Analysis of the Gas Core Actinide Transmutation Reactor (GCATR)

NASA Technical Reports Server (NTRS)

Clement, J. D.; Rust, J. H.

1977-01-01

Design power plant studies were carried out for two applications of the plasma core reactor: (1) As a breeder reactor, (2) As a reactor able to transmute actinides effectively. In addition to the above applications the reactor produced electrical power with a high efficiency. A reactor subsystem was designed for each of the two applications. For the breeder reactor, neutronics calculations were carried out for a U-233 plasma core with a molten salt breeding blanket. A reactor was designed with a low critical mass (less than a few hundred kilograms U-233) and a breeding ratio of 1.01. The plasma core actinide transmutation reactor was designed to transmute the nuclear waste from conventional LWR's. The spent fuel is reprocessed during which 100% of Np, Am, Cm, and higher actinides are separated from the other components. These actinides are then manufactured as oxides into zirconium clad fuel rods and charged as fuel assemblies in the reflector region of the plasma core actinide transmutation reactor. In the equilibrium cycle, about 7% of the actinides are directly fissioned away, while about 31% are removed by reprocessing.

Study on the leaching behavior of actinides from nuclear fuel debris

NASA Astrophysics Data System (ADS)

Kirishima, Akira; Hirano, Masahiko; Akiyama, Daisuke; Sasaki, Takayuki; Sato, Nobuaki

2018-04-01

For the prediction of the leaching behavior of actinides contained in the nuclear fuel debris generated by the Fukushima Daiichi nuclear power plant accident in Japan, simulated fuel debris consisting of a UO2-ZrO2 solid solution doped with 137Cs, 237Np, 236Pu, and 241Am tracers was synthesized and investigated. The synthesis of the debris was carried out by heat treatment at 1200 °C at different oxygen partial pressures, and the samples were subsequently used for leaching tests with Milli-Q water and seawater. The results of the leaching tests indicate that the leaching of actinides depends on the redox conditions under which the debris was generated; for example, debris generated under oxidative conditions releases more actinide nuclides to water than that generated under reductive conditions. Furthermore, we found that, as Zr(IV) increasingly substituted U(IV) in the fluorite crystal structure of the debris, the actinide leaching from the debris decreased. In addition, we found that seawater leached more actinides from the debris than pure water, which seems to be caused by the complexation of actinides by carbonate ions in seawater.

Impact of Including Higher Actinides in Fast Reactor Transmutation Analyses

DOE Office of Scientific and Technical Information (OSTI.GOV)

B. Forget; M. Asgari; R. Ferrer

2007-09-01

Previous fast reactor transmutation studies generally disregarded higher mass minor actinides beyond Cm-246 due to various considerations including deficiencies in nuclear cross-section data. Although omission of these higher mass actinides does not significantly impact the neutronic calculations and fuel cycle performance parameters follow-on neutron dose calculations related to fuel recycling, transportation and handling are significantly impacted. This report shows that including the minor actinides in the equilibrium fast reactor calculations will increase the predicted neutron emission by about 30%. In addition a sensitivity study was initiated by comparing the impact of different cross-section evaluation file for representing these minor actinides.

Importance of the (n,gamma) Cm-247 Evaluation on Neutron Emission in Fast Reactor Fuel Cycle Analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Benoit Forget; Mehdi Asgari; Rodolfo M. Ferrer

2007-11-01

As part of the GNEP program, it is envisioned to build a fast reactor for the transmutation of minor actinides. The spent nuclear fuel from the current fleet of light water reactors would be recycled, the current baseline is the UREX+1a process, and would act as a feed for the fast reactor. As the fuel is irradiated in a fast reactor a certain quantity of minor actinides would thus build up in the fuel stream creating possible concerns with the neutron emission of these minor actinides for fuel transportation, handling and fabrication. Past neutronic analyses had not tracked minor actinidesmore » above Cm-246 in the transmutation chain, because of the small influence on the overall reactor performance and cycle parameters. However, when trying to quantify the neutron emission from the recycled fuel with high minor actinide content, these higher isotopes play an essential role and should be included in the analysis. In this paper, the influence of tracking these minor actinides on the calculated neutron emission is presented. Also presented is the particular influence of choosing a different evaluated cross section data set to represent the minor actinides above Cm-246. The first representation uses the cross-sections provided by MC2-2 for all isotopes, while the second representation uses infinitely diluted ENDF/BVII.0 cross-sections for Cm-247 to Cf-252 and MC2-2 for all other isotopes.« less

Method for preparing actinide nitrides

DOEpatents

Bryan, G.H.; Cleveland, J.M.; Heiple, C.R.

1975-12-01

Actinide nitrides, and particularly plutonium and uranium nitrides, are prepared by reacting an ammonia solution of an actinide compound with an ammonia solution of a reactant or reductant metal, to form finely divided actinide nitride precipitate which may then be appropriately separated from the solution. The actinide nitride precipitate is particularly suitable for forming nuclear fuels.

Decay heat power of spent nuclear fuel of power reactors with high burnup at long-term storage

NASA Astrophysics Data System (ADS)

Ternovykh, Mikhail; Tikhomirov, Georgy; Saldikov, Ivan; Gerasimov, Alexander

2017-09-01

Decay heat power of actinides and fission products from spent nuclear fuel of power VVER-1000 type reactors at long-term storage is calculated. Two modes of storage are considered: mode in which single portion of actinides or fission products is loaded in storage facility, and mode in which actinides or fission products from spent fuel of one VVER reactor are added every year in storage facility during 30 years and then accumulated nuclides are stored without addition new nuclides. Two values of fuel burnup 40 and 70 MW·d/kg are considered for the mode of storage of single fuel unloading. For the mode of accumulation of spent fuel with subsequent storage, one value of burnup of 70 MW·d/kg is considered. Very long time of storage 105 years accepted in calculations allows to simulate final geological disposal of radioactive wastes. Heat power of fission products decreases quickly after 50-100 years of storage. The power of actinides decreases very slow. In passing from 40 to 70 MW·d/kg, power of actinides increases due to accumulation of higher fraction of 244Cm. These data are important in the back end of fuel cycle when improved cooling system of the storage facility will be required along with stronger radiation protection during storage, transportation and processing.

Actinides in the Geosphere

NASA Astrophysics Data System (ADS)

Runde, Wolfgang; Neu, Mary P.

Since the 1950s actinides have been used to benefit industry, science, health, and national security. The largest industrial application, electricity generation from uranium and thorium fuels, is growing worldwide. Thus, more actinides are being mined, produced, used and processed than ever before. The future of nuclear energy hinges on how these increasing amounts of actinides are contained in each stage of the fuel cycle, including disposition. In addition, uranium and plutonium were built up during the Cold War between the United States and the Former Soviet Union for defense purposes and nuclear energy.

Zirconium behaviour during electrorefining of actinide-zirconium alloy in molten LiCl-KCl on aluminium cathodes

NASA Astrophysics Data System (ADS)

Meier, R.; Souček, P.; Malmbeck, R.; Krachler, M.; Rodrigues, A.; Claux, B.; Glatz, J.-P.; Fanghänel, Th.

2016-04-01

A pyrochemical electrorefining process for the recovery of actinides from metallic nuclear fuel based on actinide-zirconium alloys (An-Zr) in a molten salt is being investigated. In this process actinides are group-selectively recovered on solid aluminium cathodes as An-Al alloys using a LiCl-KCl eutectic melt at a temperature of 450 °C. In the present study the electrochemical behaviour of zirconium during electrorefining was investigated. The maximum amount of actinides that can be oxidised without anodic co-dissolution of zirconium was determined at a selected constant cathodic current density. The experiment consisted of three steps to assess the different stages of the electrorefining process, each of which employing a fresh aluminium cathode. The results indicate that almost a complete dissolution of the actinides without co-dissolution of zirconium is possible under the applied experimental conditions.

Actinides in metallic waste from electrometallurgical treatment of spent nuclear fuel

NASA Astrophysics Data System (ADS)

Janney, D. E.; Keiser, D. D.

2003-09-01

Argonne National Laboratory has developed a pyroprocessing-based technique for conditioning spent sodium-bonded nuclear-reactor fuel in preparation for long-term disposal. The technique produces a metallic waste form whose nominal composition is stainless steel with 15 wt.% Zr (SS-15Zr), up to ˜ 11 wt.% actinide elements (primarily uranium), and a few percent metallic fission products. Actual and simulated waste forms show similar eutectic microstructures with approximately equal proportions of iron solid solution phases and Fe-Zr intermetallics. This article reports on an analysis of simulated waste forms containing uranium, neptunium, and plutonium.

Yttrium and rare earth stabilized fast reactor metal fuel

DOEpatents

Guon, Jerold; Grantham, LeRoy F.; Specht, Eugene R.

1992-01-01

To increase the operating temperature of a reactor, the melting point and mechanical properties of the fuel must be increased. For an actinide-rich fuel, yttrium, lanthanum and/or rare earth elements can be added, as stabilizers, to uranium and plutonium and/or a mixture of other actinides to raise the melting point of the fuel and improve its mechanical properties. Since only about 1% of the actinide fuel may be yttrium, lanthanum, or a rare earth element, the neutron penalty is low, the reactor core size can be reduced, the fuel can be burned efficiently, reprocessing requirements are reduced, and the nuclear waste disposal volumes reduced. A further advantage occurs when yttrium, lanthanum, and/or other rare earth elements are exposed to radiation in a reactor, they produce only short half life radioisotopes, which reduce nuclear waste disposal problems through much shorter assured-isolation requirements.

Hydrothermal Synthesis and Crystal Structures of Actinide Compounds

NASA Astrophysics Data System (ADS)

Runde, Wolfgang; Neu, Mary P.

Since the 1950s actinides have been used to benefit industry, science, health, and national security. The largest industrial application, electricity generation from uranium and thorium fuels, is growing worldwide. Thus, more actinides are being mined, produced, used and processed than ever before. The future of nuclear energy hinges on how these increasing amounts of actinides are contained in each stage of the fuel cycle, including disposition. In addition, uranium and plutonium were built up during the Cold War between the United States and the Former Soviet Union for defense purposes and nuclear energy. These stockpiles have been significantly reduced in the last decade.

DOE Office of Scientific and Technical Information (OSTI.GOV)

R. Wigeland; T. Taiwo; M. Todosow

The recently completed comprehensive evaluation and screening of nuclear fuel cycle options identified a number of potentially promising fuel cycles for R&D that offer what could be considered by decision-makers as having the potential for significant improvement compared to the current U.S. fuel cycle. The fuel cycles that consistently performed the best were recycle fuel cycles that used self-sustaining fast reactors operating with either U/Pu or U/TRU recycle fuel and also included options where the fast reactors provided fissile materials to support operation of thermal reactors. However, based on the evaluation criteria and metrics used in the study, there wasmore » no difference in benefit between recycle of U/Pu and U/TRU (where TRU is plutonium and the minor actinides) while there were differences in the challenges for developing and deploying such fuel cycles, with U/TRU recycle being more challenging. This observation prompted the question as to the desirability of pursuing R&D on U/TRU recycle given that there may not be an increase in benefit. As a result, activities have been pursued to further investigate the performance differences between U/Pu and U/TRU recycle based on considering issues beyond those used in the evaluation and screening study to identify, if possible, areas where there are significant benefits of U/TRU recycle compared to U/Pu recycle. These new considerations focused on several areas, but especially on the impact on disposal of the HLW, which in the case of U/Pu recycle contains all of the minor actinides along with fission products, while in the case of U/TRU recycle only contains the losses of minor actinides from the reprocessing and recycle fuel fabrication operations. This difference in content has several implications. One impact is on the time dependent decay heat which can affect handling and the use of space in a geologic repository. Another impact concerns the HLW form and volume, since presence of minor actinides may adversely affect the ability to reduce HLW volume. The short-term radioactivity and long-term radiotoxicity of the HLW is also affected, which may be of more or less importance depending on the specific geologic disposal environment. To study these potential effects, a range of waste forms and disposal environments were used in the analysis, documenting to what extent the recycle of minor actinides in addition to plutonium may offer further benefit. Another area of investigation concerned the recycle fuel, for the fast reactor and for the thermal reactors they may support. Information to date indicates that U/Pu fuel may be simpler to fabricate and has a much more extensive database than U/TRU fuel, one of the reasons for the increased challenge for developing and deploying a U/TRU fuel cycle, and also indicates that heterogeneous recycle of the minor actinides may be even more difficult as compared to homogeneous recycle. This information was reviewed and updated to reflect the most recent studies for the purpose of informing on all aspects of the differences between U/Pu and U/TRU recycle. The results of all of these investigations will be presented to provide information on the findings concerning the value of U/TRU recycle.« less

Method for reprocessing and separating spent nuclear fuels. [Patent application

DOEpatents

Krikorian, O.H.; Grens, J.Z.; Parrish, W.H. Sr.

1982-01-19

Spent nuclear fuels, including actinide fuels, volatile and nonvolatile fission products, are reprocessed and separated in a molten metal solvent housed in a separation vessel made of a carbon-containing material. A first catalyst, which promotes the solubility and permeability of carbon in the metal solvent, is included. By increasing the solubility and permeability of the carbon in the solvent, the rate at which actinide oxides are reduced (carbothermic reduction) is greatly increased. A second catalyst, included to increase the affinity for nitrogen in the metal solvent, is added to increase the rate at which actinide nitrides form after carbothermic reduction is complete.

Dissolution behavior of MgO based inert matrix fuel for the transmutation of minor actinides

NASA Astrophysics Data System (ADS)

Mühr-Ebert, E. L.; Lichte, E.; Bukaemskiy, A.; Finkeldei, S.; Klinkenberg, M.; Brandt, F.; Bosbach, D.; Modolo, G.

2018-07-01

This study explores the dissolution properties of magnesia-based inert matrix nuclear fuel (IMF) containing transuranium elements (TRU). Pure MgO pellets as well as MgO pellets containing CeO2, as surrogate for TRU oxides, and are considered as model systems for genuine magnesia based inert matrix fuel were fabricated. The aim of this study is to identify conditions at which the matrix material can be selectively dissolved during the head-end reprocessing step, allowing a separation of MgO from the actinides, whereas the actinides remain undissolved. The dissolution behavior was studied in macroscopic batch experiments as a function of nitric acid concentration, dissolution medium volume, temperature, stirring velocity, and pellet density (85, 90, 96, and 99%TD). To mimic pellets with various burn-ups the density of the here fabricated pellets was varied. MgO is soluble even under mild conditions (RT, 2.5 mol/L HNO3). The dissolution rates of MgO at different acid concentrations are rather similar, whereas the dissolution rate is strongly dependent on the temperature. Via a microscopic approach, a model was developed to describe the evolution of the pellet surface area during dissolution and determine a surface normalized dissolution rate. Moreover, dissolution rates of the inert matrix fuel containing CeO2 were determined as a function of the acid concentration and temperature. During the dissolution of MgO/CeO2 pellets the MgO dissolves completely, while CeO2 (>99%) remains undissolved. This study intends to provide a profound understanding of the chemical performance of magnesia based IMF containing fissile material. The feasibility of the dissolution of magnesia based IMF with nitric acid is discussed.

Apparatus and method for reprocessing and separating spent nuclear fuels. [Patent application

DOEpatents

Krikorian, O.H.; Grens, J.Z.; Parrish, W.H. Sr.; Coops, M.S.

1982-01-19

A method and apparatus for separating and reprocessing spent nuclear fuels includes a separation vessel housing a molten metal solvent in a reaction region, a reflux region positioned above and adjacent to the reaction region, and a porous filter member defining the bottom of the separation vessel in a supporting relationship with the metal solvent. Spent fuels are added to the metal solvent. A nonoxidizing nitrogen-containing gas is introduced into the separation vessel, forming solid actinide nitrides in the metal solvent from actinide fuels, while leaving other fission products in solution. A pressure of about 1.1 to 1.2 atm is applied in the reflux region, forcing the molten metal solvent and soluble fission products out of the vessel, while leaving the solid actinide nitrides in the separation vessel.

Apparatus and method for reprocessing and separating spent nuclear fuels. [Patent application

DOEpatents

Krikorian, O.H.; Grens, J.Z.; Parrish, W.H. Sr.

1982-01-19

Spent nuclear fuels, including actinide fuels, volatile and non-volatile fission products, are reprocessed and separated in a molten metal solvent housed in the reaction region of a separation vessel which includes a reflux region positioned above the molten tin solvent. The reflux region minimizes loss of evaporated solvent during the separation of the actinide fuels from the volatile fission products. Additionally, inclusion of the reflux region permits the separation of the more volatile fission products (noncondensable) from the less volatile ones (condensable).

The combined hybrid system: A symbiotic thermal reactor/fast reactor system for power generation and radioactive waste toxicity reduction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hollaway, W.R.

1991-08-01

If there is to be a next generation of nuclear power in the United States, then the four fundamental obstacles confronting nuclear power technology must be overcome: safety, cost, waste management, and proliferation resistance. The Combined Hybrid System (CHS) is proposed as a possible solution to the problems preventing a vigorous resurgence of nuclear power. The CHS combines Thermal Reactors (for operability, safety, and cost) and Integral Fast Reactors (for waste treatment and actinide burning) in a symbiotic large scale system. The CHS addresses the safety and cost issues through the use of advanced reactor designs, the waste management issuemore » through the use of actinide burning, and the proliferation resistance issue through the use of an integral fuel cycle with co-located components. There are nine major components in the Combined Hybrid System linked by nineteen nuclear material mass flow streams. A computer code, CHASM, is used to analyze the mass flow rates CHS, and the reactor support ratio (the ratio of thermal/fast reactors), IFR of the system. The primary advantages of the CHS are its essentially actinide-free high-level radioactive waste, plus improved reactor safety, uranium utilization, and widening of the option base. The primary disadvantages of the CHS are the large capacity of IFRs required (approximately one MW{sub e} IFR capacity for every three MW{sub e} Thermal Reactor) and the novel radioactive waste streams produced by the CHS. The capability of the IFR to burn pure transuranic fuel, a primary assumption of this study, has yet to be proven. The Combined Hybrid System represents an attractive option for future nuclear power development; that disposal of the essentially actinide-free radioactive waste produced by the CHS provides an excellent alternative to the disposal of intact actinide-bearing Light Water Reactor spent fuel (reducing the toxicity based lifetime of the waste from roughly 360,000 years to about 510 years).« less

Recovery of transplutonium elements from nuclear reactor waste

DOEpatents

Campbell, David O.; Buxton, Samuel R.

1977-05-24

A method of separating actinide values from nitric acid waste solutions resulting from reprocessing of irradiated nuclear fuels comprises oxalate precipitation of the major portion of actinide and lanthanide values to provide a trivalent fraction suitable for subsequent actinide/lanthanide partition, exchange of actinide and lanthanide values in the supernate onto a suitable cation exchange resin to provide an intermediate-lived raffinate waste stream substantially free of actinides, and elution of the actinide values from the exchange resin. The eluate is then used to dissolve the trivalent oxalate fraction prior to actinide/lanthanide partition or may be combined with the reprocessing waste stream and recycled.

Extending FEAST-METAL for analysis of low content minor actinide bearing and zirconium rich metallic fuels for sodium fast reactors

NASA Astrophysics Data System (ADS)

Karahan, Aydın

2011-07-01

Computational models in FEAST-METAL fuel behaviour code have been upgraded to simulate minor actinide bearing zirconium rich metallic fuels for use in sodium fast reactors. Increasing the zirconium content to 20-40 wt.% causes significant changes in fuel slug microstructure affecting thermal, mechanical, chemical, and fission gas behaviour. Inclusion of zirconium rich phase reduces the fission gas swelling rate significantly in early irradiation. Above the threshold fission gas swelling, formation of micro-cracks, and open pores increase material compliancy enhance diffusivity, leading to rapid fuel gas swelling, interconnected porosity development and release of the fission gases and helium. Production and release of helium was modelled empirically as a function of americium content and fission gas production, consistent with previous Idaho National Laboratory studies. Predicted fuel constituent redistribution is much smaller compared to typical U-Pu-10Zr fuel operated at EBR-II. Material properties such as fuel thermal conductivity, modulus of elasticity, and thermal expansion coefficient have been approximated using the available database. Creep rate and fission gas diffusivity of high zirconium fuel is lowered by an order of magnitude with respect to the reference low zirconium fuel based on limited database and in order to match experimental observations. The new code is benchmarked against the AFC-1F fuel assembly post irradiation examination results. Satisfactory match was obtained for fission gas release and swelling behaviour. Finally, the study considers a comparison of fuel behaviour between high zirconium content minor actinide bearing fuel and typical U-15Pu-6Zr fuel pins with 75% smear density. The new fuel has much higher fissile content, allowing for operating at lower neutron flux level compared to fuel with lower fissile density. This feature allows the designer to reach a much higher burnup before reaching the cladding dose limit. On the other hand, in order to accommodate solid fission product swelling and to control fuel clad mechanical interaction of the stiffer fuel, the fuel smear density is reduced to 70%. In addition, plenum height is increased to accommodate for fission gases.

Protected Nuclear Fuel Element

DOEpatents

Kittel, J. H.; Schumar, J. F.

1962-12-01

A stainless steel-clad actinide metal fuel rod for use in fast reactors is reported. In order to prevert cladding failures due to alloy formation between the actinide metal and the stainless steel, a mesh-like sleeve of expanded metal is interposed between them, the sleeve metal being of niobium, tantalum, molybdenum, tungsten, zirconium, or vanadium. Liquid alkali metal is added as a heat transfer agent. (AEC)

Aqueous and pyrochemical reprocessing of actinide fuels

NASA Astrophysics Data System (ADS)

Toth, L. Mac; Bond, Walter D.; Avens, Larry R.

1993-02-01

Processing of the nuclear fuel actinides has developed in two independent directions—aqueous processing and pyroprocessing. Similarities in the two processes, their goals, and restraints are indicated in brief parallel descriptions along with distinguishing advantages and areas of future development. It is suggested that from a technical viewpoint, the ultimate process might be a hybrid which incorporates the best steps of each process.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hayes, S. L.; Harp, J. M.; Chichester, H. J. M.

Research and development activities on metallic fuels in the US are focused on their potential use for actinide transmutation in future sodium fast reactors. As part of this application, there is a desire to demonstrate a multifold increase in burnup potential. A number of metallic fuel design innovations are under investigation with a view toward significantly increasing the burnup potential of metallic fuels, since higher discharge burnups equate to lower potential actinide losses during recycle. Promising innovations under investigation include: 1) lowering the fuel smeared density in order to accommodate the additional swelling expected as burnups increase, 2) utilizing anmore » annular fuel geometry for better geometrical stability at low smeared densities, as well as the potential to eliminate the need for a sodium bond, and 3) minor alloy additions to immobilize lanthanide fission products inside the metallic fuel matrix and prevent their transport to the cladding resulting in fuel-cladding chemical interaction. This paper presents results from these efforts to advance metallic fuel technology in support of high burnup and actinide transmutation objectives. Highlights include examples of fabrication of low smeared density annular metallic fuels, experiments to identify alloy additions effective in immobilizing lanthanide fission products, and early postirradiation examinations of annular metallic fuels having low smeared densities and palladium additions for fission product immobilization.« less

Incorporation mechanisms of actinide elements into the structures of U 6+ phases formed during the oxidation of spent nuclear fuel

NASA Astrophysics Data System (ADS)

Burns, Peter C.; Ewing, Rodney C.; Miller, Mark L.

1997-05-01

Uranyl oxide hydrate and uranyl silicate phases will form due to the corrosion and alteration of spent nuclear fuel under oxidizing conditions in silica-bearing solution. The actinide elements in the spent fuel may be incorporated into the structures of these secondary U6+ phases during the long-term corrosion of the UO 2 in spent fuel. The incorporation of actinide elements into the crystal structures of the alteration products may decrease actinide mobility. The crystal chemistry of the various oxidation states of the actinide elements of environmental concern is examined to identify possible incorporation mechanisms. The substitutions Pu 6+U 6+ and (Pu 5+, Np 5+)U 6+ should readily occur in many U 6+ structures, although structural modification may be required to satisfy local bond-valence requirements. Crystal-chemical characteristics of the U 6+ phases indicate that An 4+ (An: actinide)U 6+ substitution is likely to occur in the sheets of uranyl polyhedra that occur in the structures of the minerals schoepite, [(UO 2) 8O 2(OH) 12](H 2O) 12, ianthinite, [U 24+ (UO 2) 4O 6(OH) 4(H 2O) 4](H 2O) 5, becquerelite, Ca[(UO 2) 3O 2(OH) 3] 2(H 2O) 8, compreignacite, K 2[(UO 2) 3O 2(OH) 3] 2(H 2O) 8, α-uranophane, Ca[(UO 2)(SiO 3OH)] 2(H 2O) 5, and boltwoodite, K(H 2O)[(UO 2)(SiO 4)], all of which are likely to form due to the oxidation and alteration of the UO 2 in spent fuel. The incorporation of An 3+ into the sheets of the structures of α-uranophane and boltwoodite, as well as interlayer sites of various uranyl phases, may occur.

Advancing the scientific basis of trivalent actinide-lanthanide separations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nash, K.L.

For advanced fuel cycles designed to support transmutation of transplutonium actinides, several options have been demonstrated for process-scale aqueous separations for U, Np, Pu management and for partitioning of trivalent actinides and fission product lanthanides away from other fission products. The more difficult mutual separation of Am/Cm from La-Tb remains the subject of considerable fundamental and applied research. The chemical separations literature teaches that the most productive alternatives to pursue are those based on ligand donor atoms less electronegative than O, specifically N- and S-containing complexants and chloride ion (Cl{sup -}). These 'soft-donor' atoms have exhibited usable selectivity in theirmore » bonding interactions with trivalent actinides relative to lanthanides. In this report, selected features of soft donor reagent design, characterization and application development will be discussed. The roles of thiocyanate, aminopoly-carboxylic acids and lactate in separation processes are detailed. (authors)« less

Bias estimates used in lieu of validation of fission products and minor actinides in MCNP K eff calculations for PWR burnup credit casks

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mueller, Don E.; Marshall, William J.; Wagner, John C.

The U.S. Nuclear Regulatory Commission (NRC) Division of Spent Fuel Storage and Transportation recently issued Interim Staff Guidance (ISG) 8, Revision 3. This ISG provides guidance for burnup credit (BUC) analyses supporting transport and storage of PWR pressurized water reactor (PWR) fuel in casks. Revision 3 includes guidance for addressing validation of criticality (k eff) calculations crediting the presence of a limited set of fission products and minor actinides (FP&MA). Based on previous work documented in NUREG/CR-7109, recommendation 4 of ISG-8, Rev. 3, includes a recommendation to use 1.5 or 3% of the FP&MA worth to conservatively cover the biasmore » due to the specified FP&MAs. This bias is supplementary to the bias and bias uncertainty resulting from validation of k eff calculations for the major actinides in SNF and does not address extension to actinides and fission products beyond those identified herein. The work described in this report involves comparison of FP&MA worths calculated using SCALE and MCNP with ENDF/B-V, -VI, and -VII based nuclear data and supports use of the 1.5% FP&MA worth bias when either SCALE or MCNP codes are used for criticality calculations, provided the other conditions of the recommendation 4 are met. The method used in this report may also be applied to demonstrate the applicability of the 1.5% FP&MA worth bias to other codes using ENDF/B V, VI or VII based nuclear data. The method involves use of the applicant s computational method to generate FP&MA worths for a reference SNF cask model using specified spent fuel compositions. The applicant s FP&MA worths are then compared to reference values provided in this report. The applicants FP&MA worths should not exceed the reference results by more than 1.5% of the reference FP&MA worths.« less

Magnesium transport extraction of transuranium elements from LWR fuel

DOEpatents

Ackerman, John P.; Battles, James E.; Johnson, Terry R.; Miller, William E.; Pierce, R. Dean

1992-01-01

A process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels which contain rare earth and noble metal fission products. The oxide fuel is reduced with Ca metal in the presence of CaCl.sub.2 and a U-Fe alloy containing not less than about 84% by weight uranium at a temperature in the range of from about 800.degree. C. to about 850.degree. C. to produce additional uranium metal which dissolves in the U-Fe alloy raising the uranium concentration and having transuranium actinide metals and rare earth fission product metals and the noble metal fission products dissolved therein. The CaCl.sub.2 having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein is separated and electrolytically treated with a carbon electrode to reduce the CaO to Ca metal while converting the carbon electrode to CO and CO.sub.2. The Ca metal and CaCl.sub.2 is recycled to reduce additional oxide fuel. The U-Fe alloy having transuranium actinide metals and rare earth fission product metals and the noble metal fission products dissolved therein is contacted with Mg metal which takes up the actinide and rare earth fission product metals. The U-Fe alloy retains the noble metal fission products and is stored while the Mg is distilled and recycled leaving the transuranium actinide and rare earth fission products isolated.

Optimisation of composite metallic fuel for minor actinide transmutation in an accelerator-driven system

NASA Astrophysics Data System (ADS)

Uyttenhove, W.; Sobolev, V.; Maschek, W.

2011-09-01

A potential option for neutralization of minor actinides (MA) accumulated in spent nuclear fuel of light water reactors (LWRs) is their transmutation in dedicated accelerator-driven systems (ADS). A promising fuel candidate dedicated to MA transmutation is a CERMET composite with Mo metal matrix and (Pu, Np, Am, Cm)O 2-x fuel particles. Results of optimisation studies of the CERMET fuel targeting to increasing the MA transmutation efficiency of the EFIT (European Facility for Industrial Transmutation) core are presented. In the adopted strategy of MA burning the plutonium (Pu) balance of the core is minimized, allowing a reduction in the reactivity swing and the peak power form-factor deviation and an extension of the cycle duration. The MA/Pu ratio is used as a variable for the fuel optimisation studies. The efficiency of MA transmutation is close to the foreseen theoretical value of 42 kg TW -1 h -1 when level of Pu in the actinide mixture is about 40 wt.%. The obtained results are compared with the reference case of the EFIT core loaded with the composite CERCER fuel, where fuel particles are incorporated in a ceramic magnesia matrix. The results of this study offer additional information for the EFIT fuel selection.

Development of spent fuel reprocessing process based on selective sulfurization: Study on the Pu, Np and Am sulfurization

NASA Astrophysics Data System (ADS)

Kirishima, Akira; Amano, Yuuki; Nihei, Toshifumi; Mitsugashira, Toshiaki; Sato, Nobuaki

2010-03-01

For the recovery of fissile materials from spent nuclear fuel, we have proposed a novel reprocessing process based on selective sulfurization of fission products (FPs). The key concept of this process is utilization of unique chemical property of carbon disulfide (CS2), i.e., it works as a reductant for U3O8 but works as a sulfurizing agent for minor actinides and lanthanides. Sulfurized FPs and minor actinides (MA) are highly soluble to dilute nitric acid while UO2 and PuO2 are hardly soluble, therefore, FPs and MA can be removed from Uranium and Plutonium matrix by selective dissolution. As a feasibility study of this new concept, the sulfurization behaviours of U, Pu, Np, Am and Eu are investigated in this paper by the thermodynamical calculation, phase analysis of chemical analogue elements and tracer experiments.

Fundamental Studies of Irradiation-Induced Defect Formation and Fission Product Dynamics in Oxide Fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stubbins, James

2012-12-19

The objective of this research program is to address major nuclear fuels performance issues for the design and use of oxide-type fuels in the current and advanced nuclear reactor applications. Fuel performance is a major issue for extending fuel burn-up which has the added advantage of reducing the used fuel waste stream. It will also be a significant issue with respect to developing advanced fuel cycle processes where it may be possible to incorporate minor actinides in various fuel forms so that they can be 'burned' rather than join the used fuel waste stream. The potential to fission or transmutemore » minor actinides and certain long-lived fission product isotopes would transform the high level waste storage strategy by removing the need to consider fuel storage on the millennium time scale.« less

Nuclear fuel alloys or mixtures and method of making thereof

DOEpatents

Mariani, Robert Dominick; Porter, Douglas Lloyd

2016-04-05

Nuclear fuel alloys or mixtures and methods of making nuclear fuel mixtures are provided. Pseudo-binary actinide-M fuel mixtures form alloys and exhibit: body-centered cubic solid phases at low temperatures; high solidus temperatures; and/or minimal or no reaction or inter-diffusion with steel and other cladding materials. Methods described herein through metallurgical and thermodynamics advancements guide the selection of amounts of fuel mixture components by use of phase diagrams. Weight percentages for components of a metallic additive to an actinide fuel are selected in a solid phase region of an isothermal phase diagram taken at a temperature below an upper temperature limit for the resulting fuel mixture in reactor use. Fuel mixtures include uranium-molybdenum-tungsten, uranium-molybdenum-tantalum, molybdenum-titanium-zirconium, and uranium-molybdenum-titanium systems.

ADS Model in the TIRELIRE-STRATEGIE Fuel Cycle Simulation Code Application to Minor Actinides Transmutation Studies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Garzenne, Claude; Massara, Simone; Tetart, Philippe

2006-07-01

Accelerator Driven Systems offer the advantage, thanks to the core sub-criticality, to burn highly radioactive elements such as americium and curium in a dedicated stratum, and then to avoid polluting with these elements the main part of the nuclear fleet, which is optimized for electricity production. This paper presents firstly the ADS model implemented in the fuel cycle simulation code TIRELIRE-STRATEGIE that we developed at EDF R and D Division for nuclear power scenario studies. Then we show and comment the results of TIRELIRE-STRATEGIE calculation of a transition scenario between the current French nuclear fleet, and a fast reactor fleetmore » entirely deployed towards the end of the 21. century, consistently with the EDF prospective view, with 3 options for the minor actinides management:1) vitrified with fission products to be sent to the final disposal; 2) extracted together with plutonium from the spent fuel to be transmuted in Generation IV fast reactors; 3) eventually extracted separately from plutonium to be incinerated in a ADSs double stratum. The comparison of nuclear fuel cycle material fluxes and inventories between these options shows that ADSs are not more efficient than critical fast reactors for reducing the high level waste radio-toxicity; that minor actinides inventory and fluxes in the fuel cycle are more than twice as high in case of a double ADSs stratum than in case of minor actinides transmutation in Generation IV FBRs; and that about fourteen 400 MWth ADS are necessary to incinerate minor actinides issued from a 60 GWe Generation IV fast reactor fleet, corresponding to the current French nuclear fleet installed power. (authors)« less

Synthesis and characterisation of PuPO4 - a potential analytical standard for EPMA actinide quantification

NASA Astrophysics Data System (ADS)

Wright, K. E.; Popa, K.; Pöml, P.

2018-01-01

Transmutation nuclear fuels contain weight percentage quantities of actinide elements, including Pu, Am and Np. Because of the complex spectra presented by actinide elements using electron probe microanalysis (EPMA), it is necessary to have relatively pure actinide element standards to facilitate overlap correction and accurate quantitation. Synthesis of actinide oxide standards is complicated by their multiple oxidation states, which can result in inhomogeneous standards or standards that are not stable at atmospheric conditions. Synthesis of PuP4 results in a specimen that exhibits stable oxidation-reduction chemistry and is sufficiently homogenous to serve as an EPMA standard. This approach shows promise as a method for producing viable actinide standards for microanalysis.

Free Energy and Heat Capacity

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kurata, Masaki; Devanathan, Ramaswami

2015-10-13

Free energy and heat capacity of actinide elements and compounds are important properties for the evaluation of the safety and reliable performance of nuclear fuel. They are essential inputs for models that describe complex phenomena that govern the behaviour of actinide compounds during nuclear fuel fabrication and irradiation. This chapter introduces various experimental methods to measure free energy and heat capacity to serve as inputs for models and to validate computer simulations. This is followed by a discussion of computer simulation of these properties, and recent simulations of thermophysical properties of nuclear fuel are briefly reviewed.

Interim waste storage for the Integral Fast Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Benedict, R.W.; Phipps, R.D.; Condiff, D.W.

1991-01-01

The Integral Fast Reactor (IFR), which Argonne National Laboratory is developing, is an innovative liquid metal breeder reactor that uses metallic fuel and has a close coupled fuel recovery process. A pyrochemical process is used to separate the fission products from the actinide elements. These actinides are used to make new fuel for the reactor. As part of the overall IFR development program, Argonne has refurbished an existing Fuel Cycle Facility at ANL-West and is installing new equipment to demonstrate the remote reprocessing and fabrication of fuel for the Experimental Breeder Reactor II (EBR-II). During this demonstration the wastes thatmore » are produced will be treated and packaged to produce waste forms that would be typical of future commercial operations. These future waste forms would, assuming Argonne development goals are fulfilled, be essentially free of long half-life transuranic isotopes. Promising early results indicate that actinide extraction processes can be developed to strip these isotopes from waste stream and return them to the IFR type reactors for fissioning. 1 fig.« less

Preliminary Analysis of High-Flux RSG-GAS to Transmute Am-241 of PWR’s Spent Fuel in Asian Region

NASA Astrophysics Data System (ADS)

Budi Setiawan, M.; Kuntjoro, S.

2018-02-01

A preliminary study of minor actinides (MA) transmutation in the high flux profile RSG-GAS research reactor was performed, aiming at an optimal transmutation loading for present nuclear energy development. The MA selected in the analysis includes Am-241 discharged from pressurized water reactors (PWRs) in Asian region. Until recently, studies have been undertaken in various methods to reduce radiotoxicity from actinides in high-level waste. From the cell calculation using computer code SRAC2006, it is obtained that the target Am-241 which has a cross section of the thermal energy absorption in the region (group 8) is relatively large; it will be easily burned in the RSG-GAS reactor. Minor actinides of Am-241 which can be inserted in the fuel (B/T fuel) is 2.5 kg which is equivalent to Am-241 resulted from the partition of spent fuel from 2 units power reactors PWR with power 1000MW(th) operated for one year.

Analysis on fuel breeding capability of FBR core region based on minor actinide recycling doping

DOE Office of Scientific and Technical Information (OSTI.GOV)

Permana, Sidik; Novitrian,; Waris, Abdul

Nuclear fuel breeding based on the capability of fuel conversion capability can be achieved by conversion ratio of some fertile materials into fissile materials during nuclear reaction processes such as main fissile materials of U-233, U-235, Pu-239 and Pu-241 and for fertile materials of Th-232, U-238, and Pu-240 as well as Pu-238. Minor actinide (MA) loading option which consists of neptunium, americium and curium will gives some additional contribution from converted MA into plutonium such as conversion Np-237 into Pu-238 and it's produced Pu-238 converts to Pu-239 via neutron capture. Increasing composition of Pu-238 can be used to produce fissilemore » material of Pu-239 as additional contribution. Trans-uranium (TRU) fuel (Mixed fuel loading of MOX (U-Pu) and MA composition) and mixed oxide (MOX) fuel compositions are analyzed for comparative analysis in order to show the effect of MA to the plutonium productions in core in term of reactor criticality condition and fuel breeding capability. In the present study, neptunium (Np) nuclide is used as a representative of MAin trans-uranium (TRU) fuel composition as Np-MOX fuel type. It was loaded into the core region gives significant contribution to reduce the excess reactivity in comparing to mixed oxide (MOX) fuel and in the same time it contributes to increase nuclear fuel breeding capability of the reactor. Neptunium fuel loading scheme in FBR core region gives significant production of Pu-238 as fertile material to absorp neutrons for reducing excess reactivity and additional contribution for fuel breeding.« less

Transmutation of actinides in power reactors.

PubMed

Bergelson, B R; Gerasimov, A S; Tikhomirov, G V

2005-01-01

Power reactors can be used for partial short-term transmutation of radwaste. This transmutation is beneficial in terms of subsequent storage conditions for spent fuel in long-term storage facilities. CANDU-type reactors can transmute the main minor actinides from two or three reactors of the VVER-1000 type. A VVER-1000-type reactor can operate in a self-service mode with transmutation of its own actinides.

Georgia Institute of Technology research on the Gas Core Actinide Transmutation Reactor (GCATR)

NASA Technical Reports Server (NTRS)

Clement, J. D.; Rust, J. H.; Schneider, A.; Hohl, F.

1976-01-01

The program reviewed is a study of the feasibility, design, and optimization of the GCATR. The program is designed to take advantage of initial results and to continue work carried out on the Gas Core Breeder Reactor. The program complements NASA's program of developing UF6 fueled cavity reactors for power, nuclear pumped lasers, and other advanced technology applications. The program comprises: (1) General Studies--Parametric survey calculations performed to examine the effects of reactor spectrum and flux level on the actinide transmutation for GCATR conditions. The sensitivity of the results to neutron cross sections are to be assessed. Specifically, the parametric calculations of the actinide transmutation are to include the mass, isotope composition, fission and capture rates, reactivity effects, and neutron activity of recycled actinides. (2) GCATR Design Studies--This task is a major thrust of the proposed research program. Several subtasks are considered: optimization criteria studies of the blanket and fuel reprocessing, the actinide insertion and recirculation system, and the system integration. A brief review of the background of the GCATR and ongoing research is presented.

Complexation of lanthanides and actinides by acetohydroxamic acid

DOE Office of Scientific and Technical Information (OSTI.GOV)

Taylor, R.J.; Sinkov, S.I.; Choppin, G.R.

2008-07-01

Acetohydroxamic acid (AHA) has been proposed as a suitable reagent for the complexant-based, as opposed to reductive, stripping of plutonium and neptunium ions from the tributylphosphate solvent phase in advanced PUREX or UREX processes designed for future nuclear-fuel reprocessing. Stripping is achieved by the formation of strong hydrophilic complexes with the tetravalent actinides in nitric acid solutions. To underpin such applications, knowledge of the complexation constants of AHA with all relevant actinide (5f) and lanthanide (4f) ions is therefore important. This paper reports the determination of stability constants of AHA with the heavier lanthanide ions (Dy-Yb) and also U(IV) andmore » Th(IV) ions. Comparisons with our previously published AHA stability-constant data for 4f and 5f ions are made. (authors)« less

Updated and revised neutron reaction data for 237Np

NASA Astrophysics Data System (ADS)

Chen, Guochang; Wang, Jimin; Cao, Wentian; Tang, Guoyou; Yu, Baosheng

2017-09-01

Nuclear data with high accuracy for minor actinides play an important role in nuclear technology applications, including reactor design and operation, fuel cycle, estimation of the amount of minor actinides in high burn-up reactors and the minor actinides transmutation. Based on the evaluated experimental data, the updated and revised evaluation of a full set of n+237Np nuclear data from 10-5 eV ˜ 20 MeV are carried out and recommended. Mainly revised quantities are neutron multiplicities from fission reaction, inelastic, fission, (n, 2n) and (n, γ) reaction cross sections as well as angular distribution and so on. The promising results are obtained when the renewal evaluated data of 237Np will be used to instead of the evaluated data in CENDL-3.1 database.

Updated and revised neutron reaction data for 236,238Np

NASA Astrophysics Data System (ADS)

Chen, Guochang; Wang, Jimin; Cao, Wentian; Tang, Guoyou; Yu, Baosheng

2017-09-01

Nuclear data with high accuracy for minor actinides play an important role in nuclear technology applications, including reactor design and operation, fuel cycle, estimation of the amount of minor actinides in high burn-up reactors and the minor actinides transmutation. Based on a new set of neutron optical model parameter and the reaction cross section systematics of fissile isotopes, a full set of 236,238Np neutron reaction data from 10-5 eV ˜20 MeV are updated and improved through theoretical calculation. Mainly revised quantities include the total, elastic, inelastic, fission, (n, 2n) and (n, γ) reaction cross sections as well as angular distribution etc. The promising results are obtained when the renewal evaluated data of 236,238Np will replace the evaluated data in CENDL-3.1 database.

Controlling Hexavalent Americium – A Centerpiece to a Compact Nuclear Fuel Cycle

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shafer /Braley, Jenifer; Nash, Kenneth L; Lumetta, Gregg

2014-10-01

Closing the nuclear fuel cycle could be simplified by recovering the actinides U through Am as a group. This could be achieved by converting U, Np, Pu and Am to the hexavalent state. Uranium, Np and Pu are readily oxidized to the hexavalent state. Generation of hexavalent Am in acidic solutions is more difficult, as the standard reduction potential of the Am(VI) /Am(III) couple (+1.68 V in 1 M HClO4) is well outside of the electrochemical stability window of water. While the oxidation and separation of Am has been demonstrated under laboratory conditions, several issues could plague scale up andmore » implementation of this separation with used fuel. Two primary concerns are considered. The first issue concerns the stability of the oxidized Am. The second involves the undesirable co-extraction of tetravalent f-elements with the hexavalent actinides. To address the first concern regarding Am redox instability, Am reduction will be monitored under a variety of different conditions to establish the means of improving the stability of Am(VI) in the organic phase. Identifying the components contributing most significantly to its reduction will allow thoughtful modification of the process. To address the second concern, we propose to apply branched chain extractants to separate hexavalent actinides from tetravalent f-elements. Both branched monoamide and organophosphorus extractants have demonstrated significant selectivity for UO22+ versus Th4+, with separation factors generally on the order of 100. The efforts of this two-pronged research program should represent a significant step forward in the development of aqueous separations approaches designed to recover the U-Am actinides based on the availability of the hexavalent oxidation state. For the purposes of this proposal, separations based on this approach will be called SAn(VI) separations, indicating the Separation of An(VI).« less

On the Use of Thermal NF3 as the Fluorination and Oxidation Agent in Treatment of Used Nuclear Fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Scheele, Randall D.; McNamara, Bruce K.; Casella, Andrew M.

2012-05-01

This paper presents results of our investigation on the use of nitrogen trifluoride as the fluorination or fluorination/oxidation agent for use in a process for separating valuable constituents from used nuclear fuels by employing the volatility of many transition metal and actinide fluorides. Nitrogen trifluoride is less chemically and reactively hazardous than the hazardous and aggressive fluorinating agents used to prepare uranium hexafluoride and considered for fluoride volatility based nuclear fuels reprocessing. In addition, nitrogen trifluoride’s less aggressive character may be used to separate the volatile fluorides from used fuel and from themselves based on the fluorination reaction’s temperature sensitivitymore » (thermal tunability) rather than relying on differences in sublimation/boiling temperature and sorbents. Our thermodynamic calculations found that nitrogen trifluoride has the potential to produce volatile fission product and actinide fluorides from candidate oxides and metals. Our simultaneous thermogravimetric and differential thermal analyses found that the oxides of lanthanum, cerium, rhodium, and plutonium fluorinated but did not form volatile fluorides and that depending on temperature volatile fluorides formed from the oxides of niobium, molybdenum, ruthenium, tellurium, uranium, and neptunium. We also demonstrated near-quantitative removal of uranium from plutonium in a mixed oxide.« less

Overview of reductants utilized in nuclear fuel reprocessing/recycling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Patricia Paviet-Hartmann; Catherine Riddle; Keri Campbell

2013-10-01

Most of the aqueous processes developed, or under consideration worldwide for the recycling of used nuclear fuel (UNF) utilize the oxido-reduction properties of actinides to separate them from other radionuclides. Generally, after acid dissolution of the UNF, (essentially in nitric acid solution), actinides are separated from the raffinate by liquid-liquid extraction using specific solvents, associated along the process, with a particular reductant that will allow the separation to occur. For example, the industrial PUREX process utilizes hydroxylamine as a plutonium reductant. Hydroxylamine has numerous advantages: not only does it have the proper attributes to reduce Pu(IV) to Pu(III), but itmore » is also a non-metallic chemical that is readily decomposed to innocuous products by heating. However, it has been observed that the presence of high nitric acid concentrations or impurities (such as metal ions) in hydroxylamine solutions increase the likelihood of the initiation of an autocatalytic reaction. Recently there has been some interest in the application of simple hydrophilic hydroxamic ligands such as acetohydroxamic acid (AHA) for the stripping of tetravalent actinides in the UREX process flowsheet. This approach is based on the high coordinating ability of hydroxamic acids with tetravalent actinides (Np and Pu) compared with hexavalent uranium. Thus, the use of AHA offers a route for controlling neptunium and plutonium in the UREX process by complexant based stripping of Np(IV) and Pu(IV) from the TBP solvent phase, while U(VI) ions are not affected by AHA and remain solvated in the TBP phase. In the European GANEX process, AHA is also used to form hydrophilic complexes with actinides and strip them from the organic phase into nitric acid. However, AHA does not decompose completely when treated with nitric acid and hampers nitric acid recycling. In lieu of using AHA in the UREX + process, formohydroxamic acid (FHA), although not commercially available, hold promises as a replacement for AHA. FHA undergoes hydrolysis to formic acid which is volatile, thus allowing the recycling of nitric acid. Unfortunately, FHA powder was not stable in the experiments we ran in our laboratory. In addition, AHA and FHA also decompose to hydroxylamine which may undergo an autocatalytic reaction. Other reductants are available and could be extremely useful for actinides separation. The review presents the current plutonium reductants used in used nuclear fuel reprocessing and will introduce innovative and novel reductants that could become reducers for future research on UNF separation.« less

Thermal Stability of Acetohydroxamic Acid/Nitric Acid Solutions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudisill, T.S.

2002-03-13

The transmutation of transuranic actinides and long-lived fission products in spent commercial nuclear reactor fuel has been proposed as one element of the Advanced Accelerator Applications Program. Preparation of targets for irradiation in an accelerator-driven subcritical reactor would involve dissolution of the fuel and separation of uranium, technetium, and iodine from the transuranic actinides and other fission products. The UREX solvent extraction process is being developed to reject and isolate the transuranic actinides in the acid waste stream by scrubbing with acetohydroxamic acid (AHA). To ensure that a runaway reaction will not occur between nitric acid and AHA, an analoguemore » of hydroxyl amine, thermal stability tests were performed to identify if any processing conditions could lead to a runaway reaction.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lindley, Benjamin A.; Parks, Geoffrey T.; Franceschini, Fausto

Multiple recycle of long-lived actinides has the potential to greatly reduce the required storage time for spent nuclear fuel or high level nuclear waste. This is generally thought to require fast reactors as most transuranic (TRU) isotopes have low fission probabilities in thermal reactors. Reduced-moderation LWRs are a potential alternative to fast reactors with reduced time to deployment as they are based on commercially mature LWR technology. Thorium (Th) fuel is neutronically advantageous for TRU multiple recycle in LWRs due to a large improvement in the void coefficient. If Th fuel is used in reduced-moderation LWRs, it appears neutronically feasiblemore » to achieve full actinide recycle while burning an external supply of TRU, with related potential improvements in waste management and fuel utilization. In this paper, the fuel cycle of TRU-bearing Th fuel is analysed for reduced-moderation PWRs and BWRs (RMPWRs and RBWRs). RMPWRs have the advantage of relatively rapid implementation and intrinsically low conversion ratios. However, it is challenging to simultaneously satisfy operational and fuel cycle constraints. An RBWR may potentially take longer to implement than an RMPWR due to more extensive changes from current BWR technology. However, the harder neutron spectrum can lead to favourable fuel cycle performance. A two-stage fuel cycle, where the first pass is Th-Pu MOX, is a technically reasonable implementation of either concept. The first stage of the fuel cycle can therefore be implemented at relatively low cost as a Pu disposal option, with a further policy option of full recycle in the medium term. (authors)« less

Development of Metallic Fuels for Actinide Transmutation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hayes, Steven Lowe; Fielding, Randall Sidney; Benson, Michael Timothy

Research and development activities on metallic fuels are focused on their potential use for actinide transmutation in future sodium fast reactors. As part of this application, there is also a need for a near zero-loss fabrication process and a desire to demonstrate a multifold increase in burnup potential. The incorporation of Am and Np into the traditional U-20Pu-10Zr metallic fuel alloy was demonstrated in the US during the Integral Fast Reactor Program of the 1980’s and early 1990’s. However, the conventional counter gravity injection casting method performed under vacuum, previously used to fabricate these metallic fuel alloys, was not optimizedmore » for mitigating loss of the volatile Am constituent in the casting charge; as a result, approximately 40% of the Am casting charge failed to be incorporated into the as-cast fuel alloys. Fabrication development efforts of the past few years have pursued an optimized bottom-pour casting method to increase utilization of the melted charge to near 100%, and a differential pressure casting approach, performed under an argon overpressure, has been demonstrated to result in essentially no loss of Am due to volatilization during fabrication. In short, a path toward zero-loss fabrication of metallic fuels including minor actinides has been shown to be feasible. Irradiation testing of advanced metallic fuel alloys in the Advanced Test Reactor (ATR) has been underway since 2003. Testing in the ATR is performed inside of cadmium-shrouded positions to remove >99% of the thermal flux incident on the test fuels, resulting in an epi-thermal driven fuel test that is free from gross flux depression and producing an essentially prototypic radial temperature profile inside the fuel rodlets. To date, three irradiation test series (AFC-1,2,3) have been completed. Over 20 different metallic fuel alloys have been tested to burnups as high as 30% with constituent compositions of Pu up to 30%, Am up to 12%, Np up to 10%, and Zr between 10 and 60%. In general, the performance of all of these substantially disparate metallic fuel alloys has been observed to be excellent, and their irradiation behaviors are generally consistent with historic norms for metallic fuels without minor actinide additions and having lower Pu or Zr contents. Future work is being undertaken with a view toward increasing the burnup potential of metallic fuels even more. Design innovations under investigation include: 1) lowering the fuel smear density in order to accommodate more swelling, 2) annular fuel geometry to eliminate the need for a sodium bond, 3) minor alloy additions to stabilize lanthanide fission products inside the fuel and prevent their transport to the cladding where they can participate in fuel-cladding chemical interaction (FCCI), and 4) coatings/liners on the cladding inner surface to mitigate FCCI and enable higher temperature operation. This paper will present the current state of development of metallic fuels for actinide transmutation in the US. Highlights will include recent results from metallic fuel casting experiments, experiments to identify alloy additions to immobilize lanthanide fission products, and postirradiation examinations of annular metallic fuels at low burnup.« less

Complete recovery of actinides from UREX-like raffinates using a combination of hard and soft donor ligands. II. soft donor structure variation

DOE PAGES

Zalupski, Peter R.; Klaehn, John R.; Peterman, Dean R.

2015-07-30

The feasibility of simultaneous separation of uranium, neptunium, plutonium, americium, and curium from a simulated dissolved used fuel simulant adjusted to 1.0 M nitric acid is investigated using a mixture of the soft donor bis(bis-3,5-trifluoromethyl)phenyl) dithiophosphinic acid (“0”) and the hard donor synergist trioctylphosphine oxide (TOPO) dissolved in toluene. The results reported in this work are compared to our recent demonstration of a complete actinide recovery from a simulated dissolved fuel solution using a synergistic combination of bis(o-trifluoromethylphenyl)dithiophosphinic acid (“1”) and TOPO dissolved in either toluene or trifluoromethylphenyl sulfone. While the extraction efficiency of americium was enhanced for the liquid-liquidmore » system containing “0”, enabling to accomplish a trivalent An/Ln separation at 1.0 M HNO3, the extraction of neptunium was drastically diminished, relative to “1”. The partitioning behavior of curium was also negatively impacted, introducing an effective opportunity for americium/curium separation. Radiometric and spectrophotometric studies demonstrate that the complete actinide recovery using the solvent based upon “0” and TOPO is not feasible. Additionally, the importance of radiolytic degradation processes is discussed through the comparisons of extraction properties of liquid-liquid systems based on both soft donor reagents.« less

Sigma Team for Advanced Actinide Recycle FY2015 Accomplishments and Directions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moyer, Bruce A.

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 researchmore » 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 2O, 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.« less

Magnetic separation - Advanced nanotechnology for future nuclear fuel recycle

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kaur, M.; Zhang, H.; Qiang, Y.

2013-07-01

The unique properties of magnetic nanoparticles (MNPs), such as their extremely small size and high surface area to volume ratio, provide better kinetics for the adsorption of metal ions from aqueous solutions. In this work, we demonstrated the separation of minor actinides using complex conjugates of MNPs with diethylenetriamine-pentaacetic acid (DTPA) chelator. The sorption results show the strong affinity of DTPA towards Am (III) and Pu (IV) by extracting 97% and 80% of actinides, respectively. It is shown that the extraction process is highly dependent on the pH of the solution. If these long-term heat generating actinides can be efficientlymore » removed from the used fuel raffinates, the volume of material that can be placed in a given amount of repository space can be significantly increased. (authors)« less

PRELIMINARY DATA CALL REPORT ADVANCED BURNER REACTOR START UP FUEL FABRICATION FACILITY

DOE Office of Scientific and Technical Information (OSTI.GOV)

S. T. Khericha

2007-04-01

The purpose of this report is to provide data for preparation of a NEPA Environmental Impact Statement in support the U. S. Department of Energy (DOE) Global Nuclear Energy Partnership (GNEP). One of the GNEP objectives is to reduce the inventory of long lived actinide from the light water reactor (LWR) spent fuel. The LWR spent fuel contains Plutonium (Pu) -239 and other transuranics (TRU) such as Americium-241. One of the options is to transmute or burn these actinides in fast neutron spectra as well as generate the electricity. A sodium-cooled Advanced Recycling Reactor (ARR) concept has been proposed tomore » achieve this goal. However, fuel with relatively high TRU content has not been used in the fast reactor. To demonstrate the utilization of TRU fuel in a fast reactor, an Advanced Burner Reactor (ABR) prototype of ARR is proposed, which would necessarily be started up using weapons grade (WG) Pu fuel. The WG Pu is distinguished by relatively highest proportions of Pu-239 and lesser amount of other actinides. The WG Pu will be used as the startup fuel along with TRU fuel in lead test assemblies. Because such fuel is not currently being produced in the US, a new facility (or new capability in an existing facility) is being considered for fabrication of WG Pu fuel for the ABR. This report is provided in response to ‘Data Call’ for the construction of startup fuel fabrication facility. It is anticipated that the facility will provide the startup fuel for 10-15 years and will take to 3 to 5 years to construct.« less

A Blueprint for GNEP Advanced Burner Reactor Startup Fuel Fabrication Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

S. Khericha

2010-12-01

The purpose of this article is to identify the requirements and issues associated with design of GNEP Advanced Burner Reactor Fuel Facility. The report was prepared in support of providing data for preparation of a NEPA Environmental Impact Statement in support the U. S. Department of Energy (DOE) Global Nuclear Energy Partnership (GNEP). One of the GNEP objectives was to reduce the inventory of long lived actinide from the light water reactor (LWR) spent fuel. The LWR spent fuel contains Plutonium (Pu) -239 and other transuranics (TRU) such as Americium-241. One of the options is to transmute or burn thesemore » actinides in fast neutron spectra as well as generate the electricity. A sodium-cooled Advanced Recycling Reactor (ARR) concept was proposed to achieve this goal. However, fuel with relatively high TRU content has not been used in the fast reactor. To demonstrate the utilization of TRU fuel in a fast reactor, an Advanced Burner Reactor (ABR) prototype of ARR was proposed, which would necessarily be started up using weapons grade (WG) Pu fuel. The WG Pu is distinguished by relatively highest proportions of Pu-239 and lesser amount of other actinides. The WG Pu was assumed to be used as the startup fuel along with TRU fuel in lead test assemblies. Because such fuel is not currently being produced in the US, a new facility (or new capability in an existing facility) was being considered for fabrication of WG Pu fuel for the ABR. It was estimated that the facility will provide the startup fuel for 10-15 years and would take 3 to 5 years to construct.« less

Back-end of the fuel cycle - Indian scenario

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wattal, P.K.

Nuclear power has a key role in meeting the energy demands of India. This can be sustained by ensuring robust technology for the back end of the fuel cycle. Considering the modest indigenous resources of U and a huge Th reserve, India has adopted a three stage Nuclear Power Programme (NPP) based on 'closed fuel cycle' approach. This option on 'Recovery and Recycle' serves twin objectives of ensuring adequate supply of nuclear fuel and also reducing the long term radio-toxicity of the wastes. Reprocessing of the spent fuel by Purex process is currently employed. High Level Liquid Waste (HLW) generatedmore » during reprocessing is vitrified and undergoes interim storage. Back-end technologies are constantly modified to address waste volume minimization and radio-toxicity reduction. Long-term management of HLW in Indian context would involve partitioning of long lived minor actinides and recovery of valuable fission products specifically cesium. Recovery of minor actinides from HLW and its recycle is highly desirable for the sustained growth of India's NPPs. In this context, programme for developing and deploying partitioning technologies on industrial scale is pursued. The partitioned elements could be either transmuted in Fast Reactors (FRs)/Accelerated Driven Systems (ADS) as an integral part of sustainable Indian NPP. (authors)« less

Potential benefits of waste transmutation to the U.S. high-level waste respository

DOE Office of Scientific and Technical Information (OSTI.GOV)

Michaels, G.E.

1995-10-01

This paper reexamines the potential benefits of waste transmutation to the proposed U.S. geologic repository at the Yucca Mountain site based on recent progress in the performance assessment for the Yucca Mountain base case of spent fuel emplacement. It is observed that actinides are assumed to have higher solubility than in previous studies and that Np and other actinides now dominate the projected aqueous releases from a Yucca Mountain repository. Actinides are also indentified as the dominant source of decay heat in the repository, and the effect of decay heat in perturbing the hydrology, geochemistry, and thermal characteristics of Yuccamore » Mountain are reviewed. It is concluded that the potential for thermally-driven, buoyant, gas-phase flow at Yucca Mountain introduces data and modeling requirements that will increase the costs of licensing the site and may cause the site to be unattractive for geologic disposal of wastes. A transmutation-enabled cold repository is proposed that might allow licensing of a repository to be based upon currently observable characteristics of the Yucca Mountain site.« less

Nuclear fuels - Present and future

NASA Astrophysics Data System (ADS)

Olander, D.

2009-06-01

The important developments in nuclear fuels and their problems are reviewed and compared with the status of present light-water reactor fuels. The limitations of LWR fuels are reviewed with respect to important recent concerns, namely provision of outlet coolant temperatures high enough for use in H 2 production, destruction of plutonium to eliminate proliferation concerns, and burning of the minor actinides to reduce the waste repository heat load and long-term radiation hazard. In addition to current oxide-based fuel rod designs, the hydride fuel with liquid-metal thermal bonding of the fuel-cladding gap is covered. Finally, two of the most promising Generation IV reactor concepts, the very high temperature reactor and the sodium fast reactor, and the accompanying reprocessing technologies, aqueous-based UREX+1a and pyrometallurgical, are summarized. In all of the topics covered, the thermodynamics involved in the fuel's behavior under irradiation and in the reprocessing schemes are emphasized.

Trends in the short-term release of fission products and actinides to aqueous solution from used CANDU fuels at elevated temperature

NASA Astrophysics Data System (ADS)

Stroes-Gascoyne, S.

1992-08-01

A large number of short-term leaching experiments has been performed to determine fission product and actinide release from used CANDU (CANada Deuterium Uranium) fuels and to establish which factors affect release. Results are reported after30 ± 10 d leaching at 100-150°C under oxidizing (air) or reducing (Ar-3% H 2 or Ar) conditions, in various synthetic groundwaters. Cesium-137 release (0.007-6%) was positively correlated with increases in fuel power, leachant temperature and ionic strength. Strontium-90 release (0.0003-0.3%) generally increased with ionic strength, higher temperature and redox conditions. Actinide and Tc concentrations were compared to ranges calculated with a thermodynamic equilibrium model, that accounts for the uncertain geochemical parameters of a nuclear waste vault by calculating concentration ranges based on 40000 hypothetical cases. Experimental U concentrations (10 -8.5 to 10 -3 mol/kg) were higher than the model range, probably because of higher redox potentials in the experiments. Measured Pu concentrations (10 -12.5 to 10 -7 mol/kg) were at the low end of the calculated range. Americium and Cm concentrations (10 -12.5 to 10 -7 and 10 -15 to 10 -9 mol/kg, respectively) were highest under oxidizing conditions and higher temperatures. Technetium-99 concentrations (10 -5.5 to 10 -10.5 mol/kg) covered a much narrower range than calculated by the model.

Nuclear waste forms for actinides

PubMed Central

Ewing, Rodney C.

1999-01-01

The disposition of actinides, most recently 239Pu from dismantled nuclear weapons, requires effective containment of waste generated by the nuclear fuel cycle. Because actinides (e.g., 239Pu and 237Np) are long-lived, they have a major impact on risk assessments of geologic repositories. Thus, demonstrable, long-term chemical and mechanical durability are essential properties of waste forms for the immobilization of actinides. Mineralogic and geologic studies provide excellent candidate phases for immobilization and a unique database that cannot be duplicated by a purely materials science approach. The “mineralogic approach” is illustrated by a discussion of zircon as a phase for the immobilization of excess weapons plutonium. PMID:10097054

LIBS Spectral Data for a Mixed Actinide Fuel Pellet Containing Uranium, Plutonium, Neptunium and Americium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Judge, Elizabeth J.; Berg, John M.; Le, Loan A.

2012-06-18

Laser-induced breakdown spectroscopy (LIBS) was used to analyze a mixed actinide fuel pellet containing 75% UO{sub 2}/20% PuO{sub 2}/3% AmO{sub 2}/2% NpO{sub 2}. The preliminary data shown here is the first report of LIBS analysis of a mixed actinide fuel pellet, to the authors knowledge. The LIBS spectral data was acquired in a plutonium facility at Los Alamos National Laboratory where the sample was contained within a glove box. The initial installation of the glove box was not intended for complete ultraviolet (UV), visible (VIS) and near infrared (NIR) transmission, therefore the LIBS spectrum is truncated in the UV andmore » NIR regions due to the optical transmission of the window port and filters that were installed. The optical collection of the emission from the LIBS plasma will be optimized in the future. However, the preliminary LIBS data acquired is worth reporting due to the uniqueness of the sample and spectral data. The analysis of several actinides in the presence of each other is an important feature of this analysis since traditional methods must chemically separate uranium, plutonium, neptunium, and americium prior to analysis. Due to the historic nature of the sample fuel pellet analyzed, the provided sample composition of 75% UO{sub 2}/20% PuO{sub 2}/3% AmO{sub 2}/2% NpO{sub 2} cannot be confirm without further analytical processing. Uranium, plutonium, and americium emission lines were abundant and easily assigned while neptunium was more difficult to identify. There may be several reasons for this observation, other than knowing the exact sample composition of the fuel pellet. First, the atomic emission wavelength resources for neptunium are limited and such techniques as hollow cathode discharge lamp have different dynamics than the plasma used in LIBS which results in different emission spectra. Secondly, due to the complex sample of four actinide elements, which all have very dense electronic energy levels, there may be reactions and interactions occurring within the plasma, such as collisional energy transfer, that might be a factor in the reduction in neptunium emission lines. Neptunium has to be analyzed alone using LIBS to further understand the dynamics that may be occurring in the plasma of the mixed actinide fuel pellet sample. The LIBS data suggests that the emission spectrum for the mixed actinide fuel pellet is not simply the sum of the emission spectra of the pure samples but is dependent on the species present in the plasma and the interactions and reactions that occur within the plasma. Finally, many of the neptunium lines are in the near infrared region which is drastically reduced in intensity by the current optical setup and possibly the sensitivity of the emission detector in the spectral region. Once the optics are replaced and the optical collection system is modified and optimized, the probability of observing emission lines for neptunium might be increased significantly. The mixed actinide fuel pellet was analyzed under the experimental conditions listed in Table 1. The LIBS spectra of the fuel pellet are shown in Figures 1-49. The spectra are labeled with the observed wavelength and atomic species (both neutral (I) and ionic (II)). Table 2 is a complete list of the observed and literature based emission wavelengths. The literature wavelengths have references including NIST Atomic Spectra Database (NIST), B.A. Palmer et al. 'An Atlas of Uranium Emission Intensities in a Hollow Cathode Discharge' taken at the Kitt Peak National Observatory (KPNO), R.L. Kurucz 1995 Atomic Line Data from the Smithsonian Astrophysical Observatory (SAO), J. Blaise et al. 'The Atomic Spectrum of Plutonium' from Argonne National Laboratory (BFG), and M. Fred and F.S. Tomkins, 'Preliminary Term Analysis of Am I and Am II Spectra' (FT). The dash (-) shown under Ionic State indicates that the ionic state of the transition was not available. In the spectra, the dash (-) is replaced with a question mark (?). Peaks that are not assigned are most likely real features and not noise but cannot be confidently assigned to a transition without further investigation. Several peaks have multiple assignments due to limited resolution of the spectrometer used (20,000, {lambda}/{Delta}{lambda}) and without the availability, at this point in time, of pure PuO{sub 2}, AmO{sub 2}, and NpO{sub 2} to confirm the identity of the peaks. A different spectrometer was used in the plutonium facility to collect the mixed actinide fuel pellet data (Echelle 3000) than the DUO{sub 2}, ThO{sub 2} and uranium ore previously reported [6-8] (Echelle 4000) which accounts for the slight shift in the observed wavelength of the uranium emission lines.« less

Actinide management with commercial fast reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ohki, Shigeo

The capability of plutonium-breeding and minor-actinide (MA) transmutation in the Japanese commercial sodium-cooled fast reactor offers one of practical solutions for obtaining sustainable energy resources as well as reducing radioactive toxicity and inventory. The reference core design meets the requirement of flexible breeding ratio from 1.03 to 1.2. The MA transmutation amount has been evaluated as 50-100 kg/GW{sub e}y if the MA content in fresh fuel is 3-5 wt%, where about 30-40% of initial MA can be transmuted in the discharged fuel.

Ceramification: A plutonium immobilization process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rask, W.C.; Phillips, A.G.

1996-05-01

This paper describes a low temperature technique for stabilizing and immobilizing actinide compounds using a combination process/storage vessel of stainless steel, in which measured amounts of actinide nitrate solutions and actinide oxides (and/or residues) are systematically treated to yield a solid article. The chemical ceramic process is based on a coating technology that produces rare earth oxide coatings for defense applications involving plutonium. The final product of this application is a solid, coherent actinide oxide with process-generated encapsulation that has long-term environmental stability. Actinide compounds can be stabilized as pure materials for ease of re-use or as intimate mixtures withmore » additives such as rare earth oxides to increase their degree of proliferation resistance. Starting materials for the process can include nitrate solutions, powders, aggregates, sludges, incinerator ashes, and others. Agents such as cerium oxide or zirconium oxide may be added as powders or precursors to enhance the properties of the resulting solid product. Additives may be included to produce a final product suitable for use in nuclear fuel pellet production. The process is simple and reduces the time and expense for stabilizing plutonium compounds. It requires a very low equipment expenditure and can be readily implemented into existing gloveboxes. The process is easily conducted with less associated risk than proposed alternative technologies.« less

Minor Actinides-Loaded FBR Core Concept Suitable for the Introductory Period in Japan

NASA Astrophysics Data System (ADS)

Fujimura, Koji; Sasahira, Akira; Yamashita, Junichi; Fukasawa, Tetsuo; Hoshino, Kuniyoshi

According to the Japan's Framework for Nuclear Energy Policy(1), a basic scenario for fast breeder reactors (FBRs) is that they will be introduced on a commercial basis starting around 2050 replacing light water reactors (LWRs). During the FBR introduction period, the Pu from LWR spent fuel is used for FBR startup. Howerver, the FBR core loaded with this Pu has a larger burnup reactivity due to its larger isotopic content of Pu-241 than a core loaded with Pu from an FBR multi-recycling core. The increased burnup reactivity may reduce the cycle length of an FBR. We investigated, an FBR transitional core concept to confront the issues of the FBR introductory period in Japan. Core specifications are based on the compact-type sodium-cooled mixed oxide (MOX)-fueled core designed from the Japanese FBR cycle feasibility studies, because lower Pu inventory should be better for the FBR introductory period in view of its flexibility for the required reprocessing amount of LWR spent fuel to start up FBRs. The reference specifications were selected as follows. Output of 1500MWe and average discharge fuel burnup of about 150GWd/t. Minor Actinides (MAs) recovered from LWR spent fuels which provide Pu to startup FBRs are loaded to the initial loading fuels and exchanged fuels during few cycles until equilibrium. We made the MA content of the initial loading fuel four kinds like 0%, 3%, 4%, 5%. The average of the initial loading fuel is assumed to be 3%, and that of the exchange fuel is set as 5%. This 5% maximum of the MA content is based on the irradiation results of the experimental fast reactor Joyo. We evaluated the core performances including burnup characteristics and the reactivity coefficient and confirmed that transitional core from initial loading until equilibrium cycle with loaded Pu from LWR spent fuel performs similary to an FBR multi-recycling core.

Recovery of actinides from actinide-aluminium alloys by chlorination: Part III - Chlorination with HCl(g)

NASA Astrophysics Data System (ADS)

Meier, Roland; Souček, Pavel; Walter, Olaf; Malmbeck, Rikard; Rodrigues, Alcide; Glatz, Jean-Paul; Fanghänel, Thomas

2018-01-01

Two steps of a pyrochemical route for the recovery of actinides from spent metallic nuclear fuel are being investigated at JRC-Karlsruhe. The first step consists in electrorefining the fuel in molten salt medium implying aluminium cathodes. The second step is a chlorination process for the separation of actinides (An) from An-Al alloys formed on the cathodes. The chlorination process, in turn, consists of three steps; the distillation of adhered salt (1), the chlorination of An-Al by HCl/Cl2 under formation of AlCl3 and An chlorides (2), and the subsequent sublimation of AlCl3 (3). In the present work UAl2, UAl3, NpAl2, and PuAl2 were chlorinated with HCl(g) in a temperature range between 300 and 400 °C forming UCl4, NpCl4 or PuCl3 as the major An containing phases, respectively. Thermodynamic calculations were carried out to support the experimental work. The results showed a high chlorination efficiency for all used starting materials and indicated that the sublimation step may not be necessary when using HCl(g).

Benchmark Evaluation of Dounreay Prototype Fast Reactor Minor Actinide Depletion Measurements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hess, J. D.; Gauld, I. C.; Gulliford, J.

2017-01-01

Historic measurements of actinide samples in the Dounreay Prototype Fast Reactor (PFR) are of interest for modern nuclear data and simulation validation. Samples of various higher-actinide isotopes were irradiated for 492 effective full-power days and radiochemically assayed at Oak Ridge National Laboratory (ORNL) and Japan Atomic Energy Research Institute (JAERI). Limited data were available regarding the PFR irradiation; a six-group neutron spectra was available with some power history data to support a burnup depletion analysis validation study. Under the guidance of the Organisation for Economic Co-Operation and Development Nuclear Energy Agency (OECD NEA), the International Reactor Physics Experiment Evaluation Projectmore » (IRPhEP) and Spent Fuel Isotopic Composition (SFCOMPO) Project are collaborating to recover all measurement data pertaining to these measurements, including collaboration with the United Kingdom to obtain pertinent reactor physics design and operational history data. These activities will produce internationally peer-reviewed benchmark data to support validation of minor actinide cross section data and modern neutronic simulation of fast reactors with accompanying fuel cycle activities such as transportation, recycling, storage, and criticality safety.« less

Characterization of the Kinetics of NF3-Fluorination of NpO2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Casella, Andrew M.; Scheele, Randall D.; McNamara, Bruce K.

