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At least 523 records · Page 29
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Space telescope and optical reverberation mapping project. III. Optical continuum emission and broadband time delays in NGC 5548

We present ground-based optical photometric monitoring data for NGC 5548, part of an extended multiwavelength reverberation mapping campaign. The light curves have nearly daily cadence from 2014 January to July in nine filters (BVRI and ugriz). Combined with ultraviolet data from the Hubble Space Telescope and Swift, we confirm significant time delays between the continuum bands as a function of wavelength, extending the wavelength coverage from 1158 Å to the z band (∼9160 Å). We find that the lags at wavelengths longer than the V band are equal to or greater than the lags of high-ionization-state emission lines (such as He ii λ1640 and λ4686), suggesting that the continuum-emitting source is of a physical size comparable to the inner broad-line region (BLR). The trend of lag with wavelength is broadly consistent with the prediction for continuum reprocessing by an accretion disk with τ∝λ{sup 4/3}. However, the lags also imply a disk radius that is 3 times larger than the prediction from standard thin-disk theory, assuming that the bolometric luminosity is 10% of the Eddington luminosity (L=0.1L{sub Edd}). Using optical spectra from the Large Binocular Telescope, we estimate the bias of the interband continuum lags due to BLR emission observed in the filters. We find that the bias for filters with high levels of BLR contamination (∼20%) can be important for the shortest continuum lags and likely has a significant impact on the u and U bands owing to Balmer continuum emission.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

Isotope anomalies in the FE-group elements in meteorites and connections to nucleosynthesis in AGB stars

We study the effects of neutron captures in AGB stars on “Fe-group” elements, with an emphasis on Cr, Fe, and Ni. These elements show anomalies in {sup 54}Cr, {sup 58}Fe, and {sup 64}Ni in solar system materials, which are commonly attributed to supernovae (SNe). However, as large fractions of the interstellar medium (ISM) were reprocessed in AGB stars, these elements were reprocessed, too. We calculate the effects of such reprocessing on Cr, Fe, and Ni through 1.5 M{sub ⊙} and 3 M{sub ⊙} AGB models, adopting solar and 1/3 solar metallicities. All cases produce excesses of {sup 54}Cr, {sup 58}Fe, and {sup 64}Ni, while the other isotopes are little altered; hence, the observations may be explained by AGB processing. The results are robust and not dependent on the detailed initial isotopic composition. Consequences for other “Fe group” elements are then explored. They include {sup 50}Ti excesses and some production of {sup 46,47,49}Ti. In many circumstellar condensates, Ti quantitatively reflects these effects of AGB neutron captures. Scatter in the data results from small variations (granularity) in the isotopic composition of the local ISM. For Si, the main effects are instead due to variations in the local ISM from different SN sources. The problem of Ca is discussed, particularly with regard to {sup 48}Ca. The measured data are usually represented assuming terrestrial values for {sup 42}Ca/{sup 44}Ca. Materials processed in AGB stars or sources with variable initial {sup 42}Ca/{sup 44}Ca ratios can give apparent {sup 48}Ca excesses/deficiencies, attributed to SNe. The broader issue of galactic chemical evolution is also discussed in view of the isotopic granularity in the ISM.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS2016

Space Telescope and Optical Reverberation Mapping Project. III. Optical Continuum Emission and Broadband Time Delays in NGC 5548

