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用密度泛函理论(DFT)的B3LYP方法,在6-311++G(d,p)基组水平下研究了CO与OH自由基反应的微观机理.全参数优化了反应过程中各反应物、中间体、过渡态和产物的几何构型,振动分析结果证实了中间体和过渡态的真实性,IRC计算结果进一步证实了过渡态的真实性.在G3水平上计算了它们的能量,OH自由基与CO反应机理的研究结果显示:OH自由基与CO反应为双通道反应过程,分别为(1)CO+OH→IM1→TS1→CO2+H;(2)CO+OH→IM1→TS2→IM2→TS3→CO2+H.其中通道(2)的活化能较低,为主要反应通道.
The density functional theory (DFT) B3LYP method was used to study the microscopic mechanism of CO and OH radical reaction at the 6-311 ++ G (d, p) basis set. All the parameters were optimized for each reactant , Intermediates, transition states and geometries of the products. The results of vibration analysis confirm the authenticity of intermediates and transition states. The IRC results confirm the authenticity of the transition states. Their energies are calculated at G3 level. OH The results of the study on the reaction mechanism between free radicals and CO show that the reaction of OH radical and CO is a two-channel reaction process, which are (1) CO + OH → IM1 → TS1 → CO2 + H, (2) CO + OH → IM1 → TS2 → IM2 → TS3 → CO2 + H. Among them, the activation energy of channel (2) is lower, which is the main reaction channel.