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All sources NASA NTRS DOE OSTI

DOE OSTI2021

Rapid quantitative analysis of trace elements in plutonium alloys using a handheld laser-induced breakdown spectroscopy (LIBS) device coupled with chemometrics and machine learning

Here, we present the first reported quantification of trace elements in plutonium via a portable laser-induced breakdown spectroscopy (LIBS) device and demonstrate the use of chemometric analysis to enhance the handheld device's sensitivity and precision. Quantification of trace elements such as iron and nickel in plutonium metal via LIBS is a challenging problem due to the complex nature of the plutonium optical emission spectra. While rapid analysis of plutonium alloys has been demonstrated using portable LIBS devices, such as the SciAps Z300, their detection limits for trace elements are severely constrained by their achievable pulse power and length, light collection optics, and detectors. In this paper, analytical methods are evaluated as a means to circumvent the detection constraints. Three chemometric methods often used in analytical spectroscopy are evaluated; principal component regression, partial least-squares regression, and artificial neural networks. These models are evaluated based on goodness-of-fit metrics, root mean-squared error, and their achievable limits of detection (LoDs). Partial least squares proved superior for determining content of iron and nickel in plutonium metal, yielding LoDs of 15 and 20 ppm, respectively. These results of identifying the undesirable trace elements in plutonium components are critical for applications such as fabricating radioisotope thermoelectric generators or nuclear fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Temporal evolution of Pu and Cs sediment contamination in a seasonally stratified pond

There remains a lack of knowledge regarding ecosystem transfer, transport processes, and mechanisms, which influence the long-term mobility of Pu-239 and Cs-137 in natural environments. Monitoring the distribution and migration of trace radioisotopes as ecosystem tracers has the potential to provide insight into the underlying mechanisms of geochemical cycles. This study investigated the distribution of anthropogenic radionuclides Pu-239 and Cs-137 along with total organic carbon, iron, and trace element in contaminated sediments of Pond B at the Savannah River Site (SRS). Pond B received reactor cooling water from 1961 to 1964, and trace amounts of Pu-239 and Cs-137 during operations. Our study collected sediment cores to determine concentrations of Pu-239, Cs-137, and major and minor elements in solid phase, pore water and an electrochemical method was used on wet cores to determine dissolved elemental concentrations. More than 50 years after deposition, Pu-239 and Cs-137 in sediments are primarily located in the upper 5 cm in area where deposition of particulate-bound contaminants was prevalent and located between 5 and 10 cm in areas of high sedimentation, showing a limited migration of Pu-239 and Cs-137. A Factor analysis demonstrated different sediment facies across the pond resulting in a range of geochemical processes controlling accumulation of Pu and Cs. Highest concentrations appear to be controlled by particulate input from the influent canal, dominated by clay, silt, and sand minerals bearing Fe. Elevated Pu-239 in the sediments were observed in areas with high organic matter and higher deposition rate relative to the Pond B system near the outlet indicating strong association of Pu with OM and particulates. Therefore, organic matter cycling likely plays a role in Pu redistribution between sediment and overlying pond water, and deposition in organic rich sediments accumulating near the outlet. Though Pu appears to have been distributed throughout the pond, Cs-137 concentrations remained the highest near the influent canal.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

NASA NTRS2001

Clustered DNA damages induced by high and low LET radiation, including heavy ions

Clustered DNA damages--here defined as two or more lesions (strand breaks, oxidized purines, oxidized pyrimidines or abasic sites) within a few helical turns--have been postulated as difficult to repair accurately, and thus highly significant biological lesions. Further, attempted repair of clusters may produce double strand breaks (DSBs). However, until recently, there was no way to measure ionizing radiation-induced clustered damages, except DSB. We recently described an approach for measuring classes of clustered damages (oxidized purine clusters, oxidized pyrimidine clusters, abasic clusters, along with DSB). We showed that ionizing radiation (gamma rays and Fe ions, 1 GeV/amu) does induce such clusters in genomic DNA in solution and in human cells. These studies also showed that each damage cluster results from one radiation hit (and its track), thus indicating that they can be induced by very low doses of radiation, i.e. two independent hits are not required for cluster induction. Further, among all complex damages, double strand breaks comprise--at most-- ~20%, with the other clustered damages being at least 80%.

