An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption

Autores
Kresnawahjuesa, O.; Kühl, G.H.; Gorte, R.J.; Querini, Carlos Alberto
Año de publicación
2002
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The adsorption and reaction properties of an Al-free H-[Fe]ZSM-5 were examined and compared to an H-[Al]ZSM-5 sample with the same site density. H-[Fe]ZSM-5 was shown to have Brønsted acid sites in a concentration equal to the framework Fe concentration. Differential heats of adsorption for ammonia and pyridine were shown to be identical to that obtained in H-[Al]ZSM-5, with differential heats of ∼150 kJ/mol for ammonia and 200 kJ/mol for pyridine. For H-[Al]ZSM-5, adsorption of either propylene or 1-butene at room temperature resulted in rapid oligomerization. TPD–TGA measurements of the oligomers in H-[Al]ZSM-5 showed evidence for hydride-transfer reactions, in addition to simple oligomer cracking. By contrast, it was necessary to heat H-[Fe]ZSM-5 to 370 K for rapid oligomerization of propylene and oligomerization of 1-butene occurred only slowly at 295 K. TPD–TGA measurements of the oligomers in H-[Fe]ZSM-5 showed no evidence for hydride-transfer reactions and H-[Fe]ZSM-5 formed much less coke than H-[Al]ZSM-5 during steady-state reaction in 1-butene at 573 K. Adsorption measurements of 1-butene on D-[Fe]ZSM-5 suggested that the protonated complexes of 1-butene were formed but that these were relatively stable toward reaction, implying that the carbocation transition states were relatively unstable.
Fil: Kresnawahjuesa, O.. University of Pennsylvania; Estados Unidos
Fil: Kühl, G.H.. University of Pennsylvania; Estados Unidos
Fil: Gorte, R.J.. University of Pennsylvania; Estados Unidos
Fil: Querini, Carlos Alberto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Materia
Butene
Oligomerization
Fe-Zsm5
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/39273
Acceder
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network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and AdsorptionKresnawahjuesa, O.Kühl, G.H.Gorte, R.J.Querini, Carlos AlbertoButeneOligomerizationFe-Zsm5https://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The adsorption and reaction properties of an Al-free H-[Fe]ZSM-5 were examined and compared to an H-[Al]ZSM-5 sample with the same site density. H-[Fe]ZSM-5 was shown to have Brønsted acid sites in a concentration equal to the framework Fe concentration. Differential heats of adsorption for ammonia and pyridine were shown to be identical to that obtained in H-[Al]ZSM-5, with differential heats of ∼150 kJ/mol for ammonia and 200 kJ/mol for pyridine. For H-[Al]ZSM-5, adsorption of either propylene or 1-butene at room temperature resulted in rapid oligomerization. TPD–TGA measurements of the oligomers in H-[Al]ZSM-5 showed evidence for hydride-transfer reactions, in addition to simple oligomer cracking. By contrast, it was necessary to heat H-[Fe]ZSM-5 to 370 K for rapid oligomerization of propylene and oligomerization of 1-butene occurred only slowly at 295 K. TPD–TGA measurements of the oligomers in H-[Fe]ZSM-5 showed no evidence for hydride-transfer reactions and H-[Fe]ZSM-5 formed much less coke than H-[Al]ZSM-5 during steady-state reaction in 1-butene at 573 K. Adsorption measurements of 1-butene on D-[Fe]ZSM-5 suggested that the protonated complexes of 1-butene were formed but that these were relatively stable toward reaction, implying that the carbocation transition states were relatively unstable.Fil: Kresnawahjuesa, O.. University of Pennsylvania; Estados UnidosFil: Kühl, G.H.. University of Pennsylvania; Estados UnidosFil: Gorte, R.J.. University of Pennsylvania; Estados UnidosFil: Querini, Carlos Alberto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaAcademic Press Inc Elsevier Science2002-08info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/39273Kresnawahjuesa, O.; Kühl, G.H.; Gorte, R.J.; Querini, Carlos Alberto; An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption; Academic Press Inc Elsevier Science; Journal of Catalysis; 210; 1; 8-2002; 106-1150021-9517CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1006/jcat.2002.3657info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0021951702936572info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:58:30Zoai:ri.conicet.gov.ar:11336/39273instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-29 09:58:31.197CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption
title An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption
spellingShingle An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption
Kresnawahjuesa, O.
Butene
Oligomerization
Fe-Zsm5
title_short An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption
title_full An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption
title_fullStr An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption
title_full_unstemmed An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption
title_sort An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption
dc.creator.none.fl_str_mv Kresnawahjuesa, O.
