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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records

Diffusive release of uranium from contaminated sediments into capillary fringe pore water

Despite remediation efforts at the former nuclear weapons facility at the Hanford site (Washington State), leaching of uranium (U) from contaminated sediments to the ground water persists at the Hanford 300 Area. Flooding of contaminated capillary fringe sediments due to seasonal changes in the Columbia River stage has been identified as a reason of continued U supply to ground water. We investigated the release of U from Hanford capillary fringe sediments to pore water. Contaminated Hanford sediments were packed into reservoirs of centrifugal filter devices and saturated with Columbia River water for 3 to 84 days at varying solution-to-solid ratios (1:3, 1:1, 5:1, 10:1, 25:1 mL:g). After specified times, samples were centrifuged to a gravimetric water content of 0.11 ± 0.06 g g-1. Within the first three days, there was an initial rapid release of 6-9% of total U from the sediments into the pore water, independent of the solution-to-solid ratio. After 14 days of reaction, however, the experiments with the narrowest solution-to-solid ratios (1:3 and 1:1 mL:g) showed a decline in dissolved U concentrations. The removal of U from the solution phase was accompanied by removal of Ca and HCO3-. Geochemist workbench simulations, conducted using measured solution concentrations from experiments, indicated that calcite could precipitate in the 1:3 solution-to-solid ratio experiment. After the rapid initial release in the first three days for the 5:1, 10:1, and 25:1 solution-to-solid ratio experiments, there was sustained release of U into the pore water. Up to 22% of total U was released on day 84 for the 25:1 solution-to-solid ratio reaction. This sustained release of U from the sediments had diffusion-limited kinetics.

contaminated sediments↗

The impact of contamination and aging effects on the long-term laser-damage resistance of SiO 2 /HfO 2 /TiO 2 high-reflection coatings for 1054nm

The laser damage thresholds of optical coatings can degrade over time due to a variety of factors, including contamination and aging. Optical coatings deposited using electron beam evaporation are particularly susceptible to degradation due to their porous structure. In a previous study, the laser damage thresholds of optical coatings were reduced by roughly a factor of two from 2013 to 2017. The coatings in question were high reflectors for 1054 nm that contained SiO 2 and HfO 2 and/or TiO 2 layers, and they were stored in sealed PETG containers in a class 100 cleanroom with temperature control. At the time, it was not certain whether contamination or thin film aging effects were responsible for the reduced laser damage thresholds. Therefore, to better understand the role of contamination, the coatings were recleaned and the laser damage thresholds were measured again in 2018. Here, the results indicate that contamination played the most dominant role in reducing the laser damage thresholds of these optical coatings, even though they were stored in an environment that was presumed to be clean.

42 ENGINEERING↗

Geochemical, mineralogical and microbiological characteristics of sediment from a naturally reduced zone in a uranium-contaminated aquifer

Localized zones or lenses of naturally reduced sediments have the potential to play a significant role in the fate and transport of redox-sensitive metals and metalloids in aquifers. To assess the mineralogy, microbiology and redox processes that occur in these zones, several cores from a region of naturally occurring reducing conditions in a U-contaminated aquifer (Rifle, CO) were examined. Sediment samples from a transect of cores ranging from oxic/suboxic Rifle aquifer sediment to naturally reduced sediment were analyzed for U and Fe content, oxidation state, and mineralogy; reduced S phases; and solid-phase organic C content using a suite of analytical and spectroscopic techniques on bulk sediment and size fractions. Solid-phase U concentrations were higher in the naturally reduced zone, with a high proportion of the U present as U(IV). The sediments were also elevated in reduced S phases and Fe(II), indicating it is very likely that U(VI), Fe(III), and SO 4 reduction has occurred or is occurring in the sediment. The microbial community was assessed using lipid- and DNA-based techniques, and statistical redundancy analysis was performed to determine correlations between the microbial community and the geochemistry. Increased concentrations of solid-phase organic C and biomass in the naturally reduced sediment suggests that natural bioreduction is stimulated by a zone of increased organic C concentration associated with fine-grained material and lower permeability to groundwater flow. Characterization of the naturally bioreduced sediment provides an understanding of the natural processes that occur in the sediment under reducing conditions and how they may impact natural attenuation of radionuclides and other redox sensitive materials. Results also suggest the importance of recalcitrant organic C for maintaining reducing conditions and U immobilization.

