Structure matters: A scale-resolved numerical operando approach for Lithium–Sulfur batteries

Lithium–Sulfur batteries (LSBs) are believed to have a high potential for aerospace applications due to their high gravimetric energy density. However, despite decades of research and advances, they still suffer from poor rate capability and low power output, eventually preventing their practical implementation. One particular aspect we want to shed light on is the influence of the porous cathode structure on the rate performance during discharge. Therefore, we present a scale-resolved simulation methodology involving high-performance computing (HPC), which aims to provide structural insights into the electrochemical cell behavior that are experimentally hardly accessible even for modern operando methods. Our numerical operando approach employs scaling analysis for efficient model parametrization as well as rigorous parameter transfer between models of different dimensionality and is based on a coarse-grained continuum model. The latter is spatially discretized with a Discontinuous Galerkin (DG) method and advanced in time by an adaptive controller. The models and methods as well as HPC aspects of our toolbox will be critically discussed, finally showcasing the capabilities of our workflow to improve LSBs.