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

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At least 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Progress, Performance, and Prospects of Ultra-High Resolution Microcalorimeter Spectrometers

In 2005 the LANL/NIST team used a single high-resolution microcalorimeter detector to measure the gamma-ray spectrum of a plutonium sample. After more than a decade of research and development on this topic, both the technology and our general understanding of its capabilities have advanced greatly, such that a progress review is now timely. We examine the scenario of a large-scale reprocessing plant and conclude that current non-destructive analysis (NDA) methods are inadequate to safeguard such a facility to the desired levels, leading to undesirable dependence on massspectrometry (MS) destructive analysis (DA). The development of microcalorimeter detectors is intended to close the performance gap between NDA and DA methods to address the needs of nuclear facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Decommissioning Experience at Rokkasho; Standing Type Manipulator: A1000S for Dismantling Tasks - 16434

Decommissioning is a technical process which includes various steps and processes from the clean-up of radioactive materials to the progressive demolition of the plant. One of these steps is the cutting of subassemblies, like tanks, pipes or walls in small pieces suitable for the sorting and disposal. Different solutions are offered for this cutting work and can be grouped as following: - Chip forming - sawing, drilling, milling, turning etc. - Shearing - punching, stamping, scissoring. - Abrading - Grinding, lapping, polishing; water-jet. - Heat - flame cutting, plasma cutting, laser cutting. - Electro-Chemical - Etching, Electrical discharge machining (EDM). Each method has its limitations in accuracy, cost, and effect on the material. In 2013, Waelischmiller Engineering won a contract for two remote handling systems dedicated to the dismantling cell at Rokkasho Nuclear Fuel Reprocessing Facility in Japan. For this project, Inconel and other metals needed to be cut. One of the main cutting methods was decided to use of an angle grinder handled by a robotic arm. Because the use of the overhead systems (bridges and cranes) was difficult for this installation, it was determined, that the best alternative was a power manipulator A1000 installed on the floor with a pre-positioning system. The project proceeded to go forward with the adaptation of the standard A1000 with integration of a control system in a Cartesian coordinate frame; resulting in a heavy duty arm; A1000S with 6 degrees of freedom. The heavy duty power arm A1000S was developed and designed for mechanical cutting with an angle grinder, especially for thick and hard material for example stainless steel and Inconel. Cutting a thick material with an angle grinder requires repeatable precise linear motion, in order not to damage the disc. The angle grinder should be handled with a manipulator which can cut in all directions in a linear motion, since the objects which should be cut are usually very large and fixed in any direction For these requirements, the Cartesian control function was added to our standard power manipulator type A1000. In some cases, the decommissioning work includes repeated access routes or fixed access points that the manipulator arm has to pass repeatedly. For example a fixed point where the waste materials are collected, or repeated transport route that the arm has to go along for each step. For this requirement, the A1000S has been equipped with the 'Go To-Mode'. It is a 'teach and playback mode' which has been developed especially for remote operating manipulators. Quick direct teach, quick play function and an intuitive touch-panel layout are some of the features. With the Go To-Mode high working efficiency was achieved. After rigorous testing at Waelischmiller premises; the manipulator was delivered to JNFL in Rokkasho. It was found that the obtained functionality and precision can be applicable not only for the cutting with a disc grinder, but also the laser cutting method, which requires precise trajectory control. This paper will provide: - A project description, - Presentation of solution process, - Technical description of the A1000S, - Future Applications of the robotic Arm A1000S. (authors)