NASA Discipline Radiation Health↗

NASA NTRS2016

Performance Testing of a High Temperature Linear Alternator for Stirling Convertors

The NASA Glenn Research Center has conducted performance testing of a high temperature linear alternator (HTLA) in support of Stirling power convertor development for potential future Radioisotope Power Systems (RPS). The high temperature linear alternator is a modified version of that used in Sunpower's Advanced Stirling Convertor (ASC), and is capable of operation at temperatures up to 200 deg. Increasing the temperature capability of the linear alternator could expand the mission set of future Stirling RPS designs. High temperature Neodymium-Iron-Boron (Nd-Fe-B) magnets were selected for the HTLA application, and were fully characterized and tested prior to use. Higher temperature epoxy for alternator assembly was also selected and tested for thermal stability and strength. A characterization test was performed on the HTLA to measure its performance at various amplitudes, loads, and temperatures. HTLA endurance testing at 200 deg is currently underway.

Radioisotope Power System↗

NASA NTRS2016

Performance Testing of a High Temperature Linear Alternator for Stirling Convertors

The NASA Glenn Research Center has conducted performance testing of a high temperature linear alternator (HTLA) in support of Stirling power convertor development for potential future Radioisotope Power Systems (RPS). The high temperature linear alternator is a modified version of that used in Sunpowers Advanced Stirling Convertor (ASC), and is capable of operation at temperatures up to 200 C. Increasing the temperature capability of the linear alternator could expand the mission space of future Stirling RPS designs. High temperature Neodymium-Iron-Boron (Nd-Fe-B) magnets were selected for the HTLA application, and were fully characterized and tested prior to uses. Higher temperature epoxy for alternator assembly was also selected and tested for thermal stability and strength. A characterization test was performed on the HTLA to measure its performance at various amplitudes, loads, and temperatures. HTLA endurance testing at 200 C is currently underway.

Alternator Test Rig↗

NASA NTRS1999

Phototrophs in high-iron-concentration microbial mats: physiological ecology of phototrophs in an iron-depositing hot spring

At Chocolate Pots Hot Springs in Yellowstone National Park the source waters have a pH near neutral, contain high concentrations of reduced iron, and lack sulfide. An iron formation that is associated with cyanobacterial mats is actively deposited. The uptake of [(14)C]bicarbonate was used to assess the impact of ferrous iron on photosynthesis in this environment. Photoautotrophy in some of the mats was stimulated by ferrous iron (1.0 mM). Microelectrodes were used to determine the impact of photosynthetic activity on the oxygen content and the pH in the mat and sediment microenvironments. Photosynthesis increased the oxygen concentration to 200% of air saturation levels in the top millimeter of the mats. The oxygen concentration decreased with depth and in the dark. Light-dependent increases in pH were observed. The penetration of light in the mats and in the sediments was determined. Visible radiation was rapidly attenuated in the top 2 mm of the iron-rich mats. Near-infrared radiation penetrated deeper. Iron was totally oxidized in the top few millimeters, but reduced iron was detected at greater depths. By increasing the pH and the oxygen concentration in the surface sediments, the cyanobacteria could potentially increase the rate of iron oxidation in situ. This high-iron-content hot spring provides a suitable model for studying the interactions of microbial photosynthesis and iron deposition and the role of photosynthesis in microbial iron cycling. This model may help clarify the potential role of photosynthesis in the deposition of Precambrian banded iron formations.

