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At least 253 records · Page 14

Development of Stirling Convertors for Radioisotope and Fission Power Systems

NASA has been developing free-piston Stirling-cycle power convertors over the past 22 years for use in nuclear power systems that would provide electricity for space science missions to dark, dusty, or distant destinations where solar power is not practical. These nuclear power systems would generate heat from either the radioactive decay of isotopes or fission nuclear reactors. That heat would be converted to usable electricity using highly efficient Stirling convertors for a wide range of power needs needing 10s of watts to 50 kWe. NASA’s Radioisotope Power Systems (RPS) Program is maturing advanced thermoelectric and dynamic conversion technologies that would increase the system efficiency beyond what is currently possible using heritage systems to enable a larger number of robotic missions or higher power missions to solar system bodies of interest. The Dynamic Radioisotope Power Systems (DRPS) Project has matured prototype Stirling convertors to sufficiently increase the technology readiness level for infusion into flight development. Flexure and gas-bearing free-piston Stirling convertors were developed under contract by commercial partners and delivered to enable government evaluation. Gas-bearing designs have met performance and robustness requirements and were selected for flight development. This paper provides the status of SRSC test campaign and maturity level.

Dynamic↗

Sensors for measuring thermal conductivity and related methods

A sensor for measuring thermal conductivity includes an insulator, a test material over the insulator, a conductor over the test material, and a gas within an open volume adjacent the test material and the conductor. An electrical source is configured to provide an alternating current through the conductor to heat the test material. Leads are connected to the conductor and configured to connect to a voltmeter. A method of measuring thermal conductivity includes disposing the sensor in a reactor core in which a nuclear fuel undergoes irradiation and radioactive decay. An alternating current is provided from the electrical source through the conductor to heat the test material. A voltage is measured as a function of time at the leads connected to the conductor. A thermal conductivity of the test material is calculated based on the voltage measured as a function of time. Methods of forming a sensor are also disclosed.

Daw, Joshua↗

Actinide Radiation Chemistry and Used Nuclear Fuel Reprocessing

Although the actinides boast many unique physical and chemical properties, their inherent susceptibility to radioactive decay—and subsequent consequences of radiation-induced chemistry—are what make them truly interesting and challenging elements to understand. From a closed nuclear fuel cycle perspective, the ability to predict and control the effects of actinide-driven radiolysis is critical for the design, development, and deployment of advanced used nuclear fuel reprocessing strategies and technologies. The absorption of ionizing radiation from actinide decay leads to the formation of a variety of transient and steady-state radicals, ions, and molecular radiolysis products that can lead to significant changes in a reprocessing solvent system’s physical and chemical properties, which ultimately limits that process’ efficiency and longevity. Presented here is an overview of recent advances in actinide radiation chemistry as it applied to used nuclear fuel reprocessing.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Impact of Actinide Complexation on Ligand Radiolysis

Although the actinides boast many unique physical and chemical properties, their inherent susceptibility to radioactive decay are what make them truly interesting elements to study. The absorption of ionizing radiation from actinide decay leads to the formation of a variety of transient and steady-state radicals, ions, and molecular radiolysis products that can lead to significant changes in the surrounding environment, and ultimately dictate steady-state actinide redox distributions and the longevity of molecules designed for actinide complexation. Radiolysis of the latter leads to complexant destruction and the concomitant formation of degradation products that can complicate actinide studies and processes. However, the radiation chemistry of most actinide complexants have been studied in the absence of the actinides they were designed to complex, which can lead to inaccurate conclusions on longevity and degradation product distributions, as metal ion complexation has been historically shown to influence a ligand’s radiolytic behavior. Consequently, bridging this knowledge gap is important for actinide science. Here, I will discuss the impact of actinide complexation on the steady-state and time-resolved radiation-induced reactivity of a variety of complexants, including, tributyl phosphate (TBP) and N,N,N',N'-tetraoctyl diglycolamide (TODGA) .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Low Level Calibration of Liquid Scintillation Counting

