物理化学学报 >> 2012, Vol. 28 >> Issue (05): 1101-1106.doi: 10.3866/PKU.WHXB201203054

理论与计算化学 上一篇    下一篇

甲烷与含氮有机杂环化合物吸附作用的DFT研究

蒋倩1, 储伟1, 孙文晶1, 刘凤嗣1, 薛英2   

  1. 1. 四川大学化学工程学院, 成都 610065;
    2. 四川大学化学学院, 成都 610064
  • 收稿日期:2012-01-05 修回日期:2012-03-02 发布日期:2012-04-26
  • 通讯作者: 储伟, 孙文晶 E-mail:chuwei1965@scu.edu.cn; sunwenjing_a@163.com
  • 基金资助:

    国家重点基础研究发展规划项目(973) (2011CB201202)资助

A DFT Study of Methane Adsorption on Nitrogen-Containing Organic Heterocycles

JIANG Qian1, CHU Wei1, SUN Wen-Jing1, LIU Feng-Si1, XUE Ying2   

  1. 1. Department of Chemical Engineering, Sichuan University, Chengdu 610065, P. R. China;
    2. Department of Chemistry, Sichuan University, Chengdu 610064, P. R. China
  • Received:2012-01-05 Revised:2012-03-02 Published:2012-04-26
  • Contact: CHU Wei, SUN Wen-Jing E-mail:chuwei1965@scu.edu.cn; sunwenjing_a@163.com
  • Supported by:

    The project was supported by the National Key Basic Research Program of China (973) (2011CB201202).

摘要: 根据煤中氮的存在形式, 提炼出11种具有不同杂化方式及含氮量的有机环状化合物. 应用密度泛函理论(DFT)模拟方法对甲烷在这11种含氮化合物上的吸附模型进行结构优化, 并结合吸附能、电荷分布及静电势能面的分析, 从微观角度考察了甲烷与这些化合物之间的相互作用. 计算结果表明: 甲烷与含氮化合物的相互作用能在3.81-6.82 kJ·mol-1范围内, 且通过氢键和静电力相互作用; 当化合物中氮的杂化方式为sp2时, 其与甲烷的作用能大于sp3杂化方式的; 当化合物中的氮含量增加时, 可以提供更多的甲烷吸附位点.

关键词: 甲烷, 吸附, 含氮化合物, 密度泛函理论模拟方法

Abstract: In coal, nitrogen exists in a variety of forms. We presented 11 compounds of different hybridization forms and nitrogen contents. Density functional theory (DFT) simulation method was employed to study the adsorption behaviors of methane on these nitrogen-containing organic compounds. The interactions were studied and characterized by their adsorption energies, Mulliken charges and electrostatic potential surfaces. The adsorption energies varied from 3.81 to 6.82 kJ·mol-1, attributable to the weak hydrogen-bonding and electrostatic interactions. The results revealed that the adsorption energy of sp2-N with methane was higher than that of sp3-N and that higher nitrogen contents provided more positive sites for methane adsorption.

Key words: Methane, Adsorption, Nitrogen-containing compound, Density functional theory simulation method

MSC2000: 

  • O641