Functionalizing Porous Aromatic Frameworks with Polar Organic Groups for High-Capacity and Selective CO2 Separation: A Molecular Simulation Study

被引:122
作者
Babarao, Ravichandar [1 ]
Dai, Sheng [1 ,2 ]
Jiang, De-en [1 ]
机构
[1] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA
[2] Univ Tennessee, Dept Chem, Knoxville, TN 37966 USA
关键词
DER-WAALS COMPLEX; CARBON-DIOXIDE; HYDROGEN STORAGE; CATION-EXCHANGE; GAS-MIXTURES; FORCE-FIELD; AB-INITIO; ADSORPTION; CAPTURE; MEMBRANES;
D O I
10.1021/la104827p
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Porous aromatic frameworks (PAFs) were recently synthesized with the highest surface area to date; one such PAF (PAF-1) has diamond-like structure with biphenyl building blocks and exhibits exceptional thermal and hydrothermal stabilities. Herein, we computationally design new PAFs by introducing polar organic groups to the biphenyl unit and then investigate their separating power toward CO2 by using grand-canonical Monte Carlo (GCMC) simulations. Among these functional PAFs, we found that tetrahydrofuran-like ether-functionalized PAF-1 shows higher adsorption capacity for CO2 at 1 bar and 298 K (10 mol per kilogram of adsorbent) and also much higher selectivities for CO2/CH4, CO2/N-2, and CO2/H-2 mixtures when compared with the amine functionality. The electrostatic interactions are found to play a dominant role in the high CO2 selectivities of functional PAFs, as switching off atomic charges would decrease the selectivity by an order of magnitude. This work suggests that functionalizing porous frameworks with tetrahydrofuran-like ether groups is a promising way to increase CO2 adsorption capacity and selectivity, especially at ambient pressures.
引用
收藏
页码:3451 / 3460
页数:10
相关论文
共 40 条
  • [31] Computational Design of Porous Organic Frameworks for High-Capacity Hydrogen Storage by Incorporating Lithium Tetrazolide Moieties
    Sun, Yingxin
    Ben, Teng
    Wang, Lin
    Qiu, Shilun
    Sun, Huai
    [J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2010, 1 (19): : 2753 - 2756
  • [32] TORRISI A, 2009, J CHEM PHYS, P130
  • [33] TORRISI A, 2010, J CHEM PHYS, P132
  • [34] Functionalized MOFs for Enhanced CO2 Capture
    Torrisi, Antonio
    Bell, Robert G.
    Mellot-Draznieks, Caroline
    [J]. CRYSTAL GROWTH & DESIGN, 2010, 10 (07) : 2839 - 2841
  • [35] Porous Organic Polymers: Distinction from Disorder?
    Trewin, Abbie
    Cooper, Andrew I.
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (09) : 1533 - 1535
  • [36] van der Waals complex of dimethyl ether with carbon dioxide
    Van Ginderen, P
    Herrebout, WA
    van der Veken, BJ
    [J]. JOURNAL OF PHYSICAL CHEMISTRY A, 2003, 107 (28) : 5391 - 5396
  • [37] Ab initio Study of the Interactions between CO2 and N-Containing Organic Heterocycles
    Vogiatzis, Konstantinos D.
    Mavrandonakis, Andreas
    Klopper, Wim
    Froudakis, George E.
    [J]. CHEMPHYSCHEM, 2009, 10 (02) : 374 - 383
  • [38] CO2 adsorption in y and X zeolites modified by alkali metal cation exchange
    Department of Chemical Engineering, Vanderbilt University, VU Station B #351604, 2301 Vanderbilt Place, Nashville, TN 37235-1604, United States
    [J]. Microporous Mesoporous Mater., 2006, 1-3 (78-84): : 78 - 84
  • [39] 2008, MAT STUDIO 4 3
  • [40] [No title captured]