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Monitoring the Reaction Mechanism in Model Biogas Reforming by In Situ Transient and Steady‐State DRIFTS Measurements
Author(s) -
Bobadilla Luis F.,
Garcilaso Victoria,
Centeno Miguel A.,
Odriozola José A.
Publication year - 2017
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.201601379
Subject(s) - formate , chemistry , catalysis , methane , dissociation (chemistry) , reaction mechanism , activation energy , adsorption , decomposition , bifunctional , steady state (chemistry) , photochemistry , reaction intermediate , inorganic chemistry , organic chemistry
Abstract In this work, the reforming of model biogas was investigated on a Rh/MgAl 2 O 4 catalyst. 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 CH 4 and CO 2 . It was found that the reaction proceeds through of an initial pathway in which methane and CO 2 are both dissociated on Rh metallic sites and additionally a bifunctional mechanism in which methane is activated on Rh sites and CO 2 is activated on the basic sites of the support surface via a formate intermediate by H‐assisted CO 2 decomposition. Moreover, this plausible mechanism is able to explain why the observed apparent activation energy of CO 2 is much lower than that of CH 4 . Our results suggest that CO 2 dissociation facilitates CH 4 activation, because the oxygen‐adsorbed species formed in the decomposition of CO 2 are capable of reacting with the CH x species derived from methane decomposition.