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At least 631 records · Page 35

Contaminant Leach Testing of Hanford Tank 241-C-104 Residual Waste

Leach testing of Tank C-104 residual waste was completed using batch and column experiments. Tank C-104 residual waste contains exceptionally high concentrations of uranium (i.e., as high as 115 mg/g or 11.5 wt.%). This study was conducted to provide data to develop contaminant release models for Tank C-104 residual waste and Tank C-104 residual waste that has been treated with lime to transform uranium in the waste to a highly insoluble calcium uranate (CaUO4) or similar phase. Three column leaching cases were investigated. In the first case, C-104 residual waste was leached with deionized water. In the second case, crushed grout was added to the column so that deionized water contacted the grout prior to contacting the waste. In the third case, lime was mixed in with the grout. Results of the column experiments demonstrate that addition of lime dramatically reduces the leachability of uranium from Tank C-104 residual waste. Initial indications suggest that CaUO4 or a similar highly insoluble calcium rich uranium phase forms as a result of the lime addition. Additional work is needed to definitively identify the uranium phases that occur in the as received waste and the waste after the lime treatment.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Investigation of thermolytic hydrogen generation rate of tank farm simulated and actual waste

To support resolution of Potential Inadequacies in the Safety Analysis for the Savannah River Site (SRS) Tank Farm, Savannah River National Laboratory conducted research to determine the thermolytic hydrogen generation rate (HGR) with simulated and actual waste. Gas chromatography methods were developed and used with air-purged flow systems to quantify hydrogen generation from heated simulated and actual waste at rates applicable to the Tank Farm Documented Safety Analysis (DSA). Initial simulant tests with a simple salt solution plus sodium glycolate demonstrated the behavior of the test apparatus by replicating known HGR kinetics. Additional simulant tests with the simple salt solution excluding organics apart from contaminants provided measurement of the detection and quantification limits for the apparatus with respect to hydrogen generation. Testing included a measurement of HGR on actual SRS tank waste from Tank 38. A final series of measurements examined HGR for a simulant with the most common SRS Tank Farm organics at temperatures up to 140 °C. The following conclusions result from this testing.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Analysis of the tank 6f final characterization samples-2012

The Savannah River National Laboratory (SRNL) was requested by Savannah River Remediation (SRR) to provide sample preparation and analysis of the Tank 6F final characterization samples to determine the residual tank inventory prior to grouting. Fourteen residual Tank 6F solid samples from three areas on the floor of the tank were collected and delivered to SRNL between May and August 2011.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Effect of Na Concentration on Cs Distribution with Crystalline Silicotitanate in Tank Waste Simulants

Crystalline silicotitanate (CST) ion exchange media is currently utilized in the tank side cesium removal (TSCR) system on the Hanford site to remove Cs-137 from the tank waste supernate. As the main dose contributor to the liquid supernate in Hanford tank waste, it is necessary to remove the Cs-137 to expedite low activity waste processing and immobilization. Ongoing batch contact experiments with CST have been done to tease out the impact of group II metals, anions, potassium, and temperature on Cs removal to better understand bounding conditions for operations as well as aid in development of a wholesome isotherm model to predict Cs behavior in the tank waste. This paper discusses the impact of Na concentration on Cs exchange and provides insight into the challenges associated with activity coefficient estimations for modeling Cs distribution in tank waste matrices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Investigation of public exposure resulted from the radioiodine delay tank facility of nuclear medicine department

The study is carried out to assess the exposure rate that could contribute to public exposure in a radioiodine ward delay tank facility of Radiotherapy, Oncology and Nuclear Medicine, Department, Hospital Universiti Sains Malaysia (HUSM). The exposure rate at several locations including the delay tank room, doorway and at the public walking route was measured using Victoreen 415P-RYR survey meter. The radioactive level of the {sup 131}I waste was measured using Captus 3000 well counting system. The results showed that exposure rate and total count of the delay tank sample increased when the radioiodine ward was fully occupied with patient and reduced when the ward was vacant. Occupancy of radioiodine ward for two consecutive weeks had dramatically increased the exposure rate around the delay tank and radioactive level of {sup 131}I waste. The highest exposure rate and radioactive level was recorded when the ward was occupied for two consecutive weeks with 177.00 µR/h and 58.36 kcpm respectively. The exposure rate decreased 15.76 % when the door of the delay tank room was closed. The exposure rate at public walking route decreased between 15.58 % and 36.92 % as the distance increased between 1 and 3 m.

