No abstract

Lithium sulfur (Li–S) batteries have great potential as a successor to Li-ion batteries, but their commercialization has been complicated by a multitude of issues stemming from their complex multiphase chemistry. In situ X-ray tomography investigations enable direct observations to be made about a battery, providing unprecedented insight into the microstructural evolution of the sulfur cathode and shedding light on the reaction kinetics of the sulfur phase. Here, for the first time, the morphology of a sulfur cathode was visualized in 3D as a function of state of charge at high temporal and spatial resolution. While elemental sulfur was originally well-dispersed throughout the uncycled cathode, subsequent charging resulted in the formation of sulfur clusters along preferred orthogonal orientations in the cathode. The electrical conductivity of the cathode was found not to be rate-limiting, suggesting the need to optimize the loading of conductive carbon additives. The carbon and binder domain and surrounding bulk pore phase were visualized in the in situ cell, and contrast changes within both phases were successfully extracted. The applications of this technique are not limited to microstructural and morphological characterization, and the volumetric data can serve as a valuable input for true 3D computational modeling of Li–S batteries.

Although a great variety of strategies to suppress Li dendrite have been proposed for lithium metal batteries (LMBs), a deeper understanding of the factors playing a crucial role during extended electrochemical cycling is often lacking. Herein, the morphological reversibility of the Li-based anode for nextgeneration batteries under three prevalent strategies, i.e., the use of Li−Al alloys, polymer coating, and anodic aluminum oxide (AAO) membrane attachment, has been sophisticatedly investigated by nondestructive visualization. The characterizations clearly capture the unprecedented morphological evolution of the Li-based anode during the electrochemical cycling. Furthermore, the results unambiguously indicate the formation of the "dead" electrochemically generated porous structures regardless of >99% cycling efficiency shown in Li symmetric cells in all three cell configurations. The results presented here shed light on further understanding of the morphological evolution of the Li anode under different scenarios, and it also enlightens us on new research activities that may assist in propelling the commercialization of LMBs.

Transverse coherence of the x-ray beam from a bending magnet source was studied along multiple directions using a 2-D π/2 phase grating by measuring interferogram visibilities at different distances behind the grating. These measurements suggest that the preferred measuring orientation of a 2-D checkerboard grating is along the diagonal directions of the square blocks, where the interferograms have higher visibility and are not sensitive to the deviation of the duty cycle of the grating period. These observations are verified by thorough wavefront propagation simulations. The accuracy of the measured coherence values was also validated by the simulation and analytical results obtained from the source parameters. In addition, capability of the technique in probing spatially resolved local transverse coherence is demonstrated.

Grating-based X-ray and neutron interferometry tomography using phase-stepping methods generates large data sets. An improved algorithm is presented for solving for the parameters to calculate transmissions, differential phase contrast, and dark-field images. The method takes advantage of the vectorization inherent in high-level languages such as Mathematica and MATLAB and can solve a 16 × 1k × 1k data set in less than a second. In addition, the algorithm can function with partial data sets. This is demonstrated with processing of a 16-step grating data set with partial use of the original data chosen without any restriction. Also, we have calculated the reduced chi-square for the fit and notice the effect of grating support structural elements upon the differential phase contrast image and have explored expanded basis set representations to mitigate the impact.