2015-12-23

The exploitation of selected actinide and fission product fluoride volatilities has long been considered as a potentially attractive compact method for recycling used nuclear fuels to avoid generating the large volumes of radioactive waste arising from aqueous reprocessing [1-7]. The most developed process uses the aggressive and hazardous fluorinating agents hydrogen fluoride (HF) and/or molecular fluorine (F2) at high temperatures to volatilize the greatest fraction of the used nuclear fuel into a single gas stream. The volatilized fluorides are subsequently separated using a series of fractionation and condensation columns to recover the valuable fuel constituents and fission products. In pursuitmore » of a safer and less complicated approach, we investigated an alternative fluoride volatility-based process using the less hazardous fluorinating agent nitrogen trifluoride (NF3) and leveraging its less aggressive nature to selectively evolve fission product and actinide fluorides from the solid phase based on their reaction temperatures into a single recycle stream [8-15]. In this approach, successive isothermal treatments using NF3 will first evolve the more thermally susceptible used nuclear fuel constituents leaving the other constituents in the residual solids until subsequent isothermal temperature treatments cause these others to volatilize. During investigation of this process, individual neat used fuel components were treated with isothermal NF3 in an attempt to characterize the kinetics of each fluorination reaction to provide input into the design of a new volatile fluoride separations approach. In these directed investigations, complex behavior was observed between NF3 and certain solid reactants such as the actinide oxides of uranium, plutonium, and neptunium. Given the similar thermal reaction susceptibilities of neptunium oxide (NpO2) and uranium dioxide (UO2) and the importance of Np and U, we initially focused our efforts on determining the reaction kinetic parameters for NpO2. Characterizing the NF3 fluorination of NpO2 using established models for gas-solid reactions [16] proved unsuccessful so we developed a series of successive fundamental reaction mechanisms to characterize the observed successive fluorination reactions leading to production of the volatile neptunium hexafluoride (NpF6).« less

Predicting thermo-mechanical behaviour of high minor actinide content composite oxide fuel in a dedicated transmutation facility

NASA Astrophysics Data System (ADS)

Lemehov, S. E.; Sobolev, V. P.; Verwerft, M.

2011-09-01

The European Facility for Industrial Transmutation (EFIT) of the minor actinides (MA), from LWR spent fuel is being developed in the integrated project EUROTRANS within the 6th Framework Program of EURATOM. Two composite uranium-free fuel systems, containing a large fraction of MA, are proposed as the main candidates: a CERCER with magnesia matrix hosting (Pu,MA)O 2-x particles, and a CERMET with metallic molybdenum matrix. The long-term thermal and mechanical behaviour of the fuel under the expected EFIT operating conditions is one of the critical issues in the core design. To make a reliable prediction of long-term thermo-mechanical behaviour of the hottest fuel rods in the lead-cooled version of EFIT with thermal power of 400 MW, different fuel performance codes have been used. This study describes the main results of modelling the thermo-mechanical behaviour of the hottest CERCER fuel rods with the fuel performance code MACROS which indicate that the CERCER fuel residence time can safely reach at least 4-5 effective full power years.

MSFR TRU-burning potential and comparison with an SFR

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fiorina, C.; Cammi, A.; Franceschini, F.

2013-07-01

The objective of this work is to evaluate the Molten Salt Fast Reactor (MSFR) potential benefits in terms of transuranics (TRU) burning through a comparative analysis with a sodium-cooled FR. The comparison is based on TRU- and MA-burning rates, as well as on the in-core evolution of radiotoxicity and decay heat. Solubility issues limit the TRU-burning rate to 1/3 that achievable in traditional low-CR FRs (low-Conversion-Ratio Fast Reactors). The softer spectrum also determines notable radiotoxicity and decay heat of the equilibrium actinide inventory. On the other hand, the liquid fuel suggests the possibility of using a Pu-free feed composed onlymore » of Th and MA (Minor Actinides), thus maximizing the MA burning rate. This is generally not possible in traditional low-CR FRs due to safety deterioration and decay heat of reprocessed fuel. In addition, the high specific power and the lack of out-of-core cooling times foster a quick transition toward equilibrium, which improves the MSFR capability to burn an initial fissile loading, and makes the MSFR a promising system for a quick (i.e., in a reactor lifetime) transition from the current U-based fuel cycle to a novel closed Th cycle. (authors)« less

Prognosis and comparison of performances of composite CERCER and CERMET fuels dedicated to transmutation of TRU in an EFIT ADS

NASA Astrophysics Data System (ADS)

Sobolev, V.; Uyttenhove, W.; Thetford, R.; Maschek, W.

2011-07-01

The neutronic and thermomechanical performances of two composite fuel systems: CERCER with (Pu,Np,Am,Cm)O 2-x fuel particles in ceramic MgO matrix and CERMET with metallic Mo matrix, selected for transmutation of minor actinides in the European Facility for Industrial Transmutation (EFIT), were analysed aiming at their optimisation. The ALEPH burnup code system, based on MNCPX and ORIGEN codes and JEFF3.1 nuclear data library, and the modern version of the fuel rod performance code TRAFIC were used for this analysis. Because experimental data on the properties of the mixed minor-actinide oxides are scarce, and the in-reactor behaviour of the T91 steel chosen as cladding, as well as of the corrosion protective layer, is still not well-known, a set of "best estimates" provided the properties used in the code. The obtained results indicate that both fuel candidates, CERCER and CERMET, can satisfy the fuel design and safety criteria of EFIT. The residence time for both types of fuel elements can reach about 5 years with the reactivity swing within ±1000 pcm, and about 22% of the loaded MA is transmuted during this period. However, the fuel centreline temperature in the hottest CERCER fuel rod is close to the temperature above which MgO matrix becomes chemically instable. Moreover, a weak PCMI can appear in about 3 years of operation. The CERMET fuel can provide larger safety margins: the fuel temperature is more than 1000 K below the permitted level of 2380 K and the pellet-cladding gap remains open until the end of operation.

Nuclear waste disposal—pyrochlore (A2B2O7): Nuclear waste form for the immobilization of plutonium and "minor" actinides

NASA Astrophysics Data System (ADS)

Ewing, Rodney C.; Weber, William J.; Lian, Jie

2004-06-01

During the past half-century, the nuclear fuel cycle has generated approximately 1400 metric tons of plutonium and substantial quantities of the "minor" actinides, such as Np, Am, and Cm. The successful disposition of these actinides has an important impact on the strategy for developing advanced nuclear fuel cycles, weapons proliferation, and the geologic disposal of high-level radioactive waste. During the last decade, there has been substantial interest in the use of the isometric pyrochlore structure-type, A2B2O7, for the immobilization of actinides. Most of the interest has focused on titanate-pyrochlore because of its chemical durability; however, these compositions experience a radiation-induced transition from the crystalline-to-aperiodic state due to radiation damage from the alpha-decay of actinides. Depending on the actinide concentration, the titanate pyrochlore will become amorphous in less than 1000 years of storage. Recently, systematic ion beam irradiations of a variety of pyrochlore compositions has revealed that many zirconate pyrochlores do not become amorphous, but remain crystalline as a defect fluorite structure-type due to disordering of the A- and B-site cations. The zirconate pyrochlores will remain crystalline even to very high doses, greater than 100 displacements per atom. Systematic experimental studies of actinide-doped and ion beam-irradiated pyrochlore, analyses of natural U- and Th-bearing pyrochlore, and simulations of the energetics of the disordering process now provide a rather detailed understanding of the structural and chemical controls on the response of pyrochlore to radiation. These results provide a solid basis for predicting the behavior and durability of pyrochlore used to immobilize plutonium.

Transmutation Scoping Studies for a Chloride Molten Salt Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heidet, Florent; Feng, Bo; Kim, Taek

2016-01-01

Over the past few years, there has been strong renewed interest from private industry, mostly from start-up enterprises, in molten salt reactor (MSR) technologies because of the unique properties of this class of reactors. These are reactors in which the fuel is homogeneously mixed with the coolant in the form of liquid salts and is circulated continuously into and out of the active core region with on-line fuel management, salt treatment, and salt processing. In response to such wide-spread interest, Argonne National Laboratory is expanding its well-established reactor modelling and simulation expertise and infrastructure to enable detailed analysis and designmore » of MSRs. The tools being developed are able to simulate the continuous fuel flow, the complex on-line fuel management and elemental removal processes (e.g., fission product removal) using depletion steps representative of a real MSR system. Leveraging these capabilities, a parametric study on the transmutation performance of a simplified actinide-burning MSR concept that uses a chloride-based salt was performed. This type of salt has attracted attention over the more commonly discussed fluoride-based salts since no tritium is produced as a result of irradiation and it is compatible with a fast neutron spectrum. The studies discussed in this paper examine the performance of a burner MSR design with a fixed core size and power density over a range of possible fuel salt molar ratios with NaCl-MgCl2 as the carrier salt. The intent is to quantify the impact on the required transuranics content of the make-up fuel, the actinide transmutation rates, and other performance characteristics for typical burner MSR designs.« less

New generation nuclear fuel structures: Dense particles in selectively soluble matrix

NASA Astrophysics Data System (ADS)

Devlin, Dave; Jarvinen, Gordon; Patterson, Brian; Pattillo, Steve; Valdez, James; Liu, X.-Y.; Phillips, Jonathan

2009-11-01

We have developed a technology for dispersing sub-millimeter sized fuel particles within a bulk matrix that can be selectively dissolved. This may enable the generation of advanced nuclear fuels with easy separation of actinides and fission products. The large kinetic energy of the fission products results in most of them escaping from the sub-millimeter sized fuel particles and depositing in the matrix during burning of the fuel in the reactor. After the fuel is used and allowed to cool for a period of time, the matrix can be dissolved and the fission products removed for disposal while the fuel particles are collected by filtration for recycle. The success of such an approach would meet a major goal of the GNEP program to provide advanced recycle technology for nuclear energy production. The benefits of such an approach include (1) greatly reduced cost of the actinide/fission product separation process, (2) ease of recycle of the fuel particles, and (3) a radiation barrier to prevent theft or diversion of the recycled fuel particles during the time they are re-fabricated into new fuel. In this study we describe a method to make surrogate nuclear fuels of micrometer scale W (shell)/Mo (core) or HfO 2 particles embedded in an MgO matrix that allows easy separation of the fission products and their embedded particles. In brief, the method consists of physically mixing W-Mo or hafnia particles with an MgO precursor. Heating the mixture, in air or argon, without agitation, to a temperature is required for complete decomposition of the precursor. The resulting material was examined using chemical analysis, scanning electron microscopy, X-ray diffraction and micro X-ray computed tomography and found to consist of evenly dispersed particles in an MgO + matrix. We believe this methodology can be extended to actinides and other matrix materials.

Salt transport extraction of transuranium elements from LWR fuel

DOEpatents

Pierce, R.D.; Ackerman, J.P.; Battles, J.E.; Johnson, T.R.; Miller, W.E.

1992-11-03

A process is described for separating transuranium actinide values from uranium values present in spent nuclear oxide fuels which contain rare earth and noble metal fission products. The oxide fuel is reduced with Ca metal in the presence of CaCl[sub 2] and a Cu--Mg alloy containing not less than about 25% by weight Mg at a temperature in the range of from about 750 C to about 850 C to precipitate uranium metal and some of the noble metal fission products leaving the Cu--Mg alloy having transuranium actinide metals and rare earth fission product metals and some of the noble metal fission products dissolved therein. The CaCl[sub 2] having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein is separated and electrolytically treated with a carbon electrode to reduce the CaO to Ca metal while converting the carbon electrode to CO and CO[sub 2]. The Ca metal and CaCl[sub 2] is recycled to reduce additional oxide fuel. The Cu--Mg alloy having transuranium metals and rare earth fission product metals and the noble metal fission products dissolved therein is contacted with a transport salt including MgCl[sub 2] to transfer Mg values from the transport salt to the Cu--Mg alloy while transuranium actinide and rare earth fission product metals transfer from the Cu--Mg alloy to the transport salt. Then the transport salt is mixed with a Mg--Zn alloy to transfer Mg values from the alloy to the transport salt while the transuranium actinide and rare earth fission product values dissolved in the salt are reduced and transferred to the Mg--Zn alloy. 2 figs.

Salt transport extraction of transuranium elements from lwr fuel

DOEpatents

Pierce, R. Dean; Ackerman, John P.; Battles, James E.; Johnson, Terry R.; Miller, William E.

1992-01-01

A process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels which contain rare earth and noble metal fission products. The oxide fuel is reduced with Ca metal in the presence of CaCl.sub.2 and a Cu--Mg alloy containing not less than about 25% by weight Mg at a temperature in the range of from about 750.degree. C. to about 850.degree. C. to precipitate uranium metal and some of the noble metal fission products leaving the Cu--Mg alloy having transuranium actinide metals and rare earth fission product metals and some of the noble metal fission products dissolved therein. The CaCl.sub.2 having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein is separated and electrolytically treated with a carbon electrode to reduce the CaO to Ca metal while converting the carbon electrode to CO and CO.sub.2. The Ca metal and CaCl.sub.2 is recycled to reduce additional oxide fuel. The Cu--Mg alloy having transuranium metals and rare earth fission product metals and the noble metal fission products dissolved therein is contacted with a transport salt including Mg Cl.sub.2 to transfer Mg values from the transport salt to the Cu--Mg alloy while transuranium actinide and rare earth fission product metals transfer from the Cu--Mg alloy to the transport salt. Then the transport salt is mixed with a Mg--Zn alloy to transfer Mg values from the alloy to the transport salt while the transuranium actinide and rare earth fission product values dissolved in the salt are reduced and transferred to the Mg--Zn alloy.

An Approach for Validating Actinide and Fission Product Burnup Credit Criticality Safety Analyses: Criticality (k eff) Predictions

DOE PAGES

Scaglione, John M.; Mueller, Don E.; Wagner, John C.

2014-12-01

One of the most important remaining challenges associated with expanded implementation of burnup credit in the United States is the validation of depletion and criticality calculations used in the safety evaluation—in particular, the availability and use of applicable measured data to support validation, especially for fission products (FPs). Applicants and regulatory reviewers have been constrained by both a scarcity of data and a lack of clear technical basis or approach for use of the data. In this study, this paper describes a validation approach for commercial spent nuclear fuel (SNF) criticality safety (k eff) evaluations based on best-available data andmore » methods and applies the approach for representative SNF storage and transport configurations/conditions to demonstrate its usage and applicability, as well as to provide reference bias results. The criticality validation approach utilizes not only available laboratory critical experiment (LCE) data from the International Handbook of Evaluated Criticality Safety Benchmark Experiments and the French Haut Taux de Combustion program to support validation of the principal actinides but also calculated sensitivities, nuclear data uncertainties, and limited available FP LCE data to predict and verify individual biases for relevant minor actinides and FPs. The results demonstrate that (a) sufficient critical experiment data exist to adequately validate k eff calculations via conventional validation approaches for the primary actinides, (b) sensitivity-based critical experiment selection is more appropriate for generating accurate application model bias and uncertainty, and (c) calculated sensitivities and nuclear data uncertainties can be used for generating conservative estimates of bias for minor actinides and FPs. Results based on the SCALE 6.1 and the ENDF/B-VII.0 cross-section libraries indicate that a conservative estimate of the bias for the minor actinides and FPs is 1.5% of their worth within the application model. Finally, this paper provides a detailed description of the approach and its technical bases, describes the application of the approach for representative pressurized water reactor and boiling water reactor safety analysis models, and provides reference bias results based on the prerelease SCALE 6.1 code package and ENDF/B-VII nuclear cross-section data.« less

Modeling and Analysis of Actinide Diffusion Behavior in Irradiated Metal Fuel

NASA Astrophysics Data System (ADS)

Edelmann, Paul G.

There have been numerous attempts to model fast reactor fuel behavior in the last 40 years. The US currently does not have a fully reliable tool to simulate the behavior of metal fuels in fast reactors. The experimental database necessary to validate the codes is also very limited. The DOE-sponsored Advanced Fuels Campaign (AFC) has performed various experiments that are ready for analysis. Current metal fuel performance codes are either not available to the AFC or have limitations and deficiencies in predicting AFC fuel performance. A modified version of a new fuel performance code, FEAST-Metal , was employed in this investigation with useful results. This work explores the modeling and analysis of AFC metallic fuels using FEAST-Metal, particularly in the area of constituent actinide diffusion behavior. The FEAST-Metal code calculations for this work were conducted at Los Alamos National Laboratory (LANL) in support of on-going activities related to sensitivity analysis of fuel performance codes. A sensitivity analysis of FEAST-Metal was completed to identify important macroscopic parameters of interest to modeling and simulation of metallic fuel performance. A modification was made to the FEAST-Metal constituent redistribution model to enable accommodation of newer AFC metal fuel compositions with verified results. Applicability of this modified model for sodium fast reactor metal fuel design is demonstrated.

Criticality safety strategy and analysis summary for the fuel cycle facility electrorefiner at Argonne National Laboratory West

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mariani, R.D.; Benedict, R.W.; Lell, R.M.

1996-05-01

As part of the termination activities of Experimental Breeder Reactor II (EBR-II) at Argonne National Laboratory (ANL) West, the spent metallic fuel from EBR-II will be treated in the fuel cycle facility (FCF). A key component of the spent-fuel treatment process in the FCF is the electrorefiner (ER) in which the actinide metals are separated from the active metal fission products and the reactive bond sodium. In the electrorefining process, the metal fuel is anodically dissolved into a high-temperature molten salt, and refined uranium or uranium/plutonium products are deposited at cathodes. The criticality safety strategy and analysis for the ANLmore » West FCF ER is summarized. The FCF ER operations and processes formed the basis for evaluating criticality safety and control during actinide metal fuel refining. To show criticality safety for the FCF ER, the reference operating conditions for the ER had to be defined. Normal operating envelopes (NOEs) were then defined to bracket the important operating conditions. To keep the operating conditions within their NOEs, process controls were identified that can be used to regulate the actinide forms and content within the ER. A series of operational checks were developed for each operation that will verify the extent or success of an operation. The criticality analysis considered the ER operating conditions at their NOE values as the point of departure for credible and incredible failure modes. As a result of the analysis, FCF ER operations were found to be safe with respect to criticality.« less

Impact investigation of reactor fuel operating parameters on reactivity for use in burnup credit applications

NASA Astrophysics Data System (ADS)

Sloma, Tanya Noel

When representing the behavior of commercial spent nuclear fuel (SNF), credit is sought for the reduced reactivity associated with the net depletion of fissile isotopes and the creation of neutron-absorbing isotopes, a process that begins when a commercial nuclear reactor is first operated at power. Burnup credit accounts for the reduced reactivity potential of a fuel assembly and varies with the fuel burnup, cooling time, and the initial enrichment of fissile material in the fuel. With regard to long-term SNF disposal and transportation, tremendous benefits, such as increased capacity, flexibility of design and system operations, and reduced overall costs, provide an incentive to seek burnup credit for criticality safety evaluations. The Nuclear Regulatory Commission issued Interim Staff Guidance 8, Revision 2 in 2002, endorsing burnup credit of actinide composition changes only; credit due to actinides encompasses approximately 30% of exiting pressurized water reactor SNF inventory and could potentially be increased to 90% if fission product credit were accepted. However, one significant issue for utilizing full burnup credit, compensating for actinide and fission product composition changes, is establishing a set of depletion parameters that produce an adequately conservative representation of the fuel's isotopic inventory. Depletion parameters can have a significant effect on the isotopic inventory of the fuel, and thus the residual reactivity. This research seeks to quantify the reactivity impact on a system from dominant depletion parameters (i.e., fuel temperature, moderator density, burnable poison rod, burnable poison rod history, and soluble boron concentration). Bounding depletion parameters were developed by statistical evaluation of a database containing reactor operating histories. The database was generated from summary reports of commercial reactor criticality data. Through depletion calculations, utilizing the SCALE 6 code package, several light water reactor assembly designs and in-core locations are analyzed in establishing a combination of depletion parameters that conservatively represent the fuel's isotopic inventory as an initiative to take credit for fuel burnup in criticality safety evaluations for transportation and storage of SNF.

Hardening neutron spectrum for advanced actinide transmutation experiments in the ATR.

PubMed

Chang, G S; Ambrosek, R G

2005-01-01

The most effective method for transmuting long-lived isotopes contained in spent nuclear fuel into shorter-lived fission products is in a fast neutron spectrum reactor. In the absence of a fast test reactor in the United States, initial irradiation testing of candidate fuels can be performed in a thermal test reactor that has been modified to produce a test region with a hardened neutron spectrum. Such a test facility, with a spectrum similar but somewhat softer than that of the liquid-metal fast breeder reactor (LMFBR), has been constructed in the INEEL's Advanced Test Reactor (ATR). The radial fission power distribution of the actinide fuel pin, which is an important parameter in fission gas release modelling, needs to be accurately predicted and the hardened neutron spectrum in the ATR and the LMFBR fast neutron spectrum is compared. The comparison analyses in this study are performed using MCWO, a well-developed tool that couples the Monte Carlo transport code MCNP with the isotope depletion and build-up code ORIGEN-2. MCWO analysis yields time-dependent and neutron-spectrum-dependent minor actinide and Pu concentrations and detailed radial fission power profile calculations for a typical fast reactor (LMFBR) neutron spectrum and the hardened neutron spectrum test region in the ATR. The MCWO-calculated results indicate that the cadmium basket used in the advanced fuel test assembly in the ATR can effectively depress the linear heat generation rate in the experimental fuels and harden the neutron spectrum in the test region.

Criticality safety strategy for the Fuel Cycle Facility electrorefiner at Argonne National Laboratory, West

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mariani, R.D.; Benedict, R.W.; Lell, R.M.

1993-09-01

The Integral Fast Reactor being developed by Argonne National Laboratory (ANL) combines the advantages of metal-fueled, liquid-metal-cooled reactors and a closed fuel cycle. Presently, the Fuel Cycle Facility (FCF) at ANL-West in Idaho Falls, Idaho is being modified to recycle spent metallic fuel from Experimental Breeder Reactor II as part of a demonstration project sponsored by the Department of Energy. A key component of the FCF is the electrorefiner (ER) in which the actinides are separated from the fission products. In the electrorefining process, the metal fuel is anodically dissolved into a high-temperature molten salt and refined uranium or uranium/plutoniummore » products are deposited at cathodes. In this report, the criticality safety strategy for the FCF ER is summarized. FCF ER operations and processes formed the basis for evaluating criticality safety and control during actinide metal fuel refining. In order to show criticality safety for the FCF ER, the reference operating conditions for the ER had to be defined. Normal operating envelopes (NOES) were then defined to bracket the important operating conditions. To keep the operating conditions within their NOES, process controls were identified that can be used to regulate the actinide forms and content within the ER. A series of operational checks were developed for each operation that wig verify the extent or success of an operation. The criticality analysis considered the ER operating conditions at their NOE values as the point of departure for credible and incredible failure modes. As a result of the analysis, FCF ER operations were found to be safe with respect to criticality.« less

LIFE Materials: Overview of Fuels and Structural Materials Issues Volume 1

DOE Office of Scientific and Technical Information (OSTI.GOV)

Farmer, J

2008-09-08

The National Ignition Facility (NIF) project, a laser-based Inertial Confinement Fusion (ICF) experiment designed to achieve thermonuclear fusion ignition and burn in the laboratory, is under construction at the Lawrence Livermore National Laboratory (LLNL) and will be completed in April of 2009. Experiments designed to accomplish the NIF's goal will commence in late FY2010 utilizing laser energies of 1 to 1.3 MJ. Fusion yields of the order of 10 to 20 MJ are expected soon thereafter. Laser initiated fusion-fission (LIFE) engines have now been designed to produce nuclear power from natural or depleted uranium without isotopic enrichment, and from spentmore » nuclear fuel from light water reactors without chemical separation into weapons-attractive actinide streams. A point-source of high-energy neutrons produced by laser-generated, thermonuclear fusion within a target is used to achieve ultra-deep burn-up of the fertile or fissile fuel in a sub-critical fission blanket. Fertile fuels including depleted uranium (DU), natural uranium (NatU), spent nuclear fuel (SNF), and thorium (Th) can be used. Fissile fuels such as low-enrichment uranium (LEU), excess weapons plutonium (WG-Pu), and excess highly-enriched uranium (HEU) may be used as well. Based upon preliminary analyses, it is believed that LIFE could help meet worldwide electricity needs in a safe and sustainable manner, while drastically shrinking the nation's and world's stockpile of spent nuclear fuel and excess weapons materials. LIFE takes advantage of the significant advances in laser-based inertial confinement fusion that are taking place at the NIF at LLNL where it is expected that thermonuclear ignition will be achieved in the 2010-2011 timeframe. Starting from as little as 300 to 500 MW of fusion power, a single LIFE engine will be able to generate 2000 to 3000 MWt in steady state for periods of years to decades, depending on the nuclear fuel and engine configuration. Because the fission blanket in a fusion-fission hybrid system is subcritical, a LIFE engine can burn any fertile or fissile nuclear material, including un-enriched natural or depleted U and SNF, and can extract a very high percentage of the energy content of its fuel resulting in greatly enhanced energy generation per metric ton of nuclear fuel, as well as nuclear waste forms with vastly reduced concentrations of long-lived actinides. LIFE engines could thus provide the ability to generate vast amounts of electricity while greatly reducing the actinide content of any existing or future nuclear waste and extending the availability of low cost nuclear fuels for several thousand years. LIFE also provides an attractive pathway for burning excess weapons Pu to over 99% FIMA (fission of initial metal atoms) without the need for fabricating or reprocessing mixed oxide fuels (MOX). Because of all of these advantages, LIFE engines offer a pathway toward sustainable and safe nuclear power that significantly mitigates nuclear proliferation concerns and minimizes nuclear waste. An important aspect of a LIFE engine is the fact that there is no need to extract the fission fuel from the fission blanket before it is burned to the desired final level. Except for fuel inspection and maintenance process times, the nuclear fuel is always within the core of the reactor and no weapons-attractive materials are available outside at any point in time. However, an important consideration when discussing proliferation concerns associated with any nuclear fuel cycle is the ease with which reactor fuel can be converted to weapons usable materials, not just when it is extracted as waste, but at any point in the fuel cycle. Although the nuclear fuel remains in the core of the engine until ultra deep actinide burn up is achieved, soon after start up of the engine, once the system breeds up to full power, several tons of fissile material is present in the fission blanket. However, this fissile material is widely dispersed in millions of fuel pebbles, which can be tagged as individual accountable items, and thus made difficult to divert in large quantities. Several topical reports are being prepared on the materials and processes required for the LIFE engine. Specific materials of interest include: (1) Baseline TRISO Fuel (TRISO); (2) Inert Matrix Fuel (IMF) & Other Alternative Solid Fuels; (3) Beryllium (Be) & Molten Lead Blankets (Pb/PbLi); (4) Molten Salt Coolants (FLIBE/FLiNaBe/FLiNaK); (5) Molten Salt Fuels (UF4 + FLIBE/FLiNaBe); (6) Cladding Materials for Fuel & Beryllium; (7) ODS FM Steel (ODS); (8) Solid First Wall (SFW); and (9) Solid-State Tritium Storage (Hydrides).« less

Analysis of Advanced Fuel Assemblies and Core Designs for the Current and Next Generations of LWRs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ragusa, Jean; Vierow, Karen

2011-09-01

The objective of the project is to design and analyze advanced fuel assemblies for use in current and future light water reactors and to assess their ability to reduce the inventory of transuranic elements, while preserving operational safety. The reprocessing of spent nuclear fuel can delay or avoid the need for a second geological repository in the US. Current light water reactor fuel assembly designs under investigation could reduce the plutonium inventory of reprocessed fuel. Nevertheless, these designs are not effective in stabilizing or reducing the inventory of minor actinides. In the course of this project, we developed and analyzedmore » advanced fuel assembly designs with improved thermal transmutation capability regarding transuranic elements and especially minor actinides. These designs will be intended for use in thermal spectrum (e.g., current and future fleet of light water reactors in the US). We investigated various fuel types, namely high burn-up advanced mixed oxides and inert matrix fuels, in various geometrical designs that are compliant with the core internals of current and future light water reactors. Neutronic/thermal hydraulic effects were included. Transmutation efficiency and safety parameters were used to rank and down-select the various designs.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zalupski, Peter R.; Klaehn, John R.; Peterman, Dean R.

The feasibility of simultaneous separation of uranium, neptunium, plutonium, americium, and curium from a simulated dissolved used fuel simulant adjusted to 1.0 M nitric acid is investigated using a mixture of the soft donor bis(bis-3,5-trifluoromethyl)phenyl) dithiophosphinic acid (“0”) and the hard donor synergist trioctylphosphine oxide (TOPO) dissolved in toluene. The results reported in this work are compared to our recent demonstration of a complete actinide recovery from a simulated dissolved fuel solution using a synergistic combination of bis(o-trifluoromethylphenyl)dithiophosphinic acid (“1”) and TOPO dissolved in either toluene or trifluoromethylphenyl sulfone. While the extraction efficiency of americium was enhanced for the liquid-liquidmore » system containing “0”, enabling to accomplish a trivalent An/Ln separation at 1.0 M HNO3, the extraction of neptunium was drastically diminished, relative to “1”. The partitioning behavior of curium was also negatively impacted, introducing an effective opportunity for americium/curium separation. Radiometric and spectrophotometric studies demonstrate that the complete actinide recovery using the solvent based upon “0” and TOPO is not feasible. Additionally, the importance of radiolytic degradation processes is discussed through the comparisons of extraction properties of liquid-liquid systems based on both soft donor reagents.« less

Uranium chloride extraction of transuranium elements from LWR fuel

DOEpatents

Miller, W.E.; Ackerman, J.P.; Battles, J.E.; Johnson, T.R.; Pierce, R.D.

1992-08-25

A process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels containing rare earth and noble metal fission products as well as other fission products is disclosed. The oxide fuel is reduced with Ca metal in the presence of Ca chloride and a U-Fe alloy which is liquid at about 800 C to dissolve uranium metal and the noble metal fission product metals and transuranium actinide metals and rare earth fission product metals leaving Ca chloride having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein. The Ca chloride and CaO and the fission products contained therein are separated from the U-Fe alloy and the metal values dissolved therein. The U-Fe alloy having dissolved therein reduced metals from the spent nuclear fuel is contacted with a mixture of one or more alkali metal or alkaline earth metal halides selected from the class consisting of alkali metal or alkaline earth metal and Fe or U halide or a combination thereof to transfer transuranium actinide metals and rare earth metals to the halide salt leaving the uranium and some noble metal fission products in the U-Fe alloy and thereafter separating the halide salt and the transuranium metals dissolved therein from the U-Fe alloy and the metals dissolved therein. 1 figure.

Uranium chloride extraction of transuranium elements from LWR fuel

DOEpatents

Miller, William E.; Ackerman, John P.; Battles, James E.; Johnson, Terry R.; Pierce, R. Dean

1992-01-01

A process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels containing rare earth and noble metal fission products as well as other fission products is disclosed. The oxide fuel is reduced with Ca metal in the presence of Ca chloride and a U-Fe alloy which is liquid at about 800.degree. C. to dissolve uranium metal and the noble metal fission product metals and transuranium actinide metals and rare earth fission product metals leaving Ca chloride having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein. The Ca chloride and CaO and the fission products contained therein are separated from the U-Fe alloy and the metal values dissolved therein. The U-Fe alloy having dissolved therein reduced metals from the spent nuclear fuel is contacted with a mixture of one or more alkali metal or alkaline earth metal halides selected from the class consisting of alkali metal or alkaline earth metal and Fe or U halide or a combination thereof to transfer transuranium actinide metals and rare earth metals to the halide salt leaving the uranium and some noble metal fission products in the U-Fe alloy and thereafter separating the halide salt and the transuranium metals dissolved therein from the U-Fe alloy and the metals dissolved therein.

Analysis and optimization of minor actinides transmutation blankets with regards to neutron and gamma sources

NASA Astrophysics Data System (ADS)

Kooymana, Timothée; Buiron, Laurent; Rimpault, Gérald

2017-09-01

Heterogeneous loading of minor actinides in radial blankets is a potential solution to implement minor actinides transmutation in fast reactors. However, to compensate for the lower flux level experienced by the blankets, the fraction of minor actinides to be loaded in the blankets must be increased to maintain acceptable performances. This severely increases the decay heat and neutron source of the blanket assemblies, both before and after irradiation, by more than an order of magnitude in the case of neutron source for instance. We propose here to implement an optimization methodology of the blankets design with regards to various parameters such as the local spectrum or the mass to be loaded, with the objective of minimizing the final neutron source of the spent assembly while maximizing the transmutation performances of the blankets. In a first stage, an analysis of the various contributors to long and short term neutron and gamma source is carried out while in a second stage, relevant estimators are designed for use in the effective optimization process, which is done in the last step. A comparison with core calculations is finally done for completeness and validation purposes. It is found that the use of a moderated spectrum in the blankets can be beneficial in terms of final neutron and gamma source without impacting minor actinides transmutation performances compared to more energetic spectrum that could be achieved using metallic fuel for instance. It is also confirmed that, if possible, the use of hydrides as moderating material in the blankets is a promising option to limit the total minor actinides inventory in the fuel cycle. If not, it appears that focus should be put upon an increased residence time for the blankets rather than an increase in the acceptable neutron source for handling and reprocessing.

On the use of thermal NF3 as the fluorination and oxidation agent in treatment of used nuclear fuels

NASA Astrophysics Data System (ADS)

Scheele, Randall; McNamara, Bruce; Casella, Andrew M.; Kozelisky, Anne

2012-05-01

This paper presents results of our investigation on the use of nitrogen trifluoride as a fluorination or fluorination/oxidation agent for separating valuable constituents from used nuclear fuels by exploiting the different volatilities of the constituent fission product and actinide fluorides. Our thermodynamic calculations show that nitrogen trifluoride has the potential to produce volatile fission product and actinide fluorides from oxides and metals that can form volatile fluorides. Simultaneous thermogravimetric and differential thermal analyses show that the oxides of lanthanum, cerium, rhodium, and plutonium are fluorinated but do not form volatile fluorides when treated with nitrogen trifluoride at temperatures up to 550 °C. However, depending on temperature, volatile fluorides or oxyfluorides can form from nitrogen trifluoride treatment of the oxides of niobium, molybdenum, ruthenium, tellurium, uranium, and neptunium. Thermoanalytical studies demonstrate near-quantitative separation of uranium from plutonium in a mixed 80% uranium and 20% plutonium oxide. Our studies of neat oxides and metals suggest that the reactivity of nitrogen trifluoride may be adjusted by temperature to selectively separate the major volatile fuel constituent uranium from minor volatile constituents, such as Mo, Tc, Ru and from the non-volatile fuel constituents based on differences in their reaction temperatures and kinetic behaviors. This reactivity is novel with respect to that reported for other fluorinating reagents F2, BrF5, ClF3.

Applications in Nuclear Energy Security

NASA Astrophysics Data System (ADS)

Sheffield, Richard

2009-05-01

A key roadblock to development of additional nuclear power capacity is a concern over management of nuclear waste. Nuclear waste is predominantly comprised of used fuel discharged from operating nuclear reactors. The roughly 100 operating US reactors currently produce about 20% of the US electricity and will create about 87,000 tons of such discharged or ``spent'' fuel over the course of their lifetimes. The long-term radioactivity of the spent fuel drives the need for deep geologic storage that remains stable for millions of years. Nearly all issues related to risks to future generations arising from long-term disposal of such spent nuclear fuel is attributable to approximately the 1% made up primarily of minor actinides. If we can reduce or eliminate this 1% of the spent fuel, then within a few hundred years the toxic nature of the spent fuel drops below that of the natural uranium ore that was originally mined for nuclear fuel. The minor actinides can be efficiently eliminated through nuclear transmutation using as a driver fast-neutrons produced by a spallation process initiated with a high-energy proton beam. This presentation will cover the system design considerations and issues of an accelerator driven transmutation system.

Cryogenic gamma detectors enable direct detection of 236U and minor actinides for non-destructive assay [Cryogenic gamma detectors enable direct detection of minor actinides for non-destructive assay

DOE Office of Scientific and Technical Information (OSTI.GOV)

Velazquez, Miguel; Dreyer, Jonathan; Drury, Owen B.

2015-09-05

Here, we demonstrate the utility of a superconducting transition edge sensor (TES) γ-ray detector with high energy resolution and low Compton background for non-destructive assay (NDA) of a uranium sample from reprocessed nuclear fuel. We show that TES γ-detectors can separate low energy actinide γ-emissions from the background and nearby lines, even from minor isotopes whose signals are often obscured in NDA with conventional Ge detectors. Superconducting γ detectors may therefore bridge the gap between high-accuracy destructive assay (DA) and easier to-use NDA.

REGENERATION OF REACTOR FUEL ELEMENTS

DOEpatents

Roake, W.E.; Lyon, W.L.

1960-03-29

A process of concentrating by electrolysis the uraatum and/or plutonium of an aluminum alloy containing these actinides after the actinide has been partially consumed by neutron bombardment in a reactor is given. The alloy is made the anode in a system having an aluminum cathode and a cryolite electrolyte. Electrolysis from 22 to 28 ampere-hours removes a sufficient quantity of aluminum from the alloy to make it suitable for reuse.

The Efficacy of Denaturing Actinide Elements as a Means of Decreasing Materials Attractiveness

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hase, Kevin R.; Ebbinghaus, Bartley B.; Sleaford, Brad W.

2013-07-01

This paper is an extension to earlier studies that examined the attractiveness of materials mixtures containing special nuclear materials (SNM) and alternate nuclear materials (ANM). This study considers the concept of denaturing as applied to the actinide elements present in spent fuel as a means to reduce materials attractiveness. Highly attractive materials generally have low values of bare critical mass, heat content, and dose.

Conjugates of magnetic nanoparticle-actinide specific chelator for radioactive waste separation.

PubMed

Kaur, Maninder; Zhang, Huijin; Martin, Leigh; Todd, Terry; Qiang, You

2013-01-01

A novel nanotechnology for the separation of radioactive waste that uses magnetic nanoparticles (MNPs) conjugated with actinide specific chelators (MNP-Che) is reviewed with a focus on design and process development. The MNP-Che separation process is an effective way of separating heat generating minor actinides (Np, Am, Cm) from spent nuclear fuel solution to reduce the radiological hazard. It utilizes coated MNPs to selectively adsorb the contaminants onto their surfaces, after which the loaded particles are collected using a magnetic field. The MNP-Che conjugates can be recycled by stripping contaminates into a separate, smaller volume of solution, and then become the final waste form for disposal after reusing number of times. Due to the highly selective chelators, this remediation method could be both simple and versatile while allowing the valuable actinides to be recovered and recycled. Key issues standing in the way of large-scale application are stability of the conjugates and their dispersion in solution to maintain their unique properties, especially large surface area, of MNPs. With substantial research progress made on MNPs and their surface functionalization, as well as development of environmentally benign chelators, this method could become very flexible and cost-effective for recycling used fuel. Finally, the development of this nanotechnology is summarized and its future direction is discussed.

Comparison of actinide production in traveling wave and pressurized water reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Osborne, A.G.; Smith, T.A.; Deinert, M.R.

The geopolitical problems associated with civilian nuclear energy production arise in part from the accumulation of transuranics in spent nuclear fuel. A traveling wave reactor is a type of breed-burn reactor that could, if feasible, reduce the overall production of transuranics. In one possible configuration, a cylinder of natural or depleted uranium would be subjected to a fast neutron flux at one end. The neutrons would transmute the uranium, producing plutonium and higher actinides. Under the right conditions, the reactor could become critical, at which point a self-stabilizing fission wave would form and propagate down the length of the reactormore » cylinder. The neutrons from the fission wave would burn the fissile nuclides and transmute uranium ahead of the wave to produce additional fuel. Fission waves in uranium are driven largely by the production and fission of {sup 239}Pu. Simulations have shown that the fuel burnup can reach values greater than 400 MWd/kgIHM, before fission products poison the reaction. In this work we compare the production of plutonium and minor actinides produced in a fission wave to that of a UOX fueled light water reactor, both on an energy normalized basis. The nuclide concentrations in the spent traveling wave reactor fuel are computed using a one-group diffusion model and are verified using Monte Carlo simulations. In the case of the pressurized water reactor, a multi-group collision probability model is used to generate the nuclide quantities. We find that the traveling wave reactor produces about 0.187 g/MWd/kgIHM of transuranics compared to 0.413 g/MWd/kgIHM for a pressurized water reactor running fuel enriched to 4.95 % and burned to 50 MWd/kgIHM. (authors)« less

Dissolution of Used Nuclear Fuel Using a TBP/N-Paraffin Solvent

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudisill, T. S.; Shehee, T. C.; Jones, D. H.

2017-10-02

The dissolution of unirradiated used nuclear fuel (UNF) pellets pretreated for tritium removal was demonstrated using a tributly phosphate (TBP) solvent. Dissolution of pretreated fuel in TBP could potentially combine dissolution with two cycle of solvent extraction required for separating the actinides and lanthanides from other fission products. Dissolutions were performed using UNF surrogates prepared from both uranyl nitrate and uranium trioxide produced from the pretreatment process by adding selected actinide and stable fission product elements. In laboratory-scale experiments, the U dissolution efficiency ranged from 80-99+% for both the nitrate and oxide surrogate fuels. On average, 80% of the Pumore » and 50% of the Np and Am in the nitrate surrogate dissolved; however, little of the transuranic elements dissolved in the oxide form. The majority of the 3+ lanthanide elements dissolved. Only small amounts of Sr (0-1.6%) and Mo (0.1-1.7%) and essentially no Cs, Ru, Zr, or Pd dissolved.« less

An assessment of the attractiveness of material associated with thorium/uranium and uranium closed fuel cycles from a safeguards perspective

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bathke, Charles Gary; Wallace, Richard K; Hase, Kevin R

2010-01-01

This paper reports the continued evaluation of the attractiveness of materials mixtures containing special nuclear materials (SNM) associated with various proposed nuclear fuel cycles. Specifically, this paper examines two closed fuel cycles. The first fuel cycle examined is a thorium fuel cycle in which a pressurized heavy water reactor (PHWR) is fueled with mixtures of plutonium/thorium and {sup 233}U/thorium. The used fuel is then reprocessed using the THOREX process and the actinides are recycled. The second fuel cycle examined consists of conventional light water reactors (LWR) whose fuel is reprocessed for actinides that are then fed to and recycled untilmore » consumed in fast-spectrum reactors: fast reactors and accelerator driven systems (ADS). As reprocessing of LWR fuel has already been examined, this paper will focus on the reprocessing of the scheme's fast-spectrum reactors' fuel. This study will indicate what is required to render these materials as having low utility for use in nuclear weapons. Nevertheless, the results of this paper suggest that all reprocessing products evaluated so far need to be rigorously safeguarded and provided high levels of physical protection. These studies were performed at the request of the United States Department of Energy (DOE). The methodology and key findings will be presented.« less

Managing Zirconium Chemistry and Phase Compatibility in Combined Process Separations for Minor Actinide Partitioning

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wall, Nathalie; Nash, Ken; Martin, Leigh

In response to the NEUP Program Supporting Fuel Cycle R&D Separations and Waste Forms call DEFOA- 0000799, this report describes the results of an R&D project focusing on streamlining separation processes for advanced fuel cycles. An example of such a process relevant to the U.S. DOE FCR&D program would be one combining the functions of the TRUEX process for partitioning of lanthanides and minor actinides from PUREX(UREX) raffinates with that of the TALSPEAK process for separating transplutonium actinides from fission product lanthanides. A fully-developed PUREX(UREX)/TRUEX/TALSPEAK suite would generate actinides as product(s) for reuse (or transmutation) and fission products as waste.more » As standalone, consecutive unit-operations, TRUEX and TALSPEAK employ different extractant solutions (solvating (CMPO, octyl(phenyl)-N,Ndiisobutylcarbamoylmethylphosphine oxide) vs. cation exchanging (HDEHP, di-2(ethyl)hexylphosphoric acid) extractants), and distinct aqueous phases (2-4 M HNO 3 vs. concentrated pH 3.5 carboxylic acid buffers containing actinide selective chelating agents). The separate processes may also operate with different phase transfer kinetic constraints. Experience teaches (and it has been demonstrated at the lab scale) that, with proper control, multiple process separation systems can operate successfully. However, it is also recognized that considerable economies of scale could be achieved if multiple operations could be merged into a single process based on a combined extractant solvent. The task of accountability of nuclear materials through the process(es) also becomes more robust with fewer steps, providing that the processes can be accurately modeled. Work is underway in the U.S. and Europe on developing several new options for combined processes (TRUSPEAK, ALSEP, SANEX, GANEX, ExAm are examples). There are unique challenges associated with the operation of such processes, some relating to organic phase chemistry, others arising from the variable composition of the aqueous medium. This project targets in particular two problematic issues in designing combined process systems: managing the chemistry of challenging aqueous species (like Zr 4+) and optimizing the composition and properties of combined extractant organic phases.« less

Post-irradiation examinations of THERMHET composite fuels for transmutation

NASA Astrophysics Data System (ADS)

Noirot, J.; Desgranges, L.; Chauvin, N.; Georgenthum, V.

2003-07-01

The thermal behaviour of composite targets dedicated to minor actinide transmutation was studied using THERMHET (thermal behaviour of heterogeneous fuel) irradiation in the SILOE reactor. Three inert matrix fuel designs were tested (macro-mass, jingle and microdispersion) all with a MgAl 2O 4 spinel inert matrix and around 40% weight of UO 2 to simulate minor actinide inclusions. The post-irradiation examinations led to a new interpretation of the temperature measurement by thermocouples located in the central hole of the pellets. A major change in the micro-dispersed structure was detected. The examinations enabled us to understand the behaviour of the spinel during the different stages of irradiation. They revealed an amorphisation at low temperature and then a nano re-crystallisation at high temperature of the spinel in the micro-dispersed case. These results, together with those obtained in the MATINA irradiation of an equivalent structure, show the importance of the irradiation temperature on spinel behaviour.

Oxygen potentials of mixed oxide fuels for fast reactors

NASA Astrophysics Data System (ADS)

Kato, M.; Tamura, T.; Konashi, K.

2009-03-01

Oxygen potentials of homogenous (Pu0.2U0.8)O2-x and (Am0.02Pu0.30Np0.02U0.66)O2-x which have been developed as fuels for fast breeder reactors were measured at temperatures of 1473-1623 K by a gas equilibrium method using an (Ar, H2, H2O) gas mixture. The measured oxygen potentials of (Pu0.2U0.8)O2-x were about 25 kJ mol-1 lower than those of (Pu0.3U0.7)O2-x measured previously and were consistent with the values calculated by Besmann and Lindemer's model. The measured oxygen potentials of (Am0.02Pu0.30Np0.02U0.66)O2-x were slightly higher than those of MOX without minor actinides. No fuel-cladding chemical interaction is affected significantly by adding their minor actinides.

Gas core reactors for actinide transmutation and breeder applications

NASA Technical Reports Server (NTRS)

Clement, J. D.; Rust, J. H.

1978-01-01

This work consists of design power plant studies for four types of reactor systems: uranium plasma core breeder, uranium plasma core actinide transmuter, UF6 breeder and UF6 actinide transmuter. The plasma core systems can be coupled to MHD generators to obtain high efficiency electrical power generation. A 1074 MWt UF6 breeder reactor was designed with a breeding ratio of 1.002 to guard against diversion of fuel. Using molten salt technology and a superheated steam cycle, an efficiency of 39.2% was obtained for the plant and the U233 inventory in the core and heat exchangers was limited to 105 Kg. It was found that the UF6 reactor can produce high fluxes (10 to the 14th power n/sq cm-sec) necessary for efficient burnup of actinide. However, the buildup of fissile isotopes posed severe heat transfer problems. Therefore, the flux in the actinide region must be decreased with time. Consequently, only beginning-of-life conditions were considered for the power plant design. A 577 MWt UF6 actinide transmutation reactor power plant was designed to operate with 39.3% efficiency and 102 Kg of U233 in the core and heat exchanger for beginning-of-life conditions.

Enhancing BWR proliferation resistance fuel with minor actinides

NASA Astrophysics Data System (ADS)

Chang, Gray S.

2009-03-01

To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced light water reactor- LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides ( 237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu/Pu. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO 2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate-term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm 3) to the top (0.35 g/cm 3) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. The concept of MARA, which involves the use of transuranic nuclides ( 237Np and/or 241Am), significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms for peace and the intermediate-term of nuclear energy reconnaissance.

New developments and prospects on COSI, the simulation software for fuel cycle analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Eschbach, R.; Meyer, M.; Coquelet-Pascal, C.

2013-07-01

COSI, software developed by the Nuclear Energy Direction of the CEA, is a code simulating a pool of nuclear power plants with its associated fuel cycle facilities. This code has been designed to study various short, medium and long term options for the introduction of various types of nuclear reactors and for the use of associated nuclear materials. In the frame of the French Act for waste management, scenario studies are carried out with COSI, to compare different options of evolution of the French reactor fleet and options of partitioning and transmutation of plutonium and minor actinides. Those studies aimmore » in particular at evaluating the sustainability of Sodium cooled Fast Reactors (SFR) deployment and the possibility to transmute minor actinides. The COSI6 version is a completely renewed software released in 2006. COSI6 is now coupled with the last version of CESAR (CESAR5.3 based on JEFF3.1.1 nuclear data) allowing the calculations on irradiated fuel with 200 fission products and 100 heavy nuclides. A new release is planned in 2013, including in particular the coupling with a recommended database of reactors. An exercise of validation of COSI6, carried out on the French PWR historic nuclear fleet, has been performed. During this exercise quantities like cumulative natural uranium consumption, or cumulative depleted uranium, or UOX/MOX spent fuel storage, or stocks of reprocessed uranium, or plutonium content in fresh MOX fuel, or the annual production of high level waste, have been computed by COSI6 and compared to industrial data. The results have allowed us to validate the essential phases of the fuel cycle computation, and reinforces the credibility of the results provided by the code.« less

FCRD Advanced Reactor (Transmutation) Fuels Handbook

DOE Office of Scientific and Technical Information (OSTI.GOV)

Janney, Dawn Elizabeth; Papesch, Cynthia Ann

2016-09-01

Transmutation of minor actinides such as Np, Am, and Cm in spent nuclear fuel is of international interest because of its potential for reducing the long-term health and safety hazards caused by the radioactivity of the spent fuel. One important approach to transmutation (currently being pursued by the DOE Fuel Cycle Research & Development Advanced Fuels Campaign) involves incorporating the minor actinides into U-Pu-Zr alloys, which can be used as fuel in fast reactors. U-Pu-Zr alloys are well suited for electrolytic refining, which leads to incorporation rare-earth fission products such as La, Ce, Pr, and Nd. It is, therefore, importantmore » to understand not only the properties of U-Pu-Zr alloys but also those of U-Pu-Zr alloys with concentrations of minor actinides (Np, Am) and rare-earth elements (La, Ce, Pr, and Nd) similar to those in reprocessed fuel. In addition to requiring extensive safety precautions, alloys containing U, Pu, and minor actinides (Np and Am) are difficult to study for numerous reasons, including their complex phase transformations, characteristically sluggish phasetransformation kinetics, tendency to produce experimental results that vary depending on the histories of individual samples, rapid oxidation, and sensitivity to contaminants such as oxygen in concentrations below a hundred parts per million. Although less toxic, rare-earth elements such as La, Ce, Pr, and Nd are also difficult to study for similar reasons. Many of the experimental measurements were made before 1980, and the level of documentation for experimental methods and results varies widely. It is, therefore, not surprising that little is known with certainty about U-Pu-Zr alloys, particularly those that also contain minor actinides and rare-earth elements. General acceptance of results commonly indicates that there is only a single measurement for a particular property. This handbook summarizes currently available information about U, Pu, Zr, Np, Am, La, Ce, Pr, and Nd and alloys of two or three of these elements. It contains information about phase diagrams and related information (including phases and phase transformations); heat capacity, entropy, and enthalpy; thermal expansion; and thermal conductivity and diffusivity. In addition to presenting information about materials properties, the handbook attempts to provide information about how well the property is known and how much variation exists between measurements. Although it includes some results from models, its primary focus is experimental data. The Handbook is organized in two sections: one with information about the U-Pu-Zr ternary and one with information about other elements and binary and vi ternary alloys in the U-Np-Pu-Am-La-Ce-Pr-Nd-Zr system. Within each section, information about elements is presented first, followed by information about binary alloys, then information about ternary alloys. The order in which the elements in each alloy are mentioned follows the order in the first sentence of this paragraph. Much of the information on the U-Pu-Zr system repeats information from the FCRD Transmutation Fuels Handbook 2015. Most of the other data has been published elsewhere (although scattered throughout numerous references, some quite obscure); however, some data from Idaho National Laboratory is presented here for the first time. As the FCRD programmatic mission evolves, future editions of this handbook will begin to include other advanced reactor fuel designs and compositions. Hence, the title of the handbook will transition to the Advanced Reactor Fuels Handbook.« less

Cross-cutting High Surface Area Graphene-based Frameworks with Controlled Pore Structure/Dopants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gaillard, J.

The goal of this project is to enhance the performance of graphene-based materials by manufacturing specific 3D architectures. The materials have global applications regarding fuel cell catalysts, gas adsorbents, supercapacitor/battery electrodes, ion (e.g., actinide) capture, gas separation, oil adsorption, and catalysis. This research focuses on hydrogen storage for hydrogen fuel cell vehicles with a potential transformational impact on hydrogen adsorbents that exhibit high gravimetric and volumetric density, a clean energy application sought by the Department of Energy. The development of an adsorbent material would enable broad commercial opportunities in hydrogen-fueled vehicles, promote new advanced nanomanufacturing scale-up, and open other opportunitiesmore » at Savannah River National Laboratory to utilize a high surface area material that is robust, chemically stable, and radiation resistant.« less

Technical and economic assessment of different options for minor actinide transmutation: the French case

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chabert, C.; Coquelet-Pascal, C.; Saturnin, A.

Studies have been performed to assess the industrial perspectives of partitioning and transmutation of long-lived elements. These studies were carried out in tight connection with GEN-IV systems development. The results include the technical and economic evaluation of fuel cycle scenarios along with different options for optimizing the processes between the minor actinide transmutation in fast neutron reactors, their interim storage and geological disposal of ultimate waste. The results are analysed through several criteria (impacts on waste, on waste repository, on fuel cycle plants, on radiological exposure of workers, on costs and on industrial risks). These scenario evaluations take place inmore » the French context which considers the deployment of the first Sodium-cooled Fast Reactor (SFR) in 2040. 3 management options of minor actinides have been studied: no transmutation, transmutation in SFR and transmutation in an accelerator-driven system (ADS). Concerning economics the study shows that the cost overrun related to the transmutation process could vary between 5 to 9% in SFR and 26 % in the case of ADS.« less

Monte Carlo calculations of the incineration of plutonium and minor actinides of laser fusion inertial confinement fusion fission energy (LIFE) engine

NASA Astrophysics Data System (ADS)

Adem, ACIR; Eşref, BAYSAL

2018-07-01

In this paper, neutronic analysis in a laser fusion inertial confinement fusion fission energy (LIFE) engine fuelled plutonium and minor actinides using a MCNP codes was investigated. LIFE engine fuel zone contained 10 vol% TRISO particles and 90 vol% natural lithium coolant mixture. TRISO fuel compositions have Mod①: reactor grade plutonium (RG-Pu), Mod②: weapon grade plutonium (WG-Pu) and Mod③: minor actinides (MAs). Tritium breeding ratios (TBR) were computed as 1.52, 1.62 and 1.46 for Mod①, Mod② and Mod③, respectively. The operation period was computed as ∼21 years when the reference TBR > 1.05 for a self-sustained reactor for all investigated cases. Blanket energy multiplication values (M) were calculated as 4.18, 4.95 and 3.75 for Mod①, Mod② and Mod③, respectively. The burnup (BU) values were obtained as ∼1230, ∼1550 and ∼1060 GWd tM–1, respectively. As a result, the higher BU were provided with using TRISO particles for all cases in LIFE engine.

Closed DTU fuel cycle with Np recycle and waste transmutation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Beller, D.E.; Sailor, W.C.; Venneri, F.

1999-09-01

A nuclear energy scenario for the 21st century that included a denatured thorium-uranium-oxide (DTU) fuel cycle and new light water reactors (LWRs) supported by accelerator-driven transmutation of waste (ATW) systems was previously described. This coupled system with the closed DTU fuel cycle provides several improvements beyond conventional LWR (CLWR) (once-through, UO{sub 2} fuel) nuclear technology: increased proliferation resistance, reduced waste, and efficient use of natural resources. However, like CLWR fuel cycles, the spent fuel in the first one-third core discharged after startup contains higher-quality Pu than the equilibrium fuel cycle. To eliminate this high-grade Pu, Np is separated and recycledmore » with Th and U--rather than with higher actinides [(HA) including Pu]. The presence of Np in the LWR feed greatly increases the production of {sup 238}Pu so that a few kilograms of Pu generated enough alpha-decay heat that the separated Pu is highly resistant to proliferation. This alternate process also simplifies the pyrochemical separation of fuel elements (Th and U) from HAs. To examine the advantages of this concept, the authors modeled a US deployment scenario for nuclear energy that includes DTU-LWRs plus ATW`s to burn the actinides produced by these LWRs and to close the back-end of the DTU fuel cycle.« less

Ligand induced shape transformation of thorium dioxide nanocrystals.

PubMed

Wang, Gaoxue; Batista, Enrique R; Yang, Ping

2018-04-27

Nanocrystals (NCs) with size and shape dependent properties are a thriving research field. Remarkable progress has been made in the controlled synthesis of NCs of stable elements in the past two decades; however, the knowledge of the NCs of actinide compounds has been considerably limited due the difficulties in handling them both experimentally and theoretically. Actinide compounds, especially actinide oxides, play a critical role in many stages of the nuclear fuel cycle. Recently, a non-aqueous surfactant assisted approach has been developed for the synthesis of actinide oxide NCs with different morphologies, but an understanding of its control factors is still missing to date. Herein we present a comprehensive study on the low index surfaces of thorium dioxide (ThO2) and their interactions with relevant surfactant ligands using density functional calculations. A systematic picture on the thermodynamic stability of ThO2 NCs of different sizes and shapes is obtained employing empirical models based on the calculated surface energies. It is found that bare ThO2 NCs prefer the octahedral shape terminated by (111) surfaces. Oleic acid displays selective adsorption on the (110) surface, leading to the shape transformation from octahedrons to nanorods. Other ligands such as acetylacetone, oleylamine, and trioctylphosphine oxide do not modify the equilibrium shape of ThO2 NCs. This work provides atomic level insights into the anisotropic growth of ThO2 NCs that was recently observed in experiments, and thus may contribute to the controlled synthesis of actinide oxide NCs with well-defined size and shape for future applications.

The Effects of Radiation Chemistry on Solvent Extraction: 1. Conditions in Acidic Solution and a Review of TBP Radiolysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bruce J. Mincher; Guiseppe Modolo; Strephen P. Mezyk

2009-01-01

Solvent extraction is the most commonly used process scale separation technique for nuclear applications and it benefits from more than 60 years of research and development and proven experience at the industrial scale. Advanced solvent extraction processes for the separation of actinides and fission products from dissolved nuclear fuel are now being investigated worldwide by numerous groups (US, Europe, Russia, Japan etc.) in order to decrease the radiotoxic inventories of nuclear waste. While none of the advanced processes have yet been implemented at the industrial scale their development studies have sometimes reached demonstration tests at the laboratory scale. Most ofmore » the partitioning strategies rely on the following four separations: 1. Partitioning of uranium and/or plutonium from spent fuel dissolution liquors. 2. Separation of the heat generating fission products such as strontium and cesium. 3. Coextraction of the trivalent actinides and lanthanides. 4. Separation of the trivalent actinides from the trivalent lanthanides. Tributylphosphate (TBP) in the first separation is the basis of the PUREX, UREX and COEX processes, developed in Europe and the US, whereas monoamides as alternatives for TBP are being developed in Japan and India. For the second separation, many processes were developed worldwide, including the use of crown-ether extractants, like the FPEX process developed in the USA, and the CCD-PEG process jointly developed in the USA and Russia for the partitioning of cesium and strontium. In the third separation, phosphine oxides (CMPOs), malonamides, and diglycolamides are used in the TRUEX, DIAMEX and the ARTIST processes, respectively developed in US, Europe and Japan. Trialkylphosphine oxide(TRPO) developed in China, or UNEX (a mixture of several extractants) jointly developed in Russia and the USA allow all actinides to be co-extracted from acidic radioactive liquid waste. For the final separation, soft donor atom-containing ligands such as the bistriazinylbipyridines (BTBPs) or dithiophosphinic acids have been developed in Europe and China to selectively extract the trivalent actinides. However, in the TALSPEAK process developed in the USA, the separation is based on the relatively high affinity of aminopolycarboxylic acid complexants such as DTPA for trivalent actinides over lanthanides. In the DIDPA, SETFICS and the GANEX processes, developed in Japan and France, the group separation is accomplished in a reverse TALSPEAK process. A typical scenario is shown in Figure 1 for the UREX1a (Uranium Extraction version 1a) process. The initial step is the TBP extraction for the separation of recyclable uranium. The second step partitions the short-lived, highly radioactive cesium and strontium to minimize heat loading in the high-level waste repository. The third step is a group separation of the trivalent actinides and lanthanides with the last step being partitioning of the trivalent lanthanides from the actinides.« less

Radiotoxicity Characterization of Multi-Recycled Thorium Fuel - 12394

DOE Office of Scientific and Technical Information (OSTI.GOV)

Franceschini, F.; Wenner, M.; Fiorina, C.

2012-07-01

As described in companion papers, Westinghouse is proposing the implementation of a thorium based fuel cycle to burn the transuranic (TRU) contained in the used nuclear fuel. The potential of thorium as a TRU burner is described in another paper presented at this conference. This paper analyzes the long-term impact of thorium on the front-end and backend of the fuel cycle. This is accomplished by an assessment of the isotopic make-up of Th in a closed cycle and its impact on representative metrics, such as radiotoxicity, decay heat and gamma heat. The behavior in both thermal and fast neutron energymore » ranges has been investigated. Irradiation in a Th fuel PWR has been assumed as representative of the thermal range, while a Th fuel fast reactor (FR) has been employed to characterize the behavior in the high-energy range. A comparison with a U-fuel closed-cycle FR has been undertaken in an attempt of a more comprehensive evaluation of each cycle's long-term potential. As the Th fuel undergoes multiple cycles of irradiation, the isotopic composition of the recycled fuel changes. Minor Th isotopes are produced; U-232 and Pa-231 build up; the U vector gradually shifts towards increasing amounts of U-234, U-235 etc., eventually leading to the production of non negligible amounts of TRU isotopes, especially Pu-238. The impact of the recycled fuel isotopic makeup on the in-core behavior is mild, and for some aspects beneficial, i.e. the reactivity swing during irradiation is reduced as the fertile characteristics of the fuel increase. On the other hand, the front and the back-end of the fuel cycle are negatively affected due to the presence of Th-228 and U-232 and the build-up of higher actinides (Pu-238 etc.). The presence of U-232 can also be seen as advantageous as it represents an obstacle to potential proliferators. Notwithstanding the increase in the short-term radiotoxicity and decay heat in the multi-recycled fuel, the Th closed cycle has some potentially substantial advantages compared to the U cycle, such as the smaller actinide radiotoxicity and decay heat for up to 25,000 years after irradiation. In order for these benefits to materialize, the capability to reprocess and remotely manufacture industrial amounts of recycled fuel appears to be the key. Westinghouse is proposing the implementation of a thorium based fuel cycle to burn the TRU contained in the current UNF. The general approach and the potential of thorium as TRU burner is described in other papers presented at this conference. The focus of this paper is to analyze the long-term potential of thorium, once the legacy TRU has been exhausted and the thorium reactor system will become self-sufficient. Therefore, a comparison of Th closed cycle, in fast and thermal neutron energy ranges, vs. U closed cycle, in the fast energy range, has been undertaken. The results presented focus on selected backend and front-end metrics: isotopic actinide composition and potential implications on ingested radiotoxicity, decay heat and gamma heat. The evaluation confirms potential substantial improvements in the backend of the fuel cycle by transitioning to a thorium closed cycle. These benefits are the result of a much lower TRU content, in particular Pu-241, Am-241 and Pu-240, characterizing the Th vs. U actinide inventories, and the ensuing process waste to be disposed. On the other hand, the larger gamma activity of Th recycled fuel, consisting predominantly of hard gammas from U-232's decay products, is a significant challenge for fuel handling, transportation and manufacturing but can be claimed as beneficial for the proliferation resistance of the fuel. It is worth remembering that in our perspective the Th closed cycle and the U closed cycle will follow a transmutation phase which will likely take place over several decades and dictate the technologies required. These will likely include remote fuel manufacturing, regardless of the specific system adopted for the transmutation, which could then be inherited for the ensuing closed cycles. Finally, specific data related to the fuel manufacturing and separation technologies and their performance in the prospected industrial scale deployment, are key for further quantification of the potential merits of the options explored. Further studies in this direction should be warranted before making definitive conclusion. (authors)« less

High-temperature Gas Reactor (HTGR)

NASA Astrophysics Data System (ADS)

Abedi, Sajad

2011-05-01

General Atomics (GA) has over 35 years experience in prismatic block High-temperature Gas Reactor (HTGR) technology design. During this period, the design has recently involved into a modular have been performed to demonstrate its versatility. This versatility is directly related to refractory TRISO coated - particle fuel that can contain any type of fuel. This paper summarized GA's fuel cycle studies individually and compares each based upon its cycle sustainability, proliferation-resistance capabilities, and other performance data against pressurized water reactor (PWR) fuel cycle data. Fuel cycle studies LEU-NV;commercial HEU-Th;commercial LEU-Th;weapons-grade plutonium consumption; and burning of LWR waste including plutonium and minor actinides in the MHR. results show that all commercial MHR options, with the exception of HEU-TH, are more sustainable than a PWR fuel cycle. With LEU-NV being the most sustainable commercial options. In addition, all commercial MHR options out perform the PWR with regards to its proliferation-resistance, with thorium fuel cycle having the best proliferation-resistance characteristics.

A physical and economic model of the nuclear fuel cycle

NASA Astrophysics Data System (ADS)

Schneider, Erich Alfred

A model of the nuclear fuel cycle that is suitable for use in strategic planning and economic forecasting is presented. The model, to be made available as a stand-alone software package, requires only a small set of fuel cycle and reactor specific input parameters. Critical design criteria include ease of use by nonspecialists, suppression of errors to within a range dictated by unit cost uncertainties, and limitation of runtime to under one minute on a typical desktop computer. Collision probability approximations to the neutron transport equation that lead to a computationally efficient decoupling of the spatial and energy variables are presented and implemented. The energy dependent flux, governed by coupled integral equations, is treated by multigroup or continuous thermalization methods. The model's output includes a comprehensive nuclear materials flowchart that begins with ore requirements, calculates the buildup of 24 actinides as well as fission products, and concludes with spent fuel or reprocessed material composition. The costs, direct and hidden, of the fuel cycle under study are also computed. In addition to direct disposal and plutonium recycling strategies in current use, the model addresses hypothetical cycles. These include cycles chosen for minor actinide burning and for their low weapons-usable content.

Use of freeze-casting in advanced burner reactor fuel design

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lang, A. L.; Yablinsky, C. A.; Allen, T. R.

2012-07-01

This paper will detail the modeling of a fast reactor with fuel pins created using a freeze-casting process. Freeze-casting is a method of creating an inert scaffold within a fuel pin. The scaffold is created using a directional solidification process and results in open porosity for emplacement of fuel, with pores ranging in size from 300 microns to 500 microns in diameter. These pores allow multiple fuel types and enrichments to be loaded into one fuel pin. Also, each pore could be filled with varying amounts of fuel to allow for the specific volume of fission gases created by thatmore » fuel type. Currently fast reactors, including advanced burner reactors (ABR's), are not economically feasible due to the high cost of operating the reactors and of reprocessing the fuel. However, if the fuel could be very precisely placed, such as within a freeze-cast scaffold, this could increase fuel performance and result in a valid design with a much lower cost per megawatt. In addition to competitive costs, freeze-cast fuel would also allow for selective breeding or burning of actinides within specific locations in fast reactors. For example, fast flux peak locations could be utilized on a minute scale to target specific actinides for transmutation. Freeze-cast fuel is extremely flexible and has great potential in a variety of applications. This paper performs initial modeling of freeze-cast fuel, with the generic fast reactor parameters for this model based on EBR-II. The core has an assumed power of 62.5 MWt. The neutronics code used was Monte Carlo N-Particle (MCNP5) transport code. Uniform pore sizes were used in increments of 100 microns. Two different freeze-cast scaffold materials were used: ceramic (MgO-ZrO{sub 2}) and steel (SS316L). Separate models were needed for each material because the freeze-cast ceramic and metal scaffolds have different structural characteristics and overall porosities. Basic criticality results were compiled for the various models. Preliminary results show that criticality is achievable with freeze-cast fuel pins despite the significant amount of inert fuel matrix. Freeze casting is a promising method to achieve very precise fuel placement within fuel pins. (authors)« less

Science and Technology Review June 2000

DOE Office of Scientific and Technical Information (OSTI.GOV)

de Pruneda, J.H.

2000-06-01

This issue contains the following articles: (1) ''Accelerating on the ASCI Challenge''. (2) ''New Day Daws in Supercomputing'' When the ASCI White supercomputer comes online this summer, DOE's Stockpile Stewardship Program will make another significant advanced toward helping to ensure the safety, reliability, and performance of the nation's nuclear weapons. (3) ''Uncovering the Secrets of Actinides'' Researchers are obtaining fundamental information about the actinides, a group of elements with a key role in nuclear weapons and fuels. (4) ''A Predictable Structure for Aerogels''. (5) ''Tibet--Where Continents Collide''.

The chemistry of TALSPEAK: A review of the science

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nash, Kenneth L.

Here, the TALSPEAK Process (Trivalent Actinide Lanthanide Separation with Phosphorus-reagent Extraction from Aqueous Komplexes) was originally developed at Oak Ridge National Laboratory by B. Weaver and F.A. Kappelmann in the 1960s. It was envisioned initially as an alternative to the TRAMEX process (selective extraction of trivalent actinides by tertiary or quaternary amines over fission product lanthanides from concentrated LiCl solutions). TALSPEAK proposed the selective extraction of trivalent lanthanides away from the actinides, which are retained in the aqueous phase as aminopolycarboxylate complexes. After several decades of research and development, the conventional TALSPEAK process (based on di-(2-ethylhexyl) phosphoric acid (extractant) inmore » 1,4-di-isopropylbenzene (diluent) and a concentrated lactate buffer containing diethylenetriamine-N,N,N',N",N"-pentaacetic acid (actinide-selective holdback reagent)) has become a widely recognized benchmark for advanced aqueous partitioning of the trivalent 4f/5f elements. TALSPEAK chemistry has also been utilized as an actinide-selective stripping agent (Reverse TALSPEAK) with some notable success. Under ideal conditions, conventional TALSPEAK separates Am 3+ from Nd 3+ (the usual limiting pair) with a single-stage separation factor of about 100; both lighter and heavier lanthanides are more completely separated from Am 3+. Despite this apparent efficiency, TALSPEAK has not seen enthusiastic adoption for advanced partitioning of nuclear fuels at process scale for two principle reasons: 1) all adaptations of TALSPEAK chemistry to process scale applications require rigid pH control within a narrow range of pH, and 2) phase transfer kinetics are often slower than ideal. To compensate for these effects, high concentrations of the buffer (0.5-2 M H/Na lactate) are required. Acknowledgement of these complications in TALSPEAK process development has inspired significant research activities dedicated to improving understanding of the basic chemistry that controls TALSPEAK (and related processes based on the application of actinide-selective holdback reagents). In the following report, advances in understanding of the fundamental chemistry of TALSPEAK that have occurred during the past decade will be reviewed and discussed.« less

The chemistry of TALSPEAK: A review of the science

DOE PAGES

Nash, Kenneth L.

2014-11-13

Here, the TALSPEAK Process (Trivalent Actinide Lanthanide Separation with Phosphorus-reagent Extraction from Aqueous Komplexes) was originally developed at Oak Ridge National Laboratory by B. Weaver and F.A. Kappelmann in the 1960s. It was envisioned initially as an alternative to the TRAMEX process (selective extraction of trivalent actinides by tertiary or quaternary amines over fission product lanthanides from concentrated LiCl solutions). TALSPEAK proposed the selective extraction of trivalent lanthanides away from the actinides, which are retained in the aqueous phase as aminopolycarboxylate complexes. After several decades of research and development, the conventional TALSPEAK process (based on di-(2-ethylhexyl) phosphoric acid (extractant) inmore » 1,4-di-isopropylbenzene (diluent) and a concentrated lactate buffer containing diethylenetriamine-N,N,N',N",N"-pentaacetic acid (actinide-selective holdback reagent)) has become a widely recognized benchmark for advanced aqueous partitioning of the trivalent 4f/5f elements. TALSPEAK chemistry has also been utilized as an actinide-selective stripping agent (Reverse TALSPEAK) with some notable success. Under ideal conditions, conventional TALSPEAK separates Am 3+ from Nd 3+ (the usual limiting pair) with a single-stage separation factor of about 100; both lighter and heavier lanthanides are more completely separated from Am 3+. Despite this apparent efficiency, TALSPEAK has not seen enthusiastic adoption for advanced partitioning of nuclear fuels at process scale for two principle reasons: 1) all adaptations of TALSPEAK chemistry to process scale applications require rigid pH control within a narrow range of pH, and 2) phase transfer kinetics are often slower than ideal. To compensate for these effects, high concentrations of the buffer (0.5-2 M H/Na lactate) are required. Acknowledgement of these complications in TALSPEAK process development has inspired significant research activities dedicated to improving understanding of the basic chemistry that controls TALSPEAK (and related processes based on the application of actinide-selective holdback reagents). In the following report, advances in understanding of the fundamental chemistry of TALSPEAK that have occurred during the past decade will be reviewed and discussed.« less

The Complete Burning of Weapons Grade Plutonium and Highly Enriched Uranium with (Laser Inertial Fusion-Fission Energy) LIFE Engine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Farmer, J C; Diaz de la Rubia, T; Moses, E

2008-12-23

The National Ignition Facility (NIF) project, a laser-based Inertial Confinement Fusion (ICF) experiment designed to achieve thermonuclear fusion ignition and burn in the laboratory, is under construction at the Lawrence Livermore National Laboratory (LLNL) and will be completed in April of 2009. Experiments designed to accomplish the NIF's goal will commence in late FY2010 utilizing laser energies of 1 to 1.3 MJ. Fusion yields of the order of 10 to 20 MJ are expected soon thereafter. Laser initiated fusion-fission (LIFE) engines have now been designed to produce nuclear power from natural or depleted uranium without isotopic enrichment, and from spentmore » nuclear fuel from light water reactors without chemical separation into weapons-attractive actinide streams. A point-source of high-energy neutrons produced by laser-generated, thermonuclear fusion within a target is used to achieve ultra-deep burn-up of the fertile or fissile fuel in a sub-critical fission blanket. Fertile fuels including depleted uranium (DU), natural uranium (NatU), spent nuclear fuel (SNF), and thorium (Th) can be used. Fissile fuels such as low-enrichment uranium (LEU), excess weapons plutonium (WG-Pu), and excess highly-enriched uranium (HEU) may be used as well. Based upon preliminary analyses, it is believed that LIFE could help meet worldwide electricity needs in a safe and sustainable manner, while drastically shrinking the nation's and world's stockpile of spent nuclear fuel and excess weapons materials. LIFE takes advantage of the significant advances in laser-based inertial confinement fusion that are taking place at the NIF at LLNL where it is expected that thermonuclear ignition will be achieved in the 2010-2011 timeframe. Starting from as little as 300 to 500 MW of fusion power, a single LIFE engine will be able to generate 2000 to 3000 MWt in steady state for periods of years to decades, depending on the nuclear fuel and engine configuration. Because the fission blanket in a fusion-fission hybrid system is subcritical, a LIFE engine can burn any fertile or fissile nuclear material, including unenriched natural or depleted U and SNF, and can extract a very high percentage of the energy content of its fuel resulting in greatly enhanced energy generation per metric ton of nuclear fuel, as well as nuclear waste forms with vastly reduced concentrations of long-lived actinides. LIFE engines could thus provide the ability to generate vast amounts of electricity while greatly reducing the actinide content of any existing or future nuclear waste and extending the availability of low cost nuclear fuels for several thousand years. LIFE also provides an attractive pathway for burning excess weapons Pu to over 99% FIMA (fission of initial metal atoms) without the need for fabricating or reprocessing mixed oxide fuels (MOX). Because of all of these advantages, LIFE engines offer a pathway toward sustainable and safe nuclear power that significantly mitigates nuclear proliferation concerns and minimizes nuclear waste. An important aspect of a LIFE engine is the fact that there is no need to extract the fission fuel from the fission blanket before it is burned to the desired final level. Except for fuel inspection and maintenance process times, the nuclear fuel is always within the core of the reactor and no weapons-attractive materials are available outside at any point in time. However, an important consideration when discussing proliferation concerns associated with any nuclear fuel cycle is the ease with which reactor fuel can be converted to weapons usable materials, not just when it is extracted as waste, but at any point in the fuel cycle. Although the nuclear fuel remains in the core of the engine until ultra deep actinide burn up is achieved, soon after start up of the engine, once the system breeds up to full power, several tons of fissile material is present in the fission blanket. However, this fissile material is widely dispersed in millions of fuel pebbles, which can be tagged as individual accountable items, and thus made difficult to divert in large quantities. This report discusses the application of the LIFE concept to nonproliferation issues, initially looking at the LIFE (Laser Inertial Fusion-Fission Energy) engine as a means of completely burning WG Pu and HEU. By combining a neutron-rich inertial fusion point source with energy-rich fission, the once-through closed fuel-cycle LIFE concept has the following characteristics: it is capable of efficiently burning excess weapons or separated civilian plutonium and highly enriched uranium; the fission blanket is sub-critical at all times (keff < 0.95); because LIFE can operate well beyond the point at which light water reactors (LWRs) need to be refueled due to burn-up of fissile material and the resulting drop in system reactivity, fuel burn-up of 99% or more appears feasible. The objective of this work is to develop LIFE technology for burning of WG-Pu and HEU.« less

FCRD Transmutation Fuels Handbook 2015

DOE Office of Scientific and Technical Information (OSTI.GOV)

Janney, Dawn Elizabeth; Papesch, Cynthia Ann

2015-09-01

Transmutation of minor actinides such as Np, Am, and Cm in spent nuclear fuel is of international interest because of its potential for reducing the long-term health and safety hazards caused by the radioactivity of the spent fuel. One important approach to transmutation (currently being pursued by the DOE Fuel Cycle Research & Development Advanced Fuels Campaign) involves incorporating the minor actinides into U-Pu-Zr alloys, which can be used as fuel in fast reactors. It is, therefore, important to understand the properties of U-Pu-Zr alloys, both with and without minor actinide additions. In addition to requiring extensive safety precautions, alloysmore » containing U and Pu are difficult to study for numerous reasons, including their complex phase transformations, characteristically sluggish phase-transformation kinetics, tendency to produce experimental results that vary depending on the histories of individual samples, and sensitivity to contaminants such as oxygen in concentrations below a hundred parts per million. Many of the experimental measurements were made before 1980, and the level of documentation for experimental methods and results varies widely. It is, therefore, not surprising that little is known with certainty about U-Pu-Zr alloys, and that general acceptance of results sometimes indicates that there is only a single measurement for a particular property. This handbook summarizes currently available information about U, Pu, Zr, and alloys of two or three of these elements. It contains information about phase diagrams and related information (including phases and phase transformations); heat capacity, entropy, and enthalpy; thermal expansion; and thermal conductivity and diffusivity. In addition to presenting information about materials properties, it attempts to provide information about how well the property is known and how much variation exists between measurements. Although the handbook includes some references to publications about modeling, its primary focus is experimental data. Most of the data has been published elsewhere (although scattered throughout numerous references, some quite obscure); however, some data is presented here for the first time.« less

Characterization of Delayed-Particle Emission Signatures for Pyroprocessing. Part 1: ABTR Fuel Assembly.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Durkee, Jr., Joe W.

