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Lithium-ion batteries have dominated the field of electrochemical energy storage for years due to their high energy density. Recently, with the rapid development of E-mobility, the quest for high power and high energy batteries with reduced production costs has aroused great interest and is still a huge challenge. The energy density at battery level can be increased by using electrodes with thicknesses > 150 μm. However, capacity fade of thick-film electrodes at C-rates > C/2 is observed. To compensate the capacity loss, 3D architectures with a high aspect ratio are produced using ultrafast laser ablation. In addition, aqueous processing of cathodes using water-based binders can achieve environmentally friendly production and cost reduction by replacing the conventional organic PVDF binder and the toxic and volatile NMP solvent. However, the pH value of aqueous processed cathode slurries increases to 12 due to the reaction between active material and water, which decreases the specific capacity of the cells and on the other side results in chemical corrosion of the current collector during casting. In order to determine the optimal pH range and avoid the damage of the current collector, slurries with pH values ranging from 8 to 12 are manufactured.
In this work, thick-film Li(Ni0.6Mn0.2Co0.2)O2 electrodes are manufactured with aqueous binders and acid adjustment, and are subsequently structured using ultrafast laser ablation. This combination is beneficial to achieve green production, low cost, high power, and high energy application of lithium-ion batteries.
Laser direct patterning of battery materials enable a rather new technical approach in order to adjust 3D surface architectures and porosity of composite electrode materials such as LiCoO2, LiMn2O4, LiFePO4, Li(NiMnCo)O2, and Silicon. The architecture design, the increase of active surface area, and the porosity of electrodes or separator layers can be controlled by laser processes and it was shown that a huge impact on electrolyte wetting, lithium-ion diffusion kinetics, cell life-time and cycling stability can be achieved.
In general, the ultrafast laser processing can be used for precise surface texturing of battery materials. Nevertheless, regarding cost-efficient production also nanosecond laser material processing can be successfully applied for selected types of energy storage materials. A new concept for an advanced battery manufacturing including laser materials processing is presented. For developing an optimized 3D architecture for high power composite thick film electrodes electrochemical analytics and post mortem analytics using laser-induced breakdown spectroscopy were performed. Based on mapping of lithium in composite electrodes, an analytical approach for studying chemical degradation in structured and unstructured lithium-ion batteries will be presented.
In this paper, the formation of self-organized conical structures in intercalation materials such as LiCoO2 and LiNi1/3Mn1/3Co1/3O2 is investigated in detail. For this purpose, the cathode materials are exposed to excimer laser radiation with wavelengths of 248 nm and 193 nm leading to cone structures with outer dimensions in the micrometer range. The process of cone formation is investigated using laser ablation inductively coupled plasma mass spectrometry and laser-induced breakdown spectroscopy (LIBS). Cone formation can be initiated for laser fluences up to 3 J/cm2 while selective removal of lithium was observed to be one of the key issues for starting the cone formation process. It could be shown that material re-deposition supports the cone-growth process leading to a low loss of active material. Besides the cone formation process, laser-induced chemical surface modification will be analysed by LIBS.
Fs-laser microstructuring of laser-printed LiMn2O4 electrodes for manufacturing of 3D microbatteries
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