Selective Oxygen Doping of Li <sub>6.6</sub> Si <sub>0.6</sub> Sb <sub>0.4</sub> S <sub>5</sub> I Electrolyte for Enhanced Air Stability and Electrochemical Performance

The argyrodite electrolyte Li<sub>6.6</sub>Si<sub>0.6</sub>Sb<sub>0.4</sub>S<sub>5</sub>I has garnered significant interest due to its high ionic conductivity of 9.0 mS cm<sup>-1</sup>. However, its integration into composite cathodes is hindered by poor chemical and electrochemical stability, limiting its practical application. This study investigates an O doping strategy to enhance the overall performance of Li<sub>6.6</sub>Si<sub>0.6</sub>Sb<sub>0.4</sub>S<sub>5</sub>I. In contrast to previous studies, a comparative analysis of two different oxygen sources Li<sub>2</sub>O and Sb<sub>2</sub>O<sub>5</sub> is conducted. The results demonstrate that the electrochemical stability of the material obviously improves when Li<sub>2</sub>O is used as the O source, while its air stability significantly enhances when Sb<sub>2</sub>O<sub>5</sub> is used. Furthermore, Li<sub>6.6</sub>Si<sub>0.6</sub>Sb<sub>0.4</sub>S<sub>5</sub>I (and Li<sub>6.6</sub>Si<sub>0.6</sub>Sb<sub>0.4</sub>S<sub>4.9</sub>IO<sub>0.1</sub>-Li<sub>2</sub>O) is combined with Li<sub>3</sub>InCl<sub>6</sub> (and Li<sub>3.25</sub>InCl<sub>5.75</sub>O<sub>0.25</sub>) to fabricate different separator configurations. Through aging tests, the optimal separator configuration, Li<sub>3.25</sub>InCl<sub>5.75</sub>O<sub>0.25</sub>/Li<sub>6.6</sub>Si<sub>0.6</sub>Sb<sub>0.4</sub>S<sub>4.9</sub>IO<sub>0.1</sub>-Li<sub>2</sub>O, is found. Batteries assembled with this separator exhibit stable performance over 800 cycles at an upper cutoff voltage of 3.9 V (vs. Li-In), while maintaining an excellent capacity retention rate of 80.2%.

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Journal
ChemSusChem
Published
2025-09-18
DOI
https://doi.org/10.1002/cssc.202501611
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
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article

Selective Oxygen Doping of Li 6.6 Si 0.6 Sb 0.4 S 5 I Electrolyte for Enhanced Air Stability and Electrochemical Performance

Chuang Yu, Miao Deng, Ziling Jiang, Qiyue Luo et al.
ChemSusChem
Advancements in Battery Materials
article

Selective Oxygen Doping of Li 6.6 Si 0.6 Sb 0.4 S 5 I Electrolyte for Enhanced Air Stability and Electrochemical Performance

Chuang Yu, Miao Deng, Ziling Jiang, Qiyue Luo, Siwu Li, Lin Li, Chen Liu, Long Chen, Ziyu Lu, Jie Yang
article en

Abstract

The argyrodite electrolyte Li<sub>6.6</sub>Si<sub>0.6</sub>Sb<sub>0.4</sub>S<sub>5</sub>I has garnered significant interest due to its high ionic conductivity of 9.0 mS cm<sup>-1</sup>. However, its integration into composite cathodes is hindered by poor chemical and electrochemical stability, limiting its practical application. This study investigates an O doping strategy to enhance the overall performance of Li<sub>6.6</sub>Si<sub>0.6</sub>Sb<sub>0.4</sub>S<sub>5</sub>I. In contrast to previous studies, a comparative analysis of two different oxygen sources Li<sub>2</sub>O and Sb<sub>2</sub>O<sub>5</sub> is conducted. The results demonstrate that the electrochemical stability of the material obviously improves when Li<sub>2</sub>O is used as the O source, while its air stability significantly enhances when Sb<sub>2</sub>O<sub>5</sub> is used. Furthermore, Li<sub>6.6</sub>Si<sub>0.6</sub>Sb<sub>0.4</sub>S<sub>5</sub>I (and Li<sub>6.6</sub>Si<sub>0.6</sub>Sb<sub>0.4</sub>S<sub>4.9</sub>IO<sub>0.1</sub>-Li<sub>2</sub>O) is combined with Li<sub>3</sub>InCl<sub>6</sub> (and Li<sub>3.25</sub>InCl<sub>5.75</sub>O<sub>0.25</sub>) to fabricate different separator configurations. Through aging tests, the optimal separator configuration, Li<sub>3.25</sub>InCl<sub>5.75</sub>O<sub>0.25</sub>/Li<sub>6.6</sub>Si<sub>0.6</sub>Sb<sub>0.4</sub>S<sub>4.9</sub>IO<sub>0.1</sub>-Li<sub>2</sub>O, is found. Batteries assembled with this separator exhibit stable performance over 800 cycles at an upper cutoff voltage of 3.9 V (vs. Li-In), while maintaining an excellent capacity retention rate of 80.2%.

ChemSusChemVol. 18(20)
East China University of Science and Technology (CN), Xidian University (CN), Huazhong University of Science and Technology (CN)
Openalex Percentile: Top 75%
Advancements in Battery Materials
DOISourceOpenAlex
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