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To improve interface adhesion between anode film and Cu foil, ultrafast laser structuring was implemented to construct dot patterns with a variety of periodic spacing (25, 50, and 75 lm) on Cu foil. The microstructure and electrochemical performance of anode films coated on those structured Cu foils were characterized. It was shown that adhesive force of the electrodes increased as periodic distance between the dots on the Cu foil decreased. Comparison of XRD patterns of the wet slurries with the dried anode films showed that after drying in the case of 50 lm period dot structured Cu foils the most graphite particles were aligned with the c-axis, vertical to the Cu foil surface. EIS, CV, and rate capability measurements confirmed that the anode film on the 50 lm dot period Cu foil had the lowest impedance, strongest lithiation and de-lithiation peaks, and highest discharge capacity. The cycling test carried out under C/2 rate confirmed that the cells with the 50 lm dot interval Cu foil showed the highest capacity retention. We inferred that this was due to the relatively shorter diffusive path in the anode due to vertical orientation of more graphite particles against the laser structured Cu foil.

The 3D battery concept applied on silicon–graphite electrodes (Si/C) has revealed a significant improvement of battery performances, including high-rate capability, cycle stability, and cell lifetime. 3D architectures provide free spaces for volume expansion as well as additional lithium diffusion pathways into the electrodes. Therefore, the cell degradation induced by the volume change of silicon as active material can be significantly reduced, and the high-rate capability can be achieved. In order to better understand the impact of 3D electrode architectures on rate capability and degradation process of the thick film silicon–graphite electrodes, we applied laser-induced breakdown spectroscopy (LIBS). A calibration curve was established that enables the quantitative determination of the elemental concentrations in the electrodes. The structured silicon–graphite electrode, which was lithiated by 1C, revealed a homogeneous lithium distribution within the entire electrode. In contrast, a lithium concentration gradient was observed on the unstructured electrode. The lithium concentration was reduced gradually from the top to the button of the electrode, which indicated an inhibited diffusion kinetic at high C-rates. In addition, the LIBS applied on a model electrode with micropillars revealed that the lithium-ions principally diffused along the contour of laser-generated structures into the electrodes at elevated C-rates. The rate capability and electrochemical degradation observed in lithium-ion cells can be correlated to lithium concentration profiles in the electrodes measured by LIBS.