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At least 577 records · Page 32
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Sorption Modeling and Verification for Off-Gas Treatment

The project has made progress toward developing a comprehensive modeling capability for the capture of target species in off gas evolved during the reprocessing of nuclear fuel. The effort has integrated experimentation, model development, and computer code development for adsorption and absorption processes. For adsorption, a modeling library has been initiated to include (a) equilibrium models for uptake of off-gas components by adsorbents, (b) mass transfer models to describe mass transfer to a particle, diffusion through the pores of the particle and adsorption on the active sites of the particle, and (c) interconnection of these models to fixed bed adsorption modeling which includes advection through the bed. For single-component equilibria, a Generalized Statistical Thermodynamic Adsorption (GSTA) code was developed to represent experimental data from a broad range of isotherm types; this is equivalent to a Langmuir isotherm in the two-parameter case, and was demonstrated for Kr on INL-engineered sorbent HZ PAN, water sorption on molecular sieve A sorbent material (MS3A), and Kr and Xe capture on metal-organic framework (MOF) materials. The GSTA isotherm was extended to multicomponent systems through application of a modified spreading pressure surface activity model and generalized predictive adsorbed solution theory; the result is the capability to estimate multicomponent adsorption equilibria from single-component isotherms. This advance, which enhances the capability to simulate systems related to off-gas treatment, has been demonstrated for a range of real-gas systems in the literature and is ready for testing with data currently being collected for multicomponent systems of interest, including iodine and water on MS3A. A diffusion kinetic model for sorbent pellets involving pore and surface diffusion as well as external mass transfer has been established, and a methodology was developed for determining unknown diffusivity parameters from transient uptake data. Two parallel approaches have been explored for integrating the kernels described above into a mass-transport model for adsorption in fixed beds. In one, the GSTA isotherm kernel has been incorporated into the MOOSE framework; in the other approach, a focused finite-difference framework and PDE kernels have been developed. Issues, including oscillatory behavior in MOOSE solutions to advection-diffusion problems, and opportunities have been identified for each approach, and a path forward has been identified toward developing a stronger modeling platform. Experimental systems were established for collection of microscopic kinetics and equilibria data for single and multicomponent uptake of gaseous species on solid sorbents. The systems, which can operate at ambient temperature to 250°C and dew points from -69 to 17°C, are useful for collecting data needed for modeling performance of sorbents of interest. Experiments were conducted to determine applicable models and parameters for isotherms and mass transfer for water and/or iodine adsorption on MS3A. Validation experiments were also conducted for water adsorption on fixed beds of MS3A. For absorption, work involved modeling with supportive experimentation. A dynamic model was developed to simulate CO 2 absorption with chemical reaction using high alkaline content water solutions. A computer code was developed to implement the model based upon transient mass and energy balances. Experiments were conducted in a laboratory-scale column to determine model parameters. The influence of geometric parameters and operating variables on CO 2 absorption was studied over a wide range of conditions. This project has resulted in 7 publications, with 3 manuscripts in preparation. Also, 15 presentations were given at national meetings of ANS and AIChE and at Material Recovery and Waste Forms Campaign Working Group meetings.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Optimized Sampling Strategies For Non-Proliferation Monitoring: Report

Concentration data collected from the 2013 H-Canyon effluent reprocessing experiment were reanalyzed to improve the source term estimate. When errors in the model-predicted wind speed and direction were removed, the source term uncertainty was reduced to 30% of the mean. This explained the factor of 30 difference between the source term size derived from data at 5 km and 10 km downwind in terms of the time history of dissolution. The results show a path forward to develop a sampling strategy for quantitative source term calculation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Chemical durability and degradation mechanisms of HT9 based alloy waste forms with variable Zr content

In Corrosion studies were undertaken on alloy waste forms that can result from advanced electrometallurgical processing techniques to better classify their durability and degradation mechanisms. The waste forms were based on the RAW3-(URe) composition, consisting primarily of HT9 steel and other elemental additions to simulate nuclear fuel reprocessing byproducts. The solution conditions of the corrosion studies were taken from an electrochemical testing protocol, and meant to simulate conditions in a repository. The alloys durability was examined in alkaline and acidic brines.

