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At least 163 records · Page 9

Simultaneous isotopic analysis of fission product Sr, Mo, and Ru in spent nuclear fuel particles by resonance ionization mass spectrometry

Abstract Fission product Sr, Mo, and Ru isotopes in six 10-μm particles of spent fuel from a pressurized water reactor were analyzed by resonance ionization mass spectrometry (RIMS) and evaluated for utility in nuclear material characterization. Previous measurements on these same samples showed widely varying U, Pu, and Am isotopic compositions owing to the samples’ differing irradiation environments within the reactor. This is also seen in Mo and Ru isotopes, which have the added complication of exsolution from the UO 2 fuel matrix. This variability is a hindrance to interpreting data from a collection of particles with incomplete provenance since it is not always possible to assign particles to the same batch of fuel based on isotopic analyses alone. In contrast, the measured 90 Sr/ 88 Sr ratios were indistinguishable across all samples. Strontium isotopic analysis can therefore be used to connect samples with otherwise disparate isotopic compositions, allowing them to be grouped appropriately for interpretation. Strontium isotopic analysis also provides a robust chronometer for determining the time since fuel irradiation. Because of the very high sensitivity of RIMS, only a small fraction of material in each of the 10 μm samples was consumed, leaving the vast majority still available for other analyses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Optimization of radiochromic film stacks to diagnose high-flux laser-accelerated proton beams

Here, we extend flatbed scanner calibrations of GafChromic EBT3, MD-V3, and HD-V2 radiochromic films using high-precision x-ray irradiation and monoenergetic proton bombardment. By computing a visibility parameter based on fractional errors, optimal dose ranges and transitions between film types are identified. The visibility analysis is used to design an ideal radiochromic film stack for the proton energy spectrum expected from the interaction of a petawatt laser with a cryogenic hydrogen jet target.

Curry, C. B. (ORCID:000000018756181X)↗

Harvesting Isotopically Pure Ac-225 from Ra-225 Produced in Thorium Target Spallation Reaction

A method for isolating Ra-225 from linear accelerator irradiated Th metal chemical processing waste streams has been established. Separating Ra-225 from the complex matrix following proton irradiation of Th metal provides a source of isotopically pure Ac-225 free of the Ac-227 impurity that is present in accelerator-produced Ac-225. Ra isotopes are first separated from the irradiated Th target via cation exchange methods. Importantly, the Ra-containing fraction is cleaned from residual citrate via dilute nitric acid washes (0.5 M) on AG50W-X8 resin. The mixed Ra isotopes are then further purified from Ba-140 impurity using a Sr resin column. Ra elutes through the resin with successive washes of 2.5 M HNO 3 while Ba-140 is retained. Ac-225 is then harvested by loading the Ra content onto an AG50W-X8 cation exchange column where the Ra-225 parent is eluted with 2.5 M HNO 3 before the Ac-225 daughter is eluted with 8 M HNO 3 .

07 ISOTOPE AND RADIATION SOURCES↗

Status Report on Characterization of High Burnup Fuel with Advanced Nondestructive Pulsed Neutron PIE

Characterizing irradiated or spent nuclear fuels with pulsed neutron techniques provides microstructural data such as phase fractions as well as crystallographic data, e.g. lattice parameters, from diffraction analysis. Diffraction characterization is complemented by spatially resolved mapping of isotope densities from energy-resolved neutron imaging, in particular neutron absorption resonance imaging, and overall bulk isotope assay with better sensitivity for minority isotopes from neutron absorption resonance spectroscopy without spatial resolution. Furthermore, after characterization at ambient condition, heating of irradiated or spent fuel will allow to characterize differences of e.g. lattice thermal expansion or phase transition temperature and kinetics compared to fresh fuel as well as enable the study of disappearance of irradiation defects. This data enables benchmarking of predictions of properties of irradiated fuels for which otherwise experimental data is sparse. The effort described here strives to characterize a section cut from a high-burnup fuel. Volumes smaller than entire fuel pellets or rodlets as proposed here, e.g. sections cut from a fuel pellet, to pave the way to characterize entire pellets or rodlets in the future.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Cosmic-ray exposure history of North Ray and South Ray material

Cosmic-ray exposure ages for two breccias, 68815 and 69935, in the vicinity of South Ray Crater give consistent values of 2.0 plus or minus 0.2 m.y. when measured by the Kr-81-Kr, Na-22-Ne, and particle track methods. These also agree with estimates of exposure ages made by others using microcrater counts on six rocks in the same vicinity, including 69935. It is likely that this represents the age of South Ray Crater. Soils from stations close to South Ray Crater appear to be mature, well-irradiated materials containing little, if any, of a 2 m.y. component. Reviewing various lines of evidence, it is concluded that there are no compelling reasons to believe that so-called South Ray soils contain a large fraction of South Ray ejecta. However, if they do contain such ejecta, this material must have been well irradiated in situ prior to being thrown out in the South Ray event. A chip from a large boulder on the rim of North Ray Crater gives a Kr-81-Kr age of 50.6 plus or minus 3.8 m.y. Similar ages are found by the Na-22-Ne and the particle track methods. The agreement of this result with other data on large North Ray boulders fixes the age of North Ray Crater as 50 m.y.

