WorldWideScience

Sample records for actinide sesquioxide thermochemistry

  1. Thermochemistry of the alkali metal and alkaline earth-actinide complex oxides

    International Nuclear Information System (INIS)

    Fuger, J.

    1985-01-01

    After a brief discussion of the various techniques used for the preparation of actinide complex oxides, the present status of the thermochemistry of these compounds is reviewed. Perovskite-related compounds are especially considered as thermodynamic data are available for compounds of several actinides and/or several alkali and alkaline earth metals. The stabilities of the complex oxides are discussed with respect to the parent binary oxides and to the aqueous ions; trends as a function of the size and the alkali or the alkaline earth cation are presented. Suggestions for synthesis of some analogous compounds with heavier actinides are also discussed. (orig./RK)

  2. Physical properties of europium sesquioxide

    International Nuclear Information System (INIS)

    Gilchrist, K.E.; Brown, R.G.; Preston, S.D.

    1977-01-01

    Europium sesquioxide (Eu 2 O 3 ) is a neutron-absorbing material of potential use in reactor control rods and is being evaluated for use in fast reactors. This paper presents the results of physical and mechanical property measurements performed on unirradiated europia. The material exists in two useful crystallographic forms. Both the monoclinic form and a cubic variety, stabilized by the addition of 17 wt% molybdenum trioxide (MoO 3 ), have been examined. The properties reported are density, specific heat, thermal diffusivity and conductivity, thermal expansivity, Young's modulus, and strength. The data are compared with similar information in the literature. (Auth.)

  3. Actinide Sciences at ITN - Basic Studies in Chemistry with Potential Interest for Partitioning, Fuel Fabrication and More

    International Nuclear Information System (INIS)

    Almeida, M.; Dias, M.; Goncalves, A.P.; Henriques, M.S.; Lopes, E.B.; Pereira, L.C.J.; Santos, I.C.; Verbovytskyy, Y.; Waerenborgh, J.C.; Branco, J.B.; Carretas, J.M.; Cruz, A.; Ferreira, A.C.; Gasche, T.A.; Leal, J.P.; Lopes, G.; Lourenco, C.; Marcalo, J.; Maria, L.; Monteiro, B.; Mora, E.; Pereira, C.C.L.; Paiva, I.

    2010-01-01

    The current activities in the area of actinide chemistry at ITN, comprising basic research studies in inorganic and organometallic chemistry, catalysis, gas-phase ion chemistry, thermochemistry, and solid state chemistry, are briefly described. Actinide (and lanthanide) chemistry studies at ITN will be pursued connecting basic research with potential applications in nuclear and non-nuclear areas. (authors)

  4. Synthesis and Evaluation of Novel Organogermanium Sesquioxides As Antitumor Agents

    OpenAIRE

    Zhang, Chun Li; Li, Tai Hua; Niu, Shuang Huan; Wang, Rong Fu; Fu, Zhan Li; Guo, Feng Qin; Yang, Ming

    2009-01-01

    Five new organogermanium sesquioxides have been synthesized and characterized by elemental analysis and IR spectra. All the compounds were tested for antitumor activities against KB, HCT, and Bel cells in vitro. Compound 5 ( -thiocarbamido propyl germanium sesquioxide) showed excellent antitumor activity, and its inhibition yield to KB, HCT, and Bel cells was 92.9%, 84.9%, and 70.9%, respectively. A rapid method was described for the labeling compound 5 with 9 9 m T c , and the optimum labe...

  5. 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

  6. 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.

  7. Preparation of higher-actinide burnup and cross section samples

    International Nuclear Information System (INIS)

    Adair, H.L.; Kobisk, E.H.; Quinby, T.C.; Thomas, D.K.; Dailey, J.M.

    1981-01-01

    A joint research program involving the United States and the United Kingdom was instigated about four years ago for the purpose of studying burnup of higher actinides using in-core irradiation in the fast reactor at Dounreay, Scotland. Simultaneously, determination of cross sections of a wide variety of higher actinide isotopes was proposed. Coincidental neutron flux and energy spectral measurements were to be made using vanadium encapsulated dosimetry materials in the immediate region of the burnup and cross section samples. The higher actinide samples chosen for the burnup study were 241 Am and 244 Cm in the forms of Am 2 O 3 , Cm 2 O 3 , and Am 6 Cm(RE) 7 O 21 , where (RE) represents a mixture of lanthanide sesquioxides. It is the purpose of this paper to describe technology development and its application in the preparation of the fuel specimens and the cross section specimens that are being used in this cooperative program

  8. Self-irradiation and oxidation effects on americium sesquioxide and Raman spectroscopy studies of americium oxides

    Energy Technology Data Exchange (ETDEWEB)

    Horlait, Denis [CEA, DEN, DTEC/SDTC/LEMA, F-30207 Bagnols-sur-Cèze Cedex (France); Caraballo, Richard [CEA, DEN, DTCD/SECM/LMPA, F-30207 Bagnols-sur-Cèze Cedex (France); Lebreton, Florent [CEA, DEN, DTEC/SDTC/LEMA, F-30207 Bagnols-sur-Cèze Cedex (France); Jégou, Christophe [CEA, DEN, DTCD/SECM/LMPA, F-30207 Bagnols-sur-Cèze Cedex (France); Roussel, Pascal [Unité de Catalyse et Chimie du Solide, UMR 8012 CNRS, Ecole Nationale Supérieure de Chimie de Lille BP 90108, 59652 Villeneuve d’Ascq Cedex (France); Delahaye, Thibaud, E-mail: thibaud.delahaye@cea.fr [CEA, DEN, DTEC/SDTC/LEMA, F-30207 Bagnols-sur-Cèze Cedex (France)

    2014-09-15

    Americium oxides samples were characterized by X-ray diffraction (XRD) and Raman spectroscopy, with an emphasis on their structural behavior under oxidation and self-irradiation. Raman spectra of americium dioxide (AmO{sub 2}) and sesquioxide (Am{sub 2}O{sub 3}) were obtained for the first time. With the help of literature data on isostructural oxides, Raman signatures of Ia-3 C-type Am{sub 2}O{sub 3} and P-3m1 A-type Am{sub 2}O{sub 3} are identified. For AmO{sub 2,} a clear band is noted at 390 cm{sup −1}. Its nature is compared to that of the other actinide dioxides. Am{sub 2}O{sub 3} evolution under ambient conditions and against {sup 241}Am α self-irradiation was monitored by powder XRD. The sample, initially composed of A-type Am{sub 2}O{sub 3} as major phase as well as C2/m B-type and C-type structures as minor phases, progressively oxidizes to Fm-3m AmO{sub 2−δ} over a few months. On the basis of diffractogram refinements, evolutions of unit cell volumes caused by self-irradiation are also determined and discussed. - Graphical abstract: The evolution of americium oxide under ambient conditions was monitored using XRD (X-ray diffraction) and Raman spectroscopy. After a thermal treatment under reducing conditions, a polyphasic sample mainly composed of A- and C-type americium sesquioxides is evidenced by XRD and Raman spectroscopy. The sample then evolves through two processes: oxidation and self-irradiation. The first one provokes the progressive appearance of F-type americium dioxide while the initial phases disappear, whereas the main effect of the second is a structural swelling with time. - Highlights: • The first Raman spectroscopy measurements on americium oxides were performed. • Observed Am{sub 2}O{sub 3} Raman bands were identified thanks to data on analogue compounds. • AmO{sub 2} assumed T{sub 2g} band presents a shift compared to the actinide dioxide series. • Am{sub 2}O{sub 3} evolution under self-irradiation and oxidation was also

  9. Pure and doped vanadium sesquioxide: A brief experimental review

    Energy Technology Data Exchange (ETDEWEB)

    Yethiraj, M. (Los Alamos National Lab., NM (USA))

    1990-09-01

    Vanadium sesquioxide (V{sub 2}O{sub 3}) undergoes a number of phase transitions as a function of temperature and doping. These phase transformations have been studied extensively using numerous experimental techniques. In this article, the author attempts to briefly review the experimental data on the pure and doped V{sub 2}O{sub 3} system.

  10. Pure and doped vanadium sesquioxide: A brief experimental review

    Science.gov (United States)

    Yethiraj, Mohana

    1990-09-01

    Vanadium sesquioxide (V 2O 3) undergoes a number of phase transitions as a function of temperature and doping. These phase transformations have been studied extensively using numerous experimental techniques. In this article, I shall attempt to briefly review the experimental data on the pure and doped V 2O 3 system.

  11. 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

  12. Multi-orbital Effects in Optical Properties of Vanadium Sesquioxide

    OpenAIRE

    Tomczak, Jan M.; Biermann, Silke

    2008-01-01

    Vanadium sesquioxide, V2O3, boasts a rich phase diagram whose description necessitates the accounting for many-body Coulomb correlations. Spectral properties of this compound have been successfully addressed within dynamical mean field theory to an extent that results of recent angle resolved photoemission experiments have been correctly predicted. While photoemission spectroscopy probes the occupied part of the one-particle spectrum, optical experiments measure transitions into empty states ...

  13. 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)

  14. Synthesis and evaluation of novel organogermanium sesquioxides as antitumor agents.

    Science.gov (United States)

    Zhang, Chun Li; Li, Tai Hua; Niu, Shuang Huan; Wang, Rong Fu; Fu, Zhan Li; Guo, Feng Qin; Yang, Ming

    2009-01-01

    Five new organogermanium sesquioxides have been synthesized and characterized by elemental analysis and IR spectra. All the compounds were tested for antitumor activities against KB, HCT, and Bel cells in vitro. Compound 5 (gamma-thiocarbamido propyl germanium sesquioxide) showed excellent antitumor activity, and its inhibition yield to KB, HCT, and Bel cells was 92.9%, 84.9%, and 70.9%, respectively. A rapid method was described for the labeling compound 5 with (99m)Tc, and the optimum labeling conditions were investigated. The labeling yield is above 90% in pH 7.0, 20 degrees C, reaction time greater than 10 minutes, 1 mg of compound 5, and 0.075 approximately 0.1 mg of SnCl(2). The biodistribution of (99m)Tc labeled compound 5 in nude mice bearing human colonic xenografts was studied. The result showed that the tumor uptakes were 0.73, 0.97, 0.87, and 0.62 ID%/g at 1-hour, 3-hour, 6-hour, and 20-hour postinjection, respectively. T/NT (the uptake ratio for per gram of tumor over normal tissues) was 18.3 for tumor versus brain and 5.81 for tumor versus muscle at 20-hour postinjection. The tumor clearance was slow. The results showed that compound 5 may be developed to be a suitable cancer therapeutic agent.

  15. 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

  16. Gas-phase energies of actinide oxides -- an assessment of neutral and cationic monoxides and dioxides from thorium to curium

    Energy Technology Data Exchange (ETDEWEB)

    Marcalo, Joaquim; Gibson, John K.

    2009-08-10

    An assessment of the gas-phase energetics of neutral and singly and doubly charged cationic actinide monoxides and dioxides of thorium, protactinium, uranium, neptunium, plutonium, americium, and curium is presented. A consistent set of metal-oxygen bond dissociation enthalpies, ionization energies, and enthalpies of formation, including new or revised values, is proposed, mainly based on recent experimental data and on correlations with the electronic energetics of the atoms or cations and with condensed-phase thermochemistry.

  17. Gas-Phase Energetics of Actinide Oxides: An Assessment of Neutral and Cationic Monoxides and Dioxides from Thorium to Curium

    Science.gov (United States)

    Marçalo, Joaquim; Gibson, John K.

    2009-09-01

    An assessment of the gas-phase energetics of neutral and singly and doubly charged cationic actinide monoxides and dioxides of thorium, protactinium, uranium, neptunium, plutonium, americium, and curium is presented. A consistent set of metal-oxygen bond dissociation enthalpies, ionization energies, and enthalpies of formation, including new or revised values, is proposed, mainly based on recent experimental data and on correlations with the electronic energetics of the atoms or cations and with condensed-phase thermochemistry.

  18. Hyperfine interactions in 111Cd-doped lutetium sesquioxide

    International Nuclear Information System (INIS)

    Errico, L.A.; Renteria, M.; Bibiloni, A.G.; Requejo, F.G.

    1999-01-01

    We report here first Perturbed Angular Correlation (PAC) results of the electric field gradient (EFG) characterisation at 111 Cd impurities located at both non-equivalent cation sites of the bixbyite structure of Lutetium sesquioxide, between room temperature (RT) and 1273 K. The comparison with results coming from a systematic 111 Cd PAC study in bixbyites and with point-charge model (PCM) predictions shows the presence of a trapped defect at RT in the neighbourhood of the asymmetric cation site, which is completely removed at T > 623 K. The anomalous EFG temperature dependence in Lu 2 O 3 can be described in the frame of a 'two-state' model with fluctuating interactions, which enables the experimental determination of the acceptor energy level introduced by the Cd impurity in the band-gap of the semiconductor and the estimation of the oxygen vacancy density in the sample

  19. Hyperfine interactions in {sup 111}Cd-doped lutetium sesquioxide

    Energy Technology Data Exchange (ETDEWEB)

    Errico, L.A.; Renteria, M.; Bibiloni, A.G.; Requejo, F.G. [Universidad Nacional de La Plata, Programa TENAES (CONICET), Departamento de Fisica, Facultad de Ciencias Exactas (Argentina)

    1999-09-15

    We report here first Perturbed Angular Correlation (PAC) results of the electric field gradient (EFG) characterisation at {sup 111}Cd impurities located at both non-equivalent cation sites of the bixbyite structure of Lutetium sesquioxide, between room temperature (RT) and 1273 K. The comparison with results coming from a systematic {sup 111}Cd PAC study in bixbyites and with point-charge model (PCM) predictions shows the presence of a trapped defect at RT in the neighbourhood of the asymmetric cation site, which is completely removed at T > 623 K. The anomalous EFG temperature dependence in Lu{sub 2}O{sub 3} can be described in the frame of a 'two-state' model with fluctuating interactions, which enables the experimental determination of the acceptor energy level introduced by the Cd impurity in the band-gap of the semiconductor and the estimation of the oxygen vacancy density in the sample.

  20. Multi-orbital effects in optical properties of vanadium sesquioxide

    Energy Technology Data Exchange (ETDEWEB)

    Tomczak, Jan M [Research Institute for Computational Sciences, AIST, Tsukuba 305-8568 (Japan); Biermann, Silke [Japan Science and Technology Agency, CREST (Japan)], E-mail: jan.tomczak@polytechnique.edu

    2009-02-11

    Vanadium sesquioxide, V{sub 2}O{sub 3}, boasts a rich phase diagram whose description necessitates accounting for many-body Coulomb correlations. The spectral properties of this compound have been successfully addressed within dynamical mean field theory to the extent that results of recent angle-resolved photoemission experiments have been correctly predicted. While photoemission spectroscopy probes the occupied part of the one-particle spectrum, optical experiments measure transitions into empty states and thus provide complementary information. In this work, we focus on the optical properties of V{sub 2}O{sub 3} in its paramagnetic phases by employing our recently developed 'generalized Peierls approach'. We obtain results in overall satisfactory agreement with experiments. Further, we rationalize that the experimentally observed temperature dependence stems from the different coherence scales of the charge carriers involved.

  1. Multi-orbital effects in optical properties of vanadium sesquioxide

    Science.gov (United States)

    Tomczak, Jan M.; Biermann, Silke

    2009-02-01

    Vanadium sesquioxide, V2O3, boasts a rich phase diagram whose description necessitates accounting for many-body Coulomb correlations. The spectral properties of this compound have been successfully addressed within dynamical mean field theory to the extent that results of recent angle-resolved photoemission experiments have been correctly predicted. While photoemission spectroscopy probes the occupied part of the one-particle spectrum, optical experiments measure transitions into empty states and thus provide complementary information. In this work, we focus on the optical properties of V2O3 in its paramagnetic phases by employing our recently developed 'generalized Peierls approach'. We obtain results in overall satisfactory agreement with experiments. Further, we rationalize that the experimentally observed temperature dependence stems from the different coherence scales of the charge carriers involved.

  2. Electronic structure of lanthanum sesquioxide: A Compton scattering study

    Science.gov (United States)

    Sharma, Sonu; Sahariya, Jagrati; Arora, Gunjan; Ahuja, B. L.

    2014-10-01

    We present the first-ever experimental and theoretical momentum densities of La2O3. The Compton line shape is measured using a 20 Ci 137Cs Compton spectrometer at an intermediate resolution with full width at half maximum of 0.34 a.u. The experimental Compton profile is compared with the theoretical electron momentum densities computed using linear combination of atomic orbitals (LCAO) method with density functional theory (DFT). It is seen that the generalized gradient approximation (GGA) within DFT reconciles better with the experiment than other DFT based approximations, validating the GGA approximation for rare-earth sesquioxides. The energy bands and density of states computed using LCAO calculations show its wide band gap nature which is in tune with the available reflectivity and photo-absorption data. In addition, Mulliken's population and charge density are also computed and discussed.

  3. Electronic structure of lanthanum sesquioxide: A Compton scattering study

    Energy Technology Data Exchange (ETDEWEB)

    Sharma, Sonu [Department of Physics, M.L. Sukhadia University, Udaipur 313001, Rajasthan (India); Sahariya, Jagrati [Department of Physics, Manipal University Jaipur, Jaipur 303007, Rajasthan (India); Arora, Gunjan [Department of Physics, Geetanjali Institute of Technical Studies, Udaipur 313022, Rajasthan (India); Ahuja, B.L., E-mail: blahuja@yahoo.com [Department of Physics, M.L. Sukhadia University, Udaipur 313001, Rajasthan (India)

    2014-10-01

    We present the first-ever experimental and theoretical momentum densities of La{sub 2}O{sub 3}. The Compton line shape is measured using a 20 Ci {sup 137}Cs Compton spectrometer at an intermediate resolution with full width at half maximum of 0.34 a.u. The experimental Compton profile is compared with the theoretical electron momentum densities computed using linear combination of atomic orbitals (LCAO) method with density functional theory (DFT). It is seen that the generalized gradient approximation (GGA) within DFT reconciles better with the experiment than other DFT based approximations, validating the GGA approximation for rare-earth sesquioxides. The energy bands and density of states computed using LCAO calculations show its wide band gap nature which is in tune with the available reflectivity and photo-absorption data. In addition, Mulliken's population and charge density are also computed and discussed.

  4. Germane facts about germanium sesquioxide: II. Scientific error and misrepresentation.

    Science.gov (United States)

    Kaplan, Bonnie J; Andrus, G Merrill; Parish, W Wesley

    2004-04-01

    The preceding paper reviewed the anticancer properties and safety of bis (2-carboxyethylgermanium) sesquioxide (CEGS). An examination of those data leads one to question why this information has not stimulated clinical trials in patients with cancer. The answer is discussed in this paper, which traces the history to an error published in the scientific literature in 1987. The reliance by subsequent authors on secondary sources, citing only the error and not the correction published in 1988, constitutes part of the explanation of why CEGS has been neglected. A second factor is also considered: careless reporting about any germanium-based compound as if the many thousands of germanium compounds were all the same. This combination of a publication error, careless writing, and the reliance on secondary sources appears to be responsible for the neglect of the potential clinical use of this unique germanium compound.

  5. Electronic structure and ionicity of actinide oxides from first principles

    DEFF Research Database (Denmark)

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

    2010-01-01

    The ground-state electronic structures of the actinide oxides AO, A2O3, and AO2 (A=U, Np, Pu, Am, Cm, Bk, and Cf) are determined from first-principles calculations, using the self-interaction corrected local spin-density approximation. Emphasis is put on the degree of f-electron localization, which...... for AO2 and A2O3 is found to follow the stoichiometry, namely, corresponding to A4+ ions in the dioxide and A3+ ions in the sesquioxides. In contrast, the A2+ ionic configuration is not favorable in the monoxides, which therefore become metallic. The energetics of the oxidation and reduction...... in the actinide dioxides is discussed, and it is found that the dioxide is the most stable oxide for the actinides from Np onward. Our study reveals a strong link between preferred oxidation number and degree of localization which is confirmed by comparing to the ground-state configurations of the corresponding...

  6. Actinide extraction methods

    Science.gov (United States)

    Peterman, Dean R [Idaho Falls, ID; Klaehn, John R [Idaho Falls, ID; Harrup, Mason K [Idaho Falls, ID; Tillotson, Richard D [Moore, ID; Law, Jack D [Pocatello, ID

    2010-09-21

    Methods of separating actinides from lanthanides are disclosed. A regio-specific/stereo-specific dithiophosphinic acid having organic moieties is provided in an organic solvent that is then contacted with an acidic medium containing an actinide and a lanthanide. The method can extend to separating actinides from one another. Actinides are extracted as a complex with the dithiophosphinic acid. Separation compositions include an aqueous phase, an organic phase, dithiophosphinic acid, and at least one actinide. The compositions may include additional actinides and/or lanthanides. A method of producing a dithiophosphinic acid comprising at least two organic moieties selected from aromatics and alkyls, each moiety having at least one functional group is also disclosed. A source of sulfur is reacted with a halophosphine. An ammonium salt of the dithiophosphinic acid product is precipitated out of the reaction mixture. The precipitated salt is dissolved in ether. The ether is removed to yield the dithiophosphinic acid.

  7. Actinide environmental chemistry

    International Nuclear Information System (INIS)

    Silva, R.J.; Nitsche, H.; Forschungszentrum Rossendorf e.V.

    1995-01-01

    In order to predict release and transport rates, as well as design cleanup and containment methods, it is essential to understand the chemical reactions and forms of the actinides under aqueous environmental conditions. Four important processes that can occur with the actinide cations are: precipitation, complexation, sorption and colloid formation. Precipitation of a solid phase will limit the amount of actinide in solution near the solid phase and have a retarding effect on release and transport rates. Complexation increases the amount of actinide in solution and tends to increase release and migration rates. Actinides can sorb on to mineral or rock surfaces which tends to retard migration. Actinide ions can form or become associated with colloidal sized particles which can, depending on the nature of the colloid and the solution conditions, enhance or retard migration of the actinide. The degree to which these four processes progress is strongly dependent on the oxidation state of the actinide and tends to be similar for actinides in the same oxidation state. In order to obtain information on the speciation of actinides in solution, i.e., oxidation state, complexation form, dissolved or colloidal forms, the use of absorption spectroscopy has become a method of choice. The advent of the ultrasensitive, laser induced photothermal and fluorescence spectroscopies has made possible the detection and study of actinide ions at the parts per billion level. With the availability of third generation synchrotrons and the development of new fluorescence detectors, X-ray absorption spectroscopy (XAS) is becoming a powerful technique to study the speciation of actinides in the environment, particularly for reactions at the solid/solution interfaces. (orig.)

  8. Neutron Scattering Studies of Pure and Chromium - Vanadium Sesquioxide

    Science.gov (United States)

    Yethiraj, Mohana

    1985-12-01

    The metal insulator transitions in pure and chromium -doped vanadium sesquioxide (V(,2)O(,3)) were investigated using elastic and inelastic neutron scattering techniques. These samples undergo a number of transitions as a function of temperature and doping. At the highest temperature, all specimens are in a metallic (M') phase. As the temperature is lowered, samples with less than 0.5% Cr transform to a second metallic (M) state. For those samples with Cr content between 0.5% and 1.8%, the system transforms to an insulating (I') phase prior to the transition to the M phase. For samples with >1.8% Cr, the M phase is entirely bypassed. At temperatures below (TURN)160K, all samples transform to an antiferromagnetic insulating (AFI) phase. The transition to the AFI state is accompanied by a structural distortion as well. The aim of this study was to add to our understanding of the driving mechanism(s) effecting the various metal-insulator transformations and in particular, the low temperature magnetic transition.

  9. XAFS study of the local structure of vanadium sesquioxide

    Science.gov (United States)

    Frenkel, Anatoly; Stern, Edward

    1996-03-01

    Vanadium sesquioxide (V_2O_3) undergoes a metal - insulator phase transition, accompanied by structural and magnetic transitions at the same temperature, when cooled below Tc ≈ 150 K. Upon the transition, the average crystal structure determined by diffraction changes from rhombohedral to monoclinic, where the vanadium - vanadium distances increase by about 0.11 ÅIt is generally believed that the metal - insulator transition is driven by the Mott - Habbard mechanism, consistent with such an expansion of the vanadium atoms distances. The information on the average structure only is not sufficient, however, to determine the nature of the transition which is related to the change in local structure around the V atoms. We performed X - ray Absorption Fine Structure (XAFS) transmission measuremerents at the V K - edge of V_2O3 - powder below and above Tc and determined the partial pair distribution function of the V and O nearest neighbors relative to the absorbing vanadium atom. An observed difference between the local and the average structure is discussed.

  10. Germane facts about germanium sesquioxide: I. Chemistry and anticancer properties.

    Science.gov (United States)

    Kaplan, Bonnie J; Parish, W Wesley; Andrus, G Merrill; Simpson, J Steven A; Field, Catherine J

    2004-04-01

    This paper reviews the history, chemistry, safety, toxicity, and anticancer effects of the organogermanium compound bis (2-carboxyethylgermanium) sesquioxide (CEGS). A companion review follows, discussing the inaccuracies in the scientific record that have prematurely terminated research on clinical uses of CEGS. CEGS is a unique organogermanium compound first made by Mironov and coworkers in Russia and, shortly thereafter, popularized by Asai and his colleagues in Japan. Low concentrations of germanium occur in nearly all soils, plants and animal life; natural occurrence of the CEGS form is postulated but not yet demonstrated. The literature demonstrating its anticancer effect is particularly strong: CEGS induces interferon-gamma (IFN-gamma), enhances natural killer cell activity, and inhibits tumor and metastatic growth--effects often detectable after a single oral dose. In addition, oral consumption of CEGS is readily assimilated and rapidly cleared from the body without evidence of toxicity. Given these findings, the absence of human clinical trials of CEGS is unexpected. Possible explanations of why the convincing findings from animal research have not been used to support clinical trials are discussed. Clinical trials on CEGS are recommended.

  11. Database of Small Molecule Thermochemistry for Combustion

    KAUST Repository

    Goldsmith, C. Franklin

    2012-09-13

    High-accuracy ab initio thermochemistry is presented for 219 small molecules relevant in combustion chemistry, including many radical, biradical, and triplet species. These values are critical for accurate kinetic modeling. The RQCISD(T)/cc-PV∞QZ//B3LYP/6-311++G(d,p) method was used to compute the electronic energies. A bond additivity correction for this method has been developed to remove systematic errors in the enthalpy calculations, using the Active Thermochemical Tables as reference values. On the basis of comparison with the benchmark data, the 3σ uncertainty in the standard-state heat of formation is 0.9 kcal/mol, or within chemical accuracy. An uncertainty analysis is presented for the entropy and heat capacity. In many cases, the present values are the most accurate and comprehensive numbers available. The present work is compared to several published databases. In some cases, there are large discrepancies and errors in published databases; the present work helps to resolve these problems. © 2012 American Chemical Society.

  12. Database of small molecule thermochemistry for combustion.

    Science.gov (United States)

    Goldsmith, C Franklin; Magoon, Gregory R; Green, William H

    2012-09-13

    High-accuracy ab initio thermochemistry is presented for 219 small molecules relevant in combustion chemistry, including many radical, biradical, and triplet species. These values are critical for accurate kinetic modeling. The RQCISD(T)/cc-PV∞QZ//B3LYP/6-311++G(d,p) method was used to compute the electronic energies. A bond additivity correction for this method has been developed to remove systematic errors in the enthalpy calculations, using the Active Thermochemical Tables as reference values. On the basis of comparison with the benchmark data, the 3σ uncertainty in the standard-state heat of formation is 0.9 kcal/mol, or within chemical accuracy. An uncertainty analysis is presented for the entropy and heat capacity. In many cases, the present values are the most accurate and comprehensive numbers available. The present work is compared to several published databases. In some cases, there are large discrepancies and errors in published databases; the present work helps to resolve these problems.

  13. Actinide recovery process

    Science.gov (United States)

    Muscatello, Anthony C.; Navratil, James D.; Saba, Mark T.

    1987-07-28

    Process for the removal of plutonium polymer and ionic actinides from aqueous solutions by absorption onto a solid extractant loaded on a solid inert support such as polystyrenedivinylbenzene. The absorbed actinides can then be recovered by incineration, by stripping with organic solvents, or by acid digestion. Preferred solid extractants are trioctylphosphine oxide and octylphenyl-N,N-diisobutylcarbamoylmethylphosphine oxide and the like.

  14. 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

  15. Control of interface shape during high melting sesquioxide crystal growth by HEM technique

    Science.gov (United States)

    Hu, Kaiwei; Zheng, Lili; Zhang, Hui

    2018-02-01

    During crystal growth in heat exchanger method (HEM) system, the shape of the growth interface changes with the proceeding of the growth process, which limits the crystal size and reduces the quality of the crystal. In this paper, a modified HEM system is proposed to control the interface shape for growth of sesquioxide crystals. Numerical simulation is performed to predict heat transfer, melt flow and interface shape during growth of high melting sesquioxide crystals by the heat exchanger method. The results show that a flat or slightly convex interface shape is beneficial to reduce the solute pileup in front of the melt/crystal interface and decrease the radial temperature gradient inside the crystal during growth of sesquioxide crystals. The interface shape can be controlled by adjusting the gap size d and lower resistance heater power during growth. The growth rate and the melt/crystal interface position can be obtained by two measured temperatures.

  16. A Hierarchy of Homodesmotic Reactions for Thermochemistry

    Science.gov (United States)

    Schleyer, Paul v. R.

    2009-01-01

    Chemical equations that balance bond types and atom hybridization to different degrees are often used in computational thermochemistry, for example, to increase accuracy when lower levels of theory are employed. We expose the widespread confusion over such classes of equations and demonstrate that the two most widely used definitions of “homodesmotic” reactions are not equivalent. New definitions are introduced and a consistent hierarchy of reaction classes (RC1 – RC5) for hydrocarbons is constructed: isogyric (RC1) ⊇ isodesmic (RC2) ⊇ hypohomodesmotic (RC3) ⊇ homodesmotic (RC4) ⊇ hyperhomodesmotic (RC5). Each of these successively conserves larger molecular fragments. The concept of isodesmic bond separation reactions is generalized to all classes in this hierarchy, providing a unique sectioning of a given molecule for each reaction type. Several ab initio and density functional methods are applied to the bond separation reactions of 38 hydrocarbons containing five or six carbon atoms. RC4 and RC5 reactions provide bond separation enthalpies with errors consistently less than 0.4 kcal mol−1 across a wide range of theoretical levels, performing significantly better than the other reaction types and far superior to atomization routes. Our recommended bond separation reactions were demonstrated by determining the enthalpies of formation (at 298 K) of 1,3,5-hexatriyne (163.7 ± 0.4 kcal mol−1), 1,3,5,7-octatetrayne (217.6 ± 0.6 kcal mol−1), the larger polyynes C10H2 through C26H2, and an infinite acetylenic carbon chain. PMID:19182999

  17. Thermochemistry of liquid Ni–Sb–Sn alloys

    Czech Academy of Sciences Publication Activity Database

    Mishra, R.; Kroupa, Aleš; Terzieff, P.; Ipser, H.

    2012-01-01

    Roč. 536, MAY (2012), s. 68-73 ISSN 0040-6031 R&D Projects: GA MŠk(CZ) OC08053 Institutional support: RVO:68081723 Keywords : Ni-Sb-Sn alloys * thermochemistry * vapor pressure measurements Subject RIV: BJ - Thermodynamics Impact factor: 1.989, year: 2012

  18. A computational study on kinetics, mechanism and thermochemistry ...

    Indian Academy of Sciences (India)

    Home; Journals; Journal of Chemical Sciences; Volume 126; Issue 6. A computational study on kinetics, mechanism and thermochemistry of gas-phase reactions of 3-hydroxy-2-butanone with OH radicals. Nand Kishor Gour Satyendra Gupta Bhupesh Kumar Mishra Hari Ji Singh. Regular Articles Volume 126 Issue 6 ...

  19. Theoretical study on mechanism, kinetics, and thermochemistry of ...

    Indian Academy of Sciences (India)

    Home; Journals; Journal of Chemical Sciences; Volume 127; Issue 6. Theoretical study on mechanism, kinetics, and thermochemistry of the gas phase reaction of 2,2,2-trifluoroethyl butyrate with OH radicals at 298 K. Nand Kishor Gour Bhupesh Kumar Mishra Hari Ji Singh. Regular Articles Volume 127 Issue 6 June 2015 ...

  20. Moessbauer spectroscopy on actinides

    International Nuclear Information System (INIS)

    Boge, M.

    1988-01-01

    The wide spatial extend of the 5f electrons leads a broad spectrum of chemical and physical properties, in particular magnetic, in compounds of light actinides. Their behaviour goes from the localized magnetism of lanthanides to the itinerant magnetism often found in transition metals compounds. One parameter which strongly influences the magnetic character is the actinide-actinide distance. Moessbauer spectroscopy of the 59.5 KeV resonance in 237 Np allows a detailed study of local magnetic properties of the Np ion. Some results are presented on compounds of different crystallographic structure, showing the large variety of magnetic properties

  1. Metal-insulator transition in epitaxial vanadium sesquioxide thin films

    Science.gov (United States)

    Allimi, Bamidele S.

    Of all the transition metal oxides which exhibit metal-insulator transitions (MIT), one of the most extensively studied in recent years is the vanadium sesquioxide (V2O3), both from experimental and theoretical point of view. At a transition temperature of about 160 K at an ambient pressure of 1 atm, pure V2O3 transforms from a rhombohedral paramagnetic metallic (PM) to a monoclinic antiferromagnetic insulating (AFI) phase upon cooling, with a jump in the resistivity of about seven orders of magnitude. Experimental studies have focused more on bulk V2O3 and recently there have been significant interest in thin film fabrication of this material due to potential applications as thermal sensors, current limiters, Positive Temperature Coefficient (PTC) thermistors, and optical switches. This study addresses the deposition, characterization, and properties of high-quality epitaxial V2O3 thin films grown on a-, c-Al2O3 and c-LiTaO 3 substrates by a straightforward method of pulsed laser deposition (PLD). Various characterization techniques including X-ray diffraction, atomic force microscopy, scanning electron microscopy, and X-ray photoemission spectroscopy were used to examine the structural, crystallographic, and surface properties, while four point probe resistivity measurements were used to examine the electrical properties of the films. V2O3 thin films of different thicknesses ranging from 10-450 nm were deposited on c-Al 2O3 and c-LiTaO3 substrates by PLD to understand also the role of epitaxial strains. Resistivity measurements showed that depending on the thicknesses of films, different electrical transitions were exhibited by the samples. While some of the samples displayed the expected metal-insulator transition typical of bulk V2O3, some showed insulating behavior only and others exhibited metallic characteristics only over the whole temperature range. For example, for films on c-LiTaO3 with increasing film thickness, first an insulator-insulator, then a

  2. Flowerlike vanadium sesquioxide: solvothermal preparation and electrochemical properties.

    Science.gov (United States)

    Liu, Haimei; Wang, Yonggang; Li, Huiqiao; Yang, Wensheng; Zhou, Haoshen

    2010-10-25

    A novel 3D hierarchical flowerlike vanadium sesquioxide (V(2)O(3)) nano/microarchitecture consisting of numerous nanoflakes is prepared via a solvothermal approach followed by an appropriate heating treatment. The as-obtained nanostructured V(2)O(3) flower is characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) analysis, and transmission electron microscopy (TEM) (or/and high-resolution TEM, HRTEM), and it is found that the V(2)O(3) flower is constructed by single-crystalline nanoflakes. Furthermore, it is demonstrated that the surface of the flowerlike V(2)O(3) material is composed of nanostructured pores, which derive from the adsorption/desorption of nitrogen, and that the pore-size distribution depends on the unique three-dimensional interconnection between nanoflakes and on their intrinsic properties. The electrochemical behavior of the V(2)O(3) flower for lithium-ion insertion/extraction in non-aqueous solution as well as the faradaic capacitance for pesudocapacitors in a neutral aqueous solution are also investigated. A reversible discharge capacity as high as 325 mA h g(-1) is obtained at a current density of 0.02 A g(-1) from a LiClO(4)/EC:DEC electrolyte solution (i.e. LiClO(4) in ethyl carbonate and diethyl carbonate). When used as the cathode material of pesudocapacitors in Li(2)SO(4), the flowerlike oxide displayed a very high initial capacitance of 218 F g(-1) at a current density of 0.05 A g(-1). We believe that the good performance of the flowerlike V(2)O(3) electrode is most probably due to its unique 3D hierarchical nano/microarchitecture, which shows that the electrochemical properties of a cathodic material do not only depend on the oxidation state of that material but also-to a large extent-on its crystalline structure and morphology. The aforementioned properties suggest that the present V(2)O(3) flower materials may have a great potential to be employed as electrode materials in

  3. 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)

  4. 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

  5. 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).

  6. Conversion of hydrous germanium(II) oxide to germynyl sesquioxide, (HGe)/sub 2/O/sub 3/

    Energy Technology Data Exchange (ETDEWEB)

    Yang, D.J.; Jolly, W.L.; O' Keefe, A.

    1977-11-01

    The solubility, pyrolysis and vibrational spectra of hydrous germanium(II) oxide and its conversion to germynyl sesquioxide are discussed. Digestion of a suspension of Ge(II) hydroxide yielded the sesquioxide which may be a polymer consisting of Ge-H groups linked by oxygen atoms. Infrared spectra indicate that the sesquioxide (HGe)/sub 2/O/sub 3/ is structurally different from various forms of Ge(II) hydroxide not treated with hydroxide solutions. Other reactions of the different species are contrasted. (BLM)

  7. 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.)

  8. Predicted thermochemistry and unimolecular kinetics of nitrous sulfide

    DEFF Research Database (Denmark)

    Marshall, Paul; Gao, Yide; Glarborg, Peter

    2011-01-01

    (Q) and relativistic effects, D-0 for the N-S bond is estimated as 71.9 kJ mol (1), and the corresponding thermochemistry for N2S is Delta H-f(0)degrees = 205.4 kJ mol(-1) and Delta H-f(298)degrees = 202.6 kJ mol(-1) with an uncertainty of +/- 2.5 kJ mol(-1). Using CCSD(T)/aug-cc-pV(T + d) theory the minimum energy...... for dissociation of N2S k(0) = 7.6 x 10(-10) exp(-126 kJ mol(-1)/RT) cm(3) molecule(-1) s(-1) over 700-2000 K. The estimated uncertainty is a factor of 4 arising from unknown parameters for energy transfer between N2S and Ar or N-2 bath gas. The thermochemistry and kinetics were included in a mechanism for CO/H-2...

