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At least 541 records · Page 30

NESHAPs CY19 Report: Radionuclide Air Emission Report for 2019

Lawrence Livermore National Security, LLC operates facilities at Lawrence Livermore National Laboratory (LLNL) in which radionuclides are handled and stored. These facilities are subject to the U.S. Environmental Protection Agency (EPA) National Emission Standards for Hazardous Air Pollutants (NESHAPs) in Code of Federal Regulations (CFR) Title 40, Part 61, Subpart H, which regulates radionuclide emissions to air from Department of Energy (DOE) facilities. Specifically, NESHAPs limits the emission of radionuclides to the ambient air to levels resulting in an annual effective dose equivalent of 10 mrem (100 μSv) to any member of the public. Using measured and calculated emissions, and building-specific and common parameters, LLNL personnel applied the EPA-approved computer code, CAP88-PC, Version 4.0.1.17, to calculate the dose to the maximally exposed individual member of the public for the Livermore Site and Site 300. In 2019, LLNL maintained its compliance with 40 CFR 61, Subpart H. All radioactive air emissions resulted in calculated doses far below the annual 10 mrem (100 μSv) sitewide standard. The annual doses to the site-wide maximally exposed individual member of the public at the Livermore Site and Site 300 from planned and unplanned operations in 2019 are: Livermore Site: 4.3 x 10⁻³ mrem (4.3 x 10⁻² μSv); Site 300: 9.5 x 10⁻⁸ mrem (9.5 x 10⁻⁷ μSv).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

AGR-2 Loose Particle Heating Tests in the Furnace for Irradiated TRISO Testing

A furnace system was developed to thermally expose individual tristructural-isotropic (TRISO) coated particles to expand upon established postirradiation examination (PIE) safety testing that is used to explore particle failures and fission product release from compacts. Two systems were installed in the Irradiated Fuels Examination Facility (IFEL) at Oak Ridge National Laboratory (ORNL). The targeted design was intended to be simple and flexible to allow a range in conditions to be explored. Initial inert atmosphere testing indicated the presence of particle failures, so modifications to the testing approach were implemented to improve the furnace operation. Ultimately, burnback particles were analyzed to provide a direct measurement of fission product release, thus avoiding the complications from integral release that were observed during whole compact testing. Particles were exposed to temperatures ranging 1,150–1,300°C for up to 1,500 h and 1,600°C up to 500 h. No indication of uniform release of fission products such as 106 Ru, 125 Sb, or 154 Eu was observed, however, indication of particle dependent 154 Eu release was suggested for select particles. Exploration of 110m Ag release was limited to 1,150°C and 1,300°C up to 500 h. The analysis indicated that there was nonuniform release of 110m Ag and supports a possible bimodal temperature dependence on silver release.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Highly-Active and Contaminant-Tolerant Cathodes for Durable Solid Oxide Fuel Cells

