Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes

Autores
Grau, Javier Mario; Yori, Juan Carlos; Vera, Carlos Roman; Lovey, Francisco Carlos; Condo, Adriana Maria; Parera, Jose
Año de publicación
2004
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
In order to elucidate the influence of the crystal structure of zirconia on the properties of the metallic and acid function of Pt/SO42−-ZrO2, catalysts with different zirconia crystal phases were synthesized, fully tetragonal, fully monoclinic, and with a mixture of the tetragonal and monoclinic phases. Their catalytic properties were studied in the metal-catalyzed reaction of cyclohexane dehydrogenation (300 °C, 0.1 MPa, , H2/C6H12=30), the acid-catalyzed isomerization of n-butane (350 °C, 0.1 MPa, , H2/C4H10=6), and the bifunctional hydroconversion of n-octane (300 °C, 1.5 MPa, , H2/C8H18=6). TPR, XRD and FTIR of chemisorbed CO were also used in order to characterize the catalysts. The results showed a strong influence of the crystal phase on the activity of the acid function. A less marked effect was found for the metal-catalyzed reaction. An opposite relation between the two functions was seen with respect to this crystal structure influence. Among the sulfated catalysts, monoclinic Pt/SO42−-ZrO2 had the lowest activity in n-C4 isomerization and the highest activity in cyclohexane dehydrogenation. Tetragonal Pt/SO42−-ZrO2 catalysts were the most active in isomerization of n-butane. They had the lowest activity in cyclohexane dehydrogenation and their metal properties were negligible. They were also the most active in n-C8 conversion, producing mainly i-C4. Monoclinic catalysts had low cracking activity and produced mainly isooctane. Mixed phase catalysts had an intermediate behavior. While S poisoning of Pt was present as a uniform effect on all sulfated catalysts, the metal–acid behavior and the different Pt properties could be explained by a metal–support interaction between tetragonal SO42−-ZrO2 and Pt. The Pt–support interaction was analyzed both with a model of Pt particles encapsulation and a model of electron depletion. The electronic deficiency of Pt particles supported on SO42−-ZrO2 was evident in the shift of the IR bands of adsorbed CO. Further experimental work is however needed to get conclusive evidence about the nature of the Pt–support interaction.
Fil: Grau, Javier Mario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Yori, Juan Carlos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Vera, Carlos Roman. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Lovey, Francisco Carlos. Comisión Nacional de Energía Atómica; Argentina
Fil: Condo, Adriana Maria. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Parera, Jose. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Materia
So42−-Zro2
Platinum
Metal–Support Interaction
N-Butane Isomerization
N-Octane Hydroisomerization-Cracking
Metal Function
Acid Function
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:11336/55835
Acceder
id CONICETDig_3b99841ecb54e546f6d014b3a046f66a
oai_identifier_str oai:ri.conicet.gov.ar:11336/55835
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanesGrau, Javier MarioYori, Juan CarlosVera, Carlos RomanLovey, Francisco CarlosCondo, Adriana MariaParera, JoseSo42−-Zro2PlatinumMetal–Support InteractionN-Butane IsomerizationN-Octane Hydroisomerization-CrackingMetal FunctionAcid Functionhttps://purl.org/becyt/ford/2.7https://purl.org/becyt/ford/2In order to elucidate the influence of the crystal structure of zirconia on the properties of the metallic and acid function of Pt/SO42−-ZrO2, catalysts with different zirconia crystal phases were synthesized, fully tetragonal, fully monoclinic, and with a mixture of the tetragonal and monoclinic phases. Their catalytic properties were studied in the metal-catalyzed reaction of cyclohexane dehydrogenation (300 °C, 0.1 MPa, , H2/C6H12=30), the acid-catalyzed isomerization of n-butane (350 °C, 0.1 MPa, , H2/C4H10=6), and the bifunctional hydroconversion of n-octane (300 °C, 1.5 MPa, , H2/C8H18=6). TPR, XRD and FTIR of chemisorbed CO were also used in order to characterize the catalysts. The results showed a strong influence of the crystal phase on the activity of the acid function. A less marked effect was found for the metal-catalyzed reaction. An opposite relation between the two functions was seen with respect to this crystal structure influence. Among the sulfated catalysts, monoclinic Pt/SO42−-ZrO2 had the lowest activity in n-C4 isomerization and the highest activity in cyclohexane dehydrogenation. Tetragonal Pt/SO42−-ZrO2 catalysts were the most active in isomerization of n-butane. They had the lowest activity in cyclohexane dehydrogenation and their metal properties were negligible. They were also the most active in n-C8 conversion, producing mainly i-C4. Monoclinic catalysts had low cracking activity and produced mainly isooctane. Mixed phase catalysts had an intermediate behavior. While S poisoning of Pt was present as a uniform effect on all sulfated catalysts, the metal–acid behavior and the different Pt properties could be explained by a metal–support interaction between tetragonal SO42−-ZrO2 and Pt. The Pt–support interaction was analyzed both with a model of Pt particles encapsulation and a model of electron depletion. The electronic deficiency of Pt particles supported on SO42−-ZrO2 was evident in the shift of the IR bands of adsorbed CO. Further experimental work is however needed to get conclusive evidence about the nature of the Pt–support interaction.Fil: Grau, Javier Mario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Yori, Juan Carlos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Vera, Carlos Roman. