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Sample records for actinide waste forms

  1. Monazite as a suitable actinide waste form

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

    2013-03-01

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

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

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

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    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.'

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

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    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.

  5. Durability of Actinide Ceramic Waste Forms Under Conditions of Granitoid Rocks

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    Burakov, B. E.; Anderson, E. B.

    2002-02-26

    Three samples of {sup 239}Pu-{sup 241}Am-doped ceramics obtained from previous research were used for alteration experiments simulating corrosion of waste forms in ion-saturated solutions. These were ceramics based on: pyrochlore, (Ca,Hf,Pu,U,Gd){sub 2}Ti{sub 2}O{sub 7}, containing 10 wt.% Pu and 0.1 wt.% Am; zircon, (Zr,Pu)SiO{sub 4}, containing 5-6 wt.% Pu and 0.05 wt.% Am; cubic zirconia, (Zr,Gd,Pu)O{sub 2}, containing 10 wt.% Pu and 0.1 wt.% Am. All these samples were milled in an agate mortar to obtain powder with particle sizes less than 30 micron. Sample of granite taken from the depth 500-503 m was studied and then used for preparing ion-saturated water solutions. A rock sample was ground, washed and classified. A fraction with particle size 0.10-0.25 mm was selected for alteration experiments. Powdered ceramic samples were separately placed into deionized water together with ground granite (approximately 1gram granite per 12-ml water) in special Teflon{trademark} vessels and set at 90 C in the oven for 3 months. After alteration experiments, the ceramic powders were studied by precise XRD analysis. Aqueous solutions and granite grains were analyzed for Am and Pu contents. The results show that alteration did not cause significant phase transformation in all ceramic samples. For all altered samples, the Am contents in aqueous solutions after experiments were similar (approximately n x 10{sup 2} Bq/ml) as well as Am amounts absorbed on granite grains (approximately n x 10{sup 5} Bq/g). Results on Pu contents were varied: for the solutions--from 60 Bq/ml for pyrochlore ceramic to 2.1 x 10{sup 3} Bq/ml for zircon ceramic; and for the absorption on granite--from 2.6 x 10{sup 4} Bq/g for zirconia ceramic to 1.4-6.8 x 10{sup 5} Bq/g for pyrochlore and zircon ceramics.

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

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    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.

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

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

    1997-03-01

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

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

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    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.

  9. 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.

  10. 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.

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

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    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.

  12. Advanced waste forms from spent nuclear fuel

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    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.

  13. Comparative waste forms study

    Energy Technology Data Exchange (ETDEWEB)

    Wald, J.W.; Lokken, R.O.; Shade, J.W.; Rusin, J.M.

    1980-12-01

    A number of alternative process and waste form options exist for the immobilization of nuclear wastes. Although data exists on the characterization of these alternative waste forms, a straightforward comparison of product properties is difficult, due to the lack of standardized testing procedures. The characterization study described in this report involved the application of the same volatility, mechanical strength and leach tests to ten alternative waste forms, to assess product durability. Bulk property, phase analysis and microstructural examination of the simulated products, whose waste loading varied from 5% to 100% was also conducted. The specific waste forms investigated were as follows: Cold Pressed and Sintered PW-9 Calcine; Hot Pressed PW-9 Calcine; Hot Isostatic Pressed PW-9 Calcine; Cold Pressed and Sintered SPC-5B Supercalcine; Hot Isostatic pressed SPC-5B Supercalcine; Sintered PW-9 and 50% Glass Frit; Glass 76-68; Celsian Glass Ceramic; Type II Portland Cement and 10% PW-9 Calcine; and Type II Portland Cement and 10% SPC-5B Supercalcine. Bulk property data were used to calculate and compare the relative quantities of waste form volume produced at a spent fuel processing rate of 5 metric ton uranium/day. This quantity ranged from 3173 L/day (5280 Kg/day) for 10% SPC-5B supercalcine in cement to 83 L/day (294 Kg/day) for 100% calcine. Mechanical strength, volatility, and leach resistance tests provide data related to waste form durability. Glass, glass-ceramic and supercalcine ranked high in waste form durability where as the 100% PW-9 calcine ranked low. All other materials ranked between these two groupings.

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

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    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Phillips, M.L.F.; Molecke, M.A.

    1993-10-01

    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.

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

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    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.

  17. 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.

  18. 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.

  19. 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

  20. 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.

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

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    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. 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).

  3. 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.

  4. 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.

  5. 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.

  6. 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)

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

    Energy Technology Data Exchange (ETDEWEB)

    Koch, M.; Kazimi, M.S.

    1991-04-01

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Bradley, D.J.; Harvey, C.O.; Turcotte, R.P.

    1979-08-01

    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), CaCl/sub 2/ (1.66 g/l), NaHCO/sub 3/ (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 CaCl/sub 2/ 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/sup -5/ to 10/sup -8/ g/cm/sup 2//day. 25 figures, 7 tables.

  9. 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.

  10. 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.

  11. 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

  12. 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.

  13. 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.

  14. 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

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

    Energy Technology Data Exchange (ETDEWEB)

    Buckau, G.

    2005-04-01

    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

  16. 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

  17. 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

  18. Alternative solidified forms for nuclear wastes

    Energy Technology Data Exchange (ETDEWEB)

    McElroy, J.L.; Ross, W.A.

    1976-01-01

    Radioactive wastes will occur in various parts of the nuclear fuel cycle. These wastes have been classified in this paper as high-level waste, intermediate and low-level waste, cladding hulls, and residues. Solidification methods for each type of waste are discussed in a multiple barrier context of primary waste form, applicable coatings or films, matrix encapsulation, canister, engineered structures, and geological storage. The four major primary forms which have been most highly developed are glass for HLW, cement for ILW, organics for LLW, and metals for hulls.

  19. 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.

  20. 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

  1. Korean Waste Management Law and Waste Disposal Forms.

    Science.gov (United States)

    1991-03-01

    Soil Treatment Tanks) 69 Article 8. (Interim Measures on Report of Recycler or Reuser of Industrial Waste) 69 Article 9. (Interim Measures on Permit...recycling and reuse (hereinafter referred to as a "recycler and reuser of industrial waste"), pursuant to Article 23.2. of the Law, shall submit a "Filing... reuser of industrial waste, pursuant to Article 45.2., shall submit a "Modification of Recycle or Reuse of Industrial Waste" (Form No. 17), to the

  2. 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.

  3. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Buckau, G. (ed.)

    2004-07-01

    The present report describes progress within the second year of the EC-project ''Humic Substances in Performance Assessment of Nuclear Waste Disposal: Actinide and Iodine Migration in the Far-Field''. Without being a formal requirement of the commission or co-funding bodies, this report documents results in great technical detail. It is an open report and thus makes the detailed 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 23 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. (orig.)

  5. Radionuclide Retention in Concrete Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Mattigod, Shas V.; Bovaird, Chase C.; Wellman, Dawn M.; Wood, Marcus I.

    2010-09-30

    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. The information presented in the report provides data that 1) quantify radionuclide retention within concrete waste form materials similar to those used to encapsulate waste in the Low-Level Waste Burial Grounds (LLBG); 2) measure the effect of concrete waste form properties likely to influence radionuclide migration; and 3) quantify the stability of uranium-bearing solid phases of limited solubility in concrete.

  6. 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.

  7. 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.

  8. Performance Test on Polymer Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Se Yup [Korea Nuclear Engineering Co., Ltd, Seongnam (Korea, Republic of)

    2012-07-01

    Boric acid wastewater and spent ion exchange resins are generated as a low- and medium- level radioactive wastes from pressurized light water reactors. In Korea, boric acid wastewater is concentrated and dried in the form of granules, and finally solidified by using paraffin wax. In this study, polymer solidification was attempted to produce the stable waste form for the boric acid concentrates and the dewatered spent ion exchange resins. The polymer mixture which consists of epoxy resin, amine compounds and antimony trioxide was used to solidify the boric acid concentrates and the dewatered spent ion exchange resins. To evaluate the stability of polymer waste forms, a series of standardized performance tests was conducted. Also, by the requirement of the regulatory institute in Korea, an additional test was performed to estimate fire resistance and gas generation of the waste forms. A series of performance tests was conducted including compressive strength test, thermal stability test, irradiation stability test and biodegradation stability test, water immersion test, leach test, and free standing water for the polymer waste forms. In addition, a fire resistance test and an analysis of gas generation were performed on the waste forms by the requirement of the regulatory institute in Korea. From the results of the performance tests, it is believed that the polymer waste form is very stable and can satisfy the acceptance criteria for permanent disposal.

  9. 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.

  10. 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

  11. 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

  12. Liquid Secondary Waste Grout Formulation and Waste Form Qualification

    Energy Technology Data Exchange (ETDEWEB)

    Um, Wooyong [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Williams, B. D. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Snyder, Michelle M. V. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Wang, Guohui [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2016-05-23

    This report describes the results from liquid secondary waste (LSW) grout formulation and waste form qualification tests performed at Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions (WRPS) to evaluate new formulations for preparing a grout waste form with high-sulfate secondary waste simulants and the release of key constituents from these grout monoliths. Specific objectives of the LSW grout formulation and waste form qualification tests described in this report focused on five activities: 1.preparing new formulations for the LSW grout waste form with high-sulfate LSW simulants and solid characterization of the cured LSW grout waste form 2.conducting the U.S. Environmental Protection Agency (EPA) Method 1313 leach test (EPA 2012) on the grout prepared with the new formulations, which solidify sulfate-rich Hanford Tank Waste Treatment and Immobilization Plant (WTP) off-gas condensate secondary waste simulant, using deionized water (DIW) 3.conducting the EPA Method 1315 leach tests (EPA 2013) on the grout monoliths made with the new dry blend formulations and three LSW simulants (242-A evaporator condensate, Environmental Restoration Disposal Facility (ERDF) leachate, and WTP off-gas condensate) using two leachants, DIW and simulated Hanford Integrated Disposal Facility (IDF) Site vadose zone pore water (VZPW) 4.estimating the 99Tc desorption Kd (distribution coefficient) values for 99Tc transport in oxidizing conditions to support the IDF performance assessment (PA) 5.estimating the solubility of 99Tc(IV)-bearing solid phases for 99Tc transport in reducing conditions to support the IDF PA.

  13. 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.

  14. 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.

  15. Development of Alternative Technetium Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Czerwinski, Kenneth

    2013-09-13

    The UREX+1 process is under consideration for the separation of transuranic elements from spent nuclear fuel. The first steps of this process extract the fission product technicium-99 ({sup 99}Tc) into an organic phase containing tributylphosphate together with uranium. Treatment of this stream requires the separation of Tc from U and placement into a suitable waste storage form. A potential candidate waste form involves immobilizing the Tc as an alloy with either excess metallic zirconium or stainless steel. Although Tc-Zr alloys seem to be promising waste forms, alternative materials must be investigated. Innovative studies related to the synthesis and behavior of a different class of Tc materials will increase the scientific knowledge related to development of Tc waste forms. These studies will also provide a better understanding of the behavior of {sup 99}Tc in repository conditions. A literature survey has selected promising alternative waste forms for further study: technetium metallic alloys, nitrides, oxides, sulfides, and pertechnetate salts. The goals of this project are to 1) synthesize and structurally characterize relevant technetium materials that may be considered as waste forms, 2) investigate material behavior in solution under different conditions of temperature, electrochemical potential, and radiation, and 3) predict the long-term behavior of these materials.

  16. IGNEOUS INTRUSION IMPACTS ON WASTE PACKAGES AND WASTE FORMS

    Energy Technology Data Exchange (ETDEWEB)

    P. Bernot

    2004-04-19

    The purpose of this model report is to assess the potential impacts of igneous intrusion on waste packages and waste forms in the emplacement drifts at the Yucca Mountain Repository. The models are based on conceptual models and includes an assessment of deleterious dynamic, thermal, hydrologic, and chemical impacts. The models described in this report constitute the waste package and waste form impacts submodel of the Total System Performance Assessment for the License Application (TSPA-LA) model assessing the impacts of a hypothetical igneous intrusion event on the repository total system performance. This submodel is carried out in accordance with Technical Work Plan for Waste Form Degradation Modeling, Testing, and Analyses in Support of LA (BSC 2004 [DIRS:167796]) and Total System Performance Assessment-License Application Methods and Approaches (BSC 2003 [DIRS: 166296]). The technical work plan was prepared in accordance with AP-2.27Q, Planning for Science Activities. Any deviations from the technical work plan are documented in the following sections as they occur. The TSPA-LA approach to implementing the models for waste package and waste form response during igneous intrusion is based on identification of damage zones. Zone 1 includes all emplacement drifts intruded by the basalt dike, and Zone 2 includes all other emplacement drifts in the repository that are not in Zone 1. This model report will document the following model assessments: (1) Mechanical and thermal impacts of basalt magma intrusion on the invert, waste packages and waste forms of the intersected emplacement drifts of Zone 1. (2) Temperature and pressure trends of basaltic magma intrusion intersecting Zone 1 and their potential effects on waste packages and waste forms in Zone 2 emplacement drifts. (3) Deleterious volatile gases, exsolving from the intruded basalt magma and their potential effects on waste packages of Zone 2 emplacement drifts. (4) Post-intrusive physical

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  18. 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.

  19. 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.

  20. 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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1980-01-01

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

  2. 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

  3. 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.

  4. 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.

  5. 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.

  6. Alternative High-Performance Ceramic Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Sundaram, S. K. [Alfred Univ., NY (United States)

    2017-02-01

    This final report (M5NU-12-NY-AU # 0202-0410) summarizes the results of the project titled “Alternative High-Performance Ceramic Waste Forms,” funded in FY12 by the Nuclear Energy University Program (NEUP Project # 12-3809) being led by Alfred University in collaboration with Savannah River National Laboratory (SRNL). The overall focus of the project is to advance fundamental understanding of crystalline ceramic waste forms and to demonstrate their viability as alternative waste forms to borosilicate glasses. We processed single- and multiphase hollandite waste forms based on simulated waste streams compositions provided by SRNL based on the advanced fuel cycle initiative (AFCI) aqueous separation process developed in the Fuel Cycle Research and Development (FCR&D). For multiphase simulated waste forms, oxide and carbonate precursors were mixed together via ball milling with deionized water using zirconia media in a polyethylene jar for 2 h. The slurry was dried overnight and then separated from the media. The blended powders were then subjected to melting or spark plasma sintering (SPS) processes. Microstructural evolution and phase assemblages of these samples were studied using x-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersion analysis of x-rays (EDAX), wavelength dispersive spectrometry (WDS), transmission electron spectroscopy (TEM), selective area x-ray diffraction (SAXD), and electron backscatter diffraction (EBSD). These results showed that the processing methods have significant effect on the microstructure and thus the performance of these waste forms. The Ce substitution into zirconolite and pyrochlore materials was investigated using a combination of experimental (in situ XRD and x-ray absorption near edge structure (XANES)) and modeling techniques to study these single phases independently. In zirconolite materials, a transition from the 2M to the 4M polymorph was observed with increasing Ce content. The resulting

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

    Energy Technology Data Exchange (ETDEWEB)

    Riley, Brian J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Mccloy, John S. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Crum, Jarrod V. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Lepry, William C. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Rodriguez, Carmen P. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Windisch, Charles F. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Matyas, Josef [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Westman, Matthew P. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Rieck, Bennett T. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Lang, Jesse B. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Olszta, Matthew J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Pierce, David A. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2014-01-17

    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.

  8. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Ross, W.A.; Mendel, J.E.

    1979-12-01

    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 10/sup 19/ alpha-events/cm/sup 3/ 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.

  10. 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.

  11. Prediction of dissolved actinide concentrations in concentrated electrolyte solutions: a conceptual model and model results for the Waste Isolation Pilot Plant (WIPP)

    Energy Technology Data Exchange (ETDEWEB)

    Novak, C.F.; Moore, R.C. [Sandia National Labs., Albuquerque, NM (United States); Bynum, R.V. [Science Applications International Corp., Albuquerque, NM (United States)

    1996-10-25

    The conceptual model for WIPP dissolved concentrations is a description of the complex natural and artificial chemical conditions expected to influence dissolved actinide concentrations in the repository. By a set of physical and chemical assumptions regarding chemical kinetics, sorption substrates, and waste-brine interactions, the system was simplified to be amenable to mathematical description. The analysis indicated that an equilibrium thermodynamic model for describing actinide solubilities in brines would be tractable and scientifically supportable. This paper summarizes the conceptualization and modeling approach and the computational results as used in the WIPP application for certification of compliance with relevant regulations for nuclear waste repositories. The WIPP site contains complex natural brines ranging from sea water to 10x more concentrated than sea water. Data bases for predicting solubility of Am(III) (as well as Pu(III) and Nd(III)), Th(IV), and Np(V) in these brines under potential repository conditions have been developed, focusing on chemical interactions with Na, K, Mg, Cl, SO{sub 4}, and CO{sub 3} ions, and the organic acid anions acetate, citrate, EDTA, and oxalate. The laboratory and modeling effort augmented the Harvie et al. parameterization of the Pitzer activity coefficient model so that it could be applied to the actinides and oxidation states important to the WIPP system.

  12. 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

  13. Chemistry of actinides; Chimie des actinides

    Energy Technology Data Exchange (ETDEWEB)

    Vitorge, P. [CEA/Saclay, Dept. d' Entreposage et de Stockage des Dechets (DESD), 91 - Gif-sur-Yvette (France)

    1999-07-01

    This article gives the basic data of the actinides chemistry, describes then qualitatively the main parts of the fuel cycle and concludes with quantitative data. The theoretical recalls give qualitative notions to explain the chemical reactivity of actinides and to understand thus the values of the thermodynamic data which allow quantitative anticipations at equilibrium. The Thermodynamic Data Base (TDB) of the NEA-OECD and the CEA in France have recently estimated some of them in using and developing methodologies whose some are presented here. Some current problems of actinides chemistry are described: analysis of the possibilities to (1)improve the reprocessing of long-lived actinides (2)anticipate their behaviour in the environment in order to compare the impact of the different options of the wastes management. The Pourbaix diagrams summarize the chemistry in solution; the author has added information on the solubility, the influence of the ionic strength and of the complexes formation in bicarbonate/carbonate (HCO{sub 3}{sup -}/CO{sub 3}{sup 2-}) media. The discussion on the choice of the equilibrium constants allows to point out the particular points, the dubiousness and the data which have to be proved. (O.M.)

  14. 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.

  15. Electrochemical corrosion testing of metal waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Abraham, D. P.; Peterson, J. J.; Katyal, H. K.; Keiser, D. D.; Hilton, B. A.

    1999-12-14

    Electrochemical corrosion tests have been conducted on simulated stainless steel-zirconium (SS-Zr) metal waste form (MWF) samples. The uniform aqueous corrosion behavior of the samples in various test solutions was measured by the polarization resistance technique. The data show that the MWF corrosion rates are very low in groundwaters representative of the proposed Yucca Mountain repository. Galvanic corrosion measurements were also conducted on MWF samples that were coupled to an alloy that has been proposed for the inner lining of the high-level nuclear waste container. The experiments show that the steady-state galvanic corrosion currents are small. Galvanic corrosion will, hence, not be an important mechanism of radionuclide release from the MWF alloys.

  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. 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.

  18. 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

  19. 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}.

  20. 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.

  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. 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.

  3. 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.

  4. 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.

  5. 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

  6. 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.

  7. New cubic structure compounds as actinide host phases

    Energy Technology Data Exchange (ETDEWEB)

    Stefanovsky, S V [SIA Radon, 7th Rostovskii lane 2/14, Moscow 119121 (Russian Federation); Yudintsev, S V; Livshits, T S, E-mail: profstef@mtu-net.ru [Institute of Geology of Ore Deposits, Petrography, Mineralogy and Geochemistry RAS, Staromonetny lane 35, Moscow 119017 (Russian Federation)

    2010-03-15

    Various compounds with fluorite (cubic zirconia) and fluorite-derived (pyrochlore, zirconolite) structures are considered as promising actinide host phases at immobilization of actinide-bearing nuclear wastes. Recently some new cubic compounds - stannate and stannate-zirconate pyrochlores, murataite and related phases, and actinide-bearing garnet structure compounds were proposed as perspective matrices for complex actinide wastes. Zirconate pyrochlore (ideally Gd{sub 2}Zr{sub 2}O{sub 7}) has excellent radiation resistance and high chemical durability but requires high temperatures (at least 1500 deg. C) to be produced by hot-pressing from sol-gel derived precursor. Partial Sn{sup 4+} substitution for Zr{sup 4+} reduces production temperature and the compounds REE{sub 2}ZrSnO{sub 7} may be hot-pressed or cold pressed and sintered at {approx}1400 deg. C. Pyrochlore, A{sub 2}B{sub 2}O{sub 7-x} (two-fold elementary fluorite unit cell), and murataite, A{sub 3}B{sub 6}C{sub 2}O{sub 20-y} (three-fold fluorite unit cell), are end-members of the polysomatic series consisting of the phases whose structures are built from alternating pyrochlore and murataite blocks (nano-sized modules) with seven- (2C/3C/2C), five- (2C/3C), eight- (3C/2C/3C) and three-fold (3C - murataite) fluorite unit cells. Actinide content in this series reduces in the row: 2C (pyrochlore) > 7C > 5C > 8C > 3C (murataite). Due to congruent melting murataite-based ceramics may be produced by melting and the firstly segregated phase at melt crystallization is that with the highest fraction of the pyrochlore modules in its structure. The melts containing up to 10 wt. % AnO{sub 2} (An = Th, U, Np, Pu) or REE/An fraction of HLW form at crystallization zoned grains composed sequentially of the 5C {yields} 8C {yields} 3C phases with the highest actinide concentration in the core and the lowest - in the rim of the grains. Radiation resistance of the 'murataite' is comparable to titanate pyrochlores. One

  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. Final report on cermet high-level waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Kobisk, E.H.; Quinby, T.C.; Aaron, W.S.

    1981-08-01

    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.

  10. 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.

  11. 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

  12. 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

  13. 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

  14. 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.

  15. 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.

  16. Weathering Effects on Technetium Leachability from Ceramicrete Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Jong Kwon; Fadzil, Syazwani Mohd; Um, Woo Yong [Pohang University of Science and Technology, Pohang (Korea, Republic of)

    2012-05-15

    Ceramicrete waste form was developed as part of the U.S. Department of Energy's (DOE's) Office of Environmental Management program to stabilize and contain volatile radioactive contaminant such as technetium ({sup 99}Tc). Ceramicrete processing technology has been demonstrated on various waste streams and has shown to retain both radioactive and hazardous contaminants effectively. Radioactive Tc is highly soluble and mobile in the environment as pertechnetate anion. Tc is also easily volatilized. Tc can be in the waste in two oxidation states . IV and VII. Tc is volatilized even during the evaporation stage when removing excess water from HLW that contains acidic solutions of Tc(VII) as pertechnetate (TcO{sub 4}){sup -}. Common chemical weathering process to occur within waste forms in the nuclear waste repository is carbonation. In addition, since technetium ({sup 99}Tc) leachability is closely related with oxidation condition and the oxidized Tc species, pertechnetate (TcO{sub 4}{sup -}) shows much higher leachability, oxidative weathering pre-treatment of waste form is important, especially for the shallow-depth radioactive waste repositories. In 2011, an evaluation of weathering effects on Tc release from different waste forms (Cast Stone and DuraLith) was conducted in the environmental chamber with different gas mixtures to produce enhanced oxidizing or carbonation conditions. Based on the technical literature and previous testing results, Ceramicrete waste form was also selected for further weathering testing to evaluate oxidizing or carbonation effects on Tc release after weathering. Leachability Indexes (LI) of Tc from two waste forms (Cast Stone and DuraLith) without pre-treatment of O{sub 2}(g) or CO{sub 2}(g) are higher than those of waste forms with pre-treatment of the same gases to simulate enhanced oxidation and carbonation weathering conditions, respectively. The LI values of two waste forms with and without weathering are shown in Table 1

  17. Secondary Waste Cementitious Waste Form Data Package for the Integrated Disposal Facility Performance Assessment

    Energy Technology Data Exchange (ETDEWEB)

    Cantrell, Kirk J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Westsik, Joseph H. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Serne, R Jeffrey [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Um, Wooyong [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Cozzi, Alex D. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2016-05-16

    A review of the most up-to-date and relevant data currently available was conducted to develop a set of recommended values for use in the Integrated Disposal Facility (IDF) performance assessment (PA) to model contaminant release from a cementitious waste form for aqueous wastes treated at the Hanford Effluent Treatment Facility (ETF). This data package relies primarily upon recent data collected on Cast Stone formulations fabricated with simulants of low-activity waste (LAW) and liquid secondary wastes expected to be produced at Hanford. These data were supplemented, when necessary, with data developed for saltstone (a similar grout waste form used at the Savannah River Site). Work is currently underway to collect data on cementitious waste forms that are similar to Cast Stone and saltstone but are tailored to the characteristics of ETF-treated liquid secondary wastes. Recommended values for key parameters to conduct PA modeling of contaminant release from ETF-treated liquid waste are provided.

  18. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-02-15

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

  20. 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

  1. 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.

  2. Transmutation of nuclear waste. Status report RAS programme 1994: Recycling and transmutation of actinides and fission products

    Energy Technology Data Exchange (ETDEWEB)

    Cordfunke, E.H.P.; Gruppelaar, H.; Franken, W.M.P.

    1995-07-01

    This report describes the status and progress of the Dutch RAS programme on `Recycling and Transmutation of Actinides and Fission Products` over the year 1994, which is the first year of the second 4-year programme. This programme is outlined and a short progress report is given over 1994, including a listing of 23 reports and publications over the year 1994. Highlights of 1994 were: The completion of long-lived fission-product transmutation studies, the initiation of small-scale demonstration experiments in the HFR on Tc and I, the issue of reports on the potential of the ALMR (Advanced Liquid Metal Reactor) for transmutation adn the participation and international cooperation on irradiation experiments with actinides in inert matrices. The remaining chapters contain more extended contributions on recent developments and selected topics, under the headings: Benefits and risks of partitioning and transmutation, Perspective of chemical partitioning, Inert matrices, Evolutionary options (MOX), Perspective of heavy water reactors, Perspective of fast burners, Perspective of accelerator-based systems, Thorium cycle, Fission-product transmutation, End scenarios, and Executive summary and recommendations. (orig.).

  3. 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.

  4. 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.

  5. 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

  6. 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.

  7. Treatability study of absorbent polymer waste form for mixed waste treatment

    Energy Technology Data Exchange (ETDEWEB)

    Herrmann, S. D.; Lehto, M. A.; Stewart, N. A.; Croft, A. D.; Kern, P. W.

    2000-02-10

    A treatability study was performed to develop and characterize an absorbent polymer waste form for application to low level (LLW) and mixed low level (MLLW) aqueous wastes at Argonne National Laboratory-West (ANL-W). In this study absorbent polymers proved effective at immobilizing aqueous liquid wastes in order to meet Land Disposal Restrictions for subsurface waste disposal. Treatment of aqueous waste with absorbent polymers provides an alternative to liquid waste solidification via high-shear mixing with clays and cements. Significant advantages of absorbent polymer use over clays and cements include ease of operations and waste volume minimization. Absorbent polymers do not require high-shear mixing as do clays and cements. Granulated absorbent polymer is poured into aqueous solutions and forms a gel which passes the paint filter test as a non-liquid. Pouring versus mixing of a solidification agent not only eliminates the need for a mixing station, but also lessens exposure to personnel and the potential for spread of contamination from treatment of radioactive wastes. Waste minimization is achieved as significantly less mass addition and volume increase is required of and results from absorbent polymer use than that of clays and cements. Operational ease and waste minimization translate into overall cost savings for LLW and MLLW treatment.

  8. Test plan for formulation and evaluation of grouted waste forms with shine process wastes

    Energy Technology Data Exchange (ETDEWEB)

    Ebert, W. L. [Argonne National Lab. (ANL), Argonne, IL (United States); Jerden, J. L. [Argonne National Lab. (ANL), Argonne, IL (United States)

    2015-09-01

    The objective of this experimental project is to demonstrate that waste streams generated during the production of Mo99 by the SHINE Medical Technologies (SHINE) process can be immobilized in cement-based grouted waste forms having physical, chemical, and radiological stabilities that meet regulatory requirements for handling, storage, transport, and disposal.

  9. Multibarrier waste forms. Part II. Characterization and evaluation.

    Energy Technology Data Exchange (ETDEWEB)

    Rusin, J.M.; Gray, W.J.; Wald, J.W.

    1979-08-01

    The multibarrier concept for the storage of radioactive waste is to use up to three barriers to isolate radionuclides from the environment: a solidified waste inner core, an impervious coating, and a metal matrix. The four multibarrier waste forms were evaluated for thermal stability (volatility), mechanical strength (impact resistance), and leach resistance. This report discusses the characterization of the multibarrier waste forms and compares them to reference calcine and glass waste forms. The weight loss of supercalcine-ceramics after 4 h in dry air ranges between 0.01 and 1.6 wt % from 1000 to 1200/sup 0/C and is dependent upon composition. Glass marbles in a cast lead alloy offer approximately an order of magnitude decease in the wt % fines < 37 ..mu..m released after impact as compared to a glass monolith. CVD-coated supercalcine in a sintered 410 SS matrix offers up to two orders of magnitude decrease. Hot-pressed supercalcine ceramics may offer no increase in impact resistance or leach resistance over that of a glass monolith. Supercalcine may offer no advantage over waste glasses in leach resistance. Glass and PyC/Al/sub 2/O/sub 3/ coatings provide effective inert leaching barriers.

  10. 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.

  11. 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)

  12. Reference Alloy Waste Form Fabrication and Initiation of Reducing Atmosphere and Reductive Additives Study on Alloy Waste Form Fabrication

    Energy Technology Data Exchange (ETDEWEB)

    S.M. Frank; T.P. O' Holleran; P.A. Hahn

    2011-09-01

    This report describes the fabrication of two reference alloy waste forms, RAW-1(Re) and RAW-(Tc) using an optimized loading and heating method. The composition of the alloy materials was based on a generalized formulation to process various proposed feed streams resulting from the processing of used fuel. Waste elements are introduced into molten steel during alloy fabrication and, upon solidification, become incorporated into durable iron-based intermetallic phases of the alloy waste form. The first alloy ingot contained surrogate (non-radioactive), transition-metal fission products with rhenium acting as a surrogate for technetium. The second alloy ingot contained the same components as the first ingot, but included radioactive Tc-99 instead of rhenium. Understanding technetium behavior in the waste form is of particular importance due the longevity of Tc-99 and its mobility in the biosphere in the oxide form. RAW-1(Re) and RAW-1(Tc) are currently being used as test specimens in the comprehensive testing program investigating the corrosion and radionuclide release mechanisms of the representative alloy waste form. Also described in this report is the experimental plan to study the effects of reducing atmospheres and reducing additives to the alloy material during fabrication in an attempt to maximize the oxide content of waste streams that can be accommodated in the alloy waste form. Activities described in the experimental plan will be performed in FY12. The first aspect of the experimental plan is to study oxide formation on the alloy by introducing O2 impurities in the melt cover gas or from added oxide impurities in the feed materials. Reducing atmospheres will then be introduced to the melt cover gas in an attempt to minimize oxide formation during alloy fabrication. The second phase of the experimental plan is to investigate melting parameters associated with alloy fabrication to allow the separation of slag and alloy components of the melt.

