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 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.

Phase Relations and Chemical Durability of Ceramics in the Pseudo-Binary System: CaZrTi2O7–GdAlO3

2003 ◽  
Vol 807 ◽  
Author(s):  
N. P. Mikhailenko ◽  
A. V. Ochkin ◽  
S. V. Stefanovsky ◽  
O. I. Kirjanova
Keyword(s):  
Electron Microscopy ◽  
Binary System ◽  
Chemical Durability ◽  
Phase Relations ◽  
High Level Waste ◽  
X Ray Diffraction ◽  
X Ray ◽  
Ceramic Samples ◽  
High Level ◽  
System 1

ABSTRACTPhase relations in a pseudo-binary system (1-x) CaZrTi2O7- x GdAlO3 suggested for immobilization of a zirconium - rare earth – actinide fraction of high level waste were studied with X-ray diffraction and electron microscopy. Zirconolite and perovskite were found to be major phases in the ceramic samples prepared by cold pressing and sintering at 1400 and 1500 °C. At relatively low perovskite content (x < 0.5) zirconolite is the major host for Gd, which is considered as a trivalent surrogate for Am and Cm. At higher perovskite content, perovskite becomes the major host for Gd. Zirconolite is the major host phase for corrosion products (Al, Fe, Ti, Zr). Leach rates of Gd, 238Pu, and 241Am from the ceramics studied are 10−4–10−5 g/(m2d).

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.

Effect of Molybdenum and Ruthenium on the Crystallization Tendency of a New Nuclear Glass Containing High Rare-earth Concentration

2010 ◽  
Vol 1265 ◽  
Author(s):  
Daniel Caurant ◽  
Nolwenn Chouard ◽  
Odile Majerus ◽  
Jean-Luc Dussossoy ◽  
Aurelien Ledieu ◽  
...  
Keyword(s):  
Room Temperature ◽  
Nucleating Agent ◽  
High Level Waste ◽  
Optical Absorption Spectroscopy ◽  
Thermal Treatments ◽  
X Ray Diffraction ◽  
X Ray ◽  
High Level ◽  
The Impact ◽  
Crystallization Tendency

AbstractThe impact of Nd2O3, MoO3 and RuO2 addition on the competition between the crystallization of apatite Ca2Nd8(SiO4)6O2 and powellite CaMoO4 phases which both may appear in High Level Waste nuclear glass (under certain specific conditions of cooling and glass composition) has been studied on a simplified composition belonging to the system SiO2-Na2O-CaO-Al2O3-B2O3. X-ray diffraction (at room temperature and high temperature) and scanning electron microscopy measurements have been performed on five glasses under two different thermal treatments. We show that RuO2 acts as a nucleating agent for apatite. Moreover, neodymium and molybdenum cations seem to be very close in the glassy network as Nd2O3 addition stops the phase separation of molybdates and inhibits the crystallization of CaMoO4. On the contrary, MoO3 seems to favor the crystallization of apatite. For several samples, the evolution of the distribution of Nd3+ cations after crystallization was followed by optical absorption spectroscopy.

scholarly journals Study of The Effect of TiO2 Addition On The Crystalline Phases, Structure and Chemical Durability of a Nuclear Glass Ceramic

2021 ◽  
Author(s):  
Rafika SOUAG ◽  
Nour elhayet KAMEL ◽  
Dalila Moudir ◽  
Yasmina MOUHEB ◽  
Fayrouz Aouchiche
Keyword(s):  
Glass Ceramic ◽  
Glass Ceramics ◽  
Ceramic Materials ◽  
Chemical Durability ◽  
Aluminosilicate Glass ◽  
High Level Waste ◽  
X Ray Diffraction ◽  
Complex Chemical Composition ◽  
High Level ◽  
Selection Of

Abstract This study focused on the effect of TiO 2 addition on the crystallines phases’ formation, structure and chemical durability of a nuclear glass ceramic constituted by an aluminosilicate glass in the system: SiO2-Al2O3-CaO-MgO-ZrO2-TiO2 . The materials with four contents of TiO2 , ranging from 4.11 to 7.11 wt.%, are synthesized by a discontinuous method,. For the whole of materials, X-ray diffraction analysis allow identifying an aluminosilicate belonging to pyroxenes silicates family as a main phase, powelite and calzirtite. Both SEM and DTAanalyses confirmed these results. The materials FTIR analysis reveals the glass ceramics complex chemical composition. MCC1 and MCC2 tests, performed on selected glass ceramic materials, indicate that the materials with 4.11 and 5.11 wt.% TiO2 are the most durable against Si, Al, Mg and Ce elements release, in MCC2 test; The results make conclusions valuable on the selection of such glass ceramics as candidate for the disposal of high-level waste.

scholarly journals Study on Structure and Properties of La2O3-Doped Basaltic Glasses for Immobilizing Simulated Lanthanides

