Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports

Autores
Garetto, Teresita Francisca; Rincon, Eduardo Ricardo; Apesteguia, Carlos Rodolfo
Año de publicación
2004
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The combustion of propane was studied on Pt supported on MgO, alumina, and zeolites KL, HY, ZSM5 and Beta. Samples contained a similar amount of Pt, between 0.32 and 0.44%, and were characterized by employing a variety of physical and spectroscopic techniques. The catalyst activities were evaluated through both conversion versus temperature (light-off curves) and conversion versus time catalytic tests. Kinetic studies showed that the reaction is first order in propane, and zero (Pt/Al2O3, Pt/MgO) or negative (Pt/zeolites) orders in oxygen. Apparent activation energies (Ea) and pre-exponential factors (A) were determined and it was verified that the experimental data obey a Constable relation (ln A = mEa + c). Pt/Al2O3 catalysts of different metallic dispersions were prepared for investigating the effect of Pt crystallite size on combustion activity. It was found that propane oxidation is a structure insensitive reaction on Pt/Al2O3. Propane oxidation turnover rates (TOF) followed the order: Pt/MgO < Pt/Al2O3 Pt/KL < Pt/HY ≤ Pt/ZSM5 < Pt/Beta. The TOF values on Pt/acid zeolites were more than two orders of magnitude higher than on Pt/Al2O3. Propane oxidation activity was also significantly higher on Pt/KL as compared to Pt/Al2O3, despite that Al2O3 and zeolite KL supports exhibited similar acid sites density and strength. This result showed that the support acid strength did not have a major influence on propane combustion activity. Areal propane uptake was more than one order of magnitude higher on Pt/zeolites than on Pt/Al2O3 and this drastic increase in the density of propane adsorbed species may promote the alkane oxidation rate. It is proposed that the enhanced combustion activity obtained on Pt/zeolites is associated with an additional oxidation pathway from propane adsorbing on the metal-oxide interface region and reacting with oxygen spilled-over from the metal surface.
Fil: Garetto, Teresita Francisca. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Rincon, Eduardo Ricardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Apesteguia, Carlos Rodolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Materia
Propane Combustion
Pt Catalysts
Acid Zeolites
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:11336/55840

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oai_identifier_str oai:ri.conicet.gov.ar:11336/55840
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network_name_str CONICET Digital (CONICET)
spelling Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supportsGaretto, Teresita FranciscaRincon, Eduardo RicardoApesteguia, Carlos RodolfoPropane CombustionPt CatalystsAcid Zeoliteshttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2The combustion of propane was studied on Pt supported on MgO, alumina, and zeolites KL, HY, ZSM5 and Beta. Samples contained a similar amount of Pt, between 0.32 and 0.44%, and were characterized by employing a variety of physical and spectroscopic techniques. The catalyst activities were evaluated through both conversion versus temperature (light-off curves) and conversion versus time catalytic tests. Kinetic studies showed that the reaction is first order in propane, and zero (Pt/Al2O3, Pt/MgO) or negative (Pt/zeolites) orders in oxygen. Apparent activation energies (Ea) and pre-exponential factors (A) were determined and it was verified that the experimental data obey a Constable relation (ln A = mEa + c). Pt/Al2O3 catalysts of different metallic dispersions were prepared for investigating the effect of Pt crystallite size on combustion activity. It was found that propane oxidation is a structure insensitive reaction on Pt/Al2O3. Propane oxidation turnover rates (TOF) followed the order: Pt/MgO < Pt/Al2O3 Pt/KL < Pt/HY ≤ Pt/ZSM5 < Pt/Beta. The TOF values on Pt/acid zeolites were more than two orders of magnitude higher than on Pt/Al2O3. Propane oxidation activity was also significantly higher on Pt/KL as compared to Pt/Al2O3, despite that Al2O3 and zeolite KL supports exhibited similar acid sites density and strength. This result showed that the support acid strength did not have a major influence on propane combustion activity. Areal propane uptake was more than one order of magnitude higher on Pt/zeolites than on Pt/Al2O3 and this drastic increase in the density of propane adsorbed species may promote the alkane oxidation rate. It is proposed that the enhanced combustion activity obtained on Pt/zeolites is associated with an additional oxidation pathway from propane adsorbing on the metal-oxide interface region and reacting with oxygen spilled-over from the metal surface.Fil: Garetto, Teresita Francisca. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Rincon, Eduardo Ricardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Apesteguia, Carlos Rodolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaElsevier Science2004-03info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/55840Garetto, Teresita Francisca; Rincon, Eduardo Ricardo; Apesteguia, Carlos Rodolfo; Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports; Elsevier Science; Applied Catalysis B: Environmental; 48; 3; 3-2004; 167-1740926-3373CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://dx.doi.org/10.1016/j.apcatb.2003.10.004info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:20:31Zoai:ri.conicet.gov.ar:11336/55840instacron: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 10:20:31.329CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports
title Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports
spellingShingle Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports
Garetto, Teresita Francisca
Propane Combustion
