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Ultrathin Two-Dimensional Membranes Assembled by Ionic Covalent Organic Nanosheets with Reduced Apertures for Gas Separation

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    Ultrathin Two-Dimensional Membranes Assembled by Ionic Covalent Organic Nanosheets with Reduced Apertures for Gas Separation
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    • Yunpan Ying
      Yunpan Ying
      Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore 117585, Singapore
      More by Yunpan Ying
      Orcidhttp://orcid.org/0000-0002-2279-7191
    • Minman Tong
      Minman Tong
      School of Chemistry and Materials Science, Jiangsu Normal University, No. 101 of Shanghai Road, Xuzhou 221116, China
      More by Minman Tong
      Orcidhttp://orcid.org/0000-0002-9357-5684
    • Shoucong Ning
      Shoucong Ning
      Department of Materials Science and Engineering, National University of Singapore, 9 Engineering Drive 1, Singapore 117575, Singapore
      More by Shoucong Ning
    • Sai Kishore Ravi
      Sai Kishore Ravi
      Department of Materials Science and Engineering, National University of Singapore, 9 Engineering Drive 1, Singapore 117575, Singapore
      More by Sai Kishore Ravi
    • Shing Bo Peh
      Shing Bo Peh
      Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore 117585, Singapore
      More by Shing Bo Peh
    • Swee Ching Tan
      Swee Ching Tan
      Department of Materials Science and Engineering, National University of Singapore, 9 Engineering Drive 1, Singapore 117575, Singapore
      More by Swee Ching Tan
      Orcidhttp://orcid.org/0000-0003-2074-8385
    • Stephen John Pennycook
      Stephen John Pennycook
      Department of Materials Science and Engineering, National University of Singapore, 9 Engineering Drive 1, Singapore 117575, Singapore
      More by Stephen John Pennycook
      Orcidhttp://orcid.org/0000-0002-3210-6323
    • Dan Zhao*
      Dan Zhao
      Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore 117585, Singapore
      *[email protected]
      More by Dan Zhao
      Orcidhttp://orcid.org/0000-0002-4427-2150
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2020, 142, 9, 4472–4480
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    https://doi.org/10.1021/jacs.9b13825
    Published February 14, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    Covalent organic frameworks (COFs) are a promising category of porous materials possessing extensive chemical tunability, high porosity, ordered arrangements at a molecular level, and considerable chemical stability. Despite these advantages, the application of COFs as membrane materials for gas separation is limited by their relatively large pore apertures (typically >0.5 nm), which exceed the sieving requirements for most gases whose kinetic diameters are less than 0.4 nm. Herein, we report the fabrication of ultrathin two-dimensional (2D) membranes through layer-by-layer (LbL) assembly of two kinds of ionic covalent organic nanosheets (iCONs) with different pore sizes and opposite charges. Because of the staggered packing of iCONs with strong electrostatic interactions, the resultant membranes exhibit features of reduced aperture size, optimized stacking pattern, and compact dense structure without sacrificing thickness control, which are suitable for molecular sieving gas separation. One of the hybrid membranes, TpEBr@TpPa-SO3Na with a thickness of 41 nm, shows a H2 permeance of 2566 gas permeation units (GPUs) and a H2/CO2 separation factor of 22.6 at 423 K, surpassing the recent Robeson upper bound along with long-term hydrothermal stability. This strategy provides not only a high-performance H2 separation membrane candidate but also an inspiration for pore engineering of COF or 2D porous polymer membranes.

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