The goal of this work is to understand the relationships between electrode microstructure and mass transport resistances. One can use this information to predict cell performance from fundamental principles. This work includes new types of particle-scale 3D models for correlating and predicting the effects of electrode microstructure on both ionic and electronic transport. The 3D models imitate the sub-micrometer-scale arrangement of active material particles, carbon, binder, and pores and use FIB/SEM images as a basis for parameterization. The 3D models are based respectively on the statistical mechanics techniques of molecular dynamics and Monte Carlo. The approach closely related to molecular dynamics, named the dynamic particle packing (DPP) model, uses aggregates of spheres to recreate electrode microstructures. The other approach, named the stochastic grid (SG) model, is closely related to Monte Carlo techniques in which a small set of fundamental interdomain and bulk energy parameters are used to generate structures.In order to predict electrode microstructures we correlated the fundamental interdomain and bulk energy parameters for the SG model to electrode mass composition and porosity. We used the revised computer program, known as predict SG, to estimate structures of which there are no experimental measurements of electrode structure. From these predicted electrode structures we obtained electronic and ionic transport properties. This allowed us to estimate the trade-offs between ionic and electronic transport for different porosities and carbon fractions. We found from experimental measurements of electrode structure that carbon and binder formed distinct agglomerates. From the 3D models we determined at commercial fractions of carbon and binder that the conductivity of these carbon agglomerates plays a large role in determining both the electronic and ionic pathways. So in order to better understand the role that these carbon/binder agglomerates play, we explored and developed several experimental methods to find the electronic and ionic conductivity of both simulated carbon domains and complete electrode films. The goal was not only to elucidate the role carbon agglomerates play, but also to develop a non-destructive method of determining overall film properties. Although we found that a non-destructive method is extremely challenging due to probe contact resistances, we did find success in determining carbon domain properties using a delamination method.



College and Department

Ira A. Fulton College of Engineering and Technology; Chemical Engineering



Date Submitted


Document Type





electrochemistry, monte carlo, structure reconstruction, FIB imaging