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
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DOI | |
发表期刊 | |
ISSN | 1674-0068
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EISSN | 2327-2244
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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
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学校署名 | 第一
; 通讯
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资助项目 | National Natural Science Foundation of China of China[
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WOS研究方向 | Physics
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WOS类目 | Physics, Atomic, Molecular & Chemical
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WOS记录号 | WOS:000898634400006
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出版者 | |
Scopus记录号 | 2-s2.0-85138257213
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来源库 | Scopus
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引用统计 |
被引频次[WOS]:6
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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.
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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.
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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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条目包含的文件 | 条目无相关文件。 |
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