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Capability to Process and Characterize Uranium-Zirconium (U-Zr) and Uranium-Zirconium-Plutonium (U-Zr-Pu) Alloys

This work investigated co-reduction of anhydrous compounds of uranium, zirconium, and plutonium to produce uranium rich ternary nuclear fuel alloys. Metallothermic co-reduction is a novel method to produce all-metal nuclear fuels. Metal fuels offer thermal, fissility, compatibility, and security benefits over oxide fuels. Alloys of uranium–10% zirconium with plutonium contents of 0%, 2.5%, 5%, and 10% were produced, with yields of 60–85% of theoretical values in a traditional calciothermic bomb reduction apparatus. Microstructural analysis indicated transformation of uranium phase from gamma to beta and then alpha, in alternating lamellar plates typical of alpha phase uranium and delta phase uranium-zirconium, with zirconium and carbides at prior grain boundaries. Some of the analyses were inconclusive in their results and therefore require additional testing. Successful ternary co-reduction would simplify production of homogeneous feedstock and thereby streamline manufacture of homogeneous ternary metallic fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Assembly of MiniFuel Targets for Irradiation of U-Mo Fuel Specimens in the High Flux Isotope Reactor

To support the development of advanced low-enriched uranium for use in nuclear reactors, irradiation testing of U-Mo disk specimens was performed at the Oak Ridge National Laboratory (ORNL) High Flux Isotope Reactor (HFIR) to collect experimental irradiation data on this type of fuel at pressurized water reactor–relevant temperatures. U-Mo is a uranium alloy that has superior dimensional stability relative to alpha-phase uranium metal and has a substantially higher uranium density compared to UO 2 . U-Mo disks specimens were fabricated at Idaho National Laboratory and inserted into MiniFuel targets for HFIR irradiation. Three MiniFuel targets were successfully assembled, welded, tested, and delivered to HFIR, along with their quality assurance documentation. The targets were inserted into HFIR’s inner vertical experiment facility within the permanent beryllium reflector. Each target contains six disk specimens and will be irradiated in HFIR for three, four, and eight cycles, with target temperatures between 250 and 500°C. This report summarizes the experiment design, test matrix, pre-characterization of specimens, and experiment assembly.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Evolution of dislocation loops in irradiated α-Uranium: An atomistically-informed cluster dynamics investigation

An atomistically-informed mean field cluster dynamics model has been developed to investigate the nucleation and growth of prismatic loops in irradiated a-Uranium. TEM analysis of neutron irradiated a-Uranium shows the evolution of self-interstitial atom and vacancy loops on (010) and (100) crystallographic planes, respectively, resulting in an anisotropic lattice swelling of its face-centered orthorhombic crystal. To provide model parameters, the crystallography of loops and the binding energy of point defects to these loops were studied using an angular dependent EAM potential and classical molecular dynamics (MD) simulations. Furthermore, using the bond-boost hyperdynamics method, the anisotropic diffusion of interstitials and vacancies in a-Uranium was investigated. Here, the mechanisms of point defect diffusion and the associated migration energies were reported and compared with previous DFT studies. The energetics and kinetic quantities mentioned above were used in the cluster dynamics model to predict the cluster density as a function of dose rate, dose and temperature and the results were compared to the reported neutron irradiation experiments. The model predictions reveal an accumulation of small sized vacancy loops along with a population of large and growing self-interstitial loops, which closely corresponds to the TEM observations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Determination of Thermal Expansion, Defect Formation Energy, and Defect-Induced Strain of α-U Via ab Initio Molecular Dynamics

