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

Journal Article · Sat Aug 25 00:00:00 EDT 2018 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/2.0641811jes· OSTI ID:1480811

^[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)

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.

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

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

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1480811

Journal Information:: Journal of the Electrochemical Society, Vol. 165, Issue 11; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 60 works

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Optimizing the monomer structure of polyhedral oligomeric silsesquioxane for ion transport in hybrid organic–inorganic block copolymers Gao, Kevin W.; Jiang, Xi; Hoffman, Zach J. Journal of Polymer Science, Vol. 58, Issue 2 https://doi.org/10.1002/pol.20190073	journal	January 2020
Difference between approximate and rigorously measured transference numbers in fluorinated electrolytes Shah, Deep B.; Nguyen, Hien Q.; Grundy, Lorena S. Physical Chemistry Chemical Physics, Vol. 21, Issue 15 https://doi.org/10.1039/c9cp00216b	journal	January 2019
Ohm’s law for ion conduction in lithium and beyond-lithium battery electrolytes Galluzzo, Michael D.; Maslyn, Jacqueline A.; Shah, Deep B. The Journal of Chemical Physics, Vol. 151, Issue 2 https://doi.org/10.1063/1.5109684	journal	July 2019
Comparing Two Electrochemical Approaches for Measuring Transference Numbers in Concentrated Electrolytes Pesko, Danielle M.; Sawhney, Simar; Newman, John Journal of The Electrochemical Society, Vol. 165, Issue 13 https://doi.org/10.1149/2.0231813jes	journal	January 2018
Theoretical Interpretation of Ion Velocities in Concentrated Electrolytes Measured by Electrophoretic NMR Timachova, Ksenia; Newman, John; Balsara, Nitash P. Journal of The Electrochemical Society, Vol. 166, Issue 2 https://doi.org/10.1149/2.0591902jes	journal	January 2019
Lithium Transference Numbers in PEO/LiTFSA Electrolytes Determined by Electrophoretic NMR Rosenwinkel, Mark P.; Schönhoff, Monika Journal of The Electrochemical Society, Vol. 166, Issue 10 https://doi.org/10.1149/2.0831910jes	journal	January 2019
Comparing Cycling Characteristics of Symmetric Lithium-Polymer-Lithium Cells with Theoretical Predictions Pesko, Danielle M.; Feng, Zhange; Sawhney, Simar Journal of The Electrochemical Society, Vol. 165, Issue 13 https://doi.org/10.1149/2.0921813jes	journal	January 2018

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