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Quantitative chemical mapping of battery electrodes is a rather new post-mortem analytics method for identifying and describing chemical degradation processes in lithium-based battery systems. In consideration of future applications, the development of lithium-ion batteries is quite essential in order to meet requirements such as improved cell lifetime (>5000 cycles), high energy density at the cell level (>250 W h kg−1), reduced charging times ( 2500 W kg−1), and reduced manufacturing costs (<150 $ per kW h). One novel approach that can handle a contemporaneous enhancement of energy and power density is the development of a novel cell design, mandated in a three-dimensional (3D) arrangement. This so-called “3D battery concept” enables electrode configurations with improved lithium-ion diffusion kinetics and provides reduced mechanical stresses which could arise during battery cycling. Within this study, laser-induced breakdown spectroscopy (LIBS) was applied quantitatively as a powerful analytical tool in order to study chemical degradation mechanisms and the impact of 3D electrode architectures on lithium distribution. It could be shown so far that free-standing electrode architectures can provide new lithium-insertion pathways which enhance the capability of the electrode material to operate under abuse conditions. Elemental mapping and elemental depth-profiling were applied for characterizing the electrode as a function of cell lifetime and architecture. For the first time, it was demonstrated that LIBS can be used to quantitatively describe lithium distribution in a 3D battery with specific design parameters. Finally, new scientific findings regarding electrochemically driven degradation and aging mechanisms of laser-structured, embossed, and unstructured NMC electrodes were explored.

Laser-induced breakdown spectroscopy for the quantitative measurement of lithium concentration profiles in structured and unstructured electrodes