CAJ | 학술논문

用密度泛函理论中B3LYP方法详细研究了Mo＋（6S,4d5,4G,4d5）与CS2的反应机理.为了得到更为准确的活化能和反应的能量,在B3LYP优化好的结构的基础上,用耦合族理论（CCSD（T））计算了各个驻点的单点能.计算结果显示,活化C-S键的反应机理为是插入-消出机理.反应Mo＋（6S）＋CS2（1Σ）→MoS＋（4Σ-）＋CS（1Σ）在反应过程中经过六重态-四重态势能面交叉,我们确定势能面交叉点（CP）.所有的计算结果都和已有的理论和实验值进行了比较.
용밀도범함이론중B3LYP방법상세연구료Mo＋（6S,4d5,4G,4d5）여CS2적반응궤리.위료득도경위준학적활화능화반응적능량,재B3LYP우화호적결구적기출상,용우합족이론（CCSD（T））계산료각개주점적단점능.계산결과현시,활화C-S건적반응궤리위시삽입-소출궤리.반응Mo＋（6S）＋CS2（1Σ）→MoS＋（4Σ-）＋CS（1Σ）재반응과정중경과륙중태-사중태세능면교차,아문학정세능면교차점（CP）.소유적계산결과도화이유적이론화실험치진행료비교.
The quartet and doublet potential energy surfaces（PESs） for reactions of Mo＋（6S,4G） with CS2 in the gas phase have been investigated in detail by means of density functional method（B3LYP） to elucidate the mechanisms of Mo＋ reacting with CS2.The coupled cluster single-point calculations（CCSD（T）） using B3LYP optimized geometries were performed to obtain more accurate results.The sextet and quartet reactions have an insertion-elimination mechanism.It is found that the reaction of the 6S gound state of Mo＋ to yield MoS＋ is spin-forbidden Mo＋（6S）＋CS2（1Σ）→MoS＋（4Σ-）＋ CS（1Σ）and the crossing points were approximately determined.All of the results have been compared with the existing experimental and theoretical data.