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DOE OSTI2020

Million Worker Study

Radiation health issues have been an important aspect of DOE's Worker Safety and Health programs. The goal is to ensure that workers are adequately protected from the various radiological hazards associated with DOE sites and operations. Since the early 1940’s DOE has supported the conduct of epidemiologic studies of practically every DOE (AEC) facility and collected these data, now managed by the Oak Ridge Associated Universities (ORAU), in remarkable detail. In the early 2000s, the Office of Health, Safety and Security authorized access to specific DOE worker datasets. Shortly thereafter, the DOE Office of Science provided funds for a pilot study that confirmed the feasibility of the Million Worker Study (MWS), and then additional resources were provided (with other agencies) to extend the follow-up of many populations, not just DOE workers, but also atomic veterans, industrial radiographers, nuclear power plant workers and medical radiation workers (the Million Persons Study (MPS)). This proposal was a continuation of support provided by DOE, specifically to extend the follow-up of the worker populations at the Mallinckrodt Chemical Works (MCW) and Los Alamos National Laboratory (LANL). The work addresses DOE’s interest in clarifying the health risks of their workers as well as contributing knowledge on radiation risks that is relevant today with regard to compensation schemes. The findings are also important for the US public in light of the increased population exposure to medical imaging, environmental circumstances such as hydraulic fracturing, increased exposures during high altitude flights, and with regard to nuclear accidents such as Fukushima and possible terrorist events. Furthermore, it is important to consider reducing the uncertainty in current risk estimates by developing risk coefficients based on healthy American workers who are more representative of U.S. workers and the general public than 1945 Japanese survivors of the atomic bombs living in a war-torn country which experienced deprivation, malnourishment, and increased rates of infections and other diseases. But more importantly, it is important to learn whether radiation exposures received gradually over time (e.g., years) are more or less effective in causing health effects, cancer in particular, than if the radiation dose is received all at once in a fraction of a second as experienced by the Japanese atomic bomb survivors. Finally, the ability to evaluate and combine large populations with intakes of radionuclides such as uranium, radium, plutonium, americium and polonium will provide new quantitative knowledge on human health effects that hitherto has not been possible. This cost-efficient study has built on the investments made and foundations laid by investigators and government agencies, including DOE, over the past 30-40 years, which have established early worker cohorts that can now provide answers to questions on the lifetime human health risks associated with low-level radiation exposures. Collaborating institutions included: International Epidemiology Institute, Oak Ridge Associated Universities, Oak Ridge National Laboratory, Los Alamos National Laboratory, Landauer, Inc., and Vanderbilt University. Follow-up of these two populations and the integration of them with the many other cohorts (now a total of 31) in the MPS continues under a separate DOE grant (DE-AU0000046).

61 RADIATION PROTECTION AND DOSIMETRY↗

DOE OSTI2024

Experimental Investigations into the Corrosion of Alloy 625 Using NaCl-PuCl3 Molten Salt in a Natural Circulation Microloop

Molten salt reactors (MSRs) can potentially revolutionize the nuclear industry by providing a path to a near-zero nuclear waste fuel cycle, contributing to more sustainable energy sources. As a plethora of MSR developers in the United States work toward an aggressive commercialization timeline, many of their fueled-salts—notably, chloride-based compositions—have limited operational testing with nuclear material. Licensing and operating these reactors require an understanding of corrosion effects on reactor materials of construction under operational conditions. The TerraPower Molten Chloride Fast Reactor (MCFR) is a liquid-fueled chloride-salt fast reactor which has received notable interest from the utility sector based on its desirable economic characteristics. The reactor operates at low pressure but does not require the use of highly reactive chemicals, leading to a reduced use of concrete and steel during construction. Additionally, liquid fuel allows for inherently stable behavior and natural circulation during a loss-of-site-power scenario. MCFR can be refueled while operating which makes it compatible with variable generation sources such as wind and solar. MCFR is a breed-and-burn in-situ reactor that does not implement any chemical processing or separations in the fuel cycle. Only mechanical filtration of noble metals and off-gassing of noble gases are utilized while the actinides stay mixed with the fuel at all times. The MCFR will require technology development to reach commercialization. With a breed-and-burn in-situ reactor like MCFR, the transmutation of fertile U-238 to fissile Pu-239 allows for much greater fuel utilization.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Critical and Californium Source-Driven Noise Analysis Subcritical Measurements with an Unreflected Cylindrical Tank of Mixed Uranium-Plutonium Nitrate Solution

