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At least 91 records · Page 5

Specification of Radionuclide Classes for MELCOR Molten Salt Reactor Simulations

MELCOR has been used extensively to facilitate virtual investigations into severe nuclear accidents for light-water reactors (LWRs). Non-light water reactors (non-LWRs) render some LWR-centric approaches potentially unsuitable. MELCOR has been instrumental in analyzing source terms for LWRs and has recently expanded its applicability to non-LWRs. To simplify radionuclide (RN) tracking, MELCOR currently groups elements into 17 classes, each containing representative species. This grouping, optimized for LWRs, is not appropriate for non-LWRs due to the different chemistry. This necessitates a reevaluation of radionuclide transport modeling. This report introduces a new class scheme for MELCOR tailored to MSR modeling, expanding the current 17 classes to 32 and are explained in the context of a UF 4 fueled FLiBe carrier MSR. It provides a discussion and justification for the new groupings and outlines a methodology for discovering and defining additional classes in MELCOR using a sample calculated RN inventory and a Gibbs energy minimizer (GEM).

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

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; Title 40 of the U.S. Code of Federal Regulations Part 61, Subpart H) and State requirements in Washington Administrative Code 246–247: Radiation Protection – Air Emissions and 173-480: Ambient Air Quality Standards and Emission Limits for Radionuclides 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). This report describes the inventory-based methods and provides the results for the NESHAP assessment performed in January 2024 for calendar year ending 2023.

40 CFR 61 Subpart H↗

Pacific Northwest National Laboratory Facility Radionuclide Emission Points and Sampling Systems

Battelle–Pacific Northwest Division operates numerous research and development laboratories in Washington State. The U.S. Department of Energy (DOE) contracts to Battelle at Richland facilities on both the DOE Hanford Site and the Pacific Northwest National Laboratory (PNNL)-Richland campus. These facilities have the potential for radionuclide air emissions. The PNNL contract with DOE also includes operations at the PNNL-Sequim campus in Sequim, where there is also the potential for radionuclide air emissions. This document is a periodic update that describes current PNNL facility emission units and sampling systems.

54 ENVIRONMENTAL SCIENCES↗

Radionuclide Inventory Threshold for Trench 31 and 34 Located Within the 200 West Area Low-Level Burial Grounds

Trenches 31 and 34 located in the 200 West Area Low-Level Burial Ground (LLBG) are authorized for disposal of low-level and mixed low-level radioactive waste under DOE Order 435.1, Radioactive Waste Management. A revised Disposal Authorization Statement was issued in October 2023 following approval of the performance assessment (PA) and supporting technical basis documents. To be consistent with approved PA calculations, the waste acceptance criteria (WAC) needs to be updated to include concentration limits for Category 1 (CAT1) and Category 3 (CAT3) waste along with the inventory limits. This environmental calculation file (ECF) provides the inventory limits for Category 1 and Category 3 waste disposal of radionuclides at Trench 31 and 34 based on the PA calculations. The concentration limits are not calculated as they are provided in the PA itself. The inventory thresholds (or limits) are calculated for only those radionuclides that are identified in the PA as the primary dose contributors. The primary dose contributors for the groundwater pathway are technetium-99, iodine-129, niobium-94, chlorine-36, molybdenum-93, and niobium-93m while those for the air pathway are tritium and carbon-14.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Summary of Analytical Services for the Hanford Site Radionuclide NESHAP Program

