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<p>UCl₃-based halide solid electrolytes have garnered increasing interest for application in all-solid-state batteries, yet their structural characteristics, chemical composition, and ion transport mechanisms remain under debate. These uncertainties hamper their rational design and broader application. Taking PrCl<sub>3</sub> as a model system, we present a comprehensive structural investigation and reveal that foreign cations (e.g., Ta<sup>5+</sup>, Zr<sup>4+</sup> and In<sup>3+</sup>) preferentially reside in amorphous matrix rather than substituting for Pr³⁺ in crystalline PrCl₃, owing to substantial mismatches in both ionic radii and coordination numbers. Importantly, the dominant pathway for fast Li⁺ conduction lies within the amorphous phase, rather than the PrCl₃ nanocrystals or their interfacial regions. Guided by these insights, Li<sub>0.5</sub>Pr<sub>0.455</sub>Ta<sub>0.179</sub>Zr<sub>0.06</sub>Cl<sub>3</sub> is rationally designed, realizing high ionic conductivity (3.10 mS cm⁻¹) and a low activation energy (0.236 eV). These improved ion-conducting properties enables battery with a capacity retention of 71.7% at 20 mA g<sup>-1</sup> and –20 °C, and a prolonged cycle life of 1350 cycles at 100 or 200 mA g<sup>-1</sup> and –10 °C. These results underscore the critical role of amorphous phase engineering in halide electrolytes and the potential of UCl₃-type systems for low-temperature all-solid-state batteries.</p>

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Unraveling the Foreign-Cation Effect in UCl₃-Type Halide Solid Electrolytes for Low-Temperature All-Solid-State Batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月21日

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  • Pushun Lu,
  • Zhimin Zhou,
  • Shiyue Cao,
  • Jiamin Fu,
  • Weiping Li,
  • Kaiyong Tuo,
  • Suze Liang,
  • Jian Hong,
  • Jiuwei Lei,
  • Jiaxu Zhang,
  • Ziqing Wang,
  • Shutao Zhang,
  • Guantai Hu,
  • Chao Wang,
  • Tingting Liu,
  • Suting Weng,
  • Wei Xia,
  • Xuefeng Wang,
  • Xueliang Sun,
  • Changhong Wang

摘要

UCl₃-based halide solid electrolytes have garnered increasing interest for application in all-solid-state batteries, yet their structural characteristics, chemical composition, and ion transport mechanisms remain under debate. These uncertainties hamper their rational design and broader application. Taking PrCl3 as a model system, we present a comprehensive structural investigation and reveal that foreign cations (e.g., Ta5+, Zr4+ and In3+) preferentially reside in amorphous matrix rather than substituting for Pr³⁺ in crystalline PrCl₃, owing to substantial mismatches in both ionic radii and coordination numbers. Importantly, the dominant pathway for fast Li⁺ conduction lies within the amorphous phase, rather than the PrCl₃ nanocrystals or their interfacial regions. Guided by these insights, Li0.5Pr0.455Ta0.179Zr0.06Cl3 is rationally designed, realizing high ionic conductivity (3.10 mS cm⁻¹) and a low activation energy (0.236 eV). These improved ion-conducting properties enables battery with a capacity retention of 71.7% at 20 mA g-1 and –20 °C, and a prolonged cycle life of 1350 cycles at 100 or 200 mA g-1 and –10 °C. These results underscore the critical role of amorphous phase engineering in halide electrolytes and the potential of UCl₃-type systems for low-temperature all-solid-state batteries.