LaCl3-based sodium halide solid electrolytes with high ionic conductivity for all-solid-state batteries

Chengyu Fu, Yifan Li, Wenjie Xu, Xuyong Feng (), Weijian Gu, Jue Liu, Wenwen Deng, Wei Wang, A. M. Milinda Abeykoon, Laisuo Su, Lingyun Zhu, Xiaojun Wu and Hongfa Xiang ()
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Chengyu Fu: Hefei University of Technology
Yifan Li: University of Science and Technology of China
Wenjie Xu: University of Science and Technology of China
Xuyong Feng: Hefei University of Technology
Weijian Gu: Hefei University of Technology
Jue Liu: Oak Ridge National Laboratory
Wenwen Deng: Suzhou University of Science and Technology
Wei Wang: CAS Key Laboratory of Design and Assembly of Functional Nanostructures
A. M. Milinda Abeykoon: National Synchrotron Light Source II, Upton
Laisuo Su: University of Texas at Dallas
Lingyun Zhu: School of Materials Science and Engineering
Xiaojun Wu: University of Science and Technology of China
Hongfa Xiang: Hefei University of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-48712-4

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