839 research outputs found
Hot isostatically pressed zirconolite wasteforms for actinide immobilisation
In order to demonstrate the deployment of Hot Isostatic Pressing (HIP) for the immobilisation of Pu stocks and residues, a series of active and inactive zirconolite formulations have been processed and characterised. In this instance, Ce, U, and Th have been applied as chemical surrogates for Pu4+. A range of formulations targeting isovalent Zr4+ site substitution (i.e. to simulate CaZr1-xPuxTi2O7) have been processed by HIP and characterised by powder X-ray diffraction, and scanning electron microscopy, in order to determine surrogate partitioning between the host zirconolite phase, and accessory phases that may have formed during the HIP process
Model of a fluid at small and large length scales and the hydrophobic effect
We present a statistical field theory to describe large length scale effects
induced by solutes in a cold and otherwise placid liquid. The theory divides
space into a cubic grid of cells. The side length of each cell is of the order
of the bulk correlation length of the bulk liquid. Large length scale states of
the cells are specified with an Ising variable. Finer length scale effects are
described with a Gaussian field, with mean and variance affected by both the
large length scale field and by the constraints imposed by solutes. In the
absence of solutes and corresponding constraints, integration over the Gaussian
field yields an effective lattice gas Hamiltonian for the large length scale
field. In the presence of solutes, the integration adds additional terms to
this Hamiltonian. We identify these terms analytically. They can provoke large
length scale effects, such as the formation of interfaces and depletion layers.
We apply our theory to compute the reversible work to form a bubble in liquid
water, as a function of the bubble radius. Comparison with molecular simulation
results for the same function indicates that the theory is reasonably accurate.
Importantly, simulating the large length scale field involves binary arithmetic
only. It thus provides a computationally convenient scheme to incorporate
explicit solvent dynamics and structure in simulation studies of large
molecular assemblies
Influence of transition metal charge compensation species on phase assemblage in zirconolite ceramics for Pu immobilisation
Immobilisation of Pu in a zirconolite matrix (CaZrTi2O7) is a viable pathway to disposition. A-site substitution, in which Pu4+ is accommodated into the Ca2+ site in zirconolite, coupled with sufficient trivalent M3+/Ti4+ substitution (where M3+ = Fe, Al, Cr), has been systematically evaluated using Ce4+ as a structural analogue for Pu4+. A broadly similar phase assemblage of zirconolite-2M and minor perovskite was observed when targeting low levels of Ce incorporation. As the targeted Ce fraction was elevated, secondary phase formation was influenced by choice of M3+ species. Co-incorporation of Ce/Fe resulted in the stabilisation of a minor Ce-containing perovskite phase at high wasteloading, whereas considerable phase segregation was observed for Cr3+ incorporation. The most favourable substitution approach appeared to be achieved with the use of Al3+, as no perovskite or free CeO2 was observed. However, high temperature treatments of Al containing specimens resulted in the formation of a secondary Ce-containing hibonite phase
Single and vertically coupled type II quantum dots in a perpendicular magnetic field: exciton groundstate properties
The properties of an exciton in a type II quantum dot are studied under the
influence of a perpendicular applied magnetic field. The dot is modelled by a
quantum disk with radius , thickness and the electron is confined in the
disk, whereas the hole is located in the barrier. The exciton energy and
wavefunctions are calculated using a Hartree-Fock mesh method. We distinguish
two different regimes, namely (the hole is located at the radial
boundary of the disk) and (the hole is located above and below the
disk), for which angular momentum transitions are predicted with
increasing magnetic field. We also considered a system of two vertically
coupled dots where now an extra parameter is introduced, namely the interdot
distance . For each and for a sufficient large magnetic field,
the ground state becomes spontaneous symmetry broken in which the electron and
the hole move towards one of the dots. This transition is induced by the
Coulomb interaction and leads to a magnetic field induced dipole moment. No
such symmetry broken ground states are found for a single dot (and for three
vertically coupled symmetric quantum disks). For a system of two vertically
coupled truncated cones, which is asymmetric from the start, we still find
angular momentum transitions. For a symmetric system of three vertically
coupled quantum disks, the system resembles for small the pillar-like
regime of a single dot, where the hole tends to stay at the radial boundary,
which induces angular momentum transitions with increasing magnetic field. For
larger the hole can sit between the disks and the state
remains the groundstate for the whole -region.Comment: 11 pages, 16 figure
Review of zirconolite crystal chemistry and aqueous durability
Zirconolite (CaZrTi2O7) has been identified as a candidate ceramic wasteform for the immobilisation and disposal of Pu inventories, for which there is no foreseen future use. Here, we provide an overview of relevant zirconolite solid solution chemistry with respect to Ce, U and Pu incorporation, alongside a summary of the available literature on zirconolite aqueous durability. The zirconolite phase may accommodate a wide variety of tri- and tetravalent actinide and rare-earth dopants through isovalent and heterovalent solid solution, e.g. CaZr1–xPuxTi2O7 or Ca1–xPuxZrTi2–2xFe2xO7. The progressive incorporation of actinides within the zirconolite-2M parent structure is accommodated through the formation of zirconolite polytypoids, such as zirconolite-4M or 3T, depending on the choice of substitution regime and processing route. A variety of standardised durability tests have demonstrated that the zirconolite phase exhibits exceptional chemical durability, with release rates of constituent elements typically <10−5 gm−2·d−1. Further work is required to understand the extent to which polytype formation and surrogate choice influence the dissolution behaviour of zirconolite wasteforms