  13. 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

  14. 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.

  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. 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.

  17. 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...

  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. 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)

  20. 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.

  1. A literature review of actinide-carbonate mineral interactions

    Energy Technology Data Exchange (ETDEWEB)

    Stout, D.L. [Missouri Univ., Columbia, MO (United States). Dept. of Geological Sciences; Carroll, S.A. [Lawrence Livermore National Lab., CA (United States)

    1993-10-01

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

  2. Degradation modeling of the ANL ceramic waste form

    Energy Technology Data Exchange (ETDEWEB)

    Fanning, T. H.; Morss, L. R.

    2000-03-28

    A ceramic waste form composed of glass-bonded sodalite is being developed at Argonne National Laboratory (ANL) for immobilization and disposition of the molten salt waste stream from the electrometallurgical treatment process for metallic DOE spent nuclear fuel. As part of the spent fuel treatment program at ANL, a model is being developed to predict the long-term release of radionuclides under repository conditions. Dissolution tests using dilute, pH-buffered solutions have been conducted at 40, 70, and 90 C to determine the temperature and pH dependence of the dissolution rate. Parameter values measured in these tests have been incorporated into the model, and preliminary repository performance assessment modeling has been completed. Results indicate that the ceramic waste form should be acceptable in a repository environment.

  3. PF-4 actinide disposition strategy

    Energy Technology Data Exchange (ETDEWEB)

    Margevicius, Robert W [Los Alamos National Laboratory

    2010-05-28

    The dwindling amount of Security Category I processing and storage space across the DOE Complex has driven the need for more effective storage of nuclear materials at LANL's Plutonium Facility's (PF-4's) vault. An effort was begun in 2009 to create a strategy, a roadmap, to identify all accountable nuclear material and determine their disposition paths, the PF-4 Actinide Disposition Strategy (PADS). Approximately seventy bins of nuclear materials with similar characteristics - in terms of isotope, chemical form, impurities, disposition location, etc. - were established in a database. The ultimate disposition paths include the material to remain at LANL, disposition to other DOE sites, and disposition to waste. If all the actions described in the document were taken, over half of the containers currently in the PF-4 vault would been eliminated. The actual amount of projected vault space will depend on budget and competing mission requirements, however, clearly a significant portion of the current LANL inventory can be either dispositioned or consolidated.

  4. Synthesis of apatite and monazite waste form for immobilization of rare earth oxide radioactive waste

    Energy Technology Data Exchange (ETDEWEB)

    Ahn, B. G.; Park, H. S.; Kim, I. T.; Lee, H. S. [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

    2008-08-15

    In order to fabricate a monolithic waste form containing RE oxides, a vitrification at a high temperature or a ceramization by a HIP method is required. In this study, a series of monolithic wasteform with high waste loading were successfully produced at a mild condition, where the chemical structure was equivalent to the product by a high temperature process or a monolithic wasteform consisting of a durable ceramic host matrix for immobilizing RE elements.

  5. Laboratory Optimization Tests of Decontamination of Cs, Sr, and Actinides from Hanford Waste Treatment Plant Low Activity Waste Off-Gas Condensate Simulant

    Energy Technology Data Exchange (ETDEWEB)

    Taylor-Pashow, K. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Nash, C. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); McCabe, D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-01-06

    The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Off-Gas Condensate) from the off-gas system. The baseline plan for disposition of this stream is to send it to the WTP Pretreatment Facility, where it will be blended with LAW, concentrated by evaporation and recycled to the LAW vitrification facility. Alternate disposition of this stream would eliminate recycling of problematic components, and would enable less integrated operation of the LAW melter and the Pretreatment Facilities. Eliminating this stream from recycling within WTP would also substantially decrease the LAW vitrification mission duration and quantity of glass waste.

  6. 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

  7. 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.

  8. 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.

  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. 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.

  11. 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.

  12. Estimation of centerline temperature of the waste form for the rare earth waste generated from pyrochemical process

    Science.gov (United States)

    Choi, Jung-Hoon; Eun, Hee-Chul; Lee, Tae-Kyo; Lee, Ki-Rak; Han, Seung-Youb; Jeon, Min-Ku; Park, Hwan-Seo; Ahn, Do-Hee

    2017-01-01

    Estimation of centerline temperature of nuclear glass waste form for each waste stream is very essential in the period of storage because the centerline temperature being over its glass transition temperature results in the increase of leaching rate of radioactive nuclides due to the devitrification of glass waste form. Here, to verify the effects of waste form diameter and transuranic element content in the rare earth waste on the centerline temperature of the waste form, the surrogate rare earth glass waste generated from pyrochemical process was immobilized with SiO2sbnd Al2O3sbnd B2O3 glass frit system, and thermal properties of the rare earth glass waste form were determined by thermomechanical analysis and thermal conductivity analysis. The estimation of centerline temperature was carried out using the experimental thermal data and steady-state conduction equation in a long and solid cylinder type waste form. It was revealed that thermal stability of waste form in case of 0.3 m diameter was not affected by the TRU content even in the case of 80% TRU recovery ratio in the electrowinning process, meaning that the waste form of 0.3 m diameter is thermally stable due to the low centerline temperature relative to its glass transition temperature of the rare earth glass waste form.

  13. 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.

  14. Cesium incorporation in hollandite-rich multiphasic ceramic waste forms

    Science.gov (United States)

    Tumurugoti, P.; Clark, B. M.; Edwards, D. J.; Amoroso, Jake; Sundaram, S. K.

    2017-02-01

    Hollandite-rich multiphase waste form compositions processed by melt-solidification and spark plasma sintering (SPS) were characterized, compared, and validated for nuclear waste incorporation. Phase identification by x-ray diffraction (XRD) and electron back-scattered diffraction (EBSD) confirmed hollandite as the major phase present in these samples along with perovskite, pyrochlore and zirconolite. Distribution of selected elements observed by wavelength dispersive spectroscopy (WDS) maps indicated that Cs formed a secondary phase during SPS processing, which was considered undesirable. On the other hand, Cs partitioned into the hollandite phase in melt-processed samples. Further analysis of hollandite structure in melt-processed composition by selected area electron diffraction (SAED) revealed ordered arrangement of tunnel ions (Ba/Cs) and vacancies, suggesting efficient Cs incorporation into the lattice.

  15. 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.

  16. 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.

  17. 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.

  18. 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

  19. 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.

  20. Dilute condition corrosion behavior of glass-ceramic waste form

    Science.gov (United States)

    Crum, Jarrod V.; Neeway, James J.; Riley, Brian J.; Zhu, Zihua; Olszta, Matthew J.; Tang, Ming

    2016-12-01

    Borosilicate glass-ceramics are being developed to immobilize high-level waste generated by aqueous reprocessing into a stable waste form. The corrosion behavior of this multiphase waste form is expected to be complicated by multiple phases and crystal-glass interfaces. A modified single-pass flow-through test was performed on polished monolithic coupons at a neutral pH (25 °C) and 90 °C for 33 d. The measured glass corrosion rates by micro analysis in the samples ranged from 0.019 to 0.29 g m-2 d-1 at a flow rate per surface area = 1.73 × 10-6 m s-1. The crystal phases (oxyapatite and Ca-rich powellite) corroded below quantifiable rates, by micro analysis. While, Ba-rich powellite corroded considerably in O10 sample. The corrosion rates of C1 and its replicate C20 were elevated an order of magnitude by mechanical stresses at crystal-glass interface caused by thermal expansion mismatch during cooling and unique morphology (oxyapatite clustering).

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

    Energy Technology Data Exchange (ETDEWEB)

    Gibb, F.G.F. [Immobilisation Science Laboratory, Department of Engineering Materials, University of Sheffield, Sheffield S1 3JD (United Kingdom)], E-mail: f.gibb@sheffield.ac.uk; Taylor, K.J. [Department of Geography, University of Sheffield, Sheffield S10 2TN (United Kingdom); Burakov, B.E. [Laboratory of Applied Mineralogy and Radiogeochemistry, V.G. Khlopin Radium Institute, St. Petersburg 194021 (Russian Federation)

    2008-03-15

    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{sub 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.

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. 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

  7. 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.

  8. 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.

  9. Demonstration of trivalent actinide partitioning from simulated high-level liquid waste using modifier-free unsymmetrical diglycolamide in n-dodecane

    Energy Technology Data Exchange (ETDEWEB)

    Nayak, P.K.; Kumaresan, R.; Venkatesan, K.A.; Subramanian, G.G.S.; Rajeswari, S.; Antony, M.P.; Vasudeva Rao, P.R. [Indira Gandhi Centre for Atomic Research, Kalpakkam (India). Fuel Chemistry Div.; Chaurasia, Shivkumar; Bhanage, B.M. [Institute of Chemical Technology, Mumbai (India)

    2015-07-01

    Partitioning of trivalent americium from fast-reactor (FR) simulated high-level liquid waste (SHLLW) has been demonstrated, for the first time, using a modifier-free organic phase containing an unsymmetrical diglycolamide, N,N,-didodecyl-N',N'-dioctyl-3-oxapentane-1,5-diamide (D{sup 3}DODGA), in n-dodecane (n-DD). The extraction behavior of various metal ions present in the FR-SHLLW that contained about 3.2 g/L of trivalent metal ions (Am(III) and Ln(III)) was studied using a solution of 0.1 M D{sup 3}DODGA/n-DD, by batch equilibration mode. The extraction of Am(III) was accompanied by the co-extraction of all lanthanides and unwanted metal ions such as Zr(IV), Y(III), and Pd(II) from FR-SHLLW. The co-extraction of unwanted metal ions was minimized by adding a suitable aqueous soluble complexing agents to FR-SHLLW, prior to extraction. As a result, trans-1,2-diaminocyclohexane-N,N,N'N'-tetraacetic acid (CyDTA) was identified as an appropriate reagent for preventing the extraction of zirconium and palladium, that posed problems during recovery of trivalent metal ions from the loaded organic phase. The stripping of behavior of Am(III) and Ln(III) from the loaded organic phase was studied using dilute nitric acid in batch equilibration mode. Based on those results, a counter-current mixer-settler run was performed in a 20-stage mixer-settler. About 99.9% of Am(III), Ln(III) and Y(III) from FR-SHLLW in 0.1 M D{sup 3}DODGA/n-DD was achieved in 20 contacts and the recovery of Am(III) and other trivalents from the loaded organic phase was achieved in 5 contacts using 0.01 M nitric acid. The study demonstrated the possibility of using the modifier-free reagent, D{sup 3}DODGA, for the separation of trivalent actinides from FR-SHLLW.

  10. Actinide partitioning and transmutation program. Progress report, July 1--September 30, 1977

    Energy Technology Data Exchange (ETDEWEB)

    Tedder, D.W.; Blomeke, J.O. (comps.)

    1978-02-01

    In Purex process modifications, two cold runs with mixer-settlers were made on the extraction and stripping of ruthenium and zirconium without the presence of uranium. Efforts in actinide recovery from solids were directed toward the determination of dissolution parameters in various reagents for /sup 241/Am and /sup 239/Pu oxide mixtures, /sup 233/U oxide, /sup 237/Np oxide, /sup 244/Cm oxide, /sup 232/Th oxide, and PuO/sub 2/. Studies in americium-curium recovery with OPIX (oxalate precipitation and ion exchange), Talspeak, and cation exchange chromatography focused on the feasibility of forming oxalate precipitates in continuous systems, the effects of zirconium on Talspeak, and methods for removing solvent degradation products of the Talspeak system. In studies of americium-curium recovery using bidentate extractants, additional distribution coefficients for actinides and other key elements between reduced synthetic LWR waste solution and 30 percent dihexyl-N, N-diethyl-carbamylmethylene phosphonate in diisopropylbenzene were measured. Studies in the americium-curium recovery using inorganic ion exchange media to determine the pH dependence of lanthanide ion affinity for niobate, titanate, and zirconate ion exchange materials have been completed. A modified flowsheet for the extraction of uranium, neptunium, plutonium, americium, and curium from high-level liquid waste is presented. Evaluation of methods for measuring actinides from incinerator ash is continuing. A preliminary evaluation of methods for treatment of salt waste and waste waters was completed. In thermal reactor transmutation studies, waste actinides from an LWR lattice containing mixed uranium-plutonium assemblies were recycled in separate target assemblies. (LK)

  11. 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.

  12. Chromium speciation in hazardous, cement-based waste forms

    Science.gov (United States)

    Lee, J. F.; Bajt, S.; Clark, S. B.; Lamble, G. M.; Langton, C. A.; Oji, L.

    1995-02-01

    XANES and EXAFS techniques were used to determine the oxidation states and local structural environment of Cr in cement-based waste forms. Results show that Cr in untreated Portland cement formulations remains as toxic Cr 6+, while slag additives to the cement reduce Cr 6+ to the less toxic, less mobile Cr 3+ species. EXAFS analysis suggests that the Cr 6+ species is surrounded by four nearest oxygen atoms, while the reduced Cr 3+ sp ecies is surrounded by six oxygen atoms. The fitted CrO bond lengths for Cr 6+ and Cr 3+ species are around 1.66 and 1.98 Å, respectively.

  13. 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.

  14. 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)

  15. 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

  16. 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.

  17. 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.

  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

    2016-06-01

    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.

  19. 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.

  20. NMR studies of actinide dioxides

    Energy Technology Data Exchange (ETDEWEB)

    Tokunaga, Y. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan)], E-mail: tokunaga.yo@jaea.go.jp; Sakai, H.; Fujimoto, T.; Kambe, S.; Walstedt, R.E.; Ikushima, K.; Yasuoka, H. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Aoki, D.; Homma, Y. [Institute for Materials Research, Tohoku University, Oarai, Ibaraki 311-1313 (Japan); Haga, Y.; Matsuda, T.D.; Ikeda, S.; Yamamoto, E.; Nakamura, A. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Shiokawa, Y. [Institute for Materials Research, Tohoku University, Oarai, Ibaraki 311-1313 (Japan); Nakajima, K.; Arai, Y. [Department of Nuclear Energy System, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Onuki, Y. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Department of Physics, Osaka University, Toyonaka, Osaka 560-0043 (Japan)

    2007-10-11

    {sup 17}O NMR measurements have been performed on a series of the actinide dioxides, UO{sub 2}, NpO{sub 2} and PuO{sub 2}. Although the {sup 17}O NMR spectra in these materials are similar at higher temperatures, the low-temperature spectra present are significantly different. In UO{sub 2} we have observed a wide spectrum, forming a rectangular shape below T{sub N}=30 K. In NpO{sub 2}, on the other hand, the spectra broaden rather gradually and exhibit a two-peak structure below T{sub 0}=26 K. In PuO{sub 2}, neither spectrum broadening nor splitting has been observed. We show that these NMR spectra clearly indicate the different nature of the low-temperature magnetic ground states in these actinide compounds.

  1. Advances in computational actinide chemistry in China

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-04-01

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

  2. 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

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. 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

  8. 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)

  9. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Braase, Lori [Idaho National Lab. (INL), Idaho Falls, ID (United States)

    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.

  11. 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.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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

  17. The disposal of nuclear waste in space

    Science.gov (United States)

    Burns, R. E.

    1978-01-01

    The important problem of disposal of nuclear waste in space is addressed. A prior study proposed carrying only actinide wastes to space, but the present study assumes that all actinides and all fission products are to be carried to space. It is shown that nuclear waste in the calcine (oxide) form can be packaged in a container designed to provide thermal control, radiation shielding, mechanical containment, and an abort reentry thermal protection system. This package can be transported to orbit via the Space Shuttle. A second Space Shuttle delivers an oxygen-hydrogen orbit transfer vehicle to a rendezvous compatible orbit and the mated OTV and waste package are sent to the preferred destination. Preferred locations are either a lunar crater or a solar orbit. Shuttle traffic densities (which vary in time) are given and the safety of space disposal of wastes discussed.

  18. 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).

  19. 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

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

    Energy Technology Data Exchange (ETDEWEB)

    Chick, L.A.; McVay, G.L.; Mellinger, G.B.; Roberts, F.P.

    1980-12-01

    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.

  1. 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...

  2. 40 CFR 761.205 - Notification of PCB waste activity (EPA Form 7710-53).

    Science.gov (United States)

    2010-07-01

    ... 40 Protection of Environment 30 2010-07-01 2010-07-01 false Notification of PCB waste activity..., DISTRIBUTION IN COMMERCE, AND USE PROHIBITIONS PCB Waste Disposal Records and Reports § 761.205 Notification of PCB waste activity (EPA Form 7710-53). (a)(1) All commercial storers, transporters, and disposers...

  3. 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.

  4. Spent fuel treatment and mineral waste form development at Argonne National Laboratory-West

    Energy Technology Data Exchange (ETDEWEB)

    Goff, K.M.; Benedict, R.W.; Bateman, K. [Argonne National Lab., Idaho Falls, ID (United States); Lewis, M.A.; Pereira, C. [Argonne National Lab., IL (United States); Musick, C.A. [Lockheed Idaho Technologies Co., Idaho Falls, ID (United States)

    1996-07-01

    At Argonne National Laboratory-West (ANL-West) there are several thousand kilograms of metallic spent nuclear fuel containing bond sodium. This fuel will be treated in the Fuel Conditioning Facility (FCF) at ANL-West to produce stable waste forms for storage and disposal. Both mineral and metal high-level waste forms will be produced. The mineral waste form will contain the active metal fission products and the transuranics. Cold small-scale waste form testing has been on-going at Argonne in Illinois. Large-scale testing is commencing at ANL-West.

  5. Durability and degradation of HT9 based alloy waste forms with variable Ni and Cr content

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-12-31

    Short-term electrochemical and long-term hybrid electrochemical corrosion tests were performed on alloy waste forms in reference aqueous solutions that bound postulated repository conditions. The alloy waste forms investigated represent candidate formulations that can be produced with advanced electrochemical treatment of used nuclear fuel. The studies helped to better understand the alloy waste form durability with differing concentrations of nickel and chromium, species that can be added to alloy waste forms to potentially increase their durability and decrease radionuclide release into the environment.

  6. 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...

  7. NNWSI [Nevada Nuclear Waste Storage Investigations] waste form testing at Argonne National Laboratory; Semiannual report, January--June 1988

    Energy Technology Data Exchange (ETDEWEB)

    Bates, J.K.; Gerding, T.J.; Ebert, W.L.; Mazer, J.J.; Biwer, B.M. [Argonne National Lab., IL (USA)

    1990-04-01

    The Chemical Technology Division of Argonne National Laboratory is performing experiments in support of the waste package development of the Yucca Mountain Project (formerly the Nevada Nuclear Waste Storage Investigations Project). Experiments in progress include (1) the development and performance of a durability test in unsaturated conditions, (2) studies of waste form behavior in an irradiated atmosphere, (3) studies of behavior in water vapor, and (4) studies of naturally occurring glasses to be used as analogues for waste glass behavior. This report documents progress made during the period of January--June 1988. 21 refs., 37 figs., 12 tabs.

  8. The ALMR actinide burning system

    Energy Technology Data Exchange (ETDEWEB)

    Quinn, J.E. (General Electric Co., San Jose, CA (United States))

    1993-01-01

    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.

  9. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Mattus, C.H.; Mattus, A.J.

    1994-03-01

    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).

  11. 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.

  12. 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.

  13. 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.

  14. 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).

  15. 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).

  16. 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.

  17. 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.

  18. 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.

  19. 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.

  20. 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.

  1. 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.

  2. Helium and fission gas behaviour in magnesium aluminate spinel and zirconia for actinide transmutation

    NARCIS (Netherlands)

    Damen, P.M.G.

    2003-01-01

    In order to reduce the long-term radiotoxicity of spent nuclear fuel, many studies are performed on partitioning and transmutation of actinides. In such a scenario, the long-lived radio-isotopes (mostly actinides) are partitioned from the nuclear waste, and subsequently transmuted or fissioned in a

  3. 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

  4. 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.

  5. 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.

  6. 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.

  7. Recovery and chemical purification of actinides at JRC, Karlsruhe

    Science.gov (United States)

    Bokelund, H.; Apostolidis, C.; Glatz, J.-P.

    1989-07-01

    The application of actinide elements in research and in technology is many times subject to rather stringent purity requirements; often a nuclear grade quality is specified. The additional possible demand for a high isotopic purity is a special feature in the handling of these elements. The amount of actinide elements contained in or adhering to materials declared as waste should be low for safety reasons and out of economic considerations. The release of transuranium elements to the environment must be kept negligible. For these and for other reasons a keen interest in the separation of actinides from various materials exists, either for a re-use through recycling, or for their safe confinement in waste packages. This paper gives a short review of the separation methods used for recovery and purification of actinide elements over the past years in the European Institute for Transuranium Elements. The methods described here involve procedures based on precipitation, ion exchange or solvent extraction; often used in a combination. The extraction methods were preferably applied in a Chromatographie column mode. The actinide elements purified and/or separated from each other by the above methods include uranium, neptunium, plutonium, americium, curium, and californium. For the various elements the work was undertaken with different aims, ranging from reprocessing and fabrication of nuclear fuels on a kilogramme scale, over the procurement of alpha-free waste, to the preparation of neutron sources of milligramme size.

  8. Iron (III) Matrix Effects on Mineralization and Immobilization of Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Cynthia-May S. Gong; Tyler A. Sullens; Kenneth R. Czerwinski

    2006-01-01

    Abstract - A number of models for the Yucca Mountain Project nuclear waste repository use studies of actinide sorption onto well-defined iron hydroxide materials. In the case of a waste containment leak, however, a complex interaction between dissolved waste forms and failed containment vessel components can lead to immediate precipitation of migratory iron and uranyl in the silicate rich near-field environment. Use of the Fe(III) and UO22+ complexing agent acetohydroxamic acid (AHA) as a colorimetric agent for visible spectrophotometry is well-known. Using the second derivative of these spectra a distinct shift in iron complexation in the presence of silicate is seen that is not seen with uranyl or alone. Silica also decreases the ability of uranyl and ferric solutions to absorb hydroxide, hastening precipitation. These ferric silicate precipitates are highly amorphous and soluble. Precipitates formed in the presence of uranyl below ~1 mol% exhibit lower solubility than precipitates from up to 50 mol % and of uranyl silicates alone.

  9. 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.

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

    Science.gov (United States)

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

    2011-07-01

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

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

    Science.gov (United States)

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

    2013-09-15

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

  12. 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.

  13. 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, 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.

  14. 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.

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

    Science.gov (United States)

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

    1977-01-01

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

  16. 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.

  17. Device for Detecting Actinides, Method for Detecting Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Stevens, Fred J.; Wilkins-Stevens, Priscilla

    1998-10-29

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

  18. Preliminary evaluation of alternative forms for immobilization of Savannah River Plant high-level waste. [Eleven alternative solid forms

    Energy Technology Data Exchange (ETDEWEB)

    Stone, J.A.; Goforth, S.T. Jr.; Smith, P.K.

    1979-12-01

    An evaluation of available information on eleven alternative solid forms for immobilization of SRP high-level waste has been completed. Based on the assessment of both product and process characteristics, four forms were selected for more detailed evaluation: (1) borosilicate glass made in the reference process, (2) a high-silica glass made from a porous glass matrix, (3) crystalline ceramics such as supercalcine or SYNROC, and (4) ceramics coated with an impervious barrier. The assessment includes a discussion of product and process characteristics for each of the eleven forms, a cross comparison of these characteristics for the forms, and the bases for selecting the most promising forms for further study.

  19. 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.

  20. 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.

  1. Advanced waste forms research and development. First quarterly report

    Energy Technology Data Exchange (ETDEWEB)

    McCarthy, G.J.

    1975-08-05

    Activities during the last two months are described. A significant portion of time was spent reviewing the literature on the Cs/sub 2/O-Al/sub 2/O/sub 3/-SiO/sub 2/ system, on the use of clays and zeolites for Cs-fixation of aqueous wastes, and on silicate-phosphate apatite structure crystal chemistry. The results from the latest group of compatibility studies (CS-runs) were used to modify the first demonstration supercalcine formulation so that it is more in line with the actual crystalline phase formation. Supercalcine formuation 75-2 is described.

  2. 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

  3. 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.

  4. 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.

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

    Science.gov (United States)

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

    2014-04-01

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

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

    NARCIS (Netherlands)

    Nikishkin, N.

    2013-01-01

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

  7. Study on the Extraction of Actinides From Simulated High-level Liquid Waste by Mixture of DHDECMP and TBP in Kerosene

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    The distribution ratios of U(VI), Np(V), Pu(IV) and Am(III) are measured by the single stage extraction experiments of simulated high-level liquid waste with 22%DHDECMP-42%TBP/OK. The extraction behavior of U, Np, Pu and Am in simulated high-level liquid waste is determined on miniature countercurrent centrifugal contactor cascade (6 stages for extraction, 2 stages for scrubbing, 6 stages for stripping, AF : AX : AS=1 : 1.5 : 0.5; BF : BX=1 : 1). The experimental results show that removal efficiency of U(VI), Np(V), Pu(IV) and Am(III) from simulated high-level liquid waste, all of them ,is equal or more than 99.9%. The stripping efficiency of U(VI),

  8. Supercritical Carbon Dioxide-Soluble Ligands for Extracting Actinide Metal Ions from Porous Solids

    Energy Technology Data Exchange (ETDEWEB)

    Joan Brennecke; Mark Dietz; Richard Barrans; Alabert Herlinger

    2003-07-03

    Numerous types of actinide-bearing waste materials are found throughout the DOE complex. Most of these wastes consist of large volumes of non-hazardous materials contaminated with relatively small quantities of actinide elements. Separation of these wastes into their inert and radioactive components would dramatically reduce the costs of stabilization and disposal. For example, the DOE is responsible for decontaminating concrete within 7000 surplus contaminated buildings. The best technology now available for removing surface contamination from concrete involves removing the surface layer by grit blasting, which produces a large volume of blasting residue containing a small amount of radioactive material. Disposal of this residue is expensive because of its large volume and fine particulate nature. Considerable cost savings would result from separation of the radioactive constituents and stabilization of the concrete dust. Similarly, gas diffusion plants for uranium enrichment contain valuable high-purity nickel in the form of diffusion barriers. Decontamination is complicated by the extremely fine pores in these barriers, which are not readily accessible by most cleaning techniques. A cost-effect method for the removal of radioactive contaminants would release this valuable material for salvage.

  9. 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.

  10. 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)

  11. Transuranic and Low-Level Boxed Waste Form Nondestructive Assay Technology Overview and Assessment

    Energy Technology Data Exchange (ETDEWEB)

    G. Becker; M. Connolly; M. McIlwain

    1999-02-01

    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. 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.

  13. 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.

  14. 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

  15. Radiation Effects in Nuclear Waste Materials

    Energy Technology Data Exchange (ETDEWEB)

    Weber, William J.

    2005-09-30

    The objective of this project is to develop a fundamental understanding of radiation effects in glasses and ceramics, as well as the influence of solid-state radiation effects on aqueous dissolution kinetics, which may impact the performance of nuclear waste forms and stabilized nuclear materials. This work provides the underpinning science to develop improved glass and ceramic waste forms for the immobilization and disposition of high-level tank waste, excess plutonium, plutonium residues and scrap, other actinides, and other nuclear waste streams. Furthermore, this work is developing develop predictive models for the performance of nuclear waste forms and stabilized nuclear materials. Thus, the research performed under this project has significant implications for the immobilization of High-Level Waste (HLW) and Nuclear Materials, two mission areas within the Office of Environmental Management (EM). With regard to the HLW mission, this research will lead to improved understanding of radiation-induced degradation mechanisms and their effects on dissolution kinetics, as well as development of predictive models for waste form performance. In the Nuclear Materials mission, this research will lead to improvements in the understanding of radiation effects on the chemical and structural properties of materials for the stabilization and long-term storage of plutonium, highly-enriched uranium, and other actinides. The research uses plutonium incorporation, ion-beam irradiation, and electron-beam irradiation to simulate the effects of alpha decay and beta decay on relevant glasses and ceramics. The research under this project has the potential to result in improved glass and ceramic materials for the stabilization and immobilization of high-level tank waste, plutonium residues and scraps, surplus weapons plutonium, highly-enriched uranium, other actinides, and other radioactive materials.

  16. Radiation Effects in Nuclear Waste Materials

    Energy Technology Data Exchange (ETDEWEB)

    Weber, William J.

    2005-06-01

    The objective of this project is to develop a fundamental understanding of radiation effects in glasses and ceramics, as well as the influence of solid-state radiation effects on aqueous dissolution kinetics, which may impact the performance of nuclear waste forms and stabilized nuclear materials. This work provides the underpinning science to develop improved glass and ceramic waste forms for the immobilization and disposition of high-level tank waste, excess plutonium, plutonium residues and scrap, other actinides, and other nuclear waste streams. Furthermore, this work is developing develop predictive models for the performance of nuclear waste forms and stabilized nuclear materials. Thus, the research performed under this project has significant implications for the immobilization of High-Level Waste (HLW) and Nuclear Materials, two mission areas within the Office of Environmental Management (EM). With regard to the HLW mission, this research will lead to improved understanding of radiation-induced degradation mechanisms and their effects on dissolution kinetics, as well as development of predictive models for waste form performance. In the Nuclear Materials mission, this research will lead to improvements in the understanding of radiation effects on the chemical and structural properties of materials for the stabilization and long-term storage of plutonium, highly-enriched uranium, and other actinides. The research uses plutonium incorporation, ion-beam irradiation, and electron-beam irradiation to simulate the effects of alpha decay and beta decay on relevant glasses and ceramics. The research under this project has the potential to result in improved glass and ceramic materials for the stabilization and immobilization of high-level tank waste, plutonium residues and scraps, surplus weapons plutonium, highly-enriched uranium, other actinides, and other radioactive materials.