We present ground-based optical photometric monitoring data for NGC 5548, part of an extended multiwavelength reverberation mapping campaign. The light curves have nearly daily cadence from 2014 January to July in ninefilters (BVRI and ugriz). Combined with ultraviolet data from the Hubble Space Telescope and Swift, we confirm significant time delays between the continuum bands as a function of wavelength, extending the wavelength coverage from 1158 Angstrom to the z band (approximately 9160 angstrom). We find that the lags at wavelengths longer than the V band are equal to or greater than the lags of high-ionization-state emission lines (such as He pi lambdal1640 and lambda 4686), suggesting that the continuum-emitting source is of a physical size comparable to the inner broad-line region (BLR). The trend of lag with wavelength is broadly consistent with the prediction for continuum reprocessing by an accretion disk with (tau varies as lambda(exp 4/3)). However, the lags also imply a disk radius that is 3 times larger than the prediction from standardthin-disk theory, assuming that the bolometric luminosity is 10 percent of the Eddington luminosity (L 0.1L(sub Edd)).Using optical spectra from the Large Binocular Telescope, we estimate the bias of the interband continuum lagsdue to BLR emission observed in the filters. We find that the bias for filters with high levels of BLR contamination(20 percent) can be important for the shortest continuum lags and likely has a significant impact on the u and U bandsowing to Balmer continuum emission.

galaxies: active – galaxies: individual (NGC 554↗
DOE OSTI2017

Aging Processes of Silver Mordenite and Silver Functionalized Aerogel in Dry Air, Humid Air and NO/N{sub 2}

One major problem in the treatment of nuclear-fuel reprocessing off-gas streams is the loss of capacity of the adsorbents exposed to off-gas streams containing air, I{sub 2} vapor, H{sub 2}O vapor, NO and NO{sub 2} over extended periods of time. These aging processes decrease the adsorption capacity of the reduced silver exchanged mordenite (Ag{sup 0}Z) and silver functionalized silica aerogel (Ag{sup 0}-aerogel) columns during the long processing time of iodine adsorption. Significant work has been performed over the past few years at ORNL on Ag{sup 0}Z and Ag{sup 0}-aerogel aging. The Ag{sup 0}Z and Ag{sup 0}-aerogel were aged in 4 different gas streams at 150 deg. C for periods of time up to 6 months. The aging samples were then loaded with I{sub 2} to determine the capacity loss after the aging. The results are summaries in Tab. 1. It was found that both Ag{sup 0}Z and Ag{sup 0}-aerogel had different amounts of capacity loss in different gases. For example, 40% and 22% capacity loss were observed for Ag{sup 0}Z and Ag{sup 0}-aerogel when aged in dry air for 6 months, while 78% and 43% capacity loss were observed when aged in 1% NO{sub 1} for 2 months. In addition, it was found that Ag{sup 0}Z and Ag{sup 0}-aerogel had a different capacity loss when aged at the same conditions. For example, after aged in 2% NO{sub 2} for 2 months, Ag{sup 0}Z lost 30% iodine capacity, but there was no capacity loss for Ag{sup 0}- aerogel. The differences in capacity loss should be due to different aging processes occurred when Ag{sup 0}Z and Ag{sup 0}- aerogel were exposed to different gases. The mechanisms of the aging processes have not been determined and need to be studied with proper chemical and physical characterization methods. Towards this objective, experimental work is proposed and on-going to obtain data to determine the mechanisms of the aging processes of Ag{sup 0}Z and Ag{sup 0}-aerogel in different aging gas streams. In addition, models will be developed to describe the deactivation process of the adsorbents when exposed to off gases. The deactivation model will be included in the transport models for predicting the adsorption processes over these long-time periods.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Radioxenon spiked air

Four of the radioactive xenon isotopes ( 131m Xe, 133m Xe, 133 Xe and 135 Xe) with half-lives ranging from 9 h to 12 days are produced from nuclear fission and can be detected from days to weeks following their production and release. Being inert gases, they are readily transported through the atmosphere. Sources for release of radioactive xenon isotopes include operating nuclear reactors via leaks in fuel rods, medical isotope production facilities, and nuclear weapons' detonations. They are not normally released from fuel reprocessing due to the short half-lives. The Comprehensive Nuclear-Test-Ban Treaty has led to creation of the International Monitoring System. The International Monitoring System, when fully implemented, will consist of one component with 40 stations monitoring radioactive xenon around the globe. Monitoring these radioactive xenon isotopes is important to the Comprehensive Nuclear-Test-Ban Treaty in determining whether a seismically detected event is or is not a nuclear detonation. A variety of radioactive xenon quality control check standards, quantitatively spiked into various gas matrices, could be used to demonstrate that these stations are operating on the same basis in order to bolster defensibility of data across the International Monitoring System. This study focuses on Idaho National Laboratory's capability to produce three of the xenon isotopes in pure form and the use of the four xenon isotopes in various combinations to produce radioactive xenon spiked air samples that could be subsequently distributed to participating facilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2000