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Lovey, Francisco Carlos. Comisión Nacional de Energía Atómica; ArgentinaFil: Condo, Adriana Maria. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Parera, Jose. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaElsevier Science2004-07info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/55835Grau, Javier Mario; Yori, Juan Carlos; Vera, Carlos Roman; Lovey, Francisco Carlos; Condo, Adriana Maria; et al.; Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes; Elsevier Science; Applied Catalysis A: General; 265; 2; 7-2004; 141-1520926-860XCONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2004.01.010info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:54:41Zoai:ri.conicet.gov.ar:11336/55835instacron: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:34982025-09-03 09:54:41.752CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes
title Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes
spellingShingle Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes
Grau, Javier Mario
So42−-Zro2
Platinum
Metal–Support Interaction
N-Butane Isomerization
N-Octane Hydroisomerization-Cracking
Metal Function
Acid Function
title_short Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes
title_full Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes
title_fullStr Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes
title_full_unstemmed Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes
title_sort Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes
dc.creator.none.fl_str_mv Grau, Javier Mario
Yori, Juan Carlos
Vera, Carlos Roman
Lovey, Francisco Carlos
Condo, Adriana Maria
Parera, Jose
author Grau, Javier Mario
author_facet Grau, Javier Mario
Yori, Juan Carlos
Vera, Carlos Roman
Lovey, Francisco Carlos
Condo, Adriana Maria
Parera, Jose
author_role author
author2 Yori, Juan Carlos
Vera, Carlos Roman
Lovey, Francisco Carlos
Condo, Adriana Maria
Parera, Jose
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv So42−-Zro2
Platinum
Metal–Support Interaction
N-Butane Isomerization
N-Octane Hydroisomerization-Cracking
Metal Function
Acid Function
topic So42−-Zro2
Platinum
Metal–Support Interaction
N-Butane Isomerization
N-Octane Hydroisomerization-Cracking
Metal Function
Acid Function
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.7
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv In order to elucidate the influence of the crystal structure of zirconia on the properties of the metallic and acid function of Pt/SO42−-ZrO2, catalysts with different zirconia crystal phases were synthesized, fully tetragonal, fully monoclinic, and with a mixture of the tetragonal and monoclinic phases. Their catalytic properties were studied in the metal-catalyzed reaction of cyclohexane dehydrogenation (300 °C, 0.1 MPa, , H2/C6H12=30), the acid-catalyzed isomerization of n-butane (350 °C, 0.1 MPa, , H2/C4H10=6), and the bifunctional hydroconversion of n-octane (300 °C, 1.5 MPa, , H2/C8H18=6). TPR, XRD and FTIR of chemisorbed CO were also used in order to characterize the catalysts. The results showed a strong influence of the crystal phase on the activity of the acid function. A less marked effect was found for the metal-catalyzed reaction. An opposite relation between the two functions was seen with respect to this crystal structure influence. Among the sulfated catalysts, monoclinic Pt/SO42−-ZrO2 had the lowest activity in n-C4 isomerization and the highest activity in cyclohexane dehydrogenation. Tetragonal Pt/SO42−-ZrO2 catalysts were the most active in isomerization of n-butane. They had the lowest activity in cyclohexane dehydrogenation and their metal properties were negligible. They were also the most active in n-C8 conversion, producing mainly i-C4. Monoclinic catalysts had low cracking activity and produced mainly isooctane. Mixed phase catalysts had an intermediate behavior. While S poisoning of Pt was present as a uniform effect on all sulfated catalysts, the metal–acid behavior and the different Pt properties could be explained by a metal–support interaction between tetragonal SO42−-ZrO2 and Pt. The Pt–support interaction was analyzed both with a model of Pt particles encapsulation and a model of electron depletion. The electronic deficiency of Pt particles supported on SO42−-ZrO2 was evident in the shift of the IR bands of adsorbed CO. Further experimental work is however needed to get conclusive evidence about the nature of the Pt–support interaction.