Uranium (U) is often alloyed with molybdenum (Mo) or zirconium (Zr) in order to stabilize its high-temperature body-centered cubic phase for use in nuclear reactors. However, in all metallic fuel forms, the α phase of U remains in some fraction. This phase decomposition due to temperature or compositional variance can play an outsized role on fuel performance and microstructural evolution. Relatively little is known about fundamental point defect properties in α -U at non-zero temperatures, from either computational or experimental studies. This work performs the first thorough evaluation of the α phase of U via ab initio molecular dynamics (AIMD). A number of thermophysical properties are calculated as a function of temperature, including equilibrium lattice parameters, thermal expansion, and heat capacity. These results indicate a two-region behavior, with the transition at 400 K. The thermal expansion/contraction in the a / b direction occurs rapidly from 100 up to 400 K, after which a more linear and gradual change in the lattice constant takes place. The volumetric expansion matches experiments quantitatively, but the individual lattice constant expansion only matches experiments qualitatively. Point defect formation energies and induced lattice strains are also determined as a function of temperature, providing insight on defect populations and the fundamentals of irradiation growth in α -U. Interstitials induce significantly more strain than vacancies, and the nature of that strain is highly dependent on the individual lattice directions. The direction of point defect-induced lattice strain is contrary to the irradiation growth behavior of α -U. This work shows that isolated point defects cannot be the primary driving force responsible for the significant irradiation-induced growth of α -U observed experimentally.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Thermal conductivity of α -U with point defects

Here, we develop a theoretical model for thermal conductivity of α-U that combines density functional theory calculations and the coupled electron–phonon Boltzmann transport equation. The model incorporates both electron and phonon contributions to thermal conductivity and achieves good agreement with experimental data over a wide temperature range. The dominant scattering mechanism governing thermal transport in α-U at different temperatures is examined. By including phonon–defect and electron–defect scatterings in the model, we study the effect of point defects including U-vacancy, U-interstitial, and Zr-substitution on the thermal conductivity of α-U. The degradation of anisotropic thermal conductivity due to point defects as a function of defect concentration, defect type, and temperature is reported. This model provides insights into the impact of defects on both phonon and electron thermal transport. It will promote the fundamental understanding of thermal transport in α-U and provide a ground for investigation of coupled electron–phonon transport in metallic materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Groundwater Monitoring Report, U.S. Department of Energy Y-12 National Security Complex, Oak Ridge, Tennessee

This report contains the groundwater and surface water monitoring data obtained during calendar year (CY) 2019 at the U.S. Department of Energy (DOE) Y-12 National Security Complex (Y-12) on the DOE Oak Ridge Reservation (ORR) in Oak Ridge, Tennessee. The monitoring data were obtained from wells, springs, and surface water sampling locations in three hydrogeologic regimes at Y-12. The Bear Creek Hydrogeologic Regime (Bear Creek Regime) encompasses a section of Bear Creek Valley (BCV) between the west end of Y-12 and the west end of the Bear Creek Watershed (directions are in reference to the Y-12 grid system, shown as Plant North. The Upper East Fork Poplar Creek Hydrogeologic Regime (East Fork Regime) encompasses the Y-12 industrial facilities and support structures in BCV. The Chestnut Ridge Hydrogeologic Regime (Chestnut Ridge Regime) encompasses a section of Chestnut Ridge directly south of Y-12. Background information in Section 2 of this report outlines the hydrogeologic framework for groundwater and surface water quality monitoring at Y-12 and includes an overview of the groundwater contamination in each hydrogeologic regime. Section 3 provides details regarding the groundwater and surface water sampling and analysis activities implemented under the Y-12 GWPP, including sampling locations and frequency, sample collection and handling, field measurements and laboratory analytes, quality assurance (QA)/quality control (QC) sampling, data management, and data quality assessment (DQA). However, the equivalent QA/QC or DQA information for the groundwater and surface water data associated with the monitoring programs implemented by UCOR are not included in this report and instead are deferred to referenced programmatic plans and reports issued by OREM and UCOR. Section 4 of this report presents a summary evaluation of the CY 2019 monitoring data with regard to the respective objectives of surveillance monitoring and exit pathway/perimeter monitoring. The evaluation is based primarily on the analytical results for the following principal groundwater contaminants at Y-12: nitrate, uranium, gross alpha activity, gross beta activity, and volatile organic compounds (VOCs). Section 5 summarizes the most significant findings with respect to the principal contaminants along with recommendations for any proposed changes to the ongoing groundwater and surface water quality monitoring performed under the Y-12 GWPP. Technical reports and plans cited in the narrative sections of the report are listed in Section 6. Narrative sections of this report reference several appendices. Figures (maps and diagrams) and data tables (excluding data summary tables incorporated in the narrative sections) are in Appendix A and Appendix B, respectively. Appendix C contains construction details for each well sampled during CY 2019 by either the Y-12 GWPP or UCOR, along with schematic diagrams for wells equipped with Westbay™ multiport sampling equipment or Barcad® pump systems. Appendix D supports the background summary discussion in Section 2 and provides more detailed information about the hydrogeologic framework for groundwater and surface water monitoring at Y-12, including the primary sources of groundwater contamination in each hydrogeologic regime. Results for all field measurements and laboratory analyses obtained by the Y-12 GWPP and UCOR are presented in Appendix E, which also includes the sample numbers for the QA/QC samples associated with groundwater and surface water monitoring performed by the Y-12 GWPP.

