<p>Lithium-metal solid-state batteries offer advantages of high energy density and improved safety compared with lithium-ion batteries<sup><CitationRef CitationID="CR1">1</CitationRef>,<CitationRef CitationID="CR2">2</CitationRef></sup>. However, solid-state batteries fail through short-circuiting even at low charging rates (less than 1 mA cm<sup>−</sup><sup>2</sup>) due to lithium dendrite initiation and propagation<sup><CitationRef AdditionalCitationIDS="CR4" CitationID="CR3">3</CitationRef>–<CitationRef CitationID="CR5">5</CitationRef></sup>. The location of dendrite initiation is under debate, particularly regarding whether initiation occurs within the interior of the solid electrolyte<sup><CitationRef AdditionalCitationIDS="CR7 CR8" CitationID="CR6">6</CitationRef>–<CitationRef CitationID="CR9">9</CitationRef></sup> or at the surface<sup><CitationRef AdditionalCitationIDS="CR11 CR12 CR13" CitationID="CR10">10</CitationRef>–<CitationRef CitationID="CR14">14</CitationRef></sup>. Here we develop an in-plane biaxial compression method that provides direct evidence that dendrite initiation occurs within the interior of garnet Li<sub>6.6</sub>La<sub>3</sub>Zr<sub>1.6</sub>Ta<sub>0.4</sub>O<sub>12</sub> solid electrolytes during long-term cycling when the surface initiation mechanisms are rendered ineffective in shorting the cell. The biaxial compression deflects dendrite propagation so that it is perpendicular to the electric field direction, leading to the generation of an unprecedentedly high density of dendrites without short-circuiting, even at an extreme fast-charging rate of 100 mA cm<sup>−</sup><sup>2</sup>. After long-term cycling, dendrites eventually appeared throughout the entire thickness of the solid electrolyte. Under extreme cycling conditions, isolated lithium deposits are observed at grain-boundary junctions and pores, and these act as the dendrite initiation sites. This work reconciles the surface and interior initiation mechanisms in garnet solid electrolytes and demonstrates that in-plane biaxial compressive stress can prevent both from short-circuiting the cell.</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

Dendrite initiation and deflection in biaxially stressed solid electrolytes

  • Teng Cui,
  • Sunny Wang,
  • Samuel S. Lee,
  • Eddie Barks,
  • John Cattermull,
  • Celeste Melamed,
  • Zhelong Jiang,
  • Madison Morrison,
  • Leah Narun,
  • Yan-Kai Tzeng,
  • Naoki Fujii,
  • Seung Hyan Kim,
  • Xin Xu,
  • Geoff McConohy,
  • Paul M. Wallace,
  • Andrew C. Lee,
  • Xiao Cui,
  • Joon-Hyung Lee,
  • William C. Chueh,
  • X. Wendy Gu

摘要

Lithium-metal solid-state batteries offer advantages of high energy density and improved safety compared with lithium-ion batteries1,2. However, solid-state batteries fail through short-circuiting even at low charging rates (less than 1 mA cm2) due to lithium dendrite initiation and propagation35. The location of dendrite initiation is under debate, particularly regarding whether initiation occurs within the interior of the solid electrolyte69 or at the surface1014. Here we develop an in-plane biaxial compression method that provides direct evidence that dendrite initiation occurs within the interior of garnet Li6.6La3Zr1.6Ta0.4O12 solid electrolytes during long-term cycling when the surface initiation mechanisms are rendered ineffective in shorting the cell. The biaxial compression deflects dendrite propagation so that it is perpendicular to the electric field direction, leading to the generation of an unprecedentedly high density of dendrites without short-circuiting, even at an extreme fast-charging rate of 100 mA cm2. After long-term cycling, dendrites eventually appeared throughout the entire thickness of the solid electrolyte. Under extreme cycling conditions, isolated lithium deposits are observed at grain-boundary junctions and pores, and these act as the dendrite initiation sites. This work reconciles the surface and interior initiation mechanisms in garnet solid electrolytes and demonstrates that in-plane biaxial compressive stress can prevent both from short-circuiting the cell.