898 research outputs found
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CLOSURE OF HLW TANKS FORMULATION FOR A COOLING COIL GROUT
The Tank Closure and Technology Development Groups are developing a strategy for closing the High Level Waste (HLW) tanks at the Savannah River Site (SRS). Two Type IV tanks, 17 and 20 in the F-Area Tank Farm, have been successfully filled with grout. Type IV tanks at SRS do not contain cooling coils; on the other hand, the majority of the tanks (Type I, II, III and IIIA) do contain cooling coils. The current concept for closing tanks equipped with cooling coils is to pump grout into the cooling coils to prevent pathways for infiltrating water after tank closure. This task addresses the use of grout to fill intact cooling coils present in most of the remaining HLW tanks on Site. The overall task was divided into two phases. Phase 1 focused on the development of a grout formulation (mix design) suitable for filling the HLW tank cooling coils. Phase 2 will be a large-scale demonstration of the filling of simulated cooling coils under field conditions using the cooling coil grout mix design recommended from Phase 1. This report summarizes the results of Phase 1, the development of the cooling coil grout formulation. A grout formulation is recommended for the full scale testing at Clemson Environmental Technology Laboratory (CETL) that is composed by mass of 90% Masterflow (MF) 816 (a commercially available cable grout) and 10% blast furnace slag, with a water to cementitious material (MF 816 + slag) ratio of 0.33. This formulation produces a grout that meets the fresh and cured grout requirements detailed in the Task Technical Plan (2). The grout showed excellent workability under continuous mixing with minimal change in rheology. An alternative formulation using 90% MF 1341 and 10% blast furnace slag with a water to cementitious material ratio of 0.29 is also acceptable and generates less heat per gram than the MF 816 plus slag mix. However this MF 1341 mix has a higher plastic viscosity than the MF 816 mix due to the presence of sand in the MF 1341 cable grout and a lower water to solids ratio. Nevertheless, the higher viscosity grout may still meet the requirements for the cooling coil grout under certain pumping conditions or alternatively, the mix may be made more fluid by a short period of high shear mixing during production. The mixes have not been optimized for large scale production. It may be possible, for example, to adjust the water to cementitious materials ratio to provide improved performance of these mixes based on the results and conclusions of the large scale testing at CETL. Recommendations from this task include incorporation of a backup mixing/pumping system that is either integrated into the system or is available for immediate use in case of a pump or mixer failure of the primary system. A second recommendation is to conduct a laboratory scale investigation to determine the impact of operational variation on the properties of the grout. This effort would be initiated after feedback is received from the large scale testing at CETL. The purpose of this proposed variability testing is to better understand the limits of the operational variations (such as temperature and mixing time), and to identify possible approaches for remediation to ensure that the grout produced will flow effectively in the coils while still meeting the performance requirements
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POTENTIAL IMPACT OF BLENDING RESIDUAL SOLIDS FROM TANKS 18/19 MOUNDS WITH TANK 7 OPERATIONS
High level waste tanks 18F and 19F have residual mounds of waste which may require removal before the tanks can be closed. Conventional slurry pump technology, previously used for waste removal and tank cleaning, has been incapable of removing theses mounds from tanks 18F and 19F. A mechanical cleaning method has been identified that is potentially capable of removing and transferring the mound material to tank 7F for incorporation in a sludge batch for eventual disposal in high level waste glass by the Defense Waste Processing Facility. The Savannah River National Laboratory has been requested to evaluate whether the material transferred from tanks 18F/19F by the mechanical cleaning technology can later be suspended in Tank 7F by conventional slurry pumps after mixing with high level waste sludge. The proposed mechanical cleaning process for removing the waste mounds from tanks 18 and 19 may utilize a high pressure water jet-eductor that creates a vacuum to mobilize solids. The high pressure jet is also used to transport the suspended solids. The jet-eductor system will be mounted on a mechanical crawler for movement around the bottom of tanks 18 and 19. Based on physical chemical property testing of the jet-eductor system processed IE-95 zeolite and size-reduced IE-95 zeolite, the following conclusions were made: (1) The jet-eductor system processed zeolite has a mean and median particle size (volume basis) of 115.4 and 43.3 microns in water. Preferential settling of these large particles is likely. (2) The jet-eductor system processed zeolite rapidly