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At least 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

The Nature and State of Groundwater Contamination at the Nevada National Security Site: What Have We Learned from Decades of Groundwater Analysis? - 20337

The regulatory framework for remediating radionuclide contamination from underground nuclear testing at the Nevada National Security Site (NNSS) is based on a combination of characterization and modeling studies, monitoring, and institutional controls [1]. Currently, tritium is the largest contributor (∼90%) to the estimated 44.6 million-curie radionuclide inventory resulting from underground testing [2]. Because of its short half-life (12.32 years), its relative contribution reduces below 10% of the total radiologic inventory over the next 120 years as a result of radioactive decay. Although tritium levels are observed well above the Safe Drinking Water Act (SDWA) maximum contaminant levels (MCLs) in groundwater, other radionuclides are well below their MCLs except within the nuclear test near-field (nuclear test cavity and chimney) environment. In fact, most device-derived radionuclides are below their MCL in groundwater even in samples collected from this near-field environment. The distribution of radionuclides following the nuclear detonation greatly influences the availability of potential contaminants for groundwater transport. Tritium is initially distributed in the gas phase, later as tritiated water in steam, and finally as liquid water, and is available to groundwater transport away from the near-field environment. Other radionuclides that are mobile in groundwater are {sup 14}C, {sup 36}Cl, {sup 99}Tc, and {sup 129}I though their radiologic inventory is small when compared to tritium. Many radionuclides (e.g. U, Pu, Am) are incorporated to a significant extent into the melt glass at the bottom of the cavity and are accessible to groundwater primarily through the slow process of glass dissolution. These radionuclides are also adsorbed to the surfaces of the crushed rock within the cavity and chimney which limits their migration in groundwater. Although colloid facilitated transport of radionuclides at the NNSS has been observed [3], radionuclide concentrations decrease with time and migration distances due to desorption and colloid filtration processes. Current studies indicate that radionuclides associated with colloids are unlikely to migrate downgradient from NNSS underground nuclear tests at concentrations above the SDWA MCL [4][5]. The results of over 50 years of sampling, along with an understanding of these post detonation processes, indicate that tritium is the only contaminant of concern downgradient of testing and that even tritium will not exceed its MCL in groundwater after ∼120 years. Although other longer-lived radionuclides may continue to be released slowly from the near-field environment they will likely never reach levels exceeding their MCLs in groundwater downgradient of the NNSS. Groundwater monitoring will continue to verify these observations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Penetration of Fission Products Ions into Complex Solids and the Effect of Ionic Wash Methods

During washing of radiologically impacted building surfaces, penetration of radionuclide ions into complex solids associated with these surfaces may occur. This study investigates the penetration of Cs-137, Sr-85, and Eu-152 solutions into numerous common building materials and radionuclide behavior when these materials were exposed to a static bath or low-pressure flow of tap water, 0.1 M potassium chloride (KCl), and 0.5 M KCl. The decontamination efficacy and the depth profile for residual contamination were measured to determine the conditions under which applying a wash solution has benefit compared to physically removing the surface material. On asphalt, 70-80% of the radionuclides were found to be within 0.02 mm of the surface. Concrete is more porous than asphalt, and 80% of the radionuclides were within 0.2 mm of the surface for Cs-137 and Eu-152 and 50-80% for Sr-85. Water effectively removed all contaminants from hard nonporous surfaces. Finally, this paper illustrates that a wash penalty factor concept-defined as ratio of the depth at which 50% of the radioactivity is found in the washed sample divided by the depth at which 50% of radioactivity is found in the control-can serve as a way to quantify whether the wash method increases the depth at which contamination penetrates into the material and thus the material becomes more difficult to decontaminate.

building materials↗
DOE OSTI2021

Project 57 Air Monitoring Report: January 1 through December 31, 2019

On April 24, 1957, the Atomic Energy Commission (AEC) (now the Department of Energy [DOE]) conducted the Project 57 safety experiment in western Emigrant Valley northeast of the Nevada National Security Site (NNSS) (formerly the Nevada Test Site) on lands withdrawn by the Department of Defense (DOD) for the Nevada Test and Training Range (NTTR). The test was performed to (1) assess a technique for estimating plutonium distribution resulting from a nonnuclear detonation, (2) develop biomedical evaluation techniques for use in plutonium-laden environments, (3) evaluate methods of surface decontamination, and (4) evaluate instruments and field procedures for the prompt estimation of alpha contamination (Shreve, 1958). Although the test did not result in the fission of nuclear materials, it did disseminate plutonium across the land surface. Following the experiment, the AEC fenced the contaminated area and returned control of the surrounding land to the DOD. Various radiological surveys were performed in the area and the DOE expanded the demarked Contamination Area (CA) in 2007 by posting signs 200 ft to 400 ft (60 m to 120 m) outside of the original fence.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Relative permeabilities for two-phase flow through wellbore cement fractures

