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At least 19 records

Neutronics Simulations of 237Np Targets to Support Safety-Basis and 238Pu Production Assessment Efforts at the High Flux Isotope Reactor

Fueled by two highly enriched uranium-bearing fuel elements surrounded by a large concentric ring of beryllium reflector, the High Flux Isotope Reactor (HFIR) provides one of the highest neutron fluxes in the world and is used to produce unique isotopes like plutonium-238. The National Aeronautics and Space Administration use radioisotope thermoelectric generators powered by 238Pu for deep-space missions. As part of the US Department of Energy s task to reestablish the domestic production of 238Pu, a technology demonstration sub-project has been initiated to establish a new 238Pu supply chain. HFIR safety-basis neutronics calculations are being performed to ensure the target irradiations have no adverse impacts on reactor performance and to calculate data required as input to follow-on thermal-structural, thermal-hydraulic and radionuclide/dose analyses. Plutonium-238 production assessments are being performed to estimate the amount of 238Pu that can be produced in HFIR s permanent beryllium reflector. It is estimated that a total of 0.96 1.12 kg 238Pu (~1.28 1.49 kg PuO2 at 85% 238Pu/Pu purity) could be produced per year in HFIR s permanent beryllium reflector irradiation facilities if they are all utilized.

depletion↗

Electron Spin Resonance Study of Fe3+ and Mn2+ Ions in 17-Year-Old Nuclear-Waste-Glass Simulants Containing PuO2 with Different Degrees of 238Pu Substitution

Three samples of a model nuclear waste glass, DRG-P1, P2, and P3, were prepared at PNNL in 1982 with identical chemical compositions but were respectively batched with 0.0, 0.1, and 0.9 wt% of 238PuO2 (half life 87.8 years) partially replacing the 1.0 wt% 239PuO2 present in DRG-P1. In 1999, samples of these glasses were sent to the Naval Research Laboratory for electron spin resonance (ESR) measurements. No radiation-induced point defects were observed. Profound alpha decay-induced changes in the ESR spectra of the batched iron-group ions were found. The spectra recorded for DRG-P1 were shown by absolute spin counts to have ESR intensities equivalent to ~85% of the sum of the batched 8.28 mole% Fe3+ and 2.79 mole% Mn2+, assuming all of those ions to behave as paramagnetic S=5/2 states at room temperature. Separate experiments and calculations ruled out the possibility of precipitated magnetite-like precipitates comprising even so much as 0.01% of the total iron. A relatively weak ESR spectral feature observed at g=4.3 is the known signature of dilute Fe3+ in glasses. However, the strongest ESR signal was found to be characterized by a first-derivative zero crossing at g=2.06 and a peak-to-peak derivative linewidth of ~150 mT, which is virtually invariant in shape with both measurement temperature and alpha-decay dose. It was discovered that these broad line shapes could be accurately simulated as weighted sums of Lorentzian shape functions of differing widths but having the same g value. The absence of any measurable anisotropy in the broad line, coupled with the temperature invariance of its width, imply the existence of extremely strong exchange interactions within clusters of Fe3+, Fe2+, Mn2+, and Ni2+ ions characterized by extremely short-range magnetic order. The result is a speromagnetic system rather than exhibiting a distinct Néel temperature. The most evident ESR effect of 17 years of 238Pu decay is the (irreversible) lowering of the intensity of the "broad line" in rough proportion to the amount of 238Pu in the sample, with concomitant increases in the amplitude of the g=4.3 feature. It was additionally observed that cooling these glasses to successively lower temperatures gives rise to reversible lowering of the broad-line intensity and increasing of the strength of the g=4.3 feature when compared with theoretical expectation for non-interacting paramagnets. The truly remarkable observation that the broad lines could be simulated as weighted sums of pure Lorentzian functions of differing widths fortuitously opened the way for high precision measurements of the ESR intensities of experimental spectra that are far broader than the magnetic field range of the available laboratory electromagnets. The areas under the simulated absorption curves fitted to the experimental spectra in the manner described provided an empirical measure of the degrees to which the present model nuclear waste glasses had been affected by alpha-decay self irradiation. Specifically, the broad-line ESR integrated-intensity data as a function of 238Pu alphadecay dose (proportional to the 238Pu doping level in these fixed-time experiments) proved to be accurately fitted by a simple saturating exponential function asymptotic to zero for infinite-time self irradiation. This result promises a precise means of extrapolating thousands of years into the future the process of "super-vitrification" that results from the creation and rapid quenching of thermal spikes due to alpha decay in glasses immobilizing 239Pu and other actinide elements. In addition, because the ESR spectra of several very different candidate high-level nuclear waste (HLW) glass compositions containing even higher amounts of Fe2O3 are also shown here to be decomposable into sums of pure Lorentzians, the analytical method we describe should be applicable to these and many other HLW glasses containing both iron-group oxides and radionuclides.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Design and Analysis of a NPO2 Target for the Production of 238PU