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

Stationary Liquid Fuel Fast Reactor

For effective burning of hazardous transuranic (TRU) elements of used nuclear fuel, a transformational advanced reactor concept named SLFFR (Stationary Liquid Fuel Fast Reactor) was proposed based on stationary molten metallic fuel. The fuel enters the reactor vessel in a solid form, and then it is heated to molten temperature in a small melting heater. The fuel is contained within a closed, thick container with penetrating coolant channels, and thus it is not mixed with coolant nor flow through the primary heat transfer circuit. The makeup fuel is semi- continuously added to the system, and thus a very small excess reactivity is required. Gaseous fission products are also removed continuously, and a fraction of the fuel is periodically drawn off from the fuel container to a processing facility where non-gaseous mixed fission products and other impurities are removed and then the cleaned fuel is recycled into the fuel container. A reference core design and a preliminary plant system design of a 1000 MWt TRU- burning SLFFR concept were developed using TRU-Ce-Co fuel, Ta-10W fuel container, and sodium coolant. Conservative design approaches were adopted to stay within the current material performance database. Detailed neutronics and thermal-fluidic analyses were performed to develop a reference core design. Region-dependent 33-group cross sections were generated based on the ENDF/B-VII.0 data using the MC2-3 code. Core and fuel cycle analyses were performed in theta-r-z geometries using the DIF3D and REBUS-3 codes. Reactivity coefficients and kinetics parameters were calculated using the VARI3D perturbation theory code. Thermo-fluidic analyses were performed using the ANSYS FLUENT computational fluid dynamics (CFD) code. Figure 0.1 shows a schematic radial layout of the reference 1000 MWt SLFFR core, and Table 0.1 summarizes the main design parameters of SLFFR-1000 loop plant. The fuel container is a 2.5 cm thick cylinder with an inner radius of 87.5 cm. The fuel container is penetrated by twelve hexagonal control assembly (CA) guide tubes, each of which has 3.0 mm thickness and 69.4 mm flat-to-flat outer distance. The distance between two neighboring CA guide tube is selected to be 26 cm to provide an adequate space for CA driving systems. The fuel container has 18181 penetrating coolant tubes of 6.0 mm inner diameter and 2.0 mm thickness. The coolant tubes are arranged in a triangular lattice with a lattice pitch of 1.21 cm. The fuel, structure, and coolant volume fractions inside the fuel container are 0.386, 0.383, and 0.231, respectively. Separate steel reflectors and B4C shields are used outside of the fuel container. Six gas expansion modules (GEMs) of 5.0 cm thickness are introduced in the radial reflector region. Between the radial reflector and the fuel container is a 2.5 cm sodium gap. The TRU inventory at the beginning of equilibrium cycle (BOEC) is 5081 kg, whereas the TRU inventory at the beginning of life (BOL) was 3541 kg. This is because the equilibrium cycle fuel contains a significantly smaller fissile fraction than the LWR TRU feed. The fuel inventory at BOEC is composed of 34.0 a/o TRU, 41.4 a/o Ce, 23.6 a/o Co, and 1.03 a/o solid fission products. Since uranium-free fuel is used, a theoretical maximum TRU consumption rate of 1.011 kg/day is achieved. The semi-continuous fuel cycle based on the 300-batch, 1- day cycle approximation yields a burnup reactivity loss of 26 pcm/day, and requires a daily reprocessing of 32.5 kg of SLFFR fuel. This yields a daily TRU charge rate of 17.45 kg, including a makeup TRU feed of 1.011 kg recovered from the LWR used fuel. The charged TRU-Ce-Co fuel is composed of 34.4 a/o TRU, 40.6 a/o Ce, and 25.0 a/o Co.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2015