Multiple fluids are likely to exist in fractures and flow paths associated with leaky wellbores, including liquids (e.g., crude oil) and gases (e.g., gas exsolved from liquid). These fluids occupy and move through different portions of the pore spaces within the fractures depending on many factors, including fluid properties, fracture size, and the amount of the different fluids. Upward leakage of any phase, through the fracture, can contaminate water-bearing formations, create hazardous surface conditions, and compromise the functionality of the wellbore. Early signs of wellbore leaks may be expressed by anomalous pressure behavior at surface monitoring points on cavern storage wells. These pressure anomalies are difficult to interpret, necessitating knowledge of the factors that affect the multiphase flow in fractures and porous media. These parameters are critical to modeling multiphase flow in fractures. This insight can guide further diagnosis and maximize leak remediation. Here, our study focuses on the relationship of the liquid–gas relative permeabilities for representative variable-aperture wellbore cement fracture. To obtain the relative permeability of each phase, two-phase flow tests were conducted where both fluids were flowing simultaneously through a fractured wellbore cement specimen under a range of factors, namely (1) aperture size, (2) capillary numbers, and (3) viscosity ratio. The flow experiments were conducted under a range of confining stresses and flow velocities, using nitrogen gas and silicone oils (of different viscosities) in a specially designed pressure vessel. The sum of gas and oil relative permeabilities were found to be less than one under all conditions, which indicates that the presence of one phase affects the permeability of the other phase, and vice versa. Since the gas phase flow conditions include a significant inertial flow component in addition to viscous flow, the inertial flow coefficients at different saturation states are presented. The factors affecting the relationship between the relative permeabilities are discussed in detail. A new mathematical model for estimating the relative permeability of wellbore cement fracture is presented and experimentally validated.

58 GEOSCIENCES↗
DOE OSTI2022

Polydiketoenamines for a Circular Plastics Economy

The mismanagement and leakage of plastic waste into the environment are failures of modern society. Once in the environment, plastic waste degrades into microplastics on a time scale dependent on the resin chemistry and the associated biotic or abiotic process. Here, the high surface area of microplastics results in the contamination of ecosystems through the leaching of toxic chemicals compounded with plastics during manufacturing. In addition, the small size of microplastics increases the likelihood that they will be inhaled or ingested, which has led to the bioaccumulation of microplastics with documented harm. Furthermore, microplastics are more readily aerosolized and distributed by weather systems to areas remote from locations where plastic waste has been mismanaged. Consequently, the carbon cycle must now account for plastic waste discharge, degradation, and dispersal in the environment after the end of useful life on a global scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Water-polyamide chemical interplay in desalination membranes explored by ambient pressure X-ray photoelectron spectroscopy

Reverse osmosis using aromatic polyamide membranes is currently the most important technology for seawater desalination. The performance of reverse osmosis membranes is highly dependent on the interplay of their surface chemical groups with water and water contaminants. In order to better understand the underlying mechanisms of these membranes, we study ultrathin polyamide films that chemically resemble reverse osmosis membranes, using ambient pressure X-ray photoelectron spectroscopy. This technique can identify the functional groups at the membrane–water interface and allows monitoring of small shifts in the electron binding energy that indicate interaction with water. We observe deprotonation of free acid groups and formation of a ‘water complex’ with nitrogen groups in the polymer upon exposure of the membrane to water vapour. The chemical changes are reversed when water is removed from the membrane. While the correlation between functional groups and water uptake is an established one, this experiment serves to understand the nature of their chemical interaction, and opens up possibilities for tailoring future materials to specific requirements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

XPS analysis of molecular contamination and sp 2 amorphous carbon on oxidized (100) diamond

