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Title: Preparation and Characterization of a Master Blend of Plutonium Oxide for the 3013 Large Scale Shelf-Life Surveillance Project

Abstract

A mixture of chlorine-containing, impure plutonium oxides has been produced and has been given the name Master Blend. This large quantity of well-characterized chlorinecontaining material is available for use in the Integrated Surveillance and Monitoring Program for shelf-life experiments. It is intended to be representative of materials packaged to meet DOE-STD-3013.1 The Master Blend contains a mixture of items produced in Los Alamos National Laboratory’s (LANL) electro-refining pyrochemical process in the late 1990s. Twenty items were crushed and sieved, calcined to 800ºC for four hours, and blended multiple times. This process resulted in four batches of Master Blend. Calorimetry and density data on material from the four batches indicate homogeneity.

Authors:
 [1];  [1];  [1];  [1];  [1]; ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Environmental Management (EM)
OSTI Identifier:
1352389
Report Number(s):
LA-UR-17-22879
DOE Contract Number:
AC52-06NA25396
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 3013 electro-refining storagage radioactive

Citation Formats

Gillispie, Obie William, Worl, Laura Ann, Veirs, Douglas Kirk, Stroud, Mary Ann, Narlesky, Joshua Edward, Berg, John M., Kelly, Elizabeth J., Padilla, Dennis D., Bender, Beverly, Lopez, Annabelle S., Martinex, Max A., Trujillo, Leonardo A., and Wilson, Edward L. Preparation and Characterization of a Master Blend of Plutonium Oxide for the 3013 Large Scale Shelf-Life Surveillance Project. United States: N. p., 2017. Web. doi:10.2172/1352389.
Gillispie, Obie William, Worl, Laura Ann, Veirs, Douglas Kirk, Stroud, Mary Ann, Narlesky, Joshua Edward, Berg, John M., Kelly, Elizabeth J., Padilla, Dennis D., Bender, Beverly, Lopez, Annabelle S., Martinex, Max A., Trujillo, Leonardo A., & Wilson, Edward L. Preparation and Characterization of a Master Blend of Plutonium Oxide for the 3013 Large Scale Shelf-Life Surveillance Project. United States. doi:10.2172/1352389.
Gillispie, Obie William, Worl, Laura Ann, Veirs, Douglas Kirk, Stroud, Mary Ann, Narlesky, Joshua Edward, Berg, John M., Kelly, Elizabeth J., Padilla, Dennis D., Bender, Beverly, Lopez, Annabelle S., Martinex, Max A., Trujillo, Leonardo A., and Wilson, Edward L. Mon . "Preparation and Characterization of a Master Blend of Plutonium Oxide for the 3013 Large Scale Shelf-Life Surveillance Project". United States. doi:10.2172/1352389. https://www.osti.gov/servlets/purl/1352389.
@article{osti_1352389,
title = {Preparation and Characterization of a Master Blend of Plutonium Oxide for the 3013 Large Scale Shelf-Life Surveillance Project},
author = {Gillispie, Obie William and Worl, Laura Ann and Veirs, Douglas Kirk and Stroud, Mary Ann and Narlesky, Joshua Edward and Berg, John M. and Kelly, Elizabeth J. and Padilla, Dennis D. and Bender, Beverly and Lopez, Annabelle S. and Martinex, Max A. and Trujillo, Leonardo A. and Wilson, Edward L.},
abstractNote = {A mixture of chlorine-containing, impure plutonium oxides has been produced and has been given the name Master Blend. This large quantity of well-characterized chlorinecontaining material is available for use in the Integrated Surveillance and Monitoring Program for shelf-life experiments. It is intended to be representative of materials packaged to meet DOE-STD-3013.1 The Master Blend contains a mixture of items produced in Los Alamos National Laboratory’s (LANL) electro-refining pyrochemical process in the late 1990s. Twenty items were crushed and sieved, calcined to 800ºC for four hours, and blended multiple times. This process resulted in four batches of Master Blend. Calorimetry and density data on material from the four batches indicate homogeneity.},
doi = {10.2172/1352389},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Mon Apr 10 00:00:00 EDT 2017},
month = {Mon Apr 10 00:00:00 EDT 2017}
}

Technical Report:

