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Preparation and initial characterization of fluidized bed steam reforming pure-phase standards

Description: Hanford is investigating the Fluidized Bed Steam Reforming (FBSR) process for their Low Activity Waste. The FBSR process offers a low-temperature continuous method by which liquid waste can be processed with the addition of clay into a sodium aluminosilicate (NAS) waste form. The NAS waste form is mainly comprised of nepheline (NaAlSiO{sub 4}), sodalite (Na{sub 8}[AlSiO{sub 4}]{sub 6}Cl{sub 2}), and nosean (Na{sub 8}[AlSiO{sub 4}]{sub 6}SO{sub 4}). Anions such as perrhenate (ReO{sub 4}{sup -}), pertechnetate (TcO{sub 4}{sup -}), and iodine (I{sup -}) are expected to replace sulfate in the nosean structure and/or chloride in the sodalite mineral structure (atomically bonded inside the aluminosilicate cages that these mineral structures possess). In the FBSR waste form, each of these phases can exist in a variety of solid solutions that differ from the idealized forms observed in single crystals in nature. The lack of understanding of the durability of these stoichiometric or idealized mineral phases complicates the ability to deconvolute the durability of the mixed phase FBSR product since it is a combination of different NAS phases. To better understand the behavior, fabrication and testing of the individual phases of the FBSR product is required. Analytical Development (AD) of the Science and Technology directorate of the Savannah River National Laboratory (SRNL) was requested to prepare the series of phase-pure standards, consisting of nepheline, nosean, and Cl, Re, and I sodalite. Once prepared, X-ray Diffraction (XRD) analyses were used to confirm the products were phase pure. These standards are being used for subsequent characterization studies consisting of the following: single-pass flow-through (SPFT) testing, development of thermodynamic data, and x-ray diffraction (XRD) calibration curves. In addition to the above mentioned phase-pure standards, AD was tasked with fabricating a mixed Tc-Re sodalite.
Date: March 21, 2013
Creator: Missimer, D. M. & Rutherford, R. L.
Partner: UNT Libraries Government Documents Department

REACTIONS OF SODIUM PEROXIDE WITH COMPONENTS OF LEGACY PLUTONIUM MATERIALS

Description: Plutonium oxide (PuO{sub 2}) calcined at >900 C resists dissolution in nitric acid (HNO{sub 3})-potassium fluoride (KF) solutions, a common method for their dissolution. The Savannah River National Laboratory (SRNL) has developed an alternate method for large samples of PuO{sub 2}-bearing materials using sodium peroxide (Na{sub 2}O{sub 2}) fusion as a pretreatment. The products of the reaction between Na{sub 2}O{sub 2} and PuO{sub 2} have been reported in the literature. As part of the SRNL development effort, additional data about the reaction between Na{sub 2}O{sub 2} and PuO{sub 2} were required. Also needed were data concerning the reaction of Na{sub 2}O{sub 2} with other components that may be present in the feed materials. Sodium peroxide was reacted with aluminum metal (Al), beryllium metal (Be), graphite, potassium chloride (KCl), magnesium chloride (MgCl{sub 2}), and calcium chloride (CaCl{sub 2}). The paper reports and discusses the reaction products of these and related compounds with Na{sub 2}O{sub 2}.
Date: October 4, 2011
Creator: Pierce, R.; Missimer, D. & Crowder, M.
Partner: UNT Libraries Government Documents Department

THE HIGH TEMPERATURE CHEMICAL REACTIVITY OF LI2O

Description: The ultimate purpose of this study was to investigate the use of a Li-Ca mixture for direct reduction of actinide oxides to actinide metals at temperatures below 1500 C. For such a process to be successful, the products of the reduction reaction, actinide metals, Li{sub 2}O, and CaO, must all be liquid at the reaction temperature so the resulting actinide metal can coalesce and be recovered as a monolith. Since the established melting temperature of Li{sub 2}O is in the range 1427-1700 C and the melting temperature of CaO is 2654 C, the Li{sub 2}O-CaO (lithium oxidecalcium oxide) pseudo-binary system was investigated in an attempt to identify the presence of low-melting eutectic compositions. The results of our investigation indicate that there is no evidence of ternary Li-Ca-O phases or solutions melting below 1200 C. In the 1200-1500 C range utilizing MgO crucibles, there is some evidence for the formation of a ternary phase; however, it was not possible to determine the phase composition. The results of experiments performed with ZrO{sub 2} crucibles in the same temperature range did not show the formation of the possible ternary phase seen in the earlier experiment involving MgO crucibles, so it was not possible to confirm the possibility that a ternary Li-Ca-O or Li-Mg-O phase was formed. It appears that the Li{sub 2}O-CaO materials reacted, to some extent, with all of the container materials, alumina (Al{sub 2}O{sub 3}), magnesia (MgO), zirconia (ZrO{sub 2}), and 95% Pt-5% Au; however, to clarify the situation additional experiments are required. In addition to the primary purpose of this study, the results of this investigation led to the conclusions that: (1) The melting temperature of Li{sub 2}O may be as low as 1250 C, which is considerably lower than the previously published values in the range 1427-1700 C; (2) ...
Date: November 13, 2009
Creator: Kessinger, G. & Missimer, D.
Partner: UNT Libraries Government Documents Department

