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At least 343 records · Page 19

Environmental Protection Agency Drinking Water Protective Action Guides Implementation Recommendations

This report documents the analysis conducted by Sandia National Laboratories on the effect of various alterations to published methodologies to calculate Derived Response Levels for Environmental Protection Agency Drinking Water Protective Action Guides. Specifically, this study sought to assess and provide recommendations on calculation of the Derived Response Level accounting for decay during the consumption period, assess the impact of decay on laboratory Minimal Detectable Concentration in water samples as compared to the Derived Response Level, make a recommendation on the calculation of Derived Response Level consistent with existing Public Protection Methods, and make a recommendation on the use of six age groups versus eight age groups based on available dose coefficients for calculation of the Derived Response Level. The authors analyzed these various factors using nominal radionuclide mixes from four scenarios and compared calculation of the Derived Response Level accounting for decay and no decay and then compared those results to the laboratory Minimal Detectable Concentrations. The authors concluded that decay should be included in the calculation of the Derived Response Level, existing Public Protection Methods should be employed to calculate the Derived Response Level, six age groups should be used versus eight, and the use of both decay and Public Protection Methods result in little to no concern for water samples meeting the Minimum Detectable Concentration requirements. The results of this study may be used in further developing and implementing a method for the Environmental Protection Agency Water Derived Response Level calculation in the Federal Radiological Monitoring and Assessment Center Assessment Manual.

54 ENVIRONMENTAL SCIENCES↗

Evaluating county-level lung cancer incidence from environmental radiation exposure, PM 2.5 , and other exposures with regression and machine learning models

Characterizing the interplay between exposures shaping the human exposome is vital for uncovering the etiology of complex diseases. For example, cancer risk is modified by a range of multifactorial external environmental exposures. Environmental, socioeconomic, and lifestyle factors all shape lung cancer risk. However, epidemiological studies of radon aimed at identifying populations at high risk for lung cancer often fail to consider multiple exposures simultaneously. For example, moderating factors, such as PM 2.5 , may affect the transport of radon progeny to lung tissue. This ecological analysis leveraged a population-level dataset from the National Cancer Institute’s Surveillance, Epidemiology, and End-Results data (2013–17) to simultaneously investigate the effect of multiple sources of low-dose radiation (gross γ activity and indoor radon) and PM 2.5 on lung cancer incidence rates in the USA. County-level factors (environmental, sociodemographic, lifestyle) were controlled for, and Poisson regression and random forest models were used to assess the association between radon exposure and lung and bronchus cancer incidence rates. Tree-based machine learning (ML) method perform better than traditional regression: Poisson regression: 6.29/7.13 (mean absolute percentage error, MAPE), 12.70/12.77 (root mean square error, RMSE); Poisson random forest regression: 1.22/1.16 (MAPE), 8.01/8.15 (RMSE). The effect of PM 2.5 increased with the concentration of environmental radon, thereby confirming findings from previous studies that investigated the possible synergistic effect of radon and PM 2.5 on health outcomes. In summary, the results demonstrated (1) a need to consider multiple environmental exposures when assessing radon exposure’s association with lung cancer risk, thereby highlighting (1) the importance of an exposomics framework and (2) that employing ML models may capture the complex interplay between environmental exposures and health, as in the case of indoor radon exposure and lung cancer incidence.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Comparison of mercury (Hg) bioaccumulation with mono- and mixed Lemna minor and Spirodela polyrhiza cultures

Mercury (Hg) is a prevalent and harmful contaminant that persists in the environment. For phytoremediation, it is important to discover which plants can bioaccumulate meaningful amounts of Hg while also tolerating its toxicity. Additionally, increasing biodiversity could create a more resilient and self-sustaining system for remediation. This study explores whether mixed populations of Lemna minor and Spirodela polyrhiza can better bioaccumulate and tolerate Hg than monocultures. Mono- and mixed cultures of L. minor and S. polyrhiza were grown in mesocosms of 0.5 μg/L or 100 μg/L Hg ( HgCl2) spiked water for 96 h. Change in weight of duckweed was used to assess Hg tolerance. Diffusive gradients in thin-films (DGTs) were used as surrogate monitoring devices for bioavailable levels of Hg. For biomass growth, the mixed culture of the L. minor was greater than the monoculture at the high dose. The L. minor accumulated more Hg in the mixed culture at the low dose while the S. polyrhiza was higher in the mixed at the high dose. Hg speciation in water was modeled using Windermere Humic Aqueous Model 7 (WHAM7) to compare the bioavailable species indicated by the DGTs. Potentially due to the controlled conditions, the WHAM7 output of bioavailable Hg was almost 1:1 to that estimated by the DGTs, indicating good predictive capability of geochemical modeling and passive sampler DGT on metal bioavailability. Altogether, the mixed cultures statistically performed as well as or better than the monocultures when tolerating and bioaccumulating Hg. However, there needs to be further work to see if the significant differences translate into practical differences worth the extra resources to maintain multiple species.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

