(372d) Optimized Mesostructures of Li-Ion Battery Electrodes Predicted from Particle-Based Simulations

Electrochemical performance of Li-ion battery electrodes is crucially governed by the morphology of carbon-binder domain (CBD)—composed of carbon black nanoparticles and polymeric binder—in the local vicinity of electroactive particles such as LiNi_1/3Mn_1/3Co_1/3O₂. However, the effect of CBD properties, such as its cohesive strength and adhesive strength between CBD and electroactive particles, on electrode mesostructure is not well understood. This results primarily from our inability to visualize mesostructural details at sufficiently low resolution and large domain sizes within experiments, and numerical challenges associated with accurately modeling CBD topology within the complex and tortuous electrode mesostructure. This talk will describe our physics-based high-fidelity models to simulate the dynamics of micron-sized electroactive particles and nanometric CBD particles during various stages of electrode fabrication. Several experimentally-relevant compositions of CBD, electroactive material, and electrode porosities will be considered. The effect of cohesive and adhesive strength of CBD on its local topology around electroactive particles and on the porous mesostructure will be discussed. Lastly, finite element modeling of electronic and ionic conductivities of these simulated electrode mesostructures will be presented, and predictions towards mesostructure optimization for enhanced electrochemical properties will be discussed.