WorldWideScience

Sample records for actinide waste forms

  1. Nuclear waste forms for actinides

    Science.gov (United States)

    Ewing, Rodney C.

    1999-01-01

    The disposition of actinides, most recently 239Pu from dismantled nuclear weapons, requires effective containment of waste generated by the nuclear fuel cycle. Because actinides (e.g., 239Pu and 237Np) are long-lived, they have a major impact on risk assessments of geologic repositories. Thus, demonstrable, long-term chemical and mechanical durability are essential properties of waste forms for the immobilization of actinides. Mineralogic and geologic studies provide excellent candidate phases for immobilization and a unique database that cannot be duplicated by a purely materials science approach. The “mineralogic approach” is illustrated by a discussion of zircon as a phase for the immobilization of excess weapons plutonium. PMID:10097054

  2. Monazite as a suitable actinide waste form

    Energy Technology Data Exchange (ETDEWEB)

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

    2013-03-01

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

  3. Actinide Waste Forms and Radiation Effects

    Science.gov (United States)

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

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2001-03-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1997-10-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1997-03-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2006-11-16

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2006-06-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2006-06-01

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

  10. Actinide-Aluminate Speciation in Alkaline Radioactive Waste

    Energy Technology Data Exchange (ETDEWEB)

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

    2001-12-21

    Investigation of behavior of actinides in alkaline media containing AL(III) showed that no aluminate complexes of actinides in oxidation states (IIII-VIII) were formed in alkaline solutions. At alkaline precipitation IPH (10-14) of actinides in presence of AL(III) formation of aluminate compounds is not observed. However, in precipitates contained actinides (IIV)<(VI), and to a lesser degree actinides (III), some interference of components takes place that is reflected in change of solid phase properties in comparison with pure components or their mechanical mixture. The interference decreases with rise of precipitation PH and at PH 14 is exhibited very feebly. In the case of NP(VII) the individual compound with AL(III) is obtained, however it is not aluminate of neptunium(VII), but neptunate of aluminium(III) similar to neptunates of other metals obtained earlier.

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

    Science.gov (United States)

    Zänker, Harald; Hennig, Christoph

    2014-02-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2005-11-01

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

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

    Science.gov (United States)

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

    2013-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2013-11-01

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

  15. Densified waste form and method for forming

    Science.gov (United States)

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

    2015-08-25

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

  16. Preparation of Y2Ti2O7 pyrochlore glass-ceramics as potential waste forms for actinides: The effects of processing conditions

    Science.gov (United States)

    Kong, Linggen; Zhang, Yingjie; Karatchevtseva, Inna

    2017-10-01

    Glass-Y2Ti2O7 pyrochlore was fabricated by sintering the mixture of glass precursor powder and (YTi)-composite which was prepared by a soft chemistry route. X-ray diffraction and Raman spectroscopy confirmed that the phase pure pyrochlore was crystallized in-situ in amorphous glass matrix at 1200 °C with dwelling time over 1 h. Pyrochlore was formed in glass matrix with cooling rate ∼0.1-40 °C/min, and independent of addition of alkali/alkaline earth fluorides. Glass matrix was able to accommodate/dissolve small amounts of impurities and the mean pyrochlore particle size was between 1 and 2 μm in glass observed by scanning electron microscopy.

  17. Interaction of selected actinides (U, Cm) with bacteria relevant to nuclear waste disposal

    Energy Technology Data Exchange (ETDEWEB)

    Luetke, Laura

    2013-07-01

    To assess the safety of a site destined for storage of nuclear waste enhanced research effort is demanded to investigate the complex interactions of released radionuclides with parts of the environment that includes indigenous microorganisms. This work aimed at assessing the interactions of two bacterial strains with the actinides uranium and curium with a focus on thermodynamics to provide stability constants of the actinide bacteria species formed usable for modelling the distribution of these actinides in the environment. The influences of Pseudomonas fluorescens (CCUG 32456A) isolated from the granitic aquifers at Aespoe(Sweden) and a novel isolate from Mont Terri Opalinus clay (Switzerland), Paenibacillus sp. MT-2.2, were investigated. A combined approach using microbiological and spectroscopic techniques as well as potentiometry was employed to characterize the U(VI) and Cm(III) binding onto the cell surface functional groups structurally and thermodynamically. Further, due to its similar ionic radius to Cm(III) also Eu(III) was studied as non-radioactive analog.

  18. Characterization of a ceramic waste form encapsulating radioactive electrorefiner salt

    Energy Technology Data Exchange (ETDEWEB)

    Moschetti, T. L.; Sinkler, W.; DiSanto, T.; Noy, M.; Warren, A. R.; Cummings, D. G.; Johnson, S. G.; Goff, K. M.; Bateman, K. J.; Frank, S. M.

    1999-11-11

    Argonne National Laboratory has developed a ceramic waste form to immobilize radioactive waste salt produced during the electrometallurgical treatment of spent fuel. This study presents the first results from electron microscopy and durability testing of a ceramic waste form produced from that radioactive electrorefiner salt. The waste form consists of two primary phases: sodalite and glass. The sodalite phase appears to incorporate most of the alkali and alkaline earth fission products. Other fission products (rare earths and yttrium) tend to form a separate phase and are frequently associated with the actinides, which form mixed oxides. Seven-day leach test results are also presented.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-03-31

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Halada, Gary P

    2008-04-10

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Nash, Kenneth L.

    2008-11-20

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

  2. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1979-08-01

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

  4. ANSTO's waste forms for the 31. century

    Energy Technology Data Exchange (ETDEWEB)

    Vance, E.R.; Begg, B. D.; Day, R. A.; Moricca, S.; Perera, D. S.; Stewart, M. W. A.; Carter, M. L.; McGlinn, P. J.; Smith, K. L.; Walls, P. A.; Robina, M. La

    2004-07-01

    ANSTO waste form development for high-level radioactive waste is directed towards practical applications, particularly problematic niche wastes that do not readily lend themselves to direct vitrification. Integration of waste form chemistry and processing method is emphasised. Some longstanding misconceptions about titanate ceramics are dealt with. We have a range of titanate-bearing waste form products aimed at immobilisation of tank wastes and sludges, actinide-rich wastes, INEEL calcines and Na-bearing liquid wastes, Al-rich wastes arising from reprocessing of Al-clad fuels, Mo-rich wastes arising from reprocessing of U-Mo fuels, partitioned Cs-rich wastes, and {sup 99}Tc. Waste form production techniques cover hot isostatic and uniaxial pressing, sintering, and cold-crucible melting, and these are strongly integrated into waste form design. Speciation and leach resistance of Cs and alkalis in cementitious products and geo-polymers are being studied. Recently we have embarked on studies of candidate inert matrix fuels for Pu burning. We also have a considerable program directed at basic understanding of the waste forms in regard to crystal chemistry, dissolution behaviour in aqueous media, radiation damage effects and optimum processing techniques. (authors)

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

    Energy Technology Data Exchange (ETDEWEB)

    Rudisill, T.; Thompson, M.

    2011-09-20

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

  6. 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.

  7. Actinide speciation in environmental remediation

    Energy Technology Data Exchange (ETDEWEB)

    Plaue, Jon; Czerwinski, Ken R. [Massachusetts Institute of Technology, Nuclear Engineering Dept., Cambridge, MA (United States)

    2002-11-01

    Environmental actinide remediation is often performed in the absence of a clear understanding of the contaminant chemical forms. Remediation efforts are more concerned with the initial and final concentration of the contaminant actinides. Allowable final concentrations of actinides in remediation sites are mainly based on expected dose or prenegotiated levels. However, understanding the chemical forms of actinides in the environment is key to assessing their long-term behavior and developing enhanced analytical methods for their environmental detection. The dominant environmental chemical form will dictate the actinide transport behavior through solubility, colloid formation, or the interaction with natural ligands. This information can be used to evaluate the fate and potential transport of actinides. If the dominant environmental chemical species are understood, analytical methods for enhanced counting statistics and a reduction of counting error can be developed. A reduction in counting error will increase the fraction of verifiable waste below a given threshold, thereby increasing the rate of site clean up while reducing the cost. The impact of actinide speciation is presented in 2 sites contaminated with Am and Pu undergoing remediation. Actinide speciation has affected remediation strategies, regulatory response, and costs. (author)

  8. 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).

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

    Energy Technology Data Exchange (ETDEWEB)

    Novak, C.F. [ed.

    1995-08-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-03-31

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

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

    Science.gov (United States)

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

    2009-03-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-03-31

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

  13. 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.

  14. 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.

  15. 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.

  16. Demonstration of an optimized TRUEX flowsheet for partitioning of actinides from actual ICPP sodium-bearing waste using centrifugal contactors in a shielded cell facility

    Energy Technology Data Exchange (ETDEWEB)

    Law, J.D.; Brewer, K.N.; Herbst, R.S.; Todd, T.A.; Olson, L.G.

    1998-01-01

    The TRUEX process is being evaluated at the Idaho Chemical Processing Plant (ICPP) for the separation of the actinides from acidic radioactive wastes stored at the ICPP. These efforts have culminated in recent demonstrations of the TRUEX process with actual tank waste. The first demonstration was performed in 1996 using 24 stages of 2-cm diameter centrifugal contactors and waste from tank WM-183. Based on the results of this flowsheet demonstration, the flowsheet was optimized and a second flowsheet demonstration was performed. This test also was performed using 2-cm diameter centrifugal contactors and waste from tank WM-183. However, the total number of contactor stages was reduced from 24 to 20. Also, the concentration of HEDPA in the strip solution was reduced from 0.04 M to 0.01 M in order to minimize the amount of phosphate in the HLW fraction, which would be immobilized into a glass waste form. This flowsheet demonstration was performed using centrifugal contactors installed in the shielded hot cell at the ICPP Remote Analytical Laboratory. The flowsheet tested consisted of six extraction stages, four scrub stages, six strip stages, two solvent was stages, and two acid rinse stages. An overall removal efficiency of 99.79% was obtained for the actinides. As a result, the activity of the actinides was reduced from 540 nCi/g in the feed to 0.90 nCi/g in the aqueous raffinate, which is well below the NRC Class A LLW requirement of 10 nCi/g for non-TRU waste. Removal efficiencies of 99.84%, 99.97%, 99.97%, 99.85%, and 99.76% were obtained for {sup 241}Am, {sup 238}Pu, {sup 239}Pu, {sup 235}U, and {sup 238}U, respectively.

  17. Model Analysis of Low-Level Actinide Waste Disposal in Deep Boreholes

    Science.gov (United States)

    Glascoe, L. G.; Wolfsberg, A. V.

    2001-12-01

    Deep borehole disposal is considered as a possible mechanism for the safe removal of Greater Than Class C (GTCC) low level actinide waste (Am-241, Pu-239, and Pu-238). Of the three actinides in GTCC waste, only Pu-239 has a half-life greater than 500 years and, thus, will have the longest environmental presence. However, Am-241 and Pu-238 have the potential to create most of the heat associated with GTCC waste disposal in deep boreholes. Therefore, this study considers the nonisothermal release and subsequent migration toward a pumping well of the most persistent radionuclide, Pu-239, from a deep emplacement borehole taking into account the heat created by decay of all three actinides. The Finite-Element Heat- and Mass-Transfer code, FEHM, is employed to simulate three-dimensional, non-isothermal flow and solute transport using particle tracking. Multiple scenarios considering various source emplacement depths, aquifer properties, and hydraulic conditions are evaluated in a sensitivity analysis that seeks to demonstrate competing and offsetting processes affecting the concentration of Pu-239 in the pumped well 100 m down gradient from the borehole source. In general, lower groundwater fluxes, associated with lower gradients and/or lower aquifer permeabilities, lead to less dissolution of the source waste. However, conditions of decreasing groundwater flux also create larger sized capture zones by the pumping well, thus escalating the likelihood of pumping contaminants originating from a source deeper than the pumping well. Retardation by sorption of Pu-239, both in alluvial aquifers and following diffusion from fractures in a tuff aquifer, plays an important role both in delaying radionuclide migration and in reducing the peak aqueous concentration at the pumping well. This work was performed under the auspices of the U.S. Department of Energy by University of California Lawrence Livermore National Laboratory under contract No. W-7405-Eng-48. This work was

  18. 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.

  19. 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.

  20. 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

  1. Coated particle waste form development

    Energy Technology Data Exchange (ETDEWEB)

    Oma, K.H.; Buckwalter, C.Q.; Chick, L.A.

    1981-12-01

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

  2. TSA waste stream and final waste form composition

    Energy Technology Data Exchange (ETDEWEB)

    Grandy, J.D.; Eddy, T.L.; Anderson, G.L.

    1993-01-01

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

  3. Research in actinide chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Choppin, G.R.

    1993-01-01

    This research studies the behavior of the actinide elements in aqueous solution. The high radioactivity of the transuranium actinides limits the concentrations which can be studied and, consequently, limits the experimental techniques. However, oxidation state analogs (trivalent lanthanides, tetravalent thorium, and hexavalent uranium) do not suffer from these limitations. Behavior of actinides in the environment are a major USDOE concern, whether in connection with long-term releases from a repository, releases from stored defense wastes or accidental releases in reprocessing, etc. Principal goal of our research was expand the thermodynamic data base on complexation of actinides by natural ligands (e.g., OH[sup [minus

  4. 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.

  5. CMP flowsheet development for the separation of actinides from ICPP sodium-bearing waste using centrifugal contactors

    Energy Technology Data Exchange (ETDEWEB)

    Law, J.D.; Herbst, R.S.; Rodriguez, A.M.

    1995-08-01

    Previous results of lab-scale batch contacts with sodium-bearing waste (SBW) simulant suggested a potential flowsheet for partitioning actinides using solvent extraction with dihexyl-N,N-diethylcarbamoylmethyl phosphonate (DHDECMP or simply CMP) as the extractant. The suggested baseline flowsheet includes: an extraction section to remove actinides from liquid SBW into the CMP solvent (0.75 M CMP, 1.0 M TBP in Isopar-L{reg_sign}); a thermally unstable complexant (TUCS) strip section to back-extract actinides; a sodium carbonate wash section for solvent cleanup; and a dilute HNO{sub 3} rinse section to re-acidify the solvent. The purpose of these studies was to test and develop a baseline CMP flowsheet for Idaho Chemical Processing Plant (ICPP) SBW under continuous, countercurrent conditions using centrifugal contactors. This flowsheet was tested in two experiments using the Centrifugal Contactor Mockup which consists of sixteen stages of 5.5 cm diameter centrifugal contactors (procured from Oak Ridge National Laboratory). All testing was performed using non-radioactive SBW simulant. Potential flowsheets were evaluated with regard to the behavior of the non-radioactive components potentially extracted by the CMP solvent. Specifically, the behavior of the matrix components, including Fe, Hg, and Zr, was studied. In addition, Nd was added to the SBW simulant as a surrogate for {sup 241}Am. In general, the behavior of the individual components closely paralleled that anticipated from batch testing. Based on the assumption that the behavior of Am will be very similar to the behavior of the Nd surrogate, eight extraction stages are more than sufficient to reduce the actinide content in the SBW to levels well below the NRC Class A LLW criteria of 10 nCi/g. Very little Fe or Zr were extracted from the SBW simulant, resulting in only 1% of the Fe and 4% of the Zr exiting in the high-activity waste (HAW) fraction.

  6. Heterogeneous sodium fast reactor designed for transmuting minor actinide waste isotopes into plutonium fuel

    Science.gov (United States)

    Bays, Samuel Eugene

    2008-10-01

    In the past several years there has been a renewed interest in sodium fast reactor (SFR) technology for the purpose of destroying transuranic waste (TRU) produced by light water reactors (LWR). The utility of SFRs as waste burners is due to the fact that higher neutron energies allow all of the actinides, including the minor actinides (MA), to contribute to fission. It is well understood that many of the design issues of LWR spent nuclear fuel (SNF) disposal in a geologic repository are linked to MAs. Because the probability of fission for essentially all the "non-fissile" MAs is nearly zero at low neutron energies, these isotopes act as a neutron capture sink in most thermal reactor systems. Furthermore, because most of the isotopes produced by these capture reactions are also non-fissile, they too are neutron sinks in most thermal reactor systems. Conversely, with high neutron energies, the MAs can produce neutrons by fast fission. Additionally, capture reactions transmute the MAs into mostly plutonium isotopes, which can fission more readily at any energy. The transmutation of non-fissile into fissile atoms is the premise of the plutonium breeder reactor. In a breeder reactor, not only does the non-fissile "fertile" U-238 atom contribute fast fission neutrons, but also transmutes into fissile Pu-239. The fissile value of the plutonium produced by MA transmutation can only be realized in fast neutron spectra. This is due to the fact that the predominate isotope produced by MA transmutation, Pu-238, is itself not fissile. However, the Pu-238 fission cross section is significantly larger than the original transmutation parent, predominately: Np-237 and Am-241, in the fast energy range. Also, Pu-238's fission cross section and fission-to-capture ratio is almost as high as that of fissile Pu-239 in the fast neutron spectrum. It is also important to note that a neutron absorption in Pu-238, that does not cause fission, will instead produce fissile Pu-239. Given this

  7. 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

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

    Energy Technology Data Exchange (ETDEWEB)

    Randklev, E.H.

    1993-06-01

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

  9. 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); Nichols, R. L. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2017-07-31

    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, including Direct Feed Low Activity Waste (DFLAW) vitrification, 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. The powdered salt waste form produced by the ETF will be replaced by a stabilized solidified waste form for disposal in Hanford’s Integrated Disposal Facility (IDF). 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 IDF. Waste form testing to support this plan is composed of work in the near term to provide data as input to a performance assessment (PA) for Hanford’s IDF. In 2015, three Hanford Liquid Secondary Waste simulants were developed based on existing and projected waste streams. Using these waste simulants, fourteen mixes of Hanford Liquid Secondary Waste were prepared and tested varying the waste simulant, the water-to-dry materials ratio, and the dry materials blend composition.1 In FY16, testing was performed using a simulant of the EMF process condensate blended with the caustic scrubber—from the Low Activity Waste (LAW) melter—, processed through the ETF. The initial EMF-16 simulant will be based on modeling efforts performed to determine the mass balance of the ETF for the DFLAW.2 The compressive strength of all of the mixes exceeded the target of 3.4 MPa (500 psi) to meet the requirements identified as potential IDF Waste Acceptance Criteria in Table 1 of the Secondary Liquid Waste Immobilization Technology Development Plan.3 The hydraulic properties of the waste forms tested (hydraulic conductivity

  10. 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.

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

    Science.gov (United States)

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

    2015-10-01

    Aeolian and pluvial processes represent important mechanisms for the movement of actinides and fission products at the Earth's surface. Soil samples taken in the early 1970's near a Department of Energy radioactive waste disposal site (the Subsurface Disposal Area, SDA, located in southeastern Idaho) provide a case study for studying the mechanisms and characteristics of environmental actinide and (137)Cs transport in an arid environment. Multi-component mixing models suggest actinide contamination within 2.5 km of the SDA can be described by mixing between 2 distinct SDA end members and regional nuclear weapons fallout. The absence of chemical fractionation between (241)Am and (239+240)Pu with depth for samples beyond the northeastern corner and lack of (241)Am in-growth over time (due to (241)Pu decay) suggest mechanical transport and mixing of discrete contaminated particles under arid conditions. Occasional samples northeast of the SDA (the direction of the prevailing winds) contain anomalously high concentrations of Pu with (240)Pu/(239)Pu isotopic ratios statistically identical to those in the northeastern corner. Taken together, these data suggest flooding resulted in mechanical transport of contaminated particles into the area between the SDA and a flood containment dike in the northeastern corner, following which subsequent contamination spreading in the northeastern direction resulted from wind transport of discrete particles. Copyright © 2015 Elsevier Ltd. All rights reserved.

  12. Actinide oxide photodiode and nuclear battery

    Energy Technology Data Exchange (ETDEWEB)

    Sykora, Milan; Usov, Igor

    2017-12-05

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

  13. 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.

  14. 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.

  15. Development of a glass-encapsulated calcium phosphate wasteform for the immobilization of actinide and halide containing radioactive wastes from the pyrochemical reprocessing of plutonium metal

    Energy Technology Data Exchange (ETDEWEB)

    Fong, S.K. [AWE, Aldermaston, Berkshire (United Kingdom)], E-mail: shirley.fong@awe.co.uk; Donald, I.W.; Metcalfe, B.L. [AWE, Aldermaston, Berkshire (United Kingdom)

    2007-10-11

    Chloride-containing radioactive wastes are generated during the pyrochemical reprocessing of Pu metal. Immobilization of these wastes in borosilicate glass or Synroc-type ceramics is not viable due to the very low solubility of chlorides in these hosts. Alternative wasteforms, including zeolites and direct vitrification in phosphate glasses, were therefore studied. However, the preferred option was to immobilize the waste in calcium phosphate ceramics, forming a number of stable mineral phases including chlorapatite, chloride-substituted fluorapatite and spodiosite. The immobilization process developed in this study involves a solid state process in which waste and host powders are reacted in air at temperatures in the range of 700-800 deg. C. The ceramic products obtained by this process are non-hygroscopic free-flowing powders that require encapsulation in glass to produce a monolithic wasteform suitable for storage and ultimate disposal. A suitable relatively low melting temperature phosphate-based glass was identified. Durability trials of both the ceramic powder and sintered glass-ceramic hybrid wasteform indicate that both the halides and actinide surrogate ions are satisfactorily immobilized.

  16. Waste Management Strategy in The Netherlands. Part 1. Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Haverkate, B.R.W

    2002-05-08

    This report reflects the input prepared in the framework of work package 1 of the thematic network COMPAS, which deals with the identification of waste forms in EU member states and their applicant countries. In accordance with the COMPAS project plan a brief introduction of the nuclear industry in The Netherlands and some historical milestones in radioactive waste research are given first (in chapter 1), after which the current waste management policy is described (in chapter 2). Those aspects that could play a role in identifying alternative waste management strategies and influencing strategy issues have been emphasised. The current and projected radioactive waste forms will be part of this (decision) process and consequently are summarised in (chapter 3 of) this report. Finally, advanced waste reduction technologies are addressed (in chapter 4), because they could influence (future) waste management strategies. Naturally radioactive materials are also discussed in (chapter 5 of) this report.

  17. 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.

  18. Ceramic and glass radioactive waste forms

    Energy Technology Data Exchange (ETDEWEB)

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

    1977-01-01

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

  19. 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.

  20. Mixed low-level waste form evaluation

    Energy Technology Data Exchange (ETDEWEB)

    Pohl, P.I.; Cheng, Wu-Ching; Wheeler, T.; Waters, R.D.

    1997-03-01

    A scoping level evaluation of polyethylene encapsulation and vitreous waste forms for safe storage of mixed low-level waste was performed. Maximum permissible radionuclide concentrations were estimated for 15 indicator radionuclides disposed of at the Hanford and Savannah River sites with respect to protection of the groundwater and inadvertent intruder pathways. Nominal performance improvements of polyethylene and glass waste forms relative to grout are reported. These improvements in maximum permissible radionuclide concentrations depend strongly on the radionuclide of concern and pathway. Recommendations for future research include improving the current understanding of the performance of polymer waste forms, particularly macroencapsulation. To provide context to these estimates, the concentrations of radionuclides in treated DOE waste should be compared with the results of this study to determine required performance.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2007-11-01

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

  2. Igneous Intrusion Impacts on Waste Packages and Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    P. Bernot

    2004-08-16

    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 model is based on conceptual models and includes an assessment of deleterious dynamic, thermal, hydrologic, and chemical impacts. This constitutes 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 SR and LA (BSC 2003a) and Total System Performance Assessment-License Application Methods and Approaches (BSC 2002a). The technical work plan is governed by the procedures of AP-SIII.10Q, Models. Any deviations from the technical work plan are documented in 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: (1) Impacts of magma intrusion on the components of engineered barrier system (e.g., drip shields and cladding) of emplacement drifts in Zone 1, and the fate of waste forms. (2) Impacts of conducting magma heat and diffusing magma gases on the drip shields, waste packages, and cladding in the Zone 2 emplacement drifts adjacent to the intruded drifts. (3) Impacts of intrusion on Zone 1 in-drift thermal and geochemical environments, including seepage hydrochemistry. The scope of this model only includes impacts to the components stated above, and does not include impacts to other engineered barrier system (EBS) components such as the invert and

  3. 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.

  4. Evaluation of extractants and chelating resins in polishing actinide-contaminated waste streams

    Energy Technology Data Exchange (ETDEWEB)

    Schreiber, S.B.; Dunn, S.L.; Yarbro, S.L.

    1991-06-01

    At the Los Alamos National Laboratory Plutonium Facility, anion exchange is used for recovering plutonium from nitric acid solutions. Although this approach recovers >99%, the trace amounts of plutonium and other actinides remaining in the effluent require additional processing. We are doing research to develop a secondary unit operation that can directly polish the effluent so that actinide levels are reduced to below the maximum allowed for facility discharge. We selected solvent extraction, the only unit operation that can meet the stringent process requirements imposed; several carbonyl and phosphoryl extractants were evaluated and their performance characterized. We also investigated various engineering approaches for solvent extraction; the most promising was a chelating resin loaded with extractant. Our research now focuses on the synthesis of malonamides, and our goal is to bond these extractants to a resin matrix. 7 refs., 12 figs., 1 tab.

  5. 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

  6. 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.

  7. 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.

  8. 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.

  9. 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

  10. Alternative Waste Forms for Electro-Chemical Salt Waste

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-10-28

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

  11. 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.