This document is a summary of the point source analytical requirements used to demonstrate compliance for the Department of Energy (DOE) Hanford Site operations with 40 Code of Federal Regulations (CFR) Part 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 the Washington Administrative Code (WAC) 246-247, “Radiation Protection – Air Emissions.” This reference collects information from multiple source documents and is not intended to create, supersede, replace or over-ride any existing contractual, DOE, federal or state statutes, regulations, compliance agreements, orders, permits, licenses or other requirements. The requirement source document governs where any difference may exist. The Hanford Mission Integration Solutions (HMIS) Environmental organization has been contracted by DOE to manage and report data collected from the sampling and monitoring of radioactive air emissions point sources, colloquially called stacks. The Environmental organization coordinates the analyses and reporting of samples collected at various facilities across the Hanford Site. These facilities operate approximately 52 stacks that require sampling, monitoring or estimating radioactive air emissions. The stacks are operated by Bechtel National, Inc. (BNI), Central Plateau Cleanup Company (CPCCo), Hanford Tank Waste Operations & Closure (H2C), Hanford Laboratory Management and Integration (HLMI), and Pacific Northwest National Laboratory (PNNL). Stack samples from CPCCo, HLMI and H2C facilities are collected by the operating contractor staff, delivered to HMIS, and then shipped to an offsite contracted laboratory for analyses. The field and laboratory sample data uploaded into the Sample Management and Analytical Results Tracking (SMART) database are used to calculate sample volumes and concentrations. Sample concentrations are evaluated for compliance with federal and state regulations, permits, and license requirements. The SMART database also calculates total curies released for sampled point sources and stacks. Point source effluent concentrations and releases are published annually in publicly available reports. The BNI and PNNL operate several DOE-Hanford Field Office (HFO) stacks subject to the requirements of 40 CFR 61, Subpart H and WAC 246-247. The concentrations, curies released and dose modeling evaluation for these stacks are included in the DOE-HFO annual radionuclide NESHAP report. The sample collection, analyses and emissions estimates for these stacks are outside the scope of HMIS contracted responsibilities and not addressed further in this document.

54 ENVIRONMENTAL SCIENCES↗

Nondestructive determination of radionuclides in lunar samples using a large low-background gamma-ray spectrometer and a novel application of least-squares fitting

Dual-parameter gamma ray spectrometer systems with large volume Nal (Tl) crystals and low backgrounds were used for nondestructive determination of K, Th, U and cosmic ray produced radionuclides in 60 lunar samples. The total weight of samples measured with this system is 28 kg, and the individual sample weights varied from 2 to 2300 g. Samples from Apollo 11, 12, 14, 15 and 16 were measured. Operation of the spectrometers in the coincidence mode and analyzing single coincidence spectra permits the simultaneous determination of 8-10 radionuclides in each lunar sample.

Eldridge, J. S.↗

Video instrumentation for radionuclide angiocardiography.

Two types of videoscintiscopes for performing radioisotopic angiocardiography with a scintillation camera are described, and use of these instruments in performing clinical studies is illustrated. Radionuclide angiocardiography is a simple, quick and accurate procedure recommended as a screening test for patients with a variety of congenital and acquired cardiovascular lesions. When performed in conjunction with coronary arterial catheterization, dynamic radionuclide angiography may provide useful information about regional myocardial perfusion. Quantitative capabilities greatly enhance the potential of this diagnostic tool.

Kriss, J. P.↗

Positron emission reconstruction tomography for the assessment of regional myocardial metabolism by the administration of substrates labeled with cyclotron produced radionuclides

A positron emission transverse tomograph device was developed which provides transaxial sectional images of the distribution of positron-emitting radionuclides in the heart. The images provide a quantitative three-dimensional map of the distribution of activity unencumbered by the superimposition of activity originating from regions overlying and underlying the plane of interest. PETT is used primarily with the cyclotron-produced radionuclides oxygen-15, nitrogen-13 and carbon-11. Because of the participation of these atoms in metabolism, they can be used to label metabolic substrates and intermediary molecules incorporated in myocardial metabolism.

Ter-Pogossian, M. M.↗

Radionuclide measurements by accelerator mass spectrometry at Arizona

Over the past years, Tandem Accelerator Mass Spectrometry (TAMS) has become established as an important method for radionuclide analysis. In the Arizona system the accelerator is operated at a thermal voltage of 1.8MV for C-14 analysis, and 1.6 to 2MV for Be-10. Samples are inserted into a cesium sputter ion source in solid form. Negative ions sputtered from the target are accelerated to about 25kV, and the injection magnet selects ions of a particular mass. Ions of the 3+ charge state, having an energy of about 9MeV are selected by an electrostatic deflector, surviving ions pass through two magnets, where only ions of the desired mass-energy product are selected. The final detector is a combination ionization chamber to measure energy loss (and hence, Z), and a silicon surface-barrier detector which measures residual energy. After counting the trace iosotope for a fixed time, the injected ions are switched to the major isotope used for normalization. These ions are deflected into a Faraday cup after the first high-energy magnet. Repeated measurements of the isotope ratio of both sample and standards results in a measurement of the concentration of the radionuclide. Recent improvements in sample preparation for C-14 make preparation of high-beam current graphite targets directly from CO2 feasible. Except for some measurements of standards and backgrounds for Be-10 measurements to date have been on C-14. Although most results have been in archaeology and quaternary geology, studies have been expanded to include cosmogenic C-14 in meteorites. The data obtained so far tend to confirm the antiquity of Antarctic meteorites from the Allan Hills site. Data on three samples of Yamato meteorites gave terrestrial ages of between about 3 and 22 thousand years.

