Surface-functionalized mesoporous gallosilicate catalysts for the efficient and sustainable upgrading of glycerol to solketal
(2021) Green Chemistry — Vol. 23, n° 1, p. 354-366 (2021)
Files
Vivian2021GreenChemfunctionalizedGa-SiO2aerosolsolketal-preprint.pdf
postprint
Open Access - Adobe PDF
- 954.01 KB
A97-21VivianGreenChemfunctionalizedGa-silicateaerosolsolketal.pdf
Restricted Access - Adobe PDF
- 4.98 MB
Details
- Authors
Vivian, Alvise 
Aprile, Carmela
- Abstract
- Two series of functionalized mesoporous Ga silicates were prepared in a straightforward and sustainable one-pot procedure using different alkyl silanes. The efficacy of the adopted co-synthetic approach based on aerosol processing has been proved by 29Si solid-state NMR experiments revealing a degree of functionalization close to the theoretical value. The successful incorporation of gallium as single sites within the silica framework was confirmed via71Ga solid-state magic-angle-spinning NMR measurements. These materials were tested as catalysts for the synthesis of solketal from glycerol at low temperature and under solventless conditions. A systematic study evidenced the importance of a careful tuning of surface polarity, achievable with surface functionalization as well as with different thermal treatments. The solids functionalized with a low degree of methyl groups (5%) displayed enhanced performances compared to the non-functionalized analogues, highlighting the highly beneficial role of surface hydrophobicity as well as the importance of the careful tuning of the hydrophilic/hydrophobic balance. The best functionalized catalysts proved to be easily reusable for multiple catalytic runs. With such a high-performance catalyst in hand, we propose a process which shows a favorable E-factor, indicating that the production of solketal can be envisaged in a sustainable way.
- Affiliations
Citations
Vivian, A., Soumoy, L., Fusaro, L., Fiorilli, S., Debecker, D., & Aprile, C. (2021). Surface-functionalized mesoporous gallosilicate catalysts for the efficient and sustainable upgrading of glycerol to solketal. Green Chemistry, 23(1), 354-366. https://doi.org/10.1039/d0gc02562c (Original work published 2021)