Delayed Gamma-Ray Spectroscopy for Non-Destructive Assay of Nuclear Materials

High-­energy, beta-delayed gamma-­ray spectroscopy is a potential, non-­destructive assay techniques for the independent verification of declared quantities of special nuclear materials at key stages of the fuel cycle and for directly assaying nuclear material inventories for spent fuel handling, interim storage, reprocessing facilities, repository sites, and final disposal. Other potential applications include determination of MOX fuel composition, characterization of nuclear waste packages, and challenges in homeland security and arms control verification. Experimental measurements were performed to evaluate fission fragment yields, to test methods for determining isotopic fractions, and to benchmark the modeling code package. Experimental measurement campaigns were carried out at the IAC using a photo-­neutron source and at OSU using a thermal neutron beam from the TRIGA reactor to characterize the emission of high-­energy delayed gamma rays from 235 U, 239 Pu, and 241 Pu targets following neutron induced fission. Data were collected for pure and combined targets for several irradiation/spectroscopy cycle times ranging from 10/10 seconds to 15/30 minutes.The delayed gamma-ray signature of 241 Pu, a significant fissile constituent in spent fuel, was measured and compared to 239 Pu. The 241 Pu/ 239 Pu ratios varied between 0.5 and 1.2 for ten prominent lines in the 2700-­3600 keV energy range. Such significant differences in relative peak intensities make it possible to determine relative fractions of these isotopes in a mixed sample. A method for determining fission product yields by fitting the energy and time dependence of the delayed gamma-­ray emission was developed and demonstrated on a limited 235 U data set. De-­convolution methods for determining fissile fractions were developed and tested on the experimental data. The use of high count-­rate LaBr 3 detectors was investigated as a potential alternative to HPGe detectors. Modeling capabilities were added to an existing framework and codes were adapted as needed for analyzing experiments and assessing application-­specific assay concepts. A de-­convolution analysis of the delayed gamma-­ray response spectra modeled for spent fuel assemblies was performed using the same method that was applied to the experimental spectra.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Developing a Signature Based Safeguards Approach for the Electrorefiner and Salt Cleanup Unit Operations in Pyroprocessing Facilities

Traditional nuclear materials accounting does not work well for safeguards when applied to pyroprocessing. Alternate methods such as Signature Based Safeguards (SBS) are being investigated. The goal of SBS is real-time/near-real-time detection of anomalous events in the pyroprocessing facility as they could indicate loss of special nuclear material. In high-throughput reprocessing facilities, metric tons of separated material are processed that must be accounted for. Even with very low uncertainties of accountancy measurements (<0.1%) the uncertainty of the material balances is still greater than the desired level. Novel contributions of this work are as follows: (1) significant enhancement of SBS development for the salt cleanup process by creating a new gas sparging process model, selecting sensors to monitor normal operation, identifying safeguards-significant off-normal scenarios, and simulating those off-normal events and generating sensor output; (2) further enhancement of SBS development for the electrorefiner by simulating off-normal events caused by changes in salt concentration and identifying which conditions lead to Pu and Cm not tracking throughout the rest of the system; and (3) new contribution in applying statistical techniques to analyze the signatures gained from these two models to help draw real-time conclusions on anomalous events.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Final Report on Two-Stage Fast Spectrum Fuel Cycle Options

This report presents the performance characteristics of two “two-stage” fast spectrum fuel cycle options proposed to enhance uranium resource utilization and to reduce nuclear waste generation. One is a two-stage fast spectrum fuel cycle option of continuous recycle of plutonium (Pu) in a fast reactor (FR) and subsequent burning of minor actinides (MAs) in an accelerator-driven system (ADS). The first stage is a sodium-cooled FR fuel cycle starting with low-enriched uranium (LEU) fuel; at the equilibrium cycle, the FR is operated using the recovered Pu and natural uranium without supporting LEU. Pu and uranium (U) are co-extracted from the discharged fuel and recycled in the first stage, and the recovered MAs are sent to the second stage. The second stage is a sodium-cooled ADS in which MAs are burned in an inert matrix fuel form. The discharged fuel of ADS is reprocessed, and all the recovered heavy metals (HMs) are recycled into the ADS. The other is a two-stage FR/ADS fuel cycle option with MA targets loaded in the FR. The recovered MAs are not directly sent to ADS, but partially incinerated in the FR in order to reduce the amount of MAs to be sent to the ADS. This is a heterogeneous recycling option of transuranic (TRU) elements

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Performance Criteria for Capture and/or Immobilization Technologies - Milestone Report

The capture and subsequent immobilization of the four regulated volatile radionuclides ( 3 H, 14 C, 85 Kr, and 129 I) from the off-gas streams of a used nuclear fuel (UNF) reprocessing facility has been a topic of substantial research interest for the US Department of Energy and its international colleagues. Removal of some or all of these radionuclides (e.g., based upon fuel burnup, fuel type, cooling time) from the plant effluent streams prior to discharge to the environment is required to meet regulations set forth by the US Environmental Protection Agency. Upon removal, the radionuclide, as well as associated sorbents that cannot be cost-effectively regenerated, is destined for conversion to a waste form. Research in separation and capture methodologies has included a wide range of technologies, including liquid caustic scrubbing systems, solid adsorbents, and cryogenic distillation. The studies of waste forms have been correspondingly diverse. In considering the technologies available for future development and implementation of both sorbents and waste forms, it is necessary to identify benchmark measures of performance to evaluate objectively each sorbent system or waste form.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

