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<p>Although Li-ion conductivity has been the primary focus during decades of solid-electrolyte research, the mechanical compliance is equally important. For most state-of-the-art solid electrolytes, the mechanical compliance is characterized by the hardness above 1 GPa and Young’s modulus above 15 GPa. Here, we report a particularly compliant solid electrolyte, 1.4Li<sub>2</sub>O-0.75ZrCl<sub>4</sub>-0.25AlCl<sub>3</sub>, whose hardness and Young’s modulus reach 0.22 and 1.41 GPa, respectively. Meanwhile, it shows an ionic conductivity of 2.55 mS cm<sup>−1</sup> at 25 °C and an estimated cost of $43.70 L<sup>−1</sup>, considerably lower than that of the Li<sub>2</sub>ZrCl<sub>6</sub> solid electrolyte known for cost-effectiveness ($140.01 L<sup>−1</sup>). The improved mechanical compliance and fast Li-ion transport in 1.4Li<sub>2</sub>O-0.75ZrCl<sub>4</sub>-0.25AlCl<sub>3</sub> enable decent cell performance. With high positive electrode active material loading above 20 mg cm<sup>−2</sup>, these two types of cells achieve areal capacities of 3.62 mAh cm<sup>−2</sup> (85.78% capacity retention) and 3.92 mAh cm<sup>−2</sup> (90.11% capacity retention), respectively, after 100 cycles under 0.1 C at 25 °C. The simultaneous achievement of highly competitive mechanical compliance, Li-ion conductivity, and cost-effectiveness in 1.4Li<sub>2</sub>O-0.75ZrCl<sub>4</sub>-0.25AlCl<sub>3</sub> have the potential to pave the way for the realization of commercial, practical all-solid-state Li batteries.</p>

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Mechanically compliant and cost-effective 1.4Li2O-0.75ZrCl4-0.25AlCl3 solid electrolyte for all-solid-state batteries with improved cycling stability

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月8日

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  • Lv Hu,
  • Yaolong He,
  • Dong Wang,
  • Wanxia Li,
  • Jingming Yao,
  • Xiaolong Zhang,
  • Jinfeng Zhu,
  • Huaican Chen,
  • Wen Yin,
  • Yanru Wang,
  • Kejun Yan,
  • Jinzhu Wang,
  • Hui Li,
  • Fang Chen,
  • Yating Liu,
  • Junqi Lai,
  • Qi Chen,
  • Jie Ma,
  • Shuhong Jiao,
  • Guorui Wang,
  • Siqi Shi,
  • Liwei Chen,
  • Jianyu Huang,
  • Cheng Ma

摘要

Although Li-ion conductivity has been the primary focus during decades of solid-electrolyte research, the mechanical compliance is equally important. For most state-of-the-art solid electrolytes, the mechanical compliance is characterized by the hardness above 1 GPa and Young’s modulus above 15 GPa. Here, we report a particularly compliant solid electrolyte, 1.4Li2O-0.75ZrCl4-0.25AlCl3, whose hardness and Young’s modulus reach 0.22 and 1.41 GPa, respectively. Meanwhile, it shows an ionic conductivity of 2.55 mS cm−1 at 25 °C and an estimated cost of $43.70 L−1, considerably lower than that of the Li2ZrCl6 solid electrolyte known for cost-effectiveness ($140.01 L−1). The improved mechanical compliance and fast Li-ion transport in 1.4Li2O-0.75ZrCl4-0.25AlCl3 enable decent cell performance. With high positive electrode active material loading above 20 mg cm−2, these two types of cells achieve areal capacities of 3.62 mAh cm−2 (85.78% capacity retention) and 3.92 mAh cm−2 (90.11% capacity retention), respectively, after 100 cycles under 0.1 C at 25 °C. The simultaneous achievement of highly competitive mechanical compliance, Li-ion conductivity, and cost-effectiveness in 1.4Li2O-0.75ZrCl4-0.25AlCl3 have the potential to pave the way for the realization of commercial, practical all-solid-state Li batteries.