Oxidation potentials, Gibbs energies, enthalpies and entropies of actinide ions in aqueous solutions

International Nuclear Information System (INIS)

1977-01-01

The values of the Gibbs energy, enthalpy, and entropy of different actinide ions, thermodynamic characteristics of the processes of hydration of these ions, and the presently known ionization potentials of actinides are given. The enthalpy and entropy components of the oxidation potentials of actinide elements are considered. The curves of the dependence of the Gibbs energy of ion formation on the atomic number of the element and the Frost diagrams are analyzed. The diagram proposed by Frost represents the graphical dependence of the Gibbs energy of hydrated ions on the degree of oxidation of the element. Using the Frost diagram it is easy to establish whether a given ion is stable to disproportioning

Limitations of actinide recycle and waste disposal consequences

International Nuclear Information System (INIS)

Baetsle, L.H.; Raedt, C. de

1994-01-01

The paper emphasizes the impact of Light Water Reactor - Mixed Oxides introduction on the subsequent actinide management and fate of reprocessed and depleted uranium. The spent fuel from LWR-MOX contains in principle 75% of the initially produced plutonium. This new source term has to be considered together with the minor actinides from the conventional reprocessing. Subsequent LWR-MOX reprocessing in the first step in a very long term Pu + minor actinides management. Recycling of Pu + minor actinides in fast reactors to significantly reduce the Pu and minor actinides inventory (e.g. a factor of 10) is a very slow process which requires the development and operation of a large park of actinide burner reactors during an extended period of time. The overall feasibility of the P and T option will greatly depend on the massive introduction during the next century of fast neutron reactors as a replacement to the present LWR generation of nuclear power plants. (authors). 11 refs., 6 tabs., 2 figs

Synthesis and characterization of brannerite wasteforms for the immobilization of mixed oxide fuel residues

Energy Technology Data Exchange (ETDEWEB)

Bailey, D.J.; Stennett, M.C.; Hyatt, N.C. [Immobilisation Science Laboratory, Department of Materials Science and Engineering, University of Sheffield, Sheffield, S1 3JD (United Kingdom)

2016-07-01

A possible method for the reduction of civil Pu stockpiles is the reuse of Pu in mixed oxide fuel (MOX). During MOX fuel production, residues unsuitable for further recycle will be produced. Due to their high actinide content MOX residues require immobilization within a robust host matrix. Although it is possible to immobilize actinides in vitreous wasteforms; ceramic phases, such as brannerite (UTi{sub 2}O{sub 6}), are attractive due to their high waste loading capacity and relative insolubility. A range of uranium brannerite, formulated Gd{sub x}U{sub 1-x}Ti{sub 2}O{sub 6}, were prepared using a mixed oxide route. Charge compensation of divalent and trivalent cations was expected to occur via the oxidation of U{sup 4+} to higher valence states (U{sup 5+} or U{sup 6+}). Gd{sup 3+} was added to act as a neutron absorber in the final Pu bearing wasteform. X-ray powder diffraction of synthesised specimens found that phase distribution was strongly affected by processing atmosphere (air or Ar). In all cases prototypical brannerite was formed accompanied by different secondary phases dependent on processing atmosphere. Microstructural analysis (SEM) of the sintered samples confirmed the results of the X-ray powder diffraction. The preliminary results presented here indicate that brannerite is a promising host matrix for mixed oxide fuel residues. (authors)

Subsurface interactions of actinide species and microorganisms : implications for the bioremediation of actinide-organic mixtures

International Nuclear Information System (INIS)

Banaszak, J.E.; Reed, D.T.; Rittmann, B.E.

1999-01-01

By reviewing how microorganisms interact with actinides in subsurface environments, we assess how bioremediation controls the fate of actinides. Actinides often are co-contaminants with strong organic chelators, chlorinated solvents, and fuel hydrocarbons. Bioremediation can immobilize the actinides, biodegrade the co-contaminants, or both. Actinides at the IV oxidation state are the least soluble, and microorganisms accelerate precipitation by altering the actinide's oxidation state or its speciation. We describe how microorganisms directly oxidize or reduce actinides and how microbiological reactions that biodegrade strong organic chelators, alter the pH, and consume or produce precipitating anions strongly affect actinide speciation and, therefore, mobility. We explain why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions. Due to the complex interactions of the microbiological and chemical phenomena, mathematical modeling is an essential tool for research on and application of bioremediation involving co-contamination with actinides. We describe the development of mathematical models that link microbiological and geochemical reactions. Throughout, we identify the key research needs

Subsurface interactions of actinide species and microorganisms : implications for the bioremediation of actinide-organic mixtures.

Energy Technology Data Exchange (ETDEWEB)

Banaszak, J.E.; Reed, D.T.; Rittmann, B.E.

1999-02-12

By reviewing how microorganisms interact with actinides in subsurface environments, we assess how bioremediation controls the fate of actinides. Actinides often are co-contaminants with strong organic chelators, chlorinated solvents, and fuel hydrocarbons. Bioremediation can immobilize the actinides, biodegrade the co-contaminants, or both. Actinides at the IV oxidation state are the least soluble, and microorganisms accelerate precipitation by altering the actinide's oxidation state or its speciation. We describe how microorganisms directly oxidize or reduce actinides and how microbiological reactions that biodegrade strong organic chelators, alter the pH, and consume or produce precipitating anions strongly affect actinide speciation and, therefore, mobility. We explain why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions. Due to the complex interactions of the microbiological and chemical phenomena, mathematical modeling is an essential tool for research on and application of bioremediation involving co-contamination with actinides. We describe the development of mathematical models that link microbiological and geochemical reactions. Throughout, we identify the key research needs.

Subsurface interactions of actinide species and microorganisms. Implications for the bioremediation of actinide-organic mixtures

International Nuclear Information System (INIS)

Banaszak, J.E.; Rittmann, B.E.; Reed, D.T.

1999-01-01

By reviewing how microorganisms interact with actinides in subsurface environments, the way how bioremediation controls the fate of actinides is assessed. Actinides often are co-contaminants with strong organic chelators, chlorinated solvents, and fuel hydrocarbons. Bioremediation can immobilize the actinides, biodegrade the co-contaminants, or both. Actinides at the IV oxidation state are the least soluble, and microorganisms accelerate precipitation by altering the actinide's oxidation state or its speciation. The way how microorganisms directly oxidize or reduce actinides and how microbiological reactions that biodegrade strong organic chelators, alter the pH, and consume or produce precipitating anions strongly affect actinide speciation and, therefore, mobility is described. Why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions is explained. Due to the complex interactions of the microbiological and chemical phenomena, mathematical modeling is an essential tool for research on and application of bioremediation involving co-contamination with actinides. Development of mathematical models that link microbiological and geochemical reactions is described. Throughout, the key research needs are identified. (author)

Incineration of actinide targets in a pressurized water reactor spin project

International Nuclear Information System (INIS)

Puill, A.; Bergeron, J.

1993-01-01

The ability of Pressurized Water Reactors (PWR) with uranium fuel to limit the inventory growth of minor actinides (237 neptunium, and americium) produced by the French nuclear powerplants is studied. Targets containing an actinide oxide mixed to an inert matrix are loaded in some reactors. After being irradiated along with the fuel, the target is specially reprocessed. The remaining actinide and the plutonium which is produced, added to fresh actinide, are recycled in new targets. The radiotoxicity balance, with and without incineration, is examined considering that only the losses coming from the target reprocessing treated as waste. A scenario arbitrarily based on 18 years of operation results in a reduction of the radiotoxicity of the waste by a factor between 10 and 20, depending on the actinide considered. 6 refs., 6 figs., 6 tabs

Review of the treatment of actinides-bearing radioactive wastes

International Nuclear Information System (INIS)

Krause, H.

1983-01-01

Actinides bearing wastes are produced above all in the course of irradiated nuclear fuel reprocessing and during fabrication of mixed oxide fuel elements. Particular attention in research and development work must be paid to this type of waste, mainly on account of its longevity. In practical application, the specific character of the actinides bearing wastes has been largely recognized. Nevertheless, definitions and methods of treatment generally accepted worldwide are still missing today. This has no bearing as yet on present day treatment of radioactive wastes. But by the time of application of the breeder technology at the latest a special treatment concept should be available which complies with the high actinide contents and short precooling periods of the wastes

Actinides

International Nuclear Information System (INIS)

Martinot, L.; Fuger, J.

1985-01-01

The oxidation behavior of the actinides is explained on the basis of their electronic structure. The actinide elements, actinium, thorium, protactinium, uranium, neptunium, plutonium, americium, curium, berkelium, californium, einsteinium, fermium, mendelevium, nobelium, and laurencium are included. For all except the last three elements, the points of discussion are oxidation states, Gibbs energies and potentials, and potential diagram for the element in acid solution; and thermodynamic properties of these same elements are tabulated. References are cited following discussion of each element with a total of 97 references being cited. 13 tables

Neutronic analysis of the PBMR-400 full core using thorium fuel mixed with plutonium or minor actinides

International Nuclear Information System (INIS)

Acır, Adem; Coşkun, Hasan

2012-01-01

Highlights: ► Neutronic calculations for PBMR 400 were conducted with the computer codes MCNP and MONTEBURNS 2.0. ► The criticality and burnup were investigated for reactor grade plutonium and minor actinides. ► We found that the use of these new fuels in PBMRs would reduce the nuclear waste repository significantly. -- Abstract: Time evolution of criticality and burnup grades of the PBMR were investigated for reactor grade plutonium and minor actinides in the spent fuel of light water reactors (LWRs) mixed with thoria. The calculations were performed by employing the computer codes MCNP and MONTEBURNS 2.0 and using the ENDF/B-V nuclear data library. Firstly, the plutonium–thorium and minor actinides–thorium ratio was determined by using the initial k eff value of the original uranium fuel design. After the selection of the plutonium/minor actinides–thorium mixture ratio, the time-dependent neutronic behavior of the reactor grade plutonium and minor actinides and original fuels in a PBMR-400 reactor was calculated by using the MCNP code. Finally, k eff , burnup and operation time values of the fuels were compared. The core effective multiplication factor (k eff ) for the original fuel which has 9.6 wt.% enriched uranium was computed as 1.2395. Corresponding to this k eff value the reactor grade plutonium/thorium and minor actinide/thorium oxide mixtures were found to be 30%/70% and 50%/50%, respectively. The core lives for the original, the reactor grade plutonium/thorium and the minor actinide/thorium fuels were calculated as ∼3.2, ∼6.5 and ∼5.5 years, whereas, the corresponding burnups came out to be 99,000, ∼190,000 and ∼166,000 MWD/T, respectively, for an end of life k eff set equal to 1.02.

Influence of microorganisms on the oxidation state distribution of multivalent actinides under anoxic conditions

International Nuclear Information System (INIS)

Reed, Donald Timothy; Borkowski, Marian; Lucchini, Jean-Francois; Ams, David; Richmann, M.K.; Khaing, H.; Swanson, J.S.

2010-01-01

The fate and potential mobility of multivalent actinides in the subsurface is receiving increased attention as the DOE looks to cleanup the many legacy nuclear waste sites and associated subsurface contamination. Plutonium, uranium and neptunium are the near-surface multivalent contaminants of concern and are also key contaminants for the deep geologic disposal of nuclear waste. Their mobility is highly dependent on their redox distribution at their contamination source as well as along their potential migration pathways. This redox distribution is often controlled, especially in the near-surface where organic/inorganic contaminants often coexist, by the direct and indirect effects of microbial activity. Under anoxic conditions, indirect and direct bioreduction mechanisms exist that promote the prevalence of lower-valent species for multivalent actinides. Oxidation-state-specific biosorption is also an important consideration for long-term migration and can influence oxidation state distribution. Results of ongoing studies to explore and establish the oxidation-state specific interactions of soil bacteria (metal reducers and sulfate reducers) as well as halo-tolerant bacteria and Archaea for uranium, neptunium and plutonium will be presented. Enzymatic reduction is a key process in the bioreduction of plutonium and uranium, but co-enzymatic processes predominate in neptunium systems. Strong sorptive interactions can occur for most actinide oxidation states but are likely a factor in the stabilization of lower-valent species when more than one oxidation state can persist under anaerobic microbiologically-active conditions. These results for microbiologically active systems are interpreted in the context of their overall importance in defining the potential migration of multivalent actinides in the subsurface.

Phase Behavior and Equations of State of the Actinide Oxides

Science.gov (United States)

Chidester, B.; Pardo, O. S.; Panero, W. R.; Fischer, R. A.; Thompson, E. C.; Heinz, D. L.; Prescher, C.; Prakapenka, V. B.; Campbell, A.

2017-12-01

The distribution of the long-lived heat-producing actinide elements U and Th in the deep Earth has important implications for the dynamics of the mantle and possibly the energy budget of Earth's core. The low shear velocities of the Large Low-Shear Velocity Provinces (LLSVPs) on the core-mantle boundary suggests that these regions are at least partially molten and may contain concentrated amounts of the radioactive elements, as well as other large cations such as the rare Earth elements. As such, by exploring the phase behavior of actinide-bearing minerals at extreme conditions, some insight into the mineralogy, formation, and geochemical and geodynamical effects of these regions can be gained. We have performed in situ high-pressure, high-temperature synchrotron X-ray diffraction experiments and calculations on two actinide oxide materials, UO2 and ThO2, to determine their phase behavior at the extreme conditions of the lower mantle. Experiments on ThO2 reached 60 GPa and 2500 K, and experiments on UO2 reached 95 GPa and 2500 K. We find that ThO2 exists in the fluorite-type structure to 20 GPa at high temperatures, at which point it transforms to the high-pressure cotunnite-type structure and remains thus up to 60 GPa. At room temperature, an anomalous expansion of the fluorite structure is observed prior to the transition, and may signal anion sub-lattice disorder. Similarly, UO2 exists in the fluorite-type structure at ambient conditions and up to 28 GPa at high temperatures. Above these pressures, we have observed a previously unidentified phase of UO2 with a tetragonal structure as the lower-temperature phase and the cotunnite-type phase at higher temperatures. Above 78 GPa, UO2 undergoes another transition or possible dissociation into two separate oxide phases. These phase diagrams suggest that the actinides could exist as oxides in solid solution with other analogous phases (e.g. ZrO2) in the cotunnite-type structure throughout much of Earth's lower mantle.

General regularity of the oxidation potential variations and high oxidation states in the second half of the actinide series

International Nuclear Information System (INIS)

Spitsyn, V.I.; Vokhmin, V.G.; Ionova, G.V.; Pershina, V.G.

1984-01-01

Oxidation potentials (OP) PHI(4/3), PHI(5/3), PHI(6/3), PHI(5/4) and PHI(6/5) are calculated for the members of the actinide series. A semiemperic relation combining OP with explicit terms for ground level energies of actinide ions in Russell-Saunders approximation as well as known values of formal OP relative to the normal hydrogen electrode potential are used as an extrapolation function. It is shown that an increase of PHI(4/3) OP which occurs after Bsub(k) explains a low stability of the oxidation state 4 in solutions for actinides of the second half of the series. PHI(5/3) and PHI(5/4) OP in the section starting with Cm have the minimum at Cf. PHI(6/3) OP for Cm, Bk, Cf and Es are practically the same but for Cm, Bk and Es they are smaller than PHI(5/3) OP. A principle possibility of Bk(6), Cf(6) and Es(6) preparation is shown

Electronic structure and ionicity of actinide oxides from first principles

DEFF Research Database (Denmark)

Petit, Leon; Svane, Axel; Szotek, Z.

2010-01-01

The ground-state electronic structures of the actinide oxides AO, A2O3, and AO2 (A=U, Np, Pu, Am, Cm, Bk, and Cf) are determined from first-principles calculations, using the self-interaction corrected local spin-density approximation. Emphasis is put on the degree of f-electron localization, whi...

Process for obtaining sintered conglomerates with a high density of rare earth oxides and actinides

International Nuclear Information System (INIS)

Pasto, A.E.

1974-01-01

The invention concerns a method to produce agglomerates of actinide and rare earth oxides possessing a cubic-monoclinic transformation in order to obtain high densities close to the theoretical density, and the articles produced by the method. The process is based on the use of a rare earth or actinide oxide, in particular Eu 2 O 3 , with a cubic-monoclinic phase transformation, the oxide being sintered by hot compression at a temperature 50 deg C to 100 deg C above the transformation temperature. The sintered agglomerates obtained can have a purity of at least 99.9% and a density of practically 100%. These agglomerates are suitable in particular for the formation of nuclear reactor control rods [fr

Actinide partitioning and transmutation program progress report, October 1, 1976--March 31, 1977

International Nuclear Information System (INIS)

Blomeke, J.O.; Tedder, D.W.

1977-01-01

Experimental work on the 16 tasks comprising the Actinide Partitioning and Transmutation Program was initiated at the various sites. This work included the development of conceptual material balance flowsheets which define integrated waste systems supporting an LWR fuel reprocessing plant and a mixed (U-Pu) oxide fuel refabrication plant. In addition, waste subsystems were defined for experimental evaluation. Computer analysis of partitioning-transmutation, utilizing an LMFBR for transmutation, was completed for both constant and variable waste actinide generation rates

Separation and recovery of Cm from Cm-Pu mixed oxide samples containing Am impurity

International Nuclear Information System (INIS)

Hirokazu Hayashi; Hiromichi Hagiya; Mitsuo Akabori; Yasuji Morita; Kazuo Minato

2013-01-01

Curium was separated and recovered as an oxalate from a Cm-Pu mixed oxide which had been a 244 Cm oxide sample prepared more than 40 years ago and the ratio of 244 Cm to 240 Pu was estimated to 0.2:0.8. Radiochemical analyses of the solution prepared by dissolving the Cm-Pu mixed oxide in nitric acid revealed that the oxide contained about 1 at% of 243 Am impurity. To obtain high purity curium solution, plutonium and americium were removed from the solution by an anion exchange method and by chromatographic separation using tertiary pyridine resin embedded in silica beads with nitric acid/methanol mixed solution, respectively. Curium oxalate, a precursor compound of curium oxide, was prepared from the purified curium solution. 11.9 mg of Cm oxalate having some amounts of impurities, which are 243 Am (5.4 at%) and 240 Pu (0.3 at%) was obtained without Am removal procedure. Meanwhile, 12.0 mg of Cm oxalate (99.8 at% over actinides) was obtained with the procedure including Am removals. Both of the obtained Cm oxalate sample were supplied for the syntheses and measurements of the thermochemical properties of curium compounds. (author)

Relationships among oxidation-reduction and acid-base properties of the actinides in high oxidation states

International Nuclear Information System (INIS)

Morss, L.R.

1992-01-01

The first chemical identification of plutonium, its subsequent isolation on the macroscopic scale, and more recent chemical separation schemes were achieved by taking advantage of the differences among the oxidation states of uranium, neptunium, and plutonium. Many acid-base properties modify the relative stabilities of oxidation states of the actinides. In the solid state, strongly basic compounds such as Cs 2 O yield complex oxides with oxidation states of Np(VII), Pu(VI), and Am(VI) whereas more acidic compounds such as CsF yield complex fluorides with lower oxidation states. In aqueous solution, high basicity and strongly covalent complexes favor high oxidation states. In nonaqueous solvent systems, high acidity generally favors low oxidation states. This paper elucidates and attempts to interpret the effects of these acid-base properties in a systematic fashion

Molecular cluster theory of chemical bonding in actinide oxide

International Nuclear Information System (INIS)

Ellis, D.E.; Gubanov, V.A.; Rosen, A.

1978-01-01

The electronic structure of actinide monoxides AcO and dioxides AcO 2 , where Ac = Th, U, Np, Pu, Am, Cm and Bk has been studied by molecular cluster methods based on the first-principles one-electron local density theory. Molecular orbitals for nearest neighbor clusters AcO 10- 6 and AcO 12- 8 representative of monoxide and dioxide lattices were obtained using non-relativistic spin-restricted and spin-polarized Hartree-Fock-Slater models for the entire series. Fully relativistic Dirac-Slater calculations were performed for ThO, UO and NpO in order to explore magnitude of spin-orbit splittings and level shifts in valence structure. Self-consistent iterations were carried out for NpO, in which the NpO 6 cluster was embedded in the molecular field of the solid. Finally, a ''moment polarized'' model which combines both spin-polarization and relativistic effects in a consistent fashion was applied to the NpO system. Covalent mixing of oxygen 2p and Ac 5f orbitals was found to increase rapidly across the actinide series; metal s,p,d covalency was found to be nearly constant. Mulliken atomic population analysis of cluster eigenvectors shows that free-ion crystal field models are unreliable, except for the light actinides. X-ray photoelectron line shapes have been calculated and are found to compare rather well with experimental data on the dioxides

PRODUCTION OF ACTINIDE METAL

Science.gov (United States)

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)

The clearance of Pu and Am from the respiratory system of rodents after the inhalation of oxide aerosols of these actinides either alone or in combination with other metals

International Nuclear Information System (INIS)

Stather, J.W.; James, A.C.; Brightwell, J.; Rodwell, P.

1979-01-01

In this series of studies in rodents the lung clearance and tissue distribution of both plutonium and americium have been measured following their inhalation as mixed actinide oxides either alone or in combination with other metals. The aerosols used were materials to which workers in the nuclear industry may be occupationally exposed or which could be generated in the event of an accident in a reactor core or fuel fabrication plant. The studies showed that, at least for some PuO 2 aerosols, the lung model currently being used by ICRP for estimating tissue doses from inhaled actinides may overestimate, by about a factor of ten, the amount of plutonium translocated to the blood. The presence of oxides of other metals can, however, appreciably influence the clearance of plutonium from the lung. While in some mixtures plutonium dioxide behaves as an insoluble (Class Y) compound and in others as a soluble (Class W) compound, it may also have transportability characteristics between these two extremes. Americium-241 behaves as a soluble (Class W) compound when inhaled as the oxide. However, if it is present in trace quantities in mixed-oxide aerosols its behaviour depends upon that of the materials present in greatest mass. (author)

Sigma Team for Advanced Actinide Recycle FY2015 Accomplishments and Directions

Energy Technology Data Exchange (ETDEWEB)

Moyer, Bruce A. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

2015-09-30

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 research 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

Extraction chromatogrpahy of actinides, ch. 7

International Nuclear Information System (INIS)

Mueller, W.

1975-01-01

This review on extraction chromatography of actinides emphasizes the important usage of neutral (Tributylphosphate), basic (substituted ammonium salts), and acidic (HDEHP) extractants, and their application to separations of actinides in the di-to hexavalent oxidation state. Furthermore, the actinide extraction by ketones, ethers, alcohols and β-diketones is discussed

A study on the feasibility of minor actinides in BWR

International Nuclear Information System (INIS)

Abdul Waris; Budiono

2008-01-01

Preliminary study on the feasibility of actinides minor (MA) recycling without mixing them with plutonium in boiling water reactor (BWR) has been carried out. The results show that increasing of fissile MA content in mixed oxide fuel (MOX) and/or reducing void fraction can enlarge the effective multiplication factor at the beginning of cycle, but the reactor still can not obtain its criticality condition. Furthermore, dropping the void fraction results in higher reactivity swing and therefore plummeting the safety factor of the reactor. (author)

Application of plasma shield technology to the reduction, treatment, and disposal of hazardous organic and/or mixed wastes with actinide recovery

International Nuclear Information System (INIS)

Adams, B.T.; Vaughan, L.L.; Joyce, E.L. Jr.; Bieniewski, T.M.

1990-01-01

Los Alamos research activities are currently directed at the application of the shielded hydrogen plasma torch to the direct production of actinide metals from a UF 6 feedstock. Two broad classes of thermal plasma reactors are currently in widespread use: the direct current (dc) arc jet system and the radio frequency (rf) inductively coupled system. Los Alamos has improved upon the basic rf plasma tube design using the concept of a transformer. The unique feature of the Los Alamos tube is a segmented, cooled, internal radiation shield. The Los Alamos shielded plasma torch routinely achieves temperatures exceeding 10,000 K and electron densities of 10 16 /cm 3 when operated continuously at one atmosphere of argon. These highly energetic conditions are sufficient to dissociate most chemical compounds into their constituent atoms. Based upon these characteristics, Los Alamos is currently investigating the application of the shielded plasma torch technology to the destruction of organic and mixed hazardous wastes, as well as the direct production of actinide metals from the halides and oxides, without the cogeneration of contaminated wastes. 5 refs., 4 figs

Preparation of minor actinides targets or blankets by the means of Ionic Exchange Resin

Energy Technology Data Exchange (ETDEWEB)

Picart, S.; Mokhtari, H.; Ramiere, I.; Jobelin, I. [CEA, Nuclear Energy Division, RadioChemistry and Process Department, Actinides Chemistry Laboratory, BP17171, Bagnols-sur-Ceze, 30207 (France)

2009-06-15

The objective of our R and D work is the elaboration by the use of ionic exchange resin of minor actinide precursors for target or blanket dedicated to their transmutation in sodium fast reactor. From the beginning, the resin process called WAR (acronym of Weak Acid Resin) was developed in the 70's at the ORNL for the making of uranium carbide kernels for the high temperature gas reactor [1] [2]. By now, our aim is to extend this concept to the manufacturing of minor actinides oxide mixed with uranium oxides [3]. More precisely, this process can be divided in two major steps: the loading of the resin and the thermal treatment of the fully loaded resin driving either to oxide or carbide phases depending on the gas atmosphere. The difficulty stems from the preparation of the loading solutions which must fulfill precise conditions of pH in presence of actinides cations prone to hydrolysis. Furthermore, the proportions of uranium and minor actinides in solutions must be adjusted to fit the right ratio in the solid. The study presented here will then focus on the experiments and tests which enable us to optimize the fixing of minor actinides on ionic exchange resin and their carbonization in oxide. [1] G. W. Weber, R. L. Beatty et V. J. Tennery, Nuclear Technology, 35, 217-226, (1977), 'Processing and composition control of weak-acid-resin derived fuel microspheres'. [2] K. J. Notz, P. A. Haas, J. H. Shaffer, Radiochimica Acta, 25, 153-160, (1978). 'The preparation of HTGR Fissile Fuel Kernels by Uranium Loading of Ion Exchange Resin'. [3] S. Picart, H. Mokhtari, I. Ramiere, 'Plutonium Futures, The Science 2008', 7-11 july 2008, Dijon, France. 'Modelling of the ionic Exchange between a weak acid resin in its ammonium form and a minor actinide'. (authors)

Research in actinide chemistry

International Nuclear Information System (INIS)

Choppin, G.R.

1993-01-01

This research studies the behavior of the actinide elements in aqueous solution. The high radioactivity of the transuranium actinides limits the concentrations which can be studied and, consequently, limits the experimental techniques. However, oxidation state analogs (trivalent lanthanides, tetravalent thorium, and hexavalent uranium) do not suffer from these limitations. Behavior of actinides in the environment are a major USDOE concern, whether in connection with long-term releases from a repository, releases from stored defense wastes or accidental releases in reprocessing, etc. Principal goal of our research was expand the thermodynamic data base on complexation of actinides by natural ligands (e.g., OH - , CO 3 2- , PO 4 3- , humates). The research undertakes fundamental studies of actinide complexes which can increase understanding of the environmental behavior of these elements

Selective extraction of actinides from high level liquid wastes. Study of the possibilities offered by the Redox properties of actinides

International Nuclear Information System (INIS)

Adnet, J.M.

1991-07-01

Partitioning of high level liquid wastes coming from nuclear fuel reprocessing by the PUREX process, consists in the elimination of minor actinides (Np, Am, and traces of Pu and U). Among the possible processes, the selective extraction of actinides with oxidation states higher than three is studied. First part of this work deals with a preliminary step; the elimination of the ruthenium from fission products solutions using the electrovolatilization of the RuO4 compound. The second part of this work concerns the complexation and oxidation reactions of the elements U, Np, Pu and Am in presence of a compound belonging to the insaturated polyanions family: the potassium phosphotungstate. For actinide ions with oxidation state (IV) complexed with phosphotungstate anion the extraction mechanism by dioctylamine was studied and the use of a chromatographic extraction technic permitted successful separations between tetravalents actinides and trivalents actinides. Finally, in accordance with the obtained results, the basis of a separation scheme for the management of fission products solutions is proposed

Actinide speciation in the environment

International Nuclear Information System (INIS)

Choppin, G.R.

2007-01-01

Nuclear test explosions and nuclear reactor wastes and accidents have released large amounts of radioactivity into the environment. Actinide ions in waters often are not in a state of thermodynamic equilibrium and their solubility and migration behavior is related to the form in which the nuclides are introduced into the aquatic system. Chemical speciation, oxidation state, redox reactions, and sorption characteristics are necessary in predicting solubility of the different actinides, their migration behaviors and their potential effects on marine biota. The most significant of these variables is the oxidation state of the metal ion as the simultaneous presence of more than one oxidation state for some actinides in a solution complicates actinide environmental behavior. Both Np(V)O 2 + and Pu(V)O 2 + , the most significant soluble states in natural oxic waters, are relatively noncomplexing and resistant to hydrolysis and subsequent precipitation. The solubility of NpO 2 + can be as high as 10 -4 M while that of PuO 2 + is much more limited by reduction to the insoluble tetravalent species, Pu(OH) 4 , (pK sp ≥56) but which can be present in the pentavalent form in aqautic phases as colloidal material. The solubility of hexavalent UO 2 2+ in sea water is relatively high due to formation of carbonate complexes. The insoluble trivalent americium hydroxocarbonate, Am(OH)(CO 3 ) is the limiting species for the solubility of Am(III) in sea water. Thorium(IV) is present as Th(OH) 4 , in colloidal form. The chemistry of actinide ions in the environment is reviewed to show the spectrum of reactions that can occur in natural waters which must be considered in assessing the environmental behavior of actinides. Much is understood about sorption of actinides on surfaces, the mode of migration of actinides in such waters and the potential effects of these radioactive species on marine biota, but much more understanding of the behavior of the actinides in the environment is

Review of Integral Experiments for Minor Actinide Management

International Nuclear Information System (INIS)

Gil, C.S.; Glinatsis, G.; Hesketh, K.; Iwamoto, O.; Okajima, S.; Tsujimoto, K.; Jacqmin, R.; Khomyakov, Y.; Kochetkov, A.; Kormilitsyn, M.; Palmiotti, G.; Salvatores, M.; Perret, G.; Rineiski, A.; Romanello, V.; Sweet, D.

2015-01-01

Spent nuclear fuel contains minor actinides (MAs) such as neptunium, americium and curium, which require careful management. This becomes even more important when mixed oxide (MOX) fuel is being used on a large scale since more MAs will accumulate in the spent fuel. One way to manage these MAs is to transmute them in nuclear reactors, including in light water reactors, fast reactors or accelerator-driven subcritical systems. The transmutation of MAs, however, is not straightforward, as the loading of MAs generally affects physics parameters, such as coolant void, Doppler and burn-up reactivity. This report focuses on nuclear data requirements for minor actinide management, the review of existing integral data and the determination of required experimental work, the identification of bottlenecks and possible solutions, and the recommendation of an action programme for international co-operation. (authors)

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

Energy Technology Data Exchange (ETDEWEB)

Hobbs, D. T. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Shehee, T. C. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

2015-08-31

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

Fundamental aspects of actinide-zirconium pyrochlore oxides: Systematic comparison of the Pu, Am, Cm, Bk and Cf systems

International Nuclear Information System (INIS)

Haire, R.G.; Raison, P.E.

2000-01-01

Zirconium- and hafnium-based oxide materials have gained attraction for various nuclear applications. These materials have features in common with one of the early, well-publicized inorganic ceramics for immobilizing nuclear waste. Our interests have addressed the fundamental structural and chemical properties of these oxide systems. We pursued both the crystal chemical constraints of the oxide matrices, as well as the importance of the chemistry of the f-elements. By incorporating five actinide elements in our studies, we were able to compare systematically the materials science of these materials with the fundamental chemistry and electronic configurations of these actinides employed. It is expected that this basic information will be useful technologically in the realm of tailor-made materials for different applications

Actinide cation-cation complexes

International Nuclear Information System (INIS)

Stoyer, N.J.; Seaborg, G.T.

1994-12-01

The +5 oxidation state of U, Np, Pu, and Am is a linear dioxo cation (AnO 2 + ) with a formal charge of +1. These cations form complexes with a variety of other cations, including actinide cations. Other oxidation states of actinides do not form these cation-cation complexes with any cation other than AnO 2 + ; therefore, cation-cation complexes indicate something unique about AnO 2 + cations compared to actinide cations in general. The first cation-cation complex, NpO 2 + ·UO 2 2+ , was reported by Sullivan, Hindman, and Zielen in 1961. Of the four actinides that form AnO 2 + species, the cation-cation complexes of NpO 2 + have been studied most extensively while the other actinides have not. The only PuO 2 + cation-cation complexes that have been studied are with Fe 3+ and Cr 3+ and neither one has had its equilibrium constant measured. Actinides have small molar absorptivities and cation-cation complexes have small equilibrium constants; therefore, to overcome these obstacles a sensitive technique is required. Spectroscopic techniques are used most often to study cation-cation complexes. Laser-Induced Photacoustic Spectroscopy equilibrium constants for the complexes NpO 2 + ·UO 2 2+ , NpO 2 + ·Th 4+ , PuO 2 + ·UO 2 2+ , and PuO 2 + ·Th 4+ at an ionic strength of 6 M using LIPAS are 2.4 ± 0.2, 1.8 ± 0.9, 2.2 ± 1.5, and ∼0.8 M -1

Actinides, the narrowwest bands

International Nuclear Information System (INIS)

Smith, J.L.; Riseborough, P.S.

1984-01-01

A table of elements is shown that demonstrates the crossover from superconductivity to magnetism as well as regions of mixed valence. In particular, the actinides must eventually show 4f-electron like mixed valence, after the 5f-electrons become localized. There also seems to be an adiabatic continuation between heavy fermion and mixed valence behavior

Actinide science. Fundamental and environmental aspects

International Nuclear Information System (INIS)

Choppin, Gregory R.

2005-01-01

Nuclear test explosions and reactor wastes have deposited an estimated 16x10 15 Bq of plutonium into the world's aquatic systems. However, plutonium concentration in open ocean waters is orders of magnitude less, indicating that most of the plutonium is quite insolvable in marine waters and has been incorporated into sediments. Actinide ions in waters often are not in a state of thermodynamic equilibrium and their solubility and migration behavior is related to the form in which the nuclides were introduced into the aquatic system. Actinide solubility depends on such factors as pH(hydrolysis), E H (oxidation state), reaction with complexants (e.g. carbonate, phosphate, humic acid, etc.) sorption to surfaces of minerals and/or colloids, etc., in the water. The most significant of these variables is the oxidation sate of the metal ion. The simultaneous presence of more than one oxidation state for some actinides (e.g. plutonium) in a solution complicates actinide environmental behavior. Both Np(V)O 2 + and Pu(V)O 2 + , the most significant soluble states in natural oxic waters are relatively noncomplexing and resistant to hydrolysis and subsequent precipitation but can undergo reduction to the Pu(IV) oxidation state with its different elemental behavior. The solubility of NpO 2 + can be as high as 10 -4 M while that of PuO 2 + is more limited by reduction to the insoluble tetravalent species, Pu(OH) 4 , (pK SP - 56). The net solubility of hexavalent UO 2 2+ in sea water is also limited by hydrolysis; however, it has a relatively high concentration due to formation of carbonate complexes. The insoluble trivalent americium hydroxocarbonate, Am(CO) 3 (OH), is the limiting species for the solubility of Am(III) in sea water. Thorium is found exclusively as the tetravalent species and its solubility is limited by the formation of quite insoluble Th(OH) 4 . The chemistry of actinide ions in the environment is reviewed to show the spectrum of reactions that can occur in

Build-up and decay of fuel actinides in the fuel cycle of nuclear reactors

International Nuclear Information System (INIS)

Tasaka, Kanji; Kikuchi, Yasuyuki; Shindo, Ryuichi; Yoshida, Hiroyuki; Yasukawa, Shigeru

1976-05-01

For boiling water reactors, pressurized light-water reactors, pressure-tube-type heavy water reactors, high-temperature gas-cooled reactors, and sodium-cooled fast breeder reactors, uranium fueled and mixed-oxide fueled, each of 1000 MWe, the following have been studied: (1) quantities of plutonium and other fuel actinides built up in the reactor, (2) cooling behaviors of activities of plutonium and other fuel actinides in the spent fuels, and (3) activities of plutonium and other fuel actinides in the high-level reprocessing wastes as a function of storage time. The neutron cross section and decay data of respective actinide nuclides are presented, with their evaluations. For effective utilization of the uranium resources and easy reprocessing and high-level waste management, a thermal reactor must be fueled with uranium; the plutonium produced in a thermal reactor should be used in a fast reactor; and the plutonium produced in the blanket of a fast reactor is more appropriate for a fast reactor than that from a thermal reactor. (auth.)

Comparison of the thermodynamic properties and high temperature chemical behavior of lanthanide and actinide oxides

International Nuclear Information System (INIS)

Ackermann, R.J.; Rauh, E.G.

1977-01-01

The thermodynamic properties of the lanthanide and actinide oxides are examined, compared, and associated with a variety of high temperature chemical behavior. Trends are cited resulting from a number of thermodynamic and spectroscopic correlations involving solid phases, species in aqueous solution, and molecules and ions in the vapor phase. Inadequacies in the data and alternative approaches are discussed. The characterization of nonstoichiometric phases stable only at high temperatures is related to a network of heterogeneous and homogeneous equilibria. A broad perspective of similarity and dissimilarity between the lanthanides and actinides emerges and forms the basis of the projected needs for further study

Advances in computational actinide chemistry in China

Energy Technology Data Exchange (ETDEWEB)

Wang, Dongqi; Wu, Jingyi; Chai, Zhifang [Chinese Academy of Sciences, Beijing (China). Multidisciplinary Initiative Center; Su, Jing [Chinese Academy of Sciences, Shanghai (China). Div. of Nuclear Materials Science and Engineering; Li, Jun [Tsinghua Univ., Beijing (China). Dept. of Chemistry and Laboratory of Organic Optoelectronics and Molecular Engineering

2014-04-01

The advances in computational actinide chemistry made in China are reviewed. Several areas relevant to chemistry of actinides in gas, liquid, and solid phases have been explored. However, we limit the scope to selected contributions in the chemistry of molecular actinide systems in gas and liquid phases. These studies may be classified into two categories: treatment of relativistic effects, which cover the development of two- and four-component Hamiltonians and the optimization of relativistic pseudopotentials, and the applications of theoretical methods in actinide chemistry. The applications include (1) the electronic structures of actinocene, noble gas complexes, An-C multiple bonding compounds, uranyl and its isoelectronic species, fluorides and oxides, molecular systems with metal-metal bonding in their isolated forms (U{sub 2}, Pu{sub 2}) and in fullerene (U{sub 2} rate at C{sub 60}), and the excited states of actinide complexes; (2) chemical reactions, including oxidation, hydrolysis of UF{sub 6}, ligand exchange, reactivities of thorium oxo and sulfido metallocenes, CO{sub 2}/CS{sub 2} functionalization promoted by trivalent uranium complex; and (3) migration of actinides in the environment. A future outlook is discussed. (orig.)

Stabilization of actinides and lanthanides in unusually high oxidation states

International Nuclear Information System (INIS)

Eller, P.G.; Penneman, R.A.

1986-01-01

Chemical environments can be chosen which stabilize actinides and lanthanides in unusually high or low oxidation states and in unusual coordination. In many cases, one can rationalize the observed species as resulting from strong charge/size influences provided by specific sites in host lattices (e.g., Tb(IV) in BaTbO 3 or Am(IV) in polytungstate anions). In other cases, the unusual species can be considered from an acid-base viewpoint (e.g., U(III) in AsF 5 /HF solution or Pu(VII) in Li 5 PuO 6 ). In still other cases, an interplay of steric and redox effects can lead to interesting comparisons (e.g., instability of double fluoride salts of Pu(V) and Pu(VI) relative to U, Np, and Am analogues). Generalized ways to rationalize compounds containing actinides and lanthanides in unusual valences (particularly high valences), including the above and numerous other examples, will form the focus of this paper. Recently developed methods for synthesizing high valent f-element fluorides using superoxidizers and superacids at low temperatures will also be described. 65 refs., 8 figs., 9 tabs

Research on Actinides in Nuclear Fuel Cycles

International Nuclear Information System (INIS)

Song, Kyu Seok; Park, Yong Joon; Cho, Young Hwan

2010-04-01

The electrochemical/spectroscopic integrated measurement system was designed and set up for spectro-electrochemical measurements of lanthanide and actinide ions in high temperature molten salt media. A compact electrochemical cell and electrode system was also developed for the minimization of reactants, and consequently minimization of radioactive waste generation. By applying these equipment, oxidation and reduction behavior of lanthanide and actinide ions in molten salt media have been made. Also, thermodynamic parameter values are determined by interpreting the results obtained from electrochemical measurements. Several lanthanide ions exhibited fluorescence properties in molten salt. Also, UV-VIS measurement provided the detailed information regarding the oxidation states of lanthanide and actinide ions in high temperature molten salt media

Research on Actinides in Nuclear Fuel Cycles

Energy Technology Data Exchange (ETDEWEB)

Song, Kyu Seok; Park, Yong Joon; Cho, Young Hwan

2010-04-15

The electrochemical/spectroscopic integrated measurement system was designed and set up for spectro-electrochemical measurements of lanthanide and actinide ions in high temperature molten salt media. A compact electrochemical cell and electrode system was also developed for the minimization of reactants, and consequently minimization of radioactive waste generation. By applying these equipment, oxidation and reduction behavior of lanthanide and actinide ions in molten salt media have been made. Also, thermodynamic parameter values are determined by interpreting the results obtained from electrochemical measurements. Several lanthanide ions exhibited fluorescence properties in molten salt. Also, UV-VIS measurement provided the detailed information regarding the oxidation states of lanthanide and actinide ions in high temperature molten salt media

The actinides

International Nuclear Information System (INIS)

Bagnall, K.W.

1987-01-01

This chapter of coordination compound chemistry is devoted to the actinides and starts with a general survey. Most of the chapter relates to thorium and uranium but protactinium, neptunium and plutonium are included. There are sections on nitrogen, phosphorus, sulfur, selenium, tellurium and halogen ligands of the metals in their +3, +4, +5 and +6 oxidation states and of the transplutonium elements in their +2, +3, +4, and +5 oxidation states. (UK)

PREPARATION OF ACTINIDE-ALUMINUM ALLOYS

Science.gov (United States)

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)

Crystallo-chemistry of actinide nitrides (U1-yPuy)N and effect of impurities

International Nuclear Information System (INIS)

Beauvy, M.; Coulon-Picard, E.; Pelletier, M.

2004-01-01

Investigations on actinide nitrides has been done in our Laboratories for Fast Breeder Reactors since the seventies and some properties are reported to show the interest for these fuels. Today, the actinide nitrides are reconsidered as possible fuels for the future fission reactors (GFR and LMFR selected by the international forum Generation IV). The results of new investigations on crystal structure of mixed mono-nitrides (U,Pu)N, and the effects of oxygen and carbon contaminations on this structure are presented. The cubic 'NaCl-fcc' type structure of actinide nitrides AnN with space group O5/h-Fm3m does not respect the 'Vegard law' model for the mixed nitrides (U 1-y Pu y )N. These nitrides are usually considered with strong metallic character associated with partial ionic bonding, but the ionic contribution in the An-N bonding determined in this work is very important and near 41.6% for UN and PuN. From results published on resistivity of mixed nitrides, the data on bonding must be also modified for partial covalence. This is in good agreement with the experimental lattice parameters which are not compatible with dominant metallic bonding. The numbers of bonding electrons in the nitrides (U 1-y Pu y )N are reevaluated and the low values proposed comparatively with those previously published confirm the strong ionic character with high concentration of An 3+ ions. The solubility of oxygen and carbon in actinide nitrides (U 1-y Pu y )N are discussed from measurements on volume concentration of actinide oxide phase, total oxygen and carbon contents, and lattice parameter of nitrides. The oxygen solubility limit in UN is near 1000 ppm, with a lightly higher value of 1200 ppm for the mixed nitride (U 0.8 Pu 0.2 )N. The effects of oxygen or carbon atoms in the lattice of (U 1-y Pu y )N are analysed

1981 Annual Status Report. Plutonium fuels and actinide programme

International Nuclear Information System (INIS)

1981-01-01

In this 1981 report the work carried out by the European Institute for Transuranium elements is reviewed. Main topics are: operation limits of plutonium fuels: swelling of advanced fuels, oxide fuel transients, equation of state of nuclear materials; actinide cycle safety: formation of actinides (FACT), safe handling of plutonium fuel (SHAPE), aspects of the head-end processing of carbide fuel (RECARB); actinide research: crystal chemistry, solid state studies, applied actinide research

Investigations on synthesis, coordination behaviour and actinide recovery of unexplored phosphine oxides

International Nuclear Information System (INIS)

Veerashekhar Goud, E.; Pavankumar, B.B.; Das, Dhrubajyothi

2016-01-01

The search for the development of an optimum extractant for effective separation of a particular metal from a mixture is an active field of research in both chemistry and chemical engineering. These extractants find extensive application in extractive metallurgy and in nuclear fuel cycle (for the separation of actinides from other fission products). In the case of the latter, solvent extraction and ion exchange are two widely employed separation techniques. In this connection, the present paper reports synthesis and structural characterization of various new phosphine oxide derivatives. The coordination behavior of these ligands is studied with some selected lanthanides and actinides shows the proposed structures of La(III) and Th(IV) metal complexes. The purity and structural characterization of the ligands and their corresponding metal complexes are analyzed by various analytical and spectroscopic techniques. Additionally, we have applied Density functional theory (DFT) calculations to understand the electronic structure of some metal complexes formed during the extraction process. (author)

Actinide partitioning from high level liquid waste using the Diamex process

International Nuclear Information System (INIS)

Madic, C.; Blanc, P.; Condamines, N.; Baron, P.; Berthon, L.; Nicol, C.; Pozo, C.; Lecomte, M.; Philippe, M.; Masson, M.; Hequet, C.

1994-01-01

The removal of long-lived radionuclides, which belong to the so-called minor actinides elements, neptunium, americium and curium, from the high level nuclear wastes separated during the reprocessing of the irradiated nuclear fuels in order to transmute them into short-lived nuclides, can substantially decrease the potential hazards associated with the management of these nuclear wastes. In order to separate minor actinides from high-level liquid wastes (HLLW), a liquid-liquid extraction process was considered, based on the use of diamide molecules, which display the property of being totally burnable, thus they do not generate secondary solid wastes. The main extracting properties of dimethyldibutyltetradecylmalonamide (DMDBTDMA), the diamide selected for the development of the DIAMEX process, are briefly described in this paper. Hot tests of the DIAMEX process (using DMDBTDMA) related to the treatment of an mixed oxide fuels (MOX) type HLLW, were successfully performed. The minor actinide decontamination factors of the HLLW obtained were encouraging. The main results of these tests are presented and discussed in this paper. (authors). 9 refs., 2 figs., 7 tabs

Extraction chromatography of actinides

International Nuclear Information System (INIS)

Muller, W.

1978-01-01

Extraction chromatography of actinides in the oxidation state from 2 to 6 is reviewed. Data on using neutral (tbp), basic (substituted ammonium salts) and acidic [di-(2-ethylhexyl)-phosphoric acid (D2EHPA)] extracting agents ketones, esters, alcohols and β-diketones in this method are given. Using the example of actinide separation using D2EHPA, discussed are factors influencing the efficiency of their chromatography separation (nature and particle size of the carrier materials, extracting agents amount on the carrier, temperature and elution rate)

Effect of pressure on f-electron delocalization and oxidation in actinide dioxides

Energy Technology Data Exchange (ETDEWEB)

Petit, L., E-mail: leon.petit@stfc.ac.uk [Daresbury Laboratory, Daresbury, Warrington WA4 4AD (United Kingdom); Szotek, Z.; Temmerman, W.M. [Daresbury Laboratory, Daresbury, Warrington WA4 4AD (United Kingdom); Stocks, G.M. [Materials Science and Technology Division and Center for Defect Physics, Oak Ridge National Laboratory, Oak Ridge, TN 37831 (United States); Svane, A. [Department of Physics and Astronomy, University of Aarhus, DK-8000 Aarhus C (Denmark)

2014-08-01

Using first principles calculations, we have investigated f-electron delocalization and oxidation in the actinide dioxides under pressure. Whilst UO{sub 2} is found on the verge of an insulator to metal transition at the equilibrium volume, increasingly larger pressures are required to delocalize f-electrons in NpO{sub 2}, PuO{sub 2}, and AmO{sub 2}, respectively 49, 112, and 191 GPa. Compared to this broad range of pressures, the experimentally observed structural transitions, in all four dioxides, occur between 30 and 40 GPa, which leads us to conclude that the associated volume collapse is not due to f-electron delocalization. In contrast, oxidation of the dioxides is found to be linked to the degree of f-electron localization, but it emerges that for naturally occurring pressures (<10 GPa), higher oxides only exist for UO{sub 2}.

Actinide chemistry in the far field

International Nuclear Information System (INIS)

Livens, F.R.; Morris, K.; Parkman, R.; Moyes, L.

1996-01-01

The environmental chemistry of the actinides is complicated due both to the extensive redox and coordination chemistry of the elements and also to the complexity of the reactive phases encountered in natural environments. In the far field, interactions with reactive surfaces, coatings and colloidal particles will play a crucial role in controlling actinide mobility. By virtue of both their abundance and reactivity; clays and other layer aluminosilicate minerals, hydrous oxides and organic matter (humic substances) are all identified as having the potential to react with actinide ions and some possible modes of interaction are described, together with experimental evidence for their occurrence. (author)

Structural organization and spectroscopy of peptide-actinide(IV) complexes

International Nuclear Information System (INIS)

Dahou, S.

2010-01-01

The contamination of living organisms by actinide elements is at the origin of both radiological and chemical toxicity that may lead to severe dysfunction. Most of the data available on the actinide interaction with biological systems are macroscopic physiological measurements and are lacking a molecular description of the systems. Because of the intricacy of these systems, classical biochemical methods are difficult to implement. Our strategy consisted in designing simplified biomimetic peptides, and describing the corresponding intramolecular interactions with actinides. A carboxylic pentapeptide of the form DDPDD has been at the starting point of this work in order to further assess the influence of the peptide sequence on the topology of the complexes.To do so, various linear (Asp/Ala permutations, peptoids) and cyclic analogues have been synthesized. Furthermore, in order to include the hydroxamic function (with a high affinity for Fe(III)) in the peptide, both desferrioxamine and acetohydroxamic acid have been investigated. However because of difficulties in synthesis, we have not been able to test these peptides. Three actinide cations have been considered at oxidation state +IV (Th, Np, Pu) and compared to Fe(III), often considered as a biological surrogate of Pu(IV). The spatial arrangement of the peptide around the cation has been probed by spectrophotometry and X-ray Absorption Spectroscopy. The spectroscopic data and EXAFS data adjustment lead us to rationalize the topology of the complexes as a function of the peptide sequence: mix hydroxy polynuclear species for linear and cyclic peptides, mononuclear for the desferrioxamine complexes. Furthermore, significant differences have appeared between Fe(III) and actinide(IV), related to differences of reactivity in aqueous medium. (author)

Research on the chemical speciation of actinides

International Nuclear Information System (INIS)

Jung, Euo Chang; Park, K. K.; Cho, H. R.

2010-04-01

A demand for the safe and effective management of spent nuclear fuel and radioactive waste generated from nuclear power plant draws increasing attention with the growth of nuclear power industry. The objective of this project is to establish the basis of research on the actinide chemistry by using advanced laser-based highly sensitive spectroscopic systems. Researches on the chemical speciation of actinides are prerequisite for the development of technologies related to nuclear fuel cycles, especially, such as the safe management of high level radioactive wastes and the chemical examination of irradiated nuclear fuels. For supporting these technologies, laser-based spectroscopies have been performed for the chemical speciation of actinide in an aqueous solutions and the quantitative analysis of actinide isotopes in spent nuclear fuels. In this report, results on the following subjects have been summarized. (1) Development of TRLFS technology for chemical speciation of actinides, (2) Development of LIBD technology for measuring solubility of actinides, (3) Chemical speciation of plutonium complexes by using a LWCC system, (4) Development of LIBS technology for the quantitative analysis of actinides, (5) Development of technology for the chemical speciation of actinides by CE, (6) Evaluation on the chemical reactions between actinides and humic substances, (7) Chemical speciation of actinides adsorbed on metal oxides surfaces, (8) Determination of actinide source terms of spent nuclear fuel

Subcritical limits for special fissile actinides

International Nuclear Information System (INIS)

Clark, H.K.

1980-01-01

Critical masses and subcritical mass limits in oxide-water mixtures were calculated for actinide nuclides other than /sup 233/U, /sup 235/U, and /sup 239/Pu that have an odd number of neutrons in the nucleus; S/sub n/ transport theory was used together with cross sections, drawn from the GLASS multigroup library, developed to provide accurate forecasts of actinide production at Savannah River

Research on the actinide chemistry in Nuclear Fuel Cycle

Energy Technology Data Exchange (ETDEWEB)

Song, Kyseok; Park, Yong Joon; Cho, Young Hwan; and others

2012-04-15

Fundamental technique to measure chemical behaviors and properties of lanthanide and actinide in radioactive waste is necessary for the development of pryochemical process. First stage, the electrochemical/spectroscopic integrated measurement system was designed and set up for spectro-electrochemical measurements of lanthanide and actinide ions in high temperature molten salt media. A compact electrochemical cell and electrode system was also developed for the minimization of reactants, and consequently minimization of radioactive waste generation. By applying these equipments, oxidation and reduction behavior of lanthanide and actinide ions in molten salt media have been made. Also, thermodynamic parameter values are determined by interpreting the results obtained from electrochemical measurements. Several lanthanide ions exhibited fluorescence properties in molten salt. Also, UV-VIS measurement provided the detailed information regarding the oxidation states of lanthanide and actinide ions in high temperature molten salt media. In the second stage, measurement system for physical properties at pyrochemical process such as viscosity, melting point and conductivity is established, and property database at different compositions of lanthanide and actinide is collected. And, both interactions between elements and properties with different potential are measured at binary composition of actinide-lanthanide in molten salt using electrochemical/spectroscopic integrated measurement system.

Separation of lanthanides (III) and actinides (III) by calixarenes containing acetamide-phosphine oxides functions

International Nuclear Information System (INIS)

Garcia Carrera, A.; Dozol, J.F.; Rouquette, H.

