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Narlesky, Joshua Edward

Publications and source records attributed to Narlesky, Joshua Edward.

Summary of Gas Generation Behavior Observed in 3013 Surveillance and Monitoring Program Shelf-Life Experiments

Gas generation experiments have been conducted in small- and full-scale test containers at Los Alamos National Laboratory on samples of plutonium oxide material collected from plutonium processes across the DOE complex and tested at the bounding conditions for the Department of Energy 3013 Standard. The gas composition and pressures in the sealed experimental containers were measured over periods of months to years. These experiments have provided results for the formation and consumption of hydrogen and other gases. The conditions supporting the formation of flammable gas mixtures of hydrogen and oxygen in flammable gas mixtures were also determined. Different behaviors were observed between the materials tested based on their compositions, the stabilization performed on the material, and the post stabilization handling of the material. Many of the experiments are still ongoing. This report summarizes the results obtained for the gas generation behavior for high-purity plutonium oxides and salt-bearing impure plutonium oxides in sealed containers.

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3013 Fire Test 2020: Post-Test Measurements and Analysis

Sandia National Laboratory conducted fire tests on ten 3013 containers with varying amounts of water. The containers with attached manifolds were sent to Los Alamos National Laboratory for post-test measurements of the plastic deformation, the amount of water remaining on the material post-test and the mass loss. The measurements of the plastic deformation were used to determine the free gas volume in each container and manifold post-test. The disassembly of each container was documented by photographs. The amount of pre-test gas constituents is also reported using data in the Sandia Final Report.

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3013 Fire Test 2020: Post-Test Volumes

Sandia National Laboratory conducted fire tests on ten 3013 containers with varying amounts of water. The containers plastically deformed during the fire tests. The plastic deformation increased the free-gas volume within the containers. The amount of plastic deformation is measured and post-test free gas volumes at 25°C is reported.

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Relative humidity threshold for oxygen generation by high-purity plutonium dioxides in 3013 containers

High-purity plutonium dioxide with adsorbed water in a sealed container can generate oxygen, but oxygen will not be generated in low water loading conditions. A threshold for oxygen generation has been observed in the hydrogen generation rate normalized by the specific power for high-purity plutonium dioxide. Normalized hydrogen generation rates above this threshold generate oxygen and below the threshold consume oxygen. The threshold rate is determined by the amount of water adsorbed onto the surface of the oxide. The relative humidity of the atmosphere that the oxide is in equilibrium with determines the amount of physisorbed water adsorbed on the surface. We calculate the relative humidity corresponding to the threshold rate as a function of mass and specific surface area of material stored in 3013 containers. Exceeding the calculated relative humidity may result in flammable gas mixtures of hydrogen and oxygen at some time during storage.

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The 65 Elevated Risk Container Status Relative Humidity Measurements RFID RH/T Sensors in Containers [Slides]

In March of 2023, a memo was issued, drafted by the Container Management, Safety, and Engineering Team, identifying 65 elevated risk legacy containers for priority disposition at TA-55. These 65 were identified separately from the “typical” prioritization decision-making method used at TA-55 to disposition legacy items. This new technique gave important feedback and revealed improvement opportunities for the selection process of legacy containers for disposition. The DOE complex and TA-55 have a long history of nuclear operations and therefore the disposition of these legacy materials is vital.

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MIS Shelf-Life Final Report for Plutonium Oxide Item CAN92 (SSR147) from Rocky Flats Analytical Laboratory Operations

A plutonium/uranium oxide material from the Material Identification and Surveillance (MIS) Program inventory has been studied to determine the gas generation and corrosion behavior in a storage environment. Sample CAN92 represents plutonium/uranium oxides stored in 3013 containers. The material originated in the analytical laboratory at Rocky Flats. This study followed over time the gas pressure and composition of a sample with nominally 0.5 wt% water in a sealed container with an internal volume scaled to 1/400th of the volume of a 3013 container. Gas compositions had been measured periodically over 5 ½ years. The maximum observed gas pressure from gas generation was 117 kPa. The increase over the initial pressure of 77.5 kPa was largely due to the generation of nitrogen and carbon dioxide with minor amounts of hydrogen and nitrous oxide. The internal components of SSR147 were inspected 6.5 years after it was removed from the array. The inside surfaces of the inner bucket exposed to the original sample for 1,937 days had an etched appearance and general corrosion. No pitting was observed on the inner bucket that held the sample.