A three-part study is conducted using the MCNP6 Monte Carlo radiation-transport code to calculate delayed-neutron (DN) and delayed-gamma (DG) emission signatures for nondestructive assay (NDA) metal-fuel pyroprocessing. In Part 1, MCNP6 is used to produce irradiation-induced used nuclear fuel (UNF) isotopic inventories for an Argonne National Laboratory (ANL) Advanced Burner Test Reactor (ABTR) preconceptual design fuel assembly (FA) model. The initial fuel inventory consists of uranium mixed with light-water-reactor transuranic (TRU) waste and 10 wt% zirconium (U-LWR-SFTRU-10%Zr). To facilitate understanding, parametric evaluation is done using models for 3% and 5% initial 235U a% enrichments, burnups of 5, 10, 15, 20,more » 30, …, 120 GWd/MTIHM, and 3-, 5-, 10-, 20-, and 30- year cooling times. Detailed delayed-particle radioisotope source terms for the irradiate FA are created using BAMF-DRT and SOURCES3A. Using simulation tallies, DG activity ratios (DGARs) are developed for 134Cs/ 137Cs 134Cs/ 154Eu, and 154Eu/ 137Cs markers as a function of (1) burnup and (2) actinide mass, including elemental uranium, neptunium, plutonium, americium, and curium. Spectral-integrated DN emission is also tallied. The study reveals a rich assortment of DGAR behavior as a function of DGAR type, enrichment, burnup, and cooling time. Similarly, DN emission plots show variation as a function of burnup and of actinide mass. Sensitivity of DGAR and DN signatures to initial 235U enrichment, burnup, and cooling time is evident. Comparisons of the ABTR radiation signatures and radiation signatures previously reported for a generic Westinghouse oxide-fuel assembly indicate that there are pronounced differences in the ABTR and Westinghouse oxide-fuel DN and DG signatures. These differences are largely attributable to the initial TRU inventory in the ABTR fuel. The actinide and nonactinide inventories for the FA models serve as source materials for the pre- and postelectrorefining models to be reported in Parts 2 and 3.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Syarifah, Ratna Dewi, E-mail: syarifah.physics@gmail.com; Suud, Zaki, E-mail: szaki@fi.itb.ac.id

Design study of small Pressurized Water Reactors (PWRs) core loaded with uranium nitride fuel (UN) and mixed nitride fuel (UN-PuN), Pa-231 as burnable poison, and Americium has been performed. Pa-231 known as actinide material, have large capture cross section and can be converted into fissile material that can be utilized to reduce excess reactivity. Americium is one of minor actinides with long half life. The objective of adding americium is to decrease nuclear spent fuel in the world. The neutronic analysis results show that mixed nitride fuel have k-inf greater than uranium nitride fuel. It is caused by the additionmore » of Pu-239 in mixed nitride fuel. In fuel fraction analysis, for uranium nitride fuel, the optimum volume fractions are 45% fuel fraction, 10% cladding and 45% moderator. In case of UN-PuN fuel, the optimum volume fractions are 30% fuel fraction, 10% cladding and 60% coolant/ moderator. The addition of Pa-231 as burnable poison for UN fuel, enrichment U-235 5%, with Pa-231 1.6% has k-inf more than one and excess reactivity of 14.45%. And for mixed nitride fuel, the lowest value of reactivity swing is when enrichment (U-235+Pu) 8% with Pa-231 0.4%, the excess reactivity value 13,76%. The fuel pin analyze for the addition of Americium, the excess reactivity value is lower than before, because Americium absorb the neutron. For UN fuel, enrichment U-235 8%, Pa-231 1.6% and Am 0.5%, the excess reactivity is 4.86%. And for mixed nitride fuel, when enrichment (U-235+Pu) 13%, Pa-231 0.4% and Am 0.1%, the excess reactivity is 11.94%. For core configuration, it is better to use heterogeneous than homogeneous core configuration, because the radial power distribution is better.« less

Accelerator-Driven Subcritical System for Disposing of the U.S. Spent Nuclear Fuel Inventory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gohar, Yousry; Cao, Yan; Kraus, Adam R.

The current United States inventory of the spent nuclear fuel (SNF) is ~80,000 metric tons of heavy metal (MTHM), including ~131 tons of minor actinides (MAs) and ~669 tons of plutonium. This study describes a conceptual design of an accelerator-driven subcritical (ADS) system for disposing of this SNF inventory by utilizing the 131 tons of MAs inventory and a fraction of the plutonium inventory for energy production, and transmuting some long-lived fission products. An ADS system with a homogeneous subcritical fission blanket was first examined. A spallation neutron source is used to drive the blanket and it is produced frommore » the interaction of a 1-GeV proton beam with a lead-bismuth eutectic (LBE) target. The blanket has a liquid mobile fuel using LBE as the fuel carrier. The fuel materials are dissolved, mixed, or suspended in the liquid fuel carrier. Monte Carlo analyses were performed to determine the overall parameters of the concept. Steady-state Monte Carlo simulations were performed for three similar fission blankets. Except for, the loaded amount of actinide materials in the LBE is either 5, 7, or 10% of the total volume of the blanket, respectively. The neutron multiplication factors of the three blankets are ~0.98 and the initial MAs blanket inventories are ~10 tons. In addition, Monte Carlo burnup simulations using the MCB5 code were performed to analyze the performance of the three conceptual ADS systems. During operation, fresh fuel was fed into the fission blanket to adjust its reactivity and to control the system power. The burnup analysis shows that the three ADS concepts consume about 1.2 tons of actinides per full power year and produce 3 GW thermal power, with a proton beam power of 25 MW. For the blankets with 5, 7, or 10% actinide fuel particles loaded in the LBE, assuming that the ADS systems can be operated for 35 full-power years, the total MA materials consumed in the three ADS systems are about 30.6, 35.3, and 37.2 tons, respectively. Thus, the corresponding numbers of ADS systems to utilize the 131 tons of MA materials of the SNF inventory are 4.3, 3.7, or 3.5, respectively. ADS concepts with tube bundles inserted in the fission blanket were analyzed to overcome the disadvantages of the homogeneous blanket concept. The liquid lead is used as the target material, the mobile fuel carrier, and the primary coolant to avoid the polonium production from bismuth. Reactor physics and thermal-hydraulic analyses were coupled to determine the parameters of the heterogeneous fission blanket. The engineering requirements for a satisfactory operation performance of the HT-9 ferritic steel structure material have been realized. Two heterogeneous concepts of the subcritical fission blanket with the liquid lead mobile fuel inside or outside the tube bundles were considered. The heterogeneous configuration with the mobile fuel inside the tubes showed better performance than the configuration with mobile fuel outside the bundle tubes. The Monte Carlo burnup codes, MCB5 and SERPENT were both used to simulate the fuel burnup in the ADS concepts with the mobile fuels inside the tubes. The burnup analyses were carried out for 35 full power years. The results show that 5 ADS systems can dispose of the total United States inventory of the spent nuclear fuel.« less

LLNL SFA OBER SBR FY17 Program Management and Performance Report: Subsurface Biogeochemistry of Actinides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kersting, Annie B.

A major scientific challenge in environmental sciences is to identify the dominant processes controlling actinide transport in the environment. It is estimated that currently, over 2200 metric tons of anthropogenic plutonium (Pu) has accumulated worldwide, a number that increases yearly with additional spent nuclear fuel (Ewing et al., 2010). Plutonium has been shown to migrate on the scale of kilometers, giving way to a critical concern that the fundamental biogeochemical processes that control its behavior in the subsurface are not well understood (Kersting et al. 1999; Novikov et al. 2006; Santschi et al. 2002). Neptunium (Np) is less prevalent inmore » the environment; however, it is predicted to be a significant long-term dose contributor in high-level nuclear waste. Our focus on Np chemistry in this Science Plan is intended to help formulate a better understanding of Pu redox transformations in the environment and clarify the differences between the two long-lived actinides. The research approach of our Science Plan combines (1) Fundamental Mechanistic Studies that identify and quantify biogeochemical processes that control actinide behavior in solution and on solids, (2) Field Integration Studies that investigate the transport characteristics of Pu and test our conceptual understanding of actinide transport, and (3) Actinide Research Capabilities that allow us to achieve the objectives of this Scientific Focus Area (SFA) and provide new opportunities for advancing actinide environmental chemistry. These three Research Thrusts form the basis of our SFA Science Program.« less

Supercritical Fluid Extraction and Separation of Uranium from Other Actinides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Donna L. Quach; Bruce J. Mincher; Chien M. Wai

2014-06-01

This paper investigates the feasibility of separating uranium from other actinides by using supercritical fluid carbon dioxide (sc-CO2) as a solvent modified with tri-n-butylphosphate (TBP) for the development of an extraction and counter current stripping technique, which would be a more efficient and environmentally benign technology for used nuclear fuel reprocessing compared to traditional solvent extraction. Several actinides (U(VI), Np(VI), Pu(IV), and Am(III)) were extracted in sc-CO2 modified with TBP over a range of nitric acid concentrations and then the actinides were exposed to reducing and complexing agents to suppress their extractability. According to this study, the separation of uraniummore » from plutonium in sc-CO2 modified with TBP was successful at nitric acid concentrations of less than 3 M in the presence of acetohydroxamic acid or oxalic acid, and the separation of uranium from neptunium was successful at nitric acid concentrations of less than 1 M in the presence of acetohydroxamic acid, oxalic acid, or sodium nitrite.« less

Actinide Sputtering Induced by Fission with Ultra-cold Neutrons

NASA Astrophysics Data System (ADS)

Venuti, Michael; Shi, Tan; Fellers, Deion; Morris, Christopher; Makela, Mark

2017-09-01

Understanding the effects of actinide sputtering due to nuclear fission is important for a wide range of applications, including nuclear fuel storage, space science, and national defense. A new program at the Los Alamos Neutron Science Center uses ultracold neutrons (UCN) to induce fission in actinides such as uranium and plutonium. By controlling the energy of UCN, it is possible to induce fission at the sample surface within a well-defined depth. It is therefore an ideal tool for studying the effects of fission-induced sputtering as a function of interaction depth. Since the mechanism for fission-induced surface damage is not well understood, especially for samples with a surface oxide layer, this work has the potential to separate the various damage mechanisms proposed in previous works. During the irradiation with UCN, fission events are monitored by coincidence counting between prompt gamma rays using NaI detectors. Alpha spectroscopy of the ejected actinide material is performed in a custom-built ionization chamber to determine the amount of sputtered material. Actinide samples with various sample properties and surface conditions are irradiated and analyzed. In this presentation, we will discuss our experimental setup and present the preliminary results.

A Novel Fuel/Reactor Cycle to Implement the 300 Years Nuclear Waste Policy Approach - 12377

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carelli, M.D.; Franceschini, F.; Lahoda, E.J.

2012-07-01

A thorium-based fuel cycle system can effectively burn the currently accumulated commercial used nuclear fuel and move to a sustainable equilibrium where the actinide levels in the high level waste are low enough to yield a radiotoxicity after 300 years lower than that of the equivalent uranium ore. The second step of the Westinghouse approach to solving the waste 'problem' has been completed. The thorium fuel cycle has indeed the potential of burning the legacy TRU and achieve the waste objective proposed. Initial evaluations have been started for the third step, development and selection of appropriate reactors. Indications are thatmore » the probability of show-stoppers is rather remote. It is, therefore, believed that development of the thorium cycle and associated technologies will provide a permanent solution to the waste management. Westinghouse is open to the widest collaboration to make this a reality. (authors)« less

Process for recovering actinide values

DOEpatents

Horwitz, E. Philip; Mason, George W.

1980-01-01

A process for rendering actinide values recoverable from sodium carbonate scrub waste solutions containing these and other values along with organic compounds resulting from the radiolytic and hydrolytic degradation of neutral organophosphorous extractants such as tri-n butyl phosphate (TBP) and dihexyl-N,N-diethyl carbamylmethylene phosphonate (DHDECAMP) which have been used in the reprocessing of irradiated nuclear reactor fuels. The scrub waste solution is preferably made acidic with mineral acid, to form a feed solution which is then contacted with a water-immiscible, highly polar organic extractant which selectively extracts the degradation products from the feed solution. The feed solution can then be processed to recover the actinides for storage or recycled back into the high-level waste process stream. The extractant is recycled after stripping the degradation products with a neutral sodium carbonate solution.

Modelling the behaviour of oxide fuels containing minor actinides with urania, thoria and zirconia matrices in an accelerator-driven system

NASA Astrophysics Data System (ADS)

Sobolev, V.; Lemehov, S.; Messaoudi, N.; Van Uffelen, P.; Aı̈t Abderrahim, H.

2003-06-01

The Belgian Nuclear Research Centre, SCK • CEN, is currently working on the pre-design of the multipurpose accelerator-driven system (ADS) MYRRHA. A demonstration of the possibility of transmutation of minor actinides and long-lived fission products with a realistic design of experimental fuel targets and prognosis of their behaviour under typical ADS conditions is an important task in the MYRRHA project. In the present article, the irradiation behaviour of three different oxide fuel mixtures, containing americium and plutonium - (Am,Pu,U)O 2- x with urania matrix, (Am,Pu,Th)O 2- x with thoria matrix and (Am,Y,Pu,Zr)O 2- x with inert zirconia matrix stabilised by yttria - were simulated with the new fuel performance code MACROS, which is under development and testing at the SCK • CEN. All the fuel rods were considered to be of the same design and sizes: annular fuel pellets, helium bounded with the stainless steel cladding, and a large gas plenum. The liquid lead-bismuth eutectic was used as coolant. Typical irradiation conditions of the hottest fuel assembly of the MYRRHA subcritical core were pre-calculated with the MCNPX code and used in the following calculations as the input data. The results of prediction of the thermo-mechanical behaviour of the designed rods with the considered fuels during three irradiation cycles of 90 EFPD are presented and discussed.

Accelerator-driven Transmutation of Waste

NASA Astrophysics Data System (ADS)

Venneri, Francesco

1998-04-01

Nuclear waste from commercial power plants contains large quantities of plutonium, other fissionable actinides, and long-lived fission products that are potential proliferation concerns and create challenges for the long-term storage. Different strategies for dealing with nuclear waste are being followed by various countries because of their geologic situations and their views on nuclear energy, reprocessing and non-proliferation. The current United States policy is to store unprocessed spent reactor fuel in a geologic repository. Other countries are opting for treatment of nuclear waste, including partial utilization of the fissile material contained in the spent fuel, prior to geologic storage. Long-term uncertainties are hampering the acceptability and eventual licensing of a geologic repository for nuclear spent fuel in the US, and driving up its cost. The greatest concerns are with the potential for radiation release and exposure from the spent fuel for tens of thousands of years and the possible diversion and use of the actinides contained in the waste for weapons construction. Taking advantage of the recent breakthroughs in accelerator technology and of the natural flexibility of subcritical systems, the Accelerator-driven Transmutation of Waste (ATW) concept offers the United States and other countries the possibility to greatly reduce plutonium, higher actinides and environmentally hazardous fission products from the waste stream destined for permanent storage. ATW does not eliminate the need for, but instead enhances the viability of permanent waste repositories. Far from being limited to waste destruction, the ATW concept also brings to the table new technologies that could be relevant for next-generation power producing reactors. In the ATW concept, spent fuel would be shipped to the ATW site where the plutonium, transuranics and selected long-lived fission products would be destroyed by fission or transmutation in their first and only pass through the facility, using an accelerator-driven subcritical burner cooled by liquid lead/bismuth and limited pyrochemical treatment of the spent fuel and residual waste. This approach contrasts with the present-day practices of aqueous reprocessing (Europe and Japan), in which high purity plutonium is produced and used in the fabrication of fresh mixed oxide fuel (MOX) that is shipped off-site for use in light water reactors.

Assessment of a French scenario with the INPRO methodology

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vasile, A.; Fiorini, G.L.; Cazalet, J.

2006-07-01

This paper presents the French contribution to the Joint Study of the IAEA International Project on Innovative Nuclear Reactors and Fuel Cycles (INPRO). It concerns the application of the INPRO methodology to a French scenario, on the transition from present LWRs to EPRs in a first phase and to 4. generation fast reactors in a second phase during the 21. century. The scenario also considers the renewal of the present fuel cycle facilities by the third and the fourth generation ones. Present practice of plutonium recycling in PWR is replaced by the middle of the century by a global recyclingmore » of actinides, uranium, plutonium and minor actinides in fast reactors. The status and the evolution of the INPRO criteria and the corresponding indicators during the studied period are analyzed for each of the six considered areas: economics, safety, environment, waste management, proliferation resistance and infrastructure. Improvements on economic and safety are expected for both the EPR and the 4. generation systems having these improvements among their basic goals. The use of fast reactors and global recycling of actinides leads to a significant improvement on environment indicators and in particular on the natural resources utilization. The envisaged waste management policy results in significant reductions on mass, thermal loads and radiotoxicity of the final waste which only contains fission products. The use of fuels that do not relay on enriched uranium and separated plutonium increases the proliferation resistance characteristics of the future fuel cycle. The paper summarizes also some recommendations on the data, codes and methods used to support the continuous improvement of the INPRO methodology and help future assessors. (authors)« less

Safeguard monitoring of direct electrolytic reduction

NASA Astrophysics Data System (ADS)

Jurovitzki, Abraham L.

Nuclear power is regaining global prominence as a sustainable energy source as the world faces the consequences of depending on limited fossil based, CO2 emitting fuels. A key component to achieving this sustainability is to implement a closed nuclear fuel cycle. Without achieving this goal, a relatively small fraction of the energy value in nuclear fuel is actually utilized. This involves recycling of spent nuclear fuel (SNF)---separating fissile actinides from waste products and using them to fabricate fresh fuel. Pyroprocessing is a viable option being developed for this purpose with a host of benefits compared to other recycling options, such as PUREX. Notably, pyroprocessing is ill suited to separate pure plutonium from spent fuel and thus has non-proliferation benefits. Pyroprocessing involves high temperature electrochemical and chemical processing of SNF in a molten salt electrolyte. During this batch process, several intermediate and final streams are produced that contain radioactive material. While pyroprocessing is ineffective at separating pure plutonium, there are various process misuse scenarios that could result in diversion of impure plutonium into one or more of these streams. This is a proliferation risk that should be addressed with innovative safeguards technology. One approach to meeting this challenge is to develop real time monitoring techniques that can be implemented in the hot cells and coupled with the various unit operations involved with pyroprocessing. Current state of the art monitoring techniques involve external chemical assaying which requires sample removal from these unit operations. These methods do not meet International Atomic Energy Agency's (IAEA) timeliness requirements. In this work, a number of monitoring techniques were assessed for their viability as online monitoring tools. A hypothetical diversion scenario for the direct electrolytic reduction process was experimentally verified (using Nd2O3 as a surrogate for PuO2). Electrochemical analysis was demonstrated to be effective at detecting even very dilute concentrations of actinides as evidence for a diversion attempt.

AN EVALUATION OF POTENTIAL LINER MATERIALS FOR ELIMINATING FCCI IN IRRADIATED METALLIC NUCLEAR FUEL ELEMENTS

DOE Office of Scientific and Technical Information (OSTI.GOV)

D. D. Keiser; J. I. Cole

2007-09-01

Metallic nuclear fuels are being looked at as part of the Global Nuclear Energy Program for transmuting longlive transuranic actinide isotopes contained in spent nuclear fuel into shorter-lived fission products. In order to optimize the performance of these fuels, the concept of using liners to eliminate the fuel/cladding chemical interactions that can occur during irradiation of a fuel element has been investigated. The potential liner materials Zr and V have been tested using solid-solid diffusion couples, consisting of liner materials butted against fuel alloys and against cladding materials. The couples were annealed at the relatively high temperature of 700°C. Thismore » temperature would be the absolute maximum temperature present at the fuel/cladding interface for a fuel element in-reactor. Analysis was performed using a scanning electron microscope equipped with energy-dispersive and wavelengthdispersive spectrometers (SEM/EDS/WDS) to evaluate any developed diffusion structures. At 700°C, minimal interaction was observed between the metallic fuels and either Zr or V. Similarly, limited interaction was observed between the Zr and V and the cladding materials. The best performing liner material appeared to be the V, based on amounts of interaction.« less

Phytosiderophore effects on subsurface actinide contaminants: potential for phytostabilization and phytoextraction.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ruggiero, C. E.; Twary, S. N.; Deladurantaye, E.

2003-01-01

In recognition of the need for a safe, effective technology for long term Pu/Th/Actinide stabilization or removal from soils, we have begun an investigation of the potential for phytoremediation (phytostabilization and/or phytoextraction) of Pu and other actinide soil contaminants at DOE sites using phytosiderophore producing plants, and are investigating the contribution of phytosiderophores to actinide mobility in the subsurface environment. Phytoremediation and Phytostabilization have been proven to be a cost-effective, safe, efficient, and publicly acceptable technology for clean up and/or stabilization of contaminant metals . However, no phyto-based technologies have been developed for stabilization or removal of plutonium from soilsmore » and groundwater, and very few have been investigated for other actinides . Current metal-phytostabilization and phytoremediation techniques, predominately based around lead, nickel, and other soft-metal phytoextraction, will almost certainly be inadequate for plutonium due its distinct chemical properties . Phytosiderophore-based phytoremediation may provide technically and financially practical methods for remediation and long-term stewardship of soils that have low to moderate, near surface actinide contamination . We plan to demonstrate potential benefits of phytosiderophore-producing plants for long-term actinide contaminant stabilization by the plant's prevention of soil erosion and actinide migration through hydraulic control and/or through actinide removal through phytoextraction . We may also show possible harm caused by these plants through increased presence of actinide chelators that could increase actinide mobilization and migration in the subsurface environment. This information can then be directly applied by either removal of harmful plants, or be used to develop plant-based soil stabilization/remediation technologies .« less

The prospect of uranium nitride (UN) and mixed nitride fuel (UN-PuN) for pressurized water reactor

NASA Astrophysics Data System (ADS)

Syarifah, Ratna Dewi; Suud, Zaki

2015-09-01

Design study of small Pressurized Water Reactors (PWRs) core loaded with uranium nitride fuel (UN) and mixed nitride fuel (UN-PuN), Pa-231 as burnable poison, and Americium has been performed. Pa-231 known as actinide material, have large capture cross section and can be converted into fissile material that can be utilized to reduce excess reactivity. Americium is one of minor actinides with long half life. The objective of adding americium is to decrease nuclear spent fuel in the world. The neutronic analysis results show that mixed nitride fuel have k-inf greater than uranium nitride fuel. It is caused by the addition of Pu-239 in mixed nitride fuel. In fuel fraction analysis, for uranium nitride fuel, the optimum volume fractions are 45% fuel fraction, 10% cladding and 45% moderator. In case of UN-PuN fuel, the optimum volume fractions are 30% fuel fraction, 10% cladding and 60% coolant/ moderator. The addition of Pa-231 as burnable poison for UN fuel, enrichment U-235 5%, with Pa-231 1.6% has k-inf more than one and excess reactivity of 14.45%. And for mixed nitride fuel, the lowest value of reactivity swing is when enrichment (U-235+Pu) 8% with Pa-231 0.4%, the excess reactivity value 13,76%. The fuel pin analyze for the addition of Americium, the excess reactivity value is lower than before, because Americium absorb the neutron. For UN fuel, enrichment U-235 8%, Pa-231 1.6% and Am 0.5%, the excess reactivity is 4.86%. And for mixed nitride fuel, when enrichment (U-235+Pu) 13%, Pa-231 0.4% and Am 0.1%, the excess reactivity is 11.94%. For core configuration, it is better to use heterogeneous than homogeneous core configuration, because the radial power distribution is better.

Status of advanced fuel candidates for Sodium Fast Reactor within the Generation IV International Forum

DOE Office of Scientific and Technical Information (OSTI.GOV)

F. Delage; J. Carmack; C. B. Lee

2013-10-01

The main challenge for fuels for future Sodium Fast Reactor systems is the development and qualification of a nuclear fuel sub-assembly which meets the Generation IV International Forum goals. The Advanced Fuel project investigates high burn-up minor actinide bearing fuels as well as claddings and wrappers to withstand high neutron doses and temperatures. The R&D outcome of national and collaborative programs has been collected and shared between the AF project members in order to review the capability of sub-assembly material and fuel candidates, to identify the issues and select the viable options. Based on historical experience and knowledge, both oxidemore » and metal fuels emerge as primary options to meet the performance and the reliability goals of Generation IV SFR systems. There is a significant positive experience on carbide fuels but major issues remain to be overcome: strong in-pile swelling, atmosphere required for fabrication as well as Pu and Am losses. The irradiation performance database for nitride fuels is limited with longer term R&D activities still required. The promising core material candidates are Ferritic/Martensitic (F/M) and Oxide Dispersed Strengthened (ODS) steels.« less

Natural Transmutation of Actinides via the Fission Reaction in the Closed Thorium-Uranium-Plutonium Fuel Cycle

NASA Astrophysics Data System (ADS)

Marshalkin, V. Ye.; Povyshev, V. M.

2017-12-01

It is shown for a closed thorium-uranium-plutonium fuel cycle that, upon processing of one metric ton of irradiated fuel after each four-year campaign, the radioactive wastes contain 54 kg of fission products, 0.8 kg of thorium, 0.10 kg of uranium isotopes, 0.005 kg of plutonium isotopes, 0.002 kg of neptunium, and "trace" amounts of americium and curium isotopes. This qualitatively simplifies the handling of high-level wastes in nuclear power engineering.

Initial results of metal waste form development activities at ANL-West

DOE Office of Scientific and Technical Information (OSTI.GOV)

Keiser, D.D. Jr.; Westphal, B.R.; Hersbt, R.S.

1997-10-01

Argonne National Laboratory is developing a metal alloy to contain metallic waste constituents from the electrometallurgical treatment of spent nuclear fuel. This alloy will contain stainless steel (from stainless steel-clad fuel elements), {approximately}15 wt.% zirconium (from alloy fuel), fission products noble to the process (e.g., Ru, Pd, Tc, etc.), and minor amounts of actinides. The alloy will serve as a final waste form for these components and will be disposed of in a geologic repository. The alloy ingot is produced in an induction furnace situated in a hot cell using Ar cover gas. This paper discusses results from the meltingmore » campaigns that have been initiated at ANL-West to generate the metal waste form using actual process materials. In addition, metal waste form samples have been doped with Tc and selected actinides and are described in the context of how elements of interest partition between various phases in the alloy and how this distribution of elements in the alloy may affect the leaching behavior of the components in an aqueous environment. 3 refs.« less

Initial results of metal waste-form development activities at ANL-West

DOE Office of Scientific and Technical Information (OSTI.GOV)

Keiser, D.D. Jr.; Westphal, B.R.; Herbst, R.S.

1997-12-01

Argonne National Laboratory (ANL) is developing a metal alloy to contain metallic waste constituent residual from the electrometallurgical treatment of spent nuclear fuel. This alloy will contain stainless steel (from stainless steel-clad fuel elements), {approximately} 15 wt% zirconium (from alloy fuel), fission products noble to the process (e.g., ruthenium, palladium, technetium, etc.), and minor amounts of actinides. The alloy will serve as a final waste form for these components and will be disposed of in a geologic repository. The alloy ingot is produced in an induction furnace situated in a hot cell using argon cover gas. This paper discusses resultsmore » from the melting campaigns that have been initiated at ANL-West to generate the metal waste form using actual process materials. In addition, metal waste form samples have been doped with technetium and selected actinides and are described in the context of how elements of interest partition between various phases in the alloy and how this distribution of elements in the alloy may affect the leaching behavior of the components in an aqueous environment.« less

Status of the Neutron Capture Measurement on 237Np with the DANCE Array at LANSCE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Esch, E.-I.; Bond, E.M.; Bredeweg, T. A.

2005-05-24

Neptunium-237 is a major constituent of spent nuclear fuel. Estimates place the amount of 237Np bound for the Yucca Mountain high-level waste repository at 40 metric tons. The Department of Energy's Advanced Fuel Cycle Initiative program is evaluating methods for transmuting the actinide waste that will be generated by future operation of commercial nuclear power plants. The critical parameter that defines the transmutation efficiency of actinide isotopes is the neutron fission-to-capture ratio for the particular isotope in a given neutron spectrum. The calculation of transmutation efficiency therefore requires accurate fission and capture cross sections. Current 237Np evaluations available for transmutermore » system studies show significant discrepancies in both the fission and capture cross sections in the energy regions of interest. Herein we report on 237Np (n,{gamma}) measurements using the recently commissioned DANCE array.« less

Actinide Sputtering Induced by Fission with Ultra-cold Neutrons

NASA Astrophysics Data System (ADS)

Shi, Tan; Venuti, Michael; Fellers, Deion; Martin, Sean; Morris, Chris; Makela, Mark

2017-09-01

Understanding the effects of actinide sputtering due to nuclear fission is important for a wide range of applications, including nuclear fuel storage, space science, and national defense. A new program at the Los Alamos Neutron Science Center uses ultracold neutrons (UCN) to induce fission in actinides such as uranium and plutonium. By controlling the UCN energy, it is possible to induce fission at the sample surface within a well-defined depth. It is therefore an ideal tool for studying the effects of fission-induced sputtering as a function of interaction depth. Since the mechanism for fission-induced surface damage is not well understood, this work has the potential to deconvolve the various damage mechanisms. During the irradiation with UCN, NaI detectors are used to monitor the fission events and were calibrated by monitoring fission fragments with an organic scintillator. Alpha spectroscopy of the ejected actinide material is performed in an ion chamber to determine the amount of sputtered material. Actinide samples with various sample properties and surface conditions are irradiated and analyzed. In this talk, I will discuss our experimental setup and present the preliminary results from the testing of multiple samples. This work has been supported by Los Alamos National Laboratory and Seaborg Summer Research Fellowship.

SiC Schottky Diode Detectors for Measurement of Actinide Concentrations from Alpha Activities in Molten Salt Electrolyte

DOE Office of Scientific and Technical Information (OSTI.GOV)

Windl, Wolfgang; Blue, Thomas

In this project, we have designed a 4H-SiC Schottky diode detector device in order to monitor actinide concentrations in extreme environments, such as present in pyroprocessing of spent fuel. For the first time, we have demonstrated high temperature operation of such a device up to 500 °C in successfully detecting alpha particles. We have used Am-241 as an alpha source for our laboratory experiments. Along with the experiments, we have developed a multiscale model to study the phenomena controlling the device behavior and to be able to predict the device performance. Our multiscale model consists of ab initio modeling tomore » understand defect energetics and their effect on electronic structure and carrier mobility in the material. Further, we have developed the basis for a damage evolution model incorporating the outputs from ab initio model in order to predict respective defect concentrations in the device material. Finally, a fully equipped TCAD-based device model has been developed to study the phenomena controlling the device behavior. Using this model, we have proven our concept that the detector is capable of performing alpha detection in a salt bath with the mixtures of actinides present in a pyroprocessing environment.« less

Transuranic Waste Burning Potential of Thorium Fuel in a Fast Reactor - 12423

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wenner, Michael; Franceschini, Fausto; Ferroni, Paolo

Westinghouse Electric Company (referred to as 'Westinghouse' in the rest of this paper) is proposing a 'back-to-front' approach to overcome the stalemate on nuclear waste management in the US. In this approach, requirements to further the societal acceptance of nuclear waste are such that the ultimate health hazard resulting from the waste package is 'as low as reasonably achievable'. Societal acceptability of nuclear waste can be enhanced by reducing the long-term radiotoxicity of the waste, which is currently driven primarily by the protracted radiotoxicity of the transuranic (TRU) isotopes. Therefore, a transition to a more benign radioactive waste can bemore » accomplished by a fuel cycle capable of consuming the stockpile of TRU 'legacy' waste contained in the LWR Used Nuclear Fuel (UNF) while generating waste which is significantly less radio-toxic than that produced by the current open U-based fuel cycle (once through and variations thereof). Investigation of a fast reactor (FR) operating on a thorium-based fuel cycle, as opposed to the traditional uranium-based is performed. Due to a combination between its neutronic properties and its low position in the actinide chain, thorium not only burns the legacy TRU waste, but it does so with a minimal production of 'new' TRUs. The effectiveness of a thorium-based fast reactor to burn legacy TRU and its flexibility to incorporate various fuels and recycle schemes according to the evolving needs of the transmutation scenario have been investigated. Specifically, the potential for a high TRU burning rate, high U-233 generation rate if so desired and low concurrent production of TRU have been used as metrics for the examined cycles. Core physics simulations of a fast reactor core running on thorium-based fuels and burning an external TRU feed supply have been carried out over multiple cycles of irradiation, separation and reprocessing. The TRU burning capability as well as the core isotopic content have been characterized. Results will be presented showing the potential for thorium to reach a high TRU transmutation rate over a wide variety of fuel types (oxide, metal, nitride and carbide) and transmutation schemes (recycle or partition of in-bred U-233). In addition, a sustainable scheme has been devised to burn the TRU accumulated in the core inventory once the legacy TRU supply has been exhausted, thereby achieving long-term virtually TRU-free. A comprehensive 'back-to-front' approach to the fuel cycle has recently been proposed by Westinghouse which emphasizes achieving 'acceptable', low-radiotoxicity, high-level waste, with the intent not only to satisfy all technical constraints but also to improve public acceptance of nuclear energy. Following this approach, the thorium fuel cycle, due to its low radiotoxicity and high potential for TRU transmutation has been selected as a promising solution. Additional studies not shown here have shown significant reduction of decay heat. The TRU burning potential of the Th-based fuel cycle has been illustrated with a variety of fuel types, using the Toshiba ARR to perform the analysis, including scenarios with continued LWR operation of either uranium fueled or thorium fueled LWRs. These scenarios will afford overall reduction in actinide radiotoxicity, however when the TRU supply is exhausted, a continued U- 235 LWR operation must be assumed to provide TRU makeup feed. This scenario will never reach the characteristically low TRU content of a closed thorium fuel cycle with its associated potential benefits on waste radiotoxicity, as exemplified by the transition scenario studied. At present, the cases studied indicate ThC as a potential fuel for maximizing TRU burning, while ThN with nitrogen enriched to 95% N-15 shows the highest breeding potential. As a result, a transition scenario with ThN was developed to show that a sustainable, closed Th-cycle can be achieved starting from burning the legacy TRU stock and completing the transmutation of the residual TRU remaining in the core inventory after the legacy TRU external supply has been exhausted. The radiotoxicity of the actinide waste during the various phases has been characterized, showing the beneficial effect of the decreasing content of TRU in the recycled fuel as the transition to a closed Th-based fuel cycle is undertaken. Due to the back-to-front nature of the proposed methodology, detailed designs are not the first step taken when assessing a fuel cycle scenario potential. As a result, design refinement is still required and should be expected in future studies. Moreover, significant safety assessment, including determination of associated reactivity coefficients, fuel and reprocessing feasibility studies and economic assessments will still be needed for a more comprehensive and meaningful comparison against other potential solutions. With the above considerations in mind, the potential advantages of thorium fuelled reactors on HLW management optimization lead us to believe that thorium fuelled reactor systems can play a significant role in the future and deserve further consideration. (authors)« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kersting, Annie B.; Zavarin, Mavrik

A major scientific challenge in environmental sciences is to identify the dominant processes controlling actinide transport in the environment. It is estimated that currently, over 2200 metric tons of plutonium (Pu) have been deposited in the subsurface worldwide, a number that increases yearly with additional spent nuclear fuel (Ewing et al., 2010). Plutonium has been shown to migrate on the scale of kilometers, giving way to a critical concern that the fundamental biogeochemical processes that control its behavior in the subsurface are not well understood (Kersting et al., 1999; Novikov et al., 2006; Santschi et al., 2002). Neptunium (Np) ismore » less prevalent in the environment; however, it is predicted to be a significant long-term dose contributor in high-level nuclear waste. Our focus on Np chemistry in this Science Plan is intended to help formulate a better understanding of Pu redox transformations in the environment and clarify the differences between the two long-lived actinides. The research approach of our Science Plan combines (1) Fundamental Mechanistic Studies that identify and quantify biogeochemical processes that control actinide behavior in solution and on solids, (2) Field Integration Studies that investigate the transport characteristics of Pu and test our conceptual understanding of actinide transport, and (3) Actinide Research Capabilities that allow us to achieve the objectives of this Scientific Focus Area (SFA and provide new opportunities for advancing actinide environmental chemistry. These three Research Thrusts form the basis of our SFA Science Program (Figure 1).« less

The behavior and importance of lactic acid complexation in Talspeak extraction systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grimes, Travis S.; Nilsson, Mikael; Nash, Kenneth L.

2008-07-01

Advanced partitioning of spent nuclear fuel in the UREX +la process relies on the TALSPEAK process for separation of fission-product lanthanides from trivalent actinides. The classic TALSPEAK utilizes an aqueous medium of both lactic acid and diethylenetriaminepentaacetic acid and the extraction reagent di(2-ethylhexyl)phosphoric acid in an aromatic diluent. In this study, the specific role of lactic acid and the complexes involved in the extraction of the trivalent actinides and lanthanides have been investigated using {sup 14}C-labeled lactic acid. Our results show that lactic acid partitions between the phases in a complex fashion. (authors)

Process to remove rare earth from IFR electrolyte

DOEpatents

Ackerman, John P.; Johnson, Terry R.

1994-01-01

The invention is a process for the removal of rare earths from molten chloride electrolyte salts used in the reprocessing of integrated fast reactor fuel (IFR). The process can be used either continuously during normal operation of the electrorefiner or as a batch process. The process consists of first separating the actinide values from the salt before purification by removal of the rare earths. After replacement of the actinides removed in the first step, the now-purified salt electrolyte has the same uranium and plutonium concentration and ratio as when the salt was removed from the electrorefiner.

Process to remove rare earth from IFR electrolyte

DOEpatents

Ackerman, J.P.; Johnson, T.R.

1992-01-01

The invention is a process for the removal of rare earths from molten chloride electrolyte salts used in the reprocessing of integrated fast reactor fuel (IFR). The process can be used either continuously during normal operation of the electrorefiner or as a batch process. The process consists of first separating the actinide values from the salt before purification by removal of the rare earths. After replacement of the actinides removed in the first step, the now-purified salt electrolyte has the same uranium and plutonium concentration and ratio as when the salt was removed from the electrorefiner.

Process to remove rare earth from IFR electrolyte

DOEpatents

Ackerman, J.P.; Johnson, T.R.

1994-08-09

The invention is a process for the removal of rare earths from molten chloride electrolyte salts used in the reprocessing of integrated fast reactor fuel (IFR). The process can be used either continuously during normal operation of the electrorefiner or as a batch process. The process consists of first separating the actinide values from the salt before purification by removal of the rare earths. After replacement of the actinides removed in the first step, the now-purified salt electrolyte has the same uranium and plutonium concentration and ratio as when the salt was removed from the electrorefiner. 1 fig.

Synthesis of actinide nitrides, phosphides, sulfides and oxides

DOEpatents

Van Der Sluys, William G.; Burns, Carol J.; Smith, David C.

1992-01-01

A process of preparing an actinide compound of the formula An.sub.x Z.sub.y wherein An is an actinide metal atom selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, x is selected from the group consisting of one, two or three, Z is a main group element atom selected from the group consisting of nitrogen, phosphorus, oxygen and sulfur and y is selected from the group consisting of one, two, three or four, by admixing an actinide organometallic precursor wherein said actinide is selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, a suitable solvent and a protic Lewis base selected from the group consisting of ammonia, phosphine, hydrogen sulfide and water, at temperatures and for time sufficient to form an intermediate actinide complex, heating said intermediate actinide complex at temperatures and for time sufficient to form the actinide compound, and a process of depositing a thin film of such an actinide compound, e.g., uranium mononitride, by subliming an actinide organometallic precursor, e.g., a uranium amide precursor, in the presence of an effectgive amount of a protic Lewis base, e.g., ammonia, within a reactor at temperatures and for time sufficient to form a thin film of the actinide compound, are disclosed.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sarta, Jose A.; Castiblanco, Luis A

With cooperation of the International Atomic Energy Agency (IAEA) and the Department of Energy (DOE) of the United States, several calculations and tasks related to the waste disposal of spent MTR fuel enriched nominally to 93% were carried out for the conversion of the IAN-R1 Research Reactor from MTR-HEU fuel to TRIGA-LEU fuel. In order to remove the spent MTR-HEU fuel of the core and store it safely a program was established at the Instituto de Ciencias Nucleares y Energias Alternativas (INEA). This program included training, acquisition of hardware and software, design and construction of a decay pool, transfer ofmore » the spent HEU fuel elements into the decay pool and his final transport to Savannah River in United States. In this paper are presented data of activities calculated for each relevant radionuclide present in spent MTR-HEU fuel elements of the IAN-R1 Research Reactor and the total activity. The total activity calculated takes in consideration contributions of fission, activation and actinides products. The data obtained were the base for shielding calculations for the decay pool concerning the storage of spent MTR-HEU fuel elements and the respective dosimetric evaluations in the transferring operations of fuel elements into the decay pool.« less

THE EFFECT OF IONIZING RADIATION ON U6+ -PHASES

DOE Office of Scientific and Technical Information (OSTI.GOV)

S. Utsunomiya; R.C. Ewing

2005-07-07

U{sup 6+}-minerals commonly form during the alteration of uraninite and spent nuclear fuel under oxidizing conditions. By the incorporation of actinides and fissiogenic elements into their structures, U{sup 6+}-minerals may be important in retarding the migration of radionuclides released during corrosion of spent nuclear fuel. Thus, the stability and the structural transformation of the U{sup 6+}-minerals in radiation fields are of great interest.

M3FT-15OR0202212: SUBMIT SUMMARY REPORT ON THERMODYNAMIC EXPERIMENT AND MODELING

DOE Office of Scientific and Technical Information (OSTI.GOV)

McMurray, Jake W.; Brese, Robert G.; Silva, Chinthaka M.

2015-09-01

Modeling the behavior of nuclear fuel with a physics-based approach uses thermodynamics for key inputs such as chemical potentials and thermal properties for phase transformation, microstructure evolution, and continuum transport simulations. Many of the lanthanide (Ln) elements and Y are high-yield fission products. The U-Y-O and U-Ln-O ternaries are therefore key subsystems of multi-component high-burnup fuel. These elements dissolve in the dominant urania fluorite phase affecting many of its properties. This work reports on an effort to assess the thermodynamics of the U-Pr-O and U-Y-O systems using the CALPHAD (CALculation of PHase Diagrams) method. The models developed within this frameworkmore » are capable of being combined and extended to include additional actinides and fission products allowing calculation of the phase equilibria, thermochemical and material properties of multicomponent fuel with burnup.« less

Fuel development for gas-cooled fast reactors

NASA Astrophysics Data System (ADS)

Meyer, M. K.; Fielding, R.; Gan, J.

2007-09-01

The Generation IV Gas-cooled Fast Reactor (GFR) concept is proposed to combine the advantages of high-temperature gas-cooled reactors (such as efficient direct conversion with a gas turbine and the potential for application of high-temperature process heat), with the sustainability advantages that are possible with a fast-spectrum reactor. The latter include the ability to fission all transuranics and the potential for breeding. The GFR is part of a consistent set of gas-cooled reactors that includes a medium-term Pebble Bed Modular Reactor (PBMR)-like concept, or concepts based on the Gas Turbine Modular Helium Reactor (GT-MHR), and specialized concepts such as the Very High-Temperature Reactor (VHTR), as well as actinide burning concepts [A Technology Roadmap for Generation IV Nuclear Energy Systems, US DOE Nuclear Energy Research Advisory Committee and the Generation IV International Forum, December 2002]. To achieve the necessary high power density and the ability to retain fission gas at high temperature, the primary fuel concept proposed for testing in the United States is dispersion coated fuel particles in a ceramic matrix. Alternative fuel concepts considered in the US and internationally include coated particle beds, ceramic clad fuel pins, and novel ceramic 'honeycomb' structures. Both mixed carbide and mixed nitride-based solid solutions are considered as fuel phases.

Nineteenth annual actinide separations conference: Conference program and abstracts

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bronson, M.

This report contains the abstracts from the conference presentations. Sessions were divided into the following topics: Waste treatment; Spent fuel treatment; Issues and responses to Defense Nuclear Facility Safety Board 94-1; Pyrochemical technologies; Disposition technologies; and Aqueous separation technologies.

Mass and abundance 236U sensitivities at CIRCE

NASA Astrophysics Data System (ADS)

De Cesare, M.; De Cesare, N.; D'Onofrio, A.; Fifield, L. K.; Gialanella, L.; Terrasi, F.

2015-10-01

The actinides (e.g. 236U and xPu isotopes) are present in environmental samples at the ultra trace level since atmospheric tests of NWs (Nuclear Weapons) performed in the past, deliberate dumping of nuclear waste, nuclear fuel reprocessing, on a large scale and operation of NPPs (Nuclear Power Plants) on a small scale have led to the release of a wide range of radioactive nuclides in the environment. Their detection requires the most sensitive AMS (Accelerator Mass Spectrometry) techniques and at the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy, an upgraded actinide AMS system, based on a 3-MV pelletron tandem accelerator, has been operated. In this paper the progress made in order to push the 236U mass sensitivity and 236U/238U isotopic ratio down to the natural levels is reported. A uranium contamination mass of about 0.05 μg and a 236U/238U isotopic ratio sensitivities at the level of 3.2 × 10-13 are presently achievable.

Estimating the time for dissolution of spent fuel exposed to unlimited water

DOE Office of Scientific and Technical Information (OSTI.GOV)

Leider, H.R.; Nguyen, S.N.; Stout, R.B.

1991-12-01

The release of radionuclides from spent fuel cannot be precisely predicted at this point because a satisfactory dissolution model based on specific chemical processes is not yet available. However, preliminary results on the dissolution rate of UO{sub 2} and spent fuel as a function of temperature and water composition have recently been reported. This information, together with data on fragment size distribution of spent fuel, are used to estimate the dissolution response of spent fuel in excess flowing water within the framework of a simple model. In this model, the reaction/dissolution front advances linearly with time and geometry is preserved.more » This also estimates the dissolution rate of the bulk of the fission products and higher actinides, which are uniformly distributed in the UO{sub 2} matrix and are presumed to dissolve congruently. We have used a fuel fragment distribution actually observed to calculate the time for total dissolution of spent fuel. A worst-case estimate was also made using the initial (maximum) rate of dissolution to predict the total dissolution time. The time for total dissolution of centimeter size particles is estimated to be 5.5 {times} 10{sup 4} years at 25{degrees}C.« less

Electron Correlation and Tranport Properties in Nuclear Fuel Materials

NASA Astrophysics Data System (ADS)

Yin, Quan; Haule, Kristjan; Kotliar, Gabriel; Savrasov, Sergey; Pickett, Warren

2011-03-01

Using first principle LDA+DMFT method, we conduct a systematic study on the correlated electronic structures and transport properties of select actinide carbides, nitrides, and oxides, many of which are nuclear fuel materials. Our results capture the metal--insulator Mott transition within the studied systems, and the appearance of the Zhang-Rice state in uranium dioxide. More importantly, by understanding the physics underlying their transport properties, we suggest ways to improve the efficiency of currently used fuels. This work is supported by the DOE Nuclear Energy University Program, contract No. 00088708.

Development of a new casting method to fabricate U–Zr alloy containing minor actinides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jong Hwan Kim; Hoon Song; Hyung Tae Kim

2014-01-01

Metal fuel slugs of U–Zr alloys for a sodium-cooled fast reactor (SFR) have conventionally been fabricated using an injection casting method. However, casting alloys containing volatile radioactive constituents, such as Am, are problematic in a conventional injection casting method. As an alternative fabrication method, low pressure gravity casting has been developed. Casting soundness, microstructural characteristics, alloying composition, density, and fuel losses were evaluated for the following as-cast fuel slugs: U–10 wt% Zr, U–10 wt% Zr–5 wt% RE, and U–10 wt% Zr–5 wt% RE–5 wt% Mn. The U and Zr contents were uniform throughout the matrix, and impurities such as oxyen,more » carbon, and nitrogen satisfied the specification of total impurities less than 2,000 ppm. The appearance of the fuel slugs was generally sound, and the internal integrity was shown to be satisfactory based on gamma-ray radiography. In a volatile surrogate casting test, the U–Zr–RE–Mn fuel slug showed that nearly all of the manganese was retained when casting was done under an inert atmosphere.« less

Coordination characteristics of uranyl BBP complexes: Insights from an electronic structure analysis

DOE PAGES

Pemmaraju, Chaitanya Das; Copping, Roy; Smiles, Danil E.; ...

2017-03-21

Here, organic ligand complexes of lanthanide/actinide ions have been studied extensively for applications in nuclear fuel storage and recycling. Several complexes of 2,6-bis(2-benzimidazyl)pyridine (H2BBP) featuring the uranyl moiety have been reported recently, and the present study investigates the coordination characteristics of these complexes using density functional theory-based electronic structure analysis. In particular, with the aid of several computational models, the nonplanar equatorial coordination about uranyl, observed in some of the compounds, is studied and its origin traced to steric effects.

Communication—Quantitative Voltammetric Analysis of High Concentration Actinides in Molten Salts

DOE PAGES

Hoyt, Nathaniel C.; Willit, James L.; Williamson, Mark A.

2017-01-18

Previous electroanalytical studies have shown that cyclic voltammetry can provide accurate quantitative measurements of actinide concentrations at low weight loadings in molten salts. However, above 2 wt%, the techniques were found to underpredict the concentrations of the reactant species. Here this work will demonstrate that much of the discrepancy is caused by uncompensated resistance and cylindrical diffusion. An improved electroanalytical approach has therefore been developed using the results of digital simulations to take these effects into account. This approach allows for accurate electroanalytical predictions across the full range of weight loadings expected to be encountered in operational nuclear fuel processingmore » equipment.« less

Communication—Quantitative Voltammetric Analysis of High Concentration Actinides in Molten Salts

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hoyt, Nathaniel C.; Willit, James L.; Williamson, Mark A.

Previous electroanalytical studies have shown that cyclic voltammetry can provide accurate quantitative measurements of actinide concentrations at low weight loadings in molten salts. However, above 2 wt%, the techniques were found to underpredict the concentrations of the reactant species. Here this work will demonstrate that much of the discrepancy is caused by uncompensated resistance and cylindrical diffusion. An improved electroanalytical approach has therefore been developed using the results of digital simulations to take these effects into account. This approach allows for accurate electroanalytical predictions across the full range of weight loadings expected to be encountered in operational nuclear fuel processingmore » equipment.« less

Voltammetry Method Evaluation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hoyt, N.; Pereira, C.; Willit, J.

2016-07-29

The purpose of the ANL MPACT Voltammetry project is to evaluate the suitability of previously developed cyclic voltammetry techniques to provide electroanalytical measurements of actinide concentrations in realistic used fuel processing scenarios. The molten salts in these scenarios are very challenging as they include high concentrations of multiple electrochemically active species, thereby creating a variety of complications. Some of the problems that arise therein include issues related to uncompensated resistance, cylindrical diffusion, and alloying of the electrodeposited metals. Improvements to the existing voltammetry technique to account for these issues have been implemented, resulting in good measurements of actinide concentrations acrossmore » a wide range of adverse conditions.« less

ALD coating of nuclear fuel actinides materials

DOEpatents

Yacout, A. M.; Pellin, Michael J.; Yun, Di; Billone, Mike

2017-09-05

The invention provides a method of forming a nuclear fuel pellet of a uranium containing fuel alternative to UO.sub.2, with the steps of obtaining a fuel form in a powdered state; coating the fuel form in a powdered state with at least one layer of a material; and sintering the powdered fuel form into a fuel pellet. Also provided is a sintered nuclear fuel pellet of a uranium containing fuel alternative to UO.sub.2, wherein the pellet is made from particles of fuel, wherein the particles of fuel are particles of a uranium containing moiety, and wherein the fuel particles are coated with at least one layer between about 1 nm to about 4 nm thick of a material using atomic layer deposition, and wherein the at least one layer of the material substantially surrounds each interfacial grain barrier after the powdered fuel form has been sintered.

Organic and Aqueous Redox Speciation of Cu(III) Periodate Oxidized Transuranium Actinides

DOE Office of Scientific and Technical Information (OSTI.GOV)

McCann, Kevin; Sinkov, Sergey I.; Lumetta, Gregg J.

A hexavalent group actinide separation process could streamline used nuclear fuel recycle and waste management. The limiting factor to such a process compatible with current fuel dissolution practices is obtaining and maintaining hexavalent Am, in molar nitric acid due to the high reduction potential of the Am(VI)/Am(III) couple (1.68 V vs SCE). Two strong oxidants, sodium bismuthate and Cu(III) periodate, have demonstrated quantitative oxidation of Am under molar acid conditions and better than 50% recovery by diamyl amylphosphonate (DAAP) is possible under these same conditions. This work considers the use of Cu(III) periodate to oxidize Np(V) to Np(VI) and Pu(IV)more » to Pu(VI) and recover these elements by extraction with DAAP. A metal:oxidant ratio of 1:1.2 and 1:3 was necessary to quantitatively oxidize Np(V) and Pu(IV), respectively, to the hexavalent state. Extraction of hexavalent Np, Pu, and Am by 1 M DAAP in n-dodecane was measured using UV-Vis [Pu(VI), Am (VI)] and NIR [Np(VI)]. Distribution values of Am(VI) were found to match previous tracer level studies. The organic phase spectra of Np, Pu, and Am are presented and molar absorptivities are calculated for characteristic peaks. Hexavalent Pu was found to be stable in the organic phase while Np(VI) showed some reduction to Np(V) and Am was present as Am(III), Am(V), and Am(VI) species in aqueous and organic phases during the extraction experiments. These results demonstrate, for the first time, the ability to recover macroscopic amounts of americium that would be present during fuel reprocessing and are the first characterization of Am organic phase oxidation state speciation relevant to a hexavalent group actinide separation process under acidic conditions.« less

Approach for validating actinide and fission product compositions for burnup credit criticality safety analyses

DOE PAGES

Radulescu, Georgeta; Gauld, Ian C.; Ilas, Germina; ...

2014-11-01

This paper describes a depletion code validation approach for criticality safety analysis using burnup credit for actinide and fission product nuclides in spent nuclear fuel (SNF) compositions. The technical basis for determining the uncertainties in the calculated nuclide concentrations is comparison of calculations to available measurements obtained from destructive radiochemical assay of SNF samples. Probability distributions developed for the uncertainties in the calculated nuclide concentrations were applied to the SNF compositions of a criticality safety analysis model by the use of a Monte Carlo uncertainty sampling method to determine bias and bias uncertainty in effective neutron multiplication factor. Application ofmore » the Monte Carlo uncertainty sampling approach is demonstrated for representative criticality safety analysis models of pressurized water reactor spent fuel pool storage racks and transportation packages using burnup-dependent nuclide concentrations calculated with SCALE 6.1 and the ENDF/B-VII nuclear data. Furthermore, the validation approach and results support a recent revision of the U.S. Nuclear Regulatory Commission Interim Staff Guidance 8.« less

Closed Fuel Cycle Waste Treatment Strategy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vienna, J. D.; Collins, E. D.; Crum, J. V.

This study is aimed at evaluating the existing waste management approaches for nuclear fuel cycle facilities in comparison to the objectives of implementing an advanced fuel cycle in the U.S. under current legal, regulatory, and logistical constructs. The study begins with the Global Nuclear Energy Partnership (GNEP) Integrated Waste Management Strategy (IWMS) (Gombert et al. 2008) as a general strategy and associated Waste Treatment Baseline Study (WTBS) (Gombert et al. 2007). The tenets of the IWMS are equally valid to the current waste management study. However, the flowsheet details have changed significantly from those considered under GNEP. In addition, significantmore » additional waste management technology development has occurred since the GNEP waste management studies were performed. This study updates the information found in the WTBS, summarizes the results of more recent technology development efforts, and describes waste management approaches as they apply to a representative full recycle reprocessing flowsheet. Many of the waste management technologies discussed also apply to other potential flowsheets that involve reprocessing. These applications are occasionally discussed where the data are more readily available. The report summarizes the waste arising from aqueous reprocessing of a typical light-water reactor (LWR) fuel to separate actinides for use in fabricating metal sodium fast reactor (SFR) fuel and from electrochemical reprocessing of the metal SFR fuel to separate actinides for recycle back into the SFR in the form of metal fuel. The primary streams considered and the recommended waste forms include; Tritium in low-water cement in high integrity containers (HICs); Iodine-129: As a reference case, a glass composite material (GCM) formed by the encapsulation of the silver Mordenite (AgZ) getter material in a low-temperature glass is assumed. A number of alternatives with distinct advantages are also considered including a fused silica waste form with encapsulated nano-sized AgI crystals; Carbon-14 immobilized as a CaCO3 in a cement waste form; Krypton-85 stored as a compressed gas; An aqueous reprocessing high-level waste (HLW) raffinate waste immobilized by the vitrification process; An undissolved solids (UDS) fraction from aqueous reprocessing of LWR fuel either included in the borosilicate HLW glass or immobilized in the form of a metal alloy or titanate ceramics; Zirconium-based LWR fuel cladding hulls and stainless steel (SS) fuel assembly hardware super-compacted for disposal or purified for reuse (or disposal as low-level waste, LLW) of Zr by reactive gas separations; Electrochemical process salt HLW incorporated into a glass bonded Sodalite waste form; and Electrochemical process UDS and SS cladding hulls melted into an iron based alloy waste form. Mass and volume estimates for each of the recommended waste forms based on the source terms from a representative flowsheet are reported. In addition to the above listed primary waste streams, a range of secondary process wastes are generated by aqueous reprocessing of LWR fuel, metal SFR fuel fabrication, and electrochemical reprocessing of SFR fuel. These secondary wastes have been summarized and volumes estimated by type and classification. The important waste management data gaps and research needs have been summarized for each primary waste stream and selected waste process.« less

Pyroprocessing of Light Water Reactor Spent Fuels Based on an Electrochemical Reduction Technology

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ohta, Hirokazu; Inoue, Tadashi; Sakamura, Yoshiharu

A concept of pyroprocessing light water reactor (LWR) spent fuels based on an electrochemical reduction technology is proposed, and the material balance of the processing of mixed oxide (MOX) or high-burnup uranium oxide (UO{sub 2}) spent fuel is evaluated. Furthermore, a burnup analysis for metal fuel fast breeder reactors (FBRs) is conducted on low-decontamination materials recovered by pyroprocessing. In the case of processing MOX spent fuel (40 GWd/t), UO{sub 2} is separately collected for {approx}60 wt% of the spent fuel in advance of the electrochemical reduction step, and the product recovered through the rare earth (RE) removal step, which hasmore » the composition uranium:plutonium:minor actinides:fission products (FPs) = 76.4:18.4:1.7:3.5, can be applied as an ingredient of FBR metal fuel without a further decontamination process. On the other hand, the electroreduced alloy of high-burnup UO{sub 2} spent fuel (48 GWd/t) requires further decontamination of residual FPs by an additional process such as electrorefining even if RE FPs are removed from the alloy because the recovered plutonium (Pu) is accompanied by almost the same amount of FPs in addition to RE. However, the amount of treated materials in the electrorefining step is reduced to {approx}10 wt% of the total spent fuel owing to the prior UO{sub 2} recovery step. These results reveal that the application of electrochemical reduction technology to LWR spent oxide fuel is a promising concept for providing FBR metal fuel by a rationalized process.« less

Casting evaluation of U-Zr alloy system fuel slug for SFR prepared by injection casting method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Song, Hoon; Kim, Jong-Hwan; Kim, Ki-Hwan

2013-07-01

Metal fuel slugs of U-Pu-Zr alloys for Sodium-cooled Fast Reactor (SFR) have conventionally been fabricated by a vacuum injection casting method. Recently, management of minor actinides (MA) became an important issue because direct disposal of the long-lived MA can be a long-term burden for a tentative repository up to several hundreds of thousand years. In order to recycle transuranic elements (TRU) retained in spent nuclear fuel, remote fabrication capability in a shielded hot cell should be prepared. Moreover, generation of long-lived radioactive wastes and loss of volatile species should be minimized during the recycled fuel fabrication step. In order tomore » prevent the evaporation of volatile elements such as Am, alternative fabrication methods of metal fuel slugs have been studied applying gravity casting, and improved injection casting in KAERI, including melting under inert atmosphere. And then, metal fuel slugs were examined with casting soundness, density, chemical analysis, particle size distribution and microstructural characteristics. Based on these results there is a high level of confidence that Am losses will also be effectively controlled by application of a modest amount of overpressure. A surrogate fuel slug was generally soundly cast by improved injection casting method, melted fuel material under inert atmosphere.« less

Managing the Nuclear Fuel Cycle: Policy Implications of Expanding Global Access to Nuclear Power

DTIC Science & Technology

2010-03-05

However, the case of Iran raises perhaps the most critical question in this decade for strengthening the nuclear nonproliferation regime: How can...enrichment process can take advantage of the slight difference in atomic mass between 235U and 238U. The typical enrichment process requires about 10 lbs of...neutrons but can induce fission in all actinides , including all plutonium isotopes. Therefore, nuclear fuel for a fast reactor must have a higher

Candidate molten salt investigation for an accelerator driven subcritical core

NASA Astrophysics Data System (ADS)

Sooby, E.; Baty, A.; Beneš, O.; McIntyre, P.; Pogue, N.; Salanne, M.; Sattarov, A.

2013-09-01

We report a design for accelerator-driven subcritical fission in a molten salt core (ADSMS) that utilizes a fuel salt composed of NaCl and transuranic (TRU) chlorides. The ADSMS core is designed for fast neutronics (28% of neutrons >1 MeV) to optimize TRU destruction. The choice of a NaCl-based salt offers benefits for corrosion, operating temperature, and actinide solubility as compared with LiF-based fuel salts. A molecular dynamics (MD) code has been used to estimate properties of the molten salt system which are important for ADSMS design but have never been measured experimentally. Results from the MD studies are reported. Experimental measurements of fuel salt properties and studies of corrosion and radiation damage on candidate metals for the core vessel are anticipated. A special thanks is due to Prof. Paul Madden for introducing the ADSMS group to the concept of using the molten salt as the spallation target, rather than a conventional heavy metal spallation target. This feature helps to optimize this core as a Pu/TRU burner.

One-group fission cross sections for plutonium and minor actinides inserted in calculated neutron spectra of fast reactor cooled with lead-208 or lead-bismuth eutectic

DOE Office of Scientific and Technical Information (OSTI.GOV)

Khorasanov, G. L.; Blokhin, A. I.

The paper is dedicated to one-group fission cross sections of Pu and MA in LFRs spectra with the aim to increase these values by choosing a coolant which hardens neutron spectra. It is shown that replacement of coolant from Pb-Bi with Pb-208 in the fast reactor RBEC-M, designed in Russia, leads to increasing the core mean neutron energy. As concerns fuel Pu isotopes, their one-group fission cross sections become slightly changed, while more dramatically Am-241 one-group fission cross section is changed. Another situation occurs in the lateral blanket containing small quantities of minor actinides. It is shown that as amore » result of lateral blanket mean neutron energy hardening the one-group fission cross sections of Np-237, Am-241 and Am-243 increases up to 8-11%. This result allows reducing the time of minor actinides burning in FRs. (authors)« less

CY2013 Annual Report for DOE-ITU INERI 2010-006-E

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kennedy, J. Rory; Rondinella, Vincenzo V.

2014-12-01

New concepts for nuclear energy development are considered in both the USA and Europe within the framework of the Generation-IV International Forum (GIF) as well as in various US-DOE programs (e.g. the Fuel Cycle Research and Development - FCRD) and as part of the European Sustainable Nuclear Energy Technology Platform (SNE-TP). Since most new fuel cycle concepts envisage the adoption of a closed nuclear fuel cycle employing fast reactors, the fuel behavior characteristics of the various proposed advanced fuel forms must be effectively investigated using state of the art experimental techniques before implementation. More rapid progress can be achieved ifmore » effective synergy with advanced (multi-scale) modeling efforts can be achieved. The fuel systems to be considered include minor actinide (MA) transmutation fuel types such as advanced MOX, advanced metal alloy, inert matrix fuel (IMF), and other ceramic fuels like nitrides, carbides, etc., for fast neutronic spectrum conditions. Most of the advanced fuel compounds have already been the object of past examination programs, which included irradiations in research reactors. The knowledge derived from previous experience constitutes a significant, albeit incomplete body of data. New or upgraded experimental tools are available today that can extend the scientific and technological knowledge towards achieving the objectives associated with the new generation of nuclear reactors and fuels. The objectives of this project will be three-fold: (1) to extend the available knowledge on properties and irradiation behavior of high burnup and minor actinide bearing advanced fuel systems; (2) to establish a synergy with multi-scale and code development efforts in which experimental data and expertise on the irradiation behavior of nuclear fuels is properly conveyed for the upgrade/development of advanced modeling tools; (3) to promote the effective use of international resources to the characterization of irradiated fuel through exchange of expertise and information among leading experimental facilities. The priorities in this project will be set according to the down selection procedure of U.S. and European development programs.« less

Prototype Demonstration of Gamma- Blind Tensioned Metastable Fluid Neutron/Multiplicity/Alpha Detector – Real Time Methods for Advanced Fuel Cycle Applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

McDeavitt, Sean M.

The content of this report summarizes a multi-year effort to develop prototype detection equipment using the Tensioned Metastable Fluid Detector (TMFD) technology developed by Taleyarkhan [1]. The context of this development effort was to create new methods for evaluating and developing advanced methods for safeguarding nuclear materials along with instrumentation in various stages of the fuel cycle, especially in material balance areas (MBAs) and during reprocessing of used nuclear fuel. One of the challenges related to the implementation of any type of MBA and/or reprocessing technology (e.g., PUREX or UREX) is the real-time quantification and control of the transuranic (TRU)more » isotopes as they move through the process. Monitoring of higher actinides from their neutron emission (including multiplicity) and alpha signatures during transit in MBAs and in aqueous separations is a critical research area. By providing on-line real-time materials accountability, diversion of the materials becomes much more difficult. The Tensioned Metastable Fluid Detector (TMFD) is a transformational technology that is uniquely capable of both alpha and neutron spectroscopy while being “blind” to the intense gamma field that typically accompanies used fuel – simultaneously with the ability to provide multiplicity information as well [1-3]. The TMFD technology was proven (lab-scale) as part of a 2008 NERI-C program [1-7]. The bulk of this report describes the advancements and demonstrations made in TMFD technology. One final point to present before turning to the TMFD demonstrations is the context for discussing real-time monitoring of SNM. It is useful to review the spectrum of isotopes generated within nuclear fuel during reactor operations. Used nuclear fuel (UNF) from a light water reactor (LWR) contains fission products as well as TRU elements formed through neutron absorption/decay chains. The majority of the fission products are gamma and beta emitters and they represent the more significant hazards from a radiation protection standpoint. However, alpha and neutron emitting uranium and TRU elements represent the more significant safeguards and security concerns. Table 1.1 presents a representative PWR inventory of the uranium and actinide isotopes present in a used fuel assembly. The uranium and actinide isotopes (chiefly the Pu, Am and Cm elements) are all emitters of alpha particles and some of them release significant quantities of neutrons through spontaneous fissions« less

Low temperature route to uranium nitride

DOEpatents

Burrell, Anthony K.; Sattelberger, Alfred P.; Yeamans, Charles; Hartmann, Thomas; Silva, G. W. Chinthaka; Cerefice, Gary; Czerwinski, Kenneth R.

2009-09-01

A method of preparing an actinide nitride fuel for nuclear reactors is provided. The method comprises the steps of a) providing at least one actinide oxide and optionally zirconium oxide; b) mixing the oxide with a source of hydrogen fluoride for a period of time and at a temperature sufficient to convert the oxide to a fluoride salt; c) heating the fluoride salt to remove water; d) heating the fluoride salt in a nitrogen atmosphere for a period of time and at a temperature sufficient to convert the fluorides to nitrides; and e) heating the nitrides under vacuum and/or inert atmosphere for a period of time sufficient to convert the nitrides to mononitrides.

Simulation of Fast Neutronics in an Accelerator-Driven Sub-Critical Core

NASA Astrophysics Data System (ADS)

Gwyn Rosaire, C.; Sattarov, Akhdiyor; McIntyre, Peter; Tsvetkov, Pavel

2011-10-01

Accelerator-driven subcritical fission in a molten salt core (ADSMS) is being developed as a technology for green nuclear power. ADSMS burns its fertile fuel to completion, it cannot melt down, and it destroys long-lived minor actinides. The ADSMS core consists of a vessel filled with a molten salt eutectic of UCl3 and NaCl. The fast neutronics of ADSMS makes possible two unique benefits: isobreeding, a steady-state equilibrium in which ^238U is bred to ^239Pu and the ^239Pu fissions, and destruction of minor actinides, in which fission of the intermediary nuclides dominates of breeding. Results of simulations of the fast neutronics in the ADSMS core will be presented.

Experimental studies at the Idaho Chemical Processing Plant on actinide partitioning from acidic nuclear wastes

DOE Office of Scientific and Technical Information (OSTI.GOV)

McIssaac, L. D.; Baker, J. D.; Meikrantz, D. H.

1980-01-01

Wastes generated at ICPP and in the reprocessing of LWR fuel is discussed separately. DHDECMP is used as extractant. Studies on DHDECMP purification and toxicity, diluent effects, reaction kinetics, radioloysis, mixer-settler performance, etc. are reported. 10 tables, 3 figures. (DLC)

The procedure and results of calculations of the equilibrium isotopic composition of a demonstration subcritical molten salt reactor

NASA Astrophysics Data System (ADS)

Nevinitsa, V. A.; Dudnikov, A. A.; Blandinskiy, V. Yu.; Balanin, A. L.; Alekseev, P. N.; Titarenko, Yu. E.; Batyaev, V. F.; Pavlov, K. V.; Titarenko, A. Yu.

2015-12-01

A subcritical molten salt reactor with an external neutron source is studied computationally as a facility for incineration and transmutation of minor actinides from spent nuclear fuel of reactors of VVER-1000 type and for producing 233U from 232Th. The reactor configuration is chosen, the requirements to be imposed on the external neutron source are formulated, and the equilibrium isotopic composition of heavy nuclides and the key parameters of the fuel cycle are calculated.

Managing the Nuclear Fuel Cycle: Policy Implications of Expanding Global Access to Nuclear Power

DTIC Science & Technology

2009-07-01

inalienable right and, by and large, neither have U.S. government officials. However, the case of Iran raises perhaps the most critical question in this...slight difference in atomic mass between 235U and 238U. The typical enrichment process requires about 10 lbs of uranium U3O8 to produce 1 lb of low...thermal neutrons but can induce fission in all actinides , including all plutonium isotopes. Therefore, nuclear fuel for a fast reactor must have a

On the influence of the americium isotopic vector on the cooling time of minor actinides bearing blankets in fast reactors

NASA Astrophysics Data System (ADS)

Kooyman, Timothée; Buiron, Laurent; Rimpault, Gerald

2018-05-01

In the heterogeneous minor actinides transmutation approach, the nuclei to be transmuted are loaded in dedicated targets often located at the core periphery, so that long-lived heavy nuclides are turned into shorter-lived fission products by fission. To compensate for low flux level at the core periphery, the minor actinides content in the targets is set relatively high (around 20 at.%), which has a negative impact on the reprocessing of the targets due to their important decay heat level. After a complete analysis of the main contributors to the heat load of the irradiated targets, it is shown here that the choice of the reprocessing order of the various feeds of americium from the fuel cycle depends on the actual limit for fuel reprocessing. If reprocessing of hot targets is possible, it is more interesting to reprocess first the americium feed with a high 243Am content in order to limit the total cooling time of the targets, while if reprocessing of targets is limited by their decay heat, it is more interesting to wait for an increase in the 241Am content before loading the americium in the core. An optimization of the reprocessing order appears to lead to a decrease of the total cooling time by 15 years compared to a situation where all the americium feeds are mixed together when two feeds from SFR are considered with a high reprocessing limit.

