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

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F23%3A00573305" target="_blank" >RIV/61388955:_____/23:00573305 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/61389013:_____/23:00573305 RIV/00216224:14310/23:00131009

Výsledek na webu

<a href="https://hdl.handle.net/11104/0343769" target="_blank" >https://hdl.handle.net/11104/0343769</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/cctc.202300449" target="_blank" >10.1002/cctc.202300449</a>

Jazyk výsledku

angličtina

Název v původním jazyce

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

Popis výsledku v původním jazyce

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.

Název v anglickém jazyce

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

Popis výsledku anglicky

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.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

Výsledek vznikl pri realizaci vícero projektů. Více informací v záložce Projekty.

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2023

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

ChemCatChem

ISSN

1867-3880

e-ISSN

1867-3899

Svazek periodika

15

Číslo periodika v rámci svazku

13

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

16

Strana od-do

e202300449

Kód UT WoS článku

001005890400001

EID výsledku v databázi Scopus

2-s2.0-85161626858