2001-01-01

The carbamoyl methyl phosphine oxide CMPO is the well known extractant of the TRUEX process for extraction of actinides from highly salted acidic wastes. In the framework of an European research contract coordinated by CEA/DDCC. V. Boehmer (Mainz, Germany) synthesized calix(4)arenes bearing CMPO moieties either on the wide rim, or on the narrow rim. Some of these calixarenes used at a concentration 10 -3 M are more efficient than CMPO used at a two hundred fifty fold higher concentration. Moreover, calixarene skeleton leads to a strong selectivity among lanthanides, this selectivity is much less obvious for CMPO. Selectivity order is reversed according to whether CMPO unit is borne by the wide rim or the narrow rim. The most efficient calixarenes allow actinides to be separated from most of the lanthanides except the lightest ones. (authors)

Comparative Study of f-Element Electronic Structure across a Series of Multimetallic Actinide, Lanthanide-Actinide and Lanthanum-Actinide Complexes Possessing Redox-Active Bridging Ligands

Energy Technology Data Exchange (ETDEWEB)

Schelter, Eric J.; Wu, Ruilian; Veauthier, Jacqueline M.; Bauer, Eric D.; Booth, Corwin H.; Thomson, Robert K.; Graves, Christopher R.; John, Kevin D.; Scott, Brian L.; Thompson, Joe D.; Morris, David E.; Kiplinger, Jaqueline L.

2010-02-24

A comparative examination of the electronic interactions across a series of trimetallic actinide and mixed lanthanide-actinide and lanthanum-actinide complexes is presented. Using reduced, radical terpyridyl ligands as conduits in a bridging framework to promote intramolecular metal-metal communication, studies containing structural, electrochemical, and X-ray absorption spectroscopy are presented for (C{sub 5}Me{sub 5}){sub 2}An[-N=C(Bn)(tpy-M{l_brace}C{sub 5}Me4R{r_brace}{sub 2})]{sub 2} (where An = Th{sup IV}, U{sup IV}; Bn = CH{sub 2}C{sub 6}H{sub 5}; M = La{sup III}, Sm{sup III}, Yb{sup III}, U{sup III}; R = H, Me, Et) to reveal effects dependent on the identities of the metal ions and R-groups. The electrochemical results show differences in redox energetics at the peripheral 'M' site between complexes and significant wave splitting of the metal- and ligand-based processes indicating substantial electronic interactions between multiple redox sites across the actinide-containing bridge. Most striking is the appearance of strong electronic coupling for the trimetallic Yb{sup III}-U{sup IV}-Yb{sup III}, Sm{sup III}-U{sup IV}-Sm{sup III}, and La{sup III}-U{sup IV}-La{sup III} complexes, [8]{sup -}, [9b]{sup -} and [10b]{sup -}, respectively, whose calculated comproportionation constant K{sub c} is slightly larger than that reported for the benchmark Creutz-Taube ion. X-ray absorption studies for monometallic metallocene complexes of U{sup III}, U{sup IV}, and U{sup V} reveal small but detectable energy differences in the 'white-line' feature of the uranium L{sub III}-edges consistent with these variations in nominal oxidation state. The sum of this data provides evidence of 5f/6d-orbital participation in bonding and electronic delocalization in these multimetallic f-element complexes. An improved, high-yielding synthesis of 4{prime}-cyano-2,2{prime}:6{prime},2{double_prime}-terpyridine is also reported.

Applicability of molten salt oxidation to the destruction of actinide-contaminated wastes

International Nuclear Information System (INIS)

West, M.H.; Garcia, E.; Griego, W.J.; Court, D.B.; Rodriguez, L.

1992-01-01

A 1989 ban on incineration in the state of New Mexico caused cessation of actinide-contaminated cheesecloth, paper, and wood incineration within the Plutonium Facility (TA-55) at Los Alamos National Laboratory. Subsequently, plastic wipes were substituted for cheesecloth in the cleaning of glovebox interiors. However, waste minimization is not achieved by these measures since the wipes are discarded as Waste Isolation Pilot Plant certifiable wastes. After the ban was instituted, thermal decomposition of cheesecloth under argon at elevated temperature was examined and found satisfactory although scale of operation and speed were inferior to incineration. In 1991, the ban on incineration was lifted in New Mexico but Alamos has not chosen to pursue renewal of incineration at the Plutonium Facility. This paper reports that Los Alamos is looking from alternatives to incineration and thermal decomposition which are compatible with molten salt processing technology, historically a strength in actinide research at the Laboratory. Also, the technology must significantly reduce the volume of the waste upon treatment, i.e. waste minimization. Molten salt oxidation (MSO) has the promise of such a technology

MICROBIAL TRANSFORMATIONS OF TRU AND MIXED WASTES: ACTINIDE SPECIATION AND WASTE VOLUME REDUCTION.

Energy Technology Data Exchange (ETDEWEB)

FRANCIS, A.J.; DODGE, C.J.

2006-11-16

The overall goals of this research project are to determine the mechanism of microbial dissolution and stabilization of actinides in Department of Energy's (DOE) TRU wastes, contaminated sludges, soils, and sediments. This includes (1) investigations on the fundamental aspects of microbially catalyzed radionuclide and metal transformations (oxidation/reduction reactions, dissolution, precipitation, chelation); (2) understanding of the microbiological processes that control speciation and alter the chemical forms of complex inorganic/organic contaminant mixtures; and (3) development of new and improved microbially catalyzed processes resulting in immobilization of metals and radionuclides in the waste with concomitant waste volume reduction.

MICROBIAL TRANSFORMATIONS OF TRU AND MIXED WASTES: ACTINIDE SPECIATION AND WASTE VOLUME REDUCTION

Energy Technology Data Exchange (ETDEWEB)

Francis, A.J.; Dodge, C.J.

2006-06-01

The overall goals of this research project are to determine the mechanism of microbial dissolution and stabilization of actinides in Department of Energy’s (DOE) TRU wastes, contaminated sludges, soils, and sediments. This includes (i) investigations on the fundamental aspects of microbially catalyzed radionuclide and metal transformations (oxidation/reduction reactions, dissolution, precipitation, chelation); (ii) understanding of the microbiological processes that control speciation and alter the chemical forms of complex inorganic/organic contaminant mixtures; and (iii) development of new and improved microbially catalyzed processes resulting in immobilization of metals and radionuclides in the waste with concomitant waste volume reduction.

MICROBIAL TRANSFORMATIONS OF TRU AND MIXED WASTES: ACTINIDE SPECIATION AND WASTE VOLUME REDUCTION

Energy Technology Data Exchange (ETDEWEB)

Francis, A.J.; Dodge, C.J.

2006-06-01

The overall goals of this research project are to determine the mechanism of microbial dissolution and stabilization of actinides in Department of Energy's (DOE) TRU wastes, contaminated sludges, soils, and sediments. This includes (1) investigations on the fundamental aspects of microbially catalyzed radionuclide and metal transformations (oxidation/reduction reactions, dissolution, precipitation, chelation); (2) understanding of the microbiological processes that control speciation and alter the chemical forms of complex inorganic/organic contaminant mixtures; and (3) development of new and improved microbially catalyzed processes resulting in immobilization of metals and radionuclides in the waste with concomitant waste volume reduction.

Separation and preconcentration of actinides from acidic media by extraction chromatography

International Nuclear Information System (INIS)

Horwitz, E. Philip; Chiarizia, Renato; Dietz, Mark L.; Diamond, Herbert; Nelson, Donald M.

1993-01-01

A systematic examination of the effect of nitric and hydrochloric acid concentrations and of macro levels of selected elements on the sorption of actinide ions by a novel extraction chromatographic resin comprised of a solution of octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide in tri-n-butyl phosphate supported on an inert polymeric substrate is described. Actinide sorption is demonstrated to be most efficient at high (>1 M) nitric acid concentrations, although tetra- and hexavalent actinides are strongly retained even from dilute (e.g., 0.05 M) nitric acid solutions. Macro concentrations of several common anions (e.g., PO 4 3- and SO 4 2- ) or complexing agents (e.g., oxalic acid) are shown not to adversely affect the sorption of trivalent actinides, while reducing the sorption of tetravalents. Such effects, together with oxidation state adjustments, are shown to provide a basis for the sequential elution of individual actinides and for actinide isolation from environmental and biological matrices

Some aspects of synergistic extraction of actinides and lanthanides from mixed aqueous-organic media

International Nuclear Information System (INIS)

Shukla, J.P.; Subramanian, M.S.

1981-01-01

Various aspects of the synergistic extraction and separation of actinides and lanthanides from mixed aqueous-organic solutions (polar media) have been reviewed. Notable recent developments as well as its current status in solvent extraction systems where the aqueous acidic phase contains an organic solvent which is completely miscible with water, are presented briefly. In general, extraction increases in the presence of an organic component. The less polar the additive, the higher is the tendency to form neutral metal complexes which ultimately brings about an increase in the extraction. In a polar media, synergism has mostly been observed, though antagonism is not uncommon. An attempt has been made to classify the factors that play an important role in polar phase extractions. Also, their influence particularly on the extractability of actinides and lanthanides is discussed. The discussion is limited to the factors affecting the extraction equilibria, effect of dielectric constant of the polar medium, solvation of the extracting agent and to the composition and stability of the metal complex in the organic phase. Hydroxyl (OHsup(-)) bearing organic additives, e.g. alcohols, and solvents not containing the hydroxyl group such as acetone, dimethylsulphoxide, tetrahydrofuran, amides and acetonitrile etc. are the two major classes of organic additives considered in these studies. Generally, synergistic effect in extraction of the ion-association (TBP, TOPO, sulphoxides etc.) or anion exchange (amines etc.) type is relatively more pronounced compared to other extractions. A tabular summary concerning extraction of actinides and lanthanides from polar media is appended for ready reference. (author)

Experimental studies of actinides in molten salts

Energy Technology Data Exchange (ETDEWEB)

Reavis, J.G.

1985-06-01

This review stresses techniques used in studies of molten salts containing multigram amounts of actinides exhibiting intense alpha activity but little or no penetrating gamma radiation. The preponderance of studies have used halides because oxygen-containing actinide compounds (other than oxides) are generally unstable at high temperatures. Topics discussed here include special enclosures, materials problems, preparation and purification of actinide elements and compounds, and measurements of various properties of the molten volts. Property measurements discussed are phase relationships, vapor pressure, density, viscosity, absorption spectra, electromotive force, and conductance. 188 refs., 17 figs., 6 tabs.

Experimental studies of actinides in molten salts

International Nuclear Information System (INIS)

Reavis, J.G.

1985-06-01

This review stresses techniques used in studies of molten salts containing multigram amounts of actinides exhibiting intense alpha activity but little or no penetrating gamma radiation. The preponderance of studies have used halides because oxygen-containing actinide compounds (other than oxides) are generally unstable at high temperatures. Topics discussed here include special enclosures, materials problems, preparation and purification of actinide elements and compounds, and measurements of various properties of the molten volts. Property measurements discussed are phase relationships, vapor pressure, density, viscosity, absorption spectra, electromotive force, and conductance. 188 refs., 17 figs., 6 tabs

Solid-state actinide acid phosphites from phosphorous acid melts

International Nuclear Information System (INIS)

Oh, George N.; Burns, Peter C.

2014-01-01

The reaction of UO 3 and H 3 PO 3 at 100 °C and subsequent reaction with dimethylformamide (DMF) produces crystals of the compound (NH 2 (CH 3 ) 2 )[UO 2 (HPO 2 OH)(HPO 3 )]. This compound crystallizes in space group P2 1 /n and consists of layers of uranyl pentagonal bipyramids that share equatorial vertices with phosphite units, separated by dimethylammonium. In contrast, the reaction of phosphorous acid and actinide oxides at 210 °C produces a viscous syrup. Subsequent dilution in solvents and use of standard solution-state methods results in the crystallization of two polymorphs of the actinide acid phosphites An(HPO 2 OH) 4 (An=U, Th) and of the mixed acid phosphite–phosphite U(HPO 3 )(HPO 2 OH) 2 (H 2 O)·2(H 2 O). α- and β-An(HPO 2 OH) 4 crystallize in space groups C2/c and P2 1 /n, respectively, and comprise a three-dimensional network of An 4+ cations in square antiprismatic coordination corner-sharing with protonated phosphite units, whereas U(HPO 3 )(HPO 2 OH) 2 (H 2 O) 2 ·(H 2 O) crystallizes in a layered structure in space group Pbca that is composed of An 4+ cations in square antiprismatic coordination corner-sharing with protonated phosphites and water ligands. We discuss our findings in using solid inorganic reagents to produce a solution-workable precursor from which solid-state compounds can be crystallized. - Graphical abstract: Reaction of UO 3 and H 3 PO 3 at 100 °C and subsequent reaction with DMF produces crystals of (NH 2 (CH 3 ) 2 )[UO 2 (HPO 2 OH)(HPO 3 )] with a layered structure. Reaction of phosphorous acid and actinide oxides at 210 °C produces a viscous syrup and further solution-state reactions result in the crystallization of the actinide acid phosphites An(HPO 2 OH) 4 (An=U, Th), with a three-dimensional network structure, and the mixed acid phosphite–phosphite U(HPO 3 )(HPO 2 OH) 2 (H 2 O) 2 ·(H 2 O) with a layered structure. - Highlights: • U(VI), U(IV) and Th(IV) phosphites were synthesized by solution

Actinide-Aluminate Speciation in Alkaline Radioactive Waste

International Nuclear Information System (INIS)

Clark, David L.; Fedosseev, Alexander M.

2001-01-01

Investigation of behavior of actinides in alkaline media containing AL(III) showed that no aluminate complexes of actinides in oxidation states (IIII-VIII) were formed in alkaline solutions. At alkaline precipitation IPH (10-14) of actinides in presence of AL(III) formation of aluminate compounds is not observed. However, in precipitates contained actinides (IIV)<(VI), and to a lesser degree actinides (III), some interference of components takes place that is reflected in change of solid phase properties in comparison with pure components or their mechanical mixture. The interference decreases with rise of precipitation PH and at PH 14 is exhibited very feebly. In the case of NP(VII) the individual compound with AL(III) is obtained, however it is not aluminate of neptunium(VII), but neptunate of aluminium(III) similar to neptunates of other metals obtained earlier

Recent progress in actinide and lanthanide solvent extraction

International Nuclear Information System (INIS)

Musikas, C.; Hubert, H.; Benjelloun, N.; Vitorge, P.; Bonnin, M.; Forchioni, A.; Chachaty, C.

1983-04-01

Work in progress on actinide solvent extraction is briefly reviewed in this paper. 1 H and 31 P NMR are used to elucidate several fundamental unsolved problems concerning organophosphorous extractants often used in actinides extraction: determination of site of dialkylthiophosphate protonation and addition of basic phosphine oxide to dibutylthiophosphoric acid dimer. Extraction of Am III and Eu from high radioactivity level wastes by tetrasubsituted methylene diamides is investigated. Trivalent actinide-lanthanide group are separated by solvent extraction using soft donor ligand complexes which are more stable. The synergism of dinonylnaphtalene sulfonic acid (HDNNS) associated with several neutral donors like TBP, TOPO, amides are examined in the trivalent and tetravalent actinide extraction

Advanced Aqueous Separation Systems for Actinide Partitioning

Energy Technology Data Exchange (ETDEWEB)

Nash, Kenneth L.; Clark, Sue; Meier, G Patrick; Alexandratos, Spiro; Paine, Robert; Hancock, Robert; Ensor, Dale

2012-03-21

One of the most challenging aspects of advanced processing of spent nuclear fuel is the need to isolate transuranium elements from fission product lanthanides. This project expanded the scope of earlier investigations of americium (Am) partitioning from the lanthanides with the synthesis of new separations materials and a centralized focus on radiochemical characterization of the separation systems that could be developed based on these new materials. The primary objective of this program was to explore alternative materials for actinide separations and to link the design of new reagents for actinide separations to characterizations based on actinide chemistry. In the predominant trivalent oxidation state, the chemistry of lanthanides overlaps substantially with that of the trivalent actinides and their mutual separation is quite challenging.

Research on the chemical speciation of actinides

International Nuclear Information System (INIS)

Jung, Euo Chang; Park, K. K.; Cho, H. R.

2012-04-01

A demand for the safe and effective management of spent nuclear fuel and radioactive waste generated from nuclear power plant draws increasing attention with the growth of nuclear power industry. The objective of this project is to establish the basis of research on the actinide chemistry by using highly sensitive and advanced laser-based spectroscopic systems. Researches on the chemical speciation of actinides are prerequisite for the development of technologies related to nuclear fuel cycles, especially, such as the safe management of high level radioactive wastes and the chemical examination of irradiated nuclear fuels. For supporting these technologies, laser-based spectroscopies have been applied for the chemical speciation of actinide in aqueous solutions and the quantitative analysis of actinide isotopes in spent nuclear fuels. In this report, results on the following subjects have been summarized. Development of TRLFS technology for the chemical speciation of actinides, Development of laser-induced photo-acoustic spectroscopy (LPAS) system, Application of LIBD technology to investigate dynamic behaviors of actinides dissolution reactions, Development of nanoparticle analysis technology in groundwater using LIBD, Chemical speciation of plutonium complexes by using a LWCC system, Development of LIBS technology for the quantitative analysis of actinides, Evaluation on the chemical reactions between actinides and humic substances, Spectroscopic speciation of uranium-ligand complexes in aqueous solution, Chemical speciation of actinides adsorbed on metal oxides surfaces

Fundamental Thermodynamics of Actinide-Bearing Mineral Waste Forms - Final Report

Energy Technology Data Exchange (ETDEWEB)

Williamson, Mark A.; Ebbinghaus, Bartley B.; Navrotsky, Alexandra

2001-03-01

The end of the Cold War raised the need for the technical community to be concerned with the disposition of excess nuclear weapon material. The plutonium will either be converted into mixed-oxide fuel for use in nuclear reactors or immobilized in glass or ceramic waste forms and placed in a repository. The stability and behavior of plutonium in the ceramic materials as well as the phase behavior and stability of the ceramic material in the environment is not well established. In order to provide technically sound solutions to these issues, thermodynamic data are essential in developing an understanding of the chemistry and phase equilibria of the actinide-bearing mineral waste form materials proposed as immobilization matrices. Mineral materials of interest include zircon, zirconolite, and pyrochlore. High temperature solution calorimetry is one of the most powerful techniques, sometimes the only technique, for providing the fundamental thermodynamic data needed to establish optimum material fabrication parameters, and more importantly understand and predict the behavior of the mineral materials in the environment. The purpose of this project is to experimentally determine the enthalpy of formation of actinide orthosilicates, the enthalpies of formation of actinide substituted zirconolite and pyrochlore, and develop an understanding of the bonding characteristics and stabilities of these materials.

Fundamental Thermodynamics of Actinide-Bearing Mineral Waste Forms - Final Report

International Nuclear Information System (INIS)

Williamson, Mark A.; Ebbinghaus, Bartley B.; Navrotsky, Alexandra

2001-01-01

The end of the Cold War raised the need for the technical community to be concerned with the disposition of excess nuclear weapon material. The plutonium will either be converted into mixed-oxide fuel for use in nuclear reactors or immobilized in glass or ceramic waste forms and placed in a repository. The stability and behavior of plutonium in the ceramic materials as well as the phase behavior and stability of the ceramic material in the environment is not well established. In order to provide technically sound solutions to these issues, thermodynamic data are essential in developing an understanding of the chemistry and phase equilibria of the actinide-bearing mineral waste form materials proposed as immobilization matrices. Mineral materials of interest include zircon, zirconolite, and pyrochlore. High temperature solution calorimetry is one of the most powerful techniques, sometimes the only technique, for providing the fundamental thermodynamic data needed to establish optimum material fabrication parameters, and more importantly understand and predict the behavior of the mineral materials in the environment. The purpose of this project is to experimentally determine the enthalpy of formation of actinide orthosilicates, the enthalpies of formation of actinide substituted zirconolite and pyrochlore, and develop an understanding of the bonding characteristics and stabilities of these materials

Separations chemistry for actinide elements: Recent developments and historical perspective

International Nuclear Information System (INIS)

Nash, K.L.; Choppin, G.R.

1997-01-01

With the end of the cold war, the principal mission in actinide separations has changed from production of plutonium to cleanup of the immense volume of moderately radioactive mixed wastes which resulted from fifty years of processing activities. In order to approach the cleanup task from a proper perspective, it is necessary to understand how the wastes were generated. Most of the key separations techniques central to actinide production were developed in the 40's and 50's for the identification and production of actinide elements. Total actinide recovery, lanthanide/actinide separations, and selective partitioning of actinides from inert constituents are currently of primary concern. To respond to the modern world of actinide separations, new techniques are being developed for separations ranging from analytical methods to detect ultra-trace concentrations (for bioassay and environmental monitoring) to large-scale waste treatment procedures. In this report, the history of actinide separations, both the basic science and production aspects, is examined and evaluated in terms of contemporary priorities

Study of actinide paramagnetism in solution

International Nuclear Information System (INIS)

Autillo, Matthieu

2015-01-01

The physiochemical properties of actinide (An) solutions are still difficult to explain, particularly the behavioral differences between An(III) and Ln(III). The study of actinide paramagnetic behavior may be a 'simple' method to analyze the electronic properties of actinide elements and to obtain information on the ligand-actinide interaction. The objective of this PhD thesis is to understand the paramagnetic properties of these elements by magnetic susceptibility measurements and chemical shift studies. Studies on actinide electronic properties at various oxidation states in solution were carried out by magnetic susceptibility measurements in solution according to the Evans method. Unlike Ln(III) elements, there is no specific theory describing the magnetic properties of these ions in solution. To obtain accurate data, the influence of experimental measurement technique and radioactivity of these elements was analyzed. Then, to describe the electronic structure of their low energy states, the experimental results were complemented with quantum chemical calculations from which the influence of the ligand field was studied. Finally, these interpretations were applied to better understand the variations in the magnetic properties of actinide cations in chloride and nitrate media. Information about ligand-actinide interactions may be determined from an NMR chemical shift study of actinide complexes. Indeed, modifications induced by a paramagnetic complex can be separated into two components. The first component, a Fermi contact contribution (δ_c) is related to the degree of covalency in coordination bonds with the actinide ions and the second, a dipolar contribution (δ_p_c) is related to the structure of the complex. The paramagnetic induced shift can be used only if we can isolate these two terms. To achieve this study on actinide elements, we chose to work with the complexes of dipicolinic acid (DPA). Firstly, to characterize the geometrical parameters, a

Water reactivity with mixed oxide (U,Pu)O2 surfaces

International Nuclear Information System (INIS)

Gaillard, Jeremy

2013-01-01

The interaction of water with actinides oxide surfaces remains poorly understood. The adsorption of water on PuO 2 surface and (U,Pu)O 2 surface leads to hydrogen generation through radiolysis but also surface evolution. The study of water interaction with mixed oxide (U,Pu)O 2 and PuO 2 surfaces requires the implementation of non intrusive techniques. The study of the hydration of CeO 2 surface is used to study the effectiveness of different techniques. The results show that the water adsorption leads to the surface evolution through the formation of a hydroxide superficial layer. The reactivity of water on the surface depends on the calcination temperature of the oxide precursor. The thermal treatment of hydrated surfaces can regenerate the surface. The study on CeO 2 hydration emphasizes the relevancies of these techniques in studying the hydration of surfaces. The hydrogen generation through water radiolysis is studied with an experimental methodology based on constant relative humidity in the radiolysis cell. The hydrogen accumulation is linear for the first hours and then tends to a steady state content. A mechanism of hydrogen consumption is proposed to explain the existence of the steady state of hydrogen content. This mechanism enables to explain also the evolution of the oxide surface during hydrogen generation experiments as shown by the evolution of hydrogen accumulation kinetics. The accumulation kinetics depends on the dose rate, specific surface area and the relative humidity but also on the oxide aging. The plutonium percentage appears to be a crucial parameter in hydrogen accumulation kinetics. (author) [fr

Study of Thorium Phosphate Diphosphate (TPD) formation in nitric medium for the decontamination of high activity actinides bearing effluents

International Nuclear Information System (INIS)

Rousselle, Jerome

2004-01-01

Considering several activities in the nuclear industry and research, several low-level liquids wastes (LLLW) containing actinides in nitric medium must be decontaminated before being released in the environment. These liquid wastes mainly contain significant amounts of uranium(VI), neptunium(V) and plutonium(IV). In this work, two chemical ways were studied to decontaminate LLLW then to incorporate simultaneously uranium, neptunium and plutonium in the Thorium Phosphate Diphosphate (TPD). Both ways started from a nitric solution containing thorium and the actinides considered, present at their lower stable oxidation state. The first way consisted in the initial precipitation of actinide and thorium mixed oxalate. After drying the mixture containing the powder and phosphoric acid under dried argon, a poly-phase system was obtained. It was mainly composed by a thorium-actinide oxalate-phosphate. This mixture was transformed into a TPDAn solid solution (An = U, Np and/or Pu) by heating treatment at 1200 deg. C under inert atmosphere. The second way consisted in the precipitation of a precursor of TPD, identified as the Thorium Phosphate Hydrogen Phosphate loaded with the actinides considered. The gel initially formed by mixing concentrated phosphoric acid solution with the nitric actinide solution was heated at 90 - 160 deg. C in a closed PTFE container for several weeks. It led to the TPDAn solid solutions after heating at 1100 deg. C in air or under inert argon. The efficiency of both processes was evaluated through the determination of the decontamination for each actinide considered. Considering the encouraging results obtained for both kinds of processes, some complementary studies are now required before performing the effective decontamination of real Low-Level Liquid Waste using one of the methods proposed. (author) [fr

Strength of Coriolis Coupling in actinide nuclei

International Nuclear Information System (INIS)

Peker, L.K.; Rasmussen, J.O.; Hamilton, J.H.

1982-01-01

Coriolis Coupling V/sub cor/ plays an important role in deformed nuclei. V/sub cor/ is proportional to h 2 /J[j (j + 1) -Ω (Ω + 1)]/sup 1/2/ and therefore is particularly significant in the nuclei with large j and low Ω Nilsson levels close to Fermi surface: n(i/sub 13/2/) in A = 150 to 170 rare-earth nuclei and p(i/sub 13/2/) and n(j/sub 15/2/) in A greater than or equal to 224 actinide nuclei. Because of larger j (n(j/sub 15/2/) versus n(i/sub 13/2/)) and smaller deformations (β approx. = 0.22 versus β 0.28) it was reasonable to expect that in actinide nuclei Coriolis effects are stronger than in the rare earth nuclei. Recently it was realized that the strength of observed Coriolis effects depends not only on the genuine Coriolis Coupling but also on the interplay between Coriolis ad pairing forces which leads to an interference between the wave functions of two mixing rotational bands. As a consequence the effective interaction V/sub eff/ of both bands is an oscillating function of the degree of shell filling (or chemical potential lambda F). It was shown that in the rare earth nuclei this interference strongly influenced conclusions about the trends in the Coriolis coupling strength and explained many of the observed band-mixing features (the sharpness of back banding curves, details of the blocking effect etc.). From theoretical analysis it was concluded that in the majority of actinide nuclei the effective interaction V/sub eff/ is strong, and therefore the Coriolis band-mixing have to be very strong. In this paper we would like to demonstrate that contrary to these predictions experimental data suggest that Coriolis band mixing in studied actinide nuclei is relatively weak and possibly significantly weaker than in rare earth nuclei

Successive change regularity of actinide properties with atomic number

International Nuclear Information System (INIS)

Yang Xuexian

1990-08-01

The development and achievements on chemistry of actinide elements are summarised. The relations of properties of actinides to their electronic configurations of valence electronic shells are discussed. Some anomalies of solid properties, the radius contraction, the stable state effect of f 7n -orbits (n = 0, 1, 2) and the tetrad effect of oxidation states, etc., with atomic number (Z) are described. 31 figures appended show directly the successive change regularity of actinide properties with Z

Studies of thermal-hydraulics and plant systems for actinide burning fast reactor concept

International Nuclear Information System (INIS)

Yamazaki, Seiichiro; Misumi, Masahiro; Izaki, Makoto; Koike, Hiroyuki; Tanaka, Ryokichi

1984-01-01

As one of the methods to dispose long life actinide nuclides, the actinide burning fast reactor using only actinide wastes as the fuel has been proposed. Kawasaki Heavy Industries Ltd. carried out the conceptual examination on the ABFR cooled with helium gas, cooperating with Japan Atomic Energy Research Institute, and its feasibility and problems were clarified. In this report, the setting-up of various fundamental dimensions by the parameter survey of the thermal and flowing performance of the core, the examination of the thermal and flowing characteristics of the core based on the detailed power distribution, and the examination of the plant system centering around the main cooling system are outlined. The fuel is composed of actinide oxide and diluent MgO. The diluent is used for obtaining proper excess reactivity, and MgO has been taken up also in foreign countries, considering the compatibility with actinide oxide, the easiness of reprocessing and manufacture. The fuel element is of pin type, and actinide oxide and MgO pellets are in a SUS 316 cladding tube. This ABFR can treat the wastes from ten 1000 MWe power reactors, and has the power output of about 1000 MWt. (Kako, I.)

Valence instabilities as a source of actinide system inconsistencies

International Nuclear Information System (INIS)

Sandenaw, T.A.

1979-01-01

Light actinide elements alone, and in some of their alloys, may exist as a static or dynamic mixture of two configurations. Such a state can explain both a resistivity maximum and lack of magnetic order observed in so many actinide materials, and still be compatible with the existence of f-electrons in narrow bands. Impurity elements may stabilize slightly different intermediate valence states in U, Np, and Pu, thus contributing to inconsistencies in published results. The physical property behavior of mixed-valence, rare-earth compounds is very much like that observed in development of antiphase (martensitic) structures. Martensitic transformations in U, Np, and Pu, from high-temperature b. c. c. to alpha phase, may be a way of ordering an alloy-like metal of mixed or intermediate valence. The relative stability of each phase structure may depend upon its electron-valence ratio. A Hubbard model for electron correlations in a narrow energy band has been invoked in most recent theories for explaining light actinide behavior. Such a model may also be applicable to crystal symmetry changes in martensitic transformations in actinides

Physical chemistry and modelling of the sintering of actinide oxides

International Nuclear Information System (INIS)

Lechelle, Jacques

2013-01-01

This report gives a synthesis of the work I have carried out or to which I have numerically contributed to from 1996 up to 2012 in the Department of Plutonium Uranium and minor Actinides in Cadarache CEA Center. Their main goal is the study and the modeling of the sintering process of nuclear fuels which is the unifying thread of this document. Both in order to take into account the physical and chemical features of the actinide bearing oxide material and in order to combine the different transport phenomena leading to sintering, a sub-granular scale model is under development. Extension to a varying chemical composition as well as exchanges with the gaseous phase are foreseen. A simulation on a larger scale (pellet scale) is ongoing in the framework of a PhD thesis. Validation means have been tested with (U,Pu)O 2 material on the scale of the pellet (Small Angle Neutron Diffusion), on the scale of powder granules (X-Ray High Resolution Micro-Tomography) and with CeO 2 at the 'Institut de Chimie Separative' in Marcoule on a single crystal scale (Environmental Scanning Electron Microscope). The required microstructure homogeneity for nuclear fuels has led to a campaign of experimental studies about the role of Cr 2 O 3 as a sintering aid. Whole of these studies improve our understanding of fuel sintering and hence leads to an improved mastering of this process. (author) [fr

Simultaneous separation and detection of actinides in acidic solutions using an extractive scintillating resin.

Science.gov (United States)

Roane, J E; DeVol, T A

2002-11-01

An extractive scintillating resin was evaluated for the simultaneous separation and detection of actinides in acidic solutions. The transuranic extractive scintillating (TRU-ES) resin is composed of an inert macroporous polystyrene core impregnated with organic fluors (diphenyloxazole and 1,4-bis-(4-methyl-5-phenyl-2-oxazolyl)benzene) and an extractant (octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide in tributyl phosphate). The TRU-ES resin was packed into FEP Teflon tubing to produce a flow cell (0.2-mL free column volume), which is placed into a scintillation detection system to obtain pulse height spectra and time series data during loading and elution of actinides onto/from the resin. The alpha-particle absolute detection efficiencies ranged from 77% to 96.5%, depending on the alpha energy and quench. In addition to the on-line analyses, off-line analyses of the effluent can be conducted using conventional detection methods. The TRU-ES resin was applied to the quantification of a mixed radionuclide solution and two actual waste samples. The on-line characterization of the mixed radionuclide solution was within 10% of the reported activities whereas the agreement with the waste samples was not as good due to sorption onto the sample container walls and the oxidation state of plutonium. Agreement between the on-line and off-line analyses was within 35% of one another for both waste samples.

Pitched blade impeller - an option for mixing in continuous actinide reconversion process

International Nuclear Information System (INIS)

Tripathi, V.M.; Suresh Kumar, K.; Sreekumar, G.; Sugilal, G.

2016-01-01

In nuclear fuel cycle, current methodology for Pu reconversion involves Pu(IV)-oxalate precipitation as a semi continuous/batch process mode for a predetermined volume of Pu(NO 3 ) 4 solution in a long single column with a marine propeller type stirrer. In this process the slurry is being drained from bottom of the vessel leading to a possibility of accumulation of precipitate in the vessel which is an unfavorable condition for continuous process. As continuous reconversion process is a requirement to meet high through put of reprocessing plants, the conventional process has to be improvised with reference to its slurry exit point through overflow line. Although marine propeller type stirrer ensures an axial flow, it is not a choice for uniform solid suspension in a reactor vessel. A better alternate for complete suspension of solid in tall reactor is pitched blade turbine. Moreover pitched blade impellers are effective in low bottom clearance which ensures a thorough mixing of reactants. Present study focuses on feasibility of pitched blade impeller for mixing of reactants in a continuous actinide oxalate precipitation reactor with over flow line

Actinides and environmental interfaces: striving for molecular-level understanding

International Nuclear Information System (INIS)

Heino Nitsche

2005-01-01

Actinides can undergo a variety of complex chemical reactions in the environment. In addition to the formation of solid precipitates, colloids and dissolved solution species common to aqueous systems, actinide ions can interact with the surrounding geo and biomedia to change oxidation states or sorb on surfaces and colloids. The rate of migration is determined by aqueous solubility, and interactions with solid surfaces such as minerals, soils, natural organic matter, and soil microorganisms Sorption of aqueous actinide species on biological and geological matrices can be quantitatively described by a surface complexation or site-binding model. The disadvantage of this model is the difficulty in the experimental determination of the model parameters and surface reaction constants. Usually, a set of surface reactions and species are proposed based on knowledge of the solution speciation of the solute, and the reaction constants are usually derived by fitting computer-calculated absorption curves to experimental data. Because this process typically involves a large number of potentially adjustable parameters, it is likely to lead to non-unique parameter fitting and does not always result in a consistent set of parameters for the same systems. A fundamental molecular-level understanding of sorption processes of actinides on environmental surfaces is required to better understand and predict their transport behavior in nature. Several different surface spectroscopic techniques have been applied to the characterization of the adsorbed species and surface reactions and a direct determination of the sorbed species and surface reactions has become possible. The non-linear optical techniques of second harmonic and sum frequency generation (SHG and SFG) are ideally suited to study surfaces and interfaces of mineral oxides, biosurfactants and biopolymers, organic adlayers adsorbed on solid/mineral surfaces and soil organic matter, including humic and fulvic acids. Resonant

Aqueous electrochemical mechanisms in actinide residue processing. 1998 annual progress report

International Nuclear Information System (INIS)

Blanchard, D.L. Jr.; Burns, C.J.; Morris, D.E.; Smith, W.H.

1998-01-01

'New and/or improved solutions to the stabilization and volume reduction of nuclear materials processing residues are urgently needed. Mediated electrochemical oxidation/reduction (MEO/R) processes are one such approach for incinerator ash, combustibles, and other solid residues. However, questions remain concerning the mechanisms of these processes, and how they might be optimized. In addition, further research is merited to extend their range of applicability. Recent advances in the study of heterogeneous electron transfer in solid substrates have opened the door for the re-examination of electron transfer processes associated with redox mediated actinide dissolution. The authors develop a deeper understanding of the thermodynamic and mechanistic aspects of heterogeneous electron transfer that lie at the heart of these MEO/R processes. They will also develop and test new approaches based on the results of these fundamental studies using actual residue materials. Key aspects of this proposal include: (1) determination of the potential windows for oxidation/reduction of colloidal actinide oxides and actinide-bearing oxide and organic substrates and the e transfer kinetic parameters that govern the current--overpotential characteristics; (2) development of adaptations of mediation schemes and application of co-mediation reagents for oxidative and reductive dissolution based on complexation of the surface-bound or solid-phase actinides and/or the dissolved redox mediator;and (3) execution of bench-scale tests of new MEO/R schemes on actual residue materials.'

Molten salt destruction process for mixed wastes

International Nuclear Information System (INIS)

Upadhye, R.S.; Wilder, J.G.; Karlsen, C.E.

1993-04-01

We are developing an advanced two-stage process for the treatment of mixed wastes, which contain both hazardous and radioactive components. The wastes, together with an oxidant gas, such as air, are injected into a bed of molten salt comprising a mixture of sodium-, potassium-, and lithium-carbonates, with a melting point of about 580 degree C. The organic constituents of the mixed waste are destroyed through the combined effect of pyrolysis and oxidation. Heteroatoms. such as chlorine, in the mixed waste form stable salts, such as sodium chloride, and are retained in the melt. The radioactive actinides in the mixed waste are also retained in the melt because of the combined action of wetting and partial dissolution. The original process, consists of a one-stage unit, operated at 900--1000 degree C. The advanced two-stage process has two stages, one for pyrolysis and one for oxidation. The pyrolysis stage is designed to operate at 700 degree C. The oxidation stage can be operated at a higher temperature, if necessary

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

Science.gov (United States)

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.

The Thermodynamic Properties of the f-Elements and their Compounds. Part 2. The Lanthanide and Actinide Oxides

Energy Technology Data Exchange (ETDEWEB)

Konings, Rudy J. M., E-mail: rudy.konings@ec.europa.eu; Beneš, Ondrej; Kovács, Attila; Manara, Dario; Sedmidubský, David [European Commission, Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, 76125 Karlsruhe (Germany); Gorokhov, Lev; Iorish, Vladimir S.; Yungman, Vladimir; Shenyavskaya, E.; Osina, E. [Joint Institute for High Temperatures, Russian Academy of Sciences, 13-2 Izhorskaya Street, Moscow 125412 (Russian Federation)

2014-03-15

A comprehensive review of the thermodynamic properties of the oxide compounds of the lanthanide and actinide elements is presented. The available literature data for the solid, liquid, and gaseous state have been analysed and recommended values are presented. In case experimental data are missing, estimates have been made based on the trends in the two series, which are extensively discussed.

Minor actinide transmutation using minor actinide burner reactors

International Nuclear Information System (INIS)

Mukaiyama, T.; Yoshida, H.; Gunji, Y.

1991-01-01

The concept of minor actinide burner reactor is proposed as an efficient way to transmute long-lived minor actinides in order to ease the burden of high-level radioactive waste disposal problem. Conceptual design study of minor actinide burner reactors was performed to obtain a reactor model with very hard neutron spectrum and very high neutron flux in which minor actinides can be fissioned efficiently. Two models of burner reactors were obtained, one with metal fuel core and the other with particle fuel core. Minor actinide transmutation by the actinide burner reactors is compared with that by power reactors from both the reactor physics and fuel cycle facilities view point. (author)

Behavior of molybdenum in mixed-oxide fuel

International Nuclear Information System (INIS)

Giacchetti, G.; Sari, C.

1976-01-01

Metallic molybdenum, Mo--Ru--Rh--Pd alloys, barium, zirconium, and tungsten were added to uranium and uranium--plutonium oxides by coprecipitation and mechanical mixture techniques. This material was treated in a thermal gradient similar to that existing in fuel during irradiation to study the behavior of molybdenum in an oxide matrix as a function of the O/(U + Pu) ratio and some added elements. Result of ceramographic and microprobe analysis shows that when the overall O/(U + Pu) ratio is less than 2, molybdenum and Mo--Ru--Rh--Pd alloy inclusions are present in the uranium--plutonium oxide matrix. If the O/(U + Pu) ratio is greater than 2, molybdenum oxidizes to MoO 2 , which is gaseous at a temperature approximately 1000 0 C. Molybdenum oxide vapor reacts with barium oxide and forms a compound that exists as a liquid phase in the columnar grain region. Molybdenum oxide also reacts with tungsten oxide (tungsten is often present as an impurity in the fuel) and forms a compound that contains approximately 40 wt percent of actinide metals. The apparent solubility of molybdenum in uranium and uranium--plutonium oxides, determined by electron microprobe, was found to be less than 250 ppM both for hypo- and hyperstoichiometric fuels

3 and 4 oxidation state element solubilities in borosilicate glasses. Implement to actinides in nuclear glasses

International Nuclear Information System (INIS)

Cachia, J.N.

2005-12-01

In order to ensure optimal radionuclides containment, the knowledge of the actinide loading limits in nuclear waste glasses and also the comprehension of the solubilization mechanisms of these elements are essential. A first part of this manuscript deals with the study of the differences in solubility of the tri and tetravalent elements (actinides and surrogates) particularly in function of the melting temperature. The results obtained indicate that trivalent elements (La, Gd, Nd, Am, Cm) exhibit a higher solubility than tetravalent elements (Hf, Th, Pu). Consequently, it was planned to reduce plutonium at the oxidation state (III), the later being essentially tetravalent in borosilicate glasses. An innovating reduction process of multi-valent elements (cerium, plutonium) using silicon nitride has been developed in a second part of this work. Reduced plutonium-bearing glasses synthesized by Si 3 N 4 addition made it possible to double the plutonium solubility from 2 to 4 wt% at 1200 deg C. A structural approach to investigate the differences between tri and tetravalent elements was finally undertaken. These investigations were carried out by X-rays Absorption Spectroscopy (EXAFS) and NMR. Trivalent rare earth and actinide elements seem to behave as network modifiers while tetravalent elements rather present true intermediaries' behaviour. (author)

Characterization Of Actinides In Simulated Alkaline Tank Waste Sludges And Leachates

International Nuclear Information System (INIS)

Nash, Kenneth L.

2008-01-01

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 actinides 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.

CHARACTERIZATION OF ACTINIDES IN SIMULATED ALKALINE TANK WASTE SLUDGES AND LEACHATES

Energy Technology Data Exchange (ETDEWEB)

Nash, Kenneth L.

2008-11-20

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 actinides 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.

Solubility of actinides and surrogates in nuclear glasses

International Nuclear Information System (INIS)

Lopez, Ch.

2003-01-01

The nuclear wastes are currently incorporated in borosilicate glass matrices. The resulting glass must be perfectly homogeneous. The work discussed here is a study of actinide (thorium and plutonium) solubility in borosilicate glass, undertaken to assess the extent of actinide solubility in the glass and to understand the mechanisms controlling actinide solubilization. Glass specimens containing; actinide surrogates were used to prepare and optimize the fabrication of radioactive glass samples. These preliminary studies revealed that actinide Surrogates solubility in the glass was enhanced by controlling the processing temperature, the dissolution kinetic of the surrogate precursors, the glass composition and the oxidizing versus reducing conditions. The actinide solubility was investigated in the borosilicate glass. The evolution of thorium solubility in borosilicate glass was determined for temperatures ranging from 1200 deg C to 1400 deg C.Borosilicate glass specimens containing plutonium were fabricated. The experimental result showed that the plutonium solubility limit ranged from 1 to 2.5 wt% PuO 2 at 1200 deg C. A structural approach based on the determination of the local structure around actinides and their surrogates by EXAFS spectroscopy was used to determine their structural role in the glass and the nature of their bonding with the vitreous network. This approach revealed a correlation between the length of these bonds and the solubility of the actinides and their surrogates. (author)

Evaluation of the alveolar macrophage role in the pulmonary distribution of actinide oxides

International Nuclear Information System (INIS)

Guezingar-Liebard, Florence

1999-01-01

Actinide oxide inhalation is potentially a risk during the fuel fabrication process in the electronuclear industry. These particles can induce pulmonary lesions. The alveolar macrophage play an important role in the particle sequestration and transport but the actinide toxicity towards these cells is not well known. The aim of this work was to characterize the evolution of particle localisation in lungs after inhalation and to evaluate the role of macrophages in the lesion histo-genesis. We have used of a solid track detector to visualise alpha dose distribution within lung tissue. After 237 NpO 2 , MOX or PuO 2 inhalation by rats, different kinetics of clearance were observed for the sub-pleural and peri-bronchial areas compared to the others alveolar areas. For initial lung burdens that alter the lung clearance, particle aggregates were observed. Their kinetic and localisation vary depending on the aerosol, for a same global dose delivered to the lungs. This could be due to the different specific alpha activities of the particles and to the particle number deposited in the lung to obtain a similar burden but it could be also due to a chemical toxicity of neptunium higher than that of the others actinides. The flow cytometry methods developed allow us to measure apoptosis, phagocytosis and free radicals generation. After addition of soluble uranium to the culture medium, similar results were obtained using either alveolar macrophages extracted from rats or a macrophage cell line. This work confirms that alveolar macrophages are involved in the aggregate formation which induces heterogeneous dose distribution within the different lung tissues. (author) [fr

Effect of spectral characterization of gaseous fuel reactors on transmutation and burning of actinides

Energy Technology Data Exchange (ETDEWEB)

Fung, C.; Anghaie, S. [Florida Univ., Wilmington, NC (United States)

2007-07-01

Gaseous Core Reactors (GCR) are fueled with stable uranium compounds in a reflected cavity. The spectral characteristics of neutrons in GCR systems could shift from one end of the spectrum to the other end by changing design parameters such as reflector material and thickness, uranium enrichment, and the average operational temperature and pressure. The rate of actinide generation, transmutation, and burnup is highly influenced by the average neutron energy in reactor core. In particular, the production rate and isotopic mix of plutonium are highly dependent on the neutron spectrum in the reactor. Other actinides of primary interest to this work are neptunium-237 and americium-241 due to their pivotal impact on high-level nuclear waste disposal. In all cavity reactors including GCR's, the reflector material and thickness are the most important design parameters in determining the core spectrum. The increase in the gaseous fuel pressure and enrichment results in relative shift of neutron population toward energies greater than 2 eV. Reflector materials considered in this study are beryllium oxide, lithium hydride, lithium deuteride, zirconium carbide, graphite, lead, and tungsten. Results of the study suggest that the beryllium oxide and tungsten reflected GCR systems set the lower (softest) and upper (hardest) limits of neutron spectra, respectively. The inventory of actinides with half-lives greater than 1000 years can be minimized by increasing neutron flux level in the reactor core. The higher the neutron flux, the lower the inventory of these actinides. The majority of the GCR designs maintained a flux level on the order of 10{sup 15} cm{sup -2}*s{sup -1} while the PWR flux is one order of magnitude lower. The inventory of the feeder isotopes to Np{sup 237} including U{sup 237}, Pu{sup 241}, and Am{sup 241} decreases with relative shift of neutron spectrum toward higher energies. This is due to increased resonance absorption in these isotopes due to higher

Interaction of actinides with natural microporous materials: a review

International Nuclear Information System (INIS)

Misaelides, P.; Godelitsas, A.

1998-01-01

Natural microporous materials include several types of minerals such as zeolites, clay minerals, micas, iron- and manganese-oxides/hydroxides/oxyhydroxides present in various geological environments and soil formations. The transport of the actinide elements in the environment is mainly performed through aquatic pathways (streams, rivers, underground waters) and their mobility is strongly related to the interaction of their dissolved species with geological materials and especially with the highly sorptive microporous minerals. The existing studies mainly concern the sorption of Th, U, Np, Pu and Am from aqueous media by clay minerals and zeolites as well as the determination of the corresponding chemical processes taking place at the mineral-water interface. The investigation techniques also include advanced spectroscopic methods such as Extended X-ray Absorption Fine Structure Spectroscopy (EXAFS), Rutherford Backscattered Spectroscopy (RBS), X-ray Photoelectron Spectroscopy (XPS) and Raman Spectroscopy. These techniques significantly contribute to the characterization of the reacted mineral surfaces and to the explanation of the structural and compositional characteristics of the sorbed actinide species. Theoretical models regarding the aqueous chemistry and speciation of the actinides have also been developed aiming the elucidation of the complex actinide sorption mechanisms. Finally, this contribution also includes some recently obtained data concerning the interaction of actinides with todorokite (a naturally occurring microporous manganese-oxide of technological importance) and granitic micas (biotite) correlated with the nuclear waste disposal in geological formations

Removal of actinide elements from high level radioactive waste by trialkylphosphine oxide (TRPO)

International Nuclear Information System (INIS)

Song Chongli; Yang Dazhu; He Longhai; Xu Jingming; Zhu Yongjun

1992-03-01

The modified TRPO process for removing actinide elements from synthetic solution, which was taken from reprocessing of power reactor nuclear fuel, was verified by cascade experiment. Neptunium valence was adjusted in the process for improving neptunium removing efficiency. At 1 mol/L concentration of HNO 3 of feed solution and after a few stages of extraction with 30% t=TRPO kerosene, over 99.9% of Am, Pu, Np and U could be removed from HAW (high level radioactive waste) solution. The stripping of actinides loaded in TRPO are accomplished by high concentration nitric acid, oxalic acid and sodium carbonate instead of amino carboxylic complexing agents used in previous process. The actinides stripped were divided into three groups, which are Am + RE, Np + Pu, and U, and the cross contamination between them is small. Behaviours of F.P. elements are divided into three types which are not extracted, little extracted and extracted elements. The extracted elements are rare earth and Pd, Zr and Mo which are co-extracted with actinides. The separation factor between actinides and other two types of F.P.elements will increase if more scrubbing sections are added in the process. The relative concentration profile of actinide elements and Tc in various stages as well as the distribution of actinides and F.P. elements in the process stream solutions are also presented

Rapid ion-exchange separations of actinides

International Nuclear Information System (INIS)

Usuda, Shigekazu

1988-01-01

For the purpose of studying short-lived actinide nuclides, three methods for rapid ion exchange separation of actinide elements with mineral acid-alcohol mixed media were developed: anion exchange with nitric acid-methyl alcohol mixed media to separate the transplutonium and rare earth elements from target material, U or Pu and Al catcher foils; anion exchange with hydrochloric acid-methyl alcohol media to separate Am+Cm, Bk and Cf+Fm from the target, catcher foils and major fission products; and cation exchange with hydrochloric acid-methyl alcohol media and with concentrated hydrochloric acid to separate the transplutonium elements as a group from the rare earths after eliminating the large amounts of U, Al, Cu, Fe etc. The methods enable one to perform rapid and effective separation at elevated temperature (90 deg C) and immediate source preparation for alpha-ray spectrometry. (author) 47 refs.; 10 figs

Quantum-chemical consideration of extermal valent forms of actinides

International Nuclear Information System (INIS)

Ionova, G.V.; Pershina, V.G.; Spitsyn, V.I.

1982-01-01

Stability of valent forms of actinides that has not yet studied experimentally, is considered within the framework of quantum-chemical considerations. Oxidizing potentials E 0 for actinide elements are determined theoretically. A dependence of the definite valent state stability on relativistic effect is shown. A conclusion is made that oxidizing potential E 0 (4-5) for americium should be higher than E 0 (4-5) for plutonium. A relatively small oxidizing potential E 0 (4-5) for curium speaks about principle possibility of production of five-valent curium in solution, though it is less stable than the six-valent one. Oxidizing potential corresponding to transition of three-valent californium into the four-valent state should be less than the value adopted in literature. A relatively small oxidizing potential of californium E 0 (4-5) speaks about possible existence of five-valent californium in solution

Denaturing of plutonium by transmutation of minor-actinides for enhancement of proliferation resistance

International Nuclear Information System (INIS)

Sagara, Hiroshi; Saito, Masaki; Peryoga, Yoga; Ezoubtchenko, Alexey; Takivayev, Alan

2005-01-01

Feasibility study for the plutonium denaturing by utilizing minor-actinide transmutation in light water reactors has been performed. And the intrinsic feature of proliferation resistance of plutonium has been discussed based on IAEA's publication and Kessler's proposal. The analytical results show that not only 238 Pu but also other plutonium isotopes with even-mass-number have very important role for denaturing of plutonium due to their relatively large critical mass and noticeably high spontaneous fission neutron generation. With the change of the minor-actinide doping ratio in U-Pu mix oxide fuel and moderator to fuel ratio, it is found that the reactor-grade plutonium from conventional light water reactors can be denatured to satisfy the proliferation resistance criterion based on the Kessler's proposal but not to be sufficient for the criterion based on IAEA's publication. It has been also confirmed that all the safety coefficients take negative value throughout the irradiation. (author)

Actinide transmutation using inert matrix fuels versus recycle in a low conversion fast burner reactor

Energy Technology Data Exchange (ETDEWEB)

Deinert, M.R.; Schneider, E.A.; Recktenwald, G.; Cady, K.B. [The Department of Mechanical Engineering, The University of Texas at Austin, 1 University Station, C2200, Austin, 78712 (United States)

2009-06-15

Reducing the disposal burden of the long lived radioisotopes that are contained within spent uranium oxide fuel is essential for ensuring the sustainability of nuclear power. Because of their non-fertile matrices, inert matrix fuels (IMFs) could allow light-water reactors to achieve a significant burn down of plutonium and minor actinides that are that are currently produced as a byproduct of operating light-water reactors. However, the extent to which this is possible is not yet fully understood. We consider a ZrO{sub 2} based IMF with a high transuranic loading and show that the neutron fluence (and the subsequent fuel residence time required to achieve it) present a practical limit for the achievable actinide burnup. The accumulation of transuranics in spent uranium oxide fuel is a major obstacle for the sustainability of nuclear power. While commercial light-water reactors (LWR's) produce these isotopes, they can be used to transmute them. At present, the only viable option for doing this is to partly fuel reactors with mixed oxide fuel (MOX) made using recycled plutonium. However, because of parasitic neutron capture in the uranium matrix of MOX, considerable plutonium and minor actinides are also bred as the fuel is burned. A better option is to entrain the recycled isotopes in a non-fertile matrix such as ZrO{sub 2}. Inert matrices such as these were originally envisioned for burning plutonium from dismantled nuclear weapons [1]. However, because they achieve a conversion ratio of zero, they have also been considered as a better alternative to MOX [2-6]. Plutonium and minor actinides dominate the long term heat and radiological outputs from spent nuclear fuel. Recent work has shown that that IMFs can be used to reduce these outputs by at least a factor of four, on a per unit of energy generated basis [6]. The degree of reduction is strongly dependent on IMF burnup. In principle, complete transmutation of the transuranics could be achieved though this

Advanced Aqueous Separation Systems for Actinide Partitioning

Energy Technology Data Exchange (ETDEWEB)

Nash, Ken [Washington State Univ., Pullman, WA (United States); Martin, Leigh [Idaho National Lab. (INL), Idaho Falls, ID (United States); Lumetta, Gregg [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

2015-04-02

One of the most challenging aspects of advanced processing of used nuclear fuel is the separation of transplutonium actinides from fission product lanthanides. This separation is essential if actinide transmutation options are to be pursued in advanced fuel cycles, as lanthanides compete with actinides for neutrons in both thermal and fast reactors, thus limiting efficiency. The separation is difficult because the chemistry of Am3+ and Cm3+ is nearly identical to that of the trivalent lanthanides (Ln3+). The prior literature teaches that two approaches offer the greatest probability of devising a successful group separation process based on aqueous processes: 1) the application of complexing agents containing ligand donor atoms that are softer than oxygen (N, S, Cl-) or 2) changing the oxidation state of Am to the IV, V, or VI state to increase the essential differences between Am and lanthanide chemistry (an approach utilized in the PUREX process to selectively remove Pu4+ and UO22+ from fission products). The latter approach offers the additional benefit of enabling a separation of Am from Cm, as Cm(III) is resistant to oxidation and so can easily be made to follow the lanthanides. The fundamental limitations of these approaches are that 1) the soft(er) donor atoms that interact more strongly with actinide cations than lanthanides form substantially weaker bonds than oxygen atoms, thus necessitating modification of extraction conditions for adequate phase transfer efficiency, 2) soft donor reagents have been seen to suffer slow phase transfer kinetics and hydro-/radiolytic stability limitations and 3) the upper oxidation states of Am are all moderately strong oxidants, hence of only transient stability in media representative of conventional aqueous separations systems. There are examples in the literature of both approaches having been described. However, it is not clear at present that any extant process is sufficiently robust for application at the scale

Minor Actinide Transmutation Physics for Low Conversion Ratio Sodium Fast Reactors

International Nuclear Information System (INIS)

Mehdi Asgari; Samuel E. Bays; Benoit Forget; Rodolfo Ferrer

2007-01-01

The effects of varying the reprocessing strategy used in the closed cycle of a Sodium Fast Reactor (SNF) prototype are presented in this paper. The isotopic vector from the aqueous separation of transuranic (TRU) elements in Light Water Reactor (LWR) spent nuclear fuel (SNF) is assumed to also vary according to the reprocessing strategy of the closed fuel cycle. The decay heat, gamma energy, and neutron emission of the fuel discharge at equilibrium are found to vary depending on the separation strategy. The SFR core used in this study corresponds to a burner configuration with a conversion ratio of ∼0.5 based on the Super-PRISM design. The reprocessing strategies stemming from the choice of either metal or oxide fuel for the SFR are found to have a large impact on the equilibrium discharge decay heat, gamma energy, and neutron emission. Specifically, metal fuel SFR with pyroprocessing of the discharge produces the largest amount of TRU consumption (166 kg per Effective Full Power Year or EFPY), but also the highest decay heat, gamma energy, and neutron emission. On the other hand, an oxide fuel SFR with PUREX reprocessing minimizes the decay heat and related parameters of interest to a minimum, even when compared to thermal Mixed Oxide (MOX) or Inert Matrix Fuel (IMF) on a per mass basis. On an assembly basis, however, the metal SFR discharge has a lower decay heat than an equivalent oxide SFR assembly for similar minor actinide consumptions (∼160 kg/EFPY.) Another disadvantage in the oxide PUREX reprocessing scenario is that there is no consumption of americium and curium, since PUREX reprocessing separates these minor actinides (MA) and requires them to be disposed of externally

Thermochemical and thermophysical properties of minor actinide compounds

International Nuclear Information System (INIS)

Minato, Kazuo; Takano, Masahide; Otobe, Haruyoshi; Nishi, Tsuyoshi; Akabori, Mitsuo; Arai, Yasuo

2009-01-01

Burning or transmutation of minor actinides (MA: Np, Am, Cm) that are classified as the high-level radioactive waste in the current nuclear fuel cycle is an option for the advanced nuclear fuel cycle. Although the thermochemical and thermophysical properties of minor actinide compounds are essential for the design of MA-bearing fuels and analysis of their behavior, the experimental data on minor actinide compounds are limited. To support the research and development of the MA-bearing fuels, the property measurements were carried out on minor actinide nitrides and oxides. The lattice parameters and their thermal expansions were measured by high-temperature X-ray diffractometry. The specific heat capacities were measured by drop calorimetry and the thermal diffusivities by laser-flash method. The thermal conductivities were determined by the specific heat capacities, thermal diffusivities and densities. The oxygen potentials were measured by electromotive force method.

