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An, Kwangjin
Advanced Nanocatalysis Lab (An Lab)
Research Interests
  • Nanoparticle catalytsts, catalytic activity, selectivity, and stability, strong metal-support interactions, CO2 utilization, biomass conversion, Plastic Up-cycling

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Comparing the Catalytic Oxidation of Ethanol at the Solid−Gas and Solid−Liquid Interfaces over Size-Controlled Pt Nanoparticles: Striking Differences in Kinetics and Mechanism

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Title
Comparing the Catalytic Oxidation of Ethanol at the Solid−Gas and Solid−Liquid Interfaces over Size-Controlled Pt Nanoparticles: Striking Differences in Kinetics and Mechanism
Author
Sapi, AndrasLiu, FudongCai, XiaojunThompson, Christopher M.Wang, HailiangAn, KwangjinKrier, James M.Somorjai, Gabor A.
Keywords
ethanol oxidation; Heterogeneous catalysis; platinum nanoparticles; size control; sum frequency generation
Issue Date
2014-10
Publisher
AMER CHEMICAL SOC
Citation
NANO LETTERS, v.14, no.11, pp.6727 - 6730
Abstract
Pt nanoparticles with controlled size (2, 4, and 6 nm) are synthesized and tested in ethanol oxidation by molecular oxygen at 60 °C to acetaldehyde and carbon dioxide both in the gas and liquid phases. The turnover frequency of the reaction is 80 times faster, and the activation energy is 5 times higher at the gas-solid interface compared to the liquid-solid interface. The catalytic activity is highly dependent on the size of the Pt nanoparticles; however, the selectivity is not size sensitive. Acetaldehyde is the main product in both media, while twice as much carbon dioxide was observed in the gas phase compared to the liquid phase. Added water boosts the reaction in the liquid phase; however, it acts as an inhibitor in the gas phase. The more water vapor was added, the more carbon dioxide was formed in the gas phase, while the selectivity was not affected by the concentration of the water in the liquid phase. The differences in the reaction kinetics of the solid-gas and solid-liquid interfaces can be attributed to the molecular orientation deviation of the ethanol molecules on the Pt surface in the gas and liquid phases as evidenced by sum frequency generation vibrational spectroscopy. © 2014 American Chemical Society.
URI
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DOI
10.1021/nl5035545
ISSN
1530-6984
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ECHE_Journal Papers
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