物理化学学报 >> 2008, Vol. 24 >> Issue (11): 1995-1999.doi: 10.3866/PKU.WHXB20081110

研究论文 上一篇    下一篇

N2分子在UO(100)表面的吸附与解离

郑金德; 陆春海; 孙宝珍; 陈文凯   

  1. 福州大学化学系, 福州 350108; 中国工程物理研究院, 四川 绵阳 621900
  • 收稿日期:2008-05-05 修回日期:2008-07-07 发布日期:2008-11-10
  • 通讯作者: 陈文凯 E-mail:qc2008@fzu.edu.cn

Adsorption and Dissociation of N2 Molecule on UO(100) Surface

ZHENG Jin-De; LU Chun-Hai; SUN Bao-Zhen; CHEN Wen-Kai   

  1. Department of Chemistry, Fuzhou University, Fuzhou 350108, P. R. China; China Academy of Engineering Physics, Mianyang 621900, Sichuan Province, P. R. China
  • Received:2008-05-05 Revised:2008-07-07 Published:2008-11-10
  • Contact: CHEN Wen-Kai E-mail:qc2008@fzu.edu.cn

摘要: 运用密度泛函理论中广义梯度近似(GGA)的VWN-BP方法结合周期性平板模型, 研究N2在UO(100)表面的吸附. 研究表明, N2平行吸附在UO(100)表面穴位为最稳定吸附构型, 吸附能为79.0 kJ·mol-1. Mulliken布居分析显示, N2获得电子. 吸附后, N—N伸缩振动频率发生红移, 波数在1770-2143 cm-1之间. 态密度分析表明, U原子将d、f电子转移至N2的2π轨道. 计算所得解离反应的能垒为266.9 kJ·mol-1.

关键词: 密度泛函理论, N2, 吸附, 解离, 一氧化铀

Abstract: The adsorption of N2 molecule on the UO(100) surface was studied with periodic slab model by VWN-BP approach of GGA within the framework of density functional theory (DFT). The results of geometry optimization indicated that the most stable structure of adsorption was N2 adsorbed parallelly on the hollow site with an adsorption energy of 79.0 kJ·mol -1. The analysis of Mulliken population and density of states indicated that 2π antibonding orbitals of N2 molecules got electrons from d and f orbitals in uranium. The vibration wave number of N—N range from 1770 to 2143 cm-1. Complete linear synchronous transit (LST) and quadratic synchronous transit (QST) were used to search the transition state for dissociation reaction. The predicted lowest energy barrier was 266.9 kJ·mol-1.

Key words: Density functional theory, N2, Adsorption, Dissociation, UO

MSC2000: 

  • O641