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At least 883 records · Page 49
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Investigating Radiation-Induced Actinide Species in Solution

Used nuclear fuel (UNF) separation techniques that strive to separate radiotoxic americium (Am) from trivalent lanthanide fission products through oxidation state control have increased research efforts surrounding Am(V) and Am(VI). However, equivalent knowledge of the tetravalent state, Am(IV), has remained elusive, particularly in conditions more representative of UNF reprocessing, i.e., in concentrated nitric acid (HNO3). With this in mind, we have used electron pulse radiolysis to study the radiation-induced redox reaction of Am(III) with the oxidizing nitrate radical (NO3?) in 6 M HNO3: Am(III) + NO3? ? Am(IV) + NO3? . These experiments enabled us to observe the growth and decay of Am(IV) in a concentrated acidic solution for the first time. The transient Am(IV) species was found to have a lifetime of ~16 µs?sufficiently long-lived to play a critical mechanistic role in UNF reprocessing systems. Additionally, we performed the first-ever temperature-dependent kinetics study of an actinide element, elucidating unprecedented Arrhenius and Eyring activation parameters for the reaction of Am(III) with NO3?. This new knowledge provides much-needed molecular-level insights into the radiation-induced behavior of Am.

actinide↗
DOE OSTI2016

A New Group Crystallization Approach in Used Nuclear Fuel Recycling: A Look at Fission Product Behaviors

Nuclear energy has the potential to play a large role in meeting future needs of the U.S. sustainable energy strategy, as a clean, carbon-free power source. However, to take advantage of the inherent benefits, many hurdles must be overcome in order for nuclear power to achieve these expectations. One of the largest challenges faced, is the management of used nuclear fuel (UNF). Currently, no strategy has been identified to deal with the growing UNF problem, and so the UNF remains stored on site at nuclear power plants either in cooling pools or in dry cast storage. The amount of stored UNF continues to grow, and with it, so does the concern surrounding its long-term radiotoxicity. This material could be reprocessed to recover the actinides, maximizing the energy potential of the UNF and minimizing the waste generation. Not only do U and Pu, the major energy producing actinides, need to be recovered, but recovering Np and Am would make waste generated from reprocessing significantly safer for long-term storage in a geological repository. There are a number of methods currently in use to reprocess UNF; throughout Europe, the Purex process is widely implemented, while the Japanese have developed the Next process. The Next process removes a bulk of the U by crystallization prior to a Purex-like separation scheme. In the Next process, it is undesirable to have any other species removed from solution in the crystallization step, but rather the goal is to obtain a pure uranyl nitrate hexahydrate (UNH) product. Alternatively, a group separation of U-Am by a crystallization process would provide an elegant solution. Such a process has become attainable with the renewed interest in accessing Am(VI) in nitric acid solutions. In order to synthesize and stabilize Am(VI), a highly oxidizing system is required, which has only been demonstrated on a limited basis. By oxidizing Np, Pu, and Am to their hexavalent state, they can be co-crystallized with UNH, and thereby removed from solution. Recent results have demonstrated that all the hexavalent actinide (An) species are removed from solution in near proportion, by a simple reduction of temperature in 6-8 M HNO{sub 3}. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

A New Group Crystallization Approach in Used Nuclear Fuel Recycling: A Look at Fission Product Behaviors

