Aerosol-assisted sol–gel synthesis of mesoporous Ag–Ta–SiO2
catalysts for the direct upgrading of ethanol to butadiene

J 2023

Aerosol-assisted sol–gel synthesis of mesoporous Ag–Ta–SiO2 catalysts for the direct upgrading of ethanol to butadiene

DOCHAIN, Denis D., Antoine VAN DEN DAELEN, Aleš STÝSKALÍK, Vít VYKOUKAL, Damien P. DEBECKER et. al.

Basic information

Original name

Aerosol-assisted sol–gel synthesis of mesoporous Ag–Ta–SiO2 catalysts for the direct upgrading of ethanol to butadiene

Authors

DOCHAIN, Denis D., Antoine VAN DEN DAELEN, Aleš STÝSKALÍK (203 Czech Republic, belonging to the institution), Vít VYKOUKAL (203 Czech Republic, belonging to the institution) and Damien P. DEBECKER (guarantor)

Edition

RSC Sustainability, Royal Society of Chemistry, 2023, 2753-8125

Other information

Language

English

Type of outcome

Článek v odborném periodiku

Field of Study

10402 Inorganic and nuclear chemistry

Country of publisher

United Kingdom of Great Britain and Northern Ireland

Confidentiality degree

není předmětem státního či obchodního tajemství

References:

URL

RIV identification code

RIV/00216224:14310/23:00131010

Organization unit

Faculty of Science

DOI

http://dx.doi.org/10.1039/D2SU00080F

UT WoS

001277109200001

Keywords in English

ethanol; butadiene; acid catalysis; one-pot; sol-gel; aerosol

Abstract

V originále

The Lebedev process, or the direct catalytic conversion of bioethanol to butadiene, offers an up-and-coming sustainable alternative to the petrochemical route toward this high-demand C4 hydrocarbon. Since the reaction mechanism involves a cascade of dehydrogenation, hydrogen transfer and dehydration steps, a bifunctional catalyst combining both redox (for the dehydrogenation reaction) and acid (for hydrogen transfer and dehydration reactions) functionalities is required. Multi-step preparation methods are typically implemented to obtain tailored bifunctional catalysts, and one of the challenges is to balance the two functions to maximize the BD yield. Here, we disclose a straightforward, one-step, and continuous preparation method of Ta-doped SiO2 loaded with Ag nanoparticles by coupling sol–gel chemistry with aerosol processing. Combining tantalum ethoxide, silver nitrate, hydrolysed tetraethyl orthosilicate and pluronic F127 as templating agent in the aerosol process leads to mesoporous bifunctional catalysts featuring a specific surface area between 310–370 m2 g−1, a pore volume of ca. 0.5 mL g−1 and an average pore diameter of 5 nm. As attested by a variety of characterization techniques, the method leads to the homogeneous incorporation of highly dispersed tantalum species in the silica matrix, thereby creating the required acidic sites. These new catalysts have higher dehydration activity, as compared to the corresponding reference catalysts prepared by classical impregnation. Concomitantly, relatively small silver nanoparticles are stabilized (∼15 nm). The relative Ta and Ag loading can be tuned easily. In the ethanol to butadiene reaction, these aerosol-made catalysts achieve a butadiene yield of ca. 25% by optimizing the relative loadings of Ta and Ag, outcompeting the corresponding formulations prepared by impregnation.

Links

GJ20-03636Y, research and development project

Name: Nové katalyzátory pro přípravu 1,3-butadienu z ethanolu

Investor: Czech Science Foundation

LM2015041, research and development project

Name: CEITEC Nano

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

LM2015043, research and development project

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

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

LM2018127, research and development project

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

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

90110, large research infrastructures

Name: CzechNanoLab

90242, large research infrastructures

Name: CIISB III

Citovat

DOCHAIN, Denis D., Antoine VAN DEN DAELEN, Aleš STÝSKALÍK, Vít VYKOUKAL and Damien P. DEBECKER. Aerosol-assisted sol–gel synthesis of mesoporous Ag–Ta–SiO2 catalysts for the direct upgrading of ethanol to butadiene. RSC Sustainability. Royal Society of Chemistry, 2023, vol. 1, No 3, p. 599-608. ISSN 2753-8125. Available from: https://dx.doi.org/10.1039/D2SU00080F.