Serum Metabolomics and Incidence of Atrial Fibrillation (from the Atherosclerosis Risk in Communities Study)
We have previously identified associations of 2 circulating secondary bile acids (glycocholenate and glycolithocolate sulfate) with atrial fibrillation (AF) risk in 1,919 blacks in the Atherosclerosis Risk in Communities cohort. We aimed to replicate these findings in an independent sample of 2,003 white and black Atherosclerosis Risk in Communities participants, and performed a new metabolomic analysis in the combined sample of 3,922 participants, followed between 1987 and 2013. Metabolomic profiling was done in baseline serum samples using gas and liquid chromatography mass spectrometry. AF was ascertained from electrocardiograms, hospitalizations, and death certificates. We used multivariable Cox regression to estimate hazard ratios (HR) and 95% confidence intervals (95%CI) of AF by 1 standard deviation difference of metabolite levels. Over a mean follow-up of 20 years, 608 participants developed AF. Glycocholenate sulfate was associated with AF in the replication and combined samples (HR 1.10, 95% CI 1.00, 1.21 and HR 1.13, 95% CI 1.04, 1.22, respectively). Glycolithocolate sulfate was not related to AF risk in the replication sample (HR 1.02, 95% CI 0.92, 1.13). An analysis of 245 metabolites in the combined cohort identified 3 additional metabolites associated with AF after multiple-comparison correction: pseudouridine (HR 1.18, 95% CI 1.10, 1.28), uridine (HR 0.86, 95% CI 0.79, 0.93) and acisoga (HR 1.17, 95% CI 1.09, 1.26). In conclusion, we replicated a prospective association among a previously identified secondary bile acid, glycocholenate sulfate, and AF incidence, and identified new metabolites involved in nucleoside and polyamine metabolism as markers of AF risk
A feasibility investigation of laboratory based X-ray absorption spectroscopy in support of nuclear waste management
X-ray Absorption Spectroscopy is a technique of fundamental importance in nuclear waste management, as an element specific probe of speciation, which governs radionuclide solubility, immobilisation and migration. Here, we exploit recent developments in laboratory instrumentation for X-ray Absorption Spectroscopy, based on a Rowland circle geometry with a spherically bent crystal analyser, to demonstrate speciation in prototype ceramic and glass-ceramic waste forms. Laboratory and synchrotron XANES data acquired from the same materials, at the Ce and U L3 edges, were found to be in excellent quantitative agreement. We establish that analysable laboratory XANES data may be acquired, and interpreted for speciation, even from quite dilute absorber concentrations of a few mol%, albeit with data acquisition times of several hours. For materials with suitable absorber concentrations, this approach will enable routine element specific speciation studies to support rapid optimisation of radioactive waste forms and analysis of radiological materials in a purpose designed laboratory, without the risk associated with transport and manipulation at a synchrotron radiation facility
Copy Number Variations Associated With Obesity‐Related Traits in African Americans: A Joint Analysis Between GENOA and HyperGEN
Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/95398/1/oby.2012.162.pdfhttp://deepblue.lib.umich.edu/bitstream/2027.42/95398/2/oby_2790_sm_oby2012162_coi.pd
Study of the , and decays
We present an approach to study the decay modes of the into a vector
meson and a tensor meson, taking into account the nature of the ,
, resonances as dynamically generated
states from the vector meson-vector meson interaction. We evaluate four ratios
of partial decay widths in terms of a flavor dependent OZI breaking parameter
and the results obtained compare favorably with experiment. The fit to the data
is possible due to the particular strength and sign of the couplings of the
resonances to pairs of vector mesons given by the theory, thus providing a
nontrivial test for the idea of these tensor states as dynamically generated
from the vector-vector interaction.Comment: published versio
Chemical state mapping of simulant Chernobyl lava-like fuel containing material using micro-focused synchrotron X-ray spectroscopy
Uranium speciation and redox behaviour is of critical importance in the nuclear fuel cycle. X-ray absorption near-edge spectroscopy (XANES) is commonly used to probe the oxidation state and speciation of uranium, and other elements, at the macroscopic and microscopic scale, within nuclear materials. Two-dimensional (2D) speciation maps, derived from microfocus X-ray fluorescence and XANES data, provide essential information on the spatial variation and gradients of the oxidation state of redox active elements such as uranium. In the present work, we elaborate and evaluate approaches to the construction of 2D speciation maps, in an effort to maximize sensitivity to the U oxidation state at the U L3-edge, applied to a suite of synthetic Chernobyl lava specimens. Our analysis shows that calibration of speciation maps can be improved by determination of the normalized X-ray absorption at excitation energies selected to maximize oxidation state contrast. The maps are calibrated to the normalized absorption of U L3 XANES spectra of relevant reference compounds, modelled using a combination of arctangent and pseudo-Voigt functions (to represent the photoelectric absorption and multiple-scattering contributions). We validate this approach by microfocus X-ray diffraction and XANES analysis of points of interest, which afford average U oxidation states in excellent agreement with those estimated from the chemical state maps. This simple and easy-to-implement approach is general and transferrable, and will assist in the future analysis of real lava-like fuel-containing materials to understand their environmental degradation, which is a source of radioactive dust production within the Chernobyl shelter
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