WorldWideScience

Sample records for actinide chemistry

  1. Actinide chemistry in ionic liquids.

    Science.gov (United States)

    Takao, Koichiro; Bell, Thomas James; Ikeda, Yasuhisa

    2013-04-01

    This Forum Article provides an overview of the reported studies on the actinide chemistry in ionic liquids (ILs) with a particular focus on several fundamental chemical aspects: (i) complex formation, (ii) electrochemistry, and (iii) extraction behavior. The majority of investigations have been dedicated to uranium, especially for the 6+ oxidation state (UO2(2+)), because the chemistry of uranium in ordinary solvents has been well investigated and uranium is the most abundant element in the actual nuclear fuel cycles. Other actinides such as thorium, neptunium, plutonium, americium, and curiumm, although less studied, are also of importance in fully understanding the nuclear fuel engineering process and the safe geological disposal of radioactive wastes. PMID:22873132

  2. Chemistry of actinides and fission products

    International Nuclear Information System (INIS)

    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

  3. Overview of actinide chemistry in the WIPP

    Energy Technology Data Exchange (ETDEWEB)

    Borkowski, Marian [Los Alamos National Laboratory; Lucchini, Jean - Francois [Los Alamos National Laboratory; Richmann, Michael K [Los Alamos National Laboratory; Reed, Donald T [Los Alamos National Laboratory; Khaing, Hnin [Los Alamos National Laboratory; Swanson, Juliet [Los Alamos National Laboratory

    2009-01-01

    The year 2009 celebrates 10 years of safe operations at the Waste Isolation Pilot Plant (WIPP), the only nuclear waste repository designated to dispose defense-related transuranic (TRU) waste in the United States. Many elements contributed to the success of this one-of-the-kind facility. One of the most important of these is the chemistry of the actinides under WIPP repository conditions. A reliable understanding of the potential release of actinides from the site to the accessible environment is important to the WIPP performance assessment (PA). The environmental chemistry of the major actinides disposed at the WIPP continues to be investigated as part of the ongoing recertification efforts of the WIPP project. This presentation provides an overview of the actinide chemistry for the WIPP repository conditions. The WIPP is a salt-based repository; therefore, the inflow of brine into the repository is minimized, due to the natural tendency of excavated salt to re-seal. Reducing anoxic conditions are expected in WIPP because of microbial activity and metal corrosion processes that consume the oxygen initially present. Should brine be introduced through an intrusion scenario, these same processes will re-establish reducing conditions. In the case of an intrusion scenario involving brine, the solubilization of actinides in brine is considered as a potential source of release to the accessible environment. The following key factors establish the concentrations of dissolved actinides under subsurface conditions: (1) Redox chemistry - The solubility of reduced actinides (III and IV oxidation states) is known to be significantly lower than the oxidized forms (V and/or VI oxidation states). In this context, the reducing conditions in the WIPP and the strong coupling of the chemistry for reduced metals and microbiological processes with actinides are important. (2) Complexation - For the anoxic, reducing and mildly basic brine systems in the WIPP, the most important

  4. Recent progress in actinide borate chemistry.

    Science.gov (United States)

    Wang, Shuao; Alekseev, Evgeny V; Depmeier, Wulf; Albrecht-Schmitt, Thomas E

    2011-10-21

    The use of molten boric acid as a reactive flux for synthesizing actinide borates has been developed in the past two years providing access to a remarkable array of exotic materials with both unusual structures and unprecedented properties. [ThB(5)O(6)(OH)(6)][BO(OH)(2)]·2.5H(2)O possesses a cationic supertetrahedral structure and displays remarkable anion exchange properties with high selectivity for TcO(4)(-). Uranyl borates form noncentrosymmetric structures with extraordinarily rich topological relationships. Neptunium borates are often mixed-valent and yield rare examples of compounds with one metal in three different oxidation states. Plutonium borates display new coordination chemistry for trivalent actinides. Finally, americium borates show a dramatic departure from plutonium borates, and there are scant examples of families of actinides compounds that extend past plutonium to examine the bonding of later actinides. There are several grand challenges that this work addresses. The foremost of these challenges is the development of structure-property relationships in transuranium materials. A deep understanding of the materials chemistry of actinides will likely lead to the development of advanced waste forms for radionuclides present in nuclear waste that prevent their transport in the environment. This work may have also uncovered the solubility-limiting phases of actinides in some repositories, and allows for measurements on the stability of these materials. PMID:21915396

  5. Coordination chemistry for new actinide separation processes

    International Nuclear Information System (INIS)

    The amount of wastes and the number of chemical steps can be decreased by replacing the PUREX process extractant (TBP) by, N.N- dialkylamides (RCONR'2). Large amounts of deep underground storable wastes can be stored into sub-surface disposals if the long lived actinide isotopes are removed. Spent nuclear fuels reprocessing including the partitioning of the minor actinides Np, Am, Cm and their transmutation into short half lives fission products is appealing to the public who is not favorable to the deep underground storage of large amounts of long half lived actinide isotopes. In this paper coordination chemistry problems related to improved chemical separations by solvent extraction are presented. 2 tabs.; 4 refs

  6. 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.

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

    International Nuclear Information System (INIS)

    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.

  8. Actinide separation chemistry in nuclear waste streams and materials

    International Nuclear Information System (INIS)

    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

  9. 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)

    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 38th 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

  10. Chemistry of lower valent actinide halides

    Energy Technology Data Exchange (ETDEWEB)

    Lau, K.H.; Hildenbrand, D.L.

    1992-01-01

    This research effort was concerned almost entirely with the first two members of the actinide series, thorium and uranium, although the work was later extended to some aspects of the neptunium-fluorine system in a collaborative program with Los Alamos National Laboratory. Detailed information about the lighter actinides will be helpful in modeling the properties of the heavier actinide compounds, which will be much more difficult to study experimentally. In this program, thermochemical information was obtained from high temperature equilibrium measurements made by effusion-beam mass spectrometry and by effusion-pressure techniques. Data were derived primarily from second-law analysis so as to avoid potential errors in third-law calculations resulting from uncertainties in spectroscopic and molecular constants. This approach has the additional advantage of yielding reaction entropies that can be checked for consistency with various molecular constant assignments for the species involved. In the U-F, U-Cl, and U-Br systems, all of the gaseous species UX, UX{sub 2}, UX{sub 3}, UX{sub 4}, and UX{sub 5}, where X represents the halogen, were identified and characterized; the corresponding species ThX, ThX{sub 2}, ThX{sub 3}, and ThX{sub 4} were studied in the Th-F, Th-Cl, and Th-Br systems. A number of oxyhalide species in the systems U-0-F, U-0-Cl, Th-0-F, and Th-O-Cl were studied thermochemically. Additionally, the sublimation thermodynamics of NpF{sub 4}(s) and NpO{sub 2}F{sub 2}(s) were studied by mass spectrometry.

  11. Recent progress in actinide borate chemistry

    OpenAIRE

    Wang, S.; Alekseev, E .V.; Depmeier, W.; Albrecht-Schmitt, T.E.

    2011-01-01

    The use of molten boric acid as a reactive flux for synthesizing actinide borates has been developed in the past two years providing access to a remarkable array of exotic materials with both unusual structures and unprecedented properties. [ThB(5)O(6)(OH)(6)][BO(OH)(2)]·2.5H(2)O possesses a cationic supertetrahedral structure and displays remarkable anion exchange properties with high selectivity for TcO(4)(-). Uranyl borates form noncentrosymmetric structures with extraordinarily rich topol...

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

    International Nuclear Information System (INIS)

    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.)

  13. 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)

  14. Computational chemistry for nuclear waste characterization and processing. Relativistic quantum chemistry of actinides

    International Nuclear Information System (INIS)

    This paper describes some of the motivations and accomplishments of our grand challenge project of the same title and focuses upon the activities at Pacific Northwest National Laboratory. The United States Department of Energy (DOE) funded the project, which finishes this fiscal year. Its objectives were to develop and apply the methods of relativistic quantum chemistry to assists in the understanding and prediction of the chemistry of actinide and lanthanide compounds. This is important to the DOE because the production of nuclear weapons at DOE facilities has left a serious legacy of environmental contamination, including millions of gallons of highly radioactive waste stored in hundreds of tanks that have exceeded their life expectancy. Much of the radioactive waste involves actinides, and their large atomic number implies that relativistic effects have important chemical consequences. By using modern non-relativistic quantum chemistry techniques, it is now possible to calculate to high accuracy the structures, energetics, and properties of molecules containing light elements. Our implementation of relativistic quantum chemical methods will, for the first time on massively parallel computers, provide capabilities for modeling heavy-element compounds similar to those currently available for light-element compounds. (author)

  15. Separating the Minor Actinides Through Advances in Selective Coordination Chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Lumetta, Gregg J.; Braley, Jenifer C.; Sinkov, Sergey I.; Carter, Jennifer C.

    2012-08-22

    This report describes work conducted at the Pacific Northwest National Laboratory (PNNL) in Fiscal Year (FY) 2012 under the auspices of the Sigma Team for Minor Actinide Separation, funded by the U.S. Department of Energy Office of Nuclear Energy. Researchers at PNNL and Argonne National Laboratory (ANL) are investigating a simplified solvent extraction system for providing a single-step process to separate the minor actinide elements from acidic high-level liquid waste (HLW), including separating the minor actinides from the lanthanide fission products.

  16. Research on the actinide chemistry in Nuclear Fuel Cycle

    International Nuclear Information System (INIS)

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2004-07-01

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

  18. Actinides-1981

    International Nuclear Information System (INIS)

    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

  19. 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.

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

    International Nuclear Information System (INIS)

    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)O2 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 CeO2 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 Cr2O3 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)

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

    International Nuclear Information System (INIS)

    The use of nuclear energy obviously raises the question of the presence of radionuclides in the environment. Currently, their mitigation is a major issue associated with nuclear chemistry. This thesis focuses on both the trapping of radionuclides by porous solids called Metal-Organic Frameworks (MOF) and the crystal chemistry of the carboxylate of tetravalent actinides (AnIV). The academic knowledge of the reactivity of carboxylate of AnIV could help the understanding of actinides speciation in environment. We focused on the sequestration of iodine by aluminum based MOF. The functionalization (electron-donor group) of the MOF drastically enhances the iodine capture capacity. The removal of light actinides (Th and U) from aqueous solution was also investigated as well as the stability of (Al)-MOF under γ radiation. More than twenty coordination polymers based on tetravalent actinides have been synthesized and characterized by single crystal X-ray diffraction. The use of controlled hydrolysis promotes the formation of coordination polymers exhibiting polynuclear cluster ([U4], [Th6], [U6] and [U38]). In order to understand the formation of the largest cluster, the ex-situ study of the solvo-thermal synthesis of compound {U38} has also been investigated. (author)

  2. Advancing Chemistry with the Lanthanide and Actinide Elements Final Report, September 2013

    Energy Technology Data Exchange (ETDEWEB)

    Evans, William John [Univ. of California, Irvine, CA (United States)

    2013-09-11

    The objective of this research is to use the unique chemistry available from complexes of the lanthanides and actinides, as well as related heavy metals such as scandium, yttrium, and bismuth to advance chemistry in energy-related areas. The lanthanides and actinides have a combination of properties in terms of size, charge, electropositive character, and f valence orbitals that provides special opportunities to probe reactivity and catalysis in ways not possible with the other metals in the periodic table. We seek to discover reaction pathways and structural types that reveal new options in reaction chemistry related to energy. Identification of new paradigms in structure and reactivity should stimulate efforts to develop new types of catalytic processes that at present are not under consideration because either the transformation or the necessary intermediates are unknown. This project is one half of my laboratory’s DOE research which was split 50:50 between Catalysis and Heavy Element Chemistry programs in 2010. Hence, this report is for a half-project.

  3. Proceedings of the specialists' meeting on the chemistry and technology of actinide elements 2011

    International Nuclear Information System (INIS)

    This report contains the Proceedings of the 17th Specialists' Meeting on the Chemistry and Technology of Actinide Elements, which was held at Research Reactor Institute, Kyoto University, on February 15, 2012. This specialists' meeting has been held annually since 1994, and this is the 17th meeting for the fiscal year 2011. The accident of Fukushima Daiich Nuclear Power Plant, which occurred on March 11, 2011, showed the presence of defect in Japanese past approach to keep nuclear system safe. There is the need to improve existing technological and operational problems, as well as regulatory problems, but we should be aware of the significance of recovering social trust and peoples' peace of mind with the nuclear power. It should be noted that public's anxiety on the backend issue of nuclear system is remarkably big, and thus we must try to provide an understandable solution to them. In this meeting, we dealt with actinide chemistry and technology, which are related to the advanced nuclear fuel cycle development and the disposal of the HLW or TRU wastes. This is because, in the backend of the nuclear system, Actinide and TRU elements have substantial importance, because all of reprocessing, geologic disposal, and partitioning and transmutation depend significantly on the chemistry and technology of Actinides. Therefore, we have continued discussion and information exchange on the Actinide issues over 16 years, and this year's 17th meeting had a special meaning as the first one after the accident. In this context in this 17th meeting, we tried to return to the fundamentals of molten salt chemistry, which is the base of the dry reprocessing development. In addition, in order to expand our attitude by crossing over the fence of nuclear society, we tried to explore the potential of the adoption of molten salt chemistry to the general industry. This was a small new attempt in compliance with the recent tendency to nuclear power reduction in

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

    Energy Technology Data Exchange (ETDEWEB)

    Dacheux, N

    2002-07-01

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

  5. Influence of chloride ions on actinide chemistry. Effects of radiolysis and temperature

    International Nuclear Information System (INIS)

    This research thesis addresses the chemistry of radionuclides in natural waters, an issue which is related to the management of long life radioactive wastes. Chloride ions are the most concentrated ions but their weak complexing power explains the fact that they are often neglected in speciation calculations. The objective of this research is to identify the influence of chloride ions on transuranium elements (Np, Pu and Am). Their influence is investigated with respect to chemical conditions close to that of underground waters and for concentrated media related to storage conditions in saline media. The author discusses media-related corrections applied to thermodynamic functions, reports a bibliographic study on the stability of actinide chloride complexes, reports a spectrophotometric investigation of complexation by chlorides, and reports the study of the influence of chlorides in a carbonate medium (solubility of americium at different temperatures, and notably at room temperature)

  6. Probing the chemistry, electronic structure and redox energetics in pentavalent organometallic actinide complexes

    Energy Technology Data Exchange (ETDEWEB)

    Graves, Christopher R [Los Alamos National Laboratory; Vaughn, Anthony E [Los Alamos National Laboratory; Morris, David E [Los Alamos National Laboratory; Kiplinger, Jaqueline L [Los Alamos National Laboratory

    2008-01-01

    Complexes of the early actinides (Th-Pu) have gained considerable prominence in organometallic chemistry as they have been shown to undergo chemistries not observed with their transition- or lanthanide metal counterparts. Further, while bonding in f-element complexes has historically been considered to be ionic, the issue of covalence remains a subject of debate in the area of actinide science, and studies aimed at elucidating key bonding interactions with 5f-orbitals continue to garner attention. Towards this end, our interests have focused on the role that metal oxidation state plays in the structure, reactivity and spectral properties of organouranium complexes. We report our progress in the synthesis of substituted U{sup V}-imido complexes using various routes: (1) Direct oxidation of U{sup IV}-imido complexes with copper(I) salts; (2) Salt metathesis with U{sup V}-imido halides; (3) Protonolysis and insertion of an U{sup V}-imido alkyl or aryl complex with H-N{double_bond}CPh{sub 2} or N{triple_bond}C-Ph, respectively, to form a U{sup V}-imido ketimide complex. Further, we report and compare the crystallographic, electrochemical, spectroscopic and magnetic characterization of the pentavalent uranium (C{sub 5}Me{sub 5}){sub 2}U({double_bond}N-Ar)(Y) series (Y = OTf, SPh, C{triple_bond}C-Ph, NPh{sub 2}, OPh, N{double_bond}CPh{sub 2}) to further interrogate the molecular, electronic, and magnetic structures of this new class of uranium complexes.

  7. Combining theoretical chemistry and Xanes multi-edge experiments to probe actinide valence states

    International Nuclear Information System (INIS)

    Both structural and electronic properties of the actinide cations are of fundamental interest in order to describe the intramolecular interactions. The 5f and 6d orbitals are the first partially or totally vacant states of these elements and their properties reflect the nature of the actinide-ligand bond. Because of its chemical and orbital selectivities, XANES spectroscopy is useful to probe the actinides' frontier orbitals and then understand the cation reactivity toward chelating ligands. The actinide L3 edge contains structural information on the coordination polyhedron because of important scattering features. But very little electronic information can be extracted, due to the short core-hole lifetime, broadening the edge signal. On the other hand, the actinide M4,5 edges provide a better resolution and allow one to achieve electronic and structural information. Furthermore, coupling simulations of the experimental spectra and quantum chemical calculations lead to quantitative information such as the determination of the actinide coordination sphere and its effective charge. (authors)

  8. Combining theoretical chemistry and Xanes multi-edge experiments to probe actinide valence states

    Energy Technology Data Exchange (ETDEWEB)

    Fillaux, C.; Guilbaud, Ph.; Guillaumont, D.; Moisy, Ph.; Den Auwer, Ch. [CEA Valrho, Dir. de l' Energie Nucleaire (DEN/DRCP/SCPS), 30 - Marcoule (France); Berthet, J.C. [CEA Saclay, Dept. de Recherche sur l' Etat Condense, les Atomes et les Molecules (DSM/DRECAM/SCM), 91 - Gif sur Yvette (France); Conradsonc, St.D. [Los Alamos National Laboratory, Los Alamos, NM (United States); Hennig, C. [Forschungszentrum Rossendorf, ROBL at ESRF, 38 - Grenoble (France); Roques, J.; Simoni, E. [Institut de Physique Nucleaire, 91 - Orsay (France); Shuh, D.K.; Tyliszczak, T.; Castro-Rodriguez, I. [Lawrence Berkeley National Laboratory, Berkeley, CA (United States)

    2007-10-15

    Both structural and electronic properties of the actinide cations are of fundamental interest in order to describe the intramolecular interactions. The 5f and 6d orbitals are the first partially or totally vacant states of these elements and their properties reflect the nature of the actinide-ligand bond. Because of its chemical and orbital selectivities, XANES spectroscopy is useful to probe the actinides' frontier orbitals and then understand the cation reactivity toward chelating ligands. The actinide L3 edge contains structural information on the coordination polyhedron because of important scattering features. But very little electronic information can be extracted, due to the short core-hole lifetime, broadening the edge signal. On the other hand, the actinide M4,5 edges provide a better resolution and allow one to achieve electronic and structural information. Furthermore, coupling simulations of the experimental spectra and quantum chemical calculations lead to quantitative information such as the determination of the actinide coordination sphere and its effective charge. (authors)

  9. A quantum chemistry study of actinide(III) and lanthanide(III) complexes with tridentate nitrogen ligands

    Energy Technology Data Exchange (ETDEWEB)

    Guillaumont, D

    2004-07-01

    The structure and bonding in large complexes of actinide(III) and lanthanide(III) with tridentate N-donor ligands and water molecules have been investigated through quantum chemistry calculations in order to characterize the nature of the lanthanide-ligand and actinide-ligand bonds. Calculations have been performed using relativistic density functional theory on [M(L)(H{sub 2}O){sub 6}]{sup 3+}, [M(L)(H{sub 2}O){sub 5}Cl]{sup 2+} and [M(H{sub 2}O){sub 9}]{sup 3+} clusters where M = La, Ce, Nd, U, Pu, Am or Cm and L = 2,2':6'2''ter-pyridine (Terpy) or 2,6-bis(5,6-di-methyl-1,2,4-triazine-3-yl)pyridine (MeBtp). The calculated evolution of the M-L bond as a function of the cation shows that lanthanide-ligand distances decrease with the diminution of the ionic radius, whereas the actinide-ligand distances increase from uranium to americium and are shorter than Ln-N distances. These trends are explained by the presence of covalent effects in the metal-ligand decreasing in the order U > Pu > Am {approx_equal} Cm {approx_equal} Ln. (author)

  10. Research in actinide chemistry. Final report, March 1, 1993--February 28, 1996

    International Nuclear Information System (INIS)

    The present three-year grant period has been a fruitful one for the laboratory as research entered some new areas while continuing in others in which the group has been successful. As in past grant periods, the principal focus has been on complexation of actinide elements with inorganic and organic ligands. The ligands to study have been chosen for their value (known or potential) in actinide separations or for their potential role in environmental behavior of the actinides. Since the radioactivity of some actinides limits the variety of techniques which can be used in their study, we have used open-quotes oxidation state analogsclose quotes. These analogs have the same oxidation state and very similar chemical behavior but are stable or very long-lived. Also, the analogs are chosen for their redox stability to avoid uncertainties in interpretation of systems in which several oxidations may coexist (e.g., in the case of Pu). Examples of such analogs which we have used are: Nd(III), Eu(III) for Pu(III), Am(III), Cm(III); Th(IV) for U(IV), Pu(IV); NpO2+ for PuO2+; UO22+ for NpO22+, PuO22+. These analogs have allowed use of techniques which can increase significantly our understanding of actinide complexation

  11. Research in actinide chemistry. Final report, March 1, 1993--February 28, 1996

    Energy Technology Data Exchange (ETDEWEB)

    Choppin, G R

    1997-01-01

    The present three-year grant period has been a fruitful one for the laboratory as research entered some new areas while continuing in others in which the group has been successful. As in past grant periods, the principal focus has been on complexation of actinide elements with inorganic and organic ligands. The ligands to study have been chosen for their value (known or potential) in actinide separations or for their potential role in environmental behavior of the actinides. Since the radioactivity of some actinides limits the variety of techniques which can be used in their study, we have used {open_quotes}oxidation state analogs{close_quotes}. These analogs have the same oxidation state and very similar chemical behavior but are stable or very long-lived. Also, the analogs are chosen for their redox stability to avoid uncertainties in interpretation of systems in which several oxidations may coexist (e.g., in the case of Pu). Examples of such analogs which we have used are: Nd(III), Eu(III) for Pu(III), Am(III), Cm(III); Th(IV) for U(IV), Pu(IV); NpO{sub 2}{sup +} for PuO{sub 2}{sup +}; UO{sub 2}{sup 2+} for NpO{sub 2}{sup 2+}, PuO{sub 2}{sup 2+}. These analogs have allowed use of techniques which can increase significantly our understanding of actinide complexation.

  12. Chemistry of gaseous lower-valent actinide halides. Technical progress report

    International Nuclear Information System (INIS)

    Objective is to provide thermochemical data for key actinide halide and oxyhalide systems. Progress is reported on bond dissociation energies of gaseous ThCl4, ThCl3, ThCl2, and ThCl; bond dissociation energies of ruthenium fluorides; and mass spectroscopy of UF6

  13. Einsteinium chemistry in the gas phase: exploring the divalent character of heavy actinides

    International Nuclear Information System (INIS)

    The first chemical studies of the monopositive einsteinium ion, Es+, in the gas phase have been carried out, and its behavior compared to those for other actinide ions, with a particular focus on Bk+. The yield of laser-ablated EsO+ indicates that the Es+-O bond energy is significantly smaller than that of Bk+-O. Fluorination of Es+ and Bk+ through F-abstraction from hexafluoropropene demonstrated clearly the stability of the divalent state of Es: whereas by this process both BkF+ and BkF2+ are produced, only the ''divalent'' EsF+ product is formed. The reaction of Es+ with several different alkenes produced only small yields of adducts (e.g., EsC4H8+). These adducts are the first organoeinsteinium complexes to be identified. Whereas Es+ was inert towards 1,5-cyclooctadiene, in contrast Bk+ dehydrogenated this substrate to give BkC8H8+, demonstrating the greater activation activity of Bk+ than Es+ towards alkenes. The chemical behaviors observed in these studies are consistent with the predicted electronic structure and energetics of Es+, and the results obtained are discussed in the context of systematic trends across the actinide series. (orig.)

  14. Coordination chemistry of several radius-sensitive complexones and applications to lanthanide-actinide separations

    International Nuclear Information System (INIS)

    The relationships between the lanthanide complex formation equilibria and the lanthanide-actinide separation application of three radius sensitive ligands have been studied. The consecutive stepwise formation constants of the 1:1, 2:1, and 3:1 chelate species formed by the interaction of DHDMB and the tripositive lanthanides and yttrium were determined potentiometrically at 0.1 M ionic strength and 250C. Results indicate that three different coordination modes, one tridentate and two bidentate are in evidence. Tracer level 241Am - 155Eu cation-exchange experiments utilizing DHDMB eluents indicate that this dihydroxycarboxylate does not form a sufficiently strong americium complex to elute that actinide ahead of europium. The overall stability of the americium 3:1 complex appears intermediate between samarium and europium. Cation-exchange elutions of 241Am, 155Eu, and 160Tb mixtures with EEDTA solutions prove that the EEDTA ligand is capable of eluting americium ahead of all of the tripositive lanthanide cations. The minimum separation occurs with terbium, where the Am-Tb separation factor is 1.71. 1,5-diaminopentane-N,N,N',N'-tetraacetic acid (PMDTA) was synthesized using cation exchange. A mathematical method was developed for the formation constants of the protonated and unprotonated lanthanide-PMDTA complexes from potentiometry. Cation-exchange elutions of tracer quantities of Am, Eu, and Tb revealed that terbium is eluted ahead of both americium and europium

  15. Actinide chemistry using singlet-paired coupled cluster and its combinations with density functionals

    CERN Document Server

    Garza, Alejandro J; Scuseria, Gustavo E

    2015-01-01

    Singlet-paired coupled cluster doubles (CCD0) is a simplification of CCD that relinquishes a fraction of dynamic correlation in order to be able to describe static correlation. Combinations of CCD0 with density functionals that recover specifically the dynamic correlation missing in the former have also been developed recently. Here, we assess the accuracy of CCD0 and CCD0+DFT (and variants of these using Brueckner orbitals) as compared to well-established quantum chemical methods for describing ground-state properties of singlet actinide molecules. The $f^0$ actinyl series (UO$_2^{2+}$, NpO$_2^{2+}$, PuO$_2^{2+}$), the isoelectronic NUN, and Thorium (ThO, ThO$^{2+}$) and Nobelium (NoO, NoO$_2$) oxides are studied.

  16. PREFACE: Actinides 2009

    Science.gov (United States)

    Rao, Linfeng; Tobin, James G.; Shuh, David K.

    2010-07-01

    This volume of IOP Conference Series: Materials Science and Engineering consists of 98 papers that were presented at Actinides 2009, the 8th International Conference on Actinide Science held on 12-17 July 2009 in San Francisco, California, USA. This conference was jointly organized by Lawrence Livermore National Laboratory and Lawrence Berkeley National Laboratory. The Actinides conference series started in Baden-Baden, Germany (1975) and this first conference was followed by meetings at Asilomar, CA, USA (1981), Aix-en-Provence, France (1985), Tashkent, USSR (1989), Santa Fe, NM, USA (1993), Baden-Baden, Germany (1997), Hayama, Japan (2001), and Manchester, UK (2005). The Actinides conference series provides a regular venue for the most recent research results on the chemistry, physics, and technology of the actinides and heaviest elements. Actinides 2009 provided a forum spanning a diverse range of scientific topics, including fundamental materials science, chemistry, physics, environmental science, and nuclear fuels. Of particular importance was a focus on the key roles that basic actinide chemistry and physics research play in advancing the worldwide renaissance of nuclear energy. Editors Linfeng Rao Lawrence Berkeley National Laboratory (lrao@lbl.gov) James G Tobin Lawrence Livermore National Laboratory (tobin1@llnl.gov) David K Shuh Lawrence Berkeley National Laboratory (dkshuh@lbl.gov)

  17. Concentration of actinides in the food chain

    International Nuclear Information System (INIS)

    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)

  18. Synthesis, growth, and studies (crystal chemistry, magnetic chemistry) of actinide-based intermetallic compounds and alloys with a 1.1.1 stoichiometry

    International Nuclear Information System (INIS)

    The first part of this research thesis reports the study of the synthesis and reactivity of intermetallic compounds with a 1.1.1 stoichiometry. It presents the thermal properties of 1.1.1 compounds: general presentation of physical transitions, and of solid solutions and formation heat, application to actinides (reactivity analysis from phase diagrams, techniques of crystal synthesis and crystal growth. It describes experimental techniques: synthesis, determination of fusion temperature by dilatometry, methods used for crystal growth, characterisation techniques (metallography, X ray diffraction on powders, dilatometry). It discusses the obtained results in terms of characterisation of synthesised samples, of crystal growth, and of measurements of fusion temperature. The second part addresses crystal chemistry studies: structure of compounds with a 1.1.1 stoichiometry (Laves structures, Zr, Ti and Pu compounds), techniques of analysis by X-ray diffraction (on powders and on single crystals), result interpretation (UNiX compounds, AnTAl compounds with T being a metal from group VIII, AnTGa compounds, AnNiGe compounds, distance comparison, structure modifications under pressure). The third part concerns physical issues. The author addresses the following topics: physical properties of intermetallic 1.1.1 compounds (magnetism of yttrium phases, behaviour of uranium-based Laves phases, analysis of pseudo-binary diagrams, physical characteristics of uranium-based 1.1.1 compounds, predictions of physical measurements), analysis techniques (Moessbauer spectroscopy, SQUID for Superconducting Quantum Interference Device), and result interpretation

  19. Chemistry and migration behaviour of the actinides and fission products in natural aquatic systems

    International Nuclear Information System (INIS)

    The 66th PTB seminar was held on April 24th and 25th, 1986, at the Munich Technical University (TUM) in Garching in cooperation with the Institute for Radiochemistry of the Munich Technical University, the 'Nuclear Chemistry' special group of the Society of German Chemists, and UB/SN responsible for the BMFT project. The seminar was organized by the TUM's Institute for Radiochemistry. The seminar dealt with the following main topics: primary geochemical reactions and colloid formation; sorption mechamisms and migration behaviour in Konrad/Gorleben aquifer systems; sampling and experimental investigations; evaluation and interpretation of the data obtained by experiments. The seminar was to achieve the following objectives: information and exchange of experience with regard to the work carried out up to the present; if necessary, formulation of new issues to be discussed; improvement of the interdisciplinary cooperation (chemistry, geosciences, modelling). The following topics and individual aspects were of particular interest and were given special attention: complementary basic research in order to interpret, support and model the results obtained by experiments (sorption mechanisms and thermodynamic data for natural systems); comparability of batch, column and diffusion tests; transferability of laboratory data to natural systems (e.g. Gorleben, Konrad); redox transitions for Np, Tc at Eh values of the natural systems; dependence of the sorption/desorption data on different influencing factors, importance of the influencing factors and selection of data for model calculations. Subject analyses of the individual contributions have been made for the Energy data base. (orig./RB)

  20. The seventh international conference on the chemistry and migration behavior of actinides and fission products in the Geosphere MIGRATION'99 abstracts

    Energy Technology Data Exchange (ETDEWEB)

    Palmer, C

    1999-09-01

    The Migration conferences focus on recent developments in the fundamental chemistry of actinides and fission products in natural aquifer systems, their interactions and migration in the geosphere, and the processes involved in modeling their geochemical behavior. The primary mode dissemination of technical information will be early evening poster sessions designed to encourage intensive communication between the authors and participants. Daily oral sessions will be opened with invited lectures followed by contributed papers within the scope of each session. Sessions cover: (A) Chemistry of actinides and fission products in natural aquatic systems: (1) Solubilities and dissolution reactions; (2) Complexation with inorganic and organic ligands; (3) Redox reactions; (4) Colloid formation; and (5) Experimental methods. (B) Geochemical interactions and transport phenomena: (1) Diffusion and migration in geologic media; (2) Sorption/desorption phenomena; (3) Natural analog studies; (4) Effects of biological activities and organic materials; (5) Colloid transport; (6) Radionuclides in soils; and (7) Soil-remediation chemistries. (C) Data base development and modeling: (1) Data selection and evaluation; (2) Data base management; (3) Geochemical models and modeling; (4) Application of models; and (5) Validation of modeling results.

  1. 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).

  2. Proceedings of the seminar on the joint research project between JAERI and Universities. 'Actinide researches for 21st century - fusion between chemistry and engineering'. August 20-21, 1999, Japan Atomic Energy Research Inst., Tokai, Japan

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2000-06-01

    The Seminar on the Joint Research Project between JAERI and Universities was held in Tokai, August 20-21, 1999, to discuss future perspectives of the actinide researches for the nuclear fuel cycle. The papers related to the Joint Research Project on the Backend Chemistry were presented and discussed. The present report complies the papers contributed to the Seminar. (author)

  3. Research on the chemical speciation of actinides

    International Nuclear Information System (INIS)

    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

  4. Synthesis, chemistry, and catalytic activity of complexes of lanthanide and actinide metals in unusual oxidation states and coordination environments. Progress report, February 1, 1981-January 31, 1982

    International Nuclear Information System (INIS)

    The objectives of this research project are: (1) to demonstrate experimentally that the lanthanide and actinide metals have a more extensive chemistry than is presently known; (2) to develop a better understanding of the special features of the f orbital elements which will allow the design of f orbital complexes possessing unique chemical and physical properties; (3) to provide a basis for seeking unusual catalytic transformations involving these elements; and (4) to synthesize and explore the chemical and physical properties of mixed metal complexes which contain both lanthanide and transition metals. During the past year progress was made in each area. Some of the specific results are: (1) the first activation of CO by an organolanthanide complex was demonstrated; (2) the first, crystallograhically characterized, molecular lanthanide hydride complexes, the bridged dimers, [(C5H4R)2LnH(THF)]2 (R=H, CH3; Ln=Lu, Er, Y), were synthesized by hydrogenolysis of the appropriate (C5H4R)2Ln(C(CH3)3)(THF) complex; (3) [(C5H5)2(THF)ErH]2 was found to catalyze the homogeneous hydrogenation of alkynes; (4) the first trimetallic organolanthanide complex was synthesized; (5) the first polyhydridic organolanthanide complex was synthesized; (6) U(III) hydride was found to catalytically activate molecular hydrogen in alkene and alkyne hydrogenation reactions

  5. 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.

  6. 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.

  7. Successive change regularity of actinide properties with atomic number

    International Nuclear Information System (INIS)

    The development and achievements on chemistry of actinide elements are summarised. The relations of properties of actinides to their electronic configurations of valence electronic shells are discussed. Some anomalies of solid properties, the radius contraction, the stable state effect of f7n-orbits (n = 0, 1, 2) and the tetrad effect of oxidation states, etc., with atomic number (Z) are described. 31 figures appended show directly the successive change regularity of actinide properties with Z

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

    International Nuclear Information System (INIS)

    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

  9. The lanthanides and actinides

    International Nuclear Information System (INIS)

    This paper relates the chemical properties of the actinides to their position in the Mendeleev periodic system. The changes in the oxidation states of the actinides with increasing atomic number are similar to those of the 3d elements. Monovalent and divalent actinides are very similar to alkaline and alkaline earth elements; in the 3+ and 4+ oxidation states they resemble d elements in the respective oxidation states. However, in their highest oxidation states the actinides display their individual properties with only a slight resemblance to d elements. Finally, there is a profound similarity between the second half of the actinides and the first half of the lanthanides

  10. 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.)

  11. Actinide and fission product partitioning and transmutation

    International Nuclear Information System (INIS)

    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.)

  12. Actinide phosphonate complexes in aqueous solutions

    International Nuclear Information System (INIS)

    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 (-PO3H2) 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

  13. Speciation of actinides by the mean of synchrotron radiation; Speciation des actinides au moyen du rayonnement synchrotron

    Energy Technology Data Exchange (ETDEWEB)

    Simoni, E. [Institut de Physique Nucleaire, (IN2P3/CNRS) 91 - Orsay (France); Den Auwer, Ch. [CEA Marcoule, Dept. Radiochimie et Procedes (DRCP/SCPS), 30 (France)

    2005-09-01

    After having recalled the principle of the X absorption spectroscopy, the authors give examples illustrating the analytical possibilities of this technique and the different application fields concerning the actinides physico-chemistry (coordination chemistry, interface, solid state, solution). (O.M.)

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

    International Nuclear Information System (INIS)

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

  15. Actinide and fission product partitioning and transmutation

    International Nuclear Information System (INIS)

    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.)

  16. Actinide and fission product partitioning and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1997-07-01

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

  17. Chemistry

    International Nuclear Information System (INIS)

    The chemical research and development efforts related to the design and ultimate operation of molten-salt breeder reactor systems are concentrated on fuel- and coolant-salt chemistry, including the development of analytical methods for use in these systems. The chemistry of tellurium in fuel salt is being studied to help elucidate the role of this element in the intergranular cracking of Hastelloy N. Studies were continued of the effect of oxygen-containing species on the equilibrium between dissolved UF3 and dissolved UF4, and, in some cases, between the dissolved uranium fluorides and graphite, and the UC2. Several aspects of coolant-salt chemistry are under investigation. Hydroxy and oxy compounds that could be formed in molten NaBF4 are being synthesized and characterized. Studies of the chemistry of chromium (III) compounds in fluoroborate melts were continued as part of a systematic investigation of the corrosion of structural alloys by coolant salt. An in-line voltammetric method for determining U4+/U3+ ratios in fuel salt was tested in a forced-convection loop over a six-month period. (LK)

  18. Chemistry

    International Nuclear Information System (INIS)

    Research progress is reported in programs on fuel-salt chemistry, properties of compounds in the Li--Te system, Te spectroscopy UF4--H equilibria, porous electrode studies of molten salts, fuel salt-coolant salt reactions, thermodynamic properties of transition-metal fluorides, and properties of sodium fluoroborate. Developmental work on analytical methods is summarized including in-line analysis of molten MSBR fuel, analysis of coolant-salts for tritium, analysis of molten LiF--BeF2--ThF4 for Fe and analysis of LiF--BeF--ThF4 for Te

  19. Chemistry

    International Nuclear Information System (INIS)

    Research and development activities dealing with the chemical problems related to design and ultimate operation of molten-salt reactor systems are described. An experimental test stand was constructed to expose metallurgical test specimens to Te2 vapor at defined temperatures and deposition rates. To better define the chemistry of fluoroborate coolant, several aspects are being investigated. The behavior of hydroxy and oxy compounds in molten NaBF4 is being investigated to define reactions and compounds that may be involved in corrosion and/or could be involved in methods for trapping tritium. Two corrosion products of Hastelloy N, Na3CrF6 and Na5Cr3F14, were identified from fluoroborate systems. The evaluation of fluoroborate and alternate coolants continued. Research on the behavior of hydrogen and its isotopes is summarized. The solubilities of hydrogen, deuterium, and helium in Li2BeF4 are very low. The sorption of tritium on graphite was found to be significant (a few milligrams of tritium per kilogram of graphite), possibly providing a means of sequestering a portion of the tritium produced. Development of analytical methods continued with emphasis on voltammetric and spectrophotometric techniques for the in-line analysis of corrosion products such as Fe2+ and Cr3+ and the determination of the U3+/U4+ ratio in MSBR fuel salt. Similar studies were conducted with the NaBF4--NaF coolant salt. Information developed during the previous operation of the CSTF has been assessed and used to formulate plans for evaluation of in-line analytical methods in future CSTF operations. Electroanalytical and spectrophotometric research suggests that an electroactive protonic species is present in molten NaBF4--NaF, and that this species rapidly equilibrates with a volatile proton-containing species. Data obtained from the CSTF indicated that tritium was concentrated in the volatile species. (JGB)

  20. Device for Detecting Actinides, Method for Detecting Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Stevens, Fred J.; Wilkins-Stevens, Priscilla

    1998-10-29

    A heavy metal detector is provided comprising a first molecule and a second molecule, whereby the first and second molecules interact in a predetermined manner; a first region on the first molecule adapted to interact with an actinide; and a second region on the second molecule adapted to interact with the actinide, whereby the interactions of the actinide with the regions effect the predetermined manner of interaction between the molecules.

