scholarly journals Lysimeter study of commercial reactor waste forms: waste form acquisition characterization and full-scale leaching

1983 ◽  
Author(s):  
Keyword(s):  
Full Scale ◽  
Waste Form ◽  
Waste Forms ◽  
Commercial Reactor

Leaching Scale Effect for Cement-Waste Forms

1988 ◽  
Vol 127 ◽  
Author(s):  
J. C. Nomine ◽  
A. Billon ◽  
G. Courtois
Keyword(s):  
Scale Effect ◽  
Practical Method ◽  
Full Scale ◽  
Time Limit ◽  
Waste Form ◽  
Leaching Tests ◽  
Local Policy ◽  
Waste Package ◽  
Waste Forms

The confinement ability of a waste package is one of the major safety characteristics to consider in shallow land burial. In order to determine if the confinement is acceptable, in accordance with local policy, one way is to proceed to leaching tests. The practical method, for sake of simplicity, cost and time limit, is to carry out the leaching tests on laboratory samples which are easier to prepare than full-scale blocks, but the representativity of which needs to be treated with caution; it is in this context, that one of the aspect of our work concerns what is known as the “scale effect”.This study has been conducted using blocks the volumes of which are respectively of 200, 20, 2 and 0, 2 1, and made with the same cement-waste form (13 Cs) system.

Immobilization of rocky flats graphite fines residues

1999 ◽  
Vol 556 ◽  
Author(s):  
T. S. Rudisill ◽  
J. C. Marra ◽  
D. K. Peeler
Keyword(s):  
Scale Up ◽  
Glass Frit ◽  
Heating Time ◽  
Full Scale ◽  
Waste Form ◽  
Small Scale ◽  
Rocky Flats ◽  
Waste Forms ◽  
Average Residue ◽  
The Impact

AbstractThe Savannah River Technology Center (SRTC) is developing an immobilization process for graphite fines residues generated during nuclear materials production activities at the Rocky Flats Environmental Technology Site (Rocky Flats). The continued storage of this material has been identified as an item of concern. The residue was generated during the cleaning of graphite casting molds and potentially contains reactive plutonium metal. The average residue composition is 73 wt% graphite, 15 wt% calcium fluoride (CaF2), and 12 wt% plutonium oxide (PuO2 ). Approximately 950 kg of this material are currently stored at Rocky Flats.The strategy of the immobilization process is to microencapsulate the residue by mixing with a sodium borosilicate (NBS) glass frit and heating at nominally 700°C. The resulting waste form would be sent to the Waste Isolation Pilot Plant (WIPP) for disposal. Since the PuO2 concentration in the residue averages 12 wt%, the immobilization process was required to meet the intent of safeguards termination criteria by limiting plutonium recoverability based on a test developed by Rocky Flats. The test required a plutonium recovery of less than 4 g/kg of waste form when a sample was leached using a nitric acid/CaF2 dissolution flowsheet.Immobilization experiments were performed using simulated graphite fines with cerium oxide (CeO2) as a surrogate for PuO2 and with actual graphite fines residues. Small-scale surrogate experiments demonstrated that a 4:1 frit to residue ratio was adequate to prevent recovery of greater than 4 g/kg of cerium from simulated waste forms. Additional experiments investigated the impact of varying concentrations of CaF2 and the temperature/heating time cycle on the cerium recovery. Optimal processing conditions developed during these experiments were subsequently demonstrated at full-scale with surrogate materials and on a smaller scale using actual graphite fines.In general, the recovery of cerium from the full-scale waste forms was higher than for smaller scale experiments. The presence of CaF2 also caused a dramatic increase in cerium recovery not seen in the small-scale experiments. However, the results from experiments with actual graphite fines were encouraging. A 4:1 frit to residue ratio, a temperature of 700°C, and a 2 hr heating time produced waste forms with plutonium recoveries of 4±1 g/kg. With an increase in the frit to residue ratio, waste forms fabricated at this scale should meet the Rocky Flats product specification. The scale-up of the waste form fabrication process to nominally 3 kg is expected to require a 5:1 to 6:1 frit to residue ratio and maintaining the waste form centerline temperature at 700°C for 2 hr.