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MIS Shelf-Life Final Report for Plutonium Oxide Item 1000089 (SSR136 and SSR136A) from Rocky Flats Peroxide Precipitation and Calcination Process

A plutonium dioxide material from the Material Identification and Surveillance (MIS) Program inventory has been studied to determine the gas generation and corrosion behavior in a storage environment. Sample 1000089 represents product-quality plutonium oxides produced in the Rocky Flats peroxide precipitation process currently stored in 3013 containers. This study followed over time the gas pressure and composition of a sample with nominally 0.5 wt% water in a sealed container with an internal volume scaled to 1/500th of the volume of a 3013 container. Gas compositions had been measured periodically over almost 13 years. The maximum observed gas pressure was 204 kPa and was related to a temperature excursion. The maximum observed gas pressure from gas generation was 126 kPa. The increase over the initial pressure of 86.7 kPa was due to the generation of hydrogen, oxygen, and nitrogen. Carbon dioxide, methane and carbon monoxide were minor components of the headspace gas. The material exhibited unusual behavior in that the atmosphere reached flammable levels of hydrogen and oxygen within the first 30 days and remained flammable for the duration of the experiment. It has been determined that the sample inside the reactor was a mixture of the AR material, material calcined at 800 °C, and material calcined at 950 °C. The experiment was terminated in 2012 and unloaded in 2016. A new reactor, SSR136A, was loaded with the original sample freshly calcined at 950 °C. The total pressure inside SSR136A remained close to the initial value of 93 kPa. The total pressure is composed of He (steady levels after the reloading) and hydrogen which is 10% of the reactor’s total pressure. Nitrogen and oxygen compose trace amounts of the reactor headspace. The internal components of SSR136 were inspected in 2021, five years after it was removed from the array. The inside surfaces of the inner bucket exposed to the original sample for 4,576 days had an etched appearance, and pit-like features were observed in the microscopic analysis. No corrosion was observed on the SSR136A inner bucket that held the freshly calcined sample that was exposed for 1,303 days.

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Rules of Use Report Engineering evaluations of nuclear material storage containers against the packaging requirements at TA-55

A set of obligations in the yearly storage container surveillance program, ensures that a retrospective approach is applied with loaded containers in inventory to confirm compliance with all “users” to ensure nuclear material storage container requirements are being followed. Validation that packaged containers are properly used, within a specific set of container types prescribed “bounding conditions of use,” is based on meeting requirements as identified in operating procedures associated with TA55-DOP-091, TA-55 Nuclear Material Packaging, and PA-RD-01022, Nuclear Material Packaging Requirements. The surveillance plan obligation requires the application of local area nuclear material accountability software or (LANMAS) to produce queries. The data queries are used to assess attributes of containers in storage these investigations are conducted on a bi-annual basis. This rules of use (ROU) compliance process ensures proper usage of storage containers as containment systems and therefore provides effective worker protection. It is structured as a supporting effort by implementing aspects of PA-AP-01207, Nuclear Material Container Safety Management at TA-55.

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Prompt Gamma Analysis of ARIES Materials and Updates to the 2015 Calibration Equations

Prompt gamma (PG) analysis is a nondestructive, nuclear, elemental analysis technique that uses charged particle reactions to interrogate a sample, and elements present in the sample matrix are identified through the characteristic gamma-rays emitted from the product nuclei in alpha-p and alpha-n nuclear reactions. This technique has been applied to plutonium oxide packaged in over 4,000 individual 3013 containers, and the concentrations of certain light elements were determined from the integrated peak areas based on a calibration that was published previously. This report provides the results for a new population of 3013 containers packaged with oxide materials produced by the conversion of metal by Advanced Recovery and Integrated Extraction System (ARIES) project using the direct metal oxidation (DMO) process and muffle furnaces. New PG and analytical chemistry data collected since 2015 were added to the existing calibration data sets to refine the calibration parameters. Calibration equations were also developed for determining beryllium and fluorine at low concentrations in high-purity ARIES product oxides. The new fluorine calibration provides an order of magnitude greater sensitivity and results in an additional 1,408 containers in the original population identified as having fluorine as an impurity. Additionally, equations for calculating the lower limits of detection (LLDs) as a function of the actual counting time (live time) were obtained using WLS regression technique for samples in the calibration data set. This resulted in changes to the LLDs published previously.

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Comparing elemental measurements at packaging and after storage for signatures of chloride salt radiolysis

Radiolysis of hydrated alkaline earth chloride salts by alpha radiation from plutonium produces the chloride containing gases HCl and Cl 2 . These gases are known to diffuse out of the plutonium-containing material and contribute to corrosion outside of the convenience container. The alkaline earth elements remain with the plutonium-containing material as oxides or hydroxides. The amount of chlorine within the material after storage will be reduced compared to the amount at packaging. The fraction of the alkaline earth elements that are soluble after storage will be reduced compared to the amount at packaging. These signatures may be observable by comparing the chemical analysis measurements made at packaging and after storage. Comparison of measurements on a single Hanford container shows that the chloride does decrease and the alkaline earth elements have reduced solubility in water. Differences seen with other elements make conclusions difficult.

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Los Alamos National Laboratory SAVY-4000 Field Surveillance Plan (Update for 2021)

The Packaging Surveillance Program section of the Department of Energy (DOE) Manual 441.1- 1, Nuclear Material Packaging Manual (DOE 2008), requires DOE contractors to “ensure that a surveillance program is established and implemented to ensure the nuclear material storage package continues to meet its design criteria.” The Los Alamos National Laboratory (LANL) SAVY-4000 Field Surveillance Plan was first issued in fiscal year (FY) 2013. The surveillance plan is reviewed annually and updated as necessary based on SAVY-4000 surveillance findings, as well as results of the lifetime extension studies. Six surveillance plan updates have been issued, one in 2014, one in 2016, one in 2017, one in 2018 one in 2019 and one in 2020. This 2021 update documents what was actually done in 2020 and what is planned for 2021. Deviations from the 2020 surveillance plan were necessary because some of the planned surveillance containers were not available for examination.

