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At least 271 records · Page 15

The United States Plutonium Balance, 1944 - 2009

This report updates the report -Plutonium: The first 50 years- which was released by the U.S. Department of Energy (DOE) in 1996. The topic of both reports is plutonium, sometimes referred to as Pu-239, which is capable of sustaining a nuclear chain reaction and is used in nuclear weapons and for nuclear power production. This report updates 1994 data through 2009. The four most significant changes since 1994 include: (a) the completion of cleanup activities at the Rocky Flats Plant in 2005; (b) material consolidation and disposition activities, especially shipments from Hanford to the Savannah River Site; (c) the 2007 declaration of an additional 9.0 MT of weapons grade plutonium to be surplus to defense needs in the coming decades; and (d) the opening of the Waste Isolation Pilot Plant (WIPP) near Carlsbad, New Mexico in 1999.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Spectrophotometers for plutonium monitoring in HB-line

This report describes the equipment, control software, calibrations for total plutonium and plutonium oxidation state, and qualification studies for the instrument. It also provides a detailed description of the uncertainty analysis, which includes source terms associated with plutonium calibration standards, instrument drift, and inter-instrument variability. Also included are work instructions for instrument, flow cell, and optical fiber setup, work instructions for routine maintenance, and drawings and schematic diagrams.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NNSS Soils Monitoring: Plutonium Valley (CAU 366) FY2015

Desert Research Institute (DRI) is conducting a field assessment of the potential for contaminated soil transport from the Plutonium Valley Contamination Area (CA) as a result of wind transport and storm runoff in support of National Nuclear Security Administration (NNSA) efforts to complete regulatory closure of the contamination areas. The DRI work is intended to confirm the likely mechanism(s) of transport and determine the meteorological conditions that might cause movement of contaminated soils. The emphasis of the work is on collecting sediment transported by channelized storm runoff at the Plutonium Valley investigation sites. These data will inform closure plans that are being developed, which will facilitate the appropriate closure design and post-closure monitoring. In 2011, DRI installed two meteorological monitoring stations south (station #1) and north (station #2) of the Plutonium Valley CA and a runoff sediment sampling station within the CA. Temperature, wind speed, wind direction, relative humidity, precipitation, solar radiation, barometric pressure, soil temperature, and airborne particulate concentration are collected at both meteorological stations. The maximum, minimum, and average or total (as appropriate) for each of these parameters are recorded for each 10-minute interval. The sediment sampling station includes an automatically activated ISCO sampling pump with collection bottles for suspended sediment, which is activated when sufficient flow is present in the channel, and passive traps for bedload material that is transported down the channel during runoff events. This report presents data collected from these stations during fiscal year (FY) 2015.

54 ENVIRONMENTAL SCIENCES↗

MCNP Parametric Studies of Plutonium Metal and Various Interstitial Moderating Materials

Nuclear Criticality Safety (NCS) has performed calculations evaluating the effect of different interstitial materials on 5.0-kg of plutonium metal. As with all non-fissionable interstitials, the results here illustrate that it requires significant quantities of oil to be intimately mixed with plutonium, reflected by a thick layer of full-density water, to achieve the same reactivity as that of solid plutonium metal.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Estimation of Plutonium-240 Mass in Waste Tanks Using Ultra-Sensitive Detection of Radioactive Xenon Isotopes from Spontaneous Fission

This report details efforts to develop a technique which is able to detect and quantify the mass of 240 Pu in waste storage tanks and other enclosed spaces. If the isotopic ratios of the plutonium contained in the enclosed space is also known, then this technique is capable of estimating the total mass of the plutonium without physical sample retrieval and radiochemical analysis of hazardous material. Results utilizing this technique are reported for a Hanford Site waste tank (TX-118) and a well-characterized plutonium sample in a laboratory environment.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Maintaining Continuity of Knowledge on Nuclear Waste Destined for Geological Repositories. A Case Study of Plutonium Shipments to the Waste Isolation Pilot Plant (WIPP)

This study examines methods that can help maximize confidence in maintaining Continuity of Knowledge (CoK) on plutonium-bearing wastes, from a final safeguards-verification measurement through emplacement underground. The study identifies Containment and Surveillance (C/S) measures that can be applied during packaging of plutonium wastes at the Savannah River Site (SRS) in South Carolina, USA, through shipment to, and receipt and disposal at the Waste Isolation Pilot Plant (WIPP) near Carlsbad, New Mexico, USA. Results of this study could apply to countries with a Comprehensive Safeguards Agreement (CSA) that plan to dispose in a geological repository plutonium or other non-fuel nuclear materials that are under international safeguards.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Mechanical Metallurgy of Plutonium Metal, Alloys, and Allotropes [Slides]

This talk will highlight the mechanical properties of plutonium, but with some discussion of the governing (and often unusual!) underlying metallurgical fundamentals In the interest of time, this talk will focus on unalloyed plutonium metal, its temperature allotropes, and plutonium alloyed to stabilize the delta phase Most of the featured work is taken from the literature; references are provided for both attribution and further reading.