  9. Thermochemistry and Reactivity of Metals Engaged in Chemiionization

    Science.gov (United States)

    2015-12-03

    AFRL) Metal Oxide Space Cloud ( MOSC ) experiments have been conducted to test the efficiency of forming an artificial plasma cloud by this process...the MOSC results, hence, the PIs laboratory was contacted to see if we could elucidate the thermochemistry of SmO and SmO + more thoroughly. As...by only 0.08 0.07 eV. Simulations of the MOSC test using this thermodynamic information are in agreement with the experimental results from this

  10. 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

  11. 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

  12. 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)

  13. 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.)

  14. 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.

  15. Preparation of higher-actinide burnup and cross section samples. [LMFBR

    Energy Technology Data Exchange (ETDEWEB)

    Adair, H.L.; Kobisk, E.H.; Quinby, T.C.; Thomas, D.K.; Dailey, J.M.

    1981-01-01

    A joint research program involving the United States and the United Kingdom was instigated about four years ago for the purpose of studying burnup of higher actinides using in-core irradiation in the fast reactor at Dounreay, Scotland. Simultaneously, determination of cross sections of a wide variety of higher actinide isotopes was proposed. Coincidental neutron flux and energy spectral measurements were to be made using vanadium encapsulated dosimetry materials in the immediate region of the burnup and cross section samples. The higher actinide samples chosen for the burnup study were /sup 241/Am and /sup 244/Cm in the forms of Am/sub 2/O/sub 3/, Cm/sub 2/O/sub 3/, and Am/sub 6/ Cm(RE)/sub 7/O/sub 21/, where (RE) represents a mixture of lanthanide sesquioxides. It is the purpose of this paper to describe technology development and its application in the preparation of the fuel specimens and the cross section specimens that are being used in this cooperative program.

  16. 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)

  17. Recovering actinide values

    International Nuclear Information System (INIS)

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

    1980-01-01

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

  18. 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

  19. Environmental speciation of actinides.

    Science.gov (United States)

    Maher, Kate; Bargar, John R; Brown, Gordon E

    2013-04-01

    Although minor in abundance in Earth's crust (U, 2-4 ppm; Th, 10-15 ppm) and in seawater (U, 0.003 ppm; Th, 0.0007 ppm), light actinides (Th, Pa, U, Np, Pu, Am, and Cm) are important environmental contaminants associated with anthropogenic activities such as the mining and milling of uranium ores, generation of nuclear energy, and storage of legacy waste resulting from the manufacturing and testing of nuclear weapons. In this review, we discuss the abundance, production, and environmental sources of naturally occurring and some man-made light actinides. As is the case with other environmental contaminants, the solubility, transport properties, bioavailability, and toxicity of actinides are dependent on their speciation (composition, oxidation state, molecular-level structure, and nature of the phase in which the contaminant element or molecule occurs). We review the aqueous speciation of U, Np, and Pu as a function of pH and Eh, their interaction with common inorganic and organic ligands in natural waters, and some of the common U-containing minerals. We also discuss the interaction of U, Np, Pu, and Am solution complexes with common Earth materials, including minerals, colloids, gels, natural organic matter (NOM), and microbial organisms, based on simplified model system studies. These surface interactions can inhibit (e.g., sorption to mineral surfaces, formation of insoluble biominerals) or enhance (e.g., colloid-facilitated transport) the dispersal of light actinides in the biosphere and in some cases (e.g., interaction with dissimilatory metal-reducing bacteria, NOM, or Mn- and Fe-containing minerals) can modify the oxidation states and, consequently, the behavior of redox-sensitive light actinides (U, Np, and Pu). Finally, we review the speciation of U and Pu, their chemical transformations, and cleanup histories at several U.S. Department of Energy field sites that have been used to mill U ores, produce fissile materials for reactors and weapons, and store

  20. Two state coercivity driven by phase coexistence in vanadium sesquioxide/nickel bulk hybrid material

    Science.gov (United States)

    Urban, C.; Quesada, A.; Saerbeck, T.; Garcia, M. A.; de la Rubia, M. A.; Valmianski, I.; Fernández, J. F.; Schuller, I. K.

    2016-09-01

    We developed a bulk hybrid material consisting of a vanadium sesquioxide (V2O3) matrix with nickel (Ni) rich inclusions that exhibit a switchable two-state magnetic coercivity. The V2O3 matrix magnetoelastically couples with the Ni-rich inclusions and its structural phase transition causes two possible magnetic coercivity states. Differences of up to 13% in the temperature window of 14 K are observed, depending whether the transition occurs from rhombohedral to monoclinic or vice versa. These findings provide a pathway for the development of bulk switchable coercivity materials. We present routes to further enhance the magnetoelastic effect by increasing the oxide/ferromagnetic material coupling.

  1. Low-temperature magnetic ordering and structural distortions in Vanadium Sesquioxide (V$_2$O$_3$)

    OpenAIRE

    Grieger, Daniel; Fabrizio, Michele

    2015-01-01

    Vanadium Sesquioxide (V$_2$O$_3$) is an antiferromagnetic insulator below $T_{\\mathrm N}\\approx$ 155 K. The magnetic order is not of C- or G-type as one would infer from the bipartite character of the hexagonal basal plane in the high-temperature corundum structure. In fact, the N\\'eel transition is accompanied by a monoclinic distortion that makes one bond of the honeycomb plane inequivalent from the other two, thus justifying a magnetic structure with one ferromagnetic bond and two antiferr...

  2. Thermochemistry of interaction between zirconium disulfate and sulfuric acid

    International Nuclear Information System (INIS)

    Dmitrieva, S.V.; Chekmarev, A.M.; Vorob'ev, A.F.

    1988-01-01

    Thermochemistry of Zr(SO 4 ) 2 x4H 2 O (1) interaction with water and sulfuric acid solutions of different concentrations is studied. It is established that the dependence of 1 solution enthalpy on acid concentration 1-bars of a complex polyextreme nature. It is noted that the increase in exothermic nature of dissolving during the increase of H 2 SO 4 concentration from 0.05 to 0.50 mol/l is explained by zirconium hydroxosulfate and fulfate complexes substitution for hydroxocomplexes. The endothermal nature of 1 interaction with concentrated (>3 mol/l) H 2 SO 4 solutions is conditioned by the formation of acidocomplexes. It is assumed that the abrupt growth of the exothermal nature of 1 interaction with sulfuric acid solutions with the concentration less than 0.05 mol/l with water is connected with colloid formation. 12 refs.; 2 figs

  3. Synthesis and Gas Phase Thermochemistry of Germanium-Containing Compounds

    Energy Technology Data Exchange (ETDEWEB)

    Classen, Nathan Robert [Iowa State Univ., Ames, IA (United States)

    2002-01-01

    The driving force behind much of the work in this dissertation was to gain further understanding of the unique olefin to carbene isomerization observed in the thermolysis of 1,1-dimethyl-2-methylenesilacyclobutane by finding new examples of it in other silicon and germanium compounds. This lead to the examination of a novel phenylmethylenesilacyclobut-2-ene, which did not undergo olefin to carbene rearrangement. A synthetic route to methylenegermacyclobutanes was developed, but the methylenegermacyclobutane system exhibited kinetic instability, making the study of the system difficult. In any case the germanium system decomposed through a complex mechanism which may not include olefin to carbene isomerization. However, this work lead to the study of the gas phase thermochemistry of a series of dialkylgermylene precursors in order to better understand the mechanism of the thermal decomposition of dialkylgermylenes. The resulting dialkylgermylenes were found to undergo a reversible intramolecular β C-H insertion mechanism.

  4. Acid-base thermochemistry of gaseous aliphatic α-aminoacids.

    Science.gov (United States)

    Bouchoux, Guy; Huang, Sihua; Inda, Bhawani Singh

    2011-01-14

    Acid-base thermochemistry of isolated aliphatic amino acids (denoted AAA): glycine, alanine, valine, leucine, isoleucine and proline has been examined theoretically by quantum chemical computations at the G3MP2B3 level. Conformational analysis on neutral, protonated and deprotonated species has been used to identify the lowest energy conformers and to estimate the population of conformers expected to be present at thermal equilibrium at 298 K. Comparison of the G3MP2B3 theoretical proton affinities, PA, and ΔH(acid) with experimental results is shown to be correct if experimental thermochemistry is re-evaluated and adapted to the most recent acidity-basicity scales. From this point of view, a set of evaluated proton affinities of 887, 902, 915, 916, 919 and 941 kJ mol(-1), and a set of evaluated ΔH(acid) of 1433, 1430, 1423, 1423, 1422 and 1426 kJ mol(-1), is proposed for glycine, alanine, valine, leucine, isoleucine and proline, respectively. Correlations with structural parameters (Taft's σ(α) polarizability parameter and molecular size) suggest that polarizability of the side chain is the major origin of the increase in PA and decrease in ΔH(acid) along the homologous series glycine, alanine, valine and leucine/isoleucine. Heats of formation of gaseous species AAA, AAAH(+) and [AAA-H](-) were computed at the G3MP2B3 level. The present study provides previously unavailable Δ(f)H°(298) for the ionized species AAAH(+) and [AAA-H](-). Comparison with Benson's estimate, and correlation with molecular size, show that several experimental Δ(f)H°(298) values of neutral or gaseous AAA might be erroneous.

  5. 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.

  6. Actinide physicochemical data assessment and selection

    International Nuclear Information System (INIS)

    Navratil, J.D.

    1984-01-01

    There is a continuing need to have reliable physicochemical data of actinide compounds and actinide elements in aqueous solution available for nuclear engineers and scientists. These data are needed for all aspects of the nuclear fuel cycle - from the behavior of actinides in reactor fuels at high temperature and pressure to actinide behavior in geologic depository environments. This paper summarizes the status of actinide physicochemical data assessment and selection. The topics to be covered include data assessment of chemical thermodynamic properties and solubilities of actinide compounds and solution equilibria of the actinides

  7. 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)

  8. 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 actinides with the simple inputs of mass number (A) and atomic number (Z) of projectile-targets.

  9. 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

  10. 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

  11. 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

  12. Systematic thermodynamic properties of actinide metal-oxygen systems at high temperatures: Emphasis on lower valence states

    International Nuclear Information System (INIS)

    Ackermann, R.J.; Chandrasekharaiah, M.S.

    1975-01-01

    The thermodynamic data for the actinide metals and oxides (thorium to curium ) have been assessed, examined for consistency, and compared with the lanthanides. Correlations relating the enthalpies of formation of the solid oxides with the corresponding aquo ions make possible the estimation of the thermodynamic properties of AmO 2 (s) and Am 2 O 3 (s) which are in accordance with vaporization data. The known thermodynamic properties of the substoichiometric dioxides MOsub(2-x)(s) at high temperatures demonstrate the relative stabilities of valence states less than 4+ and lead to the examination of stability requirements for the sesquioxides M 2 O 3 (s) and the monoxides MO(s). Sequential trends in the gaseous metals, monoxides and dioxides are examined, compared, and contrasted with the lanthanides. (author)

  13. 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)

  14. Insulator-to-metal transition in vanadium sesquioxide: does the Mott criterion work in this case?

    Science.gov (United States)

    Pergament, Alexander; Stefanovich, Genrikh

    2012-03-01

    It is shown that the Mott criterion expressed by the simple relation a B(n c)1/3 ≈ 0.25 turns out to be quite successful in describing metal-insulator phase transitions not only in heavily doped semiconductors, but also in transition metal oxides such as VO2 and V2O3. It is found in this article that, in the case of a high-temperature transition 'paramagnetic insulator - paramagnetic metal' in vanadium sesquioxide, a B(n c)1/3 = 0.254. Difficulties connected with the analogous description of a low-temperature transition ('paramagnetic metal - antiferromagnetic insulator') in V2O3 are discussed.

  15. Structural distortions in vanadium sesquioxide (V{sub 2}O{sub 3})

    Energy Technology Data Exchange (ETDEWEB)

    Grieger, Daniel; Fabrizio, Michele [Scuola Internazionale Superiore di Studi Avanzati (SISSA), Trieste (Italy)

    2015-07-01

    Vanadium Sesquioxide (V{sub 2}O{sub 3}) has attracted large attention mainly because of its prototypical Mott insulating behaviour with negative (chemical) pressure/Chromium doping. Besides trying to shed some light on details of this transition, this contribution is primarily aimed at the structural distortions that accompany the electronic phase diagram. These are especially important near the transition to the low-temperature (T < 140 K) antiferromagnetic insulating phase, as well as in a recently discovered high-pressure monoclinic metallic phase. The relation and concurrence of the former with the antiferromagnetic ordering is investigated theoretically, which also has consequences for the appearance of the high-pressure phase. Formalisms applied for this purpose are combinations of traditional electronic structure formalisms and DFT+-like approaches.

  16. Bixbyite-type V2O3--a metastable polymorph of vanadium sesquioxide.

    Science.gov (United States)

    Weber, D; Stork, A; Nakhal, S; Wessel, C; Reimann, C; Hermes, W; Müller, A; Ressler, T; Pöttgen, R; Bredow, T; Dronskowski, R; Lerch, M

    2011-07-18

    A metastable polymorph of vanadium sesquioxide was prepared by the reaction of vanadium trifluoride with a water-saturated gaseous mixture of 10 vol % hydrogen in argon. The new polymorph crystallizes in the bixbyite-type structure. At temperatures around 823 K a transformation to the well-known corundum-type phase is observed. Quantum-chemical calculations show that the bixbyite-type structure is about 9 kJ/mol less stable than the known corundum-based one. This result, in combination with the absence of imaginary modes in the phonon density of states, supports the classification of the bixbyite-type phase as a metastable V(2)O(3) polymorph. At ~50 K a paramagnetic to canted antiferromagnetic transition is detected.

  17. Effects of organogermanium compound 2-carboxyethyl germanium sesquioxide on cardiovascular function and motor activity in rats.

    Science.gov (United States)

    Ho, C C; Chern, Y F; Lin, M T

    1990-01-01

    In rats anesthetized with urethane, intraperitoneal administration of a water-soluble organogermanium compound 2-carboxyethyl germanium sesquioxide (Ge-132) produced a dose-related reduction in either the mean arterial pressure or the heart rate. Both hypotension and bradycardia responses induced by Ge-132 injection were significantly inhibited by pretreatment of the animals with either spinal transection or bilateral vagotomy. The data indicate that Ge-132 induces both hypotension and bradycardia by promoting an activation of the parasympathetic efferent mechanisms and an inhibition of the sympathetic efferent mechanisms. On the other hand, following intraperitoneal injection of Ge-132, increased grooming and head swaying (as shown by an enhancement in fine movements monitored by an electronic activity counter) were provoked. Furthermore, the amphet-amine-induced enhancement in fine movements was potentiated by pretreatment of the animals with Ge-132. Thus, it appears that Ge-132 acts through the catecholaminergic mechanisms in the brain to induce locomotor stimulation in rats.

  18. Inhibitory effects of Ge-132 (carboxyethyl germanium sesquioxide) derivatives on enkephalin-degrading enzymes.

    Science.gov (United States)

    Komuro, T; Kakimoto, N; Katayama, T; Hazato, T

    1986-10-01

    Twenty-eight species of carboxyethyl germanium sesquioxide (Ge-132) derivatives were examined for their inhibitory effects on enkephalin-degrading enzymes that were purified from monkey brain, the longitudinal muscle layer of bovine small intestine, and human cerebrospinal fluid (CSF). A series of the sulfurized Ge-132 derivatives showed strong inhibition of these purified enzymes. The most effective ones were Ge-014 and Ge-107, which showed IC50 values of 60 and 100 micrograms/ml, respectively, for dipeptidylcarboxypeptidase from the longitudinal muscle layer. They also exhibited inhibitory activity against aminopeptidase from human CSF, the IC50 values being 450 and 440 micrograms/ml, respectively. Furthermore, these compounds showed inhibition of dipeptidylaminopeptidase from monkey brain and the longitudinal muscle layer of bovine small intestine. These compounds are expected to have analgesic effects due to their inhibition of the degradation of endogenous opioid peptides.

  19. [Subacute and subchronic oral toxicity of beta-bis carboxyethyl sesquioxide of germanium in the rat].

    Science.gov (United States)

    Anger, F; Anger, J P; Guillou, L; Sado, P A; Papillon, A

    1991-12-01

    After a brief recall of toxicological data about germanium compounds, the authors relate subacute and subchronic oral toxicities of beta bis carboxyethyl-germanium sesquioxide in rats. During 28 days and six months, male and female animals have received 1 mg/kg/day. No particular toxic symptoms, no behaviour trouble except a small decrease of body weight, in male rats, at the end of the 6-month experimentation, were observed. A light decrease of erythropoiesis and a general stimulation of cellular metabolism has been noticed after 28 days. The only marked effect was a moderate renal deficiency characterized by a tubular disease with presence of cylinders, swelling of tubulus cells and floculus amounts after 6 months. Germanium urinary excretion was constant and linked to the received dose. Six months later, no preferential accumulation in organs was observed.

  20. Anomalous compression and new high-pressure phases of vanadium sesquioxide, V2O3

    Science.gov (United States)

    Ovsyannikov, Sergey V.; Trots, Dmytro M.; Kurnosov, Alexander V.; Morgenroth, Wolfgang; Liermann, Hanns-Peter; Dubrovinsky, Leonid

    2013-09-01

    We report results of a powder x-ray diffraction (XRD) study of vanadium sesquioxide, V2O3, under pressurization in a neon pressure-transmitting medium up to 57 GPa. We have established a bulk modulus value for corundum-type V2O3 of B0 = 150 GPa at B‧ = 4. This bulk modulus value is the lowest among those known for the corundum-type-structured oxides, e.g. Al2O3, α-Fe2O3, Cr2O3, Ti2O3, and α-Ga2O3. We have proposed that this might be related to the difference in the electronic band structures: at room temperature V2O3 is metallic, but the above corundum-structured sesquioxides are semiconducting or insulating. Around ˜21-27 and ˜50 GPa we registered changes in the XRD patterns that might be addressed to phase transitions. These transitions were sluggish upon room-temperature compression, and hence we additionally facilitated them by the laser heating of one sample. We have refined the XRD patterns of only the first high-pressure phase in an orthorhombic lattice of a Rh2O3(II)-type. Our findings significantly extend the knowledge of the P-T phase diagram of V2O3 and advance the understanding of its properties. We speculate that the elastic properties of V2O3 can be closely linked to its electronic band structure and, consequently, we propose that slightly doped V2O3 (e.g. with Cr) could be a potential candidate for systems in which the bulk modulus value may be remarkably switched by moderate pressure or temperature.

  1. DFT Perspective on the Thermochemistry of Carbon Nitride Synthesis

    KAUST Repository

    Melissen, Sigismund T. A. G.

    2016-10-11

    Graphitic (g)-CxNyHz has become a popular family of photoharvesters in photocatalytic water splitting cells, as well as other applications in chemistry. In this Article, different g-CxNyHz structures were studied thermochemically using DFT. Following a benchmark study with different families of functionals, the B3LYP functional was shown to accurately capture the thermochemistry of carbon nitride synthesis. A triple-ζ polarized basis set, in combination with Civalleri’s modification to Grimme’s D2 formalism (with s6 = 0.5) for dispersion interactions, yielded accurate geometries. Grimme’s D3 formalism with Becke–Johnson damping was used to refine the energetic description of dispersion interactions. The stepwise cycloaddition of cyanamide to form melamine was shown to be exergonic, whereas the stepwise deamination of melamine to form g-C3N4 was shown to be endergonic. Of those structures respecting the [C6N9H3]n chemical formula, the structure commonly known as “melon” was found to be most stable, whereas the sp3-hybridized [C6N9H3]n elucidated by Horvath-Bordon et al. was found to be the least stable. Fully polymerized triazine-based g-C3N4 appeared slightly more stable than heptazine-based g-C3N4.

  2. 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

  3. 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

  4. 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.

  5. 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.

  6. Positron Spectroscopy of Hydrothermally Grown Actinide Oxides

    Science.gov (United States)

    2014-03-27

    POSITRON SPECTROSCOPY OF HYDROTHERMALLY GROWN ACTINIDE OXIDES THESIS Edward C. Schneider...United States Government. AFIT-ENP-14-M-33 POSITRON SPECTROSCOPY OF HYDROTHERMALLY GROWN ACTINIDE OXIDES THESIS...33 POSITRON SPECTROSCOPY OF HYDROTHERMALLY GROWN ACTINIDE OXIDES Edward C. Schneider, BS Captain, USAF Approved

  7. 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

  8. 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

  9. 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.)

  10. Actinides and Life's Origins

    Science.gov (United States)

    Adam, Zachary

    2007-12-01

    There are growing indications that life began in a radioactive beach environment. A geologic framework for the origin or support of life in a Hadean heavy mineral placer beach has been developed, based on the unique chemical properties of the lower-electronic actinides, which act as nuclear fissile and fertile fuels, radiolytic energy sources, oligomer catalysts, and coordinating ions (along with mineralogically associated lanthanides) for prototypical prebiotic homonuclear and dinuclear metalloenzymes. A four-factor nuclear reactor model was constructed to estimate how much uranium would have been required to initiate a sustainable fission reaction within a placer beach sand 4.3 billion years ago. It was calculated that about 1-8 weight percent of the sand would have to have been uraninite, depending on the weight percent, uranium enrichment, and quantity of neutron poisons present within the remaining placer minerals. Radiolysis experiments were conducted with various solvents with the use of uranium- and thorium-rich minerals (metatorbernite and monazite, respectively) as proxies for radioactive beach sand in contact with different carbon, hydrogen, oxygen, and nitrogen reactants. Radiation bombardment ranged in duration of exposure from 3 weeks to 6 months. Low levels of acetonitrile (estimated to be on the order of parts per billion in concentration) were conclusively identified in 2 setups and tentatively indicated in a 3rd by gas chromatography/mass spectrometry. These low levels have been interpreted within the context of a Hadean placer beach prebiotic framework to demonstrate the promise of investigating natural nuclear reactors as power production sites that might have assisted the origins of life on young rocky planets with a sufficiently differentiated crust/mantle structure. Future investigations are recommended to better quantify the complex relationships between energy release, radioactive grain size, fissionability, reactant phase, phosphorus

  11. Actinides and Life's Origins.

    Science.gov (United States)

    Adam, Zachary

    2007-12-01

    There are growing indications that life began in a radioactive beach environment. A geologic framework for the origin or support of life in a Hadean heavy mineral placer beach has been developed, based on the unique chemical properties of the lower-electronic actinides, which act as nuclear fissile and fertile fuels, radiolytic energy sources, oligomer catalysts, and coordinating ions (along with mineralogically associated lanthanides) for prototypical prebiotic homonuclear and dinuclear metalloenzymes. A four-factor nuclear reactor model was constructed to estimate how much uranium would have been required to initiate a sustainable fission reaction within a placer beach sand 4.3 billion years ago. It was calculated that about 1-8 weight percent of the sand would have to have been uraninite, depending on the weight percent, uranium enrichment, and quantity of neutron poisons present within the remaining placer minerals. Radiolysis experiments were conducted with various solvents with the use of uraniumand thorium-rich minerals (metatorbernite and monazite, respectively) as proxies for radioactive beach sand in contact with different carbon, hydrogen, oxygen, and nitrogen reactants. Radiation bombardment ranged in duration of exposure from 3 weeks to 6 months. Low levels of acetonitrile (estimated to be on the order of parts per billion in concentration) were conclusively identified in 2 setups and tentatively indicated in a 3(rd) by gas chromatography/mass spectrometry. These low levels have been interpreted within the context of a Hadean placer beach prebiotic framework to demonstrate the promise of investigating natural nuclear reactors as power production sites that might have assisted the origins of life on young rocky planets with a sufficiently differentiated crust/mantle structure. Future investigations are recommended to better quantify the complex relationships between energy release, radioactive grain size, fissionability, reactant phase, phosphorus

  12. 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

  13. 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

  14. Tuning Eu{sup 3+} emission in europium sesquioxide films by changing the crystalline phase

    Energy Technology Data Exchange (ETDEWEB)

    Mariscal, A., E-mail: antonio.mariscal@csic.es [Laser Processing Group, Instituto de Óptica, CSIC, C/ Serrano 121, 28006 Madrid (Spain); Quesada, A. [Ceramics for Smart Systems Group, Instituto de Cerámica y Vidrio, C/ Kelsen 5, 28049 Madrid (Spain); Camps, I. [Laser Processing Group, Instituto de Óptica, CSIC, C/ Serrano 121, 28006 Madrid (Spain); Palomares, F.J. [Instituto de Ciencia de Materiales de Madrid, C/ Sor Juana Inés de la Cruz 3, 28049 Madrid (Spain); Fernández, J.F. [Ceramics for Smart Systems Group, Instituto de Cerámica y Vidrio, C/ Kelsen 5, 28049 Madrid (Spain); Serna, R. [Laser Processing Group, Instituto de Óptica, CSIC, C/ Serrano 121, 28006 Madrid (Spain)

    2016-06-30

    Highlights: • PLD production of high quality europium sesquioxide (Eu{sub 2}O{sub 3}) films. • The deposition of Al{sub 2}O{sub 3} capping and/or buffer layers modifies the crystallization for Eu{sub 2}O{sub 3} films upon annealing. • The formation of cubic or monoclinic phases can be favored. • Eu{sup 3+} emission tuning is achieved as a consequence of crystal field effects. - Abstract: We report the growth of europium sesquioxide (Eu{sub 2}O{sub 3}) thin films by pulsed laser deposition (PLD) in vacuum at room temperature from a pure Eu{sub 2}O{sub 3} ceramic bulk target. The films were deposited in different configurations formed by adding capping and/or buffer layers of amorphous aluminum oxide (a-Al{sub 2}O{sub 3}). The optical properties, refractive index and extinction coefficient of the as deposited Eu{sub 2}O{sub 3} layers were obtained. X-ray photoelectron spectroscopy (XPS) measurements were done to assess its chemical composition. Post-deposition annealing was performed at 500 °C and 850 °C in air in order to achieve the formation of crystalline films and to accomplish photoluminescence emission. According to the analysis of X-ray diffraction (XRD) spectra, cubic and monoclinic phases were formed. It is found that the relative amount of the phases is related to the different film configurations, showing that the control over the crystallization phase can be realized by adequately designing the structures. All the films showed photoluminescence emission peaks (under excitation at 355 nm) that are attributed to the intra 4f-transitions of Eu{sup 3+} ions. The emission spectral shape depends on the crystalline phase of the Eu{sub 2}O{sub 3} layer. Specifically, changes in the hypersensitive {sup 5}D{sub 0} → {sup 7}F{sub 2} emission confirm the strong influence of the crystal field effect on the Eu{sup 3+} energy levels.

  15. 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

  16. One-Electron Physics of the Actinides

    OpenAIRE

    Toropova, A.; Marianetti, C. A.; Haule, K.; Kotliar, G.

    2007-01-01

    We present a detailed analysis of the one-electron physics of the actinides. Various LMTO basis sets are analyzed in order to determine a robust bare Hamiltonian for the actinides. The hybridization between f- an spd- states is compared with the f-f hopping in order to understand the Anderson-like and Hubbard-like contributions to itineracy in the actinides. We show that both contributions decrease strongly as one move from the light actinides to the heavy actinides, while the Anderson-like c...

  17. 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

  18. Separations of actinides, lanthanides and other metals

    Science.gov (United States)

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

    1995-01-01

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

  19. 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)

  20. Vanadium sesquioxide (V2O3)-based semiconducting temperature sensitive resistors for uncooled microbolometers

    Science.gov (United States)

    Abdel-Rahman, Mohamed; Alduraibi, Mohammad; Zia, Muhammad Fakhar; Bahidra, Esme; Alasaad, Amr

    2017-05-01

    This paper reports on a semiconducting resistor material based on vanadium sesquioxide (V2O3) with electrical resistivity and temperature coefficient of resistance (TCR) appropriate for microbolometer applications. In this work, V2O3-based semiconducting resistor material was synthesized and electrically characterized. The developed material was prepared by annealing, in O2 and N2 atmospheres, a cascaded multilayer structure composed of V2O3 (10 nm) and V (5 nm) room temperature sputter coated thin films. The developed 55 nm thin film microbolometer resistor material possessed high temperature sensitivity from 20∘C to 45∘C with a TCR of -3.68%/∘C and room temperature resistivity of 0.57 Ω ṡcm for O2 annealed samples and a TCR of -3.72%/∘C and room temperature resistivity of 0.72 Ω ṡcm for N2 annealed samples. The surface morphologies of the synthesized thin films were studied using atomic force microscopy showing no significant post-growth annealing effect on the smoothness of the samples surfaces.

  1. 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)

  2. 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

  3. 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

  4. Chronic tubulointerstitial changes induced by germanium dioxide in comparison with carboxyethylgermanium sesquioxide.

    Science.gov (United States)

    Sanai, T; Okuda, S; Onoyama, K; Oochi, N; Takaichi, S; Mizuhira, V; Fujishima, M

    1991-11-01

    Chronic nephrotoxicity was investigated in rats orally administered germanium dioxide (GeO2) and carboxyethylgermanium sesquioxide (Ge-132) for 24 weeks. Increased BUN and serum phosphate as well as decreased creatinine clearance, weight loss, anemia and liver dysfunction were apparent at week 24 only in the GeO2 treated group. Vacuolar degeneration and granular depositions were observed by light microscope in the degenerated renal distal tubules in the rats of this group, with the semiquantitative scores of tubular degeneration being 95 +/- 9% in the GeO2 group, 3 +/- 1% in the Ge-132 group and 1 +/- 1% in the control group, respectively. Electron microscopy revealed electron-dense inclusions in the swollen mitochondrial matrix of the distal tubular epithelium in the GeO2 group. Although systemic toxicities were reduced after GeO2 was discontinued at week 24, renal tubulointerstitial fibrosis became prominent even at week 40 (16 weeks after discontinuation). A Ge.K alpha X-ray spectrum was clearly demonstrated in the mitochondrial matrix of the distal tubular epithelium in the GeO2 group with the help of electron probe X-ray microanalysis. On the other hand, neither toxic effects nor renal histological abnormalities were manifested in either the Ge-132 or the control group. The renal tissue content of germanium was high at weeks 24 and 40 in the GeO2 group. From these results, it is concluded that GeO2 causes characteristic nephropathy while Ge-132 does not. In addition, it appears that residual GeO2 remains for a considerably long time even after the cessation of GeO2 intake.

  5. Pharmacokinetics of germanium after po beta-carboxyethylgermanium sesquioxide in 24 Chinese volunteers.

    Science.gov (United States)

    Long, Q C; Zeng, G X; Zhao, X L

    1996-09-01

    To compare the pharmacokinetics after po different doses of beta-carboxyethylgermanium sesquioxide (Ge-132). An atomic absorption spectrophotometric system was used to measure germanium concentrations in plasma and urine samples after po Ge-132 1 (low dose, LD), 2.5 (medium dose, MD), and 4 (high dose, HD) g.m-2 in 24 healthy volunteers (one dose per 8 subjects). T1/2 alpha (LD, 1.2 +/- 0.7 h; MD, 1.1 +/- 0.6 h; HD, 1.2 +/- 0.5 h), T1/2 beta (LD, 5.2 +/- 1.2 h; MD, 5.8 +/- 2.5 h; HD, 5.5 +/- 1.4 h) and Cl/F (LD, 33 +/- 12 L.h-1; MD, 35 +/- 10 L.h-1; HD, 33 +/- 11 L.h-1) were not dose-related. Tmax was between 0.75 h and 2 h. Cmax (LD, 5.3 +/- 2.2 mg.L-1; MD, 13 +/- 5 mg.L-1; HD 18 +/- 8 mg.L-1, HD) and AUC (LD, 31 +/- 13 mg.h.L-1; MD, 60 +/- 16 mg.h.L-1; HD, 79 +/- 42 mg.h.L-1) were positive correlation to the dose of Ge-132. Urine-eliminated germanium within 24 h accounted for 11 +/- 3% of LD, 9 +/- 3% of MD, and 6 +/- 5% of HD (calculated from Ge/F) and showed a negative correlation to the dose. 1) Intracorporal process of Ge after po Ge-132 coincided with the first-order absorption and elimination with two-compartment kinetic model; 2) The amount of germanium eliminated in urine was below 11%.

  6. Structural and vibrational study of C-type doped rare earth sesquioxide Yb2-xCoxO3

    International Nuclear Information System (INIS)

    Farhat, L. Ben; Amami, M.; Hlil, E.K.; Hassen, R. Ben

    2009-01-01

    Polycrystalline samples with general formula Yb 2-x Co x O 3 (0 2 O 3 sesquioxide. The lattice parameters are found to vary linearly with the composition x. The cationic distribution over the two non-equivalent sites 8b and 24d of the space group Ia-3 is found to be preferentially. Replacing Yb 3+ by Co 3+ introduces slight changes in the atomic coordinates leading to an increase of the mean cation-anion distances. The ability of Raman spectroscopy to detect changes in local co-ordination is utilized. A pseudo-tetrahedral coordination for the Co 3+ in the 24d site was found.

  7. 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

  8. 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

  9. Perturbed-angular-correlation study of the electric-field gradient in 181Hf-doped and implanted indium sesquioxide

    International Nuclear Information System (INIS)

    Renteria, M.; Requejo, F.G.; Bibiloni, A.G.; Pasquevich, A.F.; Shitu, J.; Freitag, K.

    1997-01-01

    We studied the hyperfine interactions of 181 Ta in In 2 O 3 by means of perturbed-angular-correlation (PAC) measurements. We prepared thin films of indium sesquioxide with different degrees of initial amorphism and implanted them with 181 Hf. Chemically prepared indium-sesquioxide powder samples were also made starting from neutron-irradiated HfCl 4 , which provides the 181 Hf PAC probes. PAC experiments were performed on each sample at room temperature, after each step of annealing programs at increasing temperatures up to the full crystallization of the samples. The results indicate that the PAC probe occupies preferentially the axially symmetric cation site. Point-charge-model calculations were performed. The calculated asymmetry parameters η were compared with those obtained in 181 Hf PAC experiments performed also on other binary oxides, showing that the symmetry of the electric-field-gradient (EFG) tensor at 181 Ta cation sites in binary oxides is mainly determined by the nearest-neighbor oxygen-ion distribution around the probe. Comparisons of the experimental results in bixbyites obtained for both PAC probes, 111 Cd and 181 Ta, show that the local EFG in bixbyites, are strongly dependent on the geometry of the sites and the electronic configuration of the probes. copyright 1997 The American Physical Society

  10. 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.

  11. 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....

  12. Low-temperature magnetic ordering and structural distortions in vanadium sesquioxide V2O3

    Science.gov (United States)

    Grieger, Daniel; Fabrizio, Michele

    2015-08-01

    Vanadium sesquioxide (V2O3 ) is an antiferromagnetic insulator below TN≈155 K . The magnetic order does not consist of only antiferromagnetic nearest-neighbor bonds, possibly excluding the interplane vanadium pairs, as one would infer from the bipartite character of the hexagonal basal plane in the high-temperature corundum structure. In fact, a magnetic structure with one ferromagnetic bond and two antiferromagnetic ones in the honeycomb plane is known experimentally to be realized, accompanied by a monoclinic distortion that makes the ferromagnetic bond inequivalent from the other two. We show here that the magnetic ordering, the accompanying monoclinic structural distortion, the magnetic anisotropy, and also the recently discovered high-pressure nonmagnetic monoclinic phase, can all be accurately described by conventional electronic structure calculations within GGA and GGA+U . Remarkably, our calculations yield that the corundum phase would be unstable to a monoclinic distortion even without magnetic ordering, thus suggesting that magnetism and lattice distortion are independent phenomena, though they reinforce each other. By means of GGA+U , we find a metal-to-insulator transition at a critical Uc. Both metal at U ≤Uc and insulator above Uc have the same magnetic order as that actually observed below TN, but different monoclinic distortions. Reassuringly, the distortion on the insulating side agrees with the experimental one. Our results are in line with DMFT calculations for the paramagnetic phase [A. I. Poteryaev et al., Phys. Rev. B 76, 085127 (2007)], 10.1103/PhysRevB.76.085127, which predict that the insulating character is driven by a correlation-enhanced crystal-field splitting between egπ and a1 g orbitals that pushes the latter above the chemical potential. We find that the a1 g orbital, although almost empty in the insulating phase, is actually responsible for the unusual magnetic order as it leads to magnetic frustration whose effect is similar

  13. Advances in chemistry of the actinide elements

    International Nuclear Information System (INIS)

    Morss, L.R.

    1984-01-01

    Recent research accomplishments that elucidate the bonding and reactivity of the actinides are highlighted in this review. Improved syntheses of protactinium and transplutonium metals and compounds have led to determination of physical properties that reveal effects of 5f interactions. Thermodynamic measurements on metals, aqueous ions, and oxides have yielded more systematic understanding of the chemistry of the entire actinide series. Advances in bonding include the preparation of new organoactinide compounds with strong sigma and π metal-carbon and metal-hydrogen bonds; the development of new actinide complexing, sequestering, and extracting agents; and the study of chemical consequences of radioactive decay on oxides and halides. New techniques that impact actinide chemistry are laser fluorescence and photochemistry, radiocoulometry, and pulse radiolysis. Progress has also been made in outlining the basic chemical behavior of the heaviest actinides and the transactinides. (orig.)

  14. Exploring actinide materials through synchrotron radiation techniques.

    Science.gov (United States)

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

    2014-12-10

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

  15. 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.

  16. Separation of actinides from lanthanides

    Science.gov (United States)

    Smith, Barbara F.; Jarvinen, Gordon D.; Ryan, Robert R.

    1989-01-01

    An organic extracting solution and an extraction method useful for separating elements of the actinide series of the periodic table from elements of the lanthanide series, where both are in trivalent form. The extracting solution consists of a primary ligand and a secondary ligand, preferably in an organic solvent. The primary ligand is a substituted monothio-1,3-dicarbonyl, which includes a substituted 4-acyl-2-pyrazolin-5-thione, such as 4-benzoyl-2,4-dihydro-5-methyl-2-phenyl-3H-pyrazol-3-thione (BMPPT). The secondary ligand is a substituted phosphine oxide, such as trioctylphosphine oxide (TOPO).

  17. 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)

  18. Forecasting of physicochemical properties of rare earth sesquioxides on the base of their electronic structure in condensed state using electronic computer

    International Nuclear Information System (INIS)

    Kutolin, S.A.; Kotyukov, V.I.; Komarova, S.N.; Smirnova, E.G.

