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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
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    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. 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.
    3. 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.
    4. 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.
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