B (C₆F₅) ₃ And Ru (acac)₃/triphos Complexes Catalyze The Alkane Of Amine Study On The Mechanism Of The Basic Reaction

At present,the rapid development of quantum chemistry has become an important method to study the mechanism of chemical reaction and to explore the internal microcosmic process.The main content of this paper is to study the N-alkylation of amine mechanism catalyzed by the complex of nonmetal borane B(C6F5)3 and transition metal Ru(acac)3/triphos complexes applying quantum chemical calculation method.The specific contents are as follows:The first chapter introduces the mechanism of alkylation of amines catalyzed by non-metallic catalysts and transition metal catalysts.The second chapter introduces the calculation method of quantum chemistry.The third chapter discusses the mechanism of nonmetal Lewis acid B(C6F5)3-catalyzed N-alkylation of amines using hydrosilanes.Under the calculation of quantum chemistry theory research software Gaussian 09,we optimize the important molecular structure in the reaction path,find the optimal transition state,and compare the various potential energy surfaces of imine generation and reduction.The results show that the alkylation reaction path of benzaldehyde and aniline contains two parts:(1)Aldehyde-Amine Condensation,the optimal pathway is aldehyde-amine condensation with assistant of H2O-B(C6F5)3,the rate-determining step barrier of 21.1 kcal/mol.(2)Imine reduction reaction,B(C6F5)3-catalyzed hydrosilation of imine-H2O is the optimal pathway.and its critical step energy barrier is 19.4 kcal/mol.The fourth chapter mainly studies the mechanism of transition metal ruthenium Ru(?)/triphos complexs catalytic N-alkylation of amines using carboxylic compounds.Under the calculation of quantum chemistry theory research software Gaussian 09,we optimize the important molecular structure in the reaction path,find the optimal transition state,and compare the potential energy surfaces of alkylation reaction.The results show that Ru(acac)3/triphos catalyzed the path of alkylation of carboxylic acid to amine critical step energy barrier was 14.3 kcal/mol.Through calculation and research of quantum chemistry theoretic meth,we can not only get the optimal path by comparison and analysis of the energy barriers of each path,but also provide effective theoretical support for the experimental research.