The efficacy of oxygen (O) surface terminations on diamond is an important factor for the performance and stability for diamond-based quantum sensors and electronics. Given the wide breadth of O-termination techniques, it can be difficult to discern which method would yield the highest and most consistent O coverage. Furthermore, the interpretation of surface characterization techniques is complicated by surface morphology and purity, which if not accounted for will yield inconsistent determination of the oxygen coverage. We present a comprehensive approach to consistently prepare and analyze oxygen termination of surfaces on (100) single-crystalline diamond. We report on x-ray photoelectron spectroscopy (XPS) characterization of diamond surfaces treated with six oxidation methods that include various wet chemical oxidation techniques, photochemical oxidation with UV illumination, and steam oxidation using atomic layer deposition (ALD). Our analysis entails a rigorous XPS peak-fitting procedure for measuring the functionalization of O-terminated diamond. The findings herein have provided molecular-level insights on oxidized surfaces in (100) diamond, including the demonstration of clear correlation between the measured oxygen atomic percentage and the presence of molecular contaminants containing nitrogen, silicon, and sulfur. We also provide a comparison of the sp 2 carbon content with the O1s atomic percentage and discern a correlation with the diamond samples treated with dry oxidation which eventually tapers off at a max O1s atomic percentage value of 7.09 ± 0.40%. Given these results, we conclude that the dry oxidation methods yield some of the highest oxygen amounts, with the ALD water vapor technique proving to be the cleanest technique out of all the oxidation methods explored in this work.

XPS↗
DOE OSTI2025

Investigation of the distribution of laser-induced damage precursors in etched grating sidewalls fabricated using inductively coupled plasma reactive-ion etching

Inductively coupled plasma reactive-ion etching for grating fabrication is explored with emphasis on the type and distribution of process-induced defects that can act as precursors to laser-induced damage initiation. To provide flexibility in the ability to perform a variety of material characterization methods, grating-like features with large pitch were fabricated in silica monolayers. The results indicate that the etch process introduces surface fluorine and subsurface carbon-containing contamination, which reduces the laser-induced damage threshold. The local relative concentrations of the laser-damage precursors introduced during the etch step of the manufacturing process were investigated using angle-resolved damage testing, taking advantage of the shift of the location of the peak electric-field intensity incident on the grating sidewall. The results suggest an increased level of etch-related defects near the base of the sidewall, with directly fluorinated silicon identified as the primary defect.

Dent, R. [Univ. of Rochester, NY (United States). ↗
DOE OSTI2022

Interactions between molecular-scale processes and hyporheic exchange for understanding Fe-S-C cycling in riparian wetlands (Final Report)

Wetlands represent some of the most productive ecosystems on the planet and critically influence global environmental health. Specifically, wetlands promote water quality by transforming nutrients and organic compounds and sequestering metals and contaminants. Riparian wetland hyporheic zones, where toxic surface water and anoxic groundwater mix, exhibit dynamic conditions that drive steep redox gradients and promote hotspots of diverse and fluctuating microbial activity. Changes in climate, water quality, and water quantity can disturb hydrologic flow and biogeochemical processing in these environments. Understanding how sulfate loading, impacted by hydrologic flux and anthropogenic inputs, influences iron and carbon cycling in wetlands will be crucial for predicting water quality issues driven by iron mineral precipitation and sorption, such as the release of heavy metals and other toxic elements. We used a fully integrated multi-scale and multi-method approach to develop a mechanistic understanding of how hydrologic flow influences coupled iron and sulfur cycles in riparian wetlands. This entailed hydrological, geochemical, and microbial observations at two locations: an anthropogenic sulfate-impacted riparian wetland in northern Minnesota, and a low-sulfate Fe-rich riparian wetland in Tims Branch at the Savannah River Site (SRS). These sites were characterized by hydrologically dynamic conditions where the stream and wetland systems oscillated between gaining (upward flow) and losing (downward flow) conditions that recharged the system occasionally with oxidants that fueled a variety of biogeochemical reactions. Aqueous geochemical measurements of surface water, groundwater, and porewater samples were made alongside solid-phase geochemical analyses of sediment gravity cores. Bulk X-ray absorption spectroscopy at the Advanced Photon Source (APS; Argonne) interrogated the speciation and distribution of Fe and S mineral phases of the sediments. Interestingly, it was discovered that, despite strongly reducing conditions, Fe(III) compounds and a variety of intermediate valence S compounds were stable in the subsurface. Indeed, compounds like thiosulfate, S(0), and intermediate valence organosulfur compounds were more prevalent than FeS and pyrite. The composition of the sediments did change with changes in hydrologic flow, showing their reactivity in changing redox conditions. The abundance of these intermediate S compounds was likely formed as a result of anaerobic oxidation by aqueous and solid-phase Fe(III) compounds, fueling a cryptic S cycle that is driving the breakdown of organic matter in the hyporheic zone. Microbiome surveys showed a core community that seemed stable across the landscape, but changed with increasing depth into the sediment. The community composition did not seem to change dramatically with changes in season or hydrologic flow, except for some organisms that have the potential to contribute to S cycling. More work is needed to confirm their functional activity. These fine process-scale analyses were placed within a dynamic field context using physical flow parameters from surface water and groundwater level measurements. These data helped shed light on sulfur-driven biogeochemical processes in hydrologically dynamic riparian wetlands, addressing a gap in our understanding about the impacts of pollution and other anthropogenic changes on ecologically sensitive environments.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Fitting the RESRAD External Dose Rate Coefficients Model to the FGR 15 Data

