Design,Synthesis And Properties Of Complexes Based On Polyazole Ligands

Coordination compounds have attracted much attention in the field of catalysis because of their high activity and stability,but their unrecoverability and high cost limit the development speed and application value of complexes.In recent years,with the development of green chemistry,supported catalysts have become one of the research focuses.In this paper,the research status of polyazole heterocyclic compounds and their metal complexes is introduced.Based on the literature research,the research of this subject is aimed at green and high efficiency.Based on the polyazole ligands,a series of supported metal catalysts were prepared.Their structures were verified by various tests,and their catalytic activities were explored in hydrogen borrowing reaction.Finally,recovery experiments were carried out.(1)Based on 1,2,4-triazole,a new tridentate N^N^N ligand(TNP)was designed and synthesized.Through the coordination with Cu(CH3CN)4PF6,a copper complex(TNP-Cu)was formed.Through the ?–? stacking and adsorption of the copper ion,the copper complexes were successfully loaded on the reduction of graphene oxide to prepare a new type of loaded copper catalyst(TNP-Cu@r GO).The catalyst was characterized by SEM,TEM,EDX,XPS to verify its structure,and It has good catalytic activity in two kinds of hydrogen borrowing reactions.At last,the recovery experiment shows that the stability of the system is general.(2)A new iridium complex(PT-Ir)was successfully prepared by coordination of(pentamethyl-cyclopentadienyl)iridium chloride dimer with phenyltetrazole as ligand.Its structure was verified by X-ray crystallographic analysis.On this basis,using(3-isocyanatopropyl)triethoxysilane as coupling agent,the inorganic phase SBA-15 is connected by hydrolysis,and the organic phase ligand phenyltetrazolium is connected by the condensation of isocyanate group and amino group.A new modified carrier is prepared,and then coordinated with [Cp*Ir Cl2]2 in methanol,leading to a recoverable heterogeneous iridium catalyst(PT-Ir@SBA-15).It was applied to the synthesis of quinoline and diaryletone,and the results show that it has good catalytic activity and selectivity.(3)the novel unsymmetrical triazolyl-pyridyl-pyridine ligand(TPP)was designed and synthesized,which were coordinated with iron bromide to obtain the Fe(II)complexes(Fe-TPP).The structure of the complex was verified by X-ray crystallographic analysis.It was a six-coordinated complex by two ligands.Based on the function of coupling agent,the complex was successfully loaded on titanium dioxide microspheres by(3-isocyanatopropyl)triethoxysilane,the structure of it(Fe-TPP-TOS)was verified by various kinds of characterization,and it has good catalytic activity and stability in the hydrogen borrowing reaction.