Visualizing Longitudinal and Transversal Strain Effects in High-Energy NMC Cathodes Induced By Intense Calendering

One of several challenges in improving the performance of lithium-ion batteries is the enhancement of energy density. Apart from the development of ever better active materials, considerable potential for improvement can be found in the complex manufacturing process. The manufacturing of lithium-ion battery cells exhibits a long, mostly sequential process chain with numerous interdependent parameters and quality-determining characteristics. Among slurry mixing and coating, calendering is the most challenging process step and considered of superior importance to the quality of the electrode. Calendering refers to compressing the porous coating layers of the electrode to a predetermined thickness. To obtain the desired energy density and to prepare a homogeneous electrode thickness it is necessary to densify the coating of the electrodes. In this, more electrochemically active material can be accommodated in every unit of electrode volume. In essence, this defines the potential energy density of the cell. As for high-energy battery cells energy density is one of the most important optimization criteria to achieve ambitious requirements for automotive applications calendering is of crucial importance.

However, compression of the electrode is not merely beneficial to the overall performance of the cell. It is a trade-off between achieving high energy density and, on the contrary, damaging the electrode’s structure by applying high mechanical forces. An effect rarely taken into account is mechanical strain induced to the electrode’s metal foil underlying the coating, which can lead to serious issues in manufacturing and malfunction of the battery cell.

This paper addresses macroscopic changes in electrode’s metal foils resulting from intense calendering procedures of high-energy NMC cathodes.  Figure 1 exemplarily depicts an area-resolved longitudinal strain map showing irreversible deformation from calendering. The left green section reflects an uncoated edge of the electrode which is not deformed during calendering. The coated section of the specimen is deformed significantly. The data is derived from before/after comparison of the electrode’s surface, conducted with a non-contact optical 3D deformation measuring system. To minimize undesired strain inducement, multi-calendering strategies are assessed which gently apply loads and at the same time still provide for highly compressed electrodes.