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Title: Self-assembled highly ordered acid layers in precisely sulfonated polyethylene produce efficient proton transport

Abstract

Recent advances in polymer synthesis have allowed remarkable control over chain microstructure and conformation. Capitalizing on such developments, we create well-controlled chain folding in sulfonated polyethylene, leading to highly uniform hydrated acid layers of sub-nanometer thickness with high proton conductivity. The linear polyethylene contains sulfonic acid groups pendant to precisely every 21st carbon atom that induce tight chain folds to form the hydrated layers, while the methylene segments crystallize. The proton conductivity is on par with Nafion® 117, the benchmark for fuel cell membranes. This is the first time that well-controlled hairpin chain folding has been utilized for proton or ion transport, and the first report of high proton conductivity within a crystalline polymer structure. This layered polyethylene-based structure is an innovative and versatile design paradigm for functional polymer membranes, opening doors to efficient and selective transport of other ions and small molecules upon appropriate selection of functional groups.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [1]; ORCiD logo [3];  [2];  [4]; ORCiD logo [1]
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  1. Pennsylvania State Univ., University Park, PA (United States)
  2. Univ. of Florida, Gainesville, FL (United States)
  3. Univ. Grenoble Alpes (France)
  4. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1473945
Report Number(s):
SAND-2018-9831J
Journal ID: ISSN 1476-1122; 667683
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 17; Journal Issue: 8; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Trigg, Edward B., Gaines, Taylor W., Maréchal, Manuel, Moed, Demi E., Rannou, Patrice, Wagener, Kenneth B., Stevens, Mark J., and Winey, Karen I. Self-assembled highly ordered acid layers in precisely sulfonated polyethylene produce efficient proton transport. United States: N. p., 2018. Web. doi:10.1038/s41563-018-0097-2.
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Trigg, Edward B., Gaines, Taylor W., Maréchal, Manuel, Moed, Demi E., Rannou, Patrice, Wagener, Kenneth B., Stevens, Mark J., & Winey, Karen I. Self-assembled highly ordered acid layers in precisely sulfonated polyethylene produce efficient proton transport. United States. https://doi.org/10.1038/s41563-018-0097-2
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Trigg, Edward B., Gaines, Taylor W., Maréchal, Manuel, Moed, Demi E., Rannou, Patrice, Wagener, Kenneth B., Stevens, Mark J., and Winey, Karen I. Mon . "Self-assembled highly ordered acid layers in precisely sulfonated polyethylene produce efficient proton transport". United States. https://doi.org/10.1038/s41563-018-0097-2. https://www.osti.gov/servlets/purl/1473945.
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@article{osti_1473945,
title = {Self-assembled highly ordered acid layers in precisely sulfonated polyethylene produce efficient proton transport},
author = {Trigg, Edward B. and Gaines, Taylor W. and Maréchal, Manuel and Moed, Demi E. and Rannou, Patrice and Wagener, Kenneth B. and Stevens, Mark J. and Winey, Karen I.},
abstractNote = {Recent advances in polymer synthesis have allowed remarkable control over chain microstructure and conformation. Capitalizing on such developments, we create well-controlled chain folding in sulfonated polyethylene, leading to highly uniform hydrated acid layers of sub-nanometer thickness with high proton conductivity. The linear polyethylene contains sulfonic acid groups pendant to precisely every 21st carbon atom that induce tight chain folds to form the hydrated layers, while the methylene segments crystallize. The proton conductivity is on par with Nafion® 117, the benchmark for fuel cell membranes. This is the first time that well-controlled hairpin chain folding has been utilized for proton or ion transport, and the first report of high proton conductivity within a crystalline polymer structure. This layered polyethylene-based structure is an innovative and versatile design paradigm for functional polymer membranes, opening doors to efficient and selective transport of other ions and small molecules upon appropriate selection of functional groups.},
doi = {10.1038/s41563-018-0097-2},
journal = {Nature Materials},
number = 8,
volume = 17,
place = {United States},
year = {Mon May 28 00:00:00 EDT 2018},
month = {Mon May 28 00:00:00 EDT 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1038/s41563-018-0097-2
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Cited by: 161 works
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Figures / Tables:

Figure 1 Figure 1: (a) DC conductivity of p21SA and Nafion® 117 via electrochemical impedance spectroscopy (EIS) as a function of relative humidity (RH) at 40°C. (b) Chemical structure and schematic rendering of the secondary structure of hydrated p21SA, showing the crystalline backbones and acid-lined water layers. (c) Water uptake, $λ$, ofmore » p21SA and Nafion® 117 as a function of RH at 40°C. $λ$ is defined as the number of water molecules per sulfonic group and is measured with a sorption balance. (d) EIS Nyquist and (e) Bode plots of the complex impedance (Z) of p21SA at 30% and 70% RH. For low humidities, part or all of the semicircle was evident in the EIS Nyquist plot, while at higher humidities, the proton conductivity time scale was faster than the maximum frequency of our impedance spectrometer (1 MHz). At all humidities, a minimum in Im(Z) was evident in the Bode plot. The DC resistance was obtained from the value of Re(Z) at the frequency of minimum Im(Z). (f) Photo of p21SA sample connected to stainless steel electrodes for EIS measurements. The electrodes were connected laterally across the film, rather than in a sandwich-like manner, to maximally expose the sample to the air for improved equilibration upon changing humidity.« less
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