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At least 199 records · Page 11

ISOCS-based Extended In Situ Gamma Spectrometry Services Tool SuperISOCS for Waste Measurements - 20275

Canberra's In Situ Object Counting System (ISOCS) is an established tool used for gamma spectrometry. It allows physical representation of complex geometries and mathematical calculation of the calibration function while avoiding the need for radioisotope standards. ISOCS provides a large range of templates to generate the geometry for most nuclear waste components in nuclear facilities. Nonetheless, there are some complex geometries where the accuracy attainable is limited by the conventional ISOCS templates. An ISOCS-based extended in-situ Gamma Spectrometry service tool has been developed, based on the so-called SuperISOCS (SISOCS) software. This tool was developed to generate the most complex geometries. The principle of geometry construction is based on the composition of 8 different primitive geometries. The primitive object is able to be cut and to change a part of an object. An object is able to overlap to another one to form a more complex object. These functions refine the modelled geometry compared to the real objects and decrease the measurement systematic error because they allow the mathematical model to represent the real-life geometry more faithfully through reducing the approximations and simplifications that need to be made The algorithm of SISOCS is the same as that of standard ISOCS. A set of calculations was done in comparison with MCNP efficiency calculation and SISOCS results. 80 different models were compared between SISOCS and MCNP, with added 30 cases compared between ISOCS and SISOCS. The average differences were less than 2%, for all energy's efficiency calculations. In this paper we illustrate the benefits that this new tool can provide, in terms of improved accuracy for complex realistic geometries, through simulation of some example scenarios. Furthermore, we demonstrate, through SISOCS modelling of the real object data test, the comparison between SISOCS to ISOCS calculations for the same geometry. This paper describes the added functions that are easily employed using SISOCS. Our results show the potential application and benefit of this technique for real waste assay projects and the way to integrate the tool into the waste assay systems. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Revival and Technology Transfer of 90SrTiO3 Production for Heat Source Applications

Demand for radioisotope power systems (RPS) appears to be on the rise, and it is unlikely that this new demand can be met by plutonium-238. As a result, new heat source designs are under development. One such design is Z1. Z1 is a strontium-90 demonstration heat source developed by Zeno Power Systems in collaboration with the University of Dayton Research Institute and the Pacific Northwest National Laboratory. SrTiO3 was chosen as the fuel form for Z1. SrTiO3 was used to produce dozens of terrestrial RPS decades ago. While this indicates the technology is proven, the skill and experience necessary to effectively produce SrTiO3 has been lost. Recapturing SrTiO3 production technology therefore became necessary. Development started with non-radioactive surrogate experiments using natural strontium. This work showed that the old Oak Ridge flowsheets for SrTiO3 production are quite robust, but some critical pieces of the technology are left out of the old documentation. Specifically, particle sizes of the reagents are critical to producing a phase pure SrTiO3. If the reagent particles are not the right size, then a significant Sr3Ti2O7 phase impurity is observed. This phase impurity was proven to be the result of an incomplete reaction between the strontium and titanium precursors. This technology was transferred to Pacific Northwest National Laboratory where the technology was adapted for use in a hot cell. With the adaptations complete, this technology was used to produce the fuel for Z1 late last year. This represents the first new heat source design produced in the U.S. in over 40 years.

90Sr, strontium titanate, SrTi03, RTG, Radioisotop↗

GPHS-RTG F5R Electrically Heated Thermal Vacuum Testing

Idaho National Laboratory (INL) has been tasked with the evaluation and refurbishment of the General Purpose Heat Source (GPHS) Radioisotope Thermoelectric Generator (RTG) Flight Unit 5 (GPHS-RTG F5R or F5R) that was defueled in 2005. This paper describes the testing of F5R in the thermal vacuum chamber and evaluation of the data demonstrating the generator meets updated Cassini-Huygens requirements. The generator produced 260 We of power at the specified 4100 Wth heat source inventory. This power exceeded the power requirement for 250 We , confirming system integrity and demonstrating that the generator is capable of potential NASA missions.

