Synergistic Interface Stability and High Room-Temperature Ionic Conductivity for Wide-Temperature All-Solid-State Batteries Based on Li6+xSixSb1-xS5I Electrolytes
Abstract
Solid-state lithium-ion batteries (LIBs) are increasingly recognized for their exceptional energy density and safety. However, their widespread adoption is challenged by persistent issues such as thermal and electrochemical instability, dendrite formation, and limited compatibility with high-voltage cathodes. Sulfide-based solid electrolytes (SEs), particularly iodide argyrodites, offer outstanding ionic conductivity and stability; however, their practical application is constrained by the formation of space-charge layers, slow ion transport, and susceptibility to dendrite penetration. To address these challenges, we synthesized a novel Li6.6Si0.6Sb0.4S5I argyrodite electrolyte via ball milling and heat treatment, achieving a remarkable room-temperature ionic conductivity of 9.9 mS cm^-1. The electrolyte was integrated with a LiNbO3-coated LiNi0.7Co0.1Mn0.2O2 cathode to form an all-solid-state battery, which demonstrated an initial discharge capacity of 171.2 mAh g^-1, retained 84.2% of its capacity after 200 cycles at 0.5C, and maintained stable cycling across a broad temperature range from -20 degrees C to 60 degrees C. Our study shows that tailored electrolyte composition and a composite cathode configuration significantly enhance cycling stability and improve interfacial protection. These findings highlight the potential of Si-doped antimony-type iodide argyrodites for next-generation high-performance all-solid-state batteries, offering durable operation under diverse thermal conditions.
Versions
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BibTeX
@misc{ming2026synergistic,
title = {{Synergistic Interface Stability and High Room-Temperature Ionic Conductivity for Wide-Temperature All-Solid-State Batteries Based on Li6+xSixSb1-xS5I Electrolytes}},
author = {Liang Ming and Qizhiran Sun and Guanping Xu and Muqing Su and Enyan Zhao and Wenzhe Gu and Weng-Fu Io and Kwun Nam Hui and Chuang Yu and Hai-Feng Li},
howpublished = {arXiv},
year = {2026},
month = jul,
doi = {10.48550/arxiv.2607.19664},
eprint = {2607.19664},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2607.19664},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Synergistic Interface Stability and High Room-Temperature Ionic Conductivity for Wide-Temperature All-Solid-State Batteries Based on Li6+xSixSb1-xS5I Electrolytes
AU - Liang Ming
AU - Qizhiran Sun
AU - Guanping Xu
AU - Muqing Su
AU - Enyan Zhao
AU - Wenzhe Gu
AU - Weng-Fu Io
AU - Kwun Nam Hui
AU - Chuang Yu
AU - Hai-Feng Li
PY - 2026
DA - 2026/07/22
PB - arXiv
DO - 10.48550/arxiv.2607.19664
UR - https://arxiv.org/abs/2607.19664
AB - Solid-state lithium-ion batteries (LIBs) are increasingly recognized for their exceptional energy density and safety. However, their widespread adoption is challenged by persistent issues such as thermal and electrochemical instability, dendrite formation, and limited compatibility with high-voltage cathodes. Sulfide-based solid electrolytes (SEs), particularly iodide argyrodites, offer outstanding ionic conductivity and stability; however, their practical application is constrained by the formation of space-charge layers, slow ion transport, and susceptibility to dendrite penetration. To address these challenges, we synthesized a novel Li6.6Si0.6Sb0.4S5I argyrodite electrolyte via ball milling and heat treatment, achieving a remarkable room-temperature ionic conductivity of 9.9 mS cm^-1. The electrolyte was integrated with a LiNbO3-coated LiNi0.7Co0.1Mn0.2O2 cathode to form an all-solid-state battery, which demonstrated an initial discharge capacity of 171.2 mAh g^-1, retained 84.2% of its capacity after 200 cycles at 0.5C, and maintained stable cycling across a broad temperature range from -20 degrees C to 60 degrees C. Our study shows that tailored electrolyte composition and a composite cathode configuration significantly enhance cycling stability and improve interfacial protection. These findings highlight the potential of Si-doped antimony-type iodide argyrodites for next-generation high-performance all-solid-state batteries, offering durable operation under diverse thermal conditions.
ER -