Electrochemical Model-Based Investigation of Thick LiFePO4 Electrode Design Parameters

The electrification of the powertrain requires enhanced performance of lithium-ion batteries, mainly in terms of energy and power density. They can be improved by optimising the positive electrode, i.e., by changing their size, composition or morphology. Thick electrodes increase the gravimetric energy density but generally have an inefficient performance. This work presents a 2D modelling approach for better understanding the design parameters of a thick LiFePO4 electrode based on the P2D model and discusses it with common literature values. With a superior macrostructure providing a vertical transport channel for lithium ions, a simple approach could be developed to find the best electrode structure in terms of macro- and microstructure for currents up to 4C. The thicker the electrode, the more important are the direct and valid transport paths within the entire porous electrode structure. On a smaller scale, particle size, binder content, porosity and tortuosity were identified as very impactful parameters, and they can all be attributed to the microstructure. Both in modelling and electrode optimisation of lithium-ion batteries, knowledge of the real microstructure is essential as the cross-validation of a cellular and lamellar freeze-casted electrode has shown. A procedure was presented that uses the parametric study when few model parameters are known.