Digital Techniques Assisted in Tailoring Electrode Structure to Optimize Electrode Kinetics

Abstract Poor rate performance limits the application of high-areal-loading electrodes in energy storage, largely due to cathode microstructure. In this study, we integrated X-ray computed tomography (XCT) with digital technology to quantify the correlation between electrode structure and internal kinetic performance of lithium-ion electrodes. Results show that electrode structure intricately influences internal kinetics, thereby affecting rate capacity and nominal potential. Based on the parametric relationship between electrode structure and electrochemical-thermal properties, we explored the effects of structural regulation on electrode performance. Vertical channels significantly enhanced the rate capability and ohmic heating rate of small-particle electrodes, while solid-phase diffusion (SPD) dominated the discharge performance of large-particle electrodes, diminishing the impact of tortuosity strategies. Furthermore, electrodes with abundant SPD barriers exhibit unidirectional propagation of reaction fronts, resulting in a deeper SPD-limited region. This observation inspired the integration of two structural strategies that favor both mass transport and reaction penetration. Optimized electrode structures enhanced energy density at high rates and accommodated diverse particle sizes and thicknesses. Additionally, the coupling effect of the heat transfer environment on electrode performance was investigated. This study presents a novel paradigm for bottom-up electrode design using microstructure-resolved model, providing both microscopic mechanisms and quantitative insights for advanced battery development.