36 MATERIALS SCIENCE↗

Mobile Plutonium Facility (MPF) Calorimeter Measurement Uncertainty

The Department of Energy’s (DOE) National Nuclear Security Administration (NNSA), specifically the Office of Material Management and Minimization (NA-23), is responsible for removing and/or securing special nuclear materials from around the globe that pose a threat to the U.S. and international community. Part of this responsibility requires developing the means to rapidly de-nuclearize weapons programs in foreign countries. The Savannah River Site (SRS) has been tasked by NA-23 to support efforts by establishing a Rapid Response Plutonium Team (RRPT) and developing/procuring the necessary equipment to accomplish the goal of removing plutonium from foreign nations. This includes development of a Mobile Plutonium Facility (MPF) with the overall objective of ensuring the operating crew’s safety while fulfilling the mission to stabilize, package, and ship special nuclear material in the most expeditious manner possible. One piece of equipment supporting this mission is a calorimeter that is to be used in the characterization of the nuclear material. This document provides an investigation of measurements conducted utilizing the MPF calorimeter with the purpose of estimating the uncertainty of its measurements. The evaluations conducted as part of this investigation have identified three sources of variation that are to be integrated into an estimate of the overall uncertainty of measurements provided by the MPF calorimeter. The sources of variation and each of their associated percent relative standard deviations (%RSDs) are base readings with a %RSD of 0.44%, electrical heat standard (EHS) measurements with a %RSD of 1.7157%, and environmental conditions with a %RSD of 0.7984%. Combining these standard deviations in quadrature yields an estimate of the %RSD for overall uncertainty of 1.943%. Note that is a one-sigma expression for the MPF calorimeter measurement uncertainty.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Rossi-α Measurements on a System Consisting of Weapons Grade Plutonium Moderated by Polyethylene [Poster]

A series of experiments nicknamed "TEX," standing for Thermal-Epithermal eXperiments, were performed at the National Criticality Experiments Research Center (NCERC) on the Planet critical assembly. The TEX experiment campaigns are a collaboration between Los Alamos National Laboratory (LANL) and Lawrence Livermore National Laboratory (LLNL) and funded by the Nuclear Criticality Safety Program (NCSP). The TEX experiment consists of several campaigns; this work specifically discusses measurements made on one series of TEX experiments designed to examine the thermal scattering law (TSL) for polyethylene. This series consisted of two different critical configurations which contain plutonium fuel. The plutonium plates are 2 in. by 3 in. by 0.125 in. Zero Power Physics Reactor (ZPPR) plates and are placed in a tray in an array of 6 plates by 4 plates wide creating a 12 in. by 12 in. square. These trays of plutonium are interleaved between polyethylene plates. These measurements differ from previous TEX experiments in that they examine a more thermal neutron spectrum than previously examined by interleaving much thicker interstitial moderating plates than the previous measurements. The two configurations differ in the thickness of polyethylene between the fissile material. While the experiment was designed to examine the TSL, this work only examines the results of Rossi-α measurements on the two different configurations. For both configurations, Rossi-α measurements were performed to experimentally validate the neutron spectrum.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Integral Experiment Final Design for Thermal/Epithermal eXperiments (TEX) Plutonium Additional Mixed Spectrum Configurations