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

Gas Retention and Release from Nuclear Legacy Waste - 16449

The retention of gas within corroded magnox sludge waste at Sellafield, UK and secondary reprocessing waste at Hanford, USA has significant economic and safety implications for decommissioning various nuclear legacy buildings, including the magnox swarf storage silos and first generation magnox storage pond. A series of laboratory scale gas retention tests within magnesium hydroxide soft sediments have revealed a 4-51 Pa yield stress range where consolidated beds could retain sufficient gas to become buoyant with respect to a water supernatant. Density inversion could lead to a Rayleigh-Taylor style instability which could result in an upward transfer of radioactive material from the consolidated bed. The applicable yield stress range suggests that such rollover events may occur in weaker sediment than previously hypothesized, based on current understanding of the fluidization and stable channel mechanisms for gas release from weak and very strong sediments respectively. X-ray computed tomography images of gas retained by 7 Pa yield stress soft sediment reveal both a stable foam layer at the top of the bed and regions dense with micro-bubbles which could provide pathways for gas transport through the bed. Extension of these pathways, hidden below the surface of the sediment, to the container walls and the foam layer could represent a novel mechanism for gas release from intermediate strength sediments of <100 Pa yield stress. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Robotics for Nuclear Monitoring and Inspection - 18029

As a greater number of the world's nuclear facilities approach the end of their planned lifetime and enter the decommissioning and dismantling phase, a greater impetus than ever is being placed on the use of novel technologies to assist in this otherwise extremely lengthy, complicated and costly process. Being host to numerous first-generation plants, as well as the Sellafield Limited nuclear reprocessing facility, the UK is now requiring the use of a range of robotic systems and is well-placed to act as a test-bed for the deployment of these platforms. Presented in this work is the overview of the wide range of robotic research that is occurring at the University of Bristol. Not limited to ground-based platforms - those developed at the University Bristol,UK, include; airborne, underwater as well as pipeline network monitoring systems. Through the application of each of these robotic systems, not only is the dose-rate otherwise experienced by the operator removed, but the costs associated with the work are also significantly reduced, as well as the speed at which it is performed dramatically increased. All the systems descried in this work have been successfully deployed at one (or multiple) nuclear sites, with the results used to inform further decommissioning - typically within environments previously uncharacterised due either to their inaccessibility or high levels of radioactivity. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2018

The Strategic Benefit of Self Shielded Boxes for Storage and Disposal of Metallic Uranic Material-18141

Sellafield Ltd, on behalf of the Nuclear Decommissioning Authority (NDA), is responsible for the management of a number of facilities whose inventories include a range of metallic uranic material. Additional fuel and fuel bearing materials exist in the NDA estate, some of which are similar to the Sellafield-managed inventory and others present different management challenges. Whilst UK Government policy directs that some of these materials are assets and are therefore managed with eventual future use in mind, there remains a large quantity of material, principally either out-of-scope for reprocessing or which derives from legacy facilities, which is likely to be disposed of to a future Geological Disposal Facility (GDF). The majority of this material is stored under wet conditions to facilitate dose shielding and heat dissipation and will therefore require removal from wet storage, consolidation and conditioning, prior to transfer to GDF. In order to accelerate high hazard and risk reduction by sooner retrieval of legacy material from wetted storage, one of the legacy storage facilities has led technical work to develop the design of Self Shielded Boxes (SSBs) and to substantiate their use for interim storage of the materials in question. Use of the SSBs would represent a change of strategy on the Sellafield Site: historically, timescales for retrieval of material have been reliant upon a waste treatment and storage/disposal route being available. SSBs provide the opportunity to retrieve uranic materials from aging legacy storage facilities for immediate buffer storage, by decoupling the timing of retrieval from the availability of an onward route. An understanding was required of the scope for defining optimal routes for each metallic uranic fuel and fuel bearing material group for safe transport and storage commensurate with current final disposal assumptions and risks, taking into account international best practice. A study is underway to understand options for transfer of material into SSBs, buffer/interim storage locations, treatment/conditioning processes and transport to the GDF. This work forms the basis of a prioritised road-map for the development of routes for study material groups aligned with ongoing and existing planned technical work, which is a pre-requisite to strategy development. The ultimate output of the study will be identification of full life cycle management strategies for metallic uranic material from an enterprise perspective. The combination of this strategic work and ongoing technical work will underpin a series of decisions to divert sub-groups of uranic material away from currently assumed baseline routes in support of earliest practicable hazard and risk reduction. Hence, each decision will reduce the scope of a placeholder future uranic fuel treatment capability, which will diminish the associated British Pound 1 bn capital cost. To date, a technical case for interim storage of uranic material in SSBs has been substantiated for around two thirds of the study materials. The requirement for a new strategy at Sellafield was driven by technical development of SSBs in response to the needs of one programme, but this prompted the study into the potential utilisation of SSBs in order to derive benefit for the wider enterprise and across the NDA estate. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

