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Title: Stable electrolyte for high voltage electrochemical double-layer capacitors

Abstract

A simple electrolyte consisting of NaPF6 salt in 1,2-dimethoxyethane (DME) can extend the voltage window of electric double-layer capacitors (EDLCs) to >3.5 V. DME does not passivate carbon electrodes at very negative potentials (near Na/Na+), extending the practical voltage window by about 1.0 V compared to standard, non-aqueous electrolytes based on acetonitrile. The voltage window is demonstrated in two- and three-electrode cells using a combination of electrochemical impedance spectroscopy (EIS), charge-discharge cycling, and measurements of leakage current. DME-based electrolytes cannot match the high conductivity of acetonitrile solutions, but they can satisfy applications that demand high energy density at moderate power. The conductivity of NaPF6 in DME is comparable to commercial lithium-ion battery electrolytes and superior to most ionic liquids. Lastly, factors that limit the voltage window and EDLC energy density are discussed, and strategies to further boost energy density are proposed.

Authors:
 [1];  [2];  [1];  [1];  [1];  [3];  [3]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Electrosynthesis Co., Lancaster, NY (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
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:
1342683
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 2; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; double layer capacitor; electrochemical window; electrolyte; ether; glyme; high voltage; supercapacitor; voltage window

Citation Formats

Ruther, Rose E., Sun, Che -Nan, Holliday, Adam, Cheng, Shiwang, Delnick, Frank M., Zawodzinski, Thomas A., and Nanda, Jagjit. Stable electrolyte for high voltage electrochemical double-layer capacitors. United States: N. p., 2016. Web. doi:10.1149/2.0951702jes.
Ruther, Rose E., Sun, Che -Nan, Holliday, Adam, Cheng, Shiwang, Delnick, Frank M., Zawodzinski, Thomas A., & Nanda, Jagjit. Stable electrolyte for high voltage electrochemical double-layer capacitors. United States. https://doi.org/10.1149/2.0951702jes
Ruther, Rose E., Sun, Che -Nan, Holliday, Adam, Cheng, Shiwang, Delnick, Frank M., Zawodzinski, Thomas A., and Nanda, Jagjit. 2016. "Stable electrolyte for high voltage electrochemical double-layer capacitors". United States. https://doi.org/10.1149/2.0951702jes. https://www.osti.gov/servlets/purl/1342683.
@article{osti_1342683,
title = {Stable electrolyte for high voltage electrochemical double-layer capacitors},
author = {Ruther, Rose E. and Sun, Che -Nan and Holliday, Adam and Cheng, Shiwang and Delnick, Frank M. and Zawodzinski, Thomas A. and Nanda, Jagjit},
abstractNote = {A simple electrolyte consisting of NaPF6 salt in 1,2-dimethoxyethane (DME) can extend the voltage window of electric double-layer capacitors (EDLCs) to >3.5 V. DME does not passivate carbon electrodes at very negative potentials (near Na/Na+), extending the practical voltage window by about 1.0 V compared to standard, non-aqueous electrolytes based on acetonitrile. The voltage window is demonstrated in two- and three-electrode cells using a combination of electrochemical impedance spectroscopy (EIS), charge-discharge cycling, and measurements of leakage current. DME-based electrolytes cannot match the high conductivity of acetonitrile solutions, but they can satisfy applications that demand high energy density at moderate power. The conductivity of NaPF6 in DME is comparable to commercial lithium-ion battery electrolytes and superior to most ionic liquids. Lastly, factors that limit the voltage window and EDLC energy density are discussed, and strategies to further boost energy density are proposed.},
doi = {10.1149/2.0951702jes},
url = {https://www.osti.gov/biblio/1342683}, journal = {Journal of the Electrochemical Society},
issn = {0013-4651},
number = 2,
volume = 164,
place = {United States},
year = {Wed Dec 28 00:00:00 EST 2016},
month = {Wed Dec 28 00:00:00 EST 2016}
}

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Cited by: 18 works
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Works referenced in this record:

Differential capacitance of the double layer at the electrode/ionic liquids interface
journal, January 2010


Comparison of various tetraalkylammonium salts as supporting electrolytes in organic electrochemical reactions
journal, August 1971


Pseudocapacitive oxide materials for high-rate electrochemical energy storage
journal, January 2014


Oxidative Stability and Initial Decomposition Reactions of Carbonate, Sulfone, and Alkyl Phosphate-Based Electrolytes
journal, April 2013


Sodium Carboxymethyl Cellulose
journal, January 2007


Suppression of aluminum current collector corrosion in ionic liquid containing electrolytes
journal, September 2012


Vinylene Carbonate as Co-Solvent for Low-Temperature Mixed Electrolyte Based Supercapacitors
journal, January 2016


Conductivity of electrolytes for rechargeable lithium batteries
journal, June 1991