    1980-01-01

    A functional dependence between physicochemical properties of rare earth sesquioxides and energy state of rare earth atom sublattice valent electrons in sesquioxides is found out. The results of calculation of a simplified zone strucrure of rare earth sesquioxides are presented. The energy of the band of metal sublattice valent electrons for rare earth oxides is presented by the Chebyshev coefficients and polynomials and is calculated in the atomic units of mass. The density, melting points, standard change of enthalpy entropy, free energy, specific heat, standard entropy, forbidden zone width, static permitivity with a relative error of 10-12%, and thermal value of seeming activation energy, tangent of a dielectric losses angle, puncture voltage in rare earth oxides with a relative error of 20% are calculated on the base of calculation of electronic structure of rare earth sesquioxide in a condensed state and regression equations of calculation of oxide physicochemical properties. It is shown that only the Chebyshev coefficients determining the metal sublattice electronic structure in an oxide are ''information'' ones, i e. they contribute into the quantitative description of the system

  19. 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

  20. 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.)

  1. Sensitivity studies and actinide nuclear data requirements

    International Nuclear Information System (INIS)

    Sola, A.; Caruso, K.

    1978-01-01

    Some problems met when using sensitivities are discussed in the first part of the paper, such as the choice of a definition for the sensitivity, the usual lack of a linear relationship between the relative error on the concentration and the relative error on the parameter on which it depends, the strong dependence of the sensitivities on the neutron flux and the question of compound sensitivities, such as those which are obtained when the reactor power is kept constant. All information pertinent to the evaluation of a given sensitivity should alway be given with the numerical value of the sensitivity. An analytical method of evaluation of the sensitivities is described in the second part of the paper. This method has been applied satisfactorily to the determination of the sensitivities to various parameters of isotopes of the uranium, neptunium, plutonium, americium and curium series. The actinide nuclear data requirements for the two cases of actinide production and of actinide transmutation are not the same and need to be dealt with separately. For instance, the time length for which information on nuclear data is required is usually fairly well known in the case of actinide build-up, while it needs to be defined in the case of actinide transmutation; these lead to different values of the sensitivities. The flux dependence of the sensitivities may also be quite different for the two cases. These questions are discussed briefly in the third part of the paper where several data requirements concerning actinide production and actinide incineration are also given

  2. 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.

  3. 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)

  4. 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

  5. Electronic structure and magnetic properties of actinides

    International Nuclear Information System (INIS)

    Fournier, J.-M.

    1975-01-01

    The study of the actinide series shows the change between transition metal behavior and lanthanide behavior, between constant weak paramagnetism for thorium and strong Curie-Weiss paramagnetism for curium. Curium is shown to be the first metal of the actinide series to be magnetically ordered, its Neel temperature being 52K. The magnetic properties of the actinides depending on all the peripheral electrons, their electronic structure was studied and an attempt was made to determine it by means of a phenomenological model. Attempts were also made to interrelate the different physical properties which depend on the outer electronic structure [fr

  6. Electronic Structure of the Actinide Metals

    DEFF Research Database (Denmark)

    Johansson, B.; Skriver, Hans Lomholt

    1982-01-01

    Some recent experimental photoelectron spectroscopic results for the actinide metals are reviewed and compared with the theoretical picture of the basic electronic structure that has been developed for the actinides during the last decade. In particular the experimental data confirm the change from...... itinerant to localized 5f electron behaviour calculated to take place between plutonium and americium. From experimental data it is shown that the screening of deep core-holes is due to 5f electrons for the lighter actinide elements and 6d electrons for the heavier elements. A simplified model for the full...

  7. Spin and orbital moments in actinide compounds

    DEFF Research Database (Denmark)

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

    1991-01-01

    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......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...

  8. 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.

  9. 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

  10. Actinide removal from spent salts

    Science.gov (United States)

    Hsu, Peter C.; von Holtz, Erica H.; Hipple, David L.; Summers, Leslie J.; Adamson, Martyn G.

    2002-01-01

    A method for removing actinide contaminants (uranium and thorium) from the spent salt of a molten salt oxidation (MSO) reactor is described. Spent salt is removed from the reactor and analyzed to determine the contaminants present and the carbonate concentration. The salt is dissolved in water, and one or more reagents are added to precipitate the thorium as thorium oxide and/or the uranium as either uranium oxide or as a diuranate salt. The precipitated materials are filtered, dried and packaged for disposal as radioactive waste. About 90% of the thorium and/or uranium present is removed by filtration. After filtration, salt solutions having a carbonate concentration >20% can be dried and returned to the reactor for re-use. Salt solutions containing a carbonate concentration salt solutions that contain less than 0.1 ppm of thorium or uranium.

  11. 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

  12. 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

  13. Thermochemistry of a Biomimetic and Rubisco-Inspired CO2 Capture System from Air

    OpenAIRE

    Andrew Muelleman; Joseph Schell; Spencer Glazer; Rainer Glaser

    2016-01-01

    In theoretical studies of chemical reactions the reaction thermochemistry is usually reported for the stoichiometric reaction at standard conditions (ΔG°, ΔH°, ΔS°). We describe the computation of the equilibrium concentrations of the CO2-adducts for the general capture reaction CO2 + Capture System ⇆ CO2-adduct (GCR) and the rubisco-type capture reaction CO2 + Capture System ⇆ CO2-adduct + H2O (RCR) with consideration of the reaction CO2(g) ⇆ CO2(aq) via Henry’s law. The resulting equations ...

  14. Actinide absorption from the gastrointestinal tract

    International Nuclear Information System (INIS)

    Sullivan, M.F.

    1981-01-01

    A summary of our research is presented, describing the importance of the animal species, route of entry, oxidation state, solubility, and organic binding on the absorption of actinides from the gastrointestinal tract. The animal species tested made little difference in absorption, nor was the oxidation state a major factor in plutonium absorption under nonfasting conditions. The organic binding of actinides to either plant or animal tissues resulted in a 2- to 4-fold increase, except for 237 Np, which caused a 10-fold decrease. The age of the animals was the major influence on absorption. In all species studied, neonates absorbed more actinide than did the adults by two or three orders of magnitude. Retention of the actinide in the intestinal mucosa of rats and swine amounted to about half the dose of 238 Pu-nitrate administered; both after gavage and inhalation

  15. 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.)

  16. 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.

  17. 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

  18. 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).

  19. 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.

  20. 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.

  1. 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.)

  2. 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

  3. 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)

  4. Recovery yield of nuclides required for satisfactory actinide recycling

    International Nuclear Information System (INIS)

    Yamana, Hajimu; Shiotsuki, Masao.

    1996-01-01

    In order to establish a visual target of actinide recovery in the actinide recycling, a rough evaluation on the required recovery yield for actinide nuclides was performed. The tendency of actinide's flow-out from actinide recycling fuel cycle was studied with a simple mathematical model. Desired magnitude of confinement of actinides was studied with analysis on the cumulative radiotoxicity going to be produced in the Japanese future period. By estimating loss factors for actinides at various waste streams of the fuel cycle, their impacts on the magnitude of total loss was studied under realistic condition of MOX-FBR system. It was concluded that, for satisfying severe goal of confinement of actinides in the actinide recycling system using MOX-FBR, drastic improvements will be required for the loss at intermediate level waste streams of reprocessing and fabrication. (author)

  5. Actinides and the sources of cosmic rays

    Science.gov (United States)

    Pfeiffer, B.; Kratz, K.-L.; Lingenfelter, R. E.; Higdon, J. C.

    2004-02-01

    The abundances of the actinide elements in the cosmic rays can provide critical constraints on the major sites of their acceleration. Using recent calculations of the r-process yields in core-collapse supernovae (SNe), we have determined the actinide abundances averaged over various assumed time intervals for their supernovae generation and their cosmic-ray acceleration. Using standard Galactic chemical evolution models, we have also determined the expected actinide abundances in the present interstellar medium. From these two components, we have calculated the U/Th and other actinide abundances expected in the SN-active cores of superbubbles, as a function of their ages and mean metallicity. We calculate the expected actinide abundances in cosmic-rays accelerated by Galactic SNe. We find that the current measurements of actinide/Pt-group and preliminary estimates of the UPuCM/Th ratio in cosmic rays are all consistent with the expected values if superbubble cores have mean metallicities of around three times solar. Future measurements of the abundance ratios will help to solve these questions. First results of experiments performed on the MIR space station (ECCO) and with balloon flights (TIGER) are promising.

  6. 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

  7. Active Thermochemical Tables: Sequential Bond Dissociation Enthalpies of Methane, Ethane, and Methanol and the Related Thermochemistry

    Energy Technology Data Exchange (ETDEWEB)

    Ruscic, Branko

    2015-07-16

    Active Thermochemical Tables (ATcT) thermochemistry for the sequential bond dissociations of methane, ethane, and methanol systems were obtained by analyzing and solving a very large thermochemical network (TN). Values for all possible C–H, C–C, C–O, and O–H bond dissociation enthalpies at 298.15 K (BDE298) and bond dissociation energies at 0 K (D0) are presented. The corresponding ATcT standard gas-phase enthalpies of formation of the resulting CHn, n = 4–0 species (methane, methyl, methylene, methylidyne, and carbon atom), C2Hn, n = 6–0 species (ethane, ethyl, ethylene, ethylidene, vinyl, ethylidyne, acetylene, vinylidene, ethynyl, and ethynylene), and COHn, n = 4–0 species (methanol, hydroxymethyl, methoxy, formaldehyde, hydroxymethylene, formyl, isoformyl, and carbon monoxide) are also presented. The ATcT thermochemistry of carbon dioxide, water, hydroxyl, and carbon, oxygen, and hydrogen atoms is also included, together with the sequential BDEs of CO2 and H2O. The provenances of the ATcT enthalpies of formation, which are quite distributed and involve a large number of relevant determinations, are analyzed by variance decomposition and discussed in terms of principal contributions. The underlying reasons for periodic appearances of remarkably low and/or unusually high BDEs, alternating along the dissociation sequences, are analyzed and quantitatively rationalized. The present ATcT results are the most accurate thermochemical values currently available for these species.

  8. Applying the Rule Space Model to Develop a Learning Progression for Thermochemistry

    Science.gov (United States)

    Chen, Fu; Zhang, Shanshan; Guo, Yanfang; Xin, Tao

    2017-12-01

    We used the Rule Space Model, a cognitive diagnostic model, to measure the learning progression for thermochemistry for senior high school students. We extracted five attributes and proposed their hierarchical relationships to model the construct of thermochemistry at four levels using a hypothesized learning progression. For this study, we developed 24 test items addressing the attributes of exothermic and endothermic reactions, chemical bonds and heat quantity change, reaction heat and enthalpy, thermochemical equations, and Hess's law. The test was administered to a sample base of 694 senior high school students taught in 3 schools across 2 cities. Results based on the Rule Space Model analysis indicated that (1) the test items developed by the Rule Space Model were of high psychometric quality for good analysis of difficulties, discriminations, reliabilities, and validities; (2) the Rule Space Model analysis classified the students into seven different attribute mastery patterns; and (3) the initial hypothesized learning progression was modified by the attribute mastery patterns and the learning paths to be more precise and detailed.

  9. Thermochemistry of a Biomimetic and Rubisco-Inspired CO2 Capture System from Air

    Directory of Open Access Journals (Sweden)

    Andrew Muelleman

    2016-07-01

    Full Text Available In theoretical studies of chemical reactions the reaction thermochemistry is usually reported for the stoichiometric reaction at standard conditions (ΔG°, ΔH°, ΔS°. We describe the computation of the equilibrium concentrations of the CO2-adducts for the general capture reaction CO2 + Capture System ⇆ CO2-adduct (GCR and the rubisco-type capture reaction CO2 + Capture System ⇆ CO2-adduct + H2O (RCR with consideration of the reaction CO2(g ⇆ CO2(aq via Henry’s law. The resulting equations are evaluated and graphically illustrated as a function of atmospheric CO2 concentration and as a function of temperature. The equations were applied to the thermochemistry of small molecule rubisco-model reactions and series of additional model reactions to illustrate the range of the Gibbs free enthalpy for the effective reversible capture and of the reaction entropy for economic CO2 release at elevated temperature. A favorable capture of free enthalpy is of course a design necessity, but not all exergonic reactions are suitable CO2 capture systems. Successful CO2 capture systems must allow for effective release as well, and this feature is controlled by the reaction entropy. The principle of using a two-pronged capture system to ensure a large negative capture entropy is explained and highlighted in the graphical abstract. It is hoped that the presentation of the numerical examples provides useful guidelines for the design of more efficient capture systems.

  10. 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).

  11. 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.

  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. 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 pc ) 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

  14. 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.

  15. 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

  16. Ultratrace analysis of transuranic actinides by laser-induced fluorescence

    Science.gov (United States)

    Miller, Steven M.

    1988-01-01

    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.

  17. 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...

  18. RECOVERY OF ACTINIDES FROM AQUEOUS NITRIC ACID SOLUTIONS

    Science.gov (United States)

    Ader, M.

    1963-11-19

    A process of recovering actinides is presented. Tetravalent actinides are extracted from rare earths in an aqueous nitric acid solution with a ketone and back-extracted from the ketone into an aqueous medium. The aqueous actinide solution thus obtained, prior to concentration by boiling, is sparged with steam to reduce its ketone to a maximum content of 3 grams per liter. (AEC)

  19. 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

  20. 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

  1. 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

  2. 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

  3. 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)

  4. 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....

  5. 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.)

  6. Ro-vibrational coupling in high temperature thermochemistry of the BBr molecule

    Science.gov (United States)

    Buchowiecki, Marcin

    2018-01-01

    High temperature thermochemistry of the BBr molecule is investigated with the classical approach in the temperature range of 300-20,000 K. The role of ro-vibrational coupling is elucidated. The internal partition function, thermal energy, heat capacity, and entropy are calculated at three levels of approximation, i.e. taking into account bound states on the ground state (1 Σ), including also two excited states (3 Π and 1 Π), and finally adding the resonance and scattering states. The influence of these approximations on studied quantities is investigated. The entropy is found to be the least sensitive to approximations in the ro-vibrational coupling and the heat capacity the most sensitive.

  7. 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

  8. 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

  9. 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

  10. Separation method of trivalent actinide and rare earth element

    International Nuclear Information System (INIS)

    Koma, Yoshikazu; Watabe, Masayuki; Nemoto, Shin-ichi.

    1997-01-01

    Trivalent actinides and rare earth elements are extracted to a solvent from highly acidic liquid wastes generated upon reprocessing of spent fuels. The concentration of nitric acid in the extracted solvent is reduced. Trivalent actinides and the rare earth elements contained in the solvent at low nitric acid concentration are separated from each other. Trivalent actinides and rare earth elements are extracted into a highly acidic solvent in the extracting step of trivalent actinides and rare earth elements. On the other hand, they can be separated by extraction only at a predetermined pH in the separation step of the rare earth elements and trivalent actinides. In the present invention, trivalent actinides and rare earth elements are separated after removing a predetermined amount of nitric acid from the solution obtained in the trivalent actinide and rare earth element extraction step to provide a proper acidic concentration. Accordingly, they can be separated satisfactorily. (T.M.)

  11. 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...

  12. 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

  13. 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.)

  14. 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

  15. 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

  16. Actinide and fission product partitioning and transmutation

    International Nuclear Information System (INIS)

    1995-01-01

    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.)

  17. 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

  18. 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

  19. 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)

  20. 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.

  1. Plutonium Futures -- The Science. Topical Conference on Plutonium and Actinides. AIP Conference Proceedings, No. 532 [APCPCS

    International Nuclear Information System (INIS)

    Pillay, K.K.S.; Kim, K.C.

    2000-01-01

    Presentations at this conference covered the topics of materials science/nuclear fuels, condensed matter physics, actinides in the environment/separation and analysis, actinides/processing, actinides/TRU wastes, materials science, TRU waste forms, nuclear fuels/isotopes, separations and process chemistry, actinides in the environment, detection and analysis, Pu and Pu compounds, actinide compounds and complexes

  2. 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

  3. 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

  4. 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.

  5. Processing of low-quality bauxite feedstock by thermochemistry-Bayer method

    Directory of Open Access Journals (Sweden)

    О. А. Дубовиков

    2016-11-01

    Full Text Available The modern production of aluminum which by its global output ranks first among the non-ferrous metals includes three main stages: ore extraction, its processing into alumina and, finally, the production of primary aluminum. Alumina production from bauxites,  being the  primary raw material in the  alumina industry,  is based  on two main methods: the Bayer method and the sintering method developed in Russia under the lead of an academician Nikolay Semenovich Kurnakov. Alumina production by the Bayer’s method is more cost effective,  but  has  higher  requirements to the  quality of the bauxite feedstock.  A great deal  of research has  been carried  out on low quality bauxites focusing firstly on finding ways to enrich the feedstock, secondly on improving the combined sequential Bayer-sintering method and thirdly on developing new hydrometallurgical ways for bauxites processing. Mechanical methods of bauxite enrichment have not yet brought any positive outcome, and a development of new hydrometallurgical high alkaline  autoclave process  faced  significant hardware  difficulties not addressed so far. For efficient processing of such low quality bauxite feedstock it is suggested to use a universal thermochemistry-Bayer method, which was developed in St. Petersburg Mining University under  the lead  of  Nikolay Ivanovich Eremin, allows to process different substandard bauxite feedstock and has a competitive costing as compared to the sintering method and combined methods. The main stages of thermochemistry-Bayer method are thermal activation of feedstock, its further desiliconization with the alkaline solution and leaching of the resultant bauxite product  under Bayer’s method. Despite high energy consumption at  the baking stage,  it  allows to condition the  low quality bauxite feedstock by neutralizing a variety of technologically harmful impurities such as organic matter, sulfide sulfur, carbonates, and at the

  6. 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

  7. 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)

  8. Actinide Isotopes for the Synthesis of Superheavy Nuclei

    Science.gov (United States)

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

    2014-09-01

    Recent research resulting in the synthesis of isotopes of new elements 113-118 has demonstrated the importance of actinide targets in superheavy element research. Oak Ridge National Laboratory (ORNL) has unique facilities for the production and processing of actinide target materials, including the High Flux Isotope Reactor (HFIR) and the Radiochemical Engineering Development Center (REDC). These facilities have provided actinide target materials that have been used for the synthesis of all superheavy (SHE) elements above Copernicium (element 112). In this paper, the use of actinide targets for SHE research and discovery is described, including recent results for element 117 using 249Bk target material from ORNL. ORNL actinide capabilities are reviewed, including production and separation/purification, availabilities of actinide materials, and future opportunities including novel target materials such as 251Cf.

  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. Microbial Transformations of Actinides and Other Radionuclides

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-01-07

    Microorganisms can affect the stability and mobility of the actinides and other radionuclides released from nuclear fuel cycle and from nuclear fuel reprocessing plants. Under appropriate conditions, microorganisms can alter the chemical speciation, solubility and sorption properties and thus could increase or decrease the concentrations of radionuclides in solution in the environment and the bioavailability. Dissolution or immobilization of radionuclides is brought about by direct enzymatic action or indirect non-enzymatic action of microorganisms. Although the physical, chemical, and geochemical processes affecting dissolution, precipitation, and mobilization of radionuclides have been extensively investigated, we have only limited information on the effects of microbial processes and biochemical mechanisms which affect the stability and mobility of radionuclides. The mechanisms of microbial transformations of the major and minor actinides U, Pu, Cm, Am, Np, the fission products and other radionuclides such as Ra, Tc, I, Cs, Sr, under aerobic and anaerobic conditions in the presence of electron donors and acceptors are reviewed.

  11. 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

  12. 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.)

  13. Actinide and fission product partitioning and transmutation

    International Nuclear Information System (INIS)

    1997-01-01

    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.)

  14. 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.)

  15. Separation of Californium from other Actinides

    Science.gov (United States)

    Mailen, J C; Ferris, L M

    1973-09-25

    A method is provided for separating californium from a fused fluoride composition containing californium and at least one element selected from the group consisting of plutonium, americium, curium, uranium, thorium, and protactinium which comprises contacting said fluoride composition with a liquid bismuth phase containing sufficient lithium or thorium to effect transfer of said actinides to the bismuth phase and then contacting the liquid bismuth phase with molten LiCl to effect selective transfer of californium to the chloride phase.

  16. 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

  17. 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

  18. 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

  19. Actinide and lanthanide separation process (ALSEP)

    Science.gov (United States)

    Guelis, Artem V.

    2013-01-15

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

  20. 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.

  1. 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.

  2. 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

  3. Uranium hexafluoride actinide transmutation reactors--preliminary design and analysis

    International Nuclear Information System (INIS)

    Wan, P.T.

    1981-01-01

    The long term hazard potential of high-level wastes from fission reactors can be reduced significantly by partitioning waste actinides from the bulk wastes and transmuting them to short-lived or stable fission product nuclides by neutron bombardment. The objectives of the present work are to establish the waste actinide transmutation performance of a uranium hexafluoride actinide transmutation reactor (UHATR) and to ascertain if it has any special advantages over light water reactors (LWRs). Using present day and near term technology, a preliminary UHATR design was defined. The reactor core consists of a cylindrical cavity filled with a mixture of U 233 F 6 and helium, surrounded on all sides by graphite. An annular actinide blanket is embedded in the graphite. Each actinide element is stainless steel clad, helium cooled and graphite moderated. Very high thermal neutron fluxes, from 10 14 to 10 15 n/cm 2 -sec, were obtained in the actinide region. For one UHATR design, calculations showed that out of 250 kg of waste actinides charged, about 75 kg net is converted to fission products after 220 days of irradiation. This is equivalent to an average waste actinide fission rate of 50% calendar year of irradiation. Compared with an LWR, the average blanket thermal flux of this UHATR is about ten to thirty times higher, leading a fifteen fold improvement in the actinide fission rate

  4. 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.)

  5. Perturbed-angular-correlation study of the electric-field gradient in {sup 181}Hf-doped and implanted indium sesquioxide

    Energy Technology Data Exchange (ETDEWEB)

    Renteria, M.; Requejo, F.G.; Bibiloni, A.G.; Pasquevich, A.F.; Shitu, J. [Departamento de Fisica, Facultad de Ciencias Exactas, Universidad Nacional de La Plata, CC N67, 1900 La Plata (Argentina); Freitag, K. [Institut fuer Strahlen- und Kernphysik der Universitaet Bonn, Nussallee 14-16, 5300 Bonn (Germany)

    1997-06-01

    We studied the hyperfine interactions of {sup 181}Ta in In{sub 2}O{sub 3} by means of perturbed-angular-correlation (PAC) measurements. We prepared thin films of indium sesquioxide with different degrees of initial amorphism and implanted them with {sup 181}Hf. Chemically prepared indium-sesquioxide powder samples were also made starting from neutron-irradiated HfCl{sub 4}, which provides the {sup 181}Hf PAC probes. PAC experiments were performed on each sample at room temperature, after each step of annealing programs at increasing temperatures up to the full crystallization of the samples. The results indicate that the PAC probe occupies preferentially the axially symmetric cation site. Point-charge-model calculations were performed. The calculated asymmetry parameters {eta} were compared with those obtained in {sup 181}Hf PAC experiments performed also on other binary oxides, showing that the symmetry of the electric-field-gradient (EFG) tensor at {sup 181}Ta cation sites in binary oxides is mainly determined by the nearest-neighbor oxygen-ion distribution around the probe. Comparisons of the experimental results in bixbyites obtained for both PAC probes, {sup 111}Cd and {sup 181}Ta, show that the local EFG in bixbyites, are strongly dependent on the geometry of the sites and the electronic configuration of the probes. {copyright} {ital 1997} {ital The American Physical Society}

  6. Elementary Steps of Syngas Reactions on Mo2C(001): Adsorption Thermochemistry and Bond Dissociation

    Energy Technology Data Exchange (ETDEWEB)

    Medford, Andrew

    2012-02-16

    Density functional theory (DFT) and ab initio thermodynamics are applied in order to investigate the most stable surface and subsurface terminations of Mo{sub 2}C(001) as a function of chemical potential and in the presence of syngas. The Mo-terminated (001) surface is then used as a model surface to evaluate the thermochemistry and energetic barriers for key elementary steps in syngas reactions. Adsorption energy scaling relations and Broensted-Evans-Polanyi relationships are established and used to place Mo{sub 2}C into the context of transition metal surfaces. The results indicate that the surface termination is a complex function of reaction conditions and kinetics. It is predicted that the surface will be covered by either C{sub 2}H{sub 2} or O depending on conditions. Comparisons to transition metals indicate that the Mo-terminated Mo{sub 2}C(001) surface exhibits carbon reactivity similar to transition metals such as Ru and Ir, but is significantly more reactive towards oxygen.

  7. Large eddy simulation of hydrogen/air scramjet combustion using tabulated thermo-chemistry approach

    Directory of Open Access Journals (Sweden)

    Cao Changmin

    2015-10-01

    Full Text Available Large eddy simulations (LES have been performed to investigate the flow and combustion fields in the scramjet of the German Aerospace Center (DLR. Turbulent combustion is modeled by the tabulated thermo-chemistry approach in combination with the presumed probability density function (PDF. A β-function is used to model the distribution of the mixture fraction, while two different PDFs, δ-function (Model I and β-function (Model II, are applied to model the reaction progress. Temperature is obtained by solving filtered energy transport equation and the reaction rate of the progress variable is rescaled by pressure to consider the effects of compressibility. The adaptive mesh refinement (AMR technique is used to properly capture shock waves, boundary layers, shear layers and flame structures. Statistical results of temperature and velocity predicted by Model II show better accuracy than that predicted by Model I. The results of scatter points and mixture fraction-conditional variables indicate the significant differences between Model I and Model II. It is concluded that second moment information in the presumed PDF of the reaction progress is very important in the simulation of supersonic combustion. It is also found that an unstable flame with extinction and ignition develops in the shear layers of bluff body and a fuel-rich partially premixed flame stabilizes in the central recirculation bubble.

  8. Computational studies of the thermochemistry for conversion of glucose to levulinic acid.

    Science.gov (United States)

    Assary, Rajeev S; Redfern, Paul C; Hammond, Jeff R; Greeley, Jeffrey; Curtiss, Larry A

    2010-07-15

    The thermochemistry of the conversion of glucose to levulinic acid through fructofuranosyl intermediates is investigated using the high-level ab initio methods G4 and G4MP2. The calculated gas phase reaction enthalpies indicate that the first two steps involving water molecule elimination are highly endothermic, while the other steps, including additional water elimination and rehydration to form levulinic acid, are exothermic. The calculated gas phase free energies indicate that inclusion of entropic effects makes the dehydration steps more favorable, although the elimination of the first water is still endothermic. Elevated temperatures and aqueous reaction environments are also predicted to make the dehydration reaction steps thermodynamically more favorable. On the basis of these enthalpy and free energy calculations, the first dehydration step in conversion of glucose to levulinic acid is likely a key step in controlling the overall progress of the reaction. An assessment of density functional theories and other theoretical methods for the calculation of the dehydration and hydration reactions in the decomposition of glucose is also presented.

  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. Extraction of DBP and MBP from actinides: application to the recovery of actinides from TBP-sodium carbonate scrub solutions

    International Nuclear Information System (INIS)

    Horwitz, E.P.; Mason, G.W.; Bloomquist, C.A.A.; Leonard, R.A.; Bernstein, G.J.

    1980-01-01

    A flowsheet for the recovery of actinides from TBP-Na 2 CO 3 scrub waste solutions has been developed, based on batch extraction data, and tested, using laboratory scale counter-current extraction techniques. The process, called the ARALEX process, utilizes 2-ethyl-1-hexanol (2-EHOH) to extract the TBP degradation products (HDBP and H 2 MBP) from acidified Na 2 CO 3 scrub waste leaving the actinides in the aqueous phase. Dibutyl and monobutyl phosphoric acids are attached to the 2-EHOH molecules through hydrogen bonds. These hydrogen bonds also diminish the ability of the HDBP and H 2 MBP to complex actinides and thus all actinides remain in the aqueous raffinate. Dilute sodium hydroxide solutions can be used to back-extract the dibutyl and monobutyl phosphoric acid esters as their sodium salts. The 2-EHOH can then be recycled. After extraction of the acidified carbonate waste with 2-EHOH, the actinides may be readily extracted from the raffinate with DHDECMP or, in the case of tetra- and hexavalent actinides, with TBP. The ARALEX process is relatively simple and involves inexpensive and readily available chamicals. The ARALEX process can also be applied to other actinide waste streams which contain appreciable concentrations of polar organic compounds that interfere with conventional actinide ion exchange and liquid-liquid extraction procedures. One such application is the removal of detergents from laundry or clean-up solutions contaminated with actinides

  11. 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

  12. 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

  13. Actinide recycle in LMFBRs as a waste management alternative

    International Nuclear Information System (INIS)

    Beaman, S.L.

    1980-01-01

    A strategy of actinide burnup in LMFBRs has been investigated as a waste management alternative to long-term storage of high level nuclear waste. This strategy has been 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. By burning the actinides in LMFBRs the long-lived isotopes can be effectively transmuted to fission products which have significantly shorter half-lives. Actinide burnup in LMFBRs rather than LWRs is preferred because the fission to capture reaction rate ratios are higher in the LMFBR, and the LMFBR performance is not highly sensitive to the addition of the actinide waste material. An actinide target assembly recycle scheme has been analyzed to determine the effects of the actinides on the LMFBR performance, including local power peaking, breeding ratio, and fissile material requirements. The overall efficiency of actinide burnout in LMFBRs has been evaluated, and equilibrium cycle conditions have been determined. The results of the actinide recycle study indicate that the actinide wastes produced by a fission reactor economy could be transmuted in fast reactors with only a two percent penalty in the fissile loading requirements and a one to two percent penalty in the breeding ratio of the host reactors. The actinide target assemblies could be tailored to give a power distribution which is comparable to that of the standard fuel assemblies. However, the total shutdown decay heat from a target assembly would be approximately 43 percent greater than that from a standard assembly

  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. Properties and applications of actinide-based ceramics

    International Nuclear Information System (INIS)

    Beauvy, M.

    1985-01-01

    The uses of the ceramics containing actinides are described excluding nuclear fuels. Their thermomechanical properties and the reasons of their poor development at this time are detailed. The discovery of new original physical properties connected with the electronic structure of the actinides allows us to expect new uses for these ceramics. 7 references are given [fr

  17. Quantum chemistry of unusual oxidation degrees of lanthanides and actinides

    International Nuclear Information System (INIS)

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

    1984-01-01

    The electronic structure and properties of actinides in unusual valence forms were considered in the framework of quantum-mechanical concepts. Hartree-Fock atomic calculations of the actinide series as well as molecular orbital calculations of octahedral oxydions of uranium, neptuniun, plutonium and americium in hight and higher valence forms, octahedral tri-and tetravalent chloride complexes from protactinium through einsteinium were conducted. A possible existence of some new valence forms of actinides was considered, based on such calculations. The cation-cation interaction mechanism was suggested. Peculiarities of the trans-effect manifestation in actinide chemistry were considered. New possibilities were shown of using the Moessbauer isomer shifts on actinide nuclei to interpret the chemical properties. The influence of relativi;tic effects on the actinide chemical properties was analyzed. A high value of the spin-orbital splitting Was snown to determine a gradual stabilization and stability of bivalent state at the and of the actinide series, substantial difference in stability of the tetravalent state of lanthanides and actinides, conceptual possibility of preparing lanthanyl groups at the end of the lanthanide series

  18. Process for making a ceramic composition for immobilization of actinides

    Science.gov (United States)

    Ebbinghaus, Bartley B.; Van Konynenburg, Richard A.; Vance, Eric R.; Stewart, Martin W.; Walls, Philip A.; Brummond, William Allen; Armantrout, Guy A.; Herman, Connie Cicero; Hobson, Beverly F.; Herman, David Thomas; Curtis, Paul G.; Farmer, Joseph

    2001-01-01

    Disclosed is a process for making a ceramic composition for the immobilization of actinides, particularly uranium and plutonium. The ceramic is a titanate material comprising pyrochlore, brannerite and rutile. The process comprises oxidizing the actinides, milling the oxides to a powder, blending them with ceramic precursors, cold pressing the blend and sintering the pressed material.

  19. Improved method for extracting lanthanides and actinides from acid solutions

    Science.gov (United States)

    Horwitz, E.P.; Kalina, D.G.; Kaplan, L.; Mason, G.W.

    1983-07-26

    A process for the recovery of actinide and lanthanide values from aqueous acidic solutions uses a new series of neutral bi-functional extractants, the alkyl(phenyl)-N,N-dialkylcarbamoylmethylphosphine oxides. The process is suitable for the separation of actinide and lanthanide values from fission product values found together in high-level nuclear reprocessing waste solutions.

  20. Studied of actinide colloids in high-ionic strength groundwaters

    International Nuclear Information System (INIS)

    Kadkhodayan, B.; Zhao, P.; Marquez, L.N.

    1995-01-01

    Proposed plans for permanent disposal of transuranic wastes in geologic repositories require the development of an actinide source-term model that predicts the total concentrations of mobile actinides both near field and far-field environments. An actinide source-term model must quantify mobile actinide-bearing species, which may be present as dissolved species in several possible oxidation states or as suspended colloidal particles. In this presentation, we describe results of experiments with several actinides in Na-Ca-Mg-Cl-SO 4 brines with ionic strengths ranging from 0.8 to 8 molal, designed to assess the formation of intrinsic colloids (Eigenkollide or real colloids), and their temporal behavior e.g., changes in concentration and size. We have implemented a test matrix that provides us with the basis to understand the behavior of actinides with +3, +4, +5, and +6 oxidation states, as a function of pH (3 to 11) and actinide concentration (10 -8 - 10 -4 molar). Colloid sizes were estimated using sequential filtration and ultrafiltration techniques. Colloidal particles were characterized with scanning electron microscopy and energy-dispersive x-ray spectrometry. The oxidation states of the actinides were investigated with absorption spectroscopy

  1. 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)

  2. 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.)

  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. 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

  5. Chemical equilibria in actinide carbonate systems

    International Nuclear Information System (INIS)

    Grenthe, I.; Robouch, P.; Vitorge, P.

    1986-01-01

    By spectrophotometric and potentiometric methods it is shown that trimers are formed in media of high ionic strength (3 M NaClO 4 ) and total concentrations of hexavalent actinides higher than 10 -3 M. The equilibrium constants for the reactions 3 MO 2 (CO 3 ) 3 4- ↔ (MO 2 ) 3 (CO 3 ) 6 6- + 3 CO 3 2- are lg K(U)=-11.3±0.1; lg K(NP)=-10.1±0.1; lg K(Pu)=-7.4±0.2. It is demonstrated that one of the cations of the trimer can be exchanged with another actinide cation: the equilibrium constants for the reactions 2 UO 2 (CO 3 ) 3 4- + MO 2 (CO 3 ) 3 4- ↔ (UO 2 ) 2 MO 2 (CO 3 ) 6 6- + 3 CO 3 3- are lg K=-11.3±0.1, -10.0±0.2 and -8.8 respectively for M=U, Np, Pu. Thus, polynuclear complexes can be efficient solution ''carriers'' for other hexavalent actinides in waste disposal. Some properties of the solid phases MO 2 CO 3 (s) are discussed. Experimental studies of chemical equilibria of americium (III, IV) are reviewed: in carbonate media americium(III) species are AmCO 3 + , Am(CO 3 ) 2 - , Am(CO 3 ) 3 3- , (Am 2 (CO 3 ) 3 ) 6 and (NaAm(CO 3 ) 2 ) s ; for americium-(IV) lg β 5 ≅ 40. In 3 M NaClO 4 solubility measurements of neptunium(V) show that lg β 1 =5.09, lg β 2 =8.15, lg β 3 =10.46, lg Ks(NaNpO 2 CO 3 )=10.56 and lg Ks(Na 3 NpO 2 (CO 3 ) 2 )=12.44; ionic strength corrections are proposed on the basis of these results. (orig.)

  6. Actinide-Aluminate Speciation in Alkaline Radioactive Waste

    Energy Technology Data Exchange (ETDEWEB)

    Dr. David L. Clark; Dr. Alexander M. Fedosseev

    2001-12-21

    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.

  7. Actinides and Rare Earths Topical Conference (Code AC)

    International Nuclear Information System (INIS)

    Tobin, J.G.

    2009-01-01

    Actinide and the Rare Earth materials exhibit many unique and diverse physical, chemical and magnetic properties, in large part because of the complexity of their f electronic structure. This Topical Conference will focus upon the chemistry, physics and materials science in Lanthanide and Actinide materials, driven by 4f and 5f electronic structure. Particular emphasis will be placed upon 4f/5f magnetic structure, surface science and thin film properties. For the actinides, fundamental actinide science and its role in resolving technical challenges posed by actinide materials will be stressed. Both basic and applied experimental approaches, including synchrotron-radiation-based investigations, as well as theoretical modeling and computational simulations, are planned to be part of the Topical Conference. Of particular importance are the issues related to the potential renaissance in Nuclear Fuels, including synthesis, oxidation, corrosion, intermixing, stability in extreme environments, prediction of properties via benchmarked simulations, separation science, environmental impact and disposal of waste products.

  8. 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

  9. 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

  10. 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)

  11. 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.)

  12. 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.)

  13. 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.

  14. 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...

  15. The radiological impact of actinides discharged to the Irish Sea

    Energy Technology Data Exchange (ETDEWEB)

    Hunt, G.J.; Smith, B.D. [CEFAS Laboratory, Pakefield Road, Lowestoft, Suffolk (United Kingdom)

    1999-08-01

    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{sup -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.)

  16. 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.)