The contribution of the neuroendocrine system to adaption after repeated daily ozone exposure in rats

Ozone-induced lung injury/inflammation dissipates despite continued exposure for 3 or more days; however, the mechanisms of adaptation/habituation remain unclear. Since ozone effects are mediated through adrenal-derived stress hormones, which also regulate longevity of centrally-mediated stress response, we hypothesized that ozone-adaptation is linked to diminution of neuroendocrine stress-axes activation and glucocorticoid levels. Male Wistar-Kyoto-rats (12-week-old) were injected with vehicle or a therapeutically-relevant dexamethasone dose (0.01-mg/kg/day; intraperitoneal) for 1-month to determine if suppression of glucocorticoid signaling was linked to adaptation. Vehicle- and dexamethasone-treated rats were exposed to air or 0.8-ppm ozone, 4 h/day × 2 or 4 days to assess the impacts of acute exposure and adaptation, respectively. Dexamethasone reduced thymus and spleen weights, circulating lymphocytes, corticosterone and increased insulin. Ozone increased lavage-fluid protein and neutrophils and decreased circulating lymphocytes at day-2 but not day-4. Ozone-induced hyperglycemia, glucose intolerance and inhibition of beta-cell insulin release occurred at day-1 but not day-3. Ozone depleted circulating prolactin, thyroid-stimulating hormone, and luteinizing-hormone at day-2 but not day-4, suggesting central mediation of adaptation. Adrenal epinephrine biosynthesis gene, Pnmt, was up-regulated after ozone exposure at both timepoints. However, genes involved in glucocorticoid biosynthesis were up-regulated after day-2 but not day-4, suggesting that acute 1- or 2-day ozone-mediated glucocorticoid increase elicits feedback inhibition to dampen hypothalamic stimulation of ACTH release in response to repeated subsequent ozone exposures. Although dexamethasone pretreatment affected circulating insulin, lymphocytes and adrenal genes, it had modest effect on ozone adaptation. In conclusion, ozone adaptation likely involves lack of hypothalamic response due to reduced availability of circulating glucocorticoids.

60 APPLIED LIFE SCIENCES↗

Exposure to an environmental mixture of polycyclic aromatic hydrocarbons induces hepatic cytochrome P450 enzymes in mice

Cytochrome P450 enzymes (CYPs) play an important role in bioactivating or detoxifying polycyclic aromatic hydrocarbons (PAHs), common environmental contaminants. While it is widely accepted that exposure to PAHs induces CYPs, effectively increasing rates of xenobiotic metabolism, dose- and time-response patterns of CYP induction are not well known. In order to better understand dose- and time-response relationships of individual CYPs following induction, we exposed B6129SF1/J mice to single or repeated doses (2-180 µmol/kg/d) of benzo[a]pyrene (BaP) or Supermix-10, a mixture of the top 10 most abundant PAHs found at the Portland Harbor Superfund Site. In hepatic microsomes from exposed mice, we measured amounts of active CYPs using activity-based protein profiling and total CYP expression using global proteomics. We observed rapid Cyp1a1 induction after 6 hr at the lowest PAH exposures and broad induction of many CYPs after 3 daily PAH doses at 72 hr following the first dose. Using samples displaying Cyp1a1 induction, we observed significantly higher metabolic affinity for BaP metabolism (Km reduced 3-fold), 3-fold higher intrinsic clearance, but no changes to the Vmax. Mice dosed with the highest PAH exposures exhibited 1.7 to 5-fold higher intrinsic clearance rates for BaP compared to controls and higher Vmax values indicating greater amounts of enzymes capable of metabolizing BaP. This study demonstrates exposure to PAHs found at Superfund Sites induces enzymes in dose- and time-dependent patterns in mice. Accounting for specific changes in enzyme profiles, and relative rates of PAH bioactivation and detoxification, and resulting risk will help translate internal dosimetry of animal models to humans and improve risk assessments of PAHs at Superfund sites.

