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At least 253 records · Page 14

National‐Scale Assessment of Total Gaseous Mercury Isotopes Across the United States

Abstract With the 2011 promulgation of the Mercury and Air Toxics Standards by the U.S. Environmental Protection Agency, and the successful negotiation by the United Nations Environment Program of the Minamata Convention, emissions of mercury (Hg) have declined in the United States. While the declines in atmospheric Hg concentrations in North America are encouraging, linking the declines to changing domestic and global source portfolios remains challenging. To address these research gaps, the U.S. Geological Survey initiated the first national‐scale effort to establish a baseline of total gaseous mercury stable isotope values at 31 sites distributed across the United States. Results indicated that unique Hg sources, such as Hg evasion from an elemental Hg contaminated site or free tropospheric intrusions in high altitude sites, were distinguishable from background atmospheric values. Minor gradients were observed across the nation, with regions of heavy industrial activity demonstrating lower δ 202 Hg, but no consistent changes in other isotopes such as Δ 199 Hg and Δ 200 Hg were observed. Furthermore, δ 202 Hg was impacted by foliar uptake and senescence but trends varied between forested regions in the northeastern and midwestern United States. These data demonstrate regional emission sources and other environmental variables can impact total gaseous Hg (TGM) isotope values, highlighting the need to characterize atmospheric Hg isotopes over larger geographical areas to evaluate changes related to national and international Hg regulations.

Tate, Michael T.↗

Extraction technique for the determination of oxygen-18 in water using preevacuated glass vials

The need for a rapid, inexpensive technique for routine 18O/16O extraction from water has arisen recently through applications in the medical sciences and in hydrology. The traditional experimental technique for determining the oxygen isotope composition of water, the CO2-H2O equilibration method, is tedious, time consuming, and involves the use of custom-made glass apparatus. Furthermore, because of potential memory effects from one sample to the next, the glassware needs to be thoroughly cleaned between runs. A few attempts have been made to improve upon the method. Attempts to analyze water directly in the source of the mass spectrometer produced large memory effects and questionable results. Commercially available apparatus for automated extraction of 18O/16O from water is generally prohibitively expensive and often is designed to interface only with the manufacturer's own mass spectrometer. The method described in this paper utilizes inexpensive, off-the-shelf, preevacuated, glass vials. Preevacuated vials have been used by others for the isotopic analysis of breath CO2 and are well tested. The vials can be purchased in bulk from scientific apparatus suppliers at a relatively low cost. These are coupled with a simplified extraction line consisting of a stainless steel syringe needle and a glass cold trap. Vials are filled with CO2 and H2O and shaken in a constant-temperature water bath for at least 90 min. Since the vials are discarded after use, no cleaning is necessary, essentially eliminating any memory effect. Reproducibility is generally better than +/- 0.05%. The only reagents required are gaseous CO2 for equilibration, a dry ice/alcohol mixture for trapping water, and liquid nitrogen for transferring the CO2.

NASA Discipline Number 52-10↗

Developing a Facility NMAC Plan

The table presented below suggests the basic information that should be covered in a facility NMAC Plan for an NMAC program that is designed for nuclear security. The topics are appropriate for and should be addressed by all facilities in their NMAC Plans. They are appropriate for NMAC Plans for nuclear power plants, research reactors, fuel manufacturing facilities, facilities that produce medical isotopes, and other facilities. The difference is in the intensity with which the various measures are applied and the thoroughness of the description of the application (i.e., the program requirements). The robustness of a facility NMAC program and the content of its NMAC Plan should be graded in accordance with the type of facility and the category of its nuclear material.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Post-irradiation Examination of Eurofer-97 Steel Irradiated to 20 dpa at 200–400°C in HFIR under the EUROfusion (ORNL-KIT) Collaboration Program

