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.

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.

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

Transmutation of Nuclear Waste and the future MYRRHA Demonstrator

NASA Astrophysics Data System (ADS)

Mueller, Alex C.

2013-03-01

While a considerable and world-wide growth of the nuclear share in the global energy mix is desirable for many reasons, there are also, in particular in the "old world" major objections. These are both concerns about safety, in particular in the wake of the Fukushima nuclear accident and concerns about the long-term burden that is constituted by the radiotoxic waste from the spent fuel. With regard to the second topic, the present contribution will outline the concept of Partitioning & Transmutation (P&T), as scientific and technological answer. Deployment of P&T may use dedicated "Transmuter" or "Burner" reactors, using a fast neutron spectrum. For the transmutation of waste with a large content (up to 50%) of (very long-lived) Minor Actinides, a sub-critical reactor, using an external neutron source is a most attractive solution. It is constituted by coupling a proton accelerator, a spallation target and a subcritical core. This promising new technology is named ADS, for accelerator-driven system. The present paper aims at a short introduction into the field that has been characterized by a high collaborative activity during the last decade in Europe, in order to focus, in its later part, on the MYRRHA project as the European ADS technology demonstrator.

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

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.

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.

Vaporisation of candidate nuclear fuels and targets for transmutation of minor actinides

NASA Astrophysics Data System (ADS)

Gotcu-Freis, P.; Hiernaut, J.-P.; Colle, J.-Y.; Nästrén, C.; Carretero, A. Fernandez; Konings, R. J. M.

2011-04-01

The thermal stability and high temperature behaviour of candidate fuels and targets for transmutation of minor actinides has been investigated. Zirconia-based solid solution, MgO-based CERCER and molybdenum-based CERMET fuels containing Am and/or Pu in various concentrations were heated up to 2700 K in a Knudsen cell coupled with a quadrupole mass spectrometer, to measure their vapour pressure and vapour composition. The results reveal that the vaporisation of the actinides from the samples is not only determined by the thermodynamics of the system but is also related to the dynamic evolution of multi-component mixtures with complex composition or microstructure.

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

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.

Accuracy Improvement of Neutron Nuclear Data on Minor Actinides

NASA Astrophysics Data System (ADS)

Harada, Hideo; Iwamoto, Osamu; Iwamoto, Nobuyuki; Kimura, Atsushi; Terada, Kazushi; Nakao, Taro; Nakamura, Shoji; Mizuyama, Kazuhito; Igashira, Masayuki; Katabuchi, Tatsuya; Sano, Tadafumi; Takahashi, Yoshiyuki; Takamiya, Koichi; Pyeon, Cheol Ho; Fukutani, Satoshi; Fujii, Toshiyuki; Hori, Jun-ichi; Yagi, Takahiro; Yashima, Hiroshi

2015-05-01

Improvement of accuracy of neutron nuclear data for minor actinides (MAs) and long-lived fission products (LLFPs) is required for developing innovative nuclear system transmuting these nuclei. In order to meet the requirement, the project entitled as "Research and development for Accuracy Improvement of neutron nuclear data on Minor ACtinides (AIMAC)" has been started as one of the "Innovative Nuclear Research and Development Program" in Japan at October 2013. The AIMAC project team is composed of researchers in four different fields: differential nuclear data measurement, integral nuclear data measurement, nuclear chemistry, and nuclear data evaluation. By integrating all of the forefront knowledge and techniques in these fields, the team aims at improving the accuracy of the data. The background and research plan of the AIMAC project are presented.

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

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.

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

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.

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.

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

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.

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.

Progress on inert matrix fuels for minor actinide transmutation in fast reactor

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

Bonnerot, Jean-Marc; Ferroud-Plattet, Marie-Pierre; Lamontagne, Jerome

2007-07-01

An extensive irradiation program has been devoted by CEA to the assessment of transmutation using minor actinide bearing inert support targets. A first irradiation experiment was performed in the fast neutron reactor Phenix, in parallel to other experiments carried out in the HFR and Siloe reactors, in order to assess the behavior under fast neutron flux of various materials intended as inert support matrix for transmutation targets. This experiment, which included the two steps MATINA 1 and MATINA 1A, was completed in 2004 and underwent complete post irradiation examinations (PIE) , whose results are presented in this paper. All themore » pure inert materials showed a satisfactory behavior under fast neutrons except Al{sub 2}O{sub 3} - which exhibits a swelling close to 11 vol. % after irradiation. In presence of UO{sub 2} fissile particles, MgAl{sub 2}O{sub 4} proved to be more stable in term of swelling as inert support than MgO and Al{sub 2}O{sub 3} matrices, under the same irradiation conditions. A second experiment ECRIX H in Phenix involving composite pellets with an MgO matrix and AmO{sub 2-x} particles was completed in 2006. The very first PIE results on ECRIX H are described in this paper. At the light of these first experiments, a second phase dedicated to the design optimization of the target was initiated and three new irradiation experiments - MATINA 2-3, CAMIX COCHIX in Phenix and HELIOS in HFR - were started in 2006 and 2007. (authors)« less

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

Energy Production and Transmutation of Nuclear Waste by Accelerator Driven Systems

NASA Astrophysics Data System (ADS)

Zhivkov, P. K.

2018-05-01

There is a significant amount of highly radiotoxic long-life nuclear waste (NW) produced by NPP (Nuclear Power Plants). Transmutation is a process which transforms NW into less radiotoxic nuclides with a shorter period of half-life by spallation neutrons or radiative capture of neutrons produced by ADS (Accelerator Driven System). In the processes of transmutation new radioactive nuclides are produced. ADS is big energy consumer equipment. It is a method for production of a high-flux and high-energy neutron field. All these processes occur in ADS simultaneously. ADS is able to transmute actinides and produce energy simultaneously. The article considers the energy production problems in ADS. Several ideas are developed regarding the solution of the global energy supply.

Role of ADS in the back-end of the fuel cycle strategies and associated design activities: The case of Japan

NASA Astrophysics Data System (ADS)

Oigawa, Hiroyuki; Tsujimoto, Kazufumi; Nishihara, Kenji; Sugawara, Takanori; Kurata, Yuji; Takei, Hayanori; Saito, Shigeru; Sasa, Toshinobu; Obayashi, Hironari

2011-08-01

Reduction of burden caused by radioactive waste management is one of the most critical issues for the sustainable utilization of nuclear power. The Partitioning and Transmutation (P&T) technology provides the possibility to reduce the amount of the radiotoxic inventory of the high-level radioactive waste (HLW) dramatically and to extend the repository capacity. The accelerator-driven system (ADS) is regarded as a powerful tool to effectively transmute minor actinides (MAs) in the "double-strata" fuel cycle strategy. The ADS has a potential to flexibly manage MA in the transient phase from light water reactors (LWRs) to fast breeder reactors (FBRs), and can co-exist with FBR symbiotically and complementarily to enhance the reliability and the safety of the commercial FBR cycle. The concept of ADS in JAEA is a lead-bismuth eutectic (LBE) cooled, tank-type subcritical reactor with the power of 800 MWth driven by a 30 MW superconducting LINAC. By such an ADS, 250 kg of MA can be transmuted annually, which corresponds to the amount of MA produced in 10 units of LWR with 1 GWe. The design study was performed mainly for the subcritical reactor and the spallation target with a beam window. In Japan, Atomic Energy Commission (AEC) has implemented the check and review (C&R) on P&T technology from 2008 to 2009. In the C&R, the benefit of P&T technology, the current status of the R&D, and the way forward to promote it were discussed.

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.

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.

Transmutation of Radioactive Nuclear Waste — Present Status and Requirement for the Problem-Oriented Nuclear Database: Approach to Scheduling the Experiments (Reactor, Target, Blanket)

NASA Astrophysics Data System (ADS)

Artisyuk, V.; Ignatyuk, A.; Korovin, Yu.; Lopatkin, A.; Matveenko, I.; Stankovskiy, A.; Titarenko, Yu.

2005-05-01

Transmutation of nuclear wastes (Minor Actinides and Long-Lived Fission Products) remains an important option to reduce the burden of high-level waste on final waste disposal in deep geological structures. Accelerator-Driven Systems (ADS) are considered as possible candidates to perform transmutation due to their subcritical operation mode that eliminates some of the serious safety penalties unavoidable in critical reactors. Specific requirements to nuclear data necessary for ADS transmutation analysis is the main subject of the ISTC Project ♯2578 which started in 2004 to identify the areas of research priorities in the future. The present paper gives a summary of ongoing project stressing the importance of nuclear data for blanket performance (reactivity behavior with associated safety characteristics) and uncertainties that affect characteristics of neutron producing target.

Transuranic inventory reduction in repository by partitioning and transmutation

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

Kang, C.H.; Kazimi, M.S.

1992-01-01

The promise of a new reprocessing technology and the issuance of Environmental Protection Agency (EPA) and U.S. Nuclear Regulatory Commission regulations concerning a geologic repository rekindle the interest in partitioning and transmutation of transuranic (TRU) elements from discharged reactor fuel as a high level waste management option. This paper investigates the TRU repository inventory reduction capability of the proposed advanced liquid metal reactors (ALMRs) and integral fast reactors (IFRs) as well as the plutonium recycled light water reactors (LWRs).

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

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.

Uranium oxide fuel cycle analysis in VVER-1000 with VISTA simulation code

NASA Astrophysics Data System (ADS)

Mirekhtiary, Seyedeh Fatemeh; Abbasi, Akbar

2018-02-01

The VVER-1000 Nuclear power plant generates about 20-25 tons of spent fuel per year. In this research, the fuel transmutation of Uranium Oxide (UOX) fuel was calculated by using of nuclear fuel cycle simulation system (VISTA) code. In this simulation, we evaluated the back end components fuel cycle. The back end component calculations are Spent Fuel (SF), Actinide Inventory (AI) and Fission Product (FP) radioisotopes. The SF, AI and FP values were obtained 23.792178 ton/y, 22.811139 ton/y, 0.981039 ton/y, respectively. The obtained value of spent fuel, major actinide, and minor actinide and fission products were 23.8 ton/year, 22.795 ton/year, 0.024 ton/year and 0.981 ton/year, respectively.

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.

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

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.

New infrastructure for studies of transmutation and fast systems concepts

NASA Astrophysics Data System (ADS)

Panza, Fabio; Firpo, Gabriele; Lomonaco, Guglielmo; Osipenko, Mikhail; Ricco, Giovanni; Ripani, Marco; Saracco, Paolo; Viberti, Carlo Maria

2017-09-01

In this work we report initial studies on a low power Accelerator-Driven System as a possible experimental facility for the measurement of relevant integral nuclear quantities. In particular, we performed Monte Carlo simulations of minor actinides and fission products irradiation and estimated the fission rate within fission chambers in the reactor core and the reflector, in order to evaluate the transmutation rates and the measurement sensitivity. We also performed a photo-peak analysis of available experimental data from a research reactor, in order to estimate the expected sensitivity of this analysis method on the irradiation of samples in the ADS considered.

A low power ADS for transmutation studies in fast systems

NASA Astrophysics Data System (ADS)

Panza, Fabio; Firpo, Gabriele; Lomonaco, Guglielmo; Osipenko, Mikhail; Ricco, Giovanni; Ripani, Marco; Saracco, Paolo; Viberti, Carlo Maria

2017-12-01

In this work, we report studies on a fast low power accelerator driven system model as a possible experimental facility, focusing on its capabilities in terms of measurement of relevant integral nuclear quantities. In particular, we performed Monte Carlo simulations of minor actinides and fission products irradiation and estimated the fission rate within fission chambers in the reactor core and the reflector, in order to evaluate the transmutation rates and the measurement sensitivity. We also performed a photo-peak analysis of available experimental data from a research reactor, in order to estimate the expected sensitivity of this analysis method on the irradiation of samples in the ADS considered.

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

Laboratory actinide partitioning - Whitlockite/liquid and influence of actinide concentration levels

NASA Technical Reports Server (NTRS)

Benjamin, T. M.; Jones, J. H.; Heuser, W. R.; Burnett, D. S.

1983-01-01

The partition coefficients between synthetic whitlockite (beta Ca-phosphate) and coexisting silicate melts are determined for the actinide elements Th, U and Pu. Experiments were performed at 1 bar pressure and 1250 C at oxygen fugacities from 10 to the -8.5 to 10 to the -0.7 bars, and partitioning was determined from trace element radiography combined with conventional electron microprobe analysis. Results show Pu to be more readily incorporated into crystalline phases than U or Th under reducing conditions, which is attributed to the observation that Pu exists primarily in the trivalent state, while U and Th are tetravalent. Corrected partition coefficients for whitlockite of 3.6, less than or equal to 0.6, 1.2, 0.5 and less than or equal to 0.002 are estimated for Pu(+3), Pu(+4), Th(+4), U(+4) and U(+6), respectively. Experiments performed at trace levels and percent levels of UO2 indicate that Si is involved in U substitution in whitlockite, and show a reduced partition coefficient at higher concentrations of U that can be explained by effects on melt structure or the fraction of tetravalent U.

Apparatus for nuclear transmutation and power production using an intense accelerator-generated thermal neutron flux

DOEpatents

Bowman, C.D.

1992-11-03

Apparatus for nuclear transmutation and power production using an intense accelerator-generated thermal neutron flux. High thermal neutron fluxes generated from the action of a high power proton accelerator on a spallation target allows the efficient burn-up of higher actinide nuclear waste by a two-step process. Additionally, rapid burn-up of fission product waste for nuclides having small thermal neutron cross sections, and the practicality of small material inventories while achieving significant throughput derive from employment of such high fluxes. Several nuclear technology problems are addressed including 1. nuclear energy production without a waste stream requiring storage on a geological timescale, 2. the burn-up of defense and commercial nuclear waste, and 3. the production of defense nuclear material. The apparatus includes an accelerator, a target for neutron production surrounded by a blanket region for transmutation, a turbine for electric power production, and a chemical processing facility. In all applications, the accelerator power may be generated internally from fission and the waste produced thereby is transmuted internally so that waste management might not be required beyond the human lifespan.

Apparatus for nuclear transmutation and power production using an intense accelerator-generated thermal neutron flux

DOEpatents

Bowman, Charles D.

1992-01-01

Apparatus for nuclear transmutation and power production using an intense accelerator-generated thermal neutron flux. High thermal neutron fluxes generated from the action of a high power proton accelerator on a spallation target allows the efficient burn-up of higher actinide nuclear waste by a two-step process. Additionally, rapid burn-up of fission product waste for nuclides having small thermal neutron cross sections, and the practicality of small material inventories while achieving significant throughput derive from employment of such high fluxes. Several nuclear technology problems are addressed including 1. nuclear energy production without a waste stream requiring storage on a geological timescale, 2. the burn-up of defense and commercial nuclear waste, and 3. the production of defense nuclear material. The apparatus includes an accelerator, a target for neutron production surrounded by a blanket region for transmutation, a turbine for electric power production, and a chemical processing facility. In all applications, the accelerator power may be generated internally from fission and the waste produced thereby is transmuted internally so that waste management might not be required beyond the human lifespan.

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.

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.

The benefits of an advanced fast reactor fuel cycle for plutonium management

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

Hannum, W.H.; McFarlane, H.F.; Wade, D.C.

1996-12-31

The United States has no program to investigate advanced nuclear fuel cycles for the large-scale consumption of plutonium from military and civilian sources. The official U.S. position has been to focus on means to bury spent nuclear fuel from civilian reactors and to achieve the spent fuel standard for excess separated plutonium, which is considered by policy makers to be an urgent international priority. Recently, the National Research Council published a long awaited report on its study of potential separation and transmutation technologies (STATS), which concluded that in the nuclear energy phase-out scenario that they evaluated, transmutation of plutonium andmore » long-lived radioisotopes would not be worth the cost. However, at the American Nuclear Society Annual Meeting in June, 1996, the STATS panelists endorsed further study of partitioning to achieve superior waste forms for burial, and suggested that any further consideration of transmutation should be in the context of energy production, not of waste management. 2048 The U.S. Department of Energy (DOE) has an active program for the short-term disposition of excess fissile material and a `focus area` for safe, secure stabilization, storage and disposition of plutonium, but has no current programs for fast reactor development. Nevertheless, sufficient data exist to identify the potential advantages of an advanced fast reactor metallic fuel cycle for the long-term management of plutonium. Advantages are discussed.« less

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

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

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.

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

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

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.

Neutron induced fission of 237Np - status, challenges and opportunities

NASA Astrophysics Data System (ADS)

Ruskov, Ivan; Goverdovski, Andrei; Furman, Walter; Kopatch, Yury; Shcherbakov, Oleg; Hambsch, Franz-Josef; Oberstedt, Stephan; Oberstedt, Andreas

2018-03-01

Nowadays, there is an increased interest in a complete study of the neutron-induced fission of 237Np. This is due to the need of accurate and reliable nuclear data for nuclear science and technology. 237Np is generated (and accumulated) in the nuclear reactor core during reactor operation. As one of the most abundant long-lived isotopes in spent fuel ("waste"), the incineration of 237Np becomes an important issue. One scenario for burning of 237Np and other radio-toxic minor actinides suggests they are to be mixed into the fuel of future fast-neutron reactors, employing the so-called transmutation and partitioning technology. For testing present fission models, which are at the basis of new generation nuclear reactor developments, highly accurate and detailed neutron-induced nuclear reaction data is needed. However, the EXFOR nuclear database for 237Np on neutron-induced capture cross-section, σγ, and fission cross-section, σf, as well as on the characteristics of capture and fission resonance parameters (Γγ, Γf, σoΓf, fragments mass-energy yield distributions, multiplicities of neutrons vn and γ-rays vγ), has not been updated for decades.

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

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

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)

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

Industrial research for transmutation scenarios

NASA Astrophysics Data System (ADS)

Camarcat, Noel; Garzenne, Claude; Le Mer, Joël; Leroyer, Hadrien; Desroches, Estelle; Delbecq, Jean-Michel

2011-04-01

This article presents the results of research scenarios for americium transmutation in a 22nd century French nuclear fleet, using sodium fast breeder reactors. We benchmark the americium transmutation benefits and drawbacks with a reference case consisting of a hypothetical 60 GWe fleet of pure plutonium breeders. The fluxes in the various parts of the cycle (reactors, fabrication plants, reprocessing plants and underground disposals) are calculated using EDF's suite of codes, comparable in capabilities to those of other research facilities. We study underground thermal heat load reduction due to americium partitioning and repository area minimization. We endeavor to estimate the increased technical complexity of surface facilities to handle the americium fluxes in special fuel fabrication plants, americium fast burners, special reprocessing shops, handling equipments and transport casks between those facilities.

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

IAEA activities in the area of partitioning and transmutation

NASA Astrophysics Data System (ADS)

Stanculescu, Alexander

2006-06-01

Four major challenges are facing the long-term development of nuclear energy: improvement of the economic competitiveness, meeting increasingly stringent safety requirements, adhering to the criteria of sustainable development, and public acceptance. Meeting the sustainability criteria is the driving force behind the topic of this paper. In this context, sustainability has two aspects: natural resources and waste management. IAEA's activities in the area of Partitioning and Transmutation (P&T) are mostly in response to the latter. While not involving the large quantities of gaseous products and toxic solid wastes associated with fossil fuels, radioactive waste disposal is today's dominant public acceptance issue. In fact, small waste quantities permit a rigorous confinement strategy, and mined geological disposal is the strategy followed by some countries. Nevertheless, political opposition arguing that this does not yet constitute a safe disposal technology has largely stalled these efforts. One of the primary reasons cited is the long life of many of the radioisotopes generated from fission. This concern has led to increased R&D efforts to develop a technology aimed at reducing the amount and radio-toxicity of long-lived radioactive waste through transmutation in fission reactors or sub-critical systems. In the frame of the Project on Technology Advances in Fast Reactors and Accelerator-Driven Systems (ADS), the IAEA initiated a number of activities on utilization of plutonium and transmutation of long-lived radioactive waste, ADS, and deuterium-tritium plasma-driven sub-critical systems. The paper presents past accomplishments, current status and planned activities of this IAEA project.

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.

The Euratom Seventh Framework Programme FP7 (2007-2011)

NASA Astrophysics Data System (ADS)

Garbil, R.

2010-10-01

The objective of the Seventh Euratom Framework Program in the area of nuclear fission and radiation protection is to establish a sound scientific and technical basis to accelerate practical developments of nuclear energy related to resource efficiency, enhancing safety performance, cost-effectiveness and safer management of long-lived radioactive waste. Key cross-cutting topics such as the nuclear fuel cycle, actinide chemistry, risk analysis, safety assessment, even societal and governance issues are linked to the individual technical areas. Research need to explore new scientific and techno- logical opportunities and to respond in a flexible way to new policy needs that arise. The following activities are to be pursued. (a) Management of radioactive waste, research on partitioning and transmutation and/or other concepts aimed at reducing the amount and/or hazard of the waste for disposal; (b) Reactor systems research to underpin the con- tinued safe operation of all relevant types of existing reactor systems (including fuel cycle facilities), life-time extension, development of new advanced safety assessment methodologies and waste-management aspects of future reactor systems; (c) Radiation protection research in particular on the risks from low doses on medical uses and on the management of accidents; (d) Infrastructures and support given to the availability of, and cooperation between, research infrastructures necessary to maintain high standards of technical achievement, innovation and safety in the European nuclear sector and Research Area. (e) Human resources, mobility and training support to be provided for the retention and further development of scientific competence, human capacity through joint training activities in order to guarantee the availability of suitably qualified researchers, engineers and employees in the nuclear sector over the longer term.

II. Inhibited Diffusion Driven Surface Transmutations

NASA Astrophysics Data System (ADS)

Chubb, Talbot A.

2006-02-01

This paper is the second of a set of three papers dealing with the role of coherent partitioning as a common element in Low Energy Nuclear Reactions (LENR), by which is meant cold-fusion related processes. This paper discusses the first step in a sequence of four steps that seem to be necessary to explain Iwamura 2-α-addition surface transmutations. Three concepts are examined: salt-metal interface states, sequential tunneling that transitions D+ ions from localized interstitial to Bloch form, and the general applicability of 2-dimensional vs. 3-dimensional symmetry hosting networks.

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.

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.

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).

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

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

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.

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

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

Actinide targets for fundamental research in nuclear physics

NASA Astrophysics Data System (ADS)

Eberhardt, K.; Düllmann, Ch. E.; Haas, R.; Mokry, Ch.; Runke, J.; Thörle-Pospiech, P.; Trautmann, N.

2018-05-01

Thin actinide layers deposited on various substrates are widely used as calibration sources in nuclear spectroscopy. Other applications include fundamental research in nuclear chemistry and -physics, e.g., the chemical and physical properties of super-heavy elements (SHE, Z > 103) or nuclear reaction studies with heavy ions. For the design of future nuclear reactors like fast-fission reactors and accelerator-driven systems for transmutation of nuclear waste, precise data for neutron absorption as well as neutron-induced fission cross section data for 242Pu with neutrons of different energies are of particular importance, requiring suitable Pu-targets. Another application includes studies of nuclear transitions in 229Th harvested as α-decay recoil product from a thin layer of its 233U precursor. For this, a thin and very smooth layer of 233U is used. We report here on the production of actinide layers mostly obtained by Molecular Plating (MP). MP is currently the only fabrication method in cases where the desired actinide material is available only in very limited amounts or possesses a high specific activity. Here, deposition is performed from organic solution applying a current density of 1-2 mA/cm2. Under these conditions target thicknesses of 500-1000 μg/cm2 are possible applying a single deposition step with deposition yields approaching 100 %. For yield determination α-particle spectroscopy, γ-spectroscopy and Neutron Activation Analysis is routinely used. Layer homogeneity is checked with Radiographic Imaging. As an alternative technique to MP the production of thin lanthanide and actinide layers by the so-called "Drop on Demand"-technique applied e.g., in ink-jet printing is currently under investigation.

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

Partitioning of K, U, and Th between sulfide and silicate liquids - Implications for radioactive heating of planetary cores

NASA Technical Reports Server (NTRS)

Murrell, M. T.; Burnett, D. S.

1986-01-01

Experimental partitioning studies are reported of K, U, and Th between silicate and FeFeS liquids designed to test the proposal that actinide partitioning into sulfide liquids is more important then K partitioning in the radioactive heating of planetary cores. For a basaltic liquid at 1450 C and 1.5 GPa, U partitioning into FeFeS liquids is five times greater than K partitioning. A typical value for the liquid partition coefficient for U from a granitic silicate liquid at one atmosphere at 1150 C and low fO2 is about 0.02; the coefficient for Th is similar. At low fO2 and higher temperature, experiments with basaltic liquids produce strong Ca and U partitioning into the sulfide liquid with U coefficient greater than one. The Th coefficient is less strongly affected.

Transmutation of All German Transuranium under Nuclear Phase Out Conditions – Is This Feasible from Neutronic Point of View?

PubMed Central

Merk, Bruno; Litskevich, Dzianis

2015-01-01

The German government has decided for the nuclear phase out, but a decision on a strategy for the management of the highly radioactive waste is not defined yet. Partitioning and Transmutation (P&T) could be considered as a technological option for the management of highly radioactive waste, therefore a wide study has been conducted. In the study group objectives for P&T and the boundary conditions of the phase out have been discussed. The fulfillment of the given objectives is analyzed from neutronics point of view using simulations of a molten salt reactor with fast neutron spectrum. It is shown that the efficient transmutation of all existing transuranium isotopes would be possible from neutronic point of view in a time frame of about 60 years. For this task three reactors of a mostly new technology would have to be developed and a twofold life cycle consisting of a transmuter operation and a deep burn phase would be required. A basic insight for the optimization of the time duration of the deep burn phase is given. Further on, a detailed balance of different isotopic inventories is given to allow a deeper understanding of the processes during transmutation in the molten salt fast reactor. The effect of modeling and simulation is investigated based on three different modeling strategies and two different code versions. PMID:26717509

Transmutation of All German Transuranium under Nuclear Phase Out Conditions - Is This Feasible from Neutronic Point of View?

PubMed

Merk, Bruno; Litskevich, Dzianis

2015-01-01

The German government has decided for the nuclear phase out, but a decision on a strategy for the management of the highly radioactive waste is not defined yet. Partitioning and Transmutation (P&T) could be considered as a technological option for the management of highly radioactive waste, therefore a wide study has been conducted. In the study group objectives for P&T and the boundary conditions of the phase out have been discussed. The fulfillment of the given objectives is analyzed from neutronics point of view using simulations of a molten salt reactor with fast neutron spectrum. It is shown that the efficient transmutation of all existing transuranium isotopes would be possible from neutronic point of view in a time frame of about 60 years. For this task three reactors of a mostly new technology would have to be developed and a twofold life cycle consisting of a transmuter operation and a deep burn phase would be required. A basic insight for the optimization of the time duration of the deep burn phase is given. Further on, a detailed balance of different isotopic inventories is given to allow a deeper understanding of the processes during transmutation in the molten salt fast reactor. The effect of modeling and simulation is investigated based on three different modeling strategies and two different code versions.

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.

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

Experimental geochemistry of Pu and Sm and the thermodynamics of trace element partitioning

NASA Technical Reports Server (NTRS)

Jones, John H.; Burnett, Donald S.

1987-01-01

An experimental study of the partitioning of Pu and Sm between diopside/liquid and whitlockite/liquid supports the hypothesis that Pu behaves as a light rare earth element during igneous processes in reducing environments. D-Pu/D-Sm is found to be about 2 for both diopsidic pyroxene and whitlockite, and the amount of fractionation would be decreased further if Pu were compared to Ce or Nd. Data indicate that temperature, rather than melt composition, is the most important control on elemental partitioning, and that P2O5 in aluminosilicate melts serves as a complexing agent for the actinides and lanthanides.

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

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)

Concept of grouping in partitioning of HLW for self-consistent fuel cycle

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

Kitamoto, A.; Mulyanto

1993-12-31

A concept of grouping for partitioning of HLW has been developed in order to examine the possibility of a self-consistent fuel recycle. The concept of grouping of radionuclides is proposed herein, such as Group MA1 (MA below Cm), Group MA2 (Cm and higher MA), Group A ({sup 99}Tc and I), Group B (Cs and Sr) and Group R (the partitioned remain of HLW). Group B is difficult to be transmuted by neutron reaction, so a radiation application in an industrial scale should be developed in the future. Group A and Group MA1 can be burned by a thermal reactor, onmore » the other hand Group MA2 should be burned by a fast reactor. P-T treatment can be optimized for the in-core and out-core system, respectively.« 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

The feasibility of using molten carbonate corrosion for separating a nuclear surrogate for plutonium oxide from silicon carbide inert matrix

NASA Astrophysics Data System (ADS)

Cheng, Ting; Baney, Ronald H.; Tulenko, James

2010-10-01

Silicon carbide is one of the prime candidates as a matrix material in inert matrix fuels (IMF) being designed to reduce the plutonium inventories. Since complete fission and transmutation is not practical in a single in-core run, it is necessary to separate the non-transmuted actinide materials from the silicon carbide matrix for recycling. In this work, SiC was corroded in sodium carbonate (Na 2CO 3) and potassium carbonate (K 2CO 3), to form water soluble sodium or potassium silicate. Separation of the transuranics was achieved by dissolving the SiC corrosion product in boiling water. Ceria (CeO 2), which was used as a surrogate for plutonium oxide (PuO 2), was not corroded in these molten salt environments. The molten salt depth, which is a distance between the salt/air interface to the upper surface of SiC pellets, significantly affected the rate of corrosion. The corrosion was faster in K 2CO 3 than in Na 2CO 3 molten salt at 1050 °C, when the initial molten salt depths were kept the same for both salts.

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

Separations in the STATS report

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

Choppin, G.R.

1996-12-31

The Separations Technology and Transmutation Systems (STATS) Committee formed a Subcommittee on Separations. This subcommittee was charged with evaluating the separations proposed for the several reactor and accelerator transmutation systems. It was also asked to review the processing options for the safe management of high-level waste generated by the defense programs, in particular, the special problems involved in dealing with the waste at the U.S. Department of Energy (DOE) facility in Hanford, Washington. Based on the evaluations from the Subcommittee on Separations, the STATS Committee concluded that for the reactor transmutation programs, aqueous separations involving a combination of PUREX andmore » TRUEX solvent extraction processes could be used. However, additional research and development (R&D) would be required before full plant-scale use of the TRUEX technology could be employed. Alternate separations technology for the reactor transmutation program involves pyroprocessing. This process would require a significant amount of R&D before its full-scale application can be evaluated.« less

Separation of Long-Lived Fission Products Tc-99 and I-129 from Synthetic Effluents by Crown Ethers

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

Paviet-Hartmann, P.; Hartmann, T.

2006-07-01

To minimize significantly the radio-toxic inventory of nuclear geological repositories to come as well as to reduce the potential of radionuclides migration and to minimize long-term exposure, the concept of partitioning and transmutation (P/T) of nuclear waste is currently discussed. Transmutation offers the possibility to convert radio-toxic radionuclides with long half-lives into radionuclides of shorter half-lives, less toxic isotopes, or even into stable isotopes. Besides the most prominent isotopes of neptunium, plutonium, americium, and curium, the long-lived fission products Tc-99 and I-129 (half-lives of 2.13 x 10{sup 5} years, and 1.57 x 10{sup 7} years, respectively) are promising candidates formore » transmutation in order to prevent their migration from a nuclear repository. Partitioning and transmutation of the most radio-toxic radionuclides will not only minimize the nuclear waste load but most importantly will significantly reduce the long-term radio-toxic hazard of nuclear waste repositories to come. Prior to the deployment of partitioning and transmutation, selective extraction techniques are required to separate the radionuclides of concern. Since the discovery of crown ethers by C. Pedersen, various applications of crown ethers have drawn much attention. Although liquid-liquid extraction of alkali and alkali earth metals by crown ethers has been extensively studied, little data is available on the extraction of Tc-99 and I-129 by crown ethers. The methods developed herein for the specific extraction of Tc-99 and I-129 provide recommendations in support of their selectively extraction from liquid radioactive waste streams, mainly ILW. We report data on the solvent extraction of Tc-99 and I-129 from synthetic effluents by six crown ethers of varying cavity dimensions and derivatization. To satisfy the needs of new extractant systems we are demonstrating that crown ether (CE) based systems have the potential to serve as selective extractants for the separation of these long lived radionuclides from high level nuclear waste (HLW), intermediate level nuclear waste (ILW), and low level nuclear waste (LLW) streams. The experimental results show that dibenzo-18-crown-6 (DB 18C6) is highly selective towards Tc-99, and dicyclohexano-18-crown-6 (DC18C6) is highly selective towards I-129. The nature of the diluent was examined and was shown to be the most influential variable in controlling the extraction coefficients of Tc-99 and I-129. Therefore the addition of polar diluent acetone to non-polar diluent toluene enhanced the distribution coefficient of Tc-99 (DTc) was by a factor of 30. For I-129, the best extraction yield was obtained after introducing tetrachloroethane. Through the process, by a single extraction step, 85 % to 95 % of Tc-99 was extracted from synthetic effluents, while 84 % to 88 % of I-129 was extracted from different acidic media. The extraction by crown ether is a fairly rapid process and the total preparation time of the chemical separation takes about 20 minutes for a batch of eight samples. (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

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

Utilization of Methacrylates and Polymer Matrices for the Synthesis of Ion Specific Resins

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

Czerwinski, Kenneth

2013-10-29

Disposal, storage, and/or transmutation of actinides such as americium (Am) will require the development of specific separation schemes. Existing efforts focus on solvent extraction systems for achieving suitable separation of actinide from lanthanides. However, previous work has shown the feasibility of ion-imprinting polymer-based resins for use in ion-exchange-type separations with metal ion recognition. Phenolic-based resins have been shown to function well for Am-Eu separations, but these resins exhibited slow kinetics and difficulties in the imprinting process. This project addresses the need for new and innovative methods for the selective separation of actinides through novel ion-imprinted resins. The project team willmore » explore incorporation of metals into extended frameworks, including the possibility of 3D polymerized matrices that can serve as a solid-state template for specific resin preparation. For example, an anhydrous trivalent f-element chain can be formed directly from a metal carbonate, and methacrylic acid from water. From these simple coordination complexes, molecules of discrete size or shape can be formed via the utilization of coordinating ligands or by use of an anionic multi-ligand system incorporating methacrylate. Additionally, alkyl methyl methacrylates have been used successfully to create template nanospaces, which underscores their potential utility as 3D polymerized matrices. This evidence provides a unique route for the preparation of a specific metal ion template for the basis of ion-exchange separations. Such separations may prove to be excellent discriminators of metal ions, even between f-elements. Resins were prepared and evaluated for sorption behavior, column properties, and proton exchange capacity.« less

Insight into the Am-O Phase Equilibria: A Thermodynamic Study Coupling High-Temperature XRD and CALPHAD Modeling.

PubMed

Epifano, Enrica; Guéneau, Christine; Belin, Renaud C; Vauchy, Romain; Lebreton, Florent; Richaud, Jean-Christophe; Joly, Alexis; Valot, Christophe; Martin, Philippe M

2017-07-03

In the frame of minor actinide transmutation, americium can be diluted in UO 2 and (U, Pu)O 2 fuels burned in fast neutron reactors. The first mandatory step to foresee the influence of Am on the in-reactor behavior of transmutation targets or fuel is to have fundamental knowledge of the Am-O binary system and, in particular, of the AmO 2-x phase. In this study, we coupled HT-XRD (high-temperature X-ray diffraction) experiments with CALPHAD thermodynamic modeling to provide new insights into the structural properties and phase equilibria in the AmO 2-x -AmO 1.61+x -Am 2 O 3 domain. Because of this approach, we were able for the first time to assess the relationships between temperature, lattice parameter, and hypostoichiometry for fcc AmO 2-x . We showed the presence of a hyperstoichiometric existence domain for the bcc AmO 1.61+x phase and the absence of a miscibility gap in the fcc AmO 2-x phase, contrary to previous representations of the phase diagram. Finally, with the new experimental data, a new CALPHAD thermodynamic model of the Am-O system was developed, and an improved version of the phase diagram is presented.

