title: Investigation of Methane Oxidation Reactions Over a Dual-Bed Catalyst System using18O Labelled DRIFTS coupling.
abstract: Low loading Pd-supported (0.2 wt % Pd) Y-stabilized zirconia (YSZ) and LaMnO3(LM) perovskite were associated to study the partial oxidation of methane using labelled18O2in the gas phase. Synthesis gas production was demonstrated to occur through an indirect reaction in which oxygen is first consumed in the total methane combustion. A Mars-van Krevelen mechanism was observed over Pd/YSZ at 425 °C to yield C16O2and C16O. A significant enhancement of the Pd/YSZ catalyst activity was achieved by the association of LM-Pd/YSZ in a dual catalyst bed, resulting in a significant increase of the oxidation rate. Vibration bands of adsorbed formate species, assumed to be intermediates to the gas production, were observed by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) coupling experiments. It was proposed that LM enables the generation of highly active singlet O2, which is activated on the YSZ oxygen vacancies to assist a rapid recovery of surface PdO and increase formate decomposition into CO and H2in Pd-supported catalyst.
authors.affiliation: Institut de Chimie des Milieux et Matériaux de Poitiers (IC2 MP), University of Poitiers, CNRS, UMR 7285, 4 rue Michel Brunet - TSA 51106 -, 86073, Cedex 9, France.
authors.forename: Melissandre
authors.initials: M
authors.lastname: Richard
authors.affiliation: Institut de Chimie des Milieux et Matériaux de Poitiers (IC2 MP), University of Poitiers, CNRS, UMR 7285, 4 rue Michel Brunet - TSA 51106 -, 86073, Cedex 9, France.
authors.forename: Daniel
authors.initials: D
authors.lastname: Duprez
authors.affiliation: Institut de Chimie des Milieux et Matériaux de Poitiers (IC2 MP), University of Poitiers, CNRS, UMR 7285, 4 rue Michel Brunet - TSA 51106 -, 86073, Cedex 9, France.
authors.forename: Nicolas
authors.initials: N
authors.lastname: Bion
authors.affiliation: Institut de Chimie des Milieux et Matériaux de Poitiers (IC2 MP), University of Poitiers, CNRS, UMR 7285, 4 rue Michel Brunet - TSA 51106 -, 86073, Cedex 9, France.
authors.forename: Fabien
authors.identifier: http://orcid.org/0000-0002-8497-7796
authors.initials: F
authors.lastname: Can
mesh_terms: D000327:Adsorption; D002248:Carbon Monoxide / Q000737:chemistry; D002384:Catalysis; D007259:Infrared Rays; D008697:Methane / Q000737:chemistry*; D010084:Oxidation-Reduction; D010103:Oxygen Isotopes / Q000737:chemistry; D017550:Spectroscopy, Fourier Transform Infrared; D013499:Surface Properties
chemical_list: D010103:Oxygen Isotopes; D002248:Carbon Monoxide; D008697:Methane
keywords: DRIFTS; isotopic exchange; methane; partial oxidation; yttrium-stabilized zirconia