Light-Enhanced Carbon Dioxide Activation and Conversion by Effective Plasmonic Coupling Effect of Pt and Au Nanoparticles

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Abstract
Photocatalytic reduction of carbon dioxide (CO2) is attractive for the production of valuable fuels and mitigating the influence of greenhouse gas emission. However, the extreme inertness of CO2 and the sluggish kinetics of photo-excited charge carrires transfer process greatly limit the conversion efficiency of CO2 photoreduction. Herein, we report that the plasmonic coupling effect of Pt and Au nanoparticles (NPs) profoundly enhance the efficiency of CO2 reduction through dry reforming of methane reaction assisted by light illumination, reducing activation energies for CO2 reduction ~30% below thermal activation energies and achieving a reaction rate 2.4 times higher than that of the thermocatalytic reaction. UV-vis absorption spectra and wavelength-dependent performances show that not only UV but also visible light play important roles in promoting CO2 reduction due to effective local surface plasmon resonances (LSPR) coupling between Pt and Au NPs. Finite-difference time-domain (FDTD) simulations and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) spectra results further reveal that effective coupling LSPR effect generates strong local electric fields and excite high concentration of hot electrons to activate the reactants and intermediate species, reduce the activation energies and accelerate the reaction rate. This work provides a new pathway towards the efficient plasmon-enhanced chemical reactions via reducing the activation energies by utilizing solar energy.
Funding Information
  • Ministry of Education, Culture, Sports, Science and Technology
  • Ministry of Science and Technology of the People's Republic of China (2014CB239301)
  • China Scholarship Council (201606320239)
  • National Natural Science Foundation of China (21633004)

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