Uncover Chemical Processes for Silica Surfaces Exposed to Atomic Oxygen Using ReaxFF Reactive Molecular Dynamics

doi:10.1021/acs.jpcc.4c05596

	Uncover Chemical Processes for Silica Surfaces Exposed to Atomic Oxygen Using ReaxFF Reactive Molecular Dynamics
	Ye XB(叶鑫斌)1,2; Hu SW(胡世威)1; Zhang G(张冠)1; Yan, Yabin 3; Sun QH(孙泉华)1,2 ; Hu Y(胡远)1
通讯作者	Hu, Yuan([email protected])
发表期刊	JOURNAL OF PHYSICAL CHEMISTRY C
	2024-12-18
页码	13
ISSN	1932-7447
摘要	The considerable level of uncertainty in the measured and calculated catalytic recombination coefficients of atomic oxygen (O) on silica (SiO2) surfaces has posed a great challenge to the accurate prediction of heating load and thereby the weight-effective design for atmospheric hypersonic vehicles. This work conducts large-scale (in terms of reaction trajectories) reactive molecular dynamics simulations based on ReaxFFSiO GSI, a ReaxFF potential function tailored for O(gas)-SiO2(surface) interactions to understand the chemical processes for the recombination of O for different SiO2 surface structures. The applicability of the present ReaxFF-based molecular dynamics is validated by the density-functional-theory calculation through O adsorption on the same SiO2 surface structures under investigation. An automatic data analyzer is developed to capture the reaction pathways and mechanisms from the vast amount of trajectories. It is found that the pathways of adsorption, active site formation, and recombination are sensitive to the surface structures. The overall recombination coefficient and its compositions from different reaction pathways vary considerably for different surface structures. We identify for the first time a reaction mechanism involving multiple active sites, which is more likely to occur than the single-site reactions and thus can potentially increase the recombination probability. These findings highlight the important role of surface structure in catalytic recombination reactions and provide a possible explanation for the huge discrepancy in the recombination coefficients from previous studies.
DOI	10.1021/acs.jpcc.4c05596
收录类别	SCI ; EI
语种	英语
WOS记录号	WOS:001380423000001
关键词[WOS]	ENERGY ACCOMMODATION ; RECOMBINATION ; ADSORPTION ; OXIDATION ; DEFECTS ; SIO2 ; COEFFICIENTS ; KINETICS ; INSIGHTS ; CRYSTAL
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
WOS类目	Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
资助项目	National Natural Science Foundation of China[XDA0380602] ; Strategic Priority Research Program of the Chinese Academy of Sciences[92271117] ; National Natural Science Foundation of China ; VESTA
项目资助者	National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; VESTA
论文分区	二类
力学所作者排名	1
RpAuthor	Hu, Yuan
引用统计
文献类型	期刊论文
条目标识符	http://dspace.imech.ac.cn/handle/311007/97995
专题	高温气体动力学国家重点实验室
作者单位	1.Chinese Acad Sci, Inst Mech, Beijing 100190, Peoples R China; 2.Univ Chinese Acad Sci, Sch Engn Sci, Beijing 100049, Peoples R China; 3.East China Univ Sci & Technol, Sch Mech Power & Engn, Shanghai 200237, Peoples R China
推荐引用方式 GB/T 7714	Ye XB,Hu SW,Zhang G,et al. Uncover Chemical Processes for Silica Surfaces Exposed to Atomic Oxygen Using ReaxFF Reactive Molecular Dynamics[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2024:13.Rp_Au:Hu, Yuan
APA	叶鑫斌,胡世威,张冠,Yan, Yabin,孙泉华,&胡远.(2024).Uncover Chemical Processes for Silica Surfaces Exposed to Atomic Oxygen Using ReaxFF Reactive Molecular Dynamics.JOURNAL OF PHYSICAL CHEMISTRY C,13.
MLA	叶鑫斌,et al."Uncover Chemical Processes for Silica Surfaces Exposed to Atomic Oxygen Using ReaxFF Reactive Molecular Dynamics".JOURNAL OF PHYSICAL CHEMISTRY C (2024):13.