Stoddard, Ethan G.↗

Concept of Operations for Advanced Reactor Spent Nuclear Fuel Management

This presentation presents a preliminary description of a concept of operations to incorporate advanced-reactor spent nuclear fuel (SNF) into an integrated waste-management system (IWMS). The evaluation includes SNF from four advanced-reactor concepts with the following fuel types: (1) small modular reactors using oxide fuels, (2) tristructural-isotropic (TRISO) fuels, (3) metallic fuels, and (4) fuel salts. To provide context for the proposed concept of operations for advanced reactors, a comparison is made with traditional light-water reactors (LWRs) to identify potential gaps in the IWMS. The technical differences between advanced reactors and LWRs are assessed to determine the feasibility of managing advanced-reactor waste streams using existing operations and technology. This presentation emphasizes fuel types from Advanced Reactor Demonstration Program reactors: Xe 100, which uses TRISO fuel and Natrium, with its metallic fuels while also analyzing management options for molten-salt reactors and advanced light-water reactors (ALWRs). Understanding the storage, transportation, and disposal requirements of SNF is dependent on both the quantity and characteristics of the SNF generated by nuclear reactors. This presentation provides a high level overview, comparing the anticipated concept of operations for different SNFs from advanced reactors. The IWMS includes at-reactor storage, transportation, potential off-site storage, potential treatment, and disposition. To assess the potential effect of advanced-reactor concept of operations on the IWMS, estimates were made for fuel characteristics that contribute to storage, transportation, disposal, and possible treatment of advanced-reactor SNF. These include canister heat load, dose rates, and criticality-control limits, which are important for determining the condition and configuration of the advanced reactor SNF. At-reactor storage of LWR SNF traditionally involves a spent-fuel pool (SFP) before transfer to an independent spent-fuel storage installation. However, some advanced-reactor concepts, particularly those using TRISO and salt fuels, do not anticipate the use of an SFP. This difference in at-reactor storage could impact the IWMS. Additionally, transportation of advanced-reactor SNF may include additional processes tied to potential off gassing, and transportation of microreactor SNF may occur within the reactor vessel. Some advanced-reactor SNF could also undergo treatment to meet requirements of an acceptable waste form for disposition, and the treatment location will be a major contributor to efficiently performing IWMS responsibilities. Moreover, the quantity of SNF generated is an important consideration for IWMS because it could affect the size of the transportation fleet and potential off-site storage requirements. Additionally, volume and heat load are the primary drivers for SNF disposition. This presentation compares potential packaging options for advanced reactor SNF with traditional LWR packaging to provide a high-level comparison for the needs of the IWMS for advanced-reactor SNF.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Health Hazards of Exposures to Radioiodine

