Mechanical, Electrical, and Ionic Behavior of Lithium‐Ion Battery Electrodes via Discrete Element Method Simulations

Herein, a discrete element method (DEM) approach is proposed to investigate the impact of the calendering process on the electrical and ionic conductivities and on the adhesion strength of Li[Ni1/3 Mn1/3 Co1/3]O2 (NMC)‐based electrodes. For this purpose, key correlations between the microstructure and these electrode‐scale properties are established using the outcomes of the simulations and real experiments. In addition, the evolution of the structure and the development of mechanical stress are also studied numerically during electrochemical cycling, offering a closer insight into the intercalation mechanism. Finally, the impact of the initial noncalendered porosity on the electrode mechanical response is examined, showing that higher initial porosities lead to lower final porosities under same calendering loads. Overall, this work demonstrates the potential of DEM simulations in improving the understanding of the microstructure and mechanics of lithium‐ion electrodes. Correlations between the microstructure and electrode macroscopic properties are established using discrete element method (DEM) simulations. The goal is to assess the impact of the calendering production step and the mechanism of intercalation on the electrode structure, mechanics, and connectivity.