54 ENVIRONMENTAL SCIENCES↗

20A44-121: Modeling and characterization of α-U to accelerate metallic fuels development [Slides]

This presentation contains a high-level description of the Idaho National Laboratory Laboratory Directed Research and Development (LDRD) project, 20A44-121: Modeling and characterization of α-U to accelerate metallic fuels development. It frames the problem, describes a motivation, outlines the research plan involving multiscale modeling and experiments, discusses impact and details research developments.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Application of the Cohn-alpha Method on Bare Highly Enriched Uranium Using Organic Scintillators [Poster]

The prompt neutron decay constant (α), can be used to calculate the lifetime of prompt fission chains within a multiplying system and verify reactor startup and shutdown. We analyze a fast, bare system consisting of highly enriched uranium (93% 235 U) hemisphere shells known as the Measurements of Uranium Subcritical and Critical (MUSiC). We measured the system with a three by-four array of organic scintillators (OSCAR) to obtain the gamma-ray and fast neutron signals. Pulse shape discrimination was used to isolate the neutron time series data. The Cohn-α method was used to estimate α for 3 supercritical measurements of Configurations 8 MUSiC. We use these estimates to linearly extrapolate α at delayed critical. These values can be compared to highly detailed simulations in MCNP6.2.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radionuclide Screening Analysis and Transport Parameters for Pahute Mesa Detonations, Nevada National Security Site

A “screening analysis” is implemented at Pahute Mesa (PM), Nevada National Security Site (NNSS), to determine subsets of the 43 radionuclides listed in the radionuclide inventory of Finnegan et al. (2016) that are of relevance or potential relevance to the hydrologic source term (HST) for assessment of radionuclide transport in groundwater. Consideration is added to how levels of contamination are defined and whether any other radionuclides not in the inventory are relevant to the HST. A model is developed to estimate a range of possible source concentrations in groundwater that account for uncertainty in partitioning into melt glass and sorption into surrounding rock of the exchange zone for the 82 PM underground nuclear tests detonated in vertical shafts. The model also accounts for the varied hydrogeochemical settings. Transport parameters needed for the screening model calculations are developed from databases for hydrogeologic units, chemistry, mineralogy, fracture spacing, fracture aperture, fracture openness, matrix porosity, bulk density, saturation, and alteration. Of key importance is consideration of diagenetic zonation of the mineralogy related to hydrothermal alteration. The screening analysis compares model results with available groundwater radiochemistry data. Consistency between screening model results and available data helps validate the model for application to all 43 radionuclides, most of which have no measurements or only non-detect measurements of concentration in groundwater. The screening analysis determines that ten radionuclides – tritium, Sr-90, I-129, Cs-137, U-232, U-233, U-234, U-238, and the total of Pu-239 and Pu-240 are relevant to the HST. Determination of relevance is primarily based on data and/or model results indicating source concentration exceeding a maximum contaminant level (MCL) out to 100 years since the time of detonation. U-238 is relevant to assessment of contamination relative to MCLs for uranium and gross alpha particle activity. Five other radionuclides – C-14, Cl-36, Tc-99, Np-237, and Pu-238 – are determined potentially relevant to the HST based on a 0.1 MCL threshold. The screening analysis recommends additional attention to the natural daughter radionuclides of the uranium series (U-238) and thorium series (Th-232) decay chains, particularly Ra-226 and Ra-228, that were not included the inventory.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Quantum enabled precision measurements of the 229Th nuclear isomer transition (final report)

