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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

SU-E-I-21: Deformation Mapping and Shape Prediction with 3D Tumor Volume Morphing

Purpose: To compare projection-based versus global correction that compensate for deadtime count loss in SPECT/CT images. Methods: SPECT/CT images of an IEC phantom (2.3GBq 99mTc) with ∼10% deadtime loss containing the 37mm (uptake 3), 28 and 22mm (uptake 6) spheres were acquired using a 2 detector SPECT/CT system with 64 projections/detector and 15 s/projection. The deadtime, Ti and the true count rate, Ni at each projection, i was calculated using the monitor-source method. Deadtime corrected SPECT were reconstructed twice: (1) with projections that were individually-corrected for deadtime-losses; and (2) with original projections with losses and then correcting the reconstructed SPECT images using a scaling factor equal to the inverse of the average fractional loss for 5 projections/detector. For both cases, the SPECT images were reconstructed using OSEM with attenuation and scatter corrections. The two SPECT datasets were assessed by comparing line profiles in xyplane and z-axis, evaluating the count recoveries, and comparing ROI statistics. Higher deadtime losses (up to 50%) were also simulated to the individually corrected projections by multiplying each projection i by exp(-a*Ni*Ti), where a is a scalar. Additionally, deadtime corrections in phantoms with different geometries and deadtime losses were also explored. The same two correction methods were carried for all these data sets. Results: Averaging the deadtime losses in 5 projections/detector suffices to recover >99% of the loss counts in most clinical cases. The line profiles (xyplane and z-axis) and the statistics in the ROIs drawn in the SPECT images corrected using both methods showed agreement within the statistical noise. The count-loss recoveries in the two methods also agree within >99%. Conclusion: The projection-based and the global correction yield visually indistinguishable SPECT images. The global correction based on sparse sampling of projections losses allows for accurate SPECT deadtime loss correction while keeping the study duration reasonable.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2016

New Formulation of Cast Stone for {sup 99}Tc Immobilization in Sulfate Rich Secondary Waste Stream - 16098

A low-temperature, cementitious waste form called Cast Stone (or grout) has been selected for solidification of the Effluent Treatment Facility (ETF)-treated wastes at the Hanford Site. Because the waste stream to be solidified may be relatively high in sulfate, the current Cast Stone dry blend formulation with ordinary Portland cement (OPC), fly ash (FA), and blast furnace slag (BFS) (47% BFS, 45% FA, and 8% OPC) may not be adequate. Thus a new formulation, called secondary waste grout, was proposed and tested. The secondary waste grout uses hydrated lime [Ca(OH){sub 2}] to tie up the sulfate initially such that ettringite [Ca{sub 6}Al{sub 2}(SO{sub 4}){sub 3}(OH){sub 12}.26(H{sub 2}O)] forms rapidly instead of forming as the cementitious waste form cures. Three different liquid waste simulants (242-A evaporator, Environmental Restoration Disposal Facility [ERDF] leachates, and Hanford Tank Waste Treatment and Immobilization Plant [WTP] off-gas condensates) were prepared and solidified using this new dry blend formulation. Baseline grout dry mixes were 20 wt% hydrated lime (HL), 35 wt% OPC, and 45 wt% BFS, and two different water-to-dry mix (w/dm) ratios (0.5 and 0.6) of free water mass to mass of dry blend were tested. After curing for a minimum of 28 days, the grout solidified waste forms were characterized and used for Tc leachability testing using the EPA 1315 Method. X-ray diffraction analysis confirmed that ∼12-15% of ettringite was formed in early stage of 28-day curing for the grouts prepared with the high sulfate WTP simulant and HL addition. In addition, the new formulation of secondary waste grout prepared with HL (20%), OPC (35%), and BFS (45%) at either 0.5 or 0.6 water to dry mix ratio yields higher average Tc interval leachability index (LI) values (12.5 to 13.9) after 28 to 90 days of leaching using deionized water, which is higher than the desired {sup 99}Tc LI value of 12 for grout destined for burial in the Integrated Disposal Facility at the Hanford Site. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

