Innovative sol-gel routes to mesoporous bifunctional catalysts for the upgrading of bioethanol to butadiene

Dochain, Denis D.;Styskalik, Ales;Debecker, Damien
(2022) 9th World Congress on Oxidation Catalysis — Location: Cardiff, UK (4.September.2022)

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  • Dochain, Denis D.UCLouvain
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  • Styskalik, AlesUCLouvain
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Abstract
Here, NHSG was used to prepare bifunctional Ta-Cu-SiO2 catalysts via the acetamide elimination route (“Ac”) and compare them with similar compositions obtained through the ether route (“Et”). Both pathways yielded mesoporous materials (SSA≈600 m2 g–1; Vp≈0.1 mL g–1; Dp≈4.0 nm for the acetamide elimination route, SSA≈700 m2 g–1; Vp≈0.1 mL g–1; Dp≈7.0 nm for the ether route). IR spectroscopy and XPS pointed to a successful Ta incorporation inside the silica matrix. For a given catalyst composition, the butadiene yield is systematically better with the catalysts obtained through the acetamide elimination route (Figure 1A). After optimization of the Cu and Ta loadings to notably maximize the selectivity of the oxidation step, the best formulation (Ac-2Ta4Cu) reached an ethanol conversion of 75 % and a butadiene yield of 36 %. The overperformance of the acetamide route is attributed to a better active sites dispersion, availability and proximity, as shown in STEM-EDS images (Figure 1), as well as XPS and IR. Cu nanoparticles are closer to more available Ta isolated sites, allowing for the long reaction mechanism to take place in a facilitated way and limiting unwanted by-products like ethylene.
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Dochain, D. D., Styskalik, A., & Debecker, D. (2022). Innovative sol-gel routes to mesoporous bifunctional catalysts for the upgrading of bioethanol to butadiene. 9th World Congress on Oxidation Catalysis, Cardiff, UK. https://hdl.handle.net/2078.5/26112