  17. THERMOCHEMISTRY OF INTERACTION REACTIONS FOR SODIUM AND ALUMINUM SULPHATES WITH COMPONENTS OF HYDRATING PORTLAND CEMENT

    Directory of Open Access Journals (Sweden)

    P. I. Yukhnevskiy

    2018-01-01

    Full Text Available Chemical additives are widely used in the technology of concrete with the purpose to solve various problems and sulphate-containing additives-electrolytes are also used as accelerators for setting and hardening of cement. Action mechanism of additive accelerators for setting and hardening of cement is rather complicated and can not be considered as well-established. An influence of sulfate-containing additives such as sodium sulfate is reduced to acceleration of cement silicate phase hydration by increasing ionic strength of the solution. In addition to it, exchange reactions of anion additive with portlandite phase (Ca(OH2 and aluminate phases of hardening cement have a significant effect on hardening process that lead to formation of readily soluble hydroxides and hardly soluble calcium salts. The influence of sulfate-containing additives on properties of water cement paste and cement stone is quite diverse and depends on salt concentration and cation type. For example, the action of the aluminum sulphate additive becomes more complicated if the additive is subjected to hydrolysis in water, which is aggravated in an alkaline medium of the water cement paste. Formation of hydrolysis products and their reaction with aluminate phases and cement portlandite lead to a significant acceleration of setting. Thus, despite the similarity of additives ensuring participation of anions in the exchange reactions, the mechanism of their influence on cement setting and hardening varies rather significantly. The present paper considers peculiar features concerning the mechanism of interaction of sodium and aluminum sulfate additives in cement compositions from the viewpoint of thermochemistry. Thermochemical equations for reactions of sulfate-containing additives with phases of hydrated cement clinker have been given in the paper. The paper contains description how to calculate thermal effects of chemical reactions and determine an influence of the formed

  18. A comprehensive iso-octane combustion model with improved thermochemistry and chemical kinetics

    KAUST Repository

    Atef, Nour

    2017-02-05

    Iso-Octane (2,2,4-trimethylpentane) is a primary reference fuel and an important component of gasoline fuels. Moreover, it is a key component used in surrogates to study the ignition and burning characteristics of gasoline fuels. This paper presents an updated chemical kinetic model for iso-octane combustion. Specifically, the thermodynamic data and reaction kinetics of iso-octane have been re-assessed based on new thermodynamic group values and recently evaluated rate coefficients from the literature. The adopted rate coefficients were either experimentally measured or determined by analogy to theoretically calculated values. Furthermore, new alternative isomerization pathways for peroxy-alkyl hydroperoxide (ȮOQOOH) radicals were added to the reaction mechanism. The updated kinetic model was compared against new ignition delay data measured in rapid compression machines (RCM) and a high-pressure shock tube. These experiments were conducted at pressures of 20 and 40 atm, at equivalence ratios of 0.4 and 1.0, and at temperatures in the range of 632–1060 K. The updated model was further compared against shock tube ignition delay times, jet-stirred reactor oxidation speciation data, premixed laminar flame speeds, counterflow diffusion flame ignition, and shock tube pyrolysis speciation data available in the literature. Finally, the updated model was used to investigate the importance of alternative isomerization pathways in the low temperature oxidation of highly branched alkanes. When compared to available models in the literature, the present model represents the current state-of-the-art in fundamental thermochemistry and reaction kinetics of iso-octane; and thus provides the best prediction of wide ranging experimental data and fundamental insights into iso-octane combustion chemistry.

  19. The thermochemistry of london dispersion-driven transition metal reactions: getting the 'right answer for the right reason'.

    Science.gov (United States)

    Hansen, Andreas; Bannwarth, Christoph; Grimme, Stefan; Petrović, Predrag; Werlé, Christophe; Djukic, Jean-Pierre

    2014-10-01

    Reliable thermochemical measurements and theoretical predictions for reactions involving large transition metal complexes in which long-range intramolecular London dispersion interactions contribute significantly to their stabilization are still a challenge, particularly for reactions in solution. As an illustrative and chemically important example, two reactions are investigated where a large dipalladium complex is quenched by bulky phosphane ligands (triphenylphosphane and tricyclohexylphosphane). Reaction enthalpies and Gibbs free energies were measured by isotherm titration calorimetry (ITC) and theoretically 'back-corrected' to yield 0 K gas-phase reaction energies (ΔE). It is shown that the Gibbs free solvation energy calculated with continuum models represents the largest source of error in theoretical thermochemistry protocols. The ('back-corrected') experimental reaction energies were used to benchmark (dispersion-corrected) density functional and wave function theory methods. Particularly, we investigated whether the atom-pairwise D3 dispersion correction is also accurate for transition metal chemistry, and how accurately recently developed local coupled-cluster methods describe the important long-range electron correlation contributions. Both, modern dispersion-corrected density functions (e.g., PW6B95-D3(BJ) or B3LYP-NL), as well as the now possible DLPNO-CCSD(T) calculations, are within the 'experimental' gas phase reference value. The remaining uncertainties of 2-3 kcal mol(-1) can be essentially attributed to the solvation models. Hence, the future for accurate theoretical thermochemistry of large transition metal reactions in solution is very promising.

  20. Electronic structure of the actinide dioxides

    International Nuclear Information System (INIS)

    Kelly, P.J.

    1980-03-01

    The electronic properties of the fluorite structured actinide dioxides have been investigated using the linear muffin tin orbital method in the atomic sphere approximation. CaF 2 with the same structure was also studied because of the relative simplicity of its electronic structure and the greater amount of experimental data available. Band structures were calculated both non self consistently and self consistently. In the non self consistent calculations the effect of changing the approximation to the exchange-correlation potential and the starting atomic configurations was examined. Using the concepts of canonical bands the effects of hybridization were investigated. In particular the 5f electrons included in the band picture were found to mix more strongly into the valence band than indicated by experiment. On this basis the 5f electrons were not included in self consistent calculations which in the density functional formalism are capable of yielding ground state properties. Because of the non participation of the f electrons in the bonding UO 2 only was considered as representative of the actinide dioxides. For comparison CaF 2 was also examined. Using Pettifor's pressure formula to determine the equilibrium condition the lattice constants were calculated to be 0.5% and 5% respectively below the experimental values. (author)

  1. 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.)

  2. 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)

  3. Evaluation of actinide biosorption by microorganisms

    Energy Technology Data Exchange (ETDEWEB)

    Happel, A.M.

    1996-06-01

    Conventional methods for removing metals from aqueous solutions include chemical precipitation, chemical oxidation or reduction, ion exchange, reverse osmosis, electrochemical treatment and evaporation. The removal of radionuclides from aqueous waste streams has largely relied on ion exchange methods which can be prohibitively costly given increasingly stringent regulatory effluent limits. The use of microbial cells as biosorbants for heavy metals offers a potential alternative to existing methods for decontamination or recovery of heavy metals from a variety of industrial waste streams and contaminated ground waters. The toxicity and the extreme and variable conditions present in many radionuclide containing waste streams may preclude the use of living microorganisms and favor the use of non-living biomass for the removal of actinides from these waste streams. In the work presented here, we have examined the biosorption of uranium by non-living, non-metabolizing microbial biomass thus avoiding the problems associated with living systems. We are investigating biosorption with the long term goal of developing microbial technologies for the remediation of actinides.

  4. 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

  5. The study of actinide solubility limiting solid phases

    International Nuclear Information System (INIS)

    Thomason, H.P.

    1988-01-01

    The literature has been surveyed for information on the identification and ageing of actinide solubility limiting solid phases. References include identification and ageing of actinide solids which do not necessarily relate to the control of solubility or the conditions found in the near-field of a repository. Methods which have been used to characterise actinide solids include X-ray diffraction, electron microscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, electrochemistry and chemical analysis. The techniques most widely used are X-ray and electron diffraction. As well as characterisation, diffraction patterns have been used to monitor changes in the crystallinity of a solid with time. The ageing of alpha active actinide solids involves two conflicting processes. An amorphous actinide precipitate will, like most solids, become more crystalline with time. The recoil energy from the alpha decay of actinides will displace some of the atoms from their lattice sites and cause a decrease in crystallinity. The crystallinity of actinide solids affects solubility and is therefore an important parameter to study. Recommendations have been made for further environmental work. (author)

  6. 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)

  7. 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

  8. Crystal growth methods dedicated to low solubility actinide oxalates

    Energy Technology Data Exchange (ETDEWEB)

    Tamain, C., E-mail: christelle.tamain@cea.fr [CEA, Nuclear Energy Division, Marcoule, RadioChemistry & Processes Department, F-30207 Bagnols sur Cèze (France); Arab-Chapelet, B. [CEA, Nuclear Energy Division, Marcoule, RadioChemistry & Processes Department, F-30207 Bagnols sur Cèze (France); Rivenet, M. [University Lille Nord de France, Unité de Catalyse et de Chimie du Solide, UCCS UMR CNRS 8181, ENSCL-USTL, B.P. 90108, F-59652 Villeneuve d’Ascq Cedex (France); Grandjean, S. [CEA, Nuclear Energy Division, Marcoule, RadioChemistry & Processes Department, F-30207 Bagnols sur Cèze (France); Abraham, F. [University Lille Nord de France, Unité de Catalyse et de Chimie du Solide, UCCS UMR CNRS 8181, ENSCL-USTL, B.P. 90108, F-59652 Villeneuve d’Ascq Cedex (France)

    2016-04-15

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

  9. 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

  10. Process to remove actinides from soil using magnetic separation

    Science.gov (United States)

    Avens, Larry R.; Hill, Dallas D.; Prenger, F. Coyne; Stewart, Walter F.; Tolt, Thomas L.; Worl, Laura A.

    1996-01-01

    A process of separating actinide-containing components from an admixture including forming a slurry including actinide-containing components within an admixture, said slurry including a dispersion-promoting surfactant, adjusting the pH of the slurry to within a desired range, and, passing said slurry through a pretreated matrix material, said matrix material adapted to generate high magnetic field gradients upon the application of a strong magnetic field exceeding about 0.1 Tesla whereupon a portion of said actinide-containing components are separated from said slurry and remain adhered upon said matrix material is provided.

  11. An emergency bioassay method for actinides in urine.

    Science.gov (United States)

    Dai, Xiongxin; Kramer-Tremblay, Sheila

    2011-08-01

    A rapid bioassay method has been developed for the sequential measurements of actinides in human urine samples. The method involves actinide separation from a urine matrix by co-precipitation with hydrous titanium oxide (HTiO), followed by anion exchange and extraction chromatography column purification, and final counting by alpha spectrometry after cerium fluoride micro-precipitation. The minimal detectable activities for the method were determined to be 20 mBq L(-1) or less for plutonium, uranium, americium and curium isotopes, with an 8-h sample turn-around time. Spike tests showed that this method would meet the requirements for actinide bioassay following a radiation emergency.

  12. 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.

  13. 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)

  14. 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

  15. 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

  16. 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

  17. 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

  18. 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....

  19. 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

  20. Separations and Actinide Science -- 2005 Roadmap

    Energy Technology Data Exchange (ETDEWEB)

    2005-09-01

    The Separations and Actinide Science Roadmap presents a vision to establish a separations and actinide science research (SASR) base composed of people, facilities, and collaborations and provides new and innovative nuclear fuel cycle solutions to nuclear technology issues that preclude nuclear proliferation. This enabling science base will play a key role in ensuring that Idaho National Laboratory (INL) achieves its long-term vision of revitalizing nuclear energy by providing needed technologies to ensure our nation's energy sustainability and security. To that end, this roadmap suggests a 10-year journey to build a strong SASR technical capability with a clear mission to support nuclear technology development. If nuclear technology is to be used to satisfy the expected growth in U.S. electrical energy demand, the once-through fuel cycle currently in use should be reconsidered. Although the once-through fuel cycle is cost-effective and uranium is inexpensive, a once-through fuel cycle requires long-term disposal to protect the environment and public from long-lived radioactive species. The lack of a current disposal option (i.e., a licensed repository) has resulted in accumulation of more than 50,000 metric tons of spent nuclear fuel. The process required to transition the current once-through fuel cycle to full-recycle will require considerable time and significant technical advancement. INL's extensive expertise in aqueous separations will be used to develop advanced separations processes. Computational chemistry will be expanded to support development of future processing options. In the intermediate stage of this transition, reprocessing options will be deployed, waste forms with higher loading densities and greater stability will be developed, and transmutation of long-lived fission products will be explored. SASR will support these activities using its actinide science and aqueous separations expertise. In the final stage, full recycle will be

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

    Science.gov (United States)

    Permana, Sidik

    2017-07-01

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

  2. Ab initio thermochemistry using optimal-balance models with isodesmic corrections: The ATOMIC protocol

    Science.gov (United States)

    Bakowies, Dirk

    2009-04-01

    A theoretical composite approach, termed ATOMIC for Ab initio Thermochemistry using Optimal-balance Models with Isodesmic Corrections, is introduced for the calculation of molecular atomization energies and enthalpies of formation. Care is taken to achieve optimal balance in accuracy and cost between the various components contributing to high-level estimates of the fully correlated energy at the infinite-basis-set limit. To this end, the energy at the coupled-cluster level of theory including single, double, and quasiperturbational triple excitations is decomposed into Hartree-Fock, low-order correlation (MP2, CCSD), and connected-triples contributions and into valence-shell and core contributions. Statistical analyses for 73 representative neutral closed-shell molecules containing hydrogen and at least three first-row atoms (CNOF) are used to devise basis-set and extrapolation requirements for each of the eight components to maintain a given level of accuracy. Pople's concept of bond-separation reactions is implemented in an ab initio framework, providing for a complete set of high-level precomputed isodesmic corrections which can be used for any molecule for which a valence structure can be drawn. Use of these corrections is shown to lower basis-set requirements dramatically for each of the eight components of the composite model. A hierarchy of three levels is suggested for isodesmically corrected composite models which reproduce atomization energies at the reference level of theory to within 0.1 kcal/mol (A), 0.3 kcal/mol (B), and 1 kcal/mol (C). Large-scale statistical analysis shows that corrections beyond the CCSD(T) reference level of theory, including coupled-cluster theory with fully relaxed connected triple and quadruple excitations, first-order relativistic and diagonal Born-Oppenheimer corrections can normally be dealt with using a greatly simplified model that assumes thermoneutral bond-separation reactions and that reduces the estimate of these

  3. 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

  4. 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.)

  5. 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

  6. 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

  7. 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.

  8. 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.

  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. 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.

  11. Actinide cross section program at ORELA

    International Nuclear Information System (INIS)

    Dabbs, J.W.T.

    1980-01-01

    The actinide cross section program at ORELA, the Oak Ridge Electron Linear Accelerator, is aimed at obtaining accurate neutron cross sections (primarily fission, capture, and total) for actinide nuclides which occur in fission reactors. Such cross sections, measured as a function of neutron energy over as wide a range of energies as feasible, comprise a data base that permits calculated predictions of the formation and removal of these nuclides in reactors. The present program is funded by the Division of Basic Energy Sciences of DOE, and has components in several divisions at ORNL. For intensively α-active nuclides, many of the existing fission cross section data have been provided by underground explosions. New measurement techniques, developed at ORELA, now permit linac measurements on fissionable nuclides with alpha half-lives as short as 28 years. Capture and capture-plus-fission measurements utilize scintillation detectors (of capture γ rays and fission neutrons) in which pulse shape discrimination plays an important role. Total cross sections can be measured at ORELA on samples of only a few milligrams. A simultaneous program of chemical and isotopic analyses of samples irradiated in EBR-II is in progress to provide benchmarks for the existing differential measurements. These analyses are being studied with updated versions of ORIGEN and with sensitivity determinations. Calculations of the sensitivity to cross section changes of various aspects of the nuclear fuel cycle are also being made. Even in this relatively mature field, many cross sections still require improvements to provide an adequate data base. Examples of recent techniques and measurements are presented. 12 figures, 3 tables

  12. 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

  13. 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

  14. 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.

  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. 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.

  17. 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

  18. 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

  19. 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)

  20. 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

  1. Rapid fusion method for determination of actinides in fecal samples

    International Nuclear Information System (INIS)

    Maxwell, S.L.; Culligan, B.K.; Hutchison, J.B.; Spencer, R.B.

    2013-01-01

    A new rapid fusion method for the determination of actinides in fecal samples has been developed at the Savannah River National Laboratory that can be used for emergency response or routine bioassay analyses. If a radiological dispersive device, improvised nuclear device or nuclear accident occur, there will be an urgent need for rapid analyses of environmental, food and bioassay matrices. If an inhalation event occurs and there is confirmed radionuclide activity present via urine analyses of individuals, fecal analyses will typically be required to determine the soluble/insoluble fraction of actinides present as a result of the event to allow a more reliable estimate of radiological dose. The new method for actinides in fecal samples uses accelerated furnace heating, a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a column separation process with stacked TEVA, TRU and DGA resin cartridges. The rapid fusion method provides rugged digestion of any refractory particles present, essential for reliable analysis of actinides in fecal samples. Alpha spectrometry was used to determine the actinide isotopes, but this method can be adapted for assay by inductively-coupled plasma mass spectrometry for actinide isotopes with longer half-lives that have sufficient mass to allow measurement. The method showed high chemical recoveries and effective removal of interferences. The determination of actinides in fecal samples can be performed in less than 12 h in an emergency with excellent quality for emergency samples. The new method, which is much less tedious and time-consuming than other reported methods, can be used for emergency or routine fecal sample analyses. This enables more timely estimates of radiological dose to be performed that utilize soluble/insoluble actinide ratios. (author)

  2. 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.)

  3. 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)

  4. 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.

  5. Threshold Photoelectron Photoion Coincidence (TPEPICO) Studies. The Road to ± 0.1 kJ/mol Thermochemistry

    Energy Technology Data Exchange (ETDEWEB)

    Baer, Tomas [Univ. of North Carolina, Chapel Hill, NC (United States)

    2013-10-14

    The threshold photoelectron photoion coincidence (TPEPICO) technique is utilized to investigate the dissociation dynamics and thermochemistry of energy selected medium to large organic molecular ions. The reactions include parallel and consecutive steps that are modeled with the statistical theory in order to extract dissociation onsets for multiple dissociation paths. These studies are carried out with the aid of molecular orbital calculations of both ions and the transition states connecting the ion structure to their products. The results of these investigations yield accurate heats of formation of ions, free radicals, and stable molecules. In addition, they provide information about the potential energy surface that governs the dissociation process. Isomerization reactions prior to dissociation are readily inferred from the TPEPICO data.

  6. 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

  7. 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

  8. Structural and electronic relationships between the lanthanide and actinide elements

    International Nuclear Information System (INIS)

    Johansson, Boerje

    2000-01-01

    The similarity and difference between the solid state properties of the 4f and 5f transition metals are pointed out. The heavier 5f elements show properties which have direct correspondence to the early 4f transition metals, suggesting a localized behaviour of the 5f electrons for those metals. On the other hand, the fact that Pu metal has a 30% lower volume than its neighbour heavier element, Am, suggests a tremendous difference in the properties of the 5f electrons for this element relative to the heavier actinides. This change in behaviour between Pu and Am can be viewed as a Mott transition within the 5f shell as a function of the atomic number Z. On the metallic 5f side of the Mott transition (i.e., early actinides), the elements show most unusual crystal structures, the common feature being their low symmetry. An analogous behaviour for the lanthanides is found in cerium metal under compression, where structures typical for the light actinides have been observed experimentally. A generalized phase diagram for the actinides is shown to contain features comparable to the individual phase diagram of Ce metal. The crystal structure behaviour of the lanthanides and heavier actinides is determined by the number of 5d (or 6d) electrons in the metallic state, since for these elements the f electrons are localized and nonbonding. For the earlier actinide metals electronic structure calculations - where the 5f orbitals are treated as part of the valence bands - account very well for the observed ground state crystal structures. The distorted structures can be understood as Peierls distortions away from the symmetric bcc structure and originate from strongly bonding 5f electrons occupying relatively narrow 5f states. High pressure is an extremely useful experimental tool to demonstrate the interrelationship between the lanthanides and the actinides

  9. Thin extractive membrane for monitoring actinides in aqueous streams.

    Science.gov (United States)

    Chavan, Vivek; Paul, Sumana; Pandey, Ashok K; Kalsi, P C; Goswami, A

    2013-09-15

    Alpha spectrometry and solid state nuclear track detectors (SSNTDs) are used for monitoring ultra-trace amount of alpha emitting actinides in different aqueous streams. However, these techniques have limitations i.e. alpha spectrometry requires a preconcentration step and SSNTDs are not chemically selective. Therefore, a thin polymer inclusion membrane (PIM) supported on silanized glass was developed for preconcentraion and determination of ultra-trace concentration of actinides by α-spectrometry and SSNTDs. PIMs were formed by spin coating on hydrophobic glass slide or solvent casting to form thin and self-supported membranes, respectively. Sorption experiments indicated that uptakes of actinides in the PIM were highly dependent on acidity of solution i.e. Am(III) sorbed up to 0.1 molL(-1) HNO₃, U(VI) up to 0.5 molL(-1) HNO₃ and Pu(IV) from HNO₃ concentration as high as 4 molL(-1). A scheme was developed for selective sorption of target actinide in the PIM by adjusting acidity and oxidation state of actinide. The actinides sorbed in PIMs were quantified by alpha spectrometry and SSNTDs. For SSNTDs, neutron induced fission-fragment tracks and α-particle tracks were registered in Garware polyester and CR-39 for quantifications of natural uranium and α-emitting actinides ((241)Am/(239)Pu/(233)U), respectively. Finally, the membranes were tested to quantify Pu in 4 molL(-1) HNO3 solutions and synthetic urine samples. Copyright © 2013 Elsevier B.V. All rights reserved.

  10. Interaction of actinides with amino acids: from peptides to proteins

    International Nuclear Information System (INIS)

    Jeanson, A.

    2008-09-01

    Structural information on complexes of actinides with molecules of biological interest is required to better understand the mechanisms of actinides transport in living organisms, and can contribute to develop new decorporation treatments. Our study is about Th(IV), Np(IV), Pu(IV) and uranyl(VI) cations, which have a high affinity for some protein domains, and Fe(III), which is the natural cation of these biological systems. In this work, chelation of actinides has been brought to light with UV-visible-Near Infra Red spectroscopy, NMR, EPR, and ultrafiltration. Determination of the structure of the complexation site has been undertaken with Exafs measurements, and of the tertiary structure of the protein with SANS measurements. The first approach was to describe the interaction modes between actinides and essential chemical functions of proteins. Thus, the Ac-AspAspProAspAsp-NH 2 peptide was studied as a possible chelate of actinides. Polynuclear species with μ-oxo or μ-hydroxo bridges were identified. The iron complex is binuclear, and the actinide ones have a higher nuclearity. The second approach was to study a real case of complexation of actinide with a protein: transferrin. Results show that around physiological ph a mononuclear complex is formed with Np(IV) and Pu(IV), while transferrin does not complex Th(IV) in the same conditions. Characteristic distances of M-transferrin complexes (M = Fe, Np, Pu) were determined. Moreover, the protein seems to be in its close conformation with Pu(IV), and in its open form with Np(IV) and UO 2 2+ . (author)

  11. 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

  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. 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

  14. Evaluation of the borosilicate glass matrix for the immobilization of actinide waste concentrates

    International Nuclear Information System (INIS)

    Scheffler, K.; Krause, H.

    1978-01-01

    During liquid storage of HLLW the formation of actinide enriched sludges is being expected due to the hydrolysis esp. of plutonium and other mechanisms. Also during melting of HLW glasses an increase of top-to-bottom actinide concentration can take place. Both effects will account for increased actinide concentrations in the glasses. The phenomena of these actinide enrichment processes are studied. Following the investigations on actinide compatibility with HLW glass a research program has been started aiming at the vitrification of special actinide waste concentrates. A hazards evaluation is established on the basis of experimental results for simulated disposal periods of millenia with respect to leaching of actinides and alpha irradiation damage. The chemical compatibility of borosilicate glass with actinides has been determined and basic considerations are drawn for the solidification of different types of alpha-bearing wastes in borosilicate glasses

  15. Ab initio LSDA and LSDA+U study of pure and Cd-doped cubic lanthanide sesquioxides

    DEFF Research Database (Denmark)

    Richard, D.; Muñoz, E.L.; Rentería, M.

    2013-01-01

    The electronic, structural, and hyperfine properties of pure and Cd-doped lanthanide (Ln) sesquioxides with the cubic bixbyite structure (Ln2O3, Ln ranging from La to Lu) have been studied using the full-potential augmented plane wave plus local orbital (APW+lo) method within the local spin density...... approximation (LSDA) and the Coulomb-corrected LSDA+U. In the case of the pure systems, our calculations show that LSDA+U gives a better representation of the band structure compared to LSDA. The predicted equilibrium structures and the electric field gradient (EFG) tensor at Ln sites were calculated...... and compared with those obtained by means of hyperfine techniques and with theoretical results obtained in In2O3, Sc2O3, and Lu2O3 reported in the literature. The origin of the EFG at Ln sites and the role played by the 4f electrons on this quantity are discussed. In the case of the Cd-doped systems, the APW...

  16. Vanadium Dioxide and Vanadium Sesquioxide Thin Films Fabricated on (0001) or (1010)Al2O3 by Reactive RF-Magnetron Sputter Deposition and Subsequent Annealing Processes

    Science.gov (United States)

    Yun, Sun Jin; Lim, Jung Wook; Noh, Jong-Su; Kim, Bong-Jun; Kim, Hyun-Tak

    2009-04-01

    Vanadium dioxide (VO2) and vanadium sesquioxide (V2O3) thin films showing an abrupt metal-insulator transition near their typical critical temperature (TC) were successfully fabricated by reactive RF magnetron sputter deposition and subsequent annealing processes. The annealing processes for preparing VO2 and V2O3 films were carried out in 30 mTorr O2 ambient and at a very low pressure (2 ×10-6 Torr), respectively. V2O3 films could be fabricated by the one-step annealing of as-deposited VOx films in contrast to the V2O3 fabrication by the two-step annealing of sol-gel V2O5 films. The annealing temperature for preparing V2O3 films (≥550 °C) was much lower than those reported in earlier works. The dependence of TC on the surface orientation of a single crystalline Al2O3 substrate was also shown for VO2 and V2O3 films. The films fabricated on (1010)-plane Al2O3 substrate showed superior characteristics to those on (0001)-Al2O3.

  17. Domains and interfaces produced by a cooperative crystal-phase transformation. Application to the hexagonal to monoclinic phase transformation of rare earth sesquioxides. 2

    International Nuclear Information System (INIS)

    Yangui, B.

    1982-01-01

    A general study of domains by crystallographic phase transformation is done in the first part of this study, taking into account the epitaxy between the two structures. Rotation domains are said to be equivalent when they correspond to the same kind of epitaxy; if not they are not equivalent domains. The A (hexagonal) to B (monoclinic) phase transformation of the rare earth sesquioxides is a cooperative one where the c-axis of A becomes the [101-bar] axis of B and the (00.1) plane of A becomes the (201-bar) plane of B. Each crystal seed of the B structure appears by epitaxial growth on the A structure; it is made of two different rotation domains which are not equivalent. Each of them has six equivalent rotation domains so that twelve rotation variants can occur in this phase transformation. All these domains can be related by a rotation about the [101-bar] axis of the B structure. They can sometimes be related by twinning or by a double twinning. In this last case a new rotation domain occurs; this phenomenon is at the origin of the formation of multistar domains which are observed in the same kind of crystallographic phase transformations. (author)

  18. A theoretical study of pressure-induced phase transitions and electronic band structure of anti-A-sesquioxide type {gamma}-Be{sub 3}N{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Paliwal, Uttam; Joshi, Kunj Bihari, E-mail: k_joshi@yahoo.com [Department of Physics, University College of Science, M.L. Sukhadia University, Udaipur-313001 (India)

    2011-06-29

    Structural parameters and electronic band structure of anti-A-sesquioxide (aAs) type {gamma}-Be{sub 3}N{sub 2} are presented following the first-principles linear combination of atomic orbitals method within the framework of a posteriori density-functional theory implemented in the CRYSTAL code. Pressure-induced phase transitions among the four polymorphs {alpha}, {beta}, cubic-{gamma} and aAs-{gamma} of Be{sub 3}N{sub 2} are examined. Enthalpy-pressure curves do not show the possibility of pressure-induced structural phase transition to the cubic-{gamma} phase. However, {alpha} {yields} aAs-{gamma} and {beta} {yields} aAs-{gamma} structural phase transitions are observed at 139 GPa and 93 GPa, respectively. Band structure calculations predict that aAs-{gamma} Be{sub 3}N{sub 2} is an indirect semiconductor with 4.73 eV bandgap at L point. Variation of bandgap with pressure and deformation potentials are studied for the {alpha}, {beta} and aAs-{gamma} polymorphs. Pressure-dependent band structure calculations reveal that, within the low-pressure limit, bandgaps of {beta} and aAs-{gamma} increase with pressure unlike {alpha}-Be{sub 3}N{sub 2}.

  19. 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.

  20. Inert matrix advantages in the transmutation balance of minor actinides

    Energy Technology Data Exchange (ETDEWEB)

    Prunier, C.; Guerin, Y. [CEA Centre d`Etudes de Cadarache, 13 - Saint-Paul-lez-Durance (France). Dept. d`Etudes des Combustibles; Zaetta, A.; Tommasi, J. [CEA Centre d`Etudes de Cadarache, 13 - Saint-Paul-lez-Durance (France). Dept. d`Etudes des Reacteurs

    1995-12-31

    The results of experimental irradiation in relation to the homogeneous concept (UO{sub 2} fuel) with a limited burn-up of 4.5 atom. % have shown that the percentage of the minor actinides Am and Np incinerated reached values of around 25% to 30% - values confirmed by calculations - for irradiation in the Phenix reactor (FR). The calculation and analysis of the quantity of nuclides formed by transmutation, especially plutonium isotopes, are also in close agreement. Using these experimental results, which are supported by the calculations, research on the incineration of minor actinides has been extended to compare the production of plutonium isotopes. Two minor actinide supports are used for this comparison: - a fuel (UO{sub 2} oxide), - an inert matrix (magnesia MgO). In both cases, a content of 45% of minor actinides (Np or Am) by weight is used to represent the heterogeneous recycling mode. Comparison shows the advantage of inert matrices relative to UO{sub 2} fuel to greatly reduce the production of plutonium for the same consumption of minor actinides. A particularly interesting case is that of heterogeneous recycling, which implements americium-based targets (magnesia with 45% americium in the form of AmO{sub 2}), placed on the periphery of the FR core (first row of blankets). (authors). 9 refs., 2 figs., 11 tabs.

  1. Gas core reactors for actinide transmutation and breeder applications

    Science.gov (United States)

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

    1978-01-01

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

  2. Solid phase extraction of actinides using graphene oxide beads

    International Nuclear Information System (INIS)

    Gujar, R.B.; Mohapatra, P.K.

    2014-01-01

    Separation of actinide ions from dilute nitric acid feed solutions is important from radioactive waste remediation point of view. A large number of separation methods are available in the literature using methods such as precipitation, ion-exchange, solvent extraction, etc. Graphene oxide (GO) are reported to be a very good sorbent for actinide ions from weakly acidic feed solutions. However, it is difficult to handle GO fine particles and any chromatographic separation is bound to be difficult as the sorbent material may be finely dispersed in the aqueous phase. It was thus thought of interest to prepare GO-based resin materials in polyether sulphone (PES) by phase inversion technique. Preparation of resins by phase inversion technique has been found to be quite efficient for metal ion separation including actinide ions. In the present work, GO based PES resin beads were prepared by phase inversion technique and the uptake of actinide and lanthanide ions. In the present work, GO based beads were prepared by phase inversion technique and the uptake of actinide and lanthanide ions (such as Am(III), Eu(III), Th(IV), Pu(IV) and U(VI)) has been studied using radiotracers

  3. 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

  4. Development of the Chalmers Grouped Actinide Extraction Process

    Directory of Open Access Journals (Sweden)

    Halleröd Jenny

    2015-12-01

    Full Text Available Several solvents for Grouped ActiNide EXtraction (GANEX processes have been investigated at Chalmers University of Technology in recent years. Four different GANEX solvents; cyclo-GANEX (CyMe4- -BTBP, 30 vol.% tri-butyl phosphate (TBP and cyclohexanone, DEHBA-GANEX (CyMe4-BTBP, 20 vol.% N,N-di-2(ethylhexyl butyramide (DEHBA and cyclohexanone, hexanol-GANEX (CyMe4-BTBP, 30 vol.% TBP and hexanol and FS-13-GANEX (CyMe4-BTBP, 30 vol.% TBP and phenyl trifluoromethyl sulfone (FS-13 have been studied and the results are discussed and compared in this work. The cyclohexanone based solvents show fast and high extraction of the actinides but a somewhat poor diluent stability in contact with the acidic aqueous phase. FS-13-GANEX display high separation factors between the actinides and lanthanides and a good radiolytic and hydrolytic stability. However, the distribution ratios of the actinides are lower, compared to the cyclohexanone based solvents. The hexanol-GANEX is a cheap solvent system using a rather stable diluent but the actinide extraction is, however, comparatively low.

  5. 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.

  6. 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

  7. 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

  8. 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.

  9. 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

  10. 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

  11. Advancing the scientific basis of trivalent actinide-lanthanide separations

    Energy Technology Data Exchange (ETDEWEB)

    Nash, K.L. [Washington State University, Department of Chemistry, PO Box 644630, Pullman, WA 99164-4630 (United States)

    2013-07-01

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

  12. Advancing the scientific basis of trivalent actinide-lanthanide separations

    International Nuclear Information System (INIS)

    Nash, K.L.

    2013-01-01

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

  13. Fuel/target concepts for transmutation of actinides

    International Nuclear Information System (INIS)

    Fernandez, A.; Haas, D.; Konings, R.J.M.; Somers, J.

    2001-01-01

    Four different concepts for fuels and targets for transmutation of (minor) actinides are discussed in the present paper. These include thorium-based mixed oxides, inert matrix mixed oxide, and composites based on mixtures oxide powders (CERCER) or mixtures of oxide and metal powders (CERMET). Fabrication methods have been investigated, especially taking account of the specific requirements for handling significant quantities of minor actinides (dust-free processes, remote handling). The processes tested at ITU are based on sol-gel and infiltration (INRAM) techniques or combination thereof. The processes are being validated first using cerium and then plutonium as simulant for the minor actinides, before the actual fabrication of Am- and Cm-containing materials begins in earnest following the completion of the construction of specially designed shielded cells (the MA-lab). (author)

  14. Review of the treatment of actinides-bearing radioactive wastes

    International Nuclear Information System (INIS)

    Krause, H.

    1983-01-01

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

  15. The Lawrence Livermore National Laboratory Intelligent Actinide Analysis System

    International Nuclear Information System (INIS)

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

    1993-01-01

    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 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 as the isotopic analysis code. The design of the IAAS reduces the need for operator intervention, operator training, and operator exposure

  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 2 O) 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. Measurement of Actinides in Molybdenum-99 Solution Analytical Procedure

    Energy Technology Data Exchange (ETDEWEB)

    Soderquist, Chuck Z. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Weaver, Jamie L. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2015-11-01

    This document is a companion report to a previous report, PNNL 24519, Measurement of Actinides in Molybdenum-99 Solution, A Brief Review of the Literature, August 2015. In this companion report, we report a fast, accurate, newly developed analytical method for measurement of trace alpha-emitting actinide elements in commercial high-activity molybdenum-99 solution. Molybdenum-99 is widely used to produce 99mTc for medical imaging. Because it is used as a radiopharmaceutical, its purity must be proven to be extremely high, particularly for the alpha emitting actinides. The sample of 99Mo solution is measured into a vessel (such as a polyethylene centrifuge tube) and acidified with dilute nitric acid. A gadolinium carrier is added (50 µg). Tracers and spikes are added as necessary. Then the solution is made strongly basic with ammonium hydroxide, which causes the gadolinium carrier to precipitate as hydrous Gd(OH)3. The precipitate of Gd(OH)3 carries all of the actinide elements. The suspension of gadolinium hydroxide is then passed through a membrane filter to make a counting mount suitable for direct alpha spectrometry. The high-activity 99Mo and 99mTc pass through the membrane filter and are separated from the alpha emitters. The gadolinium hydroxide, carrying any trace actinide elements that might be present in the sample, forms a thin, uniform cake on the surface of the membrane filter. The filter cake is first washed with dilute ammonium hydroxide to push the last traces of molybdate through, then with water. The filter is then mounted on a stainless steel counting disk. Finally, the alpha emitting actinide elements are measured by alpha spectrometry.

  19. Grouped actinide separation in advanced nuclear fuel cycles

    International Nuclear Information System (INIS)

    Glatz, J.P.; Malmbeck, R.; Ougier, M.; Soucek, P.; Murakamin, T.; Tsukada, T.; Koyama, T.

    2013-01-01

    Aiming at cleaner waste streams (containing only the short-lived fission products) a partitioning and transmutation (P-T) scheme can significantly reduce the quantities of long-lived radionuclides consigned to waste. Many issues and options are being discussed and studied at present in view of selecting the optimal route. The choice is between individual treatment of the relevant elements and a grouped treatment of all actinides together. In the European Collaborative Project ACSEPT (Actinide recycling by Separation and Transmutation), grouped separation options derived from an aqueous extraction or from a dry pyroprocessing route were extensively investigated. Successful demonstration tests for both systems have been carried out in the frame of this project. The aqueous process called GANEX (Grouped Actinide Extraction) is composed of 2 cycles, a first one to recover the major part of U followed by a co-extraction of Np, Pu, Am, and Cm altogether. The pyro-reprocessing primarily applicable to metallic fuels such as the U-Pu-Zr alloy originally developed by the Argonne National Laboratory (US) in the mid 1980s, has also been applied to the METAPHIX fuels containing up to 5% of minor actinides and 5% of lanthanides (e.g. U 60 Pu 20 -Zr 10 Am 2 Nd 3.5 Y 0.5 Ce 0.5 Gd 0.5 ). A grouped actinide separation has been successfully carried out by electrorefining on solid Al cathodes. At present the recovery of the actinides from the alloy formed with Al upon electrodeposition is under investigation, because an efficient P-T cycle requires multiple re-fabrication and re-irradiation. (authors)

  20. New cubic structure compounds as actinide host phases

    Science.gov (United States)

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

    2010-03-01

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

  1. Electron-phonon coupling of the actinide metals

    DEFF Research Database (Denmark)

    Skriver, H. L.; Mertig, I.

    1985-01-01

    The authors have estimated the strength of the electron-phonon coupling in Fr and Ra plus the light actinides Ac through Pu. The underlying self-consistent band-structure calculations were performed by the scalar relativistic linear-muffin-tin-orbital method including l quantum numbers s through g......-phonon parameter λ is found to attain its maximum value in Ac, and they predict a transition temperature of 9K for this metal. In the light actinides Th through Pu, λ is found to be of order 0.4 and within a factor of 2 of experiments which is also the accuracy found in studies of the transition metals...

  2. Method for extracting lanthanides and actinides from acid solutions

    Science.gov (United States)

    Horwitz, E. Philip; Kalina, Dale G.; Kaplan, Louis; Mason, George W.

    1985-01-01

    A process for the recovery of actinide and lanthanide values from aqueous acidic solutions with an organic extractant having the formula: ##STR1## where .phi. is phenyl, R.sup.1 is a straight or branched alkyl or alkoxyalkyl containing from 6 to 12 carbon atoms and R.sup.2 is an alkyl containing from 3 to 6 carbon atoms. The process is suitable for the separation of actinide and lanthanide values from fission product values found together in high level nuclear reprocessing waste solutions.

  3. Physics studies of higher actinide consumption in an LMR

    International Nuclear Information System (INIS)

    Hill, R.N.; Wade, D.C.; Fujita, E.K.; Khalil, H.

    1990-01-01

    The core physics aspects of the transuranic burning potential of the integral Fast Reactor (IFR) are assessed. The actinide behavior in fissile self-sufficient IFR closed cycles of 1200 MWt size is characterized, and the transuranic isotopics and risk potential of the working inventory are compared to those from a once-through LWR. The core neutronic performance effects of rare-earth impurities present in the recycled fuel are addressed. Fuel cycle strategies for burning transuranics from an external source are discussed, and specialized actinide burner designs are described

  4. Experimental studies of narrow band effects in the actinides

    Energy Technology Data Exchange (ETDEWEB)

    Brodsky, M.B.

