Influence of Counterion Structure on Conductivity of Polymerized Ionic Liquids

Keith, Jordan R.; Rebello, Nathan J.; Cowen, Benjamin J.; Ganesan, Venkat

doi:10.1021/acsmacrolett.9b00070

Title: Influence of Counterion Structure on Conductivity of Polymerized Ionic Liquids

Journal Article · Mon Mar 25 00:00:00 EDT 2019 · ACS Macro Letters

DOI:https://doi.org/10.1021/acsmacrolett.9b00070· OSTI ID:1507409

^[1]; Rebello, Nathan J. ^[1]; Cowen, Benjamin J. ^[2];

^[1]

Univ. of Texas at Austin, Austin, TX (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

We performed long-time all-atom molecular dynamics simulations of cationic polymerized ionic liquids with eight mobile counterions, systematically varying size and shape to probe their influence on the decoupling of conductivity from polymer segmental dynamics. We demonstrated rigorous identification of the dilatometric glass-transition temperature (T_g) for polymerized ionic liquids using an all-atom force field. Polymer segmental relaxation rates are presumed to be consistent for different materials at the same glass-transition-normalized temperature (T_g/T), allowing us to extract a relative order of decoupling by examining conductivity at the same T_g/T. Size, or ionic volume, cannot fully explain decoupling trends, but within certain geometric and chemical-specific classes, small ions generally show a higher degree of decoupling. This size effect is not universal and appears to be overcome when structural results reveal substantial coordination delocalization. Here, we also reveal a universal inverse correlation between ion-association structural relaxation time and absolute conductivity for these polymerized ionic liquids, supporting the ion-hopping interpretation of ion mobility in polymerized ionic liquids.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1507409

Report Number(s):: SAND-2019-3066J; 673567

Journal Information:: ACS Macro Letters, Vol. 8, Issue 4; ISSN 2161-1653

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 39 works

Citation information provided by
Web of Science

References (39)

