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Title: Tailored CO 2 -philic Gas Separation Membranes via One-Pot Thiol–ene Chemistry

Abstract

Recently, thiol–ene chemistry attracts much attention in the construction of functional polymer materials due to its versatility and fast reaction kinetics, though only a few studies have been reported on its utilization in the fabrication of elastic polymer materials. Herein, a series of elastic, poly(dimethylsiloxane)–poly(ethylene glycol) methyl ether acrylate (PDMS–PEGMEA)-based co-polymer membranes are synthesized via a one-pot thiol–ene reaction. These membranes are highly stable and exhibit tunable thermal/mechanical properties by tailoring the cross-linker and side-chain functionality. When used for gas separation application, all grafted elastomer membranes show excellent gas permeability and selectivity, and the membrane with an optimal composition (PDMS–PEGMEA 30–EOPDMS 10) has reached the Robeson upper bound (CO 2 permeability ~800 barrer and α[CO 2/N 2] ~39). The high permeability originates from the extremely fast chain mobility of PDMS molecules at the ambient temperature. Tailoring the PEGMEA content allows control of the α[CO 2/N 2] ranging from 21 to 39 by enhancing gas solubility within the membrane matrix. This study provides a promising strategy to be utilized for the gutter layer, selective layer, or their combination in the industrial gas separation modules.

Authors:
 [1]; ORCiD logo [2];  [3]; ORCiD logo [2];  [2]; ORCiD logo [2];  [4]; ORCiD logo [2]; ORCiD logo [5]; ORCiD logo [2]; ORCiD logo [6]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Georgia Inst. of Technology, Atlanta, GA (United States)
  5. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1564181
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Macromolecules
Additional Journal Information:
Journal Volume: 52; Journal Issue: 15; Journal ID: ISSN 0024-9297
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Graft Copolymer; Elastic Polymer Membrane; Poly(dimethylsiloxane); Thiol-ene; Gas Separation

Citation Formats

Hong, Tao, Cao, Peng-Fei, Zhao, Sheng, Li, Bingrui, Smith, Connor, Lehmann, Michelle, Erwin, Andrew J., Mahurin, Shannon M., Venna, Surendar R., Sokolov, Alexei P., and Saito, Tomonori. Tailored CO2 -philic Gas Separation Membranes via One-Pot Thiol–ene Chemistry. United States: N. p., 2019. Web. doi:10.1021/acs.macromol.9b00497.
Hong, Tao, Cao, Peng-Fei, Zhao, Sheng, Li, Bingrui, Smith, Connor, Lehmann, Michelle, Erwin, Andrew J., Mahurin, Shannon M., Venna, Surendar R., Sokolov, Alexei P., & Saito, Tomonori. Tailored CO2 -philic Gas Separation Membranes via One-Pot Thiol–ene Chemistry. United States. doi:10.1021/acs.macromol.9b00497.
Hong, Tao, Cao, Peng-Fei, Zhao, Sheng, Li, Bingrui, Smith, Connor, Lehmann, Michelle, Erwin, Andrew J., Mahurin, Shannon M., Venna, Surendar R., Sokolov, Alexei P., and Saito, Tomonori. Wed . "Tailored CO2 -philic Gas Separation Membranes via One-Pot Thiol–ene Chemistry". United States. doi:10.1021/acs.macromol.9b00497. https://www.osti.gov/servlets/purl/1564181.
@article{osti_1564181,
title = {Tailored CO2 -philic Gas Separation Membranes via One-Pot Thiol–ene Chemistry},
author = {Hong, Tao and Cao, Peng-Fei and Zhao, Sheng and Li, Bingrui and Smith, Connor and Lehmann, Michelle and Erwin, Andrew J. and Mahurin, Shannon M. and Venna, Surendar R. and Sokolov, Alexei P. and Saito, Tomonori},
abstractNote = {Recently, thiol–ene chemistry attracts much attention in the construction of functional polymer materials due to its versatility and fast reaction kinetics, though only a few studies have been reported on its utilization in the fabrication of elastic polymer materials. Herein, a series of elastic, poly(dimethylsiloxane)–poly(ethylene glycol) methyl ether acrylate (PDMS–PEGMEA)-based co-polymer membranes are synthesized via a one-pot thiol–ene reaction. These membranes are highly stable and exhibit tunable thermal/mechanical properties by tailoring the cross-linker and side-chain functionality. When used for gas separation application, all grafted elastomer membranes show excellent gas permeability and selectivity, and the membrane with an optimal composition (PDMS–PEGMEA30–EOPDMS10) has reached the Robeson upper bound (CO2 permeability ~800 barrer and α[CO2/N2] ~39). The high permeability originates from the extremely fast chain mobility of PDMS molecules at the ambient temperature. Tailoring the PEGMEA content allows control of the α[CO2/N2] ranging from 21 to 39 by enhancing gas solubility within the membrane matrix. This study provides a promising strategy to be utilized for the gutter layer, selective layer, or their combination in the industrial gas separation modules.},
doi = {10.1021/acs.macromol.9b00497},
journal = {Macromolecules},
issn = {0024-9297},
number = 15,
volume = 52,
place = {United States},
year = {2019},
month = {7}
}

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