In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane

Autores
Toscani, Lucía María; Zimicz, Maria Genoveva; Martins, Tereza S.; Lamas, Diego Germán; Larrondo, Susana Adelina
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
In this work we analyze the effect of adding CuO to a NiO/Ce0.9Zr0.1O2 oxide by in situ X-ray absorption near-edge structure XANES technique in Ce L3, Ni K and Cu K absorption edges in terms of sample reducibility and catalytic activity. The oxidation states of Ce, Ni and Cu cations are followed up during temperature programmed reduction (TPR) experiments in diluted hydrogen and during catalytic tests for partial oxidation of methane (POM) reaction. Redox behavior was correlated to conventional fixed bed reactor results. The effect of firing temperature, crystallite size, CeO2-ZrO2 support and the presence of Cu and/or Ni as an active phase is also analyzed. Results showed a beneficial effect of CuO addition in terms of Ce and Ni reduction. A stronger interaction of NiO species with the support was revealed upon analysis of XANES reduction profiles in sample NiO/ZDC in contrast to bimetallic CuO-NiO/ZDC sample. Reduction onset temperature was found to depend on Ni crystallite size, being markedly promoted when samples exhibited low values of crystallite size both in supported and non-supported CuO-NiO species. In situ catalytic experiments for partial oxidation of methane showed a clear interplay between the redox behavior from the Ce in the CeO2-ZrO2 support and the Ni from the active phase. Sample NiO/ZDC exhibited a continuous reduction of Ce cations in CH4:O2 feed flow, carbon formation was detected in X-ray Powder Diffraction (XPD) patterns and Ni re-oxidation was found to take place, clear indications of catalyst deactivation. In contrast, sample CuO-NiO/Ce0.9Zr0.1O2 displayed a slight re-oxidation of Ce and no re-oxidation of Ni altogether with the suppression of carbon formation.
Fil: Toscani, Lucía María. 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. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Universidad Nacional de San Martín. Instituto de Investigación en Ingeniería Ambiental; Argentina
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: Martins, Tereza S.. Universidade de Sao Paulo; Brasil
Fil: Lamas, Diego Germán. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina. Comisión Nacional de Energía Atómica. Gerencia de Área de Aplicaciones de la Tecnología Nuclear. Gerencia de Investigación Aplicada; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; 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. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Universidad Nacional de San Martín. Instituto de Investigación en Ingeniería Ambiental; Argentina
Materia
Catalysis
Partial Oxidation of Methane
XANES
Synchrotron Radiation
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/82159
Acceder
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network_name_str CONICET Digital (CONICET)
spelling In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methaneToscani, Lucía MaríaZimicz, Maria GenovevaMartins, Tereza S.Lamas, Diego GermánLarrondo, Susana AdelinaCatalysisPartial Oxidation of MethaneXANESSynchrotron Radiationhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1In this work we analyze the effect of adding CuO to a NiO/Ce0.9Zr0.1O2 oxide by in situ X-ray absorption near-edge structure XANES technique in Ce L3, Ni K and Cu K absorption edges in terms of sample reducibility and catalytic activity. The oxidation states of Ce, Ni and Cu cations are followed up during temperature programmed reduction (TPR) experiments in diluted hydrogen and during catalytic tests for partial oxidation of methane (POM) reaction. Redox behavior was correlated to conventional fixed bed reactor results. The effect of firing temperature, crystallite size, CeO2-ZrO2 support and the presence of Cu and/or Ni as an active phase is also analyzed. Results showed a beneficial effect of CuO addition in terms of Ce and Ni reduction. A stronger interaction of NiO species with the support was revealed upon analysis of XANES reduction profiles in sample NiO/ZDC in contrast to bimetallic CuO-NiO/ZDC sample. Reduction onset temperature was found to depend on Ni crystallite size, being markedly promoted when samples exhibited low values of crystallite size both in supported and non-supported CuO-NiO species. In situ catalytic experiments for partial oxidation of methane showed a clear interplay between the redox behavior from the Ce in the CeO2-ZrO2 support and the Ni from the active phase. Sample NiO/ZDC exhibited a continuous reduction of Ce cations in CH4:O2 feed flow, carbon formation was detected in X-ray Powder Diffraction (XPD) patterns and Ni re-oxidation was found to take place, clear indications of catalyst deactivation. In contrast, sample CuO-NiO/Ce0.9Zr0.1O2 displayed a slight re-oxidation of Ce and no re-oxidation of Ni altogether with the suppression of carbon formation.Fil: Toscani, Lucía María. 