In this paper, we reported the first use of phosphate fertilizers (MAP, DAP, and TSP) as heterogeneous catalysts for organic reactions. Their catalytic activities were investigated in the first time in Knoevenagel condensation of various aromatic aldehydes with malononitrile at room temperature. These minerals phosphate showed high catalytic activities and ability to be recovering and reusing without a significant loss in their catalytic activities. In order to reach the optimal reaction conditions for Knoevenagel condensation, we carried out a kinetic study of the effect of reaction time, the effect of solvent, the amount of catalysts and the variation of the range of the particles size the more active. The best conditions were obtained by the use of these fertilizers (MAP, DAP, and TSP) in their commercial status, simply crashed in powder, without any purification, using ethanol as solvent. These phosphate fertilizers prove to be very promising and effective heterogeneous catalysts for the condensation of Knoevenagel.
The novelty of this work is to propose a new process consisting to the modification of triple superphosphate (TSP) by sodium nitrate (NaNO3) for the preparation of a heterogeneous catalytic support Na2Ca(HPO4)2 (calcium hydrogen disodium phosphate). This product has been characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and infrared spectroscopy (IR). The catalytic activity of Na2Ca(HPO4)2 was examined in Knoevenagel condensation between 4-chlorobenzaldehyde and malononit rile as a model reaction. The optimization of the reaction operating conditions was carried out based on a study of the effect of various parameters, namely reaction time, the catalyst charge, the nature, and volume of solvent on the reaction yield. From these considerations, this catalyst proves its efficiency since it allows to obtain the product with excellent yields in a short reaction time. Moreover, it has been reused several times without any significant loss of its activity. The process developed herein can be considered as an ecological and economical method because the catalyst used is non-toxic, cost-effective and easy to prepare.
A simple, efficient, and green procedure has been developed for the synthesis of dihydropyrimidinones (Products of Biginelli) using phosphate fertilizers (mono-ammonium phosphate (MAP), di-ammonium phosphate (DAP) and triple super phosphate (TSP)) as catalyst. The one-step reaction involved the three compounds, which are registered aromatic aldehydes, dicarbonyl compounds and the urea/thiourea. This new method provides some advantages such as obtaining excellent yields (98%), as well as the short duration of the reaction, which may attain 2 minutes. These catalytic heterogeneous systems present also the advantage of being easily recycled.
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