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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.

Απλή Εγγραφή

URIhttp://purl.tuc.gr/dl/dias/7C52995B-7CB7-4E22-84C7-15DDEA415827-
Αναγνωριστικόhttps://doi.org/10.1016/j.apcatb.2018.10.048-
Αναγνωριστικόhttps://www.sciencedirect.com/science/article/pii/S092633731831004X-
Γλώσσαen-
Μέγεθος12 pagesen
ΤίτλοςEffect of support oxygen storage capacity on the catalytic performance of Rh nanoparticles for CO2 reforming of methaneen
ΔημιουργόςGentekakis Ioannisen
ΔημιουργόςΓεντεκακης Ιωαννηςel
ΔημιουργόςGoula Grammatikien
ΔημιουργόςΓουλα Γραμματικηel
ΔημιουργόςChatzisymeon Mariaen
ΔημιουργόςΧατζησυμεων Μαριαel
ΔημιουργόςBetsi-Argyropoulou Ioanna-Idylien
ΔημιουργόςΜπετση-Αργυροπουλου Ιωαννα-Ηδυληel
ΔημιουργόςBotzolaki Georgiaen
ΔημιουργόςΜποτζολακη Γεωργιαel
ΔημιουργόςKousi Kalliopien
ΔημιουργόςKondarides Dimitris I.en
ΔημιουργόςTaylor Martin J.en
ΔημιουργόςParlett Christopher M.A.en
ΔημιουργόςOsatiashtiani Aminen
ΔημιουργόςKyriakou Georgiosen
ΔημιουργόςHolgado Juan Pedroen
ΔημιουργόςLambert Richard M.en
ΕκδότηςElsevieren
ΠερίληψηThe 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
ΤύποςPeer-Reviewed Journal Publicationen
ΤύποςΔημοσίευση σε Περιοδικό με Κριτέςel
Άδεια Χρήσηςhttp://creativecommons.org/licenses/by/4.0/en
Ημερομηνία2020-06-29-
Ημερομηνία Δημοσίευσης2019-
Θεματική ΚατηγορίαActive sitesen
Θεματική ΚατηγορίαCO2 activationen
Θεματική ΚατηγορίαDry reforming of methaneen
Θεματική ΚατηγορίαOxygen ions spilloveren
Θεματική ΚατηγορίαOxygen storage capacityen
Θεματική ΚατηγορίαResistance to carbon depositionen
Θεματική ΚατηγορίαRhodium nanoparticlesen
Θεματική ΚατηγορίαSupport effectsen
Θεματική ΚατηγορίαSynthesis gasen
Βιβλιογραφική ΑναφοράI.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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