Behrmann, C.↗

Evaluation of AGR-3/4 In-pile Silver Release Predictions Against Post-Irradiation Examination Measurements

Fuel performance modeling codes that accurately predict the transport of radionuclides in high-temperature gas-cooled reactors that utilize tristructural isotopic (TRISO) fuel particles are an important aspect of reactor safety analyses. One objective of the Advanced Gas Reactor (AGR)-3/4 experiment was to assess the transport of fission products through fuel particles and their subsequent release into the compact matrix and structural graphite materials. This was accomplished by irradiating uranium oxycarbide (UCO) driver fuel particles and designed-to-fail (DTF) particles to serve as known sources of fission products. The fission product of particular interest when it comes to such transport is silver (Ag-110 m), as it has a 250-day half-life and has relatively high mobility in the TRISO coating layers. Furthermore, to assess the current modeling capabilities and diffusion parameters employed in the fuel performance codes PARFUME and BISON, the fractional release of silver release predicted by the two codes were compared against post-irradiation examination measurements from the AGR-3/4 experiment.

AGR-3/4 Experiment↗

Imaging and Analysis of Insoluble Electrorefiner Material

Throughout pyroprocessing efforts at the Hot Fuel Examination Facility (HFEF), insoluble material has accumulated in the Electrorefiner (ER) vessel. The objective of this effort was to analyze the accumulated material to determine its origin. Material was removed from the ER salt bath and distilled to remove excess salt prior to performing analysis. Three samples were sent for chemical and isotopic analysis and underwent an ethyl acetate-bromine dissolution to segregate the oxide fraction from the metal fraction. Actinide concentrations were determined using a quadrupole–inductively coupled plasma–mass spectrometer (Q-ICP-MS). Three additional samples were sent for morphologic and elemental analysis by scanning electron microscopy (SEM) with Energy Dispersive X-ray (EDX) analysis at the Irradiated Materials Characterization Laboratory (IMCL). Analyses suggest that the material is primarily composed of UO2. with a small fraction of metal. This study draws no single conclusion as to the origin of the insoluble material in the ER. The particle sizes and morphologies observed in SEM micrographs indicate that the larger particles observed may be a result of introducing material to the ER that has not been completely reduced in Oxide Reduction (OR) operations, which precede electrorefining. Smaller particles may be due to reactions with oxygen and moisture present in HFEF. This research suggests that microscopic analysis of fuel particles before and after OR operations (including after distillation) as well as the uranium product collected on the cathode in the ER would increase understanding about particle morphology within the pyrochemical process.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Thermal properties of U-Mo alloys irradiated under high fission power density

A variety of physical and thermal property measurements made on irradiated U-Mo alloy monolithic fuel samples with a Zr diffusion barrier and clad in Al alloy 6061 are reported. These properties form the basis for additional investigations in thermal behavior of U-Mo fuel under high performance research reactor irradiation conditions. Measurements were performed on samples harvested from fuel plates irradiated under high fission power density and surface heat flux and complement previous measurements on samples subjected to moderate fission power density and surface heat flux. Specific heat capacity of irradiated monolithic U-Mo increases with increasing temperature and fission density, but carries large uncertainties associated with thickness measurements used to determine the mass fraction of the layer constituents for extraction of the U-Mo specific heat capacity, specifically the very thin and nonuniform Zr diffusion barrier. Density of irradiated monolithic U-Mo decreases with increasing fission density resulting from fission gas swelling and porosity formation. Thermal diffusivity of irradiated monolithic U-Mo increased with increasing temperature and decreased with increasing fission density. Thermal conductivity of irradiated monolithic U-Mo increased with increasing temperature, and in general, appeared to decrease and become less sensitive to temperature with increasing fission density. Thermal conductivity measurements compared to a semi-empirical model agreed within ±30%. It is suspected that the main driver in deviation between model calculations and measurements is the fission gas swelling determination, which does not account for fission power density or irradiation temperature.

uranium (U), molybdenum, nuclear fuel, thermal con↗

Uncertainty in Annual Energy Resulting from Uncertain Irradiance Measurements

We report an analysis quantifying the contribution to uncertainty in annual energy projections from uncertainty in ground-measured irradiance. Uncertainty in measured irradiance is quantified for eight instruments by the difference from a well maintained, secondary standard pyranometer which is regarded as truthful. We construct a statistical model of irradiance uncertainty and apply the model to generate a sample of 100 annual time series of irradiance for each instrument. The sample is propagated through a common performance model for a reference photovoltaic system to quantify variation in annual energy. Although the measured irradiance varies from the reference by a few percent (standard deviation of 1-2%) the uncertainty in annual energy is on the order of a fraction of one percent. We propose a model for a factor that represents uncertainty in modeled annual energy that arises from uncertainty in ground-measured irradiance.