Pt Catalysts
Acid Zeolites
title_short Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports
title_full Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports
title_fullStr Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports
title_full_unstemmed Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports
title_sort Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports
dc.creator.none.fl_str_mv Garetto, Teresita Francisca
Rincon, Eduardo Ricardo
Apesteguia, Carlos Rodolfo
author Garetto, Teresita Francisca
author_facet Garetto, Teresita Francisca
Rincon, Eduardo Ricardo
Apesteguia, Carlos Rodolfo
author_role author
author2 Rincon, Eduardo Ricardo
Apesteguia, Carlos Rodolfo
author2_role author
author
dc.subject.none.fl_str_mv Propane Combustion
Pt Catalysts
Acid Zeolites
topic Propane Combustion
Pt Catalysts
Acid Zeolites
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 combustion of propane was studied on Pt supported on MgO, alumina, and zeolites KL, HY, ZSM5 and Beta. Samples contained a similar amount of Pt, between 0.32 and 0.44%, and were characterized by employing a variety of physical and spectroscopic techniques. The catalyst activities were evaluated through both conversion versus temperature (light-off curves) and conversion versus time catalytic tests. Kinetic studies showed that the reaction is first order in propane, and zero (Pt/Al2O3, Pt/MgO) or negative (Pt/zeolites) orders in oxygen. Apparent activation energies (Ea) and pre-exponential factors (A) were determined and it was verified that the experimental data obey a Constable relation (ln A = mEa + c). Pt/Al2O3 catalysts of different metallic dispersions were prepared for investigating the effect of Pt crystallite size on combustion activity. It was found that propane oxidation is a structure insensitive reaction on Pt/Al2O3. Propane oxidation turnover rates (TOF) followed the order: Pt/MgO < Pt/Al2O3 Pt/KL < Pt/HY ≤ Pt/ZSM5 < Pt/Beta. The TOF values on Pt/acid zeolites were more than two orders of magnitude higher than on Pt/Al2O3. Propane oxidation activity was also significantly higher on Pt/KL as compared to Pt/Al2O3, despite that Al2O3 and zeolite KL supports exhibited similar acid sites density and strength. This result showed that the support acid strength did not have a major influence on propane combustion activity. Areal propane uptake was more than one order of magnitude higher on Pt/zeolites than on Pt/Al2O3 and this drastic increase in the density of propane adsorbed species may promote the alkane oxidation rate. It is proposed that the enhanced combustion activity obtained on Pt/zeolites is associated with an additional oxidation pathway from propane adsorbing on the metal-oxide interface region and reacting with oxygen spilled-over from the metal surface.
Fil: Garetto, Teresita Francisca. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Rincon, Eduardo Ricardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Apesteguia, Carlos Rodolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
description The combustion of propane was studied on Pt supported on MgO, alumina, and zeolites KL, HY, ZSM5 and Beta. Samples contained a similar amount of Pt, between 0.32 and 0.44%, and were characterized by employing a variety of physical and spectroscopic techniques. The catalyst activities were evaluated through both conversion versus temperature (light-off curves) and conversion versus time catalytic tests. Kinetic studies showed that the reaction is first order in propane, and zero (Pt/Al2O3, Pt/MgO) or negative (Pt/zeolites) orders in oxygen. Apparent activation energies (Ea) and pre-exponential factors (A) were determined and it was verified that the experimental data obey a Constable relation (ln A = mEa + c). Pt/Al2O3 catalysts of different metallic dispersions were prepared for investigating the effect of Pt crystallite size on combustion activity. It was found that propane oxidation is a structure insensitive reaction on Pt/Al2O3. Propane oxidation turnover rates (TOF) followed the order: Pt/MgO < Pt/Al2O3 Pt/KL < Pt/HY ≤ Pt/ZSM5 < Pt/Beta. The TOF values on Pt/acid zeolites were more than two orders of magnitude higher than on Pt/Al2O3. Propane oxidation activity was also significantly higher on Pt/KL as compared to Pt/Al2O3, despite that Al2O3 and zeolite KL supports exhibited similar acid sites density and strength. This result showed that the support acid strength did not have a major influence on propane combustion activity. Areal propane uptake was more than one order of magnitude higher on Pt/zeolites than on Pt/Al2O3 and this drastic increase in the density of propane adsorbed species may promote the alkane oxidation rate. It is proposed that the enhanced combustion activity obtained on Pt/zeolites is associated with an additional oxidation pathway from propane adsorbing on the metal-oxide interface region and reacting with oxygen spilled-over from the metal surface.
publishDate 2004
dc.date.none.fl_str_mv 2004-03
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/11336/55840
Garetto, Teresita Francisca; Rincon, Eduardo Ricardo; Apesteguia, Carlos Rodolfo; Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports; Elsevier Science; Applied Catalysis B: Environmental; 48; 3; 3-2004; 167-174
0926-3373
CONICET Digital
CONICET
url http://hdl.handle.net/11336/55840
identifier_str_mv Garetto, Teresita Francisca; Rincon, Eduardo Ricardo; Apesteguia, Carlos Rodolfo; Deep oxidation of propane on Pt-supported catalysts: Drastic turnover rate enhancement using zeolite supports; Elsevier Science; Applied Catalysis B: Environmental; 48; 3; 3-2004; 167-174
0926-3373
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://dx.doi.org/10.1016/j.apcatb.2003.10.004
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
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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