Hydrophobicity Boosts Catalytic Activity: The Tailoring of
Aluminosilicates with Trimethylsilyl Groups

J 2023

Hydrophobicity Boosts Catalytic Activity: The Tailoring of Aluminosilicates with Trimethylsilyl Groups

LEONOVÁ, Lucie, Zdeněk MORAVEC, Petr SAZAMA, Jana PASTVOVA, Libor KOBERA et. al.

Basic information

Original name

Hydrophobicity Boosts Catalytic Activity: The Tailoring of Aluminosilicates with Trimethylsilyl Groups

Authors

LEONOVÁ, Lucie (203 Czech Republic, belonging to the institution), Zdeněk MORAVEC (203 Czech Republic, belonging to the institution), Petr SAZAMA, Jana PASTVOVA, Libor KOBERA, Jiri BRUS and Aleš STÝSKALÍK (203 Czech Republic, guarantor, belonging to the institution)

Edition

ChemCatChem, Wiley-VCH GmbH, 2023, 1867-3880

Other information

Language

English

Type of outcome

Článek v odborném periodiku

Field of Study

10402 Inorganic and nuclear chemistry

Country of publisher

Germany

Confidentiality degree

není předmětem státního či obchodního tajemství

References:

URL

Impact factor

Impact factor: 4.500 in 2022

RIV identification code

RIV/00216224:14310/23:00131009

Organization unit

Faculty of Science

DOI

http://dx.doi.org/10.1002/cctc.202300449

UT WoS

001005890400001

Keywords in English

acid catalysis; aluminosilicate; epoxide ring opening; ethanol dehydration; hydrophobicity

Abstract

V originále

Introducing organic groups into metal silicate catalysts and thus supposedly changing the surface hydrophobicity has been shown to enhance the catalyst performance in various reactions. However, the organic groups introduction does not unambiguously guarantee hydrophobicity control. Therefore, a thorough characterization is necessary to provide a complete view of the interaction between the catalyst surface, reactants, and products. Herein, an aluminosilicate catalyst with well-dispersed Al atoms was prepared via the non-hydrolytic sol-gel method. This material was post-synthetically modified with trimethylsilyl groups; their number on the catalyst surface was controlled via a temperature-vacuum pretreatment. In such a way, aluminosilicate materials with similar porosity, structure, and acid site strength and quality were obtained. Notably, the water sorption measurements showed that trimethylsilylated aluminosilicates adsorb 2.5–3 times less water than the parent material (p/p0=0.3). The turn-over-frequency in epoxide ring opening and ethanol dehydration scaled up with the number of trimethylsilyl groups grafted on the catalyst surface. Particularly, the heavily trimethylsilylated sample achieved three to five times higher turnover-frequency in styrene oxide aminolysis than the parent aluminosilicate material. To the best of the authors’ knowledge, it exhibited the most active Al sites for epoxide aminolysis in the present literature.

Links

GJ20-03636Y, research and development project

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

Investor: Czech Science Foundation

MUNI/A/1209/2022, interní kód MU

Name: Molekuly, komplexy, makrocykly a xerogely

Investor: Masaryk University, Molecules, complexes, macrocycles, and xerogels

MUNI/J/0007/2021, interní kód MU

Name: Tailored Catalysts for Carbon Dioxide Utilization

Investor: Masaryk University, MASH JUNIOR - MUNI Award In Science and Humanities JUNIOR

90127, large research infrastructures

Name: CIISB II

Citovat

LEONOVÁ, Lucie, Zdeněk MORAVEC, Petr SAZAMA, Jana PASTVOVA, Libor KOBERA, Jiri BRUS and Aleš STÝSKALÍK. Hydrophobicity Boosts Catalytic Activity: The Tailoring of Aluminosilicates with Trimethylsilyl Groups. ChemCatChem. Wiley-VCH GmbH, 2023, vol. 15, No 13, p. 1-17. ISSN 1867-3880. Available from: https://dx.doi.org/10.1002/cctc.202300449.

@article{2292766,
   author = {Leonová, Lucie and Moravec, Zdeněk and Sazama, Petr and Pastvova, Jana and Kobera, Libor and Brus, Jiri and Stýskalík, Aleš},
   article_number = {13},
   doi = {http://dx.doi.org/10.1002/cctc.202300449},
   keywords = {acid catalysis; aluminosilicate; epoxide ring opening; ethanol dehydration; hydrophobicity},
   language = {eng},
   issn = {1867-3880},
   journal = {ChemCatChem},
   title = {Hydrophobicity Boosts Catalytic Activity: The Tailoring of Aluminosilicates with Trimethylsilyl Groups},
   url = {https://doi.org/10.1002/cctc.202300449},
   volume = {15},
   year = {2023}
}

TY  - JOUR
ID  - 2292766
AU  - Leonová, Lucie - Moravec, Zdeněk - Sazama, Petr - Pastvova, Jana - Kobera, Libor - Brus, Jiri - Stýskalík, Aleš
PY  - 2023
TI  - Hydrophobicity Boosts Catalytic Activity: The Tailoring of Aluminosilicates with Trimethylsilyl Groups
JF  - ChemCatChem
VL  - 15
IS  - 13
SP  - 1-17
EP  - 1-17
PB  - Wiley-VCH GmbH
SN  - 18673880
KW  - acid catalysis
KW  - aluminosilicate
KW  - epoxide ring opening
KW  - ethanol dehydration
KW  - hydrophobicity
UR  - https://doi.org/10.1002/cctc.202300449
N2  - Introducing organic groups into metal silicate catalysts and thus supposedly changing the surface hydrophobicity has been shown to enhance the catalyst performance in various reactions. However, the organic groups introduction does not unambiguously guarantee hydrophobicity control. Therefore, a thorough characterization is necessary to provide a complete view of the interaction between the catalyst surface, reactants, and products. Herein, an aluminosilicate catalyst with well-dispersed Al atoms was prepared via the non-hydrolytic sol-gel method. This material was post-synthetically modified with trimethylsilyl groups; their number on the catalyst surface was controlled via a temperature-vacuum pretreatment. In such a way, aluminosilicate materials with similar porosity, structure, and acid site strength and quality were obtained. Notably, the water sorption measurements showed that trimethylsilylated aluminosilicates adsorb 2.5–3 times less water than the parent material (p/p0=0.3). The turn-over-frequency in epoxide ring opening and ethanol dehydration scaled up with the number of trimethylsilyl groups grafted on the catalyst surface. Particularly, the heavily trimethylsilylated sample achieved three to five times higher turnover-frequency in styrene oxide aminolysis than the parent aluminosilicate material. To the best of the authors’ knowledge, it exhibited the most active Al sites for epoxide aminolysis in the present literature.
ER  -

LEONOVÁ, Lucie, Zdeněk MORAVEC, Petr SAZAMA, Jana PASTVOVA, Libor KOBERA, Jiri BRUS and Aleš STÝSKALÍK. Hydrophobicity Boosts Catalytic Activity: The Tailoring of Aluminosilicates with Trimethylsilyl Groups. \textit{ChemCatChem}. Wiley-VCH GmbH, 2023, vol.~15, No~13, p.~1-17. ISSN~1867-3880. Available from: https://dx.doi.org/10.1002/cctc.202300449.

Detailed Information on Publication Record