中文版 | English
Title

Dynamic simulation on surface hydration and dehydration of monoclinic zirconia

Author
Corresponding AuthorWang,Yang Gang
Publication Years
2022-08-01
DOI
Source Title
ISSN
1674-0068
EISSN
2327-2244
Volume35Issue:4Pages:629-638
Abstract

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.

Keywords
URL[Source Record]
Indexed By
Language
English
SUSTech Authorship
First ; Corresponding
Funding Project
National Natural Science Foundation of China of China[
WOS Research Area
Physics
WOS Subject
Physics, Atomic, Molecular & Chemical
WOS Accession No
WOS:000898634400006
Publisher
Scopus EID
2-s2.0-85138257213
Data Source
Scopus
Citation statistics
Cited Times [WOS]:3
Document TypeJournal Article
Identifierhttp://kc.sustech.edu.cn/handle/2SGJ60CL/402733
DepartmentDepartment of Chemistry
Affiliation
Department of Chemistry,Guangdong Provincial Key Laboratory of Catalysis,Southern University of Science and Technology,Shenzhen,518055,China
First Author AffilicationDepartment of Chemistry
Corresponding Author AffilicationDepartment of Chemistry
First Author's First AffilicationDepartment of Chemistry
Recommended Citation
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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