Journal
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
Volume 105, Issue 10, Pages 6175-6183Publisher
WILEY
DOI: 10.1111/jace.18576
Keywords
electrochemical properties; high-entropy ceramic; Li-garnet; sintering; solid-state electrolyte
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Funding
- National Space Grant College and Fellowship Program
- Wisconsin Space Grant Consortium
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This paper demonstrated the processing and potential application of high-entropy Li-garnet LLZNTH in lithium batteries. The prepared sample showed excellent crystallinity and conductivity, laying a solid foundation for battery performance improvement.
In this paper, we demonstrated the processing of Li7La3Zr0.5Nb0.5Ta0.5Hf0.5O12 (LLZNTH) high-entropy Li-garnet with promising properties for lithium batteries. We first synthesized the LLZNTH Li-garnet powders which have a single cubic garnet phase (space group: Ia3 over bar d$Ia\bar 3d$; No. 230) without any secondary phases as well as uniform elements distributions. The prepared powders were further densified to a relative density of similar to 94% with well-crystallized grains and good contact with the neighboring grains. Minimal grain growth can be observed in the sintering time range from 8 to 20 h, which is likely due to the sluggish effects of high-entropy compounds. The sample also maintains the cubic garnet phase along with uniform elements distribution after sintering. Electrochemical characterizations indicate that the densified sample has an adequate ionic conductivity of 4.67 x 10(-4) S cm(-1) at room temperature, a low activation energy of 0.25 eV, and a low electronic conductivity in the order of 10(-8) S cm(-1). The significance of designing high-entropy electrolyte is further discussed.
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