Consolidating Electrorefined Spent Nuclear Fuel Waste: Analysis and Experiment

2003 ◽  
Author(s):  
K. J. Bateman ◽  
D. D. Capson
Keyword(s):  
Spent Nuclear Fuel ◽  
National Laboratory ◽  
Argonne National Laboratory ◽  
Fission Products ◽  
Waste Form ◽  
Processing Conditions ◽  
Production Scale ◽  
Ceramic Waste ◽  
Waste Salt ◽  
Nuclear Fuel Waste

Argonne National Laboratory has developed a process to immobilize waste salt containing fission products, uranium, and transuranic elements as chlorides in a glass-bonded ceramic waste form. This salt was generated in the electrorefining operation used in the electrometallurical treatment of spent EBR-II fuel. The ceramic waste process culminates with an elevated temperature operation. The processing conditions used by the furnace, for demonstration scale and production scale operations, are to be developed at Argonne National Laboratory. To assist in selecting the processing conditions of the furnace and to reduce the number of costly experiments, a finite difference model was developed to predict the consolidation of the ceramic waste. The model accurately predicted the heating as well as the bulk density of the ceramic waste form. The methodology used to develop the computer model and a comparison of the analysis to experimental data is presented.

scholarly journals Development of a ceramic waste form for high-level waste disposal

1999 ◽  
Vol 556 ◽  
Author(s):  
D. W. Esh ◽  
K. M. Goff ◽  
K. T. Hirsche ◽  
T. J. Battisti ◽  
M. F. Simpson ◽  
...  
Keyword(s):  
Spent Nuclear Fuel ◽  
National Laboratory ◽  
Argonne National Laboratory ◽  
Fission Products ◽  
Waste Form ◽  
High Level Waste ◽  
Durability Test ◽  
Ceramic Waste ◽  
High Level ◽  
The Impact

AbstractA ceramic waste form is being developed by Argonne National Laboratory* (ANL) as part of the demonstration of the electrometallurgical treatment of spent nuclear fuel [1]. The halide, alkaline earth, alkali, transuranic, and rare earth fission products are stabilized in zeolite which is combined with glass and processed in a hot isostatic press (HIP) to form a ceramic composite. The mineral sodalite is formed in the HIP from the zeolite precursor. The process, from starting materials to final product, is relatively simple. An overview of the processing operations is given. The metrics that have been developed to measure the success or completion of processing operations are developed and discussed. The impact of variability in processing metrics on the durability of the final product is presented. The process is demonstrated to be robust for the type and range of operation metrics considered and the performance metric (PCT durability test) against which the operation metrics are evaluated.

Production And Characterization Of A Plutonium-238 Loaded Ceramic Waste Form For The Study Of The Effects Of Alpha Decay Damage

1999 ◽  
Vol 556 ◽  
Author(s):  
M. Steven ◽  
Steven M. Frank ◽  
David W. Esh ◽  
Stephen G. Johnson ◽  
Marianne Noy ◽  
...  
Keyword(s):  
Ceramic Material ◽  
Spent Nuclear Fuel ◽  
Specific Activity ◽  
National Laboratory ◽  
Argonne National Laboratory ◽  
High Specific Activity ◽  
Fission Products ◽  
Alpha Decay ◽  
Waste Form ◽  
Ceramic Waste

AbstractArgonne National Laboratory has developed a glass-bonded sodalite ceramic waste form to immobilize fission products and plutonium that accumulate during the electrometallurgical conditioning of spent nuclear fuel. To investigate the effects of alpha decay damage on the structure and leaching characteristics of the ceramic material, 238Pu has been incorporated into the ceramic waste form. The 238pu,with its high specific activity, significantly increases the rate of alpha damage to the waste form. Long term studies have begun with periodic examination of the 238Pu loaded ceramic material. A number of characterization techniques are used to study the alpha decay damage on the structure of the waste form. In addition, PCT type leachate studies will be performed to determine the effect of alpha decay damage on the durability of the ceramic waste form. Preliminary results from this study are presented.

scholarly journals Effect of Different Glass and Zeolite-a Compositions on the Leach Resistance of Ceramic Waste Forms

1996 ◽  
Vol 465 ◽  
Author(s):  
M. A. Lewis ◽  
M. Hash ◽  
D. Glandorf
Keyword(s):  
Spent Nuclear Fuel ◽  
National Laboratory ◽  
Hot Isostatic Pressing ◽  
Argonne National Laboratory ◽  
Fission Products ◽  
Waste Form ◽  
Zeolite A ◽  
Ceramic Waste ◽  
Leach Test ◽  
Salt Phase

