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At least 1,333 records · Page 74

Recovery and Recycle of Irradiated Low-Enriched Uranium from the Production of 99 Mo

Technetium-99m ( 99m Tc), the daughter (decay product) of molybdenum-99 ( 99 Mo), is the most commonly used medical radioisotope in the world. 99 Mo is produced primarily from the fissioning of 235 U. A potential future producer, Eden Radioisotopes, is planning to irradiate low-enriched-uranium metal-foil targets for production of 99 Mo. Their plan is to recover, purify, and recycle the irradiated LEU in a new set of targets inside their facility. This study assesses processes to (1) purify and recycle uranium following 99 Mo recovery and (2) convert the uranium to metal for subsequent foil production and target fabrication. A UREX (uranium recovery by extraction) liquid–liquid extraction flowsheet that utilizes centrifugal contactors was developed using the Argonne model for universal solvent extraction (AMUSE) to recover and purify the uranium. The calculated flowsheet predicted high decontamination from Pu and most fission products and >99.99% recovery of uranium. Suggestions for conversion of the UREX U-product (uranyl nitrate in dilute nitric acid) to U metal were provided based on literature studies and earlier laboratory studies performed at Argonne National Laboratory.

07 ISOTOPE AND RADIATION SOURCES↗

Your Role as a Program Manager in Pit Production Mission Integration (PPMI-DO)

PPMI is responsible for integrating the planning, execution, and reporting for LANL’s Pit Manufacturing efforts, surplus plutonium disposition activities, the Material Recycle and Recovery (MR&R) program, and other programs of national significance. Our programmatic sponsors rely on PPMI to capitalize on the unique capabilities and expertise in PF-4 (the only Security Cat I/Haz Cat II Pu processing facility in the Nation) and other vital facilities across the laboratory to deliver on mission critical products in support of National Security.

42 ENGINEERING↗

Effects of 18 O Exchange on Neutron Emission Rates of Aging 238 PuO 2 LWRHUs

The Lightweight Radioisotope Heater Unit (LWRHU) provides about 1 Watt of thermal power to critical electrical and mechanical systems in the extreme temperatures of space, maintaining the operating temperature of the spacecraft’s scientific and general operating equipment. Los Alamos National Laboratory (LANL) designed and tested the LWRHU in the 1970s through early 1980s. The first production campaign at LANL was in the early 1980s in support of the Galileo mission in which over 100 LWRHUs were manufactured. In the mid-1990s, almost 200 LWRHUs were manufactured in support of the Cassini mission. After the primary Cassini manufacturing campaign, the Department of Energy (DOE) approved the fabrication of more than 10 additional LWRHUs as spares in 1998. The LWRHU assembly contains the following components: a fuel pellet, a vented capsule, a pyrolytic graphite insulator, and a fine-weave pierced fabric (FWPF) graphite aeroshell. The fuel pellet is a hot-pressed 238 PuO 2 cylindrical pellet that is sintered to create a ceramic pellet. The pellet is encapsulated in a platinum-rhodium encapsulation. The welded fueled clad is placed inside a pyrolytic graphite thermal insulation to protect the fuel from the heat produced in reentry events. The exterior layer of the LWRHU assembly is the FWPF aeroshell. Before sintering, PuO 2 granules are heated in a furnace at temperatures greater than or equal to 700°C under an enriched 16 O atmosphere in order to reduce trace quantities of 18 O. Because 18 O undergoes an (α,n) reaction, 18 O needs to be removed as much as possible to meet radiation emission requirements set by the Jet Propulsion Laboratory (JPL) and the National Aeronautics and Space Administration (NASA), as well as other agencies. The relative abundances of the oxygen isotopes are indicated by neutron emission rate (NER) measurements. LWRHUs are vented with a sintered platinum frit vent (George 1986). During extraterrestrial operation, the vent in the cladding allows helium from the decay of plutonium to escape and relieves pressure from the system while preventing the solids from escaping (Rinehart 1996, Tate 1982 & 1985). This vent is protected during manufacture by a platinum-30 rhodium cover. The capsule vent is activated by milling a 0.025-inch diameter hole through the protective cover to a nominal depth of 0.015 inches, generally immediately before the LWRHU is loaded into the aeroshell (George 1986). Prior to long-term storage, LWRHUs are vented and thus potentially allow infiltration of 18 O from the ambient atmosphere. Although NER decreases with age due to the reduction in emitted alpha particles, it might be expected that NER reduction is mitigated by the exchange of 18 O. However, this is not necessarily the case and no trend was observed relating NER to age other than the natural decay of 238 Pu (Mulford 2021). The most probable and dominant factor for determining specific NER was manufacturing discrepancies between individual units. It is important to understand the lack of observed 16 O- 18 O exchange and to compare LWRHU pellets as much as possible.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Independent Gamma Spectroscopy Analysis of a Plutonium Oxide Sample

