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:
-
[1];
[2];
[4];
[5];
[6];
[2];
[11];
[6];
- 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)
- Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
- Univ. of Cantabria, Santander (Spain). Chemical and Biomolecular Engineering Dept.
- Univ. of Silesia, Katowice (Poland). Inst. of Physics; Silesian Center for Education and Interdisciplinary Research, Chorzow (Poland)
- Univ. of Vigo, Marcosende, Vigo (Spain). Organic Chemistry Dept.
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
- Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
- Univ. of Warmia and Mazury, Olsztyn (Poland). Faculty of Mathematics and Computer Science
- Inst. of Non-Ferrous Metals, Gliwice (Poland)
- 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 Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- 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. https://doi.org/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. https://doi.org/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 = {Tue Sep 05 00:00:00 EDT 2017},
month = {Tue Sep 05 00:00:00 EDT 2017}
}
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Works referenced in this record:
Ionic-liquid materials for the electrochemical challenges of the future
journal, July 2009
- Armand, Michel; Endres, Frank; MacFarlane, Douglas R.
- Nature Materials, Vol. 8, Issue 8, p. 621-629
Solvent-Free Electrolytes with Aqueous Solution-Like Conductivities
journal, October 2003
- Xu, W.
- Science, Vol. 302, Issue 5644
Ionic liquids and their solid-state analogues as materials for energy generation and storage
journal, January 2016
- MacFarlane, Douglas R.; Forsyth, Maria; Howlett, Patrick C.
- Nature Reviews Materials, Vol. 1, Issue 2
Charge Transport and Glassy Dynamics in Ionic Liquids
journal, November 2011
- Sangoro, Joshua R.; Kremer, Friedrich
- Accounts of Chemical Research, Vol. 45, Issue 4
Dielectric and Viscoelastic Responses of Imidazolium-Based Ionomers with Different Counterions and Side Chain Lengths
journal, January 2014
- Choi, U. Hyeok; Ye, Yuesheng; Salas de la Cruz, David
- Macromolecules, Vol. 47, Issue 2
Dielectric relaxation behavior of polymerized ionic liquids with various charge densities
journal, June 2013
- Nakamura, Kenji; Fukao, Koji
- Polymer, Vol. 54, Issue 13
Decoupling of ionic conductivity from structural dynamics in polymerized ionic liquids
journal, January 2014
- Sangoro, J. R.; Iacob, C.; Agapov, A. L.
- Soft Matter, Vol. 10, Issue 20
Molecular Volume Effects on the Dynamics of Polymerized Ionic Liquids and their Monomers
journal, September 2015
- Choi, U. Hyeok; Mittal, Anuj; Price, Terry L.
- Electrochimica Acta, Vol. 175
Molecular Dynamics and Charge Transport in Polymeric Polyisobutylene-Based Ionic Liquids
journal, March 2016
- Frenzel, Falk; Folikumah, Makafui Y.; Schulz, Matthias
- Macromolecules, Vol. 49, Issue 7
Effect of Molecular Weight on the Ion Transport Mechanism in Polymerized Ionic Liquids
journal, June 2016
- Fan, Fei; Wang, Weiyu; Holt, Adam P.
- Macromolecules, Vol. 49, Issue 12
Ion Conduction in Polymerized Ionic Liquids with Different Pendant Groups
journal, June 2015
- Fan, Fei; Wang, Yangyang; Hong, Tao
- Macromolecules, Vol. 48, Issue 13
Highly decoupled ionic and protonic solid electrolyte systems, in relation to other relaxing systems and their energy landscapes
journal, November 2006
- Mizuno, F.; Belieres, J. -P.; Kuwata, N.
- Journal of Non-Crystalline Solids, Vol. 352, Issue 42-49
Dynamic processes in ionic glasses
journal, May 1990
- Angell, C. Austin
- Chemical Reviews, Vol. 90, Issue 3
Ionic conductivity and glass structure
journal, December 1989
- Ingram, Malcolm D.
- Philosophical Magazine B, Vol. 60, Issue 6
Progress in the use of ionic liquids as electrolyte membranes in fuel cells
journal, November 2014
- Díaz, Mariana; Ortiz, Alfredo; Ortiz, Inmaculada
- Journal of Membrane Science, Vol. 469
Conductivity Mechanism in Polymerized Imidazolium-Based Protic Ionic Liquid [HSO 3 –BVIm][OTf]: Dielectric Relaxation Studies
journal, June 2014
- Wojnarowska, Z.; Knapik, J.; Díaz, M.
- Macromolecules, Vol. 47, Issue 12
Enhanced proton transport in nanostructured polymer electrolyte/ionic liquid membranes under water-free conditions
journal, October 2010
- Kim, Sung Yeon; Kim, Suhan; Park, Moon Jeong
- Nature Communications, Vol. 1, Issue 1
Charge transport in poly-imidazole membranes: a fresh appraisal of the Grotthuss mechanism
journal, January 2012
- Mangiatordi, Giuseppe Felice; Butera, Valeria; Russo, Nino
- Physical Chemistry Chemical Physics, Vol. 14, Issue 31
Molecular Origin of Enhanced Proton Conductivity in Anhydrous Ionic Systems
journal, January 2015
- Wojnarowska, Zaneta; Paluch, Krzysztof J.; Shoifet, Evgeni
- Journal of the American Chemical Society, Vol. 137, Issue 3
Charge-transport model for conducting polymers
journal, November 2016
- Kang, Stephen Dongmin; Snyder, G. Jeffrey
- Nature Materials, Vol. 16, Issue 2
Effect of Pressure on Decoupling of Ionic Conductivity from Segmental Dynamics in Polymerized Ionic Liquids
journal, November 2015
- Wojnarowska, Z.; Knapik, J.; Jacquemin, J.
