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Electrode–electrolyte interface stability in solid state electrolyte systems: influence of coating thickness under varying residual stresses

1 Institut für Energie- und Klimaforschung IEK-2, Forschungszentrum Jülich, D-52425 Jülich, Germany
2 Institut für Energie- und Klimaforschung IEK-1, Forschungszentrum Jülich, D-52425 Jülich, Germany
3 Institut für Stromrichtertechnik und Elektrische Antriebe ISEA, RWTH Aachen University, D-52056 Aachen, Germany
4 Jülich Aachen Reseach Alliance Energy, RWTH Aachen University, D-52056 Aachen, Germany

Topical Section: Theory, simulations and modeling of materials

We introduce a model of electrode–electrolyte interfacial growth which focuses on the effect of thin coating layers on the interfacial stability in prestressed systems. We take into account transport resulting from deposition from the electrolyte, from capillarity driven surface diffusion, and from changes of the chemical potential due to the elastic energy associated with the interface profile. As model system, we use metallic lithium as electrode, LLZO as electrolyte and Al2O3 as a thin film interlayer, which is a highly relevant interfacial system in state of the art all-solid-electrolyte batteries. We consider the stability of the electrode-coating-electrolyte interface depending on the thickness of the thin film interlayer and the magnitude of the elastic prestresses. Our central approach is a linear stability analysis based on the mass conservation at the planar interface, employing approximations which are appropriate for solid state electrolytes (SSEs) like LLZ, a thin Li metal electrode and a thin coating layer with a thickness in the range of nanometres.
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