Recovering the Ionic Conductivity of Oxygen‐Doped Li3.25InCl5.75O0.25 Electrolyte through Heat Treatment: Reconstructing the Structure Damaged by Moisture

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Hauptverfasser: Miao Deng, Shiyu Liu, Siwu Li, Wenwen Hu, Ziyu Lu, Ziling Jiang, Lin Li, Kunpeng Tang, Lei Shi, Qiyue Luo, Haitao Li, Jie Yang, Chen Liu, Chuang Yu
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author Miao Deng
Shiyu Liu
Siwu Li
Wenwen Hu
Ziyu Lu
Ziling Jiang
Lin Li
Kunpeng Tang
Lei Shi
Qiyue Luo
Haitao Li
Jie Yang
Chen Liu
Chuang Yu
author_facet Miao Deng
Shiyu Liu
Siwu Li
Wenwen Hu
Ziyu Lu
Ziling Jiang
Lin Li
Kunpeng Tang
Lei Shi
Qiyue Luo
Haitao Li
Jie Yang
Chen Liu
Chuang Yu
Miao Deng
Shiyu Liu
Siwu Li
Wenwen Hu
Ziyu Lu
Ziling Jiang
Lin Li
Kunpeng Tang
Lei Shi
Qiyue Luo
Haitao Li
Jie Yang
Chen Liu
Chuang Yu
collection Wiley Open Access
contents Recovering the Ionic Conductivity of Oxygen‐Doped Li3.25InCl5.75O0.25 Electrolyte through Heat Treatment: Reconstructing the Structure Damaged by Moisture Miao Deng Shiyu Liu Siwu Li Wenwen Hu Ziyu Lu Ziling Jiang Lin Li Kunpeng Tang Lei Shi Qiyue Luo Haitao Li Jie Yang Chen Liu Chuang Yu ChemSusChem Metal halide solid‐state electrolytes, especially oxyhalides, possess a broad electrochemical stability window, optimized interfacial compatibility, and suitability for high‐voltage cathode materials, making them promising candidates for next‐generation all‐solid‐state lithium metal batteries (ASSBs). However, their commercialization is still hindered by several critical technical challenges, especially the significant moisture sensitivity. In this study, the damage to the structure and electrochemical performance of Li3.25InCl5.75O0.25 electrolyte caused by humid air exposure is evaluated, and a heat treatment is proposed and proven effective in recovering the damage. A series of spectroscopic experiments reveal that humid air exposure triggers hydrolysis and hydration reactions in Li3.25InCl5.75O0.25, leading to lattice contraction, that significantly hindering lithium‐ion transport. After thermal processing at 400 °C, the lattice is reconstructed, and the ionic conductivity reaches an 83.5% recovery (7.6 × 10−4 S cm−1 vs pristine 9.1 × 10−4 S cm−1). ASSBs based on the repaired electrolyte demonstrate excellent cycling and rate performance, retaining 76.1% capacity after 1000 cycles at 2C. The ASSBs also retains substantial capacity output under extreme temperatures (60 °C/–20 °C), further verifying the comprehensive enhancement of the heat treatment strategy on electrochemical performance and its engineering application potential. 10.1002/cssc.202500495 http://onlinelibrary.wiley.com/termsAndConditions#vor
doi_str_mv 10.1002/cssc.202500495
format Artículo Open Access
id wiley_oa_10_1002_cssc_202500495
institution Wiley Open Access
license_str_mv http://onlinelibrary.wiley.com/termsAndConditions#vor
publishDate 2025
publisher Wiley
record_format wiley_oa
spellingShingle Recovering the Ionic Conductivity of Oxygen‐Doped Li3.25InCl5.75O0.25 Electrolyte through Heat Treatment: Reconstructing the Structure Damaged by Moisture
Miao Deng
Shiyu Liu
Siwu Li
Wenwen Hu
Ziyu Lu
Ziling Jiang
Lin Li
Kunpeng Tang
Lei Shi
Qiyue Luo
Haitao Li
Jie Yang
Chen Liu
Chuang Yu
ChemSusChem
Recovering the Ionic Conductivity of Oxygen‐Doped Li3.25InCl5.75O0.25 Electrolyte through Heat Treatment: Reconstructing the Structure Damaged by Moisture Miao Deng Shiyu Liu Siwu Li Wenwen Hu Ziyu Lu Ziling Jiang Lin Li Kunpeng Tang Lei Shi Qiyue Luo Haitao Li Jie Yang Chen Liu Chuang Yu ChemSusChem Metal halide solid‐state electrolytes, especially oxyhalides, possess a broad electrochemical stability window, optimized interfacial compatibility, and suitability for high‐voltage cathode materials, making them promising candidates for next‐generation all‐solid‐state lithium metal batteries (ASSBs). However, their commercialization is still hindered by several critical technical challenges, especially the significant moisture sensitivity. In this study, the damage to the structure and electrochemical performance of Li3.25InCl5.75O0.25 electrolyte caused by humid air exposure is evaluated, and a heat treatment is proposed and proven effective in recovering the damage. A series of spectroscopic experiments reveal that humid air exposure triggers hydrolysis and hydration reactions in Li3.25InCl5.75O0.25, leading to lattice contraction, that significantly hindering lithium‐ion transport. After thermal processing at 400 °C, the lattice is reconstructed, and the ionic conductivity reaches an 83.5% recovery (7.6 × 10−4 S cm−1 vs pristine 9.1 × 10−4 S cm−1). ASSBs based on the repaired electrolyte demonstrate excellent cycling and rate performance, retaining 76.1% capacity after 1000 cycles at 2C. The ASSBs also retains substantial capacity output under extreme temperatures (60 °C/–20 °C), further verifying the comprehensive enhancement of the heat treatment strategy on electrochemical performance and its engineering application potential. 10.1002/cssc.202500495 http://onlinelibrary.wiley.com/termsAndConditions#vor
title Recovering the Ionic Conductivity of Oxygen‐Doped Li3.25InCl5.75O0.25 Electrolyte through Heat Treatment: Reconstructing the Structure Damaged by Moisture
topic ChemSusChem
url https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cssc.202500495