Nuclear energy has the potential to play a large role in meeting future needs of the U.S. sustainable energy strategy, as a clean, carbon-free power source. However, to take advantage of the inherent benefits, many hurdles must be overcome in order for nuclear power to achieve these expectations. One of the largest challenges faced, is the management of used nuclear fuel (UNF). Currently, no strategy has been identified to deal with the growing UNF problem, and so the UNF remains stored on site at nuclear power plants either in cooling pools or in dry cask storage. The amount of stored UNF continues to grow, and with it, so does the concern surrounding its long-term radiotoxicity. This material could be reprocessed to recover the actinides, maximizing the energy potential of the UNF and minimizing the waste generation. Not only do U and Pu, the major energy producing actinides, need to be recovered, but recovering Np and Am would make waste generated from reprocessing significantly safer for long-term storage in a geological repository. There are a number of methods currently in use to reprocess UNF; throughout Europe, the Purex process is widely implemented, while the Japanese have developed the Next process. The Next process removes a bulk of the U by crystallization prior to a Purex-like separation scheme. In the Next process, it is undesirable to have any other species removed from solution in the crystallization step, but rather, the goal is to obtain a pure uranyl nitrate hexahydrate (UNH) product. Alternatively, a group separation of U-Am by a crystallization process would provide an elegant solution. Such a process has become attainable with the renewed interest in accessing Am(VI) in nitric acid solutions. In order to synthesize and stabilize Am(VI) which has only been demonstrated on a limited basis, a highly oxidizing system is required. By oxidizing Np, Pu, and Am to their hexavalent state, they can be co-crystallized with UNH, and thereby removed from solution. Recent results have demonstrated that all the hexavalent actinide (An) species are removed from solution in near proportion, by a simple reduction of temperature in 6-8 M HNO{sub 3}.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Chabazite Zeolite Membranes for Krypton/Xenon Separation: Control of Membrane Properties and Process Modeling

Nuclear energy is considered to be a clean and economical means of carbon-free energy. As part of the overall process for recycling used nuclear fuel (UNF), it is necessary to develop technologies to separate the off-gases formed during the fission of uranium and plutonium in nuclear power reactors. The off-gas stream is generated during the shearing and chopping, voloxidation, and acid dissolution steps, and would have a flow rate of ∼2500 L/min assuming a typical 800 tons heavy metal/yr reprocessing facility. Kr separation from Xe is one of the steps in a proposed UNF off-gas processing flowsheet. The Kr/Xe mixture is approximately 10/90 by volume and hence the separation of Kr would reduce the volume of radioactive {sup 85}Kr waste by a factor of 10. Kr/Xe separation is challenging since they are both chemically inert species and physically very similar (0.036 nm size difference). There is no existing process for this separation that is suitable for use in UNF recycling since conventional cryogenic distillation requires highly intensive power and large system volume. Membrane-based separation using radiation-stable materials such as zeolites could be an attractive separation method, if membranes with sufficient Kr flux and selectivity can be fabricated. Zeolite membranes offer an opportunity to exploit the size difference of Kr (kinetic diameter 0.36 nm) and Xe (0.396 nm) to achieve preferential permeation of the minority component (Kr) from the mixture, leading to an efficient separation with very low energy requirements. An ideal membrane process would permeate a stream of pure Kr for storage and also produce pure Xe which has commercial value (> $8000/kg at 99+% purity). SAPO-34 is a silico-alumino-phosphate zeolite molecular sieve with CHA framework topology and containing uniform micropores (0.38 nm), intermediate in size between the kinetic diameters of Kr and Xe. It was hypothesized that SAPO-34 membranes can separate krypton and xenon by diffusivity differences. Previously we fabricated SAPO-34 membranes and showed that they are capable of separating Kr from Xe. Our previous work also indicated that there is much potential for engineering the separation properties of these membranes with a view to improving permeance and selectivity and evaluating the expected process performance. The main objectives of the present study are: 1) development of SAPO-34 membranes with enhanced membrane performance via thickness reduction and ion exchange, and 2) process modeling for technic-economic analysis of zeolite membrane systems for Kr/Xe separation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Nuclear Criticality Safety [Book Chapter]

Nuclear Criticality Safety is a field of nuclear engineering that involves worker and public safety during the handling, processing, transportation, and storage activities of fissile isotopes ( 233 U, 235 U, and 239 Pu) outside of nuclear reactors. Criticality accidents release energy as a result of accidentally producing a self-sustaining fission chain reaction. If these occur during hands-on operations the results can be lethal to worker within about 4.6 m (15 ft.) of the accident. There have been 22 process criticality accidents in the world between 1953 and 1999 resulting in physical injury, on and off-site dose, or death. Nuclear Criticality Safety involves work by qualified persons to preclude criticality accidents and their consequences by ensuring activities with fissionable materials remain subcritical, i.e., safe, during all normal and credible abnormal conditions. This article presents information about those nuclear fuel cycle steps presenting Nuclear Criticality Safety concerns that must be considered to ensure worker and public safety is assured.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Characterization of the Chlorination Products of Zirconium Alloys used for Nuclear Fuel Cladding

