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Title: Scalable Polymeric Few-Nanometer Organosilica Membranes with Hydrothermal Stability for Selective Hydrogen Separation

Abstract

Nanoporous silica membranes exhibit excellent H2/CO2 separation properties for sustainable H2 production and CO2 capture but are prepared via complicated thermal processes above 400 °C, which prevent their scalable production at a low cost. Here, we demonstrate the rapid fabrication (within 2 min) of ultrathin silica-like membranes (~3 nm) via an oxygen plasma treatment of polydimethylsiloxane-based thin-film composite membranes at 20 °C. The resulting organosilica membranes unexpectedly exhibit H2 permeance of 280-930 GPU (1 GPU = 3.347 x 10-10 mol m-2 s-1 Pa-1) and H2/CO2 selectivity of 93-32 at 200 °C, far surpassing state-of-the-art membranes and Robeson’s upper bound for H2/CO2 separation. When challenged with a 3 d simulated syngas test containing water vapor at 200 °C and a 340 d stability test, the membrane shows durable separation performance and excellent hydrothermal stability. The robust H2/CO2 separation properties coupled with excellent scalability demonstrate the great potential of these organosilica membranes for economic H2 production with minimal carbon emissions.

Authors:
 [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [4];  [3]; ORCiD logo [2]; ORCiD logo [2]
  1. Univ. at Buffalo, NY (United States); National Energy Technology Lab. (NETL), Pittsburgh, PA (United States)
  2. Univ. at Buffalo, NY (United States)
  3. National Energy Technology Lab. (NETL), Pittsburgh, PA (United States)
  4. University of Colorado at Boulder, Boulder, Colorado 80309, United States
Publication Date:
Research Org.:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
Sponsoring Org.:
USDOE; National Science Foundation (NSF)
OSTI Identifier:
1842487
Grant/Contract Number:  
89243318CFE000003; FE0026463; 1554236
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 15; Journal Issue: 7; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; silica membranes; CO2 capture; hydrogen purification; oxygen plasma; polydimethylsiloxane; H2/CO2 separation

Citation Formats

Zhu, Lingxiang, Huang, Liang, Venna, Surendar R., Blevins, Adrienne K., Ding, Yifu, Hopkinson, David P., Swihart, Mark T., and Lin, Haiqing. Scalable Polymeric Few-Nanometer Organosilica Membranes with Hydrothermal Stability for Selective Hydrogen Separation. United States: N. p., 2021. Web. doi:10.1021/acsnano.1c03492.
Zhu, Lingxiang, Huang, Liang, Venna, Surendar R., Blevins, Adrienne K., Ding, Yifu, Hopkinson, David P., Swihart, Mark T., & Lin, Haiqing. Scalable Polymeric Few-Nanometer Organosilica Membranes with Hydrothermal Stability for Selective Hydrogen Separation. United States. https://doi.org/10.1021/acsnano.1c03492
Zhu, Lingxiang, Huang, Liang, Venna, Surendar R., Blevins, Adrienne K., Ding, Yifu, Hopkinson, David P., Swihart, Mark T., and Lin, Haiqing. 2021. "Scalable Polymeric Few-Nanometer Organosilica Membranes with Hydrothermal Stability for Selective Hydrogen Separation". United States. https://doi.org/10.1021/acsnano.1c03492. https://www.osti.gov/servlets/purl/1842487.
@article{osti_1842487,
title = {Scalable Polymeric Few-Nanometer Organosilica Membranes with Hydrothermal Stability for Selective Hydrogen Separation},
author = {Zhu, Lingxiang and Huang, Liang and Venna, Surendar R. and Blevins, Adrienne K. and Ding, Yifu and Hopkinson, David P. and Swihart, Mark T. and Lin, Haiqing},
abstractNote = {Nanoporous silica membranes exhibit excellent H2/CO2 separation properties for sustainable H2 production and CO2 capture but are prepared via complicated thermal processes above 400 °C, which prevent their scalable production at a low cost. Here, we demonstrate the rapid fabrication (within 2 min) of ultrathin silica-like membranes (~3 nm) via an oxygen plasma treatment of polydimethylsiloxane-based thin-film composite membranes at 20 °C. The resulting organosilica membranes unexpectedly exhibit H2 permeance of 280-930 GPU (1 GPU = 3.347 x 10-10 mol m-2 s-1 Pa-1) and H2/CO2 selectivity of 93-32 at 200 °C, far surpassing state-of-the-art membranes and Robeson’s upper bound for H2/CO2 separation. When challenged with a 3 d simulated syngas test containing water vapor at 200 °C and a 340 d stability test, the membrane shows durable separation performance and excellent hydrothermal stability. The robust H2/CO2 separation properties coupled with excellent scalability demonstrate the great potential of these organosilica membranes for economic H2 production with minimal carbon emissions.},
doi = {10.1021/acsnano.1c03492},
url = {https://www.osti.gov/biblio/1842487}, journal = {ACS Nano},
issn = {1936-0851},
number = 7,
volume = 15,
place = {United States},
year = {Tue Jul 13 00:00:00 EDT 2021},
month = {Tue Jul 13 00:00:00 EDT 2021}
}

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