Investigation of waste form materials suitable for immobilizing actinide elements in high-level waste

International Nuclear Information System (INIS)

Hayakawa, Issei; Kamizono, Hiroshi

1992-07-01

The microstructure of waste form materials suitable for immobilizing actinide elements can be classified into the following two categories. (1) Actinide elements are immobilized in an crystallized matrix after the formation of solid solution or compounds. (2) Actinide elements are immobilized in a durable material by encapsulation. Based on crystal chemistry, durability data, phase diagrams, compositions of natural minerals, eleven oxide compounds and one non-oxide compound are pointed out to be new candidates included in category (1). The other survey on material compositions, manufacturing conditions and feasibility shows that SiC, glassy carbon, ZrO 2 , Ti-O-Si-C ceramics are preferable matrix materials included in category (2). Polymers and fine powders are suitable as starting materials for the encapsulation of actinide elements because of their excellent sinterability. (author) 50 refs

Minor Actinide Separations Using Ion Exchangers Or Ionic Liquids

International Nuclear Information System (INIS)

Hobbs, D.; Visser, A.; Bridges, N.

2011-01-01

This project seeks to determine if (1) inorganic-based ion exchange materials or (2) electrochemical methods in ionic liquids can be exploited to provide effective Am and Cm separations. Specifically, we seek to understand the fundamental structural and chemical factors responsible for the selectivity of inorganic-based ion-exchange materials for actinide and lanthanide ions. Furthermore, we seek to determine whether ionic liquids can serve as the electrolyte that would enable formation of higher oxidation states of Am and other actinides. Experiments indicated that pH, presence of complexants and Am oxidation state exhibit significant influence on the uptake of actinides and lanthanides by layered sodium titanate and hybrid zirconium and tin phosphonate ion exchangers. The affinity of the ion exchangers increased with increasing pH. Greater selectivity among Ln(III) ions with sodium titanate materials occurs at a pH close to the isoelectric potential of the ion exchanger. The addition of DTPA decreased uptake of Am and Ln, whereas the addition of TPEN generally increases uptake of Am and Ln ions by sodium titanate. Testing confirmed two different methods for producing Am(IV) by oxidation of Am(III) in ionic liquids (ILs). Experimental results suggest that the unique coordination environment of ionic liquids inhibits the direct electrochemical oxidation of Am(III). The non-coordinating environment increases the oxidation potential to a higher value, while making it difficult to remove the inner coordination of water. Both confirmed cases of Am(IV) were from the in-situ formation of strong chemical oxidizers.

The electronic structure of the lanthanides and actinides, a comparison

International Nuclear Information System (INIS)

Edelstein, N.M.

1998-01-01

Full text: Optical spectra of the two f-element series (the lanthanides and actinides) are comparable in many respects. For the trivalent ions isolated in single crystals, both series exhibit rich, narrow line spectra. These data can be analysed in terms of a parametric model based on a free-ion Hamiltonian plus the addition of a crystal field Hamiltonian. For most systems the agreement between the calculated and experimental energy levels is quite good. In the actinide series there appears to be a correlation between the magnitude of the crystal field and the inadequacy of the fits. The early actinides exhibit multiple oxidation states for which there is no precedent in the lanthanide series. The parametric model mentioned earlier has been utilized for some tetravalent actinide systems with reasonably good results. A selective survey of results describing the similarities and differences of various lanthanide and actinide systems will be given

Reversible optical sensor for the analysis of actinides in solution

International Nuclear Information System (INIS)

Lesage, B.; Picard, S.; Serein-Spirau, F.; Lereporte, J.P.

2007-01-01

In this work is presented a concept of reversible optical sensor for actinides. It is composed of a p doped conducing polymer support and of an anion complexing the actinides. The chosen conducing polymer is the thiophene-2,5-di-alkoxy-benzene whose solubility and conductivity are perfectly known. The actinides selective ligand is a lacunar poly-oxo-metallate such as P 2 W 17 O 61 10- or SiW 11 O 39 8- which are strong anionic complexing agents of actinides at the oxidation state (IV) even in a very acid medium. The sensor is prepared by spin coating of the composite mixture 'polymer + ligand' on a conducing glass electrode and then tested towards its optical and electrochemical answer in presence of uranium (IV). The absorption change due to the formation of cations complexes by poly-oxo-metallate reveals the presence of uranium (IV). After the measurement, the sensor is regenerated by anodic polarization of the support and oxidation of the uranium (IV) into uranium (VI) which weakly interacts with the poly-oxo-metallate and is then released in solution. (O.M.)

The effect of corrosion product colloids on actinide transport

International Nuclear Information System (INIS)

Gardiner, M.P.; Smith, A.J.; Williams, S.J.

1992-01-01

The near field of the proposed UK repository for ILW/LLW will contain containers of conditioned waste in contact with a cementious backfill. It will contain significant quantities of iron and steel, Magnox and Zircaloy. Colloids deriving from their corrosion products may possess significant sorption capacity for radioelements. If the colloids are mobile in the groundwater flow, they could act as a significant vector for activity transport into the far field. The desorption of plutonium and americium from colloidal corrosion products of iron and zirconium has been studied under chemical conditions representing the transition from the near field to the far field. Desorption R d values of ≥ 5 x 10 6 ml g -1 were measured for both actinides on these oxides and hydroxides when actinide sorption took place under the near-field conditions and desorption took place under the far-field conditions. Desorption of the actinides occurred slowly from the colloids under far-field conditions when the colloids had low loadings of actinide and more quickly at high loadings of actinide. Desorbed actinide was lost to the walls of the experimental vessel. (author)

Analysis of the Gas Core Actinide Transmutation Reactor (GCATR)

Science.gov (United States)

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

1977-01-01

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

Fundamental thermodynamics of actinide-bearing mineral waste forms. 1998 annual progress report

International Nuclear Information System (INIS)

Ebbinghaus, B.B.; Williamson, M.A.

1998-01-01

'The end of the Cold War raised the need for the technical community to be concerned with the disposition of excess nuclear weapon material. The plutonium will either be converted into mixed-oxide fuel for use in nuclear reactors or immobilized in glass or ceramic waste forms and placed in a repository. The stability and behavior of plutonium in the ceramic materials as well as the phase behavior and stability of the ceramic material in the environment is not well established. In order to provide technically sound solutions to these issues, thermodynamic data are essential in developing an understanding of the chemistry and phase equilibria of the actinide-bearing mineral waste form materials proposed as immobilization matrices. Mineral materials of interest include zircon, zirconolite, and pyrochlore. High temperature solution calorimetry is one of the most powerful techniques, sometimes the only technique, for providing the fundamental thermodynamic data needed to establish optimum material fabrication parameters, and more importantly, understand and predict the behavior of the mineral materials in the environment. The purpose of this project is to experimentally determine the enthalpy of formation of actinide orthosilicates, the enthalpy of formation of actinide substituted zircon, zirconolite and pyrochlore, and develop an understanding of the bonding characteristics and stability of these materials. This report summarizes work after eight months of a three year project.'

Nuclear fuel cycle-oriented actinides separation in China

Energy Technology Data Exchange (ETDEWEB)

Chen, Jing; He, Xihong; Wang, Jianchen [Tsinghua Univ., Beijing (China). Inst. of Nuclear and New Energy Technology

2014-04-01

In the last decades, the separation of actinides was widely and continuously studied in China. A few kinds of salt-free reductants to adjust Pu and Np valences have been investigated. N,N-dimethylhydroxylamine is a good reductant with high reduction rate constants for the co-reduction of Pu(IV) and Np(VI), and monomethylhydrazine is a simple compound for the individual reduction of Np(VI). Advanced PUREX based on Organic Reductants (APOR) was proposed. Trialkylphosphine oxide (TRPO) with a single functional group was found to possess strong affinity to tri-, tetra- and hexa-valent actinides. TRPO process has been first explored in China for actinides partitioning from high level waste and the good partitioning performance was demonstrated by the hot test. High extraction selectivity for trivalent actinides over lanthanides by dialkyldithiophosphinic acids was originally found in China. A separation process based on purified Cyanex 301 for the separation of Am from lanthanides was presented and successfully tested in a battery of miniature centrifugal contactors. (orig.)

Preparation of minor actinides targets or blankets by means of ionic exchange resin

Energy Technology Data Exchange (ETDEWEB)

Picart, S.; Mokhtari, H.; Jobelin, I. [CEA Marcoule, Nucl Energy Div, RadioChem and Proc Dept, Actinides Chem and Convers, F-30207 Bagnols Sur Ceze (France)

2010-07-01

The conversion of minor actinides to fuel starting materials for transmutation in a closed nuclear cycle is a big challenge for the next decades and the development of Gen(IV) nuclear systems. Conversion routes are numerous, but one needs to prove that they can be adapted to handle minor actinides. One of them is called the resin process and is particularly attractive because it stands for a 'dustless' process as it produces microspheres of oxide or carbide after thermal treatment of the loaded resin. The study presented herein focuses on the experiments and tests which enable us to optimize the fixation of minor actinides onto ionic exchange resin and their carbonization into oxide type materials. (authors)

Preparation of minor actinides targets or blankets by means of ionic exchange resin

International Nuclear Information System (INIS)

Picart, S; Mokhtari, H; Jobelin, I; Ramiere, I

2010-01-01

The conversion of minor actinides to fuel starting materials for transmutation in a closed nuclear cycle is a big challenge for the next decades and the development of Gen(IV) nuclear systems. Conversion routes are numerous, but one needs to prove that they can be adapted to handle minor actinides. One of them is called the resin process and is particularly attractive because it stands for a 'dustless' process as it produces microspheres of oxide or carbide after thermal treatment of the loaded resin. The study presented herein focuses on the experiments and tests which enable us to optimize the fixation of minor actinides onto ionic exchange resin and their carbonization into oxide type materials.

Coprecipitation of aluminium with hydroxides of tetra-, penta- and hexavalent actinides

International Nuclear Information System (INIS)

Yusov, A.B.; Budantseva, N.A.; Anan'ev, A.V.; Fedoseev, A.M.

2000-01-01

By the methods of IR spectroscopy and powder x-ray diffractometry precipitates formed in alkaline medium by actinide (4, 5, 6) in the presence of aluminium are studied. It is shown that in studied conditions formation of actinide aluminates not occurs. In the same time in the process of precipitation interaction of aluminium hydroxocomplexes with U(6) and Th(4) ions probably takes place. Hypothesis is expressed that possibility of aluminium hydroxocomplexes interaction with actinides in different oxidation state is depended on peculiarities of hydrolytic behaviour of the lasts [ru

Photochemical reactions of actinide ions

International Nuclear Information System (INIS)

Tomiyasu, Hiroshi

1995-01-01

This paper reviews the results of photochemical studies of actinide ions, which have been performed in our research group for past several years as follows: I) behavior of the excited uranyl(VI) ion; II) photo-reductions of the uranyl ion with organic and inorganic compounds; III) photo-oxidations of uranium(IV) and plutonium(III) in nitric acid solutions. (author)

JOWOG 22/2 - Actinide Chemical Technology (July 9-13, 2012)

Energy Technology Data Exchange (ETDEWEB)

Jackson, Jay M. [Los Alamos National Laboratory; Lopez, Jacquelyn C. [Los Alamos National Laboratory; Wayne, David M. [Los Alamos National Laboratory; Schulte, Louis D. [Los Alamos National Laboratory; Finstad, Casey C. [Los Alamos National Laboratory; Stroud, Mary Ann [Los Alamos National Laboratory; Mulford, Roberta Nancy [Los Alamos National Laboratory; MacDonald, John M. [Los Alamos National Laboratory; Turner, Cameron J. [Los Alamos National Laboratory; Lee, Sonya M. [Los Alamos National Laboratory

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 a 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.

Solubilities of Actinide Oxides in the KURT Groundwater

International Nuclear Information System (INIS)

Kim, Seung Soo; Baik, Min Hoon; Choi, Jong Won

2009-12-01

For the estimation of solubilities of actinides in a deep underground condition, The solubilities of UO 2 , ThO 2 , NpO 2 and Am(OH) 3 in the KURT ground water have been measured under various redox conditions, and their solubilities and aqueous species in the same conditions as the experimental solutions were also calculated by using a geochemical code. Then these results were compared with each other as well as with literature results. For the calculation of solubility of a radionuclide, the thermodynamic data of the radionuclide complex from OECD/NEA, Nagra/PSI, KAERI, JAEA, SKB and recent literatures were collected and compared. Additionally, the methods for the correction of ionic strength and temperature of the solution were described in this report. The analysis techniques and recent research for measurement of species of actinides were also introduced. The concentrations of U, Th and Np dissolved were less than 10 -7 mol/L under Eh≤-0.2 of reducing condition from experiment and calculation, and the solubility of PuO 2 (cr) was estimated as lower than that of UO 2 (cr) by 1 ∼ 2 orders. However if amount of carbonate ion in the ground water increased, the concentration of tetra-valance actinides at pH 8 ∼ 11 would be greatly increased. The 1x10 -6 mol/L of americium might be a little conservative value in KURT groundwater. While carbonate or hydroxo-carbonatec complexes were presumed to be the dominant aqueous species in -0.2 ∼ -0.3 V of Eh and weakly alkaline solution, hydroxo complexes are dominant in strong reducing and high pH solution

Partitioning of actinides from high level waste of PUREX origin using octylphenyl-N,N'-diisobutylcarbamoylmethyl phosphine oxide (CMPO)-based supported liquid membrane

International Nuclear Information System (INIS)

Ramanujam, A.; Dhami, P.S.; Gopalakrishnan, V.; Dudwadkar, N.L.; Chitnis, R.R.; Mathur, J.N.

1999-01-01

The present studies deal with the application of the supported liquid membrane (SLM) technique for partitioning of actinides from high level waste of PUREX origin. The process uses a solution of octylphenyl-N,N'-diisobutylcarbamoylmethyl phosphine oxide (CMPO) in n-dodecane as a carrier with a polytetrafluoroethylene support and a mixture of citric acid, formic acid, and hydrazine hydrate as the receiving phase. The studies involve the investigation of such parameters as carrier concentration in SLM, acidity of the feed, and the feed composition. The studies indicated good transport of actinides like neptunium, americium, and plutonium across the membrane from nitric acid medium. A high concentration of uranium in the feed retards the transport of americium, suggesting the need for prior removal of uranium from the waste. The separation of actinides from uranium-lean simulated samples as well as actual high level waste has been found to be feasible using the above technique

Minimization of actinide waste by multi-recycling of thoriated fuels in the EPR reactor

Directory of Open Access Journals (Sweden)

Nuttin A.

2012-02-01

Full Text Available The multi-recycling of innovative uranium/thorium oxide fuels for use in the European Pressurized water Reactor (EPR has been investigated. If increasing quantities of 238U, the fertile isotope in standard UO2 fuel, are replaced by 232Th, then a greater yield of new fissile material (233U is produced during the cycle than would otherwise be the case. This leads to economies of natural uranium of around 45% if the uranium in the spent fuel is multi-recycled. In addition we show that minor actinide and plutonium waste inventories are reduced and hence waste radio-toxicities and decay heats are up to a factor of 20 lower after 103 years. Two innovative fuel types named S90 and S20, ThO2 mixed with 90% and 20% enriched UO2 respectively, are compared as an alternative to standard uranium oxide (UOX and uranium/plutonium mixed oxide (MOX fuels at the longest EPR fuel discharge burn-ups of 65 GWd/t. Fissile and waste inventories are examined, waste radio-toxicities and decay heats are extracted and safety feedback coefficients are calculated.

Synthesis of tetravalent actinide chlorides. Versatile compounds for actinide chemistry

Energy Technology Data Exchange (ETDEWEB)

Maerz, Juliane [Helmholtz-Zentrum Dresden-Rossendorf e.V., Dresden (Germany). Div. Chemistry of the F-Elements

2016-07-01

Anhydrous actinide tetrachlorides (AnCl{sub 4}) were synthesized under mild conditions to provide versatile compounds for actinide chemistry. They enable a direct access to actinide complexes with organic and inorganic ligands.

Method for the concentration and separation of actinides from biological and environmental samples

International Nuclear Information System (INIS)

Horwitz, E.P.; Dietz, M.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. 3 figs

Sorption Speciation of Lanthanides/Actinides on Minerals by TRLFS, EXAFS and DFT Studies: A Review

Directory of Open Access Journals (Sweden)

Xiaoli Tan

2010-11-01

Full Text Available Lanthanides/actinides sorption speciation on minerals and oxides by means of time resolved laser fluorescence spectroscopy (TRLFS, extended X-ray absorption fine structure spectroscopy (EXAFS and density functional theory (DFT is reviewed in the field of nuclear disposal safety research. The theoretical aspects of the methods are concisely presented. Examples of recent research results of lanthanide/actinide speciation and local atomic structures using TRLFS, EXAFS and DFT are discussed. The interaction of lanthanides/actinides with oxides and minerals as well as their uptake are also of common interest in radionuclide chemistry. Especially the sorption and inclusion of radionuclides into several minerals lead to an improvement in knowledge of minor components in solids. In the solid-liquid interface, the speciation and local atomic structures of Eu(III, Cm(III, U(VI, and Np(IV/VI in several natural and synthetic minerals and oxides are also reviewed and discussed. The review is important to understand the physicochemical behavior of lanthanides/actinides at a molecular level in the natural environment.

Covalent bonding in heavy metal oxides

Energy Technology Data Exchange (ETDEWEB)

Bagus, Paul S.; Nelin, Connie J.; Hrovat, Dave A.; Ilton, Eugene S.

2017-04-07

Novel theoretical methods were used to quantify the magnitude and the energetic contributions of 4f/5f-O2p and 5d/6d-O2p interactions to covalent bonding in lanthanide and actinide oxides. Although many analyses have neglected the involvement of the frontier d orbitals, the present study shows that f and d covalency are of comparable importance. Two trends are identified. As is expected, the covalent mixing is larger when the nominal oxidation state is higher. More subtly, the importance of the nf covalent mixing decreases sharply relative to (n+1)d as the nf occupation increases. Atomic properties of the metal cations that drive these trends are identified.

Removal of inhaled industrial mixed oxide aerosols from Beagle dogs by lung lavage and chelation therapy

International Nuclear Information System (INIS)

Muggenburg, B.A.; Mewhinney, J.A.; Eidson, A.F.; Guilmette, R.A.

1978-01-01

An experiment was conducted in 15 adult Beagle dogs to evaluate lung lavage and chelation therapy for the removal of inhaled particles of mixed actinide oxides. The dogs were divided into three groups of five dogs each. Each group was exposed to an aerosol from a different industrial process. Group 1 was exposed to mixed oxide material which had been calcined at 750 0 C collected from a ball milling process. Group 2 was exposed to mixed oxide material from a centerless grinding operation which had been previously heat treated to 1750 0 C. The third group was exposed to 239 PuO 2 not containing uranium from a V-blending procedure which had been heat treated at 850 0 C. After exposure, three dogs in each group were given ten lung lavages and 18 intravenous injections of calcium trisodium diethylenetriaminepentaacetate (DTPA). All dogs were sacrificed 64 days after inhalation exposure. The tissues were radioanalyzed for plutonium and americium. Fluorimetric analyses for uranium in the tissues are in progress. The urine, feces and lavage fluid are also being analyzed for plutonium, americium and uranium. The distribution of plutonium and americium expressed as percentages of the sacrifice body burden was similar in the tissues of the treated and unteated dogs. The lungs contained most of the radionuclides with a small amount in the liver, skeleton and tracheobronchial lymph nodes. The percentage of the sacrifice body burden of americium and plutonium that was present in the lung was less in the treated dogs and was higher in the TBLN's and skeleton than in the untreated dogs. The ratio of Pu/Am was higher in the lungs than in the original material obtained from the industrial sites suggesting a shorter retention time for americium than plutonium to 64 days in the dog

Design of unique pins for irradiation of higher actinides in a fast reactor

International Nuclear Information System (INIS)

Basmajian, J.A.; Birney, K.R.; Weber, E.T.; Adair, H.L.; Quinby, T.C.; Raman, S.; Butler, J.K.; Bateman, B.C.; Swanson, K.M.

1982-03-01

The actinides produced by transmutation reactions in nuclear reactor fuels are a significant factor in nuclear fuel burnup, transportation and reprocessing. Irradiation testing is a primary source of data of this type. A segmented pin design was developed which provides for incorporation of multiple specimens of actinide oxides for irradiation in the UK's Prototype Fast Reactor (PFR) at Dounreay Scotland. Results from irradiation of these pins will extend the basic neutronic and material irradiation behavior data for key actinide isotopes

Molecular and electronic structure of actinide hexa-cyanoferrates; Structure moleculaire et electronique des hexacyanoferrates d'actinides

Energy Technology Data Exchange (ETDEWEB)

Bonhoure, I

2001-07-01

The goal of this work is to improve our knowledge on the actinide-ligand bond properties. To this end, the hexacyanoferrate entities have been used as pre-organized ligand. We have synthesized, using mild chemistry, the following series of complexes: An{sup IV}[Fe{sup II}(CN){sub 6}].xH{sub 2}O (An = Th, U, Np, Pu); Am{sup III}[Fe{sup III}(CN){sub 6}].xH{sub 2}O; Pu {sup III}[Co{sup III}(CN){sub 6}].xH{sub 2}O and K(H?)An{sup III}[Fe{sup II}(CN){sub 6}].xH{sub 2}O (An = Pu, Am). The metal oxidation states have been obtained thanks to the {nu}{sub CN}, stretching vibration and to the actinide L{sub III} absorption edge studies. As Prussian Blue, the An{sup IV}[Fe{sup II}(CN){sub 6}].xH{sub 2}O (An = Np, Pu) are class II of Robin and Day compounds. X-ray Diffraction has shown besides that these complexes crystallize in the P6{sub 3}/m space group, as the isomorphic LaKFe(CN){sub 6}.4H{sub 2}O complex used as structural model. The EXAFS oscillations at the iron K edge and at the An L{sub III} edge allowed to determine the An-N, An-O, Fe-C and Fe-N distances. The display of the multiple scattering paths for both edges explains the actinide contribution absence at the iron edge, whereas the iron signature is present at the actinide edge. We have shown that the actinide coordination sphere in actinides hexa-cyanoferrates is comparable to the one of lanthanides. However, the actinides typical behavior towards the lanthanides is brought to the fore by the An{sup IV} versus Ln{sup III} ions presence in this family of complexes. Contrarily to the 4f electrons, the 5f electrons influence the electronic properties of the compounds of this family. However, the gap between the An-N and Ln-N distances towards the corresponding metals ionic radii do not show any covalence bond evolution between the actinide and lanthanide series. (author)

Hydrothermal processing of actinide contaminated organic wastes

International Nuclear Information System (INIS)

Worl, A.; Buelow, S.J.; Le, L.A.; Padilla, D.D.; Roberts, J.H.

1997-01-01

Hydrothermal oxidation is an innovative process for the destruction of organic wastes, that occurs above the critical temperature and pressure of water. The process provides high destruction and removal efficiencies for a wide variety of organic and hazardous substances. For aqueous/organic mixtures, organic materials, and pure organic liquids hydrothermal processing removes most of the organic and nitrate components (>99.999%) and facilitates the collection and separation of the actinides. We have designed, built and tested a hydrothermal processing unit for the removal of the organic and hazardous substances from actinide contaminated liquids and solids. Here we present results for the organic generated at the Los Alamos National Laboratory Plutonium Facility

Actinide separation by electrorefining

International Nuclear Information System (INIS)

Fusselman, S.P.; Gay, R.L.; Grantham, L.F.; Grimmett, D.L.; Roy, J.J.; Inoue, T.; Hijikata, T.; Krueger, C.L.; Storvick, T.S.; Takahashi, N.

1995-01-01

TRUMP-S is a pyrochemical process being developed for the recovery of actinides from PUREX wastes. This paper describes development of the electrochemical partitioning step for recovery of actinides in the TRUMP-S process. The objectives are to remove 99 % of each actinide from PUREX wastes, with a product that is > 90 % actinides. Laboratory tests indicate that > 99 % of actinides can be removed in the electrochemical partitioning step. A dynamic (not equilibrium) process model predicts that 90 wt % product actinide content can be achieved through 99 % actinide removal. Accuracy of model simulation results were confirmed in tests with rare earths. (authors)

Multiscale structural characterizations of mixed U(iv)-An(iii) oxalates (An(iii) = Pu or Am) combining XAS and XRD measurements.

Science.gov (United States)

Arab-Chapelet, B; Martin, P M; Costenoble, S; Delahaye, T; Scheinost, A C; Grandjean, S; Abraham, F

2016-04-28

Mixed actinide(III,IV) oxalates of the general formula M2.2UAn(C2O4)5·nH2O (An = Pu or Am and M = H3O(+) and N2H5(+)) have been quantitatively precipitated by oxalic precipitation in nitric acid medium (yield >99%). Thorough multiscale structural characterization using XRD and XAS measurements confirmed the existence of mixed actinide oxalate solid solutions. The XANES analysis confirmed that the oxidation states of the metallic cations, tetravalent for uranium and trivalent for plutonium and americium, are maintained during the precipitation step. EXAFS measurements show that the local environments around U(+IV), Pu(+III) and Am(+III) are comparable, and the actinides are surrounded by ten oxygen atoms from five bidentate oxalate anions. The mean metal-oxygen distances obtained by XAS measurements are in agreement with those calculated from XRD lattice parameters.

Applicability of a valence fluctuation model to the observed physical property response of actinide materials

International Nuclear Information System (INIS)

Sandenaw, T.A.

1978-01-01

It is shown that the physical property behavior of the light actinide elements, U, Np, and Pu, and certain of their alloys, is like that of known mixed-valence, R.E. metallic compounds. It is inferred that interconfiguration fluctuation (ICF) theory should also be applicable to actinide materials

Solubility of actinides and surrogates in nuclear glasses; Solubilite des actinides et de leurs simulants dans les verres nucleaires. Limites d'incorporation et comprehension des mecanismes

Energy Technology Data Exchange (ETDEWEB)

Lopez, Ch

2003-07-01

The nuclear wastes are currently incorporated in borosilicate glass matrices. The resulting glass must be perfectly homogeneous. The work discussed here is a study of actinide (thorium and plutonium) solubility in borosilicate glass, undertaken to assess the extent of actinide solubility in the glass and to understand the mechanisms controlling actinide solubilization. Glass specimens containing; actinide surrogates were used to prepare and optimize the fabrication of radioactive glass samples. These preliminary studies revealed that actinide Surrogates solubility in the glass was enhanced by controlling the processing temperature, the dissolution kinetic of the surrogate precursors, the glass composition and the oxidizing versus reducing conditions. The actinide solubility was investigated in the borosilicate glass. The evolution of thorium solubility in borosilicate glass was determined for temperatures ranging from 1200 deg C to 1400 deg C.Borosilicate glass specimens containing plutonium were fabricated. The experimental result showed that the plutonium solubility limit ranged from 1 to 2.5 wt% PuO{sub 2} at 1200 deg C. A structural approach based on the determination of the local structure around actinides and their surrogates by EXAFS spectroscopy was used to determine their structural role in the glass and the nature of their bonding with the vitreous network. This approach revealed a correlation between the length of these bonds and the solubility of the actinides and their surrogates. (author)

Actinide partitioning-transmutation program final report. IV. Miscellaneous aspects

International Nuclear Information System (INIS)

Alexander, C.W.; Croff, A.G.

1980-09-01

This report discusses seven aspects of actinide partitioning-transmutation (P-T) which are important in any complete evaluation of this waste treatment option but which do not fall within other major topical areas concerning P-T. The so-called miscellaneous aspects considered are (1) the conceptual design of a shipping cask for highly neutron-active fresh and spent P-T fuels, (2) the possible impacts of P-T on mixed-oxide fuel fabrication, (3) alternatives for handling the existing and to-be-produced spent fuel and/or wastes until implementation of P-T, (4) the decay and dose characteristics of P-T and standard reactor fuels, (5) the implications of P-T on currently existing nuclear policy in the United States, (6) the summary costs of P-T, and (7) methods for comparing the risks, costs, and benefits of P-T

Study on the leaching behavior of actinides from nuclear fuel debris

Science.gov (United States)

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.

Orbitally-driven magnetism in light actinide systems

International Nuclear Information System (INIS)

Cooper, B.R.; Los Alamos National Lab.

1987-01-01

We are interested in understanding the solid-state behavior characteristic of the transition regime between itinerant (bonding) and localized (correlated ionic) f-electron behavior in light actinide (uranium, neptunium and plutonium) systems. For the light actinides, the degree of f-electron localization is sensitive to chemical environment and varies widely depending on specific compound or alloy. It is important for any meaningful theory to reflect this sensitivity to chemical environment. We have focussed our attention initially on magnetic behavior, since the pertinent orbitally-driven magnetic behavior is both interesting in itself and valuable as a diagnostic tool for the f-electron behavior and sensitivity to chemical environment. The key aspect of the electronic behavior is the hybridization (mixing) of the f electrons with band electrons of other than f atomic parentage. To treat effects of hybridization quantitatively, we transform the physical mixing mathematically to resonant scattering of band electrons off f electrons. Anisotropic magnetic properties provide a way to measure the weighting of resonant scattering channels, and this weighting reflects the sensitivity to chemical environment. (orig.)

Adsorption of actinides by chelating agents containing benzene rings, fixed on charcoal

International Nuclear Information System (INIS)

Valentini Ganzerli, M.T.; Crespi Caramella, V.; Maggi, L.

1999-01-01

The focus of this paper is on the analysis of the actinides in the hydrosphere to study their environmental dispersion. The 8-hydroxyquinoline family and the benzohydroxamic acid have a complexing ability towards the actinides, even if in different oxidation states. Taking advantage of this ability, their salts with some organic acids or bases were prepared. In this way compounds were obtained easily incorporated into active charcoal. Only a small amount of the prepared adsorber may be equilibrated with large sample volumes. Subsequently it can be recovered by filtration. The adsorbed ions may be then re-dissolved with a small volume of the appropriate eluting solution. The 8-hydroxy-quinolines and the 8-hydroxyquinoline produced salts with the benzilic acid. These compounds similarly behave and show wide adsorption coefficients for solutions of pH higher than 3. The adsorption takes place by means of the formation of a complex of the actinide ion with the hydroxyquinoline moiety and also with the benzilic anion. Provided that the active extracting agent is not dissolved in a medium but fixed into a solid phase, the whole adsorption process may be regarded as a solvent extraction reaction. The benzohydroxamic acid was treated with the diphenylamine or with the tribenzylamine to obtain salts, later adsorbed into the charcoal. The adsorption of actinide ions seems to take place by means of a precipitation mechanism of the actinide ions with the hydroxamate ions for solution of pH higher than 3.5. Also in this case high values were obtained for the distribution coefficients. The actinide ions act similarly in the +4 or +6 oxidation state towards the prepared adsorber series. Therefore, it is possible to use only one adsorber to concentrate all actinides. Methods of analysis of actinides in the environment may be suitably set up and the concentration step based on these new prepared adsorber may improve the whole procedure. (authors)

Fabrication of nuclear fuel by powder injection moulding: Study of the binders systems and the de-binding of feedstock containing actinide powder

International Nuclear Information System (INIS)

Bricout, J.

2012-01-01

Powder Injection Moulding (PIM) is identified as an innovative process for the nuclear fuel fabrication. Technological breakthrough compared to the current process of powder metallurgy, the impact of actinide powder's specificities on the different steps of PIM is performed. Alumina powders simulating actinide powder have been implemented with a reference binders system. Thermal and rheological studies show the injectability and the de-binding of feedstocks with adequate solid loading (≥50 %vol), thanks to the de-agglomeration during the mixing step, which allow to obtain net shape fuel pellet. Specific surface area of powders, acting as a key role in behaviour's feedstocks, has been integrated in analysis models of viscosity prediction according to the shear rate. Also conducted studies on uranium oxide powder show that the selected binders systems, which have a compatible rheological behaviour with PIM process, impact the de-agglomeration of powder and final microstructure of the fuel pellet, consistent with the results obtained on alumina powders. Independent behaviour of binders and uranium oxide powder, showing no adverse chemical reaction against the PIM process, show a residual mass of carbon of about 150 ppm after sintering. Binders system using polystyrene, resistant to radiolysis phenomena and loadable more than 50 %(vol) of actinide powder, shows the promising potential of PIM process for the fuel fabrication. (author) [fr

Chemical aspects of actinides in the geosphere: towards a rational nuclear materials management

International Nuclear Information System (INIS)

Allen, P; Sylwester, E

2001-01-01

A complete understanding of actinide interactions in the geosphere is paramount for developing a rational Nuclear and Environmental Materials Management Policy. One of the key challenges towards understanding the fate and transport of actinides is determining their speciation (i.e., oxidation state and structure). Since an element's speciation directly dictates physical properties such as toxicity and solubility, this information is critical for evaluating and controlling the evolution of an actinide element through the environment. Specific areas within nuclear and environmental management programs where speciation is important are (1) waste processing and separations; (2) wasteform materials for long-term disposition; and (3) aqueous geochemistry. The goal of this project was to develop Actinide X-ray Absorption Spectroscopy ( U S ) as a core capability at LLNL and integrate it with existing facilities, providing a multi-technique approach to actinide speciation. XAS is an element-specific structural probe which determines the oxidation state and structure for most atoms. XAS can be more incisive than other spectroscopies because it originates from an atomic process and the information is always attainable, regardless of an element's speciation. Despite the utility, XAS is relatively complex due to the need for synchrotron radiation and significant expertise with data acquisition and analysis. The coupling of these technical hurdles with the safe handling of actinides at a general user synchrotron facility such as the Stanford Synchrotron Radiation Facility (SSRL) make such experiments even more difficult. As a result, XAS has been underutilized by programs that could benefit by its application. We achieved our project goals by implementing key state-of-the-art Actinide XAS instrumentation at SSRL (Ge detector and remote positioning equipment), and by determining the chemical speciation of actinides (Th, U, and Np) in aqueous solutions, wasteform cements, and

Actinide metals

Energy Technology Data Exchange (ETDEWEB)

Brown, Paul L. [Geochem Australia, Kiama, NSW (Australia); Ekberg, Christian [Chalmers Univ. of Technology, Goeteborg (Sweden). Nuclear Chemistry/Industrial Materials Recycling

2016-07-01

All isotopes of actinium are radioactive and exist in aqueous solution only in the trivalent state. There have been very few studies on the hydrolytic reactions of actinium(III). The hydrolysis reactions for uranium would only be important in alkaline pH conditions. Thermodynamic parameters for the hydrolysis species of uranium(VI) and its oxide and hydroxide phases can be determined from the stability and solubility constants. The hydrolytic behaviour of neptunium(VI) is quite similar to that of uranium(VI). The solubility constant of NpO{sub 2}OH(am) has been reported a number of times for both zero ionic strength and in fixed ionic strength media. Americium can form four oxidation states in aqueous solution, namely trivalent, tetravalent, pentavalent and hexavalent. Desire, Hussonnois and Guillaumont determined stability constants for the species AmOH{sup 2+} for the actinides, plutonium(III), americium(III), curium(III), berkelium(III) and californium(III) using a solvent extraction technique.

Actinide metals

International Nuclear Information System (INIS)

Brown, Paul L.; Ekberg, Christian

2016-01-01

All isotopes of actinium are radioactive and exist in aqueous solution only in the trivalent state. There have been very few studies on the hydrolytic reactions of actinium(III). The hydrolysis reactions for uranium would only be important in alkaline pH conditions. Thermodynamic parameters for the hydrolysis species of uranium(VI) and its oxide and hydroxide phases can be determined from the stability and solubility constants. The hydrolytic behaviour of neptunium(VI) is quite similar to that of uranium(VI). The solubility constant of NpO 2 OH(am) has been reported a number of times for both zero ionic strength and in fixed ionic strength media. Americium can form four oxidation states in aqueous solution, namely trivalent, tetravalent, pentavalent and hexavalent. Desire, Hussonnois and Guillaumont determined stability constants for the species AmOH 2+ for the actinides, plutonium(III), americium(III), curium(III), berkelium(III) and californium(III) using a solvent extraction technique.

Thermodynamic Properties of Actinides and Actinide Compounds

Science.gov (United States)

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.

Actinide separation chemistry in nuclear waste streams and materials

International Nuclear Information System (INIS)

1997-12-01

The separation of actinide elements from various waste materials, produced either in nuclear fuel cycles or in past nuclear weapons production, represents a significant issue facing developed countries. Improvements in the efficiencies of the separation processes can be expected to occur as a result of better knowledge of the elements in these complex matrices. The Nuclear Science Committee of the OECD/NEA has established a task force of experts in actinide separation chemistry to review current and developing separation techniques and chemical processes. The report consist of eight chapters. In Chapter 1 the importance of actinide separation chemistry in the fields of waste management and its background are summarized.In Chapter 2 the types of waste streams are classified according to their relative importance, by physical form and by source of actinides. The basic data of actinide chemical thermodynamics, such as oxidation states, hydrolysis, complexation, sorption, Gibbs energies of formation, and volatility, were collected and are presented in Chapter 3. Actinide analyses related to separation processes are also mentioned in this chapter. The state of the art of actinide separation chemistry is classified in three groups, including hydrometallurgy, pyrochemical process and process based on fields, and is described in Chapter 4 along with the relationship of kinetics to separations. In Chapter 5 basic chemistry research needs and the inherent limitation on separation processes are discussed. Prioritization of research and development is discussed in Chapter 6 in the context of several attributes of waste management problems. These attributes include: mass or volume of waste; concentration of the actinide in the waste; expected difficulty of treating the wastes; short-term hazard of the waste; long-term hazard of the waste; projected cost of treatment; amount of secondary waste. Based on the priority, recommendations were made for the direction of future research

Actinide separation chemistry in nuclear waste streams and materials

Energy Technology Data Exchange (ETDEWEB)

NONE

1997-12-01

The separation of actinide elements from various waste materials, produced either in nuclear fuel cycles or in past nuclear weapons production, represents a significant issue facing developed countries. Improvements in the efficiencies of the separation processes can be expected to occur as a result of better knowledge of the elements in these complex matrices. The Nuclear Science Committee of the OECD/NEA has established a task force of experts in actinide separation chemistry to review current and developing separation techniques and chemical processes. The report consist of eight chapters. In Chapter 1 the importance of actinide separation chemistry in the fields of waste management and its background are summarized.In Chapter 2 the types of waste streams are classified according to their relative importance, by physical form and by source of actinides. The basic data of actinide chemical thermodynamics, such as oxidation states, hydrolysis, complexation, sorption, Gibbs energies of formation, and volatility, were collected and are presented in Chapter 3. Actinide analyses related to separation processes are also mentioned in this chapter. The state of the art of actinide separation chemistry is classified in three groups, including hydrometallurgy, pyrochemical process and process based on fields, and is described in Chapter 4 along with the relationship of kinetics to separations. In Chapter 5 basic chemistry research needs and the inherent limitation on separation processes are discussed. Prioritization of research and development is discussed in Chapter 6 in the context of several attributes of waste management problems. These attributes include: mass or volume of waste; concentration of the actinide in the waste; expected difficulty of treating the wastes; short-term hazard of the waste; long-term hazard of the waste; projected cost of treatment; amount of secondary waste. Based on the priority, recommendations were made for the direction of future research

Partitioning and transmutation of actinides and fission products

International Nuclear Information System (INIS)

Baetsle, L.H.

1993-01-01

The world's nuclear power plants have a total installed capacity of approximately 340 GWe. They give rise to an annual volume of approximately 9000 t of radioactive waste, which is reprocessed, separated from its plutonium content, contained, and stored in repositories to close the nuclear fuel cycle. Direct disposal is being discussed as an alternative to this procedure. As repositories in suitable types of host rock are not operational, the only viable solution is long-term interim storage above ground. If the volumes of radioactive waste are to be reduced, the longlived actinides and fission products must be partitioned. Isotope partitioning in accelerators, though still sounding like science fiction, may soon be indispensable as the third way of treating radioactive waste. The use of mixed oxide fuel in light water reactors and fast breeder reactors both help to limit waste arisings and protect the long-term continuity of raw materials supply. However, both require public acceptance if they are to succeed. (orig.) [de

Process for denitrating waste solutions containing nitrates and actinides with simultaneous separation of the actinides

International Nuclear Information System (INIS)

Gompper, K.

1986-01-01

The invention is intended to reduce the acid and nitrate content of nitrate waste solutions, to reduce the total salt content of the waste solution, to remove the actinides contained in it by precipitation, without any danger of violent reactions or an increase in the volume of the waste solution. The invention achieves this by mixing the waste solution with diethyl oxalate at room temperature and heating the mixture to at least 80 0 C. (orig./PW) [de

Neutronic and Logistic Proposal for Transmutation of Plutonium from Spent Nuclear Fuel as Mixed-Oxide Fuel in Existing Light Water Reactors

International Nuclear Information System (INIS)

Trellue, Holly R.

2004-01-01

The use of light water reactors (LWRs) for the destruction of plutonium and other actinides [especially those in spent nuclear fuel (SNF)] is being examined worldwide. One possibility for transmutation of this material is the use of mixed-oxide (MOX) fuel, which is a combination of uranium and plutonium oxides. MOX fuel is used in nuclear reactors worldwide, so a large experience base for its use already exists. However, to limit implementation of SNF transmutation to only a fraction of the LWRs in the United States with a reasonable number of license extensions, full cores of MOX fuel probably are required. This paper addresses the logistics associated with using LWRs for this mission and the design issues required for full cores of MOX fuel. Given limited design modifications, this paper shows that neutronic safety conditions can be met for full cores of MOX fuel with up to 8.3 wt% of plutonium

Process for denitrating waste solutions containing nitric acid actinides simultaneously separating the actinides

International Nuclear Information System (INIS)

Gompper, K.

1984-01-01

The invention should reduce the acid and nitrate content of waste solutions containing nitric acid as much as possible, should reduce the total salt content of the waste solution, remove the actinides contained in it by precipitation and reduce the α radio-activity in the remaining solution, without having to worry about strong reactions or an increase in the volume of the waste solution. The invention achieves this by mixing the waste solution with diethyl oxalate at room temperature and heating the mixture to at least 80 0 C. (orig.) [de

Mathematical modeling of the effects of aerobic and anaerobic chelate biodegradation on actinide speciation

International Nuclear Information System (INIS)

Banaszak, J.E.; VanBriesen, J.; Rittmann, B.E.; Reed, D.T.

1998-01-01

Biodegradation of natural and anthropogenic chelating agents directly and indirectly affects the speciation, and, hence, the mobility of actinides in subsurface environments. We combined mathematical modeling with laboratory experimentation to investigate the effects of aerobic and anaerobic chelate biodegradation on actinide [Np(IV/V), Pu(IV)] speciation. Under aerobic conditions, nitrilotriacetic acid (NTA) biodegradation rates were strongly influenced by the actinide concentration. Actinide-chelate complexation reduced the relative abundance of available growth substrate in solution and actinide species present or released during chelate degradation were toxic to the organisms. Aerobic bio-utilization of the chelates as electron-donor substrates directly affected actinide speciation by releasing the radionuclides from complexed form into solution, where their fate was controlled by inorganic ligands in the system. Actinide speciation was also indirectly affected by pH changes caused by organic biodegradation. The two concurrent processes of organic biodegradation and actinide aqueous chemistry were accurately linked and described using CCBATCH, a computer model developed at Northwestern University to investigate the dynamics of coupled biological and chemical reactions in mixed waste subsurface environments. CCBATCH was then used to simulate the fate of Np during anaerobic citrate biodegradation. The modeling studies suggested that, under some conditions, chelate degradation can increase Np(IV) solubility due to carbonate complexation in closed aqueous systems

Mathematical modelling of the effects of aerobic and anaerobic chelate biodegradation on actinide speciation

International Nuclear Information System (INIS)

Banaszak, J.E.; VanBriesen, J.M.; Rittmann, B.E.; Reed, D.T.

1998-01-01

Biodegradation of natural and anthropogenic chelating agents directly and indirectly affects the speciation, and hence, the mobility of actinides in subsurface environments. We combined mathematical modelling with laboratory experimentation to investigate the effects of aerobic and anaerobic chelate biodegradation on actinide [Np(IV/V), Pu(IV)] speciation. Under aerobic conditions, nitrilotriacetic acid (NTA) biodegradation rates were strongly influenced by the actinide concentration. Actinide-chelate complexation reduced the relative abundance of available growth substrate in solution and actinide species present or released during chelate degradation were toxic to the organisms. Aerobic bioutilization of the chelates as electron-donor substrates directly affected actinide speciation by releasing the radionuclides from complexed form into solution, where their fate was controlled by inorganic ligands in the system. Actinide speciation was also indirectly affected by pH changes caused by organic biodegradation. The two concurrent processes of organic biodegradation and actinide aqueous chemistry were accurately linked and described using CCBATCH, a computer model developed at Northwestern University to investigate the dynamics of coupled biological and chemical reactions in mixed waste subsurface environments. CCBATCH was then used to simulate the fate of Np during anaerobic citrate biodegradation. The modelling studies suggested that, under some conditions, chelate degradation can increase Np(IV) solubility due to carbonate complexation in closed aqueous systems. (orig.)

Heterogeneous all actinide recycling in LWR all actinide cycle closure concept

International Nuclear Information System (INIS)

Tondinelli, Luciano

1980-01-01

A project for the elimination of transuranium elements (Waste Actinides, WA) by neutron transmutation is developed in a commercial BWR with U-Pu (Fuel Actinides, FA) recycle. The project is based on the All Actinide Cycle Closure concept: 1) closure of the 'back end' of the fuel cycle, U-Pu coprocessing, 2) waste actinide disposal by neutron transmutation. The reactor core consists of Pu-island fuel assemblies containing WAs in target pins. Two parallel reprocessing lines for FAs and WAs are provided. Mass balance, hazard measure, spontaneous activity during 10 recycles are calculated. Conclusions are: the reduction in All Actinide inventory achieved by Heterogeneous All Actinide Recycling is on the order of 83% after 10 recycles. The U235 enrichment needed for a constant end of cycle reactivity decreases for increasing number of recycles after the 4th recycle. A diffusion-burnup calculation of the pin power peak factors in the fuel assembly shows that design limits can be satisfied. A strong effort should be devoted to the solution of the problems related to high values of spontaneous emission by the target pins

Actinides-1981

International Nuclear Information System (INIS)

1981-09-01

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

Actinides-1981

Energy Technology Data Exchange (ETDEWEB)

1981-09-01

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.

Actinides record, power calculations and activity for present isotopes in the spent fuel of a BWR

International Nuclear Information System (INIS)

Enriquez C, P.; Ramirez S, J. R.; Lucatero, M. A.

2012-10-01

The administration of spent fuel is one of the more important stages of the nuclear fuel cycle, and this has become a problem of supreme importance in countries that possess nuclear reactors. Due to this in this work, the study on the actinides record and present fission products to the discharge of the irradiated fuel in a light water reactor type BWR is shown, to quantify the power and activity that emit to the discharge and during the cooling time. The analysis was realized on a fuel assembly type 10 x 10 with an enrichment average of 3.69 wt % in U-235 and the assembly simulation assumes four cycles of operation of 18 months each one and presents an exposition of 47 G Wd/Tm to the discharge. The module OrigenArp of the Scale 6 code is the computation tool used for the assembly simulation and to obtain the results on the actinides record presents to the fuel discharge. The study covers the following points: a) Obtaining of the plutonium vector used in the fuel production of mixed oxides, and b) Power calculation and activity for present actinides to the discharge. The results presented in this work, correspond at the same time immediate of discharge (0 years) and to a cooling stage in the irradiated fuel pool (5 years). (Author)

Decommissioning of a mixed oxide fuel fabrication facility

International Nuclear Information System (INIS)

Buck, S.; Colquhoun, A.

1990-01-01

Decommissioning of the coprecipitation plant, which made plutonium/uranium oxide fuel, is a lead project in the BNFL Sellafield decommissioning programme. The overall programme has the objectives of gaining data and experience in a wide range of decommissioning operations and hence in this specific project to pilot the decommissioning of plant heavily contaminated with plutonium and other actinides. Consequently the operations have been used to test improvements in temporary containment, contamination control and decontamination methods and also to develop in situ plutonium assay, plutonium recovery and size-reduction methods. Finally the project is also yielding data on manpower requirements, personnel radiation uptake and waste arisings to help in the planning of future decommissioning projects

Research in actinide chemistry. Progress report, March 1, 1980-February 28, 1981

International Nuclear Information System (INIS)

Choppin, G.R.

1981-01-01

Visible spectroscopy, NMR ( 1 H 1 , 6 C 13 , 57 La 139 ) spectroscopy, potentiometry, and calorimetry were used in lanthanide studies which have allowed much more thorough interpretation of actinide tracer studies. In the last several years, the studies were expanded to include actinides in the IV, V and VI oxidation states. Part of the research during this time was directed to investigation of actinide interaction with naturally occurring polyelectrolytes such as humic and fulvic acids. Since redox reactions seemingly occur in some of these interactions, a study of plutonium and neptunium redox behavior in the presence of organic complexing agents was started. Preliminary data are given for reduction of Np(VI) by various organic acids

Plutonium oxides and uranium and plutonium mixed oxides. Carbon determination

International Nuclear Information System (INIS)

Anon.

Determination of carbon in plutonium oxides and uranium plutonium mixed oxides, suitable for a carbon content between 20 to 3000 ppm. The sample is roasted in oxygen at 1200 0 C, the carbon dioxide produced by combustion is neutralized by barium hydroxide generated automatically by coulometry [fr

Cerium compounds in the fashion of the light actinides

International Nuclear Information System (INIS)

Koelling, D.D.

1984-01-01

Researchers familiar with the light actinides easily recognize in cerium compounds a microcosm of the rich variety of properties seen in the light actinides. The parallelism seen between comparable cerium and actinide compounds strongly suggests that the same physical models are applicable. The most significant is the relative size of the f-orbital. Localization is generally tighter in Ce compounds than uranium compounds, making Ce roughly analogous to Np through Am. A way to see the actinide parallelism is to compare Hill plots. Compounds in the different regions of the plots (representing different physics) are isostructural compounds with the same companion (B) elements. The most common materials exhibiting a direct f-f interaction are the cubic Laves compounds. Accordingly, we have determined the band structures of CeRu 2 , CeRh 2 , CeIr 2 , CeOs 2 , and CeNi 2 . Compounds illustrative of the interaction of f-orbitals with ligand orbitals are the Cu 3 Au structured materials. Materials calculated in this class are CeRh 3 , CePd 3 , and CeSn 3 - the materials of much interest as mixed valent. Although the focus is on the Ce compounds, calculations performed on uranium isomorphs are used to highlight the interesting physics

Process analytical chemistry applied to actinide waste streams

International Nuclear Information System (INIS)

Day, R.S.

1994-01-01

The Department of Energy is being called upon to clean up it's legacy of waste from the nuclear complex generated during the cold war period. Los Alamos National Laboratory is actively involved in waste minimization and waste stream polishing activities associated with this clean up. The Advanced Testing Line for Actinide Separations (ATLAS) at Los Alamos serves as a developmental test bed for integrating flow sheet development of nitric acid waste streams with process analytical chemistry and process control techniques. The wastes require processing in glove boxes because of the radioactive components, thus adding to the difficulties of making analytical measurements. Process analytical chemistry methods provide real-time chemical analysis in support of existing waste stream operations and enhances the development of new waste stream polishing initiatives. The instrumentation and methods being developed on ATLAS are designed to supply near-real time analyses on virtually all of the chemical parameters found in nitric acid processing of actinide waste. These measurements supply information on important processing parameters including actinide oxidation states, free acid concentration, interfering anions and metal impurities

Actinide colloid generation in groundwater

International Nuclear Information System (INIS)

Kim, J.I.