NASA Discipline Exobiology↗

NASA NTRS1998

Effects of exposure to different types of radiation on behaviors mediated by peripheral or central systems

The effects of exposure to ionizing radiation on behavior may result from effects on peripheral or on central systems. For behavioral endpoints that are mediated by peripheral systems (e.g., radiation-induced conditioned taste aversion or vomiting), the behavioral effects of exposure to heavy particles (56Fe, 600 MeV/n) are qualitatively similar to the effects of exposure to gamma radiation (60Co) and to fission spectrum neutrons. For these endpoints, the only differences between the different types of radiation are in terms of relative behavioral effectiveness. For behavioral endpoints that are mediated by central systems (e.g., amphetamine-induced taste aversion learning), the effects of exposure to 56Fe particles are not seen following exposure to lower LET gamma rays or fission spectrum neutrons. These results indicate that the effects of exposure to heavy particles on behavioral endpoints cannot necessarily be extrapolated from studies using gamma rays, but require the use of heavy particles.

NASA Discipline Radiation Health↗

NASA NTRS2005

Overview of NASA Magnet and Linear Alternator Research Efforts

The Department of Energy, Lockheed Martin, Stirling Technology Company, and NASA Glenn Research Center are developing a high-efficiency, 110 watt Stirling Radioisotope Generator (SRG110) for NASA Space Science missions. NASA Glenn is conducting in-house research on rare earth permanent magnets and on linear alternators to assist in developing a free-piston Stirling convertor for the SRG110 and for developing advanced technology. The permanent magnet research efforts include magnet characterization, short-term magnet aging tests, and long-term magnet aging tests. Linear alternator research efforts have begun just recently at GRC with the characterization of a moving iron type linear alternator using GRC's alternator test rig. This paper reports on the progress and future plans of GRC's magnet and linear alternator research efforts.

Geng, Steven M.↗

NASA NTRS2005

Overview of NASA Magnet and Linear Alternator Research Efforts

Geng, Steven M.↗

NASA NTRS1987

Distributed reacceleration of cosmic rays

We develop a model in which cosmic rays, in addition to their initial acceleration by a strong shock, are continuously reaccelerated (e.g., by weak shocks) while propagating through the galaxy. The equations describing this acceleration scheme are solved analytically (approximating ionization losses by a cutoff) and numerically. Solutions for the spectra of primary and secondary cosmic rays are given in a closed analytic form, and they allow a rapid search in parameter space for viable propagation models with distributed reacceleration included. The observed boron-to-carbon ratio can be reproduced by the reacceleration theory over a range of escape parameters, some of them quite different from the standard "leaky box" model. It is also shown that even a very modest amount of reacceleration by strong shocks causes the boron-to carbon ratio to level off at sufficiently high energies, and this effect may be observed in the CRNE data. Several other curiosities in the data may be explained naturally if a modest amount of distributed reacceleration is invoked, including (a) the apparent truncation at low energy in the otherwise exponential pathlength distribution associated with the leaky box model, (b) the sub-iron isotopic anomalies and other effects noted by Silberberg et al., and (c) the discrepancy between the reported 10Be lifetime and the lifetime of cosmic rays in the dense strata of the galactic disk.

NASA Discipline Radiation Health↗

NASA NTRS1988

Does iron inhibit cryptoendolithic microbial communities?

Photosynthetic activity of three cryptoendolithic microbial communities was studied under controlled conditions in the laboratory. In two of these communities, the dominant organisms were lichens, collected from Linnaeus Terrace and from Battleship Promontory. The third community, dominated by cyanobacteria, was collected from Battleship Promontory. Both sites are in the ice-free valleys of southern Victoria Land. Previous efforts have shown how physical conditions can influence metabolic activity in endolithic communities (Kappen and Friedmann 1983; Kappen, Friedmann, and Garty 1981; Vestal, Federle, and Friedmann 1984). Biological activity can also be strongly influenced by the chemical environment. Inorganic nutrients such as nitrate, ammonia, and phosphate are often limiting factors, so their effects on photosynthetic carbon-14 bicarbonate incorporation were investigated. Iron and manganese are two metals present in Linnaeus Terrace and Battleship Promontory sandstones, and their effects on photosynthesis were also studied. The results may add to our understanding of biogeochemical interactions within this unique microbial community.