Kühl, G.H.
Gorte, R.J.
Querini, Carlos Alberto
author Kresnawahjuesa, O.
author_facet Kresnawahjuesa, O.
Kühl, G.H.
Gorte, R.J.
Querini, Carlos Alberto
author_role author
author2 Kühl, G.H.
Gorte, R.J.
Querini, Carlos Alberto
author2_role author
author
author
dc.subject.none.fl_str_mv Butene
Oligomerization
Fe-Zsm5
topic Butene
Oligomerization
Fe-Zsm5
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The adsorption and reaction properties of an Al-free H-[Fe]ZSM-5 were examined and compared to an H-[Al]ZSM-5 sample with the same site density. H-[Fe]ZSM-5 was shown to have Brønsted acid sites in a concentration equal to the framework Fe concentration. Differential heats of adsorption for ammonia and pyridine were shown to be identical to that obtained in H-[Al]ZSM-5, with differential heats of ∼150 kJ/mol for ammonia and 200 kJ/mol for pyridine. For H-[Al]ZSM-5, adsorption of either propylene or 1-butene at room temperature resulted in rapid oligomerization. TPD–TGA measurements of the oligomers in H-[Al]ZSM-5 showed evidence for hydride-transfer reactions, in addition to simple oligomer cracking. By contrast, it was necessary to heat H-[Fe]ZSM-5 to 370 K for rapid oligomerization of propylene and oligomerization of 1-butene occurred only slowly at 295 K. TPD–TGA measurements of the oligomers in H-[Fe]ZSM-5 showed no evidence for hydride-transfer reactions and H-[Fe]ZSM-5 formed much less coke than H-[Al]ZSM-5 during steady-state reaction in 1-butene at 573 K. Adsorption measurements of 1-butene on D-[Fe]ZSM-5 suggested that the protonated complexes of 1-butene were formed but that these were relatively stable toward reaction, implying that the carbocation transition states were relatively unstable.
Fil: Kresnawahjuesa, O.. University of Pennsylvania; Estados Unidos
Fil: Kühl, G.H.. University of Pennsylvania; Estados Unidos
Fil: Gorte, R.J.. University of Pennsylvania; Estados Unidos
Fil: Querini, Carlos Alberto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
description The adsorption and reaction properties of an Al-free H-[Fe]ZSM-5 were examined and compared to an H-[Al]ZSM-5 sample with the same site density. H-[Fe]ZSM-5 was shown to have Brønsted acid sites in a concentration equal to the framework Fe concentration. Differential heats of adsorption for ammonia and pyridine were shown to be identical to that obtained in H-[Al]ZSM-5, with differential heats of ∼150 kJ/mol for ammonia and 200 kJ/mol for pyridine. For H-[Al]ZSM-5, adsorption of either propylene or 1-butene at room temperature resulted in rapid oligomerization. TPD–TGA measurements of the oligomers in H-[Al]ZSM-5 showed evidence for hydride-transfer reactions, in addition to simple oligomer cracking. By contrast, it was necessary to heat H-[Fe]ZSM-5 to 370 K for rapid oligomerization of propylene and oligomerization of 1-butene occurred only slowly at 295 K. TPD–TGA measurements of the oligomers in H-[Fe]ZSM-5 showed no evidence for hydride-transfer reactions and H-[Fe]ZSM-5 formed much less coke than H-[Al]ZSM-5 during steady-state reaction in 1-butene at 573 K. Adsorption measurements of 1-butene on D-[Fe]ZSM-5 suggested that the protonated complexes of 1-butene were formed but that these were relatively stable toward reaction, implying that the carbocation transition states were relatively unstable.
publishDate 2002
dc.date.none.fl_str_mv 2002-08
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/39273
Kresnawahjuesa, O.; Kühl, G.H.; Gorte, R.J.; Querini, Carlos Alberto; An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption; Academic Press Inc Elsevier Science; Journal of Catalysis; 210; 1; 8-2002; 106-115
0021-9517
CONICET Digital
CONICET
url http://hdl.handle.net/11336/39273
identifier_str_mv Kresnawahjuesa, O.; Kühl, G.H.; Gorte, R.J.; Querini, Carlos Alberto; An Examination of Brønsted Acid Sites in H-[Fe]ZSM-5 for Olefin Oligomerization and Adsorption; Academic Press Inc Elsevier Science; Journal of Catalysis; 210; 1; 8-2002; 106-115
0021-9517
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1006/jcat.2002.3657
info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0021951702936572
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Academic Press Inc Elsevier Science
publisher.none.fl_str_mv Academic Press Inc Elsevier Science
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.070432

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