30 - DIRECT ENERGY CONVERSION↗

f‐ block MOFs: A Pathway to Heterometallic Transuranics

Abstract A novel series of heterometallic f ‐block‐frameworks including the first examples of transuranic heterometallic 238 U/ 239 Pu‐metal–organic frameworks (MOFs) and a novel monometallic 239 Pu‐analog are reported. In combination with theoretical calculations, we probed the kinetics and thermodynamics of heterometallic actinide(An)‐MOF formation and reported the first value of a U‐to‐Th transmetallation rate. We concluded that formation of uranyl species could be a driving force for solid‐state metathesis. Density of states near the Fermi edge, enthalpy of formation, band gap, proton affinity, and thermal/chemical stability were probed as a function of metal ratios. Furthermore, we achieved 97 % of the theoretical maximum capacity for An‐integration. These studies shed light on fundamental aspects of actinide chemistry and also foreshadow avenues for the development of emerging classes of An‐containing materials, including radioisotope thermoelectric generators or metalloradiopharmaceuticals.

Park, Kyoung Chul↗

f‐ block MOFs: A Pathway to Heterometallic Transuranics

Abstract A novel series of heterometallic f ‐block‐frameworks including the first examples of transuranic heterometallic 238 U/ 239 Pu‐metal–organic frameworks (MOFs) and a novel monometallic 239 Pu‐analog are reported. In combination with theoretical calculations, we probed the kinetics and thermodynamics of heterometallic actinide(An)‐MOF formation and reported the first value of a U‐to‐Th transmetallation rate. We concluded that formation of uranyl species could be a driving force for solid‐state metathesis. Density of states near the Fermi edge, enthalpy of formation, band gap, proton affinity, and thermal/chemical stability were probed as a function of metal ratios. Furthermore, we achieved 97 % of the theoretical maximum capacity for An‐integration. These studies shed light on fundamental aspects of actinide chemistry and also foreshadow avenues for the development of emerging classes of An‐containing materials, including radioisotope thermoelectric generators or metalloradiopharmaceuticals.

Park, Kyoung Chul↗

The United States Department of Energy and National Institutes of Health Collaboration: Medical Care Advances via Discovery in Physical Sciences

Over several months, representatives from the U.S. Department of Energy (DOE) Office of Science and National Institutes of Health (NIH) had a number of meetings that lead to the conclusion that innovations in the Nation's health care could be realized by more directed interactions between NIH and DOE. It became clear that the expertise amassed and instrumentation advances developed at the DOE physical science laboratories to enable cutting-edge research in particle physics could also feed innovation in medical healthcare. To meet their scientific mission, the DOE laboratories created advances in such technologies as particle beam generation, radioisotope production, high-energy particle detection and imaging, superconducting particle accelerators, superconducting magnets, cryogenics, high-speed electronics, artificial intelligence, and big data. To move forward, NIH and DOE initiated the process of convening a joint work- shop which occurred on July 12th and 13th, 2021. Here, this Special Report presents a summary of the findings of the collaborative workshop and introduces the goals of the next one.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Understanding long-term groundwater flow at Pahute Mesa and vicinity, Nevada National Security Site, USA, from naturally occurring geochemical and isotopic tracers

Abstract Recently collected naturally occurring geochemical and isotopic groundwater tracers were combined with historic data from the Pahute Mesa area of the Nevada National Security Site (NNSS), Nevada, USA, to provide insights into long-term regional groundwater flow patterns, mixing and recharge. Pahute Mesa was the site of 85 nuclear detonations between 1965 and 1992, many of them deeply buried devices that introduced radionuclides directly into groundwater. The dataset examined included major ions and field measurements, stable isotopes of hydrogen (δ 2 H), oxygen (δ 18 O), carbon (δ 13 C) and sulfur (δ 34 S), and radioisotopes of carbon ( 14 C) and chloride ( 36 Cl). Analysis of the patterns of groundwater 14 C data and the δ 2 H and δ 18 O signatures indicates that groundwater recharge is predominantly of Pleistocene age, except for a few localized areas near major ephemeral drainages. Steep gradients in sulfate (SO 4 ) and chloride (Cl) define a region near the western edge of the NNSS where high-concentration groundwater flowing south from north of the NNSS merges with dilute groundwater flowing west from eastern Pahute Mesa in a mixing zone that coincides with a groundwater trough associated with major faults. The 36 Cl/Cl and δ 34 S data suggest that the source of the high Cl and SO 4 in the groundwater was a now-dry, pluvial-age playa lake north of the NNSS. Patterns of groundwater flow indicated by the combined data sets show that groundwater is flowing around the northwest margin of the now extinct Timber Mountain Caldera Complex toward regional discharge areas in Oasis Valley.