54 ENVIRONMENTAL SCIENCES↗

Understanding Contamination; Twenty Years of Simulating Radiological Contamination

A wide variety of simulated contamination methods have been developed by researchers to reproducibly test radiological decontamination methods. Some twenty years ago a method of non-radioactive contamination simulation was proposed at the Idaho National Laboratory (INL) that mimicked the character of radioactive cesium and zirconium contamination on stainless steel. It involved baking the contamination into the surface of the stainless steel in order to 'fix' it into a tenacious, tightly bound oxide layer. This type of contamination was particularly applicable to nuclear processing facilities (and nuclear reactors) where oxide growth and exchange of radioactive materials within the oxide layer became the predominant model for material/contaminant interaction. Additional simulation methods and their empirically derived basis (from a nuclear fuel reprocessing facility) are discussed. In the last ten years the INL, working with the Defense Advanced Research Projects Agency (DARPA) and the National Homeland Security Research Center (NHSRC), has continued to develop contamination simulation methodologies. The most notable of these newer methodologies was developed to compare the efficacy of different decontamination technologies against radiological dispersal device (RDD, 'dirty bomb') type of contamination. There are many different scenarios for how RDD contamination may be spread, but the most commonly used one at the INL involves the dispersal of an aqueous solution containing radioactive Cs-137. This method was chosen during the DARPA projects and has continued through the NHSRC series of decontamination trials and also gives a tenacious 'fixed' contamination. Much has been learned about the interaction of cesium contamination with building materials, particularly concrete, throughout these tests. The effects of porosity, cation-exchange capacity of the material and the amount of dirt and debris on the surface are very important factors. The interaction of the contaminant/substrate with the particular decontamination technology is also very important. Results of decontamination testing from hundreds of contaminated coupons have lead to certain conclusions about the contamination and the type of decontamination methods being deployed. A recent addition to the DARPA initiated methodology simulates the deposition of nuclear fallout. This contamination differs from previous tests in that it has been developed and validated purely to simulate a 'loose' type of contamination. This may represent the first time that a radiologically contaminated 'fallout' stimulant has been developed to reproducibly test decontamination methods. While no contaminant/methodology may serve as a complete example of all aspects that could be seen in the field, the study of this family of simulation methods provides insight into the nature of radiological contamination.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Influence of metallic contaminants on the electrochemical and thermal behavior of Li-ion electrodes

Emerging nondestructive (direct) recycling techniques for lithium-ion batteries may introduce metallic impurities into recycled electrodes. In the present work, the impact of such nonionic contaminants on the practical performance of both anode and cathode materials is evaluated using a synergistic combination of electrochemical and thermal analysis. The impurities under study have been selected through evaluation of industrially shredded batteries, and include Fe0, Al0, Mg0, Cu0, and Si0. The electrochemical behavior of materials containing each individual contaminant at either the anode or the cathode is evaluated in both half-cell and full-cell format. Further, the first-cycle thermal signatures of full cells are used to validate and complement electrochemical signatures, and the two techniques are used in conjunction to suggest distinct mechanisms of electrochemical reactivity for the various impurities. At the anode, metallic contaminants are found to disrupt performance through direct reaction with Li and may serve as weak catalysts to accelerate electrolyte degradation. At the cathode, metallic contaminants show evidence of crossover during formation cycling to disrupt SEI formation. We suggest that coupled electrochemical and thermal analysis may be used to both identify the presence of contaminants and to elucidate specific mechanisms of reactivity for metallic impurities under anodic and cathodic conditions.

