Electrode Architecture Effects on Lithium-Ion Battery Aging: A Pseudo-Two-Dimensional Modeling Approach

Abstract This study investigates the electrochemical performance and aging behavior of lithium-ion batteries (LIBs), focusing on the architectural effects of electrode and separator geometries alongside active material particle sizes. A pseudo-two-dimensional (P2D) model is employed to simulate lithium intercalation, solid diffusion, and coupled thermal behavior across a full-factorial design space. Despite its one-dimensional formulation, the model provides an optimal balance between computational efficiency and comparative predictive capability. A range of cell configurations is analyzed by varying anode, cathode, and separator thicknesses, as well as particle sizes, to assess their coupled impact on cell performance. The results demonstrate that while smaller particle diameters mitigate solid-state diffusion limitations and enhance capacity retention specifically under high C-rates, minimizing separator thickness significantly reduces inactive mass fractions, boosting baseline specific capacity even in designs with larger commercial particles. However, higher electrode loadings lead to increased volumetric heat-generation rates, particularly within thicker electrode configurations. A comparative assessment is also conducted in terms of cell mass, enabling the estimation of specific energy and power scaled to a standard format. Although limited to relative heat-generation trends by the one-dimensional thermal approximation, the results provide practical guidelines for advanced LIB design, successfully balancing electrochemical performance, volumetric engineering, and computational cost.