A Dual Ionic Liquid-Based Low-Temperature Electrolyte System

Yifei Xu, Wendy J. Lin, Marisa Gliege, Ryan Gunckel, Zuofeng Zhao, Hongyu Yu, Lenore Dai

Research output: Contribution to journalArticle

Abstract

Ionic liquids (ILs) show a promising future as electrolytes in electrochemical devices. In particular, IL-based electrolytes bring operations at extreme temperatures to realization that conventional electrolytes fail to accomplish. Although IL electrolytes demonstrate considerable progress in high-temperature applications, their breakthroughs in devices operating at low temperatures are still very limited due to undesirable phase transitions and unsatisfying transport properties. In this study, we present an approach where, by tuning molecular interactions in the system, the designed electrolyte of an IL-based mixture can reach a lower operating temperature with improved transport properties. We have discovered that the incorporation of the IL, ethylammonium nitrate ([EA][N]), can contribute to reforming the molecular interactions within the system, which effectively resolve the crystallization accompanied with the excess of water and retain a low glass transition temperature. The reported liquid electrolyte systems based on a mixture of 1-butyl-3-methylimidazolium iodide ([BMIM][I]), [EA][N], water, and lithium iodide exhibit a glass transition temperature below -105 °C. Furthermore, the optimized electrolyte system shows significant viscosity reduction and ionic conductivity enhancement from 25 to -75 °C. The influence is also noticeable on the increased ionicity, which made the developed electrolyte comparable with other good ILs under the Walden rule. The electrochemical stability of the electrolyte system is revealed by a steady and reproducible profile of iodide/triiodide redox reactions at room temperature over a proper potential window via cyclic voltammetry. The results from this work not only provide a potential solution to applications of the iodide/triiodide redox couple-based electrochemical devices at low temperatures but also show a practical approach to obtain tailored properties of a mixture system via modifying molecular interactions.

Original languageEnglish (US)
Pages (from-to)12077-12086
Number of pages10
JournalJournal of Physical Chemistry B
Volume122
Issue number50
DOIs
StatePublished - Dec 20 2018

Fingerprint

Ionic Liquids
Ionic liquids
Electrolytes
electrolytes
Temperature
liquids
Iodides
iodides
Molecular interactions
molecular interactions
Transition Temperature
Equipment and Supplies
Transport properties
glass transition temperature
Oxidation-Reduction
Glass
nitrates
Nitrates
transport properties
High temperature applications

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

Cite this

Xu, Y., Lin, W. J., Gliege, M., Gunckel, R., Zhao, Z., Yu, H., & Dai, L. (2018). A Dual Ionic Liquid-Based Low-Temperature Electrolyte System. Journal of Physical Chemistry B, 122(50), 12077-12086. https://doi.org/10.1021/acs.jpcb.8b08815

A Dual Ionic Liquid-Based Low-Temperature Electrolyte System. / Xu, Yifei; Lin, Wendy J.; Gliege, Marisa; Gunckel, Ryan; Zhao, Zuofeng; Yu, Hongyu; Dai, Lenore.

In: Journal of Physical Chemistry B, Vol. 122, No. 50, 20.12.2018, p. 12077-12086.

Research output: Contribution to journalArticle

Xu, Y, Lin, WJ, Gliege, M, Gunckel, R, Zhao, Z, Yu, H & Dai, L 2018, 'A Dual Ionic Liquid-Based Low-Temperature Electrolyte System', Journal of Physical Chemistry B, vol. 122, no. 50, pp. 12077-12086. https://doi.org/10.1021/acs.jpcb.8b08815
Xu Y, Lin WJ, Gliege M, Gunckel R, Zhao Z, Yu H et al. A Dual Ionic Liquid-Based Low-Temperature Electrolyte System. Journal of Physical Chemistry B. 2018 Dec 20;122(50):12077-12086. https://doi.org/10.1021/acs.jpcb.8b08815
Xu, Yifei ; Lin, Wendy J. ; Gliege, Marisa ; Gunckel, Ryan ; Zhao, Zuofeng ; Yu, Hongyu ; Dai, Lenore. / A Dual Ionic Liquid-Based Low-Temperature Electrolyte System. In: Journal of Physical Chemistry B. 2018 ; Vol. 122, No. 50. pp. 12077-12086.
@article{9cba72e83642427ca1205ffceb8ea257,
title = "A Dual Ionic Liquid-Based Low-Temperature Electrolyte System",
abstract = "Ionic liquids (ILs) show a promising future as electrolytes in electrochemical devices. In particular, IL-based electrolytes bring operations at extreme temperatures to realization that conventional electrolytes fail to accomplish. Although IL electrolytes demonstrate considerable progress in high-temperature applications, their breakthroughs in devices operating at low temperatures are still very limited due to undesirable phase transitions and unsatisfying transport properties. In this study, we present an approach where, by tuning molecular interactions in the system, the designed electrolyte of an IL-based mixture can reach a lower operating temperature with improved transport properties. We have discovered that the incorporation of the IL, ethylammonium nitrate ([EA][N]), can contribute to reforming the molecular interactions within the system, which effectively resolve the crystallization accompanied with the excess of water and retain a low glass transition temperature. The reported liquid electrolyte systems based on a mixture of 1-butyl-3-methylimidazolium iodide ([BMIM][I]), [EA][N], water, and lithium iodide exhibit a glass transition temperature below -105 °C. Furthermore, the optimized electrolyte system shows significant viscosity reduction and ionic conductivity enhancement from 25 to -75 °C. The influence is also noticeable on the increased ionicity, which made the developed electrolyte comparable with other good ILs under the Walden rule. The electrochemical stability of the electrolyte system is revealed by a steady and reproducible profile of iodide/triiodide redox reactions at room temperature over a proper potential window via cyclic voltammetry. The results from this work not only provide a potential solution to applications of the iodide/triiodide redox couple-based electrochemical devices at low temperatures but also show a practical approach to obtain tailored properties of a mixture system via modifying molecular interactions.",
author = "Yifei Xu and Lin, {Wendy J.} and Marisa Gliege and Ryan Gunckel and Zuofeng Zhao and Hongyu Yu and Lenore Dai",
year = "2018",
month = "12",
day = "20",
doi = "10.1021/acs.jpcb.8b08815",
language = "English (US)",
volume = "122",
pages = "12077--12086",
journal = "Journal of Physical Chemistry B Materials",
issn = "1520-6106",
publisher = "American Chemical Society",
number = "50",