FY-2015 Methyl Iodide Deep-Bed Adsorption Test Report

Nuclear fission produces fission and activation products, including iodine-129, which could evolve into used fuel reprocessing facility off-gas systems, and could require off-gas control to limit air emissions to levels within acceptable emission limits. Deep-bed methyl iodide adsorption testing has continued in Fiscal Year 2015 according to a multi-laboratory methyl iodide adsorption test plan. Updates to the deep-bed test system have also been performed to enable the inclusion of evaporated HNO 3 and increased NO 2 concentrations in future tests. This report summarizes the result of those activities. Test results showed that iodine adsorption from gaseous methyl iodide using reduced silver zeolite (AgZ) resulted in initial iodine decontamination factors (DFs, ratios of uncontrolled and controlled total iodine levels) under 1,000 for the conditions of the long-duration test performed this year (45 ppm CH3I, 1,000 ppm each NO and NO 2 , very low H 2 O levels [3 ppm] in balance air). The mass transfer zone depth exceeded the cumulative 5-inch depth of 4 bed segments, which is deeper than the 2-4 inch depth estimated for the mass transfer zone for adsorbing I 2 using AgZ in prior deep-bed tests. The maximum iodine adsorption capacity for the AgZ under the conditions of this test was 6.2% (6.2 g adsorbed I per 100 g sorbent). The maximum Ag utilization was 51%. Additional deep-bed testing and analyses are recommended to (a) expand the data base for methyl iodide adsorption and (b) provide more data for evaluating organic iodide reactions and reaction byproducts for different potential adsorption conditions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Off-Gas Adsorption Model Capabilities and Recommendations

Off-gas treatment is required to reduce emissions from aqueous fuel reprocessing. Evaluating the products of innovative gas adsorption research requires increased computational simulation capability to more effectively transition from fundamental research to operational design. Early modeling efforts produced the Off-Gas SeParation and REcoverY (OSPREY) model that, while efficient in terms of computation time, was of limited value for complex systems. However, the computational and programming lessons learned in development of the initial model were used to develop Discontinuous Galerkin OSPREY (DGOSPREY), a more effective model. Initial comparisons between OSPREY and DGOSPREY show that, while OSPREY does reasonably well to capture the initial breakthrough time, it displays far too much numerical dispersion to accurately capture the real shape of the breakthrough curves. DGOSPREY is a much better tool as it utilizes a more stable set of numerical methods. In addition, DGOSPREY has shown the capability to capture complex, multispecies adsorption behavior, while OSPREY currently only works for a single adsorbing species. This capability makes DGOSPREY ultimately a more practical tool for real world simulations involving many different gas species. While DGOSPREY has initially performed very well, there is still need for improvement. The current state of DGOSPREY does not include any micro-scale adsorption kinetics and therefore assumes instantaneous adsorption. This is a major source of error in predicting water vapor breakthrough because the kinetics of that adsorption mechanism is particularly slow. However, this deficiency can be remedied by building kinetic kernels into DGOSPREY. Another source of error in DGOSPREY stems from data gaps in single species, such as Kr and Xe, isotherms. Since isotherm data for each gas is currently available at a single temperature, the model is unable to predict adsorption at temperatures outside of the set of data currently available. Thus, in order to improve the predictive capabilities of the model, there is a need for more single-species adsorption isotherms at different temperatures, in addition to extending the model to include adsorption kinetics. This report provides background information about the modeling process and a path forward for further model improvement in terms of accuracy and user interface.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
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↗
DOE OSTI2018

A Systems Processing Model for Molten Salt Reactors

The chemistry group within the U.S. Department of Energy Molten Salt Reactor Campaign is developing a model for the molten salt reactor system for assessing the suitability of various used fuel processing schemes. In the long run, the developed model is expected to be a tool for better understanding the interplay between the components of the molten salt reactor system including uranium resources, the molten salt reactor, the used fuel processor (e.g., reprocessing plant), and waste management. In this regard, the report proposes a theoretical framework for integrating the various components of the molten salt reactor system. Rather than being buried in implementation details for seemingly heterogeneous components of the reactor system asking for various modeling techniques, this report proposes to approximate and integrate all components with a unified mathematical framework, a discrete-time linear system. An abstracted molten salt reactor system is given as an example to illustrate the effectiveness of the proposed theoretical framework. A fully developed molten salt reactor system model (based on the proposed framework) is expected to be beneficial for various objectives including the transient and equilibrium analysis of fuel cycle scenarios and the identification of potential technology bottlenecks.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Iodobutane Deep Bed Adsorption Test Report

