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At least 19 records

A new TEVA-DGA chromatography procedure to separate Pu, Am, and Np from bulk U materials

Trace actinides present within uranium (U) material are diagnostic signatures of U processing history. For example, the emplacement of U material within the high neutron-flux environment of a nuclear reactor can cause neutron capture of U to form 241-plutonium ( 241 Pu). Plutonium-241 then decays to progeny isotopes 241-americium ( 241 Am) and 237-neptunium ( 237 Np); therefore, the presence and relative abundances of these trace actinides is indicative of the material’s production history and intended employment (Mayer et al., 2013). During a pre-detonation nuclear forensics investigation, measurement of trace actinide 241 Pu, 241 Am, and 237 Np concentrations by an analytical laboratory may be requested. However, chemically purifying these elements from bulk U is a challenging and involved procedure requiring several sequential chromatography columns across 4+ days. To expedite Pu-Am-Np separation from bulk U material, and to improve the yield recovery of these elements, this DHS Postdoc Fellowship has worked to create a new chromatography separation chemistry.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Identification of mixed sources with an organic scintillator-based radiation portal monitor

We have developed radionuclide identification algorithms for radiation portal monitor applications. One algorithm uses a spectral angle mapper to match the power spectral density of modified cumulative distribution functions of measured pulse height distributions to reference spectra, while the others rely on the decomposition of the observed spectrum as a linear mixture of known radionuclide spectra. Three algorithms were then tested for their ability to perform on-the-fly radionuclide identification on datasets acquired with a liquid organic scintillator-based pedestrian radiation portal monitor on moving special nuclear material and industrial radiological sources, as well as common medical isotopes. We quantified and compared the relative efficacies of the algorithms considered using F-score analysis. Measured radiation sources included 51 g of highly enriched uranium, 6.6 g of weapons grade plutonium, 241 Am, 133 Ba, 57 Co and 137 Cs sources with activities of several hundred kBq, as well as 260 kBq liquid solution samples of the medical isotopes 99m Tc, 111 In, 67 Ga, 123 I, 131 I, and 201 Tl. We achieved 100% positive identification, for three-second measurements of single sources moving at a source-transit speed of 1.2 m/s. For mixed sources with strongest and weakest sources having no more than a 5:1 ratio of detected counts, encouraging positive identification results were achieved with the un-mixing algorithms. Current radiation portal monitor designs suffer from a high incidence rate of nuisance radiation alarms caused in radiation portal monitor primary screenings by recent nuclear medicine patients and cargo containing large amounts of naturally occurring radioactive materials. Integrating reliable on-the-fly radionuclide identification into the radiation portal monitors could lower the number of nuisance alarms requiring time-consuming secondary inspections.

47 OTHER INSTRUMENTATION↗

Q-Spectroscopy

A new tool for rapid single-particle analysis in safeguards is described. This quantitative analysis tool has advantages over conventional methods for isotopic analysis of actinide-bearing samples. The method can be used to determine chemical age via 241 Am/ 241 Pu ''atomic clock''.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Surrogate Measurements of Actinide (n,2n) Cross Sections with NeutronSTARS

Directly measuring (n,2n) cross sections on short-lived actinides presents a number of experimental challenges. The surrogate reaction technique is an experimental method for measuring cross sections on short-­lived isotopes, and it provides a unique solution for measuring (n,2n) cross sections. This technique involves measuring a charged-­particle reaction cross section, where the reaction populates the same compound nucleus as the reaction of interest. To perform these surrogate (n,2n) cross section measurements, a silicon telescope array has been placed along a beam line at the Texas A&M University Cyclotron Institute, which is surrounded by a large tank of gadolinium-doped liquid scintillator, which acts as a neutron detector. The combination of the charge-particle and neutron-detector arrays is referred to as NeutronSTARS. In the analysis procedure for calculating the (n,2n) cross section, the neutron detection efficiency and time structure plays an important role. Due to the lack of availability of isotropic, mono-energetic neutron sources, modeling is an important component in establishing this efficiency and time structure. This report describes the NeutronSTARS array, which was designed and commissioned during this project. It also describes the surrogate reaction technique, specifically referencing a 235 U(n,2n) commissioning measurement that was fielded during the past year. Advanced multiplicity analysis techniques have been developed for this work, which should allow for efficient analysis of 241 Pu(n,2n) and 239 Pu(n,2n) cross section measurements

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

239Pu(n, 2n) and 241Pu(n, 2n) surrogate cross section measurements using NeutronSTARS

