Process–Structure–Property Correlations in Twin-Screw Extrusion of Graphitic Negative Electrode Pastes for Lithium Ion Batteries Focusing on Kneading Concentrations

A continuous mixing process with a twin-screw extruder was investigated for graphite-based negative electrode pastes for high-power applications. In the extrusion-based mixing process, the first kneading concentration is one of the key processing parameters for systematic optimization of relevant electrode paste properties like viscosity and particle size distribution. For different active materials at a constant electrode paste composition, a clear correlation of increasing kneading concentration with decreasing viscosity can be observed up to a certain reversal point, initiating a change in the trend and the rheological behavior, thus indicating a process limit. The fundamental effects causing this change and the associated impact on materials and battery performance were evaluated by applying further analytical methods and electrochemical characterization. It is revealed that the change in viscosity is associated with enhanced de-agglomeration of the carbon black additive and with partial particle grinding of the active material and thus a partial change in the interlayer distance of graphene layers and, correspondingly, the electrochemical behavior of the active material. Beyond this, correlations between processing parameters and product properties are presented. Furthermore, indicators are suggested with which monitoring of the machine parameters enables the detection of changes in the electrode paste characteristics.