FGR15 (Bellamy et al. 2025) lists external dose rate coefficients for radionuclides in soil, water and air. It has five tables of coefficients for contaminated soil; one for radionuclides on the surface of the soil and one each for radionuclides in soil layers of 1 cm, 5 cm, 15 cm and infinite thickness. Each table contains 7512 coefficients, quantifying the external dose rate from each of the 1252 ICRP107 radionuclides, to each of the six reference persons of different ages.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Oil and Natural Gas Development near and beneath Uranium Tailings Cells and Other Remediated Sites - 20358

DOE LM is responsible for maintaining remedies at more than 50 remediated sites that require active long-term surveillance and maintenance (LTS and M). Institutional controls (ICs) were established to limit human and environmental exposures to residual contamination by controlling land use, restricting access to potential hazards, and making the public aware of potential dangers from the residual contamination. ICs for each site were developed based on current and foreseeable conditions; however, these controls should evolve to mitigate potential human health and other environmental risks from unanticipated changes in activities or site conditions. Activities conducted beyond the DOE long-term care boundaries by non-DOE parties may impact the effectiveness of ICs or even the long-term stability of disposal cells and groundwater remedies. Several sites that LM manages or that will transfer to LM for LTS and M are in active oil and gas production basins. The sites are associated with uranium ore milling or nuclear test sites and have been remediated or are in the process of remediation and have no ongoing DOE mission. Particularly since 2005, hydraulic fracturing ('fracking') combined with directional drilling has dramatically increased oil and natural gas (oil/gas) production in the United States, now making it the number one hydrocarbon-producing country. Fracking has allowed production from shale and other rocks of low natural permeability that were historically not considered viable oil/gas resources. Also, because wellbores can now be drilled as many as 5 kilometers or more horizontally, hydrocarbons can be recovered from zones without having access to the surface above them. Drilling activity near Rulison, Colorado, the location of an underground nuclear detonation managed by LM, has raised public concerns that remnant radioactivity in the detonation zone could migrate to producing wells and enter the natural gas distribution system. At sites like the Falls City, Texas, Disposal site, transitioned to LM with a split estate, increased production in the region has resulted in wellbores beneath the long-term care boundary of the site. While the DOE license for Falls City was approved by the NRC in 1997 without the acquisition of the subsurface rights, NRC has raised concerns on whether this activity impacts the integrity of the cell and/or groundwater remedies. In Wyoming, LM is anticipating receiving the license for the Bear Creek site and manages the Spook site, both locations of uranium mill tailings disposal cells. These Wyoming sites are in an active region of major oil and gas development. This change in surrounding land use will require LM to work collaboratively with NRC to address these concerns. At several DOE sites radioactive waste, and often intermixed nonradioactive constituents, is permanently isolated in engineered disposal cells. At other sites, residual contamination can be present in groundwater, blast cavities, and infinite amounts within soil. Areas targeted for oil and gas development at the Texas and Wyoming sites range from depths of 2440 to 3350 meters (8000-11000 feet) below ground surface. When most site remedies were designed, oil and gas development was not considered to be an issue within the site boundary. With the more recent uses of directional drilling, fracking, and associated wastewater injections, the evaluative criteria for incoming sites and ICs for managing long-term protectiveness and regulatory compliance are changing. Although DOE surface ownership was previously thought to be a robust IC to prevent surface and subsurface development, particularly at disposal sites, that may no longer be the case. Whereas the subsurface development at Texas and Wyoming sites is currently occurring at thousands of meters beneath the surface, shallower and direct onsite development would be more of a concern for LM. The energy introduced when a well is hydraulically fractured causes microseismic events (magnitude -2 to 1.0) as the fractures propagate but does not directly cause seismic events (earthquakes) of sufficient magnitude to damage surface structures. Additionally, the extent of the hydraulic fractures is limited to the targeted depths, which are far below the surface. However, earthquakes of sufficient magnitude to damage surface structures have been attributed to the injection of wastewater into disposal wells. States that have experienced these effects have enacted regulations that limit the rate and pressures that wastewater can be injected into disposal wells. Items LM may consider are the need for monitoring the volume of water injected into nearby disposal wells and possibly installing seismic stations at sites most susceptible to damage. While the need to demonstrate that no impact from oil and gas extraction activities on a site groundwater remedy or disposal cells will vary from site to site, LM is assessing risk criteria for this activity. Though LM has not experienced an issue yet at a uranium tailings disposal site, it cannot assume that there will be none, and must address NRC concerns. LM is building on past experiences at other sites and beginning to form new processes with the hope that these concepts can be applied for other future sites. (authors)

