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

Villaluenga, Irune; Pesko, Danielle M.; Timachova, Ksenia; Feng, Zhange; Newman, John; Srinivasan, Venkat; Balsara, Nitash P.

doi:10.1149/2.0641811jes

Title: Negative Stefan-Maxwell Diffusion Coefficients and Complete Electrochemical Transport Characterization of Homopolymer and Block Copolymer Electrolytes

Abstract

Nanostructured block copolymers are of particular interest as electrolytes in batteries with lithium metal anodes. The performance of electrolytes in batteries can be predicted only if three transport coefficients (ionic conductivity, κ, salt diffusion coefficient, D, and cation transference number, t⁰₊) are known. We present complete electrochemical transport characterization of a microphase-separated SEO block copolymer electrolyte by reporting κ, D, and t⁰₊ as functions of salt concentration. We compare the properties of the block copolymer electrolyte with those of PEO homopolymer electrolytes. Negative values of t⁰₊ are observed in many cases. Recasting the transport parameters in terms of Stefan-Maxwell coefficients provides insight into the nature of ion transport in these electrolytes.

Authors:

^[1]; Pesko, Danielle M. ^[2];

^[2]; Feng, Zhange ^[3]; Newman, John ^[2];

^[4];

^[2]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Publication Date:: Sat Aug 25 00:00:00 EDT 2018

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

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

OSTI Identifier:: 1480811

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: Journal of the Electrochemical Society

Additional Journal Information:: Journal Volume: 165; Journal Issue: 11; Journal ID: ISSN 0013-4651

Publisher:: The Electrochemical Society

Country of Publication:: United States

Language:: English

Subject:: 25 ENERGY STORAGE

Citation Formats


                    Villaluenga, Irune, Pesko, Danielle M., Timachova, Ksenia, Feng, Zhange, Newman, John, Srinivasan, Venkat, and Balsara, Nitash P. Negative Stefan-Maxwell Diffusion Coefficients and Complete Electrochemical Transport Characterization of Homopolymer and Block Copolymer Electrolytes.  United States: N. p., 2018. 
        Web.  doi:10.1149/2.0641811jes.

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                    Villaluenga, Irune, Pesko, Danielle M., Timachova, Ksenia, Feng, Zhange, Newman, John, Srinivasan, Venkat, & Balsara, Nitash P. Negative Stefan-Maxwell Diffusion Coefficients and Complete Electrochemical Transport Characterization of Homopolymer and Block Copolymer Electrolytes.  United States.  https://doi.org/10.1149/2.0641811jes

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                    Villaluenga, Irune, Pesko, Danielle M., Timachova, Ksenia, Feng, Zhange, Newman, John, Srinivasan, Venkat, and Balsara, Nitash P. 2018.  
        "Negative Stefan-Maxwell Diffusion Coefficients and Complete Electrochemical Transport Characterization of Homopolymer and Block Copolymer Electrolytes".  United States.  https://doi.org/10.1149/2.0641811jes.  https://www.osti.gov/servlets/purl/1480811.

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@article{osti_1480811,

  title        = {Negative Stefan-Maxwell Diffusion Coefficients and Complete Electrochemical Transport Characterization of Homopolymer and Block Copolymer Electrolytes},

  author       = {Villaluenga, Irune and Pesko, Danielle M. and Timachova, Ksenia and Feng, Zhange and Newman, John and Srinivasan, Venkat and Balsara, Nitash P.},

  abstractNote = {Nanostructured block copolymers are of particular interest as electrolytes in batteries with lithium metal anodes. The performance of electrolytes in batteries can be predicted only if three transport coefficients (ionic conductivity, κ, salt diffusion coefficient, D, and cation transference number, t0+) are known. We present complete electrochemical transport characterization of a microphase-separated SEO block copolymer electrolyte by reporting κ, D, and t0+ as functions of salt concentration. We compare the properties of the block copolymer electrolyte with those of PEO homopolymer electrolytes. Negative values of t0+ are observed in many cases. Recasting the transport parameters in terms of Stefan-Maxwell coefficients provides insight into the nature of ion transport in these electrolytes.},

  doi          = {10.1149/2.0641811jes},

  url          = {https://www.osti.gov/biblio/1480811},
  journal      = {Journal of the Electrochemical Society},

  issn         = {0013-4651},

  number       = 11,

  volume       = 165,

  place        = {United States},

  year         = {Sat Aug 25 00:00:00 EDT 2018},

  month        = {Sat Aug 25 00:00:00 EDT 2018}

}

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Works referencing / citing this record:

Optimizing the monomer structure of polyhedral oligomeric silsesquioxane for ion transport in hybrid organic–inorganic block copolymers
journal, January 2020

Gao, Kevin W.; Jiang, Xi; Hoffman, Zach J.
Journal of Polymer Science, Vol. 58, Issue 2
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Difference between approximate and rigorously measured transference numbers in fluorinated electrolytes
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Title: Negative Stefan-Maxwell Diffusion Coefficients and Complete Electrochemical Transport Characterization of Homopolymer and Block Copolymer Electrolytes

Abstract

Citation Formats

Effect of Molecular Weight on the Mechanical and Electrical Properties of Block Copolymer Electrolytes journal, June 2007

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

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

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

Verification and Analysis of Transference Number Measurements by the Galvanostatic Polarization Method journal, January 2000

Measuring the Salt Activity Coefficient in Lithium-Battery Electrolytes journal, January 2008

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

Rubbery Block Copolymer Electrolytes for Solid-State Rechargeable Lithium Batteries journal, January 1999

Cation and anion diffusion in the amorphous phase of the polymer electrolyte (PEO) 8LiCF3SO3 journal, January 1986

Polymer Electrolytes journal, July 2013

Negative effective Li transference numbers in Li salt/ionic liquid mixtures: does Li drift in the “Wrong” direction? journal, January 2018

Determination of Lithium Ion Transference Numbers by Electrophoretic Nuclear Magnetic Resonance journal, January 1996

Ionic Conductivity of Low Molecular Weight Block Copolymer Electrolytes journal, January 2013

Nanomaterials for Rechargeable Lithium Batteries journal, April 2008

Observation of separate cation and anion electrophoretic mobilities in pure ionic liquids journal, February 2014

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

Estimation of Li+ transport number in polymer electrolytes by the combination of complex impedance and potentiostatic polarization measurements journal, September 1988

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

Polymer Electrolytes journal, August 1986

Cation/Anion Associations in Ionic Liquids Modulated by Hydration and Ionic Medium journal, April 2011

Anisotropic Ion Diffusion and Electrochemically Driven Transport in Nanostructured Block Copolymer Electrolytes journal, January 2018

Simultaneous Conduction of Electronic Charge and Lithium Ions in Block Copolymers journal, January 2012

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

Polymer electrolytes journal, January 1987

Optimizing the monomer structure of polyhedral oligomeric silsesquioxane for ion transport in hybrid organic–inorganic block copolymers journal, January 2020

Difference between approximate and rigorously measured transference numbers in fluorinated electrolytes journal, January 2019

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

Comparing Two Electrochemical Approaches for Measuring Transference Numbers in Concentrated Electrolytes journal, January 2018

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

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Effect of Molecular Weight on the Mechanical and Electrical Properties of Block Copolymer Electrolytes
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journal, February 2017

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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Verification and Analysis of Transference Number Measurements by the Galvanostatic Polarization Method
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Measuring the Salt Activity Coefficient in Lithium-Battery Electrolytes
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Electrochemical measurement of transference numbers in polymer electrolytes
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Rubbery Block Copolymer Electrolytes for Solid-State Rechargeable Lithium Batteries
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Cation and anion diffusion in the amorphous phase of the polymer electrolyte (PEO) 8LiCF3SO3
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Negative effective Li transference numbers in Li salt/ionic liquid mixtures: does Li drift in the “Wrong” direction?
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Determination of Lithium Ion Transference Numbers by Electrophoretic Nuclear Magnetic Resonance
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Ionic Conductivity of Low Molecular Weight Block Copolymer Electrolytes
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Negative Transference Numbers in Poly(ethylene oxide)-Based Electrolytes
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Estimation of Li+ transport number in polymer electrolytes by the combination of complex impedance and potentiostatic polarization measurements
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Mechanism of ion transport in PEO/LiTFSI complexes: Effect of temperature, molecular weight and end groups
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Polymer Electrolytes
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Cation/Anion Associations in Ionic Liquids Modulated by Hydration and Ionic Medium
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Anisotropic Ion Diffusion and Electrochemically Driven Transport in Nanostructured Block Copolymer Electrolytes
journal, January 2018

Simultaneous Conduction of Electronic Charge and Lithium Ions in Block Copolymers
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Effect of molecular weight on conductivity of polymer electrolytes
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Polymer electrolytes
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Optimizing the monomer structure of polyhedral oligomeric silsesquioxane for ion transport in hybrid organic–inorganic block copolymers
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Difference between approximate and rigorously measured transference numbers in fluorinated electrolytes
journal, January 2019

Ohm’s law for ion conduction in lithium and beyond-lithium battery electrolytes
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