燃烧基元反应动力学研究-氧原子与系列烯烃的反应

In hydrocarbon flames, small unsaturated hydrocarbons are crucial intermediates which mainly react with triplet ground-state oxygen atoms. It is important to consider nonadiabatic effects for these systems involved in combustion chemistry. For the reaction of O(3P) with a series of alkenes, the nonadiabatic product channels and mechanisms will be investigated both theoretically and experimentally. Theoretically, ab initio calculations are performed for both the triplet and singlet potential energy surfaces and the minimum energy crossing point between the two surfaces will be located with the Newton-Lagrange method. Experimentally, the step-scan time-resolved FTIR emission spectroscopy will be used to determine the reaction products, the rate constant and vibrational energy disposal. The nonadiabatic mechanisms and other fundamental questions such as the internal H-atom migrations are to be explored.

烯烃作为烃类燃烧中重要的中间体与氧原子等发生快速反应。对这些燃烧中重要的基元反应，非绝热效应不容忽视。本项目拟选取一系列典型烯烃和氧原子的基元反应体系，理论上，基于Newton-Lagrange方法，通过量子化学计算，确定势能面交叉点和反应途径；实验上，采用步进扫描时间分辨傅立叶变换红外发射光谱（TR-FTIR）技术，探测多种基元反应产物，测量反应速率常数，确定产物振动激发态能量分布。理论和实验研究结合，阐明振动激发和传能机制，构建燃烧过程中重要基元反应的非绝热微观机理。

烯烃作为烃类燃烧中重要的中间体与氧原子等发生快速反应。对这些燃烧中重要的基元反应，非绝热效应不容忽视。本项目研究了一系列典型烯烃和氧原子的基元反应体系，理论上，基于Newton-Lagrange方法，通过量子化学计算，确定了势能面交叉点和反应途径；实验上，采用步进扫描时间分辨傅立叶变换红外发射光谱（TR-FTIR）技术，探测到了多种基元反应产物，测量了反应速率常数，确定了产物通道分支比。理论和实验研究结合，阐明了振动激发和传能机制，构建了燃烧过程中重要基元反应的非绝热微观机理。