XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions

Autores
Zimicz, Maria Genoveva; Prado, Fernando Daniel; Soldati, Analía Leticia; Lamas, Diego Germán; Larrondo, Susana Adelina
Año de publicación
2015
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The aim of this work is to take further insight into the structural stability of cerium-zirconium catalysts under reducing, oxidizing and reaction conditions. In situ synchrotron based techniques (XANES and XPD) were used in order to determine the stability of crystal structure and the oxidation state of cerium cations in the reaction conditions prevailing in the catalytic studies. In situ XPD studies in 5 mol % H2 atmosphere revealed that no structural changes occur until 870 °C. At this temperature, the sample synthesized with glycine, which presents lower crystallite agglomeration, segregated a small quantity of a reduced phase. On the contrary, the solid synthesized with lysine, with more agglomerated crystallites, does not show structural changes in all the temperature range. Reoxidation treatments in 5 mol % O2 revealed that at 750 °C the segregated phase disappears and that the original cubic structure is restored. In situ XANES studies in the Ce LIII absorption edge indicate that under catalytic reaction conditions, the degree of reduction of Ce4+ is low, allowing the occurrence of methane oxidation. The solid is capable to deliver the oxygen of its structure when no oxygen is fed into the reactor until the 50% of cerium cations become reduced, triggering the deactivation process. Therefore, it is clear for these studies that the Ce4+ to Ce3+ ratio in the lattice is governing the catalytic behavior of the solid. The catalytic results collected during in situ XANES experiments are in excellent agreement with our previous catalytic studies performed with a laboratory fixed bed reactor.
Fil: Zimicz, Maria Genoveva. 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: Prado, Fernando Daniel. 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: Soldati, Analía Leticia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina. Comisión Nacional de Energía Atómica. Gerencia del Área de Energía Nuclear. Instituto Balseiro; Argentina
Fil: Lamas, Diego Germán. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina
Fil: Larrondo, Susana Adelina. Consejo Nacional de Investigaciones Científicas y Técnicas. Unidad de Investigación y Desarrollo Estratégico para la Defensa. Ministerio de Defensa. Unidad de Investigación y Desarrollo Estratégico para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Instituto de Investigaciones Científicas y Técnicas de las Fuerzas Armadas. Centro de Investigaciones en Sólidos; Argentina. Universidad Nacional de San Martín. Instituto de Investigación en Ingeniería Ambiental; Argentina
Materia
Catalysis
ZrO2-CeO2
CH4 oxidation
XPD
XANES
Nivel de accesibilidad
acceso abierto
Condiciones de uso
Atribución-NoComercial-CompartirIgual 2.5 Argentina (CC 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:11336/85526
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/85526
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repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation ConditionsZimicz, Maria GenovevaPrado, Fernando DanielSoldati, Analía LeticiaLamas, Diego GermánLarrondo, Susana AdelinaCatalysisZrO2-CeO2CH4 oxidationXPDXANEShttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2The aim of this work is to take further insight into the structural stability of cerium-zirconium catalysts under reducing, oxidizing and reaction conditions. In situ synchrotron based techniques (XANES and XPD) were used in order to determine the stability of crystal structure and the oxidation state of cerium cations in the reaction conditions prevailing in the catalytic studies. In situ XPD studies in 5 mol % H2 atmosphere revealed that no structural changes occur until 870 °C. At this temperature, the sample synthesized with glycine, which presents lower crystallite agglomeration, segregated a small quantity of a reduced phase. On the contrary, the solid synthesized with lysine, with more agglomerated crystallites, does not show structural changes in all the temperature range. Reoxidation treatments in 5 mol % O2 revealed that at 750 °C the segregated phase disappears and that the original cubic structure is restored. In situ XANES studies in the Ce LIII absorption edge indicate that under catalytic reaction conditions, the degree of reduction of Ce4+ is low, allowing the occurrence of methane oxidation. The solid is capable to deliver the oxygen of its structure when no oxygen is fed into the reactor until the 50% of cerium cations become reduced, triggering the deactivation process. Therefore, it is clear for these studies that the Ce4+ to Ce3+ ratio in the lattice is governing the catalytic behavior of the solid. The catalytic results collected during in situ XANES experiments are in excellent agreement with our previous catalytic studies performed with a laboratory fixed bed reactor.Fil: Zimicz, Maria Genoveva. 