Impact of Mechanical Degradation in Polycrystalline NMC Particle on the Electrochemical Performance of Lithium-Ion Batteries

Lithium-ion batteries (LIBs) are widely chosen for energy storage owing to their high coulombic efficiency and energy density. Within the positive electrode materials of LIBs, the structural integrity of secondary particles, composed of randomly oriented single-crystal primary particles, is crucial for sustained performance. These particles can fracture as a result of both mechanical stress and chemical interactions within the solid. Modelling LIBs is a complex task involving electro-chemo-mechanical phenomena and their interactions on different length scales. This study proposes a numerical modeling framework to investigate the active particle degradation and its impact on electrochemical performance. The model integrates mechanical and electrochemical processes, tracking crack evolution and mechanical failure through phase field damage. The coupled time-dependent non-linear partial differential equations are solved in a finite element framework using COMSOL Multiphysics. The model offers numerical insights into intergranular and transgranular fracture within secondary particles. The electrolyte infiltration into cracks reduces the electrochemical overpotential due to the increase in electrochemically active surface area, positively affecting performance. However, prolonged cycling with particle cracking poses severe threat to the battery performance and capacity. This comprehensive numerical modeling approach provides valuable insights into the intricate interplay of mechanical and electrochemical factors governing LIB performance and degradation.