Materials ◽  
2021 ◽  
Vol 14 (16) ◽  
pp. 4709
Author(s):  
Qin Tong ◽  
Jichuan Huo ◽  
Xingquan Zhang ◽  
Zhu Cui ◽  
Yongchang Zhu
Keyword(s):  
Thermal Stability ◽  
Chemical Stability ◽  
Glass Network ◽  
Waste Form ◽  
High Level Waste ◽  
Basaltic Glass ◽  
Consistency Test ◽  
Simulated Waste ◽  
High Level ◽  
Simulated High Level Waste

The La2O3-doped basaltic glass simulated high-level waste form (HLW) was prepared by the solid-state melt method. The simulated waste La2O3 maximum loading and the doping effect on structure, thermal stability, leaching behavior, density, and hardness of basaltic glasses were studied. XRD and SEM results show that the simulated waste loading of La2O3 in basaltic glass can be up to ~46 wt.%, and apatite (CaLa4(SiO4)3O) precipitates when the content of La2O3 reaches 56 wt.%. Raman results indicate that the addition of La2O3 breaks the Si–O–Si bond of large-membered and four-membered, but the number of A13+ involved in the formation of the network increase. Low content of La2O3 can help to repair the glass network, but it destroys the network as above 26 wt.%. DSC results show the thermal stability of simulated waste forms first increases and then decreases with the increase of La2O3 content. With the increase of La2O3 content, the density of the simulated waste form increases, and the hardness decreases. The leaching chemical stability of samples was evaluated by the ASTM Product Consistency Test (PCT) Method, which show that all the samples have good chemical stability. The leaching rates of La and Fe are three orders of magnitude lower than those of the other elements. Among them, L36 has the best comprehensive leaching performance.

scholarly journals Vitrification of High-Level Waste at the Savannah River Site

2009 ◽  
Vol 1193 ◽  
Author(s):  
Kevin M. Fox ◽  
David K. Peeler
Keyword(s):  
Savannah River Site ◽  
High Level Waste ◽  
Chemical Compositions ◽  
Savannah River ◽  
Slow Cooling ◽  
Consistency Test ◽  
And Performance ◽  
High Level ◽  
River Site ◽  
Glass Compositions

The objective of this study was to experimentally measure the properties and performance of a series of glasses with compositions that could represent high level waste Sludge Batch 5 (SB5) as vitrified at the Savannah River Site Defense Waste Processing Facility. These data were used to guide frit optimization efforts as the SB5 composition was finalized. Glass compositions for this study were developed by combining a series of SB5 composition projections with a group of candidate frits. The study glasses were fabricated using depleted uranium and their chemical compositions, crystalline contents and chemical durabilities were characterized. Trevorite was the only crystalline phase that was identified in a few of the study glasses after slow cooling, and is not of concern as spinels have been shown to have little impact on the durability of high level waste glasses. Chemical durability was quantified using the Product Consistency Test (PCT). All of the glasses had very acceptable durability performance. The results of this study indicate that a frit composition can be identified that will provide a processable and durable glass when combined with SB5.

scholarly journals X-Ray Diffraction and Product Consistency Test Results for the Phase 6 Study of Nepheline Formation in High-Level Waste Glasses

2019 ◽  
Author(s):  
Charmayne Lonergan ◽  
Jared Kroll ◽  
Chloe Skidmore ◽  
Zayne Nelson ◽  
John Vienna
Keyword(s):  
High Level Waste ◽  
Test Results ◽  
X Ray Diffraction ◽  
Consistency Test ◽  
X Ray ◽  
High Level

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.

The Impact of Fly Ash after SNCR Treated with Tannin-Based Products on AAC Production

2019 ◽  
Vol 296 ◽  
pp. 173-179 ◽  
Author(s):  
Matěj Lédl ◽  
Lucie Galvánková ◽  
Rostislav Drochytka
Keyword(s):  
Compressive Strength ◽  
Fly Ash ◽  
Bulk Density ◽  
Catalytic Reduction ◽  
Xrd Analysis ◽  
Gaseous Ammonia ◽  
X Ray Diffraction ◽  
Consistency Test ◽  
Effect Of Treatment ◽  
The Impact

This paper is focused on the effect of treatment of fly ash after selective non-catalytic reduction (SNCR) with tannin on autoclaved aerated concrete (AAC) production in order to reduce or stop ammonia leakage from the fresh mixture due to its alkalinity. A pure form of tannin and a tannin-based product „Farmatan“ were used as a treatment in dosage ranging from 0,5 g – 3 g of agent per 1 kg of fly ash. Efficient dosage was determined at 2 wt.% of fly ash by the speed of an indicator change due to gaseous ammonia diluted in water. The rheological properties of fresh mixtures were observed by consistency test in Viskomat showing that Farmatan causes delay of hydration. The results of bulk density and compressive strength testing revealed that Farmatan causes an increase of bulk density and at higher amount decreases the compressive strength because of thermal crack formation due to combined effect of delayed hydration and thixotropy. Using x-ray diffraction (XRD) analysis there were no differences in phase composition observed.

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