Materials for electrochemical capacitors
journal, November 2008


What Are Batteries, Fuel Cells, and Supercapacitors?
journal, October 2004


Aluminum Corrosion in Lithium Batteries An Investigation Using the Electrochemical Quartz Crystal Microbalance
journal, January 2000


Adiponitrile-based electrochemical double layer capacitor
journal, April 2012


Ageing behaviour of electrochemical double layer capacitors
journal, October 2007


The electrochemical behaviour of tetrahydrofuran and propylene carbonate without added electrolyte
journal, May 1990


Cycle versus voltage hold – Which is the better stability test for electrochemical double layer capacitors?
journal, March 2013


1.9V aqueous carbon–carbon supercapacitors with unequal electrode capacitances
journal, December 2012


Multifunctional MnO2−Carbon Nanoarchitectures Exhibit Battery and Capacitor Characteristics in Alkaline Electrolytes
journal, September 2009


Carbon properties and their role in supercapacitors
journal, June 2006


Identification of Surface Films Formed on Lithium in Dimethoxyethane and Tetrahydrofuran Solutions
journal, January 1988


Ageing of electrochemical double layer capacitors
journal, April 2012


On the electrochemical behavior of magnesium electrodes in polar aprotic electrolyte solutions
journal, May 1999


Electrochemical activity of carbon blacks in LiPF6-based organic electrolytes
journal, January 2014


Ionic liquid-1,2-dimethoxyethane mixture as electrolyte for high power density supercapacitors
journal, July 2016


Aluminum corrosion in electrolyte of Li-ion battery
journal, July 2002


Interconnected Carbon Nanosheets Derived from Hemp for Ultrafast Supercapacitors with High Energy
journal, May 2013


An in situ Raman study of the intercalation of supercapacitor-type electrolyte into microcrystalline graphite
journal, October 2006


A Rechargeable Cell Based on a Conductive Polymer/Metal Alloy Composite Electrode
journal, January 1989


Electrochemical Properties of Imidazolium Salt Electrolytes for Electrochemical Capacitor Applications
journal, January 1999


Performance and stability of electrochemical capacitor based on anthraquinone modified activated carbon
journal, April 2011


Carbon–ionic liquid double-layer capacitors
journal, March 2004


Mesoporous anhydrous RuO2 as a supercapacitor electrode material
journal, November 2004


Electrolyte Systems for High Withstand Voltage and Durability I. Linear Sulfones for Electric Double-Layer Capacitors
journal, January 2011


Cellulose as a binding material in graphitic anodes for Li ion batteries: a performance and degradation study
journal, February 2003


Electrolyte Systems for High Withstand Voltage and Durability II. Alkylated Cyclic Carbonates for Electric Double-Layer Capacitors
journal, January 2011


Unequalisation of electrode capacitances for enhanced energy capacity in asymmetrical supercapacitors
journal, January 2010


Carbon materials for the electrochemical storage of energy in capacitors
journal, May 2001


Carbons and Electrolytes for Advanced Supercapacitors
journal, February 2014


Aging of electrochemical double layer capacitors with acetonitrile-based electrolyte at elevated voltages
journal, June 2010


Causes of supercapacitors ageing in organic electrolyte
journal, September 2007


Double-layer and pseudocapacitance types of electrochemical capacitors and their applications to the development of hybrid devices
journal, September 2003


Ionic liquids as electrolytes
journal, August 2006


Principles and applications of electrochemical capacitors
journal, May 2000


Charge Storage Mechanism of MnO 2 Electrode Used in Aqueous Electrochemical Capacitor
journal, August 2004


Toward Reliable Values of Electrochemical Stability Limits for Electrolytes
journal, January 1999


Carbonized Chicken Eggshell Membranes with 3D Architectures as High-Performance Electrode Materials for Supercapacitors
journal, March 2012


Density, Relative Permittivity, and Viscosity of Propylene Carbonate + Dimethoxyethane Mixtures from 25 °C to 125 °C
journal, November 2000


Temperature behavior and impedance fundamentals of supercapacitors
journal, March 2006


Diagnostic analyses for mechanisms of self-discharge of electrochemical capacitors and batteries
journal, March 1997


“Double-Salt” Electrolytes for High Voltage Electrochemical Double-Layer Capacitors
journal, January 2015


Pulse-Gradient Spin-Echo 1 H, 7 Li, and 19 F NMR Diffusion and Ionic Conductivity Measurements of 14 Organic Electrolytes Containing LiN(SO 2 CF 3 ) 2
journal, January 1999


The electrochemistry of noble metal electrodes in aprotic organic solvents containing lithium salts
journal, January 1991


The Mechanisms of Lithium and Sodium Insertion in Carbon Materials
journal, January 2001


Degradation Responses of Activated-Carbon-Based EDLCs for Higher Voltage Operation and Their Factors
journal, January 2009


Oxidative-Stability Enhancement and Charge Transport Mechanism in Glyme–Lithium Salt Equimolar Complexes
journal, August 2011