A Finite Element Formulation to Three-Dimensionally Resolve Space-Charge Layers in Solid Electrolytes

TL;DR

This paper introduces a finite element model that accurately predicts the three-dimensional development of space-charge layers in solid electrolytes within realistic microstructures, addressing previous limitations in spatial resolution.

Contribution

It presents a novel finite element formulation that captures 3D space-charge layer evolution in microstructured solid electrolytes, enabling more precise simulations.

Findings

SCLs differ significantly in realistic microstructures compared to simplified models

The model enables quantification of microstructural effects on SCL formation

Effects in SCLs are predominantly one-dimensional, simplifying analysis

Abstract

All-solid-state batteries are seen as promising candidates to replace conventional batteries with liquid electrolytes in many applications. However, they are not yet feasible for many relevant applications. One particular question of interest is the identification of physical effects inside all-solid-state batteries and their quantitative influence on the performance of the entire battery cell. Simulation models can contribute to answering the aforementioned question by systematical studies, e.g. enabling or disabling certain physical effects. Especially the influence of space-charge layers (SCLs) is heavily discussed in the scientific community. So far, the different length scales of SCLs and the microstructure of a battery cell made a spatial discretization of realistic microstructures with resolved SCLs infeasible. However, thermodynamically consistent continuum models which are applied to simplified geometries are already established in the literature. In this work, we propose a model that enables the prediction of the spatial development of SCLs within geometrically resolved microstructures by exploiting that effects in SCLs are predominantly one-dimensional. With the proposed approach it is possible to quantify the geometric influence of realistic microstructures on the formation process of SCLs. SCLs in realistic microstructures remarkably differ from SCLs computed with simplified one-dimensional models which are already established in the literature.