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.

中文翻译：

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使用同步加速器透射 X 射线显微断层扫描对全固态锂离子电池进行三维建模

在这项研究中，同步加速器透射 X 射线显微镜断层扫描系统已被用于重建全固态锂离子电池 (ASSB) 电极的三维 (3D) 形态。电极由 Li(Ni1/3Mn1/3Co1/3)O2、Li1.3Ti1.7Al0.3(PO4)3 和 super-P 的混合物制成。首次开发了 3D 数值多物理模型来模拟 ASSB 的恒电流放电性能，阐明电极微结构内物理和电化学性能的空间分布。3D 模型显示了固体电解质 (SE) 和活性材料 (AM) 中广泛的电化学特性分布，这可能对 ASSB 性能产生负面影响。结果表明，在高电流速率下，空隙空间阻碍了离子的 运动并导致锂离子分布的局部不均匀性。在两种压制压力下制造的电极的模拟结果表明，较高的压力会减少空隙空间，由于更容易的锂离子传输，导致锂离子在 SE 中的分布更均匀。本研究中的方法是推进 3D ASSB 设计的关键一步，并阐明了 SE、活性材料及其界面中的物理和电化学特性分布。