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Sample records for speciation des actinides

  1. 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

  2. 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

  3. 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

  4. 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)

  5. Electrospray mass spectrometry for actinides and lanthanide speciation

    International Nuclear Information System (INIS)

    Moulin, C.; Amekraz, B.; Colette, S.; Doizi, D.; Jacopin, C.; Lamouroux, C.; Plancque, G.

    2006-01-01

    Electrospray mass spectrometry (ES-MS) is a new speciation technique that has the great interest to be able to probe the element, the ligand and the complex in order to reach the speciation. This paper will focus on the use of ES-MS for the speciation of actinides/lanthanides on several systems of interest in various fields such as the interaction between DTPA (decorporant) and europium, HEBP and uranium, BTP (new extracting agent) and lanthanides with comparison with known chemistry as well as whenever possible with other speciation techniques

  6. Speciation of actinides in marine waters

    International Nuclear Information System (INIS)

    Roberts, R.A.

    1984-01-01

    The oxidation state distribution of plutonium in seawater, pore water from marine sediments, and a series of model solutions similar to seawater was measured using a TTA solvent extraction technique and α liquid scintillation counting methods. Electromigration was used to compare migration behavior of americium in 0.7M NaCl solutions (pH 6.5 to 8.0) with the behavior calculated from predicted speciation. In all pH 8 solutions studied, Pu(VI) was rapidly reduced to Pu(V). In 0.7M NaCl, pH 8.0, and artifical seawater (no organics), the Pu(V) formed was stable. In real seawater (with organic components), a rapid reduction of Pu(VI) to Pu(IV) was also observed. The Pu(V) formed in seawater was metastable; a very slow reduction to Pu(IV) occurred. This reduction was catalyzed by light. Humic acid (obtained from marine sediments from the Bahama Islands), was added to 0.7M NaCl, pH 8.0 solutions to determine its effect on Pu redox reactions. The effect was similar to the reductions in seawater. Increasing the humic acid concentration decreased the amount of Pu(V) which was formed and favored the IV state. The americium electromigration experiments showed a +0.12 net charge for the Am complexes formed in 0.7M NaCl solutions from pH 7.0 to 8.0. This value was smaller than the charge of +0.94 calculated from predicted speciation

  7. The coupling of capillary electrophoresis-inductively coupled plasma mass spectrometer as a speciation instrument for actinides at trace level; Le couplage electrophorese capillaire-spectrometre de masse a source plasma en tant qu'instrument de speciation des actinides a l'etat de traces

    Energy Technology Data Exchange (ETDEWEB)

    Delorme, A

    2004-07-01

    An interface between the separation technique (capillary electrophoresis) and the analytical technique (Inductively Coupled Plasma - Mass Spectrometer) was developed. In that sense, bibliographic and parametric studies allowed to define necessary conditions for the good working of both techniques. The results obtained led to the realisation of an interface capillary electrophoresis / ICP-MS (CE / ICP-MS). This one was experimentally validated on classical separations (alkalis / earth-alkalis and lanthanides) and the detection limit of the analytical system was determined equal to 4 x 10{sup -11} mol.L{sup -1} for plutonium. This result exhibits a gain in detection limit of a factor higher than 10{sup 4} compared to the capillary electrophoresis in standard detection (UV). The studies were made in order to check the capacity of the CE / ICP-MS coupling as a speciation instrument for actinides at trace level and to define the associated analytical procedures. The coupling turned out to be a suited instrument for the determination of absolute electrophoretic mobilities at infinite dilution (physico-chemical property which allows to predict the migration time of an ion under an electrical field in a given electrolyte), for the determination of thermodynamic constants and for the separation of different actinide oxidation states in solution. (author)

  8. Thermodynamics proposes, kinetics decides, speciation dares: speciation of actinides in biological media

    International Nuclear Information System (INIS)

    Ansoborlo, E.

    2005-06-01

    After having recalled the content and purpose of his research thesis, the author proposes a detailed overview of the research works he performed thereafter in the field of the speciation of actinides at the level of the organism entry gates and in target tissues. These works therefore concern four important areas of research in radioprotection: bio-kinetic, toxicology, decorporation, and dosimetry studies. The author outlines how speciation studies can be useful for these different areas, and to better understand and describe, and therefore foresee, the biokinetics and toxicity of radionuclides

  9. NEARSOL, Aqueous Speciation and Solubility of Actinides for Waste Disposal

    International Nuclear Information System (INIS)

    Leach, S.J.; Pryke, D.C.

    1989-01-01

    A - Description of program or function: NEARSOL models the aqueous speciation and solubility of actinides under near-field conditions for disposal using a simple thermodynamic approach. B - Method of solution: The program draws information from a thermodynamic data base consisting of solubility products and complex formation constants for all known species, and standard electrode potentials, at 25 C, corrected for ionic strength effects. By minimising the free energy of the system through a series of iterations, a precipitating solid phase is predicted which limits the solubility, and the concentration of the main aqueous species are calculated as a function of pH. Initially the program evaluates only hydroxide and carbonate species, but the effect of sulphate, phosphate and fluoride anions can also be included. The program is simple to use, requiring inputs of: 1. Actinide(s); 2. pH range; 3. Ionic strength; 4. Redox conditions; 5. Ligand concentrations. Functions are included to calculate the distribution of the protonated and un-protonated forms of carbonate and phosphate and the value of Eh as a function of pH under disposal conditions as required. The program can further evaluate the role of free calcium ions. C - Restrictions on the complexity of the problem: None

  10. Some actinide speciation using laser induced photoacoustic spectroscopy

    International Nuclear Information System (INIS)

    Pollard, P.M.; McMillan, J.W.; Phillips, G.; Thomason, H.P.; Ewart, F.T.

    1988-01-01

    Laser induced photoacoustic spectroscopy is an attractive method for the speciation of actinides in solutions from nuclear disposal studies because it is essentially non-invasive and has a reasonably high sensitivity, down to ca 10 -8 M. A novel true dual beam system has been constructed and commissioned at Harwell with a performance at least equal to any others in existence. It is based on a XeCl excimer laser and a dye laser, beam splitter, two laser power monitors and photoacoustic cells. The wavelength scanning, data collection, and spectra processing and display are controlled by an Apricot computer. The sample and reference cells are housed in an inert atmosphere glove box. Early applications of the equipment described include measurements of Am and Np species under varying conditions of pH, Eh and carbonate concentration. The observations show some correlation with predictions made using the geochemical modelling code PHREEQE. (orig.)

  11. 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

  12. 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.)

  13. Actinide speciation in the shallow aquifer of Mortandad Canyon

    International Nuclear Information System (INIS)

    Nelson, D.M.; Polzer, W.L.

    1983-01-01

    Treated waste effluent at Los Alamos has been released to the environment in Mortandad Canyon since 1963. A study has been initiated to investigate the relative mobilities of the actinides in the shallow aquifer of Mortandad Canyon. Speciation of radionuclides and their adsorption by sediment are important parameters in the evaluation of those mobilities. Plutonium concentrations and oxidation states were measured in water collected from four test wells (MCO 4, 5, 6, 7.5). A regular decrease in 239 240 Pu concentration was observed with increasing distance from the discharge point. The large difference between the concentrations discharged (30 to 1000 pCi/l for period 1977-1982) and those in the wells (0.02 to 5.4 pCi/l) suggests that progressive loss of plutonium from the water as it moves through the alluvium is probably more important in regulating the concentrations than the variability of concentrations in the discharged effluent. The K/sub D/s for 228 Th were also determined and found to be similar to those for plutonium. The factors regulating the concentration of dissolved plutonium are probably the same as those regulating 228 Th. In contrast the K/sub D/s of 241 Am decrease regularly with distance from the discharge point and are about 100 times lower than those of plutonium and thorium for water in wells farthest from the discharge point

  14. 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

  15. Speciation of actinides in aqueous solution by time-resolved laser-induced fluorescence spectroscopy (TRLFS)

    International Nuclear Information System (INIS)

    Kimura, Takaumi; Kato, Yoshiharu; Meinrath, G.; Yoshida, Zenko; Choppin, G.R.

    1995-01-01

    Time-resolved laser-induced fluorescence spectroscopy (TRLFS) as a sensitive and selective method has been applied to the speciation of actinides in aqueous solution. Studies on hydrolysis and carbonate complexation of U(VI) and on determination of hydration number of Cm(III) are reported. (author)

  16. NEARSOL - a simple program to model actinide speciation and solubility under waste disposal conditions

    International Nuclear Information System (INIS)

    Leach, S.J.; Pryke, D.C.

    1986-05-01

    A simple program, NearSol, has been written in Fortran 77 on the Harwell Central Computer to model the aqueous speciation and solubility of actinides under near-field conditions for disposal using a simple thermodynamic approach. The methodology and running of the program are described together with a worked example. (author)

  17. 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.

  18. 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.

  19. 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

  20. Actinide, lanthanide and fission product speciation and electrochemistry in high and low temperature ionic melts

    Energy Technology Data Exchange (ETDEWEB)

    Bhatt, Anand I.; Kinoshita, Hajime; Koster, Anne L.; May, Iain; Sharrad, Clint A.; Volkovich, Vladimir A.; Fox, O. Danny; Jones, Chris J.; Lewin, Bob G.; Charnock, John M.; Hennig, Christoph

    2004-07-01

    There is currently a great deal of research interest in the development of molten salt technology, both classical high temperature melts and low temperature ionic liquids, for the electrochemical separation of the actinides from spent nuclear fuel. We are interested in gaining a better understanding of actinide and key fission product speciation and electrochemical properties in a range of melts. Our studies in high temperature alkali metal melts (including LiCl and LiCl-KCl and CsCl-NaCl eutectics) have focussed on in-situ species of U, Th, Tc and Ru using X-ray absorption spectroscopy (XAS, both EXAFS and XANES) and electronic absorption spectroscopy (EAS). We report unusual actinide speciation in high temperature melts and an evaluation of the likelihood of Ru or Tc volatilization during plant operation. Our studies in lower temperature melts (ionic liquids) have focussed on salts containing tertiary alkyl group 15 cations and the bis(tri-fluor-methyl)sulfonyl)imide anion, melts which we have shown to have exceptionally wide electrochemical windows. We report Ln, Th, U and Np speciation (XAS, EAS and vibrational spectroscopy) and electrochemistry in these melts and relate the solution studies to crystallographic characterised benchmark species. (authors)

  1. Actinide, lanthanide and fission product speciation and electrochemistry in high and low temperature ionic melts

    International Nuclear Information System (INIS)

    Bhatt, Anand I.; Kinoshita, Hajime; Koster, Anne L.; May, Iain; Sharrad, Clint A.; Volkovich, Vladimir A.; Fox, O. Danny; Jones, Chris J.; Lewin, Bob G.; Charnock, John M.; Hennig, Christoph

    2004-01-01

    There is currently a great deal of research interest in the development of molten salt technology, both classical high temperature melts and low temperature ionic liquids, for the electrochemical separation of the actinides from spent nuclear fuel. We are interested in gaining a better understanding of actinide and key fission product speciation and electrochemical properties in a range of melts. Our studies in high temperature alkali metal melts (including LiCl and LiCl-KCl and CsCl-NaCl eutectics) have focussed on in-situ species of U, Th, Tc and Ru using X-ray absorption spectroscopy (XAS, both EXAFS and XANES) and electronic absorption spectroscopy (EAS). We report unusual actinide speciation in high temperature melts and an evaluation of the likelihood of Ru or Tc volatilization during plant operation. Our studies in lower temperature melts (ionic liquids) have focussed on salts containing tertiary alkyl group 15 cations and the bis(tri-fluor-methyl)sulfonyl)imide anion, melts which we have shown to have exceptionally wide electrochemical windows. We report Ln, Th, U and Np speciation (XAS, EAS and vibrational spectroscopy) and electrochemistry in these melts and relate the solution studies to crystallographic characterised benchmark species. (authors)

  2. 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.

  3. 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.

  4. Investigation of actinides speciation within the presence of ligands of interest for decorporation

    International Nuclear Information System (INIS)

    Bonin, L.

    2008-01-01

    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)

  5. Speciation, Mobility and Fate of Actinides in the Groundwater at the Hanford Site

    International Nuclear Information System (INIS)

    Buesseler, K.O.; Dai, M.; Repeta, D.; Wacker, J.F.; Kelley, J.M.

    2003-01-01

    Plutonium and other actinides represent important contaminants in the groundwater and vadose zone at Hanford and other DOE sites. The distribution and migration of these actinides in groundwater must be understood so that these sites can be carefully monitored and effectively cleaned up, thereby minimizing risks to the public. The objective of this project was to obtain field data on the chemical and physical forms of plutonium in groundwater at the Hanford site. We focused on the 100-k and 100-n areas near the Columbia River, where prior reactor operations and waste storage was in close proximity to the river. In particular, a unique set of technical approaches were combined to look at the details of Pu speciation in groundwater, as thus its chemical affinity for soil surfaces and solubility in groundwater, as these impact directly the migration rates off site and possible mitigation possibilities one might undertake to control, or at least better monitor these releases

  6. 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.

  7. 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.

  8. 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.

  9. 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.)

  10. Complexation studies of actinides (U, Pu, Am) with linear polyamino-carboxylate ligands and sidero-chelates; Etudes de la chelation d'actinides (U, Pu, Am) par des ligands polyaminocarboxylate lineaires et des siderochelates d'interet environnemental

    Energy Technology Data Exchange (ETDEWEB)

    Nguyen, L.V.

    2010-11-25

    As part of our research endeavour aimed at developing and improving decontamination processes of wastewater containing alpha emitters, physico-chemical complexation studies of actinides (U, Pu, Am) with organic open-chain ligands such as poly-aminocarboxylic acids (H{sub 4}EDTA) and sidero-chelates (di-hydroxamic acids and desferrioxamine B) have been carried out. Gaining a clear understanding of the coordination properties of the targeted actinides is an essential step towards the selection of the most appropriate chelating agents that will exhibit high uptake efficiencies. EXAFS (Extended X-ray Absorption Fine Structure) measurements at the ESRF synchrotron enabled to elucidate the coordination scheme of uranium and plutonium complexes. Solution thermodynamic investigations were intended to provide valuable information about the nature and the stability of the uranium(VI) and americium(III) complexes prevailing at a given pH in solution. The set of stability constants determined from potentiometric and UV-visible spectrophotometric titrations, allowed to predict the speciation of the selected actinides in presence of the aforementioned ligands and to determine the pH range required for achieving 'ultimate' decontamination. (author) [French] Dans le cadre du developpement et de l'amelioration des procedes de decontamination d'effluents aqueux contamines par des radioelements emetteurs alpha, des etudes physico-chimiques sur la complexation des actinides (U, Pu, Am) avec des ligands organiques tels que des acides polyaminocarboxyliques lineaires (H{sub 4}EDTA) et des siderochelates (acides dihydroxamiques et desferrioxamine B) ont ete effectuees. La comprehension des proprietes de coordination est une etape essentielle pour selectionner les meilleurs agents chelatants qui se montreront efficaces dans le traitement des effluents. Les schemas de coordination des complexes d'uranium et de plutonium avec ces ligands ont ete determines a l

  11. Actinide speciation, further development and application of laser induced photoacoustic spectroscopy and voltammetry

    International Nuclear Information System (INIS)

    Cross, J.E.; Crossley, D.; Edwards, J.W.; Ewart, F.T.; Liezers, M.; McMillan, J.W.; Pollard, P.M.; Turner, S.

    1988-12-01

    Further work is reported on the sensitive determination of actinide species in solution using the Harwell laser induced photoacoustic spectrometer (LIPAS). To permit speciation and solubility measurements under well controlled pH and Eh conditions a combined LIPAS/electrochemical loop has been developed and is described in detail. The new equipment has been used to study uranium and neptunium species at several pH's and Eh's between +280 and -400mV. Comparison of observed species with those predicted by the thermodynamic geochemical modelling code PHREEQE has revealed differences. These, in part, can be reconciled by database refinement, but, in part, have revealed deficiencies in knowledge that require further study. The sensitivity of LIPAS for the measurement of U, Pu, Np and Am species has proved to be high, up to ca 10 -9 M, sensitivities generally being higher for alkaline solution conditions. Preliminary work indicates that LIPAS can be used to distinguish between Pu(IV) complexes with possible cellulose degradation products, typified by gluconic acid, and other organic acids likely to be present in a waste repository. (author)

  12. 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

  13. The speciation of dissolved elements in aquatic solution. Radium and actinides

    International Nuclear Information System (INIS)

    Haesaenen, E.

    1994-01-01

    In the publication, the chemistry and speciation of radium, thorium, protactinium, uranium, neptunium, lutonium, americium and curium in ground-water environment is reviewed. Special attention is given to the transuranium elements, which have a central role in the repository of nuclear wastes. The most important methods used in the speciation of these elements is presented. The laser-induced methods, developed in the 1980's, are especially discussed. These have made it possible, e.g., to speciate the transuranium elements in their very low, actual repository ground-water concentrations (10-100 ng/l). (54 refs., 10 figs., 3 tabs.)

  14. The development of a laser-induced photoacoustic facility for actinide speciation

    International Nuclear Information System (INIS)

    Ewart, F.T.; McMillan, J.W.; Pollard, P.M.; Thomason, H.P.; Liezers, M.

    1987-09-01

    A laser induced photoacoustic spectroscopy (LIPAS) facility has been developed at Harwell to measure actinide species in solution with the minimal disturbance of the species equilibria. The novel true dual beam system, which is based on an excimer laser driven dye laser and optical cells mounted on piezoelectric detectors, has high sensitivity and stability, and is capable of detecting Am(III) at ca 10 -8 M and Np(IV), (V) and (VI) at ca 10 -7 M. Samples can be measured in an inert atmosphere glove box which helps to maintain the anaerobic conditions expected in deep waste repositories. To date, LIPAS has been used to measure actinide species directly in solutions from waste programmes and to observe americium and neptunium species in solutions of varying Eh, pH and carbonate concentration. The information gained is being used to validate the data used in the geochemical/thermodynamic codes used to predict possible radionuclide species within a radioactive waste repository. (author)

  15. The development of a laser-induced photoacoustic facility for actinide speciation

    International Nuclear Information System (INIS)

    Ewart, F.T.; McMillan, J.W.; Thomason, H.P.; Liezers, M.; Pollard, P.M.

    1988-02-01

    A laser induced photoacoustic spectroscopy (LIPAS) facility has been developed at Harwell to measure actinide species in solution with the minimal disturbance of the species equilibria. The novel true dual beam system, which is based on an excimer laser driven dye laser and optical cells mounted on piezoelectric detectors, has high sensitivity and stability, and is capable of detecting Am(III) at ca 10 -8 M and Np(IV), (V) and (VI) at ca 10 -7 M. Samples can be measured in an inert atmosphere glove box which helps to maintain the anaerobic conditions expected in deep waste repositories. To date, LIPAS has been used to measure actinide species directly in solutions from waste programmes and to observe americium and neptunium species in solutions of varying Eh, pH and carbonate concentration. The information gained is being used to validate the data used in the geochemical/thermodynamic codes used to predict possible radionuclide species within a radioactive waste repository. (author)

  16. Lanthanides and actinides extraction by calixarenes containing CMPO groups; Extraction des lanthanides et des actinides au moyen de calixarenes portant des groupements CMPO

    Energy Technology Data Exchange (ETDEWEB)

    Garcia Carrera, A

    2001-07-01

    In the framework of the French program SPIN concerning the radioactive waste management, researches are performed to develop processes allowing the separation of long-lived radioisotopes in order to their transmutation or their specific conditioning. These studies deal with the extraction and the separation of trivalent lanthanides and actinides in acid solution. Many systems ''calixarene-diluent-aqueous phase'' are examined by extraction liquid-liquid and membrane transport. The extraction efficiency and the selectivity of the synthesized calixarene-CMPO and of the CMPO are compared with these cations, as the nitric acid extraction by these molecules. (A.L.B.)

  17. 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)

  18. 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)

  19. 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

  20. Actinide(IV) and actinide(VI) carbonate speciation studies by PAS and NMR spectroscopies. Yucca Mountain Project: Milestone report 3031-WBS 1.2.3.4.1.3.1

    International Nuclear Information System (INIS)

    Clark, D.L.; Ekberg, S.A.; Morris, D.E.; Palmer, P.D.; Tait, C.D.

    1994-09-01

    Pulsed-laser photoacoustic spectroscopy (PAS) and Fourier-transform nuclear magnetic resonance (NMR) spectroscopy were used to study speciation of actinide(IV) and actinide(VI) ions (Np, Pu, Am) in aqueous carbonate solutions vs of pH, carbonate concentration, actinide content, and temperature. PAS focused on Pu(IV) speciation. Stability fields on a pH (8.4 to 12.0) versus total carbonate content (0.003 to 1.0 M) plot for dilute Pu(IV) carbonate species ([Pu] tot = 1 mM) were mapped. Four plutonium species, with absorption peaks at 486, 492, 500, and 512 nm were found. Loss of a single carbonate ligand does not account for the difference in speciation for the 486 and 492 nm absorption peaks, nor can any of the observed species be identified as colloidal Pu(IV). NMR data have been obtained for UO 2 2+ , PuO 2 2+ and AmO 2 2+ . This report focuses on results for PuO 2 2+ . The ligand exchange reaction between free and coordinated carbonate on the PuO 2 (CO 3 ) 3 4- systems has been examined by variable temperature 13 C NMR spectroscopy. In each of the six different PuO 2 (CO 3 ) 3 4- samples, two NMR signals are present, one for the free carbonate ligand and one for the carbonate ligand coordinated to a paramagnetic plutonium metal center. The single 13 C resonance line for coordinated carbonate is consistent with expectations of a monomeric PuO 2 (CO 3 ) 3 4- species in solution. A modified Carr-Purcell-Meiboom-Gill NMR pulse sequence was used for determining of ligand exchange parameters for paramagnetic actinide complexes. Eyring analysis at standard conditions provided activation parameters of ΔH = 38 KJ/M and ΔS = -60 J/K for the plutonyl triscarbonate system, suggesting an associative transition state for the plutonyl(VI) carbonate complex self-exc

  1. Chemistry of tetravalent actinides phosphates. The thorium phosphate-diphosphate as immobilisation matrix of actinides; Chimie des phosphates d'actinides tetravalents. Le phosphate-diphosphate de thorium en tant que matrice d'imobilisation des actinides

    Energy Technology Data Exchange (ETDEWEB)

    Dacheux, N

    2002-07-01

    The author presents in this document its scientific works from 1992 to 2001, in order to obtain the enabling to manage scientific and chemical researches at the university Paris Sud Orsay. The first part gives an abstract of the thesis on the characterizations, lixiviation and synthesis of uranium and thorium based phosphate matrix in the framework of the search for a ceramic material usable in the radioactive waste storage. The second part presents briefly the researches realized at the CEA, devoted to a reliable, independent and accurate measure of some isotopes activity. The last part presents the abstracts of researches activities from 1996 to 2001 on the tetravalent actinides phosphates chemistry, the sintering of PDT and solid solutions of PDTU and the kinetic and thermodynamical studies of the PDT dissolution. Many references and some publication in full text are provided. (A.L.B.)

  2. 44th Journées des Actinides and 10th SPCA. Scientific Programme and Abstracts

    International Nuclear Information System (INIS)

    2014-01-01

    In the opening Session for the 10th SPCA the program of the school will be presented.The sessions of the 10th SPCA are: Physics, Chemistry,Theory, electronic structure,Nuclear forensics, Measuring systems. While the 10th SPCA lectures on crystallography, Physics, Chemistry and basics of actinides research

  3. Solubility and speciation of actinides in salt solutions and migration experiments of intermediate level waste in salt formations

    International Nuclear Information System (INIS)

    1986-01-01

    A comprehensive study into the solubility of the actinides americium and plutonium in concentrated salt solutions, the release of radionuclides from various forms of conditioned ILW and the migration behaviour of these nuclides through geological material specific to the Gorleben site in Lower Saxony is described. A detailed investigation into the characterization of four highly concentrated salt solutions in terms of their pH, Eh, inorganic carbon contents and their densities is given and a series of experiments investigating the solubility of standard americium(III) and plutonium(IV) hydroxides in these solutions is described. Transuranic mobility studies for solutions derived from the standard hydroxides through salt and sand have shown the presence of at least two types of species present of widely differing mobility; one migrating with approximately the same velocity as the solvent front and the other strongly retarded. Actinide mobility data are presented and discussed for leachates derived from the simulated ILW in cement and data are also presented for the migration of the fission products in leachates derived from real waste solidified in cement and bitumen. Relatively high plutonium mobilities were observed in the case of the former and in the case of the real waste leachates, cesium was found to be the least retarded. The sorption of ruthenium was found to be largely associated with the insoluble residues of the natural rock salt rather than the halite itself. (orig./RB)

  4. Behaviour of trivalent actinides and lanthanide elements in chloride solution; Comportement des lanthanides et transuraniens trivalents en milieu chlorhydrique

    Energy Technology Data Exchange (ETDEWEB)

    Marin, B [Commissariat a l' Energie Atomique, Fontenay-aux-Roses (France). Centre d' Etudes Nucleaires

    1969-07-01

    The aim of this work is to compare the complexation in chloride solutions of trivalent lanthanides and actinides. We have first studied the solvatation of these cations without complexation. We found a difference between Am, Cm and Rare Earths (we can separate lanthanides into Light and Heavy Rare Earths). For studying the complexation we choose the technic of electrophoresis on paper after establishing a simple theory of mobilities in complex solutions. The hydrolysis of these cations was studied and compared in chloride solutions. We have then studied the complexation with the Cl{sup -} ligand in some solutions: HCl, NH{sub 4}Cl, CaCl{sub 2}, CeCl{sub 3}, LiCl. We have established that the complexation is the same in dilute HCl solutions but in concentrated solutions the trivalent actinides are more complexed. This difference is sharper in LiCl solutions. We also proposed the different models of complex in these solutions. (author) [French] Le but de ce travail est de comparer les transuraniens et lanthanides trivalents au point de vue de leur complexation en solution chlorhydrique. Nous avons ete amenes tout d'abord a etudier la solvatation de ces cations non complexes. C'est ainsi que nous pouvons constater une difference entre Am, Cm et les lanthanides. Ces derniers pouvant se separer en lanthanides legers et lanthanides lourds. Pour etudier la complexation nous avons utilise l'electrophorese sur papier apres avoir donne une theorie simple des mobilites en milieu complexant. Apres avoir etudie et compare l'hydrolyse de ces divers cations en solution chlorhydrique, nous avons etudie leur complexation avec l'ion Cl{sup -} dans dans divers milieux: HCl, NH{sub 4}Cl, CaCl{sub 2}, CeCl{sub 3}, LiCl. ous avons note qu'en solution HCl les deux series se comportent de la meme facon pour des concentrations faibles en Cl{sup -} mais que les transuraniens se complexent plus fortement dans les solutions concentrees. Cette difference s'accroit encore dans les milieux

  5. Safe management of actinides in the nuclear fuel cycle: Role of mineralogy; La gestion des actinides dans le cycle du combustible nucleaire: le role de la mineralogie

    Energy Technology Data Exchange (ETDEWEB)

    Ewing, R.C. [Department of Nuclear Engineering and Radiological Sciences, Department of Geological Sciences, Department of Materials Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109-1005 (United States)

    2011-02-15

    During the past 60 years, more than 1800 metric tonnes of Pu, and substantial quantities of the 'minor' actinides, such as Np, Am and Cm, have been generated in nuclear reactors. Some of these transuranium elements can be a source of energy in fission reactions (e.g., {sup 239}Pu), a source of fissile material for nuclear weapons (e.g., {sup 239}Pu and {sup 237}Np), and of environmental concern because of their long-half lives and radiotoxicity (e.g., {sup 239}Pu and {sup 237}Np). There are two basic strategies for the disposition of these heavy elements: (1) to 'burn' or transmute the actinides using nuclear reactors or accelerators; (2) to 'sequester' the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, especially isometric pyrochlore, A{sub 2}B{sub 2}O{sub 7} (A rare earths; B = Ti, Zr, Sn, Hf), for the immobilization of actinides, particularly plutonium, both as inert matrix fuels and nuclear waste forms. Systematic studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high doses of alpha-decay event damage. Recent developments in our understanding of the properties of heavy element solids have opened up new possibilities for the design of advanced nuclear fuels and waste forms. (author)

  6. The reprocessing-recycling of spent nuclear fuel. Actinides separation - Application to wastes management; Le traitement-recyclage du combustible nucleaire use. La separation des actinides - Application a la gestion des dechets

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2008-07-01

    After its use in the reactor, the spent fuel still contains lot of recoverable material for an energetic use (uranium, plutonium), but also fission products and minor actinides which represent the residues of nuclear reactions. The reprocessing-recycling of the spent fuel, as it is performed in France, implies the chemical separation of these materials. The development and the industrial implementation of this separation process represent a major contribution of the French science and technology. The reprocessing-recycling allows a good management of nuclear wastes and a significant saving of fissile materials. With the recent spectacular rise of uranium prices, this process will become indispensable with the development of the next generation of fast neutron reactors. This book takes stock of the present and future variants of the chemical process used for the reprocessing of spent fuels. It describes the researches in progress and presents the stakes and recent results obtained by the CEA. content: the separation of actinides, a key factor for a sustainable nuclear energy; the actinides, a discovery of the 20. century; the radionuclides in nuclear fuels; the aquo ions of actinides; some redox properties of actinides; some complexing properties of actinide cations; general considerations about treatment processes; some characteristics of nuclear fuels in relation with their reprocessing; technical goals and specific constraints of the PUREX process; front-end operations of the PUREX process; separation and purification operations of the PUREX process; elaboration of finite products in the framework of the PUREX process; management and treatment of liquid effluents; solid wastes of the PUREX process; towards a joint management of uranium and plutonium: the COEX{sup TM} process; technical options of treatment and recycling techniques; the fuels of generation IV reactors; front-end treatment processes of advanced fuels; hydrometallurgical processes for future fuel

  7. Selective extraction of actinides by calixarenes: application to bioassay analysis; Extraction selective des actinides par les calixarenes: application a l'analyse radiotoxicologique

    Energy Technology Data Exchange (ETDEWEB)

    Boulet, B

    2006-01-15

    In the context of nuclear workers monitoring, the aim of this PhD was to selectively isolate U, Pu, and Am from urine to propose a new analytical procedure to the Medical and Biology Analysis Laboratories. The 1,3,5-OCH{sub 3}-2,4,6-OCH{sub 2}CONHOH-p-tert-butyl-calix[6]arene molecule has been selected as a promising extractant for U, Pu, and Am. Its physico-chemical properties and its affinity for UO{sub 2}{sup 2+} have been studied through two approaches, one theoretical (molecular modelling at DFT level), and one experimental. The extractions of the three actinides by the hydroxamic calix[6]arene were quantitative in liquid-liquid and solid-liquid systems. Their separation has also been shown possible and efficient. After optimization, the proposed procedure should allow the laboratories to carry out the chemical treatment of urine, before the measurement, in one day instead of the three days needed nowadays. (author)

  8. Dissolution of britholites and monazite / brabantite solid solutions doped with actinides; Etude de la dissolution de britholites et de solutions solides monazite / brabantite dopees avec des actinides

    Energy Technology Data Exchange (ETDEWEB)

    Du Fou De Kerdaniel, E

    2007-12-15

    In the field of the radwaste storage in underground repository, several matrices were considered as promising ceramics for the specific immobilization of actinides. Two of them, britholites and monazite/ brabantite solid solution, have been considered during this work. In order to examine the dissolution mechanisms occurring at the solid liquid interface, several leaching experiments have been conducted on (Ln{sup III}PO{sub 4} ), brabantite (Ca{sup II}An{sup IV}(PO{sub 4}){sub 2}: An = Th, U) and britholites (Ca{sub 9}Nd{sub 0.5}An{sub 0.5}{sup IV} (PO{sub 4}){sub 4.5}(SiO{sub 4}){sub 1.5}F{sub 2}: An = Th, U). Some steady experiments, performed in under saturation conditions for various pH and temperature conditions allowed to evaluate the long term behaviour of such matrices through their chemical durability. On the contrary, the thermodynamic equilibria were examined through the leaching experiments performed near the saturation conditions. By the way, various secondary phases, precipitated onto the surface of altered samples have been identified and characterized. Among them, the (Nd, Ca, Th) - rhabdophane, novelly prepared in over- saturation experiments for a thorium weight loading lower than 11 % appeared to be metastable. Indeed, it turns into TPHPH (Th{sub 2}(PO{sub 4}){sub 2}HPO{sub 4}.H{sub 2}O) and Nd - rhabdophane (NdPO{sub 4}.1/2H{sub 2}O) when increasing leaching time. (author)

  9. Influence of natural organic matter on the speciation of radionuclides in a geochemistry context; Influence de la matiere organique naturelle sur la speciation des radionucleides en contexte geochimique

    Energy Technology Data Exchange (ETDEWEB)

    Marang, L

    2007-09-15

    The principal aim of this work is the study of the influence of natural organic matter, in particularly humic substances (HS), on the speciation of radionuclides (RN). The studied radionuclides are cobalt (II), europium (III) and uranium (VI). It has been shown that mobility and bioavailability of a metal are related to its speciation. The NICA-Donnan model describes metal ion binding to NOM: it accounts for NOM chemical heterogeneity, competition during binding and ionic strength effects. However the model has been calibrated with a limited number of experimental data for the RN. Indeed there is only a few speciation technique available for the study of the interactions RN-HS. Within the framework of this study, we have developed and optimised speciation technique (Flux Donnan Membrane Technique and the use of an un-solubilized humic acid) in order to acquire new experimental data, we have also studied the effect of the competition on RN speciation and finally we have tested the model capacity to predict the RN behavior in laboratory or in situ. (author)

  10. 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

  11. Etude structurale et propriétés des verres peralumineux de conditionnement des produits de fission et actinides mineurs"

    OpenAIRE

    Gasnier , Estelle

    2013-01-01

    In this work, peraluminous glasses (lack of alkaline and alkaline earth ions regarding aluminum) are under study to assess the potentiality of these matrices to confine fission products and minor actinides (FPA) at higher rate than current R7T7 glass (18,5 wt % FPA). The first part of this work aims at studying the physical and chemical properties of complex peraluminous glasses containing increasing FPA rate (18.5 to 32 wt %) to compare them with the specifications. The very low crystallizat...

  12. 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

  13. 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.

  14. Separation by liquid-liquid extraction of actinides(III) from lanthanides(III) using new molecules: the picolinamides; Separation par extraction liquide-liquide des actinides(III) des lanthanides(III) par de nouvelles molecules: les picolinamides

    Energy Technology Data Exchange (ETDEWEB)

    Cordier, P Y [CEA Marcoule, Departement de Recherche en Retraitement et en Vitrification, 30 - Bagnols-sur-Ceze (France); [Clermont-Ferrand-2 Univ., 63 - Aubiere (France)

    1996-07-01

    In the field of long-lived radionuclides separation from waste generated during spent fuel reprocessing, the picolinamides have been chosen as potential extractants for the selective extraction of actinides (III) from lanthanides (III). The first studies initiated on the most simple molecule of the picolinamide family, namely 2-pyridinecarboxamide, pointed out that in an aqueous media the complexation stability constant between this ligand and Am(III) is roughly 10 times higher than the ones corresponding to Ln(III). The synthesis of lipophilic derivatives of 2-pyridinecarboxamide leaded to extraction experiments. The extraction of metallic cation by lipophilic picolinamides, according to a solvatation mechanism, is strongly dependent on the nature of the amide function: a primary amide function (group I) leads to a good extraction; on the contrary, there is a decrease for secondary (group II) and tertiary (group III) amide functions. From a theoretical point of view, this work leads finally to the following conclusions: confirmation of the importance of the presence of soft donor atoms within the extractants (nitrogen in our case) for An(III)/Ln(III). Also, sensitivity of this soft donor atom regarding the protonation reaction; prevalence in our case of the affinity of the extractant for the metallic cation over the lipophilia of the extractant to ensure good distribution coefficients. The extraction and Am(III)/Ln(III) separation performances of the picolinamides from pertechnetic media leads to the design of a possible flowsheet for the reprocessing of high level liquid waste, with the new idea of an integrated technetium reflux. (author) 105 refs.

  15. 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)

  16. 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

  17. 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.

  18. Study of radionuclides speciation with biological molecules of interest by spectrometric techniques; Etude de la speciation des radionucleides avec les molecules d'interet biologique par approche spectrometrique

    Energy Technology Data Exchange (ETDEWEB)

    Lourenco, V

    2007-07-15

    Mechanisms of complexation and accumulation of the radionuclides at the cellular and molecular level are complex and poorly known because the studies on these subjects are scarce. Within the framework of this thesis, we studied the interactions of these cations with biological molecules of interest. We chose to focus on an actinide: uranium (VI) as well as europium as an analogue of trivalent actinides. The selected biological molecules are the phyto-chelatins: their role is to protect cells against intrusions from nonessential heavy metals (thus toxic). These proteins are likely to be implied in the mechanisms of sequestration of radionuclides in living organisms. However, their structure is complex, this is why, in order to better include/understand their reactivity, we extended our studies to lower entities which constitute them (amino acid: glycine, glutamic acid and cysteine; polypeptides: glutathione reduced and oxidized forms). In particular, we determined solution speciation (stoichiometry, structure) as well as the complexing constants associated with the formation with these species. These studies were undertaken by Time Resolved Laser induced Fluorescence (TRLIF), Electro-Spray-Mass Spectrometry (ES-MS), Nuclear Magnetic Resonance (NMR), Fourier Transform Infra-Rouge spectroscopy (FTIR) and Extended X-ray Absorption Fine Structure Spectroscopy (EXAFS).The determination of the complexation constants enabled us to conclude that the complexing capacity of these molecules with respect to radionuclides was moderate (log{sub 10}K{sub 1} {<=} 3, pH 3 or 6), the formed species are mononuclear with only one ligand molecule (1:1). The interaction is performed via oxygenated (hard) groups. The direct complexation of europium with phyto-chelatins at acidic pH was studied jointly by TRLIF and ES-MS. The complexing capacity of these molecules is much higher than that of GSH from which they result. The interaction of europium with metallothioneins is, on the contrary

  19. 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)

  20. 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.

  1. 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

  2. Review and needs in actinide chemistry in relation with biological purposes

    Energy Technology Data Exchange (ETDEWEB)

    Ansoborlo, E.; Moulin, V.; Bion, L.; Doizi, D.; Moulin, C.; Cote, G.; Madic, C.; Van der Lee, J

    2004-07-01

    In case of accidental release of radionuclides in the environment, actinides could occur and may present an healthy risk for human beings. In order to study their behavior in human organism (metabolism, retention, excretion), it is of prime importance to know solution actinide chemistry, and more particularly thermodynamic constants, which will allow to determine their speciation: speciation governs biological availability and toxicity of elements and is also of great interest for decorporation purposes. In this framework, a CEA working group on speciation has been created in order to share data both on thermodynamic constants and on speciation analytical methods, interesting chemists, environmentalists and biologists. It has been focused, in a first time, on actinides. The purpose of this paper is to present the state of the art on actinide speciation within biological media and to focus on the lack of information in order to orientate future research. (authors)

  3. 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)

  4. Study of the actinide-lanthanide separation from nuclear waste by a new pyrochemical process; Etude de la separation actinides-lanthanides des dechets nucleaires par un procede pyrochimique nouveau

    Energy Technology Data Exchange (ETDEWEB)

    Lemort, F. [CEA Marcoule, Departement de Retraitement, des Dechets et du Demantelement, 30 - Bagnols-sur-Ceze (France)]|[Institut National Polytechnique, 38 - Grenoble (France)

    1997-01-01

    The theoretical extraction and separation of platinoids, actinides and lanthanides is allowed by thermodynamic using two adapted reducing agents: zinc and magnesium. Thereby, a pyrochemical method for the nuclear waste processing has been devised. The high temperature handling of the elements in fluoride forms and their processing by a reactive metallic phase required special precautions. The study of the behavior of matter in exploratory systems allowed the development of an experimental technology for the treatment and contacting of phases. The thermodynamical analysis of the experimental results shows the feasibility of the process. A model was developed to predict the distribution coefficients of zirconium, uranium and lanthanum as a function of the system composition. An estimation method was proposed in order to evaluate the distribution coefficients in diluted solution of all the actinides and lanthanides existing in the fission products between LiF CaF{sub 2} and Zn-Mg at 720 deg C. Coupled with the experimental results, the estimates results may be extrapolated to concentrated solutions allowing predictions of the separation of all actinides and lanthanides. The rapidity of element transfer is induced by a thermal effect caused by the high exothermicity of the reduction by magnesium. The kinetic coefficients have been linked with the reduction enthalpy of each element. Moreover, the kinetics seem limited by chemical reaction and not by mass transfer. (author) 66 refs.

  5. Study of irradiation effects in perovskite: use of this matrix for actinides conditioning; Effets de l'irradiation dans une perovskite: utilisation de cette matrice pour un conditionnement des actinides

    Energy Technology Data Exchange (ETDEWEB)

    Sabathier, C

    2003-07-01

    The aim of this work is to study a specific conditioning matrix (ceramics) for actinides: the strontium titanate. At first, the choice of strontium titanate is discussed as well as its structure and its ability to incorporate actinides. The different studies carried out on the irradiation effects on the strontium titanate are reviewed. The main ion-matter interactions considered in the energy range used during our experiments are given. The different devices and techniques used with ion beams to carry out our experiments according to the type of sample: monocrystal or polycrystal are described. The experimental results on the behaviour of strontium titanate in terms of irradiation, temperature and ion flux used to damage the matrix are presented. The experimental results on the different steps of strontium titanate annealing are given as well as the identifying of the defects by different analyses techniques (Rutherford backscattering spectroscopy, transmission electron spectroscopy and x-rays spectroscopy). At last, a model of the behaviour of the strontium titanate in the case of an actinide conditioning is proposed and the evolving of the strontium titanate disorder during the storage is discussed. (O.M.)

  6. 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.)

