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Title: Creation of Well-Defined “Mid-Sized” Micropores in Carbon Molecular Sieve Membranes

Abstract

Carbon molecular sieve (CMS) membranes are choices for the separation of organic molecules due to their stability, ability to be scaled at practical form factors, and the avoidance of expensive supports or complex multi-step fabrication processes. A critical challenge is the creation of “mid-range” (e.g., 5–9 Å) microstructures that allow for facile permeation of organic solvents and selection between similarly-sized guest molecules. In this work, we create these microstructures via the pyrolysis of a microporous polymer (PIM-1) under low concentrations of hydrogen gas. The introduction of H2 inhibits aromatization of the decomposing polymer and ultimately results in the creation of a well-defined bimodal pore network that exhibits an ultramicropore size of 5.1 Å. The H2 assisted CMS dense membranes show a dramatic increase in p-xylene ideal permeability (≈15 times), with little loss in p-xylene/o-xylene selectivity (18.8 vs. 25.0) when compared to PIM-1 membranes pyrolyzed under a pure argon atmosphere. This method is successfully extended to hollow fiber membranes operating in organic solvent reverse osmosis mode, highlighting the potential of this approach to be translated from the laboratory to the field.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); ExxonMobil Research and Engineering
OSTI Identifier:
1566018
Report Number(s):
LLNL-JRNL-769201
Journal ID: ISSN 1433-7851; 960479
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 58; Journal Issue: 38; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; carbon molecular sieves; hydrogen; membranes; polymers of intrinsic microporosity; xylene isomer separation

Citation Formats

Ma, Yao, Jue, Melinda L., Zhang, Fengyi, Mathias, Ronita, Jang, Hye Youn, and Lively, Ryan P. Creation of Well-Defined “Mid-Sized” Micropores in Carbon Molecular Sieve Membranes. United States: N. p., 2019. Web. doi:10.1002/anie.201903105.
Ma, Yao, Jue, Melinda L., Zhang, Fengyi, Mathias, Ronita, Jang, Hye Youn, & Lively, Ryan P. Creation of Well-Defined “Mid-Sized” Micropores in Carbon Molecular Sieve Membranes. United States. doi:10.1002/anie.201903105.
Ma, Yao, Jue, Melinda L., Zhang, Fengyi, Mathias, Ronita, Jang, Hye Youn, and Lively, Ryan P. Sat . "Creation of Well-Defined “Mid-Sized” Micropores in Carbon Molecular Sieve Membranes". United States. doi:10.1002/anie.201903105. https://www.osti.gov/servlets/purl/1566018.
@article{osti_1566018,
title = {Creation of Well-Defined “Mid-Sized” Micropores in Carbon Molecular Sieve Membranes},
author = {Ma, Yao and Jue, Melinda L. and Zhang, Fengyi and Mathias, Ronita and Jang, Hye Youn and Lively, Ryan P.},
abstractNote = {Carbon molecular sieve (CMS) membranes are choices for the separation of organic molecules due to their stability, ability to be scaled at practical form factors, and the avoidance of expensive supports or complex multi-step fabrication processes. A critical challenge is the creation of “mid-range” (e.g., 5–9 Å) microstructures that allow for facile permeation of organic solvents and selection between similarly-sized guest molecules. In this work, we create these microstructures via the pyrolysis of a microporous polymer (PIM-1) under low concentrations of hydrogen gas. The introduction of H2 inhibits aromatization of the decomposing polymer and ultimately results in the creation of a well-defined bimodal pore network that exhibits an ultramicropore size of 5.1 Å. The H2 assisted CMS dense membranes show a dramatic increase in p-xylene ideal permeability (≈15 times), with little loss in p-xylene/o-xylene selectivity (18.8 vs. 25.0) when compared to PIM-1 membranes pyrolyzed under a pure argon atmosphere. This method is successfully extended to hollow fiber membranes operating in organic solvent reverse osmosis mode, highlighting the potential of this approach to be translated from the laboratory to the field.},
doi = {10.1002/anie.201903105},
journal = {Angewandte Chemie (International Edition)},
number = 38,
volume = 58,
place = {United States},
year = {2019},
month = {6}
}

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