Ag- and Cu-Promoted Mesoporous Ta-SiO2 Catalysts Prepared by
Non-Hydrolytic Sol-Gel for the Conversion of Ethanol to
Butadiene

J 2019

Ag- and Cu-Promoted Mesoporous Ta-SiO2 Catalysts Prepared by Non-Hydrolytic Sol-Gel for the Conversion of Ethanol to Butadiene

DOCHAIN, Denis D., Aleš STÝSKALÍK and Damien P. DEBECKER

Basic information

Original name

Ag- and Cu-Promoted Mesoporous Ta-SiO2 Catalysts Prepared by Non-Hydrolytic Sol-Gel for the Conversion of Ethanol to Butadiene

Authors

DOCHAIN, Denis D. (56 Belgium), Aleš STÝSKALÍK (203 Czech Republic, guarantor, belonging to the institution) and Damien P. DEBECKER (56 Belgium)

Edition

CATALYSTS, BASEL, MDPI AG, 2019, 2073-4344

Other information

Language

English

Type of outcome

Článek v odborném periodiku

Field of Study

10402 Inorganic and nuclear chemistry

Country of publisher

Switzerland

Confidentiality degree

není předmětem státního či obchodního tajemství

References:

https://www.mdpi.com/2073-4344/9/11/920

Impact factor

Impact factor: 3.520

RIV identification code

RIV/00216224:14310/19:00113064

Organization unit

Faculty of Science

DOI

http://dx.doi.org/10.3390/catal9110920

UT WoS

000502278800046

Keywords in English

Mesoporous metallosilicate; tantalum oxide; bioethanol; bifunctional catalysts; dehydration; dehydrogenation

Abstract

V originále

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.

Links

LM2015043, research and development project

Name: Česká infrastruktura pro integrativní strukturní biologii (Acronym: CIISB)

Investor: Ministry of Education, Youth and Sports of the CR

Citovat

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. CATALYSTS. BASEL: MDPI AG, 2019, vol. 9, No 11, p. 920-933. ISSN 2073-4344. Available from: https://dx.doi.org/10.3390/catal9110920.

@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.

Detailed Information on Publication Record