The United States produces over 2000 metric tons of used nuclear fuel material per year, of which 25% is irradiated fuel cladding, and it is expected to increase for the next 50 years. Previous simulation studies have shown that in the irradiated cladding, the major activation products found are {sup 125}Sb, {sup 60}Co, and {sup 99m}Nb, and the major fission product found is {sup 137}Cs. These radioisotopes make it impossible to treat the cladding as low level waste. A chlorination process has been proposed for zirconium reprocessing as it has been proven more efficient than previous mechanical processes, redox processes, and other chemical methods (e.g. iodination). In the chlorination process, zirconium alloy cladding reacts with Cl{sub 2} at 350- 380 deg. C to produce mainly ZrCl{sub 4}. The zirconium tetrachloride has a relatively low sublimation point (331 deg. C) that allows its separation from other products, and so it can be treated as low level waste for disposal or recycling. However, previous work has observed element impurities (iron, tin, chromium, cesium, antimony, and niobium) in the recovered ZrCl{sub 4}, meaning that additional steps are necessary in a chlorination process previous to the reduction of ZrCl, to metallic Zr. The emphasis of this research summary is on the progress that has been made to isolate and characterize the impurities produced after chlorination of three previously characterized non-irradiated zirconium alloys (Zircaloy-2, Zircaloy-4, and a commercial Zr-Nb alloy) widely used as cladding materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Hestia-SWIFL: hourly anthropogenic fossil fuel CO2 and heat on the 2km WRF grid, version 1.1

The Hestia-SWIFL version 1.1 anthropogenic heat (AH) and fossil fuel CO2 (FFCO2) emissions data product represent emissions due to the combustion of fossil fuel and cement production within the state of Arizona from 2019 to 2022. This product was developed as part of the Southwest Urban Corridor Integrated Field Laboratory (SW-IFL) project, which aims to provide new knowledge and tools that address extreme heat, air quality, climate change and related urban environmental issues by integrating high-resolution observations, modeling, and civic engagement. The emissions are generated using a bottom-up/engineering approach and are tied to results generated by the Vulcan Project version 4, an effort to quantify space/time-resolved FFCO2 & AH emissions for the entire United States landscape. A large number of data sources are combined to best estimate the emissions at fine scales such as air quality emissions data, traffic flow data, building information, sociodemographic information, and fuel statistics. The AH product provides emissions for two emissions sources (transportation and point source emissions) in units of Watts per hour per square meter (W/m2) per year (annual files) or per hour (hourly files). The FFCO2 product provides emissions from nine individual emission sectors as well as the total, and in units of tons of carbon (tC) per grid cell per year or per hour. The output made available here places the native spatial resolution of the Hestia FFCO2 & AH emissions data product (points, lines, and polygons) into a regularized 2km x 2km grid at hourly and annual temporal resolutions, and stored in netCDF files. The exact spatial extent is defined by the ASU Weather Research Forecast (WRF) simulation grid. All data are processed using R/Python pm high-performance computing system. 2-27-2026 updates: Bugs in airport hourly profile (both AH and FFCO2) and building spatial patterns (FFCO2 only) were fixed. Hourly emissions are reprocessed for all years to reflect those changes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Safe Dissolution of High Flux Isotope Reactor Cores

The H-Canyon facility at the Savannah River Site is the U.S.A.’s only remaining full- scale chemical separations plant. H-Canyon maintains the capacity to safely and efficiently disposition a large inventory of excess nuclear material from across the Department of Energy (DOE) complex and used nuclear fuel from foreign and domestic research reactors. One such fuel that H-Canyon may dissolve is cores from the High Flux Isotope Reactor (HFIR). By employing realistic analysis, the need for administrative controls was eliminated. A new criticality modeling approach has eliminated the need for administrative controls for HFIR dissolution operations in H-Canyon. The primary upsets of concern are an over-mass event and an overconcentration event. Several initiating events were considered for each type of upset. Over-concentration events were deemed to be not credible by taking credit for the chemistry of acid consumption, i.e. there are not enough moles of acid to dissolve enough moles of uranium in order to reach a critical configuration. Over-mass events were deemed to be not credible by taking credit for the annular design of the fuel elements. By using realistic analysis, both types of upsets have been shown to be subcritical, and therefore administrative controls are not needed to prevent an inadvertent criticality. In this paper, the new methodology for performing criticality analyses for dissolving HFIR fuel elements will be presented, and the elimination of administrative controls will be discussed.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
NASA NTRS1982