Independent gamma spectroscopy data analysis of a plutonium oxide sample was requested on July 23, 2021. The primary request was to assess the Pu-239 activity/mass of the sample using previously collected gamma spectral data. Using the provided gamma spectral analysis report and spectral files, an independent evaluation of the data was conducted without any prior knowledge of the isotopic activity/mass of the sample.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A parallel-plate avalanche counter for the prompt fission neutron spectrum measurement

Neutrons, gamma’s, and fission fragments are among the prompt fission observables. Their precision measurements are fundamental to advance our understanding of fission and any application of fission. For our programmatic need, the χ matrix, which defines as the outgoing neutron spectrum as a function of incoming neutron energy, is sparsely populated and poorly measured for 233,235,238 U and 239,240 Pu. To improve the quality of those χ matrices, a joint LANLLLNL project was undertaken to measure their prompt fission neutron spectra at the LANSCE/WNR facility using neutron detector arrays and a charged-particle detector for the fission-fragment detection. A typical setup is shown in Fig. 1, where one of neutron detector array with a charged-particle detector is given.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Steel Corrosion Impacts on Radionuclide Immobilization

This progress report (Level 4 Milestone Number M4SF-21LL010302052) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline Activity Number SF-21LL01030205. The research is focused on actinide and radionuclide sequestration in steel corrosion products. Fuel matrix degradation models suggest that the near field is likely to be reducing at the time of canister breaching, steel corrosion, and radionuclide release, but more oxidizing conditions may prevail in the far field. The incorporation of radionuclides into corrosion phases may limit the rate of radionuclide release by sequestering a portion of the radionuclide source term. For these reasons there is a need to evaluate the incorporation of Pu and other radionuclides into various Fe-oxide phases, and to understand the behavior of coprecipitated phases during mineral recrystallization processes and during re-oxidation events. Radionuclide coprecipitation with Fe minerals may impact long-term repository performance and is an ongoing research focus at Lawrence Livermore National Laboratory.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Converter-Interfaced CHP Plant for Improved Grid-Integration, Flexibility and Resiliency

