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Abstract: In plasmon-enhanced heterogeneous catalysis, illumination accelerates reaction rates by generating hot carriers and hot surfaces in the constituent nanostructured metals. In order to understand how photogenerated carriers enhance the nonthermal reaction rate, the effects of photothermal heating and thermal gradients in the catalyst bed must be confidently and quantitatively characterized. This is a challenging task considering the conflating effects of light absorption, heat transport, and reaction energetics. Here, we introduce a methodology to distinguish the thermal and nonthermal contributions from plasmon-enhanced catalysts, demonstrated by illuminated rhodium nanoparticles on oxide supports to catalyze the CO2 methanation reaction. By simultaneously measuring the total reaction rate and the temperature gradient of the catalyst bed, the effective thermal reaction rate may be extracted. The residual nonthermal rate of the plasmon-enhanced reaction is found to grow with a superlinear dependence on illumination intensity, and its apparent quantum efficiency reaches ?46% on a Rh/TiO2 catalyst at a surface temperature of 350 °C. Heat and light are shown to work synergistically in these reactions: the higher the temperature, the higher the overall nonthermal efficiency in plasmon-enhanced catalysis.
Fuente: Nano Lett. 2018, 18, 3, 1714-1723
Publisher: American Chemical Society
Year of publication: 2018
No. of pages: 10
Publication type: Article
DOI: 10.1021/acs.nanolett.7b04776
ISSN: 1530-6984,1530-6992
Publication Url: https://doi.org/10.1021/acs.nanolett.7b04776
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ZHANG, XIAO
LI, XUEQIAN
REISH, MATTHEW E.
ZHANG, DU
SU, NEIL QIANG
YAEL GUTIERREZ VELA
FERNANDO MORENO GRACIA
YANG, WEITAO
EVERITT, HENRY O.
LIU, JIE
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