04 OIL SHALES AND TAR SANDS↗
DOE OSTI2020

Choosing the Best Modeling Platform for Radiological Risk Assessment Models - 20468

Radiological risk assessments, in the form of performance or safety assessments, are often required under regulations or guidance for remediation of contaminated land, decommissioning of contaminated buildings or structures, and radioactive waste disposal. These risk assessments are usually supported by fate and transport models that address decay and ingrowth of radionuclides, as well as their movement through engineered systems and the natural environment. These models are often projected thousands, or more, years into the future, largely because the radioactive species change through decay and ingrowth, and hence the magnitude of the radioactive effect changes with time. There are many computer codes that are available to address this type of modeling. They range from addressing specific pathways or processes such as infiltration of water, groundwater, surface water, air, biota, diffusion and advection of water and gases, to those that try to couple all processes together to evaluate the impact of fate and transport through the entire system to places in space and time to which access is assumed. These different types of codes are sometimes separated with the monikers process-level and systems-level codes, although it is often not clear that this separation does justice to the capabilities of the many codes that are available to evaluate fate and transport of radionuclides. The focus of this paper is the latter group of modeling codes. Several systems level modeling codes exist and are used. There are differences between these codes in terms of utility, flexibility, complexity and cost. The purpose of this paper is to compare a few of these codes in the context of work currently being performed by the International Atomic Energy Agency (IAEA) Modeling and Data for Radiological Impact Assessments (MODARIA) II Working Group 1 (WG1). The MODARIA II WG1's main focus is how stakeholder engaged decision analysis can, or should, be applied to radiological contamination problems so that better, longstanding, sustainable, solutions are reached. However, the WG1 also recognizes the potential impact of the modeling tools that are chosen to address radiological risk, which is often a primary objective of decision making for radiological problems. Other objectives might also be important, such as constraining costs, obtaining financing, minimizing impact on ecosystems, saving cultural resources, saving jobs, farmland, environmental justice, etc., in a full decision analysis for a given radiological contamination problem, but none of these other objectives have the same types of complex modeling needs as minimize radiological dose. Consequently, a further focus of WG1 is to evaluate the potential impacts on decision making of the choice of fate and transport, and risk assessment, modeling codes that are used to support decision making. The WG1 will produce a report at the end of 2020 that will focus on an approach to effective decision making and stakeholder engagement. The report will also consider the role that performance assessment modeling should play in the decision-making process, including the impact of the choice of modeling tools or computer codes on risk-informed decision making. Several sites around the World have been made available by Member States for these model comparisons, and several modeling tools have been considered. However, the focus of this paper is on two of the sites, one in Belgium and one in Ukraine, and on three of the tools: NORMALYSA (NORM And Legacy Site Assessment); GoldSim{sup C}, and AMBER{sup C}. The final report from this working group will also cover other modeling tools, including RESRAD, and PC-Cream{sup R}. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Analysis of Hydrology and Interim Measure Performance in the Chromium Plume at Los Alamos National Laboratory - 20498