61 RADIATION PROTECTION AND DOSIMETRY↗

Cesium Ion Exchange Testing Using Crystalline Silicotitanate with Hanford Tank Waste 241-AP-107

Pacific Northwest National Laboratory has been tasked with demonstrating the unit operations for the Low Activity Waste Pretreatment System with actual Hanford tank waste. Crystalline silicotitanate (CST) ion exchange media is planned to be used to remove cesium (137Cs) from the aqueous phases of the tank wastes. Washington River Protection Solutions requested that Hanford tank waste collected from tank 241-AP-107 be processed using conceived pretreatment steps (suspended solids removal by filtration, Cs removal by ion exchange), then vitrified. Removal of Cs from these wastes is an important processing step in preparing the waste for long-term safe storage. Bench-scale ion exchange testing with approximately 9 L of filtered AP-107 supernate was conducted using CST. Column testing was performed using prototypic LAWPS operations in a lead-lag column arrangement using 10-mL CST beds. Feed was processed until the lag column effluent reached the Hanford Tank Waste Treatment and Immobilization Plant waste acceptance criteria (WAC) for receiving supernatant waste for vitrification (a function of the Na and 137Cs concentrations), at which point, a new lag column was needed to continue processing and the original lag column was moved to the lead position. Greater than 99% of the Cs processed through the ion exchange system was collected on the CST in the columns. The AP-107 feed and column processing effluent underwent extensive characterization to better define waste characteristics and assess fractionation to the CST. Selected lead column samples were analyzed to assess particular metal analyte load characteristics. Results of these analyses will be discussed.

cesium exchange, Hanford tank waste, ion exchange↗

Rocking response of liquid-filled cylindrical tanks

The hydrodynamic response of liquid-filled storage tanks subjected to translational earthquake shaking has been the focus of studies for more than 75 years. In service, tanks experience six components of seismic input, with rocking due to support flexibility and/or rotational components of ground motion. Published theory for predicting hydrodynamic responses in rigid cylindrical tanks due to rotational seismic input is examined. Analytical solutions for pressure in the fluid and on the tank wall, and base moment are modified to account for the effects of angular displacements at the base. A finite element model of a water-filled cylindrical tank using the Arbitrary Lagrangian and Eulerian (ALE) solver in LS-DYNA is used to demonstrate the efficacy of the proposed expressions for three base rocking motions. Results from the modified analytical solutions and the finite element model are in excellent agreement.

58 GEOSCIENCES↗

HANFORD TANK CLEANUP UPDATE

Access to Hanford's single-shell radioactive waste storage tank C-107 was significantly improved when workers completed the cut of a 55-inch diameter hole in the top of the tank. The core and its associated cutting equipment were removed from the tank and encased in a plastic sleeve to prevent any potential spread of contamination. The larger tank opening allows use of a new more efficient robotic arm to complete tank retrieval.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

RESULTS FOR THE FIRST QUARTER 2011 TANK 50 WAC SLURRY SAMPLE: CHEMICAL AND RADIONUCLIDE CONTAMINANT RESULTS

This report details the chemical and radionuclide contaminant results for the characterization of the 2011 First Quarter sampling of Tank 50 for the Saltstone Waste Acceptance Criteria (WAC). Information from this characterization will be used by Waste Solidification Engineering (WSE) to support the transfer of low-level aqueous waste from Tank 50 to the Salt Feed Tank in the Saltstone Facility in Z-Area, where the waste will be immobilized. This information is also used to update the Tank 50 Waste Characterization System. The following conclusions are drawn from the analytical results provided in this report: (1) The concentrations of the reported chemical and radioactive contaminants were less than their respective WAC targets or limits unless noted in this section; (2) The reported detection limit for {sup 59}Ni is above both the requested limits from Reference 2 and the established limits in Reference 3; (3) The reported detection limit for {sup 94}Nb is above the requested limit from Reference 2; however, it is below the established limits in Reference 3. This is a change from previously reported results; (4) The reported concentration of {sup 242m}Am is above the target in Listed in Attachment 8.4 of the Saltstone WAC. This is a change from the previously reported results; (5) {sup 247}Cm and {sup 249}Cf are above the requested limits from Reference 2. However, they are below the limits established in Reference 3; (6) The reported detection limit for Norpar 13 is greater than the limit from Table 4 and Attachment 8.2 of the WAC; (7) The reported detection limit for Isopar L is greater than the limit from Table 3 of the WAC; and (8) Isopar L and Norpar 13 have limited solubility in aqueous solutions making it difficult to obtain consistent and reliable sub-samples. The values reported in this memo are the concentrations in the sub-sample as detected by the instrument; however, the results may not accurately represent the concentrations of the analytes in Tank 50.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

