Phase-field modeling of dead lithium in solid-state batteries via multiphysics coupling

Owing to, Solid-state batteries have gradually become the focus of people’s attention and research in recent years due to the advantages of high energy density and high safety factor. Lithium dendrites are a key factor affecting battery safety and service life, and in severe cases, battery short circuits can occur. Compared with liquid batteries, solid-state batteries rely on solid-state electrolytes with higher mechanical strength, which can effectively inhibit the growth of lithium dendrites, but with the increase of the number of charge-discharge cycles, the dead lithium produced by the incomplete dissolution of lithium dendrites gradually accumulates, and the performance of the battery gradually decreases. In this work, the problem of dead lithium in solid-state batteries is studied by using COMSOL Multiphysics 6.2 finite element simulation software. Due to the fact that existing research on dead lithium mainly focuses on phase field models combined with binary physics, there is little research on the influence of electrochemical parameters on dead lithium. Therefore, the phase field method is used to simulate the dissolution of lithium dendrites and the formation of dead lithium under the coupling of force-thermal-electrochemical fields. When the heat transfer model is coupled, the difference in the morphology of dead lithium before and after the coupled heat transfer model is further studied by applying an external pressure to change the stress of lithium dendrites. When the coupled mechanical field changes, the morphology of dead lithium before and after the coupled mechanical field is further studied by changing the temperature magnitude. At the same time, the effects of changes in three electrochemical parameters, namely diffusion coefficient, interfacial mobility and anisotropic strength, on the area of dead lithium are also explored. The research results indicate that when the heat transfer model or mechanical field is coupled into the phase field model, the dendrite dissolution cut-off time and dead lithium area will change. When the base rises at high temperature or when low external pressure or high external pressure is applied, the area of dead lithium decreases. For changing the electrochemical parameters, reducing the diffusion coefficient, increasing the interfacial mobility and reducing the anisotropic strength can effectively reduce the area of dead lithium.