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Title: Polybenzimidazole based random copolymers containing hexafluoroisopropylidene functional groups for gas separations at elevated temperatures

Abstract

Polybenzimidazoles (PBIs) are attractive membrane materials for H 2/CO 2 separation at hydrocarbon fuel derived synthesis gas operating conditions due to their exceptional physicochemical stability and promising permselectivity character. PBI molecular structure modification is a viable approach to disrupt chain packing altering the free-volume architecture which results in improved gas transport characteristics. This work is focused on the synthesis and characterization of novel PBI random copolymers for application as elevated temperature H 2/CO 2 membranes. The co-polymerization route is expected to result in tailorable permeability and selectivity by combining the high H 2 permeability aspect of the highly disrupted loosely packed hexafluoroisopropylidene diphenyl group containing PBI segments (6F-PBI) with the highly selective tightly packed phenylene group containing PBI segments (m-PBI). 6F/m-PBI copolymers with varying 6F-PBI and m-PBI ratios having high inherent viscosity were synthesized. The structure and ratio of the 6F- and m-PBI fractions were confirmed using FTIR and NMR spectroscopic techniques. The measured gas transport properties of copolymer thin films cast in controlled environment were measured as a function of the operating conditions. Lastly, the H 2 permeability increased while H 2/CO 2 selectivity decreased as the 6F-PBI copolymer fraction was increased.

Authors:
ORCiD logo [1];  [2];  [1];  [2]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. of South Carolina, Columbia, SC (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1467203
Alternate Identifier(s):
OSTI ID: 1396514
Report Number(s):
LA-UR-17-23507
Journal ID: ISSN 0032-3861
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Polymer
Additional Journal Information:
Journal Volume: 119; Journal Issue: C; Journal ID: ISSN 0032-3861
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Energy Sciences; Material Science; Polybenzimidazole; Random copolymer; Pre-combustion; Carbon capture; Synthesis gas; Hydrogen selective membrane

Citation Formats

Singh, Rajinder Pal, Li, Xin, Dudeck, Kevin Wade, Benicewicz, Brian C., and Berchtold, Kathryn A. Polybenzimidazole based random copolymers containing hexafluoroisopropylidene functional groups for gas separations at elevated temperatures. United States: N. p., 2017. Web. doi:10.1016/j.polymer.2017.04.075.
Singh, Rajinder Pal, Li, Xin, Dudeck, Kevin Wade, Benicewicz, Brian C., & Berchtold, Kathryn A. Polybenzimidazole based random copolymers containing hexafluoroisopropylidene functional groups for gas separations at elevated temperatures. United States. doi:10.1016/j.polymer.2017.04.075.
Singh, Rajinder Pal, Li, Xin, Dudeck, Kevin Wade, Benicewicz, Brian C., and Berchtold, Kathryn A. Fri . "Polybenzimidazole based random copolymers containing hexafluoroisopropylidene functional groups for gas separations at elevated temperatures". United States. doi:10.1016/j.polymer.2017.04.075. https://www.osti.gov/servlets/purl/1467203.
@article{osti_1467203,
title = {Polybenzimidazole based random copolymers containing hexafluoroisopropylidene functional groups for gas separations at elevated temperatures},
author = {Singh, Rajinder Pal and Li, Xin and Dudeck, Kevin Wade and Benicewicz, Brian C. and Berchtold, Kathryn A.},
abstractNote = {Polybenzimidazoles (PBIs) are attractive membrane materials for H2/CO2 separation at hydrocarbon fuel derived synthesis gas operating conditions due to their exceptional physicochemical stability and promising permselectivity character. PBI molecular structure modification is a viable approach to disrupt chain packing altering the free-volume architecture which results in improved gas transport characteristics. This work is focused on the synthesis and characterization of novel PBI random copolymers for application as elevated temperature H2/CO2 membranes. The co-polymerization route is expected to result in tailorable permeability and selectivity by combining the high H2 permeability aspect of the highly disrupted loosely packed hexafluoroisopropylidene diphenyl group containing PBI segments (6F-PBI) with the highly selective tightly packed phenylene group containing PBI segments (m-PBI). 6F/m-PBI copolymers with varying 6F-PBI and m-PBI ratios having high inherent viscosity were synthesized. The structure and ratio of the 6F- and m-PBI fractions were confirmed using FTIR and NMR spectroscopic techniques. The measured gas transport properties of copolymer thin films cast in controlled environment were measured as a function of the operating conditions. Lastly, the H2 permeability increased while H2/CO2 selectivity decreased as the 6F-PBI copolymer fraction was increased.},
doi = {10.1016/j.polymer.2017.04.075},
journal = {Polymer},
number = C,
volume = 119,
place = {United States},
year = {Fri Apr 28 00:00:00 EDT 2017},
month = {Fri Apr 28 00:00:00 EDT 2017}
}

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