Modeling of Lithium-Ion Convection Cell Effects on Reaction Distribution and Different Cathode Active Materials

Li-ion batteries (LIBs) could play a substantial role in mitigating climate change if they become more widely adopted in transportation and stationary energy storage applications. Increasing this adoption requires improvement in both power density and energy density. At the cell level, this dual requirement calls for designs and active materials that overcome challenging trade-offs in nominal cell voltage, rate capability, and loaded capacity. In our previous research, 1,2 we simulated that a convection cell with liquid electrolyte flow, using LCO, can overcome the trade-offs by enhancing accessed capacity under high-rate operation. Electrolyte flow achieves this enhancement by effectively addressing both bulk electrolyte mass transfer and thermal limitations. The flow of electrolyte raises cell voltage by promoting a uniform Li + salt concentration and regulates temperature by removing heat and lowering heat-producing overpotentials. In our current work, we extend our macrohomogeneous modeling analysis of a Li-ion convection cell to explore the impact of concentration uniformity on charge-transfer reaction distribution and the flexibility of this approach to work with different active materials. Concentration uniformity evens the reaction distribution, facilitating spatially consistent and full utilization of the active material in the electrodes. Additionally, the use of flow enables the cell to maintain rate capability across various electrode thicknesses and areal capacity loadings. At high C rates, a convection cell with flow exhibits significantly higher output capacity than a closed cell without flow. The degree of increase in running voltage and delivered capacity depends on the choice of positive electrode active material—LFP, LCO, NCA, NMC, or LMO. Finally, simulations of net power density and net energy density account for pumping energy loss across the cell. The improvement in net energy density with flow becomes substantial at high power density. W. Gao, M.J. Orella, T.J. Carney, Y. Román-Leshkov, J. Drake, F.R. Brushett, J. Electrochem. Soc. , 167 , 140551 (2020). W. Gao, J. Drake, F.R. Brushett, J. Electrochem. Soc. 170 , 090508 (2023).