Stable electrolyte for high voltage electrochemical double-layer capacitors

Ruther, Rose E.; Sun, Che -Nan; Holliday, Adam; Cheng, Shiwang; Delnick, Frank M.; Zawodzinski, Thomas A.; Nanda, Jagjit

doi:10.1149/2.0951702jes

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:

Ruther, Rose E. ^[1]; Sun, Che -Nan ^[2]; Holliday, Adam ^[1]; Cheng, Shiwang ^[1]; Delnick, Frank M. ^[1]; Zawodzinski, Thomas A. ^[3]; Nanda, Jagjit ^[3]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Electrosynthesis Co., Lancaster, NY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Publication Date:: 2016-12-28

Research Org.:: Oak Ridge National Lab. (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:: 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.

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                    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

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                    Ruther, Rose E., Sun, Che -Nan, Holliday, Adam, Cheng, Shiwang, Delnick, Frank M., Zawodzinski, Thomas A., and Nanda, Jagjit. Wed .  
"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.

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@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},

  journal      = {Journal of the Electrochemical Society},

  number       = 2,

  volume       = 164,

  place        = {United States},

  year         = {2016},

  month        = {12}

}

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1,2-Dimethoxyethane (DME) is a common electrolyte solvent for lithium metal batteries. Various DME-based electrolyte designs have improved long-term cyclability of high-voltage full cells. However, insufficient Coulombic efficiency at the Li anode and poor high-voltage stability remain a challenge for DME electrolytes. Here, we report a molecular design principle that utilizes a steric hindrance effect to tune the solvation structures of Li⁺ ions. In this work, we hypothesized that by substituting the methoxy groups on DME with larger-sized ethoxy groups, the resulting 1,2-diethoxyethane (DEE) should have a weaker solvation ability and consequently more anion-rich inner solvation shells, both of which enhancemore »« less
https://doi.org/10.1021/jacs.1c09006

Full Text Available
Properties of electric double-layer capacitors with various polymer gel electrolytes

Journal Article Liu, X ; Osaka, Tetsuya - Journal of the Electrochemical Society

Polyethylene oxide (PEO), polymethyl methacrylate (PMMA), and polyacrylonitrile (PAN) based gel electrolytes with a mixture of ethylene carbonate and propylene carbonate as plasticizer and lithium perchlorate were used to fabricate an electric double-layer capacitor (EDLC). The performance of EDLCs with these gel electrolytes was investigated by using isotropic high-density graphite electrodes. The ion conductivities of various gel electrolytes were of the order of 10{sup {minus}4} to 10{sup {minus}3} S/cm, and they decreased in the order PAN > PEO > PMMA at ambient temperature. Capacitances approaching the value of EDLCs using organic liquid electrolyte, 20 mF/cm{sup 2}, with an isotropic high-densitymore »« less
https://doi.org/10.1149/1.1837960

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

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Citation Formats

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

R&D considerations for the performance and application of electrochemical capacitors journal, December 2007

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

A dilatometric study of the voltage limitation of carbonaceous electrodes in aprotic EDLC type electrolytes by charge-induced strain journal, October 2006

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

Colossal pseudocapacitance in a high functionality–high surface area carbon anode doubles the energy of an asymmetric supercapacitor journal, January 2014

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

The study of electrolyte solutions based on solvents from the “glyme” family (linear polyethers) for secondary Li battery systems journal, January 1997

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

Anodic stability of aluminum current collectors in an ionic liquid based on the (fluorosulfonyl)(trifluoromethanesulfonyl)imide anion and its implication on high voltage supercapacitors journal, January 2014

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

The effect of different binders on electrochemical properties of LiNi1/3Mn1/3Co1/3O2 cathode material in lithium ion batteries journal, March 2013

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

Novel NaClO4 and NaPF6 Based Non-Aqueous Electrolytes for Electrical Double Layer Capacitor Application journal, April 2013

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

Comparison of the anodic behavior of aluminum current collectors in imide-based ionic liquids and consequences on the stability of high voltage supercapacitors journal, March 2014

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

The Influence of Pore Structure and Surface Groups on the Performance of High Voltage Electrochemical Double Layer Capacitors Containing Adiponitrile-Based Electrolyte journal, January 2012

Causes of supercapacitors ageing in organic electrolyte journal, September 2007

Electrochemical Properties of Organic Liquid Electrolytes Based on Quaternary Onium Salts for Electrical Double-Layer Capacitors journal, January 1994

The Study of Surface Film Formation on Noble-Metal Electrodes in Alkyl Carbonates/Li Salt Solutions, Using Simultaneous in Situ AFM, EQCM, FTIR, and EIS journal, April 1999

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

Effect of surface phosphorus functionalities of activated carbons containing oxygen and nitrogen on electrochemical capacitance journal, May 2009