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

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

LOS ALAMOS NEUTRON SCIENCE CENTER CONTRIBUTIONS TO THE DEVELOPMENT OF FUTURE POWER REACTORS

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

GAVRON, VICTOR I.; HILL, TONY S.; PITCHER, ERIC J.

The Los Alamos Neutron Science Center (LANSCE) is a large spallation neutron complex centered around an 800 MeV high-currently proton accelerator. Existing facilities include a highly-moderated neutron facility (Lujan Center) where neutrons between thermal and keV energies are produced, and the Weapons Neutron Research Center (WNR), where a bare spallation target produces neutrons between 0.1 and several hundred MeV.The LANSCE facility offers a unique capability to provide high precision nuclear data over a large energy region, including that for fast reactor systems. In an ongoing experimental program the fission and capture cross sections are being measured for a number ofmore » minor actinides relevant for Generation-IV reactors and transmutation technology. Fission experiments makes use of both the highly moderated spallation neutron spectrum at the Lujan Center, and the unmoderated high energy spectrum at WNR. By combininb measurements at these two facilities the differential fission cross section is measured relative to the {sup 235}U(n,f) standard from subthermal energies up to about 200 MeV. An elaborate data acquisition system is designed to deal with all the different types of background present when spanning 10 energy decades. The first isotope to be measured was {sup 237}Np, and the results were used to improve the current ENDF/B-VII evaluation. Partial results have also been obtained for {sup 240}Pu and {sup 242}Pu, and the final results are expected shortly. Capture cross sections are measured at LANSCE using the Detector for Advanced Neutron Capture Experiments (DANCE). This unique instrument is highly efficient in detecting radiative capture events, and can thus handle radioactive samples of half-lives as low as 100 years. A number of capture cross sections important to fast reaction applications have been measured with DANCE. The first measurement was on {sup 237}Np(n,{gamma}), and the results have been submitted for publication. Other capture measurements in progress include {sup 240}Pu and {sup 242}Pu. The United States recently announced the Global Nuclear Energy Partnership (GNEP), with the goal of closing the commercial nuclear fuel cycle while minimizing proliferation risk. GNEP achieves these goals using fast-spectrum nuclear reactors powered by new transmutation fuels that contain significant quantities of minor actinides. The proposed Materials Test Station (MTS) will provide the GNEP with a cost-effective means of obtaining domestic fast-spectrum irradiations of advanced transmutation fuel forms and structural materials, which is an important step in the fuels qualification process. The MTS will be located at the LANSCE, and will be driven by a 1.08-MW proton beam. Th epeak neutron flux in the irradiation region is 1.67 x 10{sup 15} n/cm{sup 2}/s, and the energy spectrum is similar to that of a fast reactor, with the addition of a high-energy tail. The facility is expected to operate at least 4,400 hours per year. Fuel burnup rates will exceed 4% per year, and the radiation damage rate in iron will be 18 dpa (displacements per atom) per year. The construction cost is estimated to be $73M (including 25% contingency), with annual operating costs in the range of $6M to $10M. Appropriately funded, the MTS could begin operation in 2010.« 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

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.

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

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

Nuclear transmutation in steels

NASA Astrophysics Data System (ADS)

Belozerova, A. R.; Shimanskii, G. A.; Belozerov, S. V.

2009-05-01

The investigations of the effects of nuclear transmutation in steels that are widely used in nuclear power and research reactors and in steels that are planned for the application in thermonuclear fusion plants, which are employed under the conditions of a prolonged action of neutron irradiation with different spectra, made it possible to study the effects of changes in the isotopic and chemical composition on the tendency of changes in the structural stability of these steels. For the computations of nuclear transmutation in steels, we used a program complex we have previously developed on the basis of algorithms for constructing branched block-type diagrams of nuclide transformations and for locally and globally optimizing these diagrams with the purpose of minimizing systematic errors in the calculation of nuclear transmutation. The dependences obtained were applied onto a Schaeffler diagram for steels used for structural elements of reactors. For the irradiation in fission reactors, we observed only a weak influence of the effects of nuclear transmutation in steels on their structural stability. On the contrary, in the case of irradiation with fusion neutrons, a strong influence of the effects of nuclear transmutation in steels on their structural stability has been noted.

Neutron cross section measurements at n-TOF for ADS related studies

NASA Astrophysics Data System (ADS)

Mastinu, P. F.; Abbondanno, U.; Aerts, G.; Álvarez, H.; Alvarez-Velarde, F.; Andriamonje, S.; Andrzejewski, J.; Assimakopoulos, P.; Audouin, L.; Badurek, G.; Bustreo, N.; aumann, P.; vá, F. Be; Berthoumieux, E.; Calviño, F.; Cano-Ott, D.; Capote, R.; Carrillo de Albornoz, A.; Cennini, P.; Chepel, V.; Chiaveri, E.; Colonna, N.; Cortes, G.; Couture, A.; Cox, J.; Dahlfors, M.; David, S.; Dillmann, I.; Dolfini, R.; Domingo-Pardo, C.; Dridi, W.; Duran, I.; Eleftheriadis, C.; Embid-Segura, M.; Ferrant, L.; Ferrari, A.; Ferreira-Marques, R.; itzpatrick, L.; Frais-Kölbl, H.; Fujii, K.; Furman, W.; Guerrero, C.; Goncalves, I.; Gallino, R.; Gonzalez-Romero, E.; Goverdovski, A.; Gramegna, F.; Griesmayer, E.; Gunsing, F.; Haas, B.; Haight, R.; Heil, M.; Herrera-Martinez, A.; Igashira, M.; Isaev, S.; Jericha, E.; Kadi, Y.; Käppeler, F.; Karamanis, D.; Karadimos, D.; Kerveno, M.; Ketlerov, V.; Koehler, P.; Konovalov, V.; Kossionides, E.; Krti ka, M.; Lamboudis, C.; Leeb, H.; Lindote, A.; Lopes, I.; Lozano, M.; Lukic, S.; Marganiec, J.; Marques, L.; Marrone, S.; Massimi, C.; Mengoni, A.; Milazzo, P. M.; Moreau, C.; Mosconi, M.; Neves, F.; Oberhummer, H.; O'Brien, S.; Oshima, M.; Pancin, J.; Papachristodoulou, C.; Papadopoulos, C.; Paradela, C.; Patronis, N.; Pavlik, A.; Pavlopoulos, P.; Perrot, L.; Plag, R.; Plompen, A.; Plukis, A.; Poch, A.; Pretel, C.; Quesada, J.; Rauscher, T.; Reifarth, R.; Rosetti, M.; Rubbia, C.; Rudolf, G.; Rullhusen, P.; Salgado, J.; Sarchiapone, L.; Savvidis, I.; Stephan, C.; Tagliente, G.; Tain, J. L.; Tassan-Got, L.; Tavora, L.; Terlizzi, R.; Vannini, G.; Vaz, P.; Ventura, A.; Villamarin, D.; Vincente, M. C.; Vlachoudis, V.; Vlastou, R.; Voss, F.; Walter, S.; Wendler, H.; Wiescherand, M.; Wisshak, K.

2006-05-01

A neutron Time-of-Flight facility (n_TOF) is available at CERN since 2001. The innovative features of the neutron beam, in particular the high instantaneous flux, the wide energy range, the high resolution and the low background, make this facility unique for measurements of neutron induced reactions relevant to the field of Emerging Nuclear Technologies, as well as to Nuclear Astrophysics and Fundamental Nuclear Physics. The scientific motivations that have led to the construction of this new facility are here presented. The main characteristics of the n_TOF neutron beam are described, together with the features of the experimental apparata used for cross-section measurements. The main results of the first measurement campaigns are presented. Preliminary results of capture cross-section measurements of minor actinides, important to ADS project for nuclear waste transmutation, are finally discussed.

YALINA facility a sub-critical Accelerator- Driven System (ADS) for nuclear energy research facility description and an overview of the research program (1997-2008).

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

Gohar, Y.; Smith, D. L.; Nuclear Engineering Division

2010-04-28

The YALINA facility is a zero-power, sub-critical assembly driven by a conventional neutron generator. It was conceived, constructed, and put into operation at the Radiation Physics and Chemistry Problems Institute of the National Academy of Sciences of Belarus located in Minsk-Sosny, Belarus. This facility was conceived for the purpose of investigating the static and dynamic neutronics properties of accelerator driven sub-critical systems, and to serve as a neutron source for investigating the properties of nuclear reactions, in particular transmutation reactions involving minor-actinide nuclei. This report provides a detailed description of this facility and documents the progress of research carried outmore » there during a period of approximately a decade since the facility was conceived and built until the end of 2008. During its history of development and operation to date (1997-2008), the YALINA facility has hosted several foreign groups that worked with the resident staff as collaborators. The participation of Argonne National Laboratory in the YALINA research programs commenced in 2005. For obvious reasons, special emphasis is placed in this report on the work at YALINA facility that has involved Argonne's participation. Attention is given here to the experimental program at YALINA facility as well as to analytical investigations aimed at validating codes and computational procedures and at providing a better understanding of the physics and operational behavior of the YALINA facility in particular, and ADS systems in general, during the period 1997-2008.« less

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

Chen, Jing-Yuan; Son, Jun Ho; Wang, Chao

The idea of statistical transmutation plays a crucial role in descriptions of the fractional quantum Hall effect. However, a recently conjectured duality between a critical boson and a massless two-component Dirac fermion extends this notion to gapless systems. This duality sheds light on highly nontrivial problems such as the half-filled Landau level, the superconductor-insulator transition, and surface states of strongly coupled topological insulators. Although this boson-fermion duality has undergone many consistency checks, it has remained unproven. Here, we describe the duality in a nonperturbative fashion using an exact UV mapping of partition functions on a 3D Euclidean lattice.

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

Dunn, Darrell; Poinssot, Christophe; Begg, Bruce

Management of nuclear waste remains an important international topic that includes reprocessing of commercial nuclear fuel, waste-form design and development, storage and disposal packaging, the process of repository site selection, system design, and performance assessment. Requirements to manage and dispose of materials from the production of nuclear weapons, and the renewed interest in nuclear power, in particular through the Generation IV Forum and the Advanced Fuel Cycle Initiative, can be expected to increase the need for scientific advances in waste management. A broad range of scientific and engineering disciplines is necessary to provide safe and effective solutions and address complexmore » issues. This volume offers an interdisciplinary perspective on materials-related issues associated with nuclear waste management programs. Invited and contributed papers cover a wide range of topics including studies on: spent fuel; performance assessment and models; waste forms for low- and intermediate-level waste; ceramic and glass waste forms for plutonium and high-level waste; radionuclides; containers and engineered barriers; disposal environments and site characteristics; and partitioning and transmutation.« less

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.

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

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.

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.

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.

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

Youinou, Gilles Jean-Michel

Neutron cross-sections characterize the way neutrons interact with matter. They are essential to most nuclear engineering projects and, even though theoretical progress has been made as far as the predictability of neutron cross-section models, measurements are still indispensable to meet tight design requirements for reduced uncertainties. Within the field of fission reactor technology, one can identify the following specializations that rely on the availability of accurate neutron cross-sections: (1) fission reactor design, (2) nuclear fuel cycles, (3) nuclear safety, (4) nuclear safeguards, (5) reactor monitoring and neutron fluence determination and (6) waste disposal and transmutation. In particular, the assessment ofmore » advanced fuel cycles requires an extensive knowledge of transuranics cross sections. Plutonium isotopes, but also americium, curium and up to californium isotope data are required with a small uncertainty in order to optimize significant features of the fuel cycle that have an impact on feasibility studies (e.g. neutron doses at fuel fabrication, decay heat in a repository, etc.). Different techniques are available to determine neutron cross sections experimentally, with the common denominator that a source of neutrons is necessary. It can either come from an accelerator that produces neutrons as a result of interactions between charged particles and a target, or it can come from a nuclear reactor. When the measurements are performed with an accelerator, they are referred to as differential since the analysis of the data provides the cross-sections for different discrete energies, i.e. σ(E i), and for the diffusion cross sections for different discrete angles. Another approach is to irradiate a very pure sample in a test reactor such as the Advanced Test Reactor (ATR) at INL and, after a given time, determine the amount of the different transmutation products. The precise characterization of the nuclide densities before and after neutron irradiation allows to infer energy-integrated neutron cross sections, i.e. ∫₀ ∞σ(E)φ(E)dE, where φ(E) is the neutron flux “seen” by the sample. This approach, which is usually defined and led by reactor physicists, is referred to as integral and is the object of this report. These two sources of information, i.e. differential and integral, are complementary and are used by the nuclear physicists in charge of producing the evaluated nuclear data files used by the nuclear community (ENDF, JEFF…). The generation of accurate nuclear data files requires an iterative process involving reactor physicists and nuclear data evaluators. This experimental program has been funded by the ATR National Scientific User Facility (ATR-NSUF) and by the DOE Office of Science in the framework of the Recovery Act. It has been given the name MANTRA for Measurement of Actinides Neutron TRAnsmutation.« less

Exact Boson-Fermion Duality on a 3D Euclidean Lattice

DOE PAGES

Chen, Jing-Yuan; Son, Jun Ho; Wang, Chao; ...

2018-01-05

The idea of statistical transmutation plays a crucial role in descriptions of the fractional quantum Hall effect. However, a recently conjectured duality between a critical boson and a massless two-component Dirac fermion extends this notion to gapless systems. This duality sheds light on highly nontrivial problems such as the half-filled Landau level, the superconductor-insulator transition, and surface states of strongly coupled topological insulators. Although this boson-fermion duality has undergone many consistency checks, it has remained unproven. Here, we describe the duality in a nonperturbative fashion using an exact UV mapping of partition functions on a 3D Euclidean lattice.

Exact Boson-Fermion Duality on a 3D Euclidean Lattice.

PubMed

Chen, Jing-Yuan; Son, Jun Ho; Wang, Chao; Raghu, S

2018-01-05

The idea of statistical transmutation plays a crucial role in descriptions of the fractional quantum Hall effect. However, a recently conjectured duality between a critical boson and a massless two-component Dirac fermion extends this notion to gapless systems. This duality sheds light on highly nontrivial problems such as the half-filled Landau level, the superconductor-insulator transition, and surface states of strongly coupled topological insulators. Although this boson-fermion duality has undergone many consistency checks, it has remained unproven. We describe the duality in a nonperturbative fashion using an exact UV mapping of partition functions on a 3D Euclidean lattice.

Exact Boson-Fermion Duality on a 3D Euclidean Lattice

NASA Astrophysics Data System (ADS)

Chen, Jing-Yuan; Son, Jun Ho; Wang, Chao; Raghu, S.

2018-01-01

The idea of statistical transmutation plays a crucial role in descriptions of the fractional quantum Hall effect. However, a recently conjectured duality between a critical boson and a massless two-component Dirac fermion extends this notion to gapless systems. This duality sheds light on highly nontrivial problems such as the half-filled Landau level, the superconductor-insulator transition, and surface states of strongly coupled topological insulators. Although this boson-fermion duality has undergone many consistency checks, it has remained unproven. We describe the duality in a nonperturbative fashion using an exact UV mapping of partition functions on a 3D Euclidean lattice.

Private Sector Initiative Between the U.S. and Japan

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

None

1998-09-30

OAK-A258 Private Sector Initiative Between the U.S. and Japan. This report for calendar years 1993 through September 1998 describes efforts performed under the Private Sector Initiatives contract. The report also describes those efforts that have continued with private funding after being initiated under this contract. The development of a pyrochemical process, called TRUMP-S, for partitioning actinides from PUREX waste, is described in this report. This effort is funded by the Central Research Institute of Electric Power Industry (CRIEPI), KHI, the United States Department of Energy, and Boeing.

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

The physics of sub-critical lattices in accelerator driven hybrid systems: The MUSE experiments in the MASURCA facility

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

Chauvin, J. P.; Lebrat, J. F.; Soule, R.

Since 1991, the CEA has studied the physics of hybrid systems, involving a sub-critical reactor coupled with an accelerator. These studies have provided information on the potential of hybrid systems to transmute actinides and, long lived fission products. The potential of such a system remains to be proven, specifically in terms of the physical understanding of the different phenomena involved and their modelling, as well as in terms of experimental validation of coupled systems, sub-critical environment/accelerator. This validation must be achieved through mock-up studies of the sub-critical environments coupled to a source of external neutrons. The MUSE-4 mock-up experiment ismore » planed at the MASURCA facility and will use an accelerator coupled to a tritium target. The great step between the generator used in the past and the accelerator will allow to increase the knowledge in hybrid physic and to decrease the experimental biases and the measurement uncertainties.« 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

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

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

Trace Metal-Humic Complexes in Natural Waters: Insights From Speciation Experiments

NASA Astrophysics Data System (ADS)

Stern, J. C.; Salters, V.; Sonke, J.

2006-12-01

The DOM cycle is intimately linked to the cycling and bioavailability of trace metals in aqueous environments. The presence or absence of DOM in the water column can determined whether trace elements will be present in limited quantities as a nutrient, or in surplus quantities as a toxicant. Humic substances (HS), which represent the refractory products of DOM degradation, strongly affect the speciation of trace metals in natural waters. To simulate metal-HS interactions in nature, experiments must be carried out using trace metal concentrations. Sensitive detection systems such as ICP-MS make working with small (nanomolar) concentrations possible. Capillary electrophoresis coupled with ICP-MS (CE-ICP-MS) has recently been identified as a rapid and accurate method to separate metal species and calculate conditional binding constants (log K_c) of metal-humic complexes. CE-ICP-MS was used to measure partitioning of metals between humic substances and a competing ligand (EDTA) and calculate binding constants of rare earth element (REE) and Th, Hf, and Zr-humic complexes at pH 3.5-8 and ionic strength of 0.1. Equilibrium dialysis ligand exchange (EDLE) experiments to validate the CE-ICP-MS method were performed to separate the metal-HS and metal-EDTA species by partitioning due to size exclusion via diffusion through a 1000 Da membrane. CE-ICP-MS experiments were also conducted to compare binding constants of REE with humic substances of various origin, including soil, peat, and aquatic DOM. Results of our experiments show an increase in log K_c with decrease in ionic radius for REE-humic complexes (the lanthanide contraction effect). Conditional binding constants of tetravalent metal-humic complexes were found to be several orders of magnitude higher than REE-humic complexes, indicating that tetravalent metals have a very strong affinity for humic substances. Because thorium is often used as a proxy for the tetravalent actinides, Th-HS binding constants can allow us to assess the importance of tetravalent actinide-humic complexes in groundwater transport from nuclear repositories. Our results suggest that tetravalent actinide-humic complexes couild be more important to account for in predictive speciation models than previously thought.

Structural response of Nd-stabilized zirconia and its composite under extreme conditions of swift heavy ion irradiation

NASA Astrophysics Data System (ADS)

Nandi, Chiranjit; Grover, V.; Kulriya, P. K.; Poswal, A. K.; Prakash, Amrit; Khan, K. B.; Avasthi, D. K.; Tyagi, A. K.

2018-02-01

Inert matrix fuel concept for minor actinide transmutation proposes stabilized zirconia as the major component for inert matrix. The present study explores Nd-stabilized zirconia (Zr0.8Nd0.2O1.9; Nd as surrogate for Am) and its composites for radiation tolerance against fission fragments. The introduction of MgO in the composite with stabilised zirconia is performed from the point of view to enhance the thermal conductivity. The radiation damage is also compared with Nd-stabilized zirconia co-doped with Y3+ (Zr0.8Nd0.1Y0.1O1.9) in order to mimic doping of minor actinides in Y3+ containing stabilized zirconia (Nd as surrogate for Am). The compositions were synthesized by gel combustion followed by high temperature sintering and characterised by XRD, SEM and EDS. Irradiation was carried out by 120 MeV Au ions at various fluences and irradiation induced structural changes were probed by in-situ X-ray diffraction (XRD). XRD demonstrated the retention of crystallinity for all the three samples but the extent of the damage was found to be highly dependent on the nominal composition. It was observed that introduction of Y3+ along with Nd3+ to stabilize cubic zirconia imparted poorer radiation stability. On the other hand, formation of a CERCER composite of MgO with Nd-stabilised zirconia enhanced its behaviour against swift heavy ion irradiation. Investigating these compositions by XANES spectroscopy post irradiation did not show any change in local electronic structure of constituent ions.

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

Structural study of (N{sub 2}H{sub 5},H){sub 2.9}U{sub 1.1}Ce{sub 0.9}(C{sub 2}O{sub 4}){sub 5}·10H{sub 2}O from a conventional X-ray diffraction diagram obtained on a powder synthesized by a fast vortex process

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

Brackx, E., E-mail: Emmanuelle.brackx@cea.fr; Laval, J.P.; Dugne, O.

2015-01-15

In the context of research on U/minor actinides for nuclear fuel reprocessing in the transmutation process, developments are first studied with surrogates containing uranium and lanthanides to facilitate testing. The tests consist of precipitating and calcining a hydrazinium uranium/cerium oxalate. The structure of this oxalate had not been previously determined, but was necessary to validate the physicochemical mechanisms involved. The present study, firstly demonstrates the structural similarity of the U/Ce oxalate phase (N{sub 2}H{sub 5},H){sub 2.9}U{sub 1.1}Ce{sub 0.9}(C{sub 2}O{sub 4}){sub 5}·10H{sub 2}O, synthesized using a vortex precipitator for continuous synthesis of actinide oxalates, with previously known oxalates, crystallizing in P6{submore » 3}/mmc symmetry, obtained by more classical methods. This fast precipitation process induces massive nucleation of fine powders. Their structural and microstructural determination confirms that the raw and dried phases belong to the same structural family as (NH{sub 4}){sub 2}U{sub 2}(C{sub 2}O{sub 4}){sub 5}·0.7H{sub 2}O whose structure was described by Chapelet-Arab in P6{sub 3}/mmc symmetry, using single crystal data. However, they present an extended disorder inside the tunnels of the structure, even after drying at 100 °C, between water and hydrazinium ions. This disorder is directly related to the fast vortex method. This structure determination can be used as a basis for further semi-quantitative analysis on the U/minor actinides products formed under various experimental conditions. - Highlights: • Uranium cerium oxalate precipitate characterization by X-ray powder diffraction. • Morphology characterization by SEM analysis. • Structure determination by unit cell Rietveld refinement.« 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.; 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

Theory and methods for measuring the effective multiplication constant in ADS

NASA Astrophysics Data System (ADS)

Rugama Saez, Yolanda

2001-10-01

In the thesis an absolute measurements technique for the subcriticality determination is presented. The ADS is a hybrid system where a subcritical system is fed by a proton accelerator. There are different proposals to define an ADS, one is to use plutonium and minor actinides from power plants waste as fuel to be transmuted into non radioactive isotopes (transmuter/burner, ATW). Another proposal is to use a Th232-U233 cycle (Energy Amplifier), being that thorium is an interesting and abundant fertile isotope. The development of accelerator driven systems (ADS) requires the development of methods to monitor and control the subcriticality of this kind of system without interfering with its normal operation mode. With this finality, we have applied noise analysis techniques that allow us to characterise the system when it is operating. The method presented in this thesis is based on the stochastic neutron and photon transport theory that can be implemented by presently available neutron/photon transport codes. In this work, first we analyse the stochastic transport theory which has been applied to define a parameter to determine the subcritical reactivity monitoring measurements. Finally we give the main limitations and recommendations for these subcritical monitoring methodology. As a result of the theoretical methodology, done in the first part of this thesis, a monitoring measurement technique has been developed and verified using two coupled Monte Carlo programs. The first one, LAHET, simulates the spallation collisions and the high energy transport and the other, MCNP-DSP, is used to estimate the counting statistics from a neutron/photon ray counter in a fissile system, as well as the transport for neutron with energies less than 20 MeV. From the coupling of both codes we developed the LAHET/MCNP-DSP code which, has the capability to simulate the total process in the ADS from the proton interaction to the signal detector processing. In these simulations, we compute the cross power spectral densities between pairs of detectors located inside the system which, is defined as the measured parameter. From the comparison of the theoretical predictions with the Monte Carlo simulations, we obtain some practical and simple methods to determine the system multiplication constant. (Abstract shortened by UMI.)

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

Optical Lattice Bose-Einstein Condensates and the dd Fusion - Iwamura Connection

NASA Astrophysics Data System (ADS)

Chubb, Talbot

2003-03-01

My conjecture: LENR dd fusion occurs in PdDx when a subset of the interstitial deuterons occupy tetrahedral sites in a PdDx crystallite. The tetrahedral deuterons(d's), which occupy shallow potential wells, behave as a superfluid, similar to ultracold Na atoms in shallow-well optical traps, as modeled by Jaksch et al.(D. Jaksch, et al, Phys. Rev. Lett., 81, 3108 (1998).) The tetrahedral d's form a deuteron (d) subsystem, which is neutralized by an electron subsystem containing an equal number of electrons. In the superfluid all the properties of each quasiparticle d are partitioned among N_s_i_te equivalent sites. The partitioning of the d point charge reduces the Coulomb self-repulsion within each quasiparticle pair, which causes wave function overlap at large N_s_i_t_e, allowing d-d fusion. Similarly, partitioning of the point charge of each single quasiparticle d reduces the Coulomb repulsion between it and an obstructing impurity atom, which causes wave function overlap between quasiparticle and atom at large N_s_i_t_e, allowing transmutation of the impurity atom. The Iwamura reaction(Y. Iwamura, et al, Japan J. of Appl. Physics, 41A, 4642 (2002).) is 4 ^2D^+_B_l_o_ch + 4 e^-_B_l_o_ch + ^1^3^3Cs arrow ^1^4^1Pr, with the reaction energy incoherently transferred to the lattice.

TPE/REE separation with the use of zirconium salt of HDBP

NASA Astrophysics Data System (ADS)

Glekov, R. G.; Shmidt, O. V.; Palenik, Yu. V.; Goletsky, N. D.; Sukhareva, S. Yu.; Fedorov, Yu. S.; Zilberman, B. Ya.

2003-01-01

Partitioning of long-lived radionuclides (minor actinides, fission products) is considered as TBP-compatible ZEALEX-process for extraction separation of transplutonium elements (TPE) and rare-earth elements (REE), as well as Y, Mo, Fe and residual amounts of Np, Pu, U. Zirconium salt of dibutyl phosphoric acid (ZS-HDBP) dissolved in 30 % TBP is used as a solvent. The process was tested in multistage centrifugal contactors. Lanthanides, Y and TPE, as well as Mo, Fe were extracted from high-level Purex raffinate, Am and ceric subgroup of REE being separated from the polyvalent elements by stripping with HNO3. TPE/REE partitioning was achieved in the second cycle of the ZEALEX-process using DTPA in formic acid media. The integral decontamination factor of Am from La and Ce after both cycles is >200, from Pr and Nd 20-30 and from Sm and Eu 3.6; REE strips in both cycles contained <0,1% of the initial amount of TPE.

Demonstration of the TRUEX process for partitioning of actinides from actual ICPP tank waste using centrifugal contactors in a shielded cell facility

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

Law, J.D.; Brewer, K.N.; Herbst, R.S.

1996-09-01

TRUEX is being evaluated at Idaho Chemical Processing Plant (ICPP) for separating actinides from acidic radioactive waste stored at ICPP; efforts have culminated in a recent demonstration with actual tank waste. A continuous countercurrent flowsheet test was successfully completed at ICPP using waste from tank WM-183. This demonstration was performed using 24 states of 2-cm dia centrifugal contactors in the shielded hot cell at the ICPP Remote Analytical Laboratory. The flowsheet had 8 extraction stages, 5 scrub stages, 6 strip stages, 3 solvent wash stages, and 2 acid rinse stages. A centrifugal contactor stage in the scrub section was notmore » working during testing, and the scrub feed (aqueous) solution followed the solvent into the strip section, eliminating the scrub section in the flowsheet. An overall removal efficiency of 99.97% was obtained for the actinides, reducing the activity from 457 nCi/g in the feed to 0.12 nCi/g in the aqueous raffinate, well below the NRC Class A LLW requirement of 10 nCi/g for non-TRU waste.The 0.04 M HEDPA strip section back-extracted 99.9998% of the actinide from the TRUEX solvent. Removal efficiencies of >99. 90, 99.96, 99.98, >98.89, 93.3, and 89% were obtained for {sup 241}Am, {sup 238}Pu, {sup 239}Pu, {sup 235}U, {sup 238}U, and {sup 99}Tc. Fe was partially extracted by the TRUEX solvent, resulting in 23% of the Fe exiting in the strip product. Hg was also extracted by the TRUEX solvent (73%) and stripped from the solvent in the 0.25 M Na2CO3 wash section. Only 1.4% of the Hg exited with the high activity waste strip product.« less

Analyses of transients for an 800 MW-class accelerator driven transmuter with fertile-free fuels

NASA Astrophysics Data System (ADS)

Maschek, Werner; Suzuki, Tohru; Chen, Xue-Nong; Rineiski, Andrei; Matzerath Boccaccini, Claudia; Mori, Magnus; Morita, Koji

2006-06-01

In the FUTURE Program, the development and application of fertile-free fuels for Accelerator Driven Transmuters (ADTs) has been advanced. To assess the reactor performance and safety behavior of an ADT with so-called dedicated fuels, various transient cases for an 800 MW-class Pb/Bi-cooled ADT were investigated using the SIMMER-III code. The FUTURE ADT also served as vehicle to develop and test ideas on a safety concept for such transmuters. After an extensive ranking procedure, a CERCER fuel with an MgO matrix and a CERMET fuel with a Mo-92 matrix were chosen. The transient scenarios shown here are: spurious beam trip (BT), unprotected loss of flow (ULOF) and unprotected blockage accident (UBA). Since the release of fission gas and helium after cladding failure could induce a significant positive reactivity, the gas-blowdown was investigated for the transient scenarios. The present analyses showed that power excursions could be avoided by the fuel sweep-out from the core under severe accident conditions.

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.

Measurement of the 241Am neutron capture cross section at the n_TOF facility at CERN

NASA Astrophysics Data System (ADS)

Mendoza, E.; Cano-Ott, D.; Altstadt, S.; Andriamonje, S.; Andrzejewski, J.; Audouin, L.; Balibrea, J.; Bécares, V.; Barbagallo, M.; Bečvář, F.; Belloni, F.; Berthier, B.; Berthoumieux, E.; Billowes, J.; Boccone, V.; Bosnar, D.; Brugger, M.; Calviño, F.; Calviani, M.; Carrapiço, C.; Cerutti, F.; Chiaveri, E.; Chin, M.; Colonna, N.; Cortés, G.; Cortés-Giraldo, M. A.; Diakaki, M.; Dillmann, I.; Domingo-Pardo, C.; Durán, I.; Dzysiuk, N.; Eleftheriadis, C.; Fernández-Ordóñez, M.; Ferrari, A.; Fraval, K.; Furman, V.; Gómez-Hornillos, M. B.; Ganesan, S.; García, A. R.; Giubrone, G.; Gonçalves, I. F.; González, E.; Goverdovski, A.; Gramegna, F.; Griesmayer, E.; Guerrero, C.; Gunsing, F.; Gurusamy, P.; Heftrich, T.; Heinitz, S.; Hernández-Prieto, A.; Heyse, J.; Jenkins, D. G.; Jericha, E.; Käppeler, F.; Kadi, Y.; Karadimos, D.; Katabuchi, T.; Ketlerov, V.; Khryachkov, V.; Koehler, P.; Kokkoris, M.; Kroll, J.; Krtička, M.; Lampoudis, C.; Langer, C.; Leal-Cidoncha, E.; Lederer, C.; Leeb, H.; Leong, L. S.; Lerendegui-Marco, J.; Licata, M.; Losito, R.; Manousos, A.; Marganiec, J.; Martínez, T.; Massimi, C.; Mastinu, P.; Mastromarco, M.; Mengoni, A.; Milazzo, P. M.; Mingrone, F.; Mirea, M.; Mondelaers, W.; Paradela, C.; Pavlik, A.; Perkowski, J.; Plompen, A. J. M.; Praena, J.; Quesada, J. M.; Rauscher, T.; Reifarth, R.; Riego-Perez, A.; Robles, M.; Roman, F.; Rubbia, C.; Ryan, J. A.; Sabaté-Gilarte, M.; Sarmento, R.; Saxena, A.; Schillebeeckx, P.; Schmidt, S.; Schumann, D.; Sedyshev, P.; Tagliente, G.; Tain, J. L.; Tarifeño-Saldivia, A.; Tarrío, D.; Tassan-Got, L.; Tsinganis, A.; Valenta, S.; Vannini, G.; Variale, V.; Vaz, P.; Ventura, A.; Vermeulen, M. J.; Versaci, R.; Vlachoudis, V.; Vlastou, R.; Wallner, A.; Ware, T.; Weigand, M.; Weiss, C.; Wright, T.; Žugec, P.

2017-09-01

New neutron cross section measurements of minor actinides have been performed recently in order to reduce the uncertainties in the evaluated data, which is important for the design of advanced nuclear reactors and, in particular, for determining their performance in the transmutation of nuclear waste. We have measured the 241Am(n,γ) cross section at the n_TOF facility between 0.2 eV and 10 keV with a BaF2 Total Absorption Calorimeter, and the analysis of the measurement has been recently concluded. Our results are in reasonable agreement below 20 eV with the ones published by C. Lampoudis et al. in 2013, who reported a 22% larger capture cross section up to 110 eV compared to experimental and evaluated data published before. Our results also indicate that the 241Am(n,γ) cross section is underestimated in the present evaluated libraries between 20 eV and 2 keV by 25%, on average, and up to 35% for certain evaluations and energy ranges.

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.

The CCONE Code System and its Application to Nuclear Data Evaluation for Fission and Other Reactions

NASA Astrophysics Data System (ADS)

Iwamoto, O.; Iwamoto, N.; Kunieda, S.; Minato, F.; Shibata, K.

2016-01-01

A computer code system, CCONE, was developed for nuclear data evaluation within the JENDL project. The CCONE code system integrates various nuclear reaction models needed to describe nucleon, light charged nuclei up to alpha-particle and photon induced reactions. The code is written in the C++ programming language using an object-oriented technology. At first, it was applied to neutron-induced reaction data on actinides, which were compiled into JENDL Actinide File 2008 and JENDL-4.0. It has been extensively used in various nuclear data evaluations for both actinide and non-actinide nuclei. The CCONE code has been upgraded to nuclear data evaluation at higher incident energies for neutron-, proton-, and photon-induced reactions. It was also used for estimating β-delayed neutron emission. This paper describes the CCONE code system indicating the concept and design of coding and inputs. Details of the formulation for modelings of the direct, pre-equilibrium and compound reactions are presented. Applications to the nuclear data evaluations such as neutron-induced reactions on actinides and medium-heavy nuclei, high-energy nucleon-induced reactions, photonuclear reaction and β-delayed neutron emission are mentioned.

