物理化学学报 >> 2016, Vol. 32 >> Issue (9): 2264-2270.doi: 10.3866/PKU.WHXB201606141

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放射性碘分子在Cu2O表面的吸附:第一性原理密度泛函研究

李奎1,赵耀林1,*(),邓佳1,贺朝会1,丁书江2,石伟群3   

  1. 1 西安交通大学核科学与技术学院,西安710049
    2 西安交通大学理学院应用化学系,西安710049
    3 中国科学院高能物理研究所,核辐射与核能技术重点实验室,纳米生物效应与安全性重点实验室,北京100049
  • 收稿日期:2016-04-11 发布日期:2016-09-08
  • 通讯作者: 赵耀林 E-mail:zhaoyaolin@mail.xjtu.edu.cn
  • 基金资助:
    国家自然科学基金(11275147);长江学者和高校创新团队发展计划(IRT1280)

Adsorption of Radioiodine on Cu2O Surfaces: a First-Principles Density Functional Study

Kui LI1,Yao-Lin ZHAO1,*(),Jia DENG1,Chao-Hui HE1,Shu-Jiang DING2,Wei-Qun SHI3   

  1. 1 School of Nuclear Science and Technology, Xi'an Jiaotong University, Xi'an 710049, P. R. China
    2 Department of Applied Chemistry, School of Science, Xi'an Jiaotong University, Xi'an 710049, P. R. China
    3 Key Laboratory of Nuclear Radiation and Nuclear Energy Technology and Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P. R. China
  • Received:2016-04-11 Published:2016-09-08
  • Contact: Yao-Lin ZHAO E-mail:zhaoyaolin@mail.xjtu.edu.cn
  • Supported by:
    National Natural Science Foundation of China(11275147);Program for Changjiang Scholars and Innovative Research Team in University, China(IRT1280)

摘要:

采用第一性原理密度泛函计算方法和周期性平板模型系统研究了放射性碘分子在Cu2O三个低指数表面的吸附行为。通过计算若干平衡吸附构型的结构参数和吸附能评估了不同特征吸附位的作用。构型优化计算表明所选晶面存在适度的结构弛豫。计算结果表明,与Cu2O(110)表面相比,Cu2O(100)和(111)晶面表现出更高的碘分子吸附反应活性。其中,表面氧原子位(OS)和配位未饱和铜原子位(CuCUS)分别为Cu2O(100)和(111)晶面的能量最优吸附位点。此外,针对几种典型吸附结构计算分析了其电子结构信息,以进一步阐明吸附体系之间的相互作用机理。

关键词: 放射性碘分子, Cu2O, 表面吸附, 低指数表面, 密度泛函理论计算

Abstract:

The adsorption behavior of radioiodine (I2) molecules on three different low-index surfaces of cuprous oxide (Cu2O) was systematically investigated using first-principles density functional calculations with periodic slab models. The role of typical surface adsorption sites was evaluated by calculating structural parameters of the adsorption configurations and energy features. Moderate geometry relaxation of the three low-index surfaces was observed. The results of geometry optimization and total energy calculations indicated that the Cu2O(100) and (111) surfaces exhibit higher reactivity towards I2 adsorption than the Cu2O(110) surface. The surface oxygen site (OS) was determined to be the most favorable adsorption site on the Cu2O(100) surface, while the coordinatively unsaturated copper site (CuCUS) was energetically preferred on the Cu2O(111) surface. In addition, the electronic structure information for several typical configurations were explored to explain the detailed interaction mechanism of adsorbed systems.

Key words: Radioiodine molecule, Cu2O, Surface adsorption, Low-index surface, Density functional theory calculation

MSC2000: 

  • O641