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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 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Evaluation of fuel cycle scenarios on MOX fuel recycling in PWRs and SFRs

Prospects on advanced fuel cycle scenario are considered for achieving a progressive integration of Sodium Fast Reactor (SFR) technology within the current French Pressurized Water Reactor (PWR) nuclear fleet, in a view to benefit from fissile material multi-recycling capability. A step by step process is envisioned, and emphasis is put on its potential implementation through the nuclear mass inventory calculations with the COSAC code. The overall time scale is not optimized. The first step, already implemented in several countries, the plutonium coming from the reprocessing of used Light Water Reactor (LWR) fuels is recycled into a small number of LWRs. The second step is the progressive introduction of the first SFRs, in parallel with the continuation of step 1. This second step lets to prepare the optimized multi recycling of MOX fuel which is considered in step 3. Step 3 is characterized by the introduction of a greater number of SFR and MOX management between EPR reactors and SFRs. In the final step 4, all the fleet is formed with SFRs. This study assesses the viability of each step of the overall scenario. The switch from one step to the other one could result from different constrains related to issues such as resources, waste, experience feedback, public acceptance, country policy, etc.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Two Dihydroxo-Bridged Plutonium(IV) Nitrate Dimers and Their Relevance to Trends in Tetravalent Ion Hydrolysis and Condensation

We report the room temperature synthesis and structural characterization of a μ2-hydroxobridged PuIV dimer obtained from an acidic, nitric acid solution. The discrete Pu 2 (OH) 2 (NO 3 ) 6 (H 2 O) 4 moiety crystallized with two distinct crystal structures, (1) [Pu 2 (OH) 2 (NO 3 ) 6 (H 2 O) 4 ] 2 ·11H 2 O and (2) Pu 2 (OH) 2 (NO 3 ) 6 (H 2 O) 4 ·2H 2 O, which differ primarily in the number of incorporated water molecules. High-energy X-ray scattering (HEXS) data obtained from the mother liquor showed evidence of a correlation at 3.7(10) Å but only after concentration of the stock solution. This distance is consistent with the dihydroxo-bridged distance of 3.799(1) Å seen in the solid-state structure as well as with the known Pu-Pu distance in PuO 2 . The structural characterization of a dihydroxo-bridged Pu moiety is discussed in terms of its relevance to the underlying mechanisms of tetravalent-metal-ion condensation

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Decommissioning the Belgonucleaire Dessel MOX plant: presentation of the project and situation end august 2013

Belgonucleaire has been operating the Dessel MOX plant at an industrial scale between 1986 and 2006. During this period, 40 metric tons of plutonium (HM) have been processed into 90 reloads of MOX fuel for commercial light water reactors. The decision to stop the production in 2006 and to decommission the MOX plant was the result of the shrinkage of the MOX fuel market due to political and commercial factors. As a significant part of the decommissioning project of the Dessel MOX plant, about 170 medium-sized glove-boxes and about 1.200 metric tons of structure and equipment outside the glove-boxes are planned for dismantling. The license for the dismantling of the MOX plant was granted by Royal Decree in 2008 and the dismantling started in March 2009. The dismantling works are carried out by an integrated organization under leadership and responsibility of Belgonucleaire; this organization includes 3 main contractors, namely Tecnubel N.V., the THV ('Tijdelijke HandelsVereniging') Belgoprocess / SCK-CEN and Studsvik GmbH and Tractebel Engineering as project manager. In this paper, after having described the main characteristics of the project, the authors review the different organizational and technical options considered for the decommissioning of the glove-boxes; thereafter the main decision criteria (qualification of personnel and of processes, confinement, cutting techniques and radiation protection, safety aspects, alpha-bearing waste management) are analyzed as well. Finally the progress, the feedback and the lessons learned at the end of August 2013 are presented, giving the principal's and contractors point of view. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