A High Signal-To-Noise Ultraviolet Spectrum of NGC 7469: New Support for Reprocessing of Continuum Radiation

From 1996 June 10 to 1996 July 29, the International AGN Watch monitored the Seyfert 1 galaxy NGC 7469 using the International Ultraviolet Explorer, the Rossi X-Ray Timing Explorer, and a network of ground-based observatories. On 1996 June 18, in the midst of this intensive monitoring period, we obtained a high signal-to-noise snapshot of the UV spectrum from 1150 to 3300 A, using the Faint Object Spectrograph (FOS) on the Hubble Space Telescope. This spectrum allows us to disentangle the UV continuum more accurately from the broad wings of the emission lines, to identify clean continuum windows free of contaminating emission and absorption, and to deblend line complexes such as Ly(alpha) + N V, C IV + He II + O III], Si III] + C III], and Mg II + Fe II. Using the FOS spectrum as a template, we have fitted and extracted line and continuum fluxes from the IUE monitoring data. The cleaner continuum extractions c o n h the discovery of time delays between the different UV continuum bands by Wanders et al. Our new measurements show delays increasing with wavelength for continuum bands centered at 1485, 1740, and 1825 A, relative to 1315 A with delays of 0.09, 0.28, and 0.36 days, respectively. Like many other Seyfert I galaxies, the UV spectrum of NGC 7469 shows intrinsic, blue-shifted absorption in Ly(alpha), N V, and C IV. Soft X-ray absorption is also visible in archival ASCA X-ray spectra. The strength of the UV absorption, however, is not compatible with a single-zone model in which the same material absorbs both the UV and X-ray light. Similar to other Seyfert galaxies, such as NGC 3516, the UV-absorbing gas in NGC 7469 has a lower ionization parameter and column density than the X-ray-absorbing material. While the UV and X-ray absorption does not arise in the same material, the frequent occurrence of both associated UV absorption and X-ray warm absorbers in the same galaxies suggests that the gas supply for each has a common origin.

Kriss, Gerard A.↗
NASA NTRS2020

Improvements of On-orbit Characterization of Terra MODIS Short-wave Infrared Spectral Bands Out-of-Band Responses

The short-wave infrared (SWIR) bands (5-7, 26) of Terra MODIS, which are co-located with the mid-wav e infrared (MWIR) bands (20-25) on the short and mid-wave infrared (SMIR) Focal Plane Assembly (FPA),have a known issue related to 5.3 μm out-of-band (OOB) thermal leak and electronic crosstalk that was identified prelaunch. As a result, a crosstalk correction algorithm was designed and implemented in the MODIS Level 1B (L1B) calibration. Shortly after the Terra launch, extensive efforts were under taken to help characterize and mitigate the impact due to the OOB response and crosstalk on the SWIR on-orbit calibration and, consequently, the associated L1Bdata products. In addition, special night time day mode (NTDM) operations have been regularly scheduled to derive the crosstalk correction coefficients. Since MODIS does not have a spectral band centered at 5.3 μm, its band 28 (7.325 μm) was chosen as the surrogate sending band to simulate the OOB radiances at 5.3 μm. This was largely based on the measurements from the MODIS Airborne Simulator (MAS) spectrometer field campaigns in the early months after the Terra launch. In the case of Aqua MODIS, the magnitude of the SWIR crosstalk was much smaller and band 25 (4.52 μm) was found to be more effective as the sending band for the crosstalk correction. In recent years, the Terra MODIS photovoltaic (PV) long-wave infrared (LWIR) bands (27-30)electronic crosstalk has increased considerably, especially after the spacecraft safe-mode event occurred in February2016. This accentuated degradation in the PV LWIR performance has also impacted the performance of the SWIR crosstalk correction and thus its calibration and data quality. In this paper, we examine the use of band 25 as the sending band for the Terra MODIS SWIR crosstalk correction and compare its performance with that based on band 28 as the sending band. Results indicate an improvement of on-orbit gain stability for the SWIR calibration and reduced detector to detector and sub-frame to sub-frame striping in the calibrated L1B imagery, especially during the period when the PV LWIR electronic crosstalk has become more severe. This approach has been implemented in the forward production of Terra MODIS Collection 6 and Collection 6.1,starting from July 2019, and is planned to be used for the future reprocessing of MODIS L1B and to help improve the mission-long reflectance calibration and trending stability of the SWIR bands.