The reported experiments were performed by Oak Ridge National Laboratory (ORNL) at the Battelle Northwest Laboratory’s (now Pacific Northwest National Laboratory) critical experiments facility at Hanford, Washington in 1981 and used 16 days of critical facility time, not including 10 days for setup and removal of ORNL equipment. These measurements were to assess the capability of the Cf source-driven noise analysis (CSDNA) method to measure the subcriticality (keff) of mixed U-Pu nitrate solutions. In addition to the CSNDA measurements, measurements were also performed near delayed criticality where CSDNA measurements cannot be performed. This report documents the experiments that were not reported at that time by presenting the ORNL experimental results and any online analysis performed during and shortly after the measurements. The mixed nitrate solution had a U concentration at 188 grams per liter (g/L), a Pu concentration of 280 g/L, free acid normality of 2.80, H ion molarity of 5.9 and a specific gravity of 1.754 g/cm 3 , a 240 Pu isotopic content of 7.981 wt. %, and a 235 U isotopic content of 0.724 wt. %. The stainless-steel tank for the solution had an inside diameter of 35.38 cm, an outside diameter of 35.53 cm, a height of 56.72 cm, and bottom thickness of 0.9525 cm. A Zircaloy pipe with a 3.1496 cm outside diameter, a 2.7788 cm inside diameter, and bottom thickness of 0.635 cm was available for insertion of the Cf source in the center of the fissile solution. The Cf source was also located at the outside surface of the tank (solution height varied from 10 to 53 cm) and in the center of the solution (solution height varied from 10 to 60.7 cm). The CSDNA measurements were not analyzed online to determine the subcritical neutron multiplication factors. At all subcritical states, the break frequency noise analysis data was fitted to obtain the prompt neutron decay constant. The neutron multiplication factors were determined for the two configurations of the measurements near delayed criticality. The subcritical neutron multiplication factors from the CNSDA measurements can be obtained with further analysis. However, the near delayed critical configuration, the prompt neutron decay constants, the count rates, and the measured cross and auto power spectral densities can be calculated directly for benchmarking. Much of data presented in this report are from ORNL notes—not in the ORNL logbooks. For the final benchmark analysis, the data from the Battelle Northwest Laboratory (which operated the critical facility in 1981) critical facility logbook should be consulted and be incorporated where appropriate. The purpose of this report is to document the experimental information for the measurements performed so that at a later date researchers could perform the required uncertainty and calculational analyses and documentation to use these data for an International Criticality Safety Benchmark Program (ICSBEP) or Nuclear Energy Agency benchmark. The data from these measurements are available from the ORNL Records Management Services Department, and the logbook is available from ICSBEP at Idaho National Laboratory. Preparation of the present report is part of a larger cooperative effort between Idaho National Laboratory (INL) and Oak Ridge National Laboratory (ORNL) to document more than 15 undocumented critical and subcritical experiments enumerated in ORNL/TM-2019/18 and performed by ORNL at ORCEF and other USDOE critical experiments facilities using more than 500 operational days of critical facility time.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Nuclide inventory characterization of EBR-II MOX fuel test pins

