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<p>Oxide ceramic electrolytes for realization of high-energy lithium metal batteries typically require high-temperature processes to achieve the desired phase formation and inter-particle sintering. However, such high-temperature processing can lead to compositional changes or mechanical deformation, compromising material reliability. Here, we introduce a disorder-driven, sintering-free approach to synthesize garnet-type solid electrolyte via the creation of an amorphous matrix followed by a single-step mild heat-treatment. The softened mechanical property (yield pressure, <i>P</i><sub><i>y</i></sub> = 359.8 MPa) of disordered base materials enables the facile formation of a dense amorphous matrix and the preserving of inter-particle connectivity during crystallization. The formation of the cubic-phase garnet is triggered at a lowered temperature of 350 °C, achieving a Li<sup>+</sup> ionic conductivity of 1.8 × 10<sup>–4</sup> S/cm at 25 °C through a single-step mild heat treatment at 500 °C. The disorder-driven garnet solid electrolyte exhibits electrochemical performance comparable to conventional garnet solid electrolyte sintered at &gt;1100 °C. These findings will promote the fabrication of uniform, thin, and wide solid electrolyte membranes, which is a significant hurdle in the commercialization of oxide-based lithium metal batteries, and demonstrate the untapped capabilities of garnet-type oxide solid electrolytes.</p>

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Disorder-driven sintering-free garnet-type solid electrolytes

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月5日

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  • Giyun Kwon,
  • Hyeokjo Gwon,
  • Youngjoon Bae,
  • Changhoon Jung,
  • Dong-Su Ko,
  • Min Gyu Kim,
  • Kyungho Yoon,
  • Gabin Yoon,
  • Sewon Kim,
  • In-Sun Jung,
  • Sangjun Lee,
  • Taehee Kim,
  • Ju-Sik Kim,
  • Tae Young Kim,
  • Yong Su Kim

摘要

Oxide ceramic electrolytes for realization of high-energy lithium metal batteries typically require high-temperature processes to achieve the desired phase formation and inter-particle sintering. However, such high-temperature processing can lead to compositional changes or mechanical deformation, compromising material reliability. Here, we introduce a disorder-driven, sintering-free approach to synthesize garnet-type solid electrolyte via the creation of an amorphous matrix followed by a single-step mild heat-treatment. The softened mechanical property (yield pressure, Py = 359.8 MPa) of disordered base materials enables the facile formation of a dense amorphous matrix and the preserving of inter-particle connectivity during crystallization. The formation of the cubic-phase garnet is triggered at a lowered temperature of 350 °C, achieving a Li+ ionic conductivity of 1.8 × 10–4 S/cm at 25 °C through a single-step mild heat treatment at 500 °C. The disorder-driven garnet solid electrolyte exhibits electrochemical performance comparable to conventional garnet solid electrolyte sintered at >1100 °C. These findings will promote the fabrication of uniform, thin, and wide solid electrolyte membranes, which is a significant hurdle in the commercialization of oxide-based lithium metal batteries, and demonstrate the untapped capabilities of garnet-type oxide solid electrolytes.