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

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.

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Supplementary files

Article information


Submitted
26 Jul 2020
Accepted
07 Oct 2020
First published
09 Oct 2020

Green Chem., 2020, Accepted Manuscript
Article type
Paper

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

A. Vivian, L. Soumoy, L. Fusaro, S. L. Fiorilli, D. P. Debecker and C. Aprile, Green Chem., 2020, Accepted Manuscript , DOI: 10.1039/D0GC02562C

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