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Title: Impact of Hydration and Sulfonation on the Morphology and Ionic Conductivity of Sulfonated Poly(phenylene) Proton Exchange Membranes

Abstract

Multiple computational and experimental techniques are used here to understand the nanoscale morphology and water/proton transport properties in a series of sulfonated Diels–Alder poly(phenylene) (SDAPP) membranes over a wide range of temperature, hydration, and sulfonation conditions. New synthetic methods allow us to sulfonate the SDAPP membranes to much higher ion exchange capacity levels than has been previously possible. Nanoscale phase separation between the hydrophobic polymer backbone and the hydrophilic water/sulfonic acid groups was observed for all membranes studied. We find good agreement between structure factors calculated from atomistic molecular dynamics (MD) simulations and those measured by X-ray scattering. With increasing hydration, the scattering ionomer peak in SDAPP is found to decrease in intensity. This intensity decrease is shown to be due to a reduction of scattering contrast between the water and polymer and is not indicative of any loss of nanoscale phase separation. Both MD simulations and density functional theory (DFT) calculations show that as hydration levels are increased, the nanostructure morphology in SDAPP evolves from isolated ionic domains to fully percolated water networks containing progressively weaker hydrogen bond strengths. The conductivity of the membranes is measured by electrical impedance spectroscopy and the equivalent proton conductivity calculated from pulsed-field-gradient (PFG)more » NMR diffusometry measurements of the hydration waters. Comparison of the measured and calculated conductivity reveals that in SDAPP the proton conduction mechanism evolves from being dominated by vehicular transport at low hydration and sulfonation levels to including a significant contribution from the Grötthuss mechanism (also known as structural diffusion) at higher hydration and sulfonation levels. The observed increase in conductivity reflects the impact that changing hydration and sulfonation have on the morphology and hydrogen bond network and ultimately on the membrane performance.« less

Authors:
 [1];  [2];  [3];  [4];  [1];  [5];  [3];  [2];  [5];  [1]
+ Show Author Affiliations
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Dept. of Organic Materials Science
  2. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Materials Science and Engineering
  3. Univ. of Texas, Austin, TX (United States). McKetta Dept. of Chemical Engineering
  4. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Nanoscale Sciences Dept.
  5. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Univ. of Pennsylvania, Philadelphia, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); USDOE National Nuclear Security Administration (NNSA); SNL Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)
OSTI Identifier:
1492390
Report Number(s):
SAND-2018-9649J
Journal ID: ISSN 0024-9297; 667559
Grant/Contract Number:  
NA0003525; 1720530; 1545884
Resource Type:
Accepted Manuscript
Journal Name:
Macromolecules
Additional Journal Information:
Journal Volume: 52; Journal Issue: 3; Journal ID: ISSN 0024-9297
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sorte, Eric G., Paren, Benjamin A., Rodriguez, Christina G., Fujimoto, Cy, Poirier, Cassandria, Abbott, Lauren J., Lynd, Nathaniel A., Winey, Karen I., Frischknecht, Amalie L., and Alam, Todd M. Impact of Hydration and Sulfonation on the Morphology and Ionic Conductivity of Sulfonated Poly(phenylene) Proton Exchange Membranes. United States: N. p., 2019. Web. doi:10.1021/acs.macromol.8b02013.
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Sorte, Eric G., Paren, Benjamin A., Rodriguez, Christina G., Fujimoto, Cy, Poirier, Cassandria, Abbott, Lauren J., Lynd, Nathaniel A., Winey, Karen I., Frischknecht, Amalie L., & Alam, Todd M. Impact of Hydration and Sulfonation on the Morphology and Ionic Conductivity of Sulfonated Poly(phenylene) Proton Exchange Membranes. United States. https://doi.org/10.1021/acs.macromol.8b02013
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Sorte, Eric G., Paren, Benjamin A., Rodriguez, Christina G., Fujimoto, Cy, Poirier, Cassandria, Abbott, Lauren J., Lynd, Nathaniel A., Winey, Karen I., Frischknecht, Amalie L., and Alam, Todd M. Tue . "Impact of Hydration and Sulfonation on the Morphology and Ionic Conductivity of Sulfonated Poly(phenylene) Proton Exchange Membranes". United States. https://doi.org/10.1021/acs.macromol.8b02013. https://www.osti.gov/servlets/purl/1492390.
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@article{osti_1492390,
title = {Impact of Hydration and Sulfonation on the Morphology and Ionic Conductivity of Sulfonated Poly(phenylene) Proton Exchange Membranes},
author = {Sorte, Eric G. and Paren, Benjamin A. and Rodriguez, Christina G. and Fujimoto, Cy and Poirier, Cassandria and Abbott, Lauren J. and Lynd, Nathaniel A. and Winey, Karen I. and Frischknecht, Amalie L. and Alam, Todd M.},
abstractNote = {Multiple computational and experimental techniques are used here to understand the nanoscale morphology and water/proton transport properties in a series of sulfonated Diels–Alder poly(phenylene) (SDAPP) membranes over a wide range of temperature, hydration, and sulfonation conditions. New synthetic methods allow us to sulfonate the SDAPP membranes to much higher ion exchange capacity levels than has been previously possible. Nanoscale phase separation between the hydrophobic polymer backbone and the hydrophilic water/sulfonic acid groups was observed for all membranes studied. We find good agreement between structure factors calculated from atomistic molecular dynamics (MD) simulations and those measured by X-ray scattering. With increasing hydration, the scattering ionomer peak in SDAPP is found to decrease in intensity. This intensity decrease is shown to be due to a reduction of scattering contrast between the water and polymer and is not indicative of any loss of nanoscale phase separation. Both MD simulations and density functional theory (DFT) calculations show that as hydration levels are increased, the nanostructure morphology in SDAPP evolves from isolated ionic domains to fully percolated water networks containing progressively weaker hydrogen bond strengths. The conductivity of the membranes is measured by electrical impedance spectroscopy and the equivalent proton conductivity calculated from pulsed-field-gradient (PFG) NMR diffusometry measurements of the hydration waters. Comparison of the measured and calculated conductivity reveals that in SDAPP the proton conduction mechanism evolves from being dominated by vehicular transport at low hydration and sulfonation levels to including a significant contribution from the Grötthuss mechanism (also known as structural diffusion) at higher hydration and sulfonation levels. The observed increase in conductivity reflects the impact that changing hydration and sulfonation have on the morphology and hydrogen bond network and ultimately on the membrane performance.},
doi = {10.1021/acs.macromol.8b02013},
journal = {Macromolecules},
number = 3,
volume = 52,
place = {United States},
year = {Tue Jan 15 00:00:00 EST 2019},
month = {Tue Jan 15 00:00:00 EST 2019}
}
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https://doi.org/10.1021/acs.macromol.8b02013
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