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DOE OSTI2017

Sensitivity and Uncertainty Analysis of Plutonium and Cesium Isotopes in Modeling of BR3 Reactor Spent Fuel

Nuclear forensics has a broad task to characterize recovered nuclear or radiological material and interpret the results of investigation. One approach to isotopic characterization of nuclear material obtained from a reactor is to chemically separate and perform isotopic measurements on the sample and verify the results with modeling of the sample history, for example, operation of a nuclear reactor. The major actinide plutonium and fission product cesium are commonly measured signatures of the fuel history in a reactor core. This study investigates the uncertainty of the plutonium and cesium isotope ratios of a fuel rod discharged from a research pressurized water reactor when the location of the sample is not known a priori. A sensitivity analysis showed overpredicted values for the 240 Pu/ 239 Pu ratio toward the axial center of the rod and revealed a lower probability of the rod of interest (ROI) being on the periphery of the assembly. The uncertainty analysis found the relative errors due to only the rod position and boron concentration to be 17% to 36% and 7% to 15% for the 240 Pu/ 239 Pu and 137 Cs/ 135 Cs ratios, respectively. Lastly, this study provides a method for uncertainty quantification of isotope concentrations due to the location of the ROI. Similar analyses can be performed to verify future chemical and isotopic analyses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Data Testing of Polyethylene Thermal Scattering Law with New Thermal Epithermal eXperiments (TEX) Plutonium Baseline Benchmark, PU-MET-MIXED-002

Five plutonium baseline experiments completed in September of 2018 from the Thermal Epithermal eXperiments (TEX) program have been accepted by the International Criticality Safety Benchmark Evaluation Project as PU-MET-MIXED-002 and will be included in the 2020 version of the handbook. The experiments were made up of stacked layers of plutonium Zero Power Physics Reactor (ZPPR) plates moderated by polyethylene (PE, chemical formula C2H4) to varying degrees to create configurations with five different neutron spectra, including one fast configuration, one thermal configuration, and three mixed configurations. Calculations of the benchmark show overprediction of k eff when using the most recent release of the Evaluated Nuclear Data File Version B (ENDF/B) library release (VIII.0) cross sections, particularly when compared to the previous ENDF/B-VII.1 results. One potential source of overprediction was hypothesized to be the new Molecular Dynamics (MD) generated PE Thermal Scattering Law (TSL). The overprediction was shown via calculation to not be caused by the new ENDF/B-VIII.0 thermal scattering law, and in fact the overprediction was mitigated by the new PE TSL.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Effect of Plutonium on Uranium Oxide Microstructural Fingerprint

The analysis of particulates from environmental sampling is routinely performed for nuclear forensics applications. In order to increase the tools available for nuclear forensics applications, capability development materials (CDMs), or reference particulates, are necessary for developing and benchmarking new analytical methods. Historically, these CDM particulates have been produced with highly controlled and characterized isotopic and size parameters for applications in developing and benchmarking particle sizers and mass spectrometry analytical methods [1- 4]. However, the development of CDMs with highly characterized particle morphology and phase of the particles is vital for aiding in the development and benchmarking of particle analytical methods for those parameters. In many cases, key properties such as crystallographic phase, morphology, and microstructure, may be correlated to processing history of environmental sampling particulates [5]. To that end, this work investigates determining the structural fingerprint of produced Pu-doped uranium oxide CDMs using transmission electron microscopy (TEM). The particulates, one of which shown in Figure 1, were synthesized to Fig. 1. Single particulate of uranium oxide fabricated using the THESEUS technique. develop capabilities for environmental sampling investigations. These particles are monodisperse at diameter of 1 μm and a range of plutonium concentrations from 0- 1,000 ppm. Given their small diameter, TEM analysis was ideal for studying the particulate structural fingerprint in detail. Previous investigations confirmed the external homogeneity of the particulates at different plutonium concentrations, however this analysis focuses on determining the grain structure, phase distribution, and porosity of the particulates.

