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Sample records for actinide waste forms

  1. 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

  2. Pyrochlore as nuclear waste form. Actinide uptake and chemical stability

    Energy Technology Data Exchange (ETDEWEB)

    Finkeldei, Sarah Charlotte

    2015-07-01

    Radioactive waste is generated by many different technical and scientific applications. For the past decades, different waste disposal strategies have been considered. Several questions on the waste disposal strategy remain unanswered, particularly regarding the long-term radiotoxicity of minor actinides (Am, Cm, Np), plutonium and uranium. These radionuclides mainly arise from high level nuclear waste (HLW), specific waste streams or dismantled nuclear weapons. Although many countries have opted for the direct disposal of spent fuel, from a scientific and technical point of view it is imperative to pursue alternative waste management strategies. Apart from the vitrification, especially for trivalent actinides and Pu, crystalline ceramic waste forms are considered. In contrast to glasses, crystalline waste forms, which are chemically and physically highly stable, allow the retention of radionuclides on well-defined lattice positions within the crystal structure. Besides polyphase ceramics such as SYNROC, single phase ceramics are considered as tailor made host phases to embed a specific radionuclide or a specific group. Among oxidic single phase ceramics pyrochlores are known to have a high potential for this application. This work examines ZrO{sub 2} based pyrochlores as potential nuclear waste forms, which are known to show a high aqueous stability and a high tolerance towards radiation damage. This work contributes to (1) understand the phase stability field of pyrochlore and consequences of non-stoichiometry which leads to pyrochlores with mixed cationic sites. Mixed cationic occupancies are likely to occur in actinide-bearing pyrochlores. (2) The structural uptake of radionuclides themselves was studied. (3) The chemical stability and the effect of phase transition from pyrochlore to defect fluorite were probed. This phase transition is important, as it is the result of radiation damage in ZrO{sub 2} based pyrochlores. ZrO{sub 2} - Nd{sub 2}O{sub 3} pellets

  3. 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

  4. Alloy waste forms for metal fission products and actinides isolated by spent nuclear fuel treatment

    International Nuclear Information System (INIS)

    Waste form alloys are being developed at Argonne National Laboratory for the disposal of remnant metallic wastes from an electrometallurgical process developed to treat spent nuclear fuel. This metal waste form consists of the fuel cladding (stainless steel or Zircaloy), noble metal fission products (e.g., Ru, Pd, Mo and Tc), and other metallic wastes. The main constituents of the metal waste stream are the cladding hulls (85 to 90 wt%); using the hulls as the dominant alloying component minimizes the overall waste volume as compared to vitrification or metal encapsulation. Two nominal compositions for the waste form are being developed: (1) stainless steel-15 wt% zirconium for stainless steel-clad fuels and (2) zirconium-8 wt% stainless steel for Zircaloy-clad fuels. The noble metal fission products are the primary source of radiation in the metal waste form. However, inclusion of actinides in the metal waste form is being investigated as an option for interim or ultimate storage. Simulated waste form alloys were prepared and analyzed to determine the baseline alloy microstructures and the microstructural distribution of noble metals and actinides. Corrosion tests of the metal waste form alloys indicate that they are highly resistant to corrosion

  5. 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.

  6. 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

  7. 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.'

  8. Stainless steel-zirconium alloy waste forms for metallic fission products and actinides during treatment of spent nuclear fuel

    International Nuclear Information System (INIS)

    Stainless steel-zirconium waste form alloys are being developed for the disposal of metallic wastes recovered from spent nuclear fuel using an electrometallurgical process developed by Argonne National Laboratory. The metal waste form comprises the fuel cladding, noble metal fission products and other metallic constituents. Two nominal waste form compositions are being developed: (1) stainless steel-15 wt% zirconium for stainless steel-clad fuels. The noble metal fission products are the primary source of radiation and their contribution to the waste form radioactivity has been calculated. The disposition of actinide metals in the waste alloys is also being explored. Simulated waste form alloys were prepared to study the baseline alloy microstructures and the microstructural distribution of noble metals and actinides, and to evaluate corrosion performance

  9. Pyrochlore-structured titanate ceramics for immobilisation of actinides: Hot isostatic pressing (HIPing) and stainless steel/waste form interactions

    Science.gov (United States)

    Zhang, Yingjie; Li, Huijun; Moricca, Sam

    2008-07-01

    A pyrochlore-structured titanate ceramic has been studied in respect of its overall feasibility for immobilisation of impure actinide-rich radioactive wastes through the hot isostatic pressing (HIPing) technique. The resultant waste form contains mainly pyrochlore (˜70%), rutile (˜14%) as well as perovskite (˜12%), hollandite (˜2%) and brannerite (˜1%). Optical spectroscopy confirms that uranium (used to simulate Pu) exists mainly in the stable pyrochlore-structured phase as tetravalent ions as designed. The stainless steel/waste form interactions under HIPing conditions (1280 °C/100 MPa/3 h) do not seem to change the actinide-bearing phases and therefore should have no detrimental effect on the waste form.

  10. Zirconolite-rich titanate ceramics for immobilisation of actinides - Waste form/HIP can interactions and chemical durability

    Science.gov (United States)

    Zhang, Y.; Stewart, M. W. A.; Li, H.; Carter, M. L.; Vance, E. R.; Moricca, S.

    2009-12-01

    Zirconolite-based titanate ceramics containing U plus Th or Pu have been prepared. The final consolidation to produce a dense monolithic waste form was carried out using hot isostatic pressing (HIPing) of the calcined materials within a stainless steel can. The ceramics were characterised and tested for their overall feasibility to immobilise impure Pu or separated actinide-rich radioactive wastes. As designed, tetravalent U and Pu are mainly incorporated in a durable zirconolite phase, together with Gd or Hf added as neutron absorbers. The interaction of the waste form with the HIP can was also examined. No changes in the U valences or the U/Pu-bearing phase distributions were observed at the waste form-HIP can interface.

  11. 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

  12. 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.)

  13. 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)

  14. 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.

  15. 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.

  16. 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)

  17. Pyrochlore based glass-ceramics for the immobilization of actinide-rich nuclear wastes: From concept to reality

    Science.gov (United States)

    Zhang, Y.; Zhang, Z.; Thorogood, G.; Vance, E. R.

    2013-01-01

    Pyrochlore based glass-ceramics have been developed, from concept to reality, for the immobilization of actinide-rich nuclear wastes. Compared with zirconolite based glass-ceramics, they are less sensitive to the processing redox conditions and can double actinide waste loadings thus decreasing volumes of the consolidated waste forms, and subsequently reducing the interim storage and disposal costs. More importantly, they provide an alternative flexible system to tackle radioactive wastes arising from the advanced nuclear reactors.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2006-06-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2006-11-16

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2006-06-01

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

  1. Actinides in metallic waste from electrometallurgical treatment of spent nuclear fuel

    Science.gov (United States)

    Janney, D. E.; Keiser, D. D.

    2003-09-01

    Argonne National Laboratory has developed a pyroprocessing-based technique for conditioning spent sodium-bonded nuclear-reactor fuel in preparation for long-term disposal. The technique produces a metallic waste form whose nominal composition is stainless steel with 15 wt.% Zr (SS-15Zr), up to ˜ 11 wt.% actinide elements (primarily uranium), and a few percent metallic fission products. Actual and simulated waste forms show similar eutectic microstructures with approximately equal proportions of iron solid solution phases and Fe-Zr intermetallics. This article reports on an analysis of simulated waste forms containing uranium, neptunium, and plutonium.

  2. Densified waste form and method for forming

    Energy Technology Data Exchange (ETDEWEB)

    Garino, Terry J.; Nenoff, Tina M.; Sava Gallis, Dorina Florentina

    2015-08-25

    Materials and methods of making densified waste forms for temperature sensitive waste material, such as nuclear waste, formed with low temperature processing using metallic powder that forms the matrix that encapsulates the temperature sensitive waste material. The densified waste form includes a temperature sensitive waste material in a physically densified matrix, the matrix is a compacted metallic powder. The method for forming the densified waste form includes mixing a metallic powder and a temperature sensitive waste material to form a waste form precursor. The waste form precursor is compacted with sufficient pressure to densify the waste precursor and encapsulate the temperature sensitive waste material in a physically densified matrix.

  3. Densified waste form and method for forming

    Energy Technology Data Exchange (ETDEWEB)

    Garino, Terry J.; Nenoff, Tina M.; Sava Gallis, Dorina Florentina

    2016-05-17

    Materials and methods of making densified waste forms for temperature sensitive waste material, such as nuclear waste, formed with low temperature processing using metallic powder that forms the matrix that encapsulates the temperature sensitive waste material. The densified waste form includes a temperature sensitive waste material in a physically densified matrix, the matrix is a compacted metallic powder. The method for forming the densified waste form includes mixing a metallic powder and a temperature sensitive waste material to form a waste form precursor. The waste form precursor is compacted with sufficient pressure to densify the waste precursor and encapsulate the temperature sensitive waste material in a physically densified matrix.

  4. 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

  5. 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)

  6. 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

  7. 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

  8. Glass-ceramic nuclear waste forms obtained from SiO 2-Al 2O 3-CaO-ZrO 2-TiO 2 glasses containing lanthanides (Ce, Nd, Eu, Gd, Yb) and actinides (Th): study of internal crystallization

    Science.gov (United States)

    Loiseau, P.; Caurant, D.; Baffier, N.; Mazerolles, L.; Fillet, C.

    2004-10-01

    Glass-ceramic waste forms such as zirconolite (nominally CaZrTi 2O 7) based ones can be envisaged as good candidates for minor actinides or Pu immobilization. Such materials, in which the actinides (or lanthanides used as actinide surrogates) would be preferentially incorporated into zirconolite crystals homogeneously dispersed in a durable glassy matrix, can be prepared by controlled crystallization (nucleation + crystal growth) of parent glasses belonging to the SiO 2-Al 2O 3-CaO-ZrO 2-TiO 2 system. In this work we present the effects of the nature of the minor actinide surrogate (Ce, Nd, Eu, Gd, Yb, Th) on the structure, the microstructure and the composition of the zirconolite crystals formed in the bulk of the glass-ceramics. The amount of lanthanides and thorium incorporated into zirconolite crystals is discussed in relation with the capacity of the glass to accommodate these elements and of the crystals to incorporate them in the calcium and zirconium sites of their structure.

  9. Strontium and Actinide Separations from High Level Nuclear Waste Solutions using Monosodium Titanate - Actual Waste Testing

    Energy Technology Data Exchange (ETDEWEB)

    Peters, T.B.; Barnes, M.J.; Hobbs,D.T.; Walker, D.D.; Fondeur, F.F.; Norato, M.A.; Pulmano, R.L.; Fink, S.D.

    2005-11-01

    Pretreatment processes at the Savannah River Site will separate {sup 90}Sr, alpha-emitting and radionuclides (i.e., actinides) and {sup 137}Cs prior to disposal of the high-level nuclear waste. Separation of {sup 90}Sr and alpha-emitting radionuclides occurs by ion exchange/adsorption using an inorganic material, monosodium titanate (MST). Previously reported testing with simulants indicates that the MST exhibits high selectivity for strontium and actinides in high ionic strength and strongly alkaline salt solutions. This paper provides a summary of data acquired to measure the performance of MST to remove strontium and actinides from actual waste solutions. These tests evaluated the effects of ionic strength, mixing, elevated alpha activities, and multiple contacts of the waste with MST. Tests also provided confirmation that MST performs well at much larger laboratory scales (300-700 times larger) and exhibits little affinity for desorption of strontium and plutonium during washing.

  10. 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

  11. Advanced waste forms from spent nuclear fuel

    Energy Technology Data Exchange (ETDEWEB)

    Ackerman, J.P.; McPheeters, C.C.

    1995-12-31

    More than one hundred spent nuclear fuel types, having an aggregate mass of more than 5000 metric tons (2700 metric tons of heavy metal), are stored by the United States Department of Energy. This paper proposes a method for converting this wide variety of fuel types into two waste forms for geologic disposal. The method is based on a molten salt electrorefining technique that was developed for conditioning the sodium-bonded, metallic fuel from the Experimental Breeder Reactor-II (EBR-II) for geologic disposal. The electrorefining method produces two stable, optionally actinide-free, high-level waste forms: an alloy formed from stainless steel, zirconium, and noble metal fission products, and a ceramic waste form containing the reactive metal fission products. Electrorefining and its accompanying head-end process are briefly described, and methods for isolating fission products and fabricating waste forms are discussed.

  12. The treatment and packaging of waste plutonium and waste actinides for disposal

    International Nuclear Information System (INIS)

    The objectives of this work have been to review the current state of knowledge on the treatment and packaging of unusable or surplus plutonium and other waste actinides for disposal and to identify any gaps in data essential for the development of a preferred route. The exercise was based on published data which said the quantity currently to be disposed of was 50 tonnes in oxide form. A literature review over the period 1978 to 1988 was carried out and a computerised database specific to the exercise was created. From this it is concluded that there are no insuperable problems to the formulation of a disposal route although there is none currently proven. The preferred wasteform would be a glass or synthetic rock. The major complication lies in the fissile nature of plutonium which dictates limits to the package size and places restrictions on the production and disposal routes. Additional work necessary to permit a final decision is listed. (author)

  13. 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)

  14. Conjugates of Magnetic Nanoparticle -- Actinide Specific Chelator for Radioactive Waste Separation

    Energy Technology Data Exchange (ETDEWEB)

    Maninder Kaur; Huijin Zhang; Leigh Martin; Terry Todd; You Qiang

    2013-11-01

    A novel nanotechnology for the separation of radioactive waste that uses magnetic nanoparticles (MNPs) conjugated with actinide specific chelators (MNP-Che) is reviewed with a focus on design and process development. The MNP-Che separation process is an effective way of separating heat generating minor actinides (Np, Am, Cm) from spent nuclear fuel solution to reduce the radiological hazard. It utilizes coated MNPs to selectively adsorb the contaminants onto their surfaces, after which the loaded particles are collected using a magnetic field. The MNP-Che conjugates can be recycled by stripping contaminates into a separate, smaller volume of solution, and then become the final waste form for disposal after reusing number of times. Due to the highly selective chelators, this remediation method could be both simple and versatile while allowing the valuable actinides to be recovered and recycled. Key issues standing in the way of large-scale application are stability of the conjugates and their dispersion in solution to maintain their unique properties, especially large surface area, of MNPs. With substantial research progress made on MNPs and their surface functionalization, as well as development of environmentally benign chelators, this method could become very flexible and cost-effective for recycling used fuel. Finally, the development of this nanotechnology is summarized and its future direction is discussed.

  15. Conjugates of magnetic nanoparticle-actinide specific chelator for radioactive waste separation.

    Science.gov (United States)

    Kaur, Maninder; Zhang, Huijin; Martin, Leigh; Todd, Terry; Qiang, You

    2013-01-01

    A novel nanotechnology for the separation of radioactive waste that uses magnetic nanoparticles (MNPs) conjugated with actinide specific chelators (MNP-Che) is reviewed with a focus on design and process development. The MNP-Che separation process is an effective way of separating heat generating minor actinides (Np, Am, Cm) from spent nuclear fuel solution to reduce the radiological hazard. It utilizes coated MNPs to selectively adsorb the contaminants onto their surfaces, after which the loaded particles are collected using a magnetic field. The MNP-Che conjugates can be recycled by stripping contaminates into a separate, smaller volume of solution, and then become the final waste form for disposal after reusing number of times. Due to the highly selective chelators, this remediation method could be both simple and versatile while allowing the valuable actinides to be recovered and recycled. Key issues standing in the way of large-scale application are stability of the conjugates and their dispersion in solution to maintain their unique properties, especially large surface area, of MNPs. With substantial research progress made on MNPs and their surface functionalization, as well as development of environmentally benign chelators, this method could become very flexible and cost-effective for recycling used fuel. Finally, the development of this nanotechnology is summarized and its future direction is discussed. PMID:24070142

  16. Rapid methods for determination of small amount of actinides in waste waters

    International Nuclear Information System (INIS)

    A rapid method of plutonium and actinide sum (Ac) (except uranium) determination in waste waters has been developed. For rapid isolation of 239Pu and Ac sum a method of extraction to iron hydroxide myomphate (IHM), consisting in Ac deposition on iron hydroxide, solvent extraction by monoisooctylmethylphosphinic acid and flotation of the disperse phase into solid extract of IHM, has been applied. The method permits to concentrate plutonium quantitatively from solutions in all of its forms, including colloid ones. For analysis of solid extracts α-spectroimetric instrumentation is used. The analysis sensitivity is 1 Bg/l, relative standard deviation - 0.3. 10 refs.; 1 fig.; 2 tabs

  17. Glass-ceramic nuclear waste forms obtained by crystallization of SiO 2-Al 2O 3-CaO-ZrO 2-TiO 2 glasses containing lanthanides (Ce, Nd, Eu, Gd, Yb) and actinides (Th): Study of the crystallization from the surface

    Science.gov (United States)

    Loiseau, P.; Caurant, D.

    2010-07-01

    Glass-ceramic materials containing zirconolite (nominally CaZrTi 2O 7) crystals in their bulk can be envisaged as potential waste forms for minor actinides (Np, Am, Cm) and Pu immobilization. In this study such matrices are synthesized by crystallization of SiO 2-Al 2O 3-CaO-ZrO 2-TiO 2 glasses containing lanthanides (Ce, Nd, Eu, Gd, Yb) and actinides (Th) as surrogates. A thin partially crystallized layer containing titanite and anorthite (nominally CaTiSiO 5 and CaAl 2Si 2O 8, respectively) growing from glass surface is also observed. The effect of the nature and concentration of surrogates on the structure, the microstructure and the composition of the crystals formed in the surface layer is presented in this paper. Titanite is the only crystalline phase able to significantly incorporate trivalent lanthanides whereas ThO 2 precipitates in the layer. The crystal growth thermal treatment duration (2-300 h) at high temperature (1050-1200 °C) is shown to strongly affect glass-ceramics microstructure. For the system studied in this paper, it appears that zirconolite is not thermodynamically stable in comparison with titanite growing form glass surface. Nevertheless, for kinetic reasons, such transformation (i.e. zirconolite disappearance to the benefit of titanite) is not expected to occur during interim storage and disposal of the glass-ceramic waste forms because their temperature will never exceed a few hundred degrees.

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

    International Nuclear Information System (INIS)

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

  19. Radiation effects in ceramic nuclear waste forms

    International Nuclear Information System (INIS)

    This paper reports on alpha-decay event damage (a particle and recoil-nucleus) that results in atomic-scale disorder which causes changes in the molar volume, corrosion rate, stored energy, mechanical properties, and macrostructure of ceramics. These changes particularly of volume and corrosion rate, have critical implications for the long-term durability of nuclear waste forms, such as the polyphase. Ti-based ceramic Synroc. This paper reviews data on actinide-bearing (U and Th) phases of great age (>100 m.y.) found in nature and compares these results to observation on actinide-doped phases (Pu and Cm) of nearly equivalent α-decay doses. Of particular interest is evidence for annealing of radiation damage effects over geologic periods of time under ambient conditions

  20. 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...

  1. Electrochemical/Pyrometallurgical Waste Stream Processing and Waste Form Fabrication

    Energy Technology Data Exchange (ETDEWEB)

    Steven Frank; Hwan Seo Park; Yung Zun Cho; William Ebert; Brian Riley

    2015-07-01

    This report summarizes treatment and waste form options being evaluated for waste streams resulting from the electrochemical/pyrometallurgical (pyro ) processing of used oxide nuclear fuel. The technologies that are described are South Korean (Republic of Korea – ROK) and United States of America (US) ‘centric’ in the approach to treating pyroprocessing wastes and are based on the decade long collaborations between US and ROK researchers. Some of the general and advanced technologies described in this report will be demonstrated during the Integrated Recycle Test (IRT) to be conducted as a part of the Joint Fuel Cycle Study (JFCS) collaboration between US Department of Energy (DOE) and ROK national laboratories. The JFCS means to specifically address and evaluated the technological, economic, and safe guard issues associated with the treatment of used nuclear fuel by pyroprocessing. The IRT will involve the processing of commercial, used oxide fuel to recover uranium and transuranics. The recovered transuranics will then be fabricated into metallic fuel and irradiated to transmutate, or burn the transuranic elements to shorter lived radionuclides. In addition, the various process streams will be evaluated and tested for fission product removal, electrolytic salt recycle, minimization of actinide loss to waste streams and waste form fabrication and characterization. This report specifically addresses the production and testing of those waste forms to demonstrate their compatibility with treatment options and suitability for disposal.

  2. Colloid formation during waste form reaction: implications for nuclear waste disposal

    Science.gov (United States)

    Bates, J. K.; Bradley, J.; Teetsov, A.; Bradley, C. R.; ten Brink, Marilyn Buchholtz

    1992-01-01

    Insoluble plutonium- and americium-bearing colloidal particles formed during simulated weathering of a high-level nuclear waste glass. Nearly 100 percent of the total plutonium and americium in test ground water was concentrated in these submicrometer particles. These results indicate that models of actinide mobility and repository integrity, which assume complete solubility of actinides in ground water, underestimate the potential for radionuclide release into the environment. A colloid-trapping mechanism may be necessary for a waste repository to meet long-term performance specifications.

  3. Ageing of a phosphate ceramic used to immobilize chloride-contaminated actinide waste

    Energy Technology Data Exchange (ETDEWEB)

    Metcalfe, Brian [AWE plc, Reading (United Kingdom); Donald, Ian W. [AWE plc, Reading (United Kingdom); Fong, Shirley K. [AWE plc, Reading (United Kingdom); Gerrard, Lee A. [AWE plc, Reading (United Kingdom); Strachan, Denis M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Scheele, Randall D. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2009-03-31

    At AWE, we have developed a process for the immobilization of ILW waste containing a significant quantity of chloride with Ca3(PO4)2 as the host material. Waste ions are incorporated into two phosphate-based phases, chlorapatite [Ca5(PO4)3Cl] and spodiosite [Ca2(PO4)Cl]. Non-active trials performed at AWE with Sm as the actinide surrogate demonstrated the durability of these phases in aqueous solution. Trials of the process, in which actinide-doped materials were used, wer performed at PNNL where the waste form was found to be resistant to aqueous leaching. Initial leach trials conducted on 239Pu /241Am loaded ceramic at 40°C/28 days gave normalized mass losses of 1.2 x 10-5 g.m-2 and 2.7 x 10-3 g.m-2 for Pu and Cl respectively. In order to assess the response of the phases to radiation-induced damage, accelerated ageing trials were performed on samples in which the 239Pu was replaced with 238Pu. No changes to the crystalline structure of the waste were detected in the XRD patterns after the samples had experienced an α radiation dose of 4 x 1018 g-1. Leach trials showed that there was an increase in the P and Ca release rates but no change in the Pu release rate.

  4. Microbial Transformation of TRU and Mixed Waste: Actinide Speciation and Waste Volume

    Energy Technology Data Exchange (ETDEWEB)

    Halada, Gary P

    2008-04-10

    In order to understand the susceptibility of transuranic and mixed waste to microbial degradation (as well as any mechanism which depends upon either complexation and/or redox of metal ions), it is essential to understand the association of metal ions with organic ligands present in mixed wastes. These ligands have been found in our previous EMSP study to limit electron transfer reactions and strongly affect transport and the eventual fate of radionuclides in the environment. As transuranic waste (and especially mixed waste) will be retained in burial sites and in legacy containment for (potentially) many years while awaiting treatment and removal (or remaining in place under stewardship agreements at government subsurface waste sites), it is also essential to understand the aging of mixed wastes and its implications for remediation and fate of radionuclides. Mixed waste containing actinides and organic materials are especially complex and require extensive study. The EMSP program described in this report is part of a joint program with the Environmental Sciences Department at Brookhaven National Laboratory. The Stony Brook University portion of this award has focused on the association of uranium (U(VI)) and transuranic analogs (Ce(III) and Eu(III)) with cellulosic materials and related compounds, with development of implications for microbial transformation of mixed wastes. The elucidation of the chemical nature of mixed waste is essential for the formulation of remediation and encapsulation technologies, for understanding the fate of contaminant exposed to the environment, and for development of meaningful models for contaminant storage and recovery.

  5. Glass-ceramic nuclear waste forms obtained by crystallization of SiO{sub 2}-Al{sub 2}O{sub 3}-CaO-ZrO{sub 2}-TiO{sub 2} glasses containing lanthanides (Ce, Nd, Eu, Gd, Yb) and actinides (Th): Study of the crystallization from the surface

    Energy Technology Data Exchange (ETDEWEB)

    Loiseau, P. [Laboratoire de Chimie de la Matiere Condensee de Paris (UMR CNRS 7574), Ecole Nationale Superieure de Chimie de Paris (ENSCP, Chimie-ParisTech), 11 rue Pierre et Marie Curie, 75231 Paris (France); Caurant, D., E-mail: daniel-caurant@chimie-paristech.f [Laboratoire de Chimie de la Matiere Condensee de Paris (UMR CNRS 7574), Ecole Nationale Superieure de Chimie de Paris (ENSCP, Chimie-ParisTech), 11 rue Pierre et Marie Curie, 75231 Paris (France)

    2010-07-01

    Glass-ceramic materials containing zirconolite (nominally CaZrTi{sub 2}O{sub 7}) crystals in their bulk can be envisaged as potential waste forms for minor actinides (Np, Am, Cm) and Pu immobilization. In this study such matrices are synthesized by crystallization of SiO{sub 2}-Al{sub 2}O{sub 3}-CaO-ZrO{sub 2}-TiO{sub 2} glasses containing lanthanides (Ce, Nd, Eu, Gd, Yb) and actinides (Th) as surrogates. A thin partially crystallized layer containing titanite and anorthite (nominally CaTiSiO{sub 5} and CaAl{sub 2}Si{sub 2}O{sub 8}, respectively) growing from glass surface is also observed. The effect of the nature and concentration of surrogates on the structure, the microstructure and the composition of the crystals formed in the surface layer is presented in this paper. Titanite is the only crystalline phase able to significantly incorporate trivalent lanthanides whereas ThO{sub 2} precipitates in the layer. The crystal growth thermal treatment duration (2-300 h) at high temperature (1050-1200 {sup o}C) is shown to strongly affect glass-ceramics microstructure. For the system studied in this paper, it appears that zirconolite is not thermodynamically stable in comparison with titanite growing form glass surface. Nevertheless, for kinetic reasons, such transformation (i.e. zirconolite disappearance to the benefit of titanite) is not expected to occur during interim storage and disposal of the glass-ceramic waste forms because their temperature will never exceed a few hundred degrees.

  6. CRYSTALLINE CERAMIC WASTE FORMS: REFERENCE FORMULATION REPORT

    Energy Technology Data Exchange (ETDEWEB)

    Brinkman, K.; Fox, K.; Marra, J.

    2012-05-15

    The research conducted in this work package is aimed at taking advantage of the long term thermodynamic stability of crystalline ceramics to create more durable waste forms (as compared to high level waste glass) in order to reduce the reliance on engineered and natural barrier systems. Durable ceramic waste forms that incorporate a wide range of radionuclides have the potential to broaden the available disposal options and to lower the storage and disposal costs associated with advanced fuel cycles. Assemblages of several titanate phases have been successfully demonstrated to incorporate radioactive waste elements, and the multiphase nature of these materials allows them to accommodate variation in the waste composition. Recent work has shown that they can be successfully produced from a melting and crystallization process. The objective of this report is to explain the design of ceramic host systems culminating in a reference ceramic formulation for use in subsequent studies on process optimization and melt property data assessment in support of FY13 melter demonstration testing. The waste stream used as the basis for the development and testing is a combination of the projected Cs/Sr separated stream, the Trivalent Actinide - Lanthanide Separation by Phosphorous reagent Extraction from Aqueous Komplexes (TALSPEAK) waste stream consisting of lanthanide fission products, the transition metal fission product waste stream resulting from the transuranic extraction (TRUEX) process, and a high molybdenum concentration with relatively low noble metal concentrations. In addition to the combined CS/LN/TM High Mo waste stream, variants without Mo and without Mo and Zr were also evaluated. Based on the results of fabricating and characterizing several simulated ceramic waste forms, two reference ceramic waste form compositions are recommended in this report. The first composition targets the CS/LN/TM combined waste stream with and without Mo. The second composition targets

  7. 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

  8. 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.

  9. 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.

  10. Overall assessment of actinide partitioning and transmutation for waste management purposes

    International Nuclear Information System (INIS)

    A program to establish the technical feasibility and incentives for partitioning (i.e., recovering) actinides from fuel cycle wastes and then transmuting them in power reactors to shorter-lived or stable nuclides has recently been concluded at the Oak Ridge National Laboratory. The feasibility was established by experimentally investigating the reduction that can be practicably achieved in the actinide content of the wastes sent to a geologic repository, and the incentives for implementing this concept were defined by determining the incremental costs, risks, and benefits. Eight US Department of Energy laboratories and three private companies participated in the program over its 3-year duration. A reference fuel cycle was chosen based on a self-generated plutonium recycle PWR, and chemical flowsheets based on solvent extraction and ion-exchange techniques were generated that have the potential to reduce actinides in fuel fabrication and reprocessing plant wastes to less than 0.25% of those in the spent fuel. Waste treatment facilities utilizing these flowsheets were designed conceptually, and their costs were estimated. Finally, the short-term (contemporary) risks from fuel cycle operations and long-term (future) risks from deep geologic disposal of the wastes were estimated for cases with and without partitioning and transmutation. It was concluded that, while both actinide partitioning from wastes and transmutation in power reactors appear to be feasible using currently identified and studied technology, implementation of this concept cannot be justified because of the small long-term benefits and substantially increased costs of the concept

  11. Criticality analysis of aggregations of actinides from commerical nuclear waste in geological storage

    International Nuclear Information System (INIS)

    An underground nuclear-waste terminal-storage facility for either spent fuel elements or high level waste from a reprocessing plant will contain large amounts of fissionable actinides. Such a facility must be designed to preclude the concentration of these isotopes into a critical mass. Information on the critical masses of the various isotopes present in spent fuel or high level waste is required as part of such a design effort. This study provides this information. The results of this study will be used, in conjunction with geologic transport rates of the actinide compounds, to estimate mass formation probabilities in waste repositories. A computational model was developed as part of the study to perform criticality calculations rapidly and efficiently and to produce tables and plots of actinide concentration in geologic material versus critical mass. The criticality model uses a discrete ordinates approximation to neutron transport theory and treats six energy groups and spherical geometry. Neutron cross sections were obtained from ENDF/B-IV or ENDF/B-V cross section libraries. Critical masses calculated with the computational model were checked against experimental values and against more detailed calculational values and were found to be from 30 percent less to 10 percent greater. Critical mass calculations were made for five waste types, five waste ages, five actinide elements, and four geologic compositions. Minimum critical masses were calculated for over 400 combinations of the above variables. The relative importance for criticality of the various actinides and waste types is presented in terms of the number of possible critical masses per waste container

  12. Challenges in Modeling the Degradation of Ceramic Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Devanathan, Ramaswami; Gao, Fei; Sun, Xin

    2011-09-01

    We identify the state of the art, gaps in current understanding, and key research needs in the area of modeling the long-term degradation of ceramic waste forms for nuclear waste disposition. The directed purpose of this report is to define a roadmap for Waste IPSC needs to extend capabilities of waste degradation to ceramic waste forms, which overlaps with the needs of the subconsinuum scale of FMM interests. The key knowledge gaps are in the areas of (i) methodology for developing reliable interatomic potentials to model the complex atomic-level interactions in waste forms; (ii) characterization of water interactions at ceramic surfaces and interfaces; and (iii) extension of atomic-level insights to the long time and distance scales relevant to the problem of actinide and fission product immobilization.

  13. Method of processing waste water containing actinide element by fixed tannin

    International Nuclear Information System (INIS)

    Since the waste water from a nuclear power plant is generally in an alkaline range above pH 8, in the case of processing waste water by using fixed tannin, fixed tannin is partially leached to unstable, and the adsorbing elimination rate of actinide elements contained in waste water is decreased. Accordingly, the fixed tannin is immersed and brought into contact with an aqueous solution of ammonia for pre-treatment. it is necessary that the pH value of the aqueous solution of ammonia used is higher than that of the waste water containing the actinide elements, and preferably, within a range of 10 to 12. The time of contact for ensuring the effect of the pre-treatment is at least 30 minutes for the lower limit and 60 minutes for the upper limit. In this way, the adsorbing performance itself can be improved and the processing performance for radioactive waste water can be improved. (T.M.)

  14. 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

  15. Radiation and transmutation effects relevant to solid nuclear waste forms

    International Nuclear Information System (INIS)

    Radiation effects in insulating solids are discussed in a general way as an introduction to the quite sparse published work on radiation effects in candidate nuclear waste forms other than glasses. Likely effects of transmutation in crystals and the chemical mitigation strategy are discussed. It seems probable that radiation effects in solidified HLW will not be serious if the actinides can be wholly incorporated in such radiation-resistant phases as monazite or uraninite

  16. Recovery of actinides from TBP-Na2Co3 scrub-waste solutions: the ARALEX process

    International Nuclear Information System (INIS)

    A flowsheet for the recovery of actinides from TBP-Na2CO3 scrub-waste solutions has been developed, based on batch extraction data, and tested, using laboratory-scale countercurrent extraction techniques. The process, called the ARALEX process, uses 2-ethyl-1-hexanol (2-EHOH) to extract the TBP degradation products (HDBP and H2MBP) from acidified Na2CO3 scrub waste leaving the actinides in the aqueous phase. Dibutyl and monobutyl phosphoric acids are attached to the 2-EHOH molecules through hydrogen bonds, which also diminish the ability of the HDBP and H2MBP to complex actinides. Thus all actinides remain in the aqueous raffinate. Dilute sodium hydroxide solutions can be used to back-extract the dibutyl and monobutyl phosphoric acid esters as their sodium salts. The 2-EHOH can then be recycled. After extraction of the acidified carbonate waste with 2-EHOH, the actinides may be readily extracted from the raffinate with DHDECMP or, in the case of tetra- and hexavalent actinides, with TBP. The ARALEX process can also be applied to other actinide waste streams which contain appreciable concentrations of polar organic compounds (e.g., detergents) that interfere with conventional actinide ion exchange and liquid-liquid extraction procedures. 20 figures, 6 tables

  17. Recovery of actinides from TBP-Na/sub 2/Co/sub 3/ scrub-waste solutions: the ARALEX process

    Energy Technology Data Exchange (ETDEWEB)

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

    1979-08-01

    A flowsheet for the recovery of actinides from TBP-Na/sub 2/CO/sub 3/ scrub-waste solutions has been developed, based on batch extraction data, and tested, using laboratory-scale countercurrent extraction techniques. The process, called the ARALEX process, uses 2-ethyl-1-hexanol (2-EHOH) to extract the TBP degradation products (HDBP and H/sub 2/MBP) from acidified Na/sub 2/CO/sub 3/ scrub waste leaving the actinides in the aqueous phase. Dibutyl and monobutyl phosphoric acids are attached to the 2-EHOH molecules through hydrogen bonds, which also diminish the ability of the HDBP and H/sub 2/MBP to complex actinides. Thus all actinides remain in the aqueous raffinate. Dilute sodium hydroxide solutions can be used to back-extract the dibutyl and monobutyl phosphoric acid esters as their sodium salts. The 2-EHOH can then be recycled. After extraction of the acidified carbonate waste with 2-EHOH, the actinides may be readily extracted from the raffinate with DHDECMP or, in the case of tetra- and hexavalent actinides, with TBP. The ARALEX process can also be applied to other actinide waste streams which contain appreciable concentrations of polar organic compounds (e.g., detergents) that interfere with conventional actinide ion exchange and liquid-liquid extraction procedures. 20 figures, 6 tables.

  18. Mixed Waste Focus Area - Waste form initiative

    International Nuclear Information System (INIS)

    The mission of the US Department of Energy's (DOE) Mixed Waste Focus Area (MWFA) is to provide acceptable technologies that enable implementation of mixed waste treatment systems which are developed in partnership with end-users, stakeholders, tribal governments, and regulators. To accomplish this mission, a technical baseline was established in 1996 and revised in 1997. The technical baseline forms the basis for determining which technology development activities will be supported by the MWFA. The primary attribute of the technical baseline is a set of prioritized technical deficiencies or roadblocks related to implementation of mixed waste treatment systems. The Waste Form Initiative (WFI) was established to address an identified technical deficiency related to waste form performance. The primary goal of the WFI was to ensure that the mixed low-level waste (MLLW) treatment technologies being developed, currently used, or planned for use by DOE would produce final waste forms that meet the waste acceptance criteria (WAC) of the existing and/or planned MLLW disposal facilities. The WFI was limited to an evaluation of the disposal requirements for the radioactive component of MLLW. Disposal requirements for the hazardous component are dictated by the Resource Conservation and Recovery Act (RCRA), and were not addressed. This paper summarizes the technical basis, strategy, and results of the activities performed as part of the WFI

  19. STRONTIUM AND ACTINIDE SEPARATIONS FROM HIGH LEVEL NUCLEAR WASTE SOLUTIONS USING MONOSODIUM TITANATE 1. SIMULANT TESTING

    Energy Technology Data Exchange (ETDEWEB)

    HOBBS, D. T.; BARNES, M. J.; PULMANO, R. L.; MARSHALL, K. M.; EDWARDS, T. B.; BRONIKOWSKI, M. G.; FINK, S. D.

    2005-04-14

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 137}Cs, {sup 90}Sr and alpha-emitting radionuclides (i.e., actinides) prior to disposal. Separation processes planned at SRS include caustic side solvent extraction, for {sup 137}Cs removal, and ion exchange/sorption of {sup 90}Sr and alpha-emitting radionuclides with an inorganic material, monosodium titanate (MST). The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes {sup 238}Pu, {sup 239}Pu and {sup 240}Pu. This paper provides a summary of data acquired to measure the performance of MST to remove strontium and actinides from simulated waste solutions. These tests evaluated the influence of ionic strength, temperature, solution composition and the oxidation state of plutonium.

  20. Vitreous ceramic waste form for waste immobilization

    International Nuclear Information System (INIS)

    Vitreous ceramic waste forms are being developed to complement glass waste forms in supporting DOE's environmental restoration efforts. The vitreous ceramics are composed of various metal oxide crystalline phases embedded in a silicate glass matrix. The vitreous ceramics are appropriate final waste forms for waste streams that contain large amounts of scrap metals and elements with low solubilities in glass, and have low-flux contents. Homogeneous glass waste forms are appropriate for wastes with sufficient fluxes and low metal contents. Therefore, utilization of both glass and vitreous ceramics waste forms will make vitrification technology applicable to the treatment of a much larger range of radioactive and mixed wastes. The controlled crystallization in vitreous ceramics resulted in formation of durable crystalline phases and durable residual glass matrix. The durable crystalline phases in vitreous ceramics included Ca3(PO4)2, magnetite (Fe2+Ni,Mn)Fe3+2O4, hibonite Ca(Al,Fe,Zr,Cr)12O19, baddeyelite ZrO2, zirconolite CaZrTi,O, and corundum Al2O3, which are thermodynamically more stable than normal glasses and are also less soluble in water than glasses. The durable glassy matrix in vitreous ceramics is due to the enrichment of silica and alumina during the crystallization process of vitreous ceramic formation. The vitreous ceramics showed exceptional long-term chemical durability and the processability of vitreous ceramics were also demonstrated at both bench- and pilot-scale. This paper briefly describes the use of vitreous ceramics for treating sample mixed wastes with high contents of either Cr, Fe, Zr, and Al, or alkalis

  1. ENHANCED CHEMICAL CLEANING OF SRS WASTE TANKS TO IMPROVE ACTINIDE SOLUBILITY

    Energy Technology Data Exchange (ETDEWEB)

    Rudisill, T.; Thompson, M.

    2011-09-20

    Processes for the removal of residual sludge from SRS waste tanks have historically used solutions containing up to 0.9 M oxalic acid to dissolve the remaining material following sludge removal. The selection of this process was based on a comparison of a number of studies performed to evaluate the dissolution of residual sludge. In contrast, the dissolution of the actinide mass, which represents a very small fraction of the waste, has not been extensively studied. The Pu, Np, and Am in the sludge is reported to be present as hydrated and crystalline oxides. To identify aqueous solutions which have the potential to increase the solubility of the actinides, the alkaline and mildly acidic test solutions shown below were selected as candidates for use in a series of solubility experiments. The efficiency of the solutions in solubilizing the actinides was evaluated using a simulated sludge prepared by neutralizing a HNO{sub 3} solution containing Pu, Np, and Am. The hydroxide concentration was adjusted to a 1.2 M excess and the solids were allowed to age for several weeks prior to starting the experiments. The sludge was washed with 0.01 M NaOH to prepare the solids for use. Following the addition of an equal portion of the solids to each test solution, the concentrations of Pu, Np, and Am were measured as a function of time over a 792 h (33 day) period to provide a direct comparison of the efficiency of each solution in solubilizing the actinide elements. Although the composition of the sludge was limited to the hydrated actinide oxides (and did not contain other components of demonstrated importance), the results of the study provides guidance for the selection of solutions which should be evaluated in subsequent tests with a more realistic surrogate sludge and actual tank waste.

  2. Materials Characterization Center. Second workshop on irradiation effects in nuclear waste forms. Summary report

    Energy Technology Data Exchange (ETDEWEB)

    Weber, W.J.; Turcotte, R.P.

    1982-01-01

    The purpose of this second workshop on irradiations effects was to continue the discussions initiated at the first workshop and to obtain guidance for the Materials Characterization Center in developing test methods. The following major conclusions were reached: Ion or neutron irradiations are not substitutes for the actinide-doping technique, as described by the MCC-6 Method for Preparation and Characterization of Actinide-Doped Waste Forms, in the final evaluation of any waste form with respect to the radiation effects from actinide decay. Ion or neutron irradiations may be useful for screening tests or more fundamental studies. The use of these simulation techniques as screening tests for actinide decay requires that a correlation between ion or neutron irradiations and actinide decay be established. Such a correlation has not yet been established and experimental programs in this area are highly recommended. There is a need for more fundamental studies on dose-rate effects, temperature dependence, and the nature and importance of alpha-particle effects relative to the recoil nucleus in actinide decay. There are insufficient data presently available to evaluate the potential for damage from ionizing radiation in nuclear waste forms. No additional test methods were recommended for using ion or neutron irradiations to simulate actinide decay or for testing ionization damage in nuclear waste forms. It was recognized that additional test methods may be required and developed as more data become available. An American Society for Testing and Materials (ASTM) Task Group on the Simulation of Radiation Effects in Nuclear Waste Forms (E 10.08.03) was organized to act as a continuing vehicle for discussions and development of procedures, particularly with regard to ion irradiations.

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

    International Nuclear Information System (INIS)

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

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

    International Nuclear Information System (INIS)

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

  5. Subsurface Biogeochemistry of Actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-06-29

    A major scientific challenge in environmental sciences is to identify the dominant processes controlling actinide transport in the environment. It is estimated that currently, over 2200 metric tons of plutonium (Pu) have been deposited in the subsurface worldwide, a number that increases yearly with additional spent nuclear fuel (Ewing et al., 2010). Plutonium has been shown to migrate on the scale of kilometers, giving way to a critical concern that the fundamental biogeochemical processes that control its behavior in the subsurface are not well understood (Kersting et al., 1999; Novikov et al., 2006; Santschi et al., 2002). Neptunium (Np) is less prevalent in the environment; however, it is predicted to be a significant long-term dose contributor in high-level nuclear waste. Our focus on Np chemistry in this Science Plan is intended to help formulate a better understanding of Pu redox transformations in the environment and clarify the differences between the two long-lived actinides. The research approach of our Science Plan combines (1) Fundamental Mechanistic Studies that identify and quantify biogeochemical processes that control actinide behavior in solution and on solids, (2) Field Integration Studies that investigate the transport characteristics of Pu and test our conceptual understanding of actinide transport, and (3) Actinide Research Capabilities that allow us to achieve the objectives of this Scientific Focus Area (SFA and provide new opportunities for advancing actinide environmental chemistry. These three Research Thrusts form the basis of our SFA Science Program (Figure 1).

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

    International Nuclear Information System (INIS)

    Full text of publication follows: 'Mayak' facility is a nuclear waste and spent nuclear fuel reprocessing plant located in Ural Mountains, Russia. The opened pond, Karachay Lake, was used for several decades for the discharge of low- and intermediate level waste solutions containing fission products and traces of actinides. Due to high salt concentration and high density of waste solutions, they are penetrating into the groundwater system that is represented by oxic Eh conditions. The speciation of actinides in groundwater samples collected close to Karachay Lake was studied by successive micro- and ultra-filtrations with subsequent SEM, TEM, nano-SIMS, membrane extraction and other techniques. It was established that U and Np were found in soluble fraction (pass through 10 kD ultra-filter) in the form of their bi- and tri-carbonate complexes that was supported by chemical thermodynamic calculations. In contrast, Pu and Am were bound to nano-colloids 10 kD - 50 nm in size. The SEM and TEM data indicate the presence of variety of different colloidal particles which relative concentration decrease in the row: hydrous ferric oxides (HFO) >> clays ≅ calcite > rutile ≅ hematite ≅ barite ≅ MnO2 > monazite > other phases. The SIMS with submicron resolution (Cameca nanoSIMS-50) was used to study local concentration of actinides. According to the obtained data among different colloids detected in the sample actinides were preferentially bound to HFO and MnO2 while other phases did not sorb actinides. In order to determine actinide speciation bound to HFO colloids XPS and An L3 edge XAFS measurements were done at Siberian Synchrotron Radiation Centre. The storage ring VEPP-3 with electron beam energy of 2 GeV and an average stored current of 80 mA was used as the source of radiation. Since the concentration of actinides in actual samples was too low for XAFS, the samples for measurements were prepared by contacting about 10-5 M solutions of Np(V) and Pu(V) with UFO

  7. Waste form development/test

    International Nuclear Information System (INIS)

    The main objective of this study is to investigate new solidification agents relative to their potential application to wastes generated by advanced high volume reduction technologies, e.g., incinerator ash, dry solids, and ion exchange resins. Candidate materials selected for the solidification of these wastes include a modified sulfur cement and low-density polyethylene, neither of which are currently employed commerically for the solidification of low-level waste (LLW). As both the modified sulfur cement and the polyethylene are thermoplastic materials, a heated screw type extruder is utilized in the production of waste form samples for testing and evaluation. In this regard, work is being conducted to determine the range of conditions under which these solidification agents can be satisfactorily applied to the specific LLW streams and to provide information relevant to operating parameters and process control

  8. Glass-Ceramic Waste Forms for Uranium and Plutonium Residues Wastes - 13164

    Energy Technology Data Exchange (ETDEWEB)

    Stewart, Martin W.A.; Moricca, Sam A.; Zhang, Yingjie; Day, R. Arthur; Begg, Bruce D. [Australian Nuclear Science and Technology Organisation (ANSTO), New Illawarra Road, Lucas Heights, NSW 2234 (Australia); Scales, Charlie R.; Maddrell, Ewan R. [National Nuclear Laboratory, Sellafield, Seascale, Cumbria, UK, CA20 1PG (United Kingdom); Hobbs, Jeff [Sellafield Limited, Sellafield, Seascale, Cumbria, UK, CA20 1PG (United Kingdom)

    2013-07-01

    A program of work has been undertaken to treat plutonium-residues wastes at Sellafield. These have arisen from past fuel development work and are highly variable in both physical and chemical composition. The principal radiological elements present are U and Pu, with small amounts of Th. The waste packages contain Pu in amounts that are too low to be economically recycled as fuel and too high to be disposed of as lower level Pu contaminated material. NNL and ANSTO have developed full-ceramic and glass-ceramic waste forms in which hot-isostatic pressing is used as the consolidation step to safely immobilize the waste into a form suitable for long-term disposition. We discuss development work on the glass-ceramic developed for impure waste streams, in particular the effect of variations in the waste feed chemistry glass-ceramic. The waste chemistry was categorized into actinides, impurity cations, glass formers and anions. Variations of the relative amounts of these on the properties and chemistry of the waste form were investigated and the waste form was found to be largely unaffected by these changes. This work mainly discusses the initial trials with Th and U. Later trials with larger variations and work with Pu-doped samples further confirmed the flexibility of the glass-ceramic. (authors)

  9. NNWSI waste form testing program

    International Nuclear Information System (INIS)

    A waste form testing program has been developed to ensure that the release rate of radionuclides from the engineered barrier system will meet NRC and EPA regulatory requirements. Waste form performance testing will be done under unsaturated, low water availability conditions which represent the expected repository conditions. Testing will also be done under conditions of total immersion of the waste form in repository-type water to cover the possibility that localized portions of the repository might contain standing water. Testing of reprocesses waste forms for CHLW and DHLW will use reaction vessels fabricated from Topopah Spring tuff. Chemical elements which are expected to show the highest release rates in the mildly oxidizing environment of the Topopah Spring tuff horizon at Yucca Mountain are Np and Tc. To determine the effect of residual canister material and of corrosion products from the canister/overpack, waste form testing will be done in the presence of these materials. The release rate of all radionuclides which are subject to NRC and EPA regulations will be measured, and the interactive effects of the released radionuclide and the rock reaction vessels will be determined. The testing program for spent fuel will determine the release rate from bare spent fuel pellets and from Zircaloy clad spent fuel where the cladding contains minor defects. A metal testing program for Zircaloy will establish the expected lifetime of the cladding material. Estimation of the state of cladding for fuel presently in reactor pool storage will provide baseline data for Zircaloy containment credit. 9 references, 4 figures

  10. Ageing of a phosphate ceramic used to immobilize chloride contaminated actinide waste

    Science.gov (United States)

    Metcalfe, B. L.; Donald, I. W.; Fong, S. K.; Gerrard, L. A.; Strachan, D. M.; Scheele, R. D.

    2009-03-01

    A process for the immobilization of intermediate level waste containing a significant quantity of chloride using Ca3(PO4)2 as the host material has been developed. Waste ions are incorporated into two phosphate-based phases, chlorapatite [Ca5(PO4)3Cl] and spodiosite [Ca2(PO4)Cl]. Non-active trials performed using Sm as the actinide surrogate demonstrated the durability of these phases in aqueous solution. Trials of the process, in which actinide-doped materials were used, were performed at PNNL which confirmed the wasteform resistant to aqueous leaching. Initial leach trials conducted on 239Pu/241Am loaded ceramic at 313 K/28 days gave normalized mass losses of 1.2 × 10-5 g m-2 and 2.7 × 10-3 g m-2 for Pu and Cl, respectively. In order to assess the response of the phases to radiation-induced damage, accelerated ageing trials were performed on samples in which the 239Pu was replaced with 238Pu. No changes to the crystalline structure of the waste were detected in the XRD spectra after the samples had experienced an α radiation fluence of 4 × 1018 g-1. Leach trials showed that there was an increase in the P and Ca release rates but no change in the Pu release rate.

  11. Ageing of a phosphate ceramic used to immobilize chloride contaminated actinide waste

    Energy Technology Data Exchange (ETDEWEB)

    Metcalfe, B.L. [Materials Science Research Division, AWE plc, Aldermaston, Reading (United Kingdom)], E-mail: brian.metcalfe@awe.co.uk; Donald, I.W.; Fong, S.K.; Gerrard, L.A. [Materials Science Research Division, AWE plc, Aldermaston, Reading (United Kingdom); Strachan, D.M.; Scheele, R.D. [Pacific Northwest National Laboratories, Richland, WA (United States)

    2009-03-31

    A process for the immobilization of intermediate level waste containing a significant quantity of chloride using Ca{sub 3}(PO{sub 4}){sub 2} as the host material has been developed. Waste ions are incorporated into two phosphate-based phases, chlorapatite [Ca{sub 5}(PO{sub 4}){sub 3}Cl] and spodiosite [Ca{sub 2}(PO{sub 4})Cl]. Non-active trials performed using Sm as the actinide surrogate demonstrated the durability of these phases in aqueous solution. Trials of the process, in which actinide-doped materials were used, were performed at PNNL which confirmed the wasteform resistant to aqueous leaching. Initial leach trials conducted on {sup 239}Pu/{sup 241}Am loaded ceramic at 313 K/28 days gave normalized mass losses of 1.2 x 10{sup -5} g m{sup -2} and 2.7 x 10{sup -3} g m{sup -2} for Pu and Cl, respectively. In order to assess the response of the phases to radiation-induced damage, accelerated ageing trials were performed on samples in which the {sup 239}Pu was replaced with {sup 238}Pu. No changes to the crystalline structure of the waste were detected in the XRD spectra after the samples had experienced an {alpha} radiation fluence of 4 x 10{sup 18} g{sup -1}. Leach trials showed that there was an increase in the P and Ca release rates but no change in the Pu release rate.

  12. Ageing of a phosphate ceramic used to immobilize chloride contaminated actinide waste

    Energy Technology Data Exchange (ETDEWEB)

    Metcalfe, Brian L.; Donald, Ian W.; Fong, Shirley K.; Gerrard, Lee A.; Strachan, Denis M.; Scheele, Randall D.

    2009-03-31

    AWE has developed a process for the immobilization of ILW waste containing a significant quantity of chloride using Ca3(PO4)2 as the host material. Waste ions are incorporated into two phosphate based phases, chlorapatite, Ca5(PO4)3Cl, and spodiosite, Ca2(PO4)Cl. Non-active trials performed at AWE using samarium as the actinide surrogate demonstrated the durability of these phases in aqueous solution. Trials of the process using actinide-doped material were performed at PNNL which confirmed the immobilized wasteform resistant to aqueous leaching. Initial leach trials conducted on 239Pu /241Am loaded ceramic at 40°C/28 days gave normalized mass losses of 1.2 x 10-5 g.m-2 and 2.7 x 10-3 g.m-2 for Pu and Cl respectively. In order to assess the response of the phases to radiation-induced damage, accelerated ageing trials were performed on samples in which the 239Pu was replaced by 238Pu. No changes to the crystalline structure of the waste were detected using XRD after the samples had experienced a radiation dose of 4 x 1018 α.g-1. Leach trials showed that there had been an increase in the P and Ca release rates but no change in the Pu release rate.

  13. Actinide separation of high-level waste using solvent extractants on magnetic microparticles

    International Nuclear Information System (INIS)

    Polymeric-coated ferromagnetic particles with an absorbed layer of octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) diluted by tributyl phosphate (TBP) are being evaluated for application in the separation and the recovery of low concentrations of americium and plutonium from nuclear waste solutions. Due to their chemical nature, these extractants selectively complex americium and plutonium contaminants onto the particles, which can be recovered from the waste solution using a magnet. The effectiveness of the extractant-absorbed particles at removing transuranics (TRU) from simulated solutions and various nitric acid solutions was measured by gamma and liquid scintillation counting of plutonium and americium. The HNO3 concentration range was 0.01 M to 6M. The partition coefficients (Kd) for various actinides at 2M HNO3 were determined to be between 3,000 and 30,000. These values are larger than those projected for TRU recovery by traditional liquid/liquid extraction. Results from transmission electron microscopy indicated a large dependence of Kd on relative magnetite location within the polymer and the polymer surface area. Energy disperse spectroscopy demonstrated homogeneous metal complexation on the polymer surface with no metal clustering. The radiolytic stability of the particles was determined by using 60Co gamma irradiation under various conditions. The results showed that Kd more strongly depends on the nitric acid dissolution rate of the magnetite than the gamma irradiation dose. Results of actinide separation from simulated high-level waste representative of that at various DOE sites are also discussed

  14. Bidentate organophosphorus extractants: purification, properties and applications to removal of actinides from acidic waste solutions

    Energy Technology Data Exchange (ETDEWEB)

    Schulz, W.W.; McIsaac, L.D.

    1977-05-01

    At both Hanford and Idaho, DHDECMP (dihexyl-N, N-diethylcarbamylmethylene phosphonate) continuous counter-current solvent extraction processes are being developed for removal of americium, plutonium, and, in some cases, other actinides from acidic wastes generated at these locations. Bench and, eventually, pilot and plant-scale testing and application of these processes have been substantially enhanced by the discovery of suitable chemical and physical methods of removing deleterious impurities from technical-grade DHDECMP. Flowsheet details, as well as various properties of purified DHDECMP extractants, are enumerated.

  15. Minimization of actinide waste by multirecycling of thoriated fuels in an EPR

    OpenAIRE

    2009-01-01

    This master’s thesis explores how to minimize the long-lived actinide waste that is produced in nuclear power plants by performing simulations of thoriated nuclear fuels in existing reactor designs. An European pressurized water reactor (EPR) assembly fueled with a mixture of thorium and highly enriched uranium (20% and 90% 235U) was simulated. The spent thoriated fuel is less active, and for a much shorter period of time, than uranium or uranium/plutonium fuels and less decay heat is gene...

  16. Coated particle waste form development

    International Nuclear Information System (INIS)

    Coated particle waste forms have been developed as part of the multibarrier concept at Pacific Northwest Laboratory under the Alternative Waste Forms Program for the Department of Energy. Primary efforts were to coat simulated nuclear waste glass marbles and ceramic pellets with low-temperature pyrolytic carbon (LT-PyC) coatings via the process of chemical vapor deposition (CVD). Fluidized bed (FB) coaters, screw agitated coaters (SAC), and rotating tube coaters were used. Coating temperatures were reduced by using catalysts and plasma activation. In general, the LT-PyC coatings did not provide the expected high leach resistance as previously measured for carbon alone. The coatings were friable and often spalled off the substrate. A totally different concept, thermal spray coating, was investigated at PNL as an alternative to CVD coating. Flame spray, wire gun, and plasma gun systems were evaluated using glass, ceramic, and metallic coating materials. Metal plasma spray coatings (Al, Sn, Zn, Pb) provided a two to three orders-of-magnitude increase in chemical durability. Because the aluminum coatings were porous, the superior leach resistance must be due to either a chemical interaction or to a pH buffer effect. Because they are complex, coated waste form processes rank low in process feasibility. Of all the possible coated particle processes, plasma sprayed marbles have the best rating. Carbon coating of pellets by CVD ranked ninth when compared with ten other processes. The plasma-spray-coated marble process ranked sixth out of eleven processes

  17. Loading Actinides in Multilayered Structures for Nuclear Waste Treatment: The First Case Study of Uranium Capture with Vanadium Carbide MXene.