  7. 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)

  8. Measurements of the neutron capture cross sections and incineration potentials of minor-actinides in high thermal neutron fluxes: Impact on the transmutation of nuclear wastes; Mesures des sections efficaces de capture et potentiels d'incineration des actinides mineurs dans les hauts flux de neutrons: Impact sur la transmutation des dechets

    Energy Technology Data Exchange (ETDEWEB)

    Bringer, O

    2007-10-15

    This thesis comes within the framework of minor-actinide nuclear transmutation studies. First of all, we have evaluated the impact of minor actinide nuclear data uncertainties within the cases of {sup 241}Am and {sup 237}Np incineration in three different reactor spectra: EFR (fast), GT-MHR (epithermal) and HI-HWR (thermal). The nuclear parameters which give the highest uncertainties were thus highlighted. As a result of fact, we have tried to reduce data uncertainties, in the thermal energy region, for one part of them through experimental campaigns in the moderated high intensity neutron fluxes of ILL reactor (Grenoble). These measurements were focused onto the incineration and transmutation of the americium-241, the curium-244 and the californium-249 isotopes. Finally, the values of 12 different cross sections and the {sup 241}Am isomeric branching ratio were precisely measured at thermal energy point. (author)

  9. Hybrid conducting polymer materials incorporating poly-oxo-metalates for extraction of actinides; Materiaux polymeres conducteurs hybrides incorporant des polyoxometallates pour l'extraction d'actinides

    Energy Technology Data Exchange (ETDEWEB)

    Racimor, D

    2003-09-15

    The preparation and characterization of hybrid conducting polymers incorporating poly-oxo-metalates for extracting actinides is discussed. A study of the coordination of various lanthanide cations (Ce(III), Ce(IV), Nd(III)) by the mono-vacant poly-oxo-metalate {alpha}{sub 2}-[P{sub 2}W{sub 17}O{sub 61}]{sup 10-} showed significant differences according to the cation.. Various {alpha}-A-[PW{sub 9}O{sub 34}(RPO){sub 2}]{sup 5-} hybrids were synthesized and their affinity for actinides or lanthanides was demonstrated through complexation. The first hybrid poly-oxo-metallic lanthanide complexes were then synthesized, as was the first hybrid functionalized with a pyrrole group. The electro-polymerization conditions of this pyrrole remain still to be optimized. Poly-pyrrole materials incorporating {alpha}{sub 2}-[P{sub 2}W{sub 17}O{sub 61}]{sup 10-} or its neodymium or cerium complexes as doping agents proved to be the first conducting polymer incorporating poly-oxo-metalates capable of extracting plutonium from nitric acid. (author)

  10. Speciation and evolution of cyanide compounds contained in industrial residues from coal pyrolysis; Speciation et evolution des composes cyanures contenus dans des residus industriels issus de la pyrolyse de la houille

    Energy Technology Data Exchange (ETDEWEB)

    Proffit, D.

    2002-10-15

    Occurrence of cyanide compounds, mainly [Fe(CN)6]2-/3-, in soils and groundwater is due to industrial waste deposits. The main polluting source are purifier wastes stored on former manufactured gas plant sites. In order to estimate the environmental risks associated with cyanide, a specific analytical procedure combining analyses on the solids (optical and scanning electron microscopies, infrared spectroscopy and x-ray diffraction) with analyses carried out on leachates obtained by aqueous extraction at various pHs was developed. For a given purifier waste, Prussian blue was evidenced as the major cyanide species but other minor compounds were also observed. Some of them are extremely soluble (e.g. potassium ferrocyanide) whereas others are very stable (e.g. potassium and zinc ferrocyanide). The study of other polluted solids allowed to predict the hazards linked with their storage. Measurements realized on percolation columns effluents revealed that cyanide species can migrate as colloidal species as well as under soluble forms, which confirmed some site observations where cyanide pollution was observed in soils located beneath a priori stable wastes. Such a combination of techniques can then be considered as a useful diagnosis and risk assessment tool. However, as the full procedure is rather time-consuming a partial combination of the techniques developed can even be used advantageously in some specific cases. We also developed a quantification and speciation method (spectrometric UV-Visible - mathematical code) to determine cyanide compounds concentrations in water extraction filtrates. Finally, irradiation tests of purifier wastes were carried out. They revealed that the influence of natural light could be considered as negligible in comparison to the other factors affecting cyanide compounds migration.

  11. 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)

  12. Interaction of actinides with natural microporous materials

    International Nuclear Information System (INIS)

    Misaelides, P.; Godelirsas, A.

    1998-01-01

    The existing studies mainly concern the sorption of thorium, uranium, neptunium, plutonium and americium 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 applied for this purpose include, except the conventional wet-chemical and radiochemical methods, 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 waters 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. This contribution will critically review of the existing literature, present recently obtained unpublished results and discuss the necessity of future work in the field. (authors)

  13. 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)

  14. Actinide metal processing

    International Nuclear Information System (INIS)

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

    1992-01-01

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

  15. 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.

  16. 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.

  17. Solid state synthesis and sintering of monazite-type ceramics: application to minor actinides conditioning; Synthese par voie solide et frittage de ceramiques a structure monazite. Application au conditionnement des actinides mineurs

    Energy Technology Data Exchange (ETDEWEB)

    Bregiroux, D

    2005-11-15

    In the framework of the French law of 1991 concerning the nuclear waste management, several studies are undertaken to develop specific crystalline conditioning matrices. Monazite, a rare earth (TR{sup 3+}) orthophosphate with a general formula TR{sup 3+}PO{sub 4}, is a natural mineral containing significant amount of thorium and uranium. Monazite has been proposed as a host matrix for the minor actinides (Np, Am and Cm) specific conditioning, thanks to its high resistance to self irradiation and its low solubility. Its is now of prime importance to check the conservation of these properties on synthesized materials, which implies to master all the stages of the elaboration process, from the powder synthesis to the sintering of controlled microstructure pellets. This work can be divided into two main parts: The first part deals with the synthesis by high temperature solid state route of TR{sup 3+}PO{sub 4} powders (with TR{sup 3+} = La{sup 3+} to Gd{sup 3+}, Pu{sup 3+} and Am{sup 3+}). The chemical reactions occurring during the firing of starting reagents are described in the case of monazite with only one or several cations. From these results, a protocol of synthesis is described. The incorporation of tetravalent cations (Ce{sup 4+}, U{sup 4+}, Pu{sup 4+}) in the monazite structure was also studied. The second part of the present work deals with the elaboration of controlled density and microstructure monazite pellets and their related mechanical and thermal properties. The study of crushing and sintering is presented. For the first time, experimental results are confronted with theoretical models in order to deduce the densification and grain growth mechanisms. By the comprehension of the various physicochemical phenomena occurring during the various stages of the monazite pellets elaboration process (powder synthesis, crushing, sintering...), this work allowed the development of a protocol of elaboration of controlled microstructure monazite TR{sup 3+}PO{sub 4

  18. Speciation analysis of radionuclides in the environment. NKS-B speciation project report 2007

    Energy Technology Data Exchange (ETDEWEB)

    Xiaolin Hou (Technical Univ. of Denmark, Risoe National Lab. for Sustainable Energy, Roskilde (Denmark)); Aldahan, A. (Uppsala Univ., Dept. of Earth Science, Uppsala (Sweden)); Possnert, G. (Uppsala Univ., Tandem Lab., Uppsala (Sweden)); Lujaniene, G. (Institute of Physics, Vilnius (Lithuania)); Lehto, J. (Univ. of Helsinki, Dept. of Chemistry, Helsinki (Finland)); Salbu, B. (Norwegian Univ. of Life Sciences (UMB), AAs (Norway))

    2008-07-15

    This report describes the work carried out under the NUK-B project SPECIATION 2007. In 2007, the project partners had two meeting in April and November, organized a NUK seminar on speciation and hot particles. SPECIATION 2007 t mainly focused on two issues on speciation (1) further development of speciation methods for radionuclides, and (2) investigation of speciation of radionuclides in environment. The report summarized the work done in partners labs, which includes: (1) Further development on the speciation of 129I and 127I in water samples; (2) Speciation method for 129I and 127I in air; (3) Dynamic system for fractionation of Pu and Am in soil and sediment; (4) Investigation on Re-absorption of Pu during the fractionation of Pu in soil and sediment; (5) Speciation of 129I in North Sea surface water; (6) Partition of 137Cs and 129I in the Nordic lake sediment, pore-water and lake water; (7) Sequential extraction of Pu in soil, sediment and concrete samples, (8) Pu sorption to Mn and Fe oxides in the geological materials, (10) Investigation of the adsorbed species of lanthanides and actinides on clays surfaces. In addition, two review articles on the speciation of plutonium and iodine in environmental are planned to be submitted to an international journal for publication. (au)

  19. Speciation analysis of radionuclides in the environment. NKS-B speciation project report 2007

    International Nuclear Information System (INIS)

    Hou, Xiaolin; Aldahan, A.; Possnert, G.; Lujaniene, G.; Lehto, J.; Salbu, B.

    2008-07-01

    This report describes the work carried out under the NUK-B project SPECIATION 2007. In 2007, the project partners had two meeting in April and November, organized a NUK seminar on speciation and hot particles. SPECIATION 2007 t mainly focused on two issues on speciation (1) further development of speciation methods for radionuclides, and (2) investigation of speciation of radionuclides in environment. The report summarized the work done in partners labs, which includes: (1) Further development on the speciation of 129I and 127I in water samples; (2) Speciation method for 129I and 127I in air; (3) Dynamic system for fractionation of Pu and Am in soil and sediment; (4) Investigation on Re-absorption of Pu during the fractionation of Pu in soil and sediment; (5) Speciation of 129I in North Sea surface water; (6) Partition of 137Cs and 129I in the Nordic lake sediment, pore-water and lake water; (7) Sequential extraction of Pu in soil, sediment and concrete samples, (8) Pu sorption to Mn and Fe oxides in the geological materials, (10) Investigation of the adsorbed species of lanthanides and actinides on clays surfaces. In addition, two review articles on the speciation of plutonium and iodine in environmental are planned to be submitted to an international journal for publication. (au)

  20. Monazite-type ceramics for the immobilization of minor actinides plutonium; Keramiken des Monazit-Typs zur Immobilisierung von minoren Actinoiden und Plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Heuser, Julia Maria

    2015-07-01

    The safe disposal of radioactive waste in deep geological formations is a challenging task of present and future generations. Innovative strategies as the conditioning of radionuclides in ceramic matrices can make a contribution here. This work points out monazite-type ceramics as potential waste forms for minor actinides and Pu. Several aspects concerning nuclear disposal as well as fundamental structural information were investigated. Lanthanide phosphate endmembers (LnPO{sub 4}) within the stability field of monazite (Ln = La-Gd) were synthesised within the scope of this work. To extend the knowledge of monazite phases, monoclinic TbPO{sub 4}- and DyPO{sub 4}-phases were prepared and characterised. Tb- and Dy-phosphates are situated in the xenotime stability field close to that of monazite. They can exist as metastable monazite phases. Structural characterisations of long- and short-range order were performed by X-ray diffraction, infrared (IR) and Raman spectroscopy. Structural data could be complemented, enhanced and gaps of knowledge could be filled by the first systematic consideration of the complete Ln-monazite-series (Ln = La-Dy). Furthermore, this work focuses on Sm-monazite phases. Samarium with an atomic number of 62 is located in the middle part of the lanthanides showing the monazite structure. Accordingly, it has a mean cationic radius within the Ln-monazite-series and hence shows a relative high flexibility regarding the incorporation of radionuclides with different radii. Sintering densities of SmPO{sub 4} ceramics were optimised by varying process parameters like pressure and number of pressing steps. An irregular texture as well as densities of 94% of the theoretical value could be achieved. The resistance of Sm-monazite against ionising radiation were examined. Radiation damages caused by the α-decay of radionuclides incorporated in a ceramic matrix were simulated by computer calculations and experimentally by heavy ion bombardment of Sm

  1. Partitioning of the rare earths and actinides between R7T7 nuclear glass alteration products and solution according to disposal conditions; Partage des terres rares et des actinides entre solution et produits d`alteration du verre nucleaire type R7T7 en fonction des conditions de stockage

    Energy Technology Data Exchange (ETDEWEB)

    Menard, O

    1995-10-25

    The alteration of nuclear glass by water is liable to release radionuclides into the environment. Determining the release kinetics of these elements and their aqueous chemical forms are therefore essential steps in establishing the safety of a geological repository site. Leach tests were conducted with a nonradioactive specimen of the French ``R7T7`` light water containment glass spiked with U and Th, and with two R7T7 specimens spiked with {sup 237}Np and {sup 239}Pu, respectively. The alteration solution compositions were representative of deep groundwater and contained carbonate, sulfate, phosphate, fluorine and chlorine ions. The release of U, Th, Np and Pu, as well as of the rare earths La, Ce and Nd were monitored by ICP mass spectrometry and by {alpha} spectrometry. Scanning and transmission electron microscopic examination of the nonradioactive altered glass surfaces was also performed to assess the partitioning balance for the rare earths, U and Th between the glass alteration products and solution. The mobility of these elements depends on two competing mechanisms. The rare earths and thorium are incorporated in the alteration products (gel); the retention process is assumed to involve chemisorption or coprecipitation, enhanced in the gel layer by the presence of phosphate ions in particular. Conversely, the aqueous species in the alteration solutions (mainly anions) form complexes with the actinides and rare earths; this phenomenon is particularly evident with U and Np. The presence of carbonate ions favors this mobility. Plutonium differs from U and Np in that it is adsorbed mainly on colloids formed by glass dissolution, the principal factors governing its chemical evolution in solution. (author). refs., 122 figs., 185 tabs.

  2. Development of speciation analysis for selenium in nutritional supplements by the determination of the seleno-methionine; Developpement de l'analyse de speciation du selenium dans des complements alimentaires par la determination de la selenomethionine

    Energy Technology Data Exchange (ETDEWEB)

    Sannac, S.; Labarraque, G.; Fisicaro, P. [Laboratoire National de Metrologie et d' Essai (LNE), 75 - Paris (France); Sannac, S.; Pannier, F.; Potin-Gautier, M. [Pau Univ. et des Pays de l' Adour, CNRS/UMR 5254, Lab. de Chimie Analytique, Bio-Inorganique et Environnement (IPREM), 64 (France)

    2009-07-01

    The development of a reference method in analytical chemistry is presented. Liquid chromatography with inductively coupled plasma mass spectrometry is employed to perform in speciation analysis. Applications are developed for the determination of seleno-methionine in nutritional supplements. The use of isotope dilution, a primary method, is required to enable measurement traceability. Method validation is ensured by the study of a certified reference material. (authors)

  3. Radionuclide speciation in the environment: a review

    International Nuclear Information System (INIS)

    Moulin, V.; Moulin, C.

    2001-01-01

    Speciation determination is of prime importance to explain and evaluate the mobility, the toxicity and the risk resulting from the presence of trace elements in natural systems, in particular in the case of radionuclides, in the framework of environment and waste management purposes. The present paper will then focus more specifically on the physico-chemical speciation of radionuclides, and more particularly of actinides, in the environment, with emphasis on the behavior in solution: from a chemical point of view (with important ligands including colloidal phases) using experimental data and speciation calculations, as well as from a more technical point of view (with analytical methods for in situ speciation determination and thermodynamic data determination). A review of recent papers (mainly from CEA) is presented. (orig.)

  4. Kinetic of liquid-liquid extraction for uranyl nitrate and actinides (III) and lanthanides (III) nitrates by amide extractants; Cinetique d`extraction liquide-liquide du nitrate d`uranyle et des nitrates d`actinides (III) et de lanthanides (III) par des extractants a fonction amide

    Energy Technology Data Exchange (ETDEWEB)

    Toulemonde, V [CEA Centre d` Etudes Nucleaires de Saclay, 91 -Gif-sur-Yvette (France); [CEA Centre d` Etudes de la Vallee du Rhone, 30 -Marcoule (France). Dept. d` Exploitation du Retraitement et de Demantelement

    1995-12-20

    The kinetics of liquid-liquid extraction by amide extractants have been investigated for uranyl nitrate (monoamide extractants), actinides (III) and lanthanides (III) nitrates (diamide extractants). The transfer of the metallic species from the aqueous phase to the organic phase was studied using two experimental devices: ARMOLLEX (Argonne Modified Lewis cell for Liquid Liquid Extraction) and RSC (Rotating Stabilized Cell). The main conclusions are: for the extraction of uranyl nitrate by DEHDMBA monoamide, the rate-controlling step is the complexation of the species at the interface of the two liquids. Thus, an absorption-desorption (according to Langmuir theory) reaction mechanism was proposed; for the extraction of actinides (III) and lanthanides (III) nitrates in nitric acid media by DMDBTDMA diamide, the kinetic is also limited by interfacial reactions. The behavior of Americium and Europium is very similar as fare as their reaction kinetics are concerned. (author). 89 refs.

  5. 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.

  6. Towards an interpretation of the mechanism of the actinides(III)/lanthanides(III) separation by synergistic solvent extraction with nitrogen-containing polydendate ligands; Vers une interpretation des mecanismes de la separation actinides(III)/lanthanides(III) par extraction liquide-liquide synergique impliquant des ligands polyazotes

    Energy Technology Data Exchange (ETDEWEB)

    Francois, N [CEA/VALRHO - site de Marcoule, Dept. de Recherche en Retraitement et en Vitrification, (DRRV), 30 - Marcoule (France); Universite Henri Poincare, 54 - Vandoeuvre-les-Nancy (France)

    2000-07-01

    In the field of the separation of long-lived radionuclides from the wastes produced by nuclear fuel reprocessing, aromatic nitrogen-containing polydendate ligands are potential candidates for the selective extraction, alone or in synergistic mixture with acidic extractants, of trivalent actinides from trivalent lanthanides. The first part of this work deals with the complexation of trivalent f cations with various nitrogen-containing ligands (poly-pyridine analogues). Time-resolved laser-induced fluorimetry (TRLIF) and UV-visible spectrophotometry were used to determine the nature and evaluate the stability of each complex. Among the ligands studied, the least basic Me-Btp proved to be highly selective towards americium(III) in acidic solution. In the second part, two synergistic systems (nitrogen-containing polydendate ligand and lipophilic carboxylic acid) are studied and compared in regard to the extraction and separation of lanthanides(III) and actinides(III). TRLIF and gamma spectrometry allowed the nature of the extracted complexes and the optimal conditions of efficiency of both systems to be determined. Comparison between these different studies showed that the selectivity of complexation of trivalent f cations by a given nitrogen-containing polydendate ligand could not always be linked to the Am(III)Eu(III) selectivity reached in synergistic extraction. The latter depends on the 'balance' between the acid-basic properties on the one hand, and on the hard-soft characteristics on the other hand, of both components of synergistic system. (author)

  7. Study of the selectivity of poly-nitrogenous extracting molecules in the complexation of actinides (III) and lanthanides (III) in solution in anhydrous pyridine; Etude de la selectivite de molecules extractantes polyazotees dans la complexation des actinides (III) et des lanthanides (III) en solution dans la pyridine anhydre

    Energy Technology Data Exchange (ETDEWEB)

    Riviere, Ch

    2000-10-05

    The aim of this work is to better understand the factors which contribute to the separation of lanthanides(III) and actinides(III). Polydentate nitrogenous molecules present an interesting selectivity. A thermodynamic study of the complexation in pyridine of lanthanide and uranium by the bipyridine ligand (bipy) has been carried out. The formation constants and the thermodynamic values of the different complexes have been determined. It has been shown that the bipy complexes formation is controlled by the enthalpy and unfavored by the entropy. The conductometry has revealed too a significant difference in the uranium and lanthanides complexation by the bipyridine ligand. The use of the phenanthroline ligand induces a better complexation of the metallic ions but the selectivity is not improved. On the other hand, the decrease of the basicity and the increase of the ligand denticity (for instance in the case of the use of ter-pyridine) favour the selectivity without improving the complexation. The selectivity difference for the complexation of actinides(III) and lanthanides(III) by the different studied ligands (independent systems) has been confirmed by experiments of inter-metals competition. (O.M.)

  8. Towards an interpretation of the mechanism of the actinides(III)/lanthanides(III) separation by synergistic solvent extraction with nitrogen-containing polydendate ligands; Vers une interpretation des mecanismes de la separation actinides(III)/lanthanides(III) par extraction liquide-liquide synergique impliquant des ligands polyazotes

    Energy Technology Data Exchange (ETDEWEB)

    Francois, N. [CEA/VALRHO - site de Marcoule, Dept. de Recherche en Retraitement et en Vitrification, (DRRV), 30 - Marcoule (France); Universite Henri Poincare, 54 - Vandoeuvre-les-Nancy (France)

    2000-07-01

    In the field of the separation of long-lived radionuclides from the wastes produced by nuclear fuel reprocessing, aromatic nitrogen-containing polydendate ligands are potential candidates for the selective extraction, alone or in synergistic mixture with acidic extractants, of trivalent actinides from trivalent lanthanides. The first part of this work deals with the complexation of trivalent f cations with various nitrogen-containing ligands (poly-pyridine analogues). Time-resolved laser-induced fluorimetry (TRLIF) and UV-visible spectrophotometry were used to determine the nature and evaluate the stability of each complex. Among the ligands studied, the least basic Me-Btp proved to be highly selective towards americium(III) in acidic solution. In the second part, two synergistic systems (nitrogen-containing polydendate ligand and lipophilic carboxylic acid) are studied and compared in regard to the extraction and separation of lanthanides(III) and actinides(III). TRLIF and gamma spectrometry allowed the nature of the extracted complexes and the optimal conditions of efficiency of both systems to be determined. Comparison between these different studies showed that the selectivity of complexation of trivalent f cations by a given nitrogen-containing polydendate ligand could not always be linked to the Am(III)Eu(III) selectivity reached in synergistic extraction. The latter depends on the 'balance' between the acid-basic properties on the one hand, and on the hard-soft characteristics on the other hand, of both components of synergistic system. (author)

  9. Study and development of a method allowing the identification of actinides inside nuclear waste packages, by active neutron or photon interrogation and delayed gamma-ray spectrometry; Etude et developpement d'une technique de dosage des actinides dans les colis de dechets radioactifs par interrogation photonique ou neutronique active et spectrometrie des gamma retardes

    Energy Technology Data Exchange (ETDEWEB)

    Carrel, F

    2007-10-15

    An accurate estimation of the alpha-activity of a nuclear waste package is necessary to select the best mode of storage. The main purpose of this work is to develop a non-destructive active method, based on the fission process and allowing the identification of actinides ({sup 235}U, {sup 238}U, {sup 239}Pu). These three elements are the main alpha emitters contained inside a package. Our technique is based on the detection of delayed gammas emitted by fission products. These latter are created by irradiation with the help of a neutron or photon beam. Performances of this method have been investigated after an Active Photon or Neutron Interrogation (INA or IPA). Three main objectives were fixed in the framework of this thesis. First, we measured many yields of photofission products to compensate the lack of data in the literature. Then, we studied experimental performances of this method to identify a given actinide ({sup 239}Pu in fission, {sup 235}U in photofission) present in an irradiated mixture. Finally, we assessed the application of this technique on different mock-up packages for both types of interrogation (118 l mock-up package containing EVA in fission, 220 l mock-up package with a wall of concrete in photofission). (author)

  10. 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.

  11. 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

  12. Speciation from photon to ion detection

    International Nuclear Information System (INIS)

    Moulin, C.

    2001-01-01

    New analytical techniques allowing to perform speciation in the framework of the nuclear fuel cycle are more and more needed. Among them, several laser-based analytical techniques present several advantages (non intrusive). Hence, Thermal Lensing (TL)/Photoacoustic (LIPAS), Time Resolved selective, sensitive Laser-Induced Fluorescence (TRLIF) have been used for actinides/lanthanides interaction and speciation studies in inorganic and organic matrices, Laser Ablation-Optical Emission Spectroscopy (LA-OES or LIBS) for direct studies on solids, liquids,... where in situ measurements (elemental or isotopic) are mandatory. In complementary to these photon-based methods, new ion detection methods such as ElectroSpray-Mass Spectrometry (ES-MS) seems promising for speciation studies. Principle, advantages and limitations as well as results obtained and trends for these different methods will be presented. (author)

  13. 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

  14. Study of extraction kinetics of lanthanides(III) and actinides(III) nitrates by the molecule N, N'-dimethyl-N, N'-dibutyl, tetradecylmalonamide; Etude des cinetiques d'extraction des nitrates de lanthanides (III) et d'actinides (III) par le malonamide N, N'-dimethyl-N, N'-dibutyl, tetradecylmalonamide

    Energy Technology Data Exchange (ETDEWEB)

    Daldon, M

    1999-07-01

    The kinetics of extraction of lanthanides (III) and actinides (III) nitrates by the molecule N, N'-dimethyl - N, N'-dibutyl tetra-decyl malonamide has been investigated. This study was realised with a new constant interfacial-area-stirred cell. During the qualification step of the device it appears that the reduction of the device can lead to hydrolytic perturbations. The main conclusions are: - after the determination of conditions which provide kinetics regime (diffusion of species neglectable), partial orders of the kinetics law have been obtained and lead to the establishment of the law J = k [Nd{sup 3+}] [NO{sub 3}{sup -}]{sup 3} [diamide]{sup 1}, - interfacial tension measurements and kinetics study in presence of surface-active compounds proved that the chemical limiting reaction for Nd(III) is interfacial, - the results allow to propose an adsorption-desorption reaction mechanism, - a comprehensive study of the extraction kinetics of the lanthanides(III) series and also Am(III) and Cm(III) nitrates has been realised. The lighter lanthanides (La, Ce and Pr) exhibit higher kinetics rate of extraction than the others, which differs from the tendency observed with distribution coefficients which exhibit tetrad effect. The kinetics rate of extraction of Am(III) and Cm(III) is closed to the value of Eu(III). (author)

  15. 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)

  16. 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

  17. 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)

  18. 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).

  19. 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.)

  20. Application of voxelised numerical phantoms linked to the M.C.N.P. Monte Carlo code to the realistic measurement in vivo of actinides in the lungs and contaminated wounds; Application des fantomes numeriques voxelises associes au code Monte Carlo MCNP a la mesure in vivo realiste des actinides dans les poumons et les plaies contaminees

    Energy Technology Data Exchange (ETDEWEB)

    Noelle, P

    2006-12-15

    In vivo lung counting, one of the preferred methods for monitoring people exposed to the risk of actinide inhalation, is nevertheless limited by the use of physical calibration phantoms which, for technical reasons, can only provide a rough representation of human tissue. A new approach to in vivo measurements has been developed to take advantage of advances in medical imaging and computing; this consists of numerical phantoms based on tomographic images (CT) or magnetic resonance images (R.M.I.) combined with Monte Carlo computing techniques. Under laboratory implementation of this innovative method using specific software called O.E.D.I.P.E., the main thrust of this thesis was to provide answers to the following question: what do numerical phantoms and new techniques like O.E.D.I.P.E. contribute to the improvement in calibration of low-energy in vivo counting systems? After a few developments of the O.E.D.I.P.E. interface, the numerical method was validated for systems composed of four germanium detectors, the most widespread configuration in radio bioassay laboratories (a good match was found, with less than 10% variation). This study represents the first step towards a person-specific numerical calibration of counting systems, which will improve assessment of the activity retained. A second stage focusing on an exhaustive evaluation of uncertainties encountered in in vivo lung counting was possible thanks to the approach offered by the previously-validated O.E.D.I.P.E. software. It was shown that the uncertainties suggested by experiments in a previous study were underestimated, notably morphological differences between the physical phantom and the measured person. Some improvements in the measurement procedure were then proposed, particularly new bio-metric equations specific to French measurement configurations that allow a more sensible choice of the calibration phantom, directly assessing the thickness of the torso plate to be added to the Livermore phantom

  1. 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

  2. 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

  3. Speciation and internal dosimetry: from chemical species to dosimetric models

    International Nuclear Information System (INIS)

    Paquet, F.; Frelon, S.; Cote, G.; Madic, C.

    2004-01-01

    Speciation studies refer to the distribution of species in a particular sample or matrix. These studies are necessary to improve the description, understanding and prediction of trace element kinetics and toxicity. In case of internal contamination with radionuclides, speciation studies could help to improve both the biokinetic and dosimetric models for radionuclides. There are different methods to approach the speciation of radionuclide in a biological system, depending on the degree of accuracy needed and the level of uncertainties accepted. Among them, computer modelling and experimental determination are complementary approaches. This paper describes what is known about speciation of actinides in blood, GI-tract, liver and skeleton and of their consequences in terms of internal dosimetry. The conclusion is that such studies provide very valuable data and should be targeted in the future on some specific tissues and biomolecules. (authors)

  4. The contribution of chemical speciation to internal dosimetry

    International Nuclear Information System (INIS)

    Paquet, F.; Frelon, S.; Cote, G.; Madic, C.

    2003-01-01

    Speciation studies refer to the distribution of species in a particular sample or matrix. These studies are necessary to improve the description, understanding and prediction of trace element kinetics and toxicity. In the case of internal contamination with radionuclides, speciation studies could help to improve both the biokinetic and dosimetric models for radionuclides. There are different methods to approach the speciation of radionuclides in a biological system, depending on the degree of accuracy needed and the level of uncertainties accepted. Among them, computer modelling and experimental determination are complementary approaches. This paper describes what is known about speciation of actinides in blood, GI tract, liver and skeleton and of their consequences in terms of internal dosimetry. The conclusion is that such studies provide very valuable data and should be targeted in the future on some specific tissues and biomolecules. (author)

  5. 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)

  6. 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.)

  7. 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

  8. Plutonium Speciation, Solubilization and Migration in Soils

    International Nuclear Information System (INIS)

    Neu, M.; Runde, W.

    1999-01-01

    This report summarizes research completed in the first half of a three-year project. As outlined in the authors' proposal they are focusing on (1) characterizing the plutonium at an actinide contaminated site, RFETS, including determining the origin, dispersion, and speciation of the plutonium, (2) studying environmentally important plutonium complexes, primarily hydroxides and carbonates, and (3) examining the interactions of plutonium species with manganese minerals. In the first year the authors focused on site based studies. This year they continue to characterize samples from the RFETS, study the formation and structural and spectroscopic features of environmentally relevant Pu species, and begin modeling the environmental behavior of plutonium

  9. Pourbaix diagrams of actinides in molten chlorides using an indicating electrode for oxide ion activity; Etablissement de diagrammes de Pourbaix des actinides dans les chlorures fondus au moyen d'une electrode indicatrice de l'activite des ions oxyde

    Energy Technology Data Exchange (ETDEWEB)

    Lambertin, D.; Lacquement, J. [CEA Valrho, (DCC/DRRV/SPHA), 30 - Marcoule (France)

    2000-07-01

    function of state, since it is only dependent on gas partial pressures. The pO{sup 2-} entity characterizing the melt oxo-acidity is accordingly related to Omega. The knowledge of the equilibrium constant K allows calibration of the pO{sup 2-} scale with respect to the universal Omega scale. Note also that while pO{sup 2-} and pK depend on the melt temperature and composition, this is not the case for the term involving the partial pressures of hydrogen chloride and water, so that Omega can be set independently of the working temperature. Universal potential-acidity diagrams were thus prepared. In the first method, the oxychloride is assumed to be insoluble. We therefore preferred to determine experimentally the stabilities of the element oxychloride and oxide and their physical state (solvated or precipitated) in the melt, considering the second method. For instance, the well-known cerium system was used to validate the YSZM electrode operating procedure, and potentiometric titrations of cerium chloride with carbonate anion serve to characterize the speciation of cerium in the melts as a function of acidity. Similar experiments are planned with plutonium and americium compounds. (author)

  10. 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

  11. 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

  12. Experimental study of kinetic and mechanism of dissolution of apatite structured minerals. Application to the prediction of the long term behavior of an actinides storage host matrix; Etude experimentale de la cinetique et des mecanismes d'alteration de mineraux apatitiques. Application au comportement d'une ceramique de confinement d'actinides mineurs

    Energy Technology Data Exchange (ETDEWEB)

    Chairat, C

    2005-11-15

    The motivation for this study is to assess the potential of using apatite structured ceramics as long-lived actinide storage hosts. To assess their ability to resist aqueous corrosion, the dissolution of natural fluoro-apatite and synthetic Nd-britholite (neodymium is a proxy for the trivalent actinides) was studied. Mineral surfaces were characterized using a combined spectrometric, electrokinetic and potentiometric approach and dissolution rates were measured in closed and open system reactors as a function of solution composition. Experimental results suggest apatitic minerals dissolve via distinct step sequence: 1) fluoride release, 2) release of the calcium situated in the M1, and 3) the simultaneous removal of phosphate and calcium II via the breaking of only Ca-O bonds. TST based rate equations based in this mechanism accurately describe fluoro-apatite and synthetic britholite dissolution rates as a function of solution composition. Nd release rates are limited by precipitation of Nd-rhabdophane. (author)

  13. Investigations of actinides in the context of final disposal of high-level radioactive waste. Trivalent actinides in aqueous solution

    International Nuclear Information System (INIS)

    Banik, N.L.; Boris Brendebach; Marquardt, Ch.M.

    2014-01-01

    The speciation of redox sensitive trivalent actinides Pu(III), Np(III), and U(III) has been studied in aqueous solution. The redox preparation, stabilization, and speciation of these trivalent actinides in aqueous systems are discussed here. The reductants investigated were rongalite, hydroxylamine hydrochloride, and acetohydroxamic acid and the An(III) species have been characterized by UV-Vis and XANES spectroscopy. The results show that the effectiveness of stabilization decreases generally in the order Pu(III) > Np(III) > U(III) and that the effectiveness of each reducing agent depends on the experimental conditions. More than 80 % of Pu(III) aquo species have been stabilized up to pH 5.5, whereas the Np(III) aquo ion could be stabilized in a pH range 0-2.5, and U(III) aquo ion is sufficiently stable at pH 1.0 and below over time periods suitable for experiments. However, this study gives a basis for the characterisation of the trivalent lighter actinides involved in complexation, sorption, and solid formation reactions in the future. (author)

  14. Integration of the metal ion charge neutralization model for humic acid complexation into the geochemical speciation code EQ3/6

    International Nuclear Information System (INIS)

    Brendler, V.

    2002-01-01

    Geochemical modeling often requires the consideration of humics as major complexing agent and colloid. The metal ion charge neutralization model can handle respective interactions and has therefore been integrated into the speciation software EQ3/6. An application showing the influence of the pH-dependence of the loading capacity on actinide speciation is given. (orig.)

  15. Actinide oxide photodiode and nuclear battery

    Energy Technology Data Exchange (ETDEWEB)

    Sykora, Milan; Usov, Igor

    2017-12-05

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

  16. Synthesis and characterization of low-valence actinide phosphide tellurides and ternary selenium-halide iridium complexes; Synthese und Charakterisierung niedervalenter Actinoidphosphidtelluride und ternaerer Selen-Halogenid-Komplexe des Iridiums

    Energy Technology Data Exchange (ETDEWEB)

    Stolze, Karoline

    2016-04-07

    The thesis on the synthesis and characterization of low-valence actinide phosphide tellurides and ternary selenium-halide iridium complexes includes two parts: a description of the experimental synthesis of UPTe and U2PTe2O and ThPTe and the synthesis of selenium-chloride iridium complexes and selenium-bromide iridium complexes. The characterization included X-ray diffraction and phase studies.

  17. Actinide Biocolloid Formation in Brine by Halophilic Bacteria

    Energy Technology Data Exchange (ETDEWEB)

    Gillow, J.B.; Francis, A.J.; Dodge, C.J.; Harris, R.; Beveridge, T.J.; Brady, P.V.; Papenguth, H.W.

    1999-07-28

    We examined the ability of a halophilic bacterium (WFP 1A) isolated from the Waste Isolation Pilot Plant (WIPP) site to accumulate uranium in order to determine the potential for biocolloid facilitated actinide transport. The bacterial cell Surface functional groups involved in the complexation of the actinide were determined by titration. Uranium, added as uranyl nitrate, was removed from solution at pH 5 by cells but at pH 7 and 9 very little uranium was removed due to its limited volubility. Although present as soluble species, uranyl citrate at pH 5, 7, and 9, and uranyl carbonate at pH 9 were not removed by the bacterium because they were not bioavailable due to their neutral or negative charge. Addition of uranyl EDTA to brine at pH 5, 7, and 9 resulted in the immediate precipitation of U. Transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS) analysis revealed that uranium was not only associated with the cell surface but also accumulated intracellulary as uranium-enriched granules. Extended X-ray absorption fine structure (EXAFS) analysis, of the bacterial cells indicated the bulk sample contained more than one uranium phase. Nevertheless these results show the potential for the formation of actinide bearing bacterial biocolloids that are strictly regulated by the speciation and bioavailability of the actinide.

  18. Actinide biocolloid formation in brine by halophilic bacteria

    International Nuclear Information System (INIS)

    Gillow, J.B.; Francis, A.J.; Dodge, C.J.; Harris, R.; Beveridge, T.J.; Brady, P.V.; Papenguth, H.W.

    1999-01-01

    The authors examined the ability of a halophilic bacterium (WIPP 1A) isolated from the Waste Isolation Pilot Plant (WIPP) site to accumulate uranium in order to determine the potential for biocolloid facilitated actinide transport. The bacterial cell surface functional groups involved in the complexation of the actinide were determined by titration. Uranium, added as uranyl nitrate, was removed from solution at pH 5 by cells but at pH 7 and 9 very little uranium was removed due to its limited solubility. Although present as soluble species, uranyl citrate at pH 5, 7, and 9, and uranyl carbonate at pH 9 were not removed by the bacterium because they were not bioavailable due to their neutral or negative charge. Addition of uranyl EDTA to brine at pH 5, 7, and 9 resulted in the immediate precipitation of U. Transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS) analysis revealed that uranium was not only associated with the cell surface but also accumulated intracellularly as uranium-enriched granules. Extended X-ray absorption fine structure (EXAFS) analysis of the bacterial cells indicated the bulk sample contained more than one uranium phase. Nevertheless these results show the potential for the formation of actinide bearing bacterial biocolloids that are strictly regulated by the speciation and bioavailability of the actinide

  19. Actinide Biocolloid Formation in Brine by Halophilic Bacteria

    International Nuclear Information System (INIS)

    Gillow, J.B.; Francis, A.J.; Dodge, C.J.; Harris, R.; Beveridge, T.J.; Brady, P.V.; Papenguth, H.W.

    1999-01-01

    We examined the ability of a halophilic bacterium (WFP 1A) isolated from the Waste Isolation Pilot Plant (WIPP) site to accumulate uranium in order to determine the potential for biocolloid facilitated actinide transport. The bacterial cell Surface functional groups involved in the complexation of the actinide were determined by titration. Uranium, added as uranyl nitrate, was removed from solution at pH 5 by cells but at pH 7 and 9 very little uranium was removed due to its limited volubility. Although present as soluble species, uranyl citrate at pH 5, 7, and 9, and uranyl carbonate at pH 9 were not removed by the bacterium because they were not bioavailable due to their neutral or negative charge. Addition of uranyl EDTA to brine at pH 5, 7, and 9 resulted in the immediate precipitation of U. Transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS) analysis revealed that uranium was not only associated with the cell surface but also accumulated intracellulary as uranium-enriched granules. Extended X-ray absorption fine structure (EXAFS) analysis, of the bacterial cells indicated the bulk sample contained more than one uranium phase. Nevertheless these results show the potential for the formation of actinide bearing bacterial biocolloids that are strictly regulated by the speciation and bioavailability of the actinide

  20. Actinide biocolloid formation in brine by halophilic bacteria

    International Nuclear Information System (INIS)

    Gillow, J.B.; Francis, A.J.; Dodge, C.J.; Harris, R.; Beveridge, T.J.; Brady, P.B.; Papenguth, H.W.

    1998-01-01

    The authors examined the ability of a halophilic bacterium (WIPP 1A) isolated from the Waste Isolation Pilot Plant (WIPP) site to accumulate uranium in order to determine the potential for biocolloid facilitated actinide transport. The bacterial cell surface functional groups involved in the complexation of the actinide were determined by titration. Uranium, added as uranyl nitrate, was removed from solution at pH 5 by cells but at pH 7 and 9 very little uranium was removed due to its limited solubility. Although present as soluble species, uranyl citrate at pH 5, 7, and 9, and uranyl carbonate at pH 9 were not removed by the bacterium because they were not bioavailable due to their neutral or negative charge. Addition of uranyl EDTA to brine at pH 5, 7, and 9 resulted in the immediate precipitation of U. Transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS) analysis revealed that uranium was not only associated with the cell surface but also accumulated intracellularly as uranium-enriched granules. Extended X-ray absorption fine structure (EXAFS) analysis of the bacterial cells indicated the bulk sample contained more than one uranium phase. Nevertheless these results show the potential for the formation of actinide bearing bacterial biocolloids that are strictly regulated by the speciation and bioavailability of the actinide

  1. The INE-Beamline for Actinide Research at ANKA

    Science.gov (United States)

    Brendebach, Boris; Denecke, Melissa A.; Rothe, Jörg; Dardenne, Kathy; Römer, Jürgen

    2007-02-01

    The INE-Beamline for actinide research at the synchrotron source ANKA is now fully operational. This beamline was designed, built, and commissioned by the Institut für Nukleare Entsorgung (INE) at the Forschungszentrum Karlsruhe (FZK), Germany. It is dedicated to actinide speciation investigations related to nuclear waste disposal as well as applied and basic actinide research. Experiments on radioactive samples with activities up to 106 times the limit of exemption inside a safe and flexible double containment concept are possible. The close proximity of the beamline to INE's active laboratories is unique in Europe. Currently, experiments can be performed in an X-ray energy range from around 2.15 keV (P K edge) to 24.35 keV (Pd K edge). The INE-Beamline design is optimized for spectroscopy with emphasis on surface sensitive techniques. A microfocus option is presently being installed at the INE-Beamline. Access to the INE-Beamline is possible through cooperation with INE, through the ANKA proposal system and via the European Network of Excellence for Actinide Sciences (ACTINET).

  2. Actinide recycling in reactors

    International Nuclear Information System (INIS)

    Kuesters, H.; Wiese, H.W.; Krieg, B.

    1995-01-01

    The objective is an assessment of the transmutation of long-lived actinides and fission products and the incineration of plutonium for reducing the risk potential of radioactive waste from reactors in comparison to direct waste disposal. The contribution gives an interim account on homogeneous and heterogeneous recycling of 'risk nuclides' in thermal and fast reactors. Important results: - A homogeneous 5 percent admixture of minor actinides (MA) from N4-PWRs to EFR fuel would allow a transmutation not only of the EFR MA, but in addition of the MA from 5 or 6 PWRs of equal power. However, the incineration is restricted by safety considerations. - LWR have only a very low MA incineration potential, due to their disadvantageous neutron capture/fission ratio. - In order to keep the Cm inventory at a low level, it is advantageous to concentrate the Am heterogeneously in particular fuel elements or rods. (orig./HP)

  3. Photochemistry of the actinides

    International Nuclear Information System (INIS)

    Toth, L.M.; Bell, J.T.; Friedman, H.A.