Iodine is a chemical element with atomic number 53. Iodine-127 is stable (non-radioactive) and commonly found in nature. Elemental iodine is a purple-colored solid at room temperature and pressure, but spontaneously sublimates (turns into vapor). Iodine is an essential element for life, and is required for proper functioning of the thyroid. Iodine is present in many foods, and is readily absorbed by the body and concentrated in the thyroid gland. A fraction of iodine ingested or inhaled is rapidly removed by the kidneys. The rest of the inhaled or ingested iodine is absorbed the by thyroid and retained for many months. Iodine has a biological half-life of approximately 120 days in health individuals. The biological half-life can be shorter in individuals with hyperthyroidism, and longer in individuals with hypothyroidism. Iodine has a number of radioactive isotopes, most of which have relatively short half-lives (days or weeks). Short half-life iodine isotopes are useful for a variety of medical applications, including imaging and cancer therapy. For example, Iodine-123 (half-life 13 hours) is commonly used for medical imaging of the thyroid, while iodine-131 (half-life 8 days) is used for suppressing thyroid function in individuals with hyperthyroidism or ablating (killing) thyroid cells to treat thyroid cancer. Iodine-125 (half-life 59 days) is produced in nuclear reactors, and has medical uses. Although iodine-125 can be used for thyroid imaging, Iodine-123 is more commonly used for that purpose because of its shorter half-life and higher-energy emissions. Iodine-125 is more commonly used for cancer treatment, and can be processed into small metal pellets (seeds) inserted directly into a tumor. Iodine-125 emits low-energy x-rays which can kill tumor cells and generally cannot escape the tumor, sparing other tissues. Medical iodine for imaging or treatment is typically administered orally in the form a pill or liquid solution. A typical adult thyroid scan using iodine-123 involves having the patient swallow between one and four 0.1 millicuries pills, with the exact dose dependent on the patient’s weight. This results in a whole-body committed effective dose of 80 – 320 mrem, and a thyroid equivalent dose of 1443 – 5772 mrem. Note that the whole-body effective dose relates to the overall cancer risk, while the larger equivalent dose to the thyroid only indicates that most of this risk is the result of exposure to the thyroid. These doses are considered safe, although the procedure is not recommended for pregnant or breastfeeding women. In contrast, the quantities of iodine-131 used for treatment of hyperthyroidism and thyroid cancers are much higher. For treatment of hyperthyroidism, 4 – 10 millicuries are administered, while for thyroid cancer the administration can range from 50 – 150 millicuries of I-131. In addition to medical exposures, large populations were exposed to radioiodine as result of the atomic bombings of Hiroshima and Nagasaki in Japan, and the Chernobyl nuclear accident. These populations have been carefully followed for many years to assess the effect of their radiation exposures on cancer risk. As a result, a great deal is known about the cancer risks associated with radioiodine exposure. Because iodine is concentrated in the thyroid, the principal risk of exposure to radioiodine is thyroid cancer. Children have the highest risk of thyroid cancer after exposure to radioactive iodine. According to a large study of Japanese atomic bomb survivors, an effective dose of one Sievert (100,000 mrem) has been observed to increase the risk of thyroid cancer by a factor of 9.5 in children aged zero to nine years old, by a factor of 3 in children aged 10 to 19 years old, and by barely detectable amounts in adults. Another way of quantifying the risk from radioiodine exposure is from risk coefficients, which provide the risk per unit intake of radionuclides in terms of both morbidity (any cancer) and mortality (death). Both morbidity (risk of cancer) and mortality (death) risks are shown in the table below. Note that because thyroid cancer is almost never fatal, the morbidity coefficients are much larger than the mortality coefficients.

61 RADIATION PROTECTION AND DOSIMETRY↗

Air Exchange Rate Impact on Activity Equilibrium Factors and Inhalation Fractional Equilibrium Factors for Rn, Xe, Kr, Ar, Ne, and Their Progeny in Vapor Intrusion, Risk, and Dose Models

Exposure to the radioactive noble gasses, especially radon, is of high concern and poses a significant risk to humans in an indoor air environment as the second leading cause of lung cancer in the United States. To evaluate and minimize the risks posed by these gasses, it is important to understand their radiological and physical properties. The EPA’s Radon Vapor Intrusion Screening Level (RVISL) calculator calculates indoor air RVISLs based on target working levels (WLs), target excess lifetime cancer risk (ELCR), and annual dose limits for the actinon (Rn-219), thoron (Rn-220), and radon (Rn-222) decay series. The RVISLs are based on inhalation and submersion in gas cloud exposure routes for residential and commercial settings. The RVISLs are analogous to preliminary remediation goals (PRGs) and dose compliance concentrations (DCCs), where the isotope-specific values are in units of activity concentration (activity per unit volume). If the concentration of a parent isotope of radon or its progeny is found to exceed the RVISL, then further action to ensure cleanup of the contaminant may be necessary. In residential and commercial settings, the RVISLs will vary based on the air exchange rate present. The EPA’s Radionuclide PRG and DCC Calculators also assess the risk/dose from noble gases in the air due to household use of water like showering. In this study, a computational method in MATLAB was developed to determine the impact of the air exchange rate on the activity equilibrium factor (A eq ) and the inhalation fractional equilibrium factor (F eq ). Both factors are values that reflect the equilibrium concentrations of progeny to their parent in the air. These factors have a direct impact on the RVISL, PRG, and DCC calculations of WL, ELCR, and annual dose, respectively. This study builds on a previous report that only focused on actinon, thoron, and radon by revisiting the original A eq and F eq calculation methods, as well as including the values for the Rn-207, Rn-209, Rn-210, Rn-211, Rn-215, Rn-216, Rn-217, Rn-218, Rn-223, Ne-24, Ar-42, Ar-43, Ar-44, Kr-74, Kr-75, Kr-76, Kr-77, Kr-88, Kr-89, Xe-120, Xe-121, Xe-122, Xe-123, Xe-135m, and Xe-138 decay chains, which are not currently available in literature. The EPA’s RVISL calculator will be updated to include the new A eq and F eq values for the actinon, thoron, and radon decay chains, while the rest of the calculators will incorporate all the new A eq and F eq values as appropriate.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Benchmark Exercise Report for Experimental Study of Bubble Scrubbing in Sodium Pool