The goal of this project was to develop a new approach to measuring (n,2n) reactions for isotopes of interest. We set out to measure the 239 Pu(n,2n) and 241 Pu(n,2n) cross sections by directly detecting the 2n neutrons that are emitted. With the goal of improving the 239 Pu(n,2n) cross section and to measure the 241 Pu(n,2n) cross section for the first time. To that end, we have constructed a new neutron-charged-particle detector array called NeutronSTARS. It has been described extensively in Casperson et al. [1] and in Akindele et al. [2]. We have used this new neutron-charged-particle array to measure the 241 Pu and 239 Pu fission neutron multiplicity as a function of equivalent incident-neutron energy from 100 keV to 20 MeV. We have made a preliminary determination of the 239 Pu(n,2n) and 241 Pu(n,2n) cross sections from the surrogate 240 Pu(α,α’2n) and 242 Pu(α,α’2n) reactions respectively. The experimental approach, detector array, data analysis, and results to date are summarized in the following sections.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Nuclear waste calorimeter for very large drums with 385 litres sample volume

Calorimetry is a very precise and well adapted tool for the classification of drums containing nuclear waste material depending on their level of activities (low, medium, high). A new calorimeter has been developed by SETARAM Instrumentation and the CEA Valduc in France. This new calorimeter is designed for drums having a volume bigger than 100 liters. It guarantees high operator safety by optimizing drum handling and air circulation for cooling, and optimized software for direct measurement of the quantity of nuclear material. The LVC1380 calorimeter makes it possible to work over the range 10 to 3000 mW, which corresponds to approximately 0.03 to 10 g of tritium or 3 to 955 g of {sup 241}Pu in a volume up to 385 liters. This calorimeter is based on the heat flow measurement using Peltier elements which surround the drum in the 3 dimensions and therefore measure all the heat coming from the radioactive stuff whatever its position inside the drum. Calorimeter's insulating layers constitute a thermal barrier designed to filter disturbances until they represent less than 0.001 Celsius degrees and to eliminate long term disturbances associated, for example, with laboratory temperature variations between day and night. A calibration device based on Joule effect has also been designed. Measurement time has been optimized but remains long compared with other methods of measurement such as gamma spectrometry but its main asset is to have a good accuracy for low level activities.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Delayed Gamma-Ray Spectroscopy for Non-Destructive Assay of Nuclear Materials

High-­energy, beta-delayed gamma-­ray spectroscopy is a potential, non-­destructive assay techniques for the independent verification of declared quantities of special nuclear materials at key stages of the fuel cycle and for directly assaying nuclear material inventories for spent fuel handling, interim storage, reprocessing facilities, repository sites, and final disposal. Other potential applications include determination of MOX fuel composition, characterization of nuclear waste packages, and challenges in homeland security and arms control verification. Experimental measurements were performed to evaluate fission fragment yields, to test methods for determining isotopic fractions, and to benchmark the modeling code package. Experimental measurement campaigns were carried out at the IAC using a photo-­neutron source and at OSU using a thermal neutron beam from the TRIGA reactor to characterize the emission of high-­energy delayed gamma rays from 235 U, 239 Pu, and 241 Pu targets following neutron induced fission. Data were collected for pure and combined targets for several irradiation/spectroscopy cycle times ranging from 10/10 seconds to 15/30 minutes.The delayed gamma-ray signature of 241 Pu, a significant fissile constituent in spent fuel, was measured and compared to 239 Pu. The 241 Pu/ 239 Pu ratios varied between 0.5 and 1.2 for ten prominent lines in the 2700-­3600 keV energy range. Such significant differences in relative peak intensities make it possible to determine relative fractions of these isotopes in a mixed sample. A method for determining fission product yields by fitting the energy and time dependence of the delayed gamma-­ray emission was developed and demonstrated on a limited 235 U data set. De-­convolution methods for determining fissile fractions were developed and tested on the experimental data. The use of high count-­rate LaBr 3 detectors was investigated as a potential alternative to HPGe detectors. Modeling capabilities were added to an existing framework and codes were adapted as needed for analyzing experiments and assessing application-­specific assay concepts. A de-­convolution analysis of the delayed gamma-­ray response spectra modeled for spent fuel assemblies was performed using the same method that was applied to the experimental spectra.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Applications of neutron-absorbing structural amorphous metal (SAM) coatings for criticality safety controls of used fuel storage, transportation, and disposal - 14534