Hexavalent chromium, Cr(VI), is present in the regional aquifer beneath Los Alamos National Laboratory (LANL) at concentrations greater than the New Mexico groundwater standard (50 ppb). The source of the Cr is blowdown from a power plant where potassium dichromate was used as a corrosion inhibitor from 1956 to 1972. Blowdown comingled with effluent from another source and migrated approximately 3 miles down a canyon, primarily as surface flow, until reaching an alluvial infiltration zone. The infiltrating water moved vertically through a thick (approximately 900 ft), complex stratigraphic sequence of unsaturated tuffs, basalt, and unconsolidated alluvial deposits. Horizontal transport also took place within spatially limited perched groundwater horizons in the vadose zone (VZ). Breakthrough at the regional aquifer water table is thought to have occurred in multiple hydraulic windows or 'drip points' located approximately 3 miles from the initial release site at the power plant. The regional aquifer is highly heterogeneous and anisotropic, and displays unconfined behavior in an upper zone and confined behavior at depth. The Cr(VI) contamination has so far remained confined to the upper approximately 25 m of the aquifer. The ambient hydraulic gradient in the regional aquifer is toward the east/southeast, but the water table is extremely flat in the Cr plume area compared to surrounding areas. There is some local variability in flow direction, potentially related to effects of seasonal pumping from nearby Los Alamos county water-supply wells, which draw from the regional aquifer several hundred feet below the water table. An interim measure (IM) is currently operating at the site to achieve hydraulic control of plume migration using a series of extraction wells, ion-exchange treatment, and injection along the downgradient portion of the plume. The migration of Cr contamination in the aquifer has been previously evaluated using a calibrated probabilistic numerical model, which has also been used to design the spatial configuration of extraction and injection wells for the IM, and to identify locations for monitoring wells. The model is built using the Finite Element Heat and Mass (FEHM) transfer code, and the Model Analysis and Decision Support (MADS) software is used for analyses. To date, the portion of the IM system that has operated in a continuous manner has been very effective at hydraulic control. Modifications to the flow field associated with the influence of IM pumping and injection are evaluated here, with modeling constraints to be provided by recent observations of tracers injected into both monitoring wells and IM injection wells, as well as opportunistic observations of geochemical signatures of treated ion-exchange effluent injected into IM injection wells. The tracer and geochemical data provide insights into modified flow directions within the Cr plume area that cannot be otherwise obtained. Results of the modeling work are being used to inform adaptive management of IM operations and will be a valuable tool for development and refinement of long-term remediation strategies. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Distribution Development for Residual Inventory at the New York West Valley Site - 20400

The New York State Energy Research and Development Authority (NYSERDA) is the owner of the Western New York Nuclear Service Center (WNYNSC), a 1,351 ha site located approximately 48 km south of Buffalo, New York. In 1962, Nuclear Fuel Services, Inc. (NFS) entered into Agreements with the Atomic Energy Commission and New York State to construct the first commercial reprocessing plant of nuclear fuel in the United States. NFS, a private company, built and operated the spent fuel reprocessing plant and waste disposal facilities, processing 640 Mg of spent nuclear fuel from 1966 to 1972 under an Atomic Energy Commission license. Nuclear fuel reprocessing operations ended in 1972 and never reopened, leaving behind radioactive and chemical wastes. Operations led to contamination in a number of facilities and locations. Some of that contamination has migrated from waste disposal zones to other layers, formations, and features on and off the WNYNSC. Phase I decommissioning activities are ongoing and involve the removal of a number of areas and structures that have been associated with contamination. The purpose of this work is to outline the approach for characterizing contamination not associated with disposed wastes, contaminated structures, or specific releases. In this work, the term, residual radiological activity, is used to describe environmental contamination that exists subsequent to the completion of Phase I decommissioning activities, that is not associated with disposed wastes, contaminated structures, or specific releases. Contamination from the Site was quantified relative to data that characterize the concentrations of radionuclides that exist in background. Background concentrations are those present in the area but having no influence from Site related activities. The existence of residual radiological activity that is elevated relative to background has the potential to contribute to future risks to human health and the environment. As a consequence, the residual inventory information is used to inform the West Valley Probabilistic Performance Assessment (PPA) model to characterize potential future risks to human health and the environment. The centralized West Valley Data Management System (DMS) was the source of information for the data assembled in this analysis. The DMS is a fairly large compilation consisting of thousands of records from investigation studies, with sample dates ranging from 1990 to present. Samples from monitoring wells, boreholes, geoprobe studies, surface water, surface soils, storm water outfalls, ventilation stack filters, plant and animal tissues, and more are included in the DMS. Results are typically reported in units of activity per unit volume. For the purpose of the analyses presented here, all results were converted into consistent units of pCi per unit volume. Since 1990, data have been collected from various locations across the WNYNSC at different times with varying frequency over the course of several decades. As a consequence, a number of potential issues can arise with respect to the assembly of a dataset that is deemed adequate for the characterization of residual radiological activity. These issues were assessed and resolved to the extent possible through careful consideration of the properties of the distributions. The intent was to use data which characterize the current state of the Site. Radionuclides can be designated to one of several groups depending on their origin. In this work the groups considered were 1) Naturally Occurring Radioactive Material (NORM), 2) fallout, and 3) Other (including power plant, medical research, etc). This grouping is a useful construct with respect to the interpretation of fixed laboratory results. For example, NORM radionuclides that exist within a decay chain should have approximately equivalent distributions of concentrations if they are representative of background conditions. Insights such as these can be used as a check to identify sample results that need to be further investigated or omitted due to issues associated with reported results from fixed laboratory analyses. This type of analysis provided a foundation for the assessment of the adequacy of sample results for use in subsequent components of an assessment. The general process for the assessment of residual radiological contamination at the Site consists of a sequence of several steps. First, for each analyte, several statistical tests were performed to assess the weight of evidence against the null hypothesis that the mean of the distribution of concentrations was equal to zero. If the mean of the distribution of concentrations for a given radionuclide was not found to be greater than zero, then it was removed from consideration as a component of the residual radiological contamination. If there was significant evidence to reject the hypothesis of the mean being equal to zero, the second step was to compare the distribution of the data from the Site to that of the corresponding background. A suite of tests was used to compare the distributions of the site and background data. The results of these tests were collectively used to determine if site data are elevated relative to background. The third step was to develop distributions using a Bayesian framework to characterize the distribution of mean of the increment present above background for each of the radionuclides. The Bayesian model implemented allowed for the comparison of site-specific records to background concentrations to better approximate contamination attributed to the Site. A final screening step was employed for radionuclides that exceed background. This screening step compared 95% upper confidence limits (UCLs) from the increment distribution developed in the previous step to the risk screening levels. This approach yields a list of analytes that were determined to be elevated relative to background.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Multi-Analytical Investigation of Arsenical Transfer and Remediation on Nineteenth-Century Green Books