Fuel Sustainability And Actinide Production Of Doping Minor Actinide In Water-Cooled Thorium Reactor

NASA Astrophysics Data System (ADS)

Permana, Sidik

2017-07-01

Fuel sustainability of nuclear energy is coming from an optimum fuel utilization of the reactor and fuel breeding program. Fuel cycle option becomes more important for fuel cycle utilization as well as fuel sustainability capability of the reactor. One of the important issues for recycle fuel option is nuclear proliferation resistance issue due to production plutonium. To reduce the proliferation resistance level, some barriers were used such as matrial barrier of nuclear fuel based on isotopic composition of even mass number of plutonium isotope. Analysis on nuclear fuel sustainability and actinide production composition based on water-cooled thorium reactor system has been done and all actinide composition are recycled into the reactor as a basic fuel cycle scheme. Some important parameters are evaluated such as doping composition of minor actinide (MA) and volume ratio of moderator to fuel (MFR). Some feasible parameters of breeding gains have been obtained by additional MA doping and some less moderation to fuel ratios (MFR). The system shows that plutonium and MA are obtained low compositions and it obtains some higher productions of even mass plutonium, which is mainly Pu-238 composition, as a control material to protect plutonium to be used as explosive devices.

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

The physics design of accelerator-driven transmutation systems

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

Venneri, F.

1995-10-01

Nuclear systems under study in the Los Alamos Accelerator-Driven Transmutation Technology program (ADTT) will allow the destruction of nuclear spent fuel and weapons-return plutonium, as well as the production of nuclear energy from the thorium cycle, without a long-lived radioactive waste stream. The subcritical systems proposed represent a radical departure from traditional nuclear concepts (reactors), yet the actual implementation of ADTT systems is based on modest extrapolations of existing technology. These systems strive to keep the best that the nuclear technology has developed over the years, within a sensible conservative design envelope and eventually manage to offer a safe, lessmore » expensive and more environmentally sound approach to nuclear power.« 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

Feasibility study of nuclear transmutation by negative muon capture reaction using the PHITS code

NASA Astrophysics Data System (ADS)

Abe, Shin-ichiro; Sato, Tatsuhiko

2016-06-01

Feasibility of nuclear transmutation of fission products in high-level radioactive waste by negative muon capture reaction is investigated using the Particle and Heave Ion Transport code System (PHITS). It is found that about 80 % of stopped negative muons contribute to transmute target nuclide into stable or short-lived nuclide in the case of 135Cs, which is one of the most important nuclide in the transmutation. The simulation result also indicates that the position of transmutation is controllable by changing the energy of incident negative muon. Based on our simulation, it takes approximately 8.5 × 108years to transmute 500 g of 135Cs by negative muon beam with the highest intensity currently available.

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.

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''.

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

Clinical Investigation Program Report

DTIC Science & Technology

1992-10-01

alchemists claim of transmutation of metals by asserting the fundamental differen- ii ces of metals. His medical masterwork was the Canon which remained an...1992. Blount BW: Sexually transmitted disease update. Am Acad Fam Phy, Washington, DC, Oct 1991. Blount BW: A comparison of Family Practice content

Copper Doping of Zinc Oxide by Nuclear Transmutation

DTIC Science & Technology

2014-03-27

Copper Doping of Zinc Oxide by Nuclear Transmutation THESIS Matthew C. Recker, Captain, USAF AFIT-ENP-14-M-30 DEPARTMENT OF THE AIR FORCE AIR...NUCLEAR TRANSMUTATION THESIS Presented to the Faculty Department of Engineering Physics Graduate School of Engineering and Management Air Force...COPPER DOPING OF ZINC OXIDE BY NUCLEAR TRANSMUTATION Matthew C. Recker, BS Captain, USAF Approved: //signed// 27 February 2014 John W. McClory, PhD

``Recycling'' Nuclear Power Plant Waste: Technical Difficulties and Proliferation Concerns

NASA Astrophysics Data System (ADS)

Lyman, Edwin

2007-04-01

One of the most vexing problems associated with nuclear energy is the inability to find a technically and politically viable solution for the disposal of long-lived radioactive waste. The U.S. plan to develop a geologic repository for spent nuclear fuel at Yucca Mountain in Nevada is in jeopardy, as a result of managerial incompetence, political opposition and regulatory standards that may be impossible to meet. As a result, there is growing interest in technologies that are claimed to have the potential to drastically reduce the amount of waste that would require geologic burial and the length of time that the waste would require containment. A scenario for such a vision was presented in the December 2005 Scientific American. While details differ, these technologies share a common approach: they require chemical processing of spent fuel to extract plutonium and other long-lived actinide elements, which would then be ``recycled'' into fresh fuel for advanced reactors and ``transmuted'' into shorter-lived fission products. Such a scheme is the basis for the ``Global Nuclear Energy Partnership,'' a major program unveiled by the Department of Energy (DOE) in early 2006. This concept is not new, but has been studied for decades. Major obstacles include fundamental safety issues, engineering feasibility and cost. Perhaps the most important consideration in the post-9/11 era is that these technologies involve the separation of plutonium and other nuclear weapon-usable materials from highly radioactive fission products, providing opportunities for terrorists seeking to obtain nuclear weapons. While DOE claims that it will only utilize processes that do not produce ``separated plutonium,'' it has offered no evidence that such technologies would effectively deter theft. It is doubtful that DOE's scheme can be implemented without an unacceptable increase in the risk of nuclear terrorism.

Contributions of basic nuclear physics to the nuclear waste management

NASA Astrophysics Data System (ADS)

Flocard, Hubert

2002-04-01

Nuclear fission is presently a contested method of electricity production. The issue of nuclear waste management stands out among the reasons why. On the other hand, the nuclear industry has demonstrated its capacity to reliably generate cheap electricity while producing negligible amounts of greenhouse gases. These assets explain why this form of energy is still considered among the options for the long term production of electricity at least in developed countries. However, in order to tackle the still not adequately answered question of the waste, new schemes may have to be considered. Among those which have been advanced recently, the less polluting cycles such as those based on Thorium rather than Uranium and/or the transmutation of the minor actinides and some long lived fission products of the present cycle have been actively investigated. In both cases, it turns that the basic knowledge underlying these methods is either missing or incomplete. This situation opens a window of opportunity for useful contributions from basic nuclear physicists. This article describes some of them and presents the ongoing activities as well as some of the projects put forth for the short or medium term. .

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

Nordborg, C.

A new improved version of the OECD Nuclear Energy Agency (NEA) co-ordinated Joint Evaluated Fission and Fusion (JEFF) data library, JEFF-3.1, was released in May 2005. It comprises a general purpose library and the following five special purpose libraries: activation; thermal scattering law; radioactive decay; fission yield; and proton library. The objective of the previous version of the library (JEFF-2.2) was to achieve improved performance for existing reactors and fuel cycles. In addition to this objective, the JEFF-3.1 library aims to provide users with data for a wider range of applications. These include innovative reactor concepts, transmutation of radioactive waste,more » fusion, and various other energy and non-energy related industrial applications. Initial benchmark testing has confirmed the expected very good performance of the JEFF-3.1 library. Additional benchmarking of the libraries is underway, both for the general purpose and for the special purpose libraries. A new three-year mandate to continue developing the JEFF library was recently granted by the NEA. For the next version of the library, JEFF-3.2, it is foreseen to put more effort into fission product and minor actinide evaluations, as well as the inclusion of more covariance data. (authors)« less

Recent developments in the French programme for radioactive waste management planning Act of 28 june 2006

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

Ouzounian, G.

2007-07-01

In 2005, new developments on radioactive-waste management in France were marked mostly by the preparation of the 2006 milestone specified in the act of 30 December 1991. A bill on radioactive waste management has been prepared by the Government at the beginning of 2006 and passed to the French Parliament on 15 June 2006. The Planning Act on the sustainable management of radioactive materials and wastes has been drawn from the results of the 15 years of research performed by ANDRA and the CEA on 'partitioning and transmutation of long-lived radionuclides', 'deep geological disposal' and 'conditioning and long term interimmore » storage'. Major milestones during those two last years are presented, including reviews of the Dossier 2005, official reports, the Public Debate, and finally the Planning Act. (authors)« less

United States Transuranium and Uranium Registries. Annual report February 1, 2000--January 31, 2001

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

Ehrhart, Susan M.; Filipy, Ronald E.

2001-07-01

The United States Transuranium and Uranium Registries (USTUR) comprise a human tissue research program studying the deposition, biokinetics and dosimetry of the actinide elements in humans with the primary goals of providing data fundamental to the verification, refinement, or future development of radiation protection standards for these and other radionuclides, and of determining possible bioeffects on both a macro and subcellular level attributable to exposure to the actinides. This report covers USTUR activities during the year from February 2000 through January 2001.

United States Transuranium and Uranium Registries. Annual report October 1, 1994 - September 30, 1995

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

Kathren, R.L.; Harwick, L.A.; Markel, M.J.

1996-07-01

The United States Transuranium and Uranium Registries (USTUR) comprise a human tissue research program studying the deposition, biokinetics and dosimetry of the actinide elements in humans with the primary goals of providing data fundamental to the verification, refinement, or future development of radiation protection standards for these and other radionuclides, and of determining possible bioeffects on both a macro and subcellular level attributable to exposure to the actinides. This report covers USTUR activities during the year from October 1994 through September 1995.

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.

Role of (n,2n) reactions in transmutation of long-lived fission products

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

Apse, V. A.; Kulikov, G. G., E-mail: ggkulikov@mephi.ru; Kulikov, E. G.

2016-12-15

The conditions under which (n,γ) and (n,2n) reactions can help or hinder each other in neutron transmutation of long-lived fission products (LLFPs) are considered. Isotopic and elemental transmutation for the main long-lived fission products, {sup 79}Se, {sup 93}Zr, {sup 99}Tc, {sup 107}Pd, {sup 126}Sn, {sup 129}I, and {sup 135}Cs, are considered. The effect of (n,2n) reactions on the equilibrium amount of nuclei of the transmuted isotope and the neutron consumption required for the isotope processing is estimated. The aim of the study is to estimate the influence of (n,2n) reactions on efficiency of neutron LLFP transmutation. The code TIME26 andmore » the libraries of evaluated nuclear data ABBN-93, JEF-PC, and JANIS system are applied. The following results are obtained: (1) The effect of (n,2n) reactions on the minimum number of neutrons required for transmutation and the equilibrium amount of LLFP nuclei is estimated. (2) It is demonstrated that, for three LLFP isotopes ({sup 126}Sn, {sup 129}I, and {sup 135}Cs), (n,γ) and (n,2n) reactions are partners facilitating neutron transmutation. The strongest effect of (n,2n) reaction is found for {sup 126}Sn transmutation (reduction of the neutron consumption by 49% and the equilibrium amount of nuclei by 19%).« less

Transmutation prospect of long-lived nuclear waste induced by high-charge electron beam from laser plasma accelerator

NASA Astrophysics Data System (ADS)

Wang, X. L.; Xu, Z. Y.; Luo, W.; Lu, H. Y.; Zhu, Z. C.; Yan, X. Q.

2017-09-01

Photo-transmutation of long-lived nuclear waste induced by a high-charge relativistic electron beam (e-beam) from a laser plasma accelerator is demonstrated. A collimated relativistic e-beam with a high charge of approximately 100 nC is produced from high-intensity laser interaction with near-critical-density (NCD) plasma. Such e-beam impinges on a high-Z convertor and then radiates energetic bremsstrahlung photons with flux approaching 1011 per laser shot. Taking a long-lived radionuclide 126Sn as an example, the resulting transmutation reaction yield is the order of 109 per laser shot, which is two orders of magnitude higher than obtained from previous studies. It is found that at lower densities, a tightly focused laser irradiating relatively longer NCD plasmas can effectively enhance the transmutation efficiency. Furthermore, the photo-transmutation is generalized by considering mixed-nuclide waste samples, which suggests that the laser-accelerated high-charge e-beam could be an efficient tool to transmute long-lived nuclear waste.

Friction Stir Welding of HT9 Ferritic-Martensitic Steel: An Assessment of Microstructure and Properties

DTIC Science & Technology

2013-06-01

X, where X represents lithium, sodium, beryllium, or transmutation products, such as tritium [47]. In this mechanism, the transmutation of lithium...Similar to the study by Williams, Farmer found that galvanic coupling, increased temperature and the formation of transmutation products (HF and TF), a

An improved transmutation method for quantitative determination of the components in multicomponent overlapping chromatograms.

PubMed

Shao, Xueguang; Yu, Zhengliang; Ma, Chaoxiong

2004-06-01

An improved method is proposed for the quantitative determination of multicomponent overlapping chromatograms based on a known transmutation method. To overcome the main limitation of the transmutation method caused by the oscillation generated in the transmutation process, two techniques--wavelet transform smoothing and the cubic spline interpolation for reducing data points--were adopted, and a new criterion was also developed. By using the proposed algorithm, the oscillation can be suppressed effectively, and quantitative determination of the components in both the simulated and experimental overlapping chromatograms is successfully obtained.

Fast reactor core concepts to improve transmutation efficiency

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

Fujimura, Koji; Kawashima, Katsuyuki; Itooka, Satoshi

Fast Reactor (FR) core concepts to improve transmutation efficiency were conducted. A heterogeneous MA loaded core was designed based on the 1000MWe-ABR breakeven core. The heterogeneous MA loaded core with Zr-H loaded moderated targets had a better transmutation performance than the MA homogeneous loaded core. The annular pellet rod design was proposed as one of the possible design options for the MA target. It was shown that using annular pellet MA rods mitigates the self-shielding effect in the moderated target so as to enhance the transmutation rate.

Unifying relations for scattering amplitudes

NASA Astrophysics Data System (ADS)

Cheung, Clifford; Shen, Chia-Hsien; Wen, Congkao

2018-02-01

We derive new amplitudes relations revealing a hidden unity among a wideranging variety of theories in arbitrary spacetime dimensions. Our results rely on a set of Lorentz invariant differential operators which transmute physical tree-level scattering amplitudes into new ones. By transmuting the amplitudes of gravity coupled to a dilaton and two-form, we generate all the amplitudes of Einstein-Yang-Mills theory, Dirac-Born-Infield theory, special Galileon, nonlinear sigma model, and biadjoint scalar theory. Transmutation also relates amplitudes in string theory and its variants. As a corollary, celebrated aspects of gluon and graviton scattering like color-kinematics duality, the KLT relations, and the CHY construction are inherited traits of the transmuted amplitudes. Transmutation recasts the Adler zero as a trivial consequence of the Weinberg soft theorem and implies new subleading soft theorems for certain scalar theories.

FIRST-PRINCIPLES CALCULATIONS OF INTRINSIC DEFECTS AND Mg TRANSMUTANTS IN 3C-SiC

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

Hu, Shenyang Y.; Setyawan, Wahyu; Van Ginhoven, Renee M.

2013-09-25

Silicon carbide (SiC) possesses many desirable attributes for applications in high-temperature and neutron radiation environments. These attributes include excellent dimensional and thermodynamic stability, low activation, high strength, and high thermal conductivity. Therefore, SiC based materials draw broad attention as structural materials for the first wall (FW) and blanket in fusion power plants. Under the severe high-energy neutron environment of D-T fusion systems, SiC suffers significant transmutation resulting in both gaseous and metallic transmutants. Recent calculations by Sawan, et al. [2] predict that at a fast neutron dose of ~100 dpa, there will be about 0.5 at% Mg generated in SiCmore » through nuclear transmutation. Other transmutation products, including 0.15 at% Al, 0.2 at% Be and 2.2 at% He, also emerge. Formation and migration energies of point defects in 3C-SiC have been widely investigated using density functional theory (DFT). However, the properties of defects associated with transmutants are currently not well understood. Fundamental understanding of where the transmutation products go and how they affect microstructure evolution of SiC composites will help to predict property evolution and performance of SiC-based materials in fusion reactors.« less

Transmutation of a trans-series: the Gross-Witten-Wadia phase transition

NASA Astrophysics Data System (ADS)

Ahmed, Anees; Dunne, Gerald V.

2017-11-01

We study the change in the resurgent asymptotic properties of a trans-series in two parameters, a coupling g 2 and a gauge index N, as a system passes through a large N phase transition, using the universal example of the Gross-Witten-Wadia third-order phase transition in the unitary matrix model. This transition is well-studied in the immediate vicinity of the transition point, where it is characterized by a double-scaling limit Painlevé II equation, and also away from the transition point using the pre-string difference equation. Here we present a complementary analysis of the transition at all coupling and all finite N, in terms of a differential equation, using the explicit Tracy-Widom mapping of the Gross-Witten-Wadia partition function to a solution of a Painlevé III equation. This mapping provides a simple method to generate trans-series expansions in all parameter regimes, and to study their transmutation as the parameters are varied. For example, at any finite N the weak coupling expansion is divergent, with a non-perturbative trans-series completion; on the other hand, the strong coupling expansion is convergent, and yet there is still a non-perturbative trans-series completion. We show how the different instanton terms `condense' at the transition point to match with the double-scaling limit trans-series. We also define a uniform large N strong-coupling expansion (a non-linear analogue of uniform WKB), which is much more precise than the conventional large N expansion through the transition region, and apply it to the evaluation of Wilson loops.

Transmutation Theory in the Greek Alchemical Corpus.

PubMed

Dufault, Olivier

2015-08-01

This paper studies transmutation theory as found in the texts attributed to Zosimus of Panopolis, "the philosopher Synesius," and "the philosopher Olympiodorus of Alexandria." It shows that transmutation theory (i.e. a theory explaining the complete transformation of substances) is mostly absent from the work attributed to these three authors. The text attributed to Synesius describes a gilding process, which is similar to those described by Pliny and Vitruvius. The commentary attributed to Olympiodorus is the only text studied here that describes something similar to a transmutation theory. It is unclear, however, if this was a theory of transmutation or if the writer meant something more like the literal meaning of the word "ekstrophē," a term used to describe the transformation of metals, as the "turning inside-out" of what is hidden in a substance. A similar conception of ekstrophē can be found in the works of Zosimus, who discussed transmutation to make an analogy with self-purification processes, which, from the perspective of his own anthropogony, consisted in the "turning inside-out" of the "inner human" (esō anthrōpos).

Bilingualism, Cultural Transmutation, and Fields of Coexistence: California's Spanish Language Legacy

ERIC Educational Resources Information Center

Garcia, Sara

2006-01-01

This is an historical analysis of English Only programs in California and their impact on bilingualism as a natural acquisition process. Factors that propagate bilingualism such as a continual flow of Spanish speaking immigrants, and social, economic and ethnic isolation, are delineated for theorizing about key aspects of multilingualism, the…

Partitioning problems in parallel, pipelined and distributed computing

NASA Technical Reports Server (NTRS)

Bokhari, S.

1985-01-01

The problem of optimally assigning the modules of a parallel program over the processors of a multiple computer system is addressed. A Sum-Bottleneck path algorithm is developed that permits the efficient solution of many variants of this problem under some constraints on the structure of the partitions. In particular, the following problems are solved optimally for a single-host, multiple satellite system: partitioning multiple chain structured parallel programs, multiple arbitrarily structured serial programs and single tree structured parallel programs. In addition, the problems of partitioning chain structured parallel programs across chain connected systems and across shared memory (or shared bus) systems are also solved under certain constraints. All solutions for parallel programs are equally applicable to pipelined programs. These results extend prior research in this area by explicitly taking concurrency into account and permit the efficient utilization of multiple computer architectures for a wide range of problems of practical interest.

Transmutation studies at CEA in frame of the SPIN program objectives, results and future trends

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

Salvatores, M.; Prunier, C.; Guerin, Y.

1995-10-01

In order to respond to the public concern about wastes and in particular the long-lived high level ones, a French law issued on December 30, 1991 identified the major objectives of research for the next fifteen years, before a new debate and possibly a decision on final wastes disposal in Parliament. These objectives are: (1) improvement of the wastes conditioning; (2) extraction and transmutation of the long-lived wastes in order to minimize their long term toxicity; (3) research performed in underground laboratories in order to characterize the capacity of geological structures to confine radioactive wastes (two sites have to bemore » selected for these underground laboratories, in concertation with the local population); (4) last, the study of conditioning and prolonged surface storage of wastes.« less

Transmutation doping of silicon solar cells

NASA Technical Reports Server (NTRS)

Wood, R. F.; Westbrook, R. D.; Young, R. T.; Cleland, J. W.

1977-01-01

Normal isotopic silicon contains 3.05% of Si-30 which transmutes to P-31 after thermal neutron absorption, with a half-life of 2.6 hours. This reaction is used to introduce extremely uniform concentrations of phosphorus into silicon, thus eliminating the areal and spatial inhomogeneities characteristic of chemical doping. Annealing of the lattice damage in the irradiated silicon does not alter the uniformity of dopant distribution. Transmutation doping also makes it possible to introduce phosphorus into polycrystalline silicon without segregation of the dopant at the grain boundaries. The use of neutron transmutation doped (NTD) silicon in solar cell research and development is discussed.

Modeling Radioactive Decay Chains with Branching Fraction Uncertainties

DTIC Science & Technology

2013-03-01

moments methods with transmutation matrices. Uncertainty from both half-lives and branching fractions is carried through these calculations by Monte...moment methods, method for sampling from normal distributions for half- life uncertainty, and use of transmutation matrices were leveraged. This...distributions for half-life and branching fraction uncertainties, building decay chains and generating the transmutation matrix (T-matrix

On the use of a molten salt fast reactor to apply an idealized transmutation scenario for the nuclear phase out.

PubMed

Merk, Bruno; Rohde, Ulrich; Glivici-Cotruţă, Varvara; Litskevich, Dzianis; Scholl, Susanne

2014-01-01

In the view of transmutation of transuranium (TRU) elements, molten salt fast reactors (MSFRs) offer certain advantages compared to solid fuelled reactor types like sodium cooled fast reactors (SFRs). In the first part these advantages are discussed in comparison with the SFR technology, and the research challenges are analyzed. In the second part cycle studies for the MSFR are given for different configurations--a core with U-238 fertile, a fertile free core, and a core with Th-232 as fertile material. For all cases, the transmutation potential is determined and efficient transmutation performance for the case with thorium as a fertile material as well as for the fertile free case is demonstrated and the individual advantages are discussed. The time evolution of different important isotopes is analyzed. In the third part a strategy for the optimization of the transmutation efficiency is developed. The final aim is dictated by the phase out decision of the German government, which requests to put the focus on the determination of the maximal transmutation efficiency and on an as much as possible reduced leftover of transuranium elements at the end of the reactor life. This minimal leftover is achieved by a two step procedure of a first transmuter operation phase followed by a second deep burning phase. There the U-233, which is bred in the blanket of the core consisting of thorium containing salt, is used as feed. It is demonstrated, that transmutation rates up to more than 90% can be achieved for all transuranium isotopes, while the production of undesired high elements like californium is very limited. Additionally, the adaptations needed for the simulation of a MSFR, and the used tool HELIOS 1.10 is described.

On the Use of a Molten Salt Fast Reactor to Apply an Idealized Transmutation Scenario for the Nuclear Phase Out

PubMed Central

Merk, Bruno; Rohde, Ulrich; Glivici-Cotruţă, Varvara; Litskevich, Dzianis; Scholl, Susanne

2014-01-01

In the view of transmutation of transuranium (TRU) elements, molten salt fast reactors (MSFRs) offer certain advantages compared to solid fuelled reactor types like sodium cooled fast reactors (SFRs). In the first part these advantages are discussed in comparison with the SFR technology, and the research challenges are analyzed. In the second part cycle studies for the MSFR are given for different configurations – a core with U-238 fertile, a fertile free core, and a core with Th-232 as fertile material. For all cases, the transmutation potential is determined and efficient transmutation performance for the case with thorium as a fertile material as well as for the fertile free case is demonstrated and the individual advantages are discussed. The time evolution of different important isotopes is analyzed. In the third part a strategy for the optimization of the transmutation efficiency is developed. The final aim is dictated by the phase out decision of the German government, which requests to put the focus on the determination of the maximal transmutation efficiency and on an as much as possible reduced leftover of transuranium elements at the end of the reactor life. This minimal leftover is achieved by a two step procedure of a first transmuter operation phase followed by a second deep burning phase. There the U-233, which is bred in the blanket of the core consisting of thorium containing salt, is used as feed. It is demonstrated, that transmutation rates up to more than 90% can be achieved for all transuranium isotopes, while the production of undesired high elements like californium is very limited. Additionally, the adaptations needed for the simulation of a MSFR, and the used tool HELIOS 1.10 is described. PMID:24690768

Software Partitioning Schemes for Advanced Simulation Computer Systems. Final Report.

ERIC Educational Resources Information Center

Clymer, S. J.

Conducted to design software partitioning techniques for use by the Air Force to partition a large flight simulator program for optimal execution on alternative configurations, this study resulted in a mathematical model which defines characteristics for an optimal partition, and a manually demonstrated partitioning algorithm design which…

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

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.

Report on the Synchrotron Characterization of U-Mo and U-Zr Alloys and the Modeling Results

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

Okuniewski, Maria A.; Ganapathy, Varsha; Hamilton, Brenden

2016-09-01

ABSTRACT Uranium-molybdenum (U-Mo) and uranium-zirconium (U-Zr) are two promising fuel candidates for nuclear transmutation reactors which burn long-lived minor actinides and fission products within fast spectrum reactors. The objectives of this research are centered on understanding the early stages of fuel performance through the examination of the irradiation induced microstructural changes in U-Zr and U-Mo alloys subjected to low neutron fluences. Specimens that were analyzed include those that were previously irradiated in the Advanced Test Reactor at INL. This most recent work has focused on a sub-set of the irradiated specimens, specifically U-Zr and U-Mo alloys that were irradiated tomore » 0.01 dpa at temperatures ranging from (150-800oC). These specimens were analyzed with two types of synchrotron techniques, including X-ray absorption fine structure and X-ray diffraction. These techniques provide non-destructive microstructural analysis, including phase identification and quantitation, lattice parameters, crystallite sizes, as well as bonding, structure, and chemistry. Preliminary research has shown changes in the phase fractions, crystallite sizes, and lattice parameters as a function of irradiation and temperature. Future data analyses will continue to explore these microstructural changes.« less

Summary report for the FY-2015 SACSESS Collaboration

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

Peterman, Dean Richard; Mincher, Bruce Jay

2015-09-01

During FY-2015, a collaborative research program was established by the Department of Energy-Nuclear Energy (DOE-NE) Material Recovery and Waste Form Development program and the European Union (EU) Safety of Actinide Separation Processes (SACSESS) program. One component of this collaboration was the evaluation of the radiolytic stability of a Selective ActiNide Extraction (SANEX) separation which utilized a TODGA-based organic solvent and an aqueous phase containing the hydrophilic complexing reagent, SO3-Ph-BTP. To best simulate process conditions, this experiment was irradiated in the radiolysis/hydrolysis test loop located at the Idaho National Laboratory. The effect of irradiation on a SACSESS program iSANEX formulation containingmore » a TODGA-based organic phase and a BTP-based aqueous phase was investigated using irradiations at INL in static and test loop modes. When irradiated in contact with only the acidic aqueous phase, the TODGA organic solution maintained excellent extraction performance of americium, cerium and europium to a maximum absorbed dose of nearly 0.9 MGy. When the aqueous phase was changed to that containing the aqueous soluble BTP, the irradiated aqueous phase showed a dramatic color change, but this does not appear to have adverse effects on solvent extraction performance. Only minor increases in distribution ratios for both the lanthanides and actinide were measured, and the separation factors were essentially unchanged to a maximum absorbed dose of 174 kGy. The determination of the americium, cerium, and europium distribution ratios for the remaining SACSESS test loop samples will be completed in the near future. The analysis of stable metals concentration in the the irradiated aqueous and organic phases will be completed shortly.« less

Experimental demonstration of free-space optical vortex transmutation with polygonal lenses.

PubMed

Gao, Nan; Xie, Changqing

2012-08-01

Vortex transmutation was predicted to take place when vortices interact with systems possessing discrete rotational symmetries of finite order [Phys. Rev. Lett.95, 123901 (2005)]. Here we report what is believed to be the first experimental demonstration of vortex transmutation. We show that in free space, by simply inserting polygonal lenses into the optical path, the central vorticity of a coaxially incident optical vortex can be changed following the modular transmutation rule. We generate the wavefront at the exit face of the lenses with computer generated holograms and measure the output vorticity using the interference patterns at the focal plane. The results agree well with theoretical predictions.

Infrared absorption study of neutron-transmutation-doped germanium

NASA Technical Reports Server (NTRS)

Park, I. S.; Haller, E. E.

1988-01-01

Using high-resolution far-infrared Fourier transform absorption spectroscopy and Hall effect measurements, the evolution of the shallow acceptor and donor impurity levels in germanium during and after the neutron transmutation doping process was studied. The results show unambiguously that the gallium acceptor level concentration equals the concentration of transmutated Ge-70 atoms during the whole process indicating that neither recoil during transmutation nor gallium-defect complex formation play significant roles. The arsenic donor levels appear at full concentration only after annealing for 1 h at 450 C. It is shown that this is due to donor-radiation-defect complex formation. Again, recoil does not play a significant role.

Method to Reduce Long-lived Fission Products by Nuclear Transmutations with Fast Spectrum Reactors.

PubMed

Chiba, Satoshi; Wakabayashi, Toshio; Tachi, Yoshiaki; Takaki, Naoyuki; Terashima, Atsunori; Okumura, Shin; Yoshida, Tadashi

2017-10-24

Transmutation of long-lived fission products (LLFPs: 79 Se, 93 Zr, 99 Tc, 107 Pd, 129 I, and 135 Cs) into short-lived or non-radioactive nuclides by fast neutron spectrum reactors without isotope separation has been proposed as a solution to the problem of radioactive wastes disposal. Despite investigation of many methods, such transmutation remains technologically difficult. To establish an effective and efficient transmutation system, we propose a novel neutron moderator material, yttrium deuteride (YD 2 ), to soften the neutron spectrum leaking from the reactor core. Neutron energy spectra and effective half-lives of LLFPs, transmutation rates, and support ratios were evaluated with the continuous-energy Monte Carlo code MVP-II/MVP-BURN and the JENDL-4.0 cross section library. With the YD 2 moderator in the radial blanket and shield regions, effective half-lives drastically decreased from 106 to 102 years and the support ratios reached 1.0 for all six LLFPs. This successful development and implementation of a transmutation system for LLFPs without isotope separation contributes to a the ability of fast spectrum reactors to reduce radioactive waste by consuming their own LLFPs.

A flowsheet concept for an Am/Ln separation based on Am{sup VI} solvent extraction

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

Mincher, B.J.; Law, J.D.

2013-07-01

The separation of Am from the lanthanides and curium is a key step in proposed advanced fuel cycle scenarios. The partitioning and transmutation of Am is desirable to minimize the long-term radiotoxicity of material interred in a future high-level waste repository. However, a separation amenable to process scale-up remains elusive. Higher oxidation states of americium have recently been used to demonstrate solvent extraction-based separations using conventional fuel cycle ligands. Here, the successful partitioning of Am{sup VI} from the bulk of lanthanides and curium using diamyl-amyl-phosphonate (DAAP) extraction is reported. Due to the instability of Am{sup VI} in the organic phasemore » it was readily selectively stripped to a new acidic aqueous phase to provide separation from co-extracted Ce{sup IV}. The use of NaBiO{sub 3} as an oxidant to separate Am from the lanthanides and Cm by solvent extraction has been successfully demonstrated on the bench scale. Based on these results, flowsheet concepts can be designed that result in 96 % Am recovery in the presence of a few percent of the remaining Cm and the lanthanides in two extraction contacts. Preliminary results also indicate that the DAAP extractant is robust toward γ- irradiation under realistic conditions of acidity and dissolved oxygen concentration.« 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.

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

Automatic data partitioning on distributed memory multicomputers. Ph.D. Thesis

NASA Technical Reports Server (NTRS)

Gupta, Manish

1992-01-01

Distributed-memory parallel computers are increasingly being used to provide high levels of performance for scientific applications. Unfortunately, such machines are not very easy to program. A number of research efforts seek to alleviate this problem by developing compilers that take over the task of generating communication. The communication overheads and the extent of parallelism exploited in the resulting target program are determined largely by the manner in which data is partitioned across different processors of the machine. Most of the compilers provide no assistance to the programmer in the crucial task of determining a good data partitioning scheme. A novel approach is presented, the constraints-based approach, to the problem of automatic data partitioning for numeric programs. In this approach, the compiler identifies some desirable requirements on the distribution of various arrays being referenced in each statement, based on performance considerations. These desirable requirements are referred to as constraints. For each constraint, the compiler determines a quality measure that captures its importance with respect to the performance of the program. The quality measure is obtained through static performance estimation, without actually generating the target data-parallel program with explicit communication. Each data distribution decision is taken by combining all the relevant constraints. The compiler attempts to resolve any conflicts between constraints such that the overall execution time of the parallel program is minimized. This approach has been implemented as part of a compiler called Paradigm, that accepts Fortran 77 programs, and specifies the partitioning scheme to be used for each array in the program. We have obtained results on some programs taken from the Linpack and Eispack libraries, and the Perfect Benchmarks. These results are quite promising, and demonstrate the feasibility of automatic data partitioning for a significant class of scientific application programs with regular computations.

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.

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.

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.

Radioactive Waste Management - It's Role in contributing and achieving Sustainability. R1.13 The French strategy of waste management: technical and political dimensions of sustainability

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

Bazile, F.

2007-07-01

The sustainability of an energy policy depends on the manner in which it satisfies environmental, economical and social requirements. Nuclear energy is not an exception. The objectives of the future nuclear systems, as defined in the Generation IV International Forum, tend to optimize the ability of nuclear energy to satisfy sustainable development goals. In this regard, they involve strong commitments concerning waste management policy : five designs in six are based on a closed fuel cycle, in order to minimize the volume and radiotoxicity of final waste, and to recycle the fissile materials to save natural resources. Since its beginnings,more » the French civil nuclear programme has considered a long-term perspective and has developed spent fuel reprocessing. The French current industrial technology has already permitted to recycle 96% of spent fuel materials, to save 30% of natural resources, to reduce by 5 the amount of waste and to reduce by 10 the waste radiotoxicity, all these benefits for less than 6% of the kWh total cost. This strategy has always been criticized by the nuclear opponents, precisely because they saw that it was a sustainable way, and didn't accept to consider nuclear energy as a sustainable source of power. Two arguments were put forward these criticisms. First, the cost of reprocessing versus once-through cycle and second, the risk of proliferation induced by U-Pu partitioning process. These arguments were also invoked in international debates, and they have also been pleaded by the anti-nukes during the National Debate on HLLLW, at the end of 2005, preceding the vote of a new law in 2006 by the French parliament. Fortunately they have not convinced public opinion in France nor political decision-makers. A majority of people with no regard to technical background understand that recycling and saving the natural resources are sustainable principles. And, from a technical point of view, the 6% over cost does not seem significant considering the economics of nuclear power. Lastly, the risk proliferation is more related to the front-end technologies than to the back-end ones. So, the 2006 French Law 'for a sustainable radioactive waste management' has reinforced the closed-cycle strategy and has paved the way for a long-term development of nuclear energy in the 21. century and beyond, towards the third and fourth generations of nuclear systems. It has defined an R and D programme including the continuation of partitioning-transmutation of minor actinides and their recycling in 4. generation fast reactors. In parallel, the French president has committed the French Atomic Energy Commission to implement a 4. generation prototype reactor by 2020, with international cooperation, to guarantee the permanence of technology progress. In this regard, the waste management strategy can't be built without taking into account the perspectives of development of nuclear energy. These perspectives must include the best available technologies and, in the other hand, an adaptation to the political evolutions of societies. (authors)« 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)

Efficient iteration in data-parallel programs with irregular and dynamically distributed data structures

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

Littlefield, R.J.

