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Title: Effect of cross-link density on carbon dioxide separation in polydimethylsiloxane-norbornene membranes

Abstract

The development of high performance materials for CO2 separation and capture will significantly contribute to a solution for climate change. In this work, (bicycloheptenyl) ethyl terminated polydimethylsiloxane (PDMSPNB) membranes with varied cross-link densities were synthesized via ring-opening metathesis polymerization. The developed polymer membranes show higher permeability and better selectivity than those of conventional cross-linked PDMS membrane. The achieved performance (CO2 permeability ~ 6800 Barrer and CO2/N2 selectivity ~ 14) is very promising for practical applications. The key to achieving this high performance is the use of an in-situ cross-linking method of the difunctional PDMS macromonomers, which provides lightly cross-linked membranes. By combining positron annihilation lifetime spectroscopy, broadband dielectric spectroscopy and gas solubility measurements, we have elucidated the key parameters necessary for achieving their excellent performance.

Authors:
 [1];  [2];  [3];  [1];  [2];  [1];  [2];  [1];  [2];  [4];  [1];  [5];  [5];  [2]
  1. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  4. Univ. of California, Riverside, CA (United States). Dept. of Chemistry
  5. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1224754
Alternate Identifier(s):
OSTI ID: 1266012
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Volume: 8; Journal Issue: 21; Journal ID: ISSN 1864-5631
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 54 ENVIRONMENTAL SCIENCES; carbon dioxide; membranes; permeability; polymers; ring-opening metathesis polymerization

Citation Formats

Hong, Tao, Niu, Zhenbin, Hu, Xunxiang, Gmernicki, Kevin, Cheng, Shiwang, Fan, Fei, Johnson, Joseph Casey, Hong, Eunice K., Mahurin, Shannon Mark, Jiang, De -en, Long, Brian, Mays, Jimmy, Sokolov, Alexei, and Saito, Tomonori. Effect of cross-link density on carbon dioxide separation in polydimethylsiloxane-norbornene membranes. United States: N. p., 2015. Web. doi:10.1002/cssc.201500903.
Hong, Tao, Niu, Zhenbin, Hu, Xunxiang, Gmernicki, Kevin, Cheng, Shiwang, Fan, Fei, Johnson, Joseph Casey, Hong, Eunice K., Mahurin, Shannon Mark, Jiang, De -en, Long, Brian, Mays, Jimmy, Sokolov, Alexei, & Saito, Tomonori. Effect of cross-link density on carbon dioxide separation in polydimethylsiloxane-norbornene membranes. United States. doi:10.1002/cssc.201500903.
Hong, Tao, Niu, Zhenbin, Hu, Xunxiang, Gmernicki, Kevin, Cheng, Shiwang, Fan, Fei, Johnson, Joseph Casey, Hong, Eunice K., Mahurin, Shannon Mark, Jiang, De -en, Long, Brian, Mays, Jimmy, Sokolov, Alexei, and Saito, Tomonori. Tue . "Effect of cross-link density on carbon dioxide separation in polydimethylsiloxane-norbornene membranes". United States. doi:10.1002/cssc.201500903. https://www.osti.gov/servlets/purl/1224754.
@article{osti_1224754,
title = {Effect of cross-link density on carbon dioxide separation in polydimethylsiloxane-norbornene membranes},
author = {Hong, Tao and Niu, Zhenbin and Hu, Xunxiang and Gmernicki, Kevin and Cheng, Shiwang and Fan, Fei and Johnson, Joseph Casey and Hong, Eunice K. and Mahurin, Shannon Mark and Jiang, De -en and Long, Brian and Mays, Jimmy and Sokolov, Alexei and Saito, Tomonori},
abstractNote = {The development of high performance materials for CO2 separation and capture will significantly contribute to a solution for climate change. In this work, (bicycloheptenyl) ethyl terminated polydimethylsiloxane (PDMSPNB) membranes with varied cross-link densities were synthesized via ring-opening metathesis polymerization. The developed polymer membranes show higher permeability and better selectivity than those of conventional cross-linked PDMS membrane. The achieved performance (CO2 permeability ~ 6800 Barrer and CO2/N2 selectivity ~ 14) is very promising for practical applications. The key to achieving this high performance is the use of an in-situ cross-linking method of the difunctional PDMS macromonomers, which provides lightly cross-linked membranes. By combining positron annihilation lifetime spectroscopy, broadband dielectric spectroscopy and gas solubility measurements, we have elucidated the key parameters necessary for achieving their excellent performance.},
doi = {10.1002/cssc.201500903},
journal = {ChemSusChem},
number = 21,
volume = 8,
place = {United States},
year = {2015},
month = {10}
}