  1. Recovering actinide values

    International Nuclear Information System (INIS)

    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)

  2. Actinides: why are they important biologically

    International Nuclear Information System (INIS)

    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

  3. X-Ray Absorption Spectroscopy of the Actinides

    Science.gov (United States)

    Antonio, Mark R.; Soderholm, Lynda

    The recent availability of synchrotron radiation has revolutionized actinide chemistry. This is particularly true in environmental studies, where heterogeneous samples add to the already multifaceted chemistry exhibited by these ions. Environmental samples are often inhomogeneous, chemically diverse, and amorphous or poorly crystalline. Even surrogates prepared in the laboratory to simplify the natural complexity are plagued by multiple oxidation state and varied coordination polyhedra that are a reflection of inherent 5f chemistry. For example, plutonium can be found as Pu3+ Pu4+ Pu(V)O2 +, and Pu(VI)O2 2 + within naturally occurring pH-Eh conditions, consequently complex equilibria are found between these oxidation states in one solution. In addition, dissolved actinides have significant affinities for various mineral surfaces, to which they can adsorb with or without concomitant reduction-oxidation (redox) activity, depending on details of the solution and surface conditions.

  4. Photoelectron spectra of actinide compounds

    International Nuclear Information System (INIS)

    A brief overview of the application of photoelectron spectroscopy is presented for the study of actinide materials. Phenomenology as well as specific materials are discussed with illustrative examples

  5. 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

  6. Optical techniques for actinide research

    International Nuclear Information System (INIS)

    In recent years, substantial gains have been made in the development of spectroscopic techniques for electronic properties studies. These techniques have seen relatively small, but growing, application in the field of actinide research. Photoemission spectroscopies, reflectivity and absorption studies, and x-ray techniques will be discussed and illustrative examples of studies on actinide materials will be presented

  7. 44th Journées des Actinides and 10th SPCA. Scientific Programme and Abstracts

    International Nuclear Information System (INIS)

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

  8. Actinide Speciation and Solubility in a Salt Repository (Invited)

    Science.gov (United States)

    Reed, D.; Borkowski, M.; Richmann, M.; Lucchini, J.; Khaing, H.; Swanson, J.

    2009-12-01

    The use of bedded salt deposits for the permanent disposal of nuclear waste continues to receive much attention in the United States and internationally. This is largely based on the highly successful Waste Isolation Pilot Plant (WIPP) transuranic waste repository that was opened in 1999 in Southeastern New Mexico. A bedded salt formation, such as the one in which the WIPP is located, has many advantages that make it an ideal geology for permanent disposal of nuclear waste. This includes well established mining techniques, self-sealing that lead to a naturally-induced geologic isolation, a relatively dry environment, and a favorable chemistry. Herein we report on recent progress in our investigations, as part of ongoing recertification effort for the operating WIPP repository, to establish the redox distribution and overall solubility of actinides in brine. The overall ranking of actinides, from the perspective of potential contribution to release from the WIPP, is: Pu ~ Am >>U > Th >> Np, Cm. Our recent research emphasis has centered on the redox chemistry of multivalent actinides (e.g., U, Pu and Np) with the use of oxidation-state-invariant analogs (Th and Nd) to establish the solubilities. Under a wide range of conditions investigated, the predominant oxidation states established are Pu(III) and Pu(IV) for plutonium, U(IV) and U(VI) for uranium, and Am (III) for americium. Reduction pathways for plutonium include reaction with organics, reaction with reduced iron, and bioreduction by halophiles under anaerobic conditions. Uranium(VI) can also be reduced to U(IV) by reduced iron and microbial processes. Solubility data for neodymium (+3 analog), Uranium (+6 analog) and thorium (+4 analog) in brine are also reported. These data extend our past understanding of WIPP-specific actinide chemistry and show the WIPP, and salt-based repositories in general, to be a robust repository design from the perspective of actinide containment and immobilization.

  9. Sequestering agents for the removal of actinides from waste streams

    Energy Technology Data Exchange (ETDEWEB)

    Raymond, K.N.; White, D.J.; Xu, Jide; Mohs, T.R. [Univ. of California, Berkeley, CA (United States)

    1997-10-01

    The goal of this project is to take a biomimetic approach toward developing new separation technologies for the removal of radioactive elements from contaminated DOE sites. To achieve this objective, the authors are investigating the fundamental chemistry of naturally occurring, highly specific metal ion sequestering agents and developing them into liquid/liquid and solid supported actinide extraction agents. Nature produces sideophores (e.g., Enterobactin and Desferrioxamine B) to selectivity sequester Lewis acidic metal ions, in particular Fe(III), from its surroundings. These chelating agents typically use multiple catechols or hydroxamic acids to form polydentate ligands that chelate the metal ion forming very stable complexes. The authors are investigating and developing analogous molecules into selective chelators targeting actinide(IV) ions, which display similar properties to Fe(III). By taking advantage of differences in charge, preferred coordination number, and pH stability range, the transition from nature to actinide sequestering agents has been applied to the development of new and highly selective actinide extraction technologies. Additionally, the authors have shown that these chelating ligands are versatile ligands for chelating U(VI). In particular, they have been studying their coordination chemistry and fundamental interactions with the uranyl ion [UO{sub 2}]{sup 2+}, the dominant form of uranium found in aqueous media. With an understanding of this chemistry, and results obtained from in vivo uranium sequestration studies, it should be possible to apply these actinide(IV) extraction technologies to the development of new extraction agents for the removal of uranium from waste streams.

  10. Actinides in molecules: exotic properties probed by X-ray Absorption Spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Den Auwer, C.; Moisy, P.; Guilbaud, P.; Guillaumont, D.; Simoni, E.; Conradson, S.D

    2004-07-01

    Dealing with actinide elements in molecular chemistry may result in particularly attractive and exotic physico-chemical properties. In solution, one of the spectroscopic tools able to selectively probe the structural or electronic properties of these molecules is the X-ray absorption process. Different aspects of absorption edge or EXAFS analysis related to actinide studies are presented, including phenomenological and semi-quantitative approaches. (authors)

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

    OpenAIRE

    Cary, Samantha K.; Vasiliu, Monica; Baumbach, Ryan E.; Stritzinger, Jared T.; GREEN, THOMAS D.; Diefenbach, Kariem; Cross, Justin N.; Knappenberger, Kenneth L.; Liu, Guokui; Silver, Mark A.; DePrince, A. Eugene; Polinski, Matthew J.; Van Cleve, Shelley M.; House, Jane H.; Kikugawa, Naoki

    2015-01-01

    A break in periodicity occurs in the actinide series between plutonium and americium as the result of the localization of 5f electrons. The subsequent chemistry of later actinides is thought to closely parallel lanthanides in that bonding is expected to be ionic and complexation should not substantially alter the electronic structure of the metal ions. Here we demonstrate that ligation of californium(III) by a pyridine derivative results in significant deviations in the properties of the resu...

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

    International Nuclear Information System (INIS)

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

  13. Calorimetric assay of minor actinides

    Energy Technology Data Exchange (ETDEWEB)

    Rudy, C.; Bracken, D.; Cremers, T.; Foster, L.A.; Ensslin, N.

    1996-12-31

    This paper reviews the principles of calorimetric assay and evaluates its potential application to the minor actinides (U-232-4, Am-241, Am- 243, Cm-245, Np-237). We conclude that calorimetry and high- resolution gamma-ray isotopic analysis can be used for the assay of minor actinides by adapting existing methodologies for Pu/Am-241 mixtures. In some cases, mixtures of special nuclear materials and minor actinides may require the development of new methodologies that involve a combination of destructive and nondestructive assay techniques.

  14. Calorimetric assay of minor actinides

    International Nuclear Information System (INIS)

    This paper reviews the principles of calorimetric assay and evaluates its potential application to the minor actinides (U-232-4, Am-241, Am- 243, Cm-245, Np-237). We conclude that calorimetry and high- resolution gamma-ray isotopic analysis can be used for the assay of minor actinides by adapting existing methodologies for Pu/Am-241 mixtures. In some cases, mixtures of special nuclear materials and minor actinides may require the development of new methodologies that involve a combination of destructive and nondestructive assay techniques

  15. Environmental research on actinide elements

    International Nuclear Information System (INIS)

    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

  16. Actinide elements in aquatic and terrestrial environments

    International Nuclear Information System (INIS)

    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

  17. Synthesis and structural characterization of actinide oxalate compounds

    International Nuclear Information System (INIS)

    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)

  18. 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)

  19. SACSESS – the EURATOM FP7 project on actinide separation from spent nuclear fuels

    Directory of Open Access Journals (Sweden)

    Bourg Stéphane

    2015-12-01

    Full Text Available Recycling of actinides by their separation from spent nuclear fuel, followed by transmutation in fast neutron reactors of Generation IV, is considered the most promising strategy for nuclear waste management. Closing the fuel cycle and burning long-lived actinides allows optimizing the use of natural resources and minimizing the long-term hazard of high-level nuclear waste. Moreover, improving the safety and sustainability of nuclear power worldwide. This paper presents the activities striving to meet these challenges, carried out under the Euratom FP7 collaborative project SACSESS (Safety of Actinide Separation Processes. Emphasis is put on the safety issues of fuel reprocessing and waste storage. Two types of actinide separation processes, hydrometallurgical and pyrometallurgical, are considered, as well as related aspects of material studies, process modeling and the radiolytic stability of solvent extraction systems. Education and training of young researchers in nuclear chemistry is of particular importance for further development of this field.

  20. 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)

  1. THERMODYNAMICS OF THE ACTINIDES

    Energy Technology Data Exchange (ETDEWEB)

    Cunningham, Burris B.

    1962-04-01

    Recent work on the thermodynamic properties of the transplutonium elements is presented and discussed in relation to trends in thermodynamic properties of the actinide series. Accurate values are given for room temperature lattice parameters of two crystallographic forms, (facecentred cubic) fcc and dhcp (double-hexagonal closepacked), of americium metal and for the coefficients of thermal expansion between 157 and 878 deg K (dhcp) and 295 to 633 deg K (fcc). The meiting point of the metal, and its magnetic susceptibility between 77 and 823 deg K are reported and the latter compared with theoretical values for the tripositive ion calculated from spectroscopic data. Similar data (crystallography, meiting point and magnetic susceptibility) are given for metallic curium. A value for the heat of formation of americium monoxide is reported in conjunction with crystallographic data on the monoxide and mononitride. A revision is made in the current value for the heat of formation of Am/O/sub 2/ and for the potential of the Am(III)-Am(IV) couple. The crystal structures and lattice parameters are reported for the trichloride, oxychloride and oxides of californium. (auth)

  2. 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

  3. Isotope and Nuclear Chemistry Division annual report, FY 1990, October 1, 1989--September 30, 1990

    International Nuclear Information System (INIS)

    This report describes some of the major research and development programs of the Isotope and Nuclear Chemistry Division during FY 1990. The report includes articles on weapons chemistry, environmental chemistry, actinide and transition metal chemistry, geochemistry, nuclear structure and reactions, biochemistry and nuclear medicine, materials chemistry, and INC Division facilities and laboratories

  4. Investigating Actinide Molecular Adducts From Absorption Edge Spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Den Auwer, C.; Conradson, S.D.; Guilbaud, P.; Moisy, P.; Mustre de Leon, J.; Simoni, E.; /SLAC, SSRL

    2006-10-27

    Although Absorption Edge Spectroscopy has been widely applied to the speciation of actinide elements, specifically at the L{sub III} edge, understanding and interpretation of actinide edge spectra are not complete. In that sense, semi-quantitative analysis is scarce. In this paper, different aspects of edge simulation are presented, including semi-quantitative approaches. Comparison is made between various actinyl (U, Np) aquo or hydroxy compounds. An excursion into transition metal osmium chemistry allows us to compare the structurally related osmyl and uranyl hydroxides. The edge shape and characteristic features are discussed within the multiple scattering picture and the role of the first coordination sphere as well as contributions from the water solvent are described.

  5. Accuracy Improvement of Neutron Nuclear Data on Minor Actinides

    Directory of Open Access Journals (Sweden)

    Harada Hideo

    2015-01-01

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

  6. Fabrication of actinide mononitride fuel

    International Nuclear Information System (INIS)

    Fabrication of actinide mononitride fuel in JAERI is summarized. Actinide mononitride and their solid solutions were fabricated by carbothermic reduction of the oxides in N2 or N2-H2 mixed gas stream. Sintering study was also performed for the preparation of pellets for the property measurements and irradiation tests. The products were characterized to be high-purity mononitride with a single phase of NaCl-type structure. Moreover, fuel pins containing uranium-plutonium mixed nitride pellets were fabricated for the irradiation tests in JMTR and JOYO. (author)

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

    Energy Technology Data Exchange (ETDEWEB)

    Lemonnier, St

    2006-02-15

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

  8. Computational Study of Covalency and Complexation in Actinides using Static and Dynamic Simulation and Topological Density Analysis

    OpenAIRE

    Kirker, I. D. J.

    2013-01-01

    The separation of minor actinides such as americium and curium from other actinide and lanthanide-bearing components of used nuclear fuel is a necessary part of post-processing and recycling this fuel into storable components and new fuel material. Separation ratios can be optimised using a comprehensive understanding of the differences between these elements and their aqueous chemistry. This work uses computational simulation to investigate bonding behaviour and covalency differences between...

  9. 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)

  10. Characterization Of Actinides In Simulated Alkaline Tank Waste Sludges And Leachates

    International Nuclear Information System (INIS)

    In this project, both the fundamental chemistry of actinides in alkaline solutions (relevant to those present in Hanford-style waste storage tanks), and their dissolution from sludge simulants (and interactions with supernatants) have been investigated under representative sludge leaching procedures. The leaching protocols were designed to go beyond conventional alkaline sludge leaching limits, including the application of acidic leachants, oxidants and complexing agents. The simulant leaching studies confirm in most cases the basic premise that actinides will remain in the sludge during leaching with 2-3 M NaOH caustic leach solutions. However, they also confirm significant chances for increased mobility of actinides under oxidative leaching conditions. Thermodynamic data generated improves the general level of experiemental information available to predict actinide speciation in leach solutions. Additional information indicates that improved Al removal can be achieved with even dilute acid leaching and that acidic Al(NO3)3 solutions can be decontaminated of co-mobilized actinides using conventional separations methods. Both complexing agents and acidic leaching solutions have significant potential to improve the effectiveness of conventional alkaline leaching protocols. The prime objective of this program was to provide adequate insight into actinide behavior under these conditions to enable prudent decision making as tank waste treatment protocols develop.

  11. CHARACTERIZATION OF ACTINIDES IN SIMULATED ALKALINE TANK WASTE SLUDGES AND LEACHATES

    Energy Technology Data Exchange (ETDEWEB)

    Nash, Kenneth L.

    2008-11-20

    In this project, both the fundamental chemistry of actinides in alkaline solutions (relevant to those present in Hanford-style waste storage tanks), and their dissolution from sludge simulants (and interactions with supernatants) have been investigated under representative sludge leaching procedures. The leaching protocols were designed to go beyond conventional alkaline sludge leaching limits, including the application of acidic leachants, oxidants and complexing agents. The simulant leaching studies confirm in most cases the basic premise that actinides will remain in the sludge during leaching with 2-3 M NaOH caustic leach solutions. However, they also confirm significant chances for increased mobility of actinides under oxidative leaching conditions. Thermodynamic data generated improves the general level of experiemental information available to predict actinide speciation in leach solutions. Additional information indicates that improved Al removal can be achieved with even dilute acid leaching and that acidic Al(NO3)3 solutions can be decontaminated of co-mobilized actinides using conventional separations methods. Both complexing agents and acidic leaching solutions have significant potential to improve the effectiveness of conventional alkaline leaching protocols. The prime objective of this program was to provide adequate insight into actinide behavior under these conditions to enable prudent decision making as tank waste treatment protocols develop.

  12. The JAERI and Universities joint project research reports on the 4th joint research project between JAERI and Universities on backend chemistry

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2003-02-01

    In the Joint Research Project between JAERI and Universities on Backend Chemistry, the 4th-term researches of it were performed on sixteen themes from April of 1999 to March of 2001 under the four categories, i.e. Nuclear-chemistry and physical-chemistry properties of actinides', 'Solid state chemistry and nuclear fuel engineering of actinides', 'Solution chemistry and technologies for separation and analysis of actinides' and Treatment of radioactive waste and environmental chemistry'. The present report compiled the papers contributed to the Joint Research Project. (author)

  13. Actinides recycling assessment in a thermal reactor

    International Nuclear Information System (INIS)

    Highlights: • Actinides recycling is assessed using BWR fuel assemblies. • Four fuel rods are substituted by minor actinides rods in a UO2 and in a MOX fuel assembly. • Performance of standard fuel assemblies and the ones with the substitution is compared. • Reduction of actinides is measured for the fuel assemblies containing minor actinides rods. • Thermal reactors can be used for actinides recycling. - Abstract: Actinides recycling have the potential to reduce the geological repository burden of the high-level radioactive waste that is produced in a nuclear power reactor. The core of a standard light water reactor is composed only by fuel assemblies and there are no specific positions to allocate any actinides blanket, in this assessment it is proposed to replace several fuel rods by actinides blankets inside some of the reactor core fuel assemblies. In the first part of this study, a single uranium standard fuel assembly is modeled and the amount of actinides generated during irradiation is quantified for use it as reference. Later, in the same fuel assembly four rods containing 6 w/o of minor actinides and using depleted uranium as matrix were replaced and depletion was simulated to obtain the net reduction of minor actinides. Other calculations were performed using MOX fuel lattices instead of uranium standard fuel to find out how much reduction is possible to obtain. Results show that a reduction of minor actinides is possible using thermal reactors and a higher reduction is obtained when the minor actinides are embedded in uranium fuel assemblies instead of MOX fuel assemblies

  14. Progress in molecular uranium-nitride chemistry

    OpenAIRE

    King, David M.; Liddle, Stephen T

    2014-01-01

    The coordination, organometallic, and materials chemistry of uranium nitride has long been an important facet of actinide chemistry. Following matrix isolation experiments and computational characterisation, molecular, solution-based uranium chemistry has developed significantly in the last decade or so culminating most recently in the isolation of the first examples of long-sought terminal uranium nitride linkages. Herein, the field is reviewed with an emphasis on well-defined molecular spec...

  15. Actinide recovery techniques utilizing electromechanical processes

    International Nuclear Information System (INIS)

    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

  16. Actinide Waste Forms and Radiation Effects

    Science.gov (United States)

    Ewing, R. C.; Weber, W. J.

    Over the past few decades, many studies of actinides in glasses and ceramics have been conducted that have contributed substantially to the increased understanding of actinide incorporation in solids and radiation effects due to actinide decay. These studies have included fundamental research on actinides in solids and applied research and development related to the immobilization of the high level wastes (HLW) from commercial nuclear power plants and processing of nuclear weapons materials, environmental restoration in the nuclear weapons complex, and the immobilization of weapons-grade plutonium as a result of disarmament activities. Thus, the immobilization of actinides has become a pressing issue for the twenty-first century (Ewing, 1999), and plutonium immobilization, in particular, has received considerable attention in the USA (Muller et al., 2002; Muller and Weber, 2001). The investigation of actinides and

  17. Long-term plant availability of actinides

    International Nuclear Information System (INIS)

    Environmental releases of actinide elements raise issues about which data are very limited. Quantitative information is required to assess the long-term behavior of actinides and their potential hazards resulting from the transport through food chains leading to man. Of special interest is the effect of time on the changes in the availability of actinide elements for uptake by plants from soil. This study provides valuable information on the effects of weathering and aging on the uptake of actinides from soil by range and crop plants grown under realistic field conditions

  18. MOLECULAR SPECTROSCPY AND REACTIONS OF ACTINIDES IN THE GAS PHASE AND CRYOGENIC MATRICES

    Energy Technology Data Exchange (ETDEWEB)

    Heaven, Michael C.; Gibson, John K.; Marcalo, Joaquim

    2009-02-01

    In this chapter we review the spectroscopic data for actinide molecules and the reaction dynamics for atomic and molecular actinides that have been examined in the gas phase or in inert cryogenic matrices. The motivation for this type of investigation is that physical properties and reactions can be studied in the absence of external perturbations (gas phase) or under minimally perturbing conditions (cryogenic matrices). This information can be compared directly with the results from high-level theoretical models. The interplay between experiment and theory is critically important for advancing our understanding of actinide chemistry. For example, elucidation of the role of the 5f electrons in bonding and reactivity can only be achieved through the application of experimentally verified theoretical models. Theoretical calculations for the actinides are challenging due the large numbers of electrons that must be treated explicitly and the presence of strong relativistic effects. This topic has been reviewed in depth in Chapter 17 of this series. One of the goals of the experimental work described in this chapter has been to provide benchmark data that can be used to evaluate both empirical and ab initio theoretical models. While gas-phase data are the most suitable for comparison with theoretical calculations, there are technical difficulties entailed in generating workable densities of gas-phase actinide molecules that have limited the range of species that have been characterized. Many of the compounds of interest are refractory, and problems associated with the use of high temperature vapors have complicated measurements of spectra, ionization energies, and reactions. One approach that has proved to be especially valuable in overcoming this difficulty has been the use of pulsed laser ablation to generate plumes of vapor from refractory actinide-containing materials. The vapor is entrained in an inert gas, which can be used to cool the actinide species to room

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

    Science.gov (United States)

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

    2015-01-01

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

  20. Actinide sequestration using self-assembled monolayers on mesoporous supports.

    Science.gov (United States)

    Fryxell, Glen E; Lin, Yuehe; Fiskum, Sandy; Birnbaum, Jerome C; Wu, Hong; Kemner, Ken; Kelly, Shelley

    2005-03-01

    Surfactant templated synthesis of mesoporous ceramics provides a versatile foundation upon which to create high efficiency environmental sorbents. These nanoporous ceramic oxides condense a huge amount of surface area into a very small volume. The ceramic oxide interface is receptive to surface functionalization through molecular self-assembly. The marriage of mesoporous ceramics with self-assembled monolayer chemistry creates a powerful new class of environmental sorbent materials called self-assembled monolayers on mesoporous supports (SAMMS). These SAMMS materials are highly efficient sorbents whose interfacial chemistry can be fine-tuned to selectively sequester a specific target species, such as heavy metals, tetrahedral oxometalate anions, and radionuclides. Details addressing the design, synthesis, and characterization of SAMMS materials specifically designed to sequester actinides, of central importance to the environmental cleanup necessary after 40 years of weapons-grade plutonium production, as well as evaluation of their binding affinities and kinetics are presented. PMID:15787373

  1. Paving the way for the synthesis of a series of divalent actinide complexes: a theoretical perspective.

    Science.gov (United States)

    Wu, Q-Y; Lan, J-H; Wang, C-Z; Cheng, Z-P; Chai, Z-F; Gibson, J K; Shi, W-Q

    2016-02-21

    Recently, the +2 formal oxidation state in soluble molecular complexes for lanthanides (La-Nd, Sm-Lu) and actinides (Th and U) has been discovered [W. J. Evans, et al., J. Am. Chem. Soc., 2011, 133, 15914; J. Am. Chem. Soc., 2012, 134, 8420; J. Am. Chem. Soc., 2013, 135, 13310; Chem. Sci., 2015, 6, 517]. To explore the nature of the bonding and stabilities of the low-valent actinide complexes, a series of divalent actinide species, [AnCp'3](-) (An[double bond, length as m-dash]Th-Am, Cp' = [η(5)-C5H4(SiMe3)](-)) have been investigated in THF solution using scalar relativistic density functional theory. The electronic structures and electron affinity properties were systematically studied to identify the interactions between the +2 actinide ions and Cp' ligands. The ground state electron configurations for the [AnCp'3](-) species are [ThCp'3](-) 6d(2), [PaCp'3](-) 5f(2)6d(1), [UCp'3](-) 5f(3)6d(1), [NpCp'3](-) 5f(5), [PuCp'3](-) 5f(6), and [AmCp'3](-) 5f(7), respectively, according to the MO analysis. The total bonding energy decreases from the Th- to the Am-complex and the electrostatic interactions mainly dominate the bonding between the actinide atom and ligands. The electron affinity analysis suggests that the reduction reaction of AnCp'3→ [AnCp'3](-) should become increasingly facile across the actinide series from Th to Am, in accord with the known An(iii/ii) reduction potentials. This work expands the knowledge on the low oxidation state chemistry of actinides, and further motivates and guides the synthesis of related low oxidation state compounds of 5f elements.

  2. X-ray study of chemical bonding in actinides(IV) and lanthanides(III) hexa-cyanoferrates

    International Nuclear Information System (INIS)

    Bimetallic cyanide molecular solids derived from Prussian blue are well known to foster long-range magnetic ordering and show an intense inter-valence charge transfer band resulting from an exchange interaction through the cyanide-bridge. For those reasons the ferrocyanide and ferricyanide building blocks have been chosen to study electronic delocalization and covalent character in actinide bonding using an experimental and theoretical approach based on X-ray absorption spectroscopy. In 2001, the actinide (IV) and early lanthanides (III) hexacyanoferrate have been found by powder X-ray diffraction to be isostructural (hexagonal, P63/m group). Here, extended X-ray Absorption Fine Structure (EXAFS) at the iron K-edge and actinide L3-edge have been undertaken to probe the local environment of both actinides and iron cations. In an effort to describe the cyano bridge, a double edge fitting procedure including both iron and actinide edges and based on multiple scattering approach has been developed. We have also investigated the electronic properties of these molecular solids. Low energy electronic transitions have been used iron L2,3 edge, nitrogen and carbon K-edge and also actinides N4,5 edge to directly probe the valence molecular orbitals of the complex. Using a phenomenological approach, a clear distinctive behaviour between actinides and lanthanides has been shown. Then a theoretical approach using quantum chemistry calculation has shown more specifically the effect of covalency in the actinide-ferrocyanide bond. More specifically, π interactions were underlined by both theoretical and experimental methods. Finally, in agreement with the ionic character of the lanthanide bonding no inter-valence charge transfer has been observed in the corresponding optical spectra of these compounds. On the contrary, optical spectra for actinides adducts (except for thorium) show an intense inter-valence charge transfer band like in the transition metal cases which is

  3. 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...

  4. Prompt fission neutron spectrum of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Capote, R. [International Atomic Energy Agency, Vienna (Austria); Chen, Y. -J. [China Institute of Atomic Energy, Beijing (China); Hambsch, F. J. [European Commission, Joint Research Centre - IRRM, Geel (Belgium); Jurado, B. [CENBG, CNRS/IN2P3, Gradignan (France); Kornilov, N. [Ohio Univ., Athens, OH (United States); Lestone, J. P. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Litaize, O. [CEA, DEN, DER, SPRC, Saint-Paul-Lez-Durance (France); Morillon, B. [CEA, DAM, DIF, Arpajon (France); Neudecker, D. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Oberstedt, S. [European Commission, Joint Research Centre - IRRM, Geel (Belgium); Ohsawa, T. [Kinki Univ., Osaka-fu (Japan); Otuka, N. [International Atomic Energy Agency, Vienna (Austria); Pronyaev, V. G. [Institute of Physics and Power Engineering, Obninsk (Russian Federation); Saxena, A. [Bhabha Atomic Research Centre, Mumbai (India); Schmidt, K. H. [CENBG, CNRS/IN2P3, Gradignan (France); Serot, O. [CEA, DEN, DER, SPRC, Saint-Paul-Lez-Durance (France); Shcherbakov, O. A. [Petersburg Nuclear Physics Institute of NRC " Kurchatov Institute" , Gatchina (Russian Federation); Shu, N. -C. [China Institute of Atomic Energy, Beijing (China); Smith, D. L. [Argonne National Lab. (ANL), Argonne, IL (United States); Talou, P. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Trkov, A. [International Atomic Energy Agency, Vienna (Austria); Tudora, A. C. [Univ. of Bucharest, Magurele (Romania); Vogt, R. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Univ. of California, Davis, CA (United States); Vorobyev, A. S. [Petersburg Nuclear Physics Institute of NRC " Kurchatov Institute" , Gatchina (Russian Federation)

    2016-01-06

    Here, the energy spectrum of prompt neutron emitted in fission (PFNS) plays a very important role in nuclear science and technology. A Coordinated Research Project (CRP) "Evaluation of Prompt Fission Neutron Spectra of Actinides" was established by the IAEA Nuclear Data Section in 2009, with the major goal to produce new PFNS evaluations with uncertainties for actinide nuclei.

  5. 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....

  6. 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.

  7. Actinide co-conversion by internal gelation

    International Nuclear Information System (INIS)

    Suitable microstructures and homogenous microspheres of actinide compounds are of interest for future nuclear fuel or transmutation target concepts to prevent the generation and dispersal of actinide powder. Sol-gel routes are being investigated as one of the possible solutions for producing these compounds. Preliminary work is described involving internal gelation to synthesize mixed compounds including minor actinides, particularly mixed actinide or mixed actinide-inert element compounds. A parameter study is discussed to highlight the importance of the initial broth composition for obtaining gel microspheres without major defects (cracks, craters, etc.). In particular, conditions are defined to produce gel beads from Zr(IV)/Y(III)/Ce(III) or Zr(IV)/An(III) systems. After gelation, the heat treatment of these microspheres is described for the purpose of better understanding the formation of cracks after calcination and verifying the effective synthesis of an oxide solid-solution. (authors)

  8. Actinide ion sensor for pyroprocess monitoring

    Science.gov (United States)

    Jue, Jan-fong; Li, Shelly X.

    2014-06-03

    An apparatus for real-time, in-situ monitoring of actinide ion concentrations which comprises a working electrode, a reference electrode, a container, a working electrolyte, a separator, a reference electrolyte, and a voltmeter. The container holds the working electrolyte. The voltmeter is electrically connected to the working electrode and the reference electrode and measures the voltage between those electrodes. The working electrode contacts the working electrolyte. The working electrolyte comprises an actinide ion of interest. The reference electrode contacts the reference electrolyte. The reference electrolyte is separated from the working electrolyte by the separator. The separator contacts both the working electrolyte and the reference electrolyte. The separator is ionically conductive to the actinide ion of interest. The reference electrolyte comprises a known concentration of the actinide ion of interest. The separator comprises a beta double prime alumina exchanged with the actinide ion of interest.

  9. Liquid scintillation counting techniques for the determination of some alpha emitting actinides: a review

    International Nuclear Information System (INIS)

    The present report is a review of the work on liquid scintillation counting techniques, for the determination of alpha emitting actinides like uranium, plutonium, americium etc; for the last three decades (1970-1999). It covers the progress that has taken place in conventional liquid scintillation counting employing various solvents, scintillators and extractants. There is gradual development in instrumentation from integral counting of alpha emitters to alpha liquid scintillation spectrometry to resolve and identify different alpha emitters. These advancements have led to Pulse Shape Analysis (PSA) and Photon Electron Rejecting Alpha Liquid Scintillation Spectrometry (PERALS) techniques for the determination of the alpha emitters in the presence of beta and gamma activity. These techniques allow the determination of actinides at very low levels which has increased their applications to almost all the fields of chemistry; be it biomedical, environmental, geological or process chemistry of nuclear fuels. The development of biphasic technique using various extractants to separate different elements and counting in presence of one another has been made possible. Inorganic scintillators have been recently developed which have the advantage of eliminating effects of quenching and presence of beta/gamma emitting actinides. This review will serve as a reference to those who want to carry out work in the field of determination of actinides using liquid scintillation counting techniques. (author)

  10. Ionic Interactions in Actinide Tetrahalides

    Science.gov (United States)

    Akdeniz, Z.; Karaman, A.; Tosi, M. P.

    2001-05-01

    We determine a model of the ionic interactions in AX 4 compounds (where A is an atom in the actinide series from Th to Am and X = F, Cl, Br or I) by an analysis of data on the static and dynamic structure of their molecular monomers. The potential energy function that we adopt is taken from earlier work on rare-earth trihalides [Z. Akdeniz, Z. Q q e k and M. P. Tosi, Z. Naturforsch. 55a, 861 (2000)] and in particular allows for the electronic polarizability of the actinide ion. This polarizability quantitatively determines the antisymmetric-bending vibrational mode, but its magnitude remains compatible with a symmetric tetrahedral shape of the molecule at equilibrium. The fluorides have an especially high degree of ionic character, and the interionic-force parameters for each halide of the U, Np, Pu and Am series show regular trends, suggesting that extrapolations to the other transuranic-element halides may usefully be made. The Th compounds show some deviations from these trends, and the interionic-force model that we determine for ThCl4 differs somewhat from that obtained in a previous study. We therefore return on the evaluation of the relative stability of charged oligomers of ThCl4 and ZrCl4 and find confirmation of our earlier results on this problem.

  11. The ALMR actinide burning system

    International Nuclear Information System (INIS)

    The advanced liquid-metal reactor (ALMR) actinide burning system is being developed under the sponsorship of the US Department of Energy to bring its unique capabilities to fruition for deployment in the early 21st century. The system consists of four major parts: the reactor plant, the metal fuel and its recycle, the processing of light water reactor (LWR) spent fuel to extract the actinides, and the development of a residual waste package. This paper addresses the status and outlook for each of these four major elements. The ALMR is being developed by an industrial group under the leadership of General Electric (GE) in a cost-sharing arrangement with the US Department of Energy. This effort is nearing completion of the advanced conceptual design phase and will enter the preliminary design phase in 1994. The innovative modular reactor design stresses simplicity, economics, reliability, and availability. The design has evolved from GE's PRISM design initiative and has progressed to the final stages of a prelicensing review by the US Nuclear Regulatory Commission (NRC); a safety evaluation report is expected by the end of 1993. All the major issues identified during this review process have been technically resolved. The next design phases will focus on implementation of the basic safety philosophy of passive shutdown to a safe, stable condition, even without scram, and passive decay heat removal. Economic projections to date show that it will be competitive with non- nuclear and advanced LWR nuclear alternatives

  12. Experimental studies of actinides in molten salts

    International Nuclear Information System (INIS)

    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

  13. Electronic structure and magnetic properties of actinides

    International Nuclear Information System (INIS)

    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

  14. 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.

  15. Recovery of actinides from actinide-aluminium alloys by chlorination: Part II

    OpenAIRE

    Soucek, Pavel; Cassayre, Laurent; Eloirdi, Rachel; Malmbeck, Rikard; Meier, Roland; Nourry, Christophe; Claux, Benoit; Glatz, Jean-Paul

    2014-01-01

    International audience; A chlorination route is being investigated for recovery of actinides from actinide-aluminium alloys, which originate from pyrochemical recovery of actinides from spent metallic nuclear fuel by electrochemical methods in molten LiCl-KCl. In the present work, the most important steps of this route were experimentally tested using U-Pu-Al alloy prepared by electrodeposition of U and Pu on solid aluminium plate electrodes. The investigated processes were vacuum distillatio...

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

    OpenAIRE

    Cassayre, Laurent; Soucek, Pavel; Mendes, Eric; Malmbeck, Rikard; Nourry, Christophe; Eloirdi, Rachel; Glatz, Jean-Paul

    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, chlorina...

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1999-02-12

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

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

    International Nuclear Information System (INIS)

    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

  19. Actinide recovery from pyrochemical residues

    International Nuclear Information System (INIS)

    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 62- from high-chloride low-acid solution. Americium and other metals are washed from the ion exchange column with lN HNO3-4.8M NaCl. After elution, plutonium is recovered by hydroxide precipitation, and americium is recovered by NaHCO3 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

  20. Preparation of actinide targets by electrodeposition

    Science.gov (United States)

    Trautmann, N.; Folger, H.

    1989-10-01

    Actinide targets with varying thicknesses on different substrates have been prepared by electrodeposition either from aqueous solutions or from solutions of their nitrates in isopropyl alcohol. With these techniques the actinides can be deposited almost quantitatively on various backing materials within 15 to 30 min. Targets of thorium, uranium, neptunium, plutonium, americium, curium and californium with areal densities from almost carrier-free up to 1.4 mg/cm 2 on thin beryllium, carbon, titanium, tantalum and platinum foils have been prepared. In most cases, prior to the deposition, the actinides had to be purified chemically and for some of them, due to the limited amount of material available, recycling procedures were required. Applications of actinide targets in heavy-ion reactions are briefly discussed.

  1. Actinide research to solve some practical problems

    International Nuclear Information System (INIS)

    The following topics are discussed: generation of plutonium inventories by nuclear power plants; resettlement of the Marshallese Islanders into an actinide contaminated environment; high radiation background areas of the world; and radiation hazards to uranium miners

  2. Electronic structure and correlation effects in actinides

    Energy Technology Data Exchange (ETDEWEB)

    Albers, R.C.

    1998-12-01

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

  3. BWR Assembly Optimization for Minor Actinide Recycling

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-03-22

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

  4. Lanthanides and actinides in ionic liquids

    OpenAIRE

    Binnemans, Koen

    2007-01-01

    This lecture gives an overview of the research possibilities offered by combining f-elements (lanthanides and actinides) with ionic liquids [1] Many ionic liquids are solvents with weakly coordinating anions. Solvation of lanthanide and actinide ions in these solvents is different from what is observed in conventional organic solvents and water. The poorly solvating behavior can also lead to the formation of coordination compounds with low coordination numbers. The solvation of f-elements can...

  5. Superconductivity in rare earth and actinide compounds

    International Nuclear Information System (INIS)

    Rare earth and actinide compounds and the extraordinary superconducting and magnetic phenomena they exhibit are surveyed. The rare earth and actinide compounds described belong to three classes of novel superconducting materials: high temperature, high field superconductors (intermetallics and layered cuprates); superconductors containing localized magnetic moments; heavy fermion superconductors. Recent experiments on the resistive upper critical field of high Tc cuprate superconductors and the peak effect in the critical current density of the f-electron superconductor CeRu2 are discussed. (orig.)

  6. The Actinide Transition Revisited by Gutzwiller Approximation

    Science.gov (United States)

    Xu, Wenhu; Lanata, Nicola; Yao, Yongxin; Kotliar, Gabriel

    2015-03-01

    We revisit the problem of the actinide transition using the Gutzwiller approximation (GA) in combination with the local density approximation (LDA). In particular, we compute the equilibrium volumes of the actinide series and reproduce the abrupt change of density found experimentally near plutonium as a function of the atomic number. We discuss how this behavior relates with the electron correlations in the 5 f states, the lattice structure, and the spin-orbit interaction. Our results are in good agreement with the experiments.

