Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content

Autores
Mariscal, Rafael; García Fierro, José Luis; Yori, Juan Carlos; Parera, Jose; Grau, Javier Mario
Año de publicación
2007
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The effect of the Pt/Ge atomic ratio on the catalytic activity of PtGe/Al2O3 catalysts used in n-heptane reforming was studied. The samples were prepared by the coimpregnation method on chlorinated alumina. The platinum content was 0.5 wt.%, and Ge-loading was varied to obtain Pt/Ge atomic ratios of 0.3, 0.7, 1.4, 2.1 and 3.5. Pt/Al2O3 and Ge/Al2O3 catalysts were also prepared as references. Characterization was carried out by temperature-programmed reduction (TPR), temperature-programmed desorption of ammonia (NH3-TPD), Fourier transform IR spectroscopy (FTIR) with CO as the probe molecule, X-ray photoelectron spectroscopy (XPS), cyclohexane (CH) dehydrogenation, and n-heptane reforming. The preparation method followed in this work revealed a decrease in the metallic activity of Pt due to the presence of Ge. The Ge2+ and Ge4+ species, after reduction at 500 °C, were detected on the surface of PtGe catalysts. The increase in the Ge content led to a decrease in hydrogenolysis activity and the formation of aromatics; an increase in the formation of isomers and cycloparaffins, and a reduction in the production of gas and in deactivation by coke, thereby improving catalyst stability. The results show that the maximum isoparaffin yield of all catalysts tested was obtained for a Ge-loading of 0.27 wt.% (Pt/Ge atomic ratio = 0.7). These changes in the performance of the PtGe catalysts may be attributed to the modifications occurring in the metallic and in the acid function of Pt/Al2O3 due to the introduction of Ge. The metallic catalytic activity of Pt is modified by the geometrical effect (dilution of Pt ensembles) and changes in the electronic properties of platinum. Ge addition produces a weakening of Pt/Al2O3 acid strength and an increase in the acid sites total density by the presence of Ge oxides.
Fil: Mariscal, Rafael. Instituto de Catálisis y Petroleoquímica; España
Fil: García Fierro, José Luis. Instituto de Catálisis y Petroleoquímica; España
Fil: Yori, Juan Carlos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Fil: Parera, Jose. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Fil: Grau, Javier Mario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Materia
N-Heptane Reforming
Isoparaffin Selectivity
Pt/Ge Atomic Ratio Optimization
Electronic Effect
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:11336/65257
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/65257
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge contentMariscal, RafaelGarcía Fierro, José LuisYori, Juan CarlosParera, JoseGrau, Javier MarioN-Heptane ReformingIsoparaffin SelectivityPt/Ge Atomic Ratio OptimizationElectronic Effecthttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2The effect of the Pt/Ge atomic ratio on the catalytic activity of PtGe/Al2O3 catalysts used in n-heptane reforming was studied. The samples were prepared by the coimpregnation method on chlorinated alumina. The platinum content was 0.5 wt.%, and Ge-loading was varied to obtain Pt/Ge atomic ratios of 0.3, 0.7, 1.4, 2.1 and 3.5. Pt/Al2O3 and Ge/Al2O3 catalysts were also prepared as references. Characterization was carried out by temperature-programmed reduction (TPR), temperature-programmed desorption of ammonia (NH3-TPD), Fourier transform IR spectroscopy (FTIR) with CO as the probe molecule, X-ray photoelectron spectroscopy (XPS), cyclohexane (CH) dehydrogenation, and n-heptane reforming. The preparation method followed in this work revealed a decrease in the metallic activity of Pt due to the presence of Ge. The Ge2+ and Ge4+ species, after reduction at 500 °C, were detected on the surface of PtGe catalysts. The increase in the Ge content led to a decrease in hydrogenolysis activity and the formation of aromatics; an increase in the formation of isomers and cycloparaffins, and a reduction in the production of gas and in deactivation by coke, thereby improving catalyst stability. The results show that the maximum isoparaffin yield of all catalysts tested was obtained for a Ge-loading of 0.27 wt.% (Pt/Ge atomic ratio = 0.7). These changes in the performance of the PtGe catalysts may be attributed to the modifications occurring in the metallic and in the acid function of Pt/Al2O3 due to the introduction of Ge. The metallic catalytic activity of Pt is modified by the geometrical effect (dilution of Pt ensembles) and changes in the electronic properties of platinum. Ge addition produces a weakening of Pt/Al2O3 acid strength and an increase in the acid sites total density by the presence of Ge oxides.Fil: Mariscal, Rafael. Instituto de Catálisis y Petroleoquímica; EspañaFil: García Fierro, José Luis. Instituto de Catálisis y Petroleoquímica; EspañaFil: Yori, Juan Carlos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; ArgentinaFil: Parera, Jose. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; ArgentinaFil: Grau, Javier Mario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; ArgentinaElsevier Science2007-08info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/65257Mariscal, Rafael; García Fierro, José Luis; Yori, Juan Carlos; Parera, Jose; Grau, Javier Mario; Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content; Elsevier Science; Applied Catalysis A: General; 327; 2; 8-2007; 123-1310926-860XCONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2007.05.007info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:52:46Zoai:ri.conicet.gov.ar:11336/65257instacron: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 09:52:46.668CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content
title Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content
spellingShingle Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content
Mariscal, Rafael
N-Heptane Reforming
Isoparaffin Selectivity