    1979-01-01

    It has been found that all three major actinides have a useful variety of photochemical reactions which could be used to achieve a separations process that requires fewer reagents. Several features merit enumerating: (1) Laser photochemistry is not now as uniquely important in fuel reprocessing as it is in isotopic enrichment. The photochemistry can be successfully accomplished with conventional light sources. (2) The easiest place to apply photo-reprocessing is on the three actinides U, Pu, and Np. The solutions are potentially cleaner and more amenable to photoreactions. (3) Organic-phase photoreactions are probably not worth much attention because of the troublesome solvent redox chemistry associated with the photochemical reaction. (4) Upstream process treatment on the raffinate (dissolver solution) may never be too attractive since the radiation intensity precludes the usage of many optical materials and the nature of the solution is such that light transmission into it might be totally impossible

  4. 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

  5. Analytical chemistry of actinides

    International Nuclear Information System (INIS)

    Chollet, H.; Marty, P.

    2001-01-01

    Different characterization methods specifically applied to the actinides are presented in this review such as ICP/OES (inductively coupled plasma-optical emission spectrometry), ICP/MS (inductively coupled plasma spectroscopy-mass spectrometry), TIMS (thermal ionization-mass spectrometry) and GD/OES (flow discharge optical emission). Molecular absorption spectrometry and capillary electrophoresis are also available to complete the excellent range of analytical tools at our disposal. (authors)

  6. 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

  7. Application of chemical structure and bonding of actinide oxide materials for forensic science

    International Nuclear Information System (INIS)

    Wilkerson, Marianne Perry

    2010-01-01

    We are interested in applying our understanding of actinide chemical structure and bonding to broaden the suite of analytical tools available for nuclear forensic analyses. Uranium- and plutonium-oxide systems form under a variety of conditions, and these chemical species exhibit some of the most complex behavior of metal oxide systems known. No less intriguing is the ability of AnO 2 (An: U, Pu) to form non-stoichiometric species described as AnO 2+x . Environmental studies have shown the value of utilizing the chemical signatures of these actinide oxide materials to understand transport following release into the environment. Chemical speciation of actinide-oxide samples may also provide clues as to the age, source, or process history of the material. The scientific challenge is to identify, measure and understand those aspects of speciation of actinide analytes that carry information about material origin and history most relevant to forensics. Here, we will describe our efforts in material synthesis and analytical methods development that we will use to provide the fundamental science to characterize actinide oxide molecular structures for forensic science. Structural properties and initial results to measure structural variability of uranium oxide samples using synchrotron-based X-ray Absorption Fine Structure will be discussed.

  8. Application of chemical structure and bonding of actinide oxide materials for forensic science

    Energy Technology Data Exchange (ETDEWEB)

    Wilkerson, Marianne Perry [Los Alamos National Laboratory

    2010-01-01

    We are interested in applying our understanding of actinide chemical structure and bonding to broaden the suite of analytical tools available for nuclear forensic analyses. Uranium- and plutonium-oxide systems form under a variety of conditions, and these chemical species exhibit some of the most complex behavior of metal oxide systems known. No less intriguing is the ability of AnO{sub 2} (An: U, Pu) to form non-stoichiometric species described as AnO{sub 2+x}. Environmental studies have shown the value of utilizing the chemical signatures of these actinide oxide materials to understand transport following release into the environment. Chemical speciation of actinide-oxide samples may also provide clues as to the age, source, or process history of the material. The scientific challenge is to identify, measure and understand those aspects of speciation of actinide analytes that carry information about material origin and history most relevant to forensics. Here, we will describe our efforts in material synthesis and analytical methods development that we will use to provide the fundamental science to characterize actinide oxide molecular structures for forensic science. Structural properties and initial results to measure structural variability of uranium oxide samples using synchrotron-based X-ray Absorption Fine Structure will be discussed.

  9. Determination of microscopic interactions between actinides and humic substances

    International Nuclear Information System (INIS)

    Brunel, Benoit

    2015-01-01

    Large amount of plutonium has been introduced into the environment as a result of nuclear weapons testing, and nuclear power-plant accidents. Contaminated areas, which need a particular survey, have become a very interesting place to study and understand the plutonium behaviour in the environment. Until few years ago, it was admitted that plutonium introduced into subsurface environment is relatively immobile, owing to its low solubility in ground water and strong sorption onto rocks. However, studies of contaminated areas show that humic substances, which are ubiquitous in environment, can alter the speciation of metal ion, e.g. plutonium, and thus their migration. These humic substances are major components of the natural organic matter in soil and water as well as in geological organic deposits such as lake sediments, peats and brown coals. They are complex heterogeneous mixtures of polydisperse supra-molecules formed by biochemical and chemical reactions during the decay and transformation of plant and microbial remains. The knowledge of the impact of humic substances on the plutonium migration is required to assess their transport in natural systems. However, due to the complex and heterogeneous nature of humic substances, there are a lot of difficulties in the description of microscopic interactions. The aim of this PhD thesis is to evaluate as precisely as possible interactions between actinides and humic substances. This work is divided in two parts: on the one hand humic substances will be separated to identify each component, on the other hand the speciation of actinides with characterized humic substances will be studied. In the first part of this study, new methods are developed to study the speciation of actinides with humic substances using two kinds of mass spectrometers: an ICP-MS and a high resolution mass spectrometer using various ionization devices (ESI, APCI, DART, APPI) in order to determine all active molecules for the complexation. In the

  10. A contribution to the study of the extraction of mineral acids and of actinide (IV) and (VI) cations by N,N-dialkylamides; Contribution a l'etude de l'extraction d'acides mineraux et de cations actinides aux degres d'oxydation (IV) et (VI) par des N,N-dialkylamides

    Energy Technology Data Exchange (ETDEWEB)

    Condamines, N

    1990-03-15

    N,N-dialkylamides are alternate extractants to tributylphosphate, TBP, for the actinides separation in nuclear fuel reprocessing. N,N-di (2-ethyl hexyl) butyramide and N,N-di (2 ethyl hexyl) isobutyramide are selected for their sufficient extraction and partition ability towards actinides (IV) and (VI) without coextracting fission products. Mechanisms of HNO{sub 3}, UO{sub 2}{sup 2+}, Pu{sup 4+}, Th{sup 4+} are investigated. Nitric acid extraction is due to the competitive formation of the species (HNO{sub 3})L{sub 2}, (HNO{sub 3})L, (HNO{sub 3}){sub 2}L (L: DOBA or DOiBA). An hydrogen bond is the driving force of the transfer. For low acidity media, amides are neutral extractants. Physical interactions, between free ligand and metallic complex, arise for high amide concentrations. Taking into account the non-ideality of the organic medium by a hard spheres mixture model, we estimate that such interactions are far from negligible and very specific to the amide group. Unlike TBP, when increasing acidity, amides behave as anionic extractants. DOBA and DOiBA appear to be satisfactory extractants for fuel reprocessing.

  11. Measurement of cross-sections of fission reactions induced by neutrons on actinides from the thorium cycle at n-TOF facility; Mesures de sections efficaces de fission induite par neutrons sur des actinides du cycle du thorium a n-TOF

    Energy Technology Data Exchange (ETDEWEB)

    Ferrant, L

    2005-09-01

    In the frame of innovating energy source system studies, thorium fuel cycle reactors are considered. Neutron induced fission cross section on such cycle involved actinides play a role in scenario studies. To feed them, data bases are built with experimental results and nuclear models. For some nuclei, they are not complete or in disagreement. In order to complete these data bases, we have built an original set up, consisting in an alternation of PPACs (Parallel Plate Avalanche Chamber) and ultra - thin targets, which we installed on n-TOF facility. We describe detectors, set up, and the particular care brought to target making and characterization. Fission products in coincidence are detected with precise time measurement and localization with delay line read out method. We contributed, within the n-TOF collaboration, to the CERN brand new intense spallation neutron source characterization, based on time of flight measurement, and we describe its characteristics and performances. We were able to measure such actinide fission cross sections as {sup 232}Th, {sup 234}U, {sup 233}U, {sup 237}Np, {sup 209}Bi, and {sup nat}Pb relative to {sup 235}U et {sup 238}U standards, using an innovative acquisition system. We took advantage of the lame accessible energy field, from 0.7 eV to 1 GeV, combined with the excellent energy resolution in this field. Data treatment and analysis advancement are described to enlighten performance and limits of the obtained results. (author)

  12. Heavy metals speciation in solid household waste incineration residues and contribution to the interpretation of volatilization processes; Speciation des metaux lourds dans les residus solides d'usines d'incineration d'ordures menageres et contribution a l'interpretation des processus de vaporisation

    Energy Technology Data Exchange (ETDEWEB)

    Gagnepain, B.

    1998-07-01

    Different types of solid residues of incineration plants have at first been analyzed by complementary techniques. Relative tendencies to the heavy metals speciation have been established. On the one hand, the chemical trapping of heavy metals by ashes as well as their respective mobilities have been characterized by the sequential extraction method. On the other hand, morphology of ashes, localization, repartition and chemical environment of heavy metals have been studied by X-ray microanalysis. It has been shown that Cd and Zn are highly leachable, Cr, Ni and Cu are trapped in ashes and Pb, As have intermediary behaviours with a slow mobility. Concentration gradients of heavy metals in terms of the ashes granulometry have been deduced. An experimental device for studying the vaporization of heavy metals in a fluidized bed (simulation of the heavy metals release during the incineration of household wastes) has been perfected. Experiments have been carried out in conditions (temperature, gaseous atmosphere, residence time) near those of the real processes. A model, coupling the mass and heat transfers with a thermodynamic anticipation of the heavy metals behaviour has been developed and has allowed to exploit these obtained results. (O.M.)

  13. Thermodynamic modelling of the extraction of nitrates of lanthanides by CMPO and by CMPO-like calixarene in concentrated nitric acid medium. Application in the optimization of the separation of lanthanides and actinides/lanthanides; Modelisation thermodynamique de l'extraction de nitrates de lanthanides par le CMPO et par un calixarene-CMPO en milieu acide nitrique concentre. Application a l'optimisation de la separation des lanthanides et des actinides/lanthanides

    Energy Technology Data Exchange (ETDEWEB)

    Belair, S

    2003-07-01

    The separation minor actinides / lanthanides in nitric acid medium is as one of problems of separative chemistry the most delicate within the framework of the processes allowing the recovery of long life radioelements present in the solutions of fission products. Previous studies showed that CMPO-substituted calix[4]arenes presents a better affinity for actinides than for lanthanides. To optimize the operating conditions of separation and to take into account the degree of non-ideality for the concentrated nitric solutions, we adopted a thermodynamic approach. The methodology taken to determine the number and the stoichiometry of the complexes formed in organic phase base on MIKULIN-SERGIEVSKII's model used through a software of data processing of experimental extraction isotherms. These tools are exploited at first on an extraction system engaging the CMPO, extractant reagent of actinides and lanthanides in concentrated nitric medium. The modelling of the system Ln(NO{sub 3}){sub 3}-HNO{sub 3}-H{sub 2}O/CMPO comes to confirm the results of several studies. At the same time, they allow to establish working hypotheses aiming at limiting the investigations of our researches towards the most stable complexes formed between lanthanides and CMPO-like calixarene to which the same method is then applied. An analytical expression of the selectivity of separation by the calixarene is established to determine the parameters and physico-chemical variables on which it depends. So, the ratio of the constants of extraction and the value of the activity of water of the system fixes the selectivity of separation of 2 elements. The exploitation of this relation allows to preview the influence of a variation of the concentration of nitric acid. Experiments of extraction confirm these forecasts and inform about the affinity of the calixarene with respect to lanthanides elements and to the americium. (author)

  14. Thermal neutron actinide data

    International Nuclear Information System (INIS)

    Tellier, H.

    1992-01-01

    During the 70's, the physicists involved in the cross section measurements for the low energy neutrons were almost exclusively interested in the resonance energy range. The thermal range was considered as sufficiently known. In the beginning of the 80's, reactor physicists had again to deal with the delicate problem of the power reactor temperature coefficient, essentially for the light water reactors. The measured value of the reactivity temperature coefficient does not agree with the computed one. The later is too negative. For obvious safety reasons, it is an important problem which must be solved. Several causes were suggested to explain this discrepancy. Among all these causes, the spectral shift in the thermal energy range seems to be very important. Sensibility calculations shown that this spectral shift is very sensitive to the shape of the neutron cross sections of the actinides for energies below one electron-volt. Consequently, reactor physicists require new and accurate measurements in the thermal and subthermal energy ranges. A part of these new measurement results were recently released and reviewed. The purpose of this study is to complete the preceding review with the new informations which are now available. In reactor physics the major actinides are the fertile nuclei, uranium 238, thorium 232 and plutonium 240 and the fissile nuclei, uranium 233, uranium 235 and plutonium 239. For the fertile nuclei the main datum is the capture cross section, for the fissile nuclei the data of interest are nu-bar, the fission and capture cross sections or a combination of these data such as η or α. In the following sections, we will review the neutron data of the major actinides for the energy below 1 eV

  15. 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

  16. 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)

  17. Actinide AMS at DREAMS

    Energy Technology Data Exchange (ETDEWEB)

    Khojasteh, Nasrin B.; Merchel, Silke; Rugel, Georg; Scharf, Andreas; Ziegenruecker, Rene [HZDR, Dresden (Germany); Pavetich, Stefan [HZDR, Dresden (Germany); ANU, Canberra (Australia)

    2016-07-01

    Radionuclides such as {sup 236}U and {sup 239}Pu were introduced into the environment by atmospheric nuclear weapon tests, reactor accidents (Chernobyl, Fukushima), releases from nuclear reprocessing facilities (Sellafield, La Hague), radioactive waste disposal, and accidents with nuclear devices (Palomares, Thule) [1]. Accelerator Mass Spectrometry (AMS) is the most sensitive method to measure these actinides. The DREsden AMS (DREAMS) facility is located at a 6 MV accelerator, which is shared with ion beam analytics and implantation users, preventing major modifications of the accelerator and magnetic analyzers. DREAMS was originally designed for {sup 10}Be, {sup 26}Al, {sup 36}Cl, {sup 41}Ca, and {sup 129}I. To modify the system for actinide AMS, a Time-of-Flight (TOF) beamline at the high-energy side has been installed and performance tests are on-going. Ion beam and detector simulations are carried out to design a moveable ionization chamber. Especially, the detector window and anode dimensions have to be optimized. This ionization chamber will act as an energy detector of the system and its installation is planned as closely as possible to the stop detector of the TOF beamline for highest detection efficiency.

  18. Rare earths and actinides

    International Nuclear Information System (INIS)

    Coqblin, B.

    1982-01-01

    This paper reviews the different properties of rare-earths and actinides, either as pure metals or as in alloys or compounds. Three different cases are considered: (i) First, in the case of 'normal' rare-earths which are characterized by a valence of 3, we discuss essentially the magnetic ordering, the coexistence between superconductivity and magnetism and the properties of amorphous rare-earth systems. (ii) Second, in the case of 'anomalous' rare-earths, we distinguish between either 'intermediate-valence' systems or 'Kondo' systems. Special emphasis is given to the problems of the 'Kondo lattice' (for compounds such as CeAl 2 ,CeAl 3 or CeB 6 ) or the 'Anderson lattice' (for compounds such as TmSe). The problem of neutron diffraction in these systems is also discussed. (iii) Third, in the case of actinides, we can separate between the d-f hybridized and almost magnetic metals at the beginning of the series and the rare-earth like the metals after americium. (orig.)

  19. 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.

  20. 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.

  1. Program and presentations of the 33th Actinide Days

    International Nuclear Information System (INIS)

    2003-04-01

    The 'Journees des Actinides' (JDA) is an annual conference which provides a forum for discussions on all aspects related to the chemical and physical properties of the actinides. At the 2003 meeting, mainly the following properties were discussed of actinides and a number of actinide compounds and complexes: crystal structure, crystal-phase transformations and transformation temperatures; electrical properties including superconductivity and superconducting transition temperatures; magnetic properties; specific heat and other thermodynamic properties; electronic structure, especially in condensed matter; chemical and physico-chemical properties. The relevant experimental techniques were also dealt with, such as neutron diffraction; X-ray diffraction, in particular using synchrotron radiation; photoemission techniques, electron microscopy and spectroscopy, etc. Altogether 96 contributions were presented, of which 42 were oral presentations and 54 poster presentations. A program of the meeting and texts of both type of presentations were published in electronic form in the PDF format. All contributions were inputted to INIS; the full text of the program and the presentations has been incorporated into the INIS collection of non-conventional literature on CD-ROM. (A.K.)

  2. Medium temperature reaction between lanthanide and actinide carbides and hydrogen; Reaction a temperature moyenne entre les monocarbures de lanthanides et d'actinides et l'hydrogene

    Energy Technology Data Exchange (ETDEWEB)

    Dean, G; Lorenzelli, R; Pascard, R [Commissariat a l' Energie Atomique, Fontenay-aux-Roses (France). Centre d' Etudes Nucleaires

    1964-07-01

    Hydrogen is fixed reversibly by the lanthanide and actinide mono carbides in the range 25 - 400 C, as for pure corresponding metals. Hydrogen goes into the carbides lattice through carbon vacancies and the total fixed amount is approximately equal to two hydrogen atoms per initial vacancy. Final products c.n thus be considered as carbo-hydrides of general formula M(C{sub 1-x}, H{sub 2x}). The primitive CFC, NaCl type, structure remains unchanged but expands strongly in the case of actinide carbides. With lanthanide carbides, hydrogenation induces a phase transformation with reappearance of the metal structure (HCP). Hydrogen decomposition pressures of all the studied carbo-hydrides are greater than those of the corresponding di-hydrides. (authors) [French] Les monocarbures d'actinides et de lanthanides fixent reversiblement de l'hydrogene a temperature peu elevee, a peu pres dans les memes conditions que les metaux purs correspondants. L'hydrogene penetre dans le reseau des carbures par l'intermediaire des lacunes de carbone, et la quantite totale fixee est approximativement egale a deux atomes d'hydrogene par lacune initiale. Les produits obtenus peuvent donc etre consideres comme des carbohydrures de formule generale M(C{sub 1-x}, H{sub 2x}). La structure d'origine CFC, type NaCl est conservee, mais avec une forte expansion, dans le cas des carbures d'actinides. En revanche, l'hydrogenation entraine un changement de phase cristalline avec retour a la structure du metal (HC) pour les carbures de lanthanides. Tous les carbohydrures etudies ont des tensions de decomposition en hydrogene superieures a celles des dihydrures correspondants. (auteurs)

  3. 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)

  4. Set up of an innovative methodology to measure on-line the incineration potential of minor actinides under very high neutron sources in the frame of the future prospects of the nuclear waste transmutation; Mise au point d'une methodologie innovante pour la mesure du potentiel d'incineration d'actinides mineurs sous des sources tres intenses de neutrons, dans la perspective de transmutation des dechets nucleaires

    Energy Technology Data Exchange (ETDEWEB)

    Fadil, M

    2003-03-01

    This work deals generally with the problem of nuclear waste management and especially with the transmutation of it to reduce considerably its radiotoxicity potential. The principal objective of this thesis is to show the feasibility to measure on-line the incineration potential of minor actinides irradiated under very high neutron flux. To realize this goal, we have developed fission micro-chambers able to operate, for the first time in the world, in saturation regime under a severe neutron flux. These new chambers use {sup 235}U as an active deposit. They were irradiated in the high flux reactor at Laue-Langevin Institute in Grenoble. The measurement of the saturation current delivered by these chambers during their irradiation for 26 days allowed to evaluate the burn-up of {sup 235}U. We have determined the neutron flux intensity of 1,6 10{sup 15} n.cm{sup -2}.s{sup -1} in the bottom of the irradiation tube called 'V4'. The relative uncertainty of this value is less than 4 %. This is for the first time that such high neutron flux is measured with a fission chamber. To confirm this result, we have also performed independent measurements using gamma spectroscopy of irradiated Nb and Co samples. Both results are in agreement within error bars. Simple Deposit Fission Chambers (SDFC) as above were the reference of the new generation of fission chambers that we have developed in the framework of this thesis: Double Deposit Fission Chambers (DDFC). The reference active deposit was {sup 235}U. The other deposit was the actinide that we wanted to study (e.g. {sup 237}Np and {sup 241}Am). At the end of the thesis, we present some suggestions to ameliorate the operation of the DDFC to be exploited in other transmutation applications in the future. (author)

  5. Lanthanide/Actinide Opacities

    Science.gov (United States)

    Hungerford, Aimee; Fontes, Christopher J.

    2018-06-01

    Gravitational wave observations benefit from accompanying electromagnetic signals in order to accurately determine the sky positions of the sources. The ejecta of neutron star mergers are expected to produce such electromagnetic transients, called macronovae (e.g. the recent and unprecedented observation of GW170817). Characteristics of the ejecta include large velocity gradients and the presence of heavy r-process elements, which pose significant challenges to the accurate calculation of radiative opacities and radiation transport. Opacities include a dense forest of bound-bound features arising from near-neutral lanthanide and actinide elements. Here we present an overview of current theoretical opacity determinations that are used by neutron star merger light curve modelers. We will touch on atomic physics and plasma modeling codes that are used to generate these opacities, as well as the limited body of laboratory experiments that may serve as points of validation for these complex atomic physics calculations.

  6. Relativistic studies in actinides

    International Nuclear Information System (INIS)

    Weinberger, P.; Gonis, A.

    1987-01-01

    In this review the theoretical background is given for a relativistic description for actinide systems. A short introduction is given of the density functional theory which forms the basis for a fully relativistic single-particle theory. A section on the Dirac Hamiltonian is followed by a brief summary on group theoretical concepts. Single site scattering is presented such that formal extensions to the case of the presence of an internal (external) magnetic field and/or anisotropic scattering are evident. Multiple scattering is discussed such that it can readily be applied also to the problem of dislocations. In connection with the problem of selfconsistency particular attention is drawn to the use of complex energies. Finally the various theoretical aspects discussed are illustrated through the results of numerical calculations. 101 refs.; 37 figs.; 5 tabs

  7. Significance of actinide chemistry for the long-term safety of waste disposal

    International Nuclear Information System (INIS)

    Kim, Jae Il

    2006-01-01

    A geochemical approach to the long-term safety of waste disposal is discussed in connection with the significance of actinides, which shall deliver the major radioactivity inventory subsequent to the relatively short-term decay of fission products. Every power reactor generates transuranic (TRU) elements: plutonium and minor actinides (Np, Am, Cm), which consist chiefly of long-lived nuclides emitting alpha radiation. The amount of TRU actinides generated in a fuel life period is found to be relatively small (about 1 wt% or less in spent fuel) but their radioactivity persists many hundred thousands years. Geological confinement of waste containing TRU actinides demands, as a result, fundamental knowledge on the geochemical behavior of actinides in the repository environment for a long period of time. Appraisal of the scientific progress in this subject area is the main objective of the present paper. Following the introductory discussion on natural radioactivities, the nuclear fuel cycle is briefly brought up with reference to actinide generation and waste disposal. As the long-term disposal safety concerns inevitably with actinides, the significance of the aquatic actinide chemistry is summarized in two parts: the fundamental properties relevant to their aquatic behavior and the geochemical reactions in nanoscopic scale. The constrained space of writing allows discussion on some examples only, for which topics of the primary concern are selected, e.g. apparent solubility and colloid generation, colloid-facilitated migration, notable speciation of such processes, etc. Discussion is summed up to end with how to make a geochemical approach available for the long-term disposal safety of nuclear waste or for the Performance Assessment (PA) as known generally

  8. Purex process modelling - do we really need speciation data?

    International Nuclear Information System (INIS)

    Taylor, R.J.; May, I.

    2001-01-01

    The design of reprocessing flowsheets has become a complex process requiring sophisticated simulation models, containing both chemical and engineering features. Probably the most basic chemical data needed is the distribution of process species between solvent and aqueous phases at equilibrium, which is described by mathematical algorithms. These algorithms have been constructed from experimentally determined distribution coefficients over a wide range of conditions. Distribution algorithms can either be empirical fits of the data or semi-empirical equations, which describe extraction as functions of process variables such as temperature, activity coefficients, uranium loading, etc. Speciation data is not strictly needed in the accumulation of distribution coefficients, which are simple ratios of analyte concentration in the solvent phase to that in the aqueous phase. However, as we construct process models of increasing complexity, speciation data becomes much more important both to raise confidence in the model and to understand the process chemistry at a more fundamental level. UV/vis/NIR spectrophotometry has been our most commonly used speciation method since it is a well-established method for the analysis of actinide ion oxidation states in solution at typical process concentrations. However, with the increasing availability to actinide science of more sophisticated techniques (e.g. NMR; EXAFS) complementary structural information can often be obtained. This paper will, through examples, show how we have used spectrophotometry as a primary tool in distribution and kinetic experiments to obtain data for process models, which are then validated through counter-current flowsheet trials. It will also discuss how spectrophotometry and other speciation methods are allowing us to study the link between molecular structure and extraction behaviour, showing how speciation data really is important in PUREX process modelling. (authors)

  9. Projected benefits of actinide partitioning

    International Nuclear Information System (INIS)

    Braun, C.; Goldstein, M.

    1976-05-01

    Possible benefits that could accrue from actinide separation and transmutations are presented. The time frame for implementing these processes is discussed and the expected benefits are qualitatively described. These benefits are provisionally quantified in a sample computation

  10. Environmental research on actinide elements

    International Nuclear Information System (INIS)

    Pinder, J.E. III; Alberts, J.J.; McLeod, K.W.; Schreckhise, R.G.

    1987-08-01

    The papers synthesize the results of research sponsored by DOE's Office of Health and Environmental Research on the behavior of transuranic and actinide elements in the environment. Separate abstracts have been prepared for the 21 individual papers

  11. 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)

  12. Speciation, in the nuclear fuel cycle by spectroscopic techniques

    International Nuclear Information System (INIS)

    Colette, S.; Plancque, G.; Allain, F.; Lamouroux, C.; Steiner, V.; Amekraz, B.; Moulin, C.

    2000-01-01

    New analytical techniques allowing to perform speciation in the framework of the nuclear fuel cycle are more and more needed. They have to be selective (since matrix encountered are very complex), sensitive (in order to work at representative concentration and below solubility limit), as well as non intrusive (in order to keep the image of the real solution). Among them, laser-based analytical techniques present these advantages together with the possibility to perform remote measurements via fiber optics. Hence, Time-Resolved Laser-Induced Fluorescence (TRLIF) has been used for actinides/lanthanides interaction and speciation studies in inorganic and organic matrices from the reprocessing to waste storage. Moreover, new ion detection methods such as Electro-Spray - Mass Spectrometry (ES-MS) seems promising for speciation studies. Hence, it is the first time that it is possible to directly couple a liquid at atmospheric pressure to a mass detection working at reduced pressure with a soft mode of ionisation that should allow to give informations on chemical species present. Principle, advantages and limitations as well as results obtained with the use of TRLIF and ES-MS on different systems of interest including actinides, lanthanides, fission products in interaction with simple organic molecules to very complex structure will be presented and discussed. (authors)

  13. Speciation, in the nuclear fuel cycle by spectroscopic techniques

    Energy Technology Data Exchange (ETDEWEB)

    Colette, S.; Plancque, G.; Allain, F.; Lamouroux, C.; Steiner, V.; Amekraz, B.; Moulin, C. [CEA/Saclay, Dept, des Procedes d' Enrichissement (DPE), 91 - Gif-sur-Yvette (France)

    2000-07-01

    New analytical techniques allowing to perform speciation in the framework of the nuclear fuel cycle are more and more needed. They have to be selective (since matrix encountered are very complex), sensitive (in order to work at representative concentration and below solubility limit), as well as non intrusive (in order to keep the image of the real solution). Among them, laser-based analytical techniques present these advantages together with the possibility to perform remote measurements via fiber optics. Hence, Time-Resolved Laser-Induced Fluorescence (TRLIF) has been used for actinides/lanthanides interaction and speciation studies in inorganic and organic matrices from the reprocessing to waste storage. Moreover, new ion detection methods such as Electro-Spray - Mass Spectrometry (ES-MS) seems promising for speciation studies. Hence, it is the first time that it is possible to directly couple a liquid at atmospheric pressure to a mass detection working at reduced pressure with a soft mode of ionisation that should allow to give informations on chemical species present. Principle, advantages and limitations as well as results obtained with the use of TRLIF and ES-MS on different systems of interest including actinides, lanthanides, fission products in interaction with simple organic molecules to very complex structure will be presented and discussed. (authors)

  14. The use of yield tracers for the determination of aplha-emitting actinides in the marine environment

    International Nuclear Information System (INIS)

    Harvey, B.R.; Lovett, M.B.

    1984-01-01

    The need for yield tracers and their general analytical application is briefly discussed and more fully expanded in the context of the radiochemical determination of alpha-emitting actinides. The important alpha-emitting nuclides of the actinide elements found in the marine environment are listed. The environmental significance and analytical implications arising from the multiplicity of valency states found amongst the earlier members of the actinide series are noted. The tracers that are available for analyses and their selection and suitability for particular applications are discussed and the general precautions that need to be observed in their use are given. Use of the dual tracer technique in the study of speciation of the actinides in the marine environment is discussed with special reference to plutonium in sea water. The limited applicability of plutonium as a yield tracer in the study of neptunium speciation is noted and the latest developments in the investigation of 235 Np as an alternative tracer for neptunium are given. The possibility of the joint use of americium and curium nuclides as tracers in the study of the speciation of these two elements is explored. (orig.)

  15. Speciation needs in relation with environmental and biological purposes

    International Nuclear Information System (INIS)

    Moulin, V.; Ansoborlo, E.; Bion, L.; Doizi, D.; Moulin, C.; Cote, G.; Madic, C.; Van Der Lee, J.

    2004-01-01

    Radionuclides can occur in the environment either through chronic releases of nuclear facilities, or due to incidents or accidents. In order to study their behaviour in the environment (migration, retention, transfer, and in human organisms (metabolism, retention, excretion), it is of prime importance to know their solution chemistry, and more particularly thermodynamic constants, which will allow to determine their speciation. In fact, speciation governs the migration, the bioavailability and the toxicity of elements. Moreover, this knowledge is also of great interest for decorporation or decontamination purposes. In this framework, a CEA working group on speciation has been created in order to share data both on thermodynamic constants and on speciation analytical methods, interesting chemists, environmentalists and biologists. It has been focused, in a first time, on actinides, namely Th, U, Pu, Am, Np, taking into account their most important oxidation states occurring in environmental or biological environments: Th(IV), U(IV, VI), Pu(III, IV, VI), Am(III), Np(IV, V). A particular attention was devoted to the choice of ligands (inorganic and organic) for being the most representative of environmental and biological media. The thermodynamic database used is BASSIST for Base Applied to Speciation in Solution and at Interfaces and Solubility (developed by CEA), in interaction with the code JCHESS. Different examples will be then presented on the selection of data (thermodynamic constants, ligands of interest) through benchmark exercises (case of U(VI), Am(III), Pu(IV)) which will show the lacks or weakness of knowledge. Speciation diagrams will support these discussions. Moreover, analytical methods to determine thermodynamic constants or direct speciation will also be presented and discussed. (author)

  16. Chemical durability and resistance to irradiation of LnYSiAlO (Ln=La or Ce) glasses, potential immobilization matrix of minor actinides; Durabilite chimique et comportement a l'irradiation des verres quaternaires LnYSiAlO (Ln = La ou Ce), matrice potentielle d'immobilisation d'actinides mineurs trivalents

    Energy Technology Data Exchange (ETDEWEB)

    Gavarini, St

    2002-11-01

    Rare earth aluminosilicate glasses are known for their interesting mechanical and optical properties. Recent studies have shown that their chemical durability was very good too, such they have the potential to be used in the nuclear industry for the specific immobilization of trivalent actinides. Initial dissolution rates of LaYSiAlO and CeYSiAlO were determined using a Soxhlet device (dynamic leaching). The differences linked to the nature of the rare earth element were studied by synthesizing analogous glasses that only differed in their rare earth element composition (%at.): Y-5%, La-5 %, Si-15%, Al-10% O-65%. The influence of pH on the dissolution mechanisms and kinetics was also studied by static leaching tests performed in dilute solutions of NaOH or HNO{sub 3}. Electronic defects and collision cascades, induced by a-disintegration of radioelements confined in storage matrix, can cause important modifications in the glass structure and, thus, influence its chemical durability. To simulate these effects, glass samples were irradiated with {beta} particles and heavy ions accelerated to 2,5 MeV and 200 keV, respectively. Monoliths were then leached in static bi-distilled water (pH{>=}{>=} 5.5) for one month in an autoclave heated to 90 degrees C. Initially, the structural changes caused by irradiation were determined using Raman, NMR and EPR spectroscopies. Ion {mu}-beams, SEM-EDS and XPS analysis were also performed to evaluate the potential modifications of the superficial composition. Finally, the leaching behavior was studied, for both irradiated and unirradiated samples, through solution and solid elementary characterization. (author)

  17. 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)

  18. 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

  19. Actinides and heavy fermions

    International Nuclear Information System (INIS)

    Smith, J.L.; Fisk, Z.; Ott, H.R.

    1987-01-01

    The actinide series of elements begins with f-shell electrons forming energy bands, contributing to the bonding, and possessing no magnetic moments. At americium the series switches over to localized f electrons with magnetic moments. In metallic compounds this crossover of behavior can be modified and studied. In this continuum of behavior a few compounds on the very edge of localized f-electron behavior exhibit enormous electronic heat capacities at low temperatures. This is associated with an enhanced thermal mass of the conduction electrons, which is well over a hundred times the free electron mass, and is what led to the label heavy fermion for such compounds. A few of these become superconducting at even lower temperatures. The excitement in this field comes from attempting to understand how this heaviness arises and from the likelihood that the superconductivity is different from that of previously known superconductors. The effects of thorium impurities in UBe 13 were studied as a representative system for studying the nature of the superconductivity

  20. Arsenic speciation results

    Data.gov (United States)

    U.S. Environmental Protection Agency — Linear combination fitting results of synchrotron data to determine arsenic speciation in soil samples. This dataset is associated with the following publication:...

  1. Chemical Speciation - General Information

    Science.gov (United States)

    This page includes general information about the Chemical Speciation Network that is not covered on the main page. Commonly visited documents, including calendars, site lists, and historical files for the program are listed here

  2. Searching for speciation genes

    DEFF Research Database (Denmark)

    Holt, Benjamin George; Côté, Isabelle M; Emerson, Brent C

    2011-01-01

    Closely related species that show clear phenotypic divergence, but without obvious geographic barriers, can provide opportunities to study how diversification can occur when opportunities for allopatric speciation are limited. We examined genetic divergence in the coral reef fish genus Hypoplectrus...

  3. 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

  4. 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

  5. Uranium speciation in plants

    International Nuclear Information System (INIS)

    Guenther, A.; Bernhard, G.; Geipel, G.; Reich, T.; Rossberg, A.; Nitsche, H.

    2003-01-01

    Detailed knowledge of the nature of uranium complexes formed after the uptake by plants is an essential prerequisite to describe the migration behavior of uranium in the environment. This study focuses on the determination of uranium speciation after uptake of uranium by lupine plants. For the first time, time-resolved laser-induced fluorescence spectroscopy and X-ray absorption spectroscopy were used to determine the chemical speciation of uranium in plants. Differences were detected between the uranium speciation in the initial solution (hydroponic solution and pore water of soil) and inside the lupine plants. The oxidation state of uranium did not change and remained hexavalent after it was taken up by the lupine plants. The chemical speciation of uranium was identical in the roots, shoot axis, and leaves and was independent of the uranium speciation in the uptake solution. The results indicate that the uranium is predominantly bound as uranyl(VI) phosphate to the phosphoryl groups. Dandelions and lamb's lettuce showed uranium speciation identical to lupine plants. (orig.)

  6. 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.

  7. 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.

  8. 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)

  9. 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.

  10. 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)

  11. 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.)

  12. 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

  13. 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

  14. 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)

  15. 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

  16. 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

  17. Preliminary considerations concerning actinide solubilities

    International Nuclear Information System (INIS)

    Newton, T.W.; Bayhurst, B.P.; Daniels, W.R.; Erdal, B.R.; Ogard, A.E.

    1980-01-01

    Work at the Los Alamos Scientific Laboratory on the fundamental solution chemistry of the actinides has thus far been confined to preliminary considerations of the problems involved in developing an understanding of the precipitation and dissolution behavior of actinide compounds under environmental conditions. Attempts have been made to calculate solubility as a function of Eh and pH using the appropriate thermodynamic data; results have been presented in terms of contour maps showing lines of constant solubility as a function of Eh and pH. Possible methods of control of the redox potential of rock-groundwater systems by the use of Eh buffers (redox couples) is presented

  18. Orbital effects in actinide systems

    International Nuclear Information System (INIS)

    Lander, G.H.

    1983-01-01

    Actinide magnetism presents a number of important challenges; in particular, the proximity of 5f band to the Fermi energy gives rise to strong interaction with both d and s like conduction electrons, and the extended nature of the 5f electrons means that they can interact with electron orbitals from neighboring atoms. Theory has recently addressed these problems. Often neglected, however, is the overwhelming evidence for large orbital contributions to the magnetic properties of actinides. Some experimental evidence for these effects are presented briefly in this paper. They point, clearly incorrectly, to a very localized picture for the 5f electrons. This dichotomy only enhances the nature of the challenge

  19. 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

  20. 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

  1. ENDF/B-V actinides

    International Nuclear Information System (INIS)

    Kocherov, N.; Lemmel, H.D.

    1981-01-01

    This document summarizes the contents of the actinides part of the ENDF/B-V nuclear data library released by the US National Nuclear Data Center. This library or selective retrievals of it, are available from the IAEA Nuclear Data Section. (author)

  2. Environmental research on actinide elements

    Energy Technology Data Exchange (ETDEWEB)

    Pinder, J.E. III; Alberts, J.J.; McLeod, K.W.; Schreckhise, R.G. (eds.)

    1987-08-01

    The papers synthesize the results of research sponsored by DOE's Office of Health and Environmental Research on the behavior of transuranic and actinide elements in the environment. Separate abstracts have been prepared for the 21 individual papers. (ACR)

  3. 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)

  4. Angular overlap model in actinides

    International Nuclear Information System (INIS)

    Gajek, Z.; Mulak, J.

    1991-01-01

    Quantitative foundations of the Angular Overlap Model in actinides based on ab initio calculations of the crystal field effect in the uranium (III) (IV) and (V) ions in various crystals are presented. The calculations justify some common simplifications of the model and fix up the relations between the AOM parameters. Traps and limitations of the AOM phenomenology are discussed

  5. Angular overlap model in actinides

    Energy Technology Data Exchange (ETDEWEB)

    Gajek, Z.; Mulak, J. (Polska Akademia Nauk, Wroclaw (PL). Inst. Niskich Temperatur i Badan Strukturalnych)

    1991-01-01

    Quantitative foundations of the Angular Overlap Model in actinides based on ab initio calculations of the crystal field effect in the uranium (III) (IV) and (V) ions in various crystals are presented. The calculations justify some common simplifications of the model and fix up the relations between the AOM parameters. Traps and limitations of the AOM phenomenology are discussed.

  6. Chemical aspects of incinerating highly chlorinated and actinide {alpha} contaminated organic waste: application to the Iris process; Aspects chimiques de l'incineration des dechets organiques fortement charges en chlore et contamines en actinides emetteurs {alpha}. Application au procede IRIS

    Energy Technology Data Exchange (ETDEWEB)

    Lemort, F.; Cames, B. [CEA Valrho, (DCC/DRRV/SCD), 30 - Marcoule (France)

    2000-07-01

    A fraction of the waste produced by nuclear activities is combustible, and thus suitable for incineration to produce gases, ash and fines. A typical composition representative of actual organic waste mixtures was defined for the purpose of investigating possible heat treatment processes; the composition is identified according to components Table 1 and elements Table II. The high polyvinyl chloride (PVC) content is responsible for the high chlorine potential in the process equipment. The quantity and quality of the resulting solid residue depends entirely on the inorganic load of the organic waste, whose behavior is entirely conditioned by the process conditions. For example, pure polyethylene is totally converted to gases (water and carbon dioxide), while the composition shown in Table II produces a range of oxides and chlorides. The high chlorine content results in partial chlorination of the inorganic compounds, but can also lead to interactions with the process equipment. The temperature dependent variation of the chlorination equilibrium constants of various metals clearly shows that all the elements of technological alloys may be subject to active corrosion by hydrochloric acid. However, the corresponding oxides-notably alumina-are much less sensitive to corrosion; aluminum-based alloys are therefore preferred for incinerator construction and to limit corrosion by hydrochloric acid. Thermodynamic and kinetic studies led to the development of the IRIS three-step process. Gas emissions occurring during processing of solid materials are completely oxidized in the after-burning step at 1100 deg C, and are then ducted to a HERA filtration system capable of retaining all the actinide {alpha} radionuclides. Although corrosion-related problems are attenuated in the two-step process chlorine can combine with the inorganic waste material to form chlorides with potentially damaging effects on the system; this is the case for zinc chloride and for volatile chlorides in

  7. Actinide chemistry research supporting the Waste Isolation Pilot Plant (WIPP): FY94 results

    Energy Technology Data Exchange (ETDEWEB)

    Novak, C.F. [ed.

    1995-08-01

    This document contains six reports on actinide chemistry research supporting the Waste Isolation Pilot Plant (WIPP). These reports, completed in FY94, are relevant to the estimation of the potential dissolved actinide concentrations in WIPP brines under repository breach scenarios. Estimates of potential dissolved actinide concentrations are necessary for WIPP performance assessment calculations. The specific topics covered within this document are: the complexation of oxalate with Th(IV) and U(VI); the stability of Pu(VI) in one WIPP-specific brine environment both with and without carbonate present; the solubility of Nd(III) in a WIPP Salado brine surrogate as a function of hydrogen ion concentration; the steady-state dissolved plutonium concentrations in a synthetic WIPP Culebra brine surrogate; the development of a model for Nd(III) solubility and speciation in dilute to concentrated sodium carbonate and sodium bicarbonate solutions; and the development of a model for Np(V) solubility and speciation in dilute to concentrated sodium Perchlorate, sodium carbonate, and sodium chloride media.

  8. Actinide chemistry research supporting the Waste Isolation Pilot Plant (WIPP): FY94 results

    International Nuclear Information System (INIS)

    Novak, C.F.

