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

Michal Vadai (), Daniel K. Angell, Fariah Hayee, Katherine Sytwu and Jennifer A. Dionne ()
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Michal Vadai: Stanford University
Daniel K. Angell: Stanford University
Fariah Hayee: Stanford University
Katherine Sytwu: Stanford University
Jennifer A. Dionne: Stanford University

Nature Communications, 2018, vol. 9, issue 1, 1-8

Abstract: 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.

Date: 2018
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DOI: 10.1038/s41467-018-07108-x

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