  17. Synthesis and Characterization of Templated Ion Exchange Resins for the Selective Complexation of Actinide Ions

    Energy Technology Data Exchange (ETDEWEB)

    Uy, O. Manual

    2001-03-01

    The purpose of this research is to develop a polymeric extractant for the selective complexation of uranyl ions (and subsequently other actinyl and actinide ions) from aqueous solutions (lakes, streams, waste tanks and even body fluids). Chemical insights into what makes a good complexation site will be used to synthesize reagents tailor-made for the complexation of uranyl and other actinide ions. These insights, derived from studies of molecular recognition include ion coordination number and geometry, ionic size and ionic shape, as well as ion to ligand thermodynamic affinity. Selectivity for a specific actinide ion will be obtained by providing the polymers with cavities lined with complexing ligands so arranged as to match the charge, coordination number, coordination geometry, and size of the actinide metal ion. These cavity-containing polymers will be produced by using a specific ion (or surrogate) as a template around which monomeric complexing ligands will be polymerized. The complexing ligands will be ones containing functional groups known to form stable complexes with a specific ion and less stable complexes with other cations. Prior investigator's approaches for making templated resins for metal ions have had marginal success. We have extended and amended these methodologies in our work with Pb(II) and uranyl ion, by changing the order of the steps, by the inclusion of sonication, by using higher complex loading, and the selection of functional groups with better complexation constants. This has resulted in significant improvements to selectivity. The unusual shape of the uranyl ion suggests that this approach will result in even greater selectivities than already observed for Pb(II). Preliminary data obtained for uranyl templated polymers shows unprecedented selectivity and has resulted in the first ion selective electrode for uranyl ion.

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

    Energy Technology Data Exchange (ETDEWEB)

    Lopez, Ch

    2003-07-01

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

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

    Directory of Open Access Journals (Sweden)

    Bourg Stéphane

    2015-12-01

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

  20. 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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1994-12-31

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

  2. 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.

  3. 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).

  4. 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.

  5. 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.

  6. 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.).

  7. Actinide transmutation in nuclear reactors

    Energy Technology Data Exchange (ETDEWEB)

    Bultman, J.H.

    1995-01-17

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

  8. 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.

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

    Science.gov (United States)

    Warin, Dominique

    2010-03-01

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

  10. 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...

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-09-01

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

  12. Actinides in irradiated graphite of RBMK-1500 reactor

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-10-01

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

  13. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1995-01-01

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

  15. Bentonite-Clay Waste Form for the Immobilization of Cesium and Strontium from Fuel Processing Waste Streams

    Energy Technology Data Exchange (ETDEWEB)

    Kaminski, Michael D. [Argonne National Lab. (ANL), Argonne, IL (United States); Mertz, Carol J. [Argonne National Lab. (ANL), Argonne, IL (United States)

    2016-01-01

    The physical properties of a surrogate waste form containing cesium, strontium, rubidium, and barium sintered into bentonite clay were evaluated for several simulant feed streams: chlorinated cobalt dicarbollide/polyethylene glycol (CCD-PEG) strip solution, nitrate salt, and chloride salt feeds. We sintered bentonite clay samples with a loading of 30 mass% of cesium, strontium, rubidium, and barium to a density of approximately 3 g/cm3. Sintering temperatures of up to 1000°C did not result in volatility of cesium. Instead, there was an increase in crystallinity of the waste form upon sintering to 1000ºC for chloride- and nitrate-salt loaded clays. The nitrate salt feed produced various cesium pollucite phases, while the chloride salt feed did not produce these familiar phases. In fact, many of the x-ray diffraction peaks could not be matched to known phases. Assemblages of silicates were formed that incorporated the Sr, Rb, and Ba ions. Gas evolution during sintering to 1000°C was significant (35% weight loss for the CCD-PEG waste-loaded clay), with significant water being evolved at approximately 600°C.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1980-01-01

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

  17. Secondary Waste Form Screening Test Results—THOR® Fluidized Bed Steam Reforming Product in a Geopolymer Matrix

    Energy Technology Data Exchange (ETDEWEB)

    Pires, Richard P.; Westsik, Joseph H.; Serne, R. Jeffrey; Mattigod, Shas V.; Golovich, Elizabeth C.; Valenta, Michelle M.; Parker, Kent E.

    2011-07-14

    Screening tests are being conducted to evaluate waste forms for immobilizing secondary liquid wastes from the Hanford Tank Waste Treatment and Immobilization Plant (WTP). Plans are underway to add a stabilization treatment unit to the Effluent Treatment Facility to provide the needed capacity for treating these wastes from WTP. The current baseline is to use a Cast Stone cementitious waste form to solidify the wastes. Through a literature survey, DuraLith alkali-aluminosilicate geopolymer, fluidized-bed steam reformation (FBSR) granular product encapsulated in a geopolymer matrix, and a Ceramicrete phosphate-bonded ceramic were identified both as candidate waste forms and alternatives to the baseline. These waste forms have been shown to meet waste disposal acceptance criteria, including compressive strength and universal treatment standards for Resource Conservation and Recovery Act (RCRA) metals (as measured by the toxicity characteristic leaching procedure [TCLP]). Thus, these non-cementitious waste forms should also be acceptable for land disposal. Information is needed on all four waste forms with respect to their capability to minimize the release of technetium. Technetium is a radionuclide predicted to be in the secondary liquid wastes in small quantities, but the Integrated Disposal Facility (IDF) risk assessment analyses show that technetium, even at low mass, produces the largest contribution to the estimated IDF disposal impacts to groundwater.

  18. X-ray diffraction of slag-based sodium salt waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Langton, C. A. [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)

    2014-09-30

    The attached report documents sample preparation and x-ray diffraction results for a series of cement and blended cement matrices prepared with either water or a 4.4 M Na salt solution. The objective of the study was to provide initial phase characterization for the Cementitious Barriers Partnership reference case cementitious salt waste form. This information can be used to: 1) generate a base line for the evolution of the waste form as a function of time and conditions, 2) potentially to design new binders based on mineralogy of the binder, 3) understand and predict anion and cation leaching behavior of contaminants of concern, and 4) predict performance of the waste forms for which phase solubility and thermodynamic data are available.

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

    Energy Technology Data Exchange (ETDEWEB)

    Weber, William J. [Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Zhang, Yanwen [Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering

    2016-09-20

    This is the final report of the NEUP project “Radiation and Thermal Effects on Used Nuclear Fuel and Nuclear Waste Forms.” This project started on July 1, 2012 and was successfully completed on June 30, 2016. This report provides an overview of the main achievements, results and findings through the duration of the project. Additional details can be found in the main body of this report and in the individual Quarterly Reports and associated Deliverables of this project, which have been uploaded in PICS-NE. The objective of this research was to advance understanding and develop validated models on the effects of self-radiation from beta and alpha decay on the response of used nuclear fuel and nuclear waste forms during high-temperature interim storage and long-term permanent disposition. To achieve this objective, model used-fuel materials and model waste form materials were identified, fabricated, and studied.

  20. Actinide and lanthanide separation process (ALSEP)

    Science.gov (United States)

    Guelis, Artem V.

    2013-01-15

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

  1. Chemical stability of seven years aged cement-PET composite waste form containing radioactive borate waste simulates

    Science.gov (United States)

    Saleh, H. M.; Tawfik, M. E.; Bayoumi, T. A.

    2011-04-01

    Different samples of radioactive borate waste simulate [originating from pressurized water reactors (PWR)] have been prepared and solidified after mixing with cement-water extended polyester composite (CPC). The polymer-cement composite samples were prepared from recycled poly (ethylene terephthalate) (PET) waste and cement paste (water/cement ratio of 40%). The prepared samples were left to set at room temperature (25 °C ± 5) under humid conditions. After 28 days curing time the obtained specimens were kept in their molds to age for 7 years under ambient conditions. Cement-polymer composite waste form specimens (CPCW) have been subjected to leach tests for both 137Cs and 60Co radionuclides according to the method proposed by the International Atomic Energy Agency (IAEA). Leaching tests were justified under various factors that may exist within the disposal site (e.g. type of leachant, surrounding temperature, leachant behavior, the leachant volume to CPCW surface area…). The obtained data after 260 days of leaching revealed that after 7 years of aging the candidate cement-polymer composite (CPC) containing radioactive borate waste samples are characterized by adequate chemical stability required for the long-term disposal process.

  2. Chemical stability of seven years aged cement-PET composite waste form containing radioactive borate waste simulates

    Energy Technology Data Exchange (ETDEWEB)

    Saleh, H.M., E-mail: hosamsaleh70@yahoo.com [Radioisotope Department, Atomic Energy Authority, Dokki (Egypt); Tawfik, M.E. [Department of Polymers and Pigments, National Research Center, Dokki (Egypt); Bayoumi, T.A. [Radioisotope Department, Atomic Energy Authority, Dokki (Egypt)

    2011-04-15

    Different samples of radioactive borate waste simulate [originating from pressurized water reactors (PWR)] have been prepared and solidified after mixing with cement-water extended polyester composite (CPC). The polymer-cement composite samples were prepared from recycled poly (ethylene terephthalate) (PET) waste and cement paste (water/cement ratio of 40%). The prepared samples were left to set at room temperature (25 deg. C {+-} 5) under humid conditions. After 28 days curing time the obtained specimens were kept in their molds to age for 7 years under ambient conditions. Cement-polymer composite waste form specimens (CPCW) have been subjected to leach tests for both {sup 137}Cs and {sup 60}Co radionuclides according to the method proposed by the International Atomic Energy Agency (IAEA). Leaching tests were justified under various factors that may exist within the disposal site (e.g. type of leachant, surrounding temperature, leachant behavior, the leachant volume to CPCW surface area...). The obtained data after 260 days of leaching revealed that after 7 years of aging the candidate cement-polymer composite (CPC) containing radioactive borate waste samples are characterized by adequate chemical stability required for the long-term disposal process.

  3. ENHANCING ADVANCED CANDU PROLIFERATION RESISTANCE FUEL WITH MINOR ACTINIDES

    Energy Technology Data Exchange (ETDEWEB)

    Gray S. Chang

    2010-05-01

    The advanced nuclear system will significantly advance the science and technology of nuclear energy systems and to enhance the spent fuel proliferation resistance. Minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. MAs can play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In this work, an Advanced CANDU Reactor (ACR) fuel unit lattice cell model with 43 UO2 fuel rods will be used to investigate the effectiveness of a Minor Actinide Reduction Approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance. The main MARA objective is to increase the 238Pu / Pu isotope ratio by using the transuranic nuclides (237Np and 241Am) in the high burnup fuel and thereby increase the proliferation resistance even for a very low fuel burnup. As a result, MARA is a very effective approach to enhance the proliferation resistance for the on power refueling ACR system nuclear fuel. The MA transmutation characteristics at different MA loadings were compared and their impact on neutronics criticality assessed. The concept of MARA, significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms for peace and the intermediate term of nuclear energy reconnaissance.

  4. Feasibility of metallurgical waste encapsulation in a clay formed matrix

    Science.gov (United States)

    Juhnevica, I.; Kucinska, J.; Sardiko, A.; Mezinskis, G.

    2011-12-01

    As a result of Joint Stock Company "Liepajas Metalurgs" production process there are produced certain quantity of substances that are harmful for environment and have to be encapsulated into stable structures. Company's target is modification of these substances into products that form stable compounds in order to avoid metal release in environment. Geopolymers can be synthesized from many materials with a high concentration of aluminosilicates such as metakaolin or fly ash. Heavy metal immobilization in geopolymeric structures is not thought to be caused by physical encapsulation alone, but also through adsorption of the metal ions into the geopolymer structure and possibly even bonding of the metal ions into the structure. All samples have been analyzed with X-Ray, FTIR spectroscopy; chemical analysis and compressive strength tests have been performed. Chemical analysis of geopolymeric samples shows that the main component leached from samples during the boiling in water is Na2O that can be explained by more alkaline components nature - Na2SiO3, NaOH, and SO3. Fe2O3 and ZnO are not detected in water extracts at all samples.

  5. Chemical durability and degradation mechanisms of HT9 based alloy waste forms with variable Zr content

    Energy Technology Data Exchange (ETDEWEB)

    Olson, L. N. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-10-30

    In Corrosion studies were undertaken on alloy waste forms that can result from advanced electrometallurgical processing techniques to better classify their durability and degradation mechanisms. The waste forms were based on the RAW3-(URe) composition, consisting primarily of HT9 steel and other elemental additions to simulate nuclear fuel reprocessing byproducts. The solution conditions of the corrosion studies were taken from an electrochemical testing protocol, and meant to simulate conditions in a repository. The alloys durability was examined in alkaline and acidic brines.

  6. Electrorecovery of actinides at room temperature

    Energy Technology Data Exchange (ETDEWEB)

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

    2008-01-01

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

  7. Summary Report: Glass-Ceramic Waste Forms for Combined Fission Products

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-09-23

    Glass-ceramic waste form development began in FY 2010 examining two combined waste stream options: (1) alkaline earth (CS) + lanthanide (Ln), and (2) + transition metal (TM) fission-product waste streams generated by the uranium extraction (UREX+) separations process. Glass-ceramics were successfully developed for both options however; Option 2 was selected over Option 1, at the conclusion of 2010, because Option 2 immobilized all three waste streams with only a minimal decrease in waste loading. During the first year, a series of three glass (Option 2) were fabricated that varied waste loading-WL (42, 45, and 50 mass%) at fixed molar ratios of CaO/MoO{sub 3} and B{sub 2}O{sub 3}/alkali both at 1.75. These glass-ceramics were slow cooled and characterized in terms of phase assemblage and preliminary irradiation stability. This fiscal year, further characterization was performed on the FY 2010 Option 2 glass-ceramics in terms of: static leach testing, phase analysis by transmission electron microscopy (TEM), and irradiation stability (electron and ion). Also, a new series of glass-ceramics were developed for Option 2 that varied the additives: Al{sub 2}O{sub 3} (0-6 mass%), molar ratio of CaO/MoO{sub 3} and B{sub 2}O{sub 3}/alkali (1.75 to 2.25) and waste loading (50, 55, and 60 mass%). Lastly, phase pure powellite and oxyapatite were synthesized for irradiation studies. Results of this fiscal year studies showed compositional flexibility, chemical stability, and radiation stability in the current glass-ceramic system. First, the phase assemblages and microstructure of all of the FY 2010 and 2011 glass-ceramics are very similar once subjected to the slow cool heat treatment. The phases identified in these glass-ceramics were oxyapatite, powellite, cerianite, and ln-borosilicate. This shows that variations in waste loading or additives can be accommodated without drastically changing the phase assemblage of the waste form, thus making the processing and performance

  8. Advanced Extraction Methods for Actinide/Lanthanide Separations

    Energy Technology Data Exchange (ETDEWEB)

    Scott, M.J.

    2005-12-01

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

  9. Hanford Waste Vitrification Plant Quality Assurance Program description for high-level waste form development and qualification. Revision 3, Part 2

    Energy Technology Data Exchange (ETDEWEB)

    1993-08-01

    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.

  10. DEVELOPMENT OF CERAMIC WASTE FORMS FOR AN ADVANCED NUCLEAR FUEL CYCLE

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-11-30

    A series of ceramic waste forms were developed and characterized for the immobilization of a Cesium/Lanthanide (CS/LN) waste stream anticipated to result from nuclear fuel reprocessing. Simple raw materials, including Al{sub 2}O{sub 3} and TiO{sub 2} were combined with simulated waste components to produce multiphase ceramics containing hollandite-type phases, perovskites (particularly BaTiO{sub 3}), pyrochlores and other minor metal titanate phases. Three fabrication methodologies were used, including melting and crystallizing, pressing and sintering, and Spark Plasma Sintering (SPS), with the intent of studying phase evolution under various sintering conditions. X-Ray Diffraction (XRD) and Scanning Electron Microscopy coupled with Energy Dispersive Spectroscopy (SEM/EDS) results showed that the partitioning of the waste elements in the sintered materials was very similar, despite varying stoichiometry of the phases formed. Identification of excess Al{sub 2}O{sub 3} via XRD and SEM/EDS in the first series of compositions led to a Phase II study, with significantly reduced Al{sub 2}O{sub 3} concentrations and increased waste loadings. The Phase II compositions generally contained a reduced amount of unreacted Al{sub 2}O{sub 3} as identified by XRD. Chemical composition measurements showed no significant issues with meeting the target compositions. However, volatilization of Cs and Mo was identified, particularly during melting, since sintering of the pressed pellets and SPS were performed at lower temperatures. Partitioning of some of the waste components was difficult to determine via XRD. SEM/EDS mapping showed that those elements, which were generally present in small concentrations, were well distributed throughout the waste forms.

  11. Thermodynamics of actinide complexation in solution at elevated temperatures: application of variable-temperature titration calorimetry.

    Science.gov (United States)

    Rao, Linfeng

    2007-06-01

    Studies of actinide complexation in solution at elevated temperatures provide insight into the effect of solvation and the energetics of complexation, and help to predict the chemical behavior of actinides in nuclear waste processing and disposal where temperatures are high. This tutorial review summarizes the data on the complexation of actinides at elevated temperatures and describes the methodology for thermodynamic measurements, with the emphasis on variable-temperature titration calorimetry, a highly valuable technique to determine the enthalpy and, under appropriate conditions, the equilibrium constants of complexation as well.

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

    Energy Technology Data Exchange (ETDEWEB)

    Fadil, M

    2003-03-01

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

  13. On the Durability of Nuclear Waste Forms from the Perspective of Long-Term Geologic Repository Performance

    Directory of Open Access Journals (Sweden)

    Yifeng Wang

    2013-12-01

    Full Text Available High solid/water ratios and slow water percolation cause the water in a repository to quickly (on a repository time scale reach radionuclide solubility controlled by the equilibrium with alteration products; the total release of radionuclides then becomes insensitive to the dissolution rates of primary waste forms. It is therefore suggested that future waste form development be focused on conditioning waste forms or repository environments to minimize radionuclide solubility, rather than on marginally improving the durability of primary waste forms.

  14. SPECIFIC SEQUESTERING AGENTS FOR THE ACTINIDES

    Energy Technology Data Exchange (ETDEWEB)

    Raymond, Kenneth N.; Smith, William L.; Weitl, Frederick L.; Durbin, Patricia W.; Jones, E.Sarah; Abu-Dari, Kamal; Sofen, Stephen R.; Cooper, Stephen R.

    1979-09-01

    This paper summarizes the current status of a continuing project directed toward the synthesis and characterization of chelating agents which are specific for actinide ions - especially Pu(IV) - using a biomimetic approach that relies on the observation that Pu(IV) and Fe(III) has marked similarities that include their biological transport and distribution in mammals. Since the naturally-occurring Fe(III) sequestering agents produced by microbes commonly contain hydroxamate and catecholate functional groups, these groups should complex the actinides very strongly and macrocyclic ligands incorporating these moieties are being prepared. We have reported the isolation and structure analysis of an isostructural series of tetrakis(catecholato) complexes with the general stoichiometry Na{sub 4}[M(C{sub 6}H{sub 4}O{sub 2}){sub 4}] • 21 H{sub 2}O (M = Th, U, Ce, Hf). These complexes are structural archetypes for the cavity that must be formed if an actinide-specific sequestering agent is to conform ideally to the coordination requirements of the central metal ion. The [M(cat){sub 4}]{sup 4-} complexes have the D{sub 2d} symmetry of the trigonal-faced dodecahedron.. The complexes Th [R'C(0)N(O)R]{sub 4} have been prepared where R = isopropyl and R' = t-butyl or neopentyl. The neopentyl derivative is also relatively close to an idealized D{sub 2d} dodecahedron, while the sterically more hindered t-butyl compound is distorted toward a cubic geometry. The synthesis of a series of 2, 3-dihydroxy-benzoyl amide derivatives of linear and cyclic tetraaza- and diazaalkanes is reported. Sulfonation of these compounds improves the metal complexation and in vivo removal of plutonium from test animals. These results substantially exceed the capabilities of compounds presently used for the therapeutic treatment of actinide contamination.

  15. On-line Technology Information System (OTIS): Solid Waste Management Technology Information Form (SWM TIF)

    Science.gov (United States)

    Levri, Julie A.; Boulanger, Richard; Hogan, John A.; Rodriguez, Luis

    2003-01-01

    Contents include the following: What is OTIS? OTIS use. Proposed implementation method. Development history of the Solid Waste Management (SWM) Technology Information Form (TIF) and OTIS. Current development state of the SWM TIF and OTIS. Data collection approach. Information categories. Critiques/questions/feedback.

  16. Technical support for GEIS: radioactive waste isolation in geologic formations. Volume 16. Repository preconceptual design studies: BPNL waste forms in salt

    Energy Technology Data Exchange (ETDEWEB)

    1978-04-01

    This volume, Volume 16, ''Repository Preconceptual Design Studies: BPNL Waste Forms in Salt,'' is one of a 23 volume series, ''Technical Support for GEIS: Radioactive Waste Isolation in Geologic Formations,'' Y/OWI/TM-36, which supplements the ''Contribution to Draft Generic Environmental Impact Statement on Commercial Waste Management: Radioactive Waste Isolation in Geologic Formations,'' Y/OWI/TM-44. The series provide a more complete technical basis for the preconceptual designs, resource requirements, and environmental source terms associated with isolating commercial LWR wastes in underground repositories in salt, granite, shale and basalt. Wastes are considered from three fuel cycles: uranium and plutonium recycling, no recycling of spent fuel and uranium-only recycling. This document describes a preconceptual design for a nuclear waste storage facility in salt. The waste forms assumed to arrive at the repository were supplied by Battelle Pacific Northwest Laboratories (BPNL). The facility design consists of several chambers excavated deep within a geologic formation together with access shafts and supportive surface structures. The facility design provides for: receiving and unloading waste containers; lowering them down shafts to the mine level; transporting them to the proper storage area and emplacing them in mined storage rooms. Drawings of the facility design are contained in TM-36/17, ''Drawings for Repository Preconceptual Design Studies: BPNL Waste Forms in Salt.''

  17. A comparison of new reagents and processes for hydrometallurgical processing of actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    2001-07-01

    The future viability of nuclear power as an electricity generation technology depends greatly on addressing all aspects of radioactive waste disposal. A closed fuel cycle with recycle and burnup of actinides is one important option for solving long-term waste sequestration issues. The 50 years of accumulated experience in application of solvent extraction to the processing of spent nuclear fuels uniquely qualifies this technology for actinide partitioning. However, employment of new reagents and development of new processes must be reconciled with century 21 expectations for environment protection. The interrelationship between the separations potential and waste disposal aspects of new reagents and processes are discussed in this report. (author)

  18. Development of a Waste Treatment Process to Deactivate Reactive Uranium Metal and Produce a Stable Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    Gates-Anderson, D D; Laue, C A; Fitch, T E

    2002-01-17

    This paper highlights the results of initial investigations conducted to support the development of an integrated treatment process to convert pyrophoric metallic uranium wastes to a non-pyrophoric waste that is acceptable for land disposal. Several dissolution systems were evaluated to determine their suitability to dissolve uranium metal and that yield a final waste form containing uranium specie(s) amenable to precipitation, stabilization, adsorption, or ion exchange. During initial studies, one gram aliquots of uranium metal or the uranium alloy U-2%Mo were treated with 5 to 60 mL of selected reagents. Treatment systems screened included acids, acid mixtures, and bases with and without addition of oxidants. Reagents used included hydrochloric, sulfuric, nitric, and phosphoric acids, sodium hypochlorite, sodium hydroxide and hydrogen peroxide. Complete dissolution of the uranium turnings was achieved with the H{sub 3}PO{sub 4}/HCI system at room temperature within minutes. The sodium hydroxide/hydrogen peroxide, and sodium hypochlorite systems achieved complete dissolution but required elevated temperatures and longer reaction times. A ranking system based on criteria, such as corrosiveness, temperature, dissolution time, off-gas type and amount, and liquid to solid ratio, was designed to determine the treatment systems that should be developed further for a full-scale process. The highest-ranking systems, nitric acid/sulfuric acid and hydrochloric acid/phosphoric acid, were given priority in our follow-on investigations.

  19. RED-IMPACT. Impact of partitioning, transmutation and waste reduction technologies on the final nuclear waste disposal. Synthesis report

    Energy Technology Data Exchange (ETDEWEB)

    Lensa, Werner von; Nabbi, Rahim; Rossbach, Matthias (eds.) [Forschungszentrum Juelich GmbH (Germany)

    2008-07-01

    The impact of partitioning and transmutation (P and T) and waste reduction technologies on the nuclear waste management and particularly on the final disposal has been analysed within the EU-funded RED-IMPACT project. Five representative scenarios, ranging from direct disposal of the spent fuel to fully closed cycles (including minor actinide (MA) recycling) with fast neutron reactors or accelerator-driven systems (ADS), were chosen in the project to cover a wide range of representative waste streams, fuel cycle facilities and process performances. High and intermediate level waste streams have been evaluated for all of these scenarios with the aim of analysing the impact on geological disposal in different host formations such as granite, clay and salt. For each scenario and waste stream, specific waste package forms have been proposed and their main characteristics identified. Both equilibrium and transition analyses have been applied to those scenarios. The performed assessments have addressed parameters such as the total radioactive and radiotoxic inventory, discharges during reprocessing, thermal power and radiation emission of the waste packages, corrosion of matrices, transport of radioisotopes through the engineered and geological barriers or the resulting doses from the repository. The major conclusions of include the fact, that deep geological repository to host the remaining high level waste (HLW) and possibly the long-lived intermediate level waste (ILW) is unavoidable whatever procedure is implemented to manage waste streams from different fuel cycle scenarios including P and T of long-lived transuranic actinides.

  20. Mechanical behaviour and diffusion of gas during neutron irradiation of actinides in ceramic inert matrices

    NARCIS (Netherlands)

    Neeft, E.A.C.

    2004-01-01

    Fission of actinides from nuclear waste in inert matrices (materials without uranium) can reduce the period in time that nuclear waste is more radiotoxic than uranium ore that is the rock from which ordinary reactor fuel is made. A pioneering study is performed with the inert matrices: MgO, MgAl2O4,

  1. Glass composite waste forms for iodine confined in bismuth-embedded SBA-15

    Science.gov (United States)

    Yang, Jae Hwan; Park, Hwan Seo; Ahn, Do-Hee; Yim, Man-Sung

    2016-11-01

    The aim of this study was to stabilize bismuth-embedded SBA-15 that captured iodine gas by fabrication of monolithic waste forms. The iodine containing waste was mixed with Bi2O3 (a stabilizing additive) and low-temperature sintering glass followed by pelletizing and the sintering process to produce glass composite materials. Iodine volatility during the sintering process was significantly affected by the ratio of Bi2O3 and the glass composition. It was confirmed that BiI3, the main iodine phase within bismuth-embedded SBA-15, was effectively transformed to the mixed phases of Bi5O7I and BiOI. The initial leaching rates of iodine from the glass composite waste forms ranged 10-3-10-2 g/m2 day, showing the stability of the iodine phases encapsulated by the glassy networks. It was also observed that common groundwater anions (e.g., chloride, carbonate, sulfite, and fluoride) elevated the iodine leaching rate by anion exchange reactions. The present results suggest that the glass composite waste form of bismuth-embedded SBA-15 could be a candidate material for stable storage of 129I.

  2. Yucca Mountain project canister material corrosion studies as applied to the electrometallurgical treatment metallic waste form

    Energy Technology Data Exchange (ETDEWEB)

    Keiser, D.D.

    1996-11-01

    Yucca Mountain, Nevada is currently being evaluated as a potential site for a geologic repository. As part of the repository assessment activities, candidate materials are being tested for possible use as construction materials for waste package containers. A large portion of this testing effort is focused on determining the long range corrosion properties, in a Yucca Mountain environment, for those materials being considered. Along similar lines, Argonne National Laboratory is testing a metallic alloy waste form that also is scheduled for disposal in a geologic repository, like Yucca Mountain. Due to the fact that Argonne`s waste form will require performance testing for an environment similar to what Yucca Mountain canister materials will require, this report was constructed to focus on the types of tests that have been conducted on candidate Yucca Mountain canister materials along with some of the results from these tests. Additionally, this report will discuss testing of Argonne`s metal waste form in light of the Yucca Mountain activities.

  3. Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment

    Energy Technology Data Exchange (ETDEWEB)

    Pierce, Eric M.; McGrail, B. Peter; Rodriguez, Elsa A.; Schaef, Herbert T.; Saripalli, Prasad; Serne, R. Jeffrey; Krupka, Kenneth M.; Martin, P. F.; Baum, Steven R.; Geiszler, Keith N.; Reed, Lunde R.; Shaw, Wendy J.

    2004-09-01

    This data package documents the experimentally derived input data on the representative waste glasses; LAWA44, LAWB45, and LAWC22. This data will be used for Subsurface Transport Over Reactive Multi-phases (STORM) simulations of the Integrated Disposal Facility (IDF) for immobilized low-activity waste (ILAW). The STORM code will be used to provide the near-field radionuclide release source term for a performance assessment to be issued in July 2005. Documented in this data package are data related to 1) kinetic rate law parameters for glass dissolution, 2) alkali (Na+)-hydrogen (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 (PUF) and product consistency (PCT) tests where used for accelerated weathering or aging of the glasses in order to determine a chemical reaction network of secondary phases that form. The majority of the thermodynamic data used in this data package were extracted from the thermody-namic database package shipped with the geochemical code EQ3/6, version 8.0. Because of the expected importance of 129I release from secondary waste streams being sent to IDF from various thermal treatment processes, parameter estimates for diffusional release and solubility-controlled release from cementitious waste forms were estimated from the available literature.

  4. Stability of ceramic waste forms in potential repository environments: a review

    Energy Technology Data Exchange (ETDEWEB)

    Johnston, R. J.; Palmer, R. A.

    1982-03-31

    Most scenarios for geologic disposal of high-level nuclear waste include the eventual intrusion of groundwater into the repository. Reactions in the system and eventual release of the radionuclides, if any, will be controlled by the chemistry of the groundwater, the surrounding rock, the waste form, and any engineered barrier materials that are present, as well as by the temperature and pressure of the system. This report is a compilation and evaluation of the work completed to date on interactions within the waste-form/host-rock/groundwater system at various points in its lifetime. General results from leaching experiments are presented as a basis for comparison. The factors involved in studying the complete system are discussed so that future research may avoid some of the oversights of past research. Although relatively little hard data on prototype waste-form/repository-system interactions exist at this time, the available data and their implications are discussed. Sorption studies and models for predicting radionuclide migration are also presented, again with a study of the factors involved.

