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Title: Hyperaging Tuning of a Carbon Molecular-Sieve Hollow Fiber Membrane with Extraordinary Gas-Separation Performance and Stability

Abstract

Abstract This study reports 6FDA:BPDA‐DAM polyimide‐derived hollow fiber carbon molecular‐sieve (CMS) membranes for hydrogen and ethylene separation. Since H 2 /C 2 H 4 selectivity is the lowest among H 2 /(C 1 ‐C 3 ) hydrocarbons, an optimized CMS fiber for this gas pair is useful for removing hydrogen from all‐cracked gas mixtures. A process we term hyperaging provides highly selective CMS fiber membranes by tuning CMS ultramicropores to favor H 2 over larger molecules to give a H 2 /C 2 H 4 selectivity of over 250. Hyperaging conditions and a hyperaging mechanism are discussed in terms of an expedited physical aging process, which is largely controlled by the hyperaging temperature. For the specific CMS material considered here, a hyperaging temperature beyond 90 °C but less than 250 °C works best. Hyperaging also stabilizes CMS materials against physical aging and stabilizes the performance of H 2 separation over extended periods. This work opens a door in the development of CMS materials for the separation of small molecules from large molecules.

Authors:
ORCiD logo [1];  [1];  [1];  [2];  [2];  [2];  [2];  [1]; ORCiD logo [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States)
  2. Dow Chemical Co., Freeport, TX (United States)
Publication Date:
Research Org.:
Georgia Institute of Technology, Atlanta, GA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1594570
Alternate Identifier(s):
OSTI ID: 1542474
Grant/Contract Number:  
FG02-04ER15510
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 58; Journal Issue: 34; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carbon molecular-sieve membranes; gas separation; hollow fiber; hydrocarbon; hydrogen/ethylene separation

Citation Formats

Qiu, Wulin, Vaughn, Justin, Liu, Gongping, Xu, Liren, Brayden, Mark, Martinez, Marcos, Fitzgibbons, Thomas, Wenz, Graham, and Koros, William J. Hyperaging Tuning of a Carbon Molecular-Sieve Hollow Fiber Membrane with Extraordinary Gas-Separation Performance and Stability. United States: N. p., 2019. Web. doi:10.1002/anie.201904913.
Qiu, Wulin, Vaughn, Justin, Liu, Gongping, Xu, Liren, Brayden, Mark, Martinez, Marcos, Fitzgibbons, Thomas, Wenz, Graham, & Koros, William J. Hyperaging Tuning of a Carbon Molecular-Sieve Hollow Fiber Membrane with Extraordinary Gas-Separation Performance and Stability. United States. https://doi.org/10.1002/anie.201904913
Qiu, Wulin, Vaughn, Justin, Liu, Gongping, Xu, Liren, Brayden, Mark, Martinez, Marcos, Fitzgibbons, Thomas, Wenz, Graham, and Koros, William J. Tue . "Hyperaging Tuning of a Carbon Molecular-Sieve Hollow Fiber Membrane with Extraordinary Gas-Separation Performance and Stability". United States. https://doi.org/10.1002/anie.201904913. https://www.osti.gov/servlets/purl/1594570.
@article{osti_1594570,
title = {Hyperaging Tuning of a Carbon Molecular-Sieve Hollow Fiber Membrane with Extraordinary Gas-Separation Performance and Stability},
author = {Qiu, Wulin and Vaughn, Justin and Liu, Gongping and Xu, Liren and Brayden, Mark and Martinez, Marcos and Fitzgibbons, Thomas and Wenz, Graham and Koros, William J.},
abstractNote = {Abstract This study reports 6FDA:BPDA‐DAM polyimide‐derived hollow fiber carbon molecular‐sieve (CMS) membranes for hydrogen and ethylene separation. Since H 2 /C 2 H 4 selectivity is the lowest among H 2 /(C 1 ‐C 3 ) hydrocarbons, an optimized CMS fiber for this gas pair is useful for removing hydrogen from all‐cracked gas mixtures. A process we term hyperaging provides highly selective CMS fiber membranes by tuning CMS ultramicropores to favor H 2 over larger molecules to give a H 2 /C 2 H 4 selectivity of over 250. Hyperaging conditions and a hyperaging mechanism are discussed in terms of an expedited physical aging process, which is largely controlled by the hyperaging temperature. For the specific CMS material considered here, a hyperaging temperature beyond 90 °C but less than 250 °C works best. Hyperaging also stabilizes CMS materials against physical aging and stabilizes the performance of H 2 separation over extended periods. This work opens a door in the development of CMS materials for the separation of small molecules from large molecules.},
doi = {10.1002/anie.201904913},
journal = {Angewandte Chemie (International Edition)},
number = 34,
volume = 58,
place = {United States},
year = {Tue Jun 11 00:00:00 EDT 2019},
month = {Tue Jun 11 00:00:00 EDT 2019}
}

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Free Publicly Available Full Text
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Figures / Tables:

Figure 1 Figure 1: CMS fiber separation performance vs. a) Hyperaging temperature (for 18 hrs); b) Hyperaging time (at 110 °C); c) Hyperaging temperature and hyperaging time; and (d) Limits of hyperaging temperature and hyperaging time.

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Works referenced in this record:

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.