58 GEOSCIENCES↗

Column separation of tetravalent cerium fission products from trivalent rare earth radio-isotopes

Rapid and efficient isolation of individual rare earth element (REE) radioisotopes from complex mixtures is necessary to support the fields of nuclear forensics, medical isotope production and nuclear physics measurements. The separations must be robust and generate sufficiently high purity samples for subsequent radiological analysis. Current methodologies utilize a laborious two step Ce(IV)-iodate precipitation followed by Ce(IV)-nitrate di-(2-ethylhexyl)phosphoric acid/n-heptane extraction. This work reports an alternative method to isolate Ce fission product isotopes equilibrated with milligrams of cold carrier, from the remaining REE’s using a Ce(IV)/LN-resin (Eichrom Technologies) based separation. Optimization of Ce(IV) loading, REE(III) elution volume and subsequent Ce(III) stripping step utilized 166m Ho tracer. Mixed fission product experiments provided a further test of this LN-resin method, with analysis of purified 141/144 Ce, 147 Nd and 91 Y. Overall, while decontamination factors were lower for the LN-resin method, (vs. the combined precipitation/extraction) the simplicity of the technique and the satisfactory fission product analysis results point to the efficacy of this method.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Synergistic extraction of rare earth elements, actinium, americium, and barium with TTA and Pb resin from acetate buffer solutions

The uptake behavior of 88 Y, 140 Ba, 140 La, 141 Ce, 152 Eu, 228 Ac, and 241 Am was studied with batch uptake, kinetics and column studies in a synergistic extraction system with Pb resin and 2-thenoyltrifuoroacetone in acetate-ethanol solutions. The k' values are very high (>10,000) at near neutral pH (~5 to 6) for all of the radioisotopes studied. The kinetics are reasonably fast for column separations, though the uptake rate is dependent on the concentration of 2-thenoyltrifuoroacetone. Column studies were performed to demonstrate the separation of the trivalent actinides and lanthanides from barium and common fssion products ( 99 Mo, 103 Ru).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Uptake of arsenic and selenium on iron-doped Pb resin

We report the uptake of the radioisotopes 73 As and 75 Se was characterized on Fe 3+ -doped Pb resin (Eichrom Technologies) from pH 1 to 12. There is good uptake of arsenic and selenium over a wide pH range (~ 1 to 10) with a decrease only at high pH (~ 12). Column experiments were performed to demonstrate the separations of these elements from solutions with near neutral pH values (~ 6 to 8) with high yields and high radiopurity. These separations may be relevant for a wide variety of applications especially isotope harvesting research.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Actinium purification from elemental components of stainless steel and aluminum

Radioisotopes of actinium are valuable because of their potential use in the medical industry. Actinium-225 shows promise for treating disease—like cancer—via targeted alpha therapy (TAT), and the longer-lived actinium-227 is the parent of two radionuclides with potential application in TAT radiopharmaceuticals, thorium-227 and radium-223. Continuing progress in the development of these medical applications requires robust and diverse methods for extracting and purifying actinium from a wide range of matrices. Further, to define the strengths and limitations of separation methods commonly employed in actinium processing, we characterized the performance of ion exchange and extraction chromatographic steps for removing contaminants found in stainless steel (chromium, iron, nickel, and silicon) and aluminum from actinium-227. While AG-MP1 anion exchange resin with HCl (aq) successfully removed iron, cation exchanger AG 50W-X8 removed most other contaminants. The most persistent contaminant was aluminum, which was removed using a DGA Normal extraction resin. These results are presented within the context of applying that methodology toward actinium purification strategies.