  7. Lattice effects in the light actinides

    Energy Technology Data Exchange (ETDEWEB)

    Lawson, A.C.; Cort, B.; Roberts, J.A.; Bennett, B.I.; Brun, T.O.; Dreele, R.B. von [Los Alamos National Lab., NM (United States); Richardson, J.W. Jr. [Argonne National Lab., IL (United States)

    1998-12-31

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

  8. 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.

  9. Evaluation of actinide partitioning and transmutation

    International Nuclear Information System (INIS)

    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

  10. Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes.

    Science.gov (United States)

    Carter, Tyler J; Wilson, Richard E

    2015-10-26

    The synthesis, X-ray crystal structure, vibrational and optical spectroscopy for the eight-coordinate thiocyanate compounds, [Et4 N]4 [Pu(IV) (NCS)8 ], [Et4 N]4 [Th(IV) (NCS)8 ], and [Et4 N]4 [Ce(III) (NCS)7 (H2 O)] are reported. Thiocyanate was found to rapidly reduce plutonium to Pu(III) in acidic solutions (pHthiocyanate complex [Et4 N]4 [Pu(IV) (NCS)8 ] was crystallized when a large excess of [Et4 N][NCS] was present. This compound, along with its U(IV) analogue, maintains inner-sphere thiocyanate coordination in acetonitrile based on the observation of intense ligand-to-metal charge-transfer bands. Spectroscopic and crystallographic data do not support the interaction of the metal orbitals with the ligand π system, but support an enhanced An(IV) -NCS interaction, as the Lewis acidity of the metal ion increases from Th to Pu. PMID:26493880

  11. Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes.

    Science.gov (United States)

    Carter, Tyler J; Wilson, Richard E

    2015-10-26

    The synthesis, X-ray crystal structure, vibrational and optical spectroscopy for the eight-coordinate thiocyanate compounds, [Et4 N]4 [Pu(IV) (NCS)8 ], [Et4 N]4 [Th(IV) (NCS)8 ], and [Et4 N]4 [Ce(III) (NCS)7 (H2 O)] are reported. Thiocyanate was found to rapidly reduce plutonium to Pu(III) in acidic solutions (pHcoordination in acetonitrile based on the observation of intense ligand-to-metal charge-transfer bands. Spectroscopic and crystallographic data do not support the interaction of the metal orbitals with the ligand π system, but support an enhanced An(IV) -NCS interaction, as the Lewis acidity of the metal ion increases from Th to Pu.

  12. Actinides in Solution: Disproportionation, Strong Correlations, and Emergence

    Science.gov (United States)

    Marston, Brad; Horowitz, Steven

    2010-03-01

    Plutonium in acid solutions can be found in oxidation states III through VI. There is a striking near perfect degeneracy of the reduction-oxidation (redox) potentials, each being about 1 volt. Neptunium is the only other element that approaches this degree of degeneracy. One consequence of the redox degeneracy is a marked tendency of plutonium ions to disproportionate; up to four different oxidation states can coexist simultaneously in the same solution, greatly complicating the environmental chemistry of the element. While the degeneracy could simply be a coincidence, it could also be the manifestation of a higher-level organizing principle at work. Other systems that exhibit disproportionation raise the possibility of an emergent negative-U attractive interaction. The hypothesis is tested by combining first-principles relativistic density-functional calculations using the Amsterdam Density Functional (ADF) package with exact diagonalizations of Hubbard-like models of the strong correlations between the actinide 5f electrons.

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

    Directory of Open Access Journals (Sweden)

    Xiaoli Tan

    2010-11-01

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

  14. Fuel Chemistry Division annual progress report for 1990

    International Nuclear Information System (INIS)

    The progress report gives brief descriptions of the various activities of the Fuel Chemistry Division of Bhabha Atomic Research Centre, Bombay for the year 1990. The descriptions of activities are arranged under the headings: Fuel Development Chemistry, Chemistry of Actinides, Quality Control of Nuclear Fuels, and studies related to Nuclear Materials Accounting. At the end of the report, a list of papers published in journals and presented at various conferences/symposia is also given. (author). 7 figs., 52 tabs

  15. Solubility of actinide surrogates in nuclear glasses

    International Nuclear Information System (INIS)

    This paper discusses the results of a study of actinide surrogates in a nuclear borosilicate glass to understand the effect of processing conditions (temperature and oxidizing versus reducing conditions) on the solubility limits of these elements. The incorporation of cerium oxide, hafnium oxide, and neodymium oxide in this borosilicate glass was investigated. Cerium is a possible surrogate for tetravalent and trivalent actinides, hafnium for tetravalent actinides, and neodymium for trivalent actinides. The material homogeneity was studied by optical, scanning electron microscopy. Cerium LIII XANES spectroscopy showed that the Ce3+/Cetotal ratio increased from about 0.5 to 0.9 as the processing temperature increased from 1100 to 1400 deg. C. Cerium LIII XANES spectroscopy also confirmed that the increased Ce solubility in glasses melted under reducing conditions was due to complete reduction of all the cerium in the glass. The most significant results pointed out in the current study are that the solubility limits of the actinide surrogates increases with the processing temperature and that Ce3+ is shown to be more soluble than Ce4+ in this borosilicate glass

  16. TUCS/phosphate mineralization of actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    1997-10-01

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

  17. Waste disposal aspects of actinide separation

    International Nuclear Information System (INIS)

    Two recent NRPB reports are summarized (Camplin, W.C., Grimwood, P.D. and White, I.F., The effects of actinide separation on the radiological consequences of disposal of high-level radioactive waste on the ocean bed, Harwell, National Radiological Protection Board, NRPB-R94 (1980), London, HMSO; Hill, M.D., White, I.F. and Fleishman, A.B., The effects of actinide separation on the radiological consequences of geologic disposal of high-level waste. Harwell, National Radiological Protection Board, NRPB-R95 (1980), London, HMSO). They describe preliminary environmental assessments relevant to waste arising from the reprocessing of PWR fuel. Details are given of the modelling of transport of radionuclides to man, and of the methodology for calculating effective dose equivalents in man. Emphasis has been placed on the interaction between actinide separation and the disposal options rather than comparison of disposal options. The reports show that the effects of actinide separation do depend on the disposal method. Conditions are outlined where the required substantial further research and development work on actinide separation and recycle would be justified. Toxicity indices or 'toxic potentials' can be misleading and should not be used to guide research and development. (U.K.)

  18. Minior Actinide Doppler Coefficient Measurement Assessment

    Energy Technology Data Exchange (ETDEWEB)

    Nolan E. Hertel; Dwayne Blaylock

    2008-04-10

    The "Minor Actinide Doppler Coefficient Measurement Assessment" was a Department of Energy (DOE) U-NERI funded project intended to assess the viability of using either the FLATTOP or the COMET critical assembly to measure high temperature Doppler coefficients. The goal of the project was to calculate using the MCNP5 code the gram amounts of Np-237, Pu-238, Pu-239, Pu-241, AM-241, AM-242m, Am-243, and CM-244 needed to produce a 1E-5 in reactivity for a change in operating temperature 800C to 1000C. After determining the viability of using the assemblies and calculating the amounts of each actinide an experiment will be designed to verify the calculated results. The calculations and any doncuted experiments are designed to support the Advanced Fuel Cycle Initiative in conducting safety analysis of advanced fast reactor or acceoerator-driven transmutation systems with fuel containing high minor actinide content.

  19. Research on Actinides in Nuclear Fuel Cycles

    International Nuclear Information System (INIS)

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

  20. Sequential analysis of selected actinides in urine

    International Nuclear Information System (INIS)

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

  1. 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 reduc...... 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....

  2. Actinide elements in aquatic and terrestrial environments

    International Nuclear Information System (INIS)

    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 239Np from Np(V) to Np(IV) in cotton rats; evaluation of hazards associated with transuranium releases to the biosphere; predicting Pu in bone; adsorption--solubility--complexation phenomena in actinide partitioning between sorbents and solution; comparative soil extraction data; and comparative plant uptake data

  3. 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.)

  4. Actinide and fission product separation and transmutation

    International Nuclear Information System (INIS)

    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.)

  5. Chemical compatibility of HLW borosilicate glasses with actinides

    International Nuclear Information System (INIS)

    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 230C and 1150C. (orig.)

  6. Actinide recycle in LMFBRs as a waste management alternative

    Energy Technology Data Exchange (ETDEWEB)

    Beaman, S.L.

    1979-08-21

    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.

  7. Isotope and nuclear chemistry division. Annual report, FY 1987. Progress report, October 1986-September 1987

    International Nuclear Information System (INIS)

    This report describes progress in the major research and development programs carried out in FY 1987 by the Isotope and Nuclear Chemistry Division. The report includes articles on radiochemical weapons diagnostics and research and development; other unclassified weapons research; stable and radioactive isotope production and separation; chemical biology and nuclear medicine; element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced concepts and technology; and atmospheric chemistry

  8. Treatment of actinide-containing organic waste

    International Nuclear Information System (INIS)

    A method has been developed for reducing the volume of organic wastes and recovering the actinide elements. The waste, together with gaseous oxygen (air) is introduced into a molten salt, preferably an alkali metal carbonate such as sodium carbonate. The bath is kept at 7500 - 10000C and 0.5 - 10 atm to thermally decompose and partially oxidize the waste, while substantially reducing its volume. The gaseous effluent, mainly carbon dioxide and water vapour, is vented to the atmosphere through a series of filters to remove trace amounts of actinide elements or particulate alkali metal salts. The remaining combustion products are entrained in the molten salt. Part of the molten salt-combustion product mixture is withdrawn and mixed with an aqueous medium. Insoluble combustion products are then removed from the aqueous medium and are leached with a mixture of hydrofluoric and nitric acids to solubilize the actinide elements. The actinide elements are easily recovered from the acid solution using conventional techniques. (DN)

  9. Report of the panel on inhaled actinides

    International Nuclear Information System (INIS)

    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

  10. Actinide measurements by AMS using fluoride matrices

    Science.gov (United States)

    Cornett, R. J.; Kazi, Z. H.; Zhao, X.-L.; Chartrand, M. G.; Charles, R. J.; Kieser, W. E.

    2015-10-01

    Actinides can be measured by alpha spectroscopy (AS), mass spectroscopy or accelerator mass spectrometry (AMS). We tested a simple method to separate Pu and Am isotopes from the sample matrix using a single extraction chromatography column. The actinides in the column eluent were then measured by AS or AMS using a fluoride target matrix. Pu and Am were coprecipitated with NdF3. The strongest AMS beams of Pu and Am were produced when there was a large excess of fluoride donor atoms in the target and the NdF3 precipitates were diluted about 6-8 fold with PbF2. The measured concentrations of 239,240Pu and 241Am agreed with the concentrations in standards of known activity and with two IAEA certified reference materials. Measurements of 239,240Pu and 241Am made at A.E. Lalonde AMS Laboratory agree, within their statistical uncertainty, with independent measurements made using the IsoTrace AMS system. This work demonstrated that fluoride targets can produce reliable beams of actinide anions and that the measurement of actinides using fluorides agree with published values in certified reference materials.

  11. Rapid determination of actinides in asphalt samples

    International Nuclear Information System (INIS)

    A new rapid method for the determination of actinides in asphalt samples has been developed that can be used in emergency response situations or for routine analysis. If a radiological dispersive device, improvised nuclear device or a nuclear accident such as the accident at the Fukushima Nuclear Power Plant in March, 2011 occurs, there will be an urgent need for rapid analyses of many different environmental matrices, including asphalt materials, to support dose mitigation and environmental clean-up. The new method for the determination of actinides in asphalt utilizes a rapid furnace step to destroy bitumen and organics present in the asphalt and sodium hydroxide fusion to digest the remaining sample. Sample preconcentration steps are used to collect the actinides and a new stacked TRU Resin + DGA Resin column method is employed to separate the actinide isotopes in the asphalt samples. The TRU Resin plus DGA Resin separation approach, which allows sequential separation of plutonium, uranium, americium and curium isotopes in asphalt samples, can be applied to soil samples as well. (author)

  12. Electronic Structure of the Actinide Metals

    DEFF Research Database (Denmark)

    Johansson, B.; Skriver, Hans Lomholt

    1982-01-01

    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...

  13. Placental transfer of plutonium and other actinides

    International Nuclear Information System (INIS)

    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)

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

    Science.gov (United States)

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

    2000-07-01

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

  15. MOLECULAR SPECTROSCPY AND REACTIONS OF ACTINIDES IN THE GAS PHASE AND CRYOGENIC MATRICES

    Energy Technology Data Exchange (ETDEWEB)

    Heaven, Michael C.; Gibson, John K.; Marcalo, Joaquim

    2009-02-01

    In this chapter we review the spectroscopic data for actinide molecules and the reaction dynamics for atomic and molecular actinides that have been examined in the gas phase or in inert cryogenic matrices. The motivation for this type of investigation is that physical properties and reactions can be studied in the absence of external perturbations (gas phase) or under minimally perturbing conditions (cryogenic matrices). This information can be compared directly with the results from high-level theoretical models. The interplay between experiment and theory is critically important for advancing our understanding of actinide chemistry. For example, elucidation of the role of the 5f electrons in bonding and reactivity can only be achieved through the application of experimentally verified theoretical models. Theoretical calculations for the actinides are challenging due the large numbers of electrons that must be treated explicitly and the presence of strong relativistic effects. This topic has been reviewed in depth in Chapter 17 of this series. One of the goals of the experimental work described in this chapter has been to provide benchmark data that can be used to evaluate both empirical and ab initio theoretical models. While gas-phase data are the most suitable for comparison with theoretical calculations, there are technical difficulties entailed in generating workable densities of gas-phase actinide molecules that have limited the range of species that have been characterized. Many of the compounds of interest are refractory, and problems associated with the use of high temperature vapors have complicated measurements of spectra, ionization energies, and reactions. One approach that has proved to be especially valuable in overcoming this difficulty has been the use of pulsed laser ablation to generate plumes of vapor from refractory actinide-containing materials. The vapor is entrained in an inert gas, which can be used to cool the actinide species to room

  16. Synthesis of actinide nitrides, phosphides, sulfides and oxides

    Science.gov (United States)

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

    1992-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2001-03-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-07-05

    The Plutonium Science and Manufacturing Directorate provides world-class, safe, secure, and reliable special nuclear material research, process development, technology demonstration, and manufacturing capabilities that support the nation's defense, energy, and environmental needs. We safely and efficiently process plutonium, uranium, and other actinide materials to meet national program requirements, while expanding the scientific and engineering basis of nuclear weapons-based manufacturing, and while producing the next generation of nuclear engineers and scientists. Actinide Process Chemistry (NCO-2) safely and efficiently processes plutonium and other actinide compounds to meet the nation's nuclear defense program needs. All of our processing activities are done in a world class and highly regulated nuclear facility. NCO-2's plutonium processing activities consist of direct oxide reduction, metal chlorination, americium extraction, and electrorefining. In addition, NCO-2 uses hydrochloric and nitric acid dissolutions for both plutonium processing and reduction of hazardous components in the waste streams. Finally, NCO-2 is a key team member in the processing of plutonium oxide from disassembled pits and the subsequent stabilization of plutonium oxide for safe and stable long-term storage.

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

    International Nuclear Information System (INIS)

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Williamson, M.A. [Los Alamos National Lab., NM (US); Ebbinghaus, B.B.

    1998-06-01

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

  1. Isotope and Nuclear Chemistry Division annual report, FY 1983

    Energy Technology Data Exchange (ETDEWEB)

    Heiken, J.H.; Lindberg, H.A. (eds.)

    1984-05-01

    This report describes progress in the major research and development programs carried out in FY 1983 by the Isotope and Nuclear Chemistry Division. It covers radiochemical diagnostics of weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production, separation, and applications (including biomedical applications); element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced analytical techniques; development and applications; atmospheric chemistry and transport; and earth and planetary processes.

  2. Isotope and Nuclear Chemistry Division annual report, FY 1984

    International Nuclear Information System (INIS)

    This report describes progress in the major research and development programs carried out in FY 1984 by the Isotope and Nuclear Chemistry Division. It covers radiochemical diagnostics of weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production, separation, and applications (including biomedical applications); element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced analytical techniques: development and applications; atmospheric chemistry and transport; and earth and planetary processes. 287 refs

  3. Isotope and Nuclear Chemistry Division annual report, FY 1983

    International Nuclear Information System (INIS)

    This report describes progress in the major research and development programs carried out in FY 1983 by the Isotope and Nuclear Chemistry Division. It covers radiochemical diagnostics of weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production, separation, and applications (including biomedical applications); element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced analytical techniques; development and applications; atmospheric chemistry and transport; and earth and planetary processes

  4. Fuel Chemistry Division: annual progress report for 1988

    International Nuclear Information System (INIS)

    The progress report gives the brief descriptions of various activites of the Fuel Chemistry Division of Bhabha Atomic Research Centre, Bombay for the year 1988. The descriptions of activities are arranged under the headings: Fuel Development Chemistry of Actinides, Quality Control of Fuel, and Studies related to Nuclear Material Accounting. At the end of report, a list of publications published in journals and papers presented at various conferences/symposia during 1988 is given. (author). 13 figs., 61 tabs

  5. Minor actinide transmutation on PWR burnable poison rods

    International Nuclear Information System (INIS)

    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 keff 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 keff markedly. The PWR keff 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

  6. 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.

  7. Interaction of actinide cations with synthetic polyelectrolytes

    International Nuclear Information System (INIS)

    The binding of Am+3, Th+4 and UO2+2 to polymaleic acid, polyethylenemaleic acid and polymethylvinylethermaleic acid has been measured by a solvent extraction technique at 250C and either 0.02 or 0.10 M ionic strength. The solutions were buffered over a pH range such that the percent of carboxylate groups ionized ranged from 25 to 74%. The binding was described by two constants, β1 and β2, which were evaluated after correction for complexation of the actinide cations by acetate and hydrolysis. For comparable degrees of ionization, all three polyelectrolytes showed similar binding strengths. In general, these results indicated that the binding of actinides to these synthetic polyelectrolytes is basically similar to that of natural polyelectrolytes such as humic and fulvic acids. (orig.)

  8. 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.)

  9. Actinides: from heavy fermions to plutonium metallurgy

    International Nuclear Information System (INIS)

    The actinide elements mark the emergence of 5f electrons. The f electrons possess sufficiently unusual characteristics that their participation in atomic binding often result in dramatic changes in properties. This provides an excellent opportunity to study the question of localization of electrons; a question that is paramount in predicting the physical and chemical properties of d and f electron transition metals. The transition region between localized (magnetic) and itinerant (often superconducting) behavior provides for many interesting phenomena such as structural instabilities (polymorphism), spin fluctuations, mixed valences, charge density waves, exceptional catalytic activity and hydrogen storage. This region offers most interesting behavior such as that exhibited by the actinide compounds UBe13 and UPt3. Both compounds are heavy-fermion superconductors in which both magnetic and superconducting behavior exist in the same electrons. The consequences of f-electron bonding (which appears greatest at Plutonium) show dramatic effects on phase stability, alloying behavior, phase transformations and mechanical behavior

  10. The electrochemical properties of actinide amalgams

    International Nuclear Information System (INIS)

    Standard potentials are selected for actinides (An) and their amalgams. From the obtained results, energy characteristics are calculated and analyzed for alloy formation in An-Hg systems. It is found that solutions of the f-elements in mercury are very close in properties to amalgams of the alkali and alkaline-earth metals, except that, for the active Group III metals, the ion skeletons have a greater number of realizable charged states in the condensed phase

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

    Energy Technology Data Exchange (ETDEWEB)

    Haire, R.G.

    1985-01-01

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

  12. Nuclear data for plutonium and minor actinides

    International Nuclear Information System (INIS)

    Some experience in the usage of different evaluations of neutron constants for plutonium isotopes and minor actinides (MA) is described. That experience was obtained under designing the ABBN-93 group data set which nowadays is used widely for neutronics calculations of different cores with different spectrum and shielding. Under testing of the ABBN-93 data set through different integral and macroscopic experiments the main attention was paid to fuel nuclides and cross sections for MA practically did not verify. That gave an opportunity to change MA nuclear data for more modern without verification of the hole system. This desire appeared with new data libraries JENDL-3.2, JEF-2.2 and ENDF/B-6.2, which was not accessible under designing the ABBN-93. At the same time with the reevaluation of the basic MA nuclear data the ABBN-93 and the library FOND-2 of evaluated nuclear data files, which used as the basis for retrieving of the ABBN-93 data, were added with not very important MA data. So the FOND-2 library nowadays contents nuclear data files for all actinides with the half-life time more 1 day and also those MA which produce long-life actinides

  13. Bad chemistry

    OpenAIRE

    Petsko, Gregory A

    2004-01-01

    General chemistry courses haven't changed significantly in forty years. Because most basic chemistry students are premedical students, medical schools have enormous influence and could help us start all over again to create undergraduate chemistry education that works.

  14. Recovery of actinides from actinide-aluminium alloys by chlorination: Part II

    Science.gov (United States)

    Souček, P.; Cassayre, L.; Eloirdi, R.; Malmbeck, R.; Meier, R.; Nourry, C.; Claux, B.; Glatz, J.-P.

    2014-04-01

    A chlorination route is being investigated for recovery of actinides from actinide-aluminium alloys, which originate from pyrochemical recovery of actinides from spent metallic nuclear fuel by electrochemical methods in molten LiCl-KCl. In the present work, the most important steps of this route were experimentally tested using U-Pu-Al alloy prepared by electrodeposition of U and Pu on solid aluminium plate electrodes. The investigated processes were vacuum distillation for removal of the salt adhered on the electrode, chlorination of the alloy by chlorine gas and sublimation of the AlCl3 formed. The processes parameters were set on the base of a previous thermochemical study and an experimental work using pure UAl3 alloy. The present experimental results indicated high efficiency of salt distillation and chlorination steps, while the sublimation step should be further optimised.

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

    Directory of Open Access Journals (Sweden)

    Walter Olaf

    2016-09-01

    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.

  16. Bidentate organophosphorus solvent extraction process for actinide recovery and partition

    Science.gov (United States)

    Schulz, Wallace W.

    1976-01-01

    A liquid-liquid extraction process for the recovery and partitioning of actinide values from acidic nuclear waste aqueous solutions, the actinide values including trivalent, tetravalent and hexavalent oxidation states is provided and includes the steps of contacting the aqueous solution with a bidentate organophosphorous extractant to extract essentially all of the actinide values into the organic phase. Thereafter the respective actinide fractions are selectively partitioned into separate aqueous solutions by contact with dilute nitric or nitric-hydrofluoric acid solutions. The hexavalent uranium is finally removed from the organic phase by contact with a dilute sodium carbonate solution.

  17. Transmutation of minor actinide using thorium fueled BWR core

    International Nuclear Information System (INIS)

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

  18. Research needs in metabolism and dosimetry of the actinides

    International Nuclear Information System (INIS)

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

  19. Mathematical Chemistry

    OpenAIRE

    Trinajstić, Nenad; Gutman, Ivan

    2002-01-01

    A brief description is given of the historical development of mathematics and chemistry. A path leading to the meeting of these two sciences is described. An attempt is made to define mathematical chemistry, and journals containing the term mathematical chemistry in their titles are noted. In conclusion, the statement is made that although chemistry is an experimental science aimed at preparing new compounds and materials, mathematics is very useful in chemistry, among other things, to produc...

  20. Actinide management with commercial fast reactors

    International Nuclear Information System (INIS)

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

  1. Actinide management with commercial fast reactors

    Science.gov (United States)

    Ohki, Shigeo

    2015-12-01

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

  2. The electrochemical properties of actinide amalgams

    International Nuclear Information System (INIS)

    Selection of the values of standard potentials of An actinides and their amalgams was made. On the basis of the data obtained energy characteristics of alloy formation processes in the systems An-Hg were calculated and analyzed. It is ascertained that the properties of f-element solutions in mercury are similar to those of alkali and alkaline-earth metal amalgams with the only difference, i.e. in case of active metals of group 3 the number of realized charge value of ionic frames in condensed phase increases

  3. Compilation of actinide neutron nuclear data

    International Nuclear Information System (INIS)

    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.)

  4. 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.

  5. Supercritical fluid extraction studies on actinides

    International Nuclear Information System (INIS)

    Uranyl nitrate and plutonium in its Pu (III) as well Pu (IV) form loaded onto a tissue paper was extracted completed from paper, glass, stainless steel as well as teflon matrices using modified SC-CO2. A further investigation on recovery of actinides independent of their drying period is expected to culminate into developing an universal procedure to handle Pu bearing waste for its recovery irrespective of its drying history and oxidation states. Such endeavors ultimately lead to the potential utility of the SFE technology for efficient nuclear waste management

  6. Actinide management with commercial fast reactors

    Energy Technology Data Exchange (ETDEWEB)

    Ohki, Shigeo [Japan Atomic Energy Agency, 4002, Narita-cho, O-arai-machi, Higashi-Ibaraki-gun, Ibaraki 311-1393 (Japan)

    2015-12-31

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

  7. 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 t...... 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...

  8. 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)

  9. The electronic structure of the lanthanides and actinides, a comparison

    International Nuclear Information System (INIS)

    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

  10. Fuel Chemistry Division annual progress report for 1989

    International Nuclear Information System (INIS)

    The progress report gives a brief description of the various activities of the Fuel Chemistry Division of Bhabha Atomic Research Centre, Bombay for the year 1989. The descriptions of activities are arranged under the headings: Fuel Development Chemistry, Chemical Quality Control, Chemistry of Actinides, Sol-Gel process for the non Nuclear Ceramics and Studies related to Nuclear Material Accounting.At the end of the report, a list of papers published in journals and presented at various conferences/symposia is also given. (author). 69 tabs., 6 figs

  11. Actinide Solubility and Speciation in the WIPP

    Energy Technology Data Exchange (ETDEWEB)

    Reed, Donald T. [Los Alamos National Laboratory

    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.

  12. Fusion-Fission Burner for Transuranic Actinides

    Science.gov (United States)

    Choi, Chan

    2013-10-01

    The 14-MeV DT fusion neutron spectrum from mirror confinement fusion can provide a unique capability to transmute the transuranic isotopes from light water reactors (LWR). The transuranic (TRU) actinides, high-level radioactive wastes, from spent LWR fuel pose serious worldwide problem with long-term decay heat and radiotoxicity. However, ``transmuted'' TRU actinides can not only reduce the inventory of the TRU in the spent fuel repository but also generate additional energy. Typical commercial LWR fuel assemblies for BWR (boiling water reactor) and PWR (pressurized water reactor) measure its assembly lengths with 4.470 m and 4.059 m, respectively, while its corresponding fuel rod lengths are 4.064 m and 3.851 m. Mirror-based fusion reactor has inherently simple geometry for transmutation blanket with steady-state reactor operation. Recent development of gas-dynamic mirror configuration has additional attractive feature with reduced size in central plasma chamber, thus providing a unique capability for incorporating the spent fuel assemblies into transmutation blanket designs. The system parameters for the gas-dynamic mirror-based hybrid burner will be discussed.

  13. Electronic structure of the actinide dioxides

    International Nuclear Information System (INIS)

    The electronic properties of the fluorite structured actinide dioxides have been investigated using the linear muffin tin orbital method in the atomic sphere approximation. CaF2 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 UO2 only was considered as representative of the actinide dioxides. For comparison CaF2 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)

  14. Redox reactivity and coordination chemistry of uranium

    International Nuclear Information System (INIS)

    The study and the understanding of actinides chemistry have important implications in the nuclear field both for the development of new actinides materials and the retreatment of the nuclear wastes. One of the major issues in that chemistry is that the actinides elements are known to undergo redox reaction and to form assemblies of different size and different topologies. In that context uranium can be a good model of the heavier radioelement because it is much less radioactive. So, this work concerns the synthesis and the study of the spectroscopy and the magnetic properties of several uranium based polymetallic assemblies synthesized by taking advantage of the redox properties and the coordination chemistry of uranium. The hydrolysis reactivity of trivalent uranium has been studied in absence of sterically hindered ligands and led to the synthesis of oxo/hydroxo uranium assemblies with different sizes by changing the starting complex or the reaction conditions. By following the same strategy, the controlled oxidation of trivalent uranium complexes led to an original azido/nitrido uranium complex. The coordination chemistry of the pentavalent uranyl polymer {[UO2py5][KI2py3]}n has also been studied with different ligand and in different conditions and led to several cation-cation complexes for which the stability is sufficient for studying there dismutation by proton NMR. By changing the ancillary ligands stable monomeric complexes of pentavalent uranyl complexes were also obtained. The magnetic properties of all the complexes, monomers and polymetallic complexes were studied and an antiferromagnetic coupling was observed for the cation-cation pentavalent uranyl dimer [UO2(dbm)2(K18C6)]2. (author)

  15. Gas core reactors for actinide transmutation. [uranium hexafluoride

    Science.gov (United States)

    Clement, J. D.; Rust, J. H.; Wan, P. T.; Chow, S.

    1979-01-01

    The preliminary design of a uranium hexafluoride actinide transmutation reactor to convert long-lived actinide wastes to shorter-lived fission product wastes was analyzed. It is shown that externally moderated gas core reactors are ideal radiators. They provide an abundant supply of thermal neutrons and are insensitive to composition changes in the blanket. For the present reactor, an initial load of 6 metric tons of actinides is loaded. This is equivalent to the quantity produced by 300 LWR-years of operation. At the beginning, the core produces 2000 MWt while the blanket generates only 239 MWt. After four years of irradiation, the actinide mass is reduced to 3.9 metric tonnes. During this time, the blanket is becoming more fissile and its power rapidly approaches 1600 MWt. At the end of four years, continuous refueling of actinides is carried out and the actinide mass is held constant. Equilibrium is essentially achieved at the end of eight years. At equilibrium, the core is producing 1400 MWt and the blanket 1600 MWt. At this power level, the actinide destruction rate is equal to the production rate from 32 LWRs.

  16. Separation of actinides from spent nuclear fuel: A review.

    Science.gov (United States)

    Veliscek-Carolan, Jessica

    2016-11-15

    This review summarises the methods currently available to extract radioactive actinide elements from solutions of spent nuclear fuel. This separation of actinides reduces the hazards associated with spent nuclear fuel, such as its radiotoxicity, volume and the amount of time required for its' radioactivity to return to naturally occurring levels. Separation of actinides from environmental water systems is also briefly discussed. The actinide elements typically found in spent nuclear fuel include uranium, plutonium and the minor actinides (americium, neptunium and curium). Separation methods for uranium and plutonium are reasonably well established. On the other hand separation of the minor actinides from lanthanide fission products also present in spent nuclear fuel is an ongoing challenge and an area of active research. Several separation methods for selective removal of these actinides from spent nuclear fuel will be described. These separation methods include solvent extraction, which is the most commonly used method for radiochemical separations, as well as the less developed but promising use of adsorption and ion-exchange materials.

  17. Separation of actinides from spent nuclear fuel: A review.

    Science.gov (United States)

    Veliscek-Carolan, Jessica

    2016-11-15

    This review summarises the methods currently available to extract radioactive actinide elements from solutions of spent nuclear fuel. This separation of actinides reduces the hazards associated with spent nuclear fuel, such as its radiotoxicity, volume and the amount of time required for its' radioactivity to return to naturally occurring levels. Separation of actinides from environmental water systems is also briefly discussed. The actinide elements typically found in spent nuclear fuel include uranium, plutonium and the minor actinides (americium, neptunium and curium). Separation methods for uranium and plutonium are reasonably well established. On the other hand separation of the minor actinides from lanthanide fission products also present in spent nuclear fuel is an ongoing challenge and an area of active research. Several separation methods for selective removal of these actinides from spent nuclear fuel will be described. These separation methods include solvent extraction, which is the most commonly used method for radiochemical separations, as well as the less developed but promising use of adsorption and ion-exchange materials. PMID:27427893

  18. Chemistry Notes

    Science.gov (United States)

    School Science Review, 1976

    1976-01-01

    Described are eight chemistry experiments and demonstrations applicable to introductory chemistry courses. Activities include: measure of lattice enthalpy, Le Chatelier's principle, decarboxylation of soap, use of pocket calculators in pH measurement, and making nylon. (SL)

  19. Colour Chemistry

    Science.gov (United States)

    Griffiths, J.; Rattee, I. D.

    1973-01-01

    Discusses the course offerings in pure color chemistry at two universities and the three main aspects of study: dyestuff chemistry, color measurement, and color application. Indicates that there exists a constant challenge to ingenuity in the subject discipline. (CC)

  20. Positronium chemistry

    CERN Document Server

    Green, James

    1964-01-01

    Positronium Chemistry focuses on the methodologies, reactions, processes, and transformations involved in positronium chemistry. The publication first offers information on positrons and positronium and experimental methods, including mesonic atoms, angular correlation measurements, annihilation spectra, and statistical errors in delayed coincidence measurements. The text then ponders on positrons in gases and solids. The manuscript takes a look at the theoretical chemistry of positronium and positronium chemistry in gases. Topics include quenching, annihilation spectrum, delayed coincidence

  1. Combinatorial chemistry

    DEFF Research Database (Denmark)

    Nielsen, John

    1994-01-01

    An overview of combinatorial chemistry is presented. Combinatorial chemistry, sometimes referred to as `irrational drug design,' involves the generation of molecular diversity. The resulting chemical library is then screened for biologically active compounds.......An overview of combinatorial chemistry is presented. Combinatorial chemistry, sometimes referred to as `irrational drug design,' involves the generation of molecular diversity. The resulting chemical library is then screened for biologically active compounds....

  2. Scenarios for the transmutation of actinides in CANDU reactors

    Energy Technology Data Exchange (ETDEWEB)

    Hyland, Bronwyn, E-mail: hylandb@aecl.ca [Atomic Energy of Canada Limited, Chalk River Laboratories, Chalk River, Ontario, K0J 1J0 (Canada); Gihm, Brian, E-mail: gihmb@aecl.ca [Atomic Energy of Canada Limited, 2251 Speakman Drive, Mississauga, Ontario, L5K 1B2 (Canada)

    2011-12-15

    With world stockpiles of used nuclear fuel increasing, the need to address the long-term utilization of this resource is being studied. Many of the transuranic (TRU) actinides in nuclear spent fuel produce decay heat for long durations, resulting in significant nuclear waste management challenges. These actinides can be transmuted to shorter-lived isotopes to reduce the decay heat period or consumed as fuel in a CANDU(R) reactor. Many of the design features of the CANDU reactor make it uniquely adaptable to actinide transmutation. The small, simple fuel bundle simplifies the fabrication and handling of active fuels. Online refuelling allows precise management of core reactivity and separate insertion of the actinides and fuel bundles into the core. The high neutron economy of the CANDU reactor results in high TRU destruction to fissile-loading ratio. This paper provides a summary of actinide transmutation schemes that have been studied in CANDU reactors at AECL, including the works performed in the past. The schemes studied include homogeneous scenarios in which actinides are uniformly distributed in all fuel bundles in the reactor, as well as heterogeneous scenarios in which dedicated channels in the reactor are loaded with actinide targets and the rest of the reactor is loaded with fuel. The transmutation schemes that are presented reflect several different partitioning schemes. Separation of americium, often with curium, from the other actinides enables targeted destruction of americium, which is a main contributor to the decay heat 100-1000 years after discharge from the reactor. Another scheme is group-extracted transuranic elements, in which all of the transuranic elements, plutonium (Pu), neptunium (Np), americium (Am), and curium (Cm) are extracted together and then transmuted. This paper also addresses ways of utilizing the recycled uranium, another stream from the separation of spent nuclear fuel, in order to drive the transmutation of other actinides.

  3. 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. PMID:21709501

  4. Distribution of actinides in SFR1; Aktinidfoerdelning i SFR1

    Energy Technology Data Exchange (ETDEWEB)

    Ingemansson, Tor [ALARA Engineering, Skultuna (Sweden)

    2000-02-01

    The amount of actinides in the Swedish repository for intermediate level radioactive wastes has been estimated. The sources for the actinides are mainly the purification filters of the reactors and the used fuel pools. Defect fuel elements are the originating source of the actinides. It is estimated that the 12 Swedish reactors, in total, have had 2.2 kg of fuel dissolved in their systems since start-up. About 880 g of this amount has been brought to the intermediate-level repository.

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

    International Nuclear Information System (INIS)

    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

  6. Status report on actinide and fission product transmutation studies

    International Nuclear Information System (INIS)

    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

  7. 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)

  8. Actinide interactions at microbial interfaces: an interdisciplinary challenge

    International Nuclear Information System (INIS)

    An overview on the current state of knowledge of microbial actinide interaction processes is presented. Several detailed examples of the interaction of aerobic soil bacteria (Pseudomonas, Bacillus and Deinococcus strains) with uranium and plutonium are discussed. Details of the nature of the bacterial functional groups involved in the interfacial actinide interaction process are reported. Based on time-resolved laser-induced fluorescence spectroscopy (TRLFS) and synchrotron X-ray absorption spectroscopy (XANES and EXAFS) studies, molecular-level mechanistic details of the different interaction processes are discussed. Areas of this emerging field in actinide research are outlined where additional information and integrated interdisciplinary research is required

  9. Solidification of simulated actinides by natural zircon

    Institute of Scientific and Technical Information of China (English)

    YANG Jian-Wen; LUO Shang-Geng

    2004-01-01

    Natural zircon was used as precursor material to produce a zircon waste form bearing 20wt% simulated actinides (Nd2O3 and UO2) through a solid state reaction by a typical synroc fabrication process. The fabricated zircon waste form has relatively good physical properties (density 5.09g/cm3, open porosity 4.0%, Vickers hardness 715kg/mm2). The XRD, SEM/EDS and TEM/EDS analyses indicate that there are zircon phases containing waste elements formed through the reaction. The chemical durability and radiation stability are determined by the MCC-1method and heavy ion irradiation; the results show that the zircon waste form is highly leach resistance and relatively stable under irradiation (amorphous dose 0.7dpa). From this study, the method of using a natural mineral to solidify radioactive waste has proven to be feasible.

  10. Gamma spectroscopy of neutron rich actinide nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Birkenbach, Benedikt; Geibel, Kerstin; Vogt, Andreas; Hess, Herbert; Reiter, Peter; Steinbach, Tim; Schneiders, David [Koeln Univ. (Germany). IKP; Collaboration: AGATA-Collaboration

    2013-07-01

    Excited states in neutron-rich actinide Th and U nuclei were investigated after multi nucleon transfer reactions employing the AGATA demonstrator and PRISMA setup at LNL (INFN, Italy). A primary {sup 136}Xe beam of 1 GeV hitting a {sup 238}U target was used to produce the nuclei of interest. Beam-like reaction products of Xe- and Ba isotopes after neutron transfer were selected by the PRISMA spectrometer. The recoil like particles were registered by a MCP detector inside the scattering chamber. Coincident γ-rays from excited states in beam and target like particles were measured with the position sensitive AGATA HPGe detectors. Improved Doppler correction and quality of the γ-spectra is based on the novel γ-ray tracking technique which was successfully exploited. First results on the collective properties of various Th and U isotopes are discussed.