    Science.gov (United States)

    Wang, Lin; Yuan, Liyong; Chen, Ke; Zhang, Yujuan; Deng, Qihuang; Du, Shiyu; Huang, Qing; Zheng, Lirong; Zhang, Jing; Chai, Zhifang; Barsoum, Michel W; Wang, Xiangke; Shi, Weiqun

    2016-06-29

    Efficient nuclear waste treatment and environmental management are important hurdles that need to be overcome if nuclear energy is to become more widely used. Herein, we demonstrate the first case of using two-dimensional (2D) multilayered V2CTx nanosheets prepared by HF etching of V2AlC to remove actinides from aqueous solutions. The V2CTx material is found to be a highly efficient uranium (U(VI)) sorbent, evidenced by a high uptake capacity of 174 mg g(-1), fast sorption kinetics, and desirable selectivity. Fitting of the sorption isotherm indicated that the sorption followed a heterogeneous adsorption model, most probably due to the presence of heterogeneous adsorption sites. Density functional theory calculations, in combination with X-ray absorption fine structure characterizations, suggest that the uranyl ions prefer to coordinate with hydroxyl groups bonded to the V-sites of the nanosheets via forming bidentate inner-sphere complexes. PMID:27267649

  18. Loading Actinides in Multilayered Structures for Nuclear Waste Treatment: The First Case Study of Uranium Capture with Vanadium Carbide MXene.

    Science.gov (United States)

    Wang, Lin; Yuan, Liyong; Chen, Ke; Zhang, Yujuan; Deng, Qihuang; Du, Shiyu; Huang, Qing; Zheng, Lirong; Zhang, Jing; Chai, Zhifang; Barsoum, Michel W; Wang, Xiangke; Shi, Weiqun

    2016-06-29

    Efficient nuclear waste treatment and environmental management are important hurdles that need to be overcome if nuclear energy is to become more widely used. Herein, we demonstrate the first case of using two-dimensional (2D) multilayered V2CTx nanosheets prepared by HF etching of V2AlC to remove actinides from aqueous solutions. The V2CTx material is found to be a highly efficient uranium (U(VI)) sorbent, evidenced by a high uptake capacity of 174 mg g(-1), fast sorption kinetics, and desirable selectivity. Fitting of the sorption isotherm indicated that the sorption followed a heterogeneous adsorption model, most probably due to the presence of heterogeneous adsorption sites. Density functional theory calculations, in combination with X-ray absorption fine structure characterizations, suggest that the uranyl ions prefer to coordinate with hydroxyl groups bonded to the V-sites of the nanosheets via forming bidentate inner-sphere complexes.

  19. Secondary Waste Cast Stone Waste Form Qualification Testing Plan

    Energy Technology Data Exchange (ETDEWEB)

    Westsik, Joseph H.; Serne, R. Jeffrey

    2012-09-26

    The Hanford Tank Waste Treatment and Immobilization Plant (WTP) is being constructed to treat the 56 million gallons of radioactive waste stored in 177 underground tanks at the Hanford Site. The WTP includes a pretreatment facility to separate the wastes into high-level waste (HLW) and low-activity waste (LAW) fractions for vitrification and disposal. The LAW will be converted to glass for final disposal at the Integrated Disposal Facility (IDF). Cast Stone – a cementitious waste form, has been selected for solidification of this secondary waste stream after treatment in the ETF. The secondary-waste Cast Stone waste form must be acceptable for disposal in the IDF. This secondary waste Cast Stone waste form qualification testing plan outlines the testing of the waste form and immobilization process to demonstrate that the Cast Stone waste form can comply with the disposal requirements. Specifications for the secondary-waste Cast Stone waste form have not been established. For this testing plan, Cast Stone specifications are derived from specifications for the immobilized LAW glass in the WTP contract, the waste acceptance criteria for the IDF, and the waste acceptance criteria in the IDF Permit issued by the State of Washington. This testing plan outlines the testing needed to demonstrate that the waste form can comply with these waste form specifications and acceptance criteria. The testing program must also demonstrate that the immobilization process can be controlled to consistently provide an acceptable waste form product. This testing plan also outlines the testing needed to provide the technical basis for understanding the long-term performance of the waste form in the disposal environment. These waste form performance data are needed to support performance assessment analyses of the long-term environmental impact of the secondary-waste Cast Stone waste form in the IDF

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1997-01-01

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

  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. Production, disposal, and relative toxicity of long-lived fission products and actinides in the radioactive wastes from nuclear fuel cycles

    International Nuclear Information System (INIS)

    Chapters are devoted to the following topics: predicted future development of nuclear energy in the German Federal Republic and in Western Europe, fuel cycle variations and production of fission products and actinides in the radioactive waste from reprocessed nuclear fuels, long-lived fission products and actinides in the waste streams from the reprocessing of nuclear fuels, relative toxicity index, presently preferred waste management concepts, and alternative concepts for the elimination of high-level wastes

  3. TSA waste stream and final waste form composition

    International Nuclear Information System (INIS)

    A final vitrified waste form composition, based upon the chemical compositions of the input waste streams, is recommended for the transuranic-contaminated waste stored at the Transuranic Storage Area of the Radioactive Waste Management Complex at the Idaho National Engineering Laboratory. The quantities of waste are large with a considerable uncertainty in the distribution of various waste materials. It is therefore impractical to mix the input waste streams into an ''average'' transuranic-contaminated waste. As a result, waste stream input to a melter could vary widely in composition, with the potential of affecting the composition and properties of the final waste form. This work examines the extent of the variation in the input waste streams, as well as the final waste form under conditions of adding different amounts of soil. Five prominent Rocky Flats Plant 740 waste streams are considered, as well as nonspecial metals and the ''average'' transuranic-contaminated waste streams. The metals waste stream is the most extreme variation and results indicate that if an average of approximately 60 wt% of the mixture is soil, the final waste form will be predominantly silica, alumina, alkaline earth oxides, and iron oxide. This composition will have consistent properties in the final waste form, including high leach resistance, irrespective of the variation in waste stream. For other waste streams, much less or no soil could be required to yield a leach resistant waste form but with varying properties

  4. 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)

  5. Determination of long-lived fission products and actinides in Savannah River Site HLW sludge and glass for waste acceptance

    International Nuclear Information System (INIS)

    Savannah River Site (SRS) is immobilizing the radioactive, high-level waste sludge in Tank 51 into a borosilicate glass for disposal in a geologic repository. A requirement for repository acceptance is that SRS report the concentrations of certain fission product and actinide radionuclides in the glass. This paper presents measurements of many of these concentrations in both Tank 51 sludge and the final glass. The radionuclides were measured by inductively coupled plasma mass spectrometry and α, β, and γ counting methods. Examples of the radionuclides are 90Sr, 137Cs, 238U and , 239Pu. Concentrations in the glass are 3.1 times lower due to dilution of the sludge with a nonradioactive glass forming frit in the vitrification process. Results also indicated that in both the sludge and glass the relative concentrations of the long lived fission products insoluble in caustic are in proportion to their yields from the fission of 235U waste in the SRS reactors. This allowed the calculation of a fission yield scaling factor. This factor in addition to the sludge dilution factor can be used to estimate concentrations of waste acceptance radionuclides that cannot be measured in the glass. Examples of these radionuclides are 79Se, 93Zr, and 107Pd. (author)

  6. Radium institute research on actinide separation from high-level waste. Review

    International Nuclear Information System (INIS)

    Development of efficient technologies for recovery of long-lived radionuclides from high-level wastes (HLW) is urgent for implementation of the promising management methods (transmutation and disposal), as well as for existing practice of HLW management. In Russia at 'Mayak' radiochemical plant since 1996 there has been in operation the industrial facility UE-35 which provides the recovery of cesium and strontium from HLW. The next stage is aimed at development and implementation of actinide separation technology from HLW. For this purpose the following four processes are studied and tested: processes based on chlorinated cobalt dicarbollide (ChCoDiC-process), isoamyldialkyl-phosphine oxide (POR-process), diphenyldibutylcarbamoylphosphine oxide (modified TRUEX-process) and mixture of ChCoDiC, carbamoylphosphine oxide (CMPO) and polyethylene glycol (PEG) (UNEX-process). After comprehensive study of extraction, physico-chemical and operational properties of selected extraction systems, testing of processes was conducted at test facilities with the use of actual or simulated HLW. Mixer-settlers and centrifugal contactors were used as extraction equipment in these tests. The test results show that the ChCoDiC-process can afford recovery of transplutonium and rare-earth elements (TPE and REE) from HLW and separation of them into fractions. POR-process and modified TRUEX-process enable to recover from HLW uranium, neptunium, plutonium, TPE, REE and technetium with the possibility for production of individual fractions. UNEX-process permits to attain simultaneous recovery of actinides, REE, cesium and strontium from HLW. During tests the potentialities of UNEX-process for obtaining such fractions as cesium, cesium+strontium and actinides+REE at stripping stage were demonstrated as well. (author)

  7. CERAMIC WASTE FORM DATA PACKAGE

    Energy Technology Data Exchange (ETDEWEB)

    Amoroso, J.; Marra, J.

    2014-06-13

    The purpose of this data package is to provide information about simulated crystalline waste forms that can be used to select an appropriate composition for a Cold Crucible Induction Melter (CCIM) proof of principle demonstration. Melt processing, viscosity, electrical conductivity, and thermal analysis information was collected to assess the ability of two potential candidate ceramic compositions to be processed in the Idaho National Laboratory (INL) CCIM and to guide processing parameters for the CCIM operation. Given uncertainties in the CCIM capabilities to reach certain temperatures throughout the system, one waste form designated 'Fe-MP' was designed towards enabling processing and another, designated 'CAF-5%TM-MP' was designed towards optimized microstructure. Melt processing studies confirmed both compositions could be poured from a crucible at 1600{degrees}C although the CAF-5%TM-MP composition froze before pouring was complete due to rapid crystallization (upon cooling). X-ray diffraction measurements confirmed the crystalline nature and phase assemblages of the compositions. The kinetics of melting and crystallization appeared to vary significantly between the compositions. Impedance spectroscopy results indicated the electrical conductivity is acceptable with respect to processing in the CCIM. The success of processing either ceramic composition will depend on the thermal profiles throughout the CCIM. In particular, the working temperature of the pour spout relative to the bulk melter which can approach 1700{degrees}C. The Fe-MP composition is recommended to demonstrate proof of principle for crystalline simulated waste forms considering the current configuration of INL's CCIM. If proposed modifications to the CCIM can maintain a nominal temperature of 1600{degrees}C throughout the melter, drain, and pour spout, then the CAF-5%TM-MP composition should be considered for a proof of principle demonstration.

  8. 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)

  9. 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)

  10. Leaching of actinides and technetium from simulated high-level waste glass

    International Nuclear Information System (INIS)

    Leach tests were conducted using a modified version of the IAEA procedure to study the behavior of glass waste-solution interactions. Release rates were determined for Tc, U, Np, Pu, Am, Cm, and Si in the following solutions: WIPP B salt brine, NaCl (287 g/l), NaCl (1.76 g/1), CaCl2 (1.66 g/l), NaHCO3 (2.52 g/l), and deionized water. The leach rates for all elements decreased an order of magnitude from their initial values during the first 20 to 30 days leaching time. The sodium bicarbonate solution produced the highest elemental release rates, while the saturated salt brine and deionized water in general gave the lowest release. Technetium has the highest initial release of all elements studied. The technetium release rates, however, decreased by over four orders of magnitude in 150 days of leaching time. In the prepared glass, technetium was phase separated, concentrating on internal pore surfaces. Neptunium, in all cases except CaCl2 solution, shows the highest actinide release rate. In general, curium and uranium have the lowest release rates. The range of actinide release rates is from 10-5 to 10-8 g/cm2/day. 25 figures, 7 tables

  11. A comparison of radioactive waste from first generation fusion reactors and fast fission reactors with actinide recycling

    International Nuclear Information System (INIS)

    Limitations of the fission fuel resources will presumably mandate the replacement of thermal fission reactors by fast fission reactors that operate on a self-sufficient closed fuel cycle. This replacement might take place within the next one hundred years, so the direct competitors of fusion reactors will be fission reactors of the latter rather than the former type. Also, fast fission reactors, in contrast to thermal fission reactors, have the potential for transmuting long-lived actinides into short-lived fission products. The associated reduction of the long-term activation of radioactive waste due to actinides makes the comparison of radioactive waste from fast fission reactors to that from fusion reactors more rewarding than the comparison of radioactive waste from thermal fission reactors to that from fusion reactors. Radioactive waste from an experimental and a commercial fast fission reactor and an experimental and a commercial fusion reactor has been characterized. The fast fission reactors chosen for this study were the Experimental Breeder Reactor 2 and the Integral Fast Reactor. The fusion reactors chosen for this study were the International Thermonuclear Experimental Reactor and a Reduced Activation Ferrite Helium Tokamak. The comparison of radioactive waste parameters shows that radioactive waste from the experimental fast fission reactor may be less hazardous than that from the experimental fusion reactor. Inclusion of the actinides would reverse this conclusion only in the long-term. Radioactive waste from the commercial fusion reactor may always be less hazardous than that from the commercial fast fission reactor, irrespective of the inclusion or exclusion of the actinides. The fusion waste would even be far less hazardous, if advanced structural materials, like silicon carbide or vanadium alloy, were employed

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

    Science.gov (United States)

    Rose, S. J.; Wilson, J. N.; Capellan, N.; David, S.; Guillemin, P.; Ivanov, E.; Méplan, O.; Nuttin, A.; Siem, S.

    2012-02-01

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

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

    Directory of Open Access Journals (Sweden)

    Nuttin A.

    2012-02-01

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

  14. Polyphase ceramic and glass-ceramic forms for immobilizing ICPP high-level nuclear waste

    International Nuclear Information System (INIS)

    Polyphase ceramic and glass-ceramic forms have been consolidated from simulated Idaho Chemical Processing Plant wastes by hot isostatic pressing calcined waste and chemical additives by 10000C or less. The ceramic forms can contain over 70 wt% waste with densities ranging from 3.5 to 3.85 g/cm3, depending upon the formulation. Major phases are CaF2, CaZrTi207, CaTiO3, monoclinic ZrO2, and amorphous intergranular material. The relative fraction of the phases is a function of the chemical additives (TiO2, CaO, and SiO2) and consolidation temperature. Zirconolite, the major actinide host, makes the ceramic forms extremely leach resistant for the actinide simulant U238. The amorphous phase controls the leach performance for Sr and Cs which is improved by the addition of SiO2. Glass-ceramic forms were also consolidated by HIP at waste loadings of 30 to 70 wt% with densities of 2.73 to 3.1 g/cm3 using Exxon 127 borosilicate glass frit. The glass-ceramic forms contain crystalline CaF2, Al203, and ZrSi04 (zircon) in a glass matrix. Natural mineral zircon is a stable host for 4+ valent actinides. 17 references, 3 figures, 5 tables

  15. Radiation damage in natural materials: implications for radioactive waste forms

    International Nuclear Information System (INIS)

    The long-term effect of radiation damage on waste forms, either crystalline or glass, is a factor in the evaluation of the integrity of waste disposal mediums. Natural analogs, such as metamict minerals, provide one approach for the evaluaton of radiation damage effects that might be observed in crystalline waste forms, such as supercalcine or synroc. Metamict minerals are a special class of amorphous materials which were initially crystalline. Although the mechanism for the loss of crystallinity in these minerals (mostly actinide-containing oxides and silicates) is not clearly understood, damage caused by alpha particles and recoil nuclei is critical to the metamictization process. The study of metamict minerals allows the evaluation of long-term radiation damage effects, particularly changes in physical and chemical properties such as microfracturing, hydrothermal alteration, and solubility. In addition, structures susceptible to metamictization share some common properties: (1) complex compositions; (2) some degree of covalent bonding, instead of being ionic close-packed MO/sub x/ structures; and (3) channels or interstitial voids which may accommodate displaced atoms or absorbed water. On the basis of these empirical criteria, minerals such as pollucite, sodalite, nepheline and leucite warrant careful scrutiny as potential waste form phases. Phases with the monazite or fluorite structures are excellent candidates

  16. Leaching of actinide-doped nuclear waste glass in a tuff-dominated system

    International Nuclear Information System (INIS)

    A laboratory leaching test has been performed as part of a project to evaluate the suitability of tuff rocks at Yucca Mountain, Nevada, as a site for a high-level nuclear waste repository. Glass samples were placed in water inside tuff vessels, and then the tuff vessels were placed in water inside Teflon containers. Glass-component leach rates and migration through the tuff were measured for samples of the ATM-8 actinide glass, which is a PNL 76-68 based glass doped with low levels of 99Tc, 237Np, 238U, and 239Pu to simulate wastes. Disc samples of this glass were leached at 900C for 30, 90, and 183 days inside tuff vessels using a natural groundwater (J-13 well-water) as the leachant. At the end of each leaching interval, the J-13 water present inside and outside the rock vessel was analyzed for glass components in solutions. Boron, molybdenum, and technetium appear to migrate through the rock at rates that depend on the porosity of each vessel and the time. The actinide elements were found only in the inner leachate. Normalized elemental mass loss values for boron, molybdenum, and technetium were calculated using concentrations of the inner and outer leachates and assuming a negligible retention on the rock. The maximum normalized release was 2.3 g/m2 for technetium. Boron, molybdenum, technetium, and neptunium were released linearly with respect to each other, with boron and molybdenum released at about 85% of the technetium rate, and neptunium at 5 to 10% of the technetium rate. Plutonium was found at low levels in the inner leachate but was strongly sorbed on the steel and Teflon supports. Neptunium was sorbed to a lesser extent. 8 refs., 6 figs., 6 tabs

  17. Low temperature waste form process intensification

    Energy Technology Data Exchange (ETDEWEB)

    Fox, K. M. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Cozzi, A. D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Hansen, E. K. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Hill, K. A. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-09-30

    This study successfully demonstrated process intensification of low temperature waste form production. Modifications were made to the dry blend composition to enable a 50% increase in waste concentration, thus allowing for a significant reduction in disposal volume and associated costs. Properties measurements showed that the advanced waste form can be produced using existing equipment and processes. Performance of the waste form was equivalent or better than the current baseline, with approximately double the amount of waste incorporation. The results demonstrate the feasibility of significantly accelerating low level waste immobilization missions across the DOE complex and at environmental remediation sites worldwide.

  18. Determination of long-lived fission products and actinides in Savannah River site HLW sludge and glass for waste acceptance

    International Nuclear Information System (INIS)

    Savannah River Site (SRS) is currently immobilizing the radioactive, caustic, high-level waste sludge in Tank 51 into a borosilicate glass for disposal in a geologic repository. A requirement for repository acceptance is that SRS report the concentrations of certain fission product and actinide radionuclides in the glass. This paper presents measurements of many of these concentrations in both Tank 51 sludge and the final glass. The radionuclides were measured by inductively coupled plasma - mass spectrometry and α, β, and γ counting methods. Examples of the radionuclides are Sr-90, Cs-137, U-238, Pu-239, and Cm-244. Concentrations in the glass are 3.1 times lower due to dilution of the sludge with a nonradioactive glass forming frit in the vitrification process. Results also indicated that in both the sludge and glass the relative concentrations of the long lived fission products insoluble in caustic area in proportion to their yields from the fission of U-235 in the SRS reactors. This allowed the calculation of a fission yield scaling factor. This factor in addition to the sludge dilution factor can be used to estimate concentrations of waste acceptance radionuclides that cannot be measured in the glass

  19. Radiation and Thermal Stability of Murataite Ceramics Nuclear Waste Forms

    Science.gov (United States)

    Lian, J.; Yudintsev, S. V.; Stefanovsky, S. V.

    2006-05-01

    The wide range of complex nuclear wastes requires a variety of robust hosts for long-term storage during disposal. Wastes with high actinide and iron concentrations have generated intense interest in murataite ceramics as a candidate waste form due to its four distinct cation sites as well as cation vacancies. Critical to this application is the radiation stability of the waste host. We have determined both the radiation and thermal stabilities of murataite ceramics using in situ observations in a transmission electron microscope during ion bombardment at the Electron Microscopy Center at Argonne National Laboratory. A central issue for structural stability is radiation damage-induced crystalline-to-amorphous transformation that may result in macroscopic swelling, cracking and phase decomposition. Such a response would lead to a significant change in chemical durability and release of incorporated radionuclides. We found that, murataite ceramics are susceptible to ion beam induce ordered-disordered transition and amorphization. The ion dose required for amorphization was determined as a function of temperature and the degree of initial structural disorder. The upper temperature limit for amorphization of murataites was determined to be in the range of 860 K to 1060 K for 1 MeV Kr2+ ion irradiation. Decrease of the susceptibility to irradiation induced amorphization for disordered murataite, suggests that the amorphization susceptibility depends, in part, on the initial degree of intrinsic disorder prior to irradiation. The thermal stability of murataite polytypes was studied by in-situ TEM observation. Phase decomposition with the precipitation of Fe-rich nanocrystals was induced in the murataite structure. The phase decomposition and nanocrystal formation have no significant effects on the radiation resistance of murataite ceramics used as potential host phases for the immobilization of actinides.

  20. Decay analysis of pre-actinide and trans-actinide nuclei formed using various projectiles on a 197Au target at ECN*=60 MeV

    Science.gov (United States)

    Grover, Neha; Kaur, Gurvinder; Sharma, Manoj K.

    2016-01-01

    The collective clusterization approach of the dynamical cluster decay model (DCM) has been applied to study the decay of odd mass nuclei 223Pa*, 215Fr*, 227Np*, and 233Am*, which are formed in heavy-ion-induced reactions. The aim of this study is to investigate the decay pattern and related behavior of these heavy mass nuclei formed in four distinct reactions involving different projectiles (with mass A =18 -36 ) induced on 197Au target nucleus. Further, in order to analyze the role of deformations, the calculations have been done by considering spherical choice of fragmentation as well as with inclusion of quadrupole (β2) deformation. For the heavy mass region, with fission being the dominant decay mode, an attempt has been made to investigate the effect of projectile mass in reference to fission decay patterns of the pre-actinide 215Fr* nucleus and the trans-actinide nuclei 227Np* 223Pa*, 223Am* and formed at common excitation energy, ECN*=60 MeV . Besides this, the shell closure effects and the role of orientation have been explored, which suggest the presence of a noncompound nucleus process such as quasifission (QF) for the odd mass nuclei under consideration. For both the compound nucleus and the noncompound nucleus processes, the results obtained using DCM are found to have nice agreement with experimental observations. The isotopic and isobaric analysis is also worked out so as to have a comprehensive idea about the dynamics involved.

  1. Special Form Testing of Sealed Source Encapsulation for High-Alpha-Activity Actinide Materials

    Energy Technology Data Exchange (ETDEWEB)

    Martinez, Oscar A [ORNL

    2016-01-01

    In the United States all transportation of radioactive material is regulated by the U.S. Department of Transportation (DOT). Beginning in 2008 a new type of sealed-source encapsulation package was developed and tested by Oak Ridge National Laboratory (ORNL). These packages contain high-alpha-activity actinides and are regulated and transported in accordance with the requirements for DOT Class 7 hazardous material. The DOT provides specific regulations pertaining to special form encapsulation designs. The special form designation indicates that the encapsulated radioactive contents have a very low probability of dispersion even when subjected to significant structural events. The special form designs have been shown to simplify the delivery, transport, acceptance, and receipt processes. It is intended for these sealed-source encapsulations to be shipped to various facilities making it very advantageous for them to be certified as special form. To this end, DOT Certificates of Competent Authority (CoCAs) have been sought for the design suitable for containing high-alpha-activity actinide materials. This design consists of the high-alpha-activity material encapsulated within a triangular zirconia canister, referred to as a ZipCan, tile that is then enclosed by a spherical shell. The spherical shell design, with ZipCan tile inside, was tested for compliance with the special form regulations found in 49 CFR 173.469. The spherical enclosure was subjected to 9-m impact, 1 m percussion, and 10-minute thermal tests at the Packaging Evaluation Facility located at the National Transportation Research Center in Knoxville, TN USA and operated by ORNL. Before and after each test, the test units were subjected to a helium leak check and a bubble test. The ZipCan tiles and core were also subjected to the tests required for ISO 2919:2012(E), including a Class IV impact test and heat test and subsequently subjected to helium leakage rate tests [49 CFR 173.469(a)(4)(i)]. The impact

  2. Crystalline Ceramic Waste Forms: Comparison Of Reference Process For Ceramic Waste Form Fabrication

    Energy Technology Data Exchange (ETDEWEB)

    Brinkman, K. S. [Savannah River National Laboratory; Marra, J. C. [Savannah River National Laboratory; Amoroso, J. [Savannah River National Laboratory; Tang, M. [Los Alamos National Laboratory

    2013-08-22

    The research conducted in this work package is aimed at taking advantage of the long term thermodynamic stability of crystalline ceramics to create more durable waste forms (as compared to high level waste glass) in order to reduce the reliance on engineered and natural barrier systems. Durable ceramic waste forms that incorporate a wide range of radionuclides have the potential to broaden the available disposal options and to lower the storage and disposal costs associated with advanced fuel cycles. Assemblages of several titanate phases have been successfully demonstrated to incorporate radioactive waste elements, and the multiphase nature of these materials allows them to accommodate variation in the waste composition. Recent work has shown that they can be produced from a melting and crystallization process. The objective of this report is to explore the phase formation and microstructural differences between lab scale melt processing in varying gas environments with alternative densification processes such as Hot Pressing (HP) and Spark Plasma Sintering (SPS). The waste stream used as the basis for the development and testing is a simulant derived from a combination of the projected Cs/Sr separated stream, the Trivalent Actinide - Lanthanide Separation by Phosphorous reagent Extraction from Aqueous Komplexes (TALSPEAK) waste stream consisting of lanthanide fission products, the transition metal fission product waste stream resulting from the transuranic extraction (TRUEX) process, and a high molybdenum concentration with relatively low noble metal concentrations. Melt processing as well as solid state sintering routes SPS and HP demonstrated the formation of the targeted phases; however differences in microstructure and elemental partitioning were observed. In SPS and HP samples, hollandite, pervoskite/pyrochlore, zirconolite, metallic alloy and TiO{sub 2} and Al{sub 2}O{sub 3} were observed distributed in a network of fine grains with small residual pores

  3. New Fission-Product Waste Forms: Development and Characterization

    Energy Technology Data Exchange (ETDEWEB)

    Alexandra Navrotsky

    2010-07-30

    Research performed on the program “New Fission Product Waste Forms: Development and Characterization,” in the last three years has fulfilled the objectives of the proposal which were to 1) establish ceramic waste forms for disposing of Cs, Sr and minor actinides, 2) fully characterize the phase relationships, structures and thermodynamic and kinetic stabilities of promising waste forms, 3) establish a sound technical basis for understanding key waste form properties, such as melting temperatures and aqueous durability, based on an in-depth understanding of waste form structures and thermochemistry, and 4) establish synthesis, testing, scaleup and commercialization routes for wasteform implementation through out in-kind collaborations. In addition, since Cs and Sr form new elements by radioactive decay, the behavior and thermodynamics of waste forms containing different proportions of Cs, Sr and their decay products were discovered using non-radioactive analogues. Collaborations among researchers from three institutions, UC Davis, Sandia National Laboratories, and Shott Inc., were formed to perform the primary work on the program. The unique expertise of each of the members in the areas of waste form development, structure/property relationships, hydrothermal and high temperature synthesis, crystal/glass production, and thermochemistry was critical to program success. In addition, collaborations with the Brigham Young Univeristy, Ben Gurion University, and Los Alamos National Laboratory, were established for standard entropies of ceramic waste forms, sol-gel synthesis, and high temperature synthesis. This work has had a significant impact in a number of areas. First, the studies of the thermodynamic stability of the mineral analogues provided an important technical foundation for assessment the viability of multicomponent oxide phases for Cs and Sr removal. Moreover, the thermodynamic data discovered in this program established information on the reaction

  4. Role of Microbes as Biocolloids in the Transport of Actinides from a Deep Underground Radioactive Waste Repository

    Energy Technology Data Exchange (ETDEWEB)

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

    1998-12-17

    We investigated the interaction of dissolved actinides Th, U, Np Zgpu, and Am, with a pure and a mixed culture of halophilic bactezia isolated from the Waste Isolation H.Iot Plant repository under anaerobic conditions to evaluate their potentiaI transport as biocolloids from the waste site. The sizes of the bacterial cells studied ranged from ().54 x 0.48 pm to 7.7 x 0.67pm Using sequential mimofiltration, we determined the ~~ation of actinides with fi-ee-living (mobile) bacterial cells suspended in a fluid medium containing. NaCl or M=W12 brine, at various phaes of their growth cycIes. The number of suspended kcteria rangy-d born 106 to 109 cells ml-*. Tine amount of actinide associatd with the wspend~ cell fraction (cakzdated & mol cell-*) was very Iow: Th, 10-*2; U, 10-1s - 10-lS; - ~ Np, 1o-15- 10-19; Pu, 10-ls -10-21 ; and h, 10-1* - 10-*9 ; and it varied with the bacteihl - CUIture studied. l%e differe&es in the asswiation are amibuted to the extent of bioamxmdation and biosorption by the bacteria pH, the compo&on of the brine, and the speziation and bioavaiIability of the actinides.

  5. The effects of actinide separation on the radiological consequences of geologic disposal of high-level waste

    International Nuclear Information System (INIS)

    It has often been suggested that the potential hazard to man from the disposal of high-level radioactive waste could be reduced by removing a substantial fraction of the actinide elements. In this report the effects of actinide separation on the radiological consequences of one of the disposal options currently under consideration, that of burial in deep geologic formations, are examined. The results show that the potential radiological impact of geologic disposal of high-level waste arises from both long-lived fission products and actinides (and their daughter radionuclides). Neither class of radionuclides is of overriding importance and actinide separation would therefore reduce the radiological impact to only a limited extent and over limited periods. There might be a case for attempting to reduce doses from 237Np. To achieve this it appears to be necessary to separate both neptunium and its precursor element americium. However, there are major uncertainties in the data needed to predict doses from 237Np; further research is required to resolve these uncertainties. In addition, consideration should be given to alternative methods of reducing the radiological impact of geologic disposal. The conclusions of this assessment differ considerably from those of similar studies based on the concept of toxicity indices. Use of these indices can lead to incorrect allocation of research and development effort. (author)

  6. Hanford Waste Vitrification Plant Project Waste Form Qualification Program Plan

    International Nuclear Information System (INIS)

    The US Department of Energy has created a waste acceptance process to help guide the overall program for the disposal of high-level nuclear waste in a federal repository. This Waste Form Qualification Program Plan describes the hierarchy of strategies used by the Hanford Waste Vitrification Plant Project to satisfy the waste form qualification obligations of that waste acceptance process. A description of the functional relationship of the participants contributing to completing this objective is provided. The major activities, products, providers, and associated scheduling for implementing the strategies also are presented

  7. Liquid secondary waste. Waste form formulation and qualification

    Energy Technology Data Exchange (ETDEWEB)

    Cozzi, A. D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Dixon, K. L. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Hill, K. A. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); King, W. D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Nichols, R. L. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2016-03-01

    The Hanford Site Effluent Treatment Facility (ETF) currently treats aqueous waste streams generated during Site cleanup activities. When the Hanford Tank Waste Treatment and Immobilization Plant (WTP) begins operations, a liquid secondary waste (LSW) stream from the WTP will need to be treated. The volume of effluent for treatment at the ETF will increase significantly. Washington River Protection Solutions is implementing a Secondary Liquid Waste Immobilization Technology Development Plan to address the technology needs for a waste form and solidification process to treat the increased volume of waste planned for disposal at the Integrated Disposal Facility IDF). Waste form testing to support this plan is composed of work in the near term to demonstrate the waste form will provide data as input to a performance assessment (PA) for Hanford’s IDF.

  8. Miscellaneous Waste-Form FEPs

    Energy Technology Data Exchange (ETDEWEB)

    A. Schenker

    2000-12-08

    The US DOE must provide a reasonable assurance that the performance objectives for the Yucca Mountain Project (YMP) potential radioactive-waste repository can be achieved for a 10,000-year post-closure period. The guidance that mandates this direction is under the provisions of 10 CFR Part 63 and the US Department of Energy's ''Revised Interim Guidance Pending Issuance of New US Nuclear Regulatory Commission (NRC) Regulations (Revision 01, July 22, 1999), for Yucca Mountain, Nevada'' (Dyer 1999 and herein referred to as DOE's Interim Guidance). This assurance must be demonstrated in the form of a performance assessment that: (1) identifies the features, events, and processes (FEPs) that might affect the performance of the potential geologic repository; (2) examines the effects of such FEPs on the performance of the potential geologic repository; (3) estimates the expected annual dose to a specified receptor group; and (4) provides the technical basis for inclusion or exclusion of specific FEPs.

  9. Combined Waste Form Cost Trade Study

    Energy Technology Data Exchange (ETDEWEB)

    Dirk Gombert; Steve Piet; Timothy Trickel; Joe Carter; John Vienna; Bill Ebert; Gretchen Matthern

    2008-11-01

    A new generation of aqueous nuclear fuel reprocessing, now in development under the auspices of the DOE Office of Nuclear Energy (NE), separates fuel into several fractions, thereby partitioning the wastes into groups of common chemistry. This technology advance enables development of waste management strategies that were not conceivable with simple PUREX reprocessing. Conventional wisdom suggests minimizing high level waste (HLW) volume is desirable, but logical extrapolation of this concept suggests that at some point the cost of reducing volume further will reach a point of diminishing return and may cease to be cost-effective. This report summarizes an evaluation considering three groupings of wastes in terms of cost-benefit for the reprocessing system. Internationally, the typical waste form for HLW from the PUREX process is borosilicate glass containing waste elements as oxides. Unfortunately several fission products (primarily Mo and the noble metals Ru, Rh, Pd) have limited solubility in glass, yielding relatively low waste loading, producing more glass, and greater disposal costs. Advanced separations allow matching the waste form to waste stream chemistry, allowing the disposal system to achieve more optimum waste loading with improved performance. Metals can be segregated from oxides and each can be stabilized in forms to minimize the HLW volume for repository disposal. Thus, a more efficient waste management system making the most effective use of advanced waste forms and disposal design for each waste is enabled by advanced separations and how the waste streams are combined. This trade-study was designed to juxtapose a combined waste form baseline waste treatment scheme with two options and to evaluate the cost-benefit using available data from the conceptual design studies supported by DOE-NE.

  10. Comparison of different options for minor actinide transmutation in the frame of the French law for waste management

    International Nuclear Information System (INIS)

    In the frame of the French Act for waste management which has been passed by French Parliament on June 28th, 2006, it is requested to obtain in 2012 an assessment of industrial perspectives of partitioning and transmutation of long-lived elements. These studies must be carried out in tight connection with GENIV systems development. The expected results must include the evaluation of technical and economic scenarios taking into account the optimization options between the minor actinide transmutation processes, their interim storage and geological disposal, including an analysis of several criteria. In this perspective, the CEA has established a working group named 'GT TES' (Working Group on Technical and Economic Scenarios) involving EDF and AREVA to define scenarios, the various criteria to evaluate them, to conduct these evaluations and then to highlight the key results. The group also relied on ANDRA for the geological storage studies. The scenarios evaluations take place in the French context. The nuclear energy production is supposed to remain constant during the scenarios and equal to 430 TWhe/year in accordance with the current French nuclear power installed capacity of 60 GW(e). The deployment of the first Sodium-cooled Fast Reactor (SFR) starts in 2040, considering that at this date the SFR technology should be mature. Several management schemes of minor actinides have been studied: Plutonium recycling in SFR (minor actinides are sent to the waste). Plutonium recycling and minor actinide (or Am alone) transmutation in SFR and in homogeneous mode ('Hom.'). Plutonium recycling and minor actinide (or Am alone) transmutation in SFR and in heterogeneous mode ('Het.'). Plutonium recycling in SFR and minor actinide transmutation in Accelerator-Driven-System (ADS). The criteria used to analyze these different scenarios, should take into account the viewpoint of scientists, industrials, administrations, and the general public. They are listed below: Inventories and

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

    International Nuclear Information System (INIS)

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

  12. Treatment and recycling of spent nuclear fuel. Actinide partitioning - Application to waste management

    International Nuclear Information System (INIS)

    subsequent to its in-reactor dwell time, spent fuel still contains large amounts of materials that are recoverable, for value-added energy purposes (uranium, plutonium), together with fission products, and minor actinides, making up the residues from nuclear reactions. The treatment and recycling of spent nuclear fuel, as implemented in France, entail that such materials be chemically partitioned. The development of the process involved, and its deployment on an industrial scale stand as a high achievement of French science, and technology. Treatment and recycling allow both a satisfactory management of nuclear waste to be implemented, and substantial savings, in terms of fissile material. Bolstered of late as it has been, due to spectacularly skyrocketing uranium prices, this strategy is bound to become indispensable, with the advent of the next generation of fast reactors. This Monograph surveys the chemical process used for spent fuel treatment, and its variants, both current, and future. It outlines currently ongoing investigations, setting out the challenges involved, and recent results obtained by CEA. (authors)

  13. Treatment and recycling of spent nuclear fuel. Actinide partitioning - Application to waste management

    Energy Technology Data Exchange (ETDEWEB)

    Abonneau, E.; Baron, P.; Berthon, C.; Berthon, L.; Beziat, A.; Bisel, I.; Bonin, L.; Bosse, E.; Boullis, B.; Broudic, J.C.; Charbonnel, M.C.; Chauvin, N.; Den Auwer, C.; Dinh, B.; Duhamet, J.; Escleine, J.M.; Grandjean, S.; Guilbaud, P.; Guillaneux, D.; Guillaumont, D.; Hill, C.; Lacquement, J.; Masson, M.; Miguirditchian, M.; Moisy, P.; Pelletier, M.; Ravenet, A.; Rostaing, C.; Royet, V.; Ruas, A.; Simoni, E.; Sorel, C.; Vaudano, A.; Venault, L.; Warin, D.; Zaetta, A.; Pradel, P.; Bonin, B.; Bouquin, B.; Dozol, M.; Lecomte, M.; Forestier, A.; Beauvy, M.; Berthoud, G.; Defranceschi, M.; Ducros, G.; Guerin, Y.; Latge, C.; Limoge, Y.; Madic, C.; Santarini, G.; Seiler, J.M.; Sollogoob, P.; Vernaz, E.; Bazile, F.; Parisot, J.P.; Finot, P.; Roberts, J.F

    2008-07-01

    subsequent to its in-reactor dwell time, spent fuel still contains large amounts of materials that are recoverable, for value-added energy purposes (uranium, plutonium), together with fission products, and minor actinides, making up the residues from nuclear reactions. The treatment and recycling of spent nuclear fuel, as implemented in France, entail that such materials be chemically partitioned. The development of the process involved, and its deployment on an industrial scale stand as a high achievement of French science, and technology. Treatment and recycling allow both a satisfactory management of nuclear waste to be implemented, and substantial savings, in terms of fissile material. Bolstered of late as it has been, due to spectacularly skyrocketing uranium prices, this strategy is bound to become indispensable, with the advent of the next generation of fast reactors. This Monograph surveys the chemical process used for spent fuel treatment, and its variants, both current, and future. It outlines currently ongoing investigations, setting out the challenges involved, and recent results obtained by CEA. (authors)

  14. Humic substances in performance assessment of nuclear waste disposal: Actinide and iodine migration in the far-field. Third technical progress report

    International Nuclear Information System (INIS)

    The present report describes progress within the third and final year of the EC-project 'Humic Substances in Performance Assessment of Nuclear Waste Disposal: Actinide and Iodine Migration in the Far-Field'. The work conducted within the present project builds on a number of previous activities/project supported by the Commission. It finds its continuation within different EC FP 6 instruments and also provides for additional continued cooperation through network structures resulting from the broad cooperation within the project. Without being a formal requirement of the Commission or co-funding bodies, this report documents results in great technical detail and makes the results available to a broad scientific community. The report contains an executive summary written by the coordinator. More detailed results are given as individual contributions in the form of 12 annexes. Not all results are discussed or referred to in the executive summary report and thus readers with a deeper interest also need to consult the annexes. The overall objectives were to generate knowledge about the impact of humic substances on the migration of actinides and iodine in the far-field of a nuclear waste repository. In the beginning, focus was rather on the potential enhancement due to humic colloid mediated radionuclide transport. Thereby, sources, inventory, stability and mobility of dissolved humic substances in their colloidal form formed a key topic. Other key topics were the interaction with actinides and iodine, transport studies under near-natural conditions in the laboratory, rationalization of knowledge in models and application to three migration cases for visualization of the overall outcome. Changes relative to the original objectives were given by moving emphasis of natural chemical analogue studies from the question of kinetic exchange constants for different inventories in natural and laboratory systems to the study of anthropogenic actinide contaminants in the Irish Sea

  15. DWPF waste form compliance plan (Draft Revision)

    International Nuclear Information System (INIS)

    The Department of Energy currently has over 100 million liters of high-level radioactive waste in storage at the Savannah River Site (SRS). In the late 1970's, the Department of Energy recognized that there were significant safety and cost advantages associated with immobilizing the high-level waste in a stable solid form. Several alternative waste forms were evaluated in terms of product quality and reliability of fabrication. This evaluation led to a decision to build the Defense Waste Processing Facility (DWPF) at SRS to convert the easily dispersed liquid waste to borosilicate glass. In accordance with the NEPA (National Environmental Policy Act) process, an Environmental Impact Statement was prepared for the facility, as well as an Environmental Assessment of the alternative waste forms, and issuance of a Record of Decision (in December, 1982) on the waste form. The Department of Energy, recognizing that start-up of the DWPF would considerably precede licensing of a repository, instituted a Waste Acceptance Process to ensure that these canistered waste forms would be acceptable for eventual disposal at a federal repository. This report is a revision of the DWPF compliance plan

  16. 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.)

  17. Rietveld analysis of ceramic nuclear waste forms

    Energy Technology Data Exchange (ETDEWEB)

    White, T.J. [Univ. of South Australia, Ingle Farm (Australia); Mitamura, H. [Japan Atomic Energy Research Institute, Ibaraki (Japan)

    1994-12-31

    Powder X-ray diffraction patterns were collected from three titanate waste forms - a calcine powder, a prototype ceramic without waste, and a ceramic containing 10 wt% JW-A simulated waste - and interpreted quantitatively using the Rietveld method. The calcine consisted of fluorite, pyrochlore, rutile, and amorphous material. The prototype waste form contained rutile, hollandite, zirconolite and perovskite. The phase constitution of the JW-A ceramic was freudenbergite, loveringite, hollandite, zirconolite, perovskite and baddeleyite. Procedures for the collection of X-ray data are described, as are assumptions inherent in the Rietveld approach. A selection of refined crystal data are presented.

  18. Ceramic and glass radioactive waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Readey, D.W.; Cooley, C.R. (comps.)

    1977-01-01

    This report contains 14 individual presentations and 6 group reports on the subject of glass and polycrystalline ceramic radioactive waste forms. It was the general consensus that the information available on glass as a waste form provided a good basis for planning on the use of glass as an initial waste form, that crystalline ceramic forms could also be good waste forms if much more development work were completed, and that prediction of the chemical and physical stability of the waste form far into the future would be much improved if the basic synergistic effects of low temperature, radiation and long times were better understood. Continuing development of the polycrystalline ceramic forms was recommended. It was concluded that the leach rate of radioactive species from the waste form is an important criterion for evaluating its suitability, particularly for the time period before solidified waste is permanently placed in the geologic isolation of a Federal repository. Separate abstracts were prepared for 12 of the individual papers; the remaining two were previously abstracted.

  19. 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

  20. Secondary Waste Form Down-Selection Data Package—Fluidized Bed Steam Reforming Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    Qafoku, Nikolla; Westsik, Joseph H.; Strachan, Denis M.; Valenta, Michelle M.; Pires, Richard P.

    2011-09-12

    The Hanford Site in southeast Washington State has 56 million gallons of radioactive and chemically hazardous wastes stored in 177 underground tanks (ORP 2010). The U.S. Department of Energy (DOE), Office of River Protection (ORP), through its contractors, is constructing the Hanford Tank Waste Treatment and Immobilization Plant (WTP) to convert the radioactive and hazardous wastes into stable glass waste forms for disposal. Within the WTP, the pretreatment facility will receive the retrieved waste from the tank farms and separate it into two treated process streams. These waste streams will be vitrified, and the resulting waste canisters will be sent to offsite (high-level waste [HLW]) and onsite (immobilized low-activity waste [ILAW]) repositories. As part of the pretreatment and ILAW processing, liquid secondary wastes will be generated that will be transferred to the Effluent Treatment Facility (ETF) on the Hanford Site for further treatment. These liquid secondary wastes will be converted to stable solid waste forms that will be disposed of in the Integrated Disposal Facility (IDF). To support the selection of a waste form for the liquid secondary wastes from WTP, Washington River Protection Solutions (WRPS) has initiated secondary waste form testing work at Pacific Northwest National Laboratory (PNNL). In anticipation of a down-selection process for a waste form for the Solidification Treatment Unit to be added to the ETF, PNNL is developing data packages to support that down-selection. The objective of the data packages is to identify, evaluate, and summarize the existing information on the four waste forms being considered for stabilizing and solidifying the liquid secondary wastes. At the Hanford Site, the FBSR process is being evaluated as a supplemental technology for treating and immobilizing Hanford LAW radioactive tank waste and for treating secondary wastes from the WTP pretreatment and LAW vitrification processes.

  1. Iodine waste form summary report (FY 2007).

    Energy Technology Data Exchange (ETDEWEB)

    Krumhansl, James Lee; Nenoff, Tina Maria; McMahon, Kevin A.; Gao, Huizhen; Rajan, Ashwath Natech

    2007-11-01

    This new program at Sandia is focused on Iodine waste form development for GNEP cycle needs. Our research has a general theme of 'Waste Forms by Design' in which we are focused on silver loaded zeolite waste forms and related metal loaded zeolites that can be validated for chosen GNEP cycle designs. With that theme, we are interested in materials flexibility for iodine feed stream and sequestration material (in a sense, the ability to develop a universal material independent on the waste stream composition). We also are designing the flexibility to work in a variety of repository or storage scenarios. This is possible by studying the structure/property relationship of existing waste forms and optimizing them to our current needs. Furthermore, by understanding the properties of the waste and the storage forms we may be able to predict their long-term behavior and stability. Finally, we are working collaboratively with the Waste Form Development Campaign to ensure materials durability and stability testing.

  2. 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

  3. Low-risk alternative waste forms for problematic high-level and long-lived nuclear wastes

    International Nuclear Information System (INIS)

    Full text: The highest cost component the nuclear waste clean up challenge centres on high-level waste (HLW) and consequently the greatest opportunity for cost and schedule savings lies with optimising the approach to HLW cleanup. The waste form is the key component of the immobilisation process. To achieve maximum cost savings and optimum performance the selection of the waste form should be driven by the characteristics of the specific nuclear waste to be immobilised, rather than adopting a single baseline approach. This is particularly true for problematic nuclear wastes that are often not amenable to a single baseline approach. The use of tailored, high-performance, alternative waste forms that include ceramics and glass-ceramics, coupled with mature process technologies offer significant performance improvements and efficiency savings for a nuclear waste cleanup program. It is the waste form that determines how well the waste is locked up (chemical durability), and the number of repository disposal canisters required (waste loading efficiency). The use of alternative waste forms for problematic wastes also lowers the overall risk by providing high performance HLW treatment alternatives. The benefits tailored alternative waste forms bring to the HLW cleanup program will be briefly reviewed with reference to work carried out on the following: The HLW calcines at the Idaho National Laboratory; SYNROC ANSTO has developed a process utilising a glass-ceramic combined with mature hot-isostatic pressing (HIP) technology and has demonstrated this at a waste loading of 80 % and at a 30 kg HIP scale. The use of this technology has recently been estimated to result in a 70 % reduction in waste canisters, compared to the baseline borosilicate glass technology; Actinide-rich waste streams, particularly the work being done by SYNROC ANSTO with Nexia Solutions on the Plutonium-residues wastes at Sellafield in the UK, which if implemented is forecast to result in substantial

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

    International Nuclear Information System (INIS)

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

  5. SEPARATIONS AND WASTE FORMS CAMPAIGN IMPLEMENTATION PLAN

    Energy Technology Data Exchange (ETDEWEB)

    Vienna, John D.; Todd, Terry A.; Peterson, Mary E.

    2012-11-26

    This Separations and Waste Forms Campaign Implementation Plan provides summary level detail describing how the Campaign will achieve the objectives set-forth by the Fuel Cycle Reasearch and Development (FCRD) Program. This implementation plan will be maintained as a living document and will be updated as needed in response to changes or progress in separations and waste forms research and the FCRD Program priorities.

  6. Chemical compatibility of DWPF canistered waste forms

    International Nuclear Information System (INIS)

    The Waste Acceptance Preliminary Specifications (WAPS) require that the contents of the canistered waste form are compatible with one another and the stainless steel canister. The canistered waste form is a closed system comprised of a stainless steel vessel containing waste glass, air, and condensate. This system will experience a radiation field and an elevated temperature due to radionuclide decay. This report discusses possible chemical reactions, radiation interactions, and corrosive reactions within this system both under normal storage conditions and after exposure to temperatures up to the normal glass transition temperature, which for DWPF waste glass will be between 440 and 460 degrees C. Specific conclusions regarding reactions and corrosion are provided. This document is based on the assumption that the period of interim storage prior to packaging at the federal repository may be as long as 50 years

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

    Science.gov (United States)

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

    2015-10-01

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

  8. Designing Advanced Ceramic Waste Forms for Electrochemical Processing Salt Waste

    Energy Technology Data Exchange (ETDEWEB)

    Ebert, W. L. [Argonne National Lab. (ANL), Argonne, IL (United States); Snyder, C. T. [Argonne National Lab. (ANL), Argonne, IL (United States); Frank, Steven [Argonne National Lab. (ANL), Argonne, IL (United States); Riley, Brian [Argonne National Lab. (ANL), Argonne, IL (United States)

    2016-03-01

    This report describes the scientific basis underlying the approach being followed to design and develop “advanced” glass-bonded sodalite ceramic waste form (ACWF) materials that can (1) accommodate higher salt waste loadings than the waste form developed in the 1990s for EBR-II waste salt and (2) provide greater flexibility for immobilizing extreme waste salt compositions. This is accomplished by using a binder glass having a much higher Na2O content than glass compositions used previously to provide enough Na+ to react with all of the Cl– in the waste salt and generate the maximum amount of sodalite. The phase compositions and degradation behaviors of prototype ACWF products that were made using five new binder glass formulations and with 11-14 mass% representative LiCl/KCl-based salt waste were evaluated and compared with results of similar tests run with CWF products made using the original binder glass with 8 mass% of the same salt to demonstrate the approach and select a composition for further studies. About twice the amount of sodalite was generated in all ACWF materials and the microstructures and degradation behaviors confirmed our understanding of the reactions occurring during waste form production and the efficacy of the approach. However, the porosities of the resulting ACWF materials were higher than is desired. These results indicate the capacity of these ACWF waste forms to accommodate LiCl/KCl-based salt wastes becomes limited by porosity due to the low glass-to-sodalite volume ratio. Three of the new binder glass compositions were acceptable and there is no benefit to further increasing the Na content as initially planned. Instead, further studies are needed to develop and evaluate alternative production methods to decrease the porosity, such as by increasing the amount of binder glass in the formulation or by processing waste forms in a hot isostatic press. Increasing the amount of binder glass to eliminate porosity will decrease the waste

  9. 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

  10. Lysimeter tests of SRP waste forms

    International Nuclear Information System (INIS)

    A field study, estimated to last 10 years, has been started to define leaching and migration rates of radionuclides from typical SRP buried wastes. The study utilizes 42 lysimeters (6-ft or 10-ft diameter by 10-ft deep) which have been charged with soil and waste to simulate burial ground conditions. Eight waste forms were selected for the study, which represent the bulk of the wastes generated at SRP. This report describes the lysimeter design, the physical and radiological characteristics of the wastes, and the experimental approach. Calculations have also been made which predict the migration of various radionuclides in the lysimeter soil. The calculations should provide guidance during the course of the study, and are the basis of recommendations made for collecting and interpreting data so that important parameters of migration can be evaluated

  11. Alternative Waste Forms for Electro-Chemical Salt Waste

    Energy Technology Data Exchange (ETDEWEB)

    Crum, Jarrod V.; Sundaram, S. K.; Riley, Brian J.; Matyas, Josef; Arreguin, Shelly A.; Vienna, John D.

    2009-10-28

    This study was undertaken to examine alternate crystalline (ceramic/mineral) and glass waste forms for immobilizing spent salt from the Advanced Fuel Cycle Initiative (AFCI) electrochemical separations process. The AFCI is a program sponsored by U.S. Department of Energy (DOE) to develop and demonstrate a process for recycling spent nuclear fuel (SNF). The electrochemical process is a molten salt process for the reprocessing of spent nuclear fuel in an electrorefiner and generates spent salt that is contaminated with alkali, alkaline earths, and lanthanide fission products (FP) that must either be cleaned of fission products or eventually replaced with new salt to maintain separations efficiency. Currently, these spent salts are mixed with zeolite to form sodalite in a glass-bonded waste form. The focus of this study was to investigate alternate waste forms to immobilize spent salt. On a mole basis, the spent salt is dominated by alkali and Cl with minor amounts of alkaline earth and lanthanides. In the study reported here, we made an effort to explore glass systems that are more compatible with Cl and have not been previously considered for use as waste forms. In addition, alternate methods were explored with the hope of finding a way to produce a sodalite that is more accepting of as many FP present in the spent salt as possible. This study was done to investigate two different options: (1) alternate glass families that incorporate increased concentrations of Cl; and (2) alternate methods to produce a mineral waste form.

  12. Preparation techniques for ceramic waste form powder

    International Nuclear Information System (INIS)

    The electrometallurgical treatment of spent nuclear fuels result in a chloride waste salt requiring geologic disposal. Argonne National Laboratory (ANL) is developing ceramic waste forms which can incorporate this waste. Currently, zeolite- or sodalite-glass composites are produced by hot isostatic pressing (HIP) techniques. Powder preparations include dehydration of the raw zeolite powders, hot blending of these zeolite powders and secondary additives. Various approaches are being pursued to achieve adequate mixing, and the resulting powders have been HIPed and characterized for leach resistance, phase equilibria, and physical integrity

  13. Reductive Capacity Measurement of Waste Forms for Secondary Radioactive Wastes

    Energy Technology Data Exchange (ETDEWEB)

    Um, Wooyong; Yang, Jungseok; Serne, R. Jeffrey; Westsik, Joseph H.

    2015-09-28

    The reductive capacities of dry ingredients and final solid waste forms were measured using both the Cr(VI) and Ce(IV) methods and the results were compared. Blast furnace slag (BFS), sodium sulfide, SnF2, and SnCl2 used as dry ingredients to make various waste forms showed significantly higher reductive capacities compared to other ingredients regardless of which method was used. Although the BFS exhibits appreciable reductive capacity, it requires greater amounts of time to fully react. In almost all cases, the Ce(IV) method yielded larger reductive capacity values than those from the Cr(VI) method and can be used as an upper bound for the reductive capacity of the dry ingredients and waste forms, because the Ce(IV) method subjects the solids to a strong acid (low pH) condition that dissolves much more of the solids. Because the Cr(VI) method relies on a neutral pH condition, the Cr(VI) method can be used to estimate primarily the waste form surface-related and readily dissolvable reductive capacity. However, the Cr(VI) method does not measure the total reductive capacity of the waste form, the long-term reductive capacity afforded by very slowly dissolving solids, or the reductive capacity present in the interior pores and internal locations of the solids.

  14. Reductive capacity measurement of waste forms for secondary radioactive wastes

    Science.gov (United States)

    Um, Wooyong; Yang, Jung-Seok; Serne, R. Jeffrey; Westsik, Joseph H.

    2015-12-01

    The reductive capacities of dry ingredients and final solid waste forms were measured using both the Cr(VI) and Ce(IV) methods and the results were compared. Blast furnace slag (BFS), sodium sulfide, SnF2, and SnCl2 used as dry ingredients to make various waste forms showed significantly higher reductive capacities compared to other ingredients regardless of which method was used. Although the BFS exhibits appreciable reductive capacity, it requires greater amounts of time to fully react. In almost all cases, the Ce(IV) method yielded larger reductive capacity values than those from the Cr(VI) method and can be used as an upper bound for the reductive capacity of the dry ingredients and waste forms, because the Ce(IV) method subjects the solids to a strong acid (low pH) condition that dissolves much more of the solids. Because the Cr(VI) method relies on a neutral pH condition, the Cr(VI) method can be used to estimate primarily the waste form surface-related and readily dissolvable reductive capacity. However, the Cr(VI) method does not measure the total reductive capacity of the waste form, the long-term reductive capacity afforded by very slowly dissolving solids, or the reductive capacity present in the interior pores and internal locations of the solids.

  15. Chemical aspects of incinerating highly chlorinated and actinide α contaminated organic waste: application to the Iris process

    International Nuclear Information System (INIS)

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

  16. Characterization of radioactive waste forms. Volume 2

    International Nuclear Information System (INIS)

    This document is the second yearbook for Task 3 of the European Communities 1985-89 programme of research on radioactive waste management and disposal carried out by public organizations and private firms in the Community through cost-sharing contracts with the Commission of the European Communities. The report, in two volumes, describes progress made in 1987 within the field of Task 3: Testing and evaluation of conditioned waste and engineered barriers. The first volume of the report covers Item 3.1 Characterization of low and medium level radioactive waste forms and Item 3.5. Development of test methods for quality assurance. The second volume covers Item 3.2: High-level and alpha waste characterization and Item 3.3: Other engineered barriers. Item 3.4 on the round robin study will be treated in a separate report

  17. Characterization of radioactive waste forms. Volume 1

    International Nuclear Information System (INIS)

    This document is the second yearbook for Task 3 of the European Communities 1985-89 programme of research on radioactive waste management and disposal carried out by public organizations and private firms in the Community through costsharing contracts with the Commission of the European Communities. The report, in two volumes, describes progress made in 1987 within the field of Task 3: Testing and evaluation of conditioned waste and engineered barriers. The first volume of the report covers Item 3.1 Characterization of low and medium-level radioactive waste forms and Item 3.5 Development of test methods for quality assurance. The second volume covers Item 3.2: High-level and alpha waste characterization and Item 3.3: Other engineered barriers. Item 3.4 on the round robin study will be treated in a separate report

  18. WRAP 2A Waste Form Qualification Plan

    Energy Technology Data Exchange (ETDEWEB)

    Burbank, D.A. Jr.

    1993-12-31

    WRAP Module 2A is a facility that will serve to treat retrieved, stored, and newly generated contact-handled mixed low level waste (MLLW) at the Department of Energy`s Hanford site near Richland, Washington. The treatment processes to be used are limited to non-thermal processes, defined as processes operating at a temperature less than 500{degree}F. In addition to waste pretreatment and conditioning processes including sorting, size reduction, and homogenization, the final treatment technologies will consist of immobilization, stabilization, and encapsulation to produce final waste forms that are suitable for disposal in compliance with all applicable regulatory requirements. The wide variety of chemical and physical characteristics exhibited by the WRAP 2A feed streams will necessitate the performance of a comprehensive waste form qualification (WFQ) testing program. The WFQ program will provide the technical basis supporting the process selection and will demonstrate that the selected treatment processes produce final waste forms that will meet all applicable regulatory requirements and performance specifications. This document describes the overall WRAP 2A WFQ program.

  19. Studies of high-level waste form performance at Japan Atomic Energy Research Institute

    Energy Technology Data Exchange (ETDEWEB)

    Banba, Tsunetaka; Mitamura, Hisayoshi; Kuramoto, Kenichi; Kamizono, Hiroshi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment; Inagaki, Yahohiro

    1998-02-01

    The JAERI studies on the properties of the glass and ceramic waste forms, which have been done in the last several years, are described briefly. For the long-term evaluation of glass waste form performance under repository condition, leachability has studied from the standpoints of understanding of alteration layers, effects of groundwater and effects of redox condition using the radioactive or non-radioactive glass samples. The studies revealed that (1) the reactions in the alteration layers, such as crystal growth, continue after the apparent release of elements from the glass almost ceases, (2) under somewhat reducing conditions, Fe dissolves easily into leachates, and hydrated silicate surface layer tends to dissolve more easily with Fe in reduced synthetic groundwater than in deionized water, (3) precipitation of PuO{sub 2}{center_dot}xH{sub 2}O(am) is controlling the leaching of soluble species of Pu under both redox conditions, and the dominant soluble species is Pu(OH){sub 4}{sup 0} under reducing condition. Ceramics are considered as most promising materials for the actinide-rich wastes arising from partitioning and transmutation processes because of their outstanding durability for long term. In the present study, {alpha}-decay damage effects on the density and leaching behavior of perovskite (1 of 3 main minerals forming Synroc) were investigated by an accelerated experiment using the actinide doping technique. A decrease in density of Cm-doped perovskite reaches 1.3% at a dose of 9x10{sup 17} {alpha}-decays{center_dot}g{sup -1}. The leach rate of perovskite increases with an increase in accumulated {alpha}-decay doses. Application of zirconia- and alumina-based ceramics for incorporating actinides was also investigated by inactive laboratory tests with an emphasis on crystallographic phase stability and chemical durability. The yttria-stabilized zirconia is stable crystallographically in the wide ranges of Ce and/or Nd content and have excellent

  20. Dissolution of tailored ceramic nuclear waste forms

    International Nuclear Information System (INIS)

    Dissolution experiments on polyphase, high alumina tailored ceramic nuclear waste forms developed for the chemical immobilization of Savannah River Plant nuclear waste are described. Three forms of leach tests have been adopted; bulk samples conforming to the Materials Characterization Center Static Leach Test (MCC-1), a powdered sample leach test, and a leach test performed on transmission electron microscope thin foil samples. From analysis of these tests the crystalline phases that preferentially dissolve on leaching and the product phases formed are identified and related to the tailoring and processing schemes used in forming the ceramics. The thin foil sample leaching enables the role of intergranular amorphous phases as short-circuit leaching paths in polyphase ceramics to be investigated

  1. Alternative waste forms: a comparative study

    International Nuclear Information System (INIS)

    A characterization study utilizing comparative tests has been conducted to assess product inertness of alternative waste form materials, having evaluated at this point four basic product types: sintered ceramics, glass ceramics, glass and concrete. The seven specific waste form materials studied represent simulated nuclear waste loading of 5% to 100%, processed between room temperature and 12000C and subjected to characterization tests including phase analysis, microstructure, compression testing, volatility and leach testing. Significant conclusions based upon the results obtained to date are: sintered calcine waste form PW-9 does not retain Na, Mo and Cs when leached 900C and, in fact, does not remain a solid; glass and supercalcine are alike under both hydrous and hydrothermal leach conditions with glass exhibiting a greater retention of sodium and molybdenum, supercalcine having a greater retention of cesium, and both forms approximately equal in strontium retention; volatility measurements indicate that an order of magnitude decrease in volatility occurs when a calcine waste form is incorporated in a crystalline or glassy host; glass 76-68 is superior to supercalcine SPC-5B in retention of volatiles below 11000C because of the high release of Na from SPC-5B, however, as the temperature approaches or exceeds the glass melt temperature, volatile losses of the glass equal or exceed that of SPC-5B; glass 76-68 and supercalcine SPC-5B have high compressive strengths when compared to sintered PW-9 and cement products. This is apparently due to a stronger continuum bond resulting from a glassy matrix or crystalline ingrowth over a simple mechanical agglomeration of particles

  2. Melt processed multiphase ceramic waste forms for nuclear waste immobilization

    Energy Technology Data Exchange (ETDEWEB)

    Amoroso, Jake, E-mail: jake.amoroso@srs.gov [Savannah River National Laboratory, Aiken, SC 29808 (United States); Marra, James C. [Savannah River National Laboratory, Aiken, SC 29808 (United States); Tang, Ming [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Lin, Ye; Chen, Fanglin [University of South Carolina, Columbia, SC 29208 (United States); Su, Dong [Brookhaven National Laboratory, Upton, NY 11973 (United States); Brinkman, Kyle S. [Clemson University, Clemson, SC 29634 (United States)

    2014-11-15

    Highlights: • We explored the feasibility of melt processing multiphase titanate-based ceramics. • Melt processing produced phases obtained by alternative processing methods. • Phases incorporated multiple lanthanides and transition metals. • Processing in reducing atmosphere suppressed un-desirable Cs–Mo coupling. • Cr partitions to and stabilizes the hollandite phase, which promotes Cs retention. - Abstract: Ceramic waste forms are promising hosts for nuclear waste immobilization as they have the potential for increased durability and waste loading compared with conventional borosilicate glass waste forms. Ceramics are generally processed using hot pressing, spark plasma sintering, and conventional solid-state reaction, however such methods can be prohibitively expensive or impractical at production scales. Recently, melt processing has been investigated as an alternative to solid-state sintering methods. Given that melter technology is currently in use for High Level Waste (HLW) vitrification in several countries, the technology readiness of melt processing appears to be advantageous over sintering methods. This work reports the development of candidate multi-phase ceramic compositions processed from a melt. Cr additions, developed to promote the formation and stability of a Cs containing hollandite phase were successfully incorporated into melt processed multi-phase ceramics. Control of the reduction–oxidation (Redox) conditions suppressed undesirable Cs–Mo containing phases, and additions of Al and Fe reduced the melting temperature.

  3. Melt processed multiphase ceramic waste forms for nuclear waste immobilization

    Science.gov (United States)

    Amoroso, Jake; Marra, James C.; Tang, Ming; Lin, Ye; Chen, Fanglin; Su, Dong; Brinkman, Kyle S.

    2014-11-01

    Ceramic waste forms are promising hosts for nuclear waste immobilization as they have the potential for increased durability and waste loading compared with conventional borosilicate glass waste forms. Ceramics are generally processed using hot pressing, spark plasma sintering, and conventional solid-state reaction, however such methods can be prohibitively expensive or impractical at production scales. Recently, melt processing has been investigated as an alternative to solid-state sintering methods. Given that melter technology is currently in use for High Level Waste (HLW) vitrification in several countries, the technology readiness of melt processing appears to be advantageous over sintering methods. This work reports the development of candidate multi-phase ceramic compositions processed from a melt. Cr additions, developed to promote the formation and stability of a Cs containing hollandite phase were successfully incorporated into melt processed multi-phase ceramics. Control of the reduction-oxidation (Redox) conditions suppressed undesirable Cs-Mo containing phases, and additions of Al and Fe reduced the melting temperature.

  4. I-NERI-2007-004-K, DEVELOPMENT AND CHARACTERIZATION OF NEW HIGH-LEVEL WASTE FORMS FOR ACHIEVING WASTE MINIMIZATION FROM PYROPROCESSING

    Energy Technology Data Exchange (ETDEWEB)

    S.M. Frank

    2011-09-01

    Work describe in this report represents the final year activities for the 3-year International Nuclear Energy Research Initiative (I-NERI) project: Development and Characterization of New High-Level Waste Forms for Achieving Waste Minimization from Pyroprocessing. Used electrorefiner salt that contained actinide chlorides and was highly loaded with surrogate fission products was processed into three candidate waste forms. The first waste form, a high-loaded ceramic waste form is a variant to the CWF produced during the treatment of Experimental Breeder Reactor-II used fuel at the Idaho National Laboratory (INL). The two other waste forms were developed by researchers at the Korean Atomic Energy Research Institute (KAERI). These materials are based on a silica-alumina-phosphate matrix and a zinc/titanium oxide matrix. The proposed waste forms, and the processes to fabricate them, were designed to immobilize spent electrorefiner chloride salts containing alkali, alkaline earth, lanthanide, and halide fission products that accumulate in the salt during the processing of used nuclear fuel. This aspect of the I-NERI project was to demonstrate 'hot cell' fabrication and characterization of the proposed waste forms. The outline of the report includes the processing of the spent electrorefiner salt and the fabrication of each of the three waste forms. Also described is the characterization of the waste forms, and chemical durability testing of the material. While waste form fabrication and sample preparation for characterization must be accomplished in a radiological hot cell facility due to hazardous radioactivity levels, smaller quantities of each waste form were removed from the hot cell to perform various analyses. Characterization included density measurement, elemental analysis, x-ray diffraction, scanning electron microscopy and the Product Consistency Test, which is a leaching method to measure chemical durability. Favorable results from this

  5. Evaluation and testing of sequestering agents for the removal of actinides from waste streams

    Energy Technology Data Exchange (ETDEWEB)

    Hoffman, D.C.; Romanovski, V.V.; Veeck, A.C. [Lawrence Livermore National Lab., CA (United States)] [and others

    1997-10-01

    The purpose of this project is to evaluate and test the complexing ability of a variety of promising new complexing agents synthesized by Professor Kenneth Raymond`s group at the University of California, Berkeley (ESP-CP TTP Number SF16C311). Some of these derivatives have already shown the potential for selectivity binding Pu(IV) in a wide range of solutions in the presence of other metals. Professor Raymond`s group uses molecular modeling to design and synthesize ligands based on modification of natural siderophores, or their analogs, for chelation of actinides. The ligands are then modified for use as liquid/liquid and solid/liquid extractants. The authors` group at the Glenn T. Seaborg Institute for Transactinium Science (ITS) at Lawrence Livermore National Laboratory determines the complex formation constants between the ligands and actinide ions, the capacity and time dependence for uptake on the resins, and the effect of other metal ions and pH.

  6. Alternative Electrochemical Salt Waste Forms, Summary of FY11-FY12 Results

    Energy Technology Data Exchange (ETDEWEB)

    Riley, Brian J.; Mccloy, John S.; Crum, Jarrod V.; Lepry, William C.; Rodriguez, Carmen P.; Windisch, Charles F.; Matyas, Josef; Westman, Matthew P.; Rieck, Bennett T.; Lang, Jesse B.; Olszta, Matthew J.; Pierce, David A.

    2014-03-26

    The Fuel Cycle Research and Development Program, sponsored by the U.S. Department of Energy Office of Nuclear Energy, is currently investigating alternative waste forms for wastes generated from nuclear fuel processing. One such waste results from an electrochemical separations process, called the “Echem” process. The Echem process utilizes a molten KCl-LiCl salt to dissolve the fuel. This process results in a spent salt containing alkali, alkaline earth, lanthanide halides and small quantities of actinide halides, where the primary halide is chloride with a minor iodide fraction. Pacific Northwest National Laboratory (PNNL) is concurrently investigating two candidate waste forms for the Echem spent-salt: high-halide minerals (i.e., sodalite and cancrinite) and tellurite (TeO2)-based glasses. Both of these candidates showed promise in fiscal year (FY) 2009 and FY2010 with a simplified nonradioactive simulant of the Echem waste. Further testing was performed on these waste forms in FY2011 and FY2012 to assess the possibility of their use in a sustainable fuel cycle. This report summarizes the combined results from FY2011 and FY2012 efforts.

  7. Waste Form Features, Events, and Processes

    Energy Technology Data Exchange (ETDEWEB)

    R. Schreiner

    2004-10-27

    The purpose of this report is to evaluate and document the inclusion or exclusion of the waste form features, events and processes (FEPs) with respect to modeling used to support the Total System Performance Assessment for License Application (TSPA-LA). A screening decision, either Included or Excluded, is given for each FEP along with the technical bases for screening decisions. This information is required by the Nuclear Regulatory Commission (NRC) in 10 CFR 63.114 (d, e, and f) [DIRS 156605]. The FEPs addressed in this report deal with the issues related to the degradation and potential failure of the waste form and the migration of the waste form colloids. For included FEPs, this analysis summarizes the implementation of the FEP in TSPA-LA, (i.e., how the FEP is included). For excluded FEPs, this analysis provides the technical bases for exclusion from TSPA-LA (i.e., why the FEP is excluded). This revision addresses the TSPA-LA FEP list (DTN: MO0407SEPFEPLA.000 [DIRS 170760]). The primary purpose of this report is to identify and document the analyses and resolution of the features, events, and processes (FEPs) associated with the waste form performance in the repository. Forty FEPs were identified that are associated with the waste form performance. This report has been prepared to document the screening methodology used in the process of FEP inclusion and exclusion. The analyses documented in this report are for the license application (LA) base case design (BSC 2004 [DIRS 168489]). In this design, a drip shield is placed over the waste package and no backfill is placed over the drip shield (BSC 2004 [DIRS 168489]). Each FEP may include one or more specific issues that are collectively described by a FEP name and a FEP description. The FEP description may encompass a single feature, process or event, or a few closely related or coupled processes if the entire FEP can be addressed by a single specific screening argument or TSPA-LA disposition. The FEPs are

  8. Synthesis of Waste Form in the Gd-Fe-Al-Ni-Mn-Cr-O System

    International Nuclear Information System (INIS)

    Poly-phase waste form which was the mixture of Gd3Fe2Al3O12 and (NixMn1-x)(FeyCr1-y)2O4 was synthesized. Also, we are intended to examine phase relation and physicochemical properties of coexisted phases in the compositions and to confirm accommodation relation of elements and phases. Two types of phase series were observed: Garnet-perovskite-spinel and Garnet-spinel. The compositions of garnets and spinels were nonstoichiometric, and especially, this poly-phase ceramics may be in a good waste form. The excessive Gd in garnets indicated the immobilization of higher content of actinides. The nonstoichiometric compositions of garnet and spinel were attributed to the formation of perovskite in that perovskite contained Gd, Fe and Al from garnet and Cr from spinel. (authors)

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

    Science.gov (United States)

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

    1973-01-01

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

  10. Evaluation of Cyanex 923-coated magnetic particles for the extraction and separation of lanthanides and actinides from nuclear waste streams

    Energy Technology Data Exchange (ETDEWEB)

    Shaibu, B.S. [Chemical Sciences Division, Regional Research Laboratory (CSIR), Thiruvananthapuram-695019 (India); Reddy, M.L.P. [Chemical Sciences Division, Regional Research Laboratory (CSIR), Thiruvananthapuram-695019 (India)]. E-mail: mlpreddy@yahoo.co.uk; Bhattacharyya, A. [Radiochemistry Division, B.A.R.C, Trombay, Mumbai-400085 (India); Manchanda, V.K. [Radiochemistry Division, B.A.R.C, Trombay, Mumbai-400085 (India)

    2006-06-15

    In the magnetically assisted chemical separation (MACS) process, tiny ferromagnetic particles coated with solvent extractant are used to selectively separate radionuclides and hazardous metals from aqueous waste streams. The contaminant-loaded particles are then recovered from the waste solutions using a magnetic field. The contaminants attached to the magnetic particles are subsequently removed using a small volume of stripping agent. In the present study, Cyanex 923 (trialkylphosphine oxide) coated magnetic particles (cross-linked polyacrylamide and acrylic acid entrapping charcoal and iron oxide, 1:1:1, particle size=1-60 {mu}m) are being evaluated for the possible application in the extraction and separation of lanthanides and actinides from nuclear waste streams. The uptake behaviour of Th(IV), U(VI), Am(III) and Eu(III) from nitric acid solutions was investigated by batch studies. The effects of sorption kinetics, extractant and nitric acid concentrations on the uptake behaviour of metal ions were systematically studied. The influence of fission products (Cs(I), Sr(II)) and interfering ions including Fe(III), Cr(VI), Mg(II), Mn(II), and Al(III) were investigated. The recycling capacity of the extractant-coated magnetic particles was also evaluated.

  11. Evaluation of Cyanex 923-coated magnetic particles for the extraction and separation of lanthanides and actinides from nuclear waste streams

    Science.gov (United States)

    Shaibu, B. S.; Reddy, M. L. P.; Bhattacharyya, A.; Manchanda, V. K.

    2006-06-01

    In the magnetically assisted chemical separation (MACS) process, tiny ferromagnetic particles coated with solvent extractant are used to selectively separate radionuclides and hazardous metals from aqueous waste streams. The contaminant-loaded particles are then recovered from the waste solutions using a magnetic field. The contaminants attached to the magnetic particles are subsequently removed using a small volume of stripping agent. In the present study, Cyanex 923 (trialkylphosphine oxide) coated magnetic particles (cross-linked polyacrylamide and acrylic acid entrapping charcoal and iron oxide, 1:1:1, particle size=1-60 μm) are being evaluated for the possible application in the extraction and separation of lanthanides and actinides from nuclear waste streams. The uptake behaviour of Th(IV), U(VI), Am(III) and Eu(III) from nitric acid solutions was investigated by batch studies. The effects of sorption kinetics, extractant and nitric acid concentrations on the uptake behaviour of metal ions were systematically studied. The influence of fission products (Cs(I), Sr(II)) and interfering ions including Fe(III), Cr(VI), Mg(II), Mn(II), and Al(III) were investigated. The recycling capacity of the extractant-coated magnetic particles was also evaluated.

  12. DSNF and other waste form degradation abstraction

    Energy Technology Data Exchange (ETDEWEB)

    Thornton, Thomas A.

    2000-12-20

    The purpose of this analysis/model report (AMR) is to select and/or abstract conservative degradation models for DOE-(US. Department of Energy) owned spent nuclear fuel (DSNF) and the immobilized ceramic plutonium (Pu) disposition waste forms for application in the proposed monitored geologic repository (MGR) postclosure Total System Performance Assessment (TSPA). Application of the degradation models abstracted herein for purposes other than TSPA should take into consideration the fact that they are, in general, very conservative. Using these models, the forward reaction rate for the mobilization of radionuclides, as solutes or colloids, away from the waste fondwater interface by contact with repository groundwater can then be calculated. This forward reaction rate generally consists of the dissolution reaction at the surface of spent nuclear fuel (SNF) in contact with water, but the degradation models, in some cases, may also include and account for the physical disintegration of the SNF matrix. The models do not, however, account for retardation, precipitation, or inhibition of the migration of the mobilized radionuclides in the engineered barrier system (EBS). These models are based on the assumption that all components of the DSNF waste form are released congruently with the degradation of the matrix.

  13. Development and characterization of solidified forms for high-level wastes: 1978. Annual report

    International Nuclear Information System (INIS)

    Development and characterization of solidified high-level waste forms are directed at determining both process properties and long-term behaviors of various solidified high-level waste forms in aqueous, thermal, and radiation environments. Waste glass properties measured as a function of composition were melt viscosity, melt electrical conductivity, devitrification, and chemical durability. The alkali metals were found to have the greatest effect upon glass properties. Titanium caused a slight decrease in viscosity and a significant increase in chemical durability in acidic solutions (pH-4). Aluminum, nickel and iron were all found to increase the formation of nickel-ferrite spinel crystals in the glass. Four multibarrier advanced waste forms were produced on a one-liter scale with simulated waste and characterized. Glass marbles encapsulated in a vacuum-cast lead alloy provided improved inertness with a minimal increase in technological complexity. Supercalcine spheres exhibited excellent inertness when coated with pyrolytic carbon and alumina and put in a metal matrix, but the processing requirements are quite complex. Tests on simulated and actual high-level waste glasses continue to suggest that thermal devitrification has a relatively small effect upon mechanical and chemical durabilities. Tests on the effects radiation has upon waste forms also continue to show changes to be relatively insignificant. Effects caused by decay of actinides can be estimated to saturate at near 1019 alpha-events/cm3 in homogeneous solids. Actually, in solidified waste forms the effects are usually observed around certain crystals as radiation causes amorphization and swelling of th crystals

  14. 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.

  15. Review of radiation effects in solid-nuclear-waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Weber, W.J.

    1981-09-01

    Radiation effects on the stability of high-level nuclear waste (HLW) forms are an important consideration in the development of technology to immobilize high-level radioactive waste because such effects may significantly affect the containment of the radioactive waste. Since the required containment times are long (10/sup 3/ to 10/sup 6/ years), an understanding of the long-term cumulative effects of radiation damage on the waste forms is essential. Radiation damage of nuclear waste forms can result in changes in volume, leach rate, stored energy, structure/microstructure, and mechanical properties. Any one or combination of these changes might significantly affect the long-term stability of the nuclear waste forms. This report defines the general radiation damage problem in nuclear waste forms, describes the simulation techniques currently available for accelerated testing of nuclear waste forms, and reviews the available data on radiation effects in both glass and ceramic (primarily crystalline) waste forms. 76 references.

  16. Safeguards and retrievability from waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Danker, W.

    1996-05-01

    This report describes issues discussed at a session from the PLutonium Stabilization and Immobilization Workshop related to safeguards and retrievability from waste forms. Throughout the discussion, the group probed the goals of disposition efforts, particularly an understanding of the {open_quotes}spent fuel standard{close_quotes}, since the disposition material form derives from these goals. The group felt strongly that not only the disposition goals but safeguards to meet these goals could affect the material form. Accordingly, the Department was encouraged to explore and apply safeguards as early in the implementation process as possible. It was emphasized that this was particularly true for any planned use of existing facilities. It is much easier to build safeguards approaches into the development of new facilities, than to backfit existing facilities. Accordingly, special safeguards challenges are likely to be encountered, given the cost and schedule advantages offered by use of existing facilities.

  17. DuraLith Alkali-Aluminosilicate Geopolymer Waste Form Testing for Hanford Secondary Waste

    Energy Technology Data Exchange (ETDEWEB)

    Gong, W. L.; Lutz, Werner; Pegg, Ian L.

    2011-07-21

    The primary objective of the work reported here was to develop additional information regarding the DuraLith alkali aluminosilicate geopolymer as a waste form for liquid secondary waste to support selection of a final waste form for the Hanford Tank Waste Treatment and Immobilization Plant secondary liquid wastes to be disposed in the Integrated Disposal Facility on the Hanford Site. Testing focused on optimizing waste loading, improving waste form performance, and evaluating the robustness of the waste form with respect to waste variability.

  18. In-Drift Accumulation of Fissile Material From Waste Packages Containing Plutonium Disposition Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    H.W> Stockman; S. LeStrange

    2000-09-28

    The objective of this calculation is to provide estimates of the amount of fissile material flowing out of the waste package (source term) and the accumulation of fissile elements (U and Pu) in a crushed-tuff invert. These calculations provide input for the analysis of repository impacts of the Pu-ceramic waste forms. In particular, the source term results are used as input to the far-field accumulation calculation reported in Ref. 51, and the in-drift accumulation results are used as inputs for the criticality calculations reported in Ref. 2. The results are also summarized and interpreted in Ref. 52. The scope of this calculation is the waste package (WP) Viability Assessment (VA) design, which consists of an outer corrosion-allowance material (CAM) and an inner corrosion-resistant material (CRM). This design is used in this calculation in order to be consistent with earlier Pu-ceramic degradation calculations (Ref. 15). The impact of the new Enhanced Design Alternative-I1 (EDA-11) design on the results will be addressed in a subsequent report. The design of the invert (a leveling foundation, which creates a level surface of the drift floor and supports the WP mounting structure) is consistent with the EDA-I1 design. The invert will be composed of crushed stone and a steel support structure (Ref. 17). The scope of this calculation is also defined by the nominal degradation scenario, which involves the breach of the WP (Section 10.5.1.2, Ref. 48), followed by the influx of water. Water in the WP may, in time, gradually leach the fissile components and neutron absorbers out of the ceramic waste forms. Thus, the water in the WP may become laden with dissolved actinides (e.g., Pu and U), and may eventually overflow or leak from the WP. Once the water leaves the WP, it may encounter the invert, in which the actinides may reprecipitate. Several factors could induce reprecipitation; these factors include: the high surface area of the crushed stone, and the presence of

  19. Evaluation and selection of candidate high-level waste forms

    International Nuclear Information System (INIS)

    Seven candidate waste forms being developed under the direction of the Department of Energy's National High-Level Waste (HLW) Technology Program, were evaluated as potential media for the immobilization and geologic disposal of high-level nuclear wastes. The evaluation combined preliminary waste form evaluations conducted at DOE defense waste-sites and independent laboratories, peer review assessments, a product performance evaluation, and a processability analysis. Based on the combined results of these four inputs, two of the seven forms, borosilicate glass and a titanate based ceramic, SYNROC, were selected as the reference and alternative forms for continued development and evaluation in the National HLW Program. Both the glass and ceramic forms are viable candidates for use at each of the DOE defense waste-sites; they are also potential candidates for immobilization of commercial reprocessing wastes. This report describes the waste form screening process, and discusses each of the four major inputs considered in the selection of the two forms

  20. NDA issues with RFETS vitrified waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Hurd, J.; Veazey, G.

    1998-12-31

    A study was conducted at Los Alamos National Laboratory (LANL) for the purpose of determining the feasibility of using a segmented gamma scanner (SGS) to accurately perform non-destructive analysis (NDA) on certain Rocky Flats Environmental Technology Site (RFETS) vitrified waste samples. This study was performed on a full-scale vitrified ash sample prepared at LANL according to a procedure similar to that anticipated to be used at RFETS. This sample was composed of a borosilicate-based glass frit, blended with ash to produce a Pu content of {approximately}1 wt %. The glass frit was taken to a degree of melting necessary to achieve a full encapsulation of the ash material. The NDA study performed on this sample showed that SGSs with either {1/2}- or 2-inch collimation can achieve an accuracy better than 6 % relative to calorimetry and {gamma}-ray isotopics. This accuracy is achievable, after application of appropriate bias corrections, for transmissions of about {1/2} % through the waste form and counting times of less than 30 minutes. These results are valid for ash material and graphite fines with the same degree of plutonium particle size, homogeneity, sample density, and sample geometry as the waste form used to obtain the results in this study. A drum-sized thermal neutron counter (TNC) was also included in the study to provide an alternative in the event the SGS failed to meet the required level of accuracy. The preliminary indications are that this method will also achieve the required accuracy with counting times of {approximately}30 minutes and appropriate application of bias corrections. The bias corrections can be avoided in all cases if the instruments are calibrated on standards matching the items.

  1. Review of high-level waste form properties. [146 bibliographies

    Energy Technology Data Exchange (ETDEWEB)

    Rusin, J.M.

    1980-12-01

    This report is a review of waste form options for the immobilization of high-level-liquid wastes from the nuclear fuel cycle. This review covers the status of international research and development on waste forms as of May 1979. Although the emphasis in this report is on waste form properties, process parameters are discussed where they may affect final waste form properties. A summary table is provided listing properties of various nuclear waste form options. It is concluded that proposed waste forms have properties falling within a relatively narrow range. In regard to crystalline versus glass waste forms, the conclusion is that either glass of crystalline materials can be shown to have some advantage when a single property is considered; however, at this date no single waste form offers optimum properties over the entire range of characteristics investigated. A long-term effort has been applied to the development of glass and calcine waste forms. Several additional waste forms have enough promise to warrant continued research and development to bring their state of development up to that of glass and calcine. Synthetic minerals, the multibarrier approach with coated particles in a metal matrix, and high pressure-high temperature ceramics offer potential advantages and need further study. Although this report discusses waste form properties, the total waste management system should be considered in the final selection of a waste form option. Canister design, canister materials, overpacks, engineered barriers, and repository characteristics, as well as the waste form, affect the overall performance of a waste management system. These parameters were not considered in this comparison.

  2. Review of high-level waste form properties

    International Nuclear Information System (INIS)

    This report is a review of waste form options for the immobilization of high-level-liquid wastes from the nuclear fuel cycle. This review covers the status of international research and development on waste forms as of May 1979. Although the emphasis in this report is on waste form properties, process parameters are discussed where they may affect final waste form properties. A summary table is provided listing properties of various nuclear waste form options. It is concluded that proposed waste forms have properties falling within a relatively narrow range. In regard to crystalline versus glass waste forms, the conclusion is that either glass of crystalline materials can be shown to have some advantage when a single property is considered; however, at this date no single waste form offers optimum properties over the entire range of characteristics investigated. A long-term effort has been applied to the development of glass and calcine waste forms. Several additional waste forms have enough promise to warrant continued research and development to bring their state of development up to that of glass and calcine. Synthetic minerals, the multibarrier approach with coated particles in a metal matrix, and high pressure-high temperature ceramics offer potential advantages and need further study. Although this report discusses waste form properties, the total waste management system should be considered in the final selection of a waste form option. Canister design, canister materials, overpacks, engineered barriers, and repository characteristics, as well as the waste form, affect the overall performance of a waste management system. These parameters were not considered in this comparison

  3. Formulation and Analysis of Compliant Grouted Waste Forms for SHINE Waste Streams

    Energy Technology Data Exchange (ETDEWEB)

    Ebert, William [Argonne National Lab. (ANL), Argonne, IL (United States); Pereira, Candido [Argonne National Lab. (ANL), Argonne, IL (United States); Heltemes, Thad A. [Argonne National Lab. (ANL), Argonne, IL (United States); Youker, Amanda [Argonne National Lab. (ANL), Argonne, IL (United States); Makarashvili, Vakhtang [Argonne National Lab. (ANL), Argonne, IL (United States); Vandegrift, George F. [Argonne National Lab. (ANL), Argonne, IL (United States)

    2014-01-01

    Optional grouted waste forms were formulated for waste streams generated during the production of 99Mo to be compliant with low-level radioactive waste regulations. The amounts and dose rates of the various waste form materials that would be generated annually were estimated and used to determine the effects of various waste processing options, such as the of number irradiation cycles between uranium recovery operations, different combinations of waste streams, and removal of Pu, Cs, and Sr from waste streams for separate disposition (which is not evaluated in this report). These calculations indicate that Class C-compliant grouted waste forms can be produced for all waste streams. More frequent uranium recovery results in the generation of more chemical waste, but this is balanced by the fact that waste forms for those waste streams can accommodate higher waste loadings, such that similar amounts of grouted waste forms are required regardless of the recovery schedule. Similar amounts of grouted waste form are likewise needed for the individual and combined waste streams. Removing Pu, Cs, and Sr from waste streams lowers the waste form dose significantly at times beyond about 1 year after irradiation, which may benefit handling and transport. Although these calculations should be revised after experimentally optimizing the grout formulations and waste loadings, they provide initial guidance for process development.

  4. CSNF WASTE FORM DEGRADATION: SUMMARY ABSTRACTION

    Energy Technology Data Exchange (ETDEWEB)

    J.C. CUNNANE

    2004-08-31

    The purpose of this model report is to describe the development and validation of models that can be used to calculate the release of radionuclides from commercial spent nuclear fuel (CSNF) following a hypothetical breach of the waste package and fuel cladding in the repository. The purpose also includes describing the uncertainties associated with modeling the radionuclide release for the range of CSNF types, exposure conditions, and durations for which the radionuclide release models are to be applied. This document was developed in accordance with Technical Work Plan for: Regulatory Integration Modeling and Analysis of the Waste Form and Waste Package (BSC 2004 [DIRS 169944]). This document considers radionuclides to be released from CSNF when they are available for mobilization by gas-phase mass transport, or by dissolution or colloid formation in water that may contact the fuel. Because other reports address limitations on the dissolved and colloidal radionuclide concentrations (BSC 2004 [DIRS 169944], Table 2-1), this report does not address processes that control the extent to which the radionuclides released from CSNF are mobilized and transported away from the fuel either in the gas phase or in the aqueous phase as dissolved and colloidal species. The scope is limited to consideration of degradation of the CSNF rods following an initial breach of the cladding. It considers features of CSNF that limit the availability of individual radionuclides for release into the gaseous or aqueous phases that may contact the fuel and the processes and events expected to degrade these CSNF features. In short, the purpose is to describe the characteristics of breached fuel rods and the degradation processes expected to influence radionuclide release.

  5. Plutonium-238 alpha-decay damage study of the ceramic waste form.

    Energy Technology Data Exchange (ETDEWEB)

    Frank, S M [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; Barber, T L [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; Cummings, D G [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; DiSanto, T [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; Esh, D W [U.S. Nuclear Regulatory Commission, Washington, DC 20555-0001; Giglio, J J [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; Goff, K M [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; Johnson, S G [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; Kennedy, J R [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; Jue, J-F [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; Noy, M [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; O' Holleran, T P [U.S. Department of Energy, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID 83415; Sinkler, W [UOP LLC, 25 E Algonquin Road, Des Plaines, IL 60017

    2006-03-27

    volume has expanded slightly by 0.3% again, presumably due to alpha-decay damage. (5) No bulk sample swelling was observed. (6) No amorphization of sodalite or actinide bearing phases was observed after four years of alpha-decay damage. (7) No microcracks or phase de-bonding were observed in waste form samples aged for four years. (8) In some areas of the {sup 238}Pu doped ceramic waste form material bubbles and voids were found. Bubbles and voids with similar size and density were also found in ceramic waste form samples without actinide. These bubbles and voids are interpreted as pre-existing defects. However, some contribution to these bubbles and voids from helium gas can not be ruled out. (9) Chemical durability of {sup 238}Pu CWF has not changed significantly after four years of alpha-decay exposure except for an increase in the release of salt components and Pu. Still, the plutonium release from CWF is very low at less than 0.005 g/m{sup 2}.

  6. Laboratory procedures for waste form testing

    Energy Technology Data Exchange (ETDEWEB)

    Mast, E.S.

    1994-09-19

    The 100 and 300 areas of the Hanford Site are included on the US Environmental Protection Agencies (EPA) National Priorities List under the Comprehensive Environmental Response, Compensation, and Liability Act (CERCLA). Soil washing is a treatment process that is being considered for the remediation of the soil in these areas. Contaminated soil washing fines can be mixed or blended with cementations materials to produce stable waste forms that can be used for beneficial purposes in mixed or low-level waste landfills, burial trenches, environmental restoration sites, and other applications. This process has been termed co-disposal. The Co-Disposal Treatability Study Test Plan is designed to identify a range of cement-based formulations that could be used in disposal efforts in Hanford in co-disposal applications. The purpose of this document is to provide explicit procedural information for the testing of co-disposal formulations. This plan also provides a discussion of laboratory safety and quality assurance necessary to ensure safe, reproducible testing in the laboratory.

  7. Transportation considerations related to waste forms and canisters for Defense TRU wastes

    Energy Technology Data Exchange (ETDEWEB)

    Schneider, K.J.; Andrews, W.B.; Schreiber, A.M.; Rosenthal, L.J.; Odle, C.J.

    1981-09-01

    This report identifies and discusses the considerations imposed by transportation on waste forms and canisters for contact-handled, solid transuranic wastes from the US Department of Energy (DOE) activities. The report reviews (1) the existing raw waste forms and potential immobilized waste forms, (2) the existing and potential future DOE waste canisters and shipping containers, (3) regulations and regulatory trends for transporting commercial transuranic wastes on the ISA, (4) truck and rail carrier requirements and preferences for transporting the wastes, and (5) current and proposed Type B external packagings for transporting wastes.

  8. Transportation considerations related to waste forms and canisters for Defense TRU wastes

    International Nuclear Information System (INIS)

    This report identifies and discusses the considerations imposed by transportation on waste forms and canisters for contact-handled, solid transuranic wastes from the US Department of Energy (DOE) activities. The report reviews (1) the existing raw waste forms and potential immobilized waste forms, (2) the existing and potential future DOE waste canisters and shipping containers, (3) regulations and regulatory trends for transporting commercial transuranic wastes on the ISA, (4) truck and rail carrier requirements and preferences for transporting the wastes, and (5) current and proposed Type B external packagings for transporting wastes

  9. 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

  10. 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.

  11. Waste forms, packages, and seals working group summary

    Energy Technology Data Exchange (ETDEWEB)

    Sridhar, N. [Center Antonio, TX (United States); McNeil, M.B. [Nuclear Regulatory Commission, Washington, DC (United States)

    1995-09-01

    This article is a summary of the proceedings of a group discussion which took place at the Workshop on the Role of Natural Analogs in Geologic Disposal of High-Level Nuclear Waste in San Antonio, Texas on July 22-25, 1991. The working group concentrated on the subject of radioactive waste forms and packaging. Also included is a description of the use of natural analogs in waste packaging, container materials and waste forms.

  12. Characterization of low and medium level radioactive waste forms

    International Nuclear Information System (INIS)

    The work reported was carried out during the first year of the Commission of the European Community's programme on the characterization of low and medium level waste forms. Ten reference waste forms plus others of special national interest have been identified covering PWR, BWR, GCR and reprocessing wastes. The immobilising media include the three main matrices: cement, polymers and bitumen, and a glass. Characterization is viewed as one input to quality assurance of the waste form and covers: waste-matrix compatibility, radiation effects, leaching, microbiological attack, shrinkage and swelling, ageing processes and thermal effects. The aim is a balanced programme of comparative data, predictive modelling and an undserstanding of basic mechanisms

  13. Phosphate bonded ceramics as candidate final-waste-form materials

    International Nuclear Information System (INIS)

    Room-temperature setting phosphate-bonded ceramics were studied as candidate materials for stabilization of DOE low-level problem mixed wastes which cannot be treated by other established stabilization techniques. Phosphates of Mg, Mg-Na, Al and Zr were studied to stabilize ash surrogate waste containing RCRA metals as nitrates and RCRA organics. We show that for a typical loading of 35 wt.% of the ash waste, the phosphate ceramics pass the TCLP test. The waste forms have high compression strength exceeding ASTM recommendations for final waste forms. Detailed X-ray diffraction studies and differential thermal analyses of the waste forms show evidence of chemical reaction of the waste with phosphoric acid and the host matrix. The SEM studies show evidence of physical bonding. The excellent performance in the leaching tests is attributed to a chemical solidification and physical as well as chemical bonding of ash wastes in these phosphate ceramics

  14. Physical modeling of contaminant diffusion from a cementious waste form

    International Nuclear Information System (INIS)

    Cementitious materials can be used to immobilize waste materials for disposal. The Westinghouse Hanford Company is pursuing approval of disposal technologies by which hazardous and radioactive wastes are blended or packaged with cementitious materials for disposal. Of significant concern is the mobility of the waste contaminants both from the waste form and in the arid soils of the Hanford Site. A physical model has been developed to study the diffusion of waste contaminants from simulated cementitious waste forms in unsaturated Hanford Site soils. The model can be used to predict cementitious waste form performance in a representative environment, support design of waste management facilities and technologies, and provide data for environmental permitting of proposed treatment and disposal facilities

  15. 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

  16. Alternate nuclear waste forms and interactions in geologic media

    International Nuclear Information System (INIS)

    The primary purposes of the conference on Alternate Nuclear Waste Forms and Interactions in Geologic Media were: First, to provide an opportunity for a review of the status of the research on some of the candidate alternative waste forms; second, to provide an opportunity for comparing the characteristics of alternate waste forms to those of glasses; and third, to stimulate increased interactions between those research groups that were engaged in a more basic approach to characterizing waste forms and those who were concerned with more applied aspects such as the processing of these materials. The motivating philosophy behind this third purpose of the conference was based on the idea that by operating from the soundest possible fundamental base for any of the candidate waste forms, hopefully any future unpleasant surprise - such as that alluded to earlier in the case of glass waste forms - could be avoided. Separate abstracts have been prepared for individual papers for inclusion in the Energy Data Base

  17. DURABILITY TESTING OF FLUIDIZED BED STEAM REFORMER (FBSR) WASTE FORMS

    Energy Technology Data Exchange (ETDEWEB)

    Jantzen, C

    2006-01-06

    Fluidized Bed Steam Reforming (FBSR) is being considered as a potential technology for the immobilization of a wide variety of high sodium aqueous radioactive wastes. The addition of clay and a catalyst as co-reactants converts high sodium aqueous low activity wastes (LAW) such as those existing at the Hanford and Idaho DOE sites to a granular ''mineralized'' waste form that may be made into a monolith form if necessary. Simulant Hanford and Idaho high sodium wastes were processed in a pilot scale FBSR at Science Applications International Corporation (SAIC) Science and Technology Applications Research (STAR) facility in Idaho Falls, ID. Granular mineral waste forms were made from (1) a basic Hanford Envelope A low-activity waste (LAW) simulant and (2) an acidic INL simulant commonly referred to as sodium-bearing waste (SBW). The FBSR waste forms were characterized and the durability tested via ASTM C1285 (Product Consistency Test), the Environmental Protection Agency (EPA) Toxic Characteristic Leaching Procedure (TCLP), and the Single Pass Flow Through (SPFT) test. The durability of the FBSR waste form products was tested in order to compare the measured durability to previous FBSR waste form testing on Hanford Envelope C waste forms that were made by THOR Treatment Technologies (TTT) and to compare the FBSR durability to vitreous LAW waste forms, specifically the Hanford low activity waste (LAW) glass known as the Low-activity Reference Material (LRM). The durability of the FBSR waste form is comparable to that of the LRM glass for the test responses studied.

  18. Cerium as a surrogate in the plutonium immobilization waste form

    Science.gov (United States)

    Marra, James Christopher

    In the aftermath of the Cold War, approximately 50 tonnes (MT) of weapons useable plutonium (Pu) has been identified as excess. The U.S. Department of Energy (DOE) has decided that at least a portion of this material will be immobilized in a titanate-based ceramic for final disposal in a geologic repository. The baseline formulation was designed to produce a ceramic consisting primarily of a highly substituted pyrochlore with minor amounts of brannerite and hafnia-substituted rutile. Since development studies with actual actinide materials is difficult, surrogates have been used to facilitate testing. Cerium has routinely been used as an actinide surrogate in actinide chemistry and processing studies. Although cerium appeared as an adequate physical surrogate for powder handling and general processing studies, cerium was found to act significantly different from a chemical perspective in the Pu ceramic form. The reduction of cerium at elevated temperatures caused different reaction paths toward densification of the respective forms resulting in different phase assemblages and microstructural features. Single-phase fabrication studies and cerium oxidation state analyses were performed to further quantify these behavioral differences. These studies indicated that the major phases in the final phase assemblages contained point defects likely leading to their stability. Additionally, thermochemical arguments predicted that the predominant pyrochlore phase in the ceramic was metastable. The apparent metastabilty associated with primary phase in the Pu ceramic form indicated that additional studies must be performed to evaluate the thermodynamic properties of these compounds. Moreover, the metastability of this predominant phase must be considered in assessment of long-term behavior (e.g. radiation stability) of this ceramic.

  19. The investigation of the neptunium complexes formed upon interaction of high level waste glass and boom clay media

    International Nuclear Information System (INIS)

    Since complexes formed between actinides released from high level waste glass and humic acids present in high concentration in boom clay porewater may control the actinide solubility in the clay formation, a research programme has been started to study the complexes formed between neptunium, the most critical actinide in the Belgian performance assessment studies, and boom clay porewater. The leaching experiments give a maximum solution concentration of Np in boom clay porewater of 10-6 M after 24 days. In the leachates, Np is mainly associated with colloidal particles of small sizes and is present as a mixture of two oxidation states, V and IV. The retention of Np in the glass increases with increasing SA/V (geometrical surface area on solution volume ratio). A high solution concentration is accompanied by a high retention of Np. The characterisation of the mobile boom clay organic matter (OM) gives a proton exchange capacity (PEC) equal to 2.9 meq g-1 OM at pH 8.5. Related to this value, the interaction constants (β) of the literature were reviewed and calculated according to their proton exchange capacity for the pH of interest. (orig.)

  20. Waste Classification based on Waste Form Heat Generation in Advanced Nuclear Fuel Cycles Using the Fuel-Cycle Integration and Tradeoffs (FIT) Model

    Energy Technology Data Exchange (ETDEWEB)

    Denia Djokic; Steven J. Piet; Layne F. Pincock; Nick R. Soelberg

    2013-02-01

    This study explores the impact of wastes generated from potential future fuel cycles and the issues presented by classifying these under current classification criteria, and discusses the possibility of a comprehensive and consistent characteristics-based classification framework based on new waste streams created from advanced fuel cycles. A static mass flow model, Fuel-Cycle Integration and Tradeoffs (FIT), was used to calculate the composition of waste streams resulting from different nuclear fuel cycle choices. This analysis focuses on the impact of waste form heat load on waste classification practices, although classifying by metrics of radiotoxicity, mass, and volume is also possible. The value of separation of heat-generating fission products and actinides in different fuel cycles is discussed. It was shown that the benefits of reducing the short-term fission-product heat load of waste destined for geologic disposal are neglected under the current source-based radioactive waste classification system , and that it is useful to classify waste streams based on how favorable the impact of interim storage is in increasing repository capacity.

  1. Immobilization of Technetium in a Metallic Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    S.M. Frank; D. D. Keiser, Jr.; K. C. Marsden

    2007-09-01

    Fission-product technetium accumulated during treatment of spent nuclear fuel will ultimately be disposed of in a geological repository. The exact form of Tc for disposal has yet to be determined; however, a reasonable solution is to incorporate elemental Tc into a metallic waste form similar to the waste form produced during the pyrochemical treatment of spent, sodium-bonded fuel. This metal waste form, produced at the Idaho National Laboratory, has undergone extensive qualification examination and testing for acceptance to the Yucca Mountain geological repository. It is from this extensive qualification effort that the behavior of Tc and other fission products in the waste form has been elucidated, and that the metal waste form is extremely robust in the retention of fission products, such as Tc, in repository like conditions. This manuscript will describe the metal waste form, the behavior of Tc in the waste form; and current research aimed at determining the maximum possible loading of Tc into the metal waste and subsequent determination of the performance of high Tc loaded metal waste forms.

  2. Far-Field Accumulation of Fissile Material From Waste Packages Containing Plutonium Disposition Waste Form

    International Nuclear Information System (INIS)

    The objective of this calculation is to estimate the quantity of fissile material that could accumulate in fractures in the rock beneath plutonium-ceramic (Pu-ceramic) and Mixed-Oxide (MOX) waste packages (WPs) as they degrade in the potential monitored geologic repository at Yucca Mountain. This calculation is to feed another calculation (Ref. 31) computing the probability of criticality in the systems described in Section 6 and then ultimately to a more general report on the impact of plutonium on the performance of the proposed repository (Ref. 32), both developed concurrently to this work. This calculation is done in accordance with the development plan TDP-DDC-MD-000001 (Ref. 9), item 5. The original document described in item 5 has been split into two documents: this calculation and Ref. 4. The scope of the calculation is limited to only very low flow rates because they lead to the most conservative cases for Pu accumulation and more generally are consistent with the way the effluent from the WP (called source term in this calculation) was calculated (Ref. 4). Ref. 4 (''In-Drift Accumulation of Fissile Material from WPs Containing Plutonium Disposition Waste Forms'') details the evolution through time (breach time is initial time) of the chemical composition of the solution inside the WP as degradation of the fuel and other materials proceed. It is the chemical solution used as a source term in this calculation. Ref. 4 takes that same source term and reacts it with the invert; this calculation reacts it with the rock. In addition to reactions with the rock minerals (that release Si and Ca), the basic mechanisms for actinide precipitation are dilution and mixing with resident water as explained in Section 2.1.4. No other potential mechanism such as flow through a reducing zone is investigated in this calculation. No attempt was made to use the effluent water from the bottom of the invert instead of using directly the effluent water from the WP. This

  3. Far-Field Accumulation of Fissile Material From Waste Packages Containing Plutonium Disposition Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    J.P. Nicot

    2000-09-29

    The objective of this calculation is to estimate the quantity of fissile material that could accumulate in fractures in the rock beneath plutonium-ceramic (Pu-ceramic) and Mixed-Oxide (MOX) waste packages (WPs) as they degrade in the potential monitored geologic repository at Yucca Mountain. This calculation is to feed another calculation (Ref. 31) computing the probability of criticality in the systems described in Section 6 and then ultimately to a more general report on the impact of plutonium on the performance of the proposed repository (Ref. 32), both developed concurrently to this work. This calculation is done in accordance with the development plan TDP-DDC-MD-000001 (Ref. 9), item 5. The original document described in item 5 has been split into two documents: this calculation and Ref. 4. The scope of the calculation is limited to only very low flow rates because they lead to the most conservative cases for Pu accumulation and more generally are consistent with the way the effluent from the WP (called source term in this calculation) was calculated (Ref. 4). Ref. 4 (''In-Drift Accumulation of Fissile Material from WPs Containing Plutonium Disposition Waste Forms'') details the evolution through time (breach time is initial time) of the chemical composition of the solution inside the WP as degradation of the fuel and other materials proceed. It is the chemical solution used as a source term in this calculation. Ref. 4 takes that same source term and reacts it with the invert; this calculation reacts it with the rock. In addition to reactions with the rock minerals (that release Si and Ca), the basic mechanisms for actinide precipitation are dilution and mixing with resident water as explained in Section 2.1.4. No other potential mechanism such as flow through a reducing zone is investigated in this calculation. No attempt was made to use the effluent water from the bottom of the invert instead of using directly the effluent water from the

  4. TRU waste form and package criteria meeting

    Energy Technology Data Exchange (ETDEWEB)

    None

    1977-08-01

    The broad subject of the meeting is the overall ERDA TRU waste management program, although the discussions also cover performance criteria for the Waste Isolation Pilot Plant and their implications for the overall TRU program. Separate abstracts were prepared for all ten presentations. (DLC)

  5. Ceramic waste form qualification using results from witness tubes

    International Nuclear Information System (INIS)

    A ceramic waste form has been developed to immobilize the salt waste stream from electrometallurgical treatment of spent nuclear fuel. The ceramic waste form is prepared in a hot isostatic press (HIP). The use of small, easily fabricated HIP capsules called witness tubes has been proposed as a practical way to obtain representative samples of ceramic waste form material for process monitoring, waste form qualification, and archiving. Witness tubes are filled with the same material used to fill the corresponding HIP can, and are HIPed along with the HIP can. Relevant physical, chemical, and performance (leach test) data are analyzed and compared. Differences between witness tube and HIP can materials are shown to be statistically insignificant, demonstrating that witness tubes do provide ceramic waste form material representative of the material in the corresponding HIP can.

  6. Actinide Sorption in a Brine/Dolomite Rock System: Evaluating the Degree of Conservatism in Kd Ranges used in Performance Assessment Modeling for the WIPP Nuclear Waste Repository

    Science.gov (United States)

    Dittrich, T. M.; Reed, D. T.

    2015-12-01

    The Waste Isolation Pilot Plant (WIPP) near Carlsbad, NM is the only operating nuclear waste repository in the US and has been accepting transuranic (TRU) waste since 1999. The WIPP is located in a salt deposit approximately 650 m below the surface and performance assessment (PA) modeling for a 10,000 year period is required to recertify the operating license with the US EPA every five years. The main pathway of concern for environmental release of radioactivity is a human intrusion caused by drilling into a pressurized brine reservoir below the repository. This could result in the flooding of the repository and subsequent transport in the high transmissivity layer (dolomite-rich Culebra formation) above the waste disposal rooms. We evaluate the degree of conservatism in the estimated sorption partition coefficients (Kds) ranges used in the PA based on an approach developed with granite rock and actinides (Dittrich and Reimus, 2015; Dittrich et al., 2015). Sorption onto the waste storage material (Fe drums) may also play a role in mobile actinide concentrations. We will present (1) a conceptual overview of how Kds are used in the PA model, (2) technical background of the evolution of the ranges and (3) results from batch and column experiments and model predictions for Kds with WIPP dolomite and clays, brine with various actinides, and ligands (e.g., acetate, citrate, EDTA) that could promote transport. The current Kd ranges used in performance models are based on oxidation state and are 5-400, 0.5-10,000, 0.03-200, and 0.03-20 mL g-1 for elements with oxidation states of III, IV, V, and VI, respectively. Based on redox conditions predicted in the brines, possible actinide species include Pu(III), Pu(IV), U(IV), U(VI), Np(IV), Np(V), Am(III), and Th(IV). We will also discuss the challenges of upscaling from lab experiments to field scale predictions, the role of colloids, and the effect of engineered barrier materials (e.g., MgO) on transport conditions. Dittrich

  7. 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

  8. Secondary waste form testing : ceramicrete phosphate bonded ceramics.

    Energy Technology Data Exchange (ETDEWEB)

    Singh, D.; Ganga, R.; Gaviria, J.; Yusufoglu, Y. (Nuclear Engineering Division); ( ES)

    2011-06-21

    The cleanup activities of the Hanford tank wastes require stabilization and solidification of the secondary waste streams generated from the processing of the tank wastes. The treatment of these tank wastes to produce glass waste forms will generate secondary wastes, including routine solid wastes and liquid process effluents. Liquid wastes may include process condensates and scrubber/off-gas treatment liquids from the thermal waste treatment. The current baseline for solidification of the secondary wastes is a cement-based waste form. However, alternative secondary waste forms are being considered. In this regard, Ceramicrete technology, developed at Argonne National Laboratory, is being explored as an option to solidify and stabilize the secondary wastes. The Ceramicrete process has been demonstrated on four secondary waste formulations: baseline, cluster 1, cluster 2, and mixed waste streams. Based on the recipes provided by Pacific Northwest National Laboratory, the four waste simulants were prepared in-house. Waste forms were fabricated with three filler materials: Class C fly ash, CaSiO{sub 3}, and Class C fly ash + slag. Optimum waste loadings were as high as 20 wt.% for the fly ash and CaSiO{sub 3}, and 15 wt.% for fly ash + slag filler. Waste forms for physical characterizations were fabricated with no additives, hazardous contaminants, and radionuclide surrogates. Physical property characterizations (density, compressive strength, and 90-day water immersion test) showed that the waste forms were stable and durable. Compressive strengths were >2,500 psi, and the strengths remained high after the 90-day water immersion test. Fly ash and CaSiO{sub 3} filler waste forms appeared to be superior to the waste forms with fly ash + slag as a filler. Waste form weight loss was {approx}5-14 wt.% over the 90-day immersion test. The majority of the weight loss occurred during the initial phase of the immersion test, indicative of washing off of residual unreacted

  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. The 'granite encapsulation' route to the safe disposal of Pu and other actinide

    OpenAIRE

    Gibb, F.G.F.; Taylor, K. J.; Burakov, B.E.

    2008-01-01

    Waste actinides, including plutonium, present a long-term management problem and a serious security issue. Immobilisation in mineral or ceramic waste forms for interim storage is a widely proposed first step. The safest, most secure geological disposal for Pu is in very deep boreholes and we propose that the key step to combination of these immobilisation and disposal concepts is encapsulation of the waste form in cylinders of recrystallized granite. We discuss the underpinning science, focus...

  11. Quality control of cemented waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Slate, L.J.

    1994-12-31

    To insure that cemented radwaste remains immobilized after disposal, certain standards have been set in Europe by the Commission of the European Communities. One such standard is compressive strength. If the compressive strength can be predicted during the early curing stages, time and money can be saved and the quality of the final waste form guaranteed. It was determined that the 7- and 28-day compressive strength from radwaste cementation can be predicted during the mixing and early curing stages by at least three methods. The three that were studied were maturity, rheology, and impedance. Maturity is a temperature-to-time measurement, rheology is a shear stress-to-shear rate measurement, and impedance is the opposition offered to the flow of alternating current. These three methods were employed on five different cemented radwaste concentrations with three different water-to-cement ratios; thus, a total of 15 different mix designs were considered. The results showed that the impedance was the easiest to employ for an on-line process. The results of the impedance method showed a very good relationship between impedance and water-to-cement ratio; therefore, an accurate prediction of compressive strength of cemented radwaste can be drawn from this method. The results of the theology method were very good. The method showed that concrete conforms to the Bingham plastic rheologic model, and the theology method can be used to predict the compressive strength of cemented radwaste, but may be too cumbersome. The results of the maturity method were shown to be limited in accuracy for determining compressive strength.