The Oak Ridge National Laboratory/Karlsruhe Institute of Technology (ORNL/KIT) collaboration focuses on research involving irradiation experiments and post-irradiation examinations (PIE) of isotopically modified Eurofer-97 steels for fusion reactor applications. This collaboration capitalizes on ORNL’s expertise in radiation effects on materials and its capabilities in irradiation and PIE. The research aims to qualify Fe-9Cr-based Eurofer-97 steel under simulated fusion conditions, which include high doses and high transmutation rates. A unique isotopic modification technique is utilized in the research, wherein high-transmutation isotopes such as Fe-54 and Ni-58 are alloyed into the Eurofer steel to align with the expected helium production rates in fusion reactor conditions. This report presents the results of post-irradiation mechanical testing activities for the EUROFER-97/2 specimens after irradiation to ~20 dpa at various irradiation temperatures. The irradiation doses and temperatures for the ES capsules ranged from 18.4–20.4 dpa and 202–256°C, respectively. The mechanical property datasets, obtained through baseline testing and PIE of the tensile and fracture specimens, include microhardness data from 93 irradiated and non-irradiated tensile specimens and 28 irradiated bend bar specimens, uniaxial tensile property data from 45 irradiated and non-irradiated tensile specimens, and fracture toughness data from the bend bar specimens. Further data analyses provide statistical information on the microhardness values and tensile properties, as well as the reference ductile-brittle transition temperature (T 0 ) data.

36 MATERIALS SCIENCE↗

Proceedings for the Workshop on Applied Nuclear Data Activities 2024

The Workshop for Applied Nuclear Data Activities (WANDA) is designed to increase communication among nuclear data (ND) users in multidisciplinary federal programs, ND producers, ND funders, and other ND experts. It also presents an opportunity to cross-pollinate ideas as well as introduce ND gaps identified by federal programs to ND experts and ND capabilities to the various federal ND users. WANDA 2024 included five technical sessions, three of which focused on Fusion Energy Sciences (FES)—FES Fusion Neutronics, FES Tritium Production, and FES Material Damage—and two stand-alone sessions—Isotopes and Targetry for Nuclear Data and Uncertainty Quantification. The FES sessions successfully brought new voices to the WANDA discussions, expanding the application space in which nuclear data are critical. FES programs need accurate nuclear data with realistic uncertainty quantification to properly estimate, for example, shielding, activation, tritium production, helium production, structural material integrity, and superconducting magnet operation. This includes a variety of projectile (neutrons, photons, charged particles) and target atoms. One of the action items common to all the FES sessions was a need to perform sensitivity studies to identify the prioritization of nuclear data needs. The Isotopes and Targetry session highlighted the many capabilities available to produce high-quality targets for nuclear data measurements, including 3D printing with spherical powders, combustion synthesis coupled with spin coating & electrospraying, inkjet printing, and isotopic doping. These new methods open doors for more accurate measurement, but it was also stressed that sample characterization following any method of fabrication is of the highest importance to accurately interpret nuclear data measurement results that used that sample. The Uncertainty Quantification (UQ) session was broken into two categories: nuclear data uncertainty quantification and the use of that uncertainty quantification. Thematic to the UQ session was the loss of information when going from nuclear data measurement, to evaluation, to evaluated file, and finally to neutron transport calculations. Current evaluated ND libraries typically only contain covariances, which assume that the probability distributions are Gaussian. Beyond being a simplified assumption for many evaluations, this can lead to negative values on many observables when attempting to sample the covariance. The covariance format, however, is very efficient in that a simple set of linear equations can transform uncertainty from parameters or cross sections to the application of interest. Focused collaboration is needed between nuclear data evaluators and nuclear data users to ensure that needs are being met.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Understanding the effect of specimen size on the properties of fine-grain isotropic nuclear graphite for irradiation studies: Mechanical properties

