Journal
NANO LETTERS
Volume 18, Issue 3, Pages 1714-1723Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.7b04776
Keywords
Plasmon; photocatalyst; rhodium nanoparticle's; heterogeneous catalysis; carbon dioxide reduction
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Funding
- National Science Foundation [CHE-1565657]
- Army Research Office [W911NF-15-1-0320]
- Graduate School, Duke University
- Department of Defense (DoD) through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program
- Center for the Computational Design of Functional Layered Materials, an Energy Frontier Research Center - U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) [DE-SC0012575]
- MICINN (Spanish Ministry of Science and Innovation) [FIS2013-45854-P]
- Army Research Laboratory [W911NF-17-2-0023]
- University of Cantabria
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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 photo thermal 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 similar to 46% on a Rh/TiO2 catalyst at a surface temperature of 350 degrees 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.
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