Synthesis Of Multi-nitrogen Heterocyclic Ligand And Research In Borrowing Hydrogen Reaction

Borrowing hydrogen reaction,also called the hydrogen transfer reaction,makes use of metal catalyst to take away hydrogen in the low active organic compound,activates organic compound to participate in subsequent reaction and form one intermediate,and finally metallic hydrogen restores intermediate and form a new product.Meanwhile,by-product of the reaction is water,hydrogen or ammonia and there is high atom economy during catalytic action.Therefore,borrowing hydrogen reaction is called a kind of green reaction,which is conducive to industrial production.Although this reaction have avoided abuses in some formal methods,borrowing hydrogen reaction needs large amount of catalyst,and poor selectivity and Substrate expansion affects its application value to some extent.In this paper,the synthesis of multi-nitrogen heterocyclic ligands can overcome these shortcomings,three homogenous and heterogeneous metal-catalysts can be synthesized by multi-nitrogen heterocyclic ligands,and the catalyst can be applied to hydrogen transfer reaction.Main thoughts are as follows:(1)In this paper,one kind of new 1,2,4-triazole multi-nitrogen heterocyclic ligand is synthesized,1,2,4-triazole iridium metal complex can be prepared by reaction with iridous chloride,loaded on the MCM-41,and finally one kind of heterogeneous catalyst MT-Ir is formed.Isoindoline ramification can be synthesized by borrowing hydrogen reaction between alcohols and amine under the catalyst,which is the main substance used for anti-cancer drug synthesis.Therefore,the catalyst has extremely high medical value,and the reaction can be completed under solvent-free condition.The reaction is a high-yield and high-substrate-applicability green reaction with recovered catalyst.Finally,a possible reaction mechanism was proposed in the mechanism exploration.(2)In this paper,one kind of new unsymmetrical triazole multi-nitrogen heterocyclic ligand has been synthesized.Unsymmetrical triazole iridium metal complex is prepared by reaction with iridous chloride and is loaded on the hydrotalcite.Finally,one kind of heterogeneous catalyst IPT-Ir-HT has been obtained.Double bond amine is synthesized by borrowing hydrogen reaction between amine and amine under water solvent and tends to form secondary amine by changing the solvent,which is a kind of catalyst for optional products.This reaction's solvent is water.The reaction is a high-yield and high-substrate-applicability green reaction with recovered catalyst.During mechanism explore,there is a possible reaction mechanism during the reaction of amine.(3)Finally,in this paper,1,2,3-triazole multi-nitrogen heterocyclic ligand has been synthesized.In the original plan,one kind of triazole copper metal complex can be prepared after reaction between triazole ligand and iodobis(triphenylphosphino)copper,but the triazoledoes not coordinate with iodobis(triphenylphosphino)copper by single crystal scanning,iodobis(triphenylphosphino)copper coordinates with itself,and one kind of copper cluster with three-cycle structure.The catalyst is more stable than original iodobis(triphenylphosphino)copper.For similar reaction in(2),two copper catalysts have different products.This reaction is high-yield and high-substrate-applicability,catalyst is cheap and eases to synthesize.Finally,triazole is synthesized after a borrowing hydrogen reaction between amine-hydrazine and alcohol,and there is a possible reaction mechanism for the reaction process.