MODIS, Terra, Aqua, MODIS, SWIR, calibration, out-↗
DOE OSTI2015

First Industrial Tests of a Drum Monitor Matrix Correction for the Fissile Mass Measurement in Large Volume Historic Metallic Residues with the Differential Die-away Technique

The fissile mass in radioactive waste drums filled with compacted metallic residues (spent fuel hulls and nozzles) produced at AREVA La Hague reprocessing plant is measured by neutron interrogation with the Differential Die-away measurement Technique (DDT. In the next years, old hulls and nozzles mixed with Ion-Exchange Resins will be measured. The ion-exchange resins increase neutron moderation in the matrix, compared to the waste measured in the current process. In this context, the Nuclear Measurement Laboratory (NML) of CEA Cadarache has studied a matrix effect correction method, based on a drum monitor ({sup 3}He proportional counter inside the measurement cavity). A previous study performed with the NML R and D measurement cell PROMETHEE 6 has shown the feasibility of method, and the capability of MCNP simulations to correctly reproduce experimental data and to assess the performances of the proposed correction. A next step of the study has focused on the performance assessment of the method on the industrial station using numerical simulation. A correlation between the prompt calibration coefficient of the {sup 239}Pu signal and the drum monitor signal was established using the MCNPX computer code and a fractional factorial experimental design composed of matrix parameters representative of the variation range of historical waste. Calculations have showed that the method allows the assay of the fissile mass with an uncertainty within a factor of 2, while the matrix effect without correction ranges on 2 decades. In this paper, we present and discuss the first experimental tests on the industrial ACC measurement system. A calculation vs. experiment benchmark has been achieved by performing dedicated calibration measurement with a representative drum and {sup 235}U samples. The preliminary comparison between calculation and experiment shows a satisfactory agreement for the drum monitor. The final objective of this work is to confirm the reliability of the modeling approach and the industrial feasibility of the method, which will be implemented on the industrial station for the measurement of historical wastes. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS1990

The orbital period of 4U/MXB 1636-53 (V801 Arae)

The results of CCD photometry of the optical counterpart (V801 Arae) of the X-ray burst source 4U/MXB 1636-53, obtained between 1984 and 1988 are reported. From these data, and additional measurements discussed previously, a linear orbital ephemeris P(orb) = 3.803878 + or - 0.000022 h covering the interval between 1980 and 1988 is derived. The results confirm that substantial night-to-night variations occur in the shape of the light curve, superposed on the periodic brightness variations. No evidence is found for a relation between orbital phase and the delays of optical bursts relative to the coincident X-ray bursts. The variation with orbital phase of the corresponding ratios of optical to X-ray burst fluences and peak fluxes does not follow the average optical light curve. These results suggest that substantial long-term changes occur in the spatial distribution of reprocessing matter in the binary system.

