Removing multiple outliers and single-crystal artefacts from X-ray diffraction computed tomography data

This paper reports a simple but effective filtering approach to deal with single-crystal artefacts in X-ray diffraction computed tomography (XRD-CT). In XRD-CT, large crystallites can produce spots on top of the powder diffraction rings, which, after azimuthal integration and tomographic reconstruction, lead to line/streak artefacts in the tomograms. In the simple approach presented here, the polar transform is taken of collected two-dimensional diffraction patterns followed by directional median/mean filtering prior to integration. Reconstruction of one-dimensional diffraction projection data sets treated in such a way leads to a very significant improvement in reconstructed image quality for systems that exhibit powder spottiness arising from large crystallites. This approach is not computationally heavy which is an important consideration with big data sets such as is the case with XRD-CT. The method should have application to two-dimensional X-ray diffraction data in general where such spottiness arises

Interlaced X-ray diffraction computed tomography

An X-ray diffraction computed tomography data-collection strategy that allows, post experiment, a choice between temporal and spatial resolution is reported. This strategy enables time-resolved studies on comparatively short timescales, or alternatively allows for improved spatial resolution if the system under study, or components within it, appear to be unchanging. The application of the method for studying an Mn–Na–W/SiO2 fixed-bed reactor in situ is demonstrated. Additionally, the opportunities to improve the data-collection strategy further, enabling post-collection tuning between statistical, temporal and spatial resolutions, are discussed. In principle, the interlaced scanning approach can also be applied to other pencil-beam tomographic techniques, like X-ray fluorescence computed tomography, X-ray absorption fine structure computed tomography, pair distribution function computed tomography and tomographic scanning transmission X-ray microscopy

In situ X-ray Diffraction Computed Tomography studies examining the thermal and chemical stabilities of working Ba0.5Sr0.5Co0.8Fe0.2O3-δ membranes during oxidative coupling of methane

In this study we present the results from two in situ X-ray diffraction computed tomography experiments of catalytic membrane reactors (CMRs) using Ba0.5Sr0.5Co0.8Fe0.2O3−δ (BSCF) hollow fibre membranes and Na-Mn-W/SiO2 catalyst during the oxidative coupling of methane (OCM) reaction. The negative impact of CO2, when added to the inlet gas stream, is seen to be mainly related to the C2+ yield, while no evidence of carbonate phase(s) formation is found during the OCM experiments. The main degradation mechanism of the CMR is suggested to be primarily associated with the solid-state evolution of the BSCF phase rather than the presence of CO2. Specifically, in situ XRD-CT and post-mortem SEM/EDX measurements revealed a collapse of the cubic BSCF phase, formation of secondary phases, which include needle-like structures and hexagonal Ba6Co4O12, and formation of a BaWO4 layer, the latter being a result of chemical interaction between the membrane and catalyst materials at high temperatures

Infrared absorption spectra of hot ammonia

Infrared absorption spectra of NH3 have been obtained at high resolution (0.02 cm−1) at seven temperatures between 296 and 973 K. The spectra were recorded using a Bruker IFS 125 infrared Fourier transform spectrometer in the 2400–5500 cm−1 region and empirical lower state energies have been obtained by comparison of line strengths at different temperatures. Using two reference line lists, quantum number assignments have been made for each temperature for between 1660 and 3020 transitions, with J up to 22. The line lists obtained provide accurate line positions as well as intensities and experimental lower state energies at temperatures relevant for modeling the atmospheres of brown dwarfs and exoplanets

Multi-length scale 5D diffraction imaging of Ni-Pd/CeO2-ZrO2/Al2O3 catalyst during partial oxidation of methane

A 5D diffraction imaging experiment (with 3D spatial, 1D time/imposed operating conditions and 1D scattering signal) was performed with a Ni–Pd/CeO2–ZrO2/Al2O3 catalyst. The catalyst was investigated during both activation and partial oxidation of methane (POX). The spatio-temporal resolved diffraction data allowed us to obtain unprecedented insight into the behaviour and fate of the various metal and metal oxide species and how this is affected by the heterogeneity across catalyst particles. We show firstly, how Pd promotion although facilitating Ni reduction, over time leads to formation of unstable Ni–Pd metallic alloy, rendering the impact of Pd beyond the initial reduction less important. Furthermore, in the core of the particles, where the metallic Ni is primarily supported on Al2O3, poor resistance towards coke deposition was observed. We identified that this preceded via the formation of an active yet metastable interstitial solid solution of Ni–C and led to the exclusive formation of graphitic carbon, the only polymorph of coke observed. In contrast, at the outermost part of the catalyst particle, where Ni is predominantly supported on CeO2–ZrO2, the graphite formation was mitigated but sintering of Ni crystallites was more severe