New electrode architectures promise huge potential for improving batteries’ electrochemical properties, such as power density, energy density, and lifetime. In this work, the use of laser-induced forward transfer (LIFT) was employed and evaluated as a tool for the development of advanced electrode architectures. For this purpose, it was first confirmed that the printing process has no effect on the transferred battery material by comparing the electrochemical performance of the printed anodes with state-of-the-art coated ones. For this, polyvinylidene fluoride (PVDF) was used as a binder and n-methyl-2-pyrrolidone (NMP) as a solvent, which is reported to be printable. Subsequently, multilayer electrodes with flake-like and spherical graphite particles were printed to test if a combination of their electrochemical related properties can be realized with measured specific capacities ranging from 321 mAh$·$g⁻¹ to 351 mAh$·$g⁻¹. Further, a multilayer anode design with a silicon-rich intermediate layer was printed and electrochemically characterized. The initial specific capacity was found to be 745 mAh$·$g⁻¹. The presented results show that the LIFT technology offers the possibility to generate alternative electrode designs, promoting research in the optimization of 3D battery systems.

To enhance the performance of state-of-the-art lithium-ion batteries, high-capacity silicon is increasingly introduced as active material for anodes. Furthermore, advanced batteries with new electrode architectures—so-called 3D architectures—can provide significantly enhanced electrochemical performance compared to state-of-the-art batteries. To facilitate and speed up the architectural development, the laser-induced forward transfer (LIFT) process was applied as a digital additive manufacturing method. As polyvinylidene fluoride (PVDF), the binder commonly used in the LIFT process, is not a suitable binder for silicon-containing electrodes due to its weak binding forces, polyacrylic acid (PAA) was introduced as a binder for use in printable electrode pastes. Since water as a solvent in such pastes evaporates quickly and the corresponding printing time would be too short, glycerol was added to the solvent mixture in different amounts. The silicon in the printed electrodes reaches a specific capacity of more than 3000 mAh$·{\mathrm{g}}^{–1}$ for most of the printed anodes. To further improve the electrochemical performance of the printed electrodes, as well as the rheology of the slurries, two different conductive additives with different particle sizes were used.

With the ongoing global warming energy storages as lithium-ion batteries gain more importance due to the increasing amount of generated current with renewable energies. To further boost the battery development with the focus of advanced materials and architecture the LIFT-process offers a direct digital additive manufacturing tool for fast prototyping. In this work the impact of the printing quality in dependency of the particle size was investigated with the focus of the depiction of the laser beam profile with single voxels. Since electrode inks commonly consist of materials with different particle sizes the edge quality of printed areas was analyzed in dependency of the distance between the coated slurry and the substrate and the glycerol content in the solvent mixture. In the latter study, it was shown that a certain solvent mixture exhibits an optimized edge quality for a certain distance.