SU-E-I-20: Dead Time Count Loss Compensation in SPECT/CT: Projection Versus Global Correction

Purpose: To compare projection-based versus global correction that compensate for deadtime count loss in SPECT/CT images. Methods: SPECT/CT images of an IEC phantom (2.3GBq 99mTc) with ∼10% deadtime loss containing the 37mm (uptake 3), 28 and 22mm (uptake 6) spheres were acquired using a 2 detector SPECT/CT system with 64 projections/detector and 15 s/projection. The deadtime, Ti and the true count rate, Ni at each projection, i was calculated using the monitor-source method. Deadtime corrected SPECT were reconstructed twice: (1) with projections that were individually-corrected for deadtime-losses; and (2) with original projections with losses and then correcting the reconstructed SPECT images using a scaling factor equal to the inverse of the average fractional loss for 5 projections/detector. For both cases, the SPECT images were reconstructed using OSEM with attenuation and scatter corrections. The two SPECT datasets were assessed by comparing line profiles in xyplane and z-axis, evaluating the count recoveries, and comparing ROI statistics. Higher deadtime losses (up to 50%) were also simulated to the individually corrected projections by multiplying each projection i by exp(-a*Ni*Ti), where a is a scalar. Additionally, deadtime corrections in phantoms with different geometries and deadtime losses were also explored. The same two correction methods were carried for all these data sets. Results: Averaging the deadtime losses in 5 projections/detector suffices to recover >99% of the loss counts in most clinical cases. The line profiles (xyplane and z-axis) and the statistics in the ROIs drawn in the SPECT images corrected using both methods showed agreement within the statistical noise. The count-loss recoveries in the two methods also agree within >99%. Conclusion: The projection-based and the global correction yield visually indistinguishable SPECT images. The global correction based on sparse sampling of projections losses allows for accurate SPECT deadtime loss correction while keeping the study duration reasonable.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2012

Evolution of fast reactor core spectra in changing a heavy liquid metal coolant by molten PB-208

In the paper neutron spectra of fast reactor cooled with lead-bismuth or lead-208 are given. It is shown that in changing the coolant from lead-bismuth to lead-208 the core neutron spectra of the fast reactor FR RBEC-M are hardening in whole by several percents when a little share of low energy neutrons (5 eV - 50 keV) is slightly increasing. The shift of spectra to higher energies permits to enhance the fuel fission while the increased share of low energy neutrons provides more effective conversion of uranium-238 into plutonium due to peculiarity of {sup 238}U neutron capture cross section. Good neutron and physical features of molten {sup 208}Pb permit to assume it as perspective coolant for fast reactors and accelerator driven systems. The one-group cross sections of neutron radiation capture, {sigma}(n,g), by {sup 208}Pb, {sup 238}U, {sup 99}Tc, mix of lead and bismuth, {sup nat}Pb-Bi, averaged over neutron spectra of the fast reactor RBEC-M are given. It is shown that one-group cross sections of neutron capture by material of the liquid metal coolant consisted from lead enriched with the stable lead isotope, {sup 208}Pb, are by 4-7 times smaller {sigma}(n,g) for the coolant {sup nat}Pb-Bi. The economy of neutrons in the core cooled with {sup 208}Pb can be used for reducing reactor's initial fuel load, increasing fuel breeding and transmutation of long lived fission products, for example {sup 99}Tc. Good neutron and physical features of lead enriched with {sup 208}Pb permit to consider it as a perspective low neutron absorbing coolant for fast reactors and accelerator driven systems. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2017

