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Title: Revealing the Charge Transport Mechanism in Polymerized Ionic Liquids: Insight from High Pressure Conductivity Studies

Abstract

Polymerized ionic liquids (polyILs), composed mostly of organic ions covalently bonded to the polymer backbone and free counterions, are considered as an ideal electrolytes for various electrochemical devices, including fuel cells, supercapacitors and batteries. Despite large structural diversity of these systems, all of them reveal a universal but poorly understood feature - a charge transport faster than the segmental dynamics. Here, to address this issue, we have studied three novel polymer electrolyte membrane for fuel cells as well as four single-ion conductors including highly conductive siloxane-based polyIL. Our ambient and high pressure studies revealed fundamental differences in the conducting properties of the examined systems. Finally, we demonstrate that the proposed methodology is a powerful tool to identify the charge transport mechanism in polyILs in general and thereby contribute to unraveling the microscopic nature of the decoupling phenomenon in these materials.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [3];  [3]; ORCiD logo [4];  [5];  [5]; ORCiD logo [5]; ORCiD logo [6];  [7]; ORCiD logo [2];  [8];  [9];  [10]; ORCiD logo [11]; ORCiD logo [6];  [4]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Silesia, Katowice (Poland). Inst. of Physics; Silesian Center for Education and Interdisciplinary Research, Chorzow (Poland)
  2. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
  3. Univ. of Cantabria, Santander (Spain). Chemical and Biomolecular Engineering Dept.
  4. Univ. of Silesia, Katowice (Poland). Inst. of Physics; Silesian Center for Education and Interdisciplinary Research, Chorzow (Poland)
  5. Univ. of Vigo, Marcosende, Vigo (Spain). Organic Chemistry Dept.
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  7. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy
  8. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
  9. Univ. of Warmia and Mazury, Olsztyn (Poland). Faculty of Mathematics and Computer Science
  10. Inst. of Non-Ferrous Metals, Gliwice (Poland)
  11. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1408578
Grant/Contract Number:  
[AC05-00OR22725; DEC-2014/15/B/ST3/04246]
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
[ Journal Volume: 29; Journal Issue: 19]; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Wojnarowska, Zaneta, Feng, Hongbo, Diaz, Mariana, Ortiz, Alfredo, Ortiz, Inmaculada, Knapik-Kowalczuk, Justyna, Vilas, Miguel, Verdía, Pedro, Tojo, Emilia, Saito, Tomonori, Stacy, Eric W., Kang, Nam-Goo, Mays, Jimmy W., Kruk, Danuta, Wlodarczyk, Patryk, Sokolov, Alexei P., Bocharova, Vera, and Paluch, Marian. Revealing the Charge Transport Mechanism in Polymerized Ionic Liquids: Insight from High Pressure Conductivity Studies. United States: N. p., 2017. Web. doi:10.1021/acs.chemmater.7b01658.
Wojnarowska, Zaneta, Feng, Hongbo, Diaz, Mariana, Ortiz, Alfredo, Ortiz, Inmaculada, Knapik-Kowalczuk, Justyna, Vilas, Miguel, Verdía, Pedro, Tojo, Emilia, Saito, Tomonori, Stacy, Eric W., Kang, Nam-Goo, Mays, Jimmy W., Kruk, Danuta, Wlodarczyk, Patryk, Sokolov, Alexei P., Bocharova, Vera, & Paluch, Marian. Revealing the Charge Transport Mechanism in Polymerized Ionic Liquids: Insight from High Pressure Conductivity Studies. United States. doi:10.1021/acs.chemmater.7b01658.
Wojnarowska, Zaneta, Feng, Hongbo, Diaz, Mariana, Ortiz, Alfredo, Ortiz, Inmaculada, Knapik-Kowalczuk, Justyna, Vilas, Miguel, Verdía, Pedro, Tojo, Emilia, Saito, Tomonori, Stacy, Eric W., Kang, Nam-Goo, Mays, Jimmy W., Kruk, Danuta, Wlodarczyk, Patryk, Sokolov, Alexei P., Bocharova, Vera, and Paluch, Marian. Tue . "Revealing the Charge Transport Mechanism in Polymerized Ionic Liquids: Insight from High Pressure Conductivity Studies". United States. doi:10.1021/acs.chemmater.7b01658. https://www.osti.gov/servlets/purl/1408578.
@article{osti_1408578,
title = {Revealing the Charge Transport Mechanism in Polymerized Ionic Liquids: Insight from High Pressure Conductivity Studies},
author = {Wojnarowska, Zaneta and Feng, Hongbo and Diaz, Mariana and Ortiz, Alfredo and Ortiz, Inmaculada and Knapik-Kowalczuk, Justyna and Vilas, Miguel and Verdía, Pedro and Tojo, Emilia and Saito, Tomonori and Stacy, Eric W. and Kang, Nam-Goo and Mays, Jimmy W. and Kruk, Danuta and Wlodarczyk, Patryk and Sokolov, Alexei P. and Bocharova, Vera and Paluch, Marian},
abstractNote = {Polymerized ionic liquids (polyILs), composed mostly of organic ions covalently bonded to the polymer backbone and free counterions, are considered as an ideal electrolytes for various electrochemical devices, including fuel cells, supercapacitors and batteries. Despite large structural diversity of these systems, all of them reveal a universal but poorly understood feature - a charge transport faster than the segmental dynamics. Here, to address this issue, we have studied three novel polymer electrolyte membrane for fuel cells as well as four single-ion conductors including highly conductive siloxane-based polyIL. Our ambient and high pressure studies revealed fundamental differences in the conducting properties of the examined systems. Finally, we demonstrate that the proposed methodology is a powerful tool to identify the charge transport mechanism in polyILs in general and thereby contribute to unraveling the microscopic nature of the decoupling phenomenon in these materials.},
doi = {10.1021/acs.chemmater.7b01658},
journal = {Chemistry of Materials},
number = [19],
volume = [29],
place = {United States},
year = {2017},
month = {9}
}

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