14 SOLAR ENERGY↗

Dose, LET, time and strain dependence of radiation-induced 53BP1 foci in 15 mouse strains ex vivo and associations to in vivo radiation susceptibility

We present a comparative analysis on the repair of radiation-induced DNA damage ex vivo in 15 strains of mice, including 5 inbred reference strains and 10 collaborative-cross strains, of both sexes. Non-immortalized primary skin fibroblasts derived from 76 mice were subjected to both low- and high-LET radiation (0.1, 1 and 4 Gy of X rays; 1.1 and 3 particles/100μm2 of 350 MeV/n 40Ar and 600 MeV/n 56Fe). Automated image quantification of 53BP1 radiation-induced foci (RIF) during the first 4-48 h post-irradiation was performed as a function of dose and LET. Similarly to what we had previously reported for immortalized human cell lines [1], we observed a saturation of RIF number with dose at 4h post-irradiation, with more RIF/Gy for lower LET (X rays and 40Ar) compared to 56Fe. However at later time points (24h and above), the trend was inverted with more RIF/Gy for higher LET. Our data suggest that multiple DSBs cluster into RIF: as the linear density of DSBs increases with LET, so does the probability of having more DSBs per RIF, which makes it more difficult for cells to fully resolve high-LET-induced RIF, explaining the hypersensitivity to high-LET radiation despite a low number of RIF. Taking into account the amount of clustering at a given dose and LET, but also the kinetics of DNA damage repair, we introduced a novel mathematical formalism to evaluate the number of remaining RIF over time. We showed that the newly introduced kinetic metrics can be used as surrogate biomarkers for in vivo radiation toxicity, with potential applications in radiotherapy and human space exploration. In particular, we observed an association between the repairable fraction of RIF measured in vitro and survival levels of immune cells collected from irradiated mice. Moreover, the speed of DNA damage repair correlated with spontaneous cancer incidence data collected from the Mouse Tumor Biology database, suggesting a relationship between the efficiency of DSB repair after irradiation and cancer risk. In addition to the efficacy of repair and persistent RIF levels, even the amount of spontaneous foci without irradiation was shown to be strain dependent, indicating that these phenotypes are at least partially driven by genetics, and supporting their potential as indicators of individual radiation sensitivity. [1] Neumaier, T., et al., PNAS, 2012 (8) 109:443

Radiation, DNA damage, repair kinetics↗

Organic chemistry in Titan's atmosphere

Laboratory photochemical simulations and other types of chemical simulations are discussed. The chemistry of methane, which is the major known constituent of Titan's atmosphere was examined with stress on what can be learned from photochemistry and particle irradiation. The composition of dust that comprises the haze layer was determined. Isotope fractionation in planetary atmospheres is also discussed.

Scattergood, T.↗

Proportional retention of I and radiogenic Xe-129 in preheated Allende

In order to study the effects of heat loss and redistribution of iodine and xenon on the I-Xe age, the iodine-xenon dating technique was applied to a bulk sample of the Allende chondrite and a similar sample preheated to 900 C prior to the irradiation. Little iodine or Xe-129 were lost from the high-temperature fractions of the preheated sample, and the high-temperature isochron was fully preserved. The amounts of I and radiogenic Xe-129 retained by the preheated sample were nearly proportional in those temperature fractions (900-1150 C) where most I and radiogenic X-129 were lost. However, the intermediate-temperature isochron was modified, resulting in an apparent isochron which would predate the high-temperature isochron by 6.7 + or - 1.1 m.y.

Rison, W.↗

Characteristics of Mineralogy and Space Weathering Observed on the Grains in the Fine Fraction Samples Returned From the C-type Asteroid Ryugu.

Samples returned from near-Earth C-type asteroid Ryugu by the JAXA Hayabusa2 spacecraft have been investigated from June, 2021. Our Min-Pet Fine ("sand") sub-team have investigated mineralogy and petrology and space weathering of grains in the fine fraction of the samples. Space weathering is alteration induced mainly by solar wind irradiation and micrometeoroid impact. Here, we report mineralogy and microstructural and chemical features related to space weathering of Ryugu grains.

