Faculty, Staff and Student Publications

Language

English

Publication Date

5-21-2024

Journal

Nature Communications

DOI

10.1038/s41467-024-48712-4

PMID

38773104

PMCID

PMC11109254

PubMedCentral® Posted Date

5-21-2024

PubMedCentral® Full Text Version

Post-print

Abstract

To enable high performance of all solid-state batteries, a catholyte should demonstrate high ionic conductivity, good compressibility and oxidative stability. Here, a LaCl3-based Na+ superionic conductor (Na1−xZrxLa1−xCl4) with high ionic conductivity of 2.9 × 10−4 S cm−1 (30 °C), good compressibility and high oxidative potential (3.80 V vs. Na2Sn) is prepared via solid state reaction combining mechanochemical method. X-ray diffraction reveals a hexagonal structure (P63/m) of Na1−xZrxLa1−xCl4, with Na+ ions forming a one-dimensional diffusion channel along the c-axis. First-principle calculations combining with X-ray absorption fine structure characterization etc. reveal that the ionic conductivity of Na1−xZrxLa1−xCl4 is mainly determined by the size of Na+-channels and the Na+/La3+ mixing in the one-dimensional diffusion channels. When applied as a catholyte, the NaCrO2||Na0.7Zr0.3La0.7Cl4||Na3PS4||Na2Sn all-solid-state batteries demonstrate an initial capacity of 114 mA h g−1 and 88% retention after 70 cycles at 0.3 C. In addition, a high capacity of 94 mA h g−1 can be maintained at 1 C current density.

Published Open-Access

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