Comparing Two Electrochemical Approaches for Measuring Transference Numbers in Concentrated Electrolytes

doi:10.1149/2.0231813jes

Title: Comparing Two Electrochemical Approaches for Measuring Transference Numbers in Concentrated Electrolytes

Abstract

We compare two experimental approaches for measuring the cation transference number in mixtures of polyethylene oxide (PEO) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt: the well-established current-interrupt method proposed by Ma et al. [J. Electrochem. Soc., 142, 1859 (1995)], and a more recent method based on measuring the steady-state current proposed by Balsara and Newman [J. Electrochem. Soc., 162, A2720 (2015)]. In electrolytes comprised of high molecular weight PEO, the data from the two techniques agree, highlighting the equivalence of these two approaches. However, in lower molecular weight PEO electrolytes the values of the two approaches diverge at low salt concentrations. We posit this is because the approach of Ma et al. requires measurements that are sensitive to the nature of the interface between the electrolyte and the electrode. The transference numbers measured by the approach of Balsara and Newman for both low and high molecular weight samples vary from 0.7 to -0.8 and are within experimental error throughout the entire salt concentration window.

Authors:

Pesko, Danielle M.; Sawhney, Simar; Newman, John;

Publication Date:: 2018-09-21

Research Org.:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1471808

Alternate Identifier(s):: OSTI ID: 1605215

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

Resource Type:: Published Article

Journal Name:: Journal of the Electrochemical Society

Additional Journal Information:: Journal Name: Journal of the Electrochemical Society Journal Volume: 165 Journal Issue: 13; Journal ID: ISSN 0013-4651

Publisher:: IOP Publishing - The Electrochemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Pesko, Danielle M., Sawhney, Simar, Newman, John, and Balsara, Nitash P. Comparing Two Electrochemical Approaches for Measuring Transference Numbers in Concentrated Electrolytes.  United States: N. p., 2018. 
        Web.  doi:10.1149/2.0231813jes.

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                    Pesko, Danielle M., Sawhney, Simar, Newman, John, & Balsara, Nitash P. Comparing Two Electrochemical Approaches for Measuring Transference Numbers in Concentrated Electrolytes.  United States.  doi:10.1149/2.0231813jes.

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                    Pesko, Danielle M., Sawhney, Simar, Newman, John, and Balsara, Nitash P. Fri .  
        "Comparing Two Electrochemical Approaches for Measuring Transference Numbers in Concentrated Electrolytes".  United States.  doi:10.1149/2.0231813jes.

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@article{osti_1471808,

  title        = {Comparing Two Electrochemical Approaches for Measuring Transference Numbers in Concentrated Electrolytes},

  author       = {Pesko, Danielle M. and Sawhney, Simar and Newman, John and Balsara, Nitash P.},

  abstractNote = {We compare two experimental approaches for measuring the cation transference number in mixtures of polyethylene oxide (PEO) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt: the well-established current-interrupt method proposed by Ma et al. [J. Electrochem. Soc., 142, 1859 (1995)], and a more recent method based on measuring the steady-state current proposed by Balsara and Newman [J. Electrochem. Soc., 162, A2720 (2015)]. In electrolytes comprised of high molecular weight PEO, the data from the two techniques agree, highlighting the equivalence of these two approaches. However, in lower molecular weight PEO electrolytes the values of the two approaches diverge at low salt concentrations. We posit this is because the approach of Ma et al. requires measurements that are sensitive to the nature of the interface between the electrolyte and the electrode. The transference numbers measured by the approach of Balsara and Newman for both low and high molecular weight samples vary from 0.7 to -0.8 and are within experimental error throughout the entire salt concentration window.},

  doi          = {10.1149/2.0231813jes},

  journal      = {Journal of the Electrochemical Society},

  number       = 13,

  volume       = 165,

  place        = {United States},

  year         = {2018},

  month        = {9}

}

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DOI: 10.1149/2.0231813jes

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Works referencing / citing this record:

Ohm’s law for ion conduction in lithium and beyond-lithium battery electrolytes
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Galluzzo, Michael D.; Maslyn, Jacqueline A.; Shah, Deep B.
The Journal of Chemical Physics, Vol. 151, Issue 2
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Comparing Experimental Measurements of Limiting Current in Polymer Electrolytes with Theoretical Predictions
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Lithium Transference Numbers in PEO/LiTFSA Electrolytes Determined by Electrophoretic NMR
journal, January 2019

