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<p>The development of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) solid electrolytes is challenged by the unstable Li/LLZO interface during lithium stripping and plating processes, which impedes interfacial charge transport and accelerates lithium dendrite growth. Here, a freestanding ultrathin Li-Li<sub>0.3</sub>La<sub>0.5</sub>TiO<sub>3</sub> (LLTO) composite anode with a three-dimensional interconnected mixed ionic/electronic conducting LLTO framework was developed. The mixed ionic/electronic conduction of LLTO arises from the <i>in-situ</i> reduction of transition metal ions (Ti<sup>4+</sup>) by metallic lithium. The Li-LLTO composite anode possesses good affinity toward LLZO solid electrolytes, achieving a low interfacial resistance of 11.7 Ω cm<sup>2</sup>, and a high lithium self-diffusion coefficient reaching 4.5×10<sup>−11</sup> cm<sup>2</sup>/s, about one order of magnitude higher than that of pure lithium anode. These features collectively enhance the Li-LLTO/LLZO interfacial stability, increasing the critical current density fourfold and enabling a 1300-h symmetrical cell cycling life. It delivers high-performance solid-state lithium batteries with an 80% capacity retention after 220 cycles. This advancement not only improves the performance of lithium metal anodes in solid-state batteries but also offers promising insights for next-generation high-energy-density electrochemical energy storage systems.</p>

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Mixed ionic/electronic conducting framework enabled by transition metal-ion reduction in Li-LLTO composite anodes for ultrafast lithium diffusion

  • 期刊论文

  • 发表日期：

    2025年7月9日

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  • Huilin Zhu,
  • Shiwei Deng,
  • Xinyi Kong,
  • Xing Xiang,
  • Yan Duan,
  • Jian-Fang Wu,
  • Jilei Liu

摘要

The development of Li7La3Zr2O12 (LLZO) solid electrolytes is challenged by the unstable Li/LLZO interface during lithium stripping and plating processes, which impedes interfacial charge transport and accelerates lithium dendrite growth. Here, a freestanding ultrathin Li-Li0.3La0.5TiO3 (LLTO) composite anode with a three-dimensional interconnected mixed ionic/electronic conducting LLTO framework was developed. The mixed ionic/electronic conduction of LLTO arises from the in-situ reduction of transition metal ions (Ti4+) by metallic lithium. The Li-LLTO composite anode possesses good affinity toward LLZO solid electrolytes, achieving a low interfacial resistance of 11.7 Ω cm2, and a high lithium self-diffusion coefficient reaching 4.5×10−11 cm2/s, about one order of magnitude higher than that of pure lithium anode. These features collectively enhance the Li-LLTO/LLZO interfacial stability, increasing the critical current density fourfold and enabling a 1300-h symmetrical cell cycling life. It delivers high-performance solid-state lithium batteries with an 80% capacity retention after 220 cycles. This advancement not only improves the performance of lithium metal anodes in solid-state batteries but also offers promising insights for next-generation high-energy-density electrochemical energy storage systems.