Visualizing percolation and ion transport in hybrid solid electrolytes for Li-metal batteries

Wahid Zaman, Nicholas Hortance, Marm B. Dixit, Vincent De Andrade, Kelsey B. Hatzell

Research output: Contribution to journalArticlepeer-review

86 Scopus citations

Abstract

Hybrid solid electrolytes are composed of organic (polymer) and inorganic (ceramic) ion conducting materials, and are promising options for large-scale production of solid state lithium-metal batteries. Hybrid solid electrolytes containing 15 vol% Al-LLZO demonstrate optimal ionic conductivity properties. Ionic conductivity is shown to decrease at high inorganic loadings. This optimum is most obvious above the melting temperature of polyethylene oxide where the polymer is amorphous. Structural analysis using synchrotron nanotomography reveals that the inorganic particles are highly aggregated. The aggregation size grows with inorganic content and the largest percolating clusters measured for 5 vol%, 15 vol% and 50 vol% were ∼12 μm3, 206 μm3, and 324 μm3, respectively. Enhanced transport in hybrid electrolytes is shown to be due to polymer|particle (Al-LLZO) interactions and ionic conductivity is directly related to the accessible surface area of the inorganic particles within the electrolyte. Ordered and well-dispersed structures are ideal for next generation hybrid solid electrolytes.

Original languageEnglish
Pages (from-to)23914-23921
Number of pages8
JournalJournal of Materials Chemistry A
Volume7
Issue number41
DOIs
StatePublished - 2019
Externally publishedYes

Funding

The authors were supported by the National Science Foundation under grant No. 1847029. The authors acknowledge the Vanderbilt Institute of Nanoscience and Engineering (VINSE) for access to their shared characterization facilities. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

FundersFunder number
Advanced Photon Source
DOE Office of Science
Office of Science User Facility operated
National Science Foundation1847029
U.S. Department of Energy
Argonne National Laboratory

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