Pt/Ge Atomic Ratio Optimization
Electronic Effect
title_short Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content
title_full Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content
title_fullStr Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content
title_full_unstemmed Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content
title_sort Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content
dc.creator.none.fl_str_mv Mariscal, Rafael
García Fierro, José Luis
Yori, Juan Carlos
Parera, Jose
Grau, Javier Mario
author Mariscal, Rafael
author_facet Mariscal, Rafael
García Fierro, José Luis
Yori, Juan Carlos
Parera, Jose
Grau, Javier Mario
author_role author
author2 García Fierro, José Luis
Yori, Juan Carlos
Parera, Jose
Grau, Javier Mario
author2_role author
author
author
author
dc.subject.none.fl_str_mv N-Heptane Reforming
Isoparaffin Selectivity
Pt/Ge Atomic Ratio Optimization
Electronic Effect
topic N-Heptane Reforming
Isoparaffin Selectivity
Pt/Ge Atomic Ratio Optimization
Electronic Effect
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv The effect of the Pt/Ge atomic ratio on the catalytic activity of PtGe/Al2O3 catalysts used in n-heptane reforming was studied. The samples were prepared by the coimpregnation method on chlorinated alumina. The platinum content was 0.5 wt.%, and Ge-loading was varied to obtain Pt/Ge atomic ratios of 0.3, 0.7, 1.4, 2.1 and 3.5. Pt/Al2O3 and Ge/Al2O3 catalysts were also prepared as references. Characterization was carried out by temperature-programmed reduction (TPR), temperature-programmed desorption of ammonia (NH3-TPD), Fourier transform IR spectroscopy (FTIR) with CO as the probe molecule, X-ray photoelectron spectroscopy (XPS), cyclohexane (CH) dehydrogenation, and n-heptane reforming. The preparation method followed in this work revealed a decrease in the metallic activity of Pt due to the presence of Ge. The Ge2+ and Ge4+ species, after reduction at 500 °C, were detected on the surface of PtGe catalysts. The increase in the Ge content led to a decrease in hydrogenolysis activity and the formation of aromatics; an increase in the formation of isomers and cycloparaffins, and a reduction in the production of gas and in deactivation by coke, thereby improving catalyst stability. The results show that the maximum isoparaffin yield of all catalysts tested was obtained for a Ge-loading of 0.27 wt.% (Pt/Ge atomic ratio = 0.7). These changes in the performance of the PtGe catalysts may be attributed to the modifications occurring in the metallic and in the acid function of Pt/Al2O3 due to the introduction of Ge. The metallic catalytic activity of Pt is modified by the geometrical effect (dilution of Pt ensembles) and changes in the electronic properties of platinum. Ge addition produces a weakening of Pt/Al2O3 acid strength and an increase in the acid sites total density by the presence of Ge oxides.
Fil: Mariscal, Rafael. Instituto de Catálisis y Petroleoquímica; España
Fil: García Fierro, José Luis. Instituto de Catálisis y Petroleoquímica; España
Fil: Yori, Juan Carlos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Fil: Parera, Jose. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Fil: Grau, Javier Mario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
description The effect of the Pt/Ge atomic ratio on the catalytic activity of PtGe/Al2O3 catalysts used in n-heptane reforming was studied. The samples were prepared by the coimpregnation method on chlorinated alumina. The platinum content was 0.5 wt.%, and Ge-loading was varied to obtain Pt/Ge atomic ratios of 0.3, 0.7, 1.4, 2.1 and 3.5. Pt/Al2O3 and Ge/Al2O3 catalysts were also prepared as references. Characterization was carried out by temperature-programmed reduction (TPR), temperature-programmed desorption of ammonia (NH3-TPD), Fourier transform IR spectroscopy (FTIR) with CO as the probe molecule, X-ray photoelectron spectroscopy (XPS), cyclohexane (CH) dehydrogenation, and n-heptane reforming. The preparation method followed in this work revealed a decrease in the metallic activity of Pt due to the presence of Ge. The Ge2+ and Ge4+ species, after reduction at 500 °C, were detected on the surface of PtGe catalysts. The increase in the Ge content led to a decrease in hydrogenolysis activity and the formation of aromatics; an increase in the formation of isomers and cycloparaffins, and a reduction in the production of gas and in deactivation by coke, thereby improving catalyst stability. The results show that the maximum isoparaffin yield of all catalysts tested was obtained for a Ge-loading of 0.27 wt.% (Pt/Ge atomic ratio = 0.7). These changes in the performance of the PtGe catalysts may be attributed to the modifications occurring in the metallic and in the acid function of Pt/Al2O3 due to the introduction of Ge. The metallic catalytic activity of Pt is modified by the geometrical effect (dilution of Pt ensembles) and changes in the electronic properties of platinum. Ge addition produces a weakening of Pt/Al2O3 acid strength and an increase in the acid sites total density by the presence of Ge oxides.
publishDate 2007
dc.date.none.fl_str_mv 2007-08
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/11336/65257
Mariscal, Rafael; García Fierro, José Luis; Yori, Juan Carlos; Parera, Jose; Grau, Javier Mario; Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content; Elsevier Science; Applied Catalysis A: General; 327; 2; 8-2007; 123-131
0926-860X
CONICET Digital
CONICET
url http://hdl.handle.net/11336/65257
identifier_str_mv Mariscal, Rafael; García Fierro, José Luis; Yori, Juan Carlos; Parera, Jose; Grau, Javier Mario; Evolution of the properties of PtGe/Al2O3 reforming catalysts with Ge content; Elsevier Science; Applied Catalysis A: General; 327; 2; 8-2007; 123-131
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.2007.05.007
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 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 13.070432

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