Rosenwinkel, Mark P.; Schönhoff, Monika
Journal of The Electrochemical Society, Vol. 166, Issue 10
DOI: 10.1149/2.0831910jes

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Title: Comparing Two Electrochemical Approaches for Measuring Transference Numbers in Concentrated Electrolytes

Abstract

Citation Formats

Transport Property and Raman Spectroscopic Studies of the Polymer Electrolyte System P(EO)[sub n]-NaTFSI journal, January 1998

Polymer solid electrolytes - an overview journal, December 1983

The Measurement of a Complete Set of Transport Properties for a Concentrated Solid Polymer Electrolyte Solution journal, January 1995

Universal Relationship between Conductivity and Solvation-Site Connectivity in Ether-Based Polymer Electrolytes journal, July 2016

IONIC CONDUCTIVITY AND LITHIUM TRANSFERENCE NUMBER OF POLY(ETHYLENE OXIDE):LiTFSI SYSTEM journal, February 2017

Determination of Transport Properties for Solid Electrolytes from the Impedance of Thin Layer Cells journal, January 1989

Relationship between Conductivity, Ion Diffusion, and Transference Number in Perfluoropolyether Electrolytes journal, April 2016

Analysis of Transference Number Measurements Based on the Potentiostatic Polarization of Solid Polymer Electrolytes journal, January 1995

Salt Diffusion Coefficients in Block Copolymer Electrolytes journal, January 2011

Transport Properties of LiPF[sub 6]-Based Li-Ion Battery Electrolytes journal, January 2005

Relationship between Steady-State Current in Symmetric Cells and Transference Number of Electrolytes Comprising Univalent and Multivalent Ions journal, January 2015

Ueber die Allotropie des Selens journal, January 1851

Measurement of transference numbers for lithium ion electrolytes via four different methods, a comparative study journal, April 2011

Polymer Electrolytes for Lithium-Ion Batteries journal, April 1998

Transport Properties of a High Molecular Weight Poly(propylene oxide)-LiCF[sub 3]SO[sub 3] System journal, June 1999

Optimizing Ion Transport in Polyether-Based Electrolytes for Lithium Batteries journal, April 2018

Poly(ethylene oxide) electrolytes for operation at near room temperature journal, January 1985

Electrochemical measurement of transference numbers in polymer electrolytes journal, December 1987

Polymer Electrolytes: The Key to Lithium Polymer Batteries journal, March 2000

A Differential Moving Boundary Method for Transference Numbers journal, September 1943

7Li and 19F diffusion coefficients and thermal properties of non-aqueous electrolyte solutions for rechargeable lithium batteries journal, September 1999

Transport property measurements of polymer electrolytes journal, April 1998

Phase Diagrams and Conductivity Behavior of Poly(ethylene oxide)-Molten Salt Rubbery Electrolytes journal, December 1994

Electromotive Force of the Cell with Transference and Theory of Interdiffusion of Electrolytes journal, October 1927

Effect of monomer structure on ionic conductivity in a systematic set of polyester electrolytes journal, June 2016

Mechanism of Ion Transport in Amorphous Poly(ethylene oxide)/LiTFSI from Molecular Dynamics Simulations journal, February 2006

Transport Properties of the Solid Polymer Electrolyte System P(EO) n LiTFSI journal, April 2000

Systematic Computational and Experimental Investigation of Lithium-Ion Transport Mechanisms in Polyester-Based Polymer Electrolytes journal, July 2015

Steady state current flow in solid binary electrolyte cells journal, June 1987

Negative Transference Numbers in Poly(ethylene oxide)-Based Electrolytes journal, January 2017

Mechanism of ion transport in PEO/LiTFSI complexes: Effect of temperature, molecular weight and end groups journal, October 2012

Conductivity, charge transfer and transport number—an ac-investigation of the polymer electrolyte LiSCN-poly(ethyleneoxide) journal, December 1982

Negative Stefan-Maxwell Diffusion Coefficients and Complete Electrochemical Transport Characterization of Homopolymer and Block Copolymer Electrolytes journal, January 2018