OXALATE MASS BALANCE DURING CHEMICAL CLEANING IN TANK 6F

The Savannah River Remediation (SRR) is preparing Tank 6F for closure. The first step in preparing the tank for closure is mechanical sludge removal. Following mechanical sludge removal, SRS performed chemical cleaning with oxalic acid to remove the sludge heel. Personnel are currently assessing the effectiveness of the chemical cleaning to determine whether the tank is ready for closure. SRR personnel collected liquid samples during chemical cleaning and submitted them to Savannah River National Laboratory (SRNL) for analysis. Following chemical cleaning, they collected a solid sample (also known as 'process sample') and submitted it to SRNL for analysis. The authors analyzed these samples to assess the effectiveness of the chemical cleaning process. Analysis of the anions showed the measured oxalate removed from Tank 6F to be approximately 50% of the amount added in the oxalic acid. To close the oxalate mass balance, the author collected solid samples, leached them with nitric acid, and measured the concentration of cations and anions in the leachate. Some conclusions from this work are: (1) Approximately 65% of the oxalate added as oxalic acid was removed with the decanted liquid. (2) Approximately 1% of the oxalate (added to the tank as oxalic acid) formed precipitates with compounds such as nickel, manganese, sodium, and iron (II), and was dissolved with nitric acid. (3) As much as 30% of the oxalate may have decomposed forming carbon dioxide. The balance does not fully account for all the oxalate added. The offset represents the combined uncertainty in the analyses and sampling.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Tanks 18 and 19-F equipment grout fill material evaluation and recommendations

The United States Department of Energy (US DOE) intends to remove Tanks 18-F and 19-F at the Savannah River Site (SRS) from service. The high-level waste (HLW) tanks have been isolated from the F-area Tank Farm (FTF) facilities and will be filled with cementitious grout for the purpose of: (1) physically stabilizing the empty volumes in the tanks, (2) limiting/eliminating vertical pathways from the surface to residual waste on the bottom of the tanks, (3) providing an intruder barrier, and (4) providing an alkaline, chemical reducing environment within the closure boundary to limit solubility of residual radionuclides.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

STATISTICAL ANALYSIS OF TANK 5 FLOOR SAMPLE RESULTS

Sampling has been completed for the characterization of the residual material on the floor of Tank 5 in the F-Area Tank Farm at the Savannah River Site (SRS), near Aiken, SC. The sampling was performed by Savannah River Remediation (SRR) LLC using a stratified random sampling plan with volume-proportional compositing. The plan consisted of partitioning the residual material on the floor of Tank 5 into three non-overlapping strata: two strata enclosed accumulations, and a third stratum consisted of a thin layer of material outside the regions of the two accumulations. Each of three composite samples was constructed from five primary sample locations of residual material on the floor of Tank 5. Three of the primary samples were obtained from the stratum containing the thin layer of material, and one primary sample was obtained from each of the two strata containing an accumulation. This report documents the statistical analyses of the analytical results for the composite samples. The objective of the analysis is to determine the mean concentrations and upper 95% confidence (UCL95) bounds for the mean concentrations for a set of analytes in the tank residuals. The statistical procedures employed in the analyses were consistent with the Environmental Protection Agency (EPA) technical guidance by Singh and others [2010]. Savannah River National Laboratory (SRNL) measured the sample bulk density, nonvolatile beta, gross alpha, radionuclide, inorganic, and anion concentrations three times for each of the composite samples. The analyte concentration data were partitioned into three separate groups for further analysis: analytes with every measurement above their minimum detectable concentrations (MDCs), analytes with no measurements above their MDCs, and analytes with a mixture of some measurement results above and below their MDCs. The means, standard deviations, and UCL95s were computed for the analytes in the two groups that had at least some measurements above their MDCs. The identification of distributions and the selection of UCL95 procedures generally followed the protocol in Singh, Armbya, and Singh [2010]. When all of an analyte's measurements lie below their MDCs, only a summary of the MDCs can be provided. The measurement results reported by SRNL are listed in Appendix A, and the results of this analysis are reported in Appendix B. The data were generally found to follow a normal distribution, and to be homogeneous across composite samples.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Drain Tank Information for Developing Design Basis of the Preliminary Design

