掺杂钇氧簇Y_2AlO_n~(-/0)(n=0-3)的密度泛函理论研究
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- 英文论文题名：Y_2AlO_n~(-/0)(n = 0-3) Clusters:A DFT Study
- 论文作者：陈仕芳 ; 徐若男 ; 徐磊 ; 章永凡 ; 黄昕
- 英文论文作者：Shi-Fang Chen ; Ruo-Nan Xu ; Lei Xu ; Yong-Fan Zhang ; Xin Huang ; Department of Chemistry ; University of Fuzhou
- 年：2016
- 作者机构：福州大学化学学院;
- 论文关键词：掺杂钇氧簇 ; 密度泛函理论 ; 化学键 ; 垂直电子逸出能
- 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-第十八分会：电子结构理论方法的发展与应用
- 语种：中文
- 分类号：O641.1
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第十八分会 ; 电子结构理论方法的发展与应用
- 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：228k
- 原文格式：D
- 会议级别：全国
摘要
掺杂钇氧簇在催化方面有着重要应用,钇的氧化物掺杂Al等可用做良好的催化剂或催化剂载体~([1-2])。例如,掺杂钇氧簇在一氧化碳等小分子体系表现出良好的催化活性~([1])。本文通过密度泛函理论计算,对Y_2AlO_n~(-/0)(n=0-3)团簇的几何和电子结构展开了研究。结果表明,Y_2Al~-阴离子簇的基态为C_(2v)对称性的等腰三角形结构。随着氧原子数目的增加,Y_2AlO~-阴离子簇的基态结构是在Y_2Al~-阴离子的两个钇原子间增加一个桥氧。Y_2AlO_2~-阴离子簇的基态结构是以Y_2AlO~-基态结构为基础增加一个帽氧形成的。Y_2AlO_3~-阴离子簇的基态C_S(~1A')(Fig.1a)是在Y_2AlO_2~-基态构型的Y原子与Al原子间增加一个桥氧原子,同时另一端的Y-Al键断裂形成的结构。从原子连接的方面来说,Y_2AlO_3中性簇的基态(C_S ~2A')(Fig.1b)是类似于阴离子簇的基态,此外中性Y_2AlO_n(n=0-2)的基态结构也具有类似情况。通过广义库普曼斯定理的计算,得到了Y_2AlO_3~-的第一点垂直电子逸出能(Fig.1c)为1.29 eV。此外分子轨道分析将用来解释这些钇氧簇的化学键和结构演变。
In the current work, the structural and electronic properties of Y_2AlO_n~(-/0)(n = 0-3) clusters are investigated using density functional theory calculations.The ground state of Y_2AlO_3~-(Fig.1a) is a singlet C_s(~1A') structure, which can be viewed as adding a bridging O atom between Al atom and Y atom, and broking the bond of Al atom and the other Y atom on the basic of Y_2AlO_2~-.For the neutral moiety, the ground state of Y_2AlO_3(C_s ~2A')(Fig.1b) is similar to the anion in term of atomic connectivity.The first vertical detachment energy of Y_2AlO_3~-(Fig.1c) is calculated to be 1.29 eV using the generalized Koopmans' theorem.Molecular orbital analyses are performed to elucidate the chemical bonding and structural evolution in these oxide clusters.
In the current work, the structural and electronic properties of Y_2AlO_n~(-/0)(n = 0-3) clusters are investigated using density functional theory calculations.The ground state of Y_2AlO_3~-(Fig.1a) is a singlet C_s(~1A') structure, which can be viewed as adding a bridging O atom between Al atom and Y atom, and broking the bond of Al atom and the other Y atom on the basic of Y_2AlO_2~-.For the neutral moiety, the ground state of Y_2AlO_3(C_s ~2A')(Fig.1b) is similar to the anion in term of atomic connectivity.The first vertical detachment energy of Y_2AlO_3~-(Fig.1c) is calculated to be 1.29 eV using the generalized Koopmans' theorem.Molecular orbital analyses are performed to elucidate the chemical bonding and structural evolution in these oxide clusters.
引文
[1]Ma,J.B.;Wang,Z.C.;Schlangen,M.,et al.Angew.Chem.Int.Ed.2013,52(4):1226-1230.
[2]Ma,J.B.;Wang,Z.C.;Schlangen,M.,et al.Angew.Chem.Int.Ed.2012,51(24):5991-5994.
[2]Ma,J.B.;Wang,Z.C.;Schlangen,M.,et al.Angew.Chem.Int.Ed.2012,51(24):5991-5994.