15th anniversary of polymerised ionic liquids Nishimura, Naomi; Ohno, Hiroyuki Polymer, Vol. 55, Issue 16 https://doi.org/10.1016/j.polymer.2014.02.042	journal	August 2014
Recent Advances in Innovative Polymer Electrolytes based on Poly(ionic liquid)s Shaplov, Alexander S.; Marcilla, Rebeca; Mecerreyes, David Electrochimica Acta, Vol. 175 https://doi.org/10.1016/j.electacta.2015.03.038	journal	September 2015
Frontiers in poly(ionic liquid)s: syntheses and applications Qian, Wenjing; Texter, John; Yan, Feng Chemical Society Reviews, Vol. 46, Issue 4 https://doi.org/10.1039/C6CS00620E	journal	January 2017
Polymeric ionic liquids: Broadening the properties and applications of polyelectrolytes Mecerreyes, David Progress in Polymer Science, Vol. 36, Issue 12 https://doi.org/10.1016/j.progpolymsci.2011.05.007	journal	December 2011
Molecular Dynamics Simulations of Ionic Liquids: Cation and Anion Dependence of Self-Diffusion Coefficients of Ions Tsuzuki, Seiji; Shinoda, Wataru; Saito, Hiroaki The Journal of Physical Chemistry B, Vol. 113, Issue 31 https://doi.org/10.1021/jp811128b	journal	August 2009
Effects of conformational flexibility of alkyl chains of cations on diffusion of ions in ionic liquids Tsuzuki, Seiji; Matsumoto, Hajime; Shinoda, Wataru Physical Chemistry Chemical Physics, Vol. 13, Issue 13 https://doi.org/10.1039/c0cp02087g	journal	January 2011
Molecular dynamics simulation of imidazolium-based ionic liquids. II. Transport coefficients Kowsari, M. H.; Alavi, Saman; Ashrafizaadeh, Mahmud The Journal of Chemical Physics, Vol. 130, Issue 1 https://doi.org/10.1063/1.3042279	journal	January 2009
Structural and dynamical properties of ionic liquids: Competing influences of molecular properties Spohr, Heidrun V.; Patey, G. N. The Journal of Chemical Physics, Vol. 132, Issue 15 https://doi.org/10.1063/1.3380830	journal	April 2010
Structural and dynamical properties of ionic liquids: The influence of ion size disparity Spohr, H. V.; Patey, G. N. The Journal of Chemical Physics, Vol. 129, Issue 6 https://doi.org/10.1063/1.2968544	journal	August 2008
Structural and dynamical properties of ionic liquids: The influence of charge location Spohr, H. V.; Patey, G. N. The Journal of Chemical Physics, Vol. 130, Issue 10 https://doi.org/10.1063/1.3078381	journal	March 2009
On the dielectric conductivity of molecular ionic liquids Schröder, Christian; Steinhauser, Othmar The Journal of Chemical Physics, Vol. 131, Issue 11 https://doi.org/10.1063/1.3220069	journal	September 2009
Direct Correlation between Ionic Liquid Transport Properties and Ion Pair Lifetimes: A Molecular Dynamics Study Zhang, Yong; Maginn, Edward J. The Journal of Physical Chemistry Letters, Vol. 6, Issue 4 https://doi.org/10.1021/acs.jpclett.5b00003	journal	February 2015
Decoupling of Ionic Transport from Segmental Relaxation in Polymer Electrolytes Wang, Yangyang; Agapov, Alexander L.; Fan, Fei Physical Review Letters, Vol. 108, Issue 8 https://doi.org/10.1103/PhysRevLett.108.088303	journal	February 2012
Ion Conduction in Polymerized Ionic Liquids with Different Pendant Groups Fan, Fei; Wang, Yangyang; Hong, Tao Macromolecules, Vol. 48, Issue 13 https://doi.org/10.1021/acs.macromol.5b00257	journal	June 2015
Design of superionic polymer electrolytes Wang, Yangyang; Sokolov, Alexei P. Current Opinion in Chemical Engineering, Vol. 7 https://doi.org/10.1016/j.coche.2014.09.002	journal	February 2015
Effect of Molecular Weight on the Ion Transport Mechanism in Polymerized Ionic Liquids Fan, Fei; Wang, Weiyu; Holt, Adam P. Macromolecules, Vol. 49, Issue 12 https://doi.org/10.1021/acs.macromol.6b00714	journal	June 2016
Mechanism of Conductivity Relaxation in Liquid and Polymeric Electrolytes: Direct Link between Conductivity and Diffusivity Gainaru, C.; Stacy, E. W.; Bocharova, V. The Journal of Physical Chemistry B, Vol. 120, Issue 42 https://doi.org/10.1021/acs.jpcb.6b08567	journal	October 2016
Mechanisms Underlying Ion Transport in Polymerized Ionic Liquids Mogurampelly, Santosh; Keith, Jordan R.; Ganesan, Venkat Journal of the American Chemical Society, Vol. 139, Issue 28 https://doi.org/10.1021/jacs.7b05579	journal	July 2017
Ion Transport in Cyclopropenium-Based Polymerized Ionic Liquids Griffin, Philip J.; Freyer, Jessica L.; Han, Nicholas Macromolecules, Vol. 51, Issue 5 https://doi.org/10.1021/acs.macromol.7b02546	journal	February 2018
Influence of molecular weight on ion-transport properties of polymeric ionic liquids Keith, Jordan R.; Mogurampelly, Santosh; Aldukhi, Faisal Physical Chemistry Chemical Physics, Vol. 19, Issue 43 https://doi.org/10.1039/C7CP05489K	journal	January 2017
Influence of side chain linker length on ion-transport properties of polymeric ionic liquids Keith, Jordan R.; Mogurampelly, Santosh; Wheatle, Bill K. Journal of Polymer Science Part B: Polymer Physics, Vol. 55, Issue 23 https://doi.org/10.1002/polb.24440	journal	September 2017
Ion Transport in Polymerized Ionic Liquid–Ionic Liquid Blends Mogurampelly, Santosh; Ganesan, Venkat Macromolecules, Vol. 51, Issue 23 https://doi.org/10.1021/acs.macromol.8b01460	journal	November 2018
Anion exchanged polymerized ionic liquids: High free volume single ion conductors Ye, Yuesheng; Elabd, Yossef A. Polymer, Vol. 52, Issue 5 https://doi.org/10.1016/j.polymer.2011.01.031	journal	March 2011
Polymerized Ionic Liquids: Correlation of Ionic Conductivity with Nanoscale Morphology and Counterion Volume Iacob, Ciprian; Matsumoto, Atsushi; Brennan, Marissa ACS Macro Letters, Vol. 6, Issue 9 https://doi.org/10.1021/acsmacrolett.7b00335	journal	August 2017
Design Rules for Highly Conductive Polymeric Ionic Liquids from Molecular Dynamics Simulations Cheng, Yizi; Yang, Junhong; Hung, Jui-Hsiang Macromolecules, Vol. 51, Issue 17 https://doi.org/10.1021/acs.macromol.8b00572	journal	August 2018
Molecular Volume Effects on the Dynamics of Polymerized Ionic Liquids and their Monomers Choi, U. Hyeok; Mittal, Anuj; Price, Terry L. Electrochimica Acta, Vol. 175 https://doi.org/10.1016/j.electacta.2014.12.140	journal	September 2015
Influence of Chain Rigidity and Dielectric Constant on the Glass Transition Temperature in Polymerized Ionic Liquids Bocharova, V.; Wojnarowska, Z.; Cao, Peng-Fei The Journal of Physical Chemistry B, Vol. 121, Issue 51 https://doi.org/10.1021/acs.jpcb.7b09423	journal	December 2017
Computational Study of Room Temperature Molten Salts Composed by 1-Alkyl-3-methylimidazolium CationsForce-Field Proposal and Validation de Andrade, Jones; Böes, Elvis S.; Stassen, Hubert The Journal of Physical Chemistry B, Vol. 106, Issue 51 https://doi.org/10.1021/jp0216629	journal	November 2002
Modeling Ionic Liquids Using a Systematic All-Atom Force Field Canongia Lopes, José N.; Deschamps, Johnny; Pádua, Agílio A. H. The Journal of Physical Chemistry B, Vol. 108, Issue 6 https://doi.org/10.1021/jp0362133	journal	February 2004
Molecular Force Field for Ionic Liquids Composed of Triflate or Bistriflylimide Anions Canongia Lopes, José N.; Pádua, Agílio A. H. The Journal of Physical Chemistry B, Vol. 108, Issue 43 https://doi.org/10.1021/jp0476545	journal	October 2004
Single particle dynamics in ionic liquids of 1-alkyl-3-methylimidazolium cations Urahata, Sérgio M.; Ribeiro, Mauro C. C. The Journal of Chemical Physics, Vol. 122, Issue 2 https://doi.org/10.1063/1.1826035	journal	January 2005
How to Predict the Physical Properties of Ionic Liquids: A Volume-Based Approach Slattery, John M.; Daguenet, Corinne; Dyson, Paul J. Angewandte Chemie International Edition, Vol. 46, Issue 28 https://doi.org/10.1002/anie.200700941	journal	July 2007
Ionic and molar volumes of room temperature ionic liquids Marcus, Yizhak Journal of Molecular Liquids, Vol. 209 https://doi.org/10.1016/j.molliq.2015.06.015	journal	September 2015
Empirical description and prediction of ionic liquids' properties with augmented volume-based thermodynamics Beichel, Witali; Preiss, Ulrich P.; Verevkin, Sergey P. Journal of Molecular Liquids, Vol. 192 https://doi.org/10.1016/j.molliq.2013.07.006	journal	April 2014
Relationships among Ionic Lattice Energies, Molecular (Formula Unit) Volumes, and Thermochemical Radii Jenkins, H. Donald B.; Roobottom, Helen K.; Passmore, Jack Inorganic Chemistry, Vol. 38, Issue 16 https://doi.org/10.1021/ic9812961	journal	August 1999
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Development and Testing of the OPLS All-Atom Force Field on Conformational Energetics and Properties of Organic Liquids Jorgensen, William L.; Maxwell, David S.; Tirado-Rives, Julian Journal of the American Chemical Society, Vol. 118, Issue 45 https://doi.org/10.1021/ja9621760	journal	January 1996
Refined potential model for atomistic simulations of ionic liquid [bmim][PF6] Bhargava, B. L.; Balasubramanian, S. The Journal of Chemical Physics, Vol. 127, Issue 11 https://doi.org/10.1063/1.2772268	journal	September 2007
Development of OPLS-AA Force Field Parameters for 68 Unique Ionic Liquids Sambasivarao, Somisetti V.; Acevedo, Orlando Journal of Chemical Theory and Computation, Vol. 5, Issue 4 https://doi.org/10.1021/ct900009a	journal	March 2009

