Catalytic Properties And Application Of Novel Polyazole Heterocyclic Ligands Complexes

Metal complexes have always been one of the hotspots in the field of scientific research.Because of their unique properties,many scientists will spend a lot of time to design and synthesis new metal complexes for specific reactions,so that enable the synthesized catalyst to catalyze the reaction,but with the passage of time,the synthesis of metal complexes will be limited,because this homogeneous catalyst can only do one time for reaction.From the energy point of view,it will waste resources.To maximize the utilization of resources,in order to comply with the concept of green chemistry,my work is to continue to find some inorganic materials for grafting on the basis of synthesizing metal complexes to prepare heterogeneous catalysts and apply them to organic synthesis reactions,the ultimate goal is to recycle the catalyst.(1)A pyrazolyl-pyridyl-triazole ruthenium complex was designed,and it was characterized by X-ray single crystal diffractometer,and the metal complex was connected with the inorganic support?Al₂O₃ to obtain a heterogeneous catalyst.SEM,TEM,EDX,XRD,XPS for characterization.After the catalyst was obtained,it was found that the ruthenium catalyst has high activity for the deoxycoupling reaction of 2-arylethanol.For heterogeneous catalysts,it can also be recycled,providing a green synthesis method for preparing aromatic propylene derivatives.(2)Attempt to synthesize naphthyl-pyridyl-triazolyl ruthenium complex,and connect with inorganic carrier silica to prepare supported ruthenium catalyst.In the reaction of2-aminobenzonitrile and benzyl alcohol to prepare quinazolinones derivatives to use this catalyst,the results show that both homogeneous and heterogeneous catalysts exhibit good catalytic activity in the synthesis of quinazolinones.In addition,applying the homogeneous catalyst NTP-Ru to the olefination reaction can still achieve good results.(3)A new asymmetric diphenylphosphino-pyridyl-triazole ligand and cobalt metal complex were synthesized and characterized by IR,NMR and MS.Then by Co-doping C₃N₄,the diphenylphosphino-pyridyl-triazole cobalt complex is converted into a recyclable catalyst.In the reaction of 2-aminobenzyl alcohol and ketone to synthesize quinoline,the synthesized Co@C₃N₄ composite material has high catalytic activity,and can achieve the conversion of the target product with high yield,and has good recovery performance for the synthesis of quinoline.(4)The synthesis of the pyridyl-pyridyl-triazole complex is mainly described.Two pyridine-type skeleton ligands were designed and confirmed by NMR characterization.Then new catalysts were designed.The first catalyst is homogeneous catalyst,which is NNN-Ru catalyst obtained by three coordination methods,and the second catalyst is heterogeneous catalyst.A new type of heterogeneous Ni@MR catalyst was synthesized on Merrifield resin.Moreover,the homogeneous catalyst was applied to the synthesis of pyrrole heterocycles,and the heterogeneous catalyst was applied to the?-alkylation reaction of nitriles and alcohol compounds,and good yields can be obtained.