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.citation.issue22
dc.citation.volume8
dc.contributor.authorToscani, Lucia M.
dc.contributor.authorGenoveva Zimicz, M.
dc.contributor.authorMartins, Tereza S. [UNIFESP]
dc.contributor.authorLamas, Diego G.
dc.contributor.authorLarrondo, Susana A.
dc.coverageCambridge
dc.date.accessioned2020-07-08T13:09:57Z
dc.date.available2020-07-08T13:09:57Z
dc.date.issued2018
dc.description.abstractIn 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.en
dc.description.affiliationConsejo Nacl Invest Cient & Tecn, MINDEF, UNIDEF, Dept Invest Solidos,CITEDEF, JB de La Salle 4397, RA-1603 Villa Martelli, Buenos Aires, Argentina
dc.description.affiliationUNSAM, Inst Invest & Ingn Ambiental, Campus Miguelete,25 Mayo & Francia, RA-1650 San Martin, Buenos Aires, Argentina
dc.description.affiliationUNS, CONICET, Inst Fis IFISUR, Dept Fis, Av Alem 1253, RA-8000 Bahia Blanca, Buenos Aires, Argentina
dc.description.affiliationUniv Fed Sao Paulo, UNIFESP, Dept Quim, Inst Ciencias Ambientais Quim & Farmaceut, Rua Sao Nicolau 210,2nd Floor, BR-09913030 Diadema, SP, Brazil
dc.description.affiliationUNSAM, CONICET, Escuela Ciencia & Tecnol, Campus Miguelete,25 Mayo & Francia, RA-1650 San Martin, Buenos Aires, Argentina
dc.description.affiliationComis Nacl Energia Atom, Ctr Atom Constituyentes, Gerencia Invest & Aplicac, Dept Fis Mat Condensada, Av Gen Paz 1499, RA-1650 San Martin, Buenos Aires, Argentina
dc.description.affiliationUnifespUniv Fed Sao Paulo, UNIFESP, Dept Quim, Inst Ciencias Ambientais Quim & Farmaceut, Rua Sao Nicolau 210,2nd Floor, BR-09913030 Diadema, SP, Brazil
dc.description.sourceWeb of Science
dc.description.sponsorshipCONICET
dc.description.sponsorshipNational Synchrotron Light Laboratory (LNLS)
dc.description.sponsorshipANPCyT-PICT
dc.description.sponsorshipIDLNLS: XAFS1-15329
dc.description.sponsorshipIDANPCyT-PICT: 1587
dc.format.extent12190-12203
dc.identifierhttp://dx.doi.org/10.1039/c8ra01528g
dc.identifier.citationRsc Advances. Cambridge, v. 8, n. 22, p. 12190-12203, 2018.
dc.identifier.doi10.1039/c8ra01528g
dc.identifier.fileWOS000431976000036.pdf
dc.identifier.issn2046-2069
dc.identifier.urihttps://repositorio.unifesp.br/handle/11600/54318
dc.identifier.wosWOS:000431976000036
dc.language.isoeng
dc.publisherRoyal Soc Chemistry
dc.relation.ispartofRsc Advances
dc.rightsinfo:eu-repo/semantics/openAccess
dc.titleIn situ X-ray absorption spectroscopy study of CuO-NiO/CeO2-ZrO2 oxides: redox characterization and its effect in catalytic performance for partial oxidation of methaneen
dc.typeinfo:eu-repo/semantics/article
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