Jull, A. J. T.↗

Extinct radionuclides

Extinct radionuclides, or radioactive isotopes with lifetimes of the order of 1 to 100 Myr that are now extinct in the solar system are discussed. Evidence is presented for the presence of such radionuclides in the early solar system, including Al-26, Mn-53, Pd-107, I-129, Pu-244, and Sm-146. It is suggested that the abundances of these species provide constraints on nucleosynthetic time scales and the history of solar system materials before they became the solar system. The shortest-lived species is Al-26, which may have been sufficiently abundant to be the major heat source for meteorite parent-body metamorphism or igneous differentiation.

Podosek, F. A.↗

Reclamation with Recovery of Radionuclides and Toxic Metals from Contaminated Materials, Soils, and Wastes

A process has been developed at Brookhaven National Laboratory (BNL) for the removal of metals and radionuclides from contaminated materials, soils, and waste sites. In this process, citric acid, a naturally occurring organic complexing agent, is used to extract metals such as Ba, Cd, Cr, Ni, Zn, and radionuclides Co, Sr, Th, and U from solid wastes by formation of water soluble, metal-citrate complexes. Citric acid forms different types of complexes with the transition metals and actinides, and may involve formation of a bidentate, tridentate, binuclear, or polynuclear complex species. The extract containing radionuclide/metal complex is then subjected to microbiological degradation followed by photochemical degradation under aerobic conditions. Several metal citrate complexes are biodegraded, and the metals are recovered in a concentrated form with the bacterial biomass. Uranium forms binuclear complex with citric acid and is not biodegraded. The supernatant containing uranium citrate complex is separated and upon exposure to light, undergoes rapid degradation resulting in the formation of an insoluble, stable polymeric form of uranium. Uranium is recovered as a precipitate (polyuranate) in a concentrated form for recycling or for appropriate disposal. This treatment process, unlike others which use caustic reagents, does not create additional hazardous wastes for disposal and causes little damage to soil which can then be returned to normal use.

Francis, A. J.↗

Use of simultaneous radionuclide and other trace constituent measurements to determine fluxes and atmospheric residence times

Finding a way to use atmospheric concentrations to determine source strengths and atmospheric residence times pose considerable difficulties. An approach is to use simultaneously measured radionuclide concentrations as a means of deriving fluxes and residence times for certain atmospheric trace constituents of interest. The study and use of such methods in a pilot field experiment were among the original goals of this program. Four such approaches were studied or developed; suitable sampling and analysis systems were built and tested or are in the final stages of construction; and a small scale field experiment. The evolution is reviewed of the program and the field experiment is described along with the possibilities for its eventual extension to include other species of interest. The four radionuclide based approaches studied are: Mean vertical profiles; Trajectory correlation; Boundary layer discontinuity; and Lead deposition.

Kritz, Mark↗

In-Situ Measurements of Cosmogenic Radionuclides on the Surface of Mars

Cosmogenic nuclides are produced by cosmic-ray nuclear interactions with target nuclei in rocks, soils, ice, and the atmosphere. Cosmogenic nuclides have been widely used for investigation of solar system matter for several decades. Stable nuclides, such as He-1, Ne-21, and Ar-38, are built up over time as the surface is exposed to cosmic rays. The concentrations of cosmogenic radionuclides, such as Be-10 (halflife = 1.5 Myr), Al-26 (0.705 Myr), and C-14 (5,730 yr) also build up with exposure time but reach saturation values after several half-lives. Especially after development of accelerator mass spectrometry (AMS), cosmogenic nuclides in terrestrial samples are routinely used for geomorphic studies such as glaciation, surface erosion, and tectonics, and studies of atmospheric and ocean circulation. Cosmogenic nuclides on Mars will be able to answer questions of exposure ages, erosion rates, tectonic events, and deposition rates of sediments and/or volatiles. The concentrations of cosmogenic stable nuclides gives the integrated exposure time of the rock/mineral, and the activities of radionuclides give recent records for times back as long as a few half-lives.

