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Plasmon-Enhanced Catalysis: Distinguishing Thermal and Nonthermal Effects.

Publication ,  Journal Article
Zhang, X; Li, X; Reish, ME; Zhang, D; Su, NQ; Gutiérrez, Y; Moreno, F; Yang, W; Everitt, HO; Liu, J
Published in: Nano letters
March 2018

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.

Duke Scholars

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Published In

Nano letters

DOI

EISSN

1530-6992

ISSN

1530-6984

Publication Date

March 2018

Volume

18

Issue

3

Start / End Page

1714 / 1723

Related Subject Headings

  • Nanoscience & Nanotechnology
 

Citation

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MLA
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Zhang, X., Li, X., Reish, M. E., Zhang, D., Su, N. Q., Gutiérrez, Y., … Liu, J. (2018). Plasmon-Enhanced Catalysis: Distinguishing Thermal and Nonthermal Effects. Nano Letters, 18(3), 1714–1723. https://doi.org/10.1021/acs.nanolett.7b04776
Zhang, Xiao, Xueqian Li, Matthew E. Reish, Du Zhang, Neil Qiang Su, Yael Gutiérrez, Fernando Moreno, Weitao Yang, Henry O. Everitt, and Jie Liu. “Plasmon-Enhanced Catalysis: Distinguishing Thermal and Nonthermal Effects.Nano Letters 18, no. 3 (March 2018): 1714–23. https://doi.org/10.1021/acs.nanolett.7b04776.
Zhang X, Li X, Reish ME, Zhang D, Su NQ, Gutiérrez Y, et al. Plasmon-Enhanced Catalysis: Distinguishing Thermal and Nonthermal Effects. Nano letters. 2018 Mar;18(3):1714–23.
Zhang, Xiao, et al. “Plasmon-Enhanced Catalysis: Distinguishing Thermal and Nonthermal Effects.Nano Letters, vol. 18, no. 3, Mar. 2018, pp. 1714–23. Epmc, doi:10.1021/acs.nanolett.7b04776.
Zhang X, Li X, Reish ME, Zhang D, Su NQ, Gutiérrez Y, Moreno F, Yang W, Everitt HO, Liu J. Plasmon-Enhanced Catalysis: Distinguishing Thermal and Nonthermal Effects. Nano letters. 2018 Mar;18(3):1714–1723.
Journal cover image

Published In

Nano letters

DOI

EISSN

1530-6992

ISSN

1530-6984

Publication Date

March 2018

Volume

18

Issue

3

Start / End Page

1714 / 1723

Related Subject Headings

  • Nanoscience & Nanotechnology