The existence of the nuclear isomer transition in thorium-229 was first inferred from keV lines in the gamma spectrum of uranium-233 decay more than 40 years ago. Over the years, the value of the transition energy has been refined with indirect measurements using nuclear physics techniques, and the current evidence points to transition energy in the laser-accessible vacuum ultra-violet region of the spectrum. At the start of this project, the two best measurements of the transition energy were 7.8±0.5 eV and 8.28±0.17 eV from high precision gamma ray spectroscopy and kinetic energy of internal conversion electrons, respectively. This project aimed to reduce the uncertainty in the transition energy to 10 meV using direct calorimetric measurements of the decay energy with superconducting nanowire single photon detectors (SNSPDs). Specifically, the method that was pursued was to generate thorium-229 in the excited isomer state by the alpha decay of uranium-233, embed the excited state thorium into an SNSPD, then detect the energy released when the isomer deexcites.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Examination of Digital-Delay Rossi-$\alpha$ for 252 Cf-Driven Highly Enriched Uranium Using Organic Scintillators

Neutron noise techniques constitute several analysis methods applicable to non-destructive assay. One technique is the Rossi-α method to calculate the prompt neutron decay constant (α) or its inverse, the prompt neutron period (1/α), for assemblies of fissionable material. This work evaluates a high-data-throughput measurement at the National Criticality Experiments Research Center (NCERC) with organic scintillators measuring a subcritical assembly of highly enriched uranium (HEU) metal (93% 235 U). The assembly comprises hemi shells stacked together to form fully closed shells and is driven by a Cf source at the center. The assembly is a total of 59.85 kg HEU and a k eff of 0.99, according to MCNP6.2 KCODE simulations. Measurements were acquired with a three-by-four array of 5.08-cm-diameter by 5.08-cm-length trans-stilbene crystals 166 cm from the assembly center. Two types of coincident binning methods are used to build the Rossi-α distribution of coincident neutron detections: A) type 1 binning, also known as any-and-all forward time differences, and B) type 1 binning with a digital-delay technique that is analogous to Orndoff’s use of delay cabling in early Rossi-alpha measurements. Method B) disregards same-detector coincidences and once all nearest time coincidences are collected between all detectors after a trigger, a time delay of 0.75 µs is implemented. The measured prompt neutron decay constants for both techniques are calculated from single exponential fits and the two methods are compared. Method A) shows an apparent timing discontinuity near 500 ns time differences. This timing discontinuity interferes with the fitting method used to calculate the prompt neutron decay constant. Method B) mitigates the artificial timing discontinuity and removes the disagreement of the fit. Future work will model the time-dependent detector response to discern why this timing discontinuity occurs, discern how Method B) reduces the amplitude of this timing discontinuity, and apply this method to critical assembly measurements to ultimately confirm the recommendation to use Method B) for high-data-throughput measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

In vitro toxicity assessment of uranium particulates on different human lung epithelial cell models

