IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-51068-4.html
   My bibliography  Save this article

Restructuring dynamics of surface species in bimetallic nanoparticles probed by modulation excitation spectroscopy

Author

Listed:
  • Prahlad K. Routh

    (Stony Brook University)

  • Evgeniy Redekop

    (University of Oslo)

  • Sebastian Prodinger

    (University of Oslo)

  • Jessi E. S. Hoeven

    (Utrecht University)

  • Kang Rui Garrick Lim

    (Harvard University
    Harvard University)

  • Joanna Aizenberg

    (Harvard University
    Harvard University)

  • Maarten Nachtegaal

    (Paul Scherrer Institut (PSI))

  • Adam H. Clark

    (Paul Scherrer Institut (PSI))

  • Anatoly I. Frenkel

    (Stony Brook University
    Brookhaven National Laboratory)

Abstract

Restructuring of metal components on bimetallic nanoparticle surfaces in response to the changes in reactive environment is a ubiquitous phenomenon whose potential for the design of tunable catalysts is underexplored. The main challenge is the lack of knowledge of the structure, composition, and evolution of species on the nanoparticle surfaces during reaction. We apply a modulation excitation approach to the X-ray absorption spectroscopy of the 30 atomic % Pd in Au supported nanocatalysts via the gas (H2 and O2) concentration modulation. For interpreting restructuring kinetics, we correlate the phase-sensitive detection with the time-domain analysis aided by a denoising algorithm. Here we show that the surface and near-surface species such as Pd oxides and atomically dispersed Pd restructured periodically, featuring different time delays. We propose a model that Pd oxide formation is preceded by the build-up of Pd regions caused by oxygen-driven segregation of Pd atoms towards the surface. During the H2 pulse, rapid reduction and dissolution of Pd follows an induction period which we attribute to H2 dissociation. Periodic perturbations of nanocatalysts by gases can, therefore, enable variations in the stoichiometry of the surface and near-surface oxides and dynamically tune the degree of oxidation/reduction of metals at/near the catalyst surface.

Suggested Citation

  • Prahlad K. Routh & Evgeniy Redekop & Sebastian Prodinger & Jessi E. S. Hoeven & Kang Rui Garrick Lim & Joanna Aizenberg & Maarten Nachtegaal & Adam H. Clark & Anatoly I. Frenkel, 2024. "Restructuring dynamics of surface species in bimetallic nanoparticles probed by modulation excitation spectroscopy," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-51068-4
    DOI: 10.1038/s41467-024-51068-4
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-51068-4
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-51068-4?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. Jan Knudsen & Tamires Gallo & Virgínia Boix & Marie Døvre Strømsheim & Giulio D’Acunto & Christopher Goodwin & Harald Wallander & Suyun Zhu & Markus Soldemo & Patrick Lömker & Filippo Cavalca & Mattia, 2021. "Stroboscopic operando spectroscopy of the dynamics in heterogeneous catalysis by event-averaging," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    2. See Wee Chee & Juan Manuel Arce-Ramos & Wenqing Li & Alexander Genest & Utkur Mirsaidov, 2020. "Structural changes in noble metal nanoparticles during CO oxidation and their impact on catalyst activity," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    3. Nicholas Marcella & Jin Soo Lim & Anna M. Płonka & George Yan & Cameron J. Owen & Jessi E. S. Hoeven & Alexandre C. Foucher & Hio Tong Ngan & Steven B. Torrisi & Nebojsa S. Marinkovic & Eric A. Stach , 2022. "Decoding reactive structures in dilute alloy catalysts," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    4. Charlotte Vogt & Florian Meirer & Matteo Monai & Esther Groeneveld & Davide Ferri & Rutger A. Santen & Maarten Nachtegaal & Raymond R. Unocic & Anatoly I. Frenkel & Bert M. Weckhuysen, 2021. "Dynamic restructuring of supported metal nanoparticles and its implications for structure insensitive catalysis," Nature Communications, Nature, vol. 12(1), pages 1-10, 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. Taek-Seung Kim & Christopher R. O’Connor & Christian Reece, 2024. "Interrogating site dependent kinetics over SiO2-supported Pt nanoparticles," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Yan, Xianyao & Duan, Chenyu & Yu, Shuihua & Dai, Bing & Sun, Chaoying & Chu, Huaqiang, 2024. "Recent advances on CO2 reduction reactions using single-atom catalysts," Renewable and Sustainable Energy Reviews, Elsevier, vol. 190(PB).
    3. Tanmay Ghosh & Juan Manuel Arce-Ramos & Wen-Qing Li & Hongwei Yan & See Wee Chee & Alexander Genest & Utkur Mirsaidov, 2022. "Periodic structural changes in Pd nanoparticles during oscillatory CO oxidation reaction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    4. Cameron J. Owen & Yu Xie & Anders Johansson & Lixin Sun & Boris Kozinsky, 2024. "Low-index mesoscopic surface reconstructions of Au surfaces using Bayesian force fields," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    5. Gonglei Shao & Changfei Jing & Zhinan Ma & Yuanyuan Li & Weiqi Dang & Dong Guo & Manman Wu & Song Liu & Xu Zhang & Kun He & Yifei Yuan & Jun Luo & Sheng Dai & Jie Xu & Zhen Zhou, 2024. "Dynamic coordination engineering of 2D PhenPtCl2 nanosheets for superior hydrogen evolution," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    6. Shengnan Yue & C. S. Praveen & Alexander Klyushin & Alexey Fedorov & Masahiro Hashimoto & Qian Li & Travis Jones & Panpan Liu & Wenqian Yu & Marc-Georg Willinger & Xing Huang, 2024. "Redox dynamics and surface structures of an active palladium catalyst during methane oxidation," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    7. Alexander Genest & Joaquín Silvestre-Albero & Wen-Qing Li & Notker Rösch & Günther Rupprechter, 2021. "The origin of the particle-size-dependent selectivity in 1-butene isomerization and hydrogenation on Pd/Al2O3 catalysts," Nature Communications, Nature, vol. 12(1), pages 1-8, 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_s41467-024-51068-4. 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.