Three-dimensional image based modelling of transport parameters in lithium-sulfur batteries.

An elemental sulfur electrode was imaged with X-ray micro and nano computed tomography and segmented into its constituent phases. Morphological parameters including phase fractions and pore and particle size distributions were calculated directly from labelled image data, and flux based simulations were performed to determine the effective molecular diffusivity of the pore phase and electrical conductivity of the conductive carbon and binder phase, Deff and σeff, that can be used as an input for Li-S battery modelling. In addition to its crucial role in providing electrical conductivity within the sulfur electrode, the intrinsic porosity of the carbon binder domain was found to significantly influence Li-ion transport within the electrode. Neglecting this intrinsic porosity results in an overestimation of the electrical conductivity within the sulfur electrode, and an underestimation of the tortuosity of the Li-ion conducting phase by ca. 56%. The derivation of effective transport parameters directly from image data may aid in the development of more realistic models of Li-S battery systems by reducing the reliance on empirical correlations, and the uncertainties arising from assumptions made in these correlations.

Resolving Li-Ion Battery Electrode Particles Using Rapid Lab-Based X-Ray Nano-Computed Tomography for High-Throughput Quantification.

Vast quantities of powder leave production lines each day, often with strict control measures. For quality checks to provide the most value, they must be capable of screening individual particles in 3D and at high throughput. Conceptually, X-ray computed tomography (CT) is capable of this; however, achieving lab-based reconstructions of individual particles has, until now, relied upon scan-times on the order of tens of hours, or even days, and although synchrotron facilities are potentially capable of faster scanning times, availability is limited, making in-line product analysis impractical. This work describes a preparation method and high-throughput scanning procedure for the 3D characterization of powder samples in minutes using nano-CT by full-filed transmission X-ray microscopy with zone-plate focusing optics. This is demonstrated on various particle morphologies from two next-generation lithium-ion battery cathodes: LiNi0.8Mn0.1Co0.1O2 and LiNi0.6Mn0.2Co0.2O2; namely, NMC811 and NMC622. Internal voids are detected which limit energy density and promote degradation, potentially impacting commercial application such as the drivable range of an electric vehicle.