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Plasmon-Enhanced Catalysis: Distinguishing Thermal and Nonthermal Effects

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

Editorial: American Chemical Society

 Año de publicación: 2018

Nº de páginas: 10

Tipo de publicación: Artículo de Revista

 DOI: 10.1021/acs.nanolett.7b04776

ISSN: 1530-6984,1530-6992

Url de la publicación: https://doi.org/10.1021/acs.nanolett.7b04776

Autores/as

ZHANG, XIAO

LI, XUEQIAN

REISH, MATTHEW E.

ZHANG, DU

SU, NEIL QIANG

YAEL GUTIERREZ VELA

YANG, WEITAO

EVERITT, HENRY O.

LIU, JIE