A pseudo-two-dimensional (P2D) model for FeS2 conversion cathode batteries

Conversion cathode materials are gaining interest for secondary batteries due to their high theoretical energy and power density. However, practical application as a secondary battery material is currently limited by practical issues such as poor cyclability. To better understand these materials, we have developed a pseudo-two-dimensional model for conversion cathodes. We apply this model to FeS2 - a material that undergoes intercalation followed by conversion during discharge. The model is derived from the half-cell Doyle-Fuller- Newman model with additional loss terms added to reflect the converted shell resistance as the reaction progresses. We also account for polydisperse active material particles by incorporating a variable active surface area and effective particle radius. Using the model, we show that the leading loss mechanisms for FeS2 are associated with solid-state diffusion and electrical transport limitations through the converted shell material. The polydisperse simulations are also compared to a monodisperse system, and we show that polydispersity has very little effect on the intercalation behavior yet leads to capacity loss during the conversion reaction. We provide the code as an open-source Python Battery Mathematical Modeling (PyBaMM) model that can be used to identify performance limitations for other conversion cathode materials.

Automated summary

Conversion cathode materials are of interest for secondary batteries due to their high theoretical energy and power density, but practical application is limited by issues such as poor cyclability. A pseudo-two-dimensional model has been developed for FeS2, a material that undergoes intercalation followed by conversion during discharge, revealing that solid-state diffusion and electrical transport limitations through the converted shell material are the leading loss mechanisms. Additionally, simulations comparing polydisperse and monodisperse systems show that polydispersity has minimal effect on intercalation behavior but leads to capacity loss during the conversion reaction.