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Effect of Gold Electronic State on the Catalytic Performance of Nano Gold Catalysts in n-Octanol Oxidation

AuthorsPakrieva, Ekaterina; Kolobova, Ekaterina; Kotolevich, Yulia; Pascual, Laura ; Carabineiro, Sónia A. C.; Kharlanov, Andrey N.; Pichugina, Daria; Nikitina, Nadezhda; German, Dmitrii; Zepeda Partida, Trino A.; Tiznado Vazquez, Hugo J.; Farías, Mario H.; Bogdanchikova, Nina; Cortés Corberán, Vicente ; Pestryakov, Alexey
Issue Date2-May-2020
PublisherMultidisciplinary Digital Publishing Institute
CitationNanomaterials 10 (5): 880 (2020)
AbstractThis study aims to identify the role of the various electronic states of gold in the catalytic behavior of Au/M<sub>x</sub>O<sub>y</sub>/TiO<sub>2</sub> (where M<sub>x</sub>O<sub>y</sub> are Fe<sub>2</sub>O<sub>3</sub> or MgO) for the liquid phase oxidation of <i>n</i>-octanol, under mild conditions. For this purpose, Au/M<sub>x</sub>O<sub>y</sub>/TiO<sub>2</sub> catalysts were prepared by deposition-precipitation with urea, varying the gold content (0.5 or 4 wt.%) and pretreatment conditions (H<sub>2</sub> or O<sub>2</sub>), 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, Au<sup>0</sup>, Au<sup>1+</sup> and Au<sup>3+</sup>, and their ratio determined the catalysts performance. Based on a comparison of catalytic and spectroscopic results, it may be concluded that Au<sup>+</sup> was the active site state, while Au<sup>0</sup> had negative effect, due to a partial blocking of Au<sup>0</sup> by solvent. Au<sup>3+</sup> 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 Br&oslash;nsted acid centers to Br&oslash;nsted basic centers was revealed.
Identifiersdoi: 10.3390/nano10050880
Appears in Collections:Colección MDPI
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