CHARACTERIZATION OF MODIFIED MONOSODIUM TITANATE - AN IMPROVED SORBENT FOR STRONTIUM AND ACTINIDE SEPARATIONS

Description: High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 134,137}Cs, {sup 90}Sr, and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. An inorganic sorbent, monosodium titanate (MST), is currently used to remove {sup 90}Sr and alpha-emitting radionuclides, while a caustic-side solvent extraction process is used for removing {sup 134,137}Cs. A new peroxotitanate material, modified MST, or mMST, has recently been developed and has shown increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the current baseline material, MST. This paper describes recent results focused on further characterization of this material.
Date: December 21, 2010
Creator: Hobbs, D.; Taylor-Pashow, K. & Missimer, D.
Partner: UNT Libraries Government Documents Department

RADIOACTIVE DEMONSTRATION OF FINAL MINERALIZED WASTE FORMS FOR HANFORD WASTE TREATMENT PLANT SECONDARY WASTE BY FLUIDIZED BED STEAM REFORMING USING THE BENCH SCALE REFORMER PLATFORM

Description: The U.S. Department of Energy's Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford's tank waste. Currently there are approximately 56 million gallons of highly radioactive mixed wastes awaiting treatment. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Therefore, Supplemental Treatment is required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. In addition, the WTP LAW vitrification facility off-gas condensate known as WTP Secondary Waste (WTP-SW) will be generated and enriched in volatile components such as {sup 137}Cs, {sup 129}I, {sup 99}Tc, Cl, F, and SO{sub 4} that volatilize at the vitrification temperature of 1150 C in the absence of a continuous cold cap (that could minimize volatilization). The current waste disposal path for the WTP-SW is to process it through the Effluent Treatment Facility (ETF). Fluidized Bed Steam Reforming (FBSR) is being considered for immobilization of the ETF concentrate that would be generated by processing the WTP-SW. The focus of this current report is the WTP-SW. FBSR offers a moderate temperature (700-750 C) continuous method by which WTP-SW wastes can be processed irrespective of whether they contain organics, nitrates, sulfates/sulfides, chlorides, fluorides, volatile radionuclides or other aqueous components. The FBSR technology can process these wastes into a crystalline ceramic (mineral) waste form. ...
Date: February 2, 2012
Creator: Crawford, C.; Burket, P.; Cozzi, A.; Daniel, W.; Jantzen, C. & Missimer, D.
Partner: UNT Libraries Government Documents Department

X-RAY FLUORESCENCE ANALYSIS OF HANFORD LOW ACTIVITY WASTE SIMULANTS

Description: Savannah River National Laboratory (SRNL) was requested to develop an x-ray fluorescence (XRF) spectrometry method for elemental characterization of the Hanford Tank Waste Treatment and Immobilization Plant (WTP) pretreated low activity waste (LAW) stream to the LAW Vitrification Plant. The WTP is evaluating the potential for using XRF as a rapid turnaround technique to support LAW product compliance and glass former batching. The overall objective of this task was to develop XRF analytical methods that provide the rapid turnaround time (<8 hours) requested by the WTP, while providing sufficient accuracy and precision to determine waste composition variations. For Phase 1a, SRNL (1) evaluated, selected, and procured an XRF instrument for WTP installation, (2) investigated three XRF sample methods for preparing the LAW sub-sample for XRF analysis, and (3) initiated scoping studies on AN-105 (Envelope A) simulant to determine the instrument's capability, limitations, and optimum operating parameters. After preliminary method development on simulants and the completion of Phase 1a activities, SRNL received approval from WTP to begin Phase 1b activities with the objective of optimizing the XRF methodology. Three XRF sample methods used for preparing the LAW sub-sample for XRF analysis were studied: direct liquid analysis, dried spot, and fused glass. The direct liquid method was selected because its major advantage is that the LAW can be analyzed directly without any sample alteration that could bias the method accuracy. It also is the fastest preparation technique--a typical XRF measurement could be completed in < 1hr after sample delivery. Except for sodium, the method detection limits (MDLs) for the most important analytes in solution, the hold point elements, were achieved by this method. The XRF detection limits are generally adequate for glass former batching and product composition reporting, but may be inadequate for some species (Hg, Cd, and Ba) important to land ...
Date: May 8, 2006
Creator: Jurgensen, A; David Missimer, D & Ronny Rutherford, R
Partner: UNT Libraries Government Documents Department

X-RAY FLUORESCENCE ANALYSIS OF HANFORD LOW ACTIVITY WASTE SIMULANTS METHOD DEVELOPMENT

Description: The x-ray fluorescence laboratory (XRF) in the Analytical Development Directorate (ADD) of the Savannah River National Laboratory (SRNL) was requested to develop an x-ray fluorescence spectrometry method for elemental characterization of the Hanford Tank Waste Treatment and Immobilization Plant (WTP) pretreated low activity waste (LAW) stream to the LAW Vitrification Plant. The WTP is evaluating the potential for using XRF as a rapid turnaround technique to support LAW product compliance and glass former batching. The overall objective of this task was to develop an XRF analytical method that provides rapid turnaround time (<8 hours), while providing sufficient accuracy and precision to determine variations in waste.
Date: August 8, 2007
Creator: Jurgensen, A; David Missimer, D & Ronny Rutherford, R
Partner: UNT Libraries Government Documents Department