Current production of 238Pu at Oak Ridge National Laboratory uses NpO2–aluminum cermet pellets as the feed material. The advantage of cermet is that its thermal conductivity is much higher than that of the oxide alone, which greatly reduces pellet temperatures. However, the melting point of the material is quite low due to the aluminum in the matrix, and the recovery of the 238Pu results in substantial radioactive liquid waste. There is potentially both a significant production gain and a reduction in post-irradiation processing cost and waste associated with using a pure NpO2 pellet. This work describes ongoing efforts to design a NpO2 pellet to maximize production of 238Pu in the High Flux Isotope Reactor.

McDuffee, Joel↗

Analysis of Operating Strategies Using Different Target Designs For 238Pu Production

An engineering effort is underway to re-establish capability to produce 238Pu oxide at the kilogram scale in the United States. A multi-step batch process is being developed to produce this important material. Recently, a portion of this process was studied using discrete-event simulation tools to determine whether the conceptual process might achieve its yearly production goal. The study showed the conceptual process can meet the yearly production goal under some circumstances, but process improvements would be needed to ensure greater likelihood of success. This study extends the work performed previously by examining the effects of changing the reactor target design on the yearly process output. Two new reactor target configurations are considered an aluminum-clad reactor target containing 50% greater 237Np oxide content than the original target, and a zirconium alloy-clad target using no aluminum. The results indicate that use of the new aluminum-clad target configuration may allow the process to achieve the same yearly production goal in less time using fewer targets. If the zirconium alloy-clad target is used, then even fewer targets would be needed to reach the production goal, but some process changes would be required to handle the zirconium cladding. The number of days needed to process a target batch to completion, and the steady state 238Pu oxide production rate, for each configuration are compared to the results from the initial simulation study.

campaign↗

Fabrication of a 238Pu target

Precision neutron-induced reaction data are important for modeling the network of isotope production and destruction within a given diagnostic chain. This network modeling has many applications such as the design of advanced fuel cycle for reactors and the interpretation of radiochemical data related to the stockpile stewardship and nuclear forensics projects. Our current funded effort is to improve the neutron-induced reaction data on the short-lived actinides and the specific goal is to improve the neutron capture data on {sup 238}Pu with a half-life of 87.7 years. In this report, the fabrication of a {sup 238}Pu target for the proposed measurement using the DANCE array at LANL is described. The {sup 238}Pu target was fabricated from a sample enriched to 99.35%, acquired from ORNL. A total of 395 {micro}g was electroplated onto both sides of a 3 {micro}m thick Ti foil using a custom-made plating cell, shown in Fig 1. The target-material loaded Ti foil is sandwiched between two double-side aluminized mylar foils with a thickness of 1.4 {micro}m. The mylar foil is glued to a polyimide ring. This arrangement is shown partially in Fig. 2. The assembled target is then inserted into an aluminum container with a wall thickness of 0.76 mm, shown in Fig. 3. A derlin ring is used to keep the target assembly in place. The ends of this cylindrical container are vacuum-sealed by two covers with thin Kapton foils as windows for the beam entrance and exit. Shown in Fig. 4 is details of the arrangement. This target is used for phase I of the proposed measurement on {sup 238}Pu scheduled for Nov 2010 together with the DANCE array to address the safety issues raised by LANL. Shown in Fig. 5 is the preliminary results on the yield spectrum as a function of neutron incident energy with a gate on the total {gamma}-ray energy of equivalent Q value. Since no fission PPAC is employed, the distinction between the capture and fission events cannot be made, which is important for the higher neutron incident energy. However, it indicates that a cross section of less than one barn can be measured. The second phase of this experiment will be carried out in 2011 by assembling a PPAC with the {sup 238}Pu target to extend the measurement to higher neutron incident energies by distinguishing the capture from fission events. The fission cross section becomes dominant for neutron incident energies above 30 keV. This PPAC was developed in FY2010 under the NA22 funding and performed very well for the {sup 239}Pu and {sup 241}Pu measurements. A new {sup 238}Pu target will be fabricated for the phase II measurement using the same electroplating technique.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Case Study of a Skin Puncture Contaminated with 238Pu at Los Alamos National Laboratory

