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Silica-supported, narrowly distributed, subnanometric Pt–Zn particles from single sites with high propane dehydrogenation performance

The development of highly productive, selective and stable propane dehydrogenation catalysts for propene production is strategic due to the increasing need for propene and the availability of shale gas, an abundant source of light alkanes. In that context, the combination of surface organometallic c...

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Autores principales: Rochlitz, Lukas, Searles, Keith, Alfke, Jan, Zemlyanov, Dmitry, Safonova, Olga V., Copéret, Christophe
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8148060/
https://www.ncbi.nlm.nih.gov/pubmed/34084386
http://dx.doi.org/10.1039/c9sc05599a
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author Rochlitz, Lukas
Searles, Keith
Alfke, Jan
Zemlyanov, Dmitry
Safonova, Olga V.
Copéret, Christophe
author_facet Rochlitz, Lukas
Searles, Keith
Alfke, Jan
Zemlyanov, Dmitry
Safonova, Olga V.
Copéret, Christophe
author_sort Rochlitz, Lukas
collection PubMed
description The development of highly productive, selective and stable propane dehydrogenation catalysts for propene production is strategic due to the increasing need for propene and the availability of shale gas, an abundant source of light alkanes. In that context, the combination of surface organometallic chemistry (SOMC) and a thermolytic molecular precursor (TMP) approach is used to prepare bimetallic subnanometric and narrowly distributed Pt–Zn alloyed particles supported on silica via grafting of a Pt precursor on surface OH groups present in a Zn single-site containing material followed by a H(2) reduction treatment. This material, that exhibits a Zn to Pt molar ratio of 3 : 2 in the form of alloyed Pt–Zn particles with a 0.2 to 0.4 fraction of the overall Zn amount remaining as Zn(II) sites on the silica surface, catalyzes propane dehydrogenation (PDH) with high productivity (703 g(C(3)H(6)) g(Pt)(−1) h(−1) to 375 g(C(3)H(6)) g(Pt)(−1) h(−1)) and very low deactivation rates (k(d) = 0.027 h(−1)) over 30 h at high WHSV (75 h(−1)). This study demonstrates how SOMC can provide access to highly efficient and tailored catalysts through the stepwise introduction of specific elements via grafting to generate small, homogeneously and narrowly distributed supported alloyed nanoparticles at controlled interfaces.
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spelling pubmed-81480602021-06-02 Silica-supported, narrowly distributed, subnanometric Pt–Zn particles from single sites with high propane dehydrogenation performance Rochlitz, Lukas Searles, Keith Alfke, Jan Zemlyanov, Dmitry Safonova, Olga V. Copéret, Christophe Chem Sci Chemistry The development of highly productive, selective and stable propane dehydrogenation catalysts for propene production is strategic due to the increasing need for propene and the availability of shale gas, an abundant source of light alkanes. In that context, the combination of surface organometallic chemistry (SOMC) and a thermolytic molecular precursor (TMP) approach is used to prepare bimetallic subnanometric and narrowly distributed Pt–Zn alloyed particles supported on silica via grafting of a Pt precursor on surface OH groups present in a Zn single-site containing material followed by a H(2) reduction treatment. This material, that exhibits a Zn to Pt molar ratio of 3 : 2 in the form of alloyed Pt–Zn particles with a 0.2 to 0.4 fraction of the overall Zn amount remaining as Zn(II) sites on the silica surface, catalyzes propane dehydrogenation (PDH) with high productivity (703 g(C(3)H(6)) g(Pt)(−1) h(−1) to 375 g(C(3)H(6)) g(Pt)(−1) h(−1)) and very low deactivation rates (k(d) = 0.027 h(−1)) over 30 h at high WHSV (75 h(−1)). This study demonstrates how SOMC can provide access to highly efficient and tailored catalysts through the stepwise introduction of specific elements via grafting to generate small, homogeneously and narrowly distributed supported alloyed nanoparticles at controlled interfaces. The Royal Society of Chemistry 2019-12-23 /pmc/articles/PMC8148060/ /pubmed/34084386 http://dx.doi.org/10.1039/c9sc05599a Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
Rochlitz, Lukas
Searles, Keith
Alfke, Jan
Zemlyanov, Dmitry
Safonova, Olga V.
Copéret, Christophe
Silica-supported, narrowly distributed, subnanometric Pt–Zn particles from single sites with high propane dehydrogenation performance
title Silica-supported, narrowly distributed, subnanometric Pt–Zn particles from single sites with high propane dehydrogenation performance
title_full Silica-supported, narrowly distributed, subnanometric Pt–Zn particles from single sites with high propane dehydrogenation performance
title_fullStr Silica-supported, narrowly distributed, subnanometric Pt–Zn particles from single sites with high propane dehydrogenation performance
title_full_unstemmed Silica-supported, narrowly distributed, subnanometric Pt–Zn particles from single sites with high propane dehydrogenation performance
title_short Silica-supported, narrowly distributed, subnanometric Pt–Zn particles from single sites with high propane dehydrogenation performance
title_sort silica-supported, narrowly distributed, subnanometric pt–zn particles from single sites with high propane dehydrogenation performance
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8148060/
https://www.ncbi.nlm.nih.gov/pubmed/34084386
http://dx.doi.org/10.1039/c9sc05599a
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