4.6 Article

Multicationic LDH-derived Co(x)CeMgAlO mixed oxide catalysts for the total oxidation of methane

Journal

APPLIED CATALYSIS A-GENERAL
Volume 650, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcata.2022.119001

Keywords

Layered double hydroxides; Mixed oxides catalysts; Cobalt; Cerium; Methane combustion; VOC abatement

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Several Co(x)CeMgAlO mixed oxides were prepared by calcination of LDH precursors at 750 degrees C, with different cobalt contents. The mixed oxide catalysts exhibited the coexistence of Co3O4, periclase-like and ceria phases, distributed homogeneously. The surface composition and redox properties were found to be crucial factors in determining the catalytic activity of the materials.
Several Co(x)CeMgAlO mixed oxides with different cobalt contents x between 7 and 50 at% with respect to cations, but with fixed 10 at% Ce and Mg/Al atomic ratio of 3, were obtained by the calcination of layered double hydroxide (LDH) precursors at 750 degrees C. The mixed oxide catalysts were characterized by XRD, nitrogen adsorption, DRIFT, DR-UV-Vis, SEM-EDX, including elemental mapping, XPS, H2-TPR and O2-TPO techniques. XRD analysis indicated the coexistence of Co3O4 crystallites with periclase-like and ceria phases, distributed homogeneously as shown by EDX measurements. The surface composition determined by XPS and the redox properties studied by H2-TPR and O2-TPO were shown to be key factors controlling the catalytic behavior of the investigated materials. Their catalytic performance was evaluated in the total oxidation of methane, used as a volatile organic compound (VOC) model molecule. Co(40)CeMgAlO mixed oxide showed the highest catalytic activity for methane combustion with a T50 of 528 degrees C, associated with its greatest Co/Ce surface atomic ratio and the best redox properties in the Co(x)CeMgAlO series. In addition, the influence of the contact time on the catalytic activity of the Co(40)CeMgAlO mixed oxide has been examined and its good stability was evidenced from combustion tests with prolonged time on stream. Nevertheless, the addition of water vapors to the reaction mixture induces textural and structural changes of the mixed oxide with negative consequences on its performance.

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