Mayer, Jack [Univ. of Florida, Gainesville, FL (Un↗

DOE OSTI2019

Jupiter: A Proposed Benchmark for Lead Void Worth with Plutonium

In the summer of 2017, a series of measurements were performed at the National Criticality Experiments Research Center (NCERC) in collaboration with the Japanese Atomic Energy Agency (JAEA) to measure the reactivity worth of voids in an array of lead and plutonium. This experiment, called Jupiter, measured multiple configurations of an array of aluminum boxes containing plutonium, aluminum, and lead plates. For some configurations, a selection of the lead interstitial plates were swapped with aluminum spacer frames to create “voids” in the lead interstitial material. Comparing the excess reactivity of the systems provides an empirical value of the lead void reactivity worth. These measurements were part of a larger collaboration to measure lead void reactivity worth with multiple nuclear material types and enrichments. This included other measurement series with both highly-enriched uranium (HEU), and a mixture of HEU and natural uranium to simulate low-enriched uranium (LEU). These data sets will be useful to the JAEA for a potential lead-bismuth cooled accelerator driven system. Additionally, there are not very many benchmarks in the International Criticality Safety Benchmark Evaluation Project (ICSBEP) handbook sensitive to lead cross sections. Given that lead is widely used as a radiation shield and is part of new reactor designs, having more benchmarks in the ICSBEP handbook to better support cross section validation is important. Additional integral experiments could also aid in determining whether improvements have been made in new lead cross section evaluations. A benchmark evaluation for this experiment is being proposed in order to help fulfill these needs. Such evaluations contain both measured data, results from detailed transport code models, and analyses of the uncertainties associated with each. Examples of these uncertainties include the uncertainty in the measured excess reactivity, the composition of components, or their positioning within the model. This means it is easier to make comparisons between the measured and simulated data and better understand where improvements can be made to nuclear data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2019

Two-Exponential Rossi-Alpha Analysis of Copper- and Polyethylene-Reflected Plutonium

The prompt neutron decay constant $\mathcal{α}$, which is used to infer reactivity, is estimated using the Rossi-alpha technique that is predicated on fitting Rossi-alpha histograms. The histograms are traditionally fit with a one-exponential model; however, recent work has proposed a two-exponential model to account for reflector-induced phenomenon. Recent work also validated the two-exponential model for shields, a subset of reflectors, but not for reflectors in general. Ultimately, it is desirable to validate the two-exponential model for the general shield. This work will investigate if previous 3 He measurements of plutonium reflected by copper and polyethylene, and replacement measurements where the plutonium is replaced by 252 Cf are suitable for validating the new model. Since the 3 He detectors ( 3 He gas proportional counters embedded in a polyethylene matrix) inherently contain moderating/reflector material (to increase detection efficiency), this work also investigates the use of organic scintillation detectors that can directly detect fast, fission neutrons.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2012

HB-Line Anion Exchange Purification of AFS-2 Plutonium for MOX

Non-radioactive cerium (Ce) and radioactive plutonium (Pu) anion exchange column experiments using scaled HB-Line designs were performed to investigate the feasibility of using either gadolinium nitrate (Gd) or boric acid (B as H 3 BO 3 ) as a neutron poison in the H-Canyon dissolution process. Expected typical concentrations of probable impurities were tested and the removal of these impurities by a decontamination wash was measured. Impurity concentrations are compared to two specifications - designated as Column A or Column B (most restrictive) - proposed for plutonium oxide (PuO 2 ) product shipped to the Mixed Oxide (MOX) Fuel Fabrication Facility (MFFF). Use of Gd as a neutron poison requires a larger volume of wash for the proposed Column A specification. Since boron (B) has a higher proposed specification and is more easily removed by washing, it appears to be the better candidate for use in the H-Canyon dissolution process. Some difficulty was observed in achieving the Column A specification due to the limited effectiveness that the wash step has in removing the residual B after ~4 BV's wash. However a combination of the experimental 10 BV's wash results and a calculated DF from the oxalate precipitation process yields an overall DF sufficient to meet the Column A specification. For those impurities (other than B) not removed by 10 BV's of wash, the impurity is either not expected to be present in the feedstock or process, or recommendations have been provided for improvement in the analytical detection/method or validation of calculated results. In summary, boron is recommended as the appropriate neutron poison for H-Canyon dissolution and impurities are expected to meet the Column A specification limits for oxide production in HB-Line.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2013

Los Alamos National Laboratory and Lawrence Livermore National Laboratory Plutonium Sustainment Monthly Program Report, October 2012 (Revision 8)

In October of 2012 the Plutonium Sustainment program at LANL completed or addressed the following high-level activities: 1) Completed Pollux shipment to DAF in early October in accordance with the Gemini Core Team's schedule. Unpacked Pollux at DAF and supported Gemini team in various tests and inspections. Pollux test and measurement results were all acceptable. Pollux is expected to g to U1A in November. Pu Sustainment no longer has any obligations associated with the Gemini experiment. 2) Presented to Dr. Cook on the successful assembly of the Pollux experimental device as part of the Gemini series. 3) Supported the release of the FY12 Pu Sustainment Program Implementation Plan. 4) Established the FY12 program baseline and allocated funds accordingly. 5) Meetings: a. Hosted the Pu Containment 4 th Quarter Program Review; b. Hosted the Power Supply PRT; c. Traveled to KCP for the W87 Pit IPT. All four MRT L2 Milestones (4622-4625) associated with Plutonium Sustainment are on track for success in FY13.