  5. Hydrophilic actinide complexation studied by solvent extraction radiotracer technique

    Energy Technology Data Exchange (ETDEWEB)

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

    1996-10-01

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

  6. A development of the stabilization technology for the solid form of radioactive waste

    Energy Technology Data Exchange (ETDEWEB)

    Kim, T. G.; Lee, Y. H.; Lee, K. M.; Ann, S. J.; Son, J. S. [KAERI, Taejon (Korea, Republic of)

    2003-07-01

    In this study, a modified bituminization technology has been developed, which needs no grinding of the granular resin waste, and enables the solid form to keep its shape stability as good as that of a cemented solid form. Also, the study intended to apply the developed technology to the practical treatment of radioactive resin waste. In the experiment, the granular type resin was used and the straight-run distillation bitumen with penetration rate 60/70 was used as the solidifying agent. The PE was used as the additive. The shape stability increased remarkably with the additive of PE, which act as a binder in the solid form. The shape of the solid from was maintained without failure during the long-term exposure test when the additive content of spent PE is more than 10 wt %. The proper ranges of bitumen content, PE content and operating temperature are 30-50 wt %, 10-20 wt % and 180.deg.C respectively. The bituminized solid form of radioactive resin waste by the technology of this study has the remarkably superior quality than the conventional solid forms, partially for the shape stability.

  7. PRELIMINARY ASSESSMENT OF THE LOW-TEMPERATURE WASTE FORM TECHNOLOGY COUPLED WITH TECHNETIUM REMOVAL

    Energy Technology Data Exchange (ETDEWEB)

    Fox, K.

    2014-05-13

    The U.S. Department of Energy Office of Environmental Management (EM) is engaging the national laboratories to provide the scientific and technological rigor to support EM program and project planning, technology development and deployment, project execution, and assessment of program outcomes. As an early demonstration of this new responsibility, Pacific Northwest National Laboratory (PNNL) and Savannah River National Laboratory (SRNL) have been chartered to implement a science and technology program addressing low-temperature waste forms for immobilization of DOE aqueous waste streams, including technetium removal as an implementing technology. As a first step, the laboratories examined the technical risks and uncertainties associated with the Cast Stone waste immobilization projects at Hanford. Science and technology needs were identified for work associated with 1) conducting performance assessments and risk assessments of waste form and disposal system performance, and 2) technetium chemistry in tank wastes and separations of technetium from waste processing streams. Technical approaches to address the science and technology needs were identified and an initial sequencing priority was suggested. The following table summarizes the most significant science and technology needs and associated approaches to address those needs. These approaches and priorities will be further refined and developed as strong integrated teams of researchers from national laboratories, contractors, industry, and academia are brought together to provide the best science and technology solutions. Implementation of a science and technology program that addresses these needs by pursuing the identified approaches will have immediate benefits to DOE in reducing risks and uncertainties associated with near-term decisions regarding supplemental immobilization at Hanford. Longer term, the work has the potential for cost savings and for providing a strong technical foundation for future

  8. A simplified method for estimation of jarosite and acid-forming sulfates in acid mine wastes.

    Science.gov (United States)

    Li, Jun; Smart, Roger St C; Schumann, Russell C; Gerson, Andrea R; Levay, George

    2007-02-01

    In acid base accounting (ABA) estimates of acid mine wastes, the acid potential (AP) estimate can be improved by using the net carbonate value (NCV) reactive sulfide S method rather than total S assay methods but this does not give recovery of potentially acid producing ferrous and ferric sulfates present in many wastes. For more accurate estimation of AP, an effective, site-specific method to quantify acid sulfate salts, such as jarosite and melanterite, in waste rocks has been developed and tested on synthetic and real wastes. The SPOCAS (acid sulfate soils) methods have been modified to an effective, rapid method to speciate sulfate forms in different synthetic waste samples. A three-step sequential extraction procedure has been established. These steps are: (1) argon-purged water extraction (3 min) to extract soluble Fe(II) salts (particularly melanterite), epsomite and gypsum (1 wt.% S) as copper sulfides, the second step of roasting needs to be excluded from the procedure with an increased time of 4 M HCl extraction to 16 h for jarosite determination.

  9. Actinide Solubility and Speciation in the WIPP

    Energy Technology Data Exchange (ETDEWEB)

    Reed, Donald T. [Los Alamos National Laboratory

    2015-11-02

    The presentation begins with the role and need for nuclear repositories (overall concept, international updates (Sweden, Finland, France, China), US approach and current status), then moves on to the WIPP TRU repository concept (design, current status--safety incidents of February 5 and 14, 2014, path forward), and finally considers the WIPP safety case: dissolved actinide concentrations (overall approach, oxidation state distribution and redox control, solubility of actinides, colloidal contribution and microbial effects). The following conclusions are set forth: (1) International programs are moving forward, but at a very slow and somewhat sporadic pace. (2) In the United States, the Salt repository concept, from the perspective of the long-term safety case, remains a viable option for nuclear waste management despite the current operational issues/concerns. (3) Current model/PA prediction (WIPP example) are built on redundant conservatisms. These conservatisms are being addressed in the ongoing and future research to fill existing data gaps--redox control of plutonium by Fe(0, II), thorium (analog) solubility studies in simulated brine, contribution of intrinsic and biocolloids to the mobile concentration, and clarification of microbial ecology and effects.

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

    Energy Technology Data Exchange (ETDEWEB)

    Croff, A.G.; Blomeke, J.O.; Finney, B.C.

    1980-06-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Bringer, O

    2007-10-15

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

  12. Corrosion behavior of technetium waste forms exposed to various aqueous environments

    Energy Technology Data Exchange (ETDEWEB)

    Kolman, David Gary [Los Alamos National Laboratory; Jarvinen, Gordon [Los Alamos National Laboratory; Mausolf, Edward [UNIV OF NEVADA; Czerwinski, Ken [UNIV OF NEVADA; Poineau, Frederic [UNIV OF NEVADA

    2009-01-01

    Technetium is a long-lived beta emitter produced in high yields from uranium as a waste product in spent nuclear fuel and has a high degree of environmental mobility as pertechnetate. It has been proposed that Tc be immobilized into various metallic waste forms to prevent Tc mobility while producing a material that can withstand corrosion exposed to various aqueous medias to prevent the leachability of Tc to the environment over long periods of time. This study investigates the corrosion behavior of Tc and Tc alloyed with 316 stainless steel and Zr exposed to a variety of aqueous media. To date, there is little investigative work related to Tc corrosion behavior and less related to potential Tc containing waste forms. Results indicate that immobilizing Tc into stainless steel-zirconium alloys can be a promising technique to store Tc for long periods of time while reducing the need to separately store used nuclear fuel cladding. Initial results indicate that metallic Tc and its alloys actively corrode in all media. We present preliminary corrosion rates of 100% Tc, 10% Tc - 90% SS{sub 85%}Zr{sub 15%}, and 2% Tc - 98% SS{sub 85%}Zr{sub 15%} in varying concentrations of nitric acid and pH 10 NaOH using the resistance polarization method while observing the trend that higher concentrations of Tc alloyed to the sample tested lowers the corrosion rate of the proposed waste package.

  13. Waste Form and Indrift Colloids-Associated Radionuclide Concentrations: Abstraction and Summary

    Energy Technology Data Exchange (ETDEWEB)

    R. Aguilar

    2003-06-24

    This Model Report describes the analysis and abstractions of the colloids process model for the waste form and engineered barrier system components of the total system performance assessment calculations to be performed with the Total System Performance Assessment-License Application model. Included in this report is a description of (1) the types and concentrations of colloids that could be generated in the waste package from degradation of waste forms and the corrosion of the waste package materials, (2) types and concentrations of colloids produced from the steel components of the repository and their potential role in radionuclide transport, and (3) types and concentrations of colloids present in natural waters in the vicinity of Yucca Mountain. Additionally, attachment/detachment characteristics and mechanisms of colloids anticipated in the repository are addressed and discussed. The abstraction of the process model is intended to capture the most important characteristics of radionuclide-colloid behavior for use in predicting the potential impact of colloid-facilitated radionuclide transport on repository performance.

  14. Secondary Waste Form Down-Selection Data Package—DuraLith

    Energy Technology Data Exchange (ETDEWEB)

    Mattigod, Shas V.; Westsik, Joseph H.

    2011-09-15

    This data package developed for the DuraLith wasteform includes information available in the open literature and from data obtained from testing currently underway. DuraLith is an alkali-activated geopolymer waste form developed by the Vitreous State Laboratory at The Catholic University of America (VSL-CUA) for encapsulating liquid radioactive waste. A DuraLith waste form developed for treating Hanford secondary waste liquids is prepared by alkali-activation of a mixture of ground blast furnace slag and metakaolinite with sand used as a filler material. Based on optimization tests, solid waste loading of {approx}7.5% and {approx}14.7 % has been achieved using the Hanford secondary waste S1 and S4 simulants, respectively. The Na loading in both cases is equivalent to {approx}6 M. Some of the critical parameters for the DuraLith process include, hydrogen generation and heat evolution during activator solution preparation using the waste simulant, heat evolution during and after mixing the activator solution with the dry ingredients, and a working window of {approx}20 minutes to complete the pouring of the DuraLith mixture into molds. Results of the most recent testing indicated that the working window can be extended to {approx}30 minutes if 75 wt% of the binder components, namely, blast furnace slag and metakaolin are replaced by Class F fly ash. A preliminary DuraLith process flow sheet developed by VSL-CUA for processing Hanford secondary waste indicated that 10 to 22 waste monoliths (each 48 ft3 in volume) can be produced per day. There are no current pilot-scale or full-scale DuraLith plants under construction or in operation; therefore, the cost of DuraLith production is unknown. The results of the non-regulatory leach tests, EPA Draft 1313 and 1316, Waste Simulant S1-optimized DuraLith specimens indicated that the concentrations of RCRA metals (Ag, Cd, Cr, Hg, and Pb) in the leachates were well below the Universal Treatment Standard limits in 40 CFR 268

  15. Separations and Waste Forms Research and Development FY 2013 Accomplishments Report

    Energy Technology Data Exchange (ETDEWEB)

    Not Listed

    2013-12-01

    The Separations and Waste Form Campaign (SWFC) under the U.S. Department of Energy (DOE) Fuel Cycle Research and Development Program (FCRD) 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 fiscal year (FY) 2013 accomplishments report provides a highlight of the results of the research and development (R&D) efforts performed within SWFC in FY 2013. 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 the intent of the report is to highlight the many technical accomplishments made during FY 2013.

  16. Advanced Aqueous Separation Systems for Actinide Partitioning

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-04-02

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

  17. Nuclear fuel cycle-oriented actinides separation in China

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-04-01

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

  18. Actinide biocolloid formation in brine by halophilic bacteria

    Energy Technology Data Exchange (ETDEWEB)

    Gillow, J.B.; Francis, A.J.; Dodge, C.J. [Brookhaven National Lab., Upton, NY (United States); Harris, R.; Beveridge, T.J. [Univ. of Guelph, Ontario (Canada); Brady, P.V.; Papenguth, H.W. [Sandia National Labs., Albuquerque, NM (United States)

    1998-12-31

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

  19. ACTINIDE BIOCOLLOID FORMATION IN BRINE BY HALOPHILIC BACTERIA

    Energy Technology Data Exchange (ETDEWEB)

    GILLOW,J.B.; FRANCIS,A.J.; DODGE,C.J.; HARRIS,R.; BEVERIDGE,T.J.; BRADY,P.B.; PAPENGUTH,H.W.

    1998-11-09

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

  20. Actinide Biocolloid Formation in Brine by Halophilic Bacteria

    Energy Technology Data Exchange (ETDEWEB)

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

    1999-07-28

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Emery, R.M.; Klopfer, D.C.; Baker, D.A.; Soldat, J.K. (Battelle Pacific Northwest Labs., Richland, WA (USA))

    1981-04-01

    The purpose of this work is to establish a maximum potential for transporting actinides to man via fish consumption. The study took place in U-pond, a nuclear waste pond on the Hanford Site. It has concentrations of /sup 238/U, /sup 238/Pu, sup(239,240)Pu and /sup 241/Am that are approx. 3 orders of magnitude greater than background levels. Fish living in the pond contain higher actinide concentrations than those observed in fish from any other location. Experiments were performed in U-Pond to determine maximum quantities of actinides that could accumulate in fillets and whole bodies of two centrarchid fish species. Doses to hypothetical consumers were then estimated. Results indicate that highest concentrations occurring in bluegill or bass muscle after more than a year's exposure to the pond would not be sufficient to produce a significant radiation dose to a human consumer, even if he ate 0.5 kg (of the order of 1 lb) of these fillets every day for 70 yr. Natural predators (heron or coyote), having lifetime diets of whole fish from U-Pond, would receive less radiation dose from the ingested actinides than from natural background sources.

  2. 33rd Actinide Separations Conference

    Energy Technology Data Exchange (ETDEWEB)

    McDonald, L M; Wilk, P A

    2009-05-04

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

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

    DEFF Research Database (Denmark)

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

    2010-01-01

    The ground-state electronic structures of the actinide oxides AO, A2O3, and AO2 (A=U, Np, Pu, Am, Cm, Bk, and Cf) are determined from first-principles calculations, using the self-interaction corrected local spin-density approximation. Emphasis is put on the degree of f-electron localization, whi...... lanthanide oxides. The ionic nature of the actinide oxides emerges from the fact that only those compounds will form where the calculated ground-state valency agrees with the nominal valency expected from a simple charge counting....

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-01-01

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

  5. Direct Measurement of Surface Dissolution Rates in Potential Nuclear Waste Forms: The Example of Pyrochlore.

    Science.gov (United States)

    Fischer, Cornelius; Finkeldei, Sarah; Brandt, Felix; Bosbach, Dirk; Luttge, Andreas

    2015-08-19

    The long-term stability of ceramic materials that are considered as potential nuclear waste forms is governed by heterogeneous surface reactivity. Thus, instead of a mean rate, the identification of one or more dominant contributors to the overall dissolution rate is the key to predict the stability of waste forms quantitatively. Direct surface measurements by vertical scanning interferometry (VSI) and their analysis via material flux maps and resulting dissolution rate spectra provide data about dominant rate contributors and their variability over time. Using pyrochlore (Nd2Zr2O7) pellet dissolution under acidic conditions as an example, we demonstrate the identification and quantification of dissolution rate contributors, based on VSI data and rate spectrum analysis. Heterogeneous surface alteration of pyrochlore varies by a factor of about 5 and additional material loss by chemo-mechanical grain pull-out within the uppermost grain layer. We identified four different rate contributors that are responsible for the observed dissolution rate range of single grains. Our new concept offers the opportunity to increase our mechanistic understanding and to predict quantitatively the alteration of ceramic waste forms.

  6. Calculation of cohesive energy of actinide metals

    Institute of Scientific and Technical Information of China (English)

    钱存富; 陈秀芳; 余瑞璜; 耿平; 段占强

    1997-01-01

    According to empirical electron theory of solids and molecules (EET), an equation for calculating the cohesive energy of actinide metals is given, the cohesive energy of 9 actinide metals with known crystal structure is calculated, which is identical with the experimental values on the whole, and the cohesive energy of 6 actinide metals with unknown crystal structure is forecast.

  7. EVALUATION OF THOR MINERALIZED WASTE FORMS FOR THE DOE ADVANCED REMEDIATION TECHNOLOGIES PHASE 2 PROJECT

    Energy Technology Data Exchange (ETDEWEB)

    Crawford, C.; Jantzen, C.

    2012-02-02

    The U.S. Department of Energy's (DOE) Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford's tank waste. Currently there are approximately 56 million gallons of highly radioactive mixed wastes awaiting treatment. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Therefore, Supplemental Treatment is required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. The Supplemental Treatment chosen will immobilize that portion of the retrieved LAW that is not sent to the WTP's LAW Vitrification facility into a solidified waste form. The solidified waste will then be disposed on the Hanford site in the Integrated Disposal Facility (IDF). In addition, the WTP LAW Vitrification facility off-gas condensate known as WTP Secondary Waste (WTP-SW) will be generated and enriched in volatile components such as Cs-137, I-129, Tc-99, Cl, F, and SO{sub 4} that volatilize at the vitrification temperature of 1150 C in the absence of a continuous cold cap. The current waste disposal path for the WTP-SW is to recycle it to the supplemental LAW treatment to avoid a large steady state accumulation in the pretreatment-vitrification loop. Fluidized Bed Steam Reforming (FBSR) offers a moderate temperature (700-750 C) continuous method by which LAW and/or WTP-SW wastes can be processed irrespective of whether they contain organics, nitrates

  8. EVALUATION OF THOR MINERALIZED WASTE FORMS FOR THE DOE ADVANCED REMEDIATION TECHNOLOGIES PHASE 2 PROJECT

    Energy Technology Data Exchange (ETDEWEB)

    Crawford, C.; Jantzen, C.

    2012-02-02

    The U.S. Department of Energy's (DOE) Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford's tank waste. Currently there are approximately 56 million gallons of highly radioactive mixed wastes awaiting treatment. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Therefore, Supplemental Treatment is required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. The Supplemental Treatment chosen will immobilize that portion of the retrieved LAW that is not sent to the WTP's LAW Vitrification facility into a solidified waste form. The solidified waste will then be disposed on the Hanford site in the Integrated Disposal Facility (IDF). In addition, the WTP LAW Vitrification facility off-gas condensate known as WTP Secondary Waste (WTP-SW) will be generated and enriched in volatile components such as Cs-137, I-129, Tc-99, Cl, F, and SO{sub 4} that volatilize at the vitrification temperature of 1150 C in the absence of a continuous cold cap. The current waste disposal path for the WTP-SW is to recycle it to the supplemental LAW treatment to avoid a large steady state accumulation in the pretreatment-vitrification loop. Fluidized Bed Steam Reforming (FBSR) offers a moderate temperature (700-750 C) continuous method by which LAW and/or WTP-SW wastes can be processed irrespective of whether they contain organics, nitrates

  9. Status of plutonium ceramic immobilization processes and immobilization forms

    Energy Technology Data Exchange (ETDEWEB)

    Ebbinghaus, B.B.; Van Konynenburg, R.A. [Lawrence Livermore National Lab., CA (United States); Vance, E.R.; Jostsons, A. [Australian Nuclear Science and Technology Organization, Menai (Australia)] [and others

    1996-05-01

    Immobilization in a ceramic followed by permanent emplacement in a repository or borehole is one of the alternatives currently being considered by the Fissile Materials Disposition Program for the ultimate disposal of excess weapons-grade plutonium. To make Pu recovery more difficult, radioactive cesium may also be incorporated into the immobilization form. Valuable data are already available for ceramics form R&D efforts to immobilize high-level and mixed wastes. Ceramics have a high capacity for actinides, cesium, and some neutron absorbers. A unique characteristic of ceramics is the existence of mineral analogues found in nature that have demonstrated actinide immobilization over geologic time periods. The ceramic form currently being considered for plutonium disposition is a synthetic rock (SYNROC) material composed primarily of zirconolite (CaZrTi{sub 2}O{sub 7}), the desired actinide host phase, with lesser amounts of hollandite (BaAl{sub 2}Ti{sub 6}O{sub 16}) and rutile (TiO{sub 2}). Alternative actinide host phases are also being considered. These include pyrochlore (Gd{sub 2}Ti{sub 2}O{sub 7}), zircon (ZrSiO{sub 4}), and monazite (CePO{sub 4}), to name a few of the most promising. R&D activities to address important technical issues are discussed. Primarily these include moderate scale hot press fabrications with plutonium, direct loading of PuO{sub 2} powder, cold press and sinter fabrication methods, and immobilization form formulation issues.

  10. Radiation Effects in Nuclear Waste Materials

    Energy Technology Data Exchange (ETDEWEB)

    Weber, William J.; Corrales, L. Rene; Ness, Nancy J.; Williford, Ralph E.; Heinisch, Howard L.; Thevuthasan, Suntharampillai; Icenhower, Jonathan P.; McGrail, B. Peter; Devanathan, Ramaswami; Van Ginhoven, Renee M.; Song, Jakyoung; Park, Byeongwon; Jiang, Weilin; Begg, Bruce D.; Birtcher, R. B.; Chen, X.; Conradson, Steven D.

    2000-10-02

    Radiation effects from the decay of radionuclides may impact the long-term performance and stability of nuclear waste forms and stabilized nuclear materials. In an effort to address these concerns, the objective of this project was the development of fundamental understanding of radiation effects in glasses and ceramics, particularly on solid-state radiation effects and their influence on aqueous dissolution kinetics. This study has employed experimental, theoretical and computer simulation methods to obtain new results and insights into radiation damage processes and to initiate the development of predictive models. Consequently, the research that has been performed under this project has significant implications for the High-Level Waste and Nuclear Materials focus areas within the current DOE/EM mission. In the High-Level Waste (HLW) focus area, the results of this research could lead to improvements in the understanding of radiation-induced degradation mechanisms and their effects on dissolution kinetics, as well as development of predictive models for waste form performance. In the Nuclear Materials focus area, the results of this research could lead to improvements in the understanding of radiation effects on the chemical and structural properties of materials for the stabilization and long-term storage of plutonium, highly-enriched uranium, and other actinides. Ultimately, this research could result in improved glass and ceramic materials for the stabilization and immobilization of high-level tank waste, plutonium residues and scraps, surplus weapons plutonium, highly-enriched uranium, other actinides, and other radioactive materials.

  11. Actinides and Life's Origins.

    Science.gov (United States)

    Adam, Zachary

    2007-12-01

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

  12. Preliminary considerations concerning actinide solubilities

    Energy Technology Data Exchange (ETDEWEB)

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

    1980-01-01

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

  13. Electrochemical decontamination system for actinide processing gloveboxes

    Energy Technology Data Exchange (ETDEWEB)

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

    1998-03-01

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

  14. A science-based approach to understanding waste form durability in open and closed nuclear fuel cycles

    Science.gov (United States)

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

    2007-05-01

    There are two compelling reasons for understanding source term and near-field processes in a radioactive waste 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 degraded, the waste form is a primary control on 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 source term and near-field processes. This integrated model will be used to provide a basis for understanding the behaviour of the source term over long time periods (greater than 105 years). Such a fundamental and integrated experimental and modelling 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.

  15. Product acceptance of a certified Class C low-level waste form at the West Valley Demonstration Project

    Energy Technology Data Exchange (ETDEWEB)

    Valenti, P.J. [West Valley Nuclear Services Co., Inc., NY (United States); Maestas, E.; Yeazel, J.A. [Dept. of Energy, West Valley, NY (United States). West Valley Project Office; McIntosh, T.W. [Dept. of Energy, Washington, DC (United States). Office of Remedial Action and Waste Technology

    1989-11-01

    The Department of Energy, is charged with the solidification of high-level liquid waste (HLW) remaining from nuclear fuel reprocessing activities, which were conducted at West Valley, New York between 1966 and 1972. One important aspect of the West Valley Demonstration Project`s fully integrated waste program is the treatment and conditioning of low-level wastes which result from processing liquid high-level waste. The treatment takes place in the project`s Integrated Radwaste Treatment System which removes Cesium-137 from the liquid or supernatant phase of the HLW by utilizing an ion exchange technique. The resulting decontaminated and conditioned liquid waste stream is solidified into a Class C low-level cement waste form that meets the waste form criteria specified in NRC 10 CFR 61. The waste matrix is placed in 71-gallon square drums, remotely handled and stored on site until determination of final disposition. This paper discusses the programs in place at West Valley to ensure production of an acceptable cement-based product. Topics include the short and long term test programs to predict product storage and disposal performance, description of the Process Control Plan utilized to control and maintain cement waste form product specifications and finally discuss the operational performance characteristics of the Integrated Radwaste Treatment System. Operational data and product statistics are provided.

  16. Cold crucible induction melter test for crystalline ceramic waste form fabrication: A feasibility assessment

    Science.gov (United States)

    Amoroso, Jake W.; Marra, James; Dandeneau, Christopher S.; Brinkman, Kyle; Xu, Yun; Tang, Ming; Maio, Vince; Webb, Samuel M.; Chiu, Wilson K. S.

    2017-04-01

    The first scaled proof-of-principle cold crucible induction melter (CCIM) test to process a multiphase ceramic waste form from a simulated combined (Cs/Sr, lanthanide and transition metal fission products) commercial used nuclear fuel waste stream was recently conducted in the United States. X-ray diffraction, 2-D X-ray absorption near edge structure (XANES), electron microscopy, inductively coupled plasma-atomic emission spectroscopy (and inductively coupled plasma-mass spectroscopy for Cs), and product consistency tests were used to characterize the fabricated CCIM material. Characterization analyses confirmed that a crystalline ceramic with a desirable phase assemblage was produced from a melt using a CCIM. Primary hollandite, pyrochlore/zirconolite, and perovskite phases were identified in addition to minor phases rich in Fe, Al, or Cs. The material produced in the CCIM was chemically homogeneous and displayed a uniform phase assemblage with acceptable aqueous chemical durability.

  17. Preliminary evaluation of alternative waste form solidification processes. Volume I. Identification of the processes.

    Energy Technology Data Exchange (ETDEWEB)

    Treat, R.L.; Nesbitt, J.F.; Blair, H.T.; Carter, J.G.; Gorton, P.S.; Partain, W.L.; Timmerman, C.L.

    1980-04-01

    This document contains preconceptual design data on 11 processes for the solidification and isolation of nuclear high-level liquid wastes (HLLW). The processes are: in-can glass melting (ICGM) process, joule-heated glass melting (JHGM) process, glass-ceramic (GC) process, marbles-in-lead (MIL) matrix process, supercalcine pellets-in-metal (SCPIM) matrix process, pyrolytic-carbon coated pellets-in-metal (PCCPIM) matrix process, supercalcine hot-isostatic-pressing (SCHIP) process, SYNROC hot-isostatic-pressing (SYNROC HIP) process, titanate process, concrete process, and cermet process. For the purposes of this study, it was assumed that each of the solidification processes is capable of handling similar amounts of HLLW generated in a production-sized fuel reprocessing plant. It was also assumed that each of the processes would be enclosed in a shielded canyon or cells within a waste facility located at the fuel reprocessing plant. Finally, it was assumed that all of the processes would be subject to the same set of regulations, codes and standards. Each of the solidification processes converts waste into forms that may be acceptable for geological disposal. Each process begins with the receipt of HLLW from the fuel reprocessing plant. In this study, it was assumed that the original composition of the HLLW would be the same for each process. The process ends when the different waste forms are enclosed in canisters or containers that are acceptable for interim storage. Overviews of each of the 11 processes and the bases used for their identification are presented in the first part of this report. Each process, including its equipment and its requirements, is covered in more detail in Appendices A through K. Pertinent information on the current state of the art and the research and development required for the implementation of each process are also noted in the appendices.

  18. Measurement of Actinides in Molybdenum-99 Solution Analytical Procedure

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-11-01

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

  19. Environmental research on actinide elements

    Energy Technology Data Exchange (ETDEWEB)

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

    1987-08-01

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

  20. Recovery of minor actinides from irradiated superfact fuels

    Energy Technology Data Exchange (ETDEWEB)

    Apoltolidis, C.; Glatz, J.P.; Molinet, R.; Nicholl, A.; Pagliosa, G.; Romer, K.; Bokelund, H.; Koch, L. [European Commission, JRC, Institute fuer Transuranium Elements, Karlsruhe (Germany)

    1995-12-31

    It could be demonstrated that the reprocessing of fast reactor oxide fuels containing up to 45 % MA (Np and Am), irradiated in the PHENIX reactor in the frame of a transmutation study, is possible. The fuels were dissolved under PUREX type conditions in order to determine their behaviour in the head-end step of the reprocessing process. For one of the fuels containing 20 % Am and 20 % Np before irradiation, an almost complete partitioning of actinides from the dissolver solution could be achieved. Chromatographic extraction was used for the separation of the main bulk elements U, Pu and Np, whereas centrifugal extractors were used to separate the minor actinides from the remaining high level liquid wastes (HLLW). For the relevant radio-toxic isotopes a high recovery rate from the irradiation targets was reached. Those elements are thus available for new fuel fabrication. (authors) 12 refs.

  1. Actinide-specific sequestering agents and decontamination applications

    Energy Technology Data Exchange (ETDEWEB)

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

    1981-04-07

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

  2. Low-temperature setting phosphate ceramics for stabilization of DOE problem low level mixed-waste: I. Material and waste form development

    Energy Technology Data Exchange (ETDEWEB)

    Singh, D.; Wagh, A.; Knox, L. [Argonne National Lab., Argonne, IL (United States); Mayberry, J. [Science Applications International Corp., Idaho Falls, ID (United States)

    1994-03-01

    Chemically bonded phosphate ceramics are proposed as candidates for solidification and stabilization of some of the {open_quotes}problem{close_quotes} DOE low-level mixed wastes at low-temperatures. Development of these materials is crucial for stabilization of waste streams which have volatile species and any use of high-temperature technology leads to generation of off-gas secondary waste streams. Several phosphates of Mg, Al, and Zr have been investigated as candidate materials. Monoliths of these phosphates were synthesized using chemical routes at room or slightly elevated temperatures. Detailed physical and chemical characterizations have been conducted on some of these phosphates to establish their durability. Magnesium ammonium phosphate has shown to possess excellent mechanical and as well chemical properties. These phosphates were also used to stabilize a surrogate ash waste with a loading ranging from 25-35 wt.%. Characterization of the final waste forms show that waste immobilization is due to both chemical stabilization and physical encapsulation of the surrogate waste which is desirable for waste immobilization.

  3. Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment. Erratum

    Energy Technology Data Exchange (ETDEWEB)

    Smith, Gary L. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2016-09-06

    This report refers to or contains Kg values for glasses LAWA44, LAWB45 and LAWC22 affected by calculations errors as identified by Papathanassiu et al. (2011). The corrected Kg values are reported in an erratum included in the revised version of the original report. The revised report can be referenced as follows: Pierce E. M. et al. (2004) Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment. PNNL-14805 Rev. 0 Erratum. Pacific Northwest National Laboratory, Richland, WA, USA.

  4. Waste Form Release Calculations for the 2005 Integrated Disposal Facility Performance Assessment. Erratum

    Energy Technology Data Exchange (ETDEWEB)

    Smith, Gary L. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2016-09-06

    This report refers to or contains Kg values for glasses LAWA44, LAWB45 and LAWC22 affected by calculations errors as identified by Papathanassiu et al. (2011). The corrected Kg values are reported in an erratum included in the revised version of the original report. The revised report can be referenced as follows: Pierce E. M. et al. (2004) Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment. PNNL-14805 Rev. 0 Erratum. Pacific Northwest National Laboratory, Richland, WA, USA.

