Lithium-ion batteries have become the most promising energy storage devices in recent years. However, the simultaneous increase of energy density and power density is still a huge challenge. Ultrafast laser structuring of electrodes is feasible to increase power density of lithium-ion batteries by improving the lithium-ion diffusion kinetics. The influences of laser processing pattern and film thickness on the rate capability and energy density were investigated using Li(Ni_0.6Mn_0.2Co_0.2)O₂ (NMC 622) as cathode material. NMC 622 electrodes with thicknesses from 91 µm to 250 µm were prepared, while line patterns with pitch distances varying from 200 µm to 600 µm were applied. The NMC 622 cathodes were assembled opposing lithium using coin cell design. Cells with structured, 91 µm thick film cathodes showed lesser capacity losses with C-rates 3C compared to cells with unstructured cathode. Cells with 250 µm thick film cathode showed higher discharge capacity with low C-rates of up to C/5, and the structured cathodes showed higher discharge capacity, with C-rates of up to 1C. However, the discharge capacity deteriorated with higher C-rate. An appropriate choice of laser generated patterns and electrode thickness depends on the requested battery application scenario; i.e., charge/discharge rate and specific/volumetric energy density.

The electrochemical performance of lithium-ion batteries is directly influenced by type of active material as well as its morphology. In order to evaluate the impact of particle morphology in thick-film electrodes, Li(Ni_0.6Mn_0.2Co_0.2)O₂ (NMC 622) cathodes with bilayer structure consisting of two different particle sizes were manufactured and electrochemically characterized in coin cells design. The hierarchical thick-film electrodes were generated by multiple casting using NMC 622 (TA) with small particle size of 6.7 µm and NMC 622 (BA) with large particle size of 12.8 µm. Besides, reference electrodes with one type of active material as well as with two type of materials established during mixing process (BT) were manufactured. The total film thickness of all hierarchical composite electrodes were kept constant at 150 µm, while the thicknesses of TA and BA were set at 1:2, 1:1, and 2:1. Meanwhile, three kinds of thin-film cathodes with 70 µm were applied to represent the state-of-the-art approach. Subsequently, ultrafast laser ablation was applied to generate groove structures inside the electrodes. The results demonstrate that cells with thin-film or thick-film cathode only containing TA, cells with bilayer electrode containing TBA 1:2, and cells with laser-structured electrodes show higher capacity at C/2 to 5C, respectively.

Lithium-ion batteries have led the revolution in portable electronic devices and electrical vehicles due to their high gravimetric energy density. In particular, layered cathode material Li(Ni_0.6Mn_0.2Co_0.2)O₂ (NMC 622) can deliver high specific capacities of about 180 mAh/g. However, traditional cathode manufacturing involves high processing costs and environmental issues due to the use of organic binder polyvinylidenfluoride (PVDF) and highly toxic solvent N-methyl-pyrrolidone (NMP). In order to overcome these drawbacks, aqueous processing of thick-film NMC 622 cathodes was studied using carboxymethyl cellulose and fluorine acrylic hybrid latex as binders. Acetic acid was added during the mixing process to obtain slurries with pH values varying from 7.4 to 12.1. The electrode films could be produced with high homogeneity using slurries with pH values smaller than 10. Cyclic voltammetry measurements showed that the addition of acetic acid did not affect the redox reaction of active material during charging and discharging. Rate capability tests revealed that the specific capacities with higher slurry pH values were increased at C-rates above C/5. Cells with laser structured thick-film electrodes showed an increase in capacity by 40 mAh/g in comparison to cells with unstructured electrodes.

An increase in the energy density on the cell level while maintaining a high power density can be realized by combining thick-film electrodes and the 3D battery concept. The effect of laser structuring using different pattern types on the electrochemical performance was studied. For this purpose, LiNi_0.6Mn_0.2Co_0.2O₂ (NMC 622) thick-film cathodes were prepared with a PVDF binder and were afterward structured using ultrafast laser ablation. Eight different pattern types were realized, which are lines, grids, holes, hexagonal structures, and their respective combinations. In addition, the mass loss caused by laser ablation was kept the same regardless of the pattern type. The laser-structured electrodes were assembled in coin cells and subsequently electrochemically characterized. It was found that when discharging the cells for durations of less than 2 h, a significant, positive impact of laser patterning on the electrochemical cell performance was observed. For example, when discharging was performed for one hour, cells containing laser-patterned electrodes with different structure types exhibited a specific capacity increase of up to 70 mAh/g in contrast to the reference ones. Although cells with a hole-patterned electrode exhibited a minimum capacity increase in the rate capability analysis, the combination of holes with lines, grids, or hexagons led to further capacity increases. In addition, long-term cycle analyses demonstrated the benefits of laser patterning on the cell lifetime, while cyclic voltammetry highlighted an increase in the Li-ion diffusion kinetics in cells containing hexagonal-patterned electrodes.

For the first time, the laser structuring of large-footprint electrodes with a loading of 4 mAh cm⁻² has been validated in a relevant environment, including subsequent multi-layer stack cell assembly and electrochemical characterization of the resulting high-capacity lithium-ion pouch cell prototypes, i.e., a technological readiness level of 6 has been achieved for the 3D battery concept. The structuring was performed using a high-power ultrashort-pulsed laser, resulting in well-defined line structures in electrodes without damaging the current collector, and without melting or altering the battery active materials. For cells containing structured electrodes, higher charge and discharge capacities were measured for C-rates >1C compared to reference cells based on unstructured electrodes. In addition, cells with structured electrodes showed a three-fold increase in cycle lifetime at a C-rate of 1C compared to those with reference electrodes.

Lithium-ion batteries are currently one of the most important energy storage devices for various applications. However, it remains a great challenge to achieve both high energy density and high-power density while reducing the production costs. Cells with three-dimensional electrodes realized by laser ablation are proven to have enhanced electrochemical performance compared to those with conventional two-dimensional electrodes, especially at fast charging/discharging. Nevertheless, laser structuring of electrodes is still limited in terms of achievable processing speed, and the upscaling of the laser structuring process is of great importance to gain a high technology readiness level. In the presented research, the impact of different laser structuring strategies on the electro-chemical performance was investigated on aqueous processed Li(Ni₀.₆Mn₀.₂Co₀.₂)O₂ cathodes with acid addition during the slurry mixing process. Rate capability analyses of cells with laser structured aqueous processed electrodes exhibited enhanced performance with capacity increases of up to 60 mAh/g at high current density, while a 65% decrease in ionic resistance was observed for cells with laser structured electrodes. In addition, pouch cells with laser structured acid-added electrodes maintained 29–38% higher cell capacity after 500 cycles and their end-of-life was extended by a factor of about 4 in contrast to the reference cells with two-dimensional electrodes containing common organic solvent processed polyvinylidene fluoride binder.