Nuclear Physics & Radiation Physics(73)↗

DOE OSTI2013

Process Improvement: Reduce unplanned chlorine delivery shutdowns for the plutonium purification processing [Slides]

Chlorine delivery system used by MET-1 leaked in 2012 and operations were suspended. The existing chlorine gas deliver and detection system is in need of upgrade or replacement. It is reaching the end of the 25 year design life. The current system is a bench scale system that is now running on a continuous basis ~ 10 hours per day. Chlorine is used as a reagent for a number of nuclear material metal preparation and purification applications at LANL Plutonium Facility. MET-1 uses Chlorine for purification. Benefits of improving this process immediately benefit MET-1 who deals with the throughput of Plutonium on the technical and engineering side and benefits NCO-1&2 on the safety side.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

High-Precision Plutonium Isotopic Compositions Measured on Los Alamos National Laboratory’s General’s Tanks Samples: Bearing on Model Ages, Reactor Modelling, and Sources of Material. Further Discussion of Chronometry

In this study, we re-analyzed late-1940’s, Manhattan Project era Plutonium-rich sludge samples recovered from the ''General’s Tanks'' located within the nation’s oldest Plutonium processing facility, Technical Area 21. These samples were initially characterized by lower accuracy, and lower precision mass spectrometric techniques. We report here information that was previously not discernable: the two tanks contain isotopically distinct Pu not only for the major (i.e., 240 Pu, 239 Pu) but trace ( 238 Pu , 241 Pu, 242 Pu) isotopes. Revised isotopics slightly changed the calculated 241 Am- 241 Pu model ages and interpretations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

Data Mining Techniques to Estimate Plutonium, Initial Enrichment, Burnup, and Cooling Time in Spent Fuel Assemblies

The Next Generation Safeguards Initiative (NGSI), Office of Nonproliferation and Arms Control (NPAC), National Nuclear Security Administration (NNSA) of the U.S. Department of Energy (DOE) has sponsored a multi-laboratory, university, international partner collaboration to (1) detect replaced or missing pins from spent fuel assemblies (SFA) to confirm item integrity and deter diversion, (2) determine plutonium mass and related plutonium and uranium fissile mass parameters in SFAs, and (3) verify initial enrichment (IE), burnup (BU), and cooling time (CT) of facility declaration for SFAs. A wide variety of nondestructive assay (NDA) techniques were researched to achieve these goals [Veal, 2010 and Humphrey, 2012]. In addition, the project includes two related activities with facility-specific benefits: (1) determination of heat content and (2) determination of reactivity (multiplication). In this research, a subset of 11 integrated NDA techniques was researched using data mining solutions at Los Alamos National Laboratory (LANL) for their ability to achieve the above goals.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2015

Data Mining Techniques to Estimate Plutonium, Initial Enrichment, Burnup, and Cooling Time in Spent Fuel Assemblies

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2015

Measurement of Plutonium Isotopic Composition - MGA

In this module, we will use the Canberra InSpector-2000 Multichannel Analyzer with a high-purity germanium detector (HPGe) and the MGA isotopic anlysis software to assay a variety of plutonium samples. The module provides an understanding of the MGA method, its attributes and limitations. You will assess the system performance by measuring a range of materials similar to those you may assay in your work. During the final verification exercise, the results from MGA will be combined with the 240Pueff results from neutron coincidence or multiplicity counters so that measurements of the plutonium mass can be compared with the operator-declared (certified) values.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2017

NNSS Soils Monitoring: Plutonium Valley (CAU 366) FY2016

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.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