Prioritized List of Research Needs to support MRWFD Case Study Flowsheet Advancement

DOE Office of Scientific and Technical Information (OSTI.GOV)

Law, Jack Douglas; Soelberg, Nicholas Ray

In FY-13, a case study evaluation was performed of full recycle technologies for both the processing of light-water reactor (LWR) used nuclear fuels as well as fast reactor (FR) fuel in the full recycle option. This effort focused on the identification of the case study processes and the initial preparation of material balance flowsheets for the identified technologies. In identifying the case study flowsheets, it was decided that two cases would be developed: one which identifies the flowsheet as currently developed and another near-term target flowsheet which identifies the flowsheet as envisioned within two years, pending the results of ongoingmore » research. The case study focus is on homogeneous aqueous recycle of the U/TRU resulting from the processing of LWR fuel as feed for metal fuel fabrication. The metal fuel is utilized in a sodium-cooled fast reactor, and the used fast reactor fuel is processed using electrochemical separations. The recovered U/TRU from electrochemical separations is recycled to fuel fabrication and the fast reactor. Waste streams from the aqueous and electrochemical processing are treated and prepared for disposition. Off-gas from the separations and waste processing are also treated. As part of the FY-13 effort, preliminary process unknowns and research needs to advance the near-term target flowsheets were identified. In FY-14, these research needs were updated, expanded and prioritized. This report again updates the prioritized list of research needs based upon results to date in FY-15. The research needs are listed for each of the main portions of the flowsheet: 1) Aqueous headend, 2) Headend tritium pretreatment off-gas, 3) Aqueous U/Pu/Np recovery, 4) Aqueous TRU product solidification, 5) Aqueous actinide/lanthanide separation, 6) Aqueous off-gas treatment, 7) Aqueous HLW management, 8) Treatment of aqueous process wastes, 9) E-chem actinide separations, 10) E-chem off-gas, 11) E-chem HLW management. The identified research needs were prioritized within each of these areas. No effort was made to perform an overall prioritization. This information will be used by the MRWFD Campaign leadership in research planning for FY-16. Additionally, this information will be incorporated into the next version of the Case Study Report scheduled to be issued September 2015.« less

Concept of DT fuel cycle for a fusion neutron source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Anan'ev, S.; Spitsyn, A.V.; Kuteev, B.V.

2015-03-15

A concept of DT-fusion neutron source (FNS) with the neutron yield higher than 10{sup 18} neutrons per second is under design in Russia. Such a FNS is of interest for many applications: 1) basic and applied research (neutron scattering, etc); 2) testing the structural materials for fusion reactors; 3) control of sub-critical nuclear systems and 4) nuclear waste processing (including transmutation of minor actinides). This paper describes the fuel cycle concept of a compact fusion neutron source based on a small spherical tokamak (FNS-ST) with a MW range of DT fusion power and considers the key physics issues of thismore » device. The major and minor radii are ∼0.5 and ∼0.3 m, magnetic field ∼1.5 T, heating power less than 15 MW and plasma current 1-2 MA. The system provides the fuel mixture with equal fractions of D and T (D:T = 1:1) for all FNS technology systems. (authors)« less

Skull counting in late stages after internal contamination by actinides.

PubMed

Tani, Kotaro; Shutt, Arron; Kurihara, Osamu; Kosako, Toshiso

2015-02-01

Monitoring preparation for internal contamination with actinides (e.g. Pu and Am) is required to assess internal doses at nuclear fuel cycle-related facilities. In this paper, the authors focus on skull counting in case of single-incident inhalation of (241)Am and propose an effective procedure for skull counting with an existing system, taking into account the biokinetic behaviour of (241)Am in the human body. The predicted response of the system to skull counting under a certain counting geometry was found to be only ∼1.0 × 10(-5) cps Bq(-1) 1y after intake. However, this disadvantage could be remedied by repeated measurements of the skull during the late stage of the intake due to the predicted response reaching a plateau at about the 1000th day after exposure and exceeding that in the lung counting. Further studies are needed for the development of a new detection system with higher sensitivity to perform reliable internal dose estimations based on direct measurements. © The Author 2014. Published by Oxford University Press. All rights reserved. For Permissions, please email: journals.permissions@oup.com.

Advantages of Production of New Fissionable Nuclides for the Nuclear Power Industry in Hybrid Fusion-Fission Reactors

NASA Astrophysics Data System (ADS)

Tsibulskiy, V. F.; Andrianova, E. A.; Davidenko, V. D.; Rodionova, E. V.; Tsibulskiy, S. V.

2017-12-01

A concept of a large-scale nuclear power engineering system equipped with fusion and fission reactors is presented. The reactors have a joint fuel cycle, which imposes the lowest risk of the radiation impact on the environment. The formation of such a system is considered within the framework of the evolution of the current nuclear power industry with the dominance of thermal reactors, gradual transition to the thorium fuel cycle, and integration into the system of the hybrid fusion-fission reactors for breeding nuclear fuel for fission reactors. Such evolution of the nuclear power engineering system will allow preservation of the existing structure with the dominance of thermal reactors, enable the reprocessing of the spent nuclear fuel (SNF) with low burnup, and prevent the dangerous accumulation of minor actinides. The proposed structure of the nuclear power engineering system minimizes the risk of radioactive contamination of the environment and the SNF reprocessing facilities, decreasing it by more than one order of magnitude in comparison with the proposed scheme of closing the uranium-plutonium fuel cycle based on the reprocessing of SNF with high burnup from fast reactors.

Actinide bioimaging in tissues: Comparison of emulsion and solid track autoradiography techniques with the iQID camera

PubMed Central

Miller, Brian W.; Van der Meeren, Anne; Tazrart, Anissa; Angulo, Jaime F.; Griffiths, Nina M.

2017-01-01

This work presents a comparison of three autoradiography techniques for imaging biological samples contaminated with actinides: emulsion-based, plastic-based autoradiography and a quantitative digital technique, the iQID camera, based on the numerical analysis of light from a scintillator screen. In radiation toxicology it has been important to develop means of imaging actinide distribution in tissues as these radionuclides may be heterogeneously distributed within and between tissues after internal contamination. Actinide distribution determines which cells are exposed to alpha radiation and is thus potentially critical for assessing absorbed dose. The comparison was carried out by generating autoradiographs of the same biological samples contaminated with actinides with the three autoradiography techniques. These samples were cell preparations or tissue sections collected from animals contaminated with different physico-chemical forms of actinides. The autoradiograph characteristics and the performances of the techniques were evaluated and discussed mainly in terms of acquisition process, activity distribution patterns, spatial resolution and feasibility of activity quantification. The obtained autoradiographs presented similar actinide distribution at low magnification. Out of the three techniques, emulsion autoradiography is the only one to provide a highly-resolved image of the actinide distribution inherently superimposed on the biological sample. Emulsion autoradiography is hence best interpreted at higher magnifications. However, this technique is destructive for the biological sample. Both emulsion- and plastic-based autoradiography record alpha tracks and thus enabled the differentiation between ionized forms of actinides and oxide particles. This feature can help in the evaluation of decorporation therapy efficacy. The most recent technique, the iQID camera, presents several additional features: real-time imaging, separate imaging of alpha particles and gamma rays, and alpha activity quantification. The comparison of these three autoradiography techniques showed that they are complementary and the choice of the technique depends on the purpose of the imaging experiment. PMID:29023595

Uranium beam characterization at CIRCE for background and contamination determinations.

PubMed

De Cesare, M; De Cesare, N; D'Onofrio, A; Fifield, L K; Gialanella, L; Terrasi, F

2015-09-01

The Accelerator Mass Spectrometry (AMS) is the most sensitive technique, compared either to the Inductively Coupled Plasma (ICP-MS) or Thermal Ionization (TI-MS) mass spectrometer, for the actinide (e.g. (236)U, (x)Pu isotopes) measurements. They are present in environmental samples at the ultra trace level since atmospheric tests of Nuclear Weapons (NWs) performed in the past, deliberate dumping of nuclear waste, nuclear fuel reprocessing, on a large scale, and operation of Nuclear Power Plants (NPPs), on a small scale, have led to the release of a wide range of radioactive nuclides in the environment. At the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy, an upgraded actinide AMS system, based on a 3-MV pelletron tandem accelerator, has been developed and routinely operated. At CIRCE a charge state distribution as a function of terminal voltage, the beam emittance, measured in the 20° actinides dedicated beam line, as well as the energy and position validation of the U ions were performed in order to determine the best measurement conditions. A (236)U/(238)U isotopic ratio background level of about 5×10(-12) or 3×10(-13), depending on the Time of Flight-Energy (TOF-E) configurations, as well as the spatial distribution of the (235)U, (238)U interferences ions and a (236)U contamination mass of about 0.5 fg have been determined. Copyright © 2015 Elsevier Ltd. All rights reserved.

DISTRIBUTION OF ACTINIDES BETWEEN THE AQUEOUS AND ORGANIC PHASES IN THE TALSPEAK PROCESS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudisill, T.; Kyser, E.

2010-09-02

One objective of the US Department of Energy's Office of Nuclear Energy (DOE-NE) is the development of sustainable nuclear fuel cycles which improve uranium resource utilization, maximize energy generation, minimize waste generation, improve safety, and complement institutional measures limiting proliferation risks. Activities in progress which support this objective include the development of advanced separation technologies to recover the actinides from used nuclear fuels. With the increased interest in the development of technology to allow closure of the nuclear fuel cycle, the TALSPEAK process is being considered for the separation of Am and Cm from the lanthanide fission products in amore » next generation reprocessing plant. However, at this time, the level of understanding associated with the chemistry and the control of the process variables is not acceptable for deployment of the process on an industrial scale. To address this issue, DOE-NE is supporting basic scientific studies focused on the TALSPEAK process through its Fuel Cycle Research and Development (R&D) program. One aspect of these studies is an experimental program at the Savannah River National Laboratory (SRNL) in which temperature-dependent distribution coefficients for the extraction of actinide elements in the TALSPEAK process were measured. The data were subsequently used to calculate conditional enthalpies and entropies of extraction by van't Hoff analysis to better understand the thermodynamic driving forces for the TALSPEAK process. In the SRNL studies, the distribution of Pu(III) in the TALSPEAK process was of particular interest. A small amount of Pu(III) would be present in the feed due to process losses and valence adjustment in prior recovery operations. Actinide elements such as Np and Pu have multiple stable oxidation states in aqueous solutions; therefore the oxidation state for these elements must be controlled in the TALSPEAK process, as the extraction chemistry is dependent upon the actinide's valence. Since our plans included the measurement of Pu(III) distribution coefficients using a Np(V) solution containing small amounts of {sup 238}Pu, it was necessary to demonstrate that the desired oxidation states of Np and Pu are produced and could be stabilized in a buffered lactate solution containing diethylenetriaminepentaacetic (DTPA). The stability of Np(V) and Pu(III) in lactic acid/DTPA solutions was evaluated by ultraviolet-visible (UV-vis) spectroscopy. To perform the evaluation, Np and Pu were added to solutions containing either hydroxylamine nitrate (HAN) or ferrous sulfamate (FS) as the reductant and nominally 1.5 M lactic acid/0.05 M DTPA. The pH of the solution was subsequently adjusted to nominally 2.8 as would be performed in the TALSPEAK process. In the valence adjustment study, we found that it was necessary to reduce Pu to Pu(III) prior to combining with the lactic acid and DTPA. The Pu reduction was performed using either HAN or FS. When FS was used, Np was reduced to Np(IV). The spectroscopic studies showed that Np(V) and Pu(III) are not stable in lactic acid/DTPA solutions. The stability of Np(IV)- and Pu(IV)-DTPA complexes are much greater than the stability of the Np(V)- and Pu(III)-DTPA complexes, and as a result, Np is slowly reduced to Np(IV) and Pu is slowly oxidized to Pu(IV) due to the reduced activity of the more stable complexes. When Np(V) was added to a solution containing a 1.5 M lactic acid/ammonium lactate buffer and 0.05 M DTPA, approximately 50% of the Np was reduced to Np(IV) in the first day. The fraction of Np(V) in the solution continued to diminish with time and was essentially reduced to Np(IV) after one week. When Pu(III) was added to a lactic acid/DTPA solution of the same composition, the spectrum recorded following at least two days after preparation of the solution continued to show some sign of Pu(III). The Pu(III) was completely oxidized to Pu(IV) after 3-4 days. The UV-vis spectroscopy demonstrated that Np(V) and Pu(III) were the predominate valences in the lactic acid/DTPA solution for the better part of a day following solution preparation. Based on these results, we chose to initially add HAN to the actinide tracer solution prepared for the distribution coefficient measurements (to produce Pu(III)) prior to combining with lactic acid and DTPA. The distribution coefficient measurements were expected to be complete in 2-3 h; therefore, Np(V) and Pu(III) valences would predominate in the solution during this time. Prior to adding the HAN to the actinide tracers, we added sufficient Am(III) activity to allow the measurement of distribution coefficients during the extraction experiments. Protactinium (V) distribution coefficients were also measured using the activity which was in secular equilibrium with the {sup 237}Np. The actinide distribution coefficients were measured at pH 2.8 and 3.5 and covered a range of temperatures from nominally 20 to 60 C.« less

An Approach for Validating Actinide and Fission Product Burnup Credit Criticality Safety Analyses--Criticality (keff) Predictions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Scaglione, John M; Mueller, Don; Wagner, John C

2011-01-01

One of the most significant remaining challenges associated with expanded implementation of burnup credit in the United States is the validation of depletion and criticality calculations used in the safety evaluation - in particular, the availability and use of applicable measured data to support validation, especially for fission products. Applicants and regulatory reviewers have been constrained by both a scarcity of data and a lack of clear technical basis or approach for use of the data. U.S. Nuclear Regulatory Commission (NRC) staff have noted that the rationale for restricting their Interim Staff Guidance on burnup credit (ISG-8) to actinide-only ismore » based largely on the lack of clear, definitive experiments that can be used to estimate the bias and uncertainty for computational analyses associated with using burnup credit. To address the issue of validation, the NRC initiated a project with the Oak Ridge National Laboratory to (1) develop and establish a technically sound validation approach (both depletion and criticality) for commercial spent nuclear fuel (SNF) criticality safety evaluations based on best-available data and methods and (2) apply the approach for representative SNF storage and transport configurations/conditions to demonstrate its usage and applicability, as well as to provide reference bias results. The purpose of this paper is to describe the criticality (k{sub eff}) validation approach, and resulting observations and recommendations. Validation of the isotopic composition (depletion) calculations is addressed in a companion paper at this conference. For criticality validation, the approach is to utilize (1) available laboratory critical experiment (LCE) data from the International Handbook of Evaluated Criticality Safety Benchmark Experiments and the French Haut Taux de Combustion (HTC) program to support validation of the principal actinides and (2) calculated sensitivities, nuclear data uncertainties, and the limited available fission product LCE data to predict and verify individual biases for relevant minor actinides and fission products. This paper (1) provides a detailed description of the approach and its technical bases, (2) describes the application of the approach for representative pressurized water reactor and boiling water reactor safety analysis models to demonstrate its usage and applicability, (3) provides reference bias results based on the prerelease SCALE 6.1 code package and ENDF/B-VII nuclear cross-section data, and (4) provides recommendations for application of the results and methods to other code and data packages.« less

Separation of actinides from lanthanides utilizing molten salt electrorefining

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grimmett, D.L.; Fusselman, S.P.; Roy, J.J.

1996-10-01

TRUMP-S (TRansUranic Management through Pyropartitioning Separation) is a pyrochemical process being developed to separate actinides form fission products in nuclear waste. A key process step involving molten salt electrorefining to separate actinides from lanthanides has been studied on a laboratory scale. Electrorefining of U, Np, Pu, Am, and lanthanide mixtures from molten cadmium at 450 C to a solid cathode utilizing a molten chloride electrolyte resulted in > 99% removal of actinides from the molten cadmium and salt phases. Removal of the last few percent of actinides is accompanied by lowered cathodic current efficiency and some lanthanide codeposition. Actinide/lanthanide separationmore » ratios on the cathode are ordered U > Np > Pu > Am and are consistent with predictions based on equilibrium potentials.« less

Th and U fuel photofission study by NTD for AD-MSR subcritical assembly

NASA Astrophysics Data System (ADS)

Sajo-Bohus, Laszlo; Greaves, Eduardo D.; Davila, Jesus; Barros, Haydn; Pino, Felix; Barrera, Maria T.; Farina, Fulvio

2015-07-01

During the last decade a considerable effort has been devoted for developing energy generating systems based on advanced nuclear technology within the design concepts of GEN-IV. Thorium base fuel systems such as accelerator driven nuclear reactors are one of the often mentioned attractive and affordable options. Several radiotherapy linear accelerators are on the market and due to their reliability, they could be employed as drivers for subcritical liquid fuel assemblies. Bremsstrahlung photons with energies above 5.5MeV, induce (γ,n) and (e,e'n) reactions in the W-target. Resulting gamma radiation and photo or fission neutrons may be absorbed in target materials such as thorium and uranium isotopes to induce sustained fission or nuclear transmutation in waste radioactive materials. Relevant photo driven and photo-fission reaction cross sections are important for actinides 232Th, 238U and 237Np in the radiotherapy machines energy range of 10-20 MV. In this study we employ passive nuclear track detectors (NTD) to determine fission rates and neutron production rates with the aim to establish the feasibility for gamma and photo-neutron driven subcritical assemblies. To cope with these objectives a 20 MV radiotherapy machine has been employed with a mixed fuel target. Results will support further development for a subcritical assembly employing a thorium containing liquid fuel. It is expected that acquired technological knowledge will contribute to the Venezuelan nuclear energy program.

Impacts of Heterogeneous Recycle in Fast Reactors on Overall Fuel Cycle

DOE Office of Scientific and Technical Information (OSTI.GOV)

Temitope A. Taiwo; Samuel E. Bays; Abdullatif M. Yacout

2011-03-01

A study in the United States has evaluated the attributes of the heterogeneous recycle approach for plutonium and minor actinide transmutation in fast reactor fuel cycles, with comparison to the homogeneous recycle approach, where pertinent. The work investigated the characteristics, advantages, and disadvantages of the approach in the overall fuel cycle, including reactor transmutation, systems and safety impacts, fuel separation and fabrication issues, and proliferation risk and transportation impacts. For this evaluation, data from previous and ongoing national studies on heterogeneous recycle were reviewed and synthesized. Where useful, information from international sources was included in the findings. The intent ofmore » the work was to provide a comprehensive assessment of the heterogeneous recycle approach at the current time.« less

Development of Online Spectroscopic pH Monitoring for Nuclear Fuel Reprocessing Plants: Weak Acid Schemes.

PubMed

Casella, Amanda J; Ahlers, Laura R H; Campbell, Emily L; Levitskaia, Tatiana G; Peterson, James M; Smith, Frances N; Bryan, Samuel A

2015-05-19

In nuclear fuel reprocessing, separating trivalent minor actinides and lanthanide fission products is extremely challenging and often necessitates tight pH control in TALSPEAK (Trivalent Actinide-Lanthanide Separation by Phosphorus reagent Extraction from Aqueous Komplexes) separations. In TALSPEAK and similar advanced processes, aqueous pH is one of the most important factors governing the partitioning of lanthanides and actinides between an aqueous phase containing a polyaminopolycarboxylate complexing agent and a weak carboxylic acid buffer and an organic phase containing an acidic organophosphorus extractant. Real-time pH monitoring would significantly increase confidence in the separation performance. Our research is focused on developing a general method for online determination of the pH of aqueous solutions through chemometric analysis of Raman spectra. Spectroscopic process-monitoring capabilities, incorporated in a counter-current centrifugal contactor bank, provide a pathway for online, real-time measurement of solution pH. The spectroscopic techniques are process-friendly and can be easily configured for online applications, whereas classic potentiometric pH measurements require frequent calibration/maintenance and have poor long-term stability in aggressive chemical and radiation environments. Raman spectroscopy discriminates between the protonated and deprotonated forms of the carboxylic acid buffer, and the chemometric processing of the Raman spectral data with PLS (partial least-squares) regression provides a means to quantify their respective abundances and therefore determine the solution pH. Interpretive quantitative models have been developed and validated under a range of chemical composition and pH conditions using a lactic acid/lactate buffer system. The developed model was applied to new spectra obtained from online spectral measurements during a solvent extraction experiment using a counter-current centrifugal contactor bank. The model predicted the pH of this validation data set within 11% for pH > 2, thus demonstrating that this technique could provide the capability of monitoring pH online in applications such as nuclear fuel reprocessing.

Design of a fuel element for a lead-cooled fast reactor

NASA Astrophysics Data System (ADS)

Sobolev, V.; Malambu, E.; Abderrahim, H. Aït

2009-03-01

The options of a lead-cooled fast reactor (LFR) of the fourth generation (GEN-IV) reactor with the electric power of 600 MW are investigated in the ELSY Project. The fuel selection, design and optimization are important steps of the project. Three types of fuel are considered as candidates: highly enriched Pu-U mixed oxide (MOX) fuel for the first core, the MOX containing between 2.5% and 5.0% of the minor actinides (MA) for next core and Pu-U-MA nitride fuel as an advanced option. Reference fuel rods with claddings made of T91 ferrite-martensitic steel and two alternative fuel assembly designs (one uses a closed hexagonal wrapper and the other is an open square variant without wrapper) have been assessed. This study focuses on the core variant with the closed hexagonal fuel assemblies. Based on the neutronic parameters provided by Monte-Carlo modeling with MCNP5 and ALEPH codes, simulations have been carried out to assess the long-term thermal-mechanical behaviour of the hottest fuel rods. A modified version of the fuel performance code FEMAXI-SCK-1, adapted for fast neutron spectrum, new fuels, cladding materials and coolant, was utilized for these calculations. The obtained results show that the fuel rods can withstand more than four effective full power years under the normal operation conditions without pellet-cladding mechanical interaction (PCMI). In a variant with solid fuel pellets, a mild PCMI can appear during the fifth year, however, it remains at an acceptable level up to the end of operation when the peak fuel pellet burnup ∼80 MW d kg-1 of heavy metal (HM) and the maximum clad damage of about 82 displacements per atom (dpa) are reached. Annular pellets permit to delay PCMI for about 1 year. Based on the results of this simulation, further steps are envisioned for the optimization of the fuel rod design, aiming at achieving the fuel burnup of 100 MW d kg-1 of HM.

Experimental findings on actinide recovery utilizing oxidation by peroxydisulfate followed by ion exchange: Fuel cycle research & development

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hobbs, D. T.; Shehee, T. C.

2015-08-31

Our research seeks to determine if inorganic ion-exchange materials can be exploited to provide effective minor actinide (Am, Cm) separation from lanthanides. Previous work has established that a number of inorganic and UMOF ion-exchange materials exhibit varying affinities for actinides and lanthanides, which may be exploited for effective separations. During FY15, experimental work focused on investigating methods to oxidize americium in dilute nitric and perchloric acid with subsequent ion-exchange performance measurements of ion exchangers with the oxidized americium in dilute nitric acid. Ion-exchange materials tested included a variety of alkali titanates. Americium oxidation testing sought to determine the influence thatmore » other redox active components may have on the oxidation of Am III. Experimental findings indicated that Ce III, Np V, and Ru II are oxidized by peroxydisulfate, but there are no indications that the presence of Ce III, Np V, and Ru II affected the rate or extent of americium oxidation at the concentrations of peroxydisulfate being used.« less

A Summary of Actinide Enrichment Technologies and Capability Gaps

DOE Office of Scientific and Technical Information (OSTI.GOV)

Patton, Bradley D.; Robinson, Sharon M.

2017-01-01

The evaluation performed in this study indicates that a new program is needed to efficiently provide a national actinide radioisotope enrichment capability to produce milligram-to-gram quantities of unique materials for user communities. This program should leverage past actinide enrichment, the recent advances in stable isotope enrichment, and assessments of the future requirements to cost effectively develop this capability while establishing an experience base for a new generation of researchers in this vital area. Preliminary evaluations indicate that an electromagnetic isotope separation (EMIS) device would have the capability to meet the future needs of the user community for enriched actinides. Themore » EMIS technology could be potentially coupled with other enrichment technologies, such as irradiation, as pre-enrichment and/or post-enrichment systems to increase the throughput, reduce losses of material, and/or reduce operational costs of the base EMIS system. Past actinide enrichment experience and advances in the EMIS technology applied in stable isotope separations should be leveraged with this new evaluation information to assist in the establishment of a domestic actinide radioisotope enrichment capability.« less

Analysis and Development of A Robust Fuel for Gas-Cooled Fast Reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Knight, Travis W.

2010-01-31

The focus of this effort was on the development of an advanced fuel for gas-cooled fast reactor (GFR) applications. This composite design is based on carbide fuel kernels dispersed in a ZrC matrix. The choice of ZrC is based on its high temperature properties and good thermal conductivity and improved retention of fission products to temperatures beyond that of traditional SiC based coated particle fuels. A key component of this study was the development and understanding of advanced fabrication techniques for GFR fuels that have potential to reduce minor actinide (MA) losses during fabrication owing to their higher vapor pressuresmore » and greater volatility. The major accomplishments of this work were the study of combustion synthesis methods for fabrication of the ZrC matrix, fabrication of high density UC electrodes for use in the rotating electrode process, production of UC particles by rotating electrode method, integration of UC kernels in the ZrC matrix, and the full characterization of each component. Major accomplishments in the near-term have been the greater characterization of the UC kernels produced by the rotating electrode method and their condition following the integration in the composite (ZrC matrix) following the short time but high temperature combustion synthesis process. This work has generated four journal publications, one conference proceeding paper, and one additional journal paper submitted for publication (under review). The greater significance of the work can be understood in that it achieved an objective of the DOE Generation IV (GenIV) roadmap for GFR Fuel—namely the demonstration of a composite carbide fuel with 30% volume fuel. This near-term accomplishment is even more significant given the expected or possible time frame for implementation of the GFR in the years 2030 -2050 or beyond.« less

Void forming pyrolytic carbon coating process

DOEpatents

Beatty, Ronald L.; Cook, Jackie L.

2000-01-01

A pyrolytic carbon coated nuclear fuel particle and method of making it. The fuel particle has a core composed of a refractory compound of an actinide metal. The pyrolytic carbon coating surrounds the core so as to provide a void volume therebetween. The coating has an initial density of no greater than 1.45 grams/cm.sup.3 and an anisotropy factor than 3.0 and a final density upon heat treatment above about 2000.degree. C. of greater than 1.7 grams/cm.sup.3 and an anisotropy factor greater than 5.

The procedure and results of calculations of the equilibrium isotopic composition of a demonstration subcritical molten salt reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nevinitsa, V. A., E-mail: Neviniza-VA@nrcki.ru; Dudnikov, A. A.; Blandinskiy, V. Yu.

2015-12-15

A subcritical molten salt reactor with an external neutron source is studied computationally as a facility for incineration and transmutation of minor actinides from spent nuclear fuel of reactors of VVER-1000 type and for producing {sup 233}U from {sup 232}Th. The reactor configuration is chosen, the requirements to be imposed on the external neutron source are formulated, and the equilibrium isotopic composition of heavy nuclides and the key parameters of the fuel cycle are calculated.

A Characteristics-Based Approach to Radioactive Waste Classification in Advanced Nuclear Fuel Cycles

NASA Astrophysics Data System (ADS)

Djokic, Denia

The radioactive waste classification system currently used in the United States primarily relies on a source-based framework. This has lead to numerous issues, such as wastes that are not categorized by their intrinsic risk, or wastes that do not fall under a category within the framework and therefore are without a legal imperative for responsible management. Furthermore, in the possible case that advanced fuel cycles were to be deployed in the United States, the shortcomings of the source-based classification system would be exacerbated: advanced fuel cycles implement processes such as the separation of used nuclear fuel, which introduce new waste streams of varying characteristics. To be able to manage and dispose of these potential new wastes properly, development of a classification system that would assign appropriate level of management to each type of waste based on its physical properties is imperative. This dissertation explores how characteristics from wastes generated from potential future nuclear fuel cycles could be coupled with a characteristics-based classification framework. A static mass flow model developed under the Department of Energy's Fuel Cycle Research & Development program, called the Fuel-cycle Integration and Tradeoffs (FIT) model, was used to calculate the composition of waste streams resulting from different nuclear fuel cycle choices: two modified open fuel cycle cases (recycle in MOX reactor) and two different continuous-recycle fast reactor recycle cases (oxide and metal fuel fast reactors). This analysis focuses on the impact of waste heat load on waste classification practices, although future work could involve coupling waste heat load with metrics of radiotoxicity and longevity. The value of separation of heat-generating fission products and actinides in different fuel cycles and how it could inform long- and short-term disposal management is discussed. It is shown that the benefits of reducing the short-term fission-product heat load of waste destined for geologic disposal are neglected under the current source-based radioactive waste classification system, and that it is useful to classify waste streams based on how favorable the impact of interim storage is on increasing repository capacity. The need for a more diverse set of waste classes is discussed, and it is shown that the characteristics-based IAEA classification guidelines could accommodate wastes created from advanced fuel cycles more comprehensively than the U.S. classification framework.

Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, Aaron T.; Nash, Kenneth L.

The basic features of an f-element extraction process based on a solvent composed of equimolar mixtures of Cyanex-923 (a mixed trialkyl phosphine oxide) and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) extractants in n-dodecane are investigated in this report. This system, which combines features of the TRPO and TALSPEAK processes, is based on co-extraction of trivalent lanthanides and actinides from 0.1 to 1.0 M HNO 3 followed by application of a buffered aminopolycarboxylate solution strip to accomplish a Reverse TALSPEAK selective removal of actinides. This mixed-extractant medium could enable a simplified approach to selective trivalent f-element extraction and actinide partitioning in amore » single process. As compared with other combined process applications in development for more compact actinide partitioning processes (DIAMEX-SANEX, GANEX, TRUSPEAK, ALSEP), this combination features only monofunctional extractants with high solubility limits and comparatively low molar mass. Selective actinide stripping from the loaded extractant phase is done using a glycine-buffered solution containing N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA) or triethylenetetramine-N,N,N',N'',N''',N'''-hexaacetic acid (TTHA). Lastly, the results reported provide evidence for simplified interactions between the two extractants and demonstrate a pathway toward using mixed monofunctional extractants to separate trivalent actinides (An) from fission product lanthanides (Ln).« less

Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME

DOE PAGES

Johnson, Aaron T.; Nash, Kenneth L.

2015-08-20

The basic features of an f-element extraction process based on a solvent composed of equimolar mixtures of Cyanex-923 (a mixed trialkyl phosphine oxide) and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) extractants in n-dodecane are investigated in this report. This system, which combines features of the TRPO and TALSPEAK processes, is based on co-extraction of trivalent lanthanides and actinides from 0.1 to 1.0 M HNO 3 followed by application of a buffered aminopolycarboxylate solution strip to accomplish a Reverse TALSPEAK selective removal of actinides. This mixed-extractant medium could enable a simplified approach to selective trivalent f-element extraction and actinide partitioning in amore » single process. As compared with other combined process applications in development for more compact actinide partitioning processes (DIAMEX-SANEX, GANEX, TRUSPEAK, ALSEP), this combination features only monofunctional extractants with high solubility limits and comparatively low molar mass. Selective actinide stripping from the loaded extractant phase is done using a glycine-buffered solution containing N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA) or triethylenetetramine-N,N,N',N'',N''',N'''-hexaacetic acid (TTHA). Lastly, the results reported provide evidence for simplified interactions between the two extractants and demonstrate a pathway toward using mixed monofunctional extractants to separate trivalent actinides (An) from fission product lanthanides (Ln).« less

Liquid fuel molten salt reactors for thorium utilization

DOE PAGES

Gehin, Jess C.; Powers, Jeffrey J.

2016-04-08

Molten salt reactors (MSRs) represent a class of reactors that use liquid salt, usually fluoride- or chloride-based, as either a coolant with a solid fuel (such as fluoride salt-cooled high temperature reactors) or as a combined coolant and fuel with fuel dissolved in a carrier salt. For liquid-fuelled MSRs, the salt can be processed online or in a batch mode to allow for removal of fission products as well as introduction of fissile fuel and fertile materials during reactor operation. The MSR is most commonly associated with the 233U/thorium fuel cycle, as the nuclear properties of 233U combined with themore » online removal of parasitic absorbers allow for the ability to design a thermal-spectrum breeder reactor; however, MSR concepts have been developed using all neutron energy spectra (thermal, intermediate, fast, and mixed-spectrum zoned concepts) and with a variety of fuels including uranium, thorium, plutonium, and minor actinides. Early MSR work was supported by a significant research and development (R&D) program that resulted in two experimental systems operating at ORNL in the 1960s, the Aircraft Reactor Experiment and the Molten Salt Reactor Experiment. Subsequent design studies in the 1970s focusing on thermal-spectrum thorium-fueled systems established reference concepts for two major design variants: (1) a molten salt breeder reactor (MSBR), with multiple configurations that could breed additional fissile material or maintain self-sustaining operation; and (2) a denatured molten salt reactor (DMSR) with enhanced proliferation-resistance. T MSRs has been selected as one of six most promising Generation IV systems and development activities have been seen in fast-spectrum MSRs, waste-burning MSRs, MSRs fueled with low-enriched uranium (LEU), as well as more traditional thorium fuel cycle-based MSRs. This study provides an historical background of MSR R&D efforts, surveys and summarizes many of the recent development, and provides analysis comparing thorium-based MSRs.« less

Magnetic susceptibilities of actinide 3d-metal intermetallic compounds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Muniz, R.B.; d'Albuquerque e Castro, J.; Troper, A.

1988-04-15

We have numerically calculated the magnetic susceptibilities which appear in the Hartree--Fock instability criterion for actinide 3d transition-metal intermetallic compounds. This calculation is based on a previous tight-binding description of these actinide-based compounds (A. Troper and A. A. Gomes, Phys. Rev. B 34, 6487 (1986)). The parameters of the calculation, which starts from simple tight-binding d and f bands are (i) occupation numbers, (ii) ratio of d-f hybridization to d bandwidth, and (iii) electron-electron Coulomb-type interactions.

Alternative Electrochemical Salt Waste Forms, Summary of FY11-FY12 Results

DOE Office of Scientific and Technical Information (OSTI.GOV)

Riley, Brian J.; Mccloy, John S.; Crum, Jarrod V.

2014-01-17

The Fuel Cycle Research and Development Program, sponsored by the U.S. Department of Energy Office of Nuclear Energy, is currently investigating alternative waste forms for wastes generated from nuclear fuel processing. One such waste results from an electrochemical separations process, called the “Echem” process. The Echem process utilizes a molten KCl-LiCl salt to dissolve the fuel. This process results in a spent salt containing alkali, alkaline earth, lanthanide halides and small quantities of actinide halides, where the primary halide is chloride with a minor iodide fraction. Pacific Northwest National Laboratory (PNNL) is concurrently investigating two candidate waste forms for themore » Echem spent-salt: high-halide minerals (i.e., sodalite and cancrinite) and tellurite (TeO2)-based glasses. Both of these candidates showed promise in fiscal year (FY) 2009 and FY2010 with a simplified nonradioactive simulant of the Echem waste. Further testing was performed on these waste forms in FY2011 and FY2012 to assess the possibility of their use in a sustainable fuel cycle. This report summarizes the combined results from FY2011 and FY2012 efforts.« less

Investigation of the feasibility of a small scale transmutation device

NASA Astrophysics Data System (ADS)

Sit, Roger Carson

This dissertation presents the design and feasibility of a small-scale, fusion-based transmutation device incorporating a commercially available neutron generator. It also presents the design features necessary to optimize the device and render it practical for the transmutation of selected long-lived fission products and actinides. Four conceptual designs of a transmutation device were used to study the transformation of seven radionuclides: long-lived fission products (Tc-99 and I-129), short-lived fission products (Cs-137 and Sr-90), and selective actinides (Am-241, Pu-238, and Pu-239). These radionuclides were chosen because they are major components of spent nuclear fuel and also because they exist as legacy sources that are being stored pending a decision regarding their ultimate disposition. The four designs include the use of two different devices; a Deuterium-Deuterium (D-D) neutron generator (for one design) and a Deuterium-Tritium (D-T) neutron generator (for three designs) in configurations which provide different neutron energy spectra for targeting the radionuclide for transmutation. Key parameters analyzed include total fluence and flux requirements; transmutation effectiveness measured as irradiation effective half-life; and activation products generated along with their characteristics: activity, dose rate, decay, and ingestion and inhalation radiotoxicity. From this investigation, conclusions were drawn about the feasibility of the device, the design and technology enhancements that would be required to make transmutation practical, the most beneficial design for each radionuclide, the consequence of the transmutation, and radiation protection issues that are important for the conceptual design of the transmutation device. Key conclusions from this investigation include: (1) the transmutation of long-lived fission products and select actinides can be practical using a small-scale, fusion driven transmutation device; (2) the transmutation of long-lived fission products could result in an irradiation effective half-life of a few years with a three order magnitude increase in the on-target neutron flux accomplishable through a combination of technological enhancements to the source and system design optimization; (3) the transmutation of long-lived fission products requires a thermal-slow energy spectrum to prevent the generation of activation products with half-lives even longer than the original radionuclide; (4) there is no benefit in trying to transmute short-lived fission products due to the ineffectiveness of the transmutation process and the generation of a multiplicity of counterproductive activation products; (5) for actinides, irradiation effective half-lives of < 1 year can be achieved with a four orders magnitude increase in the on-target flux; (6) the ideal neutron energy spectra for transmuting actinides is highly dependent on the particular radionuclide and its fission-to-capture ratio as they determine the generationrate of other actinides; and (7) the methodology developed in this dissertation provides a mechanism that can be used for studying the feasibility of transmuting other radionuclides, and its application can be extended to studying the production of radionuclides of interest in a transmutation process. Although large-scale transmutation technology is presently being researched world-wide for spent fuel management applications, such technology will not be viable for a couple of decades. This dissertation investigated the concept of a small-scale transmutation device using present technology. The results of this research show that with reasonable enhancements, transmutation of specific radionuclides can be practical in the near term.

The benefits of a fast reactor closed fuel cycle in the UK

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gregg, R.; Hesketh, K.

2013-07-01

The work has shown that starting a fast reactor closed fuel cycle in the UK, requires virtually all of Britain's existing and future PWR spent fuel to be reprocessed, in order to obtain the plutonium needed. The existing UK Pu stockpile is sufficient to initially support only a modest SFR 'closed' fleet assuming spent fuel can be reprocessed shortly after discharge (i.e. after two years cooling). For a substantial fast reactor fleet, most Pu will have to originate from reprocessing future spent PWR fuel. Therefore, the maximum fast reactor fleet size will be limited by the preceding PWR fleet size,more » so scenarios involving fast reactors still require significant quantities of uranium ore indirectly. However, once a fast reactor fuel cycle has been established, the very substantial quantities of uranium tails in the UK would ensure there is sufficient material for several centuries. Both the short and long term impacts on a repository have been considered in this work. Over the short term, the decay heat emanating from the HLW and spent fuel will limit the density of waste within a repository. For scenarios involving fast reactors, the only significant heat bearing actinide content will be present in the final cores, resulting in a 50% overall reduction in decay energy deposited within the repository when compared with an equivalent open fuel cycle. Over the longer term, radiological dose becomes more important. Total radiotoxicity (normalised by electricity generated) is lower for scenarios with Pu recycle after 2000 years. Scenarios involving fast reactors have the lowest radiotoxicity since the quantities of certain actinides (Np, Pu and Am) eventually stabilise. However, total radiotoxicity as a measure of radiological risk does not account for differences in radionuclide mobility once in repository. Radiological dose is dominated by a small number of fission products so is therefore not affected significantly by reactor type or recycling strategy (since the fission product will primarily be a function of nuclear energy generated). However, by reprocessing spent fuel, it is possible to immobilise the fission product in a more suitable waste form that has far more superior in-repository performance. (authors)« less

Overview of actinide chemistry in the WIPP

DOE Office of Scientific and Technical Information (OSTI.GOV)

Borkowski, Marian; Lucchini, Jean - Francois; Richmann, Michael K

2009-01-01

The year 2009 celebrates 10 years of safe operations at the Waste Isolation Pilot Plant (WIPP), the only nuclear waste repository designated to dispose defense-related transuranic (TRU) waste in the United States. Many elements contributed to the success of this one-of-the-kind facility. One of the most important of these is the chemistry of the actinides under WIPP repository conditions. A reliable understanding of the potential release of actinides from the site to the accessible environment is important to the WIPP performance assessment (PA). The environmental chemistry of the major actinides disposed at the WIPP continues to be investigated as partmore » of the ongoing recertification efforts of the WIPP project. This presentation provides an overview of the actinide chemistry for the WIPP repository conditions. The WIPP is a salt-based repository; therefore, the inflow of brine into the repository is minimized, due to the natural tendency of excavated salt to re-seal. Reducing anoxic conditions are expected in WIPP because of microbial activity and metal corrosion processes that consume the oxygen initially present. Should brine be introduced through an intrusion scenario, these same processes will re-establish reducing conditions. In the case of an intrusion scenario involving brine, the solubilization of actinides in brine is considered as a potential source of release to the accessible environment. The following key factors establish the concentrations of dissolved actinides under subsurface conditions: (1) Redox chemistry - The solubility of reduced actinides (III and IV oxidation states) is known to be significantly lower than the oxidized forms (V and/or VI oxidation states). In this context, the reducing conditions in the WIPP and the strong coupling of the chemistry for reduced metals and microbiological processes with actinides are important. (2) Complexation - For the anoxic, reducing and mildly basic brine systems in the WIPP, the most important inorganic complexants are expected to be carbonate/bicarbonate and hydroxide. There are also organic complexants in TRU waste with the potential to strongly influence actinide solubility. (3) Intrinsic and pseudo-actinide colloid formation - Many actinide species in their expected oxidation states tend to form colloids or strongly associate with non actinide colloids present (e.g., microbial, humic and organic). In this context, the relative importance of actinides, based on the TRU waste inventory, with respect to the potential release of actinides from the WIPP, is greater for plutonium and americium, and to less extent for uranium and thorium. The most important oxidation states for WIPP-relevant conditions are III and IV. We will present an update of the literature on WIPP-specific data, and a summary of the ongoing research related to actinide chemistry in the WIPP performed by the Los Alamos National Laboratory (LANL) Actinide Chemistry and Repository Science (ACRSP) team located in Carlsbad, NM [Reed 2007, Lucchini 2007, and Reed 2006].« less

Preparation of actinide boride materials via solid-state metathesis reactions and actinide dicarbollide precursors

NASA Astrophysics Data System (ADS)

Lupinetti, Anthony J.; Fife, Julie; Garcia, Eduardo; Abney, Kent D.

2000-07-01

Information gaps exist in the knowledge base needed for choosing among the alternate processes to be used in the safe conversion of fissile materials to optimal forms for safe interim storage, long-term storage, and ultimate disposition. The current baseline storage technology for various wastes uses borosilicate glasses.1 The focus of this paper is the synthesis of actinide-containing ceramic materials at low and moderate temperatures (200 °C-1000 °C) using molecular and polymeric actinide borane and carborane complexes.

Analysis of fuel cycle strategies and U.S. transition scenarios

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wigeland, Roald; Taiwo, Temitope A.

2016-10-17

The nuclear fuel cycle Evaluation and Screening (E&S) study that was completed in October 2014 [1] enabled the identification of four fuel cycle groups that are considered most promising based on a set of nine evaluation criteria: (a) six benefit criteria of Nuclear Waste Management, Proliferation Risk, Nuclear Material Security Risk, Safety, Environmental Impact, Resource Utilization, and (b) three challenge criteria of Development and Deployment Risk, Institutional Issues, Financial Risk and Economics. The E&S study was conducted at a level of analysis that is "technology- neutral," that is, without consideration of specific technologies, but using the fundamental physics characteristics ofmore » each part of the fuel cycle. The study focused on the fuel cycle performance benefits at the fuel cycle equilibrium state, with only limited consideration of transition and deployment impacts. Common characteristics of the four most promising fuel cycle options include continuous recycle of all U/Pu or U/TRU, the use of fast-spectrum reactors, and no use of uranium enrichment once fuel cycle equilibrium has been established. The high-level wastes are mainly from processing of irradiated fuel, and there would be no disposal of any spent fuel. Building on the findings of the E&S study, additional studies have been conducted in the last two years following the information exchange meeting, the 13th IEMPT, which was held in Seoul, the Republic of Korea in 2014. Insights are presented from the recent studies on the benefits and challenges of recycling minor actinides, and transition considerations to some of the most promising fuel cycle options.« less

Status of the French Research on Partitioning and Transmutation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Warin, Dominique

2007-07-01

The global energy context pleads in favor of a sustainable development of nuclear energy since the demand for energy will likely increase, whereas resources will tend to get scarcer and the prospect of global warming will drive down the consumption of fossil fuel sources. How we deal with radioactive waste is crucial in this context. The production of nuclear energy in France has been associated, since its inception, with the optimization of radioactive waste management, including the partitioning and the recycling of recoverable energetic materials. The public's concern regarding the long-term waste management made the French Government prepare and passmore » the December 1991 Law, requesting in particular, the study for fifteen years of solutions for still minimizing the quantity and the hazardousness of final waste, via partitioning and transmutation. At the end of these fifteen years of research, it is considered that partitioning techniques, which have been validated on real solutions, are at disposal. Indeed, aqueous process for separation of minor actinides from the PUREX raffinate has been brought to a point where there is reasonable assurance that industrial deployment can be successful. A key experiment has been the successful kilogram scale trials in the CEA-Marcoule Atalante facility in 2005 and this result, together with the results obtained in the frame of the successive European projects, constitutes a considerable step forward. For transmutation, CEA has conducted programs proving the feasibility of the elimination of minor actinides and fission products: fabrication of specific targets and fuels for transmutation tests in the HFR and Phenix reactors, neutronics and technology studies for critical reactors and ADS developments. Scenario studies have also allowed assessing the feasibility, at the level of cycle and fuel facilities, and the efficiency of transmutation in terms of the quantitative reduction of the final waste inventory depending of the reactor fleet (PWR-FR-ADS). Important results are now available concerning the possibility of significantly reducing the quantity and the radiotoxicity of long-lived waste in association with a sustainable development of nuclear energy. As France has confirmed its long-term approach to nuclear energy, the most effective implementation of P and T of minor actinides relies on the fast neutron GEN IV systems, which are designed to recycle and manage their own actinides. The perspective to deploy a first series of such systems around 2040 supports the idea that progress is being made: the long-term waste would only be made up of fission products, with very low amounts of minor actinides. In this sense, the new waste management law passed by the French Parliament on June 28, 2006, demands that P and T research continues in strong connection to GEN IV systems and ADS development and allowing the assessment of the industrial perspectives of such systems in 2012 and to put into operation a transmutation demo facility in 2020. (author)« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bernard, D.; Fabbris, O.

Two different experiments performed in the 8 MWth MELUSINE experimental power pool reactor aimed at analyzing 1 GWd/t spent fuel pellets doped with several actinides. The goal was to measure the averaged neutron induced capture cross section in two very different neutron spectra (a PWR-like and an under-moderated one). This paper summarizes the combined deterministic APOLLO2-stochastic TRIPOLI4 analysis using the JEFF-3.1.1 European nuclear data library. A very good agreement is observed for most of neutron induced capture cross section of actinides and a clear underestimation for the {sup 241}Am(n,{gamma}) as an accurate validation of its associated isomeric ratio are emphasized.more » Finally, a possible huge resonant fluctuation (factor of 2.7 regarding to the 1=0 resonance total orbital momenta) is suggested for isomeric ratio. (authors)« less

Evaluation of N,N-dialkylamides as promising process extractants

NASA Astrophysics Data System (ADS)

Pathak, P. N.; Prabhu, D. R.; Kanekar, A. S.; Manchanda, V. K.

2010-03-01

Studies carried out at BARC, India on the development of new extractants for reprocessing of spent fuel suggested that while straight chain N,N-dihexyloctanamide (DHOA) is promising alternative to TBP for the reprocessing of irradiated uranium based fuels, branched chain N,N-di(2-ethylhexyl)isobutyramide (D2EHIBA) is suitable for the selective recovery of 233U from irradiated Th. In advanced fuel cycle scenarios, the coprocessing of U/Pu stream appears attractive particularly with respect to development of proliferation resistant technologies. DHOA extracted Pu(IV) more efficiently than TBP, both at trace-level concentration as well as under uranium/plutonium loading conditions. Uranium extraction behavior of DHOA was however, similar to that of TBP during the extraction cycle. Stripping behavior of U and Pu (without any reductant) was better for DHOA than that of TBP. It was observed during batch studies that whereas 99% Pu is stripped in four stages in case of DHOA, only 89% Pu is stripped in case of TBP under identical experimental conditions. DHOA offered better fission product decontamination than that of TBP. GANEX (Group ActiNide EXtraction) and ARTIST (Amide-based Radio-resources Treatment with Interim Storage of Transuranics) processes proposed for actinide partitioning use branched chain amides for the selective extraction of uranium from spent fuel feed solutions. The branched-alkyl monoamide (BAMA) proposed to be used in ARTIST process is N,N-di-(2-ethylhexyl)butyramide (D2EHBA). In this context, the extraction behavior of U(VI) and Pu(IV) were compared using D2EHIBA, TBP, and D2EHBA under similar concentration of nitric acid (0.5 — 6M) and of uranium (0-50g/L). These studies suggested that D2EHIBA is a promising extractant for selective extraction of uranium over plutonium in process streams. Similarly, D2EHIBA offered distinctly better decontamination of 233U over Th and fission products under THOREX feed conditions. The possibility of simultaneous stripping and precipitation of thorium (as oxalate) from loaded organic phase was explored using 0.05M oxalic acid. Ammonium diuranate (ADU) precipitation was performed on the oxalate supernatant for the recovery of uranium. Quantitative recovery (>99.9%) of Th as well as of U was achieved. Radiolytic studies suggested that irradiated DHOA and D2EHIBA behaved better with respect to fission product decontamination as compared to that of TBP.

Performance evaluation of two-stage fuel cycle from SFR to PWR

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fei, T.; Hoffman, E.A.; Kim, T.K.

2013-07-01

One potential fuel cycle option being considered is a two-stage fuel cycle system involving the continuous recycle of transuranics in a fast reactor and the use of bred plutonium in a thermal reactor. The first stage is a Sodium-cooled Fast Reactor (SFR) fuel cycle with metallic U-TRU-Zr fuel. The SFRs need to have a breeding ratio greater than 1.0 in order to produce fissile material for use in the second stage. The second stage is a PWR fuel cycle with uranium and plutonium mixed oxide fuel based on the design and performance of the current state-of-the-art commercial PWRs with anmore » average discharge burnup of 50 MWd/kgHM. This paper evaluates the possibility of this fuel cycle option and discusses its fuel cycle performance characteristics. The study focuses on an equilibrium stage of the fuel cycle. Results indicate that, in order to avoid a positive coolant void reactivity feedback in the stage-2 PWR, the reactor requires high quality of plutonium from the first stage and minor actinides in the discharge fuel of the PWR needs to be separated and sent back to the stage-1 SFR. The electricity-sharing ratio between the 2 stages is 87.0% (SFR) to 13.0% (PWR) for a TRU inventory ratio (the mass of TRU in the discharge fuel divided by the mass of TRU in the fresh fuel) of 1.06. A sensitivity study indicated that by increasing the TRU inventory ratio to 1.13, The electricity generation fraction of stage-2 PWR is increased to 28.9%. The two-stage fuel cycle system considered in this study was found to provide a high uranium utilization (>80%). (authors)« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gehin, Jess C.; Powers, Jeffrey J.

Molten salt reactors (MSRs) represent a class of reactors that use liquid salt, usually fluoride- or chloride-based, as either a coolant with a solid fuel (such as fluoride salt-cooled high temperature reactors) or as a combined coolant and fuel with fuel dissolved in a carrier salt. For liquid-fuelled MSRs, the salt can be processed online or in a batch mode to allow for removal of fission products as well as introduction of fissile fuel and fertile materials during reactor operation. The MSR is most commonly associated with the 233U/thorium fuel cycle, as the nuclear properties of 233U combined with themore » online removal of parasitic absorbers allow for the ability to design a thermal-spectrum breeder reactor; however, MSR concepts have been developed using all neutron energy spectra (thermal, intermediate, fast, and mixed-spectrum zoned concepts) and with a variety of fuels including uranium, thorium, plutonium, and minor actinides. Early MSR work was supported by a significant research and development (R&D) program that resulted in two experimental systems operating at ORNL in the 1960s, the Aircraft Reactor Experiment and the Molten Salt Reactor Experiment. Subsequent design studies in the 1970s focusing on thermal-spectrum thorium-fueled systems established reference concepts for two major design variants: (1) a molten salt breeder reactor (MSBR), with multiple configurations that could breed additional fissile material or maintain self-sustaining operation; and (2) a denatured molten salt reactor (DMSR) with enhanced proliferation-resistance. T MSRs has been selected as one of six most promising Generation IV systems and development activities have been seen in fast-spectrum MSRs, waste-burning MSRs, MSRs fueled with low-enriched uranium (LEU), as well as more traditional thorium fuel cycle-based MSRs. This study provides an historical background of MSR R&D efforts, surveys and summarizes many of the recent development, and provides analysis comparing thorium-based MSRs.« less

An Investigation of Aggregation in Synergistic Solvent Extraction Systems

NASA Astrophysics Data System (ADS)

Jackson, Andy Steven

With an increasing focus on anthropogenic climate change, nuclear reactors present an attractive option for base load power generation with regard to air pollution and carbon emissions, especially when compared with traditional fossil fuel based options. However, used nuclear fuel (UNF) is highly radiotoxic and contains minor actinides (americium and curium) which remain more radiotoxic than natural uranium ore for hundreds of thousands of years, presenting a challenge for long-term storage . Advanced nuclear fuel recycling can reduce this required storage time to thousands of years by removing the highly radiotoxic minor actinides. Many advanced separation schemes have been proposed to achieve this separation but none have been implemented to date. A key feature among many proposed schemes is the use of more than one extraction reagent in a single extraction phase, which can lead to the phenomenon known as "synergism" in which the extraction efficiency for a combination of the reagents is greater than that of the individual extractants alone. This feature is not well understood for many systems and a comprehensive picture of the mechanism behind synergism does not exist. There are several proposed mechanisms for synergism though none have been used to model multiple extraction systems. This work examines several proposed advanced extractant combinations which exhibit synergism: 2-bromodecanoic acid (BDA) with 2,2':6',2"-terpyridine (TERPY), tri-n-butylphosphine oxide (TPBO) with 2-thenoyltrifluoro acetone (HTTA), and dinonylnaphthalene sulfonic acid (HDNNS) with 5,8-diethyl-7-hydroxy-dodecan-6-oxime (LIX). We examine two proposed synergistic mechanisms involving and attempt to verify the ability of these mechanisms to predict the extraction behavior of the chosen systems. These are a reverse micellar catalyzed extraction model and a mixed complex formation model. Neither was able to effectively predict the synergistic behavior of the systems. We further examine these systems for the presence of large reverse micellar aggregates and thermodynamic signatures of aggregation. Behaviors differed widely from system to system, suggesting the possibility of more than one mechanism being responsible for similar observed extraction trends.

Void reactivity feedback analysis for U-based and Th-based LWR incineration cycles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lindley, B.A.; Parks, G.T.; Franceschini, F.

2013-07-01

In reduced-moderation LWRs, an external supply of transuranic (TRU) can be incinerated by mixing it with a fertile isotope ({sup 238}U or {sup 232}Th) and recycling all the actinides after each cycle. Performance is limited by coolant reactivity feedback - the moderator density coefficient (MDC) must be kept negative. The MDC is worse when more TRU is loaded, but TRU feed is also needed to maintain criticality. To assess the performance of this fuel cycle in different neutron spectra, three LWRs are considered: 'reference' PWRs and reduced-moderation PWRs and BWRs. The MDC of the equilibrium cycle is analysed by reactivitymore » decomposition with perturbed coolant density by isotope and neutron energy. The results show that using {sup 232}Th as a fertile isotope yields superior performance to {sup 238}U. This is due essentially to the high resonance η of U bred from Th (U3), which increases the fissility of the U3-TRU isotope vector in the Th-fueled system relative to the U-fueled system, and also improves the MDC in a sufficiently hard spectrum. Spatial separation of TRU and U3 in the Th-fueled system renders further improvement by hardening the neutron spectrum in the TRU and softening it in the U3. This improves the TRU η and increases the negative MDC contribution from reduced thermal fission in U3. (authors)« less

Update of the α - n Yields for Reactor Fuel Materials for the Interest of Nuclear Safeguards

NASA Astrophysics Data System (ADS)

Simakov, S. P.; van den Berg, Q. Y.

2017-01-01

The neutron yields caused by spontaneous α-decay of actinides and subsequent (α,xn) reactions were re-evaluated for the reactor fuel materials UO2, UF6, PuO2 and PuF4. For this purpose, the most recent reference data for decay parameters, α-particle stopping powers and (α,xn) cross sections were collected, analysed and used in calculations. The input data and elaborated code were validated against available thick target neutron yields in pure and compound materials measured at accelerators or with radioactive sources. This paper provides the specific neutron yields and their uncertainties resultant from α-decay of actinides 241Am, 249Bk, 252Cf, 242,244Cm, 237Np, 238-242Pu, 232Th and 232-236,238U in oxide and fluoride compounds. The obtained results are an update of previous reference tables issued by the Los Alamos National Laboratory in 1991 which were used for the safeguarding of radioactive materials by passive non-destructive techniques. The comparison of the updated values with previous ones shows an agreement within one estimated uncertainty (≈ 10%) for oxides, and deviations of up to 50% for fluorides.

Radiolytic degradation of a new diglycol-diamide ligand for actinide and lanthanide co-extraction from spent nuclear fuel

NASA Astrophysics Data System (ADS)

Ossola, Annalisa; Macerata, Elena; Tinonin, Dario A.; Faroldi, Federica; Giola, Marco; Mariani, Mario; Casnati, Alessandro

2016-07-01

Within the Partitioning and Transmutation strategies, great efforts have been devoted in the last decades to the development of lipophilic ligands able to co-extract trivalent Lanthanides (Ln) and Actinides (An) from spent nuclear fuel. Because of the harsh working conditions these ligands undergo, it is important to prove their chemical and radiolytic stability during the counter-current multi-stage extraction process. In the present work the hydrolytic and radiolytic resistance of the freshly prepared and aged organic solutions containing the new ligand (2,6-bis[(N-methyl-N-dodecyl)carboxamide]-4-methoxy-tetrahydro-pyran) were investigated in order to evaluate the impact on the safety and efficiency of the process. Liquid-liquid extraction tests with spiked solutions showed that the ligand extracting performances are strongly impaired by storing the samples at room temperature and in the light. Moreover, the extracting efficiency of the irradiated samples resulted to be influenced by gamma irradiation, while selectivity remains unchanged. Preliminary mass spectrometric data showed that degradation is mainly due to the acid-catalysed reaction of the ligand carboxamide and ether groups with the 1-octanol present in the diluent.

PuS: Reflectivity

NASA Astrophysics Data System (ADS)

Troć, R.

This document is part of subvolume B6bβ`Actinide Monochalcogenides' of Volume 27 `Magnetic properties of non-metallic inorganic compounds based on transition elements' of Landolt-Börnstein - Group III `Condensed Matter'. The volume presents magnetic and related properties of monochalcogenides based on actinides and their solid solutions.

Development and Testing of Diglycolamide Functionalized Mesoporous Silica for Sorption of Trivalent Actinides and Lanthanides

DOE PAGES

Shusterman, Jennifer A.; Mason, Harris E.; Bowers, Jon; ...

2015-09-03

Sequestration of trivalent actinides and lanthanides present in used nuclear fuel and legacy wastes is necessary for appropriate long-term stewardship of these metals, particularly to prevent their release into the environment. Organically modified mesoporous silica is an efficient material for recovery and potential subsequent separation of actinides and lanthanides because of its high surface area, tunable ligand selection, and chemically robust substrate. Here, we have synthesized the first novel hybrid material composed of SBA-15 type mesoporous silica functionalized with diglycolamide ligands (DGA-SBA). Because of the high surface area substrate, the DGA-SBA was found to have the highest Eu capacity reportedmore » so far in the literature of all DGA solid-phase extractants. The sorption behavior of europium and americium on DGA-SBA in nitric and hydrochloric acid media was tested in batch contact experiments. DGA-SBA was found to have high sorption of Am and Eu in pH 1, 1 M, and 3 M nitric and hydrochloric acid concentrations, which makes it promising for sequestration of these metals from used nuclear fuel or legacy waste. The kinetics of Eu sorption were found to be two times slower than that for Am in 1 M HNO 3. Additionally, the short-term susceptibility of DGA-SBA to degradation in the presence of acid was probed using 29Si and 13C solid-state NMR spectroscopy. Finally, the material was found to be relatively stable under these conditions, with the ligand remaining intact after 24 h of contact with 1 M HNO 3, an important consideration in use of the DGA-SBA as an extractant from acidic media.« less

Development and Testing of Diglycolamide Functionalized Mesoporous Silica for Sorption of Trivalent Actinides and Lanthanides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shusterman, Jennifer A.; Mason, Harris E.; Bowers, Jon

Sequestration of trivalent actinides and lanthanides present in used nuclear fuel and legacy wastes is necessary for appropriate long-term stewardship of these metals, particularly to prevent their release into the environment. Organically modified mesoporous silica is an efficient material for recovery and potential subsequent separation of actinides and lanthanides because of its high surface area, tunable ligand selection, and chemically robust substrate. Here, we have synthesized the first novel hybrid material composed of SBA-15 type mesoporous silica functionalized with diglycolamide ligands (DGA-SBA). Because of the high surface area substrate, the DGA-SBA was found to have the highest Eu capacity reportedmore » so far in the literature of all DGA solid-phase extractants. The sorption behavior of europium and americium on DGA-SBA in nitric and hydrochloric acid media was tested in batch contact experiments. DGA-SBA was found to have high sorption of Am and Eu in pH 1, 1 M, and 3 M nitric and hydrochloric acid concentrations, which makes it promising for sequestration of these metals from used nuclear fuel or legacy waste. The kinetics of Eu sorption were found to be two times slower than that for Am in 1 M HNO 3. Additionally, the short-term susceptibility of DGA-SBA to degradation in the presence of acid was probed using 29Si and 13C solid-state NMR spectroscopy. Finally, the material was found to be relatively stable under these conditions, with the ligand remaining intact after 24 h of contact with 1 M HNO 3, an important consideration in use of the DGA-SBA as an extractant from acidic media.« less

Development and Optimization of Voltammetric Methods for Real Time Analysis of Electrorefiner Salt with High Concentrations of Actinides and Fission Products

DOE Office of Scientific and Technical Information (OSTI.GOV)

Simpson, Michael F.; Phongikaroon, Supathorn; Zhang, Jinsuo

This project addresses the problem of achieving accurate material control and accountability (MC&A) around pyroprocessing electrorefiner systems. Spent nuclear fuel pyroprocessing poses a unique challenge with respect to reprocessing technology in that the fuel is never fully dissolved in the process fluid. In this case, the process fluid is molten, anhydrous LiCl-KCl salt. Therefore, there is no traditional input accountability tank. However, electrorefiners (ER) accumulate very large quantities of fissile nuclear material (including plutonium) and should be well safeguarded in a commercial facility. Idaho National Laboratory (INL) currently operates a pyroprocessing facility for treatment of spent fuel from Experimental Breedermore » Reactor-II with two such ER systems. INL implements MC&A via a mass tracking model in combination with periodic sampling of the salt and other materials followed by destructive analysis. This approach is projected to be insufficient to meet international safeguards timeliness requirements. A real time or near real time monitoring method is, thus, direly needed to support commercialization of pyroprocessing. A variety of approaches to achieving real time monitoring for ER salt have been proposed and studied to date—including a potentiometric actinide sensor for concentration measurements, a double bubbler for salt depth and density measurements, and laser induced breakdown spectroscopy (LIBS) for concentration measurements. While each of these methods shows some promise, each also involves substantial technical complexity that may ultimately limit their implementation. Yet another alternative is voltammetry—a very simple method in theory that has previously been tested for this application to a limited extent. The equipment for a voltammetry system consists of off-the-shelf components (three electrodes and a potentiostat), which results in substantial benefits relative to cost and robustness. Based on prior knowledge of electrochemical reduction potentials for each of the species of interest, voltammetry can be used to quantify concentrations of a variety of elemental species—including uranium, plutonium, minor actinides, and rare earths. Various methods have been tested by other researchers to date—including cyclic voltammetry, square wave voltammetry, normal pulse voltammetry, etc. In most cases, it has been observed that there is a very limited concentration range for which the output can be readily correlated with concentration in the salt. Furthermore, testing to date has been limited to simple ternary salts with only a single element being quantified. While incomplete for application to MC&A for pyroprocessing, these results lead us to believe that voltammetry can be optimized based on salt properties and fundamental electrochemical rate processes to yield a highly accurate and robust method. This project is divided into four tasks jointly executed by three university research groups. This includes experimental measurement of key physical data on the systems of interest, development of a predictive voltammetry model, experimental validation of the voltammetry model, and design/verification of an optimized measurement method. This project supports the goals of the US-ROK Joint Fuel Cycle Study in addition to the NA-24 Office of the National Nuclear Security Agency and the International Atomic Energy Agency (IAEA).« less

PuS: Thermoelectric Power

NASA Astrophysics Data System (ADS)

Troć, R.

This document is part of subvolume B6bβ`Actinide Monochalcogenides' of Volume 27 `Magnetic properties of non-metallic inorganic compounds based on transition elements' of Landolt-Börnstein - Group III `Condensed Matter'. The volume presents magnetic and related properties of monochalcogenides based on actinides and their solid solutions.

An extended version of the SERPENT-2 code to investigate fuel burn-up and core material evolution of the Molten Salt Fast Reactor

NASA Astrophysics Data System (ADS)

Aufiero, M.; Cammi, A.; Fiorina, C.; Leppänen, J.; Luzzi, L.; Ricotti, M. E.

2013-10-01

In this work, the Monte Carlo burn-up code SERPENT-2 has been extended and employed to study the material isotopic evolution of the Molten Salt Fast Reactor (MSFR). This promising GEN-IV nuclear reactor concept features peculiar characteristics such as the on-line fuel reprocessing, which prevents the use of commonly available burn-up codes. Besides, the presence of circulating nuclear fuel and radioactive streams from the core to the reprocessing plant requires a precise knowledge of the fuel isotopic composition during the plant operation. The developed extension of SERPENT-2 directly takes into account the effects of on-line fuel reprocessing on burn-up calculations and features a reactivity control algorithm. It is here assessed against a dedicated version of the deterministic ERANOS-based EQL3D procedure (PSI-Switzerland) and adopted to analyze the MSFR fuel salt isotopic evolution. Particular attention is devoted to study the effects of reprocessing time constants and efficiencies on the conversion ratio and the molar concentration of elements relevant for solubility issues (e.g., trivalent actinides and lanthanides). Quantities of interest for fuel handling and safety issues are investigated, including decay heat and activities of hazardous isotopes (neutron and high energy gamma emitters) in the core and in the reprocessing stream. The radiotoxicity generation is also analyzed for the MSFR nominal conditions. The production of helium and the depletion in tungsten content due to nuclear reactions are calculated for the nickel-based alloy selected as reactor structural material of the MSFR. These preliminary evaluations can be helpful in studying the radiation damage of both the primary salt container and the axial reflectors.

Rapid determination of alpha emitters using Actinide resin.

PubMed

Navarro, N; Rodriguez, L; Alvarez, A; Sancho, C

2004-01-01

The European Commission has recently published the recommended radiological protection criteria for the clearance of building and building rubble from the dismantling of nuclear installations. Radionuclide specific clearance levels for actinides are very low (between 0.1 and 1 Bq g(-1)). The prevalence of natural radionuclides in rubble materials makes the verification of these levels by direct alpha counting impossible. The capability of Actinide resin (Eichrom Industries, Inc.) for extracting plutonium and americium from rubble samples has been tested in this work. Besides a strong affinity for actinides in the tri, tetra and hexavalent oxidation states, this extraction chromatographic resin presents an easy recovery of absorbed radionuclides. The retention capability was evaluated on rubble samples spiked with certified radionuclide standards (239Pu and 241Am). Samples were leached with nitric acid, passed through a chromatographic column containing the resin and the elution fraction was measured by LSC. Actinide retention varies from 60% to 80%. Based on these results, a rapid method for the verification of clearance levels for actinides in rubble samples is proposed.

Promises and Challenges of Thorium Implementation for Transuranic Transmutation - 13550

DOE Office of Scientific and Technical Information (OSTI.GOV)

Franceschini, F.; Lahoda, E.; Wenner, M.

2013-07-01

This paper focuses on the challenges of implementing a thorium fuel cycle for recycle and transmutation of long-lived actinide components from used nuclear fuel. A multi-stage reactor system is proposed; the first stage consists of current UO{sub 2} once-through LWRs supplying transuranic isotopes that are continuously recycled and burned in second stage reactors in either a uranium (U) or thorium (Th) carrier. The second stage reactors considered for the analysis are Reduced Moderation Pressurized Water Reactors (RMPWRs), reconfigured from current PWR core designs, and Fast Reactors (FRs) with a burner core design. While both RMPWRs and FRs can in principlemore » be employed, each reactor and associated technology has pros and cons. FRs have unmatched flexibility and transmutation efficiency. RMPWRs have higher fuel manufacturing and reprocessing requirements, but may represent a cheaper solution and the opportunity for a shorter time to licensing and deployment. All options require substantial developments in manufacturing, due to the high radiation field, and reprocessing, due to the very high actinide recovery ratio to elicit the claimed radiotoxicity reduction. Th reduces the number of transmutation reactors, and is required to enable a viable RMPWR design, but presents additional challenges on manufacturing and reprocessing. The tradeoff between the various options does not make the choice obvious. Moreover, without an overarching supporting policy in place, the costly and challenging technologies required inherently discourage industrialization of any transmutation scheme, regardless of the adoption of U or Th. (authors)« less

Effect of oxidation state and ionic strength on sorption of actinides (Th, U, Np, Am) to geologic media [Abstract and References Only

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dittrich, Timothy M.; Richmann, Michael K.; Reed, Donald T.

2015-10-30

The degree of conservatism in the estimated sorption partition coefficients (K ds) used in a performance assessment model is being evaluated based on a complementary batch and column method. The main focus of this work is to investigate the role of ionic strength, solution chemistry, and oxidation state (III-VI) in actinide sorption to dolomite rock. Based on redox conditions and solution chemistry expected at the WIPP, possible actinide species include Pu(III), Pu(IV), U(IV), U(VI), Np(IV), Np(V), Am(III), and Th(IV).

ADVANCED NUCLEAR FUEL CYCLE EFFECTS ON THE TREATMENT OF UNCERTAINTY IN THE LONG-TERM ASSESSMENT OF GEOLOGIC DISPOSAL SYSTEMS - EBS INPUT

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sutton, M; Blink, J A; Greenberg, H R

2012-04-25

The Used Fuel Disposition (UFD) Campaign within the Department of Energy's Office of Nuclear Energy (DOE-NE) Fuel Cycle Technology (FCT) program has been tasked with investigating the disposal of the nation's spent nuclear fuel (SNF) and high-level nuclear waste (HLW) for a range of potential waste forms and geologic environments. The planning, construction, and operation of a nuclear disposal facility is a long-term process that involves engineered barriers that are tailored to both the geologic environment and the waste forms being emplaced. The UFD Campaign is considering a range of fuel cycles that in turn produce a range of wastemore » forms. The UFD Campaign is also considering a range of geologic media. These ranges could be thought of as adding uncertainty to what the disposal facility design will ultimately be; however, it may be preferable to thinking about the ranges as adding flexibility to design of a disposal facility. For example, as the overall DOE-NE program and industrial actions result in the fuel cycles that will produce waste to be disposed, and the characteristics of those wastes become clear, the disposal program retains flexibility in both the choice of geologic environment and the specific repository design. Of course, other factors also play a major role, including local and State-level acceptance of the specific site that provides the geologic environment. In contrast, the Yucca Mountain Project (YMP) repository license application (LA) is based on waste forms from an open fuel cycle (PWR and BWR assemblies from an open fuel cycle). These waste forms were about 90% of the total waste, and they were the determining waste form in developing the engineered barrier system (EBS) design for the Yucca Mountain Repository design. About 10% of the repository capacity was reserved for waste from a full recycle fuel cycle in which some actinides were extracted for weapons use, and the remaining fission products and some minor actinides were encapsulated in borosilicate glass. Because the heat load of the glass was much less than the PWR and BWR assemblies, the glass waste form was able to be co-disposed with the open cycle waste, by interspersing glass waste packages among the spent fuel assembly waste packages. In addition, the Yucca Mountain repository was designed to include some research reactor spent fuel and naval reactor spent fuel, within the envelope that was set using the commercial reactor assemblies as the design basis waste form. This milestone report supports Sandia National Laboratory milestone M2FT-12SN0814052, and is intended to be a chapter in that milestone report. The independent technical review of this LLNL milestone was performed at LLNL and is documented in the electronic Information Management (IM) system at LLNL. The objective of this work is to investigate what aspects of quantifying, characterizing, and representing the uncertainty associated with the engineered barrier are affected by implementing different advanced nuclear fuel cycles (e.g., partitioning and transmutation scenarios) together with corresponding designs and thermal constraints.« less

Crystal growth methods dedicated to low solubility actinide oxalates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tamain, C., E-mail: christelle.tamain@cea.fr; Arab-Chapelet, B.; Rivenet, M.

Two novel crystal growth syntheses dedicated to low solubility actinide-oxalate systems and adapted to glove box handling are described. These methods based on the use of precursors of either actinide metal or oxalic acid have been optimized on lanthanide systems (analogue of actinides(III)) and then assessed on real actinide systems. They allow the synthesis of several actinide oxalate single crystals, Am{sub 2}(C{sub 2}O{sub 4}){sub 3}(H{sub 2}O){sub 3}·xH{sub 2}O, Th(C{sub 2}O{sub 4}){sub 2}·6H{sub 2}O, M{sub 2+x}[Pu{sup IV}{sub 2−x}Pu{sup III}{sub x}(C{sub 2}O{sub 4}){sub 5}]·nH{sub 2}O and M{sub 1−x}[Pu{sup III}{sub 1−x}Pu{sup IV}{sub x}(C{sub 2}O{sub 4}){sub 2}·H{sub 2}O]·nH{sub 2}O. It is the first timemore » that these well-known compounds are formed by crystal growth methods, thus enabling direct structural studies on transuranic element systems and acquisition of basic data beyond deductions from isomorphic (or not) lanthanide compounds. Characterizations by X-ray diffraction, UV–visible solid spectroscopy, demonstrate the potentialities of these two crystal growth methods to obtain oxalate compounds. - Graphical abstract: Two new single crystal growth methods dedicated to actinide oxalate compounds. - Highlights: • Use of diester as oxalate precursor for crystal growth of actinide oxalates. • Use of actinide oxide as precursor for crystal growth of actinide oxalates. • Crystal growth of Pu(III) and Am(III) oxalates. • Crystal growth of mixed Pu(III)/Pu(IV) oxalates.« less

Application of Radiation Chemistry to Some Selected Technological Issues Related to the Development of Nuclear Energy.

PubMed

Bobrowski, Krzysztof; Skotnicki, Konrad; Szreder, Tomasz

2016-10-01

The most important contributions of radiation chemistry to some selected technological issues related to water-cooled reactors, reprocessing of spent nuclear fuel and high-level radioactive wastes, and fuel evolution during final radioactive waste disposal are highlighted. Chemical reactions occurring at the operating temperatures and pressures of reactors and involving primary transients and stable products from water radiolysis are presented and discussed in terms of the kinetic parameters and radiation chemical yields. The knowledge of these parameters is essential since they serve as input data to the models of water radiolysis in the primary loop of light water reactors and super critical water reactors. Selected features of water radiolysis in heterogeneous systems, such as aqueous nanoparticle suspensions and slurries, ceramic oxides surfaces, nanoporous, and cement-based materials, are discussed. They are of particular concern in the primary cooling loops in nuclear reactors and long-term storage of nuclear waste in geological repositories. This also includes radiation-induced processes related to corrosion of cladding materials and copper-coated iron canisters, dissolution of spent nuclear fuel, and changes of bentonite clays properties. Radiation-induced processes affecting stability of solvents and solvent extraction ligands as well oxidation states of actinide metal ions during recycling of the spent nuclear fuel are also briefly summarized.

