Surface-functionalized mesoporous gallosilicate catalysts for the efficient and sustainable upgrading of glycerol to solketal

Alvise Vivian, Loraine Soumoy, Luca Fusaro, Sonia Lucia Fiorilli, Damien P Debecker, Carmela Aprile

Research output: Contribution to journalArticlepeer-review

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 via 71Ga 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 high-performance catalyst in hands, we propose a process which show favorable E-factor, indicating that the production of solketal can be envisaged in a sustainable way.
Original languageEnglish
JournalGreen Chemistry
DOIs
Publication statusPublished - 2020

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