Cited By (1)

Ion transport mechanisms in salt‐doped polymerized zwitterionic electrolytes Keith, Jordan R.; Ganesan, Venkat Journal of Polymer Science, Vol. 58, Issue 4 https://doi.org/10.1002/pol.20190099	journal	January 2020

Similar Records

Role of solvation site segmental dynamics on ion transport in ethylene-oxide based side-chain polymer electrolytes

Journal Article · Mon Apr 12 00:00:00 EDT 2021 · Journal of Materials Chemistry. A · OSTI ID:1507409

Bennington, Peter; Deng, Chuting; Sharon, Daniel; +4 more

Ion Conduction in Polymerized Ionic Liquids with Different Pendant Groups

Journal Article · Fri Jul 17 00:00:00 EDT 2015 · Macromolecules · OSTI ID:1507409

Fan, Fei; Wang, Yangyang; Hong, Tao; +3 more

Counterion Dynamics in Polyester-Sulfonate Ionomers with Ionic Liquid Counterions

Journal Article · Mon Apr 02 00:00:00 EDT 2012 · Macromolecules · OSTI ID:1507409

Tudryn, Gregory J; Liu, Wenjuan; Wang, Shih-Wa; +1 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Influence of Counterion Structure on Conductivity of Polymerized Ionic Liquids

Citation Formats

References (39)

Cited By (1)

Similar Records

Related Subjects