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Works referenced in this record:

Gas separation membranes from polymers of intrinsic microporosity
journal, April 2005


Positronium Annihilation in Molecular Substances
journal, June 1972

  • Tao, S. J.
  • The Journal of Chemical Physics, Vol. 56, Issue 11
  • DOI: 10.1063/1.1677067

Basis of Permeability/Selectivity Tradeoff Relations in Polymeric Gas Separation Membranes
journal, January 1999


Gas Separation, Free Volume Distribution, and Physical Aging of a Highly Microporous Spirobisindane Polymer
journal, April 2008

  • Staiger, Chad L.; Pas, Steven J.; Hill, Anita J.
  • Chemistry of Materials, Vol. 20, Issue 8
  • DOI: 10.1021/cm071722t

The Effects of Crosslinking Chemistry on CO 2 Plasticization of Polyimide Gas Separation Membranes
journal, November 2002

  • Wind, John D.; Staudt-Bickel, Claudia; Paul, Donald R.
  • Industrial & Engineering Chemistry Research, Vol. 41, Issue 24
  • DOI: 10.1021/ie0204639

The effect of crosslinking temperature on the permeability of PDMS membranes: Evidence of extraordinary CO2 and CH4 gas permeation
journal, February 2014


The Effect of Cross-Linking on Gas Permeability in Cross-Linked Poly(Ethylene Glycol Diacrylate)
journal, October 2005

  • Lin, Haiqing; Kai, Teruhiko; Freeman, Benny D.
  • Macromolecules, Vol. 38, Issue 20
  • DOI: 10.1021/ma0510136

Polymerization of [o-(trimethylgermyl)phenyl] acetylene and polymer characterization
journal, September 1993

  • Mizumoto, Tomohiro; Masuda, Toshio; Higashimura, Toshinobu
  • Journal of Polymer Science Part A: Polymer Chemistry, Vol. 31, Issue 10
  • DOI: 10.1002/pola.1993.080311016

Poly[1-(trimethylsilyl)-1-propyne] and related polymers: synthesis, properties and functions
journal, June 2001


Gas sorption, diffusion, and permeation in poly(dimethylsiloxane)
journal, February 2000


The temperature dependence of positron lifetimes in solid pivalic acid
journal, December 1981


Gas separation using polymer membranes: an overview
journal, November 1994


Power plant post-combustion carbon dioxide capture: An opportunity for membranes
journal, September 2010

  • Merkel, Tim C.; Lin, Haiqing; Wei, Xiaotong
  • Journal of Membrane Science, Vol. 359, Issue 1-2, p. 126-139
  • DOI: 10.1016/j.memsci.2009.10.041

Effects of cross-linking modification on gas separation performance of Matrimid membranes
journal, November 2003


Effect of PDMS cross-linking degree on the permeation performance of PAN/PDMS composite nanofiltration membranes
journal, October 2005


Correlation of separation factor versus permeability for polymeric membranes
journal, October 1991


Structure-permeability relationships in silicone polymers
journal, June 1987

  • Stern, S. A.; Shah, V. M.; Hardy, B. J.
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 25, Issue 6
  • DOI: 10.1002/polb.1987.090250607

Performance of nitrile-containing anions in task-specific ionic liquids for improved CO2/N2 separation
journal, May 2010


Irreversible climate change due to carbon dioxide emissions
journal, January 2009

  • Solomon, Susan; Plattner, Gian-Kasper; Knutti, Reto
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 6
  • DOI: 10.1073/pnas.0812721106

The upper bound revisited
journal, July 2008


The study of defects in crystals by positron annihilation
journal, August 1974