<p>The Ga-doped Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (Ga-LLZO) system currently exhibits the highest ionic conductivity among garnet-type solid-state electrolytes and faces persistent challenges including pore formation—arising from high-temperature disproportionation reactions and elevated sintering activity—as well as lithium filament growth and short-circuit failure at pores and grain boundaries. Effectively addressing these issues while retaining high ionic conductivity remains a major obstacle. In this study, Ce was introduced into the Ga-LLZO lattice via an in situ tuning strategy, which significantly reduced internal pore retention and suppressed the reduction of migrating Li<sup>+</sup> into dead lithium. The optimized Ce in situ tuning controlled Ga-LLZO achieved an ionic conductivity exceeding 1 mS cm<sup>−1</sup> at 25&#xa0;°C, while the critical current density (CCD) in lithium symmetric cells reached 0.7&#xa0;mA&#xa0;cm<sup>−2</sup>—twice that of unmodified Ga-LLZO. Remarkably, no short-circuiting occurred even after 2700&#xa0;h of cycling at 0.3&#xa0;mA&#xa0;cm<sup>−2</sup>, in contrast to the unmodified Ga-LLZO, which failed after only 50&#xa0;h. The corresponding full cells also demonstrated excellent cycling stability and ultra-high capacity retention, significantly outperforming unmodified Ga-LLZO. Compared with recent electrolyte modification strategies, the Ce in situ tuning controlled Ga-LLZO delivers outstanding overall performance. Moreover, it holds strong potential for synergistic integration with other advanced modification techniques, offering broad prospects for further development and practical implementation in next-generation all-solid-state batteries (ASSBs).</p> Graphical abstract <p></p>

错误:搜索内容不能为空,请输入英文关键词
错误:关键词超出字数限制,请精简
高级检索

Ce in situ tuning control in Ga-LLZO: overcoming pore formation and lithium filament growth for high-performance solid-state batteries

  • Yi-Yang Xiao,
  • Juan-Yu Yang,
  • Xiao-Bao Zhang,
  • Ning Wang,
  • Zhi-Hao Guo,
  • Wei-Liang Zeng,
  • Shi-Ang Liang,
  • Jun Chen,
  • Xiao-Wei Huang

摘要

The Ga-doped Li7La3Zr2O12 (Ga-LLZO) system currently exhibits the highest ionic conductivity among garnet-type solid-state electrolytes and faces persistent challenges including pore formation—arising from high-temperature disproportionation reactions and elevated sintering activity—as well as lithium filament growth and short-circuit failure at pores and grain boundaries. Effectively addressing these issues while retaining high ionic conductivity remains a major obstacle. In this study, Ce was introduced into the Ga-LLZO lattice via an in situ tuning strategy, which significantly reduced internal pore retention and suppressed the reduction of migrating Li+ into dead lithium. The optimized Ce in situ tuning controlled Ga-LLZO achieved an ionic conductivity exceeding 1 mS cm−1 at 25 °C, while the critical current density (CCD) in lithium symmetric cells reached 0.7 mA cm−2—twice that of unmodified Ga-LLZO. Remarkably, no short-circuiting occurred even after 2700 h of cycling at 0.3 mA cm−2, in contrast to the unmodified Ga-LLZO, which failed after only 50 h. The corresponding full cells also demonstrated excellent cycling stability and ultra-high capacity retention, significantly outperforming unmodified Ga-LLZO. Compared with recent electrolyte modification strategies, the Ce in situ tuning controlled Ga-LLZO delivers outstanding overall performance. Moreover, it holds strong potential for synergistic integration with other advanced modification techniques, offering broad prospects for further development and practical implementation in next-generation all-solid-state batteries (ASSBs).

Graphical abstract