GE Research and its partner GE Renewables have proposed the use of an interface converter solution to increase the penetration of small to medium-sized CHP (1MWe to 20MWe) into distribution grids and improve their flexibility and grid support capability. Indeed, the proposed interface converter solution thanks to presence of the grid-ready inverter, allows to streamline the compliance to grid codes requirements, reduce the interconnection delays and costs and ultimately one of the main barriers for CHP adoption by commercial and industrial facilities. An additional benefit provided by the interface converter is the use of the grid-ready inverter for reactive power which eliminates the need of sizing the generator for that capability. These two benefits highly favor the economic feasibility of converter-interfaced CHP. Five user cases, each in one of the leading U.S states for CHP potential reported by the DOE in its estimation of the U.S Technical Potential of CHP, were selected to compare the economic performances of converter-interfaced CHP as compared with directly-coupled. They include a college campus in California, a hospital in New York, a water reclamation plant in Texas, a hotel in Minnesota, and a large office building in Pennsylvania. Results showed that, the presence of the interface converter allows to increase the return on investment (ROI) by 0.5 to 2 percentage points in most of the cases (4 of 5). Indeed, the interface converter by shortening the interconnection process allows to accelerate revenues while reducing interconnection costs. Added to the reduced cost of the required generator these savings trade favorably the capital cost of the converter. The analysis also showed that the profitability of the converter-interfaced CHP is highly sensitive to the energy price, interconnection delay, and converter cost. However, it appears that if the interface converter can shorten the interconnection process by at least 6 months, adopting this solution will be more economically viable than directly-coupled configuration in almost all the +23,000 sites of the U.S Technical Potential CHP. The evaluation of the benefits of a converter-interfaced CHP also showed that it enables higher ROI when coupled with other distributed energy resources (DER) such as battery energy systems (BESS) or solar photovoltaic (PV). Indeed, in those scenario, the grid-ready inverter included in the interface converter eliminates the need of separate inverters if DC-coupling is used. On the technical performance, it has been verified that the presence of the interface converter allows to reduce by 70% to 80% the CHP short-circuit contribution to grid faults. This not only reduces the mechanical and thermal stresses exposed to the CHP electrical components but also increases the grid hosting capacity which ultimately enables higher penetrations CHP. Another key benefit of the interface converter validated with hardware-in-the-loop simulations and testing is its superior capability for reactive power support. Indeed, using a power hardware testbed with two +700kW inverters configured in back-to-back, a microgrid controller and actual facilities loads it was demonstrated that the presence of the interface converter can help maintain a power factor near ~1 or regulate the voltage to ~1.0pu at the point of common coupling. This benefit can be highly valuable if in the future, due to higher penetration of renewable distributed energy resources (DER), utilities start billing demand charge based on kVA instead of kW as currently. It was also validated that converter-interfaced CHP can dispatch heat and power commands and seamlessly switch between the two modes while consistently controlling the power factor or voltage at PCC. Indeed, the power hardware testing showed that grid-connected converter-interfaced CHP can follow either the power or heat demand while maintaining a unity power factor at converter output. This research proved that the adoption of an interface converter as the solution for interconnection of CHP system into the distribution grid can greatly improve the economic feasibility of small to medium-sized CHP as well as the plant power quality, flexibility and resiliency. Additionally, it allows increased penetrations of CHP into the distribution grid, extends their grid support capability, and facilitates the integration of BESS and PV DER by streamlining their collocation within the same facilities. This ultimately provides an opportunity for commercial and small industrial facilities in the U.S to accelerate their energy transition thanks to the high energy efficiency of CHP systems and its reliable, flexible, and resilient microgrid operation when interconnected with an interface converter.

24 POWER TRANSMISSION AND DISTRIBUTION↗

C-AAC Occupancy and Transition Out of CMR [Slides]

This in-depth evaluation was performed in order to gather information for a plan and time estimate of C-AAC space cleanout and handover to the CMR facility once programmatic operations are relocated to other facilities. C-AAC space ownership in CMR wings 1, 5, 7, and 9 have been identified down to the Team level (see subsequent slides and other supporting documentation). This plan assumes that C-AAC activities that support Pu sustainment efforts (Wings 1, 5, and 7) are relocated to PF-4 and RLUOB in mid/end FY24 and current projects in Wing 9 are completed by the end of FY24/mid FY25 (cessation of C-AAC programmatic operations in CMR). This plan assumes that no other programmatic activities are initiated in CMR (e.g. MOX fuel rods). Timing and order of cleanout of programmatic laboratory and office spaces in wings 1, 5, and 7 is dependent upon analytical chemistry operations being established and relocated to RLUOB and PF-4. Timing and order of cleanout of programmatic laboratory and office spaces in wing 9 is dependent upon completion of current projects (MR&R, Thermo Fisher drum, etc.). As C-AAC Teams move out of the CMR building and into other facilities, the spaces occupied by those teams are planned to be targeted for in depth cleanout in the order that teams and capabilities are relocated.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Project 57 Air Monitoring Report: January 1 through September 30, 2020, with a Review of the Period of Record Radionuclide Analyses

