物理化学学报 >> 2011, Vol. 27 >> Issue (03): 553-558.doi: 10.3866/PKU.WHXB20110319

理论与计算化学 上一篇    下一篇

二氧化碳在金属-有机骨架材料中吸附的阶梯现象

安晓辉, 刘大欢, 仲崇立   

  1. 北京化工大学化学工程学院, 计算化学研究室, 北京 100029
  • 收稿日期:2010-09-15 修回日期:2010-11-22 发布日期:2011-03-03
  • 通讯作者: 刘大欢 E-mail:liudh@mail.buct.edu.cn
  • 基金资助:

    国家杰出青年科学基金(20725622)和国家自然科学基金(20876006, 20821004, 20906002)资助项目

Stepped Behavior of Carbon Dioxide Adsorption in Metal-Organic Frameworks

AN Xiao-Hui, LIU Da-Huan, ZHONG Chong-Li   

  1. Laboratory of Computational Chemistry, School of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China
  • Received:2010-09-15 Revised:2010-11-22 Published:2011-03-03
  • Contact: LIU Da-Huan E-mail:liudh@mail.buct.edu.cn
  • Supported by:

    The project was supported by the National Outstanding Young Scientists Foundation of China (20725622) and National Natural Science Foundation of China ( 20876006, 20821004, 20906002).

摘要:

采用巨正则系综蒙特卡罗(GCMC)模拟方法, 对二氧化碳在5种具有相同拓扑结构的金属-有机骨架材料(IRMOFs), 即IRMOF-1, -8, -10, -14, -16中吸附产生的阶梯现象进行了详细的研究. 结果表明: 低温条件下, 孔径越大的IRMOFs越容易发生阶梯现象; 发生阶梯现象的转变压力与能够发生阶梯现象的转变温度都与孔径呈线性关系. 此外, 模拟结果进一步验证了二氧化碳分子之间的静电作用力是阶梯现象发生的关键因素. 这些规律将为金属-有机骨架材料(MOFs)的设计和改性以及二氧化碳在混合气体中的吸附分离提供有用的信息.

关键词: 吸附, 二氧化碳, 金属-有机骨架材料, 阶梯现象

Abstract:

Grand canonical Monte Carlo (GCMC) simulations were performed to study the stepped behaviors of carbon dioxide adsorption in the following five isoreticular metal-organic frameworks (IRMOFs): IRMOF-1, -8, -10, -14, -16. The simulation results show that the stepped phenomenon occurs easily when the temperature is low and the pore size is large for these IRMOFs. The critical pressure and temperature where the stepped behavior occurs show a linear relationship with the pore size. The results also further indicate that the electrostatic interaction between CO2 and CO2 molecules plays a dominant role on the stepped behavior. All these findings may provide useful information for the design and modification of MOFs for the adsorption and separation of carbon dioxide in gas mixtures.

Key words: Adsorption, Carbon dioxide, Metal-organic frameworks, Stepped behavior

MSC2000: 

  • O641