Used nuclear fuel contains fissionable materials ({sup 235}U, {sup 239}Pu, {sup 241}Pu, etc.). To prevent nuclear criticality in used fuel storage, transportation, and disposal, neutron-absorbing materials (or neutron poisons, such as borated stainless steel, Boral{sup TM}, Metamic{sup TM}, Ni-Gd, etc.) would have to be applied. Corrosion-resistant, iron-based structural-amorphous metals (SAMs) have been tested to determine their relative corrosion resistance. Many of these materials can be applied as coatings with advanced High Velocity Oxy-Fuel (HVOF) thermal-spray technology. SAM2X5, SAM1651, and other SAMs are amorphous-metal composite alloys that have been identified as having outstanding corrosion resistance. Because of its high boron content, SAM2X5 can be applied as the neutron-absorbing coatings to the metallic support structure for criticality-safety controls of used fuel in racks in wet storage pool and baskets inside the storage containers, the transportation cask, and eventually the disposal containers in repository disposal. Research and experiment conducted at Lawrence Livermore National Laboratory indicated that the high boron-containing SAM2X5 coating could be an effective criticality control material for used fuel management. The neutron irradiation experiments and the neutron transmission measurements conducted at McClellan Nuclear Radiation Center indicated that extensive fast neutron irradiation did not change the structure of the amorphous SAM2X5 melt-spun ribbons, and SAM2X5 exhibited effective neutron absorbing capability, similar to Boral{sup TM} and Metamic{sup TM}. (authors)

36 MATERIALS SCIENCE↗

Minimum critical masses and their uncertainties for several fissile nuclides and reflectors - 14296

A systematic effort was undertaken to reevaluate the minimum critical mass for several fissile nuclides and reflectors. This was done using MCNP6 in combination with several modern nuclear data libraries, viz. ENDF/B-VII.1, JENDL-4.0 and JEFF-3.1.1. This combination was benchmarked extensively against criticality safety benchmarks. The procedure to extract the minimum critical mass from the MCNP6 calculations was carefully implemented, so that it would have a negligible impact on the accuracy of the end results. All parts of the calculation, i.e. nuclear data processing, MCNP6 models, and post-processing, were applied consistently for all cases, involving varying fissile nuclides and reflectors. Results for the minimum critical mass were generated for {sup 233,235}U, {sup 236,239,241}Pu, {sup 242m}Am, {sup 243,245,247}Cm, and {sup 249,251}Cf, for the case of water moderation and water reflection. For {sup 235}U, the minimum critical mass was also calculated for cases with other reflectors, such as beryllium, heavy water, graphite, lead, and concrete. The results for the water reflection cases are in good agreement with most of the literature values, but for the cases with reflectors such as graphite, lead, or concrete, there are sizable differences. The accuracy of the results was assessed in two ways. First, a comparison was made with criticality safety benchmark results, by selecting benchmarks that resemble the minimum mass systems the most. It was clear that for {sup 233,235}U and {sup 239}Pu with water reflection, the differences in minimum critical masses between the libraries are consistent with the differences obtained for benchmark cases. The difference between the benchmark calculations and the benchmark values is then an indication of the accuracy with which one can simulate comparable systems. Secondly, sensitivity runs were performed with the new MCNP6 sensitivity option, based on ENDF/B-VII.1 nuclear data. For each fissile nuclide, the sensitivity of k{sub eff} to cross sections such as capture, fission, elastic, inelastic was calculated for the minimum critical mass case. The same was done for the {sup 1}H and {sup 16}O cross sections in the moderator and reflector. The uncertainty in k{sub eff} was calculated by combining the sensitivity profiles with the appropriate ENDF/B-VII.1 covariance matrix, using the SUSD code. As a final step, the uncertainty in k{sub eff} can be translated to an uncertainty in the minimum critical mass. (author)

42 ENGINEERING↗

Reactor Physics Analysis of Transitioning to a Thorium Fuel Cycle with Molten Salt Reactors

