Publication details

Highly porous hybrid metallosilicate materials prepared by non-hydrolytic sol-gel: Hydrothermal stability and catalytic properties in ethanol dehydration



Year of publication 2020
Type Article in Periodical
Magazine / Source Microporous and Mesoporous Materials
MU Faculty or unit

Faculty of Science

Keywords Non-hydrolytic sol-gel; Hybrid metallosilicate; Hydrothermal stability; Heterogeneous catalysis; Ethanol dehydration
Description Herein, we present novel phenylene- and xylylene-bridged silica and metallosilicate materials prepared by non-hydrolytic sol-gel. The hybrid silica are highly porous, chemically similar to periodic mesoporous organosilica (PMO), but amorphous without any pore ordering. Analogous hybrid metallosilicates are obtained by directly incorporating Al, Nb, or Sn in the hybrid silica framework. Exhibiting open texture, surface acidity and tunable hydrophobicity, these materials are excellent candidates for catalytic alcohol dehydration reactions. The gas-phase hydrothermal and thermal stability of these materials is examined. While the hybrid silica is expectedly stable, a stark decrease in stability is observed for phenylene bridged silsesquioxanes upon metal introduction. The extent of the hydrolytic Si-C(sp(2)) bond cleavage is quantitatively followed by Si-29 MAS NMR, TG analysis, and GC-FID analysis of effluent coming from samples exposed to water vapor. Two important features affecting the hydrothermal and thermal stability are identified: (i) the homogeneity of metal dispersion within the silica matrix, and (ii) the electronegativity of the incorporated metal. The stability of hybrid metallosilicates is significantly improved by replacing the phenylene bridges with xylylene bridges, due to the presence of more stable Si-C(sp(3)) bonds. Interestingly, the latter hybrid metallosilicate proves to be an active catalyst for the dehydration of ethanol to ethylene. Unlike the other hybrid materials presented here, it reaches high ethylene yields without undergoing degradation and deactivation.
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