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采用密度泛函UB3LYP/6-311+G(2d)方法研究了Fe+在基态和激发态与CO与N2O反应的反应机理.全参数优化了反应势能面上各驻点的几何构型,用频率分析方法和内禀反应坐标(IRC)方法对过渡态进行了验证,并用UB3LYP/6-311++G(3df,3pd)、单点垂直激发等方法分别进行各驻点单点能校正,四重态和六重态反应势能面交叉点CP确定,计算结果表明,该反应为两步反应,且反应机理都为插入—消去反应,势能面上的两个交叉点能够有效降低反应的活化能,这在动力学和热力学上都是有利的.
The reaction mechanism of reaction between Fe + at ground state and excited state with CO and N2O was investigated by using density functional theory UB3LYP / 6-311 + G (2d). The geometrical configurations of each stationary point on the potential surface were optimized by all parameters, The analytical method and the intrinsic reaction coordinate (IRC) method were used to verify the transition states. The single point energy of each stationary point was corrected by UB3LYP / 6-311 ++ G (3df, 3pd) The results show that the reaction is a two-step reaction, and the reaction mechanism is insertion-elimination reaction. The two crossing points on the potential energy surface can effectively reduce the activation energy of the reaction , Which is both kinetically and thermodynamically favorable.