MATERIAL PROPERTIES OF PLUTONIUM-BEARING OXIDES STORED IN STAINLESS STEEL CONTAINERS

Description: The destructive examination (DE) of 3013 containers after storage is part of the Surveillance and Monitoring Program based on the Department of Energy's standard for long-term storage of Pu (DOE-STD-3013). The stored, Pu-bearing materials may contain alkali halide contamination that varies from trace amounts of salt to about 50 weight percent, with smaller fractions of other compounds and oxides. These materials were characterized prior to packaging, and surveillance characterizations are conducted to determine the behavior of the materials during long term storage. The surveillance characterization results are generally in agreement with the pre-surveillance data. The predominant phases identified by X-ray diffraction are in agreement with the expected phase assemblages of the as-received materials. The measured densities are in reasonable agreement with the expected densities of materials containing the fraction of salts and actinide oxide specified by the pre-surveillance data. The radiochemical results are generally in good agreement with the pre-surveillance data for mixtures containing 'weapons grade' Pu (nominally 94% {sup 239}Pu and 6% {sup 240}Pu); however, the ICP-MS results from the present investigation generally produce lower concentrations of Pu than the pre-surveillance analyses. For mixtures containing 'fuel grade' Pu (nominally 81-93% {sup 239}Pu and 7-19% {sup 240}Pu), the ICP-MS results from the present investigation appear to be in better agreement with the pre-surveillance data than the radiochemistry results.
Date: February 1, 2010
Creator: Kessinger, G.; Almond, P.; Bridges, N.; Bronikowski, M.; Crowder, M.; Duffey, J. et al.
Partner: UNT Libraries Government Documents Department

Radioactive Demonstration Of Mineralized Waste Forms Made From Hanford Low Activity Waste (Tank Farm Blend) By Fluidized Bed Steam Reformation (FBSR)

Description: The U.S. Department of Energy’s Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford’s tank waste. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Hanford Tank Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Supplemental Treatment is likely to be required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. The Supplemental Treatment chosen will immobilize that portion of the retrieved LAW that is not sent to the WTP’s LAW Vitrification facility into a solidified waste form. The solidified waste will then be disposed on the Hanford site in the Integrated Disposal Facility (IDF). Fluidized Bed Steam Reforming (FBSR) offers a moderate temperature (700-750°C) continuous method by which LAW can be processed irrespective of whether the waste contain organics, nitrates, sulfates/sulfides, chlorides, fluorides, volatile radionuclides or other aqueous components. The FBSR technology can process these wastes into a crystalline ceramic (mineral) waste form. The mineral waste form that is produced by co-processing waste with kaolin clay in an FBSR process has been shown to be comparable to LAW glass, i.e. leaches Tc-99, Re and Na at <2g/m2 during ASTM C1285 (Product Consistency) durability testing. Monolithing of the granular FBSR product was investigated to prevent dispersion during transport or burial/storage. Monolithing in an inorganic geopolymer binder, which is amorphous, macro-encapsulates the granules, and ...
Date: August 21, 2013
Creator: Jantzen, C. M.; Crawford, C. L.; Bannochie, C. J.; Burket, P. R.; Cozzi, A. D.; Daniel, W. E. et al.
Partner: UNT Libraries Government Documents Department

Radioactive Demonstration Of Mineralized Waste Forms Made From Hanford Low Activity Waste (Tank SX-105, Tank AN-103, And AZ-101/102) By Fluidized Bed Steam Reformation (FBSR)

Description: Fluidized Bed Steam Reforming (FBSR) is a robust technology for the immobilization of a wide variety of radioactive wastes. Applications have been tested at the pilot scale for the high sodium, sulfate, halide, organic and nitrate wastes at the Hanford site, the Idaho National Laboratory (INL), and the Savannah River Site (SRS). Due to the moderate processing temperatures, halides, sulfates, and technetium are retained in mineral phases of the feldspathoid family (nepheline, sodalite, nosean, carnegieite, etc). The feldspathoid minerals bind the contaminants such as Tc-99 in cage (sodalite, nosean) or ring (nepheline) structures to surrounding aluminosilicate tetrahedra in the feldspathoid structures. The granular FBSR mineral waste form that is produced has a comparable durability to LAW glass based on the short term PCT testing in this study, the INL studies, SPFT and PUF testing from previous studies as given in the columns in Table 1-3 that represent the various durability tests. Monolithing of the granular product was shown to be feasible in a separate study. Macro-encapsulating the granular product provides a decrease in leaching compared to the FBSR granular product when the geopolymer is correctly formulated.
Date: September 18, 2013
Creator: Jantzen, C. M.; Crawford, C. L.; Bannochie, C. J.; Burket, P. R.; Cozzi, A. D.; Daniel, W. E. et al.
Partner: UNT Libraries Government Documents Department