密度泛函理论研究Pu+O2反应机理及键的特点
Density function theoretical study on the Pu+O2 reaction mechanism

通过建立Pu与O2反应的理论模型，采用密度泛函理论(DFT)系统研究了钚原子与氧气分子的微观反应机理。优化了反应势能面上各驻点的几何结构，并用频率分析方法和内禀反应坐标(IRC)方法验证了过渡态，得到了该反应的反应势能曲线和微观反应路径。此外，用分子中的原子理论（AIM）和电子定域函数(ELF)理论方法探究了反应过程中各原子间化学键的演化特点。结果表明，这一反应体系有两条不同的反应路径，反应产物分别是PuO2和PuO+O; 能量分析表明，生成PuO2的反应更容易发生。
The theory model of the interaction between Pu atom and O2 was built and a systematic density functional theory computational study is reported here. The structures of reactants, transition states, intermediates and final products are optimized. All the transition states are verified by the vibration analysis and intrinsic reaction coordinate calculations. The nature of the bonding evolution along the reaction pathways was explored using distinct analysis method including electron localization function(ELF), atoms-in-molecules(AIM). The results indicates that the final reaction products of O-O breakage are the PuO2 and PuO+O. In addition, the reaction of Pu+O2→PuO2 is more energy supported.