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Structural changes in noble metal nanoparticles during CO oxidation and their impact on catalyst activity

Author

Listed:
  • See Wee Chee

    (National University of Singapore
    National University of Singapore
    Fritz Haber Institute of the Max Planck Society)

  • Juan Manuel Arce-Ramos

    (Agency for Science, Technology and Research)

  • Wenqing Li

    (Agency for Science, Technology and Research)

  • Alexander Genest

    (Agency for Science, Technology and Research)

  • Utkur Mirsaidov

    (National University of Singapore
    National University of Singapore
    National University of Singapore
    National University of Singapore)

Abstract

The dynamical structure of a catalyst determines the availability of active sites on its surface. However, how nanoparticle (NP) catalysts re-structure under reaction conditions and how these changes associate with catalytic activity remains poorly understood. Using operando transmission electron microscopy, we show that Pd NPs exhibit reversible structural and activity changes during heating and cooling in mixed gas environments containing O2 and CO. Below 400 °C, the NPs form flat low index facets and are inactive towards CO oxidation. Above 400 °C, the NPs become rounder, and conversion of CO to CO2 increases significantly. This behavior reverses when the temperature is later reduced. Pt and Rh NPs under similar conditions do not exhibit such reversible transformations. We propose that adsorbed CO molecules suppress the activity of Pd NPs at lower temperatures by stabilizing low index facets and reducing the number of active sites. This hypothesis is supported by thermodynamic calculations.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-16027-9
    DOI: 10.1038/s41467-020-16027-9
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    Cited by:

    1. 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.
    2. 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.
    3. 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.
    4. 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.
    5. 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.

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