Interfacial performance evolution of ceramics-in-polymer composite electrolyte in solid-state lithium metal batteries

Abstract: The incorporation of ceramics into polymers, forming solid composite electrolytes (SCEs) leads to enhanced electrical performance of all-solid-state lithium metal batteries. This is because the dispersed ceramics particles increase the ionic conductivity, while the polymer matrix leads to better contact performance between the electrolyte and the electrode. In this study, we present a model, based on Hybrid Elements Methods, for the time-dependent Li metal and SCE rough interface mechanics, taking into account for the oxide (ceramics) inclusions (using the Equivalent Inclusion method), and the viscoelasticity of the matrix. We study the effect of LLTO particle size, weight concentration, and spatial distribution on the interface mechanical and electrical response. Moreover, considering the viscoelastic spectrum of a real PEO matrix, under a given stack pressure, we investigate the evolution over time of the mechanical and electrical performance of the interface. The presented theoretical/numerical model might be pivotal in tailoring the development of advanced solid state batteries with superior performance; indeed, we found that conditions in the SCE mixture which optimize both the contact resistivity and the interface stability in time.