  12. Removing actinides using a chromatographic resin from High Activity Waste Solutions containing metallic impurities

    Energy Technology Data Exchange (ETDEWEB)

    Pialot, H

    2004-07-01

    At the Plutonium Recycling Facility of CEA Valduc, anion exchange is used for recovering plutonium from nitric acid solutions. Although this approach recovers more than 99,9 %, the trace amounts of actinides as americium remaining in the effluent require additional processing to reduce alpha activity under the maximum allowed for surface disposal. A new process has been developed to remove actinides from these effluents with a TRUspec resin. A pilot composed of an electrochemical reactor followed by a TRUSPEC column has been designed into a glove box. Laboratory scale studies and first results on the pilot have confirmed the interesting bibliography concerning this process. The reduction of iron is effective with a yield of 98-99% and no significant retention of metallic impurities has been observed during fixing time. Moreover, Pr and Ce used as surrogates for Pu and Am are totally recovered in the elution phases. Further work will be done to validate the previous results and to qualify the overall process with active solutions.

  13. Computational Chemistry for Nuclear Waste Characterization and Processing: Relativistic Quantum Chemistry of Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Harrison, Robert J.; Bernholdt, David E.; Bursten, Bruce E.; De Jong, Wibe A.; Dixon, David A.; Dyall, Kenneth G.; Ermler, Walter V.; Fann, George I.; Hay, P. J.; Ismail Buchner, Nina; Kendall, Ricky A.; Li, Jun; Marino, Maria M.; Marsden, Colin J.; Martin, Richard L.; Minkoff, Michael; Nichols, Jeffrey A.; Nieplocha, Jarek; Pitzer, Russell M.; Pratt, Lawrence R.; Schreckenbach, Hans Georg; Seth, Michael C.; Shepard, Ron; Stevens, Rick L.; Tilson, Jeffrey L.; Wagner, Albert F.; Wang, Qi; Windus, Theresa L.; Wong, Adrian; Zhang, Zhiyong

    2002-08-02

    In the course of the 3 years we have conducted calculations on molecular structures containing actinides, lanthanides, and other heavy elements. Our calculations were done at the relativistically-correct, all-electron, 4-component calculations (DHF, MP2, and CCSD(T)), using density functional theory (DFT) with relativistic effective core potentials (RECPs), and various other methodologies. We studied the ground- and excited state structures, energetics, vibrational frequencies, and NMR, excitation and ionization spectra. In addition a considerable amount of codes and methodologies have been developed during the GC3 period, enabling us to do the extensive research described in this final report, and providing researchers worldwide with new computational chemistry tools. In this section we will give a brief overview of our activities and accomplishments, grouped by each research institution. A more extensive overview can be found in the appendices containing the full yearly reports.

  14. 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

  15. 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.

  16. Inductively coupled plasma-mass spectrometry studies of the chemistry of fission products and actinides in high level wastes: lessons that can be applied to environmental measurements

    Energy Technology Data Exchange (ETDEWEB)

    Kinard, W.F. [Dept. of Chemistry, Coll. of Charleston, SC (United States); Bibler, N.E. [Westinghouse Savannah River Technology Center (SRTC), Westinghouse Savannah River Corp., Aiken, SC (United States); Coleman, C.J. [Westinghouse Savannah River Technology Center (SRTC), Westinghouse Savannah River Corp., Aiken, SC (United States); Wyrick, S.B. [Science Applications International, Gaithersburg, MD (United States)

    1994-12-31

    Actinide and fission product concentrations in HLW (high level wastes) from the Savannah River Site (SRS) in South Carolina and from Tank 101-SY at the Hanfrod Site in the state of Washington have been measured by inductively coupled plasma-mass spectrometry. Isotopic assignments based on fission yield predictions has enabled the analyses to be made without further separations other than the chemical processing used to separate waste streams. Isotopic patterns related to weapons reactor procuction are proposed as possible tracers for environmental measurements. (orig.)

  17. Development of the scientific concept of the phosphate methods for actinide-containing waste handling (pyrochemical fuel reprocessing)

    Energy Technology Data Exchange (ETDEWEB)

    Orlova, A.I.; Orlova, V.A. [Department of Chemistry, Nizhny Novgorod State University, 23, Gagarin Ave., Nizhny Novgorod, 603950 (Russian Federation); Skiba, O.V.; Bychkov, A.V.; Volkov, Yu.F.; Lukinykh, A.N.; Tomilin, S.V.; Lizin, A.A. [Federal State Unitary Enterprise State Scientific Center, Research Institute of Atomic Reactors, Dimitrovgrad, Ulyanovsk region, 433510 (Russian Federation)

    2008-07-01

    Full text of publication follows: The crystallochemical phosphate concept in question is developed successfully in the new pyro-electrochemical reprocessing technology of irradiated fuel in molten chlorides of alkaline elements at one of the leading scientific nuclear centers - Research Institute of Atomic Reactors. Irradiated fuel is dissolved in molten chlorides of alkaline elements by mean of treating by chlorine. Then uranium and plutonium dioxides are removed electrochemically. The melt, when used many times, is contaminated by the residual actinide and contains fission products and the so called 'process' elements. This melt is unacceptable for future use. Phosphate methods can be applied for the solution of the following tasks: a) reprocessing (purification) of molten chloride salt solvents; b) conversion of the spent chloride melts to the insoluble stable crystalline product for safe storage and disposal. Within the framework of task 'a' phosphate methods may be realized by the several ways: 1) phosphate concentrating of impurities and their extraction from molten chlorides into solid phase by mean of chemical precipitation, co-precipitation, ion exchange and other chemical interactions, 2) conversion of precipitated waste phosphates to stable crystalline phosphate powders or ceramics for safe storage and disposal. (authors)

  18. 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.

  19. Waste Form Features, Events, and Processes

    Energy Technology Data Exchange (ETDEWEB)

    R. Schreiner

    2004-10-27

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

  20. Bridging the Gap in the Chemical Thermodynamic Database for Nuclear Waste Repository: Studies of the Effect of Temperature on Actinide Complexation

    Energy Technology Data Exchange (ETDEWEB)

    Rao, Linfeng; Tian, Guoxin; Xia, Yuanxian; Friese, Judah I.; Zanonato, PierLuigi; Di Bernardo, Plinio

    2009-12-21

    Recent results of thermodynamic studies on the complexation of actinides (UO{sub 2}{sup 2+}, NpO{sub 2}{sup +} and Pu{sup 4+}) with F{sup -}, SO{sub 4}{sup 2-} and H{sub 2}PO{sub 4}{sup -}/HPO{sub 4}{sup 2-} at elevated temperatures are reviewed. The data indicate that, for all systems except the 1:1 complexation of Np(V) with HPO{sub 4}{sup 2-}, the complexation of actinides is enhanced by the increase in temperature. The enhancement is primarily due to the increase in the entropy term (T{Delta}S) that exceeds the increase in the enthalpy ({Delta}H) as the temperature is increased. These data bridge the gaps in the chemical thermodynamic database for nuclear waste repository where the temperature could remain significantly higher than 25 C for a long time after the closure of the repository.

  1. 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.

  2. DSNF and other waste form degradation abstraction

    Energy Technology Data Exchange (ETDEWEB)

    Thornton, Thomas A.

    2000-12-20

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

  3. 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.

  4. 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.

  5. Thin extractive membrane for monitoring actinides in aqueous streams

    Energy Technology Data Exchange (ETDEWEB)

    Chavan, Vivek [Radiochemistry Division, Trombay, Mumbai 400 085 (India); Paul, Sumana [Fuel Chemistry Division, Trombay, Mumbai 400 085 (India); Pandey, Ashok K., E-mail: ashokk@barc.gov.in [Radiochemistry Division, Trombay, Mumbai 400 085 (India); Kalsi, P.C.; Goswami, A. [Radiochemistry Division, Trombay, Mumbai 400 085 (India)

    2013-09-15

    Highlights: • Thin polymer inclusion membrane has been developed for selective actinide sorption. • Actinide sorption in membrane is dependent on acidity and oxidation states. • A scheme for selective preconcentration of target actinide has been developed. • Quantification of actinide in membrane is possible by SSNTD or α-spectrometry. • This membrane was used for assay of Pu in acidic waste and urine -- Abstract: 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 mol L{sup −1} HNO{sub 3}, U(VI) up to 0.5 mol L{sup −1} HNO{sub 3} and Pu(IV) from HNO{sub 3} concentration as high as 4 mol L{sup −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 ({sup 241}Am/{sup 239}Pu/{sup 233}U), respectively. Finally, the membranes were tested to quantify Pu in 4 mol L{sup −1} HNO{sub 3} solutions and synthetic urine samples.

  6. Multibarrier waste forms. Part I. Development

    Energy Technology Data Exchange (ETDEWEB)

    Rusin, J.M.; Lokken, R.O.; Lukacs, J.M.; Sump, K.R.; Browning, M.F.; McCarthy, G.J.

    1978-09-01

    The multibarrier concept produces a composite waste form with enhanced inertness through improvements in thermal stability, mechanical strength, and leachability by the use of coatings and metal matrices. This report describes research and development activities resulting in the demonstration of the multibarrier concept for nonradioactive simulated waste compositions. The multibarrier concept is to utilize up to three barriers to isolate radionuclides from the environment: a solid waste inner core, an impervious coating, and a metal matrix. Two inner core materials, sintered supercalcine and glass marbles, have been demonstrated. The coating barrier provides enhanced leach, impact, and oxidation resistance as well as thermal protection during encapsulation in the metal matrix. Py/Al/sub 2/O/sub 3/ coatings deposited by chemical vapor deposition (CVD) and glass coatings have been applied to supercalcine cores to improve inertness. The purpose of the metal matrix is to improve impact resistance, protect the inner core rom any adverse environments, provide radiation shielding, and increase thermal conductivity, yielding lower internal temperatures. The development of gravity sintering and vacuum casting techniques for matrix encapsulation are discussed. Four multibarrier products were demonstrated: (1) Glass marbles encapsulated in vacuum-cast Pb-10Sn; (2) uncoated, sintered supercalcine pellets encapsulated in vacuum-cast Al-12Si; (3) glass-coated, sintered supercalcine pellets encapsulated in vacuum-cast Al-12Si; and (4) PyC/Al/sub 2/O/sub 3/-coated supercalcine encapsulated in gravity-sintered Cu. 23 figs., 20 tables.

  7. 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.

  8. 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}.

  9. Demonstration of the UNEX Process for the Simultaneous Separation of Cesium, Strontium, and the Actinides from Actual INEEL Sodium-Bearing Waste

    Energy Technology Data Exchange (ETDEWEB)

    Law, Jack Douglas; Herbst, Ronald Scott; Todd, Terry Allen; Romanovskiy, V.; Smirnov, I.; Babain, V.; Zaitsev, B.; Esimantovskiy, V.

    1999-11-01

    A universal solvent extraction (UNEX) process for the simultaneous separation of cesium, strontium, and the actinides from actual radioactive acidic tank waste was demonstrated at the Idaho National Engineering and Environmental Laboratory. The waste solution used in the countercurrent flowsheet demonstration was obtained from tank WM-185. The UNEX process uses a tertiary solvent containing 0.08 M chlorinated cobalt dicarbollide, 0.5% polyethylene glycol-400 (PEG-400), and 0.02 M diphenyl-N,N-dibutylcarbamoyl phosphine oxide (Ph2Bu2CMPO) in a diluent consisting of phenyltrifluoromethyl sulfone (FS-13). The countercurrent flowsheet demonstration was performed in a shielded cell facility using 24 stages of 2-cm diameter centrifugal contactors. Removal efficiencies of 99.4%, 99.995%, and 99.96% were obtained for 137Cs, 90Sr, and total alpha, respectively. This is sufficient to reduce the activities of 137Cs, 90Sr, and actinides in the WM-185 waste to below NRC Class A LLW requirements. Flooding and/or precipitate formation were not observed during testing. Significant amounts of the Zr (87%), Ba (>99%), Pb (98.8%), Fe (8%), Ca (10%), Mo (32%), and K (28%) were also removed from the feed with the universal solvent extraction flowsheet. 99Tc, Al, Hg, and Na were essentially inextractable (<1% extracted).

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

    Energy Technology Data Exchange (ETDEWEB)

    Kinard, W.F. [College of Charleston, SC (United States). Dept. of Chemistry; Bibler, N.E.; Coleman, C.J.; Dewberry, R.A.; Boyce, W.T. [Westinghouse Savannah River Technology Center, Aiken, SC (United States); Wyrick, S.B. [Science Applications International, Gaithersburg, MD (United States)

    1995-12-31

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

  11. Waste form development for a DC arc furnace

    Energy Technology Data Exchange (ETDEWEB)

    Feng, X.; Bloomer, P.E.; Chantaraprachoom, N.; Gong, M.; Lamar, D.A.

    1996-09-01

    A laboratory crucible study was conducted to develop waste forms to treat nonradioactive simulated {sup 238}Pu heterogeneous debris waste from Savannah River, metal waste from the Idaho National Engineering Laboratory (INEL), and nominal waste also from INEL using DC arc melting. The preliminary results showed that the different waste form compositions had vastly different responses for each processing effect. The reducing condition of DC arc melting had no significant effects on the durability of some waste forms while it decreased the waste form durability from 300 to 700% for other waste forms, which resulted in the failure of some TCLP tests. The right formulations of waste can benefit from devitrification and showed an increase in durability by 40%. Some formulations showed no devitrification effects while others decreased durability by 200%. Increased waste loading also affected waste form behavior, decreasing durability for one waste, increasing durability by 240% for another, and showing no effect for the third waste. All of these responses to the processing and composition variations were dictated by the fundamental glass chemistry and can be adjusted to achieve maximal waste loading, acceptable durability, and desired processing characteristics if each waste formulation is designed for the result according to the glass chemistry.

  12. 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.

  13. Equilibrium Temperature Profiles within Fission Product Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Kaminski, Michael D. [Argonne National Lab. (ANL), Argonne, IL (United States)

    2016-10-01

    We studied waste form strategies for advanced fuel cycle schemes. Several options were considered for three waste streams with the following fission products: cesium and strontium, transition metals, and lanthanides. These three waste streams may be combined or disposed separately. The decay of several isotopes will generate heat that must be accommodated by the waste form, and this heat will affect the waste loadings. To help make an informed decision on the best option, we present computational data on the equilibrium temperature of glass waste forms containing a combination of these three streams.

  14. 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.

  15. Quantification of the Partitioning Ratio of Minor Actinide Surrogates between Zirconolite and Glass in Glass-Ceramic for Nuclear Waste Disposal.

    Science.gov (United States)

    Liao, Chang-Zhong; Liu, Chengshuai; Su, Minhua; Shih, Kaimin

    2017-08-21

    Zirconolite-based glass-ceramic is considered a promising wasteform for conditioning minor actinide-rich nuclear wastes. Recent studies on this wasteform have sought to enhance the partitioning ratio (PR) of minor actinides in zirconolite crystal. To optimize the PR in the SiO 2 -Al 2 O 3 -CaO-TiO 2 -ZrO 2 system, a novel conceptual approach, which can be derived from the chemical composition and quantity of zirconolite crystal in glass-ceramic, was introduced based on the results of Rietveld quantitative X-ray diffraction analysis and transmission electron microscopy energy dispersive X-ray spectroscopy. To verify this new conceptual approach, the influences of the crystallization temperature, the concentration of additives, and ionic radii on the PR of various surrogates (Ce, Nd, Gd, and Yb) in zirconolite were examined. The results reveal that the PR of Nd 3+ in zirconolite can be as high as 41%, but it decreases as the crystallization temperature increases. The quantities of all phases (including crystalline and amorphous) remained nearly constant when increasing the loading of Nd 2 O 3 in glass-ceramic products crystallized at 1050 °C for 2 h. Correspondingly, the PR of Nd 3+ decreases in a linear fashion with the loading contents of Nd 2 O 3 . The radius of ions also has a great influence on the PR, and an increase in the ionic radius leads to a decrease in the PR. This new approach will be an important tool to facilitate the exploration of a glass-ceramic matrix for the disposal of minor actinide-rich nuclear wastes.

  16. 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.

  17. PASSIVATION LAYER STABILITY OF A METALLIC ALLOY WASTE FORM

    Energy Technology Data Exchange (ETDEWEB)

    Williamson, M.; Mickalonis, J.; Fisher, D.; Sindelar, R.

    2010-08-16

    Alloy waste form development under the Waste Forms Campaign of the DOE-NE Fuel Cycle Research & Development program includes the process development and characterization of an alloy system to incorporate metal species from the waste streams generated during nuclear fuel recycling. This report describes the tests and results from the FY10 activities to further investigate an Fe-based waste form that uses 300-series stainless steel as the base alloy in an induction furnace melt process to incorporate the waste species from a closed nuclear fuel recycle separations scheme. This report is focused on the initial activities to investigate the formation of oxyhydroxide layer(s) that would be expected to develop on the Fe-based waste form as it corrodes under aqueous repository conditions. Corrosion tests were used to evaluate the stability of the layer(s) that can act as a passivation layer against further corrosion and would affect waste form durability in a disposal environment.

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

    Energy Technology Data Exchange (ETDEWEB)

    Jantzen, C

    2006-01-06

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

  19. Effluent Management Facility Evaporator Bottom-Waste Streams Formulation and Waste Form Qualification Testing

    Energy Technology Data Exchange (ETDEWEB)

    Saslow, Sarah A.; Um, Wooyong; Russell, Renee L.

    2017-08-02

    This report describes the results from grout formulation and cementitious waste form qualification testing performed by Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions, LLC (WRPS). These results are part of a screening test that investigates three grout formulations proposed for wide-range treatment of different waste stream compositions expected for the Hanford Effluent Management Facility (EMF) evaporator bottom waste. This work supports the technical development need for alternative disposition paths for the EMF evaporator bottom wastes and future direct feed low-activity waste (DFLAW) operations at the Hanford Site. High-priority activities included simulant production, grout formulation, and cementitious waste form qualification testing. The work contained within this report relates to waste form development and testing, and does not directly support the 2017 Integrated Disposal Facility (IDF) performance assessment (PA). However, this work contains valuable information for use in PA maintenance past FY 2017 and future waste form development efforts. The provided results and data should be used by (1) cementitious waste form scientists to further the understanding of cementitious leach behavior of contaminants of concern (COCs), (2) decision makers interested in off-site waste form disposal, and (3) the U.S. Department of Energy, their Hanford Site contractors and stakeholders as they assess the IDF PA program at the Hanford Site. The results reported help fill existing data gaps, support final selection of a cementitious waste form for the EMF evaporator bottom waste, and improve the technical defensibility of long-term waste form risk estimates.

  20. An experimental study on dissolution kinetics of paraffin waste form

    Energy Technology Data Exchange (ETDEWEB)

    Kim, J. Y.; Jung, C. H. [Seoul National Univ., Seoul (Korea, Republic of); Choi, H. J.; Kim, C. R. [KNETEC, Taejon (Korea, Republic of)

    1999-10-01

    Ninety-day's leaching test of paraffin waste form with boric acid, cobalt, strontium and cesium was performed. In case that the mixing weight ratio of waste form between boric acid and paraffin was 78/22, which had been adopted in the concentrate waste drying system(CWDS) of domestic nuclear power plants, the cumulative fraction leached(CFL) of boric acid was about 55% after ninety days and the CFLs of cobalt, strontium and cesium were almost same value of 63%. The compressive strengths of waste form before and after the leaching test exhibited 4.53 MPa (666 psi) and 1.38 MPa(203 psi), respectively. The CFL of paraffin waste form was well expressed by diffusion-controlled dissolution model such as Jander kinetics. The cross-sectional area of specimen after the test showed that this unreacted shrinking core model can be applied to the mechanistic analysis of paraffin waste form.

  1. 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

  2. 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.

  3. 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

  4. Cobalt bis(dicarbollide) ions with covalently bonded CMPO groups as selective extraction agents for lanthanide and actinide cations from highly acidic nuclear waste solutions

    Energy Technology Data Exchange (ETDEWEB)

    Gruner, B.; Plesek, J.; Baca, J. [Academy of Sciences of the Czech Republic, Institute of Inorganic Chemistry, Prague (Czech Republic); Cisarova, I. [Charles University, Dept. of Chemistry, Faculty of Natural Sciences, Prague (Czech Republic); Dozol, J.F.; Rouquette, H. [CEA Cadarache, Dept. d' Etudes des Dechets, DED/LCD, 13 - Saint Paul lez Durance (France); Vinas, C. [Institute of Material Sciences, CSIC, Bellaterra (Spain); Selucky, P.; Rais, J. [Nuclear Research Institute plc., Rez near Prague (Czech Republic)

    2002-10-01

    A new series of boron substituted cobalt bis(dicarbollide)(1-) ion (1) derivatives of the general formula [(8-CMPO-(CH{sub 2}-CH{sub 2}O){sub 2}-1,2-C{sub 2}B{sub 9}H{sub 10})(1',2'-C{sub 2}B{sub 9}H{sub 11})-3,3'-Co]{sup -} (CMPO = Ph{sub 2}P(O)-CH{sub 2}C(O)NR, R = C{sub 4}H{sub 9} (3b), -C{sub 12}H{sub 25} (4b), -CH{sub 2}-C{sub 6}H{sub 5} (5b)) was prepared by ring cleavage of the 8-dioxane-cobalt bis(dicarbollide) (2) bi-polar compound by the respective primary amines and by subsequent reaction of the resulting amino derivatives (3a-5a) with the nitrophenyl ester of diphenyl-phosphoryl-acetic acid. The compounds were synthesized with the aim to develop a new class of more efficient extraction agents for liquid/liquid extraction of polyvalent cations, i.e. lanthanides and actinides, from high-level activity nuclear waste. All compounds were characterized by a combination of {sup 11}B NMR, {sup 1}H high field NMR, Mass Spectrometry with Electro-spray and MALDI TOF ionisation, HPLC and other techniques. The molecular structure of the supramolecular Ln{sup 3+} complex of the anion 5b was determined by single crystal X-ray diffraction analysis. Crystallographic results proved that the Ln(m) atom is bonded to three functionalized cobalt bis(dicarbollide) anions in a charge compensated complex. The cation is tightly coordinated by six oxygen atoms of the CMPO terminal groups (two of each ligand) and by three water molecules completing the metal coordination number to 9. Atoms occupying the primary coordination sphere form a tri-capped trigonal prismatic arrangement. Very high liquid-liquid extraction efficiency of all anionic species was observed. Moreover, less polar toluene can be applied as an auxiliary solvent replacing the less environmentally friendly nitro- and chlorinated solvents used in the current dicarbollide liquid-liquid extraction process. The extraction coefficients are sufficiently high for possible technological applications. (authors)

  5. Waste forms technology and performance: final report

    National Research Council Canada - National Science Library

    Committee on Waste Forms Technology and Performance; National Research Council

    2011-01-01

    "The Department of Energy's Office of Environmental Management (DOE-EM) is responsible for cleaning up radioactive waste and environmental contamination resulting from five decades of nuclear weapons production and testing...

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1997-08-01

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

  7. 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

  8. Fundamental Chemistry of the Universal Extractant (UNEX) for the Simultaneous Separation of Major Radionuclides (Cesium, Strontium, Actinides, and Lanthanides) from Radioactive Wastes

    Energy Technology Data Exchange (ETDEWEB)

    Herbst, R. Scott; Peterman, Dean R.; Luther, Thomas A.; Garn, Troy G.; Tillotson, Richard D.; Babain, Vasily A.; Smirnov, Igor V.; Stoyanov, Evgenii S.

    2004-03-28

    4 Scientists at the INEEL and KRI collaboratively developed and validated the concept of a Universal Extractant (UNEX) for simultaneously removing the major radionuclides (Cs, Sr, actinides and lanthanides) from acidic radioactive waste in a single solvent extraction process. The UNEX solvent incorporates three active extractants: chlorinated cobalt dicarbollide, polyethylene glycol and a carbamoylmethylphosphine oxide derivative, dissolved in a suitable organic diluent to simultaneously extract target radionuclides. The process chemistry is unique, but complicated, since the extractants operate synergistically to extract the radionuclides. Results indicate that water dissolved in the organic phase dramatically impacts the process chemistry. In order to investigate this phenomenon, we have varied the amount of water dissolved in the organic phase by using several different organic diluents. The results of 137Cs and 89Sr batch distribution studies for the different organic diluents will be presented. These data and data from other spectroscopic techniques will be used to elucidate the details of the extraction mechanism.