Optical bursts from 4U/MXB 1636-53

The results of observations of 15 and 26 optical bursts detected during June and July 1979 and June and July 1980, respectively, from the X-ray burst source 4U/MXB 1636-53 in a 'white light' passband are presented. The maximum burst fluxes above the persistent optical flux and integrated burst fluxes are correlated, and it appears that the maximum optical and X-ray burst fluxes are related according to a power law, consistent with optical emission from blackbody reprocessing of X-rays. The approximately linear relationship between the integrated optical and X-ray burst fluxes argues against this simple picture. The correlation of burst fluxes with waiting time since the previous burst suggests that large optical bursts come after a long waiting time. Short burst intervals observed both for optical and X-radiation suggest that not all available nuclear fuel is consumed in the thermonuclear flash which gives rise to the X-ray burst.

Pedersen, H.↗
DOE OSTI2013

Magnetic nano-sorbents for fast separation of radioactive waste

In order to find a cost effective and environmentally benign technology to treat the liquid radioactive waste into a safe and stable form for resource recycling or ultimate disposal, this study investigates the separation of radioactive elements from aqueous systems using magnetic nano-sorbents. Our current study focuses on novel magnetic nano-sorbents by attaching DTPA molecules onto the surface of double coated magnetic nanoparticles (dMNPs), and performed preliminary sorption tests using heavy metal ions as surrogates for radionuclides. The results showed that the sorption of cadmium (Cd) and lead (Pb) onto the dMNP-DTPA conjugates was fast, the equilibrium was reached in 30 min. The calculated sorption capacities were 8.06 mg/g for Cd and 12.09 mg/g for Pb. After sorption, the complex of heavy elements captured by nano-sorbents can be easily manipulated and separated from solution in less than 1 min by applying a small external magnetic field. In addition, the sorption results demonstrate that dMNP-DTPA conjugates have a very strong chelating power in highly diluted Cd and Pb solutions (1-10 μg/L). Therefore, as a simple, fast, and compact process, this separation method has a great potential in the treatment of high level waste with low concentration of transuranic elements compared to tradition nuclear waste treatment. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

Calculations of enrichment cascade performance using enrichment probabilities – a new method

A new method for calculating the performance of uranium enrichment cascades is presented. The method assigns a unique “enrichment probability” for each isotope to move up or down from the basic enrichment unit, allowing independent material balance calculations for each isotope. The formulation is much simpler than previous methods, which rely on isotopic ratios, and this method can be used when previous methods fail. This method gives the same results as published cases for 235 U enrichment and also gives good agreement with published data on minor isotopes. Some comparisons with measured data and other calculations are given. One case shows that the maximum 235 U enrichment that can be obtained by enrichment of reprocessed uranium (0.02% 234 U initial) is 82%. Another example shows a large difference in the minor isotopic content of material enriched in batches compared to continuous enrichment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Literature Review: Crud Formation at the Liquid/Liquid Interface of TBP-Based Solvent-Extraction Processes

This report summarizes the literature reviewed on crud formation at the liquid:liquid interface of solvent extraction processes. The review is focused both on classic PUREX extraction for industrial reprocessing, especially as practiced at the Hanford Site, and for those steps specific to plutonium purification that were used at the Plutonium Reclamation Facility (PRF) within the Plutonium Finishing Plant (PFP) at the Hanford Site.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Engineering Considerations for Remote Refabrication of EBR-II Fuel Elements

The development of remote controlled methods for manufacturing EBR-II fuel elements was influenced by many interacting factors. Radiation levels within the process cell have been predicted to range from 10 3 to 10 7 rad per hour. Radiation damage to organic lubricant, electrical insulations, elastic seals, and protective coatings precludes the use of many standard machine components. Heat generated in the fuel by absorbed radiation makes forced cooling necessary in many operations. Oxygen must be exluded from all operations where the fuel is exposed. Equipment must be designed for remote maintenance and component replacement within the limitation of available manipulators. The EBR-II fuel consisted of fissium alloy pins sodium bonded in stainless steel tubes. Precision casting was chosen as the basis for refabricating the fuel pins. Remote controlled equipment was developed to cast, assemble, and inspect the EBR-II fuel elements. Radiation resistant, plug-in machine components were developed to give reasonable life expectancy and to allow remote maintenance and replacement.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Technology Development Roadmap for Volatile Radionuclide Capture and Immobilization

