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From ethene to propene (ETP) on tailored silica–alumina supports with isolated Ni(ii) sites: uncovering the importance of surface nickel aluminate sites and the carbon-pool mechanism
Catalysts with well-defined isolated Ni(ii) surface sites have been prepared on three silica-based supports. The outer shells of the support were comprised either of an amorphous aluminosilicate or amorphous alumina (AlO(x)) layer – associated with a high and low density of strong Brønsted acid site...
Autores principales: | , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9528926/ https://www.ncbi.nlm.nih.gov/pubmed/36324825 http://dx.doi.org/10.1039/d2cy01272c |
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author | Chen, Zixuan Docherty, Scott R. Florian, Pierre Kierzkowska, Agnieszka Moroz, Ilia B. Abdala, Paula M. Copéret, Christophe Müller, Christoph R. Fedorov, Alexey |
author_facet | Chen, Zixuan Docherty, Scott R. Florian, Pierre Kierzkowska, Agnieszka Moroz, Ilia B. Abdala, Paula M. Copéret, Christophe Müller, Christoph R. Fedorov, Alexey |
author_sort | Chen, Zixuan |
collection | PubMed |
description | Catalysts with well-defined isolated Ni(ii) surface sites have been prepared on three silica-based supports. The outer shells of the support were comprised either of an amorphous aluminosilicate or amorphous alumina (AlO(x)) layer – associated with a high and low density of strong Brønsted acid sites (BAS), respectively. When tested for ethene-to-propene conversion, Ni catalysts with a higher density of strong BAS demonstrate a higher initial activity and productivity to propene. On all three catalysts, the propene productivity correlates closely with the concentration of C(8) aromatics, suggesting that propene may form via a carbon-pool mechanism. While all three catalysts deactivate with time on stream, the deactivation of catalysts with Ni(ii) sites on AlO(x), i.e., containing surface Ni aluminate sites, is shown to be reversible by calcination (coke removal), in contrast to the deactivation of surface Ni silicate or aluminosilicate sites, which deactivate irreversibly by forming Ni nanoparticles. |
format | Online Article Text |
id | pubmed-9528926 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-95289262022-10-31 From ethene to propene (ETP) on tailored silica–alumina supports with isolated Ni(ii) sites: uncovering the importance of surface nickel aluminate sites and the carbon-pool mechanism Chen, Zixuan Docherty, Scott R. Florian, Pierre Kierzkowska, Agnieszka Moroz, Ilia B. Abdala, Paula M. Copéret, Christophe Müller, Christoph R. Fedorov, Alexey Catal Sci Technol Chemistry Catalysts with well-defined isolated Ni(ii) surface sites have been prepared on three silica-based supports. The outer shells of the support were comprised either of an amorphous aluminosilicate or amorphous alumina (AlO(x)) layer – associated with a high and low density of strong Brønsted acid sites (BAS), respectively. When tested for ethene-to-propene conversion, Ni catalysts with a higher density of strong BAS demonstrate a higher initial activity and productivity to propene. On all three catalysts, the propene productivity correlates closely with the concentration of C(8) aromatics, suggesting that propene may form via a carbon-pool mechanism. While all three catalysts deactivate with time on stream, the deactivation of catalysts with Ni(ii) sites on AlO(x), i.e., containing surface Ni aluminate sites, is shown to be reversible by calcination (coke removal), in contrast to the deactivation of surface Ni silicate or aluminosilicate sites, which deactivate irreversibly by forming Ni nanoparticles. The Royal Society of Chemistry 2022-08-31 /pmc/articles/PMC9528926/ /pubmed/36324825 http://dx.doi.org/10.1039/d2cy01272c Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/ |
spellingShingle | Chemistry Chen, Zixuan Docherty, Scott R. Florian, Pierre Kierzkowska, Agnieszka Moroz, Ilia B. Abdala, Paula M. Copéret, Christophe Müller, Christoph R. Fedorov, Alexey From ethene to propene (ETP) on tailored silica–alumina supports with isolated Ni(ii) sites: uncovering the importance of surface nickel aluminate sites and the carbon-pool mechanism |
title | From ethene to propene (ETP) on tailored silica–alumina supports with isolated Ni(ii) sites: uncovering the importance of surface nickel aluminate sites and the carbon-pool mechanism |
title_full | From ethene to propene (ETP) on tailored silica–alumina supports with isolated Ni(ii) sites: uncovering the importance of surface nickel aluminate sites and the carbon-pool mechanism |
title_fullStr | From ethene to propene (ETP) on tailored silica–alumina supports with isolated Ni(ii) sites: uncovering the importance of surface nickel aluminate sites and the carbon-pool mechanism |
title_full_unstemmed | From ethene to propene (ETP) on tailored silica–alumina supports with isolated Ni(ii) sites: uncovering the importance of surface nickel aluminate sites and the carbon-pool mechanism |
title_short | From ethene to propene (ETP) on tailored silica–alumina supports with isolated Ni(ii) sites: uncovering the importance of surface nickel aluminate sites and the carbon-pool mechanism |
title_sort | from ethene to propene (etp) on tailored silica–alumina supports with isolated ni(ii) sites: uncovering the importance of surface nickel aluminate sites and the carbon-pool mechanism |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9528926/ https://www.ncbi.nlm.nih.gov/pubmed/36324825 http://dx.doi.org/10.1039/d2cy01272c |
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