| Abstract Scope |
We use a data-driven approach to assess the heterogeneous electrochemistry and mechanics in composite cathodes. We visualize the morphological defects at multi-scales ranging from the macroscopic composite, particle ensembles, to individual single particles. Particle fracture and interfacial debonding are identified in a large set of tomographic data. Mechanical damage of active particles is highly heterogeneous. The difference originates from the polarization of the electrolyte potential, various local conducting environments, and thus the non-uniform distribution of the activation energy for the charge transfer reaction. We model the kinetics of intergranular fracture and interfacial degradation to assess the heterogeneous mechanical damage in composite electrodes using microstructure-informed mechanics modeling. We quantify the influence of the mechanical damage on the metrics of battery performance. More interestingly, the interfacial failure reconstructs the conductive network and redistributes the electrochemical activities that render a dynamic nature of electrochemistry and mechanics evolving over time in the composite electrodes. |