1990-02-01

To implement an efficient data-parallel program on a non-shared memory MIMD multicomputer, data and computations must be properly partitioned to achieve good load balance and locality of reference. Programs with irregular data reference patterns often require irregular partitions. Although good partitions may be easy to determine, they can be difficult or impossible to implement in programming languages that provide only regular data distributions, such as blocked or cyclic arrays. We are developing Onyx, a programming system that provides a shared memory model of distributed data structures and extends the concept of data distribution to include irregular and dynamic distributions. Thismore » provides a powerful means to specify irregular partitions. Perhaps surprisingly, programs using it can also execute efficiently. In this paper, we describe and evaluate the Onyx implementation of a model problem that repeatedly executes an irregular but fixed data reference pattern. On an NCUBE hypercube, the speed of the Onyx implementation is comparable to that of carefully handwritten message-passing code.« less

Reliability assessment of MVP-BURN and JENDL-4.0 related to nuclear transmutation of light platinum group elements

NASA Astrophysics Data System (ADS)

Terashima, Atsunori; Nilsson, Mikael; Ozawa, Masaki; Chiba, Satoshi

2017-09-01

The Aprés ORIENT research program, as a concept of advanced nuclear fuel cycle, was initiated in FY2011 aiming at creating stable, highly-valuable elements by nuclear transmutation from ↓ssion products. In order to simulate creation of such elements by (n, γ) reaction succeeded by β- decay in reactors, a continuous-energy Monte Carlo burnup calculation code MVP-BURN was employed. Then, it is one of the most important tasks to con↓rm the reliability of MVP-BURN code and evaluated neutron cross section library. In this study, both an experiment of neutron activation analysis in TRIGA Mark I reactor at University of California, Irvine and the corresponding burnup calculation using MVP-BURN code were performed for validation of the simulation on transmutation of light platinum group elements. Especially, some neutron capture reactions such as 102Ru(n, γ)103Ru, 104Ru(n, γ)105Ru, and 108Pd(n, γ)109Pd were dealt with in this study. From a comparison between the calculation (C) and the experiment (E) about 102Ru(n, γ)103Ru, the deviation (C/E-1) was signi↓cantly large. Then, it is strongly suspected that not MVP-BURN code but the neutron capture cross section of 102Ru belonging to JENDL-4.0 used in this simulation have made the big di↑erence as (C/E-1) >20%.

Neutron transport-burnup code MCORGS and its application in fusion fission hybrid blanket conceptual research

NASA Astrophysics Data System (ADS)

Shi, Xue-Ming; Peng, Xian-Jue

2016-09-01

Fusion science and technology has made progress in the last decades. However, commercialization of fusion reactors still faces challenges relating to higher fusion energy gain, irradiation-resistant material, and tritium self-sufficiency. Fusion Fission Hybrid Reactors (FFHR) can be introduced to accelerate the early application of fusion energy. Traditionally, FFHRs have been classified as either breeders or transmuters. Both need partition of plutonium from spent fuel, which will pose nuclear proliferation risks. A conceptual design of a Fusion Fission Hybrid Reactor for Energy (FFHR-E), which can make full use of natural uranium with lower nuclear proliferation risk, is presented. The fusion core parameters are similar to those of the International Thermonuclear Experimental Reactor. An alloy of natural uranium and zirconium is adopted in the fission blanket, which is cooled by light water. In order to model blanket burnup problems, a linkage code MCORGS, which couples MCNP4B and ORIGEN-S, is developed and validated through several typical benchmarks. The average blanket energy Multiplication and Tritium Breeding Ratio can be maintained at 10 and 1.15 respectively over tens of years of continuous irradiation. If simple reprocessing without separation of plutonium from uranium is adopted every few years, FFHR-E can achieve better neutronic performance. MCORGS has also been used to analyze the ultra-deep burnup model of Laser Inertial Confinement Fusion Fission Energy (LIFE) from LLNL, and a new blanket design that uses Pb instead of Be as the neutron multiplier is proposed. In addition, MCORGS has been used to simulate the fluid transmuter model of the In-Zinerater from Sandia. A brief comparison of LIFE, In-Zinerater, and FFHR-E will be given.

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.

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

Potential energy surfaces of Polonium isotopes

NASA Astrophysics Data System (ADS)

Nerlo-Pomorska, B.; Pomorski, K.; Schmitt, C.; Bartel, J.

2015-11-01

The evolution of the potential energy landscape is analysed in detail for ten even-even polonium isotopes in the mass range 188\\lt A\\lt 220 as obtained within the macroscopic-microscopic approach, relying on the Lublin-Strasbourg drop model and the Yukawa-folded single-particle energies for calculating the microscopic shell and pairing corrections. A variant of the modified Funny-Hills nuclear shape parametrization is used to efficiently map possible fission paths. The approach explains the main features of the fragment partition as measured in low-energy fission along the polonium chain. The latter lies in a transitional region of the nuclear chart, and will be essential to consistently understand the evolution of fission properties from neutron-deficient mercury to heavy actinides. The ability of our method to predict fission observables over such an extended region looks promising.

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.

Transmutation of planar media singularities in a conformal cloak.

PubMed

Liu, Yichao; Mukhtar, Musawwadah; Ma, Yungui; Ong, C K

2013-11-01

Invisibility cloaking based on optical transformation involves materials singularity at the branch cut points. Many interesting optical devices, such as the Eaton lens, also require planar media index singularities in their implementation. We show a method to transmute two singularities simultaneously into harmless topological defects formed by anisotropic permittivity and permeability tensors. Numerical simulation is performed to verify the functionality of the transmuted conformal cloak consisting of two kissing Maxwell fish eyes.

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

Efficient partitioning and assignment on programs for multiprocessor execution

NASA Technical Reports Server (NTRS)

Standley, Hilda M.

1993-01-01

The general problem studied is that of segmenting or partitioning programs for distribution across a multiprocessor system. Efficient partitioning and the assignment of program elements are of great importance since the time consumed in this overhead activity may easily dominate the computation, effectively eliminating any gains made by the use of the parallelism. In this study, the partitioning of sequentially structured programs (written in FORTRAN) is evaluated. Heuristics, developed for similar applications are examined. Finally, a model for queueing networks with finite queues is developed which may be used to analyze multiprocessor system architectures with a shared memory approach to the problem of partitioning. The properties of sequentially written programs form obstacles to large scale (at the procedure or subroutine level) parallelization. Data dependencies of even the minutest nature, reflecting the sequential development of the program, severely limit parallelism. The design of heuristic algorithms is tied to the experience gained in the parallel splitting. Parallelism obtained through the physical separation of data has seen some success, especially at the data element level. Data parallelism on a grander scale requires models that accurately reflect the effects of blocking caused by finite queues. A model for the approximation of the performance of finite queueing networks is developed. This model makes use of the decomposition approach combined with the efficiency of product form solutions.

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

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

Developing an in-situ Detector of Neutron-Induced Fission for Actinide Sputtering Characterization

NASA Astrophysics Data System (ADS)

Fellers, Deion

2016-09-01

The physical mechanism describing the transfer of large amounts of energy due to fission in a material is not well understood and represents one of the modern challenges facing nuclear scientists, with applications including nuclear energy and national defense. Fission fragments cause damage to the material from sputtering of matter as they pass through or near the material's surface. We have developed a new technique at the Los Alamos Neutron Science Center for characterizing the ejecta by using ultracold neutrons (neutrons with kinetic energy less than 300 neV) to induce fission at finely controlled depths in an actinide. This program will ultimately provide a detailed description of the properties of the sputtered particles as a function of the depth of the fission in the material. A key component of this project is accurately quantifying the number of neutron induced fissions in the sample. This poster depicts the development of an in-situ detector of neutron-induced fission for the AShES (Actinide Sputtering from ultracold neutron Exposure at the Surface) experiment.

Actinide Solubility and Speciation in the WIPP [PowerPoint

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

Reed, Donald T.

2015-11-02

The presentation begins with the role and need for nuclear repositories (overall concept, international updates (Sweden, Finland, France, China), US approach and current status), then moves on to the WIPP TRU repository concept (design, current status--safety incidents of February 5 and 14, 2014, path forward), and finally considers the WIPP safety case: dissolved actinide concentrations (overall approach, oxidation state distribution and redox control, solubility of actinides, colloidal contribution and microbial effects). The following conclusions are set forth: (1) International programs are moving forward, but at a very slow and somewhat sporadic pace. (2) In the United States, the Salt repositorymore » concept, from the perspective of the long-term safety case, remains a viable option for nuclear waste management despite the current operational issues/concerns. (3) Current model/PA prediction (WIPP example) are built on redundant conservatisms. These conservatisms are being addressed in the ongoing and future research to fill existing data gaps--redox control of plutonium by Fe(0, II), thorium (analog) solubility studies in simulated brine, contribution of intrinsic and biocolloids to the mobile concentration, and clarification of microbial ecology and effects.« less

Characterization of Neutron-Induced Defects in Isotopically Enriched Lithium Tetraborate

DTIC Science & Technology

2011-03-01

that efficiently captures and transmutes neutrons into more readily detected forms of material or energy. Neutron detection is desirable to detect...be used to transmute neutrons into a more readily detectable particle or energy. Upon absorbing a thermal neutron, 6Li undergoes the reaction, 6 1...both 6Li and 10B in natural abundances unless deliberately enriched. In addition to the direct reactions, 6Li or 7Li and 16O can transmute neutrons

The Soviet Central Asian Challenge: A Neo-Gramscian Analysis.

DTIC Science & Technology

1986-09-01

transmutated into the Soviet Union. This point is fundamental to understanding why the Russians are the ruling nationality group in the Soviet Union. The Great...initial years, force and coercion were instrumental for ensuring the continued existence of the transmuted Russian Empire. The new Soviet Union also...information on .Muslim national communism s1 l (Reft. 31, i33. 26F1or an excellent article on Russian nationalism’s transmutation to Soviet communism and the

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

Dual neutral particle induced transmutation in CINDER2008

NASA Astrophysics Data System (ADS)

Martin, W. J.; de Oliveira, C. R. E.; Hecht, A. A.

2014-12-01

Although nuclear transmutation methods for fission have existed for decades, the focus has been on neutron-induced reactions. Recent novel concepts have sought to use both neutrons and photons for purposes such as active interrogation of cargo to detect the smuggling of highly enriched uranium, a concept that would require modeling the transmutation caused by both incident particles. As photonuclear transmutation has yet to be modeled alongside neutron-induced transmutation in a production code, new methods need to be developed. The CINDER2008 nuclear transmutation code from Los Alamos National Laboratory is extended from neutron applications to dual neutral particle applications, allowing both neutron- and photon-induced reactions for this modeling with a focus on fission. Following standard reaction modeling, the induced fission reaction is understood as a two-part reaction, with an entrance channel to the excited compound nucleus, and an exit channel from the excited compound nucleus to the fission fragmentation. Because photofission yield data-the exit channel from the compound nucleus-are sparse, neutron fission yield data are used in this work. With a different compound nucleus and excitation, the translation to the excited compound state is modified, as appropriate. A verification and validation of these methods and data has been performed. This has shown that the translation of neutron-induced fission product yield sets, and their use in photonuclear applications, is appropriate, and that the code has been extended correctly.

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

The End of Alchemy? The Repudiation and Persistence of Chrysopoeia at the Académie Royale des Sciences in the Eighteenth Century.

PubMed

Principe, Lawrence M

2014-01-01

The general abandonment of serious endeavor toward metallic transmutation represents a major development in the history of chemistry, yet its exact causes and timing remain unclear. This essay examines the fate of chrysopoeia at the eighteenth-century Académie Royale des Sciences. It reveals a long-standing tension between Académie chemists, who pursued transmutation, and administrators, who tried to suppress it. This tension provides background for Etienne-François Geoffroy's 1722 paper describing fraudulent practices around transmutation. Although transmutation seems to disappear after Geoffroy's paper, manuscripts reveal that most of the institution's chemists continued to pursue it privately until at least the 1760s, long after widely accepted dates for the "demise of alchemy" in learned circles.

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

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.

Transmuted of Rayleigh Distribution with Estimation and Application on Noise Signal

NASA Astrophysics Data System (ADS)

Ahmed, Suhad; Qasim, Zainab

2018-05-01

This paper deals with transforming one parameter Rayleigh distribution, into transmuted probability distribution through introducing a new parameter (λ), since this studied distribution is necessary in representing signal data distribution and failure data model the value of this transmuted parameter |λ| ≤ 1, is also estimated as well as the original parameter (⊖) by methods of moments and maximum likelihood using different sample size (n=25, 50, 75, 100) and comparing the results of estimation by statistical measure (mean square error, MSE).

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

Automatic selection of dynamic data partitioning schemes for distributed memory multicomputers

NASA Technical Reports Server (NTRS)

Palermo, Daniel J.; Banerjee, Prithviraj

1995-01-01

For distributed memory multicomputers such as the Intel Paragon, the IBM SP-2, the NCUBE/2, and the Thinking Machines CM-5, the quality of the data partitioning for a given application is crucial to obtaining high performance. This task has traditionally been the user's responsibility, but in recent years much effort has been directed to automating the selection of data partitioning schemes. Several researchers have proposed systems that are able to produce data distributions that remain in effect for the entire execution of an application. For complex programs, however, such static data distributions may be insufficient to obtain acceptable performance. The selection of distributions that dynamically change over the course of a program's execution adds another dimension to the data partitioning problem. In this paper, we present a technique that can be used to automatically determine which partitionings are most beneficial over specific sections of a program while taking into account the added overhead of performing redistribution. This system is being built as part of the PARADIGM (PARAllelizing compiler for DIstributed memory General-purpose Multicomputers) project at the University of Illinois. The complete system will provide a fully automated means to parallelize programs written in a serial programming model obtaining high performance on a wide range of distributed-memory multicomputers.

Status of plutonium ceramic immobilization processes and immobilization forms

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

Ebbinghaus, B.B.; Van Konynenburg, R.A.; Vance, E.R.

1996-05-01

Immobilization in a ceramic followed by permanent emplacement in a repository or borehole is one of the alternatives currently being considered by the Fissile Materials Disposition Program for the ultimate disposal of excess weapons-grade plutonium. To make Pu recovery more difficult, radioactive cesium may also be incorporated into the immobilization form. Valuable data are already available for ceramics form R&D efforts to immobilize high-level and mixed wastes. Ceramics have a high capacity for actinides, cesium, and some neutron absorbers. A unique characteristic of ceramics is the existence of mineral analogues found in nature that have demonstrated actinide immobilization over geologicmore » time periods. The ceramic form currently being considered for plutonium disposition is a synthetic rock (SYNROC) material composed primarily of zirconolite (CaZrTi{sub 2}O{sub 7}), the desired actinide host phase, with lesser amounts of hollandite (BaAl{sub 2}Ti{sub 6}O{sub 16}) and rutile (TiO{sub 2}). Alternative actinide host phases are also being considered. These include pyrochlore (Gd{sub 2}Ti{sub 2}O{sub 7}), zircon (ZrSiO{sub 4}), and monazite (CePO{sub 4}), to name a few of the most promising. R&D activities to address important technical issues are discussed. Primarily these include moderate scale hot press fabrications with plutonium, direct loading of PuO{sub 2} powder, cold press and sinter fabrication methods, and immobilization form formulation issues.« 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

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

In situ characterization of uranium and americium oxide solid solution formation for CRMP process: first combination of in situ XRD and XANES measurements.

PubMed

Caisso, Marie; Picart, Sébastien; Belin, Renaud C; Lebreton, Florent; Martin, Philippe M; Dardenne, Kathy; Rothe, Jörg; Neuville, Daniel R; Delahaye, Thibaud; Ayral, André

2015-04-14

Transmutation of americium in heterogeneous mode through the use of U1-xAmxO2±δ ceramic pellets, also known as Americium Bearing Blankets (AmBB), has become a major research axis. Nevertheless, in order to consider future large-scale deployment, the processes involved in AmBB fabrication have to minimize fine particle dissemination, due to the presence of americium, which considerably increases the risk of contamination. New synthesis routes avoiding the use of pulverulent precursors are thus currently under development, such as the Calcined Resin Microsphere Pelletization (CRMP) process. It is based on the use of weak-acid resin (WAR) microspheres as precursors, loaded with actinide cations. After two specific calcinations under controlled atmospheres, resin microspheres are converted into oxide microspheres composed of a monophasic U1-xAmxO2±δ phase. Understanding the different mechanisms during thermal conversion, that lead to the release of organic matter and the formation of a solid solution, appear essential. By combining in situ techniques such as XRD and XAS, it has become possible to identify the key temperatures for oxide formation, and the corresponding oxidation states taken by uranium and americium during mineralization. This paper thus presents the first results on the mineralization of (U,Am) loaded resin microspheres into a solid solution, through in situ XAS analysis correlated with HT-XRD.

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

Wieselquist, William A.

SCALE’s general depletion, activation, and spent fuel source terms analysis capabilities are enabled through a family of modules related to the main ORIGEN depletion/irradiation/decay solver. The nuclide tracking in ORIGEN is based on the principle of explicitly modeling all available nuclides and transitions in the current fundamental nuclear data for decay and neutron-induced transmutation and relies on fundamental cross section and decay data in ENDF/B VII. Cross section data for materials and reaction processes not available in ENDF/B-VII are obtained from the JEFF-3.0/A special purpose European activation library containing 774 materials and 23 reaction channels with 12,617 neutron-induced reactions belowmore » 20 MeV. Resonance cross section corrections in the resolved and unresolved range are performed using a continuous-energy treatment by data modules in SCALE. All nuclear decay data, fission product yields, and gamma-ray emission data are developed from ENDF/B-VII.1 evaluations. Decay data include all ground and metastable state nuclides with half-lives greater than 1 millisecond. Using these data sources, ORIGEN currently tracks 174 actinides, 1149 fission products, and 974 activation products. The purpose of this chapter is to describe the stand-alone capabilities and underlying methodology of ORIGEN—as opposed to the integrated depletion capability it provides in all coupled neutron transport/depletion sequences in SCALE, as described in other chapters.« less

Resolving and quantifying overlapped chromatographic bands by transmutation

PubMed

Malinowski

2000-09-15

A new chemometric technique called "transmutation" is developed for the purpose of sharpening overlapped chromatographic bands in order to quantify the components. The "transmutation function" is created from the chromatogram of the pure component of interest, obtained from the same instrument, operating under the same experimental conditions used to record the unresolved chromatogram of the sample mixture. The method is used to quantify mixtures containing toluene, ethylbenzene, m-xylene, naphthalene, and biphenyl from unresolved chromatograms previously reported. The results are compared to those obtained using window factor analysis, rank annihilation factor analysis, and matrix regression analysis. Unlike the latter methods, the transmutation method is not restricted to two-dimensional arrays of data, such as those obtained from HPLC/DAD, but is also applicable to chromatograms obtained from single detector experiments. Limitations of the method are discussed.

Next generation fuel irradiation capability in the High Flux Reactor Petten

NASA Astrophysics Data System (ADS)

Fütterer, Michael A.; D'Agata, Elio; Laurie, Mathias; Marmier, Alain; Scaffidi-Argentina, Francesco; Raison, Philippe; Bakker, Klaas; de Groot, Sander; Klaassen, Frodo

2009-07-01

This paper describes selected equipment and expertise on fuel irradiation testing at the High Flux Reactor (HFR) in Petten, The Netherlands. The reactor went critical in 1961 and holds an operating license up to at least 2015. While HFR has initially focused on Light Water Reactor fuel and materials, it also played a decisive role since the 1970s in the German High Temperature Reactor (HTR) development program. A variety of tests related to fast reactor development in Europe were carried out for next generation fuel and materials, in particular for Very High Temperature Reactor (V/HTR) fuel, fuel for closed fuel cycles (U-Pu and Th-U fuel cycle) and transmutation, as well as for other innovative fuel types. The HFR constitutes a significant European infrastructure tool for the development of next generation reactors. Experimental facilities addressed include V/HTR fuel tests, a coated particle irradiation rig, and tests on fast reactor, transmutation and thorium fuel. The rationales for these tests are given, results are provided and further work is outlined.

Study of radioactive impurities in neutron transmutation doped germanium

NASA Astrophysics Data System (ADS)

Mathimalar, S.; Dokania, N.; Singh, V.; Nanal, V.; Pillay, R. G.; Shrivastava, A.; Jagadeesan, K. C.; Thakare, S. V.

2015-02-01

A program to develop low temperature (mK) sensors with neutron transmutation doped Ge for rare event studies with a cryogenic bolometer has been initiated. For this purpose, semiconductor grade Ge wafers are irradiated with thermal neutron flux from Dhruva reactor at Bhabha Atomic Research Centre (BARC), Mumbai. Spectroscopic studies of irradiated samples have revealed that the environment of the capsule used for irradiating the sample leads to significant levels of 65Zn, 110mAg and 182Ta impurities, which can be reduced by chemical etching of approximately 50 μm thick surface layer. From measurements of the etched samples in the low background counting setup, activity due to trace impurities of 123Sb in bulk Ge is estimated to be 1 Bq / g after irradiation. These estimates indicate that in order to use the NTD Ge sensors for rare event studies, a cooldown period of 2 years would be necessary to reduce the radioactive background to ≤ 1 mBq / g.

Aqueous Electrochemical Mechanisms in Actinide Residue Processing

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

Morris, David E.; Burns, Carol J.; Smith, Wayne H.

2000-12-31

Plutonium and uranium residues (e.g., incinerator ash, combustibles, and sand/slag/crucibles) resulting from the purification and processing of nuclear materials constitute an enormous volume of ''lean'' processing waste and represent a significant fraction of the U. S. Department of Energy's (DOE) legacy waste from fifty years of nuclear weapons production activities. Much of this material is presently in storage at sites throughout the DOE weapons production complex (most notably Rocky Flats, Savannah River and Hanford) awaiting further processing and/or final disposition. The chemical and physical stability of much of this material has been called into question recently by the Defense Nuclearmore » Facility Safety Board (DNFSB) and resulted in the issuance of a mandate by the DNFSB to undertake a program to stabilize these materials [1]. The ultimate disposition for much of these materials is anticipated to be geologic repositories such as the proposed Waste Isolation Pilot Plant in New Mexico. However, in light of the mandate to stabilize existing residues and the probable concomitant increase in the volume of material to be disposed as a result of stabilization (e.g., from repackaging at lower residue densities), the projected storage volume for these wastes within anticipated geologic repositories will likely be exceeded simply to handle existing wastes. Additional processing of some of these residue waste streams to reduce radionuclide activity levels, matrix volume, or both is a potentially important strategy to achieve both stabilization and volume reduction so that the anticipated geologic repositories will provide adequate storage volume. In general, the plutonium and uranium that remains in solid residue materials exists in a very stable chemical form (e.g., as binary oxides), and the options available to remove the actinides are limited. However, there have been some demonstrated successes in this vain using aqueous phase electrochemical methods such as the Catalyzed Electrochemical Plutonium Oxide Dissolution (CEPOD) process pioneered by workers at Pacific Northwest National Laboratory in the mid-1970s [2]. The basis for most of these mediated electrochemical oxidation/reduction (MEO/R) processes is the generation of a dissolved electrochemical catalyst, such as Ag2+, which is capable of oxidizing or reducing solid-phase actinide species or actinide sorbates via 7 heterogeneous electron transfer to oxidation states that have significantly greater solubilities (e.g., PuO2(s) to PuO2 2+ (dissolved)). The solubilized actinide can then be recovered by ion exchange or other mechanisms. These aqueous electrochemical methods for residue treatment have been considered in many of the ''trade studies'' to evaluate options for stabilization of the various categories of residue materials. While some concerns generally arise (e.g., large secondary waste volumes could results since the process stream normally goes th rough anion exchange or precipitation steps to remove the actinide), the real utility and versatility of these methods should not be overlooked. They are low temperature, ambient pressure processes that operate in a non-corrosive environment. In principle, they can be designed to be highly selective for the actinides (i.e., no substrate degradation occurs), they can be utilized for many categories of residue materials with little or no modification in hardware or operating conditions, and they can conceivably be engineered to minimize secondary waste stream volume. However, some fundamental questions remain concerning the mechanisms through which these processes act, and how the processes might be optimized to maximize efficiency while minimizing secondary waste. In addition, given the success achieved to date on the limited set of residues, further research is merited to extend the range of applicability of these electrochemical methods to other residue and waste streams. The principal goal of the work described here is to develop a fundamental understanding of the heterogeneous electron transfer thermodynamics and kinetics that lie at the heart of the MEO/R processes for actinide solids and actinide species entrained in or surface-bound to residue substrates. This has been accomplished as described in detail below through spectroscopic characterization of actinide-bearing substrates and electrochemical investigations of electron transfer reactions between uranium- and plutonium- (or surrogates) bearing solids (dispersed actinide solid phases and actinides sorbed to inorganic and organic colloids) and polarizable electrode materials. In general, the actinide solids or substrate-supported species were chosen to represent relevant residue materials (e.g., incinerator ash, sand/slag/crucible, and combustibles).« 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

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

Measurement of dielectric constant of organic solvents by indigenously developed dielectric probe

NASA Astrophysics Data System (ADS)

Keshari, Ajay Kumar; Rao, J. Prabhakar; Rao, C. V. S. Brahmmananda; Ramakrishnan, R.; Ramanarayanan, R. R.

2018-04-01

The extraction, separation and purification of actinides (uranium and plutonium) from various matrices are an important step in nuclear fuel cycle. One of the separation process adopted in an industrial scale is the liquid-liquid extraction or solvent extraction. Liquid-liquid extraction uses a specific ligand/extractant in conjunction with suitable diluent. Solvent extraction or liquid-liquid extraction, involves the partitioning of the solute between two immiscible phases. In most cases, one of the phases is aqueous, and the other one is an organic solvent. The solvent used in solvent extraction should be selective for the metal of interest, it should have optimum distribution ratio, and the loaded metal from the organic phase should be easily stripped under suitable experimental conditions. Some of the important physical properties which are important for the solvent are density, viscosity, phase separation time, interfacial surface tension and the polarity of the extractant.

Transmutation: The Roots of the Dream.

ERIC Educational Resources Information Center

Karpenko, Vladimir

1995-01-01

Examines the history of alchemical attempts at transmutation and classifies them by differing approaches and techniques. Traces the development of alchemy in Asia, Europe, and the Middle East, and compares alchemy with craftsmanship. (18 references) (DDR)

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

Exploring actinide materials through synchrotron radiation techniques.

PubMed

Shi, Wei-Qun; Yuan, Li-Yong; Wang, Cong-Zhi; Wang, Lin; Mei, Lei; Xiao, Cheng-Liang; Zhang, Li; Li, Zi-Jie; Zhao, Yu-Liang; Chai, Zhi-Fang

2014-12-10

Synchrotron radiation (SR) based techniques have been utilized with increasing frequency in the past decade to explore the brilliant and challenging sciences of actinide-based materials. This trend is partially driven by the basic needs for multi-scale actinide speciation and bonding information and also the realistic needs for nuclear energy research. In this review, recent research progresses on actinide related materials by means of various SR techniques were selectively highlighted and summarized, with the emphasis on X-ray absorption spectroscopy, X-ray diffraction and scattering spectroscopy, which are powerful tools to characterize actinide materials. In addition, advanced SR techniques for exploring future advanced nuclear fuel cycles dealing with actinides are illustrated as well. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

Sample results from the integrated salt disposition program macrobatch 6 tank 21H qualifications MST solids sample

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

Peters, T. B.

2013-02-26

Savannah River National Laboratory (SRNL) performed experiments on qualification material for use in the Integrated Salt Disposition Program (ISDP) Batch 6 processing. As part of this qualification work, SRNL performed an Actinide Removal Process (ARP) test. From this test, the residual monosodium titanate (MST) was analyzed for radionuclide uptake. The results of these analyses are reported and are within historical precedent.

Electronic Transmutation (ET): Chemically Turning One Element into Another.

PubMed

Zhang, Xinxing; Lundell, Katie A; Olson, Jared K; Bowen, Kit H; Boldyrev, Alexander I

2018-03-08

The concept of electronic transmutation (ET) depicts the processes that by acquiring an extra electron, an element with the atomic number Z begins to have properties that were known to only belong to its neighboring element with the atomic number Z+1. Based on ET, signature compounds and chemical bonds that are composed of certain elements can now be designed and formed by other electronically transmutated elements. This Minireview summarizes the recent developments and applications of ET on both the theoretical and experimental fronts. Examples on the ET of Group 13 elements into Group 14 elements, Group 14 elements into Group 15 elements, and Group 15 elements into Group 16 elements are discussed. Compounds and chemical bonding composed of carbon, silicon, germanium, phosphorous, oxygen and sulfur now have analogues using transmutated boron, aluminum, gallium, silicon, nitrogen, and phosphorous. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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)

The Potential of the LFR and the ELSY Project

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

Cinotti, L; Smith, C F; Sienicki, J J

2007-03-12

This paper presents the current status of the development of the Lead-cooled Fast Reactor (LFR) in support of Generation IV (GEN IV) Nuclear Energy Systems. The approach being taken by the GIF plan is to address the research priorities of each member state in developing an integrated and coordinated research program to achieve common objectives, while avoiding duplication of effort. The integrated plan being prepared by the LFR Provisional System Steering Committee of the GIF, known as the LFR System research Plan (SRP) recognizes two principal technology tracks for pursuit of LFR technology: (1) a small, transportable system of 10-100more » MWe size that features a very long refueling interval, (2) a larger-sized system rated at about 600 MWe, intended for central station power generation and waste transmutation. This paper, in particular, describes the ongoing activities to develop the Small Secure Transportable Autonomous Reactor (SSTAR) and the European Lead-cooled SYstem (ELSY), the two research initiatives closely aligned with the overall tracks of the SRP and outlines the Proliferation-resistant Environment-friendly Accident-tolerant Continual & Economical Reactors (PEACER) conceived with particular focus on burning/transmuting of long-living TRU waste and fission fragments of concern, such as Tc and I. The current reference design for the SSTAR is a 20 MWe natural circulation pool-type reactor concept with a small shippable reactor vessel. Specific features of the lead coolant, the nitride fuel containing transuranics, the fast spectrum core, and the small size combine to promote a unique approach to achieve proliferation resistance, while also enabling fissile self-sufficiency, autonomous load following, simplicity of operation, reliability, transportability, as well as a high degree of passive safety. Conversion of the core thermal power into electricity at a high plant efficiency of 44% is accomplished utilizing a supercritical carbon dioxide Brayton cycle power converter. The ELSY reference design is a 600 MWe pool-type reactor cooled by pure lead. This concept has been under development since September 2006, and is sponsored by the Sixth Framework Programme of EURATOM. The ELSY project is being performed by a consortium consisting of twenty organizations including seventeen from Europe, two from Korea and one from the USA. ELSY aims to demonstrate the possibility of designing a competitive and safe fast critical reactor using simple engineered technical features while fully complying with the Generation IV goal of minor actinide (MA) burning capability. The use of a compact and simple primary circuit with the additional objective that all internal components be removable, are among the reactor features intended to assure competitive electric energy generation and long-term investment protection. Simplicity is expected to reduce both the capital cost and the construction time; these are also supported by the compactness of the reactor building (reduced footprint and height). The reduced footprint would be possible due to the elimination of the Intermediate Cooling System, the reduced elevation the result of the design approach of reduced-height components.« less

SRNL Development of Recovery Processes for Mark-18A Heavy Actinide Targets

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

Allender, Jeffrey S.; Bridges, Nicholas J.; Loftin, Bradley M.

2015-07-14

Savannah River National Laboratory (SRNL) and Oak Ridge National Laboratory (ORNL) are developing plans for the recovery of rare and unique isotopes contained within heavy-actinide target assemblies, specifically the Mark-18A. Mark-18A assemblies were irradiated in Savannah River Site (SRS) reactors in the 1970s under extremely high neutron-flux conditions and produced, virtually, the world's supply of plutonium-244, an isotope of key importance to high-precision actinide measurement and other scientific and nonproliferation uses; and curium highly enriched in heavy isotopes (e.g., curium-246 and curium-248). In 2015 and 2016, SRNL is pursuing tasks that would reduce program risk and budget requirements, including furthermore » characterization of unprocessed targets; engineering studies for the use of the SRNL Shielded Cells Facility (SCF) for recovery; and development of onsite and offsite shipping methods including a replacement for the heavy (70 ton) cask previously used for onsite transfer of irradiated items at SRS. A status update is provided for the characterization, including modeling using the Monte Carlo N-Particle Transport Code (MCNP); direct non-destructive assay measurements; and cask design.« 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.

Impact of minor actinide recycling on sustainable fuel cycle options

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

Heidet, F.; Kim, T. K.; Taiwo, T. A.

The recent Evaluation and Screening study chartered by the U.S. Department of Energy, Office of Nuclear Energy, has identified four fuel cycle options as being the most promising. Among these four options, the two single-stage fuel cycles rely on a fast reactor and are differing in the fact that in one case only uranium and plutonium are recycled while in the other case minor actinides are also recycled. The two other fuel cycles are two-stage and rely on both fast and thermal reactors. They also differ in the fact that in one case only uranium and plutonium are recycled whilemore » in the other case minor actinides are also recycled. The current study assesses the impact of recycling minor actinides on the reactor core design, its performance characteristics, and the characteristics of the recycled material and waste material. The recycling of minor actinides is found not to affect the reactor core performance, as long as the same cycle length, core layout and specific power are being used. One notable difference is that the required transuranics (TRU) content is slightly increased when minor actinides are recycled. The mass flows are mostly unchanged given a same specific power and cycle length. Although the material mass flows and reactor performance characteristics are hardly affected by recycling minor actinides, some differences are observed in the waste characteristics between the two fuel cycles considered. The absence of minor actinides in the waste results in a different buildup of decay products, and in somewhat different behaviors depending on the characteristic and time frame considered. Recycling of minor actinides is found to result in a reduction of the waste characteristics ranging from 10% to 90%. These results are consistent with previous studies in this domain and depending on the time frame considered, packaging conditions, repository site, repository strategy, the differences observed in the waste characteristics could be beneficial and help improve the repository performance. On the other hand, recycling minor actinides also results in an increase of the recycled fuel characteristics and therefore of the charged fuel. The radioactivity is slightly increased while the decay heat and radiotoxicities are very significantly increased. Despite these differences, the characteristics of the fuel at time of discharge remain similar whether minor actinides are recycled or not, with the exception of the inhalation radiotoxicity which is significantly larger with minor actinide recycling. After some cooling the characteristics of the discharged fuel become larger when minor actinides are recycled, potentially affecting the reprocessing plant requirements. Recycling minor actinides has a negative impact on the characteristics of the fresh fuel and will make it more challenging to fabricate fuel containing minor actinides.« less

"Can Simple Metals Be Transmuted into Gold?" Teaching Science through a Historical Approach.

ERIC Educational Resources Information Center

Mamlok, Rachel; Ben-Zvi, Ruth; Menis, Joseph; Penick, John E.

2000-01-01

Describes the development and enactment of a new teaching unit, "Can simple metals be transmuted into gold?", through an historical approach as well as teacher preparation to teach this unit. (Contains 16 references.) (ASK)

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

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.

Method and apparatus for transmutation of atomic nuclei

DOEpatents

Maenchen, John Eric; Ruiz, Carlos Leon

1998-01-01

Insuring a constant supply of radioisotopes is of great importance to medicine and industry. This invention addresses this problem, and helps to solve it by introducing a new apparatus for transmutation of isotopes which enables swift and flexible production on demand.

Application of activation methods on the Dubna experimental transmutation set-ups.

