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@article{2352429,
author = {Dochain, Denis D and Stýskalík, Aleš and Vykoukal, Vít and Vimont, Alexandre and Travert, Arnaud and Debecker, Damien P},
article_location = {WASHINGTON},
article_number = {17},
doi = {http://dx.doi.org/10.1021/acs.chemmater.3c01407},
keywords = {HETEROGENEOUS CATALYSTS; CONVERSION; ZEOLITES},
language = {eng},
issn = {0897-4756},
journal = {CHEMISTRY OF MATERIALS},
title = {Non-hydrolytic Sol-Gel Routes to Bifunctional Cu-Ta-SiO<sub>2</sub> Catalysts for the Upgrading of Ethanol to Butadiene},
url = {https://pubs.acs.org/doi/10.1021/acs.chemmater.3c01407},
volume = {35},
year = {2023}
}
TY - JOUR
ID - 2352429
AU - Dochain, Denis D - Stýskalík, Aleš - Vykoukal, Vít - Vimont, Alexandre - Travert, Arnaud - Debecker, Damien P
PY - 2023
TI - Non-hydrolytic Sol-Gel Routes to Bifunctional Cu-Ta-SiO<sub>2</sub> Catalysts for the Upgrading of Ethanol to Butadiene
JF - CHEMISTRY OF MATERIALS
VL - 35
IS - 17
SP - 7113-7124
EP - 7113-7124
PB - AMER CHEMICAL SOC
SN - 08974756
KW - HETEROGENEOUS CATALYSTS
KW - CONVERSION
KW - ZEOLITES
UR - https://pubs.acs.org/doi/10.1021/acs.chemmater.3c01407
N2 - 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.
ER -
DOCHAIN, Denis D, Aleš STÝSKALÍK, Vít VYKOUKAL, Alexandre VIMONT, Arnaud TRAVERT and Damien P DEBECKER. Non-hydrolytic Sol-Gel Routes to Bifunctional Cu-Ta-SiO\&{}lt;sub\&{}gt;2\&{}lt;/sub\&{}gt; Catalysts for the Upgrading of Ethanol to Butadiene. \textit{CHEMISTRY OF MATERIALS}. WASHINGTON: AMER CHEMICAL SOC, 2023, vol.~35, No~17, p.~7113-7124. ISSN~0897-4756. Available from: https://dx.doi.org/10.1021/acs.chemmater.3c01407.
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