Books containing heavy metals, specifically nineteenth-century green arsenical books, have been identified at Northwestern University Libraries, raising health and safety concerns related to handling. Copper acetoarsenite pigments, such as emerald green, were detected on book covers, decorative page edges, labels, and other components using noninvasive analytical techniques including X-ray fluorescence (XRF), Raman spectroscopy, and Fourier-transform infrared (FTIR) spectroscopy. Further examination of selected volumes using synchrotron radiation (SR) techniques revealed pigment migration, degradation, and arsenic transfer to adjacent books. This paper expands on initial findings through two related experiments. The first explored the transfer of arsenic using mechanical friction; Staedtler Mars® white vinyl erasers rubbed on arsenical books generated crumbs which were analyzed via scanning electron microscopy–energy-dispersive X-ray spectroscopy (SEM-EDX). Results confirmed the transfer of arsenic, copper, and lead, with decorative page edges being particularly prone to shedding arsenic onto other materials. The second experiment tested remediation methods on a book contaminated by prolonged exposure to an arsenical neighbor. Surface cleaning using erasers and a vacuum removed flecks of pigment but did not eliminate non-chromophoric arsenic as confirmed by SR analyses, which highlights its presence either as a degradation product embedded within the paper or present in the paper as part of its production process. Findings demonstrate the acute toxicity risk posed by arsenical books and support the need for safe handling protocols. However, materials with only trace levels of arsenic embedded during production may pose a lower risk of transfer. Cross contamination beyond prolonged direct contact appears limited. These results highlight critical considerations for library preservation practices and future research on arsenic in historical materials.

arsenic↗
DOE OSTI2025

Detection of trace contaminants released from rapidly heated pulsed power electrodes by laser diagnostics

Development of a capability to measure trace gas contaminants released from pulsed power electrodes would immediately impact Sandia pulsed power research. These releases occur during ultra-fast heating of metal electrodes during pulsed power discharges and can lead to substantial power losses through plasma formation. Detection of contaminants is a formidable challenge due to the need for in-situ spatially and temporally resolved measurements of trace gases in the extreme environment of ultra-fast heated metal surfaces. We investigate the feasibility of laser diagnostics for detecting contaminants, including H-atom, OH, and H 2 O. Laser-induced fluorescence and photofragmentation fluorescence showed significant plasma emission interferences and did not yield any detectable H-atom, OH, or H 2 O. Our newly developed H-atom detection using femtosecond degenerate four-wave mixing suppressed interferences and enabled detection of H-atoms. A few shots showed large signals in the near-surface region of metal foils, suggesting the formation of a wave of H-atoms from the metal.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

A Review of the Resuspension of Radioactively Contaminated Particles by Vehicle and Pedestrian Traffic—Current Theory, Practice, Gaps, and Needs

