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Silica‐Supported Au–Ag Catalysts for the Selective Hydrogenation of Butadiene

Gold and silver are miscible over the entire composition range, and form an attractive combination for fundamental studies on bimetallic catalysts. Au–Ag catalysts have shown synergistic effects for different oxidation and liquid‐phase hydrogenation reactions, but have rarely been studied for gas‐ph...

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Autores principales: Masoud, Nazila, Delannoy, Laurent, Calers, Christophe, Gallet, Jean‐Jacques, Bournel, Fabrice, de Jong, Krijn P., Louis, Catherine, de Jongh, Petra E.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6099385/
https://www.ncbi.nlm.nih.gov/pubmed/30147805
http://dx.doi.org/10.1002/cctc.201700127
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author Masoud, Nazila
Delannoy, Laurent
Calers, Christophe
Gallet, Jean‐Jacques
Bournel, Fabrice
de Jong, Krijn P.
Louis, Catherine
de Jongh, Petra E.
author_facet Masoud, Nazila
Delannoy, Laurent
Calers, Christophe
Gallet, Jean‐Jacques
Bournel, Fabrice
de Jong, Krijn P.
Louis, Catherine
de Jongh, Petra E.
author_sort Masoud, Nazila
collection PubMed
description Gold and silver are miscible over the entire composition range, and form an attractive combination for fundamental studies on bimetallic catalysts. Au–Ag catalysts have shown synergistic effects for different oxidation and liquid‐phase hydrogenation reactions, but have rarely been studied for gas‐phase hydrogenation. In this study 3 nm particles of Au, Ag and Au–Ag supported on silica (SBA‐15) were investigated as catalysts for selective hydrogenation of butadiene in an excess of propene. The Au catalyst was over an order of magnitude more active than the Ag catalyst at 120 °C. The initial activity of the Au–Ag catalysts scaled linearly with the Au‐content, suggesting a direct correlation between the surface and overall compositions of the nanoparticles and the absence of synergistic effects. All Au‐containing catalysts were highly selective to butenes (>99.9 %). The Au catalysts were stable, whereas the Au–Ag catalysts lost about half of their activity during 20 h run time at 200 °C, but the initial activity was restored by a consecutive oxidation‐reduction treatment. Near ambient pressure x‐ray photoelectron spectroscopy showed that exposure to H(2) at elevated temperatures led to a gradual enrichment of the surface of the Au–Ag nanoparticles by Ag. These observations highlight the importance of considering progressive atomic rearrangements in bimetallic nanocatalysts under reaction conditions.
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spelling pubmed-60993852018-08-24 Silica‐Supported Au–Ag Catalysts for the Selective Hydrogenation of Butadiene Masoud, Nazila Delannoy, Laurent Calers, Christophe Gallet, Jean‐Jacques Bournel, Fabrice de Jong, Krijn P. Louis, Catherine de Jongh, Petra E. ChemCatChem Full Papers Gold and silver are miscible over the entire composition range, and form an attractive combination for fundamental studies on bimetallic catalysts. Au–Ag catalysts have shown synergistic effects for different oxidation and liquid‐phase hydrogenation reactions, but have rarely been studied for gas‐phase hydrogenation. In this study 3 nm particles of Au, Ag and Au–Ag supported on silica (SBA‐15) were investigated as catalysts for selective hydrogenation of butadiene in an excess of propene. The Au catalyst was over an order of magnitude more active than the Ag catalyst at 120 °C. The initial activity of the Au–Ag catalysts scaled linearly with the Au‐content, suggesting a direct correlation between the surface and overall compositions of the nanoparticles and the absence of synergistic effects. All Au‐containing catalysts were highly selective to butenes (>99.9 %). The Au catalysts were stable, whereas the Au–Ag catalysts lost about half of their activity during 20 h run time at 200 °C, but the initial activity was restored by a consecutive oxidation‐reduction treatment. Near ambient pressure x‐ray photoelectron spectroscopy showed that exposure to H(2) at elevated temperatures led to a gradual enrichment of the surface of the Au–Ag nanoparticles by Ag. These observations highlight the importance of considering progressive atomic rearrangements in bimetallic nanocatalysts under reaction conditions. John Wiley and Sons Inc. 2017-06-12 2017-06-22 /pmc/articles/PMC6099385/ /pubmed/30147805 http://dx.doi.org/10.1002/cctc.201700127 Text en © 2017 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the http://creativecommons.org/licenses/by-nc/4.0/ License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.
spellingShingle Full Papers
Masoud, Nazila
Delannoy, Laurent
Calers, Christophe
Gallet, Jean‐Jacques
Bournel, Fabrice
de Jong, Krijn P.
Louis, Catherine
de Jongh, Petra E.
Silica‐Supported Au–Ag Catalysts for the Selective Hydrogenation of Butadiene
title Silica‐Supported Au–Ag Catalysts for the Selective Hydrogenation of Butadiene
title_full Silica‐Supported Au–Ag Catalysts for the Selective Hydrogenation of Butadiene
title_fullStr Silica‐Supported Au–Ag Catalysts for the Selective Hydrogenation of Butadiene
title_full_unstemmed Silica‐Supported Au–Ag Catalysts for the Selective Hydrogenation of Butadiene
title_short Silica‐Supported Au–Ag Catalysts for the Selective Hydrogenation of Butadiene
title_sort silica‐supported au–ag catalysts for the selective hydrogenation of butadiene
topic Full Papers
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6099385/
https://www.ncbi.nlm.nih.gov/pubmed/30147805
http://dx.doi.org/10.1002/cctc.201700127
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