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Atomically Fine-Tuning Organic–Inorganic Carbon Molecular Sieve Membranes for Hydrogen Production
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    Atomically Fine-Tuning Organic–Inorganic Carbon Molecular Sieve Membranes for Hydrogen Production
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    • Leiqing Hu
      Leiqing Hu
      Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York 14260, United States
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    • Won-Il Lee
      Won-Il Lee
      Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11794, United States
      More by Won-Il Lee
    • Kai Chen
      Kai Chen
      Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York 14260, United States
      More by Kai Chen
    • Soumyabrata Roy
      Soumyabrata Roy
      Department of Materials Science and NanoEngineering, Rice University, Houston, Texas 77005, United States
      Department of Sustainable Energy Engineering, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh 208016, India
    • Kieran Fung
      Kieran Fung
      Department of Mechanical Engineering, University of Colorado, Boulder, Colorado 80309, United States
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    • Kim Kisslinger
      Kim Kisslinger
      Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States
    • Erda Deng
      Erda Deng
      Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York 14260, United States
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    • Yifu Ding
      Yifu Ding
      Department of Mechanical Engineering, University of Colorado, Boulder, Colorado 80309, United States
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    • Pulickel M. Ajayan
      Pulickel M. Ajayan
      Department of Materials Science and NanoEngineering, Rice University, Houston, Texas 77005, United States
    • Chang-Yong Nam*
      Chang-Yong Nam
      Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11794, United States
      Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States
      *Email: [email protected]
    • Haiqing Lin*
      Haiqing Lin
      Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York 14260, United States
      *Email: [email protected]
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    ACS Nano

    Cite this: ACS Nano 2025, 19, 4, 4663–4671
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    https://doi.org/10.1021/acsnano.4c15126
    Published January 20, 2025
    Copyright © 2025 American Chemical Society

    Abstract

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    Polymeric membranes with great processability are attractive for the H2/CO2 separation required for hydrogen production from renewable biomass with carbon capture for utilization and sequestration. However, it remains elusive to engineer polymer architectures to obtain desired sub-3.3 Å ultramicropores to efficiently sieve H2 from CO2. Herein, we demonstrate a scalable way of carbonizing polybenzimidazole (PBI) at low temperatures, followed by vapor phase infiltration (VPI) to atomically narrow ultramicropores throughout the films, forming hybrid organic–inorganic carbon molecular sieves (CMSs). One VPI cycle (100 s) for the PBI carbonized at 500 °C remarkably increases H2/CO2 selectivity from 9.6 to 83 at 100 °C, surpassing Robeson’s upper bound. The CMS demonstrates a stable H2/CO2 separation performance when challenged with simulated syngas streams and can be fabricated into thin-film composite membranes, outperforming state-of-the-art membranes. The scalable approach can be ubiquitous to molecularly fine-tune ultramicropores of leading polymeric membranes to further improve their size-sieving ability and thus separation efficiency.

    Copyright © 2025 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.4c15126.

    • TEM images; SEM images; Raman spectra; XPS spectra; XRD patterns; densities, porosity, and N2 adsorption isotherms of PBITc-t; and detailed H2/CO2 separation performance and testing conditions of the membrane materials selected for comparison and TFC membranes selected for comparison (PDF)

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    ACS Nano

    Cite this: ACS Nano 2025, 19, 4, 4663–4671
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c15126
    Published January 20, 2025
    Copyright © 2025 American Chemical Society

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