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Effect of palladium on the reducibility of Mn based materials: Correlation with methane oxidation activity

hal.structure.identifierLaboratoire de catalyse en chimie organique [LACCO]
dc.contributor.authorBAYLET, Alexandre
hal.structure.identifierLaboratoire de catalyse en chimie organique [LACCO]
dc.contributor.authorROYER, Sébastien
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
dc.contributor.authorLABRUGÈRE, Christine
hal.structure.identifierLaboratoire de catalyse en chimie organique [LACCO]
dc.contributor.authorVALENCIA, Hubert
hal.structure.identifierLaboratoire de catalyse en chimie organique [LACCO]
dc.contributor.authorMARECOT, Patrice
hal.structure.identifierLaboratoire de catalyse en chimie organique [LACCO]
dc.contributor.authorTATIBOUET, Jean-Michel
hal.structure.identifierLaboratoire de catalyse en chimie organique [LACCO]
dc.contributor.authorDUPREZ, Daniel
dc.date.issued2008
dc.identifier.issn1463-9076
dc.description.abstractEnMn-based oxide supports were synthesized using different procedures: (i) carbonate co-precipitation method, leading to the formation of a hexaaluminate crystallized solid (La0.2Sr0.3Ba0.5MnAl 11O19) and (ii) solid-solid diffusion method, leading to the formation of a doped θ-Al2O3 crystallized solid (nominal composition: 60 wt% La0.2Sr0.3Ba 0.5MnAl11O19 + 40 wt% Al2O 3). Impregnation of 1.0 wt%Pd was carried out on both oxides. The solids were tested for the catalytic methane combustion up to 700°C. It was observed that adding palladium resulted in an important increase in the catalytic activity. The combined use of H2-TPR and XPS techniques reveals that only Mn3+/Mn2+ redox "couple" is present in the solids, whatever the synthesis procedure used. The fraction Mn3+/Mn is proportional to the total Mn content in the solid support, whatever the sample structure (hexaaluminate or doped θ-Al 2O3) and its morphology (large crystals or aggregates of small particles, respectively). Pd impregnation and further calcination at 650°C has no significant effect on the Mn3+/Mn fraction. However, some changes in Mn3+ reduction profile are observed, depending on the solid structure. Indeed, palladium addition strongly affects the manganese reducibility with an important shift of the reduction process to lower temperatures (∼100°C). On the basis of redox properties observed for the different catalysts, a Mars-van-Krevelen redox mechanism, with oxygen transfer from support oxides to palladium particles, is proposed to explain the difference in terms of catalytic conversion and stability with respect to a 1.0 wt%Pd/Al2O3 reference sample.
dc.language.isoen
dc.publisherRoyal Society of Chemistry
dc.subject.enMaterials
dc.subject.enOxidation
dc.subject.enMethane
dc.subject.enPalladium
dc.subject.enManganese
dc.title.enEffect of palladium on the reducibility of Mn based materials: Correlation with methane oxidation activity
dc.typeArticle de revue
dc.identifier.doi10.1039/b808289h
dc.subject.halChimie/Matériaux
bordeaux.journalPhysical Chemistry Chemical Physics
bordeaux.page5983-5992
bordeaux.volume10
bordeaux.issue39
bordeaux.peerReviewedoui
hal.identifierhal-00331195
hal.version1
hal.popularnon
hal.audienceInternationale
hal.origin.linkhttps://hal.archives-ouvertes.fr//hal-00331195v1
bordeaux.COinSctx_ver=Z39.88-2004&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.jtitle=Physical%20Chemistry%20Chemical%20Physics&rft.date=2008&rft.volume=10&rft.issue=39&rft.spage=5983-5992&rft.epage=5983-5992&rft.eissn=1463-9076&rft.issn=1463-9076&rft.au=BAYLET,%20Alexandre&ROYER,%20S%C3%A9bastien&LABRUG%C3%88RE,%20Christine&VALENCIA,%20Hubert&MARECOT,%20Patrice&rft.genre=article


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