  9. DSNF AND OTHER WASTE FORM DEGRADATION ABSTRACTION

    Energy Technology Data Exchange (ETDEWEB)

    J. CUNNANE

    2004-11-19

    Several hundred distinct types of DOE-owned spent nuclear fuel (DSNF) may potentially be disposed in the Yucca Mountain repository. These fuel types represent many more types than can be viably individually examined for their effect on the Total System Performance Assessment for the License Application (TSPA-LA). Additionally, for most of these fuel types, there is no known direct experimental test data for the degradation and dissolution of the waste form in repository groundwaters. The approach used in the TSPA-LA model is, therefore, to assess available information on each of 11 groups of DSNF, and to identify a model that can be used in the TSPA-LA model without differentiating between individual codisposal waste packages containing different DSNF types. The purpose of this report is to examine the available data and information concerning the dissolution kinetics of DSNF matrices for the purpose of abstracting a degradation model suitable for use in describing degradation of the DSNF inventory in the Total System Performance Assessment for the License Application. The data and information and associated degradation models were examined for the following types of DSNF: Group 1--Naval spent nuclear fuel; Group 2--Plutonium/uranium alloy (Fermi 1 SNF); Group 3--Plutonium/uranium carbide (Fast Flux Test Facility-Test Fuel Assembly SNF); Group 4--Mixed oxide and plutonium oxide (Fast Flux Test Facility-Demonstration Fuel Assembly/Fast Flux Test Facility-Test Demonstration Fuel Assembly SNF); Group 5--Thorium/uranium carbide (Fort St. Vrain SNF); Group 6--Thorium/uranium oxide (Shippingport light water breeder reactor SNF); Group 7--Uranium metal (N Reactor SNF); Group 8--Uranium oxide (Three Mile Island-2 core debris); Group 9--Aluminum-based SNF (Foreign Research Reactor SNF); Group 10--Miscellaneous Fuel; and Group 11--Uranium-zirconium hydride (Training Research Isotopes-General Atomics SNF). The analyses contained in this document provide an &apos

  10. Ni and Cr addition to alloy waste forms to reduce radionuclide environmental releases

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-10-11

    Reference alloy waste forms (RAW) were fabricated and underwent hybrid corrosion/immersion testing to parameterize the ANL analytical oxidative-dissolution model to enable the calculation of fractional release rates and to determine the effectiveness of Ni and Cr trim additions in reducing release rates of radionuclide surrogates. Figure 1 shows the prototypical multiphase microstructure of the alloys with each phase type contributing about equally to the exposed surface area. The waste forms tested at SRNL were variations of the RAW-6 formulation that uses HT9 as the main alloy component, and are meant to enable evaluation of the impact of Ni and Cr trim additions on the release rates of actinides and Tc-99. The test solutions were deaerated alkaline and acidic brines, ranging in pH 3 to pH 10, representing potential repositories with those conditions. The testing approach consisted of 4 major steps; 1) bare surface corrosion measurements at pH values of 3, 5, 8, and 10, 2) hybrid potentiostatic hold/exposure measurements at pH 3, 3) measurement of radionuclide concentrations and relations to anodic current from potentiostatic holds, and 4) identification of corroding phases using SEM/EDS of electrodes.

  11. 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.

  12. 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.

  13. 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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2000-02-01

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

  15. 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.).

  16. Viscosity-based high temperature waste form compositions

    Energy Technology Data Exchange (ETDEWEB)

    Reimann, G.A.

    1994-12-31

    High-temperature waste forms such as iron-enriched basalt are proposed to immobilize and stabilize a variety of low-level wastes stored at the Idaho National Engineering Laboratory. The combination of waste and soil anticipated for the waste form results in high SiO{sub 2} + Al{sub 2}O{sub 3} producing a viscous melt in an arc furnace. Adding a flux such as CaO to adjust the basicity ratio (the molar ratio of basic to acid oxides) enables tapping the furnace without resorting to extreme temperatures, but adds to the waste volume. Improved characterization of wastes will permit adjusting the basicity ratio to between 0.7 and 1.0 by blending of wastes and/or changing the waste-soil ratio. This minimizes waste form volume. Also, lower pouring temperatures will decrease electrode and refractory attrition, reduce vaporization from the melt, and, with suitable flux, facilitate crystallization. Results of laboratory tests were favorable and pilot-scale melts are planned; however, samples have not yet been subjected to leach testing.

  17. Updated Liquid Secondary Waste Grout Formulation and Preliminary Waste Form Qualification

    Energy Technology Data Exchange (ETDEWEB)

    Saslow, Sarah A. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Um, Wooyong [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Russell, Renee L. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Wang, Guohui [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Asmussen, Robert M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Sahajpal, Rahul [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2017-07-01

    This report describes the results from liquid secondary waste grout (LSWG) formulation and cementitious waste form qualification tests performed by Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions, LLC (WRPS). New formulations for preparing a cementitious waste form from a high-sulfate liquid secondary waste stream simulant, developed for Effluent Management Facility (EMF) process condensates merged with low activity waste (LAW) caustic scrubber, and the release of key constituents (e.g. 99Tc and 129I) from these monoliths were evaluated. This work supports a technology development program to address the technology needs for Hanford Site Effluent Treatment Facility (ETF) liquid secondary waste (LSW) solidification and supports future Direct Feed Low-Activity Waste (DFLAW) operations. High-priority activities included simulant development, LSWG formulation, and waste form qualification. The work contained within this report relates to waste form development and testing and does not directly support the 2017 integrated disposal facility (IDF) performance assessment (PA). However, this work contains valuable information for use in PA maintenance past FY17, and for future waste form development efforts. The provided data should be used by (i) cementitious waste form scientists to further understanding of cementitious dissolution behavior, (ii) IDF PA modelers who use quantified constituent leachability, effective diffusivity, and partitioning coefficients to advance PA modeling efforts, and (iii) the U.S. Department of Energy (DOE) contractors and decision makers as they assess the IDF PA program. The results obtained help fill existing data gaps, support final selection of a LSWG waste form, and improve the technical defensibility of long-term waste form performance estimates.

  18. Cement waste-form development for ion-exchange resins at the Rocky Flats Plant

    Energy Technology Data Exchange (ETDEWEB)

    Veazey, G.W. [Los Alamos National Labs., NM (United States); Ames, R.L. [Rocky Flats Environmental Technology Site, Golden, CO (United States)

    1997-03-01

    This report describes the development of a cement waste form to stabilize ion-exchange resins at Rocky Flats Environmental Technology Site (RFETS). These resins have an elevated potential for ignition due to inadequate wetness and contact with nitrates. The work focused on the preparation and performance evaluation of several Portland cement/resin formulations. The performance standards were chosen to address Waste Isolation Pilot Plant and Environmental Protection Agency Resource Conservation and Recovery Act requirements, compatibility with Rocky Flats equipment, and throughput efficiency. The work was performed with surrogate gel-type Dowex cation- and anion-exchange resins chosen to be representative of the resin inventory at RFETS. Work was initiated with nonactinide resins to establish formulation ranges that would meet performance standards. Results were then verified and refined with actinide-containing resins. The final recommended formulation that passed all performance standards was determined to be a cement/water/resin (C/W/R) wt % ratio of 63/27/10 at a pH of 9 to 12. The recommendations include the acceptable compositional ranges for each component of the C/W/R ratio. Also included in this report are a recommended procedure, an equipment list, and observations/suggestions for implementation at RFETS. In addition, information is included that explains why denitration of the resin is unnecessary for stabilizing its ignitability potential.

  19. Method for forming microspheres for encapsulation of nuclear waste

    Science.gov (United States)

    Angelini, Peter; Caputo, Anthony J.; Hutchens, Richard E.; Lackey, Walter J.; Stinton, David P.

    1984-01-01

    Microspheres for nuclear waste storage are formed by gelling droplets containing the waste in a gelation fluid, transferring the gelled droplets to a furnace without the washing step previously used, and heating the unwashed gelled droplets in the furnace under temperature or humidity conditions that result in a substantially linear rate of removal of volatile components therefrom.

  20. 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.

  1. LLNL SFA OBER SBR FY17 Program Management and Performance Report: Subsurface Biogeochemistry of Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Kersting, Annie B. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

    2017-06-23

    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 anthropogenic plutonium (Pu) has accumulated 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.

  2. 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.

  3. Characteristics of metal waste forms containing technetium and uranium

    Energy Technology Data Exchange (ETDEWEB)

    Fortner, J.A.; Kropf, A.J.; Ebert, W.L. [Argonne National Laboratory, Argonne, IL 60439 (United States)

    2013-07-01

    2 prototype alloys: RAW-1(Tc) and RAW-2(UTc) suitable for a wide range of waste stream compositions are being evaluated to support development of a waste form degradation model that can be used to calculate radionuclide source terms for a range of waste form compositions and disposal environments. Tests and analyses to support formulation of waste forms and development of the degradation model include detailed characterizations of the constituent phases using SEM/EDS and TEM, electrochemical tests to quantify the oxidation behavior and kinetics of the individual and coupled phases under a wide range of environmental conditions, and corrosion tests to measure the gross release kinetics of radionuclides under aggressive test conditions.

  4. Low-level radioactive waste form qualification testing

    Energy Technology Data Exchange (ETDEWEB)

    Sohal, M.S.; Akers, D.W.

    1998-06-01

    This report summarizes activities that have already been completed as well as yet to be performed by the Idaho National Engineering and Environmental Laboratory (INEEL) to develop a plan to quantify the behavior of radioactive low-level waste forms. It briefly describes the status of various tasks, including DOE approval of the proposed work, several regulatory and environmental related documents, tests to qualify the waste form, preliminary schedule, and approximate cost. It is anticipated that INEEL and Brookhaven National Laboratory will perform the majority of the tests. For some tests, services of other testing organizations may be used. It should take approximately nine months to provide the final report on the results of tests on a waste form prepared for qualification. It is anticipated that the overall cost of the waste quantifying service is approximately $150,000. The following tests are planned: compression, thermal cycling, irradiation, biodegradation, leaching, immersion, free-standing liquid tests, and full-scale testing.

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

    Science.gov (United States)

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

    2014-05-01

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

  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. Consolidated waste forms: glass marbles and ceramic pellets

    Energy Technology Data Exchange (ETDEWEB)

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

    1982-05-01

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

  8. 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)

  9. Actinide AMS at DREAMS

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-07-01

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

  10. 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.

  11. 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.

  12. 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.

  13. Institute of Energy and Climate Research IEK-6. Nuclear Waste Management report 2011/2012. Material science for nuclear waste management

    Energy Technology Data Exchange (ETDEWEB)

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

    2013-07-01

    The nuclear waste management section of the Institute of Energy and Climate Research IEK-6 in Juelich is focused on research on radiochemistry aspects/materials science relevant for the long-term safety of nuclear waste storage and disposal. Studies on innovative waste management strategies include partitioning o actinides and the development of ceramic waste forms. Structural research is covering solid state chemistry, crystallography and computational science to model actinide containing compounds. With respect to waste management concepts nondestructive essay techniques, waste treatment procedures and product quality control strategies were developed.

  14. 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.

  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. 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

  17. 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.

  18. Getters for improved technetium containment in cementitious waste forms.

    Science.gov (United States)

    Asmussen, R Matthew; Pearce, Carolyn I; Miller, Brian W; Lawter, Amanda R; Neeway, James J; Lukens, Wayne W; Bowden, Mark E; Miller, Micah A; Buck, Edgar C; Serne, R Jeffery; Qafoku, Nikolla P

    2018-01-05

    A cementitious waste form, Cast Stone, is a possible candidate technology for the immobilization of low activity nuclear waste (LAW) at the Hanford site. This work focuses on the addition of getter materials to Cast Stone that can sequester Tc from the LAW, and in turn, lower Tc release from the Cast Stone. Two getters which produce different products upon sequestering Tc from LAW were tested: Sn(II) apatite (Sn-A) that removes Tc as a Tc(IV)-oxide and potassium metal sulfide (KMS-2) that removes Tc as a Tc(IV)-sulfide species, allowing for a comparison of stability of the form of Tc upon entering the waste form. The Cast Stone with KMS-2 getter had the best performance with addition equivalent to ∼0.08wt% of the total waste form mass. The observed diffusion (Dobs) of Tc decreased from 4.6±0.2×10(-12)cm(2)/s for Cast Stone that did not contain a getter to 5.4±0.4×10(-13)cm(2)/s for KMS-2 containing Cast Stone. It was found that Tc-sulfide species are more stable against re-oxidation within getter containing Cast Stone compared with Tc-oxide and is the origin of the decrease in Tc Dobs when using the KMS-2. Copyright © 2017 Elsevier B.V. All rights reserved.

  19. 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.

  20. 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.

  1. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Kalb, P.D.; Heiser, J.H. III; Colombo, P.

    1991-07-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-08-01

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

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

    Science.gov (United States)

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

    2012-09-11

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

  5. 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.

  6. Material Recover and Waste Form Development--2016 Accomplishments

    Energy Technology Data Exchange (ETDEWEB)

    Todd, Terry A. [Idaho National Lab. (INL), Idaho Falls, ID (United States); Vienna, John [Idaho National Lab. (INL), Idaho Falls, ID (United States); Paviet, Patricia [Idaho National Lab. (INL), Idaho Falls, ID (United States)

    2016-12-01

    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). This MRWFD accomplishments report summarizes the results of the research and development (R&D) efforts performed within MRWFD in Fiscal Year (FY) 2016. Each section of the report contains an overview of the activities, results, technical point of contact, applicable references, and documents produced during the FY. This report briefly outlines campaign management and integration activities but primarily focuses on the many technical accomplishments of FY 2016. The campaign continued to use an engineering-driven, science-based approach to maintain relevance and focus.

  7. 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.

  8. 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.

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

  10. PREPARATION OF ACTINIDE-ALUMINUM ALLOYS

    Science.gov (United States)

    Moore, R.H.

    1962-09-01

    BS>A process is given for preparing alloys of aluminum with plutonium, uranium, and/or thorium by chlorinating actinide oxide dissolved in molten alkali metal chloride with hydrochloric acid, chlorine, and/or phosgene, adding aluminum metal, and passing air and/or water vapor through the mass. Actinide metal is formed and alloyed with the aluminum. After cooling to solidification, the alloy is separated from the salt. (AEC)

  11. 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.

  12. 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.

  13. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Tumurugoti, Priyatham; Sundaram, S.K.; Misture, Scott T. [Kazuo Inamori School of Engineering, The New York State College of Ceramics, Alfred University, Alfred, NY, 14802 (United States); Marra, James C. [Savannah River National Laboratory, Aiken, SC, 29808 (United States); Amoroso, Jake, E-mail: jake.amoroso@srs.gov [Savannah River National Laboratory, Aiken, SC, 29808 (United States)

    2016-05-15

    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 TiO{sub 2.} - Highlights: • Crystallization behavior during melt processing multiphase ceramics was studied. • Phase evolution order upon cooling was hollandite → perovskite → zirconolite → TiO{sub 2}. • Hollandite phases co-exists with a liquid phase at temperatures >1500 °C. • Zirconolite crystallization is complex and involves intermediate phases.

  15. Fundamental Science-Based Simulation of Nuclear Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-10-04

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

  16. 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

  17. Actinide cation-cation complexes

    Energy Technology Data Exchange (ETDEWEB)

    Stoyer, Nancy Jane [Univ. of California, Berkeley, CA (United States)

    1994-12-01

    The +5 oxidation state of U, Np, Pu, and Am is a linear dioxo cation (AnO2+) with a formal charge of +1. These cations form complexes with a variety of other cations, including actinide cations. Other oxidation states of actinides do not form these cation-cation complexes with any cation other than AnO2+; therefore, cation-cation complexes indicate something unique about AnO2+ cations compared to actinide cations in general. The first cation-cation complex, NpO2+•UO22+, was reported by Sullivan, Hindman, and Zielen in 1961. Of the four actinides that form AnO2+ species, the cation-cation complexes of NpO2+ have been studied most extensively while the other actinides have not. The only PuO2+ cation-cation complexes that have been studied are with Fe3+ and Cr3+ and neither one has had its equilibrium constant measured. Actinides have small molar absorptivities and cation-cation complexes have small equilibrium constants; therefore, to overcome these obstacles a sensitive technique is required. Spectroscopic techniques are used most often to study cation-cation complexes. Laser-Induced Photacoustic Spectroscopy equilibrium constants for the complexes NpO2+•UO22+, NpO2+•Th4+, PuO2+•UO22+, and PuO2+•Th4+ at an ionic strength of 6 M using LIPAS are 2.4 ± 0.2, 1.8 ± 0.9, 2.2 ± 1.5, and ~0.8 M-1.

  18. 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)

  19. 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.

  20. 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.

  1. Separation of trivalent actinides and lanthanides from simulated high-level waste using cobalt bis(dicarbollide) ion derivate substituted with diphenyl-N-tert.octyl-carbamoylmethylphosphine oxide

    Czech Academy of Sciences Publication Activity Database

    Selucký, P.; Lučaníková, M.; Grüner, Bohumír

    2012-01-01

    Roč. 100, č. 3 (2012), s. 179-183 ISSN 0033-8230 R&D Projects: GA MŠk LC523; GA ČR GA104/09/0668 Institutional research plan: CEZ:AV0Z40320502 Keywords : dicarbollide * CMPO * liquid-liquid extraction * actinides * lanthanides Subject RIV: CA - Inorganic Chemistry Impact factor: 1.373, year: 2012

  2. 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.

  3. Thermodynamic Properties of Actinides and Actinide Compounds

    Science.gov (United States)

    Konings, Rudy J. M.; Morss, Lester R.; Fuger, Jean

    The necessity of obtaining accurate thermodynamic quantities for the actinide elements and their compounds was recognized at the outset of the Manhattan Project, when a dedicated team of scientists and engineers initiated the program to exploit nuclear energy for military purposes. Since the end of World War II, both fundamental and applied objectives have motivated a great deal of further study of actinide thermodynamics. This chapter brings together many research papers and critical reviews on this subject. It also seeks to assess, to systematize, and to predict important properties of the actinide elements, ions, and compounds, especially for species in which there is significant interest and for which there is an experimental basis for the prediction.

  4. 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.

  5. 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.

  6. Research in actinide chemistry. Progress report, 1990--1993

    Energy Technology Data Exchange (ETDEWEB)

    Choppin, G.R.

    1993-04-01

    This research studies the behavior of the actinide elements in aqueous solution. The high radioactivity of the transuranium actinides limits the concentrations which can be studied and, consequently, limits the experimental techniques. However, oxidation state analogs (trivalent lanthanides, tetravalent thorium, and hexavalent uranium) do not suffer from these limitations. Behavior of actinides in the environment are a major USDOE concern, whether in connection with long-term releases from a repository, releases from stored defense wastes or accidental releases in reprocessing, etc. Principal goal of our research was expand the thermodynamic data base on complexation of actinides by natural ligands (e.g., OH{sup {minus}}, CO{sub 3}{sup 2{minus}}, PO{sub 4}{sup 3{minus}}, humates). The research undertakes fundamental studies of actinide complexes which can increase understanding of the environmental behavior of these elements.

  7. Stability of High-Level Radioactive Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Besmann, T.M.

    2001-06-22

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

  8. 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.

  9. Radiation damage of hollandite in multiphase ceramic waste forms

    Science.gov (United States)

    Clark, Braeden M.; Tumurgoti, Priyatham; Sundaram, S. K.; Amoroso, Jake W.; Marra, James C.; Shutthanandan, Vaithiyalingam; Tang, Ming

    2017-10-01

    Radiation damage was simulated in multiphase titanate-based ceramic waste forms using an ion accelerator to generate high energy alpha particles (He+) and an ion implanter to generate 7 MeV gold (Au3+) particles. X-ray diffraction and transmission electron microscopy were used to characterize the damaged surfaces and nearby regions. Simulated multiphase ceramic waste forms were prepared using two processing methods: spark plasma sintering and melt-processing. Both processing methods produced ceramics with similar phase assemblages consisting of hollandite-, zirconolite/pyrochlore-, and perovskite-type phases. The measured heavy ion (Au3+) penetration depth was less in spark plasma sintered samples than in melt-processed samples. Structural breakdown of the hollandite phase occurred under He+ irradiation indicated by the presence of x-ray diffraction peaks belonging to TiO2, BaTiO5, and other hollandite related phases (Ba2Ti9O20). The composition of the constituent hollandite phase affected the extent of damage induced by Au3+ ions.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1978-09-01

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

  11. Candidate waste forms for immobilisation of waste chloride salt from pyroprocessing of spent nuclear fuel

    Science.gov (United States)

    Vance, E. R.; Davis, J.; Olufson, K.; Chironi, I.; Karatchevtseva, I.; Farnan, I.

    2012-01-01

    Sodalite/glass bodies prepared by hot isostatic pressing (HIPing) at ˜850 °C/100 MPa are candidates for immobilising fission product-bearing waste KCl-LiCl pyroprocessing salts. To study the capacity of sodalite to structurally incorporate such pyroprocessing salts, K, Li, Cs, Sr, Ba and La were individually targeted for substitution in a Na site in sodalite (Na vacancies targeted as charge compensators for alkaline and rare earths) and studied by X-ray diffraction and scanning electron microscopy after sintering in the range of 800-1000 °C. K and Li appeared to enter the sodalite, but Cs, Sr and Ba formed aluminosilicate phases and La formed an oxyapatite phase. However these non-sodalite phases have reasonable resistance to water leaching. Pure chlorapatite gives superior leach resistance to sodalite, and alkalis, alkaline and rare earth ions are generally known to enter chlorapatite, but attempts to incorporate simulated waste salt formulations into HIPed chlorapatite-based preparations or to substitute Cs alone into the structure of Ca-based chlorapatite were not successful on the basis of scanning electron microscopy. The materials exhibited severe water leachability, mainly in regard to Cs release. Attempts to substitute Cs into Ba- and Sr-based chlorapatites also did not look encouraging. Consequently the use of apatite alone to retain fission product-bearing waste pyroprocessing salts from electrolytic nuclear fuel reprocessing is problematical, but chlorapatite glass-ceramics may be feasible, albeit with reduced waste loadings. Spodiosite, Ca 2(PO 4)Cl, does not appear to be suitable for incorporation of Cl-bearing waste containing fission products.

  12. Improved Consolidation Process for Producing Ceramic Waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Hash, Harry C.; Hash, Mark C.

    1998-07-24

    A process for the consolidation and containment of solid or semisolid hazardous waste, which process comprises closing an end of a circular hollow cylinder, filling the cylinder with the hazardous waste, and then cold working the cylinder to reduce its diameter while simultaneously compacting the waste. The open end of the cylinder can be sealed prior to or after the cold working process. The preferred method of cold working is to draw the sealed cylinder containing the hazardous waste through a plurality of dies to simultaneously reduce the diameter of the tube while compacting the waste. This process provides a quick continuous process for consolidating hazardous waste, including radioactive waste.

  13. Separations and Actinide Science -- 2005 Roadmap

    Energy Technology Data Exchange (ETDEWEB)

    2005-09-01

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

  14. 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.

  15. Formation of actinides in irradiated HTGR fuel elements

    Energy Technology Data Exchange (ETDEWEB)

    dos Santos, A. M.

    1976-03-15

    Actinide nuclide concentrations of 11 spent AVR fuel elements were determined experimentally. The burnup of the spheres varied in the range between 10% and 100% fifa, the Th : U ratio was 5 : 1. The separation procedures for an actinide isolation were tested with highly irradiated ThO/sub 2/. Separation and decontamination factors are presented. Build-up of /sup 232/U was discussed. The AVR breeding rate was ascertained to be 0.5. The hazard potential of high activity waste was calculated. Actinide recovery factors were proposed in order to reduce the hazard potential of the waste by an actinide removal under consideration of the reprocessing technology which is available presently.

  16. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2001-12-01

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

  18. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-08-01

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

  20. 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.

  1. 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.

  2. 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.

  3. 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. Copyright © 2014 Elsevier B.V. All rights reserved.

  4. 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.

  5. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Singh, D.; Wagh, A.S.; Cunnane, J.; Sutaria, M.; Kurokawa, S. [Argonne National Lab., IL (United States); Mayberry, J. [Science Applications International Corp., Idaho Falls, ID (United States)

    1994-12-31

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

  7. 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

  8. 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

  9. 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...

  10. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1996-09-01

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

  12. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1981-07-01

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

  14. 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.

  15. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    McGrail, B. Peter; Icenhower, Jonathan P.; Martin, Paul F.; Schaef, Herbert T.; O' Hara, Matthew J.; Rodriguez, Eugenio; Steele, Jackie L.

    2001-02-01

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

  17. The chemistry of the actinide elements, Volume II

    Energy Technology Data Exchange (ETDEWEB)

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

    1986-01-01

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

  18. Chemistry of the actinide elements. Vol. 1, 2nd Ed

    Energy Technology Data Exchange (ETDEWEB)

    Katz, J.J.; Morss, L.R.; Seaborg, L.R. (eds.)

    1986-01-01

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

  19. The chemistry of the actinide elements. Volume I

    Energy Technology Data Exchange (ETDEWEB)

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

    1986-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1988-09-01

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

  1. 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).

  2. 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).

  3. 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.

  4. Tellurite glass as a waste form for mixed alkali-chloride waste streams: Candidate materials selection and initial testing

    Energy Technology Data Exchange (ETDEWEB)

    Riley, Brian J., E-mail: brian.riley@pnnl.gov [Pacific Northwest National Laboratory, Richland, WA 99352 (United States); Rieck, Bennett T. [Washington State University, Pullman, WA 99164 (United States); McCloy, John S.; Crum, Jarrod V. [Pacific Northwest National Laboratory, Richland, WA 99352 (United States); Sundaram, S.K. [Alfred University, Alfred, NY 14802 (United States); Vienna, John D. [Pacific Northwest National Laboratory, Richland, WA 99352 (United States)

    2012-05-15

    Highlights: Black-Right-Pointing-Pointer We provide the first standardized chemical durability test on tellurite glasses. Black-Right-Pointing-Pointer The glasses we studied showed a wide variety of chemical durability. Black-Right-Pointing-Pointer The best-performing glass showed good halide retention following melting and durability testing. Black-Right-Pointing-Pointer These glasses have very high densities resulting in high volumetric waste loading ability. - Abstract: Tellurite glasses have historically been shown to host large concentrations of halides. They are here considered for the first time as a waste form for immobilizing chloride wastes, such as may be generated in the proposed molten alkali salt electrochemical separations step in nuclear fuel reprocessing. Key properties of several tellurite glasses are determined to assess acceptability as a chloride waste form. TeO{sub 2} glasses with other oxides (PbO, Al{sub 2}O{sub 3} + B{sub 2}O{sub 3}, WO{sub 3}, P{sub 2}O{sub 5}, or ZnO) were fabricated with and without 10 mass% of a simulated (non-radioactive) mixed alkali, alkaline-earth, and rare earth chloride waste. Measured chemical durability is compared for the glasses, as determined by the product consistency test (PCT), a common standardized chemical durability test often used to validate borosilicate glass waste forms. The glass with the most promise as a waste form is the TeO{sub 2}-PbO system, as it offers good halide retention, a low sodium release (by PCT) comparable with high-level waste silicate glass waste forms, and a high storage density.

