物理化学学报 >> 2016, Vol. 32 >> Issue (7): 1666-1673.doi: 10.3866/PKU.WHXB201604012

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胺基功能化的炭材料上二氧化碳吸附的密度泛函理论研究

王娟1,李世坤1,赵侦超1,周丹红2,陆安慧1,张维萍1,*()   

  1. 1 大连理工大学化工学院,精细化工国家重点实验室,辽宁大连116024
    2 辽宁师范大学功能材料化学研究所,辽宁大连116029
  • 收稿日期:2016-01-27 发布日期:2016-07-08
  • 通讯作者: 张维萍 E-mail:wpzhang@dlut.edu.cn
  • 基金资助:
    国家自然科学基金(21373035);中央高校基本科研业务费专项资金(DUT13YQ107)

Density Functional Theory Study of CO2 Adsorption in Amine-Functionalized Carbonaceous Materials

Juan WANG1,Zhen-Chao ZHAO1,Dan-Hong ZHOU2,An-Hui LU1,Wei-Ping ZHANG1,*()   

  1. 1 State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning Province, P. R. China
    2 Institute of Chemistry for Functionalized Materials, Liaoning Normal University, Dalian 116029, Liaoning Province, P. R. China
  • Received:2016-01-27 Published:2016-07-08
  • Contact: Wei-Ping ZHANG E-mail:wpzhang@dlut.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(21373035);Fundamental Research Funds for the Central Universities in China(DUT13YQ107)

摘要:

本文利用色散作用校正的密度泛函理论研究了炭材料上含氮官能团对CO2吸附的作用。通过计算比较了不同含氮官能团炭材料结构片段吸附二氧化碳后的结构参数和能量,由于较强的静电作用和形成弱氢键,含单个苯环的酰胺和吡啶类的吸附剂吸附二氧化碳的作用强于单个苯胺和吡咯类吸附剂。但当增加苯环数时,色散作用主导的吡咯型吸附剂的吸附能力显著增强。以上结果预示着酰胺和吡咯类将是大π体系中具有良好CO2吸附性能的吸附剂。因而,色散作用在CO2吸附过程中也占据着重要地位。计算得到的结果与我们之前的实验结果一致,并且将有利于筛选更有效的二氧化碳吸附剂。

关键词: 炭材料, 二氧化碳捕获, 胺基功能化, 可持续发展的化学, 密度泛函理论计算

Abstract:

Density functional theory with dispersion correction (DFT-D3) was used to investigate the effects of N-doping on the adsorption of CO2 in carbonaceous materials. The CO2 adsorption energies and equilibrium geometry parameters were studied to compare the effects of various N-containing functional groups. The adsorption energies of single amide-and pyridine-type adsorbents were higher than those of aniline-and pyrroletype adsorbents, as a result of strong electrostatic interactions and/or the formation of weak hydrogen bonds. For pyrrole-type adsorbents, the adsorption energy increased with increasing number of benzene rings, because dispersion became the dominant interaction. These findings indicate that amide-and pyrrole-type adsorbents are the most promising CO2 trappers. The calculation results are consistent with our previous experimental conclusions for N-doped carbonaceous materials and will be useful for screening carbon materials to achieve more efficient CO2 capture.

Key words: Cabonaceous material, CO2 capture, Amine-functionalization, Sustainable chemistry, DFT calculation

MSC2000: 

  • O641