Liquid Scintillation Counting (LSC) is an analytical laboratory method that quantifies the concentrations of alpha and beta emitting isotopes. The LSC method can be utilized for the detection of tritium, both environmentally and at nuclear facilities. Most LSC samples are aqueous-based and prepared as a radioactive sample dissolved or suspended in a high efficiency scintillation cocktail that converts radioactive energy into light pulses. When placed in counting vials, the liquid scintillation cocktail allows for optical coupling in which energy is released from the samples radioactive decay, and transferred to the scintillator. That energy is then absorbed to produce excited electrons that fall back to their ground-state and emit a pulse of light that is detected by the liquid scintillation analyzers photomultiplier tubes. Quench is a signal attenuation due to physical, chemical, or color interferences. To compensate for quench, quench standards of a known concentration are implemented at increasing increments of quench per vial to create a quench curve. Quench standards can be purchased pre-made or customized from the manufacturer, however, there are several issues that arise from purchasing the pre-made quench standards. The main issues with ordering pre-made quench standards is that they use higher count values, between 30,000 and 250,000 disintegrations per minute (dpm) of tritium per vial and only come in glass vials. Using higher counting standards in glass vials makes it hard to see lower concentrations in plastic vials. Additionally, when using higher energy standards the accuracy of the calibration readings tend to be lower. On the other hand, making a set of quench standards in-house allows for the customization of the dpm concentration to roughly 1,500-3,000 and preparation in plastic vials. This allows for lower activity readings that results in closer precision of the samples' true concentration. Technical Objectives: Create a quench curve and calibrate the LSA for tritium. Verify the calibration of the quench curve prior to cross sample runs. Check calibration against Quality Control (QC) reference value. Conclusion: a tritium quench curve calibration was performed using a scintillation cocktail with ultima gold (AB and AB/F), acetone (only with AB), and water (only with AB/F). By performing the tritium quench curve calibration, the counting efficiency was correlated to various levels of quench. Calibration checks with quality control standards were also performed to verify that the calibration was correct. The observed results provided acceptable values that matched the quality control standard reference values with an acceptable uncertainty. The next step will be fine tuning and cross comparison checks with legacy instrumentation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Assessing Effects of Climate Change on Legacy Waste at the Enewetak Atoll

The Republic of the Marshall Islands (RMI) is in the central Pacific Ocean ~4,500 km west of Hawaii. The Enewetak Atoll, located in the northwest part of the RMI, was the site for 43 nuclear weapon tests between 1948 and 1958. Fallout and deposition from the tests contaminated the island surfaces, lagoon waters and sediment, and nearby ocean waters at the atoll. In the 1970s, a cleanup effort collected radioactive waste and placed it in the Cactus Crater on Runit Island (also called the Runit Dome). In December 2021, Congress directed the U.S. Department of Energy to study the impacts of climate change on the Runit Dome nuclear waste disposal site. Pacific Northwest National Laboratory (PNNL) assembled a multidisciplinary team of climate scientists, ocean modelers, environmental scientists, and health physicists to assess the likely effects of remaining radionuclides at the Enewetak Atoll. PNNL’s approach focused on effects of tropical cyclones that were postulated to mobilize and transport contaminated lagoon sediments and result in human and biota exposure. PNNL’s study estimated (1) the radionuclide source term, (2) the effects of climate change on severe storms, (3) mobilization and transport of radionuclides, and (4) radiation dose to humans and biota. Radionuclides in the lagoon and/or ocean waters of the Enewetak Atoll were characterized by the U.S. Atomic Energy Commission (AEC) in 1972, Woods Hole Oceanographic Institution in 2015, and Lawrence Livermore National Laboratory in 2018. The RMI Nationwide Radiological Study was conducted in the early 1990s for radionuclides remaining in island soils. The 1972 AEC survey remains the most comprehensive source of radionuclide data on lagoon sediments. Climate change modeling at a regional scale in the central Pacific Ocean is limited. PNNL climate scientists simulated severe historical storms postulated to occur both in a recent climate (2015) and in the future (2090) using the Advanced Research Weather Research and Forecasting (WRF-ARW) model, employing a pseudo-global-warming technique. A postulated complete, future failure of the Runit Dome was also considered. PNNL developed a high-resolution regional ocean hydrodynamics model covering the entire RMI extended economic zone using the Finite Volume Coastal Ocean Model (FVCOM). The FVCOM model was run using global reanalysis data for current climate and WRF-ARW simulation for the future climate. PNNL also developed a radionuclide fate and transport model using the FVCOM Integrated Compartment Model (FVCOM-ICM) to simulate the current and future mobilization and transport of radionuclides sorbed to lagoon sediments and the exchange of radionuclides between the water and sediment. FVCOM-ICM-predicted radionuclide concentrations were then used to estimate radiation dose to humans and biota at all islands of the Enewetak Atoll. Under current climate conditions, annual radiation exposures for the southern islands including Enewetak (Fred) and Medren (Elmer) were below the current U.S. standards. Radiation doses were somewhat elevated starting at Runit Island northward and westward to Enjebi Island (Janet). The islands in the northwest quadrant, particularly Bokoluo (Alice) and Bokombako (Belle), remain relatively contaminated. The islands in the southwestern quadrant have low contamination. The highest contribution to radiation doses comes from consumption of locally grown foods. Two radionuclides, 90Sr and 137Cs, contributed the greatest fraction for most terrestrial foods. In current climate conditions, the storms temporarily increased radionuclide concentrations in the lagoon waters, increasing the radiation dose slightly. In future conditions, doses are expected to be smaller, primarily because of the radioactive decay of the shorter-lived radioisotopes of 90Sr and 137Cs. This could make all islands in the far northwest of the atoll – except Bokombako (Belle) and perhaps Bokoluo (Alice) – suitable for residency. For the f