Van Paradijs, J.↗
DOE OSTI2017

Separation of Actinides from Lanthanides in Molten Fluorides by the Modulated-Current Electrolysis

Recently, the Molten Salt Reactor (MSR) is taking a renewed attraction as one of the reactor systems highlighted by the Generation IV International Forum. It is a non-classical (liquid fuel) system which can be operated as a breeder within the {sup 232}Th-{sup 233}U fuel cycle with the very interesting breeding factor. The necessary precondition for its proper functionality is the online reprocessing within the MSR's fuel cycle. A lot of effort is given to the development of the on-line pyrochemical reprocessing technology. Among the processes considered to be suitable for this process, the electrochemical separations are highlighted. Within this context, it is necessary to study electrochemical behavior of both fissile material and fission products in the molten salt systems and to develop the processes of their extraction from the system at various stages of the whole cycle. In this contribution, the study of the electrochemical separation of U from Gd in the LiF-CaF{sub 2} molten system by the modulated current electrolysis is presented. The study of MSR-related electrochemistry will continue as a part of the new Czech MSR R and D program. The knowledge of the electrochemical behavior of actinides and lanthanides in molten fluorides is necessary to the development of any electrochemical separation process. In our previous work, electrochemical characteristics of uranium, thorium, as well as that of several lanthanides, were measured in LiF-BeF{sub 2} (the basic melt considered for the MSR concept) and Be-free melts (LiF-NaFKF, LiF-NaF, LiF-CaF{sub 2}), and added to available literature data. If the fluoride carrier melt is electrochemically stable enough, it is possible to deposit the element of interest in its basic, metallic state (e.g. uranium in all types of fluoride melts tested) by the electrolysis. In the case of insufficient electrochemical stability of the fluoride melt in which the actinides and lanthanides are dissolved for the experiments, it is possible to use a reactive working electrode made of a material which creates alloys with the element to be deposited. An alloying reaction can shift the deposition potential in a favorable direction and therefore achieve the separation of an element from the system. The use of reactive electrode can also improve the adhesion of the deposit. When two or more electroactive species are present in the system at the same time, the efficiency of their separation by an electrolysis depends on how different the deposition potentials of these two species are. If we input certain modulation to the electrolytic current, we can improve overall result of an electrolytic experiment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Savannah River Site HB-Line Plutonium Oxide Production Process Simulation Model - 17458

The AFS II/Plutonium Oxide Production process is in its initial operational phase at the Savannah River Site's (SRS) HB-Line. The process is new for the facility where it is being performed, but the facility itself has been in use on and off for over 50 years. Beginning this process inside the facility has resulted in multiple process delays, due to both equipment issues and process restrictions. In order to better understand the process and to identify ways to improve facility performance, Savannah River Nuclear Solutions (SRNS), in conjuncture with Newport News Shipbuilding (NNS), developed the HB-Line Process Simulation Model. This tool completely replicates the operations that comprise the HB-Line process and simulates all of the constraints associated with the process. The model realistically accounts for the number of personnel required for a process step, the time required for a process step to occur, rules related to the parallel operation of process steps, and realistic equipment and operational delay data. The result is a tool that allows SRNS to test different scenarios for improving the process throughput, while realistically accounting for potential process delays and restrictions. The tool is currently in use and has allowed SRNS to present to their customer, the National Nuclear Security Administration (NNSA), estimated production capabilities over wide-ranging timetables and assumptions. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Optical and near-infrared spectroscopy of the black hole Swift J1753.5–0127

We report on a multiwavelength observational campaign of the black hole (BH) X-ray binary Swift J1753.5–0127 that consists of an ESO/X-shooter spectrum supported by contemporaneous Swift/X-ray Telescope+Ultra-Violet/Optical Telescope (UVOT) and Australia Telescope Compact Array data. Interstellar medium absorption lines in the X-shooter spectrum allow us to determine E(B−V)=0.45±0.02 along the line of sight to the source. We also report detection of emission signatures of He ii λ4686, Hα, and, for the first time, H i λ10906 and Paβ. The double-peaked morphology of these four lines is typical of the chromosphere of a rotating accretion disk. Nonetheless, the paucity of disk features points toward a low level of irradiation in the system. This is confirmed through spectral energy distribution modeling, and we find that the UVOT+X-shooter continuum mostly stems from the thermal emission of a viscous disk. We speculate that the absence of reprocessing is due to the compactness of an illumination-induced envelope that fails to reflect enough incoming hard X-ray photons back to the outer regions. The disk also marginally contributes to the Compton-dominated X-ray emission and is strongly truncated, with an inner radius about 1000 times larger than the BH's gravitational radius. A near-infrared excess is present, and we associate it with synchrotron radiation from a compact jet. However, the measured X-ray flux is significantly higher than what can be explained by the optically thin synchrotron jet component. We discuss these findings in the framework of the radio-quiet versus X-ray-bright hypothesis, favoring the presence of a residual disk, predicted by evaporation models, that contributes to the X-ray emission without enhancing the radio flux.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