{sup 14}C Entry into the Atmosphere

{sup 14}C enters the atmosphere in amounts equivalent to 1.4 PBq/yr with total accumulation 140 PBq via cosmic radiation. As a result of nuclear explosions (1950–1969), its activity in the atmosphere exceeded 200 PBq. At present, {sup 14}C has been completely removed into bottom waters and sedimentary rocks in the ocean. The activity of the {sup 14}C entering the atmosphere from all operating nuclear reactors equals ~0.3 PBq/yr and the amount from all spent fuel reprocessing facilities equals ~0.06 PBq/yr. The admissible levels of {sup 14}C emissions must not exceed levels corresponding to peroral intake dose 10 μSv/yr. This is can be accomplished by means of a system of measures: reduction of the volume of technogenic gases and their {sup 12}CO{sub 2} content, combining high-efficiency purification with dispersion through high exhaust-stacks, and developing new technologies and reagents binding {sup 14}C in compact forms.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Response of soil bacteria to PUREX chemicals suggests biomarker utility and bioremediation potential

Chemicals involved in plutonium uranium reduction extraction (PUREX) can be released from nuclear reprocessing facilities and accumulate in the environment. We exposed chemically diverse soils to a range of concentrations of key chemicals used in the PUREX process. The responses of soil microbial communities are dependent on soil type, and tributyl phosphate exposure generates the most reproducible changes in microbial communities. We reconstructed the genomes of key bacteria and find several phosphotriesterase genes found only in Rhizobiaceae. The abundance of phosphotriesterase genes is significantly higher in samples exposed to tributyl phosphate. In conclusion, these phosphotriesterase genes may be involved in breakdown of tributyl phosphate, and a means of accessing phosphate for these bacteria.

Bioremediation↗
DOE OSTI2020

Strategies for thorium fuel cycle transition in the SD-TMSR

Liquid-fueled Molten Salt Reactor (MSR) systems represent advances in safety, economics, and sustainability. The MSR has been designed to operate with a Th/ 233 U fuel cycle with 233 U used as startup fissile material. Since 233 U does not exist in nature, we must examine other available fissile materials to start up these reactor concepts. This work investigates the fuel cycle and neutronics performance of the Single-fluid Double-zone Thorium-based Molten Salt Reactor (SD-TMSR) with different fissile material loadings at startup: High Assay Low Enriched Uranium (HALEU) (19.79%), Pu mixed with HALEU (19.79%), reactor-grade Pu (a mixture of Pu isotopes chemically extracted from Pressurized Water Reactor (PWR) spent nuclear fuel (SNF) with 33 GW d/tHM burnup), transuranic elements (TRU) from Light Water Reactor (LWR) SNF, and 233 U. The MSR burnup routine provided by SERPENT-2 is used to simulate the online reprocessing and refueling in the SD-TMSR. The effective multiplication factor, fuel salt composition evolution, and net production of 233 U are studied in the present work. Additionally, the neutron spectrum shift during the reactor operation is calculated. The results show that the continuous flow of reactorgrade Pu helps transition to the thorium fuel cycle within a relatively short time (≈ 4.5 years) compared to 26 years for 233 U startup fuel. Finally, using TRU as the initial fuel materials offers the possibility of operating the SD-TMSR for an extended period of time (≈ 40 years) without any external feed of 233 U.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Experimental and modeling studies of PR and ND oxalate solubility to high ionic strengths: Insight into actinide(III) oxalates

