EVALUATION OF LOW TEMPERATURE ALUMINUM DISSOLUTION IN TANK 51

Pike, J

Savannah River Site (S.C.)

关键词: Aluminium;    Uranium;    Sludges;    Radioactive Waste Processing;    Dissolution;   

DOI  :  10.2172/938798
RP-ID  :  SRNS-STI-2008-00021
RP-ID  :  DE-AC09-08SR22470
RP-ID  :  938798

美国|英语

来源: UNT Digital Library

【 摘 要 】

Liquid Waste Organization (LWO) identified aluminum dissolution as a method to mitigate the effect of having about 50% more solids in High Level Waste (HLW) sludge than previously planned. Previous aluminum dissolution performed in a HLW tank in 1982 was performed at approximately 85 C for 5 days, which became the baseline aluminum dissolution process. LWO initiated a project to modify a waste tank to meet these requirements. Subsequent to an alternative evaluation, LWO management identified an opportunity to perform aluminum dissolution on sludge destined for Sludge Batch 5, but within a limited window that would not allow time for any modifications for tank heating. A variation of the baseline process, dubbed Low Temperature Aluminum Dissolution (LTAD), was developed based on the constraint of available energy input in Tank 51 and the window of opportunity, but was not constrained to a minimum extent of dissolution, i.e. dissolve as much aluminum as possible within the time available. This process was intended to operate between 55 and 70 C, but for a significantly longer time than the baseline process. LTAD proceeded in parallel with the baseline project. The preliminary evaluation at the completion of LTAD focused on the material balance and extent of the aluminum dissolved. The range of values of extent of dissolution, 56% to 64%, resulted from the variation in liquid phase sample data available at the time. Additional solid phase data is available from a sample taken after LTAD to refine this range. This report provides additional detailed evaluation of the LTAD process based on analytical and field data and includes: a summary of the process chronology; a determination of an acceptable blending strategy for the aluminum-laden supernate stored in Tank 11; an update to the determination of aluminum dissolved using more complete sample results; a determination of the effect of LTAD on uranium, plutonium, and other metals; a determination of the rate of heat loss from a quiescent tank; and an evaluation of the aluminum dissolution rate model and actual dissolution rate. LTAD was successfully completed in Tank 51 with minimal waste tank changes. The following general conclusions may be drawn about the LTAD process: (1) Dissolution at about 60 C for 46 days dissolved 64% of the aluminum from the sludge slurry. (2) The aluminum-laden leach solution decanted to Tank 11 can be blended with a wide variety of supernates without risk of precipitating the dissolved aluminum based on thermodynamic chemical equilibrium models. (3) Uranium and plutonium leached into solution without corresponding leaching of iron or metal other than aluminum, but the total mass leached was a small fraction of the total uranium and plutonium in the sludge. (4) The concentration of uranium and plutonium in the leach solution was indistinguishable from other tank farm supernates, thus, the leach solutions can be managed relative to the risk of criticality like any other supernate. (5) A small amount of mercury leached into solution from the sludge causing the liquid phase concentration to increase 6 to 10 fold, which is consistent with the 4 to 14 fold increase observed during the 1982 aluminum dissolution demonstration. (6) Chromium did not dissolve during LTAD. (7) Chloride concentration increased in the liquid phase during LTAD due to chloride contamination in the 50% sodium hydroxide solution. (8) The rate of heat loss from Tank 51 at temperatures above 45 C appeared linear and predictable at 8E+7 cal/hr. (9) The rate of heat transfer from Tank 51 did not follow a simplified bulk heat transfer model. (10) Prediction of the aluminum dissolution rate was prone to error due to a lack of active specific surface area data of sludge particles. (11) The higher than expected dissolution rate during LTAD was likely due to smaller than expected particle sizes of most of the sludge particles. While evaluating the LTAD process, the dissolved salt solution from Tank 41 that was stored and sampled in Tank 49 was determined to be supersaturated relative to aluminum. Supersaturation in Tank 49 is not a risk to LTAD. However, storing and processing of this supernate carries a risk of solids precipitation, primarily in the form of gibbsite or boehmite. Blending with the supernate in Tank 11 neither increases nor decreases this risk. LTAD was initiated as an opportunity to substantially mitigate the planned increase in canister production and DWPF lifecycle after the realization of more sludge solids stored in the HLW tanks. As determined from the preliminary evaluation of LTAD, the direct benefit of the decanted liquid stored in Tank 11 represents 45 canisters at 34% waste loading with potential indirect benefits for much larger reductions. Application of an aluminum dissolution process to the remaining high aluminum content sludge will potentially reduce the planned canister production by several hundred canisters at 34%-38% waste loading.