235-F GoldSim Fate and Transport Model: Uncertainty Quantification

Building 235-F was configured with two missions in mind: Actinide Billet Line (ABL) and the fabrication of Pu-238 oxide for space program applications. ABL produced Np-237 billets for use in SRS reactors, whereas the design process, fabrication, and examination of Pu-238 oxide powder occurred within the following areas, respectively: Plutonium Experimental Facility (PEF), Plutonium Fuel Form (PuFF), and Old Metallography Lab (OML). By 1990 production ceased and by 2006 de-inventory occurred; however, assays have shown significant holdup remains within ABL and PuFF. As a result, 235-F is a Category 2 nuclear facility, with plans to undergo deactivation and decommission (D and D) via In-Situ Disposal (ISD). The purpose of this project is to ensure United States Environmental Protection Agency (USEPA) groundwater radiation maximum contaminant level (MCL) and dosage standards are met during the D and D of 235-F by quantifying uncertainty through probabilistic modeling and evaluation of various ISD alternatives. GoldSim is a dynamic modeling software package with a graphical, object-oriented interface capable of capturing the influence of complex system input variability on probabilistic system outcomes. A GoldSim stochastic fate and transport model for 235-F was developed and matched with a PORFLOW deterministic model to simulate probabilistic release and flow of radionuclides from ABL and PuFF into the vadose zone, the Upper Three Runs (UTR) Aquifer, and UTR Creek. The GoldSim model was used to probabilistically evaluate four ISD scenarios against USEPA groundwater radiation MCLs and dosage standards. The deterministic 235-F GoldSim fate and transport model continues to be refined to match the results of the PORFLOW deterministic model to ensure the model accurately represents radionuclide movement through the groundwater system. The stochastic variables that are utilized within the GoldSim model are founded on the most current data; a conservative perspective is taken where needed. Alignment with the PORFLOW deterministic model, coupled with input stochastic variability, allows the probabilistic 235-F GoldSim model to capture the conservative breadth of possible outcomes for radionuclide fate within this particular system. This ensures that the USEPA MCLs and dosage limits hold even in the worst case scenarios.

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

Kinetics of the high temperature oxygen exchange reaction on 238 PuO 2 powder

In this study, oxygen exchange reactions performed on PuO 2 suggest the reaction is influenced by at least three mechanisms: an internal chemical reaction, surface mobility of active species/defects, and surface exchange of gaseous oxygen with lattice oxygen. Activation energies for the surface mobility and internal chemical reaction are presented. Determining which mechanism is dominant appears to be a complex function including at least specific surface area and temperature. Thermal exposure may also impact the oxygen exchange reaction by causing reductions in the specific surface area of PuO 2 . Previous CeO 2 surrogate studies exhibit similar behavior, confirming that CeO 2 is a good qualitative surrogate for PuO 2 , in regards to the oxygen exchange reaction. Comparison of results presented here with previous work on the PuO 2 oxygen exchange reaction allows complexities in the previous work to be explained. These explanations allowed new conclusions to be drawn, many of which confirm the conclusions presented here.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2012

Analytical Capability of Plasma Spectrometry Team [Slides]

Samples analyzed were: (1) Pu and U metal; (2) Pu oxide for nuclear fuel; (3) 23 8Pu oxide for heat source; and (4) Nuclear forensic samples - filters, swipes. Sample preparations that we did were: metal dissolution, marple filter dissolution, Pu oxide closed vessel acid digestion, and column separation to remove Pu.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Progress Summary: Conducting quantum simulations of surface reactivity on actinide surfaces

Motivation: Surface chemistry of plutonium, uranium, and their oxides from gases in the ambient atmosphere of the application environment presents significant challenges due to the high degree of reactivity of the substrate and the ubiquity of these gases in experimental setups. Significance: Relatively little is known about the chemical mechanism and reaction rates for hydriding, and experimental studies would greatly benefit from detailed atomistic knowledge of the chemical reactivity on Pu and Pu-oxide surfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Improved PARE (Pressurized Airborne Release Equipment) for Damage Ratio, Airborne Release Fraction and Respirable Fraction Testing (Version 4)