1990-05-01

The progress made in the investigation of actinide colloid generation in groundwaters is summarized and discussed with particular examples relevant to an understanding of the migration behaviour of actinides in natural aquifer systems. The first part deals with the characterization of colloids: groundwater colloids, actinide real-colloids and actinide pseudocolloids. The second part concentrates on the generation processes and migration behaviour of actinide pseudocolloids, which are discussed with some notable experimental examples. Importance is stressed more on the chemical aspects of the actinide colloid generation in groundwater. This work is a contribution to the CEC project MIRAGE II, particularly, to research area: complexation and colloids. (orig.)

Fuels and targets for incineration and transmutation of actinides: the ITU programme

International Nuclear Information System (INIS)

Fernandez, A.; Glatz, J.P.; Haas, D.; Konings, R.J.M.; Somers, J.; Toscano, E.; Walker, C.T.; Wegen, D.

2000-01-01

The ITU programme for the development of fuels and targets for transmutation of actinides is presented. The fabrication of various types of oxide fuels/targets by dust-free processes is described. Selected results of post-irradiation examinations of irradiation experiments (SUPERFACT, TRABANT-1, EFTTRA-T4) are presented to demonstrate the irradiation behaviour of these fuels/targets. Finally, the future developments at ITU in this field are described, including the new shielded facility (the MA lab) for fabrication of minor actinide fuels. (authors)

Fuels and targets for incineration and transmutation of actinides: the ITU programme

Energy Technology Data Exchange (ETDEWEB)

Fernandez, A.; Glatz, J.P.; Haas, D.; Konings, R.J.M.; Somers, J.; Toscano, E.; Walker, C.T.; Wegen, D. [Eurpean Commission, Joint Research Centre, Institute for Transuranium Elements, Kurlsruhe (Germany)

2000-07-01

The ITU programme for the development of fuels and targets for transmutation of actinides is presented. The fabrication of various types of oxide fuels/targets by dust-free processes is described. Selected results of post-irradiation examinations of irradiation experiments (SUPERFACT, TRABANT-1, EFTTRA-T4) are presented to demonstrate the irradiation behaviour of these fuels/targets. Finally, the future developments at ITU in this field are described, including the new shielded facility (the MA lab) for fabrication of minor actinide fuels. (authors)

Handbook on the physics and chemistry of the actinides. V. 3

International Nuclear Information System (INIS)

Freeman, A.J.; Keller, C.

1985-01-01

It is the purpose of the Handbook to describe in detail the present understanding of the actinides by means of comprehensive, critical, broad and up to date reviews covering both physics and chemistry of these exotic elements. Volume 3 is the first of two volumes to cover the more chemical, physico-chemical, structural and environmental aspects of the actinide elements. Leading scientists from Europe, USA and P.R. China present critical reviews on important aspects of the behaviour of this radioactive group of elements. In contrast to most other elements radioactivity has, to a degree, a profound influence on the chemical behaviour of the actinides. The unusual behaviour of the 5f-elements - delocalization of the electrons for the light actinides versus localization for the heavier ones - makes them an outstanding tool for the scientist, which can be seen by the variety of oxidation states ranging from +1 to +7. Special laboratory techniques must be developed to deal with the problem of the transcurium elements only being available in small amounts (nanograms to micrograms) or only in the tracer scale. Special emphasis is also placed on the fate of actinides released in the environment, e.g. their reaction to carbonate and organic complexing agents in aquatic systems. In contrast to volumes 1 and 2 which deal mainly with the less radioactive actinides, this volume and the forthcoming volume 4 cover all actinides, in particular those which can be prepared in weighable quantities (up to fermium, element 100). refs.; figs.; tabs

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

International Nuclear Information System (INIS)

Clearfield, Abraham

2017-01-01

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

Actinide speciation bound to hydrous ferric oxide colloids in the near-field conditions of the waste pond at 'Mayak' facility (Russia)

International Nuclear Information System (INIS)

Kalmykov, St.; Khasanova, A.; Kriventsov, V.; Teterin, Y.; Novikov, A.

2007-01-01

Full text of publication follows: 'Mayak' facility is a nuclear waste and spent nuclear fuel reprocessing plant located in Ural Mountains, Russia. The opened pond, Karachay Lake, was used for several decades for the discharge of low- and intermediate level waste solutions containing fission products and traces of actinides. Due to high salt concentration and high density of waste solutions, they are penetrating into the groundwater system that is represented by oxic Eh conditions. The speciation of actinides in groundwater samples collected close to Karachay Lake was studied by successive micro- and ultra-filtrations with subsequent SEM, TEM, nano-SIMS, membrane extraction and other techniques. It was established that U and Np were found in soluble fraction (pass through 10 kD ultra-filter) in the form of their bi- and tri-carbonate complexes that was supported by chemical thermodynamic calculations. In contrast, Pu and Am were bound to nano-colloids 10 kD - 50 nm in size. The SEM and TEM data indicate the presence of variety of different colloidal particles which relative concentration decrease in the row: hydrous ferric oxides (HFO) >> clays ≅ calcite > rutile ≅ hematite ≅ barite ≅ MnO 2 > monazite > other phases. The SIMS with submicron resolution (Cameca nanoSIMS-50) was used to study local concentration of actinides. According to the obtained data among different colloids detected in the sample actinides were preferentially bound to HFO and MnO 2 while other phases did not sorb actinides. In order to determine actinide speciation bound to HFO colloids XPS and An L 3 edge XAFS measurements were done at Siberian Synchrotron Radiation Centre. The storage ring VEPP-3 with electron beam energy of 2 GeV and an average stored current of 80 mA was used as the source of radiation. Since the concentration of actinides in actual samples was too low for XAFS, the samples for measurements were prepared by contacting about 10 -5 M solutions of Np(V) and Pu(V) with

Characterization and uranium bioleaching performance of mixed iron- and sulfur-oxidizers versus iron-oxidizers

International Nuclear Information System (INIS)

Qian Li; Jing Sun; Dexin Ding; Qingliang Wang; Wenge Shi; Eming Hu; Xiaoyu Jiang; University of South China, Hengyang; Xingxing Wang

2017-01-01

In order to develop and apply mixed iron- and sulfur-oxidizers in uranium bioleaching, the characteristics of a mixed iron- and sulfur-oxidizing consortium (Consortium ISO) were comparatively investigated versus an iron-oxidizing consortium (Consortium IO). The results showed, the Consortium ISO exerted stronger oxidative ability and acid-producing ability than Consortium IO did. The synergy of sulfur-oxidizers and iron-oxidizers could change the structure and properties of the passivation substance, and work positively for eliminating the accumulation of passivation substance. In the bioleaching process, the uranium bioleaching experiments showed the recovery percentage of uranium reached 99.5% with Consortium ISO, 6.3% more than that of Consortium IO. (author)

Actinide Oxidation State and O/M Ratio in Hypostoichiometric Uranium-Plutonium-Americium U0.750Pu0.246Am0.004O2-x Mixed Oxides.

Science.gov (United States)

Vauchy, Romain; Belin, Renaud C; Robisson, Anne-Charlotte; Lebreton, Florent; Aufore, Laurence; Scheinost, Andreas C; Martin, Philippe M

2016-03-07

Innovative americium-bearing uranium-plutonium mixed oxides U1-yPuyO2-x are envisioned as nuclear fuel for sodium-cooled fast neutron reactors (SFRs). The oxygen-to-metal (O/M) ratio, directly related to the oxidation state of cations, affects many of the fuel properties. Thus, a thorough knowledge of its variation with the sintering conditions is essential. The aim of this work is to follow the oxidation state of uranium, plutonium, and americium, and so the O/M ratio, in U0.750Pu0.246Am0.004O2-x samples sintered for 4 h at 2023 K in various Ar + 5% H2 + z vpm H2O (z = ∼ 15, ∼ 90, and ∼ 200) gas mixtures. The O/M ratios were determined by gravimetry, XAS, and XRD and evidenced a partial oxidation of the samples at room temperature. Finally, by comparing XANES and EXAFS results to that of a previous study, we demonstrate that the presence of uranium does not influence the interactions between americium and plutonium and that the differences in the O/M ratio between the investigated conditions is controlled by the reduction of plutonium. We also discuss the role of the homogeneity of cation distribution, as determined by EPMA, on the mechanisms involved in the reduction process.

effects of mixed of mixed of mixed alkaline earth oxides in potash

African Journals Online (AJOL)

eobe

Si, P) are network formers, and that materials whose. Nigerian ... made by mixing sand (SiO2), potassium carbonates. (K2Co3) .... The edges of the glass were grounded using ..... surface energies of minerals; theoritical estimate for oxides ...

Review of the sorption of actinides on natural minerals

International Nuclear Information System (INIS)

Beall, G.W.

1981-01-01

Over the past few years, a large body of data concerning sorption of actinides on geologic media has been built in connection with high-level-waste disposal. The primary aim of the work has been to allow predictions of the migration behavior of these radionuclides in the case of a breach of the repository that allowed groundwater flow through the repository. As a result of this work, some new backfill materials specifically tailored for the actinides have also been designed. Several major mechanisms of sorption that appear to dominate the sorption of actinides have emerged from these studies. These mechanisms can be divided into solution reactions dominated by hydrolysis, chemisorption reactions, and oxidation-reduction reactions. Each of these mechanisms will be discussed in detail, with experimental examples. Surprisingly, one mechanism, cation exchange, does not play an important role; why it fails to operate in any significant way in the environmental pH region will be discussed. The implications of the sorption mechanisms for waste forms and backfill materials will be discussed in detail. These discussions will center primarily around the valence state of the actinide in various waste forms and the effect of various anions on leachability from waste forms and backfill materials

Used mixed oxide fuel reprocessing at RT-1 plant

Energy Technology Data Exchange (ETDEWEB)

Kolupaev, D.; Logunov, M.; Mashkin, A.; Bugrov, K.; Korchenkin, K. [FSUE PA ' Mayak' , 30, Lenins str, Ozersk, 460065 (Russian Federation); Shadrin, A.; Dvoeglazov, K. [ITCP ' PRORYV' , 2/8 Malaya Krasmoselskay str, Moscow, 107140 (Russian Federation)

2016-07-01

Reprocessing of the mixed uranium-plutonium spent nuclear fuel of the BN-600 reactor was performed at the RT-1 plant twice, in 2012 and 2014. In total, 8 fuel assemblies with a burn-up from 73 to 89 GW day/t and the cooling time from 17 to 21 years were reprocessed. The reprocessing included the stages of dissolution, clarification, extraction separation of U and Pu with purification from the fission products, refining of uranium and plutonium at the relevant refining cycles. Dissolution of the fuel composition of MOX used nuclear fuel (UNF) in nitric acid solutions in the presence of fluoride ion has occurred with the full transfer of actinides into solution. Due to the high content of Pu extraction separation of U and Pu was carried out on a nuclear-safe equipment designed for the reprocessing of highly enriched U spent nuclear fuel and Pu refining. Technological processes of extraction, separation and refining of actinides proceeded without deviations from the normal mode. The output flow of the extraction outlets in their compositions corresponded to the regulatory norms and remained at the level of the compositions of the streams resulting from the reprocessing of fuel types typical for the RT-1 plant. No increased losses of Pu into waste have been registered during the reprocessing of BN-600 MOX UNF an compare with VVER-440 uranium UNF reprocessing. (authors)

Recovery of actinides from actinide-aluminium alloys by chlorination: Part I

Energy Technology Data Exchange (ETDEWEB)

Cassayre, L., E-mail: cassayre@chimie.ups-tlse.fr [Laboratoire de Genie Chimique (LGC), Departement Procedes Electrochimiques, CNRS-UMR 5503, Universite de Toulouse III - Paul Sabatier, 31062 Toulouse (France); Soucek, P.; Mendes, E.; Malmbeck, R.; Nourry, C.; Eloirdi, R.; Glatz, J.-P. [European Commission, JRC, Institute for Transuranium Elements, Postfach 2340, 76125 Karlsruhe (Germany)

2011-07-01

Pyrochemical processes in molten LiCl-KCl are being developed in ITU for recovery of actinides from spent nuclear fuel. The fuel is anodically dissolved to the molten salt electrolyte and actinides are electrochemically reduced on solid aluminium cathodes forming solid actinide-aluminium alloys. A chlorination route is being investigated for recovery of actinides from the alloys. This route consists in three steps: Vacuum distillation for removal of the salt adhered on the electrode, chlorination of the actinide-aluminium alloys by chlorine gas and sublimation of the formed AlCl{sub 3}. A thermochemical study showed thermodynamic feasibility of all three steps. On the basis of the conditions identified by the calculations, experiments using pure UAl{sub 3} alloy were carried out to evaluate and optimise the chlorination step. The work was focused on determination of the optimal temperature and Cl{sub 2}/UAl{sub 3} molar ratio, providing complete chlorination of the alloy without formation of volatile UCl{sub 5} and UCl{sub 6}. The results showed high efficient chlorination at a temperature of 150 deg. C.

Recovery of actinides from actinide-aluminium alloys by chlorination: Part I

International Nuclear Information System (INIS)

Cassayre, L.; Soucek, P.; Mendes, E.; Malmbeck, R.; Nourry, C.; Eloirdi, R.; Glatz, J.-P.

2011-01-01

Pyrochemical processes in molten LiCl-KCl are being developed in ITU for recovery of actinides from spent nuclear fuel. The fuel is anodically dissolved to the molten salt electrolyte and actinides are electrochemically reduced on solid aluminium cathodes forming solid actinide-aluminium alloys. A chlorination route is being investigated for recovery of actinides from the alloys. This route consists in three steps: Vacuum distillation for removal of the salt adhered on the electrode, chlorination of the actinide-aluminium alloys by chlorine gas and sublimation of the formed AlCl 3 . A thermochemical study showed thermodynamic feasibility of all three steps. On the basis of the conditions identified by the calculations, experiments using pure UAl 3 alloy were carried out to evaluate and optimise the chlorination step. The work was focused on determination of the optimal temperature and Cl 2 /UAl 3 molar ratio, providing complete chlorination of the alloy without formation of volatile UCl 5 and UCl 6 . The results showed high efficient chlorination at a temperature of 150 deg. C.

Utilization of fast reactor excess neutrons for burning minor actinides and long lived FPs

International Nuclear Information System (INIS)

Kawashima, K.; Kobayashi, K.; Kaneto, K.

1995-01-01

An evaluation is made on a large MOX fuel fast reactor's capability of burning minor actinides and long lived fission products (FPs) without imposing penalties on core nuclear and safety characteristics. The excess neutrons generated in the fast reactor core are fully utilized not only to generate the fissile material but also to transmute the minor actinides and long lived FPs. The FP target assemblies which consist of Tc-99 and I-129 are loaded into the selected blanket positions whereas the minor actinides are loaded to the rest of the blanket. A long term FP accumulation scenario is also considered in the mix of FP burner fast reactor and non-burner LWRs. (author)

Sensitivity analysis of minor actinides transmutation to physical and technological parameters

International Nuclear Information System (INIS)

Kooyman, T.; Buiron, L.

2015-01-01

Minor actinides transmutation is one of the 3 main axis defined by the 2006 French law for management of nuclear waste, along with long-term storage and use of a deep geological repository. Transmutation options for critical systems can be divided in two different approaches: (a) homogeneous transmutation, in which minor actinides are mixed with the fuel. This exhibits the drawback of 'polluting' the entire fuel cycle with minor actinides and also has an important impact on core reactivity coefficients such as Doppler Effect or sodium void worth for fast reactors when the minor actinides fraction increases above 3 to 5% depending on the core; (b) heterogeneous transmutation, in which minor actinides are inserted into transmutation targets which can be located in the center or in the periphery of the core. This presents the advantage of decoupling the management of the minor actinides from the conventional fuel and not impacting the core reactivity coefficients. In both cases, the design and analyses of potential transmutation systems have been carried out in the frame of Gen IV fast reactor using a 'perturbation' approach in which nominal power reactor parameters are modified to accommodate the loading of minor actinides. However, when designing such a transmutation strategy, parameters from all steps of the fuel cycle must be taken into account, such as spent fuel heat load, gamma or neutron sources or fabrication feasibility. Considering a multi-recycling strategy of minor actinides, an analysis of relevant estimators necessary to fully analyze a transmutation strategy has been performed in this work and a sensitivity analysis of these estimators to a broad choice of reactors and fuel cycle parameters has been carried out. No threshold or percolation effects were observed. Saturation of transmutation rate with regards to several parameters has been observed, namely the minor actinides volume fraction and the irradiation time. Estimators of interest that have been

Cerium compounds in the fashion of the light actinides

International Nuclear Information System (INIS)

Koelling, D.D.

1985-01-01

Researchers familiar with the light actinides easily recognize in cerium compounds a microcosm of the rich variety of properties seen in the light actinides. The parallelism seen between comparable cerium and actinide compounds strongly suggests that the same physical models are applicable. The most significant is the relative size of the f-orbital. Localization is generally tighter in Ce compounds than uranium compounds, making Ce roughly analogous to Np through Am. A way to see the actinide parallelism is to compare Hill plots. Compounds in the different regions of the plots (representing different physics) are isostructural compounds with the same companion (B) elements. The most common materials expected to exhibit direct f-f interaction are the cubic Laves compounds. Accordingly, we have determined the band structures of CeRu 2 , CeRh 2 , CeIr 2 , and CeNi 2 . Surprisingly, it was found that an f-d interaction overshadows any direct f-f interaction in these systems. Compounds illustrative of the interaction of f-orbitals with ''ligand'' orbitals are the Cu 3 Au structured materials. Materials calculated in this class are CeRh 3 , CePd 3 , and CeSn 3 - the materials of much interest as ''mixed valent''. Although the focus is on the Ce compounds, calculations performed on uranium isomorphs are used to highlight the interesting physics. (orig.)

Plutonium and minor actinide transmutation by long irradiation in LWR

International Nuclear Information System (INIS)

Facchini, A.; Sanjust, V.

1993-01-01

An investigation was made on the conceptual possibility of burning in a thermal reactor MOX fuel together with special pins containing plutonium, minor actinides and long lived fission products, recovered from the reprocessing of previously irradiated MOX fuel and mixed with an inter matrix. Preliminary calculations showed that the long term radiotoxicity of the above special pins is reduced to reasonable levels when they are irradiated up to 20 divided-by 30 years, and cooled for some centuries. In particular, during the whole life such a reactor should be able to burn a considerable fraction of plutonium, minor actinides and long lived fission products recovered from the MOX fuel irradiated along the same period of time

Electrochemical reduction of cerium oxides in molten salts

International Nuclear Information System (INIS)

Claux, B.; Serp, J.; Fouletier, J.

2011-01-01

This brief article describes a pyrochemical process that is used by CEA to turn actinide oxides into metal actinides. This process is applied to Cerium oxides (CeO 2 ) that simulate actinide oxides well chemically as cerium belongs to the lanthanide family. The process is in fact an electrolysis of cerium oxide in a bath of molten calcium chloride salt whose temperature is between 800 and 900 Celsius degrees. At those temperatures calcium chloride becomes a ionic liquid (Ca 2+ and Cl - ) that is a good electrical conductor and is particularly well-adapted as solvent to an electrolytic process. The electrolysis current allows the transformation of solvent Ca 2+ ions into metal calcium which, in turn, can reduce cerium oxide into metal cerium through chromatically. Experimental data shows the reduction of up to 90% of 10 g samples of CeO 2 in a 6 hour long electrolysis while the best reduction rate ever known was 80% so far. This result is all the more promising that cerium oxides are more difficult to reduce than actinide oxides from the thermodynamical perspective

Recovery actinide values

International Nuclear Information System (INIS)

Horwitz, E.P.; Delphin, W.H.; Mason, G.W.

1979-01-01

A process is described 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 di-hexoxyethyl 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. (author)

3 and 4 oxidation state element solubilities in borosilicate glasses. Implement to actinides in nuclear glasses; Solubilite des elements aux degres d'oxydation (3) et (4) dans les verres de borosilicate. Application aux actinides dans les verres nucleaires

Energy Technology Data Exchange (ETDEWEB)

Cachia, J.N

2005-12-15

In order to ensure optimal radionuclides containment, the knowledge of the actinide loading limits in nuclear waste glasses and also the comprehension of the solubilization mechanisms of these elements are essential. A first part of this manuscript deals with the study of the differences in solubility of the tri and tetravalent elements (actinides and surrogates) particularly in function of the melting temperature. The results obtained indicate that trivalent elements (La, Gd, Nd, Am, Cm) exhibit a higher solubility than tetravalent elements (Hf, Th, Pu). Consequently, it was planned to reduce plutonium at the oxidation state (III), the later being essentially tetravalent in borosilicate glasses. An innovating reduction process of multi-valent elements (cerium, plutonium) using silicon nitride has been developed in a second part of this work. Reduced plutonium-bearing glasses synthesized by Si{sub 3}N{sub 4} addition made it possible to double the plutonium solubility from 2 to 4 wt% at 1200 deg C. A structural approach to investigate the differences between tri and tetravalent elements was finally undertaken. These investigations were carried out by X-rays Absorption Spectroscopy (EXAFS) and NMR. Trivalent rare earth and actinide elements seem to behave as network modifiers while tetravalent elements rather present true intermediaries' behaviour. (author)

Actinides: from heavy fermions to plutonium metallurgy

International Nuclear Information System (INIS)

Smith, J.L.; Fisk, Z.; Hecker, S.S.

1984-01-01

The actinide elements mark the emergence of 5f electrons. The f electrons possess sufficiently unusual characteristics that their participation in atomic binding often result in dramatic changes in properties. This provides an excellent opportunity to study the question of localization of electrons; a question that is paramount in predicting the physical and chemical properties of d and f electron transition metals. The transition region between localized (magnetic) and itinerant (often superconducting) behavior provides for many interesting phenomena such as structural instabilities (polymorphism), spin fluctuations, mixed valences, charge density waves, exceptional catalytic activity and hydrogen storage. This region offers most interesting behavior such as that exhibited by the actinide compounds UBe 13 and UPt 3 . Both compounds are heavy-fermion superconductors in which both magnetic and superconducting behavior exist in the same electrons. The consequences of f-electron bonding (which appears greatest at Plutonium) show dramatic effects on phase stability, alloying behavior, phase transformations and mechanical behavior

Rate Constants for Reactions of Radiation-Produced Transients in Aqueous Solutions of Actinides

International Nuclear Information System (INIS)

Gordon, S.; Sullivan, J.C.; Ross, A.B.

1986-01-01

Rate constants have been critically compiled for reactions of ions of the actinides Am, Cf, Cm, Np, Pu, Th, and U, as well as the element Tc, in different oxidation states with various chemical species in aqueous solution. The reactants include products of the radiolysis of water (hydrated electrons, hydrogen atoms, hydroxyl radicals, hydrogen peroxide) and transient species derived from other solutes (e.g., carbonate radical). The data are useful in the estimation of migration properties of actinides, which are relevant to waste management studies

Mechanisms for the reduction of actinide ions by Geobacter sulfurreducens

International Nuclear Information System (INIS)

Renshaw, J.C.; Livens, F.R.; May, I.; Lloyd, J.R.

2005-01-01

Full text of publication follows: Three of the most problematic radioactive contaminants are the actinide elements uranium, neptunium and plutonium. All three pose considerable long-term environmental risks. The most stable environmental oxidation states of uranium and neptunium are VI and V, respectively, as the di-oxo cations [UO 2 ] 2+ and [NpO 2 ] + ; both are highly soluble and so are relatively mobile and biologically available in the environment. In similar conditions, plutonium mainly exists as Pu(IV), which forms a highly insoluble hydrous oxide, although is also environmentally stable in the more soluble III, V and VI oxidation states. The bio-reduction of U(VI) by anaerobic subsurface microorganisms has been the focus of much recent interest. Both Fe(III)- and sulfate-reducing bacteria have been shown to reduce soluble [U VI O 2 ] 2+ to insoluble U IV O 2 , with c-type cytochromes involved in electron transfer to the actinide. Such transformations offer a strategy for the bio-remediation of uranium contaminated groundwater and a potential mechanism for the bio-deposition of uranium ores. The mechanism of U(VI). reduction has important implications for the potential microbial reduction of transuranic elements with environmentally stable lower oxidation states. Reduction of mobile 237 Np(V) to Np(IV) and subsequent precipitation may be advantageous whilst remobilization of immobile Pu(IV) as more soluble Pu(III) species could have important environmental implications. Conversely, selective reduction might allow targeting of particular radionuclide species. The model anaerobic bacterium Geobacter sulfurreducens is typical of those found in contaminated subsurface environments and has been shown to reduce soluble [U VI O 2 ] 2+ to insoluble U IV O 2 . In the course of this study we use X-ray absorption spectroscopy (XAS) to show that G. sulfurreducens reduces U(VI) by a one-electron reduction, forming an unstable [UO 2 ] + species which subsequently

Actinide recycle

Energy Technology Data Exchange (ETDEWEB)

Till, C; Chang, Y [Argonne National Laboratory, Argonne, IL (United States)

1990-07-01

A multitude of studies and assessments of actinide partitioning and transmutation were carried out in the late 1970s and early 1980s. Probably the most comprehensive of these was a study coordinated by Oak Ridge National Laboratory. The conclusions of this study were that only rather weak economic and safety incentives existed for partitioning and transmuting the actinides for waste management purposes, due to the facts that (1) partitioning processes were complicated and expensive, and (2) the geologic repository was assumed to contain actinides for hundreds of thousands of years. Much has changed in the few years since then. A variety of developments now combine to warrant a renewed assessment of the actinide recycle. First of all, it has become increasingly difficult to provide to all parties the necessary assurance that the repository will contain essentially all radioactive materials until they have decayed. Assurance can almost certainly be provided to regulatory agencies by sound technical arguments, but it is difficult to convince the general public that the behavior of wastes stored in the ground can be modeled and predicted for even a few thousand years. From this point of view alone there would seem to be a clear benefit in reducing the long-term toxicity of the high-level wastes placed in the repository.

Actinide recycle

International Nuclear Information System (INIS)

Till, C.; Chang, Y.

1990-01-01

A multitude of studies and assessments of actinide partitioning and transmutation were carried out in the late 1970s and early 1980s. Probably the most comprehensive of these was a study coordinated by Oak Ridge National Laboratory. The conclusions of this study were that only rather weak economic and safety incentives existed for partitioning and transmuting the actinides for waste management purposes, due to the facts that (1) partitioning processes were complicated and expensive, and (2) the geologic repository was assumed to contain actinides for hundreds of thousands of years. Much has changed in the few years since then. A variety of developments now combine to warrant a renewed assessment of the actinide recycle. First of all, it has become increasingly difficult to provide to all parties the necessary assurance that the repository will contain essentially all radioactive materials until they have decayed. Assurance can almost certainly be provided to regulatory agencies by sound technical arguments, but it is difficult to convince the general public that the behavior of wastes stored in the ground can be modeled and predicted for even a few thousand years. From this point of view alone there would seem to be a clear benefit in reducing the long-term toxicity of the high-level wastes placed in the repository

Macrophages as key elements of Mixed-oxide [U-Pu(O2)] distribution and pulmonary damage after inhalation?

Science.gov (United States)

Van der Meeren, Anne; Moureau, Agnes; Griffiths, Nina M

2014-11-01

Abstract Purpose: To investigate the consequences of alveolar macrophage (AM) depletion on Mixed OXide fuel (MOX: U, Pu oxide) distribution and clearance, as well as lung damage following MOX inhalation. Rats were exposed to MOX by nose only inhalation. AM were depleted with intratracheal administration of liposomal clodronate at 6 weeks. Lung changes, macrophage activation, as well as local and systemic actinide distribution were studied up to 3 months post-inhalation. Clodronate administration modified excretion/retention patterns of α activity. At 3 months post-inhalation lung retention was higher in clodronate-treated rats compared to Phosphate Buffered Saline (PBS)-treated rats, and AM-associated α activity was also increased. Retention in liver was higher in clodronate-treated rats and fecal and urinary excretions were lower. Three months after inhalation, rats exhibited lung fibrotic lesions and alveolitis, with no marked differences between the two groups. Foamy macrophages of M2 subtype [inducible Nitric Oxide Synthase (iNOS) negative but galectin-3 positive] were frequently observed, in correlation with the accumulation of MOX particles. AM from all MOX-exposed rats showed increased chemokine levels as compared to sham controls. Despite the transient reduced AM numbers in clodronate-treated animals no major differences on lung damage were observed as compared to non-treated rats after MOX inhalation. The higher lung activity retention in rats receiving clodronate seems to be part of a general inflammatory response and needs further investigation.

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

Energy Technology Data Exchange (ETDEWEB)

Clearfield, Abraham [Texas A & M Univ., College Station, TX (United States)

2017-10-24

As indicated in the previous annual report the goals of this project are to develop procedures for efficient separation of lanthanides from actinides and curium from americium. These processes are required for the nuclear fuel cycle to minimize the waste and recover the valuable actinides. The basis for our study is that we have prepared a group of compounds that are porous and favor the uptake of ions with charges 3+ and 4+ over ions of lesser charge. The general formula for these materials is M(O₃PC₆H₄PO₃)_1-x/2(APO₄)x·nH₂O: where M=Zr⁴⁺, Sn⁴⁺, A=H, Na, or K and X=O, 0.5, 0.8, 1.0, 1.33 and 1.61-3. One of our tasks is to determine which members of this group of compounds are effective in carrying out the required separations. A difficulty in obtaining this required information is that the compounds are amorphous. That is they are not crystalline, therefore we need to resort to synchrotron data to obtain structural data which will be presented in detail. This information will be provided as a separate section.

Study on neutron spectrum for effective transmutation of minor actinides in thermal reactors

International Nuclear Information System (INIS)

Takeda, Toshikazu; Yokoyama, Kenji

1997-01-01

The transmutation of minor actinides (MAs) has been investigated in thermal reactor cells using mixed oxide fuel with MAs. The effect of neutron spectra on transmutation is studied by changing the neutron spectra. Five transmutation rates are compared: direct fission incineration rate, capture transmutation rate, consumption rate, overall fission incineration rate and inventory difference transmutation rate. The relations between these transmutation rates and their dependence on the neutron spectrum were investigated. To effectively incinerate MAs it is necessary to maximize the overall fission incineration rate and the inventory difference transmutation rate. These transmutation rates become maximum when the fraction of neutrons below 1 eV is about 8% for the case where the MA addition is 1-3%. When the MA addition is over 5%, the transmutation rates become maximum for very hard neutron spectrum. (Author)

Frequency analysis of pulmonary tumors occurrence at the rat after exposure to actinide oxide aerosols. Risk factors identification by comparing NpO2 and PuO2

International Nuclear Information System (INIS)

Dudoignon, N.

2001-07-01

Inhalation of actinide oxide particles is potentially one route of contamination of workers, which might induce pulmonary tumours due to aerosol generation during nuclear fuel fabrication process. Dose-effect relationships for lung tumour induction have been well established from epidemiological and experimental studies. However, they do not take into account specific parameters of exposure. The aim of this study was to compare cancer incidence among groups of rats exposed either to NpO 2 or to PuO 2 , two actinide oxides with different specific activity, but with similar aerosol granulometry. During the rat life-span, lung tumour development could occur and the individual follow-up allowed the determination of lung dose at death. Although aerosol particle sizes were similar, the mean number of particles per unit of activity was 2400 times higher for NpO 2 as compared to PuO 2 . This range of variation appeared higher than the variation of specific activity (450). Initial distribution of aerosol was then much more homogeneous for neptunium. In the range of initial lung deposits studied, the only physiological changes observed concerned lung clearance and rat life- span after exposure to the highest levels of Np activity. Pathological examination performed at death showed that carcinogenic power of neptunium was 2 to 3 times higher than that of plutonium. Dose-effect relationships appeared linear and when compared to previous studies, showed an increase of lung cancer risk as the specific activity of the inhaled actinide oxide decreases. The range of risk variation can reach a factor of 10, revealing that the consideration of lung dose at death solely might not be sufficient for an accurate estimate of risk and that specific parameters of exposure, such as nature and granulometry of aerosols, should also be taken into account. (author)

Recent development in computational actinide chemistry

International Nuclear Information System (INIS)

Li Jun

2008-01-01

Ever since the Manhattan project in World War II, actinide chemistry has been essential for nuclear science and technology. Yet scientists still seek the ability to interpret and predict chemical and physical properties of actinide compounds and materials using first-principle theory and computational modeling. Actinide compounds are challenging to computational chemistry because of their complicated electron correlation effects and relativistic effects, including spin-orbit coupling effects. There have been significant developments in theoretical studies on actinide compounds in the past several years. The theoretical capabilities coupled with new experimental characterization techniques now offer a powerful combination for unraveling the complexities of actinide chemistry. In this talk, we will provide an overview of our own research in this field, with particular emphasis on applications of relativistic density functional and ab initio quantum chemical methods to the geometries, electronic structures, spectroscopy and excited-state properties of small actinide molecules such as CUO and UO 2 and some large actinide compounds relevant to separation and environment science. The performance of various density functional approaches and wavefunction theory-based electron correlation methods will be compared. The results of computational modeling on the vibrational, electronic, and NMR spectra of actinide compounds will be briefly discussed as well [1-4]. We will show that progress in relativistic quantum chemistry, computer hardware and computational chemistry software has enabled computational actinide chemistry to emerge as a powerful and predictive tool for research in actinide chemistry. (authors)

Extraction of actinides from chloride medium using pentaalkylpropanediamides

International Nuclear Information System (INIS)

Cuillerdier, C.; Musikas, C.

1991-01-01

Pyrometallurgical processes for the purification of plutonium create waste solutions containing actinides, mainly americium, in chloride medium. Studies have been undertaken to study the extraction of actinides in chloride medium (hydrochloric acid mixed with concentrated salts such as LiCl, CaCl 2 , MgCl 2 , KCl) using pentaalkylpropanediamides as extractants. Plutonium (IV) is very easily extracted, Am (III) needs a salting out agent such as LiCl. Back extraction of trivalent cations is easy in HCl <5M. Plutonium(IV) and (VI) can be stripped by reduction either with ascorbic acid or hydroxylammonium salts in weak acid medium. Several diluents can be used (aromatic, chlorinated or even aliphatic) with addition of decanol to prevent third phase formation. In conclusion diamides can be used for various wastes declassification, they are potentially completely incinerable, and, as the synthesis has been optimized, they appear to be promising extractants

Enhanced photocatalytic activity of titania-silica mixed oxide prepared via basic hydrolyzation

International Nuclear Information System (INIS)

Xie Chao; Xu Zili; Yang Qiujing; Xue Baoyong; Du Yaoguo; Zhang Jiahua

2004-01-01

Two different synthesis routes were applied to prepare TiO 2 -XSiO 2 (X denotes mol% of silica in titania-silica mixed oxides) with different silica concentrations by using ammonia water as hydrolysis catalyst. Through comparing the photocatalytic performance of two sets of mixed oxides, we found that the photocatalytic activity of mixed oxides prepared via the route which can promote homogeneity, was significantly enhanced as compared with that of counterparts prepared via the another route, and the highest photocatalytic activity obtained by adding about 9.1 mol% silica into titania was much higher than that of pure TiO 2 . The mixed oxides were investigated by means of XRD, thermal analysis, UV-vis, FT-IR and XPS. The characterization results suggest that, in comparison with pure TiO 2 , the mixed oxides exhibit smaller crystallite size and higher thermal stability which can elevate the temperature of anatase to rutile phase transformation due to the addition of silica. Furthermore, Broensted acidity, which is associated with the formation of Ti-O-Si hetero linkages where tetrahedrally coordinated silica is chemically mixed with the octahedral titania matrix, may be a very important contribution to the enhanced photocatalytic activity of titania-silica mixed oxides as well

Actinide isotopic analysis systems

International Nuclear Information System (INIS)

Koenig, Z.M.; Ruhter, W.D.; Gunnink, R.

1990-01-01

This manual provides instructions and procedures for using the Lawrence Livermore National Laboratory's two-detector actinide isotope analysis system to measure plutonium samples with other possible actinides (including uranium, americium, and neptunium) by gamma-ray spectrometry. The computer program that controls the system and analyzes the gamma-ray spectral data is driven by a menu of one-, two-, or three-letter options chosen by the operator. Provided in this manual are descriptions of these options and their functions, plus detailed instructions (operator dialog) for choosing among the options. Also provided are general instructions for calibrating the actinide isotropic analysis system and for monitoring its performance. The inventory measurement of a sample's total plutonium and other actinides content is determined by two nondestructive measurements. One is a calorimetry measurement of the sample's heat or power output, and the other is a gamma-ray spectrometry measurement of its relative isotopic abundances. The isotopic measurements needed to interpret the observed calorimetric power measurement are the relative abundances of various plutonium and uranium isotopes and americium-241. The actinide analysis system carries out these measurements. 8 figs

Studies on O/M ratio determination in uranium oxide, plutonium oxide and uranium-plutonium mixed oxide

International Nuclear Information System (INIS)

Sampath, S.; Chawla, K.L.

1975-01-01

Thermogravimetric studies were carried out in unsintered and sintered samples of uranium oxide, plutonium oxide and uranium-plutonium mixed oxide under different atmospheric conditions (air, argon and moist argon/hydrogen). Moisture loss was found to occur below 200 0 C for uranium dioxide samples, upto 700 0 C for sintered plutonium dioxide and negligible for sintered samples. The O/M ratios for non-stoichiometric uranium dioxide (sintered and unsintered), plutonium dioxide and mixed uranium and plutonium oxides (sintered) could be obtained with a precision of +- 0.002. Two reference states UOsub(2.000) and UOsub(2.656) were obtained for uranium dioxide and the reference state MOsub(2.000) was used for other cases. For unsintered plutonium dioxide samples, accurate O/M ratios could not be obtained of overlap of moisture loss with oxygen loss/gain. (author)

The inverse-trans-influence in tetravalent lanthanide and actinide bis(carbene) complexes

Science.gov (United States)

Gregson, Matthew; Lu, Erli; Mills, David P.; Tuna, Floriana; McInnes, Eric J. L.; Hennig, Christoph; Scheinost, Andreas C.; McMaster, Jonathan; Lewis, William; Blake, Alexander J.; Kerridge, Andrew; Liddle, Stephen T.

2017-02-01

Across the periodic table the trans-influence operates, whereby tightly bonded ligands selectively lengthen mutually trans metal-ligand bonds. Conversely, in high oxidation state actinide complexes the inverse-trans-influence operates, where normally cis strongly donating ligands instead reside trans and actually reinforce each other. However, because the inverse-trans-influence is restricted to high-valent actinyls and a few uranium(V/VI) complexes, it has had limited scope in an area with few unifying rules. Here we report tetravalent cerium, uranium and thorium bis(carbene) complexes with trans C=M=C cores where experimental and theoretical data suggest the presence of an inverse-trans-influence. Studies of hypothetical praseodymium(IV) and terbium(IV) analogues suggest the inverse-trans-influence may extend to these ions but it also diminishes significantly as the 4f orbitals are populated. This work suggests that the inverse-trans-influence may occur beyond high oxidation state 5f metals and hence could encompass mid-range oxidation state actinides and lanthanides. Thus, the inverse-trans-influence might be a more general f-block principle.

Phoenix type concepts for transmutation of LWR waste minor actinides

International Nuclear Information System (INIS)

Segev, M.

1994-01-01

A number of variations on the original Phoenix theme were studied. The basic rationale of the Phoenix incinerator is making oxide fuel of the LWR waste minor actinides, loading it in an FFTF-like subcritical core, then bombarding the core with the high current beam accelerated protons to generate considerable energy through spallation and fission reactions. As originally assessed, if the machine is fed with 1600 MeV protons in a 102 mA current, then 8 core modules are driven to transmute the yearly minor actinides waste of 75 1000 MW LWRs into Pu 238 and fission products; in a 2 years cycle the energy extracted is 100000 MW d/T. This performance cannot be substantiated in a rigorous analysis. A calculational consistent methodology, based on a combined execution of the Hermes, NCNP, and Korigen codes, shows, nonetheless that changes in the original Phoenix parameters can upgrade its performance.The original Phoenix contains 26 tons minor actinides in 8 core modules; 1.15 m 3 module is shaped for 40% neutron leakage; with a beam of 102 mA the 8 modules are driven to 100000 MW/T in 10.5 years, burning out the yearly minor actinide waste of 15 LWRs; the operation must be assisted by grid electricity. If the 1.15 m 3 module is shaped to allow only 28% leakage, then a beam of 102 mA will drive the 8 modules to 100000 MW/T in 3.5 years, burning out the yearly minor actinides waste of 45 LWRs. Some net grid electricity will be generated. If 25 tons minor actinides are loaded into 5 modules, each 1.72 m 3 in volume and of 24% leakage, then a 97 mA beam will drive the module to 100000 MW/T in 2.5 years, burning out the yearly minor actinides waste of 70 LWRs. A considerable amount of net grid electricity will be generated. If the lattice is made of metal fuel, and 26 tons minor actinides are loaded into 32 small modules, 0.17 m 3 each, then a 102 mA beam will drive the modules to 100000 MW/T in 2 years, burning out the yearly minor actinides waste of 72 LWRs. A considerable

Actinide recovery techniques utilizing electromechanical processes

International Nuclear Information System (INIS)

Westphal, B.R.; Benedict, R.W.

1994-01-01

Under certain conditions, the separation of actinides using electromechanical techniques may be an effective means of residue processing. The separation of granular mixtures of actinides and other materials is based on appreciable differences in the magnetic and electrical properties of the actinide elements. In addition, the high density of actinides, particularly uranium and plutonium, may render a simultaneous separation based on mutually complementary parameters. Both high intensity magnetic separation and electrostatic separation have been investigated for the concentration of an actinide waste stream. Waste stream constituents include an actinide metal alloy and broken quartz shards. The investigation of these techniques is in support of the Integral Fast Reactor (IFR) concept currently being developed at Argonne National Laboratory under the auspices of the Department of Energy

Reirradiation of mixed-oxide fuel pins at increased temperatures

International Nuclear Information System (INIS)

Lawrence, L.A.; Weber, E.T.

1976-05-01

Mixed-oxide fuel pins from EBR-II irradiations were reirradiated in the General Electric Test Reactor (GETR) at higher temperatures than experienced in EBR-II to study effects of the increased operating temperatures on thermal/mechanical and chemical behavior. The response of a mixed-oxide fuel pin to a power increase after having operated at a lower power for a significant portion of its life-time is an area of performance evaluation where little information currently exists. Results show that the cladding diameter changes resulting from the reirradiation are strongly dependent upon both prior burnup level and the magnitude of the temperature increase. Results provide the initial rough outlines of boundaries within which mixed-oxide fuel pins can or cannot tolerate power increases after substantial prior burnup at lower powers

Alternative oxidation technologies for organic mixed waste

International Nuclear Information System (INIS)

Borduin, L.C.; Fewell, T.

1998-01-01

The Mixed Waste Focus Area (MWFA) is currently supporting the development and demonstration of several alternative oxidation technology (AOT) processes for treatment of combustible mixed low-level wastes. AOTs have been defined as technologies that destroy organic material without using open-flame reactions. AOTs include both thermal and nonthermal processes that oxidize organic wastes but operate under significantly different physical and chemical conditions than incinerators. Nonthermal processes currently being studied include Delphi DETOX and acid digestion at the Savannah River Site (SRS), and direct chemical oxidation at Lawrence Livermore National Laboratory (LLNL). All three technologies are at advanced stages of development or are entering the demonstration phase. Nonflame thermal processes include catalytic chemical oxidation, which is being developed and deployed at Lawrence Berkeley National Laboratory (LBNL), and steam reforming, a commercial process being supported by the Department of Energy (DOE). Although testing is complete on some AOT technologies, most require additional support to complete some or all of the identified development objectives. Brief descriptions, status, and planned paths forward for each of the technologies are presented

Criteria for achieving actinide reduction goals

International Nuclear Information System (INIS)

Liljenzin, J.O.

1996-01-01

In order to discuss various criteria for achieving actinide reduction goals, the goals for actinide reduction must be defined themselves. In this context the term actinides is interpreted to mean plutonium and the so called ''minor actinides'' neptunium, americium and curium, but also protactinium. Some possible goals and the reasons behind these will be presented. On the basis of the suggested goals it is possible to analyze various types of devices for production of nuclear energy from uranium or thorium, such as thermal or fast reactors and accelerator driven system, with their associated fuel cycles with regard to their ability to reach the actinide reduction goals. The relation between necessary single cycle burn-up values, fuel cycle processing losses and losses to waste will be defined and discussed. Finally, an attempt is made to arrange the possible systems on order of performance with regard to their potential to reduce the actinide inventory and the actinide losses to wastes. (author). 3 refs, 3 figs, 2 tabs

Actinides: why are they important biologically

International Nuclear Information System (INIS)

Durbin, P.W.

1978-01-01

The following topics are discussed: actinide elements in energy systems; biological hazards of the actinides; radiation protection standards; and purposes of actinide biological research with regard to toxicity, metabolism, and therapeutic regimens

New strategy for minor actinides partitioning preliminary results on the electrovolatilization of ruthenium and on the stabilization of Am(IV) in nitric acid with phosphotunsgstate ligand

International Nuclear Information System (INIS)

Adnet, J.M.; Madic, C.

1989-01-01

On problems related to the long term storage in deep geological repositories of high active wastes (H.A.W.) is due to the presence of minor actinide isotopes. Thus after the decay of the fission products (≅ 300 years) the toxicity of these H.A.W. is mainly due to the minor actinides. One solution is based on actinide partitioning followed by transmutation into fission products with short half-lives. A simpler processes than those developed previously, can be based on the possible oxidation of minor actinides to the + IV or + VI oxidation states and their selective extraction. The first step to study is the elimination of the ruthenium (whose presence would be detrimental to oxidize minor actinides) which can be done by electrovolatilization of Ru on the RuO 4 form. The rate of electrovolatilization can be increased by the use of the following electronic mediators, AgI/AgII(1); CeIII/Ce(2), and CoII/CoIII(3), the efficiency of which decreases in the order: 1 > 2 > 3. The effectiveness of that process has been proven when treating real H.A.W solution produced during the study of the reprocessing of a MOX fuel irradiated to as burn-up of 52 GWd/t in a LWR: complete Ru removal was obtained. The second part of the study concerns the electrochemical oxidation of AmIII in nitric acid solutions in the presence of a strong complexing agent: P 2 W 17 O 61 K 10 (P.W.).Total americium oxidation to AmIV can be obtained in nitric acid solution with a concentration up to 8 M. No particular drawback was induced by the presence of an amount of lanthanide III (NdIII) in 6 fold excess vs P.W. The stability of AmIV was studied. The other actinides will be present in these solutions, after the electrochemical oxidation step, in the + VI or+ IV oxidation states, thus a selective extraction (vs fission products) could be performed. A possible way to extract actinide IV/P.W complexes is to use dodecylamine nitrate as extractant

Investigation of the complexation and the migration of actinides and non-radioactive substances with humic acids under geogenic conditions. Complexation of humic acids with actinides in the oxidation state IV Th, U, Np

International Nuclear Information System (INIS)

Sachs, S.; Schmeide, K.; Brendler, V.; Krepelova, A.; Mibus, J.; Geipel, G.; Heise, K.H.; Bernhard, G.

2004-03-01

Objective of this project was the study of basic interaction and migration processes of actinides in the environment in presence of humic acids (HA). To obtain more basic knowledge on these interaction processes synthetic HA with specific functional properties as well as 14 C-labeled HA were synthesized and applied in comparison to the natural HA Aldrich. One focus of the work was on the synthesis of HA with distinct redox functionalities. The obtained synthetic products that are characterized by significantly higher Fe(III) redox capacities than Aldrich HA were applied to study the redox properties of HA and the redox stability of U(VI) humate complexes. It was confirmed that phenolic OH groups play an important role for the redox properties of HA. However, the results indicate that there are also other processes than the single oxidation of phenolic OH groups and/or other functional groups contributing to the redox behavior of HA. A first direct-spectroscopic proof for the reduction of U(VI) by synthetic HA with distinct redox functionality was obtained. The complexation behavior of synthetic and natural HA with actinides (Th, Np, Pu) was studied. Structural parameters of Pu(III), Th(IV), Np(IV) and Np(V) humates were determined by X-ray absorption spectroscopy (XAS). The results show that carboxylate groups dominate the interaction between HA and actinide ions. These are predominant monodentately bound. The influence of phenolic OH groups on the Np(V) complexation by HA was studied with modified HA (blocked phenolic OH groups). The blocking of phenolic OH groups induces a decrease of the number of maximal available complexing sites of HA, whereas complex stability constant and Np(V) near-neighbor surrounding are not affected. The effects of HA on the sorption and migration behavior of actinides was studied in batch and column experiments. Th(IV) sorption onto quartz and Np(V) sorption onto granite and its mineral constituents are affected by the pH value and the

Subcritical limits for special fissile actinides

International Nuclear Information System (INIS)

Clark, H.K.

1980-01-01

Critical masses and subcritical mass limits in oxide-water mixtures were calculated for actinide nuclides other than 233 U, 235 U, and 239 Pu that have an odd number of neutrons in the nucleus: S/sub n/ transport theory was used together with cross sections, drawn from the GLASS multigroup library, developed to provide accurate forecasts of actinide production at Savannah River. The subcritical limits are 201 g for 241 Pu, 13 g for 242 /sup m/Am, 90 g for 243 Cm, 30 g for 245 Cm, 900 g for 247 Cm, 10 g for 249 Cf, and 5 g for 251 Cf. Association of 241 Pu with an equal mass of 240 Pu increases the 241 Pu limit to a value greater than that for pure 239 Pu. Association of 242 /sup m/Am with 241 Am increases the limit for the mixture to that for dry, theoretical density AmO 2 at isotopic concentrations of 242 /sup m/Am less than approx. 6%. Association of 245 Cm with 244 Cm increases the limit according to the formula 30 + 0.3 244 Cm/ 245 Cm up to the limit for dry CmO 2 . A limiting mass of 8.15 kg for plutonium containing at least 67% 238 Pu as oxide was calculated that applies (provided 240 Pu exceeds 241 Pu) with no limit on moderation. 1 figure, 5 tables

Actinide recovery techniques utilizing electromechanical processes

International Nuclear Information System (INIS)

Westphal, B.R.; Benedict, R.W.

1994-01-01

Under certain conditions, the separation of actinides using electromechanical techniques may be an effective means of residue processing. The separation of granular mixtures of actinides and other materials discussed in this report is based on appreciable differences in the magnetic and electrical properties of the actinide elements. In addition, the high density of actinides, particularly uranium and plutonium, may render a simultaneous separation based on mutually complementary parameters. Both high intensity magnetic separation and electrostatic separation have been investigated for the concentration of an actinide waste stream. Waste stream constituents include an actinide metal alloy and broken quartz shards. The investigation of these techniques is in support of the Integral Fast Reactor (IFR) concept currently being developed at Argonne National Laboratory under the auspices of the Department of Energy

Actinide Separation Demonstration Facility, Tarapur

International Nuclear Information System (INIS)

Vishwaraj, I.

2017-01-01

Partitioning of minor actinide from high level waste could have a substantial impact in lowering the radio toxicity associated with high level waste as well as it will reduce the burden on geological repository. In Indian context, the partitioned minor actinide could be routed into the fast breeder reactor systems scheduled for commissioning in the near period. The technological breakthrough in solvent development has catalyzed the partitioning programme in India, leading to the setting up and hot commissioning of the Actinide Separation Demonstration Facility (ASDF) at BARC, Tarapur. The engineering scale Actinide Separation Demonstration Facility (ASDF) has been retrofitted in an available radiological hot cell situated adjacent to the Advanced Vitrification Facility (AVS). This location advantage ensures an uninterrupted supply of high-level waste and facilitates the vitrification of the high-level waste after separation of minor actinides

Mixed oxide fuel pellet and manufacturing method thereof

International Nuclear Information System (INIS)

Yuda, Ryoichi; Ito, Ken-ichi; Masuda, Hiroshi.

1993-01-01

In a method of manufacturing nuclear fuel pellets which comprises compression molding a mixed oxide powder containing UO 2 and PuO 2 followed by sintering, a sintering agent having a composition comprising about 40 to 80 wt% of SiO 2 and the balance of Al 2 O 3 is mixed to a mixed oxide at a ratio of about 40ppm to about 0.5 wt% based on the total amount of the mixed oxide and the sintering agent, to prepare a mixture. The mixture is molded into a compression product and then sintered at a weakly acidic atmosphere at a temperature of about 1500degC to 1800degC. With such procedures, the sintering agent forms an eutectic product of a single liquid phase, PuO 2 is dispersed over the entire region of the pellet by way of the liquid phase, formation of a solid solution phase is promoted to annihilate a free PuO 2 phase. Further, growth of crystal grains is promoted. Accordingly, since the MOX fuel pellets prepared according to the present invention have a uniform solid solution state, and no free PuO 2 phase remains, increase of FP gas emission due to local nuclear fission of Pu can be avoided. (T.M.)

Selective solvent extraction of actinides associated to liquid scintillation measurements

International Nuclear Information System (INIS)

Ardois, C.; Musikas, C.

1997-01-01

The problems associated to radioactive waste disposal have acquired a special attention due, particularly, to the element instability and, consequently, to their lixiviation and to their peculiarities which are essential in the radioactivity penetration in the food chains; the other important parameters are the produced amounts and the noxiousnesses. New commercial liquid scintillation counters allow rapid α/β measurements. Associated with liquid-liquid extraction techniques, rapid and selective actinide analyses are possible. Among various actinide extractants, such as amines or organophosphorus compounds, we were particularly interested in tri-n-octyl-phosphine oxide (TOPO). Uranium, thorium and americium extractions with (TOPO) in toluene have been investigated. A systematic study of the counting parameters of a PACKARD 2550 TR/AB TM liquid scintillation analyzer is under completion

Subsurface Biogeochemistry of Actinides

Energy Technology Data Exchange (ETDEWEB)

Kersting, Annie B. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Univ. Relations and Science Education; Zavarin, Mavrik [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Inst.

2016-06-29

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) is 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).

Theoretical and experimental study of actinide complexes with monoamides and organophosphorus ligands in solution

International Nuclear Information System (INIS)

Ribokaite, Kristina

2013-01-01

Monoamides and organophosphate are of great interest for the nuclear fuel cycle. Such ligands can selectively extract actinides in liquid-liquid extraction processes. The structure of the extractant (its functional group and its alkyl substituents) has a predominant role in the selective separation of actinides. This thesis concerns the theoretical and experimental studies of model systems in the aim of better understanding of the effect on molecular structures of the complexes. Structures of actinides complexes formed with model ligands in simple media (water or methanol in the presence of nitrate ions) have been characterized. At first, the complexation of uranyl by monoamide and phosphine oxide was studied in water and methanol. Molecular Dynamics simulations and DFT calculations were used to quantify the stability of uranyl complexes with those ligands, and to determine their structural properties. The theoretical results were then compared with experimental results obtained by UV-visible, infrared, Raman and EXAFS on the same chemical systems. The results were used to highlight the greater stability of uranyl complexes with phosphine oxide and monoamides. Further spectroscopic measurements combined with molecular modeling were used to gain a better understanding of the coordination mode of nitrate ion around the uranyl in both water and methanol. Finally, DFT calculations were used to study the influence of the structure of the monoamide or organophosphorus ligand and their interaction with the actinides (IV, VI) including steric effects in the first coordination sphere. (author) [fr

Concentration of actinides in the food chain

International Nuclear Information System (INIS)

Bulman, R.A.

