Comparison and modeling of aqueous dissolution rates of various uranium oxides

Purpose of this work was to measure and model the intrinsic dissolution rates of U oxides under a variety of well-controlled conditions that are relevant to a geologic repository. When exposed to air at elevated temperature, spent fuel may form the stable phase U{sub 3}O{sub 8}. Dehydrated schoepite, UO{sub 3}{center_dot}H{sub 2}O, exists in drip tests on spent fuel. Equivalent sets of U{sub 3}O{sub 8} and UO{sub 3}{center_dot}H{sub 2}O dissolution experiments allowed a systematic examination of the effects of temperature (25-75 C), pH(8-10), and carbonate (2-200x10{sup -4}molar) concentrations at atmospheric oxygen conditions. Results indicate that UO{sub 3}{center_dot}H{sub 2}O has a much higher dissolution rate (at least tenfold) than U{sub 3}O{sub 8} under the same conditions. The intrinsic dissolution rate of unirradiated U{sub 3}O{sub 8} is about twice that of UO{sub 2}. Dissolution of both U{sub 3}O{sub 8} and UO{sub 3}{center_dot}H{sub 2}O shows a very high sensitivity to carbonate concentration. Present results show a 25 to 50-fold increase in room-temperature UO{sub 3}{center_dot}H{sub 2}O dissolution rates between the highest and lowest carbonate concentrations. As with the UO{sub 2} dissolution data, the classical observed chemical kinetic rate law was used to model the U{sub 3}O{sub 8} dissolution rate data. The pH did not have much effect on the models, in agreement with earlier analysis of the UO{sub 2} and spent fuel dissolution data. However, carbonate concentration, not temperature, had the strongest effect on the U{sub 3}O{sub 8} dissolution rate. The U{sub 3}O{sub 8} dissolution activation energy was about 6000 cal/mol, compared with 7300 and 8000 cal/mol for spent fuel and UO{sub 2}, respectively

Continued studies of calorimeter performance at the Lawrence Livermore Laboratory

Calibrations of two calorimeters used for tritium and plutonium assays were made. Data from three new standards of about 0.5, 1, and 5 W were added to the results of a previous report and analyzed together. The accuracies of both calorimeters appear to fall within the specified 0.5 percent, although the data now available for the large calorimeter is insufficient to permit a more definite conclusion. An expression of the bias correction for each calorimeter with respect to the sample power cannot be determined. The bias of the medium thermopile-type calorimeter tends to be positive, however, and that of the large resistance-bridge design appears to be negative. (auth

Analyses and hydrogen-isotope-transport calculations of current and future designs of the LLL rotating-target neutron source

Analyses of the present titanium-tritide RTNS targets are presented. These results include the hydrogen-isotope content of new and used targets, metallography, scanning electron microscopy, and hydrogen-isotope-diffusion calculations using a heat-flow finite-difference computer code. These latter calculations indicate that a combination of long target life and high neutron output is optimized when the rate of hydrogen isotope evolution from the target balances the deposition rate from the beam. Auger spectra show that carbon and oxygen species are present in the bulk and on the surface. (auth

Second order gauge invariant gravitational perturbations of a Kerr black hole

We investigate higher than the first order gravitational perturbations in the Newman-Penrose formalism. Equations for the Weyl scalar $\psi_4,$ representing outgoing gravitational radiation, can be uncoupled into a single wave equation to any perturbative order. For second order perturbations about a Kerr black hole, we prove the existence of a first and second order gauge (coordinates) and tetrad invariant waveform, $\psi_I$, by explicit construction. This waveform is formed by the second order piece of $\psi_4$ plus a term, quadratic in first order perturbations, chosen to make $\psi_I$ totally invariant and to have the appropriate behavior in an asymptotically flat gauge. $\psi_I$ fulfills a single wave equation of the form ${\cal T}\psi_I=S,$ where ${\cal T}$ is the same wave operator as for first order perturbations and $S$ is a source term build up out of (known to this level) first order perturbations. We discuss the issues of imposition of initial data to this equation, computation of the energy and momentum radiated and wave extraction for direct comparison with full numerical approaches to solve Einstein equations.Comment: 19 pages, REVTEX. Some misprints corrected and changes to improve presentation. Version to appear in PR

Neutron star accretion and the neutrino fireball

The mixing necessary to explain the Fe'' line widths and possibly the observed red shifts of 1987A is explained in terms of large scale, entropy conserving, up and down flows (calculated with a smooth particle 2-D code) taking place between the neutron star and the explosion shock wave due to the gravity and neutrino deposition. Depending upon conditions of entropy and mass flux further accretion takes place in single events, similar to relaxation oscillator, fed by the downward flows of low entropy matter. The shock, in turn, is driven by the upflow of the buoyant high entropy bubbles. Some accretion events will reach a temperature high enough to create a neutrino fireball,'' a region hot enough, 11 Mev, so as to be partially opaque to its own (neutrino) radiation. The continuing neutrino deposition drives the explosion shock until the entropy of matter flowing downwards onto the neutron star is high enough to prevent further accretion. This process should result in a robust supernova explosion