Commercial power reactors operating in the United States are light-water reactors (LWRs) fueled with low-enriched uranium (LEU) in a once-through fuel cycle; the important fissile isotopes are {sup 235}U, {sup 239}Pu, and {sup 241}Pu. In a thorium fuel cycle, the fertile isotope {sup 232}Th is converted into {sup 233}U, a fissile isotope that is not naturally occurring. In transitioning from the once-through fuel cycle to the thorium fuel cycle, the availability of man-made {sup 233}U presents a challenge: without it, the initial fissile material fueling the first reactors built in this transition is not the fissile isotope that the reactor is breeding. The transition requires an alternate fissile material until enough surplus {sup 233}U is available to start up additional reactors. In liquid-fueled molten salt reactors (MSRs), the fuel is dissolved into molten salt, which is continuously circulated through the core, simultaneously undergoing irradiation, chemical treatments and separations, and feeds. MSRs are an attractive technology in which the thorium fuel cycle can be deployed, as the {sup 233}U bred from {sup 232}Th is continuously being recycled back through the core. The bred fissile material is immediately available to fuel the core without processing or fuel fabrication. After start-up, only a fertile {sup 232}Th feed is necessary to sustain criticality in the MSR. But, in single-fluid MSRs, the initial fissile and fertile materials are mixed into the same molten fuel salt, complicating separations of initial and bred fissile materials. In solid-fuel systems, these materials are often separate. This analysis herein builds on previous work modeling thorium-fueled MSR start-up. It is based on unit cell representations of the graphite-moderated, 2250 MWt Oak Ridge National Laboratory (ORNL) Molten Salt Breeder Reactor (MSBR). This paper discusses the start-up of the first MSR in the transition to a thorium fuel cycle and identifies challenges and limitations of fuel cycle deployment with this reactor technology. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

There Are Safe Limits for Radioactivity - Does WIPP Need to Filter its Exhaust Air? - 17165

Pilot Plant (WIPP) underground repository resulted in the release of americium and plutonium (mostly {sup 241}Am) into the environment and contaminated portions of the repository, primarily along the ventilation path from the location of the incident. The WIPP uses a ventilation system to ensure that underground air is circulated through the repository and to ensure that air quality conditions are safe for the workers. Since the air in the repository exits to the surface through an exhaust shaft, this shaft is the sole potential pathway for airborne radioactivity release from the repository. During normal operations before the 2014 incident, exhaust air was released to the environment unfiltered, with an automatic switch to filtration when airborne radioactivity was detected immediately down-stream from the active waste disposal operation. However, since the radiation release event, the WIPP ventilation system has been, and will likely remain in what is called 'filtration mode,' (i.e., exhaust air is routed through a HEPA filter system). Redirection of the ventilation system through the HEPA (High Efficiency Particulate Air) filter system was necessary at the peak of the radiation release event to protect aboveground workers at the site and the public in the surrounding areas; however, it has hampered recovery efforts and has exacerbated the inherent safety issues of working underground. As a component of the Carlsbad Environmental Monitoring and Research Center's (CEMRC) WIPP environmental monitoring program, airborne radioactivity samples are collected daily in the exhaust shaft ventilation air as it reaches the surface, and before entering the HEPA filters. Since June 2014, airborne radiation levels entering the HEPA filters have averaged about 1% of a derived air concentration (DAC) for {sup 241}Am. An airborne radioactivity level of one DAC is equivalent to a potential worker internal dose exposure of 50 mSv per work year, if a worker were continuously exposed for a full work year (2000 hours). During Project Reach and throughout decontamination campaigns conducted in Panel 7 for several months in 2015, these unfiltered levels rose to 3-5% of a DAC, with a one week spike reaching almost one DAC in June 2015, during decontamination of the most heavily contaminated exhaust drift in Panel 7. Since that period, the unfiltered levels have never exceeded 2% of a DAC. Going forward, the question is, should WIPP resume unfiltered discharge of its underground ventilation air? Evaluation of more than two years of underground ventilation sampling data indicates that residual radioactivity levels in the underground no longer warrant HEPA filtration in order to meet either worker or environmental protection criteria. In terms of radiological risk at or in the vicinity of the WIPP site, the increased risk from resuming unfiltered ventilation is exceedingly small and would not result in a hypothetical dose to a member of the public in excess of the 100 micro Sv per year limit for periodic confirmatory sampling as required for operating repositories by the Environmental Protection Agency (40 CFR 191). In addition, the requirement for respiratory protection for workers underground exposed to 1-2% of a DAC is questionable, given the added industrial safety risk of heavy equipment operation while wearing respirators. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Genetic algorithm optimization of tin–copper graded shielding for improved plutonium safeguards measurements