generates settled solid yield stresses in excess of 11,000 Pascals in caustic supernates and will not be easily retrieved from Tank 7 with the existing slurry pump technology. (3) Settled size-reduced IE-95 zeolite (less than 38 microns) in caustic supernate does not generate yield stresses in excess of 600 Pascals in less than 30 days. (4) Preferential settling of size-reduced zeolite is a function of the amount of sludge and the level of dilution for the mixture. (5) Blending the size-reduced zeolite into larger quantities of sludge can reduce the amount of preferential settling. (6) Periodic dilution or resuspension due to sludge washing or other mixing requirements will increase the chances of preferential settling of the zeolite solids. (7) Mixtures of Purex sludge and size-reduced zeolite did not produce yield stresses greater than 200 Pascals for settling times less than thirty days. Most of the sludge-zeolite blends did not exceed 50 Pascals. These mixtures should be removable by current pump technology if sufficient velocities can be obtained. (8) The settling rate of the sludge-zeolite mixtures is a function of the ionic strength (or supernate density) and the zeolite- sludge mixing ratio. (9) Simulant tests indicate that leaching of Si may be an issue for the processed Tank 19 mound material. (10) Floating zeolite fines observed in water for the jet-eductor system and size-reduced zeolite were not observed when the size-reduced zeolite was blended with caustic solutions, indicating that the caustic solutions cause the fines to agglomerate. Based on the test programs described in this report, the potential for successfully removing Tank 18/19 mound material from Tank 7 with the current slurry pump technology requires the reduction of the particle size of the Tank 18/19 mound material
Sorption and fractionation of dissolved organic matter and associated phosphorus in agricultural soil
Molibility of dissolved organic matter (DOM) strongly affects the export of nitrogen (N) and phosphorus (P) from oils to surface waters. To study the sorption an mobility of dissolved organic C and P (DOC, DOP) in soil, the pH-dependent sorption of DOM to samples from Ap, EB, and Bt horizons from a Danish agircultural Humic Hapludult was investigated and a kinetic model applicable in field-scale model tested. Sorption experiments of 1 to 72 h duration were conducted at two pH levels (pH 5.0 and 7.0) and six initial DOC concentrtions (0-4.7 mmol L-1). Most sorption/desorption occurred during the first few hours. Dissolved organic carbon and DOP sorption decreased strongly with increased pH and desorption dominated at pH 7, especially for DOC. Due to fractionation during DOM sorption/desorption at DOC concentrations up to 2 mmol L-1, the solution fraction of DOM was enriched in P indicating preferred leaching of DOP. The kinetics of sorption was expressed as a function of how far the solution DOC or DOP concentrations deviate from "equilibrium". The model was able to simulate the kinetics of DOC and DOP sorption/desorption at all concentrations investigated and at both pH levels making it useful for incorporation in field-scale models for quantifying DOC and DOP dynamics
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IMPACT OF COMPOSITION AND HEAT TREATMENT ON PORE SIZE IN POROUS WALLED HOLLOW GLASS MICROSPHERES
The Savannah River National Laboratory (SRNL) developed a new geometric form: hollow glass microspheres (HGMs), with unique porous walls. The new geometric form combines the existing technology of HGMs with basic glass science knowledge in the realm of glass-in-glass phase separation. Conceptually, the development of a HGM with porous walls (referred to as a PWHGM) provides a unique system in which various media or filling agents can be incorporated into the PWHGM (via transport through the porous walls) and ultimately has the capacity to serve as a functional delivery system in various industrial applications. Applications of these types of systems could range from hydrogen storage, molecular sieves, drug and bioactive delivery systems, to environmental, chemical and biological indicators, relevant to Energy, Environmental Processing and Homeland Security fields. As a specific example, previous studies at SRNL have introduced materials capable of hydrogen storage (as well as other materials) into the interior of the PWHGMs. The goal of this project was to determine if the microstructure (i.e., pore size and pore size distribution) of a PWHGM could be altered or tailored by varying composition and/or heat treatment (time and/or temperature) conditions. The ability to tailor the microstructure through composition or heat treatments could provide the opportunity to design the PWHGM system to accommodate different additives or fill agents. To meet this objective, HGMs of various alkali borosilicate compositions were fabricated using a flame forming apparatus installed at the Aiken County Technical Laboratory (ACTL). HGMs were treated under various heat treatment conditions to induce and/or enhance glass in glass phase separation. Heat treatment temperatures ranged from 580 C to 620 C, while heat