Contaminant↗

Adapted tube cleaning practices to reduce particulate contamination at hydrogen fueling stations

The higher rate of component failure and downtime during initial operation in hydrogen stations is not well understood. The National Renewable Energy Laboratory (NREL) has been collecting failed components from retail and research hydrogen fueling stations in California and Colorado and analyzing them using an optical zoom and scanning electron microscope. The results show stainless steel metal particulate contamination. While it is difficult to definitively know the origin of the contaminants, a possible source of the metal particulates is improper tube cleaning practices. To understand the impact of different cleaning procedures, NREL performed an experiment to quantify the particulates introduced from newly cut tubes. The process of tube cutting, threading and beveling, which is performed most often during station fabrication, is shown to introduce metal contaminants and thus is an area that could benefit from improved cleaning practices. This paper shows how these particulates can be reduced, which could prevent station downtime and costly repair. These results are from the initial phase of a project in which NREL intends to further investigate the sources of particulate contamination in hydrogen stations.

30 DIRECT ENERGY CONVERSION↗

Influence of Network Model Detail on Estimated Health Effects of Drinking Water Contamination Events

Network model detail can influence the accuracy of results from analyses of water distribution systems. Previous work has shown the limitations of skeletonized network models when considering water quality and hydraulic effects. Loss of model detail is potentially less important for aggregated effects such as the systemwide health effects associated with a contamination event, but has received limited attention. The influence of model detail on such effects is examined here by comparing results obtained for contamination events using three large network models and several skeletonized versions of the models. Loss of model detail decreases the accuracy of estimated aggregated adverse effects related to contamination events. It has the potential to have a large negative influence on the results of consequence assessments and the design of contamination warning systems. However, the adverse influence on analysis results can be minimized by restricting attention to high percentile effects (i.e., 95th percentile or higher).

Davis, Michael J.↗

Molybdenum Availability Is Key to Nitrate Removal in Contaminated Groundwater Environments

ABSTRACT The concentrations of molybdenum (Mo) and 25 other metals were measured in groundwater samples from 80 wells on the Oak Ridge Reservation (ORR) (Oak Ridge, TN), many of which are contaminated with nitrate, as well as uranium and various other metals. The concentrations of nitrate and uranium were in the ranges of 0.1 μM to 230 mM and <0.2 nM to 580 μM, respectively. Almost all metals examined had significantly greater median concentrations in a subset of wells that were highly contaminated with uranium (≥126 nM). They included cadmium, manganese, and cobalt, which were 1,300- to 2,700-fold higher. A notable exception, however, was Mo, which had a lower median concentration in the uranium-contaminated wells. This is significant, because Mo is essential in the dissimilatory nitrate reduction branch of the global nitrogen cycle. It is required at the catalytic site of nitrate reductase, the enzyme that reduces nitrate to nitrite. Moreover, more than 85% of the groundwater samples contained less than 10 nM Mo, whereas concentrations of 10 to 100 nM Mo were required for efficient growth by nitrate reduction for two Pseudomonas strains isolated from ORR wells and by a model denitrifier, Pseudomonas stutzeri RCH2. Higher concentrations of Mo tended to inhibit the growth of these strains due to the accumulation of toxic concentrations of nitrite, and this effect was exacerbated at high nitrate concentrations. The relevance of these results to a Mo-based nitrate removal strategy and the potential community-driving role that Mo plays in contaminated environments are discussed.

Thorgersen, Michael P.↗

Environmental contaminants of emerging concern in seafood – European database on contaminant levels

Marine pollution gives rise to concern not only about the environment itself but also about the impact on food safety and consequently on public health. European authorities and consumers have therefore become increasingly worried about the transfer of contaminants from the marine environment to seafood. So-called “contaminants of emerging concern” are chemical substances for which no maximum levels have been laid down in EU legislation, or substances for which maximum levels have been provided but which require revision. Adequate information on their presence in seafood is often lacking and thus potential risks cannot be excluded. Assessment of food safety issues related to these contaminants has thus become urgent and imperative. A database ( (www.ecsafeseafooddbase.eu)), containing available information on the levels of contaminants of emerging concern in seafood and providing the most recent data to scientists and regulatory authorities, was developed. The present paper reviews a selection of contaminants of emerging concern in seafood including toxic elements, endocrine disruptors, brominated flame retardants, pharmaceuticals and personal care products, polycyclic aromatic hydrocarbons and derivatives, microplastics and marine toxins. Current status on the knowledge of human exposure, toxicity and legislation are briefly presented and the outcome from scientific publications reporting on the levels of these compounds in seafood is presented and discussed. - Highlights: • Development of a European database regarding contaminants of emerging concern. • Current status on knowledge of human exposure, toxicity and legislation. • Review on the occurrence of contaminants of emerging concern in seafood.