ABSTRACTA ceramic waste form is being developed at Argonne National Laboratory for waste generated during the electrometallurgical treatment of spent nuclear fuel. The waste is generated when fission products are removed from the electrolyte, LiCI-KCl eutectic. The ceramic waste form is a composite, fabricated by hot isostatic pressing a mixture of glass frit and zeolite occluded with fission products and salt. Past work has shown that the normalized release rate (NRR) is less than 1 g/m2d for all elements in a Material Characterization Center-Type 1 (MCC-1) leach test run for 28 days in deionized water at 90°C (363 K). This leach resistance is comparable to that of early Savannah River glasses. We are investigating how leach resistance is affected by changes in the cationic form of zeolite and in the glass composition. Composites were made with three forms of zeolite A and six glasses. We used three-day ASTM C1220–92 (formerly MCC-1) leach tests to screen samples for development purposes only. The leach test results show that the glass composites of zeolites 5A and 4A retain fission products equally well. The loss of cesium is small, varying from 0.1 to 0.5 wt%, while the loss of divalent and trivalent fission products is one or more orders of magnitude smaller. Composites of 5A retain chloride ion better in these short-term screens than 4A and 3A. The more leach resistant composites were made with durable glasses that were rich in silica and poor in alkaline earth oxides. The x-ray diffraction (XRD) results show that a salt phase was absent in the leach resistant composites of 5A and the better glasses but was present in the other composites with poorer leach performance. Thus, the data show that the absence of a salt phase in a composite's XRD pattern corresponds to improved leach resistance. The data also suggest that the interactions between the zeolite and glass depend on the composition of both.

scholarly journals Hot Isostatic Pressing of Ceramic Waste From Spent Nuclear Fuel

2002 ◽  
Author(s):  
Kenneth J. Bateman ◽  
Richard H. Rigg ◽  
James D. Wiest
Keyword(s):  
Spent Nuclear Fuel ◽  
National Laboratory ◽  
Hot Isostatic Pressing ◽  
Argonne National Laboratory ◽  
Fission Products ◽  
Spent Fuel ◽  
Isostatic Pressing ◽  
Ceramic Waste ◽  
Pressing Operation ◽  
Waste Salt

Argonne National Laboratory has developed a process to immobilize waste salt containing fission products, uranium, and transuranic elements as chlorides in a glass-bonded ceramic waste form. This salt was generated in the electrorefining operation used in electrometallurgical treatment of spent Experimental Breeder Reactor-II fuel. The ceramic waste process culminated with a hot isostatic pressing operation. This paper reviews the installation and operation of a hot isostatic press in a radioactive environment. Processing conditions for the hot isostatic press are presented for non-irradiated material and irradiated material. Sufficient testing was performed to demonstrate that a hot isostatic press could be used as the final step of the processing of ceramic waste for the electrometallurgical spent fuel treatment process.

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.

Preliminary Studies of the Disposition of Cesium in a Glass-Bonded Sodalite Waste form

2002 ◽  
Vol 713 ◽  
Author(s):  
Marsha J. Lambregts ◽  
Steven M. Frank
Keyword(s):  
National Laboratory ◽  
Argonne National Laboratory ◽  
Fission Products ◽  
Waste Form ◽  
Resonance Spectroscopy ◽  
Ceramic Waste ◽  
Long Term Storage ◽  
Geological Repository ◽  
Term Storage

ABSTRACTArgonne National Laboratory has developed an electrometallurgical treatment for DOE spent metallic nuclear fuel. Fission products are immobilized in a durable glass bonded sodalite ceramic waste form (CWF) suitable for long term storage in a geological repository. Cesium is estimated to be in the waste form at approximately 0.1 wt.%. The exact disposition of cesium was uncertain and it was believed to be uniformly distributed throughout the waste form. A correlation of X-ray diffractometry (XRD), electron microscopy (EM), and nuclear magnetic resonance spectroscopy (NMR) performed on surrogate ceramic waste forms with high cesium loadings found a high cesium content in the glass phase and in several non-sodalite aluminosilicate phases. Cesium was not detected in the sodalite phase.

scholarly journals Characterization of Composite Ceramic High Level Waste Forms

1997 ◽  
Vol 481 ◽  
Author(s):  
S. M. Frank ◽  
K. J. Bateman ◽  
T. DiSanto ◽  
S. G. Johnson ◽  
T. L. Moschetti ◽  
...  
Keyword(s):  
Spent Nuclear Fuel ◽  
Argonne National Laboratory ◽  
Fission Products ◽  
Composite Ceramic ◽  
Waste Form ◽  
High Level Waste ◽  
Ceramic Waste ◽  
Chloride Form ◽  
Physical Measurements ◽  
High Level

ABSTRACTArgonne National Laboratory has developed a composite ceramic waste form for the disposition of high level radioactive waste produced during electrometallurgical conditioning of spent nuclear fuel. The electrorefiner LiCl/KCl eutectic salt, containing fission products and transuranics in the chloride form, is contacted with a zeolite material which removes the fission products from the salt. After salt contact, the zeolite is mixed with a glass binder. The zeolite/glass mixture is then hot isostatic pressed (HIPed) to produce the composite ceramic waste form. The ceramic waste form provides a durable medium that is well suited to incorporate fission products and transuranics in the chloride form. Presented are preliminary results of the process qualification and characterization studies, which include chemical and physical measurements and product durability testing, of the ceramic waste form.