Analysis of Past Leaks from Waste Management Area C, Hanford, Washington - 17525

Waste Management Area C (WMA C) at the Hanford Site was actively used for several decades for storing radioactive waste in tanks, and therefore is alternatively termed a 'waste management area,' or a 'tank farm.' During its operational life, a number of documented leaks occurred within or near to the WMA. The largest ones were associated with leaks in pipelines and diversion boxes, with the inlets or outlets of the tanks, or with leaks from the tanks themselves. Contaminants associated with these leaks were released to the soil, and mobile {sup 99}Tc has reached the groundwater exceeding drinking water standards. An analysis of the impact of past leaks on groundwater resources has been undertaken as part of the overall process of closing the tank farm. The analysis of leaks was carried out using a suite of scoping cases to evaluate alternative conceptual models for the leak behavior to identify those that are in reasonable agreement with observed concentrations of {sup 99}Tc in groundwater. Comparisons of the scoping cases with available {sup 99}Tc observations indicate the following. - Several of the scoping cases produced results that are inconsistent with observations, indicating that the assumptions in those cases may not be representative of conditions in WMA C. These negative results are valuable in improving the understanding of the migration of {sup 99}Tc from WMA C. - The remaining scoping analyses produced comparable results to each other, and none were obviously superior to others in terms of explaining the {sup 99}Tc observations. When uncertainties in groundwater fluxes were taken into account, these scoping analyses were capable of producing both arrival times and concentrations consistent with observed data for {sup 99}Tc. A representative model was used to implement a forward projection of a suite of contaminants of concern to show how the contamination associated with past leaks can be expected to evolve in the future. This paper presents these results and discusses their implications on groundwater contamination at WMA C. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Analysis of isomeric ratios for medium-mass nuclei

Values of the isomeric ratios for product nuclei originating from simple charge-exchange reactions were analyzed. The cross sections for the formation of product nuclei in ground and isomeric states were calculated with the aid of the TALYS 1.4 and EMPIRE 3.2 codes. The calculated values of the isomeric ratios were compared with their experimental counterparts taken from the EXFOR database. For the {sup 86,87}Y, {sup 94,95,96,99}Tc, and {sup 44}Sc nuclei, the experimental values of the isomeric ratios exceed the respective calculated values. The nuclei in question feature weak deformations and have high-spin yrast lines and rotational bands. The possible reason behind the discrepancy between theoretical and experimental isomeric ratios is that the decay of yrast states leads with a high probability to the formation of isomeric states of detected product nuclei.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2013

Role of fast reactor and its cycle to reduce nuclear waste burden

The role of the metal fuel fast reactor with recycling of actinides and the five long-lived fission products based on the concept of the Self-Consistent Nuclear Energy System has been examined by evaluating the reduction of nuclear wastes during the transition period to this reactor system. The evaluation was done in comparison to an LWR once-through case and a conventional actinide recycling oxide fast reactor. As a result, it is quantitatively clarified that a metal fuel fast reactor with actinide and the five long-lived fission products (I{sup 129}, Tc{sup 99}, Zr{sup 93}, Cs{sup 135} and Sn{sup 126}) recycling could play a significant role in reducing the nuclear waste burden including the current LWR wastes. This can be achieved by using a fast neutron spectrum reactor enhanced with metal fuel that brings high capability as a 'waste burner'. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Integrated program for department of energy environmental management office of soil and groundwater remediation - 15426

