3D Correlative Imaging of Lithium Ion Concentration in a Vertically Oriented Electrode Microstructure with a Density...

The performance of Li⁺ ion batteries (LIBs) is hindered by steep Li⁺ ion concentration gradients in the electrodes. Although thick electrodes (≥300 µm) have the potential for reducing the proportion of inactive components inside LIBs and increasing battery energy density, the Li⁺ ion concentration gradient problem is exacerbated. Most understanding of Li⁺ ion diffusion in the electrodes is based on computational modeling because of the low atomic number (Z) of Li. There are few experimental methods to visualize Li⁺ ion concentration distribution of the electrode within a battery of typical configurations, for example, coin cells with stainless steel casing. Here, for the first time, an interrupted in situ correlative imaging technique is developed, combining novel, full-field X-ray Compton scattering imaging with X-ray computed tomography that allows 3D pixel-by-pixel mapping of both Li⁺ stoichiometry and electrode microstructure of a LiNi_0.8 Mn_0.1 Co_0.1 O₂ cathode to correlate the chemical and physical properties of the electrode inside a working coin cell battery. An electrode microstructure containing vertically oriented pore arrays and a density gradient is fabricated. It is shown how the designed electrode microstructure improves Li⁺ ion diffusivity, homogenizes Li⁺ ion concentration through the ultra-thick electrode (1 mm), and improves utilization of electrode active materials.