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

    Energy Technology Data Exchange (ETDEWEB)

    Williams, Benjamin D., E-mail: Benjamin.Williams@pnnl.gov [Pacific Northwest National Laboratory, PO Box 999, MSIN P7-54, Richland, WA 99352 (United States); Neeway, James J., E-mail: James.Neeway@pnnl.gov [Pacific Northwest National Laboratory, PO Box 999, MSIN P7-54, Richland, WA 99352 (United States); Snyder, Michelle M.V., E-mail: Michelle.ValentaSnyder@pnnl.gov [Pacific Northwest National Laboratory, PO Box 999, MSIN P7-54, Richland, WA 99352 (United States); Bowden, Mark E., E-mail: Mark.Bowden@pnnl.gov [Pacific Northwest National Laboratory, PO Box 999, MSIN P7-54, Richland, WA 99352 (United States); Amonette, James E., E-mail: Jim.Amonette@pnnl.gov [Pacific Northwest National Laboratory, PO Box 999, MSIN P7-54, Richland, WA 99352 (United States); Arey, Bruce W., E-mail: Bruce.Arey@pnnl.gov [Pacific Northwest National Laboratory, PO Box 999, MSIN P7-54, Richland, WA 99352 (United States); Pierce, Eric M., E-mail: pierceem@ornl.gov [Oak Ridge National Laboratory, PO Box 2008, MS-6035, Room 372, Oak Ridge, TN 37831 (United States); Brown, Christopher F., E-mail: Christopher.Brown@pnnl.gov [Pacific Northwest National Laboratory, PO Box 999, MSIN P7-54, Richland, WA 99352 (United States); Qafoku, Nikolla P., E-mail: Nik.Qafoku@pnnl.gov [Pacific Northwest National Laboratory, PO Box 999, MSIN P7-54, Richland, WA 99352 (United States)

    2016-05-15

    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. - Highlights: • Simulated Hanford waste was treated by the Fluidized Bed Steam Reformer (FBSR) process. • The FBSR granular product was encapsulated in a geopolymer monolith. • Leach tests were performed to examine waste form performance. • XRD revealed the structure of a previously unreported sodium aluminosilicate phase. • Monolithing of granular waste forms may lead to a reduction in crystallinity.

  6. Glass binder development for a glass-bonded sodalite ceramic waste form

    Science.gov (United States)

    Riley, Brian J.; Vienna, John D.; Frank, Steven M.; Kroll, Jared O.; Peterson, Jacob A.; Canfield, Nathan L.; Zhu, Zihua; Zhang, Jiandong; Kruska, Karen; Schreiber, Daniel K.; Crum, Jarrod V.

    2017-06-01

    This paper discusses work to develop Na2O-B2O3-SiO2 glass binders for immobilizing LiCl-KCl eutectic salt waste in a glass-bonded sodalite waste form following electrochemical reprocessing of used metallic nuclear fuel. Here, five new glasses with ∼20 mass% Na2O were designed to generate waste forms with high sodalite. The glasses were then used to produce ceramic waste forms with a surrogate salt waste. The waste forms made using these new glasses were formulated to generate more sodalite than those made with previous baseline glasses for this type of waste. The coefficients of thermal expansion for the glass phase in the glass-bonded sodalite waste forms made with the new binder glasses were closer to the sodalite phase in the critical temperature region near and below the glass transition temperature than previous binder glasses used. These improvements should result in lower probability of cracking in the full-scale monolithic ceramic waste form, leading to better long-term chemical durability.

  7. 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.

  8. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Cassayre, L., E-mail: cassayre@chimie.ups-tlse.fr [Laboratoire de Genie Chimique (LGC), Departement Procedes Electrochimiques, CNRS-UMR 5503, Universite de Toulouse III - Paul Sabatier, 31062 Toulouse (France); Soucek, P.; Mendes, E.; Malmbeck, R.; Nourry, C.; Eloirdi, R.; Glatz, J.-P. [European Commission, JRC, Institute for Transuranium Elements, Postfach 2340, 76125 Karlsruhe (Germany)

    2011-07-01

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

  10. 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.

  11. 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

  12. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Werry, E.V.; Gates, T.E.; Cabbage, K.S.; Eklund, J.D.

    1988-04-01

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

  14. Hanford Site Composite Analysis Technical Approach Description: Waste Form Release.

    Energy Technology Data Exchange (ETDEWEB)

    Hardie, S. [CH2M HILL Plateau Remediation Company, Richland, WA (United States); Paris, B. [CH2M HILL Plateau Remediation Company, Richland, WA (United States); Apted, M. [CH2M HILL Plateau Remediation Company, Richland, WA (United States)

    2017-09-14

    The U.S. Department of Energy (DOE) in DOE O 435.1 Chg. 1, Radioactive Waste Management, requires the preparation and maintenance of a composite analysis (CA). The primary purpose of the CA is to provide a reasonable expectation that the primary public dose limit is not likely to be exceeded by multiple source terms that may significantly interact with plumes originating at a low-level waste disposal facility. The CA is used to facilitate planning and land use decisions that help assure disposal facility authorization will not result in long-term compliance problems; or, to determine management alternatives, corrective actions or assessment needs, if potential problems are identified.

  15. Comparison of sodium zirconium phosphate-structured HLW forms and synroc for high-level nuclear waste immobilization

    Energy Technology Data Exchange (ETDEWEB)

    Zyryanov, V.N. [Argonne National Lab., IL (United States); Vance, E.R. [ANSTO, Menai (Australia). Materials Division

    1996-12-31

    The incorporation of (a) Cs/Sr as simulated heat-generating isotopes contained in Purex reprocessing waste, (b) simulated actinides, and (c) simulated Purex waste in sodium zirconium phosphate (NZP) has been studied. The samples were prepared by sintering, by hot pressing and by hot isostatic pressing in metal bellows containers. The short-term chemical durability of the phosphate-based material containing Purex waste was within an order of magnitude of that for Synroc-C, as measured by 7-day MCC-1 tests at 90{degrees}C. The dissolution behavior showed evidence of re-precipitation phenomena, even after times as short as 28 days. Potential for improvement of NZP-based ceramics for HLW management is discussed. 19 refs., 4 figs., 3 tabs.

  16. 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.

  17. Evaluation of actinide biosorption by microorganisms

    Energy Technology Data Exchange (ETDEWEB)

    Happel, A.M.

    1996-06-01

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

  18. Low-level waste disposal - Grout issue and alternative waste form technology

    Energy Technology Data Exchange (ETDEWEB)

    Epstein, J.L. [Westinghouse Hanford Co., Richland, WA (United States); Westski, J.H. Jr. [Pacific Northwest Lab., Richland, WA (United States)

    1993-02-01

    Based on the Record of Decision (1) for the Hanford Defense Waste Environmental Impact Statement (HDW-EIS) (2), the US Department of Energy (DOE) is planning to dispose of the low-level fraction of double-shell tank (DST) waste by solidifying the liquid waste as a cement-based grout placed in near-surface, reinforced, lined concrete vaults at the Hanford Site. In 1989, the Hanford Grout Disposal Program (HGDP) completed a full-scale demonstration campaign by successfully grouting 3,800 cubic meters (1 million gallons) of low radioactivity, nonhazardous, phosphate/sulfate waste (PSW), mainly decontamination solution from N Reactor. The HGDP is now preparing for restart of the facility to grout a higher level activity, mixed waste double-shell slurry feed (DSSF). This greater radionuclide and hazardous waste content has resulted in a number of issues confronting the disposal system and the program. This paper will present a brief summary of the Grout Treatment Facility`s components and features and will provide a status of the HGDP, concentrating on the major issues and challenges resulting from the higher radionuclide and hazardous content of the waste. The following major issues will be discussed: Formulation (cementitious mix) development; the Performance Assessment (PA) (3) to show compliance of the disposal system to long-term environmental protection objectives; and the impacts of grouting on waste volume projections and tank space needs.

  19. 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.

  20. 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.

  1. Tellurite glass as a waste form for a simulated mixed chloride waste stream: Candidate materials selection and initial testing

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-02-02

    Tellurite glasses have been researched widely for the last 60 years since they were first introduced by Stanworth. These glasses have been primarily used in research applications as glass host materials for lasers and as non-linear optical materials, though many other uses exist in the literature. Tellurite glasses have long since been used as hosts for various, and even sometimes mixed, halogens (i.e., multiple chlorides or even chlorides and iodides). Thus, it was reasonable to expect that these types of glasses could be used as a waste form to immobilize a combination of mixed chlorides present in the electrochemical separations process involved with fuel separations and processing from nuclear reactors. Many of the properties related to waste forms (e.g., chemical durability, maximum chloride loading) for these materials are unknown and thus, in this study, several different types of tellurite glasses were made and their properties studied to determine if such a candidate waste form could be fabricated with these glasses. One of the formulations studied was a lead tellurite glass, which had a low sodium release and is on-par with high-level waste silicate glass waste forms.

  2. U.S. Food Loss and Waste 2030 Champions Activity Form

    Science.gov (United States)

    To join the U.S. Food Loss and Waste 2030 Champions, organizations complete and submit the 2030 Champions form, in which they commit to reduce food loss and waste in their own operations and periodically report their progress on their website.

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

    Energy Technology Data Exchange (ETDEWEB)

    Qiang, You; Paszczynski, Andrzej; Rao, Linfeng

    2011-10-30

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

  4. Crystal growth methods dedicated to low solubility actinide oxalates

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-04-15

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Wald, J.W.; Brite, D.W.; Gurwell, W.E.; Buckwalter, C.Q.; Bunnell, L.R.; Gray, W.J.; Blair, H.T.; Rusin, J.M.

    1982-02-01

    This report details the results of research on the matrix encapsulation of high level wastes at PML over the past few years. The demonstrations and tests described were designed to illustrate how the waste materials are effected when encapsulated in an inert matrix. Candidate materials evaluated for potential use as matrices for encapslation of pelletized ceramics or glass marbles were categorized into four groups: metals, glasses, ceramics, and graphite. Two processing techniques, casting and hot pressing, were investigated as the most promising methods of formation or densification of the matrices. The major results reported deal with the development aspects. However, chemical durability tests (leach tests) of the matrix materials themselves and matrix-waste form composites are also reported. Matrix waste forms can provide a low porosity, waste-free barrier resulting in increased leach protection, higher impact strength and improved thermal conductivity compared to unencapsulated glass or ceramic waste materials. Glass marbles encapsulated in a lead matrix offer the most significant improvement in waste form stability of all combinations evaluated. This form represents a readily demonstrable process that provides high thermal conductivity, mechanical shock resistance, radiation shielding and increased chemical durability through both a chemical passivation mechanism and as a physical barrier. Other durable matrix waste forms evaluated, applicable primarily to ceramic pellets, involved hot-pressed titanium or TiO/sub 2/ materials. In the processing of these forms, near 100% dense matrices were obtained. The matrix materials had excellent compatibility with the waste materials and superior potential chemical durability. Cracking of the hot-pressed ceramic matrix forms, in general, prevented the realization of their optimum properties.

  6. Glass binder development for a glass-bonded sodalite ceramic waste form

    Energy Technology Data Exchange (ETDEWEB)

    Riley, Brian J.; Vienna, John D.; Frank, Steven M.; Kroll, Jared O.; Peterson, Jacob A.; Canfield, Nathan L.; Zhu, Zihua; Zhang, Jiandong; Kruska, Karen; Schreiber, Daniel K.; Crum, Jarrod V.

    2017-06-01

    This paper discusses work to develop Na2O-B2O3-SiO2 glass binders for immobilizing LiCl-KCl eutectic salt waste in a glass-bonded sodalite waste form following electrochemical reprocessing of used metallic nuclear fuel. Here, five new glasses with high Na2O contents were designed to generate waste forms having higher sodalite contents and fewer stress fractures. The structural, mechanical, and thermal properties of the new glasses were measured using variety of analytical techniques. The glasses were then used to produce ceramic waste forms with surrogate salt waste. The materials made using the glasses developed during this study were formulated to generate more sodalite than materials made with previous baseline glasses used. The coefficients of thermal expansion for the glass phase in the glass-bonded sodalite waste forms made with the new binder glasses were closer to the sodalite phase in the critical temperature region near and below the glass transition temperature. These improvements should result in lower probability of cracking in the full-scale monolithic ceramic waste form, leading to better long-term chemical durability. Additionally, a model generated during this study for predicting softening temperature of silicate binder glasses is presented.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-04-01

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

  8. 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

  9. 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.

  10. 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)

  11. 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.

  12. Approaches to the RAW (Actinides, Fission Products) transmutation in fusion blankets

    Energy Technology Data Exchange (ETDEWEB)

    Lopatkin, A.; Tocheniy, L. [ENTEK-RDIPE, Moscow (Russian Federation)

    1994-12-31

    Within the framework of developing the general concept of large-scale environmentally safe use of nuclear reactor energy RDIPE, executes research of ways to radically decrease the hazard of high-level radioactive wastes (actinides, fission products) to be buried into the Earth. The opportunities are appreciated for replacement and transmutation of RAW fractions and nuclides into nuclear reactor with various spectrum at various irradiation regime, including specialized reactor with utmost parameters and blankets of fusion and linac-driven reactors. The results indicate on expediency of transmutation of actinides in fast reactor in closed fuel cycle. As to fission products, one part of them can be used in radiative technologies (Cs, Sr) or reused in reactor (Zr), other part (Sm, I, Tc) can be transmuted into power-generating reactor, so that together with other after long-time (200-300 years) controllable cooling to be bured into the Earth. In blanket the considerable influence on result of actinide irradiation can are rendered by the fast neutrons (fusion ones in the case of thermonuclear reactor or spalation ones in accelerator driven machine), the threshold reactions of (n,f), (n,2n), (n,3n) and etc. The fusion reactor has wide enough opportunities to form spectrum of neutrons, optimum for reactions (n,f), (n;{gamma}), (n,2n), including threshold ones, as well as the replacement of mass of several tons of RAW are technically possible. However, at fast neutron spectrum light actinide isotopes (U-232, Pu-236) are produced in quantities on 2-3 order up then in the case of fission reactor, but at softer one the probabilities of threshold reactions of even nuclei are reduced. This scheme in general permits to ensure the completion of radiative equivalence of uranium taken from the Earth, and appropriate RAW, directed into the Earth.

  13. 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.

  14. Combined Extraction of Cesium, Strontium, and Actinides from Alkaline Media: An Extension of the Caustic-Side Solvent Extraction (CSSX) Process Technology

    Energy Technology Data Exchange (ETDEWEB)

    Kenneth Raymond

    2004-11-03

    The wastes present at DOE long-term storage sites are usually highly alkaline, and because of this, much of the actinides in these wastes are in the sludge phase. Enough actinide materials still remain in the supernatant liquid that they require separation followed by long-term storage in a geological repository. The removal of these metals from the liquid waste stream would permit their disposal as low-level waste and dramatically reduce the volume of high-level wastes.

  15. Fundamental Aspects of Zeolite Waste Form Production by Hot Isostatic Pressing

    Energy Technology Data Exchange (ETDEWEB)

    Jubin, Robert Thomas [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Bruffey, Stephanie H. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Jordan, Jacob A. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2017-02-01

    The direct conversion of iodine-bearing sorbents into a stable waste form is a research topic of interest to the US Department of Energy. The removal of volatile radioactive 129I from the off-gas of a nuclear fuel reprocessing facility will be necessary in order to comply with the regulatory requirements that apply to facilities sited within the United States (Jubin et al., 2012a), and any iodine-containing media or solid sorbents generated by this process would contain 129I and would be destined for eventual geological disposal. While recovery of iodine from some sorbents is possible, a method to directly convert iodineloaded sorbents to a durable waste form with little or no additional waste materials being formed and a potentially reduced volume would be beneficial. To this end, recent studies have investigated the conversion of iodine-loaded silver mordenite (I-AgZ) directly to a waste form by hot isostatic pressing (HIPing) (Bruffey and Jubin, 2015). Silver mordenite (AgZ), of the zeolite class of minerals, is under consideration for use in adsorbing iodine from nuclear reprocessing off-gas streams. Direct conversion of I-AgZ by HIPing may provide the following benefits: (1) a waste form of high density that is tolerant to high temperatures, (2) a waste form that is not significantly chemically hazardous, and (3) a robust conversion process that requires no pretreatment.

  16. 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.

  17. 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.

  18. FLUIDIZED BED STEAM REFORMED MINERAL WASTE FORMS: CHARACTERIZATION AND DURABILITY TESTING

    Energy Technology Data Exchange (ETDEWEB)

    Jantzen, C; Troy Lorier, T; John Pareizs, J; James Marra, J

    2007-03-31

    Fluidized Bed Steam Reforming (FBSR) is being considered as a potential technology for the immobilization of a wide variety of high sodium low activity wastes (LAW) such as those existing at the Hanford site, at the Idaho National Laboratory (INL), and the Savannah River Site (SRS). The addition of clay, charcoal, and a catalyst as co-reactants with the waste denitrates the aqueous wastes and forms a granular mineral waste form that can subsequently be made into a monolith for disposal if necessary. The waste form produced is a multiphase mineral assemblage of Na-Al-Si (NAS) feldspathoid minerals with cage and ring structures and iron bearing spinel minerals. The mineralization occurs at moderate temperatures between 650-750 C in the presence of superheated steam. The cage and ring structured feldspathoid minerals atomically bond radionuclides like Tc-99 and Cs-137 and anions such as SO4, I, F, and Cl. The spinel minerals stabilize Resource Conservation and Recovery Act (RCRA) hazardous species such as Cr and Ni. Granular mineral waste forms were made from (1) a basic Hanford Envelope A low-activity waste (LAW) simulant and (2) an acidic INL simulant commonly referred to as sodium bearing waste (SBW) in pilot scale facilities at the Science Applications International Corporation (SAIC) Science and Technology Applications Research (STAR) facility in Idaho Falls, ID. The FBSR waste forms were characterized and the durability tested via ASTM C1285 (Product Consistency Test), the Environmental Protection Agency (EPA) Toxic Characteristic Leaching Procedure (TCLP), and the Single Pass Flow Through (SPFT) test. The results of the SPFT testing and the activation energies for dissolution are discussed in this study.

  19. FLUIDIZED BED STEAM REFORMED MINERAL WASTE FORMS: CHARACTERIZATION AND DURABILITY TESTING

    Energy Technology Data Exchange (ETDEWEB)

    Jantzen, C; Troy Lorier, T; John Pareizs, J; James Marra, J

    2006-12-06

    Fluidized Bed Steam Reforming (FBSR) is being considered as a potential technology for the immobilization of a wide variety of high sodium low activity wastes (LAW) such as those existing at the Hanford site, at the Idaho National Laboratory (INL), and the Savannah River Site (SRS). The addition of clay, charcoal, and a catalyst as co-reactants with the waste denitrates the aqueous wastes and forms a granular mineral waste form that can subsequently be made into a monolith for disposal if necessary. The waste form produced is a multiphase mineral assemblage of Na-Al-Si (NAS) feldspathoid minerals with cage and ring structures and iron bearing spinel minerals. The mineralization occurs at moderate temperatures between 650-750 C in the presence of superheated steam. The cage and ring structured feldspathoid minerals atomically bond radionuclides like Tc-99 and Cs-137 and anions such as SO{sub 4}, I, F, and Cl. The spinel minerals stabilize Resource Conservation and Recovery Act (RCRA) hazardous species such as Cr and Ni. Granular mineral waste forms were made from (1) a basic Hanford Envelope A low activity waste (LAW) simulant and (2) an acidic INL simulant commonly referred to as sodium bearing waste (SBW) in pilot scale facilities at the Science Applications International Corporation (SAIC) Science and Technology Applications Research (STAR) facility in Idaho Falls, ID. The FBSR waste forms were characterized and the durability tested via ASTM C1285 (Product Consistency Test), the Environmental Protection Agency (EPA) Toxic Characteristic Leaching Procedure (TCLP), and the Single Pass Flow Through (SPFT) test. The results of the SPFT testing and the activation energies for dissolution are discussed in this study.

  20. Actinide Topological Insulator Materials with Strong Interaction

    OpenAIRE

    Zhang, X.; Zhang, H.; Wang, J.; Felser, C.; Zhang, S.-C.

    2011-01-01

    Topological band insulators have recently been discovered in spin-orbit coupled two and three dimensional systems. In this work, we theoretically predict a class of topological Mott insulators where interaction effects play a dominant role. In actinide elements, simple rocksalt compounds formed by Pu and Am lie on the boundary of metal to insulator transition. We show that interaction drives a quantum phase transition to a topological Mott insulator phase with a single Dirac cone on the surface.

  1. Performance of a Steel/Oxide Composite Waste Form for Combined Waste Steams from Advanced Electrochemical Processes

    Energy Technology Data Exchange (ETDEWEB)

    Indacochea, J. E. [Univ. of Illinois, Chicago, IL (United States); Gattu, V. K. [Univ. of Illinois, Chicago, IL (United States); Chen, X. [Univ. of Illinois, Chicago, IL (United States); Rahman, T. [Univ. of Illinois, Chicago, IL (United States)

    2017-06-15

    The results of electrochemical corrosion tests and modeling activities performed collaboratively by researchers at the University of Illinois at Chicago and Argonne National Laboratory as part of workpackage NU-13-IL-UIC-0203-02 are summarized herein. The overall objective of the project was to develop and demonstrate testing and modeling approaches that could be used to evaluate the use of composite alloy/ceramic materials as high-level durable waste forms. Several prototypical composite waste form materials were made from stainless steels representing fuel cladding, reagent metals representing metallic fuel waste streams, and reagent oxides representing oxide fuel waste streams to study the microstructures and corrosion behaviors of the oxide and alloy phases. Microelectrodes fabricated from small specimens of the composite materials were used in a series of electrochemical tests to assess the corrosion behaviors of the constituent phases and phase boundaries in an aggressive acid brine solution at various imposed surface potentials. The microstructures were characterized in detail before and after the electrochemical tests to relate the electrochemical responses to changes in both the electrode surface and the solution composition. The results of microscopic, electrochemical, and solution analyses were used to develop equivalent circuit and physical models representing the measured corrosion behaviors of the different materials pertinent to long-term corrosion behavior. This report provides details regarding (1) the production of the composite materials, (2) the protocol for the electrochemical measurements and interpretations of the responses of multi-phase alloy and oxide composites, (3) relating corrosion behaviors to microstructures of multi-phase alloys based on 316L stainless steel and HT9 (410 stainless steel was used as a substitute) with added Mo, Ni, and/or Mn, and (4) modeling the corrosion behaviors and rates of several alloy/oxide composite

  2. 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.

  3. 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.

  4. Development of thermal conditioning technology for alpha-contaminated wastes: a study on leaching characteristics and long-term safety assessment of simulated waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Seo, Yong Chil [Yonsei University, Seoul (Korea); Lee, Sang Hoon; Yoo, Jong Ik; Choi, Yong Cheol [Yonsei University, Seoul (Korea)

    2001-04-01

    Radioactive wastes should be stabilized for safe management during several hundred years. To assess stability of solidified waste forms, mechanical properties and chemical durability of the waste forms should be analyzed. Chemical durability is one of the most important factors in the assessment of waste forms, which could be examined by leaching tests. Various methods in leaching test are suggested by different organizations, but a formal test method in Korea is not ready yet. Therefore, the leaching test method applicable to various constituents is necessary for the safe management of radioactive wastes In this study, leaching behavior and characteristics of components such as solidification materials, heavy metals and radioactive nuclids were analyzed for cement waste form and glassy waste form. 58 refs., 25 figs., 8 tabs. (Author)

  5. 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.

  6. Citrate based ``TALSPEAK`` lanthanide-actinide separation process

    Energy Technology Data Exchange (ETDEWEB)

    Del Cul, G.D.; Bond, W.D.; Toth, L.M.; Davis, G.D.; Dai, S.; Metcalf, D.H.

    1994-09-01

    The potential hazard posed to future generations by long-lived radionuclides such as the transuranic elements (TRU) is perceived as a major problem associated with the use of nuclear power. TRU wastes have to remain isolated from the environment for ``geological`` periods of time. The costs of building, maintaining, and operating a ``geological TRU repository`` can be very high. Therefore, there are significant economical advantages in segregating the relatively low volume of TRU wastes from other nuclear wastes. The chemical behavior of lanthanides and actinides, 4f and 5f elements respectively, is rather similar. As a consequence, the separation of these two groups is difficult. The ``TALSPEAK`` process (Trivalent Actinide Lanthanide Separations by Phosphorus-reagent Extraction from Aqueous Complexes) is one of the few means available to separate the trivalent actinides from the lanthanides. The method is based on the preferential complexation of the trivalent actinides by an aminopolyacetic acid. Cold experiments showed that by using citric acid the deleterious effects produced by impurities such as zirconium are greatly reduced.

  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. 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.

  9. 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

  10. 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.

  11. 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.

  12. A glass-encapsulated calcium phosphate wasteform for the immobilization of actinide-, fluoride-, and chloride-containing radioactive wastes from the pyrochemical reprocessing of plutonium metal

    Science.gov (United States)

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

    2007-03-01

    Chloride-containing radioactive wastes are generated during the pyrochemical reprocessing of Pu metal. Immobilization of these wastes in borosilicate glass or Synroc-type ceramics is not feasible due to the very low solubility of chlorides in these hosts. Alternative candidates have therefore been sought including phosphate-based glasses, crystalline ceramics and hybrid glass/ceramic systems. These studies have shown that high losses of chloride or evolution of chlorine gas from the melt make vitrification an unacceptable solution unless suitable off-gas treatment facilities capable of dealing with these corrosive by-products are available. On the other hand, both sodium aluminosilicate and calcium phosphate ceramics are capable of retaining chloride in stable mineral phases, which include sodalite, Na 8(AlSiO 4) 6Cl 2, chlorapatite, Ca 5(PO 4) 3Cl, and spodiosite, Ca 2(PO 4)Cl. The immobilization process developed in this study involves a solid state process in which waste and precursor powders are mixed and reacted in air at temperatures in the range 700-800 °C. The ceramic products are non-hygroscopic free-flowing powders that only require encapsulation in a relatively low melting temperature phosphate-based glass to produce a monolithic wasteform suitable for storage and ultimate disposal.

