A dedicated apparatus has been developed for studying structural changes in amorphous and disordered crystalline materials substantially in real time. The apparatus, which can be set up on beamlines BL04B2 and BL08W at SPring-8, mainly consists of a large two-dimensional flat-panel detector and high-energy X-rays, enabling total scattering measurements to be carried out for time-resolved pair distribution function (PDF) analysis in the temperature range from room temperature to 873 K at pressures of up to 20 bar. For successful time-resolved analysis, a newly developed program was used that can monitor and process two-dimensional image data simultaneously with the data collection. The use of time-resolved hardware and software is of great importance for obtaining a detailed understanding of the structural changes in disordered materials, as exemplified by the results of commissioned measurements carried out on both beamlines. Benchmark results obtained using amorphous silica and demonstration results for the observation of sulfide glass crystallization upon annealing are introduced.

In this study, lithium reaction distributions, dependent on the charge–discharge rate, were non-destructively visualized for a commercial lithium-ion battery, using the Compton scattering imaging technique. By comparing lithium reaction distributions obtained at two different charge–discharge speeds, residual lithium ions were detected at the center of the negative electrode in a fully discharged state, at a relatively high-speed discharge rate. Moreover, we confirmed that inhomogeneous reactions were facilitated at a relatively high-speed charge–discharge rate, in both the negative and positive electrodes. A feature of our technique is that it can be applied to commercially used lithium-ion batteries, because it uses high-energy X-rays with high penetration power. Our technique thus opens a novel analyzing pathway for developing advanced batteries.

Compton scattering imaging using high-energy synchrotron x rays allows the visualization of the spatiotemporal lithiation state in lithium-ion batteries probed in operando. Here, we apply this imaging technique to the commercial 18650-type cylindrical lithium-ion battery. Our analysis of the line shapes of the Compton scattering spectra taken from different electrode layers reveals the emergence of inhomogeneous lithiation patterns during the charge-discharge cycles. Moreover, these patterns exhibit oscillations in time where the dominant period corresponds to the timescale of the charging curve.

Synchrotron-based Compton scattering imaging with intense high-energy X-rays allows the visualization of light element substances in an electrochemical device under an operando condition. In this study, we apply this imaging technique to a water-contained, porous carbon-based composite, which is used as a material for the gas diffusion layer in polymer electrolyte fuel cells. Analyses of the two-dimensional intensity images of Compton scattered X-rays provide the cross-sectional distributions of liquid water, as well as the depth dependency of the water content. In addition, the analyses reveal a significant interaction between the carbon materials and water droplets.