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Synthesis and performance of highly dispersed Cu/SiO2 catalysts for the hydrogenolysis of glycerol

Paper ID Volume ID Publish Year Pages File Format Full-Text
45313 46409 2014 12 PDF Available
Title
Synthesis and performance of highly dispersed Cu/SiO2 catalysts for the hydrogenolysis of glycerol
Abstract

The performance of Cu/SiO2 (commercial silica gel, SBA-15 and SBA-15 treated at 900 °C) catalysts for the hydrogenolysis of glycerol to propylene glycol is investigated with emphasis on the stability characteristics. Cu catalysts with large crystals, small monodisperse crystallites or a highly dispersed XRD amorphous copper phase were obtained after calcination in stagnant air, in a flow of NO/N2 or a flow of air, respectively. Analysis by XRD, N2O surface oxidation and TEM confirmed the variation of the Cu specific surface area by the calcination conditions and the type of silica support used. The different dispersion characteristics resulted in different activities (20–50% glycerol conversion), while all the catalysts proved to be highly selective towards propylene glycol (92–97%). Present results indicate that glycerol hydrogenolysis over Cu-based catalysts is a structure sensitive reaction as significant variations in initial TOF were observed as a function of varying Cu crystallites. It is shown here that the presence of a solvent greatly influences the intrinsic reaction rate and the nature of structure sensitivity. The deactivation behaviour of all catalysts was studied, and based on detailed characterization of the spent samples it was attributed to Cu sintering and the presence of strongly adsorbed species on the catalytic surface. The 18 wt%Cu/silica gel (air) catalyst presented only moderate deactivation (∼20%) while the catalyst supported on SBA-15 calcined at 900 °C (SBA900C) proved to be the most stable with negligible deactivation after three consecutive runs.

Graphical abstractFigure optionsDownload full-size imageDownload as PowerPoint slideHighlights► Glycerol selectively converted to 1,2-propanediol over Cu/SiO2 with high TOFs. ► Different calcination conditions led to different morphological characteristics. ► Glycerol hydrogenolysis proved to be a structure sensitive reaction. ► Deactivation was attributed to Cu sintering and adsorbed species on the surface. ► Thermal treatment of the parent SBA at 900 °C resulted in a stable support material.

Keywords
Glycerol hydrogenolysis; Cu/SiO2 catalysts; Calcination treatment; Deactivation; SBA-15
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Synthesis and performance of highly dispersed Cu/SiO2 catalysts for the hydrogenolysis of glycerol
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis B: Environmental - Volume 145, February 2014, Pages 108–119
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
Get Full-Text Now
Don't Miss Today's Special Offer
Price was $35.95
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Price after discount Only $4.95
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Any Questions? feel free to contact us