Adsorption Equilibrium and Modeling of Water Vapor on Reduced and Unreduced Silver-Exchanged Mordenite

This work is related to the removal of tritiated water and radioactive iodine from off-gases released during spent nuclear fuel reprocessing. Specifically, it is focused on the adsorption equilibrium of water on reduced silver mordenite (Ag 0 Z), which is the state-of-art solid adsorbent for iodine retention in the off-gas treatment. As the off-gases contain different gas species, including iodine and water, Ag 0 Z would take up iodine and water simultaneously during the adsorption process. Therefore, understanding the adsorption of water on Ag 0 Z is important and necessary for studying the performance of Ag 0 Z in off-gas treatment processes. The isotherms of water (nonradioactive water) on Ag 0 Z were obtained at temperatures of 25, 40, 60, 100, 150, and 200 °C with a continuous-flow adsorption system. The data were analyzed using the Heterogeneous Langmuir and generalized statistical thermodynamic adsorption (GSTA) models, and thermodynamic parameters of the isotherms were obtained from both models. Both models were found capable of describing the isotherms. Isotherms of water on the unreduced silver mordenite (AgZ) were also obtained at 25, 40, and 60 °C and parametrized by the GSTA model. Through the comparison of the isotherms of Ag 0 Z and AgZ, it was found that Ag 0 Z had a higher water adsorption capacity than AgZ. The comparison of their thermodynamic parameters suggested that the interaction of water molecules with the H + in Ag 0 Z was stronger than that with the Ag + in AgZ.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Sigma Team for Advanced Actinide Recycle FY2015 Accomplishments and Directions

The Sigma Team for Minor Actinide Recycle (STAAR) has made notable progress in FY 2015 toward the overarching goal to develop more efficient separation methods for actinides in support of the United States Department of Energy (USDOE) objective of sustainable fuel cycles. Research in STAAR has been emphasizing the separation of americium and other minor actinides (MAs) to enable closed nuclear fuel recycle options, mainly within the paradigm of aqueous reprocessing of used oxide nuclear fuel dissolved in nitric acid. Its major scientific challenge concerns achieving selectivity for trivalent actinides vs lanthanides. Not only is this challenge yielding to research advances, but technology concepts such as ALSEP (Actinide Lanthanide Separation) are maturing toward demonstration readiness. Efforts are organized in five task areas: 1) combining bifunctional neutral extractants with an acidic extractant to form a single process solvent, developing a process flowsheet, and demonstrating it at bench scale; 2) oxidation of Am(III) to Am(VI) and subsequent separation with other multivalent actinides; 3) developing an effective soft-donor solvent system for An(III) selective extraction using mixed N,O-donor or all-N donor extractants such as triazinyl pyridine compounds; 4) testing of inorganic and hybrid-type ion exchange materials for MA separations; and 5) computer-aided molecular design to identify altogether new extractants and complexants and theory-based experimental data interpretation. Within these tasks, two strategies are employed, one involving oxidation of americium to its pentavalent or hexavalent state and one that seeks to selectively complex trivalent americium either in the aqueous phase or the solvent phase. Solvent extraction represents the primary separation method employed, though ion exchange and crystallization play an important role. Highlights of accomplishments include: Confirmation of the first-ever electrolytic oxidation of Am(III) in a noncomplexing aqueous solution and submission of this scientific breakthrough as a paper in Science; The first-ever co-crystallization of Am(VI) with UO 2 (NO 3 ) 2 ∙ 6H 2 O, opening the door to a new approach for separating hexavalent actinides as a group; Results showing that three potentially problematic metals will not present risk in ALSEP; Improvement in ALSEP contactor stripping kinetics to acceptable performance; A comparison of centrifugal contactors vs mixer-settlers showing the former performs better in ALSEP stripping; Synthesis of new mixed N,O-donor extractants with enhanced solubility and strength for selective trivalent actinide extraction; Development of computational methods showing promise in prediction of the selectivity of new extractants for trivalent actinides vs lanthanides; An order-of-magnitude improvement in aqueous Am/Eu complexation selectivity of an alternative macrocyclic stripping agent for ALSEP, potentially enabling an option for an Am product stream free from both Ln and Cm. An alternative aqueous combination of dipicolinate complexant and malonate buffer that may present options for ALSEP and TALSPEAK (Trivalent Actinide-Lanthanide Separations by Phosphorus-reagent Extraction from Aqueous Komplexes) type separations. The ALSEP concept is advancing toward a benchtop flowsheet demonstration planned for FY 2016, and a bench-scale test bed at Idaho National Laboratory (INL) will be employed to demonstrate at least one tandem Am oxidation and separation concept. This report outlines the goals of the STAAR, significance of achieving these goals, STAAR organization around the above aims and questions, recent highlights, and future directions. The report also includes a listing of publications, reports, patents, and dissertations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS2013

