Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite
Autor(a) principal: | |
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Data de Publicação: | 2019 |
Outros Autores: | , , , , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
Texto Completo: | http://hdl.handle.net/10400.21/11496 |
Resumo: | The effect of pressure on the activity and selectivity of well-balanced Pt/H-beta zeolite bifunctional catalysts in n-hexadecane (n-C16) hydroisomerization was studied. The turnover frequency per Brønsted acid site of the catalyst decreased when the total pressure was increased due to the lower concentration of olefins at equilibrium, in line with the classical bifunctional mechanism. Conversely, when the total pressure was increased, the C16 isomer yield unexpectedly decreased in contradiction with the pure kinetic/ thermodynamic effect of olefin pressure on the reaction rates. Thanks to grand canonical Monte Carlo (GCMC) calculations, non-idealities in adsorption behavior in the zeolite micropores were revealed when a representative reaction medium was considered. Via mechanistic kinetic simulations combined with GCMC simulations for the relevant intermediate concentrations, the pressure effect on catalyst selectivity is proposed to be due to the interplay between the (light) cracked products and the (heavy) hexadecanes in the pores of beta zeolite which leads to a pressure dependency on the adsorption behavior. |
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Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeoliteBrønsted acidCatalyst decreasedOlefins at equilibriumClassical bifunctional mechanismC16 isomer yieldKinetic/thermodynamicThe effect of pressure on the activity and selectivity of well-balanced Pt/H-beta zeolite bifunctional catalysts in n-hexadecane (n-C16) hydroisomerization was studied. The turnover frequency per Brønsted acid site of the catalyst decreased when the total pressure was increased due to the lower concentration of olefins at equilibrium, in line with the classical bifunctional mechanism. Conversely, when the total pressure was increased, the C16 isomer yield unexpectedly decreased in contradiction with the pure kinetic/ thermodynamic effect of olefin pressure on the reaction rates. Thanks to grand canonical Monte Carlo (GCMC) calculations, non-idealities in adsorption behavior in the zeolite micropores were revealed when a representative reaction medium was considered. Via mechanistic kinetic simulations combined with GCMC simulations for the relevant intermediate concentrations, the pressure effect on catalyst selectivity is proposed to be due to the interplay between the (light) cracked products and the (heavy) hexadecanes in the pores of beta zeolite which leads to a pressure dependency on the adsorption behavior.Royal Society of ChemistryRCIPLMendes, Pedro S. F.Chizallet, CélinePérez-Pellitero, JavierRaybaud, PascalSilva, JoãoRibeiro, M FilipaDaudin, AntoineBouchy, Christophe2020-04-22T17:14:29Z2019-102019-10-01T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10400.21/11496engMENDES, Pedro S. F.; [et al] – Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite. Catalysis Science Technology. ISSN 2044-4753. Vol. 9, N.º 19 (2019), pp. 5368-53822044-475310.1039/c9cy00788ametadata only accessinfo:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2023-08-03T10:02:48Zoai:repositorio.ipl.pt:10400.21/11496Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-19T20:19:44.411358Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse |
dc.title.none.fl_str_mv |
Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite |
title |
Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite |
spellingShingle |
Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite Mendes, Pedro S. F. Brønsted acid Catalyst decreased Olefins at equilibrium Classical bifunctional mechanism C16 isomer yield Kinetic/thermodynamic |
title_short |
Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite |
title_full |
Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite |
title_fullStr |
Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite |
title_full_unstemmed |
Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite |
title_sort |
Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite |
author |
Mendes, Pedro S. F. |
author_facet |
Mendes, Pedro S. F. Chizallet, Céline Pérez-Pellitero, Javier Raybaud, Pascal Silva, João Ribeiro, M Filipa Daudin, Antoine Bouchy, Christophe |
author_role |
author |
author2 |
Chizallet, Céline Pérez-Pellitero, Javier Raybaud, Pascal Silva, João Ribeiro, M Filipa Daudin, Antoine Bouchy, Christophe |
author2_role |
author author author author author author author |
dc.contributor.none.fl_str_mv |
RCIPL |
dc.contributor.author.fl_str_mv |
Mendes, Pedro S. F. Chizallet, Céline Pérez-Pellitero, Javier Raybaud, Pascal Silva, João Ribeiro, M Filipa Daudin, Antoine Bouchy, Christophe |
dc.subject.por.fl_str_mv |
Brønsted acid Catalyst decreased Olefins at equilibrium Classical bifunctional mechanism C16 isomer yield Kinetic/thermodynamic |
topic |
Brønsted acid Catalyst decreased Olefins at equilibrium Classical bifunctional mechanism C16 isomer yield Kinetic/thermodynamic |
description |
The effect of pressure on the activity and selectivity of well-balanced Pt/H-beta zeolite bifunctional catalysts in n-hexadecane (n-C16) hydroisomerization was studied. The turnover frequency per Brønsted acid site of the catalyst decreased when the total pressure was increased due to the lower concentration of olefins at equilibrium, in line with the classical bifunctional mechanism. Conversely, when the total pressure was increased, the C16 isomer yield unexpectedly decreased in contradiction with the pure kinetic/ thermodynamic effect of olefin pressure on the reaction rates. Thanks to grand canonical Monte Carlo (GCMC) calculations, non-idealities in adsorption behavior in the zeolite micropores were revealed when a representative reaction medium was considered. Via mechanistic kinetic simulations combined with GCMC simulations for the relevant intermediate concentrations, the pressure effect on catalyst selectivity is proposed to be due to the interplay between the (light) cracked products and the (heavy) hexadecanes in the pores of beta zeolite which leads to a pressure dependency on the adsorption behavior. |
publishDate |
2019 |
dc.date.none.fl_str_mv |
2019-10 2019-10-01T00:00:00Z 2020-04-22T17:14:29Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://hdl.handle.net/10400.21/11496 |
url |
http://hdl.handle.net/10400.21/11496 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
MENDES, Pedro S. F.; [et al] – Interplay of the adsorption of light and heavy paraffins in hydroisomerization over H-beta zeolite. Catalysis Science Technology. ISSN 2044-4753. Vol. 9, N.º 19 (2019), pp. 5368-5382 2044-4753 10.1039/c9cy00788a |
dc.rights.driver.fl_str_mv |
metadata only access info:eu-repo/semantics/openAccess |
rights_invalid_str_mv |
metadata only access |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
application/pdf |
dc.publisher.none.fl_str_mv |
Royal Society of Chemistry |
publisher.none.fl_str_mv |
Royal Society of Chemistry |
dc.source.none.fl_str_mv |
reponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação instacron:RCAAP |
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Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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RCAAP |
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RCAAP |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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