PubMed

Stoulos, S; Fragopoulou, M; Adloff, J C; Debeauvais, M; Brandt, R; Westmeier, W; Krivopustov, M; Sosnin, A; Papastefanou, C; Zamani, M; Manolopoulou, M

2003-02-01

High spallation neutron fluxes were produced by irradiating massive heavy targets with proton beams in the GeV range. The experiments were performed at the Dubna High Energy Laboratory using the nuclotron accelerator. Two different experimental set-ups were used to produce neutron spectra convenient for transmutation of radioactive waste by (n,x) reactions. By a theoretical analysis neutron spectra can be reproduced from activation measurements. Thermal-epithermal and fast-super-fast neutron fluxes were estimated using the 197Au, 238U (n,gamma) and (n,2n) reactions, respectively. Depleted uranium transmutation rates were also studied in both experiments.

Optimal partitioning of random programs across two processors

NASA Technical Reports Server (NTRS)

Nicol, D. M.

1986-01-01

The optimal partitioning of random distributed programs is discussed. It is concluded that the optimal partitioning of a homogeneous random program over a homogeneous distributed system either assigns all modules to a single processor, or distributes the modules as evenly as possible among all processors. The analysis rests heavily on the approximation which equates the expected maximum of a set of independent random variables with the set's maximum expectation. The results are strengthened by providing an approximation-free proof of this result for two processors under general conditions on the module execution time distribution. It is also shown that use of this approximation causes two of the previous central results to be false.

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.

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.

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

Method and apparatus for transmutation of atomic nuclei

DOEpatents

Maenchen, J.E.; Ruiz, C.L.

1998-12-08

Insuring a constant supply of radioisotopes is of great importance to medicine and industry. This invention addresses this problem, and helps to solve it by introducing a new apparatus for transmutation of isotopes which enables swift and flexible production on demand. 9 figs.

Method and apparatus for transmutation of atomic nuclei

DOEpatents

Maenchen, J.E.; Ruiz, C.L.

1998-06-09

Insuring a constant supply of radioisotopes is of great importance to medicine and industry. This invention addresses this problem, and helps to solve it by introducing a new apparatus for transmutation of isotopes which enables swift and flexible production on demand. 9 figs.

Reflection, transmutation, annihilation, and resonance in two-component kink collisions

NASA Astrophysics Data System (ADS)

Alonso-Izquierdo, A.

2018-02-01

In this paper, the study of collisions between kinks arising in the family of MSTB models is addressed. Phenomena such as elastic kink reflection, mutual annihilation, kink-antikink transmutation and inelastic reflection are found and depend on the impact velocity.

Santa Muerte: Threatening the U.S. Homeland

DTIC Science & Technology

2011-03-08

7 Religious Transmutation ...Religious Transmutation Similarly, a small number of anthropologists do not support the notorious claims about Santa Muerte. They believe that...Muerte, it is no wonder that the religion is spreading globally. Random Terror Slave holding, sexual activity with minors, kidnapping, and

Copper doping of ZnO crystals by transmutation of 64Zn to 65Cu: An electron paramagnetic resonance and gamma spectroscopy study

NASA Astrophysics Data System (ADS)

Recker, M. C.; McClory, J. W.; Holston, M. S.; Golden, E. M.; Giles, N. C.; Halliburton, L. E.

2014-06-01

Transmutation of 64Zn to 65Cu has been observed in a ZnO crystal irradiated with neutrons. The crystal was characterized with electron paramagnetic resonance (EPR) before and after the irradiation and with gamma spectroscopy after the irradiation. Major features in the gamma spectrum of the neutron-irradiated crystal included the primary 1115.5 keV gamma ray from the 65Zn decay and the positron annihilation peak at 511 keV. Their presence confirmed the successful transmutation of 64Zn nuclei to 65Cu. Additional direct evidence for transmutation was obtained from the EPR of Cu2+ ions (where 63Cu and 65Cu hyperfine lines are easily resolved). A spectrum from isolated Cu2+ (3d9) ions acquired after the neutron irradiation showed only hyperfine lines from 65Cu nuclei. The absence of 63Cu lines in this Cu2+ spectrum left no doubt that the observed 65Cu signals were due to transmuted 65Cu nuclei created as a result of the neutron irradiation. Small concentrations of copper, in the form of Cu+-H complexes, were inadvertently present in our as-grown ZnO crystal. These Cu+-H complexes are not affected by the neutron irradiation, but they dissociate when a crystal is heated to 900 °C. This behavior allowed EPR to distinguish between the copper initially in the crystal and the copper subsequently produced by the neutron irradiation. In addition to transmutation, a second major effect of the neutron irradiation was the formation of zinc and oxygen vacancies by displacement. These vacancies were observed with EPR.

Method for producing nuclear fuel

DOEpatents

Haas, Paul A.

1983-01-01

Nuclear fuel is made by contacting an aqueous solution containing an actinide salt with an aqueous solution containing ammonium hydroxide, ammonium oxalate, or oxalic acid in an amount that will react with a fraction of the actinide salt to form a precipitate consisting of the hydroxide or oxalate of the actinide. A slurry consisting of the precipitate and solution containing the unreacted actinide salt is formed into drops which are gelled, calcined, and pressed to form pellets.

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.

Specification-based Error Recovery: Theory, Algorithms, and Usability

DTIC Science & Technology

2013-02-01

transmuting the specification to an implementation at run-time and reducing the performance overhead. A suite of techniques and tools were designed...in the specification, thereby transmuting the specification to an implementation at run-time and reducing the perfor- mance overhead. A suite of

Spatial heterogeneity of tungsten transmutation in a fusion device

NASA Astrophysics Data System (ADS)

Gilbert, M. R.; Sublet, J.-Ch.; Dudarev, S. L.

2017-04-01

Accurately quantifying the transmutation rate of tungsten (W) under neutron irradiation is a necessary requirement in the assessment of its performance as an armour material in a fusion power plant. The usual approach of calculating average responses, assuming large, homogenised material volumes, is insufficient to capture the full complexity of the transmutation picture in the context of a realistic fusion power plant design, particularly for rhenium (Re) production from W. Combined neutron transport and inventory simulations for representative spatially heterogeneous high-resolution models of a fusion power plant show that the production rate of Re is strongly influenced by the surrounding local spatial environment. Localised variation in neutron moderation (slowing down) due to structural steel and coolant, particularly water, can dramatically increase Re production because of the huge cross sections of giant resolved resonances in the neutron-capture reaction of 186W at low neutron energies. Calculations using cross section data corrected for temperature (Doppler) effects suggest that temperature may have a relatively lesser influence on transmutation rates.

Exploring Chemical Space with the Alchemical Derivatives.

PubMed

Balawender, Robert; Welearegay, Meressa A; Lesiuk, Michał; De Proft, Frank; Geerlings, Paul

2013-12-10

In this paper, we verify the usefulness of the alchemical derivatives in the prediction of chemical properties. We concentrate on the stability of the transmutation products, where the term "transmutation" means the change of the nuclear charge at an atomic site at constant number of electrons. As illustrative transmutations showing the potential of the method in exploring chemical space, we present some examples of increasing complexity starting with the deprotonation, continuing with the transmutation of the nitrogen molecule, and ending with the substitution of isoelectronic B-N units for C-C units and N units for C-H units in carbocyclic systems. The basis set influence on the qualitative and quantitative accuracies of the alchemical predictions was investigated. The alchemical deprotonation energy (from the second order Taylor expansion) correlates well with the vertical deprotonation energy and can be used as a preliminary indicator for the experimental deprotonation energy. The results of calculations for the BN derivatives of benzene and pyrene show that this method has great potential for efficient and accurate scanning of chemical space.

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.

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.

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.

Conjugated Gammadion Chiral Metamaterial with Uniaxial Optical Activity and Negative Refractive Index

DTIC Science & Technology

2011-01-10

in Fig. 4, we discuss a procedure of transmutation from the simple -particle chiral element to the conjugated gammadion chiral metamaterial. The...the transmutation from the simple -particle chiral element to the conjugated gammadion chiral metamaterial. The procedure shows how the magnetic or

A Partitioning and Bounded Variable Algorithm for Linear Programming

ERIC Educational Resources Information Center

Sheskin, Theodore J.

2006-01-01

An interesting new partitioning and bounded variable algorithm (PBVA) is proposed for solving linear programming problems. The PBVA is a variant of the simplex algorithm which uses a modified form of the simplex method followed by the dual simplex method for bounded variables. In contrast to the two-phase method and the big M method, the PBVA does…

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

A beamline systems model for Accelerator-Driven Transmutation Technology (ADTT) facilities

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

Todd, A.M.M.; Paulson, C.C.; Peacock, M.A.

1995-10-01

A beamline systems code, that is being developed for Accelerator-Driven Transmutation Technology (ADTT) facility trade studies, is described. The overall program is a joint Grumman, G.H. Gillespie Associates (GHGA) and Los Alamos National Laboratory effort. The GHGA Accelerator Systems Model (ASM) has been adopted as the framework on which this effort is based. Relevant accelerator and beam transport models from earlier Grumman systems codes are being adapted to this framework. Preliminary physics and engineering models for each ADTT beamline component have been constructed. Examples noted include a Bridge Coupled Drift Tube Linac (BCDTL) and the accelerator thermal system. A decisionmore » has been made to confine the ASM framework principally to beamline modeling, while detailed target/blanket, balance-of-plant and facility costing analysis will be performed externally. An interfacing external balance-of-plant and facility costing model, which will permit the performance of iterative facility trade studies, is under separate development. An ABC (Accelerator Based Conversion) example is used to highlight the present models and capabilities.« less

A beamline systems model for Accelerator-Driven Transmutation Technology (ADTT) facilities

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

Todd, Alan M. M.; Paulson, C. C.; Peacock, M. A.

1995-09-15

A beamline systems code, that is being developed for Accelerator-Driven Transmutation Technology (ADTT) facility trade studies, is described. The overall program is a joint Grumman, G. H. Gillespie Associates (GHGA) and Los Alamos National Laboratory effort. The GHGA Accelerator Systems Model (ASM) has been adopted as the framework on which this effort is based. Relevant accelerator and beam transport models from earlier Grumman systems codes are being adapted to this framework. Preliminary physics and engineering models for each ADTT beamline component have been constructed. Examples noted include a Bridge Coupled Drift Tube Linac (BCDTL) and the accelerator thermal system. Amore » decision has been made to confine the ASM framework principally to beamline modeling, while detailed target/blanket, balance-of-plant and facility costing analysis will be performed externally. An interfacing external balance-of-plant and facility costing model, which will permit the performance of iterative facility trade studies, is under separate development. An ABC (Accelerator Based Conversion) example is used to highlight the present models and capabilities.« less

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.

On-line Monitoring of Actinide Concentrations in Molten Salt Electrolyte

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

Curtis W. Johnson; Mary Lou Dunzik-Gougar; Shelly X. Li

2006-11-01

Pyroprocessing, a treatment method for spent nuclear fuel (SNF), is currently being studied at the Idaho National Laboratory. The key operation of pyroprocessing which takes place in an electrorefiner is the electrochemical separation of actinides from other constituents in spent fuel. Efficient operation of the electrorefiner requires online monitoring of actinide concentrations in the molten salt electrolyte. Square-wave voltammetry (SWV) and normal pulse voltammetry (NPV) are being investigated to assess their applicability to the measurement of actinide concentrations in the electrorefiner.

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.

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

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

An Element-Based Concurrent Partitioner for Unstructured Finite Element Meshes

NASA Technical Reports Server (NTRS)

Ding, Hong Q.; Ferraro, Robert D.

1996-01-01

A concurrent partitioner for partitioning unstructured finite element meshes on distributed memory architectures is developed. The partitioner uses an element-based partitioning strategy. Its main advantage over the more conventional node-based partitioning strategy is its modular programming approach to the development of parallel applications. The partitioner first partitions element centroids using a recursive inertial bisection algorithm. Elements and nodes then migrate according to the partitioned centroids, using a data request communication template for unpredictable incoming messages. Our scalable implementation is contrasted to a non-scalable implementation which is a straightforward parallelization of a sequential partitioner.

Neutron transmutation doped Ge bolometers

NASA Technical Reports Server (NTRS)

Haller, E. E.; Kreysa, E.; Palaio, N. P.; Richards, P. L.; Rodder, M.

1983-01-01

Some conclusions reached are as follow. Neutron Transmutation Doping (NTD) of high quality Ge single crystals provides perfect control of doping concentration and uniformity. The resistivity can be tailored to any given bolometer operating temperature down to 0.1 K and probably lower. The excellent uniformity is advantaged for detector array development.

Nuclear waste disposal utilizing a gaseous core reactor

NASA Technical Reports Server (NTRS)

Paternoster, R. R.

1975-01-01

The feasibility of a gaseous core nuclear reactor designed to produce power to also reduce the national inventories of long-lived reactor waste products through nuclear transmutation was examined. Neutron-induced transmutation of radioactive wastes is shown to be an effective means of shortening the apparent half life.

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.

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

A Robustness Testing Campaign for IMA-SP Partitioning Kernels

NASA Astrophysics Data System (ADS)

Grixti, Stephen; Lopez Trecastro, Jorge; Sammut, Nicholas; Zammit-Mangion, David

2015-09-01

With time and space partitioned architectures becoming increasingly appealing to the European space sector, the dependability of partitioning kernel technology is a key factor to its applicability in European Space Agency projects. This paper explores the potential of the data type fault model, which injects faults through the Application Program Interface, in partitioning kernel robustness testing. This fault injection methodology has been tailored to investigate its relevance in uncovering vulnerabilities within partitioning kernels and potentially contributing towards fault removal campaigns within this domain. This is demonstrated through a robustness testing case study of the XtratuM partitioning kernel for SPARC LEON3 processors. The robustness campaign exposed a number of vulnerabilities in XtratuM, exhibiting the potential benefits of using such a methodology for the robustness assessment of partitioning kernels.

Status of the VEGA Project

NASA Astrophysics Data System (ADS)

Kamanin, D. V.; Alexandrov, A. A.; Alexandrova, I. A.; Kondtatyev, N. A.; Kuznetsova, E. A.; Shvetsov, V. N.; Strekalovsky, A. O.; Strekalovsky, O. V.; Zhuchko, V. E.; Pyatkov, Yu. V.; Jacobs, N.; Malaza, V.

2015-06-01

Motivation and status of the VEGA (Velocity-Energy Guide based Array) project is presented. One armed fission fragments spectrometer with an electrostatic guide system is proposed for installation at the vertical experimental channel of the IBR-2 reactor. Scientific program aimed at investigation of new multi-body decays of actinides, shapeisomeric states in fission fragments and fission modes is reported.

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.

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.

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.

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

Compile-time estimation of communication costs in multicomputers

NASA Technical Reports Server (NTRS)

Gupta, Manish; Banerjee, Prithviraj

1991-01-01

An important problem facing numerous research projects on parallelizing compilers for distributed memory machines is that of automatically determining a suitable data partitioning scheme for a program. Any strategy for automatic data partitioning needs a mechanism for estimating the performance of a program under a given partitioning scheme, the most crucial part of which involves determining the communication costs incurred by the program. A methodology is described for estimating the communication costs at compile-time as functions of the numbers of processors over which various arrays are distributed. A strategy is described along with its theoretical basis, for making program transformations that expose opportunities for combining of messages, leading to considerable savings in the communication costs. For certain loops with regular dependences, the compiler can detect the possibility of pipelining, and thus estimate communication costs more accurately than it could otherwise. These results are of great significance to any parallelization system supporting numeric applications on multicomputers. In particular, they lay down a framework for effective synthesis of communication on multicomputers from sequential program references.

Fusion breeder

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

Moir, R.W.

1982-02-22

The fusion breeder is a fusion reactor designed with special blankets to maximize the transmutation by 14 MeV neutrons of uranium-238 to plutonium or thorium to uranium-233 for use as a fuel for fission reactors. Breeding fissile fuels has not been a goal of the US fusion energy program. This paper suggests it is time for a policy change to make the fusion breeder a goal of the US fusion program and the US nuclear energy program. The purpose of this paper is to suggest this policy change be made and tell why it should be made, and to outlinemore » specific research and development goals so that the fusion breeder will be developed in time to meet fissile fuel needs.« less

Fusion breeder

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

Moir, R.W.

1982-04-20

The fusion breeder is a fusion reactor designed with special blankets to maximize the transmutation by 14 MeV neutrons of uranium-238 to plutonium or thorium to uranium-233 for use as a fuel for fission reactors. Breeding fissile fuels has not been a goal of the US fusion energy program. This paper suggests it is time for a policy change to make the fusion breeder a goal of the US fusion program and the US nuclear energy program. The purpose of this paper is to suggest this policy change be made and tell why it should be made, and to outlinemore » specific research and development goals so that the fusion breeder will be developed in time to meet fissile fuel needs.« 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

Oil-soluble and water-soluble BTPhens and their europium complexes in octanol/water solutions: interface crossing studied by MD and PMF simulations.

PubMed

Benay, G; Wipff, G

2013-01-31

Bistriazinyl-phenantroline "BTPhen" ligands L display the remarkable feature to complex trivalent lanthanide and actinide ions, with a marked selectivity for the latter. We report on molecular dynamics studies of tetrasubstituted X(4)BTPhens: L(4+) (X = (+)Et(3)NCH(2)-), L(4-) (X = (-)SO(3)Ph-), and L(0) (X = CyMe(4)) and their complexes with Eu(III) in binary octanol/water solutions. Changes in free energies upon interface crossing are also calculated for typical solutes by potential of mean force PMF simulations. The ligands and their complexes partition, as expected, to either the aqueous or the oil phase, depending on the "solubilizing" group X. Furthermore, most of them are found to be surface active. The water-soluble L(4+) and L(4-) ligands and their (L)Eu(NO(3))(3) complexes adsorb at the aqueous side of the interface, more with L(4-) than with L(4+). The oil soluble ligand L(0) is not surface active in its endo-endo form but adsorbs on the oil side of the interface in its most polar endo-exo form, as well as in its protonated L(0)H(+) and complexed (L(0))Eu(NO(3))(3) states. Furthermore, comparing PMFs of the Eu(III) complexes with and without nitric acid shows that acidifying the aqueous phase has different effects, depending on the ligand charge. In particular, acid promotes the Eu(III) extraction by L(0) via the (L(0))(2)Eu(NO(3))(2+) complex, as observed experimentally. Overall, the results point to the importance of interfacial adsorption for the liquid-liquid extraction of trivalent lanthanide and actinide cations by BTPhens and analogues.

Generation of Escher Arts with Dual Perception.

PubMed

Lin, Shih-Syun; Morace, Charles C; Lin, Chao-Hung; Hsu, Li-Fong; Lee, Tong-Yee

2018-02-01

Escher transmutation is a graphic art that smoothly transforms one tile pattern into another tile pattern with dual perception. A classic example is the artwork called Sky and Water, in which a compelling figure-ground arrangement is applied to portray the transmutation of a bird in sky and a fish in water. The shape of a bird is progressively deformed and dissolves into the background while the background gradually reveals the shape of a fish. This paper introduces a system to create a variety of Escher-like transmutations, which includes the algorithms for initializing a tile pattern with dual figure-ground arrangement, for searching for the best matched shape of a user-specified motif from a database, and for transforming the content and shapes of tile patterns using a content-aware warping technique. The proposed system, integrating the graphic techniques of tile initialization, shape matching, and shape warping, allows users to create various Escher-like transmutations with minimal user interaction. Experimental results and conducted user studies demonstrate the feasibility and flexibility of the proposed system in Escher art generation.

Shifts in Selective Pressures on Snake Phototransduction Genes Associated with Photoreceptor Transmutation and Dim-Light Ancestry.

PubMed

Schott, Ryan K; Van Nynatten, Alexander; Card, Daren C; Castoe, Todd A; S W Chang, Belinda

2018-06-01

The visual systems of snakes are heavily modified relative to other squamates, a condition often thought to reflect their fossorial origins. Further modifications are seen in caenophidian snakes, where evolutionary transitions between rod and cone photoreceptors, termed photoreceptor transmutations, have occurred in many lineages. Little previous work, however, has focused on the molecular evolutionary underpinnings of these morphological changes. To address this, we sequenced seven snake eye transcriptomes and utilized new whole-genome and targeted capture sequencing data. We used these data to analyze gene loss and shifts in selection pressures in phototransduction genes that may be associated with snake evolutionary origins and photoreceptor transmutation. We identified the surprising loss of rhodopsin kinase (GRK1), despite a low degree of gene loss overall and a lack of relaxed selection early during snake evolution. These results provide some of the first evolutionary genomic corroboration for a dim-light ancestor that lacks strong fossorial adaptations. Our results also indicate that snakes with photoreceptor transmutation experienced significantly different selection pressures from other reptiles. Significant positive selection was found primarily in cone-specific genes, but not rod-specific genes, contrary to our expectations. These results reveal potential molecular adaptations associated with photoreceptor transmutation and also highlight unappreciated functional differences between rod- and cone-specific phototransduction proteins. This intriguing example of snake visual system evolution illustrates how the underlying molecular components of a complex system can be reshaped in response to changing selection pressures.

Preliminary neutronics design of china lead-alloy cooled demonstration reactor (CLEAR-III) for nuclear waste transmutation

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

Chen, Z.; Southwest Science and Technology Univ., No.350 Shushanhu Road, Shushan District, Hefei, Anhui, 230031; Chen, Y.

2012-07-01

China Lead-Alloy cooled Demonstration Reactor (CLEAR-III), which is the concept of lead-bismuth cooled accelerator driven sub-critical reactor for nuclear waste transmutation, was proposed and designed by FDS team in China. In this study, preliminary neutronics design studies have primarily focused on three important performance parameters including Transmutation Support Ratio (TSR), effective multiplication factor and blanket thermal power. The constraint parameters, such as power peaking factor and initial TRU loading, were also considered. In the specific design, uranium-free metallic dispersion fuel of (TRU-Zr)-Zr was used as one of the CLEAR-III fuel types and the ratio between MA and Pu was adjustedmore » to maximize transmutation ratio. In addition, three different fuel zones differing in the TRU fraction of the fuel were respectively employed for this subcritical reactor, and the zone sizes and TRU fractions were determined such that the linear powers of these zones were close to each other. The neutronics calculations and analyses were performed by using Multi-Functional 4D Neutronics Simulation System named VisualBUS and nuclear data library HENDL (Hybrid Evaluated Nuclear Data Library). In the preliminary design, the maximum TSRLLMA was {approx}11 and the blanket thermal power was {approx}1000 MW when the effective multiplication factor was 0.98. The results showed that good performance of transmutation could be achieved based on the subcritical reactor loaded with uranium-free fuel. (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

Utilization of Minor Actinides as a Fuel Component for Ultra-Long Life Bhr Configurations: Designs, Advantages and Limitations

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

Dr. Pavel V. Tsvetkov

2009-05-20

This project assessed the advantages and limitations of using minor actinides as a fuel component to achieve ultra-long life Very High Temperature Reactor (VHTR) configurations. Researchers considered and compared the capabilities of pebble-bed and prismatic core designs with advanced actinide fuels to achieve ultra-long operation without refueling. Since both core designs permit flexibility in component configuration, fuel utilization, and fuel management, it is possible to improve fissile properties of minor actinides by neutron spectrum shifting through configuration adjustments. The project studied advanced actinide fuels, which could reduce the long-term radio-toxicity and heat load of high-level waste sent to a geologicmore » repository and enable recovery of the energy contained in spent fuel. The ultra-long core life autonomous approach may reduce the technical need for additional repositories and is capable to improve marketability of the Generation IV VHTR by allowing worldwide deployment, including remote regions and regions with limited industrial resources. Utilization of minor actinides in nuclear reactors facilitates developments of new fuel cycles towards sustainable nuclear energy scenarios.« less

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

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

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.

Scent Transmutation: A New Way to Teach on Chemical Equilibrium, Distillation, and Dynamic Combinatorial Chemistry

ERIC Educational Resources Information Center

Ji, Qing; El-Hamdi, Nadia S.; Miljanic´, Ognjen S?.

2014-01-01

Esters are volatile and pleasantly smelling compounds, commonly used as food additives. Using Ti(OBu)[subscript 4]-catalyzed acyl exchange, we demonstrate a scent transmutation experiment, in which two fragrant esters swap their acyl and alkoxy substituents and are, during the course of a reactive distillation, quantitatively converted into two…

Statistical transmutation in doped quantum dimer models.

PubMed

Lamas, C A; Ralko, A; Cabra, D C; Poilblanc, D; Pujol, P

2012-07-06

We prove a "statistical transmutation" symmetry of doped quantum dimer models on the square, triangular, and kagome lattices: the energy spectrum is invariant under a simultaneous change of statistics (i.e., bosonic into fermionic or vice versa) of the holes and of the signs of all the dimer resonance loops. This exact transformation enables us to define the duality equivalence between doped quantum dimer Hamiltonians and provides the analytic framework to analyze dynamical statistical transmutations. We investigate numerically the doping of the triangular quantum dimer model with special focus on the topological Z(2) dimer liquid. Doping leads to four (instead of two for the square lattice) inequivalent families of Hamiltonians. Competition between phase separation, superfluidity, supersolidity, and fermionic phases is investigated in the four families.

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

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.

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.

Thorium Fuel Options for Sustained Transuranic Burning in Pressurized Water Reactors - 12381

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

Rahman, Fariz Abdul; Lee, John C.; Franceschini, Fausto

2012-07-01

As described in companion papers, Westinghouse is proposing the adoption of a thorium-based fuel cycle to burn the transuranics (TRU) contained in the current Used Nuclear Fuel (UNF) and transition towards a less radio-toxic high level waste. A combination of both light water reactors (LWR) and fast reactors (FR) is envisaged for the task, with the emphasis initially posed on their TRU burning capability and eventually to their self-sufficiency. Given the many technical challenges and development times related to the deployment of TRU burners fast reactors, an interim solution making best use of the current resources to initiate burning themore » legacy TRU inventory while developing and testing some technologies of later use is desirable. In this perspective, a portion of the LWR fleet can be used to start burning the legacy TRUs using Th-based fuels compatible with the current plants and operational features. This analysis focuses on a typical 4-loop PWR, with 17x17 fuel assembly design and TRUs (or Pu) admixed with Th (similar to U-MOX fuel, but with Th instead of U). Global calculations of the core were represented with unit assembly simulations using the Linear Reactivity Model (LRM). Several assembly configurations have been developed to offer two options that can be attractive during the TRU transmutation campaign: maximization of the TRU transmutation rate and capability for TRU multi-recycling, to extend the option of TRU recycling in LWR until the FR is available. Homogeneous as well as heterogeneous assembly configurations have been developed with various recycling schemes (Pu recycle, TRU recycle, TRU and in-bred U recycle etc.). Oxide as well as nitride fuels have been examined. This enabled an assessment of the potential for burning and multi-recycling TRU in a Th-based fuel PWR to compare against other more typical alternatives (U-MOX and variations thereof). Results will be shown indicating that Th-based PWR fuel is a promising option to multi-recycle and burn TRU in a thermal spectrum, while satisfying top-level operational and safety constraints. Various assembly designs have been proposed to assess the TRU burning potential of Th-based fuel in PWRs. In addition to typical homogeneous loading patterns, heterogeneous configurations exploiting the breeding potential of thorium to enable multiple cycles of TRU irradiation and burning have been devised. The homogeneous assembly design, with all pins featuring TRU in Th, has the benefit of a simple loading pattern and the highest rate of TRU transmutation, but it can be used only for a few cycles due to the rapid rise in the TRU content of the recycled fuel, which challenges reactivity control, safety coefficients and fuel handling. Due to its simple loading pattern, such assembly design can be used as the first step of Th implementation, achieving up to 3 times larger TRU transmutation rate than conventional U-MOX, assuming same fraction of MOX assemblies in the core. As the next step in thorium implementation, heterogeneous assemblies featuring a mixed array of Th-U and Th-U-TRU pins, where the U is in-bred from Th, have been proposed. These designs have the potential to enable burning an external supply of TRU through multiple cycles of irradiation, recovery (via reprocessing) and recycling of the residual actinides at the end of each irradiation cycle. This is achieved thanks to a larger breeding of U from Th in the heterogeneous assemblies, which reduces the TRU supply and thus mitigates the increase in the TRU core inventory for the multi-recycled fuel. While on an individual cycle basis the amount of TRU burned in the heterogeneous assembly is reduced with respect to the homogeneous design, TRU burning rates higher than single-pass U-MOX fuel can still be achieved, with the additional benefits of a multi-cycle transmutation campaign recycling all TRU isotopes. Nitride fuel, due its higher density and U breeding potential, together with its better thermal properties, ideally suits the objectives and constraints of the heterogeneous assemblies. However, significant technological advancements must be made before nitride fuels can be employed in an LWR: its water resistance needs to be improved and a viable technology to enrich N in N-15 must be devised. Moreover, for the nitride heterogeneous configurations examined in this study, the enhancement in TRU burning performance is achieved not only by replacing oxide with nitride fuel, but also by increasing the fuel rod size. This latter modification, allowed by the high thermal conductivity of nitride fuel, leads however to a very tight lattice, which may challenge reactor coolant pumps and assembly hold-down mechanisms, the former through an increase in core pressure drop and the latter through an increase in assembly lift-off forces. To alleviate these issues, while still achieving the large fuel-to-moderator ratios resulting from using tight lattices, wire wraps could be used in place of grid spacers. For tight lattices, typical grid spacers are hard to manufacture and their replacement with wire wraps is known to allow for a pressure drop reduction by at least 2 times. The studies, while certainly very preliminary, provide a starting point to devise an optimum strategy for TRU transmutation in Th-based PWR fuel. The viability of the scheme proposed depends on the timely phasing in of the associated technologies, with proper lead time and to solve the many challenges. These challenges are certainly substantial, and make the current once-through U-based scheme pursued in the US by far a more practical (and cheaper) option. However, when compared to other transmutation schemes, the proposed one has arguably similar challenges and unknowns with potentially bigger rewards. (authors)« less

A Recursive Method for Calculating Certain Partition Functions.

ERIC Educational Resources Information Center

Woodrum, Luther; And Others

1978-01-01

Describes a simple recursive method for calculating the partition function and average energy of a system consisting of N electrons and L energy levels. Also, presents an efficient APL computer program to utilize the recursion relation. (Author/GA)

New Quantum Diffusion Monte Carlo Method for strong field time dependent problems

NASA Astrophysics Data System (ADS)

Kalinski, Matt

2017-04-01

We have recently formulated the Quantum Diffusion Quantum Monte Carlo (QDMC) method for the solution of the time-dependent Schrödinger equation when it is equivalent to the reaction-diffusion system coupled by the highly nonlinear potentials of the type of Shay. Here we formulate a new Time Dependent QDMC method free of the nonlinearities described by the constant stochastic process of the coupled diffusion with transmutation. As before two kinds of diffusing particles (color walkers) are considered but which can further also transmute one into the other. Each of the species undergoes the hypothetical Einstein random walk progression with transmutation. The progressed particles transmute into the particles of the other kind before contributing to or annihilating the other particles density. This fully emulates the Time Dependent Schrödinger equation for any number of quantum particles. The negative sign of the real and the imaginary parts of the wave function is handled by the ``spinor'' densities carrying the sign as the degree of freedom. We apply the method for the exact time-dependent observation of our discovered two-electron Langmuir configurations in the magnetic and circularly polarized fields.

Simulating irradiation hardening in tungsten under fast neutron irradiation including Re production by transmutation

NASA Astrophysics Data System (ADS)

Huang, Chen-Hsi; Gilbert, Mark R.; Marian, Jaime

2018-02-01

Simulations of neutron damage under fusion energy conditions must capture the effects of transmutation, both in terms of accurate chemical inventory buildup as well as the physics of the interactions between transmutation elements and irradiation defect clusters. In this work, we integrate neutronics, primary damage calculations, molecular dynamics results, Re transmutation calculations, and stochastic cluster dynamics simulations to study neutron damage in single-crystal tungsten to mimic divertor materials. To gauge the accuracy and validity of the simulations, we first study the material response under experimental conditions at the JOYO fast reactor in Japan and the High Flux Isotope Reactor at Oak Ridge National Laboratory, for which measurements of cluster densities and hardening levels up to 2 dpa exist. We then provide calculations under expected DEMO fusion conditions. Several key mechanisms involving Re atoms and defect clusters are found to govern the accumulation of irradiation damage in each case. We use established correlations to translate damage accumulation into hardening increases and compare our results to the experimental measurements. We find hardening increases in excess of 5000 MPa in all cases, which casts doubts about the integrity of W-based materials under long-term fusion exposure.

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.

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.

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

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

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

Paton, Ian

The Rocky Flats Environmental Technology Site (RFETS) is a Department of Energy facility located approximately 16 miles northwest of Denver, Colorado. Processing and fabrication of nuclear weapons components occurred at Rocky Flats from 1952 through 1989. Operations at the Site included the use of several radionuclides, including plutonium-239/240 (Pu), americium-241 (Am), and various uranium (U) isotopes, as well as several types of chlorinated solvents. The historic operations resulted in legacy contamination, including contaminated facilities, process waste lines, buried wastes and surface soil contamination. Decontamination and removal of buildings at the site was completed in late 2005, culminating more than tenmore » years of active environmental remediation work. The Corrective Action Decision/Record of Decision was subsequently approved in 2006, signifying regulatory approval and closure of the site. The use of RFETS as a National Wildlife Refuge is scheduled to be in full operation by 2012. To develop a plan for remediating different types of radionuclide contaminants present in the RFETS environment required understanding the different environmental transport pathways for the various actinides. Developing this understanding was the primary objective of the Actinide Migration Evaluation (AME) project. Findings from the AME studies were used in the development of RFETS remediation strategies. The AME project focused on issues of actinide behavior and mobility in surface water, groundwater, air, soil and biota at RFETS. For the purposes of the AME studies, actinide elements addressed included Pu, Am, and U. The AME program, funded by DOE, brought together personnel with a broad range of relevant expertise in technical investigations. The AME advisory panel identified research investigations and approaches that could be used to solve issues related to actinide migration at the Site. An initial step of the AME was to develop a conceptual model to provide a qualitative description of the relationships among potential actinide sources and transport pathways at RFETS. One conceptual model was developed specifically for plutonium and americium, because of their similar geochemical and transport properties. A separate model was developed for uranium because of its different properties and mobility in the environment. These conceptual models were guidelines for quantitative analyses described in the RFETS Pathway Analysis Report, which used existing data from the literature as well as site-specific analyses, including field, laboratory and modeling studies to provide quantitative estimates of actinide migration in the RFETS environment. For pathways where more than one method was used to estimate offsite loads for a specific pathway, the method yielding the highest estimated off-site was used for comparison purposes. For all actinides studied, for pre-remediation conditions, air and surface water were identified to be the dominant transport mechanisms. The estimated annual airborne plutonium-239/240 load transported off site exceeded the surface water load by roughly a factor of 40. However, despite being the largest transport pathway, airborne radionuclide concentrations at the monitoring location with the highest measurements during the period studied were less than two percent of the allowable 10 milli-rem standard governing DOE facilities. Estimated actinide loads for other pathways were much less. Shallow groundwater was approximately two orders of magnitude lower, or 1/100 of the load conveyed in surface water. The estimated biological pathway load for plutonium was approximately five orders of magnitude less, or 1/100,000, of the load estimated for surface-water. The pathway analysis results were taken into consideration during subsequent remediation activities that occurred at the site. For example, when the 903 Pad area was remediated to address elevated concentrations of Pu and Am in the surface soil, portable tent structures were constructed to prevent wind and water erosion from occurring while remediation activities took place. Following remediation of the 903 Pad and surrounding area, coconut erosion blankets were installed to mitigate erosion effects while vegetation was reestablished [2]. These measures were effective tools to address the primary transport mechanisms identified, coupling the scientific understanding of the site with the remediation strategy.« less

Transmutation of Matter in Byzantium: The Case of Michael Psellos, the Alchemist

NASA Astrophysics Data System (ADS)

Katsiampoura, Gianna

2008-06-01

There is thus nothing paradoxical about the inclusion of alchemy in the ensemble of the physical sciences nor in the preoccupation with it on the part of learned men engaged in scientific study. In the context of the Medieval model, where discourse on the physical world was ambiguous, often unclear, and lacking the support of experimental verification, the transmutation of matter, which was the subject of alchemy, even if not attended by a host of occult features, was a process that was thought to have a probable basis in reality. What is interesting in this connection is the utilization of the scientific categories of the day for discussion of transmutation of matter and the attempt to avoid, in most instances in the texts that survive, of methods reminiscent of magic.

