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

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.

Jordi Sastre, Moritz H. Futscher, Lea Pompizi, Abdessalem Aribia, Agnieszka Priebe, Jan Overbeck, Michael Stiefel, Ayodhya N. Tiwari, Yaroslav E. Romanyuk