treatment times were either 8 or 24 hours. Of the two primary variables assessed in this study, heat treatment temperature was determined to be most effective in changing the porosity of PWHGMs. Pore diameter in a non-heat treated baseline sample is approximately 100 {angstrom} and with heat treatment at 600 C for 8 hours, the diameter is approximately 1000 {angstrom}; an increase of a factor of 10. The results of this study also indicate significant microstructural differences with only a 20 C difference in heat treatment temperature (580 C and 600 C) for constant times. The microstructural changes observed via electron microscopy as a function of heat treatment temperature were confirmed by mercury porosimetry measurements, where considerable increases in pore volume were measured. Under constant heat treatment conditions, composition may impose a secondary effect on the resulting microstructure as micrographs indicate variations in the degree of porosity. Although microstructural differences were observed among the compositions assessed, the magnitude of the impact (i.e., difference in pore size or pore volume) appears to be smaller than that associated with heat treatment temperature. With respect to heat treatment time, the results suggest that the change in the degree of porosity is minimal for samples heat treated between 8 and 24 hours (it should be noted that the assessment of the impact of time on the resulting microstructure was limited to two compositions). The minimal impact of heat treatment time (on the two glasses evaluated) was confirmed by mercury porosimetry measurements indicating that there was a very slight shift in pore diameter and very little increase in pore volume in the baseline sample. Another important parameter, which will need to be considered under manufacturing or operational conditions, is the yield of the HGM and/or PWHGM and the characteristics of the final product (i.e., not only microstructure characteristics, but perhaps strength of the PWHGM for use under certain applications). In this report, yield is defined as the percentage of feed material converted to HGMs or the percentage of HGMs converted to PWHGMs. The yield of HGM formation was found to be a strong function of composition. As the SiO{sub 2} and B{sub 2}O{sub 3} contents are increased or decreased from the baseline composition, the yield is reduced. PWHGM yield doesn't appear to be influenced by composition, but there is a noticeable increase in yield when comparing the non-heat treated samples to those that were heat treated prior to acid leaching. The results of this study suggest that PWHGM microstructures (pore size and pore volume) can be tailored or specifically designed to meet different end-user needs within certain limitations. The primary effect on the resulting microstructure is heat treatment temperature, which can produce a significant shift in pore size or volume even with a very small difference in heat treatment temperature (20 C). The ability to control the microstructure of PWHGMs provides the opportunity to design the PWHGM system to accommodate different additives or fill agents as required
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PREPARATION AND CHARACTERIZATION OF POROUS WALLED HOLLOW GLASS MICROSPHERES
Porous-walled hollow glass microspheres (PWHGMs) of a modified alkali borosilicate composition have been successfully fabricated by combining the technology of producing hollow glass microspheres (HGMs) with the knowledge associated with porous glasses. HGMs are first formed by a powder glass--flame process, which are then transformed to PWHGMs by heat treatment and subsequent treatment in acid. Pore diameter and pore volume are most influenced by heat treatment temperature. Pore diameter is increased by a factor of 10 when samples are heat treated prior to acid leaching; 100 {angstrom} in non-heat treated samples to 1000 {angstrom} in samples heat treated at 600 C for 8 hours. As heat treatment time is increased from 8 hours to 24 hours there is a slight shift increase in pore diameter and little or no change in pore volume
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IMPACT OF INCREASED ALUMINATE CONCENTRATIONS ON PROPERTIES OF SALTSTONE MIXES
One of the goals of the Saltstone variability study is to identify the operational and compositional variables that control or influence the important processing and performance properties of Saltstone mixes. The protocols developed in this variability study are ideally suited as a tool to assess the impact of proposed changes to the processing flow sheet for Liquid Waste Operations (LWO). One such proposal that is currently under consideration is to introduce a leaching step in the treatment of the High Level Waste (HLW) sludge to remove aluminum prior to vitrification at the Defense Waste Processing Facility (DWPF). This leachate would significantly increase the soluble aluminate concentrations as well as the free hydroxide ion concentration in the salt feed that will be processed at the Saltstone Processing Facility (SPF). Consequently, an initial study of the impact of increased aluminate concentration on the Saltstone