Theoretical study of the F(2P) + NH3 -> HF + NH2 reaction on an accurate potential energy surface: dynamics and kinetics

doi:10.1039/c9cp02113b

	Theoretical study of the F(2P) + NH3 -> HF + NH2 reaction on an accurate potential energy surface: dynamics and kinetics
	Tian, Li 1,2; Zhu, Yongfa 2,3; Song, Hongwei 2; Yang, Minghui 2
刊名	PHYSICAL CHEMISTRY CHEMICAL PHYSICS
	2019-06-07
卷号	21 期号:21 页码:11385-11394
ISSN号	1463-9076
DOI	10.1039/c9cp02113b
英文摘要	The highly exothermic hydrogen abstraction reaction of the F atom with NH3 is investigated using the quasi-classical trajectory method on a newly developed potential energy surface (PES) for the ground electronic state. The full-dimensional PES is constructed by fitting 41 282 ab initio energy points at the level of UCCSD(T)-F12/ aug-cc-pVTZ. The flexible fundamental invariant-neural network method is applied in the fitting, resulting in a total root mean square error of 0.13 kcal mol 1. On one hand, the calculated differential cross sections agree reasonably well with the experimental results and indicate that the reaction is dominated by the direct abstraction and stripping mechanisms while a considerable amount of reaction takes place by the indirect `` yo-yo'' mechanism. The product energy partition also reproduces well the experimental result, which can be understood according to the geometry change along the minimum energy path. On the other hand, the obtained vibrational state distribution of the product HF follows PnHF= 2 E PnHF= 1 4 PnHF= 0 4 PnHF= 3, less consistent with the scattered experimental results. In addition, the calculated thermal rate coefficients have practically no temperature dependence within the statistical errors.
资助项目	National Natural Science Foundation of China[21603266] ; National Natural Science Foundation of China[21773297]
WOS关键词	VIBRATIONAL-ENERGY DISPOSAL ; F-ATOMS ; RATE-CONSTANT ; FLUORINE-ATOMS ; DYNAMICS ; F+NH3 ; KINETICS ; SURFACE ; NETWORKS ; NH3
WOS研究方向	Chemistry ; Physics
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000471025900053
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/14466]
专题	中国科学院武汉物理与数学研究所
通讯作者	Song, Hongwei
作者单位	1.Huazhong Normal Univ, Coll Phys Sci & Technol, Wuhan 430079, Hubei, Peoples R China 2.Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Hubei, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Tian, Li,Zhu, Yongfa,Song, Hongwei,et al. Theoretical study of the F(2P) + NH3 -> HF + NH2 reaction on an accurate potential energy surface: dynamics and kinetics[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2019,21(21):11385-11394.
APA	Tian, Li,Zhu, Yongfa,Song, Hongwei,&Yang, Minghui.(2019).Theoretical study of the F(2P) + NH3 -> HF + NH2 reaction on an accurate potential energy surface: dynamics and kinetics.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,21(21),11385-11394.
MLA	Tian, Li,et al."Theoretical study of the F(2P) + NH3 -> HF + NH2 reaction on an accurate potential energy surface: dynamics and kinetics".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 21.21(2019):11385-11394.