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

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216224%3A14310%2F19%3A00113064" target="_blank" >RIV/00216224:14310/19:00113064 - isvavai.cz</a>

Výsledek na webu

<a href="https://www.mdpi.com/2073-4344/9/11/920" target="_blank" >https://www.mdpi.com/2073-4344/9/11/920</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.3390/catal9110920" target="_blank" >10.3390/catal9110920</a>

Jazyk výsledku

angličtina

Název v původním jazyce

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

Popis výsledku v původním jazyce

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.

Název v anglickém jazyce

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

Popis výsledku anglicky

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.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10402 - Inorganic and nuclear chemistry

Projekt

<a href="/cs/project/LM2015043" target="_blank" >LM2015043: Česká infrastruktura pro integrativní strukturní biologii</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)<br>I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2019

Kód důvěrnosti údajů

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

Název periodika

CATALYSTS

ISSN

2073-4344

e-ISSN

2073-4344

Svazek periodika

9

Číslo periodika v rámci svazku

11

Stát vydavatele periodika

CH - Švýcarská konfederace

Počet stran výsledku

14

Strana od-do

920-933

Kód UT WoS článku

000502278800046

EID výsledku v databázi Scopus

2-s2.0-85075003525