Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane

Autores
Costilla, Ignacio Oscar; Sanchez, Miguel Dario; Gigola, Carlos Eugenio
Año de publicación
2014
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Low loaded Pd/α-Al 2 O 3 catalysts (<0.5 wt% Pd) were characterized and tested for CH 4 reforming with CO 2 at 650 °C. The catalysts were prepared by a recharging procedure, using an organometallic precursor, followed by intermediate washing and calcination steps. FTIR spectra of adsorbed CO showed that the Pd surface structure and the particle size were dependent on the number of post-impregnation washing steps. A catalyst sample with a metal dispersion of 33% showing well defined low-index planes (by FTIR) and nearly spherical particles (by TEM) was obtained using two-washing steps. In the reaction, it exhibited a high initial activity followed by a pronounced deactivation due to carbon nanofiber's formation and sintering. TEM analysis of the used catalyst revealed the presence of spherical Pd particles at the end of the fibers that were not attached to the support surface. On the other hand, a high dispersion sample (78%) with a large fraction of Pd atoms with low coordination was obtained by applying three washing steps after impregnation. The presence of small hemispherical particles and larger nearly-flat ones attached to the support were found by TEM. In this case, the catalyst initially showed a very low activity that increased slowly up to a steady value. Although sintering also occurred and the surface structure of the used catalyst resembled the one of the low dispersion catalyst, the amount of carbon formed was quite low. The observed activation under reaction conditions was associated with the slow development of a surface structure that exhibited mainly the (1 0 0) plane favoring methane dissociation. However, the initial interaction of the particles with the support suggested by TEM micrographs seems to remain unaltered despite the particle size increase. Consequently, the process of nanofiber formation and particle separation was inhibited.
Fil: Costilla, Ignacio Oscar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Sanchez, Miguel Dario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Gigola, Carlos Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Materia
Carbon Formation
Catalyst Preparation
Dry Reforming
Particle'S Morphology
Pd (Palladium)
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:11336/77275
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/77275
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methaneCostilla, Ignacio OscarSanchez, Miguel DarioGigola, Carlos EugenioCarbon FormationCatalyst PreparationDry ReformingParticle'S MorphologyPd (Palladium)https://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2https://purl.org/becyt/ford/2.10https://purl.org/becyt/ford/2Low loaded Pd/α-Al 2 O 3 catalysts (<0.5 wt% Pd) were characterized and tested for CH 4 reforming with CO 2 at 650 °C. The catalysts were prepared by a recharging procedure, using an organometallic precursor, followed by intermediate washing and calcination steps. FTIR spectra of adsorbed CO showed that the Pd surface structure and the particle size were dependent on the number of post-impregnation washing steps. A catalyst sample with a metal dispersion of 33% showing well defined low-index planes (by FTIR) and nearly spherical particles (by TEM) was obtained using two-washing steps. In the reaction, it exhibited a high initial activity followed by a pronounced deactivation due to carbon nanofiber's formation and sintering. TEM analysis of the used catalyst revealed the presence of spherical Pd particles at the end of the fibers that were not attached to the support surface. On the other hand, a high dispersion sample (78%) with a large fraction of Pd atoms with low coordination was obtained by applying three washing steps after impregnation. The presence of small hemispherical particles and larger nearly-flat ones attached to the support were found by TEM. In this case, the catalyst initially showed a very low activity that increased slowly up to a steady value. Although sintering also occurred and the surface structure of the used catalyst resembled the one of the low dispersion catalyst, the amount of carbon formed was quite low. The observed activation under reaction conditions was associated with the slow development of a surface structure that exhibited mainly the (1 0 0) plane favoring methane dissociation. However, the initial interaction of the particles with the support suggested by TEM micrographs seems to remain unaltered despite the particle size increase. Consequently, the process of nanofiber formation and particle separation was inhibited.Fil: Costilla, Ignacio Oscar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; ArgentinaFil: Sanchez, Miguel Dario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; ArgentinaFil: Gigola, Carlos Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; ArgentinaElsevier Science2014-05-31info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/77275Costilla, Ignacio Oscar; Sanchez, Miguel Dario; Gigola, Carlos Eugenio; Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane; Elsevier Science; Applied Catalysis A: General; 478; 31-5-2014; 38-440926-860XCONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0926860X14001835info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2014.03.030info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T14:44:46Zoai:ri.conicet.gov.ar:11336/77275instacron: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:34982025-10-15 14:44:47.108CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane
title Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane
spellingShingle Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane
Costilla, Ignacio Oscar
Carbon Formation
Catalyst Preparation
Dry Reforming
Particle'S Morphology
Pd (Palladium)
title_short Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane
title_full Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane
title_fullStr Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane
title_full_unstemmed Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane
title_sort Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane
dc.creator.none.fl_str_mv Costilla, Ignacio Oscar
Sanchez, Miguel Dario
Gigola, Carlos Eugenio
author Costilla, Ignacio Oscar
author_facet Costilla, Ignacio Oscar
Sanchez, Miguel Dario
Gigola, Carlos Eugenio
author_role author
author2 Sanchez, Miguel Dario
Gigola, Carlos Eugenio
author2_role author
author
dc.subject.none.fl_str_mv Carbon Formation
Catalyst Preparation
Dry Reforming
Particle'S Morphology
Pd (Palladium)
topic Carbon Formation
Catalyst Preparation
Dry Reforming
Particle'S Morphology
Pd (Palladium)
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
https://purl.org/becyt/ford/2.10
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv Low loaded Pd/α-Al 2 O 3 catalysts (<0.5 wt% Pd) were characterized and tested for CH 4 reforming with CO 2 at 650 °C. The catalysts were prepared by a recharging procedure, using an organometallic precursor, followed by intermediate washing and calcination steps. FTIR spectra of adsorbed CO showed that the Pd surface structure and the particle size were dependent on the number of post-impregnation washing steps. A catalyst sample with a metal dispersion of 33% showing well defined low-index planes (by FTIR) and nearly spherical particles (by TEM) was obtained using two-washing steps. In the reaction, it exhibited a high initial activity followed by a pronounced deactivation due to carbon nanofiber's formation and sintering. TEM analysis of the used catalyst revealed the presence of spherical Pd particles at the end of the fibers that were not attached to the support surface. On the other hand, a high dispersion sample (78%) with a large fraction of Pd atoms with low coordination was obtained by applying three washing steps after impregnation. The presence of small hemispherical particles and larger nearly-flat ones attached to the support were found by TEM. In this case, the catalyst initially showed a very low activity that increased slowly up to a steady value. Although sintering also occurred and the surface structure of the used catalyst resembled the one of the low dispersion catalyst, the amount of carbon formed was quite low. The observed activation under reaction conditions was associated with the slow development of a surface structure that exhibited mainly the (1 0 0) plane favoring methane dissociation. However, the initial interaction of the particles with the support suggested by TEM micrographs seems to remain unaltered despite the particle size increase. Consequently, the process of nanofiber formation and particle separation was inhibited.
Fil: Costilla, Ignacio Oscar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Sanchez, Miguel Dario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Gigola, Carlos Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
description Low loaded Pd/α-Al 2 O 3 catalysts (<0.5 wt% Pd) were characterized and tested for CH 4 reforming with CO 2 at 650 °C. The catalysts were prepared by a recharging procedure, using an organometallic precursor, followed by intermediate washing and calcination steps. FTIR spectra of adsorbed CO showed that the Pd surface structure and the particle size were dependent on the number of post-impregnation washing steps. A catalyst sample with a metal dispersion of 33% showing well defined low-index planes (by FTIR) and nearly spherical particles (by TEM) was obtained using two-washing steps. In the reaction, it exhibited a high initial activity followed by a pronounced deactivation due to carbon nanofiber's formation and sintering. TEM analysis of the used catalyst revealed the presence of spherical Pd particles at the end of the fibers that were not attached to the support surface. On the other hand, a high dispersion sample (78%) with a large fraction of Pd atoms with low coordination was obtained by applying three washing steps after impregnation. The presence of small hemispherical particles and larger nearly-flat ones attached to the support were found by TEM. In this case, the catalyst initially showed a very low activity that increased slowly up to a steady value. Although sintering also occurred and the surface structure of the used catalyst resembled the one of the low dispersion catalyst, the amount of carbon formed was quite low. The observed activation under reaction conditions was associated with the slow development of a surface structure that exhibited mainly the (1 0 0) plane favoring methane dissociation. However, the initial interaction of the particles with the support suggested by TEM micrographs seems to remain unaltered despite the particle size increase. Consequently, the process of nanofiber formation and particle separation was inhibited.
publishDate 2014
dc.date.none.fl_str_mv 2014-05-31
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/11336/77275
Costilla, Ignacio Oscar; Sanchez, Miguel Dario; Gigola, Carlos Eugenio; Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane; Elsevier Science; Applied Catalysis A: General; 478; 31-5-2014; 38-44
0926-860X
CONICET Digital
CONICET
url http://hdl.handle.net/11336/77275
identifier_str_mv Costilla, Ignacio Oscar; Sanchez, Miguel Dario; Gigola, Carlos Eugenio; Palladium nanoparticle's surface structure and morphology effect on the catalytic activity for dry reforming of methane; Elsevier Science; Applied Catalysis A: General; 478; 31-5-2014; 38-44
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/url/https://www.sciencedirect.com/science/article/pii/S0926860X14001835
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2014.03.030
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
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 13.22299

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