54 ENVIRONMENTAL SCIENCES↗

Establishing a geochemical heterogeneity model for a contaminated vadose zone – Aquifer system

A large set of sediment samples from a 1600 m2 experimental plot within a 2.2 km2 vadose zone and groundwater uranium (VI) plume were subject to physical, chemical, and mineralogic characterization. The plot is being used for field experimentation on U(VI) recharge and transport processes within a persistent groundwater plume that exists in the groundwater-river interaction zone of the Columbia River at the U.S. DOE Hanford site. The samples were obtained during the installation of 35 tightly spaced (10 m separation) groundwater monitoring wells. The characterization measurements for each sample included total contaminant concentrations (U and Cu primarily), bicarbonate extractable U(VI), sequential 238U(VI) contaminant desorption Kd, 233U(VI) adsorption Kd, grain size distribution, surface area, extractable poorly crystalline Fe(III) oxides, and mineralogy. The characterization objective was to inform a conceptual model of coupled processes controlling the anomalous longevity of the plume, and to quantify the spatial heterogeneity of the contaminant inventory and the primary properties effecting reactive transport. Correlations were drawn between chemical, physical, and reaction properties, and Gaussian simulation was used to compute multiple 3-D realizations of extractable U(VI), the 233U(VI) adsorption Kd, and the distribution of the reactive < 2 mm fraction. Adsorbed contaminant U(VI) was highest in the vadose zone and the zone of seasonal water table fluctuation lying at its base. Adsorbed U(VI) was measureable, but low, in the groundwater plume region where very high hydraulic conductivities existed. The distribution of adsorbed U(VI) displayed no apparent correlation with sediment physical or chemical properties. Desorption [238U(IV)] and adsorption [233U(VI)] Kd values showed appreciable differences due to mass transfer controlled surface complexation and the effects of long subsurface residence times. The 233U(VI) adsorption Kd, a combined measure of surface complexation strength and site concentration, was relatively uniform throughout the domain, displaying correlation with fines distribution and surface area. The characterization results revealed U(VI) supplied to the groundwater plume through spatially heterogeneous recharge from residual contamination in the zone of seasonal water table fluctuation, and transport of U(VI) controlled by weak, kinetically-controlled surface complexation in the coarse-textured saturated zone. Geostatistical relationships for the adsorbed contaminant U distribution in the characterization domain allow an extrapolation to inventory at the plume scale, a critical unknown for remedial action.

contaminant heterogeniety, uranium groundwater plu↗

Bacterial Productivity in a Ferrocyanide-Contaminated Aquifer at a Nuclear Waste Site

This study examined potential microbial impacts of cyanide contamination in an aquifer affected by ferrocyanide disposal from nuclear waste processing at the US Department of Energy’s Hanford Site in south-eastern Washington State (USA). We examined bacterial productivity and microbial cell density in groundwater (GW) from wells with varying levels of recent and historical total cyanide concentrations. We used tritiated leucine (3H-Leu) uptake as a proxy for heterotrophic, aerobic bacterial productivity in the GW, and we measured cell density via nucleic acid staining followed by epifluorescence microscopy. Bacterial productivity varied widely, both among wells that had high historical and recent total cyanide (CN−) concentrations and among wells that had low total CN− values. Standing microbial biomass varied less, and was generally greater than that observed in a similar study of uranium-contaminated hyporheic-zone groundwater at the Hanford Site. Our results showed no correlation between 3H-Leu uptake and recent or historical cyanide concentrations in the wells, consistent with what is known about cyanide toxicity with respect to iron speciation. However, additional sampling of the CN− affected groundwater, both in space and time, would be needed to confirm that the CN− contamination is not affecting the GW biota.