  11. 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.

  12. 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.

  13. Pyrometallurgical processes for recovery of actinide elements

    International Nuclear Information System (INIS)

    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. Crystal chemistry of transuranium pnictides

    International Nuclear Information System (INIS)

    The synthesis and crystal chemistry of M transuranium element pnictides (M = Np, Pu, Am and Cm) are described. Msub(a) Xsub(b) binary compounds have been prepared (X = P, As, Sb, and Bi) with the following (a:b) stoechiometric ratios: (1:2), (3:4), (1:1), (4:3). MXY and M2XY2 ternary compounds (Y = O, S, Se and Te) have also been prepared. The crystal structure encountered in these compounds of Pu, Am and Cm is generally the same as in the corresponding rare-earth compounds. Thorium and uranium compounds were grouped in a distinct set where the actinide ion was considered as tetravalent. Neptunium exhibits an intermediate behaviour and was found to give either uranium-like compounds such as NpAs2, or rare-earth like compounds such as NpSn2. From the plots of the lattice constants versus the actinide atomic number, we could infer that the 5f electrons are likely to be delocalised in the compounds; no 5f - shell contraction seems to occur. Furthermore these results lead to assume that in the isostructural diantimonides of the light rare-earths, 4f wave-fonctions must be involved in the bonds just; like in the LnSbTe ternary compounds. As the f electrons delocalization is dependent on crystal structure, the various structures found in our system have been studied

  15. An atomic beam source for actinide elements: concept and realization

    International Nuclear Information System (INIS)

    For ultratrace analysis of actinide elements and studies of their atomic properties with resonance ionization mass spectroscopy (RIMS), efficient and stable sources of actinide atomic beams are required. The thermodynamics and kinetics of the evaporation of actinide elements and oxides from a variety of metals were considered, including diffusion, desorption, and associative desorption. On this basis various sandwich-type filaments were studied. The most promising system was found to consist of tantalum as the backing material, an electrolytically deposited actinide hydroxide as the source of the element, and a titanium covering layer for its reduction to the metal. Such sandwich sources were experimentally proven to be well suited for the production of atomic beams of plutonium, curium, berkelium and californium at relatively low operating temperatures and with high and reproducible yields. (orig.)

  16. Distribution of actinide elements in sediments: leaching studies

    International Nuclear Information System (INIS)

    Previous investigations have shown that Fe and Mn oxides and organic matter can significantly influence the behavior of Pu and other actinides in the environment. A sequential leaching procedure has been developed in order to investigate the solid phase distribution of the actinides in riverine and marine sediments. Seven different sedimentary fractions are defined by this leaching experiment: an exchangeable metals fraction, an organic fraction, a carbonate fraction, a Mn oxide fraction, an amorphous Fe fraction, a crystalline Fe oxide fraction and a lattice-held or residual fraction. There is also the option of including a metal sufide fraction. A preliminary experiment, analyzing only the metals and not the actinide elements, indicates that this leaching procedure (with some modifications) is a viable procedure. The subsequent data should result in information concerning the geochemical history and behavior of these actinide elements in the environment

  17. Element Partitioning in Glass-Ceramic Designed for Actinides Immobilization

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    <正>Glass-ceramics were designed for immobilization of actinides. In order to immobilizing more wastes in the matrix and to develop the optimum formulation for the glass-ceramic, it is necessary to study the

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

    International Nuclear Information System (INIS)

    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.

  19. In-situ mineralization of actinides with phytic acid

    International Nuclear Information System (INIS)

    A new approach to the remediation of actinide contamination is described. A hydrolytically unstable organophosphorus compound, phytic acid, is introduced into the contaminated environment. In the short term (up to several hundred years), phytate acts as a cation exchanger to absorb mobile actinide ions from ground waters. Ultimately, phytate decomposes to release phosphate and promote the formation of insoluble phosphate mineral phases, considered an ideal medium to immobilize actinides, as it forms compounds with the lowest solubility of any candidate mineral species. This overview will discuss the rate of hydrolysis of phytic acid, the formation of lanthanide/actinide phosphate mineral forms, the cation exchange behavior of insoluble phytate, and results from laboratory demonstration of the application to soils from the Fernald site

  20. 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.

  1. Separation of Minor Actinides from Lanthanides by Dithiophosphinic Acid Extractants

    Energy Technology Data Exchange (ETDEWEB)

    D. R. Peterman; M. R. Greenhalgh; R. D. Tillotson; J. R. Klaehn; M. K. Harrup; T. A. Luther; J. D. Law; L. M. Daniels

    2008-09-01

    The selective extraction of the minor actinides (Am(III) and Cm(III)) from the lanthanides is an important part of advanced reprocessing of spent nuclear fuel. This separation would allow the Am/Cm to be fabricated into targets and recycled to a reactor and the lanthanides to be dispositioned. This separation is difficult to accomplish due to the similarities in the chemical properties of the trivalent actinides and lanthanides. Research efforts at the Idaho National Laboratory have identified an innovative synthetic pathway yielding new regiospecific dithiophosphinic acid (DPAH) extractants. The synthesis provides DPAH derivatives that can address the issues concerning minor actinide separation and extractant stability. For this work, two new symmetric DPAH extractants have been prepared. The use of these extractants for the separation of minor actinides from lanthanides will be discussed.

  2. Clays at the natural nuclear reactor at Bangombe, Gabon: migration of actinides

    International Nuclear Information System (INIS)

    Clay minerals were examined from the natural nuclear reactor at Bangombe. The clay mineralogy of the reactor facies is: illite, kaolinite and minor chlorite (FB formation); illite with chlorite and kaolinite in hydrothermal veins (argile de pile); illite and chlorite (reactor core); and (i) chlorite and kaolinite ± illite ± smectite or (ii) illite in the underlying FA formation. Illite crystallinity values are in general highest in rocks that experienced the highest temperatures during reactor operation. Chlorite chemistry varies with respect to position around the reactor: both di-tri and trioctahedral chlorites are present in hydrothermal veins within the argile de pile, dioctahedral chlorites are present in the FA formation within cm of the reactor core, trioctahedral chlorites are present within a meter of the reactor. Chemical data for the argile de pile and the FB formation suggest that formation of the former unit occurred as a result of thermal metamorphism of the FB pelites, as opposed to large-scale dissolution of the sandstones of the FA formation. Autoradiography is used to study the sorptive characteristics of the clays for actinides. The results show that actinide sorption varies in the order: chlorite > illite ≅ kaolinite. (orig.)

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

    International Nuclear Information System (INIS)

    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.)

  4. The effect of corrosion product colloids on actinide transport

    International Nuclear Information System (INIS)

    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 Rd values of ≥ 5 x 106 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)

  5. Analysis of the Gas Core Actinide Transmutation Reactor (GCATR)

    Science.gov (United States)

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

    1977-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Perkasa, Y. S. [Department of Physics, Sunan Gunung Djati State Islamic University Bandung, Jl. A.H Nasution No. 105 Cibiru, Bandung (Indonesia); Waris, A., E-mail: awaris@fi.itb.ac.id; Kurniadi, R., E-mail: awaris@fi.itb.ac.id; Su' ud, Z., E-mail: awaris@fi.itb.ac.id [Nuclear Physics and Biophysics Research Division, Department of Physics, Faculty of Mathematics and Natural Sciences, Institut Teknologi Bandung, Jl. Ganesa No. 10 Bandung 40132 (Indonesia)

    2014-09-30

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

  7. Radiation Chemistry of Advanced TALSPEAK Flowsheet

    Energy Technology Data Exchange (ETDEWEB)

    Mincher, Bruce; Peterman, Dean; Mcdowell, Rocklan; Olson, Lonnie; Lumetta, Gregg J.

    2013-08-28

    This report summarizes the results of initial experiments designed to understand the radiation chemistry of an Advanced TALSPEAK process for separating trivalent lanthanides form the actinides. Biphasic aerated samples were irradiated and then analyzed for post-irradiation constituent concentrations and solvent extraction distribution ratios. The effects of irradiation on the TALSPEAK and Advanced TALSPEAK solvents were similar, with very little degradation of the organic phase extractant. Decomposition products were detected, with a major product in common for both solvents. This product may be responsible for the slight increase in distribution ratios for Eu and Am with absorbed dose, however; separation factors were not greatly affected.

  8. Bioinorganic Chemistry

    OpenAIRE

    Bertini, Ivano; Gray, Harry B.; Lippard, Stephen J.; Valentine, Joan Selverstone

    1994-01-01

    This book covers material that could be included in a one-quarter or one-semester course in bioinorganic chemistry for graduate students and advanced undergraduate students in chemistry or biochemistry. We believe that such a course should provide students with the background required to follow the research literature in the field. The topics were chosen to represent those areas of bioinorganic chemistry that are mature enough for textbook presentation. Although each chapter presents material...

  9. Organic chemistry

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2003-08-15

    This book with sixteen chapter explains organic chemistry on linkage isomerism such as alkane, cycloalkane, alkene, aromatic compounds, stereo selective isomerization, aromatic compounds, stereo selective isomerization, organic compounds, stereo selective isomerization, organic halogen compound, alcohol, ether, aldehyde and ketone, carboxylic acid, dicarboxylic acid, fat and detergent, amino, carbohydrate, amino acid and protein, nucleotide and nucleic acid and spectroscopy, a polymer and medical chemistry. Each chapter has introduction structure and characteristic and using of organic chemistry.

  10. Social Chemistry

    OpenAIRE

    Lichtfouse, Eric; Schwarzbauer, Jan; Robert, Didier

    2012-01-01

    International audience This article is both an essay to propose social chemistry as a new scientific discipline, and a preface of the book Environmental Chemistry for a Sustainable World. Environmental chemistry is a fast emerging discipline aiming at the understanding the fate of pollutants in ecosystems and at designing novel processes that are safe for ecosystems. Past pollution should be cleaned, future pollution should be predicted and avoided (Lichtfouse et al., 2005a). Such advices ...

  11. Computational chemistry

    OpenAIRE

    Truhlar, Donald G.; McKoy, Vincent

    2000-01-01

    Computational chemistry has come of age. With significant strides in computer hardware and software over the last few decades, computational chemistry has achieved full partnership with theory and experiment as a tool for understanding and predicting the behavior of a broad range of chemical, physical, and biological phenomena. The Nobel Prize award to John Pople and Walter Kohn in 1998 highlighted the importance of these advances in computational chemistry. With massively parallel computers ...

  12. Recent developments in out-of-plane metallocorrole chemistry across the periodic table.

    Science.gov (United States)

    Buckley, Heather L; Arnold, John

    2015-01-01

    This article presents a brief review of recent developments in metallocorrole chemistry, with a focus on species with significant displacement of the metal from the N4 plane of the corrole ring. Comparisons based on X-ray crystallographic data are made between a range of early and/or heavy transition metal, lanthanide, actinide, and main group metallocorrole species. PMID:25321078

  13. Discussion meeting on nuclear-, radio- and radiation chemistry - basics and applications

    International Nuclear Information System (INIS)

    The following fields have been represented at this meeting: 1. nuclear reactions and properties of the formed products; 2. geo- and cosmochemistry; 3. chemistry of actinides and other radioisotopes; 4. radioanalysis; 5. isotope applications; 6. nuclear fuel cycle. Single papers are listed under appropriate categories. (RB)

  14. Complex formation of the lanthanides and actinides in lower oxidation states

    International Nuclear Information System (INIS)

    The coordination chemistry of the lanthanides (ln) and actinides (An) in lower oxidation states is discussed, including the hydration-solvation properties of Ln2+ and An2+ in aqueous and aqueous-ethanolic solutions and the formation of complexes with the tetraphenylborate ion and crown ethers. Some physicochemical properties of a number of novel compounds with crown ethers are reported. In this paper the difference in the properties of Ln2+ and An2+ with an fnd0 and fn-1d1 configuration and the ability of the fn-1 d1 compounds to form mixed condensed clusters with Gd2Cl3 are discussed. The properties of Ln and An elements in various oxidation states are compared with those of elements of other groups in the periodic table

  15. Isotope and Nuclear Chemistry Division annual report FY 1986, October 1985-September 1986

    International Nuclear Information System (INIS)

    This report describes progress in the major research and development programs carried out in FY 1986 by the Isotope and Nuclear Chemistry Division. The report includes articles on radiochemical diagnostics and weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production and separation; chemical biology and nuclear medicine; element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced concepts and technology; and atmospheric chemistry

  16. Isotope and Nuclear Chemistry Division annual report FY 1985, October 1984-September 1985

    International Nuclear Information System (INIS)

    This report describes progress in the major research and development programs carried out in FY 1985 by the Isotope and Nuclear Chemistry Division. It covers radiochemical diagnostics of weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production, separation, and applications (including biomedical applications); element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiations facilities; advanced analytical techniques; development and applications; atmospheric chemistry and transport; and earth and planetary processes

  17. Isotope and Nuclear Chemistry Division annual report FY 1986, October 1985-September 1986

    Energy Technology Data Exchange (ETDEWEB)

    Heiken, J.H. (ed.)

    1987-06-01

    This report describes progress in the major research and development programs carried out in FY 1986 by the Isotope and Nuclear Chemistry Division. The report includes articles on radiochemical diagnostics and weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production and separation; chemical biology and nuclear medicine; element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced concepts and technology; and atmospheric chemistry.

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

    International Nuclear Information System (INIS)

    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-NH2 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 UO22+. (author)

  19. Actinide production in 136Xe bombardments of 249Cf

    International Nuclear Information System (INIS)

    The production cross sections for the actinide products from 136Xe bombardments of 249Cf 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 136Xe + 249Cf bombardments are compared with the production cross section distributions from other heavy ion bombardments of actinide targets, with emphasis on the comparison with the 136Xe + 248Cm 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

  20. Actinides in irradiated graphite of RBMK-1500 reactor

    International Nuclear Information System (INIS)

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

  1. Actinides in irradiated graphite of RBMK-1500 reactor

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-10-01

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

  2. Good chemistry

    OpenAIRE

    Petsko, Gregory A

    2004-01-01

    The subject matter in chemistry courses reflects almost nothing of the issues that chemists are interested in. It is important to formulate a set of topics - and a Medical College Admissions Test reflecting them - that would leave chemistry departments no choice but to change their teaching.

  3. Studies on Neutron, Photon (Bremsstrahlung and Proton Induced Fission of Actinides and Pre-Actinides

    Directory of Open Access Journals (Sweden)

    H. Naik

    2015-08-01

    Full Text Available We present the yields of various fission products determined in the reactor neutron, 3.7-18.1 MeV quasi-mono energetic neutron, 8-80 MeV bremsstrahlung and 20-45 MeV proton induced fission of 232Th and 238U using radiochemical and off-line beta or gamma ray counting. The yields of the fission products in the bremsstrahlung induced fission natPb and 209Bi with 50- 70 MeV and 2.5 GeV based on off-line gamma ray spectrometric technique were also presented. From the yields of fission products, the mass chains yields were obtained using charge distribution correction. From the mass yield distribution, the peak-to-valley (P/V ratio was obtained. The role of excitation energy on the peak-to-valley ratio and fine structure such as effect of shell closure proximity and even-odd effect of mass yield distribution were examined. The higher yields of the fission products around A=133-134, 138-140 and 143-144 and their complementary products explained from the nuclear structure effect and role of standard I and II mode of asymmetric fission. In the neutron, photon (bremsstrahlung and proton induced fission, the asymmetric mass distribution for actinides (Th, U and symmetric distribution for pre-actinides (Pb, Bi were explained from different type of potential fission barrier

  4. Photofission of actinide and pre-actinide nuclei in the quasideuteron and delta energy regions

    CERN Document Server

    Berman, B L; Cole, P L; Dodge, W R; Feldman, G; Sanabria, J C; Kolb, N; Pywell, R E; Vogt, J; Nedorezov, V; Sudov, A; Kezerashvili, G Ya

    1999-01-01

    The photofission cross sections for the actinide nuclei sup 2 sup 3 sup 2 Th, sup 2 sup 3 sup 3 sup , sup 2 sup 3 sup 5 sup , sup 2 sup 3 sup 8 U, and sup 2 sup 3 sup 7 Np have been measured from 68 to 264 MeV and those for the pre-actinide nuclei sup 1 sup 9 sup 7 Au and sup N sup A sup T Pb from 122 to 222 MeV at the Saskatchewan Accelerator Laboratory, using monoenergetic tagged photons and novel parallel-plate avalanche detectors for the fission fragments. The aim of the experiment was to obtain a comprehensive and self-consistent data set and to investigate previous anomalous results in this energy region. The fission probability for transuranic nuclei is expected to be close to unity here. However, important discrepancies have been confirmed for sup 2 sup 3 sup 7 Np and sup 2 sup 3 sup 2 Th, compared with sup 2 sup 3 sup 8 U, which have serious implications for the inferred total photoabsorption strengths, and hence call into question the 'Universal Curve' for photon absorption at these energies. High-s...

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

    Energy Technology Data Exchange (ETDEWEB)

    Johansson, Boerje [Condensed Matter Theory Group, Department of Physics, Uppsala University, Box 530, S-751 21 Uppsala (Sweden); Applied Materials Physics, Department of Materials Science and Engineering, Royal Institute of Technology, Brinellvaegen 23, SE-100 44 Stockholm (Sweden)], E-mail: borje.johansson@fysik.uu.se; Li, Sa [Applied Materials Physics, Department of Materials Science and Engineering, Royal Institute of Technology, Brinellvaegen 23, SE-100 44 Stockholm (Sweden); Department of Physics, Virginia Commonwealth University, Richmond, VA 23284 (United States)

    2007-10-11

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

  6. Rapid determination of alpha emitters using Actinide resin.

    Science.gov (United States)

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

    2004-01-01

    The European Commission has recently published the recommended radiological protection criteria for the clearance of building and building rubble from the dismantling of nuclear installations. Radionuclide specific clearance levels for actinides are very low (between 0.1 and 1 Bq g(-1)). The prevalence of natural radionuclides in rubble materials makes the verification of these levels by direct alpha counting impossible. The capability of Actinide resin (Eichrom Industries, Inc.) for extracting plutonium and americium from rubble samples has been tested in this work. Besides a strong affinity for actinides in the tri, tetra and hexavalent oxidation states, this extraction chromatographic resin presents an easy recovery of absorbed radionuclides. The retention capability was evaluated on rubble samples spiked with certified radionuclide standards (239Pu and 241Am). Samples were leached with nitric acid, passed through a chromatographic column containing the resin and the elution fraction was measured by LSC. Actinide retention varies from 60% to 80%. Based on these results, a rapid method for the verification of clearance levels for actinides in rubble samples is proposed. PMID:15177360

  7. 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.

  8. Separation of actinides and long-lived fission products from high-level radioactive wastes (a review)

    International Nuclear Information System (INIS)

    The management of high-level radioactive wastes is facilitated, if long-lived and radiotoxic actinides and fission products are separated before the final disposal. Especially important is the separation of americium, curium, plutonium, neptunium, strontium, cesium and technetium. The separated nuclides can be deposited separately from the bulk of the high-level waste, but their transmutation to short-lived nuclides is a muchmore favourable option. This report reviews the chemistry of the separation of actinides and fission products from radioactive wastes. The composition, nature and conditioning of the wastes are described. The main attention is paid to the solvent extraction chemistry of the elements and to the application of solvent extraction in unit operations of potential partitioning processes. Also reviewed is the behaviour of the elements in the ion exchange chromatography, precipitation, electrolysis from aqueous solutions and melts, and the distribution between molten salts and metals. Flowsheets of selected partitioning processes are shown and general aspects of the waste partitioning are shortly discussed. (orig.)

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

    International Nuclear Information System (INIS)

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

  10. Quantum chemistry

    CERN Document Server

    Lowe, John P

    1993-01-01

    Praised for its appealing writing style and clear pedagogy, Lowe's Quantum Chemistry is now available in its Second Edition as a text for senior undergraduate- and graduate-level chemistry students. The book assumes little mathematical or physical sophistication and emphasizes an understanding of the techniques and results of quantum chemistry, thus enabling students to comprehend much of the current chemical literature in which quantum chemical methods or concepts are used as tools. The book begins with a six-chapter introduction of standard one-dimensional systems, the hydrogen atom,

  11. Prompt Fission Neutron Spectra of Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Capote, R; Chen, Y J; Hambsch, F J; Kornilov, N V; Lestone, J P; Litaize, O; Morillon, B; Neudecker, D; Oberstedt, S; Ohsawa, T; Smith, D. L.

    2016-01-01

    The energy spectrum of prompt neutrons emitted in fission (PFNS) plays a very important role in nuclear science and technology. A Coordinated Research Project (CRP) “Evaluation of Prompt Fission Neutron Spectra of Actinides”was established by the IAEA Nuclear Data Section in 2009, with the major goal to produce new PFNS evaluations with uncertainties for actinide nuclei. The following technical areas were addressed: (i) experiments and uncertainty quantification (UQ): New data for neutron-induced fission of 233U, 235U, 238U, and 239Pu have been measured, and older data have been compiled and reassessed. There is evidence from the experimental work of this CRP that a very small percentage of neutrons emitted in fission are actually scission neutrons; (ii) modeling: The Los Alamos model (LAM) continues to be the workhorse for PFNS evaluations. Monte Carlo models have been developed that describe the fission phenomena microscopically, but further development is needed to produce PFNS evaluations meeting the uncertainty targets; (iii) evaluation methodologies: PFNS evaluations rely on the use of the least-squares techniques for merging experimental and model data. Considerable insight was achieved on how to deal with the problem of too small uncertainties in PFNS evaluations. The importance of considering that all experimental PFNS data are “shape” data was stressed; (iv) PFNS evaluations: New evaluations, including covariance data, were generated for major actinides including 1) non-model GMA evaluations of the 235U(nth,f), 239Pu(nth,f), and 233U(nth,f) PFNS based exclusively on experimental data (0.02 ≤ E ≤ 10 MeV), which resulted in PFNS average energies E of 2.00±0.01, 2.073±0.010, and 2.030±0.013 MeV, respectively; 2) LAM evaluations of neutron-induced fission spectra on uranium and plutonium targets with improved UQ for incident energies from thermal up to 30 MeV; and 3) Point-by-Point calculations for 232Th, 234U and 237Np targets; and (v) data

  12. Actinide consumption: Nuclear resource conservation without breeding

    Energy Technology Data Exchange (ETDEWEB)

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

    1991-01-01

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

  13. Actinide consumption: Nuclear resource conservation without breeding

    International Nuclear Information System (INIS)

    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

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

    International Nuclear Information System (INIS)

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

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

    International Nuclear Information System (INIS)

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

  16. Fluoride-conversion synthesis of homogeneous actinide oxide solid solutions

    Energy Technology Data Exchange (ETDEWEB)

    Silva, G W Chinthaka M [ORNL; Hunn, John D [ORNL; Yeamans, Charles B. [University of California, Berkeley; Cerefice, Gary S. [University of Nevada, Las Vegas; Czerwinski, Ken R. [University of Nevada, Las Vegas

    2011-01-01

    Here, a novel route to synthesize (U, Th)O2 solid solutions at a relatively low temperature of 1100 C is demonstrated. First, the separate actinide oxides reacted with ammonium bifluoride to form ammonium actinide fluorides at room temperature. Subsequently, this mixture was converted to the actinide oxide solid solution using a two-phased heat treatment, first at 610 C in static air, then at 1100 C in flowing argon. Solid solutions obeying Vegard s Law were synthesized for ThO2 content from 10 to 90 wt%. Microscopy showed that the (U, Th)O2 solid solutions synthesized with this method to have considerably high crystallinity and homogeneity, suggesting the suitability of material thus synthesized for sintering into nuclear fuel pellets at low temperatures.

  17. Actinide (III) solubility in WIPP Brine: data summary and recommendations

    Energy Technology Data Exchange (ETDEWEB)

    Borkowski, Marian; Lucchini, Jean-Francois; Richmann, Michael K.; Reed, Donald T.

    2009-09-01

    The solubility of actinides in the +3 oxidation state is an important input into the Waste Isolation Pilot Plant (WIPP) performance assessment (PA) models that calculate potential actinide release from the WIPP repository. In this context, the solubility of neodymium(III) was determined as a function of pH, carbonate concentration, and WIPP brine composition. Additionally, we conducted a literature review on the solubility of +3 actinides under WIPP-related conditions. Neodymium(III) was used as a redox-invariant analog for the +3 oxidation state of americium and plutonium, which is the oxidation state that accounts for over 90% of the potential release from the WIPP through the dissolved brine release (DBR) mechanism, based on current WIPP performance assessment assumptions. These solubility data extend past studies to brine compositions that are more WIPP-relevant and cover a broader range of experimental conditions than past studies.

  18. Laser resonant-ionization mass spectrometry of actinides

    International Nuclear Information System (INIS)

    Laser resonant-ionization mass spectrometry has been used to determine small amounts of actinides. The high sensitivity and selectivity of this method has been achieved by three-step photoionization of actinide atoms followed by time-of-flight measurement. The laser system for photoionization consists of a pulsed copper vapour laser of 30 W average power at a pulse repetition rate of 6.5 kHz which is coupled to three dye lasers. The time-of-flight spectrometer has a mass resolution of about 2500. Resonance signals with count rates of several kilohertz were obtained with actinide samples of 1010-1012 atoms yielding a detection limit of 108 atoms in the sample. With some improvements a detection sensitivity of about 106 atoms of plutonium, americium and curium should be reached. (orig.)

  19. Synthesis of selective extractor for minor actinide elements

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Jong Seung [Konyang University, Nonsan (Korea); Cho, Moon Hwan [Kangwon National University, Chunchon (Korea)

    1998-04-01

    To selectively co-separate the lanthanide and actinide elements (MA) such as Am or Cm ion from radioactive waste, synthesis of diamide derivatives has been accomplished. In addition, picoline amide derivatives were also synthesized for selectively separate the minor actinide elements from lanthanide elements. The content of research has don are as follows: (1) synthesis of diamide as co-extractant (2) introduction of n-tetradecyl to increase the lipophilicity (3) Picolyl chloride, intermediate of the final product, was synthesized by improved method rather than reported method. (4) The length of alkyl side chain was adjusted to increase the lipophilicity of free ligand and its derivatives able to selectively separate the actinide metal from lanthanide metal ions was successfully synthesized and determined their purity by analytical instruments. (author). 12 refs., 28 figs.

  20. Materials Chemistry

    CERN Document Server

    Fahlman, Bradley D

    2011-01-01

    The 2nd edition of Materials Chemistry builds on the strengths that were recognized by a 2008 Textbook Excellence Award from the Text and Academic Authors Association (TAA). Materials Chemistry addresses inorganic-, organic-, and nano-based materials from a structure vs. property treatment, providing a suitable breadth and depth coverage of the rapidly evolving materials field. The 2nd edition continues to offer innovative coverage and practical perspective throughout. After briefly defining materials chemistry and its history, seven chapters discuss solid-state chemistry, metals, semiconducting materials, organic "soft" materials, nanomaterials, and materials characterization. All chapters have been thoroughly updated and expanded with, for example, new sections on ‘soft lithographic’ patterning, ‘click chemistry’ polymerization, nanotoxicity, graphene, as well as many biomaterials applications. The polymer and ‘soft’ materials chapter represents the largest expansion for the 2nd edition. Each ch...

  1. Introductory Chemistry

    OpenAIRE

    Baron, Mark; Gonzalez-Rodriguez, Jose; Stevens, Gary; Gray, Nathan; Atherton, Thomas; Winn, Joss

    2010-01-01

    Teaching and Learning resources for the 1st Year Introductory Chemistry course (Forensic Science). 30 credits. These are Open Educational Resources (OER), made available for re-use under a Creative Commons license.

  2. Sequential determination of actinides in a variety of matrices

    International Nuclear Information System (INIS)

    A large number of analytical procedures for the actinides have been published, each catering for a specific need. Due to the bioassay programme in our laboratory, a need arose for a method to determine natural (Th and U) and anthropogenic actinides (Np, Pu and Am/Cm) together in a variety of samples. The method would have to be suitable for routine application: simple, inexpensive, rapid and robust. In some cases, the amount of material available is not sufficient for the determination of separate groups of actinides, and a sequential separation and measurement of the analytes would therefore be required. The types of matrices vary from aqueous samples to radiological surveillance (urine and faeces) to environmental studies (soil, sediment and fish), but the separation procedure should be able to service all of these. The working range of the method would have to cater for lower levels of the transuranium actinides in particular sample types containing higher levels of the natural actinides (U and Th). The first analytical problem to be discussed, is how to get the different sample types into the same loading solution required by a single separation approach. This entails sample dissolution or decomposition in some cases, and pre-concentration or pre-separation in others. A separation scheme is presented for the clean separation of all the actinides in a form suitable for alpha spectrometry. The development of a single column separation of the analytes of interest are looked at, as well as observations made during the development of the separation scheme, such as concentration effects. Results for test samples and certified reference materials are be presented. (author)

  3. 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.

  4. Analytical chemistry

    International Nuclear Information System (INIS)

    This book is comprised of nineteen chapters, which describes introduction of analytical chemistry, experimental error and statistics, chemistry equilibrium and solubility, gravimetric analysis with mechanism of precipitation, range and calculation of the result, volume analysis on general principle, sedimentation method on types and titration curve, acid base balance, acid base titration curve, complex and firing reaction, introduction of chemical electro analysis, acid-base titration curve, electrode and potentiometry, electrolysis and conductometry, voltammetry and polarographic spectrophotometry, atomic spectrometry, solvent extraction, chromatograph and experiments.

  5. Green Chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Collison, Melanie

    2011-05-15

    Green chemistry is the science of chemistry used in a way that will not use or create hazardous substances. Dr. Rui Resendes is working in this field at GreenCentre Canada, an offshoot of PARTEQ Innovations in Kingston, Ontario. GreenCentre's preliminary findings suggest their licensed product {sup S}witchable Solutions{sup ,} featuring 3 classes of solvents and a surfactant, may be useful in bitumen oil sands extraction.

  6. Cluster Chemistry

    Institute of Scientific and Technical Information of China (English)

    2011-01-01

    @@ Cansisting of eight scientists from the State Key Laboratory of Physical Chemistry of Solid Surfaces and Xiamen University, this creative research group is devoted to the research of cluster chemistry and creation of nanomaterials.After three-year hard work, the group scored a series of encouraging progresses in synthesis of clusters with special structures, including novel fullerenes, fullerene-like metal cluster compounds as well as other related nanomaterials, and their properties study.

  7. Analogue Study of Actinide Transport at Sites in Russia

    Energy Technology Data Exchange (ETDEWEB)

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

    2003-02-12

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

  8. Thermally unstable complexants/phosphate mineralization of actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    1996-10-01

    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. INERT-MATRIX FUEL: ACTINIDE ''BURNING'' AND DIRECT DISPOSAL

    International Nuclear Information System (INIS)

    Excess actinides result from the dismantlement of nuclear weapons (Pu) and the reprocessing of commercial spent nuclear fuel (mainly 241 Am, 244 Cm and 237 Np). In Europe, Canada and Japan studies have determined much improved efficiencies for burnup of actinides using inert-matrix fuels. This innovative approach also considers the properties of the inert-matrix fuel as a nuclear waste form for direct disposal after one-cycle of burn-up. Direct disposal can considerably reduce cost, processing requirements, and radiation exposure to workers

  10. Production of heavy actinides in incomplete fusion reactions

    Science.gov (United States)

    Antonenko, N. V.; Cherepanov, E. A.; Iljinov, A. S.; Mebel, M. V.

    1994-10-01

    We present preliminary results of calculations by the phenomenological model of the estimated yield of some heavy actinide isotopes. It is assumed that these isotopes are produced as a result of multinucleon transfers followed by neutrons and charged particle emission A.S. Iljinov and E.A. Cherepanov (1980). The yield P(sub Z, N)(E*) of primary excited actinides is found using the model of N.V. Antonenko and R.V. Jolos (1991). Absolute cross-sections for different binary reaction channels are obtained by summing the cross-sections for all subchannels with an appreciable yield according to J. Wilczynski et al. (1980).

  11. In vivo measurement of actinides in the human lung

    International Nuclear Information System (INIS)

    The problems associated with the in vivo detection and measurement of actinides in the human lung are discussed together with various measurement systems currently in use. In particular, the methods and calibration procedures employed at the Lawrence Livermore Laboratory, namely, the use of twin Phoswich detectors and a new, more realistic, tissue-equivalent phantom, are described. Methods for the measurement of chest-wall thickness, fat content, and normal human background counts are also discussed. Detection-efficiency values and minimum detectable activity estimates are given for three common actinides, 238Pu, 239Pu, and 241Am

  12. Physics studies of higher actinide consumption in an LMR

    Energy Technology Data Exchange (ETDEWEB)

    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.

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

    Science.gov (United States)

    Geckeis, Horst; Rabung, Thomas

    2008-12-12

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

  14. Fuel Chemistry Division: progress report for 1985

    International Nuclear Information System (INIS)

    Fuel Chemistry Division was formed in May 1985 to give a larger emphasis on the research and development in chemistry of the nuclear fuel cycle. The areas of research in Fuel Chemistry Division are fuel development and its chemical quality control, understanding of the fuel behaviour and post irradiation examinations, chemistry of reprocessing and waste management processes as also the basic aspects of actinide and relevant fission product elements. This report summarises the work by the staff of the Division during 1985 and also some work from the previous periods which was not reported in the progress reports of the Radiochemistry Division. The work related to the FBTR fuel was one of the highlights during this period. In the area of process chemistry useful work has been carried out for processing of plutonium bearing solutions. In the area of mass spectrometry, the determination of trace constituents by spark source mass spectrometry has been a major area of research. Significant progress has also been made in the use of alpha spectromet ry techniques for the determination of plutonium in dissolver solution and other samples. The technology of plutonium utilisation is quite complex and the Division would continue to look into the chemical aspects of this technology and provide the necessary base for future developments in this area. (author)

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

    Indian Academy of Sciences (India)

    R Tripathi; S Sodaye; K Sudarshan

    2015-08-01

    In this article, some of our recent results on fission fragment/product angular distributions are discussed in the context of non-compound nucleus fission. Measurement of fission fragment angular distribution in 28Si+176Yb reaction did not show a large contribution from the non-compound nucleus fission. 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 showed an increase in angular anisotropy with decreasing asymmetry of mass division. This observation can be explained based on the contribution from pre-equilibrium fission. Results of these studies showed that the mass dependence of anisotropy may possibly be used to distinguish pre-equilibrium fission and quasifission.

  16. Advanced Recycling Reactor with Minor Actinide Fuel

    International Nuclear Information System (INIS)

    The Advanced Recycling Reactor (ARR) with minor actinide fuel has been studied. This paper presents the pre-conceptual design of the ARR proposed by the International Nuclear Recycling Alliance (INRA) for FOA study sponsored by DOE of the United States of America (U.S.). Although the basic reactor concept is technically mature, it is not suitable for commercial use due to the need to reduce capital costs. As a result of INRA's extensive experience, it is anticipated that a non-commercial ARR1 will be viable and meet U.S. requirements by 2025. Commercial Advanced Recycling Reactor (ARR) operations are expected to be feasible in competition with LWRs by 2050, based on construction of ARR2 in 2035. The ARR based on the Japan Sodium-cooled Fast Reactor (JSFR) is a loop-typed sodium cooled reactor with MOX fuel that is selected because of much experience of SFRs in the world. Major features of key technology enhancements incorporated into the ARR are the following: Decay heat can be removed by natural circulation to improve safety. The primary cooling system consists of two-loop system and the integrated IHX/Pump to improve economics. The steam generator with the straight double-walled tube is used to improve reliability. The reactor core of the ARR1 is 70 cm high and the volume fraction of fuel is 31.6%. The conversion ratio of fissile is set up less than 0.65 and the amount of burned TRU is 45-51 kg/TWeh. According to survey of more effective TRU burning core, the oxide fuel core containing high TRU (MA 15%, Pu 35% average) with moderate pins of 12% arranged driver fuel assemblies can decrease TRU conversion ratio to 0.33 and improve TRU burning capability to 67 kg/TWeh. The moderator can enhance TRU burning, while increasing the Doppler effect and reducing the positive sodium void effect. High TRU fraction promotes TRU burning by curbing plutonium production. High Am fraction and Am blanket promote Am transmutation. The ARR1 consists of a reactor building (including

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

    Energy Technology Data Exchange (ETDEWEB)

    Rudisill, T.; Kyser, E.

    2010-09-02

    One objective of the US Department of Energy's Office of Nuclear Energy (DOE-NE) is the development of sustainable nuclear fuel cycles which improve uranium resource utilization, maximize energy generation, minimize waste generation, improve safety, and complement institutional measures limiting proliferation risks. Activities in progress which support this objective include the development of advanced separation technologies to recover the actinides from used nuclear fuels. With the increased interest in the development of technology to allow closure of the nuclear fuel cycle, the TALSPEAK process is being considered for the separation of Am and Cm from the lanthanide fission products in a next generation reprocessing plant. However, at this time, the level of understanding associated with the chemistry and the control of the process variables is not acceptable for deployment of the process on an industrial scale. To address this issue, DOE-NE is supporting basic scientific studies focused on the TALSPEAK process through its Fuel Cycle Research and Development (R&D) program. One aspect of these studies is an experimental program at the Savannah River National Laboratory (SRNL) in which temperature-dependent distribution coefficients for the extraction of actinide elements in the TALSPEAK process were measured. The data were subsequently used to calculate conditional enthalpies and entropies of extraction by van't Hoff analysis to better understand the thermodynamic driving forces for the TALSPEAK process. In the SRNL studies, the distribution of Pu(III) in the TALSPEAK process was of particular interest. A small amount of Pu(III) would be present in the feed due to process losses and valence adjustment in prior recovery operations. Actinide elements such as Np and Pu have multiple stable oxidation states in aqueous solutions; therefore the oxidation state for these elements must be controlled in the TALSPEAK process, as the extraction chemistry is

  18. Radiation Chemistry

    Science.gov (United States)

    Wojnárovits, L.

    Ionizing radiation causes chemical changes in the molecules of the interacting medium. The initial molecules change to new molecules, resulting in changes of the physical, chemical, and eventually biological properties of the material. For instance, water decomposes to its elements H2 and O2. In polymers, degradation and crosslinking take place. In biopolymers, e.g., DNS strand breaks and other alterations occur. Such changes are to be avoided in some cases (radiation protection), however, in other cases they are used for technological purposes (radiation processing). This chapter introduces radiation chemistry by discussing the sources of ionizing radiation (radionuclide sources, machine sources), absorption of radiation energy, techniques used in radiation chemistry research, and methods of absorbed energy (absorbed dose) measurements. Radiation chemistry of different classes of inorganic (water and aqueous solutions, inorganic solids, ionic liquids (ILs)) and organic substances (hydrocarbons, halogenated compounds, polymers, and biomolecules) is discussed in concise form together with theoretical and experimental backgrounds. An essential part of the chapter is the introduction of radiation processing technologies in the fields of polymer chemistry, food processing, and sterilization. The application of radiation chemistry to nuclear technology and to protection of environment (flue gas treatment, wastewater treatment) is also discussed.

