Ultrahigh Ionic Conductivity in Halide Electrolytes Enabled by Anion Framework Flexibility Engineering

Chloride-based solid electrolytes are promising for all-solid-state batteries owing to their favorable oxidative stability and mechanical deformability. However, most chlorides exhibit only moderate ionic conductivity, primarily due to the restricted ion transport imposed by their close-packed anion frameworks. In this work, we address this limitation by enhancing anion framework flexibility through lowering the negative charge on chloride anions, achieved by incorporating high-valent, highly electronegative cations, accompanied by a reduction in the lithium content. Computations reveal that this strategy substantially decreases the energy barriers for anion reorientation, leading to a more flexible anion…

• NN
  National Natural Science Foundation of China

  Awards: U22A20439, 52472272
• SF
  Shenzhen Fundamental Research Program

  Award: JCYJ20220530150200001
• SA
  Science and Technology Planning Project of Guangdong Province

  Award: 2023B0909060004
• SS
  Shenzhen Science and Technology Innovation Program

  Award: RCYX20221008092929074