Construction And Catalytic Research Of Co-Based Metal-Organic Frameworks

Transition metal catalysis has undergone several centuries of development and has made indelible contributions to the progress of human society.Contemporary chemists have been able to design and synthesize special transition metal ligands to construct valuable organic molecules with high efficiency and selectivity.Metal-organic frameworks（MOFs）are a class of emerging materials that combine metal ions or metal clusters with organic ligands through coordination.The infinite and orderly network structure makes them have excellent microporous characteristics:Large specific surface area,modifiable pore structure and more unsaturated metal active sites.Compared with traditional heterogeneous catalysts,good microporous characteristics bring unparalleled catalytic advantages for gas-liquid,gas-solid and gas-liquid-solid reactions.In recent years,the emergence of social issues such as energy crisis and environmental protection has made photocatalysis begin to emerge in the field of catalysis.With the continuous development of photocatalysis technology,more and more people have begun to pay attention to the application of MOFs on the opposite side of photocatalysis.Due to the designability of MOFs,people try to use organic dye molecules with excellent light absorption capacity as organic ligands to coordinate and combine with transition metal nodes to realize the synergistic catalysis of transition metal catalysis and photocatalysis.The heterogeneity of MOFs is also reduced.It can avoid the non-directional problem of charge transfer in a homogeneous system,and is a good platform for exploring the mechanism of synergistic catalysis.In addition,the metal nodes inside the MOFs can also achieve effective adsorption of gas molecules,which provides a very favorable reaction advantage for the photocatalytic oxidation and the photocatalytic reduction of carbon dioxide in an oxygen atmosphere,and the energy utilization of photocatalytic materials Technology upgrades have been achieved in terms of environmental friendliness,and more advanced photocatalytic reaction modes have been continuously developed.In this paper,a cobalt-based metal-organic frameworks Co-DPA with anthracene’s pyrazole-based ligand H₂DPA as the organic dye ligand and cobalt as the metal node is designed and constructed.Under the condition of light excitation,it reflects the effective activation in oxygen atmosphere.The catalytic oxidation of benzylamine compounds and compounds with active C-H bonds is realized.By optimizing the synthesis conditions of Co-DPA,a single crystal of Co-DPA was cultivated and its single crystal structure was determined by a single crystal diffractometer.At the same time,the Co-DPA was also subjected to ultraviolet,infrared,electrochemical,XRD,XPS,The photocurrent response and other test characterizations were analyzed through the characterization results to determine its photocatalytic activity and its ability to activate in oxygen.In subsequent experiments,this article tested the photocatalytic oxidation activity of Co-DPA on benzylamine compounds.Through optimization of conditions,the best reaction conditions were explored.At the same time,the photocatalytic oxidation of benzylamine compounds was also carried out as a substrate.expand.Combining the test characterization information and the discussion about the reaction phenomenon in the experiment,the possible reaction mechanism is proposed.Finally,according to the optimal photocatalytic oxidation reaction conditions that have been explored,the photocatalytic oxidation of Co-DPA on compounds with active C-H bonds was also tested.The results show that Co-DPA has good photocatalytic oxidation activity for benzylamines and materials with active C-H bonds.This paper also designed and constructed a cobalt-based metal-organic framework Co-TCA-1 with triphenylamine tricarboxylic acid as the organic ligand and cobalt as the metal node,and performed single crystal diffraction,XPS,spectroscopy,and electrochemical characterization.test.Using the microporous characteristics of MOFs and the characteristics of Lewis acidic metal cobalt nodes,this paper tested the cycloaddition catalysis of Co-TCA-1 on carbon dioxide and epoxy compounds,completed the optimization of the reaction conditions,and explored the effects of the reaction.factor.The structure shows that Co-TCA-1 has a good catalytic effect on the cycloaddition reaction of carbon dioxide and epoxy compounds.