Study On The Homogeneous Catalysis Of Carbonyl Reductive Amination Reaction With Ruthenium-Bisphosphine Bisamino Acid Complex

Organic amines are necessary chemical substances in many research fields and industrial production such as chemistry,medicine,biology and material science.Among them,primary amines are important structural units of fine chemicals and bulk chemicals,and are also general materials and key intermediates of advanced chemicals,life science molecules and polymers.It is one of the best methods to synthesize primary amines using ammonia as the ammonia source and hydrogen as the reducing agent to directly realize the catalytic reductive amination of carbonyl compounds.Although the most widely used method in the industry is the heterogeneous reductive amination reaction catalyzed by the metal element,there are still some problems as poor selectivity and difficult to modify the structure.In contrast,the homogeneous catalytic reductive amination of metal complexes has good selectivity and reactivity,but ammonium salts or stoichiometric reducing agents still exist.In order to overcome these problems,it is necessary to develop a green and environmentally-friendly homogeneous catalytic system to realize the efficient reductive amination of carbonyl compounds under the condition of using ammonia as the ammonia source and hydrogen as the reducing agent.In this paper,based on literature review,a Ru complex with a bisphosphine ligand and two carboxylate ligands was determined as a homogeneous catalyst for reductive amination reaction.The applicability of the substrate of the system was investigated,and the mechanism was studied through experimental design and nuclear magnetic analysis.The specific contents are as follows:(1)The reference method synthesizes the target Ru complex,but the synthesis of similar Fe catalysts with the same ligand was failed due to the incompatibility of the ligand with the metal and the possible steric hindrance that hinders the formation of the complex.(2)Ru homogeneously catalyzes the reductive amination of aldehydes,explores the optimal reaction conditions for template reactions and expands the substrate.(3)Ru homogeneously catalyzes the reductive amination of ketones,explores the optimal reaction conditions for template reactions and expands the substrate.(4)Mechanism research,through experimental verification to determine the progress of the reaction,and design mechanism experiments to analyze the changes in the catalyst structure during the reaction.