Does Oxygen Isotopic Heterogeneity in Refractory Inclusions and Their Wark-Lovering Rims Record Nebular Repressing?

Large systematic variations in O-isotopic compositions found within individual mineral layers of rims surrounding Ca-, Al-rich inclusions (CAIs) and at the margins of some CAIs imply formation from distinct environments [e.g., 1-3]. The O-isotope compositions of many CAIs preserve a record of the Solar nebula gas believed to initially be O-16-rich (delta O-17 less than or equal to -25%0) [4-5]. Data from a recent study of the compact Type A Allende CAI, A37, preserve a diffusion profile in the outermost ~70 micrometers of the inclusion and show greater than 25%0 variations in delta O-17 within its ~100 micrometer-thick Wark-Lovering rim (WL-rim) [3]. This and comparable heterogeneity measured in several other CAIs have been explained by isotopic mixing between the O-16-rich Solar reservoir and a second O-16-poor reservoir (probably nebular gas) with a planetary-like isotopic composition, e.g., [1,2,3,6]. However, there is mineralogical and isotopic evidence from the interiors of CAIs, in particular those from Allende, for parent body alteration. At issue is how to distinguish the record of secondary reprocessing in the nebula from that which occurred on the parent body. We have undertaken the task to study a range of CAI types with varying mineralogies, in part, to address this problem.

Simon, J. I.↗
DOE OSTI2016

Report on Concepts & Approaches for SSBD for eCHEM

The verification of special nuclear material (SNM) in spent fuel pyroprocessing is an important safeguards challenge. The detection of spontaneous fission (SF) neutrons from curium is an accepted, non-destructive technique that has been applied to verify special nuclear material (SNM) content in used fuel and other materials in the fuel cycle. The nuclear material accounting (NMA) technique at the Korea Atomic Energy Research Institute’s Reference Engineering-scale Pyroprocessing Facility (REPF) is based on the Cm balance technique. Several publications have demonstrated the safeguards benefit from using process monitoring (PM) on nuclear facilities as a complementary measure to NMA. More recently, this concept was expanded and preliminarily demonstrated for pyroprocessing. The concept of Signature Based Safeguards (SBS) is part of this expansion, and is built around the interpretation of input from various sensors in a declared facility coupled with complementary NMA methods to increase confidence and lower standard error inventory differences (SEID). The SBS methodology was conceptually developed and relies on near real time analysis of process monitoring data to detect material diversion complemented by robust containment and surveillance (C/S) measures. This work demonstrates one example of how the SBS framework can be used in the electrorefiner. In this SBS application, a combination of cyclic voltammetry (CV) and neutron counting is applied to track and monitor Pu mass balance. The main purpose of this experiment is to determine if meaningful information can be gained from CV measurements with regard to the Mg/Gd ratio. This data will be coupled with ICP-MS to verify Gd concentrations and analyzed for statistical significance. It is expected the CV data will register a significant change under the off-normal operating conditions. Knowing how to identify and interpret those changes may help inform how to target more traditional neutron counting methods, which could support a more efficient safeguards system. The experimental results will be compared with theoretical calculations and the ERAD simulations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