1976-06-01

Considerable concern is now being expressed over the discharge of actinides into the environment. This report presents a brief review of the chemistry of the actinides and examines the evidence for interaction of the actinides with some naturally-occurring chelating agents and other factors which might stimulate actinide concentration in the food chain of man. This report also reviews the evidence for concentration of actinides in plants and for uptake through the gastrointestinal tract. (author)

Thermal-hydraulics of actinide burner reactors

International Nuclear Information System (INIS)

Takizuka, Takakazu; Mukaiyama, Takehiko; Takano, Hideki; Ogawa, Toru; Osakabe, Masahiro.

1989-07-01

As a part of conceptual study of actinide burner reactors, core thermal-hydraulic analyses were conducted for two types of reactor concepts, namely (1) sodium-cooled actinide alloy fuel reactor, and (2) helium-cooled particle-bed reactor, to examine the feasibility of high power-density cores for efficient transmutation of actinides within the maximum allowable temperature limits of fuel and cladding. In addition, calculations were made on cooling of actinide fuel assembly. (author)

Stability constants of the fluoride complexes of actinides in aqueous solution and their correlation with fundamental properties

International Nuclear Information System (INIS)

Chaudhuri, N.K.; Sawant, R.M.

1997-09-01

Stability constants of the fluoride complexes of the actinides in different oxidation states measured by potentiometric method using fluoride ion selective electrode have been presented. Procedure and precautions required to overcome certain difficulties particular to actinide ions have been discussed. Literature data from various sources have been compiled. In order to have a reasonable comparison the stability constant (β 1 ) values obtained in diverse ionic strength media are converted to thermodynamic stability constant, β 1 0 , using Davies equation (a modification of Debye-Huckel equation). A correlation of the β 1 0 values with the fundamental properties of the actinide ions using various models available in the literature has been attempted. A semiempirical relation recently developed by Brown, Sylva and Ellis (BSE equation) appears to be most suitable. Using the values of ionic radii and best available values of the stability constants of a large number of metal ions from recent compilations a comparative study of the various models or relations available in the literature has been tried. For metal ions in general, the best correlation is obtained with the BSE equation. In an attempt to accommodate the unusual trend in the stability constants of the tetravalent actinides a modification in a parameter of the BSE equation has been proposed. Good agreement between the theoretically calculated and experimentally determined values for actinides in different oxidation states is then obtained in most of the cases. (author)

Actinide solubility in deep groundwaters - estimates for upper limits based on chemical equilibrium calculations

International Nuclear Information System (INIS)

Schweingruber, M.

1983-12-01

A chemical equilibrium model is used to estimate maximum upper concentration limits for some actinides (Th, U, Np, Pu, Am) in groundwaters. Eh/pH diagrams for solubility isopleths, dominant dissolved species and limiting solids are constructed for fixed parameter sets including temperature, thermodynamic database, ionic strength and total concentrations of most important inorganic ligands (carbonate, fluoride, phosphate, sulphate, chloride). In order to assess conservative conditions, a reference water is defined with high ligand content and ionic strength, but without competing cations. In addition, actinide oxides and hydroxides are the only solid phases considered. Recommendations for 'safe' upper actinide solubility limits for deep groundwaters are derived from such diagrams, based on the predicted Eh/pH domain. The model results are validated as far as the scarce experimental data permit. (Auth.)

Assessment of Partitioning Processes for Transmutation of Actinides

International Nuclear Information System (INIS)

2010-04-01

To obtain public acceptance of future nuclear fuel cycle technology, new and innovative concepts must overcome the present concerns with respect to both environmental compliance and proliferation of fissile materials. Both these concerns can be addressed through the multiple recycling of all transuranic elements (TRUs) in fast neutron reactor. This is only possible through a process known as partitioning and transmutation scheme (P and T) as this scheme is expected to reduce the long term radio-toxicity as well as the radiogenic heat production of the nuclear waste. Proliferation resistance of separated plutonium could further be enhanced by mixing with self-generated minor actinides. In addition, P and T scheme is expected to extend the nuclear fuel resources on earth about 100 times because of the recycle and reuse of fissile actinides. Several Member States are actively pursuing the research in the field of P and T and consequently several IAEA publications have addressed this topic. The present coordinated research project (CRP) focuses on the potentials in minimizing the residual TRU inventories of the discharged nuclear waste and in enhancing the proliferation resistance of the future civil nuclear fuel cycle. Partitioning approaches can be grouped into aqueous- (hydrometallurgical) and pyroprocesses. Several aqueous processes based on sequential separation of actinides from spent nuclear fuel have been developed and tested at pilot plant scale. In view of the proliferation resistance of the intermediate and final products of a P and T scheme, a group separation of all actinides together is preferable. The present CRP has gathered experts from different organisations and institutes actively involved in developing P and T scheme as mentioned in the list of contributors and also taken into consideration the studies underway in France and the UK. The scientific objectives of the CRP are: To minimize the environmental impact of actinides in the waste stream; To

Ytterbia doped nickel–manganese mixed oxide catalysts for liquid phase oxidation of benzyl alcohol

Directory of Open Access Journals (Sweden)

S.S.P. Sultana

2017-11-01

Full Text Available Nickel–manganese mixed oxides doped with 1, 3, 5 mol% ytterbia have been prepared by co-precipitation method and used in the catalytic oxidation of benzyl alcohol. Catalytic activity of these oxides calcined at 400 °C and 500 °C was studied for selective oxidation of benzyl alcohol to the corresponding aldehyde using molecular oxygen as an oxidizing agent. The results showed that thermally stable 5 mol% ytterbia doped nickel–manganese oxide [Yb2O3-(5%-Ni6MnO8] exhibited highest catalytic performance when it was calcined at 400 °C. A 100% conversion of the benzyl alcohol was achieved with >99% selectivity to benzaldehyde within a reaction period of 5 h at 100 °C. The mixed oxide prepared has been characterized by scanning election microscopy (SEM and energy dispersive X-ray analysis (EDXA, X-ray diffraction (XRD, Fourier transform infrared spectroscopy (FT-IR, thermogravimetric analysis (TGA, Brunauer–Emmett–Teller (BET and temperature programed reduction (H2-TPR.

Actinide colloid generation in groundwater. Part 2

International Nuclear Information System (INIS)

Kim, J.I.

1991-01-01

The progress made in the investigation of actinide colloid generation in groundwater is summarized and discussed with particular examples relevant to an understanding of the migration behaviour of actinides in natural aquifer systems. The first part deals with the characterization of colloids: groundwater colloids, actinide real-colloids and actinide pseudocolloids. The second part concentrates on the generation processes and migration behaviour of actinide pseudo colloids, which are discussed with some notable experimental examples. Importance is stressed more on the chemical aspects of the actinide colloid generation in groundwater. This work is a contribution to the CEC Mirage II project, in particular the complexation and colloids research area

Actinides and fission products partitioning from high level liquid waste

International Nuclear Information System (INIS)

Yamaura, Mitiko

1999-01-01

The presence of small amount of mixed actinides and long-lived heat generators fission products as 137 Cs and 90 Sr are the major problems for safety handling and disposal of high level nuclear wastes. In this work, actinides and fission products partitioning process, as an alternative process for waste treatment is proposed. First of all, ammonium phosphotungstate (PWA), a selective inorganic exchanger for cesium separation was chosen and a new procedure for synthesizing PWA into the organic resin was developed. An strong anionic resin loaded with tungstate or phosphotungstate anion enables the precipitation of PWA directly in the resinous structure by adding the ammonium nitrate in acid medium (R-PWA). Parameters as W/P ratio, pH, reactants, temperature and aging were studied. The R-PWA obtained by using phosphotungstate solution prepared with W/P=9.6, 9 hours digestion time at 94-106 deg C and 4 to 5 months aging time showed the best capacity for cesium retention. On the other hand, Sr separation was performed by technique of extraction chromatography, using DH18C6 impregnated on XAD7 resin as stationary phase. Sr is selectively extracted from acid solution and >99% was recovered from loaded column using distilled water as eluent. Concerning to actinides separations, two extraction chromatographic columns were used. In the first one, TBP(XAD7) column, U and Pu were extracted and its separations were carried-out using HNO 3 and hydroxylamine nitrate + HNO 3 as eluent. In the second one, CMP0-TBP(XAD7) column, the actinides were retained on the column and the separations were done by using (NH 4 ) 2 C 2 O 4 , DTPA, HNO 3 and HCl as eluent. The behavior of some fission products were also verified in both columns. Based on the obtained data, actinides and fission products Cs and Sr partitioning process, using TBP(XAD7) and CMP0-TBP(XAD7) columns for actinides separation, R-PWA column for cesium retention and DH18C6(XAD7) column for Sr isolation was performed

Degradation of organophosphorus pesticide parathion methyl on nanostructured titania-iron mixed oxides

Energy Technology Data Exchange (ETDEWEB)

Henych, Jiří, E-mail: henych@iic.cas.cz [Department of Material Chemistry, Institute of Inorganic Chemistry AS CR v.v.i., 25068 Řež (Czech Republic); Štengl, Václav; Slušná, Michaela; Matys Grygar, Tomáš [Department of Material Chemistry, Institute of Inorganic Chemistry AS CR v.v.i., 25068 Řež (Czech Republic); Janoš, Pavel; Kuráň, Pavel; Štastný, Martin [Faculty of the Environment, J.E. Purkyně University, Králova Výšina 7, 400 96 Ústí nad Labem (Czech Republic)

2015-07-30

Highlights: • Ti–Fe mixed oxides were synthesized via low-temperature one-pot method. • Mixed oxides were used for degradation of parathion methyl. • Pure reference oxide samples showed no degradation ability. • Mixed oxides reached 70% degree of conversion of parathion methyl. - Abstract: Titania-iron mixed oxides with various Ti:Fe ratio were prepared by homogeneous hydrolysis of aqueous solutions of titanium(IV) oxysulphate and iron(III) sulphate with urea as a precipitating agent. The synthesized samples were characterized by X-ray diffraction, Raman and infrared spectroscopy, scanning and transmission electron microscopy, XRF analysis, specific surface area (BET) and porosity determination (BJH). These oxides were used for degradation of organophosporus pesticide parathion methyl. The highest degradation efficiency approaching <70% was found for the samples with Ti:Fe ratio 0.25:1 and 1:0.25. Contrary, parathion methyl was not degraded on the surfaces of pure oxides. In general, the highest degradation rate exhibited samples consisted of the iron or titanium oxide containing a moderate amount of the admixture. However, distinct correlations between the degradation rate and the sorbent composition were not identified.

Selective extraction of trivalent actinides with hard-soft mixed donor ligands: role of intra-ligand synergism

International Nuclear Information System (INIS)

Ghanty, Tapan K.

2016-01-01

In recent years, considerable attention has been given to understand the coordination chemistry of trivalent lanthanide (Ln) and actinide (An) with various ligands because of its close link with the nuclear waste management processes. It is well known that lanthanide-actinide separation is a challenging and difficult task because of very similar chemical properties of these two series of ions, which are associated with similar ionic radii and coordination numbers. Recently, we have introduced a new concept, 'intra-ligand synergism', where hard donor atom, such as, oxygen preferentially binds to trivalent actinides (An(III)) as compared to the valence iso-electronic trivalent lanthanides (Ln(III)) in presence of another soft donor centre. In the present work, the conventional concept of selective complexation of actinides with soft donor ligands (either S or N donor) has been modified through exploiting this concept, and thereby the higher selectivity of 1,10-phenanthroline-2,9-dicarboxylamide (PDAM) based ligands, namely PDAM and its isobutyl and decyl derivatives towards Am(III) ion has been predicted theoretically through density functional calculations. Subsequently, several such amide derivatives have been synthesized to optimize the solubility of the ligands in organic phase. Finally, solvent extraction experiments have been carried out to validate the theoretical prediction on the selectivity of oxygen donor ligands towards Am(III) as compared to Eu(III), and a maximum separation factor of about 51 has been achieved experimentally using 2,9-bis(N-decylaminocarbonyl)-1,10-phenanthroline ligand. The separation factor is increased with the decrease in pH, which is very interesting since extraction of the Am 3+ ion is considered to be important under highly acidic conditions from the nuclear waste management point of view. (author)

Selective oxidation of n-butane to maleic anhydride under oxygen-deficient conditions over V-P-O mixed oxides

NARCIS (Netherlands)

Bosch, H.; Bruggink, A.A.; Ross, J.R.H.

1987-01-01

The selective oxidation of n-butane to maleic anhydride over V-P-O mixed oxides was studied under oxygen deficient conditions. The mixed oxides were prepared with P/V atomic ratios ranging from 0.7 to 1.0. Catalysts with P/V <1.0 did not show any selectivity to maleic anhydride formation, regardless

Synthesis and Evaluation of new Polyfunctional Molecules for Group Actinide Extraction

International Nuclear Information System (INIS)

Marie, C.

2009-10-01

The aim of this project is to design new extracting molecules for spent nuclear fuel reprocessing. In order to minimize the long-term residual radiotoxicity of the waste, the GANEX process is an option based on homogeneous recycling of actinides. All actinides (U, Np, Pu, Am, Cm), present in a highly acidic aqueous solution, would be extracted together and separated from fission products (especially from lanthanides) using liquid-liquid extraction. In this context, twenty new bi-topic ligands constituted of a nitrogen poly-aromatic unit functionalized by amide groups were synthesized. Liquid-liquid extraction tests with these ligands dissolved alone in the organic phase show that N, N, N', N'-tetra-alkyl-6, 6''(2, 2':6', 2''-terpyridine)-diamides are able to selectively extract actinides at different oxidation states (Np(V et VI), U(VI), Pu(IV), Am(III), Cm(III)) from an aqueous solution 3M HNO 3 . Nevertheless, actinides(III) are poorly extracted. According to crystallographic structures of complexes with Nd(III) and U(VI) determined by X-rays diffraction, these ligands are penta-dentate. In solution (methanol), complexes stoichiometries (1:1) of Nd(III), U(VI) and Pu(IV) were determined by electro-spray ionization mass spectrometry. Stability constants, evaluated by UV-visible spectrophotometry in MeOH/H 2 O solutions, confirm the selectivity of ligands toward actinides(III) with respect to lanthanides(III). Associate to nuclear magnetic resonance experiments and DFT calculations (Density Functional Theory), a better knowledge of their coordination mode was achieved. (author)

Fundamental Thermodynamics of Actinide-Bearing Mineral Waste Forms

International Nuclear Information System (INIS)

Williamson, Mark A.; Ebbinghaus, Bartley B.; Navrotsky, Alexandria

1999-01-01

The recent arms reduction treaties between the U.S. and Russia have resulted in inventories of plutonium in excess of current defense needs. Storage of this material poses significant, and unnecessary, risks of diversion, especially for Russia whose infrastructure for protecting these materials has been weakened since the collapse of the Soviet Union. Moreover, maintaining and protecting these materials in their current form is costly. The United States has about sixty metric tons of excess plutonium, half of which is high-purity weapon material. This high purity material will be converted into mixed oxide (MOX) fuel for use in nuclear reactors. The less pure excess plutonium does not meet the specifications for MOX fuel and will not be purified to meet the fuel specifications. Instead, it will be immobilized directly in a ceramic. The ceramic will be encased in a high level waste (HLW) glass monolith (i.e., the can-in-canister option) thus making a form that simulates the intrinsic security of spent nuclear fuel. The immobilized product will be placed in a HLW repository. To meet the repository requirements, the product must be shown to be durable for the intended storage time, the host matrix must be stable in the radiation environment, the solubility and leaching characteristics of the plutonium in the host material must be established, and optimum processing parameters must be determined for the entire compositional envelope of feed materials. In order to provide technically sound solutions to these issues, thermodynamic data are essential in developing an understanding of the chemistry and phase equilibria of the actinide-bearing mineral waste forms proposed as immobilization matrices. However, the relevant thermodynamic data (e.g., enthalpy, entropy, and heat capacity) for the ceramic forms are severely lacking and this information gap directly affects the Energy Department's ability to license the disposal matrices and methods. High-temperature solution

Iron-tellurium-selenium mixed oxide catalysts for the selective oxidation of propylene to acrolein

International Nuclear Information System (INIS)

Patel, B.M.; Price, G.L.

1990-01-01

This paper reports on iron-tellurium-selenium mixed oxide catalysts prepared by coprecipitation from aqueous solution investigated for the propylene to acrolein reaction in the temperature range 543-773 K. Infrared spectroscopy, electron dispersive X-ray analysis, X-ray diffraction, and isotopic tracer techniques have also been employed to characterize this catalytic system. Properties of the Fe-Te-Se mixed oxide catalysts have been compared with Fe-Te mixed oxides in an effort to deduce the functionality of Se. The selenium in the Fe-Te-Se-O catalyst has been found to be the hydrocarbon activating site. The activation energies for the acrolein and carbon dioxide formation are 71 and 54 kJ/mol, respectively. Reactions carried out with 18 O 2 have shown lattice oxygen to be primarily responsible for the formation of both acrolein and carbon dioxide. The initial and rate-determining step for acrolein formation is hydrogen abstraction as determined by an isotope effect associated with the C 3 D 6 reaction. No isotope effect is observed for carbon dioxide formation from C 3 D 6 suggesting that CO 2 is formed by parallel, not consecutive, oxidation of propylene

Minor actinide transmutation on PWR burnable poison rods

International Nuclear Information System (INIS)

Hu, Wenchao; Liu, Bin; Ouyang, Xiaoping; Tu, Jing; Liu, Fang; Huang, Liming; Fu, Juan; Meng, Haiyan

2015-01-01

Highlights: • Key issues associated with MA transmutation are the appropriate loading pattern. • Commercial PWRs are the only choice to transmute MAs in large scale currently. • Considerable amount of MA can be loaded to PWR without disturbing k eff markedly. • Loading MA to PWR burnable poison rods for transmutation is an optimal loading pattern. - Abstract: Minor actinides are the primary contributors to long term radiotoxicity in spent fuel. The majority of commercial reactors in operation in the world are PWRs, so to study the minor actinide transmutation characteristics in the PWRs and ultimately realize the successful minor actinide transmutation in PWRs are crucial problem in the area of the nuclear waste disposal. The key issues associated with the minor actinide transmutation are the appropriate loading patterns when introducing minor actinides to the PWR core. We study two different minor actinide transmutation materials loading patterns on the PWR burnable poison rods, one is to coat a thin layer of minor actinide in the water gap between the zircaloy cladding and the stainless steel which is filled with water, another one is that minor actinides substitute for burnable poison directly within burnable poison rods. Simulation calculation indicates that the two loading patterns can load approximately equivalent to 5–6 PWR annual minor actinide yields without disturbing the PWR k eff markedly. The PWR k eff can return criticality again by slightly reducing the boric acid concentration in the coolant of PWR or removing some burnable poison rods without coating the minor actinide transmutation materials from PWR core. In other words, loading minor actinide transmutation material to PWR does not consume extra neutron, minor actinide just consumes the neutrons which absorbed by the removed control poisons. Both minor actinide loading patterns are technically feasible; most importantly do not need to modify the configuration of the PWR core and

Factors affecting radium removal using mixed iron-manganese oxides

International Nuclear Information System (INIS)

Mott, H.V. Singh, S.; Kondapally, V.R.

1993-01-01

Batch experiments confirmed that sorption of radium by a mixed iron-manganese oxide solid phase shows promise for treating radium-contaminated water. The capacities of these mixed oxides for sorption of radium depend on the composition of the solid phase, the pH of the aqueous solution, and the presence of competing cations. The removal of the oxide-radium complexes from aqueous suspension by manganese greensand filtration was also investigated. It was found that influent radium concentrations of 100 pCi/L were reduced to 2--9 pCi/L by this process. Additional study of the fate of radium in manganese greensand filters is recommended before this procedure is used for drinking water treatment

Factors affecting radium removal using mixed iron-manganese oxides

Energy Technology Data Exchange (ETDEWEB)

Mott, H.V. Singh, S.; Kondapally, V.R. (South Dakota School of Mines and Technology, Rapid City, SD (United States))

1993-10-01

Batch experiments confirmed that sorption of radium by a mixed iron-manganese oxide solid phase shows promise for treating radium-contaminated water. The capacities of these mixed oxides for sorption of radium depend on the composition of the solid phase, the pH of the aqueous solution, and the presence of competing cations. The removal of the oxide-radium complexes from aqueous suspension by manganese greensand filtration was also investigated. It was found that influent radium concentrations of 100 pCi/L were reduced to 2--9 pCi/L by this process. Additional study of the fate of radium in manganese greensand filters is recommended before this procedure is used for drinking water treatment.

A literature review of actinide-carbonate mineral interactions

International Nuclear Information System (INIS)

Stout, D.L.

1993-10-01

Chemical retardation of actinides in groundwater systems is a potentially important mechanism for assessing the performance of the Waste Isolation Pilot Plant (WIPP), a facility intended to demonstrate safe disposal of transuranic waste. Rigorous estimation of chemical retardation during transport through the Culebra Dolomite, a water-bearing unit overlying the WIPP, requires a mechanistic understanding of chemical reactions between dissolved elements and mineral surfaces. This report represents a first step toward this goal by examining the literature for pertinent experimental studies of actinide-carbonate interactions. A summary of existing models is given, along with the types of experiments on which these models are based. Articles pertaining to research into actinide interactions with carbonate minerals are summarized. Select articles involving trace element-carbonate mineral interactions are also reviewed and may serve as templates for future research. A bibliography of related articles is included. Americium(III), and its nonradioactive analog neodymium(III), partition strongly from aqueous solutions into carbonate minerals. Recent thermodynamic, kinetic, and surface studies show that Nd is preferentially removed from solution, forming a Nd-Ca carbonate solid solution. Neptunium(V) is rapidly removed from solution by carbonates. Plutonium incorporation into carbonates is complicated by multiple oxidation states. Little research has been done on the radium(H) and thorium(IV) carbonate systems. Removal of uranyl ion from solution by calcite is limited to monolayer surface coverage

Some new developments in actinide solvent extraction systems

International Nuclear Information System (INIS)

Navratil, J.D.

1988-01-01

Consideration is given to application of neutral and acid organophosphoric compounds, adsorbed on various natural and synthetic carriers, in extraction chromatography for separation and isolation of actinides. It is shown that trioctylphosphine oxide (TOPO) on a solid combustible carrier represents the promising material for plutonium extraction. It was established experimentally that polyurethane foam possessed the maximal capacity with respect to TOPO; extractant losses at that after passing of 50 column volumes of nitric acid don't exceed 2 %

Safe actinide disposition in molten salt reactors

International Nuclear Information System (INIS)

Gat, U.

1997-01-01

Safe molten salt reactors (MSR) can readily accommodate the burning of all fissile actinides. Only minor compromises associated with plutonium are required. The MSRs can dispose safely of actinides and long lived isotopes to result in safer and simpler waste. Disposing of actinides in MSRs does increase the source term of a safety optimized MSR. It is concluded that the burning and transmutation of actinides in MSRs can be done in a safe manner. Development is needed for the processing to handle and separate the actinides. Calculations are needed to establish the neutron economy and the fuel management. 9 refs

Mechanical environmental transport of actinides and ¹³⁷Cs from an arid radioactive waste disposal site.

Science.gov (United States)

Snow, Mathew S; Clark, Sue B; Morrison, Samuel S; Watrous, Matthew G; Olson, John E; Snyder, Darin C

2015-10-01

Aeolian and pluvial processes represent important mechanisms for the movement of actinides and fission products at the Earth's surface. Soil samples taken in the early 1970's near a Department of Energy radioactive waste disposal site (the Subsurface Disposal Area, SDA, located in southeastern Idaho) provide a case study for studying the mechanisms and characteristics of environmental actinide and (137)Cs transport in an arid environment. Multi-component mixing models suggest actinide contamination within 2.5 km of the SDA can be described by mixing between 2 distinct SDA end members and regional nuclear weapons fallout. The absence of chemical fractionation between (241)Am and (239+240)Pu with depth for samples beyond the northeastern corner and lack of (241)Am in-growth over time (due to (241)Pu decay) suggest mechanical transport and mixing of discrete contaminated particles under arid conditions. Occasional samples northeast of the SDA (the direction of the prevailing winds) contain anomalously high concentrations of Pu with (240)Pu/(239)Pu isotopic ratios statistically identical to those in the northeastern corner. Taken together, these data suggest flooding resulted in mechanical transport of contaminated particles into the area between the SDA and a flood containment dike in the northeastern corner, following which subsequent contamination spreading in the northeastern direction resulted from wind transport of discrete particles. Copyright © 2015 Elsevier Ltd. All rights reserved.

Thermodynamic systematics of oxides of americium, curium, and neighboring elements

International Nuclear Information System (INIS)

Morss, L.R.

1984-01-01

Recently-obtained calorimetric data on the sesquioxides and dioxides of americium and curium are summarized. These data are combined with other properties of the actinide elements to elucidate the stability relationships among these oxides and to predict the behavior of neighboring actinide oxides. 45 references, 4 figures, 5 tables

Leaching of irradiated polymers: solution characterization and actinides complexation

International Nuclear Information System (INIS)

Fromentin, Elodie

2017-01-01

The first aim of this work is to study the degradation of an industrial poly-esterurethane (PURm) by radio-oxidation and then by leaching in an alkaline aqueous solution. The second aim is to measure the complexing power of hydro-soluble degradation products (HDP) with actinides. To reach these goals, PURm was first characterized and then radio-oxidized at room temperature with γ rays up to 10 MGy. Second, it was leached at pH 13.3 at different temperature values. Numerous analytical techniques were employed in order to characterize the HDP which were obtained. Europium(III) was used as an analogue of actinides(III) and the behavior of HDP with europium(III) was analyzed by time-resolved luminescence spectroscopy (TRLS). Whatever the dose received by PURm, adipic acid and butane-1,4-diol are the two main HDP in leachates. The leaching data acquired at 40 and 60 C, on the 1 MGy radio-oxidized PURm, correlate with the model given by Yoon et al. (1997). However, the data at room temperature (22 C in average) are not in agreement with the model. Nevertheless, it seems that the plateau which was reached at long-term leaching is the same whatever the temperature used in this study. The results allow to conclude that the predominant mechanism occurring during the leaching of unirradiated and radio-oxidized PURm in an alkaline medium is the hydrolysis of the soft segments ester groups. The complexation of europium(III) by HDP in alkaline medium was demonstrated. The measurement of the complexing power and the identification of ligands was achieved under certain conditions. (author) [fr

1982 Annual Status Report Plutonium Fuels and Actinide Programme

International Nuclear Information System (INIS)

Lindner, R.

1983-01-01

The programme of the Transuranium Institute has long included work on advanced fuels for fast breeder reactors. Study of the swelling of carbide and nitride fuels is now nearing completion, the retention of fission gases in bubbles of different sizes in the fuel having been quantified as function of burn-up and temperature. An important step forward has been achieved in the studies of the Equation of State of Nuclear Fuels up to 5000 K. Formation of some of the less abundant isotopes in PWR fuel has been determined experimentally. Aerosol formation during the fabrication of plutonium containing fuels, part of the activity Safe Handling of Plutonium Fuel has been studied. Head-End Processing of carbide fuels has continued experiments with high burn up mixed carbides. In the field of actinide research the preparation and characterisation of pure specimens is carried out. Effect of actinides on the properties of waste glasses is investigated

Characterization of actinide physics specimens for the US/UK joint experiment in the Dounreay Prototype Fast Reactor

International Nuclear Information System (INIS)

Walker, R.L.; Botts, J.L.; Cooper, J.H.; Adair, H.L.; Bigelow, J.E.; Raman, S.

1983-10-01

The United States and the United Kingdom are engaged in a joint research program in which samples of the higher actinides are irradiated in the Dounreay Prototype Fast Reactor in Scotland. The purpose of the porogram is (1) to study the materials behavior of selected higher actinide fuels and (2) to determine the integral cross sections of a wide variety of the higher actinide isotopes. Samples of the actinides are incorporated in fuel pins inserted in the core. For the fuel study, the actinides selected are 241 Am and 244 Cm in the form of Am 2 O 3 , Cm 2 O 3 , and Am 6 Cm(RE) 7 O 21 , where (RE) represents a mixture of lanthanides. For the cross-section determinations, the samples are milligram quantities of actinide oxides of 248 Cm, 246 Cm, 244 Cm, 243 Cm, 243 Am, 241 Am, 244 Pu, 242 Pu, 241 Pu, 240 Pu, 239 Pu, 238 Pu, 237 Np, 238 U, 236 U, 235 U, 234 U, 233 U, 232 Th, 230 Th, and 231 Pa encapsulated in vanadium. Coincident with the irradiations, neutron flux and energy spectral measurements are made with vanadium-encapsulated dosimeter materials located within the same fuel pins

Actinides burnup in a sodium fast reactor

Energy Technology Data Exchange (ETDEWEB)

Ramirez S, J. R.; Pineda A, R.; Martinez C, E.; Alonso, G., E-mail: ramon.ramirez@inin.gob.mx [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico)

2017-09-15

The burnup of actinides in a nuclear reactor is been proposed as part of an advanced nuclear fuel cycle, this process would close the fuel cycle recycling some of the radioactive material produced in the open nuclear fuel cycle. These actinides are found in the spent nuclear fuel from nuclear power reactors at the end of their burnup in the reactor. Previous studies of actinides recycling in thermal reactors show that would be possible reduce the amounts of actinides at least in 50% of the recycled amounts. in this work, the amounts of actinides that can be burned in a fast reactor is calculated, very interesting results surge from the calculations, first, the amounts of actinides generated by the fuel is higher than for thermal fuel and the composition of the actinides vector is different as in fuel for thermal reactor the main isotope is the {sup 237}Np in the fuel for fast reactor the main isotope is the {sup 241}Am, finally it is concluded that the fast reactor, also generates important amounts of waste. (Author)

Analytical applications of superacid dissolution of actinide and lanthanide substrates

International Nuclear Information System (INIS)

Avens, L.R.; Eller, P.G.; Asprey, L.B.; Abney, K.D.; Kinkead, S.A.

1987-01-01

The superacid system HF/SbF 5 is extraordinarily effective for total dissolution of actinide and lanthanide ceramic oxides, fluorides, and metals. Optical or gamma spectroscopy can be used directly on the solutions. Evaporation of the HF/SbF 5 solvent under vacuum leaves a residue which is easily dissolved by ordinary mineral acids. The resulting aqueous solutions are readily amenable to conventional analytical methods

Controlled synthesis of thorium and uranium oxide nano-crystals

International Nuclear Information System (INIS)

Hudry, Damien; Apostolidis, Christos; Walter, Olaf; Gouder, Thomas; Courtois, Eglantine; Kubel, Christian; Meyer, Daniel

2013-01-01

Very little is known about the size and shape effects on the properties of actinide compounds. As a consequence, the controlled synthesis of well-defined actinide-based nano-crystals constitutes a fundamental step before studying their corresponding properties. In this paper, we report on the non-aqueous surfactant-assisted synthesis of thorium and uranium oxide nano-crystals. The final characteristics of thorium and uranium oxide nano-crystals can be easily tuned by controlling a few experimental parameters such as the nature of the actinide precursor and the composition of the organic system (e.g., the chemical nature of the surfactants and their relative concentrations). Additionally, the influence of these parameters on the outcome of the synthesis is highly dependent on the nature of the actinide element (thorium versus uranium). By using optimised experimental conditions, monodisperse isotropic uranium oxide nano-crystals with different sizes (4.5 and 10.7 nm) as well as branched nano-crystals (overall size ca. 5 nm), nano-dots (ca. 4 nm) and nano-rods (with ultra-small diameters of 1 nm) of thorium oxide were synthesised. (authors)

Burning actinides in very hard spectrum reactors

International Nuclear Information System (INIS)

Robinson, A.H.; Shirley, G.W.; Prichard, A.W.; Trapp, T.J.

1978-01-01

The major unresolved problem in the nuclear industry is the ultimate disposition of the waste products of light water reactors. The study demonstrates the feasibility of designing a very hard spectrum actinide burner reactor (ABR). A 1100 MW/sub t/ ABR design fueled entirely with actinides reprocessed from light water reactor (LWR) wastes is proposed as both an ultimate disposal mechanism for actinides and a means of concurrently producing usable power. Actinides from discharged ABR fuel are recycled to the ABR while fission products are routed to a permanent repository. As an integral part of a large energy park, each such ABR would dispose of the waste actinides from 2 LWRs

Ni–Ta–O mixed oxide catalysts for the low temperature oxidative dehydrogenation of ethane to ethylene

KAUST Repository

Zhu, Haibo; Rosenfeld, Devon C.; Anjum, Dalaver H.; Sangaru, Shiv; Saih, Youssef; Ould-Chikh, Samy; Basset, Jean-Marie

2015-01-01

The "wet" sol-gel and "dry" solid-state methods were used to prepare Ni-Ta-O mixed oxide catalysts. The resulting Ni-Ta oxides exhibit high activity and selectivity for the low temperature oxidative dehydrogenation of ethane to ethylene. The Ta

Actinide separative chemistry

International Nuclear Information System (INIS)

Boullis, B.

2004-01-01

Actinide separative chemistry has focused very heavy work during the last decades. The main was nuclear spent fuel reprocessing: solvent extraction processes appeared quickly a suitable, an efficient way to recover major actinides (uranium and plutonium), and an extensive research, concerning both process chemistry and chemical engineering technologies, allowed the industrial development in this field. We can observe for about half a century a succession of Purex plants which, if based on the same initial discovery (i.e. the outstanding properties of a molecule, the famous TBP), present huge improvements at each step, for a large part due to an increased mastery of the mechanisms involved. And actinide separation should still focus R and D in the near future: there is a real, an important need for this, even if reprocessing may appear as a mature industry. We can present three main reasons for this. First, actinide recycling appear as a key-issue for future nuclear fuel cycles, both for waste management optimization and for conservation of natural resource; and the need concerns not only major actinide but also so-called minor ones, thus enlarging the scope of the investigation. Second, extraction processes are not well mastered at microscopic scale: there is a real, great lack in fundamental knowledge, useful or even necessary for process optimization (for instance, how to design the best extracting molecule, taken into account the several notifications and constraints, from selectivity to radiolytic resistivity?); and such a need for a real optimization is to be more accurate with the search of always cheaper, cleaner processes. And then, there is room too for exploratory research, on new concepts-perhaps for processing quite new fuels- which could appear attractive and justify further developments to be properly assessed: pyro-processes first, but also others, like chemistry in 'extreme' or 'unusual' conditions (supercritical solvents, sono-chemistry, could be

Actinides integral measurements on FCA assemblies

International Nuclear Information System (INIS)

Mukaiyama, Takehiko; Okajima, Shigeaki

1984-01-01

Actinide integral measurements were performed on eight assemblies of FCA where neutron energy spectra were shifted systematically from soft to hard in order to evaluate and modify the nuclear cross section data of major actinides. Experimental values on actinide fission rates and sample reactivity worths are compared with the calculated values using JENDL-2 and ENDF/B-V (or IV) data sets. (author)

Final Project Report for ER15351 ''A Study of New Actinide Zintl Ions Materials''

International Nuclear Information System (INIS)

Peter K. Dorhout

2007-01-01

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, phosphorus-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 metal 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

Actinide burning and waste disposal

Energy Technology Data Exchange (ETDEWEB)

Pigford, T H [University of California, Berkeley, CA (United States)

1990-07-01

Here we review technical and economic features of a new proposal for a synergistic waste-management system involving reprocessing the spent fuel otherwise destined for a U.S. high-level waste repository and transmuting the recovered actinides in a fast reactor. The proposal would require a U.S. fuel reprocessing plant, capable of recovering and recycling all actinides, including neptunium americium, and curium, from LWR spent fuel, at recoveries of 99.9% to 99.999%. The recovered transuranics would fuel the annual introduction of 14 GWe of actinide-burning liquid-metal fast reactors (ALMRs), beginning in the period 2005 to 2012. The new ALMRs would be accompanied by pyrochemical reprocessing facilities to recover and recycle all actinides from discharged ALMR fuel. By the year 2045 all of the LWR spent fuel now destined f a geologic repository would be reprocessed. Costs of constructing and operating these new reprocessing and reactor facilities would be borne by U.S. industry, from the sale of electrical energy produced. The ALMR program expects that ALMRs that burn actinides from LWR spent fuel will be more economical power producers than LWRs as early as 2005 to 2012, so that they can be prudently selected by electric utility companies for new construction of nuclear power plants in that era. Some leaders of DOE and its contractors argue that recovering actinides from spent fuel waste and burning them in fast reactors would reduce the life of the remaining waste to about 200-300 years, instead of 00,000 years. The waste could then be stored above ground until it dies out. Some argue that no geologic repositories would be needed. The current view expressed within the ALMR program is that actinide recycle technology would not replace the need for a geologic repository, but that removing actinides from the waste for even the first repository would simplify design and licensing of that repository. A second geologic repository would not be needed. Waste now planned

Actinide burning and waste disposal

International Nuclear Information System (INIS)

Pigford, T.H.

1990-01-01

Here we review technical and economic features of a new proposal for a synergistic waste-management system involving reprocessing the spent fuel otherwise destined for a U.S. high-level waste repository and transmuting the recovered actinides in a fast reactor. The proposal would require a U.S. fuel reprocessing plant, capable of recovering and recycling all actinides, including neptunium americium, and curium, from LWR spent fuel, at recoveries of 99.9% to 99.999%. The recovered transuranics would fuel the annual introduction of 14 GWe of actinide-burning liquid-metal fast reactors (ALMRs), beginning in the period 2005 to 2012. The new ALMRs would be accompanied by pyrochemical reprocessing facilities to recover and recycle all actinides from discharged ALMR fuel. By the year 2045 all of the LWR spent fuel now destined f a geologic repository would be reprocessed. Costs of constructing and operating these new reprocessing and reactor facilities would be borne by U.S. industry, from the sale of electrical energy produced. The ALMR program expects that ALMRs that burn actinides from LWR spent fuel will be more economical power producers than LWRs as early as 2005 to 2012, so that they can be prudently selected by electric utility companies for new construction of nuclear power plants in that era. Some leaders of DOE and its contractors argue that recovering actinides from spent fuel waste and burning them in fast reactors would reduce the life of the remaining waste to about 200-300 years, instead of 00,000 years. The waste could then be stored above ground until it dies out. Some argue that no geologic repositories would be needed. The current view expressed within the ALMR program is that actinide recycle technology would not replace the need for a geologic repository, but that removing actinides from the waste for even the first repository would simplify design and licensing of that repository. A second geologic repository would not be needed. Waste now planned

Interactions of Microbes found at Aespoe Underground Lab with Actinides such as Curium, Plutonium and Uranium

Energy Technology Data Exchange (ETDEWEB)

Moll, H.; Merroun, M.; Geipel, G.; Rossberg, A.; Hennig, C.; Selenska-Pobell , S.; Bernhard, G. [Forschungszentrum Dresden-Rossendorf e.V., Inst. fuer Radioc hemie, 01314 Dresden (Germany)]. e-mail: h.moll@fzd.de; Stumpf, Th. [Forschungszentru m Karlsruhe, Inst. fuer Nukleare Entsorgung, 76021 Karlsruhe (Germany)

2007-06-15

Sulfate-reducing bacteria (SRB) frequently occur in the deep granitic rock aquifers at the Aespoe Hard Rock Laboratory (Aespoe HRL), Sweden. The new SRB strain Desulfovibrio aespoeensis could be isolated. Results describing the basic interaction mechanisms of uranium, curium, and plutonium with cells of D. aespoeensis DSM 10631T will be presented. The interaction experiments with the actinides showed that the cells are able to remove all three actinides from the surrounding solution. The amount of removed actinide and the interaction mechanism varied among the different actinides. The main U(VI) removal occurred after the first 24 h. The contact time, pH and [U(VI)]initial influence the U removal efficiency. The presence of uranium caused a damaging of the cell membranes. TEM revealed an accumulation of U inside the bacterial cell. D. aespoeensis are able to form U(IV). A complex interaction mechanism takes place consisting of biosorption, bioreduction and bioaccumulation. In the case of {sup 242}Pu, solvent extractions, UV-vis- and XANES spectroscopy were used to determine the speciation of the Pu oxidation states. In the first step, the Pu(VI) and Pu(IV)-polymers are bound to the biomass. Solvent extractions showed that 97 % of the initially present Pu(VI) is reduced to Pu(V) due to the activity of the cells within the first 24 h. Most of the formed Pu(V) dissolves from the cell envelope back to the aqueous solution due to the weak complexing properties of this plutonium oxidation state. In the case of curium at a much lower metal concentration of 3x10{sup -7} M, a pure biosorption of Cm(III) on the cell envelope forming an inner-sphere surface complex most likely with organic phosphate groups was detected. To summarize, the strength of the interaction of D. aespoeensis with the selected actinides at pH 5 and actinide concentrations = 10 mg/L ([Cm] 0.07 mg/L) follows the pattern: Cm > U > Pu >> Np.

Chemistry of actinides and fission products

International Nuclear Information System (INIS)

Pruett, D.J.; Sherrow, S.A.; Toth, L.M.

1988-01-01

This task is concerned primarily with the fundamental chemistry of the actinide and fission product elements. Special efforts are made to develop research programs in collaboration with researchers at universities and in industry who have need of national laboratory facilities. Specific areas currently under investigation include: (1) spectroscopy and photochemistry of actinides in low-temperature matrices; (2) small-angle scattering studies of hydrous actinide and fission product polymers in aqueous and nonaqueous solvents; (3) kinetic and thermodynamic studies of complexation reactions in aqueous and nonaqueous solutions; and (4) the development of inorganic ion exchange materials for actinide and lanthanide separations. Recent results from work in these areas are summarized here

Breaking up of pure and simulated 'burnt' mixed oxide fuel by chemical interaction with oxidized sodium

International Nuclear Information System (INIS)

Besnard, R.; Chaudat, J.P.

1983-01-01

A large experimental program have permitted to investigate the behaviour of mixed oxide fuel coming in contact with hot oxidized sodium. The kinetic of the reaction, the size and the chemical nature of the particules after interaction have been studied. The main part of experiments have been performed using mixed oxide fuel non irradiated at first and with simulated fission products afterwards. Complementary informations have been obtained with UO 2 fuel pellets. After description of the experimental devices, the results are discussed and the importance of the main parameters, like temperature and fission products effect, are pointed out. (orig.)

Modern methods of material accounting for mixed oxide fuel fabrication facility

International Nuclear Information System (INIS)

Eggers, R.F.; Pindak, J.L.; Brouns, R.J.; Williams, R.C.; Brite, D.W.; Kinnison, R.R.; Fager, J.E.

1981-01-01

The generic requirements loss detection, and response to alarms of a contemporary material control and accounting (MCandA) philosophy have been applied to a mixed oxide fuel fabrication plant to produce a detailed preliminary MCandA system design that is generally applicable to facilities of this type. This paper summarizes and discusses detailed results of the mixed oxide fuel fabrication plant study

Catalytic Organic Transformations Mediated by Actinide Complexes

Directory of Open Access Journals (Sweden)

Isabell S. R. Karmel

2015-10-01

Full Text Available This review article presents the development of organoactinides and actinide coordination complexes as catalysts for homogeneous organic transformations. This chapter introduces the basic principles of actinide catalysis and deals with the historic development of actinide complexes in catalytic processes. The application of organoactinides in homogeneous catalysis is exemplified in the hydroelementation reactions, such as the hydroamination, hydrosilylation, hydroalkoxylation and hydrothiolation of alkynes. Additionally, the use of actinide coordination complexes for the catalytic polymerization of α-olefins and the ring opening polymerization of cyclic esters is presented. The last part of this review article highlights novel catalytic transformations mediated by actinide compounds and gives an outlook to the further potential of this field.

Modern methods of material accounting for mixed-oxide fuel-fabrication facility

International Nuclear Information System (INIS)

Eggers, R.F.; Brouns, R.J.; Brite, D.W.; Pindak, J.L.

1981-07-01

The generic requirements loss detection, and response to alarms of a contemporary material control and accounting (MC and A) philosophy have been applied to a mixed-oxide fuel-fabrication plant to produce a detailed preliminary MC and A system design that is generally applicable to facilities of this type. This paper summarizes and discusses detailed results of the mixed-oxide fuel-fabrication plant study. Topics covered in this paper include: mixed-oxide fuel-fabrication process description, process disaggregation into MC and A system control units, quantitative results of analysis of control units for abrupt and recurring loss-detection capability, impact of short- and long-term holdup on loss-detection capability, response to alarms for abrupt loss, and response to alarms for recurring loss

Burn of actinides in MOX fuel cells

International Nuclear Information System (INIS)

Martinez C, E.; Ramirez S, J. R.; Alonso V, G.

2017-09-01

The spent fuel from nuclear reactors is stored temporarily in dry repositories in many countries of the world. However, the main problem of spent fuel, which is its high radio-toxicity in the long term, is not solved. A new strategy is required to close the nuclear fuel cycle and for the sustain ability of nuclear power generation, this strategy could be the recycling of plutonium to obtain more energy and recycle the actinides generated during the irradiation of the fuel to transmute them in less radioactive radionuclides. In this work we evaluate the quantities of actinides generated in different fuels and the quantities of actinides that are generated after their recycling in a thermal reactor. First, we make a reference calculation with a regular enriched uranium fuel, and then is changed to a MOX fuel, varying the plutonium concentrations and determining the quantities of actinides generated. Finally, different amounts of actinides are introduced into a new fuel and the amount of actinides generated at the end of the fuel burn is calculated, in order to determine the reduction of minor actinides obtained. The results show that if the concentration of plutonium in the fuel is high, then the production of minor actinides is also high. The calculations were made using the cell code CASMO-4 and the results obtained are shown in section 6 of this work. (Author)

Ce-Fe-O mixed oxide as oxygen carrier for the direct partial oxidation of methane to syngas

Institute of Scientific and Technical Information of China (English)

魏永刚; 王华; 李孔斋

2010-01-01

The Ce-Fe-O mixed oxide with a ratio of Ce/Fe=7:3, which was prepared by coprecipitation method and employed as oxygen carrier, for direct partial oxidation of methane to syngas in the absence of gaseous oxygen was explored. The mixed oxide was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM), and the catalytic performances were studied in a fixed-bed quartz reactor and a thermogravimetric reactor, respectively. Approximately 99.4% H2 se...

Minor actinide transmutation - a waste management option

International Nuclear Information System (INIS)

Koch, L.

1986-01-01

The incentive to recycle minor actinides results from the reduction of the long-term α-radiological risk rather than from a better utilization of the uranium resources. Nevertheless, the gain in generated electricity by minor actinide transmutation in a fast breeder reactor can compensate for the costs of their recovery and make-up into fuel elements. Different recycling options of minor actinides are discussed: transmutation in liquid metal fast breeder reactors (LMFBRs) is possible as long as plutonium is not recycled in light water reactors (LWRs). In this case a minor actinide burner with fuel of different composition has to be introduced. The development of appropriate minor actinide fuels and their properties are described. The irradiation experiments underway or planned are summarized. A review of minor actinide partitioning from the PUREX waste stream is given. From the present constraints of LMFBR technology a reduction of the long-term α-radiological risk by a factor of 200 is deduced relative to that from the direct storage of spent LWR fuel. Though the present accumulation of minor actinides is low, nuclear transmutation may be needed when nuclear energy production has grown. (orig.)

Process for fabricating mixed-oxide powders

International Nuclear Information System (INIS)

Elmaleh, D.; Giraudel, A.

1975-01-01

A physical-chemical process for fabricating homogeneous powders suitable for sintering is described. It can be applied to the synthesis of all mixed oxides having mutually compatible and water soluble salts. As a specific example, the fabrication of lead titanate-zirconate powders used to make hot pressed ceramics is described. These ceramics show improved piezoelectric properties [fr

DISSOLUTION OF METAL OXIDES AND SEPARATION OF URANIUM FROM LANTHANIDES AND ACTINIDES IN SUPERCRITICAL CARBON DIOXIDE

Energy Technology Data Exchange (ETDEWEB)

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

2013-10-01

This paper investigates the feasibility of extracting and separating uranium from lanthanides and other actinides by using supercritical fluid carbon dioxide (sc-CO2) as a solvent modified with tri-n-butylphosphate (TBP) for the development of a counter current stripping technique, which would be a more efficient and environmentally benign technology for spent nuclear fuel reprocessing compared to traditional solvent extraction. Several actinides (U, Pu, and Np) and europium 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, uranium/europium and uranium/plutonium extraction and separation in sc-CO2 modified with TBP is successful at nitric acid concentrations of less than 6 M and at nitric acid concentrations of less than 3 M with acetohydroxamic acid or oxalic acid, respectively. A scheme for recycling uranium from spent nuclear fuel by using sc-CO2 and counter current stripping columns is presented.

Dustless fabrication process for minor actinide bearing blankets: first applications to (Ce,Gd)O2 and (U,Am)O2

International Nuclear Information System (INIS)

Caisso, M.; Lebreton, F.; Horlait, D.; Delahaye, T.; Picart, S.; Gauthe, A.; Renard, C.; Roussel, P.; Martin, P.; Neuville, D.R.; Ayral, A.

2014-01-01

Minor actinides (MA) are generated in UOX and MOX fuels during irradiation in nuclear reactors. In the framework of their recycling, transmutation of americium in fast neutron reactors through MABB (Minor Actinide-Bearing Blanket) irradiation represents a major research focus. However, MABB fabrication requires special attention due to the high radiotoxicity of MA. Currently, the fabrication of these mixed-oxide pellets follows a powder metallurgy route which generates fine particles. Dustless processes which can avoid the use of such fine, thus highly contaminant, powder in the fabrication line are recommended. In this aim, the development of a spherule route called the calcined resin microsphere pelletizing (CRMP) process has been initiated. The general approach consists of elaborating micrometric spherical mixed-oxide precursors through an adaptation of the weak acid resin (WAR) process, and their compaction into pellets before sintering. The spherule synthesis is based on the fixation of americium and uranium ions into the beads composed of an ion exchange resin, and their mineralization leading to the formation of oxide microspheres. Our study is a first step in the elaboration of mixed-oxide pellets by the CRMP process, using cerium and gadolinium as lanthanide surrogates for uranium and americium, respectively. In a first part, the resin loading with a selected Ce/Gd ratio of 80/20 is described, with the use of actinide nitrates dissolved in aqueous solution. In a second part, characterizations by TGA (thermogravimetric analysis), HT-XRD (high-temperature X-ray diffraction), HT-Raman spectroscopy and HT-XAS (high temperature X-ray absorption spectroscopy) of the loaded resin were performed to study the departure of carbon from the initial structure and the oxide formation. Key temperatures were identified, corresponding to the important steps of the formation of a gadolinium doped ceria solid solution. The organic matter departure happens around 400 K and

Minor actinides transmutation scenario studies with PWRs, FRs and moderated targets

International Nuclear Information System (INIS)

Grouiller, J.P.; Pillon, S.; Saint Jean, C. de; Varaine, F.; Leyval, L.; Vambenepe, G.; Carlier, B.

2003-01-01

Using current technologies, we have demonstrated in this study that it is theoretically possible to obtain different minor actinide transmutation scenarios with a significant gain on the waste radiotoxicity inventory. The handling of objects with Am+Cm entails the significant increase of penetrating radiation sources (neutron and γ) whatever mixed scenario is envisioned; the PWR and FR scenario involving the recycling of Am + Cm in the form of targets results in the lowest flow. In the light of these outcomes, the detailed studies has allowed to design a target sub assembly with a high fission rate (90%) and define a drawing up of reprocessing diagram with the plant head, the minor actinide separation processes (PUREX, DIAMEX and SANEX). Some technological difficulties appear in manipulating curium, principally in manufacturing where the wet process ('sol-gel') is not acquired for (Am+Cm). (author)

Preliminary comparison of three processes of AlN oxidation: dry, wet and mixed ones

Directory of Open Access Journals (Sweden)

Korbutowicz R.

2016-03-01

Full Text Available Three methods of AlN layers oxidation: dry, wet and mixed (wet with oxygen were compared. Some physical parameters of oxidized thin films of aluminum nitride (AlN layers grown on silicon Si(1 1 1 were investigated by means Energy-Dispersive X-ray Spectroscopy (EDS and Spectroscopic Ellipsometry (SE. Three series of the thermal oxidations processes were carried out at 1012 °C in pure nitrogen as carrying gas and various gas ambients: (a dry oxidation with oxygen, (b wet oxidation with water steam and (c mixed atmosphere with various process times. All the research methods have shown that along with the rising of the oxidation time, AlN layer across the aluminum oxide nitride transforms to aluminum oxide. The mixed oxidation was a faster method than the dry or wet ones.

Theoretical Studies of the Electronic Structure of the Compounds of the Actinide Elements

International Nuclear Information System (INIS)

Kaltsoyannis, Nikolas; Hay, P.J.; Li, Jun; Blaudeau, Jean-Philippe; Bursten, Bruce E.

2006-01-01

In this chapter, we will present an overview of the theoretical and computational developments that have increased our understanding of the electronic structure of actinide-containing molecules and ions. The application of modern electronic structure methodologies to actinide systems remains one of the great challenges in quantum chemistry; indeed, as will be discussed below, there is no other portion of the periodic table that leads to the confluence of complexity with respect to the calculation of ground- and excited-state energies, bonding descriptions, and molecular properties. But there is also no place in the periodic table in which effective computational modeling of electronic structure can be more useful. The difficulties in creating, isolating, and handling many of the actinide elements provide an opportunity for computational chemistry to be an unusually important partner in developing the chemistry of these elements. The importance of actinide electronic structure begins with the earliest studies of uranium chemistry and predates the discovery of quantum mechanics. The fluorescence of uranyl compounds was observed as early as 1833, a presage of the development of actinometry as a tool for measuring photochemical quantum yields. Interest in nuclear fuels has stimulated tremendous interest in understanding the properties, including electronic properties, of small actinide-containing molecules and ions, especially the oxides and halides of uranium and plutonium. The synthesis of uranocene in 1968 led to the flurry of activity in the organometallic chemistry of the actinides that continues today. Actinide organometallics (or organoactinides) are nearly always molecular systems and are often volatile, which makes them amenable to an arsenal of experimental probes of molecular and electronic structure (Marks and Fischer, 1979). Theoretical and computational studies of the electronic structure of actinide systems have developed in concert with the experimental

Supported Mixed Oxide Catalysts for the Total Oxidation of Volatile Organic Compounds

Czech Academy of Sciences Publication Activity Database

Kovanda, F.; Jirátová, Květa

2011-01-01

Roč. 176, č. 1 (2011), s. 110-115 ISSN 0920-5861. [International Symposium on Air Pollution Abatement Catalysis (APAC) /2./. Cracow, 08.09.2010-10.09.2010] R&D Projects: GA ČR GAP106/10/1762; GA ČR GA106/09/1664 Institutional research plan: CEZ:AV0Z40720504 Keywords : layered double hydroxides * mixed oxides * ethanol total oxidation Subject RIV: CI - Industrial Chemistry, Chemical Engineering Impact factor: 3.407, year: 2011

Moessbauer effect studies with actinides

International Nuclear Information System (INIS)

Stone, J.A.