    1995-08-01

    This document contains six reports on actinide chemistry research supporting the Waste Isolation Pilot Plant (WIPP). These reports, completed in FY94, are relevant to the estimation of the potential dissolved actinide concentrations in WIPP brines under repository breach scenarios. Estimates of potential dissolved actinide concentrations are necessary for WIPP performance assessment calculations. The specific topics covered within this document are: the complexation of oxalate with Th(IV) and U(VI); the stability of Pu(VI) in one WIPP-specific brine environment both with and without carbonate present; the solubility of Nd(III) in a WIPP Salado brine surrogate as a function of hydrogen ion concentration; the steady-state dissolved plutonium concentrations in a synthetic WIPP Culebra brine surrogate; the development of a model for Nd(III) solubility and speciation in dilute to concentrated sodium carbonate and sodium bicarbonate solutions; and the development of a model for Np(V) solubility and speciation in dilute to concentrated sodium Perchlorate, sodium carbonate, and sodium chloride media

  9. 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)

  10. Absorption spectra and speciation of plutonium(VI) with phosphate

    Energy Technology Data Exchange (ETDEWEB)

    Weger, H.T.; Reed, D.

    1996-02-01

    Plutonium(VI)-phosphate species in aqueous solution, at pH < 2.4, formed two species: PuO{sub 2}H{sub 2}PO{sub 4}{sup +} (characterized by an 835 nm absorption band) and the solid phase PuO{sub 2}(H{sub 2}PO{sub 4}){sub 2}. The stability constant {beta} for the PuO{sub 2}H{sub 2}PO{sub 4}{sup +} species was determined to be log {beta} = 2.1 {+-} 0.1 (ionic strength = 0.6--0.9 M) and log {beta}{sup T} = 2.6 {+-} 0.15 (zero ionic strength). Four Pu(VI)-phosphate species (absorption bands at 842, 846, 857, and 866 nm) formed at pH = 2.4 to 12.2 and are characterized by polynuclear behavior, the formation of precipitates, and colloidal properties. The 842 and 846 nm species are believed to be [PuO{sub 2}(HPO{sub 4}){sub m}]{sub n} and [PuO{sub 2}(NaPO{sub 4}){sub m}]{sub n}. The 857 and 866 nm species area as yet unidentified. The speciation of plutonium with phosphate is of interest to radionuclide migration studies because phosphate is present in many groundwaters and may be used as an actinide getter in nuclear waste disposal. An actinide getter is a complexing agent that forms insoluble phases with actinides, thereby reducing their migration.

  11. Coordination polymers: trapping of radionuclides and chemistry of tetravalent actinides (Th, U) carboxylates

    International Nuclear Information System (INIS)

    Falaise, Clement

    2014-01-01

    The use of nuclear energy obviously raises the question of the presence of radionuclides in the environment. Currently, their mitigation is a major issue associated with nuclear chemistry. This thesis focuses on both the trapping of radionuclides by porous solids called Metal-Organic Frameworks (MOF) and the crystal chemistry of the carboxylate of tetravalent actinides (AnIV). The academic knowledge of the reactivity of carboxylate of AnIV could help the understanding of actinides speciation in environment. We focused on the sequestration of iodine by aluminum based MOF. The functionalization (electron-donor group) of the MOF drastically enhances the iodine capture capacity. The removal of light actinides (Th and U) from aqueous solution was also investigated as well as the stability of (Al)-MOF under γ radiation. More than twenty coordination polymers based on tetravalent actinides have been synthesized and characterized by single crystal X-ray diffraction. The use of controlled hydrolysis promotes the formation of coordination polymers exhibiting polynuclear cluster ([U 4 ], [Th 6 ], [U 6 ] and [U 38 ]). In order to understand the formation of the largest cluster, the ex-situ study of the solvo-thermal synthesis of compound {U 38 } has also been investigated. (author)

  12. Solvent extraction separations of trivalent lanthanide and actinide ions using an aqueous aminomethanediphosphonic acid

    International Nuclear Information System (INIS)

    Jensen, M. P.

    1998-01-01

    The possibility of separating the trivalent lanthanides, represented by EU 3+ , and actinides, represented by Cf 3+ , using HDEHP in toluene and an aqueous phase containing N-piperidinomethane-1,1-diphosphotic acid, PMDPA, has been investigated. This modified aqueous phase offers potential advantages over the diethylenetriaminepentaacetic acid based TALSPEAK process because of the improved complexation properties of PMDPA in acidic solutions, and the ability to decompose PMDPA before disposal. Extraction experiments were conducted at 25 C in 2 M NaClO 4 between -log [H + ] 1 and 2. The studies enabled us to derive the aqueous phase speciation, the stability constants of the aqueous complexes, and the Cf/Eu separation factors. Despite the presence of an amino group in PMDPA that should favor the retention of the actinides in the aqueous phase, the Cf/Eu separation factors are near unity under the conditions studied

  13. 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

  14. 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

  15. Analytical evaluation of actinide sensitivities

    International Nuclear Information System (INIS)

    Sola, A.

    1977-01-01

    The analytical evaluation of the sensitivities of actinides to various parameters such as cross sections, decay constants, flux and time is presented. The formulae are applied to isotopes of the Uranium, Neptunium, Plutonium and Americium series. The agreement between analytically obtained and computer evaluated sensitivities being always good, it is throught that the formulation includes all the important parameters entering in the evaluation of sensitivities. A study of the published data is made

  16. 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

  17. Recovery of trans-plutonium elements; Recuperation des elements transplutoniens

    Energy Technology Data Exchange (ETDEWEB)

    Espie, J Y; Poncet, B; Simon, A [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

    1970-07-01

    The object of this work is to study the recovery of americium and curium from the fission-product solution obtained from the processing of irradiated fuel elements made of natural metallic uranium alloyed with aluminium, iron and silicon; these elements have been subjected to an average irradiation of 4000 MW days/ton in a gas-graphite type reactor having a thermal power of 3.7 MW/ton of uranium. The process used consists of 3 extraction cycles and one americium-curium separation: - 1) extraction cycle in 40 per cent TBP: extraction of actinides and lanthanides; elimination of fission products; - 2) extraction cycle in 8 per cent D2EHPA: decontamination from the fission products, decontamination of actinides from lanthanides; - 3) extraction cycle in 40 per cent TBP: separation of the complexing agent and concentration of the actinides; - 4) americium-curium separation by precipitation. (authors) [French] Cette etude a pour objet, la recuperation de l'americium et du curium de la solution de produits de fission provenant du traitement de combustibles irradies a base d'uranium naturel metallique allie a l'aluminium, le fer, et le silicium, et ayant subi une irradiation moyenne de 4000 MWj/t dans une pile du type graphite-gaz, dont la puissance thermique est de 3.7 MW/t d'uranium. Le procede utilise comprend 3 cycles d'extraction et une separation americium-curium: - 1. cycle d'extraction dans le TBP a 40 pour cent: extraction des actinides et des lanthanides, elimination des produits de fission; - 2. cycle d'extraction dans le D2EHPA a 8 pour cent: decontamination en produits de fission, decontamination des actinides en lanthanides; - 3. cycle d'extraction dans le TBP a 40 pour cent: separation du complexant et concentration des actinides; - 4. separation americium-curium par precipitation. (auteurs)

  18. The structure of actinide ions exchanged into native and modified zeolites and clays

    International Nuclear Information System (INIS)

    Wasserman, S. R.; Soderholm, L.; Giaquinta, D. M.

    2000-01-01

    X-ray absorption spectroscopy (XAS) has been used to investigate the structure and valence of thorium (Th 4+ ) and uranyl (UO 2 2+ ) cations exchanged into two classes of microporous aluminosilicate minerals: zeolites and smectite clays. XAS is also employed to examine the fate of the exchanged cations after modification of the mineral surface using self-assembled organic films and/or exposure to hydrothermal conditions. These treatments serve as models for the forces that ultimately determine the chemical fate of the actinide cations in the environment. The speciation of the cations depends on the pore size of the aluminosilicate, which is fixed for the zeolites and variable for the smectites

  19. Arsenic Speciation in Groundwater: Role of Thioanions

    Science.gov (United States)

    The behavior of arsenic in groundwater environments is fundamentally linked to its speciation. Understanding arsenic speciation is important because chemical speciation impacts reactivity, bioavailability, toxicity, and transport and fate processes. In aerobic environments arsen...

  20. 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.

  1. 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)

  2. 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

  3. 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....

  4. Minor Actinides Recycling in PWRs

    International Nuclear Information System (INIS)

    Delpech, M.; Golfier, H.; Vasile, A.; Varaine, F.; Boucher, L.; Greneche, D.

    2006-01-01

    Recycling of minor actinides in current and near future PWR is considered as one of the options of the general waste management strategy. This paper presents the analysis of this option both from the core physics and fuel cycle point of view. A first indicator of the efficiency of different neutron spectra for transmutation purposes is the capture to fission cross sections ratio which is less favourable by a factor between 5 to 10 in PWRs compared to fast reactors. Another indicator presented is the production of high ranking isotopes like Curium, Berkelium or Californium in the thermal or epithermal spectrum conditions of PWR cores by successive neutron captures. The impact of the accumulation of this elements on the fabrication process of such PWR fuels strongly penalizes this option. The main constraint on minor actinides loadings in PWR (or fast reactors) fuels are related to their direct impact (or the impact of their transmutation products) on the reactivity coefficients, the reactivity control means and the core kinetics parameters. The main fuel cycle physical parameters like the neutron source, the alpha decay power, the gamma and neutrons dose rate and the criticality aspects are also affected. Recent neutronic calculations based on a reference core of the Evolutionary Pressurized Reactor (EPR), indicates typical maximum values of 1 % loadings. Different fuel design options for minor actinides transmutation purposes in PWRs are presented: UOX and MOX, homogeneous and heterogeneous assemblies. In this later case, Americium loading is concentrated in specific pins of a standard UOX assembly. Recycling of Neptunium in UOX and MOX fuels was also studied to improve the proliferation resistance of the fuel. The impact on the core physics and penalties on Uranium enrichment were underlined in this case. (authors)

  5. New developments at the INE-Beamline for actinide research at ANKA

    Science.gov (United States)

    Dardenne, K.; Brendebach, B.; Denecke, M. A.; Liu, X.; Rothe, J.; Vitova, T.

    2009-11-01

    The INE-Beamline for actinide research at the synchrotron source ANKA is operated by the Institut für Nukleare Entsorgung (INE) at the Forschungszentrum Karlsruhe. Experiments on radioactive samples with activities up to 106 times the limit of exemption inside a safe and flexible double containment concept are possible. One great advantage of the beamline is its close proximity to INE's active laboratories with its equipment for manipulation of actinide materials and state-of-the-art spectroscopic, analytical, and microscopic instrumentation. This constellation is unique in Europe. The INE-Beamline is built primarily to serve INE in-house research associated with safe disposal of high level nuclear waste such as actinide speciation or coordination-, redox-, and geo-chemistry of actinides. A wide energy range from around 2.1 keV to 25 keV covering the K-edges from P to Pd and the L3, L2, and L1 edges for actinides from Th to Cm can be used. The INE-Beamline is optimized for X-ray absorption spectroscopy techniques (XANES/EXAFS), but x-ray fluorescence (XRF) analysis and powder diffraction (XRD) are also possible, as well as surface sensitive measurements in grazing incidence geometry (GI-XAFS). Upgrades of instrumentation and extension of experimental capabilities at the INE-Beamline are driven by user needs. Two of the recent upgrades are presented: 1) installation of a microfocus option for spatially resolved studies (μ-XRF, μ-XANES, μ-XRD) and investigations of small volumes (e.g., heterogeneous natural samples and diamond anvil high pressure cells); 2) construction, and commissioning of a high resolution x-ray emission spectrometer (HRXES); 3) availability of an electrochemical cell for investigation of redox sensitive systems.

  6. PIE analysis for minor actinide

    International Nuclear Information System (INIS)

    Suyama, Kenya

    2005-01-01

    Minor actinide (MA) is generated in nuclear fuel during the operation of power reactor. For fuel design, reactivity decrease due to it should be considered. Out of reactors, MA plays key role to define the property of spent fuel (SF) such as α-radioactivity, neutron emission rate, and criticality of SF. In order to evaluate the calculation codes and libraries for predicting the amount of MA, comparison between calculation results and experimentally obtained data has been conducted. In this report, we will present the status of PIE data of MA taken by post irradiation examinations (PIE) and several calculation results. (author)

  7. 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.

  8. Microbial Transformations of Actinides and Fission Products in Radioactive Waste

    Energy Technology Data Exchange (ETDEWEB)

    Francis, A. J. [Pohang Univ. Science and Technology, Pohang (Korea, Republic of)

    2011-07-01

    The environmental factors that can affect microbial growth and activity include moisture, temperature, ph, Eh, availability of organic and inorganic nutrients, and radiation. The microbial activity in a specific repository is influenced by the ambient environment of the repository, and the materials to be emplaced. For example, a repository in unsaturated igneous rock formations such as volcanic tuff rocks at Yucca Mountain is generally expected to be oxidizing; a repository in a hydrologically expected to be oxidizing; a repository in a hydrologically saturated zone, especially in sedimentary rocks, could be reducing. Sedimentary rocks contain a certain amount of organic matter, which may stimulate microbial activities and, thus maintain the repository and its surrounding areas at reducing conditions. Although the impacts of microbial activity on high-level nuclear waste and the long-term performance of the repository have not fully investigated, little microbial activity is expected in the near-field because of the radiation, lack of nutrients and the harsh conditions. However in the far-field microbial effects could be significant. Much of our understanding of the microbial effects on radionuclides stems from studies conducted with selected transuranic elements and fission products and limited studies with low-level radioactive wastes. Significant aerobic- and anaerobic-microbial activity is expected to occur in the waste because of the presence of electron donors and acceptors. The actinides initially may be present as soluble- or insoluble-forms but, after disposal, may be converted from one to the other by microorganisms. The direct enzymatic or indirect non-enzymatic actions of microbes could alter the speciation, solubility, and sorption properties of the actinides, thereby increasing or decreasing their concentrations in solution.

  9. Hitchhiking to speciation.

    Directory of Open Access Journals (Sweden)

    Daven C Presgraves

    Full Text Available The modern evolutionary synthesis codified the idea that species exist as distinct entities because intrinsic reproductive barriers prevent them from merging together. Understanding the origin of species therefore requires understanding the evolution and genetics of reproductive barriers between species. In most cases, speciation is an accident that happens as different populations adapt to different environments and, incidentally, come to differ in ways that render them reproductively incompatible. As with other reproductive barriers, the evolution and genetics of interspecific hybrid sterility and lethality were once also thought to evolve as pleiotripic side effects of adaptation. Recent work on the molecular genetics of speciation has raised an altogether different possibility-the genes that cause hybrid sterility and lethality often come to differ between species not because of adaptation to the external ecological environment but because of internal evolutionary arms races between selfish genetic elements and the genes of the host genome. Arguably one of the best examples supporting a role of ecological adaptation comes from a population of yellow monkey flowers, Mimulus guttatus, in Copperopolis, California, which recently evolved tolerance to soil contaminants from copper mines and simultaneously, as an incidental by-product, hybrid lethality in crosses with some off-mine populations. However, in new work, Wright and colleagues show that hybrid lethality is not a pleiotropic consequence of copper tolerance. Rather, the genetic factor causing hybrid lethality is tightly linked to copper tolerance and spread to fixation in Copperopolis by genetic hitchhiking.

  10. Speciation analysis of radionuclides

    International Nuclear Information System (INIS)

    Salbu, B.

    2010-01-01

    Full text: Naturally occurring and artificially produced radionuclides in the environment can be present in different physico-chemical forms (i. e. radionuclide species) varying in size (nominal molecular mass), charge properties and valence, oxidation state, structure and morphology, density, complexing ability etc. Low molecular mass (LMM) species are believed to be mobile and potentially bioavailable, while high molecular mass (HMM) species such as colloids, polymers, pseudocolloids and particles are considered inert. Due to time dependent transformation processes such as mobilization of radionuclide species from solid phases or interactions of mobile and reactive radionuclide species with components in soils and sediments, however, the original distribution of radionuclides deposited in ecosystems will change over time and influence the ecosystem behaviour. To assess the environmental impact from radionuclide contamination, information on radionuclide species deposited, interactions within affected ecosystems and the time-dependent distribution of radionuclide species influencing mobility and biological uptake is essential. The development of speciation techniques to characterize radionuclide species in waters, soils and sediments should therefore be essential for improving the prediction power of impact and risk assessment models. The present paper reviews fractionation techniques which should be utilised for radionuclide speciation purposes. (author)

  11. 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.)

  12. 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

  13. 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)

  14. 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

  15. 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.

  16. 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)

  17. 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)

  18. 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...

  19. 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

  20. 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

  1. 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.

  2. Electronic structure and correlation effects in actinides

    International Nuclear Information System (INIS)

    Albers, R.C.

    1998-01-01

    This report consists of the vugraphs given at a conference on electronic structure. Topics discussed are electronic structure, f-bonding, crystal structure, and crystal structure stability of the actinides and how they are inter-related

  3. BWR Assembly Optimization for Minor Actinide Recycling

    Energy Technology Data Exchange (ETDEWEB)

    G. Ivan Maldonado; John M. Christenson; J.P. Renier; T.F. Marcille; J. Casal

    2010-03-22

    The Primary objective of the proposed project is to apply and extend the latest advancements in LWR fuel management optimization to the design of advanced boiling water reactor (BWR) fuel assemblies specifically for the recycling of minor actinides (MAs).

  4. 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

  5. Robust membrane systems for actinide separations

    International Nuclear Information System (INIS)

    Jarvinen, Gordon D.; McCleskey, T. Mark; Bluhm, Elizabeth A.; Abney, Kent D.; Ehler, Deborah S.; Bauer, Eve; Le, Quyen T.; Young, Jennifer S.; Ford, Doris K.; Pesiri, David R.; Dye, Robert C.; Robison, Thomas W.; Jorgensen, Betty S.; Redondo, Antonio; Pratt, Lawrence R.; Rempe, Susan L.

    2000-01-01

    Our objective in this project is to develop very stable thin membrane structures containing ionic recognition sites that facilitate the selective transport of target metal ions, especially the actinides

  6. Speciation of An(IV) (Pu, Np, U and Th) in citrate media

    Energy Technology Data Exchange (ETDEWEB)

    Bonin, L.; Moisy, P. [CEA Valrho, DEN/DRCP/SCPS/LCA, Bagnols sur Ceze (France); Cote, G. [Ecole Nationale Superieure de Chimie, 75 - Paris (France)

    2008-07-01

    The acquisition of additional data concerning actinide decorporation is planned under the French nuclear and environmental toxicology program. Citric acid is a fundamental biological constituent found at relatively high concentrations in blood plasma and is involved in many biological processes. Spectrophotometry was the primary method used to determine the speciation of An(IV)-citrate systems (Th, U, Np, Pu). Complexation phenomena were identified, especially the formation of complexes with 1:1 and 1:2 stoichiometries. The corresponding conditional constants were calculated according to the experimental conditions. Depending on the acid-base form of the ligand (H{sub 2}Cit{sup -}, HCit{sup 2-} or Cit{sup 3-}) the apparent stability constants were also calculated and compared for various tetravalent actinides. (orig.)

  7. Speciation analysis on Eu(3) in aqueous solution using laser-induced breakdown spectroscopy

    International Nuclear Information System (INIS)

    Hotokezaka, H.; Tanaka, S.; Nagasaki, S.

    2001-01-01

    Investigation of the chemical behaviour of lanthanides and actinides in the geosphere is important for the safety assessment of high-level radioactive waste disposal. However, determination of speciation for lanthanides and actinides is difficult, because it is too hard to distinguish between metal ion and colloidal metal in aqueous solution. Laser-induced breakdown spectroscopy (LIBS) can detect both ions and microparticles of metals in aqueous solution, especially, high sensitive to microparticles. In this study, we analysed Eu(III) ion and Eu 2 O 3 particle in aqueous solution by LIBS, and measured the hydrolysis behaviour of Eu(III) in aqueous solution. Furthermore, we tried to detect the plasma emission of Eu(III) ions sorbed on TiO 2 particles, and also tried to observe the adsorption behaviour of Eu(III) ions onto TiO 2 particles in aqueous solution. (authors)

  8. Possible existence of backbending in actinide nuclei

    International Nuclear Information System (INIS)

    Dudek, J.; Nazarewicz, W.; Szymanski, Z.

    1982-01-01

    The possibilities for the backbending effect to occur in actinide nuclei are studied using the pairing-self-consistent independent quasiparticle method. The Hamiltonian used is that of the deformed Woods-Saxon potential plus monopole pairing term. The results of the calculations explain why there is no backbending in most actinide nuclei and simultaneously suggest that in some light neutron deficient nuclei around Th and 22 Ra a backbending effect may occur

  9. Lattice effects in the light actinides

    International Nuclear Information System (INIS)

    Lawson, A.C.; Cort, B.; Roberts, J.A.; Bennett, B.I.; Brun, T.O.; Dreele, R.B. von; Richardson, J.W. Jr.

    1998-01-01

    The light actinides show a variety of lattice effects that do not normally appear in other regions of the periodic table. The article will cover the crystal structures of the light actinides, their atomic volumes, their thermal expansion behavior, and their elastic behavior as reflected in recent thermal vibration measurements made by neutron diffraction. A discussion of the melting points will be given in terms of the thermal vibration measurements. Pressure effects will be only briefly indicated

  10. 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.

  11. Predictive Modeling in Actinide Chemistry and Catalysis

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Ping [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2016-05-16

    These are slides from a presentation on predictive modeling in actinide chemistry and catalysis. The following topics are covered in these slides: Structures, bonding, and reactivity (bonding can be quantified by optical probes and theory, and electronic structures and reaction mechanisms of actinide complexes); Magnetic resonance properties (transition metal catalysts with multi-nuclear centers, and NMR/EPR parameters); Moving to more complex systems (surface chemistry of nanomaterials, and interactions of ligands with nanoparticles); Path forward and conclusions.

  12. 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

  13. 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

  14. 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

  15. Positron Spectroscopy of Hydrothermally Grown Actinide Oxides

    Science.gov (United States)

    2014-03-27

    actinide oxides . The work described here is an attempt to characterize the quality of crystals using positron annihilation spectroscopy (PALS). The...Upadhyaya, R. V. Muraleedharan, B. D. Sharma and K. G. Prasad, " Positron lifetime studies on thorium oxide powders," Philosohical Magazine A, vol. 45... crystals . A strong foundation for actinide PALS studies was laid, but further work is required to build a more effective system. Positron Spectroscopy

  16. 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

  17. The removal of actinide metals from solution

    International Nuclear Information System (INIS)

    Hancock, R.D.; Howell, I.V.

    1980-01-01

    A process is specified for removing actinide metals (e.g. uranium) from solutions. The solution is contacted with a substrate comprising the product obtained by reacting an inorganic solid containing surface hydroxyl groups (e.g. silica gel) with a compound containing a silane grouping, a nitrogen-containing group (e.g. an amine) and other specified radicals. After treatment, the actinide metal is recovered from the substrate. (U.K.)

  18. 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)

  19. 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.)

  20. 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

  1. 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.)

  2. 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)

  3. Geochemistry of actinides. Application to the storage of high level radioactive wastes. Under the supervision of Mr Michel Treuil

    International Nuclear Information System (INIS)

    Bouabdallah, Noureddine; Cunault, Jean-Baptiste; Houtin, Gwenaelle; Leborgne, Francois; Lemaire, Celine; Lemarchand, Damien; Quitte, Ghylaine

    1997-06-01

    This collective research report first addresses the chemistry of actinides with a description of their atomic orbitals and the study of their behaviour in solution. The author addresses several aspects: historical overview on actinides, radioactivity, chemical reactions in aqueous solution, redox chemistry, speciation in solution with respect to water characteristics in deep storage conditions. The second part gathers several studies performed on a natural laboratory (the Oklo site in which nuclear reactions occurred about 2 billions years ago) and reports the modelling of radionuclide transfer within a geological system (the model is applied to the Oklo site). The third part addresses issues related to the nuclear fuel cycle, and the storage modes and materials envisaged and involved regarding the storage of high level radioactive wastes, notably in France

  4. Thoughts on environmental actinide research-future and present situation

    International Nuclear Information System (INIS)

    Yamamoto, Masayoshi

    2002-01-01

    Thoughts on environmental actinides, especially transuranium elements, are presented with emphasis on present situation and future researches. It is since 1945 that man has been in direct relationship to the significant quantities of such transuranium elements, although Pu was discovered in 1942 to exist in very small quantities in nature. Substantial amounts of these elements (Np, Pu, Am) have been distributed in the environment mainly as the result of nuclear weapon testing, followed by accident of satellite and release of radioactive substances from nuclear facilities. Chernobyl nuclear power plant accident might serve as a most recent example of such release. Considerable efforts have been devoted to the investigation of the processes involved in the transfer of radionuclides in the environment and how these can be influenced. And, many data (levels and distribution) and knowledge to understand these processes have been obtained and accumulated. The final purpose in all the research was the protection of the human being. The present trends for environmental radioactivity research (or radioecology) involves a further development of models, speciation of radionuclides, tracer studies and countermeasures of other species than man in radiological protection. Joint researches between radioecologists and specialists such as meteorology, oceanography, geology, botany, statistics and so on are more and more needed to make one of the most fascinating environmental sciences. Finally, an effort should be made to develop radioecology into a more hypothesis-oriented science, as mentioned by Platt. (author)

  5. Recovery of Actinides from Actinide-Aluminium Alloys: Chlorination Route

    International Nuclear Information System (INIS)

    Mendes, E.; Malmbeck, R.; Soucek, P.; Jardin, R.; Glatz, J.P.; Cassayre, L.

    2008-01-01

    A method for recovery of actinides (An) from An-Al alloys formed by electrochemical separation of metallic spent nuclear fuel on solid aluminium electrodes in molten chloride salts is described. The proposed route consists of three main steps: -) vacuum distillation of salt adhered on the electrodes, -) chlorination of An-Al alloy by pure chlorine gas and -) sublimation of formed AlCl 3 . A thermochemical study of the route was performed to determine important chemical reactions and to find optimum experimental conditions for all process steps. Vacuum distillation of the electrode is efficient for complete removal of remaining salt and most fission products, full chlorination of the An-Al alloys is possible at any working temperature and evaporation of AlCl 3 is achieved by heating under argon. Experiments have been carried out using U-Al alloy in order to define parameters providing full alloy chlorination without formation of volatile UCl 5 and UCl 6 . It was shown that full chlorination of An-Al alloys without An losses should be possible at a temperature approx. 150 deg. C. (authors)

  6. Recovery of Actinides from Actinide-Aluminium Alloys: Chlorination Route

    Energy Technology Data Exchange (ETDEWEB)

    Mendes, E.; Malmbeck, R.; Soucek, P.; Jardin, R.; Glatz, J.P. [European Commission, JRC, Institute for Transuranium Elements, Postfach 2340, 76125 Karlsruhe (Germany); Cassayre, L. [Laboratoire de Genie Chimique (LGC), Universite Paul Sabatier, UMR CNRS 5503, 118 route de Narbonne, 31062 Toulouse Cedex 04 (France)

    2008-07-01

    A method for recovery of actinides (An) from An-Al alloys formed by electrochemical separation of metallic spent nuclear fuel on solid aluminium electrodes in molten chloride salts is described. The proposed route consists of three main steps: -) vacuum distillation of salt adhered on the electrodes, -) chlorination of An-Al alloy by pure chlorine gas and -) sublimation of formed AlCl{sub 3}. A thermochemical study of the route was performed to determine important chemical reactions and to find optimum experimental conditions for all process steps. Vacuum distillation of the electrode is efficient for complete removal of remaining salt and most fission products, full chlorination of the An-Al alloys is possible at any working temperature and evaporation of AlCl{sub 3} is achieved by heating under argon. Experiments have been carried out using U-Al alloy in order to define parameters providing full alloy chlorination without formation of volatile UCl{sub 5} and UCl{sub 6}. It was shown that full chlorination of An-Al alloys without An losses should be possible at a temperature approx. 150 deg. C. (authors)

  7. Speciation of radionuclides in natural groundwaters: Annual report for the period October 1986 through September 1987

    International Nuclear Information System (INIS)

    Doxtader, M.M.; Beitz, J.V.; Reed, D.T.; Bates, J.K.

    1988-02-01

    Two ultrasensitive laser techniques, laser photoacoustic spectroscopy (LPAS) and laser-induced fluorescence (LIF), are being developed for the detection and speciation of trace levels of actinides in solutions typical of those expected in a high-level waste repository. An LPAS system was set up for these studies. Experiments were carried out to determine the detection limits of plutonium and americium in solution. Concurrently with the LPAS work, LIF studies were carried out on uranyl ion and curium in solution. 32 refs., 35 figs., 8 tabs

  8. Study of Np speciation in citrate medium

    Energy Technology Data Exchange (ETDEWEB)

    Bonin, L.; Den Auwer, C.; Ansoborlo, E.; Moisy, P. [CEA Valrho - DEN/DRCP/SCPS, Bagnols sur Ceze (France); Cote, G. [ENSP - LECA, UMR 7575, Paris (France)

    2007-07-01

    In the framework of the French Environmental Nuclear Toxicology program, additional experiments related to the decorporation of actinides are planned. Decorporation is the removal or release from target organs (bones, liver, kidney..), tissues or cells of radioactive material previously incorporated in them, using chelating agents or other administrated pharmaceutical agents. The contradictory data on the neptunium complexation behaviour within blood and its transfer to target organs, as well as the inefficiency of therapeutic treatments, led us to study the complexation of this element with biological constituents. Within this purpose, the in vitro behaviour of Np(IV) and Np(V) in simple media simulating biological fluids was studied. This study was more specifically focused on the behaviour of neptunium with citrate ion, which is an essential component in a number of metalloenzyme active sites. In order to determine the speciation of this system, spectrophotometry was more particularly used. Concerning the complexation phenomenon, the existence of several complexes of Np(V) with various acido-basic forms of the citrate anion was observed; regarding Np(IV), complexes with Cit{sup 3-} have been observed. From the quantitative study of these equilibria, the values of the absolute constants for the complexation of Np(IV) and Np(V) with citrate were determined. Concerning the stability of neptunium towards oxydo-reduction, it was confirmed that Np(VI) was very quickly reduced to Np(V) by the citrate anions, whereas Np(IV) was stable. In the case of Np(V), it was observed that, depending on the pH and the citrate concentration, Np(V) was unstable and was reduced to Np(IV). The E-pH diagrams, constructed using the stability constants determined in this study, showed that this instability was due to the Np(V) disproportionation. (orig.)

  9. 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

  10. 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.

  11. Modelling interaction of deep groundwaters with bentonite and radionuclide speciation

    International Nuclear Information System (INIS)

    Wanner, H.

    1986-04-01

    In the safety analysis recently reported for a potential Swiss high-level waste repository, radionuclide speciation and solubility limits are calculated for expected granitic groundwater conditions. With the objective of deriving a more realistic description of radionuclide release from the near-field, an investigation has been initiated to quantitatively specify the chemistry of the near-field. In the Swiss case, the main components of the near-field are the glass waste-matrix, a thick steel canister horizontally emplaced in a drift, and a backfill of highly compacted sodium bentonite. This report describes a thermodynamic model which is used to estimate the chemical composition of the pore water in compacted sodium bentonite. Solubility limits and speciation of important actinides and the fission product technetium in the bentonite pore water are then calculated. The model is based on available experimental data on the interaction of sodium bentonite and groundwater and represents means of extrapolation from laboratory data to repository conditions. The modelled composition of the pore water of compacted sodium bentonite, as well as the various compositions resulting from the long-term extrapolation, are used to estimate radionuclide solubilities in the near-field of a deep repository. From the chemical point of view, calcium bentonite seems to be more stable than sodium bentonite in the presence of Swiss Reference Groundwater. Since the effect of calcium bentonite on the groundwater chemical composition will be considerably less marked than that of sodium bentonite, especially with respect to key parameters for the nuclide speciation like carbonate concentration and pH, the use of calcium bentonite instead of sodium bentonite will improve the reliability in the prediction of source terms for radionuclide transport in the geosphere. (author)

  12. Actinide transmutation in nuclear reactors

    International Nuclear Information System (INIS)

    Bultman, J.H.

    1995-01-01

    An optimization method is developed to maximize the burning capability of the ALMR while complying with all constraints imposed on the design for reliability and safety. This method leads to a maximal transuranics enrichment, which is being limited by constraints on reactivity. The enrichment can be raised by using the neutrons less efficiently by increasing leakage from the fuel. With the developed optimization method, a metallic and an oxide fueled ALMR were optimized. Both reactors perform equally well considering the burning of transuranics. However, metallic fuel has a much higher heat conductivity coefficient, which in general leads to better safety characteristics. In search of a more effective waste transmuter, a modified Molten Salt Reactor was designed. A MSR operates on a liquid fuel salt which makes continuous refueling possible, eliminating the issue of the burnup reactivity loss. Also, a prompt negative reactivity feedback is possible for an overmoderated reactor design, even when the Doppler coefficient is positive, due to the fuel expansion with fuel temperature increase. Furthermore, the molten salt fuel can be reprocessed based on a reduction process which is not sensitive to the short-lived spontaneously fissioning actinides. (orig./HP)

  13. Actinide/crown ether chemistry

    International Nuclear Information System (INIS)

    Benning, M.M.

    1988-01-01

    A structural survey of actinide/crown ether compounds was conducted in order to investigate the solid state chemistry of these complexes. Several parameters - the metal size, crown type, counterion, solvent systems and reaction and crystallization conditions - were varied to correlate their importance in complexation. Under atmospheric conditions, two types of complexes were isolated, those containing only hydrogen-bonded crown interactions and instances where the crown interacts directly with the metal center. In both cases, water seems to play a very important role. When coordinated to the metal, water molecules exhibit the necessary donor properties required for the formation of hydrogen-bonded contacts. The water molecules also provide fierce competition with the crown ethers for metal-binding sites and in most cases prohibit the formation of complexes in which direct metal-ligand association exists. The results of this study indicate that direct interaction between the metal atoms and the crown ethers, in the presence of water, can only occur with polyether conformations which limit the steric replusions within the metal coordination sphere

  14. Actinide transmutation in nuclear reactors

    Energy Technology Data Exchange (ETDEWEB)

    Bultman, J H

    1995-01-17

    An optimization method is developed to maximize the burning capability of the ALMR while complying with all constraints imposed on the design for reliability and safety. This method leads to a maximal transuranics enrichment, which is being limited by constraints on reactivity. The enrichment can be raised by using the neutrons less efficiently by increasing leakage from the fuel. With the developed optimization method, a metallic and an oxide fueled ALMR were optimized. Both reactors perform equally well considering the burning of transuranics. However, metallic fuel has a much higher heat conductivity coefficient, which in general leads to better safety characteristics. In search of a more effective waste transmuter, a modified Molten Salt Reactor was designed. A MSR operates on a liquid fuel salt which makes continuous refueling possible, eliminating the issue of the burnup reactivity loss. Also, a prompt negative reactivity feedback is possible for an overmoderated reactor design, even when the Doppler coefficient is positive, due to the fuel expansion with fuel temperature increase. Furthermore, the molten salt fuel can be reprocessed based on a reduction process which is not sensitive to the short-lived spontaneously fissioning actinides. (orig./HP).

  15. Lithium actinide recycle process demonstration

    Energy Technology Data Exchange (ETDEWEB)

    Johnson, G.K.; Pierce, R.D.; McPheeters, C.C. [Argonne National Laboratory, IL (United States)

    1995-10-01

    Several pyrochemical processes have been developed in the Chemical Technology Division of Argonne Laboratory for recovery of actinide elements from LWR spent fuel. The lithium process was selected as the reference process from among the options. In this process the LWR oxide spent fuel is reduced by lithium at 650{degrees}C in the presence of molten LiCl. The Li{sub 2}O formed during the reduction process is soluble in the salt. The spent salt and lithium are recycled after the Li{sub 2}O is electrochemically reduced. The oxygen is liberated as CO{sub 2} at a carbon anode or oxygen at an inert anode. The reduced metal components of the LWR spent fuel are separated from the LiCL salt phase and introduced into an electrorefiner. The electrorefining step separates the uranium and transuranium (TRU) elements into two product streams. The uranium product, which comprises about 96% of the LWR spent fuel mass, may be enriched for recycle into the LWR fuel cycle, stored for future use in breeder reactors, or converted to a suitable form for disposal as waste. The TRU product can be recycled as fast reactor fuel or can be alloyed with constituents of the LWR cladding material to produce a stable waste form.

  16. Actinides and rare earths complexation with adenosine phosphate nucleotides

    International Nuclear Information System (INIS)

    Mostapha, Sarah

    2013-01-01

    Organophosphorus compounds are important molecules in both nuclear industry and living systems fields. Indeed, several extractants of organophosphorus compounds (such as TBP, HDEHP) are used in the nuclear fuel cycle reprocessing and in the biological field. For instance, the nucleotides are organophosphates which play a very important role in various metabolic processes. Although the literature on the interactions of actinides with inorganic phosphate is abundant, published studies with organophosphate compounds are generally limited to macroscopic and / or physiological approaches. The objective of this thesis is to study the structure of several organophosphorus compounds with actinides to reach a better understanding and develop new specific buildings blocks. The family of the chosen molecules for this procedure consists of three adenine nucleotides mono, bi and triphosphate (AMP, adenosine monophosphate - ADP, adenosine diphosphate - ATP, adenosine triphosphate) and an amino-alkylphosphate (AEP O-phosphoryl-ethanolamine). Complexes synthesis was conducted in aqueous and weakly acidic medium (2.8-4) for several lanthanides (III) (Lu, Yb, Eu) and actinides (U (VI), Th (IV) and Am (III)). Several analytical and spectroscopic techniques have been used to describe the organization of the synthesized complexes: spectrometric analysis performed by FTIR and NMR were used to identify the functional groups involved in the complexation, analysis by ESI-MS and pH-metric titration were used to determine the solution speciation and EXAFS analyzes were performed on Mars beamline of the SOLEIL synchrotron, have described the local cation environment, for both solution and solid compounds. Some theoretical approaches of DFT were conducted to identify stable structures in purpose of completing the experimental studies. All solid complexes (AMP, ADP, ATP and AEP) have polynuclear structures, while soluble ATP complexes are mononuclear. For all synthesized complexes, it has been

  17. 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

  18. Speciation and bioaccumulation in a model organism of U, Np and Am in the marine environment

    International Nuclear Information System (INIS)

    Maloubier, Melody

    2015-01-01

    The fate of natural and anthropogenic radionuclides in the environment remains a major concern in our modern nuclearized societies. Among the environmental compartments, the hydrosphere is ubiquitous and can transport compounds or elements over very long distances. The recent event of Fukushima demonstrated that the marine environment could be directly affected and this raises both scientific and societal questions. Moreover, some studies have already shown that radionuclides present in seawater can be strongly accumulated by marine organisms although their speciation is most of the time unknown. Yet this knowledge is essential to better understand the transfer mechanisms from the hydrosphere to the biosphere and to evaluate their global impact on humans. In this work, we chose to experimentally determine the speciation of three actinides in doped seawater: uranium(VI), neptunium(V) and americium(III) (and the chemical surrogate europium(III)) by coupling speciation modeling with spectroscopic tools among which Time-Resolved Laser-Induced Fluorescence (TRLIF) and X-ray Absorption Spectroscopy (XAS). Then, we have studied the accumulation process in the sponge A. cavernicola, chosen here because it is considered as a bio-monitor of heavy metal pollution. The accumulation of europium(III), americium(III) and uranium(VI) in A. cavernicola were investigated at trace and ultra-trace levels. Besides, for europium, X-ray and electronic imaging permit to localize the accumulated element in the sponge and to specify its speciation [fr

  19. 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

  20. Use of fast reactors for actinide transmutation

    International Nuclear Information System (INIS)

    1993-03-01

    The management of radioactive waste is one of the key issues in today's discussions on nuclear energy, especially the long term disposal of high level radioactive wastes. The recycling of plutonium in liquid metal fast breeder reactors (LMFBRs) would allow 'burning' of the associated extremely long life transuranic waste, particularly actinides, thus reducing the required isolation time for high level waste from tens of thousands of years to hundreds of years for fission products only. The International Working Group on Fast Reactors (IWGFR) decided to include the topic of actinide transmutation in liquid metal fast breeder reactors in its programme. The IAEA organized the Specialists Meeting on Use of Fast Breeder Reactors for Actinide Transmutation in Obninsk, Russian Federation, from 22 to 24 September 1992. The specialists agree that future progress in solving transmutation problems could be achieved by improvements in: Radiochemical partitioning and extraction of the actinides from the spent fuel (at least 98% for Np and Cm and 99.9% for Pu and Am isotopes); technological research and development on the design, fabrication and irradiation of the minor actinides (MAs) containing fuels; nuclear constants measurement and evaluation (selective cross-sections, fission fragments yields, delayed neutron parameters) especially for MA burners; demonstration of the feasibility of the safe and economic MA burner cores; knowledge of the impact of maximum tolerable amount of rare earths in americium containing fuels. Refs, figs and tabs

  1. 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.

  2. 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

  3. 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

  4. 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.

  5. X exceptionalism in Caenorhabditis speciation.

    Science.gov (United States)

    Cutter, Asher D

    2017-11-13

    Speciation genetics research in diverse organisms shows the X-chromosome to be exceptional in how it contributes to "rules" of speciation. Until recently, however, the nematode phylum has been nearly silent on this issue, despite the model organism Caenorhabditis elegans having touched most other topics in biology. Studies of speciation with Caenorhabditis accelerated with the recent discovery of species pairs showing partial interfertility. The resulting genetic analyses of reproductive isolation in nematodes demonstrate key roles for the X-chromosome in hybrid male sterility and inviability, opening up new understanding of the genetic causes of Haldane's rule, Darwin's corollary to Haldane's rule, and enabling tests of the large-X effect hypothesis. Studies to date implicate improper chromatin regulation of the X-chromosome by small RNA pathways as integral to hybrid male dysfunction. Sexual transitions in reproductive mode to self-fertilizing hermaphroditism inject distinctive molecular evolutionary features into the speciation process for some species. Caenorhabditis also provides unique opportunities for analysis in a system with XO sex determination that lacks a Y-chromosome, sex chromosome-dependent sperm competition differences and mechanisms of gametic isolation, exceptional accessibility to the development process and rapid experimental evolution. As genetic analysis of reproductive isolation matures with investigation of multiple pairs of Caenorhabditis species and new species discovery, nematodes will provide a powerful complement to more established study organisms for deciphering the genetic basis of and rules to speciation. © 2017 John Wiley & Sons Ltd.