The subsurface problems that remain at the U.S. Department of Energy (DOE) Office of Environmental Management (EM) sites are technically complex and the costs to complete the cleanup mission are expected to range from $17 billion to $21 billion. There is growing recognition that conventional remedies will not meet regulatory goals at a number of sites and alternative approaches will be required. To address the challenge, the EM Office of Soil and Groundwater Remediation created an integrated program to develop innovative scientific and technical in conjunction with engagement of stakeholders, regulators, and the public. The integrated program provides a holistic approach to assess the risk associated with the remaining challenges facing EM and develop solutions that achieve remediation goals and protect human health and the environment. The integrated program uses a systems-based framework for achieving environmental remediation goals. The framework is based on developing and updating a site conceptual model and includes steps to 1) provide the technical basis for remedial actions, 2) assessments of potential remedies, and 3) implementation and management of remedies to achieve site restoration goals. The Office of Soil and Groundwater remediation defines research and development needed to successfully define and apply the framework. Research opportunities and targets are identified in characterization and conceptual model development, predictions of site conditions, remediation, monitoring, and remediation decision support. Characterization and quantification of key subsurface uncertainties is needed to support conceptual model development, identify contaminant source zones, quantify the flux of contaminants from source terms to points of compliance, and characterize controlling processes for remediation approaches including natural attenuation. Predictive analyses are needed to support development of remediation endpoints, select and design active and in situ or passive remedies, assess remedy performance, and predict long-term contaminant behavior for design of monitoring systems. Advancements are needed to support adaptive remediation approaches and to develop long-term contaminant management strategies for complex sites, such as effective in situ treatment methods for long-lived contaminants ({sup 99}Tc, {sup 129}I, U, Hg, etc.). Monitoring tools and approaches are needed to evaluate remedy performance and plume behavior and decision support methods are needed to quantitatively evaluate remediation alternatives. The Office of Soil and Groundwater Remediation leverages scientific understanding provided through partnerships with the DOE Office of Science, the Department of Defense, and Environmental Protection Agency. These partnerships are helping EM develop scientific understanding and technologies for implementing the assessment framework. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Sorption and Transport Behavior of {sup 137}Cs, {sup 90}Sr, and {sup 99}Tc on Geological Media in Radioactive Waste Repository, South Korea - 16112

Sorption experiments and a behavior investigation for the radionuclides {sup 137}Cs, {sup 90}Sr, and {sup 99}Tc were conducted using groundwater and solid materials (mud-stone and sandstone) sampled from the Wolsong low- and intermediate-level radioactive waste repository at Gyeongju, Korea. After experiments involving batch sorption, diffusion, and a flow-through column, distribution coefficients (K{sub d}) of the radionuclides were obtained, and sorption properties for each radionuclide were analyzed. Increasing K{sub d} values were observed in the sequence {sup 137}Cs, {sup 90}Sr, and {sup 99}Tc regardless of the geological media tested. For all sorbing radionuclides, K{sub d} values for the mud-stone were observed to be higher than those for sandstone regardless of the groundwater. These higher K{sub d} values are the result of higher levels of total organic carbon in the mud-stone than were present in the sandstone. In addition, the chlorite, kaolinite, and montmorillonite contents in the mud-stone also were higher than in the sandstone. The mineralogical composition of the solid materials was observed to be important in the sorption of sorbing radionuclides. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Sorption of Anionic Iodine and Molybdenum to Multi-sorbing Barrier (MSB) Materials - 20030

A multi-sorbing barrier (MSB) material containing sodium bentonite (NaB), organoclay, and anion resin is being evaluated for containment of anionic radionuclides. Batch tests on the MSB were conducted using two non-radioactive analog isotopes ({sup 127}I, {sup 95}Mo) as surrogates for {sup 129}I and {sup 99}Tc due to their similar valence and molecular weight relative to the radionuclides. Tests were conducted on the organoclay, anion resin, and NaB individually and on NaB-resin blends with resin contents of 1% and 5% by mass. The anion resin exhibits very strong sorption of {sup 127}I and {sup 95}Mo relative to the other materials. The organoclay exhibited modest sorption of {sup 95}Mo and {sup 127}I, and NaB little sorption. The sorption isotherms follow a linear model for NaB, a Freundlich model for the organoclay, and a Langmuir model for the anion resin and NaB-resin mixtures. Combining resin with NaB significantly enhances sorption relative to NaB alone, with a larger resin fraction yielding greater sorption. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Using Rose’s metal alloy as a pinhole collimator material in preclinical small-animal imaging: A Monte Carlo evaluation