36 MATERIALS SCIENCE↗

Uncertainty improvement of 22 Na based radioactive tracer dilution for determining total mass of pyroprocessing molten salt systems by 154 Eu removal

To determine the total salt mass of the molten salt systems for pyroprocessing spent nuclear fuels, a 22 Na based radioactive tracer dilution was studied in Idaho National Laboratory in recent years. This 22 Na based RTD technique was deemed feasible, but due to the gamma energy peak of 22 Na coinciding with one of the energy peaks of 154 Eu radioisotope in the molten salt, the uncertainty of the 22 Na radioactivity in the 22 Na-spiked salt samples was quite high. To improve the uncertainty of the 22 Na based RTD technique, we proposed to chemically remove the 154 Eu of the salt samples by DGA resin for gamma spectroscopy. The effectiveness of removing 154 Eu on uncertainty improvement was evaluated. Furthermore, it was found that (1) the 154 Eu fission product effect on the uncertainty and detection limit can be effectively eliminated by chemically removing the 154 Eu during the salt sample preparation and (2) the uncertainty of 22 Na radioactivity in the salt samples for electrorefining was significantly improved from 13% to 2%, showing the potential of practical engineering application of 22 Na based RTD as a safeguards technique for molten salt systems for pyroprocessing spent nuclear fuels.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Impurity Levels in Cerium Oxide Microspheres Prepared by Internal Gelation Sol-Gel Methods

Impurity levels were measured in cerium oxide microspheres fabricated by modified internal gelation sol-gel methods. A combination of glow discharge mass spectrometry, electron impact mass spectrometry, combustion gas analysis and instrumental gas analysis were used to assess a wide range of potential elemental impurities. Low concentrations of carbon, nitrogen, and hydrogen impurities in microspheres showed a dependence on how microspheres were washed. Silicon impurities are believed to derive from silicone oil used during sol-gel processing. Spheres washed by the preferred approach had impurity levels below 100 ppm for all elements tested. For applications such as nuclear fuels, sol-gel methods could meet purity specifications as long as metal nitrate feed solutions of sufficient purity are used and microspheres are washed appropriately. In this study, cerium was used as a surrogate for plutonium-238, which is used in radioisotope power systems as a heat source, to determine whether carbon or other impurities were concentrated during internal gelation processing and remained after heat treatments. Analyses indicated low concentrations of impurities in cerium oxide microspheres after sintering steps that were well below documented limits for plutonium-238 oxide fuels. Modified washing methods, combined with a pressurized water treatment, resulted in sintered cerium oxide sol-gel microspheres with low impurity levels.

cerium oxide, sol-gel, internal gelation, microsph↗

Eddy covariance towers as sentinels of abnormal radioactive material releases

Ensuring accurate detection and attribution of abnormal releases of radioactive material is critical for protecting human health and safety. Most commonly, such detection is accomplished via active monitoring approaches involving the collection of physical samples. Further, this is labor intensive and limits the temporal and spatial resolution of any detected events to a relatively coarse level. As an alternative first step towards passive monitoring, we developed an approach using eddy flux tower data records to identify signals from a known abnormal release and quantify the extent to which that signal also occurs at other times in the data record. Through two case studies, one of which targeted the Fukushima nuclear disaster and the other targeting an abnormal release event at a radioisotope production facility in Fleurus, Belgium, we tested our approach and identified several potential heretofore unidentified abnormal events that were consistent with atmospheric circulation patterns and/or wind direction from known release sites. Because our approach is relatively simple and is resistant to systematic errors in the observational record, it has broad applicability beyond specific constituents and ecosystem types to identify a wide variety of limited-duration anomalies in flux tower data to ensure human health and industrial safety.

