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<p>The need for all-solid-state batteries with superior energy density has intensified interest in Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> garnet-type solid electrolytes. While Ta doping has proven effective for cubic phase LLZO stabilization, further research is needed in optimizing doping amount and performance for practical applications. Conventional synthesis methods often require high dopant concentrations (<i>x</i> ≥ 0.4 in Li<sub>7−<i>x</i></sub>La<sub>3</sub>Zr<sub>2−<i>x</i></sub>Ta<sub><i>x</i></sub>O<sub>12</sub>) to achieve peak performance. This study demonstrates that a successful synthesis of LLZT<i>x</i>O, <i>x</i> = 0.0–0.40&#xa0;mol ceramics resulted from a meticulously optimized solid-state synthesis protocol, featuring extended high-energy ball milling and precise sintering control, enabling superior electrochemical performance at a significantly reduced Ta doping level. Remarkably, this work outperformed many reports with higher Ta content, achieving 0.21&#xa0;eV activation energy and 1.07 mS cm⁻¹ high ionic conductivity at an optimum composition of <i>x</i> = 0.20&#xa0;mol at 30&#xa0;°C. The critical current density (CCD) of the Li metal symmetric cell was measured at 1.4&#xa0;mA·cm<sup>− 2</sup>. Structural (XRD, Rietveld refinement) and microstructural (SEM) analyses confirm the cubic phase stability and reveal highly dense, well-sintered morphology at this optimal doping level. This work contests the current view of high dopant addition by demonstrating that process optimization is a critical, often overlooked factor in maximizing dopant efficacy. It establishes an efficient, reproducible route for producing advanced solid-state batteries with high-performing garnet electrolytes.</p> Graphical abstract <p></p>

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A roadmap to high-performance Ta-doped LLZO: synergistic optimization of synthesis, microstructure and electrochemical properties

  • 期刊论文

  • 发表日期：

    2026年4月10日

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  • Emmanuel Kwame Yadzo,
  • Yueming Li,
  • Binxuan Jiang,
  • Kai Li,
  • Zhenhua Chen,
  • Xu Guo,
  • Zizheng Zhang

摘要

The need for all-solid-state batteries with superior energy density has intensified interest in Li7La3Zr2O12 garnet-type solid electrolytes. While Ta doping has proven effective for cubic phase LLZO stabilization, further research is needed in optimizing doping amount and performance for practical applications. Conventional synthesis methods often require high dopant concentrations (x ≥ 0.4 in Li7−xLa3Zr2−xTaxO12) to achieve peak performance. This study demonstrates that a successful synthesis of LLZTxO, x = 0.0–0.40 mol ceramics resulted from a meticulously optimized solid-state synthesis protocol, featuring extended high-energy ball milling and precise sintering control, enabling superior electrochemical performance at a significantly reduced Ta doping level. Remarkably, this work outperformed many reports with higher Ta content, achieving 0.21 eV activation energy and 1.07 mS cm⁻¹ high ionic conductivity at an optimum composition of x = 0.20 mol at 30 °C. The critical current density (CCD) of the Li metal symmetric cell was measured at 1.4 mA·cm− 2. Structural (XRD, Rietveld refinement) and microstructural (SEM) analyses confirm the cubic phase stability and reveal highly dense, well-sintered morphology at this optimal doping level. This work contests the current view of high dopant addition by demonstrating that process optimization is a critical, often overlooked factor in maximizing dopant efficacy. It establishes an efficient, reproducible route for producing advanced solid-state batteries with high-performing garnet electrolytes.

Graphical abstract