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采用密度泛函理论(DFT)中的B3LYP方法研究了二重态和四重态Pt+与甲烷反应的机理.通过几何构型优化和频率计算,分别获得三个过渡态,并利用内禀反应坐标(IRC)计算进行了验证.在更高的基组水平上计算了单点能,并详细讨论了二重态和四重态的势能面.结果表明在二重态势能面上的反应具有比较低的能垒,是一个放热反应,所以该反应更易于在二重态上进行.氧化加成生成中间体HPt(CH3)+的步骤需要克服一个小小的能垒.
The B3LYP method in density functional theory (DFT) was used to study the mechanism of the reaction between the doublet and the quadruplet Pt + with methane. Three geometry transitions were obtained by geometric configuration optimization and frequency calculation respectively. The intrinsic reaction coordinate (IRC) calculations. The single point energy is calculated at a higher basis set level and the potential energy planes of the double and quadruple states are discussed in detail. The results show that the response on the dipole state potential surface is relatively low The energy barrier, which is an exothermic reaction, makes the reaction easier to proceed in the doubly-charged state. The oxidative addition step to produce the intermediate HPt (CH3) + requires overcoming a small energy barrier.