Mechanistic source term (MST) analyses are likely to be an important part of advanced reactor licensing applications. For the purpose, an MST analysis code applicable to newly introduced advanced reactors, called SRT (Simplified Radionuclide Transport) code, has been developed by Argonne National Laboratory. SRT can track overall behaviors of radionuclides especially in metal fuel-based sodium fast reactors (SFRs) and microreactors. Throughout the simulation, migration inside fuel pins before failure, interaction with coolant (for SFR), removal/leakage in cover gas and containment (or confinement), and environmental dose impacts are considered alongside radioactive decay for short-lived nuclides. Among the postulated process, pool scrubbing phenomenon, especially under sodium pool condition, has been identified as high importance with limited supportive data. The phenomenon plays a crucial role in assessing the degree of radiological impacts as radioactive aerosols or vapors are efficiently and effectively removed during the process. To provide validation basis for SRT in assessing pool scrubbing performance inside sodium pools, the University of Wisconsin-Madison performed tests including extensive parametric effects. Separate effect tests were conducted to directly evaluate the SRT models and to estimate degree of contribution by each contributing factor. Specifically, bubble size, aerosol size, aerosol density, aerosol concentration, pool depth, system temperature, and bubble swarm effects were considered. According to the parametric effects, decontamination performance enhances with decreasing bubble size, large density, and deeper pool height. Aerosol concentration provides no effect for the whole range of interest, and pool temperature variation shows minor effects under the considered temperature condition. When multiple bubbles are injected generating a bubble swarm condition, DF performance further enhances by bubble interactions and turbulence characteristics. The measurement shows the exceptional importance of aerosol size range considered, with the lowest decontamination, where most radionuclides are expected to escape.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Optimal Transport as a Tool for Scientific Discovery in Radiation Biology

This report summarizes findings from research conducted for the “Exploration of the Poten tial for Artificial Intelligence and Machine Learning to Advance Low-Dose Radiation Biology Re search” (RadBio-AI) program, supported by the U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research, under Awards KP1601011/FWP CC121 and KP1601017/FWP CC121. The research reported here was undertaken in an effort to assess the potential of optimal measure transport methods as components within the larger scope of a com putational framework envisioned to support research in the radiation biology domain. Within this effort, our interest centered on enabling a unified generic framework where probabilistic modeling, inference, and statistical learning can be carried out for a wide range of data distributions. As described next in Section 1 (and in more detail in our original publication), optimal measure transport offers the possibility of such unified approach.

97 MATHEMATICS AND COMPUTING↗

In situ investigation of ion irradiation-induced amorphization of (Ge 2 Sb 2 Te 5 ) 1−x C x [0 ≤ x ≤ 0.12]

Chalcogenide thin films that undergo reversible phase changes show promise for use in next-generation nanophotonics, microelectronics, and other emerging technologies. One of the many studied compounds, Ge2Sb2Te5, has demonstrated several useful properties and performance characteristics. However, the efficacy of benchmark Ge2Sb2Te5 is restricted by amorphous phase thermal stability below ∼150 °C, limiting its potential use in high-temperature applications. In response, previous studies have added a fourth species (e.g., C) to sputter-deposited Ge2Sb2Te5, demonstrating improved thermal stability. Our current research confirms reported thermal stability enhancements and assesses the effects of carbon on crystalline phase radiation response. Through in situ transmission electron microscope irradiation studies, we examine the effect of C addition on the amorphization behavior of initially cubic and trigonal polycrystalline films irradiated using 2.8 MeV Au to various doses up to 1 × 1015 cm −2 . It was found that increased C content reduces radiation tolerance of both cubic and trigonal phases.

