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 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.

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.

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 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 Evaluation of Standard Durability Tests Towards the Qualification Process for the Glass-Zeolite Ceramic Waste Form

1996 ◽  
Vol 465 ◽  
Author(s):  
L. J. Simpson ◽  
D. J. Wronkiewicz
Keyword(s):  
Ionic Strength ◽  
Ion Exchange ◽  
Structural Integrity ◽  
Spent Nuclear Fuel ◽  
Fission Products ◽  
High Ionic Strength ◽  
Waste Form ◽  
Zeolite A ◽  
Acceptance Criteria ◽  
Ceramic Waste

ABSTRACTGlass-bonded zeolite is being developed as a potential ceramic waste form for the disposition of radionuclides associated with the U.S. Department of Energy's (DOE's) spent nuclear fuel conditioning activities. The utility of several standard durability tests [e.g., Materials Characterization Center Test #1 (MCC-1), Product Consistency Test-B (PCT-B), and Vapor Hydration Test (VHT)] was evaluated as a first step in developing methods and criteria that can be applied towards the process of qualifying this material for acceptance into the DOE Civilian Radioactive Waste Management System. The effects of pH, leachant composition, and sample surface-area-to-leachant-volume ratios on the durability test results are discussed, in an attempt to investigate the release mechanisms and other physical and chemical parameters that are important for the acceptance criteria, including the establishment of appropriate test methodologies required for product consistency measurements.Results from PCT-Bs conducted with 4 μm diameter salt-loaded zeolite powder indicate that a good correlation exists between release rate and ionic size and/or charge for the release behavior of the simulated fission products in deionized water (DRV), EJ-13 groundwater, and brine solutions. Simulated divalent and trivalent fission products [Sr, Ba, and rare earth (RE) ions] were preferentially retained in the zeolite (relative to the singly ionized cations) after tests with the salt-loaded zeolite in DIW. In general, the preferential cation release order for salt-loaded zeolite A in DrW is Li > Na ≥ K > Cs > Al > Si > RE > Sr > Ba. Results from PCT-Bs with the salt-loaded zeolite A immersed in high-ionic-strength brines at 90°C indicate a significant increase, relative to DIW tests, in the release rates of the Sr, Ba, and RE ions despite a decrease in the release of the Si and Al ions that make up the framework matrix of the zeolite. An increase in the Mg and Ca concentrations in the reacted zeolites suggests that an ion exchange process may be responsible for this increase.Vapor hydration and MCC-1 tests were performed with ceramic waste form monoliths of glass-bonded zeolite. The VHTs (temperatures at 120,150, and 200°C) provided useful information about the effect of glass composition on corrosion rates and alteration phase formation, and about the overall toughness and structural integrity of the ceramic waste form. The MCC-1 test was investigated as an alternative to the PCT for acceptance criteria measurements. The MCC-1 results indicate that corrosion testing with both DIW and high-ionic-strength leachants (that specifically affect the ion exchange behavior of the fission products) are required to fully assess the durability of the ceramic waste form. These preliminary results establish the utility of the MCC-1 test for providing possible acceptance criteria measurements, including elemental release comparisons between the environmental assessment benchmark and the ceramic waste form.

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.

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