Inhalation of uranium aerosols produced via human activities such as mining can pose a threat to human respiratory systems. Uranium oxide particulates emit short-range alpha particles that elicit DNA and direct damage, beyond associated physiochemical heavy-metal toxicity, to internal epithelial tissues. The availability of reliable in vitro models to study radiation exposure can greatly enhance our ability to understand and combat the biological impacts of exposure. However, the toxicological effects of alpha emissions and/or the oxidation states of uranium particulates vary across different human lung epithelial cell models and have not been systematically compared. We have endeavored to address this limitation by comparing impacts in three different human lung cell models: primary human bronchial and tracheal epithelial cells, primary human small airway epithelial cells, and human adenocarcinoma alveolar basal epithelial cells. Other studies have mainly investigated the toxicity of depleted uranium. Here, we compared the exposure of uranium oxide particulates (U 3 O 8 and UO 3 ) of different enrichment states on the chosen cell systems. Each cell model was exposed to 0.1, 1, 10, 50, 100, and 500 µg/mL of depleted U 3 O 8 , highly-enriched U 3 O 8 , and natural UO 3 particulates for 24 hours in submerged monolayer cultures. We compared viability and superoxide dismutase activity results across cell lines and uranium enrichment/ oxidative states. The results showed that 1) the oxide state of the particulates affected cell viability, implying that uranium’s different oxidation states contribute to different toxicological responses, and 2) each cell model reacts differently when exposed to uranium oxides, which may provide insights into the mechanistic processes associated with the exposure of radiological particulates on different biological systems. For instance, increased uranium enrichment corresponds to increased toxicity for the primary cells, but not for the immortalized cells. Our study shows that a holistic approach that incorporates similarities between model systems and types of radionuclides is required to truly develop empirical solutions for radiation exposure.

59 BASIC BIOLOGICAL SCIENCES↗

Rossi-alpha Analysis of CURIE Experiment [Slides]

Critical assembly measurement and operations are crucial to the development of benchmark data. Knowledge of the prompt neutron lifetime informs on the state of the system’s neutron spectrum. Rossi-alpha analysis can give us time-dependent information on the system. Teflon was selected, via genetic algorithm, as a moderator to target the URR in uranium for CURIE. Rossi-alpha measurements of the assembly's approach to critical using He-3 detectors estimated the prompt neutron decay constant (α) at delayed critical. α values of several subcritical measurements were then used to predict the α value at delayed critical.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Improvement of mechanistic fuel-cladding chemical interaction modeling in BISON

This report describes work performed during FY2024 under the auspices of the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program to inform and improve mechanistic models of fuel-cladding chemical interaction (FCCI) in metallic fuel. For fuel-side FCCI, atomistic simulations were performed to determine the diffusivity of iron (Fe) in the $\alpha$ and $\gamma$ phases of uranium (U). A model of liquid penetration of cladding due to melting of the fuel-side FCCI region was updated to account for the finite size of the FCCI region, and the model was validated through comparison with tests performed in the Fuel Behavior Test Apparatus (FBTA). For cladding wastage formation, a reduced-order model was improved by comparison with a multi-scale mechanistic model to better quantify the ROM parameters.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Corrosion of U233-Doped Uranium Oxide using Microfluidics Methods