Host Phases for Actinide Elements in the Metallic Waste Form

2002 ◽  
Vol 757 ◽  
Author(s):  
D. E. Janney
Keyword(s):  
Stainless Steel ◽  
Electron Microscope ◽  
Electron Diffraction ◽  
Transmission Electron Microscope ◽  
Waste Form ◽  
Dissolution Behavior ◽  
Release Rates ◽  
Waste Forms ◽  
Transmission Electron ◽  
Simulated Waste

ABSTRACTArgonne National Laboratory has developed an electrometallurgical process for conditioning spent sodium-bonded metallic reactor fuel prior to disposal. A waste stream from this process consists of stainless steel cladding hulls that contain undissolved metal fission products such as Tc, Ru, Rh, Pd, and Ag; a small amount of undissolved actinides (U, Np, Pu) also remains with the hulls. These wastes will be immobilized in a waste form whose baseline composition is stainless steel alloyed with 15 wt% Zr (SS-15Zr). Scanning electron microscope (SEM) observations of simulated metal waste forms (SS-15Zr with up to 11 wt% actinides) show eutectic intergrowths of Fe-Zr-Cr-Ni intermetallic phases with steels. The actinide elements are almost entirely in the intermetallics, where they occur in concentrations ranging from 1–20 at%. Neutron- and electron-diffraction studies of the simulated waste forms show materials with structures similar to those of Fe2Zr and Fe23Zr6.Dissolution experiments on simulated waste forms show that normalized release rates of U, Np, and Pu differ from each other and from release rates of other elements in the sample, and that release rates for U exceed those for any other element (including Fe). This paper uses transmission electron microscope (TEM) observations and results from energy-dispersive X-ray spectroscopy (EDX) and selected-area electron-diffraction (SAED) to characterize relationships between structural and chemical data and understand possible reasons for the observed dissolution behavior.Transmission electron microscope observations of simulated waste form samples with compositions SS-15Zr-2Np, SS-15Zr-5U, SS-15Zr-11U-0.6Rh-0.3Tc-0.2Pd, and SS-15Zr-10Pu suggest that the major actinide-bearing phase in all of the samples has a structure similar to that of the C15 (cubic, MgCu2-type) polymorph of Fe2Zr, and that materials with this structure exhibit significant variability in chemical compositions. Material whose structure is similar to that of the C36 (dihexagonal, MgNi2-type) polymorph of Fe2Zr was also observed, and it exhibits less chemical variability than that displayed by material with the C15 structure. The TEM data also demonstrate a range of actinide concentrations in materials with the Fe23Zr6 (cubic, Mn23Th6-type) structure.Microstructures similar to those produced during experimental deformation of Fe-10 at% Zr alloys were observed in intermetallic materials in all of the simulated waste form samples. Stacking faults and associated dislocations are common in samples with U, but rarely observed in those with Np and Pu, while twins occurred in all samples. The observed differences in dissolution behavior between samples with different actinides may be related to increased defect-assisted dissolution in samples with U.

Aging Studies of Pu-238 and -239 Containing Calcium Phosphate Ceramic Waste-forms

2013 ◽  
Vol 1518 ◽  
pp. 73-78 ◽  
Author(s):  
Shirley K. Fong ◽  
Brian L. Metcalfe ◽  
Randall D. Scheele ◽  
Denis M. Strachan
Keyword(s):  
Calcium Phosphate ◽  
Accelerated Aging ◽  
Waste Form ◽  
Calcium Phosphate Ceramic ◽  
Ceramic Waste ◽  
Waste Forms ◽  
Aging Studies ◽  
Flow Through ◽  
Pyrochemical Reprocessing

ABSTRACTA calcium phosphate ceramic waste-form has been developed at AWE for the immobilisation of chloride containing wastes arising from the pyrochemical reprocessing of plutonium. In order to determine the long term durability of the waste-form, aging trials have been carried out at PNNL. Ceramics were prepared using Pu-239 and -238, these were characterised by PXRD at regular intervals and Single Pass Flow Through (SPFT) tests after approximately 5 yrs.While XRD indicated some loss of crystallinity in the Pu-238 samples after exposure to 2.8 x 1018 α decays, SPFT tests indicated that accelerated aging had not had a detrimental effect on the durability of Pu-238 samples compared to Pu-239 waste-forms.

Progress on Ongoing Waste form HIP projects at ANSTO

MRS Advances ◽  
2018 ◽  
Vol 3 (20) ◽  
pp. 1059-1064 ◽  
Author(s):  
Eric R. Vance ◽  
Dorji T. Chavara ◽  
Daniel J. Gregg
Keyword(s):  
Spent Nuclear Fuel ◽  
Technology Development ◽  
Hot Isostatic Pressing ◽  
Waste Form ◽  
Process Technology ◽  
Ceramic Waste ◽  
Waste Forms ◽  
Produce Glass ◽  
Form Development ◽  
Year 2000

Abstract:Since the year 2000, Synroc has evolved from the titanate full-ceramic waste forms developed in the late 1970s to a hot isostatic pressing (HIP) technology platform that can be applied to produce glass, glass–ceramic, and ceramic waste forms and where there are distinct advantages over vitrification in terms of, for example, waste loading and suppressing volatile losses. This paper describes recent progress on waste form development for intermediate-level wastes from 99Mo production at ANSTO, spent nuclear fuel, fluoride pyroprocessing wastes and 129I. The microstructures and aqueous dissolution results are presented where applicable. This paper provides perspective on Synroc waste forms and recent process technology development in the nuclear waste management industry.