Electrochemical/Pyrometallurgical Waste Stream Processing and Waste Form Fabrication

DOE Office of Scientific and Technical Information (OSTI.GOV)

Steven Frank; Hwan Seo Park; Yung Zun Cho

This report summarizes treatment and waste form options being evaluated for waste streams resulting from the electrochemical/pyrometallurgical (pyro ) processing of used oxide nuclear fuel. The technologies that are described are South Korean (Republic of Korea – ROK) and United States of America (US) ‘centric’ in the approach to treating pyroprocessing wastes and are based on the decade long collaborations between US and ROK researchers. Some of the general and advanced technologies described in this report will be demonstrated during the Integrated Recycle Test (IRT) to be conducted as a part of the Joint Fuel Cycle Study (JFCS) collaboration betweenmore » US Department of Energy (DOE) and ROK national laboratories. The JFCS means to specifically address and evaluated the technological, economic, and safe guard issues associated with the treatment of used nuclear fuel by pyroprocessing. The IRT will involve the processing of commercial, used oxide fuel to recover uranium and transuranics. The recovered transuranics will then be fabricated into metallic fuel and irradiated to transmutate, or burn the transuranic elements to shorter lived radionuclides. In addition, the various process streams will be evaluated and tested for fission product removal, electrolytic salt recycle, minimization of actinide loss to waste streams and waste form fabrication and characterization. This report specifically addresses the production and testing of those waste forms to demonstrate their compatibility with treatment options and suitability for disposal.« less

Understanding the complexation of Eu3+ with potential ligands used for preferential separation of lanthanides and actinides in various stages of nuclear fuel cycle: A luminescence investigation.

PubMed

Sengupta, Arijit; Kadam, R M

2017-02-15

A systematic photoluminescence based investigation was carried out to understand the complexation of Eu 3+ with different ligands (TBP: tri-n-butyl phosphate, DHOA: di-n-hexyl octanamide, Cyanex 923: tri-n-alkyl phosphine oxide and Cyanex 272: Bis (2,4,4 trimethyl) pentyl phosphinic acid) used for preferential separation of lanthanides and actinides in various stages of nuclear fuel cycle. In case of TBP and DHOA complexes, 3 ligand molecules coordinated in monodentate fashion and 3 nitrate ion in bidentate fashion to Eu 3+ to satisfy the 9 coordination of Eu. In case of Cyanex 923 and Cyanex 272 complexes, 3 ligand molecules, 3 nitrate ion and 3 water molecules coordinated to Eu 3+ in monodentate fashion. The Eu complexes of TBP and DHOA were found to have D 3h local symmetry while that for Cyanex 923 and Cyanex 272 were C 3h . Judd-Ofelt analysis of these systems revealed that the covalency of EuO bond followed the trend DHOA>TBP>Cyanex 272>Cyanex 923. Different photophysical properties like radiative and non-radiative life time, branching ratio for different transitions, magnetic and electric dipole moment transition probabilities and quantum efficiency were also evaluated and compared for these systems. The magnetic dipole transition probability was found to be almost independent of ligand field perturbation while electric dipole transition probability for 5 D 0 - 7 F 2 transition was found to be hypersensitive with ligand field with a trend DHOA>TBP>Cyanex 272>Cyanex 923. Copyright © 2016 Elsevier B.V. All rights reserved.

Understanding the complexation of Eu3 + with potential ligands used for preferential separation of lanthanides and actinides in various stages of nuclear fuel cycle: A luminescence investigation

NASA Astrophysics Data System (ADS)

Sengupta, Arijit; Kadam, R. M.

2017-02-01

A systematic photoluminescence based investigation was carried out to understand the complexation of Eu3 + with different ligands (TBP: tri-n-butyl phosphate, DHOA: di-n-hexyl octanamide, Cyanex 923: tri-n-alkyl phosphine oxide and Cyanex 272: Bis (2,4,4 trimethyl) pentyl phosphinic acid) used for preferential separation of lanthanides and actinides in various stages of nuclear fuel cycle. In case of TBP and DHOA complexes, 3 ligand molecules coordinated in monodentate fashion and 3 nitrate ion in bidentate fashion to Eu3 + to satisfy the 9 coordination of Eu. In case of Cyanex 923 and Cyanex 272 complexes, 3 ligand molecules, 3 nitrate ion and 3 water molecules coordinated to Eu3 + in monodentate fashion. The Eu complexes of TBP and DHOA were found to have D3h local symmetry while that for Cyanex 923 and Cyanex 272 were C3h. Judd-Ofelt analysis of these systems revealed that the covalency of Eusbnd O bond followed the trend DHOA > TBP > Cyanex 272 > Cyanex 923. Different photophysical properties like radiative and non-radiative life time, branching ratio for different transitions, magnetic and electric dipole moment transition probabilities and quantum efficiency were also evaluated and compared for these systems. The magnetic dipole transition probability was found to be almost independent of ligand field perturbation while electric dipole transition probability for 5D0-7F2 transition was found to be hypersensitive with ligand field with a trend DHOA > TBP > Cyanex 272 > Cyanex 923. Supplementary Table 2: Determination of inner sphere water molecules from the different empirical formulae reported in the literature.

Promising Fuel Cycle Options for R&D – Results, Insights, and Future Directions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wigeland, Roald Arnold

2015-05-01

The Fuel Cycle Options (FCO) campaign in the U.S. DOE Fuel Cycle Research & Development Program conducted a detailed evaluation and screening of nuclear fuel cycles. The process for this study was described at the 2014 ICAPP meeting. This paper reports on detailed insights and questions from the results of the study. The comprehensive study identified continuous recycle in fast reactors as the most promising option, using either U/Pu or U/TRU recycle, and potentially in combination with thermal reactors, as reported at the ICAPP 2014 meeting. This paper describes the examination of the results in detail that indicated that theremore » was essentially no difference in benefit between U/Pu and U/TRU recycle, prompting questions about the desirability of pursuing the more complex U/TRU approach given that the estimated greater challenges for development and deployment. The results will be reported from the current effort that further explores what, if any, benefits of TRU recycle (minor actinides in addition to plutonium recycle) may be in order to inform decisions on future R&D directions. The study also identified continuous recycle using thorium-based fuel cycles as potentially promising, in either fast or thermal systems, but with lesser benefit. Detailed examination of these results indicated that the lesser benefit was confined to only a few of the evaluation metrics, identifying the conditions under which thorium-based fuel cycles would be promising to pursue. For the most promising fuel cycles, the FCO is also conducting analyses on the potential transition to such fuel cycles to identify the issues, challenges, and the timing for critical decisions that would need to be made to avoid unnecessary delay in deployment, including investigation of issues such as the effects of a temporary lack of plutonium fuel resources or supporting infrastructure. These studies are placed in the context of an overall analysis approach designed to provide comprehensive information to the decision-making process.« less

The Alliance of Advanced Process Control and Accountability – A Future Safeguards-By-Design Tool

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lumetta, Gregg J.; Bresee, James C.; Paviet, Patricia D.

For any chemical separation process producing a valuable product, a material balance is an important process control measurement. That is particularly true for the separation of actinides from irradiated nuclear fuel, not only for their intrinsic value but also because an incomplete material balance may indicate diversion for unauthorized use. The DOE Office of Nuclear Energy is currently carrying out at the Pacific Northwest National Laboratory an experimental measurement of how well and with what precision current technologies can implement near real-time actinide material balances. This measurement effort is called the CoDCon project. It involves the separation of a productmore » with a 70/30 uranium/plutonium mass ratio. Initial tests will use dissolved fuel simulants prepared with pure uranium and plutonium nitrates at the same input ratios as irradiated fuel. Subsequent testing with actual irradiated fuel would be done to verify the results obtained with simulants. The experiments will use advanced on-line instrumentation supported by dynamic process models. Since accountability uncertainties could mask diversions, the aim of the project is not only to measure present-day capabilities but also, through sensitivity analyses, to identify those measurements with the greatest potential for overall material-balance improvements. The latter results will help identify priorities for future fuel cycle R&D programs. Advanced separations process control and material accountability technologies thus have a common goal: to provide the best tools available for safeguards-by-design [defined by the International Atomic Energy Agency (IAEA) as the integration of the design of a new nuclear facility through planning, construction, operation and decommissioning]. Since the potential domestic use of CoDCon results may be later than their possible foreign applications, arrangements may be feasible for possible bilateral or multinational cooperation in the CoDCon project.« less

Diffusion of radiogenic helium in natural uranium oxides

NASA Astrophysics Data System (ADS)

Roudil, Danièle; Bonhoure, Jessica; Pik, Raphaël; Cuney, Michel; Jégou, Christophe; Gauthier-Lafaye, F.

2008-08-01

The issue of nuclear waste management - and especially spent fuel disposal - demands further research on the long-term behavior of helium and its impact on physical changes in UO 2 and (U,Pu)O 2 matrices subjected to self-irradiation. Helium produced by radioactive decay of the actinides concentrates in the grains or is trapped at the grain boundaries. Various scenarios can be considered, and can have a significant effect on the radionuclide source terms that will be accessible to water after the canisters have been breached. Helium production and matrix damage is generally simulated by external irradiation or with actinide-doped materials. A natural uranium oxide sample was studied to acquire data on the behavior of radiogenic helium and its diffusion under self-irradiation in spent fuel. The sample from the Pen Ar Ran deposit in the Vendée region of France dated at 320 ± 9 million of years was selected for its simple geological history, making it a suitable natural analog of spent fuel under repository conditions during the initial period in a closed system not subject to mass transfer with the surrounding environment. Helium outgassing measured by mass spectrometry to determine the He diffusion coefficients through the ore shows that: (i) a maximum of 5% (2.1% on average) of the helium produced during the last 320 Ma in this natural analog was conserved, (ii) about 33% of the residual helium is occluded in the matrix and vacancy defects (about 10 -5 mol g -1) and 67% in bubbles that were analyzed by HRTEM. A similar distribution has been observed in spent fuel and in (U 0.9,Pu 0.1)O 2. The results obtained for the natural Pen Ar Ran sample can be applied by analogy to spent fuel, especially in terms of the apparent solubility limit and the formation, characteristics and behavior of the helium bubbles.

Revisiting the diffusion mechanism of helium in UO2: A DFT+U study

NASA Astrophysics Data System (ADS)

Liu, X.-Y.; Andersson, D. A.

2018-01-01

The understanding of migration properties of helium atoms after their generation through α-decay of actinides in spent nuclear fuels is important for the safety of nuclear fuel storage and disposal. The diffusion of helium in UO2 is revisited by using the DFT+U simulation methodology employing the "U-ramping" method to address the issue of metastable energy states. A novel diffusion mechanism by helium interstitials, the "asymmetric hop" mechanism, is reported and compared to other diffusion mechanisms including an oxygen vacancy mediated mechanism and available experimental diffusion data. The new mechanism is shown to be the dominant one over a wide temperature range.

Fission products and nuclear fuel behaviour under severe accident conditions part 1: Main lessons learnt from the first VERDON test

NASA Astrophysics Data System (ADS)

Pontillon, Y.; Geiger, E.; Le Gall, C.; Bernard, S.; Gallais-During, A.; Malgouyres, P. P.; Hanus, E.; Ducros, G.

2017-11-01

This paper describes the first VERDON test performed at the end of September 2011 with special emphasis on the behaviour of fission products (FP) and actinides during the accidental sequence itself. Two other papers discuss in detail the post-test examination results (SEM, EPMA and SIMS) of the VERDON-1 sample. The first VERDON test was devoted to studying UO2 fuel behaviour and fission product releases under reducing conditions at very high temperature (∼2883 K), which was able to confirm the very good performance of the VERDON loop. The fuel sample did not lose its integrity during this test. According to the FP behaviour measured by the online gamma station (fuel sight), the general classification of the FP in relation to their released fraction is very accurate, and the burn-up effect on the release rate is clearly highlighted.

Room temperature electrodeposition of actinides from ionic solutions

DOEpatents

Hatchett, David W.; Czerwinski, Kenneth R.; Droessler, Janelle; Kinyanjui, John

2017-04-25

Uranic and transuranic metals and metal oxides are first dissolved in ozone compositions. The resulting solution in ozone can be further dissolved in ionic liquids to form a second solution. The metals in the second solution are then electrochemically deposited from the second solutions as room temperature ionic liquid (RTIL), tri-methyl-n-butyl ammonium n-bis(trifluoromethansulfonylimide) [Me.sub.3N.sup.nBu][TFSI] providing an alternative non-aqueous system for the extraction and reclamation of actinides from reprocessed fuel materials. Deposition of U metal is achieved using TFSI complexes of U(III) and U(IV) containing the anion common to the RTIL. TFSI complexes of uranium were produced to ensure solubility of the species in the ionic liquid. The methods provide a first measure of the thermodynamic properties of U metal deposition using Uranium complexes with different oxidation states from RTIL solution at room temperature.

The Energy and Security Nexus: A Strategic Dilemma

DTIC Science & Technology

2012-11-01

constructive criticism where it was most needed. ix Joseph Caddell also provided crucial guidance in framing the conference proposal. Finally, my thanks...conflict. Critics of biofuels further claim that diversion of land for fuel in the United States has driven up world food prices and arguably triggered...recycle and consume all actinides may provide a solution. But they arguably carry a proliferation risk. Steps can be taken to safeguard and secure

Vapor deposition of hardened niobium

DOEpatents

Blocher, Jr., John M.; Veigel, Neil D.; Landrigan, Richard B.

1983-04-19

A method of coating ceramic nuclear fuel particles containing a major amount of an actinide ceramic in which the particles are placed in a fluidized bed maintained at ca. 800.degree. to ca. 900.degree. C., and niobium pentachloride vapor and carbon tetrachloride vapor are led into the bed, whereby niobium metal is deposited on the particles and carbon is deposited interstitially within the niobium. Coating apparatus used in the method is also disclosed.

Quantitative NDA measurements of advanced reprocessing product materials containing uranium, neptunium, plutonium, and americium

NASA Astrophysics Data System (ADS)

Goddard, Braden

The ability of inspection agencies and facility operators to measure powders containing several actinides is increasingly necessary as new reprocessing techniques and fuel forms are being developed. These powders are difficult to measure with nondestructive assay (NDA) techniques because neutrons emitted from induced and spontaneous fission of different nuclides are very similar. A neutron multiplicity technique based on first principle methods was developed to measure these powders by exploiting isotope-specific nuclear properties, such as the energy-dependent fission cross sections and the neutron induced fission neutron multiplicity. This technique was tested through extensive simulations using the Monte Carlo N-Particle eXtended (MCNPX) code and by one measurement campaign using the Active Well Coincidence Counter (AWCC) and two measurement campaigns using the Epithermal Neutron Multiplicity Counter (ENMC) with various (alpha,n) sources and actinide materials. Four potential applications of this first principle technique have been identified: (1) quantitative measurement of uranium, neptunium, plutonium, and americium materials; (2) quantitative measurement of mixed oxide (MOX) materials; (3) quantitative measurement of uranium materials; and (4) weapons verification in arms control agreements. This technique still has several challenges which need to be overcome, the largest of these being the challenge of having high-precision active and passive measurements to produce results with acceptably small uncertainties.

Neutron-Induced Fission Cross Section Measurements for Full Suite of Uranium Isotopes

NASA Astrophysics Data System (ADS)

Laptev, Alexander; Tovesson, Fredrik; Hill, Tony

2010-11-01

A well established program of neutron-induced fission cross section measurement at Los Alamos Neutron Science Center (LANSCE) is supporting the Fuel Cycle Research program (FC R&D). The incident neutron energy range spans energies from sub-thermal energies up to 200 MeV by measuring both the Lujan Center and the Weapons Neutron Research center (WNR). Conventional parallel-plate fission ionization chambers with actinide deposited foils are used as a fission detector. The time-of-flight method is implemented to measure neutron energy. Counting rate ratio from investigated and standard U-235 foils is translated into fission cross section ratio. Different methods of normalization for measured ratio are employed, namely, using of actinide deposit thicknesses, normalization to evaluated data, etc. Finally, ratios are converted to cross sections based on the standard U-235 fission cross section data file. Preliminary data for newly investigated isotopes U-236 and U-234 will be reported. Those new data complete a full suite of Uranium isotopes, which were investigated with presented experimental approach. When analysis of the new measured data will is completed, data will be delivered to evaluators. Having data for full set of Uranium isotopes will increase theoretical modeling capabilities and make new data evaluations much more reliable.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gerczak, Tyler J.; Smith, Kurt R.; Petrie, Christian M.

Tristructural-isotropic (TRISO)–coated particle fuel is a promising advanced fuel concept consisting of a spherical fuel kernel made of uranium oxide and uranium carbide, surrounded by a porous carbonaceous buffer layer and successive layers of dense inner pyrolytic carbon (IPyC), silicon carbide (SiC) deposited by chemical vapor , and dense outer pyrolytic carbon (OPyC). This fuel concept is being considered for advanced reactor applications such as high temperature gas-cooled reactors (HTGRs) and molten salt reactors (MSRs), as well as for accident-tolerant fuel for light water reactors (LWRs). Development and implementation of TRISO fuel for these reactor concepts support the US Departmentmore » of Energy (DOE) Office of Nuclear Energy mission to promote safe, reliable nuclear energy that is sustainable and environmentally friendly. During operation, the SiC layer serves as the primary barrier to metallic fission products and actinides not retained in the kernel. It has been observed that certain fission products are released from TRISO fuel during operation, notably, Ag, Eu, and Sr [1]. Release of these radioisotopes causes safety and maintenance concerns.« less

Actinide oxide photodiode and nuclear battery

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sykora, Milan; Usov, Igor

Photodiodes and nuclear batteries may utilize actinide oxides, such a uranium oxide. An actinide oxide photodiode may include a first actinide oxide layer and a second actinide oxide layer deposited on the first actinide oxide layer. The first actinide oxide layer may be n-doped or p-doped. The second actinide oxide layer may be p-doped when the first actinide oxide layer is n-doped, and the second actinide oxide layer may be n-doped when the first actinide oxide layer is p-doped. The first actinide oxide layer and the second actinide oxide layer may form a p/n junction therebetween. Photodiodes including actinide oxidesmore » are better light absorbers, can be used in thinner films, and are more thermally stable than silicon, germanium, and gallium arsenide.« less

Method for the recovery of actinide elements from nuclear reactor waste

DOEpatents

Horwitz, E. Philip; Delphin, Walter H.; Mason, George W.

1979-01-01

A process for partitioning and recovering actinide values from acidic waste solutions resulting from reprocessing of irradiated nuclear fuels by adding hydroxylammonium nitrate and hydrazine to the waste solution to adjust the valence of the neptunium and plutonium values in the solution to the +4 oxidation state, thus forming a feed solution and contacting the feed solution with an extractant of dihexoxyethyl phosphoric acid in an organic diluent whereby the actinide values, most of the rare earth values and some fission product values are taken up by the extractant. Separation is achieved by contacting the loaded extractant with two aqueous strip solutions, a nitric acid solution to selectively strip the americium, curium and rare earth values and an oxalate solution of tetramethylammonium hydrogen oxalate and oxalic acid or trimethylammonium hydrogen oxalate to selectively strip the neptunium, plutonium and fission product values. Uranium values remain in the extractant and may be recovered with a phosphoric acid strip. The neptunium and plutonium values are recovered from the oxalate by adding sufficient nitric acid to destroy the complexing ability of the oxalate, forming a second feed, and contacting the second feed with a second extractant of tricaprylmethylammonium nitrate in an inert diluent whereby the neptunium and plutonium values are selectively extracted. The values are recovered from the extractant with formic acid.

Mixed Metal Phosphonate- Phosphate Resins for Separation of Lanthanides from Actinides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Clearfield, Abraham

As indicated in the previous annual report the goals of this project are to develop procedures for efficient separation of lanthanides from actinides and curium from americium. These processes are required for the nuclear fuel cycle to minimize the waste and recover the valuable actinides. The basis for our study is that we have prepared a group of compounds that are porous and favor the uptake of ions with charges 3+ and 4+ over ions of lesser charge. The general formula for these materials is M(O 3PC 6H 4PO 3) 1-x/2(APO 4)x·nH 2O: where M=Zr 4+, Sn 4+, A=H, Na,more » or K and X=O, 0.5, 0.8, 1.0, 1.33 and 1.61-3. One of our tasks is to determine which members of this group of compounds are effective in carrying out the required separations. A difficulty in obtaining this required information is that the compounds are amorphous. That is they are not crystalline, therefore we need to resort to synchrotron data to obtain structural data which will be presented in detail. This information will be provided as a separate section.« less

Atomistic modeling of the solid-state chemistry of actinide materials

NASA Astrophysics Data System (ADS)

Shuller, Lindsay C.

Materials that incorporate actinides are critical to the nuclear fuel cycle, either as nuclear fuels or nuclear waste forms. In this thesis, I examine four materials: i) ThO2-UO2 solid solutions, ii) binary ThO2-CeO2-ZrO2 solid solutions, iii) Np-doped studtite, iv) Np-doped boltwoodite. Computational methods, particularly density functional theory (DFT) calculations and Monte-Carlo (MC) simulations, are used to determine the energetics and structures of these actinide-bearing materials. The solid-solution behavior of nuclear fuels and nuclear waste forms indicate the thermodynamic stability of the material, which is important for understanding the in-reactor fuel properties and long-term stability of used fuel. The ThxU1-xO2 and ThxCe 1-xO2 binaries are almost completely miscible; however, DeltaGmix reveals a small tendency for the systems to exsolve (e.g., DeltaEexsoln(Th xU1-xO2) = 0.13 kJ/(mol cations) at 750 K). Kinetic hindrances (e.g., interfacial energy) may inhibit exsolution, especially at the low temperatures necessary to stabilize the nanoscale exsolution lamellae observed in the ThxU1-xO2 and Ce xZr1-xO2 binaries. Miscibility in the Zr-bearing binaries is limited. At 1400 °C, only 3.6 and 0.09 mol% ZrO2 is miscible in CeO2 and ThO2, respectively. The incorporation of minor amounts of Np5+,6+ into uranium alteration phases, e.g., studtite [UO2O2 (H2O)4] or boltwoodite [K(UO2)(SiO 3OH)(H2O)1.5] , may limit the mobility of aqueous neptunyl complexes released from oxidized nuclear fuels. Np6+-incorporation into studtite requires less energy than Np5+-incorporation (e.g., with source/sink = Np2O5/UO 3 DeltaEincorp(Np6+) = 0.42 eV and DeltaEincorp(Np5+) = 1.12 eV). In addition, Np6+ is completely miscible in studtite at room temperature with respect to a hypothetical Np6+-studtite. Electronic structure calculations provide insight into Np-bonding in studtite. The Np 5f orbitals are within the band gap of studtite, resulting in the narrowing of the band gap from 2.29 eV for studtite to 1.09 eV for Np-incorporated studtite. Three charge-balancing mechanisms for the substitution of Np5+ for U6+ were compared: i) addition of H+ [DeltaEincorp(bolt) = 0.79 eV; DeltaEincorp(stud) = 1.12 eV], ii) interlayer coupled substitution [DeltaEincorp (bolt) = 1.40 eV], iii) intra-layer coupled-substitution [DeltaEincorp(bolt) = 0.86 eV]. Solid-solution calculations of the intra-layer coupled-substitution mechanism, where Np 5+ and P5+ substitute for U6+ and Si 4+, predict an incorporation limit of 585 ppm at 300 °C.

Separation of americium from europium using 3,3'-dimethoxy-phenyl-bis-1,2,4-triazinyl-2,6-pyridine

DOE PAGES

Hill, Talon G.; Chin, Ai Lin; Tai, Serene; ...

2017-03-22

Development of liquid-liquid separation processes for the effective removal of the minor actinide Am(III) from used nuclear fuel using ligand-based strategies continues to be an area of significant research focus. The current investigation demonstrates the efficacy of a nitrogen-based bis-triazinyl pyridine (BTP) derivative to selectively extract Am(III) from nitric acid solutions containing light lanthanides. The performance of 3,3’-dimethoxy-phenyl-bis-1,2,4-triazinyl-2,6- pyridine (MOB-BTP) was compared to that of a camphor substituted BTP (CA-BTP). The results of this investigation demonstrate the novel 3,3’-methoxy-BTP extractant dissolved in a polar diluent was a more efficient extractant for Am(III) at a lower concentration than CA-BTP under comparablemore » conditions.« less

Separation of americium from europium using 3,3'-dimethoxy-phenyl-bis-1,2,4-triazinyl-2,6-pyridine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hill, Talon G.; Chin, Ai Lin; Tai, Serene

Development of liquid-liquid separation processes for the effective removal of the minor actinide Am(III) from used nuclear fuel using ligand-based strategies continues to be an area of significant research focus. The current investigation demonstrates the efficacy of a nitrogen-based bis-triazinyl pyridine (BTP) derivative to selectively extract Am(III) from nitric acid solutions containing light lanthanides. The performance of 3,3’-dimethoxy-phenyl-bis-1,2,4-triazinyl-2,6- pyridine (MOB-BTP) was compared to that of a camphor substituted BTP (CA-BTP). The results of this investigation demonstrate the novel 3,3’-methoxy-BTP extractant dissolved in a polar diluent was a more efficient extractant for Am(III) at a lower concentration than CA-BTP under comparablemore » conditions.« less

Fission yields data generation and benchmarks of decay heat estimation of a nuclear fuel

NASA Astrophysics Data System (ADS)

Gil, Choong-Sup; Kim, Do Heon; Yoo, Jae Kwon; Lee, Jounghwa

2017-09-01

Fission yields data with the ENDF-6 format of 235U, 239Pu, and several actinides dependent on incident neutron energies have been generated using the GEF code. In addition, fission yields data libraries of ORIGEN-S, -ARP modules in the SCALE code, have been generated with the new data. The decay heats by ORIGEN-S using the new fission yields data have been calculated and compared with the measured data for validation in this study. The fission yields data ORIGEN-S libraries based on ENDF/B-VII.1, JEFF-3.1.1, and JENDL/FPY-2011 have also been generated, and decay heats were calculated using the ORIGEN-S libraries for analyses and comparisons.

The radiation chemistry of ionic liquids: A review

DOE PAGES

Mincher, Bruce J.; Wishart, James F.

2014-07-03

Ionic liquids have received increasing attention as media for radiochemical separations. Recent literature includes examinations of the efficiencies and mechanisms of the solvent extraction of lanthanides, actinides and fission products into ionic liquid solutions. For radiochemical applications, including as replacement solvents for nuclear fuel reprocessing, a thorough understanding of the radiation chemistry of ionic liquids will be required. Such an understanding can be achieved based on a combination of steady-state radiolysis experiments coupled with post-irradiation product identification and pulse-radiolysis experiments to acquire kinetic information. These techniques allow for the elucidation of radiolytic mechanisms. This contribution reviews the current ionic liquidmore » radiation chemistry literature as it affects separations, with these considerations in mind.« less

Selective Separation of Trivalent Actinides from Lanthanides by Aqueous Processing with Introduction of Soft Donor Atoms

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kenneth L. Nash

2009-09-22

Implementation of a closed loop nuclear fuel cycle requires the utilization of Pu-containing MOX fuels with the important side effect of increased production of the transplutonium actinides, most importantly isotopes of Am and Cm. Because the presence of these isotopes significantly impacts the long-term radiotoxicity of high level waste, it is important that effective methods for their isolation and/or transmutation be developed. Furthermore, since transmutation is most efficiently done in the absence of lanthanide fission products (high yield species with large thermal neutron absorption cross sections) it is important to have efficient procedures for the mutual separation of Am andmore » Cm from the lanthanides. The chemistries of these elements are nearly identical, differing only in the slightly stronger strength of interaction of trivalent actinides with ligand donor atoms softer than O (N, Cl-, S). Research being conducted around the world has led to the development of new reagents and processes with considerable potential for this task. However, pilot scale testing of these reagents and processes has demonstrated the susceptibility of the new classes of reagents to radiolytic and hydrolytic degradation. In this project, separations of trivalent actinides from fission product lanthanides have been investigated in studies of 1) the extraction and chemical stability properties of a class of soft-donor extractants that are adapted from water-soluble analogs, 2) the application of water soluble soft-donor complexing agents in tandem with conventional extractant molecules emphasizing fundamental studies of the TALSPEAK Process. This research was conducted principally in radiochemistry laboratories at Washington State University. Collaborators at the Radiological Processing Laboratory (RPL) at the Pacific Northwest National Laboratory (PNNL) have contributed their unique facilities and capabilities, and have supported student internships at PNNL to broaden their academic experience. New information has been developed to qualify the extraction potential of a class of pyridine-functionalized tetraaza complexants indicating potential single contact Am-Nd separation factors of about 40. The methodology developed for characterization will find further application in our continuing efforts to synthesize and characterize new reagents for this separation. Significant new insights into the performance envelope and supporting information on the TALSPEAK process has also been developed.« less

Testing actinide fission yield treatment in CINDER90 for use in MCNP6 burnup calculations

DOE PAGES

Fensin, Michael Lorne; Umbel, Marissa

2015-09-18

Most of the development of the MCNPX/6 burnup capability focused on features that were applied to the Boltzman transport or used to prepare coefficients for use in CINDER90, with little change to CINDER90 or the CINDER90 data. Though a scheme exists for best solving the coupled Boltzman and Bateman equations, the most significant approximation is that the employed nuclear data are correct and complete. Thus, the CINDER90 library file contains 60 different actinide fission yields encompassing 36 fissionable actinides (thermal, fast, high energy and spontaneous fission). Fission reaction data exists for more than 60 actinides and as a result, fissionmore » yield data must be approximated for actinides that do not possess fission yield information. Several types of approximations are used for estimating fission yields for actinides which do not possess explicit fission yield data. The objective of this study is to test whether or not certain approximations of fission yield selection have any impact on predictability of major actinides and fission products. Further we assess which other fission products, available in MCNP6 Tier 3, result in the largest difference in production. Because the CINDER90 library file is in ASCII format and therefore easily amendable, we assess reasons for choosing, as well as compare actinide and major fission product prediction for the H. B. Robinson benchmark for, three separate fission yield selection methods: (1) the current CINDER90 library file method (Base); (2) the element method (Element); and (3) the isobar method (Isobar). Results show that the three methods tested result in similar prediction of major actinides, Tc-99 and Cs-137; however, certain fission products resulted in significantly different production depending on the method of choice.« less

Heterogeneous sodium fast reactor designed for transmuting minor actinide waste isotopes into plutonium fuel

NASA Astrophysics Data System (ADS)

Bays, Samuel Eugene

2008-10-01

In the past several years there has been a renewed interest in sodium fast reactor (SFR) technology for the purpose of destroying transuranic waste (TRU) produced by light water reactors (LWR). The utility of SFRs as waste burners is due to the fact that higher neutron energies allow all of the actinides, including the minor actinides (MA), to contribute to fission. It is well understood that many of the design issues of LWR spent nuclear fuel (SNF) disposal in a geologic repository are linked to MAs. Because the probability of fission for essentially all the "non-fissile" MAs is nearly zero at low neutron energies, these isotopes act as a neutron capture sink in most thermal reactor systems. Furthermore, because most of the isotopes produced by these capture reactions are also non-fissile, they too are neutron sinks in most thermal reactor systems. Conversely, with high neutron energies, the MAs can produce neutrons by fast fission. Additionally, capture reactions transmute the MAs into mostly plutonium isotopes, which can fission more readily at any energy. The transmutation of non-fissile into fissile atoms is the premise of the plutonium breeder reactor. In a breeder reactor, not only does the non-fissile "fertile" U-238 atom contribute fast fission neutrons, but also transmutes into fissile Pu-239. The fissile value of the plutonium produced by MA transmutation can only be realized in fast neutron spectra. This is due to the fact that the predominate isotope produced by MA transmutation, Pu-238, is itself not fissile. However, the Pu-238 fission cross section is significantly larger than the original transmutation parent, predominately: Np-237 and Am-241, in the fast energy range. Also, Pu-238's fission cross section and fission-to-capture ratio is almost as high as that of fissile Pu-239 in the fast neutron spectrum. It is also important to note that a neutron absorption in Pu-238, that does not cause fission, will instead produce fissile Pu-239. Given this fast fissile quality and also the fact that Pu-238 is transmuted from Np-237 and Am-241, these MAs are regarded as fertile material in the SFR design proposed by this dissertation. This dissertation demonstrates a SFR design which is dedicated to plutonium breeding by targeting Am-241 transmutation. This SFR design uses a moderated axial transmutation target that functions primarily as a pseudo-blanket fuel, which is reprocessed with the active driver fuel in an integrated recycling strategy. This work demonstrates the cost and feasibility advantages of plutonium breeding via MA transmutation by adopting reactor, reprocessing and fuel technologies previously demonstrated for traditional breeder reactors. The fuel cycle proposed seeks to find a harmony between the waste management advantages of transuranic burning SFRs and the resource sustainability of traditional plutonium breeder SFRs. As a result, the enhanced plutonium conversion from MAs decreases the burner SFR's fuel costs, by extracting more fissile value from the initial TRU purchased through SNF reprocessing.

Technical Basis for Peak Reactivity Burnup Credit for BWR Spent Nuclear Fuel in Storage and Transportation Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marshall, William BJ J; Ade, Brian J; Bowman, Stephen M

2015-01-01

Oak Ridge National Laboratory and the United States Nuclear Regulatory Commission have initiated a multiyear project to investigate application of burnup credit for boiling-water reactor (BWR) fuel in storage and transportation casks. This project includes two phases. The first phase (1) investigates applicability of peak reactivity methods currently used in spent fuel pools (SFPs) to storage and transportation systems and (2) evaluates validation of both reactivity (k eff) calculations and burnup credit nuclide concentrations within these methods. The second phase will focus on extending burnup credit beyond peak reactivity. This paper documents the first phase, including an analysis of latticemore » design parameters and depletion effects, as well as both validation components. Initial efforts related to extended burnup credit are discussed in a companion paper. Peak reactivity analyses have been used in criticality analyses for licensing of BWR fuel in SFPs over the last 20 years. These analyses typically combine credit for the gadolinium burnable absorber present in the fuel with a modest amount of burnup credit. Gadolinium burnable absorbers are used in BWR assemblies to control core reactivity. The burnable absorber significantly reduces assembly reactivity at beginning of life, potentially leading to significant increases in assembly reactivity for burnups less than 15–20 GWd/MTU. The reactivity of each fuel lattice is dependent on gadolinium loading. The number of gadolinium-bearing fuel pins lowers initial lattice reactivity, but it has a small impact on the burnup and reactivity of the peak. The gadolinium concentration in each pin has a small impact on initial lattice reactivity but a significant effect on the reactivity of the peak and the burnup at which the peak occurs. The importance of the lattice parameters and depletion conditions are primarily determined by their impact on the gadolinium depletion. Criticality code validation for BWR burnup credit at peak reactivity requires a different set of experiments than for pressurized-water reactor burnup credit analysis because of differences in actinide compositions, presence of residual gadolinium absorber, and lower fission product concentrations. A survey of available critical experiments is presented along with a sample criticality code validation and determination of undercoverage penalties for some nuclides. The validation of depleted fuel compositions at peak reactivity presents many challenges which largely result from a lack of radiochemical assay data applicable to BWR fuel in this burnup range. In addition, none of the existing low burnup measurement data include residual gadolinium measurements. An example bias and uncertainty associated with validation of actinide-only fuel compositions is presented.« less

Reactor-based management of used nuclear fuel: assessment of major options.

PubMed

Finck, Phillip J; Wigeland, Roald A; Hill, Robert N

2011-01-01

This paper discusses the current status of the ongoing Advanced Fuel Cycle Initiative (AFCI) program in the U.S. Department of Energy that is investigating the potential for using the processing and recycling of used nuclear fuel to improve radioactive waste management, including used fuel. A key element of the strategies is to use nuclear reactors for further irradiation of recovered chemical elements to transmute certain long-lived highly-radioactive isotopes into less hazardous isotopes. Both thermal and fast neutron spectrum reactors are being studied as part of integrated nuclear energy systems where separations, transmutation, and disposal are considered. Radiotoxicity is being used as one of the metrics for estimating the hazard of used fuel and the processing of wastes resulting from separations and recycle-fuel fabrication. Decay heat from the used fuel and/or wastes destined for disposal is used as a metric for use of a geologic repository. Results to date indicate that the most promising options appear to be those using fast reactors in a repeated recycle mode to limit buildup of higher actinides, since the transuranic elements are a key contributor to the radiotoxicity and decay heat. Using such an approach, there could be much lower environmental impact from the high-level waste as compared to direct disposal of the used fuel, but there would likely be greater generation of low-level wastes that will also require disposal. An additional potential waste management benefit is having the ability to tailor waste forms and contents to one or more targeted disposal environments (i.e., to be able to put waste in environments best-suited for the waste contents and forms). Copyright © 2010 Health Physics Society

Recovery of minor actinides from spent fuel using TPEN-immobilized gels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Koyama, S.; Suto, M.; Ohbayashi, H.

2013-07-01

A series of separation experiments was performed in order to study the recovery process for minor actinides (MAs), such as americium (Am) and curium (Cm), from the actual spent fuel by using an extraction chromatographic technique. N,N,N',N'-tetrakis-(4-propenyloxy-2-pyridylmethyl) ethylenediamine (TPPEN) is an N,N,N',N'-tetrakis (2-pyridylmethyl) ethylenediamine (TPEN) analogue consisting of an incorporated pyridine ring that acts as not only a ligand but also as a site for polymerization and crosslinking of the gel. The TPPEN and N-isopropylacrylamide (NIPA) were dissolved into dimethylformamide (DMF, Wako Co., Ltd.) and a silica beads polymer, and then TTPEN was immobilized chemically in a polymer gel (somore » called TPEN-gel). Mixed oxide (MOX) fuel, which was highly irradiated up to 119 GWD/MTM in the experimental fast reactor Joyo, was used as a reference spent fuel. First, uranium (U) and plutonium (Pu) were separated from the irradiated fuel using an ion-exchange method, and then, the platinum group elements were removed by CMPO to leave a mixed solution of MAs and lanthanides. The 3 mol% TPPEN-gel was packed with as an extraction column (CV: 1 ml) and then rinsed by 0.1 M NaNO{sub 3}(pH 4.0) for pH adjustment. After washing the column by 0.01 M NaNO{sub 3} (pH 4.0), Eu was detected and the recovery rate reached 93%. The MAs were then recovered by changing the eluent to 0.01 M NaNO{sub 3} (pH 2.0), and the recovery rate of Am was 48 %. The 10 mol% TPPEN-gel was used to improve adsorption coefficient of Am and a condition of eluent temperature was changed in order to confirm the temperature swing effect on TPEN-gel for MA. More than 90% Eu was detected in the eluent after washing with 0.01 M NaNO{sub 3} (pH 3.5) at 5 Celsius degrees. Americium was backwardly detected and eluted continuously during the same condition. After removal of Eu, the eluent temperature was changed to 32 Celsius degrees, then Am was detected (pH 3.0). Finally remained Am could be stripped from TPPEN-gel by changing the pH of the eluent to 2.0. These results These results prove that the proposed recovery process for MAs is a potential candidate for future reprocessing methods based on the extraction chromatographic technique. (authors)« less

Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides.

PubMed

Allred, Benjamin E; Rupert, Peter B; Gauny, Stacey S; An, Dahlia D; Ralston, Corie Y; Sturzbecher-Hoehne, Manuel; Strong, Roland K; Abergel, Rebecca J

2015-08-18

Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin-transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein-ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications.

The R-Process Alliance: 2MASS J09544277+5246414, the Most Actinide-enhanced R-II Star Known

NASA Astrophysics Data System (ADS)

Holmbeck, Erika M.; Beers, Timothy C.; Roederer, Ian U.; Placco, Vinicius M.; Hansen, Terese T.; Sakari, Charli M.; Sneden, Christopher; Liu, Chao; Lee, Young Sun; Cowan, John J.; Frebel, Anna

2018-06-01

We report the discovery of a new actinide-boost star, 2MASS J09544277+5246414, originally identified as a very bright (V = 10.1), extremely metal-poor ([Fe/H] = ‑2.99) K giant in the LAMOST survey, and found to be highly r-process-enhanced (r-II; [Eu/Fe] = +1.28]), during the snapshot phase of the R-Process Alliance (RPA). Based on a high signal-to-noise ratio (S/N), high-resolution spectrum obtained with the Harlan J. Smith 2.7 m telescope, this star is the first confirmed actinide-boost star found by RPA efforts. With an enhancement of [Th/Eu] = +0.37, 2MASS J09544277+5246414 is also the most actinide-enhanced r-II star yet discovered, and only the sixth metal-poor star with a measured uranium abundance ([U/Fe] = +1.40). Using the Th/U chronometer, we estimate an age of 13.0 ± 4.7 Gyr for this star. The unambiguous actinide-boost signature of this extremely metal-poor star, combined with additional r-process-enhanced and actinide-boost stars identified by the RPA, will provide strong constraints on the nature and origin of the r-process at early times.

Crystal growth methods dedicated to low solubility actinide oxalates

NASA Astrophysics Data System (ADS)

Tamain, C.; Arab-Chapelet, B.; Rivenet, M.; Grandjean, S.; Abraham, F.

2016-04-01

Two novel crystal growth syntheses dedicated to low solubility actinide-oxalate systems and adapted to glove box handling are described. These methods based on the use of precursors of either actinide metal or oxalic acid have been optimized on lanthanide systems (analogue of actinides(III)) and then assessed on real actinide systems. They allow the synthesis of several actinide oxalate single crystals, Am2(C2O4)3(H2O)3·xH2O, Th(C2O4)2·6H2O, M2+x[PuIV2-xPuIIIx(C2O4)5]·nH2O and M1-x[PuIII1-xPuIVx(C2O4)2·H2O]·nH2O. It is the first time that these well-known compounds are formed by crystal growth methods, thus enabling direct structural studies on transuranic element systems and acquisition of basic data beyond deductions from isomorphic (or not) lanthanide compounds. Characterizations by X-ray diffraction, UV-visible solid spectroscopy, demonstrate the potentialities of these two crystal growth methods to obtain oxalate compounds.

Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides

PubMed Central

Allred, Benjamin E.; Rupert, Peter B.; Gauny, Stacey S.; An, Dahlia D.; Ralston, Corie Y.; Sturzbecher-Hoehne, Manuel; Strong, Roland K.; Abergel, Rebecca J.

2015-01-01

Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin–transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein–ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications. PMID:26240330

Colloid-borne forms of tetravalent actinides: A brief review

NASA Astrophysics Data System (ADS)

Zänker, Harald; Hennig, Christoph

2014-02-01

Tetravalent actinides, An(IV), are usually assumed to be little mobile in near-neutral environmental waters because of their low solubility. However, there are certain geochemical scenarios during which mobilization of An(IV) in a colloid-borne (waterborne) form cannot be ruled out. A compilation of colloid-borne forms of tetravalent actinides described so far for laboratory experiments together with several examples of An(IV) colloids observed in field experiments and real-world scenarios are given. They are intended to be a knowledge base and a tool for those who have to interpret actinide behavior under environmental conditions. Synthetic colloids containing structural An(IV) and synthetic colloids carrying adsorbed An(IV) are considered. Their behavior is compared with the behavior of An(IV) colloids observed after the intentional or unintentional release of actinides into the environment. A list of knowledge gaps as to the behavior of An(IV) colloids is provided and items which need further research are highlighted.

ORIGEN-based Nuclear Fuel Inventory Module for Fuel Cycle Assessment: Final Project Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Skutnik, Steven E.

The goal of this project, “ORIGEN-based Nuclear Fuel Depletion Module for Fuel Cycle Assessment" is to create a physics-based reactor depletion and decay module for the Cyclus nuclear fuel cycle simulator in order to assess nuclear fuel inventories over a broad space of reactor operating conditions. The overall goal of this approach is to facilitate evaluations of nuclear fuel inventories for a broad space of scenarios, including extended used nuclear fuel storage and cascading impacts on fuel cycle options such as actinide recovery in used nuclear fuel, particularly for multiple recycle scenarios. The advantages of a physics-based approach (compared tomore » a recipe-based approach which has been typically employed for fuel cycle simulators) is in its inherent flexibility; such an approach can more readily accommodate the broad space of potential isotopic vectors that may be encountered under advanced fuel cycle options. In order to develop this flexible reactor analysis capability, we are leveraging the Origen nuclear fuel depletion and decay module from SCALE to produce a standalone “depletion engine” which will serve as the kernel of a Cyclus-based reactor analysis module. The ORIGEN depletion module is a rigorously benchmarked and extensively validated tool for nuclear fuel analysis and thus its incorporation into the Cyclus framework can bring these capabilities to bear on the problem of evaluating long-term impacts of fuel cycle option choices on relevant metrics of interest, including materials inventories and availability (for multiple recycle scenarios), long-term waste management and repository impacts, etc. Developing this Origen-based analysis capability for Cyclus requires the refinement of the Origen analysis sequence to the point where it can reasonably be compiled as a standalone sequence outside of SCALE; i.e., wherein all of the computational aspects of Origen (including reactor cross-section library processing and interpolation, input and output processing, and depletion/decay solvers) can be self-contained into a single executable sequence. Further, to embed this capability into other software environments (such as the Cyclus fuel cycle simulator) requires that Origen’s capabilities be encapsulated into a portable, self-contained library which other codes can then call directly through function calls, thereby directly accessing the solver and data processing capabilities of Origen. Additional components relevant to this work include modernization of the reactor data libraries used by Origen for conducting nuclear fuel depletion calculations. This work has included the development of new fuel assembly lattices not previously available (such as for CANDU heavy-water reactor assemblies) as well as validation of updated lattices for light-water reactors updated to employ modern nuclear data evaluations. The CyBORG reactor analysis module as-developed under this workscope is fully capable of dynamic calculation of depleted fuel compositions from all commercial U.S. reactor assembly types as well as a number of international fuel types, including MOX, VVER, MAGNOX, and PHWR CANDU fuel assemblies. In addition, the Origen-based depletion engine allows for CyBORG to evaluate novel fuel assembly and reactor design types via creation of Origen reactor data libraries via SCALE. The establishment of this new modeling capability affords fuel cycle modelers a substantially improved ability to model dynamically-changing fuel cycle and reactor conditions, including recycled fuel compositions from fuel cycle scenarios involving material recycle into thermal-spectrum systems.« less

Systematization of actinides using cluster analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kopyrin, A.A.; Terent`eva, T.N.; Khramov, N.N.

1994-11-01

A representation of the actinides in multidimensional property space is proposed for systematization of these elements using cluster analysis. Literature data for their atomic properties are used. Owing to the wide variation of published ionization potentials, medians are used to estimate them. Vertical dendograms are used for classification on the basis of distances between the actinides in atomic-property space. The properties of actinium and lawrencium are furthest removed from the main group. Thorium and mendelevium exhibit individualized properties. A cluster based on the einsteinium-fermium pair is joined by californium.

Actinide-contaminated Skin: Comparing Decontamination Efficacy of Water, Cleansing Gels, and DTPA Gels.

PubMed

Tazrart, A; Bolzinger, M A; Lamart, S; Coudert, S; Angulo, J F; Jandard, V; Briançon, S; Griffiths, N M

2018-07-01

Skin contamination by alpha-emitting actinides is a risk to workers during nuclear fuel production and reactor decommissioning. Also, the list of items for potential use in radiological dispersal devices includes plutonium and americium. The actinide chemical form is important and solvents such as tributyl phosphate, used to extract plutonium, can influence plutonium behavior. This study investigated skin fixation and efficacy of decontamination products for these actinide forms using viable pig skin in the Franz cell diffusion system. Commonly used or recommended decontamination products such as water, cleansing gel, diethylenetriamine pentaacetic acid, or octadentate hydroxypyridinone compound 3,4,3-LI(1,2-HOPO), as well as diethylenetriamine pentaacetic acid hydrogel formulations, were tested after a 2-h contact time with the contaminant. Analysis of skin samples demonstrated that more plutonium nitrate is bound to skin as compared to plutonium-tributyl phosphate, and fixation of americium to skin was also significant. The data show that for plutonium-tributyl phosphate all the products are effective ranging from 80 to 90% removal of this contaminant. This may be associated with damage to the skin by this complex and suggests a mechanical/wash-out action rather than chelation. For removal of americium and plutonium, both Trait Rouge cleansing gel and diethylenetriamine pentaacetic acid are better than water, and diethylenetriamine pentaacetic acid hydrogel is better than Osmogel. The different treatments, however, did not significantly affect the activity in deeper skin layers, which suggests a need for further improvement of decontamination procedures. The new diethylenetriamine pentaacetic acid hydrogel preparation was effective in removing americium, plutonium, and plutonium-tributyl phosphate from skin; such a formulation offers advantages and thus merits further assessment.

Revisiting the diffusion mechanism of helium in UO 2 : A DFT+ U study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, X. -Y.; Andersson, D. A.

The understanding of migration properties of helium atoms after their generation through α-decay of actinides in spent nuclear fuels is important for the safety of nuclear fuel storage and disposal. The diffusion of helium in UO 2 is revisited by using the DFT+U simulation methodology employing the “U-ramping” method to address the issue of metastable energy states. A novel diffusion mechanism by helium interstitials, the “asymmetric hop” mechanism, is reported and compared to other diffusion mechanisms including an oxygen vacancy mediated mechanism and available experimental diffusion data. We show that the new mechanism is the dominant one over a widemore » temperature range.« less

Revisiting the diffusion mechanism of helium in UO 2 : A DFT+ U study

DOE PAGES

Liu, X. -Y.; Andersson, D. A.

2017-11-03

The understanding of migration properties of helium atoms after their generation through α-decay of actinides in spent nuclear fuels is important for the safety of nuclear fuel storage and disposal. The diffusion of helium in UO 2 is revisited by using the DFT+U simulation methodology employing the “U-ramping” method to address the issue of metastable energy states. A novel diffusion mechanism by helium interstitials, the “asymmetric hop” mechanism, is reported and compared to other diffusion mechanisms including an oxygen vacancy mediated mechanism and available experimental diffusion data. We show that the new mechanism is the dominant one over a widemore » temperature range.« less

Monte Carlo Shielding Comparative Analysis Applied to TRIGA HEU and LEU Spent Fuel Transport

NASA Astrophysics Data System (ADS)

Margeanu, C. A.; Margeanu, S.; Barbos, D.; Iorgulis, C.

2010-12-01

The paper is a comparative study of LEU and HEU fuel utilization effects for the shielding analysis during spent fuel transport. A comparison against the measured data for HEU spent fuel, available from the last stage of spent fuel repatriation fulfilled in the summer of 2008, is also presented. All geometrical and material data for the shipping cask were considered according to NAC-LWT Cask approved model. The shielding analysis estimates radiation doses to shipping cask wall surface, and in air at 1 m and 2 m, respectively, from the cask, by means of 3D Monte Carlo MORSE-SGC code. Before loading into the shipping cask, TRIGA spent fuel source terms and spent fuel parameters have been obtained by means of ORIGEN-S code. Both codes are included in ORNL's SCALE 5 programs package. The actinides contribution to total fuel radioactivity is very low in HEU spent fuel case, becoming 10 times greater in LEU spent fuel case. Dose rates for both HEU and LEU fuel contents are below regulatory limits, LEU spent fuel photon dose rates being greater than HEU ones. Comparison between HEU spent fuel theoretical and measured dose rates in selected measuring points shows a good agreement, calculated values being greater than the measured ones both to cask wall surface (about 34% relative difference) and in air at 1 m distance from cask surface (about 15% relative difference).

Extraction of lanthanides using 1-hydroxy-6- N-octylcarboxamido-2(1 H)-pyridinone as an extractant via competitive ligand complexations between aqueous and organic phases

DOE PAGES

Williams, Neil J.; Do-Thanh, Chi -Linh; Stankovich, Joseph J.; ...

2015-12-10

Here, the ability to selectively extract lanthanides is crucial in hydrometallurgy and the nuclear fuel cycle. The capabilities of 1-hydroxy-6- N-octylcarboxamido-2(1 H)-pyridinone (octyl-HOPO) as an extractant for the separation of lanthanides and actinides were studied for the first time. Octyl-HOPO greatly outperformed the traditional ligand di-2-ethylhexyl phosphoric acid (DEHPA).

Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling

DOE PAGES

Burns, Jonathan D.; Moyer, Bruce A.

2016-08-17

Hexavalent Np, Pu, and Am individually, and as a group, have all been cocrystallized with UO 2(NO 3) 2∙ 6H 2O, constituting the first demonstration of an An(VI) group cocrystalliza- tion. The hexavalent dioxo cations of Np, Pu, and Am cocrystallize with UO 2(NO 3) 2∙ 6H 2O in near proportion with a simple reduction in temperature, while the lower valence states, An(III) and An(IV), are only slightly removed from solution. A separation of An(VI) species from An(III) ions by crystallization has been demonstrated, with an observed separation factor of 14. Separation of An(VI) species from key fission products, 95Zr,more » 95Nb, 137Cs, and 144Ce, has also been demonstrated by crystallization, with separation factors ranging from 6.5 to 71 in the absence of Am(VI), while in the presence of Am(VI), the separation factors were reduced to 0.99 7.7. One interesting observation is that Am(VI) shows increased stability in the cocrystallized form, with no reduction observed after 13 days, as opposed to in solution, in which >50% is reduced after only 10 days. The ability to cocrystallize and stabilize hexavalent actinides from solution, especially Am(VI), introduces a new separations approach that can be applied to closing the nuclear fuel cycle.« less

Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Burns, Jonathan D.; Moyer, Bruce A.

Hexavalent Np, Pu, and Am individually, and as a group, have all been cocrystallized with UO 2(NO 3) 2∙ 6H 2O, constituting the first demonstration of an An(VI) group cocrystalliza- tion. The hexavalent dioxo cations of Np, Pu, and Am cocrystallize with UO 2(NO 3) 2∙ 6H 2O in near proportion with a simple reduction in temperature, while the lower valence states, An(III) and An(IV), are only slightly removed from solution. A separation of An(VI) species from An(III) ions by crystallization has been demonstrated, with an observed separation factor of 14. Separation of An(VI) species from key fission products, 95Zr,more » 95Nb, 137Cs, and 144Ce, has also been demonstrated by crystallization, with separation factors ranging from 6.5 to 71 in the absence of Am(VI), while in the presence of Am(VI), the separation factors were reduced to 0.99 7.7. One interesting observation is that Am(VI) shows increased stability in the cocrystallized form, with no reduction observed after 13 days, as opposed to in solution, in which >50% is reduced after only 10 days. The ability to cocrystallize and stabilize hexavalent actinides from solution, especially Am(VI), introduces a new separations approach that can be applied to closing the nuclear fuel cycle.« less

Development of Xe and Kr empirical potentials for CeO 2, ThO 2, UO 2 and PuO 2, combining DFT with high temperature MD

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cooper, M. W. D.; Kuganathan, N.; Burr, P. A.

In this study, the development of embedded atom method (EAM) many-body potentials for actinide oxides and associated mixed oxide (MOX) systems has motivated the development of a complementary parameter set for gas-actinide and gas-oxygen interactions. A comprehensive set of density functional theory (DFT) calculations were used to study Xe and Kr incorporation at a number of sites in CeO 2, ThO 2, UO 2 and PuO 2. These structures were used to fit a potential, which was used to generate molecular dynamics (MD) configurations incorporating Xe and Kr at 300 K, 1500 K, 3000 K and 5000 K. Subsequent matchingmore » to the forces predicted by DFT for these MD configurations was used to refine the potential set. This fitting approach ensured weighted fitting to configurations that are thermodynamically significant over a broad temperature range, while avoiding computationally expensive DFT-MD calculations. The resultant gas potentials were validated against DFT trapping energies and are suitable for simulating combinations of Xe and Kr in solid solutions of CeO 2, ThO 2, UO 2 and PuO 2, providing a powerful tool for the atomistic simulation of conventional nuclear reactor fuel UO 2 as well as advanced MOX fuels.« less

Development of Xe and Kr empirical potentials for CeO 2, ThO 2, UO 2 and PuO 2, combining DFT with high temperature MD

DOE PAGES

Cooper, M. W. D.; Kuganathan, N.; Burr, P. A.; ...

2016-08-23

In this study, the development of embedded atom method (EAM) many-body potentials for actinide oxides and associated mixed oxide (MOX) systems has motivated the development of a complementary parameter set for gas-actinide and gas-oxygen interactions. A comprehensive set of density functional theory (DFT) calculations were used to study Xe and Kr incorporation at a number of sites in CeO 2, ThO 2, UO 2 and PuO 2. These structures were used to fit a potential, which was used to generate molecular dynamics (MD) configurations incorporating Xe and Kr at 300 K, 1500 K, 3000 K and 5000 K. Subsequent matchingmore » to the forces predicted by DFT for these MD configurations was used to refine the potential set. This fitting approach ensured weighted fitting to configurations that are thermodynamically significant over a broad temperature range, while avoiding computationally expensive DFT-MD calculations. The resultant gas potentials were validated against DFT trapping energies and are suitable for simulating combinations of Xe and Kr in solid solutions of CeO 2, ThO 2, UO 2 and PuO 2, providing a powerful tool for the atomistic simulation of conventional nuclear reactor fuel UO 2 as well as advanced MOX fuels.« less

Quantum Chemical Studies of Actinides and Lanthanides: From Small Molecules to Nanoclusters

NASA Astrophysics Data System (ADS)

Vlaisavljevich, Bess

Research into actinides is of high interest because of their potential applications as an energy source and for the environmental implications therein. Global concern has arisen since the development of the actinide concept in the 1940s led to the industrial scale use of the commercial nuclear energy cycle and nuclear weapons production. Large quantities of waste have been generated from these processes inspiring efforts to address fundamental questions in actinide science. In this regard, the objective of this work is to use theory to provide insight and predictions into actinide chemistry, where experimental work is extremely challenging because of the intrinsic difficulties of the experiments themselves and the safety issues associated with this type of chemistry. This thesis is a collection of theoretical studies of actinide chemistry falling into three categories: quantum chemical and matrix isolation studies of small molecules, the electronic structure of organoactinide systems, and uranyl peroxide nanoclusters and other solid state actinide compounds. The work herein not only spans a wide range of systems size but also investigates a range of chemical problems. Various quantum chemical approaches have been employed. Wave function-based methods have been used to study the electronic structure of actinide containing molecules of small to middle-size. Among these methods, the complete active space self consistent field (CASSCF) approach with corrections from second-order perturbation theory (CASPT2), the generalized active space SCF (GASSCF) approach, and Moller-Plesset second-order perturbation theory (MP2) have been employed. Likewise, density functional theory (DFT) has been used along with analysis tools like bond energy decomposition, bond orders, and Bader's Atoms in Molecules. From these quantum chemical results, comparison with experimentally obtained structures and spectra are made.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maloy, Stuart Andrew; Pestovich, Kimberly Shay; Anderoglu, Osman

The Fuel Cycle Research and Development program is investigating methods of transmuting minor actinides in various fuel cycle options. To achieve this goal, new fuels and cladding materials must be developed and tested to high burnup levels (e.g. >20%) requiring cladding to withstand very high doses (greater than 200 dpa) while in contact with the coolant and the fuel. To develop and qualify materials to a total fluence greater than 200 dpa requires development of advanced alloys and irradiations in fast reactors to test these alloys. Recent results from testing numerous ferritic/martensitic steels at low temperatures suggest that improvements inmore » low temperature radiation tolerance can be achieved through carefully controlling the nitrogen content in these alloys. Thus, four new heats of HT-9 were produced with controlled nitrogen content: two by Metalwerks and two by Sophisticated Alloys. Initial results on these new alloys are presented including microstructural analysis and hardness testing. Future testing will include irradiation testing with ions and in reactor.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Han, Bo-Young; Choi, Daewoong; Park, Se Hwan

Korea Atomic Energy Research Institute (KAERI) have been developing the design and deployment methodology of Laser- Induced Breakdown Spectroscopy (LIBS) instrument for safeguards application within the argon hot cell environment at Advanced spent fuel Conditioning Process Facility (ACPF), where ACPF is a facility being refurbished for the laboratory-scaled demonstration of advanced spent fuel conditioning process. LIBS is an analysis technology used to measure the emission spectra of excited elements in the local plasma of a target material induced by a laser. The spectra measured by LIBS are analyzed to verify the quality and quantity of the specific element in themore » target matrix. Recently LIBS has been recognized as a promising technology for safeguards purposes in terms of several advantages including a simple sample preparation and in-situ analysis capability. In particular, a feasibility study of LIBS to remotely monitor the nuclear material in a high radiation environment has been carried out for supporting the IAEA safeguards implementation. Fiber-Optic LIBS (FO-LIBS) deployment was proposed by Applied Photonics Ltd because the use of fiber optics had benefited applications of LIBS by delivering the laser energy to the target and by collecting the plasma light. The design of FO-LIBS instrument for the measurement of actinides in the spent fuel and high temperature molten salt at ACPF had been developed in cooperation with Applied Photonics Ltd. FO-LIBS has some advantages as followings: the detectable plasma light wavelength range is not limited by the optical properties of the thick lead-glass shield window and the potential risk of laser damage to the lead-glass shield window is not considered. The remote LIBS instrument had been installed at ACPF and then the feasibility study for monitoring actinide elements such as uranium, plutonium, and curium in process materials has been carried out. (authors)« less

Implications of Fast Reactor Transuranic Conversion Ratio

DOE Office of Scientific and Technical Information (OSTI.GOV)

Steven J. Piet; Edward A. Hoffman; Samuel E. Bays

2010-11-01

Theoretically, the transuranic conversion ratio (CR), i.e. the transuranic production divided by transuranic destruction, in a fast reactor can range from near zero to about 1.9, which is the average neutron yield from Pu239 minus 1. In practice, the possible range will be somewhat less. We have studied the implications of transuranic conversion ratio of 0.0 to 1.7 using the fresh and discharge fuel compositions calculated elsewhere. The corresponding fissile breeding ratio ranges from 0.2 to 1.6. The cases below CR=1 (“burners”) do not have blankets; the cases above CR=1 (“breeders”) have breeding blankets. The burnup was allowed to floatmore » while holding the maximum fluence to the cladding constant. We graph the fuel burnup and composition change. As a function of transuranic conversion ratio, we calculate and graph the heat, gamma, and neutron emission of fresh fuel; whether the material is “attractive” for direct weapon use using published criteria; the uranium utilization and rate of consumption of natural uranium; and the long-term radiotoxicity after fuel discharge. For context, other cases and analyses are included, primarily once-through light water reactor (LWR) uranium oxide fuel at 51 MWth-day/kg-iHM burnup (UOX-51). For CR<1, the heat, gamma, and neutron emission increase as material is recycled. The uranium utilization is at or below 1%, just as it is in thermal reactors as both types of reactors require continuing fissile support. For CR>1, heat, gamma, and neutron emission decrease with recycling. The uranium utilization exceeds 1%, especially as all the transuranic elements are recycled. exceeds 1%, especially as all the transuranic elements are recycled. At the system equilibrium, heat and gamma vary by somewhat over an order of magnitude as a function of CR. Isotopes that dominate heat and gamma emission are scattered throughout the actinide chain, so the modest impact of CR is unsurprising. Neutron emitters are preferentially found among the higher actinides, so the neutron emission varies much stronger with CR, about three orders of magnitude.« less

Porous membrane electrochemical cell for uranium and transuranic recovery from molten salt electrolyte

DOEpatents

Willit, James L [Ratavia, IL

2007-09-11

An improved process and device for the recovery of the minor actinides and the transuranic elements (TRU's) from a molten salt electrolyte. The process involves placing the device, an electrically non-conducting barrier between an anode salt and a cathode salt. The porous barrier allows uranium to diffuse between the anode and cathode, yet slows the diffusion of uranium ions so as to cause depletion of uranium ions in the catholyte. This allows for the eventual preferential deposition of transuranics present in spent nuclear fuel such as Np, Pu, Am, Cm. The device also comprises an uranium oxidation anode. The oxidation anode is solid uranium metal in the form of spent nuclear fuel. The spent fuel is placed in a ferric metal anode basket which serves as the electrical lead or contact between the molten electrolyte and the anodic uranium metal.

Porous membrane electrochemical cell for uranium and transuranic recovery from molten salt electrolyte

DOEpatents

Willit, James L [Batavia, IL

2010-09-21

An improved process and device for the recovery of the minor actinides and the transuranic elements (TRU's) from a molten salt electrolyte. The process involves placing the device, an electrically non-conducting barrier between an anode salt and a cathode salt. The porous barrier allows uranium to diffuse between the anode and cathode, yet slows the diffusion of uranium ions so as to cause depletion of uranium ions in the catholyte. This allows for the eventual preferential deposition of transuranics present in spent nuclear fuel such as Np, Pu, Am, Cm. The device also comprises an uranium oxidation anode. The oxidation anode is solid uranium metal in the form of spent nuclear fuel. The spent fuel is placed in a ferric metal anode basket which serves as the electrical lead or contact between the molten electrolyte and the anodic uranium metal.

Swelling induced by alpha decay in monazite and zirconolite ceramics: A XRD and TEM comparative study

NASA Astrophysics Data System (ADS)

Deschanels, X.; Seydoux-Guillaume, A. M.; Magnin, V.; Mesbah, A.; Tribet, M.; Moloney, M. P.; Serruys, Y.; Peuget, S.

2014-05-01

Zirconolite and monazite matrices are potential ceramics for the containment of actinides (Np, Cm, Am, Pu) which are produced over the reprocessing of spent nuclear fuel. Actinides decay mainly through the emission of alpha particles, which in turn causes most ceramics to undergo structural and textural changes (amorphization and/or swelling). In order to study the effects of alpha decays on the above mentioned ceramics two parallel approaches were set up. The first involved the use of an external irradiation source, Au, which allowed the deposited recoil energy to be simulated. The second was based on short-lived actinide doping with 238Pu, (i.e. an internal source), via the incorporation of plutonium oxide into both the monazite and zirconolite structures during synthesis. In both types of irradiation experiments, the zirconolite samples became amorphous at room temperature with damage close to 0.3 dpa; corresponding to a critical dose of 4 × 1018 α g-1 (i.e. ∼1.3 × 1021 keV cm-3). Both zirconolite samples also showed the same degree of macroscopic swelling at saturation (∼6%), with ballistic processes being the predominant damaging effect. In the case of the monazite however, the macroscopic swelling and amorphization were dependent on the nature of the irradiation. Externally, (Au), irradiated samples became amorphous while also demonstrating a saturation swelling of up to 8%. In contrast to this, the swelling of the 238Pu doped samples was much smaller at ∼1%. Also, unlike the externally (Au) irradiated monazite these 238Pu doped samples remained crystalline up to 7.5 × 1018 α g-1 (0.8 dpa). XRD, TEM and swelling measurements were used to fully characterize and interpret this behavior. The low swelling and the conservation of the crystalline state of 238Pu doped monazite samples indicates that alpha annealing took place within this material.

Non-equilibrium radiation nuclear reactor

NASA Technical Reports Server (NTRS)

Thom, K.; Schneider, R. T. (Inventor)

1978-01-01

An externally moderated thermal nuclear reactor is disclosed which is designed to provide output power in the form of electromagnetic radiation. The reactor is a gaseous fueled nuclear cavity reactor device which can operate over wide ranges of temperature and pressure, and which includes the capability of processing and recycling waste products such as long-lived transuranium actinides. The primary output of the device may be in the form of coherent radiation, so that the reactor may be utilized as a self-critical nuclear pumped laser.

REGENERATION OF REACTOR FUEL ELEMENTS

DOEpatents

Lyon, W.L.

1960-04-01

A process is described for concentrating uranium and/or plutonium metal in aluminum alloys in which the actinide content was partially consumed by neutron bombardinent. Two embodiments are claimed: Either the alloy is heated, together with zinc chloride to at least 1000 deg C whereby some aluminum, in the form of aluminum chloride, and any zinc formed volatilize; or else aluminum fluoride is added and reacted at 800 to 1000 deg O and substmospheric pressure whereby pant of the aluminum volatilizes and aluminum subfluoride.

X-ray backscatter imaging of nuclear materials

DOEpatents

Chapman, Jeffrey Allen; Gunning, John E; Hollenbach, Daniel F; Ott, Larry J; Shedlock, Daniel

2014-09-30

The energy of an X-ray beam and critical depth are selected to detect structural discontinuities in a material having an atomic number Z of 57 or greater. The critical depth is selected by adjusting the geometry of a collimator that blocks backscattered radiation so that backscattered X-ray originating from a depth less than the critical depth is not detected. Structures of Lanthanides and Actinides, including nuclear fuel rod materials, can be inspected for structural discontinuities such as gaps, cracks, and chipping employing the backscattered X-ray.

Measurement system for alpha emitters in solution

NASA Astrophysics Data System (ADS)

Robert, A.; Sella, C.; Heindl, R.

1984-08-01

The measurement of alpha emitter concentrations in solution corresponds to a need felt in particular by laboratories working on actinides and in the spent fuel reprocessing industry. The instrument present here allows this measurement continuously by the use of a new scintillator that is insensitive to corrosive liquids. The extreme thinness of the scintillator guarantees good detection selectivity of alpha particles in the presence of beta and gamma emissions. Examples of uranium-233, plutonium-239 and americium-241 concentration measurements are presented.

Addressing Fission Product Validation in MCNP Burnup Credit Criticality Calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mueller, Don; Bowen, Douglas G; Marshall, William BJ J

2015-01-01

The US Nuclear Regulatory Commission (NRC) Division of Spent Fuel Storage and Transportation issued Interim Staff Guidance (ISG) 8, Revision 3 in September 2012. This ISG provides guidance for NRC staff members’ review of burnup credit (BUC) analyses supporting transport and dry storage of pressurized water reactor spent nuclear fuel (SNF) in casks. The ISG includes guidance for addressing validation of criticality (k eff) calculations crediting the presence of a limited set of fission products and minor actinides (FP&MAs). Based on previous work documented in NRC Regulatory Guide (NUREG) Contractor Report (CR)-7109, the ISG recommends that NRC staff members acceptmore » the use of either 1.5 or 3% of the FP&MA worth—in addition to bias and bias uncertainty resulting from validation of k eff calculations for the major actinides in SNF—to conservatively account for the bias and bias uncertainty associated with the specified unvalidated FP&MAs. The ISG recommends (1) use of 1.5% of the FP&MA worth if a modern version of SCALE and its nuclear data are used and (2) 3% of the FP&MA worth for well qualified, industry standard code systems other than SCALE with the Evaluated Nuclear Data Files, Part B (ENDF/B),-V, ENDF/B-VI, or ENDF/B-VII cross sections libraries. The work presented in this paper provides a basis for extending the use of the 1.5% of the FP&MA worth bias to BUC criticality calculations performed using the Monte Carlo N-Particle (MCNP) code. The extended use of the 1.5% FP&MA worth bias is shown to be acceptable by comparison of FP&MA worths calculated using SCALE and MCNP with ENDF/B-V, -VI, and -VII–based nuclear data. The comparison supports use of the 1.5% FP&MA worth bias when the MCNP code is used for criticality calculations, provided that the cask design is similar to the hypothetical generic BUC-32 cask model and that the credited FP&MA worth is no more than 0.1 Δk eff (ISG-8, Rev. 3, Recommendation 4).« less

The chemical state of defective uranium-plutonium oxide fuel pins irradiated in sodium cooled reactors

NASA Astrophysics Data System (ADS)

Kleykamp, H.

1997-09-01

Steady-state irradiation experiments were conducted in the sodium loop of the Siloe reactor on artificially failed mixed oxide pins that had been pre-irradiated in fast reactors up to 11.5% burnup. The formation of the predominant reaction product Na 3(U,Pu)O 4 starts on the fuel surface and is terminated when a lower O/(U + Pu) threshold of the fuel is attained. The axial extent of the reaction product depends on the size of the initial cladding defect. The occurrence of secondary cracks is possible. Na(U,Pu)O 3 forms at higher fuel temperatures. The existence of Na 3U 1- xPu xO 4 is shown in pre-irradiated blanket pins after artificial defect formation. Caesium in the oxocompounds is reduced to the metallic state and is dissolved in the coolant. Evidence of a very low chemical potential of oxygen in defective fuel pins is sustained by the occurrence of actinide-platinum metal phases formed by coupled reduction of hypostoichiometric fuel with ɛ-(Mo,Tc,Ru,Rh,Pd) precipitates. Continued operation of defective pins is not hazardous by easy precautions.

Extraction of Trivalent Actinides and Lanthanides from Californium Campaign Rework Solution Using TODGA-based Solvent Extraction System

DOE Office of Scientific and Technical Information (OSTI.GOV)

Benker, Dennis; Delmau, Laetitia Helene; Dryman, Joshua Cory

This report presents the studies carried out to demonstrate the possibility of quantitatively extracting trivalent actinides and lanthanides from highly acidic solutions using a neutral ligand-based solvent extraction system. These studies stemmed from the perceived advantage of such systems over cationexchange- based solvent extraction systems that require an extensive feed adjustment to make a low-acid feed. The targeted feed solutions are highly acidic aqueous phases obtained after the dissolution of curium targets during a californium (Cf) campaign. Results obtained with actual Cf campaign solutions, but highly diluted to be manageable in a glove box, are presented, followed by results ofmore » tests run in the hot cells with Cf campaign rework solutions. It was demonstrated that a solvent extraction system based on the tetraoctyl diglycolamide molecule is capable of quantitatively extracting trivalent actinides from highly acidic solutions. This system was validated using actual feeds from a Cf campaign.« less

Impact of the deployment schedule of fast breeding reactors in the frame of French act for nuclear materials and radioactive waste management

DOE Office of Scientific and Technical Information (OSTI.GOV)

Le Mer, J.; Garzenne, C.; Lemasson, D.