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

    Energy Technology Data Exchange (ETDEWEB)

    Kenneth L. Nash

    2009-09-22

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

  20. Conception, synthesis and application of tripodands in actinide/lanthanide separation

    International Nuclear Information System (INIS)

    The purpose of this work is the synthesis of C, H, O and N containing compounds able to separate '4f' and '5f' elements by liquid/liquid extraction. In a first part, the literature's study allow us to point out actinide and lanthanide ions actual nature and the different ways offered by organic chemistry to share two metallic ions between two liquid phases. On one hand, these trivalent cations' high coordination numbers drive us to synthesize tripodands with hard sites which were fitted for complexation. On the other hand, it appeared that carboxylate or even less-hard site like pyridine chelate selectively actinides, allowing separation. In a second part, 60 ligands were synthesized. In each of the ligands families, a structural parameter changes (site nature, distance between two neighbouring sites, sites respective orientation, lipophilicity and rigidity). 2,2-dihydroxymethyl-dodecanol and 1,3,5- tri(chlorocarbonyl) benzene were chosen as core. O-alkylation and amidation reactions were also peculiarly studied. Rekker's proceeding for lipophilicity calculation was used in order to establish a structure-activity relationship. In a third part, extraction assays with radioactive effluents (152Eu and 241Am) point out extraction and separation abilities of our compounds. Different operating ways were used according as ligand is soluble in aqueous or organic phase. Organic phase-soluble compounds were compared to DcH18C6, pyridine ones to 2,4,6-tri(2-pyridyl)-l,3,5-triazine (TPTZ) and carboxylate ones to diethylenetriamine-tetracetic acid (DTPA, Talspeak proceeding). The third phase phenomenon was encountered and studied. Influence of salt, pH and organic phase were also studied. (author)

  1. The advanced liquid metal reactor actinide recycle system

    International Nuclear Information System (INIS)

    The current U.S. National Energy Strategy includes four key goals for nuclear policy: enhance safety and design standards, reduce economic risk, reduce regulatory risk, and establish an effective high-level nuclear waste program. The U.S. Department of Energy's Advanced Liquid Metal Reactor Actinide Recycle System is consistent with these objectives. The system has the ability to fulfill multiple missions with the same basic design concept. In addition to providing an option for long-term energy security, the system can be effectively utilized for recycling of actinides in light water reactor (LWR) spent fuel, provide waste management flexibility, including the reduction in the waste quantity and storage time and utilization of the available energy potential of LWR spent fuel. The actinide recycle system is comprised of (1) a compact liquid metal (sodium) cooled reactor system with optimized passive safety characteristics, and (2) pyrometallurgical metal fuel cycle presently under development of Argonne National Laboratory. The waste reduction of LWR spent fuel is accomplished by transmutation or fissioning of the longer-lived transuranic isotopes to shorter-lived fission products in the reactor. In this presentation the economical and environmental incentive of the actinide recycle system is addressed and the status of development including licensing aspects is described. 3 refs., 1 tab., 6 figs

  2. Reversible optical sensor for the analysis of actinides in solution

    International Nuclear Information System (INIS)

    In this work is presented a concept of reversible optical sensor for actinides. It is composed of a p doped conducing polymer support and of an anion complexing the actinides. The chosen conducing polymer is the thiophene-2,5-di-alkoxy-benzene whose solubility and conductivity are perfectly known. The actinides selective ligand is a lacunar poly-oxo-metallate such as P2W17O6110- or SiW11O398- which are strong anionic complexing agents of actinides at the oxidation state (IV) even in a very acid medium. The sensor is prepared by spin coating of the composite mixture 'polymer + ligand' on a conducing glass electrode and then tested towards its optical and electrochemical answer in presence of uranium (IV). The absorption change due to the formation of cations complexes by poly-oxo-metallate reveals the presence of uranium (IV). After the measurement, the sensor is regenerated by anodic polarization of the support and oxidation of the uranium (IV) into uranium (VI) which weakly interacts with the poly-oxo-metallate and is then released in solution. (O.M.)

  3. Program and presentations of the 33th Actinide Days

    International Nuclear Information System (INIS)

    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.)

  4. Preparation of actinide targets and sources using nonaqueous electrodeposition

    Energy Technology Data Exchange (ETDEWEB)

    Fowler, M.M.; Gursky, J.C.; Wilhelmy, J.B. (Los Alamos National Lab., NM (USA))

    1991-05-15

    Application of the method of 'molecular plating' to prepare actinide targets suitable for accelerator bombardment is presented. Two example applications involving {sup 229}Th and {sup 254}Es are discussed along with the merits and liabilities of the method. (orig.).

  5. Actinide Biocolloid Formation in Brine by Halophilic Bacteria

    International Nuclear Information System (INIS)

    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

  6. 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 whi...

  7. 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...

  8. 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.

  9. RAPID SEPARATION OF ACTINIDES AND RADIOSTRONTIUM IN VEGETATION SAMPLES

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.

    2010-06-01

    A new rapid method for the determination of actinides and radiostrontium in vegetation samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used in emergency response situations or for routine analysis. The actinides in vegetation method utilizes a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a streamlined column separation process with stacked TEVA, TRU and DGA Resin cartridges. Lanthanum was separated rapidly and effectively from Am and Cm on DGA Resin. Alpha emitters are prepared using rare earth microprecipitation for counting by alpha spectrometry. The purified {sup 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. The actinide and {sup 90}Sr in vegetation sample analysis can be performed in less than 8 h with excellent quality for emergency samples. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory actinide particles or vegetation residue after furnace heating is effectively digested.

  10. Functionalized pyrazines as ligands for minor actinide extraction and catalysis

    NARCIS (Netherlands)

    Nikishkin, N.

    2013-01-01

    The research presented in this thesis concerns the design of ligands for a wide range of applications, from nuclear waste treatment to catalysis. The strategies employed to design actinide-selective extractants, for instance, comprise the fine tuning of the ligand electronic properties as well as us

  11. Actinides How well do we know their stellar production?

    CERN Document Server

    Goriely, S

    2001-01-01

    The reliable evaluation of the r-process production of the actinides and careful estimates of the uncertainties affecting these predictions are key ingredients especially in nucleo-cosmochronology studies based on the analysis of very metal-poor stars or on the composition of meteorites. This type of information is also required in order to make the best possible use of future high precision data on the actinide composition of galactic cosmic rays, of the local interstellar medium, or of meteoritic grains of presumed circumstellar origin. This paper provides the practitioners in these various fields with the most detailed and careful analysis of the r-process actinide production available to-date. In total, thirty-two different multi-event canonical calculations using different nuclear ingredients or astrophysics conditions are presented, and are considered to give a fair picture of the level of reliability of the predictions of the actinide production, at least in the framework of a simple r-process model. T...

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

    International Nuclear Information System (INIS)

    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

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

    International Nuclear Information System (INIS)

    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 SFLn/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

  14. Assessment of Partitioning Processes for Transmutation of Actinides

    International Nuclear Information System (INIS)

    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

  15. 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

  16. Polymer Chemistry

    Science.gov (United States)

    Williams, Martha; Roberson, Luke; Caraccio, Anne

    2010-01-01

    This viewgraph presentation describes new technologies in polymer and material chemistry that benefits NASA programs and missions. The topics include: 1) What are Polymers?; 2) History of Polymer Chemistry; 3) Composites/Materials Development at KSC; 4) Why Wiring; 5) Next Generation Wiring Materials; 6) Wire System Materials and Integration; 7) Self-Healing Wire Repair; 8) Smart Wiring Summary; 9) Fire and Polymers; 10) Aerogel Technology; 11) Aerogel Composites; 12) Aerogels for Oil Remediation; 13) KSC's Solution; 14) Chemochromic Hydrogen Sensors; 15) STS-130 and 131 Operations; 16) HyperPigment; 17) Antimicrobial Materials; 18) Conductive Inks Formulations for Multiple Applications; and 19) Testing and Processing Equipment.

  17. Quantum chemistry

    CERN Document Server

    Lowe, John P

    2006-01-01

    Lowe's new edition assumes little mathematical or physical sophistication and emphasizes an understanding of the techniques and results of quantum chemistry. It can serve as a primary text in quantum chemistry courses, and enables students and researchers to comprehend the current literature. This third edition has been thoroughly updated and includes numerous new exercises to facilitate self-study and solutions to selected exercises.* Assumes little initial mathematical or physical sophistication, developing insights and abilities in the context of actual problems* Provides thorough treatment

  18. Actinide partitioning-transmutation program final report. I. Overall assessment

    International Nuclear Information System (INIS)

    This report is concerned with an overall assessment of the feasibility of and incentives for partitioning (recovering) long-lived nuclides from fuel reprocessing and fuel refabrication plant radioactive wastes and transmuting them to shorter-lived or stable nuclides by neutron irradiation. The principal class of nuclides considered is the actinides, although a brief analysis is given of the partitioning and transmutation (P-T) of 99Tc and 129I. The results obtained in this program permit us to make a comparison of the impacts of waste management with and without actinide recovery and transmutation. Three major conclusions concerning technical feasibility can be drawn from the assessment: (1) actinide P-T is feasible, subject to the acceptability of fuels containing recycle actinides; (2) technetium P-T is feasible if satisfactory partitioning processes can be developed and satisfactory fuels identified (no studies have been made in this area); and (3) iodine P-T is marginally feasible at best because of the low transmutation rates, the high volatility, and the corrosiveness of iodine and iodine compounds. It was concluded on the basis of a very conservative repository risk analysis that there are no safety or cost incentives for actinide P-T. In fact, if nonradiological risks are included, the short-term risks of P-T exceed the long-term benefits integrated over a period of 1 million years. Incentives for technetium and iodine P-T exist only if extremely conservative long-term risk analyses are used. Further RD and D in support of P-T is not warranted

  19. Nuclear chemistry

    International Nuclear Information System (INIS)

    Topics covered include: mass asymmetry and total kinetic energy release in the spontaneous fission of 262105; calculation of spontaneous fission properties of very heavy nuclei - 98 less than or equal to Z less than or equal to 106 and 150 less than or equal to N less than or equal to 164; energy losses for 84Kr ions in nickel, aluminium and titanium; differences in compound nuclei formed with 40Ar and 84Kr projectiles; measurement of the energy division vs. mass in highly damped reactions; ambiguities in the inference of precompound emission from excitation function analysis; selective laser one-atom detection of neutral prompt fission fragments; laser induced nuclear polarization - application to the study of spontaneous fission isomers; quadrupole and hexadecapole deformations in the actinide nuclei; high-spin states in 164Yb; contrasting behavior of h/sub 9/2/ and i/sub 13/2/ bands in 185Au; multiple band crossings in 164Er; recoil-distance measurement of lifetimes of rotational states in 164Dy, lifetimes of ground-band states in 192Pt and 194Pt and application of the rotation-alignment model; coulomb excitation of vibrational nuclei with heavy ions; surface structure of deformed nuclei; valency contribution to neutron capture in 32S; neutron capture cross section of manganese; search for superheavy elements in natural samples by neutron multiplicity counting; and gamma-ray studies on the geochemistry of achondritic meteorites

  20. Thermodynamic study of the complexation of trivalent actinide and lanthanide cations by ADPTZ, a tridentate N-donor ligand.

    Science.gov (United States)

    Miguirditchian, Manuel; Guillaneux, Denis; Guillaumont, Dominique; Moisy, Philippe; Madic, Charles; Jensen, Mark P; Nash, Kenneth L

    2005-03-01

    To better understand the bonding in complexes of f-elements by polydentate N-donor ligands, the complexation of americium(III) and lanthanide(III) cations by 2-amino-4,6-di-(pyridin-2-yl)-1,3,5-triazine (ADPTZ) was studied using a thermodynamic approach. The stability constants of the 1:1 complexes in a methanol/water mixture (75/25 vol %) were determined by UV-visible spectrophotometry for every lanthanide(III) ion (except promethium), and yttrium(III) and americium(III) cations. The thermodynamic parameters (DeltaH degrees , DeltaS degrees) of complexation were determined from the temperature dependence of the stability constants and by microcalorimetry. The trends of the variations of DeltaG degrees , DeltaH degrees , and DeltaS degrees across the lanthanide series are compared with published results for other tridentate ligands and confirm strongly ionic bonding in the lanthanide-ADPTZ complexes. Comparison of the thermodynamic properties between the Am- and Ln-ADPTZ complexes highlights an increase in stability of the complexes by a factor of 20 in favor of the americium cation. This difference arises from a more exothermic reaction enthalpy in the case of Am, which is correlated with a greater degree of covalency in the americium-nitrogen bonds. Quantum chemistry calculations performed on a series of trivalent actinide and lanthanide-ADPTZ complexes support the experimental results, showing a slightly greater covalence in the actinide-ligand bonds that originates from a charge transfer from the ligand sigma orbitals to the 5f and 6d orbitals of the actinide ion. PMID:15732980

  1. Organic chemistry

    International Nuclear Information System (INIS)

    The activities of the mycotoxin research group are discussed. This includes the isolation and structure determination of mycotoxins, plant products, the biosyntheris of mycotoxins, the synthesis and characteristics of steroids, the synthesis and mechanistic aspects of heterocyclic chemistry and the functionality of steroids over long distances. Nmr spectra and mass spectroscopy are some of the techniques used

  2. Reinventing Chemistry

    OpenAIRE

    Whitesides, George McClelland

    2015-01-01

    Chemistry is in a period of change, from an era focused on molecules and reactions, to one in which manipulations of systems of molecules and reactions will be essential parts of controlling larger systems. This Essay traces paths from the past to possible futures.

  3. Predictions For New, Exotic Actinide Species

    International Nuclear Information System (INIS)

    The approach. New, simple chemical species can be predicted by studying isoelectronic series using ab initio quantum chemistry. We currently use in most cases relativistic pseudopotentials and handle the electron correlation using density functional theory (DFT) or wave-function-based methods, from MP2 to CCSD(T). Typical codes are Gaussian 98, Turbomole or MolCas. For full four-component Dirac-Fock calculations, the DREAMS code of K. G. Dyall has been utilized. For mapping out the possible new species, complete maps of all possibilities are made, whenever possible, and the new species typically occur along the coast-line of the 'island of stability' of already known species

  4. Internal contamination by actinides after wounding: a robust rodent model for assessment of local and distant actinide retention.

    Science.gov (United States)

    Griffiths, N M; Wilk, J C; Abram, M C; Renault, D; Chau, Q; Helfer, N; Guichet, C; Van der Meeren, A

    2012-08-01

    Internal contamination by actinides following wounding may occur in nuclear fuel industry workers or subsequent to terrorist activities, causing dissemination of radioactive elements. Contamination by alpha particle emitting actinides can result in pathological effects, either local or distant from the site of entry. The objective of the present study was to develop a robust experimental approach in the rat for short- and long- term actinide contamination following wounding by incision of the skin and muscles of the hind limb. Anesthetized rats were contaminated with Mixed OXide (MOX, uranium, plutonium oxides containing 7.1% plutonium) or plutonium nitrate (Pu nitrate) following wounding by deep incision of the hind leg. Actinide excretion and tissue levels were measured as well as histological changes from 2 h to 3 mo. Humid swabs were used for rapid evaluation of contamination levels and proved to be an initial guide for contamination levels. Although the activity transferred from wound to blood is higher after contamination with a moderately soluble form of plutonium (nitrate), at 7 d most of the MOX (98%) or Pu nitrate (87%) was retained at the wound site. Rapid actinide retention in liver and bone was observed within 24 h, which increased up to 3 mo. After MOX contamination, a more rapid initial urinary excretion of americium was observed compared with plutonium. At 3 mo, around 95% of activity remained at the wound site, and excretion of Pu and Am was extremely low. This experimental approach could be applied to other situations involving contamination following wounding including rupture of the dermal, vascular, and muscle barriers.

  5. Actinides: How well do we know their stellar production?

    Science.gov (United States)

    Goriely, S.; Arnould, M.

    2001-12-01

    The reliable evaluation of the r-process production of the actinides and careful estimates of the uncertainties affecting these predictions are key ingredients especially in nucleo-cosmochronology studies based on the analysis of very metal-poor stars or on the composition of meteorites. This type of information is also required in order to make the best possible use of future high precision data on the actinide composition of galactic cosmic rays, of the local interstellar medium, or of meteoritic grains of presumed circumstellar origin. This paper provides the practitioners in these various fields with the most detailed and careful analysis of the r-process actinide production available to-date. This study is based on a version of the multi-event canonical model of the r-process which discards the largely used waiting point approximation. It considers also different combinations of models for the calculation of nuclear masses, beta -decay and fission rates. Two variants of the model used to predict nuclear reaction rates are adopted. In addition, the influence of the level of Pb and Bi production by the r-process on the estimated actinide production is evaluated by relying on the solar abundances of these two elements. In total, thirty-two different cases are presented, and are considered to give a fair picture of the level of reliability of the predictions of the actinide production, at least in the framework of a simple r-process model. This simplicity is imposed by our inability to identify the proper astrophysical sites for the r-process. As a guide to the practitioners, constraints on the actinide yield predictions and associated uncertainties are suggested on grounds of the measured abundances of r-nuclides, including Th and U, in the star CS 31082-001, and under the critical and questionable assumption of the ``universality'' of the r-process. We also define alternative constraints based on the nucleo-cosmochronological results derived from the present

  6. Physiochemical and spectroscopic behavior of actinides and lanthanides in solution, their sorption on minerals and their compounds formed with macromolecules; Comportamiento fisicoquimico y espectroscopico de actinidos y lantanidos en solucion, su sorcion sobre minerales y sus compuestos formados con macromoleculas

    Energy Technology Data Exchange (ETDEWEB)

    Jimenez R, M., E-mail: melania.jimenez@inin.gob.m [ININ, Departamento de Quimica, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico)

    2010-07-01

    From the chemical view point, the light actinides has been those most studied; particularly the uranium, because is the primordial component of the nuclear reactors. The chemical behavior of these elements is not completely defined, since they can behave as transition metals or metals of internal transition, as they are the lanthanides. The actinides are radioactive; between them they are emitters of radiation alpha, highly toxic, of live half long and some very long, and artificial elements. For all this, to know them sometimes is preferable to use their chemical similarity with the lanthanides and to study these. In particular, the migration of emitters of radiation alpha to the environment has been studied taking as model the uranium. It is necessary to mention that actinides and lanthanides elements are in the radioactive wastes of the nuclear reactors. In the Chemistry Department of the Instituto Nacional de Investigaciones Nucleares (ININ) the researches about the actinides and lanthanides began in 1983 and, between that year and 1995 several works were published in this field. In 1993 the topic was proposed as a Department project and from then around of 13 institutional projects and managerial activity have been developed, besides 4 projects approved by the National Council of Science and Technology. The objective of the projects already developed and of the current they have been contributing knowledge for the understanding of the chemical behavior of the lanthanides and actinides, as much in solution as in the solid state, their behavior in the environment and the chemistry of their complexes with recurrent and lineal macromolecules. (Author)

  7. 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)

  8. Actinide-Lanthanide separation by an electrolytic method in molten salt media: feasibility assessment of a renewed liquid cathode

    International Nuclear Information System (INIS)

    This study is part of a research program concerning the assessment of pyrochemical methods for the nuclear waste processing. The An-Ln partitioning could be achieved by an electrolytic selective extraction in molten salt media. It has been decided to focus on liquid reactive cathode which better suits to a group actinides co-recycling. The aim of the study is to propose, define and initiate the development of an electrolytic pyro-process dedicated to the quantitative and selective recovery of the actinides. Quantitativeness is related to technology, whereas selectivity is governed by chemistry. The first step consisted in selecting the adequate operating conditions, which enables a sufficient An-Ln separation. The first step consisted, by means of thermodynamic calculi and electrochemical investigations, in selecting a promising combination between molten electrolyte and cathodic material, regarding the process constraints. To improve the recovery yield, it is necessary to develop a disruptive technology: here comes the concept of a dynamic electrodeposition carried out onto liquid metallic drops. The next step consisted in designing and manufacturing a lab-scale device which enables dropping flow studies. Since interfacial phenomena are of primary meaning in such a concept, it has been decided to focus on high temperature liquid-liquid interfacial measurements. (author)

  9. Improved Actinide Neutron Capture Cross Sections Using Accelerator Mass Spectrometry

    Science.gov (United States)

    Bauder, W.; Pardo, R. C.; Kondev, F. G.; Kondrashev, S.; Nair, C.; Nusair, O.; Palchan, T.; Scott, R.; Seweryniak, D.; Vondrasek, R.; Collon, P.; Paul, M.; Youinou, G.; Salvatores, M.; Palmotti, G.; Berg, J.; Maddock, T.; Imel, G.

    2014-09-01

    The MANTRA (Measurement of Actinide Neutron TRAnsmutations) project will improve energy-integrated neutron capture cross section data across the actinide region. These data are incorporated into nuclear reactor models and are an important piece in understanding Generation IV reactor designs. We will infer the capture cross sections by measuring isotopic ratios from actinide samples, irradiated in the Advanced Test Reactor at INL, with Accelerator Mass Spectrometry (AMS) at ATLAS (ANL). The superior sensitivity of AMS allows us to extract multiple cross sections from a single sample. In order to analyze the large number of samples needed for MANTRA and to meet the goal of extracting multiple cross sections per sample, we have made a number of modifications to the AMS setup at ATLAS. In particular, we are developing a technique to inject solid material into the ECR with laser ablation. With laser ablation, we can better control material injection and potentially increase efficiency in the ECR, thus creating less contamination in the source and reducing cross talk. I will present work on the laser ablation system and preliminary results from our AMS measurements. The MANTRA (Measurement of Actinide Neutron TRAnsmutations) project will improve energy-integrated neutron capture cross section data across the actinide region. These data are incorporated into nuclear reactor models and are an important piece in understanding Generation IV reactor designs. We will infer the capture cross sections by measuring isotopic ratios from actinide samples, irradiated in the Advanced Test Reactor at INL, with Accelerator Mass Spectrometry (AMS) at ATLAS (ANL). The superior sensitivity of AMS allows us to extract multiple cross sections from a single sample. In order to analyze the large number of samples needed for MANTRA and to meet the goal of extracting multiple cross sections per sample, we have made a number of modifications to the AMS setup at ATLAS. In particular, we are

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

    International Nuclear Information System (INIS)

    The presence of small amount of mixed actinides and long-lived heat generators fission products as 137Cs and 90Sr 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 HNO3 and hydroxylamine nitrate + HNO3 as eluent. In the second one, CMP0-TBP(XAD7) column, the actinides were retained on the column and the separations were done by using (NH4)2C2O4 , DTPA, HNO3 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. (author)

  11. Marcoule institute for separation chemistry - ICSM. Scientific report 2007 - 2010

    International Nuclear Information System (INIS)

    The mixed research unit 'Institute for Separation Chemistry' was created jointly by CEA, CNRS, University of Montpellier and Ecole Nationale superieure de Chimie de Montpellier has obtained authorisation to start experiments including a few grams of depleted uranium and natural thorium in January 2010. Last takeoff was from our theory group, who started in October 2009. But the unit 'Institut de Chimie separative de Marcoule' existed as a team scattered in several places in France since 2007. At that time, monthly meetings gathered people for full days of open discussion every month, as 'Point ICSM', where colleagues from R/D Departments of the centre of Marcoule composed half of the audience. Scientific activity began in 2007 with progressive joining of ICSM of team leaders, co-workers, technicians and students, today with 38 permanent staff and 29 nonpermanent scientists and students. Most of the staff joined ICSM after or before participating to the European practical summer school in Analytical and separation chemistry, hold yearly for a full week including practical sessions since the first edition 2006 in Montpellier. Resources in Uranium are scarce, if only the 235 isotope is used. Wastes related to nuclear energy production are potentially dangerous. Since fifty years, the chemistry associated to nuclear energy production always followed the principles of green chemistry. Permanent attention in devoted to closing the life-cycle of materials and fuel, minimize wastes and ascertain the acceptability by a society via knowledge of chemistry and physical chemistry involved in the chemistry used for separation. Developing knowledge in order to propose new separation processes is the central aim of the ICSM. Enlarging this central goal to surfaces of materials, sono-chemistry as an example of green chemistry, chemistry and physical chemistry specific to actinides complete this picture. Thus, the ICSM is devoted to chemistry at the service of the nuclear energy of

  12. Theoretical study of the structure and reactivity of lanthanide and actinide based organometallic complexes; Etude theorique de la structure et de la reactivite de complexes organometalliques de lanthanides et d'actinides

    Energy Technology Data Exchange (ETDEWEB)

    Barros, N

    2007-06-15

    In this PhD thesis, lanthanide and actinide based organometallic complexes are studied using quantum chemistry methods. In a first part, the catalytic properties of organo-lanthanide compounds are evaluated by studying two types of reactions: the catalytic hydro-functionalization of olefins and the polymerisation of polar monomers. The reaction mechanisms are theoretically determined and validated, and the influence of possible secondary non productive reactions is envisaged. A second part focuses on uranium-based complexes. Firstly, the electronic structure of uranium metallocenes is analysed. An analogy with the uranyl compounds is proposed. In a second chapter, two isoelectronic complexes of uranium IV are studied. After validating the use of DFT methods for describing the electronic structure and the reactivity of these compounds, it is shown that their reactivity difference can be related to a different nature of chemical bonding in these complexes. (author)

  13. Organometallic chemistry

    OpenAIRE

    Bashkin, James K.; M.L.H. Green; Dr. M. L. H. Green

    1982-01-01

    Transition metal organometallic chemistry is a rapidly expanding field, which has an important relationship to industrial problems of petrochemical catalysis. This thesis describes studies of fundamental organometallic reaction processes, such as C-H and C-C bond formation and cleavage, and investigations of the structure and bonding of organometallic compounds. A number of techniques were used to pursue these studies, including synthesis, X-ray crystallography, and semi-em...

  14. Disk Chemistry*

    OpenAIRE

    Thi Wing-Fai

    2015-01-01

    The chemical species in protoplanetary disks react with each other. The chemical species control part of the thermal balance in those disks. How the chemistry proceeds in the varied conditions encountered in disks relies on detailed microscopic understanding of the reactions through experiments or theoretical studies. This chapter strives to summarize and explain in simple terms the different types of chemical reactions that can lead to complex species. The first part of the chapter deals wit...

  15. Interstellar chemistry

    OpenAIRE

    Klemperer, William

    2006-01-01

    In the past half century, radioastronomy has changed our perception and understanding of the universe. In this issue of PNAS, the molecular chemistry directly observed within the galaxy is discussed. For the most part, the description of the molecular transformations requires specific kinetic schemes rather than chemical thermodynamics. Ionization of the very abundant molecular hydrogen and atomic helium followed by their secondary reactions is discussed. The rich variety of organic species o...

  16. Computational chemistry

    Science.gov (United States)

    Arnold, J. O.

    1987-01-01

    With the advent of supercomputers, modern computational chemistry algorithms and codes, a powerful tool was created to help fill NASA's continuing need for information on the properties of matter in hostile or unusual environments. Computational resources provided under the National Aerodynamics Simulator (NAS) program were a cornerstone for recent advancements in this field. Properties of gases, materials, and their interactions can be determined from solutions of the governing equations. In the case of gases, for example, radiative transition probabilites per particle, bond-dissociation energies, and rates of simple chemical reactions can be determined computationally as reliably as from experiment. The data are proving to be quite valuable in providing inputs to real-gas flow simulation codes used to compute aerothermodynamic loads on NASA's aeroassist orbital transfer vehicles and a host of problems related to the National Aerospace Plane Program. Although more approximate, similar solutions can be obtained for ensembles of atoms simulating small particles of materials with and without the presence of gases. Computational chemistry has application in studying catalysis, properties of polymers, all of interest to various NASA missions, including those previously mentioned. In addition to discussing these applications of computational chemistry within NASA, the governing equations and the need for supercomputers for their solution is outlined.

  17. Review of Integral Experiments for Minor Actinide Management

    International Nuclear Information System (INIS)

    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)

  18. Preparation of isotopes and sources of actinide elements

    International Nuclear Information System (INIS)

    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: 233U, 238Pu, 242Pu, 243Cm, 242Cm, 244Cm (a); 228Th, 229Th, 234U, 237U, 239Np, 240Pu, 241Am, 248Cm (b); 237Np, 241Am (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

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  20. Lanthanide and actinide complexation studies with tetradentate 'N' donor ligands

    International Nuclear Information System (INIS)

    Because of their similar charge and chemical behaviour separation of trivalent actinides and lanthanides is an important and challenging task in nuclear fuel cycle. Soft (S,N) donor ligands show selectivity towards the trivalent actinides over the lanthanides. Out of various 'N' donor ligands studied, bis(1,2,4)triazinyl bipyridine (BTBP) and bis(1,2,4)triazinyl phenanthroline (BTPhen) were found to be most promising. In order to understand the separation behaviour of these ligands, their complexation studies with these 'f' block elements are essential. In the present work, complexation studies of various lanthanide ions (La3+, Eu3+ and Er3+) was studied with ethyl derivatives of BTBP (C2BTBP) and BTBPhen (C2BTPhen) and pentyl derivative of BTBP (C5BTBP) in acetonitrile medium using UV-Vis spectrophotometry, fluorescence spectroscopy and solution calorimetry. Computational studies were also carried out to understand the experimental results

  1. The effects of corrosion product colloids on actinide transport

    International Nuclear Information System (INIS)

    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)

  2. Evaluation of prompt neutron spectra for minor actinide nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Ohsawa, Takaaki [Kinki Univ., Higashi-Osaka, Osaka (Japan). Atomic Energy Research Inst.

    1997-03-01

    Measurement data on fission prompt neutron spectra of minor actinide (MA) is much little, and its accuracy is also unsufficient. Therefore, conventional evaluation value of fission spectra of MA was assumed for its nuclear temperature by using a method of determining from its systemicity owing to assumption of the Maxwell type distribution, but it can be said that this method consider fully to features of MA isotopes. In this paper, some evaluation calculation results are shown by adopting an evaluation method developed by authors and based on modified Madland Nix model and are conducted by concept of physical properties on target nuclei. As a result, by adopting the level density parameter of fission fragments, the inverse process cross section, the fission product yield distribution and the total release energy, effect of inverse process cross section, mass distribution of fission product, calculation results of Cm isotope and systemicity of fission spectra of actinide isotope were investigated. (G.K.)

  3. 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)

  4. 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.

  5. 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.

  6. Molecular Characterization of Actinide Oxocations from Protactinium to Plutonium

    International Nuclear Information System (INIS)

    This presentation addresses the structural characterization by EXAFS of actinide cations at oxidation states (V) and (VI) as one walks across the periodic table from Z = 91 (protactinium) to Z = 94 (plutonium). A structural comparison between Pa, U, Np and Pu oxocations in aqueous solution at formal oxidation states (V) and (VI) is carried out. These results are corroborated by quantum chemical and molecular dynamics calculations

  7. Validation of minor actinides fission neutron cross-sections

    Directory of Open Access Journals (Sweden)

    Pešić Milan P.

    2015-01-01

    Full Text Available Verification of neutron fission cross-sections of minor actinides from some recently available evaluated nuclear data libraries was carried out by comparison of the reaction rates calculated by the MCNP6.1 computer code to the experimental values. The experimental samples, containing thin layers of 235U, 237Np, 238,239,240,241Pu, 242mAm, 243Cm, 245Cm, and 247Cm, deposited on metal support and foils of 235U (pseudo-alloy 27Al + 235U, 238U, natIn, 64Zn, 27Al, and multi-component sample alloy 27Al + 55Mn + natCu + natLu + 197Au, were irradiated in the channels of the tank containing fluorine salts 0.52NaF + 0.48ZrF4, labelled as the Micromodel Salt Blanket, inserted in the lattice centre of the MAKET heavy water critical assembly at the Institute for Theoretical and Experimental Physics, Moscow. This paper is a continuation of earlier initiated scientific-research activities carried out for validation of the evaluated fission cross-sections of actinides that were supposed to be used for the quality examination of the fuel design of the accelerator driven systems or fast reactors, and consequently, determination of transmutation rates of actinides, and therefore, determination of operation parameters of these reactor facilities. These scientific-research activities were carried out within a frame of scientific projects supported by the International Science and Technology Center and the International Atomic Energy Agency co-ordinated research activities, from 1999 to 2010. Obtained results confirm that further research is needed in evaluations in order to establish better neutron cross-section data for the minor actinides and selected nuclides which could be used in the accelerator driven systems or fast reactors.

  8. EXAFS studies of actinide ions in aqueous solution

    Energy Technology Data Exchange (ETDEWEB)

    Karim, D P; Georgopoulos, P; Knapp, G S

    1979-01-01

    The applicability of the EXAFS technique in the study of actinide systems is discussed. Uranium L/sub III/-edge spectra obtained on an in-lab rotating anode EXAFS facility are presented and analyzed for crystalline UO/sub 2/F/sub 2/ and aqueous solutions containing hexavalent uranium ions. Methods for the extension of the technique to more dilute systems are discussed.

  9. 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.

  10. Chemical properties of the heavier actinides and transactinides

    International Nuclear Information System (INIS)

    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 5f147s27p. 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

  11. Prediction of thermodynamic properties of actinide and lanthanide compounds

    Institute of Scientific and Technical Information of China (English)

    LU Chunhai; NI Shijun; SUN Ying; CHEN Wenkai; ZHANG Chengjiang

    2008-01-01

    Several relationship models for thermodynamic functions of actinide and lanthanide compounds are built. The descriptors such as the difference of atomic radii between metal atoms and nonmetal atoms and the molecular mass are used in quantitative structure-activity/property relationships. The relative errors for entropy and heat capacity are less than 20% in the majority of gaseous compounds. Similar results are obtained from solid compounds.

  12. Covariance evaluation for actinide nuclear data in JENDL-4

    International Nuclear Information System (INIS)

    Full text: The JENDL-4.0 was released in March 2010. It provides neutron nuclear data for 79 actinides from Ac to Fm. All of the actinides include covariance data. The covariance data were evaluated for reaction cross sections, resonance parameters, angular distributions of elastic scattering, average number of neutrons per fission, and prompt fission neutron spectra. They were deduced basically based on the consistent methodologies with the nuclear data evaluations. Statistical processing of experimental data sometimes gives unacceptably small uncertainty compared with experimental data. They may arise from ignoring unknown errors and correlation of experimental data and also from the modeling errors. The covariance data obtained from statistical estimation using the least-squares method were sometimes modified to be reasonable taking account of consistency with dispersion of experimental data, which may reflect the uncertainties of the data. For the fast neutron fission cross sections of 6 major actinides of 233,235,238U and 239,240,241Pu were evaluated simultaneously using both cross section and their ratio data with the least- squares fitting code SOK. It gave the covariance matrices that have cross correlations between different nuclei included in the analyses. For the minor actinide, the least-squares fitting code GMA was used for fission cross section evaluation for fast neutrons. The covariance data were obtained from the calculations at the same time. For other reaction cross sections, covariance matrices were evaluated using CCONE-KALMAN code system. Sensitivities to model parameters were calculated by CCONE code and used to estimate covariance matrices of the parameters with KALMAN code. Covariance matrices for other data such as resonance parameters and average numbers of fission neutrons were also evaluated based on experimental data. The evaluated covariance data were compiled to the ENDF-6 format files and included in JENDL-4.

  13. Analytical applications of superacid dissolution of actinide and lanthanide substrates

    International Nuclear Information System (INIS)

    The superacid system HF/SbF5 is extraordinarily effective for total dissolution of actinide and lanthanide ceramic oxides, fluorides, and metals. Optical or gamma spectroscopy can be used directly on the solutions. Evaporation of the HF/SbF5 solvent under vacuum leaves a residue which is easily dissolved by ordinary mineral acids. The resulting aqueous solutions are readily amenable to conventional analytical methods. (author) 14 refs.; 1 tab

  14. Chemical and Ceramic Methods Toward Safe Storage of Actinides

    International Nuclear Information System (INIS)

    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

  15. 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.

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

    International Nuclear Information System (INIS)

    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

  17. Molecular Characterization of Actinide Oxocations from Protactinium to Plutonium

    Science.gov (United States)

    Den Auwer, C.; Guilbaud, P.; Guillaumont, D.; Moisy, P.; Digandomenico, V.; Le Naour, C.; Trubert, D.; Simoni, E.; Hennig, C.; Scheinost, A.; Conradson, S. D.

    2007-02-01

    This presentation addresses the structural characterization by EXAFS of actinide cations at oxidation states (V) and (VI) as one walks across the periodic table from Z = 91 (protactinium) to Z = 94 (plutonium). A structural comparison between Pa, U, Np and Pu oxocations in aqueous solution at formal oxidation states (V) and (VI) is carried out. These results are corroborated by quantum chemical and molecular dynamics calculations.

  18. ACTINIDE-SPECIFIC SEQUESTERING AGENTS AND DECONTAMINATION APPLICATIONS

    Energy Technology Data Exchange (ETDEWEB)

    Smith, William L.; Raymond, Kenneth N.

    1980-07-01

    We have briefly reviewed the biological hazards associated with the actinide elements. The most abundant transuranium element produced by both industrial nuclear power plants and nuclear weapons programs is plutonium. It is also potentially the most toxic - particularly due to its long-term hazard as a carcinogen if it is introduced into the body. This toxicity is due in large part to the chemical and biochemical similarities of Pu(IV) and Fe(III). Thus in mammals plutonium is transported and stored by the transport and storage systems for iron. This results in the concentration and long-term retention of an alpha-emitting radionuclide ({sup 239}Pu) at sites such as the bone marrow where cell division occurs at a high rate. The earliest attempts at removal of actinide contamination by chelation therapy were essentially heuristic in that sequestering agents known to be effective at binding other elements were tried with plutonium. The research described here is intended to be a rational approach that begins with the observation that since Fe(III) and Pu(IV) are so similar, and since microbes produce agents called siderophores that are extremely effective and selective sequestering agents for Fe(III), the construction of similar chelating agents for the actinides should be possible using the same chelating groups found in the siderophores. The incorporation of four such groups (primarily catechol and hydroxamic acid) results in multidentate chelating agents that can completely encapsulate the central actinide(IV) ion and achieve the eight-coordinate environment most favored by such ions. The continuing development and improvement of such sequestering agents has produced compounds which remove significant amounts of plutonium deposited in bone and which remove a greater fraction of the total body burden than any other chelation therapy developed to date.

