Scholarlink

<p>Lithium dendrite intrusion in solid-state batteries limits fast charging and causes short-circuiting, yet the underlying regulating mechanisms are not well-understood. Here we discover that heterogeneous Ag<sup>+</sup> doping dramatically affects lithium intrusion into Li<sub>6.6</sub>La<sub>3</sub>Zr<sub>1.6</sub>Ta<sub>0.4</sub>O<sub>12</sub> (LLZO), a brittle solid electrolyte. Nanoscale Ag<sup>+</sup> doping is achieved by thermally annealing a 3-nm-thick metallic coating on LLZO, inducing Ag–Li ion exchange and Ag diffusion into grains and grain boundaries. Density functional theory calculations and experimental characterization show negligible impact on the electronic properties and surface wettability from Ag<sup>+</sup> incorporation. Mechanically, nanoindentation experiments show a fivefold increase in the mechanical force required to fracture the surface Ag<sup>+</sup>-doped LLZO, indicating substantial doping-induced surface toughening. Operando microprobe scanning electron microscopy experiments show that the Ag<sup>+</sup>-doped LLZO surface exhibits improved lithium plating at &gt;250 mA cm<sup>−2</sup> and an electroplating diameter that is expanded by over fourfold, even under an extreme indentation stress of 3 GPa. This demonstrates enhanced defect tolerance in LLZO, rather than electronic or adhesion effects. Our study reveals a chemo-mechanical mechanism via surface heterogeneous doping, complementing present bulk design rules to minimize mechanical failures in solid-state batteries.</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

Heterogeneous doping via nanoscale coating impacts the mechanics of Li intrusion in brittle solid electrolytes

  • 期刊论文

  • 发表日期：

    2026年1月16日

查看全文
  • Xin Xu,
  • Teng Cui,
  • Geoff McConohy,
  • Harsh D. Jagad,
  • Samuel S. Lee,
  • Sunny Wang,
  • Celeste Melamed,
  • Yufei Yang,
  • Edward Barks,
  • Emma Kaeli,
  • Leah Narun,
  • Yi Cui,
  • Zewen Zhang,
  • Hye Ryoung Lee,
  • Rong Xu,
  • Melody M. Wang,
  • Levi Hoogendoorn,
  • Ajai Romana,
  • Alexis Geslin,
  • Robert Sinclair,
  • Yi Cui,
  • Yue Qi,
  • X. Wendy Gu,
  • William C. Chueh

摘要

Lithium dendrite intrusion in solid-state batteries limits fast charging and causes short-circuiting, yet the underlying regulating mechanisms are not well-understood. Here we discover that heterogeneous Ag+ doping dramatically affects lithium intrusion into Li6.6La3Zr1.6Ta0.4O12 (LLZO), a brittle solid electrolyte. Nanoscale Ag+ doping is achieved by thermally annealing a 3-nm-thick metallic coating on LLZO, inducing Ag–Li ion exchange and Ag diffusion into grains and grain boundaries. Density functional theory calculations and experimental characterization show negligible impact on the electronic properties and surface wettability from Ag+ incorporation. Mechanically, nanoindentation experiments show a fivefold increase in the mechanical force required to fracture the surface Ag+-doped LLZO, indicating substantial doping-induced surface toughening. Operando microprobe scanning electron microscopy experiments show that the Ag+-doped LLZO surface exhibits improved lithium plating at >250 mA cm−2 and an electroplating diameter that is expanded by over fourfold, even under an extreme indentation stress of 3 GPa. This demonstrates enhanced defect tolerance in LLZO, rather than electronic or adhesion effects. Our study reveals a chemo-mechanical mechanism via surface heterogeneous doping, complementing present bulk design rules to minimize mechanical failures in solid-state batteries.