Non-NASA Center↗

DOE OSTI2025

Actinium purification from elemental components of stainless steel and aluminum

Radioisotopes of actinium are valuable because of their potential use in the medical industry. Actinium-225 shows promise for treating disease—like cancer—via targeted alpha therapy (TAT), and the longer-lived actinium-227 is the parent of two radionuclides with potential application in TAT radiopharmaceuticals, thorium-227 and radium-223. Continuing progress in the development of these medical applications requires robust and diverse methods for extracting and purifying actinium from a wide range of matrices. Further, to define the strengths and limitations of separation methods commonly employed in actinium processing, we characterized the performance of ion exchange and extraction chromatographic steps for removing contaminants found in stainless steel (chromium, iron, nickel, and silicon) and aluminum from actinium-227. While AG-MP1 anion exchange resin with HCl (aq) successfully removed iron, cation exchanger AG 50W-X8 removed most other contaminants. The most persistent contaminant was aluminum, which was removed using a DGA Normal extraction resin. These results are presented within the context of applying that methodology toward actinium purification strategies.

36 MATERIALS SCIENCE↗

NASA NTRS2003

Stirling Convertor Technologies Being Developed for a Stirling Radioisotope Generator

The Department of Energy, Lockheed Martin, Stirling Technology Company (STC), and the NASA Glenn Research Center are developing a high-efficiency Stirling Radioisotope Generator (SRG) for NASA space science missions. The SRG is being developed for multimission use, including providing electric power for unmanned Mars rovers and deep space missions. On Mars, rovers with SRGs would be used for missions that might not be able to use photovoltaic power systems, such as exploration at high Martian latitudes and missions of long duration. The projected SRG system efficiency of 23 percent will reduce the required amount of radioisotope by a factor of 4 or more in comparison to currently used Radioisotope Thermoelectric Generators. The Department of Energy recently named Lockheed Martin as the system integration contractor. Lockheed Martin has begun to develop the SRG engineering unit under contract to the Department of Energy, and has contract options to develop the qualification unit and the first flight units. The developers expect the SRG to produce about 114 Wdc at the beginning of mission, using two opposed Stirling convertors and two General Purpose Heat Source modules. STC previously developed the Stirling convertor under contract to the Department of Energy and is now providing further development as a subcontractor to Lockheed Martin. Glenn is conducting an in-house technology project to assist in developing the convertor for space qualification and mission implementation. A key milestone was recently reached with the accumulation of 12 000 hr of long-term aging on two types of neodymium-iron boron permanent magnets. These tests are characterizing any possible aging in the strength or demagnetization resistance of the magnets used in the linear alternator. Preparations are underway for a thermal/vacuum system demonstration and unattended operation during endurance testing of the 55-We Technology Demonstration Convertors. In addition, Glenn is developing a charging system for the convertors to ensure clean fills of the helium working fluid and to monitor levels of any possible contaminants at different test intervals. Possible oxidation effects depend on the level of any oxygen contamination-regenerator materials and displacer radiation shields are now being evaluated for possible oxidation effects.

