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Methane dissociation on Ni(111): A seven-dimensional to nine-dimensional quantum dynamics study
Shen, Xiangjian1,2,3; Zhang, Zhaojun2,3; Zhang, Dong H.2,3
刊名JOURNAL OF CHEMICAL PHYSICS
2017-07-14
DOI10.1063/1.4991562
147期:2
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
关键词[WOS]POTENTIAL-ENERGY SURFACE ; UNIMOLECULAR RATE THEORY ; WAVE BASIS-SET ; METAL-SURFACES ; MODE SPECIFICITY ; CH4 DISSOCIATION ; LATTICE MOTION ; CHEMISORPTION ; NI(100) ; BOND
英文摘要As one benchmark system of CH4 dissociation on the Ni(111) surface, it is of great significance to explore the role of each degree of freedom (DOF) of reactant CH4 in its first C-H bond dissociation from quantum dynamics simulations. Here, the influence of the CH stretching DOF of methyl limited in C-3v symmetry is quantitatively investigated as well as the important role of azimuth. We calculated the sticking probabilities, S-0, of ground state (GS) CH4 dissociation on a rigid Ni(111) surface by performing some seven-dimensional to nine-dimensional (9D) quantum dynamics simulations based on one highly accurate and fifteen-dimensional (15D) ab initio potential energy surface which we recently developed. Our direct quantum dynamics results show that S-0 of GS CH4 on four given surface impact sites are weakly enhanced by adding the CH stretching DOF of methyl but strongly weakened by the DOF of azimuth. Furthermore, using a 9D quantum dynamics model, we improve the post-treatment model for treating the influence of surface impact sites through a linear relationship between the effective potential barriers and the distances relative to that on the transition state site. These developed high-dimensional quantum dynamics models and improved post-treatments can be usefully extended for studying some complex polyatomic gas-surface reactions by other theoretical groups. Published by AIP Publishing.
语种英语
WOS记录号WOS:000405669900023
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/152033
专题中国科学院大连化学物理研究所
作者单位1.Zhengzhou Univ, Sch Chem Engn & Energy, Res Ctr Heterogeneous Catalysis & Engn Sci, Zhengzhou 450001, Henan, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, Ctr Theoret Computat Chem, Dalian 116023, Peoples R China
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Shen, Xiangjian,Zhang, Zhaojun,Zhang, Dong H.. Methane dissociation on Ni(111): A seven-dimensional to nine-dimensional quantum dynamics study[J]. JOURNAL OF CHEMICAL PHYSICS,2017,147(2).
APA Shen, Xiangjian,Zhang, Zhaojun,&Zhang, Dong H..(2017).Methane dissociation on Ni(111): A seven-dimensional to nine-dimensional quantum dynamics study.JOURNAL OF CHEMICAL PHYSICS,147(2).
MLA Shen, Xiangjian,et al."Methane dissociation on Ni(111): A seven-dimensional to nine-dimensional quantum dynamics study".JOURNAL OF CHEMICAL PHYSICS 147.2(2017).
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