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Title: Iron-containing carbon molecular sieve membranes for advanced olefin/paraffin separations

Abstract

Here, carbon molecular sieve (CMS) dense film membranes derived from 6FDA-DAM:DABA (3:2) polyimide precursor were studied for separation of mixed olefins (C2H4 and C3H6) from paraffins (C2H6 and C3H8). Olefin-selective CMS membranes with high performance can be made by pyrolysis of metal-containing polymeric precursors. Pyrolyzed at 550 °C with a fast ramp rate, CMS membranes with integrated Fe2+ (2.2 wt% in the precursor) showed 19% higher C2H4/C2H6 and 11% higher C3H6/C3H8 sorption selectivity than that of the neat CMS membrane. Additional investigations with a quaternary mixture feed (C2 and C3 hydrocarbons) show that C2H4 permeability above 10 Barrers with C2H4/C2H6 permselectivity near 11 were achieved for the 3.2 wt% Fe loading case. While Fe incorporation did not appear to promote C3H6/C2H6 permselectivity, Fe is useful to improve C2 pair olefin/paraffin separation. Deconvolution of the C2H4/C2H6 permselectivity for our more extensively studied 2.2 wt% loading case was also revealing. While both sorption and diffusion selectivity increased due to the Fe incorporation, a larger influence is seen on the diffusion selectivity versus the sorption selectivity. Hypotheses to explain this surprising outcome are offered to guide future work.

Authors:
 [1];  [2];  [3];  [3];  [4];  [1]
+ Show Author Affiliations
  1. Georgia Institute of Technology, Atlanta, GA (United States)
  2. Dow Chemical Co., Midland, MI (United States)
  3. Dow Chemical Co., Freeport, TX (United States)
  4. Dow Chemical Co., Plaquemine, LA (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): Dow Chemical Company; USDOE
OSTI Identifier:
1594554
Alternate Identifier(s):
OSTI ID: 1496299
Grant/Contract Number:  
FG02-04ER15510; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Membrane Science
Additional Journal Information:
Journal Volume: 548; Journal Issue: C; Journal ID: ISSN 0376-7388
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; carbon molecular sieve; olefin/paraffin separation; iron-containing membrane

Citation Formats

Chu, Yu-Han, Yancey, David, Xu, Liren, Martinez, Marcos, Brayden, Mark, and Koros, William. Iron-containing carbon molecular sieve membranes for advanced olefin/paraffin separations. United States: N. p., 2017. Web. doi:10.1016/j.memsci.2017.11.052.
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Chu, Yu-Han, Yancey, David, Xu, Liren, Martinez, Marcos, Brayden, Mark, & Koros, William. Iron-containing carbon molecular sieve membranes for advanced olefin/paraffin separations. United States. https://doi.org/10.1016/j.memsci.2017.11.052
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Chu, Yu-Han, Yancey, David, Xu, Liren, Martinez, Marcos, Brayden, Mark, and Koros, William. Wed . "Iron-containing carbon molecular sieve membranes for advanced olefin/paraffin separations". United States. https://doi.org/10.1016/j.memsci.2017.11.052. https://www.osti.gov/servlets/purl/1594554.
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@article{osti_1594554,
title = {Iron-containing carbon molecular sieve membranes for advanced olefin/paraffin separations},
author = {Chu, Yu-Han and Yancey, David and Xu, Liren and Martinez, Marcos and Brayden, Mark and Koros, William},
abstractNote = {Here, carbon molecular sieve (CMS) dense film membranes derived from 6FDA-DAM:DABA (3:2) polyimide precursor were studied for separation of mixed olefins (C2H4 and C3H6) from paraffins (C2H6 and C3H8). Olefin-selective CMS membranes with high performance can be made by pyrolysis of metal-containing polymeric precursors. Pyrolyzed at 550 °C with a fast ramp rate, CMS membranes with integrated Fe2+ (2.2 wt% in the precursor) showed 19% higher C2H4/C2H6 and 11% higher C3H6/C3H8 sorption selectivity than that of the neat CMS membrane. Additional investigations with a quaternary mixture feed (C2 and C3 hydrocarbons) show that C2H4 permeability above 10 Barrers with C2H4/C2H6 permselectivity near 11 were achieved for the 3.2 wt% Fe loading case. While Fe incorporation did not appear to promote C3H6/C2H6 permselectivity, Fe is useful to improve C2 pair olefin/paraffin separation. Deconvolution of the C2H4/C2H6 permselectivity for our more extensively studied 2.2 wt% loading case was also revealing. While both sorption and diffusion selectivity increased due to the Fe incorporation, a larger influence is seen on the diffusion selectivity versus the sorption selectivity. Hypotheses to explain this surprising outcome are offered to guide future work.},
doi = {10.1016/j.memsci.2017.11.052},
journal = {Journal of Membrane Science},
number = C,
volume = 548,
place = {United States},
year = {Wed Nov 22 00:00:00 EST 2017},
month = {Wed Nov 22 00:00:00 EST 2017}
}
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https://doi.org/10.1016/j.memsci.2017.11.052
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    Works referencing / citing this record:

    A Review on the Progress in Nanoparticle/C Hybrid CMS Membranes for Gas Separation
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    A Bibliometric Survey of Paraffin/Olefin Separation Using Membranes
    journal, November 2019

    • Miranda, Débora Micheline Vaz de; Dutra, Luciana da Silva; Way, Débora
    • Membranes, Vol. 9, Issue 12
    • DOI: 10.3390/membranes9120157
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