Plutonium nuclear material safeguards is essential to ensure that states do not divert plutonium to clandestine nuclear weapons programs. Traditional safeguards methods rely on correlated neutron measurements. Detection systems based on organic scintillators, which are sensitive to fast neutrons and photons, are gaining support for use in safeguards applications due to increased capabilities and shorter measurement times compared to the current state-of-the-art. A drawback of organic scintillators in plutonium measurements is data throughput limitations; 241 Am builds up in plutonium samples and emits 60-keV gamma rays with a high specific activity. In this work, a genetic algorithm is used to design graded shielding made of tin and copper to attenuate the 60-keV gamma rays. The shield is designed to limit the attenuation of the higher-energy, fission photons, because fission photons can be used as a signature. The genetic algorithm optimization takes days to run, while a complete search space exploration would take years. The genetic algorithm was run for different levels of 60-keV gamma-ray attenuation, and the thickness of the required shielding layers was determined at each level. Tin–copper shielding was placed in front of an array of organic scintillation detectors for a measurement of approximately 4.5 kg of alpha-phase, weapons-grade plutonium, an AmLi source, and a 252 Cf source. We show that the shield successfully attenuated low-energy, non-fission gamma rays, which significantly improved the organic scintillator performance.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

241 Am Ingrowth and Its Effect on Internal Dose

Generally, plutonium has been manufactured to support commercial and military applications involving heat sources, weapons and reactor fuel. This work focuses on three typical plutonium mixtures, while observing the potential of 241 Am ingrowth and its effect on internal dose. The term “ingrowth” is used to describe 241 Am production due solely from the decay of 241 Pu as part of a plutonium mixture, where it is initially absent or present in a smaller quantity. Dose calculation models do not account for 241 Am ingrowth unless the 241 Pu quantity is specified. This work suggested that 241 Am ingrowth be considered in bioassay analysis when there is a potential of a 10% increase to the individual’s committed effective dose. It was determined that plutonium fuel mixtures, initially absent of 241 Am, would likely exceed 10% for typical reactor grade fuel aged less than 30 years; however, heat source grade and aged weapons grade fuel would normally fall below this threshold. In conclusion, although this work addresses typical plutonium mixtures following separation, it may be extended to irradiated commercial uranium fuel and is expected to be a concern in the recycling of spent fuel.

241Am↗

Should WIPP Resume Unfiltered Discharge of Underground Ventilation?

On February 14, 2014 an incident in Panel 7, Room 7 of the Waste Isolation Pilot Plant (WIPP) underground repository resulted in the release of americium and plutonium (mostly {sup 241}Am) into the environment and contaminated portions of the repository primarily along the ventilation path from the location of the incident. The WIPP uses a ventilation system to ensure that underground air is circulated throughout the repository and to ensure that conditions are safe for the workers. Since the air in the repository exits to the surface through an exhaust shaft, this shaft is the sole potential pathway for airborne radioactivity release from the repository. During normal operations, exhaust air is released to the environment unfiltered. However, since the radiation release event, the WIPP ventilation system has been, and will likely remain in what is called 'filtration mode', (i.e., exhaust air is routed through a HEPA filter system). Redirection of the ventilation system through the HEPA (High Efficiency Particulate Air) filter system was necessary at the peak of the radiation release event to protect aboveground workers at the site and the public in the surrounding areas. However, evaluation of more than two years of underground ventilation sampling data indicates that residual radioactivity levels in the underground no longer warrant HEPA filtration in order to meet either worker or environmental protection criteria. WIPP should consider resumption of the unfiltered discharge of underground ventilation to the environment. Recent sampling data indicate that there have been no detectable releases that would have resulted in a hypothetical dose to a worker or a member of the public in excess of the 0.1 mSv (10 mrem) per year limit for periodic confirmatory sampling as required for operating repositories by the Environmental Protection Agency (40 CFR 191)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Tonopah Test Range Air Monitoring: CY2018 Meteorological, Radiological, and Wind Transported Particulate Observations

