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<p>Lithium halide solid electrolytes have garnered significant attention owing to their high ionic conductivity and positive electrode compatibility. However, achieving target ionic conductivity typically requires high lithium concentration (&gt;4.3 wt%) within optimal structure, which raises costs and exacerbates air sensitivity. Here, we leverage anion clusters to synthesize a series of amorphous halide electrolytes <i>x</i>Li<sub>2</sub>SO<sub>4</sub>-ZrCl<sub>4</sub>, with optimal ionic conductivities of 1.5 mS cm<sup>-1</sup> at 30 °C and a significantly reduced lithium content of 2.4 wt%, alongside good air stability. Through neutron/synchrotron X-ray experiments, first-principles calculations and machine learning-accelerated molecular dynamics simulations, we reveal a disordered backbone of [Zr<sub>a</sub>Cl<sub>4a</sub>(SO<sub>4</sub>)]<sup>2-</sup> (1 ≤ a ≤ 4) that enables fast Li-ion diffusion via under-coordinated oxygen sites. All-solid-state lithium batteries employing these electrolytes and LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> positive electrode exhibit 81.1% capacity retention after 1400 cycles at 1 C (60 min) and 30 °C. Our findings reveal anion-cluster chemistry as an approach that transforms solid electrolyte design for advanced batteries, bridging materials science with practical energy storage innovation.</p>

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Polyanion-stabilized amorphous halide electrolytes with low lithium content for all-solid-state lithium batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月28日

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  • Wen Tang,
  • Feilong Wang,
  • Shuaika Liang,
  • Fiaz Hussain,
  • Jo-chi Tseng,
  • Pengcheng Yu,
  • Jiuwei Lei,
  • Hailun Jin,
  • Chunlei Zhao,
  • Haochang Zhang,
  • Zhepu Shi,
  • Ying Li,
  • Wen Yin,
  • Fucheng Ren,
  • Shuo Wang,
  • Zi‑Feng Ma,
  • Xueliang Sun,
  • Wei Xia

摘要

Lithium halide solid electrolytes have garnered significant attention owing to their high ionic conductivity and positive electrode compatibility. However, achieving target ionic conductivity typically requires high lithium concentration (>4.3 wt%) within optimal structure, which raises costs and exacerbates air sensitivity. Here, we leverage anion clusters to synthesize a series of amorphous halide electrolytes xLi2SO4-ZrCl4, with optimal ionic conductivities of 1.5 mS cm-1 at 30 °C and a significantly reduced lithium content of 2.4 wt%, alongside good air stability. Through neutron/synchrotron X-ray experiments, first-principles calculations and machine learning-accelerated molecular dynamics simulations, we reveal a disordered backbone of [ZraCl4a(SO4)]2- (1 ≤ a ≤ 4) that enables fast Li-ion diffusion via under-coordinated oxygen sites. All-solid-state lithium batteries employing these electrolytes and LiNi0.8Co0.1Mn0.1O2 positive electrode exhibit 81.1% capacity retention after 1400 cycles at 1 C (60 min) and 30 °C. Our findings reveal anion-cluster chemistry as an approach that transforms solid electrolyte design for advanced batteries, bridging materials science with practical energy storage innovation.