Evaluation of Cesium Sujcotitanates as an Alternative Waste Form

1996 ◽  
Vol 465 ◽  
Author(s):  
Yali Su ◽  
M. Lou Balmer ◽  
Bruce C. Bunker
Keyword(s):  
Borosilicate Glass ◽  
Thermal Conversion ◽  
Chemical Durability ◽  
Waste Form ◽  
High Level Waste ◽  
Ion Exchangers ◽  
Heat Treated ◽  
High Level ◽  
Excellent Chemical ◽  
Better Than

ABSTRACTSilicotitanate ion exchangers are potential materials for the removal of radioactive Cs and Sr from tank wastes. In this paper the viability of direct thermal conversion of Cs-loaded silicotitanates to an acceptable high level waste form has been examined. Results show that in aqueous solutions, the Cs leach rates of crystalline silicotitanates (heat treated at 800°C) are 0.04, 0.18, 0.4 g/m2day for Cs loadings of 1, 5, and 20 wt%, respectively. Heating the Cs-loaded (up to 20 wt %) silicotitanates at or above 900 °C for 1 hour further reduces the Cs leach rates to approximately zero (beyond the lppm detection limits). Moreover, Cs volatilization was found to be < 0.8 wt% at temperatures as high as 1000 °C. These results suggest that thermally converted silicotitanate ion exchangers exhibit excellent chemical durability (comparable to or better than borosilicate glass) and thus, have great potential as an alternative waste form.

Nepheline Precipitation in High-Level Waste Glasses : Compositional Effects and Impact on the Waste Form Acceptability

1996 ◽  
Vol 465 ◽  
Author(s):  
H. Li ◽  
J. D. Vienna ◽  
P. Hrma ◽  
D. E. Smith ◽  
M. J. Schweiger
Keyword(s):  
Chemical Durability ◽  
Primary Phase ◽  
Waste Form ◽  
High Level Waste ◽  
X Ray Diffraction ◽  
Consistency Test ◽  
Compositional Effects ◽  
High Level ◽  
The Impact ◽  
Glass Compositions

ABSTRACTThe impact of crystalline phase precipitation in glass during canister cooling on chemical durability of the waste form limits waste loading in glass, especially for vitrification of certain high-level waste (HLW) streams rich in Na2O and Al2O3. This study investigates compositional effects on nepheline precipitation in simulated Hanford HLW glasses during canister centerline cooling (CCC) heat treatment. It has been demonstrated that the nepheline primary phase field defined by the Na2O-Al2O3-SiO2 ternary system can be used as an indicator for screening HLW glass compositions that are prone to nepheline formation. Based on the CCC results, the component effects on increasing nepheline precipitation can be approximately ranked as Al2O3 > Na2O > Li2O ≈ K2O ≈ Fe2O3 > CaO > SiC2. The presence of nepheline in glass is usually detrimental to chemical durability. Using x-ray diffraction data in conjunction with a mass balance and a second-order mixture model for 7-day product consistency test (PCT) normalized B release, the effect of glass crystallization on glass durability can be predicted with an uncertainty less than 50% if the residual glass composition is within the range of the PCT model.

scholarly journals Spent Fuel as a Waste Form - Data Needs to Allow Long Term Performance Assessment Under Repository Disposal Conditions.

1986 ◽  
Vol 84 ◽  
Author(s):  
V. M. Oversby
Keyword(s):  
Performance Assessment ◽  
Waste Form ◽  
High Level Waste ◽  
Detailed Knowledge ◽  
Spent Fuel ◽  
Expected Performance ◽  
High Level ◽  
Term Performance ◽  
Physical And Chemical ◽  
Waste Repositories

AbstractPerformance assessment calculations are required for high level waste repositories for a period of 10,000 years under NRC and EPA regulations. In addition, the Siting Guidelines (IOCFR960) require a comparison of sites following site characterization and prior to final site selection to be made over a 100,000 year period. In order to perform the required calculations, a detailed knowledge of the physical and chemical processes that affect waste form performance will be needed for each site. While bounding calculations might be sufficient to show compliance with the requirements of IOCFR60 and 40CFRI91, the site comparison for 100,000 years will need to be based on expected performance under site specific conditions. The only case where detailed knowledge of waste form characteristics in the repository would not be needed would be where radionuclide travel times to the accessible environment can be shown to exceed 100,000 years. This paper will review the factors that affect the release of radionuclides from spemt fuel under repository conditions, summarize our present state of knowledge, and suggest areas where more work is needed in order to support the performance assessment calculations.