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2021 Hagan Container Surveillance Plan

Prior to 2021, Hagan containers were examined on an ad hoc basis as part of the SAVY-4000 surveillance plan. Given the size, aging horizon, and unique potential failure mechanisms of the Hagan population, the authors identified the need for Hagan-specific surveillance (Kelly, et al., 2020) and have developed this surveillance plan to meet that need.

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Evaluation of the Los Alamos Nuclear Material Packaging Risk Ranking Method

Repackaging nuclear material into robust containers to protect workers and the public has been ongoing at LANL and around the DOE complex for nearly two decades. The number of containers at LANL is around 5,000; limited resources for repackaging material has led to extended repackaging campaigns and the need to prioritize repackaging. Various methodologies have been used to prioritize the repackaging efforts and to demonstrate progress in risk reduction over time (e.g., Boerigter, 1997). The 2000-1 DNFSB recommendation recognized the limited DOE resources for repackaging, and acknowledged the need to “prioritize and schedule tasks to be undertaken with available funds according to consideration of risks.” Later, in DNFSB recommendation 2005-1, in addition to recommending that DOE develop a packaging standard, the Board recommended that “Characterization information should also be used to develop a surveillance program prioritized according to expected material and container risk (including, for example, material type, material form, and the age and type of container).” In response to requests and recommendations from the DOE and DNSFB to prioritize according to worker risk, a risk ranking method based on the potential consequence of dropping a container from 3 meters was developed in 2007 (Smith, 2007) and updated in 2014 (Hoffman, 2014). Various LANL implementation plans for repackaging were developed over the years using this methodology (Stone, 2014). Currently, this method is utilized in conjunction with an algorithm to mitigate programmatic risk to prioritize container repackaging and material processing (Prochnow, 2015). The purpose of this study is to document how the current risk ranking method works, how it is used and potential limitations.

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Surveillance Report on SAVY 4000 and Hagan Nuclear Material Storage Containers Update for FY2020

A Surveillance Program is in place to assess how nuclear material storage containers at LANL are aging in-service. This program is guided by the LANL Surveillance Plan which is required by DOE M441.1-1. The plan is modified as necessary to ensure that any issues identified during surveillance or laboratory studies are examined in future surveillances, and that any lifetime implications are taken into account. Under the plan, overall container integrity is evaluated by a combination of visual inspections and photographs. Multiple measurements are made to assess the SAVY 4000 performance, including, helium leakage rate, O-ring hardness (durometer), O-ring compression set, filter performance and filter water resistance. The containers for surveillance are chosen annually based on the previous surveillance program results and observations. The surveillance plan targets items believed to provide the greatest challenge to the SAVY 4000 container integrity.

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Guide for Joint Participation in a DOE Complex Wide SAVY-4000 Surveillance Program

This document describes LANL Storage Program best practices when working with other User Sites to implement DOE M441.1-1 Manual requirements through the use of the SAVY nuclear material packaging system. It is a Manual directive for Field Element Managers to review and approve the SAVY-4000 container series design (with supporting technical basis) as a packaging system for use at their respective sites. This review and approval incorporates an evaluation of the User Site methodology for SAVY surveillance and the process for documenting its nuclear materials storage program. This document aims to assist the Field Element Mangers and User Sites in the processes necessary to credit LANL SAVY surveillance for key elements of the User Site surveillance plan.

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Proposal for a Hagan Container Surveillance Plan

This white paper proposes a Hagan-specific surveillance plan. Currently, Hagan containers are examined on an ad hoc basis as part of the SAVY-4000 surveillance plan. Given the size, aging horizon, and unique potential failure mechanisms of the Hagan population, the authors believe there is a need to have a Hagan-specific surveillance plan.

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Evaluation of the 2018 Version of the Integrated Surveillance Program Database Pressure Equation

The Integrated Surveillance Program (ISP) Database Pressure Equation was developed to determine with reasonable certainty the total maximum pressure of hydrogen and other gases in packaged 3013 containers stored at Savannah River Site (SRS) in support of the destructive evaluation (DE) process. The pressure equation in the Department of Energy (DOE) 3013 Standard, “Standard for Stabilization, Packaging and Storage of Plutonium- Bearing Materials” (DOE-STD-3013-2004) used a bounding assumption that all the water is decomposed to form hydrogen. However, the results of Los Alamos National Laboratory (LANL) shelf-life experiments showed that hydrogen is consumed, and that the maximum pressures would not approach the design pressure of the 3013 container. Therefore, the ISP Database Pressure Equation was revised in 2008 to include terms for the generation of helium and hydrogen as a function of time, as well as the consumption of water and destruction of hydrogen based on shelf-life results. The 2008 ISP Database Pressure Equation provided a more reasonable estimate of the total maximum pressure in packaged 3013 containers than the pressure equation in versions of the 3013 Standard issued prior to 2018.

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