Fe(O)OH!活化甲烷反应的理论研究

摘要

采用密度泛函理论研究了气相中[Fe（O）OH]！与甲烷的反应机理。用 B3LYP 方法优化了势能面上各反应路径的过渡态和中间体等各驻点的结构，并通过振动分析和内禀反应坐标法对过渡态和中间体进行了确认，计算提出了两条可能的反应路线，揭示了[Fe（O）OH]！与甲烷的反应机理，同时对反应中存在的势能面交叉现象进行了研究，确定了最低势能交叉点处的作用机制。%The detail mechanisms of activation of methane catalyzed by [Fe(O)OH]" were studied with the density functional theory(DFT).The structures of the transition states and intermediates along the reaction pathways were optimized by B3LYP method.The transition states and intermediates were confirmed by vibra-tion analysis and intrinsic reaction coordinates(IRC)method.The computational results gave two possible reac-tion pathways and revealed the detail mechanism according to the results of the experiments.The phenomenon of cross-reaction potential energy surfaces were studied and the mechanism at the minimum cross-reaction po-tential energy point was determined.