  6. CHURCH, Category, and Speciation

    Directory of Open Access Journals (Sweden)

    Rinderknecht Jakob Karl

    2018-01-01

    Full Text Available The Roman Catholic definition of “church”, especially as applied to groups of Protestant Christians, creates a number of well-known difficulties. The similarly complex category, “species,” provides a model for applying this term so as to neither lose the centrality of certain examples nor draw a hard boundary to rule out border cases. In this way, it can help us to more adequately apply the complex ecclesiology of the Second Vatican Council. This article draws parallels between the understanding of speciation and categorization and the definition of Church since the council. In doing so, it applies the work of cognitive linguists, including George Lakoff, Zoltan Kovecses, Giles Fauconnier and Mark Turner on categorization. We tend to think of categories as containers into which we sort objects according to essential criteria. However, categories are actually built inductively by making associations between objects. This means that natural categories, including species, are more porous than we assume, but nevertheless bear real meaning about the natural world. Taxonomists dispute the border between “zebras” and “wild asses,” but this distinction arises out of genetic and evolutionary reality; it is not merely arbitrary. Genetic descriptions of species has also led recently to the conviction that there are four species of giraffe, not one. This engagement will ground a vantage point from which the Council‘s complex ecclesiology can be more easily described so as to authentically integrate its noncompetitive vision vis-a-vis other Christians with its sense of the unique place held by Catholic Church.

  7. Cancer: beyond speciation.

    Science.gov (United States)

    Vincent, Mark D

    2011-01-01

    A good account of the nature of cancer should provide not only a description of its consistent features, but also how they arise, how they are maintained, why conventional chemotherapy succeeds, and fails, and where to look for better targets. Cancer was once regarded as enigmatic and inexplicable; more recently, the "mutation theory," based on random alterations in a relatively small set of proto-oncogenes and tumor suppressor genes, has enjoyed widespread acceptance. The "mutation theory," however, is noticeable for its failure to explain the basis of differential chemosensitivity, for providing a paucity of targets, especially druggable ones, and for justifying the development of targeted therapies with, in general, disappointingly abbreviated clinical benefit. Furthermore, this theory has mistakenly predicted a widespread commonality of consistent genetic abnormalities across the range of cancers, whereas the opposite, that is, roiling macrogenomic instability, is generally the rule. In contrast, concerning what actually is consistent, that is, the suite of metabolic derangements common to virtually all, especially aggressive, cancers, the "Mutation Theory" has nothing to say. Other hypotheses merit serious consideration "aneuploidy theories" posit whole-genome instability and imbalance as causally responsible for the propagation of the tumor. Another approach, that is, "derepression atavism," suggests cancer results from the release of an ancient survival program, characterized by the emergence of remarkably primitive features such as unicellularity, fermentation, and immortality; existential goals are served by heuristic genomic instability coupled with host-to-tumor biomass interconversion, mediated by the Warburg effect, a major component of the program. Carcinogenesis is here seen as a process of de-speciation; however, genomic nonrestabilization raises issues as to where on the tree of life cancers belong, as a genuinely alternative modus vivendi

  8. CONCAWE effluent speciation project

    Energy Technology Data Exchange (ETDEWEB)

    Leonards, P.; Comber, M.; Forbes, S.; Whale, G.; Den Haan, K.

    2010-09-15

    In preparation for the implementation of the EU REACH regulation, a project was undertaken to transfer the high-resolution analytical method for determining hydrocarbon blocks in petroleum products by comprehensive two-dimensional gas chromatography (GCxGC) to a laboratory external to the petroleum industry (Institute for Environmental Studies (IVM) of the VU University of Amsterdam). The method was validated and used for the analysis of petroleum hydrocarbons extracted from refinery effluents. The report describes the technology transfer and the approaches used to demonstrate the successful transfer and application of the GCxGC methodology from analysing petroleum products to the quantitative determination of hydrocarbon blocks in refinery effluents. The report describes all the methods used for all the determinations on the effluent samples along with an overview of the results obtained which are presented in summary tables and graphs. These data have significantly improved CONCAWE's knowledge of what refineries emit in their effluents. A total of 111 Effluent Discharge Samples from 105 CONCAWE refineries in Europe were obtained in the period June 2008 to March 2009. These effluents were analysed for metals, standard effluent parameters (including COD, BOD), oil in water, BTEX and volatile organic compounds. The hydrocarbon speciation determinations and other hydrocarbon analyses are also reported. The individual refinery analytical results are included into this report, coded as per the CONCAWE system. These data will be, individually, communicated to companies and refineries. The report demonstrates that it is feasible to conduct a research programme to investigate the fate and effects of hydrocarbon blocks present in discharged refinery effluents.

  9. 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

  10. 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.

  11. Sympatric Speciation in Threespine Stickleback: Why Not?

    Directory of Open Access Journals (Sweden)

    Daniel I. Bolnick

    2011-01-01

    Full Text Available Numerous theoretical models suggest that sympatric speciation is possible when frequency-dependent interactions such as intraspecific competition drive disruptive selection on a trait that is also subject to assortative mating. Here, I review recent evidence that both conditions are met in lake populations of threespine stickleback (Gasterosteus aculeatus. Nonetheless, sympatric speciation appears to be rare or absent in stickleback. If stickleback qualitatively fit the theoretical requirements for sympatric speciation, why do they not undergo sympatric speciation? I present simulations showing that disruptive selection and assortative mating in stickleback, though present, are too weak to drive speciation. Furthermore, I summarize empirical evidence that disruptive selection in stickleback drives other forms of evolutionary diversification (plasticity, increased trait variance, and sexual dimorphism instead of speciation. In conclusion, core assumptions of sympatric speciation theory seem to be qualitatively reasonable for stickleback, but speciation may nevertheless fail because of (i quantitative mismatches with theory and (ii alternative evolutionary outcomes.

  12. Special actinide nuclides: Fuel or waste?

    International Nuclear Information System (INIS)

    Srinivasan, M.; Rao, K.S.; Dingankar, M.V.

    1989-01-01

    The special actinide nuclides such as Np, Cm, etc. which are produced as byproducts during the operation of fission reactors are presently looked upon as 'nuclear waste' and are proposed to be disposed of as part of high level waste in deep geological repositories. The potential hazard posed to future generations over periods of thousands of years by these long lived nuclides has been a persistent source of concern to critics of nuclear power. However, the authors have recently shown that each and every one of the special actinide nuclides is a better nuclear fuel than the isotopes of plutonium. This finding suggests that one does not have to resort to exotic neutron sources for transmuting/incinerating them as proposed by some researchers. Recovery of the special actinide elements from the waste stream and recycling them back into conventional fission reactors would eliminate one of the stigmas attached to nuclear energy

  13. Actinide distribution in the human skeleton

    International Nuclear Information System (INIS)

    Kathren, R.L.; McInroy, J.F.; Swint, M.J.

    1985-05-01

    Radiochemical analysis of two half skeletons donated to the United States Transuranium Registry, one from an individual with an occupationally incurred deposition of 241 Am and the other with a deposition of 239 Pu, revealed an inverse linear relationship between the concentration of actinide in the bone ash and the fraction of ash. Two distinct relationships were noted, one for the cranium and the other for the remainder of the skeleton. The results suggest that the actinide content of the skeleton as a whole, Q, can be obtained with an uncertainty of +-50% from analysis of a single sample of any bone (except the cranium) by Q = [(830 C/sub sample/)/(0.61 - f/sub sample/)], in which C/sub sample/ refers to the actinide content per g of ash and f/sub sample/ the fraction of ash (i.e., ratio of dry to wet weight) in the sample. 5 figs., 3 tabs

  14. Neutron scattering studies of the actinides

    International Nuclear Information System (INIS)

    Lander, G.H.

    1979-01-01

    The electronic structure of actinide materials presents a unique example of the interplay between localized and band electrons. Together with a variety of other techniques, especially magnetization and the Mossbauer effect, neutron studies have helped us to understand the systematics of many actinide compounds that order magnetically. A direct consequence of the localization of 5f electrons is the spin-orbit coupling and subsequent spin-lattice interaction that often leads to strongly anisotropic behavior. The unusual phase transition in UO 2 , for example, arises from interactions between quadrupole moments. On the other hand, in the monopnictides and monochalcogenides, the anisotropy is more difficult to understand, but probably involves an interaction between actinide and anion wave functions. A variety of neutron experiments, including form-factor studies, critical scattering and measurements of the elementary excitations have now been performed, and the conceptual picture emerging from these studies will be discussed

  15. Monazite as a suitable actinide waste form

    Energy Technology Data Exchange (ETDEWEB)

    Schlenz, Hartmut; Heuser, Julia; Schmitz, Stephan; Bosbach, Dirk [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Energie und Klimaforschung (IEK), Nukleare Entsorgung und Reaktorsicherheit (IEK-6); Neumann, Andreas [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Energie und Klimaforschung (IEK), Nukleare Entsorgung und Reaktorsicherheit (IEK-6); RWTH Aachen Univ. (Germany). Inst. for Crystallography

    2013-03-01

    The conditioning of radioactive waste from nuclear power plants and in some countries even of weapons plutonium is an important issue for science and society. Therefore the research on appropriate matrices for the immobilization of fission products and actinides is of great interest. Beyond the widely used borosilicate glasses, ceramics are promising materials for the conditioning of actinides like U, Np, Pu, Am, and Cm. Monazite-type ceramics with general composition LnPO{sub 4} (Ln = La to Gd) and solid solutions of monazite with cheralite or huttonite represent important materials in this field. Monazite appears to be a promising candidate material, especially because of its outstanding properties regarding radiation resistance and chemical durability. This article summarizes the most recent results concerning the characterization of monazite and respective solid solutions and the study of their chemical, thermal, physical and structural properties. The aim is to demonstrate the suitability of monazite as a secure and reliable waste form for actinides. (orig.)

  16. 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

  17. 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

  18. 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

  19. 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...

  20. Sequential analysis of selected actinides in urine

    International Nuclear Information System (INIS)

    Kramer, G.H.

    1980-07-01

    The monitoring of personnel by urinalysis for suspected contamination by actinides necessitated the development and implementation of an analytical scheme that will separate and identify alpha emitting radionuclides of these elements. The present work deals with Pu, Am, and Th. These elements are separated from an ashed urine sample by means of coprecipitation and ion exchange techniques. The final analysis is carried out by electroplating the actinides and counting in a α-spectrometer. Mean recoveries of these elements from urine are: Pu 64%, Am 74% and Th 69%. (auth)

  1. Aqueous actinide complexes: A thermochemical assessment

    International Nuclear Information System (INIS)

    Fuger, J.; Khodakovsky, I.L.; Medvedev, V.A.; Navratil, J.D.

    1979-01-01

    The scope and purpose of an assessment of the thermodynamic properties of the aqueous actinide complexes are presented. This work which, at present, is limited to inorganic ligands and three selected organic ligands (formate, acetate and oxalate), is part of an effort established by the International Atomic Energy Agency to assess the thermodynamic properties of the actinides and their compounds. The problems involved in this work are illustrated by discussing the present status of the assessment as related to a few complex species, (hydroxyl-, fluoride-, carbonate complexes). (orig.) [de

  2. Actinide elements in aquatic and terrestrial environments

    International Nuclear Information System (INIS)

    Bondietti, E.A.; Bogle, M.A.; Brantley, J.N.

    1979-01-01

    Progress is reported on the following research projects: water-sediment interactions of U, Pu, Am, and Cm; relative availability of actinide elements from abiotic to aquatic biota; comparative uptake of transuranic elements by biota bordering Pond 3513; metabolic reduction of 239 Np from Np(V) to Np(IV) in cotton rats; evaluation of hazards associated with transuranium releases to the biosphere; predicting Pu in bone; adsorption--solubility--complexation phenomena in actinide partitioning between sorbents and solution; comparative soil extraction data; and comparative plant uptake data

  3. 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

  4. Actinide phosphonate complexes in aqueous solutions

    International Nuclear Information System (INIS)

    Nash, K.L.

    1993-01-01

    Complexes formed by actinides with carboxylic acids, polycarboxylic acids, and aminopolycarboxylic acids play a central role in both the basic and process chemistry of the actinides. Recent studies of f-element complexes with phosphonic acid ligands indicate that new ligands incorporating doubly ionizable phosphonate groups (-PO 3 H 2 ) have many properties which are unique chemically, and promise more efficient separation processes for waste cleanup and environmental restoration. Simple diphosphonate ligands form much stronger complexes than isostructural carboxylates, often exhibiting higher solubility as well. In this manuscript recent studies of the thermodynamics and kinetics of f-element complexation by 1,1 and 1,2 diphosphonic acid ligands are described

  5. A worldwide perspective on actinide burning

    International Nuclear Information System (INIS)

    Burch, W.D.

    1991-01-01

    Worldwide interest has been evident over the past few years in reexamining the merits of recovering the actinides from spent light-water reactor (LWR) fuel and transmuting them in fast reactors to reduce hazards in geologic repositories. This paper will summarize some of the recent activities in this field. Several countries are embarked on programs of reprocessing and vitrification of present wastes, from which removal of the actinides is largely precluded. The United States is assessing the ideas related to the fast reactor program and the potential application to defense wastes. 18 refs., 2 figs

  6. Molecular dynamics studies of actinide nitrides

    International Nuclear Information System (INIS)

    Kurosaki, Ken; Uno, Masayoshi; Yamanaka, Shinsuke; Minato, Kazuo

    2004-01-01

    The molecular dynamics (MD) calculation was performed for actinide nitrides (UN, NpN, and PuN) in the temperature range from 300 to 2800 K to evaluate the physical properties viz., the lattice parameter, thermal expansion coefficient, compressibility, and heat capacity. The Morse-type potential function added to the Busing-Ida type potential was employed for the ionic interactions. The interatomic potential parameters were determined by fitting to the experimental data of the lattice parameter. The usefulness and applicability of the MD method to evaluate the physical properties of actinide nitrides were studied. (author)

  7. Actinide and fission product separation and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1993-07-01

    The second international information exchange meeting on actinide and fission product separation and transmutation, took place in Argonne National Laboratory in Illinois United States, on 11-13 November 1992. The proceedings are presented in four sessions: Current strategic system of actinide and fission product separation and transmutation, progress in R and D on partitioning processes wet and dry, progress in R and D on transmutation and refinements of neutronic and other data, development of the fuel cycle processes fuel types and targets. (A.L.B.)

  8. Static and dynamic deformations of actinide nuclei

    International Nuclear Information System (INIS)

    Rozmej, P.

    1985-09-01

    The zero-point quadrupole-hexadecapole vibrations have been taken into account to calculate dynamical deformations for even-even actinide nuclei. The collective and intrinsic motions are separated according to the Born-Oppenheimer approximation. The collective Hamiltonian is constructed using the macroscopic-microscopic method in the potential energy part and the cranking model in the kinetic energy part. The BCS theory with a modified oscillator potential is applied to describe the intrinsic motion of nucleons. A new set of Nilsson potential parameters, which produces a much better description of the properties of light actinide nuclei, has also been found. (orig.)

  9. Spin–orbit coupling in actinide cations

    DEFF Research Database (Denmark)

    Bagus, Paul S.; Ilton, Eugene S.; Martin, Richard L.

    2012-01-01

    The limiting case of Russell–Saunders coupling, which leads to a maximum spin alignment for the open shell electrons, usually explains the properties of high spin ionic crystals with transition metals. For actinide compounds, the spin–orbit splitting is large enough to cause a significantly reduced...... spin alignment. Novel concepts are used to explain the dependence of the spin alignment on the 5f shell occupation. We present evidence that the XPS of ionic actinide materials may provide direct information about the angular momentum coupling within the 5f shell....

  10. Scanning transmission X-ray microscopy as a speciation tool for natural organic molecules

    Energy Technology Data Exchange (ETDEWEB)

    Rothe, J.; Plaschke, M.; Denecke, M.A. [Inst. fuer Nukleare Entsorgung, Forschungszentrum Karlsruhe, Karlsruhe (Germany)

    2004-07-01

    A molecular-scale understanding of the basic processes affecting stability and transport behavior of actinide cations, complexes or hydroxide ('eigencolloid') species is prerequisite to performance assessment of nuclear waste disposal in geological formations. Depending on their functional group chemistry and macromolecular structure, naturally occurring organic molecules (NOM) possess a high tendency towards actinide complexation reactions. However, the compositional and structural heterogeneity of NOM and mixed aggregates with inorganic phases makes speciation by spectromicroscopy techniques highly desirable. The applicability of Scanning Transmission X-ray Microscopy (STXM) as a speciation tool for the characterization of NOM is demonstrated for a multifunctional natural organic acid (chlorogenic acid), Eu(III)-loaded humic acid (HA) aggregates and Eu(III)-oxo/hydroxide/HA hetero-aggregates. It is shown that in situ probing of HA functional group chemistry down to a spatial resolution < 100 nm (i.e., less than femto-liter sampled volumes) is feasible, at the same time revealing morphological details on NOM aggregates and NOM/mineral associations. (orig.)

  11. 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

  12. 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

  13. 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

  14. Transmutation of LWR waste actinides in thermal reactors

    International Nuclear Information System (INIS)

    Gorrell, T.C.

    1979-01-01

    Recycle of actinides to a reactor for transmutation to fission products is being considered as a possible means of waste disposal. Actinide transmutation calculations were made for two irradiation options in a thermal (LWR) reactor. The cases considered were: all actinides recycled in regular uranium fuel assemblies, and transuranic actinides recycled in separate mixed oxide (MOX) assemblies. When all actinides were recycled in a uranium lattice, a reduction of 62% in the transuranic inventory was achieved after 10 recycles, compared to the inventory accumulated without recycle. When the transuranics from 2 regular uranium assemblies were combined with those recycled from a MOX assembly, the transuranic inventory was reduced 50% after 5 recycles

  15. Microbial Transformations of TRU and Mixed Wastes: Actinide Speciation and Waste Volume Reduction

    International Nuclear Information System (INIS)

    Halada, Gary P.

    2006-01-01

    During the past year, both a graduate student and a visiting summer undergraduate research assistant have conducted experiments concerning interaction of metals with fresh and aged cellulosic materials

  16. Speciation and surface interactions of actinides on aged ion-exchange resins

    International Nuclear Information System (INIS)

    Morris, D.E.; Buscher, C.T.; Donohoe, R.J.

    1997-01-01

    The United States Department of Energy is presently faced with the stabilization and safe disposition of hundreds of metric tons of residue materials resulting from 50+ years of nuclear weapons production activities. These residues encompass a broad range of substrates and radionuclides and include both solid and liquid materials. Combustible residues constitute a significant fraction of the total residue inventory, and an important constituent within the combustible category is spent anion ion-exchange resins. These resins are typically utilized for the separation of plutonium from other radionuclides under strongly acidic nitric or hydrochloric acid solution conditions which favor the formation and partitioning of anionic Pu(IV) nitrato or chloride species. The spent resins are usually rinsed prior to storage as residues to reduce both acid and radionuclide concentrations, but significant radionuclide concentrations remain in these resins, and the long-term effects of concentrated acid and radiolysis on the resin integrity are relatively unexplored. Thus, new research is needed to assess the stability of these resin residues and address the need for further treatment to ensure stability prior to long-term disposal

  17. Neutral Models with Generalised Speciation

    NARCIS (Netherlands)

    Haegeman, Bart; Etienne, Rampal S.

    Hubbell's neutral theory claims that ecological patterns such as species abundance distributions can be explained by a stochastic model based on simple assumptions. One of these assumptions, the point mutation assumption, states that every individual has the same probability to speciate. Etienne et

  18. 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

  19. 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)

  20. ENDF/B-5 Actinides (Rev. 86)

    International Nuclear Information System (INIS)

    Lemmel, H.D.

    1986-05-01

    This document summarizes the contents of the Actinides part of the ENDF/B-5 nuclear data library released by the US National Nuclear Data Center. This library or selective retrievals of it, are available costfree from the IAEA Nuclear Data Section upon request. The present version of the library is the Revision of 1986. (author). Refs, figs and tabs

  1. 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

  2. Report of the panel on inhaled actinides

    International Nuclear Information System (INIS)

    Anon.

    1978-01-01

    Some topics discussed are as follows: assessment of risks to man of inhaling actinides; use of estimates for developing protection standards; epidemiology of lung cancer in exposed human populations; development of respiratory tract models; and effects in animals: dose- and effect-modifying factors

  3. Actinide and fission product partitioning and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1995-07-01

    The third international information exchange meeting on actinide and fission product partitioning and transmutation, took place in Cadarache France, on 12-14 December 1994. The proceedings are presented in six sessions : an introduction session, the major programmes and international cooperation, the systems studies, the reactors fuels and targets, the chemistry and a last discussions session. (A.L.B.)

  4. Placental transfer of plutonium and other actinides

    International Nuclear Information System (INIS)

    Griessl, I.; Stieve, F.E.

    1988-10-01

    The report is based on an extensive literature search. All data available from studies on placental transfer of plutonium and other actinides in man and animals have been collected and analysed, and the report presents the significant results as well as unresolved questions and knowledge gaps which may serve as a waypost to future research work. (orig./MG) [de

  5. Partitioning and Transmutation of minor actinides

    International Nuclear Information System (INIS)

    Koch, L.; Wellum, R.

    1991-01-01

    The partitioning of minor actinides from spent fuels and their transmutation into short-lived fission products has been the topic of two dedicated meetings organized jointly by the European Commission and the OECD. The conclusion of the last meeting in 1980, in short, was that partitioning and transmutation of minor actinides, especially in fast reactors, seemed possible. However, the incentive, which would be a reduction of the radiological hazard to the public, was too small if long-lived fission products were not included. Furthermore this meeting showed that minor actinide targets or possible nuclear fuels containing minor actinides for transmutation had not yet been developed. The European Institute for Transuranium Elements took up this task and has carried it out as a small activity for several years. Interests expressed recently by an expert meeting of the OECD/NEA (Paris, 25 April 1989), which was initiated by the proposed Japanese project Omega, led us to the conclusion that the present state of knowledge should be looked at in a workshop environment. Since the Japanese proposal within the project Omega is based on a broader approach we needed this evaluation to assess the relevance of our present activity and wanted to identifiy additional studies which might be needed to cover possible future demands from the public. This workshop was therefore organized, and participants active in the field from EC countries, the USA and Japan were invited

  6. Supercritical fluid carbon dioxide extraction of actinides

    International Nuclear Information System (INIS)

    Rao, Ankita; Tomar, B.S.

    2016-01-01

    Supercritical fluid extraction (SFE) is a process akin to liquid-liquid or solvent extraction where a Supercritical fluid (SCF) is contacted with a solid/ liquid matrix for the purpose of separating the component of interest from the original matrix. Carbon dioxide is a preferred choice as supercritical fluid (SCF) owing to its moderate critical parameter (P c = 7.38 MPa and T c = 304.1K) coupled with radiation and chemical stability, non toxic nature and low cost. Despite widespread applications for extraction of organic compounds and associated advantages especially liquid waste minimization, the SFE of metal ions was left unexplored for quite some time, as direct metal ion extraction is inefficient due charge neutralization requirement and weak solute-solvent interaction. Neutral SCF soluble metal-ligand complexation is imperative and SFE of actinides was reported only in 1994. Several studies have been carried out on SFE of uranium, thorium and plutonium from nitric acid medium employing different sets of ligands (organophosphorus, diketones, amides). Especially attractive is the possibility of direct dissolution and extraction of actinides employing ligand-acid adducts (like TBP.HNO 3 adduct) from solid matrices of different stages of nuclear fuel cycle viz. ores, spent nuclear fuels and radioactive wastes. Also, partitioning of actinides from fission products has been explored in spent nuclear fuel. These studies on supercritical fluid extraction of actinides indicate a more efficient and environmentally sustainable technology. (author)

  7. ACTINET: a European Network for Actinide Sciences

    International Nuclear Information System (INIS)

    Bernard Boullis; Pascal Chaix

    2006-01-01

    Full text of publication follows: The research in Actinide sciences appear as a strategic issue for the future of nuclear systems. Sustainability issues are clearly in connection with the way actinide elements are managed (either addressing saving natural resource, or decreasing the radiotoxicity of the waste). The recent developments in the field of minor actinide P and T offer convincing indications of what could be possible options, possible future processes for the selective recovery of minor actinides. But they point out, too, some lacks in the basic understanding of key-issues (such as for instance the control An versus Ln selectivity, or solvation phenomena in organic phases). Such lacks could be real obstacles for an optimization of future processes, with new fuel compounds and facing new recycling strategies. This is why a large and sustainable work appears necessary, here in the field of basic actinide separative chemistry. And similar examples could be taken from other aspects of An science, for various applications (nuclear fuel or transmutation targets design, or migration issues,): future developments need a strong, enlarged, scientific basis. The Network ACTINET, established with the support of the European Commission, has the following objectives: - significantly improve the accessibility of the major actinide facilities to the European scientific community, and form a set of pooled facilities, as the corner-stone of a progressive integration process, - improve mobility between the member organisations, in particular between Academic Institutions and National Laboratories holding the pooled facilities, - merge part of the research programs conducted by the member institutions, and optimise the research programs and infrastructure policy via joint management procedures, - strengthen European excellence through a selection process of joint proposals, and reduce the fragmentation of the community by putting critical mass of resources and expertise on

  8. European Europart integrated project on actinide partitioning

    International Nuclear Information System (INIS)

    Madic, C.; Hudson, M.J.

    2005-01-01

    This poster presents the objectives of EUROPART, a scientific integrated project between 24 European partners, mostly funded by the European Community within the FP6. EUROPART aims at developing chemical partitioning processes for the so-called minor actinides (MA) contained in nuclear wastes, i.e. from Am to Cf. In the case of dedicated spent fuels or targets, the actinides to be separated also include U, Pu and Np. The techniques considered for the separation of these radionuclides belong to the fields of hydrometallurgy and pyrometallurgy, as in the previous FP5 programs named PARTNEW and PYROREP. The two main axes of research within EUROPART will be: The partitioning of MA (from Am to Cf) from high burn-up UO x fuels and multi-recycled MOx fuels; the partitioning of the whole actinide family for recycling, as an option for advanced dedicated fuel cycles (and in connection with the studies to be performed in the EUROTRANS integrated project). In hydrometallurgy, the research is organised into five Work Packages (WP). Four WP are dedicated to the study of partitioning methods mainly based on the use of solvent extraction methods, one WP is dedicated to the development of actinide co-conversion methods for fuel or target preparation. The research in pyrometallurgy is organized into four WP, listed hereafter: development of actinide partitioning methods, study of the basic chemistry of trans-curium elements in molten salts, study of the conditioning of the wastes, some system studies. Moreover, a strong management team will be concerned not only with the technical and financial issues arising from EUROPART, but also with information, communication and benefits for Europe. Training and education of young researchers will also pertain to the project. EUROPART has also established collaboration with US DOE and Japanese CRIEPI. (authors)

  9. A new look at actinide recycle

    International Nuclear Information System (INIS)

    Burch, W.D.; Croff, A.G.; Rawlins, J.A.; Schulz, W.W.

    1991-01-01

    This paper will address the justification for reexamination of the value of recovering the minor actinides and certain fission products from spent light-water reactor fuels and describe some of the technical progress that has been made since the major studies of a decade ago. During this time, the US Environmental Protection Agency (EPA) and the Nuclear Regulatory Commission have begun establishing detailed criteria and regulations for geologic repositories. An examination of the hazards of waste disposal relative to the EPA release standards reveals that removal of 99.9% of the actinides (Pu, Am, and Np) reduces these hazards quite close to the EPA standards after 300 years' decay of the strontium and cesium. It may be also useful to remove and separately manage and dispose of certain of the long-lived fission products, such as 99 Tc and 129 I. Much additional work is required to fully assess the appropriate target recoveries as the hazards and risks are more closely examined and as the standards are reworked and refined. The two decades before the projected start of the US repository may present a window of opportunity to introduce several better management practices that act to simplify the repository safety issues. From a technical standpoint, significant progress has been made on recovery of the actinides from aqueous wastes though use of the TRUEX process. Additional work is required to demonstrate the application of the process to spent LWR fuels, but it appears straightforward. In addition, work at the Argonne National Laboratory on the liquid-metal reactor metal fuel cycle shows the relative simplicity of recycle of the actinides in that fast reactor cycle. Much work remains to fully demonstrate that actinides from all secondary waste streams can be removed to the target levels from both the aqueous reprocessing of LWR fuel and the pyro processes for the metal-fueled fast reactor. 9 refs., 2 figs

  10. Synroc tailored waste forms for actinide immobilization

    Energy Technology Data Exchange (ETDEWEB)

    Gregg, Daniel J.; Vance, Eric R. [Australian Nuclear Science and Technology Organisation, Kirrawee (Australia). ANSTOsynroc, Inst. of Materials Engineering

    2017-07-01

    Since the end of the 1970s, Synroc at the Australian Nuclear Science and Technology Organisation (ANSTO) has evolved from a focus on titanate ceramics directed at PUREX waste to a platform waste treatment technology to fabricate tailored glass-ceramic and ceramic waste forms for different types of actinide, high- and intermediate level wastes. The particular emphasis for Synroc is on wastes which are problematic for glass matrices or existing vitrification process technologies. In particular, nuclear wastes containing actinides, notably plutonium, pose a unique set of requirements for a waste form, which Synroc ceramic and glass-ceramic waste forms can be tailored to meet. Key aspects to waste form design include maximising the waste loading, producing a chemically durable product, maintaining flexibility to accommodate waste variations, a proliferation resistance to prevent theft and diversion, and appropriate process technology to produce waste forms that meet requirements for actinide waste streams. Synroc waste forms incorporate the actinides within mineral phases, producing products which are much more durable in water than baseline borosilicate glasses. Further, Synroc waste forms can incorporate neutron absorbers and {sup 238}U which provide criticality control both during processing and whilst within the repository. Synroc waste forms offer proliferation resistance advantages over baseline borosilicate glasses as it is much more difficult to retrieve the actinide and they can reduce the radiation dose to workers compared to borosilicate glasses. Major research and development into Synroc at ANSTO over the past 40 years has included the development of waste forms for excess weapons plutonium immobilization in collaboration with the US and for impure plutonium residues in collaboration with the UK, as examples. With a waste loading of 40-50 wt.%, Synroc would also be considered a strong candidate as an engineered waste form for used nuclear fuel and highly

  11. Complexation studies of actinides (U, Pu, Am) with linear polyamino-carboxylate ligands and sidero-chelates

    International Nuclear Information System (INIS)

    Nguyen, L.V.

    2010-01-01

    As part of our research endeavour aimed at developing and improving decontamination processes of wastewater containing alpha emitters, physico-chemical complexation studies of actinides (U, Pu, Am) with organic open-chain ligands such as poly-aminocarboxylic acids (H 4 EDTA) and sidero-chelates (di-hydroxamic acids and desferrioxamine B) have been carried out. Gaining a clear understanding of the coordination properties of the targeted actinides is an essential step towards the selection of the most appropriate chelating agents that will exhibit high uptake efficiencies. EXAFS (Extended X-ray Absorption Fine Structure) measurements at the ESRF synchrotron enabled to elucidate the coordination scheme of uranium and plutonium complexes. Solution thermodynamic investigations were intended to provide valuable information about the nature and the stability of the uranium(VI) and americium(III) complexes prevailing at a given pH in solution. The set of stability constants determined from potentiometric and UV-visible spectrophotometric titrations, allowed to predict the speciation of the selected actinides in presence of the aforementioned ligands and to determine the pH range required for achieving 'ultimate' decontamination. (author) [fr

  12. Adventures in Actinide Chemistry: A Year of Exploring Uranium and Thorium in Los Alamos

    Energy Technology Data Exchange (ETDEWEB)

    Pagano, Justin [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2016-01-08

    The first part of this collection of slides is concerned with considerations when working with actinides. The topics discussed in the document as a whole are the following: Actinide chemistry vs. transition metal chemistry--tools we can use; New synthetic methods to obtain actinide hydrides; Actinide metallacycles: synthesis, structure, and properties; and Reactivity of actinide metallacycles.

  13. Modelling interaction of deep groundwaters with bentonite and radionuclide speciation

    International Nuclear Information System (INIS)

    Wanner, H.

    1986-04-01

    In the safety analysis recently reported for a potential Swiss high-level waste repository, radionuclide speciation and solubility limits are calculated for expected granitic groundwater conditions. With the objective of deriving a more realistic description of radionuclide release from the near-field, an investigation has been initiated to quantitatively specify the chemistry of the near-field. In the Swiss case, the main components of the near-field are the glass waste-matrix, a thick steel canister horizontally emplaced in a drift, and a backfill of highly compacted sodium bentonite. This report describes a thermodynamic model which is used to estimate the chemical composition of the pore water in compacted sodium bentonite. Solubility limits and speciation of important actinides and the fission product technetium in the bentonite pore water are then calculated. The model is based on available experimental data on the interaction of sodium bentonite and groundwater and represents means of extrapolation from laboratory data to repository conditions. The basic reactions between sodium bentonite and groundwater are described by an ion-exchange model for sodium, potassium, magnesium, and calcium. The model assumes equilibrium with calcite as long as sufficient carbonates remain in the bentonite, as well as quartz saturation. It is calculated that the pore water of compacted sodium bentonite saturated with Swiss Reference Groundwater will have a pH value of 9.7 and a free carbonate activity of 8x10 -4 M. The long-term situation is modelled by the assumption that the near-field of a deep repository behaves like a mixing tank. In this way, an attempt is made to account for the continuous water exchange between the near-field and the host rock. It is found that sodium bentonite will be slowly converted to calcium bentonite. This conversion is roughly estimated to be completed after 2 million years

  14. Electrorecovery of actinides at room temperature

    Energy Technology Data Exchange (ETDEWEB)

    Stoll, Michael E [Los Alamos National Laboratory; Oldham, Warren J [Los Alamos National Laboratory; Costa, David A [Los Alamos National Laboratory

    2008-01-01

    There are a large number of purification and processing operations involving actinide species that rely on high-temperature molten salts as the solvent medium. One such application is the electrorefining of impure actinide metals to provide high purity material for subsequent applications. There are some drawbacks to the electrodeposition of actinides in molten salts including relatively low yields, lack of accurate potential control, maintaining efficiency in a highly corrosive environment, and failed runs. With these issues in mind we have been investigating the electrodeposition of actinide metals, mainly uranium, from room temperature ionic liquids (RTILs) and relatively high-boiling organic solvents. The RTILs we have focused on are comprised of 1,3-dialkylimidazolium or quaternary ammonium cations and mainly the {sup -}N(SO{sub 2}CF{sub 3}){sub 2} anion [bis(trif1uoromethylsulfonyl)imide {equivalent_to} {sup -}NTf{sub 2}]. These materials represent a class of solvents that possess great potential for use in applications employing electrochemical procedures. In order to ascertain the feasibility of using RTILs for bulk electrodeposition of actinide metals our research team has been exploring the electron transfer behavior of simple coordination complexes of uranium dissolved in the RTIL solutions. More recently we have begun some fundamental electrochemical studies on the behavior of uranium and plutonium complexes in the organic solvents N-methylpyrrolidone (NMP) and dimethylsulfoxide (DMSO). Our most recent results concerning electrodeposition will be presented in this account. The electrochemical behavior of U(IV) and U(III) species in RTILs and the relatively low vapor pressure solvents NMP and DMSO is described. These studies have been ongoing in our laboratory to uncover conditions that will lead to the successful bulk electrodeposition of actinide metals at a working electrode surface at room temperature or slightly elevated temperatures. The RTILs we

  15. Chemical speciation of neptunium in spent fuel. Annual report for period 15 August 1999 to 15 August 2000

    Energy Technology Data Exchange (ETDEWEB)

    Ken Czerwinski; Don Reed

    2000-09-01

    (B204) This project will examine the chemical speciation of neptunium in spent nuclear fuel. The R&D fields covered by the project include waste host materials and actinide chemistry. Examination of neptunium is chosen since it was identified as a radionuclide of concern by the NERI workshop. Additionally, information on the chemical form of neptunium in spent fuel is lacking. The identification of the neptunium species in spent fuel would allow a greater scientific based understanding of its long-term fate and behavior in waste forms. Research to establish the application and development of X-ray synchrotrons radiation (XSR) techniques to determine the structure of aqueous, adsorbed, and solid actinide species of importance to nuclear considerations is being conducted at Argonne. These studies extend current efforts within the Chemical Technology Division at Argonne National Laboratory to investigate actinide speciation with more conventional spectroscopic and solids characterization (e.g. SEM, TEM, and XRD) methods. Our project will utilize all these techniques for determining neptunium speciation in spent fuel. We intend to determine the chemical species and oxidation state of neptunium in spent fuel and alteration phases. Different types of spent fuel will be examined. Once characterized, the chemical behavior of the identified neptunium species will be evaluated if it is not present in the literature. Special attention will be given to the behavior of the neptunium species under typical repository near-field conditions (elevated temperature, high pH, varying Eh). This will permit a timely inclusion of project results into near-field geochemical models. Additionally, project results and methodologies have applications to neptunium in the environment, or treatment of neptunium containing waste. Another important aspect of this project is the close cooperation between a university and a national laboratory. The PI has a transuranic laboratory at MIT where

  16. Chemical speciation of neptunium in spent fuel. Annual report for period 15 August 1999 to 15 August 2000

    International Nuclear Information System (INIS)

    Ken Czerwinski; Don Reed

    2000-01-01

    (B204) This project will examine the chemical speciation of neptunium in spent nuclear fuel. The R and D fields covered by the project include waste host materials and actinide chemistry. Examination of neptunium is chosen since it was identified as a radionuclide of concern by the NERI workshop. Additionally, information on the chemical form of neptunium in spent fuel is lacking. The identification of the neptunium species in spent fuel would allow a greater scientific based understanding of its long-term fate and behavior in waste forms. Research to establish the application and development of X-ray synchrotrons radiation (XSR) techniques to determine the structure of aqueous, adsorbed, and solid actinide species of importance to nuclear considerations is being conducted at Argonne. These studies extend current efforts within the Chemical Technology Division at Argonne National Laboratory to investigate actinide speciation with more conventional spectroscopic and solids characterization (e.g. SEM, TEM, and XRD) methods. Our project will utilize all these techniques for determining neptunium speciation in spent fuel. We intend to determine the chemical species and oxidation state of neptunium in spent fuel and alteration phases. Different types of spent fuel will be examined. Once characterized, the chemical behavior of the identified neptunium species will be evaluated if it is not present in the literature. Special attention will be given to the behavior of the neptunium species under typical repository near-field conditions (elevated temperature, high pH, varying Eh). This will permit a timely inclusion of project results into near-field geochemical models. Additionally, project results and methodologies have applications to neptunium in the environment, or treatment of neptunium containing waste. Another important aspect of this project is the close cooperation between a university and a national laboratory. The PI has a transuranic laboratory at MIT where

  17. Aspects of speciation in foodstuffs

    International Nuclear Information System (INIS)

    Crews, Helen M.

    2001-01-01

    Food is the primary source of trace elements for humans and it is now generally accepted that the bioavailability of a given element and its behaviour in the body depends upon its chemical form. This point was illustrated with the example of arsenic speciation in fish in which bioaccumulation takes place in the marine food chain, however, the species of arsenic ingested by man when the fish is consumed are not toxic. It was pointed out that species information will be vital in deciding upon realistic average dietary requirements for trace elements, particularly because both deficiency or excess of an element can have detrimental consequences on an individual's health. Two examples of speciation studies with food (Cd and Se) were presented and the importance of the use of label technology which will allow studies of target analytes at physiological levels, was stressed

  18. Actinides analysis in emergency situation by on-line coupling between a calix[6]arene-based chromatography column and an Inductively Coupled Plasma-Mass Spectrometer

    International Nuclear Information System (INIS)

    Baghdadi, Sarah

    2015-01-01

    In the event of a nuclear crisis, involving actinides (U, Pu, Am) it is important to have fast analysis methods available in order to identify people that could be contaminated. Usually, they are performed in urine or faeces. Even though, analytical methods used with alpha detection are reliable they are lengthy and tedious to set up. This work consisted in developing an on-line coupling method between a calix[6]arene-based chromatography column and an inductively coupled plasma mass spectrometer (ICP-MS). To do so, a speciation study of actinides in mineralised urine was developed to understand the chemical equilibria happening during the actinides extraction. A protocol was elaborated to extract simultaneously all three actinides at pH = 5, then co-elute them with 0.25 mol.L -1 H 3 PO 4 . Recovery was 56 %, 74 % and 85 % for U, Pu and Am respectively. The column was then coupled to the ICP-MS. A parameter study helped defining mineralisation duration, extraction and elution flow-rates. It was then possible to propose an on-line coupling system allowing reaching detection limits lower than 0.5 mBq.L-1 for 238 U and 243 Am and lower than 5 mBq.L -1 for 239 Pu and 241 Am, for analysis duration lower than 6 hours. These analytical performances show the interest of this technique for a use in a nuclear crisis situation. (author)

  19. 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.

  20. 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.

  1. 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

  2. MODELING MONOMETHYLMERCURY AND TRIBUTYLTIN SPECIATION WITH EPA'S GEOCHEMICAL SPECIATION MODEL MINTEQA2

    Science.gov (United States)

    Given the complexity of the various, simultaneous (and competing) equilibrium reactions governing the speciation of ionic species in aquatic systems, EPA has developed and distributed the geochemical speciation model MINTEQA2 (Brown and Allison, 1987, Allison et al., 1991; Hydrog...

  3. On the solvation of actinide ions

    International Nuclear Information System (INIS)

    Hagberg, D.

    2007-01-01

    Complete text of publication follows: Simulation of the universal ions in water solution is a standardized tool commonly used today. The route to simulation of actinide ions is normally tough because the evaluation of the simulation parameters are normally not given empirically and standard Hartree-Fock calculations are not accurate enough. We use multiconfigurational quantum chemical calculations when deriving the parameters for actinide ion-water potential [1]. The parameters are then simulated using classical molecular dynamics. A case study of the Cm 3+ ion will be presented on the poster. Results from the simulations will be also be discussed, e.g. the radial distribution functions and the coordination number. [1] D. Hagberg, G. Karlstrom, B.O. Roos and L. Gagliardi The coordination of uranyl in water: a combined quantum chemical and molecular simulation study J. Am. Chem. Soc. 127, 14250-14256 (2005)

  4. 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

  5. Actinide and fission product separation and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1991-07-01

    The first international information exchange meeting on actinide and fission product separation and transmutation, took place in Mito in Japan, on 6-8 November 1990. It starts with a number of general overview papers to give us some broad perspectives. Following that it takes a look at some basic facts about physics and about the quantities of materials it is talking about. Then it proceeds to some specific aspects of partitioning, starting with evolution from today commercially applied processes and going on to other possibilities. At the end of the third session it takes a look at the significance of partitioning and transmutation of actinides before it embarks on two sessions on transmutation, first in reactors and second in accelerators. The last session is designed to throw back into the discussion the main points which need to be looked at when considering future work in this area. (A.L.B.)