1966-01-01

Moessbauer resonance studies in the actinide elements offer a new technique for measuring solid-state properties to a region of the periodic chart where such information is relatively sparse. It is well known that the actinides, the elements with atomic numbers from 90 to 103, form a transition series due to filling of the 5f electron shell, analogous to the rare-earth series in which the 4f shell is filled. Like the rare earths, the actinide metals and compounds are expected to exhibit a variety of interesting magnetic properties, but, unlike the rare earths, there have been few studies of the magnetic behaviour of actinides, and these properties are largely unknown. The chemical properties of the actinides have been studied somewhat more extensively, and, in contrast to the rare earths, form a multiplicity of stable valence states, especially in the lighter members of the series. It is just these properties, magnetic and chemical, for which the Moessbauer effect is a valuable probe, sensitive to the magnetic and electric environment of an atom. The rare-earth series has been a particularly fruitful region in terms of the number of elements which have been shown to exhibit the Moessbauer effect, and for this reason the exploitation of the Moessbauer effect to yield new solid-state and chemical information on the rare earths is a highly active field of research today. There is every reason to believe that the actinides can be similarly studied by the Moessbauer effect. 43 refs, 6 figs, 4 tabs

Evaluation of actinide partitioning and transmutation

International Nuclear Information System (INIS)

1982-01-01

After a few centuries of radioactive decay the long-lived actinides, the elements of atomic numbers 89-103, may constitute the main potential radiological health hazard in nuclear wastes. This is because all but a very few fission products (principally technetium-99 and iodine-129) have by then undergone radioactive decay to insignificant levels, leaving the actinides as the principal radionuclides remaining. It was therefore at first sight an attractive concept to recycle the actinides to nuclear reactors, so as to eliminate them by nuclear fission. Thus, investigations of the feasibility and potential benefits and hazards of the concept of 'actinide partitioning and transmutation' were started in numerous countries in the mid-1970s. This final report summarizes the results and conclusions of technical studies performed in connection with a four-year IAEA Co-ordinated Research Programme, started in 1976, on the ''Environmental Evaluation and Hazard Assessment of the Separation of Actinides from Nuclear Wastes followed by either Transmutation or Separate Disposal''. Although many related studies are still continuing, e.g. on waste disposal, long-term safety assessments, and waste actinide management (particularly for low and intermediate-level wastes), some firm conclusions on the overall concept were drawn by the programme participants, which are reflected in this report

Comparative studies of actinide and sub-actinide fission cross section calculation from MCNP6 and TALYS

International Nuclear Information System (INIS)

Perkasa, Y. S.; Waris, A.; Kurniadi, R.; Su'ud, Z.

2014-01-01

Comparative studies of actinide and sub-actinide fission cross section calculation from MCNP6 and TALYS have been conducted. In this work, fission cross section resulted from MCNP6 prediction will be compared with result from TALYS calculation. MCNP6 with its event generator CEM03.03 and LAQGSM03.03 have been validated and verified for several intermediate and heavy nuclides fission reaction data and also has a good agreement with experimental data for fission reaction that induced by photons, pions, and nucleons at energy from several ten of MeV to about 1 TeV. The calculation that induced within TALYS will be focused mainly to several hundred MeV for actinide and sub-actinide nuclides and will be compared with MCNP6 code and several experimental data from other evaluator

Actinide nanoparticle research

International Nuclear Information System (INIS)

Kalmykov, Stepan N.; Denecke, Melissa A.

2011-01-01

This is the first book to cover actinide nano research. It is of interest both for fundamental research into the chemistry and physics of f-block elements as well as for applied researchers such as those studying the long-term safety of nuclear waste disposal and developing remediation strategies. The authors cover important issues of the formation of actinide nano-particles, their properties and structure, environmental behavior of colloids and nanoparticles related to the safe disposal of nuclear wastes, modeling and advanced methods of characterization at the nano-scale. (orig.)

Burning minor actinides in a HTR energy spectrum

International Nuclear Information System (INIS)

Pohl, Christoph; Rütten, H. Jochem

2012-01-01

Highlights: ► Burn-up analysis for varying plutonium/minor actinide fuel compositions. ► The influence of varying heavy metal fuel element loads is investigated. ► Significant burn-up via radiative capture and subsequently fission is observed. ► Difference observed between fuel element burn-up and total actinide burning rate. - Abstract: The generation of nuclear energy by means of the existing nuclear reactor systems is based mainly on the fission of U-235. But this comes along with the capture of neutrons by the U-238 faction and results in a build-up of plutonium isotopes and minor actinides as neptunium, americium and curium. These actinides are dominant for the long time assessment of the radiological risk of a final disposal therefore a minimization of the long living isotopes is aspired. Burning the actinides in a high temperature helium cooled graphite moderated reactor (HTR) is one of these options. The use of plutonium isotopes to sustain the criticality of the system is intended to avoid on the one hand highly enriched uranium because of international regulations and on the other hand low enriched uranium because of the build up of new actinides from neutron capture in the U-238 fraction. Because initial minor actinide isotopes are typically not fissionable by thermal neutrons the idea is to fission instead the intermediate isotopes generated by the first neutron capture. This paper comprises calculations for plutonium/minor actinides/thorium fuel compositions and their correlated final burn-up for a generic pebble bed HTR based on the reference design of the 400 MW PBMR. In particular the cross sections and the neutron balance of the different minor actinide isotopes in the higher thermal energy spectrum of a HTR will be discussed. For a fuel mixture of plutonium and minor actinides a significant burn-up of these actinides up to 20% can be achieved but at the expense of a higher residual fraction of plutonium in the burned fuel. Combining

Sol-gel chemistry applied to the synthesis of polymetallic oxides including actinides reactivity and structure from solution to solid state

International Nuclear Information System (INIS)

Lemonnier, St.

2006-02-01

Minor actinides transmutation is studied at present in order to reduce the radiotoxicity of nuclear waste and the assessment of its technical feasibility requires specific designed materials. When considering americium, yttria stabilized zirconia (Am III YII Zriv)Or x is among the ceramic phases that one which presents the required physico-chemical properties. An innovative synthesis of this mixed oxide by sol-gel process is reported in this manuscript. The main aim of this work is to adjust the reactivity of the different metallic cations in aqueous media using complexing agent, in order to initiate a favourable interaction for a homogeneous elements repartition in the forming solid phase. The originality of the settled synthesis lies on an in-situ formation of a stable and monodisperse nano-particles dispersion in the presence of acetylacetone. The main reaction mechanisms have been identified: the sol stabilisation results from an original interaction between the three compounds (Zrly, trivalent cations and acetylacetone). The sol corresponds to a structured system at the nanometer scale for which zirconium and trivalent cations are homogeneously dispersed, preliminary to the sol-gel transition. Furthermore, preliminary studies were carried out with a view to developing materials. They have demonstrated that numerous innovative and potential applications can be developed by taking advantage of the direct and controlled formation of the sol and by adapting the sol-gel transition. The most illustrating result is the preparation of a sintered pellet with the composition Am0,13Zro,73Yo,0901,89 using this approach. (author)

Actinides reduction by recycling in a thermal reactor

International Nuclear Information System (INIS)

Ramirez S, J. R.; Martinez C, E.; Balboa L, H.

2014-10-01

This work is directed towards the evaluation of an advanced nuclear fuel cycle in which radioactive actinides could be recycled to remove most of the radioactive material; firstly a production reference of actinides in standard nuclear fuel of uranium at the end of its burning in a BWR reactor is established, after a fuel containing plutonium is modeled to also calculate the actinides production in MOX fuel type. Also it proposes a design of fuel rod containing 6% of actinides in a matrix of uranium from the tails of enrichment, then four standard uranium fuel rods are replaced by actinides rods to evaluate the production and transmutation thereof, the same procedure was performed in the fuel type MOX and the end actinide reduction in the fuel was evaluated. (Author)

Passive measurements of mixed-oxide fuel for nuclear nonproliferation

International Nuclear Information System (INIS)

Dolan, Jennifer L.; Flaska, Marek; Pozzi, Sara A.; Chichester, David L.

2013-01-01

We present new results on passive measurements and simulations of mixed-oxide fuel-pin assemblies. Potential tools for mixed-oxide fuel pin characterization are discussed for future nuclear-nonproliferation applications. Four EJ-309 liquid scintillation detectors coupled with an accurate pulse timing and digital, offline and optimized pulse-shape discrimination method were used. Measurement analysis included pulse-height distributions to distinguish between purely fission neutron sources and alpha-n plus fission neutrons sources. Time-dependent cross-correlation functions were analyzed to measure the fission neutron contribution to the measured sample's neutron source. The use of Monte Carlo particle transport code MCNPX-PoliMi is discussed in conjunction with the measurements

Co-Mn-Al Mixed Oxides as Catalysts for Ammonia Oxidation to N2O.

Czech Academy of Sciences Publication Activity Database

Ludvíková, Jana; Jablońska, M.; Jirátová, Květa; Chmielarz, L.; Balabánová, Jana; Kovanda, F.; Obalová, L.

2016-01-01

Roč. 42, č. 3 (2016), s. 2669-2690 ISSN 0922-6168 R&D Projects: GA ČR GA14-13750S Institutional support: RVO:67985858 Keywords : Co-Mn-Al mixed oxide s * catalytic ammonia oxidation * N2O production * mechanochemical production Subject RIV: CI - Industrial Chemistry, Chemical Engineering Impact factor: 1.369, year: 2016

Light element thermodynamics related to actinide separations

International Nuclear Information System (INIS)

Johnson, I.; Johnson, C.E.

1997-01-01

The accumulation of waste from the last five decades of nuclear reactor development has resulted in large quantities of materials of very diverse chemical composition. An electrometallurgical (EM) method is being developed to separate the components of the waste into several unique streams suitable for permanent disposal and an actinide stream suitable for retrievable storage. The principal types of nuclear wastes are spent oxide or metallic fuel. Since the EM module requires a metallic feed, and oxygen interferes with its operation, the oxide fuel has to be reduced prior to EM treatment. Further, the wastes contain, in addition to oxygen, other light elements (first- and second-row elements) that may also interfere with the operation of the EM module. The extent that these light elements interfere with the operation of the EM module has been determined by chemical thermodynamic calculations. (orig.)

Actinide recycling by pyro process for future nuclear fuel cycle system

International Nuclear Information System (INIS)

Inoue, T.

2001-01-01

Pyrometallurgical technology is one of the potential devices for the future nuclear fuel cycle. Not only economic advantage but also environmental safety and strong resistance for proliferation are required. So as to satisfy the requirements, actinide recycling applicable to LWR and FBR cycles by pyro-process has been developed over a ten-year period at the CRIEPI. The main technology is electrorefining for U and Pu separation and reductive extraction for TRU separation, which can be applied on oxide fuels through reduction process as well as metal fuels. The application of this technology for separation of TRU in HLLW through chlorination could contribute to the improvement of public acceptance with regard to geologic disposal. The main achievements are summarised as follows: - Elemental technologies such as electrorefining, reductive extraction, injection casting and salt waste treatment and solidification have been successfully developed with lots of experiments. - Fuel dissolution into molten salt and uranium recovery on solid cathode for electrorefining has been demonstrated at an engineering scale facility in Argonne National Laboratory using spent fuels and at the CRIEPI through uranium tests. - Single element tests using actinides showed Li reduction to be technically feasible; the subjects of technical feasibility on multi-element systems and on effective recycle of Li by electrolysis of Li 2 O remain to be addressed. - Concerning the treatment of HLLW for actinide separation, the conversion to chlorides through oxides has also been established through uranium tests. - It is confirmed that more than 99% of TRU nuclides can be recovered from high-level liquid waste by TRU tests. - Through these studies, the process flowsheets for reprocessing of metal and oxide fuels and for partitioning of TRU separation have been established. The subjects to be emphasised for further development are classified into three categories: process development (demonstration

Preparation of mixed oxides (Th,U)O2: an evaluation of different techniques

International Nuclear Information System (INIS)

Ayoub, Jamil Mahmoud Said

1999-01-01

An evaluation of different ways of obtaining (Th-U)O 2 mixed oxides is described. Coprecipitation, mechanical mixing of uranium and thorium powders, and the sol-gel technique were studied in order to get a large spectrum of knowledge of the process performance. The use of ultrasonic waves for the homogenization of the hydroxide mixture and microwave heating for powder drying was also investigated. Sol-gel showed the best results regarding the specific area for obtained samples. Oxide drying by microwave is an effective method to get mixed oxides for fuel fabrication. Neither coprecipitation nor mechanical mixing of the thorium and uranium oxide powders is suitable for the purpose. The obtained data are less than 70% than those achieved when sol-gel process is performed. Electronic microscopy, X-ray fluorescence and diffraction, thermogravimetry, specific gravidity and specific area determination (BET) used for sample characterization were convenient and accomplished good results. (author)

Introduction of mixed oxide fuel elements in the belgian cores

International Nuclear Information System (INIS)

Charlier, A.F.; Hollasky, N.A.

1994-01-01

The important amount of plutonium recovered from the reprocessing of spent fuel on the one hand, the national and international experience of the use of mixed oxide UO 2 -PuO 2 fuel in power reactors on the other hand, have led Belgian utilities to decide the introduction of Mixed-Oxide fuel in Doel unit 3 and Tihange unit 2 cores. The 'MOX' project has shown that it was possible without reducing safety or requiring modifications of the plant equipment. It has been approved by the Belgian 'Nuclear Safety Commission'. (authors). 1 tab., 2 figs

Potential carcinogenic effects of actinides in the environment

International Nuclear Information System (INIS)

Harley, N.H.; Pasternack, B.S.

1979-01-01

Inhalation of alpha emitting actinides delivers a dose to critical cancer sites in the human body. These sites are the bronchial epithelium and cells near bone surfaces. Inhalation of the naturally occurring actinides uranium and thorium in resuspended soil in the air results in a continuous exposure for the global population of about 0.1 fCi/m 3 for each of these actinides. The highest dose is from the natural actinide 230 Th. Over 50 yr, the dose to bronchial epithelium is 0.05 mrad and to bone surfaces 0.4 mrad. In the case of accidental environmental contamination (e.g. near a nuclear fuel reprocessing plant) the man-made actinides plutonium, americium and curium could deliver about the same alpha dose to these sites if the soil is contaminated to the same level as the natural actinides (approximately 1 pCi/g). Two nuclear accidents have already produced contamination of about this level. Exposures in this case, however, are to small local populations compared with global exposure for the natural actinides. Significant enhancement of the natural radioactive actinide pollution by combustion of all types of fossil fuel is suspected but not enough data are available to estimate total population doses. (author)

End point control of an actinide precipitation reactor

International Nuclear Information System (INIS)

Muske, K.R.

1997-01-01

The actinide precipitation reactors in the nuclear materials processing facility at Los Alamos National Laboratory are used to remove actinides and other heavy metals from the effluent streams generated during the purification of plutonium. These effluent streams consist of hydrochloric acid solutions, ranging from one to five molar in concentration, in which actinides and other metals are dissolved. The actinides present are plutonium and americium. Typical actinide loadings range from one to five grams per liter. The most prevalent heavy metals are iron, chromium, and nickel that are due to stainless steel. Removal of these metals from solution is accomplished by hydroxide precipitation during the neutralization of the effluent. An end point control algorithm for the semi-batch actinide precipitation reactors at Los Alamos National Laboratory is described. The algorithm is based on an equilibrium solubility model of the chemical species in solution. This model is used to predict the amount of base hydroxide necessary to reach the end point of the actinide precipitation reaction. The model parameters are updated by on-line pH measurements

On the suitability of lanthanides as actinide analogs

International Nuclear Information System (INIS)

Raymond, Kenneth; Szigethy, Geza

2008-01-01

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 group 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)

Review of actinide decorporation with chelating agents

Energy Technology Data Exchange (ETDEWEB)

Ansoborlo, E. [CEA Valrho, Dir. de l' Energie Nucleaire (DEN/DRCP/CETAMA), 30 - Marcoule (France); Amekraz, B.; Moulin, Ch. [CEA Saclay, Dept. de Physico-Chimie (DEN/DPC/SECR), 91 - Gif sur Yvette (France); Moulin, V. [CEA Saclay, Dir. du Developpement et de l' Innovation Nucleares (DEN/DDIN/MR), 91 - Gif Sur Yvette (France); Taran, F. [CEA Saclay (DSV/DBJC/SMMCB), 91 - Gif-sur-Yvette (France); Bailly, Th.; Burgada, R. [Centre National de la Recherche Scientifique (CNRS/LCSB/UMR 7033), 93 - Bobigny (France); Henge-Napoli, M.H. [CEA Valrho, Site de Marcoule (INSTN), 30 (France); Jeanson, A.; Den Auwer, Ch.; Bonin, L.; Moisy, Ph. [CEA Valrho, Dir. de l' Energie Nucleaire (DEN/DRCP/SCPS), 30 - Marcoule (France)

2007-10-15

In case of accidental release of radionuclides in a nuclear facility or in the environment, internal contamination (inhalation, ingestion or wound) with actinides represents a severe health risk to human beings. It is therefore important to provide effective chelation therapy or decorporation to reduce acute radiation damage, chemical toxicity, and late radiation effects. Speciation governs bioavailability and toxicity of elements and it is a prerequisite tool for the design and success of new ligands or chelating agents. The purpose of this review is to present the state-of-the-art of actinide decorporation within biological media, to recall briefly actinide metabolism, to list the basic constraints of actinide-ligand for development, to describe main tools developed and used for decorporation studies, to review mainly the chelating agents tested for actinides, and finally to conclude on the future trends in this field. (authors)

Transmutation of waste actinides in light water reactors

International Nuclear Information System (INIS)

Gorrell, T.C.

1979-04-01

Actinide recycle and transmutation calculations were made for three irradiation options of a light water reactor (LWR). The cases considered were: all actinides recycled in regular uranium fuel assemblies; transuranic actinides recycled in separate MOX assemblies with 235 U enrichment of uranium; and transuranic actinides recycled in separate MOX assemblies with plutonium enrichment of natural uranium. When all actinides were recycled in a uniform lattice, the transuranic inventory after ten recycles was 38% of the inventory accumulated without recycle. When the transuranics from two regular uranium assemblies were combined with those recycled from a MOX assembly, the transuranic inventory was reduced 50% after five recycles

Chemical compatibility of HLW borosilicate glasses with actinides

International Nuclear Information System (INIS)

Walker, C.T.; Scheffler, K.; Riege, U.

1978-11-01

During liquid storage of HLLW the formation of actinide enriched sludges is being expected. Also during melting of HLW glasses an increase of top-to-bottom actinide concentrations can take place. Both effects have been studied. Besides, the vitrification of plutonium enriched wastes from Pu fuel element fabrication plants has been investigated with respect to an isolated vitrification process or a combined one with the HLLW. It is shown that the solidification of actinides from HLLW and actinide waste concentrates will set no principal problems. The leaching of actinides has been measured in salt brine at 23 0 C and 115 0 C. (orig.) [de

A magnetic route to measure the average oxidation state of mixed-valent manganese in manganese oxide octahedral molecular sieves (OMS).

Science.gov (United States)

Shen, Xiong-Fei; Ding, Yun-Shuang; Liu, Jia; Han, Zhao-Hui; Budnick, Joseph I; Hines, William A; Suib, Steven L

2005-05-04

A magnetic route has been applied for measurement of the average oxidation state (AOS) of mixed-valent manganese in manganese oxide octahedral molecular sieves (OMS). The method gives AOS measurement results in good agreement with titration methods. A maximum analysis deviation error of +/-7% is obtained from 10 sample measurements. The magnetic method is able to (1) confirm the presence of mixed-valent manganese and (2) evaluate AOS and the spin states of d electrons of both single oxidation state and mixed-valent state Mn in manganese oxides. In addition, the magnetic method may be extended to (1) determine AOS of Mn in manganese oxide OMS with dopant "diamagnetic" ions, such as reducible V5+ (3d0) ions, which is inappropriate for the titration method due to interference of redox reactions between these dopant ions and titration reagents, such as KMnO4, (2) evaluate the dopant "paramagnetic" ions that are present as clusters or in the OMS framework, and (3) determine AOS of other mixed-valent/single oxidation state ion systems, such as Mo3+(3d3)-Mo4+(3d2) systems and Fe3+ in FeCl3.

Chlorination of UO2, PuO2, and rare-earth oxides using ZrCl4

International Nuclear Information System (INIS)

Sakamura, Yoshiharu; Inoue, Tadashi; Iwai, Takashi; Moriyama, Hirotake

2001-01-01

A new chlorination method using ZrCl 4 , which has a high reactivity with oxygen, has been investigated for more efficient oxide treatment. After actinide oxides are chlorinated and dissolved in a molten salt bath, actinide metals can be selectively collected using the electrorefining process. This process is well suited for pyrochemical reprocessing of metallic fuels. In LiCl-KCI eutectic melts, rare-earth oxides (Y 2 O 3 , La 2 O 3 , CeO 2 , and Nd 2 O 3 ) and actinide oxides (UO 2 and PuO 2 ) were chlorinated by adding ZrCl 4 . As a result, rare-earth and actinide elements were dissolved into the salt as trivalent ions and ZrO 2 was precipitated. When an excess of ZrCI 4 was added, oxides in powder form were completely chlorinated in five hours. It was demonstrated that the ZrCI 4 chlorination method, free from corrosive gas such as chlorine, was very simple and useful. (author)

The role of humic acid on the formation of HAS (hydroxy-aluminosilicate) colloid-borne actinides

Energy Technology Data Exchange (ETDEWEB)

Priemyshev, A.; Kim, M.A. [Inst. fuer Radiochemie, Technische Universitaet Muenchen, D-85748 Garching (Germany); Breban, D.; Panak, P.J.; Yun, J.I.; Kim, J.I.; Fanghanel, Th. [Inst. fuer Nukleare Entsorgung, Forschungszentrum Karlsruhe, D-76021 Karlsruhe (Germany); Mansel, A. [Inst. fuer Interdisziplinaere Isotopenforschung, Georadiochemie, Leipzig, D-04318 Leipzig (Germany)

2005-07-01

Full text of publication follows: One of the major unknowns in the process of actinide migration is the formation of their colloid-borne species. Previous studies have been directed to the incorporation of actinides into HAS (hydroxy-aluminosilicate) colloids generated by the nucleation of Si and Al. The present work further pursues the behaviour of actinides at HAS colloid formation but in the presence of humic acid that is known to be an ubiquitous groundwater constituent. The formation and degree of stability of the aluminosilicate binding for the generation of HAS colloids are investigated at first in the absence of actinides. Free and complexed Al resulting from ligand competitions reactions for the complexation of Al with mono-silicic acid, poly-silicic acid and EDTA are monitored spectroscopically by colour reaction. The second part of the study concentrates on the formation and stability of humic colloids using {sup 14}C-labeled humic acid. The activity distribution is ascertained in the ionic, colloidal and precipitated fractions under different conditions of colloid formation, e.g. as a function of pH, time, humic acid and Al concentration. The third part follows the appraisal of appropriate conditions under which stable HAS and humic colloids are formed, and their interaction with actinides, either separately or in competition. Trace actinides of different oxidation states {sup 241}Am(III), {sup 234}Th(IV) and {sup 233}U(VI) are taken for the purpose. HAS colloids generated from poly-silicic acid at neutral pH show EDTA-resistance, whereas HAS colloids formed from mono-silicic acid become EDTA-resistant only by aging (> one month). Humic acid appears to stabilize HAS colloids, unless the loading capacity of humic acid for the Al ion is exceeded. The incorporation of actinides into the colloidal phase is generally enhanced in the presence of humic acid. Synergic effects produce chimeric HAS-humic colloids into which tri-, tetra- and hexavalent actinides

Selective propene oxidation on mixed metal oxide catalysts

International Nuclear Information System (INIS)

James, David William

2002-01-01

Selective catalytic oxidation processes represent a large segment of the modern chemical industry and a major application of these is the selective partial oxidation of propene to produce acrolein. Mixed metal oxide catalysts are particularly effective in promoting this reaction, and the two primary candidates for the industrial process are based on iron antimonate and bismuth molybdate. Some debate exists in the literature regarding the operation of these materials and the roles of their catalytic components. In particular, iron antimonate catalysts containing excess antimony are known to be highly selective towards acrolein, and a variety of proposals for the enhanced selectivity of such materials have been given. The aim of this work was to provide a direct comparison between the behaviour of bismuth molybdate and iron antimonate catalysts, with additional emphasis being placed on the component single oxide phases of the latter. Studies were also extended to other antimonate-based catalysts, including cobalt antimonate and vanadium antimonate. Reactivity measurements were made using a continuous flow microreactor, which was used in conjunction with a variety of characterisation techniques to determine relationships between the catalytic behaviour and the properties of the materials. The ratio of Fe/Sb in the iron antimonate catalyst affects the reactivity of the system under steady state conditions, with additional iron beyond the stoichiometric value being detrimental to the acrolein selectivity, while extra antimony provides a means of enhancing the selectivity by decreasing acrolein combustion. Studies on the single antimony oxides of iron antimonate have shown a similarity between the reactivity of 'Sb 2 O 5 ' and FeSbO 4 , and a significant difference between these and the Sb 2 O 3 and Sb 2 O 4 phases, implying that the mixed oxide catalyst has a surface mainly comprised of Sb 5+ . The lack of reactivity of Sb 2 O 4 implies a similarity of the surface with

Reducibility of ceria-lanthana mixed oxides under temperature programmed hydrogen and inert gas flow conditions

International Nuclear Information System (INIS)

Bernal, S.; Blanco, G.; Cifredo, G.; Perez-Omil, J.A.; Pintado, J.M.; Rodriguez-Izquierdo, J.M.

1997-01-01

The present paper deals with the preparation and characterization of La/Ce mixed oxides, with La molar contents of 20, 36 and 57%. We carry out the study of the structural, textural and redox properties of the mixed oxides, comparing our results with those for pure ceria. For this aim we use temperature programmed reduction (TPR), temperature programmed desorption (TPD), nitrogen physisorption at 77 K, X-ray diffraction and high resolution electron microscopy. The mixed oxides are more easy to reduce in a flow of hydrogen than ceria. Moreover, in an inert gas flow they release oxygen in higher amounts and at lower temperatures than pure CeO 2 . The textural stability of the mixed oxides is also improved by incorporation of lanthana. All these properties make the ceria-lanthana mixed oxides interesting alternative candidates to substitute ceria in three-way catalyst formulations. (orig.)

Addressing mixed waste in plutonium processing

International Nuclear Information System (INIS)

Christensen, D.C.; Sohn, C.L.; Reid, R.A.

1991-01-01

The overall goal is the minimization of all waste generated in actinide processing facilities. Current emphasis is directed toward reducing and managing mixed waste in plutonium processing facilities. More specifically, the focus is on prioritizing plutonium processing technologies for development that will address major problems in mixed waste management. A five step methodological approach to identify, analyze, solve, and initiate corrective action for mixed waste problems in plutonium processing facilities has been developed

A new type of active actinide target for studying fission and (n,xn) reactions

International Nuclear Information System (INIS)

Belier, G.; Aupiais, J.; Varignon, C.; Vayre, S.

2011-01-01

A new type of active target for the detection of fission of actinides has been developed, it is based on α spectrometry through liquid scintillation. The target uses the liquid-liquid extraction in order to mix the actinide with the liquid organic scintillator. The actinide to be detected is inside the detector itself which maximises the efficiency of the detector. The use of an organic scintillator allows the identification of the particles emitted. Indeed, the time delay for the transfer of the energy deposited in the solvent towards the scintillating molecules depends on the type of the energy deposits: instantaneous fluorescence is obtained for direct excitation while delayed fluorescence is obtained for energy deposits through ionization. By discriminating the different slow and quick components of the photomultiplier signal it is then possible to identify the particle: beta, alpha or fission products. This target has been tested with Cf 252 irradiated with 18 MeV neutrons, the experimental data show different peaks corresponding to alpha decay (97%), spontaneous fission (3%), beta decay and recoil protons due to neutron emissions. (A.C.)

Separation of actinides and lanthanides from acidic nuclear wastes by supported liquid membranes

International Nuclear Information System (INIS)

Danesi, P.R.; Chiarizia, R.; Rickert, P.; Horwitz, E.P.

1985-01-01

Supported liquid membranes, SLM, consisting of a solution of 0.25 M octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) and 0.75 M tributylphosphate (TBP) in decalin absorbed on thin microporous polypropylene supports, have been studied for their ability to perform selective separations and concentrations of actinide and lanthanide ions from synthetic acidic nuclear wastes. The permeability coefficients of selected actinides (Am, Pu, U, Np) and of some of the other major components of the wastes have been measured using SLMs in flat-sheet and hollow-fiber configurations. The results have shown that with the thin (25 μm) flat-sheet SLMs, using Celgard 2500 as support, the membrane permeation process is mainly controlled by the rate of diffusion through the aqueous boundary layers. With the thicker (430 μm) hollow-fiber SLMs, using Accurel hollow-fibers as support, the membrane permeation process is controlled by the rate of diffusion through both the SLM and the aqueous boundary layers. Hollow-fibers SLMs exhibited lower permeability coefficients and longer life-times. The experiments have shown that the actinides can be very efficiently removed from the synthetic waste solutions to the point that the resulting solution could be considered a non-transuranic waste (less than 100 mCi/g of disposed form). The work has demonstrated that actinide removal from synthetic waste solutions is a feasible chemical process at the laboratory scale level

Transmutation of minor actinide using thorium fueled BWR core

International Nuclear Information System (INIS)

Susilo, Jati

2002-01-01

One of the methods to conduct transmutation of minor actinide is the use of BWR with thorium fuel. Thorium fuel has a specific behaviour of producing a little secondary minor actinides. Transmutation of minor actinide is done by loading it in the BWR with thorium fuel through two methods, namely close recycle and accumulation recycle. The calculation of minor actinide composition produced, weigh of minor actinide transmuted, and percentage of reminder transmutation was carried SRAC. The calculations were done to equivalent cell modeling from one fuel rod of BWR. The results show that minor actinide transmutation is more effective using thorium fuel than uranium fuel, through both close recycle and accumulation recycle. Minor actinide transmutation weight show that the same value for those recycle for 5th recycle. And most of all minor actinide produced from 5 unit BWR uranium fuel can transmuted in the 6 t h of close recycle. And, the minimal value of excess reactivity of the core is 12,15 % Δk/k, that is possible value for core operation

Actinide recovery from waste and low-grade sources

International Nuclear Information System (INIS)

Navratil, J.D.; Schulz, W.W.

1982-01-01

Actinide and nuclear fuel cycle operations generate a variety of process waste streams. New methods are needed to remove and recover actinides. More interest is also being expressed in recovering uranium from oceans, phosphoric acid, and other low grade sources. To meet the need for an up-to-date status report in the area of actinide recovery from waste and low grade sources, these papers were brought together. The papers provide an authoritative, in-depth coverage of an important area of nuclear and industrial and engineering chemistry which cover the following topics: uranium recovery from oceans and phosphoric acid; recovery of actinides from solids and liquid wastes; plutonium scrap recovery technology; and other new developments in actinide recovery processes

Methodologies For Characterising Mixed Conducting Oxides For Oxygen Membrane And SOFC Cathode Application

DEFF Research Database (Denmark)

Hendriksen, Peter Vang; Søgaard, Martin; Plonczak, Pawel

2012-01-01

Two methods for detailed characterization of the process of oxygen exchange between the gas phase and a mixed conducting solid oxide are discussed. First, the use of solid electrolyte probes for measuring the change in oxygen activity over the surface of a mixed conductor is presented and advanta......Two methods for detailed characterization of the process of oxygen exchange between the gas phase and a mixed conducting solid oxide are discussed. First, the use of solid electrolyte probes for measuring the change in oxygen activity over the surface of a mixed conductor is presented...

Nuclear waste forms for actinides

Science.gov (United States)

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

Fusion barrier characteristics of actinides

Science.gov (United States)

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 projectile target combinations. The values produced by the present formula are also compared with experiments. The present pocket formula produces fusion barrier characteristics of actinides with the simple inputs of mass number (A) and atomic number (Z) of projectile-targets.

Programme and Abstracts. 38. Journees des Actinides together with the 7. School on the Physics and Chemistry of the Actinides

Energy Technology Data Exchange (ETDEWEB)

NONE

2008-07-01

Journees des Actinides (JdA) is a traditional informal actinide forum, including physics, chemistry, and materials research. It regularly brings together experts from fields involved, taking place in a very informal way, emphasizing exchanges and discussions on current issues in actinide science. At the 38{sup th} JdA (10-15 April 2008; Wroclaw, Poland) scientific communications on the following topics on physics and chemistry of the actinides were presented: (a) inorganic and organometallic chemistry; (b) strongly correlated behaviour, superconductivity, quantum criticality; (c) materials science; (d) theory, electronic structure; (e) nuclear fuel cycle, environment.

Programme and Abstracts. 38. Journees des Actinides together with the 7. School on the Physics and Chemistry of the Actinides

International Nuclear Information System (INIS)

2008-01-01

Journees des Actinides (JdA) is a traditional informal actinide forum, including physics, chemistry, and materials research. It regularly brings together experts from fields involved, taking place in a very informal way, emphasizing exchanges and discussions on current issues in actinide science. At the 38 th JdA (10-15 April 2008; Wroclaw, Poland) scientific communications on the following topics on physics and chemistry of the actinides were presented: (a) inorganic and organometallic chemistry; (b) strongly correlated behaviour, superconductivity, quantum criticality; (c) materials science; (d) theory, electronic structure; (e) nuclear fuel cycle, environment

Dissolution of mixed oxide fuel as a function of fabrication variables

International Nuclear Information System (INIS)

Lerch, R.E.

1979-08-01

Dissolution properties of mechanically blended mixed oxide fuel were very dependent on the six fuel fabrication variables studied. Fuel sintering temperature, source of PuO 2 and PuO 2 content of the fuel had major effects: (1) as the sintering temperature was increased from 1400 to 1700 0 C, pellet dissolution was more complete; (2) pellets made from burned metal derived PuO 2 were more completely dissolved than pellets made from calcined nitrate derived PuO 2 which in turn were more completely dissolved than pellets made from calcined nitrate derived PuO 2 ; (3) as the PuO 2 content decreased from 25 to 15 wt % PuO 2 , pellet dissolution was more complete. Preferential dissolution of uranium occurred in all the mechanically blended mixed oxide. Unirradiated mixed oxide fuel pellets made by the Sol Gel process were generally quite soluble in nitric acid. Unirradiated mixed oxide fuel pellets made by the coprecipitation process dissolved completely and rapidly in nitric acid. Fuel made by the coprecipitation process was more completely dissolved than fuel made by the Sol Gel process which, in turn, was more completely dissolved than fuel made by mechanically blending UO 2 and PuO 2 as shown below. Addition of uncomplexed fluoride to nitric acid during fuel dissolution generally rendered all fuel samples completely dissolvable. In boiling 12M nitric acid, 95 to 99% of the plutonium which was going to dissolve did so in the first hour. Irradiated mechanically blended mixed oxide fuel with known fuel fabrication conditions was also subjected to fuel dissolution tests. While irradiation was shown to increase completeness of plutonium dissolution, poor dissolubility due to adverse fabrication conditions (e.g., low sintering temperature) remained after irradiation

High temperature transient deformation of mixed oxide fuels

International Nuclear Information System (INIS)

Slagle, O.D.

1986-01-01

The purpose of this paper is to present recent experimental results on fuel creep under transient conditions at high temperatures. The effect of temperature, stress, heating rate, density and grain size were considered. An empirical formulation is derived for the relationship between strain, stress, temperature and heating rate. This relationship provides a means for incorporating stress relief into the analysis of fuel-cladding interaction during an overpower transient. The effect of sample density and initial grain size is considered by varying the sample parameters. Previously derived steady-state creep relationships for the high temperature creep of mixed oxide fuel were combined with the time dependency of creep found for UO 2 to calculate a transient creep relationship for mixed oxide fuel. These calculated results were found to be in good agreement with the measured high temperature transient creep results

Actinide Source Term Program, position paper. Revision 1

International Nuclear Information System (INIS)

Novak, C.F.; Papenguth, H.W.; Crafts, C.C.; Dhooge, N.J.

1994-01-01

The Actinide Source Term represents the quantity of actinides that could be mobilized within WIPP brines and could migrate with the brines away from the disposal room vicinity. This document presents the various proposed methods for estimating this source term, with a particular focus on defining these methods and evaluating the defensibility of the models for mobile actinide concentrations. The conclusions reached in this document are: the 92 PA open-quotes expert panelclose quotes model for mobile actinide concentrations is not defensible; and, although it is extremely conservative, the open-quotes inventory limitsclose quotes model is the only existing defensible model for the actinide source term. The model effort in progress, open-quotes chemical modeling of mobile actinide concentrationsclose quotes, supported by a laboratory effort that is also in progress, is designed to provide a reasonable description of the system and be scientifically realistic and supplant the open-quotes Inventory limitsclose quotes model

Photochemical oxidation: A solution for the mixed waste dilemma

Energy Technology Data Exchange (ETDEWEB)

Prellberg, J.W.; Thornton, L.M.; Cheuvront, D.A. [Vulcan Peroxidation Systems, Inc., Tucson, AZ (United States)] [and others

1995-12-31

Numerous technologies are available to remove organic contamination from water or wastewater. A variety of techniques also exist that are used to neutralize radioactive waste. However, few technologies can satisfactorily address the treatment of mixed organic/radioactive waste without creating unacceptable secondary waste products or resulting in extremely high treatment costs. An innovative solution to the mixed waste problem is on-site photochemical oxidation. Liquid-phase photochemical oxidation has a long- standing history of successful application to the destruction of organic compounds. By using photochemical oxidation, the organic contaminants are destroyed on-site leaving the water, with radionuclides, that can be reused or disposed of as appropriate. This technology offers advantages that include zero air emissions, no solid or liquid waste formation, and relatively low treatment cost. Discussion of the photochemical process will be described, and several case histories from recent design testing, including cost analyses for the resulting full-scale installations, will be presented as examples.

Nanostructured Mn-Fe Binary Mixed Oxide: Synthesis, Characterization and Evaluation for Arsenic Removal.

Science.gov (United States)

Pillewan, Pradnya; Mukherjee, Shrabanti; Bansiwal, Amit; Rayalu, Sadhana

2014-07-01

Adsorption of arsenic on bimetallic Mn and Fe mixed oxide was carried out using both field as well as simulated water. The material was synthesized using hydrothermal method and characterized using X-ray diffraction (XRD) and scanning electron microscopy (SEM). Langmuir and Freundlich adsorption isotherms were computed using batch adsorption studies to determine the adsorption capacity of Mn-Fe binary mixed oxide for arsenic. Adsorption capacity for MFBMO obtained from Freundlich model was found to be 2.048 mg/g for simulated water and 1.084 mg/g for field water. Mn-Fe binary mixed oxide was found to be effective adsorbent for removal of arsenic from water.

Description of a reference mixed oxide fuel fabrication plant (MOFFP)

International Nuclear Information System (INIS)

1978-01-01

In order to evaluate the environment impact, due to the Mixed Oxide Fuel Fabrication Plants, work has been initiated to describe the general design and operating conditions of a reference Mixed Oxide Fuel Fabrication Plant (MOFFP) for the 1990 time frame. The various reference data and basic assumptions for the reference MOFFP plant have been defined after discussion with experts. The data reported in this document are only made available to allow an evaluation of the environmental impact due to a reference MOFFP plant. These data have therefore not to be used as recommandation, standards, regulatory guides or requirements

33rd Actinide Separations Conference

Energy Technology Data Exchange (ETDEWEB)

McDonald, L M; Wilk, P A

2009-05-04

Welcome to the 33rd Actinide Separations Conference hosted this year by the Lawrence Livermore National Laboratory. This annual conference is centered on the idea of networking and communication with scientists from throughout the United States, Britain, France and Japan who have expertise in nuclear material processing. This conference forum provides an excellent opportunity for bringing together experts in the fields of chemistry, nuclear and chemical engineering, and actinide processing to present and discuss experiences, research results, testing and application of actinide separation processes. The exchange of information that will take place between you, and other subject matter experts from around the nation and across the international boundaries, is a critical tool to assist in solving both national and international problems associated with the processing of nuclear materials used for both defense and energy purposes, as well as for the safe disposition of excess nuclear material. Granlibakken is a dedicated conference facility and training campus that is set up to provide the venue that supports communication between scientists and engineers attending the 33rd Actinide Separations Conference. We believe that you will find that Granlibakken and the Lake Tahoe views provide an atmosphere that is stimulating for fruitful discussions between participants from both government and private industry. We thank the Lawrence Livermore National Laboratory and the United States Department of Energy for their support of this conference. We especially thank you, the participants and subject matter experts, for your involvement in the 33rd Actinide Separations Conference.

33rd Actinide Separations Conference

International Nuclear Information System (INIS)

McDonald, L.M.; Wilk, P.A.

2009-01-01

Welcome to the 33rd Actinide Separations Conference hosted this year by the Lawrence Livermore National Laboratory. This annual conference is centered on the idea of networking and communication with scientists from throughout the United States, Britain, France and Japan who have expertise in nuclear material processing. This conference forum provides an excellent opportunity for bringing together experts in the fields of chemistry, nuclear and chemical engineering, and actinide processing to present and discuss experiences, research results, testing and application of actinide separation processes. The exchange of information that will take place between you, and other subject matter experts from around the nation and across the international boundaries, is a critical tool to assist in solving both national and international problems associated with the processing of nuclear materials used for both defense and energy purposes, as well as for the safe disposition of excess nuclear material. Granlibakken is a dedicated conference facility and training campus that is set up to provide the venue that supports communication between scientists and engineers attending the 33rd Actinide Separations Conference. We believe that you will find that Granlibakken and the Lake Tahoe views provide an atmosphere that is stimulating for fruitful discussions between participants from both government and private industry. We thank the Lawrence Livermore National Laboratory and the United States Department of Energy for their support of this conference. We especially thank you, the participants and subject matter experts, for your involvement in the 33rd Actinide Separations Conference.

TUCS/phosphate mineralization of actinides

Energy Technology Data Exchange (ETDEWEB)

Nash, K.L. [Argonne National Lab., IL (United States)

1997-10-01

This program has as its objective the development of a new technology that combines cation exchange and mineralization to reduce the concentration of heavy metals (in particular actinides) in groundwaters. The treatment regimen must be compatible with the groundwater and soil, potentially using groundwater/soil components to aid in the immobilization process. The delivery system (probably a water-soluble chelating agent) should first concentrate the radionuclides then release the precipitating anion, which forms thermodynamically stable mineral phases, either with the target metal ions alone or in combination with matrix cations. This approach should generate thermodynamically stable mineral phases resistant to weathering. The chelating agent should decompose spontaneously with time, release the mineralizing agent, and leave a residue that does not interfere with mineral formation. For the actinides, the ideal compound probably will release phosphate, as actinide phosphate mineral phases are among the least soluble species for these metals. The most promising means of delivering the precipitant would be to use a water-soluble, hydrolytically unstable complexant that functions in the initial stages as a cation exchanger to concentrate the metal ions. As it decomposes, the chelating agent releases phosphate to foster formation of crystalline mineral phases. Because it involves only the application of inexpensive reagents, the method of phosphate mineralization promises to be an economical alternative for in situ immobilization of radionuclides (actinides in particular). The method relies on the inherent (thermodynamic) stability of actinide mineral phases.

In vitro and in vivo measurements of the dissolution parameters of uranium and plutonium mixed oxides in biological environment

International Nuclear Information System (INIS)

Matton, S.

1999-01-01

During the mixed-oxide fuel fabrication process, inhalation is potentially the main route of internal contamination. The International Commission on Radiological Protection recommends experimental measurement of parameters such as size and dissolution rate for specific industrial compounds. First, we validated the use of PERALS (Photon Electron Rejecting Alpha Liquid Scintillation) for alpha measurement in biological samples which, in some cases, could improve detection limit. We characterised physical chemical properties in terms of size, specific area and activity of 3 different powders: MOX made according to either the MIMAS process, which showed heterogeneous chemical composition, or the SOLGEL, which showed homogeneous chemical composition and industrial PuO 2 . Their dissolution parameters, f r and s s , as defined in the simplest model proposed by ICRP 66 were measured in vivo, after inhalation in the rat, and in vitro. The statistical variation of these values were expressed as standard deviation. Moreover, in vitro studies demonstrated variation of the s s value depending on the duration of the incubation. We also developed methods to characterise interactions between UO 2 particles and phosphate ions which could be involved in the actinide toxicity. (author) [fr

Comparison of actinides and fission products recycling scheme with the normal plutonium recycling scheme in fast reactors

Directory of Open Access Journals (Sweden)

Salahuddin Asif

2013-01-01

Full Text Available Multiple recycling of actinides and non-volatile fission products in fast reactors through the dry re-fabrication/reprocessing atomics international reduction oxidation process has been studied as a possible way to reduce the long-term potential hazard of nuclear waste compared to that resulting from reprocessing in a wet PUREX process. Calculations have been made to compare the actinides and fission products recycling scheme with the normal plutonium recycling scheme in a fast reactor. For this purpose, the Karlsruhe version of isotope generation and depletion code, KORIGEN, has been modified accordingly. An entirely novel fission product yields library for fast reactors has been created which has replaced the old KORIGEN fission products library. For the purposes of this study, the standard 26 groups data set, KFKINR, developed at Forschungszentrum Karlsruhe, Germany, has been extended by the addition of the cross-sections of 13 important actinides and 68 most important fission products. It has been confirmed that these 68 fission products constitute about 95% of the total fission products yield and about 99.5% of the total absorption due to fission products in fast reactors. The amount of fissile material required to guarantee the criticality of the reactor during recycling schemes has also been investigated. Cumulative high active waste per ton of initial heavy metal is also calculated. Results show that the recycling of actinides and fission products in fast reactors through the atomics international reduction oxidation process results in a reduction of the potential hazard of radioactive waste.

Systematic study of the ion beam mixing of oxide markers into alumina

International Nuclear Information System (INIS)

Cooper, E.A.; Kung, H.; Nastasi, M.

1995-01-01

The study of ion beam mixing of layered compositions is important in two regards: first, there is the potential of alloying the layers into a new functionally different composition and, secondly, from a fundamental aspect, it is important be able to anticipate the potential damage due to degradation of the layer structure that could be caused in these materials due to a radiation environment. The authors have completed a systematic study of ion beam mixing of thin marker layers into amorphous alumina. The degree of mixing was found to be controlled by thermodynamic factors, the nature of the marker (oxidation state), and matrix crystallinity. Ballistic mixing was observed for all markers, but the mixing of some oxide markers exhibits a thermally activated regime at higher temperatures. The experiments were conducted from a low temperature of -170 C to a maximum temperature of 75O C. 210 keV Ar was used to ion beam mix the marker layer at the various temperatures. The marker spreading was analyzed using RBS. The mixing of one marker (Fe 2 O 3 ) into crystalline alumina (sapphire) was compared to that of the amorphous alumina. It was found that the marker mixed asymmetrically into the two matrix materials, with a higher degree of mixing into the amorphous matrix. TEM cross-section results verify that there is a preference for the marker to mix into the amorphous alumina layer preferentially to the crystalline layer. The interest in ion beam mixing of marker layers in ceramic systems is motivated by the fact that layered oxides are technologically important materials for fusion reactor applications

Research for actinides extractants from various wastes

International Nuclear Information System (INIS)

Musikas, C.; Cuillerdier, C.; Condamines, N.

1990-01-01

This paper is an overview of the actinides solvent extraction research undertaken in Fontenay-aux-Roses. Two kinds of extractants are investigated; those usable for the improvement of the nowadays nuclear fuels reprocessing and those necessary for advanced fuels cycles which include the minor actinides (Np, Am) recovery for a further elimination through nuclear reactions. In the first class the mono and diamides, alternative to the organophosphorus extractants, TBP and polyfunctional phosphonates, showed promising properties. The main results are discussed. For the future efficient extractants for trivalent actinides-lanthanides group separations are suitable. The point about the actinides (III) - lanthanides (III) group separation chemistry and the development of some of these extractants are given

Charged defects during alpha-irradiation of actinide oxides as revealed by Raman and luminescence spectroscopy

International Nuclear Information System (INIS)

Mohun, R.; Desgranges, L.; Léchelle, J.; Simon, P.; Guimbretière, G.; Canizarès, A.; Duval, F.; Jegou, C.; Magnin, M.; Clavier, N.; Dacheux, N.; Valot, C.; Vauchy, R.

2016-01-01

We have recently evidenced an original Raman signature of alpha irradiation-induced defects in UO 2 . In this study, we aim to determine whether the same signature also exists in different actinide oxides, namely ThO 2 and PuO 2 . Sintered UO 2 and ThO 2 were initially irradiated with 21 MeV He 2+ ions using a cyclotron device and were subjected to an in situ luminescence experiment followed by Raman analysis. In addition, a PuO 2 sample which had accumulated self-irradiation damage due to alpha particles was investigated only by Raman measurement. Results obtained for the initially white ThO 2 showed that a blue color appeared in the irradiated areas as well as luminescence signals during irradiation. However, Raman spectroscopic analysis showed the absence of Raman signature in ThO 2 . In contrast, the irradiated UO 2 and PuO 2 confirmed the presence of the Raman signature but no luminescence peaks were observed. The proposed mechanism involves electronic defects in ThO 2 , while a coupling between electronic defects and phonons is required to explain the Raman spectra for UO 2 and PuO 2 .

Combining Raman Microprobe and XPS to Study High Temperature Oxidation of Metals

International Nuclear Information System (INIS)

Windisch, Charles F.; Henager, Charles H.; Engelhard, Mark H.; Bennett, Wendy D.

2011-01-01

Raman microprobe spectroscopy was applied in studies of high-temperature air oxidation of a ferritic alloy (HT-9) in the absence and presence of zirconia coatings with the objective of evaluating the technique as a way to quickly screen candidate cladding materials and actinide-based mixed oxide fuel mixtures for advanced nuclear reactors. When oxidation was relatively uniform, Raman spectra collected using microscope optics with low spatial resolution were found to be similar to those collected with conventional Raman spectroscopy. These spectra could be used to identify major oxide corrosion products and follow changes in the composition of the oxides due to heating. However, when the oxidation films were comprised of multiple layers of varying composition, or with layers containing metallic phases, techniques with higher depth resolution and sensitivity to zero-valence metals were necessary. The requirements were met by combining Raman microprobe using different optical configurations and x-ray photoelectron spectroscopy.

Preparation of catalysts based on Ce-Mn mixed oxide by coprecipitation for combustion of n-hexane

International Nuclear Information System (INIS)

Picasso, Gino; Zavala, Cesar; Cruz, Romulo; Sun Kou, Rosario; Lopez, Alcides

2013-01-01

Catalysts based on Ce-Mn mixed with different Ce/Mn molar ratios ranging from 0,5 to 2 have been prepared by coprecipitation at pH constant with ageing times of 4, 18 and 24 h for combustion of n-hexane. XRD patterns of the mixed oxides showed the majority presence of fluorite phase. Specific BET surface areas of mixed oxides were always higher than their single counterparts and their adsorption isotherm depicted a mesoporous surface of Type IV. TPR thermograms confirmed the presence of mixed oxide phase, whose profile shifted to smaller temperatures with increasing content of ceria. Catalytic tests were performed with 2000 ppm of n-hexane and WHSV of 80 h -1 in a fixed-bed reactor. For all samples, only CO 2 and water were observed at total conversion and no partial combustion products were obtained. Ce-Mn mixed oxides were more active than simple oxide samples no matter the aging time. Mixed samples presented thermal stability in contrast with simple ones. Mixed sample with Ce/Mn molar ratio of 2 depicted the highest activity probably due to higher surface area and better reducibility ability of mixed phase. (author)

ACTINET - EU network of excellence for actinide sciences

International Nuclear Information System (INIS)

Gompper, K.

2006-01-01

ACTINET, the Network of Excellence for Actinide Sciences within the 6th EU Framework Program, was launched in March 2004 for an initial period of four years. A number of tools are available in ACTINET to serve the purposes of the project, i.e. stimulate and coordinate actinide research in Europe, promote integration, train young scientists and, in this way, ensure and enhance European competence. The large European actinide laboratories with their unique experimental and analytical equipment are available to scientists from Europe as so-called 'pool facilities' within the framework of joint research projects. Setting up a 'theoretical user lab' has turned out to be a promising way of exploiting the synergies of theory and experiment in various fields of actinide science. Joint research projects are supported within the network, working with actinides being made possible in the pool facilities. Training and instruction are ensured by seminars, workshops, and schools organized annually. In familiarizing young scientists with actinide work, ACTINET exercises training functions and contributes to ensuring and enhancing European competence in the field on the medium and long term. Even after only half of its term, ACTINET is developing into a live network, thus decisively contributing towards promoting, coordinating and integrating European actinide research. As actinides play a key role in the use of nuclear power, this benefits European industries, research centers, operators of nuclear power plants and nuclear facilities as well as licensing and regulatory authorities. (orig.)

Superconductivity in the actinides

International Nuclear Information System (INIS)

Smith, J.L.; Lawson, A.C.

1985-01-01

The trends in the occurrence of superconductivity in actinide materials are discussed. Most of them seem to show simple transition metal behavior. However, the superconductivity of americium proves that the f electrons are localized in that element and that ''actinides'' is the correct name for this row of elements. Recently the superconductivity of UBe 13 and UPt 3 has been shown to be extremely unusual, and these compounds fall in the new class of compounds now known as heavy fermion materials

Study of nuclear energy systems and double strata scenarios for minor actinides transmutation in ADS

International Nuclear Information System (INIS)

Clavel, J.B.

