WVOx Supported on Industrial Al2O3, SiO2, AC, TiO2–Al2O3 for Catalytic Dehydration of Gas-Glycerol to Acrolein
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Organometallic Chemistry
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Organometallic Chemistry
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The catalytic dehydration of glycerol to acrolein is a very attractive alternative to the propylene-based process, due to the future exhaustion of fossil feedstocks and the increasing production of biomass-based glycerol. This work aimed to study the selectivity control over Cs2.5H0.5PW12O40/Nb2O5 (CsPW-Nb). The Brønsted and Lewis acid sites were characterized by FTIR to understand the catalytic mechanism. The effects of reaction temperature (260−360 °C), oxygen co-feed ratio (0−0.175), and glycerol concentration (0.2−0.5 g/g) were studied to determine the optimum conditions for the production of acrolein. The loading of CsPW on Nb2O5 increased the Brønsted acidity and enhanced the acrolein dehydration route. Co-feeding oxygen at an appropriate ratio significantly enhanced the selectivity of the acrolein dehydration route and slightly enhanced the selectivity of the acetol dehydration route by suppressing the glycerol oligomerization reaction. The selectivity to acrolein significantly decreased when the glycerol concentration increased from 0.2 to 0.5 g/g due to increased glycerol oligomerization reactions. The acrolein selectivity in dehydration of glycerol was affected by reaction temperature, oxygen co-feeding, and glycerol concentration. The highest acrolein selectivity (76.5 %) was obtained at 320 °C, O2/N2/glycerol molar ratio of 1/5/0.16 (mol/mol), and glycerol concentration of 0.2 g/g.
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The increase of biodiesel production results in the accumulation of glycerol, which requires an increasing demand towards the study of chemical application of glycerol. Glycerol has to be transformed to other valuable chemicals, which can be used as starting materials for organic synthesis. With the final goal to find a reasonable solution for this problem we have studied the dehydration of glycerol in liquid phase using a supported HPA catalyst and developed an environmentally benign production of acrolein. Our method does not have any extreme conditions and produces a total conversion with high (93%) selectivity.
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BACKGROUND The valorization of glycerol obtained from biodiesel production is a challenging task. Effective use or conversion of crude glycerol to specific products will further reduce the cost of biodiesel production. RESULTS Vapour phase dehydration of glycerol to acrolein was investigated over solid acid catalysts containing nio-biumoxophosphate (NbP) by varying the calcination temperature. All the catalysts prepared were active for the synthesis of acrolein (conversion of glycerol was observed in the range 75–100% with selectivity to acrolein in the range 69–86%). The acidic properties are correlated with catalytic functionalities during dehydration of glycerol. CONCLUSIONS The NbP catalyst calcined at 550 °C has shown higher selectivity to acrolein with total conversion of glycerol. Calcination of the samples at 350 to 650 °C produces amorphous NbP sample, which contains significantly higher fractions of moderate acid sites than the crystalline NbP. The higher activity during glycerol dehydration and acrolein selectivity exhibited by NbP-550 catalyst is attributed to the presence of only moderate acidic sites with the majority of them Brønsted acidic sites. © 2013 Society of Chemical Industry
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