & Shuai Liu & Xinyao Lu & Jinhui Meng & Jiawei Yan & Héctor D. Abruña & Guang Feng & Tianquan Lian, 2022. "Unconventional interfacial water structure of highly concentrated aqueous electrolytes at negative electrode polarizations," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    19. Jon C. Wilson & Stavros Caratzoulas & Dionisios G. Vlachos & Yushan Yan, 2023. "Insights into solvent and surface charge effects on Volmer step kinetics on Pt (111)," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    20. Zhaoping Shi & Ji Li & Yibo Wang & Shiwei Liu & Jianbing Zhu & Jiahao Yang & Xian Wang & Jing Ni & Zheng Jiang & Lijuan Zhang & Ying Wang & Changpeng Liu & Wei Xing & Junjie Ge, 2023. "Customized reaction route for ruthenium oxide towards stabilized water oxidation in high-performance PEM electrolyzers," Nature Communications, Nature, vol. 14(1), pages 1-14, 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_s41467-024-52499-9. 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.