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题名: A global full-dimensional potential energy surface and quasiclassical trajectory study of the O(D-1) + CH4 multichannel reaction
作者: Shao, Kejie;  Fu, Bina1;  Zhang, Dong H.
刊名: PHYSICAL CHEMISTRY CHEMICAL PHYSICS
发表日期: 2015
DOI: 10.1039/c5cp04278j
卷: 17, 期:37, 页:24098-24107
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical ;  Physics, Atomic, Molecular & Chemical
研究领域[WOS]: Chemistry ;  Physics
英文摘要: We report a new global, full-dimensional ground-state potential energy surface (PES) of the O(D-1) + CH4 multichannel reaction, based on high-level ab initio calculations and fitting procedures. The PES is a permutationally invariant fit to roughly 340 000 electronic energies calculated by the MRCI + Q/aug-cc-pVTZ level of theory. Extensive quasiclassical trajectory calculations were carried out on the new PES at the collision energy of relevance to the previously universal crossed molecular beam experiments. The product branching ratios, translational energy distributions and angular distributions of OH + CH3, H + CH2OH/CH3O and H-2 + HCOH/H2CO product channels were calculated and compared with the available experimental results. Very good agreement between theory and experiment has been achieved. The O(D-1) + CH4 reaction mainly proceeds through the CH3OH intermediate via a trapped abstraction mechanism, starting with the abstraction of the hydrogen atom, rather than the direct insertion pathway with the O(D-1) atom directly inserting into the C-H bond of CH4. The process with a very short lifetime behaves like an abstraction reaction, producing a pronounced forward scattering peak as found in the OH + CH3 channel, while the process with a relatively long lifetime produces reaction products with nearly forward and backward scattering symmetry, similar to an insertion reaction, as found in other reaction channels.
关键词[WOS]: CROSSED MOLECULAR-BEAM ;  AB-INITIO ;  REACTION DYNAMICS ;  QUANTUM DYNAMICS ;  COLLISION ENERGY ;  CHLORINE ATOM ;  MECHANISM ;  PATHWAY ;  ABSTRACTION ;  REACTIVITY
语种: 英语
WOS记录号: WOS:000361543200046
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/146554
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, Ctr Theoret & Computat Chem, Dalian 116023, Peoples R China

Recommended Citation:
Shao, Kejie,Fu, Bina,Zhang, Dong H.. A global full-dimensional potential energy surface and quasiclassical trajectory study of the O(D-1) + CH4 multichannel reaction[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2015,17(37):24098-24107.
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