  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. Final report on cermet high-level waste forms

    International Nuclear Information System (INIS)

    Cermets are being developed as an alternate method for the fixation of defense and commercial high level radioactive waste in a terminal disposal form. Following initial feasibility assessments of this waste form, consisting of ceramic particles dispersed in an iron-nickel base alloy, significantly improved processing methods were developed. The characterization of cermets has continued through property determinations on samples prepared by various methods from a variety of simulated and actual high-level wastes. This report describes the status of development of the cermet waste form as it has evolved since 1977. 6 tables, 18 figures

  14. Leaching from solidified waste forms under saturated and unsaturated conditions

    International Nuclear Information System (INIS)

    The leaching behavior of nitrate ion from a cement based waste form containing low-level radioactive waste was shown to be identical under saturated and unsaturated soil conditions. Only in soils containing less than 2 wt %water did the leach rate decrease. The observation of identical leach rates under saturated and unsaturated conditions is explained by diffusion through the waste form being the limiting step. Diffusion through the soil decreases in very dry soil and the limiting step changes. These laboratory tests were verified by measurements on similar, Portland cement based waste form in a field lysimeter

  15. A study of uranium and thorium migration at the Koongarra uranium deposit with application to actinide transport from nuclear waste repositories

    International Nuclear Information System (INIS)

    One way to gain confidence in modelling possible radionuclide releases is to study natural systems which are similar to components of the multibarrier waste repository. Several such analogues are currently under study and these provide useful data about radionuclide behaviour in the natural environment. One such system is the Koongarra uranium deposit in the Northern Territory. In this dissertation, the migration of actinides, primarily uranium and thorium, has been studied as an analogue for the behaviour of transuranics in the far-field of a waste repository. The major findings of this study are: 1. the main process retarding uranium migration in the dispersion fan at Koongarra is sorption, which suppresses dissolved uranium concentrations well below solubility limits, with ferrihydrite being a major sorbing phase; 2. thorium is extremely immobile, with very low dissolved concentrations and corresponding high distribution ratios for 230Th. Overall, it is estimated that colloids are relatively unimportant in Koongarra groundwater. Uranium migrates mostly as dissolved species, whereas thorium and actinium are mostly adsorbed to larger, relatively immobile particles and the stationary phase. However, of the small amount of 230Th that passes through a 1μm filter, a significant proportion is associated with colloidal particles. Actinium appears to be slightly more mobile than thorium and is associated with colloids to a greater extent, although generally present in low concentrations. These results support the possibility of colloidal transport of trivalent and tetravalent actinides in the vicinity of a nuclear waste repository. 112 refs., 23 tabs., 32 figs

  16. Applications of inductively coupled plasma-mass spectrometry to the determination of actinides and fission products in high level radioactive wastes at the Savannah River Site

    International Nuclear Information System (INIS)

    Four years of experience in applying inductively coupled plasma-mass spectrometry (ICP-MS) to the analysis of actinides and fission products in high level waste (HLW) samples at the Savannah River Site has led to the development of a number of techniques to aid in the interpretation of the mass spectral data. The goal has been to develop rapid and reliable analytical procedures that provide the necessary chemical and isotopic information to answer the process needs of the customers. Techniques that have been developed include the writing of computer software to strip the experimental data from the instrumental data files into spreadsheets or into a spectral data processing package so that the raw mass spectra can be overlain for comparison or plotted with higher output resolution. These procedures have been applied to problems ranging from the analysis of the high level waste tanks to reactor moderator water as well as environmental samples. Criticality safety analyses in some HLW waste treatment processes depend upon actinide concentration and isotopic information generated by ICP-MS, particularly in tanks with high concentrations of 137Cs and 90Sr. Experimental results for a number of these applications will be presented. These procedures represent a considerable saving in time and expense as compared to conventional chemical separation followed by radiochemical analyses, as well as decreased radiation exposure for the analysts

  17. Secondary Waste Form Down Selection Data Package – Ceramicrete

    Energy Technology Data Exchange (ETDEWEB)

    Cantrell, Kirk J.; Westsik, Joseph H.

    2011-08-31

    As part of high-level waste pretreatment and immobilized low activity waste processing, liquid secondary wastes will be generated that will be transferred to the Effluent Treatment Facility on the Hanford Site for further treatment. These liquid secondary wastes will be converted to stable solid waste forms that will be disposed in the Integrated Disposal Facility. Currently, four waste forms are being considered for stabilization and solidification of the liquid secondary wastes. These waste forms are Cast Stone, Ceramicrete, DuraLith, and Fluidized Bed Steam Reformer. The preferred alternative will be down selected from these four waste forms. Pacific Northwest National Laboratory is developing data packages to support the down selection process. The objective of the data packages is to identify, evaluate, and summarize the existing information on the four waste forms being considered for stabilization and solidification of the liquid secondary wastes. The information included will be based on information available in the open literature and from data obtained from testing currently underway. This data package is for the Ceramicrete waste form. Ceramicrete is a relatively new engineering material developed at Argonne National Laboratory to treat radioactive and hazardous waste streams (e.g., Wagh 2004; Wagh et al. 1999a, 2003; Singh et al. 2000). This cement-like waste form can be used to treat solids, liquids, and sludges by chemical immobilization, microencapsulation, and/or macroencapsulation. The Ceramicrete technology is based on chemical reaction between phosphate anions and metal cations to form a strong, dense, durable, low porosity matrix that immobilizes hazardous and radioactive contaminants as insoluble phosphates and microencapsulates insoluble radioactive components and other constituents that do not form phosphates. Ceramicrete is a type of phosphate-bonded ceramic, which are also known as chemically bonded phosphate ceramics. The Ceramicrete

  18. Minerals as natural analogues for crystalline nuclear waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Giere, R. [Purdue University West Lafayette, Earth and Atmospheric Sciences (United States)

    2000-07-01

    Between the mining of uranium ore (mostly as uraninite) and the final disposal of nuclear waste, there are many processes and steps which together comprise the nuclear fuel cycle. Radioactive waste will be generated as long as nuclear reactors are in operation, but it is also produced by other means, e.g., during certain medical, scientific and industrial procedures. The most dangerous wastes are those resulting from the reprocessing of spent nuclear fuel and from some processes in the production and dismantling of nuclear weapons. A large part of this highly radioactive waste is present as a liquid and thus, its safe isolation from the biosphere requires immobilization of the radionuclides in a durable matrix (waste form). This is a solid which must be resistant to heat, radiation and corrosion over a geologic time scale. Three main categories of waste forms have been developed for the immobilization of radioactive waste, namely glasses, crystalline and multibarrier waste forms. One of the key properties of a nuclear waste form is its chemical durability (or resistance to corrosion), because the waste form represents the primary barrier to radionuclide release. The sciences of mineralogy and petrology have both contributed significantly to the development, characterization and performance assessment of such waste forms. The most important goal of safe nuclear waste disposal is to ensure that practically no radioactive materials reach the biosphere and, ultimately, human beings. Therefore, the design of final repositories is based on an approach that places several obstacles, or barriers, between waste and biosphere, whereby each barrier has a specific role in preventing or delaying migration of radioactive material. This multibarrier concept is different for each type of waste but, for the option of geological disposal, it generally comprises the following five barriers: (1) waste form (contains the actual waste); (2) canister (surrounds waste form; composed of a

  19. Evaluation and selection of candidate high-level waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Bernadzikowski, T. A.; Allender, J. S.; Butler, J. L.; Gordon, D. E.; Gould, Jr., T. H.; Stone, J. A.

    1982-03-01

    Seven candidate waste forms being developed under the direction of the Department of Energy's National High-Level Waste (HLW) Technology Program, were evaluated as potential media for the immobilization and geologic disposal of high-level nuclear wastes. The evaluation combined preliminary waste form evaluations conducted at DOE defense waste-sites and independent laboratories, peer review assessments, a product performance evaluation, and a processability analysis. Based on the combined results of these four inputs, two of the seven forms, borosilicate glass and a titanate based ceramic, SYNROC, were selected as the reference and alternative forms for continued development and evaluation in the National HLW Program. Both the glass and ceramic forms are viable candidates for use at each of the DOE defense waste-sites; they are also potential candidates for immobilization of commercial reprocessing wastes. This report describes the waste form screening process, and discusses each of the four major inputs considered in the selection of the two forms.

  20. Thermal stability testing of low-level waste forms

    International Nuclear Information System (INIS)

    The NRC Technical Position (TP) on Waste Form specifies that waste forms should be resistant to thermal degradation. The thermal cycle testing procedure outlined in the TP on Waste Form was carried out and is believed adequate for demonstrating the thermal stability of solidified waste forms. The inclusion of control samples and the monitoring of sample temperature are recommended additions to the test. An outline for reporting thermal cycling test results is given. To produce a data base on the applicability of the thermal cycling test, the following simulated laboratory-scale waste forms were prepared and tested: boric acid and sodium sulfate evaporator bottoms, mixed bed bead resins, and powdered resins each solidified in asphalt, cement and vinyl ester-styrene. Thermal cycling does not significantly affect the compressive strength of the solidified wastes, except powdered resins solidified in cement which disintegrated during the test and bead resins in cement which showed a loss of compressive strength. After temperature cycling, cement solidified bead resins showed areas of spalling and solidified sodium sulfate forms had surface deterioration. Asphalt solidified wastes, except powdered resins, deformed by slumping on temperature cycling. Free liquid was released from vinyl esterstyrene solidifed waste forms as a result of thermal cycling. Dewatered bead and powdered resins were also tested and no free liquid was released on temperature cycling. 11 refs., 12 figs., 4 tabs

  1. 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

  2. Preparation and leaching of radioactive INEL waste forms

    International Nuclear Information System (INIS)

    Appreciable quantities of radioactive waste are in storage at the Idaho National Engineering Laboratory (INEL). Plans are being made to convert this waste into durable solid forms for final disposal in a geological repository. Part of the inventory consists of low- and intermediate-level fission, activation, and decay products and transuranic (TRU) wastes, either stored retrievably or buried at the INEL Radioactive Waste Management area. One of the TRU wastes is a sludge from the Department of Energy Rocky Flats Plant, currently stored retrievably in 55-gallon drums. Immobilizing the TRU sludge is the primary concern of the work reported here

  3. The analysis and handling concept of minor actinides of NPP’s waste by using Ads technology

    International Nuclear Information System (INIS)

    The contents of minor actinide elements (americium, neptunium and curium) on the spent fuel inventory from PWR operation of NPP have been calculated using Vista program. The calculation used parameters: enrichment 3.968%, power 1000 M We and burn-up is 60 M Wd/kg. The result of calculation showed that the arising of minor actinide elements on the spent fuel is 16.205 kg/year and 43.471 kg/year for PWR-UOX and PWR-MOX respectively. It is also discussed a concept of the use of ADS technology for transmuting the minor actinide elements contained in spent fuels. The result of the discussion showed that an ADS of 400 M Wth will serve 7 PWRs-UOX, and on the PWR system using UOX and MOX fuels an ADS will serve 3 PWRs. (author)

  4. Enhancement of cemented waste forms by supercritical CO{sub 2} carbonation of standard portland cements

    Energy Technology Data Exchange (ETDEWEB)

    Rubin, J.B.; Carey, J.; Taylor, C.M.V.

    1997-08-01

    We are conducting experiments on an innovative transformation concept, using a traditional immobilization technique, that may significantly reduce the volume of hazardous or radioactive waste requiring transport and long-term storage. The standard practice for the stabilization of radioactive salts and residues is to mix them with cements, which may include additives to enhance immobilization. Many of these wastes do not qualify for underground disposition, however, because they do not meet disposal requirements for free liquids, decay heat, head-space gas analysis, and/or leachability. The treatment method alters the bulk properties of a cemented waste form by greatly accelerating the natural cement-aging reactions, producing a chemically stable form having reduced free liquids, as well as reduced porosity, permeability and pH. These structural and chemical changes should allow for greater actinide loading, as well as the reduced mobility of the anions, cations, and radionuclides in aboveground and underground repositories. Simultaneously, the treatment process removes a majority of the hydrogenous material from the cement. The treatment method allows for on-line process monitoring of leachates and can be transported into the field. We will describe the general features of supercritical fluids, as well as the application of these fluids to the treatment of solid and semi-solid waste forms. some of the issues concerning the economic feasibility of industrial scale-up will be addressed, with particular attention to the engineering requirements for the establishment of on-site processing facilities. Finally, the initial results of physical property measurements made on portland cements before and after supercritical fluid processing will be presented.

  5. Enhancement of cemented waste forms by supercritical CO2 carbonation of standard portland cements

    International Nuclear Information System (INIS)

    We are conducting experiments on an innovative transformation concept, using a traditional immobilization technique, that may significantly reduce the volume of hazardous or radioactive waste requiring transport and long-term storage. The standard practice for the stabilization of radioactive salts and residues is to mix them with cements, which may include additives to enhance immobilization. Many of these wastes do not qualify for underground disposition, however, because they do not meet disposal requirements for free liquids, decay heat, head-space gas analysis, and/or leachability. The treatment method alters the bulk properties of a cemented waste form by greatly accelerating the natural cement-aging reactions, producing a chemically stable form having reduced free liquids, as well as reduced porosity, permeability and pH. These structural and chemical changes should allow for greater actinide loading, as well as the reduced mobility of the anions, cations, and radionuclides in aboveground and underground repositories. Simultaneously, the treatment process removes a majority of the hydrogenous material from the cement. The treatment method allows for on-line process monitoring of leachates and can be transported into the field. We will describe the general features of supercritical fluids, as well as the application of these fluids to the treatment of solid and semi-solid waste forms. some of the issues concerning the economic feasibility of industrial scale-up will be addressed, with particular attention to the engineering requirements for the establishment of on-site processing facilities. Finally, the initial results of physical property measurements made on portland cements before and after supercritical fluid processing will be presented

  6. Development of iron phosphate ceramic waste form to immobilize radioactive waste solution

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Jongkwon; Um, Wooyong; Choung, Sungwook

    2014-05-09

    The objective of this research was to develop an iron phosphate ceramic (IPC) waste form using converter slag obtained as a by-product of the steel industry as a source of iron instead of conventional iron oxide. Both synthetic off-gas scrubber solution containing technetium-99 (or Re as a surrogate) and LiCl-KCl eutectic salt, a final waste solution from pyrochemical processing of spent nuclear fuel, were used as radioactive waste streams. The IPC waste form was characterized for compressive strength, reduction capacity, chemical durability, and contaminant leachability. Compressive strengths of the IPC waste form prepared with different types of waste solutions were 16 MPa and 19 MPa for LiCl-KCl eutectic salt and the off-gas scrubber simulant, respectively, which meet the minimum compressive strength of 3.45 MPa (500 psi) for waste forms to be accepted into the radioactive waste repository. The reduction capacity of converter slag, a main dry ingredient used to prepare the IPC waste form, was 4,136 meq/kg by the Ce(IV) method, which is much higher than those of the conventional Fe oxides used for the IPC waste form and the blast furnace slag materials. Average leachability indexes of Tc, Li, and K for the IPC waste form were higher than 6.0, and the IPC waste form demonstrated stable durability even after 63-day leaching. In addition, the Toxicity Characteristic Leach Procedure measurements of converter slag and the IPC waste form with LiCl-KCl eutectic salt met the universal treatment standard of the leachability limit for metals regulated by the Resource Conservation and Recovery Act. This study confirms the possibility of development of the IPC waste form using converter slag, showing its immobilization capability for radionuclides in both LiCl-KCl eutectic salt and off-gas scrubber solutions with significant cost savings.

  7. Development of iron phosphate ceramic waste form to immobilize radioactive waste solution

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Jongkwon [Division of Advanced Nuclear Engineering, Pohang University of Science and Technology (POSTECH), San 31, Hyoja-Dong, Pohang (Korea, Republic of); Um, Wooyong, E-mail: wooyong.um@pnnl.gov [Division of Advanced Nuclear Engineering, Pohang University of Science and Technology (POSTECH), San 31, Hyoja-Dong, Pohang (Korea, Republic of); Pacific Northwest National Laboratory, Richland, WA 99354 (United States); Choung, Sungwook [Division of Advanced Nuclear Engineering, Pohang University of Science and Technology (POSTECH), San 31, Hyoja-Dong, Pohang (Korea, Republic of)

    2014-09-15

    The objective of this research was to develop an iron phosphate ceramic (IPC) waste form using converter slag obtained as a by-product of the steel industry as a source of iron instead of conventional iron oxide. Both synthetic off-gas scrubber solution containing technetium-99 (or Re as a surrogate) and LiCl–KCl eutectic salt, a final waste solution from pyrochemical processing of spent nuclear fuel, were used as radioactive waste streams. The IPC waste form was characterized for compressive strength, reduction capacity, chemical durability, and contaminant leachability. Compressive strengths of the IPC waste form prepared with different types of waste solutions were 16 MPa and 19 MPa for LiCl–KCl eutectic salt and the off-gas scrubber simulant, respectively, which meet the minimum compressive strength of 3.45 MPa (500 psi) for waste forms to be accepted into the radioactive waste repository. The reduction capacity of converter slag, a main dry ingredient used to prepare the IPC waste form, was 4136 meq/kg by the Ce(IV) method, which is much higher than those of the conventional Fe oxides used for the IPC waste form and the blast furnace slag materials. Average leachability indexes of Tc, Li, and K for the IPC waste form were higher than 6.0, and the IPC waste form demonstrated stable durability even after 63-day leaching. In addition, the Toxicity Characteristic Leach Procedure measurements of converter slag and the IPC waste form with LiCl–KCl eutectic salt met the universal treatment standard of the leachability limit for metals regulated by the Resource Conservation and Recovery Act. This study confirms the possibility of development of the IPC waste form using converter slag, showing its immobilization capability for radionuclides in both LiCl–KCl eutectic salt and off-gas scrubber solutions with significant cost savings.

  8. Development of iron phosphate ceramic waste form to immobilize radioactive waste solution

    Science.gov (United States)

    Choi, Jongkwon; Um, Wooyong; Choung, Sungwook

    2014-09-01

    The objective of this research was to develop an iron phosphate ceramic (IPC) waste form using converter slag obtained as a by-product of the steel industry as a source of iron instead of conventional iron oxide. Both synthetic off-gas scrubber solution containing technetium-99 (or Re as a surrogate) and LiCl-KCl eutectic salt, a final waste solution from pyrochemical processing of spent nuclear fuel, were used as radioactive waste streams. The IPC waste form was characterized for compressive strength, reduction capacity, chemical durability, and contaminant leachability. Compressive strengths of the IPC waste form prepared with different types of waste solutions were 16 MPa and 19 MPa for LiCl-KCl eutectic salt and the off-gas scrubber simulant, respectively, which meet the minimum compressive strength of 3.45 MPa (500 psi) for waste forms to be accepted into the radioactive waste repository. The reduction capacity of converter slag, a main dry ingredient used to prepare the IPC waste form, was 4136 meq/kg by the Ce(IV) method, which is much higher than those of the conventional Fe oxides used for the IPC waste form and the blast furnace slag materials. Average leachability indexes of Tc, Li, and K for the IPC waste form were higher than 6.0, and the IPC waste form demonstrated stable durability even after 63-day leaching. In addition, the Toxicity Characteristic Leach Procedure measurements of converter slag and the IPC waste form with LiCl-KCl eutectic salt met the universal treatment standard of the leachability limit for metals regulated by the Resource Conservation and Recovery Act. This study confirms the possibility of development of the IPC waste form using converter slag, showing its immobilization capability for radionuclides in both LiCl-KCl eutectic salt and off-gas scrubber solutions with significant cost savings.

  9. Reference waste forms and packing material for the Nevada Nuclear Waste Storage Investigations Project

    International Nuclear Information System (INIS)

    The Lawrence Livermore National Laboratory (LLNL), Livermore, Calif., has been given the task of designing and verifying the performance of waste packages for the Nevada Nuclear Waste Storage Investigations (NNWSI) Project. NNWSI is studying the suitability of the tuffaceous rocks at Yucca Mountain, Nevada Test Site, for the potential construction of a high-level nuclear waste repository. This report gives a summary description of the three waste forms for which LLNL is designing waste packages: spent fuel, either as intact assemblies or as consolidated fuel pins, reprocessed commercial high-level waste in the form of borosilicate glass, and reprocessed defense high-level waste from the Defense Waste Processing Facility in Aiken, S.C. Reference packing material for use with the alternative waste package design for spent fuel is also described. 14 references, 8 figures, 20 tables

  10. Actinide extraction from ICPP sodium bearing waste with 0.75 M DHDECMP/TBP in Isopar L reg-sign

    International Nuclear Information System (INIS)

    Recent process development efforts at the Idaho Chemical Processing Plant include examination of solvent extraction technologies for actinide partitioning from sodium bearing waste (SBW) solutions. The use of 0.75 M dihexyl-N, N-diethylcarbamoylmethylphosphonate (DHDECMP or simply CMP) and 1.0 M tri-n-butyl phosphate (TBP) diluted in Isopar L reg-sign was explored for actinide removal from simulated SBW solutions. Experimental evaluations included batch contacts in radiotracer tests with simulated sodium bearing waste solution to measure the extraction and recovery efficiency of the organic solvent. The radioactive isotopes utilized for this study included Pu-238, Pu-239, Am-241, U-233, Np-239, Zr-95, Tc-99m, and Hg-203. Extraction contacts of the organic solvent with the traced SBW stimulant, strip (back-extraction) contacts of the loaded organic solvent with either a 1-hydroxyethane-1, 1-diphosphonic acid (HEDPA) in nitric acid solution or an oxalic acid in nitric acid solution, and solvent wash contacts with sodium carbonate were performed

  11. Waste Acceptance Testing of Secondary Waste Forms: Cast Stone, Ceramicrete and DuraLith

    Energy Technology Data Exchange (ETDEWEB)

    Mattigod, Shas V.; Westsik, Joseph H.; Chung, Chul-Woo; Lindberg, Michael J.; Parker, Kent E.

    2011-08-12

    To support the selection of a waste form for the liquid secondary wastes from WTP, Washington River Protection Solutions has initiated secondary-waste-form testing work at Pacific Northwest National Laboratory (PNNL). In anticipation of a down-selection process for a waste form for the Solidification Treatment Unit to be added to the ETF, PNNL is conducting tests on four candidate waste forms to evaluate their ability to meet potential waste acceptance criteria for immobilized secondary wastes that would be placed in the IDF. All three waste forms demonstrated compressive strengths above the minimum 3.45 MPa (500 psi) set as a target for cement-based waste forms. Further, none of the waste forms showed any significant degradation in compressive strength after undergoing thermal cycling (30 cycles in a 10 day period) between -40 C and 60 C or water immersion for 90 days. The three leach test methods are intended to measure the diffusion rates of contaminants from the waste forms. Results are reported in terms of diffusion coefficients and a leachability index (LI) calculated based on the diffusion coefficients. A smaller diffusion coefficient and a larger LI are desired. The NRC, in its Waste Form Technical Position (NRC 1991), provides recommendations and guidance regarding methods to demonstrate waste stability for land disposal of radioactive waste. Included is a recommendation to conduct leach tests using the ANS 16.1 method. The resulting leachability index (LI) should be greater than 6.0. For Hanford secondary wastes, the LI > 6.0 criterion applies to sodium leached from the waste form. For technetium and iodine, higher targets of LI > 9 for Tc and LI > 11 for iodine have been set based on early waste-disposal risk and performance assessment analyses. The results of these three leach tests conducted for a total time between 11days (ASTM C1308) to 90 days (ANS 16.1) showed: (1) Technetium diffusivity: ANSI/ANS 16.1, ASTM C1308, and EPA 1315 tests indicated that

  12. Comparison of glass and crystalline nuclear waste forms

    International Nuclear Information System (INIS)

    Nuclear waste forms may be divided into two broad categories: single phase glasses with minor crystalline components (e.g., borosilicate glasses) and crystalline waste forms, either single phase (e.g., monazite) or polyphase (e.g., SYNROC). This paper reviews the materials properties data that are available for each of these two types of waste forms. The principal data include: physical, thermal and mechanical properties, chemical durability; and radiation damage effects. Complete data are only available for borosilicate glasses and SYNROC; therefore, this comparison focuses on the performance assessment of borosilicate glass and SYNROC

  13. A study on the acceptance criteria of radioactive waste form

    International Nuclear Information System (INIS)

    It is essential to accept well solidified and packaged waste forms for the safety during the operational and post operational phase in the repository, and for this, waste the acceptance criterion is necessary for the distinction of the well solidified and packaged waste form. The objective of this report is to provide the preliminary acceptance criteria to help the later establishment of final acceptance criteria. The following factors were considered for establishing the preliminary waste acceptance criteria. 1) Matrix and waste form characteristics 2) the type of repository and its characteristics 3) establishment procedure of acceptance criteria and its technical background From this study, a qualitative preliminary criterion including the radionuclide contents, surface dose, surface contamination and so on was established. (Author)

  14. Waste form development program. Annual report, October 1982-September 1983

    Energy Technology Data Exchange (ETDEWEB)

    Colombo, P.; Kalb, P.D.; Fuhrmann, M.

    1983-09-01

    This report provides a summary of the work conducted for the Waste Form Development/Test Program at Brookhaven National Laboratory in FY 1983 under the sponsorship of the US Department of Energy's Low-Level Waste Management Program. The primary focus of this work is the investigation of new solidification agents which will provide improved immobilization of low-level radioactive wastes in an efficient, cost-effective manner. A working set of preliminary waste form evaluation criteria which could impact upon the movement of radionuclides in the disposal environment was developed. The selection of potential solidification agents for further investigation is described. Two thermoplastic materials, low-density polyethylene and a modified sulfur cement were chosen as primary candidates for further study. Three waste types were selected for solidification process development and waste form property evaluation studies which represent both new volume reduction wastes (dried evaporator concentrates and incinerator ash) and current problem wastes (ion exchange resins). Preliminary process development scoping studies were conducted to verify the compatibility of selected solidification agents and waste types and the potential for improved solidification. Waste loadings of 60 wt % Na/sub 2/SO/sub 4/, 25 wt % H/sub 3/BO/sub 3/, 25 wt % incinerator ash and 50 wt % dry ion exchange resin were achieved using low density polyethylene as a matrix material. Samples incorporating 65 wt % Na/sub 2/SO/sub 4/, 40 wt % H/sub 3/BO/sub 3/, 20 wt % incinerator ash and 40 wt % dry ion exchange resin were successfully solidified in modified sulfur cement. Additional improvements are expected for both matrix materials as process parameters are optimized. Several preliminary property evaluation studies were performed to provide the basis for an initial assessment of waste form acceptability. These included a two-week water immersion test and compressive load testing.

  15. Waste form development program. Annual report, October 1982-September 1983

    International Nuclear Information System (INIS)

    This report provides a summary of the work conducted for the Waste Form Development/Test Program at Brookhaven National Laboratory in FY 1983 under the sponsorship of the US Department of Energy's Low-Level Waste Management Program. The primary focus of this work is the investigation of new solidification agents which will provide improved immobilization of low-level radioactive wastes in an efficient, cost-effective manner. A working set of preliminary waste form evaluation criteria which could impact upon the movement of radionuclides in the disposal environment was developed. The selection of potential solidification agents for further investigation is described. Two thermoplastic materials, low-density polyethylene and a modified sulfur cement were chosen as primary candidates for further study. Three waste types were selected for solidification process development and waste form property evaluation studies which represent both new volume reduction wastes (dried evaporator concentrates and incinerator ash) and current problem wastes (ion exchange resins). Preliminary process development scoping studies were conducted to verify the compatibility of selected solidification agents and waste types and the potential for improved solidification. Waste loadings of 60 wt % Na2SO4, 25 wt % H3BO3, 25 wt % incinerator ash and 50 wt % dry ion exchange resin were achieved using low density polyethylene as a matrix material. Samples incorporating 65 wt % Na2SO4, 40 wt % H3BO3, 20 wt % incinerator ash and 40 wt % dry ion exchange resin were successfully solidified in modified sulfur cement. Additional improvements are expected for both matrix materials as process parameters are optimized. Several preliminary property evaluation studies were performed to provide the basis for an initial assessment of waste form acceptability. These included a two-week water immersion test and compressive load testing

  16. Evaluation of solidified high-level waste forms

    International Nuclear Information System (INIS)

    One of the objectives of the IAEA waste management programme is to coordinate and promote development of improved technology for the safe management of radioactive wastes. The Agency accomplished this objective specifically through sponsoring Coordinated Research Programmes on the ''Evaluation of Solidified High Level Waste Products'' in 1977. The primary objectives of this programme are to review and disseminate information on the properties of solidified high-level waste forms, to provide a mechanism for analysis and comparison of results from different institutes, and to help coordinate future plans and actions. This report is a summary compilation of the key information disseminated at the second meeting of this programme

  17. Pelleted waste form for high-level ICPP wastes

    International Nuclear Information System (INIS)

    Simulated zirconia-type calcined waste is pelletized on a 41-cm diameter disc pelletizer using 5% bentonite, 2% metakaolin, and 2% boric acid as a solid binder and 7M phosphoric plus 4M nitric acid as a liquid binder. After heat treatment at 8000C for 2 hours the pellets are impact resistant and have a leach resistance of 10-4 g/cm2 . day, based on Soxhlet leaching for 100 hours at 950C with distilled water. An integrated pilot plant is being fabricated to verify the process. 1 figure, 4 tables

  18. Transuranic contaminated waste form characterization and data base

    International Nuclear Information System (INIS)

    This report outlines the sources, quantities, characteristics and treatment of transuranic wastes in the United States. This document serves as part of the data base necessary to complete preparation and initiate implementation of transuranic wastes, waste forms, waste container and packaging standards and criteria suitable for inclusion in the present NRC waste management program. No attempt is made to evaluate or analyze the suitability of one technology over another. Indeed, by the nature of this report, there is little critical evaluation or analysis of technologies because such analysis is only appropriate when evaluating a particular application or transuranic waste streams. Due to fiscal restriction, the data base is developed from a myriad of technical sources and does not necessarily contain operating experience and the current status of all technologies. Such an effort was beyond the scope of this report

  19. Transuranic contaminated waste form characterization and data base

    Energy Technology Data Exchange (ETDEWEB)

    McArthur, W.C.; Kniazewycz, B.G.

    1980-07-01

    This report outlines the sources, quantities, characteristics and treatment of transuranic wastes in the United States. This document serves as part of the data base necessary to complete preparation and initiate implementation of transuranic wastes, waste forms, waste container and packaging standards and criteria suitable for inclusion in the present NRC waste management program. No attempt is made to evaluate or analyze the suitability of one technology over another. Indeed, by the nature of this report, there is little critical evaluation or analysis of technologies because such analysis is only appropriate when evaluating a particular application or transuranic waste streams. Due to fiscal restriction, the data base is developed from a myriad of technical sources and does not necessarily contain operating experience and the current status of all technologies. Such an effort was beyond the scope of this report.

  20. Analytical electron microscopy study of radioactive ceramic waste forms

    International Nuclear Information System (INIS)

    A ceramic waste form has been developed to immobilize the halide high-level waste stream from electrometallurgical treatment of spent nuclear fuel. Analytical electron microscopy studies, using both scanning and transmission instruments, have been performed to characterize the microstructure of this material. The microstructure consists primarily of sodalite granules (containing the bulk of the halides) bonded together with glass. The results of these studies are discussed in detail. Insight into the waste form fabrication process developed as a result of these studies is also discussed

  1. Evolution of 99Tc Species in Cementitious Nuclear Waste Form

    International Nuclear Information System (INIS)

    Technetium (Tc) is produced in large quantities as a fission product during the irradiation of 235U-enriched fuel for commercial power production and plutonium genesis for nuclear weapons. The most abundant isotope of Tc present in the wastes is 99Tc because of its high fission yield (∼6%) and long half-life (2.13x105 years). During the Cold War era, generation of fissile 239Pu for use in America's atomic weapons arsenal yielded nearly 1900 kg of 99Tc at the U.S. Department of Energy's (DOE) Hanford Site in southeastern Washington State. Most of this 99Tc is present in fuel reprocessing wastes temporarily stored in underground tanks awaiting retrieval and permanent disposal. After the wastes are retrieved from the storage tanks, the bulk of the high-level waste (HLW) and lowactivity waste (LAW) stream is scheduled to be converted into a borosilicate glass waste form that will be disposed of in a shallow burial facility called the Integrated Disposal Facility (IDF) at the Hanford Site. Even with careful engineering controls, volatilization of a fraction of Tc during the vitrification of both radioactive waste streams is expected. Although this volatilized Tc can be captured in melter off-gas scrubbers and returned to the melter, some of the Tc is expected to become part of the secondary waste stream from the vitrification process. The off-gas scrubbers downstream from the melters will generate a high pH, sodium-ammonium carbonate solution containing the volatilized Tc and other fugitive species. Effective and cost-efficient disposal of Tc found in the off-gas scrubber solution remains difficult. A cementitious waste form (Cast Stone) is one of the nuclear waste form candidates being considered to solidify the secondary radioactive liquid waste that will be generated by the operation of the waste treatment plant (WTP) at the Hanford Site. Because Tc leachability from the waste form is closely related with Tc speciation or oxidation state in both the simulant and

  2. Comparative assessment of TRU waste forms and processes. Volume II. Waste form data, process descriptions, and costs

    International Nuclear Information System (INIS)

    This volume contains supporting information for the comparative assessment of the transuranic waste forms and processes summarized in Volume I. Detailed data on the characterization of the waste forms selected for the assessment, process descriptions, and cost information are provided. The purpose of this volume is to provide additional information that may be useful when using the data in Volume I and to provide greater detail on particular waste forms and processes. Volume II is divided into two sections and two appendixes. The first section provides information on the preparation of the waste form specimens used in this study and additional characterization data in support of that in Volume I. The second section includes detailed process descriptions for the eight processes evaluated. Appendix A lists the results of MCC-1 leach test and Appendix B lists additional cost data. 56 figures, 12 tables

  3. 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.)

  4. Saltstone Vault Classification Samples Modular Caustic Side Solvent Extraction Unit/Actinide Removal Process Waste Stream April 2011

    International Nuclear Information System (INIS)

    Savannah River National Laboratory (SRNL) was asked to prepare saltstone from samples of Tank 50H obtained by SRNL on April 5, 2011 (Tank 50H sampling occurred on April 4, 2011) during 2QCY11 to determine the non-hazardous nature of the grout and for additional vault classification analyses. The samples were cured and shipped to Babcock and Wilcox Technical Services Group-Radioisotope and Analytical Chemistry Laboratory (B and W TSG-RACL) to perform the Toxic Characteristic Leaching Procedure (TCLP) and subsequent extract analysis on saltstone samples for the analytes required for the quarterly analysis saltstone sample. In addition to the eight toxic metals - arsenic, barium, cadmium, chromium, mercury, lead, selenium and silver - analytes included the underlying hazardous constituents (UHC) antimony, beryllium, nickel, and thallium which could not be eliminated from analysis by process knowledge. Additional inorganic species determined by B and W TSG-RACL include aluminum, boron, chloride, cobalt, copper, fluoride, iron, lithium, manganese, molybdenum, nitrate/nitrite as Nitrogen, strontium, sulfate, uranium, and zinc and the following radionuclides: gross alpha, gross beta/gamma, 3H, 60Co, 90Sr, 99Tc, 106Ru, 106Rh, 125Sb, 137Cs, 137mBa, 154Eu, 238Pu, 239/240Pu, 241Pu, 241Am, 242Cm, and 243/244Cm. B and W TSG-RACL provided subsamples to GEL Laboratories, LLC for analysis for the VOCs benzene, toluene, and 1-butanol. GEL also determines phenol (total) and the following radionuclides: 147Pm, 226Ra and 228Ra. Preparation of the 2QCY11 saltstone samples for the quarterly analysis and for vault classification purposes and the subsequent TCLP analyses of these samples showed that: (1) The saltstone waste form disposed of in the Saltstone Disposal Facility in 2QCY11 was not characteristically hazardous for toxicity. (2) The concentrations of the eight RCRA metals and UHCs identified as possible in the saltstone waste form were present at levels below the UTS. (3) Most

  5. SALTSTONE VAULT CLASSIFICATION SAMPLES MODULAR CAUSTIC SIDE SOLVENT EXTRACTION UNIT/ACTINIDE REMOVAL PROCESS WASTE STREAM APRIL 2011

    Energy Technology Data Exchange (ETDEWEB)

    Eibling, R.

    2011-09-28

    Savannah River National Laboratory (SRNL) was asked to prepare saltstone from samples of Tank 50H obtained by SRNL on April 5, 2011 (Tank 50H sampling occurred on April 4, 2011) during 2QCY11 to determine the non-hazardous nature of the grout and for additional vault classification analyses. The samples were cured and shipped to Babcock & Wilcox Technical Services Group-Radioisotope and Analytical Chemistry Laboratory (B&W TSG-RACL) to perform the Toxic Characteristic Leaching Procedure (TCLP) and subsequent extract analysis on saltstone samples for the analytes required for the quarterly analysis saltstone sample. In addition to the eight toxic metals - arsenic, barium, cadmium, chromium, mercury, lead, selenium and silver - analytes included the underlying hazardous constituents (UHC) antimony, beryllium, nickel, and thallium which could not be eliminated from analysis by process knowledge. Additional inorganic species determined by B&W TSG-RACL include aluminum, boron, chloride, cobalt, copper, fluoride, iron, lithium, manganese, molybdenum, nitrate/nitrite as Nitrogen, strontium, sulfate, uranium, and zinc and the following radionuclides: gross alpha, gross beta/gamma, 3H, 60Co, 90Sr, 99Tc, 106Ru, 106Rh, 125Sb, 137Cs, 137mBa, 154Eu, 238Pu, 239/240Pu, 241Pu, 241Am, 242Cm, and 243/244Cm. B&W TSG-RACL provided subsamples to GEL Laboratories, LLC for analysis for the VOCs benzene, toluene, and 1-butanol. GEL also determines phenol (total) and the following radionuclides: 147Pm, 226Ra and 228Ra. Preparation of the 2QCY11 saltstone samples for the quarterly analysis and for vault classification purposes and the subsequent TCLP analyses of these samples showed that: (1) The saltstone waste form disposed of in the Saltstone Disposal Facility in 2QCY11 was not characteristically hazardous for toxicity. (2) The concentrations of the eight RCRA metals and UHCs identified as possible in the saltstone waste form were present at levels below the UTS. (3) Most of the

  6. 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

  7. Forming artificial soils from waste materials for mine site rehabilitation

    Science.gov (United States)

    Yellishetty, Mohan; Wong, Vanessa; Taylor, Michael; Li, Johnson

    2014-05-01

    Surface mining activities often produce large volumes of solid wastes which invariably requires the removal of significant quantities of waste rock (overburden). As mines expand, larger volumes of waste rock need to be moved which also require extensive areas for their safe disposal and containment. The erosion of these dumps may result in landform instability, which in turn may result in exposure of contaminants such as trace metals, elevated sediment delivery in adjacent waterways, and the subsequent degradation of downstream water quality. The management of solid waste materials from industrial operations is also a key component for a sustainable economy. For example, in addition to overburden, coal mines produce large amounts of waste in the form of fly ash while sewage treatment plants require disposal of large amounts of compost. Similarly, paper mills produce large volumes of alkaline rejected wood chip waste which is usually disposed of in landfill. These materials, therefore, presents a challenge in their use, and re-use in the rehabilitation of mine sites and provides a number of opportunities for innovative waste disposal. The combination of solid wastes sourced from mines, which are frequently nutrient poor and acidic, with nutrient-rich composted material produced from sewage treatment and alkaline wood chip waste has the potential to lead to a soil suitable for mine rehabilitation and successful seed germination and plant growth. This paper presents findings from two pilot projects which investigated the potential of artificial soils to support plant growth for mine site rehabilitation. We found that pH increased in all the artificial soil mixtures and were able to support plant establishment. Plant growth was greatest in those soils with the greatest proportion of compost due to the higher nutrient content. These pot trials suggest that the use of different waste streams to form an artificial soil can potentially be used in mine site rehabilitation

  8. Immobilization in ceramic waste forms of the residues from treatment of mixed wastes

    International Nuclear Information System (INIS)

    The Environmental Restoration and Waste Management Applied Technology Program at LLNL is developing a Mixed Waste Management Facility to demonstrate treatment technologies that provide an alternative to incineration. As part of that program, we are developing final waste forms using ceramic processing methods for the immobilization of the treatment process residues. The ceramic phase assemblages are based on using Synroc D as a starting point and varying the phase assemblage to accommodate the differences in chemistry between the treatment process residues and the defense waste for which Synroc D was developed. Two basic formulations are used, one for low ash residues resulting from treatment of organic materials contaminated with RCRA metals, and one for high ash residues generated from the treatment of plastics and paper products. Treatment process residues are mixed with ceramic precursor materials, dried, calcined, formed into pellets at room temperature, and sintered at 1150 to 1200 degrees C to produce the final waste form. This paper discusses the chemical composition of the waste streams and waste forms, the phase assemblages that serve as hosts for inorganic waste elements, and the changes in waste form characteristics as a function of variation in process parameters

  9. Glass Ceramic Waste Forms for Combined CS+LN+TM Fission Products Waste Streams

    Energy Technology Data Exchange (ETDEWEB)

    Crum, Jarrod V.; Turo, Laura A.; Riley, Brian J.; Tang, Ming; Kossoy, Anna; Sickafus, Kurt E.

    2010-09-23

    In this study, glass ceramics were explored as an alternative waste form for glass, the current baseline, to be used for immobilizing alkaline/alkaline earth + lanthanide (CS+LN) or CS+LN+transition metal (TM) fission-product waste streams generated by a uranium extraction (UREX+) aqueous separations type process. Results from past work on a glass waste form for the combined CS+LN waste streams showed that as waste loading increased, large fractions of crystalline phases precipitated upon slow cooling.[1] The crystalline phases had no noticeable impact on the waste form performance by the 7-day product consistency test (PCT). These results point towards the development of a glass ceramic waste form for treating CS+LN or CS+LN+TM combined waste streams. Three main benefits for exploring glass ceramics are: (1) Glass ceramics offer increased solubility of troublesome components in crystalline phases as compared to glass, leading to increased waste loading; (2) The crystalline network formed in the glass ceramic results in higher heat tolerance than glass; and (3) These glass ceramics are designed to be processed by the same melter technology as the current baseline glass waste form. It will only require adding controlled canister cooling for crystallization into a glass ceramic waste form. Highly annealed waste form (essentially crack free) with up to 50X lower surface area than a typical High-Level Waste (HLW) glass canister. Lower surface area translates directly into increased durability. This was the first full year of exploring glass ceramics for the Option 1 and 2 combined waste stream options. This work has shown that dramatic increases in waste loading are achievable by designing a glass ceramic waste form as an alternative to glass. Table S1 shows the upper limits for heat, waste loading (based on solubility), and the decay time needed before treatment can occur for glass and glass ceramic waste forms. The improvements are significant for both combined waste

  10. 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

  11. Effect of Concrete Waste Form Properties on Radionuclide Migration

    Energy Technology Data Exchange (ETDEWEB)

    Mattigod, Shas V.; Bovaird, Chase C.; Wellman, Dawn M.; Skinner, De' Chauna J.; Cordova, Elsa A.; Wood, Marcus I.

    2009-09-30

    Assessing long-term performance of Category 3 waste cement grouts for radionuclide encasement requires knowledge of the radionuclide-cement interactions and mechanisms of retention (i.e., sorption or precipitation) the mechanism of contaminant release, the significance of contaminant release pathways, how waste form performance is affected by the full range of environmental conditions within the disposal facility, the process of waste form aging under conditions that are representative of processes occurring in response to changing environmental conditions within the disposal facility, the effect of waste form aging on chemical, physical, and radiological properties and the associated impact on contaminant release. This knowledge will enable accurate prediction of radionuclide fate when the waste forms come in contact with groundwater. Numerous sets of tests were initiated in fiscal years (FY) 2006-2009 to evaluate (1) diffusion of iodine (I) and technetium (Tc) from concrete into uncontaminated soil after 1 and 2 years, (2) I and rhenium (Re) diffusion from contaminated soil into fractured concrete, (3) I and Re (set 1) and Tc (set 2) diffusion from fractured concrete into uncontaminated soil, (4) evaluate the moisture distribution profile within the sediment half-cell, (5) the reactivity and speciation of uranium (VI) (U(VI)) compounds in concrete porewaters, (6) the rate of dissolution of concrete monoliths, and (7) the diffusion of simulated tank waste into concrete.

  12. Technetium Waste Form Development - Progress Report

    International Nuclear Information System (INIS)

    Analytical electron microscopy using SEM and TEM has been used to analyze a ∼5 g. ingot with composition 71.3 wt% 316SS-5.3 wt% Zr-13.2 wt% Mo-4.0 wt% Rh-6.2 wt% Re prepared at the Idaho National Laboratory. Four phase fields have been identified two of which are lamellar eutectics, with a fifth possibly present. A Zr rich phase was found distributed as fine precipitate, ∼10 (micro)m in diameter, often coating large cavities. A Mo-Fe-Re-Cr lamellar eutectic phase field appears as blocky regions ∼30 (micro)m in diameter, surrounded by a Fe-Mo-Cr lamellar eutectic phase field, and that in turn is surrounded by a Zr-Fe-Rh-Mo-Ni phase field. The eutectic phase separation reactions are different. The Mo-Fe-Re-Cr lamellar eutectic appears a result of austenitic steel forming at lower volume fraction within an Mo-Fe-Re intermetallic phase, whereas the Fe-Mo-Cr lamellar eutectic may be a result of the same intermetallic phase forming within a ferritic steel phase. Cavitation may have arisen either as a result of bubbles, or from loss of equiaxed particles during specimen preparation.

  13. Technetium Waste Form Development - Progress Report

    Energy Technology Data Exchange (ETDEWEB)

    Gelles, David S.; Ermi, Ruby M.; Buck, Edgar C.; Seffens, Rob J.; Chamberlin, Clyde E.

    2009-01-07

    Analytical electron microscopy using SEM and TEM has been used to analyze a ~5 g. ingot with composition 71.3 wt% 316SS-5.3 wt% Zr-13.2 wt% Mo-4.0 wt% Rh-6.2 wt% Re prepared at the Idaho National Laboratory. Four phase fields have been identified two of which are lamellar eutectics, with a fifth possibly present. A Zr rich phase was found distributed as fine precipitate, ~10µm in diameter, often coating large cavities. A Mo-Fe-Re-Cr lamellar eutectic phase field appears as blocky regions ~30µm in diameter, surrounded by a Fe-Mo-Cr lamellar eutectic phase field, and that in turn is surrounded by a Zr-Fe-Rh-Mo-Ni phase field. The eutectic phase separation reactions are different. The Mo-Fe-Re-Cr lamellar eutectic appears a result of austenitic steel forming at lower volume fraction within an Mo-Fe-Re intermetallic phase, whereas the Fe-Mo-Cr lamellar eutectic may be a result of the same intermetallic phase forming within a ferritic steel phase. Cavitation may have arisen either as a result of bubbles, or from loss of equiaxed particles during specimen preparation.

  14. Consolidated waste forms: glass marbles and ceramic pellets

    International Nuclear Information System (INIS)

    Glass marbles and ceramic pellets have been developed at Pacific Northwest Laboratory as part of the multibarrier concept for immobilizing high-level radioactive waste. These consolidated waste forms served as substrates for the application of various inert coatings and as ideal-sized particles for encapsulation in protective matrices. Marble and pellet formulations were based on existing defense wastes at Savannah River Plant and proposed commercial wastes. To produce marbles, glass is poured from a melter in a continuous stream into a marble-making device. Marbles were produced at PNL on a vibratory marble machine at rates as high as 60 kg/h. Other marble-making concepts were also investigated. The marble process, including a lead-encapsulation step, was judged as one of the more feasible processes for immobilizing high-level wastes. To produce ceramic pellets, a series of processing steps are required, which include: spray calcining - to dry liquid wastes to a powder; disc pelletizing - to convert waste powders to spherical pellets; sintering - to densify pellets and cause desired crystal formation. These processing steps are quite complex, and thereby render the ceramic pellet process as one of the least feasible processes for immobilizing high-level wastes

  15. Consolidated waste forms: glass marbles and ceramic pellets

    Energy Technology Data Exchange (ETDEWEB)

    Treat, R.L.; Rusin, J.M.

    1982-05-01

    Glass marbles and ceramic pellets have been developed at Pacific Northwest Laboratory as part of the multibarrier concept for immobilizing high-level radioactive waste. These consolidated waste forms served as substrates for the application of various inert coatings and as ideal-sized particles for encapsulation in protective matrices. Marble and pellet formulations were based on existing defense wastes at Savannah River Plant and proposed commercial wastes. To produce marbles, glass is poured from a melter in a continuous stream into a marble-making device. Marbles were produced at PNL on a vibratory marble machine at rates as high as 60 kg/h. Other marble-making concepts were also investigated. The marble process, including a lead-encapsulation step, was judged as one of the more feasible processes for immobilizing high-level wastes. To produce ceramic pellets, a series of processing steps are required, which include: spray calcining - to dry liquid wastes to a powder; disc pelletizing - to convert waste powders to spherical pellets; sintering - to densify pellets and cause desired crystal formation. These processing steps are quite complex, and thereby render the ceramic pellet process as one of the least feasible processes for immobilizing high-level wastes.

  16. Weathering Effect on 99Tc Leachability from Cementitious Waste Form

    International Nuclear Information System (INIS)

    The mass transfer of contaminants from the solid phase to the waste form pore water, and subsequently out of the solid waste form, is directly related to the number and size distribution of pores as well as the microstructure of the waste form. Because permeability and porosity are controlled by pore aperture size, pore volume, and pore distribution, it is important to have some indication of how these characteristics change in the waste form during weathering. Knowledge of changes in these key parameters can be used to develop predictive models that estimate diffusivity or permeability of radioactive contaminants can be used to develop predictive models that estimate diffusivity or permeability of radioactive contaminants from waste forms for long-term performance assessment. It is known that dissolution or precipitation of amorphous/crystalline phases within waste forms alters their pore structure and controls the transport of contaminants our of waste forms. One very important precipitate is calcite, which is formed as a result of carbonation reactions in cement and other high-alkalinity waste forms. Enhanced oxidation can also increase Tc leachability from the waste form. To account for these changes, weathering experiments were conducted in advance to increase our understating of the long-term Tc leachability, especially out of the cementitious waste form. Pore structure analysis was characterized using both N2 absorption analysis and XMT techniques, and the results show that cementitious waste form is a relatively highly-porous material compared to other waste forms studied in this task, Detailed characterization of Cast Stone chunks and monolith specimens indicate that carbonation reactions can change the Cast Stone pore structure, which in turn may correlate with Tc leachability. Short carbonation reaction times for the Cast Stone causes pore volume and surface area increases, while the average pore diameter decreases. Based on the changes in pore volumes

  17. Electrochemical Corrosion Studies for Modeling Metallic Waste Form Release Rates

    Energy Technology Data Exchange (ETDEWEB)

    Poineau, Frederic [Univ. of Nevada, Las Vegas, NV (United States); Tamalis, Dimitri [Florida Memorial Univ., Miami Gardens, FL (United States)

    2016-08-01

    The isotope 99Tc is an important fission product generated from nuclear power production. Because of its long half-life (t1/2 = 2.13.105 years) and beta-radiotoxicity (β-= 292 keV), it is a major concern in the long-term management of spent nuclear fuel.1 In the spent nuclear fuel, Tc is present as an alloy with Mo, Ru, Rh, and Pd called the epsilon-phase, the relative amount of which increases with fuel burn-up.2 In some separation schemes for spent nuclear fuel, Tc would be separated from the spent fuel and disposed of in a durable waste form.3 Technetium waste forms under consideration include metallic alloys, oxide ceramics and borosilicate glass.4, 5 In the development of a metallic waste form, after separation from the spent fuel, Tc would be converted to the metal, incorporated into an alloy and the resulting waste form stored in a repository.6 Metallic alloys under consideration include Tc-Zr alloys, Tc-stainless-steel alloys and Tc- Inconel alloys (Inconel is an alloy of Ni, Cr and iron which is resistant to corrosion). To predict the long term behavior of the metallic Tc waste form, understanding the corrosion properties of Tc metal and Tc alloys in various chemical environments is needed but efforts to model the behavior of Tc metallic alloys are limited. 7 One parameter that should also be considered in predicting the long-term behavior of the Tc waste form, is the ingrowth of stable Ru that occurs from the radioactive decay of 99Tc (99Tc "99Ru + β-). After a geological period of time, significant amount of Ru will be present in the Tc and may affect its corrosion properties. Studying the effect of Ru on the corrosion behavior of Tc is also of importance.

  18. Advanced waste forms research and development. Annual report

    Energy Technology Data Exchange (ETDEWEB)

    McCarthy, G.J.

    1975-06-11

    Research and development activities on advanced (alternatives to glass) nuclear waste forms are reported. The emphasis is on two phases of the work to give essential background information on supercalcine development. The first is a report of the data obtained in the study of cesium aluminosilicate for Cs and Ru fixation. Research on the compatibility of the phases formed in the complex oxide system made up of waste and additive cations is reported. The phase stability in a number of proposed formulations was determined. (JSR)

  19. Integrated AMP-PAN, TRUEX, and SREX Flowsheet Test to Remove Cesium, Surrogate Actinide Elements, and Strontium from INEEL Tank Waste Using Sorbent Columns and Centrifugal Contactors

    Energy Technology Data Exchange (ETDEWEB)

    Herbst, Ronald Scott; Law, Jack Douglas; Todd, Terry Allen; Wood, D. J.; Garn, Troy Gerry; Wade, Earlen Lawrence

    2000-02-01

    Three unit operations for the removal of selected fission products, actinides, and RCRA metals (mercury and lead) have been successfully integrated and tested for extended run times with simulated INEEL acidic tank waste. The unit operations were ion exchange for Cs removal, followed by TRUEX solvent extraction for Eu (actinide surrogate), Hg, and Re (Tc surrogate) removal, and subsequent SREX solvent extraction for Sr and Pb removal. Approximately 45 L of simulated INTEC tank waste was first processed through three ion exchange columns in series for selective Cs removal. The columns were packed with a composite ammonium molybdophosphate-polyacrylonitrile (AMP-PAN) sorbent. The experimental breakthrough data were in excellent agreement with modeling predictions based on data obtained with much smaller columns. The third column (220 cm3) was used for polishing and Cs removal after breakthrough of the up-stream columns. The Cs removal was >99.83% in the ion exchange system without interference from other species. Most of the effluent from the ion exchange (IX) system was immediately processed through a TRUEX solvent extraction flowsheet to remove europium (americium surrogate), mercury and rhenium (technetium surrogate) from the simulated waste. The TRUEX flowsheet test was performed utilizing 23 stages of 3.3-cm centrifugal contactors. Greater than 99.999% of the Eu, 96.3% of the Hg, and 56% of the Re were extracted from the simulated feed and recovered in the strip and wash streams. Over the course of the test, there was no detectable build-up of any components in the TRUEX solvent. The raffinate from the TRUEX test was stored and subsequently processed several weeks later through a SREX solvent extraction flowsheet to remove strontium, lead, and Re (Tc surrogate) from the simulated waste. The SREX flowsheet test was performed using the same centrifugal contactors used in the TRUEX test after reconfiguration and the addition of three stages. Approximately 99.9% of

  20. Performance testing of waste forms in a tuff environment

    International Nuclear Information System (INIS)

    This paper describes experimental work conducted to establish the chemical composition of water which will have reacted with Topopah Spring Member tuff prior to contact with waste packages. The experimental program to determine the behavior of spent fuel and borosilicate glass in the presence of this water is then described. Preliminary results of experiments using spent fuel segments with defects in the Zircaloy cladding are presented. Some results from parametric testing of a borosilicate glass with tuff and 304L stainless steel are also discussed. Experiments conducted using Topopah Spring tuff and J-13 well water have been conducted to provide an estimate of the post-emplacement environment for waste packages in a repository at Yucca Mountain. The results show that emplacement of waste packages should cause only small changes in the water chemistry and rock mineralogy. The changes in environment should not have any detrimental effects on the performance of metal barriers or waste forms. The NNWSI waste form testing program has provided preliminary results related to the release rate of radionuclides from the waste package. Those results indicate that release rates from both spent fuel and borosilicate glass should be below 1 part in 105 per year. Future testing will be directed toward making release rate testing more closely relevant to site specific conditions. 17 references, 7 figures

  1. The Ceramic Waste Form Process at Idaho National Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Stephen Priebe

    2007-05-01

    The treatment of spent nuclear fuel for disposition using an electrometallurgical technique results in two high-level waste forms: a ceramic waste form (CWF) and a metal waste form. Reactive metal fuel constituents, including all the transuranic metals and the majority of the fission products remain in the salt as chlorides and are processed into the CWF. The solidified salt is containerized and transferred to the CWF process where it is ground in an argon atmosphere. Zeolite 4A is ground and then dried in a mechanically-fluidized dryer. The salt and zeolite are mixed in a V-mixer and heated to 500°C to occlude the salt into the structure of the zeolite. The salt-loaded zeolite is cooled, mixed with borosilicate glass frit, and transferred to a crucible, which is placed in a furnace and heated to 925°C. During this process, known as pressureless consolidation, the zeolite is converted to the final sodalite form and the glass thoroughly encapsulates the sodalite, producing a dense, leach-resistant final waste form.