Purpose: Pinhole collimation is the most common method of high-resolution preclinical single photon emission computed tomography imaging. The collimators are usually constructed from dense materials with high atomic numbers, such as gold and platinum, which are expensive and not always flexible in the fabrication step. In this work, the authors have investigated the properties of a fusible alloy called Rose’s metal and its potential in pinhole preclinical imaging. When compared to current standard pinhole materials such as gold and platinum, Rose’s metal has a lower density and a relatively low effective atomic number. However, it is inexpensive, has a low melting point, and does not contract when solidifying. Once cast, the piece can be machined with high precision. The aim of this study was to evaluate the imaging properties for Rose’s metal and compare them with those of standard materials. Methods: After validating their Monte Carlo code by comparing its results with published data and the results from analytical calculations, they investigated different pinhole geometries by varying the collimator material, acceptance angle, aperture diameter, and photon incident angle. The penetration-to-scatter and penetration-to-total component ratios, sensitivity, and the spatial resolution were determined for gold, tungsten, and Rose’s metal for two radionuclides, {sup 99}Tc{sup m} and {sup 125}I. Results: The Rose’s metal pinhole-imaging simulations show higher penetration/total and scatter/total ratios. For example, the penetration/total is 50% for gold and 75% for Rose’s metal when simulating {sup 99}Tc{sup m} with a 0.3 mm aperture diameter and a 60° acceptance angle. However, the degradation in spatial resolution remained below 10% relative to the spatial resolution for gold for acceptance angles below 40° and aperture diameters larger than 0.5 mm. Conclusions: Extra penetration and scatter associated with Rose’s metal contribute to degradation in the spatial resolution, but this degradation is not always substantial. The most important factor besides the collimator material was the acceptance angle. This should be kept to a minimum to prevent unnecessary scatter and penetration. For {sup 125}I, the difference in spatial resolution between gold and Rose’s metal is very small, 2.2% in the worst-case scenario. Based on these results, the authors conclude that Rose’s metal is an alternative to standard materials not only for low-energy photon imaging but also for medium-energy applications that require low-cost, flexible pinhole configurations and designs, and that can tolerate a degraded spatial resolution.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2016

Role of (n,2n) reactions in transmutation of long-lived fission products

The conditions under which (n,γ) and (n,2n) reactions can help or hinder each other in neutron transmutation of long-lived fission products (LLFPs) are considered. Isotopic and elemental transmutation for the main long-lived fission products, {sup 79}Se, {sup 93}Zr, {sup 99}Tc, {sup 107}Pd, {sup 126}Sn, {sup 129}I, and {sup 135}Cs, are considered. The effect of (n,2n) reactions on the equilibrium amount of nuclei of the transmuted isotope and the neutron consumption required for the isotope processing is estimated. The aim of the study is to estimate the influence of (n,2n) reactions on efficiency of neutron LLFP transmutation. The code TIME26 and the libraries of evaluated nuclear data ABBN-93, JEF-PC, and JANIS system are applied. The following results are obtained: (1) The effect of (n,2n) reactions on the minimum number of neutrons required for transmutation and the equilibrium amount of LLFP nuclei is estimated. (2) It is demonstrated that, for three LLFP isotopes ({sup 126}Sn, {sup 129}I, and {sup 135}Cs), (n,γ) and (n,2n) reactions are partners facilitating neutron transmutation. The strongest effect of (n,2n) reaction is found for {sup 126}Sn transmutation (reduction of the neutron consumption by 49% and the equilibrium amount of nuclei by 19%).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2017

Precipitation of Epsilon Particles in Metal Doped Ceria Irradiated with Energetic Ions

