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

Amaresh Samuthira Pandian, X. Chelsea Chen, Jihua Chen, Bradley S. Lokitz, Rose E. Ruther, Guang Yang, Kun Lou, Jagjit Nanda, Frank M. Delnick, Nancy J. Dudney

Research output: Contribution to journalArticlepeer-review

71 Scopus citations

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. A remarkable Li+ transference number of 0.79 is discovered for the composite electrolyte.

Original languageEnglish
Pages (from-to)153-164
Number of pages12
JournalJournal of Power Sources
Volume390
DOIs
StatePublished - Jun 30 2018

Funding

This research at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) , under contract DE-AC05-00OR22725 , was sponsored by the Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office's Advanced Battery Materials Research program. SEM, TEM and DSC experiments were conducted at the Center for Nanophase Materials Sciences (CNMS), a User Facility sponsored by DOE Office of Science. J. C. characterized the polymer and composite electrolyte using TEM and B. L. conducted the DSC measurements at CNMS. We thank Brion Hoffmann from Ohara Corporation for supplying ceramic electrolyte powders.

FundersFunder number
DOE Office of Science
U.S. Department of EnergyDE-AC05-00OR22725
Battelle
Office of Energy Efficiency and Renewable Energy
Oak Ridge National Laboratory

    Keywords

    • Aqueous processing
    • Composite electrolyte
    • Lithium ion conductivity
    • Solid state lithium battery
    • Spray coating

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