<p>Metal alloy negative electrodes are promising candidates for lithium all-solid-state batteries due to their high specific capacity and low cost. However, chemo-mechanical degradation and atomic transport limitations in the solid state remain unresolved challenges. Herein, we demonstrate a&#xa0;lithium-aluminum alloy negative electrode design (Li<sub><i>x</i></sub>Al<sub>1</sub>, <i>x</i> = molar ratio of lithium to aluminum) based on a comprehensive understanding of the&#xa0;underlying diffusion mechanisms within the lithium-poor α (0 ≤ <i>x</i> ≤ 0.05) and lithium-rich β phases (0.95 ≤ <i>x</i> ≤ 1). The lithium-aluminum alloy negative electrodes with a higher lithium to aluminum&#xa0;ratio facilitate lithium migration through the β-LiAl phases, which serve as highly lithium-conductive channels with a lithium diffusion coefficient that is&#xa0;ten orders of magnitude higher than that of the α phase. In addition, a bulk dense negative electrode and an intimate negative electrode-electrolyte interface is demonstrated in the cross-sections of the lithium-aluminum alloy negative electrodes. Consequently, a high-rate capability of 7 mA cm<sup>−2</sup> is attained in LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub>-based full-cell operation. The optimal cell configuration of Li<sub>0.5</sub>Al<sub>1</sub> | |LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> shows stable lithium reversibility during 2000 cycles with a capacity retention of 83% at 4 mA cm<sup>−2</sup> with a LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> loading of 5 mAh cm<sup>−2</sup>.</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

Lithium diffusion-controlled Li-Al alloy negative electrode for all-solid-state battery

  • Yuju Jeon,
  • Dong Ju Lee,
  • Hongkui Zheng,
  • Sesha Sai Behara,
  • Jung-Pil Lee,
  • Junlin Wu,
  • Feng Li,
  • Wei Tang,
  • Lanshuang Zhang,
  • Yu-Ting Chen,
  • Dapeng Xu,
  • Jiyoung Kim,
  • Min-Sang Song,
  • Anton Van der Ven,
  • Kai He,
  • Zheng Chen

摘要

Metal alloy negative electrodes are promising candidates for lithium all-solid-state batteries due to their high specific capacity and low cost. However, chemo-mechanical degradation and atomic transport limitations in the solid state remain unresolved challenges. Herein, we demonstrate a lithium-aluminum alloy negative electrode design (LixAl1, x = molar ratio of lithium to aluminum) based on a comprehensive understanding of the underlying diffusion mechanisms within the lithium-poor α (0 ≤ x ≤ 0.05) and lithium-rich β phases (0.95 ≤ x ≤ 1). The lithium-aluminum alloy negative electrodes with a higher lithium to aluminum ratio facilitate lithium migration through the β-LiAl phases, which serve as highly lithium-conductive channels with a lithium diffusion coefficient that is ten orders of magnitude higher than that of the α phase. In addition, a bulk dense negative electrode and an intimate negative electrode-electrolyte interface is demonstrated in the cross-sections of the lithium-aluminum alloy negative electrodes. Consequently, a high-rate capability of 7 mA cm−2 is attained in LiNi0.8Co0.1Mn0.1O2-based full-cell operation. The optimal cell configuration of Li0.5Al1 | |LiNi0.8Co0.1Mn0.1O2 shows stable lithium reversibility during 2000 cycles with a capacity retention of 83% at 4 mA cm−2 with a LiNi0.8Co0.1Mn0.1O2 loading of 5 mAh cm−2.