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Title: Unexpectedly Strong Size-Sieving Ability in Carbonized Polybenzimidazole for Membrane H2/CO2 Separation

Abstract

Polymers with high permeability and strong size-sieving ability are needed for H2/CO2 separation at temperatures ranging from 100 to 300 °C to enable an energy-efficient precombustion CO2 capture process. However, such polymers usually suffer from a permeability/selectivity tradeoff, that is, polymers with high permeability tend to exhibit a weak size-sieving ability and thus low selectivity. In this work, we demonstrate that carbonization of a suitable polymer precursor (i.e., polybenzimidazole or PBI) generates microcavities (leading to high H2 permeability) and ultramicroporous channels (leading to strong size-sieving ability and thus high H2/CO2 selectivity). Specifically, carbonization of PBI at 900 °C (CMS@900) doubles H2 permeability and increases H2/CO2 selectivity from 14 to 80 at 150 °C. When tested with simulated syngas-containing equimolar H2 and CO2 in the presence of water vapor for 120 h, CMS@900 exhibits stable H2 permeability of ≈36 barrer and H2/CO2 selectivity of ≈53 at 150 °C, above Robeson’s 2008 upper bound and demonstrating robustness against physical aging and CO2 plasticization.

Authors:
 [1];  [1]; ORCiD logo [1];  [2];  [2]; ORCiD logo [3];  [4]; ORCiD logo [1]; ORCiD logo [1]
  1. State Univ. of New York (SUNY), Buffalo, NY (United States)
  2. Commonwealth Scientific and Industrial Research Organization (CSIRO) Future Industries, Clayton, SV (Australia)
  3. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  4. Univ. of Waterloo, ON (Canada)
Publication Date:
Research Org.:
State Univ. of New York (SUNY), Buffalo, NY (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE), Clean Coal and Carbon Management
OSTI Identifier:
1601453
Alternate Identifier(s):
OSTI ID: 1864402
Grant/Contract Number:  
FE0031636; 1554236
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 11; Journal Issue: 50; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; carbon capture; hydrogen production; carbon molecular sieve membranes; polybenzimidazole; H2/CO2 separation

Citation Formats

Omidvar, Maryam, Nguyen, Hien, Huang, Liang, Doherty, Cara M., Hill, Anita J., Stafford, Christopher M., Feng, Xianshe, Swihart, Mark T., and Lin, Haiqing. Unexpectedly Strong Size-Sieving Ability in Carbonized Polybenzimidazole for Membrane H2/CO2 Separation. United States: N. p., 2019. Web. doi:10.1021/acsami.9b16966.
Omidvar, Maryam, Nguyen, Hien, Huang, Liang, Doherty, Cara M., Hill, Anita J., Stafford, Christopher M., Feng, Xianshe, Swihart, Mark T., & Lin, Haiqing. Unexpectedly Strong Size-Sieving Ability in Carbonized Polybenzimidazole for Membrane H2/CO2 Separation. United States. https://doi.org/10.1021/acsami.9b16966
Omidvar, Maryam, Nguyen, Hien, Huang, Liang, Doherty, Cara M., Hill, Anita J., Stafford, Christopher M., Feng, Xianshe, Swihart, Mark T., and Lin, Haiqing. Thu . "Unexpectedly Strong Size-Sieving Ability in Carbonized Polybenzimidazole for Membrane H2/CO2 Separation". United States. https://doi.org/10.1021/acsami.9b16966. https://www.osti.gov/servlets/purl/1601453.
@article{osti_1601453,
title = {Unexpectedly Strong Size-Sieving Ability in Carbonized Polybenzimidazole for Membrane H2/CO2 Separation},
author = {Omidvar, Maryam and Nguyen, Hien and Huang, Liang and Doherty, Cara M. and Hill, Anita J. and Stafford, Christopher M. and Feng, Xianshe and Swihart, Mark T. and Lin, Haiqing},
abstractNote = {Polymers with high permeability and strong size-sieving ability are needed for H2/CO2 separation at temperatures ranging from 100 to 300 °C to enable an energy-efficient precombustion CO2 capture process. However, such polymers usually suffer from a permeability/selectivity tradeoff, that is, polymers with high permeability tend to exhibit a weak size-sieving ability and thus low selectivity. In this work, we demonstrate that carbonization of a suitable polymer precursor (i.e., polybenzimidazole or PBI) generates microcavities (leading to high H2 permeability) and ultramicroporous channels (leading to strong size-sieving ability and thus high H2/CO2 selectivity). Specifically, carbonization of PBI at 900 °C (CMS@900) doubles H2 permeability and increases H2/CO2 selectivity from 14 to 80 at 150 °C. When tested with simulated syngas-containing equimolar H2 and CO2 in the presence of water vapor for 120 h, CMS@900 exhibits stable H2 permeability of ≈36 barrer and H2/CO2 selectivity of ≈53 at 150 °C, above Robeson’s 2008 upper bound and demonstrating robustness against physical aging and CO2 plasticization.},
doi = {10.1021/acsami.9b16966},
journal = {ACS Applied Materials and Interfaces},
number = 50,
volume = 11,
place = {United States},
year = {Thu Nov 21 00:00:00 EST 2019},
month = {Thu Nov 21 00:00:00 EST 2019}
}

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