Takaaki Noguchi↗

Mineralogy and space weathering found in the fine-grained samples returned from the C-type asteroid Ryugu

The JAXA Hayabusa2 spacecraft returned samples from near-Earth C-type asteroid Ryugu. Our Hayabusa2-initial-analysisMin-Pet Fine (“Sand”) team has investigated mineralogy and petrology and space weathering of grains in the fine-grained fraction of the samples. Space weathering is alteration induced mainly by solar wind irradiation and micrometeoroid impact. Here, we report the mineralogy, microstructural, and chemical features related to space weathering of the Ryugu grains.

Takaaki Noguchi↗

The influence of cloud cover on the reliability of satellite-based solar resource data

Satellite-based solar resource data are often developed and validated by using binary cloudiness categories: clear sky or overcast cloudy sky. To investigate the reliability of solar resource data in partially cloudy conditions, we estimate cloud fraction using two distinct algorithms: a physical retrieval model using surface observed global horizontal irradiance (GHI) and direct normal irradiance (DNI) and a temporal average of cloud mask data estimated by the observed DNI. Our analysis reveals a significant presence of scattered clouds, broken clouds, and mismatches between satellite- and surface-based cloud data at 17 surface sites across the contiguous United States, though confidently clear and cloudy conditions collectively account for more than 70 % of the data. Solar radiation is computed using the National Solar Radiation Database (NSRDB) algorithm and validated using surface observations. Here, our findings suggest that, in the presence of scattered clouds, NSRDB data for clear-sky conditions can be subject to significant overestimation. In cloudy-sky conditions classified by satellite data, DNI computed by the Fast All-sky Radiation Model for Solar applications with DNI (FARMS-DNI) can be underestimated when limited clouds are detected by surface observations. The bias observed in several cloudiness categories indicates that the NSRDB is exceptionally accurate in confidently clear conditions. However, clear-sky conditions with scattered clouds and mismatched cloud data contribute significantly to the overall uncertainties in the NSRDB. Therefore, future improvements in solar resource data should involve development and implementation of satellite-derived cloud fraction and should consider a novel radiative transfer model accounting for amplified cloud reflection. The evaluation within cloudiness categories also provides a physical rationale for the superior performance of FARMS-DNI compared to the Direct Insolation Simulation Code (DISC) in both cloudy-sky and all-sky conditions.

14 SOLAR ENERGY↗

Surface Irradiances of Edition 4.0 Clouds and the Earth's Radiant Energy System (CERES) Energy Balanced and Filled (EBAF) Data Product

The algorithm to produce the Clouds and the Earth’s Radiant Energy System (CERES) Edition 4.0 (Ed4) Energy Balanced and Filled (EBAF)-surface data product is explained. The algorithm forces computed topof- atmosphere (TOA) irradiances to match with Ed4 EBAF-TOA irradiances by adjusting surface, cloud, and atmospheric properties. Surface irradiances are subsequently adjusted using radiative kernels. The adjustment process is composed of two parts: bias correction and Lagrange multiplier. The bias in temperature and specific humidity between 200 and 500 hPa used for the irradiance computation is corrected based on observations by Atmospheric Infrared Sounder (AIRS). Similarly, the bias in the cloud fraction is corrected based on observations by Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) and CloudSat. Remaining errors in surface, cloud, and atmospheric properties are corrected in the Lagrange multiplier process. Ed4 global annual mean (January 2005 through December 2014) surface net shortwave (SW) and longwave (LW) irradiances increase by 1.3Wm22 and decrease by 0.2Wm22, respectively, compared to EBAF Edition 2.8 (Ed2.8) counterparts (the previous version), resulting in an increase in net SW 1LWsurface irradiance of 1.1Wm22. The uncertainty in surface irradiances over ocean, land, and polar regions at various spatial scales are estimated. The uncertainties in all-sky global annual mean upward and downward shortwave irradiance are 3 and 4Wm22, respectively, and the uncertainties in upward and downward longwave irradiance are 3 and 6Wm22, respectively. With an assumption of all errors being independent, the uncertainty in the global annual mean surface LW 1 SW net irradiance is 8Wm22.

Kato, Seiji↗

Characterisation of nano-scale precipitates in BOR60 irradiated T91 steel using atom probe tomography

Atom probe tomography has characterised the microstructural changes in T91 steel after BOR60 reactor irradiation at five temperatures between 376 °C and 524 °C to doses between 14.6 dpa and 35.1 dpa. Irradiation-induced precipitation and segregation to carbide/matrix interface induced by neutron irradiation has been characterised. Atom probe tomography characterisation shows that Mn, Ni, Si -rich (MNS-rich) clusters form in T91 steel irradiated in BOR60 reactor at temperatures between 376 °C and 415 °C, which is not observed at higher temperatures 460 °C and 524 °C. Additionally, the number density, volume fraction and composition of MNS-rich clusters have been characterised. Ni, Mn, Si and P is found to segregate at carbide matrix interface after irradiation at lower temperature and only P segregation is observed at 524 °C.

36 MATERIALS SCIENCE↗