A comparison of flare forecasting methods. II. Benchmarks, metrics and performance results for operational solar flare forecasting systems

YesSolar flares are extremely energetic phenomena in our Solar System. Their impulsive, often drastic radiative increases, in particular at short wavelengths, bring immediate impacts that motivate solar physics and space weather research to understand solar flares to the point of being able to forecast them. As data and algorithms improve dramatically, questions must be asked concerning how well the forecasting performs; crucially, we must ask how to rigorously measure performance in order to critically gauge any improvements. Building upon earlier-developed methodology (Barnes et al. 2016, Paper I), international representatives of regional warning centers and research facilities assembled in 2017 at the Institute for Space-Earth Environmental Research, Nagoya University, Japan to – for the first time – directly compare the performance of operational solar flare forecasting methods. Multiple quantitative evaluation metrics are employed, with focus and discussion on evaluation methodologies given the restrictions of operational forecasting. Numerous methods performed consistently above the “no skill” level, although which method scored top marks is decisively a function of flare event definition and the metric used; there was no single winner. Following in this paper series we ask why the performances differ by examining implementation details (Leka et al. 2019, Paper III), and then we present a novel analysis method to evaluate temporal patterns of forecasting errors in (Park et al. 2019, Paper IV). With these works, this team presents a well-defined and robust methodology for evaluating solar flare forecasting methods in both research and operational frameworks, and today’s performance benchmarks against which improvements and new methods may be compared

Age-Related Differences in Socio-demographic and Behavioral Determinants of HIV Testing and Counseling in HPTN 043/NIMH Project Accept

Youth represent a large proportion of new HIV infections worldwide, yet their utilization of HIV testing and counseling (HTC) remains low. Using the post-intervention, cross-sectional, population-based household survey done in 2011 as part of HPTN 043/NIMH Project Accept, a cluster-randomized trial of community mobilization and mobile HTC in South Africa (Soweto and KwaZulu Natal), Zimbabwe, Tanzania and Thailand, we evaluated age-related differences among socio-demographic and behavioral determinants of HTC in study participants by study arm, site, and gender. A multivariate logistic regression model was developed using complete individual data from 13,755 participants with recent HIV testing (prior 12 months) as the outcome. Youth (18–24 years) was not predictive of recent HTC, except for high-risk youth with multiple concurrent partners, who were less likely (aOR 0.75; 95% CI 0.61–0.92) to have recently been tested than youth reporting a single partner. Importantly, the intervention was successful in reaching men with site specific success ranging from aOR 1.27 (95% CI 1.05–1.53) in South Africa to aOR 2.30 in Thailand (95% CI 1.85–2.84). Finally, across a diverse range of settings, higher education (aOR 1.67; 95% CI 1.42, 1.96), higher socio-economic status (aOR 1.21; 95% CI 1.08–1.36), and marriage (aOR 1.55; 95% CI 1.37–1.75) were all predictive of recent HTC, which did not significantly vary across study arm, site, gender or age category (18–24 vs. 25–32 years)

CSNF Waste Form Degradation, Summary Abstraction

The purpose of this analysis is to provide a current summary of data and updated models for commercial spent nuclear fuel (CSNF) intrinsic (forward) dissolution (high water-flow) rates. A summary of the chemical interaction of UO{sub 2} with groundwater and its components is given in the initial analysis section. This analysis also provides a comparison of the three types of CSNF dissolution measurements available within and outside of the program. The three types of dissolution tests available are semi-static/batch, low-flow/drip, and high-flow/flow-through tests. This analysis also provides a summary of the gap and grain boundary radionuclide inventories of clad spent fuel. The final analysis topic is a comparison of the current knowledge of uranium mineral phases that form in laboratory tests with spent fuel and UO{sub 2} with the mineral assemblages found in natural uranium-bearing sites. This analysis will be incorporated into the Waste Form Degradation Process Model Report (PMR) for the Total Systems Performance Assessment-Site Recommendation. This report was developed in accordance with the technical product development plan Waste Package Materials Department Analysis and Modeling Reports Supporting the Waste Form PMR (CRWMS M and O 1999c). These models of CSNF degradation are bounding models that apply to all UO{sub 2}-based spent fuel expected to be disposed in a repository. These models are valid within the range of qualified experimental data: pH down to 3 and up to 10, oxygen pressure from 0.002 to 0.2 atmospheres, carbonate/bicarbonate concentrations from 2 x 10{sup -4} to 2 x 10{sup -2} molar. At pHs less than or equal to 7, these models are only shown to be valid at CO{sub 2} pressures of 10{sup -3} atmospheres. Corroborating data outside of these ranges indicate that the valid ranges may extend beyond those stated

Review of hydrogen isotope permeability through materials

This report is the first part of a comprehensive summary of the literature on hydrogen isotope permeability through materials that do not readily form hydrides. While we mainly focus on pure metals with low permeabilities because of their importance to tritium containment, we also give data on higher-permeability materials such as iron, nickel, steels, and glasses