Deactivation mechanism of Ni supported on Mg-Al spinel during autothermal reforming of model biogas
Autor: | Montenegro Camacho, Y.S., Bensaid, S., Lorentzou, S., Vlachos, N., Pantoleontos, G., Konstandopoulos, A., Meunier, F.C., Werzner, E., Herrmann, A., Rau, F., Krause, H., Rezaei, E., Ortona, A., Gianella, S., Khinsky, A., Antonini, M., Marchisio, L., Vilardo, F., Trimis, D., Fino, D., Landrivon, Emmanuel, Lafleur, Matthieu, Bougie, Francis, Larachi, Faïçal, Fongarland, Pascal, Iliuta, Maria, Luneau, Mathilde, Gianotti, Elia, Meunier, Frédéric, Mirodatos, Claude, Puzenat, Eric, Schuurman, Y., Guilhaume, N. |
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Přispěvatelé: | Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), IRCELYON-Ingéniérie, du matériau au réacteur (ING), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Claude Bernard Lyon 1 (UCBL), IRCELYON-Catalyse Hétérogène pour la Transition Energétique (CATREN) |
Rok vydání: | 2017 |
Předmět: |
Nial
Materials science chemistry.chemical_element 02 engineering and technology engineering.material 010402 general chemistry 7. Clean energy 01 natural sciences Catalysis Methane chemistry.chemical_compound ComputingMilieux_MISCELLANEOUS General Environmental Science computer.programming_language Methane reformer Process Chemistry and Technology Spinel Non-blocking I/O Metallurgy [CHIM.CATA]Chemical Sciences/Catalysis 021001 nanoscience & nanotechnology [SDE.ES]Environmental Sciences/Environmental and Society 0104 chemical sciences [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry Nickel chemistry Chemical engineering 13. Climate action engineering 0210 nano-technology computer Syngas |
Zdroj: | Applied Catalysis B: Environmental Applied Catalysis B: Environmental, Elsevier, 2017, 203 (45), pp.289-299. ⟨10.1016/j.apcatb.2016.10.023⟩ Applied Catalysis B: Environmental, Elsevier, 2017, 203, pp.289-299. ⟨10.1016/j.apcatb.2016.10.023⟩ |
ISSN: | 0926-3373 |
DOI: | 10.1016/j.apcatb.2016.10.023 |
Popis: | SSCI-VIDE+ECI2D:ING+MLU:EGI:FRM:CMI:EPU:YSC:NOG; International audience; Nickel supported on Mg-Al oxides was studied in the autothermal reforming (ATR) of model biogas at 700 degrees C. Ni/Mg0.4Al2O3.4 deactivated with time on stream and the cause of deactivation was investigated and identified. Ni was readily oxidized to NiO in the presence of O-2. While NiO was essentially inactive for the reforming reaction, this oxide was yet active for methane combustion. Exhaustion of the O-2 supply at front of the catalyst bed enabled the remaining CH4 to be steam and dry reformed on the metallic Ni left downstream. Gradual formation of NiAl2O4 spinel was also observed, likely caused by the higher temperature prevailing in the exothermic combustion zone that favors the diffusion of nickel cations into the alumina structure. In contrast to NiO, NiAl2O4 spinel was poorly active for CH4 oxidation. The frontline associated with the formation of the NiAl2O4 spinel phase eventually reached the end of the catalyst bed, resulting in a complete loss of activity. No significant coke deposition could be evidenced here. The Ni deactivation profile was adequately fitted using a methane ATR kinetic model that included a linear decrease in the number of Ni metallic sites. Addition of Rh/Mg1.1Al2O4.1 in front of a nickel-based catalyst led to a stable activity. Using this dual-bed system, no NiAl2O4 formation was identified after reaction. (C) 2016 Elsevier B.V. All rights reserved. |
Databáze: | OpenAIRE |
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