The Research Of Functional Metal Organic Frameworks Catalyzed Tandem Reaction

In recent years, metal-organic frameworks (MOFs) as a catalyst in the field of synthetic chemistry has been significant development. MOFs have the highest porosity in all materials and their pore size, shape, and dimensions can be finely regulated. The design diversity of MOFs materials for its application in the field of catalysis provides a clear advantage. The active sites of MOFs may be present on the metal or metal cluster nodes, organic ligands and it also can be the active guest that introduced into the pores or voids of the MOFs. The metal-organic frameworks can be chemically designed as a functional material with multiple catalytic active sites at the same time, which makes it possible for a catalyst to catalyze a tandem reaction.In the first chapter, we briefly introduced the structure and application performance of metal-organic frameworks materials,summarize the research achievements of metal-organic frameworks from birth to rapid development, and the current research status of functional MOFs materials in catalysis of tandem reaction.The second chapter has introduced the synthesis and activation methods of MIL-101 (Al,Cr,Fe) and NH2-MIL-101 (Al,Cr,Fe) series of metal-organic frameworks materials, and chemical characterization was carried out. XRD and IR show that two series of MOFs materials have been successfully synthesized, and the crystallinity of NH2-MIL-101 (M =Al,Cr,Fe) can be clearly compared.In the third chapter, we used NH2-MIL-101 (Al, Cr, Fe) to catalyze a tandem reaction: Deacetalization reaction-Knoevenagel condensation reaction, all the materials show good catalytic effect. Under the optimum reaction conditions, we compared the catalytic effect of NH2-MIL-101 (M = Al, Cr, Fe) on the tandem reaction. The theoretical analysis shows that crystal crystallinity is an important reason for the difference of their catalytic effect.In the fourth chapter, the noble metal Pd nanoparticles were introduced into the pores of NH2-MIL-101 (Al, Cr, Fe) by over-impregnation method and the functional materials Pd@NH2,MIL-101 (Al, Cr, Fe) were synthesized. The chemical characterization showed that Pd nanoparticles were successfully introduced into the pores of MOFs and the loading process did not destroy the framework and functional sites of MOFs.In the fifth chapter, we used Pd@NH2-MIL-101 (Al, Cr, Fe) to catalyze a tandem reaction: Alcohol oxidation reaction-Knoevenagel condensation reaction. they all show good catalytic effect. Under the optimum reaction conditions, the catalytic effect of Pd@NH2-MIL-101 (M = Al, Cr, Fe) on the tandem reaction was compared. The theoretical analysis shows that the uniformity of the nanoparticles in the pores and the synergistic effect between the ions are important reasons for the difference of their catalytic effect.The sixth chapter summarized the work we have done, and provide reference for the research of metal skeleton materials in the catalytic reaction.