    1976-01-01

    In many actinide metallic systems the f-electrons exhibit band behavior. This is a consequence of direct f-f wave function overlap or hybridization of f-electrons with s-, p-, and d-electrons. The f-bands can be responsible for large electronic densities of states at the Fermi level which may lead to band magnetism of various types. Although the concept of valence instabilities must be approached cautiously especially in the light actinides, it would not be surprising to observe them in the future, especially in Am compounds.

  5. Experimental studies of narrow band effects in the actinides

    International Nuclear Information System (INIS)

    Brodsky, M.B.

    1976-01-01

    In many actinide metallic systems the f-electrons exhibit band behavior. This is a consequence of direct f-f wave function overlap or hybridization of f-electrons with s-, p-, and d-electrons. The f-bands can be responsible for large electronic densities of states at the Fermi level which may lead to band magnetism of various types. Although the concept of valence instabilities must be approached cautiously especially in the light actinides, it would not be surprising to observe them in the future, especially in Am compounds

  6. Complexes of actinides with naturally occuring organic substances - Literature survey

    International Nuclear Information System (INIS)

    Olofsson, U.; Allard, B.

    1983-02-01

    Properties of naturally occurring humic and fulvic acids and their formation of actinide complexes are reviewed. Actinides in all the oxdation states III, IV, V and VI would form complexes with many humic and fulvic acids, comparable in strength to the hydroxide and carbonate complexes. Preliminary experiments have shown, that the presence of predominantly humic acid complexes would significantly reduce the sorption of americium on geologic media. This does not, however, necessarily lead to a potentially enhanced mobility under environmental conditions, since humic and fulvic acids carrying trace metals also would be strongly bound to e.g. clayish material. (author)

  7. Physics studies of higher actinide consumption in an LMR

    International Nuclear Information System (INIS)

    Hill, R.N.; Wade, D.C.; Fujita, E.K.; Khalil, H.S.

    1990-01-01

    The core physics aspects of the transuranic burning potential of the Integral Fast Reactor (IFR) are assessed. The actinide behavior in fissile self-sufficient IFR closed cycles of 1200 MWt size is characterized, and the transuranic isotopics and risk potential of the working inventory are compared to those from a once-through LWR. The core neutronic performance effects of rare-earth impurities present in the recycled fuel are addressed. Fuel cycle strategies for burning transuranics from an external source are discussed, and specialized actinide burner designs are described. 4 refs., 4 figs., 3 tabs

  8. Thermally unstable complexants/phosphate mineralization of actinides

    International Nuclear Information System (INIS)

    Nash, K.

    1996-01-01

    In situ immobilization is an approach to isolation of radionuclides from the hydrosphere that is receiving increasing attention. Rather than removing the actinides from contaminated soils, this approach transforms the actinides into intrinsically insoluble mineral phases resistant to leaching by groundwater. The principal advangates of this concept are the low cost and low risk of operator exposure and/or dispersion of the radionuclides to the wider environment. The challenge of this approach is toe accomplish the immobilization without causing collateral damage to the environment (the cure shouldn't be worse than the disease) and verification of system performance

  9. Thermodynamic properties of actinide aqueous species relevant to geochemical problems

    International Nuclear Information System (INIS)

    Fuger, J.

    1992-01-01

    The status of our knowledge of the basic thermodynamic properties of the aqueous complexes of the actinides in their different valency states with two environmentally important ligands, namely hydroxide and carbonate is overviewed. Even in the case of uranium which has been the most studied, gaps are found among the relative wealth of trustworthy formation constants, especially for the less stable valence states. The need for substantial improvement of our knowledge in the case of the other actinides, especially transuranium elements, is outlined. The relative scarcity of enthalpy of formation data is also stressed. (orig.)

  10. New molecules for the separation of actinides (III): the picolinamides

    International Nuclear Information System (INIS)

    Cordier, P.Y.; Condamines, N.; Berthon, L.; Madic, C.

    1994-01-01

    Minor actinide partitioning from high level liquid wastes produced during the reprocessing of nuclear fuels by the Purex process, requires the design of new extracting molecules. These new extractants must be able to separate, for example, actinides from lanthanides. This separation is very difficult, due to the similar chemical properties of these metallic species, but it can possibly be reached by using extractants with soft donor atoms (N or S). Some new molecules : the picolinamides are investigated in this way. The general chemical formula and the behaviour of these compounds in acidic media are given. (O.L.). 3 refs

  11. New molecules for the separation of actinides (III): the picolinamides

    Energy Technology Data Exchange (ETDEWEB)

    Cordier, P.Y.; Condamines, N.; Berthon, L.; Madic, C.

    1994-12-31

    Minor actinide partitioning from high level liquid wastes produced during the reprocessing of nuclear fuels by the Purex process, requires the design of new extracting molecules. These new extractants must be able to separate, for example, actinides from lanthanides. This separation is very difficult, due to the similar chemical properties of these metallic species, but it can possibly be reached by using extractants with soft donor atoms (N or S). Some new molecules : the picolinamides are investigated in this way. The general chemical formula and the behaviour of these compounds in acidic media are given. (O.L.). 3 refs.

  12. CANDU - a versatile reactor for plutonium disposition or actinide burning

    International Nuclear Information System (INIS)

    Chan, P.S.W.; Gagnon, M.J.N.; Boczar, P.G.; Ellis, R.J.; Verrall, R.A.

    1997-10-01

    High neutron economy, on-line refuelling, and a simple fuel-bundle design result in a high degree of versatility in the use of the CANDU reactor for the disposition of weapons-derived plutonium and for the annihilation of long-lived radioactive actinides, such as plutonium, neptunium, and americium isotopes, created in civilian nuclear power reactors. Inherent safety features are incorporated into the design of the bundles carrying the plutonium and actinide fuels. This approach enables existing CANDU reactors to operate with various plutonium-based fuel cycles without requiring major changes to the current reactor design. (author)

  13. Novel complexing agents for the efficient separation of actinides and remediation of actinide-contaminated sites

    International Nuclear Information System (INIS)

    Baisden, P.; Kadkhodayan, B.

    1996-01-01

    Research into the coordination chemistry of transactinide elements should provide us with new fundamental knowledge about structure, geometry, and stability of these metal complexes. Our approach involves the design, synthesis, and characterization of open-quotes expanded porphyrinclose quotes macrocyclic ligands which coordinate the actinide metal cations with high thermodynamic affinity and kinetic stability. We can use the knowledge from understanding the fundamental coordination chemistry of these elements as a stepping stone to heavy metal detoxification, radioactive waste cleanup, and possibly radioactive isotope separation. The critical components of this research endeavor, along with the viability of metal complex formation, will be correlated to ring size and core geometry of the ligand and, the atomic radius, oxidation state, coordination geometry and coordination number of the transactinium metal ion. These chelating agents may have certain applications to the solution of some radioactive waste problems if they can be attached to polymer supports and used to chemically separate the radioactive components in waste

  14. Chemistry of tetravalent actinides phosphates. The thorium phosphate-diphosphate as immobilisation matrix of actinides

    International Nuclear Information System (INIS)

    Dacheux, N.

    2002-01-01

    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.)

  15. 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

  16. Actinide removal from molten salts by chemical oxidation and salt distillation

    Energy Technology Data Exchange (ETDEWEB)

    McNeese, J.A.; Garcia, E.; Dole, V.R. [Los Alamos National Laboratory, NM (United States)] [and others

    1995-10-01

    Actinide removal from molten salts can be accomplished by a two step process where the actinide is first oxidized to the oxide using a chemical oxidant such as calcium carbonate or sodium carbonate. After the actinide is precipitated as an oxide the molten salt is distilled away from the actinide oxides leaving a oxide powder heel and an actinide free distilled salt that can be recycled back into the processing stream. This paper discusses the chemistry of the oxidation process and the physical conditions required to accomplish a salt distillation. Possible application of an analogous process sequence for a proposed accelerator driven transmutation molten salt process is also discussed.

  17. 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)

  18. Actinide and Fission Product Partitioning and Transmutation

    International Nuclear Information System (INIS)

    2015-06-01

    The benefits of partitioning and transmutation (P and T) have now been established worldwide and, as a result, many countries are pursuing R and D programmes to advance the technologies associated with P and T. In this context, the OECD Nuclear Energy Agency (NEA) has organised a series of biennial information exchange meetings to provide experts with a forum to present and discuss state-of-the-art developments in the field of partitioning and transmutation since 1990. The OECD Nuclear Energy Agency Information Exchange Meeting on Actinides and Fission Products Partitioning and Transmutation is a forum for experts to present and discuss the state-of-the-art development in the field of P and T. Thirteen meetings have been organised so far and held in Japan, the United States, France, Belgium, Spain, the Republic of Korea and the Czech Republic. This 13. meeting was hosted by Seoul National University (Seoul, Republic of Korea) and was organised in co-operation with the International Atomic Energy Agency (IAEA) and the European Community (EC). The meeting covered strategic and scientific developments in the field of P and T such as: fuel cycle strategies and transition scenarios, the role of P and T in the potential evolution of nuclear energy as part of the future energy mix; radioactive waste management strategies; transmutation fuels and targets; advances in pyro and aqueous separation processes; P and T specific technology requirements (materials, spallation targets, coolants, etc.); transmutation systems: design, performance and safety; impact of P and T on the fuel cycle; fabrication, handling and transportation of transmutation fuels. A total of 103 presentations (39 oral and 64 posters) were discussed among the 110 participants from 19 countries and 2 international organisations. The meeting consisted of one plenary session where national and international programmes were presented followed by 5 technical sessions: - Fuel Cycle Strategies and Transition

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

    International Nuclear Information System (INIS)

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

    1979-01-01

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

  20. Method for recovery of actinides from actinide-bearing scrap and waste nuclear material using O/sub 2/F/sub 2/

    Science.gov (United States)

    Asprey, L.B.; Eller, P.G.

    1984-09-12

    Method for recovery of actinides from nuclear waste material containing sintered and other oxides thereof and from scrap materials containing the metal actinides using O/sub 2/F/sub 2/ to generate the hexafluorides of the actinides present therein. The fluorinating agent, O/sub 2/F/sub 2/, has been observed to perform the above-described tasks at sufficiently low temperatures that there is virtually no damage to the containment vessels. Moreover, the resulting actinide hexafluorides are not detroyed by high temperature reactions with the walls of the reaction vessel. Dioxygen difluoride is readily prepared, stored and transferred to the place of reaction.

  1. High temperature electrical conductivity of yttrium sesquioxide under entremely low oxygen pressure; Gokuteion sansoatsuka ni okeru ittoria no koon denki dendosei

    Energy Technology Data Exchange (ETDEWEB)

    Yoneoka, T.; Terai, T. [The University of Tokyo, Tokyo (Japan). Faculty of Engineering; Takahashi, Y. [Chuo University, Tokyo (Japan)

    1996-01-20

    Yttrium sesquioxide (yttria) is considered to be one of the most hopeful candidate materials for a collector electrode of the separated uranium atom in a laser uranium enrichment system. In order to confirm a required property for the electrode, the conductivity measurement of yttria was performed under a simulated condition in the presence of molten uranium. Because of the extremely low oxygen pressure in the U-UO2 system such a condition was locally realized by placing yttria specimens between plates of titanium or vanadium at high temperature. The specimens were reduced in advance to hypostoichiometry with titanium or vanadium plates under the condition of 1600 K and 2.5 Ms in vacuo. The electrical conductivity measurement was performed by the AC four-probe method in the temperature range of about 900-1600 K and the frequency range of 60 Hz-30 kHz. The electrical conductivity of hypostoichiometric yttria reduced by titanium was higher than that of intrinsic germanium at room temperature (2.1 S/m). This specimen showed the characteristic behavior in the temperature dependence of conductivity; the conductivity showed semiconductor-like behavior in the range of 1400-1600 K, while it had a minimum at about 1250 K and again increased below this temperature. That of hypostoichiometric yttria reduced by vanadium was much lower than that of the specimen, educed with titanium and followed a straight line in the Arrhenius plot above 1000 K. The conductivities of both hypostoichiometric specimens were independent of frequency, which means the conduction carrier was the electron or electron hole. From the oxygen concentration of the metals which were used for the reduction, the oxygen pressures equilibrated with the yttria specimens here estimated to discuss the relation to the measured conductivities. 19 refs., 8 figs., 1 tab.

  2. Physical and chemical characterization of actinides in soil from Johnston Atoll

    International Nuclear Information System (INIS)

    Wolf, S.F.; Bates, J.K.; Buck, E.C.; Dietz, N.L.; Fortner, J.A.; Brown, N.R.

    1997-01-01

    Characterization of the actinide content of a sample of contaminated coral soil from Johnston Atoll, the site of three non-nuclear destructs of nuclear warhead-carrying THOR missiles in 1962, revealed that >99% of the total actinide content is associated with discrete bomb fragments. After removal of these fragments, there was an inverse correlation between actinide content and soil particle size in particles from 43 to 0.4 μm diameter. Detailed analyses of this remaining soil revealed no discrete actinide phase in these soil particles, despite measurable actinide content. Observations indicate that exposure to the environment has caused the conversion of relatively insoluble actinide oxides to the more soluble actinyl oxides and actinyl carbonate coordinated complexes. This process has led to dissolution of actinides from discrete particles and migration to the surrounding soil surfaces, resulting in a dispersion greater than would be expected by physical transport of discrete particles alone. 26 refs., 4 figs., 1 tab

  3. Chemical and physical data for the actinide elements and their compounds

    International Nuclear Information System (INIS)

    Perry, D.L.

    1994-01-01

    The chemistry of the actinide elements, elements comprising the 5f block of elements in the Periodic Table, has become increasingly more important with respect to the environment. This is especially true regarding the need for an understanding of these elements and their reactions in the remediation of sites that have been previously used for nuclear materials production, processing, and fabrication. A detailed knowledge of the chemical and physical properties of these elements is also necessary for deriving rigorous codes and models for the chemical transport of the actinides in soils and groundwaters. This paper is centered around a discussion of the various data resources for the chemical and physical properties of actinides and actinide-based materials. The classes of actinides covered include oxides, sulfides, hydroxides, carbonates, salts, and the heavier chalcogenides. Additionally, data sources for actinide materials used in the nuclear (and other) industry are discussed, as are compounds of actinide elements

  4. Theoretical investigations of the thermochemistry, structures, and internal rotation of conjugated polyynes

    Science.gov (United States)

    Jarowski, Peter D.

    Chapter 1 discusses the thermochemistry of conjugated double and triple bonds. The conjugation stabilization energies of dienes and diynes are considerably larger than estimates based on heat of hydrogenation differences between 1,3-butadiyne and 1-butyne as well as between 1,3-butadiene and 1-butene. Such comparisons do not take into account the counterbalancing hyperconjugative stabilization of the partially hydrogenated products by their ethyl groups. When alkyl hyperconjugation is considered, the conjugation stabilization of diynes (≈ 9.3 kcal/mol) is found by two methods (involving isomerization of non-conjugated into conjugated isomers and heats of hydrogenation) to be larger than that of dienes (≈ 8.2 kcal/mol). In Chapter 2 the stabilization of substituted organic radicals, relative to methyl, are computed using bond separation energies and the block localized wavefunction method. These energies are typically evaluated from C-H bond dissociation energies (computed here by the CBS-RAD method). However, this method gives stabilization energies of an increasing number of mono-, di-, and tri-substituted vinyl and ethynyl substituents, which differ from the predictions of Perturbation Molecular Orbital (PMO) and Huckel Molecular Orbital (HMO) theory. The saturation (attenuation) effect for both series should be monotonic and small. Instead, the attenuation computed by the allylic series is larger than that predicted by HMO theory and the behavior of the propargylic series is erratic. These discrepancies arise from the use of bond dissociation energy data in the evaluations, which depend not only on the stabilization of the radicals, but also on the substantial substituent effects (e.g., hyperconjugation) on the energies of the reference hydrocarbons. New evaluation schemes are proposed that avoid such complications and thus estimate radical stabilization effects directly; the results agree with PMO and HMO theories. Substitution effects are analyzed using

  5. Economic analysis of the hydrogen production by means of the thermo-chemistry process iodine-sulfur with nuclear energy

    International Nuclear Information System (INIS)

    Solorzano S, C.; Francois L, J. L.

    2011-11-01

    In this work an economic study was realized about a centralized plant of hydrogen production that works by means of a thermo-chemistry cycle of sulfur-iodine and uses heat coming from a nuclear power plant of IV generation, with base in the software -Hydrogen Economic Evaluation Programme- obtained through the IAEA. The sustainable technology that is glimpsed next for the generation of hydrogen is to great scale and based on processes of high temperature coupled to nuclear power plants, being the most important the cycle S-I and the electrolysis to high temperature, for what objective references are presented that can serve as base for the taking of decisions for its introduction in Mexico. After detailing the economic models that uses the software for the calculation of the even cost of hydrogen production and the characteristics, so much of the nuclear plant constituted by fourth generation reactors, as of the plant of hydrogen production, is proposed a -base- case, obtaining a preliminary even cost of hydrogen production with this process; subsequently different cases are studied starting from which are carried out sensibility analysis in several parameters that could rebound in this cost, taking into account that these reactors are still in design and planning stages. (Author)

  6. 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.

  7. Actinide recycling for reactor waste mass and radiotoxicity reduction

    International Nuclear Information System (INIS)

    Renard, A.; Maldague, T.; Pilate, S.; Journet, J.; Rome, M.; Harislur, A.; Vergnes, J.

    1994-01-01

    The long-term radiotoxicity of nuclear waste from a Light Water Reactor fuel is analyzed; it can be reduced by multiple recycling of actinides in fast reactors. The capabilities of a first recycling in the light water reactor itself are evaluated with regard to implications on reactor physics and core management. Two main options are compared with their penalties and efficiency

  8. Experimental Evaluation of Actinide Transport in a Fractured Granodiorite

    Energy Technology Data Exchange (ETDEWEB)

    Dittrich, Timothy M. [Los Alamos National Laboratory; Reimus, Paul W. [Los Alamos National Laboratory

    2015-03-16

    The objective of this study was to demonstrate and evaluate new experimental methods for quantifying the potential for actinide transport in deep fractured crystalline rock formations. We selected a fractured granodiorite at the Grimsel Test Site (GTS) in Switzerland as a model system because field experiments have already been conducted with uranium and additional field experiments using other actinides are planned at the site. Thus, working on this system provides a unique opportunity to compare lab experiment results with fieldscale observations. Rock cores drilled from the GTS were shipped to Los Alamos National Laboratory, characterized by x-ray diffraction and microscopy, and used in batch sorption and column breakthrough experiments. Solutions with pH 6.8 and 8.8 were tested. Solutions were switched to radionuclide-free synthetic Grimsel groundwater after near-steady actinide/colloid breakthrough occurred in column experiments. We are currently evaluating actinide adsorption/desorption rates as a function of water chemistry (initial focus on pH), with future testing planned to evaluate the influence of carbonate concentrations, flow rates, and mineralogy in solutions and suspensions with bentonite colloids. (auth)

  9. Calculation of enthalpies of formation of actinide nitrides

    Czech Academy of Sciences Publication Activity Database

    Sedmidubský, D.; Konings, R.J.M.; Novák, Pavel

    2005-01-01

    Roč. 344, - (2005), s. 40-44 ISSN 0022-3115 Institutional research plan: CEZ:AV0Z1010914 Keywords : enthalpy * actinide nitrides * ab-initio theory Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 1.414, year: 2005

  10. Surface energy and work function of the light actinides

    DEFF Research Database (Denmark)

    Kollár, J.; Vitos, Levente; Skriver, Hans Lomholt

    1994-01-01

    We have calculated the surface energy and work function of the light actinides Fr, Ra, Ac, Th, Pa, U, Np, and Pu by means of a Green's-function technique based on the linear-muffin-tin-orbitals method within the tight-binding representation. In these calculations we apply an energy functional which...

  11. Colloid-borne forms of tetravalent actinides: a brief review.

    Science.gov (United States)

    Zänker, Harald; Hennig, Christoph

    2014-02-01

    Tetravalent actinides, An(IV), are usually assumed to be little mobile in near-neutral environmental waters because of their low solubility. However, there are certain geochemical scenarios during which mobilization of An(IV) in a colloid-borne (waterborne) form cannot be ruled out. A compilation of colloid-borne forms of tetravalent actinides described so far for laboratory experiments together with several examples of An(IV) colloids observed in field experiments and real-world scenarios are given. They are intended to be a knowledge base and a tool for those who have to interpret actinide behavior under environmental conditions. Synthetic colloids containing structural An(IV) and synthetic colloids carrying adsorbed An(IV) are considered. Their behavior is compared with the behavior of An(IV) colloids observed after the intentional or unintentional release of actinides into the environment. A list of knowledge gaps as to the behavior of An(IV) colloids is provided and items which need further research are highlighted. Copyright © 2013 Elsevier B.V. All rights reserved.

  12. Synthesis and structural characterization of actinide oxalate compounds

    International Nuclear Information System (INIS)

    Tamain, C.

    2011-01-01

    Oxalic acid is a well-known reagent to recover actinides thanks to the very low solubility of An(IV) and An(III) oxalate compounds in acidic solution. Therefore, considering mixed-oxide fuel or considering minor actinides incorporation in ceramic fuel materials for transmutation, oxalic co-conversion is convenient to synthesize mixed oxalate compounds, precursors of oxide solid solutions. As the existing oxalate single crystal syntheses are not adaptable to the actinide-oxalate chemistry or to their manipulation constrains in gloves box, several original crystal growth methods were developed. They were first validate and optimized on lanthanides and uranium before the application to transuranium elements. The advanced investigations allow to better understand the syntheses and to define optimized chemical conditions to promote crystal growth. These new crystal growth methods were then applied to a large number of mixed An1(IV)-An2(III) or An1(IV)-An2(IV) systems and lead to the formation of the first original mixed An1(IV)-An2(III) and An1(IV)-An2(IV) oxalate single crystals. Finally thanks to the first thorough structural characterizations of these compounds, single crystal X-ray diffraction, EXAFS or micro-RAMAN, the particularly weak oxalate-actinide compounds structural database is enriched, which is essential for future studied nuclear fuel cycles. (author) [fr

  13. Review of the sorption of actinides on natural minerals

    International Nuclear Information System (INIS)

    Beall, G.W.

    1981-01-01

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

  14. 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.)

  15. Actinide Sputtering Induced by Fission with Ultra-cold Neutrons

    Science.gov (United States)

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

    2017-09-01

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

  16. Inhaled actinides: some safety issues and some research problems

    International Nuclear Information System (INIS)

    Bair, W.J.

    1978-01-01

    The following topics are discussed: limited research funds; risk coefficients for inhaled particles; the hot particle hypothesis; the Gofman-Martell contention; critical tissues for inhaled actinides inhalation hazards associated with future nuclear fuel cycles; and approach to be used by the inhalation panel

  17. 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).

  18. Cerium compounds in the fashion of the light actinides

    International Nuclear Information System (INIS)

    Koelling, D.D.

    1984-01-01

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

  19. Soft X-ray scanning transmission x-ray microscopy (STXM) of actinide materials

    International Nuclear Information System (INIS)

    Shuh, D.K.; Nilsson, H.J.; Wilson, R.E.; Tyliszczak, T.; Nico, P.S.; Werme, L.; Nilsson, H.J.; Werme, L.

    2007-01-01

    Full text of publication follows: Scanning transmission X-ray microscopy (STXM) spectro-microscopy at the Advanced Light Source Molecular Environmental Science (ALS-MES) Beamline 11.0.2 has been utilized to investigate actinide materials, particulates, and actinide-related materials. The ALS-MES STXM utilizes near-edge X-ray absorption fine structure (NEXAFS) at the actinide 4d core level edges (700 eV to 900 eV) to obtain direct spectroscopic information from actinide materials and is capable of imaging particles in several modes, both with a spatial resolution better than 30 nm. An important characteristic of the ALS-MES STXM is the capability to directly probe light clement K-edges by NEXAFS, such as the oxygen and nitrogen K-edges, that are frequently key constituents of actinide materials. The safety precautions for STXM investigations of actinides require sealed encapsulation of the actinide materials between two thin silicon nitride windows. This practical level of experimental safety makes STXM an efficient method for collecting NEXAFS spectra from radioactive materials. The results from early studies of model, light actinide oxides will be presented, demonstrating the experimental capabilities and limitations of soft X-ray STXM spectro-microscopy for investigations of actinide materials. The spectroscopic results from recent transuranic STXM investigations, along with their light element constituents, will be presented. The imaging capabilities of STXM provide a means to observe the morphology actinide-containing particulates, even when fully-hydrated, at a level that approaches the nano-scale. The results from actinide, radionuclide, and lanthanide (used as a surrogate or for a direct comparison to actinide behaviour) experiments including those focused on elucidating fundamental bonding characteristics and of environmental interests, will also be highlighted. However, there are drawbacks and the need to work at the actinide 4d edges imposes cross

  20. Innovative SANEX process for trivalent actinides separation from PUREX raffinate

    International Nuclear Information System (INIS)

    Sypula, Michal

    2013-01-01

    Recycling of nuclear spent fuel and reduction of its radiotoxicity by separation of long-lived radionuclides would definitely help to close the nuclear fuel cycle ensuring sustainability of the nuclear energy. Partitioning of the main radiotoxicity contributors followed by their conversion into short-lived radioisotopes is known as partitioning and transmutation strategy. To ensure efficient transmutation of the separated elements (minor actinides) the content of lanthanides in the irradiation targets has to be minimised. This objective can be attained by solvent extraction using highly selective ligands that are able to separate these two groups of elements from each other. The objective of this study was to develop a novel process allowing co-separation of minor actinides and lanthanides from a high active acidic feed solution with subsequent actinide recovery using just one cycle, so-called innovative SANEX process. The conditions of each step of the process were optimised to ensure high actinide separation efficiency. Additionally, screening tests of several novel lipophilic and hydrophilic ligands provided by University of Twente were performed. These tests were aiming in better understanding the influence of the extractant structural modifications onto An(III)/Ln(III) selectivity and complexation properties. Optimal conditions for minor actinides separation were found and a flow-sheet of a new innovative SANEX process was proposed. Tests using a single centrifugal contactor confirmed high Eu(III)/Am(III) separation factor of 15 while the lowest SF Ln/Am obtained was 6,5 (for neodymium). In addition, a new masking agent for zirconium was found as a substitution for oxalic acid. This new masking agent (CDTA) was also able to mask palladium without any negative influence on An(III)/Ln(III). Additional tests showed no influence of CDTA on plutonium present in the feed solution unlike oxalic acid which causes Pu precipitation. Therefore, CDTA was proposed as a Zr

  1. Assessment of Partitioning Processes for Transmutation of Actinides

    International Nuclear Information System (INIS)

    2010-04-01

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

  2. Innovative SANEX process for trivalent actinides separation from PUREX raffinate

    Energy Technology Data Exchange (ETDEWEB)

    Sypula, Michal

    2013-07-01

    Recycling of nuclear spent fuel and reduction of its radiotoxicity by separation of long-lived radionuclides would definitely help to close the nuclear fuel cycle ensuring sustainability of the nuclear energy. Partitioning of the main radiotoxicity contributors followed by their conversion into short-lived radioisotopes is known as partitioning and transmutation strategy. To ensure efficient transmutation of the separated elements (minor actinides) the content of lanthanides in the irradiation targets has to be minimised. This objective can be attained by solvent extraction using highly selective ligands that are able to separate these two groups of elements from each other. The objective of this study was to develop a novel process allowing co-separation of minor actinides and lanthanides from a high active acidic feed solution with subsequent actinide recovery using just one cycle, so-called innovative SANEX process. The conditions of each step of the process were optimised to ensure high actinide separation efficiency. Additionally, screening tests of several novel lipophilic and hydrophilic ligands provided by University of Twente were performed. These tests were aiming in better understanding the influence of the extractant structural modifications onto An(III)/Ln(III) selectivity and complexation properties. Optimal conditions for minor actinides separation were found and a flow-sheet of a new innovative SANEX process was proposed. Tests using a single centrifugal contactor confirmed high Eu(III)/Am(III) separation factor of 15 while the lowest SF{sub Ln/Am} obtained was 6,5 (for neodymium). In addition, a new masking agent for zirconium was found as a substitution for oxalic acid. This new masking agent (CDTA) was also able to mask palladium without any negative influence on An(III)/Ln(III). Additional tests showed no influence of CDTA on plutonium present in the feed solution unlike oxalic acid which causes Pu precipitation. Therefore, CDTA was proposed as

  3. Actinide science with soft x-ray synchrotron radiation

    International Nuclear Information System (INIS)

    Shuh, D.

    2002-01-01

    Several workshops, some dating back more than fifteen years, recognised both the potential scientific impact and opportunities that would be made available by the capability to investigate actinide materials in the vacuum ultraviolet (VUV)/soft X-ray region of the synchrotron radiation (SR) spectrum. This spectral region revolutionized the approach to surface materials chemistry and physics nearly two decades ego. The actinide science community was unable to capitalize on these SR methodologies for the study of actinide materials until recently because of radiological safety concerns. ,The Advanced Light Source (ALS) at LBNL is a third-generation light source providing state-of-the-art performance in the VUV/soft X-ray region. Along with corresponding improvements in detector and vacuum technology, the ALS has rendered experiments with small amounts of actinide materials possible. In particular, it has been the emergence and development of micro-spectroscopic techniques that have enabled investigations of actinide materials at the ALS. The primary methods for the experimental investigation of actinide materials in the VUV/soft X-ray region are the complementary photoelectron spectroscopies, near-edge X-ray absorption fine structure (NEXAFS) and X-ray emission spectroscopy (XES) techniques. Resonant photo-emission is capable of resolving the 5f electron contributions to actinide bonding and can be used to characterise the electronic structure of actinide materials. This technique is clearly a most important methodology afforded by the tunable SR source. Core level and valence band photoelectron spectroscopies are valuable for the characterisation of the electronic properties of actinide materials, as well as for general analytical purposes. High-resolution core-level photo-emission and resonant photo-emission measurements from the a (monoclinic) and δ (FCC) allotropic phases of plutonium metal have been collected on beam line 7.0 at the ALS and the spectra show

  4. Fission product and actinide data status in ENDF/B

    International Nuclear Information System (INIS)

    England, T.R.; Young, P.G.; Schenter, R.E.; Mann, F.M.; Reich, C.W.

    1984-01-01

    The US Evaluated Nuclear Data Files (ENDF/B) have been very successful in this country and internationally. The data are used directly in calculations or as a reference for comparison with new measurements and other international data bases. The data formats, being particularly suited for computer processing codes, have been recommended by the IAEA as the preferred method of exchange for international data. Part of this success is due to a remarkably free exchange of data nationally and internationally. Additionally, of course, it is due to the many needs for such a comprehensive, evaluated data base. The current version, ENDF/B-V was released in 1979 and 1980. Both ENDF/B-IV and -V were greatly expanded in the areas of fission products and actinides, and the cross section evaluations have been improved in each new version. ENDF/B-VI was originally scheduled for completion in late 1986. However, this schedule is now questionable, as is, the extent of its content. Comments are directed at the improvements we feel are needed for ENDF/B-VI, irrespective of the time scale or probability of implementation. Additionally, we limit our considerations to fission products and heavy nuclides (which we loosely call actinides) and specifically to plans at Los Alamos National Laboratory (LANL), Hanford Engineering and Development Laboratory (HEDL), and Idaho National Engineering Laboratory (INEL). In our coverage we emphasize cross sections and yields for fission products and decay data for both fission products and actinides. We do not attempt complete coverage of planned evaluations of actinide cross sections nor other ENDF/B general and special purpose files (e.g., General Purpose, Activation, Standards, etc.), although some of the data we cite lies in those files. However, our summary of data content in the current ENDF/B-V files is complete for fission products and actinides

  5. Systematic study of neutron induced reactions of the actinide nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Maslov, V.M. [Akadehmiya Navuk Belarusi, Minsk (Belarus). Inst. Radyyatsyjnykh Fizika-Khimichnykh Prablem; Kikuchi, Yasuyuki

    1996-06-01

    A statistical theory is used for the calculation of the neutron-induced reaction cross sections of actinide nuclides from 10 keV up to 20 MeV. Available experimental data bases for major actinides were extensively used to develop theoretical tools for consistent evaluation of neutron data of minor actinides. The approach employed up to the second chance fission threshold is based on the full-scale Hauser-Feshbach theory, a phenomenological modelling of level densities, the giant dipole resonance model for gamma-ray emission, the double-humped fission barrier model and the coupled channel optical model calculations. The pairing, collective and shell effects are introduced into the level density model for equilibrium and saddle point deformations. Step-like structures observed in fission cross section of {sup 235}U around 1 MeV incident neutron energies are interpreted as due to pairing effects. Pairing correlation parameters are adjusted to fit the fission cross section slope in the first plateau region. The level density collective effect inclusion influences drastically the extracted experimental fission barrier parameters due to the inner saddle point asymmetry. The shell effects dumping is manifested as a consistent fit of fission data above the second chance fission threshold. In case of minor actinides, fission data fits are used as a constraint for capture and inelastic scattering cross section predictions. The capture cross sections were analyzed with the allowance for (n,{gamma}n`) and (n,{gamma}f) reactions. To fit the high-energy tails in the (n,2n) reaction, the pre-equilibrium processes in the neutron channel were included. All these effects were modelled, and the model parameters were obtained using major actinides neutron data. The resulted parameter systematics were applied for analysis of available data and prediction of capture, inelastic scattering, (n,2n), (n,3n) reaction and fission cross sections. (J.P.N.). 87 refs.

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

    International Nuclear Information System (INIS)

    Dahou, S.

    2010-01-01

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

  7. Lauriston S. Taylor Lecture: the quest for therapeutic actinide chelators.

    Science.gov (United States)

    Durbin, Patricia W

    2008-11-01

    All of the actinides are radioactive. Taken into the body, they damage and induce cancer in bone and liver, and in the lungs if inhaled, and U(VI) is a chemical kidney poison. Containment of radionuclides is fundamental to radiation protection, but if it is breached accidentally or deliberately, decontamination of exposed persons is needed to reduce the consequences of radionuclide intake. The only known way to reduce the health risks of internally deposited actinides is to accelerate their excretion with chelating agents. Ethylendiaminetetraacetic acid (EDTA) and diethylenetriaminepentaacetic acid (DTPA) were introduced in the 1950's. DTPA is now clinically accepted, but its oral activity is low, it must be injected as a Ca(II) or Zn(II) chelate to avoid toxicity, and it is structurally unsuitable for chelating U(VI) or Np(V). Actinide penetration into the mammalian iron transport and storage systems suggested that actinide ions would form stable complexes with the Fe(III)-binding units found in potent selective natural iron chelators (siderophores). Testing of that biomimetic approach began in the late 1970's with the design, production, and assessment for in vivo Pu(IV) chelation of synthetic multidentate ligands based on the backbone structures and Fe(III)-binding groups of siderophores. New efficacious actinide chelators have emerged from that program, in particular, octadentate 3,4,3-LI(1,2-HOPO) and tetradentate 5-LIO(Me-3,2-HOPO) have potential for clinical acceptance. Both are much more effective than CaNa3-DTPA for decorporation of Pu(IV), Am(III), U(VI), and Np(IV,V), they are orally active, and toxicity is acceptably low at effective dosage.

  8. The effect of high pressures on actinide metals

    International Nuclear Information System (INIS)

    Benedict, U.

    1987-01-01

    The solid state properties of the actinides are controlled by the dualism of the localized and itinerant (delocalized) configuration of the 5f electrons. This dualism allows to define two main subgroups. At ambient pressures the first subgroup, of elements with atomic number 91 to 94, is characterized by 5f electrons in an itinerant state and the second subgroup, atomic number 95 to 98, by 5f electrons in a localized state. The latter means that these electrons have well defined energy levels and do not contribute to the metallic bond. The other two subgroups consist of thorium, as a subgroup of its own because its 5f levels are practically unoccupied in the ground state configuration, and of the five heaviest elements with atomic number 99 to 103. The most remarkable effect of pressure on the actinide metals is that due to closer contact between the lattice atoms, localized 5f electrons can become itinerant, hybridise with the conduction electrons and participate in the metallic bond. In this chapter the high-pressure structural behaviour of actinide metals is reviewed. Section 3 gives an introduction into the techniques of generating and measuring pressure and of determining various physical properties of the actinides under pressure and describes a few high-pressure devices and methods. Sections 4 to 7 treat the high-pressure results for each subgroup separately. In section 8 the results of the preceding sections are brought together in a graphical representation which consists of interconnecting binary phase diagrams of neighbouring actinide metals. 155 refs.; 14 figs.; 7 tabs. (H.W.)

  9. The INE-Beamline for actinide science at ANKA

    Science.gov (United States)

    Rothe, J.; Butorin, S.; Dardenne, K.; Denecke, M. A.; Kienzler, B.; Löble, M.; Metz, V.; Seibert, A.; Steppert, M.; Vitova, T.; Walther, C.; Geckeis, H.

    2012-04-01

    Since its inauguration in 2005, the INE-Beamline for actinide research at the synchrotron source ANKA (KIT North Campus) provides dedicated instrumentation for x-ray spectroscopic characterization of actinide samples and other radioactive materials. R&D work at the beamline focuses on various aspects of nuclear waste disposal within INE's mission to provide the scientific basis for assessing long-term safety of a final nuclear waste repository. The INE-Beamline is accessible for the actinide and radiochemistry community through the ANKA proposal system and the European Union Integrated Infrastructure Initiative ACTINET-I3. Experiments with activities up to 1 × 10+6 times the European exemption limit are feasible within a safe but flexible containment concept. Measurements with monochromatic radiation are performed at photon energies varying between ˜2.1 keV (P K-edge) and ˜25 keV (Pd K-edge), including the lanthanide L-edges and the actinide M- and L3-edges up to Cf. The close proximity of the INE-Beamline to INE controlled area labs offers infrastructure unique in Europe for the spectroscopic and microscopic characterization of actinide samples. The modular beamline design enables sufficient flexibility to adapt sample environments and detection systems to many scientific questions. The well-established bulk techniques x-ray absorption fine structure (XAFS) spectroscopy in transmission and fluorescence mode have been augmented by advanced methods using a microfocused beam, including (confocal) XAFS/x-ray fluorescence detection and a combination of (micro-)XAFS and (micro-)x-ray diffraction. Additional instrumentation for high energy-resolution x-ray emission spectroscopy has been successfully developed and tested.

