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<p>Quasi-solid-state electrolytes, which integrate the safety characteristics of inorganic materials, the flexibility of polymers, and the high ionic conductivity of liquid electrolytes, represent a transitional solution for high-energy-density lithium batteries. However, the mechanisms by which inorganic fillers enhance multiphase interfacial conduction remain inadequately understood. In this work, we synthesized composite quasi-solid-state electrolytes with high inorganic content to investigate interfacial phenomena and achieve enhanced electrode interface stability. Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> particles, through surface anion anchoring, improve Li<sup>+</sup> transference numbers and facilitate partial dissociation of solvated Li<sup>+</sup> structures, resulting in superior ion transport kinetics that achieve an ionic conductivity of 0.51&#xa0;mS&#xa0;cm<sup>−1</sup> at room temperature. The high mass fraction of inorganic components additionally promotes the formation of more stable interfacial layers, enabling lithium-symmetric cells to operate without short-circuiting for 6000&#xa0;h at 0.1&#xa0;mA&#xa0;cm<sup>−2</sup>. Furthermore, this system demonstrates exceptional stability in 5&#xa0;V-class lithium metal full cells, maintaining 80.5% capacity retention over 200 cycles at 0.5C. These findings guide the role of inorganic interfaces in composite electrolytes and demonstrate their potential for advancing high-voltage lithium battery technology.</p>

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Enhancement of Li+ Transport Through Intermediate Phase in High-Content Inorganic Composite Quasi-Solid-State Electrolytes

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年6月11日

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  • Haoyang Yuan,
  • Wenjun Lin,
  • Changhao Tian,
  • Mihaela Buga,
  • Tao Huang,
  • Aishui Yu

摘要

Quasi-solid-state electrolytes, which integrate the safety characteristics of inorganic materials, the flexibility of polymers, and the high ionic conductivity of liquid electrolytes, represent a transitional solution for high-energy-density lithium batteries. However, the mechanisms by which inorganic fillers enhance multiphase interfacial conduction remain inadequately understood. In this work, we synthesized composite quasi-solid-state electrolytes with high inorganic content to investigate interfacial phenomena and achieve enhanced electrode interface stability. Li1.3Al0.3Ti1.7(PO4)3 particles, through surface anion anchoring, improve Li+ transference numbers and facilitate partial dissociation of solvated Li+ structures, resulting in superior ion transport kinetics that achieve an ionic conductivity of 0.51 mS cm−1 at room temperature. The high mass fraction of inorganic components additionally promotes the formation of more stable interfacial layers, enabling lithium-symmetric cells to operate without short-circuiting for 6000 h at 0.1 mA cm−2. Furthermore, this system demonstrates exceptional stability in 5 V-class lithium metal full cells, maintaining 80.5% capacity retention over 200 cycles at 0.5C. These findings guide the role of inorganic interfaces in composite electrolytes and demonstrate their potential for advancing high-voltage lithium battery technology.