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In-situ observation of plasmon-controlled photocatalytic dehydrogenation of individual palladium nanoparticles

Author

Listed:
  • Michal Vadai

    (Stanford University)

  • Daniel K. Angell

    (Stanford University)

  • Fariah Hayee

    (Stanford University)

  • Katherine Sytwu

    (Stanford University)

  • Jennifer A. Dionne

    (Stanford University)

Abstract

Plasmonic nanoparticle catalysts offer improved light absorption and carrier transport compared to traditional photocatalysts. However, it remains unclear how plasmonic excitation affects multi-step reaction kinetics and promotes site-selectivity. Here, we visualize a plasmon-induced reaction at the sub-nanoparticle level in-situ and in real-time. Using an environmental transmission electron microscope combined with light excitation, we study the photocatalytic dehydrogenation of individual palladium nanocubes coupled to gold nanoparticles with sub-2 nanometer spatial resolution. We find that plasmons increase the rate of distinct reaction steps with unique time constants; enable reaction nucleation at specific sites closest to the electromagnetic hot spots; and appear to open a new reaction pathway that is not observed without illumination. These effects are explained by plasmon-mediated population of excited-state hybridized palladium-hydrogen orbitals. Our results help elucidate the role of plasmons in light-driven photochemical transformations, en-route to design of site-selective and product-specific photocatalysts.

Suggested Citation

  • Michal Vadai & Daniel K. Angell & Fariah Hayee & Katherine Sytwu & Jennifer A. Dionne, 2018. "In-situ observation of plasmon-controlled photocatalytic dehydrogenation of individual palladium nanoparticles," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-07108-x
    DOI: 10.1038/s41467-018-07108-x
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    Cited by:

    1. Ananta Dey & Amal Mendalz & Anna Wach & Robert Bericat Vadell & Vitor R. Silveira & Paul Maurice Leidinger & Thomas Huthwelker & Vitalii Shtender & Zbynek Novotny & Luca Artiglia & Jacinto Sá, 2024. "Hydrogen evolution with hot electrons on a plasmonic-molecular catalyst hybrid system," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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