Fil: Grau, Javier Mario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Yori, Juan Carlos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Vera, Carlos Roman. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Lovey, Francisco Carlos. Comisión Nacional de Energía Atómica; Argentina
Fil: Condo, Adriana Maria. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Parera, Jose. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
description In order to elucidate the influence of the crystal structure of zirconia on the properties of the metallic and acid function of Pt/SO42−-ZrO2, catalysts with different zirconia crystal phases were synthesized, fully tetragonal, fully monoclinic, and with a mixture of the tetragonal and monoclinic phases. Their catalytic properties were studied in the metal-catalyzed reaction of cyclohexane dehydrogenation (300 °C, 0.1 MPa, , H2/C6H12=30), the acid-catalyzed isomerization of n-butane (350 °C, 0.1 MPa, , H2/C4H10=6), and the bifunctional hydroconversion of n-octane (300 °C, 1.5 MPa, , H2/C8H18=6). TPR, XRD and FTIR of chemisorbed CO were also used in order to characterize the catalysts. The results showed a strong influence of the crystal phase on the activity of the acid function. A less marked effect was found for the metal-catalyzed reaction. An opposite relation between the two functions was seen with respect to this crystal structure influence. Among the sulfated catalysts, monoclinic Pt/SO42−-ZrO2 had the lowest activity in n-C4 isomerization and the highest activity in cyclohexane dehydrogenation. Tetragonal Pt/SO42−-ZrO2 catalysts were the most active in isomerization of n-butane. They had the lowest activity in cyclohexane dehydrogenation and their metal properties were negligible. They were also the most active in n-C8 conversion, producing mainly i-C4. Monoclinic catalysts had low cracking activity and produced mainly isooctane. Mixed phase catalysts had an intermediate behavior. While S poisoning of Pt was present as a uniform effect on all sulfated catalysts, the metal–acid behavior and the different Pt properties could be explained by a metal–support interaction between tetragonal SO42−-ZrO2 and Pt. The Pt–support interaction was analyzed both with a model of Pt particles encapsulation and a model of electron depletion. The electronic deficiency of Pt particles supported on SO42−-ZrO2 was evident in the shift of the IR bands of adsorbed CO. Further experimental work is however needed to get conclusive evidence about the nature of the Pt–support interaction.
publishDate 2004
dc.date.none.fl_str_mv 2004-07
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/11336/55835
Grau, Javier Mario; Yori, Juan Carlos; Vera, Carlos Roman; Lovey, Francisco Carlos; Condo, Adriana Maria; et al.; Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes; Elsevier Science; Applied Catalysis A: General; 265; 2; 7-2004; 141-152
0926-860X
CONICET Digital
CONICET
url http://hdl.handle.net/11336/55835
identifier_str_mv Grau, Javier Mario; Yori, Juan Carlos; Vera, Carlos Roman; Lovey, Francisco Carlos; Condo, Adriana Maria; et al.; Crystal phase dependent metal-support interactions in Pt/SO42--ZrO2 catalysts for hydroconversion of n-alkanes; Elsevier Science; Applied Catalysis A: General; 265; 2; 7-2004; 141-152
0926-860X
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2004.01.010
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
application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science
publisher.none.fl_str_mv 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 13.13397

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