화학공학소재연구정보센터
Applied Catalysis A: General, Vol.536, 85-96, 2017
Reconstructed Mg-Al hydrotalcites prepared by using different rehydration and drying time: Physico-chemical properties and catalytic performance in aldol condensation
Aldol condensation in presence of reconstructed hydrotalcites as basic catalysts is well documented and attracts an increased attention because it allows producing complex molecules starting from relatively simpler ones. Nevertheless, more studies are necessary for the better understanding of preparation factors that affect the physico-chemical properties of these materials and their catalytic performance. This work considers the effect of the duration of the liquid-phase rehydration of Mg-Al mixed oxide as well as the drying duration of prepared samples on their physico-chemical properties and performance in aldol condensation of furfural and acetone. The properties of all materials were investigated by XRD, TGA, TGAMS, SEM and DRIFT. Experiments on aldol condensation of furfural and acetone were performed by using a stirred batch reactor at T = 25 degrees C with Ac:F =5 molar ratio. The characterization of the prepared materials showed that the recovery of HTC structure occurred within a few seconds of the contact between Mg-Al mixed oxide with liquid water. The content of functional species in all reconstituted HTCs was nearly constant and independent on preparation conditions while the amount of physisorbed water in the prepared samples decreased with increasing drying time. The calcination of as-prepared HTC followed by the subsequent rehydration of Mg-Al mixed oxide resulted in the replacement of > 90% carbonate groups on hydroxyls which are Brensted basic sites. Consequently, the activity of the reconstructed HTCs in aldol condensation of furfural and acetone was significantly higher compared to Mg-Al mixed oxide. The catalytic performance of rehydrated materials was almost independent on rehydration time while furfural conversion decreased if carrying out the reaction in an aqueous medium with increased water content. On the other hand, properly dried reconstructed HTC with the absence of physisorbed water also exhibited a very low activity in the reaction. The effect of Cannizzaro reaction as a simultaneous process with aldol condensation on the composition of reaction products was also considered. The obtained results may be useful for optimizing the preparation conditions of reconstructed HTC as a basic catalyst as well as for evaluating their performance during long-term catalytic tests. (C) 2017 Elsevier B.V. All rights reserved.