This paper describes an improved version of the PARE (Pressurized Airborne Release Equipment) system (Sutter 1983a and Sutter 1983b and Ballinger et al 1987) for powder venting testing. This effort seeks to improve the accuracy of risk estimation for the venting of pressurized powders and the venting of gases through pressurized powders. This includes experimental measurement for estimating DR (damage ratio), ARF (airborne release fraction) and RF (respirable fraction) quantities. The present study was performed to address previously indicated problematic factors (i.e. noted gaps) (US DOE 1994).

42 ENGINEERING↗
NASA NTRS1972

Radiation from plutonium 238 used in space applications

The principal mode of the nuclear decay of plutonium 238 is by alpha particle emission at a rate of 17 curies per gram. Gamma radiation also present in nuclear fuels arises primarily from the nuclear de-excitation of daughter nuclei as a result of the alpha decay of plutonium 238 and reactor-produced impurities. Plutonium 238 has a spontaneous fission half life of 4.8 x 10 to the 10th power years. Neutrons associated with this spontaneous fission are emitted at a rate of 28,000 neutrons per second per gram. Since the space fuel form of plutonium 238 is the oxide pressed into a cermet with molybdenum, a contribution to the neutron emission rate arises from (alpha, n) reactions with 0-17 and 0-18 which occur in natural oxygen.

Keenan, T. K.↗
DOE OSTI2013

Analysis of advanced european nuclear fuel cycle scenarios including transmutation and economical estimates

In this work the transition from the existing Light Water Reactors (LWR) to the advanced reactors is analyzed, including Generation III+ reactors in a European framework. Four European fuel cycle scenarios involving transmutation options have been addressed. The first scenario (i.e., reference) is the current fleet using LWR technology and open fuel cycle. The second scenario assumes a full replacement of the initial fleet with Fast Reactors (FR) burning U-Pu MOX fuel. The third scenario is a modification of the second one introducing Minor Actinide (MA) transmutation in a fraction of the FR fleet. Finally, in the fourth scenario, the LWR fleet is replaced using FR with MOX fuel as well as Accelerator Driven Systems (ADS) for MA transmutation. All scenarios consider an intermediate period of GEN-III+ LWR deployment and they extend for a period of 200 years looking for equilibrium mass flows. The simulations were made using the TR-EVOL code, a tool for fuel cycle studies developed by CIEMAT. The results reveal that all scenarios are feasible according to nuclear resources demand (U and Pu). Concerning to no transmutation cases, the second scenario reduces considerably the Pu inventory in repositories compared to the reference scenario, although the MA inventory increases. The transmutation scenarios show that elimination of the LWR MA legacy requires on one hand a maximum of 33% fraction (i.e., a peak value of 26 FR units) of the FR fleet dedicated to transmutation (MA in MOX fuel, homogeneous transmutation). On the other hand a maximum number of ADS plants accounting for 5% of electricity generation are predicted in the fourth scenario (i.e., 35 ADS units). Regarding the economic analysis, the estimations show an increase of LCOE (Levelized cost of electricity) - averaged over the whole period - with respect to the reference scenario of 21% and 29% for FR and FR with transmutation scenarios respectively, and 34% for the fourth scenario. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2013