  5. Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment Erratum

    Energy Technology Data Exchange (ETDEWEB)

    Smith, Gary L. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2016-09-06

    This report refers to or contains Kg values for glasses LAWA44, LAWB45 and LAWC22 affected by calculations errors as identified by Papathanassiu et al. (2011). The corrected Kg values are reported in an erratum included in the revised version of the original report. The revised report can be referenced as follows: Pierce E. M. et al. (2004) Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment. PNNL-14805 Rev. 0 Erratum. Pacific Northwest National Laboratory, Richland, WA, USA.

  6. Waste Form Release Calculations for the 2005 Integrated Disposal Facility Performance Assessment Erratum

    Energy Technology Data Exchange (ETDEWEB)

    Smith, Gary L. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2016-09-06

    This report refers to or contains Kg values for glasses LAWA44, LAWB45 and LAWC22 affected by calculations errors as identified by Papathanassiu et al. (2011). The corrected Kg values are reported in an erratum included in the revised version of the original report. The revised report can be referenced as follows: Pierce E. M. et al. (2004) Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment. PNNL-14805 Rev. 0 Erratum. Pacific Northwest National Laboratory, Richland, WA, USA.

  7. TAILORING INORGANIC SORBENTS FOR SRS STRONTIUM AND ACTINIDE SEPARATIONS: OPTIMIZED MONOSODIUM TITANATE PHASE II FINAL REPORT

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D; Thomas Peters, T; Michael Poirier, M; Mark Barnes, M; Major Thompson, M; Samuel Fink, S

    2007-06-29

    This document provides a final report of Phase II testing activities for the development of a modified monosodium titanate (MST) that exhibits improved strontium and actinide removal characteristics compared to the baseline MST material. The activities included determining the key synthesis conditions for preparation of the modified MST, preparation of the modified MST at a larger scale by a commercial vendor, demonstration of the strontium and actinide removal characteristics with actual tank waste supernate and measurement of filtration characteristics. Key findings and conclusions include the following. Testing evaluated three synthetic methods and eleven process parameters for the optimum synthesis conditions for the preparation on an improved form of MST. We selected the post synthesis method (Method 3) for continued development based on overall sorbate removal performance. We successfully prepared three batches of the modified MST using Method 3 procedure at a 25-gram scale. The laboratory prepared modified MST exhibited increased sorption kinetics with simulated and actual waste solutions and similar filtration characteristics to the baseline MST. Characterization of the modified MST indicated that the post synthesis treatment did not significantly alter the particle size distribution, but did significantly increase the surface area and porosity compared to the original MST. Testing indicated that the modified MST exhibits reduced affinity for uranium compared to the baseline MST, reducing risk of fissile loading. Shelf-life testing indicated no change in strontium and actinide performance removal after storing the modified MST for 12-months at ambient laboratory temperature. The material releases oxygen during the synthesis and continues to offgas after the synthesis at a rapidly diminishing rate until below a measurable rate after 4 months. Optima Chemical Group LLC prepared a 15-kilogram batch of the modified MST using the post synthesis procedure (Method

  8. Study of the behavior of actinides continuously recycled in a hard spectrum reactor

    Energy Technology Data Exchange (ETDEWEB)

    Schofield, P.E.

    1980-12-01

    The behavior of actinides continuously recycled through the central region of an EBR-II type reactor was studied. Such a reactor would convert long-lived nuclear wastes to short-lived isotopes, and simultaneously produce useful power. This process is proposed as an alternative to the geological isolation of long-lived actinide wastes. A driver region of 50% U-235 enriched fuel provided a nearly-constant spectrum and flux that was extremely hard compared to standard LMFBRs. This resulted in a high fission-to-capture ratio for most isotopes. The original actinide fuel was the discharge from a LWR, cooled for two years, with 99.9% of the uranium and plutonium removed by chemical processing. Comparison was made between removal of both Pu and U and removal of only U in subsequent cycles. The latter case resulted in substantial quantities of trans-plutonics burned per cycle.

  9. Neutron capture measuremetns on minor actinides at the n_TOF facility at CERN: past, present and future

    OpenAIRE

    Cano Ott, Daniel; Colonna, Nicola; Tagliente, G.; Belloni, Fabio; Calviño Tavares, Francisco; Cortés Rossell, Guillem Pere; Poch Parés, Agustí; Pretel Sánchez, Carme

    2011-01-01

    The successful development of advanced nuclear systems for sustainable energy production and nuclear waste management depends on high quality nuclear data libraries. Recent sensitivity stud- ies and reports [1-3] have identi ed the need for substantially improving the accuracy of neutron cross-section data for minor actinides. The n TOF collaboration has initiated an ambitious exper- imental program for the measurement of neutron capture cross sections of minor actinides. Two e...

  10. Separation of tc from Uranium and development of metallic Technetium waste forms

    Science.gov (United States)

    Mausolf, Edward John

    The isotope Technetium-99 (99Tc) is a major fission product of the nuclear industry. In the last decade, approximately 20 tons of 99Tc have been produced by the US nuclear industry. Due to its long half-life (t1/2 = 214,000 yr), beta radiotoxicity, and high mobility as pertechnetate [TcO4]-, Tc represents long-term concern to the biosphere. Various options have been considered to manage 99Tc. One of them is its separation from spent fuel, conversion to the metal and incorporation into a metallic waste form for long-term disposal. After dissolution of spent fuel in nitric acid and extraction of U and Tc in organic media, previously developed methods can be used to separate Tc from U, convert the separate Tc stream to the metal and reuse the uranium component of the fuel. A variety of metallic waste forms, ranging from pure Tc metal to ternary Tc alloys combined with stainless steel (SS) and Zr are proposed. The goal of this work was to examine three major questions: What is the optimal method to separate Tc from U? After separation, what is the most efficient method to convert the Tc stream to Tc metal? Finally, what is the corrosion behavior of Tc metal, Tc-SS alloys and Tc-Zr-SS alloys in 0.01M NaCl? The goal is to predict the long term behavior of Tc metallic waste in a hypothetical storage environment. In this work, three methods have been used to separate Tc from U: anionic exchange resin, liquid-liquid extraction and precipitation. Of the three methods studied, anionic exchange resins is the most selective. After separation of Tc from U, three different methods were studied to convert the Tc stream to the metal: thermal treatment under hydrogen atmosphere, electrochemical and chemical reduction of pertechnetate in aqueous media. The thermal treatment of the Tc stream under hydrogen atmosphere is the preferred method to produce Tc metal. After Tc metal is isolated, it will be incorporated into a metal host phase. Three different waste forms were produced for

  11. Terahertz Time-Domain Spectroscopy for In Situ Monitoring of Ceramic Nuclear Waste Forms

    Science.gov (United States)

    Clark, Braeden M.; Sundaram, S. K.

    2016-10-01

    The use of terahertz time-domain spectroscopy (THz-TDS) is presented as a non-contact method for in situ monitoring of ceramic waste forms. Single-phase materials of zirconolite (CaZrTi2O7), pyrochlore (Nd2Ti2O7), and hollandite (BaCs0.3Cr2.3Ti5.7O16 and BaCs0.3CrFeAl0.3Ti5.7O16) were characterized. The refractive index and dielectric properties in THz frequencies demonstrate the ability to distinguish between these materials. Differences in processing methods show distinct changes in both the THz-TDS spectra and optical and dielectric properties of these ceramic phases. The temperature dependence of the refractive index and relative permittivity of pyrochlore and zirconolite materials in the range of 25-200 °C is found to follow an exponential increasing trend. This can also be used to monitor the temperature of the ceramic waste forms on storage over extended geological time scales.

  12. Closed Fuel Cycle Waste Treatment Strategy

    Energy Technology Data Exchange (ETDEWEB)

    Vienna, J. D. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Collins, E. D. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Crum, J. V. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Ebert, W. L. [Argonne National Lab. (ANL), Argonne, IL (United States); Frank, S. M. [Idaho National Lab. (INL), Idaho Falls, ID (United States); Garn, T. G. [Idaho National Lab. (INL), Idaho Falls, ID (United States); Gombert, D. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Jones, R. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Jubin, R. T. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Maio, V. C. [Idaho National Lab. (INL), Idaho Falls, ID (United States); Marra, J. C. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Matyas, J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Nenoff, T. M. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Riley, B. J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Sevigny, G. J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Soelberg, N. R. [Idaho National Lab. (INL), Idaho Falls, ID (United States); Strachan, D. M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Thallapally, P. K. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Westsik, J. H. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2015-02-01

    This study is aimed at evaluating the existing waste management approaches for nuclear fuel cycle facilities in comparison to the objectives of implementing an advanced fuel cycle in the U.S. under current legal, regulatory, and logistical constructs. The study begins with the Global Nuclear Energy Partnership (GNEP) Integrated Waste Management Strategy (IWMS) (Gombert et al. 2008) as a general strategy and associated Waste Treatment Baseline Study (WTBS) (Gombert et al. 2007). The tenets of the IWMS are equally valid to the current waste management study. However, the flowsheet details have changed significantly from those considered under GNEP. In addition, significant additional waste management technology development has occurred since the GNEP waste management studies were performed. This study updates the information found in the WTBS, summarizes the results of more recent technology development efforts, and describes waste management approaches as they apply to a representative full recycle reprocessing flowsheet. Many of the waste management technologies discussed also apply to other potential flowsheets that involve reprocessing. These applications are occasionally discussed where the data are more readily available. The report summarizes the waste arising from aqueous reprocessing of a typical light-water reactor (LWR) fuel to separate actinides for use in fabricating metal sodium fast reactor (SFR) fuel and from electrochemical reprocessing of the metal SFR fuel to separate actinides for recycle back into the SFR in the form of metal fuel. The primary streams considered and the recommended waste forms include; Tritium in low-water cement in high integrity containers (HICs); Iodine-129: As a reference case, a glass composite material (GCM) formed by the encapsulation of the silver Mordenite (AgZ) getter material in a low-temperature glass is assumed. A number of alternatives with distinct advantages are also considered including a fused silica waste form

  13. Extended Development Work to Validate a HLW Calcine Waste Form via INL's Cold Crucible Induction Melter

    Energy Technology Data Exchange (ETDEWEB)

    James A. King; Vince Maio

    2011-09-01

    To accomplish calcine treatment objectives, the Idaho Clean-up Project contractor, CWI, has chosen to immobilize the calcine in a glass-ceramic via the use of a Hot-Isostatic-Press (HIP); a treatment selection formally documented in a 2010 Record of Decision (ROD). Even though the HIP process may prove suitable for the calcine as specified in the ROD and validated in a number of past value engineering sessions, DOE is evaluating back-up treatment methods for the calcine as a result of the technical, schedule, and cost risk associated with the HIPing process. Consequently DOE HQ has requested DOE ID to make INL's bench-scale cold-crucible induction melter (CCIM) available for investigating its viability as a process alternate to calcine treatment. The waste form is the key component of immobilization of radioactive waste. Providing a solid, stable, and durable material that can be easily be stored is the rationale for immobilization of radioactive waste material in glass, ceramic, or glass-ceramics. Ceramic waste forms offer an alternative to traditional borosilicate glass waste forms. Ceramics can usually accommodate higher waste loadings than borosilicate glass, leading to smaller intermediate and long-term storage facilities. Many ceramic phases are known to possess superior chemical durability as compared to borosilicate glass. However, ceramics are generally multiphase systems containing many minor phase that make characterization and prediction of performance within a repository challenging. Additionally, the technologies employed in ceramic manufacture are typically more complex and expensive. Thus, many have proposed using glass-ceramics as compromise between in the more inexpensive, easier to characterize glass waste forms and the more durable ceramic waste forms. Glass-ceramics have several advantages over traditional borosilicate glasses as a waste form. Borosilicate glasses can inadvertently devitrify, leading to a less durable product that could

  14. Distribution and Solubility of Radionuclides and Neutron Absorbers in Waste Forms for Disposition of Plutonium Ash and Scraps, Excess Plutonium, and Miscellaneous Spent Nuclear Fuels

    Energy Technology Data Exchange (ETDEWEB)

    Dr. Denis M. Strachan; Dr. David K. Shuh; Dr. Rodney C. Ewing; Dr. Eric R. Vance

    2002-09-23

    The initial goal of this project was to investigate the solubility of radionuclides in glass and other potential waste forms for the purpose of increasing the waste loading in glass and ceramic waste forms. About one year into the project, the project decided to focus on two potential waste forms - glass at PNNL and itianate ceramics at the Australian Nuclear Science and Technology Organisation (ANSTO).

  15. DEVELOPMENT OF AN IMPROVED TITANATE-BASED SORBENT FOR STRONTIUM AND ACTINIDE SEPARATIONS UNDER STRONGLY ALKALINE CONDITIONS

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D.; Peters, T.; Taylor-Pashow, K.; Fink, S.

    2010-02-18

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 134,137}Cs, {sup 90}Sr, and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes at SRS include the sorption of {sup 90}Sr and alpha-emitting radionuclides onto monosodium titanate (MST) and caustic side solvent extraction of {sup 137}Cs. The MST and separated {sup 137}Cs is encapsulated along with the sludge fraction of high-level waste (HLW) into a borosilicate glass waste form for eventual entombment at a federal repository. The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes {sup 238}Pu, {sup 239}Pu, and {sup 240}Pu; {sup 237}Np; and uranium isotopes, {sup 235}U and {sup 238}U. This paper describes recent results evaluating the performance of an improved sodium titanate material that exhibits increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the current baseline material, MST.

  16. Radioactive Demonstration Of Mineralized Waste Forms Made From Hanford Low Activity Waste (Tank SX-105 And AN-103) By Fluidized Bed Steam Reformation

    Energy Technology Data Exchange (ETDEWEB)

    Jantzen, Carol; Herman, Connie; Crawford, Charles; Bannochie, Christopher; Burket, Paul; Daniel, Gene; Cozzi, Alex; Nash, Charles; Miller, Donald; Missimer, David

    2014-01-10

    One of the immobilization technologies under consideration as a Supplemental Treatment for Hanford’s Low Activity Waste (LAW) is Fluidized Bed Steam Reforming (FBSR). The FBSR technology forms a mineral waste form at moderate processing temperatures thus retaining and atomically bonding the halides, sulfates, and technetium in the mineral phases (nepheline, sodalite, nosean, carnegieite). Additions of kaolin clay are used instead of glass formers and the minerals formed by the FBSR technology offers (1) atomic bonding of the radionuclides and constituents of concern (COC) comparable to glass, (2) short and long term durability comparable to glass, (3) disposal volumes comparable to glass, and (4) higher Na2O and SO{sub 4} waste loadings than glass. The higher FBSR Na{sub 2}O and SO{sub 4} waste loadings contribute to the low disposal volumes but also provide for more rapid processing of the LAW. Recent FBSR processing and testing of Hanford radioactive LAW (Tank SX-105 and AN-103) waste is reported and compared to previous radioactive and non-radioactive LAW processing and testing.

  17. INTERNATIONAL PROGRAM: SUMMARY REPORT ON THE PROPERTIES OF CEMENTITIOUS WASTE FORMS

    Energy Technology Data Exchange (ETDEWEB)

    Harbour, J

    2007-03-02

    This report provides a summary of the results on the properties of cementitious waste forms obtained as part of the International Program. In particular, this report focuses on the results of Task 4 of the Program that was initially entitled ''Improved Retention of Key Contaminants of Concern in Low Temperature Immobilized Waste Forms''. Task 4 was a joint program between Khlopin Radium Institute and the Savannah River National Laboratory. The task evolved during this period into a study of cementitious waste forms with an expanded scope that included heat of hydration and fate and transport modeling. This report provides the results for Task 4 of the International Program as of the end of FY06 at which time funding for Task 4 was discontinued due to the needs of higher priority tasks within the International Program. Consequently, some of the subtasks were only partially completed, but it was considered important to capture the results up to this point in time. Therefore, this report serves as the closeout report for Task 4. The degree of immobilization of Tc-99 within the Saltstone waste form was measured through monolithic and crushed grout leaching tests. An effective diffusion coefficient of 4.8 x 10{sup -12} (Leach Index of 11.4) was measured using the ANSI/ANS-16.1 protocol which is comparable with values obtained for tank closure grouts using a dilute salt solution. The leaching results show that, in the presence of concentrated salt solutions such as those that will be processed at the Saltstone Production Facility, blast furnace slag can effectively reduce pertechnetate to the immobile +4 oxidation state. Leaching tests were also initiated to determine the degree of immobilization of selenium in the Saltstone waste form. Results were obtained for the upper bound of projected selenium concentration ({approx}5 x 10{sup -3} M) in the salt solution that will be treated at Saltstone. The ANSI/ANS 16.1 leaching tests provided a value for the

  18. Round-robin testing of a reference glass for low-activity waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Ebert, W. L.; Wolf, S. F.

    1999-12-06

    A round robin test program was conducted with a glass that was developed for use as a standard test material for acceptance testing of low-activity waste glasses made with Hanford tank wastes. The glass is referred to as the low-activity test reference material (LRM). The program was conducted to measure the interlaboratory reproducibility of composition analysis and durability test results. Participants were allowed to select the methods used to analyze the glass composition. The durability tests closely followed the Product Consistency Test (PCT) Method A, except that tests were conducted at both 40 and 90 C and that parallel tests with a reference glass were not required. Samples of LRM glass that had been crushed, sieved, and washed to remove fines were provided to participants for tests and analyses. The reproducibility of both the composition and PCT results compare favorably with the results of interlaboratory studies conducted with other glasses. From the perspective of reproducibility of analysis results, this glass is acceptable for use as a composition standard for nonradioactive components of low-activity waste forms present at >0.1 elemental mass % and as a test standard for PCTS at 40 and 90 C. For PCT with LRM glass, the expected test results at the 95% confidence level are as follows: (1) at 40 C: pH = 9.86 {+-} 0.96; [B] = 2.30 {+-} 1.25 mg/L; [Na] = 19.7 {+-} 7.3 mg/L; [Si] = 13.7 {+-} 4.2 mg/L; and (2) at 90 C: pH = 10.92 {+-} 0.43; [B] = 26.7 {+-} 7.2 mg/L; [Na] = 160 {+-} 13 mg/L; [Si] = 82.0 {+-} 12.7 mg/L. These ranges can be used to evaluate the accuracy of PCTS conducted at other laboratories.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1994-06-01

    The Integral Fast Reactor (IFR) under development by Argonne National Laboratory uses metallic fuels instead of ceramics. This allows electrorefining of spent fuels and presents opportunities for recycling minor actinide elements. Four minor actinides ({sup 237}Np, {sup 240}Pu, {sup 241}Am, and {sup 243}Am) determine the waste storage requirements of spent fuel from all types of fission reactors. These nuclides behave the same as uranium and other plutonium isotopes in electrorefining, so they can be recycled back to the reactor without elaborate chemical processing. An experiment has been designed to demonstrate the effectiveness of the high-energy neutron spectra of the IFR in consuming these four nuclides and plutonium. Eighteen sets of seven actinide and five light metal targets have been selected for ten day exposure in the Experimental Breeder Reactor-2 which serves as a prototype of the IFR. Post-irradiation analyses of the exposed targets by gamma, alpha, and mass spectroscopy are used to determine nuclear reaction-rates and neutron spectra. These experimental data increase the authors` confidence in their ability to predict reaction rates in candidate IFR designs using a variety of neutron transport and diffusion programs.

  20. Determination of Uncertainties for +III and +IV Actinide Solubilities in the WIPP Geochemistry Model for the 2009 Compliance Recertification Application

    Science.gov (United States)

    Ismail, A. E.; Xiong, Y.; Nowak, E. J.; Brush, L. H.

    2009-12-01

    The Waste Isolation Pilot Plant (WIPP) is a U.S. Department of Energy (DOE) repository in southeast New Mexico for defense-related transuranic (TRU) waste. Every five years, the DOE is required to submit an application to the Environmental Protection Agency (EPA) demonstrating the WIPP’s continuing compliance with the applicable EPA regulations governing the repository. Part of this recertification effort involves a performance assessment—a probabilistic evaluation of the repository performance with respect to regulatory limits on the amount of releases from the repository to the accessible environment. One of the models used as part of the performance assessment process is a geochemistry model, which predicts solubilities of the radionuclides in the brines that may enter the repository in the different scenarios considered by the performance assessment. The dissolved actinide source term comprises actinide solubilities, which are input parameters for modeling the transport of radionuclides as a result of brine flow through and from the repository. During a performance assessment, the solubilities are modeled as the product of a “base” solubility determined from calculations based on the chemical conditions expected in the repository, and an uncertainty factor that describes the potential deviations of the model from expected behavior. We will focus here on a discussion of the uncertainties. To compute a cumulative distribution function (CDF) for the uncertainties, we compare published, experimentally measured solubility data to predictions made using the established WIPP geochemistry model. The differences between the solubilities observed for a given experiment and the calculated solubilities from the model are used to form the overall CDF, which is then sampled as part of the performance assessment. We will discuss the methodology used to update the CDF’s for the +III actinides, obtained from data for Nd, Am, and Cm, and the +IV actinides, obtained

  1. Preliminary evaluation of alternative waste form solidification processes. Volume II. Evaluation of the processes

    Energy Technology Data Exchange (ETDEWEB)

    1980-08-01

    This Volume II presents engineering feasibility evaluations of the eleven processes for solidification of nuclear high-level liquid wastes (HHLW) described in Volume I of this report. Each evaluation was based in a systematic assessment of the process in respect to six principal evaluation criteria: complexity of process; state of development; safety; process requirements; development work required; and facility requirements. The principal criteria were further subdivided into a total of 22 subcriteria, each of which was assigned a weight. Each process was then assigned a figure of merit, on a scale of 1 to 10, for each of the subcriteria. A total rating was obtained for each process by summing the products of the subcriteria ratings and the subcriteria weights. The evaluations were based on the process descriptions presented in Volume I of this report, supplemented by information obtained from the literature, including publications by the originators of the various processes. Waste form properties were, in general, not evaluated. This document describes the approach which was taken, the developent and application of the rating criteria and subcriteria, and the evaluation results. A series of appendices set forth summary descriptions of the processes and the ratings, together with the complete numerical ratings assigned; two appendices present further technical details on the rating process.

  2. FORM AND AGING OF PLUTONIUM IN SAVANNAH RIVER SITE WASTE TANK 18

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D.

    2012-02-24

    This report provides a summary of the effects of aging on and the expected forms of plutonium in Tank 18 waste residues. The findings are based on available information on the operational history of Tank 18, reported analytical results for samples taken from Tank 18, and the available scientific literature for plutonium under alkaline conditions. These findings should apply in general to residues in other waste tanks. However, the operational history of other waste tanks should be evaluated for specific conditions and unique operations (e.g., acid cleaning with oxalic acid) that could alter the form of plutonium in heel residues. Based on the operational history of other tanks, characterization of samples from the heel residues in those tanks would be appropriate to confirm the form of plutonium. During the operational period and continuing with the residual heel removal periods, Pu(IV) is the dominant oxidation state of the plutonium. Small fractions of Pu(V) and Pu(VI) could be present as the result of the presence of water and the result of reactions with oxygen in air and products from the radiolysis of water. However, the presence of Pu(V) would be transitory as it is not stable at the dilute alkaline conditions that currently exists in Tank 18. Most of the plutonium that enters Savannah River Site (SRS) high-level waste (HLW) tanks is freshly precipitated as amorphous plutonium hydroxide, Pu(OH){sub 4(am)} or hydrous plutonium oxide, PuO{sub 2(am,hyd)} and coprecipitated within a mixture of hydrous metal oxide phases containing metals such as iron, aluminum, manganese and uranium. The coprecipitated plutonium would include Pu{sup 4+} that has been substituted for other metal ions in crystal lattice sites, Pu{sup 4+} occluded within hydrous metal oxide particles and Pu{sup 4+} adsorbed onto the surface of hydrous metal oxide particles. The adsorbed plutonium could include both inner sphere coordination and outer sphere coordination of the plutonium. PuO{sub 2

  3. FORM AND AGING OF PLUTONIUM IN SAVANNAH RIVER SITE WASTE TANK 18

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D.

    2012-02-24

    This report provides a summary of the effects of aging on and the expected forms of plutonium in Tank 18 waste residues. The findings are based on available information on the operational history of Tank 18, reported analytical results for samples taken from Tank 18, and the available scientific literature for plutonium under alkaline conditions. These findings should apply in general to residues in other waste tanks. However, the operational history of other waste tanks should be evaluated for specific conditions and unique operations (e.g., acid cleaning with oxalic acid) that could alter the form of plutonium in heel residues. Based on the operational history of other tanks, characterization of samples from the heel residues in those tanks would be appropriate to confirm the form of plutonium. During the operational period and continuing with the residual heel removal periods, Pu(IV) is the dominant oxidation state of the plutonium. Small fractions of Pu(V) and Pu(VI) could be present as the result of the presence of water and the result of reactions with oxygen in air and products from the radiolysis of water. However, the presence of Pu(V) would be transitory as it is not stable at the dilute alkaline conditions that currently exists in Tank 18. Most of the plutonium that enters Savannah River Site (SRS) high-level waste (HLW) tanks is freshly precipitated as amorphous plutonium hydroxide, Pu(OH){sub 4(am)} or hydrous plutonium oxide, PuO{sub 2(am,hyd)} and coprecipitated within a mixture of hydrous metal oxide phases containing metals such as iron, aluminum, manganese and uranium. The coprecipitated plutonium would include Pu{sup 4+} that has been substituted for other metal ions in crystal lattice sites, Pu{sup 4+} occluded within hydrous metal oxide particles and Pu{sup 4+} adsorbed onto the surface of hydrous metal oxide particles. The adsorbed plutonium could include both inner sphere coordination and outer sphere coordination of the plutonium. PuO{sub 2

  4. Initial Evaluation of Processing Methods for an Epsilon Metal Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    Crum, Jarrod V.; Strachan, Denis M.; Zumhoff, Mac R.

    2012-06-11

    During irradiation of nuclear fuel in a reactor, the five metals, Mo, Pd, Rh, Ru, and Tc, migrate to the fuel grain boundaries and form small metal particles of an alloy known as epsilon metal ({var_epsilon}-metal). When the fuel is dissolved in a reprocessing plant, these metal particles remain behind with a residue - the undissolved solids (UDS). Some of these same metals that comprise this alloy that have not formed the alloy are dissolved into the aqueous stream. These metals limit the waste loading for a borosilicate glass that is being developed for the reprocessing wastes. Epsilon metal is being developed as a waste form for the noble metals from a number of waste streams in the aqueous reprocessing of used nuclear fuel (UNF) - (1) the {var_epsilon}-metal from the UDS, (2) soluble Tc (ion-exchanged), and (3) soluble noble metals (TRUEX raffinate). Separate immobilization of these metals has benefits other than allowing an increase in the glass waste loading. These materials are quite resistant to dissolution (corrosion) as evidenced by the fact that they survive the chemically aggressive conditions in the fuel dissolver. Remnants of {var_epsilon}-metal particles have survived in the geologically natural reactors found in Gabon, Africa, indicating that they have sufficient durability to survive for {approx} 2.5 billion years in a reducing geologic environment. Additionally, the {var_epsilon}-metal can be made without additives and incorporate sufficient foreign material (oxides) that are also present in the UDS. Although {var_epsilon}-metal is found in fuel and Gabon as small particles ({approx}10 {micro}m in diameter) and has survived intact, an ideal waste form is one in which the surface area is minimized. Therefore, the main effort in developing {var_epsilon}-metal as a waste form is to develop a process to consolidate the particles into a monolith. Individually, these metals have high melting points (2617 C for Mo to 1552 C for Pd) and the alloy is

  5. Implications of transmutation on the defect chemistry in crystalline waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Uberuaga, B.P., E-mail: blas@lanl.go [Materials Science and Technology Division, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Jiang, C.; Stanek, C.R.; Sickafus, K.E. [Materials Science and Technology Division, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Marks, N.A. [Nanochemistry Research Institute, Curtin University of Technology, P.O. Box U1987, Perth, WA 6845 (Australia); Carter, D.J.; Rohl, A.L. [Nanochemistry Research Institute, Curtin University of Technology, P.O. Box U1987, Perth, WA 6845 (Australia); iVEC, Technology Park, Kensington, WA 6151 (Australia)

    2010-10-01

    Radioactive decay within the solid state creates chemical environments which are typically incommensurate with the initial host structure. Using a combined theoretical and computational approach, we discuss this 'transmutation problem' in the context of the short-lived fission products Cs-137 and Sr-90. We show how a Kroeger-Vink treatment is insufficient for understanding defects arising from transmutation, and present density functional theory data for chemical evolution within two prototypical hosts, CsCl and SrTiO{sub 3}. While the latter has a strong driving force for phase separation with increasing Zr content, the Cs(Ba)Cl system is surprisingly stable. The sharp difference between these two findings points to the need for better understanding of novel chemistry in nuclear waste forms.

  6. Effect Of Oxidation On Chromium Leaching And Redox Capacity Of Slag-Containing Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Almond, P. M. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Stefanko, D. B. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Langton, C. A. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2013-03-01

    The rate of oxidation is important to the long-term performance of reducing salt waste forms because the solubility of some contaminants, e.g., technetium, is a function of oxidation state. TcO4- in the salt solution is reduced to Tc(IV) and has been shown to react with ingredients in the waste form to precipitate low solubility sulfide and/or oxide phases [Shuh, et al., 1994, Shuh, et al., 2000, Shuh, et al., 2003]. Upon exposure to oxygen, the compounds containing Tc(IV) oxidize to the pertechnetate ion, Tc(VII)O4-, which is very soluble. Consequently the rate of technetium oxidation front advancement into a monolith and the technetium leaching profile as a function of depth from an exposed surface are important to waste form performance and ground water concentration predictions. An approach for measuring contaminant oxidation rate (effective contaminant specific oxidation rate) based on leaching of select contaminants of concern is described in this report. In addition, the relationship between reduction capacity and contaminant oxidation is addressed. Chromate was used as a non-radioactive surrogate for pertechnetate in simulated waste form samples. Depth discrete subsamples were cut from material exposed to Savannah River Site (SRS) field cured conditions. The subsamples were prepared and analyzed for both reduction capacity and chromium leachability. Results from field-cured samples indicate that the depth at which leachable chromium was detected advanced further into the sample exposed for 302 days compared to the sample exposed to air for 118 days (at least 50 mm compared to at least 20 mm). Data for only two exposure time intervals is currently available. Data for additional exposure times are required to develop an equation for the oxidation front progression. Reduction capacity measurements (per the Angus-Glasser method, which is a measurement of the ability of a material to chemically reduce Ce(IV) to Ce

  7. AN INITIAL ASSESSMENT OF POTENTIAL PRODUCTION TECHNOLOGIES FOR EPSILON-METAL WASTE FORMS

    Energy Technology Data Exchange (ETDEWEB)

    Rohatgi, Aashish; Strachan, Denis M.