The objective of this project is to investigate the fundamental degradation methods occurring in solid oxide fuel cell (SOFC) cathodes when exposed to chromium and carbon dioxide contamination and to rationally design alkaline earth-based catalysts to increase stability and tolerance to contaminate poisoning. With a mechanistic and fundamental understanding of the degradation methods, advanced catalytic surface modifications can be applied to reduce degradation. The specific technical objectives are: (1) To identify/develop new catalysts (alkaline-earth based-) that are compatible chemically with the state-of-the-art cathode materials at high temperatures required for fabrication and with contaminates commonly encountered under operating conditions; (2) To improve the infiltration process for optimal control of the thickness, composition, and uniformity of the catalyst coatings; (3) To evaluate the electro-catalytic activity toward ORR of the chemically-stable materials when exposed to different types of contaminants using electrical conductivity relaxation measurements on bar samples and performance evaluation of catalyst-infiltrated cathodes; (4) To unravel the contamination-tolerant mechanisms of the new catalyst coatings under realistic environmental conditions (with different types of contaminants) using powerful in situ and in operando characterization techniques performed on model cells with thin-film/pattern electrodes, as guided by modeling and simulation; (5) To establish scientific basis for rational design of new catalysts of high tolerance to contaminants; (6) To validate the long term stability of modified LSCF cathodes in commercially available cells/stacks under ROC. Alkaline earth-based catalysts have been systematically explored and tested under various contamination conditions. BaCoO 3-δ (BCO) was shown to produce the best catalytic activity enhancement as well as stability in a variety of contaminating conditions, including CO 2 and chromium. The microstructural evolution was investigated with SEM, EDS, and Raman spectroscopy, showing the BCO catalyst prevents the formation of insulating SrCrO 4 by forming electrically conductive BaCrO 4 . Electrochemical relaxation measurements determined the BCO catalyst coatings increased the surface diffusion coefficient but did not significantly affect the diffusion coefficient and determined an optimum surface modification layer of 100 nm. A novel Ba 0.9 Co 0.7 Fe 0.2 Nb 0.1 O x (BCFN) catalyst was also shown to have excellent stability in chromium containing atmospheres. A novel surface sol-gel (SSG) surface modification, which offers superior thickness and compositional control, was applied to SOFCs to produce BaO catalyst coatings. SSG BaO coatings were shown to produce conformal coatings on the electrode surface, greatly4 increasing stability in chromium containing atmospheres. An atomic level mechanistic approach was applied to investigate the stability of PrBa 0.8 Ca 0.2 Co 2 O 5+δ (PBCC) with respect to a variety of common contaminants, demonstrating thermodynamically its superior stability in CO 2 containing atmospheres. Finally, the best catalyst coatings demonstrated in this project, BCO and PBCC, were applied to full cells which demonstrated superior stability for over 300 hours in CO 2 and Cr atmospheres.

30 DIRECT ENERGY CONVERSION↗

Highly-Active and Contaminant-Tolerant Cathodes for Durable Solid Oxide Fuel Cells

The objective of this project is to investigate the fundamental degradation methods occurring in solid oxide fuel cell (SOFC) cathodes when exposed to chromium and carbon dioxide contamination and to rationally design alkaline earth-based catalysts to increase stability and tolerance to contaminate poisoning. With a mechanistic and fundamental understanding of the degradation methods, advanced catalytic surface modifications can be applied to reduce degradation. The specific technical objectives are: (1) To identify/develop new catalysts (alkaline-earth based-) that are compatible chemically with the state-of-the-art cathode materials at high temperatures required for fabrication and with contaminates commonly encountered under operating conditions; (2) To improve the infiltration process for optimal control of the thickness, composition, and uniformity of the catalyst coatings; (3) To evaluate the electro-catalytic activity toward ORR of the chemically-stable materials when exposed to different types of contaminants using electrical conductivity relaxation measurements on bar samples and performance evaluation of catalyst-infiltrated cathodes; (4) To unravel the contamination-tolerant mechanisms of the new catalyst coatings under realistic environmental conditions (with different types of contaminants) using powerful in situ and in operando characterization techniques performed on model cells with thin-film/pattern electrodes, as guided by modeling and simulation; (5) To establish scientific basis for rational design of new catalysts of high tolerance to contaminants; (6) To validate the long term stability of modified LSCF cathodes in commercially available cells/stacks under ROC. Alkaline earth-based catalysts have been systematically explored and tested under various contamination conditions. BaCoO 3-δ (BCO) was shown to produce the best catalytic activity enhancement as well as stability in a variety of contaminating conditions, including CO 2 and chromium. The microstructural evolution was investigated with SEM, EDS, and Raman spectroscopy, showing the BCO catalyst prevents the formation of insulating SrCrO 4 by forming electrically conductive BaCrO 4 . Electrochemical relaxation measurements determined the BCO catalyst coatings increased the surface diffusion coefficient but did not significantly affect the diffusion coefficient and determined an optimum surface modification layer of 100 nm. A novel Ba 0.9 Co 0.7 Fe 0.2 Nb 0.1 O x (BCFN) catalyst was also shown to have excellent stability in chromium containing atmospheres. A novel surface sol-gel (SSG) surface modification, which offers superior thickness and compositional control, was applied to SOFCs to produce BaO catalyst coatings. SSG BaO coatings were shown to produce conformal coatings on the electrode surface, greatly 4 increasing stability in chromium containing atmospheres. An atomic level mechanistic approach was applied to investigate the stability of PrBa 0.8 Ca 0.2 Co 2 O 5+δ (PBCC) with respect to a variety of common contaminants, demonstrating thermodynamically its superior stability in CO 2 containing atmospheres. Finally, the best catalyst coatings demonstrated in this project, BCO and PBCC, were applied to full cells which demonstrated superior stability for over 300 hours in CO 2 and Cr atmospheres