New approaches for MOX multi-recycling

Due to its low fissile content after irradiation, Pu from used MOX fuel is considered by some as not recyclable in LWR (Light Water Reactors). The point of this paper is hence to go back to those statements and provide a new analysis based on AREVA extended experience in the fields of fissile and fertile material management and optimized waste management. This is done using the current US fuel inventory as a case study. MOX Multi-recycling in LWRs is a closed cycle scenario where U and Pu management through reprocessing and recycling leads to a significant reduction of the used assemblies to be stored. The recycling of Pu in MOX fuel is moreover a way to maintain the self-protection of the Pu-bearing assemblies. With this scenario, Pu content is also reduced repetitively via a multi-recycling of MOX in LWRs. Simultaneously, {sup 238}Pu content decreases. All along this scenario, HLW (High-Level Radioactive Waste) vitrified canisters are produced and planned for deep geological disposal. Contrary to used fuel, HLW vitrified canisters do not contain proliferation materials. Moreover, the reprocessing of used fuel limits the space needed on current interim storage. With MOX multi-recycling in LWR, Pu isotopy needs to be managed carefully all along the scenario. The early introduction of a limited number of SFRs (Sodium Fast Reactors) can therefore be a real asset for the overall system. A few SFRs would be enough to improve the Pu isotopy from used LWR MOX fuel and provide a Pu-isotopy that could be mixed back with multi-recycled Pu from LWRs, hence increasing the Pu multi-recycling potential in LWRs.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2019

Characterization of Tc-99 Speciation and Chemical Composition of 241-AN-102 Tank Waste Supernatant - 19201

Technetium (Tc) in its isotopic form {sup 99}Tc is generated in high yields from the fission of {sup 235}U and {sup 239}Pu. A significant inventory of {sup 99}Tc remains at the U.S. Department of Energy's Hanford Site, and it is one of the most difficult contaminants to address. In the strongly alkaline solutions that are typical of Hanford tank waste, Tc exists as both pertechnetate (TcO{sub 4}{sup -} in oxidation state VII) and in reduced forms (oxidation state <VII) collectively known as non-pertechnetate species. Pertechnetate is a well-characterized anionic Tc species that can be removed from low-activity waste by anion exchange or other methods. There is no definitive information on the origin or a comprehensive description of the non-pertechnetate species in Hanford tanks. Designing strategies for effective management of Tc, including separation and immobilization, requires an understanding of the molecular structure of the non-pertechnetate species and their identification in actual tank waste samples. Developing this advanced understanding would facilitate development of new technologies for treating dissimilar Tc species. Toward this objective, a spectroscopic library of the Tc(I) [fac-Tc(CO){sub 3}]{sup +} and Tc(IV, VI, VII) compounds was generated using a range of techniques and applied to the characterization of actual 241-AN-102 tank waste supernatant. A sample of the 241-AN-102 tank waste (collected in 2013) was processed to remove {sup 137}Cs by spherical resorcinol-formaldehyde (sRF) ion exchange resin after the sodium concentration was adjusted to 5.6 M. The Cs-loaded sRF column was eluted with 0.45 M HNO{sub 3}. As-received AN-102, Cs-depleted AN-102 effluent, and sRF eluate fractions were comprehensively characterized for chemical composition and speciation of Tc using {sup 99}Tc nuclear magnetic resonance (NMR) spectroscopy and X-ray absorption spectroscopy. The results of these analyses demonstrated for the first time that non-pertechnetate Tc present in the 241-AN-102 tank waste is composed of several low-valent Tc species, including the Tc(I) [fac-Tc(CO){sub 3}L{sub 3}]{sup +}, Tc(IV), and possibly Tc(VI) compounds. This is the second experimental observation of the [fac-Tc(CO){sub 3}L{sub 3}]{sup +} species in the Hanford tank waste that highlights their importance for waste processing. In addition, the chemical composition of the 241-AN-102 tank waste was characterized with the focus on small chelators. (authors)

