  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.