2012-01-01

The French law of 28 June 2006 regarding advanced nuclear waste management requires a scientific assessment to define future industrial strategies. The present PhD thesis was carried in this framework and concerns specifically the research axis of minor actinides transmutation. A high power Accelerator Driven System (ADS) concept is developed at SUBATECH for this purpose. A 1 GeV proton beam feeds three liquid lead-bismuth spallation targets. The Multiple Spallation Target (MUST) ADS reaches the thermal powers up to 1 GW with a high specific power. A nuclear reactor dimensioning method has been developed and applied to different double strata scenarios. In these scenarios, SFR (Sodium Fast Reactors) or PWR (Pressurized Water Reactors) power reactors produce minor actinides that will be transmuted into ADS. In each core (SFR and ADS), the plutonium multi-reprocessing strategy is performed while ADS subcritical core also multi-reprocesses minor actinides. To limit the core reactivity and improve the fuel thermal conductivity, the minor actinides fuel is mixed with MgO inert matrix. Nuclear branches with lead and sodium coolants for the ADS, have been studied for different irradiation times and two transmutation strategies have been assessed: whether whole minor actinides, whether americium only is transmuted. The thesis presents precisely the MUST ADS design methodology and the calculations to get a fuel composition at equilibrium. Then a one cycle evolution is performed and analysed for the fuel and the multiplication factor. Radiotoxicity and thermal power of the waste produced are then compared. Finally, the study of double strata scenarios is performed to analyse the plutonium and minor actinides inventories in cycle and also the waste produced according to the transmutation strategies applied and the first stratum evolution. (author)

Development of advanced mixed oxide fuels for plutonium management

International Nuclear Information System (INIS)

Eaton, S.; Beard, C.; Buksa, J.; Butt, D.; Chidester, K.; Havrilla, G.; Ramsey, K.

1997-01-01

A number of advanced Mixed Oxide (MOX) fuel forms are currently being investigated at Los Alamos National Laboratory that have the potential to be effective plutonium management tools. Evolutionary Mixed Oxide (EMOX) fuel is a slight perturbation on standard MOX fuel, but achieves greater plutonium destruction rates by employing a fractional nonfertile component. A pure nonfertile fuel is also being studied. Initial calculations show that the fuel can be utilized in existing light water reactors and tailored to address different plutonium management goals (i.e., stabilization or reduction of plutonium inventories residing in spent nuclear fuel). In parallel, experiments are being performed to determine the feasibility of fabrication of such fuels. Initial EMOX pellets have successfully been fabricated using weapons-grade plutonium. (author)

Development of advanced mixed oxide fuels for plutonium management

International Nuclear Information System (INIS)

Eaton, S.; Beard, C.; Buksa, J.; Butt, D.; Chidester, K.; Havrilla, G.; Ramsey, K.

1997-06-01

A number of advanced Mixed Oxide (MOX) fuel forms are currently being investigated at Los Alamos National Laboratory that have the potential to be effective plutonium management tools. Evolutionary Mixed Oxide (EMOX) fuel is a slight perturbation on standard MOX fuel, but achieves greater plutonium destruction rates by employing a fractional nonfertile component. A pure nonfertile fuel is also being studied. Initial calculations show that the fuel can be utilized in existing light water reactors and tailored to address different plutonium management goals (i.e., stabilization or reduction of plutonium inventories residing in spent nuclear fuel). In parallel, experiments are being performed to determine the feasibility of fabrication of such fuels. Initial EMOX pellets have successfully been fabricated using weapons-grade plutonium

Mixed chemical-induced oxidative stress in occupational exposure ...

African Journals Online (AJOL)

Mixed chemical-induced oxidative stress in occupational exposure in Nigerians. JI Anetor, SA Yaqub, GO Anetor, AC Nsonwu, FAA Adeniyi, S Fukushima. Abstract. Exposure to single chemicals and associated disorders in occupational environments has received significant attention. Understanding these events holds ...

Recycle of LWR [Light Water Reactor] actinides to an IFR [Integral Fast Reactor

International Nuclear Information System (INIS)

Pierce, R.D.; Ackerman, J.P.; Johnson, G.K.; Mulcahey, T.P.; Poa, D.S.

1991-01-01

A large quantity of actinide elements is present in irradiated Light Water Reactor (LWR) fuel that is stored throughout the world. Because of the high fission-to-capture ratio for the transuranium (TRU) elements with the high-energy neutrons in the metal-fueled Integral Fast Reactor (IFR), that reactor can consume these elements effectively. The stored fuel represents a valuable resource for an expanding application of fast power reactors. In addition, removal of the TRU elements from the spent LWR fuel has the potential for increasing the capacity of a high-level waste facility by reducing the heat loads and increasing the margin of safety in meeting licensing requirements. Argonne National Laboratory (ANL) is developing a pyrochemical process, which is compatible with the IFR fuel cycle, for the recovery of TRU elements from LWR fuel. The proposed product is a metallic actinide ingot, which can be introduced into the electrorefining step of the IFR process. The major objective of the LWR fuel recovery process is high TRU element recovery, with decontamination a secondary issue, because fission product removal is accomplished in the IFR process. The extensive pyrochemical processing studies of the 1960s and 1970s provide a basis for the design of possible processes. Two processes were selected for laboratory-scale investigation. One is based on the Salt Transport Process studied at ANL for mixed-oxide fast reactor fuel, and the other is based on the blanket processing studies done for ANL's second Experimental Breeder Reactor (EBR-2). This paper discusses the two processes and is a status report on the experimental studies. 5 refs., 2 figs., 2 tabs

Grain growth kinetics in uranium-plutonium mixed oxides

International Nuclear Information System (INIS)

Sari, C.

1986-01-01

Grain growth rates were investigated in uranium-plutonium mixed oxide specimens with oxygen-to-metal ratios 1.97 and 2.0. The specimens in the form of cylindrical pellets were heated in a temperature gradient similar to that existing in a fast reactor. The results are in agreement with the cubic rate law. The mean grain size D(μm) after annealing for time t (min) is represented by D 3 -D 0 3 =1.11x10 12 . exp(-445870/RT).t and D 3 -D 0 3 =2.55x10 9 .exp(-319240/RT).t for specimens with overall oxygen-to-metal ratios 1.97 and 2.0, respectively (activation energies expressed in J/mol). An example for the influence of the oxygen-to-metal ratio on the grain growth in mixed oxide fuel during operation in a fast reactor is also given. (orig.)

Reactor physics aspects of burning actinides in a nuclear reactor

International Nuclear Information System (INIS)

Hage, W.; Schmidt, E.

1978-01-01

A short review of the different recycling strategies of actinides other than fuel treated in the literature, is given along with nuclear data requirements for actinide build-up and transmutation studies. The effects of recycling actinides in a nuclear reactor on the flux distribution, the infinite neutron multiplication factor, the reactivity control system, the reactivity coefficients and the delayed neutron fraction are discussed considering a notional LWR or LMFBR as an Actinide Trasmutaton Reactor. Some operational problems of Actinide Transmutation reactors are mentioned, which are caused by the α-decay heat and the neutron sources of Actinide Target Elements

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

Science.gov (United States)

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

2012-05-01

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

Ultratrace analysis of transuranic actinides by laser-induced fluorescence

Science.gov (United States)

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.

Process for recovery of plutonium from fabrication residues of mixed fuels consisting of uranium oxide and plutonium oxide

International Nuclear Information System (INIS)

Heremanns, R.H.; Vandersteene, J.J.

1983-01-01

The invention concerns a process for recovery of plutonium from fabrication residues of mixed fuels consisting of uranium oxide and plutonium oxide in the form of PuO 2 . Mixed fuels consisting of uranium oxide and plutonium oxide are being used more and more. The plants which prepare these mixed fuels have around 5% of the total mass of fuels as fabrication residue, either as waste or scrap. In view of the high cost of plutonium, it has been attempted to recover this plutonium from the fabrication residues by a process having a purchase price lower than the price of plutonium. The problem is essentially to separate the plutonium, the uranium and the impurities. The residues are fluorinated, the UF 6 and PuF 6 obtained are separated by selective absorption of the PuF 6 on NaF at a temperature of at least 400 0 C, the complex obtained by this absorption is dissolved in nitric acid solution, the plutonium is precipitated in the form of plutonium oxalate by adding oxalic acid, and the precipitated plutonium oxalate is calcined

40 CFR 721.10006 - Mixed metal oxide (generic).

Science.gov (United States)

2010-07-01

... 40 Protection of Environment 30 2010-07-01 2010-07-01 false Mixed metal oxide (generic). 721.10006 Section 721.10006 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) TOXIC SUBSTANCES...) of this section. (2) The significant new uses are: (i) Industrial, commercial, and consumer...

Electron donating and acid-base properties of cerium oxide and its mixed oxides with alumina

International Nuclear Information System (INIS)

Sugunan, S.; Jalaja, J.M.

1994-01-01

The electron donating properties of cerium oxide activated at 300, 500 and 800 degC and of its mixed oxides with alumina were examined based on the adsorption of electron acceptors exhibiting different electron affinities. The surface acidity/basicity of the oxides was determined by titrimetry; the H 0,max values are given. The limit of electron transfer from the oxide surface lies within the region of 1.77 and 2.40 eV in terms of the electron affinity of the electron acceptor. Cerium oxide promotes the electron donor nature of alumina while leaving the limit of electron transfer unchanged. 2 tabs., 4 figs., 13 refs

Actinide isotopes in the marine environment

International Nuclear Information System (INIS)

Holm, E.; Fukai, R.

1986-01-01

Studies of actinide isotopes in the environment are important not only from the viewpoint of their radiological effects on human life, but also from the fact that they act as excellent biochemical and geochemical tracers especially in the marine environment. For several of the actinide isotopes there is still a lack of basic data on concentration levels and further investigations on their chemical and physical speciation are required to understand their behaviour in the marine environment. The measured and estimated activity concentration levels of artificial actinides are at present in general a few orders of magnitude lower than those of the natural ones and their concentration factors in biota are relatively low, except in a few species of macroalgae and phytoplankton. The contribution from seafood to total ingestion of actinides by the world population is a few per cent and, therefore, the dose to man from these long-lived radionuclides caused by seafood ingestion is usually low. (orig.)

Application of cylinder symmetry to iron and titanium oxidation by oxygen or hydrogen-water vapour mixes

International Nuclear Information System (INIS)

Raynaud, Pierre

1980-01-01

This research thesis addresses the study of the oxidation reaction in the case of corrosion of iron by oxygen, hydrogen sulphide or hydrogen-water vapour mixes, and in the case of oxidation of titanium and of titanium nitride by hydrogen-water vapour mixes. It first addresses the corrosion of iron by oxygen with an experiment performed in cylinder symmetry: description of operational conditions, discussion of kinetic curves, development of a law of generation of multiple layers in cylinder symmetry, analytical exploitation of experimental results. The second part addresses the oxidation of iron by hydrogen-water vapour mixes: experimental conditions, influence of temperature on kinetics, micrographic study (oxide morphology, coating morphology, interpretation of differences with the case of plane symmetry), discussion of the influence of cylinder symmetry on oxidation kinetics. The third part addresses the oxidation of titanium by hydrogen-water vapour mixes: global kinetic evolution, reaction products and micrographic examination, morphology and texture studies, discussion of the oxidation mechanism and of cylinder symmetry [fr

Actinide recycle in LMFBRs as a waste management alternative

International Nuclear Information System (INIS)

Beaman, S.L.

1979-01-01

A strategy of actinide burnup in fast reactor systems has been investigated as an approach for reducing the long term hazards and storage requirements of the actinide waste elements and their decay daughters. The actinide recycle studies also included plutonium burnup studies in the event that plutonium is no longer required as a fuel. Particular emphasis was placed upon the timing of the recycle program, the requirements for separability of the waste materials, and the impact of the actinides on the reactor operations and performance. It is concluded that actinide recycle and plutonium burnout are attractive alternative waste management concepts. 25 refs., 14 figs., 34 tabs

Thin layers in actinide research

International Nuclear Information System (INIS)

Gouder, T.

1998-01-01

Surface science research at the ITU is focused on the synthesis and surface spectroscopy studies of thin films of actinides and actinide compounds. The surface spectroscopies used are X-ray and ultra violet photoelectron spectroscopy (XPS and UPS, respectively), and Auger electron spectroscopy (AES). Thin films of actinide elements and compounds are prepared by sputter deposition from elemental targets. Alloy films are deposited from corresponding alloy targets and could be used, in principle, as replicates of these targets. However, there are deviations between alloy film and target composition, which depend on the deposition conditions, such as pressure and target voltage. Mastering of these effects may allow us to study stoichiometric film replicates instead of thick bulk compounds. As an example, we discuss the composition of U-Ni films prepared from a UNi 5 target. (orig.)

Rapid determination of actinides in seawater samples

International Nuclear Information System (INIS)

Maxwell, S.L.; Culligan, B.K.; Hutchison, J.B.; Utsey, R.C.; McAlister, D.R.

2014-01-01

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 used 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. (author)

Solvent-Free Selective Oxidation of Toluene with O2 Catalyzed by Metal Cation Modified LDHs and Mixed Oxides

Directory of Open Access Journals (Sweden)

Xiaoli Wang

2016-01-01

Full Text Available A series of metal cation modified layered-double hydroxides (LDHs and mixed oxides were prepared and used to be the selective oxidation of toluene with O2. The results revealed that the modified LDHs exhibited much higher catalytic performance than their parent LDH and the modified mixed oxides. Moreover, the metal cations were also found to play important roles in the catalytic performance and stabilities of modified catalysts. Under the optimal reaction conditions, the highest toluene conversion reached 8.7% with 97.5% of the selectivity to benzyldehyde; moreover, the catalytic performance remained after nine catalytic runs. In addition, the reaction probably involved a free-radical mechanism.

Different Abilities of Eight Mixed Cultures of Methane-oxidizing Bacteria to Degrade TCE

DEFF Research Database (Denmark)

Broholm, Kim; Christensen, Thomas Højlund; Jensen, Bjørn K.

1993-01-01

The ability of eight mixed cultures of methane-oxidizing bacteria to degrade trichloroethylene (TCE) was examined in laboratory batch experiments. This is one of the first reported works studying TCE degradation by mixed cultures of methane-oxidizing bacteria at 10°C, a common temperature for soils...... methanol, but only for a limited time period of about 5 days. Several explanations for the discontinued degradation of TCE are given. An experiment carried out to re-activate the methane-oxidizing bacteria after 8 days of growth on methanol by adding methane did not immediately result in degradation...... of methane and TCE. During the first 10–15 days after the addition of methane a significant degradation of methane and a minor degradation of TCE were observed. This experiment revealed that the ability of mixed cultures of methane-oxidizing bacteria to degrade TCE varied significantly even though...

Radiochemistry and actinide chemistry

International Nuclear Information System (INIS)

Guillaumont, R.; Peneloux, A.

1989-01-01

The analysis of trace amounts of actinide elements by means of radiochemistry, is discussed. The similarities between radiochemistry and actinide chemistry, in the case of species amount by cubic cm below 10 12 , are explained. The parameters which allow to define what are the observable chemical reactions, are given. The classification of radionuclides in micro or macrocomponents is considered. The validity of the mass action law and the partition function in the definition of the average number of species for trace amounts, is investigated. Examples illustrating the results are given

Interaction between actinides and protein: the calmodulin

International Nuclear Information System (INIS)

Brulfert, Florian

2016-01-01

Considering the environmental impact of the Fukushima nuclear accident, it is fundamental to study the mechanisms governing the effects of the released radionuclides on the biosphere and thus identify the molecular processes generating the transport and deposition of actinides, such as neptunium and uranium. However, the information about the microscopic aspect of the interaction between actinides and biological molecules (peptides, proteins...) is scarce. The data being mostly reported from a physiological point of view, the structure of the coordination sites remains largely unknown. These microscopic data are indeed essential for the understanding of the interdependency between structural aspect, function and affinity.The Calmodulin (CaM) (abbreviation for Calcium-Modulated protein), also known for its affinity towards actinides, acts as a metabolic regulator of calcium. This protein is a Ca carrier, which is present ubiquitously in the human body, may also bind other metals such as actinides. Thus, in case of a contamination, actinides that bind to CaM could avoid the protein to perform properly and lead to repercussions on a large range of vital functions.The complexation of Np and U was studied by EXAFS spectroscopy which showed that actinides were incorporated in a calcium coordination site. Once the thermodynamical and structural aspects studied, the impact of the coordination site distortion on the biological efficiency was analyzed. In order to evaluate these consequences, a calorimetric method based on enzyme kinetics was developed. This experiment, which was conducted with both uranium (50 - 500 nM) and neptunium (30 - 250 nM) showed a decrease of the heat produced by the enzymatic reaction with an increasing concentration of actinides in the medium. Our findings showed that the Calmodulin actinide complex works as an enzymatic inhibitor. Furthermore, at higher neptunium (250 nM) and uranium (500 nM) concentration the metals seem to have a poison

On the hazard accumulation of actinide waste in a Pu-fueled LMFBR power economy with and without by-product actinide recycling

International Nuclear Information System (INIS)

Anselmi, L.; Caruso, K.; Hage, W.; Schmidt, E.

1979-01-01

The actinide waste arisings in terms of hazard potential for ingestion and inhalation are given for a Pu-fueled LMFBR Power Economy as function of decay time. The data were assessed for two simplified fuel cycles, one considering the recycling of by-product actinides and the other their complete discharge to the high-level waste. Two durations of nuclear power and several loss fractions of actinides to the waste were considered. The major contributors in form of chemical elements or isotopes to the actinide waste hazard built up during the nuclear power duration were identified for various decay intervals

Transmutation of minor actinides in a Candu thorium borner

International Nuclear Information System (INIS)

Sahin, S.; Sahin, H. M.; Acir, A.; Yalcin, S.; Yildiz, K.; Sahin, N.; Altinok, T.; Alkan, M.

2007-01-01

latter is used for denaturized the new 2 33U fuel with 2 38U. The temporal variation of the criticality k ∞ and the burn-up values of the reactor have been calculated by full power operation for a period of 20 years. The criticality starts by k ∞ = ∼ 1.48 for both fuel compositions. A sharp decrease of the criticality has been observed in the first year as a consequence of rapid plutonium burnout. The criticality becomes quasi constant after the 2nd year and remains above k ∞ > 1.06 for ∼ 20 years. After the 2nd year, the CANDU reactor begins to operate practically as a thorium burner. Nuclear waste actinides can also be used as a booster fissile fuel material in form of mixed fuel with thorium in a CANDU reactor in order to assure the initial criticality at startup. In the third phase, two different fuel compositions have been found useful to provide sufficient reactor criticality over a long operation period: 1) 95% thoria (ThO 2 ) + 5% minor actinides MAO 2 and 2) 95% ThO 2 + 5% MAO 2 + 5% UO 2 . The latter allows a higher degree of nuclear safeguarding thorough denaturing the new 2 33U fuel with 2 38U. The temporal variation of the criticality k ∞ and the burn-up values of the reactor have been calculated by full power operation for a period of 10 years. The criticality starts by k ∞ > 1.3 for both fuel compositions. A sharp decrease of the criticality has been observed in the first year as a consequence of rapid plutonium burnout in the actinide fuel. The criticality becomes quasi constant after the 2nd year and remains close to k ∞ =∼1.06 for ∼ 10 years. After the 2nd year, the CANDU reactor begins to operate practically as a thorium burner. Finally, in the fourth phase, a CANDU reactor fueled with a mixed fuel made of thoria (ThO 2 ) and the totality of nuclear waste actinides has been investigated. The mixed fuel composition has been varied in radial direction to achieve a uniform power distribution and fuel burn up in the fuel bundle. The

Cathodic electrodeposition of mixed molybdenum tungsten oxides from peroxo-polymolybdotungstate solutions.

Science.gov (United States)

Kondrachova, Lilia; Hahn, Benjamin P; Vijayaraghavan, Ganesh; Williams, Ryan D; Stevenson, Keith J

2006-12-05

Mixed molybdenum tungsten trioxide films of varying stoichiometry (MoxW1 - xO3, 0 cathodic electrodeposition on indium tin oxide (ITO)-coated glass substrates from aqueous peroxo-polymolybdotungstate solutions. Electrochemical quartz crystal microbalance (EQCM), cyclic voltammetry, and chronocoulometry were used to gain insight into the electrodeposition mechanism. The compositional and structural properties were characterized for MoxW1 - xO3 films deposited at intermediate potentials (-0.35 V vs Ag/AgCl) and sintered at 250 degrees C using energy-dispersive spectroscopy, X-ray diffraction, and Raman spectroscopy. These studies reveal that films consist of homogeneously mixed MoxW1 - xO3, with an enriched Mo content ranging in composition from 0.4 < x < 0.7 depending upon the mol % Mo present in the deposition solution. Chronoamperometry and spectroelectrochemical measurements were conducted to estimate lithium ion diffusion coefficients and coloration efficiencies for the mixed metal oxide films in 1 M LiClO4/propylene carbonate. The subtle interplay between structural and compositional properties due to the uniform mixing of Mo and W oxide components shows that electrochromic and lithium ion transport properties are moderately enhanced relative to those of single-component WO3 and MoO3 and demonstrate improved structural stability over pure MoO3 polymorphs during electrochemical cycling.

Correlation of retention of lanthanide and actinide complexes with stability constants and their speciation

Energy Technology Data Exchange (ETDEWEB)

Datta, A.; Sivaraman, N.; Viswanathan, K.S.; Ghosh, Suddhasattwa; Srinivasan, T.G.; Vasudeva Rao, P.R. [Indira Gandhi Centre for Atomic Research, Kalpakkam (India). Chemistry Group

2013-03-01

The present study describes a correlation that is developed from retention of lanthanide and actinide complexes with the stability constant. In these studies, an ion-pairing reagent, camphor-10-sulphonic acid (CSA) was used as the modifier and organic acids such as {alpha}-hydroxy isobutyric acid ({alpha}-HIBA), mandelic acid, lactic acid and tartaric acid were used as complexing reagent for elution. From these studies, a correlation has been established between capacity factor of a metal ion, concentration of ion-pairing reagent and complexing agent with the stability constant of metal complex. Based on these studies, it has been shown that the stability constant of lanthanide and actinide complexes can be estimated using a single lanthanide calibrant. Validation of the method was carried out with the complexing agents such as {alpha}-HIBA and lactic acid. It was also demonstrated that data from a single chromatogram can be used for estimation of stability constant at various ionic strengths. These studies also demonstrated that the method can be applied for estimation of stability constant of actinides with a ligand whose value is not reported yet, e.g., ligands of importance in the lanthanide-actinide separations, chelation therapy etc. The chromatographic separation method is fast and the estimation of stability constant can be done in a very short time, which is a significant advantage especially in dealing with radioactive elements. The stability constant data was used to derive speciation data of plutonium in different oxidation states as well as that of americium with {alpha}-HIBA. The elution behavior of actinides such as Pu and Am from reversed phase chromatographic technique could be explained based on these studies. (orig.)

Actinide recovery from pyrochemical residues

International Nuclear Information System (INIS)

Avens, L.R.; Clifton, D.G.; Vigil, A.R.

1984-01-01

A new process for recovery of plutonium and americium from pyrochemical waste has been demonstrated. It is based on chloride solution anion exchange at low acidity, which eliminates corrosive HCl fumes. Developmental experiments of the process flowsheet concentrated on molten salt extraction (MSE) residues and gave >95% plutonium and >90% americium recovery. The recovered plutonium contained 6 = from high chloride-low acid solution. Americium and other metals are washed from the ion exchange column with 1N HNO 3 -4.8M NaCl. The plutonium is recovered, after elution, via hydroxide precipitation, while the americium is recovered via NaHCO 3 precipitation. All filtrates from the process are discardable as low-level contaminated waste. Production-scale experiments are now in progress for MSE residues. Flow sheets for actinide recovery from electrorefining and direct oxide reduction residues are presented and discussed

Actinide recovery from pyrochemical residues

International Nuclear Information System (INIS)

Avens, L.R.; Clifton, D.G.; Vigil, A.R.

1985-05-01

We demonstrated a new process for recovering plutonium and americium from pyrochemical waste. The method is based on chloride solution anion exchange at low acidity, or acidity that eliminates corrosive HCl fumes. Developmental experiments of the process flow chart concentrated on molten salt extraction (MSE) residues and gave >95% plutonium and >90% americium recovery. The recovered plutonium contained 6 2- from high-chloride low-acid solution. Americium and other metals are washed from the ion exchange column with lN HNO 3 -4.8M NaCl. After elution, plutonium is recovered by hydroxide precipitation, and americium is recovered by NaHCO 3 precipitation. All filtrates from the process can be discardable as low-level contaminated waste. Production-scale experiments are in progress for MSE residues. Flow charts for actinide recovery from electro-refining and direct oxide reduction residues are presented and discussed

Structural characterization of the Actinides (III) and (IV) - DOTA complexes

International Nuclear Information System (INIS)

Audras, Matthieu

2014-01-01

The polyamino-carboxylate anions have been identified as compounds of interest in the operations of actinide separation, in actinide migration in the environment and in human radio-toxicology. The structural characterization of complexes formed between actinides and polyamino-carboxylates ligands is essential for a better understanding of actinide-ligands interactions. Among the polyamino-carboxylate anions, the DOTA ligand (1,4,7,10-tetraaza-cyclododecane tetraacetic acid) is described as a very strong complexing agent of the lanthanides(III), but has been little studied with actinides. The objective of this thesis is to describe the complexes formed between the actinides (III) and (IV) and the DOTA ligand, and compare them with the lanthanide complexes. For this, an approach has been introduced to characterize the complexes by complementary analytical techniques (spectrophotometry, electro-spray ionization mass spectrometry, NMR, EXAFS, electrochemistry), but also by calculations of theoretical chemistry to help the interpretation of the experimental data. The formation of a 1:1 complex is observed with the actinides(III) (plutonium and americium) as for lanthanides(III): rapid formation of intermediate species which evolves slowly towards the formation of a limit complex. Within this complex, the cation is located inside the cavity formed by the ligand. Four nitrogen atoms and four oxygen atoms from the carboxylate functions are involved in the coordination sphere of the cation. However, differences were observed in the bond lengths formed between the cation and the nitrogen atoms (the bonds are somewhat shorter in the case of actinide complexes) as well as the complexation kinetics, which is slightly faster for the actinides(III) than for lanthanide(III) ions of equivalent radius. The same behavior was observed in solution upon complexation of actinides(IV) (uranium, plutonium and neptunium): slow formation of a 1:1 complex (actinide(IV):ligand) in wherein the

Calculated investigation of actinide transmutation in the BOR-60 reactor

International Nuclear Information System (INIS)

Zhemkov, I.Yu.; Ishunina, O.V.; Yakovleva, I.V.

2000-01-01

One of the prospective actinide burner reactor type is the fast reactor with a 'hard' spectrum and small breeding factor, which is the BOR-60. The calculated investigations demonstrate that Loading up to 40% of minor-actinides to the BOR-60 reactor did not lead to the considerable change of neutron-physical characteristics. The performed calculations show that the BOR- 60 reactor possesses a high efficiency of the minor-actinide and plutonium bum-up (up to 37 kg/(TW · h)) hat is comparable with properties of the actinide burner-reactors under design. The BOR-60 reactor can provide a homogeneous minor-actinide Loading (minor-actinide addition to the standard fuel) to the core and heterogeneous Loading (as separate assemblies-targets with a high minor-actinide fraction) to the first rows of a radial blanket that allows the optimum usage of the reactor and its characteristics. (authors)

Dynamics and Thermochemistry of Oxygen Uptake by a Mixed Ce-Pr Oxide

Science.gov (United States)

Sinev, M. Yu.; Fattakhova, Z. T.; Bychkov, V. Yu.; Lomonosov, V. I.; Gordienko, Yu. A.

2018-03-01

The dynamics of oxygen uptake by mixed Ce0.55Pr0.45O2-x oxide is studied in a pulsed oxygen supply mode using in situ high-temperature heat flow differential scanning calorimetry. It is stated that the oxidation proceeds in two regimes: a fast one at the beginning of the oxidation process, and a slow one, which is controlled by the diffusion of oxygen through the bulk of the solid at the later stages of the process. Analysis of the shape of calorimetric profiles reveals some processes, accompanied by heat release, that occur in the sample in the absence of oxygen in the gas phase. These could be due to both the redistribution of consumed oxygen in the oxide lattice and the lattice relaxation associated with the transformation of phases with different arrangements of oxygen vacancies in them. The heat effect (which diminishes from 60 to 40 kJ/mol in the course of oxygen uptake) associated with the oxidation of the reduced form of mixed Ce-Pr oxide, corresponds to the oxidation of praseodymium ions from (3+) to (4+).

Actinide removal from aqueous solution with activated magnetite

International Nuclear Information System (INIS)

Kochen, R.L.; Thomas, R.L.

1987-01-01

An actinide aqueous waste treatment process using activated magnetite has been developed at Rocky Flats. The use and effectiveness of various magnetites in lowering actinide concentrations in aqueous solution are described. Experiments indicate that magnetite particle size and pretreatment (activation of the magnetite surface with hydroxyl ions greatly influence the effective use of magnetite as an actinide adsorbent. With respect to actinide removal, Ba(OH) 2 -activated magnetite was more effective over a broader pH range than was NaOH-activated magnetite. About 50% less Ba(OH) 2 -activated magnetite was required to lower plutonium concentration from 10 -4 to 10 -8 g/l. 7 refs., 8 tabs

Formation of actinides in irradiated HTGR fuel elements

Energy Technology Data Exchange (ETDEWEB)

dos Santos, A. M.

1976-03-15

Actinide nuclide concentrations of 11 spent AVR fuel elements were determined experimentally. The burnup of the spheres varied in the range between 10% and 100% fifa, the Th : U ratio was 5 : 1. The separation procedures for an actinide isolation were tested with highly irradiated ThO/sub 2/. Separation and decontamination factors are presented. Build-up of /sup 232/U was discussed. The AVR breeding rate was ascertained to be 0.5. The hazard potential of high activity waste was calculated. Actinide recovery factors were proposed in order to reduce the hazard potential of the waste by an actinide removal under consideration of the reprocessing technology which is available presently.

Ground-state electronic structure of actinide monocarbides and mononitrides

DEFF Research Database (Denmark)

Petit, Leon; Svane, Axel; Szotek, Z.

2009-01-01

The self-interaction corrected local spin-density approximation is used to investigate the ground-state valency configuration of the actinide ions in the actinide monocarbides, AC (A=U,Np,Pu,Am,Cm), and the actinide mononitrides, AN. The electronic structure is characterized by a gradually increa...

Insertion compounds of transition-metal and uranium oxides

International Nuclear Information System (INIS)

Chippindale, A.M.; Dickens, P.G.; Powell, A.V.

1991-01-01

Several transition-metal and actinide oxides, in which the metal occurs in a high oxidation state, have open covalent structures and are capable of incorporating alkali and other electropositive metals under mild conditions to form insertion compounds A x MO n . These are solids which have several features in common: Over a range of compositions, A x MO n exists as one or more stable or metastable phases in which the structure of the parent oxide MO n is largely retained and the insertion element A is accommodated interstitially. Insertion is accompanied by a redox process A=A i . + e - M in which M is reduced and the electronic properties of the parent oxide change to those typical of a mixed-valence compound. The insertion process xA + MO n = A x MO n can be reversed, at least to some extent, by chemical or electrochemical reaction, with retention of structure (topotactic reaction). This review concentrates on methods of synthesis, characterisation, crystal structure and thermochemistry of these insertion compounds. It updates and extends previous work. (author)

A catalytic wet oxidation process for mixed waste volume reduction/recycling

International Nuclear Information System (INIS)

Dhooge, Patrick M.

1992-01-01

Mixed wastes have presented a challenge to treatment and destruction technologies. A recently developed catalytic wet oxidation method has promising characteristics for volume reduction and recycling of mixed wastes. The process utilizes iron (III) as an oxidant in the presence of homogeneous cocatalysts which increase organics' oxidation rates and the rate of oxidation of iron (II) by oxygen. The reaction is conducted in an aqueous mineral acid solution at temperatures of 373 - 573 deg K. The mineral acid should solvate a number of heavy metals, including U and Pu. Studies of reaction rates show that the process can oxidize a wide range of organic compounds including aromatics and chlorinated hydrocarbons. Rate constants in the range of 10 -7 to 10 -4 sec -1 , depending on the cocatalyst, acidity, type of anions, type of organic, temperature, and time. Activation energies ranged from 25. to 32. KJ/mole. Preliminary measurements of the extent of oxidation which could be obtained ranged from 80% for trichloroethylene to 99.8% for 1,2,4-trimethylbenzene; evidence was obtained that absorption by the fluorocarbon liners of the reaction bombs allowed some of the organics to escape exposure to the catalyst solution. The results indicate that complete oxidation of the organics used here, and presumably many others, can be achieved. (author)

Fabrication experience with mixed-oxide LWR fuels at the BELGONUCLEAIRE plant

International Nuclear Information System (INIS)

Vanhellemont, G.

1979-01-01

For nearly 20 years BELGONUCLEAIRE has been involved in a steadily growing effort to increase its production of mixed oxides. This programme has ranged from basic research and process development through a pilot-scale unit to today's mixed-oxide fuel fabrication plant at Dessel, which has been in operation for just over 5 years. The reference fabrication flow sheet includes UO 2 , PuO 2 and a scraped powder preparation, sintered ground pellets as well as rod fabrication and assembling. With regard to quality, attention is especially paid to the process monitoring and quality controls at the qualification step and during the routine production. Entirely different types of thermal UO 2 -PuO 2 fuel pellets, rods and assemblies have been manufactured for PWR and BWR operation. For these fabrications, some diagrams of the results with regard to the required technical specifications are presented. Special emphasis is placed on the occasional deviations of some finished products from the specifications and on the solutions applied to avoid such problems. Concerning the actual capacity of the mixed-oxide fuel fabrication plant, several limiting factors due to the nature of plutonium itself are discussed. Taking into account all these ambient limitations, a reference PWR mixed-oxide fuel output of nominally 18 t/a is obtained. The industrial feasibility of UO 2 -PuO 2 fuel fabrication has been thoroughly demonstrated by the present BELGONUCLEAIRE plant. The experience obtained has led to progressive improvements of the fabrication process and adaptation of the product controls in order to ensure the requested quality levels. (author)

Ni–Ta–O mixed oxide catalysts for the low temperature oxidative dehydrogenation of ethane to ethylene

KAUST Repository

Zhu, Haibo

2015-09-01

The "wet" sol-gel and "dry" solid-state methods were used to prepare Ni-Ta-O mixed oxide catalysts. The resulting Ni-Ta oxides exhibit high activity and selectivity for the low temperature oxidative dehydrogenation of ethane to ethylene. The Ta/(Ni + Ta) atomic ratios (varying from 0 to 0.11 in "wet" sol-gel method, and from 0 to 0.20 in "dry" solid-state method) as well as the preparation methods used in the synthesis, play important roles in controlling catalyst structure, activity, selectivity and stability in the oxidative dehydrogenation of ethane. Electron microscopy characterizations (TEM, EELS mapping, and HAADF-STEM) clearly demonstrate that the Ta atoms are inserted into NiO crystal lattice, resulting in the formation of a new Ni-Ta oxide solid solution. More Ta atoms are found to be located at the lattice sites of crystal surface in sol-gel catalyst. While, a small amount of thin layer of Ta2O5 clusters are detected in solid-state catalyst. Further characterization by XRD, N2 adsorption, SEM, H2-TPR, XPS, and Raman techniques reveal different properties of these two Ni-Ta oxides. Due to the different properties of the Ni-Ta oxide catalysts prepared by two distinct approaches, they exhibit different catalytic behaviors in the ethane oxidative dehydrogenation reaction at low temperature. Thus, the catalytic performance of Ni-Ta-O mixed oxide catalysts can be systematically modified and tuned by selecting a suitable synthesis method, and then varying the Ta content. ©2015 Elsevier Inc. All rights reserved.

Role of bacteria as biocolloids in the transport of actinides from a deep underground radioactive waste repository

International Nuclear Information System (INIS)

Francis, A.J.; Gillow, J.B.; Dodge, C.J.; Dunn, M.; Mantione, K.; Strietelmeier, B.A.; Pansoy-Hjelvik, M.E.; Papenguth, H.W.

1998-01-01

We investigated the interaction of dissolved actinides 232 Th, 238 U, 237 Np, 239 Pu, and 243 Am, with a pure and a mixed culture of halophilic bacteria isolated from the waste isolation pilot plant repository under anaerobic conditions to evaluate their potential transport as biocolloids from the waste site. The sizes of the bacterial cells studied ranged from 0.54 x 0.48 μm to 7.7 x 0.67 μm (1 x w). Using sequential microfiltration, we determined the association of actinides with free-living (mobile) bacterial cells suspended in a fluid medium containing NaCl or MgCl 2 brine, at various phases of their growth cycles. The number of suspended bacteria ranged from 10 6 to 10 9 cells ml -1 . The amount of actinide associated with the suspended cell fraction (calculated as mol cell -1 ) was very low: Th, 10 -12 ; U, 10 -15 -10 -18 ; Np, 10 -15 -10 -19 ; Pu, 10 -18 -10 -21 ; and Am, 10 -18 -10 -19 ; and it varied with the bacterial culture studied. The differences in the association are attributed to the extent of bioaccumulation and biosorption by the bacteria, pH, the composition of the brine, and the speciation and bioavailability of the actinides. (orig.)

Sol-gel chemistry applied to the synthesis of polymetallic oxides including actinides reactivity and structure from solution to solid state; Synthese par voie douce d'oxydes polymetalliques incluant des actinides: reactivite et structure de la solution au solide

Energy Technology Data Exchange (ETDEWEB)

Lemonnier, St

2006-02-15

Minor actinides transmutation is studied at present in order to reduce the radiotoxicity of nuclear waste and the assessment of its technical feasibility requires specific designed materials. When considering americium, yttria stabilized zirconia (Am{sup III} YII Zriv)Or{sub x} is among the ceramic phases that one which presents the required physico-chemical properties. An innovative synthesis of this mixed oxide by sol-gel process is reported in this manuscript. The main aim of this work is to adjust the reactivity of the different metallic cations in aqueous media using complexing agent, in order to initiate a favourable interaction for a homogeneous elements repartition in the forming solid phase. The originality of the settled synthesis lies on an in-situ formation of a stable and monodisperse nano-particles dispersion in the presence of acetylacetone. The main reaction mechanisms have been identified: the sol stabilisation results from an original interaction between the three compounds (Zrly, trivalent cations and acetylacetone). The sol corresponds to a structured system at the nanometer scale for which zirconium and trivalent cations are homogeneously dispersed, preliminary to the sol-gel transition. Furthermore, preliminary studies were carried out with a view to developing materials. They have demonstrated that numerous innovative and potential applications can be developed by taking advantage of the direct and controlled formation of the sol and by adapting the sol-gel transition. The most illustrating result is the preparation of a sintered pellet with the composition Am0,13Zro,73Yo,0901,89 using this approach. (author)

Heterogeneous Partial (ammOxidation and Oxidative Dehydrogenation Catalysis on Mixed Metal Oxides

Directory of Open Access Journals (Sweden)

Jacques C. Védrine

2016-01-01

Full Text Available This paper presents an overview of heterogeneous partial (ammoxidation and oxidative dehydrogenation (ODH of hydrocarbons. The review has been voluntarily restricted to metal oxide-type catalysts, as the partial oxidation field is very broad and the number of catalysts is quite high. The main factors of solid catalysts for such reactions, designated by Grasselli as the “seven pillars”, and playing a determining role in catalytic properties, are considered to be, namely: isolation of active sites (known to be composed of ensembles of atoms, Me–O bond strength, crystalline structure, redox features, phase cooperation, multi-functionality and the nature of the surface oxygen species. Other important features and physical and chemical properties of solid catalysts, more or less related to the seven pillars, are also emphasized, including reaction sensitivity to metal oxide structure, epitaxial contact between an active phase and a second phase or its support, synergy effect between several phases, acid-base aspects, electron transfer ability, catalyst preparation and activation and reaction atmospheres, etc. Some examples are presented to illustrate the importance of these key factors. They include light alkanes (C1–C4 oxidation, ethane oxidation to ethylene and acetic acid on MoVTe(SbNb-O and Nb doped NiO, propene oxidation to acrolein on BiMoCoFe-O systems, propane (ammoxidation to (acrylonitrile acrylic acid on MoVTe(SbNb-O mixed oxides, butane oxidation to maleic anhydride on VPO: (VO2P2O7-based catalyst, and isobutyric acid ODH to methacrylic acid on Fe hydroxyl phosphates. It is shown that active sites are composed of ensembles of atoms whose size and chemical composition depend on the reactants to be transformed (their chemical and size features and the reaction mechanism, often of Mars and van Krevelen type. An important aspect is the fact that surface composition and surface crystalline structure vary with reaction on stream until

Neutron nuclear data evaluation for actinide nucleic

International Nuclear Information System (INIS)

Chen Guochang; Yu Baosheng; Duan Junfeng; Ge Zhigang; Cao Wentian; Tang Guoyou; Shi Zhaomin; Zou Yubin

2010-01-01

The nuclear data with high accuracy for minor actinides are playing an important role in nuclear technology applications, including reactor design and operation, fuel cycle concepts, estimation of the amount of minor actinides in high burn-up reactors and the minor actinides transmutation. Through describe the class of nuclear data and nuclear date library, and introduce the procedure of neutron nuclear data evaluation. 234 U(n, f) and 237 Np(n, 2n) reaction experimental data evaluation was evaluated. The fission nuclear data are updated and improved. (authors)

Feasibility studies of actinide recycle in LMFBRs as a waste management alternative

International Nuclear Information System (INIS)

Beaman, S.L.; Aitken, E.A.

1976-01-01

A strategy of actinide burnup in LMFBRs is being investigated as a waste management alternative to long term storage of high level nuclear waste. This strategy is being evaluated because many of the actinides in the waste from spent-fuel reprocessing have half-lives of thousands of years and an alternative to geological storage may be desired. From a radiological viewpoint, the actinides and their daughters dominate the waste hazard for decay times beyond about 400 years. Actinide burnup in LMFBRs may be an attractive alternative to geological storage because the actinides can be effectively transmuted to fission products which have significantly shorter half-lives. Actinide burnup in LMFBRs rather than LWRs is preferred because the ratio of fission reaction rate to capture reaction rate for the actinides is higher in an LMFBR, and an LMFBR is not so sensitive to the addition of the actinide isotopes. An actinide target assembly recycle scheme is evaluated to determine the effects of the actinides on the LMFBR performance, including local power peaking, breeding ratio, and fissile material requirements. Several schemes are evaluated to identify any major problems associated with reprocessing and fabrication of recycle actinide-containing assemblies. The overall efficiency of actinide burnout in LMFBRs is evaluated, and equilibrium cycle conditions are determined. It is concluded that actinide recycle in LMFBRs offers an attractive alternative to long term storage of the actinides, and does not significantly affect the performance of the host LMFBR. Assuming a 0.1 percent or less actinide loss during reprocessing, a 0.1 percent loss of less during fabrication, and proper recycle schemes, virtually all of the actinides produced by a fission reactor economy could be transmuted in fast reactors

Room temperature electrodeposition of actinides from ionic solutions

Science.gov (United States)

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

2017-04-25

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

Flexible Electronics Powered by Mixed Metal Oxide Thin Film Transistors

Science.gov (United States)

Marrs, Michael

A low temperature amorphous oxide thin film transistor (TFT) and amorphous silicon PIN diode backplane technology for large area flexible digital x-ray detectors has been developed to create 7.9-in. diagonal backplanes. The critical steps in the evolution of the backplane process include the qualification and optimization of the low temperature (200 °C) metal oxide TFT and a-Si PIN photodiode process, the stability of the devices under forward and reverse bias stress, the transfer of the process to flexible plastic substrates, and the fabrication and assembly of the flexible detectors. Mixed oxide semiconductor TFTs on flexible plastic substrates suffer from performance and stability issues related to the maximum processing temperature limitation of the polymer. A novel device architecture based upon a dual active layer improves both the performance and stability. Devices are directly fabricated below 200 ºC on a polyethylene naphthalate (PEN) substrate using mixed metal oxides of either zinc indium oxide (ZIO) or indium gallium zinc oxide (IGZO) as the active semiconductor. The dual active layer architecture allows for adjustment to the saturation mobility and threshold voltage stability without the requirement of high temperature annealing, which is not compatible with flexible plastic substrates like PEN. The device performance and stability is strongly dependent upon the composition of the mixed metal oxide; this dependency provides a simple route to improving the threshold voltage stability and drive performance. By switching from a single to a dual active layer, the saturation mobility increases from 1.2 cm2/V-s to 18.0 cm2/V-s, while the rate of the threshold voltage shift decreases by an order of magnitude. This approach could assist in enabling the production of devices on flexible substrates using amorphous oxide semiconductors. Low temperature (200°C) processed amorphous silicon photodiodes were developed successfully by balancing the tradeoffs

Role of Cu-Mg-Al mixed oxide catalysts in lignin depolymerization in supercritical ethanol

NARCIS (Netherlands)

Huang, X.; Ceylanpinar, A.; Koranyi, T.I.; Boot, M.D.; Hensen, E.J.M.

2015-01-01

We investigate the role of Cu-Mg-Al mixed oxides in depolymerization of soda lignin in supercritical ethanol. A series of mixed oxides with varying Cu content and (Cu+Mg)/Al ratio were prepared. The optimum catalyst containing 20 wt% Cu and having a (Cu+Mg)/Al ratio of 4 yielded 36 wt% monomers

Actinide Solubility and Speciation in the WIPP [PowerPoint

International Nuclear Information System (INIS)

Reed, Donald T.

2015-01-01

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 repository 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.

Actinide Solubility and Speciation in the WIPP [PowerPoint

Energy Technology Data Exchange (ETDEWEB)

Reed, Donald T. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

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 repository 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.

Band structure studies of actinide systems

International Nuclear Information System (INIS)

Koelling, D.D.

1976-01-01

The nature of the f-orbitals in an actinide system plays a crucial role in determining the electronic properties. It has long been realized that when the actinide separation is small enough for the f-orbitals to interact directly, the system will exhibit itinerant electron properties: an absence of local moment due to the f-orbitals and sometimes even superconductivity. However, a number of systems with the larger actinide separation that should imply local moment behavior also exhibit intinerant properties. Such systems (URh 3 , UIr 3 , UGe 3 , UC) were examined to learn something about the other f-interactions. A preliminary observation made is that there is apparently a very large and ansiotropic mass enhancement in these systems. There is very good reason to believe that this is not solely due to large electron--electron correlations but to a large electron--phonon interaction as well. These features of the ''non-magnetic'', large actinide separation systems are discussed in light of our results to date. Finally, the results of some recent molecular calculations on actinide hexafluorides are used to illustrate the shielding effects on the intra-atomic Coulomb term U/sub f-f/ which would appear in any attempt to study the formation of local moments. As one becomes interested in materials for which a band structure is no longer an adequate model, this screened U/sub ff/ is the significant parameter and efforts must be made to evaluate it in solid state systems

Isotopic mixing in carbon monoxide catalyzed by zinc oxide

International Nuclear Information System (INIS)

Carnisio, G.; Garbassi, F.; Petrini, G.; Parravano, G.

1978-01-01

The rate of the isotopic mixing in CO has been studied at 300 0 C, for CO partial pressures from 6 to 100 Torr and a total pressure of 250 Torr on ZnO catalysts. Significant deviations from a first-order rate in p/sub co/ were found. The rate of oxygen exchange between ZnO and gas-phase CO was also measured and the results were employed to calculate the fraction of surface sites active for the CO isotopic mixing. Values on the order of 0.001 were found. The turnover rate and surface collision efficiency varied between 0.7 and 107 min -1 and 0.13 and 2.24 x 10 -8 , respectively. H 2 additions to CO increased the rate of isotopic mixing, whereas the rate of H 2 + D 2 was decreased by the presence of CO. The H 2 + D 2 rate was faster than that of isotopic mixing in CO, but as the ratio p/sub H 2 //p/sub co/ decreased the rates became about equal. It is argued that on ZnO samples, in which the rate of CO isotopic mixing and the rate of ZnO--CO oxygen exchange were influenced in a similar manner by the CO pressure, the isotopic mixing in CO took place via the ZnO oxygen, while oxide oxygen participation was not kinetically significant for ZnO samples in which the two reactions had different kinetics. The crucial factor controlling the path followed by the isotopic mixing in CO seems to be the surface Zn/O ratio, since a close correlation was found between the former and the reaction kinetics of the CO isotopic mixing reaction. Solid-state conditions which may vary the Zn/O surface ratio (foreign additions) are indicated. The implications of these findings to the problem of product selectivity from CO-H 2 mixtures reacting on metal oxide surfaces are discussed

Properties of minor actinide nitrides

International Nuclear Information System (INIS)

Takano, Masahide; Itoh, Akinori; Akabori, Mitsuo; Arai, Yasuo; Minato, Kazuo

2004-01-01

The present status of the research on properties of minor actinide nitrides for the development of an advanced nuclear fuel cycle based on nitride fuel and pyrochemical reprocessing is described. Some thermal stabilities of Am-based nitrides such as AmN and (Am, Zr)N were mainly investigated. Stabilization effect of ZrN was cleary confirmed for the vaporization and hydrolytic behaviors. New experimental equipments for measuring thermal properties of minor actinide nitrides were also introduced. (author)

Critical experiments with mixed oxide fuel

International Nuclear Information System (INIS)

Harris, D.R.

1997-01-01

This paper very briefly outlines technical considerations in performing critical experiments on weapons-grade plutonium mixed oxide fuel assemblies. The experiments proposed would use weapons-grade plutonium and Er 2 O 3 at various dissolved boron levels, and for specific fuel assemblies such as the ABBCE fuel assembly with five large water holes. Technical considerations described include the core, the measurements, safety, security, radiological matters, and licensing. It is concluded that the experiments are feasible at the Rensselaer Polytechnic Institute Reactor Critical Facility. 9 refs

ALMR potential for actinide consumption

International Nuclear Information System (INIS)

Cockey, C.L.; Thompson, M.L.

1992-01-01

The Advanced Liquid Metal Reactor (ALMR) is a US Department of Energy (DOE) sponsored fast reactor design based on the Power Reactor, Innovative Small Module (PRISM) concept originated by General Electric. This reactor combines a high degree of passive safety characteristics with a high level of modularity and factory fabrication to achieve attractive economics. The current reference design is a 471 MWt modular reactor fueled with ternary metal fuel. This paper discusses actinide transmutation core designs that fit the design envelope of the ALMR and utilize spent LWR fuel as startup material and for makeup. Actinide transmutation may be accomplished in the ALMR core by using either a breeding or burning configuration. Lifetime actinide mass consumption is calculated as well as changes in consumption behavior throughout the lifetime of the reactor. Impacts on system operational and safety performance are evaluated in a preliminary fashion. Waste disposal impacts are discussed. (author)

Synthesis and evaluation structure/extracting and complexing properties of new bi-topic ligands for group actinides extraction

International Nuclear Information System (INIS)

Bisson, J.

2011-01-01

The aim of this project is to design and study new extractants for spent nuclear fuel reprocessing. To decrease the long-term radiotoxicity of the waste, the GANEX process is an option to homogeneously recycle actinides. All actinides (U, Np, Pu, Am, Cm) would be extracted together from a highly acidic media and separated from fission products (especially from lanthanides). In this context, fourteen new bi-topic ligands constituted of a nitrogen poly-aromatic unit from the dipyridyl-phenanthroline and dipyridyl-1,3,5-triazine families and functionalized by amid groups were synthesized. Extraction studies performed with some of these ligands confirmed their interest to selectively separate actinides at different oxidation states from an aqueous solution 3M HNO 3 . To determine the influence of ligands structure on cation complexation, a study in a homogenous media (MeOH/H 2 O) has been carried out. Electro-spray ionization mass spectrometry have been used to characterize the complexes stoichiometries formed with several cations (Eu 3+ , Nd 3+ , Am 3+ , Pu 4+ and NpO 2 + ). Stability constants, evaluated by UV-Visible spectrophotometry, confirm the selectivity of these ligands toward actinides. Lanthanides and actinides complexes have also been characterized in the solid state by infra-red spectroscopy and X-Ray diffraction. Associated to nuclear magnetic resonance experiments and DFT calculations (Density Functional Theory), a better knowledge of their coordination mode was achieved. (author) [fr

A comparative study on determination of composition of uranium thorium mixed oxides by tube and radioisotope excited EDXRF

International Nuclear Information System (INIS)

Dhara, Sangita; Sanjay Kumar, S.; Misra, N.L.; Aggarwal, S.K.; Singh, Ajit Kumar; Lodha, G.S.

2009-01-01

Energy Dispersive X-ray Fluorescence (EDXRF) methods for determination of uranium and thorium in their mixed oxide matrices using tube and radioisotope excitation sources have been developed. The methodology involves preparation of mixed oxide calibration/sample mixtures of uranium and thorium oxides, mixing of fixed amount of internal standard Yttrium in form of Yttrium oxide, pelletizing these mixtures after thorough mixing and recording their EDXRF spectra using Rh target as well as 109 Cd radioisotope source. The samples were analysed for uranium and thorium on the basis of calibration plots

Electronic structure and core-level spectra of light actinide dioxides in the dynamical mean-field theory

Czech Academy of Sciences Publication Activity Database

Kolorenč, Jindřich; Shick, Alexander; Lichtenstein, A.I.

2015-01-01

Roč. 92, č. 8 (2015), "085125-1"-"085125-10" ISSN 1098-0121 R&D Projects: GA ČR GC15-05872J Institutional support: RVO:68378271 Keywords : electronic-structure calculations * dynamical mean-field theory * Mott insulators * actinides * oxides * photoemission Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 3.736, year: 2014

Synergy of FexCe1-xO2 mixed oxides for N2O decomposition

NARCIS (Netherlands)

Perez-Alonso, FJ; Melian Cabrera, Ignacio; Granados, ML; Kapteijn, F; Fierro, JLG

2006-01-01

Fe-Ce mixed oxides prepared by coprecipitation showed considerable synergy in N2O decomposition when compared with pure metal oxide counterparts. The mixed system also displayed higher stability in reaction at high temperature. Through characterisation by XRD, XPS and TPR, the activity-stability

Actinide recycle potential in the integral fast reactor

International Nuclear Information System (INIS)

Chang, Y.I.

1993-01-01

The Integral Fast Reactor (IFR) fuel cycle holds promise for substantial improvements in economics, diversion-resistance, and waste management. In the IFR pyroprocessing, minor actinides accompany plutonium product stream, and therefore, actinide recycle occurs naturally. The fast neutron spectrum of the IFR makes it an ideal actinide burner, as well. This paper discusses technical features of the IFR fuel cycle, its technical progress, the development status, and potential implications on long-term waste management

The radiological impact of actinides discharged to the Irish Sea

International Nuclear Information System (INIS)

Hunt, G.J.; Smith, B.D.

1999-01-01

This paper describes the radiological effects of releases of actinides to the Irish Sea from Sellafield, the major source. Exposure pathways to man since the commencement of discharges in 1952 are reviewed; the importance of actinides began to increase with increased discharges in the 1970s. With the demise of the porphyra/laverbread pathway due to transport difficulties, the pathway due to fish and shellfish consumption became critical, particularly for actinides through molluscan shellfish. A reassessment on the current basis of effective dose shows that peak exposures to the critical group of about 2 mSv yr -1 were received in the mid-1970s, about 30% of which was due to actinides. Effective doses have since reduced but the relative importance of actinides is greater, due to the interplay of discharges of radionuclides from Sellafield and their behaviour in the environment. Additive doses through sea food due to releases of natural radionuclides from the Marchon phosphate plant at Whitehaven are also considered, although the actinide component from this source has been small. Exposures due to actinides from Sellafield via other pathways are shown to be much lower than those involving sea food. Collective doses are also considered; these peaked at about 300 man-Sv to the European population (including the UK) in 1979, with only a few percent due to actinides. As in the case of critical group doses, the relative importance of actinides has increased in recent years within the decreasing total collective dose. For both critical group and collective doses, therefore, the actinide component needs to be kept under review. (Copyright (c) 1999 Elsevier Science B.V., Amsterdam. All rights reserved.)