Metallic particles precipitated from fission products in oxide fuel matrix (e.g., UO{sub 2}) have a great impact on the thermal and mechanical properties of the fuel. A burn-up of 40 MWd/kg U results in the conversion of 4% of the uranium to approximately 3% fission products and 1% transuranium elements. Epsilon phase is the major metallic phase of the precipitates with a hexagonal-closed packed (HCP) crystal structure. It can exist in a variety of metallic forms in UO{sub 2}, but typically, it consists of five metals: Mo, Pd, Rh, Ru and Tc. Epsilon particles can form over a wide range of stoichiometries in the five metal system. Simulated compositions with Re as a surrogate for Tc have been investigated as a waste form for {sup 99}Tc, an isotope with a long half-life of 2.13 10{sup 5} years and a high solubility under oxidizing conditions in addition to Mo in the corrosion process. There is a pressing need to understand the factors influencing the formation and growth of the metallic phase in fuel. Efforts are currently underway to perform careful neutron irradiation of nuclear fuel under controlled conditions in a test reactor, recover metallic phases that may be present, and characterize the resulting structure and chemistry. Due to the long duration, high cost and radiological concerns associated with neutron irradiation and sample characterizations, ion irradiation studies of a surrogate material with a full control of the processing parameters can emulate different stages of the particle precipitation, which can add a tremendous value to reactor-based studies. This presentation reports our recent ion irradiation results on the metallic particle precipitation under various irradiation and thermal annealing conditions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

Technetium Immobilization Forms Literature Survey

Of the many radionuclides and contaminants in the tank wastes stored at the Hanford site, technetium-99 ( 99 Tc) is one of the most challenging to effectively immobilize in a waste form for ultimate disposal. Within the Hanford Tank Waste Treatment and Immobilization Plant (WTP), the Tc will partition between both the high-level waste (HLW) and low-activity waste (LAW) fractions of the tank waste. The HLW fraction will be converted to a glass waste form in the HLW vitrification facility and the LAW fraction will be converted to another glass waste form in the LAW vitrification facility. In both vitrification facilities, the Tc is incorporated into the glass waste form but a significant fraction of the Tc volatilizes at the high glass-melting temperatures and is captured in the off-gas treatment systems at both facilities. The aqueous off-gas condensate solution containing the volatilized Tc is recycled and is added to the LAW glass melter feed. This recycle process is effective in increasing the loading of Tc in the LAW glass but it also disproportionally increases the sulfur and halides in the LAW melter feed which increases both the amount of LAW glass and either the duration of the LAW vitrification mission or the required supplemental LAW treatment capacity.

technetium↗
DOE OSTI2016

Radiopharmaceuticals for SPECT cancer detection

The purpose of the study was to assess the efficacy of single photon emission computed tomography (SPECT) with {sup 199}Tl and {sup 99}mTc-MIBI in the detection of breast, laryngeal and hypopharyngeal cancers. A total of 220 patients were included into the study: 120 patients with breast lesions (100 patients with breast cancer and 20 patients with benign breast tumors) and 100 patients with laryngeal/hypopharyngeal diseases (80 patients with laryngeal/hypopharyngeal cancer and 20 patients with benign laryngeal/hypopharyngeal lesions). No abnormal {sup 199}Tl uptake was seen in all patients with benign breast and laryngeal lesions, indicating a 100% specificity of {sup 199}Tl SPECT. In the breast cancer patients, the increased {sup 199}Tl uptake in the breast was visualized in 94.8% patients, {sup 99m}Tc-MIBI—in 93.4% patients. The increased {sup 199}Tl uptake in axillary lymph nodes was detected in 60% patients, and {sup 99m}Tc-MIBI—in 93.1% patients. In patients with laryngeal/hypopharyngeal cancer, the sensitivity of SPECT with {sup 199}Tl and {sup 99m}Tc-MIBI was 95%. The {sup 199}Tl SPECT sensitivity in identification of regional lymph node metastases in the patients with laryngeal/hypopharyngeal cancer was 75% and the {sup 99m}Tc-MIBI SPECT sensitivity was 17%. The data obtained showed that SPECT with {sup 199}Tl and {sup 99m}Tc-MIBI can be used as one of the additional imaging methods in detection of tumors.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2020

