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Title: Gas separation mechanism of CO 2 selective amidoxime-poly(1-trimethylsilyl-1-propyne) membranes

Polymeric membranes for CO 2 separation have drawn significant attention in academia and industry. We prepared amidoxime-functionalized poly(1-trimethylsilyl-1-propyne) (AO-PTMSP) membranes through hydrosilylation and post-polymerization modification. Compared to neat PTMSP membranes, the AO-PTMSP membranes showed significant enhancements in CO 2/N 2 gas separation performance (CO 2 permeability ~6000 Barrer; CO 2/N 2 selectivity 17). This systematic study provides clear guidelines on how to tune the CO 2-philicity within PTMSP matrices and the effects on gas selectivity. Key parameters for elucidating the gas transport mechanism were discussed based on CO 2 sorption measurements and fractional free volume estimates. The effect of the AO content on CO 2/N 2 selectivity was further examined by means of density functional theory calculations. Here, both experimental and theoretical data provide consistent results that conclusively show that CO 2/N 2 separation performance is enhanced by increased CO 2 polymer interactions.
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1] ;  [3] ;  [1] ;  [3] ;  [1] ;  [2]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Polymer Chemistry
Additional Journal Information:
Journal Volume: 8; Journal Issue: 21; Journal ID: ISSN 1759-9954
Publisher:
Royal Society of Chemistry
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC); USDOE Office of Fossil Energy (FE)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1361374

Feng, Hongbo, Hong, Tao, Mahurin, Shannon Mark, Vogiatzis, Konstantinos D., Gmernicki, Kevin R., Long, Brian K., Mays, Jimmy W., Oak Ridge National Lab., Sokolov, Alexei P., Oak Ridge National Lab., Kang, Nam -Goo, and Saito, Tomonori. Gas separation mechanism of CO2 selective amidoxime-poly(1-trimethylsilyl-1-propyne) membranes. United States: N. p., Web. doi:10.1039/C7PY00056A.
Feng, Hongbo, Hong, Tao, Mahurin, Shannon Mark, Vogiatzis, Konstantinos D., Gmernicki, Kevin R., Long, Brian K., Mays, Jimmy W., Oak Ridge National Lab., Sokolov, Alexei P., Oak Ridge National Lab., Kang, Nam -Goo, & Saito, Tomonori. Gas separation mechanism of CO2 selective amidoxime-poly(1-trimethylsilyl-1-propyne) membranes. United States. doi:10.1039/C7PY00056A.
Feng, Hongbo, Hong, Tao, Mahurin, Shannon Mark, Vogiatzis, Konstantinos D., Gmernicki, Kevin R., Long, Brian K., Mays, Jimmy W., Oak Ridge National Lab., Sokolov, Alexei P., Oak Ridge National Lab., Kang, Nam -Goo, and Saito, Tomonori. 2017. "Gas separation mechanism of CO2 selective amidoxime-poly(1-trimethylsilyl-1-propyne) membranes". United States. doi:10.1039/C7PY00056A. https://www.osti.gov/servlets/purl/1361374.
@article{osti_1361374,
title = {Gas separation mechanism of CO2 selective amidoxime-poly(1-trimethylsilyl-1-propyne) membranes},
author = {Feng, Hongbo and Hong, Tao and Mahurin, Shannon Mark and Vogiatzis, Konstantinos D. and Gmernicki, Kevin R. and Long, Brian K. and Mays, Jimmy W. and Oak Ridge National Lab. and Sokolov, Alexei P. and Oak Ridge National Lab. and Kang, Nam -Goo and Saito, Tomonori},
abstractNote = {Polymeric membranes for CO2 separation have drawn significant attention in academia and industry. We prepared amidoxime-functionalized poly(1-trimethylsilyl-1-propyne) (AO-PTMSP) membranes through hydrosilylation and post-polymerization modification. Compared to neat PTMSP membranes, the AO-PTMSP membranes showed significant enhancements in CO2/N2 gas separation performance (CO2 permeability ~6000 Barrer; CO2/N2 selectivity 17). This systematic study provides clear guidelines on how to tune the CO2-philicity within PTMSP matrices and the effects on gas selectivity. Key parameters for elucidating the gas transport mechanism were discussed based on CO2 sorption measurements and fractional free volume estimates. The effect of the AO content on CO2/N2 selectivity was further examined by means of density functional theory calculations. Here, both experimental and theoretical data provide consistent results that conclusively show that CO2/N2 separation performance is enhanced by increased CO2 polymer interactions.},
doi = {10.1039/C7PY00056A},
journal = {Polymer Chemistry},
number = 21,
volume = 8,
place = {United States},
year = {2017},
month = {5}
}

Works referenced in this record:

Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: Design and assessment of accuracy
journal, January 2005
  • Weigend, Florian; Ahlrichs, Reinhart
  • Physical Chemistry Chemical Physics, Vol. 7, Issue 18, p. 3297-3305
  • DOI: 10.1039/b508541a

Polymer nanosieve membranes for CO2-capture applications
journal, April 2011
  • Du, Naiying; Park, Ho Bum; Robertson, Gilles P.
  • Nature Materials, Vol. 10, Issue 5, p. 372-375
  • DOI: 10.1038/nmat2989

van der Waals Volumes and Radii
journal, March 1964
  • Bondi, A.
  • The Journal of Physical Chemistry, Vol. 68, Issue 3, p. 441-451
  • DOI: 10.1021/j100785a001

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