Actinide oxalates are chemical compounds important to nuclear industry, ranging from actinide separation in waste reprocessing, to production of specialty actinides, and to disposal of high level nuclear waste (HLW) and spent nuclear fuel (SNF). In this study, the solubility constants for Pr 2 (C 2 O 4 ) 3 •10H 2 O and Nd 2 (C 2 O 4 ) 3 •10H 2 O by performing solubility experiments in HNO 3 and mixtures of HNO 3 and H 2 C 2 O 4 at 23.0 ± 0.2 °C have been determined. The targeted starting materials, Pr 2 (C 2 O 4 ) 3 •10H 2 O and Nd 2 (C 2 O 4 ) 3 •10H 2 O, were successfully synthesized at room temperature using PrCl 3 , NdCl 3 and oxalic acid as the source metrials. Then, we utilized the targeted solubility-controlling phases to conduct solubility measurements. There was no phase change over the entire periods of experiments, demonstrating that Pr 2 (C 2 O 4 ) 3 •10H 2 O and Nd 2 (C 2 O 4 ) 3 •10H 2 O were the solubility-controlling phases in our respective experiments. Based on our experimental data, we have developed a thermodynamic model for Pr 2 (C 2 O 4 ) 3 •10H 2 O and Nd 2 (C 2 O 4 ) 3 •10H 2 O in the mixtures of HNO 3 and H 2 C 2 O 4 to high ionic strengths. The model for Pr 2 (C 2 O 4 ) 3 •10H 2 O reproduces well the reported experimental data for Pu 2 (C 2 O 4 ) 3 •10H 2 O, which are not utilized for the model development, demonstrating that Pr(III) is an excellent analog for Pu(III). Similarly, the model for Nd 2 (C 2 O 4 ) 3 •10H 2 O reproduces the solubility of Am 2 (C 2 O 4 ) 3 •10H 2 O and Cm 2 (C 2 O 4 ) 3 •10H 2 O. The Pitzer model was used for the calculation of activity coefficients. Based on the published, well established model for dissociation constants for oxalic acid and stability constants for actinide-oxalate complexes [i.e., AmC 2 O 4 + , and Am(C 2 O 4 ) 2 - ] to high ionic strengths, we have obtained the solubility constants (log 10 K 0 ) for the following reactions at 25 °C, Pr 2 (C 2 O 4 ) 3 •10H 2 O ⇌ 2Pr 3+ + 3C 2 O 4 2- + 10H 2 O(l). Nd 2 (C 2 O 4 ) 3 •10H 2 O ⇌ 2Nd 3+ + 3C 2 O 4 2- + 10H 2 O(l). to be -30.82 ± 0.30 (2σ), and - 31.14 ± 0.35 (2σ), respectively. These values for can be directly applied to Pu 2 (C 2 O 4 ) 3 •10H 2 O, Am 2 (C 2 O 4 ) 3 •10H 2 O and Cm 2 (C 2 O 4 ) 3 •10H 2 O. The model established for actinide oxalates by this study provides the needed knowledge with regard to solubilities of actinide/REE oxalates at various ionic strengths, and is expected to find applications in many fields, including the geological disposal of nuclear waste and the mobility of REE under the surface conditions, as Pr 2 (C 2 O 4 ) 3 •10H 2 O and Nd 2 (C 2 O 4 ) 3 •10H 2 O can be regarded as the pure Pr and Nd end-members of deveroite, a recently discovered natural REE oxalate with the following stoichiometry, (Ce 1.01 Nd 0.33 La 0.32 Pr 0.11 Y 0.11 Sm 0.01 Pb 0.04 U 0.03 Th 0.01 Ca 0.04 ) 2.01 (C 2 O 4 ) 2.99 •9.99H 2 O. Regarding its importance in the geological disposal of nuclear waste, Am 2 (C 2 O 4 ) 3 •10H 2 O/Pu 2 (C 2 O 4 ) 3 •10H 2 O/Cm 2 (C 2 O 4 ) 3 •10H 2 O can be the source-term phase for actinides, as demonstrated by the instance in the disposal in clay/shale formations. This is exemplified by the stability of Am 2 (C 2 O 4 ) 3 •10H 2 O in comparison with Am(OH) 3 (am), Am(OH) 3 (s) and AmCO 3 (OH)(s) under the relevant geological repository conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Evaluation of corrosion coupons exposed to molten-chloride electrorefiner salts long term

