Non-hydrolytic Sol-Gel Routes to Bifunctional Cu-Ta-SiO<sub>2</sub> Catalysts for the Upgrading of Ethanol to Butadiene
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216224%3A14310%2F23%3A00132623" target="_blank" >RIV/00216224:14310/23:00132623 - isvavai.cz</a>
Result on the web
<a href="https://pubs.acs.org/doi/10.1021/acs.chemmater.3c01407" target="_blank" >https://pubs.acs.org/doi/10.1021/acs.chemmater.3c01407</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1021/acs.chemmater.3c01407" target="_blank" >10.1021/acs.chemmater.3c01407</a>
Alternative languages
Result language
angličtina
Original language name
Non-hydrolytic Sol-Gel Routes to Bifunctional Cu-Ta-SiO<sub>2</sub> Catalysts for the Upgrading of Ethanol to Butadiene
Original language description
The one-step catalytic conversion of bio-based ethanol to 1,3-butadiene is an attractive way to produce this important C4 building block, to be exploited as a sustainable drop-in chemical in the tire and nylon industry. For this catalytic process, bifunctional catalysts combining both redox and acidic properties are required. Here, we leverage non-hydrolytic sol-gel (NHSG) chemistry to prepare tailored Cu-Ta-SiO2 catalysts featuring an open texture, dispersed acidic Ta sites, and small Cu nanoparticles. In the ether route, silicon tetrachloride and tantalum pentachloride undergo polycondensation reactions with diisopropyl ether as the oxygen donor. In the acetamide elimination route, silicon tetraacetate reacts with pentakis(dimethylamido)tantalum(V). In both routes, copper(II) acetylacetonate is added and trapped in a tantalosilicate matrix. Upon calcination, CuO nanoparticles form and the resulting bifunctional material develop a mesoporous texture with specific surface areas in the 650-950 m(2) g(-1) range, pore volumes between 0.75 and 0.90 cm(3) g(-1), and average pore diameters above 3 nm. With the help of NH3-TPD, FTIR, CO- and pyridine-adsorbed FTIR, XRD, XPS, and STEM-EDS, we demonstrate that the catalysts made via the acetamide elimination route show higher performance in the ethanol-to-butadiene reaction, with low selectivity in dehydration byproducts, owing to moderate Lewis acidity, smaller Cu nanoparticles, and higher active site proximity. After optimization of the Ta and Cu loadings, a butadiene productivity as high as 0.38 g(BD) g(cat)(-1) h(-1) is obtained, surpassing state-of-the-art catalysts with similar formulations and tested under similar reaction conditions.
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10402 - Inorganic and nuclear chemistry
Result continuities
Project
Result was created during the realization of more than one project. More information in the Projects tab.
Continuities
P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)<br>S - Specificky vyzkum na vysokych skolach<br>I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace
Others
Publication year
2023
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
CHEMISTRY OF MATERIALS
ISSN
0897-4756
e-ISSN
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Volume of the periodical
35
Issue of the periodical within the volume
17
Country of publishing house
US - UNITED STATES
Number of pages
12
Pages from-to
7113-7124
UT code for WoS article
001059698900001
EID of the result in the Scopus database
2-s2.0-85169900085