Confocal μ-XRF, μ-XAFS, and μ-XRD Studies of Sediment from a Nuclear Waste Disposal Natural Analogue Site and Fractured Granite Following a Radiotracer Migration Experiment

Spectrochimica Acta Part B: Atomic Spectroscopy

Nolf

Janssens

et al. 2008

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Results from combined µ-XRF and µ-XRD investigations of a uranium-rich tertiary sediment from a nuclear repository natural analog site in Ruprechtov, Czech Republic, are reported. The goal of the investigations is to identify arsenopyrite from diffraction patterns obtained in As-rich areas of the sample. Arsenopyrite has been revealed to be present in the sediment as thin coatings on the surface of Fe nodules from previous µ-XANES results and observed linear dependencies between Fe and As(0) distributions obtained from µ-XRF measurements. In thin sections of the sediment investigated here we find, however, neither diffraction reflections expected for arsenopyrite nor for other As-sulfides. The As(0) phase is likely present in the form of very small grains, or it is amorphous. Statistical analysis of the µ-XRD data using unsupervised classification and principle component analysis from selected sample areas also indicate that pyrite and siderite, but no arsenopyrite, are the sole diffracting phases. That pyrite and siderite are found in the same sample is an indication that the pH of the sediment environment during diagenesis must have been neutral. This allows us to refine our hypothesis for the mechanism of uranium immobilization.

Section: Introductionmentioning

confidence: 87%

µ-X-ray fluorescence and µ-X-ray diffraction investigations of sediment from the Ruprechtov nuclear waste disposal natural analog site

Spectrochimica Acta Part B: Atomic Spectroscopy

Nolf

Janssens

et al. 2008

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“…[30,[152][153][154]. An example of μ-XRF and μ-XAS speciation investigation of neptunium in fractured granite follows, and is intended to demonstrate the utility of the techniques [155][156][157].…”

Section: Nuclear Wastesmentioning

confidence: 99%

Recent advances in analysis of trace elements in environmental samples by X-ray based techniques (IUPAC Technical Report)

Terzano

Pure and Applied Chemistry

Falkenberg

et al. 2019

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Trace elements analysis is a fundamental challenge in environmental sciences. Scientists measure trace elements in environmental media in order to assess the quality and safety of ecosystems and to quantify the burden of anthropogenic pollution. Among the available analytical techniques, X-ray based methods are particularly powerful, as they can quantify trace elements in situ. Chemical extraction is not required, as is the case for many other analytical techniques. In the last few years, the potential for X-ray techniques to be applied in the environmental sciences has dramatically increased due to developments in laboratory instruments and synchrotron radiation facilities with improved sensitivity and spatial resolution. In this report, we summarize the principles of the X-ray based analytical techniques most frequently employed to study trace elements in environmental samples. We report on the most recent developments in laboratory and synchrotron techniques, as well as advances in instrumentation, with a special attention on X-ray sources, detectors, and optics. Lastly, we inform readers on recent applications of X-ray based analysis to different environmental matrices, such as soil, sediments, waters, wastes, living organisms, geological samples, and atmospheric particulate, and we report examples of sample preparation.

“…The granite stems from an underground laboratory (the Swedish Äspö Hard Rock Laboratory), where the migration of radionuclides under near-real in situ conditions can be investigated [1]. These investigations are relevant for safety of nuclear waste disposal.…”

Section: Introductionmentioning

confidence: 99%

Spatially resolved micro-X-ray fluorescence and micro-X-ray absorption fine structure study of a fractured granite bore core following a radiotracer experiment

Spectrochimica Acta Part B: Atomic Spectroscopy

Brendebach

Nolf

et al. 2009

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Spatially resolved X-ray absorption and fluorescence investigation with a micrometer-scale resolution on actinide-containing samples provide information necessary for safety assessment of nuclear waste disposal. In this paper one example of such an experiment is presented. This example entails neptunium speciation in a fractured granite bore core from the Swedish Äspö Hard Rock Laboratory following a radiotracer experiment using µ-XAFS and µ-XRF. In order to probe micro-volumes below the surface in the granite samples and thereby avoid potential changes in the Np speciation during cutting of the bore core, a confocal irradiation-detection geometry is employed. µ-XAFS results for a selected granite bore core cross section with~3 nmol Np/g reveal that Np, originally introduced as Np(V) in the tracer cocktail, is present in the granite in its reduced Np(IV) form. The Np(IV) is often present as particles, tens of µm in size. Elemental distribution maps show the tracer Np to be located in fissures and permeable channels not larger than 100 µm. The Np distribution appears often correlated with Zn also present in some fissures. We observe small granite fissures containing Fe (presumably Fe(II)), where we do not detect any Np. It is feasible that inflowing Np(V) has a shorter residence time in large fractures, while in the smaller fissures migration is slower, leading to longer residence times, i.e., reaction times, where it is reduced to less soluble Np(IV) and becomes thereby immobilized.