The presentation describes the incident, evaluation, and treatment path of a plutonium contaminated skin puncture wound at Los Alamos National Laboratory. Treatment included chelation and excision. The post evaluation concluded that psychological harm was the most significant health effect in this particular case and that quick treatment was vital toward a positive outcome. Treatment efficacy declines rapidly with time. Additional wrriten materials were prepared for all radiation workers and their families to improve safety education.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

PLANTS AS BIO-MONITORS FOR 137CS, 238PU, 239, 240PU AND 40K AT THE SAVANNAH RIVER SITE

The nuclear fuel cycle generates a considerable amount of radioactive waste, which often includes nuclear fission products, such as strontium-90 ({sup 90}Sr) and cesium-137 ({sup 137}Cs), and actinides such as uranium (U) and plutonium (Pu). When released into the environment, large quantities of these radionuclides can present considerable problems to man and biota due to their radioactive nature and, in some cases as with the actinides, their chemical toxicity. Radionuclides are expected to decay at a known rate. Yet, research has shown the rate of elimination from an ecosystem to differ from the decay rate due to physical, chemical and biological processes that remove the contaminant or reduce its biological availability. Knowledge regarding the rate by which a contaminant is eliminated from an ecosystem (ecological half-life) is important for evaluating the duration and potential severity of risk. To better understand a contaminants impact on an environment, consideration should be given to plants. As primary producers, they represent an important mode of contamination transfer from sediments and soils into the food chain. Contaminants that are chemically and/or physically sequestered in a media are less likely to be bio-available to plants and therefore an ecosystem.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Post-Irradiation Examination of 237Np Targets for 238Pu Production

Oak Ridge National Laboratory is recovering the US 238 Pu production capability and the first step in the process has been to evaluate the performance of a 237 Np target cermet pellet encased in an aluminum clad. The process proceeded in 3 steps; the first step was to irradiate capsules of single pellets composed of NpO 2 and aluminum power to examine their shrinkage and gas release. These pellets were formed by compressing sintered NpO 2 and aluminum powder in a die at high pressure followed by sintering in a vacuum furnace. Three temperatures were chosen for sintering the solution precipitated NpO 2 power used for pellet fabrication. The second step was to irradiate partial targets composed of 8 pellets in a semi-prototypical arrangement at the two best performing sintering temperatures to determine which temperature gave a pellet that performed the best under the actual planned irradiation conditions. The third step was to irradiate ~50 pellets in an actual target configuration at design irradiation conditions to assess pellet shrinkage and gas release, target heat transfer, and dimensional stability. The higher sintering temperature appeared to offer the best performance after one cycle of irradiation by having the least shrinkage, thus keeping the heat transfer gap between the pellets and clad small minimizing the pellet operating temperature. The final result of the testing was a target that can meet the initial production goals, satisfy the reactor safety requirements, and can be fabricated in production quantities. The current focus of the program is to verify that the target can be remotely dissembled, the pellets dissolved, and the 238 Pu recovered. Tests are being conducted to examine these concerns and to compare results to code predictions. Once the performance of the full length targets has been quantified, the pellet 237 Np loading will be revisited to determine if it can be increased to increase 238 Pu production.

