Flow-synthesis of mesoporous silicas and their use in the preparation of magnetic catalysts for Knoevenagel condensation reactions

Mesoporous silica MCM-41 was successfully prepared by flow synthesis in a microreactor at shorter reaction times (i.e., minutes versus day) at high yield (i.e., 60% calcined sample) to give particles of more uniform size and shape compared to MCM-41 prepared by conventional batch synthesis. Magnetic iron oxide nanoparticles were incorporated and organic amines (i.e., propylamine and propyl diethylene amine) were grafted to obtain magnetic mesoporous catalysts for the Knoevenagel condensation reactions of benzaldehyde with ethyl cyanoacetate, ethyl acetoacetate and diethyl malonate. The incorporation of magnetic nanoparticles and large organic amines can hinder reactants access to the catalyst resulting in lower reactivity. NH2-magMCM-41 showed superb catalyst activity and selectivity for the all three Knoevenagel condensation reactions studied. The catalyst can be easily dispersed into solution and rapidly removed by a magnet for recovery and reuse.

Flow-synthesis of MCM-41 in a microfluidic reactor produces small spherical MCM-41 particles (0.5 ± 0.1 μm) with narrow particle size distribution that could be converted into high active magnetic mesoporous base catalysts for Knoevenagel condensation reactions.Figure optionsDownload high-quality image (175 K)Download as PowerPoint slideHighlights
► Flow-synthesis of MCM-41 was successfully implemented in a microfluidic reactor.
► MCM-41 with smaller particle size and narrow PSD was obtained by flow-synthesis at 2 min residence time.
► The MCM-41 was successfully converted into magnetic mesoporous base catalysts after incorporating magnetic nanoparticles and grafting organic amines.
► NH2-magMCM-41 with grafted propylamines have superb catalytic activity and selectivity for Knoevenagel condensation reaction.
► NH2-magMCM-41 is easily dispersed into the reaction mixture and can be readily recovered using a magnet.