Non-Ideality in Solvent Extraction Systems: PNNL FY 2014 Status Report

The overall objective of this project is to develop predictive modeling capabilities for advanced fuel cycle separation processes by gaining a fundamental quantitative understanding of non-ideality effects and speciation in relevant aqueous and organic solutions. Aqueous solutions containing actinides and lanthanides encountered during nuclear fuel reprocessing have high ionic strength and do not behave as ideal solutions. Activity coefficients must be calculated to take into account the deviation from ideality and predict their behavior. In FY 2012-2013, a convenient method for determining activity effects in aqueous electrolyte solutions was developed. Our initial experiments demonstrated that water activity and osmotic coefficients of the electrolyte solutions can be accurately measured by the combination of two techniques, a Water Activity Meter and Vapor Pressure Osmometry (VPO). The water activity measurements have been conducted for binary lanthanide solutions in wide concentration range for all lanthanides (La-Lu with the exception of Pm). The osmotic coefficients and Pitzer parameters for each binary system were obtained by the least squares fitting of the water activity data. However, application of Pitzer model for the quantitative evaluation of the activity effects in the multicomponent mixtures is difficult due to the large number of the required interaction parameters. In FY 2014, the applicability of the Bromley model for the determination of the Ln(NO 3 ) 3 activity coefficients was evaluated. The new Bromley parameters for the binary Ln(NO 3 ) 3 electrolytes were obtained based on the available literature and our experimental data. This allowed for the accurate prediction of the Ln(NO 3 ) 3 activity coefficients for the binary Ln(NO 3 ) 3 electrolytes. This model was then successfully implemented for the determination of the Ln(NO 3 ) 3 activity coefficients in the ternary Nd(NO 3 ) 3 /HNO 3 /H2O, Eu(NO 3 ) 3 /HNO 3 /H 2 O, and Eu(NO 3 ) 3 /NaNO 3 /H 2 O systems. The main achievement of this work is the verified pathway for the estimation of the activity coefficients in the multicomponent aqueous electrolyte systems. The accurate Bromley electrolytes contributions obtained in this work for the entire series of lanthanide(III) nitrates (except Pm) can be applied for predicting activity coefficients and non-ideality effects for multi-component systems containing these species. This work also provides the proof-of-principle of extending the model to more complex multicomponent systems. Moreover, this approach can also be applied to actinide-containing electrolyte systems, for determination of the activity coefficients in concentrated radioactive solutions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

High‐Frequency Intermittency in Observed and Model‐Simulated Precipitation

Abstract A newly reprocessed, bias‐corrected version of hourly satellite observations that provides global coverage of precipitation at high space‐time resolution is evaluated and compared with climate model simulations. Irregular subdaily fluctuations are the dominant component around the world, greater than variance of daily mean precipitation, and much greater than variance associated with the mean diurnal cycle of precipitation. Irregular subdaily fluctuations of precipitation are severely underestimated by models, even after taking into account the observational “error bars” implied by different space‐time resolutions. Variance of daily mean precipitation is less severely underestimated. Although mean diurnal cycle amplitudes vary among the models, this component is but a small part of total precipitation variance. Therefore, the total precipitation variance is significantly underestimated by models in general. Further exploration of model‐data discrepancies in precipitation at high‐time frequency may lead to new and useful climate model diagnostics.

54 ENVIRONMENTAL SCIENCES↗