  10. The INE-Beamline for actinide science at ANKA

    International Nuclear Information System (INIS)

    Rothe, J.; Dardenne, K.; Denecke, M. A.; Kienzler, B.; Loeble, M.; Metz, V.; Steppert, M.; Vitova, T.; Geckeis, H.; Butorin, S.; Seibert, A.; Walther, C.

    2012-01-01

    Since its inauguration in 2005, the INE-Beamline for actinide research at the synchrotron source ANKA (KIT North Campus) provides dedicated instrumentation for x-ray spectroscopic characterization of actinide samples and other radioactive materials. R and D work at the beamline focuses on various aspects of nuclear waste disposal within INE's mission to provide the scientific basis for assessing long-term safety of a final nuclear waste repository. The INE-Beamline is accessible for the actinide and radiochemistry community through the ANKA proposal system and the European Union Integrated Infrastructure Initiative ACTINET-I3. Experiments with activities up to 1 x 10 +6 times the European exemption limit are feasible within a safe but flexible containment concept. Measurements with monochromatic radiation are performed at photon energies varying between ∼2.1 keV (P K-edge) and ∼25 keV (Pd K-edge), including the lanthanide L-edges and the actinide M- and L3-edges up to Cf. The close proximity of the INE-Beamline to INE controlled area labs offers infrastructure unique in Europe for the spectroscopic and microscopic characterization of actinide samples. The modular beamline design enables sufficient flexibility to adapt sample environments and detection systems to many scientific questions. The well-established bulk techniques x-ray absorption fine structure (XAFS) spectroscopy in transmission and fluorescence mode have been augmented by advanced methods using a microfocused beam, including (confocal) XAFS/x-ray fluorescence detection and a combination of (micro-)XAFS and (micro-)x-ray diffraction. Additional instrumentation for high energy-resolution x-ray emission spectroscopy has been successfully developed and tested.

  11. Actinide-aluminate Speciation in Alkaline Radioactive Waste

    International Nuclear Information System (INIS)

    Clark, David C.; Krot, Nikolai N.

    2000-01-01

    Highly alkaline radioactive waste tanks contain a number of transuranic species, in particular U, Np, Pu, and Am-the exact forms of which are currently unknown. Knowledge of actinide speciation under highly alkaline conditions is essential towards understanding and predicting their solubility and sorption behavior in tanks, determining whether chemical separations are needed for waste treatment, and designing separations processes. Baseline washing of tank sludges with NaOH solutions is being proposed to reduce the volume of HLW. Alkaline pretreatment of HLW will be needed to remove aluminum [as NaAl(OH)4] because it significantly reduces the HLW volume; however, the aluminate ion [Al(OH)4 -] enhances actinide solubility via an unknown mechanism. Thus, alkaline wash residues may require an additional treatment to remove actinides. The results of this research will determine the nature TRU (U, Np, Pu, Am) speciation with aluminate anions under alkaline, oxidizing tank-like conditions. Specific issues to be addressed include solubility of these actinides, speciation in aluminate-containing alkaline supernatants, the role of actinide redox states on solubility, and partitioning between supernatant and solid phases, including colloids. Studies will include thermodynamics, kinetics, spectroscopy, electrochemistry, and surface science. We have already determined, for example, that certain high valent forms of Np and Pu are very soluble under alkaline conditions due to the formation of anionic hydroxo complexes, AnO2(OH)4 2- and AnO2(OH)5 3-. The presence of aluminate ions causes the actinide solubilities to increase, although the exact species are not known. We are currently characterizing the high valent TRU elements bound to oxo, water, OH-, and Al(OH)4 -, ligands under waste-like conditions. These waste-like conditions are in the range of 1-3 M excess hydroxide, ∼0.2 M carbonate, ∼0.5 M aluminate, for a total sodium of 2-4 M. Molecular structure-specific probes

  12. Extraction of DBP and MBP from actinides: application to the recovery of actinides from TBP--Na2CO3 scrub solutions

    International Nuclear Information System (INIS)

    Horwitz, E.P.; Mason, G.W.; Bloomquist, C.A.A.; Leonard, R.A.; Bernstein, G.J.

    1979-01-01

    A flowsheet for the recovery of actinides from TBP--Na 2 CO 3 scrub waste solutions has been developed, based on batch extraction data, and tested, using laboratory scale counter-current extraction techniques. The process utilizes 2-ethyl-1-hexanol (2-EHOH) to extract the TBP degradation products (HDBP and H 2 MBP) from acidified Na 2 CO 3 scrub waste leaving the actinides in the aqueous phase. Dibutyl and monobutyl phosphoric acids are attached to the 2-EHOH molecules through hydrogen bonds. These hydrogen bonds also diminish the ability of the HDBP and H 2 MBP to complex actinides and thus all actinides remain in the aqueous raffinate. Dilute sodium hydroxide solutions can be used to back-extract the dibutyl and monobutyl phosphoric acid esters as their sodium salts. The 2-EHOH can then be recycled. After extraction of the acidified carbonate waste with 2-EHOH, the actinides may be readily extracted from the raffinate with DHDECMP or, in the case of tetra- and hexavalent actinides, with TBP. The alcohol extraction (ARALEX) process is relatively simple and involves inexpensive and readily available chemicals. The ARALEX process can also be applied to other actinide waste streams which contain appreciable concentrations of polar organic compounds that interfere with conventional actinide ion exchange and liquid--liquid extraction procedures

  13. 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)

  14. ACTINIDE-ALUMINATE SPECIATION IN ALKALINE RADIOACTIVE WASTE

    International Nuclear Information System (INIS)

    Clark-Deaborg, David

    2001-01-01

    Highly alkaline radioactive waste tanks contain a number of transuranic species, in particular U, Np, Pu, and Am--the exact forms of which are currently unknown. Knowledge of actinide speciation under highly alkaline conditions is essential towards understanding and predicting their solubility and sorption behavior in tanks, determining whether chemical separations are needed for waste treatment, and designing separations processes. Baseline washing of tank sludges with NaOH solutions is being proposed to reduce the volume of HLW. Alkaline pretreatment of HLW will be needed to remove aluminum [as NaAl(OH) 4 ] because it significantly reduces the HLW volume; however, aluminate [Al(OH) 4 - ] enhances actinide solubility via an unknown mechanism. Thus, alkaline wash residues may require an additional treatment to remove actinides. The results of this research will determine the nature TRU (Np, Pu, Am) speciation with aluminate anions under alkaline, oxidizing tank-like conditions. Specific issues to be addressed include solubility of these actinides, speciation in aluminate-containing alkaline supernatants, the role of actinide redox states on solubility, and partitioning between supernatant and solid phases, including colloids. Studies will include thermodynamics, kinetics, spectroscopy, electrochemistry, etc. It is already known, for example, that certain high valent forms of NF and Pu are very soluble under alkaline conditions due to the formation of anionic hydroxo complexes, AnO 2 (OH) 4 2- and AnO 2 (OH) 5 3- . The presence of aluminate ions causes the actinide solubilities to increase, although the exact species have only been determined during this program. We are continuing to characterize high-valent TRU elements bound to oxo, water, OH - , under waste-like and sludge washing conditions. These conditions are in the range of 1-3 M excess hydroxide, ∼0.2 M carbonate, ∼0.5 M aluminate, for a total sodium of 2-4 mols/kg. Molecular structure-specific probes

  15. Actinides and fission products partitioning from high level liquid waste

    International Nuclear Information System (INIS)

    Yamaura, Mitiko

    1999-01-01

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

  16. Actinide coordination chemistry: towards the limits of the periodic table; Chimie de coordination des actinides: vers les frontieres du tableau periodique

    Energy Technology Data Exchange (ETDEWEB)

    Den Auwer, C.; Moisy, P. [CEA Marcoule (DEN/DRCP/SCPS), 30 (France); Simoni, E. [Paris-11 Univ., 91 - Orsay (France). Inst. de Physique Nucleaire

    2009-05-15

    Actinide elements represent a distinct chemical family at the bottom of the periodic table. Among the major characteristics of this 14 element family is their high atomic numbers and their radioactivity. Actinide chemistry finds its roots in the history of the 20. century and plays a very important role in our contemporary world. Energetic as well as technical challenges are facing the development of nuclear energy. In this pedagogical introduction to actinide chemistry, the authors draw a comparison between the actinides family and the chemistry of two other families, lanthanides and transition metals. This article focuses on molecular and aqueous chemistry. It has been based on class notes aiming to present an overview of the chemical diversity of actinides, and its future challenges for modern science. (authors)

  17. Determination of bis-carboxyethyl germanium sesquioxide by gas chromatography with microwave-induced plasma-atomic emission detection after derivatization with alkyl chloroformates.

    Science.gov (United States)

    Trikas, E; Zachariadis, G A; Rosenberg, E

    2014-05-01

    Organic germanium compounds, especially Ge-132, more corrctly denoted as bis-beta-carboxyethyl germanium sesquioxide ([Ge(=O)CH2CH2CO2H]2O), are of continued interest as they are said to promote health and display anticancer activity. Although these beneficial effects have never been substantiated by comprehensive clinical studies, this drug can still be obtained through various sources and is usually marketed as a nutritional supplementation rather than an anticancer medication. As the quality standards under which this drug is produced are unknown, the need for an effective quality control of these products arises. To date, Ge-132 is considered generally as a safe compound for application in contrast to inorganic germanium which demonstrates severe renal toxicity. In this paper, a new approach to the determination of Ge-132, based on derivatization by ethyl chloroformate reagent (ECF), in the presence of ethanol and pyridine in the mixture, and subsequent analysis by gas chromatography coupled with microwave-induced plasma-atomic emission detection (GC-MIP-AED), is reported. Reaction conditions of the derivatization procedure were optimized with particular respect to the reagent (ECF) and catalyst (pyridine) concentrations. The proposed method is capable of distinguishing Ge-132 from inorganic germanium. The derivatization procedure was also tested with the use of methyl chloroformate (MCF) as alternative reagent, providing interesting additional information about the nature of the final product and the proposed reaction scheme. Among the two types of chloroformates, i.e., MCF and ECF, the latter proved to be more suitable for the proposed method, providing a calibration curve of superior sensitivity and linearity compared with the one obtained with MCF. The method was applied successfully in three real samples, two food supplements, and one commercially available fertilizer. The analysis of the Ge-132 derivative showed good linearity in the concentration of 1

  18. Photochemistry in terrestrial exoplanet atmospheres. III. Photochemistry and thermochemistry in thick atmospheres on super Earths and mini Neptunes

    International Nuclear Information System (INIS)

    Hu, Renyu; Seager, Sara

    2014-01-01

    Some super Earths and mini Neptunes will likely have thick atmospheres that are not H 2 -dominated. We have developed a photochemistry-thermochemistry kinetic-transport model for exploring the compositions of thick atmospheres on super Earths and mini Neptunes, applicable for both H 2 -dominated atmospheres and non-H 2 -dominated atmospheres. Using this model to study thick atmospheres for wide ranges of temperatures and elemental abundances, we classify them into hydrogen-rich atmospheres, water-rich atmospheres, oxygen-rich atmospheres, and hydrocarbon-rich atmospheres. We find that carbon has to be in the form of CO 2 rather than CH 4 or CO in a H 2 -depleted water-dominated thick atmosphere and that the preferred loss of light elements from an oxygen-poor carbon-rich atmosphere leads to the formation of unsaturated hydrocarbons (C 2 H 2 and C 2 H 4 ). We apply our self-consistent atmosphere models to compute spectra and diagnostic features for known transiting low-mass exoplanets GJ 1214 b, HD 97658 b, and 55 Cnc e. For GJ 1214 b, we find that (1) C 2 H 2 features at 1.0 and 1.5 μm in transmission and C 2 H 2 and C 2 H 4 features at 9-14 μm in thermal emission are diagnostic for hydrocarbon-rich atmospheres; (2) a detection of water-vapor features and a confirmation of the nonexistence of methane features would provide sufficient evidence for a water-dominated atmosphere. In general, our simulations show that chemical stability has to be taken into account when interpreting the spectrum of a super Earth/mini Neptune. Water-dominated atmospheres only exist for carbon to oxygen ratios much lower than the solar ratio, suggesting that this kind of atmospheres could be rare.

  19. Effects of humic substances on the migration of radionuclides: Complexation of actinides with humic substances

    International Nuclear Information System (INIS)

    Kim, J.I.; Rhee, D.S.; Wimmer, H.; Buckau, G.; Klenze, R.; Decambox, P.; Moulin, C.; Moulin, V.; Tits, J.; Marquardt, C.; Herrmann, G.; Trautmann, N.; Dierckx, A.; Vancluysen, J.; Maes, A.

    1992-09-01

    The aim of the present research programme is to study the complexation behaviour of actinide ions with humic substances in natural aquifer systems and hence to quantify the effect of humic substances on the actinide migration. Aquatic humic substances commonly found in all groundwaters in different concentrations have a strong tendency towards complexation with actinide ions. This is one of the major geochemical reactions but hitherto least quantified. Therefore, the effect of humic substances on the actinide migration is poorly understood. In the present research programme the complexation of actinide ions with humic substances will be described thermodynamically. This description will be based on a model being as simple as possible to allow an easy introduction of the resulting constants into geochemical modelling of the actinide migration. (orig.)

  20. Effects of humic substances on the migration of radionuclides: complexation of actinides with humic substances

    International Nuclear Information System (INIS)

    Kim, J.I.; Buckau, G.

    1993-01-01

    The aim of the present research programme is to study the complexation behaviour of actinide ions with humic substances in natural aquifer systems and hence to quantify the effect of humic substances on the actinide migration. Aquatic humic substances commonly found in all groundwaters in different concentrations have a strong tendency towards complexation with actinide ions. This is one of the major geochemical reactions but hitherto least quantified. Therefore, the effect of humic substances on the actinide migration is poorly understood. In the present research programme the complexation of actinide ions with humic substances will be described thermodynamically. This description will be based on a model being as simple as possible to allow an easy introduction of the resulting constants into geochemical modelling of the actinide migration. 13 refs

  1. Preparation of isotopes and sources of actinide elements

    International Nuclear Information System (INIS)

    Madic, C.; Bourges, J.; Koehly, G.

    1984-09-01

    As the C.E.A. possesses no isotopic separation facility, the productions of isotopes of actinide elements are performed: a) by neutron irradiation and chemical treatment of special targets, b) by milking decay products from stocks of aged actinide elements, c) by chemical treatment of alpha active wastes. These productions concern the following isotopes: 233 U, 238 Pu, 242 Pu, 243 Cm, 242 Cm, 244 Cm (a); 228 Th, 229 Th, 234 U, 237 U, 239 Np, 240 Pu, 241 Am, 248 Cm (b); 237 Np, 241 Am (c). These isotopes are produced to satisfy French and international needs and are sent to users in various forms: solutions, metals, oxides, fluorides, or in different sources forms. The preparation of the sources represents an important field of activities divided into two parts: 1/Industrial sources: production of large series of different sources, 2/ Scientific sources: production of sources suitable for a specific scientific problem. A large overview of these activities is given

  2. Status of measurements of fission neutron spectra of Minor Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Drapchinsky, L.; Shiryaev, B. [V.G. Khlopin Radium Inst., Saint Petersburg (Russian Federation)

    1997-03-01

    The report considers experimental and theoretical works on studying the energy spectra of prompt neutrons emitted in spontaneous fission and neutron induced fission of Minor Actinides. It is noted that neutron spectra investigations were done for only a small number of such nuclei, most measurements, except those of Cf-252, having been carried out long ago by obsolete methods and imperfectapparatus. The works have no detailed description of experiments, analysis of errors, detailed numerical information about results of experiments. A conclusion is made that the available data do not come up to modern requirements. It is necessary to make new measurements of fission prompt neutron spectra of transuranium nuclides important for the objectives of working out a conception of minor actinides transmutation by means of special reactors. (author)

  3. Biogeochemistry of actinides: a nuclear fuel cycle perspective

    International Nuclear Information System (INIS)

    Bondietti, E.A.; Trabalka, J.R.; Garten, C.T.; Killough, G.G.

    1979-01-01

    Through an examination of the comparative behavior of the actinide elements in terrestrial and aquatic food chains, the anticipated accumulation behavior of the transuranium elements by people was described. The available data suggests that Pu, Am, and Cm will not accumulate to a greater degree than U in the skeletons of individuals exposed to environmentally dispersed activity. The nature of the contamination event, the chemical and physical associations in soils and sediments, the proximity to the contamination site - all will influence observed behavior. Because of the establishment of regulatory guidelines for limiting chronic exposure to transuranium elements, research on environmental behavior must address the question of accumulation by people. In the absence of lifetime accumulation data and the paucity of contaminated sites, approaches such as those documented in this paper may aid in understanding and evaluating the hazards of releasing actinide elements to the biosphere

  4. Atomic properties of actinide ions with particle-hole configurations

    Science.gov (United States)

    Safronova, M. S.; Safronova, U. I.; Kozlov, M. G.

    2018-01-01

    We study the effects of higher-order electronic correlations in the systems with particle-hole excited states using a relativistic hybrid method that combines configuration interaction and linearized coupled-cluster approaches. We find the configuration interaction part of the calculation sufficiently complete for eight electrons while maintaining good quality of the effective coupled-cluster potential for the core. Excellent agreement with experiment was demonstrated for a test case of La3 +. We apply our method for homolog actinide ions Th4 + and U6 + which are of experimental interest due to a puzzle associated with the resonant excitation Stark ionization spectroscopy method. These ions are also of interest to actinide chemistry.

  5. Development of a remote bushing for actinide vitrification

    International Nuclear Information System (INIS)

    Schumacher, R.F.; Ramsey, W.G.; Johnson, F.M.

    1996-01-01

    The Savannah River Site (SRS) and the Savannah River Technology Center (SRTC) are combining their existing experience in handling highly radioactive, special nuclear materials with commercial glass fiberization technology in order to assemble a small vitrification system for radioactive actinide solutions. The vitrification system or open-quotes brushingclose quotes, is fabricated from platinum-rhodium alloy and is based on early marble remelt fiberization technology. Advantages of this unique system include its relatively small size, reliable operation, geometrical safety (nuclear criticality), and high temperature capability. The bushing design should be capable of vitrifying a number of the actinide nuclear materials, including solutions of americium/curium, neptunium, and possibly plutonium. State of the art, mathematical and oil model studies are being combined with basic engineering evaluations to verify and improve the thermal and mechanical design concepts

  6. Actinide-specific sequestering agents and decontamination applications

    Energy Technology Data Exchange (ETDEWEB)

    Smith, William L. [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials and Molecular Research Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Raymond, Kenneth N. [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials and Molecular Research Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry

    1981-04-07

    With the commercial development of nuclear reactors, the actinides have become very important industrial elements. A major concern of the nuclear industry is the biological hazard associated with nuclear fuels and their wastes. The acute chemical toxicity of tetravalent actinides, as exemplified by Th(IV), is similar to Cr(III) or Al(III). However, the acute toxicity of 239Pu(IV) is similar to strychnine, which is much more toxic than any of the non-radioactive metals such as mercury. Although the more radioactive isotopes of the transuranium elements are more acutely toxic by weight than plutonium, the acute toxicities of 239Pu, 241Am, and 244Cm are nearly identical in radiation dose, ~100 μCi/kg in rodents. Finally and thus, the extreme acute toxicity of 239Pu is attributed to its high specific activity of alpha emission.

  7. Review of Integral Experiments for Minor Actinide Management

    International Nuclear Information System (INIS)

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

    2015-01-01

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

  8. Development of ion beam sputtering techniques for actinide target preparation

    International Nuclear Information System (INIS)

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

    1985-01-01

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

  9. Superabsorbing gel for actinide, lanthanide, and fission product decontamination

    Science.gov (United States)

    Kaminski, Michael D.; Mertz, Carol J.

    2016-06-07

    The present invention provides an aqueous gel composition for removing actinide ions, lanthanide ions, fission product ions, or a combination thereof from a porous surface contaminated therewith. The composition comprises a polymer mixture comprising a gel forming cross-linked polymer and a linear polymer. The linear polymer is present at a concentration that is less than the concentration of the cross-linked polymer. The polymer mixture is at least about 95% hydrated with an aqueous solution comprising about 0.1 to about 3 percent by weight (wt %) of a multi-dentate organic acid chelating agent, and about 0.02 to about 0.6 molar (M) carbonate salt, to form a gel. When applied to a porous surface contaminated with actinide ions, lanthanide ions, and/or other fission product ions, the aqueous gel absorbs contaminating ions from the surface.

  10. Quantum chemical calculations on structures of actinide complexes

    International Nuclear Information System (INIS)

    Satoru, Tsushima; Tobias, Reich

    2002-01-01

    The results of our recent theoretical calculations on the structures and the hydration numbers of actinide complexes are discussed together with EXAFS data. The hydration number determined from the calculated Gibbs free energy (inclusive of the solvation energy) was found to be different from the hydration number determined from the electronic energy at 0 K, 0 atm. The roles of entropy and solvation energy were found to be important with regard to the stability of the actinide complexes. The structures of the aqueous uranyl complexes obtained by EXAFS measurements were compared with the structures obtained by 'gas phase' quantum chemical calculations. The importance of including the secondary co-ordination shell and counter-ions is discussed in this paper. (authors)

  11. Analytical separations of lanthanides and actinides by capillary electrophoresis.

    Science.gov (United States)

    Janos, Pavel

    2003-06-01

    The separation of lanthanide and actinide elements belongs to one of the most challenging tasks of the separation science, due to a great similarity in their physical and chemical properties. The electrophoretic separation can be accomplished in the presence of suitable complex-forming agents, from which alpha-hydroxyisobutyric acid (HIBA) has been used most often. In the most effective capillary electrophoretic mode--capillary zone electrophoresis (CZE)--a complete separation of lanthanide ions can be accomplished within a few minutes. Various electrophoretic methods can be relatively easily adopted for the determinations of individual lanthanide elements in certain kinds of technical materials, concentrates, precursors, etc., where the high speed and low costs of analysis characteristics of capillary electrophoresis (CE) may be advantageously exploited. Electrophoretic techniques may also be employed for speciation studies, especially for examinations of the behavior of actinides in the environment.

  12. The pentavalent actinide solution chemistry in the environment.

    Science.gov (United States)

    Topin, Sylvain; Aupiais, Jean

    2016-03-01

    With regard to environmental monitoring of certain nuclear facilities, pentavalent actinides, in particular neptunium and plutonium, play a key role, as the chief soluble, mobile forms of actinides. In the past five years, investigations carried out by hyphenating capillary electrophoresis to ICP-MS (CE-ICP-MS) have allowed a number of hitherto unknown thermodynamic data to be determined for Np(V) and Pu(V) interactions with the chief environmentally abundant anions. For the first time, data were provided for Pu(V) interactions with carbonate, sulfate, oxalate, chloride, and nitrate ions, allowing the Np(V)/Pu(V) analogy to be verified experimentally. Knowledge of Np(V) chemistry, especially in carbonate, and sulfate media, was also refined. These CE-ICP-MS studies, combined with some earlier findings, have brought about a renewal in the knowledge of An(V) chemistry in solution. Copyright © 2016 Elsevier Ltd. All rights reserved.

  13. Actinide analytical program for characterization of Hanford waste

    International Nuclear Information System (INIS)

    Johnson, S.J.; Winters, W.I.

    1977-01-01

    The objective of this program has been to develop faster, more accurate methods for the concentration and determination of actinides at their maximum permissible concentration (MPC) levels in a controlled zone. These analyses are needed to characterize various forms of Hanford high rad waste and to support characterization of products and effluents from new waste management processes. The most acceptable methods developed for the determination of 239 Pu, 238 Pu, 237 Np, 241 Am, and 243 Cm employ solvent extraction with the addition of tracer isotopes. Plutonium and neptunium are extracted from acidified waste solutions into Aliquat-336. Americium and curium are then extracted from the waste solution at the same acidity into dihexyl-N,N-diethylcarbamylmethylenephosphonate (DHDECMP). After back extraction into an aqueous matrix, these actinides are electrodeposited on steel disks for alpha energy analysis. Total uranium and total thorium are also isolated by solvent extraction and determined spectrophotometrically

  14. Single particle orbitals of the heaviest known actinide nuclei

    International Nuclear Information System (INIS)

    Ahmad, I.

    1992-01-01

    Single particle states in the actinide nuclei have been well characterized by decay scheme, (n, γ) and one nucleon transfer reaction studies. The energies of the single particle states are used to calculate the shell corrections which may give rise to stable superheavy elements. Large shell corrections for the superheavy elements arise from the gaps in the proton single-particle spectrum at Z = 114 and in the neutron single-particle spectrum at N = 184. The gap at Z = 114 is determined by the splitting of the f 7/2 and f 5/2 orbitals and the gap at N = 184 is determined by the locations of the h 11/2 , k 17/2 and j 13/2 spherical orbitals. Many of these states have been identified in very heavy actinide nuclei. Experiments identifying these states and the relation of the observed energies to the stability of superheavy elements are discussed

  15. Transmutation of fission products and actinide waste at Hanford

    Energy Technology Data Exchange (ETDEWEB)

    Daemen, L.L.; Pitcher, E.J.; Russell, G.J. [Los Alamos National Laboratory, NM (United States)

    1995-10-01

    The authors studied the neutronics of an ATW system for the transmutation of the fission products ({sup 99}Tc in particular) and the type of actinide waste stored in several tanks at Hanford. The heart of the system is a highly-efficient neutron production target. It is surrounded by a blanket containing a moderator/reflector material, as well as the products to be transmuted. The fission products are injected into the blanket in the form of an aqueous solution in heavy water, whereas an aqueous actinides slurry is circulated in the outer part of the blanket. For the sake of definiteness, the authors focussed on {sup 99}Tc (the most difficult fission product to transmute), and {sup 239}Pu, {sup 237}Np, and {sup 241}Am. Because of the low thermal neutron absorption cross-section of {sup 99}Tc, considerable care and effort must be devoted to the design of a very efficient neutron source.

  16. A reexamination of the incentives for actinide burning

    International Nuclear Information System (INIS)

    Croff, A.G.; Forsberg, C.W.; Ludwig, S.B.

    1990-01-01

    The incentives for actinide burning (AB), also known as partitioning and transmutation, were extensively evaluated over a decade ago by US and foreign investigators. The conclusion was that the cost and short-term risk increases resulting from AB substantially outweighed the long-term reduction in repository risk. However, during the intervening years, many factors relevant to this evaluation have changed, such as (a) expectations concerning the ease with which a repository could be sited and licensed, (b) issuance by regulators of a repository licensing standard and supporting criteria, (c) the scenario to which AB is compared, and (d) new technologies for fuel and waste processing. This paper reexamines the incentives for undertaking actinide burning the content of these new factors. 10 refs., 3 figs

  17. 1982 Annual Status Report Plutonium Fuels and Actinide Programme

    International Nuclear Information System (INIS)

    Lindner, R.

    1983-01-01

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

  18. Selective solvent extraction of actinides associated to liquid scintillation measurements

    International Nuclear Information System (INIS)

    Ardois, C.; Musikas, C.

    1997-01-01

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

  19. Actinide extraction by substituted amides or diamides from carboxylic acids

    International Nuclear Information System (INIS)

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

    1987-01-01

    Amides are studied for use in reprocessing, these solvents can be incinerated and radiolytic degradation have no effect on the process. Main research fields are: 1) Monoamides type RCONR 2 allow U (VI) and Pu (IV) extraction like TBP. Ramified R and R' increase the amount of U extracted, the selectivity U/Pu and U + Pu/Fission products. A counter current test gave encouraging results. 2) Diamides for trivalent actinide extraction from radioactive wastes and especially malonamides. Extraction coefficient in function of HNO 3 concentration are measured for Am (III), En (III), Pu (IV), U (VI) and Zr (IV). Zr should be complexed in aqueous phase to avoid extraction with actinides. Selection of solvent is not yet possible but amides are interesting as alternate extractants [fr

  20. The effects of corrosion product colloids on actinide transport

    International Nuclear Information System (INIS)

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

    1991-11-01

    This report assesses the possible effects of colloidal corrosion products on the transport of actinides from the near field of radioactive waste repositories. The desorption of plutonium and americium from colloidal corrosion products of iron and zirconium was studied under conditions simulating a transition from near-field to far-field environmental conditions. Desorption of actinides occurred slowly from the colloids under far-field conditions. Measurements of particle stability showed all the colloids to be unstable in the near field. Stability increased under far-field conditions or as a result of the evolution of the near field. Migration of colloids from the near field is unlikely except in the presence of organic materials. (Author)

  1. Observation of large scissors resonance strength in actinides.

    Science.gov (United States)

    Guttormsen, M; Bernstein, L A; Bürger, A; Görgen, A; Gunsing, F; Hagen, T W; Larsen, A C; Renstrøm, T; Siem, S; Wiedeking, M; Wilson, J N

    2012-10-19

    The orbital M1 scissors resonance has been measured for the first time in the quasicontinuum of actinides. Particle-γ coincidences are recorded with deuteron and (3)He-induced reactions on (232)Th. The residual nuclei (231,232,233)Th and (232,233) Pa show an unexpectedly strong integrated strength of B(M1)=11-15μ(n)(2) in the E(γ)=1.0-3.5 MeV region. The increased γ-decay probability in actinides due to scissors resonance is important for cross-section calculations for future fuel cycles of fast nuclear reactors and may also have an impact on stellar nucleosynthesis.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-02-24

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

  3. Behaviour of actinides in room temperature ionic liquids

    International Nuclear Information System (INIS)

    Bosse, E.

    2008-07-01

    The room temperature ionic liquids are potentially interesting for the treatment of nuclear fuel. But the knowledge of the behaviour of actinides in the ionic liquids is fragmented because these solvents are new, young and many. In a first time, the ionic liquids [BuMeIm][Tf 2 N] and [MeBu 3 N][Tf 2 N] have been studied in α and γ irradiation with different atmosphere (argon and air) and concentrations of water. ESIMS, NMR and liquid chromatography coupled ESI-MS analysis demonstrate a multitude of degradation products but in very small quantities. This good radiolytic stability makes it a major advantage for the studies of actinides. In a second time, the interaction between an anionic complex of uranium (UCl 6 2- ) and the cation of the ionic liquid and too the study of the hydrolysis of An 4+ (An uranium, neptunium, plutonium) were conducted in different ionic liquids ([MeBu 3 N][Tf 2 N], [BuMe 2 Im][Tf 2 N] and [BuMeIm][Tf 2 N]). The experimental results showed that the intensity of these interactions between UCl 6 2- anion and the ionic liquid cation depends on the latter and follows the order: MeBu 3 N + ∼ BuMe 2 Im + ≤BuMeIm + . In addition, the results obtained by UV/Vis spectroscopy showed that the reaction of hydrolysis in the ionic liquids is slow, secondary compared to the oxidation or the disproportionation and that the amount of water in ionic liquid must be relatively large compared to the concentration of actinide. The results from the coupling of different analytical techniques (NMR, mass spectrometry, UV-Visible, Infra-red, Electrochemistry..) have allowed a first approach in the understanding of the actinides in the room temperature ionic liquids. (author)

  4. Chemical and Ceramic Methods Toward Safe Storage of Actinides

    International Nuclear Information System (INIS)

    P.E.D. Morgan; R.M. Housley; J.B. Davis; M.L. DeHaan

    2005-01-01

    A very important, extremely-long-term, use for monazite as a radwaste encapsulant has been proposed. The use of ceramic La-monazite for sequestering actinides (isolating them from the environment), especially plutonium and some other radioactive elements (e.g., fission-product rare earths), had been especially championed by Lynn Boatner of ORNL. Monazite may be used alone or, copying its compatibility with many other minerals in nature, may be used in diverse composite combinations

  5. Determination of actinides in urine and fecal samples

    Science.gov (United States)

    McKibbin, Terry T.

    1993-01-01

    A method of determining the radioactivity of specific actinides that are carried in urine or fecal sample material is disclosed. The samples are ashed in a muffle furnace, dissolved in an acid, and then treated in a series of steps of reduction, oxidation, dissolution, and precipitation, including a unique step of passing a solution through a chloride form anion exchange resin for separation of uranium and plutonium from americium.

  6. Synthesis and characterization of tetravalent actinide orthophosphates with alkali metals

    International Nuclear Information System (INIS)

    Volkov, Yu.F.; Melkaya, R.F.; Spiryakov, V.I.; Timofeev, G.A.

    1995-01-01

    A series of double phosphates of formula AM 2 (PO 4 ) 3 , where A = Li, Na, K, Rb, Cs; M = U, Np, Pu, is prepared by solid-state reactions. Various polymorphic modifications of AM 2 (PO 4 ) 3 are identified by using X-ray diffraction and IR spectroscopic analyses of the products from stepwise annealing. The crystal structure type, thermal stability of the modifications, and nature of the polymorphic transformations depend on the nature of the actinide and alkali metal

  7. Specific heat of actinide compounds at low temperature

    International Nuclear Information System (INIS)

    Novion, C. de.

    1975-01-01

    Actinide compounds show phenomena of self-heating and recovery of self-irradiation induced defects which imply the development of apparatus and special methods for the measurement of their specific heat at low temperature. The case of insulating or semiconductor compounds is considered, with emphasis on the oxides MO 2 . The problem of 5f electrons in metallic compounds, then pure metals and the self-irradiation problems are examined [fr

  8. Impact of actinide recycle on nuclear fuel cycle health risks

    International Nuclear Information System (INIS)

    Michaels, G.E.

    1992-06-01

    The purpose of this background paper is to summarize what is presently known about potential impacts on the impacts on the health risk of the nuclear fuel cycle form deployment of the Advanced Liquid Metal Reactor (ALMR) 1 and Integral Fast Reactor (IF) 2 technology as an actinide burning system. In a companion paper the impact on waste repository risk is addressed in some detail. Therefore, this paper focuses on the remainder of the fuel cycle

  9. Chemical properties of the heavier actinides and transactinides

    Energy Technology Data Exchange (ETDEWEB)

    Hulet, E.K.

    1981-01-01

    The chemical properties of each of the elements 99 (Es) through 105 are reviewed and their properties correlated with the electronic structure expected for 5f and 6d elements. A major feature of the heavier actinides, which differentiates them from the comparable lanthanides, is the increasing stability of the divalent oxidation state with increasing atomic number. The divalent oxidation state first becomes observable in the anhydrous halides of californium and increases in stability through the series to nobelium, where this valency becomes predominant in aqueous solution. In comparison with the analogous 4f electrons, the 5f electrons in the latter part of the series are more tightly bound. Thus, there is a lowering of the 5f energy levels with respect to the Fermi level as the atomic number increases. The metallic state of the heavier actinides has not been investigated except from the viewpoint of the relative volatility among members of the series. In aqueous solutions, ions of these elements behave as a normal trivalent actinides and lanthanides (except for nobelium). Their ionic radii decrease with increasing nuclear charge which is moderated because of increased screening of the outer 6p electrons by the 5f electrons. The actinide series of elements is completed with the element lawrencium (Lr) in which the electronic configuration is 5f/sup 14/7s/sup 2/7p. From Mendeleev's periodicity and Dirac-Fock calculations, the next group of elements is expected to be a d-transition series corresponding to the elements Hf through Hg. The chemical properties of elements 104 and 105 only have been studied and they indeed appear to show the properties expected of eka-Hf and eka-Ta. However, their nuclear lifetimes are so short and so few atoms can be produced that a rich variety of chemical information is probably unobtainable.

  10. Chemical and Ceramic Methods Toward Safe Storage of Actinides

    Energy Technology Data Exchange (ETDEWEB)

    P.E.D. Morgan; R.M. Housley; J.B. Davis; M.L. DeHaan

    2005-08-19

    A very import, extremely-long-term, use for monazite as a radwaste encapsulant has been proposed. THe use of ceramic La-monazite for sequestering actinides (isolating them from the environment), especially plutonium and some other radioactive elements )e.g., fission-product rare earths), had been especially championed by Lynn Boatner of ORNL. Monazite may be used alone or, copying its compatibility with many other minerals in nature, may be used in diverse composite combinations.

  11. Diffusion of actinides in glasses containing model radioactive wastes

    International Nuclear Information System (INIS)

    Ivanov, I.A.; Sedov, V.M.; Gulin, A.N.; Shatkov, V.M.; Shashukov, E.A.

    1990-01-01

    Diffusion coefficients of 237 Np, 239 Pu and 241 Am radionuclides in two model alumophosphate and alumoborosilicate glasses at the temperatures, somewhat lower than their transformation temperature, were determined. It is ascertained that actinides are one of the least mobile elements. It is shown that the glass crystallization results in the increase of 237 Np diffusion mobility. Low enough amount of water absorbed by crystallized alumophosphate glass intensifies low-temperature migration of 237 Np

  12. Diffusion of actinides in glasses containing simulated radioactive wastes

    International Nuclear Information System (INIS)

    Ivanov, I.A.; Sedov, V.M.; Gulin, A.N.; Shatkov, V.M.; Shashukov, E.A.

    1991-01-01

    Diffusion coefficients of radionuclides 237 Pu, 239 Pu and 241 Am in simulated alumina phosphate and alumina borosilicate glasses at temperatures lower than their transformation temperatures were determined. Actinides are known to be the least mobile elements. It is shown that crystallization of glasses leads to increasing 237 Np diffusion mobility. It is also shown that a rather small quantity of water absorbed by a crystallized alumina phosphate glass intensifies low-temperature migration of 237 Np. (author) 6 refs.; 2 tabs

  13. Microphysics Confronted Photoevaporation: Full (Magneto-)Hydrodynamic Simulations Coupled with Consistent Thermochemistry and Radiative Transfer in Protoplanetary Disks and Planet Atmospheres

    Science.gov (United States)

    Wang, Lile

    2018-01-01

    Mechanisms related to microphysics, including thermochemistry and radiative transfer, are important in astrophysical processes but difficult to calculate. Equipped with the computation power of GPUs, we explore protoplanetary disks (PPDs) and planet atmospheres (PAs) by coupling consistent microphysics with (magneto-)hydrodynamics in photoevaporation driven by ultraviolet and X-ray radiation from the host star, which is an important dispersal mechanism for PPDs and PAs. We develop updated understandings towards the underlying processes that determine the local thermo-/hydrodynamic evolution, as well as the global structures, of photoevaporating systems. Observable molecules including CO, OH and H2O may re-form and survive at relatively high wind temperatures due to reactions being out of equilibrium. Mass-loss rates are sensitive to the intensity of radiation in energy bands that interact directly with hydrogen. Comparison with previous works shows that mass loss rates are also sensitive to the treatment of both the hydrodynamics and the thermochemistry. Divergent results concerning the efficiency of X-ray photoevaporation are traced in part to differing assumptions about dust and other coolants.

  14. Establishment of a room temperature molten salt capability to measure fundamental thermodynamic properties of actinide elements

    International Nuclear Information System (INIS)

    Smith, W.H.; Costa, D.A.

