Study On Preparation And Catalytic Performance Of Metal Ruthenium-based Immobilized Photocatalyst

Transition metal complexes can catalyze organic synthesis under light induction,and such substances that play a catalytic role under light induction are called photocatalysts.These metal complexes that can catalyze organic synthesis under light induction mainly include complexes of noble metals such as ruthenium and iridium.At present,such catalysts are mainly used in homogeneous catalytic reaction systems.Since it is difficult to recycle the catalyst for homogeneous reaction,this article intends to immobilize the ruthenium complex on the carrier to study its preparation process and catalytic performance.The details are as follows:1.Preparation and characterization of immobilized ruthenium complex photocatalystUsing organic polymer resin as the carrier,pretreating the carrier with methylamine,ethylamine,dimethylamine and aniline,and then fixing the photocatalyst terpyridine ruthenium chloride hexahydrate on the carrier,successfully preparing the immobilized ruthenium complex Photocatalyst,and analyzed the preparation process of the solid-supported ruthenium complex photocatalyst according to the material properties and reaction characteristics,and constructed the process flow of the solid-supported ruthenium complex photocatalyst:elimination reaction,solid-liquid separation,washing solid-liquid separation,After drying,a photocatalyst supported by a ruthenium complex can be obtained.The structure,morphology and specific surface area of the prepared ruthenium complex photocatalyst were analyzed by element analysis,infrared absorption spectroscopy,atomic absorption spectroscopy,transmission electron microscopy and specific surface area.The results showed that the catalyst was successfully immobilized on the supports of different pretreatment methods.Among them,the catalyst pretreated with methylamine had the largest amount of 2.148 mg/gcatalyst;the catalyst pretreated with dimethylamine had the least amount of catalyst immobilized.0.171 mg/gcatalyst.2.Photocatalytic preparation of benzil with different biphenylalkynes as raw materialsTaking the synthesis of benzil as the research object,the raw materials of the reaction are biphenylalkynes,4-chlorothiophenol and oxygen.The above-mentioned solid-supported ruthenium complex photocatalysts are used as catalysts to study the reaction under different catalysts.Yield.The results show that the performance of the catalyst prepared by methylamine pretreatment is the best,with a yield of 51%,followed by the ruthenium complex photocatalyst pretreated with aniline,with a yield of 35%;while the yield of the ruthenium complex pretreated with ethylamine and dimethylamine is 35%.The complex photocatalyst cannot catalyze the progress of the reaction.The immobilized ruthenium complex photocatalyst pretreated with methylamine has a catalytic effect in the oxidation of different diphenylalkynes to benzyl.3.Study on the photocatalytic preparation of bibenzoyl by immobilized ruthenium complexTaking the reaction of synthesizing bibenzoyl as the research object,the raw materials of the reaction are diphenylacetylene,4-chlorothiophenol and oxygen,and the optimal solid-supported catalyst obtained in the above process is used as the catalyst.The effects of reaction time,catalyst dosage,reducing agent dosage and catalyst application times on yield were discussed.The results show that with the increase of the reaction time,the amount of catalyst,and the amount of p-chlorothiophenol,the yield gradually increases and eventually stabilizes,at 0.2 mmol diphenylacetylene,0.1 g catalyst,0.4 mmol 4-chlorothiophenol,Room temperature,under air conditions,under 5 W blue light irradiation for 8 hours,the yield can reach up to 53%;the number of catalyst cycles has no obvious effect on the yield,and the purpose of recycling is achieved.4.Study on the photocatalytic preparation of N-acetyl-1,2-diarylethylamine by immobilized ruthenium complexTaking the synthesis of N-acetyl-1,2-diarylethylamine as the research object,the raw materials of the reaction are p-nitrobenzenediazonium tetrafluoroborate,4-chlorostyrene,water and acetonitrile,and the catalyst is solid Supported ruthenium complex photocatalyst.The applicability of the catalyst is further discussed;the influence of reaction time,catalyst dosage,reactant ratio and the number of catalyst applications on the yield is discussed.The results show that the catalyst has applicability in the synthesis of N-acetyl-1,2-diarylethylamine;as the reaction time,the amount of catalyst,and the amount of reducing agent increase,the yield gradually increases and eventually stabilizes.,In 0.2 mmol p-nitrobenzenediazonium tetrafluoroborate,0.4 mmol 4-chlorostyrene,0.2 mmol H2O,0.09g catalyst,0.8 mL acetonitrile as the reactant and solvent at the same time at room temperature(25℃)5 Under W blue light irradiation for 5 hours,the yield can reach up to 54%;the number of catalyst applications has no significant effect on the yield.