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Title: Facile and scalable fabrication of polymer-ceramic composite electrolyte with high ceramic loadings

Abstract

Solid state electrolytes are a promising alternative to flammable liquid electrolytes for high-energy lithium battery applications. In this work polymer-ceramic composite electrolyte membrane with high ceramic loading (greater than 60 vol%) is fabricated using a model polymer electrolyte poly(ethylene oxide) + lithium trifluoromethane sulfonate and a lithium-conducting ceramic powder. The effects of processing methods, choice of plasticizer and varying composition on ionic conductivity of the composite electrolyte are thoroughly investigated. The physical, structural and thermal properties of the composites are exhaustively characterized. We demonstrate that aqueous spray coating followed by hot pressing is a scalable and inexpensive technique to obtain composite membranes that are amazingly dense and uniform. The ionic conductivity of composites fabricated using this protocol is at least one order of magnitude higher than those made by dry milling and solution casting. The introduction of tetraethylene glycol dimethyl ether further increases the ionic conductivity. The composite electrolyte's interfacial compatibility with metallic lithium and good cyclability is verified by constructing lithium symmetrical cells. As a result, a remarkable Li+ transference number of 0.79 is discovered for the composite electrolyte.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1439943
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 390; Journal Issue: C; Journal ID: ISSN 0378-7753
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Composite electrolyte; Aqueous processing; Spray coating; Lithium ion conductivity; Solid state lithium battery

Citation Formats

Pandian, Amaresh Samuthira, Chen, Xi Chelsea, Chen, Jihua, Lokitz, Bradley S., Ruther, Rose E., Yang, Guang, Lou, Kun, Nanda, Jagjit, Delnick, Frank M., and Dudney, Nancy J. Facile and scalable fabrication of polymer-ceramic composite electrolyte with high ceramic loadings. United States: N. p., 2018. Web. doi:10.1016/j.jpowsour.2018.04.006.
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Pandian, Amaresh Samuthira, Chen, Xi Chelsea, Chen, Jihua, Lokitz, Bradley S., Ruther, Rose E., Yang, Guang, Lou, Kun, Nanda, Jagjit, Delnick, Frank M., & Dudney, Nancy J. Facile and scalable fabrication of polymer-ceramic composite electrolyte with high ceramic loadings. United States. https://doi.org/10.1016/j.jpowsour.2018.04.006
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Pandian, Amaresh Samuthira, Chen, Xi Chelsea, Chen, Jihua, Lokitz, Bradley S., Ruther, Rose E., Yang, Guang, Lou, Kun, Nanda, Jagjit, Delnick, Frank M., and Dudney, Nancy J. Tue . "Facile and scalable fabrication of polymer-ceramic composite electrolyte with high ceramic loadings". United States. https://doi.org/10.1016/j.jpowsour.2018.04.006. https://www.osti.gov/servlets/purl/1439943.
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@article{osti_1439943,
title = {Facile and scalable fabrication of polymer-ceramic composite electrolyte with high ceramic loadings},
author = {Pandian, Amaresh Samuthira and Chen, Xi Chelsea and Chen, Jihua and Lokitz, Bradley S. and Ruther, Rose E. and Yang, Guang and Lou, Kun and Nanda, Jagjit and Delnick, Frank M. and Dudney, Nancy J.},
abstractNote = {Solid state electrolytes are a promising alternative to flammable liquid electrolytes for high-energy lithium battery applications. In this work polymer-ceramic composite electrolyte membrane with high ceramic loading (greater than 60 vol%) is fabricated using a model polymer electrolyte poly(ethylene oxide) + lithium trifluoromethane sulfonate and a lithium-conducting ceramic powder. The effects of processing methods, choice of plasticizer and varying composition on ionic conductivity of the composite electrolyte are thoroughly investigated. The physical, structural and thermal properties of the composites are exhaustively characterized. We demonstrate that aqueous spray coating followed by hot pressing is a scalable and inexpensive technique to obtain composite membranes that are amazingly dense and uniform. The ionic conductivity of composites fabricated using this protocol is at least one order of magnitude higher than those made by dry milling and solution casting. The introduction of tetraethylene glycol dimethyl ether further increases the ionic conductivity. The composite electrolyte's interfacial compatibility with metallic lithium and good cyclability is verified by constructing lithium symmetrical cells. As a result, a remarkable Li+ transference number of 0.79 is discovered for the composite electrolyte.},
doi = {10.1016/j.jpowsour.2018.04.006},
journal = {Journal of Power Sources},
number = C,
volume = 390,
place = {United States},
year = {Tue Apr 24 00:00:00 EDT 2018},
month = {Tue Apr 24 00:00:00 EDT 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1016/j.jpowsour.2018.04.006
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Graphical Abstract Graphical Abstract: We demonstrate that aqueous spray coating followed by hot pressing is a scalable and inexpensive technique to obtain composite membranes that are amazingly dense and uniform. The ionic conductivity of composites fabricated using this protocol is at least one order of magnitude higher than those made by drymore » milling and solution casting.« less
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    Mechanical Stress Induced Current Focusing and Fracture in Grain Boundaries
    journal, January 2019

    • Barai, Pallab; Higa, Kenneth; Ngo, Anh T.
    • Journal of The Electrochemical Society, Vol. 166, Issue 10
    • DOI: 10.1149/2.0321910jes
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