Lessons Learned Siting and Successfully Processing U.S. DOE Radioactive Wastes Using a High Throughput Vitrification Process

2003 ◽  
Author(s):  
Robert E. Prince ◽  
Bradley W. Bowan
Keyword(s):  
The United States ◽  
Lessons Learned ◽  
Volume Reduction ◽  
Waste Form ◽  
High Level Waste ◽  
Hanford Site ◽  
High Level ◽  
Low Activity ◽  
The U.S ◽  
Ceramic Melter

This paper describes actual experience applying a technology to achieve volume reduction while producing a stable waste form for low and intermediate level liquid (L/ILW) wastes, and the L/ILW fraction produced from pre-processing of high level wastes. The chief process addressed will be vitrification. The joule-heated ceramic melter vitrification process has been used successfully on a number of waste streams produced by the U.S. Department of Energy (DOE). This paper will address lessons learned in achieving dramatic improvements in process throughput, based on actual pilot and full-scale waste processing experience. Since 1991, Duratek, Inc., and its long-term research partner, the Vitreous State Laboratory of The Catholic University of America, have worked to continuously improve joule heated ceramic melter vitrification technology in support of waste stabilization and disposition in the United States. From 1993 to 1998, under contact to the DOE, the team designed, built, and operated a joule-heated melter (the DuraMelterTM) to process liquid mixed (hazardous/low activity) waste material at the Savannah River Site (SRS) in South Carolina. This melter produced 1,000,000 kilograms of vitrified waste, achieving a volume reduction of approximately 70 percent and ultimately producing a waste form that the U.S. Environmental Protection Agency (EPA) delisted for its hazardous classification. The team built upon its SRS M Area experience to produce state-of-the-art melter technology that will be used at the DOE’s Hanford site in Richland, Washington. Since 1998, the DuraMelterTM has been the reference vitrification technology for processing both the high level waste (HLW) and low activity waste (LAW) fractions of liquid HLW waste from the U.S. DOE’s Hanford site. Process innovations have doubled the throughput and enhanced the ability to handle problem constituents in LAW. This paper provides lessons learned from the operation and testing of two facilities that provide the technology for a vitrification system that will be used in the stabilization of the low level fraction of Hanford’s high level tank wastes.

Effect of Li, Fe, and B Addition on the Crystallization Behavior of Sodium Aluminosilicate Glasses as Analogues for Hanford High Level Waste Glasses

MRS Advances ◽  
2016 ◽  
Vol 2 (10) ◽  
pp. 549-555 ◽  
Author(s):  
José Marcial ◽  
Mostafa Ahmadzadeh ◽  
John S. McCloy
Keyword(s):  
Function Analysis ◽  
High Level Waste ◽  
X Ray Diffraction ◽  
X Ray ◽  
High Sodium ◽  
Chemical Ordering ◽  
Sodium Aluminosilicate ◽  
Aluminosilicate Glasses ◽  
Heat Treated ◽  
High Level

ABSTRACTCrystallization of aluminosilicates during the conversion of Hanford high-level waste (HLW) to glass is a function of the composition of the glass-forming melt. In high-sodium, high-aluminum waste streams, the crystallization of nepheline (NaAlSiO4) removes chemically durable glass-formers from the melt, leaving behind a residual melt that is enriched in less durable components, such as sodium and boron. We seek to further understand the effect of lithium, boron, and iron addition on the crystallization of model silicate glasses as analogues for the complex waste glass. Boron and iron behave as glass intermediates which allow for crystallization when present in low additions but frustrate crystallization in high additions. In this work, we seek to compare the average structures of quenched and heat treated glasses through Raman spectroscopy, X-ray diffraction, vibrating sample magnetometry, and X-ray pair distribution function analysis. The endmembers of this study are feldspathoid-like (LiAlSiO4, NaAlSiO4, NaBSiO4, and NaFeSiO4), pyroxene-like (LiAlSi2O6, NaAlSi2O6, NaBSi2O6, and NaFeSi2O6), and feldspar-like (LiAlSi3O8, NaAlSi3O8, NaBSi3O8, and NaFeSi3O8). Such a comparison will provide further insight on the complex relationship between the average chemical ordering and topology of glass on crystallization.

