论文部分内容阅读
运用密度泛函理论(DFT)中的B3LYP方法,U原子用含相对论有效原子实势(ECP)校正的基组(SDD),C、O原子采用6-311+G(d)基组,对气相中U+和CO2的反应进行了理论研究.通过研究二重和四重自旋态的反应势能面(PESs),优化得到了两条反应路径的反应物、中间体、过渡态和产物的结构.用“两态反应”(TSR)分析反应机理,结果表明体系的优先选择路径为高自旋态进入和低自旋态离开反应,发生在四重态和二重态的自旋多重度的改变使得整个反应系统能以一个低能反应途径进行.
By using the B3LYP method in density functional theory (DFT), the basic group (SDD) of the U atom with the relativistic effective atom real potential (ECP) and the 6-311 + G (d) The reaction between U + and CO2 in the gas phase has been studied theoretically.By studying the potential energy surfaces (PESs) of the double and quadruple spin states, the structures of the reactants, intermediates, transition states and products of the two reaction paths are optimized The reaction mechanism was analyzed by the “two - state reaction” (TSR). The results show that the preferred routes of the system are the high spin states entering and the low spin states leaving the reaction, the spin multiplicity occurring in the quadruple states and the double states Changes make the entire reaction system to a low-energy reaction path.