The Study Of Catalytic Activity To Epoxidation And N-Acylation Reaction Catalyzed By Basic Zeolite ETS-10 And Its Heteroatom Catalyst

In the area of organic synthesis,chalcone and its epoxides are very important intermediate product and precursor for their further transformation to final products synthesized by the ring opening of epoxide,addition reaction of chalcone double bonds and addition of carbonyl.Many functional group organic compounds are prepared through these transformation.Acid amide are also common nitrogenous organic compounds for their extensive application in agrochemical production and pharmaceutical synthesis.They are also indispensable functional group and chemical structure of vital component of life entity.In traditional organic synthesis,most reactions are studied by homogeneous metal catalysts equipped with organic ligands to improve their reaction activity.However,the preparation of homogeneous organic-metal catalysts are very complicated and harmful to environment.Therefore,it is extremely urgent to develop high catalytic activity,economical and recyclable heterogeneous catalysts.Zeolite is a kind of porous material with unique open-framework structure unit,which provide it a degree of acidity,basicity and catalytic activity.Due to the multi-functionalization feature of zeolite,it has extensive applications in organic synthesis and develops into research hotspot of organic area for the past few years.According to these feature and advantages of zeolite,we synthesized basic zeolite ETS-10 and transition metals or noble doped ETS-10 catalysts ourselves in this paper and applied to organic synthesis,which perform high catalytic reactivity as heterogeneous catalysts.This paper include four parts below:The first part: this paper summarized the applications of homogeneous organic metal catalysts in some common coupling reactions,the important role of base in organic synthesis reactions and the development of heterogeneous catalysis.It also elaborated the characteristics and advantages of zeolite and its applications in organic synthesis.The second part: we prepared basic zeolite ETS-10 and studied its catalytic activity to the oxidation coupling reaction of benzaldehyde and styrene,which realized metal-free heterogeneous catalysis to this reaction.Furthermore,we provided the reaction mechanism of this reaction through the capture and detection of radical.The third part: we synthesized transition metals Fe?Co?Ni?Cu doped heteroatom ETS-10 catalyst and applied to the oxidation coupling reaction of benzaldehyde and styrene to study their catalytic activity and compare to that of metal-free ETS-10 catalyst.It suggests that heteroatom ETS-10 perform higher catalytic activity and selectivity compared to ETS-10 and they can catalyze the reaction at harsher conditions.The fourth part: we constructed Pd?NO3?2-CuCl-ETS-10 bimetallic catalyst through iron exchange and discussed its reactivity to N-acyl reaction of N,N-dimethyl benzyl amine.Compared to single-metal catalysis and other zeolite carrier,Pd?NO₃?₂-CuCl-ETS-10 enjoys the advantages of bimetallic catalyst in the reaction which can not be replaced by other catalysts.