  19. Future nuclear fuel cycles: Prospect and challenges for actinide recycling

    Science.gov (United States)

    Warin, Dominique

    2010-03-01

    The global energy context pleads in favour of a sustainable development of nuclear energy since the demand for energy will likely increase, whereas resources will tend to get scarcer and the prospect of global warming will drive down the consumption of fossil fuel. In this context, nuclear power has the worldwide potential to curtail the dependence on fossil fuels and thereby to reduce the amount of greenhouse gas emissions while promoting energy independence. How we deal with nuclear radioactive waste is crucial in this context. In France, the public's concern regarding the long-term waste management made the French Governments to prepare and pass the 1991 and 2006 Acts, requesting in particular the study of applicable solutions for still minimizing the quantity and the hazardousness of final waste. This necessitates High Active Long Life element (such as the Minor Actinides MA) recycling, since the results of fuel cycle R&D could significantly change the challenges for the storage of nuclear waste. HALL recycling can reduce the heat load and the half-life of most of the waste to be buried to a couple of hundred years, overcoming the concerns of the public related to the long-life of the waste and thus aiding the "burying approach" in securing a "broadly agreed political consensus" of waste disposal in a geological repository. This paper presents an overview of the recent R and D results obtained at the CEA Atalante facility on innovative actinide partitioning hydrometallurgical processes. For americium and curium partitioning, these results concern improvements and possible simplifications of the Diamex-Sanex process, whose technical feasibility was already demonstrated in 2005. Results on the first tests of the Ganex process (grouped actinide separation for homogeneous recycling) are also discussed. In the coming years, next steps will involve both better in-depth understanding of the basis of these actinide partitioning processes and, for the new promising

  20. Molecular cluster theory of chemical bonding in actinide oxide

    International Nuclear Information System (INIS)

    The electronic structure of actinide monoxides AcO and dioxides AcO2, where Ac = Th, U, Np, Pu, Am, Cm and Bk has been studied by molecular cluster methods based on the first-principles one-electron local density theory. Molecular orbitals for nearest neighbor clusters AcO10-6 and AcO12-8 representative of monoxide and dioxide lattices were obtained using non-relativistic spin-restricted and spin-polarized Hartree-Fock-Slater models for the entire series. Fully relativistic Dirac-Slater calculations were performed for ThO, UO and NpO in order to explore magnitude of spin-orbit splittings and level shifts in valence structure. Self-consistent iterations were carried out for NpO, in which the NpO6 cluster was embedded in the molecular field of the solid. Finally, a ''moment polarized'' model which combines both spin-polarization and relativistic effects in a consistent fashion was applied to the NpO system. Covalent mixing of oxygen 2p and Ac 5f orbitals was found to increase rapidly across the actinide series; metal s,p,d covalency was found to be nearly constant. Mulliken atomic population analysis of cluster eigenvectors shows that free-ion crystal field models are unreliable, except for the light actinides. X-ray photoelectron line shapes have been calculated and are found to compare rather well with experimental data on the dioxides

  1. Crystalline matrices for the immobilization of plutonium and actinides

    Energy Technology Data Exchange (ETDEWEB)

    Anderson, E.B.; Burakov, E.E.; Galkin, Ya.B.; Starchenko, V.A.; Vasiliev, V.G. [V.G. Khlopin Radium Institute, St. Petersburg (Russian Federation)

    1996-05-01

    The management of weapon plutonium, disengaged as a result of conversion, is considered together with the problem of the actinide fraction of long-lived high level radioactive wastes. It is proposed to use polymineral ceramics based on crystalline host-phases: zircon ZrSiO{sub 4} and zirconium dioxide ZrO{sub 2}, for various variants of the management of plutonium and actinides (including the purposes of long-term safe storage or final disposal from the human activity sphere). It is shown that plutonium and actinides are able to form with these phases on ZrSiO{sub 4} and ZrO{sub 2} was done on laboratory level by the hot pressing method, using the plasmochemical calcination technology. To incorporate simulators of plutonium into the structure of ZrSiO{sub 4} and ZrO{sub 2} in the course of synthesis, an original method developed by the authors as a result of studying the high-uranium zircon (Zr,U) SiO{sub 4} form Chernobyl {open_quotes}lavas{close_quotes} was used.

  2. The chemical thermodynamics of actinide elements and compounds

    International Nuclear Information System (INIS)

    This compilation forms the twelfth part of a comprehensive assessment and selection of actinide thermodynamic data. The other parts of the compilation deal mostly with actinide elements and compounds. This part, which is the last one to be published in this Series, concerns inorganic actinide complexes in aqueous solution. The properties considered include the stability constant as a function of ionic strength and temperature and, whenever possible, enthalpy and entropy values. The present assessment is based on a literature survey that was terminated in early 1989. In tabulating literature data, only experimental results were used; estimates as well as recalculated data were ignored. Unlike in previous assessments of this kind in this assessment the selection of a best value is discussed and justified, and reasons are given for the rejection of data. In addition, our estimates of the thermodynamic properties, based on interrelationships between analogous systems, are given when this can be done reliably. Another essential aim of this assessment is to indicate those areas in which additional research is required. Refs

  3. Toward laser ablation Accelerator Mass Spectrometry of actinides

    Science.gov (United States)

    Pardo, R. C.; Kondev, F. G.; Kondrashev, S.; Nair, C.; Palchan, T.; Scott, R.; Seweryniak, D.; Vondrasek, R.; Paul, M.; Collon, P.; Deibel, C.; Youinou, G.; Salvatores, M.; Palmotti, G.; Berg, J.; Fonnesbeck, J.; Imel, G.

    2013-01-01

    A project to measure neutron capture cross sections of a number of actinides in a reactor environment by Accelerator Mass Spectrometry (AMS) at the ATLAS facility of Argonne National Laboratory is underway. This project will require the precise and accurate measurement of produced actinide isotopes in many (>30) samples irradiated in the Advanced Test Reactor at Idaho National Laboratory with neutron fluxes having different energy distributions. The AMS technique at ATLAS is based on production of highly-charged positive ions in an electron cyclotron resonance (ECR) ion source followed by acceleration in the ATLAS linac and mass-to-charge (m/q) measurement at the focus of the Fragment Mass Analyzer. Laser ablation was selected as the method of feeding the actinide material into the ion source because we expect it will have higher efficiency and lower chamber contamination than either the oven or sputtering techniques, because of a much narrower angular distribution of emitted material. In addition, a new multi-sample holder/changer to allow quick change between samples and a computer-controlled routine allowing fast tuning of the accelerator for different beams, are being developed. An initial test run studying backgrounds, detector response, and accelerator scaling repeatability was conducted in December 2010. The project design, schedule, and results of the initial test run to study backgrounds are discussed.

  4. Value of 236U to actinide-only burnup credit

    International Nuclear Information System (INIS)

    The US Department of Energy (DOE) submitted a topical report to the US Nuclear Regulatory Commission (NRC) in May 1995 in order to gain approval of a method for criticality analysis of transport packages that takes account for the change in actinide isotopes with burnup [pressurized water reactors (PWRs) only]. Historically, the NRC has conservatively assumed that the fuel was in its initial conditions (without any burnable absorbers). In order to permit credit for the changes in actinide content, the NRC has required validation of the depletion and criticality codes for spent nuclear fuel, justification of conservative depletion modeling, and finally confirmation measurements before loading. The NRC requested additional information on March 22, 1996. The DOE responded by a revision of the topical report in May 1997. The NRC again responded with another set of requests of additional information in April 1998. In that set of questions, the NRC challenged the use of 236U in burnup credit. Uranium-236 is not found in any significant amount in any available critical experiments. The authors explore the value of 236U to actinide-only burnup credit

  5. RAPID SEPARATION METHOD FOR ACTINIDES IN EMERGENCY AIR FILTER SAMPLES

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.; Noyes, G.; Culligan, B.

    2010-02-03

    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 {sup 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 {sup 90}Sr in air filter results were reported in {approx}4 hours with excellent quality.

  6. Behavior of actinides in the Integral Fast Reactor fuel cycle

    Energy Technology Data Exchange (ETDEWEB)

    Courtney, J.C. [Louisiana State Univ., Baton Rouge, LA (United States). Nuclear Science Center; Lineberry, M.J. [Argonne National Lab., Idaho Falls, ID (United States). Technology Development Div.

    1994-06-01

    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 ({sup 237}Np, {sup 240}Pu, {sup 241}Am, and {sup 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 plutonium. Eighteen sets of seven actinide and five light metal targets have been selected for ten day exposure in the Experimental Breeder Reactor-2 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.

  7. 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...... of competing localized and delocalized f-electron configurations underlies the ground states of NpC, PuC, AmC, NpN, and PuN. The fully localized 5f-electron configuration is realized in CmC (f7), CmN (f7), and AmN (f6). The observed sudden increase in lattice parameter from PuN to AmN is found to be related...... increasing degree of f electron localization from U to Cm, with the tendency toward localization being slightly stronger in the (more ionic) nitrides compared to the (more covalent) carbides. The itinerant band picture is found to be adequate for UC and acceptable for UN, while a more complex manifold...

  8. 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...

  9. 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)

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

    International Nuclear Information System (INIS)

    This contribution presents a small piece of research work at KIT-INE dealing with the speciation of redox sensitive trivalent actinides like Pu(III), Np(III), and U(III) in aqueous solution. The redox preparation, stabilization, and speciation of trivalent actinide in aqueous systems are discussed here. The reductants investigated were rongalite, HYA (hydroxylamine hydrochloride), and AHA (acetohydroxamic acid). The time dependence of An(III) stability at different pH values was investigated. The An(III) species in aqueous solution have been characterized by UV-Vis and XANES spectroscopy. A broader overview of the work at KIT-INE is given in the oral presentation at the NUCAR2013 conference. (author)

  11. Factors affecting actinide solubility in a repository for spent fuel, 1

    International Nuclear Information System (INIS)

    The main tasks in the study were to get information on the chemical conditions in a repository for spent fuel and information on factors affecting releases of actinides from spent fuel and solubility of actinides in a repository for spent fuel. The work in this field started at the Reactor Laboratory of the Technical Research Centre of Finland (VTT) in 1982. This is a report on the effects on the main parameters, Eh, pH, carbonate, organic compounds, colloids, microbes and radiation on the actinide solubility in the nearfield of the repository. Another task has been to identify available models and reported experience from actinide solubility calculations with different codes. 167 refs

  12. Utilization of Minor Actinides (Np, Am, Cm) in Nuclear Power Reactor

    Science.gov (United States)

    Gerasimov, A.; Bergelson, B.; Tikhomirov, G.

    2014-06-01

    Calculation research of the utilization process of minor actinides (transmutation with use of power released) is performed for specialized power reactor of the VVER type operating on the level of electric power of 1000 MW. Five subsequent cycles are considered for the reactor with fuel elements containing minor actinides along with enriched uranium. It was shown that one specialized reactor for the one cycle (900 days) can utilize minor actinides from several VVER-1000 reactors without any technological and structural modifications. Power released because of minor actinide fission is about 4% with respect to the total power

  13. Theoretical chemistry periodicities in chemistry and biology

    CERN Document Server

    Eyring, Henry

    1978-01-01

    Theoretical Chemistry: Periodicities in Chemistry and Biology, Volume 4 covers the aspects of theoretical chemistry. The book discusses the stably rotating patterns of reaction and diffusion; the chemistry of inorganic systems exhibiting nonmonotonic behavior; and population cycles. The text also describes the mathematical modeling of excitable media in neurobiology and chemistry; oscillating enzyme reactions; and oscillatory properties and excitability of the heart cell membrane. Selected topics from the theory of physico-chemical instabilities are also encompassed. Chemists, mechanical engin

  14. Extending Stannyl Anion Chemistry to the Actinides: Synthesis and Characterization of a Uranium-Tin Bond.

    Science.gov (United States)

    Winston, Matthew S; Batista, Enrique R; Yang, Ping; Tondreau, Aaron M; Boncella, James M

    2016-06-01

    We have synthesized a rare example of a uranium(IV) stannyl (κ(4)-N(CH2CH2NSi((i)Pr)3)3U(SnMe3), 1) via transmetalation with LiSnMe3. This complex has been characterized crystallographically and shown to have a U-Sn bond length of 3.3130(3) Å, substantially longer than the only other crystallographically observed U-Sn bond (3.166 Å). Computational studies suggest that the U-Sn bond in 1 is highly polarized, with significant charge transfer to the stannylate ligand. We briefly discuss plausible mechanistic scenarios for the formation of 1, which may be relevant to other transmetalation processes involving heavy main group atoms. Furthermore, we demonstrate the reducing ability of [SnMe3](-) in the absence of strongly donating ligands on U(IV). PMID:27219499

  15. Plutonium(IV) complexation by diglycolamide ligands - coordination chemistry insight into TODGA-based actinide separations

    NARCIS (Netherlands)

    Reilly, S.D.; Gaunt, A.J.; Scott, B.L.; Modolo, G.; Iqbal, M.; Verboom, W.; Sarsfield, M.J.

    2012-01-01

    Complexation of Pu(IV) with TMDGA, TEDGA, and TODGA diglycolamide ligands was followed by vis-NIR spectroscopy. A crystal structure determination reveals that TMDGA forms a 1:3 homoleptic Pu(IV) complex with the nitrate anions forced into the outer coordination sphere

  16. Advanced processes for minor actinides recycling: studies towards potential industrialization

    International Nuclear Information System (INIS)

    In June 2006, a new act on sustainable management of radioactive waste was voted by the French parliament with a national plan on radioactive materials and radioactive waste management (PNG-MDR). Concerning partitioning and transmutation, the program is connected to 4. generation reactors, in which transmutation of minor actinides could be operated. In this frame, the next important milestone is 2012, with the assessment of the possible transmutation roads, which are either homogeneous recycling of the minor actinides in the whole reactor fleet, with a low content of M.A (∼3%) in all fuel assemblies, or heterogeneous recycling of the minor actinides in about one third of the reactor park, with a higher content of M.A. (∼20%) in dedicated targets dispatched in the periphery of the reactor. Advanced processes for the recycling of minor actinides are being developed to address the challenges of these various management options. An important part of the program consists in getting closer to process implementation conditions. The processes based on liquid-liquid extraction benefit from the experience gained by operating the PUREX process at the La Hague plant. In the field of extracting apparatus, a large experience is available. In the field of extracting apparatus, a large experience is already available. Nevertheless, the processes present specificities which have to be considered more precisely. They have been classified in the following fields: - Evolution of the simulation codes, including phenomenological representations: with such a simulation tool, it will be possible to assess operating tolerances, lead sensitivity studies and calculate transient states; - Definition of the implementation conditions in continuous contactors (such as pulse columns), according to the extractant physico-chemical characteristics; - Scale-up of new extractants, such as malonamides used in the DIAMEX process, facing purity specifications and costs estimation; - Solvent clean

  17. Surface chemistry

    CERN Document Server

    Desai, KR

    2008-01-01

    The surface Chemistry of a material as a whole is crucially dependent upon the Nature and type of surfaces exposed on crystallites. It is therefore vitally important to independently Study different, well - defined surfaces through surface analytical techniques. In addition to composition and structure of surface, the subject also provides information on dynamic light scattering, micro emulsions, colloid Stability control and nanostructures. The present book endeavour to bring before the reader that the understanding and exploitation of Solid state phenomena depended largely on the ability to

  18. Semiannual Report of the Chemistry Department, June--November 1966

    International Nuclear Information System (INIS)

    This semiannual report of the Chemistry Department of the Cea of Fontenay-aux Roses, presents in its first part researches on the chemical analysis, the treatment of fairly and slightly active effluents, the uranium treatment, studies on electrometallurgy, studies on corrosion and studies on filtration and elimination on sea water of hard compounds. The second part is devoted to the study of aqueous reprocessing of irradiated fuels (laboratory and pilot plant), anhydrous reprocessing, actinides elements isotopes preparation and study, fission products concentrated solution vitrification study and fundamental studies on acid-base properties. (A.L.B.)

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

    International Nuclear Information System (INIS)

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

  20. NATO Advanced Study Institute on Fundamental and Technological Aspects of Organo-f-Element Chemistry

    CERN Document Server

    Fragalà, Ignazio

    1985-01-01

    The past decade has seen a dramatic acceleration of activity and interest in phenomena surrounding lanthanide and actinide organo­ metallic compounds. Around the world, active research in organo-f­ element synthesis, chemistry, catalysis, crystallography, and quantum chemistry is in progress. This activity has spanned a remarkably wide range of disciplines, from synthetic/mechanistic inorganic and organic chemistry to radiochemistry, catalytic chemistry, spectroscopy (vibra­ tional, optical, magnetic resonance, photoelectron, Mossbauer), X-ray and neutron diffraction structural analysis, as well as to crystal field and molecular orbital theoretical studies at the interface of chemistry and physics. These investigations have been motivated both by fundamental and applied goals. The evidence that f-element organo­ metallic compounds have unique chemical and physical properties which cannot be duplicated by organometallic compounds of d-block elements has suggested many new areas of endeavor and application....

  1. New Insights into the Chemistry of Imidodiphosphinates from Investigations of Tellurium-Centered Systems

    OpenAIRE

    Chivers, Tristram; Ritch, Jamie; Robertson, Stuart; Konu, Jari; Tuononen, Heikki

    2010-01-01

    Dichalcogenido-imidodiphosphinates, [N(PR2E)2]− (R = alkyl, aryl), are chelating ligands that readily form cyclic complexes with main group metals, transition metals, lanthanides, and actinides. Since their discovery in the early 1960s, researchers have studied the structural chemistry of the resulting metal complexes (where E = O, S, Se) extensively and identified a variety of potential applications, including as NMR shift reagents, luminescent complexes in photonic devices, or single-source...

  2. Magnetic susceptibility of actinide(iii) cations: an experimental and theoretical study.

    Science.gov (United States)

    Autillo, Matthieu; Guerin, Laetitia; Bolvin, Hélène; Moisy, Philippe; Berthon, Claude

    2016-03-01

    In a previous paper, the influence of radioactive decay (α and β(-)) on magnetic susceptibility measurements by the Evans method has been demonstrated by the study of two americium isotopes. To characterize more accurately this phenomenon and particularly its influence on the Curie law, a new study has been performed on two uranium isotopes ((238)U and (233)U) and on tritiated water ((3)H2O). The results on the influence of α emissions have established a relationship between changes in the temperature dependence and the radioactivity in solution. Regarding the β(-) emissions, less influence was observed while no temperature dependence linked to this kind of radioactive emission could be identified. Once magnetic susceptibility measurements of actinide(iii) cations were corrected from radioactivity effects, methods of quantum chemistry have been used on free ions and aquo complexes to calculate the electronic structure explaining the magnetic properties of Pu(iii), Am(iii) and Cm(iii). The ligand field effect on the magnetic behavior (the Curie constant and temperature-independent susceptibilities) was analyzed by considering different solvation environments. PMID:26864302

  3. Studies of the chemistry of transuranium elements and technetium at the Institute of Physical Chemistry, Russian Academy of Sciences, supported by the US Department of Energy

    International Nuclear Information System (INIS)

    Studies at Hanford in the 1980s revealed the potential for actinides to form stable soluble complexes in alkaline media, simulating radioactive tank waste. Pu(IV) hydrous oxide and Pu(VI) solubility increased with hydroxide concentration, ionic strength, and aluminate/carbonate concentrations. Subsequent contacts between US and Russian researchers in 1993 led to a technical literature review of the chemistry of TRU and Tc in alkaline media; this review addresses oxidation states, solubility, speciation, redox reactions, electrochemistry, radiation chemistry, and separations in alkaline media. As an outgrowth, a program of fundamental and applied chemistry studies of TRU and Tc is being conducted at IPC/RAS with US DOE support: solubility, redox reagents, coprecipitation, and radiation chemistry. This overview provides information on the Hanford Site tank waste system, US DOE technological needs, and IPC/RAS developments

  4. Cyclodextrin chemistry

    International Nuclear Information System (INIS)

    The chemistry of cyclodextrins was studied. This study included synthesising some cyclodextrin derivatives, preparing selected inclusion complexes with cyclodextrin and investigating the effects of gamma irradiation on cyclodextrins and certain linear oligosaccharides. This report presents a brief review of the structure and properties of cyclodextrins, the synthesis of cyclodextrin derivatives, their complexation and applications. This is followed by a description of the synthesis of some cyclodextrin derivatives and the preparation of inclusion complexes of cyclodextrin with some organic compounds. Finally, the effects of gamma irradiation on cyclodextrins, some of their derivatives and certain structurally related carbohydrates are discussed. The gamma irradiation studies were carried out for two reasons: to study the effects of gamma irradiation on cyclodextrins and their derivatives; and to investigate selectivity during the gamma irradiation of cyclodextrin derivatives

  5. Combustion chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Brown, N.J. [Lawrence Berkeley Laboratory, CA (United States)

    1993-12-01

    This research is concerned with the development and use of sensitivity analysis tools to probe the response of dependent variables to model input variables. Sensitivity analysis is important at all levels of combustion modeling. This group`s research continues to be focused on elucidating the interrelationship between features in the underlying potential energy surface (obtained from ab initio quantum chemistry calculations) and their responses in the quantum dynamics, e.g., reactive transition probabilities, cross sections, and thermal rate coefficients. The goals of this research are: (i) to provide feedback information to quantum chemists in their potential surface refinement efforts, and (ii) to gain a better understanding of how various regions in the potential influence the dynamics. These investigations are carried out with the methodology of quantum functional sensitivity analysis (QFSA).

  6. Systematic Characteristics of Fast Neutron Fission Cross Sections for Actinide Nuclei

    Institute of Scientific and Technical Information of China (English)

    2011-01-01

    The neutron fission cross sections of actinide nuclei are important data for the design of nuclear reactor and nuclear engineering, and so on. So far, there has been a certain amount of experimental data for the fission cross sections of actinide nuclei. However,

  7. 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)

  8. Separation of actinides from lanthanides using acidic organophosphorus compounds: extraction chromatographic studies

    International Nuclear Information System (INIS)

    The partitioning of actinides from HLW using TBP and CMPO generates a mixture of actinides and lanthanides as one of the secondary streams. The paper discusses the results of the extraction chromatographic separation using KSM-17 and HDEHP supported on Chromosorb-102. (author)

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

    International Nuclear Information System (INIS)

    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)

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

    NARCIS (Netherlands)

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

    2014-01-01

    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

  11. Public perception of chemistry

    OpenAIRE

    Stražar, Alenka

    2015-01-01

    The thesis deals with the perception of chemistry among the public, which reflects the stereotypes that people have about chemistry. It presents the existing classification of stereotypes about chemistry and their upgrade. An analysis of movies that reflect the existing perception of chemistry in the public is written. Literature on selected aspects of the application of chemistry in movies is collected and analyzed. A qualification of perception of chemistry in the movies is presented based ...

  12. Use of high gradient magnetic separation for actinide application

    International Nuclear Information System (INIS)

    Decontamination of materials such as soils or waste water that contain radioactive isotopes, heavy metals, or hazardous components is a subject of great interest. Magnetic separation is a physical separation process that segregates materials on the basis of magnetic susceptibility. Because the process relies on physical properties, separations can be achieved while producing a minimum of secondary waste. Most traditional physical separation processes effectively treat particles larger than 70 microns. In many situations, the radioactive contaminants are found concentrated in the fine particle size fraction of less than 20 microns. For effective decontamination of the fine particle size fraction most current operations resort to chemical dissolution methods for treatment. High gradient magnetic separation (HGMS) is able to effectively treat particles from 90 to ∼0.1 micron in diameter. The technology is currently used on the 60 ton per hour scale in the kaolin clay industry. When the field gradient is of sufficiently high intensity, paramagnetic particles can be physically captured and separated from extraneous nonmagnetic material. Because all actinide compounds are paramagnetic, magnetic separation of actinide containing mixtures is feasible. The advent of reliable superconducting magnets also makes magnetic separation of weakly paramagnetic species attractive. HGMS work at Los Alamos National Laboratory (LANL) is being developed for soil remediation, waste water treatment and treatment of actinide chemical processing residues. LANL and Lockheed Environmental Systems and Technologies Company (LESAT) have worked on a co-operative research and development agreement (CRADA) to develop HGMS for radioactive soil decontamination. The program is designed to transfer HGMS from the laboratory and other industries for the commercial treatment of radioactive contaminated materials. 9 refs., 2 figs., 2 tabs

  13. Final Report on Actinide Glass Scintillators for Fast Neutron Detection

    Energy Technology Data Exchange (ETDEWEB)

    Bliss, Mary; Stave, Jean A.

    2012-10-01

    This is the final report of an experimental investigation of actinide glass scintillators for fast-neutron detection. It covers work performed during FY2012. This supplements a previous report, PNNL-20854 “Initial Characterization of Thorium-loaded Glasses for Fast Neutron Detection” (October 2011). The work in FY2012 was done with funding remaining from FY2011. As noted in PNNL-20854, the glasses tested prior to July 2011 were erroneously identified as scintillators. The decision was then made to start from “scratch” with a literature survey and some test melts with a non-radioactive glass composition that could later be fabricated with select actinides, most likely thorium. The normal stand-in for thorium in radioactive waste glasses is cerium in the same oxidation state. Since cerium in the 3+ state is used as the light emitter in many scintillating glasses, the next most common substitute was used: hafnium. Three hafnium glasses were melted. Two melts were colored amber and a third was clear. It barely scintillated when exposed to alpha particles. The uses and applications for a scintillating fast neutron detector are important enough that the search for such a material should not be totally abandoned. This current effort focused on actinides that have very high neutron capture energy releases but low neutron capture cross sections. This results in very long counting times and poor signal to noise when working with sealed sources. These materials are best for high flux applications and access to neutron generators or reactors would enable better test scenarios. The total energy of the neutron capture reaction is not the only factor to focus on in isotope selection. Many neutron capture reactions result in energetic gamma rays that require large volumes or high densities to detect. If the scintillator is to separate neutrons from gamma rays, the capture reactions should produce heavy particles and few gamma rays. This would improve the detection of a

  14. MINOR ACTINIDE SEPARATIONS USING ION EXCHANGERS OR IONIC LIQUIDS

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-09-20

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

  15. Hybridization effects in selected actinides and their compounds

    Science.gov (United States)

    El-Khatib, Sami T.

    Many actinide systems exhibit 'unusual' phenomena that differ from the normal text-book behavior. This occurs because the 5f electrons of the actinides and their compounds experience a delicate balance between local-moment and itinerant magnetism. It is well established that strong-electron correlations affect the different properties in such systems. Even though the actinides and their compounds have been extensively studied in recent decades, both experimentally and theoretically, to date, no complete understanding of the full range of their properties has been achieved. My thesis focuses mainly on understanding the role of 5f electrons and their interactions with the electron states of the surrounding ligands. Particularly, the effect of the 5f-ligand hybridization in the development of bulk properties is investigated. The experimental studies utilized macroscopic techniques, such as magnetization, electrical-resistivity, specific-heat and resonant-ultrasound-spectroscopy measurements, as well as microscopic techniques, such as neutron-diffraction and muon-spin-resonance studies. The results are used to disentangle the importance of direct 5f--5f overlap and 5 f-ligand hybridization. The following features have been investigated in this thesis: (a) the dual nature of hybridization effects (magnetic moment reduction vs. exchange mediation) was studied for two isostructural uranium compounds U2Pd2Sn and U2Ni2 In; (b) the formation of complex magnetic structures and its connection to the hybridization effects was studied for UCuSn, UPdSn and UPdGe; (c) the tuning of the hybridization to critical values through substitutions was attempted for two single crystals of UCoAl1-xSn x and UNi1-xRh xAl alloys; (d) the effects of compositional deficiencies was studied for the copper-deficient compound in UCu1.5Sn 2; and finally, (e) the influence of strong electron correlations on the elastic properties was studied in the case of alpha-Pu.

  16. Review of alpha-particle spectrometric measurements of actinides

    International Nuclear Information System (INIS)

    At present the silicon surface-barrier detector is the most used α-particle detector mainly due to its high energy resolution, excellent stability, low background and low cost. In this presentation various parameters of importance for α-particle spectrometry are discussed, i.e. energy resolution and interval selection, energy calibration, background and peak tailing. Examples of α-particle spectra recorded from various actinides (Th, U, Np, Pu, Am, and Cm) separated from environmental samples are shown, and the choice of yield determinants is discussed for each case. (author)

  17. Hydrometallurgical minor actinide separation in hollow fiber modules

    International Nuclear Information System (INIS)

    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)

  18. Neutron absorption spectroscopy for identification of light elements in actinides

    International Nuclear Information System (INIS)

    We are developing cryogenic high-energy resolution fast-neutron spectrometers using superconducting transition-edge sensors (TES) for nuclear science and non-proliferation applications. Fast neutrons are absorbed in 94% enriched 6LiF single crystals with volumes of ∼1 cm3 in an exothermic 6Li(n,α)3H capture reaction. The neutron energy is measured from the subsequent temperature rise with a Mo/Cu multilayer TES. Fast-neutron spectra from a 252Cf source show an energy resolution of 55 kev. Here, we discuss the instrument performance, with emphasis on the identification of light elements in actinide matrices

  19. Voluntary activities on actinides by the public in Peninsula Shimokita

    International Nuclear Information System (INIS)

    Peninsula Shimokita is known as a Nuclear Peninsula. A technical term actinides', however, is not used among the public here. It is not only used, but also is not probably known among them, although an investigation for the terminology and vocabulary on the nuclear science and technology among the public in this district has not ever performed. The terms in use here widely are uranium (-235, -238), plutonium (-239), and trans-uranium elements for what are heavier than the uranium. The present paper will report on voluntary activities by the public in the Penin. Shimokita performed after the neutron criticality accident at JCO Tokai of a company for nuclear fuel conversion. (author)

  20. Fission of actinides using a table-top laser

    CERN Document Server

    Schwoerer, H; Sauerbrey, R; Galy, J; Magill, J; Rondinella, V; Schenkel, R; Butz, T

    2003-01-01

    Powerful table-top lasers are now available in the laboratory and can be used to induce nuclear reactions. We report the first demonstration of nuclear fission using a high repetition rate table-top laser with intensities of 10 sup 2 sup 0 W/cm sup 2. Actinide photo-fission has been achieved in both sup 2 sup 3 sup 8 U and sup 2 sup 3 sup 2 Th from the high-energy Bremsstrahlung radiation produced by laser acceleration of electrons. The fission products were identified by time-resolved gamma-spectroscopy. (authors)

  1. 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.

  2. Electron-phonon coupling of the actinide metals

    DEFF Research Database (Denmark)

    Skriver, H. L.; Mertig, I.

    1985-01-01

    -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...... be related to the changeover from an s-to- d to an s-to-f electronic transition and a related change in the topology of the Fermi surface...

  3. Heavy element and actinide decay data: UKHEDD-2 data files

    International Nuclear Information System (INIS)

    A re-evaluation has been made of the decay data for 126 heavy elements and actinides of direct application in nuclear fuel cycle calculations. Computer-based data files have been produced in ENDF/B-VI format, including lists of the references used to produce the proposed decay schemes and comments that identify their inadequacies. These evaluated data include half-lives, average decay energies, branching ratios, alpha, beta and gamma-ray energies and emission probabilities, internal conversion coefficients, spontaneous fission decay data and all associated uncertainties. (author)

  4. Formation of new actinide nuclides and their reaction cross section

    International Nuclear Information System (INIS)

    Helium jet transfer system, which had been designed and constructed for the study of actinide nuclides, was examined for the transfer efficiency of recoils and fission products formed in the nuclear reaction induced by α particles. The efficiency was found to be close to unity for products coming out of a 232Th target bombarded with 110 MeV α particles of intensity less than 40 nA. Residual radio-activities of a target chamber and a collection chamber were also measured. (author)

  5. Geochemistry of actinides and fission products in natural aquifer systems

    International Nuclear Information System (INIS)

    The progress in the research area of the community project MIRAGE: 'Geochemistry of actinides and fission products in natural aquatic systems' has been reviewed. This programme belongs to a specific research and technical development programme for the European Atomic Energy Community in the field of management and storage of radioactive waste. The review summarizes research progresses in subject areas: complexation with organics, colloid generation in groundwater and basic retention mechanisms in the framework of the migration of radionuclides in the geosphere. The subject areas are being investigated by 23 laboratories under interlaboratory collaborations or independent studies. (orig.)

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  7. Selective extraction of trivalent actinides from lanthanides with dithiophosphinic acids and tributylphosphate

    Energy Technology Data Exchange (ETDEWEB)

    Jarvinen, G.; Barrans, R.; Schroeder, N.; Wade, K.; Jones, M.; Smith, B.F. [Los Alamos National Lab., NM (United States); Mills, J.; Howard, G. [Texas Tech Univ., Lubbock, TX (United States); Freiser, H.; Muralidharan, S. [Arizona Univ., Tucson, AZ (United States)

    1995-01-01

    A variety of chemical systems have been developed to separate trivalent actinides from lanthanides based on the slightly stronger complexation of the trivalent actinides with ligands that contain soft donor atoms. The greater stability of the actinide complexes in these systems has often been attributed to a slightly greater covalent bonding component for the actinide ions relative to the lanthanide ions. The authors have investigated several synergistic extraction systems that use ligands with a combination of oxygen and sulfur donor atoms that achieve a good group separation of the trivalent actinides and lanthanides. For example, the combination of dicyclohexyldithiophosphinic acid and tributylphosphate has shown separation factors of up to 800 for americium over europium in a single extraction stage. Such systems could find application in advanced partitioning schemes for nuclear waste.

  8. Science Update: Inorganic Chemistry.

    Science.gov (United States)

    Rawls, Rebecca

    1981-01-01

    Describes areas of inorganic chemistry which have changed dramatically in the past year or two, including photochemistry, electrochemistry, organometallic complexes, inorganic reaction theory, and solid state chemistry. (DS)

  9. Measurement of standard potentials of actinides (U,Np,Pu,Am) in LiCl-KCl eutectic salt and separation of actinides from rare earths by electrorefining

    International Nuclear Information System (INIS)

    Pyrochemical separation of actinides from rare earths in LiCl-KCl eutectic-liquid metal systems has been studied. The electromotive forces of galvanic cells of the form, Ag vertical stroke Ag(I), LiCl-KCl parallel actinide(III), LiCl-KCl vertical stroke actinide, were measured and standard potentials were determined for uranium, neptunium and plutonium to be -1.283 V, -1.484 V and -1.593 V (at 450 C vs. Ag/AgCl (1wt%-AgCl)), respectively. A typical cyclic voltammogram of americium chloride has two cathodic peaks, which suggests reduction Am(III)→Am(II) occurs followed by reduction of Am(II) to americium metal. Standard potential of Am(II)/Am(0) was estimated to be -1.642 V. Electrorefining experiments to separate actinides (U, Np, Pu and Am) from rare earths (Y, La, Ce, Nd and Gd) in LiCl-KCl eutectic salt were carried out. It was shown that the actinide metals were recovered on the cathodes and that americium was the most difficult to separate from rare earths. The actinide separation will be achieved by means of the combination of electrorefining with multistage extraction. (orig.)

  10. Review of actinide-sediment reactions with an annotated bibliography

    Energy Technology Data Exchange (ETDEWEB)

    Ames, L.L.; Rai, D.; Serne, R.J.

    1976-02-10

    The annotated bibliography is divided into sections on chemistry and geochemistry, migration and accumulation, cultural distributions, natural distributions, and bibliographies and annual reviews. (LK)

  11. Trace Chemistry

    Science.gov (United States)

    Radhakrishnan, Krishnan; Whitefield, Philip

    1999-01-01

    The goals of the trace chemistry group were to identify the processes relevant to aerosol and aerosol precursor formation occurring within aircraft gas turbine engines; that is, within the combustor, turbine, and nozzle. The topics of discussion focused on whether the chemistry of aerosol formation is homogeneous or heterogeneous; what species are important for aerosol and aerosol precursor formation; what modeling/theoretical activities to pursue; what experiments to carry out that both support modeling activities and elucidate fundamental processes; and the role of particulates in aerosol and aerosol precursor formation. The consensus of the group was that attention should be focused on SO2, SO3, and aerosols. Of immediate concern is the measurement of the concentration of the species SO3, SO2, H2SO4 OH, HO2, H2O2, O, NO, NO2, HONO, HNO3, CO, and CO2 and particulates in various engines, both those currently in use and those in development. The recommendation was that concentration measurements should be made at both the combustor exit and the engine exit. At each location the above species were classified into one of four categories of decreasing importance, Priority I through IV, as follows: Combustor exit: Priority I species - SO3:SO2 ratio, SO3, SO2, and particulates; Priority II species: OH and O; Priority III species - NO and NO2; and Priority IV species - CO and CO2. For the Engine exit: Priority I species - SO3:SO2 ratio, SO3, SO2,H2SO4, and particulates; Priority II species: OH,HO2, H2O2, and O; Priority III species - NO, NO2, HONO, and HNO3; and Priority IV species - CO and CO2. Table I summarizes the anticipated concentration range of each of these species. For particulate matter, the quantities of interest are the number density, size distribution, and composition. In order to provide data for validating multidimensional reacting flow models, it would be desirable to make 2-D, time-resolved measurements of the concentrations of the above species and

  12. Migration chemistry

    International Nuclear Information System (INIS)

    Migration chemistry, the influence of chemical -, biochemical - and physico-chemical reactions on the migration behaviour of pollutants in the environment, is an interplay between the actual natur of the pollutant and the characteristics of the environment, such as pH, redox conditions and organic matter content. The wide selection of possible pollutants in combination with varying geological media, as well as the operation of different chemical -, biochemical - and physico-chemical reactions compleactes the prediction of the influence of these processes on the mobility of pollutants. The report summarizes a wide range of potential pollutants in the terrestrial environment as well as a variety of chemical -, biochemical - and physico-chemical reactions, which can be expected to influence the migration behaviour, comprising diffusion, dispersion, convection, sorption/desorption, precipitation/dissolution, transformations/degradations, biochemical reactions and complex formation. The latter comprises the complexation of metal ions as well as non-polar organics to naturally occurring organic macromolecules. The influence of the single types of processes on the migration process is elucidated based on theoretical studies. The influence of chemical -, biochemical - and physico-chemical reactions on the migration behaviour is unambiguous, as the processes apparently control the transport of pollutants in the terrestrial environment. As the simple, conventional KD concept breaks down, it is suggested that the migration process should be described in terms of the alternative concepts chemical dispersion, average-elution-time and effective retention. (AB) (134 refs.)

  13. The radiation chemistry of ionic liquids: A review

    International Nuclear Information System (INIS)

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

  14. Stabilization of actinides and lanthanides in unusually high oxidation states

    Energy Technology Data Exchange (ETDEWEB)

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

    1986-01-01

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

  15. APPLICATION OF ABSORPTION SPECTROSCOPY TO ACTINIDE PROCESS ANALYSIS AND MONITORING

    Energy Technology Data Exchange (ETDEWEB)

    Lascola, R.; Sharma, V.

    2010-06-03

    The characteristic strong colors of aqueous actinide solutions form the basis of analytical techniques for actinides based on absorption spectroscopy. Colorimetric measurements of samples from processing activities have been used for at least half a century. This seemingly mature technology has been recently revitalized by developments in chemometric data analysis. Where reliable measurements could formerly only be obtained under well-defined conditions, modern methods are robust with respect to variations in acidity, concentration of complexants and spectral interferents, and temperature. This paper describes two examples of the use of process absorption spectroscopy for Pu analysis at the Savannah River Site, in Aiken, SC. In one example, custom optical filters allow accurate colorimetric measurements of Pu in a stream with rapid nitric acid variation. The second example demonstrates simultaneous measurement of Pu and U by chemometric treatment of absorption spectra. The paper concludes with a description of the use of these analyzers to supplement existing technologies in nuclear materials monitoring in processing, reprocessing, and storage facilities.

