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

Journal Article · · Chemistry of Materials
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

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.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725; DEC-2014/15/B/ST3/04246
OSTI ID:
1408578
Journal Information:
Chemistry of Materials, Vol. 29, Issue 19; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 30 works
Citation information provided by
Web of Science

References (43)

Ionic-liquid materials for the electrochemical challenges of the future journal July 2009
Solvent-Free Electrolytes with Aqueous Solution-Like Conductivities journal October 2003
Ionic liquids and their solid-state analogues as materials for energy generation and storage journal January 2016
Charge Transport and Glassy Dynamics in Ionic Liquids journal November 2011
Dielectric and Viscoelastic Responses of Imidazolium-Based Ionomers with Different Counterions and Side Chain Lengths journal January 2014
Dielectric relaxation behavior of polymerized ionic liquids with various charge densities journal June 2013
Decoupling of ionic conductivity from structural dynamics in polymerized ionic liquids journal January 2014
Molecular Volume Effects on the Dynamics of Polymerized Ionic Liquids and their Monomers journal September 2015
Molecular Dynamics and Charge Transport in Polymeric Polyisobutylene-Based Ionic Liquids journal March 2016
Effect of Molecular Weight on the Ion Transport Mechanism in Polymerized Ionic Liquids journal June 2016
Ion Conduction in Polymerized Ionic Liquids with Different Pendant Groups journal June 2015
Highly decoupled ionic and protonic solid electrolyte systems, in relation to other relaxing systems and their energy landscapes journal November 2006
Dynamic processes in ionic glasses journal May 1990
Ionic conductivity and glass structure journal December 1989
Progress in the use of ionic liquids as electrolyte membranes in fuel cells journal November 2014
Conductivity Mechanism in Polymerized Imidazolium-Based Protic Ionic Liquid [HSO 3 –BVIm][OTf]: Dielectric Relaxation Studies journal June 2014
Enhanced proton transport in nanostructured polymer electrolyte/ionic liquid membranes under water-free conditions journal October 2010
Charge transport in poly-imidazole membranes: a fresh appraisal of the Grotthuss mechanism journal January 2012
Molecular Origin of Enhanced Proton Conductivity in Anhydrous Ionic Systems journal January 2015
Charge-transport model for conducting polymers journal November 2016
Effect of Pressure on Decoupling of Ionic Conductivity from Segmental Dynamics in Polymerized Ionic Liquids journal November 2015
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
Intramolecular hydroalkoxylation in Brønsted acidic ionic liquids and its application to the synthesis of (±)-centrolobine journal January 2011
One-pot conversion of carbohydrates into gamma-valerolactone catalyzed by highly cross-linked ionic liquid polymer and Co/TiO 2 journal January 2015
The ORCA program system: The ORCA program system journal June 2011
Broadband Dielectric Spectroscopy book January 2003
Fundamental questions relating to ion conduction in disordered solids journal March 2009
Anomalous Electrical Conductivity Behavior at Elevated Pressure in the Protic Ionic Liquid Procainamide Hydrochloride journal January 2012
Recent progress on dielectric properties of protic ionic liquids journal January 2015
Comments on the electric modulus function journal January 2005
Role of hydrogen bonds in the supercooled dynamics of glass-forming liquids at high pressures journal January 2008
Experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former journal August 2017
High pressure study of molecular dynamics of protic ionic liquid lidocaine hydrochloride journal June 2012
Amorphous Protic Ionic Systems as Promising Active Pharmaceutical Ingredients: The Case of the Sumatriptan Succinate Drug journal January 2016
Heterogeneous Dynamics of Prototypical Ionic Glass CKN Monitored by Physical Aging journal January 2013
Invariance of conductivity relaxation under pressure and temperature variations at constant conductivity relaxation time in 0.4 Ca ( N O 3 ) 2 0.6 KN O 3 journal December 2014
On the scaling behavior of electric conductivity in [C 4 mim][NTf 2 ] journal January 2014
On the complexity of proton conduction phenomena journal November 2000
The mechanism of proton conduction in phosphoric acid journal April 2012
High Pressure as a Key Factor to Identify the Conductivity Mechanism in Protic Ionic Liquids journal November 2013
Supercooled dynamics of glass-forming liquids and polymers under hydrostatic pressure journal May 2005
Mechanism of Conductivity Relaxation in Liquid and Polymeric Electrolytes: Direct Link between Conductivity and Diffusivity journal October 2016
Diffusion in ionic liquids: the interplay between molecular structure and dynamics journal January 2011

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Block Copolymers: Synthesis, Self-Assembly, and Applications journal October 2017

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