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Continuous supercritical solvothermal preparation of nanostructured ceria-zirconia as supports for dry methane reforming catalysts
The Journal of Supercritical Fluids ( IF 3.4 ) Pub Date : 2020-04-18 , DOI: 10.1016/j.supflu.2020.104855
Aimery Auxéméry , Brigitte Botello Frias , Ekaterina Smal , Katarzyna Dziadek , Gilles Philippot , Piotr Legutko , Michail Simonov , Sébastien Thomas , Andrzej Adamski , Vladislav Sadykov , Ksenia Parkhomenko , Anne-Cécile Roger , Cyril Aymonier

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.



中文翻译:

连续超临界溶剂热法制备纳米结构二氧化铈-氧化锆作为甲烷干重整催化剂的载体

纳米结构的Ce x Zr 1-x O 2系统(0≤x≤0.75)通过连续超临界溶剂热溶胶-凝胶法合成,在乙醇/水混合物中结合了醇盐和硝酸盐前体而制得。它们随后被用作镍浸渍的载体(10重量%),以获得用于甲烷(DRM)反应的干重整的催化剂。参考铈X的Zr 1-x Ö 2(X = 0.50)体系制备通过在纳米结构材料催化潜力的比较研究中,传统的共沉淀法被用作镍浸渍的载体。用XRD,拉曼光谱,SEM,TEM,EDS,化学吸附等方法研究了制备的纳米结构载体和含镍催化剂的形貌和结构性能。选择DRM反应的条件以比较在制备的催化材料存在下的活性,稳定性以及焦炭形成的选择性。已经发现,在选择的条件下,工业催化剂导致严重的焦化,并迅速失去活性。而纳米结构的Ce x Zr 1-x O 2发现(0≤x≤0.75)材料是DRM中镍分散和焦炭控制的有前途的支持。在这项研究中,在其他纳米结构材料中,浸渍有镍的纳米结构Ce 0.50 Zr 0.50 O 2材料显示出最高的TOF和最小的焦炭形成选择性。连续超临界溶剂热法可以制备纳米结构的混合氧化物材料,这些材料有望成为支持各种活性金属分散体和控制焦化可能丰富的反应中焦炭的载体。

更新日期:2020-04-18
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