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

The development of high performance materials for CO 2 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 (CO 2 permeability ~ 6800 Barrer and CO 2/N 2 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:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Volume: 8; Journal Issue: 21; Journal ID: ISSN 1864-5631
Publisher:
ChemPubSoc Europe
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 54 ENVIRONMENTAL SCIENCES; carbon dioxide; membranes; permeability; polymers; ring-opening metathesis polymerization
OSTI Identifier:
1224754
Alternate Identifier(s):
OSTI ID: 1266012

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., 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. 2015. "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}
}

Works referenced in this record:

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

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

The upper bound revisited
journal, July 2008