Characterization of 3 mixed oxide (MOX) fuel pins from the Experimental Breeder Reactor II (EBR-II) SPA-2/-2B experiment program was performed in support of the Advanced Reactor Experiments for Sodium Fast Reactor Fuels (ARES) joint project between Idaho National Laboratory (INL) and the Japan Atomic Energy Agency (JAEA). The characterization efforts were performed to enable transient testing in the Transient Reactor Test (TREAT) facility at INL and will include post irradiation examination (PIE) and other analyses. MOX fuel pins UW02009, 02011, and 06024 were historically irradiated from 1989 to 1994 for a total of 822.42 effective full power days (EFPDs) and peak burnup of approximately 14.3 at.% (atomic percent of heavy metal atoms, ∼134.4 GWd/t). They had since been placed in storage until a future use was identified. Characterization of the fission products and activation of each fuel pin was necessary to enable removal from storage and subsequent irradiation testing or PIE activities. The initial fuel pin geometry and composition were established using historical documentation. Irradiation history details were utilized to compute irradiated and decayed fuel pin masses, atomic densities, and activities. A pellet-wise axial neutron flux was also computed to assist in evaluation of the axial distribution of {sup 235}U and {sup 239}Pu, per pellet, within each of the test fuel pins. The results computed herein supported experiment design for advanced high-burnup MOX fuel designs under slow transient overpower (MOXTOP) conditions, which was Phase I of the ARES project. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2022

Recent 238 Pu Production Activities at Idaho National Laboratory

The Plutonium-238 ( 238 Pu) Production program at Idaho National Laboratory (INL) is actively qualifying irradiation targets containing 237 Np for the Advanced Test Reactor (ATR) to produce 238 Pu for future National Aeronautics and Space Administration missions. INL qualified and loaded seven targets in the ATR’s south flux trap for cycle 169A, which occurred in Spring 2021. The irradiation qualification program has expanded to additional ATR irradiation positions after two baseline production targets in three positions validated significant production of 238 Pu. The validation model was followed by the PFS-1 experimental test in the ATR Critical Facility that verified 238 Pu production cross sections. This paper outlines the progress and status of the 238 Pu production program at INL. The qualification effort, safety analysis, hardware status, and future activities for qualification of an updated target design for use in the ATR are discussed.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2021

Effects of 18 O Exchange on Neutron Emission Rates of Aging 238 PuO 2 LWRHUs

The Lightweight Radioisotope Heater Unit (LWRHU) provides about 1 Watt of thermal power to critical electrical and mechanical systems in the extreme temperatures of space, maintaining the operating temperature of the spacecraft’s scientific and general operating equipment. Los Alamos National Laboratory (LANL) designed and tested the LWRHU in the 1970s through early 1980s. The first production campaign at LANL was in the early 1980s in support of the Galileo mission in which over 100 LWRHUs were manufactured. In the mid-1990s, almost 200 LWRHUs were manufactured in support of the Cassini mission. After the primary Cassini manufacturing campaign, the Department of Energy (DOE) approved the fabrication of more than 10 additional LWRHUs as spares in 1998. The LWRHU assembly contains the following components: a fuel pellet, a vented capsule, a pyrolytic graphite insulator, and a fine-weave pierced fabric (FWPF) graphite aeroshell. The fuel pellet is a hot-pressed 238 PuO 2 cylindrical pellet that is sintered to create a ceramic pellet. The pellet is encapsulated in a platinum-rhodium encapsulation. The welded fueled clad is placed inside a pyrolytic graphite thermal insulation to protect the fuel from the heat produced in reentry events. The exterior layer of the LWRHU assembly is the FWPF aeroshell. Before sintering, PuO 2 granules are heated in a furnace at temperatures greater than or equal to 700°C under an enriched 16 O atmosphere in order to reduce trace quantities of 18 O. Because 18 O undergoes an (α,n) reaction, 18 O needs to be removed as much as possible to meet radiation emission requirements set by the Jet Propulsion Laboratory (JPL) and the National Aeronautics and Space Administration (NASA), as well as other agencies. The relative abundances of the oxygen isotopes are indicated by neutron emission rate (NER) measurements. LWRHUs are vented with a sintered platinum frit vent (George 1986). During extraterrestrial operation, the vent in the cladding allows helium from the decay of plutonium to escape and relieves pressure from the system while preventing the solids from escaping (Rinehart 1996, Tate 1982 & 1985). This vent is protected during manufacture by a platinum-30 rhodium cover. The capsule vent is activated by milling a 0.025-inch diameter hole through the protective cover to a nominal depth of 0.015 inches, generally immediately before the LWRHU is loaded into the aeroshell (George 1986). Prior to long-term storage, LWRHUs are vented and thus potentially allow infiltration of 18 O from the ambient atmosphere. Although NER decreases with age due to the reduction in emitted alpha particles, it might be expected that NER reduction is mitigated by the exchange of 18 O. However, this is not necessarily the case and no trend was observed relating NER to age other than the natural decay of 238 Pu (Mulford 2021). The most probable and dominant factor for determining specific NER was manufacturing discrepancies between individual units. It is important to understand the lack of observed 16 O- 18 O exchange and to compare LWRHU pellets as much as possible.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

