Pore Network Modelling of Galvanostatic Discharge Behaviour of Lithium-Ion Battery Cathodes

The performance of Lithium-Ion batteries (LIB’s) strongly depends on 3D microstructure and continued research is needed for the development and optimization of electrode designs to further reduce cost and improve performance and durability. In this work, a pore network modelling approach is presented to understand the structure-performance relationship of porous cathodes of LIB’s. It was demonstrated that pore network models can efficiently predict the rate-dependent capacity of an electrode using only a 3-phase tomogram as input. The developed modelling framework was used to perform structural analysis on two Li(Ni0.5Mn0.3Co0.2)O2 (NMC532) cathodes of different thickness and calendaring pressure and revealed important insights of microstructural heterogeneities inside porous structures, including spatial distribution of concentration, potential and state of lithiation in electrolyte, active material and carbon binder domain. The computational performance of the pore network model was analyzed, and excellent performance was demonstrated, taking hours instead of weeks for a similar direct numerical simulation. The novel modelling framework reported in this study will enable the study of local heterogeneities in other types of cathode material to help screen next-generation electrode designs, augmenting and informing time-consuming cell fabrication and laboratory testing.