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Synthesis of Porous, Nitrogen-Doped Adsorption/Diffusion Carbonaceous Membranes for Efficient CO2 Separation

Authors

  • Xiang Zhu,

    1. State Key Laboratory of Chemical Engineering and Department of Chemistry, East China University of Science and Technology, Shanghai 200237, P.R. China
    2. Chemical Sciences Divisions, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
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  • Songhai Chai,

    1. Chemical Sciences Divisions, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
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  • Chengcheng Tian,

    1. State Key Laboratory of Chemical Engineering and Department of Chemistry, East China University of Science and Technology, Shanghai 200237, P.R. China
    2. Chemical Sciences Divisions, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
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  • Pasquale F. Fulvio,

    1. Chemical Sciences Divisions, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
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  • Kee Sung Han,

    1. Chemical Sciences Divisions, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
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  • Edward W. Hagaman,

    1. Chemical Sciences Divisions, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
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  • Gabriel M. Veith,

    1. Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
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  • Shannon M. Mahurin,

    Corresponding author
    1. Chemical Sciences Divisions, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
    • Chemical Sciences Divisions, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
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  • Suree Brown,

    1. Department of Chemistry, University of Tennessee, Knoxville, TN 37966, USA
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  • Honglai Liu,

    Corresponding author
    1. State Key Laboratory of Chemical Engineering and Department of Chemistry, East China University of Science and Technology, Shanghai 200237, P.R. China
    • State Key Laboratory of Chemical Engineering and Department of Chemistry, East China University of Science and Technology, Shanghai 200237, P.R. China
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  • Sheng Dai

    Corresponding author
    1. Chemical Sciences Divisions, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
    2. Department of Chemistry, University of Tennessee, Knoxville, TN 37966, USA
    • Chemical Sciences Divisions, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
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Abstract

A porous, nitrogen-doped carbonaceous free-standing membrane (TFMT-550) is prepared by a facile template-free method using letrozole as an intermediate to a triazole-functionalized-triazine framework, followed by carbonization. Such adsorption/diffusion membranes exhibit good separation performance of CO2 over N2 and surpassing the most recent Robeson upper bound. An exceptional ideal CO2/N2 permselectivity of 47.5 was achieved with a good CO2 permeability of 2.40 × 10−13 mol m m−2 s−1 Pa−1. The latter results arise from the presence of micropores, narrow distribution of small mesopores and from the strong dipole–quadrupole interactions between the large quadrupole moment of CO2 molecules and the polar sites associated with N groups (e.g., triazine units) within the framework.

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