25-Pin metallic fuel performance benchmark case based on the EBR-II X430 experiments series

A metallic fuel benchmark case was developed for the fuel performance code BISON based on 25 uranium-zirconium and uranium-plutonium-zirconium pins of the Experimental Breeder Reactor II X430 experiment series. Results of the benchmarks were compared with measurements and calculations made at the time of the experiment as well as subsequent measurements reported in 2019. The comparisons were used to quantify the accuracy of the BISON predictions and to identify patterns in the BISON differences.BISON predicted burnup, plenum pressure, and fission gas release fractions accurately. BISON temperature predictions were somewhat cooler than the temperatures determined at the time of the experiment but appeared to be reasonably accurate considering uncertainties in the legacy temperature calculations, uncertainties in the legacy linear heat rate calculations, and the high sensitivities of the BISON-predicted temperatures to BISON inputs. Fuel axial elongation predictions had errors correlated to fuel composition; BISON tended to underpredict the elongation of binary fuels and overpredict the elongation of ternary fuels. BISON cladding radial dilation predictions were also significantly lower than legacy PIE measurements.Recommendations were made to improve the BISON fuel gaseous swelling model to account for fuel composition, to add additional capabilities to the coolant channel temperature model to ease benchmark development, and to continue developing benchmark cases based on a wide range of experiments in several reactors. Once a wide array of benchmarks is developed, an attempt can be made to enhance or calibrate BISON models to improve the cladding dilation predictions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Automated Inspection of Criticality Control Overpacks for Surplus Plutonium Disposition: Qualification Update – 25313

In an effort to reduce the amount of nuclear waste in South Carolina, the Department of Energy (DOE) tasked the Savannah River Site (SRS) with diluting and disposing of the amount of plutonium in the state. This process involves the movement and shipment of over 100,000 criticality control overpacks (CCOs) throughout the project lifespan, lending itself to the use of automation to reduce worker radiation exposure and more efficiently utilize human capital. Due to the large scope, this overarching process was broken down into several different “automation projects” to be developed. The first opportunity pursued was the receipt and inspection of empty CCO drums coming into SRS, identified as Automation Project 1 (AP1), and is the focus of this paper. AP1 was developed to unpack incoming CCOs and inspect them for unwanted foreign objects and any damage to the drum or its contents. This process is accomplished by the combination of an automated guided vehicle (AGV) that delivers CCOs to a robotic arm which uses a suite of custom tools to disassemble a CCO, inspect the inside and outside of the CCO and its inner criticality control container (CCC), reassemble the CCC and CCO, and apply a tamper indicating device (TID) to the inspected drum. In past years, the robotic work cell had been developed in a small-scale testing facility for proof-of-concept. This year, major improvements were made to the robotic work cell to perform the process, including integration into the final facility where CCOs will be inspected. Other technical improvements include the implementation of sensor feedback and safety relays into the control system to allow the state of the work cell to be better tracked, and additional development of the TID application process to complete the robotic inspection. Further enhancements were made to the robotic vision processes and robot pathing, as well as development on a computer vision inspection process to detect inspection criteria anomalies in CCOs. In addition to developmental improvements, the work cell underwent a six-month testing period to ensure the project requirements were met. Results of this testing period demonstrate the work cell’s capability to meet project throughput goals at an acceptable level, successfully document the status of each CCO inspected, and reduce the toll on technical operations’ human power by two thirds. At the time of this paper, the work cell is capable of autonomously handling up to eight CCOs with an AGV, delivering CCOs to and from the robot work cell, and having a robotic arm perform a full receipt and inspection procedure on each CCO. Moving forward, repeatability will be improved so that these CCOs can be run back-to-back seamlessly, as well as improving the system to handle more significant edge cases and failure modes.

