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Elucidating the effect of hydrophobicity of methyl-functionalized mesoporous titanosilicate in the epoxidation of olefins
Manangon Perugachi, Pedro Daniel;Smeets, Valentin;Vivian, Alvise;Aprile, Carmela;Gaigneaux, Eric;et.al.
(2022) 9th World Congress on Oxidation Catalysis — Location: Cardiff, UK (2022.September.4AD)
Methyl-functionalization was achieved by a partial substitution of tetraethoxy silane (TEOS) by methyltriethoxy silane (MTES) in different ratios. Titanium butoxide (TiBut) was used as Ti precursor to reach nominal Ti molar ratios (Ti/(Si+Ti)) of 0.020 and 0.025. The precursor solution was atomized, and the collected powder was aged and calcined at 623 K. Solid-State 29Si-NMR, FTIR, TGA and vapor-phase water adsorption showed that methyl moieties were effectively incorporated, conferring a hydrophobic character to the Ti-SiO2 catalysts. Our Ti- SiO2 catalysts exhibited three effective degrees of methyl-functionalization: 3%, 9%, and 14%, which were compared to a pristine Ti-SiO2 as a reference. ICP-AES, DRUV, XPS, and N2 physisorption demonstrated that Ti dispersion and textural properties were both successfully preserved upon the incorporation of the methyl moieties. Hydrophobic Ti-SiO2 showed higher catalytic performance in the epoxidation of cyclooctene with tert-butyl hydroperoxide than the pristine analogous prepared without MTES. In addition to isolating the positive effect of hydrophobization of Ti-SiO2 on their catalytic performance, this work demonstrates that the aerosol route is more advantageous than the conventional sol-gel route to prepare functionalized mesoporous Ti-SiO2 catalysts with highly dispersed active sites.
Manangon Perugachi, P. D., Smeets, V., Vivian, A., Aprile, C., Debecker, D., & Gaigneaux, E. (2022). Elucidating the effect of hydrophobicity of methyl-functionalized mesoporous titanosilicate in the epoxidation of olefins. 9th World Congress on Oxidation Catalysis, Cardiff, UK. https://hdl.handle.net/2078.5/25048