Tailoring sub-3.3 Å ultramicropores in advanced carbon molecular sieve membranes for blue hydrogen production
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- Leiqing Hu
- Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.
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- Vinh T. Bui
- Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.
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- Ajay Krishnamurthy
- Theiss Research, La Jolla, CA 92037, USA.
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- Shouhong Fan
- Department of Mechanical Engineering, University of Colorado, Boulder, CO 80309, USA.
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- Wenji Guo
- Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.
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- Sankhajit Pal
- Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.
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- Xiaoyi Chen
- Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.
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- Gengyi Zhang
- Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.
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- Yifu Ding
- Department of Mechanical Engineering, University of Colorado, Boulder, CO 80309, USA.
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- Rajinder P. Singh
- Materials Physics and Applications Division, Carbon Capture and Separations for Energy Applications (CaSEA) Labs, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
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- Monica Lupion
- Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.
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- Haiqing Lin
- Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.
説明
<jats:p> Carbon molecular sieve (CMS) membranes prepared by carbonization of polymers containing strongly size-sieving ultramicropores are attractive for high-temperature gas separations. However, polymers need to be carbonized at extremely high temperatures (900° to 1200°C) to achieve sub-3.3 Å ultramicroporous channels for H <jats:sub>2</jats:sub> /CO <jats:sub>2</jats:sub> separation, which makes them brittle and impractical for industrial applications. Here, we demonstrate that polymers can be first doped with thermolabile cross-linkers before low-temperature carbonization to retain the polymer processability and achieve superior H <jats:sub>2</jats:sub> /CO <jats:sub>2</jats:sub> separation properties. Specifically, polybenzimidazole (PBI) is cross-linked with pyrophosphoric acid (PPA) via H bonding and proton transfer before carbonization at ≤600°C. The synergistic PPA doping and subsequent carbonization of PBI increase H <jats:sub>2</jats:sub> permeability from 27 to 140 Barrer and H <jats:sub>2</jats:sub> /CO <jats:sub>2</jats:sub> selectivity from 15 to 58 at 150°C, superior to state-of-the-art polymeric materials and surpassing Robeson’s upper bound. This study provides a facile and effective way to tailor subnanopore size and porosity in CMS membranes with desirable molecular sieving ability. </jats:p>
収録刊行物
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- Science Advances
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Science Advances 8 (10), 2022-03-11
American Association for the Advancement of Science (AAAS)
