Liquidus Temperature of Spinel Precipitating High-Level Waste Glasses

1996 ◽  
Vol 465 ◽  
Author(s):  
M. Mika ◽  
M. J. Schweiger ◽  
J. D. Vienna ◽  
P. Hrma
Keyword(s):  
Mixture Models ◽  
Crystalline Phase ◽  
Liquidus Temperature ◽  
Glass Composition ◽  
High Level Waste ◽  
Hanford Site ◽  
High Iron ◽  
Negative Effect ◽  
High Level ◽  
Glass Viscosity

ABSTRACTThe liquidus temperature (TL) often limits the loading of high-level waste in glass through the constraint that TL must be at least 100°C below the temperature at which the glass viscosity is 5 Pa-s. In this study, values of TL for spinel primary crystalline phase were measured as a function of glass composition. The test glasses were based on high-iron Hanford Site tank wastes. All studied glasses precipitated spinel (Ni,Fe,Mn)(Cr,Fe)2O4 as the primary crystalline phase. TL was increased by additions of Cr2O3, NiO, Al2O3, Fe2O3, MgO, and MnO; while Li2O, Na2O, B2O3, and SiO2 had a negative effect. Empirical mixture models were fitted to data.

Liquidus Temperature Model for Hanford High-Level Waste Glasses with High Concentrations of Zirconia

1996 ◽  
Vol 465 ◽  
Author(s):  
J. V. Crum ◽  
M. J. Schweiger ◽  
P. Hrma ◽  
J. D. Vienna
Keyword(s):  
Crystalline Phase ◽  
Liquidus Temperature ◽  
Heat Treating ◽  
Primary Phase ◽  
High Level Waste ◽  
Mass Fractions ◽  
High Concentrations ◽  
Phase Glass ◽  
High Level ◽  
Temperature Furnace

ABSTRACTA study was conducted on glasses based on a simulated transuranic waste with high concentrations of ZrO2and Bi2O3 to determine the compositional dependence of primary crystalline phases and liquidus temperature (TL). Starting from a baseline composition, glasses were formulated by changing mass fractions of Al2O3, B2O3, Bi2O3, CeO2, Li2O, Na2O, P2O5, SiO2, and ZrO2, one at a time, while keeping the remaining components in the same relative proportions as in the baseline glass. Liquidus temperature was measured by heat treating glass samples for 24 h in a uniform temperature furnace. The primary crystalline phase in the baseline glass and the majority of the glasses was zircon (ZrSiO4). A change in the concentration of certain components (Al2O3, ZrO2, Li2O, B2O3 and SiO2) changed the primary phase to baddeleyite (ZrO2), while cerium oxide (CeO2) precipitated from glasses with more than 3 wt% CeO2. Zircon TL was strongly increased by Al2O3, Zrb2 and CeO2, and slightly by P2O5 and SiO2; decreased strongly by Li2O and Na2O and moderately by B2O3. A first-order model was constructed for TL as a function of composition for zircon primary crystalline phase glass.

scholarly journals The effect of high-level waste glass composition on spinel liquidus temperature

2014 ◽  
Vol 384 ◽  
pp. 32-40 ◽  
Author(s):  
Pavel Hrma ◽  
Brian J. Riley ◽  
Jarrod V. Crum ◽  
Josef Matyas
Keyword(s):  
Liquidus Temperature ◽  
Glass Composition ◽  
Waste Glass ◽  
High Level Waste ◽  
High Level

Study of Glass-Ceramic Waste Forms

1997 ◽  
Vol 506 ◽  
Author(s):  
S.V. Stefanovsky ◽  
S.V. Ioudintsev ◽  
B.S. Nikonov ◽  
B.I. Omelianenko ◽  
T.N. Lashtchenova
Keyword(s):  
Glass Ceramic ◽  
Glass Composition ◽  
Glass Ceramics ◽  
High Level Waste ◽  
Matrix Glass ◽  
Crystalline Phases ◽  
Cell Parameters ◽  
The Matrix ◽  
High Level ◽  
Similar Unit