The Department of Energy (DOE) Nuclear Technology Research and Development (NTRD) Program Material Recovery and Waste Form Development (MRWFD) Campaign Off-gas Sigma Team has supported research and development on iodine control and iodine waste forms for the past several years. As a part of this on-going research, two deep-bed iodobutane adsorption tests have been performed with higher NO x levels. High (>1,000) iodine decontamination factors (DFs, the ratios of the inlet iodine concentrations divided by the outlet iodine concentrations, when the gas flowrate is constant) were achieved with both the silver aerogel and silver zeolite sorbents. The iodine adsorption mass transfer zone (the depth of the sorbent bed in which adsorption is occurring at any specific time) for these tests was estimated at 4 inches for both sorbents under the test conditions. Silver utilization for silver aerogel sorbent reached 41% (up to 12 g adsorbed iodine per 100 g silver aerogel sorbent), while silver utilization reached 43% (up to 6.8 g adsorbed iodine per 100 g silver zeolite sorbent). These values are generally consistent with results for prior methyl iodide adsorption tests. The results also indicate that, during iodine adsorption process, the organic iodide molecule decomposes so that the iodine can be adsorbed. Even when sorbent breakthrough is reached, the organic iodide molecule continues to decompose; and the unadsorbed iodine that passes through bed is no longer in the form of the original organic iodide; but in the form of iodine compounds that are soluble in NaOH solutions, such as HI or I 2 . This research and development has included iodine adsorption tests using a laboratory-scale test system containing segmented fixed beds of iodine adsorbents in series. Non-radioactive synthetic gas mixtures were blended from air, nitrogen, NO, NO 2 , water, and the target iodine compounds to represent dissolver off-gas (DOG) streams from used nuclear fuel aqueous reprocessing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Organic Iodine Capture from Vessel Off-gas

The Department of Energy (DOE) Nuclear Fuel Cycle and Supply Chain Program Material Recovery and Waste Form Development (MRWFD) Campaign Off-gas Sigma Team has performed research and development on iodine control and iodine waste forms for the past several years. This research and development has included iodine adsorption tests using a laboratory-scale test system containing multiple-segmented fixed beds of iodine adsorbents. Iodine capture performance has been tested using non-radioactive synthetic gas mixtures blended from air, nitrogen, NO, NO2, water, and the target iodine compounds diatomic iodine (I2), representing likely inorganic iodides, and methyl iodide (iodomethane, CH3I) and 1-iodobutane (butyl iodide) a surrogates for potential organic iodides, that could exist in dissolver off-gas (DOG) and vessel off-gas (VOG) streams from used nuclear fuel aqueous reprocessing.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗
DOE OSTI2022

Dehalogenation reactions between halide salts and phosphate compounds

Reactions between phosphoric acid [H 3 PO 4 ] or ammonium hydrogen phosphates [i.e., NH 4 H 2 PO 4 , (NH 4 ) 2 HPO 4 ] and halide salts can be used to dehalogenate (remove halides from) salt-based waste streams, where the process of removing halides yields products that have more efficient disposal pathways for repository storage. In this context, the term efficiency is defined as higher waste loadings and simplified immobilization processes with potential for recycle of certain salt components (e.g., 37 Cl as H 37 Cl or NH 4 37 Cl). The main streams identified for these processes are nuclear wastes generated during electrochemical reprocessing of used nuclear fuel as well as used halide salts from molten salt reactor operation. The potential byproducts of these reactions are fairly consistent across the range of halide species (i.e., F, Cl, Br, I) where the most common are hydrogen halides [e.g., HCl (g) ] or ammonium halides (e.g., NH 4 Cl). However, trihalide compounds (e.g., NCl 3 ), nitrogen triiodide ammine adducts [NI 3 ·(NH 3 ) x ], and ammonium triiodide (NH 4 I 3 ) are also possible. Several of these byproducts (i.e., NCl 3 , NBr 3 , NI 3 , and NH 4 I 3 ) are shock-sensitive contact explosives so their production in these processes must be tracked and carefully controlled, which includes methods of immediate neutralization upon production such as direct transport to a caustic scrubber for dissolution. Several benefits arise from utilizing H 3 PO 4 as the phosphate additive during dehalogenation reactions for making iron phosphate waste forms including more oxidized iron (higher Fe 3+ :Fe 2+ ratios), higher chemical durabilities, and the avoidance of trihalides, but the byproducts are hydrogen halides, which are corrosive and require special handling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Peering through the dust: NuSTAR observations of two FIRST-2MASS red quasars

