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.

Základní údaje

Originální název

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

Autoři

LEONOVÁ, Lucie (203 Česká republika, domácí), Zdeněk MORAVEC (203 Česká republika, domácí), Petr SAZAMA, Jana PASTVOVA, Libor KOBERA, Jiri BRUS a Aleš STÝSKALÍK (203 Česká republika, garant, domácí)

Vydání

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

Další údaje

Jazyk

angličtina

Typ výsledku

Článek v odborném periodiku

Obor

10402 Inorganic and nuclear chemistry

Stát vydavatele

Německo

Utajení

není předmětem státního či obchodního tajemství

Odkazy

URL

Impakt faktor

Impact factor: 4.500 v roce 2022

Kód RIV

RIV/00216224:14310/23:00131009

Organizační jednotka

Přírodovědecká fakulta

DOI

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

UT WoS

001005890400001

Klíčová slova anglicky

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

Štítky

CF BIC, CF CRYO, CF NMR, rivok

Příznaky

Mezinárodní význam, Recenzováno

Změněno: 15. 10. 2024 14:57, Ing. Jana Kuchtová

Anotace

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.

Návaznosti

GJ20-03636Y, projekt VaV

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

Investor: Grantová agentura ČR, Nové katalyzátory pro přípravu 1,3-butadienu z ethanolu

MUNI/A/1209/2022, interní kód MU

Název: Molekuly, komplexy, makrocykly a xerogely

Investor: Masarykova univerzita, Molekuly, komplexy, makrocykly a xerogely

MUNI/J/0007/2021, interní kód MU

Název: Tailored Catalysts for Carbon Dioxide Utilization

Investor: Masarykova univerzita, Tailored Catalysts for Carbon Dioxide Utilization, MASH JUNIOR - MUNI Award In Science and Humanities JUNIOR

90127, velká výzkumná infrastruktura

Název: CIISB II

Citovat

LEONOVÁ, Lucie, Zdeněk MORAVEC, Petr SAZAMA, Jana PASTVOVA, Libor KOBERA, Jiri BRUS a Aleš STÝSKALÍK. Hydrophobicity Boosts Catalytic Activity: The Tailoring of Aluminosilicates with Trimethylsilyl Groups. ChemCatChem. Wiley-VCH GmbH, 2023, roč. 15, č. 13, s. 1-17. ISSN 1867-3880. Dostupné z: 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 a Aleš STÝSKALÍK. Hydrophobicity Boosts Catalytic Activity: The Tailoring of Aluminosilicates with Trimethylsilyl Groups. \textit{ChemCatChem}. Wiley-VCH GmbH, 2023, roč.~15, č.~13, s.~1-17. ISSN~1867-3880. Dostupné z: https://dx.doi.org/10.1002/cctc.202300449.

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