The Nature and State of Groundwater Contamination at the Nevada National Security Site: What Have We Learned from Decades of Groundwater Analysis? - 20337

The regulatory framework for remediating radionuclide contamination from underground nuclear testing at the Nevada National Security Site (NNSS) is based on a combination of characterization and modeling studies, monitoring, and institutional controls [1]. Currently, tritium is the largest contributor (∼90%) to the estimated 44.6 million-curie radionuclide inventory resulting from underground testing [2]. Because of its short half-life (12.32 years), its relative contribution reduces below 10% of the total radiologic inventory over the next 120 years as a result of radioactive decay. Although tritium levels are observed well above the Safe Drinking Water Act (SDWA) maximum contaminant levels (MCLs) in groundwater, other radionuclides are well below their MCLs except within the nuclear test near-field (nuclear test cavity and chimney) environment. In fact, most device-derived radionuclides are below their MCL in groundwater even in samples collected from this near-field environment. The distribution of radionuclides following the nuclear detonation greatly influences the availability of potential contaminants for groundwater transport. Tritium is initially distributed in the gas phase, later as tritiated water in steam, and finally as liquid water, and is available to groundwater transport away from the near-field environment. Other radionuclides that are mobile in groundwater are {sup 14}C, {sup 36}Cl, {sup 99}Tc, and {sup 129}I though their radiologic inventory is small when compared to tritium. Many radionuclides (e.g. U, Pu, Am) are incorporated to a significant extent into the melt glass at the bottom of the cavity and are accessible to groundwater primarily through the slow process of glass dissolution. These radionuclides are also adsorbed to the surfaces of the crushed rock within the cavity and chimney which limits their migration in groundwater. Although colloid facilitated transport of radionuclides at the NNSS has been observed [3], radionuclide concentrations decrease with time and migration distances due to desorption and colloid filtration processes. Current studies indicate that radionuclides associated with colloids are unlikely to migrate downgradient from NNSS underground nuclear tests at concentrations above the SDWA MCL [4][5]. The results of over 50 years of sampling, along with an understanding of these post detonation processes, indicate that tritium is the only contaminant of concern downgradient of testing and that even tritium will not exceed its MCL in groundwater after ∼120 years. Although other longer-lived radionuclides may continue to be released slowly from the near-field environment they will likely never reach levels exceeding their MCLs in groundwater downgradient of the NNSS. Groundwater monitoring will continue to verify these observations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Performance Assessment for the Waste Management Area C at the Hanford Site in Southeast Washington - 17515