grout properties was performed. The projected compositions and ranges of the aluminate rich salt stream (which includes the blending strategy) are not yet available and consequently, in this initial report, two separate salt stream compositions were investigated. The first stream starts with the previously projected baseline composition of the salt solution that will be fed to SPF from the Salt Waste Processing Facility (SWPF). The second stream is the solution that results from washing of the current Tank 51 sludge and subsequent transfer of the salt solution to Tank 11. The SWPF simulant has higher nitrate and lower free hydroxide than the Tank 11 simulant. In both of these cases, the aluminate was varied up to a maximum of 0.40 to 0.45M aluminate in order to evaluate the impact of increasing aluminate ion concentration on the grout properties. In general, the fresh grout properties of mixes made with SWPF and Tank 11 simulants were relatively insensitive to an increase in aluminate concentration in the salt solutions. However, the overall trends observed as the aluminate concentration increased in the salt solution were decreased Bingham Plastic yield stress and plastic viscosity, greater flowability of the grout, and reduced gel times and bleed volume for SWPF based mixes. On the other hand, the set times increased significantly with increasing aluminate concentration in the salt solutions. For the SWPF mixes, the set time increased from 1 to 4 days and for the Tank 11 mixes, the set time increased from 1 to 2 days. Heat of hydration measurements were consistent with the increased set times with extended induction periods (2 to 4 days) as aluminate concentration increased in the salt solution. This extended induction period of heat evolution observed with increasing aluminate concentrations must be addressed for Saltstone operations to avoid exceeding temperature limits. It is anticipated that the induction period will be temperature dependent and should be measured for future projections and included in the thermal modeling. The overall heat generation was greater in the mixes containing higher concentrations of aluminate. In fact, for the total heat release values calculated using curve fitting for longer times, the amount of heat was increased by 33% for SWPF based solutions and by 46% for Tank 11 based solutions. The larger amount of heat from mixes containing higher aluminate concentration must be accounted for in the modeling effort which determines the pour schedule for Saltstone. The increased induction periods were shown to be associated with hydration reactions of the blast furnace slag. The rate of heat generation with high aluminate solutions and Portland cement were only accelerated whereas high aluminate mixes containing blast furnace slag only showed the characteristic increase in induction time that was observed with mixes prepared using the premix blend of cementitious materials. It was shown that fly ash does not react significantly during the first seven days of curing but then undergoes an accelerated burst for 15 days before beginning to level off. The total amount of heat generated from a fly ash only mix with SWPF solution containing aluminate at 0.33 M is approximately 100 J/g vs. 87 J/g for SWPF with 0.11 M aluminate. Finally, the heat of hydration measurements revealed that the ternary system of cementitious materials (premix) leads to interactions between the hydration reactions of these three components that actually reduce the overall heat generation compared to the summation of the heats of hydration for mixes made only from portland cement, blast furnace slag or fly ash
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IMPACT OF ALUMINATE IONS ON THE PROPERTIES OF SALTSTONE GROUT MIXES
It is important to identify and control the operational and compositional variables that impact the important processing and performance properties of Saltstone grout mixes. The grout that is produced at the Saltstone Production Facility (SPF) is referred to as Saltstone and is a waste form that immobilizes low concentrations of radionuclides as well as certain toxic metals. The Saltstone will be disposed of in vaults at Savannah River Site (SRS). An effort referred to as the Saltstone Variability Study has been initiated to achieve this goal. The protocols developed in this variability study are also ideally suited as a tool to assess the impact of proposed changes to the processing flow sheet for Liquid Waste Operations at SRS. One such proposal that is currently under consideration is to introduce a leaching step in the treatment of the High Level Waste (HLW) sludge to remove aluminum prior to vitrification at the Defense Waste Processing Facility (DWPF). This leachate would significantly increase the soluble aluminate concentration in the salt feed that will be processed at the SPF. Consequently, an initial study of the impact of increased aluminate concentration on the Saltstone grout properties was performed. Prior work by Lukens (1) showed that aluminate in the salt solutions increases the amount of heat generation
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