Infrared and Raman study of the PEO-LiTFSI polymer electrolyte journal, April 1998

Pulsed‐field gradient nuclear magnetic resonance as a tool for studying translational diffusion: Part 1. Basic theory journal, January 1997

Electrophoretic NMR journal, January 1994

Über Gemischte elektrische Leitung in einheitlichen festen Verbindungen journal, February 1927

Ion Association and Ion Solvation Effects at the Crystalline−Amorphous Phase Transition in PEO−LiTFSI journal, August 2000

Effect of molecular weight on conductivity of polymer electrolytes journal, November 2011

Ohm’s law for ion conduction in lithium and beyond-lithium battery electrolytes journal, July 2019

Comparing Experimental Measurements of Limiting Current in Polymer Electrolytes with Theoretical Predictions journal, January 2019

Lithium Transference Numbers in PEO/LiTFSA Electrolytes Determined by Electrophoretic NMR journal, January 2019

Transport Property and Raman Spectroscopic Studies of the Polymer Electrolyte System P(EO)[sub n]-NaTFSI
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Polymer solid electrolytes - an overview
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The Measurement of a Complete Set of Transport Properties for a Concentrated Solid Polymer Electrolyte Solution
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Universal Relationship between Conductivity and Solvation-Site Connectivity in Ether-Based Polymer Electrolytes
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Relationship between Conductivity, Ion Diffusion, and Transference Number in Perfluoropolyether Electrolytes
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Analysis of Transference Number Measurements Based on the Potentiostatic Polarization of Solid Polymer Electrolytes
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Salt Diffusion Coefficients in Block Copolymer Electrolytes
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Relationship between Steady-State Current in Symmetric Cells and Transference Number of Electrolytes Comprising Univalent and Multivalent Ions
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Ueber die Allotropie des Selens
journal, January 1851

Measurement of transference numbers for lithium ion electrolytes via four different methods, a comparative study
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Polymer Electrolytes for Lithium-Ion Batteries
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Transport Properties of a High Molecular Weight Poly(propylene oxide)-LiCF[sub 3]SO[sub 3] System
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Optimizing Ion Transport in Polyether-Based Electrolytes for Lithium Batteries
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Poly(ethylene oxide) electrolytes for operation at near room temperature
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Electrochemical measurement of transference numbers in polymer electrolytes
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A Differential Moving Boundary Method for Transference Numbers
journal, September 1943

7Li and 19F diffusion coefficients and thermal properties of non-aqueous electrolyte solutions for rechargeable lithium batteries
journal, September 1999

Transport property measurements of polymer electrolytes
journal, April 1998

Phase Diagrams and Conductivity Behavior of Poly(ethylene oxide)-Molten Salt Rubbery Electrolytes
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Electromotive Force of the Cell with Transference and Theory of Interdiffusion of Electrolytes
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Effect of monomer structure on ionic conductivity in a systematic set of polyester electrolytes
journal, June 2016

Mechanism of Ion Transport in Amorphous Poly(ethylene oxide)/LiTFSI from Molecular Dynamics Simulations
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Transport Properties of the Solid Polymer Electrolyte System P(EO) _n LiTFSI
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Systematic Computational and Experimental Investigation of Lithium-Ion Transport Mechanisms in Polyester-Based Polymer Electrolytes
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Steady state current flow in solid binary electrolyte cells
journal, June 1987

Negative Transference Numbers in Poly(ethylene oxide)-Based Electrolytes
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Mechanism of ion transport in PEO/LiTFSI complexes: Effect of temperature, molecular weight and end groups
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Conductivity, charge transfer and transport number—an ac-investigation of the polymer electrolyte LiSCN-poly(ethyleneoxide)
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Infrared and Raman study of the PEO-LiTFSI polymer electrolyte
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Pulsed‐field gradient nuclear magnetic resonance as a tool for studying translational diffusion: Part 1. Basic theory
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Electrophoretic NMR
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Über Gemischte elektrische Leitung in einheitlichen festen Verbindungen
journal, February 1927

Ion Association and Ion Solvation Effects at the Crystalline−Amorphous Phase Transition in PEO−LiTFSI
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Effect of molecular weight on conductivity of polymer electrolytes
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Ohm’s law for ion conduction in lithium and beyond-lithium battery electrolytes
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