    2011-03-01

    This report examines and ranks a total of seven materials processing techniques that may be potentially utilized to consolidate the undissolved solids from nuclear fuel reprocessing into a low-surface area form. Commercial vendors of processing equipment were contacted and literature researched to gather information for this report. Typical equipment and their operation, corresponding to each of the seven techniques, are described in the report based upon the discussions and information provided by the vendors. Although the report does not purport to describe all the capabilities and issues of various consolidation techniques, it is anticipated that this report will serve as a guide by highlighting the key advantages and disadvantages of these techniques. The processing techniques described in this report were broadly classified into those that employed melting and solidification, and those in which the consolidation takes place in the solid-state. Four additional techniques were examined that were deemed impractical, but were included for completeness. The techniques were ranked based on criteria such as flexibility in accepting wide-variety of feed-stock (chemistry, form, and quantity), ease of long-term maintenance, hot cell space requirements, generation of additional waste streams, cost, and any special considerations. Based on the assumption of ~2.5 L of waste to be consolidated per day, sintering based techniques, namely, microwave sintering, spark plasma sintering and hot isostatic pressing, were ranked as the top-3 choices, respectively. Melting and solidification based techniques were ranked lower on account of generation of volatile phases and difficulties associated with reactivity and containment of the molten metal.

  8. Oxyhydroxy Silicate Colloids: A New Type of Waterborne Actinide(IV) Colloids

    OpenAIRE

    Zänker, Harald; Weiss, Stephan; Hennig, Christoph; Brendler, Vinzenz; Ikeda‐Ohno, Atsushi

    2016-01-01

    Abstract At the near‐neutral and reducing aquatic conditions expected in undisturbed ore deposits or in closed nuclear waste repositories, the actinides Th, U, Np, and Pu are primarily tetravalent. These tetravalent actinides (AnIV) are sparingly soluble in aquatic systems and, hence, are often assumed to be immobile. However, AnIV could become mobile if they occur as colloids. This review focuses on a new type of AnIV colloids, oxyhydroxy silicate colloids. We herein discuss the chemical cha...

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

    Science.gov (United States)

    Kaminski, Michael D.; Mertz, Carol J.

    2016-06-07

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

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

    Science.gov (United States)

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

    2012-08-01

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

  11. Minor Actinides Loading Optimization for Proliferation Resistant Fuel Design - BWR

    Energy Technology Data Exchange (ETDEWEB)

    G. S. Chang; Hongbin Zhang

    2009-09-01

    One approach to address the United States Nuclear Power (NP) 2010 program for the advanced light water reactor (LWR) (Gen-III+) intermediate-term spent fuel disposal need is to reduce spent fuel storage volume while enhancing proliferation resistance. One proposed solution includes increasing burnup of the discharged spent fuel and mixing minor actinide (MA) transuranic nuclides (237Np and 241Am) in the high burnup fuel. Thus, we can reduce the spent fuel volume while increasing the proliferation resistance by increasing the isotopic ratio of 238Pu/Pu. For future advanced nuclear systems, MAs are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. A typical boiling water reactor (BWR) fuel unit lattice cell model with UO2 fuel pins will be used to investigate the effectiveness of adding MAs (237Np and/or 241Am) to enhance proliferation resistance and improve fuel cycle performance for the intermediate-term goal of future nuclear energy systems. However, adding MAs will increase plutonium production in the discharged spent fuel. In this work, the Monte-Carlo coupling with ORIGEN-2.2 (MCWO) method was used to optimize the MA loading in the UO2 fuel such that the discharged spent fuel demonstrates enhanced proliferation resistance, while minimizing plutonium production. The axial averaged MA transmutation characteristics at different burnup were compared and their impact on neutronics criticality and the ratio of 238Pu/Pu discussed.

  12. Optimized data flow for the waste form documentation of compactable radioactive wastes; Optimierter Datenfluss zur Erstellung von Abfallgebindedokumentationen fuer pressbare radioaktive Abfaelle

    Energy Technology Data Exchange (ETDEWEB)

    Lange, M. [GNS Gesellschaft fuer Nuklear-Service mbH, Essen (Germany); Risch, R. [WTI Wissenschaftlich-Technische Ingenieurleistung GmbH, Juelich (Germany)

    2010-05-15

    According to the national radiation protection regulations (Strahlenschutzverordnung)it is necessary to perform a detailed documentation on radioactive materials, including the waste flow, transport and storage. The book-keeping system AVK is an authorized data base system. The authors describe the data relevant sheets, the activity calculation procedure based on local dose rate measurements and gamma spectroscopy and the necessary documents for the licensing procedure. For a structured and efficient waste form documentation a data base (PIKA-AS: project information and control system) was developed by GNS that includes all documentation relevant data from different measuring and calculation activities.

  13. Prompt fission neutron spectrum of actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-01-06

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

  14. Interaction of actinides with amino acids: from peptides to proteins; Interaction des actinides avec les acides amines: du peptide a la proteine

    Energy Technology Data Exchange (ETDEWEB)

    Jeanson, A

    2008-09-15

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

  15. Supplemental Immobilization Cast Stone Technology Development and Waste Form Qualification Testing Plan

    Energy Technology Data Exchange (ETDEWEB)

    Westsik, Joseph H.; Serne, R. Jeffrey; Pierce, Eric M.; Cozzi, Alex; Chung, Chul-Woo; Swanberg, David J.

    2013-05-31

    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). The pretreatment facility will have the capacity to separate all of the tank wastes into the HLW and LAW fractions, and the HLW Vitrification Facility will have the capacity to vitrify all of the HLW. However, a second immobilization facility will be needed for the expected volume of LAW requiring immobilization. A number of alternatives, including Cast Stone—a cementitious waste form—are being considered to provide the additional LAW immobilization capacity.

  16. Actinide ion sensor for pyroprocess monitoring

    Science.gov (United States)

    Jue, Jan-fong; Li, Shelly X.

    2014-06-03

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

  17. Catalytic Organic Transformations Mediated by Actinide Complexes

    Directory of Open Access Journals (Sweden)

    Isabell S. R. Karmel

    2015-10-01

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

  18. Radioactive Demonstration Of Mineralized Waste Forms Made From Hanford Low Activity Waste (Tank Farm Blend) By Fluidized Bed Steam Reformation (FBSR)

    Energy Technology Data Exchange (ETDEWEB)

    Jantzen, C. M. [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); 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); Daniel, W. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Hall, H. K. [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)

    2013-08-01

    The U.S. Department of Energy’s Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford’s tank waste. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Hanford Tank Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Supplemental Treatment is likely to be required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. The Supplemental Treatment chosen will immobilize that portion of the retrieved LAW that is not sent to the WTP’s LAW Vitrification facility into a solidified waste form. The solidified waste will then be disposed on the Hanford site in the Integrated Disposal Facility (IDF). Fluidized Bed Steam Reforming (FBSR) offers a moderate temperature (700-750°C) continuous method by which LAW can be processed irrespective of whether the waste contain organics, nitrates, sulfates/sulfides, chlorides, fluorides, volatile radionuclides or other aqueous components. The FBSR technology can process these wastes into a crystalline 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 comparable to LAW glass, i.e. leaches Tc-99, Re and Na at <2g/m2 during ASTM C1285 (Product Consistency) durability testing. Monolithing of the granular FBSR product was investigated to prevent dispersion during transport or burial/storage. Monolithing in an inorganic geopolymer binder, which is

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

    Directory of Open Access Journals (Sweden)

    Kooyman Timothée

    2015-01-01

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

  20. INTERNATIONAL PROGRAM: SUMMARY REPORT ON THE PROPERTIES OF CEMENTITIOUS WASTE FORMS

    Energy Technology Data Exchange (ETDEWEB)

    Harbour, J

    2007-03-02

    This report provides a summary of the results on the properties of cementitious waste forms obtained as part of the International Program. In particular, this report focuses on the results of Task 4 of the Program that was initially entitled ''Improved Retention of Key Contaminants of Concern in Low Temperature Immobilized Waste Forms''. Task 4 was a joint program between Khlopin Radium Institute and the Savannah River National Laboratory. The task evolved during this period into a study of cementitious waste forms with an expanded scope that included heat of hydration and fate and transport modeling. This report provides the results for Task 4 of the International Program as of the end of FY06 at which time funding for Task 4 was discontinued due to the needs of higher priority tasks within the International Program. Consequently, some of the subtasks were only partially completed, but it was considered important to capture the results up to this point in time. Therefore, this report serves as the closeout report for Task 4. The degree of immobilization of Tc-99 within the Saltstone waste form was measured through monolithic and crushed grout leaching tests. An effective diffusion coefficient of 4.8 x 10{sup -12} (Leach Index of 11.4) was measured using the ANSI/ANS-16.1 protocol which is comparable with values obtained for tank closure grouts using a dilute salt solution. The leaching results show that, in the presence of concentrated salt solutions such as those that will be processed at the Saltstone Production Facility, blast furnace slag can effectively reduce pertechnetate to the immobile +4 oxidation state. Leaching tests were also initiated to determine the degree of immobilization of selenium in the Saltstone waste form. Results were obtained for the upper bound of projected selenium concentration ({approx}5 x 10{sup -3} M) in the salt solution that will be treated at Saltstone. The ANSI/ANS 16.1 leaching tests provided a value for the

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

    Directory of Open Access Journals (Sweden)

    Taieb J.

    2010-03-01

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

  2. Evidence of Technetium and Iodine from a Sodalite-Bearing Ceramic Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    Neeway, James J.; Qafoku, Nikolla; Williams, Benjamin D.; Snyder, Michelle MV; Brown, Christopher F.; Pierce, Eric M.

    2016-03-01

    Current plans for nuclear waste vitrification at the Hanford Tank Waste Treatment and Immobilization Plant (WTP) lack the capacity to treat all of the low activity waste (LAW) that is not encapsulated in the vitrified product. Several technologies are being considered to treat the excess LAW. One such technology is Fluidized Bed Steam Reforming (FBSR). The FBSR process results in a granular product composed of feldspathoid mineral phases that immobilize the major components in the LAW as well as other contaminants of concern (COCs), with Tc and I expected to be present in sodalite cages formed during the process. In order to meet compressive strength requirements at the Hanford Integrated Disposal Facility (IDF), the granular product may be encapsulated in a monolith. To demonstrate the ability of the technology to serve the mission of managing excess LAW, Single Pass Flow-Through (SPFT) tests have been performed on non-radioactive granular materials and granular materials encapsulated in a geopolymer binder produced at the engineering- and bench-scale as well as a granular product produced at the bench scale with actual Hanford tank waste. SPFT tests were conducted at 40 °C for durations up to 2 months with a flow-through solution buffered at pH 9. The forward reaction rate of the non-radioactive mineral product dissolution based on Si release for the granular product was measured to be (6.2 ± 2.1) × 10-4 g/m2d for the engineering-scale product and (13 ± 4.9) × 10-4 g/m2d for the bench-scale product. The resulting non-radioactive monoliths showed forward reaction rates based on Si release of (3.4 ± 1.1) × 10-4 g/m2d for the engineering-scale material and (4.2 ± 1.5) × 10-4 g/m2d for the bench-scale material demonstrating that encapsulation of the FBSR granular product in a monolith does not significantly alter the performance of the material. Finally, an FBSR granular product created at the bench scale using actual Hanford LAW gave similar release values

  3. Development of a new generation of waste form for entrapment and immobilization of highly volatile and soluble radionuclides.

    Energy Technology Data Exchange (ETDEWEB)

    Rodriguez, Mark Andrew; Bencoe, Denise Nora; Brinker, C. Jeffrey; Murphy, Andrew Wilson; Holt, Kathleen Caroline; Turnham, Rigney; Kruichak, Jessica Nicole; Tellez, Hernesto; Miller, Andy; Xiong, Yongliang; Pohl, Phillip Isabio; Ockwig, Nathan W.; Wang, Yifeng; Gao, Huizhen

    2010-09-01

    The United States is now re-assessing its nuclear waste disposal policy and re-evaluating the option of moving away from the current once-through open fuel cycle to a closed fuel cycle. In a closed fuel cycle, used fuels will be reprocessed and useful components such as uranium or transuranics will be recovered for reuse. During this process, a variety of waste streams will be generated. Immobilizing these waste streams into appropriate waste forms for either interim storage or long-term disposal is technically challenging. Highly volatile or soluble radionuclides such as iodine ({sup 129}I) and technetium ({sup 99}Tc) are particularly problematic, because both have long half-lives and can exist as gaseous or anionic species that are highly soluble and poorly sorbed by natural materials. Under the support of Sandia National Laboratories (SNL) Laboratory-Directed Research & Development (LDRD), we have developed a suite of inorganic nanocomposite materials (SNL-NCP) that can effectively entrap various radionuclides, especially for {sup 129}I and {sup 99}Tc. In particular, these materials have high sorption capabilities for iodine gas. After the sorption of radionuclides, these materials can be directly converted into nanostructured waste forms. This new generation of waste forms incorporates radionuclides as nano-scale inclusions in a host matrix and thus effectively relaxes the constraint of crystal structure on waste loadings. Therefore, the new waste forms have an unprecedented flexibility to accommodate a wide range of radionuclides with high waste loadings and low leaching rates. Specifically, we have developed a general route for synthesizing nanoporous metal oxides from inexpensive inorganic precursors. More than 300 materials have been synthesized and characterized with x-ray diffraction (XRD), BET surface area measurements, and transmission electron microscope (TEM). The sorption capabilities of the synthesized materials have been quantified by using stable

  4. Ionic Interactions in Actinide Tetrahalides

    Science.gov (United States)

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

    2001-05-01

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

  5. Physical barrier effect of geopolymeric waste form on diffusivity of cesium and strontium.

    Science.gov (United States)

    Jang, J G; Park, S M; Lee, H K

    2016-11-15

    The present study investigates the physical barrier effect of geopolymeric waste form on leaching behavior of cesium and strontium. Fly ash-based geopolymers and slag-blended geopolymers were used as solidification agents. The leaching behavior of cesium and strontium from geopolymers was evaluated in accordance with ANSI/ANS-16.1. The diffusivity of cesium and strontium in a fly ash-based geopolymer was lower than that in Portland cement by a factor of 10(3) and 10(4), respectively, showing significantly improved immobilization performance. The leaching resistance of fly ash-based geopolymer was relatively constant regardless of the type of fly ash. The diffusivity of water-soluble cesium and strontium ions were highly correlated with the critical pore diameter of the binder. The critical pore diameter of the fly ash-based geopolymer was remarkably smaller than those of Portland cement and slag-blended geopolymer; consequently, its ability physically to retard the diffusion of nuclides (physical barrier effect) was superior.

  6. Identification of lead chemical form in mine waste materials by X-ray absorption spectroscopy

    Science.gov (United States)

    Taga, Raijeli L.; Zheng, Jiajia; Huynh, Trang; Ng, Jack; Harris, Hugh H.; Noller, Barry

    2010-06-01

    X-ray absorption spectroscopy (XAS) provides a direct means for measuring lead chemical forms in complex samples. In this study, XAS was used to identify the presence of plumbojarosite (PbFe6(SO4)4(OH)12) by lead L3-edge XANES spectra in mine waste from a small gold mining operation in Fiji. The presence of plumbojarosite in tailings was confirmed by XRD but XANES gave better resolution. The potential for human uptake of Pb from tailings was measured using a physiologically based extract test (PBET), an in-vitro bioaccessibility (BAc) method. The BAc of Pb was 55%. Particle size distribution of tailings indicated that 40% of PM10 particulates exist which could be a potential risk for respiratory effects via the inhalation route. Food items collected in the proximity of the mine site had lead concentrations which exceed food standard guidelines. Lead within the mining lease exceeded sediment guidelines. The results from this study are used to investigate exposure pathways via ingestion and inhalation for potential risk exposure pathways of Pb in that locality. The highest Pb concentration in soil and tailings was 25,839 mg/kg, exceeding the Australian National Environment Protection Measure (NEPM) soil health investigation levels.

  7. Sets of Reports and Articles Regarding Cement Wastes Forms Containing Alpha Emitters that are Potentially Useful for Development of Russian Federation Waste Treatment Processes for Solidification of Weapons Plutonium MOX Fuel Fabrication Wastes for

    Energy Technology Data Exchange (ETDEWEB)

    Jardine, L J

    2003-06-12

    This is a set of nine reports and articles that were kindly provided by Dr. Christine A. Langton from the Savannah River Site (SRS) to L. J. Jardine LLNL in June 2003. The reports discuss cement waste forms and primarily focus on gas generation in cement waste forms from alpha particle decays. However other items such as various cement compositions, cement product performance test results and some cement process parameters are also included. This set of documents was put into this Lawrence Livermore National Laboratory (LLNL) releasable report for the sole purpose to provide a set of documents to Russian technical experts now beginning to study cement waste treatment processes for wastes from an excess weapons plutonium MOX fuel fabrication facility. The intent is to provide these reports for use at a US RF Experts Technical Meeting on: the Management of Wastes from MOX Fuel Fabrication Facilities, in Moscow July 9-11, 2003. The Russian experts should find these reports to be very useful for their technical and economic feasibility studies and the supporting R&D activities required to develop acceptable waste treatment processes for use in Russia as part of the ongoing Joint US RF Plutonium Disposition Activities.

  8. Dissolution models for glassy waste forms; Modeles de dissolution des formes de dechets a base de verre

    Energy Technology Data Exchange (ETDEWEB)

    Harvey, K.B.

    1995-06-01

    As a part of the Canadian Nuclear Fuel Waste Management Program (CNFWMP), a suite of models has been developed that describe the dissolution of a glass under a variety of conditions. This work had two aims: to develop and present the models in such a way that the equations associated with models could be used to unambiguously extract the fundamental dissolution constants of a glass from experimental data, and to demonstrate the correspondence between models and experiments over a sufficiently broad range of conditions such that the models could be used with confidence to forecast performance under conditions that might not be realistically accessible to experiments.

  9. Experimental studies of actinides in molten salts

    Energy Technology Data Exchange (ETDEWEB)

    Reavis, J.G.

    1985-06-01

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

  10. Spin and orbital moments in actinide compounds

    DEFF Research Database (Denmark)

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

    1991-01-01

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

  11. Possibility of fusion power reactor to transmute minor actinides of spent nuclear fuel

    Energy Technology Data Exchange (ETDEWEB)

    Serikov, A. E-mail: serikov@nfi.kiae.ru; Shatalov, G.; Sheludjakov, S.; Shpansky, Yu.; Vasiliev, N

    2002-12-01

    A possibility to use fusion power reactor (FPR) is considered for burning long-life elements of spent nuclear fuel in parallel with energy production. In this study a principal design of FPR blanket was examined for transmutation of long-life minor actinides (Np, Am, Cm). A production of minor actinide isotopes is equal to 20-30 kg/1 GW{sub (e)} year for now operating fission reactors, and their amounts will rise with the expected growth of fission reactor power. These isotopes have long-life time and can be dangerous in big amounts in future. Plutonium isotopes are not included in an assumption that they will be used in fission reactors. The major goals of the study were to determine FPR blanket composition corresponding to fast transmutation rate of actinides and tritium self-supply simultaneously. Tritium breeding ratio (TBR) was obtained at level 1.11 for water cooling and reached up 1.56 in variant with helium-cooled assemblies with Np nitride. It was concluded that rows with actinides from processed waste fuel should be arranged near the plasma first wall. Advantages of helium above water cooling are observed in the twice-increased loading of waste fissionable materials and essential increase of achievable TBR. Burnout of Np, Am, Cm would remain at a level {approx}40-50% after 4 full power years.

  12. Fiscal Year 2010 Summary Report on the Epsilon-Metal Phase as a Waste Form for 99 Tc

    Energy Technology Data Exchange (ETDEWEB)

    Strachan, Denis M.; Crum, Jarrod V.; Buck, Edgar C.; Riley, Brian J.; Zumhoff, Mac R.

    2010-09-30

    Epsilon metal (ε-metal) is generated in nuclear fuel during irradiation. This metal consists of Pd, Ru, Rh, Mo, and some Te. These accumulate at the UO2 grain boundaries as small (ca 5 µm) particles. These metals have limited solubility in the acid used to dissolve fuel during reprocessing and in typical borosilicate glass. These must be treated separately to improve overall waste loading in glass. This low solubility and their survival in 2 Gy-old natural reactors led us to investigate them as a waste form for the immobilization of 99Tc and 107Pd, two very long-lived isotopes.

  13. Radioactive Demonstration Of Mineralized Waste Forms Made From Hanford Low Activity Waste (Tank Farm Blend) By Fluidized Bed Steam Reformation (FBSR)

    Energy Technology Data Exchange (ETDEWEB)

    Jantzen, C. M. [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); 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); Daniel, W. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Hall, H. K. [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)

    2013-08-01

    The U.S. Department of Energy’s Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford’s tank waste. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Hanford Tank Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Supplemental Treatment is likely to be required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. The Supplemental Treatment chosen will immobilize that portion of the retrieved LAW that is not sent to the WTP’s LAW Vitrification facility into a solidified waste form. The solidified waste will then be disposed on the Hanford site in the Integrated Disposal Facility (IDF). Fluidized Bed Steam Reforming (FBSR) offers a moderate temperature (700-750°C) continuous method by which LAW can be processed irrespective of whether the waste contain organics, nitrates, sulfates/sulfides, chlorides, fluorides, volatile radionuclides or other aqueous components. The FBSR technology can process these wastes into a crystalline 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 comparable to LAW glass, i.e. leaches Tc-99, Re and Na at <2g/m2 during ASTM C1285 (Product Consistency) durability testing. Monolithing of the granular FBSR product was investigated to prevent dispersion during transport or burial/storage. Monolithing in an inorganic geopolymer binder, which is

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1999-02-12

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

  15. Removal of cesium using coconut fiber in raw and modified forms for the treatment of radioactive liquid wastes

    Energy Technology Data Exchange (ETDEWEB)

    Jesus, Nella N.M. de; Nobre, Vanessa B.; Potiens Junior, Ademar J.; Sakata, Solange K., E-mail: sksakata@ipen.br [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil); Di Vitta, Patricia B. [Universidade de Sao Paulo (USP), SP (Brazil). Instituto de Quimica

    2013-07-01

    Sorption is one of the most studied methods to reduce the volume of radioactive waste streams. Cesium-137 is a radioisotope formed by the fission of uranium and it can cause health problems due to its easy assimilation by cells. The aim of this study is to evaluate the potential of coconut fiber in removing cesium from radioactive liquid wastes; this process can help in disposing radioactive waste. The experiments were performed in batch and the particle size of the fiber ranged between 0.30 mm and 0.50 mm. The fiber was treated with hydrogen peroxide in alkaline medium. The following parameters were analyzed: contact time, pH and concentration of cesium ions in aqueous solution. After the experiments the samples were filtered and cesium remaining in solution was quantified by inductively coupled plasma optical emission spectrometry. (author)

  16. BWR Assembly Optimization for Minor Actinide Recycling

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-03-22

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

  17. Advanced Aqueous Separation Systems for Actinide Partitioning

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-03-21

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

  18. Preliminary parametric performance assessment of potential final waste forms for alpha low-level waste at the Idaho National Engineering Laboratory. Revision 1

    Energy Technology Data Exchange (ETDEWEB)

    Smith, T.H.; Sussman, M.E. [Lockheed Idaho Technologies Co., Idaho Falls, ID (United States); Myers, J.; Djordjevic, S.M.; DeBiase, T.A.; Goodrich, M.T.; DeWitt, D. [IT Corp., Albuquerque, NM (United States)

    1995-08-01

    This report presents a preliminary parametric performance assessment (PA) of potential waste disposal systems for alpha-contaminated, mixed, low-level waste (ALLW) currently stored at the Transuranic Storage Area of INEL. The ALLW, which contains from 10 to 100 nCi/g of transuranic (TRU) radionuclides, is awaiting treatment and disposal. The purpose of this study was to examine the effects of several parameters on the radiological-confinement performance of potential disposal systems for the ALLW. The principal emphasis was on the performance of final waste forms (FWFs). Three categories of FWF (cement, glass, and ceramic) were addressed by evaluating the performance of two limiting FWFs for each category. Performance at five conceptual disposal sites was evaluated to illustrate the effects of site characteristics on the performance of the total disposal system. Other parameters investigated for effects on receptor dose included inventory assumptions, TRU radionuclide concentration, FWF fracture, disposal depth, water infiltration rates, subsurface-transport modeling assumptions, receptor well location, intrusion scenario assumptions, and the absence of waste immobilization. These and other factors were varied singly and in some combinations. The results indicate that compliance of the treated and disposed ALLW with the performance objectives depends on the assumptions made, as well as on the FWF and the disposal site. Some combinations result in compliance, while others do not. The implications of these results for decision making relative to treatment and disposal of the INEL ALLW are discussed. The report compares the degree of conservatism in this preliminary parametric PA against that in four other PAs and one risk assessment. All of the assessments addressed the same disposal site, but different wastes. The report also presents a qualitative evaluation of the uncertainties in the PA and makes recommendations for further study.

  19. Remaining Sites Verification Package for the 120-F-1 Glass Dump Waste Site, Waste Site Reclassification Form 2008-028

    Energy Technology Data Exchange (ETDEWEB)

    J. M. Capron

    2008-06-27

    The 120-F-1 waste site consisted of two dumping areas located 660 m southeast of the 105-F Reactor containing laboratory equipment and bottles, demolition debris, light bulbs and tubes, small batteries, small drums, and pesticide contaminated soil. It is probable that 108-F was the source of the debris but the material may have come from other locations within the 100-F Area. In accordance with this evaluation, the verification sampling results support a reclassification of this site to Interim Closed Out. The results of verification sampling show that residual contaminant concentrations do not preclude any future uses and allow for unrestricted use of shallow zone soils. The results also demonstrate that residual contaminant concentrations are protective of groundwater and the Columbia River.

  20. Materials for Tc Capture to Increase Tc Retention in Glass Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    Luksic, Steven A.; Hrma, Pavel R.; Kruger, Albert A.

    2016-04-01

    99Technetium is a long-lived fission product found in the tank waste at the Hanford site in Washington State. In its heptavalent species, it is volatile at the temperatures used in Hanford Tank Waste Treatment and Immobilization Plant vitrification melters, and thus is challenging to incorporate into waste glass. In order to decrease volatility and thereby increase retention, technetium can be converted into more thermally stable species. Several mineral phases, such as spinel, are able to incorporate tetravalent technetium in a chemically durable and thermally stable lattice, and these hosts may promote the decreased volatility that is desired. In order to be usefully implemented, there must be a synthetic rout to these phases that is compatible with both technetium chemistry and current Hanford Tank Waste Treatment and Immobilization Plant design. Synthetic routes for spinel and other potential host phases are examined.

  1. The Actinide Transition Revisited by Gutzwiller Approximation

    Science.gov (United States)

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

    2015-03-01

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

  2. Predictive Modeling in Actinide Chemistry and Catalysis

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-05-16

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

  3. Lattice effects in the light actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    1998-12-31

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

  4. Transmutation of actinides in power reactors.

    Science.gov (United States)

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

    2005-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

    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

    Current plans for nuclear waste vitrification at the Hanford Tank Waste Treatment and Immobilization Plant (WTP) lack the capacity to treat all of the low activity waste (LAW) that is not encapsulated in the vitrified product. Fluidized Bed Steam Reforming (FBSR) is one of the supplemental technologies under consideration to fill this gap. The FBSR process results in a granular product mainly composed of feldspathoid mineral phases that encapsulate the LAW and other contaminants of concern (COCs). In order to better understand the characteristics of the FBSR product, characterization testing has been performed on the granular product as well as the granular product encapsulated in a monolithic geopolymer binder. The non-radioactive simulated tank waste samples created for use in this study are the result of a 2008 Department of Energy sponsored Engineering Scale Technology Demonstration (ESTD) in 2008. These samples were created from waste simulant that was chemically shimmed to resemble actual tank waste, and rhenium has been used as a substitute for technetium. Another set of samples was created by the Savannah River Site Bench-Scale Reformer (BSR) using a chemical shim of Savannah River Site Tank 50 waste in order to simulate a blend of 68 Hanford tank wastes. This paper presents results from coal and moisture removal tests along with XRD, SEM, and BET analyses showing that the major mineral components are predominantly sodium aluminosilicate minerals and that the mineral product is highly porous. Results also show that the materials pass the short-term leach tests: the Toxicity Characteristic Leaching Procedure (TCLP) and Product Consistency Test (PCT).

  6. High-temperature vacuum distillation separation of plutonium waste salts

    Energy Technology Data Exchange (ETDEWEB)

    Garcia, E. [Los Alamos National Lab., NM (United States)

    1996-10-01

    In this task, high-temperature vacuum distillation separation is being developed for residue sodium chloride-potassium chloride salts resulting from past pyrochemical processing of plutonium. This process has the potential of providing clean separation of the salt and the actinides with minimal amounts of secondary waste generation. The process could produce chloride salt that could be discarded as low-level waste (LLW) or low actinide content transuranic (TRU) waste, and a concentrated actinide oxide powder that would meet long-term storage standards (DOE-DTD-3013-94) until a final disposition option for all surplus plutonium is chosen.

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

    Energy Technology Data Exchange (ETDEWEB)

    Bliss, Mary; Stave, Jean A.

    2012-10-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Wilkerson, Marianne Perry [Los Alamos National Laboratory

    2010-01-01

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

  9. Revisiting the melting temperature of NpO2 and the challenges associated with high temperature actinide compound measurements

    NARCIS (Netherlands)

    Böhler, R.; Welland, M.J.; De Bruycker, F.; Boboridis, K.; Janssen, A.; Eloirdi, R.; Konings, R.J.M.; Manara, D.