An initial performance assessment (PA) of Single-Shell Tank (SST) Waste Management Area C (WMA C) located at the U.S. Department of Energy's (DOE) Hanford Site in southeastern Washington has been completed to satisfy the requirements of the Hanford Federal Facility Agreement and Consent Order (HFFACO), as well as other Federal requirements and State-approved closure plans and permits. The WMA C PA assesses the fate, transport, and impacts of radionuclides within residual wastes left in tanks and ancillary equipment and facilities in their assumed closed configuration, and the subsequent risks to humans into the far future. This PA focused on radiological impacts has been developed to meet the requirements for a closure authorization under DOE O 435.1 that includes a waste incidental to reprocessing determination for residual wastes remaining in tanks, ancillary equipment, and facilities. PA results indicate that the performance objectives and measures for the all-pathways dose, the air pathway dose, the radon flux, and groundwater protection are met for both the 1,000-year compliance time period (2020 to 3020) and the post-compliance period (3020 to 12020). The peak dose for the all-pathways analysis in the 1,000-year compliance period is associated with the air pathway, with the peak dose of 4 x 10{sup -5} mSv/yr dominated by tritium resulting from upward gaseous diffusive flux from the residual waste. The peak dose within the sensitivity/uncertainty analysis time period (1,000 to 10,000 years after closure) occurs at about 1,500 years after closure, and results primarily from a peak in {sup 99}Tc groundwater concentration at 100 m down-gradient of the facility. The peak total dose within the sensitivity/uncertainty analysis time period is 0.001 mSv/yr. For all of the sensitivity analyses and uncertainty analyses evaluated, the disposal system also met the performance objectives. In the uncertainty analysis performed with the system level model based on GoldSim{sup C}, the highest calculated groundwater dose in the compliance period was about 7 x 10{sup -4} mSv/yr, and the highest calculated peak dose in the sensitivity/uncertainty analysis period was 0.025 mSv/yr.Doses associated with hypothetical inadvertent human intrusion were calculated for all sources in WMA C and compared to the acute and chronic performance measures in DOE O 435.1. The calculated doses for acute and chronic exposure scenario from potential intrusion into a waste transfer pipeline remain below the DOE O 435.1 performance measure for the time period evaluated beyond 100 years after closure. Acute exposure from drilling into the waste yielded a dose of about 0.36 mSv after the assumed 100-year institutional control period, well below the 5 mSv performance measure for acute exposure. Chronic exposure to waste from drill cuttings in a rural pasture scenario resulted in a dose of about 0.08 mSv/yr after the assumed 100-year institutional control period, well below the 1 mSv/yr performance measure for chronic exposure. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2011

Synthesis, Structure Elucidation, and Redox Properties of [superscript 99]Tc Complexes of Lacunary Wells-Dawson Polyoxometalates: Insights into Molecular [superscript 99]Tc-Metal Oxide Interactions

The isotope {sup 99}Tc ({beta}{sub max}, 293.7; half-life, 2.1 x 10{sup 5} years) is an abundant product of uranium-235 fission in nuclear reactors and is present throughout the radioactive waste stored in underground tanks at the Hanford and Savannah River sites. Understanding and controlling the extensive redox chemistry of {sup 99}Tc is important in identifying tunable strategies to separate {sup 99}Tc from spent fuel and from waste tanks and, once separated, to identify and develop an appropriately stable waste form for {sup 99}Tc. Polyoxometalates (POMs), nanometer-sized models for metal oxide solid-state materials, are used in this study to provide a molecular level understanding of the speciation and redox chemistry of incorporated {sup 99}Tc. In this study, {sup 99}Tc complexes of the ({alpha}{sub 2}-P{sub 2}W{sub 17}O{sub 61}){sup 10-} and ({alpha}{sub 1}-P{sub 2}W{sub 17}O{sub 61}){sup 10-} isomers were prepared. Ethylene glycol was used as a 'transfer ligand' to minimize the formation of TcO{sub 2} {center_dot} xH{sub 2}O. The solution structures, formulations, and purity of TcVO({alpha}{sub 1}/{alpha}{sub 2}-P{sub 2}W{sub 17}O{sub 61}){sup 7-} were determined by multinuclear NMR. X-ray absorption spectroscopy of the complexes is in agreement with the formulation and structures determined from {sup 31}P and {sup 183}W NMR. Preliminary electrochemistry results are consistent with the EXAFS results, showing a facile reduction of the TcVO({alpha}{sub 1}-P{sub 2}W{sub 17}O{sub 61}){sup 7-} species compared to the TcVO({alpha}{sub 2}-P{sub 2}W{sub 17}O{sub 61}){sup 7-} analog. The {alpha}{sub 1} defect is unique in that a basic oxygen atom is positioned toward the {alpha}{sub 1} site, and the Tc{sup V}O center appears to form a dative metal-metal bond with a framework W site. These attributes may lead to the assistance of protonation events that facilitate reduction. Electrochemistry comparison shows that the ReV analogs are about 200 mV more difficult to reduce in accordance with periodic trends.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