The DOE Environmental Management Nevada Program (EM NV) identified the Project 57 contaminated area as Corrective Action Unit (CAU) 415, Project 57 No. 1 Plutonium Dispersion Site, which consisted of one Corrective Action Site (CAS): NAFR-23- 02, Pu Contaminated Soil (U.S. DOE, 2014). The CAS included several Project 57 operational facilities in addition to the plutonium-contaminated soil. With approval of the State of Nevada Division of Environmental Protection, the DOE closed the Project 57 surface soil contamination site in October 2020. Closure was accomplished by installing a clean soil cap constructed over ground zero and the surrounding areas of the CA that may be entrained with wind-transported soil particles. After completion of the ground zero cap in October 2020, DRI discontinued monitoring of meteorological and associated environmental conditions at the Project 57 site as directed by DOE EM NV. Navarro dismantled air monitoring stations P57-3 and P57-4 and removed the equipment on October 20, 2020. This report presents the meteorological and dust observations and radiological analyses accomplished during the approximately 10 months when the air monitoring data collection equipment was operational during CY2020.

54 ENVIRONMENTAL SCIENCES↗

The First Neptunium Dioxide Neutron Diffraction Experiment at HFIR

Here we present the first neutron diffraction experiment of a 50 mg sample of neptunium(IV) dioxide (NpO 2 ) powder at the High Flux Isotope Reactor (HFIR) using the wide-angle neutron diffractometer (WAND 2 ) HB-2C. We also provide a brief literature survey to pinpoint gaps in the crystal, electronic, and magnetic structure of NpO 2 to determine the optimum experiment to be pursued in the next HFIR user proposal cycle. Characterizing actinide materials with neutron diffraction, inelastic scattering, neutron imaging, polarized neutron studies, and small-angle neutron scattering techniques will increase our understanding of 5f electron behavior and elucidate atomic and magnetic structural properties. This strategy will help fill gaps in the literature and provide theoretical physicists with the data needed to build physical and chemical models to guide and validate computational methods. These methods may be used for predicting structural and chemical features of actinide-based materials. This proof-of-principle effort begins to uncover how to advance actinide science and technology at Oak Ridge National Laboratory (ORNL) using neutron capabilities. This effort has already sparked collaborative discussions between researchers outside the Radioisotope Science and Technology Division, including theoretical physicists from the Nuclear Nonproliferation Division and beamline scientists in the Neutron Scattering Division. We intend to continue pursuing neutron experiments and develop a scientific strategy focused on studying transuranium elements (e.g., Np, Pu, Am, and Cm) using the advanced neutron capabilities at ORNL.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Event Response and Criticality Alarm Systems [Slides]

The smallest accident, in terms of fission yield and dose rate, that a criticality alarm system is required to detect. Need for a CAS shall be evaluated for all activities in which the inventory in individual unrelated areas exceeds 700g U-235, 500g U-233, 450 g Pu-239 OR 450g of any combination of these three isotopes. Unique configurations exist such that critical mass requirements may be less than the limits noted above.

61 RADIATION PROTECTION AND DOSIMETRY↗

LLNL International Working Group on Gamma Spectrometry - Preparation of IDB Dataset