In 1963, the U.S. Department of Energy (DOE) (formerly the Atomic Energy Commission [AEC]), implemented Operation Roller Coaster on the Tonopah Test Range (TTR) and an adjacent area of the Nevada Test and Training Range (NTTR) (formerly the Nellis Air Force Range). This operation resulted in radionuclide-contaminated soils at the Double Tracks site and Clean Slate I, II, and III sites. This report documents observations made during ongoing monitoring of radiological, meteorological, and dust conditions at stations installed adjacent to the Clean Slate sites and at the TTR Sandia National Laboratories (SNL) Range Operations Center (ROC). The primary objective of the monitoring effort is to support the DOE Environmental Management Nevada Program (EM NV) in the safe remediation of the environmental legacy of nuclear device development and testing by determining if wind blowing across the Clean Slate sites is transporting particles of radionuclide-contaminated soil beyond the physical and administrative boundaries of the sites, and to provide information for designing long-term monitoring of the sites. The monitoring program in 2018 included five stations. Station 400, located within TTR Area 3 and near the ROC, monitors conditions near the local workforce center. Stations 401 and 403 are located on the northern and southeastern perimeter fence lines, respectively, of the Clean Slate III site. Stations 404 and 405 are along the northern and eastern boundary fence, respectively, at Clean Slate II. The stations are generally downwind of the contaminated areas during either northwesterly or southerly winds, which are the predominant wind directions. The stations—which are similar in design to the Community Environmental Monitoring Program (CEMP) stations operating at locations surrounding the Nevada National Security Site and TTR—include meteorological instruments and continuous-flow, low-volume air samplers. Three pressurized ionization chambers for measuring gamma energy are in use at Stations 400, 401, and 403. Saltation sensors and saltation traps are deployed at the stations adjacent to the Clean Slate sites. Detailed meteorological data are recorded on data loggers, with periodic uploads via a satellite system to the Western Regional Climate Center (WRCC) at Desert Research Institute (DRI), to monitor instrument and site conditions. Air filter samples are collected every two weeks and the deposits in the saltation traps are collected when a sufficient sample mass for analysis has accumulated (generally a six- to eight-month interval). Monitoring at TTR in calendar year (CY) 2018 provided surveillance of both ambient conditions, and ground disturbance associated with remediation activities at Clean Slate II and III. The first half of CY2018 data from Stations 404 and 405 at Clean Slate II were collected during remediation activities at that site, and data collected during the final third of the year at Stations 401 and 403 at Clean Slate III coincided with remediation work at the site. Ambient conditions prevailed at Station 400 throughout the year. Dust transport by suspension and saltation is strongly dependent on wind speed. Concentrations of PM 10 (particulate matter of aerodynamic diameter ≤10 micrometers [μm], a size fraction of small particles that are suspended in the air and can be easily inhaled) remain low until winds exceed approximately 32 kilometers per hour (km/hr) (20 miles per hour [mph]). Saltation particle counts also increase above the same general threshold wind speed. Wind speeds in excess of 32 km/hr (20 mph) occur less than three percent of the time at the sites. Ground disturbing remediation activities were carried out at Clean Slate II from October 31, 2017, until July 26, 2018. Station 404 is located closest to the remediation area and is downwind of the area when winds are from the south. By late November, analysis of dust from the air sampler at Station 404 registered increases in plutonium-239+240 ( 239+240 Pu) concentrations. Peak plutonium concentrations, accompanied by elevated gross alpha concentrations and the detection of americium-241 ( 241 Am) by gamma spectroscopy, occurred between March and May 2018. During spring and early summer of 2018, elevated radionuclide concentrations were also measured in dust collected from the air sampler at Station 405, which is more than twice the distance from the remediation activity as Station 404. A minor but sustained increase in gross alpha concentration of suspended dust collected at Stations 400, 401, and 403 was also observed starting in May 2018 and continuing into August. Stations 401 and 403 are approximately 4.8 to 6.4 km (three to four miles) from Clean Slate II and Station 400 is approximately 13 km (eight miles) from that site. The radionuclide content of material that saltated into the passive Big Spring Number Eight (BSNE) traps during the Clean Slate II remediation period increased in both the traps facing toward and away from the fenced contamination area at Station 404, with the largest increases in concentration (almost five times the previous 239+240 Pu concentration) observed in the traps facing the fenced area. The radionuclide concentration in material in the trap facing away from the fence more than doubled from that measured in 2017. A similar increase was observed for the saltation trap facing away from the fenced area at Station 405, although no increase was observed for material captured in the trap facing the fenced area. Particles ranging in size from 50 to 500 µm generally