The Role of Local Inhomogeneities on Dendrite Growth in LLZO-Based Solid Electrolytes

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

doi:10.1149/1945-7111/ab9b08

The Role of Local Inhomogeneities on Dendrite Growth in LLZO-Based Solid Electrolytes

Journal Article · Thu Jun 18 00:00:00 EDT 2020 · Journal of the Electrochemical Society (Online)

DOI:https://doi.org/10.1149/1945-7111/ab9b08· OSTI ID:1633826

; Ngo, Anh T.; Narayanan, Badri; Higa, Kenneth; Curtiss, Larry A.; Srinivasan, Venkat

The majority of the ceramic solid electrolytes (LLZO, LATP) demonstrate polycrystalline grain/grain-boundary (G/GB) microstructure. Higher lithium (Li) concentration and lower mechanical stiffness result in current focusing at the GBs. Growth of Li dendrites through local inhomogeneities and subsequent short circuit of the cell is a major concern. Recent studies have revealed that bulk Li metal is a viscoplastic material that has low (~0.3 MPa) and high (~1.0 MPa) yield strength during deformation at smaller and larger rates of strain, respectively. It has been argued that during deposition at smaller current densities, due to its lower yield strength, Li metal should demonstrate plastic flow against stiff ceramic electrolytes, and Li dendrites will be prevented from penetrating through solid electrolytes. In this manuscript, a multiscale modeling framework has been developed for predicting properties of GBs and the bulk of ceramic electrolytes using atomistic calculations for input to mesoscale models. Using the parameters obtained from the atomistic simulations, the mesoscale model reveals that, given enough time, even at low charge rates, lithium dendrites can grow through the GBs of LLZO. The present multiscale model results also provide information regarding the dendrite growth velocity through LLZO.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Laboratory Computing Resource Center (LCRC); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

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

OSTI ID:: 1633826

Alternate ID(s):: OSTI ID: 1760205
OSTI ID: 1660758

Journal Information:: Journal of the Electrochemical Society (Online), Journal Name: Journal of the Electrochemical Society (Online) Journal Issue: 10 Vol. 167; ISSN 1945-7111

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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atomistic modeling
grain/grain-boundary
lithium dendrite growth
mesoscale analysis
microstructure

The Role of Local Inhomogeneities on Dendrite Growth in LLZO-Based Solid Electrolytes

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