Study of styrene butadiene rubber and sodium methyl cellulose as binder for negative electrodes in lithium-ion batteries journal, October 2006

NaClO4 and NaPF6 as potential non-aqueous electrolyte salts for electrical double layer capacitor application journal, November 2012

Temperature behavior and impedance fundamentals of supercapacitors journal, March 2006

Characteristics of non-aqueous quaternary solvent mixture and Na-salts based supercapacitor electrolytes in a wide temperature range journal, March 2014

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

A comparison of the aging of electrochemical double layer capacitors with acetonitrile and propylene carbonate-based electrolytes at elevated voltages journal, February 2010

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

Simultaneous Electrochemical Dual‐Electrode Exfoliation of Graphite toward Scalable Production of High‐Quality Graphene journal, July 2019

Casein‐Derived Activated Carbon: Turning Expired Milk into Active Material for Electrochemical Capacitors journal, December 2019

Towards fast-charging technologies in Li + /Na + storage: from the perspectives of pseudocapacitive materials and non-aqueous hybrid capacitors journal, January 2019

Towards fast-charging technologies in Li+/Na+ storage: from the perspectives of pseudocapacitive materials and non-aqueous hybrid capacitors text, January 2019

Casein-Derived Activated Carbon: Turning Expired Milk into Active Material for Electrochemical Capacitors text, January 2020

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

R&D considerations for the performance and application of electrochemical capacitors
journal, December 2007

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

A dilatometric study of the voltage limitation of carbonaceous electrodes in aprotic EDLC type electrolytes by charge-induced strain
journal, October 2006

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

Colossal pseudocapacitance in a high functionality–high surface area carbon anode doubles the energy of an asymmetric supercapacitor
journal, January 2014

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

The study of electrolyte solutions based on solvents from the “glyme” family (linear polyethers) for secondary Li battery systems
journal, January 1997

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

Anodic stability of aluminum current collectors in an ionic liquid based on the (fluorosulfonyl)(trifluoromethanesulfonyl)imide anion and its implication on high voltage supercapacitors
journal, January 2014

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

The effect of different binders on electrochemical properties of LiNi1/3Mn1/3Co1/3O2 cathode material in lithium ion batteries
journal, March 2013

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

Novel NaClO4 and NaPF6 Based Non-Aqueous Electrolytes for Electrical Double Layer Capacitor Application
journal, April 2013

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

Comparison of the anodic behavior of aluminum current collectors in imide-based ionic liquids and consequences on the stability of high voltage supercapacitors
journal, March 2014

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

The Influence of Pore Structure and Surface Groups on the Performance of High Voltage Electrochemical Double Layer Capacitors Containing Adiponitrile-Based Electrolyte
journal, January 2012

Causes of supercapacitors ageing in organic electrolyte
journal, September 2007

Electrochemical Properties of Organic Liquid Electrolytes Based on Quaternary Onium Salts for Electrical Double-Layer Capacitors
journal, January 1994

The Study of Surface Film Formation on Noble-Metal Electrodes in Alkyl Carbonates/Li Salt Solutions, Using Simultaneous in Situ AFM, EQCM, FTIR, and EIS
journal, April 1999

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

Effect of surface phosphorus functionalities of activated carbons containing oxygen and nitrogen on electrochemical capacitance
journal, May 2009

Study of styrene butadiene rubber and sodium methyl cellulose as binder for negative electrodes in lithium-ion batteries
journal, October 2006

NaClO4 and NaPF6 as potential non-aqueous electrolyte salts for electrical double layer capacitor application
journal, November 2012

Temperature behavior and impedance fundamentals of supercapacitors
journal, March 2006

Characteristics of non-aqueous quaternary solvent mixture and Na-salts based supercapacitor electrolytes in a wide temperature range
journal, March 2014

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

A comparison of the aging of electrochemical double layer capacitors with acetonitrile and propylene carbonate-based electrolytes at elevated voltages
journal, February 2010

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

Simultaneous Electrochemical Dual‐Electrode Exfoliation of Graphite toward Scalable Production of High‐Quality Graphene
journal, July 2019

Casein‐Derived Activated Carbon: Turning Expired Milk into Active Material for Electrochemical Capacitors
journal, December 2019

Towards fast-charging technologies in Li ⁺ /Na ⁺ storage: from the perspectives of pseudocapacitive materials and non-aqueous hybrid capacitors
journal, January 2019

Towards fast-charging technologies in Li+/Na+ storage: from the perspectives of pseudocapacitive materials and non-aqueous hybrid capacitors
text, January 2019

Casein-Derived Activated Carbon: Turning Expired Milk into Active Material for Electrochemical Capacitors
text, January 2020