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  • The Department of Energy (DOE) is embarking upon a program to store large quantities of plutoniumbearing materials for up to fifty years. The Los Alamos National Laboratory Shelf Life Project was established to bound the behavior of plutoniumbearing material meeting the DOE 3013 Standard. The shelf life study monitors temperature, pressure and gas composition over oxide materials in a limited number of large-scale 3013 inner containers and in many small-scale containers. For the large-scale study, baseline plutonium oxides, oxides exposed to high-humidity atmospheres, and oxides containing chloride salt impurities are planned. The first largescale container represents a baseline and containsmore » dry plutonium oxide prepared according to the 3013 Standard. This container has been observed for pressure, temperature and gas compositional changes for less than a year. Results indicate that no detectable changes in pressure and gas composition are observed.« less
  • In this report, Los Alamos scientists characterize properties relevant to storage of an impure plutonium oxide (74 mass % plutonium) in accordance with the Department of Energy (DOE) standard DOE-STD-3013-96. This oxide is of interest because it is the first impure plutonium oxide sample to be evaluated and it is similar to other materials that must be stored. Methods used to characterize the oxide at certain points during calcination include surface-area analyses, mass loss-on-ignition (LOI) measurements, elemental analysis, moisture-adsorption measurements, and quantitative supercritical-CO{sub 2} extraction of adsorbed water. Significant decreases in the LOI and surface area occurred as the oxidemore » was calcined at progressively increasing temperatures. Studies indicate that supercritical-CO{sub 2} extraction is an effective method for removing adsorbed water from oxides. We extracted the water from powdered oxides (high-purity ZrO{sub 2}, pure PuO{sub 2}, and impure plutonium oxide) using CO{sub 2} at 3000 psi pressure and 75{degrees}C, and we quantitatively determined it by using gravimetric and dew-point procedures. The effectiveness of the extraction method is demonstrated by good agreement between the amounts of water extracted from pure zirconium and plutonium dioxides and the mass changes obtained from LOI analyses. However, the amount of moisture (0.025 mass %) extracted from the impure plutonium oxide after it had been calcined at 950{degrees}C and stored for a period of months is much less than the LOI value (0.97 mass %). These results imply that the impure plutonium oxide is free of adsorbed water after calcination at 950{degrees}C, even though the sample does not satisfy the LOI requirement of <0.50 mass % for storage.« less
  • This document presents a site-specific DOE-STD-3013 (3013) surveillance program for 3013 material stored at Lawrence Livermore National Laboratory (LLNL) in the B332 Plutonium Facility. The 3013 standard requires the development of a surveillance program to assure the long-term safety of plutonium storage in 3013 compliant containers. A complex-wide Integrated Surveillance Program in Support of Long-Term Storage of Plutonium-Bearing Materials (ISP)(LA-UR-00-3246, Revision 1, March 2001) has been developed to give guidance on an acceptable surveillance approach and to set up a mechanism to integrate surveillance activities and facilitate the sharing of lessons learned. This LLNL 3013 surveillance program has been developedmore » following guidelines established for Storage Sites in the ISP and is sufficient for the storage in the LLNL Plutonium Facility. The LLNL 3013 surveillance program must be coupled with the DOE complex wide Materials Identification and Surveillance (MIS) program and the ISP led by Savannah River Site (SRS). These programs support the technical basis for continuing safe storage of plutonium packages and provide the technical basis for the limited scope of the site-specific LLNL 3013 surveillance program. The LLNL 3013 surveillance program calls for surveillance of 3013 packages to begin approximately three years after packaging of the first oxide. One percent of the stored packages per year will be randomly selected and nondestructively examined (NDE) by LLNL per the guidelines of the ISP. Additional packages may be selected for NDE if recommended by the ISP Steering Committee and agreed upon by the MIS Working Group. One selected package will be shipped to SRS for destructive analysis each year starting when SRS can receive them. This is expected to be in FY2007. We expect to store a maximum of 400 3013 packages. This would result in an expected maximum of 4 surveillances per year. The activities outlined in the program evolved from the current understanding of materials behavior and may be significantly modified as the knowledge base increases. This surveillance program is a living document that will be revised based on information gathered through this program as well through the MIS, ISP and lessons learned from other DOE storage sites.« less
  • A set of six long-term, full-scale experiments were initiated to determine the type and extent of corrosion that occurs in 3013 containers packaged with chloride-bearing plutonium oxide materials. The materials were exposed to a high relative humidity environment representative of actual packaging conditions for the materials in storage. The materials were sealed in instrumented, inner 3013 containers with corrosion specimens designed to test the corrosiveness of the environment inside the containers under various conditions. This report focuses on initial loading conditions that are used to establish a baseline to show how the conditions change throughout the storage lifetime of themore » containers.« less