4.6 Article

Plasmon-assisted facile selective gaseous isopropanol dehydrogenation over Ag nanocubes

期刊

CATALYSIS SCIENCE & TECHNOLOGY
卷 12, 期 1, 页码 94-104

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1cy01454d

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资金

  1. National Natural Science Foundation of China [51772230]
  2. National Key Research and Development of China [2017YFE0192600]
  3. 111 Project [B18038]
  4. Open Foundation of Key Laboratory for UV-Emitting Materials and Technology of the Ministry of Education, Northeast Normal University [135130013]

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The study focuses on the dehydrogenation of isopropanol over monodisperse Ag nanocubes, revealing that light illumination can enhance the reaction efficiency without compromising selectivity. Factors such as reaction temperatures, light wavelengths, light intensities, and nanocube sizes are investigated to understand their influence on catalytic yields. Plasmonic non-thermal effect is found to have a low contribution to the light-induced increase in catalytic activity.
In the current research, monodisperse Ag nanocubes are synthesized and characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), field-emission transmittance electron microscopy (FE-TEM), X-ray photoelectron spectroscopy (XPS), and UV-vis photospectrometry. It is seen that isopropanol can be dehydrogenated to acetone over Ag nanocubes in high selectivity at near-room temperatures. Light illumination leads to an increase in the isopropanol dehydrogenation efficiency without decreasing the selectivity. The effects of reaction temperatures, light wavelengths, light intensities, and sizes of the Ag nanocubes on the catalytic yields are investigated in detail. The result reveals that plasmonic heating has a low contribution to the light-induced increase of the catalytic activity, which could be ascribed to a plasmonic non-thermal effect. It is seen that the dehydrogenation activity is dependent on alpha-hydrogen activation. As compared to methanol, ethanol, and N-propanol, isopropanol presents the highest light-induced catalytic activity because of the most active alpha-hydrogens. It is considered that the hot electron transfer from the Ag nanocubes to molecular O-2 accelerates oxygen activation for isopropanol dehydrogenation.

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