Programs at Oak Ridge National Laboratory are investigating the effects of neutron irradiation in the High Flux Isotope Reactor (HFIR) on properties of fine-grain isotropic nuclear graphites. Specimens were irradiated in the HFIR flux trap, which requires using specimens that are smaller than the sizes recommended by ASTM standards. Here, this work has investigated whether subsized specimens can be used to reliably predict strength behavior. The results show that (1) tensile strength was loosely coupled to specimen volume, (2) the compression specimens had a slightly higher strength for larger volumes, (3) the uniaxial flexural strength was nearly independent of specimen effective area for one orientation whereas the other orientation showed a slight strength–size scaling Weibull behavior, and (4) equibiaxial flexural strength followed traditional strength–size scaling Weibull behavior. These results suggest that fine-grain graphite is more similar to ceramics than to medium- and large-grained graphite with respect to both the strength-limiting flaws (Griffith theory) and the effect of machining on the strength behavior. This work shows that using specimens that are smaller than ASTM recommendations are suitable for investigating the strength changes caused by neutron irradiation because the primary interest is the relative change in the strength distribution parameters rather than their absolute values.

36 MATERIALS SCIENCE↗

Understanding the effect of specimen size on the properties of fine-grain isotropic nuclear graphite for irradiation studies: Physical, electrical, thermal properties

Programs at Oak Ridge National Laboratory are investigating the effects of neutron irradiation in the High Flux Isotope Reactor (HFIR) on properties of fine-grain nuclear graphites. Specimens were irradiated in the HFIR flux trap, which required using specimens that are smaller than the sizes recommended by ASTM standards. Here, this work has investigated whether subsized specimens can be used to reliably determine the measured physical (density, elastic moduli, and electrical resistivity) and thermal properties (coefficient of thermal conductivity and thermal conductivity). The results show the specimen sizes in this investigation had a minimal influence on any of the measured properties. Even for the properties where size influenced the measured value (density and thermal conductivity), an explanation is provided, and the consequences can be accounted for in post-irradiation results. This work demonstrated that using subsized specimens for physical and thermal property measurements is suitable when necessary for fine-grain isotropic graphite.

36 MATERIALS SCIENCE↗

Baseline Hypothetical Facility for the Production of 131 I and 99 Mo using Activation Targets

This report describes a hypothetical facility for production of medical radioisotopes via activation under the Proliferation Resistance and Optimization (PRO-X) program. The facility uses neutron activation of non-special nuclear material (SNM) to produce the medical isotopes 131 I and 99 Mo at a throughput of 60 Ci/week of 131 I and 5 Ci/week of 99 Mo. The hypothetical design was carried out using a 10 MWt research reactor. The precursors used for the activation process were TeO2 for 131 I and MoO 3 for 99 Mo. The processes are performed in 3 hot cells used for target receipt, extraction, purification low specific activity (LSA) generator introduction, and packaging. A fourth hotcell is used for waste processing. The hot cell processing area takes up a footprint of 15.4 m 2 with the total footprint of the facility, including space for administrative offices, non-rad labs, quality assurance, and radiation buffer areas set at 763 m 2 . Waste is produced at a weekly rate of 257.8 g low activity solid waste and 8032.7 mL of low activity liquid waste, 8032 mL of which is water. This baseline hypothetical facility for production of medical isotopes via activation was then compared and contrasted to the hypothetical facility for production of medical isotopes via fission products to show the differences in approach for the two production modes. The two production modes had several highlighted differences including the overall facility and hot cell layout, the type and amount of waste produced by the respective facilities, and economic factors impacting production mode. Finally, a decision tree for which production mode might be more beneficial for an entrant into medical isotope production was developed based on the differences examined and the desired output of medical isotopes desired by the entrant.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Measurement of isotopic separation of argon with the prototype of the cryogenic distillation plant Aria for dark matter searches