- Macromolecules, Vol. 48, Issue 23
Effect of Chain Rigidity on the Decoupling of Ion Motion from Segmental Relaxation in Polymerized Ionic Liquids: Ambient and Elevated Pressure Studies
journal, August 2017
- Wojnarowska, Zaneta; Feng, Hongbo; Fu, Yao
- Macromolecules, Vol. 50, Issue 17
Intramolecular hydroalkoxylation in Brønsted acidic ionic liquids and its application to the synthesis of (±)-centrolobine
journal, January 2011
- Jeong, Yunkyung; Kim, Do-Young; Choi, Yunsil
- Org. Biomol. Chem., Vol. 9, Issue 2
One-pot conversion of carbohydrates into gamma-valerolactone catalyzed by highly cross-linked ionic liquid polymer and Co/TiO 2
journal, January 2015
- Zhou, Huacong; Song, Jinliang; Kang, Xinchen
- RSC Advances, Vol. 5, Issue 20
The ORCA program system: The ORCA program system
journal, June 2011
- Neese, Frank
- Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 1
Fundamental questions relating to ion conduction in disordered solids
journal, March 2009
- Dyre, Jeppe C.; Maass, Philipp; Roling, Bernhard
- Reports on Progress in Physics, Vol. 72, Issue 4
Anomalous Electrical Conductivity Behavior at Elevated Pressure in the Protic Ionic Liquid Procainamide Hydrochloride
journal, January 2012
- Wojnarowska, Z.; Roland, C. M.; Swiety-Pospiech, A.
- Physical Review Letters, Vol. 108, Issue 1
Recent progress on dielectric properties of protic ionic liquids
journal, January 2015
- Wojnarowska, Zaneta; Paluch, Marian
- Journal of Physics: Condensed Matter, Vol. 27, Issue 7
Comments on the electric modulus function
journal, January 2005
- Hodge, I. M.; Ngai, K. L.; Moynihan, C. T.
- Journal of Non-Crystalline Solids, Vol. 351, Issue 2
Role of hydrogen bonds in the supercooled dynamics of glass-forming liquids at high pressures
journal, January 2008
- Roland, C. M.; Casalini, R.; Bergman, R.
- Physical Review B, Vol. 77, Issue 1
Experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former
journal, August 2017
- Wojnarowska, Z.; Rams-Baron, M.; Knapik-Kowalczuk, J.
- Scientific Reports, Vol. 7, Issue 1
High pressure study of molecular dynamics of protic ionic liquid lidocaine hydrochloride
journal, June 2012
- Swiety-Pospiech, A.; Wojnarowska, Z.; Pionteck, J.
- The Journal of Chemical Physics, Vol. 136, Issue 22
Amorphous Protic Ionic Systems as Promising Active Pharmaceutical Ingredients: The Case of the Sumatriptan Succinate Drug
journal, January 2016
- Wojnarowska, Z.; Knapik, J.; Rams-Baron, M.
- Molecular Pharmaceutics, Vol. 13, Issue 3
Heterogeneous Dynamics of Prototypical Ionic Glass CKN Monitored by Physical Aging
journal, January 2013
- Paluch, M.; Wojnarowska, Z.; Hensel-Bielowka, S.
- Physical Review Letters, Vol. 110, Issue 1
Invariance of conductivity relaxation under pressure and temperature variations at constant conductivity relaxation time in
journal, December 2014
- Wojnarowska, Z.; Ngai, K. L.; Paluch, M.
- Physical Review E, Vol. 90, Issue 6
On the scaling behavior of electric conductivity in [C 4 mim][NTf 2 ]
journal, January 2014
- Wojnarowska, Z.; Jarosz, G.; Grzybowski, A.
- Phys. Chem. Chem. Phys., Vol. 16, Issue 38
On the complexity of proton conduction phenomena
journal, November 2000
- Kreuer, K.
- Solid State Ionics, Vol. 136-137, Issue 1-2
The mechanism of proton conduction in phosphoric acid
journal, April 2012
- Vilčiauskas, Linas; Tuckerman, Mark E.; Bester, Gabriel
- Nature Chemistry, Vol. 4, Issue 6
High Pressure as a Key Factor to Identify the Conductivity Mechanism in Protic Ionic Liquids
journal, November 2013
- Wojnarowska, Z.; Wang, Y.; Pionteck, J.
- Physical Review Letters, Vol. 111, Issue 22
Supercooled dynamics of glass-forming liquids and polymers under hydrostatic pressure
journal, May 2005
- Roland, C. M.; Hensel-Bielowka, S.; Paluch, M.
- Reports on Progress in Physics, Vol. 68, Issue 6
Mechanism of Conductivity Relaxation in Liquid and Polymeric Electrolytes: Direct Link between Conductivity and Diffusivity
journal, October 2016
- Gainaru, C.; Stacy, E. W.; Bocharova, V.
- The Journal of Physical Chemistry B, Vol. 120, Issue 42
Diffusion in ionic liquids: the interplay between molecular structure and dynamics
journal, January 2011
- Sangoro, J. R.; Iacob, C.; Naumov, S.
- Soft Matter, Vol. 7, Issue 5
Works referencing / citing this record:
Block Copolymers: Synthesis, Self-Assembly, and Applications
journal, October 2017
- Feng, Hongbo; Lu, Xinyi; Wang, Weiyu
- Polymers, Vol. 9, Issue 12