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: Prado, Fernando Daniel. 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: Soldati, Analía Leticia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina. Comisión Nacional de Energía Atómica. Gerencia del Área de Energía Nuclear. Instituto Balseiro; ArgentinaFil: Lamas, Diego Germán. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; ArgentinaFil: Larrondo, Susana Adelina. Consejo Nacional de Investigaciones Científicas y Técnicas. Unidad de Investigación y Desarrollo Estratégico para la Defensa. Ministerio de Defensa. Unidad de Investigación y Desarrollo Estratégico para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Instituto de Investigaciones Científicas y Técnicas de las Fuerzas Armadas. Centro de Investigaciones en Sólidos; Argentina. Universidad Nacional de San Martín. Instituto de Investigación en Ingeniería Ambiental; ArgentinaAmerican Chemical Society2015-08-28info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/85526Zimicz, Maria Genoveva; Prado, Fernando Daniel; Soldati, Analía Leticia; Lamas, Diego Germán; Larrondo, Susana Adelina; XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions; American Chemical Society; Journal of Physical Chemistry C; 119; 33; 28-8-2015; 19210-192171932-7447CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpcc.5b05253info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpcc.5b05253info:eu-repo/semantics/openAccessAtribución-NoComercial-CompartirIgual 2.5 Argentina (CC BY-NC-SA 2.5 AR)https://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:46:26Zoai:ri.conicet.gov.ar:11336/85526instacron: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 09:46:27.205CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions
title XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions
spellingShingle XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions
Zimicz, Maria Genoveva
Catalysis
ZrO2-CeO2
CH4 oxidation
XPD
XANES
title_short XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions
title_full XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions
title_fullStr XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions
title_full_unstemmed XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions
title_sort XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions
dc.creator.none.fl_str_mv Zimicz, Maria Genoveva
Prado, Fernando Daniel
Soldati, Analía Leticia
Lamas, Diego Germán
Larrondo, Susana Adelina
author Zimicz, Maria Genoveva
author_facet Zimicz, Maria Genoveva
Prado, Fernando Daniel
Soldati, Analía Leticia
Lamas, Diego Germán
Larrondo, Susana Adelina
author_role author
author2 Prado, Fernando Daniel
Soldati, Analía Leticia
Lamas, Diego Germán
Larrondo, Susana Adelina
author2_role author
author
author
author
dc.subject.none.fl_str_mv Catalysis
ZrO2-CeO2
CH4 oxidation
XPD
XANES
topic Catalysis
ZrO2-CeO2
CH4 oxidation
XPD
XANES
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv The aim of this work is to take further insight into the structural stability of cerium-zirconium catalysts under reducing, oxidizing and reaction conditions. In situ synchrotron based techniques (XANES and XPD) were used in order to determine the stability of crystal structure and the oxidation state of cerium cations in the reaction conditions prevailing in the catalytic studies. In situ XPD studies in 5 mol % H2 atmosphere revealed that no structural changes occur until 870 °C. At this temperature, the sample synthesized with glycine, which presents lower crystallite agglomeration, segregated a small quantity of a reduced phase. On the contrary, the solid synthesized with lysine, with more agglomerated crystallites, does not show structural changes in all the temperature range. Reoxidation treatments in 5 mol % O2 revealed that at 750 °C the segregated phase disappears and that the original cubic structure is restored. In situ XANES studies in the Ce LIII absorption edge indicate that under catalytic reaction conditions, the degree of reduction of Ce4+ is low, allowing the occurrence of methane oxidation. The solid is capable to deliver the oxygen of its structure when no oxygen is fed into the reactor until the 50% of cerium cations become reduced, triggering the deactivation process. Therefore, it is clear for these studies that the Ce4+ to Ce3+ ratio in the lattice is governing the catalytic behavior of the solid. The catalytic results collected during in situ XANES experiments are in excellent agreement with our previous catalytic studies performed with a laboratory fixed bed reactor.
