Mixed Ionic Liquid Improves Electrolyte Dynamics in Supercapacitors
Abstract
Well-tailored mixtures of distinct ionic liquids can act as optimal electrolytes that extend the operating electrochemical window and improve charge storage density in supercapacitors. Here, we explore two room-temperature ionic liquids, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EmimTFSI) and 1-ethyl-3-methylimidazolium tetrafluoroborate (EmimBF4). We study their electric double-layer behavior in the neat state and as binary mixtures on the external surfaces of onion-like carbon electrodes using quasielastic neutron scattering (QENS) and classical density functional theory techniques. Computational results reveal that a mixture with 4:1 EmimTFSI/EmimBF4 volume ratio displaces the larger [TFSI–] anions with smaller [BF4–] ions, leading to an excess adsorption of [Emim+] cations near the electrode surface. These findings are corroborated by the manifestation of nonuniform ion diffusivity change, complementing the description of structural modifications with changing composition, from QENS measurements. Molecular-level understanding of ion packing near electrodes provides insight for design of ionic liquid formulations that enhance the performance of electrochemical energy storage devices.
- Authors:
-
[1];
[3];
[2];
[4];
[1]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Univ. of California, Riverside, CA (United States)
- Drexel Univ., Philadelphia, PA (United States); U.S. Naval Research Lab., Washington, D.C. (United States)
- Drexel Univ., Philadelphia, PA (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1439150
- Alternate Identifier(s):
- OSTI ID: 1482459
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 122; Journal Issue: 19; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Osti, Naresh C., Gallegos, Alejandro, Dyatkin, Boris, Wu, Jianzhong, Gogotsi, Yury, and Mamontov, Eugene. Mixed Ionic Liquid Improves Electrolyte Dynamics in Supercapacitors. United States: N. p., 2018.
Web. doi:10.1021/acs.jpcc.8b02521.
Osti, Naresh C., Gallegos, Alejandro, Dyatkin, Boris, Wu, Jianzhong, Gogotsi, Yury, & Mamontov, Eugene. Mixed Ionic Liquid Improves Electrolyte Dynamics in Supercapacitors. United States. https://doi.org/10.1021/acs.jpcc.8b02521
Osti, Naresh C., Gallegos, Alejandro, Dyatkin, Boris, Wu, Jianzhong, Gogotsi, Yury, and Mamontov, Eugene. Thu .
"Mixed Ionic Liquid Improves Electrolyte Dynamics in Supercapacitors". United States. https://doi.org/10.1021/acs.jpcc.8b02521. https://www.osti.gov/servlets/purl/1439150.
@article{osti_1439150,
title = {Mixed Ionic Liquid Improves Electrolyte Dynamics in Supercapacitors},
author = {Osti, Naresh C. and Gallegos, Alejandro and Dyatkin, Boris and Wu, Jianzhong and Gogotsi, Yury and Mamontov, Eugene},
abstractNote = {Well-tailored mixtures of distinct ionic liquids can act as optimal electrolytes that extend the operating electrochemical window and improve charge storage density in supercapacitors. Here, we explore two room-temperature ionic liquids, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EmimTFSI) and 1-ethyl-3-methylimidazolium tetrafluoroborate (EmimBF4). We study their electric double-layer behavior in the neat state and as binary mixtures on the external surfaces of onion-like carbon electrodes using quasielastic neutron scattering (QENS) and classical density functional theory techniques. Computational results reveal that a mixture with 4:1 EmimTFSI/EmimBF4 volume ratio displaces the larger [TFSI–] anions with smaller [BF4–] ions, leading to an excess adsorption of [Emim+] cations near the electrode surface. These findings are corroborated by the manifestation of nonuniform ion diffusivity change, complementing the description of structural modifications with changing composition, from QENS measurements. Molecular-level understanding of ion packing near electrodes provides insight for design of ionic liquid formulations that enhance the performance of electrochemical energy storage devices.},
doi = {10.1021/acs.jpcc.8b02521},
journal = {Journal of Physical Chemistry. C},
number = 19,
volume = 122,
place = {United States},
year = {Thu Apr 19 00:00:00 EDT 2018},
month = {Thu Apr 19 00:00:00 EDT 2018}
}
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