  16. Tomography of actinides by photofission in bulky radioactive waste packages

    International Nuclear Information System (INIS)

    Quantifying actinides using non-destructive methods, in radioactive waste packages, is a great stake to turn packages towards appropriate storage facility. But the nature of radiations emitted by actinides (alpha radiations) makes the detection of those very difficult for large volume packages characterization. Indeed, the emitted radiation is too weak, either to be detected by emission tomography or to reach required sensitivities. Therefore, it is necessary to turn to an external probing source. Tomography based on detection of delayed neutrons induced by photofission, allows to probe bulky packages. We demonstrate the suitability of this method to an industrial stage. Firstly, we determine and qualify projection matrix which connects measures at reconstructed activity of tomographic picture. Thus, during measurements on a model and a real package, we carry out convincing tomographic reconstructions with real acquisition conditions. More, we prove that it is possible to take all disruptive chemical element into account, for tomographic reconstructions, in order to obtain the best image of activity. So, we propose a finalised tomographic device, integrating a shielding cell, and checking all the activity and distribution activity criterions fixed for acceptance of radioactive waste packages in superficial storage facility. (author)

  17. Electrochemical reduction of actinides oxides in molten salts

    International Nuclear Information System (INIS)

    Reactive metals are currently produced from their oxide by multiple steps reduction techniques. A one step route from the oxide to the metal has been suggested for metallic titanium production by electrolysis in high temperature molten chloride salts. In the so-called FFC process, titanium oxide is electrochemically reduced at the cathode, generating O2- ions, which are converted on a graphite anode into carbon oxide or dioxide. After this process, the spent salt can in principle be reused for several batches which is particularly attractive for a nuclear application in terms of waste minimization. In this work, the electrochemical reduction process of cerium oxide (IV) is studied in CaCl2 and CaCl2-KCl melts to understand the oxide reduction mechanism. Cerium is used as a chemical analogue of actinides. Electrolysis on 10 grams of cerium oxide are made to find optimal conditions for the conversion of actinides oxides into metals. The scale-up to hundred grams of oxide is also discussed. (author)

  18. Energy-Dependent Fission Q Values Generalized for All Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Vogt, R

    2008-09-25

    We generalize Madland's parameterization of the energy release in fission to obtain the dependence of the fission Q values on incident neutron energy, E{sub n}, for all major and minor actinides. These Q(E{sub n}) parameterizations are included in the ENDL2008 release. This paper describes calculations of energy-dependent fission Q values based on parameterizations of the prompt energy release in fission [1], developed by Madland [1] to describe the prompt energy release in neutron-induced fission of {sup 235}U, {sup 238}U, and {sup 239}Pu. The energy release is then related to the energy deposited during fission so that experimentally measurable quantities can be used to obtain the Q values. A discussion of these specific parameterizations and their implementation in the processing code for Monte Carlo neutron transport, MCFGEN, [2] is described in Ref. [3]. We extend this model to describe Q(E) for all actinides, major and minor, in the Evaluated Nuclear Data Library (ENDL) 2008 release, ENDL2008.

  19. Minor actinides transmutation strategies in sodium fast reactors

    International Nuclear Information System (INIS)

    In minor actinides transmutation strategies for fast spectrum reactors, different possibilities regarding the core loading are considered. We study both homogeneous patterns (HOM) with various minor actinides (MA) content values and heterogeneous schemes (HET) with higher percentages of MA (Np, Am and Cm) at the periphery of reactor. We analyze the capability of transmutation of each design and the reactivity coefficients such as the Doppler constant, void worth and the fraction of delayed neutrons. The EVOLCODE2 code is the computational tool used in this study. It is based on MCNPX and ORIGEN/ACAB codes and allows carrying out burn-up calculations to get the isotopic evolution of fuel composition. Among the three strategies studied (HOM 2.5 %, HOM 4% and HET 20 %) for a possible design of a Sodium Cooled Fast Breeder Reactor, the one with better transmutation results is the HOM 4%, which shows higher absolute and relative values (12 Kg-MA/TWe, 29% respectively). Concerning transmutation in blankets with 20% MA content, results show a very little or no transmutation values when considering Np, Am and Cm together, though a positive small value for Np and Am is obtained

  20. Removal of actinides from dilute waste waters using polymer filtration

    International Nuclear Information System (INIS)

    More stringent US Department of Energy discharge regulations for waste waters containing radionuclides (30 pCi/L total alpha) require the development of new processes to meet the new discharge limits for actinide metal ions, particularly americium and plutonium, while minimizing waste. We have been investigating a new technology, polymer filtration, that has the potential for effectively meeting these new limits. Traditional technology uses basic iron precipitation which produces large amounts of waste sludge. The new technology is based on using water-soluble chelating polymers with ultrafiltration for physical separation. The actinide metal ions are selectively bound to the polymer and can not pass through the membrane. Small molecules and nonbinding metals pass through the membrane. Advantages of polymer filtration technology compared to ion, exchange include rapid kinetics because the binding is occurring in a homogenous solution and no mechanical strength requirement on the polymer. We will present our results on the systematic development of a new class of water-soluble chelating polymers and their binding ability from dilute acid to near neutral waters

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

    International Nuclear Information System (INIS)

    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

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

    Energy Technology Data Exchange (ETDEWEB)

    Claro, Luiz H. [Instituto de Estudos Avancados (IEAv/CTA), Sao Jose dos Campos, SP (Brazil)], e-mail: luizhenu@ieav.cta.br

    2009-07-01

    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{sub 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{infinity} 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)

  3. Hollow fibre supported liquid membrane based separations of actinides

    International Nuclear Information System (INIS)

    Renaissance in nuclear energy is poised to make a significant contribution to the diversification of clean energy resources and to reduce the burden of CO2 in atmosphere. Its sustainability lies in using nature's mineral resources in an efficient and environmentally friendly way. One of the major challenges in the nuclear energy programme has, however, been the management of radioactive waste in a manner which allays apprehensions about its adverse impact on the environment. Innovative approaches are being devised internationally to treat spent nuclear fuel as a source of valuables. Separation of long-lived radionuclides such as actinides and fission products from high level radioactive waste is a challenging task for the chemists working on the reprocessing and waste management processes involved at the tail end of nuclear fuel cycle. Amongst the various separation techniques, liquid membrane based separation methods are becoming increasingly popular due to factors such as ligand economy, high efficiency and low power consumption. Techniques such as emulsion liquid membrane and hollow fibre based non-dispersive solvent extraction methods are reported to be more efficient than the solvent extraction based separation methods which have limitations of emulsion/third phase or crud formation. In the present article, an attempt has been made to review the work carried out internationally as well as in the author's laboratory on liquid membrane based actinides separations during last few years with a particular focus on the use of hollow fibre supported liquid membranes. (author)

  4. Actinide production from xenon bombardments of curium-248

    International Nuclear Information System (INIS)

    Production cross sections for many actinide nuclides formed in the reaction of 129Xe and 132Xe with 248Cm 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 136Xe + 248Cm reaction at a similar energy. When compared to the reaction with 136Xe, 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, 129Xe, 132Xe, and 136Xe with 197Au, 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

  5. Diamond for Actinide Traces Detection and Spectrometry in Liquids

    International Nuclear Information System (INIS)

    We describe here a new approach for the detection and identification of actinides (Am, Pu, Cm etc) at very low activity levels in aqueous solution. The measurement consists at first in the electro-precipitation of the actinides ions as insoluble hydroxides directly onto a boron doped nanocrystalline diamond (BNCD) electrode deposited on an α-particle detector (Si or Si-PIN diode), followed by α-particles detection using front-end nuclear electronics. After α-particles counting, spectrometry, the detector can be easily decontaminated using anodization in aqueous solution to be able to be reused at once. The detection limit of the described prototype system can be estimated as low as a few mBq=L (for one day counting) to several mBq=L for 5 h counting and currently achieved energy resolution amounts to ΔEFW HM/Eα = 2.3% for pulse height spectra of 5.486 MeV α-particles emitted by 241Am, measured directly in water. (authors)

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

    International Nuclear Information System (INIS)

    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

  7. Liaison activities with the Institute of Physical Chemistry, Russian Academy of Sciences: FY 1997

    International Nuclear Information System (INIS)

    The Institute of Physical Chemistry of the Russian Academy of Sciences is conducting a program of fundamental and applied research into the chemistry of the actinides and technetium in alkaline media such as are present in the Hanford Site underground waste storage tanks. This work is being coordinated and the results disseminated through a technical liaison maintained at the Pacific Northwest National Laboratory. The technical liaison is performing laboratory studies on plutonium chemistry in alkaline media. The activities at the Institute of Physical Chemistry and through the liaison are pursued to improve understanding of the chemical behavior of key long-lived radioactive elements under current operating and proposed tank waste processing conditions. Both activities are supported by the Efficient Separations and Processing Crosscutting Program under the Office of Science and Technology of the U.S. Department of Energy

  8. Liaison activities with the Institute of Physical Chemistry, Russian Academy of Sciences: FY 1997

    Energy Technology Data Exchange (ETDEWEB)

    Delegard, C.H.; Elovich, R.J.

    1997-09-01

    The Institute of Physical Chemistry of the Russian Academy of Sciences is conducting a program of fundamental and applied research into the chemistry of the actinides and technetium in alkaline media such as are present in the Hanford Site underground waste storage tanks. This work is being coordinated and the results disseminated through a technical liaison maintained at the Pacific Northwest National Laboratory. The technical liaison is performing laboratory studies on plutonium chemistry in alkaline media. The activities at the Institute of Physical Chemistry and through the liaison are pursued to improve understanding of the chemical behavior of key long-lived radioactive elements under current operating and proposed tank waste processing conditions. Both activities are supported by the Efficient Separations and Processing Crosscutting Program under the Office of Science and Technology of the U.S. Department of Energy.

  9. Actinide-to-carbon bonds in Cp2An(alkyl)2, -(butadiene), -(metallacyclopentadiene), and -(cyclobutadiene) complexes

    International Nuclear Information System (INIS)

    The electronic structure of actinide bis(cyclopentadienyl)dialkyl, -butadiene, -metallacyclopentadiene, and -cyclobutadiene complexes is examined. Some Cp*2Th(alkyl)2 complexes display an interesting structural deformation in which a Th-C-C(alkyl) angle (α) opens up considerably. A molecular orbital analysis of Cp2Th(C2H5)2 traces the deformation to the characteristic shape of the d/sub σ/ fragment orbital of Cp2Th(C2H5)+. The potential energy curve for the ethyl pivoting was found to be very soft, with a shallow minimum at α ∼ 1600. Nonrigidity of the ethyl orientation indicates that not only an α hydrogen but also a β hydrogen can come close to Th without a loss of Th-C bond strength; the discussion should provide a theoretical basis for understanding important aspects of C-H activation chemistry involving actinide centers. The Cp2An(s-cis-C4H6) complex was calculated to be 0.74 eV (Th) or 0.42 eV (U) more stable than its s-trans-C4H6 isomer, in contrast to the analogous Cp2Zr(C4H6) complex where the stability of the two geometrical isomers was well-balanced. The σ2,π character of the s-cis-C4H6 coordination to An is somewhat less pronounced than that in the Zr congener, in harmony with the X-ray structures, while highly negative charges are accumulated on the s-cis-C4H6 terminal carbons

  10. Phytosiderophore Effects on Subsurface Actinide Contaminants: Potential for Phytostabilization and Phytoextraction

    Energy Technology Data Exchange (ETDEWEB)

    Ruggiero, Christy

    2005-06-01

    This project seeks to understand the influence of phytosiderophore-producing plants (grasses, including crops such as wheat and barley) on the biogeochemistry of actinide and other metal contaminants in the subsurface environment, and to determine the potential of phytosiderophore-producing plants for phytostabilization and phytoextraction of actinides and some metal soil contaminants. Phytosiderophores are secreted by graminaceous plants such as barley and wheat for the solubilization, mobilization and uptake of Fe and other essential nutrients from soils. The ability for these phytosiderophores to chelate and absorb actinides using the same uptake system as for Fe is being investigated though characterization of actinide-phytosiderophore complexes (independently of plants), and characterization of plant uptake of such complexes. We may also show possible harm caused by these plants through increased chelation of actinides that increase in actinide mobilization & migration in the subsurface environment. This information can then be directly applied by either removal of harmful plants, or can be used to develop plant-based soil stabilization/remediation technologies. Such technologies could be the low-cost, low risk solution to many DOE actinide contamination problems.

  11. 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

  12. Industrial Chemistry and School Chemistry: Making Chemistry Studies More Relevant

    Science.gov (United States)

    Hofstein, Avi; Kesner, Miri

    2006-01-01

    In this paper, we present the development and implementation over the period of more than 15 years of learning materials focusing on industrial chemistry as the main theme. The work was conducted in the Department of Science Teaching at the Weizmann Institute of Science, Israel. The project's general goal was to teach chemistry concepts in the…

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

    International Nuclear Information System (INIS)

    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

  14. Conjugates of Actinide Chelator-Magnetic Nanoparticles for Used Fuel Separation Technology

    Energy Technology Data Exchange (ETDEWEB)

    Qiang, You; Paszczynski, Andrzej; Rao, Linfeng

    2011-10-30

    The actinide separation method using magnetic nanoparticles (MNPs) functionalized with actinide specific chelators utilizes the separation capability of ligand and the ease of magnetic separation. This separation method eliminated the need of large quantity organic solutions used in the liquid-liquid extraction process. The MNPs could also be recycled for repeated separation, thus this separation method greatly reduces the generation of secondary waste compared to traditional liquid extraction technology. The high diffusivity of MNPs and the large surface area also facilitate high efficiency of actinide sorption by the ligands. This method could help in solving the nuclear waste remediation problem.

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

    International Nuclear Information System (INIS)

    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

  16. From Matter to Life:Chemistry?Chemistry!

    Institute of Scientific and Technical Information of China (English)

    Jean-Marie; LEHN

    2007-01-01

    1 Results Animate as well as inanimate matter,living organisms as well as materials,are formed of molecules and of the organized entities resulting from the interaction of molecules with each other.Chemistry provides the bridge between the molecules of inanimate matter and the highly complex molecular architectures and systems which make up living organisms. Synthetic chemistry has developed a very powerful set of methods for constructing ever more complex molecules.Supramolecular chemistry seeks to con...

  17. Green chemistry: A tool in Pharmaceutical Chemistry

    OpenAIRE

    Smita Talaviya; Falguni Majumdar

    2012-01-01

    Green chemistry expresses an area of research developing from scientific discoveries about pollution awareness and it utilizes a set of principles that reduces or eliminates the use or generation of hazardous substances in all steps of particular synthesis or process. Chemists and medicinal scientists can greatly reduce the risk to human health and the environment by following all the valuable principles of green chemistry. The most simple and direct way to apply green chemistry in pharmaceut...

  18. 7th Nuclear Chemistry, Radiochemistry and Radiation Chemistry Symposium

    International Nuclear Information System (INIS)

    The conference heard a total of 58 papers of which 56 were incorporated in INIS, namely those dealing with radioimmunoassay, radiation shielding materials, and radiochemistry of technetium, iodine, uranium, rare earths and actinides. (MR)

  19. Chemistry Rocks: Redox Chemistry as a Geologic Tool.

    Science.gov (United States)

    Burns, Mary Sue

    2001-01-01

    Applies chemistry to earth science, uses rocks in chemistry laboratories, and teaches about transition metal chemistry, oxidation states, and oxidation-reduction reactions from firsthand experiences. (YDS)

  20. Actinides and rare earths complexation with adenosine phosphate nucleotides

    International Nuclear Information System (INIS)

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

  1. Scissors strength in the quasi-continuum of actinides

    Directory of Open Access Journals (Sweden)

    Guttormsen M.

    2014-03-01

    Full Text Available The M1-scissors resonance has been measured for the first time in the quasi-continuum of actinides. The strength and position of the resonances in 231,232,233Th were determined by particle-γ coincidences using deuteron induced reactions on a 232Th target. The residual nuclei show a strong integrated strength of BM1 = 9 − 11 µn2 in the Eγ = 1.0 − 3.5 MeV region. The presence of the scissors resonance modifies significantly the (n,γ cross section, which has impact on fuel-cycle simulations of fast nuclear reactors and nucleosynthesis in explosive stellar environments.

  2. Instrumentation for high-efficiency, high-sensitivity actinide analysis

    International Nuclear Information System (INIS)

    This is the final report of a 3-year project. We have developed a high-efficiency thermal ionization source that provides one to two orders of magnitude improvement in sample utilization efficiency in comparison with the traditional filament-type ion source currently used in thermal ionization mass spectrometry. This improved sample utilization efficiency results in a proportional increase in sample throughput and proportional decrease in analysis time. Coupling this source with a quadrupole mass spectrometer results in an instrument system for high-efficiency actinide analysis and other applications. In addition to its high efficiency, the sample used in this source can be much smaller than that in previous tube-type sources. The compact structure of the cavity makes it more applicable to any type of mass spectrometer and the whole instrument is small and transportable

  3. Two new animal models for actinide toxicity studies

    International Nuclear Information System (INIS)

    Two small rodent species, the grasshopper mouse (Onychomys leucogaster) and the deer mouse (Peromyscus maniculatus) have tenacious retention in the liver and skeleton of plutonium and americium. The retention following intraperitoneal injection of Pu and Am in citrate solution ranged from 20 to 47% (liver) and 19 to 42% (skeleton), relatively independent of post-injection times, varying from 30 to 125 days. Based on observations extended to 125 days post-injection, the biological half-times appeared to be long. Both of these rodents are relatively long-lived (median lifespans of approximately 1400 days), breed well in captivity, and adapt suitably to laboratory conditions. It is suggested that these two species of mice, in which plutonium is partitioned between the skeleton and liver in a manner similar to that of man, may be useful animal models for actinide toxicity studies

  4. Fabrication of indigenous computer controlled photoacoustic spectrometer for actinide spectroscopy

    International Nuclear Information System (INIS)

    The photoacoustic spectroscopy (PAS) monitoring the non-radiative de-excitation process is a powerful tool for investigating the absorption spectra of almost any type of samples like opaque solids, turbid solutions etc. Actinide compounds due to high probability of non-radiative relaxation process are good candidates for PAS investigations and also without any need for good optical quality crystals of these compounds. In addition, this technique is extremely useful for determination of thermal properties like thermal conductivity, diffusivity and related properties like phase transitions, thickness of thin film etc. In the present paper details of fabrication of indigenous PAS unit using low cost easily available components and interfacing this unit to a personal computer are given

  5. Flammability Analysis For Actinide Oxides Packaged In 9975 Shipping Containers

    Energy Technology Data Exchange (ETDEWEB)

    Laurinat, James E.; Askew, Neal M.; Hensel, Steve J.

    2013-03-21

    Packaging options are evaluated for compliance with safety requirements for shipment of mixed actinide oxides packaged in a 9975 Primary Containment Vessel (PCV). Radiolytic gas generation rates, PCV internal gas pressures, and shipping windows (times to reach unacceptable gas compositions or pressures after closure of the PCV) are calculated for shipment of a 9975 PCV containing a plastic bottle filled with plutonium and uranium oxides with a selected isotopic composition. G-values for radiolytic hydrogen generation from adsorbed moisture are estimated from the results of gas generation tests for plutonium oxide and uranium oxide doped with curium-244. The radiolytic generation of hydrogen from the plastic bottle is calculated using a geometric model for alpha particle deposition in the bottle wall. The temperature of the PCV during shipment is estimated from the results of finite element heat transfer analyses.

  6. Decorporation of actinides: a review of recent research

    International Nuclear Information System (INIS)

    This paper reports progress on some of the research priorities identified in the Guidebook for the Treatment of Accidental Contamination of Workers published in 1992. It concludes: that the oral administration of DTPA could be an effective procedure for plutonium (Pu) and americium (Am) inhaled as nitrates; that 3,4,3-LI (1,2-HOPO) is the most effective siderophore analogue yet tested for the decorporation of these actinides, and thorium (Th); and that for thorium the efficacy of treatment will be strongly dependent on the radionuclide, and hence mass, likely to be incorporated under different exposure scenarios. No effective treatment regimens appear to be available for neptunium (Np) and uranium (U). (orig.)

  7. Actinide-only burnup credit for spent fuel transport

    International Nuclear Information System (INIS)

    A conservative methodology is described that would allow taking credit for burn up in the criticality safety analysis of spent nuclear fuel packages. Requirements for its implementation include isotopic and criticality validation, generation of package loading criteria using limiting parameters, and assembly burn up verification by measurement. The method allows credit for the changes in the 234U, 235U, 236U, 238U, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, and 241Am concentrations with burnup. No credit for fission product neutron absorbers is taken. Analyses are included regarding the methodology's financial benefits and conservative margin. It is estimated that the proposed actinide-only burnup credit methodology would save 20% of the transport costs. Nevertheless, the methodology includes a substantial margin. Conservatism due to the isotopic correction factors, limiting modelling parameters, limiting axial profiles and exclusion of the fission products ranges from 10 to 25% k. (author)

  8. Facilities for preparing actinide or fission product-based targets

    CERN Document Server

    Sors, M

    1999-01-01

    Research and development work is currently in progress in France on the feasibility of transmutation of very long-lived radionuclides such as americium, blended with an inert medium such as magnesium oxide and pelletized for irradiation in a fast neutron reactor. The process is primarily designed to produce ceramics for nuclear reactors, but could also be used to produce targets for accelerators. The Actinide Development Laboratory is part of the ATALANTE complex at Marcoule, where the CEA investigates reprocessing, liquid and solid waste treatment and vitrification processes. The laboratory produces radioactive sources; after use, their constituents are recycled, notably through R and D programs requiring such materials. Recovered americium is purified, characterized and transformed for an experiment known as ECRIX, designed to demonstrate the feasibility of fabricating americium-based ceramics and to determine the reactor transmutation coefficients.

  9. 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

  10. EXAFS studies of sodium silicate glasses containing dissolved actinides

    International Nuclear Information System (INIS)

    Sodium silicate glasses containing dissolved Th, U, Np, and Pu have been studied using the EXAFS technique. Th4+, U4+, Np4+, and Pu4+ ions in the silicate glasses are 8-fold coordinated to oxygen neighbors. The higher valent U6+ and Np5+ ions have complex local symmetries. The U6+ ions appear in a uranyl configuration with 2 oxygen atoms at 1.85A and 4 at 2.25A from the U ion. The Np5+ local symmetry is more complex and difficult to determine uniquely. The U6+ glasses show substantial clustering of the uranium atoms. A structural model, with nearly planar uranyl sheets sandwiched between alkali and silica layers, is used to explain the U6+ EXAFS data. This model allows us to understand why U6+ ions are much more soluble in the glasses than the actinide 4+ ions. 4 references, 2 figures

  11. The electronic g matrix of some actinide complexes

    International Nuclear Information System (INIS)

    Complete text of publication follows: The molecular g-factors are crucial parameters in Electron Paramagnetic Resonance (EPR) spectroscopy. They parametrize the Zeeman effect that involves the interaction of a spin magnetic moment with a magnetic field. Before the 90's, g-factors were mostly calculated by semi-empirical methods while in the last decade, ab initio techniques have been developed based on wave functions or density functional theories either using a sum over states (SOS) expansion or using response theory [1]. We have recently proposed an alternative method based on wave function theory including spin-orbit effects by the SO-RASSI method [2]. This method has been applied with success to small molecules containing atoms until the third series of the transition metals and to a mixed-valence bimetallic complex[3] and in this work, it is applied to actinide complexes with a 5f1 configuration. To our knowledge, only few attempts have been made to calculate g-factors of actinide complexes from first principles [4, 5]. Relativistic effects in actinide complexes are important, so the deviation of g-factors from the value of the free electron is large and can even become negative. Most of the experiments measuring magnetic properties of actinide complexes date from the sixties. EPR and magnetic susceptibilities give the absolute values of the g-factors while experiment using circularly polarized light provide the sign of the product of the three factors. Magnetic properties of these compounds are easily understood using ligand field theory models. In the first part of this presentation, we will discuss the arbitrary character of the g-matrix and specially of the effect of phase factors and of the choice of the spin quantification axis and we will show that only the G tensor gg* has a physical significance. In the second part, equilibrium distances, excitation energies and g-factors of the AnXq-6 series with An = Pa,U,Np and X = F,Cl,Br are calculated using the

  12. Angular distributions in the neutron-induced fission of actinides

    CERN Multimedia

    In 2003 the n_TOF Collaboration performed the fission cross section measurement of several actinides ($^{232}$Th, $^{233}$U, $^{234}$U, $^{237}$Np) at the n_TOF facility using an experImental setup made of Parallel Plate Avalanche Counters (PPAC). The method based on the detection of the 2 fragments in coincidence allowed to clearly disentangle the fission reactions among other types of reactions occurring in the spallation domain. We have been therefore able to cover the very broad neutron energy range 1eV-1GeV, taking full benefit of the unique characteristics of the n_TOF facility. Figure 1 shows an example obtained in the case of $^{237}$Np where the n_ TOF measurement showed that the cross section was underestimated by a large factor in the resonance region.

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

    International Nuclear Information System (INIS)

    Partitioning the actinides in spent fuel and transmuting them in actinide-burning liquid-metal reactors (ALMRs) is a potential method of reducing public risks from the geologic disposal of nuclear waste. In this paper, the authors present a comparison of radionuclide releases from burial at Yucca Mountain of spent fuel and of ALMR wastes. Two waste disposal schemes are considered. In each, the heat generation of the wastes at emplacement is 9.88 x 107 W, the maximum for the repository. In the first scheme, the repository contains 86,700 tonnes of initial heavy metal (IHM) of light water reactor (LWR) spent fuel. In the second scheme, all current LWRs operate for a 40-yr lifetime, producing a total of 84,000 tonnes IHM of spent fuel. This spent fuel is treated using a pyrochemical process in which 98.4% of the uranium and 99.8% of the neptunium, plutonium, americium, and curium are extracted and fabricated into ALMR fuel, with the reprocessing wastes destined for the repository. The ALMR requires this fuel for its startup and first two reloads; thereafter, it is self-sufficient. Spent ALMR fuel is also pyrochemically reprocessed: 99.9% of the transuranics is recovered and recycled into ALMR fuel, and the wastes are placed in the repository. Thus, in the second scheme, the repository contains the wastes from reprocessing all of the LWR spent fuel plus the maximum amount of ALMR reprocessing wastes allowed in the repository based on its heat generation limit

  14. Constitutional dynamic chemistry: bridge from supramolecular chemistry to adaptive chemistry.

    Science.gov (United States)

    Lehn, Jean-Marie

    2012-01-01

    Supramolecular chemistry aims at implementing highly complex chemical systems from molecular components held together by non-covalent intermolecular forces and effecting molecular recognition, catalysis and transport processes. A further step consists in the investigation of chemical systems undergoing self-organization, i.e. systems capable of spontaneously generating well-defined functional supramolecular architectures by self-assembly from their components, thus behaving as programmed chemical systems. Supramolecular chemistry is intrinsically a dynamic chemistry in view of the lability of the interactions connecting the molecular components of a supramolecular entity and the resulting ability of supramolecular species to exchange their constituents. The same holds for molecular chemistry when the molecular entity contains covalent bonds that may form and break reversibility, so as to allow a continuous change in constitution by reorganization and exchange of building blocks. These features define a Constitutional Dynamic Chemistry (CDC) on both the molecular and supramolecular levels.CDC introduces a paradigm shift with respect to constitutionally static chemistry. The latter relies on design for the generation of a target entity, whereas CDC takes advantage of dynamic diversity to allow variation and selection. The implementation of selection in chemistry introduces a fundamental change in outlook. Whereas self-organization by design strives to achieve full control over the output molecular or supramolecular entity by explicit programming, self-organization with selection operates on dynamic constitutional diversity in response to either internal or external factors to achieve adaptation.The merging of the features: -information and programmability, -dynamics and reversibility, -constitution and structural diversity, points to the emergence of adaptive and evolutive chemistry, towards a chemistry of complex matter.

  15. Actinide coordination sphere in various U, Np and Pu nitrato coordination complexes

    International Nuclear Information System (INIS)

    Waste management of nuclear fuel represents one of the major environmental concerns of the decade. To recycle fissile valuable materials, intimate knowledge of complexation mechanisms involved in the solvent extraction processes is indispensable. Evolution of the actinide coordination sphere of AnO2(NO3)2TBP-type complexes (an = U, Np, Pu; TBP = tributylphosphate) with the actinide valence state have been probed by XAS at the metal LIII edge. Dramatic changes in the actinide coordination sphere appeared when the An(VI) metal is reduced to An(IV). However, no significant evolution in the actinide environment has been noticed across the series UO22+, NpO22+ and PuO22+. (au)

  16. Organophosphorus reagents in actinide separations: Unique tools for production, cleanup and disposal

    Energy Technology Data Exchange (ETDEWEB)

    Nash, K. L.

    2000-01-12

    Interactions of actinide ions with phosphate and organophosphorus reagents have figured prominently in nuclear science and technology, particularly in the hydrometallurgical processing of irradiated nuclear fuel. Actinide interactions with phosphorus-containing species impact all aspects from the stability of naturally occurring actinides in phosphate mineral phases through the application of the bismuth phosphate and PUREX processes for large-scale production of transuranic elements to the development of analytical separation and environment restoration processes based on new organophosphorus reagents. In this report, an overview of the unique role of organophosphorus compounds in actinide production, disposal, and environment restoration is presented. The broad utility of these reagents and their unique chemical properties is emphasized.

  17. Basic research on solvent extraction of actinide cations with diamide compounds

    Energy Technology Data Exchange (ETDEWEB)

    Sasaki, Yuji [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1998-11-01

    Newly synthesized 4 diamide compounds were tested for solvent extraction of actinide cations. It is obvious that N,N`-dimethyl-N,N`-dihexyl-3-oxapentanediamide (DMDHOPDA) can extract Eu(III), Th(IV), U(VI), Np(V), and Am(III) into organic solvent. Other 3 diamides hardly extract actinide ions, which is supposed that the reasons come from the difference of their chemical structures. In the synergistic extraction with a diamide and thenoyltrifluoroacetone (TTA), all diamides work as a extractant. Furthermore, by examining extracted species, it was confirmed that there are 4 kinds of chemical species of actinides with diamide and TTA. Finally, the mutual separation method of actinide (III), (IV), (V) and (VI) ions by solvent extraction using DMDHOPDA and TTA were developed. (author). 147 refs.

  18. Fission product and actinide data evaluations for ENDF/B--V

    Energy Technology Data Exchange (ETDEWEB)

    Schenter, R.E.

    1978-05-01

    The planned content and performance of fission product and actinide nuclide evaluations for the ENDF/B-V collection of data are reviewed. Representative values of parameters for a few nuclides are shown. 10 figures, 5 tables. (RWR)

  19. Nuclear data uncertainty analysis on a minor actinide burner for transmuting spent fuel

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hangbok

    1998-08-01

    A comprehensive sensitivity and uncertainty analysis was performed on a 1200 MWt minor actinides burner designed for a low burnup reactivity swing, negative doppler coefficient, and low sodium void worth. Sensitivities of the performance parameters were generated using depletion perturbation methods for the constrained close fuel cycle of the reactor. The uncertainty analysis was performed using the sensitivity and covariance data taken from ENDF-B/V and other published sources. The uncertainty analysis of a liquid metal reactor for burning minor actinide has shown that uncertainties in the nuclear data of several key minor actinide isotopes can introduce large uncertainties in the predicted performance of the core. The relative uncertainties in the burnup swing, doppler coefficient, and void worth were conservatively estimated to be 180 %, 97 %, and 46 %, respectively. An analysis was performed to prioritize the minor actinide reactions for reducing the uncertainties. (author). 41 refs., 17 tabs., 1 fig.

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

    International Nuclear Information System (INIS)

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

  1. Immobilization of actinide wastes in ceramics for long-term disposal

    OpenAIRE

    Soe, Khin Soe

    2006-01-01

    Glass can undergo devitrification with time and the incorporation of actinides with their alpha-decay in MeV-range due to compacted alpha-recoiled irradiation over 10^6 years storage leads to expansion and phase transformation of nuclear waste glasses. Moreover, the maximum tolerable amount of actinides that can be incorporated in glass is approximately 5%. The development of ceramics adapted for nuclear-waste immobilization is the focus of this dissertation. The yttria-stabilized zirconia c...

  2. An instrument for the investigation of actinides with spin resolved photoelectron spectroscopy and bremsstrahlung isochromat spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Yu, S.-W. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Tobin, J. G. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Chung, B. W. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

    2011-01-01

    A new system for spin resolved photoelectron spectroscopy and bremsstrahlung isochromat spectroscopy has been built and commissioned at Lawrence Livermore National Laboratory for the investigation of the electronic structure of the actinides.Actinide materials are very toxic and radioactive and therefore cannot be brought to most general user facilities for spectroscopic studies. The technical details of the new system and preliminary data obtained therein will be presented and discussed.

  3. Multidimensionally-constrained relativistic mean-field study of triple-humped barriers in actinides

    OpenAIRE

    Zhao, Jie; Lu, Bingnan; Vretenar, Dario; Zhao, En-Guang; Zhou, Shan-Gui

    2014-01-01

    Potential energy surfaces (PES's) of actinide nuclei are characterized by a two-humped barrier structure. At large deformations beyond the second barrier the occurrence of a third one was predicted by Mic-Mac model calculations in the 1970s, but contradictory results were later reported. In this paper, triple-humped barriers in actinide nuclei are investigated with covariant density functional theory (CDFT). Calculations are performed using the multidimensionally-constrained relativistic mean...

  4. The complex formation of selected actinides (U, Np, Cm) with microbial ligands

    International Nuclear Information System (INIS)

    One of the urgent tasks in the field of nuclear technology is the final storage of radioactive substances. As a part of the safety requirements the protection of humans and the environment from the danger of radioactive substances in case of the release from the final storage is essential. For performing long-term safety calculations the detailed understanding of the physico-chemical effects and influences which cause the mobilisation and transport of actinides are necessary. The presented work was a discrete part of a project, which was focused on the clarification of the influence of microorganisms on the migration of actinides in case of the release of actinides from a final storage. The influence of microbial produced substances on the mobilisation of selected actinides was studied thereby. The microbial produced substances studied in this project were synthesized by bacteria from the Pseudomonas genus under special conditions. Fluorescent Pseudomonads secrete bacterial pyoverdin-type siderophores with a high potential to complex and transport metals, especially iron(III). The aim of the project was to determine how and under which conditions the bioligands are able to complex also radioactive substances and therefore to transport them. For this work the alpha-emitting actinides uranium, curium and neptunium were chosen because their long-life cycle and their radiotoxicity are a matter of particular interest. This work dealed with the interaction of the actinides U(VI), Np(V) and Cm(III) with model ligands simulating the functionality of the pyoverdins. So, such bioligands can essentially influence the behaviour of actinides in the environment. The results of this work contribute to a better understanding and assessment of the influence of the microbial ligands to the mobilisation and migration of the radionuclides. The outcomes could be used to quantify the actinide-mobilising effect of the bioligands, which are released, for example, in the vicinity of a

  5. Production of actinide isotopes in simulated PWR fuel and their influence on inherent neutron emission

    International Nuclear Information System (INIS)

    This report describes calculations that examine the sensitivity of actinide isotopes to various reactor parameters. The impact of actinide isotope build-up, depletion, and decay on the neutron source rate in a spent-fuel assembly is determined, and correlations between neutron source rates and spent-fuel characteristics such as exposure, fissile content, and plutonium content are established. The application of calculations for evaluating experimental results is discussed

  6. SACSESS – the EURATOM FP7 project on actinide separation from spent nuclear fuels

    OpenAIRE

    Bourg Stéphane; Geist Andreas; Narbutt Jerzy

    2015-01-01

    Recycling of actinides by their separation from spent nuclear fuel, followed by transmutation in fast neutron reactors of Generation IV, is considered the most promising strategy for nuclear waste management. Closing the fuel cycle and burning long-lived actinides allows optimizing the use of natural resources and minimizing the long-term hazard of high-level nuclear waste. Moreover, improving the safety and sustainability of nuclear power worldwide. This paper presents the activities strivin...

  7. Radiochemical separation of actinides for their determination in environmental samples and waste products

    Energy Technology Data Exchange (ETDEWEB)

    Gleisberg, B. [Nuclear Engineering and Analytics Rossendorf, Inc. (VKTA), Dresden (Germany)

    1997-03-01

    The determination of low level activities of actinides in environmental samples and waste products makes high demands on radiochemical separation methods. Artificial and natural actinides were analyzed in samples form the surrounding areas of NPP and of uranium mines, incorporation samples, solutions containing radioactive fuel, solutions and solids resutling from the process, and in wastes. The activities are measured by {alpha}-spectrometry and {gamma}-spectrometry. (DG)

  8. DAE-BRNS symposium on spectroscopy of lanthanides and actinides (SLA-99)

    International Nuclear Information System (INIS)

    Spectroscopy of lanthanides and actinides, due to the rich and complex interactions of the f electrons, is of immense interest to basic sciences and technology. This volume covers both basic and applied aspects of the spectroscopy of lanthanides and actinides and also include the recent developments and emerging areas. The papers have been classified in several broad categories namely theoretical studies, high resolution spectroscopy, laser spectroscopy, solid state spectroscopy, analytical spectroscopy, optics and instrumentation and applications. Papers relevant to INIS are indexed separately

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1977-01-01

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

  10. Why Faster is Better : On Minor Actinide Transmutation in Hard Neutron

    OpenAIRE

    Westlén, Daniel

    2007-01-01

    In this thesis, options for efficient transmutation of transuranium elements are discussed. The focus is on plutonium, americium and curium mainly because of their long-term contribution to the radiotoxicity of spent nuclear fuel. Two innovative helium-cooled core designs are proposed, dedicated to the transmutation of actinides. The performance of the more promising of the two is studied in realistic transient fuel cycle scenarios. During the 1150 day irradiation cycle, a minor actinide cons...

  11. Green chemistry: A tool in Pharmaceutical Chemistry

    Directory of Open Access Journals (Sweden)

    Smita Talaviya

    2012-07-01

    Full Text Available Green chemistry expresses an area of research developing from scientific discoveries about pollution awareness and it utilizes a set of principles that reduces or eliminates the use or generation of hazardous substances in all steps of particular synthesis or process. Chemists and medicinal scientists can greatly reduce the risk to human health and the environment by following all the valuable principles of green chemistry. The most simple and direct way to apply green chemistry in pharmaceuticals is to utilize eco-friendly, non-hazardous, reproducible and efficient solvents and catalysts in synthesis of drug molecules, drug intermediates and in researches involving synthetic chemistry. Microwave synthesis is also an important tool of green chemistry by being an energy efficient process.

  12. Environmental chemistry: Volume A

    Energy Technology Data Exchange (ETDEWEB)

    Yen, T.F.