  2. Fire testing of fully active medium-level waste forms

    International Nuclear Information System (INIS)

    The effect of heat on packaged intermediate level waste (ILW) has been studied. This was done in order to be able to predict the behaviour of the ILW under accident conditions involving fire during transport or at the repository. In the study, experimental data were obtained and used in the development and validation of theoretical models to describe aspects of the behaviour of the waste form when subjected to heat. The prime objective was to be able to predict the amounts of radioactive materials released from a given incident. Four ILW streams were selected for experimental study. These four were chosen as the minimum that could be studied to provide a set of data that could be used in the prediction of the behaviour of the majority of ILW produced in the UK. Heating experiments were carried out on a small scale using packaged ILW samples made from active wastes or inactive simulants. Data were obtained on temperatures in the waste form, production of volatile materials, carry-forward of solid particulate materials and carry-forward of radionuclides. The results were used, together with data from full-scale experiments with inactive simulant ILW carried out at Winfrith, to develop and validate a theoretical model. This model calculates the temperature profiles within a package of immobilized ILW as a function of the applied heating conditions. The temperature of the waste form is used to predict the release of radioactive materials from the package. 4 refs., 65 figs., 13 tabs

  3. State of the art report on bituminized waste forms of radioactive wastes

    International Nuclear Information System (INIS)

    In this report, research and development results on the bituminization of radioactive wastes are closely reviewed, especially those regarding waste treatment technologies, waste solidifying procedures and the characteristics of asphalt and solidified forms. A new concept of the bituminization method is suggested in this report which can improve the characteristics of solidified forms. Stable solid forms with high leach resistance, high thermal resistance and good compression strength were produced by the suggested bituminization method, in which spent polyethylene from agricultural farms was added. This report can help further research and development of improved bituminized forms of radioactive wastes that will maintain long term stabilities in disposal sites. (author). 59 refs., 19 tabs., 18 figs

  4. State of the art report on bituminized waste forms of radioactive wastes

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Tae Kook; Shon, Jong Sik; Kim, Kil Jeong; Lee, Kang Moo; Jung, In Ha

    1998-03-01

    In this report, research and development results on the bituminization of radioactive wastes are closely reviewed, especially those regarding waste treatment technologies, waste solidifying procedures and the characteristics of asphalt and solidified forms. A new concept of the bituminization method is suggested in this report which can improve the characteristics of solidified forms. Stable solid forms with high leach resistance, high thermal resistance and good compression strength were produced by the suggested bituminization method, in which spent polyethylene from agricultural farms was added. This report can help further research and development of improved bituminized forms of radioactive wastes that will maintain long term stabilities in disposal sites. (author). 59 refs., 19 tabs., 18 figs

  5. 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

  6. Characteristics of borosilicate waste glass form for high-level radioactive waste

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Seung Soo; Chun, Kwan Sik; Choi, Jong Won; Kang, Chul Hyung

    2001-03-01

    Basic data, required for the design and the performance assessment of a repository of HLW, suchas the chemical composition and the characteristics of the borosilicate waste glass have been identified according to the burn-ups of spent PWR fuels. The diemnsion of waste canister is 430mm in diameter and 1135mm in length, and the canister should hold less than 2kwatts of heat from their decay of radionuclides contained in the HLW. Based on the reprocessing of 5 years-cooled spent fuel, one canister could hold about 11.5wt.% and 10.8wt.% of oxidized HLW corresponding to their burn-ups of 45,000MWD/MTU and 55,000MWD/MTU, respectively. These waste forms have been recommanded as the reference waste forms of HLW. The characteristics of these wastes as a function of decay time been evaluated. However, after a specific waste form and a specific site for the disposal would be selected, the characteristics of the waste should be reevaluated under the consideration of solidification period, loaded waste, storage condition and duration, site circumstances for the repository system and its performance assessment.

  7. Technical area status report for low-level mixed waste final waste forms. Volume 2, Appendices

    Energy Technology Data Exchange (ETDEWEB)

    Mayberry, J.L.; Huebner, T.L. [Science Applications International Corp., Idaho Falls, ID (United States); Ross, W. [Pacific Northwest Lab., Richland, WA (United States); Nakaoka, R. [Los Alamos National Lab., NM (United States); Schumacher, R. [Westinghouse Savannah River Co., Aiken, SC (United States); Cunnane, J.; Singh, D. [Argonne National Lab., IL (United States); Darnell, R. [EG and G Idaho, Inc., Idaho Falls, ID (United States); Greenhalgh, W. [Westinghouse Hanford Co., Richland, WA (United States)

    1993-08-01

    This report presents information on low-level mixed waste forms.The descriptions of the low-level mixed waste (LLMW) streams that are considered by the Mixed Waste Integrated Program (MWIP) are given in Appendix A. This information was taken from descriptions generated by the Mixed Waste Treatment Program (MWTP). Appendix B provides a list of characteristic properties initially considered by the Final Waste Form (FWF) Working Group (WG). A description of facilities available to test the various FWFs discussed in Volume I of DOE/MWIP-3 are given in Appendix C. Appendix D provides a summary of numerous articles that were reviewed on testing of FWFS. Information that was collected by the tests on the characteristic properties considered in this report are documented in Appendix D. The articles reviewed are not a comprehensive list, but are provided to give an indication of the data that are available.

  8. Technical area status report for low-level mixed waste final waste forms

    International Nuclear Information System (INIS)

    This report presents information on low-level mixed waste forms.The descriptions of the low-level mixed waste (LLMW) streams that are considered by the Mixed Waste Integrated Program (MWIP) are given in Appendix A. This information was taken from descriptions generated by the Mixed Waste Treatment Program (MWTP). Appendix B provides a list of characteristic properties initially considered by the Final Waste Form (FWF) Working Group (WG). A description of facilities available to test the various FWFs discussed in Volume I of DOE/MWIP-3 are given in Appendix C. Appendix D provides a summary of numerous articles that were reviewed on testing of FWFS. Information that was collected by the tests on the characteristic properties considered in this report are documented in Appendix D. The articles reviewed are not a comprehensive list, but are provided to give an indication of the data that are available

  9. Method of making nanostructured glass-ceramic waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Gao, Huizhen; Wang, Yifeng; Rodriguez, Mark A.; Bencoe, Denise N.

    2014-07-08

    A waste form for and a method of rendering hazardous materials less dangerous is disclosed that includes fixing the hazardous material in nanopores of a nanoporous material, reacting the trapped hazardous material to render it less volatile/soluble, and vitrifying the nanoporous material containing the less volatile/soluble hazardous material.

  10. Mixture for solidification of liquid radioactive wastes into stable forms

    International Nuclear Information System (INIS)

    A mixture is proposed for cementing liquid radioactive wastes into chemically stable, mechanically strong, transportable and storable forms. The mixture consists of 60-80 wt.% Portland cement, 5-15 wt.% flue silica dust and 15-25 wt.% zeolitic tuffite. (Z.S.)

  11. Microstructural characterization of glass and ceramic simulated waste forms

    International Nuclear Information System (INIS)

    The microstructures of three nonradioactive glass samples simulating three Hanford process waste forms were characterized. Two samples of iodine sodalite which simulate the fixation of radioactive iodine were also characterized. X-ray diffraction, electron microscopy + x-ray energy dispersive spectrometry, and electron microprobe analysis were used in the characterization

  12. 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.

  13. The role of chemical reaction in waste-form performance

    International Nuclear Information System (INIS)

    The dissolution rate of waste solids in a geologic repository is a complex function of waste form geometry, chemical raction rate, exterior flow field, and chemical environment. We present here an analysis to determine the stady-state mass transfer rate, over the entire range of flow conditions relevant to geologic disposal of nuclear waste. The equations for steady-state mass transfer with a chemical-reaction-rate boundary condition are solved by three different mathematical techniques which supplement each other. This theory is illustrated with laboratory leach data for borosilicate-glass and a spherical spent-fuel waste form under typical repository conditions. For borosilicate glass waste in the temperature range of 57/degree/C to 250/degree/C, dissolution rate in a repository is determined for a wide range of chemical reaction rates and for Peclet numbers from zero to well over 100, far beyond any Peclet values expected in a repository. Spent-fuel dissolution in a repository is also investigated, based on the limited leach data now available. 10 refs., 4 figs., 1 tab

  14. Preparation of a technology development roadmap for the Accelerator Transmutation of Waste (ATW) System : report of the ATW separations technologies and waste forms technical working group

    International Nuclear Information System (INIS)

    In response to a Congressional mandate to prepare a roadmap for the development of Accelerator Transmutation of Waste (ATW) technology, a Technical Working Group comprised of members from various DOE laboratories was convened in March 1999 for the purpose of preparing that part of the technology development roadmap dealing with the separation of certain radionuclides for transmutation and the disposal of residual radioactive wastes from these partitioning operations. The Technical Working Group for ATW Separations Technologies and Waste Forms completed its work in June 1999, having carefully considered the technology options available. A baseline process flowsheet and backup process were identified for initial emphasis in a future research, development and demonstration program. The baseline process combines aqueous and pyrochemical processes to permit the efficient separation of the uranium, technetium, iodine and transuranic elements from the light water reactor (LWR) fuel in the head-end step. The backup process is an all- pyrochemical system. In conjunction with the aqueous process, the baseline flowsheet includes a pyrochemical process to prepare the transuranic material for fabrication of the ATW fuel assemblies. For the internal ATW fuel cycle the baseline process specifies another pyrochemical process to extract the transuranic elements, Tc and 1 from the ATW fuel. Fission products not separated for transmutation and trace amounts of actinide elements would be directed to two high-level waste forms, one a zirconium-based alloy and the other a glass/sodalite composite. Baseline cost and schedule estimates are provided for a RD and D program that would provide a full-scale demonstration of the complete separations and waste production flowsheet within 20 years

  15. Preparation of a technology development roadmap for the Accelerator Transmutation of Waste (ATW) System : report of the ATW separations technologies and waste forms technical working group.

    Energy Technology Data Exchange (ETDEWEB)

    Collins, E.; Duguid, J.; Henry, R.; Karell, E.; Laidler, J.; McDeavitt, S.; Thompson, M.; Toth, M.; Williamson, M.; Willit, J.

    1999-08-12

    In response to a Congressional mandate to prepare a roadmap for the development of Accelerator Transmutation of Waste (ATW) technology, a Technical Working Group comprised of members from various DOE laboratories was convened in March 1999 for the purpose of preparing that part of the technology development roadmap dealing with the separation of certain radionuclides for transmutation and the disposal of residual radioactive wastes from these partitioning operations. The Technical Working Group for ATW Separations Technologies and Waste Forms completed its work in June 1999, having carefully considered the technology options available. A baseline process flowsheet and backup process were identified for initial emphasis in a future research, development and demonstration program. The baseline process combines aqueous and pyrochemical processes to permit the efficient separation of the uranium, technetium, iodine and transuranic elements from the light water reactor (LWR) fuel in the head-end step. The backup process is an all- pyrochemical system. In conjunction with the aqueous process, the baseline flowsheet includes a pyrochemical process to prepare the transuranic material for fabrication of the ATW fuel assemblies. For the internal ATW fuel cycle the baseline process specifies another pyrochemical process to extract the transuranic elements, Tc and 1 from the ATW fuel. Fission products not separated for transmutation and trace amounts of actinide elements would be directed to two high-level waste forms, one a zirconium-based alloy and the other a glass/sodalite composite. Baseline cost and schedule estimates are provided for a RD&D program that would provide a full-scale demonstration of the complete separations and waste production flowsheet within 20 years.

  16. 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

  17. Testing of high-level waste forms under repository conditions

    International Nuclear Information System (INIS)

    The workshop on testing of high-level waste forms under repository conditions was held on 17 to 21 October 1988 in Cadarache, France, and sponsored by the Commission of the European Communities (CEC), the Commissariat a l'energie atomique (CEA) and the Savannah River Laboratory (US DOE). Participants included representatives from Australia, Belgium, Denmark, France, Germany, Italy, Japan, the Netherlands, Sweden, Switzerland, The United Kingdom and the United States. The first part of the conference featured a workshop on in situ testing of simulated nuclear waste forms and proposed package components, with an emphasis on the materials interface interactions tests (MIIT). MIIT is a sevent-part programme that involves field testing of 15 glass and waste form systems supplied by seven countries, along with potential canister and overpack materials as well as geologic samples, in the salt geology at the Waste Isolation Pilot Plant (WIPP) in Carlsbad, New Mexico, USA. This effort is still in progress and these proceedings document studies and findings obtained thus far. The second part of the meeting emphasized multinational experimental studies and results derived from repository systems simulation tests (RSST), which were performed in granite, clay and salt environments

  18. Diffusion-based leaching models for glassy waste forms

    International Nuclear Information System (INIS)

    Most scenarios for the disposal of high-level nuclear wastes assume burial under conditions in which only a limited quantity of groundwater will contact the waste form. In order to model these conditions, it is necessary to describe the release of species from a waste form matrix in contact with a limited volume of leachant in which the concentration of released species is not zero and is itself a function of release rate. Eight leaching models are presented that include the cases of a dissolving and a nondissolving matrix, finite, infinite, and replenished leachant volumes, and a matrix covered by a surface layer with different properties. The equations that describe these models assume a linear concentration profile of the diffusing species within the waste form and apply Fick's first law to obtain the leach rate. In three cases a direct comparison is possible between the solutions of these equations and solutions obtained by use of the diffusion equation derived from Fick's second law. Good agreement is found. The equations given are convenient for use with programmable calculators

  19. Radiation damage studies related to nuclear waste forms

    International Nuclear Information System (INIS)

    Much of the previously reported work on alpha radiation effects on crystalline phases of importance to nuclear waste forms has been derived from radiation effects studies of composite waste forms. In the present work, two single-phase crystalline materials, Gd2Ti2O7 (pyrochlore) and CaZrTi2O7 (zirconolite), of relative importance to current waste forms were studied independently by doping with 244Cm at the 3 wt % level. Changes in the crystalline structure measured by x-ray diffraction as a function of dose show that damage ingrowth follows an expected exponential relationship of the form ΔV/V0 = A[1-exp(-BD)]. In both cases, the materials became x-ray amorphous before the estimated saturation value was reached. The predicted magnitudes of the unit cell volume changes at saturation are 5.4% and 3.5%, respectively, for Gd2Ti2O7 and CaZrTi2O7. The later material exhibited anisotropic behavior in which the expansion of the monoclinic cell in the c0 direction was over five times that of the a0 direction. The effects of transmutations on the properties of high-level waste solids have not been studied until now because of the long half-lives of the important fission products. This problem was circumvented in the present study by preparing materials containing natural cesium and then irradiating them with neutrons to produce 134Cs, which has only a 2y half-life. The properties monitored at about one year intervals following irradiation have been density, leach rate and microstructure. A small amount of x-ray diffraction work has also been done. Small changes in density and leach rate have been observed for some of the materials, but they were not large enough to be of any consequence for the final disposal of high level wastes

  20. 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)

  1. Research and development of waste forms for geological disposal

    International Nuclear Information System (INIS)

    Ceramics are candidate materials for immobilizing high-level waste (HLW) stemming from the reprocessing of spent fuels. We are proceeding with R and D on two types of ceramic waste form : a polyphase titanate ceramic named Synroc and three kinds of single-phase zirconium ceramics. The effect of self-irradiation damage on the long-term integrity of Synroc due to alpha decay was studied under a cooperative program between JAERI and ANSTO. The hot-pressed polyphase titanate ceramic (10 wt% waste loading) was doped with 244Cm to accumulate a dose of 1.6 x 1018 alpha decays/g. The phase assemblage of the curium-doped titanate ceramic included freudenbergite and loveringite in addition to three main phases: hollandite, perovskite and zirconolite. Accumulation of alpha decays was accompanied by a gradual decrease in density. The change in density was -2.7 % after an equivalent age of 45000 years. The durability of three single-phase zirconium ceramics which contained the appropriate amount of simulated high-level waste elements was examined at 90degC and 150degC in hydrochloric acid or deionized water. The waste forms examined included 10 mol% Y2O3-stabilized ZrO2, La2Zr2O7 with a pyrochlore structure, and CaZrO3 with a perovskite structure. La2Zr2O7 showed excellent durability, and leach rates of all constituents were less than about 10-4 g·m-2·day-1 at 150degC in deionized water. This suggests that La2Zr2O7 is a promising candidate material for immobilization of waste elements from HLW. (J.P.N.)

  2. Measurements of Mercury Released from Solidified/Stabilized Waste Forms

    International Nuclear Information System (INIS)

    This report covers work performed during FY 1999-2000 in support of treatment demonstrations conducted for the Mercury Working Group of the U.S. Department of Energy (DOE) Mixed Waste Focus Area. In order to comply with the requirements of the Resource Conservation and Recovery Act, as implemented by the U.S. Environmental Protection Agency (EPA), DOE must use one of these procedures for wastes containing mercury at levels above 260 ppm: a retorting/roasting treatment or an incineration treatment (if the wastes also contain organics). The recovered radioactively contaminated mercury must then be treated by an amalgamation process prior to disposal. The DOE Mixed Waste Focus Area and Mercury Working Group are working with the EPA to determine if some alternative processes could treat these types of waste directly, thereby avoiding for DOE the costly recovery step. They sponsored a demonstration in which commercial vendors applied their technologies for the treatment of two contaminated waste soils from Brookhaven National Laboratory. Each soil was contaminated with ∼4500 ppm mercury; however, one soil had as a major radioelement americium-241, while the other contained mostly europium-152. The project described in this report addressed the need for data on the mercury vapor released by the solidified/stabilized mixed low-level mercury wastes generated during these demonstrations as well as the comparison between the untreated and treated soils. A related work began in FY 1998, with the measurement of the mercury released by amalgamated mercury, and the results were reported in ORNL/TM-13728. Four treatments were performed on these soils. The baseline was obtained by thermal treatment performed by SepraDyne Corp., and three forms of solidification/stabilization were employed: one using sulfur polymer cement (Brookhaven National Laboratory), one using portland cement [Allied Technology Group (ATG)], and a third using proprietary additives (Nuclear Fuel Services)

  3. Electrochemical Corrosion Studies for Modeling Metallic Waste Form Release Rates

    Energy Technology Data Exchange (ETDEWEB)

    Poineau, Frederic [Univ. of Nevada, Las Vegas, NV (United States); Tamalis, Dimitri [Florida Memorial Univ., Miami Gardens, FL (United States)

    2016-08-01

    The isotope 99Tc is an important fission product generated from nuclear power production. Because of its long half-life (t1/2 = 2.13 ∙ 105 years) and beta-radiotoxicity (β⁻ = 292 keV), it is a major concern in the long-term management of spent nuclear fuel. In the spent nuclear fuel, Tc is present as an alloy with Mo, Ru, Rh, and Pd called the epsilon-phase, the relative amount of which increases with fuel burn-up. In some separation schemes for spent nuclear fuel, Tc would be separated from the spent fuel and disposed of in a durable waste form. Technetium waste forms under consideration include metallic alloys, oxide ceramics and borosilicate glass. In the development of a metallic waste form, after separation from the spent fuel, Tc would be converted to the metal, incorporated into an alloy and the resulting waste form stored in a repository. Metallic alloys under consideration include Tc–Zr alloys, Tc–stainless steel alloys and Tc–Inconel alloys (Inconel is an alloy of Ni, Cr and iron which is resistant to corrosion). To predict the long-term behavior of the metallic Tc waste form, understanding the corrosion properties of Tc metal and Tc alloys in various chemical environments is needed, but efforts to model the behavior of Tc metallic alloys are limited. One parameter that should also be considered in predicting the long-term behavior of the Tc waste form is the ingrowth of stable Ru that occurs from the radioactive decay of 99Tc (99Tc → 99Ru + β⁻). After a geological period of time, significant amounts of Ru will be present in the Tc and may affect its corrosion properties. Studying the effect of Ru on the corrosion behavior of Tc is also of importance. In this context, we studied the electrochemical behavior of Tc metal, Tc-Ni alloys (to model Tc-Inconel alloy) and Tc-Ru alloys in acidic media. The study of Tc-U alloys has also been performed in order to better understand the

  4. Low sintering temperature glass waste forms for sequestering radioactive iodine

    Science.gov (United States)

    Nenoff, Tina M.; Krumhansl, James L.; Garino, Terry J.; Ockwig, Nathan W.

    2012-09-11

    Materials and methods of making low-sintering-temperature glass waste forms that sequester radioactive iodine in a strong and durable structure. First, the iodine is captured by an adsorbant, which forms an iodine-loaded material, e.g., AgI, AgI-zeolite, AgI-mordenite, Ag-silica aerogel, ZnI.sub.2, CuI, or Bi.sub.5O.sub.7I. Next, particles of the iodine-loaded material are mixed with powdered frits of low-sintering-temperature glasses (comprising various oxides of Si, B, Bi, Pb, and Zn), and then sintered at a relatively low temperature, ranging from 425.degree. C. to 550.degree. C. The sintering converts the mixed powders into a solid block of a glassy waste form, having low iodine leaching rates. The vitrified glassy waste form can contain as much as 60 wt % AgI. A preferred glass, having a sintering temperature of 500.degree. C. (below the silver iodide sublimation temperature of 500.degree. C.) was identified that contains oxides of boron, bismuth, and zinc, while containing essentially no lead or silicon.

  5. Crystallization behavior during melt-processing of ceramic waste forms

    Science.gov (United States)

    Tumurugoti, Priyatham; Sundaram, S. K.; Misture, Scott T.; Marra, James C.; Amoroso, Jake

    2016-05-01

    Multiphase ceramic waste forms based on natural mineral analogs are of great interest for their high chemical durability, radiation resistance, and thermodynamic stability. Melt-processed ceramic waste forms that leverage existing melter technologies will broaden the available disposal options for high-level nuclear waste. This work reports on the crystallization behavior in selected melt-processed ceramics for waste immobilization. The phase assemblage and evolution of hollandite, zirconolite, pyrochlore, and perovskite type structures during melt processing were studied using thermal analysis, x-ray diffraction, and electron microscopy. Samples prepared by melting followed by annealing and quenching were analyzed to determine and measure the progression of the phase assemblage. Samples were melted at 1500 °C and heat-treated at crystallization temperatures of 1285 °C and 1325 °C corresponding to exothermic events identified from differential scanning calorimetry measurements. Results indicate that the selected multiphase composition partially melts at 1500 °C with hollandite coexisting as crystalline phase. Perovskite and zirconolite phases crystallized from the residual melt at temperatures below 1350 °C. Depending on their respective thermal histories, different quenched samples were found to have different phase assemblages including phases such as perovskite, zirconolite and TiO2.

  6. Tailored ceramic consolidation forms for ICPP waste compositions

    International Nuclear Information System (INIS)

    This paper reports a polyphase tailored ceramic developed for the consolidation of simulated ICPP (Idaho Chemical Processing Plant)-type high Zr content high-level waste (HLW) calcines. The ceramic is specifically designed to provide chemically stable host phases for each species present in the HLW and to maximize waste volume reduction through high loadings and form density. The ceramic is designed for a 73 wt% waste loading with a density of 3.35 ± 0.05 (g/cm3). The major phase in the ceramic is a high-silica glass, which contains the neutron poison boron as well as the majority of the nonrefractory species in the waste. The primary crystalline phases are calcium fluoride, calcium-yttrium stabilized cubic zirconia, a hexagonal apatite type silicate containing the plutonium simulant Ce, and a Cd metal phase. Minor phases include zircon, zirconolite, and a sphene-type. Leaching testing and microscopic analysis shows the ceramic form to be chemically durable, with only the glass phase showing any detectable dissolution in deionized water at 90 degrees C

  7. Polyethylene encapsulatin of nitrate salt wastes: Waste form stability, process scale-up, and economics

    International Nuclear Information System (INIS)

    A polyethylene encapsulation system for treatment of low-level radioactive, hazardous, and mixed wastes has been developed at Brookhaven National Laboratory. Polyethylene has several advantages compared with conventional solidification/stabilization materials such as hydraulic cements. Waste can be encapsulated with greater efficiency and with better waste form performance than is possible with hydraulic cement. The properties of polyethylene relevant to its long-term durability in storage and disposal environments are reviewed. Response to specific potential failure mechanisms including biodegradation, radiation, chemical attack, flammability, environmental stress cracking, and photodegradation are examined. These data are supported by results from extensive waste form performance testing including compressive yield strength, water immersion, thermal cycling, leachability of radioactive and hazardous species, irradiation, biodegradation, and flammability. The bench-scale process has been successfully tested for application with a number of specific ''problem'' waste streams. Quality assurance and performance testing of the resulting waste form confirmed scale-up feasibility. Use of this system at Rocky Flats Plant can result in over 70% fewer drums processed and shipped for disposal, compared with optimal cement formulations. Based on the current Rocky Flats production of nitrate salt per year, polyethylene encapsulation can yield an estimated annual savings between $1.5 million and $2.7 million, compared with conventional hydraulic cement systems. 72 refs., 23 figs., 16 tabs

  8. Technical viability and development needs for waste forms and facilities

    Energy Technology Data Exchange (ETDEWEB)

    Pegg, I.; Gould, T.

    1996-05-01

    The objective of this breakout session was to provide a forum to discuss technical issues relating to plutonium-bearing waste forms and their disposal facilities. Specific topics for discussion included the technical viability and development needs associated with the waste forms and/or disposal facilities. The expected end result of the session was an in-depth (so far as the limited time would allow) discussion of key issues by the session participants. The session chairs expressed allowance for, and encouragement of, alternative points of view, as well as encouragement for discussion of any relevant topics not addressed in the paper presentations. It was not the intent of this session to recommend or advocate any one technology over another.

  9. Preliminary waste form characteristics report Version 1.0. Revision 1

    Energy Technology Data Exchange (ETDEWEB)

    Stout, R.B.; Leider, H.R. [eds.

    1991-10-11

    This report focuses on radioactive waste form characteristics that will be used to design a waste package and an engineered barrier system (EBS) for a suitable repository as part of the Yucca Mountain Project. The term waste form refers to irradiated reactor fuel, other high-level waste (HLW) in various physical forms, and other radioactive materials (other than HLW) which are received for emplacement in a geologic repository. Any encapsulating of stabilizing matrix is also referred to as a waste form.

  10. The ‘granite encapsulation’ route to the safe disposal of Pu and other actinides

    Science.gov (United States)

    Gibb, F. G. F.; Taylor, K. J.; Burakov, B. E.

    2008-03-01

    Waste actinides, including plutonium, present a long-term management problem and a serious security issue. Immobilisation in mineral or ceramic waste forms for interim storage is a widely proposed first step. The safest, most secure geological disposal for Pu is in very deep boreholes and we propose that the key step to combination of these immobilisation and disposal concepts is encapsulation of the waste form in cylinders of recrystallized granite. We discuss the underpinning science, focusing on experimental work, and consider implementation. Finally, we present and discuss analyses of zircon, UO 2 and Ce-doped cubic zirconia from high pressure and temperature experiments in granitic melts that demonstrate the viability of this solution and that actinides can be isolated from the environment for millions, maybe hundreds of millions, of years.

  11. Waste form characterization and its relationship to transportation accident analysis

    International Nuclear Information System (INIS)

    The response of potential waste forms should be determined for extreme transportation environments that must be postulated for environmental impact analysis and also for hypothetical accident conditions to which packagings and contents must be subjected for licensing purposes. The best approach may be to test materials up to and beyond their failure point; such an approach would establish failure thresholds. Specification of what denotes failure would be defined by existing or proposed regulations or dictated by requirements developed from accident analysis. Responses to physical and thermal insults are the most important for licensing or analysis and need to be thoroughly characterized. Others in need of characterization might be responses to extreme chemical environments and to intense and prolonged radiation exposure. A complete characterization of waste-form responses would be desirable for environments that are considered extreme for transportation accidents but which may be typical for processing or disposal environments. In addition, the characterizations that are performed must be completed in laboratory environments which can be readily correlated to accident environments and must be meaningfully conveyed to a transportation impact analyst. As an example, leaching data as commonly presented are not usable to the analyst and are obtained under conditions that are not directly applicable to conditions of most transportation accidents. Transportation analysts are in need of data useful for calculating environmental impacts and for licensing of packagings. Future waste form development programs and associated decisions should consider the needs of transportation analysts

  12. The Ceramic Waste Form Process at the Idaho National Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Ken Bateman; Stephen Priebe

    2006-08-01

    The treatment of spent nuclear fuel for disposition using an electrometallurgical technique results in two high-level waste forms: a ceramic waste form (CWF) and a metal waste form (MWF). The CWF is a composite of sodalite and glass, which stabilizes the active fission products (alkali, alkaline earths, and rare earths) and transuranic (TRU) elements. Reactive metal fuel constituents, including all the TRU metals and the majority of the fission products remain in the salt as chlorides and are processed into the CWF. The solidified salt is containerized and transferred to the CWF process where it is ground in an argon atmosphere. Zeolite 4A is dried in a mechanically-fluidized dryer to about 0.1 wt% moisture and ground to a particle-size range of 45µ to 250µ. The salt and zeolite are mixed in a V-mixer and heated to 500°C for about 18 hours. During this process, the salt occludes into the structure of the zeolite. The salt-loaded zeolite (SLZ) is cooled and then mixed with borosilicate glass frit with a comparable particle-size range. The SLZ/glass mixture is transferred to a crucible, which is placed in a furnace and heated to 925°C. During this process, known as pressureless consolidation, the zeolite is converted to the final sodalite form and the glass thoroughly encapsulates the sodalite, producing a dense, leach-resistant final waste form. During the last several years, changes have occurred to the process, including: particle size of input materials and conversion from hot isostatic pressing to pressureless consolidation, This paper is intended to provide the current status of the CWF process focusing on the adaptation to pressureless consolidation. Discussions will include impacts of particle size on final waste form and the pressureless consolidation cycle. A model will be presented that shows the heating and cooling cycles and the effect of radioactive decay heat on the amount of fission products that can be incorporated into the CWF.

  13. Radiation damage effects in pyrochlore and zirconolite ceramic matrices for the immobilization of actinide-rich wastes

    Energy Technology Data Exchange (ETDEWEB)

    Lumpkin, G.R.; Begg, B.D.; Smith, K.L. [Materials Div., Australian Nuclear Science and Technology Organisation, Menai, NSW (Australia)

    2000-07-01

    Actinide-doping experiments using short-lived {sup 238}Pu and {sup 244}Cm have demonstrated that pyrochlore and zirconolite become fully amorphous at a dose of 0.2-0.5 x 10{sup 16} {alpha}/mg at ambient temperature and exhibit bulk swelling of 5-7%. Detailed studies of natural samples have included determination of the critical amorphization dose, long-term annealing rate, microstructural changes as a function of dose, and the thermal histories of the host rocks. Together, the laboratory based work and studies of natural samples indicate that the critical amorphization dose will increase by about a factor of 2-4 for samples stored at temperatures of 100-200 deg. C for up to 10 million years. These studies of alpha-decay damage have been complemented by heavy ion irradiation studies over the last ten years. Most of the irradiation work has concerned the critical amorphization dose as a function of temperature in thin films; however, some work has been carried out on bulk samples. The irradiation work indicates that most pyrochlore and zirconolite compositions will have similar critical amorphization doses at low temperatures (e.g., below 300-400 deg. C). Pyrochlore with Zr as the major B-site cation transform to a defect fluorite structure with increasing ion irradiation dose, but do not become amorphous. (authors)

  14. Support for DOE program in mineral waste-form development

    International Nuclear Information System (INIS)

    This research investigation relates to sintered simulation ceramic waste forms of the generic SYNROC compositional type. Though they have been formulated with simulated wastes only, they serve as prototypes for potential hot, processed, crystalline waste forms whose combined thermodynamic stability and physical integrity are considered to render them capable of long-term imobilization of high-level radwastes under deep geologic disposal conditions. The problems involved are nontrivial, largely because of the very complex nature of the radwastes: a typical waste stream would contain more than 31 cation species. When the stabilizing matrix constituents are included, the final batch composition must successfully account (and find substitutional homes for some 35 different cation species. One of the important objectives of this study thus has been to develop a computer-based method for simulating these complex ion substitutions, and for calculating the resultant phase demands and batch formulations. Primary goals of the study have been (1) use of that computer simulation capability to incorporate rationally the radwaste ions from a specific waste stream (PW-7a) into the available SYNROC lattice sites and (2) utilization of existing ceramic processing and sintering methodologies to assure (and to understand) the attainment of high density, fine microstructure, full phase development and other features of the sintered product which are known to relate directly to its integrity and leach resistance. Though improved resistance to leaching has been a continuing goal, time and budget constraints have precluded initiation of any leachability studies of these new compositions during this contract period. 27 references, 15 figures, 6 tables

  15. 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...

  16. Transuranic contaminated waste form characterization and data base

    International Nuclear Information System (INIS)

    This volume contains 5 appendices. Title listing are: technologies for recovery of transuranics; nondestructive assay of TRU contaminated wastes; miscellaneous waste characteristics; acceptance criteria for TRU waste; and TRU waste treatment technologies

  17. Description of DWPF reference waste form and canister

    Energy Technology Data Exchange (ETDEWEB)

    1981-06-01

    This document describes the reference waste form and canister for the Defense Waste Processing Facility (DWPF). The facility is planned for location at the Savannah River Plant in Aiken, SC, and is scheduled for construction authorization during FY-1983. The reference canister is fabricated of 24-in.-OD 304L stainless steel pipe with a dished bottom, domed head, and lifting and welding flanges on the head neck. The overall canister length is 9 ft 10 in., with a wall thickness of 3/8-in. (schedule 20 pipe). The canister length was selected to reduce equipment cell height in the DWPF to a practical size. The canister diameter was selected to ensure that a filled canister with its shipping cask could be accommodated on a legal-weight truck. The overall dimensions and weight appear to be generally compatible with preliminary assessments of repository requirements. The reference waste form is borosilicate glass containing approximately 28 wt % sludge oxides with the balance glass frit. Borosilicate glass was chosen because of its high resistance to leaching by water, its relatively high solubility for nuclides found in the sludge, and its reasonably low melting temperature. The glass frit contains approximately 58% SiO/sub 2/ and 15% B/sub 2/O/sub 3/. This composition results in a low average leachability in the waste form of approximately 5 x 10/sup -9/ g/cm/sup 2/-day based on /sup 137/Cs over 365 days in 25/sup 0/C water. The canister is filled with 3260 lb of glass which occupies about 85% of the free canister volume. The filled canister will generate approximately 425 watts when filled with oxides from 5-year-old sludge and 15-year-old supernate from the Stage 1 and Stage 2 processes. The radionuclide content of the canister is about 150,000 curies, with a radiation level of 2 x 10/sup 4/ rem/hour at 1 cm.

  18. Immobilization of fission products in phosphate ceramic waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Singh, D.; Wagh, A. [Argonne National Lab., IL (United States)

    1997-10-01

    Chemically bonded phosphate ceramics (CBPCs) have several advantages that make them ideal candidates for containing radioactive and hazardous wastes. In general, phosphates have high solid-solution capacities for incorporating radionuclides, as evidenced by several phosphates (e.g., monazites and apatites) that are natural analogs of radioactive and rare-earth elements. The phosphates have high radiation stability, are refractory, and will not degrade in the presence of internal heating by fission products. Dense and hard CBPCs can be fabricated inexpensively and at low temperature by acid-base reactions between an inorganic oxide/hydroxide powder and either phosphoric acid or an acid-phosphate solution. The resulting phosphates are extremely insoluble in aqueous media and have excellent long-term durability. CBPCs offer the dual stabilization mechanisms of chemical fixation and physical encapsulation, resulting in superior waste forms. The goal of this task is develop and demonstrate the feasibility of CBPCs for S/S of wastes containing fission products. The focus of this work is to develop a low-temperature CBPC immobilization system for eluted {sup 99}Tc wastes from sorption processes.

  19. A Fabrication of Salt-Loaded Ceramic Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Jeong-Guk; Lee, Jae-Hee; Kim, Hwan-Yong; Lee, Sung-Ho; Kim, In-Tae [Korea Atomic Energy Research Institute, Taejon (Korea, Republic of)

    2006-07-01

    The waste salts such as molten LiCl salt from an oxide fuel reduction process and molten LiCl-KCl eutectic salt from an electro refining process must meet the acceptance criteria for a disposal in geological repository. Two of the more important criteria in waste form containing chloride salts are known to be leach resistance and waste form durability. According to US Argonne National Laboratory (ANL), a ceramic waste form (CWF), which was prepared by pressureless consolidation (PC) of eutectic LiCl-KCl salt loaded zeolite (SLZ), has as a good quality as that of high level radioactive waste (HLW) glass. ANL has developed the CWF fabrication method as follows: The eutectic LiCl-KCl salt recovered from the electorefiner is size-reduced to facilitate occlusion in zeolite by crushing and grinding under an argon atmosphere. The crushed salt is mechanically mixed with dried zeolite 4A in a V-mixer at a salt loading about 10 mass % then heated to about 723 K for 16 h to occlude salt within the zeolite cages. And the SLZ is then mixed with a borosilicate binder glass in a V-mixer (without heating) at a 3:1 mass ratio. The mixture is loaded into fill cans the processed at about 1188 K for about 72 h. As the mixture is heated above about 1123 K during the encapsulating step, the SLZ converts to the mineral sodalite, Na{sub 8}(AlSiO{sub 4}){sub 6}Cl{sub 2}, which incorporates most of the occluded salt into its structure. The glass becomes sufficiently fluid during bonded sodalite material referred to as the CWF, which contains 8 mass % salt. We also developed the CWR fabrication technology for a waste LiCl salt from an electrolytic reduction process (ACP; advanced spent fuel conditioning process). A melting point of the LiCl salt is higher than that of the eutectic LiCl-KCl salt, therefore, a crystalline behavior during producing CWF is somewhat different from that of ANL. Therefore, the changes of immobilization media, which had been started from zeolite A, for the

  20. Technical area status report for low-level mixed waste final waste forms. Volume 1

    Energy Technology Data Exchange (ETDEWEB)

    Mayberry, J.L.; DeWitt, L.M. [Science Applications International Corp., Idaho Falls, ID (United States); Darnell, R. [EG and G Idaho, Inc., Idaho Falls, ID (United States)] [and others

    1993-08-01

    The Final Waste Forms (FWF) Technical Area Status Report (TASR) Working Group, the Vitrification Working Group (WG), and the Performance Standards Working Group were established as subgroups to the FWF Technical Support Group (TSG). The FWF TASR WG is comprised of technical representatives from most of the major DOE sites, the Nuclear Regulatory Commission (NRC), the EPA Office of Solid Waste, and the EPA`s Risk Reduction Engineering Laboratory (RREL). The primary activity of the FWF TASR Working Group was to investigate and report on the current status of FWFs for LLNM in this TASR. The FWF TASR Working Group determined the current status of the development of various waste forms described above by reviewing selected articles and technical reports, summarizing data, and establishing an initial set of FWF characteristics to be used in evaluating candidate FWFS; these characteristics are summarized in Section 2. After an initial review of available information, the FWF TASR Working Group chose to study the following groups of final waste forms: hydraulic cement, sulfur polymer cement, glass, ceramic, and organic binders. The organic binders included polyethylene, bitumen, vinyl ester styrene, epoxy, and urea formaldehyde. Section 3 provides a description of each final waste form. Based on the literature review, the gaps and deficiencies in information were summarized, and conclusions and recommendations were established. The information and data presented in this TASR are intended to assist the FWF Production and Assessment TSG in evaluating the Technical Task Plans (TTPs) submitted to DOE EM-50, and thus provide DOE with the necessary information for their FWF decision-making process. This FWF TASR will also assist the DOE and the MWIP in establishing the most acceptable final waste forms for the various LLMW streams stored at DOE facilities.

  1. Technical area status report for low-level mixed waste final waste forms

    International Nuclear Information System (INIS)

    The Final Waste Forms (FWF) Technical Area Status Report (TASR) Working Group, the Vitrification Working Group (WG), and the Performance Standards Working Group were established as subgroups to the FWF Technical Support Group (TSG). The FWF TASR WG is comprised of technical representatives from most of the major DOE sites, the Nuclear Regulatory Commission (NRC), the EPA Office of Solid Waste, and the EPA's Risk Reduction Engineering Laboratory (RREL). The primary activity of the FWF TASR Working Group was to investigate and report on the current status of FWFs for LLNM in this TASR. The FWF TASR Working Group determined the current status of the development of various waste forms described above by reviewing selected articles and technical reports, summarizing data, and establishing an initial set of FWF characteristics to be used in evaluating candidate FWFS; these characteristics are summarized in Section 2. After an initial review of available information, the FWF TASR Working Group chose to study the following groups of final waste forms: hydraulic cement, sulfur polymer cement, glass, ceramic, and organic binders. The organic binders included polyethylene, bitumen, vinyl ester styrene, epoxy, and urea formaldehyde. Section 3 provides a description of each final waste form. Based on the literature review, the gaps and deficiencies in information were summarized, and conclusions and recommendations were established. The information and data presented in this TASR are intended to assist the FWF Production and Assessment TSG in evaluating the Technical Task Plans (TTPs) submitted to DOE EM-50, and thus provide DOE with the necessary information for their FWF decision-making process. This FWF TASR will also assist the DOE and the MWIP in establishing the most acceptable final waste forms for the various LLMW streams stored at DOE facilities

  2. Preparation of plutonium waste forms with ICPP calcined high-level waste

    International Nuclear Information System (INIS)

    Glass and glass-ceramic forms developed for the immobilization of calcined high-level wastes generated by Idaho Chemical Processing Plant (ICPP) fuel reprocessing activities have been investigated for ability to immobilize plutonium and to simultaneously incorporate calcined waste as an anti-proliferation barrier. Within the forms investigated, crystallization of host phases result in an increased loading of plutonium as well as its incorporation into potentially more durable phases than the glass. The host phases were initially formed and characterized with cerium (Ce+4) as a surrogate for plutonium (Pu+4) and samarium as a neutron absorber for criticality control. Verification of the surrogate testing results were then performed replacing cerium with plutonium. All testing was performed with surrogate calcined high-level waste. The results of these tests indicated that a potentially useful host phase, based on zirconia, can be formed either by devitrification or solid state reaction in the glass studied. This phase incorporates plutonium as well as samarium and the calcined waste becomes part of the matrix. Its ease of formation makes it potentially useful in excess plutonium dispositioning. Other durable host phases for plutonium and samarium, including zirconolite and zircon have been formed from zirconia or alumina calcine through cold press-sintering techniques and hot isostatic pressing. Host phase formation experiments conducted through vitrification or by cold press-sintering techniques are described and the results discussed. Recommendations are given for future work that extends the results of this study

  3. Activity release from waste packages containing LL and IL waste forms under mechanical and thermal stresses

    International Nuclear Information System (INIS)

    For transport and handling of radioactive waste packages in an underground repository safety assessments are being performed to keep any unacceptable radiation hazards from the operational staff and the population in the site neighborhood. Therefore experiments were carried out to determine source terms for activity release from waste packages containing cemented waste forms in case of heavy mechanical and thermal impacts. Mechanical impact was applied by drop test with a maximum energy input of 3.105 Nm. A special cage construction around the target (reinforced concrete covered by a 80 mm steel plate) allows the collection of the airborne fines with a particle size of < 10 μm by using micro filters in a defined geometry. In addition, in two experiments the particle fraction with an aerodynamic diameter between 1 μm and 20 μm was determined using a cascade impactor. Additional laboratory experiments were performed to determine comparative values for different waste forms. In case of thermal impact, the temperature profiles in the waste forms were measured and the release of added indicators (Cs, Sr, Eu) was determined. Further laboratory experiments were performed with inactive samples to determine the temperature dependence of water release (Thermogravimetric-Analysis)

  4. Commercial high-level-waste management: options and economics. A comparative analysis of the ceramic and glass waste forms

    Energy Technology Data Exchange (ETDEWEB)

    McKisson, R.L.; Grantham, L.F.; Guon, J.; Recht, H.L.

    1983-02-25

    Results of an estimate of the waste management costs of the commercial high-level waste from a 3000 metric ton per year reprocessing plant show that the judicious use of the ceramic waste form can save about $2 billion during a 20-year operating campaign relative to the use of the glass waste form. This assumes PWR fuel is processed and the waste is encapsulated in 0.305-m-diam canisters with ultimate emplacement in a BWIP-type horizontal-borehole repository. The estimated total cost (capital and operating) of the management in the ceramic form is $2.0 billion, and that of the glass form is $4.0 billion. Waste loading and waste form density are the driving factors in that the low-waste loading (25%) and relatively low density (3.1 g/cm/sup 3/) characteristic of the glass form require several times as many canisters to handle a given waste throughput than is needed for the ceramic waste form whose waste loading capability exceeds 60% and whose waste density is nominally 5.2 g/cm/sup 3/) characteristic of the glass form requires several times as many canisters to handle a given waste throughput than is needed for the ceramic waste form whose waste loading capability exceeds 60% and whose waste density is nominally 5.2 g/cm/sup 3/. The minimum-cost ceramic waste form has a 60 wt. % waste loading of commercial high-level waste and requires 25 years storage before emplacement in basalt with delayed backfill. Because of the process flexibility allowed by the availability of the high-waste loading of the ceramic form, the intermediate-level liquid waste stream can be mixed with the high-level liquid waste stream and economically processed and emplaced. The cost is greater by $0.3 billion than that of the best high-level liquid waste handling process sequence ($2.3 billion vs $2.0 billion), but this difference is less than the cost of the separate disposal of the intermediate-level liquid waste.

  5. Commercial high-level-waste management: options and economics. A comparative analysis of the ceramic and glass waste forms

    International Nuclear Information System (INIS)

    Results of an estimate of the waste management costs of the commercial high-level waste from a 3000 metric ton per year reprocessing plant show that the judicious use of the ceramic waste form can save about $2 billion during a 20-year operating campaign relative to the use of the glass waste form. This assumes PWR fuel is processed and the waste is encapsulated in 0.305-m-diam canisters with ultimate emplacement in a BWIP-type horizontal-borehole repository. The estimated total cost (capital and operating) of the management in the ceramic form is $2.0 billion, and that of the glass form is $4.0 billion. Waste loading and waste form density are the driving factors in that the low-waste loading (25%) and relatively low density (3.1 g/cm3) characteristic of the glass form require several times as many canisters to handle a given waste throughput than is needed for the ceramic waste form whose waste loading capability exceeds 60% and whose waste density is nominally 5.2 g/cm3) characteristic of the glass form requires several times as many canisters to handle a given waste throughput than is needed for the ceramic waste form whose waste loading capability exceeds 60% and whose waste density is nominally 5.2 g/cm3. The minimum-cost ceramic waste form has a 60 wt. % waste loading of commercial high-level waste and requires 25 years storage before emplacement in basalt with delayed backfill. Because of the process flexibility allowed by the availability of the high-waste loading of the ceramic form, the intermediate-level liquid waste stream can be mixed with the high-level liquid waste stream and economically processed and emplaced. The cost is greater by $0.3 billion than that of the best high-level liquid waste handling process sequence ($2.3 billion vs $2.0 billion), but this difference is less than the cost of the separate disposal of the intermediate-level liquid waste

  6. Radiation damage studies related to nuclear waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Gray, W.J.; Wald, J.W.; Turcotte, R.P.

    1981-12-01

    Much of the previously reported work on alpha radiation effects on crystalline phases of importance to nuclear waste forms has been derived from radiation effects studies of composite waste forms. In the present work, two single-phase crystalline materials, Gd/sub 2/Ti/sub 2/O/sub 7/ (pyrochlore) and CaZrTi/sub 2/O/sub 7/ (zirconolite), of relative importance to current waste forms were studied independently by doping with /sup 244/Cm at the 3 wt % level. Changes in the crystalline structure measured by x-ray diffraction as a function of dose show that damage ingrowth follows an expected exponential relationship of the form ..delta..V/V/sub 0/ = A(1-exp(-BD)). In both cases, the materials became x-ray amorphous before the estimated saturation value was reached. The predicted magnitudes of the unit cell volume changes at saturation are 5.4% and 3.5%, respectively, for Gd/sub 2/Ti/sub 2/O/sub 7/ and CaZrTi/sub 2/O/sub 7/. The later material exhibited anisotropic behavior in which the expansion of the monoclinic cell in the c/sub 0/ direction was over five times that of the a/sub 0/ direction. The effects of transmutations on the properties of high-level waste solids have not been studied until now because of the long half-lives of the important fission products. This problem was circumvented in the present study by preparing materials containing natural cesium and then irradiating them with neutrons to produce /sup 134/Cs, which has only a 2y half-life. The properties monitored at about one year intervals following irradiation have been density, leach rate and microstructure. A small amount of x-ray diffraction work has also been done. Small changes in density and leach rate have been observed for some of the materials, but they were not large enough to be of any consequence for the final disposal of high level wastes.

  7. Modeling minor actinide multiple recycling in a lead-cooled fast reactor to demonstrate a fuel cycle without long-lived nuclear waste

    Directory of Open Access Journals (Sweden)

    Stanisz Przemysław

    2015-09-01

    Full Text Available The concept of closed nuclear fuel cycle seems to be the most promising options for the efficient usage of the nuclear energy resources. However, it can be implemented only in fast breeder reactors of the IVth generation, which are characterized by the fast neutron spectrum. The lead-cooled fast reactor (LFR was defined and studied on the level of technical design in order to demonstrate its performance and reliability within the European collaboration on ELSY (European Lead-cooled System and LEADER (Lead-cooled European Advanced Demonstration Reactor projects. It has been demonstrated that LFR meets the requirements of the closed nuclear fuel cycle, where plutonium and minor actinides (MA are recycled for reuse, thereby producing no MA waste. In this study, the most promising option was realized when entire Pu + MA material is fully recycled to produce a new batch of fuel without partitioning. This is the concept of a fuel cycle which asymptotically tends to the adiabatic equilibrium, where the concentrations of plutonium and MA at the beginning of the cycle are restored in the subsequent cycle in the combined process of fuel transmutation and cooling, removal of fission products (FPs, and admixture of depleted uranium. In this way, generation of nuclear waste containing radioactive plutonium and MA can be eliminated. The paper shows methodology applied to the LFR equilibrium fuel cycle assessment, which was developed for the Monte Carlo continuous energy burnup (MCB code, equipped with enhanced modules for material processing and fuel handling. The numerical analysis of the reactor core concerns multiple recycling and recovery of long-lived nuclides and their influence on safety parameters. The paper also presents a general concept of the novel IVth generation breeder reactor with equilibrium fuel and its future role in the management of MA.

  8. Crystalline ceramics: Waste forms for the disposal of weapons plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Ewing, R.C.; Lutze, W. [New Mexico Univ., Albuquerque, NM (United States); Weber, W.J. [Pacific Northwest Lab., Richland, WA (United States)

    1995-05-01

    At present, there are three seriously considered options for the disposition of excess weapons plutonium: (i) incorporation, partial burn-up and direct disposal of MOX-fuel; (ii) vitrification with defense waste and disposal as glass ``logs``; (iii) deep borehole disposal (National Academy of Sciences Report, 1994). The first two options provide a safeguard due to the high activity of fission products in the irradiated fuel and the defense waste. The latter option has only been examined in a preliminary manner, and the exact form of the plutonium has not been identified. In this paper, we review the potential for the immobilization of plutonium in highly durable crystalline ceramics apatite, pyrochlore, monazite and zircon. Based on available data, we propose zircon as the preferred crystalline ceramic for the permanent disposition of excess weapons plutonium.

  9. Transmission electron microscopy analysis of corroded metal waste forms.

    Energy Technology Data Exchange (ETDEWEB)

    Dietz, N. L.

    2005-04-15

    This report documents the results of analyses with transmission electron microscopy (TEM) combined with energy dispersive X-ray spectroscopy (EDS) and selected area electron diffraction (ED) of samples of metallic waste form (MWF) materials that had been subjected to various corrosion tests. The objective of the TEM analyses was to characterize the composition and microstructure of surface alteration products which, when combined with other test results, can be used to determine the matrix corrosion mechanism. The examination of test samples generated over several years has resulted in refinements to the TEM sample preparation methods developed to preserve the orientation of surface alteration layers and the underlying base metal. The preservation of microstructural spatial relationships provides valuable insight for determining the matrix corrosion mechanism and for developing models to calculate radionuclide release in repository performance models. The TEM results presented in this report show that oxide layers are formed over the exposed steel and intermetallic phases of the MWF during corrosion in aqueous solutions and humid air at elevated temperatures. An amorphous non-stoichiometric ZrO{sub 2} layer forms at the exposed surfaces of the intermetallic phases, and several nonstoichiometric Fe-O layers form over the steel phases in the MWF. These oxide layers adhere strongly to the underlying metal, and may be overlain by one or more crystalline Fe-O phases that probably precipitated from solution. The layer compositions are consistent with a corrosion mechanism of oxidative dissolution of the steel and intermetallic phases. The layers formed on the steel and intermetallic phases form a continuous layer over the exposed waste form, although vertical splits in the layer and corrosion in pits and crevices were seen in some samples. Additional tests and analyses are needed to verify that these layers passivate the underlying metals and if passivation can break

  10. Fundamental Science-Based Simulation of Nuclear Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Devanathan, Ramaswami; Gao, Fei; Sun, Xin; Khaleel, Mohammad A.

    2010-10-04

    This report presents a hierarchical multiscale modeling scheme based on two-way information exchange. To account for all essential phenomena in waste forms over geological time scales, the models have to span length scales from nanometer to kilometer and time scales from picoseconds to millenia. A single model cannot cover this wide range and a multi-scale approach that integrates a number of different at-scale models is called for. The approach outlined here involves integration of quantum mechanical calculations, classical molecular dynamics simulations, kinetic Monte Carlo and phase field methods at the mesoscale, and continuum models. The ultimate aim is to provide science-based input in the form of constitutive equations to integrated codes. The atomistic component of this scheme is demonstrated in the promising waste form xenotime. Density functional theory calculations have yielded valuable information about defect formation energies. This data can be used to develop interatomic potentials for molecular dynamics simulations of radiation damage. Potentials developed in the present work show a good match for the equilibrium lattice constants, elastic constants and thermal expansion of xenotime. In novel waste forms, such as xenotime, a considerable amount of data needed to validate the models is not available. Integration of multiscale modeling with experimental work is essential to generate missing data needed to validate the modeling scheme and the individual models. Density functional theory can also be used to fill knowledge gaps. Key challenges lie in the areas of uncertainty quantification, verification and validation, which must be performed at each level of the multiscale model and across scales. The approach used to exchange information between different levels must also be rigorously validated. The outlook for multiscale modeling of wasteforms is quite promising.

  11. Crystalline Ceramic Waste Forms: Report Detailing Data Collection In Support Of Potential FY13 Pilot Scale Melter Test

    Energy Technology Data Exchange (ETDEWEB)

    Brinkman, K. S.; Amoroso, J.; Marra, J. C.; Fox, K. M.

    2012-09-21

    The research conducted in this work package is aimed at taking advantage of the long term thermodynamic stability of crystalline ceramics to create more durable waste forms (as compared to high level waste glass) in order to reduce the reliance on engineered and natural barrier systems. Durable ceramic waste forms that incorporate a wide range of radionuclides have the potential to broaden the available disposal options and to lower the storage and disposal costs associated with advanced fuel cycles. Assemblages of several titanate phases have been successfully demonstrated to incorporate radioactive waste elements, and the multiphase nature of these materials allows them to accommodate variation in the waste composition. Recent work has shown that they can be successfully produced from a melting and crystallization process. The objective of this report is to summarize the data collection in support of future melter demonstration testing for crystalline ceramic waste forms. The waste stream used as the basis for the development and testing is a combination of the projected Cs/Sr separated stream, the Trivalent Actinide - Lanthanide Separation by Phosphorous reagent Extraction from Aqueous Komplexes (TALSPEAK) waste stream consisting of lanthanide fission products, the transition metal fission product waste stream resulting from the transuranic extraction (TRUEX) process, and a high molybdenum concentration with relatively low noble metal concentrations. The principal difficulties encountered during processing of the ?reference ceramic? waste form by a melt and crystallization process were the incomplete incorporation of Cs into the hollandite phase and the presence of secondary Cs-Mo non-durable phases. In the single phase hollandite system, these issues were addressed in this study by refining the compositions to include Cr as a transition metal element and the use of Ti/TiO{sub 2} buffer to maintain reducing conditions. Initial viscosity studies of ceramic waste

  12. Naturally occurring crystalline phases: analogues for radioactive waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Haaker, R.F.; Ewing, R.C.

    1981-01-01

    Naturally occurring mineral analogues to crystalline phases that are constituents of crystalline radioactive waste forms provide a basis for comparison by which the long-term stability of these phases may be estimated. The crystal structures and the crystal chemistry of the following natural analogues are presented: baddeleyite, hematite, nepheline; pollucite, scheelite;sodalite, spinel, apatite, monazite, uraninite, hollandite-priderite, perovskite, and zirconolite. For each phase in geochemistry, occurrence, alteration and radiation effects are described. A selected bibliography for each phase is included.

  13. Naturally occurring crystalline phases: analogues for radioactive waste forms

    International Nuclear Information System (INIS)

    Naturally occurring mineral analogues to crystalline phases that are constituents of crystalline radioactive waste forms provide a basis for comparison by which the long-term stability of these phases may be estimated. The crystal structures and the crystal chemistry of the following natural analogues are presented: baddeleyite, hematite, nepheline; pollucite, scheelite;sodalite, spinel, apatite, monazite, uraninite, hollandite-priderite, perovskite, and zirconolite. For each phase in geochemistry, occurrence, alteration and radiation effects are described. A selected bibliography for each phase is included

  14. Technical Progress Report on Single Pass Flow Through Tests of Ceramic Waste Forms for Plutonium Immobilization

    Energy Technology Data Exchange (ETDEWEB)

    Zhao, P; Roberts, S; Bourcier, W

    2000-12-01

    This report updates work on measurements of the dissolution rates of single-phase and multi-phase ceramic waste forms in flow-through reactors at Lawrence Livermore National Laboratory. Previous results were reported in Bourcier (1999). Two types of tests are in progress: (1) tests of baseline pyrochlore-based multiphase ceramics; and (2) tests of single-phase pyrochlore, zirconolite, and brannerite (the three phases that will contain most of the actinides). Tests of the multi-phase material are all being run at 25 C. The single-phase tests are being run at 25, 50, and 75 C. All tests are being performed at ambient pressure. The as-made bulk compositions of the ceramics are given in Table 1. The single pass flow-through test procedure [Knauss, 1986 No.140] allows the powdered ceramic to react with pH buffer solutions traveling upward vertically through the powder. Gentle rocking during the course of the experiment keeps the powder suspended and avoids clumping, and allows the system to behave as a continuously stirred reactor. For each test, a cell is loaded with approximately one gram of the appropriate size fraction of powdered ceramic and reacted with a buffer solution of the desired pH. The buffer solution compositions are given in Table 2. All the ceramics tested were cold pressed and sintered at 1350 C in air, except brannerite, which was sintered at 1350 C in a CO/CO{sub 2} gas mixture. They were then crushed, sieved, rinsed repeatedly in alcohol and distilled water, and the desired particle size fraction collected for the single pass flow-through tests (SPFT). The surface area of the ceramics measured by BET ranged from 0.1-0.35 m{sup 2}/g. The measured surface area values, average particle size, and sample weights for each ceramic test are given in the Appendices.