In the frame of the French Act of June 28, 2006 on 'a sustainable management of nuclear materials and radioactive waste' EDF R and D assesses various research scenarios of transition between the actual French fleet and a Generation IV fleet with a closed fuel cycle where plutonium is multi-recycled. The basic scenarios simulate a deployment of 60 GWe of Sodium-cooled Fast Reactors (SFRs) in two steps: one third from 2040 to 2050 and the rest from 2080 to 2100 (scenarios 2040). These research scenarios assume that SFR technology will be ready for industrial deployment in 2040. One of themore » many sensitivity analyses that EDF, as a nuclear power plant operator, must evaluate is the impact of a delay of SFR technology in terms of uranium consumptions, plutonium needs and fuel cycle utilities gauging. The sensitivity scenarios use the same assumptions as scenarios 2040 but they simulate a different transition phase: SFRs are deployed in one step between 2080 and 2110 (scenarios 2080). As the French Act states to conduct research on minor actinides (MA) management, we studied different options for 2040 and 2080 scenarios: no MA transmutation, americium transmutation in heterogeneous mode based on americium Bearing Blankets (AmBB) in SFRs and all MA transmutation in heterogeneous mode based on MA Bearing Blankets (MABB). Moreover, we studied multiple parameters that could impact the deployment of these reactors (SFR load factor, increase of the use of MOX in Light Water Reactors, increase of the cooling time in spent nuclear fuel storage...). Each scenario has been computed with the EDF R and D fuel cycle simulation code TIRELIRE-STRATEGIE and optimized to meet various fuel cycle constraints such as using the reprocessing facility with long period of constant capacity, keeping the temporary stored mass of plutonium and MA under imposed limits, recycling older assemblies first... These research scenarios show that the transition from the current PWR fleet to an equivalent fleet of Generation IV SFR can follow different courses. The design of SFR-V2B that we used in our studies needs a high inventory of plutonium resulting in tension on this resource. Several options can be used in order to loosen this tension: our results lead to favour the use of axial breeding blanket in SFR. Load factor of upcoming reactors has to be regarded with attention as it has a high impact on plutonium resource for a given production of electricity. The deployment of SFRs beginning in 2080 instead of 2040 following the scenarios we described creates higher tensions on reprocessing capacity, separated plutonium storage and spent fuel storage. In the frame of the French Act, we studied minor actinides transmutation. The flux of MA in all fuel cycle plants is really high, which will lead to decay heat, a and neutron emission related problems. In terms of reduction of MA inventories, the deployment of MA transmutation cycle must not delay the installation of SFRs. The plutonium production in MABB and AmBB does not allow reducing the use of axial breeding blankets. The impact of MA or Am transmutation over the high level waste disposal is more important if the SFRs are deployed later. Transmutation option (americium or all MA) does not have a significant impact on the number of canister produced nor on its long-term thermal properties. (authors)« less

Thermal Conductivity of Metallic Uranium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hin, Celine

This project has developed a modeling and simulation approaches to predict the thermal conductivity of metallic fuels and their alloys. We focus on two methods. The first method has been developed by the team at the University of Wisconsin Madison. They developed a practical and general modeling approach for thermal conductivity of metals and metal alloys that integrates ab-initio and semi-empirical physics-based models to maximize the strengths of both techniques. The second method has been developed by the team at Virginia Tech. This approach consists of a determining the thermal conductivity using only ab-initio methods without any fitting parameters. Bothmore » methods were complementary. The models incorporated both phonon and electron contributions. Good agreement with experimental data over a wide temperature range were found. The models also provided insight into the different physical factors that govern the thermal conductivity under different temperatures. The models were general enough to incorporate more complex effects like additional alloying species, defects, transmutation products and noble gas bubbles to predict the behavior of complex metallic alloys like U-alloy fuel systems under burnup. 3 Introduction Thermal conductivity is an important thermal physical property affecting the performance and efficiency of metallic fuels [1]. Some experimental measurement of thermal conductivity and its correlation with composition and temperature from empirical fitting are available for U, Zr and their alloys with Pu and other minor actinides. However, as reviewed in by Kim, Cho and Sohn [2], due to the difficulty in doing experiments on actinide materials, thermal conductivities of metallic fuels have only been measured at limited alloy compositions and temperatures, some of them even being negative and unphysical. Furthermore, the correlations developed so far are empirical in nature and may not be accurate when used for prediction at conditions far from those used in the original fitting. Moreover, as fuels burn up in the reactor and fission products are built up, thermal conductivity is also significantly changed [3]. Unfortunately, fundamental understanding of the effect of fission products is also currently lacking. In this project, we probe thermal conductivity of metallic fuels with ab initio calculations, a theoretical tool with the potential to yield better accuracy and predictive power than empirical fitting. This work will both complement experimental data by determining thermal conductivity in wider composition and temperature ranges than is available experimentally, and also develop mechanistic understanding to guide better design of metallic fuels in the future. So far, we focused on α-U perfect crystal, the ground-state phase of U metal. We focus on two methods. The first method has been developed by the team at the University of Wisconsin Madison. They developed a practical and general modeling approach for thermal conductivity of metals and metal alloys that integrates ab-initio and semi-empirical physics-based models to maximize the strengths of both techniques. The second method has been developed by the team at Virginia Tech. This approach consists of a determining the thermal conductivity using only ab-initio methods without any fitting parameters. Both methods were complementary and very helpful to understand the physics behind the thermal conductivity in metallic uranium and other materials with similar characteristics. In Section I, the combined model developed at UWM is explained. In Section II, the ab-initio method developed at VT is described along with the uranium pseudo-potential and its validation. Section III is devoted to the work done by Jianguo Yu at INL. Finally, we will present the performance of the project in terms of milestones, publications, and presentations.« less

Quantification of Cation Sorption to Engineered Barrier Materials Under Extreme Conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Powell, Brian; Schlautman, Mark; Rao, Linfeng

The objective of this research is to examine mechanisms and thermodynamics of actinide sorption to engineered barrier materials (iron (oxyhydr)oxides and bentonite clay) for nuclear waste repositories under high temperature and high ionic strength conditions using a suite of macroscopic and microscopic techniques which will be coupled with interfacial reaction models. Gaining a mechanistic understanding of interfacial processes governing the sorption/sequestration of actinides at mineral-water interfaces is fundamental for the accurate prediction of actinide behavior in waste repositories. Although macroscale sorption data and various spectroscopic techniques have provided valuable information regarding speciation of actinides at solid-water interfaces, significant knowledge gapsmore » still exist with respect to sorption mechanisms and the ability to quantify sorption, particularly at high temperatures and ionic strengths. This objective is addressed through three major tasks: (1) influence of oxidation state on actinide sorption to iron oxides and clay minerals at elevated temperatures and ionic strengths; (2) calorimetric titrations of actinide-mineral suspensions; (3) evaluation of bentonite performance under repository conditions. The results of the work will include a qualitative conceptual model and a quantitative thermodynamic speciation model describing actinide partitioning to minerals and sediments, which is based upon a mechanistic understanding of specific sorption processes as determined from both micro-scale and macroscale experimental techniques. The speciation model will be a thermodynamic aqueous and surface complexation model of actinide interactions with mineral surfaces that is self-consistent with macroscopic batch sorption data, calorimetric and potentiometric titrations, X-ray absorption Spectroscopy (XAS, mainly Extended X-ray Absorption Fine Structure (EXAFS)), and electron microscopy analyses. The novelty of the proposed work lies largely in the unique system conditions which will be examined (i.e. elevated temperature and ionic strength) and the manner in which the surface complexation model will be developed in terms of specific surface species identified using XAS. These experiments will thus provide a fundamental understanding of the chemical and physical processes occurring at the solid-solution interface under expected repository conditions. Additionally, the focus on thermodynamic treatment of actinide ion interactions with minerals as proposed will provide information on the driving forces involved and contribute to the overall understanding of the high affinity many actinide ions have for oxide surfaces. The utility of this model will be demonstrated in this work through a series of advective and diffusive flow experiments.« less

Multifaceted Modularity: A Key for Stepwise Building of Hierarchical Complexity in Actinide Metal–Organic Frameworks

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dolgopolova, Ekaterina A.; Ejegbavwo, Otega A.; Martin, Corey R.

Growing necessity for efficient nuclear waste management is a driving force for development of alternative architectures towards fundamental understanding of mechanisms involved in actinide integration inside extended structures. In this manuscript, metal-organic frameworks (MOFs) were investigated as a model system for engineering radionuclide containing materials through utilization of unprecedented MOF modularity, which cannot be replicated in any other type of materials. Through the implementation of recent synthetic advances in the MOF field, hierarchical complexity of An-materials were built stepwise, which was only feasible due to preparation of the first examples of actinide-based frameworks with “unsaturated” metal nodes. The first successfulmore » attempts of solid-state metathesis and metal node extension in An-MOFs are reported, and the results of the former approach revealed drastic differences in chemical behavior of extended structures versus molecular species. Successful utilization of MOF modularity also allowed us to structurally characterize the first example of bimetallic An-An nodes. To the best of our knowledge, through combination of solid-state metathesis, guest incorporation, and capping linker installation, we were able to achieve the highest Th wt% in mono- and bi-actinide frameworks with minimal structural density. Overall, combination of a multistep synthetic approach with homogeneous actinide distribution and moderate solvothermal conditions could make MOFs an exceptionally powerful tool to address fundamental questions responsible for chemical behavior of An-based extended structures, and therefore, shed light on possible optimization of nuclear waste administration.« less

Actinide geochemistry: from the molecular level to the real system.

PubMed

Geckeis, Horst; Rabung, Thomas

2008-12-12

Geochemical processes leading to either mobilization or retention of radionuclides in an aquifer system are significantly influenced by their interaction with rock, sediment and colloid surfaces. Therefore, a sound safety assessment of nuclear waste disposal requires the elucidation and quantification of those processes. State-of-the-art analytical techniques as e.g. laser- and X-ray spectroscopy are increasingly applied to study solid-liquid interface reactions to obtain molecular level speciation insight. We have studied the sorption of trivalent lanthanides and actinides onto aluminium oxides, hydroxides and purified clay minerals by the time-resolved laser fluorescence spectroscopy and X-ray-absorption spectroscopy. Chemical constitution and structure of surface bound actinides are proposed based on spectroscopic information. Open questions still remain with regard to the exact nature of mineral surface ligands and the mineral/water interface. Similarities of spectroscopic data obtained for M(III) sorbed onto gamma-alumina, and clay minerals suggest the formation of very comparable inner-sphere surface complexes such as S-O-An(III)(OH)x(2-x)(H2O)5-x at pH > 5. Those speciation data are found consistent with those predicted by surface complexation modelling. The applicability of data obtained for pure mineral phases to actinide sorption onto heterogeneously composed natural clay rock is examined by experiments and by geochemical modelling. Good agreement of experiment and model calculations is found for U(VI) and trivalent actinide/lanthanide sorption to natural clay rock. The agreement of spectroscopy, geochemical modelling and batch experiments with natural rock samples and purified minerals increases the reliability in model predictions. The assessment of colloid borne actinide migration observed in various laboratory and field studies calls for detailed information on actinide-colloid interaction. Kinetic stabilization of colloid bound actinides can be due to inclusion into inorganic colloid matrix or by macromolecular rearrangement in case of organic, humic/fulvic like colloids. Only a combination of spectroscopy, microscopy and classical batch sorption experiments can help to elucidate the actinide-colloid interaction mechanisms and thus contribute to the assessment of colloids for radionuclide migration.

New cubic structure compounds as actinide host phases

NASA Astrophysics Data System (ADS)

Stefanovsky, S. V.; Yudintsev, S. V.; Livshits, T. S.

2010-03-01

Various compounds with fluorite (cubic zirconia) and fluorite-derived (pyrochlore, zirconolite) structures are considered as promising actinide host phases at immobilization of actinide-bearing nuclear wastes. Recently some new cubic compounds — stannate and stannate-zirconate pyrochlores, murataite and related phases, and actinide-bearing garnet structure compounds were proposed as perspective matrices for complex actinide wastes. Zirconate pyrochlore (ideally Gd2Zr2O7) has excellent radiation resistance and high chemical durability but requires high temperatures (at least 1500 °C) to be produced by hot-pressing from sol-gel derived precursor. Partial Sn4+ substitution for Zr4+ reduces production temperature and the compounds REE2ZrSnO7 may be hot-pressed or cold pressed and sintered at ~1400 °C. Pyrochlore, A2B2O7-x (two-fold elementary fluorite unit cell), and murataite, A3B6C2O20-y (three-fold fluorite unit cell), are end-members of the polysomatic series consisting of the phases whose structures are built from alternating pyrochlore and murataite blocks (nano-sized modules) with seven- (2C/3C/2C), five- (2C/3C), eight- (3C/2C/3C) and three-fold (3C — murataite) fluorite unit cells. Actinide content in this series reduces in the row: 2C (pyrochlore) > 7C > 5C > 8C > 3C (murataite). Due to congruent melting murataite-based ceramics may be produced by melting and the firstly segregated phase at melt crystallization is that with the highest fraction of the pyrochlore modules in its structure. The melts containing up to 10 wt. % AnO2 (An = Th, U, Np, Pu) or REE/An fraction of HLW form at crystallization zoned grains composed sequentially of the 5C → 8C → 3C phases with the highest actinide concentration in the core and the lowest — in the rim of the grains. Radiation resistance of the "murataite" is comparable to titanate pyrochlores. One more promising actinide hosts are ferrites with garnet structure. The matrices containing sometime complex fluorite structure oxide as an extra phase have leach and radiation resistance similar to the other well-known actinide waste forms.

Local Symmetry Effects in Actinide 4f X-ray Absorption in Oxides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Butorin, Sergei M.; Modin, Anders; Vegelius, Johan R.

2016-03-23

A systematic X-ray absorption study at actinide N 6,7 (4f → 6d transitions) edges was performed for light-actinide oxides including data obtained for the first time for NpO 2, PuO 2, and UO 3. The measurements were supported by ab initio calculations based on local-density-approximation with added 5f-5f Coulomb interaction (LDA+U). Improved energy resolution compared to common experiments at actinide L 2,3 (2p → 6d transitions) edges allowed us to resolve the major structures of the unoccupied 6d density of states (DOS) and estimate the crystal-field splittings in the 6d shell directly from the spectra of light-actinide dioxides. The measurementsmore » demonstrated an enhanced sensitivity of the N 6,7 spectral shape to changes in the compound crystal structure. Finally, for nonstoichiometric NpO 2-x, the filling of the entire band gap with Np 6d states was observed thus supporting a phase coexistence of Np metal and stoichiometric NpO 2 which is in agreement with the tentative Np-O phase diagram.« less

Final Report on Two-Stage Fast Spectrum Fuel Cycle Options

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Won Sik; Lin, C. S.; Hader, J. S.

2016-01-30

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 dischargedmore » 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« less

Actinide metal processing

DOEpatents

Sauer, Nancy N.; Watkin, John G.

1992-01-01

A process of converting an actinide metal such as thorium, uranium, or plnium to an actinide oxide material by admixing the actinide metal in an aqueous medium with a hypochlorite as an oxidizing agent for sufficient time to form the actinide oxide material and recovering the actinide oxide material is provided together with a low temperature process of preparing an actinide oxide nitrate such as uranyl nitrte. Additionally, a composition of matter comprising the reaction product of uranium metal and sodium hypochlorite is provided, the reaction product being an essentially insoluble uranium oxide material suitable for disposal or long term storage.

Actinide metal processing

DOEpatents

Sauer, N.N.; Watkin, J.G.

1992-03-24

A process for converting an actinide metal such as thorium, uranium, or plutonium to an actinide oxide material by admixing the actinide metal in an aqueous medium with a hypochlorite as an oxidizing agent for sufficient time to form the actinide oxide material and recovering the actinide oxide material is described together with a low temperature process for preparing an actinide oxide nitrate such as uranyl nitrate. Additionally, a composition of matter comprising the reaction product of uranium metal and sodium hypochlorite is provided, the reaction product being an essentially insoluble uranium oxide material suitable for disposal or long term storage.

Brief overview of the long-lived radionuclide separation processes developed in france in connection with the spin program

NASA Astrophysics Data System (ADS)

Madic, Charles; Bourges, Jacques; Dozol, Jean-François

1995-09-01

To reduce the long-term potential hazards associated with the management of nuclear wastes generated by nuclear fuel reprocessing, one alternative is the transmutation of long-lived radionuclides into short-lived radionuclides by nuclear means (P & T strategy). In this context, according to the law passed by the French Parliament on 30 December 1991, the CEA launched the SPIN program for the design of long-lived radionuclide separation and nuclear incineration processes. The research in progress to define separation processes focused mainly on the minor actinides (neptunium, americium and curium) and some fission products, like cesium and technetium. To separate these long-lived radionuclides, two strategies were developed. The first involves research on new operating conditions for improving the PUREX fuel reprocessing technology. This approach concerns the elements neptunium and technetium (iodine and zirconium can also be considered). The second strategy involves the design of new processes; DIAMEX for the co-extraction of minor actinides from the high-level liquid waste leaving the PUREX process, An(III)/Ln(III) separation using tripyridyltriazine derivatives or picolinamide extracting agents; SESAME for the selective separation of americium after its oxidation to Am(IV) or Am(VI) in the presence of a heteropolytungstate ligand, and Cs extraction using a new class of extracting agents, calixarenes, which exhibit exceptional Cs separation properties, especially in the presence of sodium ion. This lecture focuses on the latest achievements in these research areas.

Sensitivity Analysis and Optimization of the Nuclear Fuel Cycle: A Systematic Approach

NASA Astrophysics Data System (ADS)

Passerini, Stefano

For decades, nuclear energy development was based on the expectation that recycling of the fissionable materials in the used fuel from today's light water reactors into advanced (fast) reactors would be implemented as soon as technically feasible in order to extend the nuclear fuel resources. More recently, arguments have been made for deployment of fast reactors in order to reduce the amount of higher actinides, hence the longevity of radioactivity, in the materials destined to a geologic repository. The cost of the fast reactors, together with concerns about the proliferation of the technology of extraction of plutonium from used LWR fuel as well as the large investments in construction of reprocessing facilities have been the basis for arguments to defer the introduction of recycling technologies in many countries including the US. In this thesis, the impacts of alternative reactor technologies on the fuel cycle are assessed. Additionally, metrics to characterize the fuel cycles and systematic approaches to using them to optimize the fuel cycle are presented. The fuel cycle options of the 2010 MIT fuel cycle study are re-examined in light of the expected slower rate of growth in nuclear energy today, using the CAFCA (Code for Advanced Fuel Cycle Analysis). The Once Through Cycle (OTC) is considered as the base-line case, while advanced technologies with fuel recycling characterize the alternative fuel cycle options available in the future. The options include limited recycling in L WRs and full recycling in fast reactors and in high conversion LWRs. Fast reactor technologies studied include both oxide and metal fueled reactors. Additional fuel cycle scenarios presented for the first time in this work assume the deployment of innovative recycling reactor technologies such as the Reduced Moderation Boiling Water Reactors and Uranium-235 initiated Fast Reactors. A sensitivity study focused on system and technology parameters of interest has been conducted to test the robustness of the conclusions presented in the MIT Fuel Cycle Study. These conclusions are found to still hold, even when considering alternative technologies and different sets of simulation assumptions. Additionally, a first of a kind optimization scheme for the nuclear fuel cycle analysis is proposed and the applications of such an optimization are discussed. Optimization metrics of interest for different stakeholders in the fuel cycle (economics, fuel resource utilization, high level waste, transuranics/proliferation management, and environmental impact) are utilized for two different optimization techniques: a linear one and a stochastic one. Stakeholder elicitation provided sets of relative weights for the identified metrics appropriate to each stakeholder group, which were then successfully used to arrive at optimum fuel cycle configurations for recycling technologies. The stochastic optimization tool, based on a genetic algorithm, was used to identify non-inferior solutions according to Pareto's dominance approach to optimization. The main tradeoff for fuel cycle optimization was found to be between economics and most of the other identified metrics. (Copies available exclusively from MIT Libraries, libraries.mit.edu/docs - docs mit.edu)

The nature of chemical bonding in actinide and lanthanide ferrocyanides determined by X-ray absorption spectroscopy and density functional theory.

PubMed

Dumas, Thomas; Guillaumont, Dominique; Fillaux, Clara; Scheinost, Andreas; Moisy, Philippe; Petit, Sébastien; Shuh, David K; Tyliszczak, Tolek; Den Auwer, Christophe

2016-01-28

The electronic properties of actinide cations are of fundamental interest to describe intramolecular interactions and chemical bonding in the context of nuclear waste reprocessing or direct storage. The 5f and 6d orbitals are the first partially or totally vacant states in these elements, and the nature of the actinide ligand bonds is related to their ability to overlap with ligand orbitals. Because of its chemical and orbital selectivities, X-ray absorption spectroscopy (XAS) is an effective probe of actinide species frontier orbitals and for understanding actinide cation reactivity toward chelating ligands. The soft X-ray probes of the light elements provide better resolution than actinide L3-edges to obtain electronic information from the ligand. Thus coupling simulations to experimental soft X-ray spectral measurements and complementary quantum chemical calculations yields quantitative information on chemical bonding. In this study, soft X-ray XAS at the K-edges of C and N, and the L2,3-edges of Fe was used to investigate the electronic structures of the well-known ferrocyanide complexes K4Fe(II)(CN)6, thorium hexacyanoferrate Th(IV)Fe(II)(CN)6, and neodymium hexacyanoferrate KNd(III)Fe(II)(CN)6. The soft X-ray spectra were simulated based on quantum chemical calculations. Our results highlight the orbital overlapping effects and atomic effective charges in the Fe(II)(CN)6 building block. In addition to providing a detailed description of the electronic structure of the ferrocyanide complex (K4Fe(II)(CN)6), the results strongly contribute to confirming the actinide 5f and 6d orbital oddity in comparison to lanthanide 4f and 5d.

The nature of chemical bonding in actinide and lanthanide ferrocyanides determined by X-ray absorption spectroscopy and density functional theory

DOE PAGES

Dumas, Thomas; Guillaumont, Dominique; Fillaux, Clara; ...

2016-01-01

The electronic properties of actinide cations are of fundamental interest to describe intramolecular interactions and chemical bonding in the context of nuclear waste reprocessing or direct storage. The 5f and 6d orbitals are the first partially or totally vacant states in these elements, and the nature of the actinide ligand bonds is related to their ability to overlap with ligand orbitals. Because of its chemical and orbital selectivities, X-ray absorption spectroscopy (XAS) is an effective probe of actinide species frontier orbitals and for understanding actinide cation reactivity toward chelating ligands. The soft X-ray probes of the light elements provide bettermore » resolution than actinide L 3 -edges to obtain electronic information from the ligand. Thus coupling simulations to experimental soft X-ray spectral measurements and complementary quantum chemical calculations yields quantitative information on chemical bonding. In this study, soft X-ray XAS at the K-edges of C and N, and the L 2,3 -edges of Fe was used to investigate the electronic structures of the well-known ferrocyanide complexes K 4 Fe II (CN) 6 , thorium hexacyanoferrate Th IV Fe II (CN) 6 , and neodymium hexacyanoferrate KNd III Fe II (CN) 6 . The soft X-ray spectra were simulated based on quantum chemical calculations. Our results highlight the orbital overlapping effects and atomic effective charges in the Fe II (CN) 6 building block. In addition to providing a detailed description of the electronic structure of the ferrocyanide complex (K 4 Fe II (CN) 6 ), the results strongly contribute to confirming the actinide 5f and 6d orbital oddity in comparison to lanthanide 4f and 5d.« less

Separations of actinides, lanthanides and other metals

DOEpatents

Smith, Barbara F.; Jarvinen, Gordon D.; Ensor, Dale D.

1995-01-01

An organic extracting solution comprised of a bis(acylpyrazolone or a substituted bis(acylpyrazolone) and an extraction method useful for separating certain elements of the actinide series of the periodic table having a valence of four from one other, and also from one or more of the substances in a group consisting of hexavalent actinides, trivalent actinides, trivalent lanthanides, trivalent iron, trivalent aluminum, divalent metals, and monovalent metals and also from one or more of the substances in a group consisting of hexavalent actinides, trivalent actinides, trivalent lanthanides, trivalent iron, trivalent aluminum, divalent metals, and monovalent metals and also useful for separating hexavalent actinides from one or more of the substances in a group consisting of trivalent actinides, trivalent lanthanides, trivalent iron, trivalent aluminum, divalent metals, and monovalent metals.

Actinide-ion sensor

DOEpatents

Li, Shelly X; Jue, Jan-fong; Herbst, Ronald Scott; Herrmann, Steven Douglas

2015-01-13

An apparatus for the real-time, in-situ monitoring of actinide-ion concentrations. A working electrolyte is positioned within the interior of a container. The working electrolyte is separated from a reference electrolyte by a separator. A working electrode is at least partially in contact with the working electrolyte. A reference electrode is at least partially in contact with the reference electrolyte. A voltmeter is electrically connected to the working electrode and the reference electrode. The working electrolyte comprises an actinide-ion of interest. The separator is ionically conductive to the actinide-ion of interest. The separator comprises an actinide, Zr, and Nb. Preferably, the actinide of the separator is Am or Np, more preferably Pu. In one embodiment, the actinide of the separator is the actinide of interest. In another embodiment, the separator further comprises P and O.

Actinide halide complexes

DOEpatents

Avens, Larry R.; Zwick, Bill D.; Sattelberger, Alfred P.; Clark, David L.; Watkin, John G.

1992-01-01

A compound of the formula MX.sub.n L.sub.m wherein M is a metal atom selected from the group consisting of thorium, plutonium, neptunium or americium, X is a halide atom, n is an integer selected from the group of three or four, L is a coordinating ligand selected from the group consisting of aprotic Lewis bases having an oxygen-, nitrogen-, sulfur-, or phosphorus-donor, and m is an integer selected from the group of three or four for monodentate ligands or is the integer two for bidentate ligands, where the sum of n+m equals seven or eight for monodentate ligands or five or six for bidentate ligands, a compound of the formula MX.sub.n wherein M, X, and n are as previously defined, and a process of preparing such actinide metal compounds including admixing the actinide metal in an aprotic Lewis base as a coordinating solvent in the presence of a halogen-containing oxidant, are provided.

Actinide halide complexes

DOEpatents

Avens, L.R.; Zwick, B.D.; Sattelberger, A.P.; Clark, D.L.; Watkin, J.G.

1992-11-24

A compound is described of the formula MX[sub n]L[sub m] wherein M is a metal atom selected from the group consisting of thorium, plutonium, neptunium or americium, X is a halide atom, n is an integer selected from the group of three or four, L is a coordinating ligand selected from the group consisting of aprotic Lewis bases having an oxygen-, nitrogen-, sulfur-, or phosphorus-donor, and m is an integer selected from the group of three or four for monodentate ligands or is the integer two for bidentate ligands, where the sum of n+m equals seven or eight for monodentate ligands or five or six for bidentate ligands. A compound of the formula MX[sub n] wherein M, X, and n are as previously defined, and a process of preparing such actinide metal compounds are described including admixing the actinide metal in an aprotic Lewis base as a coordinating solvent in the presence of a halogen-containing oxidant.

Molten salt reactor neutronics and fuel cycle modeling and simulation with SCALE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Betzler, Benjamin R.; Powers, Jeffrey J.; Worrall, Andrew

Current interest in advanced nuclear energy and molten salt reactor (MSR) concepts has enhanced interest in building the tools necessary to analyze these systems. A Python script known as ChemTriton has been developed to simulate equilibrium MSR fuel cycle performance by modeling the changing isotopic composition of an irradiated fuel salt using SCALE for neutron transport and depletion calculations. Some capabilities in ChemTriton that have improved, include a generic geometry capable of modeling multi-zone and multi-fluid systems, enhanced time-dependent feed and separations, and a critical concentration search. Although more generally applicable, the capabilities developed to date are illustrated in thismore » paper in three applied problems: (1) simulating the startup of a thorium-based MSR fuel cycle (a likely scenario requires the first of these MSRs to be started without available 233U); (2) determining the effect of the removal of different fission products on MSR operations; and (3) obtaining the equilibrium concentration of a mixed-oxide light-water reactor fuel in a two-stage fuel cycle with a sodium fast reactor. Moreover, the third problem is chosen to demonstrate versatility in an application to analyze the fuel cycle of a non-MSR system. During the first application, the initial fuel salt compositions fueled with different sources of fissile material are made feasible after (1) removing the associated nonfissile actinides after much of the initial fissile isotopes have burned and (2) optimizing the thorium concentration to maintain a critical configuration without significantly reducing breeding capability. In the second application, noble metal, volatile gas, and rare earth element fission products are shown to have a strong negative effect on criticality in a uranium-fueled thermal-spectrum MSR; their removal significantly increases core lifetime (by 30%) and fuel utilization. In the third application, the fuel of a mixed-oxide light-water reactor approaches an equilibrium composition after 20 depletion steps, demonstrating the potential for the longer time scales required to achieve equilibrium for solid-fueled systems over liquid fuel systems. This time to equilibrium can be reduced by starting with an initial fuel composition closer to that of the equilibrium fuel, reducing the need to handle time-dependent fuel compositions.« less

Molten salt reactor neutronics and fuel cycle modeling and simulation with SCALE

DOE PAGES

Betzler, Benjamin R.; Powers, Jeffrey J.; Worrall, Andrew

2017-03-01

Current interest in advanced nuclear energy and molten salt reactor (MSR) concepts has enhanced interest in building the tools necessary to analyze these systems. A Python script known as ChemTriton has been developed to simulate equilibrium MSR fuel cycle performance by modeling the changing isotopic composition of an irradiated fuel salt using SCALE for neutron transport and depletion calculations. Some capabilities in ChemTriton that have improved, include a generic geometry capable of modeling multi-zone and multi-fluid systems, enhanced time-dependent feed and separations, and a critical concentration search. Although more generally applicable, the capabilities developed to date are illustrated in thismore » paper in three applied problems: (1) simulating the startup of a thorium-based MSR fuel cycle (a likely scenario requires the first of these MSRs to be started without available 233U); (2) determining the effect of the removal of different fission products on MSR operations; and (3) obtaining the equilibrium concentration of a mixed-oxide light-water reactor fuel in a two-stage fuel cycle with a sodium fast reactor. Moreover, the third problem is chosen to demonstrate versatility in an application to analyze the fuel cycle of a non-MSR system. During the first application, the initial fuel salt compositions fueled with different sources of fissile material are made feasible after (1) removing the associated nonfissile actinides after much of the initial fissile isotopes have burned and (2) optimizing the thorium concentration to maintain a critical configuration without significantly reducing breeding capability. In the second application, noble metal, volatile gas, and rare earth element fission products are shown to have a strong negative effect on criticality in a uranium-fueled thermal-spectrum MSR; their removal significantly increases core lifetime (by 30%) and fuel utilization. In the third application, the fuel of a mixed-oxide light-water reactor approaches an equilibrium composition after 20 depletion steps, demonstrating the potential for the longer time scales required to achieve equilibrium for solid-fueled systems over liquid fuel systems. This time to equilibrium can be reduced by starting with an initial fuel composition closer to that of the equilibrium fuel, reducing the need to handle time-dependent fuel compositions.« less

Americium characterization by X-ray fluorescence and absorption spectroscopy in plutonium uranium mixed oxide

NASA Astrophysics Data System (ADS)

Degueldre, Claude; Cozzo, Cedric; Martin, Matthias; Grolimund, Daniel; Mieszczynski, Cyprian

2013-06-01

Plutonium uranium mixed oxide (MOX) fuels are currently used in nuclear reactors. The actinides in these fuels need to be analyzed after irradiation for assessing their behaviour with regard to their environment and the coolant. In this work the study of the atomic structure and next-neighbour environment of Am in the (Pu,U)O2 lattice in an irradiated (60 MW d kg-1) MOX sample was performed employing micro-X-ray fluorescence (µ-XRF) and micro-X-ray absorption fine structure (µ-XAFS) spectroscopy. The chemical bonds, valences and stoichiometry of Am (˜0.66 wt%) are determined from the experimental data gained for the irradiated fuel material examined in its peripheral zone (rim) of the fuel. In the irradiated sample Am builds up as Am3+ species within an [AmO8]13- coordination environment (e.g. >90%) and no (<10%) Am(IV) or (V) can be detected in the rim zone. The occurrence of americium dioxide is avoided by the redox buffering activity of the uranium dioxide matrix.

Roadmap to an Engineering-Scale Nuclear Fuel Performance & Safety Code

DOE Office of Scientific and Technical Information (OSTI.GOV)

Turner, John A; Clarno, Kevin T; Hansen, Glen A

2009-09-01

Developing new fuels and qualifying them for large-scale deployment in power reactors is a lengthy and expensive process, typically spanning a period of two decades from concept to licensing. Nuclear fuel designers serve an indispensable role in the process, at the initial exploratory phase as well as in analysis of the testing results. In recent years fuel performance capabilities based on first principles have been playing more of a role in what has traditionally been an empirically dominated process. Nonetheless, nuclear fuel behavior is based on the interaction of multiple complex phenomena, and recent evolutionary approaches are being applied moremore » on a phenomenon-by-phenomenon basis, targeting localized problems, as opposed to a systematic approach based on a fundamental understanding of all interacting parameters. Advanced nuclear fuels are generally more complex, and less understood, than the traditional fuels used in existing reactors (ceramic UO{sub 2} with burnable poisons and other minor additives). The added challenges are primarily caused by a less complete empirical database and, in the case of recycled fuel, the inherent variability in fuel compositions. It is clear that using the traditional approach to develop and qualify fuels over the entire range of variables pertinent to the U.S. Department of Energy (DOE) Office of Nuclear Energy on a timely basis with available funds would be very challenging, if not impossible. As a result the DOE Office of Nuclear Energy has launched the Nuclear Energy Advanced Modeling and Simulation (NEAMS) approach to revolutionize fuel development. This new approach is predicated upon transferring the recent advances in computational sciences and computer technologies into the fuel development program. The effort will couple computational science with recent advances in the fundamental understanding of physical phenomena through ab initio modeling and targeted phenomenological testing to leapfrog many fuel-development activities. Realizing the full benefits of this approach will likely take some time. However, it is important that the developmental activities for modeling and simulation be tightly coupled with the experimental activities to maximize feedback effects and accelerate both the experimental and analytical elements of the program toward a common objective. The close integration of modeling and simulation and experimental activities is key to developing a useful fuel performance simulation capability, providing a validated design and analysis tool, and understanding the uncertainties within the models and design process. The efforts of this project are integrally connected to the Transmutation Fuels Campaign (TFC), which maintains as a primary objective to formulate, fabricate, and qualify a transuranic-based fuel with added minor actinides for use in future fast reactors. Additional details of the TFC scope can be found in the Transmutation Fuels Campaign Execution Plan. This project is an integral component of the TFC modeling and simulation effort, and this multiyear plan borrowed liberally from the Transmutation Fuels Campaign Modeling and Simulation Roadmap. This document provides the multiyear staged development plan to develop a continuum-level Integrated Performance and Safety Code (IPSC) to predict the behavior of the fuel and cladding during normal reactor operations and anticipated transients up to the point of clad breach.« less

Nonaqueous actinide hydride dissolution and production of actinide $beta$- diketonates

DOEpatents

Crisler, L.R.

1975-11-11

Actinide beta-diketonate complex molecular compounds are produced by reacting a beta-diketone compound with a hydride of the actinide material in a mixture of carbon tetrachloride and methanol. (auth)

Dehydration of plutonium or neptunium trichloride hydrate

DOEpatents

Foropoulos, Jr., Jerry; Avens, Larry R.; Trujillo, Eddie A.

1992-01-01

A process of preparing anhydrous actinide metal trichlorides of plutonium or neptunium by reacting an aqueous solution of an actinide metal trichloride selected from the group consisting of plutonium trichloride or neptunium trichloride with a reducing agent capable of converting the actinide metal from an oxidation state of +4 to +3 in a resultant solution, evaporating essentially all the solvent from the resultant solution to yield an actinide trichloride hydrate material, dehydrating the actinide trichloride hydrate material by heating the material in admixture with excess thionyl chloride, and recovering anhydrous actinide trichloride is provided.

Dehydration of plutonium or neptunium trichloride hydrate

DOEpatents

Foropoulos, J. Jr.; Avens, L.R.; Trujillo, E.A.

1992-03-24

A process is described for preparing anhydrous actinide metal trichlorides of plutonium or neptunium by reacting an aqueous solution of an actinide metal trichloride selected from the group consisting of plutonium trichloride or neptunium trichloride with a reducing agent capable of converting the actinide metal from an oxidation state of +4 to +3 in a resultant solution, evaporating essentially all the solvent from the resultant solution to yield an actinide trichloride hydrate material, dehydrating the actinide trichloride hydrate material by heating the material in admixture with excess thionyl chloride, and recovering anhydrous actinide trichloride.

Theoretical Prediction of Am(III)/Eu(III) Selectivity to Aid the Design of Actinide-Lanthanide Separation Agents

DOE PAGES

Bryantsev, Vyacheslav S.; Hay, Benjamin P.

2015-03-20

Selective extraction of minor actinides from lanthanides is a critical step in the reduction of radiotoxicity of spent nuclear fuels. However, the design of suitable ligands for separating chemically similar 4f- and 5f-block trivalent metal ions poses a significant challenge. Furthermore, first-principles calculations should play an important role in the design of new separation agents, but their ability to predict metal ion selectivity has not been systematically evaluated. We examine the ability of several density functional theory methods to predict selectivity of Am(III) and Eu(III) with oxygen, mixed oxygen–nitrogen, and sulfur donor ligands. The results establish a computational method capablemore » of predicting the correct order of selectivities obtained from liquid–liquid extraction and aqueous phase complexation studies. To allow reasonably accurate predictions, it was critical to employ sufficiently flexible basis sets and provide proper account of solvation effects. The approach is utilized to estimate the selectivity of novel amide-functionalized diazine and 1,2,3-triazole ligands.« less

Piezomagnetism and magnetoelastic memory in uranium dioxide

DOE PAGES

Jaime, M.; Saul, A.; Salamon, M.; ...

2017-07-24

Uranium dioxide (UO 2) is a prime nuclear fuel and perhaps the most thoroughly studied actinide material to date. Its thermal and magnetic properties remain, however, a puzzle resulting from strong couplings between magnetism and lattice vibrations. The magnetic state of this cubic material is characterized by a non- collinear antiferromagnetic structure and multidomain Jahn-Teller distortions that could be behind novel thermal properties. Here we show that single crystals of UO 2, subjected to magnetic fields up to 95 T in the magnetic state, exhibit the abrupt appearance of positive linear magnetostriction leading to a trigonal distortion. Upon reversal ofmore » the field the linear term also reverses sign, a hallmark of piezomagnetism. The switching phenomenon occurs at ± 18 T and persists during subsequent field reversals, demonstrating robust magneto-elastic memory. This is the first example of piezomagnetism in an actinide spin system and the magneto-elastic memory loop here is nearly an order of magnitude wider in field than those previously observed, making UO 2 the hardest piezomagnet known. The possibility of an inverse phase with reduced magnetocrystalline anisotropy is considered to explain these effects.« less

Piezomagnetism and magnetoelastic memory in uranium dioxide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jaime, M.; Saul, A.; Salamon, M.

Uranium dioxide (UO 2) is a prime nuclear fuel and perhaps the most thoroughly studied actinide material to date. Its thermal and magnetic properties remain, however, a puzzle resulting from strong couplings between magnetism and lattice vibrations. The magnetic state of this cubic material is characterized by a non- collinear antiferromagnetic structure and multidomain Jahn-Teller distortions that could be behind novel thermal properties. Here we show that single crystals of UO 2, subjected to magnetic fields up to 95 T in the magnetic state, exhibit the abrupt appearance of positive linear magnetostriction leading to a trigonal distortion. Upon reversal ofmore » the field the linear term also reverses sign, a hallmark of piezomagnetism. The switching phenomenon occurs at ± 18 T and persists during subsequent field reversals, demonstrating robust magneto-elastic memory. This is the first example of piezomagnetism in an actinide spin system and the magneto-elastic memory loop here is nearly an order of magnitude wider in field than those previously observed, making UO 2 the hardest piezomagnet known. The possibility of an inverse phase with reduced magnetocrystalline anisotropy is considered to explain these effects.« less

Radioactive waste disposal via electric propulsion

NASA Technical Reports Server (NTRS)

Burns, R. E.

1975-01-01

It is shown that space transportation is a feasible method of removal of radioactive wastes from the biosphere. The high decay heat of the isotopes powers a thermionic generator which provides electrical power for ion thrust engines. The massive shields (used to protect ground and flight personnel) are removed in orbit for subsequent reuse; the metallic fuel provides a shield for the avionics that guides the orbital stage to solar system escape. Performance calculations indicate that 4000 kg. of actinides may be removed per Shuttle flight. Subsidiary problems - such as cooling during ascent - are discussed.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

This report contains viewgraphs on the following topics. The advanced light source U8 undulator beamline, 20--300 eV; gas-phase actinide studies with synchrotron radiation; atomic structure calculations for heavy atoms; flux growth of single crystal uranium intermetallics: Extension to transuranics; x-ray absorption near-edge structure studies of actinide compounds; surface as a new stage for studying actinides: Theoretical study of the surface electronic structure of uranium; magnetic x-ray scattering experiments at resonant energies; beamline instruments for radioactive materials; the search for x-ray absorption magnetic circular dichroism in actinide materials: preliminary experiments using UFe[sub 2] and U-S; the laser plasma laboratory light source:more » a source of preliminary transuranic data; electron spectroscopy of heavy fermion actinide materials; study of thin layers of actinides. Present status and future use of synchrotron radiation; electronic structure and correlated-electron theory for actinide materials; and heavy fermion and kondo phenomena in actinide materials.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

This report contains viewgraphs on the following topics. The advanced light source U8 undulator beamline, 20--300 eV; gas-phase actinide studies with synchrotron radiation; atomic structure calculations for heavy atoms; flux growth of single crystal uranium intermetallics: Extension to transuranics; x-ray absorption near-edge structure studies of actinide compounds; surface as a new stage for studying actinides: Theoretical study of the surface electronic structure of uranium; magnetic x-ray scattering experiments at resonant energies; beamline instruments for radioactive materials; the search for x-ray absorption magnetic circular dichroism in actinide materials: preliminary experiments using UFe{sub 2} and U-S; the laser plasma laboratory light source:more » a source of preliminary transuranic data; electron spectroscopy of heavy fermion actinide materials; study of thin layers of actinides. Present status and future use of synchrotron radiation; electronic structure and correlated-electron theory for actinide materials; and heavy fermion and kondo phenomena in actinide materials.« less

Actinide migration in Johnston Atoll soil

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wolf, S. F.; Bates, J. K.; Buck, E. C.

1997-02-01

Characterization of the actinide content of a sample of contaminated coral soil from Johnston Atoll, the site of three non-nuclear destructs of nuclear warhead-carrying THOR missiles in 1962, revealed that >99% of the total actinide content is associated with discrete bomb fragments. After removal of these fragments, there was an inverse correlation between actinide content and soil particle size in particles from 43 to 0.4 {micro}m diameter. Detailed analyses of this remaining soil revealed no discrete actinide phase in these soil particles, despite measurable actinide content. Observations indicate that exposure to the environment has caused the conversion of relatively insolublemore » actinide oxides to the more soluble actinyl oxides and actinyl carbonate coordinated complexes. This process has led to dissolution of actinides from discrete particles and migration to the surrounding soil surfaces, resulting in a dispersion greater than would be expected by physical transport of discrete particles alone.« less

Combination of thermal and electric properties' measurement techniques in a single setup suitable for radioactive materials in controlled environments and based on the 3ω approach

NASA Astrophysics Data System (ADS)

Shrestha, K.; Gofryk, K.

2018-04-01

We have designed and developed a new experimental setup, based on the 3ω method, to measure thermal conductivity, heat capacity, and electrical resistivity of a variety of samples in a broad temperature range (2-550 K) and under magnetic fields up to 9 T. The validity of this method is tested by measuring various types of metallic (copper, platinum, and constantan) and insulating (SiO2) materials, which have a wide range of thermal conductivity values (1-400 W m-1 K-1). We have successfully employed this technique for measuring the thermal conductivity of two actinide single crystals: uranium dioxide and uranium nitride. This new experimental approach for studying nuclear materials will help us to advance reactor fuel development and understanding. We have also shown that this experimental setup can be adapted to the Physical Property Measurement System (Quantum Design) environment and/or other cryocooler systems.

Characteristic of molten fluoride salt system LiF-BeF2 (Flibe) and LiF-NaF-KF (Flinak) as coolant and fuel carrier in molten salt reactor (MSR)

NASA Astrophysics Data System (ADS)

Bahri, Che Nor Aniza Che Zainul; Al-Areqi, Wadee'ah Mohd; Ruf, Mohd'Izzat Fahmi Mohd; Majid, Amran Ab.

2017-01-01

Interest of fluoride salts have recently revived due to the high temperature application in nuclear reactors. Molten Salt Reactor (MSR) was designed to operate at high temperature in range 700 - 800°C and its fuel is dissolved in a circulating molten fluoride salt mixture. Molten fluoride salts are stable at high temperature, have good heat transfer properties and can dissolve high concentration of actinides and fission product. The aim of this paper was to discuss the physical properties (melting temperature, density and heat capacity) of two systems fluoride salt mixtures i.e; LiF-BeF2 (Flibe) and LiF-NaF-KF (Flinak) in terms of their application as coolant and fuel solvent in MSR. Both of these salts showed almost same physical properties but different applications in MSR. The advantages and the disadvantages of these fluoride salt systems will be discussed in this paper.

Renovation of the hot press in the Plutonium Experimental Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Congdon, J.W.; Nelson, G.H.

1990-03-05

The Plutonium Experimental Facility (PEF) will be used to develop a new fuel pellet fabrication process and to evaluate equipment upgrades. The facility was used from 1978 until 1982 to optimize the parameters for fuel pellet production using a process which was developed at Los Alamos National Laboratory. The PEF was shutdown and essentially abandoned until mid-1987 when the facility renovations were initiated by the Actinide Technology Section (ATS) of SRL. A major portion of the renovation work was related to the restart of the hot press system. This report describes the renovations and modifications which were required to restartmore » the PEF hot press. The primary purpose of documenting this work is to help provide a basis for Separations to determine the best method of renovating the hot press in the Plutonium Fuel Fabrication (PuFF) facility. This report also includes several SRL recommendations concerning the renovation and modification of the PuFF hot press. 4 refs.« less

Molten salts and nuclear energy production

NASA Astrophysics Data System (ADS)

Le Brun, Christian

2007-01-01

Molten salts (fluorides or chlorides) were considered near the beginning of research into nuclear energy production. This was initially due to their advantageous physical and chemical properties: good heat transfer capacity, radiation insensitivity, high boiling point, wide range solubility for actinides. In addition it was realised that molten salts could be used in numerous situations: high temperature heat transfer, core coolants with solid fuels, liquid fuel in a molten salt reactor, solvents for spent nuclear solid fuel in the case of pyro-reprocessing and coolant and tritium production in the case of fusion. Molten salt reactors, one of the six innovative concepts chosen by the Generation IV international forum, are particularly interesting for use as either waste incinerators or thorium cycle systems. As the neutron balance in the thorium cycle is very tight, the possibility to perform online extraction of some fission product poisons from the salt is very attractive. In this article the most important questions that must be addressed to demonstrate the feasibility of molten salt reactor will be reviewed.

Synthesis and Characterization of Templated Ion Exchange Resins for the Selective Complexion of Actinide Ions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Murrray, George M.; Uy, O. Manuel

The purpose of this research is to develop polymeric extractants for the selective complexation of uranyl ions (and subsequently other actinyl and actinide ions) from aqueous solutions. Selectivity for a specific actinide ion is obtained by providing the polymers with cavities lined with complexing ligands so arranged as to match the charge, coordination number, coordination geometry, and size of the actinide ion. These cavity-containing polymers are produced by using a specific actinide ion (or surrogate) as a template around which monomeric complexing ligands are polymerized. The polymers provide useful sequestering agents for removing actinide ions from wastes and will formmore » the basis for a variety of analytical techniques for actinide determination.« less

Impact of Americium-241 (n,γ) Branching Ratio on SFR Core Reactivity and Spent Fuel Characteristics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hiruta, Hikaru; Youinou, Gilles J.; Dixon, Brent W.

An accurate prediction of core physics and fuel cycle parameters largely depends on the order of details and accuracy in nuclear data taken into account for actual calculations. 241Am is a major gateway nuclide for most of minor actinides and thus important nuclide for core physics and fuel-cycle calculations. The 241Am(n,?) branching ratio (BR) is in fact the energy dependent (see Fig. 1), therefore, it is necessary to taken into account the spectrum effect on the calculation of the average BR for the full-core depletion calculations. Moreover, the accuracy of the BR used in the depletion calculations could significantly influencemore » the core physics performance and post irradiated fuel compositions. The BR of 241Am(n,?) in ENDF/B-VII.0 library is relatively small and flat in thermal energy range, gradually increases within the intermediate energy range, and even becomes larger at the fast energy range. This indicates that the properly collapsed BR for fast reactors could be significantly different from that of thermal reactors. The evaluated BRs are also differ from one evaluation to another. As seen in Table I, average BRs for several evaluated libraries calculated by means of a fast spectrum are similar but have some differences. Most of currently available depletion codes use a pre-determined single value BR for each library. However, ideally it should be determined on-the-fly basis like that of one-group cross sections. These issues provide a strong incentive to investigate the effect of different 241Am(n,?) BRs on core and spent fuel parameters. This paper investigates the impact of the 241Am(n,?) BR on the results of SFR full-core based fuel-cycle calculations. The analysis is performed by gradually increasing the value of BR from 0.15 to 0.25 and studying its impact on the core reactivity and characteristics of SFR spent fuels over extended storage times (~10,000 years).« less

Positron Spectroscopy of Hydrothermally Grown Actinide Oxides

DTIC Science & Technology

2014-03-27

POSITRON SPECTROSCOPY OF HYDROTHERMALLY GROWN ACTINIDE OXIDES THESIS Edward C. Schneider...United States Government. AFIT-ENP-14-M-33 POSITRON SPECTROSCOPY OF HYDROTHERMALLY GROWN ACTINIDE OXIDES THESIS...33 POSITRON SPECTROSCOPY OF HYDROTHERMALLY GROWN ACTINIDE OXIDES Edward C. Schneider, BS Captain, USAF Approved

Actinide Waste Forms and Radiation Effects

NASA Astrophysics Data System (ADS)

Ewing, R. C.; Weber, W. J.

Over the past few decades, many studies of actinides in glasses and ceramics have been conducted that have contributed substantially to the increased understanding of actinide incorporation in solids and radiation effects due to actinide decay. These studies have included fundamental research on actinides in solids and applied research and development related to the immobilization of the high level wastes (HLW) from commercial nuclear power plants and processing of nuclear weapons materials, environmental restoration in the nuclear weapons complex, and the immobilization of weapons-grade plutonium as a result of disarmament activities. Thus, the immobilization of actinides has become a pressing issue for the twenty-first century (Ewing, 1999), and plutonium immobilization, in particular, has received considerable attention in the USA (Muller et al., 2002; Muller and Weber, 2001). The investigation of actinides and

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cappiello, M.; Hobbins, R.; Penny, K.

As part of the Department of Energy Advanced Fuel Cycle program, a series of fuels development irradiation tests have been performed in the Advanced Test Reactor (ATR) at the Idaho National Laboratory. These tests are providing excellent data for advanced fuels development. The program is focused on the transmutation of higher actinides which best can be accomplished in a sodium-cooled fast reactor. Because a fast test reactor is no longer available in the US, a special test vehicle is used to achieve near-prototypic fast reactor conditions (neutron spectra and temperature) for use in ATR (a water-cooled thermal reactor). As partmore » of the testing program, there were many successful tests of advanced fuels including metals and ceramics. Recently however, there have been three experimental campaigns using metal fuels that experienced failure during irradiation. At the request of the program, an independent review committee was convened to review the post-test analyses performed by the fuels development team, to assess the conclusions of the team for the cause of the failures, to assess the adequacy and completeness of the analyses, to identify issues that were missed, and to make recommendations for improvements in the design and operation of future tests. Although there is some difference of opinion, the review committee largely agreed with the conclusions of the fuel development team regarding the cause of the failures. For the most part, the analyses that support the conclusions are sufficient.« less

The thermal conductivity of mixed fuel U xPu 1-xO 2: molecular dynamics simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Xiang-Yang; Cooper, Michael William Donald; Stanek, Christopher Richard

2015-10-16

Mixed oxides (MOX), in the context of nuclear fuels, are a mixture of the oxides of heavy actinide elements such as uranium, plutonium and thorium. The interest in the UO 2-PuO 2 system arises from the fact that these oxides are used both in fast breeder reactors (FBRs) as well as in pressurized water reactors (PWRs). The thermal conductivity of UO 2 fuel is an important material property that affects fuel performance since it is the key parameter determining the temperature distribution in the fuel, thus governing, e.g., dimensional changes due to thermal expansion, fission gas release rates, etc. Formore » this reason it is important to understand the thermal conductivity of MOX fuel and how it differs from UO 2. Here, molecular dynamics (MD) simulations are carried out to determine quantitatively, the effect of mixing on the thermal conductivity of U xPu 1-xO 2, as a function of PuO 2 concentrations, for a range of temperatures, 300 – 1500 K. The results will be used to develop enhanced continuum thermal conductivity models for MARMOT and BISON by INL. These models express the thermal conductivity as a function of microstructure state-variables, thus enabling thermal conductivity models with closer connection to the physical state of the fuel.« less

Comparative analysis of thorium and uranium fuel for transuranic recycle in a sodium cooled Fast Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

C. Fiorina; N. E. Stauff; F. Franceschini

2013-12-01

The present paper compares the reactor physics and transmutation performance of sodium-cooled Fast Reactors (FRs) for TRansUranic (TRU) burning with thorium (Th) or uranium (U) as fertile materials. The 1000 MWt Toshiba-Westinghouse Advanced Recycling Reactor (ARR) conceptual core has been used as benchmark for the comparison. Both burner and breakeven configurations sustained or started with a TRU supply, and assuming full actinide homogeneous recycle strategy, have been developed. State-of-the-art core physics tools have been employed to establish fuel inventory and reactor physics performances for equilibrium and transition cycles. Results show that Th fosters large improvements in the reactivity coefficients associatedmore » with coolant expansion and voiding, which enhances safety margins and, for a burner design, can be traded for maximizing the TRU burning rate. A trade-off of Th compared to U is the significantly larger fuel inventory required to achieve a breakeven design, which entails additional blankets at the detriment of core compactness as well as fuel manufacturing and separation requirements. The gamma field generated by the progeny of U-232 in the U bred from Th challenges fuel handling and manufacturing, but in case of full recycle, the high contents of Am and Cm in the transmutation fuel impose remote fuel operations regardless of the presence of U-232.« less

Ultratrace analysis of transuranic actinides by laser-induced fluorescence

DOEpatents

Miller, S.M.

1983-10-31

Ultratrace quantities of transuranic actinides are detected indirectly by their effect on the fluorescent emissions of a preselected fluorescent species. Transuranic actinides in a sample are coprecipitated with a host lattice material containing at least one preselected fluorescent species. The actinide either quenches or enhances the laser-induced fluorescence of the preselected fluorescent species. The degree of enhancement or quenching is quantitatively related to the concentration of actinide in the sample.

On the Suitability of Lanthanides as Actinide Analogs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Szigethy, Geza; Raymond, Kenneth N.

2008-04-11

With the current level of actinide materials used in civilian power generation and the need for safe and efficient methods for the chemical separation of these species from their daughter products and for long-term storage requirements, a detailed understanding of actinide chemistry is of great importance. Due to the unique bonding properties of the f-elements, the lanthanides are commonly used as structural and chemical models for the actinides, but differences in the bonding between these 4f and 5f elements has become a question of immediate applicability to separations technology. This brief overview of actinide coordination chemistry in the Raymond groupmore » at UC Berkeley/LBNL examines the validity of using lanthanide analogs as structural models for the actinides, with particular attention paid to single crystal X-ray diffraction structures. Although lanthanides are commonly accepted as reasonable analogs for the actinides, these comparisons suggest the careful study of actinide materials independent of their lanthanide analogs to be of utmost importance to present and future efforts in nuclear industries.« less

Physical and chemical characterization of actinides in soil from Johnston Atoll

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wolf, S.F.; Bates, J.K.; Buck, E.C.

1997-02-01

Characterization of the actinide content of a sample of contaminated coral soil from Johnston Atoll, the site of three non-nuclear destructs of nuclear warhead-carrying THOR missiles in 1962, revealed that >99% of the total actinide content is associated with discrete bomb fragments. After removal of these fragments, there was an inverse correlation between actinide content and soil particle size in particles from 43 to 0.4 {mu}m diameter. Detailed analyses of this remaining soil revealed no discrete actinide phase in these soil particles, despite measurable actinide content. Observations indicate that exposure to the environment has caused the conversion of relatively insolublemore » actinide oxides to the more soluble actinyl oxides and actinyl carbonate coordinated complexes. This process has led to dissolution of actinides from discrete particles and migration to the surrounding soil surfaces, resulting in a dispersion greater than would be expected by physical transport of discrete particles alone. 26 refs., 4 figs., 1 tab.« less

OECD/NEA Ongoing activities related to the nuclear fuel cycle

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cornet, S.M.; McCarthy, K.; Chauvin, N.

2013-07-01

As part of its role in encouraging international collaboration, the OECD Nuclear Energy Agency is coordinating a series of projects related to the Nuclear Fuel Cycle. The Nuclear Science Committee (NSC) Working Party on Scientific Issues of the Nuclear Fuel Cycle (WPFC) comprises five different expert groups covering all aspects of the fuel cycle from front to back-end. Activities related to fuels, materials, physics, separation chemistry, and fuel cycles scenarios are being undertaken. By publishing state-of-the-art reports and organizing workshops, the groups are able to disseminate recent research advancements to the international community. Current activities mainly focus on advanced nuclearmore » systems, and experts are working on analyzing results and establishing challenges associated to the adoption of new materials and fuels. By comparing different codes, the Expert Group on Advanced Fuel Cycle Scenarios is aiming at gaining further understanding of the scientific issues and specific national needs associated with the implementation of advanced fuel cycles. At the back end of the fuel cycle, separation technologies (aqueous and pyrochemical processing) are being assessed. Current and future activities comprise studies on minor actinides separation and post Fukushima studies. Regular workshops are also organized to discuss recent developments on Partitioning and Transmutation. In addition, the Nuclear Development Committee (NDC) focuses on the analysis of the economics of nuclear power across the fuel cycle in the context of changes of electricity markets, social acceptance and technological advances and assesses the availability of the nuclear fuel and infrastructure required for the deployment of existing and future nuclear power. The Expert Group on the Economics of the Back End of the Nuclear Fuel Cycle (EBENFC), in particular, is looking at assessing economic and financial issues related to the long term management of spent nuclear fuel. (authors)« less

Atlas of Atomic Spectral Lines of Neptunium Emitted by Inductively Coupled Plasma

DOE Office of Scientific and Technical Information (OSTI.GOV)

DeKalb, E.L. and Edelson, M. C.

1987-08-01

Optical emission spectra from high-purity Np-237 were generated with a glovebox-enclosed inductively coupled plasma (ICP) source. Spectra covering the 230-700 nm wavelength range are presented along with general commentary on the methodology used in collecting the data. The Ames Laboratory Nuclear Safeguards and Security Program has been charged with the task of developing optical spectroscopic methods to analyze the composition of spent nuclear fuels. Such materials are highly radioactive even after prolonged 'cooling' and are chemically complex. Neptunium (Np) is a highly toxic by-product of nuclear power generation and is found, in low abundance, in spent nuclear fuels. This atlasmore » of the optical emission spectrum of Np, as produced by an inductively coupled plasma (ICP) spectroscopic source, is part of a general survey of the ICP emission spectra of the actinide elements. The ICP emission spectrum of the actinides originates almost exclusively from the electronic relaxation of excited, singly ionized species. Spectral data on the Np ion emission spectrum (i.e., the Np II spectrum) have been reported by Tomkins and Fred [1] and Haaland [2]. Tomkins and Fred excited the Np II spectrum with a Cu spark discharge and identified 114 Np lines in the 265.5 - 436.3 nm spectral range. Haaland, who corrected some spectral line misidentifications in the work of Tomkins and Fred, utilized an enclosed Au spark discharge to excite the Np II spectrum and reported 203 Np lines within the 265.4 - 461.0 nm wavelength range.« less

JOWOG 22/2 - Actinide Chemical Technology (July 9-13, 2012)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jackson, Jay M.; Lopez, Jacquelyn C.; Wayne, David M.

2012-07-05

The Plutonium Science and Manufacturing Directorate provides world-class, safe, secure, and reliable special nuclear material research, process development, technology demonstration, and manufacturing capabilities that support the nation's defense, energy, and environmental needs. We safely and efficiently process plutonium, uranium, and other actinide materials to meet national program requirements, while expanding the scientific and engineering basis of nuclear weapons-based manufacturing, and while producing the next generation of nuclear engineers and scientists. Actinide Process Chemistry (NCO-2) safely and efficiently processes plutonium and other actinide compounds to meet the nation's nuclear defense program needs. All of our processing activities are done in amore » world class and highly regulated nuclear facility. NCO-2's plutonium processing activities consist of direct oxide reduction, metal chlorination, americium extraction, and electrorefining. In addition, NCO-2 uses hydrochloric and nitric acid dissolutions for both plutonium processing and reduction of hazardous components in the waste streams. Finally, NCO-2 is a key team member in the processing of plutonium oxide from disassembled pits and the subsequent stabilization of plutonium oxide for safe and stable long-term storage.« less

Crystalline matrices for the immobilization of plutonium and actinides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Anderson, E.B.; Burakov, E.E.; Galkin, Ya.B.

1996-05-01

The management of weapon plutonium, disengaged as a result of conversion, is considered together with the problem of the actinide fraction of long-lived high level radioactive wastes. It is proposed to use polymineral ceramics based on crystalline host-phases: zircon ZrSiO{sub 4} and zirconium dioxide ZrO{sub 2}, for various variants of the management of plutonium and actinides (including the purposes of long-term safe storage or final disposal from the human activity sphere). It is shown that plutonium and actinides are able to form with these phases on ZrSiO{sub 4} and ZrO{sub 2} was done on laboratory level by the hot pressingmore » method, using the plasmochemical calcination technology. To incorporate simulators of plutonium into the structure of ZrSiO{sub 4} and ZrO{sub 2} in the course of synthesis, an original method developed by the authors as a result of studying the high-uranium zircon (Zr,U) SiO{sub 4} form Chernobyl {open_quotes}lavas{close_quotes} was used.« less

Requirements for Predictive Density Functional Theory Methods for Heavy Materials Equation of State

NASA Astrophysics Data System (ADS)

Mattsson, Ann E.; Wills, John M.

2012-02-01

The difficulties in experimentally determining the Equation of State of actinide and lanthanide materials has driven the development of many computational approaches with varying degree of empiricism and predictive power. While Density Functional Theory (DFT) based on the Schr"odinger Equation (possibly with relativistic corrections including the scalar relativistic approach) combined with local and semi-local functionals has proven to be a successful and predictive approach for many materials, it is not giving enough accuracy, or even is a complete failure, for the actinides. To remedy this failure both an improved fundamental description based on the Dirac Equation (DE) and improved functionals are needed. Based on results obtained using the appropriate fundamental approach of DFT based on the DE we discuss the performance of available semi-local functionals, the requirements for improved functionals for actinide/lanthanide materials, and the similarities in how functionals behave in transition metal oxides. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

Electrodeposition of biaxially textured layers on a substrate

DOEpatents

Bhattacharya, Raghu N; Phok, Sovannary; Spagnol, Priscila; Chaudhuri, Tapas

2013-11-19

Methods of producing one or more biaxially textured layer on a substrate, and articles produced by the methods, are disclosed. An exemplary method may comprise electrodepositing on the substrate a precursor material selected from the group consisting of rare earths, transition metals, actinide, lanthanides, and oxides thereof. An exemplary article (150) may comprise a biaxially textured base material (130), and at least one biaxially textured layer (110) selected from the group consisting of rare earths, transition metals, actinides, lanthanides, and oxides thereof. The at least one biaxially textured layer (110) is formed by electrodeposition on the biaxially textured base material (130).

The JRC-ITU approach to the safety of advanced nuclear fuel cycles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fanghaenel, T.; Rondinella, V.V.; Somers, J.

2013-07-01

The JRC-ITU safety studies of advanced fuels and cycles adopt two main axes. First the full exploitation of still available and highly relevant knowledge and samples from past fuel preparation and irradiation campaigns (complementing the limited number of ongoing programmes). Secondly, the shift of focus from simple property measurement towards the understanding of basic mechanisms determining property evolution and behaviour of fuel compounds during normal, off-normal and accident conditions. The final objective of the second axis is the determination of predictive tools applicable to systems and conditions different from those from which they were derived. State of the art experimentalmore » facilities, extensive networks of partnerships and collaboration with other organizations worldwide, and a developing programme for training and education are essential in this approach. This strategy has been implemented through various programs and projects. The SUPERFACT programme constitutes the main body of existing knowledge on the behavior in-pile of MOX fuel containing minor actinides. It encompassed all steps of a closed fuel cycle. Another international project investigating the safety of a closed cycle is METAPHIX. In this case a U-Pu19-Zr10 metal alloy containing Np, Am and Cm constitutes the fuel. 9 test pins have been prepared and irradiated. In addition to the PIE (Post Irradiation Examination), pyrometallurgical separation of the irradiated fuel has been performed, to demonstrate all the steps of a multiple recycling closed cycle and characterize their safety relevant aspects. Basic studies like thermodynamic fuel properties, fuel-cladding-coolant interactions have also been carried out at JRC-ITU.« less

Method for recovery of actinides from actinide-bearing scrap and waste nuclear material using O/sub 2/F/sub 2/

DOEpatents

Asprey, L.B.; Eller, P.G.

1984-09-12

Method for recovery of actinides from nuclear waste material containing sintered and other oxides thereof and from scrap materials containing the metal actinides using O/sub 2/F/sub 2/ to generate the hexafluorides of the actinides present therein. The fluorinating agent, O/sub 2/F/sub 2/, has been observed to perform the above-described tasks at sufficiently low temperatures that there is virtually no damage to the containment vessels. Moreover, the resulting actinide hexafluorides are not detroyed by high temperature reactions with the walls of the reaction vessel. Dioxygen difluoride is readily prepared, stored and transferred to the place of reaction.

Actinide extraction methods

DOEpatents

Peterman, Dean R [Idaho Falls, ID; Klaehn, John R [Idaho Falls, ID; Harrup, Mason K [Idaho Falls, ID; Tillotson, Richard D [Moore, ID; Law, Jack D [Pocatello, ID

2010-09-21

Methods of separating actinides from lanthanides are disclosed. A regio-specific/stereo-specific dithiophosphinic acid having organic moieties is provided in an organic solvent that is then contacted with an acidic medium containing an actinide and a lanthanide. The method can extend to separating actinides from one another. Actinides are extracted as a complex with the dithiophosphinic acid. Separation compositions include an aqueous phase, an organic phase, dithiophosphinic acid, and at least one actinide. The compositions may include additional actinides and/or lanthanides. A method of producing a dithiophosphinic acid comprising at least two organic moieties selected from aromatics and alkyls, each moiety having at least one functional group is also disclosed. A source of sulfur is reacted with a halophosphine. An ammonium salt of the dithiophosphinic acid product is precipitated out of the reaction mixture. The precipitated salt is dissolved in ether. The ether is removed to yield the dithiophosphinic acid.

On the suitability of lanthanides as actinide analogs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Raymond, Kenneth; Szigethy, Geza

2008-07-01

With the current level of actinide materials used in civilian power generation and the need for safe and efficient methods for the chemical separation of these species from their daughter products and for long-term storage requirements, a detailed understanding of actinide chemistry is of great importance. Due to the unique bonding properties of the f-elements, the lanthanides are commonly used as structural and chemical models for the actinides, but differences in the bonding between these 4f and 5f elements has become a question of immediate applicability to separations technology. This brief overview of actinide coordination chemistry in the Raymond groupmore » at UC Berkeley/LBNL examines the validity of using lanthanide analogs as structural models for the actinides, with particular attention paid to single crystal X-ray diffraction structures. Although lanthanides are commonly accepted as reasonable analogs for the actinides, these comparisons suggest the careful study of actinide materials independent of their lanthanide analogs to be of utmost importance to present and future efforts in nuclear industries. (authors)« less

Gas core reactors for actinide transmutation. [uranium hexafluoride

NASA Technical Reports Server (NTRS)

Clement, J. D.; Rust, J. H.; Wan, P. T.; Chow, S.

1979-01-01

The preliminary design of a uranium hexafluoride actinide transmutation reactor to convert long-lived actinide wastes to shorter-lived fission product wastes was analyzed. It is shown that externally moderated gas core reactors are ideal radiators. They provide an abundant supply of thermal neutrons and are insensitive to composition changes in the blanket. For the present reactor, an initial load of 6 metric tons of actinides is loaded. This is equivalent to the quantity produced by 300 LWR-years of operation. At the beginning, the core produces 2000 MWt while the blanket generates only 239 MWt. After four years of irradiation, the actinide mass is reduced to 3.9 metric tonnes. During this time, the blanket is becoming more fissile and its power rapidly approaches 1600 MWt. At the end of four years, continuous refueling of actinides is carried out and the actinide mass is held constant. Equilibrium is essentially achieved at the end of eight years. At equilibrium, the core is producing 1400 MWt and the blanket 1600 MWt. At this power level, the actinide destruction rate is equal to the production rate from 32 LWRs.

A computationally simple model for determining the time dependent spectral neutron flux in a nuclear reactor core

NASA Astrophysics Data System (ADS)

Schneider, E. A.; Deinert, M. R.; Cady, K. B.

2006-10-01

The balance of isotopes in a nuclear reactor core is key to understanding the overall performance of a given fuel cycle. This balance is in turn most strongly affected by the time and energy-dependent neutron flux. While many large and involved computer packages exist for determining this spectrum, a simplified approach amenable to rapid computation is missing from the literature. We present such a model, which accepts as inputs the fuel element/moderator geometry and composition, reactor geometry, fuel residence time and target burnup and we compare it to OECD/NEA benchmarks for homogeneous MOX and UOX LWR cores. Collision probability approximations to the neutron transport equation are used to decouple the spatial and energy variables. The lethargy dependent neutron flux, governed by coupled integral equations for the fuel and moderator/coolant regions is treated by multigroup thermalization methods, and the transport of neutrons through space is modeled by fuel to moderator transport and escape probabilities. Reactivity control is achieved through use of a burnable poison or adjustable control medium. The model calculates the buildup of 24 actinides, as well as fission products, along with the lethargy dependent neutron flux and the results of several simulations are compared with benchmarked standards.

Converting Maturing Nuclear Sites to Integrated Power Production Islands

DOE PAGES

Solbrig, Charles W.

2011-01-01

Nuclear islands, which are integrated power production sites, could effectively sequester and safeguard the US stockpile of plutonium. A nuclear island, an evolution of the integral fast reactor, utilizes all the Transuranics (Pu plus minor actinides) produced in power production, and it eliminates all spent fuel shipments to and from the site. This latter attribute requires that fuel reprocessing occur on each site and that fast reactors be built on-site to utilize the TRU. All commercial spent fuel shipments could be eliminated by converting all LWR nuclear power sites to nuclear islands. Existing LWR sites have the added advantage ofmore » already possessing a license to produce nuclear power. Each could contribute to an increase in the nuclear power production by adding one or more fast reactors. Both the TRU and the depleted uranium obtained in reprocessing would be used on-site for fast fuel manufacture. Only fission products would be shipped to a repository for storage. The nuclear island concept could be used to alleviate the strain of LWR plant sites currently approaching or exceeding their spent fuel pool storage capacity. Fast reactor breeding ratio could be designed to convert existing sites to all fast reactors, or keep the majority thermal.« less

Dynamic leaching studies of 48 MWd/kgU UO2 commercial spent nuclear fuel under oxic conditions

NASA Astrophysics Data System (ADS)

Serrano-Purroy, D.; Casas, I.; González-Robles, E.; Glatz, J. P.; Wegen, D. H.; Clarens, F.; Giménez, J.; de Pablo, J.; Martínez-Esparza, A.

2013-03-01

The leaching of a high-burn-up spent nuclear fuel (48 MWd/KgU) has been studied in a carbonate-containing solution and under oxic conditions using a Continuously Stirred Tank Flow-Through Reactor (CSTR). Two samples of the fuel, one prepared from the centre of the pellet (labelled CORE) and another one from the fuel pellet periphery, enriched with the so-called High Burn-Up Structure (HBS, labelled OUT) have been used.For uranium and actinides, the results showed that U, Np, Am and Cm gave very similar normalized dissolution rates, while Pu showed slower dissolution rates for both samples. In addition, dissolution rates were consistently two to four times lower for OUT sample compared to CORE sample.Considering the fission products release the main results are that Y, Tc, La and Nd dissolved very similar to uranium; while Cs, Sr, Mo and Rb have up to 10 times higher dissolution rates. Rh, Ru and Zr seemed to have lower dissolution rates than uranium. The lowest dissolution rates were found for OUT sample.Three different contributions were detected on uranium release, modelled and attributed to oxidation layer, fines and matrix release.

Towards Synthesis and Usage of Actinide-Bearing REE Phosphate age Standards: A Progress Report

NASA Astrophysics Data System (ADS)

Pyle, J. M.; Cherniak, D. J.

2006-05-01

Electron microprobe (EMP) dates result from a concentration-time unit conversion, so use of a concentration- based (rather than isotope-ratio based) fictive age standard is warranted. This observation has motivated our mineral synthesis program, aimed at producing actinide-doped REE phosphate EMP dating standards that meet the following criteria: 1) known concentrations of U, Th, and Pb; 2) homogeneous intragrain distribution of all components; 3) of suitable size, either as a single-crystal or polycrystalline sintered ceramic. Single-crystal synthesis of actinide-doped LaPO4 by flux-growth methods results in disproportionation of lanthanide and flux, alkali, and actinide components into phosphate and oxide phases, respectively, and flux- growth methods were abandoned. Actinide-doped La phosphate is successfully prepared by high-T annealing and hydrothermal processing of microcrystalline phosphate; both homogeneity and charge-balance of (Ca, Th, Pb)-bearing LaPO4 increase with increasing solvent acidity during cold-seal hydrothermal synthesis. A combination of pressing and high-T (1400° C) sintering transforms fine-grained (0.1-10 μm) run- products to ceramic pellets with 90-95% theoretical density. Our most recent runs focused on a target composition of La80(CaTh)17(CaU)2(PbTh)1PO4 processed with 6% 2M HCl at 820° C, 0.75 kbar for 1 week. The run products are 0.1-2 μm crystals identified by XRD as La-actinide phosphate solid solution. 2 μm grains (N=16) give a composition (mean±2 sd) of La79.77(1.26)(CaTh)17.87(1.00)(CaU)1.53(0.42)(PbTh)0.82(0.09)PO4. Th (8.07-9.13 wt. %) is homogeneous at the level of analytical precision, and the Pb concentration range (3500-4350 ppm) is restricted relative to untreated precipitate. Uranium concentration values are more variable (6500-10000 ppm). This run yields a fictive age of 702±4 Ma (mean±2 se), compared to the fictive age of 794 Ma for the target composition.

Controlling Actinide Hydration in Mixed Solvent Systems: Towards Tunable Solvent Systems to Close the Fuel Cycle

DOE Office of Scientific and Technical Information (OSTI.GOV)

Clark, Sue B.

2016-10-31

The goal of this project has been to define the extent of hydration the f-elements and other cations in mixed solvent electrolyte systems. Methanol-water and other mixed solvent systems have been studied, where the solvent dielectric constant was varied systematically. Thermodynamic and spectroscopic studies provide details concerning the energetics of complexation and other reactions of these cations. This information has also been used to advance new understanding of the behavior of these cations in a variety of systems, ranging from environmental studies, chromatographic approaches, and ionization processes for mass spectrometry.

Reference commercial high-level waste glass and canister definition

NASA Astrophysics Data System (ADS)

Slate, S. C.; Ross, W. A.; Partain, W. L.

1981-09-01

Technical data and performance characteristics of a high level waste glass and canister intended for use in the design of a complete waste encapsulation package suitable for disposal in a geologic repository are presented. The borosilicate glass contained in the stainless steel canister represents the probable type of high level waste product that is produced in a commercial nuclear-fuel reprocessing plant. Development history is summarized for high level liquid waste compositions, waste glass composition and characteristics, and canister design. The decay histories of the fission products and actinides (plus daughters) calculated by the ORIGEN-II code are presented.

Evaluation of Mass Filtered, Time Dilated, Time-of-Flight Mass Spectrometry

DTIC Science & Technology

2010-01-01

Figure 4.4: Mass resolution dependence on field for selected actinides and surrogates...45 Figure 4.7: Mass resolution dependence on field for selected actinides and actinide surrogates, modeled with no initial...system. A somewhat better mass resolution would need to be achieved in order to separate hydride molecules in the actinide region. However, the

Electron-Transfer-Enhanced Cation-Cation Interactions in Homo- and Heterobimetallic Actinide Complexes: A Relativistic Density Functional Theory Study.