The Aria cryogenic distillation plant, located in Sardinia, Italy, is a key component of the DarkSide-20k experimental program for WIMP dark matter searches at the INFN Laboratori Nazionali del Gran Sasso, Italy. Aria is designed to purify the argon, extracted from underground wells in Colorado, USA, and used as the DarkSide-20k target material, to detector-grade quality. In this paper, we report the first measurement of argon isotopic separation by distillation with the 26 m tall Aria prototype. We discuss the measurement of the operating parameters of the column and the observation of the simultaneous separation of the three stable argon isotopes: ${}^{36}\hbox {Ar}$, ${}^{38}\textrm{Ar}$, and ${}^{40}\textrm{Ar}$. We also provide a detailed comparison of the experimental results with commercial process simulation software. This measurement of isotopic separation of argon is a significant achievement for the project, building on the success of the initial demonstration of isotopic separation of nitrogen using the same equipment in 2019.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

140,142 Cerium Resolved Resonance Region Evaluation [Slides]

The presentation covers an overview of 140,142 Ce Isotopes, including new evaluations of 140,142 Ce that were requested by the Hanford Plutonium Finishing plant to the Nuclear Criticality Safety Program. It also discusses current ENDF/B-VIII.0 evaluation, which has an error in the 1-2 keV range. It was evaluated using multi-level Breit-Wigner and 142Ce has room for extending resolved resonance region current upper limit from 13 keV. The presentation also discusses new transmission and capture measurements of nat Ce and 142 Ce from Klaus Guber. It also states that no known integral experiments prominently feature Cerium.

07 ISOTOPE AND RADIATION SOURCES↗

Delayed Critical and Subcritical Experiments with Polyethylene Moderated Unreflected Thin 15 in. Diameter HEU Metal Plates

The thin ~15 in. diameter highly enriched uranium (HEU) metal plates were assembled to delayed criticality at the Oak Ridge Critical Experiments Facility (ORCEF) in 1969 with various thicknesses of polyethylene (varying from 1/16 to 2$\frac{3}{8}$ inches) between uranium metal plates. The average 235 U enrichment was 93.27 wt. %. These unreflected critical configurations contained 4$\frac{2}{3}$ to 20$\frac{5}{6}$ thin 15 in. diameter HEU metal plates (on loan from Los Alamos National Laboratory [LANL] and shipped to Oak Ridge National Laboratory [ORNL] on June 3, 1969). Depending on the thickness of polyethylene, the enriched uranium masses varying from 28,053 to 135,148 grams. Fractional plate sections consisted of the appropriate number of 60° pie sections. In addition to the measurement at delayed criticality, subcritical measurements were also performed by the inverse kinetic rod drop method. Prompt neutron decay constant measurements were also performed by the Rossi alpha and randomly pulsed neutron method using a time-tagged spontaneous fission californium neutron source; these are briefly reported here. At the time of these measurements in 1969, the thin HEU metal plates were in near-pristine condition with extremely little oxidation, allowing better descriptions of the uranium plates than the use of these plates in a heavily oxidized and deteriorated condition in recent reflected benchmark experiments at the LANL facility at the Nevada Test Site with these same thin highly enriched uranium metal plates. This report documents the experimental information for the measurements performed so that later researchers can perform the required uncertainty and calculational analyses and documentation to use these data for an International Nuclear Criticality Safety Benchmark Evaluation Program (ICSBEP) or a Nuclear Energy Agency (NEA) benchmark. Data from the experiments described should be acceptable for use as criticality safety benchmark experiments for the ICSBEP and the NEA nuclear criticality safety benchmark program once the uncertainty analysis on the measured neutron multiplication factors is completed. Additional data—such as the dimensional inspection reports, uranium isotopic information, and other relevant particulars—should be retrieved from the Y-12 Plant or LANL and incorporated in the final ICSBEP benchmark. Based on previous ICSBEP benchmarks with this enriched uranium metal at ORCEF, the uncertainties in $k_{eff}$ could be as low as ± 0.0002 for some configurations. Other experiments with smaller-diameter than 15 in. diameter HEU metal plates have been benchmarked in HEU-METFAST-001. The prompt neutron time decay measurements could be the basis for an International Reactor Physics Benchmark Program. Preparation of the present report is part of an effort at ORNL to document more than 15 undocumented critical and subcritical experiments enumerated in ORNL/TM-2019/18 and performed by ORNL at ORCEF and other US Department of Energy critical experiments facilities using more than 500 operational days of critical facility time. This work for this report publication was supported by the Nuclear Criticality, Radiation Transport and Safety NCSP Program at ORNL.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Low-temperature carbonate concretions in the Martian meteorite ALH84001: evidence from stable isotopes and mineralogy