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. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Universidad Nacional de San Martín. Instituto de Investigación en Ingeniería Ambiental; ArgentinaFil: 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: Martins, Tereza S.. Universidade de Sao Paulo; BrasilFil: Lamas, Diego Germán. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina. Comisión Nacional de Energía Atómica. Gerencia de Área de Aplicaciones de la Tecnología Nuclear. Gerencia de Investigación Aplicada; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; 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. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Universidad Nacional de San Martín. Instituto de Investigación en Ingeniería Ambiental; ArgentinaRoyal Society of Chemistry2018-03info: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/11336/82159Toscani, Lucía María; Zimicz, Maria Genoveva; Martins, Tereza S.; Lamas, Diego Germán; Larrondo, Susana Adelina; In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane; Royal Society of Chemistry; RSC Advances; 8; 22; 3-2018; 12190-122032046-2069CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/content/articlelanding/2018/RA/C8RA01528Ginfo:eu-repo/semantics/altIdentifier/doi/10.1039/C8RA01528Ginfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:28:01Zoai:ri.conicet.gov.ar:11336/82159instacron: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 10:28:01.323CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane
title In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane
spellingShingle In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane
Toscani, Lucía María
Catalysis
Partial Oxidation of Methane
XANES
Synchrotron Radiation
title_short In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane
title_full In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane
title_fullStr In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane
title_full_unstemmed In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane
title_sort In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane
dc.creator.none.fl_str_mv Toscani, Lucía María
Zimicz, Maria Genoveva
Martins, Tereza S.
Lamas, Diego Germán
Larrondo, Susana Adelina
author Toscani, Lucía María
author_facet Toscani, Lucía María
Zimicz, Maria Genoveva
Martins, Tereza S.
Lamas, Diego Germán
Larrondo, Susana Adelina
author_role author
author2 Zimicz, Maria Genoveva
Martins, Tereza S.
Lamas, Diego Germán
Larrondo, Susana Adelina
author2_role author
author
author
author
dc.subject.none.fl_str_mv Catalysis
Partial Oxidation of Methane
XANES
Synchrotron Radiation
topic Catalysis
Partial Oxidation of Methane
XANES
Synchrotron Radiation
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv In this work we analyze the effect of adding CuO to a NiO/Ce0.9Zr0.1O2 oxide by in situ X-ray absorption near-edge structure XANES technique in Ce L3, Ni K and Cu K absorption edges in terms of sample reducibility and catalytic activity. The oxidation states of Ce, Ni and Cu cations are followed up during temperature programmed reduction (TPR) experiments in diluted hydrogen and during catalytic tests for partial oxidation of methane (POM) reaction. Redox behavior was correlated to conventional fixed bed reactor results. The effect of firing temperature, crystallite size, CeO2-ZrO2 support and the presence of Cu and/or Ni as an active phase is also analyzed. Results showed a beneficial effect of CuO addition in terms of Ce and Ni reduction. A stronger interaction of NiO species with the support was revealed upon analysis of XANES reduction profiles in sample NiO/ZDC in contrast to bimetallic CuO-NiO/ZDC sample. Reduction onset temperature was found to depend on Ni crystallite size, being markedly promoted when samples exhibited low values of crystallite size both in supported and non-supported CuO-NiO species. In situ catalytic experiments for partial oxidation of methane showed a clear interplay between the redox behavior from the Ce in the CeO2-ZrO2 support and the Ni from the active phase. Sample NiO/ZDC exhibited a continuous reduction of Ce cations in CH4:O2 feed flow, carbon formation was detected in X-ray Powder Diffraction (XPD) patterns and Ni re-oxidation was found to take place, clear indications of catalyst deactivation. In contrast, sample CuO-NiO/Ce0.9Zr0.1O2 displayed a slight re-oxidation of Ce and no re-oxidation of Ni altogether with the suppression of carbon formation.
