Modeling of an all-solid-state battery with a composite positive electrode

Abstract

All solid-state batteries are considered as the most promising battery technology due to their safety and high energy density. This study presents an advanced mathematical model that accurately simulates the complex behavior of all-solid-state lithium-ion batteries with composite positive electrodes. The partial differential equations of ionic transport and potential dynamics in the electrode and electrolyte are solved and reduced to a low-order system with Padé approximation. Moreover, the imperfect contact and the electrical double layers at the solid-solid interface are also taken into consideration. Subsequent experiments are conducted for the blocked cell and half-cells to extract parameters. Next, the parameterized model is validated with extensive experimental data from NCM811/LPSC/Li_4.4Si batteries, illustrating the superior capability of predicting cell voltage with an average RMSE of 19.5 mV for the discharging/charging phases and 2.8 mV for the end of relaxation under a total of 15 conditions. From the simulations, it can be concluded that the limiting factors for battery performance are overpotentials caused by concentration polarization within positive particles and interface reactions. Finally, through a parameter sensitivity analysis, we offer strategic guidelines for optimizing battery performance, thus enhancing the development efficiency of ASSBs.