Preparation Of SiMoV_n@rht-MOF-1 And Catalytic Reaction Of Alkylbenzene And Alcohol Oxidation

The oxidation reaction,which is commonly employed in the chemical industry to generate ketones,aldehydes,carboxylic acids,and other oxygen-containing functional groups,is an important aspect of modern organic chemistry.However,in an industrial carbonyl compound manufacturing system dominated by potassium permanganate,the homogeneous catalyst frequently encounters issues such as reaction vessel corrosion and recovery difficulty.As a result,developing a non-polluting,recyclable catalyst to replace the existing system remains a difficult task in the sector.To begin,three types of vanadium substituted silicomolybdic heteropoly acids with Keggin structure were prepared using a step-by-step acidizing method,then loaded into the metal-organic cage of rht-MOF-1 using a solvothermal one-pot method,yielding a series of SiMoV_n@rht-MOF-1.Based on the preliminary determination of its composition and properties by means of IR,TG and XRD,it is confirmed that SiMoVn is successfully immobilized in the pore structure of rht-MOF-1 by means of single crystal diffraction.After that,we applied the synthesized crystal complexes to the heterogeneous oxidation of alkylbenzene and alcohols,and proved that the catalysis and stability of SiMoVn@rht-MOF-1 are better than most of the reported similar catalysts,and successfully overcome the inherent shortcomings of difficult recovery and easy elution of POMs.Finally,the possible mechanism of selective catalytic oxidation was verified by EPR,XPS and radical quenching experiments.To sum up,the research content of this paper puts forward a new idea for the improvement of POMs catalysts,which is helpful to solve the defects such as difficult recovery and easy deactivation of the existing transition metal heterogeneous catalysts.It also provides a unique solution and reference value for scientific problems such as precision synthesis,heterogeneous catalysis and reaction mechanism of POMs@MOFs materials.