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Stroboscopic operando spectroscopy of the dynamics in heterogeneous catalysis by event-averaging

Author

Listed:
  • Jan Knudsen

    (Lund University
    Lund University)

  • Tamires Gallo

    (Lund University)

  • Virgínia Boix

    (Lund University)

  • Marie Døvre Strømsheim

    (Norwegian University of Science and Technology (NTNU))

  • Giulio D’Acunto

    (Lund University)

  • Christopher Goodwin

    (Stockholm University)

  • Harald Wallander

    (Lund University)

  • Suyun Zhu

    (Lund University)

  • Markus Soldemo

    (Stockholm University)

  • Patrick Lömker

    (Deutsches Elektronen-Synchrotron DESY)

  • Filippo Cavalca

    (Lund University)

  • Mattia Scardamaglia

    (Lund University)

  • David Degerman

    (Stockholm University)

  • Anders Nilsson

    (Stockholm University)

  • Peter Amann

    (Stockholm University)

  • Andrey Shavorskiy

    (Lund University)

  • Joachim Schnadt

    (Lund University
    Lund University)

Abstract

Heterogeneous catalyst surfaces are dynamic entities that respond rapidly to changes in their local gas environment, and the dynamics of the response is a decisive factor for the catalysts’ action and activity. Few probes are able to map catalyst structure and local gas environment simultaneously under reaction conditions at the timescales of the dynamic changes. Here we use the CO oxidation reaction and a Pd(100) model catalyst to demonstrate how such studies can be performed by time-resolved ambient pressure photoelectron spectroscopy. Central elements of the method are cyclic gas pulsing and software-based event-averaging by image recognition of spectral features. A key finding is that at 3.2 mbar total pressure a metallic, predominantly CO-covered metallic surface turns highly active for a few seconds once the O2:CO ratio becomes high enough to lift the CO poisoning effect before mass transport limitations triggers formation of a √5 oxide.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26372-y
    DOI: 10.1038/s41467-021-26372-y
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    References listed on IDEAS

    as
    1. Johan Zetterberg & Sara Blomberg & Johan Gustafson & Jonas Evertsson & Jianfeng Zhou & Emma C. Adams & Per-Anders Carlsson & Marcus Aldén & Edvin Lundgren, 2015. "Spatially and temporally resolved gas distributions around heterogeneous catalysts using infrared planar laser-induced fluorescence," Nature Communications, Nature, vol. 6(1), pages 1-8, November.
    2. Matthijs A. Spronsen & Joost W. M. Frenken & Irene M. N. Groot, 2017. "Observing the oxidation of platinum," Nature Communications, Nature, vol. 8(1), pages 1-7, December.
    3. Uta Hejral & Patrick Müller & Olivier Balmes & Diego Pontoni & Andreas Stierle, 2016. "Tracking the shape-dependent sintering of platinum–rhodium model catalysts under operando conditions," Nature Communications, Nature, vol. 7(1), pages 1-8, April.
    4. Jing Cao & Ali Rinaldi & Milivoj Plodinec & Xing Huang & Elena Willinger & Adnan Hammud & Stefan Hieke & Sebastian Beeg & Luca Gregoratti & Claudiu Colbea & Robert Schlögl & Markus Antonietti & Mark G, 2020. "In situ observation of oscillatory redox dynamics of copper," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
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    Cited by:

    1. 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.

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