This report presents the final design (CED-2) for three additional mixed-spectra configurations for plutonium Thermal/Epithermal eXperiments (TEX) to target the intermediate energy region (IER-553). The baseline cases of IER-184 (PU-MET-MIXED-002 [2]) spanned the entire fission energy spectrum. Case 3, which had a median fission energy (MFE) of approximately 6E-5 MeV and had a fission fraction of about 42% in the intermediate energy range, resulted in a $k_{eff}$ overestimation of 1.1%. Compared to 749 previous ICSBEP plutonium benchmarks, the baseline cases accurately predicted the experiments in the thermal and fast regions where the majority of benchmarks inhabit. The benchmarks in the intermediate energy region to date are sparse and overestimate $k_{eff}$ with an average C/E between 1.02 and 1.03. The additional proposed configurations span the whole of the intermediate energy region. The experimental design utilizes the plutonium/aluminum metal alloy Zero Power Physics Reactor (ZPPR) Plutonium-Aluminum No-Nickel (PANN) plates with varying polyethylene moderator thicknesses to span the intermediate fission energy region. Each of the cases have varying fractions of thermal, intermediate, and fast fissions. The designs were chosen to maximize the intermediate energy fraction. The experiment will take place on the universal critical assembly machine, Planet. The layers will be split as equally as possible between the lower platen and the upper stationary platform of Planet. The upper half of the experimental configuration will also have an upper reflector of polyethylene of specified thicknesses to achieve criticality when the lower platen is raised fully. The previous IER-184 configurations, specifically Case 3, were used to determine the configurations for the additional experiments and neutronics calculations were used to fine-tune the configurations to ensure criticality. The quadrature sum uncertainty in Δ$k_{eff}$ for Case 3 in PU-MET-MIXED-002 was found to be 0.00219. Section 3.8 gives a detailed description of the uncertainties calculated. The additional configurations, which are based directly on Case 3, are expected to have similar uncertainties. However, it is possible to reduce the overall uncertainty of Δ$k_{eff}$ for the additional configurations using the knowledge obtained from the calculations in the benchmark.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Plutonium Oxidation State Distribution under WIPP Relevant Conditions (Rev. 2)

The oxidation state of plutonium in the Waste Isolation Pilot Plant (WIPP) environment has been a topic of interest since the initial compliance certification application. Plutonium (Pu) was initially expected to be present primarily as Pu(IV), but since the presence of Pu(III) could not be ruled out, it was also included in performance assessment (PA) calculations. The redox of the other variant actinides, uranium (U) and neptunium (Np), are also coupled to the plutonium redox. This led to a position in performance assessment calculations that is commonly referred to as “50/50”. In which half of the PA realizations assume solubility is dominated by the low oxidation state [U(IV), Np(IV), Pu(III)] and the other half assume solubility is dominated by the higher oxidation state [U(VI), Np(V), Pu(IV)]. Recently, a joint group of WIPP project participants from Los Alamos National Laboratory (LANL), Sandia National Laboratories (SNL), and the Department of Energy’s Carlsbad Field Office (DOE-CBFO) agreed on a new path forward for the oxidation state model in PA which will decouple the redox active actinides and will instead consider their redox as a function of E h . This will take the current binary approach and turn it into a system with four possible redox states.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Gamma radiation characteristics of plutonium dioxide fuel

Investigation of plutonium dioxide as an isotopic fuel for Radioisotope Thermoelectric Generators yielded the isotopic composition of production-grade plutonium dioxide fuel, sources of gamma radiation produced by plutonium isotopes, and the gamma flux at the surface.

Gingo, P. J.↗

A Plutonium-Contaminated Wound, 1985, USA

A hand injury occurred at a U.S. facility in 1985 involving a pointed shaft (similar to a meat thermometer) that a worker was using to remove scrap solid plutonium from a plastic bottle. The worker punctured his right index finger on the palm side at the metacarpal-phalangeal joint. The wound was not through-and- through, although it was deep. The puncture wound resulted in deposition of ~48 kBq of alpha activity from the weapons-grade plutonium mixture with a nominal 12 to 1 Pu-alpha to {sup 241}Am-alpha ratio. This case clearly showed that DTPA was very effective for decorporation of plutonium and americium. The case is a model for management of wounds contaminated with transuranics: (1) a team approach for dealing with all of the issues surrounding the incident, including the psychological, (2) early surgical intervention for foreign-body removal, (3) wound irrigation with DTPA solution, and (4) early and prolonged DTPA administration based upon bioassay and in vivo dosimetry.

61 RADIATION PROTECTION AND DOSIMETRY↗

Characterizing surplus US plutonium for disposition

The United States (US) has identified 61.5 metric tons (MT) of plutonium that is permanently excess to use in nuclear weapons programs, including 47.2 MT of weapons-grade plutonium. Surplus inventories will be stored safely by the Department of Energy (DOE) and then transferred to facilities that will prepare the plutonium for permanent disposition. The Savannah River National Laboratory (SRNL) operates a Feed Characterization program for the Office of Fissile Materials Disposition (OFMD) of the National Nuclear Security Administration (NNSA) and the DOE Office of Environmental Management (DOE-EM). SRNL manages a broad program of item tracking through process history, laboratory analysis, and non-destructive assay. A combination of analytical techniques allows SRNL to predict the isotopic and chemical properties that qualify materials for disposition through the Mixed Oxide (MOX) Fuel Fabrication Facility (MFFF). The research also defines properties that are important for other disposition paths, including disposal to the Waste Isolation Pilot Plant (WIPP) as transuranic waste (TRUW) or to high-level waste (HLW) systems.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