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

Impact of Isotope Fidelity on Fuel Cycle Calculations

The purpose of this study is to examine the importance of the isotopic composition of plutonium on PWR MOX fuel fabrication as part of a multi-tiered fuel cycle, and the effect of its evolution during a transition. Two main effects can modify the isotopic composition of the plutonium used to build the PWR-MOX fuel: decay and depletion. This analysis is based on a transition of the nuclear fuel cycle to a configuration identified as 'Evaluation Group 29' or 'EG29', in the recently-published Evaluation and Screening (E and S) report. The EG29 fuel cycle corresponds to a double strata fleet. The first stratum is composed of sodium-cooled fast reactors (SFRs) multi-recycling plutonium. Surplus plutonium is sent to the second stratum composed of pressurized water reactors with full mixed oxide (U/Pu)O{sub 2} cores (MOX-PWRs). The PWR stratum is also multi-recycling its plutonium. The target energy generation ratio for the final EG29 system is 70:30 (SFR:PWR), with a 1% annual growth in nuclear energy demand. All the calculation of this study have been performed using the Cyclus fuel cycle simulator framework. The facility models are from the Cycamore package, developed by the Cyclus team, and containing a Pu-equivalent fuel fabrication model as well as a simple fixed mixing ratio fuel fabrication model. A new neural network model has also been contributed to the Cyclus environment using the cyCLASS tool, allowing the use of the fuel fabrication and depletion models from the CLASS tool in Cyclus. (authors)

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2022

Quantitative XPS of plutonium: Evaluation of the Pu4f peak shape, relative sensitivity factors and estimated detection limits

We report that high-resolution X-ray photoelectron spectra have been acquired from sputter cleaned and in situ oxidized samples of α-plutonium and a face-centred cubic δ-plutonium–gallium alloy. The differences in the Pu4f peak shape in these two materials have been investigated, and the poorly screened satellite peaks have been quantified. Curve fitting parameters for the Pu4p 3/2 , Pu4d 5/2 , Pu4f and Pu6p 3/2 photoelectron peaks are reported, and relative sensitivity factors have been determined. The Pu4f curve fit model has been applied to data acquired using different spectrometers and alloys. Examples of quantification of the plutonium spectra are provided and minimum detection limits are calculated for common impurities in plutonium metal.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Building flexibility into the design of a pilot plant for the immobilisation of Pu containing residues and wastes

NNL and ANSTO on behalf of Sellafield Ltd have developed a process for the immobilisation of a range of Pu containing wastes and residues. Following the inactive demonstration of the technology the project is now focusing on the design of an active pilot plant capable of validating the technology and ultimately immobilising a waste inventory containing around 100 kg plutonium. The diverse wastes from which it is uneconomic to recover Pu, require a flexible process with a wide product envelope capable of producing a wasteform suitable for disposal in a UK repository. Ceramics, glass ceramics and metal encapsulated waste-forms can be delivered by the process line which incorporates size reduction and heat treatment techniques with the aim of feeding a hot isostatic pressing process designed to deliver the highly durable waste-forms. Following a demonstration of feasibility, flowsheet development is progressing to support the design which has the aim of a fully flexible facility based in NNL's Central Laboratory on the Sellafield site. Optimisation of the size reduction, mixing and blending operations is being carried out using UO{sub 2} as a surrogate for PuO{sub 2}. This work is supporting the potential of using an enhanced glass ceramic formulation in place of the full ceramic with the aim of simplifying glove box operations. Heat treatment and subsequent HIPing strategies are being explored in order to eliminate any carbon from the feeds without increasing the valence state of the uranium present in some of the inventory which can result in an unwanted increase in wasteform volumes. The HIP and ancillary systems are being specifically designed to meet the requirements of the Sellafield site and within the constraints of the NNL Central Laboratory. The HIP is being configured to produce consolidated product cans consistent with the requirements of ongoing storage and disposal. With the aim of one cycle per day, the facility will deliver its mission of immobilising the identified waste and residues inventory within 3 years. During that period it will also be used to demonstrate the potential of this technology to deliver the immobilisation of a proportion of the UK plutonium stockpile that may not be suitable for use as MOx fuel should that decision be taken. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

An economic analysis of a light and heavy water moderated reactor synergy: burning americium using recycled uranium