TEM Analysis of Corrosion Products From a Radioactive Stainless Steel-based Alloy

2000 ◽  
Vol 6 (S2) ◽  
pp. 368-369
Author(s):  
N.L. Dietz ◽  
D.D Keiser
Keyword(s):  
Stainless Steel ◽  
Spent Nuclear Fuel ◽  
National Laboratory ◽  
Argonne National Laboratory ◽  
Fission Products ◽  
Waste Form ◽  
Metallic Sodium ◽  
Geologic Repository ◽  
Tem Analysis ◽  
Waste Forms

Argonne National Laboratory has developed an electrometallurgical treatment process for metallic spent nuclear fuel from the Experimental Breeder Reactor-II. This process stabilizes metallic sodium and separates usable uranium from fission products and transuranic elements that are contained in the fuel. The fission products and other waste constituents are placed into two waste forms: a ceramic waste form that contains the transuranic elements and active fission products such as Cs, Sr, I and the rare earth elements, and a metal alloy waste form composed primarily of stainless steel (SS), from claddings hulls and reactor hardware, and ∼15 wt.% Zr (from the U-Zr and U-Pu-Zr alloy fuels). The metal waste form (MWF) also contains noble metal fission products (Tc, Nb, Ru, Rh, Te, Ag, Pd, Mo) and minor amounts of actinides. Both waste forms are intended for eventual disposal in a geologic repository.

Ion Implantation Studies of Nuclear Waste Forms

1981 ◽  
Vol 6 ◽  
Author(s):  
Clyde J. M. Northrup ◽  
George W. Arnold ◽  
Thomas J. Headley
Keyword(s):  
Nuclear Waste ◽  
Borosilicate Glass ◽  
Alpha Decay ◽  
Lead Ions ◽  
Waste Form ◽  
Elastic Recoil ◽  
Elastic Recoil Detection ◽  
Waste Forms ◽  
Basic Studies ◽  
Nuclear Waste Forms

ABSTRACTThe first observations of physical and chemical changes induced by lead implantation damage and leaching are reported for two proposed U.S. nuclear waste forms (PNL 76–68 borosilicate glass and Sandia titanate ceramics) for commercial wastes. To simulate the effects of recoil nucleii due to alpha decay, the materials were implanted with lead ions at equivalent doses up to approximately 1 × 1019 a decays/cm3 . In the titanate waste form, the zirconolite, perovskite, hollandite, and rutile phases all exhibited a mottled appearance in the transmission electron microscope (TEM) typical of defect clusters in radiation damaged, crystalline solids. One titanate phase containing uranium was found by TEM to be amorphous after implantation at the highest dose. No enhanced leaching (deionized water, room temperature, 24 hours) of the irradiated titanate waste form, including the amorphous phase, was detected by TEM, but Rutherford backscattering (RBS) suggested a loss of cesium and calcium after 21 hours of leaching. The RBS spectra also indicated enhanced leaching from the PNL 76–68 borosilicate glass after implantation with lead ions, in general agreement with the observations of Dran, et al. [6,7] on other irradiated materials. Elastic recoil detection spectroscopy (ERD), used to profile hydrogen after leaching, showed penetration of the hydrogen to several thousand angstroms for both the implanted and unimplanted materials. These basic studies identified techniques to follow the changes that occur on implantation and leaching of complex amorphous and crystalline waste forms. These studies were not designed to produce comparisons between waste forms of gross leach rates.

Fluidized Bed Steam Reformed (FBSR) Mineral Waste Forms: Characterization and Durability Testing

2006 ◽  
Vol 985 ◽  
Author(s):  
Carol Jantzen ◽  
Troy H. Lorier ◽  
John M. Pareizs ◽  
James C. Marra
Keyword(s):  
Fluidized Bed ◽  
Environmental Protection Agency ◽  
National Laboratory ◽  
Pilot Scale ◽  
Waste Form ◽  
High Sodium ◽  
Waste Forms ◽  
Ring Structures ◽  
Low Activity ◽  
Mineral Waste

AbstractFluidized 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.

Comparison of the Leachability of Three TRU Cement Waste Forms

1982 ◽  
Vol 15 ◽  
Author(s):  
Wayne Ross ◽  
Joseph Westsik ◽  
Frank Roberts ◽  
Clark Harvey
Keyword(s):  
Elevated Temperatures ◽  
Waste Form ◽  
Cold Pressing ◽  
Waste Forms ◽  
Leach Test

ABSTRACTCement waste forms prepared by three processes, casting, cold pressing, and FUETAP (Formed Under Elevated Temperatures and Pressure) have been compared for their leachability by using the MCC-1 leach test. The results indicate that releases of plutonium are not controlled by the waste form matrix and that there is no significant overall advantage to any of the three cement processes from a leachability viewpoint.

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