ESTIMATING IMPURITIES IN SURPLUS PLUTONIUM FOR DISPOSITION

The United States holds at least 61.5 metric tons (MT) of plutonium that is permanently excess to use in nuclear weapons programs, including 47.2 MT of weapons-grade plutonium. Surplus inventories will be stored safely by the Department of Energy (DOE) and then transferred to facilities that will prepare the plutonium for permanent disposition. The Savannah River National Laboratory (SRNL) operates a Feed Characterization program for the Office of Fissile Materials Disposition of the National Nuclear Security Administration and the DOE Office of Environmental Management. Many of the items that require disposition are only partially characterized, and SRNL uses a variety of techniques to predict the isotopic and chemical properties that are important for processing through the Mixed Oxide Fuel Fabrication Facility and alternative disposition paths. Recent advances in laboratory tools, including Prompt Gamma Analysis and Peroxide Fusion treatment, provide data on the existing inventories that will enable disposition without additional, costly sampling and destructive analysis.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

TRACKING SURPLUS PLUTONIUM FROM WEAPONS TO DISPOSITION

Supporting nuclear nonproliferation and global security principles, beginning in 1994 the United States has withdrawn more than 50 metric tons (MT) of government-controlled plutonium from potential use in nuclear weapons. The Department of Energy (DOE), including the National Nuclear Security Administration, established protocols for the tracking of this "excess" and "surplus" plutonium, and for reconciling the current storage and utilization of the plutonium to show that its management is consistent with the withdrawal policies. Programs are underway to ensure the safe and secure disposition of the materials that formed a major part of the weapons stockpile during the Cold War, and growing quantities have been disposed as waste, after which they are not included in traditional nuclear material control and accountability (NMC&A) data systems. A combination of resources is used to perform the reconciliations that form the basis for annual reporting to DOE, to U.S. Department of State, and to international partners including the International Atomic Energy Agency.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Initial Testing of Mediated Electrochemical Oxidation for Inclusion in the Plutonium-238 Production Program

Oak Ridge National Laboratory is currently restarting the United States’ capability to produce kilogram quantities of 238Pu annually for space power applications. This involves the purification of 238Pu from neutron-irradiated 237Np targets and conversion to heat-source plutonium oxide product for shipment to Los Alamos National Laboratory. Dissolution of the plutonium oxide product material is required to obtain an isotopic assay and impurity analysis of the product material. In addition, any off-specification product will need to be dissolved for re-purification. An electrochemical method that produces highly oxidizing ions in solution is currently being investigated as a rapid method for dissolving these plutonium oxide samples.

Myhre, Kristian↗

Custom Equipment Development for Processing of Surplus Plutonium

The Strategic Laboratory Assessment (SLA), a collaborative team of SRNL and ORNL personnel, has been established to advance the objectives of the Surplus Plutonium Disposition (SPD) Project, by identifying and developing technologies to accelerate disposition, reduce life cycle costs, minimize worker radiation exposure, improve worker safety, and minimize Surplus Plutonium Disposition Program risks. [1] The SLA team has identified can cutting and plutonium (Pu) oxide size reduction as two glovebox processes where technology enhancements would be valuable. The DOESTD-3013 package currently in use for Pu downblending requires cutting two nested cans before the inner convenience can that holds the Pu oxide may be accessed for further processing. A rotary tubing-style cutter is used for opening the 3013 packages within the glovebox. Collet changeouts are required between cutting of the outer and inner cans. The SLA team is currently developing and testing an adjustable-clamp can cutter design that eliminates collet changeouts and allows cutting of the outer and inner can at the same time, resulting in significant reduction of radiological dose and process time, as well as improved ergonomics. To meet the Pu oxide particle size requirement, size reduction of Pu oxide agglomerations must be performed within the process gloveboxes. The SLA team has identified jaw crushing technology as an alternative to the currently employed rotary mill. Jaw crusher advantages include reduced dust within the glovebox, increased batch sizes, and easier integration with other glovebox processes due to the flow-through nature of jaw crushing. Commercially manufactured jaw crushers are either too large and/or too heavy for implementation in the SPD gloveboxes, so the SLA team is developing and testing a custom jaw crusher to meet the needs of the SPD Project.

Krementz, Daniel [Savannah River National Laborato↗