Corrosion mitigation has long been considered a challenge in long-term service of both pyrochemical reprocessing and molten salt reactor applications. Corrosion coupons consisting of 2.25Cr 1Mo ASME SA387 Grade 22 Class 2 steel, were installed in a uranium electrorefiner containing molten chloride salt at 500°C. This electrorefiner went into service at Idaho National Laboratory in 1994. Seven of these coupons were removed in 2019 (i.e., submerged in molten salt for 25 years) for analysis and characterization including neutron imaging, optical microscopy, scanning electron microscopy, and wave/energy dispersive x-ray spectroscopy. The results showed that all seven coupons experienced between 30 to 175 µm of surface degradation without evidence of brittle fracture. Meaning there was no evidence of accelerated corrosion or fractures, and the average steel surface loss was of less than 5 µm per year. All indications were that the environmental conditions inside the electrorefiner were favorable for the steel alloy.

36 - MATERIALS SCIENCE↗
DOE OSTI2025

Chemically and Mechanically Recyclable Vitrimers from Carbon Dioxide-Based Polycarbonates

Designing thermoset materials with dynamic crosslinks is an important strategy to mitigate rising global carbon dioxide emission levels. The development of polymers from sustainable feedstocks, with efficient manufacturing methods, for high-value applications, and with circular end-of-use solutions is essential for advancing material technologies. One approach involves exploiting carbon dioxide itself as feedstock to create high performance, sustainable materials, by enchaining 50 mol% CO2 via copolymerization with epoxides to yield polycarbonates. This work describes the synthesis, end-functionalization, and curing of poly(propylene carbonate) (PPC) and poly(cyclohexene carbonate) (PCHC) into beta-hydroxy ester vitrimers. These vitrimers demonstrate the ability to be mechanically reprocessed up to 3 times with retention of the material’s properties through dynamic transesterification exchange reactions. The polycarbonate vitrimers with gel fractions exceeding 90 % exhibit high tensile strength (> 50 MPa) and Young’s modulus (> 2 GPa), achieved by varying repeat unit structure in the polymer backbone from the low Tg PPC to the more rigid high Tg PCHC structures. Owing to an entropically favorable chain back-biting mechanism, the network chains can be cleaved and depolymerized into cyclic small molecules. In the case of PCHC, this process enables repolymerization back to polycarbonates with 69 wt.% CO2 retention through life-cycles. The promising mechanical performance and recyclability of these CO2-based polycarbonate vitrimers indicate their potential for sustainable, high-performance materials, paving the way for future innovations in circular polymer technologies and carbon capture utilization.

36 MATERIALS SCIENCE↗
DOE OSTI2024

NO 2 -mediated voloxidation for iodine separation from cesium iodide surrogates

Heterogeneous NO 2 -mediated oxidation of uranium, also known as advanced voloxidation, is a proposed head-end reprocessing method for used nuclear fuel. An advantage of advanced voloxidation is the removal of volatile fission products, which complicate downstream separation and containment challenges leading to increased processing economics. Iodine, one of the volatile species of interest, has exhibited varied results in this process. Using CsI as a surrogate material, this work mimics the effect of NO 2 -based voloxidation on iodine and sheds light on the factors that influence the solid–gas phase reaction. Solid-state analysis using Fourier transform infrared attenuated total reflectance spectroscopy and scanning electron microscopy with energy-dispersive X-ray spectroscopy confirmed the conversion of CsI to CsNO 3 . Iodine separation ranged from 46% to 100% across multiple tests. Iodine separation was most effective when multiple recharges of NO 2 were administered. In conclusion, at the bench scale, liberating iodine from CsI appears to occur within 1 h, but the presence of surface H 2 O and the composition of the NO x reagent mixtures greatly influence its success.

advanced voloxidation↗
DOE OSTI2016

ORNL experience and perspectives related to processing of thorium and 233 U for nuclear fuel

Thorium-based nuclear fuel cycles have received renewed attention in both research and public circles since about the year 2000. Much of the attention has been focused on nuclear fission energy production that utilizes thorium as a fertile element for producing fissionable 233 U for recycle in thermal reactors, fast reactors, or externally driven systems. Here, lesser attention has been paid to other fuel cycle operations that are necessary for implementation of a sustainable thorium-based fuel cycle such as reprocessing and fabrication of recycle fuels containing 233 U.

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

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↗