Dispersion of U-series natural radionuclides in stream sediments from Edale, UK

The spatial distribution of 238U-series radionuclides, specifically 238U, 234U, 230Th and 226Ra, has been determined in stream sediments from Edale, Derbyshire, United Kingdom, to explore the behaviour of U-series radionuclides during weathering.</p

Identification and characterization of radioactive particles in the environment

Radioactive particles have been released into the environment from different sources (e.g. nuclear weapon tests, nuclear accidents, nuclear reprocessing plants, and use of depleted uranium (DU) munitions). Nuclear fuel particles have been released from authorised discharges of low-level radioactive effluent into the Irish Sea sediments from the nuclear fuel reprocessing plant at Sellafield, UK. Following the use of depleted uranium munitions in the Gulf wars and the Balkan conflicts, the environmental impact of depleted uranium and its behaviour in the environment have been of great concern. In this thesis, nuclear fuel particles released from Sellafield and retained in the intertidal Irish Sea salt marsh sediments, and DU particles arising from testing of DU munitions against hard targets and corrosion of DU metal buried in soil at Eskmeals firing range, UK, were investigated using a range of microanalytical, analytical and radiometric techniques. The particles were characterised in terms of size and morphology, elemental and radionuclide compositions, isotopic composition of associated radionuclides and, crystalline structure of uranium forms. The results demonstrate the usefulness of the applied techniques in characterising environmental radioactive particles, and lead to better understanding of the origin, behaviour and fate of these particles in the environment. The nuclear fuel particles were 1-20 µm in size, composed mainly of uranium and irradiated in the reactor as the transuranium elements (Np, Pu, Am and Cm) can be identified. The isotopic composition of uranium and plutonium suggest that these particles are derived from reprocessing of spent fuel. The results demonstrated the persistence for some decades of irradiated fuel particles in estuarine marine environment.DU particles from firing impacts were oxidized uranium forms (UO2 and U3O8) and composed mainly of uranium with few molten particles composed of a mixture of uranium and iron. DU particles from corrosion processes were mainly sand grains coated with metaschoepite corrosion product. The results showed the diversity of particles which can be produced through the use of DU munitions and the potential for these to persist in the environment for many years.EThOS - Electronic Theses Online ServiceUniversity of Aleppo, SyriaGBUnited Kingdo

Multimodal x-ray microanalysis of a UFeO4 : evidence for the environmental stability of ternary U(v) oxides from depleted uranium munitions testing

An environmentally aged radioactive particle of UFeO4 recovered from soil contaminated with munitions depleted uranium (DU) was characterised by microbeam synchrotron X-ray analysis. Imaging of uranium speciation by spatially resolved X-ray diffraction (μ-XRD) and X-ray absorption spectroscopy (μ-XAS) was used to localise UFeO4 in the particle, which was coincident with a distribution of U(V). The U oxidation state was confirmed using X-ray Absorption Near Edge Structure (μ-XANES) spectroscopy as +4.9 ± 0.15. Le-Bail fitting of the particle powder XRD pattern confirmed the presence of UFeO4 and a minor alteration product identified as chernikovite (H3O)(UO2)(PO4)·3H2O. Refined unit cell parameters for UFeO4 were in good agreement with previously published values. Uranium–oxygen interatomic distances in the first co-ordination sphere were determined by fitting of Extended X-ray Absorption Fine Structure (μ-EXAFS) spectroscopy. The average first shell U–O distance was 2.148 ± 0.012 Å, corresponding to a U valence of +4.96 ± 0.13 using bond valence sum analysis. Using bond distances from the published structure of UFeO4, U and Fe bond valence sums were calculated as +5.00 and +2.83 respectively, supporting the spectroscopic analysis and confirming the presence of a U(V)/Fe(III) pair. Overall this investigation provides important evidence for the stability of U(V) ternary oxides, in oxic, variably moist surface environment conditions for at least 25 years

Cesium and Strontium Contamination of Nuclear Plant Stainless Steel : Implications for Decommissioning and Waste Minimization

Stainless steels can become contaminated with radionuclides at nuclear sites. Their disposal as radioactive waste would be costly. If the nature of steel contamination could be understood, effective decontamination strategies could be designed and implemented during nuclear site decommissioning in an effort to release the steels from regulatory control. Here, batch uptake experiments have been used to understand Sr and Cs (fission product radionuclides) uptake onto AISI Type 304 stainless steel under conditions representative of spent nuclear fuel storage (alkaline ponds) and PUREX nuclear fuel reprocessing (HNO3). Solution (ICP-MS) and surface measurements (GD-OES depth profiling, TOF-SIMS, and XPS) and kinetic modeling of Sr and Cs removal from solution were used to characterize their uptake onto the steel and define the chemical composition and structure of the passive layer formed on the steel surfaces. Under passivating conditions (when the steel was exposed to solutions representative of alkaline ponds and 3 and 6 M HNO3), Sr and Cs were maintained at the steel surface by sorption/selective incorporation into the Cr-rich passive film. In 12 M HNO3, corrosion and severe intergranular attack led to Sr diffusion into the passive layer and steel bulk. In HNO3, Sr and Cs accumulation was also commensurate with corrosion product (Fe and Cr) readsorption, and in the 12 M HNO3 system, XPS documented the presence of Sr and Cs chromates.Peer reviewe

Casimir force acting on magnetodielectric bodies embedded in media

Within the framework of macroscopic quantum electrodynamics, general expressions for the Casimir force acting on linearly and causally responding magnetodielectric bodies that can be embedded in another linear and causal magnetodielectric medium are derived. Consistency with microscopic harmonic-oscillator models of the matter is shown. The theory is applied to planar structures and proper generalizations of Casimir's and Lifshitz-type formulas are given.Comment: 15 pages, 2 figures; minor additions and corrections, to appear in PR

Isotopic and Compositional Variations in Single Nuclear Fuel Pellet Particles Analyzed by Nanoscale Secondary Ion Mass Spectrometry

Article published under an ACS AuthorChoice LicenseThe Collaborative Materials Exercise (CMX) is organized by the Nuclear Forensics International Technical Working Group, with the aim of advancing the analytical capabilities of the participating organizations and providing feedback on the best approaches to a nuclear forensic investigation. Here, model nuclear fuel materials from the 5th CMX iteration were analyzed using a NanoSIMS 50L (CAMECA) in order to examine inhomogeneities in the U-235/U-238 ratio and trace element abundance within individual, micrometer scale particles. Two fuel pellets were manufactured for the exercise and labelled CMX-5A and CMX-5B. These pellets were created using different processing techniques, but both had a target enrichment value of U-235/U-238 = 0.01. Particles from these pellets were isolated for isotopic and trace element analysis. Fifteen CMX-5A particles and 20 CMX-5B particles were analyzed, with both sample types displaying inhomogeneities in the U isotopic composition at a sub-micrometer scale within individual particles. Typical particle diameters were similar to 1.5 to 41 mu m for CMX-5A and similar to 1 to 61 mu m for CMX-5B. The CMX-5A particles were shown to be more isotopically homogeneous, with a mean U-235/U-238 atom ratio of 0.0130 +/- 0.0066. The CMX-5B particles showed a predominantly depleted mean U-235/U-238 atom ratio of 0.0063 +/- 0.0094, which is significantly different to the target enrichment value of the pellet and highlights the potential variation of U-235/U-238 in U fuel pellets at the micrometer scale. This study details the successful application of the NanoSIMS 50L in a mock nuclear forensic investigation by optimizing high-resolution imaging for uranium isotopics.Peer reviewe