Equipment upgrades for the Pu-238 program

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

Congdon, J.W.; Stephens, W.D.; Marra, J.E.

1990-02-14

Much of the equipment and instrumentation in the Pu-238 production facilities is more than 15 years old. Significant improvements have been made in the available instrumentation, in particular, due to the application of microprocessors and lasers. The Actinide Technology Section of SRL has selected and is in the process of evaluating several state-of-the-art instruments which have potential applications in the Pu-238 program. The ease of operation and the accuracy of the instruments have been improved and, in most cases, the cost of the instruments have decreased. 5 refs.

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

Predictions of Actinide Solubilities under Near-Field Conditions Expected in the WIPP

NASA Astrophysics Data System (ADS)

Brush, L. H.; Xiong, Y.

2009-12-01

The Waste Isolation Pilot Plant (WIPP) is a U.S. Department of Energy (DOE) repository in southeast New Mexico for defense-related transuranic (TRU) waste. The repository, which opened in March 1999, is located at a subsurface depth of 655 m (2150 ft) in the Salado Fm., a Permian bedded-salt formation. The repository will eventually contain the equivalent of 844,000 208 L (55 gal) drums of TRU waste. After filling the rooms and access drifts and installing panel closures, creep closure of the salt will crush the steel waste containers in most cases and encapsulate the waste. The WIPP actinide source term model used for long-term performance assessment (PA) of the repository comprises dissolved and suspended submodels (solubilities and colloids). This presentation will describe the solubilities. From the standpoint of long-term PA, the order of importance of the radioelements in the TRU waste to be emplaced in the WIPP is Pu ~ Am >> U > Th >> Np ~ Cm and fission products. The DOE has included all of these actinides, but not fission products, in the WIPP Actinide Source Term Program (ASTP). Anoxic corrosion of Fe- and Al-base metals and microbial consumption of cellulosic, plastic, and rubber materials will produce gas and create strongly reducing conditions in the WIPP after closure. The use of MgO as an engineered barrier to consume microbially produced CO2 will result in low fCO2 and basic pH. Under these conditions, Th, U, Np, Pu, and Am will speciate essentially entirely as Th(IV), U(IV), Np(IV), Pu(III), and Am(III); or Th(IV), U(VI), Np(V), Pu(IV), and Am(III). The DOE has developed thermodynamic speciation-and-solubility models for +III, +IV, and +V actinides in brines. Experimental data for Nd, Am, and Cm species were used to parameterize the +III Pitzer activity-coefficient model; data for Th species were used for the +IV model; and data for Np(V) species were used for the +V model. These models include the effects of the organic ligands acetate, citrate, EDTA, and oxalate in TRU waste. The oxidation-state analogy was then used to extend the +III model to Pu(III), and the +IV model to Pu(IV), U(IV), and Np(IV). The solubility of U(VI) was estimated. For the recent WIPP Compliance Recertification Application PA Baseline Calculations, we calculated actinide solubilities with fCO2 buffered at 3.14 × 10-6 atm by the brucite-hydromagnesite carbonation reaction, with pH maintained at ~9 by the brucite dissolution-precipitation reaction, and with estimated concentrations of the organic ligands in brines from the Salado and the Castile Fm., which underlies the Salado. The calculated +III, +IV, and +V solubilities are 1.56 × 10-6, 5.64 × 10-8, and 4.07 × 10-7 M, respectively, in Salado brine; and 1.51 × 10-6, 6.98 × 10-8, and 8.75 × 10-7 M in Castile brine. The U(VI) solubility estimated for both brines is 1 × 10-3 M. This research is funded by WIPP programs administered by the U.S. Department of Energy. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy’s National Nuclear Security Administration under contract DE-AC04-94AL85000.

Hypergraph partitioning implementation for parallelizing matrix-vector multiplication using CUDA GPU-based parallel computing

NASA Astrophysics Data System (ADS)

Murni, Bustamam, A.; Ernastuti, Handhika, T.; Kerami, D.

2017-07-01

Calculation of the matrix-vector multiplication in the real-world problems often involves large matrix with arbitrary size. Therefore, parallelization is needed to speed up the calculation process that usually takes a long time. Graph partitioning techniques that have been discussed in the previous studies cannot be used to complete the parallelized calculation of matrix-vector multiplication with arbitrary size. This is due to the assumption of graph partitioning techniques that can only solve the square and symmetric matrix. Hypergraph partitioning techniques will overcome the shortcomings of the graph partitioning technique. This paper addresses the efficient parallelization of matrix-vector multiplication through hypergraph partitioning techniques using CUDA GPU-based parallel computing. CUDA (compute unified device architecture) is a parallel computing platform and programming model that was created by NVIDIA and implemented by the GPU (graphics processing unit).

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)

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.

The 230Th correction is the 1st priority for accurate dates of young zircons: U/Th partitioning experiments and measurements

NASA Astrophysics Data System (ADS)

Krawczynski, M.; McLean, N.

2017-12-01

One of the most accurate and useful ways of determining the age of rocks that formed more than about 500,000 years ago is uranium-lead (U-Pb) geochronology. Earth scientists use U-Pb geochronology to put together the geologic history of entire regions and of specific events, like the mass extinction of all non-avian dinosaurs about 66 million years ago or the catastrophic eruptions of supervolcanoes like the one currently centered at Yellowstone. The mineral zircon is often utilized because it is abundant, durable, and readily incorporates uranium into its crystal structure. But it excludes thorium, whose isotope 230Th is part of the naturally occurring isotopic decay chain from 238U to 206Pb. Calculating a date from the relative abundances of 206Pb and 238U therefore requires a correction for the missing 230Th. Existing experimental and observational constraints on the way U and Th behave when zircon crystallizes from a melt are not known precisely enough, and thus currently the uncertainty in dates introduced by they `Th correction' is one of the largest sources of systematic error in determining dates. Here we present preliminary results on our study of actinide partitioning between zircon and melt. Experiments have been conducted to grow zircon from melts doped with U and Th that mimic natural magmas at a range of temperatures, and compositions. Synthetic zircons are separated from their coexisting glass and using high precision and high-spatial-resolution techniques, the abundance and distribution of U and Th in each phase is determined. These preliminary experiments are the beginning of a study that will result in precise determination of the zircon/melt uranium and thorium partition coefficients under a wide variety of naturally occurring conditions. This data will be fit to a multidimensional surface using maximum likelihood regression techniques, so that the ratio of partition coefficients can be calculated for any set of known parameters. The results of this study will reduce the largest source of uncertainty in dating young zircons and improve the accuracy of U-Pb dates, improving our ability to tell time during geologic processes. The attainment of more accurate timing of the geologic timescale is important to geologists of all disciplines, from paleontology to planetary cosmochemistry to geobiology.

Determination of Uncertainties for +III and +IV Actinide Solubilities in the WIPP Geochemistry Model for the 2009 Compliance Recertification Application

NASA Astrophysics Data System (ADS)

Ismail, A. E.; Xiong, Y.; Nowak, E. J.; Brush, L. H.

2009-12-01

The Waste Isolation Pilot Plant (WIPP) is a U.S. Department of Energy (DOE) repository in southeast New Mexico for defense-related transuranic (TRU) waste. Every five years, the DOE is required to submit an application to the Environmental Protection Agency (EPA) demonstrating the WIPP’s continuing compliance with the applicable EPA regulations governing the repository. Part of this recertification effort involves a performance assessment—a probabilistic evaluation of the repository performance with respect to regulatory limits on the amount of releases from the repository to the accessible environment. One of the models used as part of the performance assessment process is a geochemistry model, which predicts solubilities of the radionuclides in the brines that may enter the repository in the different scenarios considered by the performance assessment. The dissolved actinide source term comprises actinide solubilities, which are input parameters for modeling the transport of radionuclides as a result of brine flow through and from the repository. During a performance assessment, the solubilities are modeled as the product of a “base” solubility determined from calculations based on the chemical conditions expected in the repository, and an uncertainty factor that describes the potential deviations of the model from expected behavior. We will focus here on a discussion of the uncertainties. To compute a cumulative distribution function (CDF) for the uncertainties, we compare published, experimentally measured solubility data to predictions made using the established WIPP geochemistry model. The differences between the solubilities observed for a given experiment and the calculated solubilities from the model are used to form the overall CDF, which is then sampled as part of the performance assessment. We will discuss the methodology used to update the CDF’s for the +III actinides, obtained from data for Nd, Am, and Cm, and the +IV actinides, obtained from data for Th, and present results for the calculations of the updated CDF’s. We compare the CDF’s to the distributions computed for the previous recertification, and discuss the potential impact of the changes on the geochemistry model. This research is funded by WIPP programs administered by the U.S. Department of Energy. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy’s National Nuclear Security Administration under contract DE-AC04-94AL85000.

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.

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.

Analysis methodology and development of a statistical tool for biodistribution data from internal contamination with actinides.

PubMed

Lamart, Stephanie; Griffiths, Nina M; Tchitchek, Nicolas; Angulo, Jaime F; Van der Meeren, Anne

2017-03-01

The aim of this work was to develop a computational tool that integrates several statistical analysis features for biodistribution data from internal contamination experiments. These data represent actinide levels in biological compartments as a function of time and are derived from activity measurements in tissues and excreta. These experiments aim at assessing the influence of different contamination conditions (e.g. intake route or radioelement) on the biological behavior of the contaminant. The ever increasing number of datasets and diversity of experimental conditions make the handling and analysis of biodistribution data difficult. This work sought to facilitate the statistical analysis of a large number of datasets and the comparison of results from diverse experimental conditions. Functional modules were developed using the open-source programming language R to facilitate specific operations: descriptive statistics, visual comparison, curve fitting, and implementation of biokinetic models. In addition, the structure of the datasets was harmonized using the same table format. Analysis outputs can be written in text files and updated data can be written in the consistent table format. Hence, a data repository is built progressively, which is essential for the optimal use of animal data. Graphical representations can be automatically generated and saved as image files. The resulting computational tool was applied using data derived from wound contamination experiments conducted under different conditions. In facilitating biodistribution data handling and statistical analyses, this computational tool ensures faster analyses and a better reproducibility compared with the use of multiple office software applications. Furthermore, re-analysis of archival data and comparison of data from different sources is made much easier. Hence this tool will help to understand better the influence of contamination characteristics on actinide biokinetics. Our approach can aid the optimization of treatment protocols and therefore contribute to the improvement of the medical response after internal contamination with actinides.

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

Cone-like rhodopsin expressed in the all-cone retina of the colubrid pine snake as a potential adaptation to diurnality.

PubMed

Bhattacharyya, Nihar; Darren, Benedict; Schott, Ryan K; Tropepe, Vincent; Chang, Belinda S W

2017-07-01

Colubridae is the largest and most diverse family of snakes, with visual systems that reflect this diversity, encompassing a variety of retinal photoreceptor organizations. The transmutation theory proposed by Walls postulates that photoreceptors could evolutionarily transition between cell types in squamates, but few studies have tested this theory. Recently, evidence for transmutation and rod-like machinery in an all-cone retina has been identified in a diurnal garter snake ( Thamnophis ), and it appears that the rhodopsin gene at least may be widespread among colubrid snakes. However, functional evidence supporting transmutation beyond the existence of the rhodopsin gene remains rare. We examined the all-cone retina of another colubrid, Pituophis melanoleucus , thought to be more secretive/burrowing than Thamnophis We found that P. melanoleucus expresses two cone opsins (SWS1, LWS) and rhodopsin (RH1) within the eye. Immunohistochemistry localized rhodopsin to the outer segment of photoreceptors in the all-cone retina of the snake and all opsin genes produced functional visual pigments when expressed in vitro Consistent with other studies, we found that P. melanoleucus rhodopsin is extremely blue-shifted. Surprisingly, P. melanoleucus rhodopsin reacted with hydroxylamine, a typical cone opsin characteristic. These results support the idea that the rhodopsin-containing photoreceptors of P. melanoleucus are the products of evolutionary transmutation from rod ancestors, and suggest that this phenomenon may be widespread in colubrid snakes. We hypothesize that transmutation may be an adaptation for diurnal, brighter-light vision, which could result in increased spectral sensitivity and chromatic discrimination with the potential for colour vision. © 2017. Published by The Company of Biologists Ltd.

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.

Discovering Link Communities in Complex Networks by an Integer Programming Model and a Genetic Algorithm

PubMed Central

Li, Zhenping; Zhang, Xiang-Sun; Wang, Rui-Sheng; Liu, Hongwei; Zhang, Shihua

2013-01-01

Identification of communities in complex networks is an important topic and issue in many fields such as sociology, biology, and computer science. Communities are often defined as groups of related nodes or links that correspond to functional subunits in the corresponding complex systems. While most conventional approaches have focused on discovering communities of nodes, some recent studies start partitioning links to find overlapping communities straightforwardly. In this paper, we propose a new quantity function for link community identification in complex networks. Based on this quantity function we formulate the link community partition problem into an integer programming model which allows us to partition a complex network into overlapping communities. We further propose a genetic algorithm for link community detection which can partition a network into overlapping communities without knowing the number of communities. We test our model and algorithm on both artificial networks and real-world networks. The results demonstrate that the model and algorithm are efficient in detecting overlapping community structure in complex networks. PMID:24386268

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

Data compression of discrete sequence: A tree based approach using dynamic programming

NASA Technical Reports Server (NTRS)

Shivaram, Gurusrasad; Seetharaman, Guna; Rao, T. R. N.

1994-01-01

A dynamic programming based approach for data compression of a ID sequence is presented. The compression of an input sequence of size N to that of a smaller size k is achieved by dividing the input sequence into k subsequences and replacing the subsequences by their respective average values. The partitioning of the input sequence is carried with the intention of reducing the mean squared error in the reconstructed sequence. The complexity involved in finding the partitions which would result in such an optimal compressed sequence is reduced by using the dynamic programming approach, which is presented.

Summary of Research Activities. Academic Departments, 1979-1980.

DTIC Science & Technology

1979-10-01

studied, including recycling, geologic storage, transmutation , ejection from earth, and seabed disposal. Currently, the most favored methods are...official society. (4) The poem ultimately celebrates in a sort of poetic eucharist the regenerative power of poetry to transmute the bread and wine of...Union prevails. Such a view becomes commonplace after Burr’s political enemies attack him as a Catiline, Cain, and sexual predator. Influenced by these

The Changing Nature of Warfare, the Factors Mediating Future Conflict, and Implications for SOF

DTIC Science & Technology

2006-04-01

most commonly used vernacular today, one is describing the person’s sexual orientation.13 The English language is replete with other words that have...countries and those that are technologically more advanced, primarily due to labor cost differentials. Globaliza- tion has transmuted economics from a...fascination with forensic sci- ences, ala the acclaimed television pro- gram CSI, has transmuted from civilian criminal proceedings to microscopic

FIRST-PRINCIPLES CALCULATIONS OF CHARGE STATES AND FORMATION ENERGIES OF Mg, Al, and Be TRANSMUTANTS IN 3C-SiC

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

Hu, Shenyang Y.; Setyawan, Wahyu; Jiang, Weilin

2014-08-28

The Vienna Ab-initio Simulation Package (VASP) is employed to calculate charge states and the formation energies of Mg, Al and Be transmutants at different lattice sites in 3C-SiC. The results provide important information on the dependence of the most stable charge state and formation energy of Mg, Al, Be and vacancies on electron potentials.

Electric Spark Discharges in Water. Low-energy Nuclear Transmutations and Light Leptonic Magnetic Monopoles in an Extended Standard Model

NASA Astrophysics Data System (ADS)

Stumpf, Harald

2017-08-01

Light leptonic magnetic monopoles were predicted by Lochak [G. Lochak, Intern. J. Theor. Phys. 24, 1019 (1985).]. Experimental indications based on nuclear transmutations were announced by Urutskoiev et al. [L. I. Urutskoiev, V. I. Liksonov, V. G. Tsinoev, Ann. Fond. L. de Broglie 27, Nr.4, 791 (2002).] and Urutskoev [L. J. Urutskoev, Ann. Fond. L. de Broglie 29, 1149 (2004).]. A theoretical interpretation of these transmutations is proposed under the assumption that light leptonic magnetic monopoles are created during spark discharges in water. The latter should be excited neutrinos according to Lochak. This hypothesis enforces the introduction of an extended Standard Model described in previous papers. The most important results of this study are (i) that multiple proton captures are responsible for the variety of transmutations and that leptonic magnetic monopoles are involved in these processes (ii) that electromagnetic duality can be established for bound states of leptonic monopoles although massive monopoles are in general unstable (iii) that criteria for the emission of leptonic magnetic monopoles and for their catalytic effect on weak decays are set up and elaborated. The study can be considered as a contribution to the efforts of Urutskoiev and Lochak to understand the reasons for accidents in power plants.

Crystal Growth and Characterization of THO2 and UxTh1-xO2

DTIC Science & Technology

2013-03-01

bulk actinide crystals would open up new possibilities for the detection of weapons of mass destruction, the study of the effect of aging on...way of growing bulk actinide materials of optical quality. These refractory oxide single crystals offer potential applications in thorium nuclear...fuel technology, wide-band-gap uranium-based direct-conversion solid state neutron detectors, and understanding how actinide fuels age with time. ThO2

Molecular Quantum Mechanics: Analytic Gradients and Beyond - Program and Abstracts

DTIC Science & Technology

2007-06-03

Kutzelnigg (Bochum, Germany) Chair: Pekka Pyykko (Helsinki, Finland) Which Masses are Vibrating or Rotating in a Molecule? 15:40-16:15 O30...Krylov (Los Angeles, CA, U.S.A.) Multiconfigurational Quantum Chemistry for Actinide Containing Systems: From Isolated Molecules to Condensed...the genetic algorithm will be critically assessed. For B4n, the double rings are notably stable. The DFT calculations provide strong indications of

Keeping the Momentum and Nuclear Forensics at Los Alamos National Laboratory

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

Steiner, Robert Ernest; Dion, Heather M.; Dry, Donald E.

LANL has 70 years of experience in nuclear forensics and supports the community through a wide variety of efforts and leveraged capabilities: Expanding the understanding of nuclear forensics, providing training on nuclear forensics methods, and developing bilateral relationships to expand our understanding of nuclear forensic science. LANL remains highly supportive of several key organizations tasked with carrying forth the Nuclear Security Summit messages: IAEA, GICNT, and INTERPOL. Analytical chemistry measurements on plutonium and uranium matrices are critical to numerous programs including safeguards accountancy verification measurements. Los Alamos National Laboratory operates capable actinide analytical chemistry and material science laboratories suitable formore » nuclear material and environmental forensic characterization. Los Alamos National Laboratory uses numerous means to validate and independently verify that measurement data quality objectives are met. Numerous LANL nuclear facilities support the nuclear material handling, preparation, and analysis capabilities necessary to evaluate samples containing nearly any mass of an actinide (attogram to kilogram levels).« less

Understanding Release from Actinide Targets -- Recent Results from RIB Development

NASA Astrophysics Data System (ADS)

Kronenberg, Andreas; Carter, H. K.; Spejewski, E. H.; Stracener, D. W.

2006-10-01

Development of ion beams of short-lived isotopes is crucial for modern nuclear structure and nuclear astrophysics. The Holifield Radioactive Ion Beam Facility at Oak Ridge National Laboratory uses the ISOL (Isotope Separation Online) technique to provide radioactive ion beams. So far, uranium carbide has been used as a target to produce neutron-rich fission fragments. Thermodynamic calculations indicate the possibility of in-situ chemical side band formations of volatile species of refractory metals, such as V and Re. These elements release out of oxide targets after production in a nuclear reaction, and can occur only through in-situ formation of their volatile oxide. These have been confirmed experimentally. The results from recent, more detailed investigations of ThO2, UB4 and other actinide targets as well as conclusions from systematic studies will be presented. This research was sponsored by the NNSA under Stewardship Science Academic Alliance program through DOE Cooperative Agreement # DE-FC03-3NA00143.

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.

Characterization of Nonlinear Systems with Memory by Means of Volterra Expansions with Frequency Partitioning: Application to a Cicada Mating Call

DTIC Science & Technology

2010-06-15

Partitioning Application to a Cicada Mating Call Albert H. Nuttall Adaptive Methods Inc. Derke R. Hughes NUWC Division Newport IVAVSEA WARFARE...Frequency Partitioning: Application to a Cicada Mating Call 5a. CONTRACT NUMBER 5b. GRANT NUMBER 5c. PROGRAM ELEMENT NUMBER 6. AUTHOR(S) Albert H... cicada mating call with a distinctly non-white and non-Gaussian excitation gives good results for the estimated first- and second-order kernels and

DEVELOPMENT AND APPLICATION OF EQUILIBRIUM PARTITIONING SEDIMENT GUIDELINES IN THE ASSESSMENT OF SEDIMENT PAH CONTAMINATION

EPA Science Inventory

The U.S. Environmental Protection Agency used insights and methods from its water quality criteria program to develop ESGs. The discovery that freely-dissolved contaminants were the toxic form led to equilibrium partitioning being chosen to model the distribution of contaminants...

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.

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

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.

Vortex transmutation.

PubMed

Ferrando, Albert; Zacarés, Mario; García-March, Miguel-Angel; Monsoriu, Juan A; de Córdoba, Pedro Fernández

2005-09-16

Using group theory arguments and numerical simulations, we demonstrate the possibility of changing the vorticity or topological charge of an individual vortex by means of the action of a system possessing a discrete rotational symmetry of finite order. We establish on theoretical grounds a "transmutation pass" determining the conditions for this phenomenon to occur and numerically analyze it in the context of two-dimensional optical lattices. An analogous approach is applicable to the problems of Bose-Einstein condensates in periodic potentials.

NEUTRON FLUX INTENSITY DETECTION

DOEpatents

Russell, J.T.

1964-04-21

A method of measuring the instantaneous intensity of neutron flux in the core of a nuclear reactor is described. A target gas capable of being transmuted by neutron bombardment to a product having a resonance absorption line nt a particular microwave frequency is passed through the core of the reactor. Frequency-modulated microwave energy is passed through the target gas and the attenuation of the energy due to the formation of the transmuted product is measured. (AEC)

Hydrogen bond disruption in DNA base pairs from (14)C transmutation.

PubMed

Sassi, Michel; Carter, Damien J; Uberuaga, Blas P; Stanek, Christopher R; Mancera, Ricardo L; Marks, Nigel A

2014-09-04

Recent ab initio molecular dynamics simulations have shown that radioactive carbon does not normally fragment DNA bases when it decays. Motivated by this finding, density functional theory and Bader analysis have been used to quantify the effect of C → N transmutation on hydrogen bonding in DNA base pairs. We find that (14)C decay has the potential to significantly alter hydrogen bonds in a variety of ways including direct proton shuttling (thymine and cytosine), thermally activated proton shuttling (guanine), and hydrogen bond breaking (cytosine). Transmutation substantially modifies both the absolute and relative strengths of the hydrogen bonding pattern, and in two instances (adenine and cytosine), the density at the critical point indicates development of mild covalent character. Since hydrogen bonding is an important component of Watson-Crick pairing, these (14)C-induced modifications, while infrequent, may trigger errors in DNA transcription and replication.

The Changes of Energy Interactions between Nucleus Function and Mitochondria Functions Causing Transmutation of Chronic Inflammation into Cancer Metabolism.

PubMed

Ponizovskiy, Michail R

2016-01-01

Interactions between nucleus and mitochondria functions induce the mechanism of maintenance stability of cellular internal energy according to the first law of thermodynamics in able-bodied cells and changes the mechanisms of maintenance stability of cellular internal energy creating a transition stationary state of ablebodied cells into quasi-stationary pathologic states of acute inflammation transiting then into chronic inflammation and then transmuting into cancer metabolism. The mechanisms' influences of intruding etiologic pathologic agents (microbe, virus, etc.) lead to these changes of energy interactions between nucleus and mitochondria functions causing general acute inflammation, then passing into local chronic inflammation, and reversing into cancer metabolism transmutation. Interactions between biochemical processes and biophysical processes of cellular capacitors' operations create a supplementary mechanism of maintenance stability of cellular internal energy in the norm and in pathology. Discussion of some scientific works eliminates doubts of the authors of these works.

Application of neutron transmutation doping method to initially p-type silicon material.

PubMed

Kim, Myong-Seop; Kang, Ki-Doo; Park, Sang-Jun

2009-01-01

The neutron transmutation doping (NTD) method was applied to the initially p-type silicon in order to extend the NTD applications at HANARO. The relationship between the irradiation neutron fluence and the final resistivity of the initially p-type silicon material was investigated. The proportional constant between the neutron fluence and the resistivity was determined to be 2.3473x10(19)nOmegacm(-1). The deviation of the final resistivity from the target for almost all the irradiation results of the initially p-type silicon ingots was at a range from -5% to 2%. In addition, the burn-up effect of the boron impurities, the residual (32)P activity and the effect of the compensation characteristics for the initially p-type silicon were studied. Conclusively, the practical methodology to perform the neutron transmutation doping of the initially p-type silicon ingot was established.

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

Air Traffic Sector Configuration Change Frequency

NASA Technical Reports Server (NTRS)

Chatterji, Gano Broto; Drew, Michael

2009-01-01

Several techniques for partitioning airspace have been developed in the literature. The question of whether a region of airspace created by such methods can be used with other days of traffic, and the number of times a different partition is needed during the day is examined in this paper. Both these aspects are examined for the Fort Worth Center airspace sectors. A Mixed Integer Linear Programming method is used with actual air traffic data of ten high-volume low-weather-delay days for creating sectors. Nine solutions were obtained for each two-hour period of the day by partitioning the center airspace into two through 18 sectors in steps of two sectors. Actual track-data were played back with the generated partitions for creating histograms of the traffic-counts. The best partition for each two-hour period was then identified based on the nine traffic-count distributions. Numbers of sectors in such partitions were analyzed to determine the number of times a different configuration is needed during the day. One to three partitions were selected for the 24-hour period, and traffic data from ten days were played back to test if the traffic-counts stayed below the threshold values associated with these partitions. Results show that these partitions are robust and can be used for longer durations than they were designed for

A strategy to load balancing for non-connectivity MapReduce job

NASA Astrophysics Data System (ADS)

Zhou, Huaping; Liu, Guangzong; Gui, Haixia

2017-09-01

MapReduce has been widely used in large scale and complex datasets as a kind of distributed programming model. Original Hash partitioning function in MapReduce often results the problem of data skew when data distribution is uneven. To solve the imbalance of data partitioning, we proposes a strategy to change the remaining partitioning index when data is skewed. In Map phase, we count the amount of data which will be distributed to each reducer, then Job Tracker monitor the global partitioning information and dynamically modify the original partitioning function according to the data skew model, so the Partitioner can change the index of these partitioning which will cause data skew to the other reducer that has less load in the next partitioning process, and can eventually balance the load of each node. Finally, we experimentally compare our method with existing methods on both synthetic and real datasets, the experimental results show our strategy can solve the problem of data skew with better stability and efficiency than Hash method and Sampling method for non-connectivity MapReduce task.

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.

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.

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

Georgia Tech Studies of Sub-Critical Advanced Burner Reactors with a D-T Fusion Tokamak Neutron Source for the Transmutation of Spent Nuclear Fuel

NASA Astrophysics Data System (ADS)

Stacey, W. M.

2009-09-01

The possibility that a tokamak D-T fusion neutron source, based on ITER physics and technology, could be used to drive sub-critical, fast-spectrum nuclear reactors fueled with the transuranics (TRU) in spent nuclear fuel discharged from conventional nuclear reactors has been investigated at Georgia Tech in a series of studies which are summarized in this paper. It is found that sub-critical operation of such fast transmutation reactors is advantageous in allowing longer fuel residence time, hence greater TRU burnup between fuel reprocessing stages, and in allowing higher TRU loading without compromising safety, relative to what could be achieved in a similar critical transmutation reactor. The required plasma and fusion technology operating parameter range of the fusion neutron source is generally within the anticipated operational range of ITER. The implications of these results for fusion development policy, if they hold up under more extensive and detailed analysis, is that a D-T fusion tokamak neutron source for a sub-critical transmutation reactor, built on the basis of the ITER operating experience, could possibly be a logical next step after ITER on the path to fusion electrical power reactors. At the same time, such an application would allow fusion to contribute to meeting the nation's energy needs at an earlier stage by helping to close the fission reactor nuclear fuel cycle.

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

The use of MOX caramel fuel mixed with 241Am, 242mAm and 243Am as burnable absorber actinides for the MTR research reactors.

PubMed

Shaaban, Ismail; Albarhoum, Mohamad

2017-07-01

The MOX (UO 2 &PuO 2 ) caramel fuel mixed with 241 Am, 242m Am and 243 Am as burnable absorber actinides was proposed as a fuel of the MTR-22MW reactor. The MCNP4C code was used to simulate the MTR-22MW reactor and estimate the criticality and the neutronic parameters, and the power peaking factors before and after replacing its original fuel (U 3 O 8 -Al) by the MOX caramel fuel mixed with 241 Am, 242m Am and 243 Am actinides. The obtained results of the criticality, the neutronic parameters, and the power peaking factors for the MOX caramel fuel mixed with 241 Am, 242m Am and 243 Am actinides were compared with the same parameters of the U 3 O 8 -Al original fuel and a maximum difference is -6.18% was found. Additionally, by recycling 2.65% and 2.71% plutonium and 241 Am, 242m Am and 243 Am actinides in the MTR-22MW reactor, the level of 235 U enrichment is reduced from 4.48% to 3% and 2.8%, respectively. This also results in the reduction of the 235 U loading by 32.75% and 37.22% for the 2.65%, the 2.71% plutonium and 241 Am, 242m Am and 243 Am actinides, respectively. Copyright © 2017 Elsevier Ltd. All rights reserved.

Prediction of gas/particle partitioning of polybrominated diphenyl ethers (PBDEs) in global air: A theoretical study

NASA Astrophysics Data System (ADS)

Li, Y.-F.; Ma, W.-L.; Yang, M.

2015-02-01

Gas/particle (G/P) partitioning of semi-volatile organic compounds (SVOCs) is an important process that primarily governs their atmospheric fate, long-range atmospheric transport, and their routes of entering the human body. All previous studies on this issue are hypothetically based on equilibrium conditions, the results of which do not predict results from monitoring studies well in most cases. In this study, a steady-state model instead of an equilibrium-state model for the investigation of the G/P partitioning behavior of polybrominated diphenyl ethers (PBDEs) was established, and an equation for calculating the partition coefficients under steady state (KPS) of PBDEs (log KPS = log KPE + logα) was developed in which an equilibrium term (log KPE = log KOA + logfOM -11.91 where fOM is organic matter content of the particles) and a non-equilibrium term (log α, caused by dry and wet depositions of particles), both being functions of log KOA (octanol-air partition coefficient), are included. It was found that the equilibrium is a special case of steady state when the non-equilibrium term equals zero. A criterion to classify the equilibrium and non-equilibrium status of PBDEs was also established using two threshold values of log KOA, log KOA1, and log KOA2, which divide the range of log KOA into three domains: equilibrium, non-equilibrium, and maximum partition domain. Accordingly, two threshold values of temperature t, tTH1 when log KOA = log KOA1 and tTH2 when log KOA = log KOA2, were identified, which divide the range of temperature also into the same three domains for each PBDE congener. We predicted the existence of the maximum partition domain (the values of log KPS reach a maximum constant of -1.53) that every PBDE congener can reach when log KOA ≥ log KOA2, or t ≤ tTH2. The novel equation developed in this study was applied to predict the G/P partition coefficients of PBDEs for our Chinese persistent organic pollutants (POPs) Soil and Air Monitoring Program, Phase 2 (China-SAMP-II) program and other monitoring programs worldwide, including in Asia, Europe, North America, and the Arctic, and the results matched well with all the monitoring data, except those obtained at e-waste sites due to the unpredictable PBDE emissions at these sites. This study provided evidence that the newly developed steady-state-based equation is superior to the equilibrium-state-based equation that has been used in describing the G/P partitioning behavior over decades. We suggest that the investigation on G/P partitioning behavior for PBDEs should be based onsteady-state, not equilibrium state, and equilibrium is just a special case of steady-state when non-equilibrium factors can be ignored. We also believe that our new equation provides a useful tool for environmental scientists in both monitoring and modeling research on G/P partitioning of PBDEs and can be extended to predict G/P partitioning behavior for other SVOCs as well.

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

Joint Actinide Shock Physics Experimental Research - JASPER

ScienceCinema

None

2018-01-16

Commonly known as JASPER the Joint Actinide Shock Physics Experimental Research facility is a two stage light gas gun used to study the behavior of plutonium and other materials under high pressures, temperatures, and strain rates.

The DD Cold Fusion-Transmutation Connection

NASA Astrophysics Data System (ADS)

Chubb, Talbot A.

2005-12-01

LENR theory must explain dd fusion, alpha-addition transmutations, radiationless nuclear reactions, and three-body nuclear particle reactions. Reaction without radiation requires many-body D Bloch+ periodicity in both location and internal structure dependencies. Electron scattering leads to mixed quantum states. The radiationless dd fusion reaction is 2-D Bloch+ -> {}4 He Bloch2+. Overlap between {}4 He Bloch2+ and surface Cs leads to alpha absorption. In the Iwamura et al. studies active deuterium is created by scattering at diffusion barriers.

Neutron Transmutation Doped (NTD) germanium thermistors for sub-mm bolometer applications

NASA Technical Reports Server (NTRS)

Haller, E. E.; Itoh, K. M.; Beeman, J. W.

1996-01-01

Recent advances in the development of neutron transmutation doped (NTD) semiconductor thermistors fabricated from natural and controlled isotopic composition germanium are reported. The near ideal doping uniformity that can be achieved with the NTD process, the device simplicity of NTD Ge thermistors and the high performance of cooled junction field effect transistor preamplifiers led to the widespread acceptance of these thermal sensors in ground-based, airborne and spaceborne radio telescopes. These features made possible the development of efficient bolometer arrays.

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.

Rapid method to determine actinides and 89/90Sr in limestone and marble samples

DOE PAGES

Maxwell, Sherrod L.; Culligan, Brian; Hutchison, Jay B.; ...

2016-04-12

A new method for the determination of actinides and radiostrontium in limestone and marble samples has been developed that utilizes a rapid sodium hydroxide fusion to digest the sample. Following rapid pre-concentration steps to remove sample matrix interferences, the actinides and 89/90Sr are separated using extraction chromatographic resins and measured radiometrically. The advantages of sodium hydroxide fusion versus other fusion techniques will be discussed. Lastly, this approach has a sample preparation time for limestone and marble samples of <4 hours.

