4.2 Article

Blocking lithium dendrite growth in solid-state batteries with an ultrathin amorphous Li-La-Zr-O solid electrolyte

Journal

COMMUNICATIONS MATERIALS
Volume 2, Issue 1, Pages -

Publisher

SPRINGERNATURE
DOI: 10.1038/s43246-021-00177-4

Keywords

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Funding

  1. Swiss National Science Foundation [200021_172764]
  2. joint Empa-Fraunhofer ISC project IE4B under the ICON funding line
  3. Strategic Focus Area (SFA) Advanced Manufacturing of the ETH Domain (project X-Ray Diagnostics)
  4. Empa internal project SUISSE-battery
  5. Swiss Commission for Technology and Innovation (CTI) project [25592.1PFNM-NM]
  6. Swiss National Science Foundation (SNF) [200021_172764] Funding Source: Swiss National Science Foundation (SNF)

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Research has shown that tuning the lithium stoichiometry in LLZO can form an amorphous phase, effectively blocking the growth of lithium dendrites, increasing ionic conductivity while maintaining high electronic insulation. The amorphous Li-La-Zr-O as a dendrite blocking layer shows excellent performance in microbatteries, promising to accelerate the development of better solid-state batteries.
Lithium dendrites have become a roadblock in the realization of solid-state batteries with lithium metal as high-capacity anode. The presence of surface and bulk defects in crystalline electrolytes such as the garnet Li7La3Zr2O12 (LLZO) facilitates the growth of these hazardous lithium filaments. Here we explore the amorphous phase of LLZO as a lithium dendrite shield owing to its grain-boundary-free microstructure, stability against lithium metal, and high electronic insulation. By tuning the lithium stoichiometry, the ionic conductivity can be increased by 4 orders of magnitude while retaining a negligible electronic conductivity. In symmetric cells, plating-stripping shows no signs of lithium penetration up to 3.2 mA cm(-2). The dense conformal nature of the films enables microbatteries with an electrolyte thickness of only 70 nm, which can be cycled at 10C for over 500 cycles. The application of this material as a coating on crystalline LLZO lowers the interface resistance and increases the critical current density. The effectiveness of the amorphous Li-La-Zr-O as dendrite blocking layer can accelerate the development of better solid-state batteries. The formation and growth of dendrites in solid-state lithium metal batteries is a common cause of failure. Here, thin-film amorphous Li-La-Zr-O shows high resistance to lithium penetration, making it promising for thin-film solid-state batteries and as a coating for bulk ceramic electrolyte.

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