Some reddened quasars appear to be transitional objects in the paradigm of merger-induced black hole growth/galaxy evolution, where a heavily obscured nucleus starts to be unveiled by powerful quasar winds evacuating the surrounding cocoon of dust and gas. Hard X-ray observations are able to peer through this gas and dust, revealing the properties of circumnuclear obscuration. Here, we present NuSTAR and XMM-Newton/Chandra observations of FIRST-2MASS-selected red quasars F2M 0830+3759 and F2M 1227+3214. We find that though F2M 0830+3759 is moderately obscured (N{sub H,Z} = (2.1 ± 0.2) × 10{sup 22} cm{sup −2}) and F2M 1227+3214 is mildly absorbed (N{sub H,Z}=3.4{sub −0.7}{sup +0.8}×10{sup 21} cm{sup −2}) along the line of sight, heavier global obscuration may be present in both sources, with N{sub H,S}=3.7{sub −2.6}{sup +4.1}×10{sup 23} cm{sup −2} and <5.5 × 10{sup 23} cm{sup −2} for F2M 0830+3759 and F2M 1227+3214, respectively. F2M 0830+3759 also has an excess of soft X-ray emission below 1 keV, which is well accommodated by a model where 7% of the intrinsic X-ray emission from the active galactic nucleus (AGN) is scattered into the line of sight. While F2M 1227+3214 has a dust-to-gas ratio (E(B – V)/N{sub H}) consistent with the Galactic value, the value of E(B – V)/N{sub H} for F2M 0830+3759 is lower than the Galactic standard, consistent with the paradigm that the dust resides on galactic scales while the X-ray reprocessing gas originates within the dust sublimation zone of the broad-line region. The X-ray and 6.1 μm luminosities of these red quasars are consistent with the empirical relations derived for high-luminosity, unobscured quasars, extending the parameter space of obscured AGNs previously observed by NuSTAR to higher luminosities.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2016

On the optical-X-ray correlation from outburst to quiescence in low-mass X-ray binaries: the representative cases of V404 Cyg and Cen X-4

Low-mass X-ray binaries (LMXBs) show evidence of a global correlation of debated origin between X-ray and optical luminosity. We study for the first time this correlation in two transient LMXBs, the black hole (BH) V404 Cyg and the neutron star Cen X-4, over six orders of magnitude in X-ray luminosity, from outburst to quiescence. After subtracting the contribution from the companion star, the Cen X-4 data can be described by a single power-law correlation of the form L{sub opt}∝ L{sub X}{sup 0.44}, consistent with disk reprocessing. We find a similar correlation slope for V404 Cyg in quiescence (0.46) and a steeper one (0.56) in the outburst hard state of 1989. However, V404 Cyg is about 160–280 times optically brighter, at a given 3–9 keV X-ray luminosity, compared to Cen X-4. This ratio is a factor of 10 smaller in quiescence, where the normalization of the V404 Cyg correlation also changes. Once the bolometric X-ray emission is considered and the known main differences between V404 Cyg and Cen X-4 are taken into account (a larger compact object mass, accretion disk size, and the presence of a strong jet contribution in the hard state for the BH system), the two systems lie on the same correlation. In V404 Cyg, the jet dominates spectrally at optical–infrared frequencies during the hard state but makes a negligible contribution in quiescence, which may account for the change in its correlation slope and normalization. These results provide a benchmark to compare with data from the 2015 outburst of V404 Cyg and, potentially, other transient LMXBs as well.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2016

FIRST IMAGES OF DEBRIS DISKS AROUND TWA 7, TWA 25, HD 35650, AND HD 377

We present the first images of four debris disks observed in scattered light around the young (4–250 Myr old) M dwarfs TWA 7 and TWA 25, the K6 star HD 35650, and the G2 star HD 377. We obtained these images by reprocessing archival Hubble Space Telescope NICMOS coronagraph data with modern post-processing techniques as part of the Archival Legacy Investigation of Circumstellar Environments program. All four disks appear faint and compact compared with other debris disks resolved in scattered light. The disks around TWA 25, HD 35650, and HD 377 appear very inclined, while TWA 7's disk is viewed nearly face-on. The surface brightness of HD 35650's disk is strongly asymmetric. These new detections raise the number of disks resolved in scattered light around M and late-K stars from one (the AU Mic system) to four. This new sample of resolved disks enables comparative studies of heretofore scarce debris disks around low-mass stars relative to solar-type stars.

79 ASTRONOMY AND ASTROPHYSICS↗