Experimentally Validated Three‐Dimensional Modeling of Organic‐Based Sodium‐Ion Battery Electrode Manufacturing

Abstract Lithium‐ion batteries (LIBs) have triggered the transition from internal combustion engine cars to electric vehicles, and are also making inroads into the grid storage sector, but the future quantity of batteries necessary poses several challenges in terms of raw material availability and sustainability. For this reason, many alternative chemistries are being proposed, such as substituting lithium with other more abundant elements, like sodium, or shifting from inorganic to organic‐based active materials, all of which require the development and testing of new chemistries. The electrode properties are not only a function of the chemistry, but also of the electrode manufacturing and resulting microstructure. In this work, we applied a three‐dimensional computational workflow, initially developed in the context of inorganic‐based electrodes for LIBs, to simulate the manufacturing of sodium‐ion battery anodes using an in‐house synthesized organic‐based active material. This computational workflow accounts for the slurry, its drying, and electrode calendering steps, and was validated by comparing simulated and experimental properties of the slurry and electrode. In addition, the calendering step was studied computationally to identify optimal electrode compressions, and the trend observed was confirmed experimentally through galvanostatic cycling in half‐cell configuration. The positive results shown here are an important demonstration of the chemistry neutrality of our manufacturing models, paving the way towards their application to both commercial and novel chemistries.