The martian meteorite ALH84001 contains small, disk-shaped concretions of carbonate with concentric chemical and mineralogical zonation. Oxygen isotope compositions of these concretions, measured by ion microprobe, range from delta18O = +9.5 to +20.5 per thousand. Most of the core of one concretion is homogeneous (16.7 +/- 1.2 per thousand) and over 5 per thousand higher in delta18O than a second concretion. Orthopyroxene that hosts the secondary carbonates is isotopically homogeneous (delta18O = 4.6 +/- 1.2 per thousand). Secondary SiO2 has delta18O = 20.4 per thousand. Carbon isotope ratios measured from the core of one concretion average delta13C = 46 +/- 8 per thousand, consistent with formation on Mars. The isotopic variations and mineral compositions offer no evidence for high temperature (>650 degrees C) carbonate precipitation and suggest non-equilibrium processes at low temperatures (< approximately 300 degrees C).

NASA Center JSC↗

Operation of GRETINA at NSCL

This proposal funded the continued operation of the Gamma-ray Energy tracking Array GRETINA as a user device at the National Superconducting Cyclotron Laboratory (NSCL) at Michigan State University. This was a continuation and covered the operation from January 1, 2017 to December 31, 2017. Twenty-three experiments were completed with GRETINA at NSCL. GRETINA was installed at the reaction target position of the high-resolution, large-acceptance S800 spectrograph and the program started on October 15, 2017. The campaign capitalized on the opportunities provided by NSCL’s energetic rare isotope beams produced by projectile fragmentation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Investigating Similarity Differences for Light-water-Moderated and Polyethylene-Moderated Systems

Oak Ridge National Laboratory has performed validation studies in support of Pacific Northwest National Laboratory’s analysis of the Sum-of-Fractions method. Work in a companion paper examines the validation methods and results for various mixtures of fissile isotopes in various concentrations moderated and reflected by water and polyethylene. Those results indicate a greater coverage of critical experiments for validating water moderated and reflected systems versus those moderated and reflected with polyethylene.

07 ISOTOPE AND RADIATION SOURCES↗

Simulation of Isotopic Concentrations and Gamma Spectra from Dynamic Fission Sources

A tool was developed to rapidly generate synthetic gamma-ray spectra to evaluate safeguards material control and accounting methods for liquid-fueled molten salt reactors. Molten salt reactor operations pose unique challenges to nuclear safeguards methods and protocols compared to deployed reactors designs (e.g., light water reactors). This research evaluates the use of gamma-ray spectroscopy to monitor fission product isotopic flow through a reactor model to understand expected operations and investigate changes to the spectra with material diversion scenarios. The large design space of molten salt reactors (e.g., liquid-fueled, liquid-cooled, online separations) could potentially lead to many measurement points within the reactor system. The developed analytical tool generates and evaluates synthetic gamma-ray spectra from dynamic reactor simulations by extracting isotopic inventory to generate source terms. An implementation in the Gamma Detector Response and Analysis Software (GADRAS) Application Program Interface (API) uses the source terms, a model of the reactor component, a detector response function, and measurement plan to quickly generate and analyze spectra. Prospective measurements are then evaluated in the more accurate but slower Geant4 simulations. Utilization of the developed modeling tool and analysis of the subsequent spectra enables optimization of collimation, shielding requirements, and expected count rates that are used to determine key measurement points in the modeled reactor design.

