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
Autor(a) principal: | |
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Data de Publicação: | 2018 |
Outros Autores: | , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNIFESP |
Texto Completo: | https://repositorio.unifesp.br/handle/11600/54318 http://dx.doi.org/10.1039/c8ra01528g |
Resumo: | 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 : O-2 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 reoxidation of Ce and no re-oxidation of Ni altogether with the suppression of carbon formation. |
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Toscani, Lucia M.Genoveva Zimicz, M.Martins, Tereza S. [UNIFESP]Lamas, Diego G.Larrondo, Susana A.2020-07-08T13:09:57Z2020-07-08T13:09:57Z2018Rsc Advances. Cambridge, v. 8, n. 22, p. 12190-12203, 2018.2046-2069https://repositorio.unifesp.br/handle/11600/54318http://dx.doi.org/10.1039/c8ra01528gWOS000431976000036.pdf10.1039/c8ra01528gWOS:000431976000036In 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 : O-2 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 reoxidation of Ce and no re-oxidation of Ni altogether with the suppression of carbon formation.CONICETNational Synchrotron Light Laboratory (LNLS)ANPCyT-PICTConsejo Nacl Invest Cient & Tecn, MINDEF, UNIDEF, Dept Invest Solidos,CITEDEF, JB de La Salle 4397, RA-1603 Villa Martelli, Buenos Aires, ArgentinaUNSAM, Inst Invest & Ingn Ambiental, Campus Miguelete,25 Mayo & Francia, RA-1650 San Martin, Buenos Aires, ArgentinaUNS, CONICET, Inst Fis IFISUR, Dept Fis, Av Alem 1253, RA-8000 Bahia Blanca, Buenos Aires, ArgentinaUniv Fed Sao Paulo, UNIFESP, Dept Quim, Inst Ciencias Ambientais Quim & Farmaceut, Rua Sao Nicolau 210,2nd Floor, BR-09913030 Diadema, SP, BrazilUNSAM, CONICET, Escuela Ciencia & Tecnol, Campus Miguelete,25 Mayo & Francia, RA-1650 San Martin, Buenos Aires, ArgentinaComis Nacl Energia Atom, Ctr Atom Constituyentes, Gerencia Invest & Aplicac, Dept Fis Mat Condensada, Av Gen Paz 1499, RA-1650 San Martin, Buenos Aires, ArgentinaUniv Fed Sao Paulo, UNIFESP, Dept Quim, Inst Ciencias Ambientais Quim & Farmaceut, Rua Sao Nicolau 210,2nd Floor, BR-09913030 Diadema, SP, BrazilLNLS: XAFS1-15329ANPCyT-PICT: 1587Web of Science12190-12203engRoyal Soc ChemistryRsc AdvancesIn situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: redox characterization and its effect in catalytic performance for partial oxidation of methaneinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleCambridge822info:eu-repo/semantics/openAccessreponame:Repositório Institucional da UNIFESPinstname:Universidade Federal de São Paulo (UNIFESP)instacron:UNIFESPORIGINALWOS000431976000036.pdfapplication/pdf1343355${dspace.ui.url}/bitstream/11600/54318/1/WOS000431976000036.pdfd8dc3d77e2494c1fbce9e85320db9482MD51open accessTEXTWOS000431976000036.pdf.txtWOS000431976000036.pdf.txtExtracted texttext/plain68056${dspace.ui.url}/bitstream/11600/54318/8/WOS000431976000036.pdf.txtda04b1c060ad0aa4d8870de245daa8c8MD58open accessTHUMBNAILWOS000431976000036.pdf.jpgWOS000431976000036.pdf.jpgIM Thumbnailimage/jpeg7351${dspace.ui.url}/bitstream/11600/54318/10/WOS000431976000036.pdf.jpg509819596989647c160484d2fdf5f117MD510open access11600/543182023-06-05 19:24:54.205open accessoai:repositorio.unifesp.br:11600/54318Repositório InstitucionalPUBhttp://www.repositorio.unifesp.br/oai/requestopendoar:34652023-06-05T22:24:54Repositório Institucional da UNIFESP - Universidade Federal de São Paulo (UNIFESP)false |
dc.title.en.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, Lucia M. |
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 |
author |
Toscani, Lucia M. |
author_facet |
Toscani, Lucia M. Genoveva Zimicz, M. Martins, Tereza S. [UNIFESP] Lamas, Diego G. Larrondo, Susana A. |
author_role |
author |
author2 |
Genoveva Zimicz, M. Martins, Tereza S. [UNIFESP] Lamas, Diego G. Larrondo, Susana A. |
author2_role |
author author author author |
dc.contributor.author.fl_str_mv |
Toscani, Lucia M. Genoveva Zimicz, M. Martins, Tereza S. [UNIFESP] Lamas, Diego G. Larrondo, Susana A. |
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 : O-2 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 reoxidation of Ce and no re-oxidation of Ni altogether with the suppression of carbon formation. |
publishDate |
2018 |
dc.date.issued.fl_str_mv |
2018 |
dc.date.accessioned.fl_str_mv |
2020-07-08T13:09:57Z |
dc.date.available.fl_str_mv |
2020-07-08T13:09:57Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
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format |
article |
status_str |
publishedVersion |
dc.identifier.citation.fl_str_mv |
Rsc Advances. Cambridge, v. 8, n. 22, p. 12190-12203, 2018. |
dc.identifier.uri.fl_str_mv |
https://repositorio.unifesp.br/handle/11600/54318 http://dx.doi.org/10.1039/c8ra01528g |
dc.identifier.issn.none.fl_str_mv |
2046-2069 |
dc.identifier.file.none.fl_str_mv |
WOS000431976000036.pdf |
dc.identifier.doi.none.fl_str_mv |
10.1039/c8ra01528g |
dc.identifier.wos.none.fl_str_mv |
WOS:000431976000036 |
identifier_str_mv |
Rsc Advances. Cambridge, v. 8, n. 22, p. 12190-12203, 2018. 2046-2069 WOS000431976000036.pdf 10.1039/c8ra01528g WOS:000431976000036 |
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https://repositorio.unifesp.br/handle/11600/54318 http://dx.doi.org/10.1039/c8ra01528g |
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Royal Soc Chemistry |
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Royal Soc Chemistry |
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