Computer program for calculating and fitting thermodynamic functions

NASA Technical Reports Server (NTRS)

Mcbride, Bonnie J.; Gordon, Sanford

1992-01-01

A computer program is described which (1) calculates thermodynamic functions (heat capacity, enthalpy, entropy, and free energy) for several optional forms of the partition function, (2) fits these functions to empirical equations by means of a least-squares fit, and (3) calculates, as a function of temperture, heats of formation and equilibrium constants. The program provides several methods for calculating ideal gas properties. For monatomic gases, three methods are given which differ in the technique used for truncating the partition function. For diatomic and polyatomic molecules, five methods are given which differ in the corrections to the rigid-rotator harmonic-oscillator approximation. A method for estimating thermodynamic functions for some species is also given.

Optimal Clustering in Graphs with Weighted Edges: A Unified Approach to the Threshold Problem.

ERIC Educational Resources Information Center

Goetschel, Roy; Voxman, William

1987-01-01

Relations on a finite set V are viewed as weighted graphs. Using the language of graph theory, two methods of partitioning V are examined: selecting threshold values and applying them to a maximal weighted spanning forest, and using a parametric linear program to obtain a most adhesive partition. (Author/EM)

Using a Partitioned Treatment Design to Examine the Effect of Project WET

ERIC Educational Resources Information Center

D'Agostino, Jerome V.; Schwartz, Kerry L.; Cimetta, Adriana D.; Welsh, Megan E.

2007-01-01

Although young people in 50 U.S. states and 21 countries learn about water resources through Project WET (Water Education for Teachers), few researchers have conducted summative evaluations of the program. The authors employed a partitioned, or differential, treatments design in which two groups of 6th-grade students received overlapping but…

RAPID SEPARATION METHOD FOR EMERGENCY WATER AND URINE SAMPLES

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

Maxwell, S.; Culligan, B.

2008-08-27

The Savannah River Site Environmental Bioassay Lab participated in the 2008 NRIP Emergency Response program administered by the National Institute for Standards and Technology (NIST) in May, 2008. A new rapid column separation method was used for analysis of actinides and {sup 90}Sr the NRIP 2008 emergency water and urine samples. Significant method improvements were applied to reduce analytical times. As a result, much faster analysis times were achieved, less than 3 hours for determination of {sup 90}Sr and 3-4 hours for actinides. This represents a 25%-33% improvement in analysis times from NRIP 2007 and a {approx}100% improvement compared tomore » NRIP 2006 report times. Column flow rates were increased by a factor of two, with no significant adverse impact on the method performance. Larger sample aliquots, shorter count times, faster cerium fluoride microprecipitation and streamlined calcium phosphate precipitation were also employed. Based on initial feedback from NIST, the SRS Environmental Bioassay Lab had the most rapid analysis times for actinides and {sup 90}Sr analyses for NRIP 2008 emergency urine samples. High levels of potential matrix interferences may be present in emergency samples and rugged methods are essential. Extremely high levels of {sup 210}Po were found to have an adverse effect on the uranium results for the NRIP-08 urine samples, while uranium results for NRIP-08 water samples were not affected. This problem, which was not observed for NRIP-06 or NRIP-07 urine samples, was resolved by using an enhanced {sup 210}Po removal step, which will be described.« less

Final Technical Report

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

Dr. Asok K. Ray

2012-05-22

During the past decades, considerable theoretical efforts have been devoted to studying the electronic and geometric structures and related properties of surfaces. Such efforts are particularly important for systems like the actinides for which experimental work is relatively difficult to perform due to material problems and toxicity. The actinides are characterized by a gradual filling of the 5f-electron shell with the degree of localization increasing with the atomic number Z along the last series of the periodic table. The open shell of the 5f electrons determines the atomic, molecular, and solid state properties of the actinide elements and their compoundsmore » and understanding the quantum mechanics of the 5f electrons is the defining issue in the chemistry and physics of actinide elements. These elements are also characterized by the increasing prominence of relativistic effects and their studies can, in fact, help us understand the role of relativity throughout the periodic table. However, the electronic and geometric structures of the actinides, specifically the trans-uranium actinides and the roles of the 5f electrons in chemical bonding are still not well understood. This is crucial not only for our understanding of the actinides but also for the fact that the actinides constitute 'the missing link' between the d transition elements and the lanthanides. The 5f orbitals have properties intermediate between those of localized 4f and delocalized 3d orbitals. Thus, a proper understanding of the actinides will help us understand the behavior of the lanthanides and transition metals as well. In fact, there is an urgent need for continued extensive and detailed theoretical research in this area to provide significant and deep understandings of the electronic and geometric structures of the actinides. In this work, we have performed electronic structure studies for plutonium (Pu), americium (Am), and curium (Cm) surfaces, and molecular adsorptions on Pu and Am surfaces. In particular, the region at the boundary of Pu and Am, is widely believed to be the crossover region between d-like itinerant and f-like localized behavior The eventual goal is a complete understanding of the surface chemistry and physics processes of all actinide surfaces, defining the chemistry and physics of such heavy elements. Among the actinides, plutonium, with five 5f electrons in the solid state, is arguably the most complex, fascinating, and enigmatic element known to mankind and has attracted extraordinary scientific and technological interests because of its unique properties, generating a significant body of research in diverse areas, including superconductivity. Pu has, at least, six stable allotropes between room temperature and melting at atmospheric pressure, indicating that the valence electrons can hybridize into a number of complex bonding arrangements. Central and critical questions relate to the electronic structure, localization of the 5f electrons and the magnetism of Pu. For the light-actinides, from Th to Pu, the 5f electrons are believed to be delocalized, hybridizing with the 6d and 7s electrons. For the heavier actinides, Am and beyond, the 5f electrons are localized with the 5f orbitals progressively lower in energy relative to the 6d configuration. Hence, Pu is in a position where the 5f electronic behavior changes from itinerant to localized. As far as magnetism is concerned, a majority of the theoretical calculations continues to claim the existence of magnetism while almost all the experimental results do not find any support for such claims. The second element of interest to us, namely americium, occupies a central position in the actinide series with respect to the involvement of 5f electrons in metallic bonding. It is widely believed that the 5f electrons in Am are localized and that Am undergoes a series of crystallographic phase changes with pressure. Fully-relativistic all electron surface studies of the different phases of Am, initially for the dhcp and the fcc surfaces, can and have provided us with valuable information about chemical bonding in Am and the transitions from f-electron delocalization to f-electron localization in trans-uranium compounds. In particular, a comparative study of the electronic structures of the Pu and Am surfaces using the techniques of all-electron modern density functional theory and beyond can provide significant information about the role of 5f electrons in bond formation as also the localization of the 5f electrons, matters of considerable controversies. The change from metallic 5f bonding into local-moment nonbonding configurations that takes place between Pu and Am is rather unique in the periodic table and is at the very heart of our understanding of electronic structure. We believe that, considering the narrow bandwidth of surface states, any transition from itinerant to localized behavior first takes place at the actinide surfaces with possible reconstructions.« less

Potentiometric Sensor for Real-Time Remote Surveillance of Actinides in Molten Salts

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

Natalie J. Gese; Jan-Fong Jue; Brenda E. Serrano

2012-07-01

A potentiometric sensor is being developed at the Idaho National Laboratory for real-time remote surveillance of actinides during electrorefining of spent nuclear fuel. During electrorefining, fuel in metallic form is oxidized at the anode while refined uranium metal is reduced at the cathode in a high temperature electrochemical cell containing LiCl-KCl-UCl3 electrolyte. Actinides present in the fuel chemically react with UCl3 and form stable metal chlorides that accumulate in the electrolyte. This sensor will be used for process control and safeguarding of activities in the electrorefiner by monitoring the concentrations of actinides in the electrolyte. The work presented focuses onmore » developing a solid-state cation conducting ceramic sensor for detecting varying concentrations of trivalent actinide metal cations in eutectic LiCl-KCl molten salt. To understand the basic mechanisms for actinide sensor applications in molten salts, gadolinium was used as a surrogate for actinides. The ß?-Al2O3 was selected as the solid-state electrolyte for sensor fabrication based on cationic conductivity and other factors. In the present work Gd3+-ß?-Al2O3 was prepared by ion exchange reactions between trivalent Gd3+ from GdCl3 and K+-, Na+-, and Sr2+-ß?-Al2O3 precursors. Scanning electron microscopy (SEM) was used for characterization of Gd3+-ß?-Al2O3 samples. Microfocus X-ray Diffraction (µ-XRD) was used in conjunction with SEM energy dispersive X-ray spectroscopy (EDS) to identify phase content and elemental composition. The Gd3+-ß?-Al2O3 materials were tested for mechanical and chemical stability by exposing them to molten LiCl-KCl based salts. The effect of annealing on the exchanged material was studied to determine improvements in material integrity post ion exchange. The stability of the ß?-Al2O3 phase after annealing was verified by µ-XRD. Preliminary sensor tests with different assembly designs will also be presented.« less

Emergence of californium as the second transitional element in the actinide series

PubMed Central

Cary, Samantha K.; Vasiliu, Monica; Baumbach, Ryan E.; Stritzinger, Jared T.; Green, Thomas D.; Diefenbach, Kariem; Cross, Justin N.; Knappenberger, Kenneth L.; Liu, Guokui; Silver, Mark A.; DePrince, A. Eugene; Polinski, Matthew J.; Van Cleve, Shelley M.; House, Jane H.; Kikugawa, Naoki; Gallagher, Andrew; Arico, Alexandra A.; Dixon, David A.; Albrecht-Schmitt, Thomas E.

2015-01-01

A break in periodicity occurs in the actinide series between plutonium and americium as the result of the localization of 5f electrons. The subsequent chemistry of later actinides is thought to closely parallel lanthanides in that bonding is expected to be ionic and complexation should not substantially alter the electronic structure of the metal ions. Here we demonstrate that ligation of californium(III) by a pyridine derivative results in significant deviations in the properties of the resultant complex with respect to that predicted for the free ion. We expand on this by characterizing the americium and curium analogues for comparison, and show that these pronounced effects result from a second transition in periodicity in the actinide series that occurs, in part, because of the stabilization of the divalent oxidation state. The metastability of californium(II) is responsible for many of the unusual properties of californium including the green photoluminescence. PMID:25880116

Innovative power conversion system for the French SFR prototype, ASTRID

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

Cachon, L.; Biscarrat, C.; Morin, F.

2012-07-01

In the framework of the French Act of 28 June 2006 about nuclear materials and waste management, the prototype ASTRID (Advanced Sodium Technological Reactor for Industrial Demonstration), foreseen in operation by the 20's, will have to demonstrate not only the minor actinide transmutation capability, but also the progress made in Sodium Fast Reactor (SFR) technology on an industrial scale, by qualifying innovative options. Some of these options still require improvements, especially in the field of operability and safety. In fact, one of the main issues with the standard steam/water Power Conversion System (PCS) of SFR is the fast and energeticmore » chemical reaction between water and sodium, which could occur in steam generators in case of tube failure. To manage the sodium/water reaction, one way consists in minimizing the impact of such event: hence studies are carried out on steam generator design, improvement of the physical knowledge of this phenomenon, development of numerical simulation to predict the reaction onset and consequences, and associated detection improvement. On the other hand, the other way consists in eliminating sodium/water reaction. In this frame, the CEA contribution to the feasibility evaluation of an alternative innovative PCS (replacing steam/water by 180 bar pressurised nitrogen) is focused on the following main topics: - The parametric study leading to nitrogen selection: the thermodynamic cycle efficiency optimisation on Brayton cycles is performed with several gases at different pressures. - The design of innovative compact heat exchangers for the gas loop: here the key points are the nuclear codification associated with inspection capability, the innovative welding process and the thermal-hydraulic and thermal-mechanic optimisations. After a general introduction of the ASTRID project, this paper presents in detail these different feasibility studies being led on the innovative gas PCS for an SFR. (authors)« 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.

Development of oxygen meters for the use in lead-bismuth

NASA Astrophysics Data System (ADS)

Konys, J.; Muscher, H.; Voß, Z.; Wedemeyer, O.

2001-07-01

Liquid lead and the eutectic lead-bismuth alloy (PbBi) are considered both as a spallation target and coolant of an accelerator driven system (ADS) for the transmutation of long-lived actinides from nuclear waste into shorter living isotopes. It is known that both, pure lead and PbBi, exhibit a high corrosivity against austenitic and ferritic steels, because of the high solubility of nickel and iron in PbBi. One way of reducing the strong corrosion is the in situ formation of stable oxide scales on the steel surfaces. Thermodynamic calculations and experimental results have confirmed, that the control of oxygen in lead or PbBi within a defined activity range can lead to acceptable corrosion rates. To control the level of oxygen dissolved in lead or PbBi, a sensor for measuring the oxygen activity is required. Within the sodium fast breeder reactor development, an adequate technique was established for estimating oxygen in liquid sodium. This knowledge can be used for other metal/oxygen systems like oxygen in PbBi. For measuring the oxygen activity and calculating its concentration, the relevant thermodynamic and solubility data have to be considered. Two reference electrode systems: Pt/air and In/In 2O 3 (both based on yttria-stabilized zirconia as solid electrolyte) are investigated to evaluate their electromotive force (EMF)-temperature dependency in saturated and unsaturated oxygen solutions. Results with both types of oxygen meters in PbBi at different oxygen levels were compared with theoretical calculations. The experimental data indicate that the design, construction and integration of an oxygen control unit in a large scale PbBi-loop seems to be very feasible.

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.

Spallation reaction study for the long-lived fission product 107Pd

NASA Astrophysics Data System (ADS)

Wang, He; Otsu, Hideaki; Sakurai, Hiroyoshi; Ahn, DeukSoon; Aikawa, Masayuki; Ando, Takashi; Araki, Shouhei; Chen, Sidong; Nobuyuki, Chiga; Doornenbal, Pieter; Fukuda, Naoki; Isobe, Tadaaki; Kawakami, Shunsuke; Kawase, Shoichiro; Kin, Tadahiro; Kondo, Yosuke; Koyama, Shunpei; Kubono, Shigeru; Maeda, Yukie; Makinaga, Ayano; Matsushita, Masafumi; Matsuzaki, Teiichiro; Michimasa, Shin'ichiro; Momiyama, Satoru; Nagamine, Shunsuke; Nakamura, Takashi; Nakano, Keita; Niikura, Megumi; Ozaki, Tomoyuki; Saito, Atsumi; Saito, Takeshi; Shiga, Yoshiaki; Shikata, Mizuki; Shimizu, Yohei; Shimoura, Susumu; Sumikama, Toshiyuki; Söderström, Pär-Anders; Suzuki, Hiroshi; Takeda, Hiroyuki; Takeuchi, Satoshi; Taniuchi, Ryo; Togano, Yasuhiro; Tsubota, Junichi; Uesaka, Meiko; Watanabe, Yasushi; Watanabe, Yukinobu; Wimmer, Kathrin; Yamamoto, Tatsuya; Yoshida, Koichi

2017-02-01

Spallation reactions for the long-lived fission product 107Pd have been studied for the purpose of nuclear waste transmutation. The cross sections on the proton- and deuteron-induced spallation were obtained at 196 and 118 MeV/nucleon in inverse kinematics at the RIKEN Radioactive Isotope Beam Factory. Both the target and energy dependences of cross sections have been investigated systematically. It was found that the proton-induced cross sections at 196 MeV/nucleon are close to those for deuteron obtained at 118 MeV/nucleon for the light-mass products. The experimental data are compared with the SPACS semi-empirical parameterization and the PHITS calculations including both the intranuclear cascade and evaporation processes. Our data give a design goal of proton/deuteron flux for the transmutation of 107Pd using the spallation reaction. In addition, it is found that the spallation reaction at 118 MeV/nucleon may have an advantage over the 107Pd transmutation because of the low production of other long-lived radioactive isotopes.

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

The behaviour of transuranic mixed oxide fuel in a Candu-900 reactor

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

Morreale, A. C.; Ball, M. R.; Novog, D. R.

2012-07-01

The production of transuranic actinide fuels for use in current thermal reactors provides a useful intermediary step in closing the nuclear fuel cycle. Extraction of actinides reduces the longevity, radiation and heat loads of spent material. The burning of transuranic fuels in current reactors for a limited amount of cycles reduces the infrastructure demand for fast reactors and provides an effective synergy that can result in a reduction of as much as 95% of spent fuel waste while reducing the fast reactor infrastructure needed by a factor of almost 13.5 [1]. This paper examines the features of actinide mixed oxidemore » fuel, TRUMOX, in a CANDU{sup R}* nuclear reactor. The actinide concentrations used were based on extraction from 30 year cooled spent fuel and mixed with natural uranium in 3.1 wt% actinide MOX fuel. Full lattice cell modeling was performed using the WIMS-AECL code, super-cell calculations were analyzed in DRAGON and full core analysis was executed in the RFSP 2-group diffusion code. A time-average full core model was produced and analyzed for reactor coefficients, reactivity device worth and online fuelling impacts. The standard CANDU operational limits were maintained throughout operations. The TRUMOX fuel design achieved a burnup of 27.36 MWd/kg HE. A full TRUMOX fuelled CANDU was shown to operate within acceptable limits and provided a viable intermediary step for burning actinides. The recycling, reprocessing and reuse of spent fuels produces a much more sustainable and efficient nuclear fuel cycle. (authors)« less

Run-time scheduling and execution of loops on message passing machines

NASA Technical Reports Server (NTRS)

Crowley, Kay; Saltz, Joel; Mirchandaney, Ravi; Berryman, Harry

1989-01-01

Sparse system solvers and general purpose codes for solving partial differential equations are examples of the many types of problems whose irregularity can result in poor performance on distributed memory machines. Often, the data structures used in these problems are very flexible. Crucial details concerning loop dependences are encoded in these structures rather than being explicitly represented in the program. Good methods for parallelizing and partitioning these types of problems require assignment of computations in rather arbitrary ways. Naive implementations of programs on distributed memory machines requiring general loop partitions can be extremely inefficient. Instead, the scheduling mechanism needs to capture the data reference patterns of the loops in order to partition the problem. First, the indices assigned to each processor must be locally numbered. Next, it is necessary to precompute what information is needed by each processor at various points in the computation. The precomputed information is then used to generate an execution template designed to carry out the computation, communication, and partitioning of data, in an optimized manner. The design is presented for a general preprocessor and schedule executer, the structures of which do not vary, even though the details of the computation and of the type of information are problem dependent.

Run-time scheduling and execution of loops on message passing machines

NASA Technical Reports Server (NTRS)

Saltz, Joel; Crowley, Kathleen; Mirchandaney, Ravi; Berryman, Harry

1990-01-01

Sparse system solvers and general purpose codes for solving partial differential equations are examples of the many types of problems whose irregularity can result in poor performance on distributed memory machines. Often, the data structures used in these problems are very flexible. Crucial details concerning loop dependences are encoded in these structures rather than being explicitly represented in the program. Good methods for parallelizing and partitioning these types of problems require assignment of computations in rather arbitrary ways. Naive implementations of programs on distributed memory machines requiring general loop partitions can be extremely inefficient. Instead, the scheduling mechanism needs to capture the data reference patterns of the loops in order to partition the problem. First, the indices assigned to each processor must be locally numbered. Next, it is necessary to precompute what information is needed by each processor at various points in the computation. The precomputed information is then used to generate an execution template designed to carry out the computation, communication, and partitioning of data, in an optimized manner. The design is presented for a general preprocessor and schedule executer, the structures of which do not vary, even though the details of the computation and of the type of information are problem dependent.

METHOD FOR THE PREPARATION OF STABLE ACTINIDE METAL OXIDE-CONTAINING SLURRIES AND OF THE OXIDES THEREFOR

DOEpatents

Hansen, R.S.; Minturn, R.E.

1958-02-25

This patent deals with a method of preparing actinide metal oxides of a very fine particle size and of forming stable suspensions therefrom. The process consists of dissolving the nitrate of the actinide element in a combustible organic solvent, converting the solution obtained into a spray, and igniting the spray whereby an oxide powder is obtained. The oxide powder is then slurried in an aqueous soiution of a substance which is adsorbable by said oxides, dspersed in a colloid mill whereby a suspension is obtained, and electrodialyzed until a low spectiic conductance is reached.

Analogue Study of Actinide Transport at Sites in Russia

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

Novikov, A P; Simmons, A M; Halsey, W G

2003-02-12

The U. S. Department of Energy (DOE) and the Russian Academy of Sciences (RAS) are engaged in a three-year cooperative study to observe the behavior of actinides in the natural environment at selected disposal sites and/or contamination sites in Russia. The purpose is to develop experimental data and models for actinide speciation, mobilization and transport processes in support of geologic repository design, safety and performance analyses. Currently at the mid-point of the study, the accomplishments to date include: evaluation of existing data and data needs, site screening and selection, initial data acquisition, and development of preliminary conceptual models.

Method for extracting lanthanides and actinides from acid solutions by modification of Purex solvent

DOEpatents

Horwitz, E.P.; Kalina, D.G.

1984-05-21

A process has been developed for the extraction of multivalent lanthanide and actinide values from acidic waste solutions, and for the separation of these values from fission product and other values, which utilizes a new series of neutral bi-functional extractants, the alkyl(phenyl)-N, N-dialkylcarbamoylmethylphosphine oxides, in combination with a phase modifier to form an extraction solution. The addition of the extractant to the Purex process extractant, tri-n-butylphosphate in normal paraffin hydrocarbon diluent, will permit the extraction of multivalent lanthanide and actinide values from 0.1 to 12.0 molar acid solutions.

SOLVENT EXTRACTION PROCESS FOR SEPARATING ACTINIDE AND LANTHANIDE METAL VALUES

DOEpatents

Hildebrandt, R.A.; Hyman, H.H.; Vogler, S.

1962-08-14

A process of countercurrently extracting an aqueous mineral acid feed solution for the separation of actinides from lanthanides dissolved therern is described. The feed solution is made acid-defrcient with alkali metal hydroxide prior to.contact with acid extractant; during extraction, however, acid is transferred from organic to aqueous solution and the aqueous solution gradually becomes acid. The acid-deficient phase ' of the process promotes the extraction of the actinides, while the latter acid phase'' of the process improves retention of the lanthanides in the aqueous solution. This provides for an improved separation. (AEC)

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

Photochemical route to actinide-transition metal bonds: synthesis, characterization and reactivity of a series of thorium and uranium heterobimetallic complexes.

PubMed

Ward, Ashleigh L; Lukens, Wayne W; Lu, Connie C; Arnold, John

2014-03-05

A series of actinide-transition metal heterobimetallics has been prepared, featuring thorium, uranium, and cobalt. Complexes incorporating the binucleating ligand N[ο-(NHCH2P(i)Pr2)C6H4]3 with either Th(IV) (4) or U(IV) (5) and a carbonyl bridged [Co(CO)4](-) unit were synthesized from the corresponding actinide chlorides (Th: 2; U: 3) and Na[Co(CO)4]. Irradiation of the resulting isocarbonyls with ultraviolet light resulted in the formation of new species containing actinide-metal bonds in good yields (Th: 6; U: 7); this photolysis method provides a new approach to a relatively unusual class of complexes. Characterization by single-crystal X-ray diffraction revealed that elimination of the bridging carbonyl and formation of the metal-metal bond is accompanied by coordination of a phosphine arm from the N4P3 ligand to the cobalt center. Additionally, actinide-cobalt bonds of 3.0771(5) Å and 3.0319(7) Å for the thorium and uranium complexes, respectively, were observed. The solution-state behavior of the thorium complexes was evaluated using (1)H, (1)H-(1)H COSY, (31)P, and variable-temperature NMR spectroscopy. IR, UV-vis/NIR, and variable-temperature magnetic susceptibility measurements are also reported.

Photochemical route to actinide-transition metal bonds: synthesis, characterization and reactivity of a series of thorium and uranium heterobimetallic complexes

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

Ward, Ashleigh; Lukens, Wayne; Lu, Connie

2014-04-01

A series of actinide-transition metal heterobimetallics has been prepared, featuring thorium, uranium and cobalt. Complexes incorporating the binucleating ligand N[-(NHCH2PiPr2)C6H4]3 and Th(IV) (4) or U(IV) (5) with a carbonyl bridged [Co(CO)4]- unit were synthesized from the corresponding actinide chlorides (Th: 2; U: 3) and Na[Co(CO)4]. Irradiation of the isocarbonyls with ultraviolet light resulted in the formation of new species containing actinide-metal bonds in good yields (Th: 6; U: 7); this photolysis method provides a new approach to a relatively rare class of complexes. Characterization by single-crystal X-ray diffraction revealed that elimination of the bridging carbonyl is accompanied by coordination ofmore » a phosphine arm from the N4P3 ligand to the cobalt center. Additionally, actinide-cobalt bonds of 3.0771(5) and 3.0319(7) for the thorium and uranium complexes, respectively, were observed. The solution state behavior of the thorium complexes was evaluated using 1H, 1H-1H COSY, 31P and variable-temperature NMR spectroscopy. IR, UV-Vis/NIR, and variable-temperature magnetic susceptibility measurements are also reported.« less

Transmutation of skyrmions to half-solitons driven by the nonlinear optical spin Hall effect.

PubMed

Flayac, H; Solnyshkov, D D; Shelykh, I A; Malpuech, G

2013-01-04

We show that the spin domains, generated in the linear optical spin Hall effect by the analog of spin-orbit interaction for exciton polaritons, are associated with the formation of a Skyrmion lattice. In the nonlinear regime, the spin anisotropy of the polariton-polariton interactions results in a spatial compression of the domains and in a transmutation of the Skyrmions into oblique half-solitons. This phase transition is associated with both the focusing of the spin currents and the emergence of a strongly anisotropic emission pattern.

Mercury Phase II Study - Mercury Behavior across the High-Level Waste Evaporator System

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

Bannochie, C. J.; Crawford, C. L.; Jackson, D. G.

2016-06-17

The Mercury Program team’s effort continues to develop more fundamental information concerning mercury behavior across the liquid waste facilities and unit operations. Previously, the team examined the mercury chemistry across salt processing, including the Actinide Removal Process/Modular Caustic Side Solvent Extraction Unit (ARP/MCU), and the Defense Waste Processing Facility (DWPF) flowsheets. This report documents the data and understanding of mercury across the high level waste 2H and 3H evaporator systems.

Handling Data Skew in MapReduce Cluster by Using Partition Tuning

PubMed

Gao, Yufei; Zhou, Yanjie; Zhou, Bing; Shi, Lei; Zhang, Jiacai

2017-01-01

The healthcare industry has generated large amounts of data, and analyzing these has emerged as an important problem in recent years. The MapReduce programming model has been successfully used for big data analytics. However, data skew invariably occurs in big data analytics and seriously affects efficiency. To overcome the data skew problem in MapReduce, we have in the past proposed a data processing algorithm called Partition Tuning-based Skew Handling (PTSH). In comparison with the one-stage partitioning strategy used in the traditional MapReduce model, PTSH uses a two-stage strategy and the partition tuning method to disperse key-value pairs in virtual partitions and recombines each partition in case of data skew. The robustness and efficiency of the proposed algorithm were tested on a wide variety of simulated datasets and real healthcare datasets. The results showed that PTSH algorithm can handle data skew in MapReduce efficiently and improve the performance of MapReduce jobs in comparison with the native Hadoop, Closer, and locality-aware and fairness-aware key partitioning (LEEN). We also found that the time needed for rule extraction can be reduced significantly by adopting the PTSH algorithm, since it is more suitable for association rule mining (ARM) on healthcare data. © 2017 Yufei Gao et al.

Handling Data Skew in MapReduce Cluster by Using Partition Tuning.

PubMed

Gao, Yufei; Zhou, Yanjie; Zhou, Bing; Shi, Lei; Zhang, Jiacai

2017-01-01

The healthcare industry has generated large amounts of data, and analyzing these has emerged as an important problem in recent years. The MapReduce programming model has been successfully used for big data analytics. However, data skew invariably occurs in big data analytics and seriously affects efficiency. To overcome the data skew problem in MapReduce, we have in the past proposed a data processing algorithm called Partition Tuning-based Skew Handling (PTSH). In comparison with the one-stage partitioning strategy used in the traditional MapReduce model, PTSH uses a two-stage strategy and the partition tuning method to disperse key-value pairs in virtual partitions and recombines each partition in case of data skew. The robustness and efficiency of the proposed algorithm were tested on a wide variety of simulated datasets and real healthcare datasets. The results showed that PTSH algorithm can handle data skew in MapReduce efficiently and improve the performance of MapReduce jobs in comparison with the native Hadoop, Closer, and locality-aware and fairness-aware key partitioning (LEEN). We also found that the time needed for rule extraction can be reduced significantly by adopting the PTSH algorithm, since it is more suitable for association rule mining (ARM) on healthcare data.

Handling Data Skew in MapReduce Cluster by Using Partition Tuning

PubMed Central

Zhou, Yanjie; Zhou, Bing; Shi, Lei

2017-01-01

The healthcare industry has generated large amounts of data, and analyzing these has emerged as an important problem in recent years. The MapReduce programming model has been successfully used for big data analytics. However, data skew invariably occurs in big data analytics and seriously affects efficiency. To overcome the data skew problem in MapReduce, we have in the past proposed a data processing algorithm called Partition Tuning-based Skew Handling (PTSH). In comparison with the one-stage partitioning strategy used in the traditional MapReduce model, PTSH uses a two-stage strategy and the partition tuning method to disperse key-value pairs in virtual partitions and recombines each partition in case of data skew. The robustness and efficiency of the proposed algorithm were tested on a wide variety of simulated datasets and real healthcare datasets. The results showed that PTSH algorithm can handle data skew in MapReduce efficiently and improve the performance of MapReduce jobs in comparison with the native Hadoop, Closer, and locality-aware and fairness-aware key partitioning (LEEN). We also found that the time needed for rule extraction can be reduced significantly by adopting the PTSH algorithm, since it is more suitable for association rule mining (ARM) on healthcare data. PMID:29065568

The Installation Restoration Program Toxicology Guide. Volume 4

DTIC Science & Technology

1989-07-01

64.15 64-5 JP-4 Fuel-Water Partition Coefficients (K,) for Selected Hydrocarbons .......................... 64-20 04-6 Acute Toxicity of Components of JP...65.11 65-3 Equilibrium Partitioning of Select Gasoline Hydrocarbons in Model Environments ............... 65-14 65-4 Acute Toxicity of Components o...66-27 66-5 Acute Toxicity of Components of Fuel Oils ............ 66-37 67-1 Composition Dat,- for Stoddard Solvent

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.

Liquid-liquid extraction of actinides, lanthanides, and fission products by use of ionic liquids: from discovery to understanding.

PubMed

Billard, Isabelle; Ouadi, Ali; Gaillard, Clotilde

2011-06-01

Liquid-liquid extraction of actinides and lanthanides by use of ionic liquids is reviewed, considering, first, phenomenological aspects, then looking more deeply at the various mechanisms. Future trends in this developing field are presented.

Development of ion beam sputtering techniques for actinide target preparation

NASA Astrophysics Data System (ADS)

Aaron, W. S.; Zevenbergen, L. A.; Adair, H. L.

1985-06-01

Ion beam sputtering is a routine method for the preparation of thin films used as targets because it allows the use of a minimum quantity of starting material, and losses are much lower than most other vacuum deposition techniques. Work is underway in the Isotope Research Materials Laboratory (IRML) at ORNL to develop the techniques that will make the preparation of actinide targets up to 100 μg/cm 2 by ion beam sputtering a routinely available service from IRML. The preparation of the actinide material in a form suitable for sputtering is a key to this technique, as is designing a sputtering system that allows the flexibility required for custom-ordered target production. At present, development work is being conducted on low-activity actinides in a bench-top system. The system will then be installed in a hood or glove box approved for radioactive materials handling where processing of radium, actinium, and plutonium isotopes among others will be performed.

Molecular orbital studies of the bonding in heavy element organometallics: Progress report

NASA Astrophysics Data System (ADS)

Bursten, B. E.

1988-03-01

Over the past two years we have made considerable progress in the understanding of the bonding in heavy element mononuclear and binuclear complexes. For mononuclear complexes, our strategy has been to study the orbital interactions between the actinide metal center and the surrounding ligands. One particular system which has been studied extensively is X sub 3 AnL (where X = Cp, Cl, NH sub 2 ; An = actinide; and L = neutral or anionic ligand). We are interested not only in the mechanics of the An-X orbital interactions, but also how the relative donor characteristics of X may influence coordination of the fourth ligand L to the actinide. For binuclear systems, we are interested not only in homobimetallic complexes, but also in heterobimetallic complexes containing actinides and transition metals. In order to make the calculations of such large systems tractable, we have transferred the X-alpha-SW codes to the newly acquired Cray XMP24 at the Ohio Supercomputer Center. This has resulted in significant savings of money and time.

Emergence of californium as the second transitional element in the actinide series

DOE PAGES

Cary, Samantha K.; Vasiliu, Monica; Baumbach, Ryan E.; ...

2015-04-16

A break in periodicity occurs in the actinide series between plutonium and americium as the result of the localization of 5f electrons. The subsequent chemistry of later actinides is thought to closely parallel lanthanides in that bonding is expected to be ionic and complexation should not substantially alter the electronic structure of the metal ions. Here we demonstrate that ligation of californium(III) by a pyridine derivative results in significant deviations in the properties of the resultant complex with respect to that predicted for the free ion. We expand on this by characterizing the americium and curium analogues for comparison, andmore » show that these pronounced effects result from a second transition in periodicity in the actinide series that occurs, in part, because of the stabilization of the divalent oxidation state. As a result, the metastability of californium(II) is responsible for many of the unusual properties of californium including the green photoluminescence.« less

A unified picture of the crystal structures of metals

NASA Astrophysics Data System (ADS)

Söderlind, Per; Eriksson, Olle; Johansson, Börje; Wills, J. M.; Boring, A. M.

1995-04-01

THE crystal structures of the light actinides have intrigued physicists and chemists for several decades1. Simple metals and transition metals have close-packed, high-symmetry structures, such as body-centred cubic, face-centred cubic and hexagonal close packing. In contrast, the structures of the light actinides are very loosely packed and of low symmetry-tetragonal, orthorhombic and monoclinic. To understand these differences, we have performed total-energy calculations, as a function of volume, for both high-and low-symmetry structures of a simple metal (aluminium), a non-magnetic transition metal (niobium), a ferromagnetic transition metal (iron) and a light actinide (uranium). We find that the crystal structure of all of these metals is determined by the balance between electrostatic (Madelung) interactions, which favour high symmetry, and a Peierls distortion of the crystal lattice, which favours low symmetry. We show that simple metals and transition metals can adopt low-symmetry structures on expansion of the lattice; and we predict that, conversely, the light actinides will undergo transitions to structures of higher symmetry on compression.

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

Method for decontamination of nickel-fluoride-coated nickel containing actinide-metal fluorides

DOEpatents

Windt, N.F.; Williams, J.L.

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 contianing 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.

Actinide and lanthanide separation process (ALSEP)

DOEpatents

Guelis, Artem V.

2013-01-15

The process of the invention is the separation of minor actinides from lanthanides in a fluid mixture comprising, fission products, lanthanides, minor actinides, rare earth elements, nitric acid and water by addition of an organic chelating aid to the fluid; extracting the fluid with a solvent comprising a first extractant, a second extractant and an organic diluent to form an organic extractant stream and an aqueous raffinate. Scrubbing the organic stream with a dicarboxylic acid and a chelating agent to form a scrubber discharge. The scrubber discharge is stripped with a simple buffering agent and a second chelating agent in the pH range of 2.5 to 6.1 to produce actinide and lanthanide streams and spent organic diluents. The first extractant is selected from bis(2-ethylhexyl)hydrogen phosphate (HDEHP) and mono(2-ethylhexyl)2-ethylhexyl phosphonate (HEH(EHP)) and the second extractant is selected from N,N,N,N-tetra-2-ethylhexyl diglycol amide (TEHDGA) and N,N,N',N'-tetraoctyl-3-oxapentanediamide (TODGA).