  15. Engineering-Scale Demonstration of DuraLith and Ceramicrete Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Josephson, Gary B.; Westsik, Joseph H.; Pires, Richard P.; Bickford, Jody; Foote, Martin W.

    2011-09-23

    To support the selection of a waste form for the liquid secondary wastes from the Hanford Waste Immobilization and Treatment Plant, Washington River Protection Solutions (WRPS) has initiated secondary waste form testing on four candidate waste forms. Two of the candidate waste forms have not been developed to scale as the more mature waste forms. This work describes engineering-scale demonstrations conducted on Ceramicrete and DuraLith candidate waste forms. Both candidate waste forms were successfully demonstrated at an engineering scale. A preliminary conceptual design could be prepared for full-scale production of the candidate waste forms. However, both waste forms are still too immature to support a detailed design. Formulations for each candidate waste form need to be developed so that the material has a longer working time after mixing the liquid and solid constituents together. Formulations optimized based on previous lab studies did not have sufficient working time to support large-scale testing. The engineering-scale testing was successfully completed using modified formulations. Further lab development and parametric studies are needed to optimize formulations with adequate working time and assess the effects of changes in raw materials and process parameters on the final product performance. Studies on effects of mixing intensity on the initial set time of the waste forms are also needed.

  16. Garnet nuclear waste forms – Solubility at repository conditions

    Energy Technology Data Exchange (ETDEWEB)

    Caporuscio, F.A., E-mail: floriec@lanl.gov [EES-14, Los Alamos National Laboratory, NM 87545 (United States); Scott, B.L. [MPA-MSID, Los Alamos National Laboratory, NM 87545 (United States); Xu, H. [EES-14, Los Alamos National Laboratory, NM 87545 (United States); Feller, R.K. [Effect Materials Research Group, BASF Corporation, 500 White Plains Road, Tarrytown, NY 10591 (United States)

    2014-01-15

    Highlights: • Rare-earth elements are a significant waste stream produced by nuclear fuel cycles. • Suitability of garnets as potential waste forms. • Single-crystal X-ray structural refinements for grossular, LuAG and YAG. • Garnets have low solubility, flexible crystal structure to take on large cations. • Demonstrate garnets are potentially robust waste forms for radioactive REE. -- Abstract: Radioactive rare-earth elements (REEs) constitute a significant waste stream produced from modified open and full nuclear fuel cycles. Immobilization of these REE radionuclides is thus important for sustainable nuclear energy growth. In this work, we investigated the suitability of garnets as potential waste forms for REEs by measuring their aqueous stability at repository conditions. Three garnet samples, including one natural grossular (Ca{sub 3}Al{sub 2}Si{sub 3}O{sub 12}) and two synthetic phases (LuAG – Lu{sub 3}Al{sub 5}O{sub 12} and YAG – Y{sub 3}Al{sub 5}O{sub 12}), were studied. Single-crystal X-ray structural refinements show that the unit-cell volumes increase from 1657.19 Å{sup 3} for grossular to 1679.8 Å{sup 3} for LuAG and to 1721.7 Å{sup 3} for YAG. This trend is due to increases in ionic radii in both the 8-coordinated X (from Ca to Lu to Y) and 4-coordinated Z (from Si to Al) cations. Hydrothermal experiments of the three samples were performed at 200 °C and 150 bar for 4 weeks using water and brine solutions to evaluate their solubility. The natural grossular sample exhibited Al leach rates ranging from 2.5 × 10{sup −4} to 6.43 × 10{sup −5} g/L·day and Ca leach rates from 1.39 × 10{sup −3} to 4.57 × 10{sup −3} g/L·day, indicating incongruent nature of the cation dissolution. The LuAG sample exhibited Lu leach rates of 3.73 × 10{sup −4} to 2.19 × 10{sup −4} g/L·day, and the YAG sample had Y leach rates of 1.29 × 10{sup −4} to 5.64 × 10{sup −5} g/L·day. Although these samples are generally more soluble in

  17. Proposed research and development plan for mixed low-level waste forms

    International Nuclear Information System (INIS)

    The objective of this report is to recommend a waste form program plan that addresses waste form issues for mixed low-level waste (MLLW). The report compares the suitability of proposed waste forms for immobilizing MLLW in preparation for permanent near-surface disposal and relates them to their impact on the U.S. Department of Energy's mixed waste mission. Waste forms are classified into four categories: high-temperature waste forms, hydraulic cements, encapsulants, and specialty waste forms. Waste forms are evaluated concerning their ability to immobilize MLLW under certain test conditions established by regulatory agencies and research institutions. The tests focused mainly on leach rate and compressive strength. Results indicate that all of the waste forms considered can be tailored to give satisfactory performance immobilizing large fractions of the Department's MLLW inventory. Final waste form selection will ultimately be determined by the interaction of other, often nontechnical factors, such as economics and politics. As a result of this report, three top-level programmatic needs have been identified: (1) a basic set of requirements for waste package performance and disposal; (2) standardized tests for determining waste form performance and suitability for disposal; and (3) engineering experience operating production-scale treatment and disposal systems for MLLW

  18. Proposed research and development plan for mixed low-level waste forms

    Energy Technology Data Exchange (ETDEWEB)

    O`Holleran, T.O.; Feng, X.; Kalb, P. [and others

    1996-12-01

    The objective of this report is to recommend a waste form program plan that addresses waste form issues for mixed low-level waste (MLLW). The report compares the suitability of proposed waste forms for immobilizing MLLW in preparation for permanent near-surface disposal and relates them to their impact on the U.S. Department of Energy`s mixed waste mission. Waste forms are classified into four categories: high-temperature waste forms, hydraulic cements, encapsulants, and specialty waste forms. Waste forms are evaluated concerning their ability to immobilize MLLW under certain test conditions established by regulatory agencies and research institutions. The tests focused mainly on leach rate and compressive strength. Results indicate that all of the waste forms considered can be tailored to give satisfactory performance immobilizing large fractions of the Department`s MLLW inventory. Final waste form selection will ultimately be determined by the interaction of other, often nontechnical factors, such as economics and politics. As a result of this report, three top-level programmatic needs have been identified: (1) a basic set of requirements for waste package performance and disposal; (2) standardized tests for determining waste form performance and suitability for disposal; and (3) engineering experience operating production-scale treatment and disposal systems for MLLW.

  19. Description of DWPF reference waste form and canister

    International Nuclear Information System (INIS)

    This document describes the reference waste form and canister for the Defense Waste Processing Facility (DWPF). The facility is planned for location at the Savannah River Plant in Aiken, SC, and is scheduled for construction authorization during FY-1983. The reference canister is fabricated of 24-in.-OD 304L stainless steel pipe with a dished bottom, domed head, and lifting and welding flanges on the head neck. The overall canister length is 9 ft 10 in., with a wall thickness of 3/8-in. (schedule 20 pipe). The canister length was selected to reduce equipment cell height in the DWPF to a practical size. The canister diameter was selected to ensure that a filled canister with its shipping cask could be accommodated on a legal-weight truck. The overall dimensions and weight appear to be generally compatible with preliminary assessments of repository requireiajps. The rabarajca saspa bkri is bkrksilicapa class cojtaining approximately 28 wt % sludge oxides with the balance glass frit. Borosilicate glass was chosen because of its high resistance to leaching by water, its relatively high solubility for nuclides found in the sludge, and its reasonably low melting temperature. The glass frit contains approximately 58% SiO2 and 15% B2O3. This composition results in a low average leachability in the waste form of approximately 5 x 10-9 g/cm2-day based on 137Cs over 365 days in 250C water. The canister is filled with 3260 lb of glass which occupies about 85% of the free canister volume. The filled canister will generate approximately 425 watts when filled with oxides from 5-year-old sludge and 15-year-old supernate from the Stage 1 and Stage 2 processes. The radionuclide content of the canister is about 150,000 curies, with a radiation level of 2 x 104 rem/hour at 1 cm

  20. Stability of High-Level Radioactive Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Besmann, T.M.

    2001-06-22

    High-level waste (HLW) glass compositions, processing schemes, limits on waste content, and corrosion/dissolution release models are dependent on an accurate knowledge of melting temperatures and thermochemical values. Unfortunately, existing models for predicting these temperatures are empirically-based, depending on extrapolations of experimental information. In addition, present models of leaching behavior of glass waste forms use simplistic assumptions or experimentally measured values obtained under non-realistic conditions. There is thus a critical need for both more accurate and more widely applicable models for HLW glass behavior, which this project addressed. Significant progress was made in this project on modeling HLW glass. Borosilicate glass was accurately represented along with the additional important components that contain iron, lithium, potassium, magnesium, and calcium. The formation of crystalline inclusions in the glass, an issue in Hanford HLW formulations, was modeled and shown to be predictive. Thus the results of this work have already demonstrated practical benefits with the ability to map compositional regions where crystalline material forms, and therefore avoid that detrimental effect. With regard to a fundamental understanding, added insights on the behavior of the components of glass have been obtained, including the potential formation of molecular clusters. The EMSP project had very significant effects beyond the confines of Environmental Management. The models developed for glass have been used to solve a very costly problem in the corrosion of refractories for glass production. The effort resulted in another laboratory, Sandia National Laboratories-Livermore, to become conversant in the techniques and to apply those through a DOE Office of Industrial Technologies project joint with PPG Industries. The glass industry as a whole is now cognizant of these capabilities, and there is a Glass Manufacturer's Research Institute

  1. 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

  2. Material Recovery and Waste Form Development FY 2015 Accomplishments Report

    Energy Technology Data Exchange (ETDEWEB)

    Todd, Terry Allen [Idaho National Lab. (INL), Idaho Falls, ID (United States); Braase, Lori Ann [Idaho National Lab. (INL), Idaho Falls, ID (United States)

    2015-11-01

    The Material Recovery and Waste Form Development (MRWFD) Campaign under the U.S. Department of Energy (DOE) Fuel Cycle Technologies (FCT) Program is responsible for developing advanced separation and waste form technologies to support the various fuel cycle options defined in the DOE Nuclear Energy Research and Development Roadmap, Report to Congress, April 2010. The FY 2015 Accomplishments Report provides a highlight of the results of the research and development (R&D) efforts performed within the MRWFD Campaign in FY-14. Each section contains a high-level overview of the activities, results, technical point of contact, applicable references, and documents produced during the fiscal year. This report briefly outlines campaign management and integration activities, but primarily focuses on the many technical accomplishments made during FY-15. The campaign continued to utilize an engineering driven-science-based approach to maintain relevance and focus. There was increased emphasis on development of technologies that support near-term applications that are relevant to the current once-through fuel cycle.

  3. DuraLith geopolymer waste form for Hanford secondary waste: Correlating setting behavior to hydration heat evolution

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Hui; Gong, Weiliang, E-mail: gongw@vsl.cua.edu; Syltebo, Larry; Lutze, Werner; Pegg, Ian L.

    2014-08-15

    Highlights: • Quantitative correlations firstly established for cementitious waste forms. • Quantitative correlations firstly established for geopolymeric materials. • Ternary DuraLith geopolymer waste forms for Hanford radioactive wastes. • Extended setting times which improve workability for geopolymer waste forms. • Reduced hydration heat release from DuraLith geopolymer waste forms. - Abstract: The binary furnace slag-metakaolin DuraLith geopolymer waste form, which has been considered as one of the candidate waste forms for immobilization of certain Hanford secondary wastes (HSW) from the vitrification of nuclear wastes at the Hanford Site, Washington, was extended to a ternary fly ash-furnace slag-metakaolin system to improve workability, reduce hydration heat, and evaluate high HSW waste loading. A concentrated HSW simulant, consisting of more than 20 chemicals with a sodium concentration of 5 mol/L, was employed to prepare the alkaline activating solution. Fly ash was incorporated at up to 60 wt% into the binder materials, whereas metakaolin was kept constant at 26 wt%. The fresh waste form pastes were subjected to isothermal calorimetry and setting time measurement, and the cured samples were further characterized by compressive strength and TCLP leach tests. This study has firstly established quantitative linear relationships between both initial and final setting times and hydration heat, which were never discovered in scientific literature for any cementitious waste form or geopolymeric material. The successful establishment of the correlations between setting times and hydration heat may make it possible to efficiently design and optimize cementitious waste forms and industrial wastes based geopolymers using limited testing results.

  4. 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.

  5. 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.

  6. 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

  7. 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.

  8. Wet oxidative degradation of cellulosic wastes 5- chemical and thermal properties of the final waste forms

    International Nuclear Information System (INIS)

    In this study, the residual solution arising from the wet oxidative degradation of solid organic cellulosic materials, as one of the component of radioactive solid wastes, using hydrogen peroxide as oxidant. Were incorporated into ordinary Portland cement matrix. Leaching as well as thermal characterizations of the final solidified waste forms were evaluated to meet the final disposal requirements. Factors, such as the amount of the residual solution incorporated, types of leachant. Release of different radionuclides and freezing-thaw treatment, that may affect the leaching characterization. Were studied systematically from the data obtained, it was found that the final solid waste from containing 35% residual solution in tap water is higher than that in ground water or sea water. Based on the data obtained from thermal analysis, it could be concluded that incorporating the residual solution form the wet oxidative degradation of cellulosic materials has no negative effect on the hydration of cement materials and consequently on the thermal stability of the final solid waste from during the disposal process

  9. Reference waste form, basalts, and ground water systems for waste interaction studies

    Energy Technology Data Exchange (ETDEWEB)

    Deju, R.A.; Ledgerwood, R.K.; Long, P.E.

    1978-09-01

    This report summarizes the type of waste form, basalt, and ground water compositions to be used in theoretical and experimental models of the geochemical environment to be simulated in studying a typical basalt repository. Waste forms to be used in the experiments include, and are limited to, glass, supercalcine, and spent unreprocessed fuel. Reference basalts selected for study include the Pomona member and the Umtanum Unit, Shwana Member, of the Columbia River Basalt Group. In addition, a sample of the Basalt International Geochemical Standard (BCR-1) will be used for cross-comparison purposes. The representative water to be used is of a sodium bicarbonate composition as determined from results of analyses of deep ground waters underlying the Hanford Site. 12 figures, 13 tables.

  10. 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

  11. Silica based gel as a potential waste form for high level waste from fuel reprocessing

    International Nuclear Information System (INIS)

    To assess the feasibility of safe disposal of high-level radioactive waste as synthetic clay, or material that would react with ground water to form clay, experiments have been carried out to determine the hydrothermal crystallisation and leaching behaviour of silica based gels fired at 900 deg C. Crystallisation rates at a pressure of 500 bars and at temperatures below 400 deg C are negligible and this more or less precludes pre-disposal production of synthetic clay on the scale required. Leaching experiments suggest that the leach rates of Cs from gels by distilled water are higher than those of boro-silicate glasses and SYNROC at the lower temperatures that would be preferred for geological storage. However, amounts of bulk dissolution of gels may be lower than those of boro-silicate glasses. The initial leaching behaviour of gels might be considerably improved by hot compaction at 900 to 1000 deg C. Consideration of likely waste form dissolution behaviour in a repository environment suggests that gels of appropriate composition might perform as well as, or better than, boro-silicate glasses. A novel hypothetical plant is described that could produce the gel waste form on the scale required on a more or less continuous basis. (author)

  12. Simultaneous photon and neutron interrogation using an electron accelerator in order to quantify actinides in encapsulated radioactive wastes

    International Nuclear Information System (INIS)

    Measuring out alpha emitters, such as (234,235,236,238U 238,239,240,242,244Pu, 237Np 241,243Am...), in solid radioactive waste, allows us to quantify the alpha activity in a drum and then to classify it. The SIMPHONIE (SIMultaneous PHOton and Neutron Interrogation Experiment) method, developed in this Ph.D. work, combines both the Active Neutron Interrogation and the Induced Photofission Interrogation techniques simultaneously. Its purpose is to quantify in only one measurement, fissile (235U, 239,241Pu...) and fertile (236,238U, 238,240Pu...) elements separately. In the first chapter of this Ph.D. report, we present the principle of the Radioactive Waste Management in France. The second chapter deals with the physical properties of neutron fission and of photofission. These two nuclear reactions are the basis of the SIMPHONIE method. Moreover, one of our purposes was to develop the ELEPHANT (ELEctron PHoton And Neutron Transport) code in view to simulate the electron, photon and neutron transport, including the (γ, n), (γ, 2n) and (γ, f) photonuclear reactions that are not taken into account in the MCNP4 (Monte Carlo N-Particle) code. The simulation codes developed and used in this work are detailed in the third chapter. Finally, the fourth chapter gives the experimental results of SIMPHONIE obtained by using the DGA/ETCA electron linear accelerators located at Arcueil, France. Fissile (235U, 239Pu) and fertile (238U) samples were studied. Furthermore, comparisons between experimental results and calculated data of photoneutron production in tungsten, copper, praseodymium and beryllium by using an electron LINear Accelerator (LINAC) are given. This allows us to evaluate the validity degree of the ELEPHANT code, and finally the feasibility of the SIMPHONIE method. (author)

  13. Effects of aqueous environment on long-term durability of phosphate-bonded ceramic waste forms

    International Nuclear Information System (INIS)

    Over the last few years, Argonne National Laboratory has been developing room-temperature-setting chemically-bonded phosphate ceramics for solidifying and stabilizing low-level mixed wastes. This technology is crucial for stabilizing waste streams that contain volatile species and off-gas secondary waste streams generated by high-temperature treatment of such wastes. Magnesium phosphate ceramic has been developed to treat mixed wastes such as ash, salts, and cement sludges. Waste forms of surrogate waste streams were fabricated by acid-base reactions between the mixtures of magnesium oxide powders and the wastes, and phosphoric acid or acid phosphate solutions. Dense and hard ceramic waste forms are produced in this process. The principal advantage of this technology is that the contaminants are immobilized by both chemical stabilization and subsequent microencapsulation of the reaction products. This paper reports the results of durability studies conducted on waste forms made with ash waste streams spiked with hazardous and radioactive surrogates. Standard leaching tests such as ANS 16.1 and TCLP were conducted on the final waste forms. Fates of the contaminants in the final waste forms were established by electron microscopy. In addition, stability of the waste forms in aqueous environments was evaluated with long-term water-immersion tests

  14. Development of Polymeric Waste Forms for the Encapsulation of Toxic Wastes Using an Emulsion-Encapsulation Based Process

    Energy Technology Data Exchange (ETDEWEB)

    Evans, R.; Quach, A.; Birnie, D. P.; Saez, A. E.; Ela, W. P.; Zeliniski, B. J. J.; Xia, G.; Smith, H.

    2003-01-01

    Developed technologies in vitrification, cement, and polymeric materials manufactured using flammable organic solvents have been used to encapsulate solid wastes, including low-level radioactive materials, but are impractical for high salt-content waste streams (Maio, 1998). In this work, we investigate an emulsification process for producing an aqueous-based polymeric waste form as a preliminary step towards fabricating hybrid organic/inorganic polyceram matrices. The material developed incorporates epoxy resin and polystyrene-butadiene (PSB) latex to produce a waste form that is non-flammable, light weight, of relatively low cost, and that can be loaded to a relatively high weight content of waste materials. Sodium nitrate was used as a model for the salt waste. Small-scale samples were manufactured and analyzed using leach tests designed to measure the diffusion coefficient and leachability index for the fastest diffusing species in the waste form, the salt ions. The microstructure and composition of the samples were probed using SEM/EDS techniques. The results show that some portion of the salt migrates towards the exterior surfaces of the waste forms during the curing process. A portion of the salt in the interior of the sample is contained in polymer corpuscles or sacs. These sacs are embedded in a polymer matrix phase that contains fine, well-dispersed salt crystals. The diffusion behavior observed in sections of the waste forms indicates that samples prepared using this emulsion process meet or exceed the leachability criteria suggested for low level radioactivity waste forms.

  15. Impeding 99Tc(IV) mobility in novel waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Mal Soon; Um, Wooyong; Wang, Guohui; Kruger, Albert A.; Lukens, Wayne W.; Rousseau, Roger J.; Glezakou, Vassiliki Alexandra

    2016-06-30

    Technetium (99Tc) is a long-lived radioactive fission product whose mobility in the subsurface is largely governed by its oxidation state1. Immobilization of Tc in mineral substrates is crucial for radioactive waste management and environmental remediation. Tc(IV) incorporation in spinels2, 3 has been proposed as a novel method to increase Tc retention in glass waste forms. However, experiments with Tc-magnetite under high temperature and oxic conditions showed re-oxidation of Tc(IV) to volatile pertechnetate Tc(VII)O4-.4, 5 Here we address this problem with large-scale ab initio molecular dynamics simulations and propose that elevated temperatures, 1st row transition metal dopants can significantly enhance Tc retention in the order Co > Zn > Ni. Experiments with doped spinels at T=700 ºC provided quantitative confirmation of increased Tc retention in the same order predicted by theory. This work highlights the power of modern state-of-the-art simulations to provide essential insights and generate bottom-up design criteria of complex oxide materials at elevated temperatures.

  16. Impeding 99Tc(IV) mobility in novel waste forms

    Science.gov (United States)

    Lee, Mal-Soon; Um, Wooyong; Wang, Guohui; Kruger, Albert A.; Lukens, Wayne W.; Rousseau, Roger; Glezakou, Vassiliki-Alexandra

    2016-06-01

    Technetium (99Tc) is an abundant, long-lived radioactive fission product whose mobility in the subsurface is largely governed by its oxidation state. Tc immobilization is crucial for radioactive waste management and environmental remediation. Tc(IV) incorporation in spinels has been proposed as a novel method to increase Tc retention in glass waste forms during vitrification. However, experiments under high-temperature and oxic conditions show reoxidation of Tc(IV) to volatile pertechnetate, Tc(VII). Here we examine this problem with ab initio molecular dynamics simulations and propose that, at elevated temperatures, doping with first row transition metal can significantly enhance Tc retention in magnetite in the order Co>Zn>Ni. Experiments with doped spinels at 700 °C provide quantitative confirmation of the theoretical predictions in the same order. This work highlights the power of modern, state-of-the-art simulations to provide essential insights and generate theory-inspired design criteria of complex materials at elevated temperatures.

  17. Impeding (99)Tc(IV) mobility in novel waste forms.

    Science.gov (United States)

    Lee, Mal-Soon; Um, Wooyong; Wang, Guohui; Kruger, Albert A; Lukens, Wayne W; Rousseau, Roger; Glezakou, Vassiliki-Alexandra

    2016-01-01

    Technetium ((99)Tc) is an abundant, long-lived radioactive fission product whose mobility in the subsurface is largely governed by its oxidation state. Tc immobilization is crucial for radioactive waste management and environmental remediation. Tc(IV) incorporation in spinels has been proposed as a novel method to increase Tc retention in glass waste forms during vitrification. However, experiments under high-temperature and oxic conditions show reoxidation of Tc(IV) to volatile pertechnetate, Tc(VII). Here we examine this problem with ab initio molecular dynamics simulations and propose that, at elevated temperatures, doping with first row transition metal can significantly enhance Tc retention in magnetite in the order Co>Zn>Ni. Experiments with doped spinels at 700 °C provide quantitative confirmation of the theoretical predictions in the same order. This work highlights the power of modern, state-of-the-art simulations to provide essential insights and generate theory-inspired design criteria of complex materials at elevated temperatures. PMID:27357121

  18. Impeding 99Tc(IV) mobility in novel waste forms

    Science.gov (United States)

    Lee, Mal-Soon; Um, Wooyong; Wang, Guohui; Kruger, Albert A.; Lukens, Wayne W.; Rousseau, Roger; Glezakou, Vassiliki-Alexandra

    2016-01-01

    Technetium (99Tc) is an abundant, long-lived radioactive fission product whose mobility in the subsurface is largely governed by its oxidation state. Tc immobilization is crucial for radioactive waste management and environmental remediation. Tc(IV) incorporation in spinels has been proposed as a novel method to increase Tc retention in glass waste forms during vitrification. However, experiments under high-temperature and oxic conditions show reoxidation of Tc(IV) to volatile pertechnetate, Tc(VII). Here we examine this problem with ab initio molecular dynamics simulations and propose that, at elevated temperatures, doping with first row transition metal can significantly enhance Tc retention in magnetite in the order Co>Zn>Ni. Experiments with doped spinels at 700 °C provide quantitative confirmation of the theoretical predictions in the same order. This work highlights the power of modern, state-of-the-art simulations to provide essential insights and generate theory-inspired design criteria of complex materials at elevated temperatures. PMID:27357121

  19. Alternative Electrochemical Salt Waste Forms, Summary of FY2010 Results

    Energy Technology Data Exchange (ETDEWEB)

    Riley, Brian J.; Rieck, Bennett T.; Crum, Jarrod V.; Matyas, Josef; McCloy, John S.; Sundaram, S. K.; Vienna, John D.

    2010-08-01

    In FY2009, PNNL performed scoping studies to qualify two waste form candidates, tellurite (TeO2-based) glasses and halide minerals, for the electrochemical waste stream for further investigation. Both candidates showed promise with acceptable PCT release rates and effective incorporation of the 10% fission product waste stream. Both candidates received reprisal for FY2010 and were further investigated. At the beginning of FY2010, an in-depth literature review kicked off the tellurite glasses study. The review was aimed at ascertaining the state-of-the-art for chemical durability testing and mixed chloride incorporation for tellurite glasses. The literature review led the authors to 4 unique binary and 1 unique ternary systems for further investigation which include TeO2 plus the following: PbO, Al2O3-B2O3, WO3, P2O5, and ZnO. Each system was studied with and without a mixed chloride simulated electrochemical waste stream and the literature review provided the starting points for the baseline compositions as well as starting points for melting temperature, compatible crucible types, etc. The most promising glasses in each system were scaled up in production and were analyzed with the Product Consistency Test, a chemical durability test. Baseline and PCT glasses were analyzed to determine their state, i.e., amorphous, crystalline, phase separated, had undissolved material within the bulk, etc. Conclusions were made as well as the proposed direction for FY2011 plans. Sodalite was successfully synthesized by the sol-gel method. The vast majority of the dried sol-gel consisted of sodalite with small amounts of alumino-silicates and unreacted salt. Upon firing the powders made by sol-gel, the primary phase observed was sodalite with the addition of varying amounts of nepheline, carnegieite, lithium silicate, and lanthanide oxide. The amount of sodalite, nepheline, and carnegieite as well as the bulk density of the fired pellets varied with firing temperature, sol

  20. Waste form characteristics report, revision 1.3

    Energy Technology Data Exchange (ETDEWEB)

    Leider, H.R.; Stout, R.B.

    1998-07-01

    This Waste Form Characteristics Report (WFCR) update, Version 1.3, incorporates substantial additions and changes to following 10 sections of the WFCR: 2.1.3.1 Cladding Degradation; 2.1.3.2 UO2 Oxidation in Fuel; 2.1.3.5 Dissolution Release from UO{sub 2}; 2.2.1.5 Fracture /Fragmentation Studies of Glass; 2.2.2.2 Dissolution Radionuclide Release from Glass; 2.2.2.3 Soluble-Precipitated/Colloidal Species from Glass; 3.2.2 Spent-Fuel Oxidation Models; 3.4.2 Spent-Fuel Dissolution Models; 3.5.1 Glass Dissolution Experimental Parameters; and 3.5.2 Glass Dissolution Models.

  1. Microscopic characterization of crystalline phases in waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Buck, E.C.; Dietz, N.L.; Wronkiewicz, D.J.; Bates, J.K. [Argonne National Lab., IL (United States); Millar, A. [Purdue Univ., West Lafayette, IN (United States)

    1995-07-01

    Transmission electron microscopy (TEM) has been used to determine the microstructure of crystalline phases present in zirconium- and titanium-bearing glass crystalline composite (GCC) waste forms. The GCC materials were found to contain spinels (maghemite), zirconolites, perovskites (CaTiO{sub 3}) and plagiociase feldspar (anorthite) mineral phases. The structure of the uranium and cerium-bearing monoclinic zirconolite was characterized by medium resolution TEM imaging and electron and X-ray diffraction (XRD). The phase was found to contain high levels of iron in comparison to Synroc-type zirconolites. Excess zirconium in zirconolite has resulted in martensitic baddeleyite (ZrO{sub 2}) formation. Anorthite (CaAl{sub 2}Si{sub 2}O{sub 8}) was present as elongated crystallites within a calcium-rich aluminosilicate glass. Lead and iron-bearing anorthite lying along distinct precipitates were occasionally observed within the an crystallographic planes.

  2. Progress in forming bottom barriers under waste sites

    Energy Technology Data Exchange (ETDEWEB)

    Carter, E.E. [Carter Technologies, Sugar Land, TX (United States)

    1997-12-31

    The paper describes an new method for the construction, verification, and maintenance of underground vaults to isolate and contain radioactive burial sites without excavation or drilling in contaminated areas. The paper begins with a discussion of previous full-scale field tests of horizontal barrier tools which utilized high pressure jetting technology. This is followed by a discussion of the TECT process, which cuts with an abrasive cable instead of high pressure jets. The new method is potentially applicable to more soil types than previous methods and can form very thick barriers. Both processes are performed from the perimeter of a site and require no penetration or disturbance of the active waste area. The paper also describes long-term verification methods to monitor barrier integrity passively.

  3. Radionuclide Incorporation and Long Term Performance of Apatite Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Jianwei [Louisiana State Univ., Baton Rouge, LA (United States); Lian, Jie [Rensselaer Polytechnic Inst., Troy, NY (United States); Gao, Fei [Univ. of Michigan, Ann Arbor, MI (United States)

    2016-01-04

    This project aims to combines state-of-the-art experimental and characterization techniques with atomistic simulations based on density functional theory (DFT) and molecular dynamics (MD) simulations. With an initial focus on long-lived I-129 and other radionuclides such as Cs, Sr in apatite structure, specific research objectives include the atomic scale understanding of: (1) incorporation behavior of the radionuclides and their effects on the crystal chemistry and phase stability; (2) stability and microstructure evolution of designed waste forms under coupled temperature and radiation environments; (3) incorporation and migration energetics of radionuclides and release behaviors as probed by DFT and molecular dynamics (MD) simulations; and (4) chemical durability as measured in dissolution experiments for long term performance evaluation and model validation.

  4. 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

  5. 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.

  6. 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

  7. Material Recovery and Waste Form Development FY 2014 Accomplishments Report

    Energy Technology Data Exchange (ETDEWEB)

    Lori Braase

    2014-11-01

    Develop advanced nuclear fuel cycle separation and waste management technologies that improve current fuel cycle performance and enable a sustainable fuel cycle, with minimal processing, waste generation, and potential for material diversion.

  8. Radiation and Thermal Effects on Used Nuclear Fuel and Nuclear Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Weber, William [Univ. of Tennessee, Knoxville, TN (United States)

    2016-09-20

    disordered defect-fluorite crystalline structure in Gd2Zr2O7, which are the phase-transformed structures that will form due to selfNEUP 12-3528 Final Report iv irradiation from alpha-decay during interim storage; consequently, it is these structures that are of interest and concern for long-term evaluation. These phase-transformed materials were implanted with helium ions to fluences equivalent to peak helium concentrations 0.1, 1.0 and 12 at% helium, which correspond to expected helium concentrations at 1000, 100,000 and over 1 million years, respectively, for a waste form containing 25 wt.% 239Pu. Some of these helium implanted samples were further irradiated to simulate the response of the amorphous and disordered fluorite structures to radiation damage processes from alpha decay during long-term immobilization in a geologic repository. The combined irradiation dose (12 dpa) in these samples corresponds to 3,000 years of storage for a waste form containing 25 wt% 239Pu, 10,000 years for a waste form containing 10 wt% 239Pu, 25,000 years of storage for a waste form containing 5 wt% minor actinides, and 1 million years of storage for a waste form containing 25 wt% loading of commercial high-level nuclear waste. Helium bubbles did not formed under any conditions for samples containing 0.1 or 1.0 at% helium, even after irradiations at 700 K. However, in the case of Gd2Ti2O7 and Gd2Zr2O7 samples implanted with a peak helium concentration of 12 at%, helium bubbles with diameters of 1 to 3 nm were observed in both materials. The critical helium concentration for bubble formation in amorphous Gd2Ti2O7 was determined to be about 6 at% helium, while in the defect-fluorite Gd2Zr2O7 the critical concentration is 4.6 at% helium. In amorphous Gd2Ti2O7, helium

  9. MODELING SOLIDIFICATION-INDUCED STRESSES IN CERAMIC WASTE FORMS CONTAINING NUCLEAR WASTES

    Energy Technology Data Exchange (ETDEWEB)

    Charles W. Solbrig; Kenneth J. Bateman

    2010-11-01

    The goal of this work is to produce a ceramic waste form (CWF) that permanently occludes radioactive waste. This is accomplished by absorbing radioactive salts into zeolite, mixing with glass frit, heating to a molten state 915 C to form a sodalite glass matrix, and solidifying for long-term storage. Less long term leaching is expected if the solidifying cooling rate doesn’t cause cracking. In addition to thermal stress, this paper proposes that a stress is formed during solidification which is very large for fast cooling rates during solidification and can cause severe cracking. A solidifying glass or ceramic cylinder forms a dome on the cylinder top end. The temperature distribution at the time of solidification causes the stress and the dome. The dome height, “the length deficit,” produces an axial stress when the solid returns to room temperature with the inherent outer region in compression, the inner in tension. Large tensions will cause cracking of the specimen. The temperature deficit, derived by dividing the length deficit by the coefficient of thermal expansion, allows solidification stress theory to be extended to the circumferential stress. This paper derives the solidification stress theory, gives examples, explains how to induce beneficial stresses, and compares theory to experimental data.

  10. Immobilization of fission products in phosphate ceramic waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Singh, D. [Argonne National Lab., IL (United States)

    1996-10-01

    The goal of this project is to develop and demonstrate the feasibility of a novel low-temperature solidification/stabilization (S/S) technology for immobilizing waste streams containing fission products such as cesium, strontium, and technetium in a chemically bonded phosphate ceramic. This technology can immobilize partitioned tank wastes and decontaminate waste streams containing volatile fission products.

  11. Naturally occurring glasses: analogues for radioactive waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Ewing, R.C.; Haaker, R.F.

    1979-04-01

    Volcanic glasses are very often altered by weathering and leaching and recrystallize to their fine-grained equivalents (rhyolites, felsites). The oldest volcanic glasses are dated at 40 million years before the present, but the majority are much younger. Devitrification textures was produced experimentally; and hydration rates for volcanic glasses were determined as a function of composition, temperature, and climate. Presence of water and temperature are the most important rate controlling variables. Even material that may still be described as glassy often exhibits evidence of alteration and recrystallization. Of the volcanic glasses that are preserved in the geologic record, it would be rare to describe such a glass as pristine. Despite the common alteration and recrystallization effects observed in volcanic glasses, glasses formed as a result of impact, tektites and lunar glasses, may occur in substantially unaltered form. In the case of tektites, their resistance to alteration is a result of their high SiO/sub 2/ content and low alkali content. Lunar glasses have been preserved for hundreds of millions of years because they exist in an environment with a low oxygen fugacity and an extremely low water vapor partial presssure. Thus one might expect glasses of particular compositions or in specific types of environment to be stable for long periods of time. These conclusions are applied to radioactive waste disposal over several time periods (0-30h, 30h-20y, 20-200y).

  12. Hanford Waste Vitrification Plant Quality Assurance Program description for high-level waste form development and qualification

    International Nuclear Information System (INIS)

    The Hanford Waste Vitrification Plant Project has been established to convert the high-level radioactive waste associated with nuclear defense production at the Hanford Site into a waste form suitable for disposal in a deep geologic repository. The Hanford Waste Vitrification Plant will mix processed radioactive waste with borosilicate material, then heat the mixture to its melting point (vitrification) to forin a glass-like substance that traps the radionuclides in the glass matrix upon cooling. The Hanford Waste Vitrification Plant Quality Assurance Program has been established to support the mission of the Hanford Waste Vitrification Plant. This Quality Assurance Program Description has been written to document the Hanford Waste Vitrification Plant Quality Assurance Program

  13. Development of a ceramic waste form for high-level waste disposal

    International Nuclear Information System (INIS)

    A ceramic waste form is being developed by Argonne National Laboratory (ANL) as part of the demonstration of the electrometallurgical treatment of spent nuclear fuel. The halide, alkaline earth, alkali, transuranic, and rare earth fission products are stabilized in zeolite which is combined with glass and processed in a hot isostatic press (HIP) to form a ceramic composite. The mineral sodalite is formed in the HIP from the zeolite precursor. The process, from starting materials to final product, is relatively simple. An overview of the processing operations is given. The metrics that have been developed to measure the success or completion of processing operations are developed and discussed. The impact of variability in processing metrics on the durability of the final product is presented

  14. Immobilization of 99Tc in low-temperature phosphate ceramic waste forms

    International Nuclear Information System (INIS)

    Radionuclides such as 99Tc are by-products of fission reactions in high-level wastes. Technetium poses a serious environmental threat because it is easily oxidized into its highly leachable pertechnetate form. Magnesium potassium phosphate ceramics have been developed to treat 99Tc that has been separated and eluted from simulated high-level tank wastes by sorption processes. Dense and hard ceramic waste forms were fabricated by acid-base reactions between mixtures of magnesium oxide powders and wastes, and acid phosphate solutions. Standard leaching tests, such as ANS 16.1 and the Product Consistency Test, were conducted on the final waste forms to establish their performance. The fate of the contaminants in the final waste forms was established with scanning electron microscopy techniques. In addition, stability of the waste forms in aqueous environments was evaluated by long-term water immersion tests

  15. DuraLith geopolymer waste form for Hanford secondary waste: correlating setting behavior to hydration heat evolution.

    Science.gov (United States)

    Xu, Hui; Gong, Weiliang; Syltebo, Larry; Lutze, Werner; Pegg, Ian L

    2014-08-15

    The binary furnace slag-metakaolin DuraLith geopolymer waste form, which has been considered as one of the candidate waste forms for immobilization of certain Hanford secondary wastes (HSW) from the vitrification of nuclear wastes at the Hanford Site, Washington, was extended to a ternary fly ash-furnace slag-metakaolin system to improve workability, reduce hydration heat, and evaluate high HSW waste loading. A concentrated HSW simulant, consisting of more than 20 chemicals with a sodium concentration of 5 mol/L, was employed to prepare the alkaline activating solution. Fly ash was incorporated at up to 60 wt% into the binder materials, whereas metakaolin was kept constant at 26 wt%. The fresh waste form pastes were subjected to isothermal calorimetry and setting time measurement, and the cured samples were further characterized by compressive strength and TCLP leach tests. This study has firstly established quantitative linear relationships between both initial and final setting times and hydration heat, which were never discovered in scientific literature for any cementitious waste form or geopolymeric material. The successful establishment of the correlations between setting times and hydration heat may make it possible to efficiently design and optimize cementitious waste forms and industrial wastes based geopolymers using limited testing results.

  16. Characterization of low and medium-level radioactive waste forms. Joint annual progress report 1982

    International Nuclear Information System (INIS)

    The work reported was carried out during the second year of the Commission of the European Communities programme on the characterization of low and medium-level waste forms. Ten reference waste forms plus others of special national interest have been identified covering PWR, BWR, GCR and reprocessing wastes. The immobilizing media include the three main matrices: cement, polymers and bitumen, and a glass. Characterization is viewed as one input to quality assurance of the waste form and covers: waste-matrix compatibility, radiation effects, leaching, microbiological attack, shrinkage and swelling, ageing processes and thermal effects. The aim is a balanced programme of comparative data, predictive modelling and an understanding of basic mechanisms

  17. Radiation effects in glass and glass-ceramic waste forms for the immobilization of CANDU UO2 fuel reprocessing waste

    International Nuclear Information System (INIS)

    AECL has investigated three waste forms for the immobilization of high-level liquid wastes that would arise if used CANDU fuels were reprocessed at some time in the future to remove fissile materials for the fabrication of new power reactor fuel. These waste forms are borosilicate glasses, aluminosilicate glasses and titanosilicate glass-ceramics. This report discusses the potential effects of alpha, beta and gamma radiation on the releases of radionuclides from these waste forms as a result of aqueous corrosion by groundwaters that would be present in an underground waste disposal vault. The report discusses solid-state damage caused by radiation-induced atomic displacements in the waste forms as well as irradiation of groundwater solutions (radiolysis), and their potential effects on waste-form corrosion and radionuclide release. The current literature on radiation effects on borosilicate glasses and in ceramics is briefly reviewed, as are potential radiation effects on specialized waste forms for the immobilization of 129I, 85Kr and 14C. (author). 104 refs., 9 tabs., 5 figs

  18. 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

  19. 10CFR61 waste form conformance program for asphalted radwaste

    International Nuclear Information System (INIS)

    With the enactment of Title 10, Code of Federal Regulations, Part 61, ''Licensing Requirements for Land Disposal of Radioactive Waste'' came the imposition of new requirements on licensees who dispose of radioactive waste via shallow land burial. Specifically, 10CFR61 both imposed a waste classification system requiring segregation of waste according to hazard and established waste performance characteristics required to enhance stability of the burial site. In order to provide licensees with guidance regarding implementation of applicable requirements of 10CFR61, the NRC Low Level Waste Licensing Branch issued two Technical Positions. To demonstrate compliance of asphalted radwaste produced with oxidized asphalt with 10CRF61 criteria and the NRC's Technical Position, five utilities combined resources. The five utilities sponsoring the program were Public Service Electric and Gas Company, Niagara Mohawk Power Company, Detroit Edison Company, New Hampshire Yankee, and Consumers Power Company

  20. MINERALIZATION OF RADIOACTIVE WASTES BY FLUIDIZED BED STEAM REFORMING (FBSR): COMPARISONS TO VITREOUS WASTE FORMS, AND PERTINENT DURABILITY TESTING

    Energy Technology Data Exchange (ETDEWEB)

    Jantzen, C

    2008-12-26

    The Savannah River National Laboratory (SRNL) was requested to generate a document for the Washington State Department of Ecology and the U.S. Environmental Protection Agency that would cover the following topics: (1) A description of the mineral structures produced by Fluidized Bed Steam Reforming (FBSR) of Hanford type Low Activity Waste (LAW including LAWR which is LAW melter recycle waste) waste, especially the cage structured minerals and how they are formed. (2) How the cage structured minerals contain some contaminants, while others become part of the mineral structure (Note that all contaminants become part of the mineral structure and this will be described in the subsequent sections of this report). (3) Possible contaminant release mechanisms from the mineral structures. (4) Appropriate analyses to evaluate these release mechanisms. (5) Why the appropriate analyses are comparable to the existing Hanford glass dataset. In order to discuss the mineral structures and how they bond contaminants a brief description of the structures of both mineral (ceramic) and vitreous waste forms will be given to show their similarities. By demonstrating the similarities of mineral and vitreous waste forms on atomic level, the contaminant release mechanisms of the crystalline (mineral) and amorphous (glass) waste forms can be compared. This will then logically lead to the discussion of why many of the analyses used to evaluate vitreous waste forms and glass-ceramics (also known as glass composite materials) are appropriate for determining the release mechanisms of LAW/LAWR mineral waste forms and how the durability data on LAW/LAWR mineral waste forms relate to the durability data for LAW/LAWR glasses. The text will discuss the LAW mineral waste form made by FBSR. The nanoscale mechanism by which the minerals form will be also be described in the text. The appropriate analyses to evaluate contaminant release mechanisms will be discussed, as will the FBSR test results to

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

    Energy Technology Data Exchange (ETDEWEB)

    Carrel, F

    2007-10-15

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

  2. Characterisation of Nd-doped calcium aluminosilicate parent glasses designed for the preparation of zirconolite-based glass-ceramic waste forms

    International Nuclear Information System (INIS)

    Zirconolite-based (nominally CaZrTi2O7) glass-ceramics belonging to the SiO2Al2O3-CaO- ZrO3-TiO2 system are good waste forms for the specific immobilisation of actinides. The understanding of their crystallisation processes implies to investigate the structure of the glass. Thus, the environment around Ti, Zr (nucleating agents) and Nd (trivalent actinides surrogate) was characterised in parent glasses. Electron spin resonance (ESR) study of the small amount of Ti3+ occurring in the glass enabled to identify two types of sites for titanium: the main one is of C4v or D4h symmetry. EXAFS showed that Zr occupied a quite well defined 6-7-fold coordinated site with second neighbours which could correspond to Ca/Ti and Zr. Nd environment was probed by optical spectroscopies (absorption, fluorescence), ESR and EXAFS. All these techniques demonstrated that the environment around Nd was very constrained by the glassy network. Notably, Nd occupies a highly distorted 8-9-fold coordinated site in the parent glass. (authors)

  3. Annual report on the development and characterization of solidified forms for nuclear wastes, 1979

    International Nuclear Information System (INIS)

    Development and characterization of solidified nuclear waste forms is a major continuing effort at Pacific Northwest Laboratory. Contributions from seven programs directed at understanding chemical composition, process conditions, and long-term behaviors of various nuclear waste forms are included in this report. The major findings of the report are included in extended figure captions that can be read as brief technical summaries of the research, with additional information included in a traditional narrative format. Waste form development proceeded on crystalline and glass materials for high-level and transuranic (TRU) wastes. Leaching studies emphasized new areas of research aimed at more basic understanding of waste form/aqueous solution interactions. Phase behavior and thermal effects research included studies on crystal phases in defense and TRU waste glasses and on liquid-liquid phase separation in borosilicate waste glasses. Radiation damage effects in crystals and glasses from alpha decay and from transmutation are reported

  4. Secondary Waste Form Development and Optimization—Cast Stone

    Energy Technology Data Exchange (ETDEWEB)

    Sundaram, S. K.; Parker, Kent E.; Valenta, Michelle M.; Pitman, Stan G.; Chun, Jaehun; Chung, Chul-Woo; Kimura, Marcia L.; Burns, Carolyn A.; Um, Wooyong; Westsik, Joseph H.

    2011-07-14

    Washington River Protection Services is considering the design and construction of a Solidification Treatment Unit (STU) for the Effluent Treatment Facility (ETF) at Hanford. The ETF is a Resource Conservation and Recovery Act-permitted, multi-waste, treatment and storage unit and can accept dangerous, low-level, and mixed wastewaters for treatment. The STU needs to be operational by 2018 to receive secondary liquid wastes generated during operation of the Hanford Tank Waste Treatment and Immobilization Plant (WTP). The STU to ETF will provide the additional capacity needed for ETF to process the increased volume of secondary wastes expected to be produced by WTP.

  5. Chemical and mechanical performance properties for various final waste forms -- PSPI scoping study

    Energy Technology Data Exchange (ETDEWEB)

    Farnsworth, R.K.; Larsen, E.D.; Sears, J.W.; Eddy, T.L.; Anderson, G.L.

    1996-09-01

    The US DOE is obtaining data on the performance properties of the various final waste forms that may be chosen as primary treatment products for the alpha-contaminated low-level and transuranic waste at the INEL`s Transuranic Storage Area. This report collects and compares selected properties that are key indicators of mechanical and chemical durability for Portland cement concrete, concrete formed under elevated temperature and pressure, sulfur polymer cement, borosilicate glass, and various forms of alumino-silicate glass, including in situ vitrification glass and various compositions of iron-enriched basalt (IEB) and iron-enriched basalt IV (IEB4). Compressive strength and impact resistance properties were used as performance indicators in comparative evaluation of the mechanical durability of each waste form, while various leachability data were used in comparative evaluation of each waste form`s chemical durability. The vitrified waste forms were generally more durable than the non-vitrified waste forms, with the iron-enriched alumino-silicate glasses and glass/ceramics exhibiting the most favorable chemical and mechanical durabilities. It appears that the addition of zirconia and titania to IEB (forming IEB4) increases the leach resistance of the lanthanides. The large compositional ranges for IEB and IEB4 more easily accommodate the compositions of the waste stored at the INEL than does the composition of borosilicate glass. It appears, however, that the large potential variation in IEB and IEB4 compositions resulting from differing waste feed compositions can impact waste form durability. Further work is needed to determine the range of waste stream feed compositions and rates of waste form cooling that will result in acceptable and optimized IEB or IEB4 waste form performance. 43 refs.

  6. Determination of the Rate of Formation of Hydroceramic Waste Forms made with INEEL Calcined Wastes

    Energy Technology Data Exchange (ETDEWEB)

    Barry Scheetz; Johnson Olanrewaju

    2001-10-15

    The formulation, synthesis, characterization and hydration kinetics of hydroceramic waste forms designed as potential hosts for existing INEEL calcine high-level wastes have been established as functions of temperature and processing time. Initial experimentations were conducted with several aluminosilicate pozzolanic materials, ranging from fly ash obtained from various power generating coal and other combustion industries to reactive alumina, natural clays and ground bottled glass powders. The final selection criteria were based on the ease of processing, excellent physical properties and chemical durability (low-leaching) determined from the PCT test produced in hydroceramic. The formulation contains vermiculite, Sr(NO32), CsC1, NaOH, thermally altered (calcined natural clay) and INEEL simulated calcine high-level nuclear wastes and 30 weight percent of fluorinel blend calcine and zirconia calcine. Syntheses were carried out at 75-200 degree C at autogeneous water pressure (100% relative humidity) at various time intervals. The resulting monolithic compact products were hard and resisted breaking when dropped from a 5 ft height. Hydroceramic host mixed with fluorinel blend calcine and processed at 75 degree C crumbled into rice hull-side grains or developed scaly flakes. However, the samples equally possessed the same chemical durability as their unbroken counterparts. Phase identification by XRD revealed that hydroceramic host crystallized type zeolite at 75-150 degree C and NaP1 at 175-200 degree C in addition to the presence of quartz phase originating from the clay reactant. Hydroceramic host mixed with either fluorinel blend calcine or zirconia calcine crystallized type A zeolite at 75-95 degree C, formed a mixture of type A zeolite and hydroxysodalite at 125-150 degree C and hydroxysodalite at 175-200 degree C. Quartz, calcium fluoride and zirconia phases from the clay reactant and the two calcine wastes were also detected. The PCT test solution

  7. 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.

  8. Nuclear waste management technical support in the development of nuclear waste form criteria for the NRC. Task 1. Waste package overview

    International Nuclear Information System (INIS)

    In this report the current state of waste package development for high level waste, transuranic waste, and spent fuel in the US and abroad has been assessed. Specifically, reviewed are recent and on-going research on various waste forms, container materials and backfills and tentatively identified those which are likely to perform most satisfactorily in the repository environment. Radiation effects on the waste package components have been reviewed and the magnitude of these effects has been identified. Areas requiring further research have been identified. The important variables affecting radionuclide release from the waste package have been described and an evaluation of regulatory criteria for high level waste and spent fuel is presented. Finally, for spent fuel, high level, and TRU waste, components which could be used to construct a waste package having potential to meet NRC performance requirements have been described and identified

  9. Nuclear waste management technical support in the development of nuclear waste form criteria for the NRC. Task 1. Waste package overview

    Energy Technology Data Exchange (ETDEWEB)

    Dayal, R.; Lee, B.S.; Wilke, R.J.; Swyler, K.J.; Soo, P.; Ahn, T.M.; McIntyre, N.S.; Veakis, E.

    1982-02-01

    In this report the current state of waste package development for high level waste, transuranic waste, and spent fuel in the US and abroad has been assessed. Specifically, reviewed are recent and on-going research on various waste forms, container materials and backfills and tentatively identified those which are likely to perform most satisfactorily in the repository environment. Radiation effects on the waste package components have been reviewed and the magnitude of these effects has been identified. Areas requiring further research have been identified. The important variables affecting radionuclide release from the waste package have been described and an evaluation of regulatory criteria for high level waste and spent fuel is presented. Finally, for spent fuel, high level, and TRU waste, components which could be used to construct a waste package having potential to meet NRC performance requirements have been described and identified.

  10. Standard test method for static leaching of monolithic waste forms for disposal of radioactive waste

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2010-01-01

    1.1 This test method provides a measure of the chemical durability of a simulated or radioactive monolithic waste form, such as a glass, ceramic, cement (grout), or cermet, in a test solution at temperatures <100°C under low specimen surface- area-to-leachant volume (S/V) ratio conditions. 1.2 This test method can be used to characterize the dissolution or leaching behaviors of various simulated or radioactive waste forms in various leachants under the specific conditions of the test based on analysis of the test solution. Data from this test are used to calculate normalized elemental mass loss values from specimens exposed to aqueous solutions at temperatures <100°C. 1.3 The test is conducted under static conditions in a constant solution volume and at a constant temperature. The reactivity of the test specimen is determined from the amounts of components released and accumulated in the solution over the test duration. A wide range of test conditions can be used to study material behavior, includin...

  11. MICROBIAL LEACHING OF CHROMIUM FROM SOLIDIFIED WASTE FORMS – A KINETIC STUDY

    OpenAIRE

    Carmalin Sophia Ayyappan

    2015-01-01

    In this study, Thiobacillus thiooxidans (T. thiooxidans) was used to study the microbial stability / degradation of cement-based waste forms. The waste forms contained a chromium salt (CrCl3·6H2O), cement and other additives viz., lime and gypsum in two different proportions. The experimental samples of all the simulated waste forms showed evidence of microbial growth as indicated by substantial increase in sulfate. Chromium leached from the waste forms was found to be lowest in cement – lime...

  12. Quality checking task force destructive testing of active waste forms

    International Nuclear Information System (INIS)

    The implications of sampling and testing of full size active packages of intermediate level wastes are summarised in this report. Sampling operations are technically feasible but a major difficulty will be the disposal of secondary waste. A literature survey indicated that destructive testing of wasteforms is not carried out as a routine operation in Europe or the USA. (author)

  13. Transuranic contaminated waste form characterization and data base

    Energy Technology Data Exchange (ETDEWEB)

    Kniazewycz, B.G.; McArthur, W.C.

    1980-07-01

    This volume contains appendices A to F. The properties of transuranium (TRU) radionuclides are described. Immobilization of TRU wastes by bituminization, urea-formaldehyde polymers, and cements is discussed. Research programs at DOE facilities engaged in TRU waste characterization and management studies are described.

  14. Immobilization of fission products in phosphate ceramic waste forms

    International Nuclear Information System (INIS)

    Argonne National Laboratory (ANL) is developing chemically bonded phosphate ceramics (CBPCs) to treat low-level mixed wastes, particularly those containing volatiles and pyrophorics that cannot be treated by conventional thermal processes. This work was begun under ANL''s Laboratory Directed Research and Development funds, followed by further development with support from EM-50''s Mixed Waste Focus Area

  15. Transuranic contaminated waste form characterization and data base

    International Nuclear Information System (INIS)

    This volume contains appendices A to F. The properties of transuranium (TRU) radionuclides are described. Immobilization of TRU wastes by bituminization, urea-formaldehyde polymers, and cements is discussed. Research programs at DOE facilities engaged in TRU waste characterization and management studies are described

  16. Process considerations for hot pressing ceramic nuclear waste forms

    International Nuclear Information System (INIS)

    Spray calcined simulated ceramic nuclear waste powders were hot pressed in graphite, nickel-lined graphite and ZrO2-lined Al2O3 dies. Densification, initial off-gas, waste element retention and pellet-die interactions were evaluated. Indicated process considerations and limitations are discussed. 15 figures

  17. Improved polyphase ceramic form for high-level defense nuclear waste

    International Nuclear Information System (INIS)

    An improved ceramic nuclear waste form and fabrication process have been developed using simulated Savannah River Plant defense high-level waste compositions. The waste form provides flexibility with respect to processing conditions while exhibiting superior resistance to ground water leaching than other currently proposed forms. The ceramic, consolidated by hot-isostatic pressing at 10400C and 10,000 psi, is composed of six major phases, nepheline, zirconolite, a murataite-type cubic phase, magnetite-type spinel, a magnetoplumbite solid solution, and perovskite. The waste form provides multiple crystal lattice sites for the waste elements, minimizes amorphous intergranular material, and can accommodate waste loadings in excess of 60 wt %. The fabrication of the ceramic can be accomplished with existing manufacturing technology and eliminates the effects of radionuclide volatilization and off-gas induced corrosion experienced with the molten processes for vitreous form production

  18. Nuclear waste form risk assessment for US defense waste at Savannah River Plant. Annual report fiscal year 1980

    Energy Technology Data Exchange (ETDEWEB)

    Cheung, H.; Jackson, D.D.; Revelli, M.A.

    1981-07-01

    Waste form dissolution studies and preliminary performance analyses were carried out to contribute a part of the data needed for the selection of a waste form for the disposal of Savannah River Plant defense waste in a deep geologic repository. The first portion of this work provides descriptions of the chemical interactions between the waste form and the geologic environment. We reviewed critically the dissolution/leaching data for borosilicate glass and SYNROC. Both chemical kinetic and thermodynamic models were developed to describe the dissolution process of these candidate waste forms so as to establish a fundamental basis for interpretation of experimental data and to provide directions for future experiments. The complementary second portion of this work is an assessment of the impacts of alternate waste forms upon the consequences of disposal in various proposed geological media. Employing systems analysis methodology, we began to evaluate the performance of a generic waste form for the case of a high risk scenario for a bedded salt repository. Results of sensitivity analysis, uncertainty analyses, and sensitivity to uncertainty analysis are presented.

