Understanding the limitations of thick electrodes on the rate capability of high-energy density lithium-ion batteries

Abstract

As a core component of transportation electrification, lithium-ion batteries need to address two critical challenges: achieving high energy density and enabling fast charging. However, changes in electrode thickness could result in a trade-off between these two characteristics. Herein, the impact of electrode thickness on the electrochemical performance, thermal behavior, as well as energy and power density of LiNi0.8Co0.1Mn0.1O2(NCM)/graphite batteries are investigated through mathematical modeling. Underutilization of active materials of the thick electrode is identified as the primary limitation on rate capability, which can be attributed to the slow solid-state diffusion and poor electrolyte transport within the electrode, especially the enlarged concentration gradients in the solid phase and the lithium depletion in the electrolyte phase during high-rate charging. Evolutions of local current density and heat generation rate along the electrode thickness are compared, identifying the underlying mechanism of inducing uneven reaction kinetics inside the battery. The trade-off between the energy and power density as a function of electrode thickness is investigated based on the limitations of charge transfer and mass transport. Furthermore, the rate-limiting factors under various application requirements are elucidated. This study will provide guidance for the electrode design of high-energy-density batteries with fast-charging capabilities.