Thieme, Lanny G.↗

DOE OSTI2020

Innovations in Sustainable Passive Wastewater Treatment - 20236

Sustainable water treatment systems, engineered to mimic natural processes and utilize natural materials, yield economic and environmental benefits through reductions in long term operational inputs, including: power, chemicals, and labor. Golder is an industry leader in the development and implementation of sustainable technologies at operating and closed mines. We continue to innovate these technologies and customize solutions to meet client needs by applying past experience and focused research. Sustainable (or passive) water treatment systems include ponds, wetlands, flow-through natural media beds, and limestone drains. These systems can blend in with a natural environment, are highly cost-effective for long-term water treatment, and can outcompete traditional active treatment technologies. Application of sustainable technologies relative to active technologies can be influenced by the influent water matrix, effluent limitations, flow rate of water requiring treatment, and available land area. In this presentation, four Golder-developed systems are reviewed as case studies, demonstrating our continued progressive approach to advancing sustainable water treatment technologies to meet industry needs. These case studies focus on design innovations and operational performance from data collected from the operational systems. Resources (power, chemicals, labor) required for the operation of each case study are compared with those that would be required for operation of their active treatment technology alternatives. - Case Study 1 presents an anaerobic biochemical reactor (BCR), a technology typically implemented for metals treatment and acid neutralization, for the treatment of sulfate to low concentrations (<250 mg/L). Active treatment via reverse osmosis (RO) membrane filtration is typically required for treatment of sulfate to similar concentrations, this innovation provides potential for sustainable treatment to replace the need for energy, chemical, labor, and waste (brine) intensive RO treatment for specific applications. Magnetite waste rock materials from the site were upcycled for use in this system to provide sequestration of the sulfide generated in the BCR. - Case Study 2 examines another novel application of the conventional BCR, modified for the removal of radionuclides and metals (uranium, radium, and selenium) at a closed uranium mine. - Case Study 3 presents implementation of sustainable treatment for mine drain water from a historic mine site, now a state park with around 100,000 visitors per year. The system includes a pond, wetland, and manganese removal bed surrounded by public trails designed to maintain the character of the park. The system treats for arsenic, iron, and manganese at relatively high flows (up to 1,200 gpm), with large seasonal fluctuations in flow and quality. - Case Study 4 is a unique project for which Golder is currently designing a sustainable treatment system, with no energy input, to treat nitrate in mine water post-closure at a site near the arctic circle. In this unprecedented application, climate, management of freshet, and space availability presented substantial technical challenges. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS2003

Three-Dimensional Magnetic Analysis Technique Developed for Evaluating Stirling Convertor Linear Alternators

The Department of Energy, the Stirling Technology Company (STC), and the NASA Glenn Research Center are developing Stirling convertors for Stirling radioisotope generators to provide electrical power for future NASA deep space missions. STC is developing the 55-We technology demonstration convertor (TDC) under contract to the Department of Energy. The Department of Energy recently named Lockheed Martin as the system integration contractor for the Stirling radioisotope generator development project. Lockheed Martin will develop the Stirling radioisotope generator engineering unit and has contract options to develop the qualification unit and the first flight unit. Glenn s role includes an in-house project to provide convertor, component, and materials testing and evaluation in support of the overall power system development. As a part of this work, Glenn has established an in-house Stirling research laboratory for testing, analyzing, and evaluating Stirling machines. STC has built four 55-We convertors for NASA, and these are being tested at Glenn. A cross-sectional view of the 55-We TDC is shown in the figure. Of critical importance to the successful development of the Stirling convertor for space power applications is the development of a lightweight and highly efficient linear alternator. In support, Glenn has been developing finite element analysis and finite element method tools for performing various linear alternator thermal and electromagnetic analyses and evaluating design configurations. A three-dimensional magnetostatic finite element model of STC's 55-We TDC linear alternator was developed to evaluate the demagnetization fields affecting the alternator magnets. Since the actual linear alternator hardware is symmetric to the quarter section about the axis of motion, only a quarter section of the alternator was modeled. The components modeled included the mover laminations, the neodymium-iron-boron magnets, the stator laminations, and the copper coils. The three-dimensional magnetostatic model was then coupled with a circuit simulator model of the alternator load and convertor controller. The coupled model was then used to generate alternator terminal voltage and current predictions. The predicted voltage and current waveforms agreed well with the experimental data, which tended to validate the accuracy of the coupled model. The model was then used to generate predictions of the demagnetization fields acting on the alternator magnets for the alternator under load. The preliminary model predictions indicate that the highest potential for demagnetization is along the inside surface of the uncovered magnets. The demagnetization field for the uncovered magnets when the mover is positioned at the end of a stroke is higher than it is when the mover is at the position of maximum induced voltage or maximum alternator current. Assuming normal load conditions, the model predicted that the onset of demagnetization is most likely to occur for magnet temperatures above 101 C.

