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Open AccessArticle

Supported Gold Nanoparticles as Catalysts in Peroxidative and Aerobic Oxidation of 1-Phenylethanol under Mild Conditions

1
Research School of Chemistry & Applied Biomedical Sciences, National Research Tomsk Polytechnic University, Lenin Av. 30, 634050 Tomsk, Russia
2
Centro de Química Estrutural, Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais, 1049-001 Lisboa, Portugal
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Instituto de Catálisis y Petroleoquímica, Consejo Superior de Investigaciones Científicas, Marie Curie 2, 28049 Madrid, Spain
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Department of Chemistry, Moscow State University, 1–3 Leninskiye Gory, 119991 Moscow, Russia
5
Centro de Nanocienciasy Nanotecnología, Universidad Nacional Autónoma de México, Ensenada 22800, Mexico
*
Authors to whom correspondence should be addressed.
Nanomaterials 2020, 10(1), 151; https://doi.org/10.3390/nano10010151
Received: 15 December 2019 / Revised: 3 January 2020 / Accepted: 9 January 2020 / Published: 15 January 2020
(This article belongs to the Special Issue Catalysis by Metal-Oxide Nanostructures)
The efficiency of Au/TiO2 based catalysts in 1-phenylethanol oxidation was investigated. The role of support modifiers (La2O3 or CeO2), influence of gold loading (0.5% or 4%) and redox pretreatment atmosphere, catalyst recyclability, effect of oxidant: tert-butyl hydroperoxide (TBHP) or O2, as well as the optimization of experimental parameters of the reaction conditions in the oxidation of this alcohol were studied and compared with previous studies on 1-octanol oxidation. Samples were characterized by temperature-programmed oxygen desorption (O2-TPD) method. X-ray photoelectron spectroscopy (XPS) measurements were carried out for used catalysts to find out the reason for deactivation in 1-phenylethanol oxidation. The best catalytic characteristics were shown by catalysts modified with La2O3, regardless of the alcohol and the type of oxidant. When O2 was used, the catalysts with 0.5% Au, after oxidative pretreatment, showed the highest activity in both reactions. The most active catalysts in 1-phenylethanol oxidation with TBHP were those with 4% Au and the H2 treatment, while under the same reaction conditions, 0.5% Au and O2 treatment were beneficial in 1-octanol oxidation. Despite the different chemical nature of the substrates, it seems likely that Au+(Auδ+) act as the active sites in both oxidative reactions. Density functional theory (DFT) simulations confirmed that the gold cationic sites play an essential role in 1-phenylethanol adsorption. View Full-Text
Keywords: gold; heterogeneous catalysis; alcohol oxidation; 1-phenylethanol; TBHP; DFT gold; heterogeneous catalysis; alcohol oxidation; 1-phenylethanol; TBHP; DFT
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Pakrieva, E.; P. C. Ribeiro, A.; Kolobova, E.; M. D. R. S. Martins, L.; A. C. Carabineiro, S.; German, D.; Pichugina, D.; Jiang, C.; J. L. Pombeiro, A.; Bogdanchikova, N.; Cortés Corberán, V.; Pestryakov, A. Supported Gold Nanoparticles as Catalysts in Peroxidative and Aerobic Oxidation of 1-Phenylethanol under Mild Conditions. Nanomaterials 2020, 10, 151.

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