  19. Hot-pressed barium sulphate ceramic waste forms for direct immobilization of medium level Magnox waste

    International Nuclear Information System (INIS)

    A possible method of treatment for Magnox cladding waste is by dissolution in nitric acid and precipitation of barium sulphate-based floc with which radioactive ions are co-precipitated. The floc could then be immobilized in a matrix material such as cement or bitumen to give the waste form, or alternatively can be converted directly into a waste form by hot pressing. This paper describes the direct conversion of barium sulphate floc, containing simulated radwaste, into a synthetic, ceramic version of the natural mineral barite by a hot-pressing route. By variation of the parameters pressure, temperature and time, optimum conditions for consolidation of the floc to > 90% theoretical density on a laboratory scale are found to be 22.5 MPa, 9000C for 10 minutes. Using a pressure of 15 MPa, at 9000C for 30 min., hot-pressed billets of BaSO4 have been made on a 5 kg scale. In going from the magnox waste to the hot-pressed barium sulphate a volume reduction factor approx. 18 is achieved. The principal phases in the product are found to be BaSO4, MgO and Fe3O4, and the degree of consolidation achieved depends on the MgO content. The leaching behaviour of the hot-pressed materials in 1000C, 3 day Soxhlet tests also depends on the MgO content, and on the consequent level of open porosity. If there is porosity accessible to the leach water, MgO at the internal surfaces is converted to Mg(OH)2, which deposits within the pores, and a weight gain is registered in the Soxhlet test. If, however, there is no open porosity, a weight loss occurs, and leach rates approx. 4 x 10-7 kg/m2/sec are found. In contrast, pure BaSO4, hot-pressed to similar densities, shows no variation in leaching behaviour over a wide range of open porosities, and gives Soxhlet leach rates approx. 8 x 10-8 kg/m2/sec. 6 figures, 2 tables

  20. Development of technetium alloy waste forms for advanced nuclear energy cycles

    International Nuclear Information System (INIS)

    The Fuel Cycle Technologies (FCT) Program within the Office of Nuclear Energy of the U.S. Department of Energy is charged with developing nuclear fuel cycle options that improve use of actinide resources, responsibly manage wastes, improve and limit proliferation risk. Technetium is a fission product of particular concern for disposal in a repository because of its high fission yield, long half-life, and high solubility and mobility in groundwater as pertechnetate. For example, modeling studies for the former Yucca Mountain repository site indicated that technetium would be an important dose contributor after closure of the repository, in the first 10,000 years. The FCT Program is investigating a range of potential repository environments for ultimate disposal of fission products including technetium from advanced nuclear fuel recycling schemes

  1. Leaching of a zirconolite ceramic waste-form under proton and He{sup 2+} irradiation

    Energy Technology Data Exchange (ETDEWEB)

    Tribet, M.; Toulhoat, N. [Univ. de Lyon, Univ. Lyon1, CNRS/IN2P3, UMR5822, Inst. de Physique Nucleaire de Lyon (IPNL), Villeurbanne (France); Moncoffre, N.; Jegou, C. [CEA/DEN/DTCD/SECM, Bagnols sur Ceze (France); Leturcq, G. [CEA/DEN/DRCP/SCPS, Bagnols sur Ceze (France); Corbel, C. [CEA/DSM/DRECAM/LSI, Ecole Polytechnique, Palaiseau (France); Toulhoat, P. [Univ. Lyon, Univ. Lyon1, CNRS/ISA, UFR de Chimie Biochimie, Villeurbanne (France)

    2008-07-01

    In the hypothesis of a nuclear waste geological disposal, zirconolite is a candidate host material for minor tri- and tetra-valent actinides arising from enhanced nuclear spent fuel reprocessing and partitioning. Its chemical durability has been studied here under charged particle-induced radiolysis (He{sup 2+} and proton external beams) to identify possible effects on dissolution rates and mechanisms in pure water. Two experimental geometries have been used to evaluate the influence of the following parameters: solid irradiation and total deposited energy. Results on the evolution of the elemental releases due to the enhanced dissolution of the zirconolite surface during charged particle-induced irradiation of water are presented. Under radiolysis, elemental releases are first kinetically controlled. When the titanium and the zirconium releases reach (or exceed) their corresponding hydroxide solubility limits, the zirconolite dissolution becomes thermodynamically controlled. (orig.)

  2. 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

  3. Preparation and characterization of polyphase ceramic for fixation of actinides and fission products

    International Nuclear Information System (INIS)

    Two basic crystalline phases, a fluorite type, calcia stabilized zirconia, and a magnetoplumbite type, CaAl12O19, have been studied for incorporating the full range of waste compositions in to polyphase ceramic forms. The phase assemblage provides crystalline host phases, with stable mineral analogues, for many radionuclides in the waste. Fluorite is considered to be suitable host phase for the fixation of actinides and lanthanides. Magnetoplumbite-like structure can accommodate a wide range of elements with various charges and ionic radii. These kinds of compounds, in addition, present good chemical inertia. (author)

  4. Waste Form Release Data Package for the 2001 Immobilized Low-Activity Waste Performance Assessment

    International Nuclear Information System (INIS)

    This data package documents the experimentally derived input data on the representative waste glasses LAWABP1 and HLP-31 that will be used for simulations of the immobilized lowactivity waste disposal system with the Subsurface Transport Over Reactive Multiphases (STORM) code. The STORM code will be used to provide the near-field radionuclide release source term for a performance assessment to be issued in March of 2001. Documented in this data package are data related to (1) kinetic rate law parameters for glass dissolution, (2) alkali-H ion exchange rate, (3) chemical reaction network of secondary phases that form in accelerated weathering tests, and (4) thermodynamic equilibrium constants assigned to these secondary phases. The kinetic rate law and Na+-H+ ion exchange rate were determined from single-pass flow-through experiments. Pressurized unsaturated flow and vapor hydration experiments were used for accelerated weathering or aging of the glasses. The majority of the thermodynamic data were extracted from the thermodynamic database package shipped with the geochemical code EQ3/6. However, several secondary reaction products identified from laboratory tests with prototypical LAW glasses were not included in this database, nor are the thermodynamic data available in the open literature. One of these phases, herschelite, was determined to have a potentially significant impact on the release calculations and so a solubility product was estimated using a polymer structure model developed for zeolites. Although this data package is relatively complete, final selection of ILAW glass compositions has not been done by the waste treatment plant contractor. Consequently, revisions to this data package to address new ILAW glass formulations are to be regularly expected.

  5. Evaluation of remote smearing of DWPF canistered waste forms

    International Nuclear Information System (INIS)

    The Savannah River Site (SRS) is evaluating the variables of the remote smearing process for monitoring transferable contamination on the waste glass canisters at the Defense Waste Processing Facility (DWPF). Smearing for transferable contamination is typically done by hand, but in this case, due to the nature of the high level waste within the canisters, remote smearing is required. The effectiveness of the smear pad was determined under varying conditions (distance traveled, force applied, and canister surface), as well as the relative importance of these factors. It was concluded that the remote smear is more reliable than the hand smear

  6. Molecular Environmental Science Using Synchrotron Radiation: Chemistry and Physics of Waste Form Materials

    Energy Technology Data Exchange (ETDEWEB)

    Lindle, Dennis W.

    2011-04-21

    Production of defense-related nuclear materials has generated large volumes of complex chemical wastes containing a mixture of radionuclides. The disposition of these wastes requires conversion of the liquid and solid-phase components into durable, solid forms suitable for long-term immobilization. Specially formulated glass compositions and ceramics such as pyrochlores and apatites are the main candidates for these wastes. An important consideration linked to the durability of waste-form materials is the local structure around the waste components. Equally important is the local structure of constituents of the glass and ceramic host matrix. Knowledge of the structure in the waste-form host matrices is essential, prior to and subsequent to waste incorporation, to evaluate and develop improved waste-form compositions based on scientific considerations. This project used the soft-x-ray synchrotron-radiation-based technique of near-edge x-ray-absorption fine structure (NEXAFS) as a unique method for investigating oxidation states and structures of low-Z elemental constituents forming the backbones of glass and ceramic host matrices for waste-form materials. In addition, light metal ions in ceramic hosts, such as titanium, are also ideal for investigation by NEXAFS in the soft-x-ray region. Thus, one of the main objectives was to understand outstanding issues in waste-form science via NEXAFS investigations and to translate this understanding into better waste-form materials, followed by eventual capability to investigate “real” waste-form materials by the same methodology. We conducted several detailed structural investigations of both pyrochlore ceramic and borosilicate-glass materials during the project and developed improved capabilities at Beamline 6.3.1 of the Advanced Light Source (ALS) to perform the studies.

  7. XAF/XANES studies of plutonium-loaded sodalite/glass composite waste forms.

    Energy Technology Data Exchange (ETDEWEB)

    Aase, S. B.; Kropf, A. J.; Lewis, M. A.; Reed, D. T.; Richmann, M. K.

    1999-07-14

    A sodalite/glass ceramic waste form has been developed to immobilize highly radioactive nuclear wastes in chloride form, as part of an electrochemical cleanup process. Simulated waste forms have been fabricated which contain plutonium and are representative of the salt from the electrometallurgical process to recover uranium from spent nuclear fuel. X-ray absorption fine structure spectroscopy (XAFS) and x-ray absorption near-edge spectroscopy (XANES) studies were performed to determine the location, oxidation state and form of the plutonium within these waste forms. Plutonium, in the non-fission-element case, was found to segregate as plutonium(IV) oxide with a crystallite size of at least 20 nm. With fission elements present, the crystallite size was about 2 nm. No plutonium was observed within the sodalite or glass in the waste form.

  8. XAF/XANES studies of plutonium-loaded sodalite/glass composite waste forms

    International Nuclear Information System (INIS)

    A sodalite/glass ceramic waste form has been developed to immobilize highly radioactive nuclear wastes in chloride form, as part of an electrochemical cleanup process. Simulated waste forms have been fabricated which contain plutonium and are representative of the salt from the electrometallurgical process to recover uranium from spent nuclear fuel. X-ray absorption fine structure spectroscopy (XAFS) and x-ray absorption near-edge spectroscopy (XANES) studies were performed to determine the location, oxidation state and form of the plutonium within these waste forms. Plutonium, in the non-fission-element case, was found to segregate as plutonium(IV) oxide with a crystallite size of at least 20 nm. With fission elements present, the crystallite size was about 2 nm. No plutonium was observed within the sodalite or glass in the waste form

  9. Nuclear waste-form risk assessment for US Defense waste at Savannah River Plant. Annual report FY 1981

    International Nuclear Information System (INIS)

    Savannah River Plant has been supporting the Lawrence Livermore National Laboratory in its present effort to perform risk assessments of alternative waste forms for defense waste. This effort relates to choosing a suitable combination of solid form and geologic medium on the basis of risk of exposure to future generations; therefore, the focus is on post-closure considerations of deep geologic repositories. The waste forms being investigated include borosilicate glass, SYNROC, and others. Geologic media under consideration are bedded salt, basalt, and tuff. The results of our work during FY 1981 are presented in this, our second annual report. The two complementary tasks that comprise our program, analysis of waste-form dissolution and risk assessment, are described

  10. Special waste-form lysimeters-arid: Three-year monitoring report

    International Nuclear Information System (INIS)

    Regulations governing the disposal of commercial low-level waste require all liquid waste to be solidified before burial. Most waste must be solidified into a rigid matrix such as cement or plastic to prevent waste consolidation and site slumping after burial. These solidification processes affect the rate at which radionuclides and other solutes are released into the soil. In 1983, a program was initiated at Pacific Northwest Laboratory to study the release of waste from samples of low-level radioactive waste that had been commercially solidified. The primary method used by this program is to bury sample waste forms in field lysimeters and monitor leachate composition from the release and transport of solutes. The lysimeter facility consists of 10 lysimeters, each containing one sample of solidified waste. Five different waste forms are being tested, allowing duplicate samples of each one to be evaluated. The samples were obtained from operating nuclear power plants and are actual waste forms routinely generated at these facilities. All solidification was accomplished by commercial processes. Sample size is a partially filled 210-L drum. All containers were removed prior to burial leaving the bare waste form in contact with the lysimeter soil. 11 refs., 14 figs., 16 tabs

  11. An experimental survey of the factors that affect leaching from low-level radioactive waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Dougherty, D.R.; Pietrzak, R.F.; Fuhrmann, M.; Colombo, P.

    1988-09-01

    This report represents the results of an experimental survey of the factors that affect leaching from several types of solidified low-level radioactive waste forms. The goal of these investigations was to determine those factors that accelerate leaching without changing its mechanism(s). Typically, although not in every case,the accelerating factors include: increased temperature, increased waste loading (i.e., increased waste to binder ratio), and decreased size (i.e., decreased waste form volume to surface area ratio). Additional factors that were studied were: increased leachant volume to waste form surface area ratio, pH, leachant composition (groundwaters, natural and synthetic chelating agents), leachant flow rate or replacement frequency and waste form porosity and surface condition. Other potential factors, including the radiation environment and pressure, were omitted based on a survey of the literature. 82 refs., 236 figs., 13 tabs.

  12. Characterization and durability testing of a glass-bonded ceramic waste form

    International Nuclear Information System (INIS)

    Argonne National Laboratory is developing a glass bonded ceramic waste form for encapsulating the fission products and transuranics from the conditioning of metallic reactor fuel. This waste form is currently being scaled to the multi-kilogram size for encapsulation of actual high level waste. This paper will present characterization and durability testing of the ceramic waste form. An emphasis on results from application of glass durability tests such as the Product Consistency Test and characterization methods such as X-ray diffraction and scanning electron microscopy. The information presented is based on a suite of tests utilized for assessing product quality during scale-up and parametric testing

  13. Thermophysical Properties of Multiphase Borosilicate Glass-Ceramic Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Nelson, Andrew T. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Crum, Jarrod V. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Tang, Ming [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Rouxel, T. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2014-01-22

    Multiphase borosilicate glass-ceramics represent one candidate to contain radioactive nuclear waste separated from used nuclear fuel. In this work, the thermophysical properties from room temperature to 1273 K were investigated for four different borosilicate glass-ceramic compositions containing waste loadings from 42 to 60 wt% to determine the sensitivity of these properties to waste loading, as-fabricated microstructure, and potential evolutions in microstructure brought about by temperature transients. The thermal expansion, specific heat capacity, thermal diffusivity, and thermal conductivity are presented. The impact of increasing waste loading is shown to have a small but measurable effect on the thermophysical properties between the four compositions, contrasted to a much greater impact observed when transitioning from predominantly crystalline to amorphous systems. Thermal cycling below 1273 K was not found to measurably impact the thermophysical properties of the compositions investigated here.

  14. Heat of Hydration of Low Activity Cementitious Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Nasol, D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-07-23

    During the curing of secondary waste grout, the hydraulic materials in the dry mix react exothermally with the water in the secondary low-activity waste (LAW). The heat released, called the heat of hydration, can be measured using a TAM Air Isothermal Calorimeter. By holding temperature constant in the instrument, the heat of hydration during the curing process can be determined. This will provide information that can be used in the design of a waste solidification facility. At the Savannah River National Laboratory (SRNL), the heat of hydration and other physical properties are being collected on grout prepared using three simulants of liquid secondary waste generated at the Hanford Site. From this study it was found that both the simulant and dry mix each had an effect on the heat of hydration. It was also concluded that the higher the cement content in the dry materials mix, the greater the heat of hydration during the curing of grout.

  15. Assessment of spent-fuel waste-form/stabilizer alternatives for geologic disposal

    International Nuclear Information System (INIS)

    The Office of Nuclear Waste Isolation (ONWI) is studying the possibility of burying canisterized unreprocessed spent fuel in a deep geologic repository. One aspect of this study is an assessment of the possible spent fuel waste forms. The fuel performance portion of the Waste Form Assessment was to evaluate five candidate spent fuel waste forms for postemplacement performance with emphasis on their ability to retard the release of radionuclides to the repository geology. Spent fuel waste forms under general consideration were: (1) unaltered fuel assembly; (2) fuel assembly with end fittings removed to shorten the length; (3 rods vented to remove gases and resealed; (4) disassembled fuel bundles to close-pack the rods; and (5) rods chopped and fragments immobilized in a matrix material. Thirteen spent fuel waste forms, classified by generic stabilizer type, were analyzed for relative in-repository performance based on: (1) waste form/stabilizer support against lithostatic pressure; (2) long-term stability for radionuclide retention; (3) minimization of cladding degradation; (4) prevention of canister/repository breach due to pressurization; (5) stabilizer heat transfer; (6) the stabilizer as an independent barrier to radionuclide migration; and (7) prevention of criticality. The waste form candidates were ranked as follows: (1) the best waste form/stabilizer combination is the intact assembly, with or without end bells, vented (and resealed) or unvented, with a solid stabilizer; (2) a suitable alternative is the combination of bundled close-packed rods with a solid stabilizer around the outside of the bundle to resist lithostatic pressure; and (3) the other possible waste forms are of lower ranking with the worst waste form/stabilizer combination being the intact assembly with a gas stabilizer or the chopped fuel

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

    International Nuclear Information System (INIS)

    The aim of this project is to design and study new extractants for spent nuclear fuel reprocessing. To decrease the long-term radiotoxicity of the waste, the GANEX process is an option to homogeneously recycle actinides. All actinides (U, Np, Pu, Am, Cm) would be extracted together from a highly acidic media and separated from fission products (especially from lanthanides). In this context, fourteen new bi-topic ligands constituted of a nitrogen poly-aromatic unit from the dipyridyl-phenanthroline and dipyridyl-1,3,5-triazine families and functionalized by amid groups were synthesized. Extraction studies performed with some of these ligands confirmed their interest to selectively separate actinides at different oxidation states from an aqueous solution 3M HNO3. To determine the influence of ligands structure on cation complexation, a study in a homogenous media (MeOH/H2O) has been carried out. Electro-spray ionization mass spectrometry have been used to characterize the complexes stoichiometries formed with several cations (Eu3+, Nd3+, Am3+, Pu4+ and NpO2+). Stability constants, evaluated by UV-Visible spectrophotometry, confirm the selectivity of these ligands toward actinides. Lanthanides and actinides complexes have also been characterized in the solid state by infra-red spectroscopy and X-Ray diffraction. Associated to nuclear magnetic resonance experiments and DFT calculations (Density Functional Theory), a better knowledge of their coordination mode was achieved. (author)

  17. 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)

  18. Description of Defense Waste Processing Facility reference waste form and canister. Revision 1

    Energy Technology Data Exchange (ETDEWEB)

    Baxter, R.G.

    1983-08-01

    The Defense Waste Processing Facility (DWPF) will be located at the Savannah River Plant in Aiken, SC, and is scheduled for construction authorization during FY-1984. The reference waste form is borosilicate glass containing approx. 28 wt % sludge oxides, with the balance glass frit. Borosilicate glass was chosen because of its high resistance to leaching by water, its relatively high solubility for nuclides found in the sludge, and its reasonably low melting temperature. The glass frit contains about 58% SiO/sub 2/ and 15% B/sub 2/O/sub 3/. Leachabilities of SRP waste glasses are expected to approach 10/sup -8/ g/m/sup 2/-day based upon 1000-day tests using glasses containing SRP radioactive waste. Tests were performed under a wide variety of conditions simulating repository environments. The canister is filled with 3260 lb of glass which occupies about 85% of the free canister volume. The filled canister will generate approx. 470 watts when filled with oxides from 5-year-old sludge and 15-year-old supernate from the sludge and supernate processes. The radionuclide content of the canister is about 177,000 ci, with a radiation level of 5500 rem/h at canister surface contact. The reference canister is fabricated of standard 24-in.-OD, Schedule 20, 304L stainless steel pipe with a dished bottom, domed head, and a combined lifting and welding flange on the head neck. The overall canister length is 9 ft 10 in. with a 3/8-in. wall thickness. The 3-m canister length was selected to reduce equipment cell height in the DWPF to a practical size. The canister diameter was selected as an optimum size from glass quality considerations, a logical size for repository handling and to ensure that a filled canister with its double containment shipping cask could be accommodated on a legal-weight truck. The overall dimensions and weight appear to be compatible with preliminary assessments of repository requirements. 10 references.

  19. Evaluation of sulfur polymer cement as a waste form for the immobilization of low-level radioactive or mixed waste

    International Nuclear Information System (INIS)

    Sulfur polymer cement (SPC), also called modified sulphur cements, is a relatively new material in the waste immobilization field, although it was developed in the late seventies by the Bureau of Mines. The physical and chemical properties of SPC are interesting (e.g., development of high mechanical strength in a short time and high resistance to many corrosive environments). Because of its very low permeability and porosity, SPC is especially impervious to water, which, in turn, has led to its consideration for immobilization of hazardous or radioactive waste. Because it is a thermosetting process, the waste is encapsulated by the sulfur matrix; therefore, very little interaction occurs between the waste species and the sulfur (as there can be when waste prevents the set of portland cement-based waste forms)

  20. Alternative Electrochemical Salt Waste Forms, Summary of FY/CY2011 Results

    Energy Technology Data Exchange (ETDEWEB)

    Riley, Brian J.; McCloy, John S.; Crum, Jarrod V.; Rodriguez, Carmen P.; Windisch, Charles F.; Lepry, William C.; Matyas, Josef; Westman, Matthew P.; Rieck, Bennett T.; Lang, Jesse B.; Pierce, David A.

    2011-12-01

    This report summarizes the 2011 fiscal+calendar year efforts for developing waste forms for a spent salt generated in reprocessing nuclear fuel with an electrochemical separations process. The two waste forms are tellurite (TeO2-based) glasses and sol-gel-derived high-halide mineral analogs to stable minerals found in nature.

  1. Waste acceptance product specifications for vitrified high-level waste forms

    International Nuclear Information System (INIS)

    The Department of Energy (DOE) Office of Environmental Restoration and Waste Management (EM) has developed Waste Acceptance Product Specifications (EM-WAPS). The EM-WAPS will be the basis for defining product acceptance criteria compatible with the requirements of the Civilian Radioactive Waste Management System (CRWMS). The relationship between the EM-WAPS and the CRWMS Systems Requirements document (WA-SRD) will be discussed. The impact of the EM-WAPS on the Savannah River Sit (SRS) Defense Waste Processing Facility's (DWPF) Waste Acceptance Program, Waste Qualification Run planning, and startup schedule will also be reported. 14 refs., 2 tabs

  2. 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

  3. Application of the NNWSI [Nevada Nuclear Waste Storage Investigations] unsaturated test method to actinide doped SRL [Savannah River Laboratory] 165 type glass

    Energy Technology Data Exchange (ETDEWEB)

    Bates, J.K.; Gerding, T.J.

    1990-08-01

    The results of tests done using the Unsaturated Test Method are presented. These tests, done to determine the suitability of glass in a potential high-level waste repository as developed by the Nevada Nuclear Waste Storage Investigations Project, simulate conditions anticipated for the post-containment phase of the repository when only limited contact between the waste form and water is expected. The reaction of glass occurs via processes that are initiated due to glass/water vapor and glass/liquid water contact. Vapor interaction results in the initiation of an exchange process between water and the more mobile species (alkalis and boron) in the glass. The liquid reaction produces interactions similar to those seen in standard leaching tests, except due to the limited amount of water present and the presence of partially sensitized 304L stainless steel, the formation of reaction products greatly exceeds that found in MCC-1 type leach tests. The effect of sensitized stainless steel on the reaction is to enhance breakdown of the glass matrix thereby increasing the release of the transuranic elements from the glass. However, most of the Pu and Am released is entrained by either the metal components of the test or by the reaction phases, and is not released to solution. 16 refs., 20 figs., 17 tabs.

  4. Measurements of the neutron capture cross sections and incineration potentials of minor-actinides in high thermal neutron fluxes: Impact on the transmutation of nuclear wastes

    International Nuclear Information System (INIS)

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

  5. Immobilization of fission products in low-temperature ceramic waste forms

    International Nuclear Information System (INIS)

    Over the last few years, Argonne National Laboratory has been developing room-temperature-setting chemically bonded phosphate ceramics (CBPCs) for use in solidifying and stabilizing low-level mixed wastes. The focus of this work is development of CBPCs for use with fission-product wastes generated from high-level waste (HLW) tank cleaning or other decontamination and decommissioning activities. The volatile fission products such as Tc, Cs, and Sr removed from HLW need to be disposed of in a low-temperature immobilization system. Specifically, this paper reports on the solidification and stabilization of separated 99Tc from Los Alamos National Laboratory's complexation-elution process. Using rhenium as a surrogate form technetium, we fabricated CBPC waste forms by acid-base reactions. Dense and hard ceramic waste forms are produced in this process. The principal advantage of this technology is that the contaminants are immobilized by both chemical stabilization and subsequent microencapsulation of the reaction products. This paper reports the results of durability studies conducted on waste forms made with 35 wt.% waste loading. Standard leaching tests such as ANS 16.1 and PCT were conducted on the final waste forms. In addition, stability of the waste forms in aqueous environments was evaluated by long-term water-immersion tests

  6. Experiment close out of lysimeter field testing of low-level radioactive waste forms

    International Nuclear Information System (INIS)

    The Field Lysimeter Investigations: Low-Level Waste Data Base Development Program is obtaining information on the performance of radioactive waste forms. These experiments were recently shut down and the contents of the lysimeters have been examined in accordance with a detailed waste form and soil sampling plan. Ion-exchange resins from a commercial nuclear power station were solidified into waste forms using portland cement and vinyl ester-styrene. These waste forms were tested to (a) obtain information on performance of waste forms in typical disposal environments, (b) compare field results with bench leach studies, (c) develop a low-level waste data base for use in performance assessment source term calculations, and (d) apply the DUST computer code to compare predicted cumulative release to actual field data. The program, funded by the Nuclear Regulatory Commission (NRC), includes observed radio nuclide releases from waste forms in field lysimeters at two test sites over 10 years of successful operation. The purpose of this paper is to present the results of the examination of waste forms and soils of the two lysimeter arrays after shut down. During this examination, the waste forms were characterized after removal from the lysimeters and the results compared to the findings of the original characterizations. Vertical soil cores were taken from the soil columns and analyzed with radiochemistry to define movement of radionuclides in the soils after release from the waste forms. A comparison is made of the DUST and BLT code predictions of releases and movement, using recently developed partition coefficients and leachate measurements, to actual radio nuclide movement through the soil columns as determined from these core analyses

  7. Melt processed crystalline ceramic waste forms for advanced nuclear fuel cycles: CRP T21027 1813: Processing technologies for high level waste, formulation of matrices and characterization of waste forms, Task 17208: Final report

    Energy Technology Data Exchange (ETDEWEB)

    Amoroso, J. W. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Marra, J. C. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-08-26

    A multi-phase ceramic waste form is being developed at the Savannah River National Laboratory (SRNL) for treatment of secondary waste streams generated by reprocessing commercial spent nuclear. The envisioned waste stream contains a mixture of transition, alkali, alkaline earth, and lanthanide metals. Ceramic waste forms are tailored (engineered) to incorporate waste components as part of their crystal structure based on knowledge from naturally found minerals containing radioactive and non-radioactive species similar to the radionuclides of concern in wastes from fuel reprocessing. The ability to tailor ceramics to mimic naturally occurring crystals substantiates the long term stability of such crystals (ceramics) over geologic timescales of interest for nuclear waste immobilization [1]. A durable multi-phase ceramic waste form tailored to incorporate all the waste components has the potential to broaden the available disposal options and thus minimize the storage and disposal costs associated with aqueous reprocessing. This report summarizes results from three years of work on the IAEA Coordinated Research Project on “Processing technologies for high level waste, formulation of matrices and characterization of waste forms” (T21027), and specific task “Melt Processed Crystalline Ceramic Waste Forms for Advanced Nuclear Fuel Cycles” (17208).

  8. Melt processed crystalline ceramic waste forms for advanced nuclear fuel cycles: CRP T21027 1813: Processing technologies for high level waste, formulation of matrices and characterization of waste forms, task 17208: Final report

    Energy Technology Data Exchange (ETDEWEB)

    Amoroso, J. W. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Marra, J. C. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-08-26

    A multi-phase ceramic waste form is being developed at the Savannah River National Laboratory (SRNL) for treatment of secondary waste streams generated by reprocessing commercial spent nuclear. The envisioned waste stream contains a mixture of transition, alkali, alkaline earth, and lanthanide metals. Ceramic waste forms are tailored (engineered) to incorporate waste components as part of their crystal structure based on knowledge from naturally found minerals containing radioactive and non-radioactive species similar to the radionuclides of concern in wastes from fuel reprocessing. The ability to tailor ceramics to mimic naturally occurring crystals substantiates the long term stability of such crystals (ceramics) over geologic timescales of interest for nuclear waste immobilization [1]. A durable multi-phase ceramic waste form tailored to incorporate all the waste components has the potential to broaden the available disposal options and thus minimize the storage and disposal costs associated with aqueous reprocessing. This report summarizes results from three years of work on the IAEA Coordinated Research Project on “Processing technologies for high level waste, formulation of matrices and characterization of waste forms” (T21027), and specific task “Melt Processed Crystalline Ceramic Waste Forms for Advanced Nuclear Fuel Cycles” (17208).

  9. Influence of bacteria on lanthanide and actinide transfer from specific soil components (humus, soil minerals and vitrified municipal solid waste incinerator bottom ash) to corn plants: Sr-Nd isotope evidence

    International Nuclear Information System (INIS)

    Experiments have been performed to test the stability of vitrified municipal solid waste (MSW) incinerator bottom ash under the presence of bacteria (Pseudomonas aeruginosa) and plants (corn). The substratum used for the plant growth was a humus-rich soil mixed with vitrified waste. For the first time, information on the stability of waste glasses in the presence of bacteria and plants is given. Results show that inoculated plant samples contained always about two times higher lanthanide and actinide element concentrations. Bacteria support the element transfer since plants growing in inoculated environment developed a smaller root system but have higher trace element concentrations. Compared with the substratum, plants are light rare earth element (LREE) enriched. The vitrified bottom ash has to some extent been corroded by bacteria and plant activities as indicated by the presence of Nd (REE) and Sr from the vitrified waste in the plants. 87Sr/86Sr and 143Nd/144Nd isotope ratios of plants and soil components allow the identification of the corroded soil components and confirm that bacteria accelerate the assimilation of elements from the vitrified bottom ash. These findings are of importance for landfill disposal scenarios, and similar experiments should be performed in order to better constrain the processes of microbially mediated alteration of the MSW glasses in the biosphere

  10. Influence of bacteria on lanthanide and actinide transfer from specific soil components (humus, soil minerals and vitrified municipal solid waste incinerator bottom ash) to corn plants: Sr-Nd isotope evidence

    Energy Technology Data Exchange (ETDEWEB)

    Aouad, Georges [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France); Stille, Peter [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France)]. E-mail: pstille@illite.u-strasbg.fr; Crovisier, Jean-Louis [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France); Geoffroy, Valerie A. [UMR 7156 Universite Louis-Pasteur/CNRS, Genetique Moleculaire, Genomique Microbiologie, Departement Micro-organisme, Genomes, Environnement, 28 rue Goethe, 67083 Strasbourg Cedex (France); Meyer, Jean-Marie [UMR 7156 Universite Louis-Pasteur/CNRS, Genetique Moleculaire, Genomique Microbiologie, Departement Micro-organisme, Genomes, Environnement, 28 rue Goethe, 67083 Strasbourg Cedex (France); Lahd-Geagea, Majdi [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France)

    2006-11-01

    Experiments have been performed to test the stability of vitrified municipal solid waste (MSW) incinerator bottom ash under the presence of bacteria (Pseudomonas aeruginosa) and plants (corn). The substratum used for the plant growth was a humus-rich soil mixed with vitrified waste. For the first time, information on the stability of waste glasses in the presence of bacteria and plants is given. Results show that inoculated plant samples contained always about two times higher lanthanide and actinide element concentrations. Bacteria support the element transfer since plants growing in inoculated environment developed a smaller root system but have higher trace element concentrations. Compared with the substratum, plants are light rare earth element (LREE) enriched. The vitrified bottom ash has to some extent been corroded by bacteria and plant activities as indicated by the presence of Nd (REE) and Sr from the vitrified waste in the plants. {sup 87}Sr/{sup 86}Sr and {sup 143}Nd/{sup 144}Nd isotope ratios of plants and soil components allow the identification of the corroded soil components and confirm that bacteria accelerate the assimilation of elements from the vitrified bottom ash. These findings are of importance for landfill disposal scenarios, and similar experiments should be performed in order to better constrain the processes of microbially mediated alteration of the MSW glasses in the biosphere.

  11. Mineral assemblage transformation of a metakaolin-based waste form after geopolymer encapsulation

    Science.gov (United States)

    Williams, Benjamin D.; Neeway, James J.; Snyder, Michelle M. V.; Bowden, Mark E.; Amonette, James E.; Arey, Bruce W.; Pierce, Eric M.; Brown, Christopher F.; Qafoku, Nikolla P.

    2016-05-01

    Mitigation of hazardous and radioactive waste can be improved through conversion of existing waste to a more chemically stable and physically robust waste form. One option for waste conversion is the fluidized bed steam reforming (FBSR) process. The resulting FBSR granular material was encapsulated in a geopolymer matrix referred to here as Geo-7. This provides mechanical strength for ease in transport and disposal. However, it is necessary to understand the phase assemblage evolution as a result of geopolymer encapsulation. In this study, we examine the mineral assemblages formed during the synthesis of the multiphase ceramic waste form. The FBSR granular samples were created from waste simulant that was chemically adjusted to resemble Hanford tank waste. Another set of samples was created using Savannah River Site Tank 50 waste simulant in order to mimic a blend of waste collected from 68 Hanford tank. Waste form performance tests were conducted using the product consistency test (PCT), the Toxicity Characteristic Leaching Procedure (TCLP), and the single-pass flow-through (SPFT) test. X-ray diffraction analyses revealed the structure of a previously unreported NAS phase and indicate that monolith creation may lead to a reduction in crystallinity as compared to the primary FBSR granular product.

  12. FY-87 packing fabrication techniques (commercial waste form) results

    International Nuclear Information System (INIS)

    This report covers the investigation of fabrication techniques associated with the development of suitable materials and methods to provide a prefabricated packing for waste packages for the Basalt Waste Isolation Project (BWIP). The principal functions of the packing are to minimize container corrosion during the 300 to 1000 years following repository closure and provide long-term control of the release of radionuclides from the waste package. The investigative work, discussed in this report, was specifically conceived to develop the design criteria for production of full-scale prototypical packing rings. The investigative work included the preparation of procedures, the preparation of fabrication materials, physical properties, and the determination of the engineering properties. The principal activities were the preparation of the materials and the determination of the physical properties. 21 refs., 20 figs., 14 tabs

  13. 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.

  14. Fluidized bed steam reformed mineral waste form performance testing to support Hanford Supplemental Low Activity Waste Immobilization Technology Selection

    Energy Technology Data Exchange (ETDEWEB)

    Jantzen, C. M. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Pierce, E. M. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Bannochie, C. J. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Burket, P. R. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Cozzi, A. D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Crawford, C. L. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Daniel, W. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Fox, K. M. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Herman, C. C. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Miller, D. H. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Missimer, D. M. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Nash, C. A. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Williams, M. F. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Brown, C. F. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Qafoku, N. P. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Neeway, J. J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Valenta, M. M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Gill, G. A. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Swanberg, D. J. [Washington River Protection Solutions (WRPS), Richland, WA (United States); Robbins, R. A. [Washington River Protection Solutions (WRPS), Richland, WA (United States); Thompson, L. E. [Washington River Protection Solutions (WRPS), Richland, WA (United States)

    2015-10-01

    This report describes the benchscale testing with simulant and radioactive Hanford Tank Blends, mineral product characterization and testing, and monolith testing and characterization. These projects were funded by DOE EM-31 Technology Development & Deployment (TDD) Program Technical Task Plan WP-5.2.1-2010-001 and are entitled “Fluidized Bed Steam Reformer Low-Level Waste Form Qualification”, Inter-Entity Work Order (IEWO) M0SRV00054 with Washington River Protection Solutions (WRPS) entitled “Fluidized Bed Steam Reforming Treatability Studies Using Savannah River Site (SRS) Low Activity Waste and Hanford Low Activity Waste Tank Samples”, and IEWO M0SRV00080, “Fluidized Bed Steam Reforming Waste Form Qualification Testing Using SRS Low Activity Waste and Hanford Low Activity Waste Tank Samples”. This was a multi-organizational program that included Savannah River National Laboratory (SRNL), THOR® Treatment Technologies (TTT), Pacific Northwest National Laboratory (PNNL), Oak Ridge National Laboratory (ORNL), Office of River Protection (ORP), and Washington River Protection Solutions (WRPS). The SRNL testing of the non-radioactive pilot-scale Fluidized Bed Steam Reformer (FBSR) products made by TTT, subsequent SRNL monolith formulation and testing and studies of these products, and SRNL Waste Treatment Plant Secondary Waste (WTP-SW) radioactive campaign were funded by DOE Advanced Remediation Technologies (ART) Phase 2 Project in connection with a Work-For-Others (WFO) between SRNL and TTT.

  15. Demonstrating compliance with the waste acceptance preliminary specifications on foreign materials within DWPF canistered waste forms (U)

    International Nuclear Information System (INIS)

    The Defense Waste Processing Facility (DWPF) will employ a waste acceptance program based on the Waste Acceptance Preliminary Specifications (WAPS). These specifications require, among other criteria, that the canistered waste form contain no free liquids, free gases, organics, or explosives. Of particular importance is the absence of liquid water. This paper summarizes efforts and discusses experiments at the Savannah River Site for demonstrating compliance with the foreign materials specifications of the WAPS. Existing data, already in the literature, is being combined with the results of new experiments. For the volatility of the waste glass, documented work is combined with new results of thermogravimetric analysis experiments on simulated waste glass samples produced during scale glass melter campaigns. The volatility of these glass samples provides evidence that no free liquids, free gases, organics, or explosives are released upon heating the waste glass to its glass transition temperature. To show compliance of the absence of liquid water, documented work is being combined with the results of new experiments involving measurement of the internal gas pressure, the composition of the gas within the canisters, and the relative humidity of sealed, canistered waste forms produced during large-scale glass melter runs and the upcoming cold runs of the DWPF. (orig.)

  16. A powder metallurgy approach for production of innovative radioactive waste forms

    International Nuclear Information System (INIS)

    The feasibility of producing a single metal-matrix composite form rather than two separate forms consisting of a cast metal alloy ingot (such as Type 316SS + Zr) and a ceramic glass-bonded zeolite Na12(AlO2)12(SiO2)12 has been demonstrated. This powder metallurgy approach consists of mixing the powder of the two separate waste forms together followed by compaction by hot isostatic pressing. Such a radioactive waste form would have the potential advantages of reducing the total waste volume, good thermal conductivity, stability, and surfaces with limited oxide layer formation. 5 refs., 8 figs., 2 tabs

  17. 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.

  18. 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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2001-12-01

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

  20. 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.

  1. A study on characterization and evaluation methodologies of radioactive waste forms for safe disposal

    Energy Technology Data Exchange (ETDEWEB)

    Seo, Y. C.; Lee, G. S.; Kim, G. J.; Nam, H.; Seok, J. H. [Yonsei Univ., Seoul (Korea, Republic of)

    2004-02-15

    The contents and scope of the study are summarized as follows : elicitation of significant items for characteristic assessment about stability analysis of radioactive waste forms for safe disposal, compressive strength, free water, leaching rate, and weatherability. Suggestion of assessment methods through the characteristic test of waste forms, comparison of assessment methods and suggestion of suitable testing methods about the above stated 4 items. Assessment modeling development for long-term stability of radioactive waste forms, weatherometric test of waste forms, expectation modeling development through VOM(Valance-Oxygen Model). Suggestion of determination standard together assessment testing methods and description about the standard. Explanation to be suitable guideline and regulation of waste handling and acceptance.

  2. Advanced waste form and Melter development for treatment of troublesome high-level wastes

    Energy Technology Data Exchange (ETDEWEB)

    Marra, James [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Kim, Dong -Sang [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Maio, Vincent [Idaho National Lab. (INL), Idaho Falls, ID (United States)

    2015-10-01

    A number of waste components in US defense high level radioactive wastes (HLW) have proven challenging for current Joule heated ceramic melter (JHCM) operations and have limited the ability to increase waste loadings beyond already realized levels. Many of these “troublesome" waste species cause crystallization in the glass melt that can negatively impact product quality or have a deleterious effect on melter processing. Recent efforts at US Department of Energy laboratories have focused on understanding crystallization behavior within HLW glass melts and investigating approaches to mitigate the impacts of crystallization so that increases in waste loading can be realized. Advanced glass formulations have been developed to highlight the unique benefits of next-generation melter technologies such as the Cold Crucible Induction Melter (CCIM). Crystal-tolerant HLW glasses have been investigated to allow sparingly soluble components such as chromium to crystallize in the melter but pass out of the melter before accumulating.The Hanford site AZ-101 tank waste composition represents a waste group that is waste loading limited primarily due to high concentrations of Fe2O3 (also with high Al2O3 concentrations). Systematic glass formulation development utilizing slightly higher process temperatures and higher tolerance to spinel crystals demonstrated that an increase in waste loading of more than 20% could be achieved for this waste composition, and by extension higher loadings for wastes in the same group. An extended duration CCIM melter test was conducted on an AZ-101 waste simulant using the CCIM platform at the Idaho National Laboratory (INL). The melter was continually operated for approximately 80 hours demonstrating that the AZ-101 high waste loading glass composition could be readily processed using the CCIM technology. The resulting glass was close to the targeted composition and exhibited excellent durability in both

  3. Conceptual waste package interim product specifications and data requirements for disposal of borosilicate glass defense high-level waste forms in salt geologic repositories

    International Nuclear Information System (INIS)

    The conceptual waste package interim product specifications and data requirements presented are applicable specifically to the normal borosilicate glass product of the Defense Waste Processing Facility (DWPF). They provide preliminary numerical values for the defense high-level waste form parameters and properties identified in the waste form performance specification for geologic isolation in salt repositories. Subject areas treated include containment and isolation, operational period safety, criticality control, waste form/production canister identification, and waste package performance testing requirements. This document was generated for use in the development of conceptual waste package designs in salt. It will be revised as additional data, analyses, and regulatory requirements become available

  4. Conceptual waste package interim product specifications and data requirements for disposal of borosilicate glass defense high-level waste forms in salt geologic repositories

    Energy Technology Data Exchange (ETDEWEB)

    1983-06-01

    The conceptual waste package interim product specifications and data requirements presented are applicable specifically to the normal borosilicate glass product of the Defense Waste Processing Facility (DWPF). They provide preliminary numerical values for the defense high-level waste form parameters and properties identified in the waste form performance specification for geologic isolation in salt repositories. Subject areas treated include containment and isolation, operational period safety, criticality control, waste form/production canister identification, and waste package performance testing requirements. This document was generated for use in the development of conceptual waste package designs in salt. It will be revised as additional data, analyses, and regulatory requirements become available.

  5. Data Package for Secondary Waste Form Down-Selection—Cast Stone

    Energy Technology Data Exchange (ETDEWEB)

    Serne, R. Jeffrey; Westsik, Joseph H.

    2011-09-05

    Available literature on Cast Stone and Saltstone was reviewed with an emphasis on determining how Cast Stone and related grout waste forms performed in relationship to various criteria that will be used to decide whether a specific type of waste form meets acceptance criteria for disposal in the Integrated Disposal Facility (IDF) at Hanford. After the critical review of the Cast Stone/Saltstone literature, we conclude that Cast Stone is a good candidate waste form for further consideration. Cast stone meets the target IDF acceptance criteria for compressive strength, no free liquids, TCLP leachate are below the UTS permissible concentrations and leach rates for Na and Tc-99 are suiteably low. The cost of starting ingredients and equipment necessary to generate Cast Stone waste forms with secondary waste streams are low and the Cast Stone dry blend formulation can be tailored to accommodate variations in liquid waste stream compositions. The database for Cast Stone short-term performance is quite extensive compared to the other three candidate waste solidification processes. The solidification of liquid wastes in Cast Stone is a mature process in comparison to the other three candidates. Successful production of Cast Stone or Saltstone has been demonstrated from lab-scale monoliths with volumes of cm3 through m3 sized blocks to 210-liter sized drums all the way to the large pours into vaults at Savannah River. To date over 9 million gallons of low activity liquid waste has been solidified and disposed in concrete vaults at Savannah River.

  6. MICROBIAL LEACHING OF CHROMIUM FROM SOLIDIFIED WASTE FORMS – A KINETIC STUDY

    Directory of Open Access Journals (Sweden)

    Carmalin Sophia Ayyappan

    2015-06-01

    Full Text Available In this study, Thiobacillus thiooxidans (T. thiooxidans was used to study the microbial stability / degradation of cement-based waste forms. The waste forms contained a chromium salt (CrCl3·6H2O, cement and other additives viz., lime and gypsum in two different proportions. The experimental samples of all the simulated waste forms showed evidence of microbial growth as indicated by substantial increase in sulfate. Chromium leached from the waste forms was found to be lowest in cement – lime solidified waste forms (0.061 mg·l-1 and highest in cement gypsum waste forms (0.22 mg·l-1 after 30 days of exposure. These values were lower than the toxicity characteristic leaching procedure (TCLP, regulatory limit (5 mg·l-1. Model equations based on two shrinking core models (acid dissolution and bulk diffusion model, were used to analyze the kinetics of microbial degradation of cement based waste forms. The bulk diffusion model was observed to fit the data better than the acid dissolution model, as indicated by good correlation coefficients.

  7. Evaluation of interim and final waste forms for the newly generated liquid low-level waste flowsheet

    International Nuclear Information System (INIS)

    The purpose of this review is to evaluate the final forms that have been proposed for radioactive-containing solid wastes and to determine their application to the solid wastes that will result from the treatment of newly generated liquid low-level waste (NGLLLW) and Melton Valley Storage Tank (MVST) supernate at the Oak Ridge National Laboratory (ORNL). Since cesium and strontium are the predominant radionuclides in NGLLLW and MVST supernate, this review is focused on the stabilization and solidification of solid wastes containing these radionuclides in cement, glass, and polymeric materials-the principal waste forms that have been tested with these types of wastes. Several studies have shown that both cesium and strontium are leached by distilled water from solidified cement, although the leachabilities of cesium are generally higher than those of strontium under similar conditions. The situation is exacerbated by the presence of sulfates in the solution, as manifested by cracking of the grout. Additives such as bentonite, blast-furnace slag, fly ash, montmorillonite, pottery clay, silica, and zeolites generally decrease the cesium and strontium release rates. Longer cement curing times (>28 d) and high ionic strengths of the leachates, such as those that occur in seawater, also decrease the leach rates of these radionuclides. Lower cesium leach rates are observed from vitrified wastes than from grout waste forms. However, significant quantities of cesium are volatilized due to the elevated temperatures required to vitrify the waste. Hence, vitrification will generally require the use of cleanup systems for the off-gases to prevent their release into the atmosphere

  8. 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)

  9. State-of-the-art review of materials properties of nuclear waste forms

    International Nuclear Information System (INIS)

    The Materials Characterization Center (MCC) was established at the Pacific Northwest Laboratory to assemble a standardized nuclear waste materials data base for use in research, systems and facility design, safety analyses, and waste management decisions. This centralized data base will be provided through the means of a Nuclear Waste Materials Handbook. The first issue of the Handbook will be published in the fall of 1981 in looseleaf format so that it can be updated as additional information becomes available. To ensure utmost reliability, all materials data appearing in the Handbook will be obtained by standard procedures defined in the Handbook and approved by an independent Materials Review Board (MRB) comprised of materials experts from Department of Energy laboratories and from universities and industry. In the interim before publication of the Handbook there is need for a report summarizing the existing materials data on nuclear waste forms. This review summarizes materials property data for the nuclear waste forms that are being developed for immobilization of high-level radioactive waste. It is intended to be a good representation of the knowledge concerning the properties of HLW forms as of March 1981. The table of contents lists the following topics: introduction which covers waste-form categories, and important waste-form materials properties; physical properties; mechanical properties; chemical durability; vaporization; radiation effects; and thermal phase stability

  10. State-of-the-art review of materials properties of nuclear waste forms.

    Energy Technology Data Exchange (ETDEWEB)

    Mendel, J. E.; Nelson, R. D.; Turcotte, R. P.; Gray, W. J.; Merz, M. D.; Roberts, F. P.; Weber, W. J.; Westsik, Jr., J. H.; Clark, D. E.

    1981-04-01

    The Materials Characterization Center (MCC) was established at the Pacific Northwest Laboratory to assemble a standardized nuclear waste materials data base for use in research, systems and facility design, safety analyses, and waste management decisions. This centralized data base will be provided through the means of a Nuclear Waste Materials Handbook. The first issue of the Handbook will be published in the fall of 1981 in looseleaf format so that it can be updated as additional information becomes available. To ensure utmost reliability, all materials data appearing in the Handbook will be obtained by standard procedures defined in the Handbook and approved by an independent Materials Review Board (MRB) comprised of materials experts from Department of Energy laboratories and from universities and industry. In the interim before publication of the Handbook there is need for a report summarizing the existing materials data on nuclear waste forms. This review summarizes materials property data for the nuclear waste forms that are being developed for immobilization of high-level radioactive waste. It is intended to be a good representation of the knowledge concerning the properties of HLW forms as of March 1981. The table of contents lists the following topics: introduction which covers waste-form categories, and important waste-form materials properties; physical properties; mechanical properties; chemical durability; vaporization; radiation effects; and thermal phase stability.

  11. Performance of high level waste forms and engineered barriers under repository conditions

    International Nuclear Information System (INIS)

    The IAEA initiated in 1977 a co-ordinated research programme on the ''Evaluation of Solidified High-Level Waste Forms'' which was terminated in 1983. As there was a continuing need for international collaboration in research on solidified high-level waste form and spent fuel, the IAEA initiated a new programme in 1984. The new programme, besides including spent fuel and SYNROC, also placed greater emphasis on the effect of the engineered barriers of future repositories on the properties of the waste form. These engineered barriers included containers, overpacks, buffer and backfill materials etc. as components of the ''near-field'' of the repository. The Co-ordinated Research Programme on the Performance of High-Level Waste Forms and Engineered Barriers Under Repository Conditions had the objectives of promoting the exchange of information on the experience gained by different Member States in experimental performance data and technical model evaluation of solidified high level waste forms, components of the waste package and the complete waste management system under conditions relevant to final repository disposal. The programme includes studies on both irradiated spent fuel and glass and ceramic forms as the final solidified waste forms. The following topics were discussed: Leaching of vitrified high-level wastes, modelling of glass behaviour in clay, salt and granite repositories, environmental impacts of radionuclide release, synroc use for high--level waste solidification, leachate-rock interactions, spent fuel disposal in deep geologic repositories and radionuclide release mechanisms from various fuel types, radiolysis and selective leaching correlated with matrix alteration. Refs, figs and tabs

  12. Process description and plant design for preparing ceramic high-level waste forms

    International Nuclear Information System (INIS)

    The ceramics process flow diagram has been simplified and upgraded to utilize only two major processing steps - fluid-bed calcination and hot isostatic press consolidating. Full-scale fluid-bed calcination has been used at INEL to calcine high-level waste for 18 y; and a second-generation calciner, a fully remotely operated and maintained calciner that meets ALARA guidelines, started calcining high-level waste in 1982. Full-scale hot isostatic consolidation has been used by DOE and commercial enterprises to consolidate radioactive components and to encapsulate spent fuel elements for several years. With further development aimed at process integration and parametric optimization, the operating knowledge of full-scale demonstration of the key process steps should be rapidly adaptable to scale-up of the ceramic process to full plant size. Process flowsheets used to prepare ceramic and glass waste forms from defense and commercial high-level liquid waste are described. Preliminary layouts of process flow diagrams in a high-level processing canyon were prepared and used to estimate the preliminary cost of the plant to fabricate both waste forms. The estimated costs for using both options were compared for total waste management costs of SRP high-level liquid waste. Using our design, for both the ceramic and glass plant, capital and operating costs are essentially the same for both defense and commercial wastes, but total waste management costs are calculated to be significantly less for defense wastes using the ceramic option. It is concluded from this and other studies that the ceramic form may offer important advantages over glass in leach resistance, waste loading, density, and process flexibility. Preliminary economic calculations indicate that ceramics must be considered a leading candidate for the form to immobilize high-level wastes

  13. Performance evaluation of pyrochlore ceramic waste forms by single pass flow through testing

    Science.gov (United States)

    Zhao, P.; Bourcier, W. L.; Esser, B. K.; Shaw, H. F.

    2000-07-01

    Titanate-based ceramic waste forms for the disposal of nuclear wastes have been the subjects of numerous studies over the past decades. In order to assess the performance of this ceramic in a potential Yucca Mountain high-level waste (HLW) repository, it is necessary to understand the kinetics and mechanisms of corrosion of the ceramic under repository conditions. To this end, we are conducting single pass flow-through (SPFT) dissolution tests on ceramics relevant to Pu disposition.

  14. Process description and plant design for preparing ceramic high-level waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Grantham, L.F.; McKisson, R.L.; Guon, J.; Flintoff, J.F.; McKenzie, D.E.

    1983-02-25

    The ceramics process flow diagram has been simplified and upgraded to utilize only two major processing steps - fluid-bed calcination and hot isostatic press consolidating. Full-scale fluid-bed calcination has been used at INEL to calcine high-level waste for 18 y; and a second-generation calciner, a fully remotely operated and maintained calciner that meets ALARA guidelines, started calcining high-level waste in 1982. Full-scale hot isostatic consolidation has been used by DOE and commercial enterprises to consolidate radioactive components and to encapsulate spent fuel elements for several years. With further development aimed at process integration and parametric optimization, the operating knowledge of full-scale demonstration of the key process steps should be rapidly adaptable to scale-up of the ceramic process to full plant size. Process flowsheets used to prepare ceramic and glass waste forms from defense and commercial high-level liquid waste are described. Preliminary layouts of process flow diagrams in a high-level processing canyon were prepared and used to estimate the preliminary cost of the plant to fabricate both waste forms. The estimated costs for using both options were compared for total waste management costs of SRP high-level liquid waste. Using our design, for both the ceramic and glass plant, capital and operating costs are essentially the same for both defense and commercial wastes, but total waste management costs are calculated to be significantly less for defense wastes using the ceramic option. It is concluded from this and other studies that the ceramic form may offer important advantages over glass in leach resistance, waste loading, density, and process flexibility. Preliminary economic calculations indicate that ceramics must be considered a leading candidate for the form to immobilize high-level wastes.

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

    International Nuclear Information System (INIS)

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

  16. 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

  17. Comparative risk assessments for the production and interim storage of glass and ceramic waste forms: defense waste processing facility

    International Nuclear Information System (INIS)

    The Defense Waste Processing Facility (DWPF) for immobilizing nuclear high level waste (HLW) is scheduled to be built at the Savannah River Plant (SRP). High level waste is produced when SRP reactor components are subjected to chemical separation operations. Two candidates for immobilizing this HLW are borosilicate glass and crystalline ceramic, either being contained in weld-sealed stainless steel canisters. A number of technical analyses are being conducted to support a selection between these two waste forms. The present document compares the risks associated with the manufacture and interim storage of these two forms in the DWPF. Process information used in the risk analysis was taken primarily from a DWPF processibility analysis. The DWPF environmental analysis provided much of the necessary environmental information. To perform the comparative risk assessments, consequences of the postulated accidents are calculated in terms of: (1) the maximum dose to an off-site individual; and (2) the dose to off-site population within 80 kilometers of the DWPF, both taken in terms of the 50-year inhalation dose commitment. The consequences are then multiplied by the estimated accident probabilities to obtain the risks. The analyses indicate that the maximum exposure risk to an individual resulting from the accidents postulated for both the production and interim storage of either waste form represents only an insignificant fraction of the natural background radiation of about 90 mrem per year per person in the local area. They also show that there is no disaster potential to the off-site population. Therefore, the risks from abnormal events in the production and the interim storage of the DWPF waste forms should not be considered as a dominant factor in the selection of the final waste form

  18. Molecular environmental science using synchrotron radiation:Chemistry and physics of waste form materials

    Energy Technology Data Exchange (ETDEWEB)

    Lindle, Dennis W.; Shuh, David K.

    2005-02-28

    Production of defense-related nuclear materials has generated large volumes of complex chemical wastes containing a mixture of radionuclides. The disposition of these wastes requires conversion of the liquid and solid-phase components into durable, solid forms suitable for long-term immobilization [1]. Specially formulated glass compositions, many of which have been derived from glass developed for commercial purposes, and ceramics such as pyrochlores and apatites, will be the main recipients for these wastes. The performance characteristics of waste-form glasses and ceramics are largely determined by the loading capacity for the waste constituents (radioactive and non-radioactive) and the resultant chemical and radiation resistance of the waste-form package to leaching (durability). There are unique opportunities for the use of near-edge soft-x-ray absorption fine structure (NEXAFS) spectroscopy to investigate speciation of low-Z elements forming the backbone of waste-form glasses and ceramics. Although nuclear magnetic resonance (NMR) is the primary technique employed to obtain speciation information from low-Z elements in waste forms, NMR is incompatible with the metallic impurities contained in real waste and is thus limited to studies of idealized model systems. In contrast, NEXAFS can yield element-specific speciation information from glass constituents without sensitivity to paramagnetic species. Development and use of NEXAFS for eventual studies of real waste glasses has significant implications, especially for the low-Z elements comprising glass matrices [5-7]. The NEXAFS measurements were performed at Beamline 6.3.1, an entrance-slitless bend-magnet beamline operating from 200 eV to 2000 eV with a Hettrick-Underwood varied-line-space (VLS) grating monochromator, of the Advanced Light Source (ALS) at LBNL. Complete characterization and optimization of this beamline was conducted to enable high-performance measurements.

  19. Waste vitrification: prediction of acceptable compositions in a lime-soda-silica glass-forming system

    International Nuclear Information System (INIS)

    A model is presented based upon calculated bridging oxygens which allows the prediction of the region of acceptable glass compositions for a lime-soda-silica glass-forming system containing mixed waste. The model can be used to guide glass formulation studies (e.g., treatability studies) or assess the applicability of vitrification to candidate waste streams

  20. 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.

