Abstract
The performance of lithium-ion batteries is limited by suboptimal energy density and power capability. A feasible approach is designing 3D electrode architectures where lithium ion transport in the electrolyte and active material can be optimized for improving the energy/power density. In this study, the influence of active material morphology and 3D electrode configurations is investigated with particular emphasis on solid-state transport and resulting implications on the performance. A morphology-detailed computational modeling is presented which simulates lithium transport in disparate 3D electrode configurations. The resulting lithium concentration in the 3D electrode constructs during discharging, relaxation, and charging process reveal a local sate of charge map. This is correlated with the electrode performance. This study demonstrates the role of active particle morphology and 3D architecture on the electrode relaxation behavior, which determines the resulting concentration gradient and performance.