EAGER: Collaborative Research: Shear Dependent Reaction Kinetics in Particulate Electrochemical Energy Storage

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Lithium-ion batteries are considered the pre-eminent storage device for portable electronics, emerging green technologies, and electric vehicles. However, additives that are used to boost electronic and ionic conductivities of the electrode materials comprise about 1/3 of the battery volume, undermining both energy and power density of the cell, as well as impairing the cycle life of the system. Redox flow batteries on the other hand have shown great advantages on their scale-up flexibility, but their energy density is limited by the solubility of metal ion redox couples in liquid solvents. Recently, a new concept of flowing ion-storing semi-solid electroactive materials into and from a battery assembly to create a high energy and power density redox flow battery has been proposed. Realizing the tremendous potential of this new concept requires a fundamental understanding of the effects of moving electrode particles and flowing electrolytes on ion/charge transport as well as charging/discharging kinetics compared with those in static battery configurations. This collaborative project brings together Dr. Steingart specializing on electrochemical energy storage systems and Dr. Sun on complex fluids physics, integrating expertise on rheology, reaction chemistry, materials processing, and battery performance for the realization of semi- solid flow battery concept. The objective of this EAGER project is to create a baseline methodology for characterizing and predicting the electrochemical-mechanical coupling behavior of large mass fraction flowing slurry electrodes through integrated modeling and experiments.Intellectual MeritIn the semi-solid flow battery configuration, positive and/or negative electrode slurries are usually non- Newtonian and their stability is extremely challenging. Using an optically transparent flow cell and rate shear viscometry, the effect of interpacticle packing and flow on conductivity, and reaction rate are directly determined. By running conductivity experiments in parallel with overall reaction experiments, the PIs can decouple the electrical conductivity. Through the insights provided by our particle transport mechanism-resolved, electrochemistry-coupled model, PIs will be able to understand the coupled behavior of flow, viscosity, ionic conductivity, electrical conductivity, particle size, particle size distribution and electrode kinetics in semi-solid electrode flow systems.Broader ImpactsThe development of more cost-effective, long lasting, and high energy/power-density battery solution is a crucial step toward the electrification of the nation?s personal transportation and more stable and efficient electrical grids. Semi-solid flow batteries enable high energy density storage while removing lifetime concerns from the reacting material. This project builds a new exciting collaboration between chemical and mechanical engineers at Princeton and Drexel to enable efficient, reliable flow batteries. Both graduate and undergraduate students will benefit from the interdisciplinary nature of the proposed project.