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用密度泛函理论DFT-UB3LYP方法,对2Sr+,2Ba+采用相对论校正赝势基组SDD,对C,N,O采用6-311+G(2d)基组,计算研究了气相中碱土金属离子2Sr+,2Ba+催化N2O(X1∑+)+CO(X1∑+)→N2(X1∑+g)+CO2(X1∑+g)反应的微观机理.优化了二重态势能面上各反应物、中间体和过渡态的构型特征,并用频率分析方法和内禀反应坐标方法(IRC)对过渡态进行了验证.2Sr+和2Ba+转化N2O,CO为N2,CO2的循环催化反应的计算所得结论与实验结果相同,两者的反应路径相似,两步进行的主反应都各包括两个反应通道.并通过分析NBO电荷分布对各反应复合物形成时电荷的变化作了相应讨论.
Using density functional theory (DFT-UB3LYP) method, the relativistic pseudopotential group SDD was adopted for 2Sr + and 2Ba +, and the group 6-311 + G (2d) was used for C, N and O calculations. , 2Ba + catalyzed the reaction mechanism of N2O (X1Σ +) + CO (X1Σ +) → N2 (X1Σ + g) + CO2 (X1Σ + And the transition state, and the transition state was verified by frequency analysis method and intrinsic reaction coordinate method (IRC). The conclusion and experimental results of the cyclic catalytic reaction of 2Sr + and 2Ba + conversion of N 2 O and CO into N 2 and CO 2 were obtained. Similarly, the two reaction paths are similar, and the main reactions in two steps each include two reaction channels, and the charge changes during the formation of each reaction complex are discussed by analyzing the NBO charge distribution.