Tokamak Cooling Water System (TCWS) drain tanks (DTs) serve two functions: normal operation and safety operation. Normal DTs are used for regular maintenance operations when draining is necessary. Safety DTs are used to receive the water leaked into the Vacuum Vessel (VV) after an in-vessel loss of coolant accident (LOCA) event. The preliminary design of the DTs shall be based on the information provided by this document. The capacity of the normal DTs is estimated based on the internal volume of in-vessel components [e.g., First Wall/Blanket (FW/BLK) and Divertor (DIV)]; Neutral Beam Injector (NBI) components; and TCWS piping, heat exchangers, electric heaters, pump casing, pressurizers, and valves. Water volumes have been updated based on 2004-design information, changes adopted because of approved Project Change Requests (PCRs), and data verification by US ITER and AREVA Federal Services, the US ITER A and E Company. Two tanks will store water from normal draining operations of the FW/BLK and DIV Primary Heat Transfer Systems (PHTSs). One tank will store water from normal draining operations of the NBI PHTS. The capacity of the safety DTs is based on analysis of a design basis accident: a large leak from in-vessel components. There are two safety DTs that will receive water from a VV LOCA event and drainage from the VV, as needed. In addition, there is one sump tank for the DIV that will be used for collecting drain water from the draining and drying processes and specifically for draining the DIV system as the DIV cassette lines are at a lower elevation than the DT connection point. Information documented in this report must be refined and verified during the preliminary design of the DTs, and there are several aspects to be considered to complete the preliminary design. Input to these design considerations is discussed in this report and includes, but is not limited to, water inventory; operating procedures/maintenance; Failure Modes and Effects Analysis (FMEA); tank layout and dimensions, including design margin; classification under French Nuclear Pressure Directives, Equipements Sous Pression Nucleaires (ESPN); and adaptations for construction.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Results for the first quarter 2012 tank 50 wac slurry sample: chemical and radionuclide contaminant results

This report details the chemical and radionuclide contaminant results for the characterization of the 2012 First Quarter sampling of Tank 50 for the Saltstone Waste Acceptance Criteria (WAC). Information from this characterization will be used by Waste Solidification Engineering (WSE) to support the transfer of low-level aqueous waste from Tank 50 to the Salt Feed Tank in the Saltstone Facility in Z-Area, where the waste will be immobilized. This information is also used to update the Tank 50 Waste Characterization System. The following conclusions are drawn from the analytical results provided in this memorandum: (1) The concentrations of the reported chemical and radioactive contaminants were less than their respective WAC targets or limits unless noted in this section; (2) The reported detection limit for {sup 94}Nb is above the requested limit from Reference 2 but below the estimated limit in Reference 3; (3) {sup 247}Cm and {sup 249}Cf are above the requested limits from Reference 2. however, they are below the limits established in Reference 3; (4) The reported detection limit for Norpar 13 is greater than the limit from Table 4 and Attachment 8.2 of the WAC; (5) The reported detection limit for Isopar L is greater than the limit from Table 3 of the WAC; (6) Isopar L and Norpar 13 have limited solubility in aqueous solutions making it difficult to obtain consistent and reliable sub-samples, the values reported in this report are the concentrations in the sub-sample as detected by the instrument; however, the results may not accurately represent the concentrations of the analytes in Tank 50; and (7) The low insoluble solids content increases the measurement uncertainty for insoluble species.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Results For The First Quarter 2012 Tank 50 WAC Slurry Sample: Chemical And Radionuclide Contaminant Results

This report details the chemical and radionuclide contaminant results for the characterization of the 2012 First Quarter sampling of Tank 50 for the Saltstone Waste Acceptance Criteria (WAC). Information from this characterization will be used by Waste Solidification Engineering (WSE) to support the transfer of low-level aqueous waste from Tank 50 to the Salt Feed Tank in the Saltstone Facility in Z-Area, where the waste will be immobilized. This information is also used to update the Tank 50 Waste Characterization System. The following conclusions are drawn from the analytical results provided in this memorandum: The concentrations of the reported chemical and radioactive contaminants were less than their respective WAC targets or limits unless noted; The reported detection limit for 94 Nb is above the requested limit but below the estimated limit; 247 Cm and 249 Cf are above the requested limits. However, they are below the limits established; The reported detection limit for Norpar 13 is greater than the limit from the WAC; The reported detection limit for Isopar L is greater than the limit from WAC; Isopar L and Norpar 13 have limited solubility in aqueous solutions making it difficult to obtain consistent and reliable sub-samples; The values reported in this report are the concentrations in the sub-sample as detected by the instrument, however, the results may not accurately represent the concentrations of the analytes in Tank 50; The low insoluble solids content increases the measurement uncertainty for insoluble species.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Chemical Differences Between Sludge Solids at the F and H Area Tank Farms

