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At least 145 records · Page 8

Rapid extraction of short-lived isotopes from a buffer gas cell for use in gas-phase chemistry experiments, Part II: On-line studies with short-lived accelerator-produced radionuclides

We report a novel combination of advanced gas-chromatography and detection systems coupled to a buffer-gas cell was characterized on-line to allow gas-phase chemical studies of accelerator-produced short-lived α -decaying mercury, francium, and astatine isotopes. These were produced in 40 Ar- and 48 Ca-induced nuclear fusion–evaporation reactions, subsequently isolated in the recoil separators MARS at Texas A&M University, USA, and TASCA at GSI Darmstadt, Germany, before being thermalized in a buffer-gas-stopping cell. From the latter, the nuclear reaction products were extracted into gas-phase chromatographic systems, suitable for registering α-decaying short-lived radionuclides, such as isotopes of superheavy elements. Efficiencies of 21(3)% for 204-209 Fr were reached for the extraction into the optimized miniCOMPACT gas-chromatography setup, indicating that this technique enables the identification of isotopes of volatile as well as non-volatile elements. These studies guide the path towards chemical investigations of superheavy elements beyond flerovium, which are out of reach with currently used setups.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

3D Printed Microfluidic Supported Liquid Membrane Module for Radionuclide Separations

Microfluidic supported liquid membrane extraction is a promising technique for microliter-scale radionuclide separations because it requires very small reagent volumes and combines extraction and stripping in a single unit operation. Flat sheet supported liquid membrane (FS-SLM) modules with 100, 200, 300, and 400 μm deep channels were fabricated at a cost of less than 5 USD in material using a commercially available resin three-dimensional (3D) printer. The performance of these modules was characterized by quantifying uranium transport across a 15 v/v% tributyl phosphate (TBP) liquid membrane at flow rates between 5 and 60 μL min –1 and developing a two-dimensional (2D) numerical transport model for the system. The extent of uranium extraction was found to increase with increasing residence time and decreasing channel depth, with quantitative extraction occurring at the slowest flow rates and shallowest channel depths. The numerical model agreed well with the experimental extraction results. Time-dependent calculations showed that the modules reach steady state in fewer than 9 min and that there is a considerable buildup of uranium in the membrane during that time.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Removal of radionuclides from acidic solution by activated carbon impregnated with methyl- and carboxy-benzotriazoles

The removal efficiencies of metals commonly used to model the fate and transport of aqueous uranium and radioactive its daughter products, were observed on activated carbons impregnated with different benzotriazole derivatives. Acidic solutions containing U(VI), Sr(II), Eu(III), and Ce(III) were used to determine the immobilization potential of carboxybenzotriazole (CBT) and methylbenzotriazole (MeBT), where these derivatives were sorbed to different types of granular activated carbon (GAC). This sorption behavior can be predicted by Redlich–Peterson model. Flow-through column tests showed that the immobilization of uranium and some of its daughter products, significantly improves in response to oxidized GACs saturated with carboxybenzotrzole (CBT), which reached a maximum elimination for U(VI) at 260 BV, Eu(III) at 114 BV, Ce(III) at 126 BV, and Sr(II) at 100. MeBT significantly desorbed from GAC under acidic conditions. Trace amounts of CBT were observed in some column effluents, but this did not appear to alter the effectiveness of metal removal, regardless of the model radionuclide studied. These results suggest that enhanced immobilization of selected metals on GAC, can be achieved by impregnating oxidized activated carbon with carboxylated benzotriazoles, and that metal removal efficiency on this media, is related to their valence and ionic radius in acidic environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The new Device for Indirect Capture Experiments on Radionuclides at LANSCE: Efforts on measuring the resonance(s) responsible for the extremely large 88 Zr (n,γ) cross section

The thermal neutron capture cross section of 88 Zr was recently reported to be the second largest in nature with the largest resonance integral measured. Presumably, these very large values are caused by a resonance or resonances very near thermal energy. Determining their energies and widths, and hence the shape of the cross section away from thermal energies,is useful for applications. The short half-life (83.4 days) and associated large background, renders direct measurements of the neutron capture cross section impossible using current techniques. However, it is possible to measure the total neutron cross section, and hence the resonance properties, using the newly commissioned Device for Indirect Capture Experiments on Radionuclides (DICER) at the Los Alamos Neutron Science Center (LANSCE). Transmission measurements are utilized as a surrogate method to perform capture measurements. The 88 Zr needed for a DICER measurement was produced at the Isotope Production Facility (IPF) and cleanly separated from the production target material. A description of the new instrument, efforts and preliminary results on 88 Zr will be presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Building confidence in models for complex barrier systems for radionuclides

