乙酸在氧化铈不同模型表面吸附行为的差异性研究
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- 英文论文题名：Acetic acid adsorption on CeO_2 surface
- 论文作者：王渭娜 ; Ping Yang ; 王文亮
- 英文论文作者：Weina Wang ; Ping Yang ; Wenliang Wang ; School of Chemistry & Chemical Engineering ; Shaanxi Normal University ; Theoretical Division ; Los Alamos National Laboratory
- 年：2016
- 作者机构：陕西师范大学化学化工学院;Theoretical Division,Los Alamos National Laboratory;
- 论文关键词：氧化铈 ; slab模型 ; 团簇模型 ; 吸附
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第十五分会：表界面结构调控与催化
- 语种：中文
- 分类号：O647.3
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第十五分会 ; 表界面结构调控与催化
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：186k
- 原文格式：D
- 会议级别：全国
摘要
实验方面研究小分子在纳米氧化铈表面的吸附行为时,得到结果存在差异性。Stubenrauch等人[1]认为有机羧酸在氧化铈表面以脱质子化方式吸附在表面,有机羧酸根离子与表面通过monodentate模式键合。然而,已有的其他研究结果认为bridging bidentate模式比monodentate模式稳定[2-3]。因此本工作采用CeO_2(111)表面的slab模型和Ce19O32的团簇模型模拟纳米氧化铈表面,系统研究了乙酸在纳米氧化铈表面的吸附。研究结果表明:无论规整CeO_2(111)表面、氧缺陷CeO_(2-x)(111)表面还是Ce19O32团簇,乙酸分子均可按解离态吸附或分子态吸附方式存在于氧化铈表面上,其中解离态吸附方式更具有稳定性;乙酸分子与氧化铈表面存在多种结合方式,即monodentate,bidentate和chelating bidentate,在CeO_(2-x)(111)表面上最稳定的键合方式bridging bidentate模式;而对Ce19O32团簇,chelating bidentate模式则是乙酸分子在其表面吸附的最稳定方式。
Acetic acid adsorption on CeO_2(111) and Ce_(19)O_(32) nanoparticle surface was investigated using DFT+U.Both molecular state and dissociative state were identified on these surfaces via monodentate,bidentate and chelating bidentate.Regardless of the surface structure,acetic acid dissociates on the surface is more stable than molecular adsorbs,whereas the binding modes are different from each other.For CeO_(2-x)(111) surface,the most stable configuration is acetate binding to surface via bridging bidentate mode;whereas for Ce19O32 nanoparticle surface,the most stable configuration is acetate binding to surface via chelating bidentate mode.
Acetic acid adsorption on CeO_2(111) and Ce_(19)O_(32) nanoparticle surface was investigated using DFT+U.Both molecular state and dissociative state were identified on these surfaces via monodentate,bidentate and chelating bidentate.Regardless of the surface structure,acetic acid dissociates on the surface is more stable than molecular adsorbs,whereas the binding modes are different from each other.For CeO_(2-x)(111) surface,the most stable configuration is acetate binding to surface via bridging bidentate mode;whereas for Ce19O32 nanoparticle surface,the most stable configuration is acetate binding to surface via chelating bidentate mode.
引文
[1]Stubenrauch,J.;Brosha,E.;Vohs J.M.Catal.Today.1996,28(4):431.
[2]Senanayake,S.D.;Mullins,D.R.J.Phys.Chem.C.2008,112(26):9744.
[3]Gordon,W.O.;Xu,Y.;Mullins,D.R.Phys.Chem.Chem.Phys.2009,11(47):11171.
[2]Senanayake,S.D.;Mullins,D.R.J.Phys.Chem.C.2008,112(26):9744.
[3]Gordon,W.O.;Xu,Y.;Mullins,D.R.Phys.Chem.Chem.Phys.2009,11(47):11171.