Fil: Zimicz, Maria Genoveva. 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: Prado, Fernando Daniel. 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: Soldati, Analía Leticia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina. Comisión Nacional de Energía Atómica. Gerencia del Área de Energía Nuclear. Instituto Balseiro; Argentina
Fil: Lamas, Diego Germán. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina
Fil: Larrondo, Susana Adelina. Consejo Nacional de Investigaciones Científicas y Técnicas. Unidad de Investigación y Desarrollo Estratégico para la Defensa. Ministerio de Defensa. Unidad de Investigación y Desarrollo Estratégico para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Instituto de Investigaciones Científicas y Técnicas de las Fuerzas Armadas. Centro de Investigaciones en Sólidos; Argentina. Universidad Nacional de San Martín. Instituto de Investigación en Ingeniería Ambiental; Argentina
description The aim of this work is to take further insight into the structural stability of cerium-zirconium catalysts under reducing, oxidizing and reaction conditions. In situ synchrotron based techniques (XANES and XPD) were used in order to determine the stability of crystal structure and the oxidation state of cerium cations in the reaction conditions prevailing in the catalytic studies. In situ XPD studies in 5 mol % H2 atmosphere revealed that no structural changes occur until 870 °C. At this temperature, the sample synthesized with glycine, which presents lower crystallite agglomeration, segregated a small quantity of a reduced phase. On the contrary, the solid synthesized with lysine, with more agglomerated crystallites, does not show structural changes in all the temperature range. Reoxidation treatments in 5 mol % O2 revealed that at 750 °C the segregated phase disappears and that the original cubic structure is restored. In situ XANES studies in the Ce LIII absorption edge indicate that under catalytic reaction conditions, the degree of reduction of Ce4+ is low, allowing the occurrence of methane oxidation. The solid is capable to deliver the oxygen of its structure when no oxygen is fed into the reactor until the 50% of cerium cations become reduced, triggering the deactivation process. Therefore, it is clear for these studies that the Ce4+ to Ce3+ ratio in the lattice is governing the catalytic behavior of the solid. The catalytic results collected during in situ XANES experiments are in excellent agreement with our previous catalytic studies performed with a laboratory fixed bed reactor.
publishDate 2015
dc.date.none.fl_str_mv 2015-08-28
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/11336/85526
Zimicz, Maria Genoveva; Prado, Fernando Daniel; Soldati, Analía Leticia; Lamas, Diego Germán; Larrondo, Susana Adelina; XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions; American Chemical Society; Journal of Physical Chemistry C; 119; 33; 28-8-2015; 19210-19217
1932-7447
CONICET Digital
CONICET
url http://hdl.handle.net/11336/85526
identifier_str_mv Zimicz, Maria Genoveva; Prado, Fernando Daniel; Soldati, Analía Leticia; Lamas, Diego Germán; Larrondo, Susana Adelina; XPD and XANES Studies of Ce0.9Zr0.1O2 Nanocatalysts under Redox and Catalytic CH4 Oxidation Conditions; American Chemical Society; Journal of Physical Chemistry C; 119; 33; 28-8-2015; 19210-19217
1932-7447
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpcc.5b05253
info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpcc.5b05253
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
Atribución-NoComercial-CompartirIgual 2.5 Argentina (CC BY-NC-SA 2.5 AR)
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv Atribución-NoComercial-CompartirIgual 2.5 Argentina (CC BY-NC-SA 2.5 AR)
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
application/pdf
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application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
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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