The primary source of waste solids received into the F Area Tank Farm (FTF) was from PUREX processing performed to recover uranium and plutonium from irradiated depleted uranium targets. In contrast, two primary sources of waste solids were received into the H Area Tank Farm (HTF): a) waste from PUREX processing; and b) waste from H-modified (HM) processing performed to recover uranium and neptunium from burned enriched uranium fuel. Due to the differences between the irradiated depleted uranium targets and the burned enriched uranium fuel, the average compositions of the F and H Area wastes are markedly different from one another. Both F and H Area wastes contain significant amounts of iron and aluminum compounds. However, because the iron content of PUREX waste is higher than that of HM waste, and the aluminum content of PUREX waste is lower than that of HM waste, the iron to aluminum ratios of typical FTF waste solids are appreciably higher than those of typical HTF waste solids. Other constituents present at significantly higher concentrations in the typical FTF waste solids include uranium, nickel, ruthenium, zinc, silver, cobalt and copper. In contrast, constituents present at significantly higher concentrations in the typical HTF waste solids include mercury, thorium, oxalate, and radionuclides U-233, U-234, U-235, U-236, Pu-238, Pu-242, Cm-244, and Cm-245. Because of the higher concentrations of Pu-238 in HTF, the long-term concentrations of Th-230 and Ra-226 (from Pu-238 decay) will also be higher in HTF. The uranium and plutonium distributions of the average FTF waste were found to be consistent with depleted uranium and weapons grade plutonium, respectively (U-235 comprised 0.3 wt% of the FTF uranium, and Pu-240 comprised 6 wt% of the FTF plutonium). In contrast, at HTF, U-235 comprised 5 wt% of the uranium, and Pu-240 comprised 17 wt% of the plutonium, consistent with enriched uranium and high burn-up plutonium. X-ray diffraction analyses of various FTF and HTF samples indicated that the primary crystalline compounds of iron in sludge solids are Fe 2 O 3 , Fe 3 O 4 , and FeO(OH), and the primary crystalline compounds of aluminum are Al(OH) 3 and AlO(OH). Also identified were carbonate compounds of calcium, magnesium, and sodium; a nitrated sodium aluminosilicate; and various uranium compounds. Consistent with expectations, oxalate compounds were identified in solids associated with oxalic acid cleaning operations. The most likely oxidation states and chemical forms of technetium are assessed in the context of solubility, since technetium-99 is a key risk driver from an environmental fate and transport perspective. The primary oxidation state of technetium in SRS sludge solids is expected to be Tc(IV). In salt waste, the primary oxidation state is expected to be Tc(VII). The primary form of technetium in sludge is expected to be a hydrated technetium dioxide, TcO 2 ⋅ xH 2 O, which is relatively insoluble and likely co-precipitated with iron. In salt waste solutions, the primary form of technetium is expected to be the very soluble pertechnetate anion, TcO 4 - . The relative differences between the F and H Tank Farm waste provide a basis for anticipating differences that will occur as constituents of FTF and HTF waste residue enter the environment over the long-term future. If a constituent is significantly more dominant in one of the Tank Farms, its long-term environmental contribution will likely be commensurately higher, assuming the environmental transport conditions of the two Tank Farms share some commonality. It is in this vein that the information cited in this document is provided - for use during the generation, assessment, and validation of Performance Assessment modeling results.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Development of a Chemistry-Based, Predictive Method for Determining the Amount of Non-Pertechnetate Technetium in the Hanford Tanks (FY 2012 Progress Report)

This report describes investigations directed toward understanding the extent of the presence of highly alkaline soluble, non-pertechnetate technetium (n-Tc) in the Hanford Tank supernatants. The goals of this report are to: a) present a review of the available literature relevant to the speciation of technetium in the Hanford tank supernatants, b) attempt to establish a chemically logical correlation between available Hanford tank measurements and the presence of supernatant soluble n-Tc, c) use existing measurement data to estimate the amount of n-Tc in the Hanford tank supernatants, and d) report on any likely, process-friendly methods to eventually sequester soluble n-Tc from Hanford tank supernatants.

Hanford Tanks↗

Mixing Study for JT-71/72 Tanks

All modeling calculations for the mixing operations of miscible fluids contained in HB-Line tanks, JT-71/72, were performed by taking a three-dimensional Computational Fluid Dynamics (CFD) approach. The CFD modeling results were benchmarked against the literature results and the previous SRNL test results to validate the model. Final performance calculations were performed by using the validated model to quantify the mixing time for the HB-Line tanks. The mixing study results for the JT-71/72 tanks show that, for the cases modeled, the mixing time required for blending of the tank contents is no more than 35 minutes, which is well below 2.5 hours of recirculation pump operation. Therefore, the results demonstrate the adequacy of 2.5 hours’ mixing time of the tank contents by one recirculation pump to get well mixed.

42 ENGINEERING↗