Prasad, Rajiv↗

BISON Simulated and Experimental Fission Product Release Comparisons from Reradiated AGR-3/4 Compacts During High Temperature Heating Tests

The fuel performance modeling code BISON was used to predict the release of fission products iodine-131 (131I), xenon-133 (133Xe), and krypton-85 (85Kr) from four re-irradiated AGR-3/4 fuel compacts containing tristructural isotropic (TRISO) coated particles during high-temperature isothermal heating tests. The AGR-3/4 fuel compacts were irradiated in the Advanced Test Reactor (ATR) as part of the third and fourth series of planned experiments to support the Advanced Gas Reactor (AGR) Program. They were subsequently stored and re-irradiated in the Neutron Radiography (NRAD) reactor for approximately five days and then stored for another five to eight days before being subjected to isothermal heating tests in the Fuel Accident Condition Simulation (FACS furnace) for 200 to 300 hours at temperatures between 1000°C and 1600°C to evaluate fission product release at elevated temperatures. New nuclide-specific fission product source term models for the three nuclides of interest were developed using the reactor multiphysics code Griffin and implemented into BISON to support this work. The new source term models were incorporated into coupled compact- and particle-scale BISON simulations, which predict spatially- and temporally-resolved radionuclide generation, radioactive decay, transport, and release throughout the entire irradiation history, including the initial ATR irradiation, NRAD re-irradiations, FACS heating tests, and intermediate periods spent in storage. The experimentally measured fission product release from the heating tests were compared to modeling release predictions calculated by BISON to evaluate how well the code compares to experimental results. Overall, the experimental measured and BISON predicted comparative release results varied but generally agreed to within 5 particle equivalents. Comparative release results identified general observations to take into consideration to help refine future models and reduce uncertainties associated with both the measurement results and predictive results. This includes developing new uranium oxycarbide (UCO) specific kernel diffusivities for the three isotopes examined to more accurately reflect the material properties of the fuel form. Deriving new diffusivities will aid in producing a more informed BISON model

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Unravelling the radiation-induced redox chemistry of plutonium ions in aqueous solution

Plutonium plays a critical role in nuclear fuel cycle technologies, but our understanding of its fundamental radiation-induced redox chemistry is limited. Changes in oxidation states affect the speciation and transport of plutonium ions in solution. For example, solvent extraction techniques used to separate and recover plutonium from used nuclear fuel rely on the selective formation, maintenance, and complexation of specific plutonium oxidation states. However, radiolytically generated radicals, ions, and molecules can drive the oxidation state distribution of plutonium ions far from equilibrium, ultimately changing the physical and chemical properties of the bulk system. These radiation-induced processes are inevitable due to the ionizing radiation fields generated by the radioactive decay of plutonium and its daughter nuclides. Therefore, mechanistically understanding how plutonium's various oxidation states respond to ionizing radiation is essential for predicting its behavior in solution. Here, we present significant advances in our understanding of radiation-induced plutonium redox chemistry by using time-resolved (electron pulse) and dose accumulation (alpha and gamma) irradiation techniques, along with quantitative multiscale modeling methods.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