Nishiizumi, K.↗

Compositions and methods for removal of toxic metals and radionuclides

The present invention relates to compositions and methods for the removal of toxic metals or radionuclides from source materials. Toxic metals may be removed from source materials using a clay, such as attapulgite or highly cationic bentonite, and chitin or chitosan. Toxic metals may also be removed using volcanic ash alone or in combination with chitin or chitosan. Radionuclides may be removed using volcanic ash alone or in combination with chitin or chitosan.

Cuero, Raul G.↗

Constraining the Surface Exposure Age of Asteroid Bennu Using Cosmogenic Radionuclides in an OSIRIS-REx Aggregate Sample and Individual Particles

Observations by NASA’s OSIRIS-REx spacecraft of asteroid Bennu revealed evidence that this small rubble-pile asteroid experiences several active surface processes that likely control its recent surface exposure history. In October 2020, the spacecraft collected a surface sample from a relatively young ~20 m diameter crater (Hokioi) on asteroid Bennu, and the sample was successfully delivered to Earth on September 24, 2023. Based on the population of craters >50 m diameter, Bennu’s surface is 0.1–1 Ga old, but the old surface is affected by recent processes including smaller meteoroid impacts, mass movement, and particle ejections. The sampling location within Hokioi crater was selected based on its relatively flat surface devoid of large boulders, but the crater floor is also believed to be one of the youngest surfaces on asteroid Bennu, with an age of <100 kyr. As the crater is ~2 m deep, the samples that were collected by OSIRIS-REx may have been relatively shielded from cosmic rays during most of its recent history. This scenario is different from the samples that were collected by Hayabusa2 from asteroid Ryugu, where cosmogenic noble gas and radionuclides indicate cosmic-ray exposure (CRE) ages of ~5 Myr near the surface. Our goal is to understand the recent exposure history of surface samples of asteroid Bennu utilizing radionuclides ( 10 Be, 26 Al, 36 Cl, 41 Ca) produced by both galactic (GCR) and solar (SCR) cosmic rays. With half- lives ranging from 0.1 to 1.36 million years (Myr), the concentrations of these cosmogenic nuclides provide information on the duration and exposure conditions (irradiation depth) of these samples on a timescale of a few Myr. This work will test one of the OSIRIS-REx mission’s driving hypotheses about asteroid Bennu’s recent evolution: that Hokioi crater is part of a population of small (25 m) spectrally red craters on Bennu that are less than 0.1 Myr old.

K. C. Welten↗

Radionuclide Transport Simulations Supporting Proposed Borehole Waste Disposal in Israel

A scientific collaboration between the U.S. and Israel is underway to assess the suitability of a potential site for subsurface radioactive waste disposal in the Negev Desert, Israel. The Negev Desert has several favorable attributes for geologic disposal, including an arid climate, a deep vadose zone, interlayered low-permeability lithologies, and carbonate rocks with high uranium-sorption potential. These features may provide a robust natural barrier to radionuclide migration. Geologic and laboratory characterization data from the Negev Desert are incorporated into multiphase flow and transport models, solved using PFLOTRAN, to aid in site characterization and risk analysis that will support decision-making for waste disposal in an intermediate-depth borehole design. The lithology with the greatest uranium sorption potential at the site is phosphorite. We use modeling to evaluate the ability of this layer to impact uranium transport around a proposed disposal borehole. The current objective of the simulations is focused on characterizing hypothetical leakage from waste canisters and subsequent uranium migration under three infiltration scenarios. Here, we describe a hydrogeologic model based on data from a local exploratory borehole and present results for uranium flow and transport simulations under varying infiltration scenarios. We find that under the current climate conditions, it is likely that uranium will remain in the near-field of the borehole for thousands of years. However, under a hypothesized extreme climate scenario representing an increase in infiltration by a factor of 300x above present-day values, uranium may break through the phosphorite layer and exit the base of the model domain (~200 m above the water table) within 1000 years. Simulation results have direct implications for the planning of nuclear waste disposal in the Negev Desert, and specifically in intermediate-depth boreholes.

58 GEOSCIENCES↗

Air Quality & Radionuclide Monitoring at the NNSS

Presentation on NNSS environmental compliance work, specifically air quality and radionuclide monitoring in the environment. Presentation to be given at NFO's Tribal Update Meeting April 11, 2023. Presentation is due to DRI on March 28.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