Plymale, Andrew (ORCID:0000000333070155)↗

Evaluation and mitigation of trace 210Pb contamination on copper surfaces

Clean materials are required to construct and operate many low-background physics experiments. High-purity copper has found broad use because of its physical properties and availability. In this paper, we describe methods to assay and mitigate Pb-210 contamination on copper surfaces, such as from exposure to environmental radon or coming from bulk impurities. We evaluated the efficacy of wet etching on commercial samples and observed that Po-210 contamination from the copper bulk does not readily pass into solution. During the etch, the polonium appears to trap at the copper-etchant boundary, such that it is effectively concentrated at the copper surface. We observed a different behavior for Pb-210; high-sensitivity measurements of the alpha emissivity versus time indicate the lowest level of Pb-210 contamination ever reported for a commercial copper surface: 0 +/- 12 nBq/cm2 (1-sigma). Additionally, we have demonstrated the effectiveness of mitigating trace Pb-210 and Po-210 surface backgrounds using custom, high-purity electroplating techniques. These approaches were evaluated utilizing assays performed with an XIA UltraLo-1800 alpha spectrometer.

radon, copper, copper cleaning, dark matter, Pb-21↗

Contamination control and assay results for the Majorana Demonstrator ultra clean components

The Majorana Demonstrator is a neutrinoless double beta decay experiment utilizing enriched Ge-76 detectors in 2 separate modules inside of a common solid shield at the Sanford Underground Research Facility. The Demonstrator has utilized world leading assay sensitivities to develop clean materials and processes for producing ultra-pure copper and plastic components. This experiment is now operating, and initial data provide new insights into the success of cleaning and processing. Post production copper assays after the completion of Module 1 showed an increase in U and Th contamination in finished parts compared to starting bulk material. A revised cleaning method and additional round of surface contamination studies prior to Module 2 construction have provided evidence that more rigorous process control can reduce surface contamination. In conclusion, this article describes the assay results and discuss further studies to take advantage of assay capabilities for the purpose of maintaining ultra clean fabrication and process design.

36 MATERIALS SCIENCE↗

Controlling excited-state contamination in nucleon matrix elements

We present a detailed analysis of methods to reduce statistical errors and excited-state contamination in the calculation of matrix elements of quark bilinear operators in nucleon states. All the calculations were done on a 2+1-flavor ensemble with lattices of size 32 3 × 64 generated using the rational hybrid Monte Carlo algorithm at 𝑎 = 0.081 fm and with 𝑀 𝜋 = 312 MeV. The statistical precision of the data is improved using the all-mode-averaging method. We compare two methods for reducing excited-state contamination: a variational analysis and a 2-state fit to data at multiple values of the source-sink separation 𝑡 sep . We show that both methods can be tuned to significantly reduce excited-state contamination and discuss their relative advantages and cost effectiveness. Here a detailed analysis of the size of source smearing used in the calculation of quark propagators and the range of values of 𝑡 sep needed to demonstrate convergence of the isovector charges of the nucleon to the 𝑡 sep → ∞ estimates is presented.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Characterization of the Deltaproteobacteria in contaminated and uncontaminated stream sediments and identification of potential mercury methylators

Microbial communities were examined in surface stream sediments at 5 contaminated sites and 1 control site near Oak Ridge, TN, USA, to identify bacteria that could be contributing to mercury (Hg) methylation. The phylogenetic composition of the sediment bacterial community was examined over 3 quarterly sampling periods (36 samples) using 16S rRNA gene pyrosequencing. Only 3064 sequences (0.85% of the total community) were identified as Deltaproteobacteria, the only group known to methylate Hg, using the Ribosomal Database Project classifier at the 99% confidence threshold. Constrained ordination techniques indicated statistically significant positive linear correlations between Desulfobulbus spp., Desulfonema spp. and Desulfobacca spp. and methyl-Hg concentrations at the Hg-contaminated sites. In contrast, the distribution of organisms related to Byssovorax spp. was significantly correlated to inorganic carbon, nitrate and uranium concentrations but not to Hg or methyl-Hg. Overall, the abundance and richness of Deltaproteobacteria sequences were higher in uncontaminated sediments, while the majority of the members present at the contaminated sites were either known potential metal-reducers/methylators or metal tolerant species. Given the abundance relative to other known Hg methylators and the association with methyl-Hg, Desulfobulbus spp. is considered a prime candidate for involvement in Hg methylation in these streams.

59 BASIC BIOLOGICAL SCIENCES↗