An “Off-Gas and Waste Forms Strategy Workshop” was held in Washington, D.C. on January 31, and February 1, 2023, to review the current state of the art (baseline) technologies for capturing and immobilizing these volatile radionuclides in waste forms (WFs). The discussions in that workshop were used to develop a roadmap for future research and development to mature technologies that are presently not ready for use in a commercial reprocessing facility and develop and demonstrate technologies that provide more safety, more simplicity, or lower costs compared to the current baseline.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

A Coincident CdTe Detector Array for Enhanced Nuclear Process Monitoring

Nuclear fuel cycle aqueous separation processes desire improved real-time material characterization and process monitoring techniques; gamma coincidence spectroscopy has the potential to meet this need in these high throughput and high radiation environments based on its ability to reduce background noise, thereby enhancing detection limits and improving isotopic identification accuracy. A detector array composed of three CdTe detectors was designed to surround a chemical processing pipe in a reprocessing facility and evaluate the feasibility of passively assaying the nuclear materials flowing though this measurement point. This array uses commercial off the shelf components that are radiation hard and highly efficiency at low energies relevant to actinide photon signatures. Detector efficiency characterizations, coincidence detection, and potential configuration improvements are presented here.

Good, Erin C.↗
DOE OSTI2013

Quantification of UV-Visible and Laser Spectroscopic Techniques for Materials Accountability and Process Control

Ultraviolet–visible spectroscopy (UV–Visible) and time-resolved laser fluorescence spectroscopy (TRLFS) optical techniques can permit on-line analysis of actinide elements in a solvent extraction process in real time. These techniques have been used for measuring actinide speciation and concentration under laboratory conditions and are easily adaptable to multiple sampling geometries, such as dip probes, fiber-optic sample cells, and flow-through cell geometries. To fully exploit these techniques, researchers must determine the fundamental speciation of target actinides and the resulting influence on spectroscopic properties. Detection limits, process conditions, and speciation of key actinide components can be established and utilized in a range of areas, particularly those related to materials accountability and process control. Through this project, researchers will develop tools and spectroscopic techniques to evaluate solution extraction conditions and concentrations of U, Pu, and Cm in extraction processes, addressing areas of process control and materials accountability. The team will evaluate UV– Visible and TRLFS for use in solvent extraction-based separations. Ongoing research is examining efficacy of UV-Visible spectroscopy to evaluate uranium and plutonium speciation under conditions found in the UREX process and using TRLFS to evaluate Cm speciation and concentration in the TALSPEAK process. A uranyl and plutonium nitrate UV–Visible spectroscopy study met with success, which supports the utility and continued exploration of spectroscopic methods for evaluation of actinide concentrations and solution conditions for other aspects of the UREX+ solvent extraction scheme. This project will examine U and Pu absorbance in TRUEX and TALSPEAK, perform detailed examination of Cm in TRUEX and TALSPEAK, study U laser fluorescence, and apply project data to contactors. The team will also determine peak ratios as a function of solution concentrations for the UV-Visible spectroscopy studies. The use of TRLFS to examine Cm and U will provide data to evaluate lifetime, peak location, and peak ratios (mainly for U). The bases for the spectroscopic techniques have been investigated, providing fundamental evidence for the application’s utility.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Project Overview: LA07-LAB072-PD02

The goal of this project was to identify and characterize sources of plutonium processing signatures, and understand how fate and transport impact these signatures, with an emphasis on establishing a foundation for the use of aerosolized particle characteristics as indicators of historic and current activities within a facility. Targeted activities included: 1) Pu metal reprocessing via direct oxide reduction, 2) Breakout of α-phase and δ-phase materials, 3) CNC machining of alloyed, δ-phase Pu metal, and 4) Low speed cutting of unalloyed, α-phase metal and alloyed, δ-phase Pu metal.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