摘要
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.
The carbonylation of methanol to methyl formate catalyzed by Co(Ⅱ)-complex has been investigated by using the B3 LYP level of density functional theory with the 6-311+G(2 d,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 coordinate calculations. At the same time, charge analyses of the reactants and the products are made. The energy barriers of catalytic process and non-catalytic process are compared. The results showed that the activation energy decreases obviously after the catalyst is involved.
作者
成莉燕
张建辉
燕鹏华
慕红梅
CHENG Li-Yan;ZHANG Jian-Hui;YAN Peng-Hua;MU Hong-Mei(Department ofMetallurgical Engineering,Lanzhou Resources & Environment Voc-Tech College,Lanzhou 730021,China;Lanzhou Petrochemical Research Center,Lanzhou 730060,China)
出处
《原子与分子物理学报》
CAS
北大核心
2019年第2期193-198,共6页
Journal of Atomic and Molecular Physics
基金
甘肃省自然科学基金(1606RJZA029)
兰州资源环境职业技术学院科研团队项目(T2016-15)
兰州资源环境职业技术学院科研项目(Z2016-08)
关键词
甲醇羰基化
钴络合物
甲酸甲酯
密度泛函理论
Methanol carbonylation
Co(Ⅱ)-complex
Methyl formate
Density functional theory