The modeling and simulation of the Cement-clay Interaction-Diffusion field (CI-D) experiment at the Mont Terri site in Switzerland presented here demonstrates that it is possible to capture the multiscale physical and chemical features of natural and engineered barrier systems for radionuclides. The simulations are successfully carried out with the newly developed CrunchODiTi high-performance computing software that accounts for multiple continua, including a continuum representing the electrical double layer (EDL) developed along negatively charged clay particles in clay rock. The simulation also accounts for both the complex three-dimensional (3D) geometry, expected as the norm in a geological waste repository, and the anisotropy of the geological formation. In addition, the high resolution of the model makes it possible to include "skin effects" developed at the interface between highly reactive materials, in this case between the high pH cement and the circumneutral but electrostatic Opalinus Clay. The successful history matching with the field experiment demonstrates that the distinct geochemical and physical properties of the cement and the Opalinus Clay in the CI-D experiment can be accounted for. Such analyses are essential for developing a defensible safety case for the underground storage of radioactive waste.

Sarsenbayev, Dauren↗

Transformational Challenge Reactor Safety Design and Radionuclide Retention Strategy

An integrated safety design and radionuclide (RN) retention strategy is developed to support the Transformational Challenge Reactor (TCR) demonstration. This demonstration aims to showcase viability for rapid deployment of a novel reactor by leveraging the advances in materials, manufacturing, and computational sciences through a highly integrated and agile design and development approach. This strategy provides a logical description and understanding of how RNs are contained within the facility. Rather than discussing fission product barriers individually between separate design and safety basis reports, this paper provides a consistent description and narrative to better facilitate regulatory interactions and focus safety design efforts. The principal barriers credited include the various coating layers in the tristructural isotropic (TRISO) fuel particle, the silicon carbide (SiC) matrix hosting the particles within the fuel element, the helium pressure boundary, and the confinement system. The choice and assumed performance of the credited barriers are highly conservative, which is a direct reflection of the low hazard that the TCR demonstration presents and the need to simplify and focus the safety review process accordingly. However, the strategy and the associated framework are generalized and may be adopted and tailored to support other advanced reactor demonstration efforts.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Measurements of Extinct Radionuclides in Filter Paper Samples

Radiochemical diagnostics rely on measurements of short-lived fission product isotopes. Once months to years have passed since isotope formation, the most useful short-lived signatures have decayed away and become extinct. Recent work at our lab has developed new methods to reconstruct the concentrations of extinct radionuclides using mass spectrometry to measure the stable daughter elements formed from radioactive decay. However, the applicability of these techniques to different types of samples has not been fully investigated.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Worker Safety and Radionuclide Intakes [Slides]

Our team detects intakes of radionuclides using urine bioassay and confirms the people responsible for protecting workers from radiation are limiting or preventing intakes. Plutonium or americium enter the body by inhalation, or a wound and stays in the body for decades. Committed Effective Dose (CED(50)) is the total dose an intake will cause over 50 years after it happens. Radiation can’t escape the body, so we look in urine. There is almost never enough radiation to make an employee sick. It takes months and multiple samples to confirm. Most “elevated” samples turn out to be false alarms.

61 RADIATION PROTECTION AND DOSIMETRY↗

Interpretation of Mineralogical Diagenesis for Assessment of Radionuclide Transport at Pahute Mesa, Nevada National Security Site

Pahute Mesa (PM) in southern Nevada was one of the four principal underground nuclear testing areas at the Nevada National Security Site (NNSS), known as the “Nevada Test Site” until 2010 (Figure 1). Eighty-two underground nuclear tests were conducted at PM in northwestern corner of NNSS (USDOE, 2015). The PM area of underground nuclear testing is located near the center of the Pahute Mesa and Oasis Valley (PM-OV) groundwater basin, which discharges to the southwest near Oasis Valley (OV) north of Beatty, Nevada (Fenelon et al. 2016; Jackson et al., 2020). Most of the PM tests were located at depths near or below the regional water table and, therefore, present potential sources of groundwater contamination from release of test-related radionuclides.

58 GEOSCIENCES↗

Determining Unabated Airborne Radionuclide Emissions Monitoring Requirements Using Inventory-Based Methods

Compliance with the airborne radionuclide emission monitoring requirements in the National Emission Standards for Hazardous Air Pollutants (NESHAP; 40 CFR Part 61, Subpart H) and State requirements in Washington Administrative Code 246–247 and 173-480 were evaluated for Pacific Northwest National Laboratory (PNNL) operations. Additional guidance may be found in the U.S. Department of Energy Handbook, Environmental Radiological Effluent Monitoring and Environmental Surveillance. To meet regulatory requirements, reviews of planned or proposed projects and activities provide the basis for implementing necessary monitoring adjustments or for implementing changes to projects and activities in a timely manner. Potential unabated off-site doses were evaluated for emission locations managed by PNNL and licensed to the Department of Energy. These locations were at facilities in Richland, Washington (i.e., the Hanford Site and PNNL-Richland Campus) and in Sequim, Washington, (PNNL-Sequim Campus, which formerly was known as the Marine Sciences Laboratory). This report describes the inventory-based methods and provides the results for the NESHAP assessment performed in January 2021 for calendar year ending 2020.

