期刊
APPLIED CATALYSIS A-GENERAL
卷 504, 期 -, 页码 533-541出版社
ELSEVIER
DOI: 10.1016/j.apcata.2014.10.005
关键词
Hydrotalcite; Sonication; Copper; Acetaldehyde; Ethanol
资金
- Fonds Europeen de Developpement Regional (FEDER)
- CNRS
- Region Nord-Pas-de-Calais
- Ministere de l'Education Nationale de l'Enseignement Superieur et de la Recherche
- National Agency of Research [ANR-09-CP2D-19-01]
Hydrotalcite-type Mg6-xCuxAl2(OH)(16)CO3 center dot 4H(2)O solids (with x=0, 1, 3, 5) were synthesized as precursors of mixed oxides obtained by subsequent calcination. Two families of samples (synthesized by coprecipitation with and without sonication) were thoroughly characterized by XRD, TG-TDA, H-2-TPR, NMR, SEM and N-2-physisorption. Their reactivity towards ethanol was further assessed. Sonication enabled considerably reducing the preparation duration. MgO and Al2O3 were formed upon calcination of the hydrotalcites under air at 400 degrees C, while copper-enriched phases (e.g. CuO, spinel like structure...) were formed from the solids with higher Cu contents. Magnesium atoms substitution by copper atoms in the hydrotalcite structure was evidenced for the first time in this kind of materials using high-resolution solid state NMR. Indeed, a very unusual but remarkable Fermi contact effect was responsible for specific features observed on the NMR spectra. Further, partial substitution of magnesium by copper led to an increase in specific surface area, with the formation of particles of a smaller size. Copper addition considerably enhanced the dehydrogenation properties of the solids at low temperature (similar to 250 degrees C), with a higher reactivity towards ethanol, and higher selectivities to acetaldehyde. (C) 2014 Elsevier B.V. All rights reserved.
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