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Electrode manufacturing is at the core of the lithium ion battery (LIB)fabrication process. The electrode microstructure and the electrochemicalperformance are determined by the adopted manufacturing parameters. However, inview of the strong interdependencies between these parameters, evaluating theirinfluence on the performance is not a trivial task. In this work we present anexperimentally validated 3D-resolved electrochemical model of a NMC111-basedelectrode which reveals how slurry formulation and calendering degree affectthe electrode performance. A series of electrodes with different formulationsand calendering degrees were fabricated at the experimental level.Corresponding three-dimensional manufacturing models were built based on thesame experimental manufacturing parameters to generate the digital counterpartsof the experimental electrodes that were then used in the electrochemicalmodel. The results of simulations and experiments were compared individually.Among the manufacturing parameters analyzed, we found that the major factorslinking manufacturing parameters and electrode performance are the carbon andbinder domain (CBD) distribution within the electrode volume, and theelectrostatic potential difference between the electrode and the currentcollector. A well-connected electronic conductive network throughout theelectrode is vital for ensuring full utilization of active material, and it wasfound that increasing calendering degree is effective in reducing interfacialimpedance. This work uncovers, based on a dual modeling/experimental approach,the essence of how electrode manufacturing process takes effect on electrodeperformance by influencing its microstructure.

An Experimentally-Validated 3D Electrochemical Model Revealing Electrode Manufacturing Parameters Effects on Battery Performance