NNSS Soils Monitoring: Plutonium Valley (CAU 366) FY2017

Desert Research Institute (DRI) is conducting a field assessment of the potential for radionuclide-contaminated soil transport from the Plutonium Valley Dispersion Sites Contamination Area (CA) as a result of both wind transport and storm runoff. This activity supports U.S. Department of Energy (DOE) Environmental Management Nevada Program (EM-NV) efforts to establish post-closure monitoring plans for the Plutonium Valley Dispersion Sites Corrective Action Unit (CAU) 366. The DRI work is intended to identify the likely mechanism(s) of transport and determine the meteorological conditions that might cause the movement of radionuclide-contaminated soils. The emphasis of the work is on collecting sediment transported by channelized storm runoff and measurement of airborne dust concentrations and associated wind conditions. These data will facilitate the appropriate post-closure monitoring program.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Validation of Modified Controlled-potential coulometric assay of Plutonium

The test method for the Controlled- potential coulometric assay of plutonium used in SRNL F/H laboratories was modified in accordance to ISO 12183- Nuclear fuel technology—Controlled-potential coulometric assay of plutonium. The modifications will expand the possible drying and pre-treatment techniques which in turn will expand the type of samples that could be analyzed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2018

Innovative Plutonium Waste Forms: Acceptability to Shipp to WIPP

The mission of the Waste Isolation Pilot Plant in New Mexico is the safe and permanent disposition of transuranic radioactive waste from atomic energy defense activities of the United States. The plant consists of an underground repository in a salt formation that is free of flowing water, easily mined, impermeable, and geologically stable. The salt rock naturally seals fractures and closes openings over time. The repository is now anticipated to receive a greater amount of plutonium materials than originally envisioned. An engineered waste form for safe and efficient transport and long-term disposal of plutonium materials is an urgent need. An optimal waste form could also reduce the disposition life cycle and its associated costs to the taxpayer.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Broad Scope Analysis of the MOX Fuel Fabrication Facility and Disposition of Plutonium

The Plutonium Management and Disposition Agreement (PMDA), signed into effect in 2000, between the United States and Russia, was made in a post-Cold War effort to dispose of military-useable material, a combined 68 metric tons of weapon-grade plutonium. The United States has been pursuing a disposition path through conversion to MOX fuel for use in current commercial nuclear reactors. The Savannah River Site’s (SRS) MOX Fuel Fabrication Facility (MFFF, the MOX facility) began construction in 2007 with intent to uphold the United States’ half of the agreement. In the FY2017 budget, the Obama administration proposed a termination of the MFFF after lack of sufficient funding to the project, which caused paralyzing delays and drastically inflated costs for completion. Prolonged construction, piled costs, and divergent policies between shifting administrations have resulted in turmoil between the United States and Russia, culminating with the proposed abandonment of the MOX disposition path and being used as a justification by Russia to withdraw from the agreement until the United States is able to identify a clear plan, fulfilling the requirements set forth by the PMDA. The leading expedient to replace MOX fuel is the dilute and dispose method, which leaves uncertainty for the SRS MFFF and places reliance on New Mexico’s Waste Isolation Pilot Plant (WIPP) to legally accommodate the additional and unaccounted waste. If the current capacity of WIPP proves insufficient, construction of a new repository for transuranic waste would only incur additional costs and regulatory burdens, along with extreme schedule delays. Future proposed adaptations of the SRS MFFF include pit production, which would require complex and costly alterations to be operational at the current site. Restrictions from Congress, such as mandating the proposed solution to abandoning MFFF must equal half of the costs required for completing the facility, have fueled severely underestimated quotations of these alternatives. The increasing pressure from both Russia and South Carolina government officials to make a decision could result in the pursuit of another doomed project, leaving the United States with even further sunk costs and strained international relations. This paper will summarize the involved history of the MFFF, explicate the recourses to salvage the facility for pit production, and provide postulation on the dilute and dispose method.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Multiyear Analysis of the Fate and Transport of Contaminated Soils at Plutonium Valley and the Smoky Site, Nevada National Security Site

Desert Research Institute (DRI) has collected approximately 10 years of atmospheric and hydrologic data at Plutonium Valley and the Smoky Site on the Nevada National Security Site to identify the potential for radionuclide-contaminated soils to be transported via wind and water. Plutonium preferentially binds to finer soil particles (Shinn et al., 1993; Miller et al., 2015), which can be transported through erosion processes. Data collected by DRI are used to determine the mechanisms and thresholds that result in the transport of radionuclide-contaminated soils, and climate model projections are used to understand how these mechanisms may change in the future. This work will help identify the parameters and threshold conditions that should be incorporated into post-closure monitoring plans for these and other Soils Corrective Action Unit (CAU) sites.

54 ENVIRONMENTAL SCIENCES↗