4.8 Article

Size-Dependent Chemomechanical Failure of Sulfide Solid Electrolyte Particles during Electrochemical Reaction with Lithium

Journal

NANO LETTERS
Volume 22, Issue 1, Pages 411-418

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c04076

Keywords

Solid-state batteries; Chemomechanical failure; Size effect; Sulfide solid electrolyte

Funding

  1. National Natural Science Foundation of China [51971245, 52022088, 51772262, 21406191, U20A20336, 21935009]
  2. Beijing Natural Science Foundation [2202046]
  3. Fok Ying-Tong Education Foundation of China [171064]
  4. Natural Science Foundation of Hebei Province [F2021203097, B2020203037, B2018203297]
  5. Hunan Innovation Team [2018RS3091]
  6. Institute for Basic Science of South Korea [IBS-R019-D1]
  7. Vehicles Technology Office, of the U.S. Department of Energy [DEAC02-05CH11231]

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This study demonstrates a strong size effect in the chemomechanical failure of Li10GeP2S12 (LGPS) solid electrolyte particles, with no failure observed when the particle size is less than 1 μm.
The very high ionic conductivity of Li10GeP2S12 (LGPS) solid electrolyte (SE) makes it a promising candidate SE for solid-state batteries in electrical vehicles. However, chemomechanical failure, whose mechanism remains unclear, has plagued its widespread applications. Here, we report in situ imaging lithiation-induced failure of LGPS SE. We revealed a strong size effect in the chemomechanical failure of LGPS particles: namely, when the particle size is greater than 3 mu m, fracture/pulverization occurred; when the particle size is between 1 and 3 mu m, microcracks emerged; when the particle size is less than 1 mu m, no chemomechanical failure was observed. This strong size effect is interpreted by the interplay between elastic energy storage and dissipation. Our finding has important implications for the design of high-performance LGPS SE, for example, by reducing the particle size to less than 1 mu m the chemomechanical failure of LGPS SE can be mitigated.

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