ABSTRACTSince the early of the 1990s the method of inductive melting in a cold crucible (IMCC) has been applied at SIA “Radon” for production of various wasteforms, including glasses and Synroc-type ceramics. Sphene-based glass-ceramics composed of glass and crystalline phases were considered as appropriate wasteform for High Level Waste immobilisation. Investigation of two glass-ceramic specimens prepared with the IMCC has been performed using optical microscopy, XRD, SEM/EDS, and TEM methods. The samples produced consist of vitreous and crystalline phases. The vitreous phase consists of two varieties of glass formed by the immiscibility of the initial melt onto two separate liquids. One of the glasses is observed as spherical microinclusions in the matrix glass. The glass of the microspheres are differed from the matrix glass composition by higher contents of Ca, Ti, Ce, Sr, Zr (or Cr), while the matrix glass contains higher amounts of Si, Al, and alkalies. The crystalline phases with sphene- and perrierite-like structures have been also occurred. Their total quantity reaches up to 50 vol.%. The synthetic perrierite has similar unit-cell parameters with its natural mineral analogs with the only exception in two-fold value of c dimension. Zr, Ce, and Sr are incorporated into synthetic sphene and perrierite, while Cs is hosted by the glass phases.

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.

Improved Third Generation Peristaltic Crawler for Removal of High-Level Waste Plugs in United States Department of Energy Hanford Site Pipelines

2013 ◽  
Author(s):  
Gabriela Vazquez ◽  
Tomas Pribanic
Keyword(s):  
Fatigue Testing ◽  
Experimental Tests ◽  
Department Of Energy ◽  
High Level Waste ◽  
Pipeline System ◽  
United States Department ◽  
Third Generation ◽  
Test Bed ◽  
Hanford Site ◽  
High Level

There are approximately 56 million gallons (212km3) of high level waste (HLW) at the U.S. Department of Energy (DOE) Hanford Site. It is scheduled that by the year 2040, the HLW is to be completely transferred to secure double-shell tanks (DST) from the leaking single-tanks (SST) via transfer pipeline system. Blockages have formed inside the pipes during transport because of the variety in composition and characteristics of the waste. These full and partial plugs delay waste transfers and require manual intervention to repair, therefore are extremely expensive, consuming millions of dollars and further threatening the environment. To successfully continue the transfer of waste through the pipelines, DOE site engineers are in need of a technology that can accurately locate the blockages and unplug the pipelines. In this study, the proposed solution to remediate blockages formed in pipelines is the use of a peristaltic crawler: a pneumatically/hydraulically operated device that propels itself in a worm-like motion through sequential fluctuations of pressure in its air cavities. The crawler is also equipped with a high-pressure water nozzle used to clear blockages inside the pipelines. The crawler is now in its third generation. Previous generations showed limitations in its durability, speed, and maneuverability. Latest improvements include an automation of sequence that prevents kickback, a front-mounted inspection camera for visual feedback, and a thinner wall outer bellow for improved maneuverability. Different experimental tests were conducted to evaluate the improvements of crawler relative to its predecessors using a pipeline test-bed assembly. Anchor force tests, unplugging tests, and fatigue testing for both the bellow and rubber rims have yet to be conducted and thus results are not presented in this research. Experiments tested bellow force and response, cornering maneuverability, and straight line navigational speed. The design concept and experimental test results are reported.

Spinel Settling in HLW Melters

2001 ◽  
Author(s):  
Josef Matyáš ◽  
Jaroslav Kloužek ◽  
Lubomír Němec ◽  
Miroslav Trochta
Keyword(s):  
Liquidus Temperature ◽  
Linear Growth ◽  
Critical Level ◽  
High Level Waste ◽  
Input Concentration ◽  
Average Temperature ◽  
Input Size ◽  
Waste Loading ◽  
High Level ◽  
The Impact

Abstract The efficiency of high-level waste (HLW) melters is limited by spinel settling and accumulation on the melter bottom if the waste loading is increased above a certain limit at which spinel crystallizes from the melt. Spinel accumulation interferes with melter operation and shortens melter lifetime. The mathematical modeling of spinel settling in a HLW melter was applied to define the critical level of spinel deposition during the lifetime of the melter and the corresponding increase in waste loading. In this study, spinel settled on the bottom, slant melter walls, and in the output pipe with a linear growth of spinel-sludge thickness after its concentration stabilized inside the melter. The calculations provided a higher concentration of spinel crystals in the melter regions where the temperature was lower then the liquidus temperature, i.e., T<TL. The effects of the following parameters on sludge-layer thickness were examined: 1) the impact of input concentration of spinel crystals of the same size, 2) the impact of different input size of spinel crystals of the same concentration entering from cold cap (melting batch on the melt surface), and 3) the influence of the average temperature (Tavg) inside of the melting space. The calculations showed that higher a concentration and bigger crystals caused thicker sludge layers in the melter, either because of a higher settling density of crystals or because of their higher settling rate. The nucleation of spinel crystals plays a more important role with decreasing of average temperature inside of the melter, and the thicker layer was formed at lower average temperatures.

