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

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

Optimization of K-edge subtraction imaging using a pixellated spectroscopic detector

Conventional K-edge subtraction imaging is based around the acquisition of two separate images at energies respectively below and above the K-edge of a contrast agent. This implies increased patient dose with respect to a conventional procedure and potentially incorrect image registration due to patient motion. © 2012 IEEE

Tungsten Bronze Barium Neodymium Titanate (Ba 6–3 Nd 8+2 Ti 18 O 54 ): An Intrinsic Nanostructured Material and Its Defect Distribution

We investigated the structure of the tungsten bronze barium neodymium titanates Ba6–3nNd8+2nTi18O54, which are exploited as microwave dielectric ceramics. They form a complex nanostructure, which resembles a nanofilm with stacking layers of ∼12 Å thickness. The synthesized samples of Ba6–3nNd8+2nTi18O54 (n = 0, 0.3, 0.4, 0.5) are characterized by pentagonal and tetragonal columns, where the A cations are distributed in three symmetrically inequivalent sites. Synchrotron X-ray diffraction and electron energy loss spectroscopy allowed for quantitative analysis of the site occupancy, which determines the defect distribution. This is corroborated by density functional theory calculations. Pentagonal columns are dominated by Ba, and tetragonal columns are dominated by Nd, although specific Nd sites exhibit significant concentrations of Ba. The data indicated significant elongation of the Ba columns in the pentagonal positions and of the Nd columns in tetragonal positions involving a zigzag arrangement of atoms along the b lattice direction. We found that the preferred Ba substitution occurs at Nd[3]/[4] followed by Nd[2] and Nd[1]/[5] sites, which is significantly different to that proposed in earlier studies. Our results on the Ba6–3nNd8+2nTi18O54 “perovskite” superstructure and its defect distribution are particularly valuable in those applications where the optimization of material properties of oxides is imperative; these include not only microwave ceramics but also thermoelectric materials, where the nanostructure and the distribution of the dopants will reduce the thermal conductivity

Operando and Postreaction Diffraction Imaging of the La-Sr/CaO Catalyst in the Oxidative Coupling of Methane Reaction

A La−Sr/CaO catalyst was studied operando during the oxidative coupling of methane (OCM) reaction using the X-ray diffraction computed tomography technique. Full-pattern Rietveld analysis was performed in order to track the evolving solid-state chemistry during the temperature ramp, OCM reaction, as well as after cooling to room temperature. We observed a uniform distribution of the catalyst main components: La2O3, CaO−SrO mixed oxide, and the hightemperature rhombohedral polymorph of SrCO3. These were stable initially in the reaction; however, doubling the gas hourly space velocity resulted in the decomposition of SrCO3 to SrO, which subsequently led to the formation of a second CaO−SrO mixed oxide. These two mixed CaO−SrO oxides differed in terms of the extent of Sr incorporation into their unit cell. By applying Vegard’s law during the Rietveld refinement, it was possible to create maps showing the spatial variation of Sr occupancy in the mixed CaO−SrO oxides. The formation of the Srdoped CaO species is expected to have an important role in this system through the enhancement of the lattice oxygen diffusion as well as increased catalyst basicity