Here, the resuspension of radioactively contaminated particles in a built environment, such as from urban surfaces like foliage, building exteriors, and roadways, is described empirically by current plume and dosimetry models used for hazard assessment and long-term risk purposes. When applying these models to radiological contamination emergencies affecting urban areas, the accuracy of the results for recent contamination deposition is impacted in two main ways. First, the data supporting the underlying resuspension equations was acquired for open, quiescent conditions with no vehicle traffic or human activities, so it is not necessarily representative of the urban environment. Second, mechanical disturbance by winds in urban canyons and during emergency operations caused by vehicle traffic and human activities are not directly considered by the equations. Accordingly, plume and dosimetry models allow the user to input certain compensating values, but the models do not necessarily supply users instructions on what values to use. This manuscript reviews the available literature to comprehensively and consistently pool data for resuspension due to mechanically induced resuspension applicable to urban contamination. Because there are few studies that directly measured radioactive resuspension due to vehicles and pedestrians, this review novelly draws on a range of other studies involving non-radioactive particles, ranging from outdoor air pollution emissions to indoor allergen transport. The results lead to tabulated, recommended values for specific conditions in the emergency phase to help users of plume and dosimetry models maintain the conservativeness needed to properly capture the potential radiation dose posed by mechanically induced resuspension. These values are of benefit to model users until better data are available. The results also suggest the types of data that may result in improved plume and dose modeling.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2020

Contaminant Migration Modeling to Support the In Situ Decommissioning of Hardened Nuclear Facilities - 20215

The decommissioning of hardened nuclear facilities provides a unique challenge in balancing current worker dose with exposure to future receptors and media. In situ decommissioning (ISD) is a cost-effective and safe option for the closure of such facilities but requires a detailed understanding of the threat that radioactive and hazardous constituents remaining in the facilities pose to groundwater and surrounding surface water. The Savannah River Site (SRS) extensively employs contaminant migration models within the decommissioning process to develop site-specific removal, grouting, and monitoring strategies in support of safe and effective final end states of nuclear facilities. This work discusses the use of contaminant migration modeling in the ISD process at SRS, including specific examples from the closure of P-Reactor and R-Reactor, Building 235-F, F-Canyon and F/H Laboratory Complex. Migration models developed during the closure of P-Reactor and R-Reactor were divided into four source areas: the reactor vessel, the process area, the disassembly basin, and the purification wing. Each source area was assigned a specific inventory and migration pathway and was then subject to varying hypothetical removal, capping, and grouting schemes. Modeling indicated that groundwater Maximum Concentration Limits (MCLs) might be exceeded if no action was taken for eleven and ten constituents of concern (COCs) at P-Reactor and R-Reactor, respectively. These exceedances could occur in as few as 200 to 500 years. Alternatively, the migration modeling demonstrated that the selected ISD actions reduced contaminant mobility which allowed for significant radioactive decay and resulted in fewer predicted exceedances of groundwater MCLs (five COCs for P-Reactor; eight COCs for R-Reactor). In response to the modeling results for P-Reactor and R-Reactor, effectiveness monitoring programs were developed to target contaminants, specific to each reactor, that may migrate to groundwater. Contaminant migration modeling also revealed that roof collapse was a large factor in the release of COCs to the environment, giving rise to roof improvements, and an inspection and vegetation control program to ensure roof stability over time. Contaminant migration modeling is also aiding in the closure planning for hardened facilities in F Area. Building 235-F housed the Actinide Billet Line, which produced Np-237 billets for irradiation in SRS reactors, and the Plutonium Fuel Form (PuFF) facility that produced Pu-238 heat sources for the space program. As a result of these missions, areas within Building 235-F contain considerable residual amounts of both Pu-238 and Np-237. Contaminant migration modeling of Building 235-F was originally performed in 2012 to identify the feasibility of ISD and the amount of radioactive material removal required to prevent the exceedance of groundwater MCLs. The original model indicated that a 60% reduction in the PuFF facility Pu-238 inventory could keep groundwater concentrations below standards, while Np-237 did not pose a threat to groundwater. However, updates to the model with an emphasis on source impact pathways revealed that, due to the orientation of the source areas relative to groundwater flow, no amount of reasonable removal of Pu-238 would keep groundwater concentrations below MCLs and that Np-237 could be a large contributor to localized MCL exceedances. With this insight, the refined 2019 model is being used to assist in the development of grouting plans specific to each facility source area, where bentonite may be utilized to slow the migration of Pu-238 and its daughter products from the PuFF facility and a reducing grout may decrease Np-237 transport by ensuring the nuclide remains in the less mobile +IV oxidation state. The beginning phases of contaminant migration modeling are underway for F-Canyon and associated facilities using lessons learned from the Reactors and Building 235-F. A contaminant migration pathway, similar to the pathway used for the reactor vessels, is being developed for the hot and warm canyons. The F-Canyon inventories are being spatially refined to identify specific and localized source zones, comparable to Building 235-F, that may impact groundwater. Contaminant migration modeling provides vital input within the ISD process, from facility investigation to post closure effectiveness monitoring, making it a valuable tool in the development of safe and effective end states for hardened nuclear facilities at SRS. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