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

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hang Bok

    1998-08-01

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

  14. 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.

  15. Microstructural characterization of halite inclusion in a glass-bonded ceramic waste form.

    Energy Technology Data Exchange (ETDEWEB)

    Luo, J. S.; Ebert, W. L.

    2000-12-14

    A glass-bonded ceramic waste form is being developed to immobilize radioactively contaminated chloride waste salts generated during the conditioning of spent sodium-bonded nuclear fuel for disposal. The waste salt is first mixed with zeolite A to occlude the salt into cavities in the zeolite structure. The salt-loaded zeolite is then mixed with a borosilicate glass and consolidated by hot isostatic pressing. During this process, the zeolite converts to the mineral sodalite, which retains most of the waste salt, and small amounts of halite are generated. Halite inclusions have been observed within micron- to submicron-sized pores that form within the glass phase in the vicinity of the sodalite/glass interface. These inclusions are important because they may contain small amounts of radionuclide contaminants (eg {sup 135}Cs and {sup 129}I),and may affect the corrosion behavior of the waste form. Optical microscopy, scanning electron microscopy, and transmission electron microscopy were used to characterize the chemical nature and distribution of halite inclusions in the waste form.

  16. 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

  17. 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).

  18. 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).

  19. 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.

  20. 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.).

  1. A study of transformation water - soluble forms of hevy metals at waste incenerator for detoxicationof ash.

    Directory of Open Access Journals (Sweden)

    Bilets'ka V. А.

    2011-11-01

    Full Text Available The complex research processes of transformation of soluble forms of heavy metals in sediment interaction with ash. Proved that the adsorption processes of immobilization lead to a significant decrease of soluble forms of heavy metals in the waste.

  2. Finite element analysis of ion transport in solid state nuclear waste form materials

    Science.gov (United States)

    Rabbi, F.; Brinkman, K.; Amoroso, J.; Reifsnider, K.

    2017-09-01

    Release of nuclear species from spent fuel ceramic waste form storage depends on the individual constituent properties as well as their internal morphology, heterogeneity and boundary conditions. Predicting the release rate is essential for designing a ceramic waste form, which is capable of effectively storing the spent fuel without contaminating the surrounding environment for a longer period of time. To predict the release rate, in the present work a conformal finite element model is developed based on the Nernst Planck Equation. The equation describes charged species transport through different media by convection, diffusion, or migration. And the transport can be driven by chemical/electrical potentials or velocity fields. The model calculates species flux in the waste form with different diffusion coefficient for each species in each constituent phase. In the work reported, a 2D approach is taken to investigate the contributions of different basic parameters in a waste form design, i.e., volume fraction, phase dispersion, phase surface area variation, phase diffusion co-efficient, boundary concentration etc. The analytical approach with preliminary results is discussed. The method is postulated to be a foundation for conformal analysis based design of heterogeneous waste form materials.

  3. 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...

  4. 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

  5. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2008-07-01

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

  7. Nuclear waste-form risk assessment for US defense waste at Savannah River Plant. Annual report FY, 1982

    Energy Technology Data Exchange (ETDEWEB)

    Cheung, H.; Edwards, L.L.; Harvey, T.F.

    1982-08-09

    A network model was developed to simulate the hydrological flow and the transport of radionuclides from a deep geological repository to the biosphere subsequent to closure. By means of very efficient computational methods for solving the fundamental differential equations, a code was developed to treat in great detail the effects of waste form characteristics and of repository designs on the repository risks. It is possible to examine near field effects heretofore not attempted. Without sacrificing the essential details of description, the code can also be applied to perform probabilistic risk analyses to high confidence levels. Analytical results showed: (1) for waste form release rates greater than approximately 5 x 10/sup -7//yr, dose to man is insensitive to release rate and release rate uncertainty; (2) significant reduction in dose can be achieved through simple design modifications; (3) a basalt repository generally does not perform as well as a salt repository; and (4) disruptive events are relatively unimportant for repository safety. 82 references.

  8. 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.

  9. 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.

  10. 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.

  11. 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.

  12. Actinide-zirconia based materials for nuclear applications: Cubic stabilized zirconia versus pyrochlore oxide

    Science.gov (United States)

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

    2000-07-01

    Concepts about nuclear energy and nuclear materials have changed considerably over the past six decades. Regardless of one's position on the nuclear generation of electric power, there are serious needs for pursuing fundamental and technological science of existing actinide materials. These needs are best addressed by obtaining an atomic and molecular understanding of these actinides and actinide containing materials. Although electro-nuclear energy is considered less polluting in terms of uncontrolled releases (e.g., SO2, heavy metals, CO2, etc.) into the environment, its use produces solid wastes, which offer a challenge for scientists. Fortunately, concepts are being developed to appropriately handle these materials after irradiation, reprocessing, etc.

  13. Assessment of the Cast Stone Low-Temperature Waste Form Technology Coupled with Technetium Removal - 14379

    Energy Technology Data Exchange (ETDEWEB)

    Brown, Christopher F.; Rapko, Brian M.; Serne, R. Jeffrey; Westsik, Joseph H.; Cozzi, Alex; Fox, Kevin M.; Mccabe, Daniel J.; Nash, C. A.; Wilmarth, William R.

    2014-03-03

    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) were 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 and technetium removal projects at Hanford. Science and technology gaps 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 separation of technetium from waste processing streams. Technical approaches to address the science and technology gaps were identified and an initial sequencing priority was suggested. A subset of research was initiated in 2013 to begin addressing the most significant science and technology gaps. The purpose of this paper is to report progress made towards closing these gaps and provide notable highlights of results achieved to date.

  14. 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.

  15. Actinide transmutation in nuclear reactors

    Energy Technology Data Exchange (ETDEWEB)

    Ganev, I.K.; Lopatkin, A.V.; Naumov, V.V.; Tocheny, L.V.

    1993-12-31

    Of some interest is the comparison between the actinide nuclide burning up (fission) rates such as americium 241, americium 242, curium 244, and neptunium 237, in the reactors with fast or thermal neutron spectra.

  16. 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)

  17. 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

  18. Purification of alkaline solutions and wastes from actinides and technetium by coprecipitation with some carriers using the method of appearing reagents: Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Peretrukhin, V.F.; Silin, V.I.; Kareta, A.V.; Gelis, A.V.; Shilov, V.P.; German, K.E.; Firsova, E.V.; Maslennikov, A.G.; Trushina, V.E. [Russian Academy of Sciences, Moscow (Russian Federation). Inst. of Physical Chemistry

    1998-09-01

    The coprecipitation of transuranium elements (TRU) and technetium from alkaline solutions and from simulants of Hanford Site tank wastes has been studied in reducing and oxidizing conditions on uranium(IV,VI) hydroxocompounds, tetraalkylammonium perrhenate and perchlorate, and on hydroxides of Fe(III), Co(III), Mn(II), and Cr(III) using the method of appearing reagents (MAR). Coprecipitations in alkaline solution have been shown to give high decontamination factors (DF) at low content of carrier and in the presence of high salt concentrations. Uranium(IV) hydroxide in concentrations higher than 3 {times} 10{sup {minus}3} M coprecipitates Pu and Cm in any oxidation state from 0.2 to 4 M NaOH with DFs of 110 to 1000 and Np and Tc with DFs of 51 to 176. Technetium (VII) coprecipitates with (5 to 8) {times} 10{sup {minus}4} M tetrabutylammonium (TBA) perrhenate in 0.01 to 0.02 M TBA hydroxide from 0.5 to 1.5 M NaOH to give DFs of 150 to 200. Coprecipitations of Np and Pu with Co(OH){sub 3}, Fe(OH){sub 3}, Cr(OH){sub 3}, and Mn(OH){sub 2} obtained by the MAR from precursors in the range from pH 10.5 to 0.4 M NaOH give DFs from 80 to 400.

  19. Setting and Stiffening of Cementitious Components in Cast Stone Waste Form for Disposal of Secondary Wastes from the Hanford waste treatment and immobilization plant

    Energy Technology Data Exchange (ETDEWEB)

    Chung, Chul-Woo; Chun, Jaehun; Um, Wooyong; Sundaram, S. K.; Westsik, Joseph H.

    2013-04-01

    Cast stone is a cementitious waste form, a viable option to immobilize secondary nuclear liquid wastes generated from Hanford vitrification plant. While the strength and radioactive technetium leaching of different waste form candidates have been reported, no study has been performed to understand the flow and stiffening behavior of Cast Stone, which is essential to ensure the proper workability, especially considering necessary safety as a nuclear waste form in a field scale application. The rheological and ultrasonic wave reflection (UWR) measurements were used to understand the setting and stiffening Cast Stone batches. X-ray diffraction (XRD) was used to find the correlation between specific phase formation and the stiffening of the paste. Our results showed good correlation between rheological properties of the fresh Cast Stone mixture and phase formation during hydration of Cast Stone. Secondary gypsum formation originating from blast furnace slag was observed in Cast Stone made with low concentration simulants. The formation of gypsum was suppressed in high concentration simulants. It was found that the stiffening of Cast Stone was strongly dependent on the concentration of simulant. A threshold concentration for the drastic change in stiffening was found at 1.56 M Na concentration.

  20. 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.

  1. 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)

  2. Corrosion Behavior and Microstructure Influence of Glass-Ceramic Nuclear Waste Forms

    Energy Technology Data Exchange (ETDEWEB)

    Matthew Asmussen, R. [Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, WA.; Neeway, James J. [Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, WA.; Kaspar, Tiffany C. [Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, WA.; Crum, Jarrod V. [Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, WA.

    2017-06-16

    Glass ceramic waste forms present a potentially viable technology for the long term immobilization and disposal of liquid nuclear wastes. Through control of chemistry during fabrication, such waste forms can have designed secondary crystalline phases within a borosilicate glass matrix. In this work, a glass ceramic containing powellite and oxyapatite secondary phases was tested for its corrosion properties in dilute conditions using single pass flow through testing (SPFT). Three glass ceramic samples were prepared using different cooling rates to produce samples with varying microstructure sizes. In testing at 90 °C in buffered pH 7 and pH 9 solutions, it was found that increasing pH and decreasing microstructure size (resulting from rapid cooling during fabrication) both led to a reduction in overall corrosion rate. The phases of the glass ceramic were found, using a combination of solutions analysis, SEM and AFM, to corrode preferably in the order of powellite > bulk glass matrix > oxyapatite.

  3. 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.

  4. 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.

  5. Performance testing of grout-based waste forms for the solidification of anion exchange resins

    Energy Technology Data Exchange (ETDEWEB)

    Morgan, I.L.; Bostick, W.D.

    1990-10-01

    The solidification of spent ion exchanges resins in a grout matrix as a means of disposing of spent organic resins produced in the nuclear fuel cycle has many advantages in terms of process simplicity and economy, but associated with the process is the potential for water/cement/resins to interact and degrade the integrity of the waste form solidified. Described in this paper is one possible solution to preserving the integrity of these solidified waste forms: the encapsulation of beaded anion exchange resins in grout formulations containing ground granulated blast furnace slag, Type I-II (mixed) portland cement, and additives (clays, amorphous silica, silica fume, and fly ash). The results of the study reported herein show the cured waste form tested has a low leach rate for nitrate ion from the resin (and a low leach rate is inferred for Tc-99) and acceptable durability as assessed by the water immersion and freezing/thawing test protocols. The results also suggest a tested surrogate waste form prepared in vinyl ester styrene binder performs satisfactorily against the wetting/drying criterion, and it should offer additional insight into future work on the solidification of spent organic resins. 26 refs., 4 figs., 5 tabs.

  6. Partitioning of Mercury from Actinides in the TRUEX Process

    Energy Technology Data Exchange (ETDEWEB)

    Fiskum, Sandra K.(BATTELLE (PACIFIC NW LAB)); Rapko, Brian M.(BATTELLE (PACIFIC NW LAB)); Lumetta, Gregg J.(BATTELLE (PACIFIC NW LAB))

    2000-11-01

    A mercury complexant, L-cysteine hydrochloride, was tested for use in separating Hg from actinides during TRUEX processing of wastes at the Idaho National Engineering and Environmental Laboratory (INEEL). Mercury, americium, plutonium and uranyl distributions from TRUEX solvent were characterized over a nitric acid concentration range of 0.01 to 2 M. The applicability of cysteine was also evaluated for selective Hg complexation in an INEEL sodium-bearing waste simulant. A test was also conducted to evaluate the applicability of cysteine to separate Hg from Sr in the SREX process with Sr Resin used as a stand-in for the SREX process solvent. In all cases, the use of L-cysteine HCl retained Hg in the aqueous phase while causing no or little perturbation in the actinide and Sr distribution behavior.

  7. The INE-Beamline for actinide science at ANKA.

    Science.gov (United States)

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

    2012-04-01

    Since its inauguration in 2005, the INE-Beamline for actinide research at the synchrotron source ANKA (KIT North Campus) provides dedicated instrumentation for x-ray spectroscopic characterization of actinide samples and other radioactive materials. R&D work at the beamline focuses on various aspects of nuclear waste disposal within INE's mission to provide the scientific basis for assessing long-term safety of a final nuclear waste repository. The INE-Beamline is accessible for the actinide and radiochemistry community through the ANKA proposal system and the European Union Integrated Infrastructure Initiative ACTINET-I3. Experiments with activities up to 1 × 10(+6) times the European exemption limit are feasible within a safe but flexible containment concept. Measurements with monochromatic radiation are performed at photon energies varying between ~2.1 keV (P K-edge) and ~25 keV (Pd K-edge), including the lanthanide L-edges and the actinide M- and L3-edges up to Cf. The close proximity of the INE-Beamline to INE controlled area labs offers infrastructure unique in Europe for the spectroscopic and microscopic characterization of actinide samples. The modular beamline design enables sufficient flexibility to adapt sample environments and detection systems to many scientific questions. The well-established bulk techniques x-ray absorption fine structure (XAFS) spectroscopy in transmission and fluorescence mode have been augmented by advanced methods using a microfocused beam, including (confocal) XAFS/x-ray fluorescence detection and a combination of (micro-)XAFS and (micro-)x-ray diffraction. Additional instrumentation for high energy-resolution x-ray emission spectroscopy has been successfully developed and tested. © 2012 American Institute of Physics

  8. Managing Zirconium Chemistry and Phase Compatibility in Combined Process Separations for Minor Actinide Partitioning

    Energy Technology Data Exchange (ETDEWEB)

    Wall, Nathalie [Washington State Univ., Pullman, WA (United States); Nash, Ken [Washington State Univ., Pullman, WA (United States); Martin, Leigh [Washington State Univ., Pullman, WA (United States)

    2017-03-17

    In response to the NEUP Program Supporting Fuel Cycle R&D Separations and Waste Forms call DEFOA- 0000799, this report describes the results of an R&D project focusing on streamlining separation processes for advanced fuel cycles. An example of such a process relevant to the U.S. DOE FCR&D program would be one combining the functions of the TRUEX process for partitioning of lanthanides and minor actinides from PUREX(UREX) raffinates with that of the TALSPEAK process for separating transplutonium actinides from fission product lanthanides. A fully-developed PUREX(UREX)/TRUEX/TALSPEAK suite would generate actinides as product(s) for reuse (or transmutation) and fission products as waste. As standalone, consecutive unit-operations, TRUEX and TALSPEAK employ different extractant solutions (solvating (CMPO, octyl(phenyl)-N,Ndiisobutylcarbamoylmethylphosphine oxide) vs. cation exchanging (HDEHP, di-2(ethyl)hexylphosphoric acid) extractants), and distinct aqueous phases (2-4 M HNO3 vs. concentrated pH 3.5 carboxylic acid buffers containing actinide selective chelating agents). The separate processes may also operate with different phase transfer kinetic constraints. Experience teaches (and it has been demonstrated at the lab scale) that, with proper control, multiple process separation systems can operate successfully. However, it is also recognized that considerable economies of scale could be achieved if multiple operations could be merged into a single process based on a combined extractant solvent. The task of accountability of nuclear materials through the process(es) also becomes more robust with fewer steps, providing that the processes can be accurately modeled. Work is underway in the U.S. and Europe on developing several new options for combined processes (TRUSPEAK, ALSEP, SANEX, GANEX, ExAm are examples). There are unique challenges associated with the operation of such processes, some relating to organic phase chemistry, others arising from the

  9. 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)

  10. Properties of SYNROC C nuclear-waste form: a state-of-the-art review

    Energy Technology Data Exchange (ETDEWEB)

    Oversby, V.M.

    1982-09-01

    SYNROC C is a titanate ceramic waste form designed to contain the waste generated by the reprocessing of commercial nuclear reactor fuel. The properties of SYNROC C are described with particular emphasis on the distribution of chemical elements in SYNROC, the fabrication of good quality specimens, and the chemical durability of SYNROC. Data obtained from testing of natural mineral analogues of SYNROC minerals are briefly discussed. The information available on radiation effects in SYNROC in relation to structural alteration and changes in chemical durability are summarized. 26 references, 2 figures, 18 tables.

  11. 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.

  12. 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.

  13. 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.

  14. Studies of Actinides Reduction on Iron Surfaces by Means ofResonant Inelastic X-ray Scattering

    Energy Technology Data Exchange (ETDEWEB)

    Kvashnina, K.O.; Butorin, S.M.; Shuh, D.K.; Ollila, K.; Soroka,I.; Guo, J.-H.; Werme, L.; Nordgren, J.

    2006-09-18

    The interaction of actinides with corroded iron surfaces was studied using resonant inelastic x-ray scattering (RIXS) spectroscopy at actinide 5d edges. RIXS profiles, corresponding to the f-f excitations are found to be very sensitive to the chemical states of actinides in different systems. Our results clearly indicate that U(VI) (as soluble uranyl ion) was reduced to U(IV) in the form of relatively insoluble uranium species, indicating that the iron presence significantly affects the mobility of actinides, creating reducing conditions. Also Np(V) and Pu (VI) in the ground water solution were getting reduced by the iron surface to Np(IV) and Pu (IV) respectively. Studying the reduction of actinides compounds will have an important process controlling the environmental behavior. Using RIXS we have shown that actinides, formed by radiolysis of water in the disposal canister, are likely to be reduced on the inset corrosion products and prevent release from the canister.

  15. 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

  16. 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.

  17. Repository performance assessment of waste forms from the electrometallurgical treatment of sodium-bonded spent nuclear fuel

    Energy Technology Data Exchange (ETDEWEB)

    Morris, E. E.; Fanning, T. H.; Feldman, E. E.; Petri, M. C.

    2000-03-20

    The ceramic and metal waste forms produced by electrometallurgical treatment of sodium-bonded spent nuclear fuel are undergoing evaluation as to how they will perform within the geologic repository which is proposed to be built at Yucca Mountain. An initial assessment, making use of preliminary degradation models for the waste forms, is described. The analyses are performed with a simplified version of the Total System Performance Assessment--Viability Assessment repository model. Results indicate that the ability of the ceramic and metal waste forms to retain radionuclides is similar to and sometimes better than defense high-level waste glass.

  18. 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

  19. Setting and stiffening of cementitious components in Cast Stone waste form for disposal of secondary wastes from the Hanford waste treatment and immobilization plant

    Energy Technology Data Exchange (ETDEWEB)

    Chung, Chul-Woo; Chun, Jaehun, E-mail: jaehun.chun@pnnl.gov; Um, Wooyong; Sundaram, S.K.; Westsik, Joseph H.

    2013-04-01

    Cast Stone is a cementitious waste form, a viable option to immobilize secondary nuclear liquid wastes generated from the Hanford Waste Treatment and Immobilization Plant. However, no study has been performed to understand the flow and stiffening behavior, which is essential to ensure proper workability and is important to safety in a nuclear waste field-scale application. X-ray diffraction, rheology, and ultrasonic wave reflection methods were used to understand the specific phase formation and stiffening of Cast Stone. Our results showed a good correlation between rheological properties of the fresh mixture and phase formation in Cast Stone. Secondary gypsum formation was observed with low concentration simulants, and the formation of gypsum was suppressed in high concentration simulants. A threshold concentration for the drastic change in stiffening was found at 1.56 M Na concentration. It was found that the stiffening of Cast Stone was strongly dependent on the concentration of simulant. Highlights: • A combination of XRD, UWR, and rheology gives a better understanding of Cast Stone. • Stiffening of Cast Stone was strongly dependent on the concentration of simulant. • A drastic change in stiffening of Cast Stone was found at 1.56 M Na concentration.

  20. Actinides and Life's Origins

    Science.gov (United States)

    Adam, Zachary

    2007-12-01

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

  1. DEVELOPMENT & TESTING OF A CEMENT BASED SOLID WASTE FORM USING SYNTHETIC UP-1 GROUNDWATER

    Energy Technology Data Exchange (ETDEWEB)

    COOKE, G.A.; LOCKREM, L.L.

    2006-11-10

    The Effluent Treatment Facility (ETF) in the 200 East Area of the Hanford Site is investigating the conversion of several liquid waste streams from evaporator operations into solid cement-based waste forms. The cement/waste mixture will be poured into plastic-lined mold boxes. After solidification the bags will be removed from the molds and sealed for land disposal at the Hanford Site. The RJ Lee Group, Inc. Center for Laboratory Sciences (CLS) at Columbia Basin College (CBC) was requested to develop and test a cementitious solids (CS) formulation to solidify evaporated groundwater brine, identified as UP-1, from Basin 43. Laboratory testing of cement/simulant mixtures is required to demonstrate the viability of cement formulations that reduce the overall cost, minimize bleed water and expansion, and provide suitable strength and cure temperature. Technical support provided mixing, testing, and reporting of values for a defined composite solid waste form. In this task, formulations utilizing Basin 43 simulant at varying wt% solids were explored. The initial mixing consisted of making small ({approx} 300 g) batches and casting into 500-mL Nalgene{reg_sign} jars. The mixes were cured under adiabatic conditions and checked for bleed water and consistency at recorded time intervals over a 1-week period. After the results from the preliminary mixing, four formulations were selected for further study. The testing documentation included workability, bleed water analysis (volume and pH) after 24 hours, expansivity/shrinkage, compressive strength, and selected Toxicity Characteristic Leaching Procedure (TCLP) leach analytes of the resulting solid waste form.

  2. 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.

  3. 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.

  4. Silica-based waste form for immobilization of iodine from reprocessing plant off-gas streams

    Energy Technology Data Exchange (ETDEWEB)

    Matyáš, Josef, E-mail: Josef.Matyas@pnnl.gov [Radiological Materials & Technology Development, Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352 (United States); Canfield, Nathan [Electrochemical Materials and Systems, Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352 (United States); Sulaiman, Sannoh; Zumhoff, Mac [Radiological Materials & Technology Development, Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352 (United States)

    2016-08-01

    A high selectivity and sorption capacity for iodine and a feasible consolidation to a durable SiO{sub 2}-based waste form makes silver-functionalized silica aerogel (Ag{sup 0}-aerogel) an attractive choice for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. Hot uniaxial pressing of iodine-loaded Ag{sup 0}-aerogel (20.2 mass% iodine) at 1200 °C for 30 min under 29 MPa pressure provided a partially sintered product with residual open porosity of 16.9% that retained ∼93% of sorbed iodine. Highly iodine-loaded Ag{sup 0}-aerogel was successfully consolidated by hot isostatic pressing at 1200 °C with a 30-min hold and under 207 MPa. The fully densified waste form had a bulk density of 3.3 × 10{sup 3} kg/m{sup 3} and contained ∼39 mass% iodine. The iodine was retained in the form of nano- and micro-particles of AgI that were uniformly distributed inside and along boundaries of fused silica grains. - Highlights: • Silver-functionalized silica aerogel is an effective sorbent and a viable waste form for iodine. • Simultaneous application of fast heating rates and high pressures produced a fully dense product. • HIPing produced a fully consolidated waste form with a bulk density of 3.3 × 10{sup 3} kg/m{sup 3} and containing ∼39 mass% of iodine.

  5. Effect of aluminum and silicon reactants and hip soak time on characteristics of glass-ceramic waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Vinjamuri, K. [Idaho National Engineering Labs., Idaho Falls, ID (United States)

    1994-12-31

    The effects of aluminum and silicon reactants and process soak time on total and normalized elemental leach rates and microstructure of glass-ceramic waste forms are investigated. Glass-ceramic waste forms were prepared by hot isostatically pressing (HIPing) a pre-compacted mixture of pilot plant fluorinel-sodium calcine, Al, and Si metal powders at 1050{degrees}C, 138 MPa for 4 hours. The formulation with 2 wt% Al was HIPed for 4, 8, 16 and 24 hours at 1050{degrees}C and 138 MPa. The leach rates remained essentially constant for the 2 wt% Al waste form that was HIPed for 4, 8, 16 and 24 hours at the same temperature and pressure. However, the leach rates increased in the waste forms where the Si content was increased. The 2 wt% Al waste form appears to be the potential candidate for immobilization of the fluorinel-sodium calcine stored onsite at the Idaho Chemical Processing Plant.

  6. 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.