PubMed

Zheng, Ming; Chen, Fang-Yuan; Tian, Jia-Nan; Pan, Qing-Jiang

2018-04-02

To provide deep insight into cation-cation interactions (CCIs) involving hexavalent actinyl species that are major components in spent nuclear fuel and pose important implications for the effective removal of radiotoxic pollutants in the environment, a series of homo- and heterobimetallic actinide complexes supported by cyclopentadienyl (Cp) and polypyrrolic macrocycle (H 4 L) ligands were systematically investigated using relativistic density functional theory. The metal sort in both parts of (THF)(H 2 L)(OAn VI O) and (An') III Cp 3 from U to Np to Pu, as well as the substituent bonding to Cp from electron-donating Me to H to electron-withdrawing Cl, SiH 3 , and SiMe 3 , was changed. Over 0.70 electrons are unraveled to transfer from the electron-rich U III to the electron-deficient An VI of the actinyl moiety, leading to a more stable An V -U IV isomer; in contrast, uranylneptunium and uranylplutonium complexes behave as electron-resonance structures between VI-III and V-IV. These were further corroborated by geometrical and electronic structures. The energies of CCIs (i.e., O exo -An' bonds) were calculated to be -19.6 to -41.2 kcal/mol, affording those of OUO-Np (-23.9 kcal/mol) and OUO-Pu (-19.6 kcal/mol) with less electron transfer (ET) right at the low limit. Topological analyses of the electron density at the O exo -An' bond critical points demonstrate that the CCIs are ET or dative bonds in nature. A positive correlation has been built between the CCIs' strength and corresponding ET amount. It is concluded that the CCIs of O exo -An' are driven by the electrostatic attraction between the actinyl oxo atom (negative) and the actinide ion (positive) and enhanced by their ET. Finally, experimental syntheses of (THF)(H 2 L)(OU VI O)(An') III Cp 3 (An' = U and Np) were well reproduced by thermodynamic calculations that yielded negative free energies in a tetrahydrofuran solution but a positive one for their uranylplutonium analogue, which was synthetically inaccessible. So, our thermodynamics would provide implications for the synthetic possibility of other theoretically designed bimetallic actinide complexes.

RECOVERY OF ACTINIDES FROM AQUEOUS NITRIC ACID SOLUTIONS

DOEpatents

Ader, M.

1963-11-19

A process of recovering actinides is presented. Tetravalent actinides are extracted from rare earths in an aqueous nitric acid solution with a ketone and back-extracted from the ketone into an aqueous medium. The aqueous actinide solution thus obtained, prior to concentration by boiling, is sparged with steam to reduce its ketone to a maximum content of 3 grams per liter. (AEC)

A summary of sodium-cooled fast reactor development

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aoto, Kazumi; Dufour, Philippe; Hongyi, Yang

Much of the basic technology for the Sodium-cooled fast Reactor (SFR) has been established through long term development experience with former fast reactor programs, and is being confirmed by the Phénix end-of-life tests in France, the restart of Monju in Japan, the lifetime extension of BN-600 in Russia, and the startup of the China Experimental Fast Reactor in China. Planned startup in 2014 for new SFRs: BN-800 in Russia and PFBR in India, will further enhance the confirmation of the SFR basic technology. Nowadays, the SFR development has advanced to aiming at establishment of the Generation-IV system which is dedicatedmore » to sustainable energy generation and actinide management, and several advanced SFR concepts are under development such as PRISM, JSFR, ASTRID, PGSFR, BN-1200, and CFR-600. Generation-IV International Forum is an international collaboration framework where various R&D activities are progressing on design of system and component, safety and operation, advanced fuel, and actinide cycle for the Generation-IV SFR development, and will play a beneficial role of promoting them thorough providing an opportunity to share the past experience and the latest data of design and R&D among countries developing SFR.« less

Uranium (III)-Plutonium (III) co-precipitation in molten chloride

NASA Astrophysics Data System (ADS)

Vigier, Jean-François; Laplace, Annabelle; Renard, Catherine; Miguirditchian, Manuel; Abraham, Francis

2018-02-01

Co-management of the actinides in an integrated closed fuel cycle by a pyrochemical process is studied at the laboratory scale in France in the CEA-ATALANTE facility. In this context the co-precipitation of U(III) and Pu(III) by wet argon sparging in LiCl-CaCl2 (30-70 mol%) molten salt at 705 °C is studied. Pu(III) is prepared in situ in the molten salt by carbochlorination of PuO2 and U(III) is then introduced as UCl3 after chlorine purge by argon to avoid any oxidation of uranium up to U(VI) by Cl2. The oxide conversion yield through wet argon sparging is quantitative. However, the preferential oxidation of U(III) in comparison to Pu(III) is responsible for a successive conversion of the two actinides, giving a mixture of UO2 and PuO2 oxides. Surprisingly, the conversion of sole Pu(III) in the same conditions leads to a mixture of PuO2 and PuOCl, characteristic of a partial oxidation of Pu(III) to Pu(IV). This is in contrast with coconversion of U(III)-Pu(III) mixtures but in agreement with the conversion of Ce(III).

Electrowinning of U-Pu onto inert solid cathode in LiCl-KCl eutectic melts containing UCl3 and PuCl3

NASA Astrophysics Data System (ADS)

Sakamura, Yoshiharu; Murakami, Tsuyoshi; Tada, Kohei; Kitawaki, Shinichi

2018-04-01

Electrowinning process was investigated for extracting actinides from molten salts used for the pyrochemical reprocessing of spent nuclear fuels. The separation of actinides from lanthanides is expected to be enhanced by employing inert solid cathodes due to larger potential differences on these cathodes. In this study, the co-deposition behavior of Pu and U metals onto an inert solid cathode made of tungsten was examined in LiCl-KCl eutectic melts containing UCl3 and PuCl3 at 773 K. The standard potential of U3+/U is 0.31 V more positive than that of Pu3+/Pu. The U3+ concentration was varied in the range of 0.11-0.66 wt%, while the Pu3+ concentration was maintained at approximately 2.9 wt%. When the U3+ concentration was not sufficiently low, the deposited U metal readily grew outward from the electrode surface and the electrode surface area rapidly increased, which facilitated only the deposition of U metal. It was estimated that metallic Pu can be efficiently collected along with U at U3+ concentrations lower than ∼0.2 wt%.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shrestha, K.; Antonio, D.; Jaime, M.

Uranium nitride (UN) is one of the most studied actinide materials as it is a promising fuel for the next generation of nuclear reactors. Despite large experimental and theoretical efforts, some of the fundamental questions such as degree of 5 f–electron localization/delocalization and its relationship to magneto-vibrational properties are not resolved yet. We show that the magnetostriction of UN measured in pulsed magnetic fields up to 65 T and below the Néel temperature is large and exhibits complex behavior with two transitions. While the high field anomaly is a field-induced metamagnetic-like transition and affects both magnetisation and magnetostriction, the lowmore » field anomaly does not contribute to the magnetic susceptibility. Our data suggest a change in the nature of the metamagnetic transition from first to second order-like at a tricritical point at T tri ~24 K and H tri ~52 T. The induced magnetic moment at 60 T might suggest that only one subset of magnetic moments has aligned along the field direction. Using the results obtained here we have constructed a magnetic phase diagram of UN. Our studies demonstrate that dilatometry in high fields is an effective method to investigate the magneto-structural coupling in actinide materials.« less

Thermal NF3 fluorination/oxidation of cobalt, yttrium, zirconium, and selected lanthanide oxides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Scheele, Randall D.; McNamara, Bruce K.; Casella, Andrew M.

2013-02-01

This paper presents results of our continuing investigation on the use of nitrogen trifluoride as a fluorination or fluorination/oxidation agent for separating valuable constituents from used nuclear fuels by exploiting the different volatilities of the constituent fission product and actinide fluorides. This article focuses on fission products that do not have volatile fluorides or oxyfluorides at expected operations temperatures. Our thermodynamic calculations show that nitrogen trifluoride has the potential to completely fluorinate fission product oxides to their fluorides. Simultaneous thermogravimetric and differential thermal analyses show that the oxides of cobalt, zirconium, and the lanthanides are fluorinated but do not formmore » volatile fluorides when treated with nitrogen trifluoride at temperatures up to 550°C. Our studies of gadolinium-doped commercial nuclear fuel indicate that nitrogen trifluoride can extract uranium from the non-volatile gadolinium.« less

Bidentate organophosphorus solvent extraction process for actinide recovery and partition

DOEpatents

Schulz, Wallace W.

1976-01-01

A liquid-liquid extraction process for the recovery and partitioning of actinide values from acidic nuclear waste aqueous solutions, the actinide values including trivalent, tetravalent and hexavalent oxidation states is provided and includes the steps of contacting the aqueous solution with a bidentate organophosphorous extractant to extract essentially all of the actinide values into the organic phase. Thereafter the respective actinide fractions are selectively partitioned into separate aqueous solutions by contact with dilute nitric or nitric-hydrofluoric acid solutions. The hexavalent uranium is finally removed from the organic phase by contact with a dilute sodium carbonate solution.

Calcium titanium silicate based glass-ceramic for nuclear waste immobilisation

NASA Astrophysics Data System (ADS)

Sharma, K.; Srivastav, A. P.; Goswami, M.; Krishnan, Madangopal

2018-04-01

Titanate based ceramics (synroc) have been studied for immobilisation of nuclear wastes due to their high radiation and thermal stability. The aim of this study is to synthesis glass-ceramic with stable phases from alumino silicate glass composition and study the loading behavior of actinides in glass-ceramics. The effects of CaO and TiO2 addition on phase evolution and structural properties of alumino silicate based glasses with nominal composition x(10CaO-9TiO2)-y(10Na2O-5 Al2O3-56SiO2-10B2O3); where z = x/y = 1.4-1.8 are reported. The glasses are prepared by melt-quench technique and characterized for thermal and structural properties using DTA and Raman Spectroscopy. Glass transition and peak crystallization temperatures decrease with increase of CaO and TiO2 content, which implies the weakening of glass network and increased tendency of glasses towards crystallization. Sphene (CaTiSiO5) and perovskite (CaTiO3) crystalline phases are confirmed from XRD which are well known stable phase for conditioning of actinides. The microsturcture and elemental analysis indicate the presence of actinide in stable crystalline phases.

Physics and potentials of fissioning plasmas for space power and propulsion

NASA Technical Reports Server (NTRS)

Thom, K.; Schwenk, F. C.; Schneider, R. T.

1976-01-01

Fissioning uranium plasmas are the nuclear fuel in conceptual high-temperature gaseous-core reactors for advanced rocket propulsion in space. A gaseous-core nuclear rocket would be a thermal reactor in which an enriched uranium plasma at about 10,000 K is confined in a reflector-moderator cavity where it is nuclear critical and transfers its fission power to a confining propellant flow for the production of thrust at a specific impulse up to 5000 sec. With a thrust-to-engine weight ratio approaching unity, the gaseous-core nuclear rocket could provide for propulsion capabilities needed for manned missions to the nearby planets and for economical cislunar ferry services. Fueled with enriched uranium hexafluoride and operated at temperatures lower than needed for propulsion, the gaseous-core reactor scheme also offers significant benefits in applications for space and terrestrial power. They include high-efficiency power generation at low specific mass, the burnup of certain fission products and actinides, the breeding of U-233 from thorium with short doubling times, and improved convenience of fuel handling and processing in the gaseous phase.

Helium in inert matrix dispersion fuels

NASA Astrophysics Data System (ADS)

van Veen, A.; Konings, R. J. M.; Fedorov, A. V.

2003-07-01

The behaviour of helium, an important decay product in the transmutation chains of actinides, in dispersion-type inert matrix fuels is discussed. A phenomenological description of its accumulation and release in CERCER and CERMET fuel is given. A summary of recent He-implantation studies with inert matrix metal oxides (ZrO 2, MgAl 2O 4, MgO and Al 2O 3) is presented. A general picture is that for high helium concentrations helium and vacancy defects form helium clusters which convert into over-pressurized bubbles. At elevated temperature helium is released from the bubbles. On some occasions thermal stable nano-cavities or nano-pores remain. On the basis of these results the consequences for helium induced swelling and helium storage in oxide matrices kept at 800-1000 °C will be discussed. In addition, results of He-implantation studies for metal matrices (W, Mo, Nb and V alloys) will be presented. Introduction of helium in metals at elevated temperatures leads to clustering of helium to bubbles. When operational temperatures are higher than 0.5 melting temperature, swelling and helium embrittlement might occur.

The thermodynamics of pyrochemical processes for liquid metal reactor fuel cycles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, I.

1987-01-01

The thermodynamic basis for pyrochemical processes for the recovery and purification of fuel for the liquid metal reactor fuel cycle is described. These processes involve the transport of the uranium and plutonium from one liquid alloy to another through a molten salt. The processes discussed use liquid alloys of cadmium, zinc, and magnesium and molten chloride salts. The oxidation-reduction steps are done either chemically by the use of an auxiliary redox couple or electrochemically by the use of an external electrical supply. The same basic thermodynamics apply to both the salt transport and the electrotransport processes. Large deviations from idealmore » solution behavior of the actinides and lanthanides in the liquid alloys have a major influence on the solubilities and the performance of both the salt transport and electrotransport processes. Separation of plutonium and uranium from each other and decontamination from the more noble fission product elements can be achieved using both transport processes. The thermodynamic analysis is used to make process design computations for different process conditions.« less

The Potential of Different Concepts of Fast Breeder Reactor for the French Fleet Renewal

DOE Office of Scientific and Technical Information (OSTI.GOV)

Massara, Simone; Tetart, Philippe; Lecarpentier, David

2006-07-01

The performances of different concepts of Fast Breeder Reactor (Na-cooled, He-cooled and Pb-cooled FBR) for the current French fleet renewal are analyzed in the framework of a transition scenario to a 100% FBR fleet at the end of the 21. century. Firstly, the modeling of these three FBR types by means of a semi-analytical approach in TIRELIRE - STRATEGIE, the EDF fuel cycle simulation code, is presented, together with some validation elements against ERANOS, the French reference code system for neutronic FBR analysis (CEA). Afterwards, performances comparisons are made in terms of maximum deployable power, natural uranium consumption and wastemore » production. The results show that the FBR maximum deployable capacity, independently from the FBR technology, is highly sensitive to the fuel cycle options, like the spent nuclear fuel cooling time or the Minor Actinides management strategy. Thus, some of the key parameters defining the dynamic of FBR deployment are highlighted, to inform the orientation of R and D in the development and optimization of these systems. (authors)« less

Experimental Investigations into U/TRU Recovery using a Liquid Cadmium Cathode and Salt Containing High Rare Earth Concentrations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shelly X. Li; Steven D. Herrmann; Michael F. Simpson

2009-09-01

Experimental Investigations into U/TRU Recovery using a Liquid Cadmium Cathode and Salt Containing High Rare Earth Concentrations Shelly X. Li, Steven D. Herrmann, and Michael F. Simpson Pyroprocessing Technology Department Idaho National Laboratory P.O. Box 1625, Idaho Falls, ID 83415 USA Abstract - A series of six bench-scale liquid cadmium cathode (LCC) tests was performed to obtain basic separation data with focus on the behavior of rare earth elements. The electrolyte used for the tests was a mixed salt from the Mk-IV and Mk-V electrorefiners, in which spent metal fuels from Experimental Breeder Reactor-II (EBR-II) had been processed. Rare earthmore » (RE) chlorides, such as NdCl3, CeCl3, LaCl3, PrCl3, SmCl3, and YCl3, were spiked into the salt prior to the first test to create an extreme case for investigating rare earth contamination of the actinides collected by a LCC. For the first two LCC tests, an alloy with the nominal composition of 41U-30Pu-5Am-3Np-20Zr-1RE was loaded into the anode baskets as the feed material. The anode feed material for Runs 3 to 6 was spent ternary fuel (U-19Pu-10Zr). The Pu/U ratio in the salt varied from 0.6 to 1.3. Chemical and radiochemical analytical results confirmed that U and transuranics can be collected into the LCC as a group under the given run conditions. The RE contamination level in the LCC product was up to 6.7 wt% of the total metal collected. The detailed data for partitioning of actinides and REs in the salt and Cd phases are reported in the paper.« less

An Approach for Validating Actinide and Fission Product Burnup Credit Criticality Safety Analyses-Isotopic Composition Predictions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Radulescu, Georgeta; Gauld, Ian C; Ilas, Germina

2011-01-01

The expanded use of burnup credit in the United States (U.S.) for storage and transport casks, particularly in the acceptance of credit for fission products, has been constrained by the availability of experimental fission product data to support code validation. The U.S. Nuclear Regulatory Commission (NRC) staff has noted that the rationale for restricting the Interim Staff Guidance on burnup credit for storage and transportation casks (ISG-8) to actinide-only is based largely on the lack of clear, definitive experiments that can be used to estimate the bias and uncertainty for computational analyses associated with using burnup credit. To address themore » issues of burnup credit criticality validation, the NRC initiated a project with the Oak Ridge National Laboratory to (1) develop and establish a technically sound validation approach for commercial spent nuclear fuel (SNF) criticality safety evaluations based on best-available data and methods and (2) apply the approach for representative SNF storage and transport configurations/conditions to demonstrate its usage and applicability, as well as to provide reference bias results. The purpose of this paper is to describe the isotopic composition (depletion) validation approach and resulting observations and recommendations. Validation of the criticality calculations is addressed in a companion paper at this conference. For isotopic composition validation, the approach is to determine burnup-dependent bias and uncertainty in the effective neutron multiplication factor (keff) due to bias and uncertainty in isotopic predictions, via comparisons of isotopic composition predictions (calculated) and measured isotopic compositions from destructive radiochemical assay utilizing as much assay data as is available, and a best-estimate Monte Carlo based method. This paper (1) provides a detailed description of the burnup credit isotopic validation approach and its technical bases, (2) describes the application of the approach for representative pressurized water reactor and boiling water reactor safety analysis models to demonstrate its usage and applicability, (3) provides reference bias and uncertainty results based on a quality-assurance-controlled prerelease version of the Scale 6.1 code package and the ENDF/B-VII nuclear cross section data.« less

Actinide ion sensor for pyroprocess monitoring

DOEpatents

Jue, Jan-fong; Li, Shelly X.

2014-06-03

An apparatus for real-time, in-situ monitoring of actinide ion concentrations which comprises a working electrode, a reference electrode, a container, a working electrolyte, a separator, a reference electrolyte, and a voltmeter. The container holds the working electrolyte. The voltmeter is electrically connected to the working electrode and the reference electrode and measures the voltage between those electrodes. The working electrode contacts the working electrolyte. The working electrolyte comprises an actinide ion of interest. The reference electrode contacts the reference electrolyte. The reference electrolyte is separated from the working electrolyte by the separator. The separator contacts both the working electrolyte and the reference electrolyte. The separator is ionically conductive to the actinide ion of interest. The reference electrolyte comprises a known concentration of the actinide ion of interest. The separator comprises a beta double prime alumina exchanged with the actinide ion of interest.

Multifaceted Modularity: A Key for Stepwise Building of Hierarchical Complexity in Actinide Metal-Organic Frameworks.

PubMed

Dolgopolova, Ekaterina A; Ejegbavwo, Otega A; Martin, Corey R; Smith, Mark D; Setyawan, Wahyu; Karakalos, Stavros G; Henager, Charles H; Zur Loye, Hans-Conrad; Shustova, Natalia B

2017-11-22

Growing necessity for efficient nuclear waste management is a driving force for development of alternative architectures toward fundamental understanding of mechanisms involved in actinide (An) integration inside extended structures. In this manuscript, metal-organic frameworks (MOFs) were investigated as a model system for engineering radionuclide containing materials through utilization of unprecedented MOF modularity, which cannot be replicated in any other type of materials. Through the implementation of recent synthetic advances in the MOF field, hierarchical complexity of An-materials was built stepwise, which was only feasible due to preparation of the first examples of actinide-based frameworks with "unsaturated" metal nodes. The first successful attempts of solid-state metathesis and metal node extension in An-MOFs are reported, and the results of the former approach revealed drastic differences in chemical behavior of extended structures versus molecular species. Successful utilization of MOF modularity also allowed us to structurally characterize the first example of bimetallic An-An nodes. To the best of our knowledge, through combination of solid-state metathesis, guest incorporation, and capping linker installation, we were able to achieve the highest Th wt % in mono- and biactinide frameworks with minimal structural density. Overall, the combination of a multistep synthetic approach with homogeneous actinide distribution and moderate solvothermal conditions could make MOFs an exceptionally powerful tool to address fundamental questions responsible for chemical behavior of An-based extended structures and, therefore, shed light on possible optimization of nuclear waste administration.

Method for fluorination of actinide fluorides and oxyfluorides using O/sub 2/F/sub 2/

DOEpatents

Eller, P.G.; Malm, J.G.; Penneman, R.A.

1984-08-01

The present invention relates generally to methods of fluorination and more particularly to the use of O/sub 2/F/sub 2/ for the preparation of actinide hexafluorides, and for the extraction of deposited actinides and fluorides and oxyfluorides thereof from reaction vessels. The experiments set forth hereinabove demonstrate that the room temperature or below use of O/sub 2/F/sub 2/ will be highly beneficial for the preparation of pure actinide hexafluorides from their respective tetrafluorides without traces of HF being present as occurs using other fluorinating agents: and decontamination of equipment previously exposed to actinides: e.g., walls, feed lines, etc.

Actinides-1981

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

Abstracts of 134 papers which were presented at the Actinides-1981 conference are presented. Approximately half of these papers deal with electronic structure of the actinides. Others deal with solid state chemistry, nuclear physic, thermodynamic properties, solution chemistry, and applied chemistry.

Nonaqueous method for dissolving lanthanide and actinide metals

DOEpatents

Crisler, L.R.

1975-11-11

Lanthanide and actinide beta-diketonate complex molecular compounds are produced by reacting a beta-diketone compound with a lanthanide or actinide element in the elemental metallic state in a mixture of carbon tetrachloride and methanol.

Protactinium and the intersection of actinide and transition metal chemistry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wilson, Richard E.; De Sio, Stephanie; Vallet, Valérie

The role of the 5f and 6d orbitals in the chemistry of the actinide elements has been of considerable interest since their discovery and synthesis. Relativistic effects cause the energetics of the 5f and 6d orbitals to change as the actinide series is traversed left to right imparting a rich and complex chemistry. The 5f and 6d atomic states cross in energy at protactinium (Pa), making it a potential intersection between transition metal and actinide chemistries. Herein, we report the synthesis of a Pa-peroxo cluster, A(6)(Pa4O(O-2)(6)F-12) [A = Rb, Cs, (CH3)(4)N], formed in pursuit of an actinide polyoxometalate. Quantum chemicalmore » calculations at the density functional theory level demonstrate equal 5f and 6d orbital participation in the chemistry of Pa and increasing 5f orbital participation for the heavier actinides. Periodic changes in orbital character to the bonding in the early actinides highlights the influence of the 5f orbitals in their reactivity and chemical structure.« less

Prediction of trivalent actinide amino(poly)carboxylate complex stability constants using linear free energy relationships with the lanthanide series

DOE Office of Scientific and Technical Information (OSTI.GOV)

Uhnak, Nic E.

Prediction of Trivalent Actinide Amino(poly)carboxylate Complex Stability Constants Using Linear Free Energy Relationships with the Lanthanide Series Alternative title: LFER Based Prediction of An(III) APC Stability Constants There is a gap in the literature regarding the complexation of amino(poly)carboxylate (APC) ligands with trivalent actinides (An(III))). The chemistry of the An(III) is nearly identical to that of the trivalent lanthanides Lns, but the An(III) express a slight enhancement when binding APC ligands. Presented in this report is a simple method of predicting the stability constants of the An(III), Pu, Am, Cm, Bk and Cf by using linear free energy relationships (LFER)more » of the An and the lanthanide (Ln) series for 91 APCs. This method produced An stability constants within uncertainty to available literature values for most ligands.« less

Coordination Chemistry of a Strongly-Donating Hydroxylamine with Early Actinides: An Investigation of Redox Properties and Electronic Structure

DOE Office of Scientific and Technical Information (OSTI.GOV)

McSkimming, Alex; Su, Jing; Cheisson, Thibault

Separations of f-block elements are a critical aspect of nuclear waste processing. Redox-based separations offer promise, but challenges remain in stabilizing and differentiating actinides in high oxidation states. The investigation of new ligand types that provide thermodynamic stabilization to high-valent actinides is essential for expanding their fundamental chemistry and to elaborate new separation techniques and storage methods. We report herein the preparation and characterization of Th and U complexes of the pyridyl-hydroxylamine ligand, N-tert-butyl-N-(pyridin-2-yl)hydroxylamine (pyNO–). Electrochemical studies performed on the homoleptic complexes [M(pyNO) 4] (M = Th, U) revealed significant stabilization of the U complex upon one-electron oxidation. The saltmore » [U(pyNO) 4] + was isolated by chemical oxidation of [U(pyNO) 4]; spectroscopic and computational data support assignment as a U V cation.« less

Coordination Chemistry of a Strongly-Donating Hydroxylamine with Early Actinides: An Investigation of Redox Properties and Electronic Structure

DOE PAGES

McSkimming, Alex; Su, Jing; Cheisson, Thibault; ...

2018-03-23

Separations of f-block elements are a critical aspect of nuclear waste processing. Redox-based separations offer promise, but challenges remain in stabilizing and differentiating actinides in high oxidation states. The investigation of new ligand types that provide thermodynamic stabilization to high-valent actinides is essential for expanding their fundamental chemistry and to elaborate new separation techniques and storage methods. We report herein the preparation and characterization of Th and U complexes of the pyridyl-hydroxylamine ligand, N-tert-butyl-N-(pyridin-2-yl)hydroxylamine (pyNO–). Electrochemical studies performed on the homoleptic complexes [M(pyNO) 4] (M = Th, U) revealed significant stabilization of the U complex upon one-electron oxidation. The saltmore » [U(pyNO) 4] + was isolated by chemical oxidation of [U(pyNO) 4]; spectroscopic and computational data support assignment as a U V cation.« less

Inert matrix fuel neutronic, thermal-hydraulic, and transient behavior in a light water reactor

NASA Astrophysics Data System (ADS)

Carmack, W. J.; Todosow, M.; Meyer, M. K.; Pasamehmetoglu, K. O.

2006-06-01

Currently, commercial power reactors in the United States operate on a once-through or open cycle, with the spent nuclear fuel eventually destined for long-term storage in a geologic repository. Since the fissile and transuranic (TRU) elements in the spent nuclear fuel present a proliferation risk, limit the repository capacity, and are the major contributors to the long-term toxicity and dose from the repository, methods and systems are needed to reduce the amount of TRU that will eventually require long-term storage. An option to achieve a reduction in the amount, and modify the isotopic composition of TRU requiring geological disposal is 'burning' the TRU in commercial light water reactors (LWRs) and/or fast reactors. Fuel forms under consideration for TRU destruction in light water reactors (LWRs) include mixed-oxide (MOX), advanced mixed-oxide, and inert matrix fuels. Fertile-free inert matrix fuel (IMF) has been proposed for use in many forms and studied by several researchers. IMF offers several advantages relative to MOX, principally it provides a means for reducing the TRU in the fuel cycle by burning the fissile isotopes and transmuting the minor actinides while producing no new TRU elements from fertile isotopes. This paper will present and discuss the results of a four-bundle, neutronic, thermal-hydraulic, and transient analyses of proposed inert matrix materials in comparison with the results of similar analyses for reference UOX fuel bundles. The results of this work are to be used for screening purposes to identify the general feasibility of utilizing specific inert matrix fuel compositions in existing and future light water reactors. Compositions identified as feasible using the results of these analyses still require further detailed neutronic, thermal-hydraulic, and transient analysis study coupled with rigorous experimental testing and qualification.

The use of nuclear data in the field of nuclear fuel recycling

NASA Astrophysics Data System (ADS)

Martin, Julie-Fiona; Launay, Agnès; Grassi, Gabriele; Binet, Christophe; Lelandais, Jacques; Lecampion, Erick

2017-09-01

AREVA NC La Hague facility is the first step of the nuclear fuel recycling process implemented in France. The processing of the used fuel is governed by high standards of criticality-safety, and strong expectations on the quality of end-products. From the received used fuel assemblies, the plutonium and the uranium are extracted for further energy production purposes within the years following the reprocessing. Furthermore, the ultimate waste - fission products and minor actinides on the one hand, and hulls and end-pieces on the other hand - is adequately packaged for long term disposal. The used fuel is therefore separated into very different materials, and time scales which come into account may be longer than in some other nuclear fields of activity. Given the variety of the handled nuclear materials, as well as the time scales at stake, the importance given to some radionuclides, and hence to the associated nuclear data, can also be specific to the AREVA NC La Hague plant. A study has thus been led to identify a list of the most important radionuclides for the AREVA NC La Hague plant applications, relying on the running constraints of the facility, and the end-products expectations. The activities at the AREVA NC La Hague plant are presented, and the methodology to extract the most important radionuclides for the reprocessing process is detailed.

Uranium nitride as LWR TRISO fuel: Thermodynamic modeling of U-C-N

NASA Astrophysics Data System (ADS)

Besmann, Theodore M.; Shin, Dongwon; Lindemer, Terrence B.

2012-08-01

TRISO coated particle fuel is envisioned as a next generation replacement for current urania pellet fuel in LWR applications. To obtain adequate fissile loading the kernel of the TRISO particle will likely need to be UN instead of UO2. In support of the necessary development effort for this new fuel system, an assessment of phase regions of interest in the U-C-N system was undertaken as the fuel will be prepared by the carbothermic reduction of the oxide followed by nitriding, will be in equilibrium with carbon within the TRISO particle, and will react with minor actinides and fission products. The phase equilibria and thermochemistry of the U-C-N system is reviewed, including nitrogen pressure measurements above various phase fields. Measurements were used to confirm an ideal solution model of UN and UC adequately represents the UC1-xNx phase. Agreement with the data was significantly improved by effectively adjusting the Gibbs free energy of UN by +12 kJ/mol. This also required adjustment of the value for the sesquinitride by +17 kJ/mol to obtain agreement with phase equilibria. The resultant model together with reported values for other phases in the system was used to generate isothermal sections of the U-C-N phase diagram. Nitrogen partial pressures were also computed for regions of interest.

Method for fluorination of actinide fluorides and oxyfluorides thereof using O.sub.2 F.sub.2

DOEpatents

Eller, Phillip G.; Malm, John G.; Penneman, Robert A.

1988-01-01

Method for fluorination of actinides and fluorides and oxyfluorides thereof using O.sub.2 F.sub.2 which generates actinide hexafluorides, and for removal of actinides and compounds thereof from surfaces upon which they appear as unwanted deposits. The fluorinating agent, O.sub.2 F.sub.2, has been observed to readily perform the above-described tasks at sufficiently low temperatures that there is virtually no damage to the containment vessels. Moreover, the resulting actinide hexafluorides are thereby not destroyed by high temperature reactions with the walls of the reaction vessel. Dioxygen difluoride is easily prepared, stored and transferred to the desired place of reaction.

Method for fluorination of actinide fluorides and oxyfluorides thereof using O[sub 2]F[sub 2

DOEpatents

Eller, P.G.; Malm, J.G.; Penneman, R.A.

1988-11-08

Method is described for fluorination of actinides and fluorides and oxyfluorides thereof using O[sub 2]F[sub 2] which generates actinide hexafluorides, and for removal of actinides and compounds thereof from surfaces upon which they appear as unwanted deposits. The fluorinating agent, O[sub 2]F[sub 2], has been observed to readily perform the above-described tasks at sufficiently low temperatures that there is virtually no damage to the containment vessels. Moreover, the resulting actinide hexafluorides are thereby not destroyed by high temperature reactions with the walls of the reaction vessel. Dioxygen difluoride is easily prepared, stored and transferred to the desired place of reaction.

Thermodynamic Properties of Actinides and Actinide Compounds

NASA Astrophysics Data System (ADS)

Konings, Rudy J. M.; Morss, Lester R.; Fuger, Jean

The necessity of obtaining accurate thermodynamic quantities for the actinide elements and their compounds was recognized at the outset of the Manhattan Project, when a dedicated team of scientists and engineers initiated the program to exploit nuclear energy for military purposes. Since the end of World War II, both fundamental and applied objectives have motivated a great deal of further study of actinide thermodynamics. This chapter brings together many research papers and critical reviews on this subject. It also seeks to assess, to systematize, and to predict important properties of the actinide elements, ions, and compounds, especially for species in which there is significant interest and for which there is an experimental basis for the prediction.

Separation of actinides using capillary extraction chromatography-inductively coupled plasma mass spectrometry.

PubMed

Peterson, Dominic S; Montoya, Velma M

2009-08-01

Trace levels of actinides have been separated on capillary extraction chromatography columns. Detection of the actinides was achieved using an inductively coupled plasma mass spectrometer, which was coupled with the extraction chromatography system. In this study, we compare 30-cm long, 4.6 mm i.d. columns to capillary columns (750 microm i.d.) with lengths from 30 cm up to 150 cm. The columns that were tested were packed with TRU resin. We were able to separate a mixture of five actinides ((232)Th, (238)U, (237)Np, (239)Pu, and (241)Am). This work has application to rapid bioassay as well as automated separations of actinide materials.

The interaction of human serum albumin with selected lanthanide and actinide ions: Binding affinities, protein unfolding and conformational changes.

PubMed

Ali, Manjoor; Kumar, Amit; Kumar, Mukesh; Pandey, Badri N

2016-04-01

Human serum albumin (HSA), the most abundant soluble protein in blood plays critical roles in transportation of biomolecules and maintenance of osmotic pressure. In view of increasing applications of lanthanides- and actinides-based materials in nuclear energy, space, industries and medical applications, the risk of exposure with these metal ions is a growing concern for human health. In present study, binding interaction of actinides/lanthanides [thorium: Th(IV), uranium: U(VI), lanthanum: La(III), cerium: Ce(III) and (IV)] with HSA and its structural consequences have been investigated. Ultraviolet-visible, Fourier transform-infrared, Raman, Fluorescence and Circular dichroism spectroscopic techniques were applied to study the site of metal ions interaction, binding affinity determination and the effect of metal ions on protein unfolding and HSA conformation. Results showed that these metal ions interacted with carbonyl (CO..:)/amide(N..-H) groups and induced exposure of aromatic residues of HSA. The fluorescence analysis indicated that the actinide binding altered the microenvironment around Trp214 in the subdomain IIA. Binding affinity of U(VI) to HSA was slightly higher than that of Th(IV). Actinides and Ce(IV) altered the secondary conformation of HSA with a significant decrease of α-helix and an increase of β-sheet, turn and random coil structures, indicating a partial unfolding of HSA. A correlation was observed between metal ion's ability to alter HSA conformation and protein unfolding. Both cationic effects and coordination ability of metal ions seemed to determine the consequences of their interaction with HSA. Present study improves our understanding about the protein interaction of these heavy ions and their impact on its secondary structure. In addition, binding characteristics may have important implications for the development of rational antidote for the medical management of health effects of actinides and lanthanides. Copyright © 2016 Elsevier B.V. and Société Française de Biochimie et Biologie Moléculaire (SFBBM). All rights reserved.

Nuclear Data Needs for Generation IV Nuclear Energy Systems

NASA Astrophysics Data System (ADS)

Rullhusen, Peter

2006-04-01

Nuclear data needs for generation IV systems. Future of nuclear energy and the role of nuclear data / P. Finck. Nuclear data needs for generation IV nuclear energy systems-summary of U.S. workshop / T. A. Taiwo, H. S. Khalil. Nuclear data needs for the assessment of gen. IV systems / G. Rimpault. Nuclear data needs for generation IV-lessons from benchmarks / S. C. van der Marck, A. Hogenbirk, M. C. Duijvestijn. Core design issues of the supercritical water fast reactor / M. Mori ... [et al.]. GFR core neutronics studies at CEA / J. C. Bosq ... [et al]. Comparative study on different phonon frequency spectra of graphite in GCR / Young-Sik Cho ... [et al.]. Innovative fuel types for minor actinides transmutation / D. Haas, A. Fernandez, J. Somers. The importance of nuclear data in modeling and designing generation IV fast reactors / K. D. Weaver. The GIF and Mexico-"everything is possible" / C. Arrenondo Sánchez -- Benmarks, sensitivity calculations, uncertainties. Sensitivity of advanced reactor and fuel cycle performance parameters to nuclear data uncertainties / G. Aliberti ... [et al.]. Sensitivity and uncertainty study for thermal molten salt reactors / A. Biduad ... [et al.]. Integral reactor physics benchmarks- The International Criticality Safety Benchmark Evaluation Project (ICSBEP) and the International Reactor Physics Experiment Evaluation Project (IRPHEP) / J. B. Briggs, D. W. Nigg, E. Sartori. Computer model of an error propagation through micro-campaign of fast neutron gas cooled nuclear reactor / E. Ivanov. Combining differential and integral experiments on [symbol] for reducing uncertainties in nuclear data applications / T. Kawano ... [et al.]. Sensitivity of activation cross sections of the Hafnium, Tanatalum and Tungsten stable isotopes to nuclear reaction mechanisms / V. Avrigeanu ... [et al.]. Generating covariance data with nuclear models / A. J. Koning. Sensitivity of Candu-SCWR reactors physics calculations to nuclear data files / K. S. Kozier, G. R. Dyck. The lead cooled fast reactor benchmark BREST-300: analysis with sensitivity method / V. Smirnov ... [et al.]. Sensitivity analysis of neutron cross-sections considered for design and safety studies of LFR and SFR generation IV systems / K. Tucek, J. Carlsson, H. Wider -- Experiments. INL capabilities for nuclear data measurements using the Argonne intense pulsed neutron source facility / J. D. Cole ... [et al.]. Cross-section measurements in the fast neutron energy range / A. Plompen. Recent measurements of neutron capture cross sections for minor actinides by a JNC and Kyoto University Group / H. Harada ... [et al.]. Determination of minor actinides fission cross sections by means of transfer reactions / M. Aiche ... [et al.] -- Evaluated data libraries. Nuclear data services from the NEA / H. Henriksson, Y. Rugama. Nuclear databases for energy applications: an IAEA perspective / R. Capote Noy, A. L. Nichols, A. Trkov. Nuclear data evaluation for generation IV / G. Noguère ... [et al.]. Improved evaluations of neutron-induced reactions on americium isotopes / P. Talou ... [et al.]. Using improved ENDF-based nuclear data for candu reactor calculations / J. Prodea. A comparative study on the graphite-moderated reactors using different evaluated nuclear data / Do Heon Kim ... [et al.].

Assessment of Metaborate Fusion for the Rapid Dissolution of Solid Samples: Suitability with the Northstar ARSIIe

DTIC Science & Technology

2016-07-01

goal of this project was to develop a rapid dissolution methodology for solid environmental samples and a crude pre- concentration of actinides ...environmental solid samples needed to be removed from the samples prior to actinide separation on the ARSIIe system. As a result of this project, two...procedures were developed, one applicable to the pre-concentration of the actinides only and a second for the pre-concentration of both actinides and

Method for the concentration and separation of actinides from biological and environmental samples

DOEpatents

Horwitz, E. Philip; Dietz, Mark L.

1989-01-01

A method and apparatus for the quantitative recover of actinide values from biological and environmental sample by passing appropriately prepared samples in a mineral acid solution through a separation column of a dialkyl(phenyl)-N,N-dialylcarbamoylmethylphosphine oxide dissolved in tri-n-butyl phosphate on an inert substrate which selectively extracts the actinide values. The actinide values can be eluted either as a group or individually and their presence quantitatively detected by alpha counting.

Method for separating actinides. [Patent application; stripping of Np from organic extractant

DOEpatents

Friedman, H.A.; Toth, L.M.

1980-11-10

An organic solution used for processing spent nuclear reactor fuels is contacted with an aqueous nitric acid solution to strip Np(VI), U(VI), and Pu(IV) from the organic solution into the acid solution. The acid solution is exposed to ultraviolet light, which reduces Np(VI) to Np(V) without reducing U(VI) and Pu(IV). Since the solubility of Np(V) in the organic solution is much lower than that of Np(VI), U(VI), and Pu(IV), a major part of the Np is stripped from the organic solution while leaving most of the U and Pu therein.

Nuclear forensic analysis of a non-traditional actinide sample

DOE PAGES

Doyle, Jamie L.; Kuhn, Kevin John; Byerly, Benjamin; ...

2016-06-15

Nuclear forensic publications, performance tests, and research and development efforts typically target the bulk global inventory of intentionally safeguarded materials, such as plutonium (Pu) and uranium (U). Other materials, such as neptunium (Np), pose a nuclear security risk as well. Trafficking leading to recovery of an interdicted Np sample is a realistic concern especially for materials originating in countries that reprocesses fuel. Using complementary forensic methods, potential signatures for an unknown Np oxide sample were investigated. Measurement results were assessed against published Np processes to present hypotheses as to the original intended use, method of production, and origin for thismore » Np oxide.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mac Donald, Philip Elsworth; Buongiorno, Jacopo; Davis, Cliff Bybee

The purpose of this collaborative Idaho National Engineering and Environmental Laboratory (INEEL) and Massachusetts Institute of Technology (MIT) Laboratory Directed Research and Development (LDRD) project is to investigate the suitability of lead or lead-bismuth cooled fast reactors for producing low-cost electricity as well as for actinide burning. The goal is to identify and analyze the key technical issues in core neutronics, materials, thermal-hydraulics, fuels, and economics associated with the development of this reactor concept. Work has been accomplished in four major areas of research: core neutronic design, plant engineering, material compatibility studies, and coolant activation. The publications derived from workmore » on this project (since project inception) are listed in Appendix A.« less

Nuclear forensic analysis of a non-traditional actinide sample.

PubMed

Doyle, Jamie L; Kuhn, Kevin; Byerly, Benjamin; Colletti, Lisa; Fulwyler, James; Garduno, Katherine; Keller, Russell; Lujan, Elmer; Martinez, Alexander; Myers, Steve; Porterfield, Donivan; Spencer, Khalil; Stanley, Floyd; Townsend, Lisa; Thomas, Mariam; Walker, Laurie; Xu, Ning; Tandon, Lav

2016-10-01

Nuclear forensic publications, performance tests, and research and development efforts typically target the bulk global inventory of intentionally safeguarded materials, such as plutonium (Pu) and uranium (U). Other materials, such as neptunium (Np), pose a nuclear security risk as well. Trafficking leading to recovery of an interdicted Np sample is a realistic concern especially for materials originating in countries that reprocesses fuel. Using complementary forensic methods, potential signatures for an unknown Np oxide sample were investigated. Measurement results were assessed against published Np processes to present hypotheses as to the original intended use, method of production, and origin for this Np oxide. Published by Elsevier B.V.

Chemical Technology Division, Annual technical report, 1991

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1992-03-01

Highlights of the Chemical Technology (CMT) Division's activities during 1991 are presented. In this period, CMT conducted research and development in the following areas: (1) electrochemical technology, including advanced batteries and fuel cells; (2) technology for fluidized-bed combustion and coal-fired magnetohydrodynamics; (3) methods for treatment of hazardous and mixed hazardous/radioactive waste; (4) the reaction of nuclear waste glass and spent fuel under conditions expected for an unsaturated repository; (5) processes for separating and recovering transuranic elements from nuclear waste streams; (6) recovery processes for discharged fuel and the uranium blanket in the Integral Fast Reactor (IFR); (7) processes for removalmore » of actinides in spent fuel from commercial water-cooled nuclear reactors and burnup in IFRs; and (8) physical chemistry of selected materials in environments simulating those of fission and fusion energy systems. The Division also conducts basic research in catalytic chemistry associated with molecular energy resources; chemistry of superconducting oxides and other materials of interest with technological application; interfacial processes of importance to corrosion science, catalysis, and high-temperature superconductivity; and the geochemical processes involved in water-rock interactions occurring in active hydrothermal systems. In addition, the Analytical Chemistry Laboratory in CMT provides a broad range of analytical chemistry support services to the technical programs at Argonne National Laboratory (ANL).« less

Chemical Technology Division, Annual technical report, 1991

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1992-03-01

Highlights of the Chemical Technology (CMT) Division`s activities during 1991 are presented. In this period, CMT conducted research and development in the following areas: (1) electrochemical technology, including advanced batteries and fuel cells; (2) technology for fluidized-bed combustion and coal-fired magnetohydrodynamics; (3) methods for treatment of hazardous and mixed hazardous/radioactive waste; (4) the reaction of nuclear waste glass and spent fuel under conditions expected for an unsaturated repository; (5) processes for separating and recovering transuranic elements from nuclear waste streams; (6) recovery processes for discharged fuel and the uranium blanket in the Integral Fast Reactor (IFR); (7) processes for removalmore » of actinides in spent fuel from commercial water-cooled nuclear reactors and burnup in IFRs; and (8) physical chemistry of selected materials in environments simulating those of fission and fusion energy systems. The Division also conducts basic research in catalytic chemistry associated with molecular energy resources; chemistry of superconducting oxides and other materials of interest with technological application; interfacial processes of importance to corrosion science, catalysis, and high-temperature superconductivity; and the geochemical processes involved in water-rock interactions occurring in active hydrothermal systems. In addition, the Analytical Chemistry Laboratory in CMT provides a broad range of analytical chemistry support services to the technical programs at Argonne National Laboratory (ANL).« less

A new code for modelling the near field diffusion releases from the final disposal of nuclear waste

NASA Astrophysics Data System (ADS)

Vopálka, D.; Vokál, A.

2003-01-01

The canisters with spent nuclear fuel produced during the operation of WWER reactors at the Czech power plants are planned, like in other countries, to be disposed of in an underground repository. Canisters will be surrounded by compacted bentonite that will retard the migration of safety-relevant radionuclides into the host rock. A new code that enables the modelling of the critical radionuclides transport from the canister through the bentonite layer in the cylindrical geometry was developed. The code enables to solve the diffusion equation for various types of initial and boundary conditions by means of the finite difference method and to take into account the non-linear shape of the sorption isotherm. A comparison of the code reported here with code PAGODA, which is based on analytical solution of the transport equation, was made for the actinide chain 4N+3 that includes 239Pu. A simple parametric study of the releases of 239Pu, 129I, and 14C into geosphere is discussed.

Thermal and physicochemical properties important for the long term behavior of nuclear waste glasses

NASA Astrophysics Data System (ADS)

Matzke, Hj.; Vernaz, E.

High level nuclear waste from reprocessing of spent nuclear fuel has to be solidified in a stable matrix for safe long-time storage. Vitrification in borosilicate glasses is the technique accepted worldwide as the best combination of engineering constraints from fabrication and physicochemical properties of the matrix. A number of different glasses was developed in different national programs. The criteria and the reasons for selecting the final compositions are described briefly. Emphasis is placed on the French product R7T7 and on thermal and physicochemical properties though glasses developed in other national projects (e.g., the German product GP 98/12, etc.) are also treated. The basic physical and mechanical properties and the chemical durability of the glass in contact with water are described. The basic mechanisms of aqueous corrosion are discussed and the evolving modelling of the leaching process is dealt with, as well as effects of container material, backfill, etc. The thermal behavior has also been studied and extensive data exist on diffusion of glass constituents (Na) and of interesting elements of the waste such as the alkalis Rb and Cs or the actinides U and Pu, as well as on crystallization processes in the glass during storage at elevated temperatures. Emphasis is placed on the radiation stability of the glasses, based on extensive studies using short-lived actinides (e.g., 244Cm) or ion implantation to produce the damage expected during long storage at an accelerated rate. The radiation stability is shown to be very good, if realistic damage conditions are used. The knowledge accumulated in the past years is used to evaluate and predict the long-term evolution of the glass under storage conditions.

Analysis of large soil samples for actinides

DOEpatents

Maxwell, III; Sherrod, L [Aiken, SC

2009-03-24

A method of analyzing relatively large soil samples for actinides by employing a separation process that includes cerium fluoride precipitation for removing the soil matrix and precipitates plutonium, americium, and curium with cerium and hydrofluoric acid followed by separating these actinides using chromatography cartridges.

Method for the concentration and separation of actinides from biological and environmental samples

DOEpatents

Horwitz, E.P.; Dietz, M.L.

1989-05-30

A method and apparatus for the quantitative recover of actinide values from biological and environmental sample by passing appropriately prepared samples in a mineral acid solution through a separation column of a dialkyl(phenyl)-N,N-dialylcarbamoylmethylphosphine oxide dissolved in tri-n-butyl phosphate on an inert substrate which selectively extracts the actinide values. The actinide values can be eluted either as a group or individually and their presence quantitatively detected by alpha counting. 3 figs.

Fate and transport of plutonium-239 + 240 and Americium-241 in the soil of Rocky Flats, Colorado

DOE Office of Scientific and Technical Information (OSTI.GOV)

Litaor, M.I.; Barth, G.R.; Zika, E.M.

1996-07-01

Actinides contamination of soils around Rocky Flats, CO, resulted from leaking drums of Pu-contaminated oil stored at an outdoor site. The transport of these actinides through the soil to groundwater was studied using an advanced monitoring system (MS). The fully automated, remotely controlled MS gathered real-time data on soil water content, groundwater level, and timing of gravitationally flowing water. Controlled rain simulations coupled with measurements of volume flux and actinide activities provided essential information about the fate and transport of Pu-239 + 240 and Am-241. Volume fluxes at most sampling locations were similar, regardless of the antecedent moisture or themore » duration, frequency, and intensity of the simulated rain. Actinide activities were not correlated with the measured volume flux, or the duration, frequency, and intensity of the simulated rain. Flow was facilitated primarily via macropore channeling. The relatively short residence time precluded a continuous interaction between the soil and the flowing water, which minimized the movement of actinides in the soil. Actinide activities in the interstitial water collected from the upper 20 cm of the soil were significantly higher (P>0.001) than water collected at deeper sampling depths (20-70 cm). Actinide activity in water samples from the deepest sampling depth (40-70 cm) did not exceed 0.4 Bq/L. These results suggest that, under the experimental conditions, the movement of actinides was restricted to the top 20 cm. A transport mechanism involving discrete Pu oxide particles, coupled with macropore channeling is proposed to explain the observed actinide activities in the soil. 31 refs., 6 figs., 7 tabs.« less

Microscopic Fuel Particles Produced by Self-Assembly of Actinide Nanoclusters on Carbon Nanomaterials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Na, Chongzheng

2016-10-17

Many consider further development of nuclear power to be essential for sustained development of society; however, the fuel forms currently used are expensive to recycle. In this project, we sought to create the knowledge and knowhow that are needed to produce nanocomposite materials by directly depositing uranium nanoclusters on networks of carbon-­ based nanomaterials. The objectives of the proposed work were to (1) determine the control of uranium nanocluster surface chemistry on nanocomposite formation, (2) determine the control of carbon nanomaterial surface chemistry on nanocomposite formation, and (3) develop protocols for synthesizing uranium-­carbon nanomaterials. After examining a wide variety ofmore » synthetic methods, we show that synthesizing graphene-­supported UO 2 nanocrystals in polar ethylene glycol compounds by polyol reduction under boiling reflux can enable the use of an inexpensive graphene precursor graphene oxide in the production of uranium-carbon nanocomposites in a one-­pot process. We further show that triethylene glycol is the most suitable solvent for producing nanometer-­sized UO 2 crystals compared to monoethylene glycol, diethylene glycol, and polyethylene glycol. Graphene-­supported UO 2 nanocrystals synthesized with triethylene glycol show evidence of heteroepitaxy, which can be beneficial for facilitating heat transfer in nuclear fuel particles. Furthermore, we show that graphene-supported UO 2 nanocrystals synthesized by polyol reduction can be readily stored in alcohols, preventing oxidation from the prevalent oxygen in air. Together, these methods provide a facile approach for preparing and storing graphene-supported UO nanocrystals for further investigation and development under ambient conditions.« less

Precise U and Pu isotope ratio measurements in nuclear samples by hyphenating capillary electrophoresis and MC-ICPMS.

PubMed

Martelat, Benoit; Isnard, Helene; Vio, Laurent; Dupuis, Erwan; Cornet, Terence; Nonell, Anthony; Chartier, Frederic

2018-06-22

Precise isotopic and elemental characterization of spent nuclear fuel is a major concern for the validation of the neutronic calculation codes and waste management strategy in the nuclear industry. Generally, the elements of interest, particularly U and Pu which are the two major elements present in spent fuel, are purified by ion exchange or extractant resins before off-line measurements by thermal ionization mass spectrometry. The aim of the present work was to develop a new analytical approach based on capillary electrophoresis (CE) hyphenated to a multicollector inductively coupled plasma mass spectrometer (MC-ICPMS) for online isotope ratio measurements. An electrophoretic separation protocol of U, Pu and the fraction containing fission products and minor actinides (Am and Cm) was developed using acetic acid as the electrolyte and complexing agent. The instrumentation for CE was designed to be used in a glove box and a laboratory-built interface was developed for hyphenation with MC-ICPMS. The separation was realized with only a few nL of a solution of spent nuclear fuel and the reproducibilities obtained on the U and Pu isotope ratios were on the order of a few ‰ which is comparable to those obtained by thermal ionization mass spectrometer (TIMS). This innovative protocol allowed a tremendous reduction of the analyte masses from μg to ng and also a drastic reduction of the liquid waste production from mL to μL. In addition, the time of analysis was shorted by at least a factor three. All of these improved parameters are of major interest for nuclear applications.

Waste Minimization Study on Pyrochemical Reprocessing Processes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Boussier, H.; Conocar, O.; Lacquement, J.

2006-07-01

Ideally a new pyro-process should not generate more waste, and should be at least as safe and cost effective as the hydrometallurgical processes currently implemented at industrial scale. This paper describes the thought process, the methodology and some results obtained by process integration studies to devise potential pyro-processes and to assess their capability of achieving this challenging objective. As example the assessment of a process based on salt/metal reductive extraction, designed for the reprocessing of Generation IV carbide spent fuels, is developed. Salt/metal reductive extraction uses the capability of some metals, aluminum in this case, to selectively reduce actinide fluoridesmore » previously dissolved in a fluoride salt bath. The reduced actinides enter the metal phase from which they are subsequently recovered; the fission products remain in the salt phase. In fact, the process is not so simple, as it requires upstream and downstream subsidiary steps. All these process steps generate secondary waste flows representing sources of actinide leakage and/or FP discharge. In aqueous processes the main solvent (nitric acid solution) has a low boiling point and evaporate easily or can be removed by distillation, thereby leaving limited flow containing the dissolved substance behind to be incorporated in a confinement matrix. From the point of view of waste generation, one main handicap of molten salt processes, is that the saline phase (fluoride in our case) used as solvent is of same nature than the solutes (radionuclides fluorides) and has a quite high boiling point. So it is not so easy, than it is with aqueous solutions, to separate solvent and solutes in order to confine only radioactive material and limit the final waste flows. Starting from the initial block diagram devised two years ago, the paper shows how process integration studies were able to propose process fittings which lead to a reduction of the waste variety and flows leading at an 'ideal' new block diagram allowing internal solvent recycling, and self eliminating reactants. This new flowsheet minimizes the quantity of inactive inlet flows that would have inevitably to be incorporated in a final waste form. The study identifies all knowledge gaps to be filled and suggest some possible R and D issues to confirm or infirm the feasibility of the proposed process fittings. (authors)« less

Tricritical point from high-field magnetoelastic and metamagnetic effects in UN.

PubMed

Shrestha, K; Antonio, D; Jaime, M; Harrison, N; Mast, D S; Safarik, D; Durakiewicz, T; Griveau, J-C; Gofryk, K

2017-07-26

Uranium nitride (UN) is one of the most studied actinide materials as it is a promising fuel for the next generation of nuclear reactors. Despite large experimental and theoretical efforts, some of the fundamental questions such as degree of 5 f-electron localization/delocalization and its relationship to magneto-vibrational properties are not resolved yet. Here we show that the magnetostriction of UN measured in pulsed magnetic fields up to 65 T and below the Néel temperature is large and exhibits complex behavior with two transitions. While the high field anomaly is a field-induced metamagnetic-like transition and affects both magnetisation and magnetostriction, the low field anomaly does not contribute to the magnetic susceptibility. Our data suggest a change in the nature of the metamagnetic transition from first to second order-like at a tricritical point at T tri  ∼ 24 K and H tri  ∼ 52 T. The induced magnetic moment at 60 T might suggest that only one subset of magnetic moments has aligned along the field direction. Using the results obtained here we have constructed a magnetic phase diagram of UN. These studies demonstrate that dilatometry in high fields is an effective method to investigate the magneto-structural coupling in actinide materials.

Tricritical point from high-field magnetoelastic and metamagnetic effects in UN

DOE PAGES

Shrestha, K.; Antonio, D.; Jaime, M.; ...

2017-07-26

Uranium nitride (UN) is one of the most studied actinide materials as it is a promising fuel for the next generation of nuclear reactors. Despite large experimental and theoretical efforts, some of the fundamental questions such as degree of 5 f–electron localization/delocalization and its relationship to magneto-vibrational properties are not resolved yet. We show that the magnetostriction of UN measured in pulsed magnetic fields up to 65 T and below the Néel temperature is large and exhibits complex behavior with two transitions. While the high field anomaly is a field-induced metamagnetic-like transition and affects both magnetisation and magnetostriction, the lowmore » field anomaly does not contribute to the magnetic susceptibility. Our data suggest a change in the nature of the metamagnetic transition from first to second order-like at a tricritical point at T tri ~24 K and H tri ~52 T. The induced magnetic moment at 60 T might suggest that only one subset of magnetic moments has aligned along the field direction. Using the results obtained here we have constructed a magnetic phase diagram of UN. Our studies demonstrate that dilatometry in high fields is an effective method to investigate the magneto-structural coupling in actinide materials.« less

PLANTS AS BIO-MONITORS FOR 137CS, 238PU, 239, 240PU AND 40K AT THE SAVANNAH RIVER SITE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Caldwell, E.; Duff, M.; Ferguson, C.

2010-12-16

The nuclear fuel cycle generates a considerable amount of radioactive waste, which often includes nuclear fission products, such as strontium-90 ({sup 90}Sr) and cesium-137 ({sup 137}Cs), and actinides such as uranium (U) and plutonium (Pu). When released into the environment, large quantities of these radionuclides can present considerable problems to man and biota due to their radioactive nature and, in some cases as with the actinides, their chemical toxicity. Radionuclides are expected to decay at a known rate. Yet, research has shown the rate of elimination from an ecosystem to differ from the decay rate due to physical, chemical andmore » biological processes that remove the contaminant or reduce its biological availability. Knowledge regarding the rate by which a contaminant is eliminated from an ecosystem (ecological half-life) is important for evaluating the duration and potential severity of risk. To better understand a contaminants impact on an environment, consideration should be given to plants. As primary producers, they represent an important mode of contamination transfer from sediments and soils into the food chain. Contaminants that are chemically and/or physically sequestered in a media are less likely to be bio-available to plants and therefore an ecosystem.« less

PROCESS OF PRODUCING ACTINIDE METALS

DOEpatents

Magel, T.T.

1959-07-14

The preparation of actinide metals in workable, coherent form is described. In general, the objects of the invention are achieved by heating a mixture of an oxide and a halide of an actinide metal such as uranium with an alkali metal on alkaline earth metal reducing agent in the presence of iodine.

Process to remove actinides from soil using magnetic separation

DOEpatents

Avens, Larry R.; Hill, Dallas D.; Prenger, F. Coyne; Stewart, Walter F.; Tolt, Thomas L.; Worl, Laura A.

1996-01-01

A process of separating actinide-containing components from an admixture including forming a slurry including actinide-containing components within an admixture, said slurry including a dispersion-promoting surfactant, adjusting the pH of the slurry to within a desired range, and, passing said slurry through a pretreated matrix material, said matrix material adapted to generate high magnetic field gradients upon the application of a strong magnetic field exceeding about 0.1 Tesla whereupon a portion of said actinide-containing components are separated from said slurry and remain adhered upon said matrix material is provided.

Actinide targets for the synthesis of super-heavy elements

DOE PAGES

Roberto, J.; Alexander, Charles W.; Boll, Rose Ann; ...

2015-06-18

Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing themore » production of rare actinides including 249Bk, 251Cf, and 254Es are described.« less

Magnetocrystalline anisotropy in UMn 2 Ge 2 and related Mn-based actinide ferromagnets

DOE PAGES

Parker, David S.; Ghimire, Nirmal; Singleton, John; ...

2015-05-04

We presenmore » t magnetization isotherms in pulsed magnetic fields up to 62 Tesla, supported by first principles calculations, demonstrating a huge uniaxial magnetocrystalline anisotropy energy - approximately 20 MJ/m 3 - in UMn 2 Ge 2 . This large anisotropy results from the extremely strong spin-orbit coupling affecting the uranium 5 f electrons, which in the calculations exhibit a substantial orbital moment exceeding 2 μ B. Finally, we also find from theoretical calculations that a number of isostructural Mn-actinide compounds are expected to have similarly large anisotropy.« less

The reduced transition probabilities for excited states of rare-earths and actinide even-even nuclei

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghumman, S. S.

The theoretical B(E2) ratios have been calculated on DF, DR and Krutov models. A simple method based on the work of Arima and Iachello is used to calculate the reduced transition probabilities within SU(3) limit of IBA-I framework. The reduced E2 transition probabilities from second excited states of rare-earths and actinide even–even nuclei calculated from experimental energies and intensities from recent data, have been found to compare better with those calculated on the Krutov model and the SU(3) limit of IBA than the DR and DF models.

NEW COLUMN SEPARATION METHOD FOR EMERGENCY URINE SAMPLES

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maxwell, S; Brian Culligan, B

2007-08-28

The Savannah River Site Environmental Bioassay Lab participated in the 2007 NRIP Emergency Response program administered by the National Institute for Standards and Technology (NIST) in May, 2007. A new rapid column separation method was applied directly to the NRIP 2007 emergency urine samples, with only minimal sample preparation to reduce preparation time. Calcium phosphate precipitation, previously used to pre-concentrate actinides and Sr-90 in NRIP 2006 urine and water samples, was not used for the NRIP 2007 urine samples. Instead, the raw urine was acidified and passed directly through the stacked resin columns (TEVA+TRU+SR Resins) to separate the actinides andmore » strontium from the NRIP urine samples more quickly. This improvement reduced sample preparation time for the NRIP 2007 emergency urine analyses significantly. This approach works well for small volume urine samples expected during an emergency response event. Based on initial feedback from NIST, the SRS Environmental Bioassay Lab had the most rapid analysis times for actinides and strontium-90 analyses for NRIP 2007 urine samples.« less

Actinide electronic structure and atomic forces

NASA Astrophysics Data System (ADS)

Albers, R. C.; Rudin, Sven P.; Trinkle, Dallas R.; Jones, M. D.

2000-07-01

We have developed a new method[1] of fitting tight-binding parameterizations based on functional forms developed at the Naval Research Laboratory.[2] We have applied these methods to actinide metals and report our success using them (see below). The fitting procedure uses first-principles local-density-approximation (LDA) linear augmented plane-wave (LAPW) band structure techniques[3] to first calculate an electronic-structure band structure and total energy for fcc, bcc, and simple cubic crystal structures for the actinide of interest. The tight-binding parameterization is then chosen to fit the detailed energy eigenvalues of the bands along symmetry directions, and the symmetry of the parameterization is constrained to agree with the correct symmetry of the LDA band structure at each eigenvalue and k-vector that is fit to. By fitting to a range of different volumes and the three different crystal structures, we find that the resulting parameterization is robust and appears to accurately calculate other crystal structures and properties of interest.

A combined Cyanex-923/HEH[EHP]/Dodecane solvent for recovery of transuranic elements from used nuclear fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, A.; Nash, K.L.

2013-07-01

The separation of minor actinides from fission product lanthanides remains a primary challenge for enabling the recycle of used nuclear fuel. To minimize the complexity of materials handling, combining extractant processes has become an increasingly attractive option. Unfortunately, combined processes sometimes suffer reduced utility due to strong dipole-dipole interactions between the extractants. The results reported here describe a system based on a combination of commercially available extractants Cyanex-923 and HEH[EHP]. In contrast to other combined extractant systems, these extractant molecules exhibit comparatively weak interactions, reducing the impact of secondary interactions. In this process, mixtures containing equal ratios of Cyanex-923 andmore » HEH[EHP] were seen to co-extract americium and the lanthanides from nitric acid solutions. Stripping of An(III) was effectively achieved through contact with an aqueous phase comprised of glycine (for pH control) and a polyamino-poly-carboxylate stripping reagent that selectively removes An(III) from the extractant phase. The lanthanides can then be stripped from the loaded organic phase contacting with high nitric acid concentrations. Extraction of fission products zirconium and molybdenum was also investigated and potential strategies for their management have been identified. The work presented demonstrates the feasibility of combining Cyanex-923 and HEH[EHP] for separating and recovering the transuranic elements from the Ln(III). (authors)« less

Defense Technical Information Center Thesaurus

DTIC Science & Technology

2000-10-01

acquisition radar 4 + Indicates existence of further generic levels of the term DTIC Thesaurus Actuators Acridines Actinide series (cont.) Activated sintering...BT Heterocyclic compounds+ Uranium+ BT Sintering Acrilan Actinide series compounds Activated sludge process use Acrylonitrile polymers RT Actinide...Waste treatment+ Protactinium compounds Acronyms Thorium compounds+ Activation use Abbreviations Transuranium compounds+ UF Energizing Uranium compounds

Abundance of live 244Pu in deep-sea reservoirs on Earth points to rarity of actinide nucleosynthesis

PubMed Central

Wallner, A.; Faestermann, T.; Feige, J.; Feldstein, C.; Knie, K.; Korschinek, G.; Kutschera, W.; Ofan, A.; Paul, M.; Quinto, F.; Rugel, G.; Steier, P.

2015-01-01

Half of the heavy elements including all actinides are produced in r-process nucleosynthesis, whose sites and history remain a mystery. If continuously produced, the Interstellar Medium is expected to build-up a quasi-steady state of abundances of short-lived nuclides (with half-lives ≤100 My), including actinides produced in r-process nucleosynthesis. Their existence in today’s interstellar medium would serve as a radioactive clock and would establish that their production was recent. In particular 244Pu, a radioactive actinide nuclide (half-life=81 My), can place strong constraints on recent r-process frequency and production yield. Here we report the detection of live interstellar 244Pu, archived in Earth’s deep-sea floor during the last 25 My, at abundances lower than expected from continuous production in the Galaxy by about 2 orders of magnitude. This large discrepancy may signal a rarity of actinide r-process nucleosynthesis sites, compatible with neutron-star mergers or with a small subset of actinide-producing supernovae. PMID:25601158

The role of the 5f valence orbitals of early actinides in chemical bonding

PubMed Central

Vitova, T.; Pidchenko, I.; Fellhauer, D.; Bagus, P. S.; Joly, Y.; Pruessmann, T.; Bahl, S.; Gonzalez-Robles, E.; Rothe, J.; Altmaier, M.; Denecke, M. A.; Geckeis, H.

2017-01-01

One of the long standing debates in actinide chemistry is the level of localization and participation of the actinide 5f valence orbitals in covalent bonds across the actinide series. Here we illuminate the role of the 5f valence orbitals of uranium, neptunium and plutonium in chemical bonding using advanced spectroscopies: actinide M4,5 HR-XANES and 3d4f RIXS. Results reveal that the 5f orbitals are active in the chemical bonding for uranium and neptunium, shown by significant variations in the level of their localization evidenced in the spectra. In contrast, the 5f orbitals of plutonium appear localized and surprisingly insensitive to different bonding environments. We envisage that this report of using relative energy differences between the 5fδ/ϕ and 5fπ*/5fσ* orbitals as a qualitative measure of overlap-driven actinyl bond covalency will spark activity, and extend to numerous applications of RIXS and HR-XANES to gain new insights into the electronic structures of the actinide elements. PMID:28681848

The role of the 5f valence orbitals of early actinides in chemical bonding

NASA Astrophysics Data System (ADS)

Vitova, T.; Pidchenko, I.; Fellhauer, D.; Bagus, P. S.; Joly, Y.; Pruessmann, T.; Bahl, S.; Gonzalez-Robles, E.; Rothe, J.; Altmaier, M.; Denecke, M. A.; Geckeis, H.

2017-07-01

One of the long standing debates in actinide chemistry is the level of localization and participation of the actinide 5f valence orbitals in covalent bonds across the actinide series. Here we illuminate the role of the 5f valence orbitals of uranium, neptunium and plutonium in chemical bonding using advanced spectroscopies: actinide M4,5 HR-XANES and 3d4f RIXS. Results reveal that the 5f orbitals are active in the chemical bonding for uranium and neptunium, shown by significant variations in the level of their localization evidenced in the spectra. In contrast, the 5f orbitals of plutonium appear localized and surprisingly insensitive to different bonding environments. We envisage that this report of using relative energy differences between the 5fδ/φ and 5fπ*/5fσ* orbitals as a qualitative measure of overlap-driven actinyl bond covalency will spark activity, and extend to numerous applications of RIXS and HR-XANES to gain new insights into the electronic structures of the actinide elements.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Selle, J E

Attempts were made to apply the Kaufman method of calculating binary phase diagrams to the calculation of binary phase diagrams between the rare earths, actinides, and the refractory transition metals. Difficulties were encountered in applying the method to the rare earths and actinides, and modifications were necessary to provide accurate representation of known diagrams. To calculate the interaction parameters for rare earth-rare earth diagrams, it was necessary to use the atomic volumes for each of the phases: liquid, body-centered cubic, hexagonal close-packed, and face-centered cubic. Determination of the atomic volumes of each of these phases for each element is discussedmore » in detail. In some cases, empirical means were necessary. Results are presented on the calculation of rare earth-rare earth, rare earth-actinide, and actinide-actinide diagrams. For rare earth-refractory transition metal diagrams and actinide-refractory transition metal diagrams, empirical means were required to develop values for the enthalpy of vaporization for rare earth elements and values for the constant (C) required when intermediate phases are present. Results of using the values determined for each element are presented.« less

Method for recovery of actinides from refractory oxides thereof using O.sub. F.sub.2

DOEpatents

Asprey, Larned B.; Eller, Phillip G.

1988-01-01

Method for recovery of actinides from nuclear waste material containing sintered and other oxides thereof using O.sub.2 F.sub.2 to generate the hexafluorides of the actinides present therein. The fluorinating agent, O.sub.2 F.sub.2, has been observed to perform the above-described tasks at sufficiently low temperatures that there is virtually no damage to the containment vessels. Moreover, the resulting actinide hexafluorides are not destroyed by high temperature reactions with the walls of the reaction vessel. Dioxygen difluoride is readily prepared, stored and transferred to the place of reaction.

DOE Office of Scientific and Technical Information (OSTI.GOV)

B.R. Westphal; J.C. Price; R.D. Mariani

The pyroprocessing of used nuclear fuel via electrorefining requires the continued addition of uranium trichloride to sustain operations. Uranium trichloride is utilized as an oxidant in the system to allow separation of uranium metal from the minor actinides and fission products. The inventory of uranium trichloride had diminished to a point that production was necessary to continue electrorefiner operations. Following initial experimentation, cupric chloride was chosen as a reactant with uranium metal to synthesize uranium trichloride. Despite the variability in equipment and charge characteristics, uranium trichloride was produced in sufficient quantities to maintain operations in the electrorefiner. The results andmore » conclusions from several experiments are presented along with a set of optimized operating conditions for the synthesis of uranium trichloride.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schwantes, Jon M.

Kelly Fitzgerald Kelly Fitzgerald assisted with laboratory testing for an ongoing R&D project known as Electrochemically Modulated Separation (EMS) for on-line rapid preseparations of actinides prior to mass spectrometry analysis. Ryne Burgess Ryne Burgess used SCALE 5.1 ORIGEN-ARP to predict isotope libraries for the Units 1, 2 and 3 reactors and Unit 4 spent fuel pool for comparing against measurements of environmental sampled collected at the site in order to identify the source terms of the accident. Comparison of the cesium 134/137 and cesium 136/137 ratios observed in environmental samples and ORIGEN-ARP predictions indicated that the Unit 4 Spent Fuelmore » Pool did not significantly contribute to radionuclide release during the Fukushima Daiichi accident.« less

Comparing the 2,2'-Biphenylenedithiophosphinate Binding of Americium with Neodymium and Europium

DOE PAGES

Cross, Justin N.; Macor, Joseph A.; Bertke, Jeffery A.; ...

2016-09-15

Advancing our understanding of the minor actinides (Am, Cm) versus lanthanides is key for developing advanced nuclear-fuel cycles. Here in this paper, we describe the preparation of (NBu 4)Am[S 2P( tBu 2C 12H 6)] 4 and two isomorphous lanthanide complexes, namely one with a similar ionic radius (i.e., Nd III) and an isoelectronic one (Eu III). The results include the first measurement of an Am-S bond length, with a mean value of 2.921(9) Å, by single-crystal X-ray diffraction. Comparison with the Eu III and Nd III complexes revealed subtle electronic differences between the complexes of Am III and the lanthanides.

Rapid determination of actinides in seawater samples

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.

2014-03-09

A new rapid method for the determination of actinides in seawater samples has been developed at the Savannah River National Laboratory. The actinides can be measured by alpha spectrometry or inductively-coupled plasma mass spectrometry. The new method employs novel pre-concentration steps to collect the actinide isotopes quickly from 80 L or more of seawater. Actinides are co-precipitated using an iron hydroxide co-precipitation step enhanced with Ti +3 reductant, followed by lanthanum fluoride co-precipitation. Stacked TEVA Resin and TRU Resin cartridges are used to rapidly separate Pu, U, and Np isotopes from seawater samples. TEVA Resin and DGA Resin were usedmore » to separate and measure Pu, Am and Cm isotopes in seawater volumes up to 80 L. This robust method is ideal for emergency seawater samples following a radiological incident. It can also be used, however, for the routine analysis of seawater samples for oceanographic studies to enhance efficiency and productivity. In contrast, many current methods to determine actinides in seawater can take 1–2 weeks and provide chemical yields of ~30–60 %. This new sample preparation method can be performed in 4–8 h with tracer yields of ~85–95 %. By employing a rapid, robust sample preparation method with high chemical yields, less seawater is needed to achieve lower or comparable detection limits for actinide isotopes with less time and effort.« less

Study on separation of minor actinides from HLLW with new extractant of TODGA-DHOA/Kerosene

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ye, Guo-an; Zhu, Wen-bin; Li, Feng-feng

2013-07-01

The extraction behavior of U, Np, Pu, Am, rare earth elements and Sr from nitric acid solutions by TODGA/dodecan, DHOA/dodecane and TODGA-DHOA/dodecane were investigated, respectively. Based on experimental results, a separation process was proposed for minor actinide isolation from high level liquid waste (HLLW): the TODGA-DHOA/kerosene system. The multi-stage counter-current cascade experiments were carried out for the purpose by 0.1 mol/l TODGA-1.0 mol/l DHOA/kerosene with miniature mixer- settler contactor rigs (8 stages for extraction, 6 stages for scrubbing, 8 stages for first stripping, 8 stages for second stripping). The results show that the recovery efficiencies of the actinides and lanthanidesmore » are more than 99.9%, whereas less than 1% Sr was extracted by 0.1 mol/l TODGA - 1.0 mol/l DHOA/kerosene. The stripping efficiencies of U, Np and Pu are more than 95% in the first stripping step by 0.5 mol/l HNO{sub 3} + 0.5 mol/l AHA(aceto-hydroxamic acid), all of the remained actinides and lanthanides can be stripped by 0.01 mol/l HNO{sub 3} in the second stripping step. 99% Sr was extracted by 0.1 mol/l TODGA/kerosene, so Sr can be recovered efficiently directly from the raffinate by 0.1 mol/l TODGA/kerosene. (authors)« less

Novel Separation of Actinides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mariella, R

The separation of actinides and other elements of interest for nuclear forensics and threat reduction is currently performed using decades-old chemistries and ion-exchange columns. We propose to determine the technical feasibility of a novel method for separating actinide ions in solution. This method is based upon isotachophoresis (ITP), which has been applied in the purification of pharmaceuticals and other biochemical applications. This technique has the potential to separate inorganic ions more effectively than existing methods, which is key to analyzing very small samples. We will perform a quantitative assessment of the effectiveness of specific isotachophoretic approaches including predicting the physicalmore » and chemical properties, such as ion mobility, of inorganic ions under specific solvent conditions using a combination of ab initio calculations and semi-empirical methods. We expect to obtain a thorough understanding of the analytical systems parameters under which ITP is most effective for the separation of inorganic samples, including the influence of the double layer surrounding actinide ions, the Debye length for different ions and ion complexes, and Debye-Hueckel limits. Inorganic separations are key to nuclear forensics for countering terrorism and nuclear proliferation. If found to be feasible and potentially superior to currently used separation approaches, ITP could provide the conceptual basis for an improved means to separate samples of nuclear explosion debris for nuclear forensic analysis, in support of the Laboratory's missions in homeland and national security.« less

A review on solid phase extraction of actinides and lanthanides with amide based extractants.