54 ENVIRONMENTAL SCIENCES↗

High Flux Isotope Reactor (HFIR)

Oak Ridge National Laboratory’s High Flux Isotope Reactor (HFIR) is the highest-flux reactor-based neutron source in the United States. HFIR’s intense neutron flux and state-of-the-art facilities result in world-class capabilities, including neutron scattering, radioisotope production, materials irradiation, and neutron activation analysis. HFIR’s multimission capabilities are attributed to its versatile high-power-density core design consisting of a series of concentric regions, including a flux trap target region, an inner fuel element, an outer fuel element, a control element region, and a beryllium reflector. The pressurized, light-water-cooled research reactor operates at 85 MW and is fueled by 9.4 kg 235U.

Chandler, David↗

Razorback – A reactor transient analysis code for large rapid reactivity additions in a natural circulation research reactor

Research reactors play an important role in higher education, scientific research, and medical radioisotope production around the world. It is thus important to ensure the safety of facility workers and the public. This work presents a new reactor transient analysis code referred to as Razorback. The code has been developed for the evaluation of large rapid reactivity addition in research reactors. Its initial focus is the Annular Core Research Reactor (ACRR) at Sandia National Laboratories. Results have been validated against ACRR pulse operations. Razorback models the reactor kinetics, fuel element heat transfer, fuel element thermal expansion, and natural circulation coolant channel thermal-hydraulic response. Simulation results for ACRR pulse operations are shown to agree very well with operational data obtained from the ACRR. Finally, Razorback is expected to be a valuable tool for ACRR pulse performance prediction and ACRR reactor safety analyses.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Californium-252 production at the High Flux Isotope Reactor - II: Comparison between the highly enriched uranium and a proposed low-enriched uranium core

This is the second paper on a 252 Cf production study performed in support of efforts to convert the High Flux Isotope Reactor (HFIR) from highly enriched uranium (HEU) to low-enriched uranium (LEU) fuel. The first paper primarily focuses on validating computational tools and nuclear data. This companion paper evaluates another critical aspect: the 252 Cf production capability with a proposed LEU core. HFIR must maintain its world-class performance and missions following conversion and because 252 Cf is a vital, multipurpose neutron-emitting radioisotope, the ability to efficiently produce 252 Cf must be preserved. In this study, the HFIRCON transport and depletion tool, several nuclear data libraries, and Campaign 78 data were used to compute 252 Cf production, sensitivity, and safety metrics. Further, results indicate the 252 Cf production and production rates are slightly higher with a 95MW th LEU core compared with those obtained with the 85MW th HEU core. Additionally, the target peak fission rate densities, discharge cumulative fission densities, and heat deposition rates with the LEU core are within a few percent of those calculated with the HEU core. The findings suggest HFIR’s 252 Cf production capability can be effectively maintained with an LEU core without adversely affecting the safety metrics.

07 ISOTOPE AND RADIATION SOURCES↗

Californium-252 production at the High Flux Isotope Reactor - I: Validation study using campaign data

This paper presents a series of 252 Cf production validation and code-to-code comparison studies performed based on data from the production campaigns at the High Flux Isotope Reactor (HFIR). These studies support efforts to convert HFIR from using highly enriched uranium (HEU) fuel to low-enriched uranium (LEU) fuel. HFIR must maintain its world-class performance and missions following this conversion, and because 252 Cf is a vital neutron-emitting radioisotope used for a variety of high-impact applications (e.g., reactor startup, cancer treatment), the ability to efficiently produce 252 Cf must be preserved. In this work, the HFIRCON, Shift, ORIGEN, and TCOMP codes were deployed, and several sets of data libraries were investigated to better understand the calculation codes and the data biases. As-loaded target composition data, as-run irradiation history data, and post-irradiation measurements from recent multi-cycle irradiation campaigns of the HEU core were used to validate and determine methodology biases. Further, the findings demonstrated a good agreement, with results falling within 3 standard deviations of measurements. This paper lays the ground work for the second paper, which evaluates and compares 252 Cf production and safety metrics with the HEU core and a proposed LEU core.

07 ISOTOPE AND RADIATION SOURCES↗