  7. Fabrication and Properties of Technetium-Bearing Pyrochlores and Perovskites as Potential Waste Forms - 13222

    Energy Technology Data Exchange (ETDEWEB)

    Hartmann, Thomas [University of Nevada - Las Vegas, Harry Reid Center, 4505 S. Maryland Parkway, Box 4009, Las Vegas, NV 89154-4009 (United States); Alaniz, Ariana J. [University of Nevada - Las Vegas, Howard R. Hughes College of Engineering, 4505 S. Maryland Parkway, Box 4009, Las Vegas, NV 89154-4009 (United States); Antonio, Daniel J. [University of Nevada - Las Vegas, Department of Physics and Astronomy, 4505 S. Maryland Parkway, Box 4002, Las Vegas, NV 89154-4002 (United States)

    2013-07-01

    Technetium-99 (t{sub 1/2}= 2.13x10{sup 5} years) is important from a nuclear waste perspective and is one of the most abundant, long-lived radioisotopes in used nuclear fuel (UNF). As such, it is targeted in UNF separation strategies such as UREX+, for isolation and encapsulation in solid waste forms for storage in a nuclear repository. We report here results regarding the incorporation of Tc-99 into ternary oxides of different structure types: pyrochlore (Nd{sub 2}Tc{sub 2}O{sub 7}), perovskite (SrTcO{sub 3}), and layered perovskite (Sr{sub 2}TcO{sub 4}). The goal was to determine synthesis conditions of these potential waste forms to immobilize Tc-99 as tetravalent technetium and to harvest crystallographic, thermophysical and hydrodynamic data. The objective of this research is to provide fundamental crystallographic and thermophysical data on advanced ceramic Tc-99 waste forms such as pyrochlore, perovskite, and layered perovskite in support of our current efforts on the corrosion of technetium-bearing waste forms. The ceramic Tc-99-bearing waste forms exhibit good crystallinity. The lattice parameters and crystal structures of the technetium host phases could be refined with high accuracies of ±3, ±4, and ±7 fm (10{sup -15} m), for Nd{sub 2}Tc{sub 2}O{sub 7}, SrTcO{sub 3}, and Sr{sub 2}TcO{sub 4}, respectively. The associated refinement residuals (R{sub Wp}) for the patterns are 4.1 %, 4.7 % and 6.7 %, and the refinement residuals for the individual phases (R{sub Bragg}) are 2.0 %, 2.4 % and 3.9 %, respectively. Thermophysical properties of the oxides SrTcO{sub 3}, Sr{sub 2}TcO{sub 4}, and Nd{sub 2}Tc{sub 2}O{sub 7} were analyzed using AC magnetic susceptibility measurements to further harvest information on the critical temperature (T{sub c}) for superconductivity. In our experiments the strontium technetates, SrTcO{sub 3} and Sr{sub 2}TcO{sub 4}, show superconductivity at rather high critical temperatures of T{sub c} = 7.8 K and 7 K, respectively. On the

  8. 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.

  9. INNOVATIVE TECHNIQUES AND TECHNOLOGY APPLICATION IN MANAGEMENT OF REMOTE HANDLED AND LARGE SIZED MIXED WASTE FORMS

    Energy Technology Data Exchange (ETDEWEB)

    BLACKFORD LT

    2008-02-04

    of RCRA storage regulations, reduce costs for waste management by nearly 50 percent, and create a viable method for final treatment and disposal of these waste forms that does not impact retrieval project schedules. This paper is intended to provide information to the nuclear and environmental clean-up industry with the experience of CH2M HILL and ORP in managing these highly difficult waste streams, as well as providing an opportunity for sharing lessons learned, including technical methods and processes that may be applied at other DOE sites.

  10. Radiation damage of a glass-bonded zeolite waste form using ion irradiation.

    Energy Technology Data Exchange (ETDEWEB)

    Allen, T. R.; Storey, B. G.

    1997-12-05

    Glass-bonded zeolite is being considered as a candidate ceramic waste form for storing radioactive isotopes separated from spent nuclear fuel in the electrorefining process. To determine the stability of glass-bonded zeolite under irradiation, transmission electron microscope samples were irradiated using high energy helium, lead, and krypton. The major crystalline phase of the waste form, which retains alkaline and alkaline earth fission products, loses its long range order under both helium and krypton irradiation. The dose at which the long range crystalline structure is lost is about 0.4 dpa for helium and 0.1 dpa for krypton. Because the damage from lead is localized in such a small region of the sample, damage could not be recognized even at a peak damage of 50 dpa. Because the crystalline phase loses its long range structure due to irradiation, the effect on retention capacity needs to be further evaluated.

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

    Energy Technology Data Exchange (ETDEWEB)

    None, None

    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.

  12. 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

  13. 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.

  14. 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.

  15. 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

  16. 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)

  17. External Criticality Risk of Immobilized Plutonium Waste Form in a Geologic Repository

    Energy Technology Data Exchange (ETDEWEB)

    J. McClure

    2001-03-12

    This purpose of this technical report is to provide a comprehensive summary of the waste package (WP) external criticality-related risk of the Plutonium Disposition ceramic waste form, which is being developed and evaluated by the Office of Fissile Materials Disposition of the United States Department of Energy (DOE). Potential accumulation of the fissile materials, {sup 239}Pu and {sup 235}U, in rock formations having a favorable chemical environment for such actions, requires analysis because autocatalytic configurations, while unlikely to form, never-the-less have consequences which are undesirable and require evaluation. Secondly, the WP design has evolved necessitating a re-evaluation of the internal WP degradation scenarios that contribute to the external source terms. The scope of this study includes a summary of the revised WP degradation calculations, a summary of the accumulation mechanisms in fractures and lithophysae in the tuff beneath the WP footprint, and a summary of the criticality risk calculations from any accumulated fissile material. Accumulations of fissile material external to the WP sufficient to pose a potential criticality risk require a deposition mechanism operating over sufficient time to reach required levels. The transporting solution concentrations themselves are well below critical levels (CRWMS 2001e). The ceramic waste form consists of Pu immobilized in ceramic disks, which would be embedded in High-Level Waste (HLW) glass in the standard HLW glass disposal canister. The ceramic disks would occupy approximately 12% of the HLW canister volume, while most of the remaining 88% of the volume would be occupied by HLW glass.

  18. Chemistry of the actinide elements. Vol. 2. 2. Ed

    Energy Technology Data Exchange (ETDEWEB)

    Katz, J.J.; Morss, L.R.; Seaborg, G.T. (eds.)

    1986-01-01

    This is a comprehensive, exposition of the chemistry and related properties of the 5f series of elements: actinium, thorium, protactinium, uranium and the first eleven transuranium elements. The descriptions of each element include accounts of their history, separation, metallurgy, solid-state chemistry, solution chemistry, thermodynamics and kinetics. Additionally, separate chapters on spectroscopy, magnetochemistry, thermodynamics, solids, the metallic state, complex ions and organometallic compounds emphasize the comparative chemistry and unique properties of the actinide series of elements. Comprehensive list of properties of all actinide compounds and ions in solution are given, and there are special sections on such topics as biochemistry, superconductivity, radioisotope safety, and waste management, as well as discussion of the transactinides and future elements.

  19. 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.

  20. Sigma Team for Minor Actinide Separation: PNNL FY 2010 Status Report

    Energy Technology Data Exchange (ETDEWEB)

    Lumetta, Gregg J.; Sinkov, Sergey I.; Neiner, Doinita; Levitskaia, Tatiana G.; Braley, Jenifer C.; Carter, Jennifer C.; Warner, Marvin G.; Pittman, Jonathan W.; Rapko, Brian M.

    2010-08-24

    Work conducted at Pacific Northwest National Laboratory (PNNL) in FY 2010 addressed two lines of inquiry. The two hypotheses put forth were: 1. The extractants from the TRUEX( ) process (CMPO)( ) and from the TALSPEAK( ) process (HDEHP)( ) can be combined into a single process solvent to separate 1) the lanthanides and actinides from acidic high-level waste and 2) the actinides from the lanthanides in a single solvent extraction process. (Note: This combined process will hereafter be referred to as the TRUSPEAK process.) A series of empirical measurements performed (both at PNNL and Argonne National Laboratory) in FY 2009 supported this hypothesis, but also indicated some nuances to the chemistry. Lanthanide/americium separation factors of 12 and higher were obtained with a prototypic TRUSPEAK solvent when extracting the lanthanides from a citrate-buffered DTPA( ) solution. Although the observed separation factors are sufficiently high to design an actinide/lanthanide separation process, a better understanding of the chemistry is expected to lead to improved solvent formulations and improved process performance. Work in FY 2010 focused on understanding the synergistic extraction behavior observed for Nd(III) and Am(III) when extracted into mixtures of CMPO and HDEHP. The interaction between CMPO and HDEHP in dodecane was investigated by 31P NMR spectroscopy, and an adduct of the type CMPO•HDEHP was found to form. The formation of this adduct will reduce the effective extractant concentrations and must be taken into account when modeling metal ion extraction data in this system. Studies were also initiated to determine the Pitzer parameters for Nd(III) in lactate media. 2. Higher oxidation states (e.g., +5 and +6) of Am can be stabilized in solution by complexation with uranophilic ligands, and this chemistry can be exploited to separate Am from Cm. To test this hypothesis, the previously reported stereognostic uranophilic ligands NPB( ) and ETAC(e) were

  1. 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.

  2. Cordierite containing ceramic membranes from smectetic clay using natural organic wastes as pore-forming agents

    Directory of Open Access Journals (Sweden)

    W. Misrar

    2017-06-01

    Full Text Available Cordierite ceramic membranes were manufactured from natural clay, oxides and organic wastes as pore forming agents. Mixtures aforementioned materials with the pore-forming agents (up to 10 wt.% were investigated in the range 1000–1200 °C using thermal analysis, X-ray diffraction, scanning electron microscopy, mercury porosimetry and filtration tests. Physical properties (density, water absorption and bending strength were correlated to the processing factors (pore-forming agent addition, firing temperature and soaking time. The results showed that cordierite together with spinel, diopside and clinoenstatite neoformed. SEM analysis revealed heterogeneous aspects. The results of the response surface methodology showed that the variations of physical properties versus processing parameters were well described by the used polynomial model. The addition of pore forming agent and temperature were the most influential factors. Filtration tests were performed on the best performing sample. The results allowed to testify that these membranes could be used in waste water treatment.

  3. 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.

  4. Enhancing BWR proliferation resistance fuel with minor actinides

    Science.gov (United States)

    Chang, Gray S.

    2009-03-01

    To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced light water reactor- LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides ( 237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu/Pu. For future advanced nuclear systems, 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. As a result, 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. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO 2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate-term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm 3) to the top (0.35 g/cm 3) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. The concept of MARA, which involves the use of transuranic nuclides ( 237Np and/or 241Am), 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

  5. 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

  6. Silica-based waste form for immobilization of iodine from reprocessing plant off-gas streams

    Energy Technology Data Exchange (ETDEWEB)

    Matyáš, Josef; Canfield, Nathan; Sulaiman, Sannoh; Zumhoff, Mac

    2016-08-01

    A high selectivity and sorption capacity for iodine and a feasible consolidation to a durable SiO2-based waste form makes silver-functionalized silica aerogel (Ag0-aerogel) an attractive choice for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. Hot uniaxial pressing of iodine-loaded Ag0-aerogel (20.2 mass% iodine) at 1200°C for 30 min under 29 MPa pressure provided a partially sintered product with residual open porosity of 16.9% that retained ~93% of sorbed iodine. Highly iodine-loaded Ag0-aerogel was successfully consolidated by hot isostatic pressing at 1200°C with a 30-min hold and under 207 MPa. The fully densified waste form had a bulk density of 3.3 g/cm3 and contained ~39 mass% iodine. The iodine was retained in the form of nano- and micro-particles of AgI that were uniformly distributed inside and along boundaries of fused silica grains.

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

    Energy Technology Data Exchange (ETDEWEB)

    Rostaing, C.; Baron, P.; Warin, D.; Duhamet, J.; Ochem, D. [CEA, Bagnols sur Ceze, Gard 30207 (France)

    2009-06-15

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

  8. 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.

  9. A conceptual performance assessment model of the dissolved actinide source term for the WIPP

    Energy Technology Data Exchange (ETDEWEB)

    Weiner, R.F.; Stockman, C.T.; Wang, Y.; Novak, C.F.

    1996-12-31

    This paper presents a performance assessment model of dissolved actinide concentrations for the Waste Isolation Pilot Plant (WIPP). The model assesses the concentration of each actinide oxidation state and combines these concentrations with an oxidation state distribution. The chemical behavior of actinides in the same oxidation state is presumed to be very similar for almost all situations, but exceptions arising from experimental evidence are accommodated. The code BRAGFLO calculates the gas pressure, brine mass, gas volume, and mass of remaining Fe and cellulosics for each time step and computational cell. The total CO{sub 2} in the repository and dissolved Ca(OH){sub 2} is estimated. Lookup tables are constructed for pmH and f(CO{sub 2}) as a function of brine type and volume, moles of CO{sub 2}, and Ca(OH){sub 2}. Amounts of five soluble complexants are considered. A model based on the formulation of Harvie et al. produces tables of solubilities for each actinide oxidation state as a function of pmH, f(CO{sub 2}), brine composition, and complexant. Experimental data yield lookup tables of fractions of Th, U, Np, Pu, and Am in each oxidation state as a function of f(CO{sub 2}) and complexant. The tables are then used to provide a concentration of a particular actinide at particular values of pmH and f(CO{sub 2}). Under steady-state conditions, the oxidation state of each actinide that is most stable in the particular chemical environment controls the concentration of that actinide in solution. In the absence of steady-state conditions, the oxidation state distribution of interest is that of the dissolved actinide, and the oxidation states may be treated as if they were separate compounds.

  10. CLADDING DEGRADATION COMPONENT IN WASTE FORM DEGRADATION MODEL IN TSPA-SR

    Energy Technology Data Exchange (ETDEWEB)

    E. Siegmann; R.P. Rechard

    2001-01-19

    The U.S. Department of Energy (DOE) has prepared a total system performance assessment for a site recommendation (TSPA-SR), if suitable, on Yucca Mountain for disposal of radioactive waste. Discussed here is the Cladding Degradation Component of the Waste Form Degradation Model (WF Model), of the TSPA-SR. The Cladding Degradation Component determines the degradation rate of the Zircaloy cladding on commercial spent nuclear fuel (CSNF) and, thereby, the CSNF matrix exposed and radioisotopes available for dissolution in any water present. Since the 1950s, most CSNF has been clad with less than 1 mm (usually between 600 and 900 {micro}m) of Zircaloy, a zirconium alloy. Zircaloy cladding is not a designed engineered barrier of the Yucca Mountain disposal system, but rather is an existing characteristic of the CSNF that is important to determining the release rate of radioisotopes once the waste package (WP) has breached. Although studies of cladding degradation from fluoride [F] began at Lawrence Livermore National Laboratory as early as 1984, cladding as a characteristic of the waste was not considered in TSPAs, conducted in the early 1990s. However, enough information on cladding performance has accumulated in the literature such that cladding was considered in 1993 when examining the performance of DOE spent nuclear (DSNF) and most recently in TSPA for the viability assessment (TSPA-VA). The Nuclear Regulatory Commission (NRC) currently uses cladding data as the basis for extending the period of wet storage, for licensing dry storage facilities, and for licensing shipping casks for CNSF.

  11. Final Project Report CFA-14-6357: A New Paradigm for Understanding Multiphase Ceramic Waste Form Performance

    Energy Technology Data Exchange (ETDEWEB)

    Brinkman, Kyle [Clemson Univ., SC (United States); Bordia, Rajendra [Clemson Univ., SC (United States); Reifsnider, Kenneth [Univ. of South Carolina, Columbia, SC (United States); Chiu, Wilson [Univ. of Connecticut, Storrs, CT (United States); Amoroso, Jake [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2017-12-28

    This project fabricated model multiphase ceramic waste forms with processing-controlled microstructures followed by advanced characterization with synchrotron and electron microscopy-based 3D tomography to provide elemental and chemical state-specific information resulting in compositional phase maps of ceramic composites. Details of 3D microstructural features were incorporated into computer-based simulations using durability data for individual constituent phases as inputs in order to predict the performance of multiphase waste forms with varying microstructure and phase connectivity.

  12. Cement-based radioactive waste hosts formed under elevated temperatures and pressures (FUETAP concretes) for Savannah River Plant high-level defense waste

    Energy Technology Data Exchange (ETDEWEB)

    Dole, L.R.; Rogers, G.C.; Morgan, M.T.; Stinton, D.P.; Kessler, J.H.; Robinson, S.M.; Moore, J.G.

    1983-03-01

    Concretes that are formed under elevated temperatures and pressures (called FUETAP) are effective hosts for high-level radioactive defense wastes. Tailored concretes developed at the Oak Ridge National Laboratory (ORNL) have been prepared from common Portland cements, fly ash, sand, clays, and waste products. These concretes are produced by accelerated curing under mild autoclave conditions (85 to 200/sup 0/C, 0.1 to 1.5 MPa) for 24 h. The solids are subsequently dewatered (to remove unbound water) at 250/sup 0/C for 24 h. The resulting products are strong (compressive strength, 40 to 100 MPa), leach resistant (plutonium leaches at the rate of 10 pg/(cm/sup 2/.d)), and radiolytically stable, monolithic waste forms (total gas value = 0.005 molecule/100 eV). This report summarizes the results of a 4-year FUETAP development program for Savannah River Plant (SRP) high-level defense wastes. It addresses the major questions concerning the performance of concretes as radioactive waste forms. These include leachability, radiation stability, thermal stability, thermal conductivity, impact strength, permeability, phase complexity, and effect of waste composition.

  13. Storing Waste in Ceramic

    Energy Technology Data Exchange (ETDEWEB)

    Bourcier, W L; Sickafus, K

    2004-07-20

    result of waste processing. A number of ceramic waste forms have been developed that minimize these problems and provide a potentially useful host for radionuclides. For ceramics, the mineralogy can be tailored to the waste stream by selecting solid mineral phases with structural sites that can accommodate the waste elements, as well as newly formed radioactive decay elements. Radiation damage can be minimized by selecting mineral phases that allow atoms to renew or regain their original crystalline structure, a process known as annealing. For example, actinide phosphate minerals anneal more readily than actinide silicate minerals. Despite the superior thermodynamic stability of crystalline materials, borosilicate glasses have become the preferred waste forms. One reason is that the processing technologies associated with this glass are believed to be easier to adapt to handling highly radioactive material.

  14. 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

  15. 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.

  16. Aqueous recovery of actinides from aluminum alloys

    Energy Technology Data Exchange (ETDEWEB)

    Gray, J.H.; Chostner, D.F.; Gray, L.W.

    1989-01-01

    Early in the 1980's, a joint Rocky Flats/Savannah River program was established to recover actinides from scraps and residues generated during Rocky Flats purification operations. The initial program involved pyrochemical treatment of Molten Salt Extraction (MSE) chloride salts and Electrorefining (ER) anode heel metal to form aluminum alloys suitable for aqueous processing at Savannah River. Recently Rocky Flats has expressed interest in expanding the aluminum alloy program to include treatment of chloride salt residues from a modified Molten Salt Extraction process and from the Electrorefining purification operations. Samples of the current aluminum alloy buttons were prepared at Rocky Flats and sent to Savannah River Laboratory for flowsheet development and characterization of the alloys. A summary of the scrub alloy-anode heel alloy program will be presented along with recent results from aqueous dissolution studies of the new aluminum alloys. 2 figs., 4 tabs.

  17. Specific sequestering agents for iron and the actinides

    Energy Technology Data Exchange (ETDEWEB)

    Raymond, K.N.

    1983-06-01

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

  18. 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

  19. 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.

  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. 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.

  2. Development of methodology to evaluate microbially influenced degradation of cement-solidified low-level radioactive waste forms

    Energy Technology Data Exchange (ETDEWEB)

    Rogers, R.D.; Hamilton, M.A.; Veeh, R.H.; McConnell, J.W. [Idaho National Engineering Lab., Idaho Falls, ID (United States)

    1994-12-31

    Because of its apparent structural integrity, cement has been widely used in the United States as a binder to solidify Class B and C low-level radioactive waste (LLW). However, the resulting cement preparations are susceptible to failure due to the actions of stress and environment. An environmentally mediated process that could affect cement stability is the action of naturally occurring microorganisms. The US Nuclear Regulatory Commission (NRC), recognizing this eventuality, stated that the effects of microbial action on waste form integrity must be addressed. This paper provides present results from an ongoing program that addresses the effects of microbially influenced degradation (MID) on cement-solidified LLW. Data are provided on the development of an evaluation method using acid-producing bacteria. Results are from work with one type of these bacteria, the sulfur-oxidizing Thiobacillus. This work involved the use of a system in which laboratory- and vendor-manufactured, simulated waste forms were exposed on an intermittent basis to media containing thiobacilli. Testing demonstrated that MID has the potential to severely compromise the structural integrity of ion-exchange resin and evaporator-bottoms waste that is solidified with cement. In addition, it was found that a significant percentage of calcium and other elements were leached from the treated waste forms. Also, the surface pH of the treated specimens decreased to below 2. These conditions apparently contributed to the physical deterioration of simulated waste forms after 60 days of exposure to the thiobacilli.

  3. 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.

  4. 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

  5. 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.

  6. Calculated Atomic Volumes of the Actinide Metals

    DEFF Research Database (Denmark)

    Skriver, H.; Andersen, O. K.; Johansson, B.

    1979-01-01

    The equilibrium atomic volume is calculated for the actinide metals. It is possible to account for the localization of the 5f electrons taking place in americium.......The equilibrium atomic volume is calculated for the actinide metals. It is possible to account for the localization of the 5f electrons taking place in americium....

  7. 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

  8. 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.

  9. 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

  10. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Pet' kov, Vladimir; Asabina, Elena, E-mail: e.a.asabina@gmail.com; Loshkarev, Vladimir; Sukhanov, Maksim

    2016-04-01

    We have summarized our data and literature ones on the thermophysical properties and hydrolytic stability of Sr{sub 0.5}Zr{sub 2}(PO{sub 4}){sub 3} compound as a host NaZr{sub 2}(PO{sub 4}){sub 3}-type (NZP) structure for immobilization of {sup 90}Sr-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 Sr{sub 0.5}Zr{sub 2}(PO{sub 4}){sub 3}. Calculated values of thermal conductivity coefficients at zero porosity in the range 298–673 K were 1.86–2.40 W·m{sup −1} K{sup −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 Sr{sup 2+} 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 Sr{sup 2+} ions into distilled water. Feeble sinterability constrains practical applications of NZP substances, that is why known in literature methods of Sr{sub 0.5}Zr{sub 2}(PO{sub 4}){sub 3} dense ceramics obtaining have been reviewed. - Graphical abstract: The ability of Sr{sub 0.5}Zr{sub 2}(PO{sub 4}){sub 3} using as a perspective nuclear waste form, resistant to radiation damage, has been investigated. The obtained results highlight several concerns with application of Sr{sub 0.5}Zr{sub 2}(PO{sub 4}){sub 3} material as a host matrix, which is stable to extreme environmental condition action and able to include 90Sr radioisotope into insoluble framework structure. - Highlights: • The ability of Sr{sub 0.5}Zr{sub 2}(PO{sub 4}){sub 3} using as a nuclear waste form was investigated. • Its heat capacity, thermal expansion and thermal conductivity were studied. • Its stability in distilled water, aggressive (acid and alkaline) media was

  12. M3FT-17OR0301070211 - Preparation of Hot Isostatically Pressed AgZ Waste Form Samples

    Energy Technology Data Exchange (ETDEWEB)

    Jubin, Robert Thomas [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Bruffey, Stephanie H. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Jordan, Jacob A. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2017-10-01

    The production of radioactive iodine-bearing waste forms that exhibit long-term stability and are suitable for permanent geologic disposal has been the subject of substantial research interest. One potential method of iodine waste form production is hot isostatic pressing (HIP). Recent studies at Oak Ridge National Laboratory (ORNL) have investigated the conversion of iodine-loaded silver mordenite (I-AgZ) directly to a waste form by HIP. ORNL has performed HIP with a variety of sample compositions and pressing conditions. The base mineral has varied among AgZ (in pure and engineered forms), silver-exchanged faujasite, and silverexchanged zeolite A. Two iodine loading methods, occlusion and chemisorption, have been explored. Additionally, the effects of variations in temperature and pressure of the process have been examined, with temperature ranges of 525°C–1,100°C and pressure ranges of 100–300 MPa. All of these samples remain available to collaborators upon request. The sample preparation detailed in this document is an extension of that work. In addition to previously prepared samples, this report documents the preparation of additional samples to support stability testing. These samples include chemisorbed I-AgZ and pure AgI. Following sample preparation, each sample was processed by HIP by American Isostatic Presses Inc. and returned to ORNL for storage. ORNL will store the samples until they are requested by collaborators for durability testing. The sample set reported here will support waste form durability testing across the national laboratories and will provide insight into the effects of varied iodine content on iodine retention by the produced waste form and on potential improvements in waste form durability provided by the zeolite matrix.

  13. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Westsik, Joseph H. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Serne, R. Jeffrey [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Pierce, Eric M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Cozzi, Alex [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Chung, Chul-Woo [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Swanberg, David J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    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.

  15. Neutron-induced capture cross sections of short-lived actinides with the surrogate reaction method

    Directory of Open Access Journals (Sweden)

    Gunsing F.