@article{2292768,
   author = {Dochain, Denis D. and Van Den Daelen, Antoine and Stýskalík, Aleš and Vykoukal, Vít and Debecker, Damien P.},
   article_number = {3},
   doi = {http://dx.doi.org/10.1039/D2SU00080F},
   keywords = {ethanol; butadiene; acid catalysis; one-pot; sol-gel; aerosol},
   language = {eng},
   issn = {2753-8125},
   journal = {RSC Sustainability},
   title = {Aerosol-assisted sol–gel synthesis of mesoporous Ag–Ta–SiO2 catalysts for the direct upgrading of ethanol to butadiene},
   url = {https://doi.org/10.1039/D2SU00080F},
   volume = {1},
   year = {2023}
}

TY  - JOUR
ID  - 2292768
AU  - Dochain, Denis D. - Van Den Daelen, Antoine - Stýskalík, Aleš - Vykoukal, Vít - Debecker, Damien P.
PY  - 2023
TI  - Aerosol-assisted sol–gel synthesis of mesoporous Ag–Ta–SiO2 catalysts for the direct upgrading of ethanol to butadiene
JF  - RSC Sustainability
VL  - 1
IS  - 3
SP  - 599-608
EP  - 599-608
PB  - Royal Society of Chemistry
SN  - 27538125
KW  - ethanol
KW  - butadiene
KW  - acid catalysis
KW  - one-pot
KW  - sol-gel
KW  - aerosol
UR  - https://doi.org/10.1039/D2SU00080F
N2  - The Lebedev process, or the direct catalytic conversion of bioethanol to butadiene, offers an up-and-coming sustainable alternative to the petrochemical route toward this high-demand C4 hydrocarbon. Since the reaction mechanism involves a cascade of dehydrogenation, hydrogen transfer and dehydration steps, a bifunctional catalyst combining both redox (for the dehydrogenation reaction) and acid (for hydrogen transfer and dehydration reactions) functionalities is required. Multi-step preparation methods are typically implemented to obtain tailored bifunctional catalysts, and one of the challenges is to balance the two functions to maximize the BD yield. Here, we disclose a straightforward, one-step, and continuous preparation method of Ta-doped SiO2 loaded with Ag nanoparticles by coupling sol–gel chemistry with aerosol processing. Combining tantalum ethoxide, silver nitrate, hydrolysed tetraethyl orthosilicate and pluronic F127 as templating agent in the aerosol process leads to mesoporous bifunctional catalysts featuring a specific surface area between 310–370 m2 g−1, a pore volume of ca. 0.5 mL g−1 and an average pore diameter of 5 nm. As attested by a variety of characterization techniques, the method leads to the homogeneous incorporation of highly dispersed tantalum species in the silica matrix, thereby creating the required acidic sites. These new catalysts have higher dehydration activity, as compared to the corresponding reference catalysts prepared by classical impregnation. Concomitantly, relatively small silver nanoparticles are stabilized (∼15 nm). The relative Ta and Ag loading can be tuned easily. In the ethanol to butadiene reaction, these aerosol-made catalysts achieve a butadiene yield of ca. 25% by optimizing the relative loadings of Ta and Ag, outcompeting the corresponding formulations prepared by impregnation.
ER  -

DOCHAIN, Denis D., Antoine VAN DEN DAELEN, Aleš STÝSKALÍK, Vít VYKOUKAL and Damien P. DEBECKER. Aerosol-assisted sol–gel synthesis of mesoporous Ag–Ta–SiO2 catalysts for the direct upgrading of ethanol to butadiene. \textit{RSC Sustainability}. Royal Society of Chemistry, 2023, vol.~1, No~3, p.~599-608. ISSN~2753-8125. Available from: https://dx.doi.org/10.1039/D2SU00080F.

Detailed Information on Publication Record