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Quasiclassical Trajectory Study of the Reaction of CD4 with O(1D)
Ke-jie Shao,Bi-na Fu*,Dong H. Zhang*
Author NameAffiliationE-mail
Ke-jie Shao State Key Laboratory of Molecular Reaction Dynamics and Center for Theoretical and Computational Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China  
Bi-na Fu* State Key Laboratory of Molecular Reaction Dynamics and Center for Theoretical and Computational Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China bina@dicp.ac.cn 
Dong H. Zhang* State Key Laboratory of Molecular Reaction Dynamics and Center for Theoretical and Computational Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China zhangdh@dicp.ac.cn 
Abstract:
Extensive quasiclassical trajectory calculations for the O(1D)+CD4 multichannel reaction were carried out on a new global potential energy surface fit by permutationally invariant polynomials. The product branching ratios, translational energy distributions, and angular distributions of OD+CD3, D+CD2OD/CD3O, and D2+DCOD/D2CO product channels were calculated and compared with the available experimental results. Good agreement between theory and experiment has been achieved, indicating small isotope effects for the title reaction. The O(1D)+CD4 reaction mainly proceeds through the CD3OD intermediate via the trapped abstraction mechanism, with initial abstraction of the D atom rather than the direct insertion, followed by decomposition of CD3OD into various products.
Key words:  Multichannel reaction, Reaction dynamics, Quasiclassical trajectory, Potential energy surface
FundProject:
O(1D)和CD4反应的准经典轨线
邵科杰,傅碧娜*,张东辉*
摘要:
在新的全域势能面上, 用准经典轨线方法细致地研究了O(1D)+CD4多通道化学反应的动力学.这个势能面是用交换不变多项式方法基于MRC+Q/aug-cc-pVTZ从头算点拟合得到的.通过计算得到了产物OD+CD3、D+CD2OD/CD3O和D2+DCOD/D2CO的分支比、平动能分布以及角度分布,结果显示理论与实验吻合得较好, 从而说明了这个反应的同位素取代效应很小. 研究表明,O(1D)+CD4反应是经过陷入的抽取机理发生的: 最初主要通过D原子的抽取,并不是之前人们认为的直接C-D键的插入形成CD3OD中间物后再进而解离成各个产物通道.
关键词:  多通道反应,反应动力学,准经典轨线,势能面
DOI:10.1063/1674-0068/28/cjcp1507152
分类号: