TY - JOUR

T1 - Understanding the origin of lithium dendrite branching in Li6.5La3Zr1.5Ta0.5O12 solid-state electrolyte via microscopy measurements

AU - Yildirim, Can

AU - Flatscher, Florian

AU - Ganschow, Steffen

AU - Lassnig, Alice

AU - Gammer, Christoph

AU - Todt, Juraj

AU - Keckes, Jozef

AU - Rettenwander, Daniel

N1 - Publisher Copyright: © The Author(s) 2024.

PY - 2024/9/18

Y1 - 2024/9/18

N2 - Lithium dendrite growth in inorganic solid-state electrolytes acts as a main stumbling block for the commercial development of all-solid-state lithium batteries. Indeed, Li dendrites often lead to solid-state electrolyte fractures, undermining device integrity and safety. Despite the significance of these issues, the mechanisms driving the solid-state electrolyte fracture process at the microscopic level remain poorly understood. Here, via operando optical and ex situ dark field X-ray microscopy measurements of LiSn∣single-crystal Li6.5La3Zr1.5Ta0.5O12∣LiSn symmetric cells, we provide insights into solid-state electrolyte strain patterns and lattice orientation changes associated with dendrite growth. We report the observation of dislocations in the immediate vicinity of dendrite tips, including one instance where a dislocation is anchored directly to a tip. This latter occurrence in single-crystalline ceramics suggests an interplay between dendrite proliferation and dislocation formation. We speculate that the mechanical stress induced by dendrite expansion triggers dislocation generation. These dislocations seem to influence the fracture process, potentially affecting the directional growth and branching observed in lithium dendrites.

AB - Lithium dendrite growth in inorganic solid-state electrolytes acts as a main stumbling block for the commercial development of all-solid-state lithium batteries. Indeed, Li dendrites often lead to solid-state electrolyte fractures, undermining device integrity and safety. Despite the significance of these issues, the mechanisms driving the solid-state electrolyte fracture process at the microscopic level remain poorly understood. Here, via operando optical and ex situ dark field X-ray microscopy measurements of LiSn∣single-crystal Li6.5La3Zr1.5Ta0.5O12∣LiSn symmetric cells, we provide insights into solid-state electrolyte strain patterns and lattice orientation changes associated with dendrite growth. We report the observation of dislocations in the immediate vicinity of dendrite tips, including one instance where a dislocation is anchored directly to a tip. This latter occurrence in single-crystalline ceramics suggests an interplay between dendrite proliferation and dislocation formation. We speculate that the mechanical stress induced by dendrite expansion triggers dislocation generation. These dislocations seem to influence the fracture process, potentially affecting the directional growth and branching observed in lithium dendrites.

UR - http://www.scopus.com/inward/record.url?scp=85204417942&partnerID=8YFLogxK

U2 - 10.1038/s41467-024-52412-4

DO - 10.1038/s41467-024-52412-4

M3 - Article

C2 - 39294112

AN - SCOPUS:85204417942

VL - 15.2024

JO - Nature Communications

JF - Nature Communications

SN - 2041-1723

IS - 1

M1 - 8207

ER -