TY - JOUR
T1 - LaCl3-based sodium halide solid electrolytes with high ionic conductivity for all-solid-state batteries
AU - Fu, Chengyu
AU - Li, Yifan
AU - Xu, Wenjie
AU - Feng, Xuyong
AU - Gu, Weijian
AU - Liu, Jue
AU - Deng, Wenwen
AU - Wang, Wei
AU - Abeykoon, A. M.Milinda
AU - Su, Laisuo
AU - Zhu, Lingyun
AU - Wu, Xiaojun
AU - Xiang, Hongfa
N1 - Publisher Copyright:
© The Author(s) 2024.
PY - 2024/12
Y1 - 2024/12
N2 - 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 × 10−4S 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.
AB - 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 × 10−4S 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.
UR - http://www.scopus.com/inward/record.url?scp=85193983057&partnerID=8YFLogxK
U2 - 10.1038/s41467-024-48712-4
DO - 10.1038/s41467-024-48712-4
M3 - Article
C2 - 38773104
AN - SCOPUS:85193983057
SN - 2041-1723
VL - 15
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 4315
ER -