  6. Chemistry of the actinide elements. Second edition

    International Nuclear Information System (INIS)

    Katz, J.J.; Seaborg, G.T.; Morss, L.R.

    1987-01-01

    This is an exhaustive, updated discourse on the chemistry of Actinides, Volume 1 contains a systematic coverage of the elements Ac, Th, Pa, U, Np, and Pu, which constitutes Part 1 of the work. The characterization of each element is discussed in terms of its nuclear properties, occurrence, preparation, atomic and metallic properties, chemistry of specific compounds, and solution chemistry. The first part of Volume 2 follows the same format as Volume 1 but is confined to the elements Am, Cm, Bk, Cf, and Es, plus a more condensed coverage of the Transeinsteinium elements (Fm, Md, No, Lw, and 104-109). Part 2 of this volume is devoted to a discussion of the actinide elements in general, with a specific focus on electronic spectra, thermodynamic and magnetic properties, the metallic state, structural chemistry, solution kinetics, organometallic chemistry for σ- and π-bonded compounds, and some concluding remarks on the superheavy elements

  7. The thermodynamic functions of gaseous actinide elements

    International Nuclear Information System (INIS)

    Rand, M.H.

    1979-01-01

    The actinide gases have large number of unobserved energy states - up to 3 x 10 6 for Pu(g) - which could contribute to the partition function and its derivatives, from which the thermal functions of these gases are calculated. Existing compilations have simply ignored these levels. By making reasonable assumptions as to the distribution of these energy states, their effect on the functions can be calculated. It is concluded that the existing compilations will be inadequate above approximately 2000K. The effect is particularly marked on the heat capacity. For example, when unobserved levels for Pu(g) are included, the heat capacity of Pu(g) reaches a maximum value of more than 12R at 3200K. Similar considerations will apply to the gaseous actinide ions. (orig.) [de

  8. Actinide and fission product separation and transmutation

    International Nuclear Information System (INIS)

    1991-01-01

    The first international information exchange meeting on actinide and fission product separation and transmutation, took place in Mito in Japan, on 6-8 November 1990. It starts with a number of general overview papers to give us some broad perspectives. Following that it takes a look at some basic facts about physics and about the quantities of materials it is talking about. Then it proceeds to some specific aspects of partitioning, starting with evolution from today commercially applied processes and going on to other possibilities. At the end of the third session it takes a look at the significance of partitioning and transmutation of actinides before it embarks on two sessions on transmutation, first in reactors and second in accelerators. The last session is designed to throw back into the discussion the main points which need to be looked at when considering future work in this area. (A.L.B.)

  9. Seventeen-coordinate actinide helium complexes

    Energy Technology Data Exchange (ETDEWEB)

    Kaltsoyannis, Nikolas [School of Chemistry, The University of Manchester (United Kingdom)

    2017-06-12

    The geometries and electronic structures of molecular ions featuring He atoms complexed to actinide cations are explored computationally using density functional and coupled cluster theories. A new record coordination number is established, as AcHe{sub 17}{sup 3+}, ThHe{sub 17}{sup 4+}, and PaHe{sub 17}{sup 4+} are all found to be true geometric minima, with the He atoms clearly located in the first shell around the actinide. Analysis of AcHe{sub n}{sup 3+} (n=1-17) using the quantum theory of atoms in molecules (QTAIM) confirms these systems as having closed shell, charge-induced dipole bonding. Excellent correlations (R{sup 2}>0.95) are found between QTAIM metrics (bond critical point electron densities and delocalization indices) and the average Ac-He distances, and also with the incremental He binding energies. (copyright 2017 Wiley-VCH Verlag GmbH and Co. KGaA, Weinheim)

  10. Actinide uptake by transferrin and ferritin metalloproteins

    International Nuclear Information System (INIS)

    Den Auwer, C.; Llorens, I.; Moisy, Ph.; Vidaud, C.; Goudard, F.; Barbot, C.; Solari, P.L.; Funke, H.

    2005-01-01

    In order to better understand the mechanisms of actinide uptake by specific biomolecules, it is essential to explore the intramolecular interactions between the cation and the protein binding site. Although this has long been done for widely investigated transition metals, very few studies have been devoted to complexation mechanisms of actinides by active chelation sites of metalloproteins. In this field, X-ray absorption spectroscopy has been extensively used as a structural and electronic metal cation probe. The two examples that are presented here are related to two metalloproteins in charge of iron transport and storage in eukaryote cells: transferrin and ferritin. U(VI)O 2 2+ , Np(IV) and Pu(IV) have been selected because of their possible role as contaminant from the geosphere. (orig.)

  11. Minor actinide transmutation in accelerator driven systems

    Energy Technology Data Exchange (ETDEWEB)

    Friess, Friederike [IANUS, TU Darmstadt (Germany)

    2015-07-01

    Transmutation of radioactive waste, the legacy of nuclear energy use, gains rising interest. This includes the development of facilities able to transmute minor actinides (MA) into stable or short-lived isotopes before final disposal. The most common proposal is to use a double-strata approach with accelerator-driven-systems (ADS) for the efficient transmutation of MA and power reactors to dispose plutonium. An ADS consists of a sub-critical core that reaches criticality with neutrons supplied by a spallation target. An MCNP model of the ADS system Multi Purpose Research Reactor for Hightech Applications will be presented. Depletion calculations have been performed for both standard MOX fuel and transmutation fuel with an increased content of minor actinides. The resulting transmutation rates for MAs are compared to published values. Special attention is given to selected fission products such as Tc-99 and I-129, which impact the radiation from the spent fuel significantly.

  12. 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

  13. 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

  14. 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)

  15. 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

  16. Actinide and fission product partitioning and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1997-07-01

    The fourth international information exchange meeting on actinide and fission product partitioning and transmutation, took place in Mito City in Japan, on 111-13 September 1996. The proceedings are presented in six sessions: the major programmes and international cooperation, the partitioning and transmutation programs, feasibility studies, particular separation processes, the accelerator driven transmutation, and the chemistry of the fuel cycle. (A.L.B.)

  17. Actinide burning in the integral fast reactor

    International Nuclear Information System (INIS)

    Chang, Y.I.

    1993-01-01

    During the past few years, Argonne National Laboratory has been developing the integral fast reactor (IFR), an advanced liquid-metal reactor concept. In the IFR, the inherent properties of liquid-metal cooling are combined with a new metallic fuel and a radically different refining process to allow breakthroughs in passive safety, fuel cycle economics, and waste management. A key feature of the IFR concept is its unique pyroprocessing. Pyroprocessing has the potential to radically improve long-term waste management strategies by exploiting the following attributes: 1. Minor actinides accompany plutonium product stream; therefore, actinide recycling occurs naturally. Actinides, the primary source of long-term radiological toxicity, are removed from the waste stream and returned to the reactor for in situ burning, generating useful energy. 2. High-level waste volume from pyroprocessing call be reduced substantially as compared with direct disposal of spent fuel. 3. Decay heat loading in the repository can be reduced by a large factor, especially for the long-term burden. 4. Low-level waste generation is minimal. 5. Troublesome fission products, such as 99 Tc, 129 I, and 14 C, are contained and immobilized. Singly or in combination, the foregoing attributes provide important improvements in long-term waste management in terms of the ease in meeting technical performance requirements (perhaps even the feasibility of demonstrating that technical performance requirements can be met) and perhaps also in ultimate public acceptance. Actinide recycling, if successfully developed, could well help the current repository program by providing an opportunity to enhance capacity utilization and by deferring the need for future repositories. It also represents a viable technical backup option in the event unforeseen difficulties arise in the repository licensing process

  18. BWR Assembly Optimization for Minor Actinide Recycling

    International Nuclear Information System (INIS)

    Maldonado, G. Ivan; Christenson, John M.; Renier, J.P.; Marcille, T.F.; Casal, J.

    2010-01-01

    The Primary objective of the proposed project is to apply and extend the latest advancements in LWR fuel management optimization to the design of advanced boiling water reactor (BWR) fuel assemblies specifically for the recycling of minor actinides (MAs). A top-level objective of the Advanced Fuel Cycle Systems Analysis program element of the DOE NERI program is to investigate spent fuel treatment and recycling options for current light water reactors (LWRs). Accordingly, this project targets to expand the traditional scope of nuclear fuel management optimization into the following two complementary specific objectives: (1) To develop a direct coupling between the pin-by-pin within-bundle loading control variables and core-wide (bundle-by-bundle) optimization objectives, (2) to extend the methodology developed to explicitly encompass control variables, objectives, and constraints designed to maximize minor actinide incineration in BWR bundles and cycles. The first specific objective is projected to 'uncover' dormant thermal margin made available by employing additional degrees of freedom within the optimization process, while the addition of minor actinides is expected to 'consume' some of the uncovered thermal margin. Therefore, a key underlying goal of this project is to effectively invest some of the uncovered thermal margin into achieving the primary objective.

  19. Measurement of actinide neutron cross sections

    International Nuclear Information System (INIS)

    Firestone, Richard B.; Nitsche, Heino; Leung, Ka-Ngo; Perry, DaleL.; English, Gerald

    2003-01-01

    The maintenance of strong scientific expertise is critical to the U.S. nuclear attribution community. It is particularly important to train students in actinide chemistry and physics. Neutron cross-section data are vital components to strategies for detecting explosives and fissile materials, and these measurements require expertise in chemical separations, actinide target preparation, nuclear spectroscopy, and analytical chemistry. At the University of California, Berkeley and the Lawrence Berkeley National Laboratory we have trained students in actinide chemistry for many years. LBNL is a leader in nuclear data and has published the Table of Isotopes for over 60 years. Recently, LBNL led an international collaboration to measure thermal neutron capture radiative cross sections and prepared the Evaluated Gamma-ray Activation File (EGAF) in collaboration with the IAEA. This file of 35, 000 prompt and delayed gamma ray cross-sections for all elements from Z=1-92 is essential for the neutron interrogation of nuclear materials. LBNL has also developed new, high flux neutron generators and recently opened a 1010 n/s D+D neutron generator experimental facility

  20. Value of burnup credit beyond actinides

    International Nuclear Information System (INIS)

    Lancaster, D.; Fuentes, E.; Kang, Chi.

    1997-01-01

    DOE has submitted a topical report to the NRC justifying burnup credit based only on actinide isotopes (U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, and Am-241). When this topical report is approved, it will allow a great deal of the commercial spent nuclear fuel to be transported in significantly higher capacity casks. A cost savings estimate for shipping fuel in 32 assembly (burnup credit) casks as opposed to 24 assembly (non-burnup credit) casks was previously presented. Since that time, more detailed calculations have been performed using the methodology presented in the Actinide-Only Burnup Credit Topical Report. Loading curves for derated casks have been generated using actinide-only burnup credit and are presented in this paper. The estimates of cost savings due to burnup credit for shipping fuel utilizing 32, 30, 28, and 24 assembly casks where only the 24 assembly cask does not burnup credit have been created and are discussed. 4 refs., 2 figs

  1. 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)

  2. 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

  3. 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

  4. Preparation, properties, and some recent studies of the actinide metals

    International Nuclear Information System (INIS)

    Haire, R.G.

    1985-01-01

    The actinide elements form a unique series of metals. The variation in their physial properties combined with the varying availability of the different elements offers a challenge to the preparative scientist. This article provides a brief review of selected methods used for preparing μg to kg amounts of the actinide metals and the properties of these metals. In addition, some recent studies on selected actinide metals are discussed. 62 refs

  5. Hydrothermal decomposition of actinide(IV oxalates: a new aqueous route towards reactive actinide oxide nanocrystals

    Directory of Open Access Journals (Sweden)

    Walter Olaf

    2016-01-01

    Full Text Available The hydrothermal decomposition of actinide(IV oxalates (An= Th, U, Pu at temperatures between 95 and 250 °C is shown to lead to the production of highly crystalline, reactive actinide oxide nanocrystals (NCs. This aqueous process proved to be quantitative, reproducible and fast (depending on temperature. The NCs obtained were characterised by X-ray diffraction and TEM showing their size to be smaller than 15 nm. Attempts to extend this general approach towards transition metal or lanthanide oxalates failed in the 95–250 °C temperature range. The hydrothermal decomposition of actinide oxalates is therefore a clean, flexible and powerful approach towards NCs of AnO2 with possible scale-up potential.

  6. 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

  7. 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.)

  8. Transport methods as complementary tools for speciation purposes

    International Nuclear Information System (INIS)

    Fourest, B.; Sladkov, V.

    2005-01-01

    Transport methods, and especially capillary electrophoresis, are shown to bring with a high simplicity and efficiently useful complementary data to solve some speciation problems. Their application in this aim is particularly interesting in the case of actinides or solutions resulting from the radioactive waste management. In the present article, three examples are proposed to illustrate this point. In the first one, the open-end capillary method is applied to point out the hydrolyzed species of Pa(V) over a wide pH range. The difficulties overcome in this case are related to the very low concentration and specific properties of the element under consideration. The second illustration concerns the complexation of uranyl by the anionic forms of some long-lived fission products (MO x n- , with M=I and Se). For the study of these systems, capillary electrophoresis appears to be a method particularly simple and efficient. The last example deals with the quantification of selenate and selenite ions in the presence of nitrate. Capillary electrophoresis is found to be especially appropriate to the simultaneous determination of these two anionic species in such media. (orig.)

  9. 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

  10. Impact of Eu(III) on mammalian cells as a function of its speciation

    Energy Technology Data Exchange (ETDEWEB)

    Sachs, Susanne; Heller, Anne; Geipel, Gerhard; Bernhard, Gert [Helmholtz-Zentrum Dresden-Rossendorf, Institute of Resource Ecology, Bautzner Landstr. 400, 01328 Dresden (Germany)

    2014-07-01

    In the case of the accidental release of long-lived radionuclides, e.g., actinides, into the environment, knowledge of their behavior in bio-systems is necessary to asses and to prevent radiological and chemical induced adverse health effects. This includes knowledge of the bioavailability and chemo-/radio-toxicity of these elements for/onto cells, which are governed to a large extent by their speciation [1,2]. In order to gain a better process understanding, we study the interaction of trivalent actinides/lanthanides with mammalian cells on a cellular level combining biochemical and analytical methods. Results of these studies can contribute to the estimation of low dose effects and the development of new decontamination strategies. The cellular tolerance of FaDu cells (human squamous cell carcinoma cell line) toward Eu(III) as an analog for trivalent actinides as well as its uptake into the cells has been studied as a function of the Eu(III) concentration and nutrient composition. To differentiate between chemo-toxic and radio-toxic effects of Eu(III), {sup 152}Eu (β{sup -}, ε) was applied as radioactive tracer besides europium with natural isotope composition. The Eu(III) speciation in the cell culture media has been investigated by time-resolved laser-induced fluorescence spectroscopy as well as by solubility studies in combination with ultrafiltration, ultracentrifugation, cation and anion analysis. These results are used to correlate cytotoxicity and uptake of Eu(III) on/into the cells with its chemical speciation in the nutrient. Presently, we are studying the interaction of Eu(III) with NRK-52E cells (rat kidney epithelial-like cells). The results of these studies will be discussed and compared to those obtained with FaDu cells. From the studies with FaDu cells it was concluded that the Eu(III) cytotoxicity onto these cells depends on the Eu(III) concentration and is influenced by its chemical speciation. This was also reported, for instance, for the

  11. 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

  12. Uranium speciation in Fernald soils

    International Nuclear Information System (INIS)

    Morris, D.E.; Conradson, S.D.; Tait, C.D.; Chisholm-Brause, C.J.; Berg, J.; Musgrave, J.

    1992-01-01

    This report details progress made from January 1 to May 31, 1992 in this analytical support task to determine the speciation of uranium in contaminated soil samples from the Fernald Environmental Management Project site under the auspices of the Uranium in Soils Integrated Demonstration funded through the US DOE's Office of Technology Development. The authors' efforts have focused on characterization of soil samples collected by S.Y. Lee (Oak Ridge National Laboratory) from five locales at the Fernald site. These were chosen to sample a broad range of uranium source terms. On the basis of x-ray absorption spectroscopy data, they have determined that the majority of uranium (> 80--90%) exists in the hexavalent oxidation state for all samples examined. This is a beneficial finding from the perspective of remediation, because U(VI) species are more soluble in general than uranium species in other oxidation states. Optical luminescence data from many of the samples show the characteristic structured yellow-green emission from the uranyl (UO 2 2+ ) moiety. The luminescence data also suggest that much of the uranium in these soils is present as well-crystallized UO 2 2+ species. Some clear spectroscopic distinctions have been noted for several samples that illustrate significant differences in the speciation (1) from site to site, (2) within different horizons at the same site, and (3) within different size fractions of the soils in the same horizon at the same site. This marked heterogeneity in uranyl speciation suggests that several soil washing strategies may be necessary to reduce the total uranium concentrations within these soils to regulatory limits

  13. Speciation of Pb in industrially polluted soils

    DEFF Research Database (Denmark)

    Jensen, Pernille Erland; Ottosen, Lisbeth M.; Pedersen, Anne Juul

    2006-01-01

    This study was aimed at elucidating the importance of original Pb-speciation versus soil-characteristics to mobility and distribution of Pb in industrially polluted soils. Ten industrially polluted Danish surface soils were characterized and Pb speciation was evaluated through SEM-EDX studies...

  14. Non-compound nucleus fission in actinide and pre-actinide regions

    Indian Academy of Sciences (India)

    Data on the evaporation residue cross-sections, in addition to those on mass and angular distributions, are necessary for better understanding of the contribution from non-compound nucleus fission in the pre-actinide region. Measurement of mass-resolved angular distribution of fission products in 20Ne+232Th reaction ...

  15. Synergistic extraction of actinides : Part I. Hexa-and pentavalent actinides

    International Nuclear Information System (INIS)

    Patil, S.K.; Ramakrishna, V.V.

    1980-01-01

    A detailed discussion on the reported literature on the synergistic extraction of hexa- and pentavalent actinide ions, by different combinations of extractants and from different aqueous media, is presented. Structural aspects of the various complexes involved in synergism also are reviewed. A short account of the applications based on synergistic extraction is also given. (author)

  16. Advances in Ecological Speciation: an integrative approach.

    Science.gov (United States)

    Faria, Rui; Renaut, Sebastien; Galindo, Juan; Pinho, Catarina; Melo-Ferreira, José; Melo, Martim; Jones, Felicity; Salzburger, Walter; Schluter, Dolph; Butlin, Roger

    2014-02-01

    The role of natural selection in promoting reproductive isolation has received substantial renewed interest within the last two decades. As a consequence, the study of ecological speciation has become an extremely productive research area in modern evolutionary biology. Recent innovations in sequencing technologies offer an unprecedented opportunity to study the mechanisms involved in ecological speciation. Genome scans provide significant insights but have some important limitations; efforts are needed to integrate them with other approaches to make full use of the sequencing data deluge. An international conference 'Advances in Ecological Speciation' organized by the University of Porto (Portugal) aimed to review current progress in ecological speciation. Using some of the examples presented at the conference, we highlight the benefits of integrating ecological and genomic data and discuss different mechanisms of parallel evolution. Finally, future avenues of research are suggested to advance our knowledge concerning the role of natural selection in the establishment of reproductive isolation during ecological speciation. © 2013 John Wiley & Sons Ltd.

  17. Research needs in metabolism and dosimetry of the actinides

    International Nuclear Information System (INIS)

    Richmond, C.R.

    1978-01-01

    The following topics are discussed: uranium mine and mill tailings; environmental standards; recommendations of NCRP and ICRP; metabolic models and health effects; life-time exposures to actinides and other alpha emitters; high-specific-activity actinide isotopes versus naturally occurring isotopic mixtures of uranium isotopes; adequacy of the n factor; and metabolism and dosimetry;

  18. 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.)

  19. 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

  20. Actinide extractants for the nuclear industry of the future

    International Nuclear Information System (INIS)

    Musikas, C.; Morisseau, J.C.; Hoel, P.; Guillaume, B.

    1987-06-01

    Non organo-phosphorus extractants properties regarding the extractions of actinides in nuclear fuels reprocessing are presented. N,N-dialkylamides are proposed as alternatives to TBP.N,N'-tetraalkylamides or pentaalkyl propane diamides properties are reported. They show that those bidentate extractants are alternatives to bidentate organophosphorus extractants for actinides (III) extraction from concentrated nitric acid. 11 figs, 15 refs

  1. 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

  2. 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)

  3. 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)

  4. Thermodynamic analysis of light-actinide elements

    International Nuclear Information System (INIS)

    Brosh, Eli; Makov, Guy; Shneck, Roni Z.

    2005-01-01

    The thermophysical properties of the alpha phases of the light actinide elements Th, U, Np and Pu were analysed. For each of the analysed elements, the Gibbs free-energy was modelled by an explicit function of temperature T and pressure P over the whole relevant T-P range, in a manner compatible with the CALPHAD (Calculation of Alloy Phase Diagrams) method. Several adjustable model-parameters were fitted to available experimental results. The model is based on a new semi-empirical equation of state, which interpolates with Thomas-Fermi type models for the volume and with the Dulong-Petit value for the heat capacity, at extreme pressures

  5. Determination of actinides using ICP-SFMS

    International Nuclear Information System (INIS)

    Nygren, Ulrika

    2006-01-01

    Interest in the determination of the actinides using ICP-MS has steadily increased with the development of systems capable of more sensitive and precise measurements. However, the analysis of less abundant actinides such as Pu and Am is not straightforward due to the need for chemical separation of these elements prior to determination. In many applications of mass-spectrometric actinide analysis, isotope ratio measurements are important, either for the analysis of the isotopic composition of, e.g., U or Pu in the sample, or for quantitative determinations using isotope dilution mass spectrometry. In order to achieve high precision and accuracy in an isotope ratio measurement, corrections for instrumentally induced systematic errors, e.g., due to dead-time and mass bias, need to be considered. In this thesis, different aspects of actinide analysis using ICP-SFMS have been addressed. In Papers I and III, separation procedures based on solid phase extraction for Pu, Am and U were developed and evaluated with respect to chemical yield and separation from elements causing spectral interferences. Applications of the analytical procedures developed comprised measurement of the 240 Pu/ 2 3 9Pu ratio in environmental reference materials, and age determination of Pu based on the 241 Pu/ 241 Am and 240 Pu/ 236 U ratios. In the application of different separation procedures for Pu, previously unidentified spectral interferences were discovered. In Paper II, these interferences were identified as lanthanide phosphate ions and the composition and formation of these species with respect to different instrumental parameters were further examined. Due to the importance of precise and accurate isotope ratio determination, a thorough investigation of the instrumental dead time of an ICP-SFMS system was performed. The dead time was evaluated via both isotope ratio and electronic measurements of the output from the detector amplifier. It was found that the overall uncertainty in ratio

  6. Photofissility of actinide nuclei at intermediate energies

    International Nuclear Information System (INIS)

    Deppman, A.; Tavares, O.A.P.; Duarte, S.B.; Oliveira, E.C. de; Arruda-Neto, J.D.T.; Pina, S.R. de; Likhachev, V.P.; Mesa, J.; Goncalves, M.

    2001-08-01

    We analyze the recent experimental data on photofissility for 237 Np, 238 U, and 232 Th at incident photon energies above 200 MeV. For this analysis, we developed a Monte carlo algorithm for the nuclear evaporation process in photonuclear reactions. This code is used in association with the multi-collisional model for the photon-induced intranuclear cascade process. Our results show a good quantitative and qualitative agreement with the experimental data. It is shown that the emission of protons and alpha particles at the evaporation stage is an important component for the non-saturation of the actinides photofissility up to, at least, 1GeV. (author)

  7. Thermal decomposition of lanthanide and actinide tetrafluorides

    International Nuclear Information System (INIS)

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

    1988-01-01

    The thermal stabilities of several lanthanide/actinide tetrafluorides have been studied using mass spectrometry to monitor the gaseous decomposition products, and powder X-ray diffraction (XRD) to identify solid products. The tetrafluorides, TbF 4 , CmF 4 , and AmF 4 , have been found to thermally decompose to their respective solid trifluorides with accompanying release of fluorine, while cerium tetrafluoride has been found to be significantly more thermally stable and to congruently sublime as CeF 4 prior to appreciable decomposition. The results of these studies are discussed in relation to other relevant experimental studies and the thermodynamics of the decomposition processes. 9 refs., 3 figs

  8. Electronic structure of the light actinides

    International Nuclear Information System (INIS)

    Dunlap, B.D.

    1976-01-01

    In the last few years, considerable advances have been made in our understanding of the properties of the light actinides. Although these are 5f transition elements formally equivalent to the lanthanide (4f) elements, these materials show a much more varied behavior due to the larger spatial extent and ionizability of the 5f electrons. A review is given of some areas of current interest, especially where hyperfine measurements have played an active role. These include studies of a variety of magnetic phenomena, systematics of isomer shift measurements, and studies of paramagnetic relaxation

  9. Fission cross section measurements for minor actinides

    Energy Technology Data Exchange (ETDEWEB)

    Fursov, B. [IPPE, Obninsk (Russian Federation)

    1997-03-01

    The main task of this work is the measurement of fast neutron induced fission cross section for minor actinides of {sup 238}Pu, {sup 242m}Am, {sup 243,244,245,246,247,248}Cm. The task of the work is to increase the accuracy of data in MeV energy region. Basic experimental method, fissile samples, fission detectors and electronics, track detectors, alpha counting, neutron generation, fission rate measurement, corrections to the data and error analysis are presented in this paper. (author)

  10. Status of nuclear data for actinides

    Energy Technology Data Exchange (ETDEWEB)

    Guzhovskii, B.Y.; Gorelov, V.P.; Grebennikov, A.N. [Russia Federal Nuclear Centre, Arzamas (Russian Federation)] [and others

    1995-10-01

    Nuclear data required for transmutation problem include many actinide nuclei. In present paper the analysis of neutron fission, capture, (n,2n) and (n,3n) reaction cross sections at energy region from thermal point to 14 MeV was carried out for Th, Pa, U, Np, Pu, Am and Cm isotops using modern evaluated nuclear data libraries and handbooks of recommended nuclear data. Comparison of these data indicates on substantial discrepancies in different versions of files, that connect with quality and completeness of original experimental data.

  11. Compilation of actinide neutron nuclear data

    International Nuclear Information System (INIS)

    1979-01-01

    The Swedish nuclear data committee has compiled a selected set of neutron cross section data for the 16 most important actinide isotopes. The aim of the report is to present available data in a comprehensible way to allow a comparison between different evaluated libraries and to judge about the reliability of these libraries from the experimental data. The data are given in graphical form below about 1 ev and above about 10 keV shile the 2200 m/s cross sections and resonance integrals are given in numerical form. (G.B.)

  12. Thermodynamics of carbothermic synthesis of actinide mononitrides

    International Nuclear Information System (INIS)

    Ogawa, T.; Shirasu, Y.; Minato, K.; Serizawa, H.

    1997-01-01

    Carbothermic synthesis will be further applied to the fabrication of nitride fuels containing minor actinides (MA) such as neptunium, americium and curium. A thorough understanding of the carbothermic synthesis of UN will be beneficial in the development of the MA-containing fuels. Thermodynamic analysis was carried out for conditions of practical interest in order to better understand the recent fabrication experiences. Two types of solution phases, oxynitride and carbonitride phases, were taken into account. The Pu-N-O ternary isotherm was assessed for the modelling of M(C, N, O). With the understanding of the UN synthesis, the fabrication problems of Am-containing nitrides are discussed. (orig.)

  13. Calculated Bulk Properties of the Actinide Metals

    DEFF Research Database (Denmark)

    Skriver, Hans Lomholt; Andersen, O. K.; Johansson, B.

    1978-01-01

    Self-consistent relativistic calculations of the electronic properties for seven actinides (Ac-Am) have been performed using the linear muffin-tin orbitals method within the atomic-sphere approximation. Exchange and correlation were included in the local spin-density scheme. The theory explains...... the variation of the atomic volume and the bulk modulus through the 5f series in terms of an increasing 5f binding up to plutonium followed by a sudden localisation (through complete spin polarisation) in americium...

  14. 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

  15. 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

  16. 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

  17. 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.)

  18. Chemical speciation of radionuclides in contaminant plumes at the Chalk River Nuclear Laboratories

    International Nuclear Information System (INIS)

    Champ, D.R.

    1986-01-01

    Experimental disposals of liquid and glassified wastes directly into the sands of the Perch Lake basin, Ontario, Canada, have resulted in the formation of well-defined subsurface contaminant plumes in the groundwater flow system. Using large volume water sampling techniques we have detected low concentrations of several long-lived radionuclides including isotopes of Pu, Am, Cm, Tc, I, Sr and Cs. The particulate and ionic speciation results from these studies support the conclusions of previous laboratory column studies that transport of radionuclides, particularly Cs and Pu, on particulates and/or colloids could be a significant mobilization mechanism in groundwater flow systems. We also propose, based on a comparison of the plume data with previous detailed studies on 60 Co that complexation reactions with natural as well as synthetic organic ligands can yield mobile anionic species of the actinides and lanthanides. Further detailed studies will be required to support this postulate. (author)

  19. Interfacing capillary electrophoresis with inductively coupled plasma mass spectrometry for redox speciation of plutonium

    International Nuclear Information System (INIS)

    Ambard, C.; Delorme, A.; Baglan, N.; Aupiais, J.; Pointurier, F.; Madic, C.

    2005-01-01

    A robust and efficient interface between a capilary electrophoresis (CE) and an ICP-MS for actinide speciation studies was developed. This interface was made of two stainless steel T-shape pieces connected to the ICP-MS through a PFA-50 nebulizer. Fast separations (typically in less than 15 min) were obtained. The performances of the technique in terms of chemical separations carried out by the capillary electrophoresis and in terms of detection limits were investigated. Concerning the detection limit of the CE-ICP-MS system for plutonium, it was determined as 5 x 10 -10 mol L -1 or 9 x 10 -18 mol under our injection conditions. The coupling enables to separate at least three (III, V and VI) of the four plutonium oxidation states which can exist in aqueous solutions and to monitor oxidation and reduction processes. (orig.)

  20. 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

    presence of HA. HA exhibits a significant influence on the transport of U(IV) and U(VI) in a laboratory quartz sand system. In order to provide the basis for a more reliable modeling of the actinide transport, the metal ion complexation with HA has to be integrated into existing geochemical speciation codes. Within this project the metal ion charge neutralization model was embedded into the geochemical modeling code EQ3/6. In addition to that, a digital data base was developed which covers HA complexation data basing on the charge neutralization model. (orig.)

  1. 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 ocidation state IV Th, U, Np

    Energy Technology Data Exchange (ETDEWEB)

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

    2004-03-01

    and the presence of HA. HA exhibits a significant influence on the transport of U(IV) and U(VI) in a laboratory quartz sand system. In order to provide the basis for a more reliable modeling of the actinide transport, the metal ion complexation with HA has to be integrated into existing geochemical speciation codes. Within this project the metal ion charge neutralization model was embedded into the geochemical modeling code EQ3/6. In addition to that, a digital data base was developed which covers HA complexation data basing on the charge neutralization model. (orig.)

  2. Recycle of LWR actinides to an IFR

    International Nuclear Information System (INIS)

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

    1991-01-01

    Large quantities of actinide elements are present in irradiated light water reactor 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 metal-fueled integral fast reactors (IFR), that reactor can consume these elements effectively. The stored fuel may represent valuable resource for the expanding application of fast power reactors. In addition, the removal of TRU elements from spent LWR fuel has the potential for increasing the capacity of high level waste facilities by reducing the heat load and may increase the margin of safety in meeting licensing requirement. Argonne National Laboratory 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. Two pyrochemical processes, that is, salt transport process and blanket processing study, are discussed in this paper. Also the experimental studies are reported. (K.I.)

  3. 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

  4. The dose from actinides in the environment

    International Nuclear Information System (INIS)

    Harley, Naomi H.; Pasternack, Bernard S.

    1978-01-01

    We attempt to evaluate the health effects on local populations from the nuclear power industry. The nuclides which are thought to be most hazardous are the long-lived, alpha-emitting isotopes of plutonium, americium and curium. These long-lived alpha emitters will almost certainly be dispersed in the environment during fuel reprocessing. Their effect is local, not global and at worst a single community could be affected. The most important pathway for exposure to the actinides is through inhalation following resuspension of contaminated soil particles. The most important alpha dose estimates are to cells in bronchial epithelium and cells on bone surfaces. These alpha dose estimates are calculated for a dispersal which contaminates soil with 1 pCi/g of each of the nuclides Pu 238,239 , Am 241 , Cm 242,244 . These bronchial and bone cell dose estimates are compared with those from the naturally occurring actinide 232 Th (and daughters) which are normally found in soil at a level of about 1 pCi/g. (author)

  5. Consistent biokinetic models for the actinide elements

    International Nuclear Information System (INIS)

    Leggett, R.W.

    2001-01-01

    The biokinetic models for Th, Np, Pu, Am and Cm currently recommended by the International Commission on Radiological Protection (ICRP) were developed within a generic framework that depicts gradual burial of skeletal activity in bone volume, depicts recycling of activity released to blood and links excretion to retention and translocation of activity. For other actinide elements such as Ac, Pa, Bk, Cf and Es, the ICRP still uses simplistic retention models that assign all skeletal activity to bone surface and depicts one-directional flow of activity from blood to long-term depositories to excreta. This mixture of updated and older models in ICRP documents has led to inconsistencies in dose estimates and interpretation of bioassay for radionuclides with reasonably similar biokinetics. This paper proposes new biokinetic models for Ac, Pa, Bk, Cf and Es that are consistent with the updated models for Th, Np, Pu, Am and Cm. The proposed models are developed within the ICRP's generic model framework for bone-surface-seeking radionuclides, and an effort has been made to develop parameter values that are consistent with results of comparative biokinetic data on the different actinide elements. (author)

  6. US EPA's SPECIATE 4.4 Database: Development and Uses

    Science.gov (United States)

    SPECIATE is the U.S. Environmental Protection Agency’s (EPA) repository of volatile organic gas and particulate matter (PM) speciation profiles of air pollution sources. EPA released SPECIATE 4.4 in early 2014 and, in total, the SPECIATE 4.4 database includes 5,728 PM, volatile o...

  7. 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

  8. An independent method for data selection of long-life radionuclides (actinides and fission products) in the geosphere

    International Nuclear Information System (INIS)

    Henry, M.; Merceron, T.

    1994-01-01

    An independent method for data selection of long-life radio-nuclides based on the electronegativity equalization principle is proposed to predict the speciation of metal cations as a function of the solution pH. Hydrolysis, condensation and complexation reactions of metal cations in aqueous media are, by this simple model, unified and can be analyzed in terms of electronegativities, oxidation states and coordination numbers with a specific PC software. This paper describes the thermodynamical basis and the underlying concepts of the model in relation to aqueous actinide chemistry of elements such as U and Tc. It is then shown that the model could provide a complementary approach to existing softwares based on thermodynamic data bases allowing to make intelligent and reasonnable choices for the various complexes to consider in complex geochemical codes. (orig.)

  9. Neptunium speciation (complexation and redox behaviour) in aqueous citrate medium

    International Nuclear Information System (INIS)

    Bonin, L.; Ansoborlo, E.; Moisy, Ph.

    2005-01-01

    Full text of publication follows: In the framework of the French Environmental Nuclear Toxicology programme, additional experiments related to the decorporation of actinides are planned. The lack of information on the neptunium behaviour within blood and the inefficiency of therapeutic treatments, led us to study the complexation of this element with basic anions. Within this purpose, the in vitro behaviour of Np IV and Np V in simple media simulating biological media was studied: blood plasma is one of the media of interest and it can be simulated, from a chemical point of view, by an aqueous solution with pH 7.4, containing ions such as citrate (1.6 10 -4 mol/L), lactate (1.5 10 -3 mol/L), CO 3 2- (2.5 10 -2 mol/L), PO 4 3- (1.1 10 -3 mol/L), SO 4 2- (3.3 10 -4 mol/L) and Cl - (9 10 -2 mol/L). This study was more specifically focused on the behaviour of neptunium with citrate ion, which is also a basic ligand to consider when one wishes to study the migration of actinides in the environment, since it exists in significant amounts in the ground due to its production by the plants. In order to determine the speciation of this system, spectrophotometry was more particularly used. Concerning the complexation phenomenon, the existence of several complexes of Np V with various acid-basic forms of the citrate anion was observed; regarding Np IV , two complexes, with 1:1 and 1:2 stoichiometry, have been respectively observed. The reactivity of Np VI is probably similar to the behaviour of U VI , which is reported in literature to form a complex with a 1:1 stoichiometry with the Cit 3- anion From the quantitative study of these equilibria, it has been possible to determine the values of various equilibrium constants. Concerning the stability of neptunium towards oxido-reduction, it was confirmed that Np VI was very quickly reduced to Np V by the citrate anions, whereas Np IV was stable. In the case of Np V , it was observed that, depending on the pH and the citrate

  10. Speciation Analysis of Radionuclides in the Environment - NSK-B SPECIATION project report 2009

    DEFF Research Database (Denmark)

    Hou, Xiaolin; Aldahan, Ala; Possnert, Göran

    . Speciation of radionuclides in soils and sediments includes: Sequential extraction of radionuclides in sediments and of trace elements in soil samples. Sequential extraction of radionuclides in aerosols and particles has also been performed. Further-more, sorption experiments have been performed......, sediments, particles); and (3) Intercomparison excise for speciation analysis of radionu-clides in soil and sediment. This report summarizes the work completed in the project partners’ laboratories, Method developments include: Development of an rapid and in-suit separation method for the speciation...... analysis of 129I in seawater samples; Development of a simple method for the speciation analysis of 129I in fresh water and seawater samples; Development of an on-line HPLC-ICP-MS method for the direct speciation analysis of 127I in water and leachate samples; Speciation of radionuclides in water includes...

  11. 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

  12. 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)

  13. Speciation analysis of radionuclides in the environment - NSK-B SPECIATION project report 2009

    International Nuclear Information System (INIS)

    Hou, X.; Aldahan, A.; Possnert, G.; Lujaniene, G.; Lehto, J.; Skipperud, L.; Lind, O.C.; Salbu, B.

    2009-10-01

    The second stage of the NKS-B project SPECIATION was complemented in 2008-2009, which mainly focus on three aspects: (1) Further improvement and development of methods for speciation analysis of radionuclides; (2) Investigation of speciation of some radionuclides in the environment (water, sediments, particles); and (3) Intercomparison excise for speciation analysis of radionuclides in soil and sediment. This report summarizes the work completed in the project partners' laboratories. Method developments include: Development of an rapid and in-suit separation method for the speciation analysis of 129I in seawater samples; Development of a simple method for the speciation analysis of 129I in fresh water and seawater samples; Development of an on-line HPLC-ICP-MS method for the direct speciation analysis of 127I in water and leachate samples; Speciation of radionuclides in water includes: Speciation of 129I and 127I in time-series precipitation samples collected in Denmark 2001-2006 and its application for the investigation of geochemistry and atmospheric chemistry of iodine, Speciation of radionuclides in Ob and Yenisey Rivers, and Speciation of 129I and 127I in Lake Heimdalen water. Speciation of radionuclides in soils and sediments includes: Sequential extraction of radionuclides in sediments and of trace elements in soil samples. Sequential extraction of radionuclides in aerosols and particles has also been performed. Furthermore, sorption experiments have been performed to investigate the association of Pu, Am and Cs with different geological materials. The intercomparison exercises included sequential extraction of Pu, 137Cs, U, Th, and 129I in one soil and one sediment standard reference materials (NIST-4354, IAEA-375) and Pu in sediment collected from the Lake Heimdalen, Norway. (author)

  14. Speciation analysis of radionuclides in the environment - NSK-B SPECIATION project report 2009

    Energy Technology Data Exchange (ETDEWEB)

    Hou, X. (Technical Univ. of Denmark, Risoe National Lab. for Sustainable Energy, Roskilde (Denmark)); Aldahan, A. (Uppsala Univ., Dept. of Earth Science (Sweden)); Possnert, G. (Uppsala Univ., Tandem Lab. (Sweden)); Lujaniene, G. (Univ. of Helsinki, Lab. of Radiochemistry (Finland)); Lehto, J. (Institute of Physics (Lithuania)); Skipperud, L.; Lind, O.C.; Salbu, B. (Norwegian Univ. of Life Sciences, Isotope Lab., AAs (Norway))

    2009-10-15

    The second stage of the NKS-B project SPECIATION was complemented in 2008-2009, which mainly focus on three aspects: (1) Further improvement and development of methods for speciation analysis of radionuclides; (2) Investigation of speciation of some radionuclides in the environment (water, sediments, particles); and (3) Intercomparison excise for speciation analysis of radionuclides in soil and sediment. This report summarizes the work completed in the project partners' laboratories. Method developments include: Development of an rapid and in-suit separation method for the speciation analysis of 129I in seawater samples; Development of a simple method for the speciation analysis of 129I in fresh water and seawater samples; Development of an on-line HPLC-ICP-MS method for the direct speciation analysis of 127I in water and leachate samples; Speciation of radionuclides in water includes: Speciation of 129I and 127I in time-series precipitation samples collected in Denmark 2001-2006 and its application for the investigation of geochemistry and atmospheric chemistry of iodine, Speciation of radionuclides in Ob and Yenisey Rivers, and Speciation of 129I and 127I in Lake Heimdalen water. Speciation of radionuclides in soils and sediments includes: Sequential extraction of radionuclides in sediments and of trace elements in soil samples. Sequential extraction of radionuclides in aerosols and particles has also been performed. Furthermore, sorption experiments have been performed to investigate the association of Pu, Am and Cs with different geological materials. The intercomparison exercises included sequential extraction of Pu, 137Cs, U, Th, and 129I in one soil and one sediment standard reference materials (NIST-4354, IAEA-375) and Pu in sediment collected from the Lake Heimdalen, Norway. (author)

  15. 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

  16. 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

  17. 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

  18. General survey of applications which require actinide nuclear data

    International Nuclear Information System (INIS)

    Raman, S.

