Mechanical Stress Induced Current Focusing and Fracture in Grain Boundaries

Barai, Pallab; Higa, Kenneth; Ngo, Anh T.; Curtiss, Larry A.; Srinivasan, Venkat

doi:10.1149/2.0321910jes

Title: Mechanical Stress Induced Current Focusing and Fracture in Grain Boundaries

Journal Article · 30 May 2019 · Journal of the Electrochemical Society

DOI: https://doi.org/10.1149/2.0321910jes · OSTI ID:1812866

^[1]; Higa, Kenneth ^[2]; Ngo, Anh T. ^[1]; Curtiss, Larry A. ^[1];

^[1]

Argonne National Lab. (ANL), Argonne, IL (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Solid state electrolytes (SSEs) with garnet structures and chemical composition Li₇La₃Zr₂O12 (LLZO) are being actively considered as the electrolyte for next-generation lithium ion batteries. These LLZO-based ceramic SSEs are polycrystalline and possess distinct grain-interior/grain-boundary (GI/GB) microstructure. Lithium dendrite growth through these GI and GB domains is considered to be the largest bottleneck preventing their successful implementation. Dendrite growth has been observed to occur predominantly within the GB regions. While this would be expected if the GB regions were more ionically conductive than the GI regions, there is significant disagreement over the relative conductivities of these two regions. The present work demonstrates that dendrite growth can occur preferentially in the GB regions even when the GI regions have higher ionic conductivity. Electrochemical potential changes induced by mechanical stress within the GI and GB domains reveals that the magnitude of effective stress induced current density within the elastically softer GB is larger than in the mechanically stiffer GI, which leads to enhanced lithium deposition in GB and subsequent dendrite growth. Finally, the present work additionally examines the impact of applied current density and grain size on current focusing in the GB regions, and also finds that SSE fractures initiate from the GB regions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357; AC02-05CH11231

OSTI ID:: 1812866

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 10 Vol. 166; ISSN 0013-4651

Publisher:: IOP Publishing - The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Mechanical Stress Induced Current Focusing and Fracture in Grain Boundaries

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