01 COAL, LIGNITE, AND PEAT↗

PDRD Project 19039 - All metal vacuum scroll pump development for tritium

Currently the United States relies on a single source, foreign company, Eumeca (formerly Normetex) for the supply of an all metal vacuum scroll pump to process tritium. This “one of a kind”, all metal, vacuum scroll pump utilizes no “wetted”, polymeric materials that degrade prematurely when exposed to tritium. U.S. based vacuum scroll pump suppliers typically utilize a polymer, Teflon®, as a tip seal material at the edge of the scroll impellers for proper pump function. Teflon® is known to degrade within a relatively short time frame (approximately 1 year) when continually exposed to tritium gas. This degradation results in “flaking” of the Teflon® material which results in particulate contamination of the process gas stream. While filtration of the particulate is possible, doing so requires additional maintenance which is costly in a glovebox environment. In addition, filtration can degrade pumping system performance as particulate collects in the filter media over time. To date, all of the well established U.S and European based vacuum scroll pump manufacturers have been uninterested in developing an all metal vacuum scroll pump that does not use a polymeric scroll tip seal. This position is taken as the vacuum scroll pump manufacturers do not see a large enough market to make it profitable for them to develop and market an all metal vacuum scroll pump. In the mid 2000s, one company, Air Squared, Inc., a small Original Equipment Manufacturer (OEM) specializing in design and fabrication of custom scroll vacuum pumps and compressors, was willing to pursue the effort. The first design effort incorporated Vespel® as a polymeric tip seal material. Results of this effort led to realizing the affect that the Met-Bel MB-601 metal bellows pump has on performance when used as a backing pump for an all metal vacuum scroll pump without a scroll tip seal. As a result, Air Squared subsequently designed an all metal vacuum scroll pump without a tip seal material for evaluation. Although the initial, all metal version of the Air Squared pump was found deficient in regard to scroll impeller stiffness, which resulted in scroll contact, general design and pump performance was verified to be adequate. SRS PDRD Project 19039 was launched in 2019 as a 3rd attempt with Air Squared, Inc. in regard to development of an all metal vacuum scroll pump for consideration as an equivalent to the Eumeca/ Normetex pump. The effort specified 300 series stainless steel for the scroll impellers, all metal sealing, and design to meet tritium throughput and ultimate vacuum requirements. In addition, a 60 psig design pressure rating requirement was specified for the pump containment boundary. The 3rd generation Air Squared pump has been designed, fabricated, and has received preliminary testing. Preliminary testing has indicated proper leak tightness and pump performance. However, work continues regarding development of a pumping chamber containment bellows that can be subjected to 66 psig without damage to the bellows. Work will continue in 2020 and 2021 to pursue a pumping chamber containment bellows that meets the pressure rating requirement.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Multi-Element Water Content System Instrument Handbook