    2012-01-01

    This work revisits the melting behaviour of neptunium dioxide, an actinide compound which can be produced in the nuclear fuel during operation, and which has an important impact on the nuclear fuel and waste radioactivity especially on the very long term. The present experimental approach employs re

  10. AgI-MOR Loading Effect on the Durability of the Sandia Low Temperature Sintering GCM Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    Nenoff, Tina Maria [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Brady, Patrick Vane. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Mowry, Curtis D. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Garino, Terry J. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

    2014-09-01

    Herein, we study the durability of the Sandia Bi-Si oxide Glass Composite Material (GCM) waste form when formulated with different weight percent levels of AgI-MOR. The post-iodine exposure AgI-MOR material was provided to SNL by ORNL. Durability results for the GCM fabricated with 22 and 25% AgI-MOR indicate releases of Ag and I at the same low rates as 15% AgI-MOR GCM, and by the same mechanism. Iodine and Ag release is controlled by the low solubility of an amorphous, hydrated silver iodide, not by the surface-controlled dissolution of I2- loaded Ag-Mordenite. Based on this data, we postulate that much higher loading levels of AgIMOR are probable in this GCM waste form, and limits will govern by retention of mechanical integrity of the GCM versus the solubility of silver iodide.

  11. Charge-coupled Substituted Garnets (Y3-xCa0.5xM0.5x)Fe5O12 (M = Ce, Th): Structure and Stability as Crystalline Nuclear Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Guo, Xiaofeng; Kukkadapu, Ravi K.; Lanzirotti, Anthony; Newville, Mathew; Engelhard, Mark H.; Sutton , Steven R.; Navrotsky, Alexandra

    2015-04-20

    The garnet structure has been proposed as a potential crystalline nuclear waste form for accommodation of actinide elements, especially uranium (U). In this study, yttrium iron garnet (YIG) as a model garnet host was studied for the incorporation of U analogs, cerium (Ce), and thorium (Th), incorporated by a charge-coupled substitution with calci-um (Ca) for yttrium (Y) in YIG, namely 2Y3+ = Ca2+ + M4+, where M4+ = Ce4+ or Th4+. Single phase garnets Y3-xCa0.5xM0.5xFe5O12, synthesized by the citrate-nitrate combustion method, were obtained up to x = 0.7. Ce was confirmed to be tetravalent by X-ray absorption spectroscopy and X-ray photoelectron spectroscopy. X-ray diffraction and 57Fe-Mössbauer spectroscopy indicated that the samples are single phase, M4+ and Ca2+ cations are restricted to the c-site, the nature of M4+ has only a minor effect on the structure, and the local environments of both the tetrahedral and octahedral Fe3+ are systematically affected by the extent of substitution, especially on the tetrahedral sublattice. The charge coupled substitution has advantages in incorporating Ce/Th and in stabilizing the substituted phases, compared to a single substitution strategy. Enthalpies of formation of garnets were obtained by high temperature oxide melt solution calorimetry, and the enthalpies of substitution of Ce and Th were determined. The thermodynamic analysis demonstrates that the substituted garnets are entropically rather than energetically stabilized. This suggests that such garnets may form and persist in repositories at high temperature but might decompose near room temperature. These structural and thermodynamic findings shed light on possible incorporation of U in this garnet system.

  12. Charge-coupled substituted garnets (Y3-xCa0.5xM0.5x)Fe5O12 (M = Ce, Th): structure and stability as crystalline nuclear waste forms.

    Science.gov (United States)

    Guo, Xiaofeng; Kukkadapu, Ravi K; Lanzirotti, Antonio; Newville, Matthew; Engelhard, Mark H; Sutton, Stephen R; Navrotsky, Alexandra

    2015-04-20

    The garnet structure has been proposed as a potential crystalline nuclear waste form for accommodation of actinide elements, especially uranium (U). In this study, yttrium iron garnet (YIG) as a model garnet host was studied for the incorporation of U analogs, cerium (Ce) and thorium (Th), incorporated by a charge-coupled substitution with calcium (Ca) for yttrium (Y) in YIG, namely, 2Y(3+) = Ca(2+) + M(4+), where M(4+) = Ce(4+) or Th(4+). Single-phase garnets Y3-xCa0.5xM0.5xFe5O12 (x = 0.1-0.7) were synthesized by the citrate-nitrate combustion method. Ce was confirmed to be tetravalent by X-ray absorption spectroscopy and X-ray photoelectron spectroscopy. X-ray diffraction and (57)Fe-Mössbauer spectroscopy indicated that M(4+) and Ca(2+) cations are restricted to the c site, and the local environments of both the tetrahedral and the octahedral Fe(3+) are systematically affected by the extent of substitution. The charge-coupled substitution has advantages in incorporating Ce/Th and in stabilizing the substituted phases compared to a single substitution strategy. Enthalpies of formation of garnets were obtained by high temperature oxide melt solution calorimetry, and the enthalpies of substitution of Ce and Th were determined. The thermodynamic analysis demonstrates that the substituted garnets are entropically rather than energetically stabilized. This suggests that such garnets may form and persist in repositories at high temperature but might decompose near room temperature.

  13. Synthesis and Evaluation of new Polyfunctional Molecules for Group Actinide Extraction; Synthese et evaluation de Nouvelles Molecules Polyfonctionnelles pour la Separation Groupee des Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Marie, C.

    2009-10-15

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

  14. Actinide Solubility and Speciation in the WIPP [PowerPoint

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-11-02

    The presentation begins with the role and need for nuclear repositories (overall concept, international updates (Sweden, Finland, France, China), US approach and current status), then moves on to the WIPP TRU repository concept (design, current status--safety incidents of February 5 and 14, 2014, path forward), and finally considers the WIPP safety case: dissolved actinide concentrations (overall approach, oxidation state distribution and redox control, solubility of actinides, colloidal contribution and microbial effects). The following conclusions are set forth: (1) International programs are moving forward, but at a very slow and somewhat sporadic pace. (2) In the United States, the Salt repository concept, from the perspective of the long-term safety case, remains a viable option for nuclear waste management despite the current operational issues/concerns. (3) Current model/PA prediction (WIPP example) are built on redundant conservatisms. These conservatisms are being addressed in the ongoing and future research to fill existing data gaps--redox control of plutonium by Fe(0, II), thorium (analog) solubility studies in simulated brine, contribution of intrinsic and biocolloids to the mobile concentration, and clarification of microbial ecology and effects.

  15. Heat capacities of lanthanide and actinide monazite-type ceramics

    Science.gov (United States)

    Kowalski, Piotr M.; Beridze, George; Vinograd, Victor L.; Bosbach, Dirk

    2015-09-01

    (Ln, An)xPO4 monazite-type ceramics are considered as potential matrices for the disposal of nuclear waste. In this study we computed the heat capacities and the standard entropies of these compounds using density functional perturbation theory. The calculations of lanthanide monazites agree well with the existing experimental data and provide information on the variation of the standard heat capacities and entropies along the lanthanide series. The results for AnPO4 monazites are similar to those obtained for the isoelectronic lanthanide compounds. This suggests that the missing thermodynamic data on actinide monazites could be similarly computed or assessed based on the properties of their lanthanide analogs. However, the computed heat capacity of PuPO4 appear to be significantly lower than the measured data. We argue that this discrepancy might indicate potential problems with the existing experimental data or with their interpretation. This shows a need for further experimental studies of the heat capacities of actinide-bearing, monazite-type ceramics.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-07-01

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

  17. The EBR-II X501 Minor Actinide Burning Experiment

    Energy Technology Data Exchange (ETDEWEB)

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

    2008-01-01

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

  18. Simultaneous photon and neutron interrogation using an electron accelerator in order to quantify actinides in encapsulated radioactive wastes; Double interrogation simultanee neutrons et photons utilisant un accelerateur d'electrons pour la caracterisation separee des actinides dans les dechets radioactifs enrobes

    Energy Technology Data Exchange (ETDEWEB)

    Jallu, F

    1999-09-24

    Measuring out alpha emitters, such as ({sup 234,235,236,238}U {sup 238,239,240,242,}2{sup 44P}u, {sup 237}Np {sup 241,243}Am...), 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 ({sup 235}U, {sup 239,241}Pu...) and fertile ({sup 236,238}U, {sup 238,240}Pu...) 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 ({gamma}, n), ({gamma}, 2n) and ({gamma}, 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 ({sup 235}U, {sup 239}Pu) and fertile ({sup 238}U) 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)

  19. Strategic Design and Optimization of Inorganic Sorbents For Cesium, Strontium and Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D.; Nyman, M.; Clearfield, A.; Maginn, E.

    2006-06-01

    The basic science goal in this project identifies structure/affinity relationships for selected radionuclides and existing sorbents. The task will apply this knowledge to the design and synthesis of new sorbents that will exhibit increased affinity for cesium, strontium and actinide separations. The target problem focuses on the treatment of high-level nuclear wastes. The general approach can likewise be applied to nonradioactive separations.

  20. Investigation of microscopic radiation damage in waste forms using ODNMR and AEM techniques. 1997 annual progress report

    Energy Technology Data Exchange (ETDEWEB)

    Liu, G.

    1997-09-01

    'This project seeks to understand the microscopic effects of radiation damage in nuclear waste forms. The authors approach to this challenge encompasses studies in electron microscopy, laser spectroscopy, and computational modeling and simulation. During this first year of the project, efforts have focused on a-decay induced microscopic damage in crystalline orthophosphates (YPO{sub 4} and LuPO{sub 4}) that contain the short-lived a-emitting isotope {sup 244}Cm (t{sub 1/2} = 18.1 y). The samples that they studied were synthesized in 1980 and the initial {sup 244}Cm concentration was {approximately}1%. Studying these materials is of importance to nuclear waste management because of the opportunity to gain insight into accumulated radiation damage and the influence of aging on such damage. These factors are critical to the long-term performance of actual waste forms [1]. Lanthanide orthophosphates, including LuPO{sub 4} and YPO{sub 4}, have been suggested as waste forms for high level nuclear waste [2] and potential hosts for excess weapons plutonium [3,4]. The work is providing insight into the characteristics of these previously known radiation-resistant materials. They have observed loss of crystallinity (partial amorphization) as a direct consequence of prolonged exposure to intense alpha radiolysis in these materials. More importantly, the observation of microscopic cavities in these aged materials provides evidence of significant chemical decomposition that may be difficult to detect in the earlier stages of radiation damage. The preliminary results show that, in characterizing crystalline compounds as high level nuclear waste forms, chemical decomposition effects may be more important than lattice amorphization which has been the focus of many previous studies. More extensive studies, including in-situ analysis of the dynamics of thermal annealing of self-radiation induced amorphization and cavity formation, will be conducted on these aged {sup 244}Cm

  1. Laboratory Testing of Bulk Vitrified Low-Activity Waste Forms to Support the 2005 Integrated Disposal Facility Performance Assessment

    Energy Technology Data Exchange (ETDEWEB)

    Pierce, Eric M.; McGrail, B. Peter; Bagaasen, Larry M.; Rodriguez, Elsa A.; Wellman, Dawn M.; Geiszler, Keith N.; Baum, Steven R.; Reed, Lunde R.; Crum, Jarrod V.; Schaef, Herbert T.

    2006-06-30

    The purpose of this report is to document the results from laboratory testing of the bulk vitri-fied (BV) waste form that was conducted in support of the 2005 integrated disposal facility (IDF) performance assessment (PA). Laboratory testing provides a majority of the key input data re-quired to assess the long-term performance of the BV waste package with the STORM code. Test data from three principal methods, as described by McGrail et al. (2000a; 2003a), are dis-cussed in this testing report including the single-pass flow-through test (SPFT) and product con-sistency test (PCT). Each of these test methods focuses on different aspects of the glass corrosion process. See McGrail et al. (2000a; 2003a) for additional details regarding these test methods and their use in evaluating long-term glass performance. In addition to evaluating the long-term glass performance, this report discusses the results and methods used to provided a recommended best estimate of the soluble fraction of 99Tc that can be leached from the engineer-ing-scale BV waste package. These laboratory tests are part of a continuum of testing that is aimed at improving the performance of the BV waste package.

  2. Laboratory Testing of Bulk Vitrified Low-Activity Waste Forms to Support the 2005 Integrated Disposal Facility Performance Assessment

    Energy Technology Data Exchange (ETDEWEB)

    Pierce, Eric M.; McGrail, B. Peter; Bagaasen, Larry M.; Rodriguez, Elsa A.; Wellman, Dawn M.; Geiszler, Keith N.; Baum, Steven R.; Reed, Lunde R.; Crum, Jarrod V.; Schaef, Herbert T.

    2005-03-31

    The purpose of this report is to document the results from laboratory testing of the bulk vitri-fied (BV) waste form that was conducted in support of the 2005 integrated disposal facility (IDF) performance assessment (PA). Laboratory testing provides a majority of the key input data re-quired to assess the long-term performance of the BV waste package with the STORM code. Test data from three principal methods, as described by McGrail et al. (2000a; 2003a), are dis-cussed in this testing report including the single-pass flow-through test (SPFT) and product con-sistency test (PCT). Each of these test methods focuses on different aspects of the glass corrosion process. See McGrail et al. (2000a; 2003a) for additional details regarding these test methods and their use in evaluating long-term glass performance. In addition to evaluating the long-term glass performance, this report discusses the results and methods used to provided a recommended best estimate of the soluble fraction of 99Tc that can be leached from the engineer-ing-scale BV waste package. These laboratory tests are part of a continuum of testing that is aimed at improving the performance of the BV waste package.

  3. CORRELATION OF POLYCHLORINATED NAPHTHALENES WITH POLYCHLORINATED DIBENZOFURANS FORMED FROM WASTE INCINERATION

    Science.gov (United States)

    Isomer composition of polychlorinated naphthalenes (PCNs) was measured for municipal waste incinerator fly ash samples,and for emission samples produced from soot and copper deposit experiments conducted at EPA. Two types of PCN isomer patterns were identified. One pattern cxonta...

  4. Assessment of SFR fuel pin performance codes under advanced fuel for minor actinide transmutation

    Energy Technology Data Exchange (ETDEWEB)

    Bouineau, V.; Lainet, M.; Chauvin, N.; Pelletier, M. [French Alternative Energies and Atomic Energy Commission - CEA, CEA Cadarache, DEN/DEC/SESC, 13108 Saint Paul lez Durance (France); Di Marcello, V.; Van Uffelen, P.; Walker, C. [European Commission, Joint Research Centre, Institute for Transuranium Elements, Hermann-von-Helmholtz-Platz 1, D- 76344 Eggenstein-Leopoldshafen (Germany)

    2013-07-01

    Americium is a strong contributor to the long term radiotoxicity of high activity nuclear waste. Transmutation by irradiation in nuclear reactors of long-lived nuclides like {sup 241}Am is, therefore, an option for the reduction of radiotoxicity and residual power packages as well as the repository area. In the SUPERFACT Experiment four different oxide fuels containing high and low concentrations of {sup 237}Np and {sup 241}Am, representing the homogeneous and heterogeneous in-pile recycling concepts, were irradiated in the PHENIX reactor. The behavior of advanced fuel materials with minor actinide needs to be fully characterized, understood and modeled in order to optimize the design of this kind of fuel elements and to evaluate its performances. This paper assesses the current predictability of fuel performance codes TRANSURANUS and GERMINAL V2 on the basis of post irradiation examinations of the SUPERFACT experiment for pins with low minor actinide content. Their predictions have been compared to measured data in terms of geometrical changes of fuel and cladding, fission gases behavior and actinide and fission product distributions. The results are in good agreement with the experimental results, although improvements are also pointed out for further studies, especially if larger content of minor actinide will be taken into account in the codes. (authors)

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

    Energy Technology Data Exchange (ETDEWEB)

    Dacheux, N

    2002-07-01

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

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

    CERN Document Server

    Sors, M

    1999-01-01

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

  7. Fabrication of uranium-based ceramics using internal gelation for the conversion of trivalent actinides; Herstellung uranbasierter Keramiken mittel interner Gelierung zur Konversion trivalenter Actinoiden

    Energy Technology Data Exchange (ETDEWEB)

    Daniels, Henrik

    2012-07-01

    Alternative to today's direct final waste disposal strategy of long-lived radionuclides, for example the minor actinides neptunium, americium, curium and californium, is their selective separation from the radioactive wastestream with subsequent transmutation by neutron irradiation. Hereby it is possible to obtain nuclides with a lower risk-potential concerning their radiotoxicity. 1 neutron irradiation can be carried out either with neutron sources or in the next generation of nuclear reactors. Before the treatment, the minor actinides need to be converted in a suitable chemical and physical form. Internal gelation offers a route through which amorphous gel-spheres can be obtained directly from a metal-salt solution. Due to the presence of different types of metal ions as well as changing pH-values in a stock solution, a complex hydrolysis behaviour of these elements before and during gelation occurs. Therefore, investigations with uranium and neodymium as a minor actinide surrogate were carried out. As a result of suitable gelation-parameters, uraniumneodymium gel-spheres were successfully synthesised. The spheres also stayed intact during the subsequent thermal treatment. Based upon these findings, uranium-plutonium and uranium-americium gels were successfully created. For theses systems, the determined parameters for the uraniumneodymium gelation could also be applied. Additionally, investigations to reduce the acidity of uranium-based stock solutions for internal gelation were carried out. The necessary amount of urea and hexamethylenetetramine to induce gelation could hereby be decreased. This lead to a general increase of the gel quality and made it possible to carry out uranium-americium gelation in the first place. To investigate the stability of urea and hexamethylenetetramine, solutions of these chemicals were irradiated with different radiation doses. These chemicals showed a high stability against radiolysis in aqueous solutions.

  8. Irradiation effect on leaching behavior and form of heavy metals in fly ash of municipal solid waste incinerator.

    Science.gov (United States)

    Nam, Sangchul; Namkoong, Wan

    2012-01-15

    Fly ash from a municipal solid waste incinerator (MSWI) is commonly classified as hazardous waste. High-energy electron beam irradiation systems have gained popularity recently as a clean and promising technology to remove environmental pollutants. Irradiation effects on leaching behavior and form of heavy metals in MSWI fly ash have not been investigated in any significant detail. An electron beam accelerator was used in this research. Electron beam irradiation on fly ash significantly increased the leaching potential of heavy metals from fly ash. The amount of absorbed dose and the metal species affected leaching behavior. When electron beam irradiation intensity increased gradually up to 210 kGy, concentration of Pb and Zn in the leachate increased linearly as absorbed dose increased, while that of Cu underwent no significant change. Concentration of Pb and Zn in the leachate increased up to 15.5% (10.7 mg/kg), and 35.6% (9.6 mg/kg) respectively. However, only 4.8% (0.3mg/kg) increase was observed in the case of Cu. The results imply that irradiation has significant effect on the leaching behavior of heavy metals in fly ash, and the effect is quite different among the metal species tested in this study. A commonly used sequential extraction analysis which can classify a metal species into five forms was conducted to examine any change in metal form in the irradiated fly ash. Notable change in metal form in fly ash was observed when fly ash was irradiated. Change in Pb form was much greater than that of Cu form. Change in metal form was related to leaching potential of the metals. Concentration of heavy metal in leachate was positively related to the exchangeable form which is the most mobile. It may be feasible to treat fly ash by electron beam irradiation for selective recovery of valuable metals or for pretreatment prior to conventional processes.

  9. Reduction of minor actinides for recycling in a light water reactor; Reduccion de actinidos menores por reciclado en un reactor de agua ligera

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-09-15

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

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

    Directory of Open Access Journals (Sweden)

    Salahuddin Asif

    2013-01-01

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

  11. Electronic Structure of the Actinide Metals

    DEFF Research Database (Denmark)

    Johansson, B.; Skriver, Hans Lomholt

    1982-01-01

    Some recent experimental photoelectron spectroscopic results for the actinide metals are reviewed and compared with the theoretical picture of the basic electronic structure that has been developed for the actinides during the last decade. In particular the experimental data confirm the change from...... itinerant to localized 5f electron behaviour calculated to take place between plutonium and americium. From experimental data it is shown that the screening of deep core-holes is due to 5f electrons for the lighter actinide elements and 6d electrons for the heavier elements. A simplified model for the full...... LMTO electronic structure calculations is introduced. In this model the spd and 5f electronic contributions are treated as separable entities. It is shown that the model reproduces quite well the results from the full treatment. The equilibrium volume, cohesive energy and bulk modulus are calculated...

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-02-01

    temperature or below. For many spectroscopic measurements, low temperatures have been achieved by co-condensing the actinide vapor in rare gas or inert molecule host matrices. Spectra recorded in matrices are usually considered to be minimally perturbed. Trapping the products from gas-phase reactions that occur when trace quantities of reactants are added to the inert host gas has resulted in the discovery of many new actinide species. Selected aspects of the matrix isolation data were discussed in chapter 17. In the present chapter we review the spectroscopic matrix data in terms of its relationship to gas-phase measurements, and update the description of the new reaction products found in matrices to reflect the developments that have occurred during the past two years. Spectra recorded in matrix environments are usually considered to be minimally perturbed, and this expectation is borne out for many closed shell actinide molecules. However, there is growing evidence that significant perturbations can occur for open shell molecules, resulting in geometric distortions and/or electronic state reordering. Studies of actinide reactions in the gas phase provide an opportunity to probe the relationship between electronic structure and reactivity. Much of this work has focused on the reactions of ionic species, as these may be selected and controlled using various forms of mass spectrometry. As an example of the type of insight derived from reaction studies, it has been established that the reaction barriers for An+ ions are determined by the promotion energies required to achieve the 5fn6d7s configuration. Gas-phase reaction studies also provide fundamental thermodynamic properties such as bond dissociation and ionization energies. In recent years, an increased number of gas-phase ion chemistry studies of bare (atomic) and ligated (molecular) actinide ions have appeared, in which relevant contributions to fundamental actinide chemistry have been made. These studies were initiated

  13. Conceptual study of fusion-driven system for nuclear waste transmutation

    Energy Technology Data Exchange (ETDEWEB)

    Hong, B.G., E-mail: bghong@jbnu.ac.kr

    2014-10-15

    A conceptual study of a fusion-driven system for nuclear waste transmutation using a low aspect ratio (LAR) tokamak as a neutron source is performed. A configuration of the LAR tokamak neutron source optimised with respect to both transmutation rate and the tritium breeding ratio for aspect ratio A in the range of 1.5–2.0 is found. The transmutation characteristics of both transuranic actinides and minor actinides are investigated and compared. When the transuranic actinides are loaded in the blanket, the neutron multiplication factor decreases from its initial value, k{sub eff} = 0.95, but with the minor actinides loaded in the blanket, the neutron multiplication factor shows a peak value during burn-up. The peak value can be controlled by adjusting the blanket dimensions. To transmute the nuclear waste effectively, an equilibrium fuel cycle is developed for both transuranic actinide and minor actinide transmutation.

  14. Actinide and fission product separation and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1993-07-01

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

  15. Spin–orbit coupling in actinide cations

    DEFF Research Database (Denmark)

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

    2012-01-01

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

  16. Extraction of metals using supercritical fluid and chelate forming legand

    Science.gov (United States)

    Wai, Chien M.; Laintz, Kenneth E.

    1998-01-01

    A method of extracting metalloid and metal species from a solid or liquid material by exposing the material to a supercritical fluid solvent containing a chelating agent is described. The chelating agent forms chelates that are soluble in the supercritical fluid to allow removal of the species from the material. In preferred embodiments, the extraction solvent is supercritical carbon dioxide and the chelating agent is a fluorinated .beta.-diketone. In especially preferred embodiments the extraction solvent is supercritical carbon dioxide, and the chelating agent comprises a fluorinated .beta.-diketone and a trialkyl phosphate, or a fluorinated .beta.-diketone and a trialkylphosphine oxide. Although a trialkyl phosphate can extract lanthanides and actinides from acidic solutions, a binary mixture comprising a fluorinated .beta.-diketone and a trialkyl phosphate or a trialkylphosphine oxide tends to enhance the extraction efficiencies for actinides and lanthanides. The method provides an environmentally benign process for removing contaminants from industrial waste without using acids or biologically harmful solvents. The method is particularly useful for extracting actinides and lanthanides from acidic solutions. The chelate and supercritical fluid can be regenerated, and the contaminant species recovered, to provide an economic, efficient process.

  17. Extraction of metals using supercritical fluid and chelate forming ligand

    Science.gov (United States)

    Wai, C.M.; Laintz, K.E.

    1998-03-24

    A method of extracting metalloid and metal species from a solid or liquid material by exposing the material to a supercritical fluid solvent containing a chelating agent is described. The chelating agent forms chelates that are soluble in the supercritical fluid to allow removal of the species from the material. In preferred embodiments, the extraction solvent is supercritical carbon dioxide and the chelating agent is a fluorinated {beta}-diketone. In especially preferred embodiments the extraction solvent is supercritical carbon dioxide, and the chelating agent comprises a fluorinated {beta}-diketone and a trialkyl phosphate, or a fluorinated {beta}-diketone and a trialkylphosphine oxide. Although a trialkyl phosphate can extract lanthanides and actinides from acidic solutions, a binary mixture comprising a fluorinated {beta}-diketone and a trialkyl phosphate or a trialkylphosphine oxide tends to enhance the extraction efficiencies for actinides and lanthanides. The method provides an environmentally benign process for removing contaminants from industrial waste without using acids or biologically harmful solvents. The method is particularly useful for extracting actinides and lanthanides from acidic solutions. The chelate and supercritical fluid can be regenerated, and the contaminant species recovered, to provide an economic, efficient process. 7 figs.

  18. Five-Year Implementation Plan For Advanced Separations and Waste Forms Capabilities at the Idaho National Laboratory (FY 2011 to FY 2015)

    Energy Technology Data Exchange (ETDEWEB)

    Not Listed

    2011-03-01

    DOE-NE separations research is focused today on developing a science-based understanding that builds on historical research and focuses on combining a fundamental understanding of separations and waste forms processes with small-scale experimentation coupled with modeling and simulation. The result of this approach is the development of a predictive capability that supports evaluation of separations and waste forms technologies. The specific suite of technologies explored will depend on and must be integrated with the fuel development effort, as well as an understanding of potential waste form requirements. This five-year implementation plan lays out the specific near-term tactical investments in people, equipment and facilities, and customer capture efforts that will be required over the next five years to quickly and safely bring on line the capabilities needed to support the science-based goals and objectives of INL’s Advanced Separations and Waste Forms RD&D Capabilities Strategic Plan.

  19. New data on mineral forms of rare metals in phosphogypsum wastes

    Science.gov (United States)

    Samonov, A. E.

    2011-09-01

    Phosphogypsum is an industrial waste of the processing of Khibiny apatite concentrate into chemical fertilizers by sulfurous technology. This is a valuable and promising technogenous rare-metal feedstock. The samples of fresh and old phosphogypsum were studied using precision physical techniques of analytical electron microscopy and X-ray spectral microanalysis. These studies allowed the discovery of new and unusual mineral compositions including strontium and rare earth metals in mineral fractions of phosphogypsum. The appearance of a new generation of technogenous rare-metal raw material permits us to characterize the prospects of its industrial use and to develop nonwaste technologies of its complex treatment.

  20. Laboratory Testing of Bulk Vitrified Low-Activity Waste Forms to Support the 2005 Integrated Disposal Facility Performance Assessment. Erratum

    Energy Technology Data Exchange (ETDEWEB)

    Smith, Gary L. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2016-09-06

    This report refers to or contains Kg values for glasses LAWA44, LAWB45 and LAWC22 affected by calculations errors as identified by Papathanassiu et al. (2011). The corrected Kg values are reported in an erratum included in the revised version of the original report. The revised report can be referenced as follows: Pierce E. M. et al. (2004) Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment. PNNL-14805 Rev. 0 Erratum. Pacific Northwest National Laboratory, Richland, WA, USA.

  1. Laboratory Testing of Bulk Vitrified Low-Activity Waste Forms to Support the 2005 Integrated Disposal Facility Performance Assessment Erratum

    Energy Technology Data Exchange (ETDEWEB)

    Smith, Gary L. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2016-09-06

    This report refers to or contains Kg values for glasses LAWA44, LAWB45 and LAWC22 affected by calculations errors as identified by Papathanassiu et al. (2011). The corrected Kg values are reported in an erratum included in the revised version of the original report. The revised report can be referenced as follows: Pierce E. M. et al. (2004) Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment. PNNL-14805 Rev. 0 Erratum. Pacific Northwest National Laboratory, Richland, WA, USA.

  2. Utilization of Minor Actinides as a Fuel Component for Ultra-Long Life Bhr Configurations: Designs, Advantages and Limitations

    Energy Technology Data Exchange (ETDEWEB)

    Dr. Pavel V. Tsvetkov

    2009-05-20

    This project assessed the advantages and limitations of using minor actinides as a fuel component to achieve ultra-long life Very High Temperature Reactor (VHTR) configurations. Researchers considered and compared the capabilities of pebble-bed and prismatic core designs with advanced actinide fuels to achieve ultra-long operation without refueling. Since both core designs permit flexibility in component configuration, fuel utilization, and fuel management, it is possible to improve fissile properties of minor actinides by neutron spectrum shifting through configuration adjustments. The project studied advanced actinide fuels, which could reduce the long-term radio-toxicity and heat load of high-level waste sent to a geologic repository and enable recovery of the energy contained in spent fuel. The ultra-long core life autonomous approach may reduce the technical need for additional repositories and is capable to improve marketability of the Generation IV VHTR by allowing worldwide deployment, including remote regions and regions with limited industrial resources. Utilization of minor actinides in nuclear reactors facilitates developments of new fuel cycles towards sustainable nuclear energy scenarios.

  3. Actinide ion extraction using room temperature ionic liquids: opportunities and challenges for nuclear fuel cycle applications.

    Science.gov (United States)

    Mohapatra, Prasanta Kumar

    2017-02-14

    Studies on the extraction of actinide ions from radioactive feeds have great relevance in nuclear fuel cycle activities, mainly in the back end processes focused on reprocessing and waste management. Room temperature ionic liquid (RTIL) based diluents are becoming increasingly popular due to factors such as more efficient extraction vis-à-vis molecular diluents, higher metal loading, higher radiation resistance, etc. The fascinating chemistry of the actinide ions in RTIL based solvent systems due to complex extraction mechanisms makes it a challenging area of research. By the suitable tuning of the cationic and anionic parts of the ionic liquids, their physical properties such as density, dielectric constant and viscosity can be changed which are considered key parameters in metal ion extraction. Aqueous solubility of the RTILs, which can lead to significant loss in the solvent inventory, can be avoided by appending the extractant moieties onto the ionic liquid. While the low vapour pressure and non-flammability of the ionic liquids make them appear as 'green' diluents, their aqueous solubility raises concerns of environmental hazards. The present article gives a summary of studies carried out on actinide ion extraction and presents perspectives of its applications in the nuclear fuel cycle. The article discusses various extractants used for actinide ion extraction and at many places, comparison is made vis-à-vis molecular diluents which includes the nature of the extracted species and the mechanism of extraction. Results of studies on rare earth elements are also included in view of their similarities with the trivalent minor actinides.