07 ISOTOPE AND RADIATION SOURCES↗

Preconceptual Feasibility Study to Evaluate Alternative Means to Produce Plutonium-238

There is currently no large-scale production of 238Pu in the United States. Feasibility studies were performed at the Idaho National Laboratory to assess the capability of developing alternative 238Pu production strategies. Initial investigations indicate potential capability to provision radioisotope-powered systems for future space exploration endeavors. For the short term production of 238Pu, sealed canisters of dilute 237Np solution in nitric acid could be irradiated in the Advanced Test Reactor (ATR). Targets in the large and medium “I” positions of the ATR were irradiated over a simulated period of 306 days and analyzed using MCNP5 and ORIGEN2.2. Approximately 0.5 kg of 238Pu could be produced annually in the ATR with purity greater than 92%. Optimization of the irradiation cycles could further increase the purity to greater than 98%. Whereas the typical purity of space batteries is between 80 to 85%, the higher purity 238Pu produced in the ATR could be blended with existing lower-purity inventory to produce useable material. Development of irradiation methods in the ATR provides the fastest alterative to restart United States 238Pu production. The analysis of 238Pu production in the ATR provides the technical basis for production using TRIGA® (Training, Research, Isotopes, General Atomics) nuclear reactors. Preliminary analyses envisage a production rate of approximately 0.7 kg annually using a single dedicated 5-MW TRIGA reactor with continuous flow loops to achieve high purity product. Two TRIGA reactors represent a robust means of providing at over 1 kg/yr of 238Pu annually using dilute solution targets of 237Np in nitric acid. Further collaboration and optimization of reactor design, radiochemical methods, and systems analyses would further increase annual 238Pu throughput, while reducing the currently evaluated reactor requirements.

07 ISOTOPE AND RADIATION SOURCES↗

Development of an Efficient Approach to Perform Neutronics Simulations for Plutonium-238 Production

Conversion of 238Pu decay heat into usable electricity is imperative to power National Aeronautics and Space Administration (NASA) deep space exploration missions; however, the current stockpile of 238Pu is diminishing and the quality is less than ideal. In response, the US Department of Energy and NASA have undertaken a program to reestablish a domestic 238Pu production program and a technology demonstration sub-project has been initiated. Neutronics simulations for 238Pu production play a vital role in this project because the results guide reactor safety-basis, target design and optimization, and post-irradiation examination activities. A new, efficient neutronics simulation tool written in Python was developed to evaluate, with the highest fidelity possible with approved tools, the time-dependent nuclide evolution and heat deposition rates in 238Pu production targets irradiated in the High Flux Isotope Reactor (HFIR). The Python Activation and Heat Deposition Script (PAHDS) was developed specifically for experiment analysis in HFIR and couples the MCNP5 and SCALE 6.1.3 software quality assured tools to take advantage of an existing high-fidelity MCNP HFIR model, the most up-to-date ORIGEN code, and the most up-to-date nuclear data. Three cycle simulations were performed with PAHDS implementing ENDF/B-VII.0, ENDF/B-VII.1, and the Hybrid Library GPD-Rev0 cross-section libraries. The 238Pu production results were benchmarked against VESTA-obtained results and the impact of various cross-section libraries on the calculated metrics were assessed.

depletion↗

Design Studies for the Optimization of 238 Pu Production in NpO 2 Targets Irradiated at the High Flux Isotope Reactor