Studies of the Fundamental Chemistry of Hanford Tank Sludges

2003 ◽  
Author(s):  
Gregg J. Lumetta ◽  
Brian M. Rapko ◽  
Herman M. Cho
Keyword(s):  
Complex Mixture ◽  
Chemical Species ◽  
Department Of Energy ◽  
High Level Waste ◽  
Resonance Spectroscopy ◽  
X Ray Diffraction ◽  
Hanford Site ◽  
Mineral Phases ◽  
Fe Oxyhydroxides ◽  
High Level

The U.S. Department of Energy has embarked on an effort to retrieve, immobilize, and dispose of the 2.1 × 105 m3 of radioactive tank wastes that were generated during weapons production and other operations at the Hanford Site in Washington State. One of the major challenges associated with this effort is the processing of the 4.2 × 104 m3 of high-level waste sludges. These sludges consist of a complex mixture of amorphous and crystalline mineral phases. The current plan for processing the sludge solids consists of leaching with aqueous NaOH, washing out the NaOH and dissolved components, then vitrifying the solids in borosilicate glass. The purpose of the NaOH leaching step is to remove components such as Al, Cr, and P that can lead to the production of an unacceptable quantity of high-level waste glass. In this paper, we will discuss the chemistry underlying the leaching and washing processes, focusing on the specific mineral phases present in the sludge solids and how these phases respond to the leaching process. The chemical phases present in the Hanford tank sludge solids have been identified through microscopy coupled with electron diffraction and through powder X-ray diffraction. We have also recently been applying nuclear magnetic resonance spectroscopy to characterize chemical species in tank sludge solids. Numerous chemical species have been identified including the aluminum oxy/hydroxides gibbsite and boehmite, aluminosilicates, iron oxy/hydroxides, and mixed Cr/Fe oxyhydroxides. Identification of these phases has led to a more fundamental understanding of the behavior of the various sludge components during leaching; in turn, this understanding will allow for improved process flow sheets. For example, we have shown that certain tank sludges are high in boehmite, Υ-AIOOH. This mineral phase is much more refractory than other AI phases such as gibbsite. Thus, more severe leaching conditions (e.g., increased temperature, NaOH concentration, and leaching duration) are required to remove AI from wastes high in boehmite.

Parametric Study of the Corrosion Behaviour in Static Distilled Water of Simulated European Reference High Level Waste Glasses

1984 ◽  
Vol 44 ◽  
Author(s):  
Pierre Ph. Van Iseghem ◽  
W. Timmermans ◽  
R. De Batist
Keyword(s):  
Diffusion Processes ◽  
Glass Composition ◽  
Corrosion Behaviour ◽  
Research Programme ◽  
Community Research ◽  
High Level Waste ◽  
Distilled Water ◽  
Controlling Mechanism ◽  
Saturation Effects ◽  
High Level

AbstractThe corrosion behaviour in distilled water of five simulated European reference high level waste glasses has been investigated for times up to 8 months. The glasses were chosen in accordance with the Joint European Community research programme on HLW form characterization: two French glasses (SON58, SON64), one British glass (UK209) and two glasses designed to incorporate HLW stored at the Eurochemic plant in Belgium (SM58 and SAN60). In the reference condition (90°C, SA.V−1 = 1 cm−1) the leaching was characterized mainly by diffusion processes and by the onset of saturation in the leachate (these saturation effects were found to depend on glass composition). In more dilute conditions (SA.V−1 = 0.1 cm−1), matrix dissolution was the rate controlling mechanism. Increasing the leachant temperature to 150°C and higher lead to pronounced surface crystallization and, at least for one glass (SAN60), to an increased corrosion.

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