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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...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
John Wiley and Sons Inc.
2017
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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. |
format | Online Article Text |
id | pubmed-6099385 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2017 |
publisher | John Wiley and Sons Inc. |
record_format | MEDLINE/PubMed |
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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