Spivey, Nicholas↗

DOE OSTI2025

Advanced Computational Modeling of High-Level Waste Vitrification at the Hanford Site

The U.S. Department of Energy (DOE) has selected vitrification for stabilizing legacy tank waste at the Hanford site, where radioactive waste from plutonium production was historically stored in underground tanks. This waste will be separated into low-activity waste (LAW) and high-level waste (HLW) fractions and processed at the Waste Treatment and Immobilization Plant (WTP). At WTP, glass melters are used for the vitrification of radioactive tank waste, transforming it into a stable borosilicate glass form for safe long-term storage. The melter vessel is constructed from highly durable and heat-resistant materials, where the vitrification process occurs. The main regions that are modeled are the melt pool, plenum, cold cap, riser/discharge chamber, and surrounding structure with insulation layers. Forced convection induced by air bubblers at the base of the melter ensure uniform temperature distribution and provide heat to the cold cap layer. The cold cap is a region of reacting batch feed that floats on top of the molten glass and is where the batch-to-glass reactions occur. Joule heating provided by electrodes mounted along the vertical walls of the melter and immersed directly in the glass, generates the necessary heat for the net endothermic conversion processes that occur in the cold cap. The high temperatures, radioactivity, and opaque nature of the glass prevent direct observation inside the melters. Therefore, computational models are essential for providing insight into factors that affect melter throughput. Thermocouples in the plenum provide operators with plenum temperature measurements. Operational adjustments include bubbling rate, voltage supplied to the electrodes, feed adjustments, and glass removal rate. Different computational fluid dynamics (CFD) models have been developed, each serving a specific purpose. There are CFD models of different scale melters, as well as models that capture the two-phase flow interfaces of rising bubbles in the molten glass or models with a simplified molten glass region so that the surrounding structure and plenum can be feasibly incorporated. Pilot-scale melter models have been developed to serve as validation of the methods employed in the simulation of the full-scale WTP melters. Models incorporating resolved bubbling are used to develop momentum source terms to implement into a single phase, multi-region, steady-state flow model that is being validated by measured process parameters such as glass production rate, voltage, input power, plenum temperatures, etc. The resolved bubbling model uses the multiphase volume of fluid approach to model the system with a high-resolution interface capturing scheme to maintain sharp interfaces between the molten glass and the air phase. The suite of CFD models is continually being improved to incorporate more realistic physics and achieve faster turnaround time. For example, an incremental controller is implemented to automatically adjust electrode voltage within the simulation to a molten glass set point temperature of 1150°C. Newer models feature improved meshes to ensure conformal meshes between regions and eliminate unnecessary mesh refinement in areas that are not of interest (such as boundary layers in offgas ports). Instead of explicitly modeling the structural, refractory, and insulation layers of the melter, a thermal resistance approach is used with published correlations used for boundary conditions. The development of robust and efficient CFD models will be instrumental in enabling the WTP to successfully fulfill its mission of safely stabilizing legacy nuclear waste.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