Electrode manufacturing is at the core of the lithium ion battery (LIB) fabrication process. The electrode microstructure and the electrochemical performance are determined by the adopted manufacturing parameters. However, in view of the strong interdependencies between these parameters, evaluating their influence on the performance is not a trivial task. In this work we present an experimentally validated 3D-resolved electrochemical model of a NMC111-based electrode which reveals how slurry formulation and calendering degree affect the electrode performance. A series of electrodes with different formulations and calendering degrees were fabricated at the experimental level. Corresponding three-dimensional manufacturing models were built based on the same experimental manufacturing parameters to generate the digital counterparts of the experimental electrodes that were then used in the electrochemical model. The results of simulations and experiments were compared individually. Among the manufacturing parameters analyzed, we found that the major factors linking manufacturing parameters and electrode performance are the carbon and binder domain (CBD) distribution within the electrode volume, and the electrostatic potential difference between the electrode and the current collector. A well-connected electronic conductive network throughout the electrode is vital for ensuring full utilization of active material, and it was found that increasing calendering degree is effective in reducing interfacial impedance. This work uncovers, based on a dual modeling/experimental approach, the essence of how electrode manufacturing process takes effect on electrode performance by influencing its microstructure.