The SEA Model WCM-2000 multi-element water content system was designed to provide aircraft and wind tunnel users with a single, rugged sensor to simultaneously measure liquid water content (LWC), total water content (TWC), and ice water content (IWC). The instrument consists of four heated stainless steel elements, each with a different shape or size. Each element is directly heated by low-voltage DC current flowing through the element. These elements are maintained at a constant temperature, typically 140°C, by a digital closed-loop control system. Three of the heated elements are exposed directly to the airstream and incoming cloud water. A fourth element, the reference/comp element, is arranged to be exposed to the airflow but not to incoming cloud water. This element is used to establish the “dry power term” that is subtracted from the other three elements’ power readings to establish the measured water content.

54 ENVIRONMENTAL SCIENCES↗

HEAF Cable Fragility Testing at the Solar Furnace at the NSTTF

In order to establish a zone of influence (ZOI) due to a high energy arcing fault (HEAF) environment, the fragility of the targets must be determined. The high heat flux/short duration exposure of a HEAF is considerably different than that of a traditional hydrocarbon fire, which previous research has addressed. The previous failure metrics (e.g., internal jacket temperature of a cable exposed to a fire) were based on low heat flux/long duration exposures. Because of this, evaluation of different physics and failure modes was considered to evaluate the fragility of cables exposed to a HEAF. Tests on cable targets were performed at high heat flux/short duration exposures to gain insight on the relevant physics and failure modes. These tests yielded data on several relevant failure modes, including electrical failure and sustained ignition. Additionally, the results indicated a relationship between the total energy of exposure and the damage state of the cable target. This data can be used to inform the fragility of the targets.

42 ENGINEERING↗

Study of the niobium oxide structure and microscopic effect of plasma processing on the Nb surface

A study of the niobium oxide structure is presented here, focusing on the niobium suboxides. Multiple steps of argon sputtering and XPS measurements were carried out until the metal surface was exposed. Subsequently, the sample was exposed to air for different time intervals and the oxide regrowth was studied. In addition, three Nb samples prepared with different surface treatments were studied before and after being subjected to plasma processing. The scope is investigating the microscopic effect that the reactive oxygen contained in the glow discharge may have on the niobium surface. This study suggests that the Nb 2 O 5 thickness may increase. Nevertheless, since the Nb 2 O 5 is dielectric, its thickening would not negatively affect the cavity performance.

36 MATERIALS SCIENCE↗

Study of the Niobium Oxide Structure and Microscopic Effect of Plasma Processing on the Nb Surface

A study of the niobium oxide structure is presented here, focusing on the niobium suboxides. Multiple steps of argon sputtering and XPS measurements were carried out until the metal surface was exposed. Subsequently, the sample was exposed to air for different time intervals and the oxide regrowth was studied. In addition, three Nb samples prepared with different surface treatments were studied before and after being subjected to plasma processing. The scope is investigating the microscopic effect that the reactive oxygen contained in the glow discharge may have on the niobium surface. This study suggests that the Nb 2 O 5 thickness may increase. Nevertheless, since the Nb 2 O 5 is dielectric, its thickening would not negatively affect the cavity performance.

36 MATERIALS SCIENCE↗

Smart Ventilation Controls for Occupancy and Auxiliary Fan Use Across U.S. Climates