  4. Characteristics of spent fuel, high-level waste, and other radioactive wastes which may require long-term isolation: Appendix 3A, ORIGEN2 decay tables for immobilized high-level waste, Appendix 3B, Interim high-level waste forms, Appendix 3C, User's guide to the high-level waste PC data base

    Energy Technology Data Exchange (ETDEWEB)

    1987-12-01

    The purpose of this report, and the information contained in the associated computerized data bases, is to establish the DOE/OCRWM reference characteristics of the radioactive waste materials that may be accepted by DOE for emplacement in he mined geologic disposal system. This report provides relevant technical data for use by DOE and its supporting contractors and is not intended to be a policy document. This document is backed up by five PC-compatible data bases, written in a user-oriented, menu-driven format, which were developed for this purpose. The data bases are the LWR Assemblies Data Base; the LWR Radiological Data Base; the LWR Quantities Data Base; the LWR NFA Hardware Data Base; and the High-Level Waste Data Base. The above data bases may be ordered using the included form. Volume 6 contains decay tables for immobilized high-level waste, information on interim high-level waste forms, and a user's guide to the high-level waste PC data base.

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

    Energy Technology Data Exchange (ETDEWEB)

    Foerstendorf, Harald; Mueller, Katharina; Steudtner, Robin (eds.)

    2014-07-01

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

  6. Scalar Static Polarizabilities of Lanthanides and Actinides

    CERN Document Server

    Dzuba, V A; Flambaum, V V

    2014-01-01

    We calculate scalar static polarizabilities for lanthanides and actinides, the atoms with open $4f$ or $5f$ subshell. We show that polarizabilities of the low states are approximately the same for all states of given configuration and present a way of calculating them reducing valence space to just two or three valence electrons occupying $6s$ and $5d$ states for lanthanides or $7s$ and $6d$ states for actinides while $4f$ and $5f$ states are considered to be in the core. Configuration interaction technique is used to calculate polarizabilities of lanthanides and actinides for all states of the $4f^n6s^2$ and $4f^{n-1}6s^25d$ configurations of lanthanides and all states of the $5f^{n}7s^2$ and $5f^{n-1}7s^26d$ configurations of actinides. Polarizability of the electron core (including f-orbitals) has been calculated in the RPA approximation.

  7. Actinide and fission product partitioning and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1995-07-01

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

  8. Actinide valences in xenotime and monazite

    Energy Technology Data Exchange (ETDEWEB)

    Vance, E.R. [Institute of Materials Engineering, Australian Nuclear Science and Technology Organisation, Locked Bag 2001 Kirrawee DC, NSW 2232 (Australia); Zhang, Y., E-mail: yzx@ansto.gov.au [Institute of Materials Engineering, Australian Nuclear Science and Technology Organisation, Locked Bag 2001 Kirrawee DC, NSW 2232 (Australia); McLeod, T.; Davis, J. [Institute of Materials Engineering, Australian Nuclear Science and Technology Organisation, Locked Bag 2001 Kirrawee DC, NSW 2232 (Australia)

    2011-02-28

    Tetravalent U, Np and Pu can be substituted by ceramic methods into the rare earth site of xenotime and monazite in air atmospheres using Ca ions as charge compensators, while no evidence of penta- or hexavalent actinide ions was found. Some Pu{sup 3+} and Np{sup 3+} can be incorporated in xenotime samples fired in a reducing atmosphere.

  9. Standard practice for prediction of the long-term behavior of materials, including waste forms, used in engineered barrier systems (EBS) for geological disposal of high-level radioactive waste

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2007-01-01

    1.1 This practice describes test methods and data analyses used to develop models for the prediction of the long-term behavior of materials, such as engineered barrier system (EBS) materials and waste forms, used in the geologic disposal of spent nuclear fuel (SNF) and other high-level nuclear waste in a geologic repository. The alteration behavior of waste form and EBS materials is important because it affects the retention of radionuclides by the disposal system. The waste form and EBS materials provide a barrier to release either directly (as in the case of waste forms in which the radionuclides are initially immobilized), or indirectly (as in the case of containment materials that restrict the ingress of groundwater or the egress of radionuclides that are released as the waste forms and EBS materials degrade). 1.1.1 Steps involved in making such predictions include problem definition, testing, modeling, and model confirmation. 1.1.2 The predictions are based on models derived from theoretical considerat...

  10. Photoproducts of carminic acid formed by a composite from Manihot dulcis waste.

    Science.gov (United States)

    Antonio-Cisneros, Cynthia M; Dávila-Jiménez, Martín M; Elizalde-González, María P; García-Díaz, Esmeralda

    2015-04-15

    Carbon-TiO2 composites were obtained from carbonised Manihot dulcis waste and TiO2 using glycerol as an additive and thermally treating the composites at 800 °C. Furthermore, carbon was obtained from manihot to study the adsorption, desorption and photocatalysis of carminic acid on these materials. Carminic acid, a natural dye extracted from cochineal insects, is a pollutant produced by the food industry and handicrafts. Its photocatalysis was observed under different atmospheres, and kinetic curves were measured by both UV-Vis and HPLC for comparison, yielding interesting differences. The composite was capable of decomposing approximately 50% of the carminic acid under various conditions. The reaction was monitored by UV-Vis spectroscopy and LC-ESI-(Qq)-TOF-MS-DAD, enabling the identification of some intermediate species. The deleterious compound anthracene-9,10-dione was detected both in N2 and air atmospheres.

  11. Engineering test plan for US/UK higher actinides irradiations tests

    Energy Technology Data Exchange (ETDEWEB)

    Basmajian, J A

    1981-03-01

    The objective of the Higher Actinides Irradiations Program is to verify the neutronic and irradiation performance of americium and curium oxides in a fast reactor. The data obtained from the irradiation will be used to assess the basic neutronics parameters for actinide elements and determine the irradiation potential of the oxides of {sup 241}Am and {sup 244}Cm. This information has application in breeder reactor physics, fuel cycle analysis and assessment of waste management options. The irradiation test program is a cooperative effort wherein the US is supplying the completed irradiation test pins, while the UK will perform the irradiation in their Prototype Fast Reactor (PFR). Postirradiation examination and data analyses will be conducted on a cooperative basis, with some examinations performed in the UK and others in the US. 5 figs., 5 tabs.

  12. Simulation of alpha decay of actinides in iron phosphate glasses by ion irradiation

    Energy Technology Data Exchange (ETDEWEB)

    Dube, Charu L., E-mail: dubecharu@gmail.com; Stennett, Martin C.; Gandy, Amy S.; Hyatt, Neil C.

    2016-03-15

    Highlights: • Alpha decay of actinides in iron phosphate glasses is simulated by employing ion irradiation technique. • FTIR and Raman spectroscopic measurements confirm modification of glass network. • The depolymerisation of glass network after irradiation is attributed to synergetic effect of nuclear and electronic losses. - Abstract: A surrogate approach of ion beam irradiation is employed to simulate alpha decay of actinides in iron phosphate nuclear waste glasses. Bismuth and helium ions of different energies have been selected for simulating glass matrix modification owing to radiolysis and ballistic damage due to recoil atoms. Structural modification and change in coordination number of network former were probed by employing Reflectance Fourier-Transform Infrared (FT-IR), and Raman spectroscopies as a consequence of ion irradiation. Depolymerisation is observed in glass sample irradiated at intermediate energy of 2 MeV. Helium blisters of micron size are seen in glass sample irradiated at low helium ion energy of 30 keV.

  13. Actinide neutron induced cross section measurements using the oscillation technique in the Minerve reactor

    Energy Technology Data Exchange (ETDEWEB)

    Bernard, B.; Leconte, P.; Gruel, A.; Antony, M.; Di-Salvo, J.; Hudelot, J.P.; Pepino, A.; Lecluze, A. [CEA Cadarache, DEN/CAD/DER/SPRC/LEPh, 13 - Saint-Paul-lez-Durance (France)

    2009-07-01

    CEA is deeply involved research programs concerning nuclear fuel advanced studies (actinides, plutonium), waste management, the scientific and technical support of French PWR reactors and EPR reactor, and innovative systems. In this framework, specific neutron integral experiments have been carried out in the critical ZPR (zero power reactor) facilities of the CEA at Cadarache such as MINERVE, EOLE and MASURCA. This paper deals with MINERVE Pool Reactor experiments. MINERVE is mainly devoted to neutronics studies of different reactor core types. The aim is to improve the knowledge of the integral absorption cross sections of actinides (OSMOSE program), of new absorbers (OCEAN program) and also for fission Products (CBU program) in thermal, epithermal and fast neutron spectra. (authors)

  14. Stabilization of NaCl-containing cuttings wastes in cement concrete by in situ formed mineral phases.

    Science.gov (United States)

    Filippov, Lev; Thomas, Fabien; Filippova, Inna; Yvon, Jacques; Morillon-Jeanmaire, Anne

    2009-11-15

    Disposal of NaCl-containing cuttings is a major environmental concern due to the high solubility of chlorides. The present work aims at reducing the solubility of chloride by encapsulation in low permeability matrix as well as lowering its solubility by trapping into low-solubility phases. Both the studied materials were cuttings from an oil-based mud in oil drillings containing about 50% of halite, and cuttings in water-based mud from gas drilling containing 90% of halite. A reduction in the amount of dissolved salt from 41 to 19% according to normalized leaching tests was obtained by addition of potassium ortho-phosphate in the mortar formula of oil-based cuttings, while the aluminium dihydrogeno-phosphate is even more efficient for the stabilization of water-based cuttings with a NaCl content of 90%. Addition of ortho-phosphate leads to form a continuous and weakly soluble network in the cement matrix, which reduces the release of salt. The formed mineralogical phases were apatite and hydrocalumite. These phases encapsulate the salt grains within a network, thus lowering its interaction with water or/and trap chloride into low-solubility phases. The tested approaches allow to develop a confinement process of NaCl-containing waste of various compositions that can be applied to wastes, whatever the salt content and the nature of the drilling fluids (water or oil).

  15. Prototype Development of Remote Operated Hot Uniaxial Press (ROHUP) to Fabricate Advanced Tc-99 Bearing Ceramic Waste Forms - 13381

    Energy Technology Data Exchange (ETDEWEB)

    Alaniz, Ariana J.; Delgado, Luc R.; Werbick, Brett M. [University of Nevada - Las Vegas, Howard R. Hughes College of Engineering, 4505 S. Maryland Parkway, Box 454009, Las Vegas, NV 89154-4009 (United States); Hartmann, Thomas [University of Nevada - Las Vegas, Harry Reid Canter, 4505 S. Maryland Parkway, Box 454009, Las Vegas, NV 89154-4009 (United States)

    2013-07-01

    The objective of this senior student project is to design and build a prototype construction of a machine that simultaneously provides the proper pressure and temperature parameters to sinter ceramic powders in-situ to create pellets of rather high densities of above 90% (theoretical). This ROHUP (Remote Operated Hot Uniaxial Press) device is designed specifically to fabricate advanced ceramic Tc-99 bearing waste forms and therefore radiological barriers have been included in the system. The HUP features electronic control and feedback systems to set and monitor pressure, load, and temperature parameters. This device operates wirelessly via portable computer using Bluetooth{sup R} technology. The HUP device is designed to fit in a standard atmosphere controlled glove box to further allow sintering under inert conditions (e.g. under Ar, He, N{sub 2}). This will further allow utilizing this HUP for other potential applications, including radioactive samples, novel ceramic waste forms, advanced oxide fuels, air-sensitive samples, metallic systems, advanced powder metallurgy, diffusion experiments and more. (authors)

  16. Structural organization and spectroscopy of peptide-actinide(IV) complexes; Organisation structurale et spectroscopie de peptides susceptibles de complexer les actinides(IV)

    Energy Technology Data Exchange (ETDEWEB)

    Dahou, S.

    2010-11-05

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Garcia Carrera, A

    2001-07-01

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

  18. Institute of Energy and Climate Research IEK-6. Nuclear waste management and reactor safety report 2009/2010. Material science for nuclear waste management

    Energy Technology Data Exchange (ETDEWEB)

    Klinkenberg, M.; Neumeier, S.; Bosbach, D. (eds.)

    2011-07-01

    Due to the use of nuclear energy about 17.000 t (27.000 m{sup 3}) of high level waste and about 300.000 m{sup 3} of low and intermediated level waste will have accumulated in Germany until 2022. Research in the Institute of Energy and Climate Research (IEK-6), Nuclear Waste Management and Reactor Safety Division focuses on fundamental and applied aspects of the safe management of nuclear waste - in particular the nuclear aspects. In principle, our research in Forschungszentrum Juelich is looking at the material science/solid state aspects of nuclear waste management. It is organized in several research areas: The long-term safety of nuclear waste disposal is a key issue when it comes to the final disposal of high level nuclear waste in a deep geological formation. We are contributing to the scientific basis for the safety case of a nuclear waste repository in Germany. In Juelich we are focusing on a fundamental understanding of near field processes within a waste repository system. The main research topics are spent fuel corrosion and the retention of radionuclides by secondary phases. In addition, innovative waste management strategies are investigated to facilitate a qualified decision on the best strategy for Germany. New ceramic waste forms for disposal in a deep geological formation are studied as well as the partitioning of long-lived actinides. These research areas are supported by our structure research group, which is using experimental and computational approaches to examine actinide containing compounds. Complementary to these basic science oriented activities, IEK-6 also works on rather applied aspects. The development of non-destructive methods for the characterisation of nuclear waste packages has a long tradition in Juelich. Current activities focus on improving the segmented gamma scanning technique and the prompt gamma neutron activation analysis. Furthermore, the waste treatment group is developing concepts for the safe management of nuclear

  19. Management of Salt Waste from Electrochemical Processing of Used Nuclear Fuel

    Energy Technology Data Exchange (ETDEWEB)

    Michael F. Simpson; Michael N. Patterson; Joon Lee; Yifeng Wang; Joshua Versey; Ammon Williams; Supathorn Phongikaroon; James Allensworth; Man-Sung Yim

    2013-10-01

    Electrochemical processing of used nuclear fuel involves operation of one or more cells containing molten salt electrolyte. Processing of the fuel results in contamination of the salt via accumulation of fission products and transuranic (TRU) actinides. Upon reaching contamination limits, the salt must be removed and either disposed or treated to remove the contaminants and recycled back to the process. During development of the Experimental Breeder Reactor-II spent fuel treatment process, waste salt from the electrorefiner was to be stabilized in a ceramic waste form and disposed of in a high-level waste repository. With the cancellation of the Yucca Mountain high-level waste repository, other options are now being considered. One approach that involves direct disposal of the salt in a geologic salt formation has been evaluated. While waste forms such as the ceramic provide near-term resistance to corrosion, they may not be necessary to ensure adequate performance of the repository. To improve the feasibility of direct disposal, recycling a substantial fraction of the useful salt back to the process equipment could minimize the volume of the waste. Experiments have been run in which a cold finger is used for this purpose to crystallize LiCl from LiCl/CsCl. If it is found to be unsuitable for transportation, the salt waste could also be immobilized in zeolite without conversion to the ceramic waste form.

  20. DEVELOPMENT OF PROTOTYPE TITANATE ION EXCHANGE LOADED MEMBRANES FOR STRONTIUM, CESIUM AND ACTINIDE DECONTAMINATION FROM AQUEOUS MEDIA

    Energy Technology Data Exchange (ETDEWEB)

    Oji, L; Keisha Martin, K; David Hobbs, D

    2008-05-30

    We have successfully incorporated high surface area particles of titanate ion exchange materials (monosodium titanate and crystalline silicotitanate) with acceptable particle size distribution into porous and inert support membrane fibrils consisting of polytetrafluoroethylene (Teflon{reg_sign}), polyethylene and cellulose materials. The resulting membrane sheets, under laboratory conditions, were used to evaluate the removal of surrogate radioactive materials for cesium-137 and strontium-90 from high caustic nuclear waste simulants. These membrane supports met the nominal requirement for nonchemical interaction with the embedded ion exchange materials and were porous enough to allow sufficient liquid flow. Some of this 47-mm size stamped out prototype titanium impregnated ion exchange membrane discs was found to remove more than 96% of dissolved cesium-133 and strontium-88 from a caustic nuclear waste salt simulants. Since in traditional ion exchange based column technology monosodium titanate (MST) is known to have great affinity for the sorbing of other actinides like plutonium, neptunium and even uranium, we expect that the MST-based membranes developed here, although not directly evaluated for uptake of these three actinides because of costs associated with working with actinides which do not have 'true' experimental surrogates, would also show significant affinity for these actinides in aqueous media. It was also observed that crystalline silicotitanate impregnated polytetrafluoroethylene or polyethylene membranes became less selective and sorbed both cesium and strontium from the caustic aqueous salt simulants.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-12-10

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

  2. Criticality investigations for the fixed bed nuclear reactor using thorium fuel mixed with plutonium or minor actinides

    Energy Technology Data Exchange (ETDEWEB)

    Sahin, Suemer [Beykoz Lojistik Meslek Yueksekokulu, Beykoz, Istanbul (Turkey)], E-mail: sumer@gazi.edu.tr; Sahin, Haci Mehmet; Acir, Adem [Beykoz Lojistik Meslek Yueksekokulu, Istanbul (Turkey); Al-Kusayer, Tawfik Ahmed [King Saud University, College of Engineering, P.O. Box 800, Riyadh 11421 (Saudi Arabia)

    2009-08-15

    Prospective fuels for a new reactor type, the so called fixed bed nuclear reactor (FBNR) are investigated with respect to reactor criticality. These are (1) low enriched uranium (LEU); (2) weapon grade plutonium + ThO{sub 2}; (3) reactor grade plutonium + ThO{sub 2}; and (4) minor actinides in the spent fuel of light water reactors (LWRs) + ThO{sub 2}. Reactor grade plutonium and minor actinides are considered as highly radio-active and radio-toxic nuclear waste products so that one can expect that they will have negative fuel costs. The criticality calculations are conducted with SCALE5.1 using S{sub 8}-P{sub 3} approximation in 238 neutron energy groups with 90 groups in thermal energy region. The study has shown that the reactor criticality has lower values with uranium fuel and increases passing to minor actinides, reactor grade plutonium and weapon grade plutonium. Using LEU, an enrichment grade of 9% has resulted with k{sub eff} = 1.2744. Mixed fuel with weapon grade plutonium made of 20% PuO{sub 2} + 80% ThO{sub 2} yields k{sub eff} = 1.2864. Whereas a mixed fuel with reactor grade plutonium made of 35% PuO{sub 2} + 65% ThO{sub 2} brings it to k{sub eff} = 1.267. Even the very hazardous nuclear waste of LWRs, namely minor actinides turn out to be high quality nuclear fuel due to the excellent neutron economy of FBNR. A relatively high reactor criticality of k{sub eff} = 1.2673 is achieved by 50% MAO{sub 2} + 50% ThO{sub 2}. The hazardous actinide nuclear waste products can be transmuted and utilized as fuel in situ. A further output of the study is the possibility of using thorium as breeding material in combination with these new alternative fuels.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-01-08

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

  4. Actinide production from xenon bombardments of curium-248

    Energy Technology Data Exchange (ETDEWEB)

    Welch, R.B.

    1985-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1986-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Lascola, R.; Sharma, V.

    2010-06-03

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

  7. The Italian R D activitie in teh field of treatment and conditioning of 'third category' (high level) liquid radioactive wastes

    Energy Technology Data Exchange (ETDEWEB)

    Venditti, P.; Grossi, G.

    1989-10-01

    This paper summarizes the most significant R D activities carried out by ENEA (Italian Commission for Alternative Energy Sources) in support of the management of high-level radioactive wastes presently stored, in Italy, in liquid form. These R D activities concern essentially: - the treatment and conditioning of the liquid HLW produced by the experimental reprocessing pilot facilities EURX and ITREC (chemical processing, vitrification, characterization of borosilicate glass); - the treatment of liquid alpha bearing wastes produced by the experimental MOX fuel facility at CRE Casaccia (Italy) (chemical processing for selective removal of all actinides).

  8. Systematic investigation of the strontium zirconium phosphate ceramic form for nuclear waste immobilization

    Science.gov (United States)

    Pet'kov, Vladimir; Asabina, Elena; Loshkarev, Vladimir; Sukhanov, Maksim

    2016-04-01

    We have summarized our data and literature ones on the thermophysical properties and hydrolytic stability of Sr0.5Zr2(PO4)3 compound as a host NaZr2(PO4)3-type (NZP) structure for immobilization of 90Sr-containing radioactive waste. Absence of any polymorphic transformations on the temperature dependence of its heat capacity between 7 and 665 K is caused by the stability of crystalline Sr0.5Zr2(PO4)3. Calculated values of thermal conductivity coefficients at zero porosity in the range 298-673 K were 1.86-2.40 W·m-1 K-1. The compound may be classified as low thermal expanding material due to its average linear thermal expansion coefficient. Study of the hydrolytic stability in acid and alkaline media has shown that the relative mass fraction of Sr2+ ions, released into aggressive leaching media, didn't exceed 1% of the mass of sample. Soxhlet leaching studies have shown substantial resistance towards the release of Sr2+ ions into distilled water. Feeble sinterability constrains practical applications of NZP substances, that is why known in literature methods of Sr0.5Zr2(PO4)3 dense ceramics obtaining have been reviewed.

  9. Materials Characterization Center workshop on leaching mechanisms of nuclear waste forms, May 19-21, 1982, Gaithersburg, Maryland. Summary report

    Energy Technology Data Exchange (ETDEWEB)

    Mendel, J.E. (comp.)

    1982-08-01

    This is a report of the second workshop on the leaching mechanism of nuclear waste forms, which was held at Geithersburg, Maryland, May 19-21, 1982. The first session of the workshop was devoted to progress reports by participants in the leaching mechanisms program. These progress reports, as prepared by the participants, are given in Section 3.0. The goal of the remainder of the workshop was to exchange information on the development of repository-relevant leach testing techniques, often called interactions testing. To this end, a wide spectrum of investigators, many of whose work is sponsored by DOE's Nuclear Waste Terminal Storage (NWTS) project, made presentations at the workshop. These presentations were a significant and beneficial part of the workshop and are summarized in Sections 4.0, 5.0 and 6.0 according to the workshop agenda topics. In many cases, the presenters provided a written version of their presentation which has been included verbatim; in the other cases, the workshop chairman has supplied a brief synopsis. Twenty-one papers have been abstracted and indexed for inclusion in the data base.

  10. Cement As a Waste Form for Nuclear Fission Products: The Case of (90)Sr and Its Daughters.

    Science.gov (United States)

    Dezerald, Lucile; Kohanoff, Jorge J; Correa, Alfredo A; Caro, Alfredo; Pellenq, Roland J-M; Ulm, Franz J; Saúl, Andrés

    2015-11-17

    One of the main challenges faced by the nuclear industry is the long-term confinement of nuclear waste. Because it is inexpensive and easy to manufacture, cement is the material of choice to store large volumes of radioactive materials, in particular the low-level medium-lived fission products. It is therefore of utmost importance to assess the chemical and structural stability of cement containing radioactive species. Here, we use ab initio calculations based on density functional theory (DFT) to study the effects of (90)Sr insertion and decay in C-S-H (calcium-silicate-hydrate) in order to test the ability of cement to trap and hold this radioactive fission product and to investigate the consequences of its β-decay on the cement paste structure. We show that (90)Sr is stable when it substitutes the Ca(2+) ions in C-S-H, and so is its daughter nucleus (90)Y after β-decay. Interestingly, (90)Zr, daughter of (90)Y and final product in the decay sequence, is found to be unstable compared to the bulk phase of the element at zero K but stable when compared to the solvated ion in water. Therefore, cement appears as a suitable waste form for (90)Sr storage.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1991-01-01

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

  12. Production of Welding Fluxes Using Waste Slag Formed in Silicomanganese Smelting

    Science.gov (United States)

    Kozyrev, N. A.; Kryukov, R. E.; Kozyreva, O. E.; Lipatova, U. I.; Filonov, A. V.

    2016-04-01

    The possibility in principle of using slag, which is formed in the silicon-manganese smelting process, in producing welding fluxes is shown. The composition of and technology used for a new fused flux has been designed. A comparative evaluation of the new flux and the widely used AN-348 type flux was done. It has been proved that the new flux has high strength properties.

  13. Actinide Isotopes for the Synthesis of Superheavy Nuclei

    Science.gov (United States)

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

    2014-09-01

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

  14. Standard test method for accelerated leach test for diffusive releases from solidified waste and a computer program to model diffusive, fractional leaching from cylindrical waste forms

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2008-01-01

    1.1 This test method provides procedures for measuring the leach rates of elements from a solidified matrix material, determining if the releases are controlled by mass diffusion, computing values of diffusion constants based on models, and verifying projected long-term diffusive releases. This test method is applicable to any material that does not degrade or deform during the test. 1.1.1 If mass diffusion is the dominant step in the leaching mechanism, then the results of this test can be used to calculate diffusion coefficients using mathematical diffusion models. A computer program developed for that purpose is available as a companion to this test method (Note 1). 1.1.2 It should be verified that leaching is controlled by diffusion by a means other than analysis of the leach test solution data. Analysis of concentration profiles of species of interest near the surface of the solid waste form after the test is recommended for this purpose. 1.1.3 Potential effects of partitioning on the test results can...

  15. Actinide and fission product separation and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1991-07-01

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

  16. Microbial Transformations of Actinides and Other Radionuclides

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-01-07

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

  17. Actinide and fission product partitioning and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1997-07-01

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

  18. DEVELOPMENT OF AN IMPROVED SODIUM TITANATE FOR THE PRETREATMENT OF NUCLEAR WASTE AT THE SAVANNAH RIVER SITE

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D

    2008-01-22

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove Cs-137, Sr-90 and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes planned at SRS include sorption of Sr-90 and alpha-emitting radionuclides onto monosodium titanate (MST) and caustic side solvent extraction, for Cs-137 removal. The MST and separated Cs-137 will be encapsulated into a borosilicate glass waste form for eventual entombment at the federal repository. The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes Pu-238, Pu-239 and Pu-240. This paper describes recent results to produce an improved sodium titanate material that exhibits increased removal kinetics and capacity for Sr-90 and alpha-emitting radionuclides compared to the baseline MST material.

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

    Directory of Open Access Journals (Sweden)

    Walter Olaf

    2016-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-07-05

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

  1. Fast methods for determination of antropogenic actinides and U/Th-series isotopes in aqueous samples.

    Science.gov (United States)

    Eikenberg, J; Bajo, S; Beer, H; Hitz, J; Ruethi, M; Zumsteg, I; Letessier, P

    2004-01-01

    Rapid and simple methods are applied at the PSI radioanalytical laboratory for determining anthropogenic actinides in waste and nuclear reactor waters (U, Pu, Am, Cm) as well as for analysis of naturally occurring alpha-emitters in continental river and ground water. Anion exchange chromatography followed by alpha-spectrometry as well as alpha/beta-LSC is applied for the reactor coolant waters. To avoid alpha-spectrum interference between 238Pu and 241Am at 5.5 MeV, the Pu-fraction is purified using anion exchange resin. Prior to the separation of the Pu-fraction, all actinides (U, Pu, Am, Cm) are adsorbed batch-wise under stirring onto Actinide Resin and subsequent decomposition of the reagent. The residue is then re-dissolved in a sulfate buffer solution for electrolytic deposition. In tabular water samples isotopes of Ra and Po are analyzed additionally via sorption onto manganese coated discs (Ra) and deposition on silver discs (Po). For counting times of 1 day and use of 0.1-1l sample aliquots, detection limits of a few mBql(-1) can be obtained easily.

  2. Study on separation of minor actinides from HLLW with new extractant of TODGA-DHOA/Kerosene

    Energy Technology Data Exchange (ETDEWEB)

    Ye, Guo-an; Zhu, Wen-bin; Li, Feng-feng; Lin, Ru-shan; Li, Hui-rong [China Institute of Atomic Energy, P.O.Box 275-26, Beijing 102413 (China)

    2013-07-01

    The extraction behavior of U, Np, Pu, Am, rare earth elements and Sr from nitric acid solutions by TODGA/dodecan, DHOA/dodecane and TODGA-DHOA/dodecane were investigated, respectively. Based on experimental results, a separation process was proposed for minor actinide isolation from high level liquid waste (HLLW): the TODGA-DHOA/kerosene system. The multi-stage counter-current cascade experiments were carried out for the purpose by 0.1 mol/l TODGA-1.0 mol/l DHOA/kerosene with miniature mixer- settler contactor rigs (8 stages for extraction, 6 stages for scrubbing, 8 stages for first stripping, 8 stages for second stripping). The results show that the recovery efficiencies of the actinides and lanthanides are more than 99.9%, whereas less than 1% Sr was extracted by 0.1 mol/l TODGA - 1.0 mol/l DHOA/kerosene. The stripping efficiencies of U, Np and Pu are more than 95% in the first stripping step by 0.5 mol/l HNO{sub 3} + 0.5 mol/l AHA(aceto-hydroxamic acid), all of the remained actinides and lanthanides can be stripped by 0.01 mol/l HNO{sub 3} in the second stripping step. 99% Sr was extracted by 0.1 mol/l TODGA/kerosene, so Sr can be recovered efficiently directly from the raffinate by 0.1 mol/l TODGA/kerosene. (authors)

  3. Hydrothermal processing of radioactive combustible waste

    Energy Technology Data Exchange (ETDEWEB)

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

    1998-09-01

    Hydrothermal processing has been demonstrated for the treatment of radioactive combustible materials for the US Department of Energy. A hydrothermal processing system was designed, built and tested for operation in a plutonium glovebox. Presented here are results from the study of the hydrothermal oxidation of plutonium and americium contaminated organic wastes. Experiments show the destruction of the organic component to CO{sub 2} and H{sub 2}O, with 30 wt.% H{sub 2}O{sub 2} as an oxidant, at 540 C and 46.2 MPa. The majority of the actinide component forms insoluble products that are easily separated by filtration. A titanium liner in the reactor and heat exchanger provide corrosion resistance for the oxidation of chlorinated organics. The treatment of solid material is accomplished by particle size reduction and the addition of a viscosity enhancing agent to generate a homogeneous pumpable mixture.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1990-12-01

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

  5. Monazite-type ceramics for conditioning of minor actinides. Structural characterization and properties

    Energy Technology Data Exchange (ETDEWEB)

    Babel