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Zirconium doped mesoporous silica catalysts for dehydration of glycerol to high added-value products

Paper ID Volume ID Publish Year Pages File Format Full-Text
40886 45869 2012 9 PDF Available
Title
Zirconium doped mesoporous silica catalysts for dehydration of glycerol to high added-value products
Abstract

A series of zirconium doped mesoporous silica, with different Si/Zr molar ratios, has been synthesized and tested in the gas-phase dehydration of glycerol. The surface characterization of these solids by using NH3-TPD and pyridine adsorption coupled to FTIR spectroscopy has revealed the existence of well dispersed acid sites, mainly of Lewis type, associated to Zr(IV) species deficiently coordinated located on the pore walls of the siliceous framework. These acid catalysts are active in the glycerol dehydration, increasing the conversion with the zirconium content until values higher than 90 mol% for a Si/Zr molar ratio of 4, at 325 °C after 5 h of reaction. However, the catalysts suffer deactivation, which is more important when zirconium oxide is incorporated by impregnation of mesoporous MCM-41 silica. The main reaction products were acrolein, acetaldehyde and acetol. Moreover, the catalysts with a SiZr molar ratio higher than 5 are more selective to acetaldehyde. The acrolein yield was, in all cases, lower than 15 mol% after 24 h of TOS, but a pretreatment under a helium flow saturated with water vapour allows reaching an acrolein yield of 28 mol% and ameliorates the stability of catalysts. The selectivity towards acrolein and hydroxyacetone can be explained by considering the influence of the nature of active sites.

Graphical abstractFigure optionsDownload full-size imageDownload high-quality image (75 K)Download as PowerPoint slideHighlights► SiZrx catalysts display both Brönsted and Lewis acid sites. ► They are active in the gas-phase dehydration of glycerol. ► Long-term stability is ameliorated by steaming treatment of catalysts. ► The selectivity can be explained by considering the nature of acid sites.

Keywords
Mesoporous silica; Glycerol; Zirconium oxide; Acid catalysis; Acrolein
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Zirconium doped mesoporous silica catalysts for dehydration of glycerol to high added-value products
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis A: General - Volumes 433–434, 8 August 2012, Pages 179–187
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
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Price was $35.95
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Price after discount Only $4.95
100% Money Back Guarantee
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