Environmental chemistry of the actinide elements

International Nuclear Information System (INIS)

Rao Linfeng

1986-01-01

The environmental chemistry of the actinide elements is a new branch of science developing with the application of nuclear energy on a larger and larger scale. Various aspects of the environmental chemistry of the actinide elements are briefly reviewed in this paper, such as its significance in the nuclear waste disposal, its coverage of research fields and possible directions for future study

Actinide separations by supported liquid membranes

International Nuclear Information System (INIS)

Danesi, P.R.; Horwitz, E.P.; Rickert, P.; Chiarizia, R.

1984-01-01

The work has demonstrated that actinide removal from synthetic waste solutions using both flat-sheet and hollow-fiber SLM's is a feasible chemical process at the laboratory scale level. The process is characterized by the typical features of SLM's processes: very small quantities of extractant required; the potential for operations with high feed/strip volume ratios, resulting in a corresponding concentration factor of the actinides; and simplicity of operation. Major obstacles to the implementation of the SLM technology to the decontamination of liquid nuclear wastes are the probable low resistance of polypropylene supports to high radiation fields, which may prevent the application to high-level nuclear wastes; the unknown lifetime of the SLM; and the high Na content of the separated actinide solution

Analysis of large soil samples for actinides

Science.gov (United States)

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.

Ion sensing properties of vanadium/tungsten mixed oxides

International Nuclear Information System (INIS)

Guidelli, Eder Jose; Guerra, Elidia Maria; Mulato, Marcelo

2011-01-01

Vanadium/tungsten mixed oxide (V 2 O 5 /WO 3 ) sensing membranes were deposited on glassy carbon substrates and used as the H + sensor of the extended gate field effect transistor (EGFET) device. X-ray diffractograms indicated a decrease of the interplanar spacing of V 2 O 5 after the insertion of WO 3 revealing that the lamellar structure is under compressive stress. The crystallinity increases with increasing WO 3 molar ratio. The film is not homogeneous, with more WO 3 material sitting at the surface. This influences the response of pH sensors using the EGFET configuration. The maximum sensitivity of 68 mV pH -1 was obtained for the sample with 5% WO 3 molar ratio. For higher WO 3 molar ratios, the behavior is not linear. It can be concluded that V 2 O 5 dominates for acidic solutions while WO 3 dominates for basic solutions. Therefore, the mixed oxide with low amount of WO 3 is the main candidate for further use as biosensor.

Spin and orbital moments in actinide compounds

DEFF Research Database (Denmark)

Lebech, B.; Wulff, M.; Lander, G.H.

1991-01-01

The extended spatial distribution of both the transition-metal 3d electrons and the actinide 5f electrons results in a strong interaction between these electron states when the relevant elements are alloyed. A particular interesting feature of this hybridization, which is predicted by single...... experiments designed to determine the magnetic moments at the actinide and transition-metal sublattice sites in compounds such as UFe2, NpCo2, and PuFe2 and to separate the spin and orbital components at the actinide sites. The results show, indeed, that the ratio of the orbital to spin moment is reduced...

Evaluating the efficacy of a minor actinide burner

International Nuclear Information System (INIS)

Dobbin, K.D.; Kessler, S.F.; Nelson, J.V.; Omberg, R.P.; Wootan, D.W.

1993-06-01

The efficacy of a minor actinide burner can be evaluated by comparing safety and economic parameters to the support ratio. Minor actinide mass produced per unit time in this number of Light Water Reactors (LWRs) can be burned during the same time period in one burner system. The larger the support ratio for a given set of safety and economic parameters, the better. To illustrate this concept, the support ratio for selected Liquid Metal Reactor (LMR) burner core designs was compared with corresponding coolant void worths, a fundamental safety concern following the Chernobyl accident. Results can be used to evaluate the cost in reduced burning of minor actinides caused by LMR sodium void reduction efforts or to compare with other minor actinide burner systems

U{sub x}Th{sub 1-x}(C{sub 2}O{sub 4}){sub 2} solide characterisation studies

Energy Technology Data Exchange (ETDEWEB)

Carrigan, C.; Taylor, R.; Sarsfield, M. [National Nuclear Laboratory, Sellafield, Seascale, Cumbria, CA20 1PG (United Kingdom)

2016-07-01

Many advanced reprocessing schemes under development are aimed at co-processing and co-conversion of actinides, unlike current reprocessing plants that produce separate uranium and plutonium products. The most well developed option for the co-conversion stage is probably oxalate co-precipitation, followed by the thermal co-conversion to a mixed oxide product. It is thus envisaged that future processes will avoid separation of plutonium from uranium and instead allow part of the uranium to flow with the plutonium, resulting in co-precipitation as the oxalate, and finally co-conversion to a mixed uranium-plutonium oxide (MOX), which can be fabricated into recycled nuclear fuel for further energy generation. The co-crystallisation of uranium (IV) and plutonium (III) into a single oxalate structure ensures the homogenous distribution of the 2 actinides at the molecular scale. The joint conversion of uranium and plutonium to the oxide form makes it possible to remove the complicated step of blending and grinding the 2 distinct oxide powders, as currently employed for the purposes of MOX fuel fabrication. This concept can also be extended to other actinides, including minor actinides from partitioning processes such as SANEX (Selective Actinide Extraction) and GANEX (Grouped Actinide Extraction) processes or even a thorium containing product from recycle of thorium based fuels. A selection of U{sub x}Th{sub 1-x}(C{sub 2}O{sub 4}){sub 2} solids at varying concentrations of uranium and thorium were prepared by oxalate co-precipitation. Uranium (VI) was conditioned electrochemically at -0.7 V to uranium (IV), in the presence of hydrazine. The reduced uranium (IV) in nitric acid was mixed with thorium nitrate solutions at different concentration ratios with oxalic acid. The mixed tetravalent uranium-thorium oxalate solid products have been characterised by Raman and IR spectroscopies. The influence of thorium substituted into the uranium oxalate structure was evaluated

U_xTh_1_-_x(C_2O_4)_2 solide characterisation studies

International Nuclear Information System (INIS)

Carrigan, C.; Taylor, R.; Sarsfield, M.

2016-01-01

Many advanced reprocessing schemes under development are aimed at co-processing and co-conversion of actinides, unlike current reprocessing plants that produce separate uranium and plutonium products. The most well developed option for the co-conversion stage is probably oxalate co-precipitation, followed by the thermal co-conversion to a mixed oxide product. It is thus envisaged that future processes will avoid separation of plutonium from uranium and instead allow part of the uranium to flow with the plutonium, resulting in co-precipitation as the oxalate, and finally co-conversion to a mixed uranium-plutonium oxide (MOX), which can be fabricated into recycled nuclear fuel for further energy generation. The co-crystallisation of uranium (IV) and plutonium (III) into a single oxalate structure ensures the homogenous distribution of the 2 actinides at the molecular scale. The joint conversion of uranium and plutonium to the oxide form makes it possible to remove the complicated step of blending and grinding the 2 distinct oxide powders, as currently employed for the purposes of MOX fuel fabrication. This concept can also be extended to other actinides, including minor actinides from partitioning processes such as SANEX (Selective Actinide Extraction) and GANEX (Grouped Actinide Extraction) processes or even a thorium containing product from recycle of thorium based fuels. A selection of U_xTh_1_-_x(C_2O_4)_2 solids at varying concentrations of uranium and thorium were prepared by oxalate co-precipitation. Uranium (VI) was conditioned electrochemically at -0.7 V to uranium (IV), in the presence of hydrazine. The reduced uranium (IV) in nitric acid was mixed with thorium nitrate solutions at different concentration ratios with oxalic acid. The mixed tetravalent uranium-thorium oxalate solid products have been characterised by Raman and IR spectroscopies. The influence of thorium substituted into the uranium oxalate structure was evaluated. Several vibrational modes

Sol-gel chemistry applied to the synthesis of polymetallic oxides including actinides reactivity and structure from solution to solid state; Synthese par voie douce d'oxydes polymetalliques incluant des actinides: reactivite et structure de la solution au solide

Energy Technology Data Exchange (ETDEWEB)

Lemonnier, St

2006-02-15

Minor actinides transmutation is studied at present in order to reduce the radiotoxicity of nuclear waste and the assessment of its technical feasibility requires specific designed materials. When considering americium, yttria stabilized zirconia (Am{sup III} YII Zriv)Or{sub x} is among the ceramic phases that one which presents the required physico-chemical properties. An innovative synthesis of this mixed oxide by sol-gel process is reported in this manuscript. The main aim of this work is to adjust the reactivity of the different metallic cations in aqueous media using complexing agent, in order to initiate a favourable interaction for a homogeneous elements repartition in the forming solid phase. The originality of the settled synthesis lies on an in-situ formation of a stable and monodisperse nano-particles dispersion in the presence of acetylacetone. The main reaction mechanisms have been identified: the sol stabilisation results from an original interaction between the three compounds (Zrly, trivalent cations and acetylacetone). The sol corresponds to a structured system at the nanometer scale for which zirconium and trivalent cations are homogeneously dispersed, preliminary to the sol-gel transition. Furthermore, preliminary studies were carried out with a view to developing materials. They have demonstrated that numerous innovative and potential applications can be developed by taking advantage of the direct and controlled formation of the sol and by adapting the sol-gel transition. The most illustrating result is the preparation of a sintered pellet with the composition Am0,13Zro,73Yo,0901,89 using this approach. (author)

About the correlation between electronic configurations of actinide ions and the properties of their compounds

International Nuclear Information System (INIS)

Ionova, G.V.; Spytsyn, V.I.

1979-01-01

The main purpose of this paper is to show the importance of the reconstruction energies on the actinide properties both in solid state and solutions. As a consequence of the specific dualism localization-delocalization of the 5f and 6d electrons, charge waves can occur in crystal compounds at low temperature. In an extended two-band Hubbard model which takes into account the intra- and inter-site Coulomb interactions as well as the kinetic energy, the criteria for the occurrence of the charge and orbital waves are obtained. Orbital ordering can be accompanied by spin density wave formation. Partial attention is given to the occurrence of supraconductivity, it is proposed that electron pair formation in a mixed valence state is one of the important mechanisms of supraconductivity state formation. The influence of the excitation energy on the stability and geometry is analysed. Estimates of the Cm(IV-V), Cm(V-VI) and Cm(VI-VII) oxidation potentials are given. It is shown that distortion from the linear to the bent structure is possible for AnO 2 + cations

Production and measurement of minor actinides in the commercial fuel cycle

International Nuclear Information System (INIS)

Stanbro, W.D.

1997-03-01

The minor actinide elements, particularly neptunium and americium, are produced as a normal byproduct of the operation of thermal power reactors. Because of the existence of long-lived isotopes of these elements, they constitute the major sources of the residual radiation in spent fuel or in wastes resulting from reprocessing. This has led to examinations by some countries of the possibility of separating the minor actinides from waste products. The papers found in this report address the production of minor actinides in common thermal power reactors as well as approaches to measure these materials in various media. The first paper in this volume, open-quotes Production of Minor Actinides in the Commercial Fuel Cycle,close quotes uses calculations with the ORIGEN2 reactor and decay code to estimate the amounts of minor actinides in spent fuel and separated plutonium as a function of reactor irradiation and the time after discharge. The second paper, open-quotes Destructive Assay of Minor Actinides,close quotes describes a number of promising approaches for the chemical analysis of minor actinides in the various forms in which they are found at reprocessing plants. The next paper, open-quotes Hybrid KED/XRF Measurement of Minor Actinides in Reprocessing Plants,close quotes uses the results of a simulation model to examine the possible applications of the hybrid KED/XRF instrument to the determination of minor actinides in some of the solutions found in reprocessing plants. In open-quotes Calorimetric Assay of Minor Actinides,close quotes the authors show some possible extensions of this powerful technique beyond the normal plutonium assays to include the minor actinides. Finally, the last paper in this volume, open-quotes Environment Measurements of Transuranic Nuclides,close quotes discusses what is known about the levels of the minor actinides in the environment and ways to analyze for these materials in environmental matrices

Trends in actinide processing at Hanford

International Nuclear Information System (INIS)

Harmon, H.D.

1993-09-01

In 1989, the mission at the Hanford Site began a dramatic and sometimes painful transition. The days of production--as we used to know it--are over. Our mission officially has become waste management and environmental cleanup. This mission change didn't eliminate many jobs--in fact, budgets have grown dramatically to support the new mission. Most all of the same skilled crafts, engineers, and scientists are still required for the new mission. This change has not eliminated the need for actinide processing, but it has certainly changed the focus that our actinide chemists and process engineers have. The focus used to be on such things as increasing capacity, improving separations efficiency, and product purity. Minimizing waste had become a more important theme in recent years and it is still a very important concept in the waste management and environmental cleanup arena. However, at Hanford, a new set of words dominates the actinide process scene as we work to deal with actinides that still reside in a variety of forms at the Hanford Site. These words are repackage, stabilize, remove, store and dispose. Some key activities in each of these areas are described in this report

Transmutation of actinides in power reactors.

Science.gov (United States)

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

2005-01-01

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

Separation of actinides and their transmutation

International Nuclear Information System (INIS)

Bouchard, M.; Bathelier, M.; Cousin, M.

1978-08-01

Neutron irradiation of long-half-life actinides for transmutation into elements with shorter half-life is investigated as a means to reduce the long-term hazards of these actinides. The effectiveness of the method is analysed by applying it to fission product solutions from the first extraction cycle of fuel reprocessing plants. Basic principles, separation techniques and transmutation efficiencies are studied and discussed in detail

Study on remain actinides recovery in pyro reprocessing

International Nuclear Information System (INIS)

Suharto, Bambang

1996-01-01

The spent fuel reprocessing by dry process called pyro reprocessing have been studied. Most of U, Pu and MA (minor actinides) from the spent fuel will be recovered and be fed back to the reactor as new fuel. Accumulation of remain actinides will be separated by extraction process with liquid cadmium solvent. The research was conducted by computer simulation to calculate the stage number required. The calculation's results showed on the 20 stages extractor more than 99% actinides can be separated. (author)

Heat capacity measurements and XPS studies on uranium-lanthanum mixed oxides

International Nuclear Information System (INIS)

Venkata Krishnan, R.; Mittal, V.K.; Babu, R.; Senapati, Abhiram; Bera, Santanu; Nagarajan, K.

2011-01-01

Research highlights: → Heat capacity measurements were carried out on (U 1-y La y )O 2±x (y = 0.2, 0.4, 0.6, and 0.8) using differential scanning calorimeter (DSC) in the temperature range 298-800 K. → Enthalpy increment measurements were carried out on the above solid solution using high temperature drop calorimetry in the temperature range 800-1800 K. → Chemical states of U and La in the solid solutions of mixed oxides were determined using X-ray photoelectron spectroscopy (XPS). → The anomalous increase in the heat capacity is attributed to certain thermal excitation process namely Frenkel pair defect of oxygen. → From the XPS investigation, it is observed that the O/M ratio at the surface is higher than that to the bulk. → In uranium rich mixed oxide samples, the surface O/M is greater than 2 whereas that in La rich mixed oxides, it is less than 2, though the bulk O/M in all the samples are less than 2. - Abstract: Heat capacity measurements were carried out on (U 1-y La y )O 2±x (y = 0.2, 0.4, 0.6, and 0.8) using differential scanning calorimeter (DSC) in the temperature range 298-800 K. Enthalpy increment measurements were carried out on the above solid solutions using high temperature drop calorimetry in the temperature range 800-1800 K. Chemical states of U and La in the solid solutions of mixed oxides were determined using X-ray photoelectron spectroscopy (XPS). Oxygen to metal ratios of (U 1-y La y )O 2±x were estimated from the ratios of different chemical states of U present in the sample. Anomalous increase in the heat capacity is observed for (U 1-y La y )O 2±x (y = 0.4, 0.6 and 0.8) with onset temperatures in the range of 1000-1200 K. The anomalous increase in the heat capacity is attributed to certain thermal excitation process, namely, Frenkel pair defect of oxygen. The heat capacity value of (U 1-y La y )O 2±x (y = 0.2, 0.4, 0.6, and 0.8) at 298 K are 65.3, 64.1, 57.7, 51.9 J K -1 mol -1 , respectively. From the XPS investigations

The Properties of Trilaurylmethylammonium Nitrate as an Extractant for Trivalent Actinides. RCN Report

International Nuclear Information System (INIS)

Ooyen, J. van

1970-03-01

The concept of the group of the actinide elements as a f-type transition series within the periodic system was first launched by G.T. Seaborg in 1944]. In this transition series the filling up of the 5 f electron shell would cause a close similarity with the lanthanide series. This proved to be a very fruitful hypothesis in the prediction of the properties of the new elements americium and curium that soon were discovered. The new hypothesis necessitated a shift of the accepted ideas concerning the place of the elements thorium, protactinium and uranium in the periodic table. In fact, the chemistry of these elements had never been considered to be so closely parallel to that of the lanthanides. On the contrary, the trend in the stability of the oxidation states had been interpreted to indicate that these elements would belong to group IVA, VA and VIA respectively. It is undeniable that there are marked differences in oxidation states between the lanthanide elements and the first six elements of the actinide series. However, physical and chemical investigations both of the newly discovered elements and the elements actinium to uranium disclosed many resemblances with the lanthanides that had not been noticed before in this group. The actinide elements - and more in particular the transuranium elements - have been the subject of a number of monographs covering the discovery, the synthesis, the systematics, the chemistry, and (or) the nuclear properties of these elements. It is for this reason that the scope of the following sections in this chapter will be limited to a summary of the chemistry in sofar as it is relevant to the investigations described in the following chapters, viz., the properties of the elements in aqueous systems and more in particular in those systems containing nitrate ions

Use of fast-spectrum reactors for actinide burning

International Nuclear Information System (INIS)

Chang, Yoon I.

1991-01-01

Finally, Integral Fast Reactor (IFR) pyroprocessing has been developed only in recent years and it appears to have potential as a relatively uncomplicated, effective actinide recovery process. In fact, actinide recycling occurs naturally in the IFR fuel cycle. Although still very much developmental, the entire IFR fuel cycle will be demonstrated on prototype-scale in conjunction with the EBR-II and its refurbished Fuel Cycle Facility starting in late 1991. A logical extension to this work, therefore, is to establish whether this IFR pyrochemical processing can be applied to extracting actinides from LWR spent fuel. This paper summarizes current thinking on the rationale for actinide recycle, its ramifications on the geologic repository and the current high-level waste management plans, and the necessary development programs. 4 figs., 4 tabs

Disposition of actinides released from high-level waste glass

International Nuclear Information System (INIS)

Ebert, W.L.; Bates, J.K.; Buck, E.C.; Gong, M.; Wolf, S.F.

1994-01-01

The disposition of actinide elements released from high-level waste glasses into a tuff groundwater in laboratory tests at 90 degrees C at various glass surface area/leachant volume ratios (S/V) between dissolved, suspended, and sorbed fractions has been measured. While the maximum release of actinides is controlled by the corrosion rate of the glass matrix, their solubility and sorption behavior affects the amounts present in potentially mobile phases. Actinide solubilities are affected by the solution pH and the presence of complexants released from the glass, such as sulfate, phosphate, and chloride, radiolytic products, such as nitrate and nitrite, and carbonate. Sorption onto inorganic colloids formed during lass corrosion may increase the amounts of actinides in solution, although subsequent sedimentation of these colloids under static conditions leads to a significant reduction in the amount of actinides in solution. The solution chemistry and observed actinide behavior depend on the S/V of the test. Tests at high S/V lead to higher pH values, greater complexant concentrations, and generate colloids more quickly than tests at low S/V. The S/V also affects the rate of glass corrosion

Thermodynamic study on the complexation of Trivalent actinide and lanthanide cation by N-donor ligands in homogeneous conditions; Etude thermodynamique de la complexation des ions actinide (III) et lanthanide (III) par des ligands polyazotes en milieu homogene

Energy Technology Data Exchange (ETDEWEB)

Miguirditchian, M

2004-07-01

Polydentate N-donor ligands, alone or combined with a synergic acid, may selectively extract minor actinides(III) from lanthanide(III) ions, allowing to develop separation processes of long-live radioelements. The aim of the researches carried out during this thesis was to better understand the chemical mechanisms of the complexation of f-elements by Adptz, a tridentate N-donor ligand, in homogeneous conditions. A thermodynamic approach was retained in order to estimate, from an energetic point of view, the influence of the different contributions to the reaction, and to acquire a complete set of thermodynamic data on this reaction. First, the influence of the nature of the cation on the thermodynamics was considered. The stability constants of the 1/1 complexes were systematically determined by UV-visible spectrophotometry for every lanthanide ion (except promethium) and for yttrium in a mixed solvent methanol/water in volume proportions 75/25%. The thermodynamic parameters ({delta}H{sup 0} {delta}{sup S}) of complexation were estimated by the van't Hoff method and by micro-calorimetry. The trends of the variations across the lanthanide series are compared with similar studies. The same methods were applied to the study of three actinide(III) cations: plutonium, americium and curium. The comparison of these values with those obtained for the lanthanides highlights the increase of stability of these complexes by a factor of 20 in favor of the actinide cations. This gap is explained by a more exothermic reaction and is associated, in the data interpretation, to a higher covalency of the actinide(III)-nitrogen bond. Then, the influence of the change of solvent composition on the thermodynamic of complexation was studied. The thermodynamic parameters of the complexation of europium(III) by Adptz were determined for several fractions of methanol. The stability of the complex formed increases with the percentage of methanol in the mixed solvent, owing to an

Nonaqueous method for dissolving lanthanide and actinide metals

International Nuclear Information System (INIS)

Crisler, L.R.

1975-01-01

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

Biotransformation of uranium and other actinides in radioactive wastes

International Nuclear Information System (INIS)

Francis, A.J.

1998-01-01

Microorganisms affect the solubility, bioavailability, and mobility of actinides in radioactive wastes. Under appropriate conditions, actinides are solubilized or stabilized by the direct enzymatic or indirect nonenzymatic actions of microorganisms. Biotransformation of various forms of uranium (ionic, inorganic, and organic complexes) by aerobic and anaerobic microorganisms has been extensively studied, whereas limited information is available on other important actinides (Th, Np, Pu, and Am). Fundamental information on the mechanisms of biotransformation of actinides by microbes under various environmental conditions will be useful in predicting the long-term performance of waste repositories and in developing strategies for waste management and remediation of contaminated sites. (orig.)

Influence of additives on the structure and microstructure of lanthanides and actinides oxalates

International Nuclear Information System (INIS)

Haidon, Blaise; Vitart, Anne-Lise; Rivenet, Murielle; Arab-Chapelet, Benedicte; Roussel, Pascal; Delahaye, Thibaud; Grandjean, Stephane; Abraham, Francis

2015-07-01

Oxalic conversion is a well-known process in the nuclear industry where it is used for precipitating plutonium as an oxalate thereafter calcinated into an oxide. As there is a strong relationship between the morphology of the oxalate precursor and that of the resulting oxide, it is of interest to control the oxalate structure and microstructure during the precipitation step. The influence of additives on the precipitation of neodymium (III) oxalates, non-radioactive analogs of actinides (III) oxalates, was explored. With the use of nitrilotri-methylphosphonic acid (NTMP), the structure and microstructure of the neodymium oxalates are different from that obtained without additive. (authors)

Comparative study for minor actinide transmutation in various fast reactor core concepts

International Nuclear Information System (INIS)

Ohki, S.

2001-01-01

A comparative evaluation of minor actinide (MA) transmutation property was performed for various fast reactor core concepts. The differences of MA transmutation property were classified by the variations of fuel type (oxide, nitride, metal), coolant type (sodium, lead, carbon dioxide) and design philosophy. Both nitride and metal fuels bring about 10% larger MA transmutation amount compared with oxide fuel. The MA transmutation amount is almost unchanged by the difference between sodium and lead coolants, while carbon dioxide causes a reduction by about 10% compared with those. The changes of MA transmutation property by fuel and coolant types are comparatively small. The effects caused by the difference of core design are rather significant. (author)

Strategies for minority actinides transmutation in fast reactors

International Nuclear Information System (INIS)

Perez-Martin, S.; Martin-Fuertes, F.; Alvarez-Velarde, F.

2010-01-01

Presentation of the strategies that can be followed in fast reactors designed for the fourth generation to reduce the inventory of minority actinides generated in current light water reactors, as the actinides generation in fast reactor.

Actinide-handling experience for training and education of future expert under J-ACTINET

International Nuclear Information System (INIS)

Osaka, Masahiko; Sato, Isamu; Miwa, Shuhei; Konashi, Kenji; Li, Dexin; Homma, Yoshiya; Yamamura, Tomoo; Hayashi, Hirokazu; Minato, Kazuo; Sekimoto, Syun; Kubota, Takumi; Fukutani, Satoshi; Hori, Junichi; Okumura, Ryo; Uehara, Akihiro; Fujii, Toshiyuki; Yamana, Hajimu; Kurosaki, Ken; Muta, Hiroaki; Ohishi, Yuji; Yamanaka, Shinsuke; Uno, Masayoshi; Yaita, Tsuyoshi

2011-01-01

Summer schools for future experts have successfully been completed under Japan Actinide Network (J-ACTINET) for the purpose of development of human resources who are expected to be engaged in every areas of actinide-research/engineering. The first summer school was held in Ibaraki-area in August 2009, followed by the second one in Kansai-area in August 2010. Two summer schools have focused on actual experiences of actinides in actinide-research fields for university students and young researchers/engineers as an introductory course of actinide-researches. Many efforts were made to awaken interests into actinide-researches inside the participants during short periods of schools, 3 to 4 days. As actinides must be handled inside special apparatuses such as an air-tight globe-box with well-trained and qualified technicians, programs were optimized for effective experiences of actinides-handling. Several quasi actinide-handling experiences at the actinide-research fields have attracted attentions of participants at the first school in Ibaraki-area. The actual experiments using actinides-containing solutions have been carried out at the second school in Kansai-area. Future summer schools will be held every year for the sustainable human resource development in various actinide-research fields, together with other training and education programs conducted by the J-ACTINET. (author)

The effects of actinide separation on the radiological consequences of disposal of high-level radioactive waste on the ocean bed

International Nuclear Information System (INIS)

Camplin, W.C.; Grimwood, P.D.; White, I.F.

1980-01-01

One option in the management of high-level radioactive wastes is to separate the actinides prior to vitrification and disposal. This option is examined in the context of disposal of high-level wastes on the deep ocean bed. The initial quantity of waste corresponds to the generation of 1000 GW(e)y of nuclear energy, and the actinide-separation process is assumed to remove 99% of all elements of atomic number greater than that of actinium. The models used to describe the dispersion of activity from a single disposal site on the bed of the Atlantic Ocean represent both local dispersion and long-term mixing. Collective doses and doses to individuals are calculated for six potential pathways: ingestion of fish, crustacea, molluscs, plankton and seaweed, and external irradiation from contaminated beach sediments. The period from 400 to 1,000,000 years after disposal is considered. The potential radiological impact from disposal of high-level waste without separation of actinides on the ocean bed arises from the actinides; isotopes of americium, neptunium and plutonium give the highest doses. Actinide separation would reduce these doses in proportion to the effectiveness of the separation process, until doses become determined by fission products rather than actinides: the achievable dose reduction would be a factor of approximately a hundred, or less for certain pathways. This reduction applies only to doses to the public from waste disposal: no account was taken of doses arising from the separation process itself or from the management of the separated actinides. The results of the assessment are contrasted with those of similar studies based on toxicity indices. Major deficiencies are identified in the use of toxicity indices as a basis for decision-making. (author)

Actinide-specific complexing agents: their structural and solution chemistry

International Nuclear Information System (INIS)

Raymond, K.N.; Freeman, G.E.; Kappel, M.J.

1983-07-01

The synthesis of a series of tetracatecholate ligands designed to be specific for Pu(IV) and other actinide(IV) ions has been achieved. Although these compounds are very effective as in vivo plutonium removal agents, potentiometric and voltammetric data indicate that at neutral pH full complexation of the Pu(IV) ion by all four catecholate groups does not occur. Spectroscopic results indicate that the tetracatecholates, 3,4,3-LICAMS and 3,4,3-LICAMC, complex Am(III). The Am(IV)/(III)-catecholate couple (where catecholate = 3,4,3-LICAMS or 3,4,3-LICAMC) is not observed, but may not be observable due to the large currents associated with ligand oxidation. However, within the potential range where ligand oxidation does not occur, these experiments indicate that the reduction potential of free Am(IV)/(III) is probably greater than or equal to + 2.6 V vs NHE or higher. Proof of the complexation of americium in the trivalent oxidation state by 3,4,3-LICAMS and 3,4,3-LICAMC elimates the possibility of tetracatholates stabilizing Am(IV) in vivo

Impact of minor actinide recycling on sustainable fuel cycle options

Energy Technology Data Exchange (ETDEWEB)

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

2017-11-01

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 while 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

Proceedings of the symposium Actinides 2006 - Basic Science, Applications and Technology

International Nuclear Information System (INIS)

Blobaum, Kerri J.M.; Chandler, Elaine A.; Havela, Ladislav; Maple, M. Brian; Neu, Mary P.

2007-01-01

These proceedings from the September 2006 symposium includes papers presented on experimental and modeling work with the intention of broadening understanding of the field of actinide research. Actinides have gained attention recently because of their roles in the threat of nuclear terrorism (e.g., 'dirty bombs') and the use of nuclear power to offset fossil fuel consumption. Actinide science is the study of the elements with atomic numbers in the range of 90 to 103, which includes uranium and plutonium. Beyond the well-known nuclear reactions of these heavy radioactive metals, the large electron clouds with 5f electrons in the outer shell yield fascinating and complex chemistries, crystal structures, and physical properties. Traditionally, actinide research has been divided among three scientific disciplines: chemistry (nuclear chemistry and radiochemistry); physics (condensed matter physics and electronic structure); and materials science (metallurgy). Modern actinide research, however, has become an interdisciplinary blend of these traditional fields, and it also incorporates developing fields such as environmental chemistry and superconductivity. Improved scientific understanding of actinides is needed for development of materials for actinide detection and nuclear fuels, and for safer management of nuclear waste. Recently, there has been a resurgence of actinide science at national laboratories and universities. The current multidisciplinary approach to actinide science lays the groundwork for understanding the connection between the 5f electronic structure and observed chemical reactions and physical properties such as structural phase transformations and novel ground states. This work provides many opportunities for new researchers in actinide science. These proceedings gather 25 selected papers among the 53 presentations given at this symposium

Atomic transport properties in UO2 and mixed oxides (U,Pu)O2

International Nuclear Information System (INIS)

Matzke, H.

1987-01-01

Atomic diffusion processes in UO 2 and in the fast-breeder reactor fuel, (U,Pu)O 2 are reviewed. Emphasis is given to the slower-moving species, i.e. U and Pu. Self-diffusion, chemical diffusion, diffusion in a thermal gradient, enhancement of diffusion by radiation and fission and the operative diffusion mechanisms are discussed. The main parameter, besides the temperature, is the oxygen-to-metal ratio (O/M ratio) of the oxide. The experimental results are compared with recent calculations reported elsewhere in this volume. Also treated are effects of the possible lambda-transition at ca.2600 K in UO 2 on high-temperature kinetic processes. The present knowledge on the diffusion and mobility of fission products with emphasis on volatile and gaseous elements, and of other actinides with emphasis on their valence states are treated. Gaps in our knowledge are pointed out and the relevance of the available results for oxide fuel during reactor operation is discussed. Whereas much is known for the as-produced 'virgin' fuel, more results are urgently needed for oxides with higher burn-ups containing a few per cent fission products. Finally, technological applications of the diffusion results are treated. As an example, important savings in cost, energy and time in fuel sintering were recently achieved based on basic studies of diffusion properties of UO 2 . (author)

Synthesis of mesoporous cerium-zirconium mixed oxides by hydrothermal templating method

Institute of Scientific and Technical Information of China (English)

无

2008-01-01

Mesoporous cerium-zirconium mixed oxides were prepared by hydrothermal method using cetyl trimethyl ammonium bromide (CTAB) as template.The effects of amount of template,pH value of solution and hydrothermal temperature on mesostructure of samples were systematically investigated.The final products were characterized by XRD,TEM,FT-IR,and BET.The results indicate that all the cerium-zirconium mixed oxides present a meso-structure.At molar ratio of n(CTAB)/n((Ce)+(Zr))=0.15,pH value of 9,and hydrothermal temperature of 120 ℃,the samples obtained possess a specific surface area of 207.9 m2/g with pore diameter of 3.70 nm and pore volume of 0.19 cm3/g.

A manufacturing process for a mixed-oxide type superconducting material

International Nuclear Information System (INIS)

Gendre, P.; Regnier, P.; Schmirgeld-Mignot, L.; Marquet, A.

1995-01-01

In order to produce high temperature superconducting materials such as YBaCuO and Bi 2 Sr 2 Ca Cu 2 O 8 , a process is presented which consists in an electrodeposition on a conductive substrate of successive layers made of the metallic elements composing the superconductor, with only one element in each layer; between each layer deposition, an intermediary oxide-reaction thermal treatment is carried out; a global oxidation thermal treatment is then finally conducted to produce the mixed oxide material. Narrow superconducting transitions and high critical current densities are possible. 3 refs., 4 figs

Casting of metallic fuel containing minor actinide additions

International Nuclear Information System (INIS)

Trybus, C.L.; Henslee, S.P.; Sanecki, J.E.

1992-01-01

A significant attribute of the Integral Fast Reactor (IFR) concept is the transmutation of long-lived minor actinide fission products. These isotopes require isolation for thousands of years, and if they could be removed from the waste, disposal problems would be reduced. The IFR utilizes pyroprocessing of metallic fuel to separate auranium, plutonium, and the minor actinides from nonfissionable constituents. These materials are reintroduced into the fuel and reirradiated. Spent IFR fuel is expected to contain low levels of americium, neptunium, and curium because the hard neutron spectrum should transmute these isotopes as they are produced. This opens the possibility of using an IFR to trnasmute minor actinide waste from conventional light water reactors (LWRs). A standard IFR fuel is based on the alloy U-20% Pu-10% Zr (in weight percent). A metallic fuel system eases the requirements for reprocessing methods and enables the minor actinide metals to be incorporated into the fuel with simple modifications to the basic fuel casting process. In this paper, the authors report the initial casting experience with minor actinide element addition to an IFR U-Pu-Zr metallic fuel

The role of actinide burning and the Integral Fast Reactor in the future of nuclear power

Energy Technology Data Exchange (ETDEWEB)

Hollaway, W.R.; Lidsky, L.M.; Miller, M.M.

1990-12-01

A preliminary assessment is made of the potential role of actinide burning and the Integral Fast Reactor (IFR) in the future of nuclear power. The development of a usable actinide burning strategy could be an important factor in the acceptance and implementation of a next generation of nuclear power. First, the need for nuclear generating capacity is established through the analysis of energy and electricity demand forecasting models which cover the spectrum of bias from anti-nuclear to pro-nuclear. The analyses take into account the issues of global warming and the potential for technological advances in energy efficiency. We conclude, as do many others, that there will almost certainly be a need for substantial nuclear power capacity in the 2000--2030 time frame. We point out also that any reprocessing scheme will open up proliferation-related questions which can only be assessed in very specific contexts. The focus of this report is on the fuel cycle impacts of actinide burning. Scenarios are developed for the deployment of future nuclear generating capacity which exploit the advantages of actinide partitioning and actinide burning. Three alternative reactor designs are utilized in these future scenarios: The Light Water Reactor (LWR); the Modular Gas-Cooled Reactor (MGR); and the Integral Fast Reactor (FR). Each of these alternative reactor designs is described in some detail, with specific emphasis on their spent fuel streams and the back-end of the nuclear fuel cycle. Four separation and partitioning processes are utilized in building the future nuclear power scenarios: Thermal reactor spent fuel preprocessing to reduce the ceramic oxide spent fuel to metallic form, the conventional PUREX process, the TRUEX process, and pyrometallurgical reprocessing.

The role of actinide burning and the Integral Fast Reactor in the future of nuclear power

International Nuclear Information System (INIS)

Hollaway, W.R.; Lidsky, L.M.; Miller, M.M.

1990-12-01

A preliminary assessment is made of the potential role of actinide burning and the Integral Fast Reactor (IFR) in the future of nuclear power. The development of a usable actinide burning strategy could be an important factor in the acceptance and implementation of a next generation of nuclear power. First, the need for nuclear generating capacity is established through the analysis of energy and electricity demand forecasting models which cover the spectrum of bias from anti-nuclear to pro-nuclear. The analyses take into account the issues of global warming and the potential for technological advances in energy efficiency. We conclude, as do many others, that there will almost certainly be a need for substantial nuclear power capacity in the 2000--2030 time frame. We point out also that any reprocessing scheme will open up proliferation-related questions which can only be assessed in very specific contexts. The focus of this report is on the fuel cycle impacts of actinide burning. Scenarios are developed for the deployment of future nuclear generating capacity which exploit the advantages of actinide partitioning and actinide burning. Three alternative reactor designs are utilized in these future scenarios: The Light Water Reactor (LWR); the Modular Gas-Cooled Reactor (MGR); and the Integral Fast Reactor (FR). Each of these alternative reactor designs is described in some detail, with specific emphasis on their spent fuel streams and the back-end of the nuclear fuel cycle. Four separation and partitioning processes are utilized in building the future nuclear power scenarios: Thermal reactor spent fuel preprocessing to reduce the ceramic oxide spent fuel to metallic form, the conventional PUREX process, the TRUEX process, and pyrometallurgical reprocessing

Investigation of actinides speciation within the presence of ligands of interest for decorporation; Etude de la speciation des actinides vis-a-vis de ligands d'interet pour la decorporation

Energy Technology Data Exchange (ETDEWEB)

Bonin, L

2008-01-15

Data about the behaviour of actinides in biological media are required in order to investigate their decorporation. Those data are obtained through in vivo experiments and the study of chemical speciation of actinides within the presence of biological constituents. A part of this work consists in the development of a method leading to the determination of the speciation of actinides at the oxidation state +IV within the presence of a complexing species, as well as its structure. The method was applied to two types of ligands: 1) a constituent of blood plasma: the citrate anion. The various complexes formed were investigated and their formation constants were quantified. The coordination mode of the ligand was then clarified through a structural study of the complexes, underlining the role of only one carboxylic site and of the alcohol function. 2) chelating agents used for decorporation. The formation constants of complexes of An(IV) with NTA and DTPA were determined. The coordination number of the metallic cation in those complexes as well as the role of the nitrogen atom were proved. Lastly, the behaviour of Pu(IV) within the presence of LIHOPO was investigated. This chelating agent, more efficient than DTPA in the case of in vivo decorporation of Np, forms very stable complexes with the metallic cation. One of those complexes can be assumed to present a stoichiometry 2:3. (author)

Actinide Sequestration Using Self-Assembled Monolayers on Mesoporous Supports

International Nuclear Information System (INIS)

Fryxell, Glen E.; Lin, Yuehe; Fiskum, Sandra K.; Birnbaum, Jerome C.; Wu, Hong; Kemner, K. M.; Kelly, Shelley

2005-01-01

Surfactant templated synthesis of mesoporous ceramics provides a versatile foundation upon which to create high efficiency environmental sorbents. These nanoporous ceramic oxides condense a huge amount of surface area into a very small volume. The ceramic oxide interface is receptive to surface functionalization through molecular self-assembly. The marriage of mesoporous ceramics with self-assembled monolayer chemistry creates a powerful new class of environmental sorbent materials called self-assembled monolayers on mesoporous supports (SAMMS). These SAMMS materials are highly efficient sorbents, whose interfacial chemistry can be fine-tuned to selectively sequester a specific target species, such as heavy metals, tetrahedral oxometallate anions and radionuclides. Details addressing the design, synthesis and characterization of SAMMS materials specifically designed to sequester actinides, of central importance to the environmental clean-up necessary after 40 years of weapons grade plutonium production, as well as evaluation of their binding affinities and kinetics are presented

Continuous precipitation of mineral products: influence of mixing conditions on the co-precipitation of cerium-zirconium mixed oxides

International Nuclear Information System (INIS)

Di Patrizio, Nicolas

2015-01-01

An automated experimental set-up with rapid mixers is used to study the influence of mixing conditions on the co-precipitation of cerium-zirconium mixed oxides. The intensity of mixing is controlled by the inlet flow rates of the reacting solutions. An engulfment model is used to estimate a mixing time from the measurement of a segregation index by the Villermaux-Dushman reaction system. Three geometries of Hartridge Roughton mixers are compared. Mixing performance is better when a separate mixing chamber upstream of a narrower outlet pipe is present. A better mixing decreases the maximal reducibility temperature of the material and increases the crystal strains of the particles calcined at 1100 C. This is probably due to a better homogenization of the particles content. The important incorporation of nitrates in the particle at the outlet of the mixers shows precipitation occurs while the mixing process is not finished. This experimental result was confirmed by numerical simulation and an estimation of sur-saturations during the mixing process. (author)

Comparative evaluation of DHDECMP [dihexyl-N,N-diethylcarbamoyl-methylphosphonate] and CMPO [octylphenyl-N,N,-diisobutylcarbamoylmethylphosphine oxide] as extractants for recovering actinides from nitric acid waste streams

International Nuclear Information System (INIS)

Marsh, S.F.; Yarbro, S.L.

1988-02-01

Certain neutral, bifunctional organophosphorous compounds are of special value to the nuclear industry. Dihexyl-N,N-diethylcarbomoylmethylphosphonate (DHDECMP) and octylphenyl-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) are highly selective extractants for removing actinide and lanthanide elements from nitric acid. We obtained these two extractants from newly available commercial sources and evaluated them for recovering Am(III), Pu(IV), and U(VI) from nitric acid waste streams of plutonium processing operations. Variables included the extractant (DHSECMP or CMPO), extractant/tributylphosphate ratio, diluent, nitrate concentration, nitrate salt/nitric acid ratio, fluoride concentration, and contact time. Based on these experimental data, we selected DHDECMP as the perferred extractant for this application. 18 refs., 30 figs

High temperature vaporization/decomposition studies of lanthanide and actinide fluorides

International Nuclear Information System (INIS)

Gibson, J.K.; Haire, R.G.

1987-01-01

Binary fluorides of the lanthanide and actinide elements comprise a fundamental class of compounds. The authors' investigations of their basic high temperature vaporization and/or decomposition behavior are aimed at elucidating more fully the thermal properties of selected tri- and tetrafluorides and extending such investigations to fluorides which have not been studied previously. Depending on the particular system and the specific experimental conditions, the authors' measurements can provide such information as the enthalpy associated with a congruent vaporization process and/or the relative stabilities of fluorides containing a lanthanide/actinide element in different oxidation states. The authors are also studying the congruent vaporization of selected lanthanide trifluorides with particular emphasis on two areas. The first concerns the variation in the enthalpies of sublimation of the trifluorides across the lanthanide series. Although this variation is rather small (δ5 kcal where ΔH/sub subl/ is approximately 100 kcal), it is larger than observed for other lanthanide trihalides and is unusually irregular. To examine this reported variation more closely, they are attempting to measure relative vapor pressures/enthalpies of vaporization by studying mixtures of two or more lanthanide trifluorides by the technique discussed above

A novel dipicolinamide-dicarbollide synergistic solvent system for actinide extraction

Energy Technology Data Exchange (ETDEWEB)

Patil, Ajay Bhagwan [Bhabha Atomic Research Centre, Mumbai (India). Radiochemistry Div.; Pune Univ. (India). Garware Research Centre; Pathak, Priyanath; Mohapatra, Prasanta Kumar [Bhabha Atomic Research Centre, Mumbai (India). Radiochemistry Div.; Shinde, Vaishali Sanjay [Pune Univ. (India). Garware Research Centre; Alyapyshev, M.Yu.; Babain, Vasiliy A. [Federal Agency for Atomic Energy, St. Petersburg (Russian Federation). V.G. Khlopin Radium Institute

2014-09-01

Solvent extraction studies of several actinide ions such as Am(III), U(VI), Np(IV), Np(VI), Pu(IV) were carried out from nitric acid medium using a synergistic mixture of N,N'-diethyl-N,N'-di(para)fluorophenyl-2,6-dipicolinamide, (DEtD(p)FPhDPA, DPA), and hydrogen dicarbollylcobaltate (H{sup +}CCD{sup -}) dissolved in phenyltrifluoromethylsulphone (PTMS). The effects of different parameters such as aqueous phase acidity (0.01-3 M HNO{sub 3}), oxidation states of metal ions, ligand concentration, nature of diluent and temperature on the extraction behavior of metal ions were studied. The extracted Am(III) species was determined as H{sup +}[Am(DPA){sub 2}(CCD){sub 4}]{sup -} With increasing aqueous phase acidities, the extractability of both Am(III) and Eu(III) was found to decrease. The synergistic mixture showed better extraction in mM concentrations as compared to previously studied dipicolinamides. The thermodynamic studies were performed to calculate heat of extraction reaction and the extraction constants. The proposed synergistic mixture showed good extraction for all the metal ions, though lanthanide actinide separation results are not encouraging. (orig.)

Synergy of FexCe1−xO2 mixed oxides for N2O decomposition

NARCIS (Netherlands)

Perez-Alonso, F.J.; Melián-Cabrera, I.; López Granados, M.; Kapteijn, F.; Fierro, J.L.G.

2006-01-01

Fe–Ce mixed oxides prepared by coprecipitation showed considerable synergy in N2O decomposition when compared with pure metal oxide counterparts. The mixed system also displayed higher stability in reaction at high temperature. Through characterisation by XRD, XPS and TPR, the activity–stability

Calculated Atomic Volumes of the Actinide Metals

DEFF Research Database (Denmark)

Skriver, H.; Andersen, O. K.; Johansson, B.

1979-01-01

The equilibrium atomic volume is calculated for the actinide metals. It is possible to account for the localization of the 5f electrons taking place in americium.......The equilibrium atomic volume is calculated for the actinide metals. It is possible to account for the localization of the 5f electrons taking place in americium....

Citrate based ''TALSPEAK'' lanthanide-actinide separation process

International Nuclear Information System (INIS)

Del Cul, G.D.; Bond, W.D.; Toth, L.M.; Davis, G.D.; Dai, S.; Metcalf, D.H.

1994-09-01

The potential hazard posed to future generations by long-lived radionuclides such as the transuranic elements (TRU) is perceived as a major problem associated with the use of nuclear power. TRU wastes have to remain isolated from the environment for ''geological'' periods of time. The costs of building, maintaining, and operating a ''geological TRU repository'' can be very high. Therefore, there are significant economical advantages in segregating the relatively low volume of TRU wastes from other nuclear wastes. The chemical behavior of lanthanides and actinides, 4f and 5f elements respectively, is rather similar. As a consequence, the separation of these two groups is difficult. The ''TALSPEAK'' process (Trivalent Actinide Lanthanide Separations by Phosphorus-reagent Extraction from Aqueous Complexes) is one of the few means available to separate the trivalent actinides from the lanthanides. The method is based on the preferential complexation of the trivalent actinides by an aminopolyacetic acid. Cold experiments showed that by using citric acid the deleterious effects produced by impurities such as zirconium are greatly reduced

Modeling of Cd(II) sorption on mixed oxide

International Nuclear Information System (INIS)

Waseem, M.; Mustafa, S.; Naeem, A.; Shah, K.H.; Hussain, S.Y.; Safdar, M.

2011-01-01

Mixed oxide of iron and silicon (0.75 M Fe(OH)3:0.25 M SiO/sub 2/) was synthesized and characterized by various techniques like surface area analysis, point of zero charge (PZC), energy dispersive X-rays (EDX) spectroscopy, Thermogravimetric and differential thermal analysis (TG-DTA), Fourier transform infrared spectroscopy (FTIR) and X-rays diffraction (XRD) analysis. The uptake of Cd/sup 2+/ ions on mixed oxide increased with pH, temperature and metal ion concentration. Sorption data have been interpreted in terms of both Langmuir and Freundlich models. The Xm values at pH 7 are found to be almost twice as compared to pH 5. The values of both DH and DS were found to be positive indicating that the sorption process was endothermic and accompanied by the dehydration of Cd/sup 2+/. Further, the negative value of DG confirms the spontaneity of the reaction. The ion exchange mechanism was suggested to take place for each Cd/sup 2+/ ions at pH 5, whereas ion exchange was found coupled with non specific adsorption of metal cations at pH 7. (author)

Proposal for experiments with actinide elements

International Nuclear Information System (INIS)

Sanchez, R.G.

1994-01-01

An analytical study was conducted in which critical masses for some actinide isotopes were calculated with the Monte Carlo Neutron Photon (MCNP) Transport computer code. Different spherical computer models were used for even- and odd-neutron nuclides. Critical masses obtained are tabulated for Np-237, Pu-242, Am-241, Am-243, Pu-241, and Am-242m, together with indirect experimental data. Experimental data are needed for actinides with odd number of neutrons

Modification of Co-Mn-Al Mixed Oxide with Potassium and Its Effect on Deep Oxidation of VOC

Czech Academy of Sciences Publication Activity Database

Jirátová, Květa; Mikulová, Jana; Klempa, Jan; Grygar, Tomáš; Bastl, Zdeněk; Kovanda, F.

2009-01-01

Roč. 361, 1-2 (2009), s. 106-116 ISSN 0926-860X R&D Projects: GA ČR GA104/07/1400 Institutional research plan: CEZ:AV0Z40720504; CEZ:AV0Z40320502; CEZ:AV0Z40400503 Keywords : mixed oxide catalysts * VOC total oxidation * potassium promoter Subject RIV: CC - Organic Chemistry Impact factor: 3.564, year: 2009

Storage capacity and oxygen mobility in mixed oxides from transition metals promoted by cerium

Energy Technology Data Exchange (ETDEWEB)

Perdomo, Camilo [Estado Sólido y Catálisis Ambiental (ESCA), Departamento de Química, Facultad de Ciencias, Universidad Nacional de Colombia, Carrera 30 45-03, Bogotá (Colombia); Pérez, Alejandro [Grupo de Investigación Fitoquímica (GIFUJ), Departamento de Química, Facultad de Ciencias, Pontificia Universidad Javeriana, Carrera 7 No. 43-82, Bogotá D.C (Colombia); Molina, Rafael [Estado Sólido y Catálisis Ambiental (ESCA), Departamento de Química, Facultad de Ciencias, Universidad Nacional de Colombia, Carrera 30 45-03, Bogotá (Colombia); Moreno, Sonia, E-mail: smorenog@unal.edu.co [Estado Sólido y Catálisis Ambiental (ESCA), Departamento de Química, Facultad de Ciencias, Universidad Nacional de Colombia, Carrera 30 45-03, Bogotá (Colombia)

2016-10-15

Highlights: • Ce addition to the catalysts improves the availability of oxygen in the materials. • Mixed oxide with Co and Cu exhibits the best oxygen transport properties. • Co presence improves O{sub 2} mobility in the catalysts. • The presence of Cu in the solids improves redox properties. - Abstract: The oxygen mobility and storage capacity of Ce-Co/Cu-MgAl or Ce–MgAl mixed oxides, obtained by hydrotalcite precursors, were evaluated using Toluene-temperature-programmed-reaction, {sup 18}O{sub 2} isotopic exchange and O{sub 2}-H{sub 2} titration. The presence of oxygen vacancies-related species was evaluated by means of Electron Paramagnetic Resonance. A correlation was found between the studied properties and the catalytic activity of the oxides in total oxidation processes. It was evidenced that catalytic activity depends on two related processes: the facility with which the solid can be reduced and its ability to regenerate itself in the presence of molecular oxygen in the gas phase. These processes are enhanced by Cu-Co cooperative effect in the mixed oxides. Additionally, the incorporation of Ce in the Co-Cu catalysts improved their oxygen transport properties.

Storage capacity and oxygen mobility in mixed oxides from transition metals promoted by cerium

International Nuclear Information System (INIS)

Perdomo, Camilo; Pérez, Alejandro; Molina, Rafael; Moreno, Sonia

2016-01-01

Highlights: • Ce addition to the catalysts improves the availability of oxygen in the materials. • Mixed oxide with Co and Cu exhibits the best oxygen transport properties. • Co presence improves O 2 mobility in the catalysts. • The presence of Cu in the solids improves redox properties. - Abstract: The oxygen mobility and storage capacity of Ce-Co/Cu-MgAl or Ce–MgAl mixed oxides, obtained by hydrotalcite precursors, were evaluated using Toluene-temperature-programmed-reaction, 18 O 2 isotopic exchange and O 2 -H 2 titration. The presence of oxygen vacancies-related species was evaluated by means of Electron Paramagnetic Resonance. A correlation was found between the studied properties and the catalytic activity of the oxides in total oxidation processes. It was evidenced that catalytic activity depends on two related processes: the facility with which the solid can be reduced and its ability to regenerate itself in the presence of molecular oxygen in the gas phase. These processes are enhanced by Cu-Co cooperative effect in the mixed oxides. Additionally, the incorporation of Ce in the Co-Cu catalysts improved their oxygen transport properties.

Actinide science with soft x-ray synchrotron radiation

International Nuclear Information System (INIS)

Shuh, D.

2002-01-01

Several workshops, some dating back more than fifteen years, recognised both the potential scientific impact and opportunities that would be made available by the capability to investigate actinide materials in the vacuum ultraviolet (VUV)/soft X-ray region of the synchrotron radiation (SR) spectrum. This spectral region revolutionized the approach to surface materials chemistry and physics nearly two decades ego. The actinide science community was unable to capitalize on these SR methodologies for the study of actinide materials until recently because of radiological safety concerns. ,The Advanced Light Source (ALS) at LBNL is a third-generation light source providing state-of-the-art performance in the VUV/soft X-ray region. Along with corresponding improvements in detector and vacuum technology, the ALS has rendered experiments with small amounts of actinide materials possible. In particular, it has been the emergence and development of micro-spectroscopic techniques that have enabled investigations of actinide materials at the ALS. The primary methods for the experimental investigation of actinide materials in the VUV/soft X-ray region are the complementary photoelectron spectroscopies, near-edge X-ray absorption fine structure (NEXAFS) and X-ray emission spectroscopy (XES) techniques. Resonant photo-emission is capable of resolving the 5f electron contributions to actinide bonding and can be used to characterise the electronic structure of actinide materials. This technique is clearly a most important methodology afforded by the tunable SR source. Core level and valence band photoelectron spectroscopies are valuable for the characterisation of the electronic properties of actinide materials, as well as for general analytical purposes. High-resolution core-level photo-emission and resonant photo-emission measurements from the a (monoclinic) and δ (FCC) allotropic phases of plutonium metal have been collected on beam line 7.0 at the ALS and the spectra show