Li-ion battery electrode manufacturing is raising broad interest from both experimental and computational perspectives, due to its impact on the electrode and cell cost, mechanical and electrochemical properties. Among the different manufacturing processes, drying can trigger heterogeneities within the electrode mesostructure because of additive migration. Despite acknowledging that these heterogeneities significantly affect electrode properties, the drying step is often under evaluated at the experimental level and modeled through homogenized approaches. In this work, we present the first physics-based three-dimensional model able to mimic additive migration during drying, unlocking the generation of three-dimensional heterogeneous electrode mesostructures. We analyzed the effect of drying rate on the final electrode mesostructure, the dynamics of additive migration and how the developed heterogeneities affect the following manufacturing step, i.e., calendering. The results are in agreement with previous experimental findings and indicate trends not previously disclosed. Lastly, the implementation of complex drying protocols (three-stage drying) was tested and compared to its experimental counterpart.

由于其对电极和电池成本、机械和电化学性能的影响，锂离子电池电极制造从实验和计算的角度引起了广泛的兴趣。在不同的制造过程中，由于添加剂迁移，干燥会引发电极细观结构内的异质性。尽管承认这些异质性会显着影响电极性能，但干燥步骤通常在实验水平上评估不足，并通过均质化方法进行建模。在这项工作中，我们提出了第一个基于物理的三维模型，能够模拟干燥过程中的添加剂迁移，解锁三维异质电极细观结构的生成。我们分析了干燥速率对最终电极细观结构的影响，即压延。结果与先前的实验结果一致，并表明先前未公开的趋势。最后，测试了复杂干燥协议（三级干燥）的实施，并与其实验对应物进行了比较。