    1976-01-01

    This review paper discusses the actinide waste problem, the buildup of toxic isotopes in the fuel, the neutron activity associated with irradiated fuel, the 252 Cf buildup problem, and the production of radioisotope power sources as broad areas that require actinide cross-section data. Decay data enter into the area of radiological safety and health physics. This paper also discusses a few cross-section measurements in progress at the Oak Ridge Electron Linear Accelerator. The availability of actinide samples through the Transuranium Program at Oak Ridge is discussed in considerable detail. The present data status with respect to the various applications is reviewed along with recommendations for improving the data base

  19. Review of actinide nitride properties with focus on safety aspects

    Energy Technology Data Exchange (ETDEWEB)

    Albiol, Thierry [CEA Cadarache, St Paul Lez Durance Cedex (France); Arai, Yasuo [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    2001-12-01

    This report provides a review of the potential advantages of using actinide nitrides as fuels and/or targets for nuclear waste transmutation. Then a summary of available properties of actinide nitrides is given. Results from irradiation experiments are reviewed and safety relevant aspects of nitride fuels are discussed, including design basis accidents (transients) and severe (core disruptive) accidents. Anyway, as rather few safety studies are currently available and as many basic physical data are still missing for some actinide nitrides, complementary studies are proposed. (author)

  20. Minor Actinide Laboratory at JRC-ITU: Fuel fabrication facility

    International Nuclear Information System (INIS)

    Fernandez, A.; McGinley, J.; Somers, J.

    2008-01-01

    The Minor Actinide Laboratory (MA-lab) of the Institute for Transuranium Elements is a unique facility for the fabrication of fuels and targets containing minor actinides (MA). It is of key importance for research on Partitioning and Transmutation in Europe, as it is one of the only dedicated facilities for the fabrication of MA containing materials, either for property measurements or for the production of test pins for irradiation experiments. In this paper a detailed description of the MA-Lab facility and the fabrication processes developed to fabricate fuels and samples containing high content of minor actinides is given. In addition, experience gained and improvements are also outlined. (authors)

  1. Status report on actinide and fission product transmutation studies

    International Nuclear Information System (INIS)

    1997-06-01

    The management of radioactive waste is one of the key issues in today's political and public discussions on nuclear energy. One of the fields that looks into the future possibilities of nuclear technology is the neutronic transmutation of actinides and of some most important fission products. Studies on transmutation of actinides are carried out in various countries and at an international level. This status report which gives an up-to-date general overview of current and planned research on transmutation of actinides and fission products in non-OECD countries, has been prepared by a Technical Committee meeting organized by the IAEA in September 1995. 168 refs, 16 figs, 34 tabs

  2. Report of the panel on practical problems in actinide biology

    International Nuclear Information System (INIS)

    Anon.

    1978-01-01

    Practical problems are classified as the need to make operational decisions, the need for regulatory assessment either of individual facilities or of generic actions, and the overt appearance of radiobiological effects in man or radioactivity in man or the environment. Topics discussed are as follows: simulated reactor accident; long term effects of low doses; effects of repeated exposures to actinides; inhaled uranium mine air contaminants; metabolism and dosimetry; environmental equilibrium models; patterns of alpha dosimetry; internal dose calculations; interfaces between actinide biology and environmental studies; removal of actinides deposited in the body; and research needs related to uranium isotopes

  3. Critical masses for the even-neutron-numbered transuranium actinides

    International Nuclear Information System (INIS)

    Westfall, R.M.

    1981-01-01

    As part of a standards effort of the American Nuclear Society to establish subcritical mass limits for the transuranium actinides, critical masses were calculated for seven actinides, critical masses were calculated for seven actinide elements in bare, water-reflected, and steel-reflected metal systems. For the nuclides /sup 242/Pu and /sup 241/Am, values obtained with ENDF/B-V cross-section data were in much better agreement with values inferred from experimental measurement than were initial values calculated with ENDF/B-IV data. A brief description of the analytical methods employed is followed by a presentation of the results. 10 refs

  4. Actinide and Xenon reactivity effects in ATW high flux systems

    International Nuclear Information System (INIS)

    Woosley, M.; Olson, K.; Henderson, D.L.

    1995-01-01

    In this paper, initial system reactivity response to flux changes caused by the actinides and xenon are investigated separately for a high flux ATW system. The maximum change in reactivity after a flux change due to the effect of the changing quantities of actinides is generally at least two orders of magnitude smaller than either the positive or negative reactivity effect associated with xenon after a shutdown or start-up. In any transient flux event, the reactivity response of the system to xenon will generally occlude the response due to the actinides

  5. Actinide and xenon reactivity effects in ATW high flux systems

    International Nuclear Information System (INIS)

    Woosley, M.; Olson, K.; Henderson, D. L.; Sailor, W. C.

    1995-01-01

    In this paper, initial system reactivity response to flux changes caused by the actinides and xenon are investigated separately for a high flux ATW system. The maximum change in reactivity after a flux change due to the effect of the changing quantities of actinides is generally at least two orders of magnitude smaller than either the positive or negative reactivity effect associated with xenon after a shutdown or start-up. In any transient flux event, the reactivity response of the system to xenon will generally occlude the response due to the actinides

  6. Self-interaction corrected local spin density calculations of actinides

    DEFF Research Database (Denmark)

    Petit, Leon; Svane, Axel; Szotek, Z

    2010-01-01

    We use the self-interaction corrected local spin-density approximation in order to describe localization-delocalization phenomena in the strongly correlated actinide materials. Based on total energy considerations, the methodology enables us to predict the ground-state valency configuration...... of the actinide ions in these compounds from first principles. Here we review a number of applications, ranging from electronic structure calculations of actinide metals, nitrides and carbides to the behaviour under pressure of intermetallics, and O vacancies in PuO2....

  7. Actinide and Xenon reactivity effects in ATW high flux systems

    Energy Technology Data Exchange (ETDEWEB)

    Woosley, M. [Univ. of Virginia, Charlottesville, VA (United States); Olson, K.; Henderson, D.L. [Univ. of Wisconsin, Madison, WI (United States)] [and others

    1995-10-01

    In this paper, initial system reactivity response to flux changes caused by the actinides and xenon are investigated separately for a high flux ATW system. The maximum change in reactivity after a flux change due to the effect of the changing quantities of actinides is generally at least two orders of magnitude smaller than either the positive or negative reactivity effect associated with xenon after a shutdown or start-up. In any transient flux event, the reactivity response of the system to xenon will generally occlude the response due to the actinides.

  8. Pb speciation results in amended soils

    Data.gov (United States)

    U.S. Environmental Protection Agency — The dataset shows the distribution of Pb phases resulting from various amendments to change Pb speciation. This dataset is associated with the following publication:...

  9. Speciation of radionuclides in the environment

    International Nuclear Information System (INIS)

    Gunten, H.R. von; Benes, P.

    1994-02-01

    Methods for the determination of the speciation of radionuclides in aerosols, in aquatic solutions, in sediments, soils and rocks are reviewed. At present, most of the results about speciation are deduced from model calculations, model experiments, and separation of species (forms) of radionuclides, e.g., by sequential extraction procedures. Methods of direct determination of speciation of radionuclides (e.g. by laser induced spectroscopy) are in general not yet sensitive enough for a measurement of the very low concentrations of radionuclides in the environment. The methodological part of this paper is followed by a review of the very abundant literature about speciation of important radionuclides in the environment, i.e. in the atmosphere, hydrosphere and lithosphere. The review does not include the biosphere. Literature up to spring 1993 is included (with a few more recent additions). (author)

  10. Evolution: sympatric speciation the eusocial way

    DEFF Research Database (Denmark)

    Boomsma, Jacobus Jan; Nash, David Richard

    2014-01-01

    Sympatric speciation normally requires particular conditions of ecological niche differentiation. However, ant social parasites have been suspected to arise sympatrically, because (dis)loyalty to eusocial kin-structures induces disruptive selection for dispersal and inbreeding. A new study docume...

  11. Dearborn GC-MS organic speciation data

    Data.gov (United States)

    U.S. Environmental Protection Agency — Ambient particulate matter organic speciation data from July - August, 2011. This dataset is associated with the following publication: Lynam, M., T. Dvonch, J....

  12. Aerosol Chemical Speciation Monitor (ACSM) Instrument Handbook

    Energy Technology Data Exchange (ETDEWEB)

    Watson, Thomas B. [Brookhaven National Lab. (BNL), Upton, NY (United States)

    2017-08-15

    The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) measures particle mass loading and chemical composition in real time for non-refractory sub-micron aerosol particles. The ACSM is designed for long-term unattended deployment and routine monitoring applications.

  13. ANALYSE DES PERCEPTIONS LOCALES ET DES FACTEURS ...

    African Journals Online (AJOL)

    AISA

    1Faculté des Sciences Agronomiques (FSA), Université d'Abomey-Calavi (UAC), 01 BP 526 Cotonou Bénin. Email : cgbemavo@yahoo.fr. 2Institut National des Recherches Agricoles du Bénin, Centre de Recherches Agricoles d'Agonkanmey (CRA-A),. Laboratoire des Sciences du Sol, Eau et Environnement (LSSEE).

  14. Fission properties of very heavy actinides

    International Nuclear Information System (INIS)

    Hoffman, D.C.

    1979-01-01

    The existing data on neutron-emission, kinetic-energy and mass distributions, and half-lives for spontaneous fission of the heavy actinides are reviewed. A comparison of the data for the Fm isotopes with heavier and lighter nuclides suggests that the properties of the heavy Fm isotopes may be unique and can qualitatively be explained on the basis of fragment shell effects, i.e., symmetric fission results in two fragments with configurations close to the doubly magic 132 Sn nucleus. The effect of excitation energy and the use of systematics and theoretical predictions of fission properties and half-lives in the identification of new heavy element isotopes is discussed. 54 references

  15. Actinide elements in aquatic and terrestrial environments

    International Nuclear Information System (INIS)

    Bondietti, E.A.

    1978-01-01

    Progress is reported in terrestrial ecology studies with regard to plutonium in biota from the White Oak Creek forest; comparative distribution of plutonium in two forest ecosystems; an ecosystem model of plutonium dynamics; actinide element metabolism in cotton rats; and crayfish studies. Progress is reported in aquatic studies with regard to transuranics in surface waters, frogs, benthic algae, and invertebrates from pond 3513; and radioecology of transuranic elements in cotton rats bordering waste pond 3513. Progress is also reported in stability of trivalent plutonium in White Oak Lake water; chemistry of plutonium, americium, curium, and uranium in pond water; uranium, thorium, and plutonium in small mammals; and effect of soil pretreatment on the distribution of plutonium

  16. Determination of actinides by alpha spectrometric methods

    International Nuclear Information System (INIS)

    Galanda, D.

    2011-01-01

    The submitted thesis in its first part concern with content determination of plutonium, americium, uranium, thorium radionuclides, like the most significant representatives of actinides in environmental patterns, where by the primary consideration is a focusing on content of these actinides in samples of superior mycotic organisms - mushrooms. Following the published studies the mushrooms were monitored as organisms that could verify most of attributes putted on bioindicators in term of observation of substantial radionuclides in living environment. There were analyzed two groups of samples that came from two chosen locations, one of them is situated in Eastern Slovakia and the second one in West Slovakia. Except for mushrooms samples the examined radionuclides volumes were determined even in specimens of soil sub-base and some plants from chosen localities. The liquid - liquid extraction methods were used for determination of mass activities of actinides in samples for radiochemical separation of monitored radionuclides. The obtained results of plutonium and americium mass activities determination's lead us to carry out experiments that proved abilities of superior mycotic organisms to absorb and accumulate alpha radionuclides in their textures. We choose the oyster mushroom (Pleurotus ostreatus) species as an experimental object. Sporocarps of this mushroom were cultivated on substratum which is commercially exploited to cultivate it whereby this substratum was purposely contaminated by known activities of 239 Pu and 241 Am. We prepared five autonomous samples together. The values of mass activities of 239 Pu and 241 Am obtained by following analysis of prepared samples showed the ability of mushrooms to absorb observed actinides in their texture structures. On the basis of obtained mass activities it was possible to evaluate and numerically determine a transmitting factor's attributes of monitored radionuclides in sporocarps and in sub-base. Accordingly we

  17. Actinide behavior in the integral fast reactor

    International Nuclear Information System (INIS)

    Courtney, J.C.

    1993-05-01

    Goal of this project is to determine the consumption of Np-237, Pu-240, Am-241, and Am-243 in the Integral Fast Reactor (IFR) fuel cycle. These four actinides set the long term waste management criteria for spent nuclear fuel; if it can be demonstrated that they can be efficiently consumed in the IFR, then requirements for nuclear waste repositories can be much less demanding. Irradiations in the Experimental Breeder Reactor II (EBR-II) at Argonne National Laboratory's site near Idaho Falls, Idaho, will be conducted to determine fission and transmutation rates for the four nuclides. The experimental effort involves target package design, fabrication, quality assurance, and irradiation. Post irradiation analyses are required to determine the fission rates and neutron spectra in the EBR-II core

  18. Development of Metallic Fuels for Actinide Transmutation

    Energy Technology Data Exchange (ETDEWEB)

    Hayes, Steven Lowe [Idaho National Laboratory; Fielding, Randall Sidney [Idaho National Laboratory; Benson, Michael Timothy [Idaho National Laboratory; Chichester, Heather Jean MacLean [Idaho National Laboratory; Carmack, William Jonathan [Idaho National Laboratory

    2015-09-01

    Research and development activities on metallic fuels are focused on their potential use for actinide transmutation in future sodium fast reactors. As part of this application, there is also a need for a near zero-loss fabrication process and a desire to demonstrate a multifold increase in burnup potential. The incorporation of Am and Np into the traditional U-20Pu-10Zr metallic fuel alloy was demonstrated in the US during the Integral Fast Reactor Program of the 1980’s and early 1990’s. However, the conventional counter gravity injection casting method performed under vacuum, previously used to fabricate these metallic fuel alloys, was not optimized for mitigating loss of the volatile Am constituent in the casting charge; as a result, approximately 40% of the Am casting charge failed to be incorporated into the as-cast fuel alloys. Fabrication development efforts of the past few years have pursued an optimized bottom-pour casting method to increase utilization of the melted charge to near 100%, and a differential pressure casting approach, performed under an argon overpressure, has been demonstrated to result in essentially no loss of Am due to volatilization during fabrication. In short, a path toward zero-loss fabrication of metallic fuels including minor actinides has been shown to be feasible. Irradiation testing of advanced metallic fuel alloys in the Advanced Test Reactor (ATR) has been underway since 2003. Testing in the ATR is performed inside of cadmium-shrouded positions to remove >99% of the thermal flux incident on the test fuels, resulting in an epi-thermal driven fuel test that is free from gross flux depression and producing an essentially prototypic radial temperature profile inside the fuel rodlets. To date, three irradiation test series (AFC-1,2,3) have been completed. Over 20 different metallic fuel alloys have been tested to burnups as high as 30% with constituent compositions of Pu up to 30%, Am up to 12%, Np up to 10%, and Zr between 10

  19. Role of actinide behavior in waste management

    International Nuclear Information System (INIS)

    Bartlett, J.W.

    1976-01-01

    For purposes of assessing the safety of repositories of radioactive wastes placed in geologic isolation, actinide behavior in the environment has been interpreted in terms of five steps of prediction: analysis of repository stability; geosphere transport; the geosphere-biosphere interface; biosphere transport; and biosphere consequences. Each step in the analysis requires models of nuclide behavior and data on the physical and chemical properties of the radioactivity. The scope of information required in order to make reliable safety assessments has been outlined. All steps in the assessment process are coupled; reliable models and data are therefore needed for each step. The prediction phase of safety assessment is also coupled to activities concerned with waste treatment, selection of the final form of the waste, and selection of repository sites and designs. Results of the predictions can impact these activities

  20. 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.)

  1. Solution speciation of plutonium and Americium at an Australian legacy radioactive waste disposal site.

    Science.gov (United States)

    Ikeda-Ohno, Atsushi; Harrison, Jennifer J; Thiruvoth, Sangeeth; Wilsher, Kerry; Wong, Henri K Y; Johansen, Mathew P; Waite, T David; Payne, Timothy E

    2014-09-02

    During the 1960s, radioactive waste containing small amounts of plutonium (Pu) and americium (Am) was disposed in shallow trenches at the Little Forest Burial Ground (LFBG), located near the southern suburbs of Sydney, Australia. Because of periodic saturation and overflowing of the former disposal trenches, Pu and Am have been transferred from the buried wastes into the surrounding surface soils. The presence of readily detected amounts of Pu and Am in the trench waters provides a unique opportunity to study their aqueous speciation under environmentally relevant conditions. This study aims to comprehensively investigate the chemical speciation of Pu and Am in the trench water by combining fluoride coprecipitation, solvent extraction, particle size fractionation, and thermochemical modeling. The predominant oxidation states of dissolved Pu and Am species were found to be Pu(IV) and Am(III), and large proportions of both actinides (Pu, 97.7%; Am, 86.8%) were associated with mobile colloids in the submicron size range. On the basis of this information, possible management options are assessed.

  2. Using hydrogeochemical data from natural environments to improve models of radionuclide speciation in groundwaters

    International Nuclear Information System (INIS)

    Read, D.; Hooker, P.

    1991-01-01

    It is essential that computer-based models used in the safety assessment of radioactive waste repositories accurately represent the processes occurring in real field systems. Confidence in long-term predictions of radionuclide migration will then depend upon the completeness of data available, particularly those obtained from the disposal site, and correct implementation of the model. The study of natural geochemical systems provides information on the adequacy of the underlying generic database and enhances our understanding of the transport mechanisms which form the basis of performance assessment. This paper concentrates on speciation-solubility modelling and describes four natural occurrences of uranium, each of which displays a different facet of uranium migration behaviour. The attributes of each site and the means by which uranium is immobilised are described. Retardation is highly species specific and this is illustrated through the use of site data in equilibrium speciation and coupled chemical transport calculations. Oxidation of U(IV) to U(VI) species promotes leaching of uranium ore at all the locations studied, emphasising the need to ensure that reducing conditions persist in a repository dominated by its actinide inventory. 5 figs., 46 refs

  3. Radiochemical studies of neutron deficient actinide isotopes

    International Nuclear Information System (INIS)

    Williams, K.E.

    1978-04-01

    The production of neutron deficient actinide isotopes in heavy ion reactions was studied using alpha, gamma, x-ray, and spontaneous fission detection systems. A new isotope of berkelium, 242 Bk, was produced with a cross-section of approximately 10 μb in reactions of boron on uranium and nitrogen on thorium. It decays by electron capture with a half-life of 7.0 +- 1.3 minutes. The alpha-branching ratio for this isotope is less than 1% and the spontaneous fission ratio is less than 0.03%. Studies of (Heavy Ion, pxn) and (Heavy Ion, αxn) transfer reactions in comparison with (Heavy ion, xn) compound nucleus reactions revealed transfer reaction cross-sections equal to or greater than the compound nucleus yields. The data show that in some cases the yield of an isotope produced via a (H.I.,pxn) or (H.I.,αxn) reaction may be higher than its production via an xn compound nucleus reaction. These results have dire consequences for proponents of the ''Z 1 + Z 2 = Z/sub 1+2/'' philosophy. It is no longer acceptable to assume that (H.I.,pxn) and (H.I.,αxn) product yields are of no consequence when studying compound nucleus reactions. No evidence for spontaneous fission decay of 228 Pu, 230 Pu, 232 Cm, or 238 Cf was observed indicating that strictly empirical extrapolations of spontaneous fission half-life data is inadequate for predictions of half-lives for unknown neutron deficient actinide isotopes

  4. Archetypes for actinide-specific chelating agents

    International Nuclear Information System (INIS)

    Smith, W.L.

    1980-01-01

    The complexes of uranium and thorium with monomeric hydroxamic acids can serve as archetypes for an optimized macrochelate designed for tetravalent actinides. The eight-coordinate complexes, Th(i-PrN(O)C(O)R) 4 , where R = tert-butyl or R = neopentyl, have been synthesized and their structures have been determined by x-ray diffraction. The bulky alkyl substituents impart remarkable volatility and hydrocarbon solubility to these complexes, and the steric interactions of these substituents largely determine the structures. When R = tert-butyl, the substituents occupy the corners of a tetrahedron and force the complex into a distorted cubic geometry with crystallographic S 4 symmetry. Insertion of a methylene group between the carbonyl carbon and the tert-butyl group relaxes the steric requirements, and the coordination polyhedron of the neopentyl derivative is close to the mmmm isomer of the trigonal-faced dodecahedron. Uranium tetrachloride was quantitatively oxidized via an oxygen transfer reaction with two equivalents of N-phenylbenzohydroxamic acid anion (PBHA) in tetrahydrofuran (THF) to form UO 2 Cl(PBHA)(THF) 2 and benzanilide. The structure of the uranyl complex has been determined from x-ray diffraction data; the linear uranyl ion is surrounded by a planar pentagonal array composed of two hydroxamate oxygen atoms, a chloride ion and two THF oxygens, such that the chloride ion is opposite the hydroxamate group. That the THF and phenyl rings are twisted from this equatorial plane limits the molecular geometry to that of the C 1 point group. Some aspects of the chemistry of hydroxamic acids and of their incorporation into molecules that may serve as precursors of tetravalent actinide specific sequestering agents have also been investigated

  5. Radiochemical studies of neutron deficient actinide isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Williams, K.E.

    1978-04-01

    The production of neutron deficient actinide isotopes in heavy ion reactions was studied using alpha, gamma, x-ray, and spontaneous fission detection systems. A new isotope of berkelium, /sup 242/Bk, was produced with a cross-section of approximately 10 ..mu..b in reactions of boron on uranium and nitrogen on thorium. It decays by electron capture with a half-life of 7.0 +- 1.3 minutes. The alpha-branching ratio for this isotope is less than 1% and the spontaneous fission ratio is less than 0.03%. Studies of (Heavy Ion, pxn) and (Heavy Ion, ..cap alpha..xn) transfer reactions in comparison with (Heavy ion, xn) compound nucleus reactions revealed transfer reaction cross-sections equal to or greater than the compound nucleus yields. The data show that in some cases the yield of an isotope produced via a (H.I.,pxn) or (H.I.,..cap alpha..xn) reaction may be higher than its production via an xn compound nucleus reaction. These results have dire consequences for proponents of the ''Z/sub 1/ + Z/sub 2/ = Z/sub 1+2/'' philosophy. It is no longer acceptable to assume that (H.I.,pxn) and (H.I.,..cap alpha..xn) product yields are of no consequence when studying compound nucleus reactions. No evidence for spontaneous fission decay of /sup 228/Pu, /sup 230/Pu, /sup 232/Cm, or /sup 238/Cf was observed indicating that strictly empirical extrapolations of spontaneous fission half-life data is inadequate for predictions of half-lives for unknown neutron deficient actinide isotopes.

  6. Pyrometallurgical processes for recovery of actinide elements

    International Nuclear Information System (INIS)

    Battles, J.E.; Laidler, J.J.; McPheeters, C.C.; Miller, W.E.

    1994-01-01

    A metallic fuel alloy, nominally U-20-Pu-lOZr, is the key element of the Integral Fast Reactor (IFR) fuel cycle. Metallic fuel permits the use of an innovative, simple pyrometallurgical process, known as pyroprocessing, (the subject of this report), which features fused salt electrorefining of the spent fuel. Electrorefining separates the actinide elements from fission products, without producing a separate stream of plutonium. The plutonium-bearing product is contaminated with higher actinides and with a minor amount of rare earth fission products, making it diversion resistant while still suitable as a fuel material in the fast spectrum of the IFR core. The engineering-scale demonstration of this process will be conducted in the refurbished EBR-II Fuel Cycle Facility, which has entered the start-up phase. An additional pyrometallurgical process is under development for extracting transuranic (TRU) elements from Light Water Reactor (LWR) spent fuel in a form suitable for use as a feed to the IFR fuel cycle. Four candidate extraction processes have been investigated and shown to be chemically feasible. The main steps in each process are oxide reduction with calcium or lithium, regeneration of the reductant and recycle of the salt, and separation of the TRU product from the bulk uranium. Two processes, referred to as the lithium and salt transport (calcium reductant) processes, have been selected for engineering-scale demonstration, which is expected to start in late 1993. An integral part of pyroprocessing development is the treatment and packaging of high-level waste materials arising from the operations, along with the qualification of these waste forms for disposal in a geologic repository

  7. Studies of actinides in a superanoxic fjord

    Energy Technology Data Exchange (ETDEWEB)

    Roos, P.

    1997-04-01

    Water column and sediment profiles of Pu, Am, Th and U have been obtained in the superanoxic Framvaren fjord, southern Norway. The concentration of bomb test fallout Pu, Am as well as `dissolved` Th in the bottom water are the highest recorded in the marine environment. The behaviour of the actinides in the anoxic water mass is to a large extent governed by the behaviour of the colloidal material. Ultrafiltration reveals that 40-60% of the actinides are associated to the large colloids, surprisingly this is valid also for U. The sediment acts as a source for Pu, Am, and Th to the water column but primarily as a sink for U. The remobilization of Pu, Am and Th is evident from the water column profiles which have similar diffusion shape profiles as other constituents originating from the sediments. The vertical eddy diffusion coefficient calculated from the Pu profile is in the same order of magnitude as reported from the H{sub 2}S profile. Decreased bottom water concentrations (but a constant water column inventory) between 1989 and 1995 as well as pore water Pu concentrations nearly identical to the overlaying bottom water indicates that the present Pu flux from the sediments are low. Contrary to Pu and Am, the water column Th inventory ({sup 232}Th and {sup 230}Th) continues to increase. The flux of {sup 232}Th from the sediments was determined from changes in water column inventory between 1989 and 1995 and from a pore water profile to be in the order of 2-8 Bq/m{sup 2}/y. 208 refs.

  8. Pyrometallurgical processes for recovery of actinide elements

    Energy Technology Data Exchange (ETDEWEB)

    Battles, J.E.; Laidler, J.J.; McPheeters, C.C.; Miller, W.E.

    1994-01-01

    A metallic fuel alloy, nominally U-20-Pu-lOZr, is the key element of the Integral Fast Reactor (IFR) fuel cycle. Metallic fuel permits the use of an innovative, simple pyrometallurgical process, known as pyroprocessing, (the subject of this report), which features fused salt electrorefining of the spent fuel. Electrorefining separates the actinide elements from fission products, without producing a separate stream of plutonium. The plutonium-bearing product is contaminated with higher actinides and with a minor amount of rare earth fission products, making it diversion resistant while still suitable as a fuel material in the fast spectrum of the IFR core. The engineering-scale demonstration of this process will be conducted in the refurbished EBR-II Fuel Cycle Facility, which has entered the start-up phase. An additional pyrometallurgical process is under development for extracting transuranic (TRU) elements from Light Water Reactor (LWR) spent fuel in a form suitable for use as a feed to the IFR fuel cycle. Four candidate extraction processes have been investigated and shown to be chemically feasible. The main steps in each process are oxide reduction with calcium or lithium, regeneration of the reductant and recycle of the salt, and separation of the TRU product from the bulk uranium. Two processes, referred to as the lithium and salt transport (calcium reductant) processes, have been selected for engineering-scale demonstration, which is expected to start in late 1993. An integral part of pyroprocessing development is the treatment and packaging of high-level waste materials arising from the operations, along with the qualification of these waste forms for disposal in a geologic repository.

  9. Studies of actinides in a superanoxic fjord

    International Nuclear Information System (INIS)

    Roos, P.

    1997-04-01

    Water column and sediment profiles of Pu, Am, Th and U have been obtained in the superanoxic Framvaren fjord, southern Norway. The concentration of bomb test fallout Pu, Am as well as 'dissolved' Th in the bottom water are the highest recorded in the marine environment. The behaviour of the actinides in the anoxic water mass is to a large extent governed by the behaviour of the colloidal material. Ultrafiltration reveals that 40-60% of the actinides are associated to the large colloids, surprisingly this is valid also for U. The sediment acts as a source for Pu, Am, and Th to the water column but primarily as a sink for U. The remobilization of Pu, Am and Th is evident from the water column profiles which have similar diffusion shape profiles as other constituents originating from the sediments. The vertical eddy diffusion coefficient calculated from the Pu profile is in the same order of magnitude as reported from the H 2 S profile. Decreased bottom water concentrations (but a constant water column inventory) between 1989 and 1995 as well as pore water Pu concentrations nearly identical to the overlaying bottom water indicates that the present Pu flux from the sediments are low. Contrary to Pu and Am, the water column Th inventory ( 232 Th and 230 Th) continues to increase. The flux of 232 Th from the sediments was determined from changes in water column inventory between 1989 and 1995 and from a pore water profile to be in the order of 2-8 Bq/m 2 /y. 208 refs

  10. Molecular and supramolecular speciation of monoamide extractant systems

    International Nuclear Information System (INIS)

    Ferru, G.

    2012-01-01

    DEHiBA (N,N-di-(ethyl-2-hexyl)isobutyramide, a monoamide, was chosen as selective extractant for the recovery of uranium in the first cycle of the GANEX process, which aims to realize the grouped extraction of actinides in the second step of the process. The aim of this work is an improved description of monoamide organic solutions in alkane diluent after solutes extraction: water, nitric acid and uranyl nitrate. A parametric study was undertaken to characterize species at molecular scale (by IR spectroscopy, UV-visible spectroscopy, time-resolved laser-induced fluorescence spectroscopy, and electro-spray ionisation mass spectrometry) and at supramolecular scale (by vapor pressure osmometry and small angle X-ray scattering coupled to molecular dynamic simulations). Extraction isotherms were modelled taking into account the molecular and supramolecular speciation. These works showed that the organization of the organic solution depends on the amide concentration, the nature and the concentration of the extracted solute. Three regimes can be distinguished. 1/For extractant concentration less than 0.5 mol/L, monomers are predominate species. 2/ For extractant concentrations between 0.5 and 1 mol/L, small aggregates are formed containing 2 to 4 molecules of monoamide. 3/ For more concentrated solutions (greater than 1 mol/L), slightly larger species can be formed after water or nitric acid extraction. Concerning uranyl nitrate extraction, an important and strong organization of the organic phase is observed, which no longer allows the formation of well spherical defined aggregates. At molecular scale, complexes are not sensitive to the organization of the solution: the same species are observed, regardless of the solute and extractant concentrations in organic phase. (author) [fr

  11. Actinide targets for the synthesis of super-heavy elements

    International Nuclear Information System (INIS)

    Roberto, J.B.; Alexander, C.W.; Boll, R.A.; Burns, J.D.; Ezold, J.G.; Felker, L.K.; Hogle, S.L.; Rykaczewski, K.P.

    2015-01-01

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of "4"8Ca beams on actinide targets. These target materials, including "2"4"2Pu, "2"4"4Pu, "2"4"3Am, "2"4"5Cm, "2"4"8Cm, "2"4"9Cf, and "2"4"9Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing the production of rare actinides including "2"4"9Bk, "2"5"1Cf, and "2"5"4Es are described.

  12. Advanced techniques for actinide spectroscopy (ATAS 2012). Abstract book

    Energy Technology Data Exchange (ETDEWEB)

    Foerstendorf, Harald; Mueller, Katharina; Steudtner, Robin [eds.

    2012-07-01

    The abstract book of the International workshop on advanced techniques for actinide spectroscopy (ATAS 2012) include contributions concerning the following issues: environmental applications, NMR spectroscopy, vibrational spectroscopy, X-ray spectroscopy and theory, technical application: separation processes, emission spectroscopy.

  13. Advanced techniques for actinide spectroscopy (ATAS 2012). Abstract book

    International Nuclear Information System (INIS)

    Foerstendorf, Harald; Mueller, Katharina; Steudtner, Robin

    2012-01-01

    The abstract book of the International workshop on advanced techniques for actinide spectroscopy (ATAS 2012) include contributions concerning the following issues: environmental applications, NMR spectroscopy, vibrational spectroscopy, X-ray spectroscopy and theory, technical application: separation processes, emission spectroscopy.

  14. 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

  15. The chemistry of the actinide elements. Volume I

    International Nuclear Information System (INIS)

    Katz, J.J.; Seaborg, G.T.; Morss, L.R.

    1986-01-01

    The Chemistry of the Actinide Elements is a comprehensive, contemporary and authoritative exposition of the chemistry and related properties of the 5f series of elements: actinium, thorium, protactinium, uranium and the first eleven. This second edition has been completely restructured and rewritten to incorporate current research in all areas of actinide chemistry and chemical physics. The descriptions of each element include accounts of their history, separation, metallurgy, solid-state chemistry, solution chemistry, thermo-dynamics and kinetics. Additionally, separate chapters on spectroscopy, magnetochemistry, thermodynamics, solids, the metallic state, complex ions and organometallic compounds emphasize the comparative chemistry and unique properties of the actinide series of elements. Comprehensive lists of properties of all actinide compounds and ions in solution are given, and there are special sections on such topics as biochemistry, superconductivity, radioisotope safety, and waste management, as well as discussion of the transactinides and future elements

  16. 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

  17. 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.

  18. 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.

  19. 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

  20. What fits best minor actinides as a die material?

    International Nuclear Information System (INIS)

    Hinfray, J.

    2003-01-01

    Zirconolite might be the die material used to confine actinides definitively. Cea's teams have been investigating the ability of zirconolite to trap actinide atoms in its own crystal structure. These studies have been performed with 239 Pu that presents the same ability to set chemical links with the constituents of the die as 3 minor actinides do. Crystal materials like zirconolite are more sensitive to self irradiation than glass. The next step of the characterization of zirconolite is to evaluate its capacity to sustain self alpha irradiation. In order to do so, 238 Pu is used since its relatively short period (T = 87 years) allows an acceleration of the process : damages cumulated in the die material in 2 years will be equivalent to those produced by minor actinides for millions years. The results will be known in 2004. (A.C.)

  1. Leaching of actinides from nuclear waste glass: French experience

    International Nuclear Information System (INIS)

    Vernaz, E.Y.; Godon, N.

    1991-01-01

    The activity concentration versus time of a typical LWR glass shows that after 300 years most of the activity is attributable to three actinides (Np, Pu and Am) and to 99 Tc. This activity decreases slowly, and some 50.000 years are necessary before the activity concentration drops to the level of the richest natural ores. This paper reviews the current state of knowledge concerning the kinetics of actinide release from glass subjected to aqueous leaching

  2. Chemical factors controlling actinide sorption in the environment

    International Nuclear Information System (INIS)

    Beall, G.W.; Allard, B.

    1979-01-01

    The solid geologic media and the aqueous phase are of equal importance for the retention of actinides in the environment. The composition of the water is largely determined by the mineralogical composition of the rock that it is in equilibrium with. The chemical form of the actinides and their sorption, are highly dependent on the composition of the water with respect to pH, redox potential, and concentration of anions like carbonate, phosphate, fluoride, and organic acids

  3. Actinides complexes in solvent extraction. The amide type of extractants

    International Nuclear Information System (INIS)

    Musikas, C.; Condamines, N.; Charbonnel, M.C.; Hubert, H.

    1989-01-01

    The N,N-dialkylamides and the N,N'-tetraalkyl. 2-alkyl 1,3-diamide propane are two promising classes of extractants which could replace advantageously the organophosphorus molecules for the separations of the actinide. The main advantages of the amides lie in their complete incinerability and the small interference of their radiolytic and hydrolytic degradation products for the processes. The actinide extraction chemistry with various amides is reviewed in this paper

  4. Extraction of tetravalent and hexavalent actinide ions by tetraheptylammonium nitrate

    International Nuclear Information System (INIS)

    Swarup, Rajendra; Patil, S.K.

    1977-01-01

    Extraction of Th(IV), Np(IV), Pu(IV), U(VI), Np(VI), and Pu(VI) by tetraheptylammonium nitrate in Solvesso-100 has been studied from nitric acid medium. Attempts were made to identify the complex species in the organic phase by studying the dependence of the distribution coefficient of the actinide on amine concentration and taking the absorption spectra of the organic phase containing actinide ions. A compound tetraheptylammonium trinitratodioxouranate (VI) has been isolated and characterised. (author)

  5. Electronic structure and properties of rare earth and actinide intermetallics

    International Nuclear Information System (INIS)

    Kirchmayr, H.R.

    1984-01-01

    There are 188 contributions, experimental and theoretical, a few on rare earth and actinide elements but mostly on rare earth and actinide intermetallic compounds and alloys. The properties dealt with include 1) crystal structure, 2) magnetic properties and magnetic structure, 3) magnetic phase transformations and valence fluctuations, 4) electrical properties and superconductivity and their temperature, pressure and magnetic field dependence. A few papers deal with crystal growth and novel measuring methods. (G.Q.)

  6. Methods for separating actinides from reprocessing and refabrication plant wastes

    International Nuclear Information System (INIS)

    Tedder, D.W.; Finney, B.C.; Blomeke, J.O.

    1979-01-01

    Chemical processing flowsheets have been developed to partition actinides from all actinide-bearing LWR fuel reprocessing and refabrication plant wastes. These wastes include high-activity-level liquids, scrap recovery liquors, HEPA filters and incinerator ashes, and chemical salt wastes such as sodium carbonate scrub solutions, detergent cleanup streams, and alkaline off-gas scrubber liquors. The separations processes that were adopted for this study are based on solvent extraction, cation exchange chromatography, and leaching with Ce 4+ -HNO 3 solution

  7. Mixer-settler performance evaluation in actinide extraction

    International Nuclear Information System (INIS)

    Camilo, R.L.; Goncalves, M.A.; Carvalho, E.I.; Nakazone, A.K.; Araujo, B.F. de; Araujo, J.A.

    1988-07-01

    This paper deals with four conceptions of mixer-settlers used for actinide purification and recovery. By means of the uranium concentration profiles in the organic and aqueous phases, the evaluation of each mixer-settler was made. The main purpose of this work is the data acquisition, for adapting the different contactor types to actinide recovery by liquid-liquid extraction, in the nuclear fuel cycle. (autor) [pt

  8. Selfish X chromosomes and speciation.

    Science.gov (United States)

    Patten, Manus M

    2017-12-27

    In two papers published at about the same time almost thirty years ago, Frank (Evolution, 45, 1991a, 262) and Hurst and Pomiankowski (Genetics, 128, 1991, 841) independently suggested that divergence of meiotic drive systems-comprising genes that cheat meiosis and genes that suppress this cheating-might provide a general explanation for Haldane's rule and the large X-effect in interspecific hybrids. Although at the time, the idea was met with skepticism and a conspicuous absence of empirical support, the tide has since turned. Some of the clearest mechanistic explanations we have for hybrid male sterility involve meiotic drive systems, and several other cases of hybrid sterility are suggestive of a role for meiotic drive. In this article, I review these ideas and their descendants and catalog the current evidence for the meiotic drive model of speciation. In addition, I suggest that meiotic drive is not the only intragenomic conflict to involve the X chromosome and contribute to hybrid incompatibility. Sexually and parentally antagonistic selection pressures can also pit the X chromosome and autosomes against each other. The resulting intragenomic conflicts should lead to co-evolution within populations and divergence between them, thus increasing the likelihood of incompatibilities in hybrids. I provide a sketch of these ideas and interpret some empirical patterns in the light of these additional X-autosome conflicts. © 2017 John Wiley & Sons Ltd.

  9. 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)

  10. 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

  11. 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.

  12. 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.

  13. 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

  14. Protactinium and the intersection of actinide and transition metal chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Wilson, Richard E.; De Sio, Stephanie; Vallet, Valérie

    2018-02-12

    The role of the 5f and 6d orbitals in the chemistry of the actinide elements has been of considerable interest since their discovery and synthesis. Relativistic effects cause the energetics of the 5f and 6d orbitals to change as the actinide series is traversed left to right imparting a rich and complex chemistry. The 5f and 6d atomic states cross in energy at protactinium (Pa), making it a potential intersection between transition metal and actinide chemistries. Herein, we report the synthesis of a Pa-peroxo cluster, A(6)(Pa4O(O-2)(6)F-12) [A = Rb, Cs, (CH3)(4)N], formed in pursuit of an actinide polyoxometalate. Quantum chemical calculations at the density functional theory level demonstrate equal 5f and 6d orbital participation in the chemistry of Pa and increasing 5f orbital participation for the heavier actinides. Periodic changes in orbital character to the bonding in the early actinides highlights the influence of the 5f orbitals in their reactivity and chemical structure.

  15. 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

  16. Modelisation des effets physico-techniques pour la conception des ...

    African Journals Online (AJOL)

    automatisation dans les installations industrielles a besoin d'une régulation automatique des commandes des processus technologiques pour lesquelles certaines contraintes sont à relever compte tenu des exigences des innovations scientifiques de ...

  17. Speciation of plutonium during sorption and diffusion in Opalinus clay

    International Nuclear Information System (INIS)

    Kaplan, Ugras

    2013-01-01

    The presented work was carried out in the framework of the BMWi-project ''Interaction and migration of actinides in natural clay rocks taking into account humic substances and clay organic matter - Interactions of neptunium and plutonium with natural clay rocks''. For the long-term safety assessments of nuclear repositories, the possible migration of the radiotoxic wastes into the environment must be considered. Due to its long half-life (T 1/2 = 24000 y) 239 Pu has a significant contribution to the radiotoxicity of spent nuclear fuel in a repository after long periods of storage. The redox-sensitive plutonium has a very complicated chemical behavior. In aqueous solution under environmental relevant conditions Pu can exist in oxidation states +III to +VI and it can exist in up to four oxidation states simultaneously in a solution. Clays are considered as a possible host rock formation for of high-level radioactive waste disposal. Therefore, detailed information on the mobilization and immobilization of plutonium through / into the groundwater from a repository are of special interest. In this work new insights into the interaction between Pu and natural Opalinus clay (OPA, Mont Terri, Switzerland) are obtained with regard to the disposal of heat-generating radioactive waste in a deep geological repository.rnThe focus of this work was on the determination of the speciation of Pu on the mineral surface after sorption and diffusion process by different synchrotron based techniques (μ-XRF, μ-XANES/-EXAFS, μ-XRD, and EXAFS/XANES). The interaction between Pu and OPA was studied in batch sorption and diffusion experiments in dependence of various experimental parameters (e.g. pH, Pu oxidation state). Sorption experiments showed that some experimental parameters (e.g. temperature, humic acid) have a significant impact on the sorption of Pu on OPA. Speciation studies were performed as a function of various chemical parameters on powder samples form batch experiments as

  18. Interface reactions of actinides on muscovite; Grenzflaechenreaktionen von Actiniden an Muskovit

    Energy Technology Data Exchange (ETDEWEB)

    Hellebrandt, Stefan

    2017-11-06

    adsorbed U was detected at the muscovite interface according to all methods applied, despite the larger concentration of the adsorbate. This difference in the sorption behavior can be explained by the different redox behavior of U and Pu. U will stay mainly in its predominant oxidation state VI, due to its higher stability compared to Pu, while Pu will be present as Pu(VI), but also in a greater extent in its reduced oxidation states. Due to this difference Pu is able to form nanoparticles, whereas this is not the case for U. The third part compares the sorption of trivalent actinides Am(III) and Cm(III) and their homolog Eu(III) on alumino-silicates muscovite (phyllosilicate) and orthoclase (framework silicate). Under acidic conditions all elements adsorb as outer-sphere complexes, while the relative amount of inner-sphere sorption increases with increasing pH. At higher pH a transition from adsorbed aquoions to adsorbed hydrolysis-species and eventually a ternary sorption complex is observed. While TRLFS itself is a strong tool to investigate the speciation of metals in solution or in contact with a mineral surface the complementary use of SXS techniques is able to improve these findings. The results of this work, achieved by using modern methods such as X-ray scattering techniques (CTR/RAXR) and TRLFS, have afforded new insights into the surface reactivity of a wide range of actinides (Th, U, Pu, Am, and Cm) in contact with muscovite and orthoclase. New influence factors could be identified in the influence of the background electrolyte on the sorption behavior, where both cation and anion affect the actinide's retention. The different redox behavior of redox-active actinides like U and Pu also influenced the sorption behavior tremendously, even in contact with the redox-inactive mineral muscovite. The complementary use of surface X-ray diffraction and laser spectroscopic methods was instrumental to enable us to investigate the distribution, occupancy, and

  19. 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

  20. How Facilitation May Interfere with Ecological Speciation

    Directory of Open Access Journals (Sweden)

    P. Liancourt

    2012-01-01

    Full Text Available Compared to the vast literature linking competitive interactions and speciation, attempts to understand the role of facilitation for evolutionary diversification remain scarce. Yet, community ecologists now recognize the importance of positive interactions within plant communities. Here, we examine how facilitation may interfere with the mechanisms of ecological speciation. We argue that facilitation is likely to (1 maintain gene flow among incipient species by enabling cooccurrence of adapted and maladapted forms in marginal habitats and (2 increase fitness of introgressed forms and limit reinforcement in secondary contact zones. Alternatively, we present how facilitation may favour colonization of marginal habitats and thus enhance local adaptation and ecological speciation. Therefore, facilitation may impede or pave the way for ecological speciation. Using a simple spatially and genetically explicit modelling framework, we illustrate and propose some first testable ideas about how, when, and where facilitation may act as a cohesive force for ecological speciation. These hypotheses and the modelling framework proposed should stimulate further empirical and theoretical research examining the role of both competitive and positive interactions in the formation of incipient species.

