物理化学学报 >> 2011, Vol. 27 >> Issue (05): 1095-1102.doi: 10.3866/PKU.WHXB20110440

理论与计算化学 上一篇    下一篇

氧化锆小团簇的结构和稳定性

赵高峰, 向兵, 沈学峰, 孙建敏, 白燕枝, 王渊旭   

  1. 河南大学物理与电子学院, 计算材料科学研究所, 河南 开封 475004
  • 收稿日期:2010-12-21 修回日期:2011-03-04 发布日期:2011-04-28
  • 通讯作者: 赵高峰 E-mail:zgf@henu.edu.cn
  • 基金资助:

    国家自然科学基金(10804027, 11011140321)资助项目

Structures and Stabilities of Small Zirconium Oxide Clusters

ZHAO Gao-Feng, XIANG Bing, SHEN Xue-Feng, SUN Jian-Min, BAI Yan-Zhi, WANG Yuan-Xu   

  1. Institute of Computational Materials Science, School of Physics and Electronics, Henan University, Kaifeng 475004, Henan Province, P. R. China
  • Received:2010-12-21 Revised:2011-03-04 Published:2011-04-28
  • Contact: ZHAO Gao-Feng E-mail:zgf@henu.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (10804027, 11011140321).

摘要:

利用密度泛函理论在广义梯度近似(GGA)和Perdew-Wang交换关联泛函条件下研究了小团簇ZrmOn (1≤m≤5, 1≤n≤2m)的几何结构和稳定性. 结果表明: 所有团簇的最低能量结构可通过锆团簇的连续氧化获得, 一般情况下O原子占据在Zr团簇的桥位. (ZrO2)3和(ZrO2)5团簇的基态结构符合配位数规则和成键规律. 此外, 讨论了氧化锆团簇的分解通道和分解能, 值得指出的是在Zr原子数相同时ZrmO2m-1团簇(除了Zr4O7)存在最大的分解能.

关键词: 密度泛函理论, 氧化锆团簇, 分解通道, 成键规律

Abstract:

The geometric structures and stabilities of small ZrmOn (1≤m≤5, 1≤n≤2m) clusters were studied using density functional theory (DFT) calculations with the Perdew-Wang exchange correlation functional and the generalized gradient approximation (GGA). The lowest energy structures of all these clusters were obtained by the sequential oxidation of the small “core” zirconium clusters. In general, the O atoms prefer the bridge sites along the Zrm skeleton. The ground-state structures of the (ZrO2)3 and (ZrO2)5 clusters are consistent with coordination number rules and bonding regularity. The fragmentation channels and fragmentation energies of the small zirconium oxide clusters were discussed. We found that the ZrmO2m-1 clusters (not including Zr4O7) had the largest fragmentation energy among the clusters with the same number of zirconium atoms.

Key words: Density functional theory, Zirconium oxide cluster, Fragmentation channel, Bonding regularity

MSC2000: 

  • O641