Performance of Borosilicate Glass High-Level Waste Forms in Disposal Systems

1986 ◽  
Vol 73 (2) ◽  
pp. 139-139
Author(s):  
Edward J. Hennelly ◽  
E. I. Du Pont de Nemours
Keyword(s):  
Borosilicate Glass ◽  
High Level Waste ◽  
Waste Forms ◽  
High Level

Wipp Waste Package Testing on Simulated DHLW: Emplacement

1984 ◽  
Vol 44 ◽  
Author(s):  
Martin A. Molecke
Keyword(s):  
Thermal Loading ◽  
Accelerated Aging ◽  
Waste Form ◽  
Future Application ◽  
High Level Waste ◽  
Glass Waste ◽  
Waste Package ◽  
High Level ◽  
Artificial Introduction ◽  
Materials Behavior

AbstractSeveral series of simulated (nonradioactive) defense high-level waste (DHLW) package tests have recently been emplaced in the WIPP, a research and development facility authorized to demonstrate the safe disposal of defense-related wastes. The primary purpose of these 3-to-7 year duration tests is to evaluate the in situ materials performance of waste package barriers (canisters, overpacks, backfills, and nonradioactive DHLW glass waste form) for possible future application to a licensed waste repository in salt. This paper describes all test materials, instrumentation, and emplacement and testing techniques, and discusses progress of the various tests.These tests are intended to provide information on materials behavior (i.e., corrosion, metallurgical and geochemical alterations, waste form durability, surface interactions, etc.), as well as comparison between several waste package designs, fabrications details, and actual costs.These experiments involve 18 full-size simulated DHLW packages (approximately 3.0 m x 0.6 m diameter) emplaced in vertical boreholes in the salt drift floor. Six of the test packages contain internal electrical heaters (470 W/canister), and were emplaced under approximately reference DHLW repository conditions. Twelve other simulated DHLW packages were emplaced tinder accelerated-aging or overtest conditions, including the artificial introduction of brine, and a thermal loading approximately three to four times higher than reference. Eight of these 12 test packages contain 1500 W/canister electrical heaters; the other four are filled with DHLW glass.

Affinity Rate Law Failure to Describe Sodium Borosilicate Glass Alteration Kinetics

2003 ◽  
Vol 807 ◽  
Author(s):  
P. Frugier ◽  
S. Gin ◽  
C. Jégou
Keyword(s):  
Borosilicate Glass ◽  
Chemical System ◽  
High Level Waste ◽  
Critical Examination ◽  
Sodium Borosilicate Glass ◽  
Kinetic Rate ◽  
Rate Law ◽  
Passionate Debate ◽  
Experimental Findings ◽  
High Level

ABSTRACTSimplified glass compositions were chosen to improve our knowledge of the alteration kinetics of complex glasses dedicated to the confinement of high-level waste. Since 1998, the sodium borosilicate glass system is at the center of a passionate debate between an affinity-based kinetic rate law and a protective surface layer theory. All the authors who have investigated ternary 68/14/18 SiO2–B2O3–Na2O glass agree on the fact that the affinity law cannot satisfactorily account for its alteration kinetics. Some authors explained that these discrepancies between classical kinetic rate law and experimental findings could be due to macromolecular amorphous separation in the 68/14/18 sodium borosilicate system and that this simplified glass could be divided into 90% reedmergnerite (NaBSi3O8) and 10% diborate (Na2O–2B2O3). This article provides evidence of the homogeneity of ternary 68/18/14 SiO2–B2O3–Na2O glass at nanometric scale and shows that even phase separation at less than nanometric scale could not explain the inability of hydrated glass-solution affinity laws to describe its alteration. The relative simplicity of the SiO2–B2O3–Na2O chemical system allows a critical examination of the macroscopic alteration laws developed over the last twenty years based only on the hydrated glass-solution chemical affinity without taking into account the formation and reactivity of the gel or its passivating properties.

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 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.

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