title: Monitoring the Reaction Mechanism in Model Biogas Reforming by In Situ Transient and Steady-State DRIFTS Measurements.
abstract: In this work, the reforming of model biogas was investigated on a Rh/MgAl2O4catalyst. In situ transient and steady-state diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements were used to gain insight into the reaction mechanism involved in the activation of CH4and CO2. It was found that the reaction proceeds through of an initial pathway in which methane and CO2are both dissociated on Rh metallic sites and additionally a bifunctional mechanism in which methane is activated on Rh sites and CO2is activated on the basic sites of the support surface via a formate intermediate by H-assisted CO2decomposition. Moreover, this plausible mechanism is able to explain why the observed apparent activation energy of CO2is much lower than that of CH4. Our results suggest that CO2dissociation facilitates CH4activation, because the oxygen-adsorbed species formed in the decomposition of CO2are capable of reacting with the CHxspecies derived from methane decomposition.
authors.affiliation: Instituto de Ciencia de Materiales de Sevilla, Centro Mixto Universidad de Sevilla-CSIC, 49 Av. Américo Vespucio, 41092, Sevilla, Spain.
authors.forename: Luis F
authors.initials: LF
authors.lastname: Bobadilla
authors.affiliation: Instituto de Ciencia de Materiales de Sevilla, Centro Mixto Universidad de Sevilla-CSIC, 49 Av. Américo Vespucio, 41092, Sevilla, Spain.
authors.forename: Victoria
authors.initials: V
authors.lastname: Garcilaso
authors.affiliation: Instituto de Ciencia de Materiales de Sevilla, Centro Mixto Universidad de Sevilla-CSIC, 49 Av. Américo Vespucio, 41092, Sevilla, Spain.
authors.forename: Miguel A
authors.initials: MA
authors.lastname: Centeno
authors.affiliation: Instituto de Ciencia de Materiales de Sevilla, Centro Mixto Universidad de Sevilla-CSIC, 49 Av. Américo Vespucio, 41092, Sevilla, Spain.
authors.forename: José A
authors.initials: JA
authors.lastname: Odriozola
mesh_terms: D000537:Aluminum Oxide / Q000737:chemistry; D056804:Biofuels; D002245:Carbon Dioxide / Q000737:chemistry; D002384:Catalysis; D008274:Magnesium / Q000737:chemistry; D012238:Rhodium / Q000737:chemistry; D017550:Spectroscopy, Fourier Transform Infrared
chemical_list: D056804:Biofuels; D002245:Carbon Dioxide; D012238:Rhodium; D008274:Magnesium; D000537:Aluminum Oxide
keywords: IR spectroscopy; biogas reforming; reaction mechanisms; rhodium; syngas