Fil: Toscani, Lucía María. 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. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Universidad Nacional de San Martín. Instituto de Investigación en Ingeniería Ambiental; Argentina
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: Martins, Tereza S.. Universidade de Sao Paulo; Brasil
Fil: Lamas, Diego Germán. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina. Comisión Nacional de Energía Atómica. Gerencia de Área de Aplicaciones de la Tecnología Nuclear. Gerencia de Investigación Aplicada; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; 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. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Universidad Nacional de San Martín. Instituto de Investigación en Ingeniería Ambiental; Argentina
description In this work we analyze the effect of adding CuO to a NiO/Ce0.9Zr0.1O2 oxide by in situ X-ray absorption near-edge structure XANES technique in Ce L3, Ni K and Cu K absorption edges in terms of sample reducibility and catalytic activity. The oxidation states of Ce, Ni and Cu cations are followed up during temperature programmed reduction (TPR) experiments in diluted hydrogen and during catalytic tests for partial oxidation of methane (POM) reaction. Redox behavior was correlated to conventional fixed bed reactor results. The effect of firing temperature, crystallite size, CeO2-ZrO2 support and the presence of Cu and/or Ni as an active phase is also analyzed. Results showed a beneficial effect of CuO addition in terms of Ce and Ni reduction. A stronger interaction of NiO species with the support was revealed upon analysis of XANES reduction profiles in sample NiO/ZDC in contrast to bimetallic CuO-NiO/ZDC sample. Reduction onset temperature was found to depend on Ni crystallite size, being markedly promoted when samples exhibited low values of crystallite size both in supported and non-supported CuO-NiO species. In situ catalytic experiments for partial oxidation of methane showed a clear interplay between the redox behavior from the Ce in the CeO2-ZrO2 support and the Ni from the active phase. Sample NiO/ZDC exhibited a continuous reduction of Ce cations in CH4:O2 feed flow, carbon formation was detected in X-ray Powder Diffraction (XPD) patterns and Ni re-oxidation was found to take place, clear indications of catalyst deactivation. In contrast, sample CuO-NiO/Ce0.9Zr0.1O2 displayed a slight re-oxidation of Ce and no re-oxidation of Ni altogether with the suppression of carbon formation.
publishDate 2018
dc.date.none.fl_str_mv 2018-03
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/11336/82159
Toscani, Lucía María; Zimicz, Maria Genoveva; Martins, Tereza S.; Lamas, Diego Germán; Larrondo, Susana Adelina; In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane; Royal Society of Chemistry; RSC Advances; 8; 22; 3-2018; 12190-12203
2046-2069
CONICET Digital
CONICET
url http://hdl.handle.net/11336/82159
identifier_str_mv Toscani, Lucía María; Zimicz, Maria Genoveva; Martins, Tereza S.; Lamas, Diego Germán; Larrondo, Susana Adelina; In situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: Redox characterization and its effect in catalytic performance for partial oxidation of methane; Royal Society of Chemistry; RSC Advances; 8; 22; 3-2018; 12190-12203
2046-2069
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://pubs.rsc.org/en/content/articlelanding/2018/RA/C8RA01528G
info:eu-repo/semantics/altIdentifier/doi/10.1039/C8RA01528G
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
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dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
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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