  1. Speciation of zinc in contaminated soils

    International Nuclear Information System (INIS)

    Stephan, Chadi H.; Courchesne, Francois; Hendershot, William H.; McGrath, Steve P.; Chaudri, Amar M.; Sappin-Didier, Valerie; Sauve, Sebastien

    2008-01-01

    The chemical speciation of zinc in soil solutions is critical to the understanding of its bioavailability and potential toxic effects. We studied the speciation of Zn in soil solution extracts from 66 contaminated soils representative of a wide range of field conditions in both North America and Europe. Within this dataset, we evaluated the links among the dissolved concentrations of zinc and the speciation of Zn 2+ , soil solution pH, total soil Zn, dissolved organic matter (DOM), soil organic matter (SOM) and the concentrations of different inorganic anions. The solid-liquid partitioning coefficient (K d ) for Zn ranged from 17 to 13,100 L kg -1 soil. The fraction of dissolved Zn bound to DOM varied from 60% to 98% and the soil solution free Zn 2+ varied from 40% to 60% of the labile Zn. Multiple regression equations to predict free Zn 2+ , dissolved Zn and the solid-liquid partitioning of Zn are given for potential use in environmental fate modeling and risk assessment. The multiple regressions also highlight some of the most important soil properties controlling the solubility and chemical speciation of zinc in contaminated soils. - We studied the relationships among the chemical speciation of Zn in soil solution extracts from 66 contaminated soils and various physicochemical properties of the soils

  2. Speciation by Symbiosis: the Microbiome and Behavior.

    Science.gov (United States)

    Shropshire, J Dylan; Bordenstein, Seth R

    2016-03-31

    Species are fundamental units of comparison in biology. The newly discovered importance and ubiquity of host-associated microorganisms are now stimulating work on the roles that microbes can play in animal speciation. We previously synthesized the literature and advanced concepts of speciation by symbiosis with notable attention to hybrid sterility and lethality. Here, we review recent studies and relevant data on microbes as players in host behavior and behavioral isolation, emphasizing the patterns seen in these analyses and highlighting areas worthy of additional exploration. We conclude that the role of microbial symbionts in behavior and speciation is gaining exciting traction and that the holobiont and hologenome concepts afford an evolving intellectual framework to promote research and intellectual exchange between disciplines such as behavior, microbiology, genetics, symbiosis, and speciation. Given the increasing centrality of microbiology in macroscopic life, microbial symbiosis is arguably the most neglected aspect of animal and plant speciation, and studying it should yield a better understanding of the origin of species. Copyright © 2016 Shropshire and Bordenstein.

  3. Actinide production in 136Xe bombardments of 249Cf

    International Nuclear Information System (INIS)

    Gregorich, K.E.

    1985-08-01

    The production cross sections for the actinide products from 136 Xe bombardments of 249 Cf at energies 1.02, 1.09, and 1.16 times the Coulomb barrier were determined. Fractions of the individual actinide elements were chemically separated from recoil catcher foils. The production cross sections of the actinide products were determined by measuring the radiations emitted from the nuclides within the chemical fractions. The chemical separation techniques used in this work are described in detail, and a description of the data analysis procedure is included. The actinide production cross section distributions from these 136 Xe + 249 Cf bombardments are compared with the production cross section distributions from other heavy ion bombardments of actinide targets, with emphasis on the comparison with the 136 Xe + 248 Cm reaction. A technique for modeling the final actinide cross section distributions has been developed and is presented. In this model, the initial (before deexcitation) cross section distribution with respect to the separation energy of a dinuclear complex and with respect to the Z of the target-like fragment is given by an empirical procedure. It is then assumed that the N/Z equilibration in the dinuclear complex occurs by the transfer of neutrons between the two participants in the dinuclear complex. The neutrons and the excitation energy are statistically distributed between the two fragments using a simple Fermi gas level density formalism. The resulting target-like fragment initial cross section distribution with respect to Z, N, and excitation energy is then allowed to deexcite by emission of neutrons in competition with fission. The result is a final cross section distribution with respect to Z and N for the actinide products. 68 refs., 33 figs., 6 tabs

  4. Actinides in irradiated graphite of RBMK-1500 reactor

    Energy Technology Data Exchange (ETDEWEB)

    Plukienė, R., E-mail: rita@ar.fi.lt; Plukis, A.; Barkauskas, V.; Gudelis, A.; Gvozdaitė, R.; Duškesas, G.; Remeikis, V.

    2014-10-01

    Highlights: • Activation of actinides in the graphite of the RBMK-1500 reactor was analyzed. • Numerical modeling using SCALE 6.1 and MCNPX was used for actinide calculation. • Measurements of the irradiated graphite sample were used for model validation. • Results are important for further decommissioning process of the RBMK type reactors. - Abstract: The activation of graphite in the nuclear power plants is the problem of high importance related with later graphite reprocessing or disposal. The activation of actinide impurities in graphite due to their toxicity determines a particular long term risk to waste management. In this work the activation of actinides in the graphite constructions of the RBMK-1500 reactor is determined by nuclear spectrometry measurements of the irradiated graphite sample from the Ignalina NPP Unit I and by means of numerical modeling using two independent codes SCALE 6.1 (using TRITON-VI sequence) and MCNPX (v2.7 with CINDER). Both models take into account the 3D RBMK-1500 reactor core fragment with explicit graphite construction including a stack and a sleeve but with a different simplification level concerning surrounding graphite and construction of control roads. The verification of the model has been performed by comparing calculated and measured isotope ratios of actinides. Also good prediction capabilities of the actinide activation in the irradiated graphite have been found for both calculation approaches. The initial U impurity concentration in the graphite model has been adjusted taking into account the experimental results. The specific activities of actinides in the irradiated RBMK-1500 graphite constructions have been obtained and differences between numerical simulation results, different structural parts (sleeve and stack) as well as comparison with previous results (Ancius et al., 2005) have been discussed. The obtained results are important for further decommissioning process of the Ignalina NPP and other RBMK

  5. Fast neutron scattering on actinide nuclei

    International Nuclear Information System (INIS)

    1982-01-01

    More and more sophisticated neutron experiments have been carried out with better samples in several laboratories and it was necessary to intercompare them. In this respect, let us quote for example (n,n'e) and (n,n'#betta#) measurements. Moreover, high precision (p,p), (p,p') and (p,n) measurements have been made, thus supplementing neutron experiments in the determination of the parameters of the optical model, still widely used to describe the neutron-nucleus interaction. The optical model plays a major role and it is therefore essential to know it well. The spherical optical model is still very useful, especially because of its simplicity and of the relatively short calculation times, but is obviously insufficient to treat deformed nuclei such as actinides. For accurate calculations about these nuclei, it is necessary to use a deformed potential well and solve a set of coupled equations, hence long computational times. The importance of compound nucleus formation at low energy requires also a good knowledge of the statistical model together with that of all the reaction mechanisms which are involved, including fission for which an accurate barrier is necessary and, of course, well-adjusted level densities. The considerations form the background of the Scientific Programme set up by a Programme Committee whose composition is given further on in this book

  6. Electrochemical decontamination system for actinide processing gloveboxes

    International Nuclear Information System (INIS)

    Wedman, D.E.; Lugo, J.L.; Ford, D.K.; Nelson, T.O.; Trujillo, V.L.; Martinez, H.E.

    1998-03-01

    An electrolytic decontamination technology has been developed and successfully demonstrated at Los Alamos National Laboratory (LANL) for the decontamination of actinide processing gloveboxes. The technique decontaminates the interior surfaces of stainless steel gloveboxes utilizing a process similar to electropolishing. The decontamination device is compact and transportable allowing it to be placed entirely within the glovebox line. In this way, decontamination does not require the operator to wear any additional personal protective equipment and there is no need for additional air handling or containment systems. Decontamination prior to glovebox decommissioning reduces the potential for worker exposure and environmental releases during the decommissioning, transport, and size reduction procedures which follow. The goal of this effort is to reduce contamination levels of alpha emitting nuclides for a resultant reduction in waste level category from High Level Transuranic (TRU) to low Specific Activity (LSA, less than or equal 100 nCi/g). This reduction in category results in a 95% reduction in disposal and disposition costs for the decontaminated gloveboxes. The resulting contamination levels following decontamination by this method are generally five orders of magnitude below the LSA specification. Additionally, the sodium sulfate based electrolyte utilized in the process is fully recyclable which results in the minimum of secondary waste. The process bas been implemented on seven gloveboxes within LANL's Plutonium Facility at Technical Area 55. Of these gloveboxes, two have been discarded as low level waste items and the remaining five have been reused

  7. Synthesis of crystalline ceramics for actinide immobilisation

    International Nuclear Information System (INIS)

    Burakov, B.; Gribova, V.; Kitsay, A.; Ojovan, M.; Hyatt, N.C.; Stennett, M.C.

    2007-01-01

    Methods for the synthesis of ceramic wasteforms for the immobilization of actinides are common to those for non-radioactive ceramics: hot uniaxial pressing (HUP); hot isostatic pressing (HIP); cold pressing followed by sintering; melting (for some specific ceramics, such as garnet/perovskite composites). Synthesis of ceramics doped with radionuclides is characterized with some important considerations: all the radionuclides should be incorporated into crystalline structure of durable host-phases in the form of solid solutions and no separate phases of radionuclides should be present in the matrix of final ceramic wasteform; all procedures of starting precursor preparation and ceramic synthesis should follow safety requirements of nuclear industry. Synthesis methods that avoid the use of very high temperatures and pressures and are easily accomplished within the environment of a glove-box or hot cell are preferable. Knowledge transfer between the V. G. Khlopin Radium Institute (KRI, Russia) and Immobilisation Science Laboratory (ISL, UK) was facilitated in the framework of a joint project supported by UK Royal Society. In order to introduce methods of precursor preparation and ceramic synthesis we selected well-known procedures readily deployable in radiochemical processing plants. We accounted that training should include main types of ceramic wasteforms which are currently discussed for industrial applications. (authors)

  8. Carbon potential measurement on some actinide carbides

    International Nuclear Information System (INIS)

    Anthonysamy, S.; Ananthasivan, K.; Kaliappan, I.; Chandramouli, V.; Vasudeva Rao, P.R.; Mathews, C.K.; Jacob, K.T.

    1994-01-01

    Uranium-Plutonium mixed carbides with a Pu/(U+Pu) ratio of 0.55 are to be used as the fuel in the Fast Breeder Test Reactor (FBTR) at Kalpakkam, India. Carburization of the stainless steel clad by this fuel is determined by its carbon potential. Because the carbon potential of this fuel composition is not available in the literature, it was measured by the methane-hydrogen gas equilibration technique. The sample was equilibrated with purified hydrogen and the equilibrium methane-to-hydrogen ratio in the gas phase was measured with a flame ionization detector. The carbon potential of the ThC-ThC 2 as well as Mo-Mo 2 C system, which is an important binary in the actinide-fission product-carbon systems, were also measured by this technique in the temperature range 973 to 1,173 K. The data for the Mo-Mo 2 C system are in agreement with values reported in the literature. The results for the ThC-ThC 2 system are different from estimated values with large uncertainty limits given in the literature. The data on (U, Pu) mixed carbides indicates the possibility of stainless steel clad attack under isothermal equilibrium conditions

  9. Microbial transformations of actinides in the environment

    Energy Technology Data Exchange (ETDEWEB)

    Livens, F R [Centre for Radiochemistry Research, School of Chemistry, University of Manchester, Oxford Road, Manchester M13 9PL (United Kingdom); Al-Bokari, M [Institute of Atomic Energy Research, King Abdulaziz City for Science and Technology, P. O. Box 6086, Riyadh 11442 (Saudi Arabia); Fomina, M; Gadd, G M [College of Life Sciences, University of Dundee, Dundee DD1 5EH (United Kingdom); Geissler, A; Lloyd, J R; Vaughan, D J [School of Earth, Atmospheric and Environmental Sciences, and Williamson Research Centre for Molecular Environmental Science, University of Manchester, Oxford Road, Manchester M13 9PL (United Kingdom); Renshaw, J C, E-mail: francis.livens@manchester.ac.uk [School of Geography, Earth and Environmental Sciences, University of Birmingham, Edgbaston, Birmingham, B15 2TT (United Kingdom)

    2010-03-15

    The diversity of microorganisms is still far from understood, although many examples of the microbial biotransformation of stable, pollutant and radioactive elements, involving Bacteria, Archaea and Fungi, are known. In estuarine sediments from the Irish Sea basin, which have been labelled by low level effluent discharges, there is evidence of an annual cycle in Pu solubility, and microcosm experiments have demonstrated both shifts in the bacterial community and changes in Pu solubility as a result of changes in redox conditions. In the laboratory, redox transformation of both U and Pu by Geobacter sulfurreducens has been demonstrated and EXAFS spectroscopy has been used to understand the inability of G. sufurreducens to reduce Np(V). Fungi promote corrosion of metallic U alloy through production of a range of carboxylic acid metabolites, and are capable of translocating the dissolved U before precipitating it externally to the hyphae, as U(VI) phosphate phases. These examples illustrate the far-reaching but complex effects which microorganisms can have on actinide behaviour.

  10. New Routes to Lanthanide and Actinide Nitrides

    Energy Technology Data Exchange (ETDEWEB)

    Butt, D.P.; Jaques, B.J.; Osterberg, D.D. [Boise State University, 1910 University Dr., Boise, Idaho 83725-2075 (United States); Marx, B.M. [Concurrent Technologies Corporation, Johnstown, PA (United States); Callahan, P.G. [Carnegie Mellon University, Pittsburgh, PA (United States); Hamdy, A.S. [Central Metallurgical R and D Institute, Helwan, Cairo (Egypt)

    2009-06-15

    The future of nuclear energy in the U.S. and its expansion worldwide depends greatly on our ability to reduce the levels of high level waste to minimal levels, while maintaining proliferation resistance. Implicit in the so-called advanced fuel cycle is the need for higher levels of fuel burn-up and consequential use of complex nuclear fuels comprised of fissile materials such as Pu, Am, Np, and Cm. Advanced nitride fuels comprised ternary and quaternary mixtures of uranium and these actinides have been considered for applications in advanced power plants, but there remain many processing challenges as well as necessary qualification testing. In this presentation, the advantages and disadvantages of nitride fuels are discussed. Methods of synthesizing the raw materials and sintering of fuels are described including a discussion of novel, low cost routes to nitrides that have the potential for reducing the cost and footprint of a fuel processing plant. Phase pure nitrides were synthesized via four primary methods; reactive milling metal flakes in nitrogen at room temperature, directly nitriding metal flakes in a pure nitrogen atmosphere, hydriding metal flakes prior to nitridation, and carbo-thermically reducing the metal oxide and carbon mixture prior to nitridation. In the present study, the sintering of UN, DyN, and their solid solutions (U{sub x}, Dy{sub 1-x}) (x = 1 to 0.7) were also studied. (authors)

  11. Criticality and thermal analyses of separated actinides

    International Nuclear Information System (INIS)

    Bakker, E.

    2004-01-01

    Curium and americium pose special problems in the chemical preparation of spent fuel for transmutation. Once separated from the other actinides, the isotopes can lead to nuclear fission with the subsequent release of a large amount of radiation. A neutron criticality code was used to determine k eff for varying quantities of Cm 2 O 3 and Am 2 O 3 held within spherical or cylindrical containers. These geometries were investigated both in air and in water. Recommendations are made on the maximum amount of Cm 2 O 3 and Am 2 O 3 that can be safely stored or handled before encountering criticality. Several isotopes of curium and americium also generate a significant amount of heat by radioactive decay. If kilogram quantities are stored in a container, for example, the material may heat to an equilibrium temperature that exceeds its melting temperature. The heat generation of curium and americium present even more restriction on the mass of that can safely be contained in one location. (author)

  12. High performance separation of lanthanides and actinides

    International Nuclear Information System (INIS)

    Sivaraman, N.; Vasudeva Rao, P.R.

    2011-01-01

    The major advantage of High Performance Liquid Chromatography (HPLC) is its ability to provide rapid and high performance separations. It is evident from Van Deemter curve for particle size versus resolution that packing materials with particle sizes less than 2 μm provide better resolution for high speed separations and resolving complex mixtures compared to 5 μm based supports. In the recent past, chromatographic support material using monolith has been studied extensively at our laboratory. Monolith column consists of single piece of porous, rigid material containing mesopores and micropores, which provide fast analyte mass transfer. Monolith support provides significantly higher separation efficiency than particle-packed columns. A clear advantage of monolith is that it could be operated at higher flow rates but with lower back pressure. Higher operating flow rate results in higher column permeability, which drastically reduces analysis time and provides high separation efficiency. The above developed fast separation methods were applied to assay the lanthanides and actinides from the dissolver solutions of nuclear reactor fuels

  13. variabilite des productions et des revenus des exploitations

    African Journals Online (AJOL)

    3Centre de coopération internationale en recherche agronomique pour le développement (CIRAD), UMR Innovation,. Montpellier, France. Doubangolo COULIBALY, Email kone_b@yahoo.fr. RESUME. La durabilité des systèmes de production à base de coton dans un contexte de variabilité des prix aux producteurs et de ...

  14. Anaerobic Digestion Alters Copper and Zinc Speciation.

    Science.gov (United States)

    Legros, Samuel; Levard, Clément; Marcato-Romain, Claire-Emmanuelle; Guiresse, Maritxu; Doelsch, Emmanuel

    2017-09-19

    Anaerobic digestion is a widely used organic waste treatment process. However, little is known on how it could alter the speciation of contaminants in organic waste. This study was focused on determining the influence of anaerobic digestion on the speciation of copper and zinc, two metals that generally occur at high concentration in organic waste. Copper and zinc speciation was investigated by X-ray absorption spectroscopy in four different raw organic wastes (predigestion) and their digested counterparts (postdigestion, i.e., digestates). The results highlighted an increase in the digestates of the proportion of amorphous or nanostructured copper sulfides as well as amorphous or nanostructured zinc sulfides and zinc phosphate as compared to raw waste. We therefore suggest that the environmental fate of these elements would be different when spreading either digestates or raw waste on cropland.

  15. Loss of speciation rate will impoverish future diversity

    OpenAIRE

    Rosenzweig, Michael L.

    2001-01-01

    Human activities have greatly reduced the amount of the earth's area available to wild species. As the area they have left declines, so will their rates of speciation. This loss of speciation will occur for two reasons: species with larger geographical ranges speciate faster; and loss of area drives up extinction rates, thus reducing the number of species available for speciation. Theory predicts steady states in species diversity, and fossils suggest that these have t...

  16. Redox speciation of final repository relevant elements using separation methods in combination with ICP mass spectrometry

    International Nuclear Information System (INIS)

    Graser, Carl-Heinrich

    2015-01-01

    The long-term safety assessment for nuclear waste repositories requires a detailed understanding of the chemistry of actinide elements in the geosphere. The development of advanced analytical tools is required to gain detailed insights into actinide redox speciation in a given system. The mobility of radionuclides is mostly determined by the geochemical conditions which control the redox state of radionuclides. Besides the longlived radionuclides plutonium (Pu) and neptunium (Np), which are key elements in high level nuclear waste, iron (Fe) represents a main component in natural systems controlling redox related geochemical processes. Analytical techniques for determining oxidation state distribution for redox sensitive radionuclides and other metal ions often have a lack of sensitivity. The detection limits of these methods (i.e. UV/vis, TRLFS, XANES) are in general in the range of ≥ 10 -6 mol.L -1 . As a consequence ultrasensitive new analytical techniques are required. Capillary electrophoresis (CE) and ion chromatography (IC) are powerful separation methods for metal ions. In the course of this thesis different speciation method for iron, neptunium and plutonium were optimized. With the optimized setup redox speciation analysis of these elements in different samples were done. Furthermore CE hyphenated to inductively coupled plasma sector field mass spectrometry (CE - ICP - SF - MS) was used to measure the redox speciation of Pu (III, IV, V, VI), Np (IV, V, VI) and Fe (II, III) at concentrations lower than 10 -7 mol.L -1 . CE coupling and separation parameters such as sample gas pressure, make up flow rate, capillary position, auxiliary gas flow, as well as the electrolyte system were optimized to obtain the maximum sensitivity. The methodes detection limits are 10 -12 mol.L -1 for Np and Pu. The various oxidation state species of Pu and Np in different samples were separated by application of an acetate based electrolyte system. The separation of Fe (II

  17. Partitioning of minor actinides: research at Juelich and Karlsruhe Research Centres

    International Nuclear Information System (INIS)

    Geist, A.; Weigl, M.; Gompper, K.; Modolo, G.

    2007-01-01

    Full text of publication follows. The work on minor actinide (MA) partitioning carried out at Karlsruhe and Juelich is integrated in the EC FP6 programme, EUROPART. Studies include the DIAMEX process (co-extraction of MA and lanthanides from PUREX raffinate) and the SANEX process (separation of MA from lanthanides). Aspects ranging from developing and improving highly selective and efficient extraction reagents, to fundamental structural studies, to process development and testing are covered. SANEX is a challenge in separation chemistry because of the chemical similarity of trivalent actinides and lanthanides. The extracting agents 2,6-di(5,6-di-propyl-1,2,4-triazine-3-yl)pyridine (n-Pr-BTP), developed at Karlsruhe, and the synergetic mixture of di(chloro-phenyl)di-thio-phosphinic acid (R2PSSH) with tri-n-octyl-phosphine oxide (TOPO), developed at Juelich, are considered a breakthrough because of their high separation efficiency in acidic systems. Separation factors for americium over lanthanides of more than 30 (R2PSSH+TOPO) and 130 (n-Pr-BTP) are achieved. To gain understanding of these selectivities, comparative investigations on the structures of curium and europium complexed with these SANEX ligands were performed at Karlsruhe. Extended X-ray absorption fine structure (EXAFS) analysis revealed distinct structural differences between curium and europium complexed with R2PSSH + TOPO, though no such differences were found for n-Pr-BTP. These investigations were therefore complemented by time-resolved laser fluorescence spectroscopic investigations (TRLFS), showing complex stabilities and speciation to differ between n-Pr-BTP complexes of curium and europium. Kinetics of mass transfer was studied for both R2PSSH+TOPO and n-Pr-BTP systems. For the R2PSSH + TOPO system, diffusion was identified to control extraction rates. For the n-Pr-BTP system, a slow chemical reaction was identified as the rate-controlling process. These results were implemented into computer

  18. The development of chemical speciation analysis

    International Nuclear Information System (INIS)

    Martin, R.; Santana, J.L.; Lima, L.; De La Rosa, D.; Melchor, K.

    2003-01-01

    The knowledge of many metals species on the environmental, its bioaccumulation, quantification and its effect in human body has been studied by a wide researchers groups in the last two decades. The development of speciation analysis has an vertiginous advance close to the developing of novel analytical techniques. Separation and quantification at low level is a problem that's has been afford by a coupling of high resolution chromatographic techniques like HPLC and HRGC with a specific method of detection (ICP-MS or CV-AAS). This methodological approach make possible the success in chemical speciation nowadays

  19. Incidence and Speciation of Candida Species among Non-gravid ...

    African Journals Online (AJOL)

    This study investigated the incidence and speciation of Candida species among non-gravid young females, using commercially available chromogenic Candida speciation media (CHROM agar) for the identification/speciation of medically important yeast and yeastlike organisms in a routine clinical mycology laboratory.

  20. EPAs SPECIATE 4.4 Database: Development and Uses

    Science.gov (United States)

    SPECIATE is the U.S. Environmental Protection Agency’s (EPA) repository of source category-specific particulate matter (PM), volatile organic gas, and other gas speciation profiles of air pollutant emissions. Abt Associates, Inc. developed SPECIATE 4.4 through a collaborat...

  1. 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

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

    Science.gov (United States)

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

    2015-08-18

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

  3. Elimination of waste actinides by recycling them to nuclear reactors

    International Nuclear Information System (INIS)

    McKay, H.A.C.

    1981-01-01

    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 decayed to insignificant levels, leaving the actinides as the principal hazardous species remaining. It is therefore at first sight an attractive idea to recycle the actinides in nuclear reactors, so as to eliminate them by nuclear fission. There are good reasons for examining the idea in detail, and studies have been carried out in a number of countries. These have culminated recently in international conferences at the European Joint Research Centre at Ispra in Italy and at Austin, Texas in the USA as well as in the issue of an IAEA Technical Report entitled An Evaluation of Actinide Partitioning and Transmutation, a product of a four-year IAEA Co-ordinated Research Programme, on which the present article is based. The term partitioning refers to the separation of the actinides from nuclear fuel cycle wastes, a necessary preliminary step to their introduction into reactors for transmutation by nuclear fission. The complete scheme will be referred to as P-T, i.e. partitioning-transmutation

  4. The actinides-a beautiful ending of the Periodic Table

    International Nuclear Information System (INIS)

    Johansson, Boerje; Li, Sa

    2007-01-01

    The 5f elements, actinides, show many properties which have direct correspondence to the 4f transition metals, the lanthanides. The remarkable similarity between the solid state properties of compressed Ce and the actinide metals is pointed out in the present paper. The α-γ transition in Ce is considered as a Mott transition, namely, from delocalized to localized 4f states. An analogous behavior is also found for the actinide series, where the sudden volume increase from Pu to Am can be viewed upon as a Mott transition within the 5f shell as a function of the atomic number Z. On the itinerant side of the Mott transition, the earlier actinides (Pa-Pu) show low symmetry structures at ambient conditions; while across the border, the heavier elements (Am-Cf) present the dhcp structure, an atomic arrangement typical for the trivalent lanthanide elements with localized 4f magnetic moments. The reason for an isostructural Mott transition of the f electron in Ce, as opposed to the much more complicated cases in the actinides, is identified. The strange appearance of the δ-phase (fcc) in the phase diagram of Pu is another consequence of the border line behavior of the 5f electrons. The path leading from δ-Pu to α-Pu is identified

  5. Hydrophilic actinide complexation studied by solvent extraction radiotracer technique

    Energy Technology Data Exchange (ETDEWEB)

    Rydberg, J [Chalmers Univ. of Technology, Goeteborg (Sweden). Dept. of Nuclear Chemistry and Radiochemistry Consultant Group, Vaestra Froelunda (Sweden)

    1996-10-01

    Actinide migration in the ground water is enhanced by the formation of water soluble complexes. It is essential to the risk analysis of a wet repository to know the concentration of central atoms and the ligands in the ground water, and the stability of complexes formed between them. Because the chemical behavior at trace concentrations often differ from that at macro concentrations, it is important to know the chemical behavior of actinides at trace concentrations in ground water. One method used for such investigations is the solvent extraction radiotracer (SXRT) technique. This report describes the SXRT technique in some detail. A particular reason for this analysis is the claim that complex formation constants obtained by SXRT are less reliable than results obtained by other techniques. It is true that several difficulties are encountered in the application of SXRT technique to actinide solution, such as redox instability, hydrophilic complexation by side reactions and sorption, but it is also shown that a careful application of the SXRT technique yields results as reliable as by any other technique. The report contains a literature survey on solvent extraction studies of actinide complexes formed in aqueous solutions, particularly by using the organic reagent thenoyltrifluoroacetone (TTA) dissolved in benzene or chloroform. Hydrolysis constants obtained by solvent extraction are listed as well as all actinide complexes studied by SX with inorganic and organic ligands. 116 refs, 11 tabs.

  6. Hydrophilic actinide complexation studied by solvent extraction radiotracer technique

    International Nuclear Information System (INIS)

    Rydberg, J.

    1996-10-01

    Actinide migration in the ground water is enhanced by the formation of water soluble complexes. It is essential to the risk analysis of a wet repository to know the concentration of central atoms and the ligands in the ground water, and the stability of complexes formed between them. Because the chemical behavior at trace concentrations often differ from that at macro concentrations, it is important to know the chemical behavior of actinides at trace concentrations in ground water. One method used for such investigations is the solvent extraction radiotracer (SXRT) technique. This report describes the SXRT technique in some detail. A particular reason for this analysis is the claim that complex formation constants obtained by SXRT are less reliable than results obtained by other techniques. It is true that several difficulties are encountered in the application of SXRT technique to actinide solution, such as redox instability, hydrophilic complexation by side reactions and sorption, but it is also shown that a careful application of the SXRT technique yields results as reliable as by any other technique. The report contains a literature survey on solvent extraction studies of actinide complexes formed in aqueous solutions, particularly by using the organic reagent thenoyltrifluoroacetone (TTA) dissolved in benzene or chloroform. Hydrolysis constants obtained by solvent extraction are listed as well as all actinide complexes studied by SX with inorganic and organic ligands. 116 refs, 11 tabs

  7. Actinide partitioning-transmutation program final report. III. Transmutation studies

    International Nuclear Information System (INIS)

    Wachter, J.W.; Croff, A.G.

    1980-07-01

    Transmutation of the long-lived nuclides contained in fuel cycle wastes has been suggested as a means of reducing the long-term toxicity of the wastes. A comprehensive program to evaluate the feasibility and incentives for recovering the actinides from wastes (partitioning) and transmuting them to short-lived or stable nuclides has been in progress for 3 years under the direction of Oak Ridge National Laboratory (ORNL). This report constitutes the final assessment of transmutation in support of this program. Included are (1) a summary of recent transmutation literature, (2) a generic evaluation of actinide transmutation in thermal, fast, and other transmutation devices, (3) a preliminary evaluation of 99 Tc and 129 I transmutation, and (4) a characterization of a pressurized-water-reactor fuel cycle with and without provisions for actinide recovery and transmutation for use in other parts of the ORNL program. The principal conclusion of the report is that actinide transmutation is feasible in both thermal and fast reactors, subject to demonstrating satisfactory fuel performance, with relatively little impact on the reactor. It would also appear that additional transmutation studies are unwarranted until a firm decision to proceed with actinide transmutation has been made by the responsible authorities

  8. Potential radiation dose from eating fish exposed to actinide contamination

    International Nuclear Information System (INIS)

    Emery, R.M.; Klopfer, D.C.; Baker, D.A.; Soldat, J.K.

    1980-01-01

    The purpose of this work is to establish a maximum potential for transporting actinides to man via fish consumption. The study took place in U-Pond, a nuclear waste pond on the Hanford Site. It has concentrations of 238 U, 238 Pu, /sup 239,240/Pu and 241 Am that are approximately three orders of magnitude greater than background levels. Fish living in the pond contain higher actinide concentrations than those observed in fish from any other location. Experiments were performed in U-pond to determine maximum quantities of actinides that could accumulate in fillets and whole bodies of two centrarchid fish species. Doses to hypothetical consumers were then estimated by assuming that actinide behavior in their bodies was similar to that defined for Standard Man by the International Commission on Radiological Protection. Results indicate that highest concentrations occurring in bluegill or bass muscle after more than a year's exposure to the pond would not be sufficient to produce a significant radiation dose to a human consumer, even if he ate 0.5 kg (∼1 lb) of these fillets every day for 70 years. Natural predators (heron or coyote), having lifetime diets of whole fish from U-Pond, would receive less radiation dose from the ingested actinides than from natural background sources. 34 refs., 5 figs., 4 tabs

  9. 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

  10. Formation of actinides in irradiated HTGR fuel elements

    International Nuclear Information System (INIS)

    Santos, A.M. dos.

    1976-03-01

    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 actinide isolation were tested with highly irradiated ThO 2 . Separation and decontamination factors are presented. Actinide nuclide formation can be described by exponential functions of the type ln msub(nuclide) = A + B x % fifa. The empirical factors A and B were calculated performing a least squares analysis. Build-up of 232 U was discussed. According to the experimental results, 232 U is mainly produced from 230 Th, a certain amount (e.g. about 20% at a 10 5 MWd/t burnup) originated from a (n,2n) reaction of 233 U; a formation from 233 Th by a (n,2n) followed by a (n,γ) reaction was not observed. The AVR breeding rate was ascertained to be 0.5. The hazard potential of high activity waste was calculated. After a 1,000 years' storage time, the elements Pa, Am and Cm will no longer influence the total hazard index. Actinide recovery factors were proposed in order to reduce the hazard potential of the waste by an actinide removal in consideration of the reprocessing technology which is available presently. (orig.) [de

  11. A Summary of Actinide Enrichment Technologies and Capability Gaps

    Energy Technology Data Exchange (ETDEWEB)

    Patton, Bradley D. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Robinson, Sharon M. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2017-01-01

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

  12. 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

  13. The prediction of minor actinides amounts accumulated in the spent fuel in China

    International Nuclear Information System (INIS)

    Zhou Peide

    2000-01-01

    The amounts of the Minor Actinides accumulated in the spent fuel are predicted according to the Nuclear Power Plant development plan envisaged in China. The Minor Actinides generated in the spent fuel unloaded from a typical PWR per year are calculated. The decay characteristics of the Minor Actinides during storage and cooling period are also calculated. At last, the Minor Actinides amounts accumulated in all spent fuel which were unloaded before sometime are given

  14. Fission theory and actinide fission data

    Energy Technology Data Exchange (ETDEWEB)

    Michaudon, A.

    1975-06-01

    The understanding of the fission process has made great progress recently, as a result of the calculation of fission barriers, using the Strutinsky prescription. Double-humped shapes were obtained for nuclei in the actinide region. Such shapes could explain, in a coherent manner, many different phenomena: fission isomers, structure in near-threshold fission cross sections, intermediate structure in subthreshold fission cross sections and anisotropy in the emission of the fission fragments. A brief review of fission barrier calculations and relevant experimental data is presented. Calculations of fission cross sections, using double-humped barrier shapes and fission channel properties, as obtained from the data discussed previously, are given for some U and Pu isotopes. The fission channel theory of A. Bohr has greatly influenced the study of low-energy fission. However, recent investigation of the yields of prompt neutrons and γ rays emitted in the resonances of {sup 235}U and {sup 239}Pu, together with the spin determination for many resonances of these two nuclei cannot be explained purely in terms of the Bohr theory. Variation in the prompt neutron and γ-ray yields from resonance to resonance does not seem to be due to such fission channels, as was thought previously, but to the effect of the (n,γf) reaction. The number of prompt fission neutrons and the kinetic energy of the fission fragments are affected by the energy balance and damping or viscosity effects in the last stage of the fission process, from saddle point to scission. These effects are discussed for some nuclei, especially for {sup 240}Pu.

  15. Actinide consumption: Nuclear resource conservation without breeding

    Energy Technology Data Exchange (ETDEWEB)

    Hannum, W.H.; Battles, J.E.; Johnson, T.R.; McPheeters, C.C.

    1991-01-01

    A new approach to the nuclear power issue based on a metallic fast reactor fuel and pyrometallurgical processing of spent fuel is showing great potential and is approaching a critical demonstration phase. If successful, this approach will complement and validate the LWR reactor systems and the attendant infrastructure (including repository development) and will alleviate the dominant concerns over the acceptability of nuclear power. The Integral Fast Reactor (IFR) concept is a metal-fueled, sodium-cooled pool-type fast reactor supported by a pyrometallurgical reprocessing system. The concept of a sodium cooled fast reactor is broadly demonstrated by the EBR-II and FFTF in the US; DFR and PFR in the UK; Phenix and SuperPhenix in France; BOR-60, BN-350, BN-600 in the USSR; and JOYO in Japan. The metallic fuel is an evolution from early EBR-II fuels. This fuel, a ternary U-Pu-Zr alloy, has been demonstrated to be highly reliable and fault tolerant even at very high burnup (160-180,000 MWd/MT). The fuel, coupled with the pool type reactor configuration, has been shown to have outstanding safety characteristics: even with all active safety systems disabled, such a reactor can survive a loss of coolant flow, a loss of heat sink, or other major accidents. Design studies based on a small modular approach show not only its impressive safety characteristics, but are projected to be economically competitive. The program to explore the feasibility of actinide recovery from spent LWR fuel is in its initial phase, but it is expected that technical feasibility could be demonstrated by about 1995; DOE has not yet committed funds to achieve this objective. 27 refs.

  16. Theoretical modelling of actinide spectra in solution

    International Nuclear Information System (INIS)

    Danilo, Cecile

    2009-01-01

    The framework of this PhD is the interpretation of Nuclear Magnetic Relaxation Dispersion experiments performed on solvated U"4"+, NpO_2"+ and PuO_2"2"+, which all have a f"2 configuration. Unexpectedly the two actinyl ions have a much higher relaxivity than U"4"+,. One possible explanation is that the electronic relaxation rate is faster for Uranium(IV) than for the actinyl ions. We address this problem by exploring the electronic spectrum of the three compounds in gas phase and in solution with a two-step SOCI (Spin-Orbit Configuration-Interaction) method. The influence of electron correlation (treated in the first step) and spin-orbit relaxation effects (considered in the second step) has been discussed thoroughly. Solvent effects have been investigated as well. Another issue that has been questioned is the accuracy of Density Functional Theory for the study of actinide species. This matter has been discussed by comparing its performance to wave-function based correlated methods. The chemical problem chosen was the water exchange in [UO_2"2"+ (H_2O)_5]. We looked at the associative and at the dissociative mechanisms using a model with one additional water in the second hydration sphere. The last part of the thesis dealt with the spectroscopy of coordinated Uranyl(V). Absorption spectrum of Uranyl(V) with various ligands has been recorded. The first sharp absorption bands in the Near-Infrared region were assigned to the Uranium centered 5f-5f transitions, but uncertainties remained for the assignment of transitions observed in the Visible region. We computed the spectra of naked UO_2"+ and [UO_2(CO_3)_3]"5"- to elucidate the spectral changes induced by the carbonate ligands. (author) [fr

  17. Actinide consumption: Nuclear resource conservation without breeding

    International Nuclear Information System (INIS)

    Hannum, W.H.; Battles, J.E.; Johnson, T.R.; McPheeters, C.C.

    1991-01-01

    A new approach to the nuclear power issue based on a metallic fast reactor fuel and pyrometallurgical processing of spent fuel is showing great potential and is approaching a critical demonstration phase. If successful, this approach will complement and validate the LWR reactor systems and the attendant infrastructure (including repository development) and will alleviate the dominant concerns over the acceptability of nuclear power. The Integral Fast Reactor (IFR) concept is a metal-fueled, sodium-cooled pool-type fast reactor supported by a pyrometallurgical reprocessing system. The concept of a sodium cooled fast reactor is broadly demonstrated by the EBR-II and FFTF in the US; DFR and PFR in the UK; Phenix and SuperPhenix in France; BOR-60, BN-350, BN-600 in the USSR; and JOYO in Japan. The metallic fuel is an evolution from early EBR-II fuels. This fuel, a ternary U-Pu-Zr alloy, has been demonstrated to be highly reliable and fault tolerant even at very high burnup (160-180,000 MWd/MT). The fuel, coupled with the pool type reactor configuration, has been shown to have outstanding safety characteristics: even with all active safety systems disabled, such a reactor can survive a loss of coolant flow, a loss of heat sink, or other major accidents. Design studies based on a small modular approach show not only its impressive safety characteristics, but are projected to be economically competitive. The program to explore the feasibility of actinide recovery from spent LWR fuel is in its initial phase, but it is expected that technical feasibility could be demonstrated by about 1995; DOE has not yet committed funds to achieve this objective. 27 refs

  18. 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

  19. Civili, langue des Baloango

    DEFF Research Database (Denmark)

    Mavoungou, Paul Achille; Ndinga-Koumba-Binza, Hugues Steve

    , Congo, Angola, etc.) issus de la décolonisation. Il présente de façon succincte quelques phénomènes historiques, phonologiques, morphosyntaxiques, homonymiques et analogiques de la langue. Des faits sémantiques des emprunts linguistiques y sont également décrits dans le cadre des changements...

  20. The Lawrence Livermore National Laboratory Intelligent Actinide Analysis System

    International Nuclear Information System (INIS)

    Buckley, W.M.; Carlson, J.B.; Koenig, Z.M.

    1993-07-01

    The authors have developed an Intelligent Actinide Analysis System (IAAS) for Materials Management to use in the Plutonium Facility at the Lawrence Livermore National Laboratory. The IAAS will measure isotopic ratios for plutonium and other actinides non-destructively by high-resolution gamma-ray spectrometry. This system will measure samples in a variety of matrices and containers. It will provide automated control of many aspects of the instrument that previously required manual intervention and/or control. The IAAS is a second-generation instrument, based on the authors' experience in fielding gamma isotopic systems, that is intended to advance non-destructive actinide analysis for nuclear safeguards in performance, automation, ease of use, adaptability, systems integration and extensibility to robotics. It uses a client-server distributed monitoring and control architecture. The IAAS uses MGA 3 as the isotopic analysis code. The design of the IAAS reduces the need for operator intervention, operator training, and operator exposure