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A global full-dimensional potential energy surface and quasiclassical trajectory study of the O(D-1) + CH4 multichannel reaction
Shao, Kejie; Fu, Bina1; Zhang, Dong H.
Source PublicationPHYSICAL CHEMISTRY CHEMICAL PHYSICS
2015
DOI10.1039/c5cp04278j
Volume17Issue:37Pages:24098-24107
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS Research AreaChemistry ; Physics
WOS KeywordCROSSED MOLECULAR-BEAM ; AB-INITIO ; REACTION DYNAMICS ; QUANTUM DYNAMICS ; COLLISION ENERGY ; CHLORINE ATOM ; MECHANISM ; PATHWAY ; ABSTRACTION ; REACTIVITY
AbstractWe 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.
Language英语
WOS IDWOS:000361543200046
Citation statistics
Cited Times:8[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/146554
Collection中国科学院大连化学物理研究所
Affiliation1.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
GB/T 7714
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.
APA Shao, Kejie,Fu, Bina,&Zhang, Dong H..(2015).A global full-dimensional potential energy surface and quasiclassical trajectory study of the O(D-1) + CH4 multichannel reaction.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,17(37),24098-24107.
MLA Shao, Kejie,et al."A global full-dimensional potential energy surface and quasiclassical trajectory study of the O(D-1) + CH4 multichannel reaction".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 17.37(2015):24098-24107.
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