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Silica-supported isolated gallium sites as highly active, selective and stable propane dehydrogenation catalysts
Single-site gallium centers on the surface of silica are prepared via grafting of [Ga(OSi(OtBu)(3))(3)(THF)] on SiO(2–700) followed by a thermolysis step. The resulting surface species corresponds to well-defined tetra-coordinate gallium single-sites, [([triple bond, length as m-dash]SiO)(3)Ga(XOSi[...
Autores principales: | , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Royal Society of Chemistry
2017
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5433511/ https://www.ncbi.nlm.nih.gov/pubmed/28553501 http://dx.doi.org/10.1039/c6sc05178b |
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author | Searles, Keith Siddiqi, Georges Safonova, Olga V. Copéret, Christophe |
author_facet | Searles, Keith Siddiqi, Georges Safonova, Olga V. Copéret, Christophe |
author_sort | Searles, Keith |
collection | PubMed |
description | Single-site gallium centers on the surface of silica are prepared via grafting of [Ga(OSi(OtBu)(3))(3)(THF)] on SiO(2–700) followed by a thermolysis step. The resulting surface species corresponds to well-defined tetra-coordinate gallium single-sites, [([triple bond, length as m-dash]SiO)(3)Ga(XOSi[triple bond, length as m-dash])] (X = –H or [triple bond, length as m-dash]Si) according to IR, X-ray absorption near-edge structure and extended X-ray absorption fine structure analysis. These gallium sites show high activity, selectivity and stability for propane dehydrogenation with an initial turnover frequency of 20 per h per gallium center, propylene selectivity of ≥93% and remarkable stability over 20 h. The stability of the catalyst probably results from site-isolation of the active site on a non-reducible support such as silica, diminishing facile reduction typical of Ga(2)O(3)-based catalysts. |
format | Online Article Text |
id | pubmed-5433511 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2017 |
publisher | Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-54335112017-05-26 Silica-supported isolated gallium sites as highly active, selective and stable propane dehydrogenation catalysts Searles, Keith Siddiqi, Georges Safonova, Olga V. Copéret, Christophe Chem Sci Chemistry Single-site gallium centers on the surface of silica are prepared via grafting of [Ga(OSi(OtBu)(3))(3)(THF)] on SiO(2–700) followed by a thermolysis step. The resulting surface species corresponds to well-defined tetra-coordinate gallium single-sites, [([triple bond, length as m-dash]SiO)(3)Ga(XOSi[triple bond, length as m-dash])] (X = –H or [triple bond, length as m-dash]Si) according to IR, X-ray absorption near-edge structure and extended X-ray absorption fine structure analysis. These gallium sites show high activity, selectivity and stability for propane dehydrogenation with an initial turnover frequency of 20 per h per gallium center, propylene selectivity of ≥93% and remarkable stability over 20 h. The stability of the catalyst probably results from site-isolation of the active site on a non-reducible support such as silica, diminishing facile reduction typical of Ga(2)O(3)-based catalysts. Royal Society of Chemistry 2017-04-01 2017-01-03 /pmc/articles/PMC5433511/ /pubmed/28553501 http://dx.doi.org/10.1039/c6sc05178b Text en This journal is © The Royal Society of Chemistry 2017 https://creativecommons.org/licenses/by-nc/3.0/This is an Open Access article distributed under the terms of the Creative Commons Attribution-NonCommercial 3.0 Unported License (http://creativecommons.org/licenses/by-nc/3.0/ (https://creativecommons.org/licenses/by-nc/3.0/) ) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is properly cited. |
spellingShingle | Chemistry Searles, Keith Siddiqi, Georges Safonova, Olga V. Copéret, Christophe Silica-supported isolated gallium sites as highly active, selective and stable propane dehydrogenation catalysts |
title | Silica-supported isolated gallium sites as highly active, selective and stable propane dehydrogenation catalysts
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title_full | Silica-supported isolated gallium sites as highly active, selective and stable propane dehydrogenation catalysts
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title_fullStr | Silica-supported isolated gallium sites as highly active, selective and stable propane dehydrogenation catalysts
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title_full_unstemmed | Silica-supported isolated gallium sites as highly active, selective and stable propane dehydrogenation catalysts
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title_short | Silica-supported isolated gallium sites as highly active, selective and stable propane dehydrogenation catalysts
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title_sort | silica-supported isolated gallium sites as highly active, selective and stable propane dehydrogenation catalysts |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5433511/ https://www.ncbi.nlm.nih.gov/pubmed/28553501 http://dx.doi.org/10.1039/c6sc05178b |
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