钴络合物催化甲醇羰基化制甲酸甲酯反应的理论研究

本文运用密度泛函理论B3LYP方法,对C、O、H采用6-311+G(2d,p)基组,计算研究了钴络合物催化甲醇羰基化制甲酸甲酯反应的微观机理,优化了各反应物、中间体和过渡态的构型特征,用频率分析方法和内禀反应坐标方法对过渡态进行了验证,同时对各中间体进行电荷分析.对比了催化过程与非催化过程的能垒.结果表明,有催化剂参与后反应活化能明显降低.

Kinetic study for the reaction of carbonylation of methanol to methyl formate catalyzed by Co(II)-complex

The carbonylation of methanol to methyl formate catalyzed by Co(II)-complex has been investigated by using the B3LYP level of density functional theory, the 6-311+G(2d,p) basis set for C, H and O. The geometries for the reactants, the transition states and the products are completely optimized. All the transition states are verified by the vibrational analysis and the internal reaction coordinatecalculations. At the same time, charge analysis of the reactants and the products. The energy barrier of catalytic process and non-catalytic process is compared. The results showed that the activation energy decreased obviously after the catalyst was involved.