  1. Advanced waste form and melter development for treatment of troublesome high-level wastes

    Energy Technology Data Exchange (ETDEWEB)

    Marra, James [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Kim, Dong -Sang [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Maio, Vincent [Idaho National Lab. (INL), Idaho Falls, ID (United States)

    2015-09-02

    A number of waste components in US defense high level radioactive wastes (HLW) have proven challenging for current Joule heated ceramic melter (JHCM) operations and have limited the ability to increase waste loadings beyond already realized levels. Many of these "troublesome" waste species cause crystallization in the glass melt that can negatively impact product quality or have a deleterious effect on melter processing. Recent efforts at US Department of Energy laboratories have focused on understanding crystallization behavior within HLW glass melts and investigating approached to mitigate the impacts of crystallization so that increases in waste loading can be realized. Advanced glass formulations have been developed to highlight the unique benefits of next-generation melter technologies such as the Cold Crucible Induction Melter (CCIM). Crystal-tolerant HLW glasses have been investigated to allow sparingly soluble components such as chromium to crystallize in the melter but pass out of the melter before accumulating.

  2. A Science-based Approach to Development of Durable Waste Forms

    Science.gov (United States)

    Peters, M. T.; Ewing, R. C.

    2006-05-01

    There are two compelling reasons for the importance of understanding the source term and near-field processes in a geologic repository. First, almost all of the radioactivity is initially in the waste form, mainly in the spent nuclear fuel (SNF) or nuclear waste glass. Second, over long periods, after the engineered barriers are no longer important, it is the waste form that controls the release of radioactivity. Thus, it is essential to know the physical and chemical state of the waste form after hundreds of thousands of years. The United States Department of Energy's Yucca Mountain Repository Program has initiated a long-term program to develop a basic understanding of the fundamental mechanisms of radionuclide release and a quantification of the release as repository conditions evolve over time. Specifically, the research program addresses four critical areas: a) SNF dissolution mechanisms and rates; b) formation and properties of U6+- secondary phases; c) waste form-waste package interactions in the near-field; and d) integration of in-package chemical and physical processes. The ultimate goal is to integrate the scientific results into a larger scale model of the source term and near-field processes. This integrated model will be used to provide a basis for understanding the behavior of the source term over long time periods (greater than 100,000 years). Such a fundamental and integrated experimental and modeling approach to source term processes can also be readily applied to development of advanced waste forms as part of a closed nuclear fuel cycle. Specifically, a fundamental understanding of candidate waste form materials stability in high temperature/high radiation environments and near-field geochemical/hydrologic processes could enable development of advanced waste forms "tailored" to specific geologic settings.

  3. Development and testing of matrices for the encapsulation of glass and ceramic nuclear waste forms

    International Nuclear Information System (INIS)

    This report details the results of research on the matrix encapsulation of high level wastes at PML over the past few years. The demonstrations and tests described were designed to illustrate how the waste materials are effected when encapsulated in an inert matrix. Candidate materials evaluated for potential use as matrices for encapslation of pelletized ceramics or glass marbles were categorized into four groups: metals, glasses, ceramics, and graphite. Two processing techniques, casting and hot pressing, were investigated as the most promising methods of formation or densification of the matrices. The major results reported deal with the development aspects. However, chemical durability tests (leach tests) of the matrix materials themselves and matrix-waste form composites are also reported. Matrix waste forms can provide a low porosity, waste-free barrier resulting in increased leach protection, higher impact strength and improved thermal conductivity compared to unencapsulated glass or ceramic waste materials. Glass marbles encapsulated in a lead matrix offer the most significant improvement in waste form stability of all combinations evaluated. This form represents a readily demonstrable process that provides high thermal conductivity, mechanical shock resistance, radiation shielding and increased chemical durability through both a chemical passivation mechanism and as a physical barrier. Other durable matrix waste forms evaluated, applicable primarily to ceramic pellets, involved hot-pressed titanium or TiO2 materials. In the processing of these forms, near 100% dense matrices were obtained. The matrix materials had excellent compatibility with the waste materials and superior potential chemical durability. Cracking of the hot-pressed ceramic matrix forms, in general, prevented the realization of their optimum properties

  4. Fabrication and Pre-irradiation Characterization of a Minor Actinide and Rare Earth Containing Fast Reactor Fuel Experiment for Irradiation in the Advanced Test Reactor

    Energy Technology Data Exchange (ETDEWEB)

    Timothy A. Hyde

    2012-06-01

    The United States Department of Energy, seeks to develop and demonstrate the technologies needed to transmute the long-lived transuranic actinide isotopes contained in spent nuclear fuel into shorter lived fission products, thereby decreasing the volume of material requiring disposal and reducing the long-term radiotoxicity and heat load of high-level waste sent to a geologic repository. This transmutation of the long lived actinides plutonium, neptunium, americium and curium can be accomplished by first separating them from spent Light Water Reactor fuel using a pyro-metalurgical process, then reprocessing them into new fuel with fresh uranium additions, and then transmuted to short lived nuclides in a liquid metal cooled fast reactor. An important component of the technology is developing actinide-bearing fuel forms containing plutonium, neptunium, americium and curium isotopes that meet the stringent requirements of reactor fuels and materials.

  5. Testing and evaluation of solidified high-level waste forms

    International Nuclear Information System (INIS)

    The report describes research by several laboratories on the behaviour, in aqueous and salt environments, of borosilicate glass ceramics proposed for the solidification of nuclear wastes by the European Community. Results were obtained on inactive simulates, doped materials, and on borosilicate glass containing real radioactive waste. The influence of many important parameters were studied: leaching mode, nature of the leachant, pH, pressure, temperature, duration of the treatment, etc. The results of tests lasting for as little as a few hours or for as long as several hundred days, at temperatures up to 2000C or under pressures up to 200 bars, are presented. Numerous analytical techniques (ESCA, EMP, IRR, SEM, etc.) were used to determine the structure and the chemical composition of the altered layer developed by hydration at the glass surface. Information is also given on physical properties of the borosilicate glass: crystallization phase separation, alpha-irradiation stability, mechanical and thermal stability, etc. Finally, preliminary results on the structure and composition of hollandite ceramics are given

  6. Alpha damage in non-reference waste form matrix materials

    International Nuclear Information System (INIS)

    Although bitumen is the matrix material currently used for European α-bearing intermediate level waste streams, polymer and polymer-modified cement matrices could have advantages over bitumen for such wastes. Two organic matrix systems have been studied - an epoxide resin, and an epoxide modified cement. Alpha irradiations were carried out by incorporating 241Am at approx. 0.9 Ci/l. Comparisons have been made with unirradiated material and with materials which had been γ-irradiated to the same dose as the α-irradiated samples. Measurements were made of dimensional changes, mechanical properties and the leaching behaviour of 241Am and 137Cs. A limited amount of swelling (< 3%) was observed in α-irradiated epoxide resin; none was observed in the epoxide modified cement. Gamma irradiation to 300 kGy has no significant effect on the mechanical properties of either system. However, alpha irradiation to the same dose produced significant changes in flexural strength, an increase for the polymer and a decrease for the polymer-cement. Leaching in these systems was found to be a diffusion-controlled process; alpha irradiation to approx. 250 kGy has little effect on the leaching behaviour of either system. (author)

  7. Chemical and Charge Imbalance Induced by Radionuclide Decay: Effects on Waste Form Structure

    Energy Technology Data Exchange (ETDEWEB)

    Van Ginhoven, Renee M.; Jaffe, John E.; Jiang, Weilin; Strachan, Denis M.

    2011-04-01

    This is a milestone document covering the activities to validate theoretical calculations with experimental data for the effect of the decay of 90Sr to 90Zr on materials properties. This was done for a surragate waste form strontium titanate.

  8. Conditioning of radioactive waste solutions by cementation

    International Nuclear Information System (INIS)

    For the cementation of the low and intermediate level evaporator concentrates resulting from the reprocessing of spent fuel numerous experiments were performed to optimize the waste form composition and to characterize the final waste form. Concerning the cementation process, properties of the waste/cement suspension were investigated. These investigations include the dependence of viscosity, bleeding, setting time and hydration heat from the waste cement slurry composition. For the characterization of the waste forms, the mechanical, thermal and chemical stability were determined. For special cases detailed investigations were performed to determine the activity release from waste packages under defined mechanical and thermal stresses. The investigations of the interaction of the waste forms with aqueous solutions include the determination of the Cs/Sr release, the corrosion resistance and the release of actinides. The Cs/Sr release was determined in dependence of the cement type, additives, setting time and sample size. (orig./DG)

  9. Coupling of Nuclear Waste Form Corrosion and Radionuclide Transports in Presence of Relevant Repository Sediments

    Energy Technology Data Exchange (ETDEWEB)

    Wall, Nathalie A. [Washington State Univ., Pullman, WA (United States); Neeway, James J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Qafoku, Nikolla P. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Ryan, Joseph V. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2015-09-30

    Assessments of waste form and disposal options start with the degradation of the waste forms and consequent mobilization of radionuclides. Long-term static tests, single-pass flow-through tests, and the pressurized unsaturated flow test are often employed to study the durability of potential waste forms and to help create models that predict their durability throughout the lifespan of the disposal site. These tests involve the corrosion of the material in the presence of various leachants, with different experimental designs yielding desired information about the behavior of the material. Though these tests have proved instrumental in elucidating various mechanisms responsible for material corrosion, the chemical environment to which the material is subject is often not representative of a potential radioactive waste repository where factors such as pH and leachant composition will be controlled by the near-field environment. Near-field materials include, but are not limited to, the original engineered barriers, their resulting corrosion products, backfill materials, and the natural host rock. For an accurate performance assessment of a nuclear waste repository, realistic waste corrosion experimental data ought to be modeled to allow for a better understanding of waste form corrosion mechanisms and the effect of immediate geochemical environment on these mechanisms. Additionally, the migration of radionuclides in the resulting chemical environment during and after waste form corrosion must be quantified and mechanisms responsible for migrations understood. The goal of this research was to understand the mechanisms responsible for waste form corrosion in the presence of relevant repository sediments to allow for accurate radionuclide migration quantifications. The rationale for this work is that a better understanding of waste form corrosion in relevant systems will enable increased reliance on waste form performance in repository environments and potentially

  10. Coupling of Nuclear Waste Form Corrosion and Radionuclide Transports in Presence of Relevant Repository Sediments

    International Nuclear Information System (INIS)

    Assessments of waste form and disposal options start with the degradation of the waste forms and consequent mobilization of radionuclides. Long-term static tests, single-pass flow-through tests, and the pressurized unsaturated flow test are often employed to study the durability of potential waste forms and to help create models that predict their durability throughout the lifespan of the disposal site. These tests involve the corrosion of the material in the presence of various leachants, with different experimental designs yielding desired information about the behavior of the material. Though these tests have proved instrumental in elucidating various mechanisms responsible for material corrosion, the chemical environment to which the material is subject is often not representative of a potential radioactive waste repository where factors such as pH and leachant composition will be controlled by the near-field environment. Near-field materials include, but are not limited to, the original engineered barriers, their resulting corrosion products, backfill materials, and the natural host rock. For an accurate performance assessment of a nuclear waste repository, realistic waste corrosion experimental data ought to be modeled to allow for a better understanding of waste form corrosion mechanisms and the effect of immediate geochemical environment on these mechanisms. Additionally, the migration of radionuclides in the resulting chemical environment during and after waste form corrosion must be quantified and mechanisms responsible for migrations understood. The goal of this research was to understand the mechanisms responsible for waste form corrosion in the presence of relevant repository sediments to allow for accurate radionuclide migration quantifications. The rationale for this work is that a better understanding of waste form corrosion in relevant systems will enable increased reliance on waste form performance in repository environments and potentially

  11. 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.

  12. EXAFS/XANES studies of plutonium-loaded sodalite/glass waste forms

    International Nuclear Information System (INIS)

    A sodalite/glass ceramic waste form is being developed to immobilize highly radioactive nuclear wastes in chloride form, as part of an electrochemical cleanup process. Two types of simulated waste forms were studied: where the plutonium was alone in an LiCl/KCl matrix and where simulated fission-product elements were added representative of the electrometallurgical treatment process used to recover uranium from spent nuclear fuel also containing plutonium and a variety of fission products. Extended X-ray absorption fine structure spectroscopy (EXAFS) and X-ray absorption near-edge spectroscopy (XANES) studies were performed to determine the location, oxidation state, and particle size of the plutonium within these waste form samples. Plutonium was found to segregate as plutonium(IV) oxide with a crystallite size of at least 4.8 nm in the non-fission-element case and 1.3 nm with fission elements present. No plutonium was observed within the sodalite in the waste form made from the plutonium-loaded LiCl/KCl eutectic salt. Up to 35% of the plutonium in the waste form made from the plutonium-loaded simulated fission-product salt may be segregated with a heavy-element nearest neighbor other than plutonium or occluded internally within the sodalite lattice

  13. EXAFS/XANES studies of plutonium-loaded sodalite/glass waste forms

    Science.gov (United States)

    Richmann, Michael K.; Reed, Donald T.; Kropf, A. Jeremy; Aase, Scott B.; Lewis, Michele A.

    2001-09-01

    A sodalite/glass ceramic waste form is being developed to immobilize highly radioactive nuclear wastes in chloride form, as part of an electrochemical cleanup process. Two types of simulated waste forms were studied: where the plutonium was alone in an LiCl/KCl matrix and where simulated fission-product elements were added representative of the electrometallurgical treatment process used to recover uranium from spent nuclear fuel also containing plutonium and a variety of fission products. Extended X-ray absorption fine structure spectroscopy (EXAFS) and X-ray absorption near-edge spectroscopy (XANES) studies were performed to determine the location, oxidation state, and particle size of the plutonium within these waste form samples. Plutonium was found to segregate as plutonium(IV) oxide with a crystallite size of at least 4.8 nm in the non-fission-element case and 1.3 nm with fission elements present. No plutonium was observed within the sodalite in the waste form made from the plutonium-loaded LiCl/KCl eutectic salt. Up to 35% of the plutonium in the waste form made from the plutonium-loaded simulated fission-product salt may be segregated with a heavy-element nearest neighbor other than plutonium or occluded internally within the sodalite lattice.

  14. Summary of Uranium Solubility Studies in Concrete Waste Forms and Vadose Zone Environments

    Energy Technology Data Exchange (ETDEWEB)

    Golovich, Elizabeth C.; Wellman, Dawn M.; Serne, R. Jeffrey; Bovaird, Chase C.

    2011-09-30

    One of the methods being considered for safely disposing of Category 3 low-level radioactive wastes is to encase the waste in concrete. Concrete encasement would contain and isolate the waste packages from the hydrologic environment and act as an intrusion barrier. The current plan for waste isolation consists of stacking low-level waste packages on a trench floor, surrounding the stacks with reinforced steel, and encasing these packages in concrete. These concrete-encased waste stacks are expected to vary in size with maximum dimensions of 6.4 m long, 2.7 m wide, and 4 m high. The waste stacks are expected to have a surrounding minimum thickness of 15 cm of concrete encasement. These concrete-encased waste packages are expected to withstand environmental exposure (solar radiation, temperature variations, and precipitation) until an interim soil cover or permanent closure cover is installed and to remain largely intact thereafter. Any failure of concrete encasement may result in water intrusion and consequent mobilization of radionuclides from the waste packages. This report presents the results of investigations elucidating the uranium mineral phases controlling the long-term fate of uranium within concrete waste forms and the solubility of these phases in concrete pore waters and alkaline, circum-neutral vadose zone environments.

  15. Leaching tests of simulated Cogema bituminized waste form

    Energy Technology Data Exchange (ETDEWEB)

    Nakayama, S.; Akimoto, T.; Iida, Y.; Nagano, T. [Japan Atomic Energy Research Institute, Tokai, Ibaraki (Japan)

    2000-07-01

    The leaching behavior of COGEMA-type bituminized radioactive waste was studied for the atmospheric and anaerobic conditions. Active and inactive laboratory-scale bitumen samples, including two major salts of NaNO{sub 3} and BaSO{sub 4}, were contacted with deionized water, an alkaline solution (0.01 mol/L Ca(OH){sub 2} or 0.03 mol/L KOH), or a saline solution (0.5 mol/L KCl). It was found that the release of salt was reduced in the Ca(OH){sub 2} solution compared with deionized water under the atmospheric conditions. No significant difference in the concentrations of {sup 237}Np in leachants contacted with the samples for 7 days was observed between the atmospheric and the anaerobic conditions. (authors)

  16. Forming of information support for estimate of potential danger of storage points of the decontamination wastes

    International Nuclear Information System (INIS)

    By now 92 storage points of the decontamination wastes that formed in result of decontamination of settlements after the Chernobyl accident is registered on the territory of Belarus. The most of theirs were placed in the unfavorable for storage of radioactive wastes places. It was examine the forming of information support for estimate of potential danger of the storage points of decontamination wastes that base on results of investigations of objects, field and laboratory investigations, theoretical researches, using of literary information about features of radionuclides migration through engineering and natural barriers to water-bearing horizon is examination

  17. Materials Characterization Center meeting on impact testing of waste forms. Summary report

    International Nuclear Information System (INIS)

    A meeting was held on March 25-26, 1981 to discuss impact test methods for waste form materials to be used in nuclear waste repositories. The purpose of the meeting was to obtain guidance for the Materials Characterization Center (MCC) in preparing the MCC-10 Impact Test Method to be approved by the Materials Review Board. The meeting focused on two essential aspects of the test method, namely the mechanical process, or impact, used to effect rapid fracture of a waste form and the analysis technique(s) used to characterize particulates generated by the impact

  18. Comparison of mechanical properties of glass-bonded sodalite and borosilicate glass high-level waste forms

    Energy Technology Data Exchange (ETDEWEB)

    O' Holleran, T. P.; DiSanto, T.; Johnson, S. G.; Goff, K. M.

    2000-05-09

    Argonne National Laboratory has developed a glass-bonded sodalite waste form to immobilize the salt waste stream from electrometallurgical treatment of spent nuclear fuel. The waste form consists of 75 vol.% crystalline sodalite and 25 vol.% glass. Microindentation fracture toughness measurements were performed on this material and borosilicate glass from the Defense Waste Processing Facility using a Vickers indenter. Palmqvist cracking was confined for the glass-bonded sodalite waste form, while median-radial cracking occurred in the borosilicate glass. The elastic modulus was measured by an acoustic technique. Fracture toughness, microhardness, and elastic modulus values are reported for both waste forms.

  19. Continuous-flow leach testing method for various nuclear waste forms

    International Nuclear Information System (INIS)

    Nuclear waste is planned to be buried in deep geological repositories. If these repositories were ever invaded by ground water, the waste form could be corroded and the nuclear waste released to the surrounding geologic medium. The rate at which this flowing ground water corrodes the waste form can be studied using the Lawrence Livermore National Laboratory's single-pass continuous-flow leaching test. This repository-relevant leaching test places the waste form of interest into a flowing stream of leachant. The flow rates can be set to approximate the low flow rates encountered in actual aquifers. The leachant contacts the waste only once and then exits the cell where it is collected and analyzed. Such a scheme avoids potential solution saturation problems encountered with static tests. The composition of leachants used with this test has ranged from saturated salt brine to distilled water. Temperature has been varied from 250C to 750C. These values cover the range of ambient temperatures expected at depths of 2 to 3 km. This test was designed to reproduce conditions of a flooded repository in the laboratory. The testing methodology is discussed as well as examples of data obtained from leaching a variety of waste forms under various conditions

  20. DEVELOPMENT QUALIFICATION AND DISPOSAL OF AN ALTERNATIVE IMMOBILIZED LOW-ACTIVITY WASTE FORM AT THE HANFORD SITE

    Energy Technology Data Exchange (ETDEWEB)

    SAMS TL; EDGE JA; SWANBERG DJ; ROBBINS RA

    2011-01-13

    Demonstrating that a waste form produced by a given immobilization process is chemically and physically durable as well as compliant with disposal facility acceptance criteria is critical to the success of a waste treatment program, and must be pursued in conjunction with the maturation of the waste processing technology. Testing of waste forms produced using differing scales of processing units and classes of feeds (simulants versus actual waste) is the crux of the waste form qualification process. Testing is typically focused on leachability of constituents of concern (COCs), as well as chemical and physical durability of the waste form. A principal challenge regarding testing immobilized low-activity waste (ILAW) forms is the absence of a standard test suite or set of mandatory parameters against which waste forms may be tested, compared, and qualified for acceptance in existing and proposed nuclear waste disposal sites at Hanford and across the Department of Energy (DOE) complex. A coherent and widely applicable compliance strategy to support characterization and disposal of new waste forms is essential to enhance and accelerate the remediation of DOE tank waste. This paper provides a background summary of important entities, regulations, and considerations for nuclear waste form qualification and disposal. Against this backdrop, this paper describes a strategy for meeting and demonstrating compliance with disposal requirements emphasizing the River Protection Project (RPP) Integrated Disposal Facility (IDF) at the Hanford Site and the fluidized bed steam reforming (FBSR) mineralized low-activity waste (LAW) product stream.

  1. DEVELOPMENT, QUALIFICATION, AND DISPOSAL OF AN ALTERNATIVE IMMOBILIZED LOW-ACTIVITY WASTE FORM AT THE HANFORD SITE

    International Nuclear Information System (INIS)

    Demonstrating that a waste form produced by a given immobilization process is chemically and physically durable as well as compliant with disposal facility acceptance criteria is critical to the success of a waste treatment program, and must be pursued in conjunction with the maturation of the waste processing technology. Testing of waste forms produced using differing scales of processing units and classes of feeds (simulants versus actual waste) is the crux of the waste form qualification process. Testing is typically focused on leachability of constituents of concern (COCs), as well as chemical and physical durability of the waste form. A principal challenge regarding testing immobilized low-activity waste (ILAW) forms is the absence of a standard test suite or set of mandatory parameters against which waste forms may be tested, compared, and qualified for acceptance in existing and proposed nuclear waste disposal sites at Hanford and across the Department of Energy (DOE) complex. A coherent and widely applicable compliance strategy to support characterization and disposal of new waste forms is essential to enhance and accelerate the remediation of DOE tank waste. This paper provides a background summary of important entities, regulations, and considerations for nuclear waste form qualification and disposal. Against this backdrop, this paper describes a strategy for meeting and demonstrating compliance with disposal requirements emphasizing the River Protection Project (RPP) Integrated Disposal Facility (IDF) at the Hanford Site and the fluidized bed steam reforming (FBSR) mineralized low-activity waste (LAW) product stream.

  2. 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.

  3. Vitrified municipal waste as a host form for high-level nuclear waste

    International Nuclear Information System (INIS)

    Preparing glass to be used as a radioactive waste immobilizer from municipal waste is the aim of this paper. Up to 90 wt% of municipal waste was obtained by burning the raw waste at 700 deg C for 5 h; this were successfully vitrified into borosilicate and sodium borate glasses at ∼1,200 deg C. The long term behavior of such glass is one of the most important factors, which is determined by their durability in aqueous solution. Experimental durability data of the prepared glass immersed in ground water together with γ-irradiation was found to be affected according to the different irradiation doses. In addition, thermal analysis and glass surface morphology were investigated. The evolution of the damage on the studied properties was correlated to the changes in the glass network depending on their composition and irradiation dose. The results showed that glass matrix containing higher amount of municipal waste possess high durability and low thermal expansion after being gamma irradiated. The results showed that glass containing higher amount of municipal waste possess high durability and low thermal expansion after irradiation. (author)

  4. A Glass-Ceramic Waste Forms for the Immobilization of Rare Earth Oxides from the Pyroprocessing Waste salt

    Energy Technology Data Exchange (ETDEWEB)

    Ahn, Byung-Gil; Park, Hwan-Seo; Kim, Hwan-Young; Kim, In-Tae [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

    2008-05-15

    The fission product of rare earth (RE) oxide wastes are generates during the pyroprocess . Borosilicate glass or some ceramic materials such as monazite, apatite or sodium zirconium phosphate (NZP) have been a prospective host matrix through lots of experimental results. Silicate glasses have long been the preferred waste form for the immobilization of HLW. In immobilization of the RE oxides, the developed process on an industrial scale involves their incorporation into a glass matrix, by melting under 1200 {approx} 1300 .deg. C. Instead of the melting process, glass powder sintering is lower temperature ({approx} 900 .deg. C) required for the process which implies less demanding conditions for the equipment and a less evaporation of volatile radionuclides. This study reports the behaviors, direct vitrification of RE oxides with glass frit, glass powder sintering of REceramic with glass frit, formation of RE-apatite (or REmonazite) ceramic according to reaction temperature, and the leach resistance of the solidified waste forms.

  5. Use of tetraaza-macrocycles for complexation of actinides in aqueous solutions. Validation of the process for the treatment of waste waters

    International Nuclear Information System (INIS)

    This report makes one's contribution to the study of the reactivity of free or fixed tetraaza-macrocycles. The major interest of this work concerns the following key-points: - Synthesis, spectral characterization and X-ray diffraction study of tetraaza-macrocycles N-tetra-functionalized, - Synthesis, physicochemical, chemicals and X-ray studies of macrocyclic complex in lanthanides and actinides series, - Synthesis and characterization of tetraaza-macrocycles grafted on organic and inorganic polymers, - Reactivity of macrocyclic ligands grafted on Merrifield's resin or silica gel in cerium, europium, uranium, plutonium and americium series, - Extraction of heavy metals in a solid-liquid process and measurements of a pilot. (author)

  6. Computational Efficient Upscaling Methodology for Predicting Thermal Conductivity of Nuclear Waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Li, Dongsheng; Sun, Xin; Khaleel, Mohammad A.

    2011-09-28

    This study evaluated different upscaling methods to predict thermal conductivity in loaded nuclear waste form, a heterogeneous material system. The efficiency and accuracy of these methods were compared. Thermal conductivity in loaded nuclear waste form is an important property specific to scientific researchers, in waste form Integrated performance and safety code (IPSC). The effective thermal conductivity obtained from microstructure information and local thermal conductivity of different components is critical in predicting the life and performance of waste form during storage. How the heat generated during storage is directly related to thermal conductivity, which in turn determining the mechanical deformation behavior, corrosion resistance and aging performance. Several methods, including the Taylor model, Sachs model, self-consistent model, and statistical upscaling models were developed and implemented. Due to the absence of experimental data, prediction results from finite element method (FEM) were used as reference to determine the accuracy of different upscaling models. Micrographs from different loading of nuclear waste were used in the prediction of thermal conductivity. Prediction results demonstrated that in term of efficiency, boundary models (Taylor and Sachs model) are better than self consistent model, statistical upscaling method and FEM. Balancing the computation resource and accuracy, statistical upscaling is a computational efficient method in predicting effective thermal conductivity for nuclear waste form.

  7. Crichtonite structure type (AM21O38 and A2M19O36) as a host phase in crystalline waste form ceramics

    International Nuclear Information System (INIS)

    Previous studies of ceramic crystalline waste forms, e.g. Synroc, tailored ceramics, and supercalcine, have concentrated on phases which are major constituents in the formulations: zirconolite, pyrochlore, hollandite, perovskite and zircon. These phases usually occur as members of multi-phase assemblages which are required for the incorporation of the wide variety of radionuclide elements present in the waste and the non-radioactive components added during reprocessing and pretreatment. The crichtonite structure (AM21O38 and A2M19O36), based on crystallo-chemical considerations and natural compositional analogues, may effectively incorporate both fission products and actinides. The naturally occurring crichtonite structure types include Sr (crichtonite), Ca and REE (loveringite), Na (landauite), REE and U (davidite), K (mathiasite), Ba (lindsleyite), and Pb (senaite), which are classified based on the dominant, large cations occupying the A-site. The crystal structure contains three types of sites of distinct size, from very large, M0, intermediate (M1, M3, M4, and M5), to small (M2). Numerous coupled substitutions within these cation sites allow for charge balance. Synthesis experiments were completed on the Ba-, Sr-, Ca-, and K-member compositions at 3 GPa and 1,150 C. Low pressure synthesis should be possible, as natural minerals mostly occur in low-P systems. Reaction products were characterized by powder X-ray diffraction, scanning electron microscopy and electron microprobe analysis. In addition to the crichtonite phases, rutile, spinel, perovskite and armacolite were identified as well. The Crichtonite structure type is estimated to accommodate waste loading of up to 30 wt. % PW-4B waste

  8. 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

  9. 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.

  10. Properties of SYNROC-D nuclear waste form: a state-of-the-art reivew

    International Nuclear Information System (INIS)

    SYNROC is a titanate-based ceramic waste form being developed to immobilize high-level nuclear reactor wastes. SYNROC-D is a unique variation of SYNROC designed to contain high-level defense wastes, particularly those in storage at the Savannah River Plant (SRP). In this report, we review results from physical property and performance tests on SYNROC-D containing simulated SRP wastes. These results provide a data base for comparing SYNROC-D with other defense waste forms. The test data are grouped into three categories: (1) waste loading, (2) mechanical and thermal properties, (3) leach resistance. We also examine the possible effects of radiation damage on SYNROC during long-term storage in a geologic repository. The test data were collected from a series of SYNROC-D samples prepared as part of a comparative testing program initiated by Savannah River Laboratory. These samples were prepared by conventional ceramic hot-pressing techniques and then characterized by x-ray diffraction, scanning electron microscopy and electron microprobe analysis. Whenever possible, standardized test procedures were used for evaluating the waste form properties. For example, leach rates were measured using the Material Characterization Center's (MCC) standard MCC-1 and MCC-2 tests. 66 references

  11. Transuranic and Low-Level Boxed Waste Form Nondestructive Assay Technology Overview and Assessment

    International Nuclear Information System (INIS)

    The Mixed Waste Focus Area (MWFA) identified the need to perform an assessment of the functionality and performance of existing nondestructive assay (NDA) techniques relative to the low-level and transuranic waste inventory packaged in large-volume box-type containers. The primary objectives of this assessment were to: (1) determine the capability of existing boxed waste form NDA technology to comply with applicable waste radiological characterization requirements, (2) determine deficiencies associated with existing boxed waste assay technology implementation strategies, and (3) recommend a path forward for future technology development activities, if required. Based on this assessment, it is recommended that a boxed waste NDA development and demonstration project that expands the existing boxed waste NDA capability to accommodate the indicated deficiency set be implemented. To ensure that technology will be commercially available in a timely fashion, it is recommended this development and demonstration project be directed to the private sector. It is further recommended that the box NDA technology be of an innovative design incorporating sufficient NDA modalities, e.g., passive neutron, gamma, etc., to address the majority of the boxed waste inventory. The overall design should be modular such that subsets of the overall NDA system can be combined in optimal configurations tailored to differing waste types

  12. Evaluation of final waste forms and recommendations for baseline alternatives to group and glass

    Energy Technology Data Exchange (ETDEWEB)

    Bleier, A.

    1997-09-01

    An assessment of final waste forms was made as part of the Federal Facilities Compliance Agreement/Development, Demonstration, Testing, and Evaluation (FFCA/DDT&E) Program because supplemental waste-form technologies are needed for the hazardous, radioactive, and mixed wastes of concern to the Department of Energy and the problematic wastes on the Oak Ridge Reservation. The principal objective was to identify a primary waste-form candidate as an alternative to grout (cement) and glass. The effort principally comprised a literature search, the goal of which was to establish a knowledge base regarding four areas: (1) the waste-form technologies based on grout and glass, (2) candidate alternatives, (3) the wastes that need to be immobilized, and (4) the technical and regulatory constraints on the waste-from technologies. This report serves, in part, to meet this goal. Six families of materials emerged as relevant; inorganic, organic, vitrified, devitrified, ceramic, and metallic matrices. Multiple members of each family were assessed, emphasizing the materials-oriented factors and accounting for the fact that the two most prevalent types of wastes for the FFCA/DDT&E Program are aqueous liquids and inorganic sludges and solids. Presently, no individual matrix is sufficiently developed to permit its immediate implementation as a baseline alternative. Three thermoplastic materials, sulfur-polymer cement (inorganic), bitumen (organic), and polyethylene (organic), are the most technologically developed candidates. Each warrants further study, emphasizing the engineering and economic factors, but each also has limitations that regulate it to a status of short-term alternative. The crystallinity and flexible processing of sulfur provide sulfur-polymer cement with the highest potential for short-term success via encapsulation. Long-term immobilization demands chemical stabilization, which the thermoplastic matrices do not offer. Among the properties of the remaining

  13. Evaluation of final waste forms and recommendations for baseline alternatives to grout and glass

    International Nuclear Information System (INIS)

    An assessment of final waste forms was made as part of the Federal Facilities Compliance Agreement/Development, Demonstration, Testing, and Evaluation (FFCA/DDT ampersand E) Program because supplemental waste-form technologies are needed for the hazardous, radioactive, and mixed wastes of concern to the Department of Energy and the problematic wastes on the Oak Ridge Reservation. The principal objective was to identify a primary waste-form candidate as an alternative to grout (cement) and glass. The effort principally comprised a literature search, the goal of which was to establish a knowledge base regarding four areas: (1) the waste-form technologies based on grout and glass, (2) candidate alternatives, (3) the wastes that need to be immobilized, and (4) the technical and regulatory constraints on the waste-from technologies. This report serves, in part, to meet this goal. Six families of materials emerged as relevant; inorganic, organic, vitrified, devitrified, ceramic, and metallic matrices. Multiple members of each family were assessed, emphasizing the materials-oriented factors and accounting for the fact that the two most prevalent types of wastes for the FFCA/DDT ampersand E Program are aqueous liquids and inorganic sludges and solids. Presently, no individual matrix is sufficiently developed to permit its immediate implementation as a baseline alternative. Three thermoplastic materials, sulfur-polymer cement (inorganic), bitumen (organic), and polyethylene (organic), are the most technologically developed candidates. Each warrants further study, emphasizing the engineering and economic factors, but each also has limitations that regulate it to a status of short-term alternative. The crystallinity and flexible processing of sulfur provide sulfur-polymer cement with the highest potential for short-term success via encapsulation. Long-term immobilization demands chemical stabilization, which the thermoplastic matrices do not offer. Among the properties of the

  14. Actinide partitioning and recovery of valuables from HLW

    International Nuclear Information System (INIS)

    The Indian nuclear power programme is sustained by adoption of a closed fuel cycle where in the fissile and fertile materials are recycled by reprocessing of spent fuel. The reprocessing step leads to the generation of high level waste which is presently vitrified using borosilicate matrices. With the nuclear power profile on the brink of an exponential increase, it becomes imperative to consider and adopt cross-cut technologies that would not only lead to a substantial reduction in repository capacity both in terms of volumes and thermal loads but also lead to a reduction in radiotoxicity of the waste forms. Partitioning of high level waste (HLW) is the first step towards achieving the above objectives. Developmental efforts in the last decade have placed partitioning of high level waste in the realms of practical application. This paper will present a compilation of various R and D efforts on development of processes and technologies under consideration for partitioning of high level waste in the Indian context. While numerous laboratory trials are being pursued, some of them which have matured for plant scale demonstration are related to partitioning of actinides from acidic high level waste and recovery of cesium and strontium from high level waste. A structured R and D framework has been worked out to develop deployable processes and technologies for their demonstration on engineering scale. One of the most defining step in this work is selection of potentially successful extraction system based on the systematic study on the extraction properties and their optimization for full scale studies. (author)

  15. Characteristics of high-level radioactive waste forms for their disposal

    International Nuclear Information System (INIS)

    In order to develop a deep geological repository for a high-level radioactive waste coming from reprocessing of spent nuclear fuels discharged from our domestic nuclear power plants, the the required characteristics of waste form are dependent upon a solidifying medium and the amount of waste loading in the medium. And so, by the comparative analysis of the characteristics of various waste forms developed up to the present, a suitable medium is recommended.The overall characteristics of the latter is much better than those of the former, but the change of the properties due to an amorphysation by radiation exposure and its thermal expansion has not been clearly identified yet. And its process has not been commercialized. However, the overall properties of the borosilicate glass waste forms are acceptable for their disposal, their production cost is reasonable and their processes have already been commercialized. And plenty informations of their characteristics and operational experiences have been accumulated. Consequently, it is recommended that a suitable medium solidifying the HLW is a borosilicate glass and its composition for the identification of a reference waste form would be based on the glass frit of R7T7

  16. Characteristics of high-level radioactive waste forms for their disposal

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Seung Soo; Chun, Kwan Sik; Kang, Chul Hyung

    2000-12-01

    In order to develop a deep geological repository for a high-level radioactive waste coming from reprocessing of spent nuclear fuels discharged from our domestic nuclear power plants, the the required characteristics of waste form are dependent upon a solidifying medium and the amount of waste loading in the medium. And so, by the comparative analysis of the characteristics of various waste forms developed up to the present, a suitable medium is recommended.The overall characteristics of the latter is much better than those of the former, but the change of the properties due to an amorphysation by radiation exposure and its thermal expansion has not been clearly identified yet. And its process has not been commercialized. However, the overall properties of the borosilicate glass waste forms are acceptable for their disposal, their production cost is reasonable and their processes have already been commercialized. And plenty informations of their characteristics and operational experiences have been accumulated. Consequently, it is recommended that a suitable medium solidifying the HLW is a borosilicate glass and its composition for the identification of a reference waste form would be based on the glass frit of R7T7.

  17. Evaluation of low and intermediate level radioactive solidified waste forms and packages

    International Nuclear Information System (INIS)

    Evaluation of low and intermediate level radioactive waste forms and packages with respect to compliance with quality and safety requirements for transport, interim storage and disposal has become a very important part of the radioactive waste management strategy in many countries. The evaluation of waste forms and packages provides precise basic data for regulatory bodies to establish safety requirements, and implement quality control and quality assurance procedures for radioactive waste management programmes. The requirements depend very much upon the disposal option selected, treatment technology used, waste form characteristics, package quality and other factors. The regulatory requirements can also influence the methodology of waste form/package evaluation together with selection and analysis of data for quality control and safety assurance. A coordinated research programme started at the end of 1985 and brought together 12 participants from 11 countries. The results of the programme and each particular project were discussed at three Research Coordination Meetings held in Cairo, Egypt, in May, 1986; in Beijing, China, in April, 1998; and at Harwell Laboratory, United Kingdom, in November, 1989. This document summarises the salient features and results achieved during the four year investigation and a recommendation for future work in this area. Refs, figs and tabs

  18. Preliminary Waste Form Compliance Plan for the Idaho National Engineering and Environmental Laboratory High-Level Waste

    Energy Technology Data Exchange (ETDEWEB)

    B. A. Staples; T. P. O' Holleran

    1999-05-01

    The Department of Energy (DOE) has specific technical and documentation requirements for high-level waste (HLW) that is to be placed in a federal repository. This document describes in general terms the strategy to be used at the Idaho National Engineering and Environmental Laboratory (INEEL) to demonstrate that vitrified HLW, if produced at the INEEL, meets these requirements. Waste form, canister, quality assurance, and documentation specifications are discussed. Compliance strategy is given, followed by an overview of how this strategy would be implemented for each specification.

  19. RADIOACTIVE DEMONSTRATION OF FINAL MINERALIZED WASTE FORMS FOR HANFORD WASTE TREATMENT PLANT SECONDARY WASTE BY FLUIDIZED BED STEAM REFORMING USING THE BENCH SCALE REFORMER PLATFORM

    Energy Technology Data Exchange (ETDEWEB)

    Crawford, C.; Burket, P.; Cozzi, A.; Daniel, W.; Jantzen, C.; Missimer, D.

    2012-02-02

    ceramic (mineral) waste form. The mineral waste form that is produced by co-processing waste with kaolin clay in an FBSR process has been shown to be as durable as LAW glass. Monolithing of the granular FBSR product is being investigated to prevent dispersion during transport or burial/storage, but is not necessary for performance. A Benchscale Steam Reformer (BSR) was designed and constructed at the SRNL to treat actual radioactive wastes to confirm the findings of the non-radioactive FBSR pilot scale tests and to qualify the waste form for applications at Hanford. BSR testing with WTP SW waste surrogates and associated analytical analyses and tests of granular products (GP) and monoliths began in the Fall of 2009, and then was continued from the Fall of 2010 through the Spring of 2011. Radioactive testing commenced in 2010 with a demonstration of Hanford's WTP-SW where Savannah River Site (SRS) High Level Waste (HLW) secondary waste from the Defense Waste Processing Facility (DWPF) was shimmed with a mixture of {sup 125/129}I and {sup 99}Tc to chemically resemble WTP-SW. Prior to these radioactive feed tests, non-radioactive simulants were also processed. Ninety six grams of radioactive granular product were made for testing and comparison to the non-radioactive pilot scale tests. The same mineral phases were found in the radioactive and non-radioactive testing.

  20. FY16 Annual Accomplishments - Waste Form Development and Performance: Evaluation Of Ceramic Waste Forms - Comparison Of Hot Isostatic Pressed And Melt Processed Fabrication Methods

    Energy Technology Data Exchange (ETDEWEB)

    Amoroso, J. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Dandeneau, C. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2016-10-13

    FY16 efforts were focused on direct comparison of multi-phase ceramic waste forms produced via melt processing and HIP methods. Based on promising waste form compositions previously devised at SRNL[13], simulant material was prepared at SRNL and a portion was sent to the Australian Nuclear Science and Technology Organization (ANSTO) for HIP treatments, while the remainder of the material was melt processed at SRNL. The microstructure, phase formation, elemental speciation, and leach behavior, and radiation stability of the fabricated ceramics was performed. In addition, melt-processed ceramics designed with different fractions of hollandite, zirconolite, perovskite, and pyrochlore phases were investigated. for performance and properties. Table 1 lists the samples studied.

  1. Waste-Form Development Program. Annual progress report, October 1981-September 1982

    Energy Technology Data Exchange (ETDEWEB)

    Neilson, R.M. Jr.; Colombo, P.

    1982-09-01

    Low-level wastes (LLW) at nuclear facilities have traditionally been solidified using portland cement (with and without additives). Urea-formaldehyde has been used for LLW solidification while bitumen (asphalt) and thermosetting polymers will be applied to domestic wastes in the near future. Operational difficulties have been observed with each of these solidification agents. Such difficulties include incompatibility with waste constitutents inhibiting solidification, premature setting, free standing water and fires. Some specific waste types have proven difficult to solidify with one or more of the contemporary agents. Similar problems are also anticipated for the solidification of new wastes, which are generated using advanced volume reduction technologies, and with the application of additional agents which may be introduced in the near future for the solidification of LLW. In the Waste Form Development program, contemporary solidification agents are being investigated relative to their potential applications to major fuel cycle and non-fuel cycle LLW streams. The range of conditions under which these solidification agents can be satisfactorily applied to specific LLW streams is being determined. These studies are primarily directed towards defining operating parameters for both improved solidification of problem wastes such as ion exchange resins, organic liquids and oils for which prevailing processes, as currently employed, appear to be inadequate, and solidification of new LLW streams including high solids content evaporator concentrates, dry solids, and incinerator ash generated from advanced volume reduction technologies. Solidified waste forms are tested and evaluated to demonstrate compliance with waste form performance and shallow land burial (SLB) acceptance criteria and transportation requirements (both as they currently exist and as they are anticipated to be modified with time).

  2. Waste-Form Development Program. Annual progress report, October 1981-September 1982

    International Nuclear Information System (INIS)

    Low-level wastes (LLW) at nuclear facilities have traditionally been solidified using portland cement (with and without additives). Urea-formaldehyde has been used for LLW solidification while bitumen (asphalt) and thermosetting polymers will be applied to domestic wastes in the near future. Operational difficulties have been observed with each of these solidification agents. Such difficulties include incompatibility with waste constitutents inhibiting solidification, premature setting, free standing water and fires. Some specific waste types have proven difficult to solidify with one or more of the contemporary agents. Similar problems are also anticipated for the solidification of new wastes, which are generated using advanced volume reduction technologies, and with the application of additional agents which may be introduced in the near future for the solidification of LLW. In the Waste Form Development program, contemporary solidification agents are being investigated relative to their potential applications to major fuel cycle and non-fuel cycle LLW streams. The range of conditions under which these solidification agents can be satisfactorily applied to specific LLW streams is being determined. These studies are primarily directed towards defining operating parameters for both improved solidification of problem wastes such as ion exchange resins, organic liquids and oils for which prevailing processes, as currently employed, appear to be inadequate, and solidification of new LLW streams including high solids content evaporator concentrates, dry solids, and incinerator ash generated from advanced volume reduction technologies. Solidified waste forms are tested and evaluated to demonstrate compliance with waste form performance and shallow land burial (SLB) acceptance criteria and transportation requirements (both as they currently exist and as they are anticipated to be modified with time)

  3. Fracture toughness measurements on a glass bonded sodalite high-level waste form.

    Energy Technology Data Exchange (ETDEWEB)

    DiSanto, T.; Goff, K. M.; Johnson, S. G.; O' Holleran, T. P.

    1999-05-19

    The electrometallurgical treatment of metallic spent nuclear fuel produces two high-level waste streams; cladding hulls and chloride salt. Argonne National Laboratory is developing a glass bonded sodalite waste form to immobilize the salt waste stream. The waste form consists of 75 Vol.% crystalline sodalite (containing the salt) with 25 Vol.% of an ''intergranular'' glassy phase. Microindentation fracture toughness measurements were performed on representative samples of this material using a Vickers indenter. Palmqvist cracking was confirmed by post-indentation polishing of a test sample. Young's modulus was measured by an acoustic technique. Fracture toughness, microhardness, and Young's modulus values are reported, along with results from scanning electron microscopy studies.

  4. Final waste forms project: Performance criteria for phase I treatability studies

    International Nuclear Information System (INIS)

    This document defines the product performance criteria to be used in Phase I of the Final Waste Forms Project. In Phase I, treatability studies will be performed to provide open-quotes proof-of-principleclose quotes data to establish the viability of stabilization/solidification (S/S) technologies. This information is required by March 1995. In Phase II, further treatability studies, some at the pilot scale, will be performed to provide sufficient data to allow treatment alternatives identified in Phase I to be more fully developed and evaluated, as well as to reduce performance uncertainties for those methods chosen to treat a specific waste. Three main factors influence the development and selection of an optimum waste form formulation and hence affect selection of performance criteria. These factors are regulatory, process-specific, and site-specific waste form standards or requirements. Clearly, the optimum waste form formulation will require consideration of performance criteria constraints from each of the three categories. Phase I will focus only on the regulatory criteria. These criteria may be considered the minimum criteria for an acceptable waste form. In other words, a S/S technology is considered viable only if it meet applicable regulatory criteria. The criteria to be utilized in the Phase I treatability studies were primarily taken from Environmental Protection Agency regulations addressed in 40 CFR 260 through 265 and 268; and Nuclear Regulatory Commission regulations addressed in 10 CFR 61. Thus the majority of the identified criteria are independent of waste form matrix composition (i.e., applicable to cement, glass, organic binders etc.)

  5. Final waste forms project: Performance criteria for phase I treatability studies

    Energy Technology Data Exchange (ETDEWEB)

    Gilliam, T.M. [Oak Ridge National Lab., TN (United States); Hutchins, D.A. [Martin Marietta Energy Systems, Inc., Oak Ridge, TN (United States); Chodak, P. III [Massachusetts Institute of Technology (United States)

    1994-06-01

    This document defines the product performance criteria to be used in Phase I of the Final Waste Forms Project. In Phase I, treatability studies will be performed to provide {open_quotes}proof-of-principle{close_quotes} data to establish the viability of stabilization/solidification (S/S) technologies. This information is required by March 1995. In Phase II, further treatability studies, some at the pilot scale, will be performed to provide sufficient data to allow treatment alternatives identified in Phase I to be more fully developed and evaluated, as well as to reduce performance uncertainties for those methods chosen to treat a specific waste. Three main factors influence the development and selection of an optimum waste form formulation and hence affect selection of performance criteria. These factors are regulatory, process-specific, and site-specific waste form standards or requirements. Clearly, the optimum waste form formulation will require consideration of performance criteria constraints from each of the three categories. Phase I will focus only on the regulatory criteria. These criteria may be considered the minimum criteria for an acceptable waste form. In other words, a S/S technology is considered viable only if it meet applicable regulatory criteria. The criteria to be utilized in the Phase I treatability studies were primarily taken from Environmental Protection Agency regulations addressed in 40 CFR 260 through 265 and 268; and Nuclear Regulatory Commission regulations addressed in 10 CFR 61. Thus the majority of the identified criteria are independent of waste form matrix composition (i.e., applicable to cement, glass, organic binders etc.).

  6. Determination of the Structure of Vitrified Hydroceramic/CBC Waste Form Glasses Manufactured from DOE Reprocessing Waste

    Energy Technology Data Exchange (ETDEWEB)

    Scheetz, B.E.; White, W. B.; Chesleigh, M.; Portanova, A.; Olanrewaju, J.

    2005-05-31

    The selection of a glass-making option for the solidification of nuclear waste has dominated DOE waste form programs since the early 1980's. Both West Valley and Savannah River are routinely manufacturing glass logs from the high level waste inventory in tank sludges. However, for some wastes, direct conversion to glass is clearly not the optimum strategy for immobilization. INEEL, for example, has approximately 4400 m{sup 3} of calcined high level waste with an activity that produces approximately 45 watts/m{sup 3}, a rather low concentration of radioactive constituents. For these wastes, there is value in seeking alternatives to glass. An alternative approach has been developed and the efficacy of the process demonstrated that offers a significant savings in both human health and safety exposures and also a lower cost relative to the vitrification option. The alternative approach utilizes the intrinsic chemical reactivity of the highly alkaline waste with the addition of aluminosilicate admixtures in the appropriate proportions to form zeolites. The process is one in which a chemically bonded ceramic is produced. The driving force for reaction is derived from the chemical system itself at very modest temperatures and yet forms predominantly crystalline phases. Because the chemically bonded ceramic requires an aqueous medium to serve as a vehicle for the chemical reaction, the proposed zeolite-containing waste form can more adequately be described as a hydroceramic. The hydrated crystalline materials are then subject to hot isostatic pressing (HIP) which partially melts the material to form a glass ceramic. The scientific advantages of the hydroceramic/CBC approach are: (1) Low temperature processing; (2) High waste loading and thus only modest volumetric bulking from the addition of admixtures; (3) Ability to immobilize sodium; (4) Ability to handle low levels of nitrate (2-3% NO{sub 3}{sup -}); (5) The flexibility of a vitrifiable waste; and (6) A process

  7. Radionuclide Retention Mechanisms in Secondary Waste-Form Testing: Phase II

    Energy Technology Data Exchange (ETDEWEB)

    Um, Wooyong; Valenta, Michelle M.; Chung, Chul-Woo; Yang, Jungseok; Engelhard, Mark H.; Serne, R. Jeffrey; Parker, Kent E.; Wang, Guohui; Cantrell, Kirk J.; Westsik, Joseph H.

    2011-09-26

    This report describes the results from laboratory tests performed at Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions (WRPS) to evaluate candidate stabilization technologies that have the potential to successfully treat liquid secondary waste stream effluents produced by the Hanford Tank Waste Treatment and Immobilization Plant (WTP). WRPS is considering the design and construction of a Solidification Treatment Unit (STU) for the Effluent Treatment Facility (ETF) at Hanford. The ETF, a multi-waste, treatment-and-storage unit that has been permitted under the Resource Conservation and Recovery Act (RCRA), can accept dangerous, low-level, and mixed wastewaters for treatment. The STU needs to be operational by 2018 to receive secondary liquid waste generated during operation of the WTP. The STU will provide the additional capacity needed for ETF to process the increased volume of secondary waste expected to be produced by WTP. This report on radionuclide retention mechanisms describes the testing and characterization results that improve understanding of radionuclide retention mechanisms, especially for pertechnetate, {sup 99}TcO{sub 4}{sup -} in four different waste forms: Cast Stone, DuraLith alkali aluminosilicate geopolymer, encapsulated fluidized bed steam reforming (FBSR) product, and Ceramicrete phosphate bonded ceramic. These data and results will be used to fill existing data gaps on the candidate technologies to support a decision-making process that will identify a subset of the candidate waste forms that are most promising and should undergo further performance testing.

  8. Standard test method for splitting tensile strength for brittle nuclear waste forms

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    1989-01-01

    1.1 This test method is used to measure the static splitting tensile strength of cylindrical specimens of brittle nuclear waste forms. It provides splitting tensile-strength data that can be used to compare the strength of waste forms when tests are done on one size of specimen. 1.2 The test method is applicable to glass, ceramic, and concrete waste forms that are sufficiently homogeneous (Note 1) but not to coated-particle, metal-matrix, bituminous, or plastic waste forms, or concretes with large-scale heterogeneities. Cementitious waste forms with heterogeneities >1 to 2 mm and 5 mm can be tested using this procedure provided the specimen size is increased from the reference size of 12.7 mm diameter by 6 mm length, to 51 mm diameter by 100 mm length, as recommended in Test Method C 496 and Practice C 192. Note 1—Generally, the specimen structural or microstructural heterogeneities must be less than about one-tenth the diameter of the specimen. 1.3 This test method can be used as a quality control chec...

  9. Reduction in nitrate leaching from a concrete waste form by using waterproofing admixture additions

    International Nuclear Information System (INIS)

    Admixture additions of active lime and tricalcium aluminate reduced leach rate about 20% during a seven-day test of a concrete waste form containing a nitrate bearing, aqueous waste. CaO was 5% more effective and, in SEM examination, appeared to hydrate to CaOH which expanded in the concrete pores and blocked water movement. Over time, this compound appeared to dissolve slowly in the water, and the barrier layer it produced slowly receded into the specimen interior

  10. Erosion of magnesium potassium phosphate ceramic waste forms.

    Energy Technology Data Exchange (ETDEWEB)

    Goretta, K. C.

    1998-11-20

    Phosphate-based chemically bonded ceramics were formed from magnesium potassium phosphate (MKP) binder and either industrial fly ash or steel slag. The resulting ceramics were subjected to solid-particle erosion by a stream of either angular Al{sub 2}O{sub 3} particles or rounded SiO{sub 2} sand. Particle impact angles were 30 or 90{degree} and the impact velocity was 50 m/s. Steady-state erosion rates, measured as mass lost from a specimen per mass of impacting particle, were dependent on impact angle and on erodent particle size and shape. Material was lost by a combination of fracture mechanisms. Evolution of H{sub 2}O from the MKP phase appeared to contribute significantly to the material loss.

  11. Secondary Waste Form Screening Test Results—Cast Stone and Alkali Alumino-Silicate Geopolymer

    Energy Technology Data Exchange (ETDEWEB)

    Pierce, Eric M.; Cantrell, Kirk J.; Westsik, Joseph H.; Parker, Kent E.; Um, Wooyong; Valenta, Michelle M.; Serne, R. Jeffrey

    2010-06-28

    PNNL is conducting screening tests on the candidate waste forms to provide a basis for comparison and to resolve the formulation and data needs identified in the literature review. This report documents the screening test results on the Cast Stone cementitious waste form and the Geopolymer waste form. Test results suggest that both the Cast Stone and Geopolymer appear to be viable waste forms for the solidification of the secondary liquid wastes to be treated in the ETF. The diffusivity for technetium from the Cast Stone monoliths was in the range of 1.2 × 10-11 to 2.3 × 10-13 cm2/s during the 63 days of testing. The diffusivity for technetium from the Geopolymer was in the range of 1.7 × 10-10 to 3.8 × 10-12 cm2/s through the 63 days of the test. These values compare with a target of 1 × 10-9 cm2/s or less. The Geopolymer continues to show some fabrication issues with the diffusivities ranging from 1.7 × 10-10 to 3.8 × 10-12 cm2/s for the better-performing batch to from 1.2 × 10-9 to 1.8 × 10-11 cm2/s for the poorer-performing batch. In the future more comprehensive and longer term performance testing will be conducted, to further evaluate whether or not these waste forms will meet the regulation and performance criteria needed to cost-effectively dispose of secondary wastes.

  12. Evaluation study on silica/polymer-based CA-BTP adsorbent for the separation of minor actinides from simulated high-level liquid wastes

    International Nuclear Information System (INIS)

    A silica/polymer-based CA-BTP/SiO2-P adsorbent was prepared to separate minor actinides and some key radionuclides from HLLW. The adsorption properties of CA-BTP/SiO2-P toward 238U(VI), 239Pu(IV), 241Am(III), 99Tc(VII), 152Eu(III), and some typical fission products were studied. CA-BTP/SiO2-P stability against c-radiation was also evaluated. It found CA-BTP/SiO2-P showed very poor adsorption abilities toward U(VI) and most experimental FPs, while CA-BTP/SiO2-P exhibited higher adsorption abilities toward 241Am(III), 239Pu(IV), and 99Tc(VII) in 0.5-1 M HNO3 solution. Moreover, dry CA-BTP/SiO2-P demonstrated no instability when the radiation dose was up to 161 kGy. CA-BTP/SiO2-P adsorbent is a potential candidate for separating 241Am(III), 239Pu(IV), and 99Tc(VII) from HLLW. (author)

  13. Microstructures of Melt-Processed and Spark Plasma Sintered Ceramic Waste Forms

    Science.gov (United States)

    Clark, B. M.; Tumurugoti, P.; Sundaram, S. K.; Amoroso, J. W.; Marra, J. C.; Brinkman, K. S.

    2014-12-01

    Hollandite-rich ceramic waste forms have been demonstrated to exhibit high durability while simultaneously accommodating a wide range of radionuclides in their matrices. This paper presents preliminary results on the preparation and characterization of ceramic waste forms prepared by two different methods—melt processing and spark plasma sintering (SPS). Both processes resulted in similar phase assemblages but exhibited different microstructures depending on processing method. The SPS samples exhibited fine-grained (<1 µm) and dispersed phases, whereas the melt-processed sample contained larger grains (10-20 µm) of specific phases. Additional data will need to be collected on the aqueous leaching durability and radiation resistance to evaluate each processing method for waste form performance.