}

TY - JOUR

T1 - A Dual Ionic Liquid-Based Low-Temperature Electrolyte System

AU - Xu, Yifei

AU - Lin, Wendy J.

AU - Gliege, Marisa

AU - Gunckel, Ryan

AU - Zhao, Zuofeng

AU - Yu, Hongyu

AU - Dai, Lenore

PY - 2018/12/20

Y1 - 2018/12/20

N2 - Ionic liquids (ILs) show a promising future as electrolytes in electrochemical devices. In particular, IL-based electrolytes bring operations at extreme temperatures to realization that conventional electrolytes fail to accomplish. Although IL electrolytes demonstrate considerable progress in high-temperature applications, their breakthroughs in devices operating at low temperatures are still very limited due to undesirable phase transitions and unsatisfying transport properties. In this study, we present an approach where, by tuning molecular interactions in the system, the designed electrolyte of an IL-based mixture can reach a lower operating temperature with improved transport properties. We have discovered that the incorporation of the IL, ethylammonium nitrate ([EA][N]), can contribute to reforming the molecular interactions within the system, which effectively resolve the crystallization accompanied with the excess of water and retain a low glass transition temperature. The reported liquid electrolyte systems based on a mixture of 1-butyl-3-methylimidazolium iodide ([BMIM][I]), [EA][N], water, and lithium iodide exhibit a glass transition temperature below -105 °C. Furthermore, the optimized electrolyte system shows significant viscosity reduction and ionic conductivity enhancement from 25 to -75 °C. The influence is also noticeable on the increased ionicity, which made the developed electrolyte comparable with other good ILs under the Walden rule. The electrochemical stability of the electrolyte system is revealed by a steady and reproducible profile of iodide/triiodide redox reactions at room temperature over a proper potential window via cyclic voltammetry. The results from this work not only provide a potential solution to applications of the iodide/triiodide redox couple-based electrochemical devices at low temperatures but also show a practical approach to obtain tailored properties of a mixture system via modifying molecular interactions.

AB - Ionic liquids (ILs) show a promising future as electrolytes in electrochemical devices. In particular, IL-based electrolytes bring operations at extreme temperatures to realization that conventional electrolytes fail to accomplish. Although IL electrolytes demonstrate considerable progress in high-temperature applications, their breakthroughs in devices operating at low temperatures are still very limited due to undesirable phase transitions and unsatisfying transport properties. In this study, we present an approach where, by tuning molecular interactions in the system, the designed electrolyte of an IL-based mixture can reach a lower operating temperature with improved transport properties. We have discovered that the incorporation of the IL, ethylammonium nitrate ([EA][N]), can contribute to reforming the molecular interactions within the system, which effectively resolve the crystallization accompanied with the excess of water and retain a low glass transition temperature. The reported liquid electrolyte systems based on a mixture of 1-butyl-3-methylimidazolium iodide ([BMIM][I]), [EA][N], water, and lithium iodide exhibit a glass transition temperature below -105 °C. Furthermore, the optimized electrolyte system shows significant viscosity reduction and ionic conductivity enhancement from 25 to -75 °C. The influence is also noticeable on the increased ionicity, which made the developed electrolyte comparable with other good ILs under the Walden rule. The electrochemical stability of the electrolyte system is revealed by a steady and reproducible profile of iodide/triiodide redox reactions at room temperature over a proper potential window via cyclic voltammetry. The results from this work not only provide a potential solution to applications of the iodide/triiodide redox couple-based electrochemical devices at low temperatures but also show a practical approach to obtain tailored properties of a mixture system via modifying molecular interactions.

UR - http://www.scopus.com/inward/record.url?scp=85058950771&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85058950771&partnerID=8YFLogxK

U2 - 10.1021/acs.jpcb.8b08815

DO - 10.1021/acs.jpcb.8b08815

M3 - Article

VL - 122

SP - 12077

EP - 12086

JO - Journal of Physical Chemistry B Materials

JF - Journal of Physical Chemistry B Materials

SN - 1520-6106

IS - 50

ER -