Smart Ventilation has been developed as a way to reduce the energy associated with ventilation by changing when ventilation happens and how much ventilation occurs at any given time. In high performance buildings with low envelope and appliance related loads, ventilation is becoming a bigger part of the total building energy use and needs to be addressed if performance targets are to be met. This work explores the development and performance of smart ventilation controls based on occupancy and auxiliary fan operation that provide annual dwelling unit ventilation equivalence to ASHRAE Standard 62.2-2016. A prototype high performance home compliant with U.S. DOE Building America Zero Energy Ready program requirements was simulated using the REGCAP tool with and without smart controls across 15 U.S. DOE climate zones. Balanced and unbalanced IAQ fans were independently simulated, and all smart controlled fans had airflows double the reference 62.2-2016 airflow. Three idealized occupancy patterns were examined: 1st shift (a typical daily work/school absence), an extended 1st shift with more time spent out of the home evenings and weekends and 3rd shift (night work). The Occupancy controller turns the IAQ fan off during unoccupied periods, and it resumes ventilation upon their return. While unoccupied, contaminants are allowed to accumulate in the space, because occupants are not exposed to these contaminants. When occupants return home, they are exposed to these higher contaminant concentrations, and the controller increases the ventilation rate sufficiently to ensure equivalence with a continuous IAQ fan. Accounting for pollutant emissions that occur during unoccupied periods (as required by ASHRAE 62.2-2016), sharply distinguishes our occupancy controls from past Demand Controlled Ventilation systems. This new accounting method results in equivalent contaminant exposure, as well as lower reductions in average ventilation rates and lower energy savings. Smart controls were demonstrated that saved HVAC energy (i.e., avoided heating/cooling load, as well as fan energy)—averaging between 6 and 46% of ventilation-related energy use depending on the control strategy and occupancy pattern assumptions. The greatest savings were in the combined Auxiliary Fan + Occupancy control. Energy savings increased with climate heating demand and longer unoccupied time periods. The 3rd shift occupancy pattern had better performance, due to the thermal benefit of reducing the ventilation rate during the cold nighttime hours. This same effect provided a cooling energy benefit in hotter locations for the 1st shift. Overall, savings from occupancy-based smart controls were low, because of the recovery period required after occupants return home, during which the airflow is double the 62.2 reference. This recovery is required to maintain equivalence with the ASHRAE standard. Occupancy-based control performance was improved when combined with sensing auxiliary fans and when providing a pre-occupancy flush out of one- or two-hours. Performance was similarly improved if the ASHRAE Standard were to recognize that pollutant emissions are lower during unoccupied periods, iii allowing a lower target ventilation rate during unoccupied periods (not currently in the standard) (see Full vs. Half AEQ in this report). Finally, over-sized unbalanced fans that are cycled on-and-off by a smart controller (or timer) were found to substantially increase annual average air exchange and energy use relative to a continuous unbalanced fan due to the effects of superposition with natural infiltration.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Sister Rod Destructive Examinations (FY2021) Appendix J: Leaching of High Burnup Used Nuclear Fuel in De-ionized Water

As a part of the DOE NE High Burnup Spent Fuel Data Project, Oak Ridge National Laboratory (ORNL) is performing destructive examinations (DEs) of high burnup (HBU) (>45 GWd/MTU) spent nuclear fuel (SNF) rods from the North Anna Nuclear Power Station operated by Dominion Energy. The SNF rods, called sister rods or sibling rods, are all HBU and include four different kinds of fuel rod cladding: standard Zircaloy-4 (Zirc-4), low-tin Zirc-4, ZIRLO, and M5. The leaching experiment was a part of a larger study by Yadukrishnan Sasikumar in defending his doctoral thesis at The Open University, School of Engineering and Innovation [13]. It utilized post-CIRFT Sister Rod test specimens that were slated for disposal. The leaching experiment aims to understand the trends in the radiolytic dissolution of High Burnup Spent Nuclear Fuel (SNF) when exposed to water (e.g., in-reactor or in-pool cladding failures). Specimens from a baseline M5-clad rod and a heat-treated M5 rod were cut from the fractured CIRFT specimens and placed in 100 mL de-ionized water for a period of 128 days. Both radial and axial sections were cut to provide different surface areas of fuel in contact with the leachate. During the four-month exposure period, aliquot samples of the leachate were analyzed gamma spectroscopy and inductively coupled plasma mass spectrometry (ICP-MS). The analysis quantified the amount of fuel leached into the solutions and provided individual isotopic release fractions (of 30+ isotopes) which were compared as a function of time and surface area of fuel exposed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

