Abstract
In this study, a synchrotron transmission X-ray microscopy tomography system has been utilized to reconstruct the three-dimensional (3D) morphology of all-solid-state lithium-ion battery (ASSB) electrodes. The electrode was fabricated with a mixture of Li(Ni1/3Mn1/3Co1/3)O2, Li1.3Ti1.7Al0.3(PO4)3, and super-P. For the first time, a 3D numerical multi-physics model was developed to simulate the galvanostatic discharge performance of an ASSB, elucidating the spatial distribution of physical and electrochemical properties inside the electrode microstructure. The 3D model shows a wide range of electrochemical properties distribution in the solid electrolyte (SE) and the active material (AM) which might have a negative effect on ASSB performance. The results show that at high current rates, the void space hinders the ions’ movement and causes local inhomogeneity in the lithium-ion distribution. The simulation results for electrodes fabricated under two pressing pressures reveal that higher pressure decreases the void spaces, leading to a more uniform distribution of lithium ions in the SE due to more facile lithium ion transport. The approach in this study is a key step moving forward in the design of 3D ASSBs and sheds light on the physical and electrochemical property distribution in the SE, active material, and their interface.
Published Version
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