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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...

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Autores principales: Chen, Zixuan, Docherty, Scott R., Florian, Pierre, Kierzkowska, Agnieszka, Moroz, Ilia B., Abdala, Paula M., Copéret, Christophe, Müller, Christoph R., Fedorov, Alexey
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2022
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.
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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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