Geng, Steven M.↗

DOE OSTI2020

GeoMelt{sup R} In-Container Vitrification (ICV){sup TM} for Fukushima Daiichi Water Treatment Secondary Wastes - 20212

The Japanese government is supporting development work implemented jointly by Veolia subsidiaries Kurion Japan, K.K., Veolia Nuclear Solutions (VNS), Inc., and Veolia Nuclear Solutions Federal Services, LLC for treating radioactive waste generated from Fukushima Daiichi Nuclear Power Station (NPS) water treatment using the GeoMelt{sup TM} In-Container Vitrification (ICV){sup TM} technology. The initial work consisted of glass formulation and engineering-scale testing which was completed in 2018, in the frame of an IRID (International Research Institute for Nuclear Decommissioning) program as part of a project subsidized by Japan's Ministry of Economy, Trade and Industry (METI). The Fukushima Daiichi NPS Mid- and Long-Term Road-map requires investigation of methods to stabilize solid wastes (and to immobilize radioisotopes in the wastes) generated as a result of emergency response and decommissioning activities. Cooling water treatment has resulted in a significant amount of solid and slurry secondary wastes (mostly adsorbents and ion-exchange materials) which will require processing at some point. GeoMelt{sup R} ICV{sup TM} is a joule-heated melter technology which uses a refractory-lined single-use container combining the melter and disposal container. There is no pouring required nor concerns with refractory corrosion which allows the process to accommodate a wide range of waste chemistries and high waste loadings. The testing described here consisted of three engineering-scale melts, each processing between 212 kg and 240 kg of waste simulants, glass formers, and non-radioactive cesium (Cs) and strontium (Sr) tracers. Continuous isokinetic stack sampling of off-gas emissions was performed for each test in order to calculate Cs and Sr retention in the glass wasteform. Single-pass retention of Cs in the final glass wasteform ranged from 91.46 to 99.30%, and single-pass retention of Sr ranged from 99.76 to 100%. Planned particulate recycle will increase these retention levels. Melt 1 processed a mixture of KUR-EH (a zeolite-based ion-exchange material), simulated Advanced Liquid Processing System (ALPS) Carbonate and Iron Slurries, and glass additives. Melt 2 processed a mixture of KUR-EH, KUR-TSG (a titanate-based adsorbent), and glass additives. Melt 3 processed a mixture of KUR-EH, simulated barium sulfate/iron ferrocyanide sludge (AREVA sludge), and glass additives. Waste loadings for these melts ranged from 70 weight percent (wt%) to 82 wt%. Vitrification produces a waste form much denser than the stored water treatment secondary waste wastes, resulting in significant volume reduction. Volume reductions for the three tests ranged from 74 to 79 vol%. Vitrification produces a chemically durable wasteform. Pacific Northwest National Laboratory (PNNL) tested three glass samples from each engineering-scale melt) by the Materials Characterization Center 1 (MCC-1) test, an international standard leach test of the chemical durability of nuclear waste glasses. PNNL also obtained one U.S. reference glass (EA Glass) and two Japan reference glasses P0798) and tested these under the same MCC-1 conditions (90 deg. C, 10 m-1, DIW, and 7, 14, 28-day) as the GeoMelt{sup R} ICV{sup TM} glasses. The GeoMelt{sup R} ICV{sup TM} glasses exhibited lower total normalized releases and 14- to 28-day normalized release rates than the three reference glasses. These results suggest that the GeoMelt{sup R} ICV{sup TM} glasses have durabilities on par with high-level waste glasses under standard test conditions. Post-melt process sampling and analysis indicated no Cs migration into the melter refractory materials and very little deposition of Cs or Sr onto the melter hood or off-gas piping internals. The results of the testing indicated good Cs retention in the glass, high volume reduction and waste loadings, and excellent chemical durability. These factors are important to minimize treatment costs and to protect workers and the environment. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