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@article{1627860,
author = {Dochain, Denis D. and Stýskalík, Aleš and Debecker, Damien P.},
article_location = {BASEL},
article_number = {11},
doi = {http://dx.doi.org/10.3390/catal9110920},
keywords = {Mesoporous metallosilicate; tantalum oxide; bioethanol; bifunctional catalysts; dehydration; dehydrogenation},
language = {eng},
issn = {2073-4344},
journal = {CATALYSTS},
title = {Ag- and Cu-Promoted Mesoporous Ta-SiO2 Catalysts Prepared by Non-Hydrolytic Sol-Gel for the Conversion of Ethanol to Butadiene},
url = {https://www.mdpi.com/2073-4344/9/11/920},
volume = {9},
year = {2019}
}
TY - JOUR
ID - 1627860
AU - Dochain, Denis D. - Stýskalík, Aleš - Debecker, Damien P.
PY - 2019
TI - Ag- and Cu-Promoted Mesoporous Ta-SiO2 Catalysts Prepared by Non-Hydrolytic Sol-Gel for the Conversion of Ethanol to Butadiene
JF - CATALYSTS
VL - 9
IS - 11
SP - 920-933
EP - 920-933
PB - MDPI AG
SN - 20734344
KW - Mesoporous metallosilicate
KW - tantalum oxide
KW - bioethanol
KW - bifunctional catalysts
KW - dehydration
KW - dehydrogenation
UR - https://www.mdpi.com/2073-4344/9/11/920
L2 - https://www.mdpi.com/2073-4344/9/11/920
N2 - The direct catalytic conversion of bioethanol to butadiene, also known as the Lebedev process, is one of the most promising solution to replace the petro-based production of this important bulk chemical. Considering the intricate reaction mechanism-where a combination of acid-catalyzed dehydration reactions and metal-catalyzed dehydrogenation have to take place simultaneously-tailor-made bifunctional catalysts are required. We propose to use non-hydrolytic sol-gel (NHSG) chemistry to prepare mesoporous Ta-SiO2 materials which are further promoted by Ag via impregnation. An acetamide elimination route is presented, starting from silicon tetraacetate and pentakis(dimethylamido)tantalum(V), in the presence of a Pluronic surfactant. The catalysts display advantageous texture, with specific surface area in the 600-1000 m(2) g(-1) range, large pore volume (0.6-1.0 mL g(-1)), an average pore diameter of 4 nm and only a small contribution from micropores. Using an array of characterization techniques, we show that NHSG allows achieving a high degree of dispersion of tantalum, mainly incorporated as single sites in the silica matrix. The presence of these monomeric TaOx active sites is responsible for the much higher dehydration ability, as compared to the corresponding catalyst prepared by impregnation of Ta onto a pristine silica support. We attempt to optimize the butadiene yield by changing the relative proportion of Ta and Ag and by tuning the space velocity. We also demonstrate that Ag or Cu can be introduced directly in one step, during the NHSG process. Copper doping is shown to be much more efficient than silver doping to guide the reaction towards the production of butadiene.
ER -
DOCHAIN, Denis D., Aleš STÝSKALÍK and Damien P. DEBECKER. Ag- and Cu-Promoted Mesoporous Ta-SiO2 Catalysts Prepared by Non-Hydrolytic Sol-Gel for the Conversion of Ethanol to Butadiene. \textit{CATALYSTS}. BASEL: MDPI AG, 2019, vol.~9, No~11, p.~920-933. ISSN~2073-4344. Available from: https://dx.doi.org/10.3390/catal9110920.
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