36 MATERIALS SCIENCE↗

Application of electron beam technology to decompose persistent emerging drinking water contaminants: poly- and perfluoroalkyl substances (PFAS) and 1,4-Dioxane

Poly- and perfluoroalkyl substances (PFAS) and 1,4-dioxane are persistent emerging contaminants that are currently under consideration for federal and state-specific regulations in drinking water. Both PFAS and 1,4-dioxane are highly resistant to degradation and are not effectively removed by conventional drinking water treatment systems. Results from the Unregulated Contaminant Monitoring Rule 3 survey showed that >540 sites across the nation are contaminated with both PFAS and 1,4-dioxane. Hence, there is a need to identify technologies that can effectively remove both these contaminants. Water treatment via electron beam (e-beam) has been proven effective at treating a wide range of contaminants, including perfluorooctane sulfonate (PFOS), perfluorooctanoate (PFOA), polychlorinated biphenyls, and trichloroethylene. While the e-beam process is often considered similar to advanced oxidation processes (AOPs), e-beam technology is unique in that it produces both highly oxidizing and reducing species at the same time. The specific objectives of this study were to: (i) determine the effectiveness of 9 MeV electrons provided by the Fermilab’s Accelerator Application Development and Demonstration (A2D2) tool to decompose PFAS and 1,4-dioxane; (ii) assess the formation of byproducts during water treatment; (iii) apply the optimized treatment to field groundwater samples contaminated with PFAS and 1,4-dioxane, and (iv) assess the energy demands for the treatment of these contaminants using e-beam. Results from this study showed that e-beam is effective in treating both 1,4-dioxane and PFAS. Complete degradation of 1,4-dioxane was observed at a dose of 5 kGy for an initial concentration of up to 1 ppm without the need for any sample modification. The electrical energy per order (EEo) for treatment of 1,4-dioxane ranged from 0.46 to 0.72 kWh/m 3 /order and was comparable and even lower, in some cases, than other AOP technologies. Alkaline conditions (pH 13) and low dissolved oxygen concentration (2 mg/L) highly favored the treatment of PFAS by e-beam. Greater than 90% removal of PFOA and PFOS from an initial concentration of 100 to 500 ppb was achieved at a dose of 250 kGy and 500 kGy, respectively, under optimized conditions. The degradation efficiency was not significantly changed when treating other PFAS of fluorinated carbon chain length of 5 to 7 individually at 250 kGy with a removal ranging from 85¬–99% for different compounds. Short chain PFAS (perfluorobutanoate: PFBA and perfluorobutane sulfonate: PFBS) did not degrade under the same conditions at 250 kGy, but 70 to 99% degradation was observed at a higher dose of 1000 kGy. Short chain PFAS (perfluorohexanoate: PFHxA (C5) and perfluoroheptanoate: PFHpA (C6)) were detected after treatment of PFOA, but not after PFOS treatment. Inability to close the mass balance through targeted analysis suggests the presence of other intermediates not detectable by available analytical methods. When treating PFAS mixture containing ten compounds at equimolar concentration of 0.05 µM each, preferential degradation of polyfluorinated compound (6:2 fluorotelomer sulfonate or 6:2 FTS) followed by C8 and C7 compounds was observed as a function of increasing e-beam dose. About 30% degradation of ΣPFAS was observed at 250 kGy and no further removal was observed up to a dose of 1000 kGy. C4 to C6 PFASs showed no degradation, while C3 PFAS (PFBS) showed an increase in concentration by 34% at 1000 kGy due to formation from the breakdown of other long chain PFAS. These results suggested that (a) the reaction kinetics is likely different for different PFAS based on chain length, functional group, and the degree of fluorination of the carbon chain, and (b) there may be intermediates generated from the degradation of 6:2 FTS and C7/C8 compounds that can potentially scavenge hydrated electrons needed for reaction with the untreated PFAS molecules. Treatment of three PFAS-contaminated groundwater samples from two US states showed similar trends as observed in the treatment of equimolar PFAS mixtures. Up to 71% removal of ΣPFAS was achieved in real groundwater samples at 750 kGy and data trend suggested that higher degradation is feasible if higher doses (>1MGy) are applied to treat field samples to overcome matrix effects and competing species. Calculated EEo for PFAS ranged from as low as ~48 to 1081 kWh/m 3 /order depending on the type of PFAS treated. These values are comparable and even lower, in some cases, than other destructive technologies employed for PFAS treatment such as ultrasound, plasma, and photochemical treatment. The results from this study indicate e-beam is a promising approach under favorable conditions and should be explored further as an end-of-train treatment option for PFAS destruction.