The aim of work this year has been to investigate the role of alpha (α)-radiation and hydrogen (H 2 ) on the corrosion of uranium oxide (UO 2 ) using a microfluidic device. The microfluidic device, termed the Particle-Attached Microfluidic Electrochemical Cell, (PAMEC), enables monitoring of the UO 2 electrochemical corrosion potential (E corr ) under different environments, including de-aerated conditions and in the presence of dissolved H 2 . The Si 3 N 4 window allows us to study morphological and chemical changes under an electron microscope. We have previously demonstrated that the PAMEC matches the results from bulk electrochemical tests with UO 2 [1]. We used the high specific activity uranium (U) isotope, 233 U, (t 1/2 = 160,000 years) incorporated into UO 2 , to generate a localized a-field. The objective of the experiments were to mimic the radiation environment that would be experience at the surface of aged spent nuclear fuel (SNF) during long-term geologic disposal under anoxic conditions. Wittman et al. [2] predicted that in the presence of a pure a-radiation field and under H 2 conditions, the concentration of the radiolytic oxidant H 2 O 2 would be suppressed or even eliminated. In a UO 2 corrosion experiment this would be exhibited through a lowering of the measured UO 2 corrosion potential compared to identical conditions in the absence of dissolved H 2 . We found that the predictions of Wittman and co-workers were supported and that the corrosion potential of the 233 U-doped UO 2 in solution lowered with presence of H 2 gas and increased in the absence of H 2 , when under anoxic conditions. The PAMEC experiments indicate that H 2 O 2 has been eliminated in a solution sparged with H 2 while exposed to an a-radiation field. The corrosion potential of the a-doped 233 U(10%)- 238 UO 2 in a solution sparged with Ar/H 2 matched the corrosion potential of 238 UO 2 in solution sparged with air. This clearly demonstrated that the H 2 O 2 had been eliminated and that the only oxidant present was O 2 in this system in complete agreement with the modeling results of Wittman et al. These results point to the need to improve the Fuel Matrix Degradation (FMD) Process Model training data set that is being used in the FMD surrogate model that is being developed for the repository program. The incorporation of realistic radiation chemistry will improve the scientific basis for the FMD Model.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

In-Field Alpha Spectrometer Development FY2022 Mid-Year Report

In response to needs identified by the International Atomic Energy Agency (IAEA), Idaho National Laboratory (INL) has developed an In-Field Alpha Spectrometer (IFAS) to allow IAEA safeguards inspectors to collect samples of uranium hexafluoride (UF 6 ) at processing facilities, to perform field assessments to verify uranium enrichment. For sample collection, the IFAS method uses Single-Use Destructive Assay (SUDA) samplers, developed at Pacific Northwest National Laboratory (PNNL), which contain thin zeolite coatings that trap UF6 gas and convert it to the safer, more stable form uranyl fluoride (as a dihydrate, UO 2 F 2 ·2H 2 O). For alpha spectrometry, the IFAS instrument employs a large area silicon semiconductor transducer to detect and record alpha particle energy-deposition events. Over the course of this project INL, PNNL, Oak Ridge National Laboratory worked to optimize the SUDA sample design for alpha spectrometry, to optimize processes for manufacturing, loading, and shipping SUDA samples, and to allow the measurement of loaded SUDA samples. In fiscal year (FY) 2022 INL has bene investigating the reproducibility and measurement precision of IFAS measurements and the associated determination of uranium enrichment.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Mortality among Tennessee Eastman Corporation (TEC) uranium processing workers, 1943–2019

Background: There are few occupational studies of women exposed to ionizing radiation. During World War II, the Tennessee Eastman Corporation (TEC) operated an electromagnetic field separation facility of 1152 calutrons to obtain enriched uranium (235U) used for the Hiroshima atomic bomb. Thousands of women were involved in these operations. Materials and methods: We report a new study was conducted of 13,951 women and 12,699 men employed at TEC between 1943 and 1947 for at least 90 days. Comprehensive dose reconstruction techniques were used to estimate lung doses from the inhalation of uranium dust based on airborne measurements. Vital status through 2018/2019 was obtained from the National Death Index, Social Security Death Index, Tennessee death records and online public record databases. Analyses included standardized mortality ratios (SMRs) and Cox proportional hazards models. Results: Most workers were hourly (77.7%), white (95.6%), born before 1920 (58.3%), worked in dusty environments (57.0%), and had died (94.9%). Vital status was confirmed for 97.4% of the workers. Women were younger than men when first employed: mean ages 25.0 years and 33.0 years, respectively. The estimated mean absorbed dose to the lung was 32.7 mGy (max 1048 mGy) for women and 18.9 mGy (max 501 mGy) for men. The mean dose to thoracic lymph nodes (TLNs) was 127 mGy. Statistically significant SMRs were observed for lung cancer (SMR 1.25; 95% CI 1.19, 1.31; n = 1654), nonmalignant respiratory diseases (NMRDs) (1.23; 95% CI 1.19, 1.28; n = 2585), and cerebrovascular disease (CeVD) (1.13; 95% CI 1.08, 1.18; n = 1945). For lung cancer, the excess relative rate (ERR) at 100 mGy (95% CI) was 0.01 (–0.10, 0.12; n = 652) among women, and –0.15 (–0.38, 0.07; n = 1002) among men based on a preferred model for men with lung doses <300 mGy. NMRD and non-Hodgkin lymphoma were not associated with estimated absorbed dose to the lung or TLN. Conclusions: There was little evidence that radiation increased the risk of lung cancer, suggesting that inhalation of uranium dust and the associated high-LET alpha particle exposure to lung tissue experienced over a few years is less effective in causing lung cancer than other types of exposures. There was no statistically significant difference in the lung cancer risk estimates between men and women. The elevation of certain causes of death such as CeVD is unexplained and will require additional scrutiny of workplace or lifestyle factors given that radiation is an unlikely contributor since only the lung and lymph nodes received appreciable dose.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

