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At least 667 records · Page 37

Corrective Action Investigation Plan for Corrective Action Unit 568: Area 3 Plutonium Dispersion Sites Nevada National Security Site, Nevada

CAU 568 is a grouping of sites where there has been a suspected release of contamination associated with nuclear testing. This document describes the planned investigation of CAU 568, which comprises the following corrective action sites (CASs): (1) 03-23-17, S-3I Contamination Area; (2) 03-23-19, T-3U Contamination Area; (3) 03-23-20, Otero Contamination Area; (4) 03-23-22, Platypus Contamination Area; (5) 03-23-23, San Juan Contamination Area; and (6) 03-23-26, Shrew/Wolverine Contamination Area. These sites are being investigated because existing information on the nature and extent of potential contamination is insufficient to evaluate and recommend corrective action alternatives (CAAs). Additional information will be obtained by conducting a corrective action investigation before evaluating CAAs and selecting the appropriate corrective action for each CAS. The results of the field investigation will support a defensible evaluation of viable CAAs that will be presented in the investigation report.

54 ENVIRONMENTAL SCIENCES↗

Corrective Action Decision Document/Closure Report for Corrective Action Unit 571: Area 9 Yucca Flat Plutonium Dispersion Sites, Nevada National Security Site, Nevada, Revision 0 with ROTC 1

The purpose of this CADD/CR is to provide documentation and justification that no further corrective action is needed for the closure of CAU 571 based on the implementation of corrective actions. This includes a description of investigation activities, an evaluation of the data, and a description of corrective actions that were performed. The CAIP provides information relating to the scope and planning of the investigation. Therefore, that information will not be repeated in this document.

54 ENVIRONMENTAL SCIENCES↗

Streamlined approach for environmental restoration (SAFER) plan for corrective action unit 412: clean slate I plutonium dispersion (TTR) tonopah test range, Nevada, revision 0

This Streamlined Approach for Environmental Restoration (SAFER) Plan addresses the actions needed to achieve closure for Corrective Action Unit (CAU) 412. CAU 412 is located on the Tonopah Test Range and consists of a single corrective action site (CAS), TA-23-01CS, Pu Contaminated Soil. There is sufficient information and historical documentation from previous investigations and the 1997 interim corrective action to recommend closure of CAU 412 using the SAFER process. Based on existing data, the presumed corrective action for CAU 412 is clean closure. However, additional data will be obtained during a field investigation to document and verify the adequacy of existing information and determine whether the CAU 412 closure objectives have been achieved. This SAFER Plan provides the methodology to gather the necessary information for closing the CAU.The following summarizes the SAFER activities that will support the closure of CAU 412:• Collect environmental samples from designated target populations to confirm or disprove the presence of contaminants of concern (COCs) as necessary to supplement existing information.• If no COCs are present, establish clean closure as the corrective action. • If COCs are present, the extent of contamination will be defined and further corrective actions will be evaluated with the stakeholders (NDEP, USAF).• Confirm the preferred closure option is sufficient to protect human health and the environment.

01 COAL, LIGNITE, AND PEAT↗

In-Situ Gamma-Ray Assay of the West Cell Line in the 235-F Plutonium Fuel Form Facility

On August 29 th , 2013, scientists from SRNL took a series of in-situ gamma-ray measurements in the maintenance trench beneath Cells 6-9 on the west line of the PuFF facility using an uncollimated, high-purity germanium detector. The detector efficiency was estimated using a combination of MCNP simulations and empirical measurements. Data analysis was performed using three gamma-rays emitted by Pu-238 (99.85 keV, 152.7 keV, and 766.4 keV) providing three independent estimates of the mass of Pu-238 holdup in each of the cells. The weighted mean of these three results was used as the best estimate of Pu-238 holdup in the West Cell Line of PuFF. The results of the assay measurements are found in the table below along with the results from the scoping assay performed in 2006. All uncertainties in this table (as well as the rest of the report) are given as 1σ. The total holdup in the West Cell Line was 2.4 ± 0.7 grams. This result is 0.6 g higher than the previous estimate, a 0.4σ difference.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

In-Situ Gamma-Ray Assay of the East Cell Line in the 235-F Plutonium Fuel Form Facility