AGC-4 As-Run Uncertainty Analysis

The concept of measuring neutron flux (or fluence rate) with activation foils has existed since the late 1940s and is a well-used methodology. Activation foils are selected for their unique isotopic cross sections that create reaction products with desirable properties: relatively simple radioactive decay scheme, measurable quantities of gamma-rays or betas, and half-lives appropriate for the irradiation and decay durations of the experiment. The activation materials, deemed flux wires, fluence wires, dosimeters, or flux foils, are fabricated to have a mass appropriate for the irradiation as well so the measurement using a radiation detector following the irradiation is sufficient but not overwhelming in terms of total activity. Activation measurement results are expressed in terms of reaction rate, which can then be used to “adjust” the neutron spectrum. The Advanced Graphite Creep (AGC)-4 experiment contained 26 flux wire packages, each containing an iron and a niobium wire inside a vanadium capsule. For all stackup positions, the value of fast to thermal neutrons is higher than expected, but the total neutron fluence is near the predicted value of ~2 x 1022 n/cm2. As compared to the predicted neutron spectrum, there are four takeaways in the results as compared to the predicted ATR irradiation: 1) Additional fast (fission) neutrons present, 2) Spectrum hardening due to temperature, 3) Spectrum hardening due to container attenuation, 4) Total neutron fluence is close to predicted values. Since the neutron energy spectrum is a key parameter when attributing neutron damage in materials, the adjusted energy-dependent spectrum and the total neutron fluence results from the dosimeters can be incorporated for future calculations.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The aluminium-26 distribution in a cosmological simulation of a Milky Way-type Galaxy

Context . The 1.8 MeV γ -rays corresponding to the decay of the radioactive isotope 26 Al (with a half-life of 0.72 Myr ) have been observed by the SPI detector on the INTEGRAL spacecraft and extensively used as a tracer of star formation and current nucleosynthetic activity in the Milky Way Galaxy. Further information is encoded in the observation related to the higher 26 Al content found in regions of the Galaxy with the highest line-of-sight (LoS) velocity relative to an observer located in the Solar System. However, this feature remains unexplained. Aims . We ran a cosmological “zoom-in” chemodynamical simulation of a Milky Way-type galaxy, including the production and decays of radioactive nuclei in a fully self-consistent way. We then analyzed the results to follow the evolution of 26 Al throughout the lifetime of the simulated galaxy to provide a new method for interpreting the 26 Al observations. Methods . We included the massive star sources of 26 Al in the Galaxy and its radioactive decay into a state-of-the-art galactic chemical evolution model, coupled with cosmological growth and hydrodynamics. This approach allowed us to follow the spatial and temporal evolution of the 26 Al content in the simulated galaxy. Results . Our results are in agreement with the observations with respect to the fact that gas particles in the simulation with relatively higher 26 Al content also have the highest LoS velocities. On the other hand, gas particles with relatively lower 26 Al content (i.e., not bright enough to be observed) generally display the lowest LoS velocities. However, this result is not conclusive because the overall rotational velocity of our simulated galaxy is higher than that observed for cold CO gas in the Milky Way Galaxy. Furthermore, we found no significant correlation between gas temperature, rotational velocity, and 26 Al content at any given radius. We also found the presence of transient 26 Al-rich spots at low LoS velocities and we show that one such spot had been captured by the INTEGRAL/SPI data. Based on our model, we present a prediction for the detection of 1.8 MeV γ -rays by the future COSI mission. We find that according to our model, the new instrument will be able to observe similar 26 Al-emission patterns to those seen by INTEGRAL/SPI.