An economic analysis is presented for a proposed synergistic system between 2 nuclear utilities, one operating light water reactors (LWR) and another running a fleet of heavy water moderated reactors (HWR). Americium is partitioned from LWR spent nuclear fuel (SNF) to be transmuted in HWRs, with a consequent averted disposal cost to the LWR operator. In return, reprocessed uranium (RU) is supplied to the HWRs in sufficient quantities to support their operation both as power generators and americium burners. Two simplifying assumptions have been made. First, the economic value of RU is a linear function of the cost of fresh natural uranium (NU), and secondly, plutonium recycling for a third utility running a mixed oxide (MOX) fuelled reactor fleet has been already taking place, so that the extra cost of americium recycling is manageable. We conclude that, in order for this scenario to be economically attractive to the LWR operator, the averted disposal cost due to partitioning americium from LWR spent fuel must exceed 214 dollars per kg, comparable to estimates of the permanent disposal cost of the high level waste (HLW) from reprocessing spent LWR fuel. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2013

Comparison of REMIX vs. MOX fuel characteristics in multiple recycling in VVER reactor

Multiple recycling of regenerated uranium-plutonium fuel in thermal reactors of VVER-1000 type with high enriched uranium feeding (REMIX-fuel) gives a possibility to terminate the accumulation of spent nuclear fuels (SNF) and Pu and decrease the accumulation of irradiated uranium by an order of magnitude. Results of comparison of VVER-1000 nuclear fuel cycle characteristics vs different fuel types such as UOX, MOX and REMIX-fuel have been presented. REMIX fuel (Regenerated Mixture of U-, Pu oxides) is the mixture of plutonium and uranium extracted from SNF and refined from other actinides and fission products with the addition of enriched uranium to provide the power potential necessary. The savings in terms of uranium quantities and separation works in the nuclear energy system (NES) with reactors using REMIX-fuel compared to the NES with uranium-fuelled reactors are shown to be of about 30% and 8%, respectively. For the NES with thermal reactors partially loaded with MOX-fuel, the uranium and separation works saving of about 14% would be obtained. Production of neptunium and americium in reactors with REMIX-fuel in steady state increases by a factor 3, and production of curium - by 10 compared to the reactors with UOX-fuel. This increase of minor actinide buildup is owed to the multiple recycling of plutonium. It should be noted that in this case all fuel assemblies contain high-background plutonium, and their manufacturing involves an expensive technology. Besides, management of REMIX-fuel will require special protection measures even during the fresh fuel manufacturing phase. The above-said gives ground to state that the use of REMIX fuel would be questionable in economic aspect.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Sources, seasonal cycling, and fate of plutonium in a seasonally stratified and radiologically contaminated pond

Unlike short-term laboratory experiments, studies at sites historically contaminated with radionuclides can provide insight into contaminant migration behavior at environmentally-relevant decadal timescales. One such site is Pond B, a seasonally stratified reservoir within Savannah River Site (SC, USA) has low levels (μBq L –1 ) of plutonium in the water column. Here, we evaluate the origin of plutonium using high-precision isotope measurements, investigate the impact of water column geochemistry on plutonium cycling during different stratification periods, and re-evaluate long-term mass balance of plutonium in the pond. New isotopic data confirm that reactor-derived plutonium overwhelms input from Northern Hemisphere fallout at this site. Two suggested mechanisms for observed plutonium cycling in the water column include: (1) reductive dissolution of sediment-derived Fe(III)-(oxyhydr)oxides during seasonal stratification and (2) plutonium stabilization complexed strongly to Fe(III)-particulate organic matter (POM) complexes. While plutonium may be mobilized to a limited extent by stratification and reductive dissolution, peak plutonium concentrations are in shallow waters and associated with Fe(III)-POM at the inception of stratification. This suggests that plutonium release from sediments during stratification is not the dominant mechanism driving plutonium cycling in the pond. Importantly, our analysis suggests that the majority is retained in shallow sediments and may become increasingly recalcitrant.

54 ENVIRONMENTAL SCIENCES↗