O'Brien, Sean↗

Transport Modeling of As-Run ATR Cycles to Support U-10Mo Research Reactor Fuel Qualification Experiment

The Department of Energy’s (DOE) Office of Materials Management and Minimization has been tasked with converting the five remaining United States High Performance Research Reactors (U.S. HPRR) from highly enriched uranium to low-enriched uranium. The Nuclear Regulatory Commission (NRC) regulates Massachusetts Institute of Technology Reactor (MITR), Missouri University Research Reactor (MURR), and National Bureau of Standards Reactor (NBSR); and DOE regulates the High Flux Isotope Reactor and Advanced Test Reactor (ATR). To meet the high demands of these reactors, the U.S. HPRR program has chosen to use 90% uranium - 10% molybdenum (U-10Mo) monolithic fuel. This plate-type fuel will undergo multiple irradiation experiment campaigns in ATR, from mini-plates to full element tests, over a large range of operating conditions. This will provide data in support of the fuel qualification of each reactor. This summary focuses on the as-run neutronic analysis of the first series of mini-plate (MP-1) experiments, which have been irradiated in the ATR. MP-1 experiment’s main goal is to demonstrate the fabrication process and meet the fuel irradiation performance requirements with primary focus on the fuel plates associated with the three NRC reactors, with a small focus on the low power requirements of the ATR fuel. The MP-1 experiments are planned to be the basis of the monolithic U-10Mo fuel for qualification through the NRC.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Transport Modeling of As-Run ATR Cycles for U-10Mo Fuel Qualification Experiment

The Department of Energy’s (DOE) Office of Materials Management and Minimization has been tasked with converting the five remaining United States High Performance Research Reactors (U.S. HPRR) from highly enriched uranium to low-enriched uranium. The Nuclear Regulatory Commission (NRC) regulates Massachusetts Institute of Technology Reactor (MITR), Missouri University Research Reactor (MURR), and National Bureau of Standards Reactor (NBSR); and DOE regulates the High Flux Isotope Reactor and Advanced Test Reactor (ATR). To meet the high demands of these reactors, the U.S. HPRR program has chosen to use 90% uranium - 10% molybdenum (U-10Mo) monolithic fuel. This plate-type fuel will undergo multiple irradiation experiment campaigns in ATR, from mini-plates to full element tests, over a large range of operating conditions. This will provide data in support of the fuel qualification of each reactor. This summary focuses on the as-run neutronic analysis of the first series of mini-plate (MP-1) experiments, which have been irradiated in the ATR. MP-1 experiment’s main goal is to demonstrate the fabrication process and meet the fuel irradiation performance requirements with primary focus on the fuel plates associated with the three NRC reactors, with a small focus on the low power requirements of the ATR fuel. The MP-1 experiments are planned to be the basis of the monolithic U-10Mo fuel for qualification through the NRC.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Climatic forcing of carbon-oxygen isotopic covariance in temperate-region marl lakes

Carbon and oxygen stable isotopic compositions of lacustrine carbonate from a southeastern Michigan marl lake display linear covariance over a range of 4.0% Peedee belemnite (PDB) in oxygen and 3.9% (PDB) in carbon. Mechanisms of delta 13 C-delta 18 O coupling conventionally attributed to lake closure in arid-region basins are inapplicable to hydrologically open lake systems. Thus, an alternative explanation of isotopic covariance in temperate region dimictic marl lakes is required. We propose that isotopic covariance is a direct record of change in regional climate. In short-residence-time temperate-region lake basins, summer meteoric precipitation is enriched in 18O relative to winter values, and summer organic productivity enriches epilimnic dissolved inorganic carbon in 13C. Thus, climate change toward longer summers and/or shorter winters could result in greater proportions of warm-month meteoric precipitation, longer durations of warm-month productivity, and net long-term enrichment in carbonate 18O and 13C. Isotopic covariance observed in the Michigan marl lake cores is interpreted to reflect postglacial warming from 10 to 3 ka followed by cooler mean annual temperature, a shift toward greater proportions of seasonal summer precipitation, a shortening of the winter season, or some combination of these three factors.

NASA Discipline Number 52-30↗