The spectral information and associated metadata, including source information, detector setup, and shielding configuration is described in human readable, comma-separated text files (csv). Five csv files are associated with each material type and include the following information (where [Isotope] is U, Pu, and MOX): [Isotope]_measurement_metadata - Metadata of the measurement configuration, including material composition at time of acquisition (decay corrected from certificate date). Data that is unique to a measurement configuration e.g. detector geometry, source-detector distance, analyzer and other electronics used, attenuating materials are provided in this file. [Isotope]_spectrum_metadata - The information that is unique to the spectrum. This includes detector specifications (e.g. date of acquisition, number of channels, gain (keV/channel), energy range, real and live time, full width half-maximum (FWHM) of the 186 or 208 peak for uranium or plutonium measurements, respectively. [Isotope]_source_metadata - The source material used for the measurement, this includes the ratio and uncertainties of isotopes present and processing information of the material. In addition, the certificate information for the source material is listed. [Isotope]_spectrum_counts_metadata - The counts per channel for each spectrum. This data is linked via the UID.spectrum index to the measurement_metadata file. [Isotope]_spectrum_checksum_metadata The MD5 checksum for the original spectrum file. This data is linked via the UID.spectrum index to the measurement_metadata file. This information is provided to prevent duplication of entries in the database.

42 ENGINEERING↗

Analysis of Tank 38H (HTF-38-21-95, -96) and Tank 43H (HTF-43-21-97, -98) Samples for Support of the Enrichment Control and Corrosion Control Programs

SRNL analyzed samples from Tank 38H and Tank 43H to support ECP and CCP. The results indicate the concentrations of most species in the Tank 38H surface sample increased from the previous surface sample. The Tank 38H sub-surface sample shows only minor changes in concentration for soluble species in the solution (e.g., Na, Al, Cs-137) relative to the previous sample, but a small decrease in concentrations for species typically associated with sludge solids (e.g., U, Pu, Fe, Si) likely because of a decrease in sludge solids from the previous sample. The large differences in the concentrations of major components between the Tank 38H surface and sub-surface samples indicate significant stratification of solution species within the tank.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

238 PuO 2 In Vitro Lung Dissolution Rate and Particle Size Determination for Material Involved in the June 8, 2020 Incident at the Los Alamos National Laboratory PF-4 Facility

As part of the LANL response to the June 8, 2020 238 PuO 2 inhalation exposure incident in PF-4, the Nuclear and Radiochemistry Group (C-NR) was asked to assist in determining the lung dissolution rate and particle size distribution of the airborne material. These material characteristics, along with urine and fecal bioassay data, are used by the Radiation Protection Services (RP-SVS) internal dosimetrists to refine dose estimates for exposed workers. Similar to previous studies, an in vitro lung dissolution rate study was performed to assess how fast 238 Pu is cleared from the lungs. Given that PuO 2 is a relatively insoluble material, it dissolves very slowly and requires in vitro studies of 100 or more days to estimate dissolution rates. This report details the results of a 100 day in vitro dissolution rate study and the particle size characteristics of 238 PuO 2 collected on an air filters during the incident. Results show that the 238 PuO 2 involved in this incident has behavior comparable to PuO 2 from previous in vitro studies, with approximately 1% of material dissolving quickly, and 99% of the material dissolving very slowly, with a half-time of approximately 120 years. This is somewhat slower than what was determined in a previous study of LANL 238 PuO 2 , which had an experimental dissolution half-time of 3 years, but significantly faster than 3000 years measured for 239 PuO 2 . Particle size distribution measurements indicate that particle sizes range from 0.10 µm – 6 µm, with most < 2 µm, which is reasonable based on our understanding of the process history of the 238 PuO 2 . Particle size, specific surface area, calcining temperature, specific activity, and age all are known factors that can impact the dissolution rate of refractory materials, however, there are too few studies to quantify the exact influence of these parameters on a measured dissolution rate. The results of this study add to that knowledge base, and provide new insights into the dissolution rates for this LANL process-specific 238 PuO 2 material.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Test Results for Checking Reliability of Selected ENDF/B-VIII.0 Evaluated Uncertainties

This report summarizes error messages obtained from counter-checking whether 1 H, 9 Be, 12 C, 27 Al, 235,238 U and 238–242 Pu relative uncertainties of ENDF/B-VIII.0 are realistic. Large parts of this report were generated automatically by the code CovVal. This code allows to test the reliability of relative uncertainties of any isotope. It gives generic error and warning messages if evaluated relative uncertainties of a particular reaction are likely under- or over-estimated. In addition to these error and warning messages, I added comments whether the flagged uncertainties are truly under- or overestimated. I call out these uncertainties that should be further investigated and corrected by an evaluator for an upcoming release of ENDF/B-VIII.1.