Wehmeyer, B. (ORCID:0009000254149292)↗

Controlling T c of iridium films using the proximity effect

A superconducting Transition-Edge Sensor (TES) with low-$T_c$ is essential in a high resolution calorimetric detection. With a motivation of developing sensitive calorimeters for applications in cryogenic neutrinoless double beta decay searches, we have been investigating methods to reduce the $T_c$ of an Ir film down to 20 mK. Utilizing the proximity effect between a superconductor and a normal metal, we found two room temperature fabrication recipes of making Ir-based low-$T_c$ films. In the first approach, an Ir film sandwiched between two Au films, a Au/Ir/Au trilayer, has a tunable $T_c$ in the range of 20-100 mK depending on the relative thicknesses. In the second approach, a paramagnetic Pt thin film is used to create Ir/Pt bilayer with a tunable $T_c$ in the same range. We present detailed study of fabrication and characterization of Ir-based low-$T_c$ films, and compare the experimental results to theoretical models. We show that Ir-based films with predictable and reproducible critical temperature can be consistently fabricated for use in large scale detector applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Quantifying fission yields at the National Ignition Facility using depleted uranium foil experiments

There are programs for high-Z shell experiments at the National Ignition Facility (NIF). For shells made of actinide material, a quantitative fission diagnostic is needed in order to determine how much fission took place and whether the fission was sufficient to produce a non-negligible heat source in the burning capsule. Here, we present a viable coupled experimental and theoretical technique for making quantitative fission measurements possible. The proposed scheme involves using a well-characterized set of depleted uranium foils outside an NIF capsule to verify the conversion of xenon and krypton fission fragments collected at the Radiochemical Analysis of Gaseous Samples (RAGS) facility into total fission yield. We present the calculations needed for this conversion, including the decays in and out of fission fragment chains during the RAGS pump-down of the NIF chamber.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Experiments on the origin of molecular chirality by parity non-conservation during beta-decay

Experiments are described to test a theory for the origin of optical activity wherein the longitudinally polarized electrons resulting from parity violation during radioactive beta decay, and their resulting circularly polarized Bremsstrahlung, might interact asymmetrically with organic matter to yield optically active products. Experiments involve subjecting a number of racemic and optically active amino acid samples to irradiation in a 61700 Ci90SR-90Y beta radiation source for a period of 1.34 years, then examining them for any asymmetric effects by means of optical rotatory dispersion and analytical gas chromatography. In the cases of D,L-leucine, norleucine, norvaline and proline as solids, of D,L-leucine in solution and of D,L-tyrosine in alkaline solution no optical rotation was observed during CRD measurements in the 250-630 nm spectral region. While slight differences were noted in the percent radiolysis of solid D- (12.7%) and L-leucine (16.2%) as determined by GC, no enrichment of either enantiomer was found.

Bonner, W. A.↗

Effects of He Ion Irradiation in Simple Borosilicate Glasses for HLW Immobilisation - 20324

High-level radioactive waste (HLW) consists of fission products and minor actinides. Borosilicate glass is the host material of choice in most countries to safely immobilize HLW, followed by eventual geological disposal. HLW glasses will experience both self-heating and self-irradiation effects due to the decay of fission products and minor actinides present therein. During the first 500 years of geological disposal, beta-gamma decay will be the main source of radiation due to short half-lives of fission products, as compared to very long-lived actinides which will be responsible for irradiation over much longer timescales. High-energy alpha particles and alpha recoil nuclei can potentially have significant impact (stored energy, volume change, accumulated dose, chemical durability) on the performance of the wasteform over longer timescales. Thus, to ensure safe and economic disposal over geological periods (10{sup 4} - 10{sup 6} years), the assessment of performance and properties in terms of radiation effects becomes indispensable. This work aims to simulate the effects of alpha decay in radioactive waste glasses. Two international glasses, namely UK 'MW' lithium-sodium borosilicate and Indian sodium-barium borosilicate, which are being used as HLW immobilization matrices by the UK and India respectively, were prepared by a melt-quench method and annealed below their glass transition temperatures. Both glasses were irradiated with 650 KeV He{sup 2+} ions with doses ranging from 10{sup 15} to 10{sup 17} ions/cm{sup 2}. Structural analysis was carried out using electron paramagnetic resonance (EPR) and Raman spectroscopies. First derivative continuous wave EPR spectra were recorded for all pristine and irradiated glass monoliths at room temperature using an X-band (frequency 9.6 GHz) EPR Bruker spectrometer. Results from EPR analyses showed the formation of irradiation induced paramagnetic centers at g ∼ 2.00 in all irradiated glasses. Raman spectra of pristine and irradiated samples were acquired, and showed notable changes in glass structure post-irradiation, with the emergence of a broad Raman band at 1560 cm{sup -1} upon irradiation with high fluences. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