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.
Surface-functionalized mesoporous gallosilicate catalysts for the efficient and sustainable upgrading of glycerol to solketal / Vivian, A.; Soumoy, L.; Fusaro, L.; Fiorilli, S.; Debecker, D. P.; Aprile, C.. - In: GREEN CHEMISTRY. - ISSN 1463-9262. - ELETTRONICO. - 23:1(2021), pp. 354-366.
|Titolo:||Surface-functionalized mesoporous gallosilicate catalysts for the efficient and sustainable upgrading of glycerol to solketal|
|Data di pubblicazione:||2021|
|Digital Object Identifier (DOI):||http://dx.doi.org/10.1039/d0gc02562c|
|Appare nelle tipologie:||1.1 Articolo in rivista|