Efforts to reestablish a domestic 238 Pu production capability in support of National Aeronautics and Space Administration mission objectives are ongoing throughout the U.S. Department of Energy complex. The Plutonium-238 Supply Project (PSP) was initiated in response to a report published by the National Research Council in 2011 stating that “without a restart of 238 Pu production, it will be impossible for the United States, or any other country, to conduct certain important types of planetary missions after this decade.” The PSP is targeting a sustained, constant production rate of 1.5 kg/year of heat source PuO 2 for several years. Design and optimization studies of 237 Np-bearing targets are underway at Oak Ridge National Laboratory (ORNL). It is anticipated that targets will be irradiated in ORNL’s High Flux Isotope Reactor (HFIR) and in the Advanced Test Reactor (ATR) at Idaho National Laboratory. A variety of target materials, containments, arrangements, and irradiation histories have been analyzed, and the results indicate that a sufficient quantity of 238 Pu can be produced in HFIR and ATR to fulfill the PSP’s constant production rate target. This paper focuses on the design and optimization of new target configurations containing pellets that are (1) ~93% of the theoretical density of NpO 2 , (2) loaded into pins of cladding materials that can be handled as solid waste following postirradiation 238 Pu recovery operations, (3) irradiated in various vertical experiment facility (VXF) locations in the HFIR permanent beryllium reflector, and (4) rotated within and/or moved to another VXF location following each HFIR operational cycle to maximize 238Pu production and minimize peak heat generation rates.

07 ISOTOPE AND RADIATION SOURCES↗

Stirling to Flight Initiative

NASA has a consistent need for radioisotope power systems (RPS) to enable robotic scientific missions for planetary exploration that has been present for over four decades and will continue into the foreseeable future, as documented in the most recent Planetary Science Decadal Study Report. As RPS have evolved throughout the years, there has also grown a desire for more efficient power systems, allowing NASA to serve as good stewards of the limited plutonium-238 (238Pu), while also supporting the ever-present need to minimize mass and potential impacts to the desired science measurements. In fact, the recent Nuclear Power Assessment Study (NPAS) released in April 2015 resulted in several key conclusion regarding RPS, including affirmation that RPS will be necessary well into the 2030s (at least) and that 238Pu is indeed a precious resource requiring efficient utilization and preservation. Stirling Radioisotope Generators (SRGs) combine a Stirling cycle engine powered by a radioisotope heater unit into a single generator system. Stirling engine technology has been under development at NASA Glenn Research Center (GRC) in partnership with the Department of Energy (DOE) since the 1970's. The most recent design, the 238Pu-fueled Advanced Stirling Radioisotope Generator (ASRG), was offered as part of the NASA Discovery 2010 Announcement of Opportunity (AO). The Step-2 selections for this AO included two ASRG-enabled concepts, the Titan Mare Explorer (TiME) and the Comet Hopper (CHopper), although the only non-nuclear concept, InSight, was ultimately chosen. The DOE's ASRG contract was terminated in 2013. Given that SRGs utilize significantly less 238Pu than traditional Radioisotope Thermoelectric Generators (RTGs) - approximately one quarter of the nuclear fuel, to produce similar electrical power output - they provide a technology worthy of consideration for meeting the aforementioned NASA objectives. NASA's RPS Program Office has recently investigated a new Stirling to Flight (S2F) initiative with the objective of developing a 100-500 We Stirling generator system. Additionally, a different approach is being devised for this initiative to avoid pitfalls of the past, and apply lessons learned from the recent ASRG experience. Two key aspects of this initiative are a Stirling System Technology Maturation Effort, and a Surrogate Mission Team (SMT) intended to provide clear mission pull and requirements context. The S2F project seeks to lead directly into a DOE flight system development of a new SRG. This paper will detail the proposed S2F initiative, and provide specifics on the key efforts designed to pave a forward path for bringing Stirling technology to flight.

Robotics↗

Increased Plutonium-238 Production via High Flux Isotope Reactor Permanent Beryllium Reflector Redesign

Irradiation of 237Np-bearing targets in the permanent beryllium reflector (PBR) of Oak Ridge National Laboratory’s (ORNL) High Flux Isotope Reactor (HFIR) results in high-purity 238Pu that can be used as a reliable power source for deep space and planetary National Aeronautics and Space Administration missions. However, HFIR’s 238Pu production capability is constrained by the available irradiation volume in its PBR. In preparation for the HFIR beryllium change-out in 2023, ORNL staff have redesigned the PBR to include six additional irradiation sites, be more versatile with respect to irradiation and scattering experiments, and enhance its thermal-structural performance. The new PBR design offers large potential increases in annual 238Pu production at ORNL.

Chandler, David↗