    2010-03-01

    Full Text Available Determination of neutron-capture cross sections of short-lived nuclei is opening the way to understand and clarify the properties of many nuclei of interest for nuclear structure physics, nuclear astrophysics and particularly for transmutation of nuclear wastes. The surrogate approach is well-recognized as a potentially very useful method to extract neutron cross sections for low-energy compound-nuclear reactions and to overcome the difficulties related to the target radioactivity. In this work we will assess where we stand on these neutron-capture cross section measurements and how we can achieve the short-lived Minor Actinides nuclei involved in the nuclear fuel cycle. The CENBG collaboration applied the surrogate method to determine the neutron-capture cross section of 233Pa (T1/2 = 27 d. The 233Pa (n,γ cross section is then deduced from the measured gamma decay probability of 234Pa compound nucleus formed via the surrogate 232Th(3He,p reaction channel. The obtained cross section data, covering the neutron energy range 0.1 to 1 MeV, have been compared with the predictions of the Hauser-Feshbach statistical model. The importance of establishing benchmarks is stressed for the minor actinides region. However, the lack of desired targets led us to propose recently the 174Yb (3He,pγ reaction as a surrogate reaction for the (n,γ predetermined benchmark cross section of 175Lu. An overview of the experimental setup combining gamma ray detectors such as Ge and C6D6 in coincidence with light charged particles ΔE-E Telescopes will be presented and preliminary results will be discussed.

  16. 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

  17. Polyoxometalates for Radioactive Waste Treatment - Final Report - 06/15/1996 - 09/14/2000

    Energy Technology Data Exchange (ETDEWEB)

    Pope, Michael T.

    2000-09-14

    The research was directed primarily towards the use of polyoxometalate complexes for separation of lanthanide, actinide, and technetium species from aqueous waste solutions, such as the Hanford Tank Wastes. Selective binding of these species responsible for much of the high level waste (HWL) activity, can reduce the volume of material to be subsequently vitrified or otherwise converted for long-term storage. A secondary objective was to explore the direct conversion of the polyoxometalate complexes into possible waste forms, oxide bronzes, thereby avoiding additional handling and energy-intensive vitrification procedures. Although the advantages of polyoxometalate anions (POMs) lie in their high thermal and radiolytical stabilities, that has been no attempt to exploit the remarkable variety of these complexes beyond the use of the two anions mentioned above. Our broad knowledge of POM chemistry has allowed us to address and rectify this omission. The innovative aspects of the project are: (a) the selective sequestration of lanthanide and actinide cations by a POM system in the presence of excess alkali and transition metal cations; (b) the formation of the first examples of POM complexes of UO2-2+ and their extraction into nonaqueous solvents; (c) the thermal conversion of ammonium salts of lanthanide and actinide POM complexes into inert oxide bronzes at relatively low temperatures; and (d) the direct formation of highly thermally-robust niobate and tantalate complexes of Re (surrogate for Tc) in highly basic solutions.

  18. Comparison of leaching Behavior of {sup 137}Cs and {sup 60}Co in the Simulated Paraffin Waste Form

    Energy Technology Data Exchange (ETDEWEB)

    Kwak, Kyoung-Kil; Ji, Young-Yong; Ryu, Young-Gerl; Kim, Ki-Hong [Korea Atomic Energy Research Institute, Taejon (Korea, Republic of)

    2006-07-01

    The evaluation on the leachability of waste form incorporated various radionuclides, plays an important role in the development of solidification matrix, safety analysis for the choice of the suitable waste management system, and quality assurance of the waste treatment process (installations). Various foreign countries have been developed and standardized the leaching test method compatible to their social circumstances because the results of leaching test are very important in quality control of waste forms and in the comparison of results obtained from many laboratories. The leaching test methods can be classified according to the purpose for use, the interval period of renewal of leachant, and the mixing existence of leachant. In this study, the leaching test were performed for the paraffin waste forms Incorporated {sup 60}Co and {sup 137}Cs by using HEPSE method, ANS 16.1 which are popular in IAEA, USA. Those 2 tests are different in the exposing area to the leachant, the number of renewal of leachant, the total leaching time, the presentation (or calculation) of the leaching results, and type of leachant. And we evaluated the leaching test results with the semi-infinitive diffusion model.

  19. 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.

  20. 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

  1. 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.

  2. 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

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

    Science.gov (United States)

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

    1985-06-01

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

  4. Actinide partitioning studies using dihexyl-N,N-diethycarbamolymehtyl phosphonate and dissolved zirconium calcine

    Energy Technology Data Exchange (ETDEWEB)

    Brewer, K.N.; Herbst, R.S.; Law, J.D.; Garn, T.G.; Tillotson, R.D.; Todd, T.A.

    1996-01-01

    A baseline flowsheet capable of partitioning the transuranic (TRU) elements from dissolved zirconium calcines has been developed. The goal of the TRU partitioning process is to remove the TRUs from solutions of dissolved zirconium calcines to below the 10 CFR 61.55 Class A waste limit of 10 nCi/g. Extraction, scrub, strip, and wash distribution coefficients for several elements, including the actinides, were measured in the laboratory by performing equal volume batch contacts. A solvent containing diheyl-N, N- diethylcarbamoylmethyl phosphonate (CMP), tributylphosphate (TBP), and a branched chain hydrocarbon as the diluent were used to develop this process. A non-radioactive zirconium pilot-plant calcine was spiked with the TRUs, U, Tc, or a radioactive isotope of zirconium to simulate the behavior of these elements in actual dissolved zirconium calcine feed. Distribution coefficient data obtained from laboratory testing were used to recommend: (1) solvent composition, (2) scrub solutions capable of selectively removing extracted zirconium while minimizing actinide recycle, (3) optimized strip solutions which quantitatively recover extracted actinides, and (4) feed adjustments necessary for flowsheet efficiency. Laboratory distribution coefficients were used in conjunction with the Generic TRUEX Model (GTM) to develop and recommend a flowsheet for testing in the 5.5-cm Centrifugal Contractor Mockup. GTM results indicate that the recommended flowsheet should remove the actinides from dissolved zirconium calcine feed to below the Class A waste limit of 10 nCi/g. Less than 0.01 wt% of the extracted zirconium will report to the high- activity waste (HAW) fraction using the 0.05 M H{sub 2}C{sub 2}O{sub 4} in 3.0 M HNO{sub 3} scrub, and greater than 99% of the extracted actinides are recovered with 0.001 M HEDPA.

  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. Copyright © 2016 Elsevier B.V. All rights reserved.

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

    Energy Technology Data Exchange (ETDEWEB)

    Jang, J.G.; Park, S.M.; Lee, H.K., E-mail: haengki@kaist.ac.kr

    2016-11-15

    Highlights: • Physical immobilization of radionuclides in geopolymer was quantitatively assessed. • Fly ash-based geopolymer showed excellent immobilization performance. • Diffusivity of soluble Cs and Sr was highly correlated with critical pore diameter. - Abstract: 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{sup 3} and 10{sup 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.

  7. 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.

  8. 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).

  9. Spin and orbital moments in actinide compounds

    DEFF Research Database (Denmark)

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

    1991-01-01

    The extended spatial distribution of both the transition-metal 3d electrons and the actinide 5f electrons results in a strong interaction between these electron states when the relevant elements are alloyed. A particular interesting feature of this hybridization, which is predicted by single-electron...... band-structure calculations, is that the orbital moments of the actinide 5f electrons are considerably reduced from the values anticipated by a simple application of Hund's rules. To test these ideas, and thus to obtain a measure of the hybridization, we have performed a series of neutron scattering...... 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...

  10. 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.

  11. Forms of avoidance and care of waste as subject of legal regulation

    Directory of Open Access Journals (Sweden)

    Šogorov Stevan

    2011-01-01

    Full Text Available Identification of subject of legal regulation of waste as part of environmental protection law is main goal of this article. Author's starting position is that creation of waste is necessary side product of process of humanization of nature and he points out most important methods for solving that problem. Hierarchy of priorities of solving problem of waste is considered as important. First priority is avoidance of creation of waste, second priority is its material and energetic use, and finally its disposal. Relevant provisions of Waste managing Act of Republic of Serbia of 2009 are argument for acceptance of that hierarchy. Yet there are possible and acceptable exceptions regarding application of existing hierarchy and they represent final part of this article.

  12. DURABILITY TESTING OF FLUIDIZED BED STEAM REFORMER WASTE FORMS FOR SODIUM BEARING WASTE AT IDAHO NATIONAL LABORATORY

    Energy Technology Data Exchange (ETDEWEB)

    Crawford, C; Carol Jantzen, C

    2007-08-27

    Fluidized Bed Steam Reforming (FBSR) processing of Sodium Bearing Waste simulants was performed in December 2006 by THOR{sup sm} Treatment Technologies LLC (TTT) The testing was performed at the Hazen Research Inc. (HRI) pilot plant facilities in Golden, CO. FBSR products from these pilot tests on simulated waste representative of the SBW at the Idaho Nuclear Technology and Engineering Center (INTEC) were subsequently transferred to the Savannah River National Laboratory (SRNL) for characterization and leach testing. Four as-received Denitration and Mineralization Reformer (DMR) granular/powder samples and four High Temperature Filter (HTF) powder samples were received by SRNL. FBSR DMR samples had been taken from the ''active'' bed, while the HTF samples were the fines collected as carryover from the DMR. The process operated at high fluidizing velocities during the mineralization test such that nearly all of the product collected was from the HTF. Active bed samples were collected from the DMR to monitor bed particle size distribution. Characterization of these crystalline powder samples shows that they are primarily Al, Na and Si, with > 1 wt% Ca, Fe and K. The DMR samples contained less than 1 wt% carbon and the HTF samples ranged from 13 to 26 wt% carbon. X-ray diffraction analyses show that the DMR samples contained significant quantities of the Al{sub 2}O{sub 3} startup bed. The DMR samples became progressively lower in starting bed alumina with major Na/Al/Si crystalline phases (nepheline and sodium aluminosilicate) present as cumulative bed turnover occurred but 100% bed turnover was not achieved. The HTF samples also contained these major crystalline phases. Durability testing of the DMR and HTF samples using the ASTM C1285 Product Consistency Test (PCT) 7-day leach test at 90 C was performed along with several reference glass samples. Comparison of the normalized leach rates for the various DMR and HTF components was made with the

  13. Thermodynamic and Microstructural Mechanisms in the Corrosion of Advanced Ceramic Tc-bearing Waste Forms and Thermophysical Properties

    Energy Technology Data Exchange (ETDEWEB)

    Hartmann, Thomas [Univ. of Nevada, Las Vegas, NV (United States). Dept. of Mechanical Engineering

    2017-09-01

    Technetium-99 (Tc, t1/2 = 2.13x105 years) is a challenge from a nuclear waste perspective and is one of the most abundant, long-lived radioisotopes found in used nuclear fuel (UNF). Within the Hanford Tank Waste Treatment and Immobilization Plant, technetium volatilizes at typical glass melting temperature, is captured in the off-gas treatment system and recycled back into the feed to eventually increase Tc-loadings of the glass. The aim of this NEUP project was to provide an alternative strategy to immobilize fission technetium as durable ceramic waste form and also to avoid the accumulation of volatile technetium within the off gas melter system in the course of vitrifying radioactive effluents in a ceramic melter. During this project our major attention was turned to the fabrication of chemical durable mineral phases where technetium is structurally bond entirely as tetravalent cation. These mineral phases will act as the primary waste form with optimal waste loading and superior resistance against leaching and corrosion. We have been very successful in fabricating phase-pure micro-gram amounts of lanthanide-technetium pyrochlores by dry-chemical synthesis. However, upscaling to a gram-size synthesis route using either dry- or wet-chemical processing was not always successful, but progress can be reported on a variety of aspects. During the course of this 5-year NEUP project (including a 2-year no-cost extension) we have significantly enhanced the existing knowledge on the fabrication and properties of ceramic technetium waste forms.

  14. 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.

  15. Detection of the actinides and cesium from environmental samples

    Science.gov (United States)

    Snow, Mathew Spencer

    Detection of the actinides and cesium in the environment is important for a variety of applications ranging from environmental remediation to safeguards and nuclear forensics. The utilization of multiple different elemental concentrations and isotopic ratios together can significantly improve the ability to attribute contamination to a unique source term and/or generation process; however, the utilization of multiple elemental "signatures" together from environmental samples requires knowledge of the impact of chemical fractionation for various elements under a variety of environmental conditions (including predominantly aqueous versus arid conditions). The research reported in this dissertation focuses on three major areas: 1. Improving the understanding of actinide-mineral interactions at ultra-low concentrations. Chapter 2 reports a batch sorption and modeling study of Np(V) sorption to the mineral goethite from attomolar to micromolar concentrations. 2. Improving the detection capabilities for Thermal Ionization Mass Spectrometry (TIMS) analyses of ultra-trace cesium from environmental samples. Chapter 4 reports a new method which significantly improves the chemical yields, purification, sample processing time, and ultimately, the detection limits for TIMS analyses of femtogram quantities of cesium from a variety of environmental sample matrices. 3. Demonstrating how actinide and cesium concentrations and isotopic ratios from environmental samples can be utilized together to determine a wealth of information including environmental transport mechanisms (e.g. aqueous versus arid transport) and information on the processes which generated the original material. Chapters1, 3 and 5 demonstrate these principles using Pu, Am, Np, and Cs concentrations and isotopic ratios from contaminated soils taken near the Subsurface Disposal Area (SDA) of Idaho National Laboratory (INL) (a low level radioactive waste disposal site in southeastern Idaho).

  16. 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.

  17. Roadmap for disposal of Electrorefiner Salt as Transuranic Waste.

    Energy Technology Data Exchange (ETDEWEB)

    Rechard, Robert P. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Trone, Janis R. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Kalinina, Elena Arkadievna [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Wang, Yifeng [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Hadgu, Teklu [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Sanchez, Lawrence C. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

    2017-12-01

    The experimental breeder reactor (EBR-II) used fuel with a layer of sodium surrounding the uranium-zirconium fuel to improve heat transfer. Disposing of EBR-II fuel in a geologic repository without treatment is not prudent because of the potentially energetic reaction of the sodium with water. In 2000, the US Department of Energy (DOE) decided to treat the sodium-bonded fuel with an electrorefiner (ER), which produces metallic uranium product, a metallic waste, mostly from the cladding, and the salt waste in the ER, which contains most of the actinides and fission products. Two waste forms were proposed for disposal in a mined repository; the metallic waste, which was to be cast into ingots, and the ER salt waste, which was to be further treated to produce a ceramic waste form. However, alternative disposal pathways for metallic and salt waste streams may reduce the complexity. For example, performance assessments show that geologic repositories can easily accommodate the ER salt waste without treating it to form a ceramic waste form. Because EBR-II was used for atomic energy defense activities, the treated waste likely meets the definition of transuranic waste. Hence, disposal at the Waste Isolation Pilot Plant (WIPP) in southern New Mexico, may be feasible. This report reviews the direct disposal pathway for ER salt waste and describes eleven tasks necessary for implementing disposal at WIPP, provided space is available, DOE decides to use this alternative disposal pathway in an updated environmental impact statement, and the State of New Mexico grants permission.

  18. 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.

  19. Diversity of spore-forming bacteria in cattle manure, slaughterhouse waste and samples from biogas plants

    National Research Council Canada - National Science Library

    Bagge, E; Persson, M; Johansson, K-E

    2010-01-01

    .... In this study, the effect of the biogas process on Bacillus spp. and Clostridium spp. was investigated. We analysed 97 faecal samples, 20 slaughterhouse waste samples and 60 samples collected at different stages in the biogas process...

  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. Neutron-based measurements for nondestructive assay of minor actinides produced in nuclear power reactors

    Energy Technology Data Exchange (ETDEWEB)

    Stewart, J.E.; Eccleston, G.W.; Ensslin, N.; Cremers, T.L.; Foster, L.A.; Menlove, H.O.; Rinard, P.M.

    1996-10-01

    Because of their impacts on long-term storage of high-level radioactive waste and their value as nuclear fuels, measurement and accounting of the minor actinides produced in nuclear power reactors are becoming significant issues. This paper briefly reviews the commercial nuclear fuel cycle with emphasis on reprocessing plants and key measurement points therein. Neutron signatures and characteristics are compared and contrasted for special nuclear materials (SNMs) and minor actinides (MAs). The paper focuses on application of neutron-based nondestructive analysis (NDA) methods that can be extended for verification of MAs. We describe current IAEA methods for NDA of SNMs and extension of these methods to satisfy accounting requirements for MAs in reprocessing plant dissolver solutions, separated products, and high-level waste. Recommendations for further systems studies and development of measurement methods are also included.

  2. 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).

  3. 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)

  4. 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.

  5. 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.

  6. 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.

  7. Workshop on the leaching mechanisms of nuclear-waste forms, October 27-28, 1981. Summary report

    Energy Technology Data Exchange (ETDEWEB)

    Mendel, J.E. (comp.)

    1982-04-01

    The purpose of this informal workshop was to initiate the program and achieve the following goals: (1) acquaint laboratory investigators (data generators) with the needs of the mathematical modelers (data users). Session I was devoted to a tutorial by D.D. Jackson, mathematical modeler for the leaching mechanisms program, on PROTOCOL, a general case waste form leaching model; (2) define important testing parameters, based on the present state of knowledge. To achieve this, a number of important testing parameters were identified for special discussion in Session II; (3) develop an understanding of the interrelationships between the activities of leaching mechanisms program participants, and begin definition of the specific role of each participant in the overall program; and (4) establish good communication between the leaching mechanisms program and related programs, particularly the waste form leaching program at the Savannah River Laboratory (SRL) and the various Nuclear Waste Terminal Storage (NWTS) waste package programs. The agenda for the workshop is attached as Appendix A; a list of attendees is in Appendix B. Because this workshop was devoted to preliminary planning for the leaching mechanisms program, the presentations and discussions were purposely kept informal. This report represents a synopsis of the proceedings that has been prepared by the leaching mechanisms coordinator and reviewed by the workshop participants.

  8. Strategic Design and Optimization of Inorganic Sorbents for Cesium, Strontium and Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Maginn, Edward J.

    2005-07-01

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

  9. 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.

  10. 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)

  11. 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.

  12. Spent nuclear fuel as a waste form for geologic disposal: Assessment and recommendations on data and modeling needs

    Energy Technology Data Exchange (ETDEWEB)

    Van Luik, A.E.; Apted, M.J.; Bailey, W.J.; Haberman, J.H.; Shade, J.S.; Guenther, R.E.; Serne, R.J.; Gilbert, E.R.; Peters, R.; Williford, R.E.

    1987-09-01

    This study assesses the status of knowledge pertinent to evaluating the behavior of spent nuclear fuel as a waste form in geologic disposal systems and provides background information that can be used by the DOE to address the information needs that pertain to compliance with applicable standards and regulations. To achieve this objective, applicable federal regulations were reviewed, expected disposal environments were described, the status of spent-fuel modeling was summarized, and information regarding the characteristics and behavior of spent fuel was compiled. This compiled information was then evaluated from a performance modeling perspective to identify further information needs. A number of recommendations were made concerning information still needed to enhance understanding of spent-fuel behavior as a waste form in geologic repositories. 335 refs., 22 figs., 44 tabs.

  13. Report on Intact and Degraded Criticality for Selected Plutonium Waste Forms in a Geologic Repository, Volume I: MOX SNF

    Energy Technology Data Exchange (ETDEWEB)

    J.A. McClure

    1998-09-21

    As part of the plutonium waste form development and down-select process, repository analyses have been conducted to evaluate the long-term performance of these forms for repository acceptance. Intact and degraded mode criticality analysis of the mixed oxide (MOX) spent fuel is presented in Volume I, while Volume II presents the evaluations of the waste form containing plutonium immobilized in a ceramic matrix. Although the ceramic immobilization development program is ongoing, and refinements are still being developed and evaluated, this analysis provides value through quick feed-back to this development process, and as preparation for the analysis that will be conducted starting in fiscal year (FY) 1999 in support of the License Application. While no MOX fuel has been generated in the United States using weapons-usable plutonium, Oak Ridge National Laboratory (ORNL) has conducted calculations on Westinghouse-type reactors to determine the expected characteristics of such a fuel. These spent nuclear fuel (SNF) characteristics have been used to determine the long-term potential for criticality in a repository environment. In all instances the methodology and scenarios used in these analyses are compatible with those developed and used for Commercial Spent Nuclear Fuel (CSNF) and Defense High Level Waste (DHLW), as tailored for the particular characteristics of the waste forms. This provides a common basis for comparison of the results. This analysis utilizes dissolution, solubility, and thermodynamic data that are currently available. Additional data on long-term behavior is being developed, and later analyses (FY 99) to support the License Application will use the very latest information that has been generated. Ranges of parameter values are considered to reflect sensitivity to uncertainty. Most of the analysis is focused on those parameter values that produce the worst case results, so that potential licensing issues can be identified.

  14. 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)

  15. Technical justifications for the tests and criteria in the waste form technical position appendix on cement stabilization

    Energy Technology Data Exchange (ETDEWEB)

    Siskind, B.; Cowgill, M.G.

    1992-01-01

    As part of its technical assistance to the Nuclear Regulatory Commission (NRC), Brookhaven National Laboratory (BNL) developed a background document for the cement stabilization appendix, Appendix A, to Rev. 1 of the Technical Position on Waste Form (TP). Here we present an overview of this background document, which provides technical justification for the stability tests to be performed on cement-stabilized waste forms and for the criteria posed in each test, especially for those tests which have been changed from their counterparts in the May 1983 Rev. 0 TP. We address guidelines for procedures from Appendix A which are considered in less detail or not at all in the Rev. 0 of the TP, namely, qualification specimen preparation (mixing, curing, storage), statistical sampling and analysis, process control program specimen preparation and examination, and surveillance specimens. For each waste form qualification test, criterion or procedural guidelines, we consider the reason for its inclusion in Appendix A, the changes from Rev. 0 of the TP (if applicable), and a discussion of the justification or rationale for these changes.

  16. Technical justifications for the tests and criteria in the waste form technical position appendix on cement stabilization

    Energy Technology Data Exchange (ETDEWEB)

    Siskind, B.; Cowgill, M.G.

    1992-04-01

    As part of its technical assistance to the Nuclear Regulatory Commission (NRC), Brookhaven National Laboratory (BNL) developed a background document for the cement stabilization appendix, Appendix A, to Rev. 1 of the Technical Position on Waste Form (TP). Here we present an overview of this background document, which provides technical justification for the stability tests to be performed on cement-stabilized waste forms and for the criteria posed in each test, especially for those tests which have been changed from their counterparts in the May 1983 Rev. 0 TP. We address guidelines for procedures from Appendix A which are considered in less detail or not at all in the Rev. 0 of the TP, namely, qualification specimen preparation (mixing, curing, storage), statistical sampling and analysis, process control program specimen preparation and examination, and surveillance specimens. For each waste form qualification test, criterion or procedural guidelines, we consider the reason for its inclusion in Appendix A, the changes from Rev. 0 of the TP (if applicable), and a discussion of the justification or rationale for these changes.

  17. 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.

  18. 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.)

  19. 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.

  20. Actinide bioimaging in tissues: Comparison of emulsion and solid track autoradiography techniques with the iQID camera.

    Directory of Open Access Journals (Sweden)

    Stephanie Lamart

    Full Text Available This work presents a comparison of three autoradiography techniques for imaging biological samples contaminated with actinides: emulsion-based, plastic-based autoradiography and a quantitative digital technique, the iQID camera, based on the numerical analysis of light from a scintillator screen. In radiation toxicology it has been important to develop means of imaging actinide distribution in tissues as these radionuclides may be heterogeneously distributed within and between tissues after internal contamination. Actinide distribution determines which cells are exposed to alpha radiation and is thus potentially critical for assessing absorbed dose. The comparison was carried out by generating autoradiographs of the same biological samples contaminated with actinides with the three autoradiography techniques. These samples were cell preparations or tissue sections collected from animals contaminated with different physico-chemical forms of actinides. The autoradiograph characteristics and the performances of the techniques were evaluated and discussed mainly in terms of acquisition process, activity distribution patterns, spatial resolution and feasibility of activity quantification. The obtained autoradiographs presented similar actinide distribution at low magnification. Out of the three techniques, emulsion autoradiography is the only one to provide a highly-resolved image of the actinide distribution inherently superimposed on the biological sample. Emulsion autoradiography is hence best interpreted at higher magnifications. However, this technique is destructive for the biological sample. Both emulsion- and plastic-based autoradiography record alpha tracks and thus enabled the differentiation between ionized forms of actinides and oxide particles. This feature can help in the evaluation of decorporation therapy efficacy. The most recent technique, the iQID camera, presents several additional features: real-time imaging, separate imaging of

  1. The Actinide-Lanthanide Separation Process

    Energy Technology Data Exchange (ETDEWEB)

    Lumetta, Gregg J.; Gelis, Artem V.; Carter, Jennifer C.; Niver, Cynthia M.; Smoot, Margaret R.

    2014-02-21

    The Actinide-Lanthanide SEParation (ALSEP) process is described. The process uses an extractant phase consisting of either N,N,N',N'-tetraoctyldiglycolamide (TODGA) or N,N,N',N'-tetra(2 ethylhexyl)diglycolamide (T2EHDGA) combined with 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]). The neutral TODGA or T2EHDGA serves to co-extract the trivalent actinide and lanthanide ions from nitric acid media. Switching the aqueous phase chemistry to a citrate buffered diethylenetriaminepentaacetic acid (DTPA) solution at pH 2.5 to 4 results in selective transfer of the actinides to the aqueous phase, thus resulting in separation of these two groups of elements.

  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.

    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.

  3. 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.

  4. 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)

  5. 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.

  6. Strategic Design and Optimization of Inorganic Sorbents for Cesium, Strontium and Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Clearfield, Abraham

    2005-07-01

    It has been determined that poorly crystalline CST and SNT prepared at low temperature (100-150 deg. C) exhibit much faster kinetics in uptake of Sr2+. 2. In-situ X-ray studies has shown that SNT is a precursor phase to the formation of CST. 3. It is possible to form mixtures of CST and SNT in a single reactant mix by control of temperature and time of reaction. 4. It has been found that addition of a small amount of Cs+ to the reactant mix for the preparation of Nb-CST allows formation of the crystals in one day rather than ten days at 200 deg. C. 5. These discoveries suggest that a proper mix of sorbents (SNT, CST, Nb-CST) can be made easily at low cost that would remove all the HLW at the Savannah River site with a single in-tank procedure. Research Objective The basic science goal in this project is to identify structure/affinity relationships for selected radionuclides and existing sorbents. The research will then apply this knowledge to the design and synthesis of sorbents that will exhibit increased cesium, strontium and actinide removal. The target problem focuses on the treatment of high-level nuclear wastes. The general approach can likewise be applied to non-radioactive separations.