New Insight into Nuclear Reactions in Solids

NASA Astrophysics Data System (ADS)

Miley, George H.

2003-04-01

Earlier work by the author disclosed evidence for nuclear transmutations in multi-layer thin-film Ni/Pd electrodes loaded to a high ratio of hydrogen/film metal using an electrolytic technique [1]. Non-natural isotopes abundances were found for select products. A distinctive characteristic of this and similar experiments by others is a product yield curve vs. mass with four high yield peaks distributed between low and high masses. Attempts to explain this observation have evolved around the original swimming electron layer (SEL) theory [2]. In addition, CR-39 track detector measurements have revealed low-level emission of 1.6 MeV protons and 16 MeV alpha particles from the front face of the thin film electrodes during runs [3]. Most recently Mitsubishi Corp. researchers have reported a real-time transmutation measurement using built-in XPS diagnostics where a surface layer of Sr-88 was transmuted into Mo-96 over a 200 hour run period during the diffusion of deuterium through a multi-layer thin-film Pd/CaO substrate [4]. Likewise in a companion experiment, Cs-133 was transmuted into Pr-141. These products exhibit a large deviation from natural isotopic abundance, and the characteristic signature is a mass change of 8 and charge change of 4. These various phenomena along with a preliminary theory involving SEL and orbital mixing will be presented. The objective is to provide a unified understanding of both types of experiments presented in Refs. 1 and 3. [1] G.H. Miley and J. A. Patterson, "Nuclear Transmutations in Thin-Film Nickel Coatings Undergoing Electrolysis," J. New Energy, 1, 3, 5-30 (1996). [2] H. Hora, et al., "Screening in Cold Fusion Derived from D D Reactions," Physics Ltrs. A, 175, 138-143, (1993). [3] A. Lipson, et al., "In-situ long - range alpha particles and X-ray detection in Pd thin film-cathodes during electrolysis in, Li2SO4/H2O, Bult. APS, 47, 1,Pt. II, 1219, Indianapolis, (2002). [4] Y. Iwamura, T. Itoh, et al., "Low energy nuclear reaction induced by D gas permeation through multilayer film," Japanese J. Physics, 41, pt. 1, 7A, 4642, (2002).

Centrifugal Tensioned Metastable Fluid Detectors for Trace Radiation Sources: Experimental Verification and Military Employment

DTIC Science & Technology

2016-06-01

used in both CTMFD and Beckman LS 6500 Scintillation System. Actinide   Mass  of  Nalgene  (g)  Mass  of  Cap (g)  Mass  of  Nalgene,  Cap, 50 mL...both CTMFD and Beckman LS 6500 Scintillation System. Actinide   Mass  of  Nalgene  and Cap  (g)  Mass  of  Nalgene, Cap,  50 mL Acetone  (g)  Mass  of...testing comparing the CTMFD’s capabilities of actinide spectroscopy and neutron detection against other detection systems with similar capabilities. The

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.

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.

Transmutation approximations for the application of hybrid Monte Carlo/deterministic neutron transport to shutdown dose rate analysis

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

Biondo, Elliott D.; Wilson, Paul P. H.

In fusion energy systems (FES) neutrons born from burning plasma activate system components. The photon dose rate after shutdown from resulting radionuclides must be quantified. This shutdown dose rate (SDR) is calculated by coupling neutron transport, activation analysis, and photon transport. The size, complexity, and attenuating configuration of FES motivate the use of hybrid Monte Carlo (MC)/deterministic neutron transport. The Multi-Step Consistent Adjoint Driven Importance Sampling (MS-CADIS) method can be used to optimize MC neutron transport for coupled multiphysics problems, including SDR analysis, using deterministic estimates of adjoint flux distributions. When used for SDR analysis, MS-CADIS requires the formulation ofmore » an adjoint neutron source that approximates the transmutation process. In this work, transmutation approximations are used to derive a solution for this adjoint neutron source. It is shown that these approximations are reasonably met for typical FES neutron spectra and materials over a range of irradiation scenarios. When these approximations are met, the Groupwise Transmutation (GT)-CADIS method, proposed here, can be used effectively. GT-CADIS is an implementation of the MS-CADIS method for SDR analysis that uses a series of single-energy-group irradiations to calculate the adjoint neutron source. For a simple SDR problem, GT-CADIS provides speedups of 200 100 relative to global variance reduction with the Forward-Weighted (FW)-CADIS method and 9 ± 5 • 104 relative to analog. As a result, this work shows that GT-CADIS is broadly applicable to FES problems and will significantly reduce the computational resources necessary for SDR analysis.« less

Transmutation approximations for the application of hybrid Monte Carlo/deterministic neutron transport to shutdown dose rate analysis

DOE PAGES

Biondo, Elliott D.; Wilson, Paul P. H.

2017-05-08

In fusion energy systems (FES) neutrons born from burning plasma activate system components. The photon dose rate after shutdown from resulting radionuclides must be quantified. This shutdown dose rate (SDR) is calculated by coupling neutron transport, activation analysis, and photon transport. The size, complexity, and attenuating configuration of FES motivate the use of hybrid Monte Carlo (MC)/deterministic neutron transport. The Multi-Step Consistent Adjoint Driven Importance Sampling (MS-CADIS) method can be used to optimize MC neutron transport for coupled multiphysics problems, including SDR analysis, using deterministic estimates of adjoint flux distributions. When used for SDR analysis, MS-CADIS requires the formulation ofmore » an adjoint neutron source that approximates the transmutation process. In this work, transmutation approximations are used to derive a solution for this adjoint neutron source. It is shown that these approximations are reasonably met for typical FES neutron spectra and materials over a range of irradiation scenarios. When these approximations are met, the Groupwise Transmutation (GT)-CADIS method, proposed here, can be used effectively. GT-CADIS is an implementation of the MS-CADIS method for SDR analysis that uses a series of single-energy-group irradiations to calculate the adjoint neutron source. For a simple SDR problem, GT-CADIS provides speedups of 200 100 relative to global variance reduction with the Forward-Weighted (FW)-CADIS method and 9 ± 5 • 104 relative to analog. As a result, this work shows that GT-CADIS is broadly applicable to FES problems and will significantly reduce the computational resources necessary for SDR analysis.« less

Strainrange partitioning behavior of the nickel-base superalloys, Rene' 80 and in 100

NASA Technical Reports Server (NTRS)

Halford, G. R.; Nachtigall, A. J.

1978-01-01

A study was made to assess the ability of the method of Strainrange Partitioning (SRP) to both correlate and predict high-temperature, low cycle fatigue lives of nickel base superalloys for gas turbine applications. The partitioned strainrange versus life relationships for uncoated Rene' 80 and cast IN 100 were also determined from the ductility normalized-Strainrange Partitioning equations. These were used to predict the cyclic lives of the baseline tests. The life predictability of the method was verified for cast IN 100 by applying the baseline results to the cyclic life prediction of a series of complex strain cycling tests with multiple hold periods at constant strain. It was concluded that the method of SRP can correlate and predict the cyclic lives of laboratory specimens of the nickel base superalloys evaluated in this program.

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.

Trace Uranium Partitioning in a Multiphase Nano-FeOOH System.

PubMed

McBriarty, Martin E; Soltis, Jennifer A; Kerisit, Sebastien; Qafoku, Odeta; Bowden, Mark E; Bylaska, Eric J; De Yoreo, James J; Ilton, Eugene S

2017-05-02

The characterization of trace elements in minerals using extended X-ray absorption fine structure (EXAFS) spectroscopy constitutes a first step toward understanding how impurities and contaminants interact with the host phase and the environment. However, limitations to EXAFS interpretation complicate the analysis of trace concentrations of impurities that are distributed across multiple phases in a heterogeneous system. Ab initio molecular dynamics (AIMD)-informed EXAFS analysis was employed to investigate the immobilization of trace uranium associated with nanophase iron (oxyhydr)oxides, a model system for the geochemical sequestration of radiotoxic actinides. The reductive transformation of ferrihydrite [Fe(OH) 3 ] to nanoparticulate iron oxyhydroxide minerals in the presence of uranyl (UO 2 ) 2+ (aq) resulted in the preferential incorporation of U into goethite (α-FeOOH) over lepidocrocite (γ-FeOOH), even though reaction conditions favored the formation of excess lepidocrocite. This unexpected result is supported by atomically resolved transmission electron microscopy. We demonstrate how AIMD-informed EXAFS analysis lifts the strict statistical limitations and uncertainty of traditional shell-by-shell EXAFS fitting, enabling the detailed characterization of the local bonding environment, charge compensation mechanisms, and oxidation states of polyvalent impurities in complex multiphase mineral systems.

Spontaneous Partitioning of Californium from Curium: Curious Cases from the Crystallization of Curium Coordination Complexes

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

Cary, Samantha K.; Silver, Mark A.; Liu, Guokui

The reaction of 248CmCl3 with excess 2,6-pyridinedicarboxylic acid (DPA) under mild solvothermal conditions results in crystallization of the tris-chelate complex Cm(HDPA)3·H2O. Approximately half of the curium remains in solution at the end of this process, and evaporation of the mother liquor results in crystallization of the bis-chelate complex [Cm(HDPA)- (H2DPA)(H2O)2Cl]Cl·2H2O. 248Cm is the daughter of the α decay of 252Cf and is extracted in high purity from this parent. However, trace amounts of 249,250,251Cf are still present in all samples of 248Cm. During the crystallization of Cm(HDPA)3·H2O and [Cm(HDPA)(H2DPA)(H2O)2Cl]Cl·2H2O, californium(III) spontaneously separates itself from the curium complexes and is foundmore » doped within crystals of DPA in the form of Cf(HDPA)3. These results add to the growing body of evidence that the chemistry of californium is fundamentally different from that of earlier actinides.« less

Trace Uranium Partitioning in a Multiphase Nano-FeOOH System

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

McBriarty, Martin E.; Soltis, Jennifer A.; Kerisit, Sebastien

The characterization of trace elements in minerals using extended X-ray absorption fine structure (EXAFS) spectroscopy constitutes a first step toward understanding how impurities and contaminants interact with the host phase and the environment. However, limitations to EXAFS interpretation complicate the analysis of trace concentrations of impurities that are distributed across multiple phases in a heterogeneous system. Ab initio molecular dynamics (AIMD)-informed EXAFS analysis was employed to investigate the immobilization of trace uranium associated with nanophase iron (oxyhydr)oxides, a model system for the geochemical sequestration of radiotoxic actinides. The reductive transformation of ferrihydrite [Fe(OH)3] to nanoparticulate iron oxyhydroxide minerals in themore » presence of uranyl (UO 2) 2+(aq) resulted in the preferential incorporation of U into goethite (α-FeOOH) over lepidocrocite (γ-FeOOH), even though reaction conditions favored the formation of excess lepidocrocite. This unexpected result is supported by atomically resolved transmission electron microscopy. We demonstrate how AIMD-informed EXAFS analysis lifts the strict statistical limitations and uncertainty of traditional shell-by-shell EXAFS fitting, enabling the detailed characterization of the local bonding environment, charge compensation mechanisms, and oxidation states of polyvalent impurities in complex multiphase mineral systems.« less

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

Evaluation of possible physical-chemical processes that might lead to separations of actinides in ORNL waste tanks

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

Del Cul, G.D.; Toth, L.M.; Bond, W.D.

The concern that there might be some physical-chemical process which would lead to a separation of the poisoning actinides ({sup 232}Th, {sup 238}U) from the fissionable ones ({sup 239}Pu, {sup 235}U) in waste storage tanks at Oak Ridge National Laboratory has led to a paper study of potential separations processes involving these elements. At the relatively high pH values (>8), the actinides are normally present as precipitated hydroxides. Mechanisms that might then selectively dissolve and reprecipitate the actinides through thermal processes or additions of reagents were addressed. Although redox reactions, pH changes, and complexation reactions were all considered, only themore » last type was regarded as having any significant probability. Furthermore, only carbonate accumulation, through continual unmonitored air sparging of the tank contents, could credibly account for gross transport and separation of the actinide components. From the large amount of equilibrium data in the literature, concentration differences in Th, U, and Pu due to carbonate complexation as a function of pH have been presented to demonstrate this phenomenon. While the carbonate effect does represent a potential separations process, control of long-term air sparging and solution pH, accompanied by routine determinations of soluble carbonate concentration, should ensure that this separations process does not occur.« less

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.

Study of extraterrestrial disposal of radioactive wastes. Part 3: Preliminary feasibility screening study of space disposal of the actinide radioactive wastes with 1 percent and 0.1 percent fission product contamination

NASA Technical Reports Server (NTRS)

Hyland, R. E.; Wohl, M. L.; Finnegan, P. M.

1973-01-01

A preliminary study was conducted of the feasibility of space disposal of the actinide class of radioactive waste material. This waste was assumed to contain 1 and 0.1 percent residual fission products, since it may not be feasible to completely separate the actinides. The actinides are a small fraction of the total waste but they remain radioactive much longer than the other wastes and must be isolated from human encounter for tens of thousands of years. Results indicate that space disposal is promising but more study is required, particularly in the area of safety. The minimum cost of space transportation would increase the consumer electric utility bill by the order of 1 percent for earth escape and 3 percent for solar escape. The waste package in this phase of the study was designed for normal operating conditions only; the design of next phase of the study will include provisions for accident safety. The number of shuttle launches per year required to dispose of all U.S. generated actinide waste with 0.1 percent residual fission products varies between 3 and 15 in 1985 and between 25 and 110 by 2000. The lower values assume earth escape (solar orbit) and the higher values are for escape from the solar system.

Object kinetic Monte Carlo model for neutron and ion irradiation in tungsten: Impact of transmutation and carbon impurities

NASA Astrophysics Data System (ADS)

Castin, N.; Bonny, G.; Bakaev, A.; Ortiz, C. J.; Sand, A. E.; Terentyev, D.

2018-03-01

We upgrade our object kinetic Monte Carlo (OKMC) model, aimed at describing the microstructural evolution in tungsten (W) under neutron and ion irradiation. Two main improvements are proposed based on recently published atomistic data: (a) interstitial carbon impurities, and their interaction with radiation-induced defects (point defect clusters and loops), are more accurately parameterized thanks to ab initio findings; (b) W transmutation to rhenium (Re) upon neutron irradiation, impacting the diffusivity of radiation defects, is included, also relying on recent atomistic data. These essential amendments highly improve the portability of our OKMC model, providing a description for the formation of SIA-type loops under different irradiation conditions. The model is applied to simulate neutron and ion irradiation in pure W samples, in a wide range of fluxes and temperatures. We demonstrate that it performs a realistic prediction of the population of TEM-visible voids and loops, as compared to experimental evidence. The impact of the transmutation of W to Re, and of carbon trapping, is assessed.

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

Capote, R.; Chen, Y. -J.; Hambsch, F. -J.

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.

Sarment: Python modules for HMM analysis and partitioning of sequences.

PubMed

Guéguen, Laurent

2005-08-15

Sarment is a package of Python modules for easy building and manipulation of sequence segmentations. It provides efficient implementation of usual algorithms for hidden Markov Model computation, as well as for maximal predictive partitioning. Owing to its very large variety of criteria for computing segmentations, Sarment can handle many kinds of models. Because of object-oriented programming, the results of the segmentation are very easy tomanipulate.

Applying graph partitioning methods in measurement-based dynamic load balancing

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

Bhatele, Abhinav; Fourestier, Sebastien; Menon, Harshitha

Load imbalance leads to an increasing waste of resources as an application is scaled to more and more processors. Achieving the best parallel efficiency for a program requires optimal load balancing which is a NP-hard problem. However, finding near-optimal solutions to this problem for complex computational science and engineering applications is becoming increasingly important. Charm++, a migratable objects based programming model, provides a measurement-based dynamic load balancing framework. This framework instruments and then migrates over-decomposed objects to balance computational load and communication at runtime. This paper explores the use of graph partitioning algorithms, traditionally used for partitioning physical domains/meshes, formore » measurement-based dynamic load balancing of parallel applications. In particular, we present repartitioning methods developed in a graph partitioning toolbox called SCOTCH that consider the previous mapping to minimize migration costs. We also discuss a new imbalance reduction algorithm for graphs with irregular load distributions. We compare several load balancing algorithms using microbenchmarks on Intrepid and Ranger and evaluate the effect of communication, number of cores and number of objects on the benefit achieved from load balancing. New algorithms developed in SCOTCH lead to better performance compared to the METIS partitioners for several cases, both in terms of the application execution time and fewer number of objects migrated.« less

Correlations, soliton modes, and non-Hermitian linear mode transmutation in the one-dimensional noisy Burgers equation.

PubMed

Fogedby, Hans C

2003-08-01

Using the previously developed canonical phase space approach applied to the noisy Burgers equation in one dimension, we discuss in detail the growth morphology in terms of nonlinear soliton modes and superimposed linear modes. We moreover analyze the non-Hermitian character of the linear mode spectrum and the associated dynamical pinning, and mode transmutation from diffusive to propagating behavior induced by the solitons. We discuss the anomalous diffusion of growth modes, switching and pathways, correlations in the multisoliton sector, and in detail the correlations and scaling properties in the two-soliton sector.

Neutron-transmutation-doped germanium bolometers

NASA Technical Reports Server (NTRS)

Palaio, N. P.; Rodder, M.; Haller, E. E.; Kreysa, E.

1983-01-01

Six slices of ultra-pure germanium were irradiated with thermal neutron fluences between 7.5 x 10 to the 16th and 1.88 x 10 to the 18th per sq cm. After thermal annealing the resistivity was measured down to low temperatures (less than 4.2 K) and found to follow the relationship rho = rho sub 0 exp(Delta/T) in the hopping conduction regime. Also, several junction FETs were tested for noise performance at room temperature and in an insulating housing in a 4.2 K cryostat. These FETs will be used as first stage amplifiers for neutron-transmutation-doped germanium bolometers.

Dimensional Transmutation by Monopole Condensation in QCD

NASA Astrophysics Data System (ADS)

Cho, Y. M.

2015-01-01

The dimensional transmutation by the monopole condensation in QCD is reviewed. Using Abelian projection of the gauge potential which projects out the monopole potential gauge independently, we we show that there are two types of gluons: the color neutral binding gluons which plays the role of the confining agent and the colored valence gluons which become confined prisoners. With this we calculate the one-loop QCD effective potential and show the monopole condensation becomes the true vacuum of QCD. We propose to test the existence of two types of gluons experimentally by re-analyzing the existing gluon jets data.

Computer programs to characterize alloys and predict cyclic life using the total strain version of strainrange partitioning: Tutorial and users manual, version 1.0

NASA Technical Reports Server (NTRS)

Saltsman, James F.

1992-01-01

This manual presents computer programs for characterizing and predicting fatigue and creep-fatigue resistance of metallic materials in the high-temperature, long-life regime for isothermal and nonisothermal fatigue. The programs use the total strain version of Strainrange Partitioning (TS-SRP). An extensive database has also been developed in a parallel effort. This database is probably the largest source of high-temperature, creep-fatigue test data available in the public domain and can be used with other life prediction methods as well. This users manual, software, and database are all in the public domain and are available through COSMIC (382 East Broad Street, Athens, GA 30602; (404) 542-3265, FAX (404) 542-4807). Two disks accompany this manual. The first disk contains the source code, executable files, and sample output from these programs. The second disk contains the creep-fatigue data in a format compatible with these programs.

Theory of Photoemission in Actinides

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

Svane, Axel

2008-07-01

A theory is presented which describes the photoemission spectra of actinide compounds starting from the atomic limit of isolated actinide ions. The multiplets of the ion are calculated and an additional term is introduced to describe the interaction with the sea of conduction electrons. This leads to complex mixed-valent ground states, which describes well the rich spectrum observed for PuSe. In particular, the three-peak feature, which is often seen in Pu and Pu compounds in the vicinity of the Fermi level originates from f{sup 6} {yields} f{sup 5} emission. The theory is further applied to PuSb, PuCoGa{sub 5} and Am.more » (author)« less

Method for extracting lanthanides and actinides from acid solutions by modification of purex solvent

DOEpatents

Horwitz, E. Philip; Kalina, Dale G.

1986-01-01

A process for the recovery of actinide and lanthanide values from aqueous solutions with an extraction solution containing 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 and phase modifiers in a water-immiscible hydrocarbon diluent. The addition of the extractant to the Purex process extractant, tri-n-butylphosphate in normal paraffin hydrocarbon diluent, will permit the extraction of multivalent lanthanide and actinide values from 0.1 to 12.0 molar acid solutions.

SEPARATION OF TRANSURANIC ELEMENTS FROM RARE EARTH COMPOUNDS

DOEpatents

Kohman, T.P.

1961-11-21

A process of separating neptunium and plutonium values from rare earths and alkaline earth fission products present on a solid mixed actinide carrier (Th or U(IV) oxalate or fluoride) --fission product carrier (LaF/sub 3/, CeF/sub 3/, SrF/sub 2/, CaF/sub 2/, YF/sub 3/, La oxalate, cerous oxalate, Sr oxalate, Ca oxalate or Y oxalate) by extraction of the actinides at elevated temperature with a solution of ammonium fluoride and/or ammonium oxalate is described. Separation of the fission-product-containing carriers from the actinide solution formed and precipitation of the neptunium and plutonium from the solution with mineral acid are also accomplished. (AEC)

Dynamic Airspace Configuration

NASA Technical Reports Server (NTRS)

Bloem, Michael J.

2014-01-01

In air traffic management systems, airspace is partitioned into regions in part to distribute the tasks associated with managing air traffic among different systems and people. These regions, as well as the systems and people allocated to each, are changed dynamically so that air traffic can be safely and efficiently managed. It is expected that new air traffic control systems will enable greater flexibility in how airspace is partitioned and how resources are allocated to airspace regions. In this talk, I will begin by providing an overview of some previous work and open questions in Dynamic Airspace Configuration research, which is concerned with how to partition airspace and assign resources to regions of airspace. For example, I will introduce airspace partitioning algorithms based on clustering, integer programming optimization, and computational geometry. I will conclude by discussing the development of a tablet-based tool that is intended to help air traffic controller supervisors configure airspace and controllers in current operations.

Actinide Corroles: Synthesis and Characterization of Thorium(IV) and Uranium(IV) bis(-chloride) Dimers

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

Ward, Ashleigh L.; Buckley, Heather L.; Gryko, Daniel T.

2013-12-01

The first synthesis and structural characterization of actinide corroles is presented. Thorium(IV) and uranium(IV) macrocycles of Mes2(p-OMePh)corrole were synthesised and characterized by single-crystal X-ray diffraction, UV-Visible spectroscopy, variable-temperature 1H NMR, ESI mass spectrometry and cyclic voltammetry.

Titanium Pyrophosphate for Removal of Trivalent Heavy Metals and Actinides Simulated by Retention of Europium

PubMed Central

Flores-Espinosa, Rosa María; Ordoñez-Regil, Eduardo; Fernández-Valverde, Suilma Marisela

2017-01-01

This work addresses the synthesis of titanium pyrophosphate, as well as the characterization and evaluation of the sorption process of europium, for removal of trivalent heavy metals and actinides simulate. The evaluation of the surface properties of titanium pyrophosphate was carried out determining the surface roughness and surface acidity constants. The values obtained from the determination of the surface roughness of the synthesized solid indicate that the surface of the material presents itself as slightly smooth. The FITEQL program was used to fit the experimental titration curves to obtain the surface acidity constants: log⁡K+ = 3.59 ± 0.06 and log⁡K− = −3.90 ± 0.05. The results of sorption kinetics evidenced that the pseudo-order model explains the retention process of europium, in which the initial sorption velocity was 8.3 × 10−4 mg g−1 min−1 and kinetic constant was 1.8 × 10−3 g mg min−1. The maximum sorption capacity was 0.6 mg g−1. The results obtained from sorption edge showed the existence of two bidentate complexes on the surface. PMID:28785720

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

Burning high-level TRU waste in fusion fission reactors

NASA Astrophysics Data System (ADS)

Shen, Yaosong

2016-09-01

Recently, the concept of actinide burning instead of a once-through fuel cycle for disposing spent nuclear fuel seems to get much more attention. A new method of burning high-level transuranic (TRU) waste combined with Thorium-Uranium (Th-U) fuel in the subcritical reactors driven by external fusion neutron sources is proposed in this paper. The thorium-based TRU fuel burns all of the long-lived actinides via a hard neutron spectrum while outputting power. A one-dimensional model of the reactor concept was built by means of the ONESN_BURN code with new data libraries. The numerical results included actinide radioactivity, biological hazard potential, and much higher burnup rate of high-level transuranic waste. The comparison of the fusion-fission reactor with the thermal reactor shows that the harder neutron spectrum is more efficient than the soft. The Th-U cycle produces less TRU, less radiotoxicity and fewer long-lived actinides. The Th-U cycle provides breeding of 233U with a long operation time (>20 years), hence significantly reducing the reactivity swing while improving safety and burnup.

Assessment for advanced fuel cycle options in CANDU

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

Morreale, A.C.; Luxat, J.C.; Friedlander, Y.

2013-07-01

The possible options for advanced fuel cycles in CANDU reactors including actinide burning options and thorium cycles were explored and are feasible options to increase the efficiency of uranium utilization and help close the fuel cycle. The actinide burning TRUMOX approach uses a mixed oxide fuel of reprocessed transuranic actinides from PWR spent fuel blended with natural uranium in the CANDU-900 reactor. This system reduced actinide content by 35% and decreased natural uranium consumption by 24% over a PWR once through cycle. The thorium cycles evaluated used two CANDU-900 units, a generator and a burner unit along with a drivermore » fuel feedstock. The driver fuels included plutonium reprocessed from PWR, from CANDU and low enriched uranium (LEU). All three cycles were effective options and reduced natural uranium consumption over a PWR once through cycle. The LEU driven system saw the largest reduction with a 94% savings while the plutonium driven cycles achieved 75% savings for PWR and 87% for CANDU. The high neutron economy, online fuelling and flexible compact fuel make the CANDU system an ideal reactor platform for many advanced fuel cycles.« less

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).

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

Properties of pure single crystals of actinide compounds

NASA Astrophysics Data System (ADS)

Vogt, O.

1989-07-01

Actinide research started with substances of poor quality and a multitude of "unexplainable" results mostly found on powder samples of doubtful quality exerted some pressure on the crystal growers. As an example we may mention the measurements on UP. Type I antiferromagnetism was found below 123 K by neutron diffraction experiments on powdered samples. At 23 K another transition becomes apparent in susceptibility measurements. The change of the magnetic moments associated with this transition remained unexplained. It was only after the discovery of multi k structures in other actinide compounds that the need was seen to perform even inelastic neutron diffraction experiments on single crystals so that finally the true nature of the transition in UP could be revealed. NpAs is another illustrative example for the fact that sometimes it takes decades to get a clear understanding for things even so simple as macroscopic magnetic properties. The main reason for the need of single crystals is certainly the anisotropy of the magnetic moment encountered in all actinide compounds. Self-heating effects may prevent research on big crystals or might call for isotopic purity of certain samples.

Lanthanide and actinide chemistry at high C/O ratios in the solar nebula

NASA Technical Reports Server (NTRS)

Lodders, Katharina; Fegley, Bruce, Jr.

1993-01-01

Chemical equilibrium calculations were performed to study the condensation chemistry of the REE and actinides under the highly reducing conditions which are necessary for the formation of the enstatite chondrites. Our calculations confirm that the REE and actinides condensed into oldhamite (CaS), the major REE and actinide host phase in enstatite chondrites, at a carbon-oxygen (C/O) ratio not less than 1 in an otherwise solar gas. Five basic types of REE abundance patterns, several of which are analogous to REE abundance patterns observed in the Ca, Al-rich inclusions in carbonaceous chondrites, are predicted to occur in meteoritic oldhamites. All of the reported REE patterns in oldhamites in enstatite chondrites can be interpreted in terms of our condensation calculations. The observed patterns fall into three of the five predicted categories. The reported Th and U enrichments and ratios in meteoritic oldhamites are also consistent with predictions of the condensation calculations. Pure REE sulfides are predicted to condense in the 10 exp -6 to 10 exp -9 bar range and may be found in enstatite chondrites if they formed in this pressure range.

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

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

Prediction of distribution coefficient from structure. 1. Estimation method.

PubMed

Csizmadia, F; Tsantili-Kakoulidou, A; Panderi, I; Darvas, F

1997-07-01

A method has been developed for the estimation of the distribution coefficient (D), which considers the microspecies of a compound. D is calculated from the microscopic dissociation constants (microconstants), the partition coefficients of the microspecies, and the counterion concentration. A general equation for the calculation of D at a given pH is presented. The microconstants are calculated from the structure using Hammett and Taft equations. The partition coefficients of the ionic microspecies are predicted by empirical equations using the dissociation constants and the partition coefficient of the uncharged species, which are estimated from the structure by a Linear Free Energy Relationship method. The algorithm is implemented in a program module called PrologD.

New Parallel Algorithms for Landscape Evolution Model

NASA Astrophysics Data System (ADS)

Jin, Y.; Zhang, H.; Shi, Y.

2017-12-01

Most landscape evolution models (LEM) developed in the last two decades solve the diffusion equation to simulate the transportation of surface sediments. This numerical approach is difficult to parallelize due to the computation of drainage area for each node, which needs huge amount of communication if run in parallel. In order to overcome this difficulty, we developed two parallel algorithms for LEM with a stream net. One algorithm handles the partition of grid with traditional methods and applies an efficient global reduction algorithm to do the computation of drainage areas and transport rates for the stream net; the other algorithm is based on a new partition algorithm, which partitions the nodes in catchments between processes first, and then partitions the cells according to the partition of nodes. Both methods focus on decreasing communication between processes and take the advantage of massive computing techniques, and numerical experiments show that they are both adequate to handle large scale problems with millions of cells. We implemented the two algorithms in our program based on the widely used finite element library deal.II, so that it can be easily coupled with ASPECT.

Soft X-ray scanning transmission X-ray microscopy (STXM) of actinide particles.

PubMed

Nilsson, Hans J; Tyliszczak, Tolek; Wilson, Richard E; Werme, Lars; Shuh, David K

2005-09-01

A descriptive account is given of our most recent research on the actinide dioxides with the Advanced Light Source Molecular Environmental Science (ALS-MES) Beamline 11.0.2 soft X-ray scanning transmission X-ray microscope (STXM) at the Lawrence Berkeley National Laboratory (LBNL). The ALS-MES STXM permits near-edge X-ray absorption fine structure (NEXAFS) and imaging with 30-nm spatial resolution. The first STXM spectromicroscopy NEXAFS spectra at the actinide 4d5/2 edges of the imaged transuranic particles, NpO2 and PuO2, have been obtained. Radiation damage induced by the STXM was observed in the investigation of a mixed oxidation state particle (Np(V,VI)) and was minimized during collection of the actual spectra at the 4d5/2 edge of the Np(V,VI) solid. A plutonium elemental map was obtained from an irregular PuO2 particle with the dimensions of 650 x 650 nm. The Pu 4d5/2 NEXAFS spectra were collected at several different locations from the PuO2 particle and were identical. A representative oxygen K-edge spectrum from UO2 was collected and resembles the oxygen K-edge from the bulk material. The unique and current performance of the ALS-MES STXM at extremely low energies (ca. 100 eV) that may permit the successful measurement of the actinide 5d edge is documented. Finally, the potential of STXM as a tool for actinide investigations is briefly discussed.

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

CMPO purity tests in the TRUEX solvent using americium-241

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

Brewer, K.N.; Herbst, R.S.; Tranter, T.J.

1993-12-01

The Transuranic Extraction (TRUEX) Process was developed by E.P. Horwitz and coworkers at Argonne National Laboratory (ANL) to separate the +4, +6, and +3 actinides from acidic aqueous solutions of nuclear wastes. Octyl (phenyl)-N-N-diisobutyl-carbamoylmethylphosphine oxide (CMPO) is the active actinide complexant used in the TRUEX solvent. CMPO is combined with tributyl phosphate (TBP) in an organic diluent, typically n-dodecane, to form the TRUEX solvent. Small quantities of impurities in the CMPO resulting from: (1) synthesis, (2) acid hydrolysis, or (3) radiolysis can result in actinide stripping problems from the solvent. The impurity, octylphenylphosphinic acid (POPPA), ia a powerful extractant atmore » low acid concentrations which may be formed during CMPO synthesis. Consequently, commercial CMPO may contain sufficient quantities of POPPA to significantly impact the stripping of actinides from the TRUEX solvent. The purpose of these tests was to (1) determine if commercially available CMPO is sufficiently pure to alleviate actinide stripping problems from the TRUEX process and (2) to determine if solvent cleanup methods are sufficient to purify the commercially purchased CMPO. Extraction and solvent cleanup methodologies used by Horwitz and coworkers at ANL were used to determine CMPO purity with {sup 241}Am. The improvement of the americium distribution coefficient in dilute nitric acid resulting from further purifying this CMPO is not significant enough to warrant additional CMPO purifying steps. The commercially purchased CMPO is found to be acceptable to use, as received, in a full-scale TRUEX process.« less

Applications of time-resolved laser fluorescence spectroscopy to the environmental biogeochemistry of actinides.

PubMed

Collins, Richard N; Saito, Takumi; Aoyagi, Noboru; Payne, Timothy E; Kimura, Takaumi; Waite, T David

2011-01-01

Time-resolved laser fluorescence spectroscopy (TRLFS) is a useful means of identifying certain actinide species resulting from various biogeochemical processes. In general, TRLFS differentiates chemical species of a fluorescent metal ion through analysis of different excitation and emission spectra and decay lifetimes. Although this spectroscopic technique has largely been applied to the analysis of actinide and lanthanide ions having fluorescence decay lifetimes on the order of microseconds, such as UO , Cm, and Eu, continuing development of ultra-fast and cryogenic TRLFS systems offers the possibility to obtain speciation information on metal ions having room-temperature fluorescence decay lifetimes on the order of nanoseconds to picoseconds. The main advantage of TRLFS over other advanced spectroscopic techniques is the ability to determine in situ metal speciation at environmentally relevant micromolar to picomolar concentrations. In the context of environmental biogeochemistry, TRLFS has principally been applied to studies of (i) metal speciation in aqueous and solid phases and (ii) the coordination environment of metal ions sorbed to mineral and bacterial surfaces. In this review, the principles of TRLFS are described, and the literature reporting the application of this methodology to the speciation of actinides in systems of biogeochemical interest is assessed. Significant developments in TRLFS methodology and advanced data analysis are highlighted, and we outline how these developments have the potential to further our mechanistic understanding of actinide biogeochemistry. American Society of Agronomy, Crop Science Society of America, and Soil Science Society of America.

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.

Calculation and analysis of cross-sections for p+184W reactions up to 200 MeV

NASA Astrophysics Data System (ADS)

Sun, Jian-Ping; Zhang, Zheng-Jun; Han, Yin-Lu

2015-08-01

A set of optimal proton optical potential parameters for p+ 184W reactions are obtained at incident proton energy up to 250 MeV. Based on these parameters, the reaction cross-sections, elastic scattering angular distributions, energy spectra and double differential cross sections of proton-induced reactions on 184W are calculated and analyzed by using theoretical models which integrate the optical model, distorted Born wave approximation theory, intra-nuclear cascade model, exciton model, Hauser-Feshbach theory and evaporation model. The calculated results are compared with existing experimental data and good agreement is achieved. Supported by National Basic Research Program of China, Technology Research of Accelerator Driven Sub-critical System for Nuclear Waste Transmutation (2007CB209903) and Strategic Priority Research Program of Chinese Academy of Sciences, Thorium Molten Salt Reactor Nuclear Energy System (XDA02010100)

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.

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.

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.