On September 17 th -19 th , 2013, scientists from SRNL took a series of in-situ gamma-ray measurements in the maintenance trench beneath Cells 1-5 on the east line of the PuFF facility using a well-collimated, high-purity germanium detector. The cell interiors were assayed along with the furnaces and storage coolers that protrude beneath the cells. The detector efficiency was estimated using a combination of MCNP simulations and empirical measurements. Data analysis was performed using three gamma-rays emitted by Pu-238 (99.85 keV, 152.7 keV, and 766.4 keV) providing three independent estimates of the mass of Pu-238 holdup in each of the cells. The weighted mean of these three results was used as the best estimate of Pu-238 holdup in the East Cell Line of PuFF. The results of the assay measurements are found in the table on the following page along with the results from the scoping assay performed in 2006. All uncertainties in this table (as well as the rest of the report) are reported at 1σ. Summing the assay results and treating MDAs as M 238Pu = 0 ± MDA, the total holdup in the East Cell Line was 240 ± 40 grams. This result is 100 grams lower than the previous estimate, a 0.55σ difference. The uncertainty in the Pu-238 holdup is also reduced substantially relative to the 2006 scoping assay. However, the current assay results are in agreement with the 2006 scoping assay results due to the large uncertainty associated with the 2006 scoping assays. The current assay results support the conclusion that the 2006 results bound the Pu-238 mass in Cells 1-5. These results should be considered preliminary since additional measurements of the East Cell line are scheduled for 2017 and 2018. Those measurements will provide detailed information about the distribution of Pu-238 in the cells to be used to refine the results of the current assay.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Plutonium Immobilization and Mobilization by Soil Organic Matter

The human and environmental risks associated with Pu disposal, remediation, and nuclear accidents scenarios stems mainly from the very long half-lives of several of its isotopes. The SRS, holding one-third of the nation’s Pu inventory, has a long-term stewardship commitment to investigation of Pu behavior in the groundwater and downgradient vast wetlands. Pu is believed to be essentially immobile due to its low solubility and high particle reactivity to mineral phase or natural organic matter (NOM). For example, in sediments collected from a region of SRS, close to a wetland and a groundwater plume, 239,240Pu concentrations suggest immobilization by NOM compounds, as Pu correlate with NOM contents. Micro-SXRF data indicate, however, that Pu does not correlate with Fe. However, previous studies reported Pu can be transported several kilometers in surface water systems, in the form of a colloidal organic matter carrier, through wind/water interactions. The role of NOM in both immobilizing or re-mobilizing Pu thus has been demonstrated. Our results indicate that more Pu (IV) than (V) was bound to soil colloidal organic matter (COM), amended at far-field concentrations. Contrary to expectations, the presence of NOM in the F-Area soil did not enhance Pu fixation to the organic-rich soil, when compared to the organic-poor soil or the mineral phase from the same soil source, due to the formation of COM-bound Pu. Most importantly, Pu uptake by organic-rich soil decreased with increasing pH because more NOM in the colloidal size desorbed from the particulate fraction at elevated pH, resulting in greater amounts of Pu associated with the COM fraction. This is in contrast to previous observations with low-NOM sediments or minerals, which showed increased Pu uptake with increasing pH levels. This demonstrates that despite Pu immobilization by NOM, COM can convert Pu into a more mobile form. Sediment Pu concentrations in the SRS F-Area wetland were correlated to total organic carbon and total nitrogen contents and even more strongly to hydroxamate siderophore (HS) concentrations. The HS were detected in the particulate or colloidal phases of the sediments but not in the low molecular fractions (< 1000 Da). Macromolecules which scavenged the majority of the potentially mobile Pu were further separated from the bulk mobile organic matter fraction (“water extract”) via isoelectric focusing experiment (IEF). An ESI FTICR-MS spectral comparison of the IEF extract and a siderophore standard (desferrioxamine; DFO) suggested the presence of HS functionalities in the IEF extract.

54 ENVIRONMENTAL SCIENCES↗

Precision Plutonium Thermodynamics

This presentation discusses some of the fundamental characteristics of a solid and how they can be used to observe thermodynamic changes.