  7. Strategic Design and Optimization of Inorganic Sorbents for Cesium, Strontium and Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Clearfield, Abraham

    2005-07-01

    It has been determined that poorly crystalline CST and SNT prepared at low temperature (100-150 C) exhibit much faster kinetics in uptake of Sr2+. In-situ X-ray studies has shown that SNT is a precursor phase to the formation of CST. It is possible to form mixtures of CST and SNT in a single reactant mix by control of temperature and time of reaction. It has been found that addition of a small amount of Cs+ to the reactant mix for the preparation of Nb-CST allows formation of the crystals in one day rather than ten days at 200 C. These discoveries suggest that a proper mix of sorbents (SNT, CST, Nb-CST) can be made easily at low cost that would remove all the HLW at the Savannah River site with a single in-tank procedure. The basic science goal in this project is to identify structure/affinity relationships for selected radionuclides and existing sorbents. The research will then apply this knowledge to the design and synthesis of sorbents that will exhibit increased cesium, strontium and actinide removal. The target problem focuses on the treatment of high-level nuclear wastes. The general approach can likewise be applied to non-radioactive separations.

  8. Hydroceramics, a ''new'' cementitious waste form material for U.S. defense-type reprocessing waste

    Energy Technology Data Exchange (ETDEWEB)

    Siemer, Darryl D.

    2002-09-01

    A ''hydroceramic'' (HC) is a concrete which possesses mineralogy similar to the zeolitized rock indigenous to the USA's current ''basis'' high level radioactive waste (HLW) repository site, Yucca Mountain (YM). It is made by curing a mixture of inorganic waste, calcined clay, vermiculite, Na{sub 2}S, NaOH, plus water under hydrothermal conditions. The product differs from conventional Portland cement and/or slag-based concretes (''grouts'') in that it is primarily comprised of alkali aluminosilicate ''cage minerals'' (cancrinites, sodalites, and zeolites)rather than hydrated calcium silicates (C-S-H in cement-chemistry shorthand). Consequently it microencapsulates individual salt molecules thereby rendering them less leachable than they are from conventional grouts. A fundamental difference between the formulations of HCs and radwaste-type glasses is that the latter contain insufficient aluminum to form insoluble minerals with all of the alkali metals in them. This means that the imposition of worst-case ''repository failure'' (hydrothermal) conditions would cause a substantial fraction of such glasses to alter to water-soluble forms. Since the same conditions tend to reduce the solubility of HC concretes, they constitute a more rugged immobilization sub-system. This paper compares leach characteristics of HCs with those of radwaste-type glasses and points out why hydroceramic solidification makes more sense than vitrification for US defense-type reprocessing waste. (orig.)

  9. Spin–orbit coupling in actinide cations

    DEFF Research Database (Denmark)

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

    2012-01-01

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

  10. 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.)

  11. Radioactive iodine waste (5) I-129 fixation by silica-coated zeolite distributed in extremely low solubility non-organic matrix-multi-layered distributed waste-form for I-129

    Energy Technology Data Exchange (ETDEWEB)

    Yanagisawa, Ichiro [Kobe Shipyard and Machinery Works, Mitsubishi Heavy Industries Ltd., Kobe, Hyogo (Japan); Izumi, Jun; Oka, Nobuki; Tomonaga, Nariyuki [Nagasaki Research and Development Center, Mitsubishi Heavy Industries Ltd., Ngasaki (Japan); Kitao, Hideo [Omiya Research and Development Department, Nuclear Development Corporation, Saitama (Japan); Neyama, Atsushi [Computer Software Development Co., Ltd., Tokyo (Japan); Katurai, Kiyomichi [Nuclear Systems Engineering Center, Mitsubishi Heavy Industries Ltd., Yokohama, Kanagawa (Japan)

    1999-12-01

    A multi-layered distributed waste-form concept for I-129 fixation has been proposed and experiments have been carried out in order to select iodine-bearing adsorbents. The goal of this waste-form development is to realize a very low releasing rate of I-129 for a long period of more than hundred thousands years. The waste-form consists of iodine-bearing zeolite particles and extremely low solubility matrix such as apatite. With a screening test of inorganic iodine adsorbents, Ca-Ag-A type zeolite (Ag exchange rate: 20%) was selected as a suitable iodine-bearing adsorbent. (author)

  12. 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.

  13. Glass-ceramic waste forms for immobilization of the fluorinel-sodium, alumina, and zirconia calcines stored at the Idaho Chemical Processing Plant

    Energy Technology Data Exchange (ETDEWEB)

    Vinjamuri, K. [Idaho National Engineering Lab., Idaho Falls, ID (United States)

    1994-12-31

    Glass-ceramics appear to be very good candidate waste forms for immobilization of the calcined high level solid wastes, fluorinel-sodium (Fl/Na), alumina and zirconia that are stored at the Idaho Chemical Processing Plant (ICPP). Candidate experimental glass-ceramics were synthesized at ICPP by hot isostatically pressing (HIPing) a mixture of precompacted pilot plant calcine and additives. The glass-ceramic waste forms for immobilization of the Fl/Na, alumina, and zirconia calcines consist of 70 wt% Fl/Na calcine, 23.9 wt% SiO{sub 2}, 5 wt% Ti, 1.1 wt% B{sub 2}O{sub 3}; 70 wt% alumina calcine, 30 wt% SiO{sub 2}; and 70 wt% zirconia calcine, 20.25 wt% SiO{sub 2}, 5 wt% Ti, 2.25 wt% Na{sub 2}O, 1.75 wt% B{sub 2}O{sub 3}, 0.75 wt% Li{sub 2}O, respectively. The characteristics of the waste forms including density, chemical durability, glass and crystalline phases, and the microstructure are investigated. The 14-day MCC-1 total mass loss rates and the normalized elemental leach rates for aluminum, boron, calcium, cadmium, chromium, cesium, potassium, silicon, sodium, strontium, titanium, and zirconium are all less than 1 g/m{sup 2}-day. The crystalline phases for the Fl/Na and zirconia waste forms include zirconia, zircon, calcium fluoride, and titanates. In addition, cadmium sulphide in Fl/Na, and cadmium metal in zirconia waste form were also identified. The crystalline phases for the alumina waste form are alpha, gamma, and delta alumina, cristobalite, albite, and mullite. Glass phase separation was not observed in alumina and zirconia waste forms. The observed glass phase separation in Fl/Na waste form appears to be chemically durable.

  14. The effects of actinide based fuels on incremental cross sections in a Candu reactor

    Energy Technology Data Exchange (ETDEWEB)

    Morreale, A.C.; Ball, M.R.; Novog, D.R.; Luxat, J.C., E-mail: morreaac@mcmaster.ca, E-mail: ballmr@mcmaster.ca, E-mail: novog@mcmaster.ca, E-mail: luxatj@mcmaster.ca [Department of Engineering Physics, McMaster University, Ontario (Canada)

    2011-07-01

    The reprocessing of spent fuel such as the extraction of actinide materials for use in mixed oxide fuels is a key component of reducing the end waste from nuclear power plant operations. Using recycled spent fuels in current reactors is becoming a popular option to help close the fuel cycle. In order to ensure safe and consistent operations in existing facilities, the properties of these fuels must be compatible with current reactor designs. This paper examines the features of actinide mixed oxide fuel, TRUMOX, in a CANDU reactor. Specifically, the effect of this fuel design on the incremental cross sections related to the use of adjuster rods is investigated. The actinide concentrations studied in this work were based on extraction from thirty year cooled spent fuel and mixed with natural uranium to yield a MOX fuel of 4.75% actinide by weight. The incremental cross sections were calculated using the DRAGON neutron transport code. The results for the actinide fuel were compared to those for standard natural uranium fuel and for a slightly enriched (1% U-235) fuel designed to reduce void reactivity. Adjuster reactivity effect calculations and void reactivity simulations were also performed. The impact of the adjuster on reactivity decreased by as much as 56% with TRUMOX fuel while the CVR was reduced by 71% due to the addition of central burnable poison. The incremental cross sections were largely affected by the use of the TRUMOX fuel primarily due to its increased level of fissile material (five times that of NU). The largest effects are in the thermal neutron group where the Σ{sub T} value is increased by 46.7%, the Σ{sub ny)} values increased by 13.0% and 9.9%. The value associated with thermal fission, υΣ{sub f}, increased by 496.6% over regular natural uranium which is expected due to the much higher reactivity of the fuel. (author)

  15. Actinide measurements by AMS using fluoride matrices

    Energy Technology Data Exchange (ETDEWEB)

    Cornett, R.J., E-mail: Jack.Cornett@uottawa.ca [André E. Lalonde AMS Laboratory, University of Ottawa, 150 Louis Pasteur, Ottawa, ON K1N 6N5 (Canada); Department of Earth Sciences, University of Ottawa, 150 Louis Pasteur, Ottawa, ON K1N 6N5 (Canada); Kazi, Z.H. [André E. Lalonde AMS Laboratory, University of Ottawa, 150 Louis Pasteur, Ottawa, ON K1N 6N5 (Canada); Department of Earth Sciences, University of Ottawa, 150 Louis Pasteur, Ottawa, ON K1N 6N5 (Canada); Zhao, X.-L. [André E. Lalonde AMS Laboratory, University of Ottawa, 150 Louis Pasteur, Ottawa, ON K1N 6N5 (Canada); Department of Physics, University of Ottawa, 150 Louis Pasteur, Ottawa, ON K1N 6N5 (Canada); Chartrand, M.G. [André E. Lalonde AMS Laboratory, University of Ottawa, 150 Louis Pasteur, Ottawa, ON K1N 6N5 (Canada); Department of Earth Sciences, University of Ottawa, 150 Louis Pasteur, Ottawa, ON K1N 6N5 (Canada); Charles, R.J.; Kieser, W.E. [André E. Lalonde AMS Laboratory, University of Ottawa, 150 Louis Pasteur, Ottawa, ON K1N 6N5 (Canada); Department of Physics, University of Ottawa, 150 Louis Pasteur, Ottawa, ON K1N 6N5 (Canada)

    2015-10-15

    Actinides can be measured by alpha spectroscopy (AS), mass spectroscopy or accelerator mass spectrometry (AMS). We tested a simple method to separate Pu and Am isotopes from the sample matrix using a single extraction chromatography column. The actinides in the column eluent were then measured by AS or AMS using a fluoride target matrix. Pu and Am were coprecipitated with NdF{sub 3}. The strongest AMS beams of Pu and Am were produced when there was a large excess of fluoride donor atoms in the target and the NdF{sub 3} precipitates were diluted about 6–8 fold with PbF{sub 2}. The measured concentrations of {sup 239,240}Pu and {sup 241}Am agreed with the concentrations in standards of known activity and with two IAEA certified reference materials. Measurements of {sup 239,240}Pu and {sup 241}Am made at A.E. Lalonde AMS Laboratory agree, within their statistical uncertainty, with independent measurements made using the IsoTrace AMS system. This work demonstrated that fluoride targets can produce reliable beams of actinide anions and that the measurement of actinides using fluorides agree with published values in certified reference materials.

  16. 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.)

  17. Electronic Structure of the Actinide Metals

    DEFF Research Database (Denmark)

    Johansson, B.; Skriver, Hans Lomholt

    1982-01-01

    itinerant to localized 5f electron behaviour calculated to take place between plutonium and americium. From experimental data it is shown that the screening of deep core-holes is due to 5f electrons for the lighter actinide elements and 6d electrons for the heavier elements. A simplified model for the full...

  18. Calculated Bulk Properties of the Actinide Metals

    DEFF Research Database (Denmark)

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

    1978-01-01

    Self-consistent relativistic calculations of the electronic properties for seven actinides (Ac-Am) have been performed using the linear muffin-tin orbitals method within the atomic-sphere approximation. Exchange and correlation were included in the local spin-density scheme. The theory explains t...

  19. Film-forming ability of collagen hydrolysate extracted from leather solid wastes with chitosan.

    Science.gov (United States)

    Ocak, Buğra

    2017-12-01

    Discharges of huge quantities of leather solid wastes by leather industries and the increased use of synthetic packaging films have raised serious concerns on account of their environmental impacts. The paper focuses on the development and characterization of potential environmentally friendly composite films using collagen hydrolysate (CH) extracted from leather solid wastes and chitosan (C) to assess the feasibility of producing polymeric materials suitable for applications in packaging and wrapping purposes. Solid collagen-based protein hydrolysate was extracted from chromium-tanned leather wastes and analyzed to determine its chemical properties. With the goal of improving the physico-chemical performance of CH, three types of composite films (CH75/C25, CH50/C50, CH25/C75) were prepared with increasing concentrations of C, and some of their physical and functional properties were characterized. The results indicated that the addition of C caused increase (p < 0.05) in the thickness, tensile strength (TS), elasticity modulus (EM), and water vapor permeability (WVP), leading to stronger films as compared with CH film, but significantly (p < 0.05) decreased the elongation at break (EAB) and solubility of films (p < 0.05). The light barrier measurements present low values of transparency at 600 nm of the CH/C films, indicating that the films are very transparent and they have excellent barrier properties against UV light. The structural properties investigated by FTIR and DSC showed total miscibility between both polymers. Scanning electron micrographs revealed that CH/C composite films showed a compact homogeneous structure. These results demonstrate the potential application of CH/C composite films in packaging industry.

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

    Science.gov (United States)

    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 characteristics of these colloids and the potential implication for their environmental behavior. The binary oxyhydroxy silicate colloids of AnIV could be potentially more mobile as a waterborne species than the well‐known mono‐component oxyhydroxide colloids. PMID:27957406

  1. 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.

  2. Emergence of interest groups on hazardous waste siting: how do they form and survive

    Energy Technology Data Exchange (ETDEWEB)

    Williams, R.G.; Payne, B.A.

    1985-10-30

    This paper discusses the two components of the facilitative setting that are important for group formation. The first component, the ideological component, provides the basic ideas that are adopted by the emerging group. The ideological setting for group formation is produced by such things as antinuclear news coverage and concentration of news stories on hazardous waste problems, on ideas concerning the credibility of the federal government, and on the pervasivensee of ideas about general environmental problems. The organizational component of the facilitative setting provides such things as leadership ability, flexible time, resources, and experience. These are important for providing people, organization, and money to achieve group goals. By and large, the conditions conducive to group formation, growth, and survival are outside the control of decision-makers. Agencies and project sponsors are currently caught in a paradox. Actively involving the public in the decision-making process tends to contribute to the growth and survival of various interest groups. Not involving the public means damage to credibility and conflict with values concerning participatory democracy. Resolution in this area can only be achieved when a comprehensive, coordinated national approach to hazardous waste management emerges. 26 refs.

  3. Investigation of hydrocarbon fractions form waste plastic recycling by FTIR, GC, EDXRFS and SEC techniques.

    Science.gov (United States)

    Miskolczi, N; Bartha, L

    2008-04-24

    Waste high-density polyethylene was converted into different hydrocarbon fractions by thermal and thermo-catalytic batch cracking. For the catalytic degradation of waste plastics three different catalysts (equilibrium FCC, HZSM-5 and clinoptilolite) were used. Catalysts differ basically in their costs and activity due to the differences of micro- and macroporous surface areas and furthermore the Si/Al ratio and acidities are also different. Mild pyrolysis was used at 430 degrees C and the reaction time was 45 min in each case. The composition of products was defined by gas chromatography, Fourier transform infrared spectroscopy, size exclusion chromatography, energy-dispersive X-ray fluorescence spectroscopy and other standardized methods. The effects of catalysts on the properties of degradation products were investigated. Both FCC and clinoptilolite catalysts had considerably catalytic activity to produce light hydrocarbon liquids, while HZSM-5 catalyst produced the highest amount of gaseous products. In case of liquids, carbon numbers were distributed within the C5-C23 range depending on the cracking parameters. Decomposition of the carbon chain could be followed by GC and both by FTIR and SEC techniques in case of volatile fractions and residues. Catalysts increased yields of valuable volatile fractions and moreover catalysts caused both carbon chain isomerization and switching of the position of double bonds.

  4. Candidate Low-Temperature Glass Waste Forms for Technetium-99 Recovered from Hanford Effluent Management Facility Evaporator Concentrate

    Energy Technology Data Exchange (ETDEWEB)

    Ding, Mei [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Tang, Ming [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Rim, Jung Ho [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Chamberlin, Rebecca M. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2017-07-24

    Alternative treatment and disposition options may exist for technetium-99 (99Tc) in secondary liquid waste from the Hanford Direct-Feed Low-Activity Waste (DFLAW) process. One approach includes development of an alternate glass waste form that is suitable for on-site disposition of technetium, including salts and other species recovered by ion exchange or precipitation from the EMF evaporator concentrate. By recovering the Tc content from the stream, and not recycling the treated concentrate, the DFLAW process can potentially be operated in a more efficient manner that lowers the cost to the Department of Energy. This report provides a survey of candidate glass formulations and glass-making processes that can potentially incorporate technetium at temperatures <700 °C to avoid volatilization. Three candidate technetium feed streams are considered: (1) dilute sodium pertechnetate loaded on a non-elutable ion exchange resin; (2) dilute sodium-bearing aqueous eluent from ion exchange recovery of pertechnetate, or (3) technetium(IV) oxide precipitate containing Sn and Cr solids in an aqueous slurry. From the technical literature, promising candidate glasses are identified based on their processing temperatures and chemical durability data. The suitability and technical risk of three low-temperature glass processing routes (vitrification, encapsulation by sintering into a glass composite material, and sol-gel chemical condensation) for the three waste streams was assessed, based on available low-temperature glass data. For a subset of candidate glasses, their long-term thermodynamic behavior with exposure to water and oxygen was modeled using Geochemist’s Workbench, with and without addition of reducing stannous ion. For further evaluation and development, encapsulation of precipitated TcO2/Sn/Cr in a glass composite material based on lead-free sealing glasses is recommended as a high priority. Vitrification of pertechnetate in aqueous anion exchange eluent solution

  5. 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.)

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-01-08

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

  7. 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.

  8. 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.

  9. 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.

  10. Physical, Chemical and Structural Evolution of Zeolite-Containing Waste Forms Produced from Metakaolinite and Calcined Sodium Bearing Waste (HLW and/or LLW)

    Energy Technology Data Exchange (ETDEWEB)

    Grutzeck, Michael W.

    2005-06-27

    Zeolites are extremely versatile. They can adsorb liquids and gases and serve as cation exchange media. They occur in nature as well cemented deposits. The ancient Romans used blocks of zeolitized tuff as a building material. Using zeolites for the management of radioactive waste is not a new idea, but a process by which the zeolites can be made to act as a cementing agent is. Zeolitic materials are relatively easy to synthesize from a wide range of both natural and man-made substances. The process under study is derived from a well known method in which metakaolin (an impure thermally dehydroxylated kaolinite heated to {approx}700 C containing traces of quartz and mica) is mixed with sodium hydroxide (NaOH) and reacted in slurry form (for a day or two) at mildly elevated temperatures. The zeolites form as finely divided powders containing micrometer ({micro}m) sized crystals. However, if the process is changed slightly and only just enough concentrated sodium hydroxide solution is added to the metakaolinite to make a thick crumbly paste and then the paste is compacted and cured under mild hydrothermal conditions (60-200 C), the mixture will form a hard ceramic-like material containing distinct crystalline tectosilicate minerals (zeolites and feldspathoids) imbedded in an X-ray amorphous hydrated sodium aluminosilicate matrix. Due to its lack of porosity and vitreous appearance we have chosen to call this composite a ''hydroceramic''.

  11. Synthetic murataite-3C, a complex form for long-term immobilization of nuclear waste. Crystal structure and its comparison with natural analogues

    Energy Technology Data Exchange (ETDEWEB)

    Pakhomova, Anna S.; Krivovichev, Sergey V. [St. Petersburg State Univ. (Russian Federation). Dept. of Crystallography; Yudintsev, Sergey V. [Institute of Geology of Ore Deposits, Petrography, Mineralogy and Geochemistry, St. Petersburg (Russian Federation); Stefanovsky, Sergey V. [MosNPO Radon, Moscow (Russian Federation)

    2013-03-01

    The structure of synthetic murataite-3C intended for long-term immobilization of high-level radioactive waste has been solved using crystals prepared by melting in an electric furnace at 1500 C. The material is cubic, F- anti 43m, a = 14.676(15) A, V = 3161.31(57) A{sup 3}. The structure is based upon a three-dimensional framework consisting of {alpha}-Keggin [Al{sup [4]}Ti{sub 12}{sup [6]}O{sub 40}] clusters linked by sharing the O5 atoms. The Keggin-cluster-framework interpenetrates with the metal-oxide substructure that can be considered as a derivative of the fluorite structure. The crystal chemical formula of synthetic murataite-3C derived from the obtained structure model can be written as {sup [8]}Ca{sub 6}{sup [8]}Ca{sub 4}{sup [6]}Ti{sub 12}{sup [5]}Ti{sub 4}{sup [4]}AlO{sub 42}. Its comparison with the natural murataite shows that the synthetic material has a noticeably less number of vacancies in the cation substructure and contains five instead of four symmetrically independent cation positions. The presence of the additional site essentially increases the capacity of synthetic murataite with respect to large heavy cations such as actinides, rare earth and alkaline earth metals in comparison with the material of natural origin. (orig.)

  12. 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. Copyright © 2014 Elsevier Ltd. All rights reserved.

  13. Elaboration of phosphate ceramics as a safe form for halide salt waste immobilization of `dry` fuel reprocessing

    Energy Technology Data Exchange (ETDEWEB)

    Orlova, A.I.; Petkov, V.I.; Egorkova, O.V.; Kurazhkovskaya, V.S.; Kemenov, D.V. [Nizhny Novgorod State Univ. Chemical Dept., Nizhny Novgorod (Russian Federation); Skiba, O.V.

    1997-12-31

    The conception of high level radwaste immobilization from M{sup 1}-containing molten salts and their solid forms into NZP-like structure phosphate ceramics are considered. The crystal-chemical principle on radionuclide incorporation into this structure is described. The prepared NZP ceramics was tested and it was shown that they had stability to action of such factors as temperature (up to 1200-1600degC), pressure (up to 500 MPa), radiation ({gamma}, up to 5{center_dot}10{sup 8} Gy), water solutions (up to 400degC, 60 MPa). Their structure is able to contain alkali elements up to 30-40%. Such monophase phosphate compositions may be formed at process of alkali chloride wastes solidification. The reactions of alkali chlorides, radionuclides, with phosphates are taken up here. (author)

  14. 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...

  15. 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.

  16. 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

  17. 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.)

  18. 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.

  19. Actinide uptake by transferrin and ferritin metalloproteins

    Energy Technology Data Exchange (ETDEWEB)

    Den Auwer, C.; Llorens, I.; Moisy, Ph. [CEA Marcoule DEN/DRCP/SCPS, Bagnols sur Ceze (France); Vidaud, C. [CEA Marcoule DSV/DIEP/SBTN, Bagnols sur Ceze (France); Goudard, F.; Barbot, C. [Univ. de Nantes, Faculte des Sciences, Biochim., Nantes (France); Solari, P.L. [BM29, ESRF, Grenoble (France); Funke, H. [FZR, Rossendorf beamline (BM20), ESRF, Grenoble (France)

    2005-07-01

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

  20. 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.

  1. Enhanced 99 Tc retention in glass waste form using Tc(IV)-incorporated Fe minerals

    Energy Technology Data Exchange (ETDEWEB)

    Um, Wooyong; Luksic, Steven A.; Wang, Guohui; Saslow, Sarah; Kim, Dong-Sang; Schweiger, Michael J.; Soderquist, Chuck Z.; Bowden, Mark E.; Lukens, Wayne W.; Kruger, Albert A.

    2017-11-01

    Technetium (99Tc) immobilization by doping into iron oxide mineral phases may alleviate the problems with Tc volatility during vitrification of nuclear waste. Reduced Tc, Tc(IV), substitutes for Fe(III) in the crystal structure by a process of Tc reduction from Tc(VII) to Tc(IV) followed by co-precipitation of Fe oxide minerals. Two Tc-incorporated Fe minerals (Tc-goethite and Tc-magnetite/maghemite) were prepared and tested for Tc retention in glass melt samples at temperatures between 600 – 1,000 oC. After being cooled, the solid glass specimens prepared at different temperatures were analyzed for Tc oxidation state using Tc K-edge XANES. In most samples, Tc was partially oxidized from Tc(IV) to Tc(VII) as the melt temperature increased. However, Tc retention in glass melt samples prepared using Tc-incorporated Fe minerals were moderately higher than in glass prepared using KTcO4 because of limited and delayed Tc volatilization.

  2. 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.)

  3. 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.

  4. Natural glass from Deccan volcanic province: an analogue for radioactive waste form

    Science.gov (United States)

    Rani, Nishi; Shrivastava, J. P.; Bajpai, R. K.

    2015-11-01

    Deccan basaltic glass is associated with the differentiation centres of the vast basaltic magmas erupted in a short time span. Its suitability as a radioactive waste containment chiefly depends on alteration behaviour; however, detailed work is needed on this glass. Therefore, the basaltic glass was treated under hydrothermal-like conditions and then studied to understand its alteration. Moreover, comparison of these results with the naturally altered glass is also documented in this paper. Solutions