Self-Organization of Electroactive Suspensions in Discharging Slurry Batteries: A Mesoscale Modeling Investigation.

We report a comprehensive modeling-based study of electroactive suspensions in slurry redox flow batteries undergoing discharge. A three-dimensional kinetic Monte Carlo model based on the variable step size method is used to describe the electrochemical discharge of a silicon/carbon slurry electrode in static mode (i.e., no fluid flow conditions). The model accounts for Brownian motion of particles, volume expansion of silicon upon lithium insertion, and formation and destruction of conducting carbon networks. Coupled to an electrochemical model, this study explores the impact of carbon fraction in the slurry and applied c-rate on the specific capacity. The trends obtained are analyzed by following the behavior of parameters such as number of contacts between electroactive particles and the percentage of electroactive silicon particles. Furthermore, instead of studying the bulk behavior of the slurry, here the focus is given to the slurry/current collector interface in order to illustrate its importance. Hereby, it is demonstrated how this modeling tool can lead to deeper understanding and optimization of electroactive particle suspensions in redox flow batteries.