07 ISOTOPE AND RADIATION SOURCES↗

Including Chi-Nu 235 U PFNS Experimental Data into an ENDF/B-VIII.1 Release Candidate Evaluation

This report documents an evaluation of 235 U prompt fission neutron spectra (PFNS) that is a release candidate for the upcoming U.S. nuclear data library, ENDF/B-VIII.1. This evaluation differs from its predecessor, ENDF/B-VIII.0, mainly by the inclusion of 235 U PFNS measured by the Chi-Nu team of LANL and LLNL. This data set is the first one that covers the 235 U PFNS for continuous incident-neutron energies of 1⁻20 MeV and outgoing-neutron energies from 10 keV⁻10 MeV with high precision. Previous data sets were either measured in a limited energy range or with less precision. Hence, these new Chi-Nu data provide decisive information for the evaluation. The resulting evaluated data correspond well to the new experimental PFNS. The evaluated PFNS also produce average mean energies and 239 Pu/ 235 U PFNS in agreement with associated Chi-Nu data. If one uses the new evaluated data to predict the neutron multiplication factor, k eff , of selected ICSBEP critical assemblies, the differences of simulated values compared to those using ENDF/B-VIII.0 is modest (less than 55 pcm). This difference in k eff can be easily accommodated by changes in the 235 U average prompt fission neutron multiplicity that is currently being re-evaluated. In addition to that, the new PFNS predict on average 235 U LLNL pulsed-sphere neutron-leakage spectra better than ENDF/B-VIIII.0 PFNS.

235U↗

Fission In R-process Elements (Quarterly Report – FY2022Q1)

There are 3 tasks in FY22: (1) 9.9: Potential energy surfaces for odd-mass actinides 238 U and 232 Th (DFTNESS); (2) 9.10: Potential energy surfaces for even-even minor actinides (DFTNESS); and (3) 9.11: Independent and cumulative yields for 239 Pu and 235 U based on E* "law" extracted from TDDFT runs (FREYA).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Algal Biomass Conversion to Fuels via Combined Algae Processing (CAP) (2021 State of Technology and Future Research)

The annual State of Technology (SOT) assessment is an essential activity for platform research conducted under the Bioenergy Technologies Office. It allows for the impact of research progress to be quantified in terms of economic improvements in the overall biofuel production process for a particular biomass processing pathway, whether based on terrestrial or algal biomass feedstocks. As such, initial benchmarks can be established for currently demonstrated performance, and progress can be tracked towards out-year goals to ultimately demonstrate economically viable biofuel technologies. NREL's algae state of technology benchmarking efforts focus both on front-end algal biomass production and separately on back-end conversion to fuels through NREL's "combined algae processing" (CAP) pathway. The production model is based on outdoor long-term cultivation data, enabled by comprehensive algal biomass production trials conducted under the Development of Integrated Screening, Cultivar Optimization, and Verification Research consortium (DISCOVR) efforts, driven by data furnished by Arizona State University (ASU) at the Arizona Center for Algae Technology and Innovation (AzCATI) testbed site. The CAP model is based on experimental efforts conducted under NREL research and development projects. This report focuses on back-end conversion of algal biomass through the CAP pathway, highlighting the 2021 updates to minimum fuel selling price (MFSP). This update maintains an important recent inclusion of polyurethane (PU) previously incorporated in the 2020 SOT as a value-added coproduct. Relative to the 2020 SOT case, this indicates a minimal increase of $0.10-$0.14/GGE (roughly 2%) for both the acids and BDO pathways, attributed to minimal increases in upstream algal biomass costs from slightly lower demonstrated cultivation productivities in the 2021 SOT.

09 BIOMASS FUELS↗