A Diffuse-Interface Model for Predicting the Evolution of Metallic Negative Electrodes and Interfacial Voids in Solid-State Batteries with Homogeneous and Polycrystalline Solid Electrolyte Separators

Chatterjee, Sourav; Tonks, Michael; Gardner, William; Sessim, Marina

doi:10.1149/1945-7111/aded38

Title: A Diffuse-Interface Model for Predicting the Evolution of Metallic Negative Electrodes and Interfacial Voids in Solid-State Batteries with Homogeneous and Polycrystalline Solid Electrolyte Separators

Journal Article · Wed Jul 23 00:00:00 UTC 2025 · Journal of The Electrochemical Society

DOI: https://doi.org/10.1149/1945-7111/aded38 · OSTI ID:2587882

^[1]; Tonks, Michael ^[2]; Gardner, William ^[3]; Sessim, Marina ^[3]

Univ. of Florida, Gainesville, FL (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Univ. of Florida, Gainesville, FL (United States)
QuantumScape Battery, Inc., San Jose, CA (United States)

Here, this paper presents a novel diffuse-interface electrochemical model that simultaneously simulates the evolution of the metallic negative electrode and interfacial voids during the stripping and plating processes in solid-state batteries. The utility and validity of this model are demonstrated for the first time on a cell with a sodium (Na) negative electrode and a Na-β″-alumina ceramic solid electrolyte (SE) separator. Three examples are simulated. First, stripping and plating with a perfect electrode/electrolyte interface; second, stripping and plating with a single interfacial void at the electrode/electrolyte interface; third, stripping with multiple interfacial voids. Both homogeneous and polycrystalline SEs with low and high-conductivity grain boundaries (GBs) are considered for all three examples. Heterogeneous GB conductivity marginally impacts the thickness of the Na electrode in cases with a perfect electrode/electrolyte interface. Moreover, it results in local changes to void growth due to the interactions between the void edge and the GBs. The void growth rate is a linear function of the flux of Na atoms at the void edge, which in turn depends on the applied current density. We also show that the void coalescence rate increases with applied current density and can be marginally influenced by GB conductivity.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 2587882

Report Number(s):: LLNL--JRNL-2001706

Journal Information:: Journal of The Electrochemical Society, Journal Name: Journal of The Electrochemical Society Journal Issue: 7 Vol. 172; ISSN 1945-7111; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: A Diffuse-Interface Model for Predicting the Evolution of Metallic Negative Electrodes and Interfacial Voids in Solid-State Batteries with Homogeneous and Polycrystalline Solid Electrolyte Separators

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