Optimizing Structural Patterns for 3D Electrodes in Lithium-Ion Batteries for Enhanced Fast-Charging Capability and Reduced Lithium Plating

The most common pattern types for anode structuring, in particular the line, grid, and hexagonal-arranged hole pattern were evaluated in a comparable setup in full-cells and symmetrical cells. The cells with structured electrodes were compared to reference cells with unstructured anodes of similar areal capacity (4.3 mAh cm-2) and the onset of lithium plating during fast-charging was determined in situ by differential voltage analysis of the voltage relaxation and ex situ by post-mortem analysis. Furthermore, electrochemical impedance spectroscopy measurements on symmetrical cells were used to determine the ionic resistance of structured and unstructured electrodes of similar areal capacity. All cells with structured electrodes showed lower ionic resistances and an onset of lithium plating shifted to higher C-rates compared to cells with unstructured electrodes. The structure patterns with capillary structures, i.e., lines and grids, showed significant reduced lithium plating during fast-charging and a higher rate capability compared to reference cells with unstructured electrodes and cells with hole structured electrodes. The continuous rewetting of the electrode with liquid electrolyte by capillary forces and the reduced ionic resistance of the 3D electrode are identified as key factors in improving overall battery performance. The data of the studied cells were used to calculate the resulting energy and power densities of prospective commercial pouch cells and potential pitfalls in the comparison to cells with unstructured electrodes were identified.