36 MATERIALS SCIENCE↗

2015 In-Situ Gamma-Ray Assay of the West Cell Line in the 235-F Plutonium Fuel Form Facility

In November and December 2015, scientists from SRNL took a series of in-situ gamma-ray measurements through the windows in front of Cells 6-9 on the west line of the PuFF facility using a shielded, 120% high-purity germanium detector. The detector efficiency was estimated using a combination of MCNP simulations and empirical measurements. Where possible, the distribution of the Pu-238 in the cells was determined using the Germanium Gamma-ray Imager (GeGI). This distribution was then fed into the MCNP model to quantify the Pu-238 in each cell. Data analysis was performed using three gamma rays emitted by Pu-238 (99.85 keV, 152.7 keV, and 766.4 keV) providing three independent estimates of the mass of Pu-238 holdup in each of the cells.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Ab initio study of the effects of dilute defects on the local structure of unalloyed δ-plutonium

We used density functional theory to examine the effects impurities and vacancies in the dilute limit in order to explore the effects on the local structure of the unalloyed face centered cubic δ-Pu lattice. The impurities considered are the radioactive daughter U or stabilizers in δ-phase stabilizer Ga. These impurities were placed at various interstitial sites, including octahedral, tetrahedral, and split interstitial along the (100) direction, as well as substitutional lattice sites. Self-interstitials, mono and di-vacancies were also considered. In addition we examined impurity-vacancy complexes at first and second nearest neighboring distances from each other. Radial distribution functions were plotted to gauge the local structural variations around the defect within the lattice and volume change with structural variation quantifies influence on thermodynamics. These local distortions will be discussed in this report.

36 MATERIALS SCIENCE↗

Addendum to the Closure Report for Corrective Action Unit 411: Double Tracks Plutonium Dispersion (Nellis), Nevada Test and Training Range, Nevada, Revision 0

The Corrective Action Unit (CAU) 411 Closure Report (CR) was published in June 2016 (NNSA/NFO, 2016). The purpose of this addendum is to clarify language in the CR relating to the field instrument for the detection of low-energy radiation (FIDLER), provide the waste disposal documentation for waste generated during the corrective action investigation (CAI), and reference a letter from the U.S. Air Force (USAF) regarding the closure of CAU 411.

54 ENVIRONMENTAL SCIENCES↗

Closure Report for Corrective Action Unit 568: Area 3 Plutonium Dispersion Sites Nevada National Security Site, Nevada, Revision 1

The purpose of this CR is to provide documentation and justification that no further corrective action is needed for the closure of CAU 568 based on the implementation of corrective actions. This includes a description of closure activities that were performed and an evaluation of the verification data. The CAP (NNSA/NFO, 2016a) and ROTC-1 (NNSA/NFO, 2016c) provide information relating to the selection of CAAs and the reasoning behind their selection. The CADD (NNSA/NFO, 2015) identifies the release sites that require additional corrective action and presents information supporting the selection of CAAs.

54 ENVIRONMENTAL SCIENCES↗

Plutonium Migration during the Leaching of Cemented Radioactive Waste Sludges

One of the most challenging components of the UK nuclear legacy is Magnox sludge, arising from the corrosion of Mg alloy-clad irradiated metallic U fuel that has been stored in high pH ponds. The sludges mainly comprise Mg hydroxide and carbonate phases, contaminated with fission products and actinides, including Pu. Cementation and deep geological disposal is one option for the long-term management of this material, but there is a need to understand how Pu may be leached from the waste, if it is exposed to groundwater. Here, we show that cemented Mg(OH) 2 powder prepared with Pu(IV) aq is altered on contact with water to produce a visibly altered ‘leached zone’, which penetrates several hundred microns into the sample. In turn, this zone shows slow leaching of Pu, with long-term leaching rates between 1.8–4.4 × 10 -5 % of total Pu per day. Synchrotron micro-focus X-ray fluorescence mapping identified decreased Pu concentration within the ‘leached zone’. A comparison of micro-focus X-ray absorption spectroscopy (µ-XAS) spectra collected across both leached and unleached samples showed little variation, and indicated that Pu was present in a similar oxidation state and coordination environment. Fitting of the XANES spectra between single oxidation state standards and EXAFS modeling showed that Pu was present as a mixture of Pu(IV) and Pu(V). The change in Pu oxidation from the stock solution suggests that partial Pu oxidation occurred during sample ageing. Similarity in the XAS spectra from all samples, with different local chemistries, indicated that the Pu oxidation state was not perturbed by macro-scale variations in cement chemistry, surface oxidation, sample aging, or the leaching treatment. These experiments have demonstrated the potential for leaching of Pu from cementitious waste forms, and its underlying significance requires further investigation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