A Rapid Sequential Separation Method for Determination of Actinides and TENORM in Fracking Wastes - 20223

With recent advances in unconventional drilling technology in the US and around the world, the risks of environmental contamination and exposure due to technologically enhanced naturally occurring radioactive materials (TENORM) from fracking wastes have also surfaced. Although the Permian Basin (southeastern New Mexico, western Texas) has long been a modest producer of oil, the advent of fracking technology a decade ago turned it into hot property for producers. A 2018 assessment of undiscovered, technically recoverable continuous oil and gas resources by the U.S. Geological Survey estimates an average 46.3 billion barrels of oil and 281 trillion cubic feet of gas. This is likely to increase the use of unconventional drilling and TENORM generation. TENORM concentrations in oil and gas exploration and production waste can be several hundred to several thousand times higher than background TENORM concentrations. Both the thorium and uranium decay chains contribute to airborne radionuclides arising from the radon gas escaping the ground and subsequently decaying as airborne particulates. Additionally, radon decay products {sup 210}Pb and {sup 210}Po can build up in scale on the internal surfaces of oil and gas handling pipes and in sludge in refineries, becoming potential inhalation and ingestion hazards for workers. Furthermore, southeastern NM is also home to world's only licensed and operating transuranic nuclear waste repository, the DoE's Waste Isolation Pilot Plant (WIPP). Plutonium isotopes ({sup 239+240}Pu) and {sup 241}Am, are expected to account for more than 99% of the total radioactivity scheduled for disposal in the WIPP repository. Thus, an improved understanding of the environmental fate and transport of TENORM, liberated by unconventional drilling, is essential to assess how best to protect individuals and the environment. In this context, accurate measurement of TENORM and actinides in environmental and biological samples is essential. In this presentation, a new sequential method for the separation and pre-concentration of actinides (Pu, Am, Np) and TENORM (Po, U and Th) derived from oil and gas exploration is proposed. The TEVA method involves a rapid co-precipitation step to remove matrix interferences from the samples, followed by plutonium oxidation state adjustment to Pu (IV) and an incubation period of ∼ 1 hour at 50-60 deg. C to allow the resultant Po (II) to oxidize into Po(IV). The polonium, neptunium, thorium and plutonium are then separated on a TEVA column, while americium and uranium are separated on a TRU column. After separation, the alpha counting source was prepared by micro-precipitation with copper sulfide (CuS) for polonium and neodymium fluoride (NdF{sub 3}) for actinides. The efficiency and reliability of the procedures were tested by analyzing filter, drinking water and frack sand samples. The method is simple, robust and can be performed quickly with excellent removal of interferences, high chemical recovery and very good alpha peak resolution. (authors)

07 ISOTOPE AND RADIATION SOURCES↗