scholarly journals Incorporation of radionuclides from the electrometallurgical treatment of spent fuel into a ceramic waste form

1999 ◽  
Vol 556 ◽  
Author(s):  
C. Pereira ◽  
M. C. Hash ◽  
M. A. Lewis ◽  
M. K. Richmann ◽  
J. Basco
Keyword(s):  
Ion Exchange ◽  
Molten Salt ◽  
Nuclear Fuel ◽  
Argonne National Laboratory ◽  
Fission Products ◽  
Experimental Results ◽  
Waste Form ◽  
Chloride Salt ◽  
Zeolite A ◽  
Ceramic Waste

AbstractAn electrometallurgical process is being developed at Argonne National Laboratory to treat spent metallic nuclear fuel. In this process, the spent nuclear fuel is electrorefined in a molten salt to separate uranium from the other constituents of the fuel. The treatment process generates a contaminated chloride salt that is incorporated into a ceramic waste form. The ceramic waste form, a composite of sodalite and glass, contains the fission products (rare earths, alkalis, alkaline earth metals, and halides) and transuranic radionuclides that accumulated in the electrorefiner salt. These radionuclides are incorporated into zeolite A, which can fully accommodate the salt in its crystal structure. The radionuclides are incorporated into the zeolite by hightemperature blending or by ion exchange. In the blending process the salt and zeolite are simply tumbled together at >450°C (723 K), but in the ion exchange process, which yields a product more highly concentrated in fission products, the molten salt is passed through a bed of the zeolite. In either case, the salt-loaded zeolite A is mixed with glass frit and hot isostatically pressed to produce a monolithic leach resistant waste form.Zeolite is converted to sodalite during hot pressing. This paper presents experimental results on the experimental results on the fission product uptake of the zeolite as a function of time and salt composition.

scholarly journals Microstructure and Leaching Characteristics of a Technetium Containing Metal Waste Form

1999 ◽  
Vol 556 ◽  
Author(s):  
S. G. Johnson ◽  
D. D. Keiser ◽  
M. Noy ◽  
T. O'Holleran ◽  
S. M. Frank
Keyword(s):  
Stainless Steel ◽  
National Laboratory ◽  
Argonne National Laboratory ◽  
Fission Products ◽  
Point Of View ◽  
Waste Form ◽  
Nominal Composition ◽  
Spent Fuel ◽  
Waste Forms ◽  
Metal Waste

AbstractArgonne National Laboratory is developing an electrometallurgical treatment for spent fuel from the experimental breeder reactor II. A product of this treatment process is a metal waste form that incorporates the stainless steel cladding hulls, zirconium from the fuel and the fission products that are noble to the process, i.e., Tc, Ru, Pd, Rh, Ag. The nominal composition of this waste form is stainless steel/15 wt% zirconium/ 1–4 wt% noble metal fission products. The behavior of technetium is of particular importance from a disposal point of view for this waste form due to its long half life, 2.14E5 years, and its mobility in groundwater. To address these concerns a limited number of spiked metal waste forms were produced containing Tc. These surrogate waste forms were then studied using scanning electron microscopy (SEM) and selected leaching tests.

scholarly journals Alpha-Decay Radiation Damage Study of a Glass-Bonded Sodalite Ceramicwaste form

2002 ◽  
Vol 713 ◽  
Author(s):  
S.M. Frank ◽  
T. L. Barber ◽  
T. DiSanto ◽  
K. M. Goff ◽  
S. G. Johnson ◽  
...  
Keyword(s):  
Spent Nuclear Fuel ◽  
Fission Products ◽  
Alpha Decay ◽  
Weight Percent ◽  
Department Of Energy ◽  
Waste Form ◽  
Plutonium Dioxide ◽  
Ceramic Waste ◽  
Transmission Electron ◽  
Immersion Testing

ABSTRACTEffects of alpha decay on the ceramic waste form used to immobilize fission products and actinides accumulated from electrometallurgical treatment of Department of Energy metallic spent nuclear fuel is being studied. This involved the preparation of a surrogate ceramic waste form containing two-weight percent plutonium-238 and monitoring changes to the waste form resulting from alpha-decay damage. The phase assembly of the ceramic waste form consists of glass-bonded sodalite with small quantities of nepheline, halite and plutonium dioxide. The waste form has been monitored for three years and has acquired an internal alpha-decay dose of 1 × 1018 disintegrations per gram of material. Methods used to monitor the material include: density determination, chemical durability measured by immersion testing, microscopy and powder xray diffraction. The investigation has, to date, found little alteration to the waste form due to alpha-decay damage. X-ray diffraction analysis has detected a unit cell volume increase of 0.7 percent of the plutonium dioxide phase. Furthermore, bubbles and/or voids have been observed by transmission electron microscopy in the sodalite and glass phase. The origin of these defects is unclear and under investigation.

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