    1999-08-01

    This is an extensive introduction to environmental chemistry for engineering and chemical professionals. The contents of Volume A include a brief review of basic chemistry prior to coverage of litho, atmo, hydro, pedo, and biospheres.

  13. CHINESE JOURNAL OF CHEMISTRY

    Institute of Scientific and Technical Information of China (English)

    2000-01-01

    @@Chinese Journal of Chemistry is an international journal published in English by the Chinese Chemical Society with its editorial office hosted by Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences.

  14. Reduction of minor actinides for recycling in a light water reactor

    International Nuclear Information System (INIS)

    The aim of actinide transmutation from spent nuclear fuel is the reduction in mass of high-level waste which must be stored in geological repositories and the lifetime of high-level waste; these two achievements will reduce the number of repositories needed, as well as the duration of storage. The present work is directed towards the evaluation of an advanced nuclear fuel cycle in which the minor actinides (Np, Am and Cm) could be recycled to remove most of the radioactive material; a reference of actinides production in standard nuclear fuel of uranium at the end of its burning in a BWR is first established, after a design of fuel rod containing 6% of minor actinides in a matrix of uranium from the enrichment lines is proposed, then 4 fuel rods of standard uranium are replaced by 4 actinides bars to evaluate the production and transmutation of them and finally the minor actinides reduction in the fuel is evaluated. In the development of this work the calculation tool are the codes: Intrepin-3, Casmo-4 and Simulate-3. (Author)

  15. Gross actinide preconcentration using phosphonate-based ligand and cloud point extraction

    International Nuclear Information System (INIS)

    A procedure for the effective separation and determination of the most abundant actinides relevant to the nuclear industry (U, Th, Np, Pu and Am) was developed based on cloud point extraction (CPE) using H2DEH[MDP] (P,P-di-(2-ethylhexyl) methanediphosphonic acid) as a ligand. The extractability of actinides with varying concentrations of nitric acid and hydrochloric acid were assessed. The robustness of the method was demonstrated for environmental matrices such as reference materials and spiked liquid samples for the quantification of the gross actinide content. This analytical strategy may replace traditional sample preparation techniques used in radiological methods for gross measurements of radioactivity, and may act as a rapid screening tool in emergency situations. The developed method is a greener alternative to common radiochemical sample preparation techniques such as co-precipitation or evaporation. The formation of a small-volume surfactant-rich phase containing the complexed actinides enables rapid, highly selective and great enrichment of the analytes in this phase. The proposed method shows good extraction and separation yield compared to existing methods, since the surfactant-rich phase is soluble in water and can therefore be redispersed quantitatively in a medium compatible with mass spectrometry while providing fast isolation of the actinide content. Separation of actinides can be achieved after by wet ashing of the surfactant-rich phase obtained by CPE if coupled to the proper radiochemical separation scheme. (author)

  16. Electrochemical separation of actinides and fission products in molten salt electrolyte

    Science.gov (United States)

    Gay, R. L.; Grantham, L. F.; Fusselman, S. P.; Grimmett, D. L.; Roy, J. J.

    1995-09-01

    Molten salt electrochemical separation may be applied to accelerator-based conversion (ABC) and transmutation systems by dissolving the fluoride transport salt in LiCl-KCl eutectic solvent. The resulting fluoride-chloride mixture will contain small concentrations of fission product rare earths (La, Nd, Gd, Pr, Ce, Eu, Sm, and Y) and actinides (U, Np, Pu, Am, and Cm). The Gibbs free energies of formation of the metal chlorides are grouped advantageously such that the actinides can be deposited on a solid cathode with the majority of the rare earths remaining in the electrolyte. Thus, the actinides are recycled for further transmutation. Rockwell and its partners have measured the thermodynamic properties of the metal chlorides of interest (rare earths and actinides) and demonstrated separation of actinides from rare earths in laboratory studies. A model is being developed to predict the performance of a commercial electrochemical cell for separations starting with PUREX compositions. This model predicts excellent separation of plutonium and other actinides from the rare earths in metal-salt systems.

  17. Calculation of binary phase diagrams between the actinide elements, rare earth elements, and transition metal elements

    International Nuclear Information System (INIS)

    Attempts were made to apply the Kaufman method of calculating binary phase diagrams to the calculation of binary phase diagrams between the rare earths, actinides, and the refractory transition metals. Difficulties were encountered in applying the method to the rare earths and actinides, and modifications were necessary to provide accurate representation of known diagrams. To calculate the interaction parameters for rare earth-rare earth diagrams, it was necessary to use the atomic volumes for each of the phases: liquid, body-centered cubic, hexagonal close-packed, and face-centered cubic. Determination of the atomic volumes of each of these phases for each element is discussed in detail. In some cases, empirical means were necessary. Results are presented on the calculation of rare earth-rare earth, rare earth-actinide, and actinide-actinide diagrams. For rare earth-refractory transition metal diagrams and actinide-refractory transition metal diagrams, empirical means were required to develop values for the enthalpy of vaporization for rare earth elements and values for the constant (C) required when intermediate phases are present. Results of using the values determined for each element are presented

  18. Organic chemistry experiment

    Energy Technology Data Exchange (ETDEWEB)

    Mun, Seok Sik

    2005-02-15

    This book deals with organic chemistry experiments, it is divided five chapters, which have introduction, the way to write the experiment report and safety in the laboratory, basic experiment technic like recrystallization and extraction, a lot of organic chemistry experiments such as fischer esterification, ester hydrolysis, electrophilic aromatic substitution, aldol reaction, benzoin condensation, wittig reaction grignard reaction, epoxidation reaction and selective reduction. The last chapter introduces chemistry site on the internet and way to find out reference on chemistry.

  19. Frontiers in Gold Chemistry

    OpenAIRE

    Mohamed, Ahmed A.

    2015-01-01

    Basic chemistry of gold tells us that it can bond to sulfur, phosphorous, nitrogen, and oxygen donor ligands. The Frontiers in Gold Chemistry Special Issue covers gold complexes bonded to the different donors and their fascinating applications. This issue covers both basic chemistry studies of gold complexes and their contemporary applications in medicine, materials chemistry, and optical sensors. There is a strong belief that aurophilicity plays a major role in the unending applications of g...

  20. Green Chemistry and Education.

    Science.gov (United States)

    Hjeresen, Dennis L.; Schutt, David L.; Boese, Janet M.

    2000-01-01

    Many students today are profoundly interested in the sustainability of their world. Introduces Green Chemistry and its principles with teaching materials. Green Chemistry is the use of chemistry for pollution prevention and the design of chemical products and processes that are environmentally benign. (ASK)

  1. Effects of humic substances on the migration of radionuclides: Complexation of actinides with humic substances. 1. progress report

    International Nuclear Information System (INIS)

    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. This programme is a continuation of the activities of the COCO group in the second phase of the CEC-MIRAGE project. (orig.)

  2. Actinides reduction by recycling in a thermal reactor; Reduccion de actinidos por reciclado en un reactor termico

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-10-15

    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)

  3. Sensitivity analysis of minor actinides transmutation to physical and technological parameters

    Directory of Open Access Journals (Sweden)

    Kooyman Timothée

    2015-01-01

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

  4. Surface chemistry essentials

    CERN Document Server

    Birdi, K S

    2013-01-01

    Surface chemistry plays an important role in everyday life, as the basis for many phenomena as well as technological applications. Common examples range from soap bubbles, foam, and raindrops to cosmetics, paint, adhesives, and pharmaceuticals. Additional areas that rely on surface chemistry include modern nanotechnology, medical diagnostics, and drug delivery. There is extensive literature on this subject, but most chemistry books only devote one or two chapters to it. Surface Chemistry Essentials fills a need for a reference that brings together the fundamental aspects of surface chemistry w

  5. The New Color of Chemistry: Green Chemistry

    Directory of Open Access Journals (Sweden)

    Zuhal GERÇEK

    2012-01-01

    Full Text Available Green chemistry which is the new application of chemistry rules provides solutions to problems that mankind is faced with climate changes, sustainable agriculture, energy, toxics, depletion of natural sources e.g. designing new chemicals and processes that production and utilization of hazardous matters. So, it is the indispensible tool for sustainable development. Current and future chemists should consider the human health and ecological issues in their professional life. In order to provide a solution for this requirement, green chemistry rules and under standings should be primarily taken in the university curriculum and at all educational levels.

  6. Annual report 1984 Chemistry Department

    International Nuclear Information System (INIS)

    This report contains a brief survey of the main activities in the Chemistry Department. All articles and reports published and lectures given in 1984 are presented. The facilities and equipment are mentioned briefly. The activities are divided into the following groups: radioisotope chemistry, analytical- and organic chemistry , environmental chemistry, polymer chemistry, geochemistry and waste disposal, radical chemistry, positron annihilation, mineral processing, and general. (author)

  7. Minor actinides partitioning and transmutation technology in France

    International Nuclear Information System (INIS)

    real solutions derived from the La Hague process, the CEA demonstrated the feasibility of extracting minor actinides using a process that can be extrapolated on the industrial scale. The CEA also conducted programmes proving the technical feasibility of the elimination of minor actinides by transmutation. With the help of the CNRS (France) in particular we developed high strength ceramic matrices to contain any radionuclides extracted by enhanced separation that might be deemed unsuitable for transmutation. (author)

  8. Summary Report for April, May and June, 1951, Chemistry Division, Section C-1

    Energy Technology Data Exchange (ETDEWEB)

    Manning, W. M. [Argonne National Lab. (ANL), Argonne, IL (United States). Chemistry Division; Osborne, D. W. [Argonne National Lab. (ANL), Argonne, IL (United States). Chemistry Division

    1951-08-01

    This is a summary report for April, May and June, 1951, in the Chemistry Division, Section C-1 of Argonne National Laboratory. Topics include Nuclear Chemistry and Radiochemistry with specifics about the following: 1) U238 (n,2n) Cross Section WIthin a Uranium Slug, and 2) Possible Occurrence of Si32 in Nature. Basic Chemistry is also covered, going into the following subjects: 1) Heats of Solution of Salts in Organic Solvents, 2) Effect of Coordination on Absorption Spectra of Anions, 3) Entropy, Enthalpy, and Heat Capacity of Thorium Dioxide from 10 to 300°K, 4) The Thermodynamics of Neptunium Ions, 5) Migration of Ions in Ion-Exchange Resins During Electrolysis, and 5) Mutual Separation of Lanthanides and Actinides by Solvent Extraction Techniques.

  9. Reversible optical sensor for the analysis of actinides in solution; Capteur optique reversible pour l'analyse des actinides en solution

    Energy Technology Data Exchange (ETDEWEB)

    Lesage, B.; Picard, S. [CEA Marcoule, Dept. de Radiochimie et Procedes, Service de Chimie des Procedes de Separation, Lab. de Chimie des Actinides, 30 (France); Serein-Spirau, F.; Lereporte, J.P. [Ecole Nationale Superieure de Chimie de Montpellier (ENSCM), CNRS UMR 5076, Lab. Heterochimie Moleculaire et Macromoleculaire, 34 - Montpellier (France)

    2007-07-01

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

  10. Spectroscopic and computational investigation of actinium coordination chemistry

    Science.gov (United States)

    Ferrier, Maryline G.; Batista, Enrique R.; Berg, John M.; Birnbaum, Eva R.; Cross, Justin N.; Engle, Jonathan W.; La Pierre, Henry S.; Kozimor, Stosh A.; Lezama Pacheco, Juan S.; Stein, Benjamin W.; Stieber, S. Chantal E.; Wilson, Justin J.

    2016-08-01

    Actinium-225 is a promising isotope for targeted-α therapy. Unfortunately, progress in developing chelators for medicinal applications has been hindered by a limited understanding of actinium chemistry. This knowledge gap is primarily associated with handling actinium, as it is highly radioactive and in short supply. Hence, AcIII reactivity is often inferred from the lanthanides and minor actinides (that is, Am, Cm), with limited success. Here we overcome these challenges and characterize actinium in HCl solutions using X-ray absorption spectroscopy and molecular dynamics density functional theory. The Ac-Cl and Ac-OH2O distances are measured to be 2.95(3) and 2.59(3) Å, respectively. The X-ray absorption spectroscopy comparisons between AcIII and AmIII in HCl solutions indicate AcIII coordinates more inner-sphere Cl1- ligands (3.2+/-1.1) than AmIII (0.8+/-0.3). These results imply diverse reactivity for the +3 actinides and highlight the unexpected and unique AcIII chemical behaviour.

  11. Spectroscopic and computational investigation of actinium coordination chemistry

    Science.gov (United States)

    Ferrier, Maryline G.; Batista, Enrique R.; Berg, John M.; Birnbaum, Eva R.; Cross, Justin N.; Engle, Jonathan W.; La Pierre, Henry S.; Kozimor, Stosh A.; Lezama Pacheco, Juan S.; Stein, Benjamin W.; Stieber, S. Chantal E.; Wilson, Justin J.

    2016-01-01

    Actinium-225 is a promising isotope for targeted-α therapy. Unfortunately, progress in developing chelators for medicinal applications has been hindered by a limited understanding of actinium chemistry. This knowledge gap is primarily associated with handling actinium, as it is highly radioactive and in short supply. Hence, AcIII reactivity is often inferred from the lanthanides and minor actinides (that is, Am, Cm), with limited success. Here we overcome these challenges and characterize actinium in HCl solutions using X-ray absorption spectroscopy and molecular dynamics density functional theory. The Ac–Cl and Ac–OH2O distances are measured to be 2.95(3) and 2.59(3) Å, respectively. The X-ray absorption spectroscopy comparisons between AcIII and AmIII in HCl solutions indicate AcIII coordinates more inner-sphere Cl1– ligands (3.2±1.1) than AmIII (0.8±0.3). These results imply diverse reactivity for the +3 actinides and highlight the unexpected and unique AcIII chemical behaviour. PMID:27531582

  12. Spectroscopic and computational investigation of actinium coordination chemistry.

    Science.gov (United States)

    Ferrier, Maryline G; Batista, Enrique R; Berg, John M; Birnbaum, Eva R; Cross, Justin N; Engle, Jonathan W; La Pierre, Henry S; Kozimor, Stosh A; Lezama Pacheco, Juan S; Stein, Benjamin W; Stieber, S Chantal E; Wilson, Justin J

    2016-01-01

    Actinium-225 is a promising isotope for targeted-α therapy. Unfortunately, progress in developing chelators for medicinal applications has been hindered by a limited understanding of actinium chemistry. This knowledge gap is primarily associated with handling actinium, as it is highly radioactive and in short supply. Hence, Ac(III) reactivity is often inferred from the lanthanides and minor actinides (that is, Am, Cm), with limited success. Here we overcome these challenges and characterize actinium in HCl solutions using X-ray absorption spectroscopy and molecular dynamics density functional theory. The Ac-Cl and Ac-OH2O distances are measured to be 2.95(3) and 2.59(3) Å, respectively. The X-ray absorption spectroscopy comparisons between Ac(III) and Am(III) in HCl solutions indicate Ac(III) coordinates more inner-sphere Cl(1-) ligands (3.2±1.1) than Am(III) (0.8±0.3). These results imply diverse reactivity for the +3 actinides and highlight the unexpected and unique Ac(III) chemical behaviour. PMID:27531582

  13. The New Color of Chemistry: Green Chemistry

    OpenAIRE

    GERÇEK, Zuhal

    2012-01-01

    Green chemistry which is the new application of chemistry rules provides solutions to problems that mankind is faced with climate changes, sustainable agriculture, energy, toxics, depletion of natural sources e.g. designing new chemicals and processes that production and utilization of hazardous matters. So, it is the indispensible tool for sustainable development. Current and future chemists should consider the human health and ecological issues in their professional life. In order to provid...

  14. Philosophy of Chemistry or Philosophy with Chemistry?

    OpenAIRE

    Bernadette Bensaude-Vincent

    2014-01-01

    Chemistry deserves more philosophical attention not so much to do justice to a long-neglected science or to enhance its cultural prestige, but to undermine a number of taken-for-granted assumptions about scientific rationality and more importantly to diversify our metaphysical views of nature and reality. In brief, this paper does not make the case for a philosophy of chemistry. It rather urges philosophers of science to listen to chemists and discuss what they learn from them. Because over t...

  15. Structure of early actinides(V) in acidic solutions

    Energy Technology Data Exchange (ETDEWEB)

    Di Giandomenico, M.V.; Le Naour, C.; Simoni, E. [CNRS/Univ. Paris-Sud, Inst. de Physique Nucleaire, Orsay (France); Guillaumont, D.; Moisy, P.; Den Auwer, C. [CEA Marcoule, DHN/DRCP/SCPS, Bagnols sur Ceze (France); Hennig, C. [Forschungszentrum Rossendorf, Dresden (Germany); Conradson, S.D. [Los Alamos National Lab., Los Alamos, NM (United States)

    2009-07-01

    Protactinium occupies a key position in the actinide series between thorium and uranium. In aqueous acidic solution, it is stable at oxidation state (V), occurring either as an oxocation or as a naked ion, depending on the media. Very few structural information on the hydration sphere of Pa(V) in acidic medium is available, in particular in hydrofluoric acid. Combined EXAFS and theoretical calculations have been used in this work to characterize the protactinium coordination sphere at various HF concentrations. The correlation of the XAFS data with quantum chemical calculations provides complementary structural and electronic models from ab initio techniques. At HF concentrations from 0.5 to 0.05 M, both theoretical calculations and EXAFS data suggest that the protactinium coordination sphere is mainly composed of fluoride ions. At the lowest HF concentration, the occurrence of a monooxo bond is observed with EXAFS, in agreement with the literature. A comparison of these data with related neptunium(V) and plutonium(V) diooxocations in perchloric acid is also presented. (orig.)

  16. Structure of early actinides(V) in acidic solutions

    International Nuclear Information System (INIS)

    Protactinium occupies a key position in the actinide series between thorium and uranium. In aqueous acidic solution, it is stable at oxidation state (V), occurring either as an oxocation or as a naked ion, depending on the media. Very few structural information on the hydration sphere of Pa(V) in acidic medium is available, in particular in hydrofluoric acid. Combined EXAFS and theoretical calculations have been used in this work to characterize the protactinium coordination sphere at various HF concentrations. The correlation of the XAFS data with quantum chemical calculations provides complementary structural and electronic models from ab initio techniques. At HF concentrations from 0.5 to 0.05 M, both theoretical calculations and EXAFS data suggest that the protactinium coordination sphere is mainly composed of fluoride ions. At the lowest HF concentration, the occurrence of a monooxo bond is observed with EXAFS, in agreement with the literature. A comparison of these data with related neptunium(V) and plutonium(V) diooxocations in perchloric acid is also presented. (orig.)

  17. Effects of organic degradation products on the sorption of actinides

    International Nuclear Information System (INIS)

    Previous work has shown that products from the chemical degradation of cellulosic matter can significantly reduce sorption of uranium(VI) and plutonium(IV) on geological materials. Uranium(IV) batch sorption experiments have now been performed to study the effect of organic degradation products in a reducing environment. Thorium(IV) sorption has also been studied since thorium is an important radioelement in its own right and has potential use as a simulant for other tetravalent actinides. Sorption onto London clay, Caithness flagstones and St. Bees sandstone was investigated. Experimental conditions were chosen to simulate both those expected close to cementitious repository (pH ∝ 11) and at the edge of the zone of migration of the alkaline plume (pH ∝ 8). Work was carried out with both authentic degradation products and with gluconate, acting as a well-characterized simulant for cellulosic degradation products. The results show that the presence of organic species can cause a reduction in sorption. This is especially so in the presence of a high concentration of gluconate ions, but the reduction is significantly less with authentic degradation products. (orig.)

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

    International Nuclear Information System (INIS)

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

  19. Functionalization of mesoporous materials for lanthanide and actinide extraction.

    Science.gov (United States)

    Florek, Justyna; Giret, Simon; Juère, Estelle; Larivière, Dominic; Kleitz, Freddy

    2016-10-14

    Among the energy sources currently available that could address our insatiable appetite for energy and minimize our CO2 emission, solar, wind, and nuclear energy currently occupy an increasing portion of our energy portfolio. The energy associated with these sources can however only be harnessed after mineral resources containing valuable constituents such as actinides (Ac) and rare earth elements (REEs) are extracted, purified and transformed into components necessary for the conversion of energy into electricity. Unfortunately, the environmental impacts resulting from their manufacture including the generation of undesirable and, sometimes, radioactive wastes and the non-renewable nature of the mineral resources, to name a few, have emerged as challenges that should be addressed by the scientific community. In this perspective, the recent development of functionalized solid materials dedicated to selective elemental separation/pre-concentration could provide answers to several of the above-mentioned challenges. This review focuses on recent advances in the field of mesoporous solid-phase (SP) sorbents designed for REEs and Ac liquid-solid extraction. Particular attention will be devoted to silica and carbon sorbents functionalized with commonly known ligands, such as phosphorus or amide-containing functionalities. The extraction performances of these new systems are discussed in terms of sorption capacity and selectivity. In order to support potential industrial applications of the silica and carbon-based sorbents, their main drawbacks and advantages are highlighted and discussed.

  20. Peculiarities of phase formation in synthesis of actinide waste forms

    International Nuclear Information System (INIS)

    The phase formation processes by synthesis of the materials with the zirconolite and pyrochlore structure are studied through the methods of the x-ray phase analysis and electron microscopy with the purpose of optimizing the conditions for production of the matrices, used for immobilization of the actinide-containing wastes. It is established, that 20 hours are required for achieving the equilibrium in the CaO-TiO2-ZrO2 system at 1300 deg C and 5 hours - at 1450-1550 deg C. More than 20 hours are required for achieving the equilibrium in the Gd2O3-TiO2 system at 1100 deg C, less than 20 hours at 1200 deg C, about 1 hour - at 1300 deg C and less than 1 hour - at 1400-1550 deg C. The slowest phase formation processes take place in the Gd2O3-ZrO2 system, whereby at 1550 deg C no complete synthesis was observed even during 48 hours. The products of reactions, performed at lower temperatures or durations, contained the components of the initial charge along with the target phases with the zirconolite or pyrochlore structure

  1. Actinide recycle potential in the IFR [Integral Fast Reactor

    International Nuclear Information System (INIS)

    Rising concern about the greenhouse effect reinforces the need to reexamine the question of a next-generation reactor concept that can contribute significantly toward substitution for fossil-based energy generation. Even with only the nuclear capacity on-line today, world-wide reasonably assured uranium resources would last for only about 50 years. If nuclear is to make a significant contribution, breeding is a fundamental requirement. Uranium resources can then be extended by two orders of magnitude, making nuclear essentially a renewable energy source. The key technical elements of the IFR concept are metallic fuel and fuel cycle technology based on pyroprocessing. Pyroprocessing is radically different from the conventional PUREX reprocessing developed for the LWR oxide fuel. Chemical feasibility of pyroprocessing has been demonstrated. The next major step in the IFR development program will be the full-scale pyroprocessing demonstration to be carried out in conjunction with EBR-II. IFR fuel cycle closure based on pyroprocessing can also have a dramatic impact on the waste management options, and in particular on the actinide recycling. 6 figs

  2. Outcomes on Oxide Fuel Development for Minor Actinides Recycling

    International Nuclear Information System (INIS)

    A state of the art review is given of minor actinide (MA)-bearing oxide fuel development for sodium fast reactors (SFRs) and accelerator driven systems (ADS). The homogeneous recycle option in SFRs, where small amounts of MAs are diluted in (U,Pu)O2-x driver fuels, emerges as a technically sound approach, reinforced by national and international programmes. Its technology readiness level is appropriate to implement irradiation tests from pin to bundle scale. Regarding the heterogeneous recycle option in SFRs, a comprehensive database regarding inert matrix fuels is available as the result of ~35 irradiation tests. The promising results gained with MgO, Mo and ZrO2 matrices have to be completed by post-irradiation examinations on optimized fuel microstructures. On the other hand, a first step in the long term (MA,U)O2-x fuel development process is under investigation with MARIOS and DIAMINO tests in the HFR and OSIRIS, before the implementation of prototypical irradiation tests. For ADS, very informative feedback from inert matrix fuel developments has been completed by dedicated collaborative programmes, including major irradiations for the fuel performance assessment from HELIOS and FUTURIX-FTA experiments, whose post-irradiation examinations are under way. (author)

  3. New insights into formation of trivalent actinides complexes with DTPA

    International Nuclear Information System (INIS)

    Complexation of trivalent actinides with DTPA (diethylenetriamine pentaacetic acid) was studied as a function of pcH and temperature in (Na,H)Cl medium of 0.1 M ionic strength. Formation constants of both complexes AnHDTPA- and AnDTPA2- (where An stands for Am, Cm, and Cf) were determined by TRLFS, CE-ICP-MS, spectrophotometry, and solvent extraction. The values of formation constants obtained from the different techniques are coherent and consistent with reinterpreted literature data, showing a higher stability of Cf complexes than Am and Cm complexes. The effect of temperature indicates that formation constants of protonated and non protonated complexes are exothermic with a high positive entropic contribution. DFT calculations were also performed on the An/DTPA system. Geometry optimizations were conducted on AnDTPA2- and AnHDTPA- considering all possible protonation sites. For both complexes, one and two water molecules in the first coordination sphere of curium were also considered. DFT calculations indicate that the lowest energy structures correspond to protonation on oxygen that is not involved in An-DTPA bonds and that the structures with two water molecules are not stable. (authors)

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

    Energy Technology Data Exchange (ETDEWEB)

    Wilkerson, Marianne Perry [Los Alamos National Laboratory

    2010-01-01

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

  5. Minor actinide fission induced by multi-nucleon transfer reaction in inverse kinematics

    Directory of Open Access Journals (Sweden)

    Taieb J.

    2010-03-01

    Full Text Available In the framework of nuclear waste incineration and design of new generation nuclear reactors, experimental data on fission probabilities and on fission fragment yields of minor actinides are crucial to design prototypes. Transfer-induced fission has proven to be an efficient method to study fission probabilities of actinides which cannot be investigated with standard techniques due to their high radioactivity. We report on the preliminary results of an experiment performed at GANIL that investigates fission probabilities with multi-nucleon transfer reactions in inverse kinematics between a 238U beam on a 12C target. Actinides from U to Cm were produced with an excitation energy range from 0 to 30 MeV. In addition, inverse kinematics allowed to characterize the fission fragments in mass and charge. A key point of the analysis resides in the identification of the actinides produced in the different transfer channels. The new annular telescope SPIDER was used to tag the target-like recoil nucleus of the transfer reaction and to determine the excitation energy of the actinide. The fission probability for each transfer channel is accessible and the preliminary results for 238U are promising.

  6. Status of development of actinide blanket processing flowsheets for accelerator transmutation of nuclear waste

    International Nuclear Information System (INIS)

    An accelerator-driven subcritical nuclear system is briefly described that transmutes actinides and selected long-lived fission products. An application of this accelerator transmutation of nuclear waste (ATW) concept to spent fuel from a commercial nuclear power plant is presented as an example. The emphasis here is on a possible aqueous processing flowsheet to separate the actinides and selected long-lived fission products from the remaining fission products within the transmutation system. In the proposed system the actinides circulate through the thermal neutron flux as a slurry of oxide particles in heavy water in two loops with different average residence times: one loop for neptunium and plutonium and one for americium and curium. Material from the Np/Pu loop is processed with a short cooling time (5-10 days) because of the need to keep the total actinide inventory, low for this particular ATW application. The high radiation and thermal load from the irradiated material places severe constraints on the separation processes that can be used. The oxide particles are dissolved in nitric acid and a quarternary, ammonium anion exchanger is used to extract neptunium, plutonium, technetium, and palladium. After further cooling (about 90 days), the Am, Cm and higher actinides are extracted using a TALSPEAK-type process. The proposed operations were chosen because they have been successfully tested for processing high-level radioactive fuels or wastes in gram to kilogram quantities

  7. Plutonium and minor actinide utilisation in a pebble-bed high temperature reactor

    International Nuclear Information System (INIS)

    This paper contains results of the analysis of the pebble-bed high temperature gas-cooled PUMA reactor loaded with plutonium and minor actinide (Pu/MA) fuel. Starting from knowledge and experience gained in the Euratom FP5 projects HTR-N and HTR-N1, this study aims at demonstrating the potential of high temperature reactors to utilize or transmute Pu/MA fuel. The work has been performed within the Euratom FP6 project PUMA. A number of different fuel types and fuel configurations have been analyzed and compared with respect to incineration performance and safety-related reactor parameters. The results show the excellent plutonium and minor actinide burning capabilities of the high temperature reactor. The largest degree of incineration is attained in the case of an HTR fuelled by pure plutonium fuel as it remains critical at very deep burnup of the discharged pebbles. Addition of minor actinides to the fuel leads to decrease of the achievable discharge burnup and therefore smaller fraction of actinides incinerated during reactor operation. The inert-matrix fuel design improves the transmutation performance of the reactor, while the 'wallpaper' fuel does not have advantage over the standard fuel design in this respect. After 100 years of decay following the fuel discharge, the total amount of actinides remains almost unchanged for all of the fuel types considered. Among the plutonium isotopes, only the amount of Pu-241 is reduced significantly due to its relatively short half-life. (authors)

  8. Plutonium and minor actinide utilisation in a pebble-bed high temperature reactor

    Energy Technology Data Exchange (ETDEWEB)

    Petrov, B. Y.; Kuijper, J. C.; Oppe, J.; De Haas, J. B. M. [Nuclear Research and Consultancy Group, Westerduinweg 3, 1755 ZG Petten (Netherlands)

    2012-07-01

    This paper contains results of the analysis of the pebble-bed high temperature gas-cooled PUMA reactor loaded with plutonium and minor actinide (Pu/MA) fuel. Starting from knowledge and experience gained in the Euratom FP5 projects HTR-N and HTR-N1, this study aims at demonstrating the potential of high temperature reactors to utilize or transmute Pu/MA fuel. The work has been performed within the Euratom FP6 project PUMA. A number of different fuel types and fuel configurations have been analyzed and compared with respect to incineration performance and safety-related reactor parameters. The results show the excellent plutonium and minor actinide burning capabilities of the high temperature reactor. The largest degree of incineration is attained in the case of an HTR fuelled by pure plutonium fuel as it remains critical at very deep burnup of the discharged pebbles. Addition of minor actinides to the fuel leads to decrease of the achievable discharge burnup and therefore smaller fraction of actinides incinerated during reactor operation. The inert-matrix fuel design improves the transmutation performance of the reactor, while the 'wallpaper' fuel does not have advantage over the standard fuel design in this respect. After 100 years of decay following the fuel discharge, the total amount of actinides remains almost unchanged for all of the fuel types considered. Among the plutonium isotopes, only the amount of Pu-241 is reduced significantly due to its relatively short half-life. (authors)

  9. Partitioning technologies and actinide science: towards pilot facilities in Europe (ACSEPT project)

    International Nuclear Information System (INIS)

    ACSEPT is an essential contribution to the demonstration, in the long term, of the potential benefits of actinide recycling to minimize the burden on the geological repositories. To succeed, ACSEPT is organized into three technical domains: (i) Considering technically mature aqueous separation processes, ACSEPT works to optimize and select the most promising ones dedicated either to actinide partitioning or to grouped actinide separation. A substantial review was undertaken either to be sure that the right molecule families are being studied, or, on the contrary, to identify new candidates. Results of the first hot tests allowed the validation of some process options. (ii) Concerning pyrochemical separation processes, ACSEPT is focused on the enhancement of the two reference cores of process selected within EUROPART with specific attention to the exhaustive electrolysis in molten chloride (quantitative recovery of the actinides with the lowest amount of fission products) and to actinide back-extraction from an An-Al alloy. R and D efforts are also brought to key scientific and technical issues compulsory for building a complete separation process (head-end steps, salt treatment for recycling and waste management). (iii) By integrating all the experimental results within engineering and systems studies, both in hydro and pyro domains, ACSEPT will deliver relevant flowsheets and recommendations to prepare for future demonstration at a pilot level, in relation with strategies developed through the SNE-TP. In addition, a training and education programme is implemented to share the knowledge among the partitioning community and the future generations of researchers

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

    International Nuclear Information System (INIS)

    We are interested in applying our understanding of actinide chemical structure and bonding to broaden the suite of analytical tools available for nuclear forensic analyses. Uranium- and plutonium-oxide systems form under a variety of conditions, and these chemical species exhibit some of the most complex behavior of metal oxide systems known. No less intriguing is the ability of AnO2 (An: U, Pu) to form non-stoichiometric species described as AnO2+x. Environmental studies have shown the value of utilizing the chemical signatures of these actinide oxide materials to understand transport following release into the environment. Chemical speciation of actinide-oxide samples may also provide clues as to the age, source, or process history of the material. The scientific challenge is to identify, measure and understand those aspects of speciation of actinide analytes that carry information about material origin and history most relevant to forensics. Here, we will describe our efforts in material synthesis and analytical methods development that we will use to provide the fundamental science to characterize actinide oxide molecular structures for forensic science. Structural properties and initial results to measure structural variability of uranium oxide samples using synchrotron-based X-ray Absorption Fine Structure will be discussed.

  11. Technical requirements for the actinide source-term waste test program

    International Nuclear Information System (INIS)

    This document defines the technical requirements for a test program designed to measure time-dependent concentrations of actinide elements from contact-handled transuranic (CH TRU) waste immersed in brines similar to those found in the underground workings of the Waste Isolation Pilot Plant (WIPP). This test program wig determine the influences of TRU waste constituents on the concentrations of dissolved and suspended actinides relevant to the performance of the WIPP. These influences (which include pH, Eh, complexing agents, sorbent phases, and colloidal particles) can affect solubilities and colloidal mobilization of actinides. The test concept involves fully inundating several TRU waste types with simulated WIPP brines in sealed containers and monitoring the concentrations of actinide species in the leachate as a function of time. The results from this program will be used to test numeric models of actinide concentrations derived from laboratory studies. The model is required for WIPP performance assessment with respect to the Environmental Protection Agency's 40 CFR Part 191B

  12. Gas core reactors for actinide transmutation and breeder applications. Annual report

    International Nuclear Information System (INIS)

    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

  13. Safe management of actinides in the nuclear fuel cycle: Role of mineralogy

    Science.gov (United States)

    Ewing, Rodney C.

    2011-02-01

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

  14. Thermally unstable complexants: Stability of lanthanide/actinide complexes, thermal instability of the ligands, and applications in actinide separations

    Energy Technology Data Exchange (ETDEWEB)

    Nash, K.L.; Rickert, P.G.

    1991-01-01

    Water soluble complexing agents are commonly used in separations to enhance the selectivity of both ion exchange and solvent extraction processes. Applications of this type in the treatment of nuclear wastes using conventional complexing agents have found mixed success due to the nature of the complexants. In addition, the residual solutions containing these species have led to potentially serious complications in waste storage. To overcome some of the limitations of carboxylic acid and aminopolycarboxylate ligands, we have initiated a program to investigate the complexing ability, thermal/oxidative instability, and separation potential of a group of water soluble organophosphorus compounds which we call Thermally Unstable Complexants, or simply TUCS. Complexants of this type appear to be superior to conventional analogues in a number of respects. In this report, we will summarize our research to date on the actinide/lanthanide complexes with a series of substituted methanediphosphonic acids, the kinetics of their oxidative decomposition, and a few applications which have been developed for their use. 17 refs., 5 figs., 3 tab.

  15. Plutonium Chemistry in the UREX+ Separation Processes

    Energy Technology Data Exchange (ETDEWEB)

    ALena Paulenova; George F. Vandegrift, III; Kenneth R. Czerwinski

    2009-10-01

    The project "Plutonium Chemistry in the UREX+ Separation Processes” is led by Dr. Alena Paulenova of Oregon State University under collaboration with Dr. George Vandegrift of ANL and Dr. Ken Czerwinski of the University of Nevada at Las Vegas. The objective of the project is to examine the chemical speciation of plutonium in UREX+ (uranium/tributylphosphate) extraction processes for advanced fuel technology. Researchers will analyze the change in speciation using existing thermodynamics and kinetic computer codes to examine the speciation of plutonium in aqueous and organic phases. They will examine the different oxidation states of plutonium to find the relative distribution between the aqueous and organic phases under various conditions such as different concentrations of nitric acid, total nitrates, or actinide ions. They will also utilize techniques such as X-ray absorbance spectroscopy and small-angle neutron scattering for determining plutonium and uranium speciation in all separation stages. The project started in April 2005 and is scheduled for completion in March 2008.

  16. Journal of Business Chemistry

    OpenAIRE

    2013-01-01

    The Journal of Business Chemistry examines issues associated with leadership and management for chemists and managers working in chemical research or industry. This journal is devoted to improving and developing the field of Business Chemistry. The Journal of Business Chemistry publishes peer-reviewed papers (including case studies) and essays. Areas for possible publication in include: leadership issues in the chemical and biochemical industry, such as teamwork, team building, mentoring, coa...

  17. Mathematical Thinking in Chemistry

    OpenAIRE

    José L. Villaveces; Guillermo Restrepo

    2012-01-01

    Mathematical chemistry is often thought to be a 20th-century subdiscipline of chemistry, but in this paper we discuss several early chemical ideas and some landmarks of chemistry as instances of the mathematical way of thinking; many of them before 1900. By the mathematical way of thinking, we follow Weyl's description of it in terms of functional thinking, i.e. setting up variables, symbolizing them, and seeking for functions relating them. The cases we discuss are Plato's triangles, Geoffro...

  18. Orbital interactions in chemistry

    CERN Document Server

    Albright, Thomas A; Whangbo, Myung-Hwan

    2013-01-01

    Explains the underlying structure that unites all disciplines in chemistry Now in its second edition, this book explores organic, organometallic, inorganic, solid state, and materials chemistry, demonstrating how common molecular orbital situations arise throughout the whole chemical spectrum. The authors explore the relationships that enable readers to grasp the theory that underlies and connects traditional fields of study within chemistry, thereby providing a conceptual framework with which to think about chemical structure and reactivity problems. Orbital Interactions

  19. The Chemistry Institute

    OpenAIRE

    Fontecave, Marc

    2015-01-01

    Chemistry at the Collège de France has received particular attention over the last few years. After the departures of Profs Jean-Marie Lehn and Jacques Livage, new ambition for developing this discipline has led to the creation of several Chairs: Prof. Marc Fontecave’s Chair of Chemistry of Biological Processes in 2008, Prof. Clément Sanchez’ Chair of Chemistry of Hybrid Materials in 2011, and the Chair of Chemistry of Materials and Energy, which Prof. Jean-Marie Tarascon has held since 2014....

  20. Group theory and chemistry

    CERN Document Server

    Bishop, David M

    1993-01-01

    Group theoretical principles are an integral part of modern chemistry. Not only do they help account for a wide variety of chemical phenomena, they simplify quantum chemical calculations. Indeed, knowledge of their application to chemical problems is essential for students of chemistry. This complete, self-contained study, written for advanced undergraduate-level and graduate-level chemistry students, clearly and concisely introduces the subject of group theory and demonstrates its application to chemical problems.To assist chemistry students with the mathematics involved, Professor Bishop ha