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Title: Structural correlations tailor conductive properties in polymerized ionic liquids

Abstract

Polymerized ionic liquids (PolyILs) are enticing materials for applications in electrochemical devices spanning from fuel cells to capacitors and batteries. In principle, PolyILs have a competitive advantage over traditional electrolytes in being single ion conductors and thus enabling a transference number close to unity. Despite this perceived advantage, surprisingly low room temperature ionic conductivities measured in the lab raise an important fundamental question: how does the molecular structure mediate conductivity? Here, wide-angle X-ray scattering (WAXS), vibrational sum frequency generation (vSFG), and density functional theory (DFT) calculations were used to study the bulk and interfacial structure of PolyILs, while broad band dielectric spectroscopy (BDS) was used to probe corresponding dynamics and conductive properties for a series of the PolyIL samples with tunable chemistries and structures. Our results reveal that the size of the mobile anions has a tremendous impact on chain packing in PolyILs that wasn’t addressed previously. Larger mobile ions tend to create a well-packed structure, while smaller ions frustrate chain packing. The magnitude of these changes and level of structural heterogeneity are shown to depend on the chemical functionality and flexibility of studied PolyILs. Moreover, these experimental and computational results provide new insight into the correlation between conductivity andmore » structure in PolyILs, suggesting that structural heterogeneity helps to reduce the activation energy for ionic conductivity in the glassy state.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3];  [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [1]
+ Show Author Affiliations
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Université de Montpellier (France)
  3. Univ. of Tennessee, Knoxville, TN (United States)
  4. Center for Nanophase Materials Sciences; Oak Ridge National Laboratory; Oak Ridge; USA; Computational Sciences & Engineering Division
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Silesia, Chorzow (Poland)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1542209
Alternate Identifier(s):
OSTI ID: 1528657
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 21; Journal Issue: 27; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Doughty, Benjamin, Genix, Anne-Caroline, Popov, Ivan, Li, Bingrui, Zhao, Sheng, Saito, Tomonori, Lutterman, Daniel A., Sacci, Robert L., Sumpter, Bobby G., Wojnarowska, Zaneta, and Bocharova, Vera. Structural correlations tailor conductive properties in polymerized ionic liquids. United States: N. p., 2019. Web. doi:10.1039/c9cp02268f.
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Doughty, Benjamin, Genix, Anne-Caroline, Popov, Ivan, Li, Bingrui, Zhao, Sheng, Saito, Tomonori, Lutterman, Daniel A., Sacci, Robert L., Sumpter, Bobby G., Wojnarowska, Zaneta, & Bocharova, Vera. Structural correlations tailor conductive properties in polymerized ionic liquids. United States. https://doi.org/10.1039/c9cp02268f
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Doughty, Benjamin, Genix, Anne-Caroline, Popov, Ivan, Li, Bingrui, Zhao, Sheng, Saito, Tomonori, Lutterman, Daniel A., Sacci, Robert L., Sumpter, Bobby G., Wojnarowska, Zaneta, and Bocharova, Vera. Tue . "Structural correlations tailor conductive properties in polymerized ionic liquids". United States. https://doi.org/10.1039/c9cp02268f. https://www.osti.gov/servlets/purl/1542209.
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@article{osti_1542209,
title = {Structural correlations tailor conductive properties in polymerized ionic liquids},
author = {Doughty, Benjamin and Genix, Anne-Caroline and Popov, Ivan and Li, Bingrui and Zhao, Sheng and Saito, Tomonori and Lutterman, Daniel A. and Sacci, Robert L. and Sumpter, Bobby G. and Wojnarowska, Zaneta and Bocharova, Vera},
abstractNote = {Polymerized ionic liquids (PolyILs) are enticing materials for applications in electrochemical devices spanning from fuel cells to capacitors and batteries. In principle, PolyILs have a competitive advantage over traditional electrolytes in being single ion conductors and thus enabling a transference number close to unity. Despite this perceived advantage, surprisingly low room temperature ionic conductivities measured in the lab raise an important fundamental question: how does the molecular structure mediate conductivity? Here, wide-angle X-ray scattering (WAXS), vibrational sum frequency generation (vSFG), and density functional theory (DFT) calculations were used to study the bulk and interfacial structure of PolyILs, while broad band dielectric spectroscopy (BDS) was used to probe corresponding dynamics and conductive properties for a series of the PolyIL samples with tunable chemistries and structures. Our results reveal that the size of the mobile anions has a tremendous impact on chain packing in PolyILs that wasn’t addressed previously. Larger mobile ions tend to create a well-packed structure, while smaller ions frustrate chain packing. The magnitude of these changes and level of structural heterogeneity are shown to depend on the chemical functionality and flexibility of studied PolyILs. Moreover, these experimental and computational results provide new insight into the correlation between conductivity and structure in PolyILs, suggesting that structural heterogeneity helps to reduce the activation energy for ionic conductivity in the glassy state.},
doi = {10.1039/c9cp02268f},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 27,
volume = 21,
place = {United States},
year = {Tue Jan 01 00:00:00 EST 2019},
month = {Tue Jan 01 00:00:00 EST 2019}
}
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