40 CFR 61 Subpart H↗

Bounding Radionuclide Release Estimates for a Hypothetical Power Reactor Accident

The object of this study is to provide an estimate of bounding radionuclide releases from a nuclear power plant accident. The time frame of interest is the release phase from the initiating event through 30 days. The maximum credible initiating event includes an initial failure of the containment function with a primary system leak. All estimates include a complete loss-of-onsite power and no successful mitigative actions. The active safety injection systems are also assumed failed. The review considers the following commonly deployed reactor designs in the following order of interest: RBMK 1000, VVER-440, VVER-1000, 1000 MWe PWR, 1000 MWe BWR, BN-800, and the 600 MWe CANDU/PHWR. The review also considers spent fuel pool accident scenarios.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Unclassified Source Term and Radionuclide Data for the Groundwater Flow and Contaminant Transport Model for Corrective Action Units 101 and 102: Central and Western Pahute Mesa, Nye County, Nevada, Revision 1

This report documents the evaluation of information and data available on the unclassified source term and radionuclide (RN) contamination for Central and Western Pahute Mesa (PM): Corrective Action Units (CAUs) 101 and 102. The Central and Western PM CAUs constitute two areas of the Nevada National Security Site (NNSS) used for underground nuclear testing (Figure 1-1). Eighty-five underground nuclear tests were conducted at the PM CAUs between 1965 and 1992 (NNSA/NFO, 2015b). Underground nuclear tests deposit radioactive elements in the subsurface, resulting in groundwater contamination in the vicinity of the underground test locations. At the PM CAUs, the testing resulted in more than 2.68 × 10 7 curies (Ci) of radioactivity (decay-corrected to September 30, 2012) remaining underground (Finnegan et al., 2016). Of the 85 underground nuclear tests conducted at the PM CAUs, three were shallow tests detonated within 200 meters (m) of the surface and referred to as the “near-surface tests”; the remaining 82 were detonated deeper than 200 m below ground surface (bgs) and are referred to as the “deep underground tests” in this document.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

M4SF-22LL010302052-Radionuclide Incorporation Model for Corrosion Products

This progress report (Level 4 Milestone Number M4SF-22LL010302052) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline Activity Number SF-22LL01030205. The research is focused on actinide and radionuclide sequestration in steel corrosion products.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Summary of Analytical Services for the Hanford Site Radionuclide NESHAP Program

This document serves as a summary of the analytical requirements used to demonstrate compliance on the Department of Energy (DOE) Hanford Site to 40 CFR 61, “National Emission Standards for Hazardous Air Pollutants,” (NESHAP) Subpart H, “National Emission Standards for Emissions of Radionuclides Other Than Radon From Department of Energy Facilities,” and WAC 246-247, “Radiation Protection – Air Emissions.” This document is a reference summarizing information from multiple existing requirement source documents and does not create, supersede, replace or over-ride any existing contractual, DOE, federal, state, permit or license requirement. The requirement source documents govern where any differences may exist.

54 ENVIRONMENTAL SCIENCES↗

Partitioning of Radionuclides in Various Streams of the Mo-99 Purification Process

The Universal Neutron Irradiator (UNI) was designed to irradiate a small volume of uranium solution and to achieve high fission power without creating a large radionuclide (RN) inventory. The UNI system is equipped with a fully enclosed off-gas system with online hydrogen gas monitoring to prevent the production of an explosive atmosphere, as well as storage cylinders for capturing fission gases. It also includes a catalytic recombiner in the target capsule (to immediately recombine radiolytic hydrogen and oxygen gas in the system) and access ports for sampling the target solution and capsule headspace. In UNI Phase I experiments, 50 mL of uranyl sulfate solution was irradiated at 0.3–0.5 W/mL fission power using a tantalum target assembly to produce photoneutrons via irradiation with an electron beam. The purposes of the Phase I experiments were to test the efficacy of adding 200 ppm Fe 2+ to the target solution to prevent uranyl peroxide precipitation under representative irradiation conditions, and to monitor iodine speciation in the irradiated uranyl sulfate solution. The focus of the UNI Phase II experiments was to use an irradiated uranyl sulfate solution containing a mixture of fission products and monitor their distribution in various streams during the primary recovery column (titania-based column) that separates Mo-99 from uranium. Irradiations were designed to create sufficient activity for tracking their distribution in various processing streams using a combination of gamma counting and inductively coupled plasma mass spectrometry (ICP-MS) analyses. Obtained data will be used to better understand the composition of waste streams, accumulation of RN on the titania column, and identify what RNs accumulate in the uranyl sulfate solution. Furthermore, this knowledge will allow us to determine waste classifications for various streams produced during the Mo-99 purification process and develop an appropriate waste clean-up strategy.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