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

Can Yildirim, Florian Flatscher, Steffen Ganschow, Alice Lassnig, Christoph Gammer, Juraj Todt, Jozef Keckes and Daniel Rettenwander ()
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Can Yildirim: European Synchrotron Radiation Facility
Florian Flatscher: NTNU Norwegian University of Science and Technology
Steffen Ganschow: Leibniz-Institut für Kristallzüchtung
Alice Lassnig: Erich Schmid Institute of Materials Science
Christoph Gammer: Erich Schmid Institute of Materials Science
Juraj Todt: Erich Schmid Institute of Materials Science
Jozef Keckes: Erich Schmid Institute of Materials Science
Daniel Rettenwander: NTNU Norwegian University of Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-52412-4

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