1,4-Dioxane↗

SCALE Analyses of Scenarios in the Molten Salt Reactor Fuel Cycle

In support of the US Nuclear Regulatory Commission non-light-water reactor fuel cycle demonstration project, the capabilities of SCALE 6.3.1 for radionuclide characterization, criticality, and shielding were demonstrated through several scenarios in a molten salt reactor (MSR) nuclear fuel cycle. Three scenarios were selected for this study, with the molten salt breeder reactor (MSBR) serving as the reference design. The original thorium-based fuel salt used in MSBR was replaced with a 235 U-enriched fuel salt to better reflect anticipated future MSR concepts. The first scenario focused on the fuel salt preparation stage. Criticality analyses, using SCALE/CSAS-Shift and SCALE/SAMPLER, examined potential critical configurations in the fresh fuel salt container based on variables such as 235 U enrichment, UF 4 molar fraction, temperature, and container geometry. The second scenario explored the release of fission products during reactor operation in which the tritium buildup in the primary fuel salt was quantified through depletion calculations using SCALE/TRITON with continuous fuel makeup and fractional fission product removal. This scenario also assessed radioactivity levels in the off-gas system (OGS), quantifying radiotoxic nuclides that could be released into the environment. SCALE/SAMPLER was employed to perform uncertainty quantification to identify key operating parameters influencing the buildup of radiotoxic nuclides in the OGS. Additionally, radiation dose rates were calculated using SCALE/MAVRIC to estimate the maximum exposure levels within the reactor cell complex during operation. The final scenario evaluated the decay heat and radioactivity of the primary fuel salt collected in the drain tank, as well as the radiation dose rate outside the building from the presence of the drain tank. Overall, the application of SCALE’s various capabilities for radionuclide inventory generation, criticality analysis, and shielding in MSR fuel cycles was successfully demonstrated across these scenarios.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Worst Case Sabotage Consequence Modeling for Advanced Reactors

Under proposed rulemaking by the United States Nuclear Regulatory Commission, advanced reactor licensees may qualify for a reduction in onsite responders if the consequences from a sabotage attack do not exceed 25 rem at the reactor site boundary 2 hours after a release occurs. This work presents a preliminary assessment of the feasibility of meeting the 25 rem at the site boundary criteria. Using advanced reactor radionuclide inventories radiological release estimates created by collaborators at Oak Ridge National Laboratory, the MACCS consequence analysis code was used to investigate the distance at the dose from hypothetical sabotage events reaches 25 rem for different advanced reactor technologies. It was found that the distance to 25 rem depended heavily on sampled weather conditions and sabotage release fractions, and further refinement of release fractions and MACCS modeling parameters is recommended.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Empirical evidence that mean soil contaminant concentration is not a conservative indicator of external exposure to wildlife

Adequate information on external exposure is often a limiting factor in ecological risk assessments because of a lack of exposure data for free-ranging animals as they interact with a heterogeneous distribution of contaminants. Instead, most wildlife exposure data are estimated from model simulations. However, empirical exposure data are rarely available to verify model results, or to test fundamental assumptions inherent in exposure assessments. We used novel, GPS-coupled radiation dosimeters on reindeer (Rangifer tarandus) to quantify their external exposure for five months in a Chernobyl fallout affected mountainous area of Norway. The exposure data were then used to test a fundamental assumption in screening-level risk assessments: Mean soil contaminant concentrations can be used to conservatively estimate chronic external exposures to representative animals. External exposure and GPS coordinates were obtained hourly and compared to model simulations of exposure based on airborne surveys of 137 Cs soil contamination. Our objectives were to determine 1) if modelled dose estimates based on mean 137 Cs soil concentrations were conservative, and 2) if modelled dose estimates could be improved by adjusting for spatial–temporal heterogeneity of contaminants using 137 Cs concentrations within reindeers’ GPS-defined home ranges and core areas. We found that external exposure modelled from mean soil contaminant concentrations underestimated exposure by 70% compared to empirical measurements from GPS-dosimeter collars worn on individual animals. Using area-weighted mean contaminant levels within the animals’ home range improved the model estimates, but still underestimated the field dosimeter data by 53%. The best estimate of external exposure was obtained when high-use areas within their home range, along with spatial heterogeneity of the contaminant, was accounted for by using area-weighted mean soil contaminant levels within GPS-derived core areas. Accounting for temporal use of core areas within animals’ home range provided a 24% improvement. Here, a comparison of our analyses to similar work performed on Chernobyl wolves found the two studies concur that risk assessors should be cautious in relying on the paradigm of using averaged soil contaminant levels to provide conservative estimates of external exposure to representative individuals. Results of modelled external exposure based on mean soil contaminant concentrations could misguide assessors and cause inappropriate management decisions.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Evaluating Precision of Measured Radionuclide Ambient Air Concentrations

