Continuous supercritical solvothermal preparation of nanostructured ceria-zirconia as supports for dry methane reforming catalysts

Aimery Auxéméry (1) , Brigitte Botello Frias (2) , Ekaterina Smal (3) , Katarzyna Dziadek (4) , Gilles Philippot (1) , Piotr Legutko (4) , Michail Simonov (3) , Sébastien Thomas (1) , Andrzej Adamski (4) , Vladislav Sadykov (3) , Ksenia Parkhomenko (2) , Anne-Cecile Roger (2) , Cyril Aymonier (1)

1 ICMCB - Institut de Chimie de la Matière Condensée de Bordeaux
2 ICPEES - Institut de chimie et procédés pour l'énergie, l'environnement et la santé
3 Boreskov Institute of Catalysis
4 Faculty of Chemistry

The nanostructured CexZr1-xO2 systems (0 ≤ x ≤ 0.75) were prepared combining alkoxide and nitrate precursors in an ethanol/water mixture by the continuous supercritical solvothermal sol-gel like synthesis. They were subsequently used as supports for nickel impregnation (10 wt.%) to obtain catalysts for dry reforming of methane (DRM) reaction. A reference CexZr1-xO2 (x = 0.50) system prepared via conventional coprecipitation method was used as a support for nickel impregnation in the comparative study of the nanostructured materials’ catalytic potential. The morphological and structural properties of the prepared nanostructured supports and Ni-containing catalysts were investigated by numerous techniques as XRD, Raman spectroscopy, SEM, TEM, EDS, chemisorption and others. The conditions of DRM reaction were chosen in order to compare the activity, the stability as well as the selectivity of coke formation in the presence of the prepared catalytic materials. It was found that the industrial catalyst leads to heavy coking in the chosen conditions with a rapid loss of activity. While the nanostructured CexZr1-xO2 (0 ≤ x ≤ 0.75) materials are found to be promising supports for Ni dispersion and coke control in DRM. In this study the nanostructured Ce0.50Zr0.50O2 material impregnated with nickel shown the highest TOF and the smallest selectivity of coke formation in DRM among other nanostructured materials. The continuous supercritical solvothermal method allows to prepare nanostructured mixed oxide materials that could be promising supports for different active metals dispersion and for coke control in the reactions where coking may be abundant.

Mots clés: Flow synthesis; Supercritical solvothermal synthesis; Dry reforming of methane; Carbon dioxide valorization; Nanocatalysts; Nickel; Mixed oxides; Ceria-Zirconia

Domaines: Matériaux

Aimery Auxéméry, Brigitte Botello Frias, Ekaterina Smal, Katarzyna Dziadek, Gilles Philippot, et al.. Continuous supercritical solvothermal preparation of nanostructured ceria-zirconia as supports for dry methane reforming catalysts. Journal of Supercritical Fluids, 2020, 162, 104855 (10 p.). ⟨10.1016/j.supflu.2020.104855⟩. ⟨hal-02570555⟩