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题名

Dynamic simulation on surface hydration and dehydration of monoclinic zirconia

作者
通讯作者Wang,Yang Gang
发表日期
2022-08-01
DOI
发表期刊
ISSN
1674-0068
EISSN
2327-2244
卷号35期号:4页码:629-638
摘要

The commonly used oxide-supported metal catalysts are usually prepared in aqueous phase, which then often need to undergo calcination before usage. Therefore, the surface hydration and dehydration of oxide supports are critical for the realistic modeling of supported metal catalysts. In this work, by ab initio molecular dynamics (AIMD) simulations, the initial anhydrous monoclinic ZrO2(1¯11) surfaces are evaluated within explicit solvents in aqueous phase at mild temperatures. During the simulations, all the two-fold-coordinated O sites will soon be protonated to form the acidic hydroxyls (HOL), remaining the basic hydroxyls (HO*) on Zr. The basic hydroxyls (HO*) can easily diffuse on surfaces via the active proton exchange with the undissociated adsorption water (H2O*). Within the temperatures ranging from 273 K to 373 K, in aqueous phase a certain representative equilibrium hydrated m-ZrO2(1¯11) surface is obtained with the coverage (θ) of 0.75 on surface Zr atoms. Later, free energies on the stepwise surface water desorption are calculated by density functional theory to mimic the surface dehydration under the mild calcination temperatures lower than 800 K. By obtaining the phase diagrams of surface dehydration, the representative partially hydrated m-ZrO2(1¯11) surfaces (0.25≤θ<0.75) at various calcination temperatures are illustrated. These hydrated m-ZrO2(1¯11) surfaces can be crucial and readily applied for more realistic modeling of ZrO2 catalysts and ZrO2-supported metal catalysts.

关键词
相关链接[Scopus记录]
收录类别
语种
英语
学校署名
第一 ; 通讯
资助项目
National Natural Science Foundation of China of China[
WOS研究方向
Physics
WOS类目
Physics, Atomic, Molecular & Chemical
WOS记录号
WOS:000898634400006
出版者
Scopus记录号
2-s2.0-85138257213
来源库
Scopus
引用统计
被引频次[WOS]:6
成果类型期刊论文
条目标识符http://sustech.caswiz.com/handle/2SGJ60CL/402733
专题理学院_化学系
作者单位
Department of Chemistry,Guangdong Provincial Key Laboratory of Catalysis,Southern University of Science and Technology,Shenzhen,518055,China
第一作者单位化学系
通讯作者单位化学系
第一作者的第一单位化学系
推荐引用方式
GB/T 7714
Xia,Guang Jie,Wang,Yang Gang. Dynamic simulation on surface hydration and dehydration of monoclinic zirconia[J]. 化学物理学报,2022,35(4):629-638.
APA
Xia,Guang Jie,&Wang,Yang Gang.(2022).Dynamic simulation on surface hydration and dehydration of monoclinic zirconia.化学物理学报,35(4),629-638.
MLA
Xia,Guang Jie,et al."Dynamic simulation on surface hydration and dehydration of monoclinic zirconia".化学物理学报 35.4(2022):629-638.
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