PubMed

Ansari, Seraj A; Mohapatra, Prasanta K

2017-05-26

Solid phase extraction is gaining attention from separation scientists due to its high chromatographic utility. Though both grafted and impregnated forms of solid phase extraction resins are popular, the later is easy to make by impregnating a given organic extractant on to an inert solid support. Solid phase extraction on an impregnated support, also known as extraction chromatography, combines the advantages of liquid-liquid extraction and the ion exchange chromatography methods. On the flip side, the impregnated extraction chromatographic resins are less stable against leaching out of the organic extractant from the pores of the support material. Grafted resins, on the other hand, have a higher stability, which allows their prolong use. The goal of this article is a brief literature review on reported actinide and lanthanide separation methods based on solid phase extractants of both the types, i.e., (i) ligand impregnation on the solid support or (ii) ligand functionalized polymers (chemically bonded resins). Though the literature survey reveals an enormous volume of studies on the extraction chromatographic separation of actinides and lanthanides using several extractants, the focus of the present article is limited to the work carried out with amide based ligands, viz. monoamides, diamides and diglycolamides. The emphasis will be on reported applied experimental results rather than on data pertaining fundamental metal complexation. Copyright © 2017 Elsevier B.V. All rights reserved.

Nuclear Methods for Transmutation of Nuclear Waste: Problems, Perspextives, Cooperative Research - Proceedings of the International Workshop

NASA Astrophysics Data System (ADS)

Khankhasayev, Zhanat B.; Kurmanov, Hans; Plendl, Mikhail Kh.

1996-12-01

The Table of Contents for the full book PDF is as follows: * Preface * I. Review of Current Status of Nuclear Transmutation Projects * Accelerator-Driven Systems — Survey of the Research Programs in the World * The Los Alamos Accelerator-Driven Transmutation of Nuclear Waste Concept * Nuclear Waste Transmutation Program in the Czech Republic * Tentative Results of the ISTC Supported Study of the ADTT Plutonium Disposition * Recent Neutron Physics Investigations for the Back End of the Nuclear Fuel Cycle * Optimisation of Accelerator Systems for Transmutation of Nuclear Waste * Proton Linac of the Moscow Meson Factory for the ADTT Experiments * II. Computer Modeling of Nuclear Waste Transmutation Methods and Systems * Transmutation of Minor Actinides in Different Nuclear Facilities * Monte Carlo Modeling of Electro-nuclear Processes with Nonlinear Effects * Simulation of Hybrid Systems with a GEANT Based Program * Computer Study of 90Sr and 137Cs Transmutation by Proton Beam * Methods and Computer Codes for Burn-Up and Fast Transients Calculations in Subcritical Systems with External Sources * New Model of Calculation of Fission Product Yields for the ADTT Problem * Monte Carlo Simulation of Accelerator-Reactor Systems * III. Data Basis for Transmutation of Actinides and Fission Products * Nuclear Data in the Accelerator Driven Transmutation Problem * Nuclear Data to Study Radiation Damage, Activation, and Transmutation of Materials Irradiated by Particles of Intermediate and High Energies * Radium Institute Investigations on the Intermediate Energy Nuclear Data on Hybrid Nuclear Technologies * Nuclear Data Requirements in Intermediate Energy Range for Improvement of Calculations of ADTT Target Processes * IV. Experimental Studies and Projects * ADTT Experiments at the Los Alamos Neutron Science Center * Neutron Multiplicity Distributions for GeV Proton Induced Spallation Reactions on Thin and Thick Targets of Pb and U * Solid State Nuclear Track Detector and Radiochemical Studies on the Transmutation of Nuclei Using Relativistic Heavy Ions * Experimental and Theoretical Study of Radionuclide Production on the Electronuclear Plant Target and Construction Materials Irradiated by 1.5 GeV and 130 MeV Protons * Neutronics and Power Deposition Parameters of the Targets Proposed in the ISTC Project 17 * Multicycle Irradiation of Plutonium in Solid Fuel Heavy-Water Blanket of ADS * Compound Neutron Valve of Accelerator-Driven System Sectioned Blanket * Subcritical Channel-Type Reactor for Weapon Plutonium Utilization * Accelerator Driven Molten-Fluoride Reactor with Modular Heat Exchangers on PB-BI Eutectic * A New Conception of High Power Ion Linac for ADTT * Pions and Accelerator-Driven Transmutation of Nuclear Waste? * V. Problems and Perspectives * Accelerator-Driven Transmutation Technologies for Resolution of Long-Term Nuclear Waste Concerns * Closing the Nuclear Fuel-Cycle and Moving Toward a Sustainable Energy Development * Workshop Summary * List of Participants

Nuclear Fuels & Materials Spotlight Volume 5

DOE Office of Scientific and Technical Information (OSTI.GOV)

Petti, David Andrew

2016-10-01

As the nation's nuclear energy laboratory, Idaho National Laboratory brings together talented people and specialized nuclear research capability to accomplish our mission. This edition of the Nuclear Fuels and Materials Division Spotlight provides an overview of some of our recent accomplishments in research and capability development. These accomplishments include: • Evaluation and modeling of light water reactor accident tolerant fuel concepts • Status and results of recent TRISO-coated particle fuel irradiations, post-irradiation examinations, high-temperature safety testing to demonstrate the accident performance of this fuel system, and advanced microscopy to improve the understanding of fission product transport in this fuel system.more » • Improvements in and applications of meso and engineering scale modeling of light water reactor fuel behavior under a range of operating conditions and postulated accidents (e.g., power ramping, loss of coolant accident, and reactivity initiated accidents) using the MARMOT and BISON codes. • Novel measurements of the properties of nuclear (actinide) materials under extreme conditions, (e.g. high pressure, low/high temperatures, high magnetic field) to improve the scientific understanding of these materials. • Modeling reactor pressure vessel behavior using the GRIZZLY code. • New methods using sound to sense temperature inside a reactor core. • Improved experimental capabilities to study the response of fusion reactor materials to a tritium plasma. Throughout Spotlight, you'll find examples of productive partnerships with academia, industry, and government agencies that deliver high-impact outcomes. The work conducted at Idaho National Laboratory helps spur innovation in nuclear energy applications that drive economic growth and energy security. We appreciate your interest in our work here at Idaho National Laboratory, and hope that you find this issue informative.« less

Actinide recovery process

DOEpatents

Muscatello, Anthony C.; Navratil, James D.; Saba, Mark T.

1987-07-28

Process for the removal of plutonium polymer and ionic actinides from aqueous solutions by absorption onto a solid extractant loaded on a solid inert support such as polystyrenedivinylbenzene. The absorbed actinides can then be recovered by incineration, by stripping with organic solvents, or by acid digestion. Preferred solid extractants are trioctylphosphine oxide and octylphenyl-N,N-diisobutylcarbamoylmethylphosphine oxide and the like.

Improved method for extracting lanthanides and actinides from acid solutions

DOEpatents

Horwitz, E.P.; Kalina, D.G.; Kaplan, L.; Mason, G.W.

1983-07-26

A process for the recovery of actinide and lanthanide values from aqueous acidic solutions uses a new series of neutral bi-functional extractants, the alkyl(phenyl)-N,N-dialkylcarbamoylmethylphosphine oxides. The process is suitable for the separation of actinide and lanthanide values from fission product values found together in high-level nuclear reprocessing waste solutions.

Prompt fission neutron spectra of actinides

DOE PAGES

Capote, R.; Chen, Y. -J.; Hambsch, F. -J.; ...

2016-01-06

Here, the energy spectrum of prompt neutrons emitted in fission (PFNS) plays a very important role in nuclear science and technology. A Coordinated Research Project (CRP) "Evaluation of Prompt Fission Neutron Spectra of Actinides" was established by the IAEA Nuclear Data Section in 2009, with the major goal to produce new PFNS evaluations with uncertainties for actinide nuclei.

Actinide recovery process

DOEpatents

Muscatello, A.C.; Navratil, J.D.; Saba, M.T.

1985-06-13

Process for the removal of plutonium polymer and ionic actinides from aqueous solutions by absorption onto a solid extractant loaded on a solid inert support such as polystyrene-divinylbenzene. The absorbed actinides can then be recovered by incineration, by stripping with organic solvents, or by acid digestion. Preferred solid extractants are trioctylphosphine oxide and octylphenyl-N,N-diisobutylcarbamoylmethylphosphine oxide and the like. 2 tabs.

Process for making a ceramic composition for immobilization of actinides

DOEpatents

Ebbinghaus, Bartley B.; Van Konynenburg, Richard A.; Vance, Eric R.; Stewart, Martin W.; Walls, Philip A.; Brummond, William Allen; Armantrout, Guy A.; Herman, Connie Cicero; Hobson, Beverly F.; Herman, David Thomas; Curtis, Paul G.; Farmer, Joseph

2001-01-01

Disclosed is a process for making a ceramic composition for the immobilization of actinides, particularly uranium and plutonium. The ceramic is a titanate material comprising pyrochlore, brannerite and rutile. The process comprises oxidizing the actinides, milling the oxides to a powder, blending them with ceramic precursors, cold pressing the blend and sintering the pressed material.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Diaconescu, Paula L.; Garcia, Evan

The objective of our research project was to study the reactivity of uranium complexes supported by ferrocene-based ligands. In addition, this research provides training of graduate students as the next generation of actinide scientists.

Chemical Technology Division annual technical report, 1992

DOE Office of Scientific and Technical Information (OSTI.GOV)

Battles, J.E.; Myles, K.M.; Laidler, J.J.

1993-06-01

In this period, CMT conducted research and development in the following areas: (1) electrochemical technology, including advanced batteries and fuel cells; (2) technology for fluidized-bed combustion and coal-fired magnetohydrodynamics; (3) methods for treatment of hazardous waste, mixed hazardous/radioactive waste, and municipal solid waste; (4) the reaction of nuclear waste glass and spent fuel under conditions expected for an unsaturated repository; (5) processes for separating and recovering transuranic elements from nuclear waste streams, treating water contaminated with volatile organics, and concentrating radioactive waste streams; (6) recovery processes for discharged fuel and the uranium blanket in the Integral Fast Reactor (EFR); (7)more » processes for removal of actinides in spent fuel from commercial water-cooled nuclear reactors and burnup in IFRs; and (8) physical chemistry of selected materials (corium; Fe-U-Zr, tritium in LiAlO{sub 2} in environments simulating those of fission and fusion energy systems. The Division also conducts basic research in catalytic chemistry associated with molecular energy resources and novel` ceramic precursors; materials chemistry of superconducting oxides, electrified metal/solution interfaces, and molecular sieve structures; and the geochemical processes involved in water-rock interactions occurring in active hydrothermal systems. In addition, the Analytical Chemistry Laboratory in CMT provides a broad range of analytical chemistry support services to the technical programs at Argonne National Laboratory (ANL).« less

Validation of the Physics Analysis used to Characterize the AGR-1 TRISO Fuel Irradiation Test

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sterbentz, James W.; Harp, Jason M.; Demkowicz, Paul A.

2015-05-01

The results of a detailed physics depletion calculation used to characterize the AGR-1 TRISO-coated particle fuel test irradiated in the Advanced Test Reactor (ATR) at the Idaho National Laboratory are compared to measured data for the purpose of validation. The particle fuel was irradiated for 13 ATR power cycles over three calendar years. The physics analysis predicts compact burnups ranging from 11.30-19.56% FIMA and cumulative neutron fast fluence from 2.21?4.39E+25 n/m 2 under simulated high-temperature gas-cooled reactor conditions in the ATR. The physics depletion calculation can provide a full characterization of all 72 irradiated TRISO-coated particle compacts during and post-irradiation,more » so validation of this physics calculation was a top priority. The validation of the physics analysis was done through comparisons with available measured experimental data which included: 1) high-resolution gamma scans for compact activity and burnup, 2) mass spectrometry for compact burnup, 3) flux wires for cumulative fast fluence, and 4) mass spectrometry for individual actinide and fission product concentrations. The measured data are generally in very good agreement with the calculated results, and therefore provide an adequate validation of the physics analysis and the results used to characterize the irradiated AGR-1 TRISO fuel.« less

Assessment of the Neutronic and Fuel Cycle Performance of the Transatomic Power Molten Salt Reactor Design

DOE Office of Scientific and Technical Information (OSTI.GOV)

Robertson, Sean; Dewan, Leslie; Massie, Mark

This report presents results from a collaboration between Transatomic Power Corporation (TAP) and Oak Ridge National Laboratory (ORNL) to provide neutronic and fuel cycle analysis of the TAP core design through the Department of Energy Gateway for Accelerated Innovation in Nuclear (GAIN) Nuclear Energy Voucher program. The TAP concept is a molten salt reactor using configurable zirconium hydride moderator rod assemblies to shift the neutron spectrum in the core from mostly epithermal at beginning of life to thermal at end of life. Additional developments in the ChemTriton modeling and simulation tool provide the critical moderator-to-fuel ratio searches and time-dependent parametersmore » necessary to simulate the continuously changing physics in this complex system. The implementation of continuous-energy Monte Carlo transport and depletion tools in ChemTriton provide for full-core three-dimensional modeling and simulation. Results from simulations with these tools show agreement with TAP-calculated performance metrics for core lifetime, discharge burnup, and salt volume fraction, verifying the viability of reducing actinide waste production with this concept. Additional analyses of mass feed rates and enrichments, isotopic removals, tritium generation, core power distribution, core vessel helium generation, moderator rod heat deposition, and reactivity coeffcients provide additional information to make informed design decisions. This work demonstrates capabilities of ORNL modeling and simulation tools for neutronic and fuel cycle analysis of molten salt reactor concepts.« less

The separation of lanthanides and actinides in supercritical fluid carbon dioxide

DOE PAGES

Mincher, Bruce J.; Wai, Chien M.; Fox, Robert V.; ...

2015-10-28

Supercritical fluid carbon dioxide presents an attractive alternative to conventional solvents for recovery of the actinides and lanthanides. Carbon dioxide is a good solvent for fluorine and phosphate-containing ligands, including the traditional tributylphosphate ligand used in process-scale uranium separations. Actinide and lanthanide oxides may even be directly dissolved in carbon dioxide containing the complexes formed between these ligands and mineral acids, obviating the need for large volumes of acids for leaching and dissolution, and the corresponding organic liquid–liquid solvent extraction solutions. As a result, examples of the application of this novel technology for actinide and lanthanide separations are presented.

Viscosity Meaurement Technique for Metal Fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ban, Heng; Kennedy, Rory

2015-02-09

Metallic fuels have exceptional transient behavior, excellent thermal conductivity, and a more straightforward reprocessing path, which does not separate out pure plutonium from the process stream. Fabrication of fuel containing minor actinides and rare earth (RE) elements for irradiation tests, for instance, U-20Pu-3Am-2Np-1.0RE-15Zr samples at the Idaho National Laboratory, is generally done by melt casting in an inert atmosphere. For the design of a casting system and further scale up development, computational modeling of the casting process is needed to provide information on melt flow and solidification for process optimization. Therefore, there is a need for melt viscosity data, themore » most important melt property that controls the melt flow. The goal of the project was to develop a measurement technique that uses fully sealed melt sample with no Americium vapor loss to determine the viscosity of metallic melts and at temperatures relevant to the casting process. The specific objectives of the project were to: develop mathematical models to establish the principle of the measurement method, design and build a viscosity measurement prototype system based on the established principle, and calibrate the system and quantify the uncertainty range. The result of the project indicates that the oscillation cup technique is applicable for melt viscosity measurement. Detailed mathematical models of innovative sample ampoule designs were developed to not only determine melt viscosity, but also melt density under certain designs. Measurement uncertainties were analyzed and quantified. The result of this project can be used as the initial step toward the eventual goal of establishing a viscosity measurement system for radioactive melts.« less

Enhancing the actinide sciences in Europe through hot laboratories networking and pooling: from ACTINET to TALISMAN

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bourg, S.; Poinssot, C.

2013-07-01

Since 2004, Europe supports the strengthening of the European actinides sciences scientific community through the funding of dedicated networks: (i) from 2004 to 2008, the ACTINET6 network of excellence (6. Framework Programme) gathered major laboratories involved in nuclear research and a wide range of academic research organisations and universities with the specific aims of funding and implementing joint research projects to be performed within the network of pooled facilities; (ii) from 2009 to 2013, the ACTINET-I3 integrated infrastructure initiative (I3) supports the cost of access of any academics in the pooled EU hot laboratories. In this continuation, TALISMAN (Trans-national Accessmore » to Large Infrastructures for a Safe Management of Actinides) gathers now the main European hot laboratories in actinides sciences in order to promote their opening to academics and universities and strengthen the EU-skills in actinides sciences. Furthermore, a specific focus is set on the development of advanced cutting-edge experimental and spectroscopic capabilities, the combination of state-of-the art experimental with theoretical first-principle methods on a quantum mechanical level and to benefit from the synergy between the different scientific and technical communities. ACTINET-I3 and TALISMAN attach a great importance and promote the Education and Training of the young generation of actinides scientists in the Trans-national access but also by organizing Schools (general Summer Schools or Theoretical User Lab Schools) or by granting students to attend International Conference on actinide sciences. (authors)« less

The efficacy of denaturing actinide elements as a means of decreasing materials attractiveness

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hase, K.R.; Bathke, C.G.; Ebbinghaus, B.B.

2013-07-01

This study considers the concept of denaturing as applied to the actinide elements present in spent fuel as a means to reduce materials attractiveness. Highly attractive materials generally have low values of bare critical mass, heat content, and dose. To denature an attractive element, its spent-fuel isotopic composition (isotopic vector) is intentionally modified by introducing sufficient quantities of a significantly less attractive isotope to dilute the concentration of a highly attractive isotope so that the overall attractiveness of the element is reduced. The authors used FOM (Figure of Merit) formula as the material attractiveness metric for their parametric determination ofmore » the attractiveness of the Pu and U. Materials attractiveness needs to be considered in three distinct phases in the process to construct a nuclear explosive device (NED): the acquisition phase, processing phase, and utilization phase. The results show that denaturing uranium with {sup 238}U is actually an effective means of reducing the attractiveness. For uranium with a large minority of {sup 235}U, a mixture of 80% {sup 238}U to 20% {sup 235}U is required to reduce the attractiveness to low. For uranium with a large concentration of {sup 233}U, a mixture of 88% {sup 238}U to 12% {sup 233}U is required to reduce the attractiveness to low. The results also show that denaturing plutonium with {sup 238}Pu is less effective than denaturing uranium with {sup 238}U. Using {sup 238}Pu as the denaturing agent would require 80% or more by mass in order to reduce the attractiveness to low. No amount of {sup 240}Pu is enough to reduce the plutonium attractiveness below medium. The combination of {sup 238}Pu and {sup 240}Pu would require approximately 70% {sup 238}Pu and 25% {sup 240}Pu by mass to reduce the plutonium attractiveness to low.« less

PREPARATION OF ACTINIDE-ALUMINUM ALLOYS

DOEpatents

Moore, R.H.

1962-09-01

BS>A process is given for preparing alloys of aluminum with plutonium, uranium, and/or thorium by chlorinating actinide oxide dissolved in molten alkali metal chloride with hydrochloric acid, chlorine, and/or phosgene, adding aluminum metal, and passing air and/or water vapor through the mass. Actinide metal is formed and alloyed with the aluminum. After cooling to solidification, the alloy is separated from the salt. (AEC)

PRODUCTION OF ACTINIDE METAL

DOEpatents

Knighton, J.B.

1963-11-01

A process of reducing actinide oxide to the metal with magnesium-zinc alloy in a flux of 5 mole% of magnesium fluoride and 95 mole% of magnesium chloride plus lithium, sodium, potassium, calcium, strontium, or barium chloride is presented. The flux contains at least 14 mole% of magnesium cation at 600-- 900 deg C in air. The formed magnesium-zinc-actinide alloy is separated from the magnesium-oxide-containing flux. (AEC)

Trace concentration - Huge impact: Nitrate in the calcite/Eu(III) system

NASA Astrophysics Data System (ADS)

Hofmann, Sascha; Voïtchovsky, Kislon; Schmidt, Moritz; Stumpf, Thorsten

2014-01-01

The interactions of trivalent lanthanides and actinides with secondary mineral phases such as calcite is of high importance for the safety assessment of deep geological repositories for high level nuclear waste (HLW). Due to similar ionic radii, calcium-bearing mineral phases are suitable host minerals for Ln(III) and An(III) ions. Especially calcite has been proven to retain these metal ions effectively by both surface complexation and bulk incorporation. Since anionic ligands (e.g., nitrate) are omnipresent in the geological environment and due to their coordinating properties, their influence on retentive processes should not be underestimated. Nitrate is a common contaminant in most HLW forms as a result of using nitric acid in fuel reprocessing. It is also formed by microbial activity under aerobic conditions. In this study, atomic force microscopy investigations revealed a major influence of nitrate upon the surface of calcite crystals. NaNO3 causes serious modifications even in trace amounts (<10-7 M) and forms a soft surface layer of low crystallinity on top of the calcite crystal. Time-resolved laser fluorescence spectroscopy of Eu(III) showed that, within this layer, Eu(III) ions are incorporated, while losing most of their hydration shell. The results show that solid solution modelling for actinides in calcite must take into account the presence of nitrate in pore and ground waters.

Application of annular centrifugal contactors in the hot test of the improved total partitioning process for high level liquid waste.

PubMed

Duan, Wuhua; Chen, Jing; Wang, Jianchen; Wang, Shuwei; Feng, Xiaogui; Wang, Xinghai; Li, Shaowei; Xu, Chao

2014-08-15

High level liquid waste (HLLW) produced from the reprocessing of the spent nuclear fuel still contains moderate amounts of uranium, transuranium (TRU) actinides, (90)Sr, (137)Cs, etc., and thus constitutes a permanent hazard to the environment. The partitioning and transmutation (P&T) strategy has increasingly attracted interest for the safe treatment and disposal of HLLW, in which the partitioning of HLLW is one of the critical technical issues. An improved total partitioning process, including a TRPO (tri-alkylphosphine oxide) process for the removal of actinides, a CESE (crown ether strontium extraction) process for the removal of Sr, and a CECE (calixcrown ether cesium extraction) process for the removal of Cs, has been developed to treat Chinese HLLW. A 160-hour hot test of the improved total partitioning process was carried out using 72-stage 10-mm-dia annular centrifugal contactors (ACCs) and genuine HLLW. The hot test results showed that the average DFs of total α activity, Sr and Cs were 3.57 × 10(3), 2.25 × 10(4) and 1.68 × 10(4) after the hot test reached equilibrium, respectively. During the hot test, 72-stage 10-mm-dia ACCs worked stable, continuously with no stage failing or interruption of the operation. Copyright © 2014 Elsevier B.V. All rights reserved.

The shortest Th-Th distance from a new type of quadruple bond.

PubMed

Hu, Han-Shi; Kaltsoyannis, Nikolas

2017-02-15

Compounds featuring unsupported metal-metal bonds between actinide elements remain highly sought after yet confined experimentally to inert gas matrix studies. Notwithstanding this paucity, actinide-actinide bonding has been the subject of extensive computational research. In this contribution, high level quantum chemical calculations at both the scalar and spin-orbit levels are used to probe the Th-Th bonding in a range of zero valent systems of general formula LThThL. Several of these compounds have very short Th-Th bonds arising from a new type of Th-Th quadruple bond with a previously unreported electronic configuration featuring two unpaired electrons in 6d-based δ bonding orbitals. H 3 AsThThAsH 3 is found to have the shortest Th-Th bond yet reported (2.590 Å). The Th 2 unit is a highly sensitive probe of ligand electron donor/acceptor ability; we can tune the Th-Th bond from quadruple to triple, double and single by judicious choice of the L group, up to 2.888 Å for singly-bonded ONThThNO.

2017 Report for New LANL Physical Vapor Deposition Capability

DOE Office of Scientific and Technical Information (OSTI.GOV)

Roman, Audrey Rae; Zhao, Xinxin; Bond, Evelyn M.

There is an urgent need at LANL to achieve uniform, thin film actinide targets that are essential for nuclear physics experiments. The target preparation work is currently performed externally by Professor Walter Loveland at Oregon State University, who has made various evaporated actinide targets such as Th and U for use on several nuclear physics measurements at LANSCE. We are developing a vapor deposition capability, with the goal of evaporating Th and U in the Actinide Research Facility (ARF) at TA-48. In the future we plan to expand this work to evaporating transuranic elements, such as Pu. The ARF ismore » the optimal location for evaporating actinides because this lab is specifically dedicated to actinide research. There are numerous instruments in the ARF that can be used to provide detailed characterization of the evaporated thin films such as: Table top Scanning Electron Microscope, In-situ X-Ray Diffraction, and 3D Raman spectroscopy. These techniques have the ability to determine the uniformity, surface characterization, and composition of the deposits.« less

Formation of unprecedented actinidecarbon triple bonds in uranium methylidyne molecules

PubMed Central

Lyon, Jonathan T.; Hu, Han-Shi; Andrews, Lester; Li, Jun

2007-01-01

Chemistry of the actinide elements represents a challenging yet vital scientific frontier. Development of actinide chemistry requires fundamental understanding of the relative roles of actinide valence-region orbitals and the nature of their chemical bonding. We report here an experimental and theoretical investigation of the uranium methylidyne molecules X3UCH (X = F, Cl, Br), F2ClUCH, and F3UCF formed through reactions of laser-ablated uranium atoms and trihalomethanes or carbon tetrafluoride in excess argon. By using matrix infrared spectroscopy and relativistic quantum chemistry calculations, we have shown that these actinide complexes possess relatively strong UC triple bonds between the U 6d-5f hybrid orbitals and carbon 2s-2p orbitals. Electron-withdrawing ligands are critical in stabilizing the U(VI) oxidation state and sustaining the formation of uranium multiple bonds. These unique UC-bearing molecules are examples of the long-sought actinide-alkylidynes. This discovery opens the door to the rational synthesis of triple-bonded actinidecarbon compounds. PMID:18024591

A Screened Hybrid DFT Study of Actinide Oxides, Nitrides, and Carbides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wen, Xiaodong; Martin, Richard L.; Scuseria, Gustavo E.

2013-06-27

A systematic study of the structural, electronic, and magnetic properties of actinide oxides, nitrides, and carbides (AnX1–2 with X = C, N, O) is performed using the Heyd–Scuseria–Ernzerhof (HSE) hybrid functional. Our computed results show that the screened hybrid HSE functional gives a good description of the electronic and structural properties of actinide dioxides (strongly correlated insulators) when compared with available experimental data. However, there are still some problems reproducing the electronic properties of actinide nitrides and carbides (strongly correlated metals). In addition, in order to compare with the results by HSE, the structures, electronic, and magnetic properties of thesemore » actinide compounds are also investigated in the PBE and PBE+U approximation. Interestingly, the density of states of UN obtained with PBE compares well with the experimental photoemission spectra, in contrast to the hybrid approximation. This is presumably related to the need of additional screening in the Hartree–Fock exchange term of the metallic phases.« less

Ceramicrete stabilization of U-and Pu-bearing materials

DOEpatents

Wagh, Arun S.; Maloney, M. David; Thompson, Gary H.

2007-11-13

A method of stabilizing nuclear material is disclosed. Oxides or halides of actinides and/or transuranics (TRUs) and/or hydrocarbons and/or acids contaminated with actinides and/or TRUs are treated by adjusting the pH of the nuclear material to not less than about 5 and adding sufficient MgO to convert fluorides present to MgF.sub.2; alumina is added in an amount sufficient to absorb substantially all hydrocarbon liquid present, after which a binder including MgO and KH.sub.2PO.sub.4 is added to the treated nuclear material to form a slurry. Additional MgO may be added. A crystalline radioactive material is also disclosed having a binder of the reaction product of calcined MgO and KH.sub.2PO.sub.4 and a radioactive material of the oxides and/or halides of actinides and/or transuranics (TRUs). Acids contaminated with actinides and/or TRUs, and/or actinides and/or TRUs with or without oils and/or greases may be encapsulated and stabilized by the binder.

Matrix infrared spectra and electronic structure calculations of the first actinide borylene: FB=ThF(2).

PubMed

Wang, Xuefeng; Roos, Björn O; Andrews, Lester

2010-03-14

Laser-ablated Th atoms react with BF(3) during condensation in excess argon at 6 K to form the first actinide borylene (FB=ThF(2)) and actinide-boron multiple bond. Three new product absorptions in the B-F and Th-F stretching regions of matrix infrared spectra are assigned to FB=ThF(2) from comparison to theoretically predicted vibrational frequencies.

CHARACTERIZATION OF ACTINIDES IN SIMULATED ALKALINE TANK WASTE SLUDGES AND LEACHATES

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nash, Kenneth L.

In this project, both the fundamental chemistry of actinides in alkaline solutions (relevant to those present in Hanford-style waste storage tanks), and their dissolution from sludge simulants (and interactions with supernatants) have been investigated under representative sludge leaching procedures. The leaching protocols were designed to go beyond conventional alkaline sludge leaching limits, including the application of acidic leachants, oxidants and complexing agents. The simulant leaching studies confirm in most cases the basic premise that actinides will remain in the sludge during leaching with 2-3 M NaOH caustic leach solutions. However, they also confirm significant chances for increased mobility of actinidesmore » under oxidative leaching conditions. Thermodynamic data generated improves the general level of experiemental information available to predict actinide speciation in leach solutions. Additional information indicates that improved Al removal can be achieved with even dilute acid leaching and that acidic Al(NO3)3 solutions can be decontaminated of co-mobilized actinides using conventional separations methods. Both complexing agents and acidic leaching solutions have significant potential to improve the effectiveness of conventional alkaline leaching protocols. The prime objective of this program was to provide adequate insight into actinide behavior under these conditions to enable prudent decision making as tank waste treatment protocols develop.« less

Reducing Actinide Production Using Inert Matrix Fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Deinert, Mark

2017-08-23

The environmental and geopolitical problems that surround nuclear power stem largely from the longlived transuranic isotopes of Am, Cm, Np and Pu that are contained in spent nuclear fuel. New methods for transmuting these elements into more benign forms are needed. Current research efforts focus largely on the development of fast burner reactors, because it has been shown that they could dramatically reduce the accumulation of transuranics. However, despite five decades of effort, fast reactors have yet to achieve industrial viability. A critical limitation to this, and other such strategies, is that they require a type of spent fuel reprocessingmore » that can efficiently separate all of the transuranics from the fission products with which they are mixed. Unfortunately, the technology for doing this on an industrial scale is still in development. In this project, we explore a strategy for transmutation that can be deployed using existing, current generation reactors and reprocessing systems. We show that use of an inert matrix fuel to recycle transuranics in a conventional pressurized water reactor could reduce overall production of these materials by an amount that is similar to what is achievable using proposed fast reactor cycles. Furthermore, we show that these transuranic reductions can be achieved even if the fission products are carried into the inert matrix fuel along with the transuranics, bypassing the critical separations hurdle described above. The implications of these findings are significant, because they imply that inert matrix fuel could be made directly from the material streams produced by the commercially available PUREX process. Zirconium dioxide would be an ideal choice of inert matrix in this context because it is known to form a stable solid solution with both fission products and transuranics.« less

Survey of glass plutonium contents and poison selection

DOE Office of Scientific and Technical Information (OSTI.GOV)

Plodinec, M.J.; Ramsey, W.G.; Ellison, A.J.G.

1996-05-01

If plutonium and other actinides are to be immobilized in glass, then achieving high concentrations in the glass is desirable. This will lead to reduced costs and more rapid immobilization. However, glasses with high actinide concentrations also bring with them undersirable characteristics, especially a greater concern about nuclear criticality, particularly in a geologic repository. The key to achieving a high concentration of actinide elements in a glass is to formulate the glass so that the solubility of actinides is high. At the same time, the glass must be formulated so that the glass also contains neutron poisons, which will preventmore » criticality during processing and in a geologic repository. In this paper, the solubility of actinides, particularly plutonium, in three types of glasses are discussed. Plutonium solubilities are in the 2-4 wt% range for borosilicate high-level waste (HLW) glasses of the type which will be produced in the US. This type of glass is generally melted at relatively low temperatures, ca. 1150{degrees}C. For this melting temperature, the glass can be reformulated to achieve plutonium solubilities of at least 7 wt%. This low melting temperature is desirable if one must retain volatile cesium-137 in the glass. If one is not concerned about cesium volatility, then glasses can be formulated which can contain much larger amounts of plutonium and other actinides. Plutonium concentrations of at least 15 wt% have been achieved. Thus, there is confidence that high ({ge}5 wt%) concentrations of actinides can be achieved under a variety of conditions.« less

Actinide Sorption in a Brine/Dolomite Rock System: Evaluating the Degree of Conservatism in Kd Ranges used in Performance Assessment Modeling for the WIPP Nuclear Waste Repository

NASA Astrophysics Data System (ADS)

Dittrich, T. M.; Reed, D. T.

2015-12-01

The Waste Isolation Pilot Plant (WIPP) near Carlsbad, NM is the only operating nuclear waste repository in the US and has been accepting transuranic (TRU) waste since 1999. The WIPP is located in a salt deposit approximately 650 m below the surface and performance assessment (PA) modeling for a 10,000 year period is required to recertify the operating license with the US EPA every five years. The main pathway of concern for environmental release of radioactivity is a human intrusion caused by drilling into a pressurized brine reservoir below the repository. This could result in the flooding of the repository and subsequent transport in the high transmissivity layer (dolomite-rich Culebra formation) above the waste disposal rooms. We evaluate the degree of conservatism in the estimated sorption partition coefficients (Kds) ranges used in the PA based on an approach developed with granite rock and actinides (Dittrich and Reimus, 2015; Dittrich et al., 2015). Sorption onto the waste storage material (Fe drums) may also play a role in mobile actinide concentrations. We will present (1) a conceptual overview of how Kds are used in the PA model, (2) technical background of the evolution of the ranges and (3) results from batch and column experiments and model predictions for Kds with WIPP dolomite and clays, brine with various actinides, and ligands (e.g., acetate, citrate, EDTA) that could promote transport. The current Kd ranges used in performance models are based on oxidation state and are 5-400, 0.5-10,000, 0.03-200, and 0.03-20 mL g-1 for elements with oxidation states of III, IV, V, and VI, respectively. Based on redox conditions predicted in the brines, possible actinide species include Pu(III), Pu(IV), U(IV), U(VI), Np(IV), Np(V), Am(III), and Th(IV). We will also discuss the challenges of upscaling from lab experiments to field scale predictions, the role of colloids, and the effect of engineered barrier materials (e.g., MgO) on transport conditions. Dittrich, T.M., Reimus, P.W. 2015. Uranium transport in a crushed granodiorite: experiments and reactive transport modeling. J Contam Hydrol 175-176: 44-59. Dittrich, T.M., Boukhalfa, H., Ware, S.D., Reimus, P.W. 2015. Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids. J Environ Radioactiv 148: 170-182.

Chemistry of transuranium elements in salt-base repository

DOE Office of Scientific and Technical Information (OSTI.GOV)

Borkowski, Marian; Reed, Donald T; Lucchini, Jean - Francois

2010-12-02

The mobility and potential release of actinides into the accessible environment continues to be the key performance assessment concern of nuclear repositories. Actinide, in particular plutonium speciation under the wide range of conditions that can exist in the subsurface is complex and depends strongly on the coupled effects of redox conditions, inorganic/organic complexation, and the extent/nature of aggregation. Understanding the key factors that define the potential for actinide migration is, in this context, an essential and critical part of making and sustaining a licensing case for a nuclear repository. Herein we report on recent progress in a concurrent modeling andmore » experimental study to determine the speciation of plutonium, uranium and americium in high ionic strength Na-CI-Mg brines. This is being done as part of the ongomg recertification effort m the Waste Isolation Pilot Plant (WIPP). The oxidation-state specific solubility of actinides were established in brine as function of pC{sub H+}, brine composition and the presence and absence of organic chelating agents and carbonate. An oxidation-state invariant analog approach using Nd{sup 3+} and Th{sup 4+} was used for An{sup 3+} and An{sup 4+} respectively. These results show that organic ligands and hydrolysis are key factors for An(III) solubility, hydrolysis at pC{sub H+} above 8 is predominate for An(IV) and carbonates are the key factor for U(VI) solubility. The effect of high ionic strength and brine components measured in absence of carbonates leads to measurable increased in overall solubility over analogous low ionic strength groundwater. Less is known about the bioreduction of actinides by halo-tolerant microorganisms, but there is now evidence that bioreduction does occur and is analogous, in many ways, to what occurs with soil bacteria. Results of solubility studies that focus on Pitzer parameter corrections, new species (e.g. borate complexation), and the thermodynamic parameters for modeling are discussed.« less

The MSFR as a flexible CR reactor: the viewpoint of safety

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fiorina, C.; Cammi, A.; Franceschini, F.

2013-07-01

In this paper, the possibility has first been discussed of using the liquid-fuelled Molten Salt Fast Reactor (MSFR) as a flexible conversion ratio (CR) reactor without design modification. By tuning the reprocessing rate it is possible to determine the content of fission products in the core, which in turn can significantly affect the neutron economy without incurring in solubility problems. The MSFR can thus be operated as U-233 breeder (CR>1), iso-breeder (CR=1) and burner reactor (CR<1). In particular a 40 year doubling time can be achieved, as well as a considerable Transuranics and MA (minor actinide) burning rate equal tomore » about 150 kg{sub HN}/GWE-yr. The safety parameters of the MSFR have then been evaluated for different fuel cycle strategies. Th use and a softer spectrum combine to give a strong Doppler coefficient, one order of magnitude higher compared to traditional fast reactors (FRs). The fuel expansion coefficient is comparable to the Doppler coefficient and is only mildly affected by core compositions, thus assisting the fuel cycle flexibility of the MSFR. βeff and generation time are comparable to the case of traditional FRs, if a static fuel is assumed. A notable reduction of βeff is caused by salt circulation, but a low value of this parameter is a limited concern in the MSFR thanks to the lack of a burnup reactivity swing and of positive feedbacks. A simple approach has also been developed to evaluate the MSFR capabilities to withstand all typical double-fault accidents, for different fuel cycle options.« less

Two-Dimensional Neutronic and Fuel Cycle Analysis of the Transatomic Power Molten Salt Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Betzler, Benjamin R.; Powers, Jeffrey J.; Worrall, Andrew

2017-01-15

This status report presents the results from the first phase of the collaboration between Transatomic Power Corporation (TAP) and Oak Ridge National Laboratory (ORNL) to provide neutronic and fuel cycle analysis of the TAP core design through the Department of Energy Gateway for Accelerated Innovation in Nuclear, Nuclear Energy Voucher program. The TAP design is a molten salt reactor using movable moderator rods to shift the neutron spectrum in the core from mostly epithermal at beginning of life to thermal at end of life. Additional developments in the ChemTriton modeling and simulation tool provide the critical moderator-to-fuel ratio searches andmore » time-dependent parameters necessary to simulate the continuously changing physics in this complex system. Results from simulations with these tools show agreement with TAP-calculated performance metrics for core lifetime, discharge burnup, and salt volume fraction, verifying the viability of reducing actinide waste production with this design. Additional analyses of time step sizes, mass feed rates and enrichments, and isotopic removals provide additional information to make informed design decisions. This work further demonstrates capabilities of ORNL modeling and simulation tools for analysis of molten salt reactor designs and strongly positions this effort for the upcoming three-dimensional core analysis.« less

Clean-in-Place and Reliability Testing of a Commercial 12.5-cm Annular Centrifugal Contactor at the INL

DOE Office of Scientific and Technical Information (OSTI.GOV)

N. R. Mann; T. G. Garn; D. H. Meikrantz

2007-09-01

The renewed interest in advancing nuclear energy has spawned the research of advanced technologies for recycling nuclear fuel. A significant portion of the advanced fuel cycle includes the recovery of selected actinides by solvent extraction methods utilizing centrifugal contactors. Although the use of centrifugal contactors for solvent extraction is widely known, their operation is not without challenges. Solutions generated from spent fuel dissolution contain unknown quantities of undissolved solids. A majority of these solids will be removed via various methods of filtration. However, smaller particles are expected to carry through to downstream solvent extraction processes and equipment. In addition, solids/precipitatesmore » brought about by mechanical or chemical upsets are another potential area of concern. During processing, particulate captured in the rotor assembly by high centrifugal forces eventually forms a cake-like structure on the inner wall introducing balance problems and negatively affecting phase separations. One of the features recently developed for larger engineering scale Annular Centrifugal Contactors (ACCs) is the Clean-In-Place (CIP) capability. Engineered spray nozzles were installed into the hollow central rotor shaft in all four quadrants of the rotor assembly. This arrangement allows for a very convenient and effective method of solids removal from within the rotor assembly.« less

Clean-in-Place and Reliability Testing of a Commercial 12.5 cm Annular Centrifugal Contactor at the INL

DOE Office of Scientific and Technical Information (OSTI.GOV)

N. R. Mann; T. G. Garn; D. H. Meikrantz

2007-09-01

The renewed interest in advancing nuclear energy has spawned the research of advanced technologies for recycling nuclear fuel. A significant portion of the advanced fuel cycle includes the recovery of selected actinides by solvent extraction methods utilizing centrifugal contactors. Although the use of centrifugal contactors for solvent extraction is widely known, their operation is not without challenges. Solutions generated from spent fuel dissolution contain unknown quantities of undissolved solids. A majority of these solids will be removed via various methods of filtration. However, smaller particles are expected to carry through to downstream solvent extraction processes and equipment. In addition, solids/precipitatesmore » brought about by mechanical or chemical upsets are another potential area of concern. During processing, particulate captured in the rotor assembly by high centrifugal forces eventually forms a cake-like structure on the inner wall introducing balance problems and negatively affecting phase separations. One of the features recently developed for larger engineering scale Annular Centrifugal Contactors (ACCs) is the Clean-In-Place (CIP) capability. Engineered spray nozzles were installed into the hollow central rotor shaft in all four quadrants of the rotor assembly. This arrangement allows for a very convenient and effective method of solids removal from within the rotor assembly.« less

Lanl Neutron-Induced Fission Cross Section Measurement Program

NASA Astrophysics Data System (ADS)

Laptev, A. B.; Tovesson, F.; Hill, T. S.

2014-09-01

A well established program of neutron-induced fission cross section measurement at Los Alamos Neutron Science Center (LANSCE) is supporting the Fuel Cycle Research program (FC R&D). Combining measurements at two LANSCE facilities, the Lujan Center and the Weapons Neutron Research facility (WNR), cover neutron energies over 10 orders of magnitude: from sub-thermal up to 200 MeV. A parallel-plate fission ionization chamber was used as a fission fragment detector. The 235U(n,f) standard was used as the reference. Fission cross sections have been measured for multiple actinides. The new data presented here completes the suite of long-lived Uranium isotopes that were investigated with this experimental approach. The cross section data are presented in comparison with existing evaluations and previous measurements.

Comparing the new generation accelerator driven subcritical reactor system (ADS) to traditional critical reactors

NASA Astrophysics Data System (ADS)

Kemah, Elif; Akkaya, Recep; Tokgöz, Seyit Rıza

2017-02-01

In recent years, the accelerator driven subcritical reactors have taken great interest worldwide. The Accelerator Driven System (ADS) has been used to produce neutron in subcritical state by the external proton beam source. These reactors, which are hybrid systems, are important in production of clean and safe energy and conversion of radioactive waste. The ADS with the selection of reliability and robust target materials have been the new generation of fission reactors. In addition, in the ADS Reactors the problems of long-lived radioactive fission products and waste actinides encountered in the fission process of the reactor during incineration can be solved, and ADS has come to the forefront of thorium as fuel for the reactors.

Composite nuclear fuel fabrication methodology for gas fast reactors

NASA Astrophysics Data System (ADS)

Vasudevamurthy, Gokul

An advanced fuel form for use in Gas Fast Reactors (GFR) was investigated. Criteria for the fuel includes operation at high temperature (˜1400°C) and high burnup (˜150 MWD/MTHM) with effective retention of fission products even during transient temperatures exceeding 1600°C. The GFR fuel is expected to contain up to 20% transuranics for a closed fuel cycle. Earlier evaluations of reference fuels for the GFR have included ceramic-ceramic (cercer) dispersion type composite fuels of mixed carbide or nitride microspheres coated with SiC in a SiC matrix. Studies have indicated that ZrC is a potential replacement for SiC on account of its higher melting point, increased fission product corrosion resistance and better chemical stability. The present work investigated natural uranium carbide microspheres in a ZrC matrix instead of SiC. Known issues of minor actinide volatility during traditional fabrication procedures necessitated the investigation of still high temperature but more rapid fabrication techniques to minimize these anticipated losses. In this regard, fabrication of ZrC matrix by combustion synthesis from zirconium and graphite powders was studied. Criteria were established to obtain sufficient matrix density with UC microsphere volume fractions up to 30%. Tests involving production of microspheres by spark erosion method (similar to electrodischarge machining) showed the inability of the method to produce UC microspheres in the desired range of 300 to 1200 mum. A rotating electrode device was developed using a minimum current of 80A and rotating at speeds up to 1500 rpm to fabricate microspheres between 355 and 1200 mum. Using the ZrC process knowledge, UC electrodes were fabricated and studied for use in the rotating electrode device to produce UC microspheres. Fabrication of the cercer composite form was studied using microsphere volume fractions of 10%, 20%, and 30%. The macrostructure of the composite and individual components at various stages were characterized to understand the required fabrication techniques and at the same time meet the necessary GFR fuel characteristics.

Sustained Recycle in Light Water and Sodium-Cooled Reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Steven J. Piet; Samuel E. Bays; Michael A. Pope

2010-11-01

From a physics standpoint, it is feasible to sustain recycle of used fuel in either thermal or fast reactors. This paper examines multi-recycle potential performance by considering three recycling approaches and calculating several fuel cycle parameters, including heat, gamma, and neutron emission of fresh fuel; radiotoxicity of waste; and uranium utilization. The first recycle approach is homogeneous mixed oxide (MOX) fuel assemblies in a light water reactor (LWR). The transuranic portion of the MOX was varied among Pu, NpPu, NpPuAm, or all-TRU. (All-TRU means all isotopes through Cf-252.) The Pu case was allowed to go to 10% Pu in freshmore » fuel, but when the minor actinides were included, the transuranic enrichment was kept below 8% to satisfy the expected void reactivity constraint. The uranium portion of the MOX was enriched uranium. That enrichment was increased (to as much as 6.5%) to keep the fuel critical for a typical LWR irradiation. The second approach uses heterogeneous inert matrix fuel (IMF) assemblies in an LWR - a mix of IMF and traditional UOX pins. The uranium-free IMF fuel pins were Pu, NpPu, NpPuAm, or all-TRU. The UOX pins were limited to 4.95% U-235 enrichment. The number of IMF pins was set so that the amount of TRU in discharged fuel from recycle N (from both IMF and UOX pins) was made into the new IMF pins for recycle N+1. Up to 60 of the 264 pins in a fuel assembly were IMF. The assembly-average TRU content was 1-6%. The third approach uses fast reactor oxide fuel in a sodium-cooled fast reactor with transuranic conversion ratio of 0.50 and 1.00. The transuranic conversion ratio is the production of transuranics divided by destruction of transuranics. The FR at CR=0.50 is similar to the CR for the MOX case. The fast reactor cases had a transuranic content of 33-38%, higher than IMF or MOX.« less

MYRRHA: A multipurpose nuclear research facility

NASA Astrophysics Data System (ADS)

Baeten, P.; Schyns, M.; Fernandez, Rafaël; De Bruyn, Didier; Van den Eynde, Gert

2014-12-01

MYRRHA (Multi-purpose hYbrid Research Reactor for High-tech Applications) is a multipurpose research facility currently being developed at SCK•CEN. MYRRHA is based on the ADS (Accelerator Driven System) concept where a proton accelerator, a spallation target and a subcritical reactor are coupled. MYRRHA will demonstrate the ADS full concept by coupling these three components at a reasonable power level to allow operation feedback. As a flexible irradiation facility, the MYRRHA research facility will be able to work in both critical as subcritical modes. In this way, MYRRHA will allow fuel developments for innovative reactor systems, material developments for GEN IV and fusion reactors, and radioisotope production for medical and industrial applications. MYRRHA will be cooled by lead-bismuth eutectic and will play an important role in the development of the Pb-alloys technology needed for the LFR (Lead Fast Reactor) GEN IV concept. MYRRHA will also contribute to the study of partitioning and transmutation of high-level waste. Transmutation of minor actinides (MA) can be completed in an efficient way in fast neutron spectrum facilities, so both critical reactors and subcritical ADS are potential candidates as dedicated transmutation systems. However critical reactors heavily loaded with fuel containing large amounts of MA pose reactivity control problems, and thus safety problems. A subcritical ADS operates in a flexible and safe manner, even with a core loading containing a high amount of MA leading to a high transmutation rate. In this paper, the most recent developments in the design of the MYRRHA facility are presented.

Application of gaseous core reactors for transmutation of nuclear waste

NASA Technical Reports Server (NTRS)

Schnitzler, B. G.; Paternoster, R. R.; Schneider, R. T.

1976-01-01

An acceptable management scheme for high-level radioactive waste is vital to the nuclear industry. The hazard potential of the trans-uranic actinides and of key fission products is high due to their nuclear activity and/or chemical toxicity. Of particular concern are the very long-lived nuclides whose hazard potential remains high for hundreds of thousands of years. Neutron induced transmutation offers a promising technique for the treatment of problem wastes. Transmutation is unique as a waste management scheme in that it offers the potential for "destruction" of the hazardous nuclides by conversion to non-hazardous or more manageable nuclides. The transmutation potential of a thermal spectrum uranium hexafluoride fueled cavity reactor was examined. Initial studies focused on a heavy water moderated cavity reactor fueled with 5% enriched U-235-F6 and operating with an average thermal flux of 6 times 10 to the 14th power neutrons/sq cm-sec. The isotopes considered for transmutation were I-129, Am-241, Am-242m, Am-243, Cm-243, Cm-244, Cm-245, and Cm-246.

MA transmutation performance in the optimized MYRRHA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Malambu, E.; Van den Eynde, G.; Fernandez, R.

MYRRHA (multi-purpose hybrid research reactor for high-tech applications) is a multipurpose research facility currently being developed at SCK-CEN. It will be able to work in both critical and subcritical modes and, cooled by lead-bismuth eutectic. In this paper the minor actinides (MA) transmutation capabilities of MYRRHA are investigated. (Pu + Am, U) MOX fuel and (Np + Am + Cm, Pu) Inert Matrix Fuel test samples have been loaded in the central channel of the MYRRHA critical core and have been irradiated during five cycles, each one consisting of 90 days of operation at 100 MWth and 30 days ofmore » shutdown. The reactivity worth of the test fuel assembly was about 1.1 dollar. A wide range of burn-up level has been achieved, extending from 42 to 110 MWd/kg HM, the samples with lower MA-to-Pu ratios reaching the highest burn-up. This study has highlighted the importance of the initial MA content, expressed in terms of MA/Pu ratio, on the transmutation rate of MA elements. For (Pu + Am, U) MOX fuel samples, a net build-up of MA is observed when the initial content of MA is very low (here, 1.77 wt% MA/Pu) while a net decrease in MA is observed in the sample with an initial content of 5 wt%. This suggests the existence of some 'equilibrium' initial MA content value beyond which a net transmutation is achievable.« less

A Multireference Density Functional Approach to the Calculation of the Excited States of Uranium Ions

DTIC Science & Technology

2007-03-01

approach. xiv A MULTIREFERENCE DENSITY FUNCTIONAL APPROACH TO THE CALCULATION OF THE EXCITED STATES OF URANIUM IONS I. Introduction Actinide chemistry, in...oxidation state of the uranium atom. Uranium, like most early actinides , can possess a wide range of oxidation states, ranging from +3 to +6, due in part...in predicting the electronic spectra for heavy element compounds. The first difficulty is that relativistic effects for actinides are significant

Predictive Modeling in Actinide Chemistry and Catalysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Ping

2016-05-16

These are slides from a presentation on predictive modeling in actinide chemistry and catalysis. The following topics are covered in these slides: Structures, bonding, and reactivity (bonding can be quantified by optical probes and theory, and electronic structures and reaction mechanisms of actinide complexes); Magnetic resonance properties (transition metal catalysts with multi-nuclear centers, and NMR/EPR parameters); Moving to more complex systems (surface chemistry of nanomaterials, and interactions of ligands with nanoparticles); Path forward and conclusions.

Actinides and Life's Origins.

PubMed

Adam, Zachary

2007-12-01

There are growing indications that life began in a radioactive beach environment. A geologic framework for the origin or support of life in a Hadean heavy mineral placer beach has been developed, based on the unique chemical properties of the lower-electronic actinides, which act as nuclear fissile and fertile fuels, radiolytic energy sources, oligomer catalysts, and coordinating ions (along with mineralogically associated lanthanides) for prototypical prebiotic homonuclear and dinuclear metalloenzymes. A four-factor nuclear reactor model was constructed to estimate how much uranium would have been required to initiate a sustainable fission reaction within a placer beach sand 4.3 billion years ago. It was calculated that about 1-8 weight percent of the sand would have to have been uraninite, depending on the weight percent, uranium enrichment, and quantity of neutron poisons present within the remaining placer minerals. Radiolysis experiments were conducted with various solvents with the use of uraniumand thorium-rich minerals (metatorbernite and monazite, respectively) as proxies for radioactive beach sand in contact with different carbon, hydrogen, oxygen, and nitrogen reactants. Radiation bombardment ranged in duration of exposure from 3 weeks to 6 months. Low levels of acetonitrile (estimated to be on the order of parts per billion in concentration) were conclusively identified in 2 setups and tentatively indicated in a 3(rd) by gas chromatography/mass spectrometry. These low levels have been interpreted within the context of a Hadean placer beach prebiotic framework to demonstrate the promise of investigating natural nuclear reactors as power production sites that might have assisted the origins of life on young rocky planets with a sufficiently differentiated crust/mantle structure. Future investigations are recommended to better quantify the complex relationships between energy release, radioactive grain size, fissionability, reactant phase, phosphorus release, and possible abiotic production of sugars, amino acids, activated phosphorus, prototypical organometallic enzymes, and oligomer catalysts at a single putative beach site.

Actinides and Life's Origins

NASA Astrophysics Data System (ADS)

Adam, Zachary

2007-12-01

There are growing indications that life began in a radioactive beach environment. A geologic framework for the origin or support of life in a Hadean heavy mineral placer beach has been developed, based on the unique chemical properties of the lower-electronic actinides, which act as nuclear fissile and fertile fuels, radiolytic energy sources, oligomer catalysts, and coordinating ions (along with mineralogically associated lanthanides) for prototypical prebiotic homonuclear and dinuclear metalloenzymes. A four-factor nuclear reactor model was constructed to estimate how much uranium would have been required to initiate a sustainable fission reaction within a placer beach sand 4.3 billion years ago. It was calculated that about 1-8 weight percent of the sand would have to have been uraninite, depending on the weight percent, uranium enrichment, and quantity of neutron poisons present within the remaining placer minerals. Radiolysis experiments were conducted with various solvents with the use of uranium- and thorium-rich minerals (metatorbernite and monazite, respectively) as proxies for radioactive beach sand in contact with different carbon, hydrogen, oxygen, and nitrogen reactants. Radiation bombardment ranged in duration of exposure from 3 weeks to 6 months. Low levels of acetonitrile (estimated to be on the order of parts per billion in concentration) were conclusively identified in 2 setups and tentatively indicated in a 3rd by gas chromatography/mass spectrometry. These low levels have been interpreted within the context of a Hadean placer beach prebiotic framework to demonstrate the promise of investigating natural nuclear reactors as power production sites that might have assisted the origins of life on young rocky planets with a sufficiently differentiated crust/mantle structure. Future investigations are recommended to better quantify the complex relationships between energy release, radioactive grain size, fissionability, reactant phase, phosphorus release, and possible abiotic production of sugars, amino acids, activated phosphorus, prototypical organometallic enzymes, and oligomer catalysts at a single putative beach site.

Method for decontamination of nickel-fluoride-coated nickel containing actinide-metal fluorides

DOEpatents

Windt, Norman F.; Williams, Joe L.

1983-01-01

The invention is a process for decontaminating particulate nickel contaminated with actinide-metal fluorides. In one aspect, the invention comprises contacting nickel-fluoride-coated nickel with gaseous ammonia at a temperature effecting nickel-catalyzed dissociation thereof and effecting hydrogen-reduction of the nickel fluoride. The resulting nickel is heated to form a melt and a slag and to effect transfer of actinide metals from the melt into the slag. The melt and slag are then separated. In another aspect, nickel containing nickel oxide and actinide metals is contacted with ammonia at a temperature effecting nickel-catalyzed dissociation to effect conversion of the nickel oxide to the metal. The resulting nickel is then melted and separated as described. In another aspect nickel-fluoride-coated nickel containing actinide-metal fluorides is contacted with both steam and ammonia. The resulting nickel then is melted and separated as described. The invention is characterized by higher nickel recovery, efficient use of ammonia, a substantial decrease in slag formation and fuming, and a valuable increase in the service life of the furnace liners used for melting.

Rapid determination of actinides in asphalt samples

DOE PAGES

Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.

2014-01-12

A new rapid method for the determination of actinides in asphalt samples has been developed that can be used in emergency response situations or for routine analysis If a radiological dispersive device (RDD), Improvised Nuclear Device (IND) or a nuclear accident such as the accident at the Fukushima Nuclear Power Plant in March, 2011 occurs, there will be an urgent need for rapid analyses of many different environmental matrices, including asphalt materials, to support dose mitigation and environmental clean up. The new method for the determination of actinides in asphalt utilizes a rapid furnace step to destroy bitumen and organicsmore » present in the asphalt and sodium hydroxide fusion to digest the remaining sample. Sample preconcentration steps are used to collect the actinides and a new stacked TRU Resin + DGA Resin column method is employed to separate the actinide isotopes in the asphalt samples. The TRU Resin plus DGA Resin separation approach, which allows sequential separation of plutonium, uranium, americium and curium isotopes in asphalt samples, can be applied to soil samples as well.« less

Energetics and Defect Interactions of Complex Oxides for Energy Applications

NASA Astrophysics Data System (ADS)

Solomon, Jonathan Michael

The goal of this dissertation is to employ computational methods to gain greater insights into the energetics and defect interactions of complex oxides that are relevant for today's energy challenges. To achieve this goal, the development of novel computational methodologies are required to handle complex systems, including systems containing nearly 650 ions and systems with tens of thousands of possible atomic configurations. The systems that are investigated in this dissertation are aliovalently doped lanthanum orthophosphate (LaPO4) due to its potential application as a proton conducting electrolyte for intermediate temperature fuel cells, and aliovalently doped uranium dioxide (UO2) due to its importance in nuclear fuel performance and disposal. First we undertake density-functional-theory (DFT) calculations on the relative energetics of pyrophosphate defects and protons in LaPO4, including their binding with divalent dopant cations. In particular, for supercell calculations with 1.85 mol% Sr doping, we investigate the dopant-binding energies for pyrophosphate defects to be 0.37 eV, which is comparable to the value of 0.34 eV calculated for proton-dopant binding energies in the same system. These results establish that dopant-defect interactions further stabilize proton incorporation, with the hydration enthalpies when the dopants are nearest and furthest from the protons and pyrophosphate defects being -1.66 eV and -1.37 eV, respectively. Even though our calculations show that dopant binding enhances the enthalpic favorability of proton incorporation, they also suggest that such binding is likely to substantially lower the kinetic rate of hydrolysis of pyrophosphate defects. We then shift our focus to solid solutions of fluorite-structured UO 2 with trivalent rare earth fission product cations (M3+=Y, La) using a combination of ionic pair potential and DFT based methods. Calculated enthalpies of formation with respect to constituent oxides show higher energetic stability for La solid solutions than for Y. Additionally, calculations performed for different atomic configurations show a preference for reduced (increased) oxygen vacancy coordination around La (Y) dopants. The current results are shown to be qualitatively consistent with related calculations and calorimetric measurements of heats of formation in other trivalent doped fluorite oxides, which show a tendency for increasing stability and increasing preference for higher oxygen coordination with increasing size of the trivalent impurity. We expand this investigation by considering a series of trivalent rare earth fission product cations, specifically, Y3+ (1.02 A, Shannon radius with eightfold coordination), Dy3+ (1.03 A), Gd 3+ (1.05 A), Eu3+ (1.07 A), Sm3+ (1.08 A), Pm3+ (1.09 A), Nd3+ (1.11 A), Pr3+ (1.13 A), Ce3+ (1.14 A) and La3+ (1.16 A). Compounds with ionic radius of the M3+ species smaller or larger than 1.09 A are found to have energetically preferred defect ordering arrangements. Systems with preferred defect ordering arrangements are suggestive of defect clustering in short range ordered solid solutions, which is expected to limit oxygen ion mobility and therefore the rate of oxidation of spent nuclear fuel. Finally, the energetics of rare earth substituted (M3+= La, Y, and Nd) UO2 solid solutions are investigated by employing a combination of calorimetric measurements and DFT based computations. The calorimetric studies are performed by Lei Zhang and Professor Alexandra Navrotsky at the University of Calfornia, Davis, as part of a joint computational/ experimental collaborative effort supported through the Materials Science of Actinides Energy Frontier Research Center. Calculated and measured formation enthalpies agree within 10 kJ/mol for stoichiometric oxygen/metal compositions. To better understand the factors governing the stability and defect binding in rare earth substituted urania solid solutions, systematic trends in the energetics are investigated based on the present results and previous computational and experimental thermochemical studies of rare earth substituted fluorite oxides. A consistent trend towards increased energetic stability with larger size mismatch between the smaller host tetravalent cation and the larger rare earth trivalent cation is found for both actinide and non-actinide fluorite oxide systems where aliovalent substitution of M cations is compensated by oxygen vacancies. However, the large exothermic oxidation enthalpy in the UO2 based systems favors compositions with higher oxygen-to-metal ratios where charge compensation occurs through the formation of uranium cations with higher oxidation states.

From carbon to actinides: A new universal 1MV accelerator mass spectrometer at ANSTO

NASA Astrophysics Data System (ADS)

Wilcken, K. M.; Hotchkis, M.; Levchenko, V.; Fink, D.; Hauser, T.; Kitchen, R.

2015-10-01

A new 1 MV NEC pelletron AMS system at ANSTO is presented. The spectrometer comprises large radius magnets for actinide measurements. A novel feature of the system is fast switching between isotopes both at low and high energy sections allowing measurements of up to 8 isotopes within a single sequence. Technical details and layout of the spectrometer is presented. Performance data for 14C, 10Be, 26Al and actinides demonstrate the system is ready for routine AMS measurements.

Pocket formula for nuclear deformations of actinides

NASA Astrophysics Data System (ADS)

Manjunatha, H. C.; Sridhar, K. N.

2018-06-01

We have formulated a pocket formula for quadrupole (β2), octupole (β3), hexadecapole (β4) and hexacontatetrapole (β6) deformation of the nuclear ground state of all isotopes of actinide nuclei (89 < Z < 103). This formula is first of its kind and produces a nuclear deformation of all isotopes actinide nuclei 89 < Z < 103 with simple inputs of Z and A. Hence, this formula is useful in the fields of nuclear physics to study the structure and interaction of nuclei.

Method for extracting lanthanides and actinides from acid solutions

DOEpatents

Horwitz, E. Philip; Kalina, Dale G.; Kaplan, Louis; Mason, George W.

1985-01-01

A process for the recovery of actinide and lanthanide values from aqueous acidic solutions with an organic extractant having the formula: ##STR1## where .phi. is phenyl, R.sup.1 is a straight or branched alkyl or alkoxyalkyl containing from 6 to 12 carbon atoms and R.sup.2 is an alkyl containing from 3 to 6 carbon atoms. The process is suitable for the separation of actinide and lanthanide values from fission product values found together in high level nuclear reprocessing waste solutions.

RAPID DETERMINATION OF ACTINIDES IN URINE BY INDUCTIVELY-COUPLED PLASMA MASS SPECTROMETRY AND ALPHA SPECTROMETRY: A HYBRID APPROACH

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maxwell, S.; Jones, V.

2009-05-27

A new rapid separation method that allows separation and preconcentration of actinides in urine samples was developed for the measurement of longer lived actinides by inductively coupled plasma mass spectrometry (ICP-MS) and short-lived actinides by alpha spectrometry; a hybrid approach. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration, if required, is performed using a streamlined calcium phosphate precipitation. Similar technology has been applied to separate actinides prior to measurement by alpha spectrometry, but this new method has been developed with elution reagents now compatible with ICP-MS as well. Purified solutions are splitmore » between ICP-MS and alpha spectrometry so that long- and short-lived actinide isotopes can be measured successfully. The method allows for simultaneous extraction of 24 samples (including QC samples) in less than 3 h. Simultaneous sample preparation can offer significant time savings over sequential sample preparation. For example, sequential sample preparation of 24 samples taking just 15 min each requires 6 h to complete. The simplicity and speed of this new method makes it attractive for radiological emergency response. If preconcentration is applied, the method is applicable to larger sample aliquots for occupational exposures as well. The chemical recoveries are typically greater than 90%, in contrast to other reported methods using flow injection separation techniques for urine samples where plutonium yields were 70-80%. This method allows measurement of both long-lived and short-lived actinide isotopes. 239Pu, 242Pu, 237Np, 243Am, 234U, 235U and 238U were measured by ICP-MS, while 236Pu, 238Pu, 239Pu, 241Am, 243Am and 244Cm were measured by alpha spectrometry. The method can also be adapted so that the separation of uranium isotopes for assay is not required, if uranium assay by direct dilution of the urine sample is preferred instead. Multiple vacuum box locations may be set-up to supply several ICP-MS units with purified sample fractions such that a high sample throughput may be achieved, while still allowing for rapid measurement of short-lived actinides by alpha spectrometry.« less

Implementation of a Thermodynamic Solver within a Computer Program for Calculating Fission-Product Release Fractions

NASA Astrophysics Data System (ADS)

Barber, Duncan Henry

During some postulated accidents at nuclear power stations, fuel cooling may be impaired. In such cases, the fuel heats up and the subsequent increased fission-gas release from the fuel to the gap may result in fuel sheath failure. After fuel sheath failure, the barrier between the coolant and the fuel pellets is lost or impaired, gases and vapours from the fuel-to-sheath gap and other open voids in the fuel pellets can be vented. Gases and steam from the coolant can enter the broken fuel sheath and interact with the fuel pellet surfaces and the fission-product inclusion on the fuel surface (including material at the surface of the fuel matrix). The chemistry of this interaction is an important mechanism to model in order to assess fission-product releases from fuel. Starting in 1995, the computer program SOURCE 2.0 was developed by the Canadian nuclear industry to model fission-product release from fuel during such accidents. SOURCE 2.0 has employed an early thermochemical model of irradiated uranium dioxide fuel developed at the Royal Military College of Canada. To overcome the limitations of computers of that time, the implementation of the RMC model employed lookup tables to pre-calculated equilibrium conditions. In the intervening years, the RMC model has been improved, the power of computers has increased significantly, and thermodynamic subroutine libraries have become available. This thesis is the result of extensive work based on these three factors. A prototype computer program (referred to as SC11) has been developed that uses a thermodynamic subroutine library to calculate thermodynamic equilibria using Gibbs energy minimization. The Gibbs energy minimization requires the system temperature (T) and pressure (P), and the inventory of chemical elements (n) in the system. In order to calculate the inventory of chemical elements in the fuel, the list of nuclides and nuclear isomers modelled in SC11 had to be expanded from the list used by SOURCE 2.0. A benchmark calculation demonstrates the improvement in agreement of the total inventory of those chemical elements included in the RMC fuel model to an ORIGEN-S calculation. ORIGEN-S is the Oak Ridge isotope generation and depletion computer program. The Gibbs energy minimizer requires a chemical database containing coefficients from which the Gibbs energy of pure compounds, gas and liquid mixtures, and solid solutions can be calculated. The RMC model of irradiated uranium dioxide fuel has been converted into the required format. The Gibbs energy minimizer has been incorporated into a new model of fission-product vaporization from the fuel surface. Calculated release fractions using the new code have been compared to results calculated with SOURCE IST 2.0P11 and to results of tests used in the validation of SOURCE 2.0. The new code shows improvements in agreement with experimental releases for a number of nuclides. Of particular significance is the better agreement between experimental and calculated release fractions for 140La. The improved agreement reflects the inclusion in the RMC model of the solubility of lanthanum (III) oxide (La2O3) in the fuel matrix. Calculated lanthanide release fractions from earlier computer programs were a challenge to environmental qualification analysis of equipment for some accident scenarios. The new prototype computer program would alleviate this concern. Keywords: Nuclear Engineering; Material Science; Thermodynamics; Radioactive Material, Gibbs Energy Minimization, Actinide Generation and Depletion, FissionProduct Generation and Depletion.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Levitskaia, Tatiana G.; Chatterjee, Sayandev; Pence, Natasha K.

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

Electrochemistry of actinides and fission products in molten salts-Data review

NASA Astrophysics Data System (ADS)

Zhang, Jinsuo

2014-04-01

The thermodynamic and electrochemical properties of actinides and fission products in the molten salt determine the pyroprocessing separation performance. Extensive measurements have been carried out to provide fundamental data for evaluating the separation efficiency and technology feasibility of pyroprocessing although the technology has been very well developed in laboratory. The state of the art of fundamental data for substance or materials involved in pyropocessing will be reviewed in the present article. The available data will be summarized and reanalyzed. New correlations, which extend the available data to a broad range of applications, will be developed based on available data from different measurements. Further research topics on providing fundamental data that is needed for scaling the current laboratory technology to industrial applications are identified.

Fusion barrier characteristics of actinides

NASA Astrophysics Data System (ADS)

Manjunatha, H. C.; Sridhar, K. N.

2018-03-01

We have studied fusion barrier characteristics of actinide compound nuclei with atomic number range 89 ≤ Z ≤ 103 for all projectile target combinations. After the calculation of fusion barrier heights and positions, we have searched for their parameterization. We have achieved the empirical formula for fusion barrier heights (VB), positions (RB), curvature of the inverted parabola (ħω) of actinide compound nuclei with atomic number range 89 ≤ Z ≤ 103 for all projectile target combinations (6

Electronic structure of free and doped actinides: N and Z dependences of energy levels and electronic structure parameters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kulagin, N.

2005-02-15

Theoretical study of electronic structure of antinide ions and its dependence on N and Z are presented in this paper. The main 5f{sup N} and excited 5f{sup N}n'l'{sup N'} configurations of actinides have been studied using Hartree-Fock-Pauli approximation. Results of calculations of radial integrals and the energy of X-ray lines for all 5f ions with electronic state AC{sup +1}-AC{sup +4} show approximate dependence on N and Z. A square of N and cubic of Z are ewalized for the primary electronic parameters of the actinides. Theoretical values of radial integrals for free actinides and for ions in a cluster AC{supmore » +n}:[L]{sub k} are compared, too.« less

Support for Students and Young Scientists to Participate in the 2009 Actinides Conference to be held in San Francisco, CA, Sunday, 12 July 2009 -- Friday, 17 July 2009

DOE Office of Scientific and Technical Information (OSTI.GOV)

Raymond, Kenneth N.

2011-04-08

Early career scientist were provided support to attend and participate in the Actinides 2009 (AN2009) International Conference held in San Francisco, California from 12-17 July 2011. This is the premier conference in the field of actinide chemistry, physics, and materials science of the actinide elements. Participation in the preeminent scientific meeting in actinide science keeps the U.S at the forefront of developments in this key field. The specific involvement of early career scientists combats the loss of expertise in the aforementioned critical areas related to f-element chemistry such as energy, homeland, and environmental security. Without these trained scientists, the U.S.more » will not be able to properly exploit nuclear technology to its fullest and will not be able to address its energy needs in either an environmentally safe or cost–effective manner nor will it be able to provide for its national defense. Furthermore, the early career scientists added greatly to the scientific content of the meeting and stimulates early career scientists to remain in the filed of actinide science. Providing support for participation in the AN2009 Conference via registration fee waivers, hotel cost support, and travel cost support, was extremely effective in securing the participation of early career scientists that would have not otherwise been able to attend.« less

Final Project Report for ER15351 “A Study of New Actinide Zintl Ion Materials”

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peter K. Dorhout

2007-11-12

The structural chemistry of actinide main-group metal materials provides the fundamental basis for the understanding of structural coordination chemistry and the formation of materials with desired or predicted structural features. The main-group metal building blocks, comprising sulfur-group, phosphorous-group, or silicon-group elements, have shown versatility in oxidation state, coordination, and bonding preferences. These building blocks have allowed us to elucidate a series of structures that are unique to the actinide elements, although we can find structural relationships to transition metal and 4f-element materials. In the past year, we investigated controlled metathesis and self-propagating reactions between actinide metal halides and alkali metalmore » salts of main-group metal chalcogenides such as K-P-S salts. Ternary plutonium thiophosphates have resulted from these reactions at low temperature in sealed ampules. we have also focused efforts to examine reactions of Th, U, and Pu halide salts with other alkali metal salts such as Na-Ge-S and Na-Si-Se and copper chloride to identify if self-propagating reactions may be used as a viable reaction to prepare new actinide materials and we prepared a series of U and Th copper chalcogenide materials. Magnetic measurements continued to be a focus of actinide materials prepared in our laboratory. We also contributed to the XANES work at Los Alamos by preparing materials for study and for comparison with environmental samples.« less

Challenges in the quality assurance of elemental and isotopic analyses in the nuclear domain benefitting from high resolution ICP-OES and sector field ICP-MS.

PubMed

Krachler, Michael; Alvarez-Sarandes, Rafael; Van Winckel, Stefaan

Accurate analytical data reinforces fundamentally the meaningfulness of nuclear fuel performance assessments and nuclear waste characterization. Regularly lacking matrix-matched certified reference materials, quality assurance of elemental and isotopic analysis of nuclear materials remains a challenging endeavour. In this context, this review highlights various dedicated experimental approaches envisaged at the European Commission-Joint Research Centre-Institute for Transuranium Elements to overcome this limitation, mainly focussing on the use of high resolution-inductively coupled plasma-optical emission spectrometry (HR-ICP-OES) and sector field-inductively coupled plasma-mass spectrometry (SF-ICP-MS). However, also α- and γ-spectrometry are included here to help characterise extensively the investigated actinide solutions for their actual concentration, potential impurities and isotopic purity.

Thermal reactions of uranium metal, UO 2, U 3O 8, UF 4, and UO 2F 2 with NF 3 to produce UF 6

NASA Astrophysics Data System (ADS)

McNamara, Bruce; Scheele, Randall; Kozelisky, Anne; Edwards, Matthew

2009-11-01

This paper demonstrates that NF 3 fluorinates uranium metal, UO 2, UF 4, UO 3, U 3O 8, and UO 2F 2·2H 2O to produce the volatile UF 6 at temperatures between 100 and 550 °C. Thermogravimetric and differential thermal analysis reaction profiles are described that reflect changes in the uranium fluorination/oxidation state, physiochemical effects, and instances of discrete chemical speciation. Large differences in the onset temperatures for each system investigated implicate changes in mode of the NF 3 gas-solid surface interaction. These studies also demonstrate that NF 3 is a potential replacement fluorinating agent in the existing nuclear fuel cycle and in actinide volatility reprocessing.