move by saltation processes and are not expected to significantly contribute to dose for someone breathing in the standard respiratory zone for adult humans (1.5 to 1.7 m [4.9 to 5.6 ft] above ground level) because they are too large to be entrained in the air as suspended dust. Remediation activities at Clean Slate III began on September 5, 2018, and continued until a brief hiatus started on December 20, 2018. Although Station 401 is much closer to the remediation area than Station 403, the first increase in gross alpha and 239+240 Pu concentrations was noted in dust from filters collected at Station 403 in early November 2018. The highest radionuclide concentrations of 2018 at the Clean Slate III stations were recorded in air samples taken from Stations 401 and 403 in late December 2018 and these concentrations were comparable between the two station locations. Gamma rate data measured by the PICs was slightly higher than the annual average at Stations 401 and 403 after remediation activities began, but no single measurement was outside of the range observed in 2018 prior to remediation activities. No increase in radionuclide concentration was observed for the Clean Slate III remediation time period on air filters collected from the other stations. Radiological monitoring at Station 400—which is located at the ROC, and therefore the closest regularly staffed work location to the Clean Slate sites—recorded a higher mean gross alpha activity from dust collected on air sampler filters than in previous years. The individual biweekly air filters yielded measurements of gross alpha that were at or below the mean plus one standard deviation measured in CY2017, except for the period from April 25, 2018, through September 12, 2018. Nonetheless, gamma spectroscopy of all air filters from Station 400 identified only naturally occurring radionuclides, with no detection of americium-241 ( 241 Am) (which is used as an indicator of plutonium-241[ 241 Pu]). Alpha spectroscopy of selected air filters collected at Station 400 did not detect plutonium-238 ( 238 Pu) or 239+240 Pu above the analytical detection limit. Gross beta and gamma exposure rate data were comparable to data from regional CEMP stations. No saltation traps are deployed at Station 400. Considering the ambient monitoring periods during CY2018, the monitoring stations adjacent to the Clean Slate sites recorded above-background 238 Pu and 239+240 Pu concentrations (SNL, 1998; Turner et al., 2003) in samples collected by passive saltation traps and on selected air filters. These observations were consistent with previous years and indicated that radionuclide movement occurred under ambient conditions by processes of both saltation and suspension. The presence of radionuclides in all saltation traps, both upwind and downwind of the fenced contamination areas, was consistent with previous radiological survey results (EG&G, 1979) that show lower concentration radiologically contaminated material dispersed outside the fenced area. Although 239+240 Pu concentrations in the air filter samples were sometimes orders of magnitude higher than background, the concentrations were below risk-based action levels defined for an industrial area worker scenario (U.S. DOE, 2014). The interception of airborne dust with above-background radionuclide concentrations demonstrates that dispersal processes are continuing. Strong winds are the driver for both suspension and saltation of dust and soil. The recorded wind speed and PM10 during remediation activities at Clean Slate II and III identified discrete wind events lasting approximately five to eight hours each, which accounted for the greatest PM 10 concentrations at the monitoring stations. These events captured the effect of winds from the northwest and from the south. The observed differences in dust loading and radionuclide concentrations for the monitoring stations when they were either upwind or downwind of the contamination area identify the remediation area as a source of plutonium contaminated dust. The increase in concentration of radionuclides in airborne dust during the remediation activities, compared with measurements under previous ambient conditions (mean 239+240 Pu concentrations during remediation activities are approximately nine to 40 times higher compared to pre-remediation concentrations, depending on monitoring station), highlights the impact of land disturbance on wind-borne contaminant transport from the Clean Slate test areas. The meteorological and particulate matter monitoring indicated that conditions for wind-borne contaminant movement exist at the Clean Slate sites, and that transport of radionuclide-contaminated soil by both suspension and saltation occurred under ambient conditions and accelerated when the sites were disturbed. The 239+240 Pu alpha spectroscopy results indicated that airborne concentrations during remediation activities ranged from 2 × 10-16 to 380 × 10-16 µCi/ml. These results can be compared to the derived air concentration limit for 239 Pu of 6 × 10-11 µCi/ml for occupational workers contained in Code of Federal Regulations 10 CFR 835, Occupational Radiation Protection. Even though the air sampling results document an increase in concentration during remediation activities, the observed concentrations are less than 0.06 percent of the occupational limit. The Corrective Action Unit (CAU) closure strategy uses a risk-based approach, whereby acceptable contaminant concentrations are determined as a function of anticipated human exposure.

