Research In Mesoporous Nanoreactor And On-water Reaction

On the basis of predecessors’ research, an interesting phenomenon was found: some special catalysts could influence the chemical equilibrium of esterification reaction, even change the chemical reaction equilibrium constant. On this basis, we found that mesoporous nanoreactor(a kind of heterogeneous catalyst) and the waterphase system(a kind of heterogeneous reaction medium) can influence the microprocess of organic reactions. Accordingly, the process would influence the reaction kinetics, reaction thermodynamics, chemical reaction selectivity and the enantioselective.We mainly research of mesoporous inorganic nanoreactor MCM- 41, SBA- 15 and disordered mesoporous silica. After modifying them, the mesoporous channel can be used as a special kind of micro environmental and impact reaction process. We investigated the effect of nanoreactor as a catalyst for Michael reaction and the aza-Michael reaction. Experiments have the huge specific surface energy of nanoreactor will directly affect the energy of compounds and the microprocess of reactions. As a concrete manifestation, the reaction rate would increase and the reaction yield or selectivity would improve.In the process of research, we found that nanoreactor can promote certain reaction, but other reactions were suppressed by nanoreactor. In view of this, we have surveyed the effect of heterogeneous medium(on-water reaction). Compared with nanoreactor, on-water reaction not only has the advantages of nanoreactor but also has the characteristic that nanoreactor does not own.The paper is divided into the following two parts:The first part introduces the inorganic porous nanoreactor, micellar nanoreactor, biological nanoreactor, other kind of nanoreactor and their application. We mainly introduced mesoporous nanoreactor MCM-41 and SBA-15.Then, we summarized some main theory explanation of on-water reaction.The second part is the experiment content, mainly including the following aspects:1. Preparation of a series of mesoporous nanoreactor, such as the modified product of mesoporous nanoreactor MCM-41/SBA-15. And these catalysts were characterized;2. Aza-Michael reaction as the model reaction, the effect of nanoreactor PMoA/MCM-41 was studied;3. In the catalytic process of the nanoreactor PMoA/MCM-41 for the azaMichael reaction of hydrazide with unsaturated ketones, we investigated the effect of nanoreactor for the chemical selectivity;4 In the catalytic process of the nanoreactor MCM-41-QN for the Michael reaction of chalcone ketones with malononitrile, we investigated the effect of nanoreactor for the enantioselectivity;5. The Knoevenagel condensation under on-water condition was studied. We proposed a new mechanism and predict a new on-water reaction.