Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation

Ekaterina Pakrieva, Ekaterina Kolobova, Yulia Kotolevich, Laura Pascual, Sónia A. C. Carabineiro, Andrey N. Kharlanov, Daria Pichugina, Nadezhda Nikitina, Dmitrii German, Trino A. Zepeda Partida, Hugo J. Tiznado Vazquez, Mario H. Farías, Nina Bogdanchikova, Vicente Cortés Corberán, Alexey Pestryakov

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Abstract

This study aims to identify the role of the various electronic states of gold in the catalytic behavior of Au/MxOy/TiO2 (where MxOy are Fe2O3 or MgO) for the liquid phase oxidation of n-octanol, under mild conditions. For this purpose, Au/MxOy/TiO2 catalysts were prepared by deposition-precipitation with urea, varying the gold content (0.5 or 4 wt.%) and pretreatment conditions (H2 or O2), and characterized by low temperature nitrogen adsorption-desorption, X-ray powder diffraction (XRD), energy dispersive spectroscopy (EDX), scanning transmission electron microscopy-high angle annular dark field (STEM HAADF), diffuse reflectance Fourier transform infrared (DRIFT) spectroscopy of CO adsorption, temperature-programmable desorption (TPD) of ammonia and carbon dioxide, and X-ray photoelectron spectroscopy (XPS). Three states of gold were identified on the surface of the catalysts, Au0, Au1+ and Au3+, and their ratio determined the catalysts performance. Based on a comparison of catalytic and spectroscopic results, it may be concluded that Au+ was the active site state, while Au0 had negative effect, due to a partial blocking of Au0 by solvent. Au3+ also inhibited the oxidation process, due to the strong adsorption of the solvent and/or water formed during the reaction. Density functional theory (DFT) simulations confirmed these suggestions. The dependence of selectivity on the ratio of Brønsted acid centers to Brønsted basic centers was revealed.

Original languageEnglish
Article number880
JournalNanomaterials
Volume10
Issue number5
DOIs
Publication statusPublished - May 2020

Keywords

  • Acid-base centers
  • DFT
  • Gold active sites
  • Gold catalysts
  • Gold electronic state
  • Metal content
  • N-octanol oxidation
  • Pretreatment atmosphere
  • Selectivity
  • Solvent adsorption
  • Support modifiers

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    Pakrieva, E., Kolobova, E., Kotolevich, Y., Pascual, L., Carabineiro, S. A. C., Kharlanov, A. N., Pichugina, D., Nikitina, N., German, D., Partida, T. A. Z., Vazquez, H. J. T., Farías, M. H., Bogdanchikova, N., Corberán, V. C., & Pestryakov, A. (2020). Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation. Nanomaterials, 10(5), [880]. https://doi.org/10.3390/nano10050880