Hydrogen abstraction/addition reactions in soot surface growth

doi:10.1039/d0cp06406h

CORC > 力学研究所 > 中国科学院力学研究所 > 流固耦合系统力学重点实验室(2012-)

	Hydrogen abstraction/addition reactions in soot surface growth
	Chu, Qingzhao 2,3; Shi, Baolu 2; Wang, Hongyu 3; Chen, Dongping 3; Liao LJ(廖丽涓)1
刊名	PHYSICAL CHEMISTRY CHEMICAL PHYSICS
	2021-01-28
卷号	23 期号:4 页码:3071-3086
ISSN号	1463-9076
DOI	10.1039/d0cp06406h
通讯作者	Chen, Dongping(dc516@bit.edu.cn) ; Liao, Lijuan(liaohuanxin@hotmail.com)
英文摘要	The hydrogen abstraction (HB) and addition reactions (HD) by H radicals are examined on a series of polycyclic aromatic hydrocarbon (PAH) monomers and models of quasi-surfaces using quasi-classical trajectory (QCT) method. QCT results reproduce the rate constants of HB reactions on PAH monomers from density functional theory (DFT) in the range of 1500-2700 K. The PAH size has a minor impact on the rates of HB reactions, especially at temperatures beyond 2100 K. In contrast, HD reactions have a clear size dependence, and a larger PAH yields a higher rate. It was also found that the preferred reaction pathway changes from HB to HD reactions at similar to 1900 K. The rates of surface HB and HD reactions exceed those in the gas phase by nearly one factor of magnitude. Further analysis of the detailed trajectory of the QCT method reveals that about 50% of surface reactions can be attributed to the events of surface diffusion, which depends on the local energy transfer in gas-surface interactions. However, this phenomenon is not preferred in PAH monomers, as expected. Our finding here questions the treatment of the surface reactions of soot as the product of the first collision between the gaseous species and particle surface. The surface diffusion-induced reactions should be accounted for in the rates of the surface HB and HD reactions. The rate constants of HB and HD reactions on each reactive site (surface zig-zag, surface free-edge and pocket free-edge sites) were calculated by QCT method, and are recommended for the further development of surface chemistry models in soot formation.
分类号	二类/Q1
资助项目	National Natural Science Foundation of China[21961122007] ; National Natural Science Foundation of China[51806016] ; National Natural Science Foundation of China[11672314] ; National Natural Science Foundation of China[51676016] ; Beijing Institute of Technology Research Fund Program for Young Scholars
WOS研究方向	Chemistry ; Physics
语种	英语
WOS记录号	WOS:000614634000057
资助机构	National Natural Science Foundation of China ; Beijing Institute of Technology Research Fund Program for Young Scholars
其他责任者	Chen, Dongping ; Liao, Lijuan
内容类型	期刊论文
源URL	[http://dspace.imech.ac.cn/handle/311007/86127]
专题	力学研究所_流固耦合系统力学重点实验室(2012-)
作者单位	1.Chinese Acad Sci, Inst Mech, Key Lab Mech Fluid Solid Coupling Syst, Beijing 100190, Peoples R China 2.Beijing Inst Technol, Sch Aerosp Engn, Beijing 100081, Peoples R China; 3.Beijing Inst Technol, State Key Lab Explos Sci & Technol, Beijing 100081, Peoples R China;
推荐引用方式 GB/T 7714	Chu, Qingzhao,Shi, Baolu,Wang, Hongyu,et al. Hydrogen abstraction/addition reactions in soot surface growth[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2021,23(4):3071-3086.
APA	Chu, Qingzhao,Shi, Baolu,Wang, Hongyu,Chen, Dongping,&廖丽涓.(2021).Hydrogen abstraction/addition reactions in soot surface growth.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,23(4),3071-3086.
MLA	Chu, Qingzhao,et al."Hydrogen abstraction/addition reactions in soot surface growth".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 23.4(2021):3071-3086.