Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation
Por:
Pakrieva, Ekaterina, Kolobova, Ekaterina, Kotolevich, Yulia, Pascual, Laura, Carabineiro S.A.C., Kharlanov, Andrey N., Pichugina, Daria, Nikitina, Nadezhda, German, Dmitrii, Partida T.A.Z., Vazquez H.J.T., Farias, Mario H., Bogdanchikova, Nina, Corberán V.C., Pestryakov, Alexey
Publicada:
1 ene 2020
Resumen:
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. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
Filiaciones:
Pakrieva, Ekaterina:
Research School of Chemistry & Applied Biomedical Sciences, National Research Tomsk Polytechnic University, Lenin Av. 30, Tomsk, 634050, Russian Federation
Instituto de Catálisis y Petroleoquímica, Consejo Superior de InvestigacionesCientíficas, Marie Curie 2, Madrid, 28049, Spain
Natl Res Tomsk Polytech Univ, Res Sch Chem & Appl Biomed Sci, Lenin Av 30, Tomsk 634050, Russia
CSIC, Inst Catalisis & Petroleoquim, Marie Curie 2, Madrid 28049, Spain
Kolobova, Ekaterina:
Research School of Chemistry & Applied Biomedical Sciences, National Research Tomsk Polytechnic University, Lenin Av. 30, Tomsk, 634050, Russian Federation
Natl Res Tomsk Polytech Univ, Res Sch Chem & Appl Biomed Sci, Lenin Av 30, Tomsk 634050, Russia
Kotolevich, Yulia:
Centro de Nanociencias y Nanotecnología, Universidad Nacional Autónoma de México, P.O. Box 14, Ensenada, 22800, Mexico
Univ Nacl Autonoma Mexico, Ctr Nanociencias & Nanotecnol, POB 14, Ensenada 22800, Baja California, Mexico
Pascual, Laura:
Instituto de Catálisis y Petroleoquímica, Consejo Superior de InvestigacionesCientíficas, Marie Curie 2, Madrid, 28049, Spain
CSIC, Inst Catalisis & Petroleoquim, Marie Curie 2, Madrid 28049, Spain
Carabineiro S.A.C.:
LAQV-REQUIMTE, Department of Chemistry, NOVA School of Science and Technology, Universidade, NOVA de Lisboa, Caparica, 2829-516, Portugal
Kharlanov, Andrey N.:
Department of Chemistry, Lomonosov Moscow State University, 1-3 Leninskiye Gory, GSP-1, Moscow, 119991, Russian Federation
Lomonosov Moscow State Univ, Dept Chem, 1-3 Leninskiye Gory,GSP-1, Moscow 119991, Russia
Pichugina, Daria:
Department of Chemistry, Lomonosov Moscow State University, 1-3 Leninskiye Gory, GSP-1, Moscow, 119991, Russian Federation
Lomonosov Moscow State Univ, Dept Chem, 1-3 Leninskiye Gory,GSP-1, Moscow 119991, Russia
Nikitina, Nadezhda:
Department of Chemistry, Lomonosov Moscow State University, 1-3 Leninskiye Gory, GSP-1, Moscow, 119991, Russian Federation
Lomonosov Moscow State Univ, Dept Chem, 1-3 Leninskiye Gory,GSP-1, Moscow 119991, Russia
German, Dmitrii:
Research School of Chemistry & Applied Biomedical Sciences, National Research Tomsk Polytechnic University, Lenin Av. 30, Tomsk, 634050, Russian Federation
Natl Res Tomsk Polytech Univ, Res Sch Chem & Appl Biomed Sci, Lenin Av 30, Tomsk 634050, Russia
Partida T.A.Z.:
Centro de Nanociencias y Nanotecnología, Universidad Nacional Autónoma de México, P.O. Box 14, Ensenada, 22800, Mexico
Vazquez H.J.T.:
Centro de Nanociencias y Nanotecnología, Universidad Nacional Autónoma de México, P.O. Box 14, Ensenada, 22800, Mexico
Farias, Mario H.:
Centro de Nanociencias y Nanotecnología, Universidad Nacional Autónoma de México, P.O. Box 14, Ensenada, 22800, Mexico
Univ Nacl Autonoma Mexico, Ctr Nanociencias & Nanotecnol, POB 14, Ensenada 22800, Baja California, Mexico
Bogdanchikova, Nina:
Centro de Nanociencias y Nanotecnología, Universidad Nacional Autónoma de México, P.O. Box 14, Ensenada, 22800, Mexico
Univ Nacl Autonoma Mexico, Ctr Nanociencias & Nanotecnol, POB 14, Ensenada 22800, Baja California, Mexico
Corberán V.C.:
Instituto de Catálisis y Petroleoquímica, Consejo Superior de InvestigacionesCientíficas, Marie Curie 2, Madrid, 28049, Spain
Pestryakov, Alexey:
Research School of Chemistry & Applied Biomedical Sciences, National Research Tomsk Polytechnic University, Lenin Av. 30, Tomsk, 634050, Russian Federation
Natl Res Tomsk Polytech Univ, Res Sch Chem & Appl Biomed Sci, Lenin Av 30, Tomsk 634050, Russia
Univ NOVA Lisboa, NOVA Sch Sci & Technol, Dept Chem, LAQV REQUIMTE, P-2829516 Caparica, Portugal
|