Kinetics and dynamics of the NH3 + H -> NH2 + H-2 reaction using transition state methods, quasi-classical trajectories, and quantum-mechanical scattering

CORC > 武汉物理与数学研究所 > 中国科学院武汉物理与数学研究所 > 2011年以前论文发表（包括2011年）

	Kinetics and dynamics of the NH3 + H -> NH2 + H-2 reaction using transition state methods, quasi-classical trajectories, and quantum-mechanical scattering
	Corchado, Jose C.1; Espinosa-Garcia, Joaquin 1; Yang, Minghui 2
刊名	JOURNAL OF CHEMICAL PHYSICS
	2011-07-07
卷号	135 期号:1
英文摘要	On a recent analytical potential energy surface developed by two of the authors, an exhaustive kinetics study, using variational transition state theory with multidimensional tunneling effect, and dynamics study, using both quasi-classical trajectory and full-dimensional quantum scattering methods, was carried out to understand the reactivity of the NH3 + H -> NH2 + H-2 gas-phase reaction. Initial state-selected time-dependent wave packet calculations using a full-dimensional model were performed, where the total reaction probabilities were calculated for the initial ground vibrational state and for four excited vibrational states of ammonia. Thermal rate constants were calculated for the temperature range 200-2000 K using the three methods and compared with available experimental data. We found that (a) the total reaction probabilities are very small, (b) the symmetric and asymmetric N-H stretch excitations enhance the reactivity, (c) the quantum-mechanical calculated thermal rate constants are about one order of magnitude smaller than the transition state theory results, which reproduce the experimental evidence, and (d) quasi-classical trajectory calculations, which were performed with the main goal of analyzing the influence of the zero-point energy problem on the final dynamics results, reproduce the quantum scattering calculations on the same surface. (C) 2011 American Institute of Physics. [doi: 10.1063/1.3605242]
WOS标题词	Science & Technology ; Physical Sciences
类目[WOS]	Physics, Atomic, Molecular & Chemical
研究领域[WOS]	Physics
关键词[WOS]	POTENTIAL-ENERGY SURFACE ; TRANSITION-STATE THEORY ; ZERO-POINT-ENERGY ; CLASSICAL TRAJECTORY CALCULATIONS ; ABSTRACTION REACTION ; CONSTANTS
收录类别	SCI
语种	英语
WOS记录号	WOS:000292524200017
公开日期	2015-12-01
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/8206]
专题	武汉物理与数学研究所_2011年以前论文发表（包括2011年）
作者单位	1.Univ Extremadura, Dept Quim Fis, E-06071 Badajoz, Spain 2.Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Peoples R China
推荐引用方式 GB/T 7714	Corchado, Jose C.,Espinosa-Garcia, Joaquin,Yang, Minghui. Kinetics and dynamics of the NH3 + H -> NH2 + H-2 reaction using transition state methods, quasi-classical trajectories, and quantum-mechanical scattering[J]. JOURNAL OF CHEMICAL PHYSICS,2011,135(1).
APA	Corchado, Jose C.,Espinosa-Garcia, Joaquin,&Yang, Minghui.(2011).Kinetics and dynamics of the NH3 + H -> NH2 + H-2 reaction using transition state methods, quasi-classical trajectories, and quantum-mechanical scattering.JOURNAL OF CHEMICAL PHYSICS,135(1).
MLA	Corchado, Jose C.,et al."Kinetics and dynamics of the NH3 + H -> NH2 + H-2 reaction using transition state methods, quasi-classical trajectories, and quantum-mechanical scattering".JOURNAL OF CHEMICAL PHYSICS 135.1(2011).