Finite Element Simulation of NMC Particle Fracture During Calendering: A Route to Optimize Electrode Microstructures

Beyond active material intrinsic properties, the electrode manufacturing process is a crucial step to reach high energy density and long‐life of Li‐ion batteries. In particular, very high pressures are applied to the electrode during the calendering step, that directly influence the microstructure and the electrochemical performances. This article reports the first calendering simulation of a nickel‐manganese‐cobalt (NMC) cathode using a finite element method, including the post‐fracturation behavior of the secondary NMC particles. Calibrated with nanoindentation experiments, the mechanical model provides stress–strain predictions fully consistent with experimental data. On assemblies up to 100 particles, simulations reveal three calendering regimes along compression: particle rearrangement, moderate‐pressure fracturing, and complete crushing. The model shows the strong sensitivity of the electrode microstructure to the calendering pressure level, and can thus be used as a guidance in the multicriteria optimization of the manufacturing process.