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Implications of Ga promotion and metal–oxide interface from tailored PtGa propane dehydrogenation catalysts supported on carbon
Propane Dehydrogenation is a key technology, where Pt-based catalysts have widely been investigated in industry and academia, with development exploring the use of promoters (Sn, Zn, Ga, etc.) and additives (Na, K, Ca, Si, etc.) towards improved catalytic performances. Recent studies have focused on...
Autores principales: | , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10646969/ https://www.ncbi.nlm.nih.gov/pubmed/38020386 http://dx.doi.org/10.1039/d3sc04711c |
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author | Brack, Enzo Plodinec, Milivoj Willinger, Marc-Georg Copéret, Christophe |
author_facet | Brack, Enzo Plodinec, Milivoj Willinger, Marc-Georg Copéret, Christophe |
author_sort | Brack, Enzo |
collection | PubMed |
description | Propane Dehydrogenation is a key technology, where Pt-based catalysts have widely been investigated in industry and academia, with development exploring the use of promoters (Sn, Zn, Ga, etc.) and additives (Na, K, Ca, Si, etc.) towards improved catalytic performances. Recent studies have focused on the role of Ga promotion: while computations suggest that Ga plays a key role in enhancing catalytic selectivity and stability of PtGa catalysts through Pt-site isolation as well as morphological changes, experimental evidence are lacking because of the use of oxide supports that prevent more detailed investigation. Here, we develop a methodology to generate Pt and PtGa nanoparticles with tailored interfaces on carbon supports by combining surface organometallic chemistry (SOMC) and specific thermolytic molecular precursors containing or not siloxide ligands. This approach enables the preparation of supported nanoparticles, exhibiting or not an oxide interface, suitable for state-of-the art electron microscopy and XANES characterization. We show that the introduction of Ga enables the formation of homogenously alloyed, amorphous PtGa nanoparticles, in sharp contrast to highly crystalline monometallic Pt nanoparticles. Furthermore, the presence of an oxide interface is shown to stabilize the formation of small particles, at the expense of propene selectivity loss (formation of cracking side-products, methane/ethene), explaining the use of additives such as Na, K and Ca in industrial catalysts. |
format | Online Article Text |
id | pubmed-10646969 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-106469692023-10-25 Implications of Ga promotion and metal–oxide interface from tailored PtGa propane dehydrogenation catalysts supported on carbon Brack, Enzo Plodinec, Milivoj Willinger, Marc-Georg Copéret, Christophe Chem Sci Chemistry Propane Dehydrogenation is a key technology, where Pt-based catalysts have widely been investigated in industry and academia, with development exploring the use of promoters (Sn, Zn, Ga, etc.) and additives (Na, K, Ca, Si, etc.) towards improved catalytic performances. Recent studies have focused on the role of Ga promotion: while computations suggest that Ga plays a key role in enhancing catalytic selectivity and stability of PtGa catalysts through Pt-site isolation as well as morphological changes, experimental evidence are lacking because of the use of oxide supports that prevent more detailed investigation. Here, we develop a methodology to generate Pt and PtGa nanoparticles with tailored interfaces on carbon supports by combining surface organometallic chemistry (SOMC) and specific thermolytic molecular precursors containing or not siloxide ligands. This approach enables the preparation of supported nanoparticles, exhibiting or not an oxide interface, suitable for state-of-the art electron microscopy and XANES characterization. We show that the introduction of Ga enables the formation of homogenously alloyed, amorphous PtGa nanoparticles, in sharp contrast to highly crystalline monometallic Pt nanoparticles. Furthermore, the presence of an oxide interface is shown to stabilize the formation of small particles, at the expense of propene selectivity loss (formation of cracking side-products, methane/ethene), explaining the use of additives such as Na, K and Ca in industrial catalysts. The Royal Society of Chemistry 2023-10-25 /pmc/articles/PMC10646969/ /pubmed/38020386 http://dx.doi.org/10.1039/d3sc04711c Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/ |
spellingShingle | Chemistry Brack, Enzo Plodinec, Milivoj Willinger, Marc-Georg Copéret, Christophe Implications of Ga promotion and metal–oxide interface from tailored PtGa propane dehydrogenation catalysts supported on carbon |
title | Implications of Ga promotion and metal–oxide interface from tailored PtGa propane dehydrogenation catalysts supported on carbon |
title_full | Implications of Ga promotion and metal–oxide interface from tailored PtGa propane dehydrogenation catalysts supported on carbon |
title_fullStr | Implications of Ga promotion and metal–oxide interface from tailored PtGa propane dehydrogenation catalysts supported on carbon |
title_full_unstemmed | Implications of Ga promotion and metal–oxide interface from tailored PtGa propane dehydrogenation catalysts supported on carbon |
title_short | Implications of Ga promotion and metal–oxide interface from tailored PtGa propane dehydrogenation catalysts supported on carbon |
title_sort | implications of ga promotion and metal–oxide interface from tailored ptga propane dehydrogenation catalysts supported on carbon |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10646969/ https://www.ncbi.nlm.nih.gov/pubmed/38020386 http://dx.doi.org/10.1039/d3sc04711c |
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