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Effect of support oxygen storage capacity on the catalytic performance of Rh nanoparticles for CO2 reforming of methane

Gentekakis Ioannis, Goula Grammatiki, Chatzisymeon Maria, Betsi-Argyropoulou Ioanna-Idyli, Botzolaki Georgia, Kousi Kalliopi, Kondarides Dimitris I., Taylor Martin J., Parlett Christopher M.A., Osatiashtiani Amin, Kyriakou Georgios, Holgado Juan Pedro, Lambert Richard M.

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URIhttp://purl.tuc.gr/dl/dias/7C52995B-7CB7-4E22-84C7-15DDEA415827-
Identifierhttps://doi.org/10.1016/j.apcatb.2018.10.048-
Identifierhttps://www.sciencedirect.com/science/article/pii/S092633731831004X-
Languageen-
Extent12 pagesen
TitleEffect of support oxygen storage capacity on the catalytic performance of Rh nanoparticles for CO2 reforming of methaneen
CreatorGentekakis Ioannisen
CreatorΓεντεκακης Ιωαννηςel
CreatorGoula Grammatikien
CreatorΓουλα Γραμματικηel
CreatorChatzisymeon Mariaen
CreatorΧατζησυμεων Μαριαel
CreatorBetsi-Argyropoulou Ioanna-Idylien
CreatorΜπετση-Αργυροπουλου Ιωαννα-Ηδυληel
CreatorBotzolaki Georgiaen
CreatorΜποτζολακη Γεωργιαel
CreatorKousi Kalliopien
CreatorKondarides Dimitris I.en
CreatorTaylor Martin J.en
CreatorParlett Christopher M.A.en
CreatorOsatiashtiani Aminen
CreatorKyriakou Georgiosen
CreatorHolgado Juan Pedroen
CreatorLambert Richard M.en
PublisherElsevieren
Content SummaryThe effects of the metal oxide support on the activity, selectivity, resistance to carbon deposition and high temperature oxidative aging on the Rh-catalyzed dry reforming of methane (DRM) were investigated. Three Rh catalysts supported on oxides characterized by very different oxygen storage capacities and labilities (γ-Al2O3, alumina-ceria-zirconia (ACZ) and ceria-zirconia (CZ)) were studied in the temperature interval 400–750 °C under both integral and differential reaction conditions. ACZ and CZ promoted CO2 conversion, yielding CO-enriched synthesis gas. Detailed characterization of these materials, including state of the art XPS measurements obtained via sample transfer between reaction cell and spectrometer chamber, provided clear insight into the factors that determine catalytic performance. The principal Rh species detected by post reaction XPS was Rh0, its relative content decreasing in the order Rh/CZ(100%)>Rh/ACZ(72%)>Rh/γ-Al2O3(55%). The catalytic activity followed the same order, demonstrating unambiguously that Rh0 is indeed the key active site. Moreover, the presence of CZ in the support served to maintain Rh in the metallic state and minimize carbon deposition under reaction conditions. Carbon deposition, low in all cases, increased in the order Rh/CZ < Rh/ACZ < Rh/γ-Al2O3 consistent with a bi-functional reaction mechanism whereby backspillover of labile lattice O2− contributes to carbon oxidation, stabilization of Rh0 and modification of its surface chemistry; the resulting O vacancies in the support providing centers for dissociative adsorption of CO2. The lower apparent activation energy observed with CZ-containing samples suggests that CZ is a promising support component for use in low temperature DRM.en
Type of ItemPeer-Reviewed Journal Publicationen
Type of ItemΔημοσίευση σε Περιοδικό με Κριτέςel
Licensehttp://creativecommons.org/licenses/by/4.0/en
Date of Item2020-06-29-
Date of Publication2019-
SubjectActive sitesen
SubjectCO2 activationen
SubjectDry reforming of methaneen
SubjectOxygen ions spilloveren
SubjectOxygen storage capacityen
SubjectResistance to carbon depositionen
SubjectRhodium nanoparticlesen
SubjectSupport effectsen
SubjectSynthesis gasen
Bibliographic CitationI.V. Yentekakis, G. Goula, M. Hatzisymeon, I. Betsi-Argyropoulou, G. Botzolaki, K. Kousi, D.I. Kondarides, M.J. Taylor, C.M.A. Parlett, A. Osatiashtiani, G. Kyriakou, J.P. Holgado and R.M. Lambert, "Effect of support oxygen storage capacity on the catalytic performance of Rh nanoparticles for CO2 reforming of methane," Appl. Catal. B-Environ., vol. 243, pp. 490-501, Apr. 2019. doi: 10.1016/j.apcatb.2018.10.048en

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