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Title: Visible light plasmonic heating of Au-ZnO for the catalytic reduction of CO2

Abstract

Plasmonic excitation of Au nanoparticles attached to the surface of ZnO catalysts using low power 532 nm laser illumination leads to significant heating of the catalyst and the conversion of CO2 and H2 reactants to CH4 and CO products. Temperature-calibrated Raman spectra of ZnO phonons show that intensity-dependent plasmonic excitation can controllably heat Au–ZnO from 30 to ~600 °C and simultaneously tune the CH4 : CO product ratio. The laser induced heating and resulting CH4 : CO product distribution agrees well with predictions from thermodynamic models and temperature-programmed reaction experiments indicating that the reaction is a thermally driven process resulting from the plasmonic heating of the Au-ZnO. The apparent quantum yield for CO2 conversion under continuous wave (cw) 532 nm laser illumination is 0.030%. The Au-ZnO catalysts are robust and remain active after repeated laser exposure and cycling. The light intensity required to initiate CO2 reduction is low ( ~2.5 x 105 W m-2) and achievable with solar concentrators. Our results illustrate the viability of plasmonic heating approaches for CO2 utilization and other practical thermal catalytic applications.

Authors:
 [1];  [2];  [3];  [4];  [4];  [2];  [4]
  1. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States). URS Corp., South Park, PA (United States)
  2. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States); West Virginia Univ., Morgantown, WV (Unied States). Dept. of Physics
  3. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States). Univ. of Pittsburgh, PA (United States). Dept. of Chemical and Petroleum Engineering
  4. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
Publication Date:
Research Org.:
National Energy Technology Lab. (NETL), Pittsburgh, PA, and Morgantown, WV (United States). In-house Research
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1129493
Report Number(s):
A-CONTR-PUB-010
Journal ID: ISSN 2040-3364; NANOHL
Grant/Contract Number:  
FE0004000
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 5; Journal Issue: 15; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; plasmonic catalysts, photocatalysis, CO2 reduction, Au nanocrystals

Citation Formats

Wang, Congjun, Ranasingha, Oshadha, Natesakhawat, Sittichai, Ohodnicki, Paul R., Andio, Mark, Lewis, James P., and Matranga, Christopher. Visible light plasmonic heating of Au-ZnO for the catalytic reduction of CO2. United States: N. p., 2013. Web. doi:10.1039/c3nr02001k.
Wang, Congjun, Ranasingha, Oshadha, Natesakhawat, Sittichai, Ohodnicki, Paul R., Andio, Mark, Lewis, James P., & Matranga, Christopher. Visible light plasmonic heating of Au-ZnO for the catalytic reduction of CO2. United States. doi:10.1039/c3nr02001k.
Wang, Congjun, Ranasingha, Oshadha, Natesakhawat, Sittichai, Ohodnicki, Paul R., Andio, Mark, Lewis, James P., and Matranga, Christopher. Tue . "Visible light plasmonic heating of Au-ZnO for the catalytic reduction of CO2". United States. doi:10.1039/c3nr02001k. https://www.osti.gov/servlets/purl/1129493.
@article{osti_1129493,
title = {Visible light plasmonic heating of Au-ZnO for the catalytic reduction of CO2},
author = {Wang, Congjun and Ranasingha, Oshadha and Natesakhawat, Sittichai and Ohodnicki, Paul R. and Andio, Mark and Lewis, James P. and Matranga, Christopher},
abstractNote = {Plasmonic excitation of Au nanoparticles attached to the surface of ZnO catalysts using low power 532 nm laser illumination leads to significant heating of the catalyst and the conversion of CO2 and H2 reactants to CH4 and CO products. Temperature-calibrated Raman spectra of ZnO phonons show that intensity-dependent plasmonic excitation can controllably heat Au–ZnO from 30 to ~600 °C and simultaneously tune the CH4 : CO product ratio. The laser induced heating and resulting CH4 : CO product distribution agrees well with predictions from thermodynamic models and temperature-programmed reaction experiments indicating that the reaction is a thermally driven process resulting from the plasmonic heating of the Au-ZnO. The apparent quantum yield for CO2 conversion under continuous wave (cw) 532 nm laser illumination is 0.030%. The Au-ZnO catalysts are robust and remain active after repeated laser exposure and cycling. The light intensity required to initiate CO2 reduction is low ( ~2.5 x 105 W m-2) and achievable with solar concentrators. Our results illustrate the viability of plasmonic heating approaches for CO2 utilization and other practical thermal catalytic applications.},
doi = {10.1039/c3nr02001k},
journal = {Nanoscale},
number = 15,
volume = 5,
place = {United States},
year = {2013},
month = {1}
}

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