TY - JOUR

T1 - Continuous supercritical solvothermal preparation of nanostructured ceria-zirconia as supports for dry methane reforming catalysts

AU - Auxéméry, Aimery

AU - Frias, Brigitte Botello

AU - Smal, Ekaterina

AU - Dziadek, Katarzyna

AU - Philippot, Gilles

AU - Legutko, Piotr

AU - Simonov, Michail

AU - Thomas, Sébastien

AU - Adamski, Andrzej

AU - Sadykov, Vladislav

AU - Parkhomenko, Ksenia

AU - Roger, Anne Cécile

AU - Aymonier, Cyril

N1 - Funding Information: The authors acknowledge the European ERANet RUS Plus program for financial support in the frames of the project “NiCe - Design of Ni/ceria-zirconia nanomaterials by continuous synthesis in supercritical medium: tuning catalytic properties”. This work was performed as a part of the large international collaboration GDRI “Catalytic valorization of biomass” supported by CNRS in France and RFBR in Russia . The Polish authors thank for the financial support the National Centre for Research and Development in the framework of NiCe ERANet RUS Plus - S&T project (5/RUSPLUS – S&T/2016). Katarzyna Dziadek acknowledges the Erasmus + Program for the financial support. Aimery Auxemery acknowledges the Innovation Fund Denmark in the frames of the GCAM project for the financial support. The authors from ICMCB acknowledge CNRS, the University of Bordeaux and Bordeaux INP and also the “ Région Nouvelle-Aquitaine ” for their financial support. The authors thank Dr Thierry Dintzer for fruitful discussion on the SEM results. Publisher Copyright: © 2020 Elsevier B.V. Copyright: Copyright 2020 Elsevier B.V., All rights reserved.

PY - 2020/8/1

Y1 - 2020/8/1

N2 - 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.

AB - 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.

KW - Carbon dioxide valorization

KW - Ceria-Zirconia

KW - Dry reforming of methane

KW - Flow synthesis

KW - Mixed oxides

KW - Nanocatalysts

KW - Nickel

KW - Supercritical solvothermal synthesis

KW - METAL-OXIDE NANOPARTICLES

KW - SIZE

KW - CEO2 NANOCRYSTALS

KW - HYDROTHERMAL SYNTHESIS

KW - ALCOHOLS

KW - RAMAN-SCATTERING

KW - SPECTROSCOPY

KW - WATER

UR - http://www.scopus.com/inward/record.url?scp=85083736958&partnerID=8YFLogxK

U2 - 10.1016/j.supflu.2020.104855

DO - 10.1016/j.supflu.2020.104855

M3 - Article

AN - SCOPUS:85083736958

VL - 162

JO - Journal of Supercritical Fluids

JF - Journal of Supercritical Fluids

SN - 0896-8446

M1 - 104855

ER -