    1998-01-01

    This is the final report of a six-month, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory (LANL). The goal of this work was to establish a capability for the measurement of fundamental thermodynamic properties of actinide elements in room temperature molten salts. This capability will be used to study in detail the actinide chloro- and oxo- coordination chemistries that dominate in the chloride-based molten salt media. Uranium will be the first actinide element under investigation

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1982-03-01

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

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

    Science.gov (United States)

    Horwitz, E.P.; Dietz, M.L.

    1989-05-30

    A method and apparatus for the quantitative recover of actinide values from biological and environmental sample by passing appropriately prepared samples in a mineral acid solution through a separation column of a dialkyl(phenyl)-N,N-dialylcarbamoylmethylphosphine oxide dissolved in tri-n-butyl phosphate on an inert substrate which selectively extracts the actinide values. The actinide values can be eluted either as a group or individually and their presence quantitatively detected by alpha counting. 3 figs.

  17. Production and measurement of minor actinides in the commercial fuel cycle

    International Nuclear Information System (INIS)

    Stanbro, W.D.

    1997-03-01

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

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

    International Nuclear Information System (INIS)

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

    1982-03-01

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

  19. A literature review of actinide-carbonate mineral interactions

    International Nuclear Information System (INIS)

    Stout, D.L.

    1993-10-01

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

  20. A reexamination of the incentives for actinide burning

    International Nuclear Information System (INIS)

    Croff, A.G.; Forsberg, C.W.; Ludwig, S.B.

    1990-01-01

    Actinide burning (AB) is a concept that would greatly reduce the amounts of long-lived transuranic (TRU) nuclides in wastes going to the repository. The concept is implemented by intensified processing to reduce actinide losses to wastes and subsequent recycling of the actinides to liquid-metal reactors (LMRs). As a result, AB may simultaneously (a) simplify waste management by fissioning the TRU nuclides to shorter lived nuclides, (b) generate electricity, and (c) greatly extend uranium resources. In previous studies, researchers at the Oak Ridge National Laboratory compared the long-term repository risk reduction from AB to increases in cost and contemporary risk. They concluded that incentives for AB did not exist. Similar conclusions were reached by European investigators. During the decade since these studies, there have been two major developments related to the incentives for AB. The first is that the challenges inherent in characterizing, licensing, and funding a repository have become clearer and are larger than originally anticipated. The second development is the establishment of an Environmental Protection Agency (EPA) standard and US Nuclear Regulatory Commission (NRC) criteria to provide a specific measure of repository acceptability, as opposed to the many assumptions and calculations inherent in previous analyses. Consequently, the incentives for AB have been reexamined in the context of these developments and are discussed in this paper

  1. Actinide behavior in the Integral Fast Reactor. Final project report

    International Nuclear Information System (INIS)

    Courtney, J.C.

    1994-11-01

    The Integral Fast Reactor (IFR) under development by Argonne National Laboratory uses metallic fuels instead of ceramics. This allows electrorefining of spent fuels and presents opportunities for recycling minor actinide elements. Four minor actinides ( 237 Np, 240 Pu, 241 Am, and 243 Am) determine the waste storage requirements of spent fuel from all types of fission reactors. These nuclides behave the same as uranium and other plutonium isotopes in electrorefining, so they can be recycled back to the reactor without elaborate chemical processing. An experiment has been designed to demonstrate the effectiveness of the high-energy neutron spectra of the IFR in consuming these four nuclides and weapons grade plutonium. Eighteen sets of seven actinide and five light metal targets have been selected for seven day exposure in the Experimental Breeder Reactor-II which serves as a prototype of the IFR. Post-irradiation analyses of the exposed targets by gamma, alpha, and mass spectroscopy are used to determine nuclear reaction rates and neutron spectra. These experimental data increase the authors confidence in their ability to predict reaction rates in candidate IFR designs using a variety of neutron transport and diffusion programs

  2. Development of ion beam sputtering techniques for actinide target preparation

    Science.gov (United States)

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

    1985-06-01

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

  3. 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

    A series of static leach tests was conducted using glasses developed for vitrifying tank wastes at the Savannah River Site to monitor the disposition of actinide elements upon corrosion of the glasses. In these tests, glasses produced from SRL 131 and SRL 202 frits were corroded at 90 degrees C in a tuff groundwater. Tests were conducted using crushed glass at different glass surface area-to-solution volume (S/V) ratios to assess the effect of the S/V on the solution chemistry, the corrosion of the glass, and the disposition of actinide elements. Observations regarding the effects of the S/V on the solution chemistry and the corrosion of the glass matrix have been reported previously. This paper highlights the solution analyses performed to assess how the S/V used in a static leach test affects the disposition of actinide elements between fractions that are suspended or dissolved in the solution, and retained by the altered glass or other materials

  4. Rapid separation method for actinides in emergency air filter samples.

    Science.gov (United States)

    Maxwell, Sherrod L; Culligan, Brian K; Noyes, Gary W

    2010-12-01

    A new rapid method for the determination of actinides and strontium in air filter samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used in emergency response situations. The actinides and strontium in air filter method utilizes a rapid acid digestion method and a streamlined column separation process with stacked TEVA, TRU and Sr Resin cartridges. Vacuum box technology and rapid flow rates are used to reduce analytical time. Alpha emitters are prepared using cerium fluoride microprecipitation for counting by alpha spectrometry. The purified (90)Sr fractions are mounted directly on planchets and counted by gas flow proportional counting. The method showed high chemical recoveries and effective removal of interferences. This new procedure was applied to emergency air filter samples received in the NRIP Emergency Response exercise administered by the National Institute for Standards and Technology (NIST) in April, 2009. The actinide and (90)Sr in air filter results were reported in less than 4 h with excellent quality. Copyright 2010 Elsevier Ltd. All rights reserved.

  5. Advances in Metallic Fuels for High Burnup and Actinide Transmutation

    Energy Technology Data Exchange (ETDEWEB)

    Hayes, S. L.; Harp, J. M.; Chichester, H. J. M.; Fielding, R. S.; Mariani, R. D.; Carmack, W. J.

    2016-10-01

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

  6. 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

  7. Actinides and lanthanides under pressure: the pseudopotential approach; Actinides et terres rares sous pression: approche pseudopotentiel

    Energy Technology Data Exchange (ETDEWEB)

    Richard, N

    2002-07-01

    In the Density Functional Theory Framework, the pseudopotential formalism offers a broader scope of study than other theoretical methods such as global relaxation of the parameters of the cell or ab initio molecular dynamics simulations. This method has been widely used to study light elements or transition metals but never to study f elements. We have generated two non local norm conserving Trouillier-Martins pseudopotentials (one in LDA and one in GGA) for the cerium. To check the validity of the pseudopotentials, we have calculated the equilibrium volume and the incompressibility modulus and compared our results to previous all-electron calculations. If the GGA and non linear core corrections are used, the equation of state is in a good agreement with the experimental equation of state. A static study of the previously proposed high pressure phases give a transitions fcc-a''(I)-bct. Using the pseudopotentials we have generated, an ab initio molecular dynamics simulation at constant pressure, in the region between 5 and 12 GPa where the stable phase of cerium is not well defined, lead us to predict that a centred monoclinic structure, as the a''(I) phase previously observed in some experiments, is the most stable phase. We have also generated pseudopotentials for the light actinides (Th, Pa, U and Np). We have study their phase transitions under pressure at zero temperature. We compared our results with all electron results. The structure parameters have always been relaxed in this study. And for the first time in pseudopotential calculation, the spin-orbit coupling has been taken into account. The curves describing the variation of the volume or the incompressibility modulus depending on the elements and the phase transitions are always in agreement with the one found in the all electron calculations. (author)

  8. Separation of actinides using capillary extraction chromatography-inductively coupled plasma mass spectrometry.

    Science.gov (United States)

    Peterson, Dominic S; Montoya, Velma M

    2009-08-01

    Trace levels of actinides have been separated on capillary extraction chromatography columns. Detection of the actinides was achieved using an inductively coupled plasma mass spectrometer, which was coupled with the extraction chromatography system. In this study, we compare 30-cm long, 4.6 mm i.d. columns to capillary columns (750 microm i.d.) with lengths from 30 cm up to 150 cm. The columns that were tested were packed with TRU resin. We were able to separate a mixture of five actinides ((232)Th, (238)U, (237)Np, (239)Pu, and (241)Am). This work has application to rapid bioassay as well as automated separations of actinide materials.

  9. Performance considerations of nuclear reactor actinide recycle as a waste management alternative

    International Nuclear Information System (INIS)

    Murphy, D.J. Jr.

    1978-01-01

    Transplutonium actinide disposal by fission reactor recycle is examined. The neutronic parameters are evaluated for several average reactor neutron flux energies in the range 325 to 1071 keV. Simplified one-dimensional analytical models of CRBR and EBR-2 in conjunction with the computer codes ANISN and DEER are used for the computations. Results indicate that if the average neutron flux energy is large enough (above approx. 580 keV), then the transplutonium waste actinides behave more as fuels than as wastes. Using the same volumetric power density and radial geometry as EBR-2, a ''generic actinide burner reactor'' model, fueled solely with transplutonium actinides, is studied. Results show that the actinides are neutronically reactive enough to support a critical chain reaction. The long-term burnup performance indicates that equilibrium is established faster as average flux spectrum energy increases. Increasing the power density increases the time required to establish equilibrium. The specific reactivity (fuel value) and the long-term burnup performance of several actinide--lanthanide mixtures are evaluated. It is shown that although the lanthanides degrade the fuel value of the mixture, the time required to establish equilibrium actinide concentration is essentially unchanged. Ananalysis of the sensitivity of the results to uncertainties in the actinide nuclear cross section data show that the long-term actinide burnup performance is only slightly affected by relatively large uncertainties in the nuclear area

  10. The role of transferrin in actinide(IV) uptake: comparison with iron(III).

    Science.gov (United States)

    Jeanson, Aurélie; Ferrand, M; Funke, Harald; Hennig, Christoph; Moisy, Philippe; Solari, Pier Lorenzo; Vidaud, Claude; Den Auwer, Christophe

    2010-01-25

    The impact of actinides on living organisms has been the subject of numerous studies since the 1950s. From a general point of view, these studies show that actinides are chemical poisons as well as radiological hazards. Actinides in plasma are assumed to be mainly complexed to transferrin, the iron carrier protein. This paper casts light on the uptake of actinides(IV) (thorium, neptunium, plutonium) by transferrin, focusing on the pH dependence of the interaction and on a molecular description of the cation binding site in the protein. Their behavior is compared with that of iron(III), the endogenous transferrin cation, from a structural point of view. Complementary spectroscopic techniques (UV/Vis spectrophotometry, microfiltration coupled with gamma spectrometry, and X-ray absorption fine structure) have been combined in order to propose a structural model for the actinide-binding site in transferrin. Comparison of our results with data available on holotransferrin suggests some similarities between the behavior of Fe(III) and Np(IV)/Pu(IV)/ Np(IV) is not complexed at pH actinide edge have allowed a structural model of the actinide binding site to be elaborated: at least one tyrosine residue could participate in the actinide coordination sphere (two for iron), forming a mixed hydroxo-transferrin complex in which actinides are bound with transferrin both through An-tyrosine and through An--OH bonds. A description of interatomic distances is provided.

  11. EUROPART: an European integrated project on actinide partitioning

    International Nuclear Information System (INIS)

    Madic, C.; Baron, P.; Hudson, M.J.

    2006-01-01

    Full text of publication follows: The EUROPART project is a scientific integrated project between 24 European partners, from 10 countries, mostly funded by the European Community within the FP6, together with CRIEPI from Japan and ANSTO from Australia. 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 the treatment 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 European FP5 programs named PARTNEW, CALIXPART and PYROREP, respectively. The two main axes of research within EUROPART are: 1/ the partitioning of MA (from Am to Cf) from wastes issuing from the reprocessing of high burn-up UOX fuels and multi-recycled MOX fuels, 2/ the partitioning of the whole actinide family of elements for recycling, as an option for advanced dedicated fuel cycles (this work will be connected to the studies to be performed within the EUROTRANS European integrated project). In hydrometallurgy, the research is organized in five Work Packages (WP). Four are dedicated to the study of partitioning methods mainly based on the use of solvent extraction methods and of solid extractants, one WP is dedicated to the development of actinide co-conversion methods for fuel or target preparations. The research in pyrometallurgy is organized into four WPs, listed hereafter: (i) study of the basic chemistry of transuranium elements and of some fission products in molten salts (chlorides, fluorides), (ii) development of actinide partitioning methods, (iii) study of the conditioning of the salt wastes, (iv) system studies. Moreover, a strong management team is concerned not only with the technical and financial issues arising from EUROPART, but also with information, communication and benefits for Europe

  12. Chemical interaction of tetravalent actinides simulators and the engineering barrier

    International Nuclear Information System (INIS)

    Chain, Pablo; Alba, Maria D.; Castro, Miguel A.; Pavon, Esperanza; Mar Orta, M.

    2010-01-01

    Document available in extended abstract form only. The Deep Geological Repository (DGR) is the most internationally accepted option for the storage of high radioactive wastes. This confinement is based on the Multi-barrier Concept where the engineered barrier is a crucial safety wise. Nowadays, bentonite is accepted as the best argillaceous material in the engineered barrier of DGR. Additionally to its well-known physical role, a chemical interaction between lutetium, as actinide simulator, and the smectite has been demonstrated. The existence of a reaction mechanism, which was not previously described, based on the chemical interaction between the lanthanide cations and the orthosilicate anions of the lamellar structure has been identified. This finding has aroused the interest of the scientific community because lanthanides are used as simulators of high activity radionuclide (HAR) in agreement with the guidelines established in the bibliography. It has been observed that in conditions of moderate temperature and pressure a chemical interaction exists between smectites and rare earth elements (RE) and phases of insoluble di-silicate, RE 2 Si 2 O 7 , which would immobilize RE, are generated. It is remarkable that the reaction extends to all the set of the smectites, although they do not display the same reactivity, the saponite being the most reactive. The main isotopes present in the HLW belong to the actinide elements Np, Pu, Am and Cm, in addition to uranium generated by neutron capture during the fuel combustion process. The study of the mobilization of actinide (IV) thorough the bentonite barrier is limited because of their radioactivity. However, U(IV), Np(IV), Pu(IV) and Th(IV) can be simulated by the stable isotopes of the Zr(IV) and Hf(IV), because they exhibit ionic radius and physicochemical properties very similar to those of the actinide elements. It is the main objective of this research to investigate the chemical interaction of Zr(IV) as actinide

  13. ACTINET-I3 Summer School on Analytical Innovation in the field of actinide recycling - Slides of the presentations

    International Nuclear Information System (INIS)

    Poinssot, Ch.; Nash, K.L.; Puget, P.; Szabo, Z.; Vallet, V.; Berthon, L.; Duhamet, J.; Wipff, G.; Dufreche, J.F.; Walter, P.; Thiebaut, D.; Toulhoat, P.; Aupiais, J.; Amatore, C.

    2011-01-01

    This conference dealt with 3 main topics: analytical innovation in separation processes (hyphenated techniques, analytical chips,...), actinide recycling (extraction, interfaces, processes,...) and chemistry and thermodynamics of actinides. This document is composed of the slides of the presentations

  14. Plutonium and Minor Actinide Management in Thermal High-Temperature Gas-Cooled Reactors. Publishable Final Activity Report

    Energy Technology Data Exchange (ETDEWEB)

    Kuijper, J.C., E-mail: kuijper@nrg.eu [Nuclear Research and Consultancy Group (NRG), Petten (Netherlands); Somers, J.; Van Den Durpel, L.; Chauvet, V.; Cerullo, N.; Cetnar, J.; Abram, T.; Bakker, K.; Bomboni, E.; Bernnat, W.; Domanska, J.G.; Girardi, E.; De Haas, J.B.M.; Hesketh, K.; Hiernaut, J.P.; Hossain, K.; Jonnet, J.; Kim, Y.; Kloosterman, J.L.; Kopec, M.; Murgatroyd, J.; Millington, D.; Lecarpentier, D.; Lomonaco, G.; McEachern, D.; Meier, A.; Mignanelli, M.; Nabielek, H.; Oppe, J.; Petrov, B.Y.; Pohl, C.; Ruetten, H.J.; Schihab, S.; Toury, G.; Trakas, C.; Venneri, F.; Verfondern, K.; Werner, H.; Wiss, T.; Zakova, J.

    2010-11-15

    designs and their ability to accept a variety of Pu- and Pu/MA-based fuels (possibly in combination with thorium), and to obtain a significant reduction of the Pu- respectively Pu/MA content, while maintaining, to a large extent, the well-known standard (U-fuelled) HTR safety characteristics. However, this will require some changes in the reactor design. Studies have furthermore shown that fuel with a 'diluted' kernel ('inert-matrix') improves the transmutation performance of the reactor. A study on proliferation resistance, taking into account several possible proliferation pathways, highlights that a prismatic (V)HTR core would be amenable to conventional safeguards accounting and verification procedures, with fuel blocks accounted for individually in the same way as LWR fuel assemblies. However, a modified approach would be needed in pebble bed cores because of the impracticability of accounting for individual fuel spheres. When dealing with minor actinide bearing fuel helium generation is an important issue. Experiments have shown that He will be released from the kernel, but not from fresh kernels. Indeed, fresh fuel has shown a remarkable stability up to 2500 degrees C. For modelling purposes, 100% release of helium from the kernel is justified. The diluted kernel concept was first invoked by Belgonucleaire brings many benefits. The fuel modelling studies have clearly indicated the advantages that can be gained by dilution. Essentially, for a given buffer layer thickness, more volume is available to accommodate the CO and He released. Chemical thermodynamic models have been deployed to design a kernel that will show limited CO production. The most important point here is that substoichiometric Pu or Am oxides are essential. Further improvement can be achieved by chemical buffering of the fuel by the addition of Ce sesquioxide, which takes up oxygen to form the dioxide. Ultimately any coated particle design must be validated in an irradiation test

  15. Plutonium and Minor Actinide Management in Thermal High-Temperature Gas-Cooled Reactors. Publishable Final Activity Report

    International Nuclear Information System (INIS)

    Kuijper, J.C.; Somers, J.; Van Den Durpel, L.; Chauvet, V.; Cerullo, N.; Cetnar, J.; Abram, T.; Bakker, K.; Bomboni, E.; Bernnat, W.; Domanska, J.G.; Girardi, E.; De Haas, J.B.M.; Hesketh, K.; Hiernaut, J.P.; Hossain, K.; Jonnet, J.; Kim, Y.; Kloosterman, J.L.; Kopec, M.; Murgatroyd, J.; Millington, D.; Lecarpentier, D.; Lomonaco, G.; McEachern, D.; Meier, A.; Mignanelli, M.; Nabielek, H.; Oppe, J.; Petrov, B.Y.; Pohl, C.; Ruetten, H.J.; Schihab, S.; Toury, G.; Trakas, C.; Venneri, F.; Verfondern, K.; Werner, H.; Wiss, T.; Zakova, J.

    2010-11-01

    variety of Pu- and Pu/MA-based fuels (possibly in combination with thorium), and to obtain a significant reduction of the Pu- respectively Pu/MA content, while maintaining, to a large extent, the well-known standard (U-fuelled) HTR safety characteristics. However, this will require some changes in the reactor design. Studies have furthermore shown that fuel with a 'diluted' kernel ('inert-matrix') improves the transmutation performance of the reactor. A study on proliferation resistance, taking into account several possible proliferation pathways, highlights that a prismatic (V)HTR core would be amenable to conventional safeguards accounting and verification procedures, with fuel blocks accounted for individually in the same way as LWR fuel assemblies. However, a modified approach would be needed in pebble bed cores because of the impracticability of accounting for individual fuel spheres. When dealing with minor actinide bearing fuel helium generation is an important issue. Experiments have shown that He will be released from the kernel, but not from fresh kernels. Indeed, fresh fuel has shown a remarkable stability up to 2500 degrees C. For modelling purposes, 100% release of helium from the kernel is justified. The diluted kernel concept was first invoked by Belgonucleaire brings many benefits. The fuel modelling studies have clearly indicated the advantages that can be gained by dilution. Essentially, for a given buffer layer thickness, more volume is available to accommodate the CO and He released. Chemical thermodynamic models have been deployed to design a kernel that will show limited CO production. The most important point here is that substoichiometric Pu or Am oxides are essential. Further improvement can be achieved by chemical buffering of the fuel by the addition of Ce sesquioxide, which takes up oxygen to form the dioxide. Ultimately any coated particle design must be validated in an irradiation test. Though not possible to perform an irradiation programme

  16. Plutonium and Minor Actinide Management in Thermal High-Temperature Gas-Cooled Reactors. Publishable Final Activity Report

    International Nuclear Information System (INIS)

    Kuijper, J.C.; Somers, J.; Van Den Durpel, L.

    2013-01-01

    of Pu- and Pu/MA-based fuels (possibly in combination with thorium), and to obtain a significant reduction of the Pu- respectively Pu/MA content, while maintaining, to a large extent, the well-known standard (U-fuelled) HTR safety characteristics. However, this will require some changes in the reactor design. Studies have furthermore shown that fuel with a 'diluted' kernel ('inert-matrix') improves the transmutation performance of the reactor. A study on proliferation resistance, taking into account several possible proliferation pathways, highlights that a prismatic (V)HTR core would be amenable to conventional safeguards accounting and verification procedures, with fuel blocks accounted for individually in the same way as LW fuel assemblies. However, a modified approach would be needed in pebble bed cores because of the impracticability of accounting for individual fuel spheres. When dealing with minor actinide bearing fuel helium generation is an important issue. Experiments have shown that He will be released from the kernel, but not from fresh kernels. Indeed, fresh fuel has shown a remarkable stability – up to 2500 °C. For modelling purposes, 100% release of helium from the kernel is justified. The diluted kernel concept was first invoked by Belgonucleaire brings many benefits. The fuel modelling studies have clearly indicated the advantages that can be gained by dilution. Essentially, for a given buffer layer thickness, more volume is available to accommodate the CO and He released. Chemical thermodynamic models have been deployed to design a kernel that will show limited CO production. The most important point here is that substoichiometric Pu or Am oxides are essential. Further improvement can be achieved by chemical buffering of the fuel by the addition of Ce sesquioxide, which takes up oxygen to form the dioxide. Ultimately any coated particle design must be validated in an irradiation test. Though not possible to perform an irradiation programme in the

  17. Avalanches in vanadium sesquioxide nanodevices

    Science.gov (United States)

    Wang, Siming; Ramírez, Juan Gabriel; Schuller, Ivan K.

    2015-08-01

    The resistance versus temperature across the metal-insulator transition (MIT) of V2O3 nanodevices exhibits multiple discontinuous jumps. The jump sizes range over three orders of magnitude in resistance and their distribution follows a power law, implying that the MIT of V2O3 occurs through avalanches. While the maximum jump size depends on the device size, the power law exponent for V2O3 is independent of device geometry and different than the one found earlier in V O2 . A two-dimensional random percolation model exhibits a power law distribution different from the one found in V2O3 . Instead, the model gives a similar exponent found in another vanadium oxide, V O2 . Our results suggest that the MITs of V O2 and V2O3 are produced by different mechanisms.

  18. Troubles in the systematic prediction of transition metal thermochemistry with contemporary out-of-the-box methods

    KAUST Repository

    Minenkov, Yury

    2016-03-22

    The recently developed DLPNO-CCSD(T) method and 7 popular DFT functionals (B3LYP, M06, M06L, PBE, PBE0, TPSS and TPSSh) with and without an empirical dispersion term have been tested to reproduce 111 gas phase reaction enthalpies involving 11 different transition metals. Our calculations, corrected for both relativistic effects and basis set incompleteness, indicate that most of the methods applied with default settings perform with acceptable accuracy on average. Nevertheless, our calculations also evidenced unexpected and non systematic large deviations for specific cases. For group 12 metals (Zn, Cd, Hg) most of the methods provided mean unsigned errors (MUE) less than 5.0 kcal/mol, with DLPNO-CCSD(T) and PBE methods performing excellently (MUE lower 2.0 kcal/mol). Problems started with group 4 metals (Ti and Zr). Best performer for Zr complexes with a MUE of 1.8 kcal/mol, PBE0-D3, provides a MUE larger than 8 kcal/mol for Ti. DLPNO-CCSD(T) provides a reasonable MUE of 3.3 kcal/mol for Ti reactions, but gives MUE a larger than 14.4 kcal/mol for Zr complexes, with all the larger deviations for reactions involving ZrF4. Large and non-systematic errors have been obtained for group 6 metals (Mo and W), for 8 reactions containing Fe, Cu, Nb and Re complexes. Finally, for the whole set of 111 reactions, the DLPNO-CCSD(T), B3LYP-D3 and PBE0-D3 methods turned out to be the best performers, both providing MUE below 5.0 kcal/mol. Since DFT results cannot be systematically improved and large non-systematic deviations of 20-30 kcal/mol were obtained even for best performers, our results indicates that current DFT methods are still unable to provide robust predictions in transition metal thermochemistry, at least for the functionals explored in this work. The same conclusion holds for both DLPNO-CCSD(T) and canonical CCSD(T) methods when used entirely as out-of-the-box. However if careful investigation core correlation is performed, relativistic effects are properly included

  19. Photochemistry in terrestrial exoplanet atmospheres. III. Photochemistry and thermochemistry in thick atmospheres on super Earths and mini Neptunes

    Energy Technology Data Exchange (ETDEWEB)

    Hu, Renyu; Seager, Sara, E-mail: hury@caltech.edu [Department of Earth, Atmospheric and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA 02139 (United States)

    2014-03-20

    Some super Earths and mini Neptunes will likely have thick atmospheres that are not H{sub 2}-dominated. We have developed a photochemistry-thermochemistry kinetic-transport model for exploring the compositions of thick atmospheres on super Earths and mini Neptunes, applicable for both H{sub 2}-dominated atmospheres and non-H{sub 2}-dominated atmospheres. Using this model to study thick atmospheres for wide ranges of temperatures and elemental abundances, we classify them into hydrogen-rich atmospheres, water-rich atmospheres, oxygen-rich atmospheres, and hydrocarbon-rich atmospheres. We find that carbon has to be in the form of CO{sub 2} rather than CH{sub 4} or CO in a H{sub 2}-depleted water-dominated thick atmosphere and that the preferred loss of light elements from an oxygen-poor carbon-rich atmosphere leads to the formation of unsaturated hydrocarbons (C{sub 2}H{sub 2} and C{sub 2}H{sub 4}). We apply our self-consistent atmosphere models to compute spectra and diagnostic features for known transiting low-mass exoplanets GJ 1214 b, HD 97658 b, and 55 Cnc e. For GJ 1214 b, we find that (1) C{sub 2}H{sub 2} features at 1.0 and 1.5 μm in transmission and C{sub 2}H{sub 2} and C{sub 2}H{sub 4} features at 9-14 μm in thermal emission are diagnostic for hydrocarbon-rich atmospheres; (2) a detection of water-vapor features and a confirmation of the nonexistence of methane features would provide sufficient evidence for a water-dominated atmosphere. In general, our simulations show that chemical stability has to be taken into account when interpreting the spectrum of a super Earth/mini Neptune. Water-dominated atmospheres only exist for carbon to oxygen ratios much lower than the solar ratio, suggesting that this kind of atmospheres could be rare.

  20. J-ACTINET activities of training and education for actinide science research

    International Nuclear Information System (INIS)

    Miato, Kazuo; Konashi, Kenji; Yamana, Hajimu; Yamanaka, Shinsuke; Nagasaki, Shinya; Ikeda, Yasuhisa; Sato, Seichi; Arita, Yuji; Idemitsu, Kazuya; Koyama, Tadafumi

    2011-01-01

    Actinide science research is indispensable to maintain sustainable development of innovative nuclear technology, especially advanced fuels, partitioning/reprocessing, and waste management. For actinide science research, special facilities with containment and radiation shields are needed to handle actinide materials since actinide elements are γ-, α- and neutron-emitters. The number of facilities for actinide science research has been decreased, especially in universities, due to the high maintenance cost. J-ACTINET was established in 2008 to promote and facilitate actinide science research in close cooperation with the facilities and to foster many of young scientists and engineers to be actively engaged in the fields of actinide science. The research program was carried out, through which young researchers were expected to learn how to make experiments with advanced experimental tools and to broaden their horizons. The summer schools and computational science school were held to provide students, graduate students, and young researchers with the opportunities to come into contact with actinide science research. In these schools, not only the lectures, but also the practical exercises were made as essential part. The overseas dispatch program was also carried out, where graduate students and young researchers were sent to the international summer schools and conferences. (author)

  1. 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.)

  2. Invisible structures in the X-ray absorption spectra of actinides

    NARCIS (Netherlands)

    Kvashnina, Kristina O.; De Groot, Frank M F

    The X-ray absorption spectra of actinides are discussed with an emphasis on the fundamental effects that influence their spectral shape, including atomic multiplet theory, charge transfer theory and crystal field theory. Many actinide spectra consist of a single peak and it is shown that the use of

  3. First-principles phase stability, bonding, and electronic structure of actinide metals

    International Nuclear Information System (INIS)

    Söderlind, Per

    2014-01-01

    The actinide elemental metals are scare, often toxic and radio active, causing challenges for both experiments and theory while offering fascinating physics. For practical purposes they are the prevalent building blocks for materials where nuclear properties are of interest. Here, however, we are focusing on fundamental properties of the actinides related to their electronic structure and characteristic bonding in the condensed state. The series of actinides is naturally divided into two segments. First, the set of lighter actinides thorium through plutonium, often referred to as the early actinides, displays a variation of the atomic volume reminiscent of what is seen in transition metals, suggesting a gradual occupation of bonding 5f states. Second, the heavier (late) actinides, Am and onwards, demonstrate volume behaviors comparable to the rare-earth metals that implies nonbonding 5f states. Arguably, one can distinguish plutonium metal as special case lying between these two subsets because it shares some features from both. Therefore, we discuss the early actinides, plutonium metal, and the late actinides separately applying first-principles density-functional-theory (DFT) calculations. The analysis includes successes and failures of the theory to describe primarily phase stability, bonding, and electronic structure

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

    International Nuclear Information System (INIS)

    Sandenaw, T.A.

    1978-01-01

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

  5. Biological pathways and chemical behavior of plutonium and other actinides in the environment

    International Nuclear Information System (INIS)

    Dahlman, R.C.; Bondietti, E.A.; Eyman, L.D.

    1976-01-01

    The principal long-lived actinide elements that may enter the environment from either U or Pu fuel cycles are Pu, Am, Cm, and Np. Approximately 25% of the alpha activity estimated to be released to the atmosphere from the LMFBR fuel cycle will be contributed by 241 Am, 242 Cm, and 244 Cm. The balance of the alpha activity will come from Pu isotopes. Activities of 242 Cm, 244 Cm, 241 Am, 243 Am, and 237 Np in waste may exceed concentrations of Pu isotopes in waste after various periods of decay. Thorium and uranium isotopes may also be released by operations of the thorium fuel cycle. Environmental actinides are discussed under the following headings: sources of man-made actinide elements; pathways of exposure; environmental chemistry of actinides; uptake of actinides by plants; distribution of actinides in components of White Oak Lake; entry of actinides into terrestrial food chains; relationship between chemical behavior and uptake of actinides by organisms; and behavior of Pu in freshwater and marine food chains

  6. Polymer Inclusion Membrane Containing a Tripodal Diglycolamide Ligand: Actinide Ion Uptake and Transport Studies

    NARCIS (Netherlands)

    Mahanty, B.; Mohapatra, P.K.; Raut, D.R.; Das, D.K.; Behere, P.G.; Afzal, M.; Verboom, Willem

    2016-01-01

    A cellulose triacetate (CTA)-based polymer inclusion membrane (PIM) containing a C-pivot tripodal diglycolamide (T-DGA) as the carrier extractant and 2-nitrophenyl octyl ether (NPOE) as the plasticizer shows potential for the uptake of actinides from acidic feed solutions. The uptake of actinides

  7. 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

  8. Actinide Partitioning and Transmutation Program. Progress report, April 1--June 30, 1977

    Energy Technology Data Exchange (ETDEWEB)

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

    1977-10-01

    Experimental work on the 16 tasks comprising the Actinide Partitioning and Transmutation Program was continued. Summaries of work are given on Purex Process modifications, actinide recovery, Am-Cm recovery, radiation effects on ion exchangers, LMFBR transmutation studies, thermal reactor transmutation studies, fuel cycle studies, and partitioning-transmutation evaluation. (JRD)

  9. Alpha decay and cluster decay of some neutron-rich actinide nuclei

    Indian Academy of Sciences (India)

    2017-02-09

    Feb 9, 2017 ... Abstract. Nuclei in the actinide region are good in exhibiting cluster radioactivity. In the present work, the half-lives of α-decay and heavy cluster emission from certain actinide nuclei have been calculated using cubic plus Yukawa plus exponential model (CYEM). Our model has a cubic potential for the ...

  10. Actinides in Hanford Tank Waste Simulants: Chemistry of Selected Species in Oxidizing Alkaline Solutions

    International Nuclear Information System (INIS)

    Nash, Kenneth L.; Laszak, Ivan; Borkowski, Marian; Hancock, Melissa; Rao, Linfeng; Reed, Wendy

    2004-01-01

    To enhance removal of selected troublesome nonradioactive matrix elements (P, Cr, Al, S) from the sludges in radioactive waste tanks at the Hanford site, various chemical washing procedures have been evaluated. It is intended that leaching should leave the actinides in the residual sludge phase for direct vitrification. Oxidative treatment with strongly alkaline solutions has emerged as the best approach to accomplishing this feat. However, because the most important actinide ions in the sludge can exist in multiple oxidation states, it is conceivable that changes in actinide oxidation state speciation could interfere with hopes and plans for actinide insolubility. In this presentation, we discuss both the impact of oxidative alkaline leachants on actinide oxidation state speciation and the chemistry of oxidized actinide species in the solution phase. Actinide oxidation does occur during leaching, but the solubility behavior is complex. Mixed ligand complexes may dominate solution phase speciation of actinides under some circumstances. This work was supported by the U.S. Department of Energy, Offices of Science and Waste Management, Environmental Management Science Program under Contract DEAC03- 76SF0098 at Lawrence Berkeley National Laboratory and Contract W-31-109- ENG-38 at Argonne National Laboratory

  11. Solubilities of Actinide Oxides in the KURT Groundwater

    International Nuclear Information System (INIS)

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

    2009-12-01

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

  12. Neutronics design study on a minor actinide burner for transmuting spent fuel

    International Nuclear Information System (INIS)

    Choi, Hang Bok

    1998-08-01

    A liquid metal reactor was designed for the primary purpose of burning the minor actinide waste from commercial light water reactors. The design was constrained to maintain acceptable safety performance as measured by the burnup reactivity swing, the doppler coefficient, and the sodium void worth. Sensitivity studies were performed for homogeneous and decoupled core designs, and a minor actinide burner design was determined to maximize actinide consumption and satisfy safety constraints. One of the principal innovations was the use of two core regions, with a fissile plutonium outer core and an inner core consisting only of minor actinides. The physics studies performed here indicate that a 1200 MWth core is able to transmute the annual minor actinide inventory of about 16 LWRs and still exhibit reasonable safety characteristics. (author). 34 refs., 22 tabs., 14 figs

  13. Incineration of actinide targets in a pressurized water reactor spin project

    International Nuclear Information System (INIS)

    Puill, A.; Bergeron, J.

    1993-01-01

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

  14. Optimization of extraction chromatography separations of trace levels of actinides with ICP-MS detection.

    Science.gov (United States)

    Peterson, Dominic S; Plionis, Alexander A; Gonzales, Edward R

    2007-07-01

    The separation of trace level actinides has been evaluated on extraction chromatography columns. Detection of the actinides was achieved through the use of an inductively coupled plasma MS (ICP-MS). The columns that we tested were prepared from a commercial TRU resin. The separation of the actinides was optimized for several parameters including particle size, column length, packing pressure, and eluent flow rate. We also examined the possibility of reducing or eliminating oxalic acid in the eluents in order to improve the performance of the mass spectrometer. We were able to separate a mixture of five actinides ((232)Th,( 238)U,( 237)Np, (239)Pu,( 243)Am) in less than 4 min. This work has application to rapid bioassay as well as for automated separations of actinide materials.

  15. The selective extraction of oxidized minor actinides: a possible route for the Actinex program

    International Nuclear Information System (INIS)

    Adnet, J.M.; Brossard, P.; Bourges, J.

    1993-01-01

    In the SPIN programme, defined by CEA to improve the management of high level nuclear waste, a part called ACTINEX is specially devoted to the extraction of long-lived alpha emitters and fission products from high level liquid waste issuing from the PUREX process. Concerning the actinides elements, as U and Pu are already recovered, the main objective to reach is now the quantitative extraction of Np and Am. The transmutation of these recovered actinides into short-lived radionuclides is then forecast. This paper deals with the possibilities to define a minor actinides partitioning process based on the selective extraction of actinides oxidized to their oxidation states higher than three. It essentially focuses on americium chemistry. Finally, two general separation scheme for minor actinide partitioning are proposed and discussed. (authors). 5 figs., 13 refs

  16. Studies on the properties of hard-spectrum, actinide fissioning reactors. Final report

    International Nuclear Information System (INIS)

    Nelson, J.B.; Prichard, A.W.; Schofield, P.E.; Robinson, A.H.; Spinrad, B.I.

    1980-01-01

    It is technically feasible to construct an operable (e.g., safe and stable) reactor to burn waste actinides rapidly. The heart of the concept is a driver core of EBR-II type, with a central radial target zone in which fuel elements, made entirely of waste actinides are exposed. This target fuel undergoes fission, as a result of which actinides are rapidly destroyed. Although the same result could be achieved in more conventionally designed LWR or LMFBR systems, the fast spectrum reactor does a much more efficient job, by virtue of the fact that in both LWR and LMFBR reactors, actinide fission is preceded by several captures before a fissile nuclide is formed. In the fast spectrum reactor that is called ABR (actinide burning reactor), these neutron captures are short-circuited

  17. New conceptual process for the extraction of actinides based on oxapentane-diamides

    International Nuclear Information System (INIS)

    Jing Chen; Shuwei Wang

    2007-01-01

    Several diamide derivates were synthesized in our laboratory. The extraction of actinides and some fission products by these compounds were studied. N,N,N',N'-tetra-(2-ethylhexyl)-3-oxa pentanediamide (TEHOPDA) was proven to be a suitable extractant for the removal of actinides from nitric acid solution. The actinides can be stripped from the loaded solvent by the dilute nitric acid. TEHOPDA showed a high loading capacity to actinides and lanthanides with a mixture of n-octanol and kerosene as the diluent. Considering the effective-extraction and easy-stripping of actinides, 0.25 mol/l TEHOPDA - 30% n-octanol + 70% kerosene was selected as the solvent. A cascade extraction experiment was carried out with the simulated dissolver solution of spend fuel as feed. 99.99% U and 99.999% Am, Pu, and Np were extracted in a 4-stage test. Based on the experimental results, a conceptual reprocessing process was proposed. (author)

  18. Phase Behavior and Equations of State of the Actinide Oxides

    Science.gov (United States)

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

    2017-12-01

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

  19. Solid-state actinide acid phosphites from phosphorous acid melts

    International Nuclear Information System (INIS)

    Oh, George N.; Burns, Peter C.