54 ENVIRONMENTAL SCIENCES↗

Recycle of Am-241 obtained from long term stored plutonium for use in radioisotope power systems - 15035

Pu-238 has been used as a power source for spacecraft since the early days of space exploration. It has proven to be an effective source of power where the use of solar generated power is impractical. Its application for use in spacecraft power systems was developed by the USA and Russia who have spent many $ 100s of millions on its development and production. However, the original facilities for the production of Pu-238 are no longer in use and existing worldwide stockpiles have reduced to levels sufficient for only one or two further missions. Production of Pu-238 requires considerable facilities including a nuclear reactor and reprocessing plants that are very expensive to build and operate. The European Space Agency (ESA) has assessed the options for post-launch power generation in future European space missions and has made the decision to pursue the use of Am-241 as an alternative isotope to power future European Radioisotope Power Systems (RPS). What makes Am-241 attractive for the European market is its 100% isotopically pure production from the decay of Pu-241 in separated civil plutonium stockpiles. Historically, Europe has relied on collaborations with the USA or Russia to access these nuclear power sources. During 2009, the European Space Agency (ESA) funded a project to examine the cost and practicality of establishing a European source of material suitable for Radioisotope Power Systems (RPS). The study concluded that a small number of radioisotopes could be used in RPSs. On further review two leading candidates, Am-241 and Pu-238, were selected for further study. Whilst Pu-238 was recognized as the isotope of choice for use in RPSs, the costs of setting up a European based production facility was prohibitively expensive. Although Am-241 has a number of limitations compared to Pu-238, the much reduced production costs make Am-241 an attractive option for European based production of RPSs. Despite its lower power density of ∼ 0.11 Wth/g, Am-241 is viewed as a potential alternative to Pu-238 because of its availability within the nuclear fuel cycle. During the reprocessing of spent nuclear fuel plutonium is separated as a chemically pure PuO{sub 2} product, containing around 3-11% w/w of the Pu-241 isotope, and placed into storage. During storage the Pu-241 isotope beta decays to Am-241 with a half-life of 14.4 years. {sub 94}{sup 241}Pu → (β 14.4 y) {sub 95}{sup 241}Am. This process has resulted in many 100 kgs of americium growing into the civil plutonium stockpile in the UK; material that is of value in generating heat sources and is able to be recycled. The key benefit of Am-241 as a potential European RPS source isotope is the availability of feed material along with the facilities to process it. It is expected that aged civil PuO{sub 2} will contain 25-50 g Am-241 per kg PuO{sub 2} depending on the source. A conceptual flowsheet using facilities for separating americium from plutonium is expected to produce on average 8.4 kg Am/year. ESA are now following their published road-map of studies to develop flight ready RTGs and RHUs. This has included the development and testing of the flowsheet to be used for production of Am-241. The project has focused on underpinning the conceptual flowsheet, using aged plutonium in NNL's PuMA laboratory. This has underpinned the design of a plant to produce a steady supply of Am-241. The scope of the overall project is 'store to store' - the starting point is aged plutonium currently housed in existing Sellafield stores and the end point is the storage of separated plutonium and americium powders on the Sellafield site. The full scale process is planned to be housed within the NNL's Central Laboratory in an existing facility designed for plutonium active operations. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Updated Reference VTR Core for CD-1

A preliminary reference core design was previously developed for the Versatile Test Reactor. The main features are that it is a 300 MW th sodium-cooled fast reactor using ternary metallic fuel U-20Pu-10Zr and able to achieve peak fast fluxes (E n > 0.1 MeV) in excess of 4.0x10 15 n/cm 2 -s. The plutonium in the fuel was assumed to be “reactor grade”, with a fissile quality of about 72% (i.e., 239 Pu and 241 Pu comprise 72% of the plutonium isotopes), and the uranium was assumed to be low-enriched uranium with 5% 235 U. This preliminary core design has been used through the CD-0 phase of the VTR project. Progression of the work after CD-0 led to revising, updating and refining the reference VTR core design, based on considerations from the various VTR teams: fuel, experiment, safety, and plant design teams. The objective of this report is to summarize the various changes made and details added to the model, to provide a description of the updated reference VTR core design and of its performance characteristics. This includes the traditional reactor physics characteristics, fuel cycle details, reactivity coefficients, temperature distributions, control rod worths and shutdown requirements. All of these define the updated “reference VTR core” intended to be used through CD-1.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Improved plutonium and americium photon branching ratios from microcalorimeter gamma spectroscopy

Photon branching ratios are critical input data for activities such as nuclear materials protection and accounting because they allow material compositions to be extracted from measurements of gamma-ray intensities. Uncertainties in these branching ratios are often a limiting source of uncertainty in composition determination. Here, we use high statistics, high resolution - (60–70 eV full-width-at-half-maximum at 100 keV) gamma-ray spectra acquired using microcalorimeter sensors to substantially reduce the uncertainties for 11 plutonium ( 238 Pu, 239 Pu, 241 Pu) and 241 Am branching ratios important for material control and accountability and nuclear forensics in the energy range of 125 keV to 208 keV. Lastly, we show a reduction in uncertainty of over a factor of three for one branching ratio and a factor of 2–3 for four branching ratios.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