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<p>Solid electrolytes are promising candidates for safe, high-energy battery systems. Composite solid electrolytes, in particular, hold the potential to combine high ionic conductivity with stable electrode interfaces. However, a fundamental trade-off often exists between ion conduction and mechanical properties. Here we present a composite solid electrolyte design that decouples ion conduction from mechanical flexibility, achieving a high ionic conductivity of 10.2 mS cm<sup>−1</sup> at 25 °C while maintaining close mechanical contact with the electrode. The composite architecture consists of alternating layers of perpendicularly aligned (PA) Li<sub>0.3</sub>Cd<sub>0.85</sub>PS<sub>3</sub> nanosheets, to establish continuous superionic conduction pathways, and Li-containing polyethylene oxide (PEO) layers, to ensure flexibility and interfacial compatibility. At 25 °C, this PA-Li<sub>0.3</sub>Cd<sub>0.85</sub>PS<sub>3</sub>/PEO electrolyte enables Li||LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> coin cells (stack pressure during assembly &lt;0.5 MPa) to retain 92% discharge capacity after 600 cycles at 0.2 mA cm<sup>−2</sup>, with an average cycling Coulombic efficiency of 99.9%, and also facilitates practical use of pressure-less (stack pressure &lt;0.1 MPa) Li||LiFePO<sub>4</sub> pouch cells. This composite design strategy is further validated by substituting Cd with Mn in the inorganic sulfide nanosheets to produce a PA-Li<sub>0.46</sub>Mn<sub>0.77</sub>PS<sub>3</sub>/PEO electrolyte, exhibiting an ionic conductivity of 6.1 mS cm<sup>−1</sup> at 25 °C and good mechanical flexibility.</p>

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Superionic composite electrolytes with continuously perpendicular-aligned pathways for pressure-less all-solid-state lithium batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月15日

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  • Xuexia Lan,
  • Zhen Li,
  • Chao Zhao,
  • Ziyong Li,
  • Yi Zeng,
  • Yuxuan Liu,
  • Qiutan Liu,
  • Xiangjie Li,
  • Lili Zhang,
  • Zhengjie Chen,
  • Xiaoxiao Feng,
  • Jiahong Wang,
  • Feng Ding,
  • Renzong Hu,
  • Jing Peng,
  • Hui-Ming Cheng

摘要

Solid electrolytes are promising candidates for safe, high-energy battery systems. Composite solid electrolytes, in particular, hold the potential to combine high ionic conductivity with stable electrode interfaces. However, a fundamental trade-off often exists between ion conduction and mechanical properties. Here we present a composite solid electrolyte design that decouples ion conduction from mechanical flexibility, achieving a high ionic conductivity of 10.2 mS cm−1 at 25 °C while maintaining close mechanical contact with the electrode. The composite architecture consists of alternating layers of perpendicularly aligned (PA) Li0.3Cd0.85PS3 nanosheets, to establish continuous superionic conduction pathways, and Li-containing polyethylene oxide (PEO) layers, to ensure flexibility and interfacial compatibility. At 25 °C, this PA-Li0.3Cd0.85PS3/PEO electrolyte enables Li||LiNi0.8Co0.1Mn0.1O2 coin cells (stack pressure during assembly <0.5 MPa) to retain 92% discharge capacity after 600 cycles at 0.2 mA cm−2, with an average cycling Coulombic efficiency of 99.9%, and also facilitates practical use of pressure-less (stack pressure <0.1 MPa) Li||LiFePO4 pouch cells. This composite design strategy is further validated by substituting Cd with Mn in the inorganic sulfide nanosheets to produce a PA-Li0.46Mn0.77PS3/PEO electrolyte, exhibiting an ionic conductivity of 6.1 mS cm−1 at 25 °C and good mechanical flexibility.