    2014-01-01

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

  20. Comparison of fission and capture cross sections of minor actinides

    International Nuclear Information System (INIS)

    Nakagawa, Tsuneo; Iwamoto, Osamu

    2003-01-01

    The fission and capture cross sections of minor actinides given in JENDL-3.3 are compared with other evaluated data and experimental data. The comparison was made for 32 nuclides of Th-227, 228, 229, 230, 233, 234, Pa-231, 232, 233, U-232, 234, 236, 237, Np-236, 237, 238, Pu-236, 237, 238, 242, 244, Am-241, 242, 242m, 243, Cm-242, 243, 244, 245, 246, 247 and 248. Given in the present report are figures of these cross sections and tables of cross sections at 0.0253 eV and resonance integrals. (author)

  1. Manifestation of cluster effects in the structure of actinides

    Science.gov (United States)

    Shneidman, T. M.; Adamian, G. G.; Antonenko, N. V.; Jolos, R. V.; Zhou, Shan-Gui

    2016-01-01

    We developed a cluster model which allows to take into account both shape deformation parameters and cluster degrees of freedom. The model is based on the assumption that the wave function of nucleus can be treated as a superposition of a mononucleus and two-cluster configurations. The model is applied to describe the multiple negative-parity bands in deformed actinides. Special emphasis is made on the investigation of the recently measured positive parity 0+2 rotational band of reflection-asymmetric nature in 240Pu. The results suggest that this band might be understood as the one built on the lowest excited state in mass asymmetry degree of freedom.

  2. Manifestation of cluster effects in the structure of actinides

    OpenAIRE

    Shneidman T.M.; Adamian G.G.; Antonenko N.V.; Jolos R.V.; Zhou Shan-Gui

    2016-01-01

    We developed a cluster model which allows to take into account both shape deformation parameters and cluster degrees of freedom. The model is based on the assumption that the wave function of nucleus can be treated as a superposition of a mononucleus and two-cluster configurations. The model is applied to describe the multiple negative-parity bands in deformed actinides. Special emphasis is made on the investigation of the recently measured positive parity 0+2 rotational band of reflection-as...

  3. Status of the lanthanides and actinides in the periodic table

    International Nuclear Information System (INIS)

    Holden, N.E.

    1985-01-01

    In extended discussions and correspondence with Ekkehard Fluck, the author was made aware of a problem with the Periodic Table, i.e., which element should be shown in the main table as the representative of the lanthanide series and the actinide series. In earlier discussion, he came to the conclusion that lanthanum and actinium are not the elements which should appear, but rather lutetium and lawrencium are more appropriate for inclusion in their place. This paper will attempt to justify the reasons for the above conclusions. 4 refs

  4. Advances in fuel materials for the transmutation of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Prunier, C.

    1994-12-31

    The physical feasibility of actinides, spent fuels and fission products burning in fission reactors is well understood. In fast reactors, this operation is more favourable. The homogeneous recycling mode has had a preliminary validation in Phenix (the Super fact experiment). For the heterogenous recycling mode, past experience for {sup 238} Pu production in thermal spectrum was obtained with Np O{sub 2}-Mg O targets. An irradiation experiment in Phenix blanket is foreseen with the same type of target. The {sup 237} Np problem seems to be most conveniently treated, even in the short term, by homogeneous recycling with Pu in fast reactors. (author). 15 figs., 4 tabs.

  5. Calculated investigation of actinide transmutation in the BOR-60 reactor

    International Nuclear Information System (INIS)

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

    2001-01-01

    In the course of reactor operation the formation of fission products and accumulation of minor-actinides and plutonium take place in the nuclear fuel. These materials define the radiation hazard to a great extent. Of one possible ways lowering the activity of irradiated nuclear fuel is transmutation of long-lived radioactive isotopes in the stable or short-lived ones, that allows to facilitate the problem of the high-level waste and to improve the efficiency of nuclear fuel use at the expense of its recycling and burnup increasing. (authors)

  6. Actinide neutron-induced fission cross section measurements at LANSCE

    Energy Technology Data Exchange (ETDEWEB)

    Tovesson, Fredrik K [Los Alamos National Laboratory; Laptev, Alexander B [Los Alamos National Laboratory; Hill, Tony S [INL

    2010-01-01

    Fission cross sections of a range of actinides have been measured at the Los Alamos Neutron Science Center (LANSCE) in support of nuclear energy applications in a wide energy range from sub-thermal energies up to 200 MeV. A parallel-plate ionization chamber are used to measure fission cross sections ratios relative to the {sup 235}U standard while incident neutron energies are determined using the time-of-flight method. Recent measurements include the {sup 233,238}U, {sup 239-242}Pu and {sup 243}Am neutron-induced fission cross sections. Obtained data are presented in comparison with ex isting evaluations and previous data.

  7. Lanthanides and actinides extraction by calixarenes containing CMPO groups

    International Nuclear Information System (INIS)

    Garcia Carrera, A.

    2001-01-01

    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.)

  8. Detection of Actinides via Nuclear Isomer De-Excitation

    Energy Technology Data Exchange (ETDEWEB)

    Francy, Christopher J. [Oregon State Univ., Corvallis, OR (United States)

    2009-07-01

    This dissertation discusses a data collection experiment within the Actinide Isomer Identification project (AID). The AID project is the investigation of an active interrogation technique that utilizes nuclear isomer production, with the goal of assisting in the interdiction of illicit nuclear materials. In an attempt to find and characterize isomers belonging to 235U and its fission fragments, a 232Th target was bombarded with a monoenergetic 6Li ion beam, operating at 45 MeV.

  9. Hydrometallurgical minor actinide separation in hollow fiber modules

    International Nuclear Information System (INIS)

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

    2004-01-01

    Hollow fiber modules (HFM) were used as phase contacting devices for hydrometallurgical minor actinide separation in the Partitioning and Transmutation context. Two single-HFM setups, one using commercially available HFM, the other one using miniature HFM, have been developed and manufactured. Several very successful DIAMEX and SANEX once-through tests were performed. The major advantage of the new miniature HFM is their size drastically reducing chemicals consumption: only several 10 mL of feed phases are required for a test. (authors)

  10. 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

  11. Actinide chemistry and electronuclear cycle: contribution of synchrotron radiation; Chimie des actinides et cycle electronucleaire L'apport du rayonnement synchrotron

    Energy Technology Data Exchange (ETDEWEB)

    Den Auwer, Ch. [CEA Marcoule, Direction de l' Energie Nucleaire, Departement de Radiochimie et Chimie des Procedes, SCPS, F-30207 Bagnols-sur-Ceze (France)

    2011-07-01

    The topics related to actinide chemistry involved in the civil nuclear industry follow the electronuclear cycle: mining-enrichment, physical chemistry of the nuclear fuel, behavior in reactors, selective extraction for fuel reprocessing, storage, environmental impact, and human toxicology. In order to characterize the actinide properties, dedicated synchrotron beam lines are necessary, although scarce. This article focuses on synchrotron studies related to the elaboration of the nuclear fuel, its reprocessing, the storage in glass matrices and the bio-environmental impact. (author)

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

    International Nuclear Information System (INIS)

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

    2007-01-01

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

  13. Current and future studies of actinides materials at the advanced light source

    International Nuclear Information System (INIS)

    Shuh, D.K.

    2002-01-01

    The vacuum ultraviolet (VUV)/soft X-ray region of the synchrotron radiation (SR) spectrum has revolutionized the approach to surface materials chemistry/physics. This spectral region has long been recognised for its potential to afford investigations of fundamental actinide science and to provide an improved analytical surface characterisation capabilities for actinide materials. Previously, the actinide science community was unable to take advantage of the opportunities afforded by VUV/soft X-ray SR methodologies because of radiological safety concerns and the need to prepare pristine actinide materials compatible with experiments in ultra-high vacuum end stations. With the advent of third-generation light sources operating in the VUV/soft X-ray region, such as the Advanced Light Source (ALS) at LBNL, experiments with small amounts of actinide materials are possible. Actinide investigations at the ALS are based on a graded approach to radioactive materials safety and are conducted with the assistance of LBNL Environment, Health and Safety (EH and S) personnel during the experiments. LBNL EH and S personnel have many years of experience supporting experiments utilising radioactive materials at LBNL user-based accelerator facilities. The SR techniques and technologies used in this energy region have continued to mature, permitting more complicated investigations and enabling new spectroscopic approaches. Of particular importance for work with actinides is the development of the micro-spectroscopy and spectro-microscopy capabilities on several beamlines at the ALS. These capabilities allow the use of small amounts of actinide material. In addition, these techniques can provide information on the spatial distribution of actinide species that complements the spectral information. Early demonstrations of the ability to safely collect data from actinide micro-samples and the active support of the ALS for such experiments has led to the investigations of actinide

  14. Conservative axial burnup distributions for actinide-only burnup credit

    International Nuclear Information System (INIS)

    Kang, C.; Lancaster, D.

    1997-11-01

    Unlike the fresh fuel approach, which assumes the initial isotopic compositions for criticality analyses, any burnup credit methodology must address the proper treatment of axial burnup distributions. A straightforward way of treating a given axial burnup distribution is to segment the fuel assembly into multiple meshes and to model each burnup mesh with the corresponding isotopic compositions. Although this approach represents a significant increase in modeling efforts compared to the uniform average burnup approach, it can adequately determine the reactivity effect of the axial burnup distribution. A major consideration is what axial burnup distributions are appropriate for use in light of many possible distributions depending on core operating conditions and histories. This paper summarizes criticality analyses performed to determine conservative axial burnup distributions. The conservative axial burnup distributions presented in this paper are included in the Topical Report on Actinide-Only Burnup Credit for Pressurized Water Reactor Spent Nuclear Fuel Packages, Revision 1 submitted in May 1997 by the US Department of Energy (DOE) to the US Nuclear Regulatory Commission (NRC). When approved by NRC, the conservative axial burnup distributions may be used to model PWR spent nuclear fuel for the purpose of gaining actinide only burnup credit

  15. Actinide production from xenon bombardments of curium-248

    International Nuclear Information System (INIS)

    Welch, R.B.

    1985-01-01

    Production cross sections for many actinide nuclides formed in the reaction of 129 Xe and 132 Xe with 248 Cm at bombarding energies slightly above the coulomb barrier were determined using radiochemical techniques to isolate these products. These results are compared with cross sections from a 136 Xe + 248 Cm reaction at a similar energy. When compared to the reaction with 136 Xe, the maxima in the production cross section distributions from the more neutron deficient projectiles are shifted to smaller mass numbers, and the total cross section increases for the production of elements with atomic numbers greater than that of the target, and decreases for lighter elements. These results can be explained by use of a potential energy surface (PES) which illustrates the effect of the available energy on the transfer of nucleons and describes the evolution of the di-nuclear complex, an essential feature of deep-inelastic reactions (DIR), during the interaction. The other principal reaction mechanism is the quasi-elastic transfer (QE). Analysis of data from a similar set of reactions, 129 Xe, 132 Xe, and 136 Xe with 197 Au, aids in explaining the features of the Xe + Cm product distributions, which are additionally affected by the depletion of actinide product yields due to deexcitation by fission. The PES is shown to be a useful tool to predict the general features of product distributions from heavy ion reactions

  16. Actinides transmutation - a comparison of results for PWR benchmark

    International Nuclear Information System (INIS)

    Claro, Luiz H.

    2009-01-01

    The physical aspects involved in the Partitioning and Transmutation (P and T) of minor actinides (MA) and fission products (FP) generated by reactors PWR are of great interest in the nuclear industry. Besides these the reduction in the storage of radioactive wastes are related with the acceptability of the nuclear electric power. From the several concepts for partitioning and transmutation suggested in literature, one of them involves PWR reactors to burn the fuel containing plutonium and minor actinides reprocessed of UO 2 used in previous stages. In this work are presented the results of the calculations of a benchmark in P and T carried with WIMSD5B program using its new cross sections library generated from the ENDF-B-VII and the comparison with the results published in literature by other calculations. For comparison, was used the benchmark transmutation concept based in a typical PWR cell and the analyzed results were the k∞ and the atomic density of the isotopes Np-239, Pu-241, Pu-242 and Am-242m, as function of burnup considering discharge of 50 GWd/tHM. (author)

  17. Effects of actinide burning on waste disposal at Yucca Mountain

    International Nuclear Information System (INIS)

    Hirschfelder, J.

    1992-01-01

    Release rates of 15 radionuclides from waste packages expected to result from partitioning and transmutation of Light-Water Reactor (LWR) and Actinide-Burning Liquid-Metal Reactor (ALMR) spent fuel are calculated and compared to release rates from standard LWR spent fuel packages. The release rates are input to a model for radionuclide transport from the proposed geologic repository at Yucca Mountain to the water table. Discharge rates at the water table are calculated and used in a model for transport to the accessible environment, defined to be five kilometers from the repository edge. Concentrations and dose rates at the accessible environment from spent fuel and wastes from reprocessing, with partitioning and transmutation, are calculated. Partitioning and transmutation of LWR and ALMR spent fuel reduces the inventories of uranium, neptunium, plutonium, americium and curium in the high-level waste by factors of 40 to 500. However, because release rates of all of the actinides except curium are limited by solubility and are independent of package inventory, they are not reduced correspondingly. Only for curium is the repository release rate much lower for reprocessing wastes

  18. Supercritical fluid extraction and separation of uranium from other actinides.

    Science.gov (United States)

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

    2014-06-15

    The feasibility of separating U from nitric acid solutions of mixed actinides using tri-n-butylphosphate (TBP)-modified supercritical fluid carbon dioxide (sc-CO2) was investigated. The actinides U, Np, Pu, and Am were extracted into sc-CO2 modified with TBP from a range of nitric acid concentrations, in the absence of, or in the presence of, a number of traditional reducing and/or complexing agents to demonstrate the separation of these metals from U under sc-CO2 conditions. The separation of U from Pu using sc-CO2 was successful at nitric acid concentrations of less than 3M in the presence of acetohydroxamic acid (AHA) or oxalic acid (OA) to mitigate Pu extraction, and the separation of U from Np was successful at nitric acid concentrations of less than 1M in the presence of AHA, OA, or sodium nitrite to mitigate Np extraction. Americium was not well extracted under any condition studied. Copyright © 2014 Elsevier B.V. All rights reserved.

  19. The EBR-II X501 Minor Actinide Burning Experiment

    Energy Technology Data Exchange (ETDEWEB)

    W. J. Carmack; M. K. Meyer; S. L. Hayes; H. Tsai

    2008-01-01

    The X501 experiment was conducted in EBR II as part of the Integral Fast Reactor program to demonstrate minor actinide burning through the use of a homogeneous recycle scheme. The X501 subassembly contained two metallic fuel elements loaded with relatively small quantities of americium and neptunium. Interest in the behavior of minor actinides (MA) during fuel irradiation has prompted further examination of existing X501 data and generation of new data where needed in support of the U.S. waste transmutation effort. The X501 experiment is one of the few MA bearing fuel irradiation tests conducted worldwide, and knowledge can be gained by understanding the changes in fuel behavior due to addition of MAs. Of primary interest are the effect of the MAs on fuel cladding chemical interaction and the redistribution behavior of americium. The quantity of helium gas release from the fuel and any effects of helium on fuel performance are also of interest. It must be stressed that information presented at this time is based on the limited PIE conducted in 1995–1996 and, currently, represents a set of observations rather than a complete understanding of fuel behavior. This report provides a summary of the X501 fabrication, characterization, irradiation, and post irradiation examination.

  20. Physical chemistry and modelling of the sintering of actinide oxides

    International Nuclear Information System (INIS)

    Lechelle, Jacques

    2013-01-01

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

  1. Neutron diffraction and the physical properties of the light actinides

    International Nuclear Information System (INIS)

    Lawson, A.C.; Cort, B.; Roberts, J.A.; Bennett, B.I.; Richardson, J.W. Jr.

    1998-01-01

    For the past few years the authors have been applying the techniques of neutron powder diffraction to questions arising from the peculiar properties of the light actinide metals. The peculiar properties include complicated crystal structures, leading to complex phase diagrams; anomalous elastic and thermal expansion behavior; and surprisingly low melting points, especially for plutonium. The authors have made neutron diffraction studies of α-thorium, α-neptunium, α-uranium, and α- and δ-plutonium. A great deal has been learned from a study of the temperature dependence of the thermal vibrations of the light actinides. These can be determined using neutron diffraction to measure the Debye-Waller factors in powder diffraction experiments. The same neutron diffraction experiments also give information on the linear coefficient of thermal expansion α. This quantity is also strongly temperature dependent. Other neutron diffraction work is in progress, including attempts to solve some of the unknown alloy structures of Pu, and texture analysis via pole-figure measurements. The texture measurements are of particular interest, given the elastic anisotropy. High-quality data on Pu require the use of the nonabsorbing 242 Pu isotope, and this is a disadvantage. However, the high penetration of neutrons into most materials means that many safety problems can be solved by encapsulation of the radioactive material in V or other metal

  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. Advanced techniques in actinide spectroscopy (ATAS 2014). Abstract book

    International Nuclear Information System (INIS)

    Foerstendorf, Harald; Mueller, Katharina; Steudtner, Robin

    2014-01-01

    In 2012, The Institute of Resource Ecology at the Helmholtz-Zentrum Dresden Rossendorf organized the first international workshop of Advanced Techniques in Actinide Spectroscopy (ATAS). A very positive feedback and the wish for a continuation of the workshop were communicated from several participants to the scientific committee during the workshop and beyond. Today, the ATAS workshop has been obviously established as an international forum for the exchange of progress and new experiences on advanced spectroscopic techniques for international actinide and lanthanide research. In comparison to already established workshops and conferences on the field of radioecology, one main focus of ATAS is to generate synergistic effects and to improve the scientific discussion between spectroscopic experimentalists and theoreticians. The exchange of ideas in particular between experimental and theoretical applications in spectroscopy and the presentation of new analytical techniques are of special interest for many research institutions working on the improvement of transport models of toxic elements in the environment and the food chain as well as on reprocessing technologies of nuclear and non-nuclear waste. Spectroscopic studies in combination with theoretical modelling comprise the exploration of molecular mechanisms of complexation processes in aqueous or organic phases and of sorption reactions of the contaminants on mineral surfaces to obtain better process understanding on a molecular level. As a consequence, predictions of contaminant's migration behaviour will become more reliable and precise. This can improve the monitoring and removal of hazardous elements from the environment and hence, will assist strategies for remediation technologies and risk assessment. Particular emphasis is placed on the results of the first inter-laboratory Round-Robin test on actinide spectroscopy (RRT). The main goal of RRT is the comprehensive molecular analysis of the actinide complex

  4. Actinide recovery from combustible waste: the Ce(IV)-NHO3 system. Final report

    International Nuclear Information System (INIS)

    Thompson, G.H.; Childs, E.L.; Kochen, R.L.; Schmunk, R.H.; Smith, C.M.

    1979-01-01

    Actinides in ash can be leached effectively by refluxing with Ce(IV) in HNO 3 ; solubilization of actinide in ash was greater than or equal to 95% at ash concentrations to 30 g/l in stirred leachant. Plutonium and americium were the actinides present in the ash. Solubilized plutonium and americium were recovered from Ce(IV)-HNO 3 solution by solvent extraction. Extraction of plutonium into 30% tributyl phosphate in n-dodecane gave 99.99% recovery. The plutonium-depleted solution was then extracted with 30% dihexyl-N,N-diethylcarbamolylmethylenephosphonate (DHDECMP). Americium recovery was 99.64%. The Ce(IV)-HNO 3 system was compared with the HF-HNO 3 system now in common use. Advantages of the former included less equipment corrosion, no volatilization of silica, safe oxidation of carbon residues, minimal secondary waste (Ce is recycled), and better solubilization of actinide in the initial contact. However, additional contacts do not significantly improve solubilization, and a small fraction of actinide is not solubilized with Ce(IV)-HNO 3 that can be solubilized by HF-HNO 3 . The effect of the fission product ruthenium on the dissolution of actinides in the Ce(IV)-HNO 3 system was investigated briefly, and a method for removing the ruthenium electrolytically was developed. Several process flowsheets were also considered. Actinide recovery requirements will suggest which of these might best be used. 6 figures, 7 tables

  5. Actinide recovery from combustible waste: the Ce(IV)-NHO/sub 3/ system. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Thompson, G. H.; Childs, E. L.; Kochen, R. L.; Schmunk, R. H.; Smith, C. M.

    1979-09-14

    Actinides in ash can be leached effectively by refluxing with Ce(IV) in HNO/sub 3/; solubilization of actinide in ash was greater than or equal to 95% at ash concentrations to 30 g/l in stirred leachant. Plutonium and americium were the actinides present in the ash. Solubilized plutonium and americium were recovered from Ce(IV)-HNO/sub 3/ solution by solvent extraction. Extraction of plutonium into 30% tributyl phosphate in n-dodecane gave 99.99% recovery. The plutonium-depleted solution was then extracted with 30% dihexyl-N,N-diethylcarbamolylmethylenephosphonate (DHDECMP). Americium recovery was 99.64%. The Ce(IV)-HNO/sub 3/ system was compared with the HF-HNO/sub 3/ system now in common use. Advantages of the former included less equipment corrosion, no volatilization of silica, safe oxidation of carbon residues, minimal secondary waste (Ce is recycled), and better solubilization of actinide in the initial contact. However, additional contacts do not significantly improve solubilization, and a small fraction of actinide is not solubilized with Ce(IV)-HNO/sub 3/ that can be solubilized by HF-HNO/sub 3/. The effect of the fission product ruthenium on the dissolution of actinides in the Ce(IV)-HNO/sub 3/ system was investigated briefly, and a method for removing the ruthenium electrolytically was developed. Several process flowsheets were also considered. Actinide recovery requirements will suggest which of these might best be used. 6 figures, 7 tables.

  6. The study of actinide solubility limiting solid phases - a literature survey

    International Nuclear Information System (INIS)

    Thomason, H.P.

    1988-03-01

    It is important to identify the solid phases which control the solubilities of the actinides in a cementitious repository and to determine the effect of ageing on these solid phases. This literature survey contains information on the identification and ageing of actinide solubility limiting solid phases and includes references which do not necessarily relate to the control of solubility or the conditions found in the near-field of a repository of the methods which have been used to characterise actinide solids. The techniques most widely used are X-ray and electron diffraction, although they require a solid to be crystalline in order to identify it. As well as characterisation, diffraction patterns have been used to monitor changes in the crystallinity of a solid with time. The ageing of alpha active actinide solids involves two conflicting processes. An amorphous actinide precipitate will, like most solids, become more crystalline with time. However, the recoil energy from the alpha decay of actinides will displace some of the atoms from their lattice sites and cause a decrease in crystallinity. The crystallinity of actinide solids affects solubility and is therefore an important parameter to study. Recommendations have been made for further experimental work. (author)

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

    Science.gov (United States)

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

    2018-01-01

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

  8. An Advanced TALSPEAK Concept for Separating Minor Actinides. Part 2. Flowsheet Test with Actinide-spiked Simulant

    Energy Technology Data Exchange (ETDEWEB)

    Wilden, Andreas [Forschungszentrum Jülich GmbH, Institut für Energie – und Klimaforschung – Nukleare Entsorgung und Reaktorsicherheit (IEK-6), Jülich, Germany; Lumetta, Gregg J. [Nuclear Science and Engineering Group, Pacific Northwest National Laboratory, Richland, DC, USA; Sadowski, Fabian [Forschungszentrum Jülich GmbH, Institut für Energie – und Klimaforschung – Nukleare Entsorgung und Reaktorsicherheit (IEK-6), Jülich, Germany; Schmidt, Holger [Forschungszentrum Jülich GmbH, Institut für Energie – und Klimaforschung – Nukleare Entsorgung und Reaktorsicherheit (IEK-6), Jülich, Germany; Schneider, Dimitri [Forschungszentrum Jülich GmbH, Institut für Energie – und Klimaforschung – Nukleare Entsorgung und Reaktorsicherheit (IEK-6), Jülich, Germany; Gerdes, Markus [Forschungszentrum Jülich GmbH, Institut für Energie – und Klimaforschung – Nukleare Entsorgung und Reaktorsicherheit (IEK-6), Jülich, Germany; Law, Jack D. [Aqueous Separations and Radiochemistry Department, Idaho National Laboratory, Idaho Falls, ID, USA; Geist, Andreas [Karlsruhe Institute of Technology (KIT), Institute for Nuclear Waste Disposal (INE), Karlsruhe, Germany; Bosbach, Dirk [Forschungszentrum Jülich GmbH, Institut für Energie – und Klimaforschung – Nukleare Entsorgung und Reaktorsicherheit (IEK-6), Jülich, Germany; Modolo, Giuseppe [Forschungszentrum Jülich GmbH, Institut für Energie – und Klimaforschung – Nukleare Entsorgung und Reaktorsicherheit (IEK-6), Jülich, Germany

    2017-08-17

    A solvent extraction system has been developed for separating trivalent actinides from lanthanides. This “Advanced TALSPEAK” system uses 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester to extract the lanthanides into a n-dodecane-based solvent phase, while the actinides are retained in a citrate-buffered aqueous phase by complexation to N-(2-hydroxyethyl)ethylenediamine-N,N',N'-triacetic acid. Batch distribution measurements indicate that the separation of americium from the light lanthanides decreases as the pH decreases. For example, the separation factor between La and Am increases from 2.5 at pH 2.0 to 19.3 at pH 3.0. However, previous investigations indicated that the extraction rates for the heavier lanthanides decrease with increasing pH. So, a balance between these two competing effects is required. An aqueous phase in which the pH was set at 2.6 was chosen for further process development because this offered optimal separation, with a minimum separation factor of ~8.4, based on the separation between La and Am. Centrifugal contactor single-stage efficiencies were measured to characterize the performance of the system under flow conditions.

  9. Advanced Extraction Methods for Actinide/Lanthanide Separations

    Energy Technology Data Exchange (ETDEWEB)

    Scott, M.J.

    2005-12-01

    The separation of An(III) ions from chemically similar Ln(III) ions is perhaps one of the most difficult problems encountered during the processing of nuclear waste. In the 3+ oxidation states, the metal ions have an identical charge and roughly the same ionic radius. They differ strictly in the relative energies of their f- and d-orbitals, and to separate these metal ions, ligands will need to be developed that take advantage of this small but important distinction. The extraction of uranium and plutonium from nitric acid solution can be performed quantitatively by the extraction with the TBP (tributyl phosphate). Commercially, this process has found wide use in the PUREX (plutonium uranium extraction) reprocessing method. The TRUEX (transuranium extraction) process is further used to coextract the trivalent lanthanides and actinides ions from HLLW generated during PUREX extraction. This method uses CMPO [(N, N-diisobutylcarbamoylmethyl) octylphenylphosphineoxide] intermixed with TBP as a synergistic agent. However, the final separation of trivalent actinides from trivalent lanthanides still remains a challenging task. In TRUEX nitric acid solution, the Am(III) ion is coordinated by three CMPO molecules and three nitrate anions. Taking inspiration from this data and previous work with calix[4]arene systems, researchers on this project have developed a C3-symmetric tris-CMPO ligand system using a triphenoxymethane platform as a base. The triphenoxymethane ligand systems have many advantages for the preparation of complex ligand systems. The compounds are very easy to prepare. The steric and solubility properties can be tuned through an extreme range by the inclusion of different alkoxy and alkyl groups such as methyoxy, ethoxy, t-butoxy, methyl, octyl, t-pentyl, or even t-pentyl at the ortho- and para-positions of the aryl rings. The triphenoxymethane ligand system shows promise as an improved extractant for both tetravalent and trivalent actinide recoveries form

  10. Advanced Extraction Methods for Actinide/Lanthanide Separations

    International Nuclear Information System (INIS)

    Scott, M.J.

    2005-01-01

    The separation of An(III) ions from chemically similar Ln(III) ions is perhaps one of the most difficult problems encountered during the processing of nuclear waste. In the 3+ oxidation states, the metal ions have an identical charge and roughly the same ionic radius. They differ strictly in the relative energies of their f- and d-orbitals, and to separate these metal ions, ligands will need to be developed that take advantage of this small but important distinction. The extraction of uranium and plutonium from nitric acid solution can be performed quantitatively by the extraction with the TBP (tributyl phosphate). Commercially, this process has found wide use in the PUREX (plutonium uranium extraction) reprocessing method. The TRUEX (transuranium extraction) process is further used to coextract the trivalent lanthanides and actinides ions from HLLW generated during PUREX extraction. This method uses CMPO [(N, N-diisobutylcarbamoylmethyl) octylphenylphosphineoxide] intermixed with TBP as a synergistic agent. However, the final separation of trivalent actinides from trivalent lanthanides still remains a challenging task. In TRUEX nitric acid solution, the Am(III) ion is coordinated by three CMPO molecules and three nitrate anions. Taking inspiration from this data and previous work with calix[4]arene systems, researchers on this project have developed a C3-symmetric tris-CMPO ligand system using a triphenoxymethane platform as a base. The triphenoxymethane ligand systems have many advantages for the preparation of complex ligand systems. The compounds are very easy to prepare. The steric and solubility properties can be tuned through an extreme range by the inclusion of different alkoxy and alkyl groups such as methyoxy, ethoxy, t-butoxy, methyl, octyl, t-pentyl, or even t-pentyl at the ortho- and para-positions of the aryl rings. The triphenoxymethane ligand system shows promise as an improved extractant for both tetravalent and trivalent actinide recoveries form

  11. Design, synthesis, and evaluation of polyhydroxamate chelators for selective complexation of actinides

    International Nuclear Information System (INIS)

    Gopalan, A.; Jacobs, H.; Koshti, N.; Stark, P.; Huber, V.; Dasaradhi, L.; Caswell, W.; Smith, P.; Jarvinen, G.

    1995-01-01

    Specific chelating polymers targeted for actinides have much relevance to problems involving remediation of nuclear waste. Goal is to develop polymer supported, ion specific extraction systems for removing actinides and other hazardous metal ions from wastewaters. This is part of an effort to develop chelators for removing actinide ions such as Pu from soils and waste streams. Selected ligands are being attached to polymeric backbones to create novel chelating polymers. These polymers and other water soluble and insoluble polymers have been synthesized and are being evaluated for ability to selectively remove target metal ions from process waste streams

  12. Operating procedures for the manufacture of radioactive SYNROC in the actinide laboratory

    International Nuclear Information System (INIS)

    Western, K.F.

    1986-03-01

    The purpose of this manual is to acquaint the operator with the procedures required to manufacture SYNROC-containing radioactive materials in the SYNROC actinide laboratory, Lucas Heights Research Laboratories. The actinide-doped SYNROC production facility is a series of four interconnected glove boxes and one free-standing glove box. The samples of radioactive SYNROC produced in the actinide laboratory are used to carry out physical testing of the product at various laboratories on site, e.g. leach testing, auto-radiographic examination, electron-microscopc examination, atomic absorption spectrophotometry and analysis

  13. Proceedings of the specialists' meeting on the chemistry and technology of actinide elements 1998

    International Nuclear Information System (INIS)

    Kimura, Itsuro; Moriyama, Hirotake

    1999-03-01

    This report contains the Proceedings of the 5th Specialist's Meeting on the Chemistry and Technology of Actinide Elements which was held at the Research Reactor Institute, Kyoto University, on December 21 and 22, 1998. In the meeting, the present status and future prospects of the studies related with the management of minor actinides were discussed. Results of the studies such as the OMEGA project were presented and discussed for future development of technologies for partitioning and transmutation of minor actinides. (J.P.N.)

  14. Design, synthesis, and evaluation of polyhydroxamate chelators for selective complexation of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Gopalan, A.; Jacobs, H.; Koshti, N.; Stark, P.; Huber, V.; Dasaradhi, L.; Caswell, W. [New Mexico State Univ., Las Cruces, NM (United States); Smith, P.; Jarvinen, G. [Los Alamos National Lab., NM (United States)

    1995-08-01

    Specific chelating polymers targeted for actinides have much relevance to problems involving remediation of nuclear waste. Goal is to develop polymer supported, ion specific extraction systems for removing actinides and other hazardous metal ions from wastewaters. This is part of an effort to develop chelators for removing actinide ions such as Pu from soils and waste streams. Selected ligands are being attached to polymeric backbones to create novel chelating polymers. These polymers and other water soluble and insoluble polymers have been synthesized and are being evaluated for ability to selectively remove target metal ions from process waste streams.

  15. Photoelectron spectroscopy of 4f, 5f, and 2p orbital electrons and the thermochemistry of uranium oxides

    International Nuclear Information System (INIS)

    Murch, G.E.; Thorn, R.J.

    1979-01-01

    The basic reaction describing the partial pressure of oxygen in equilibrium with UO 2 +x is resolved into a set of elementary reactions for which the energies can be obtained through 5f- an 2p-orbital electron energies measured with X-ray photoelectron spectroscopy. It is shown that the energies of the valence orbitals are a direct measure of the oxygen potential and that the orbital binding energies adjusted for the coulombic self potential are linearly related to the ionicity derived from the optical dispersion theory of Phillips and van Vechten. Measurements of the O 2- (1s 2 ---) orbital energies in alkaline earth and UO 2 and ThO 2 indicates an ionicity of o.93 for the two actinide dioxides. From measurements of the intensities of the photoelectron emitted from the 5f orbital in uranium metal, uranium dioxide and uranium tetrafluoride it is shown that the densities of electrons in the 5f orbitals are the same in U,UO 2 and UF 4 . (orig.) [de

  16. Comprehensive Study of the Solubility, Thermochemistry, Ion Exchange, and Precipitation Kinetics of NO3 Cancrinite and NO3 Sodalite

    International Nuclear Information System (INIS)

    Navrotsky, Alexandra; Liu, Qinyuan

    2004-01-01

    The precipitation of aluminosilicate phases from caustic nuclear wastes has proven to be problematic in a number of processes including radionuclide separations (cementation of columns by aluminosilicate phases), tank emptying (aluminosilicate tank heels), and condensation of wastes in evaporators (aluminosilicate precipitates in the evaporators, providing nucleation sites for growth of critical masses of radioactive actinide salts). In a collaboration between SNL and UCD, we have investigated why and how these phases form, and which conditions favor the formation of which phases. These studies have involved synthesis and characterization of aluminosilicate phases formed using a variety of synthesis techniques, kinetics of precipitation, structural investigations of aluminosilicate phases, thermodynamic calculations of aluminosilicate solubility, calorimetric studies of aluminosilicate precipitation, and a limited investigation of radionuclide partitioning and ion exchange processes (involving typical tank fluid chemistries and these materials). The predominant phases that are observed in the aluminosilicate precipitates from basic tanks wastes (i.e. Hanford, Savannah River Site ''SRS'' wastes) are the salt enclathrated zeolites: sodium nitrate, sodium carbonate and sodium hydroxide sodalite and cancrinite. These phases precipitate readily from the high ionic strength, highly basic solutions at ambient temperatures as well as at elevated temperatures, with or without the presence of an external Al and Si source (both are contained in the waste solutions), and upon interactions with reactive soil components such as clays

  17. Fundamental Thermodynamics of Actinide-Bearing Mineral Waste Forms

    International Nuclear Information System (INIS)

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

    1999-01-01

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

  18. FY2011 Annual Report for the Actinide Isomer Detection Project

    International Nuclear Information System (INIS)

    Warren, Glen A.; Francy, Christopher J.; Ressler, Jennifer J.; Erikson, Luke E.; Tatishvili, Gocha; Hatarik, R.

    2011-01-01

    This project seeks to identify a new signature for actinide element detection in active interrogation. This technique works by exciting and identifying long-lived nuclear excited states (isomers) in the actinide isotopes and/or primary fission products. Observation of isomers in the fission products will provide a signature for fissile material. For the actinide isomers, the decay time and energy of the isomeric state is unique to a particular isotope, providing an unambiguous signature for SNM. This project entails isomer identification and characterization and neutron population studies. This document summarizes activities from its third year - completion of the isomer identification characterization experiments and initialization of the neutron population experiments. The population and decay of the isomeric state in 235U remain elusive, although a number of candidate gamma rays have been identified. In the course of the experiments, a number of fission fragment isomers were populated and measured (Ressler 2010). The decays from these isomers may also provide a suitable signature for the presence of fissile material. Several measurements were conducted throughout this project. This report focuses on the results of an experiment conducted collaboratively by PNNL, LLNL and LBNL in December 2010 at LBNL. The measurement involved measuring the gamma-rays emitted from an HEU target when bombarded with 11 MeV neutrons. This report discussed the analysis and resulting conclusions from those measurements. There was one strong candidate, at 1204 keV, of an isomeric signature of 235U. The half-life of the state is estimated to be 9.3 μs. The measured time dependence fits the decay time structure very well. Other possible explanations for the 1204-keV state were investigated, but they could not explain the gamma ray. Unfortunately, the relatively limited statistics of the measurement limit, and the lack of understanding of some of the systematic of the experiment, limit

  19. Specific sequestering agents for iron and the actinides

    Energy Technology Data Exchange (ETDEWEB)

    Raymond, K.N.

    1983-06-01

    The transuranium actinide ions represent one unique environmental hazard associated with the waste of the nuclear power industry. A major component associated with that waste and a potential hazard is plutonium. The synthesis of metal-ion-specific complexing agents for ions such as Pu(IV) potentially represents a powerful new approach to many of the problems posed by waste treatment. This document is a progress report of a rational approach to the synthesis of such chelating agents based on the similarities of Pu(IV) and Fe(III), the structures of naturally-occurring complexing agents which are highly specific for Fe(III), and the incorporation of the same kinds of ligating groups present in the iron complexes to make octadentate complexes highly specific for plutonium. Both thermodynamic and animal test results indicate that a relatively high degree of success has already been achieved in this aim.

  20. Solid-state actinide acid phosphites from phosphorous acid melts

    Energy Technology Data Exchange (ETDEWEB)

    Oh, George N. [Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame, 156 Fitzpatrick Hall, Notre Dame, IN 46556 (United States); Burns, Peter C., E-mail: pburns@nd.edu [Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame, 156 Fitzpatrick Hall, Notre Dame, IN 46556 (United States); Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN 46556 (United States)

    2014-07-01

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