According to AIRNET – Quality Assurance Project Plan for the Radiological Air Sampling Network, SOP-5140, Revision 2 (to become EPC-CP-PIP-5140): “The regulation 40 CFR Part 61.93 requires that the system be able to readily detect a dose of 1.0 mrem above background. Following statistical principles and assuming 95% confidence for such a measurement, we require that 95% of all measurements must fall within two standard deviations of the mean. This represents the minimum acceptable precision for decision making.” An independent assessment of the Rad-NESHAP program completed in early 2019 found that no documentation existed proving that the Airnet data meets the precision defined above. Therefore, to address this particular finding, Airnet concentration data was pulled from the Environmental Information Management (EIM), a cloud-based database maintained by Locus Technologies, for analysis.

54 ENVIRONMENTAL SCIENCES↗

Tailoring Corrosion Resistance of Additively Manufactured Metals with Atomic Layer Deposition

The goal of this work is to develop a scalable post-manufacturing capability at LANL that utilizes atomic layer deposition (ALD) for corrosion-resistant coatings onto additively manufactured (AM) metals. This will provide fundamentally new and essential capabilities towards the interchangeability of AM metals with traditionally wrought or machined material. This will be accomplished by (1) formulating novel ALD precursor doses and film thicknesses onto as-printed coupons of AM metals and (2) providing electrochemical characterization of corrosion susceptibility as a function of deposited film thickness. While ALD is well-established, the unique aspect (risk) of this work is application to rough AM surfaces. This risk is mitigated by repeating ALD deposition cycles, where thicker coatings laterally branch, resulting in a uniform coating. This risk will be assessed in the phase 1 feasibility study, wherein the application of ALD coatings to small AM coupon surfaces will be demonstrated using existing hardware and characterization tools at Sigma. This study alone will provide ground-breaking insight on the compatibility of ALD coating techniques with AM metals. Going beyond the phase 1 study, a standalone deposition chamber will be built, so full AM components can be coated and tested. While this MFR investment is focused on corrosion mitigation, it is critical to highlight external benefits of this technique outside the scope of this proposed study. ALD has extraordinary universality, whereby almost any material can be given almost any coating or graded density coating with atomic precision; and, the only limiting factors to scalability is the size of the dosing chamber. The self-limiting reactions intrinsic to ALD offers high conformity to part geometry and tolerance, even for internal surfaces where electroplating or conventional chemical vapor deposition falls short due to differential diffusion. This uniquely positions ALD at the forefront of post-manufacturing strategies for AM components, especially for those with complex geometry and internal surfaces.

36 MATERIALS SCIENCE↗

Verification and Validation Tests of Gamma Library of MC2-3 for Coupled Neutron and Gamma Heating Calculation

For the accurate assessment of the heat generation rate in fast reactors, the gamma library of MC2 -3 and the MC2 -3 + GAMSOR procedure employing the coupled neutron and gamma heating calculation has been thoroughly verified against Monte Carlo results and validated using the ZPPR-15D gamma dose measurement data. NJOY outputs are post-processed in a consistent way with the NJOY procedure to avoid any missing data or double counting of data. Prompt heating for 379 out of 391 isotopes in the gamma library was verified against MCNP6.2 to within 1% relative error in total heating for most isotopes. For both a simple one-dimensional slab problem representing a sodium cooled fast reactor and the Experimental Breeder Reactor II (EBR-II) benchmark problem, the root-mean-square values of assembly power error were less than 0.5% for fuel assemblies, ~1% in blankets and ~1 to ~3% in reflectors compared to MCNP6.2 results. The most plausible cause for the 3% error in a reflector assembly is believed to be the error in the multigroup neutron cross sections for the reflector assembly. For validation, gamma doses measured with thermoluminiscent dosimeters (TLDs) in the ZPPR-15D experiment were calculated using GAMSOR. Due to the uncertainty in the TLD measurement with regards to the energy deposition of photons and neutrons, the validation data leads to a 12.7% uncertainty on the experimental measurement. With this uncertainty bound, the calculated doses all fell within one standard deviation of the measured value. Combined with the accurate calculation of reaction rate distributions and neutron spectrum measurements, these results indicate good agreement for the neutron and gamma heating calculations that were performed.

coupled neutron and gamma heating↗