【摘要】 用量子化学从头计算方法 ,在HF/ 6 31++G 水平研究了臭氧与CH自由基反应的微观机理 ,优化得到反应途径上的反应物、过渡态、中间体和产物的构型 ,通过振动分析对过渡态和中间体进行了确认 .用MP4 / 6 31++G / /HF/ 6 31++G 方法计算能量 ,同时进行零点能校正 .研究结果表明 :CH与O3反应首先生成环状中间体HCO3,且该步反应表现为亲电反应特征 ,然后中间体裂解生成HCO和O2 ,该反应为强放热反应 .更多还原

【Abstract】 The mechanism of the reaction CH+O 3→HCO+O 2 has been studied by using ab initio MO method. The geometries of reactants, transition state, intermediate and products have been optimized with HF/6 31++G ** basis set, which were verified by frequency analysis. The single point calculation of the species have been performed by Mфller Plesset Perturbation theory up to 4th order. The zero point energies are also corrected, the results show that the reaction molecules combine with each other firstly to form an cyclic intermediate(HCO 3), furthermore, the intermediate property is eletrophilic addition.Followed by decomposition of the intermediate to give HCO and O 2,the reaction is strong exothermic reaction.更多还原