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.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Capturing Carbonation: Understanding Kinetic Complexities through a New Era of Electron Microscopy

Cryogenic plasma focused ion beam (PFIB) electron microscopy analysis is applied to visualizing ex situ (surface industrial) and in situ (subsurface geologic) carbonation products, to advance understanding of carbonation kinetics. Ex situ carbonation is investigated using NIST fly ash standard #2689 exposed to aqueous sodium bicarbonate solutions for brief periods of time. In situ carbonation pathways are investigated using volcanic flood basalt samples from Schaef et al. (2010) exposed to aqueous CO 2 solutions by them. The fly ash reaction products at room temperature show small amounts of incipient carbonation, with calcite apparently forming via surface nucleation. Reaction products at 75° C show beginning stages of an iron carbonate phase, e.g., siderite or ankerite, common phases in subsurface carbon sequestration environments. This may suggest an alternative to calcite in carbonation low calcium-bearing fly ashes. Flood basalt carbonation reactions show distinct zonation with high calcium and calcium-magnesium bearing zones alternating with high iron-bearing zones. The calcium-magnesium zones are notable with occurrence of localized pore space. Oscillatory zoning in carbonate minerals is distinctly associated with far-from-equilibrium conditions where local chemical environments fluctuate via a coupling of reaction with transport. The high porosity zones may reflect a precursor phase (e.g., aragonite) with higher molar volume that then “ripens” to the high-Mg calcite phase-plus-porosity. These observations reveal that carbonation can proceed with evolving local chemical environments, formation and disappearance of metastable phases, and evolving reactive surface areas. Together this work shows that future application of cryo-PFIB in carbonation studies would provide advanced understanding of kinetic mechanisms for optimizing industrial-scale and commercial-scale applications.

36 MATERIALS SCIENCE↗

LANL PVC bag-out-bag replacement [Slides]

The US material at 8 months aging, at room temperature and exposed to gamma at 80 degrees C has been completed. The FTIR data does not show any discernible difference between the US APU-ether material and the British material. There are some differences and the curves of the FTIR, but the behavior shows that the US material is behaving comparable to the British material. The British Blue sample exposed to gamma at 70 degrees C did have an observable change in the contact angle. This was the only notable change between the two different types of polymer the TGA on both the US and the British had no observable difference. Mechanical testing samples (dog-bones) are being prepared for tensile, shear, and puncture testing. This data will be provided in later meetings. Mass spec testing is needed to measure the headspace gases that are being seen during the aging study to better health characterize the radiolytic degradation of the APU ether samples, this is also ongoing.

36 MATERIALS SCIENCE↗

Specifications of EBR-II Neutron Radiography Method Description and Digitization Approach

All neutron radiography (NRAD) images of fuel pins in Argonne’s collection were originally generated using the NRAD imaging facility established in the Hot Fuel Examination Facility (HFEF) at Idaho National Laboratory (INL). The NRAD reactor facility was built in 1977 and has been operating since. The reactor is a TRIGA-type reactor operating at a power level of 250 kWth to provide a neutron source for radiography imaging. The reactor is equipped with two beam tubes (i.e., east beam tube and north beam tube) to guide the neutron beams to two radiography stations. The east radiography station is directly under the HFEF main cell and is dedicated for specimens already in the HFEF hot cell. The north radiography station is outside of the main HFEF hot cell and allows NRAD imaging of non-irradiated items. The NRAD images of EBR-II irradiated metallic fuel pins were taken in the east radiography station. Thermal neutrons have the capability to transmit through most materials and are ideal for NRAD imaging. However, because of their high thermal neutron absorption cross-section, fissile materials (e.g., highly-enriched nuclear fuels) may not be as transmissible to thermal neutrons. This is also the case for oversize specimens with extraneous thickness. Epithermal neutron imaging is therefore used as a complement to thermal neutron NRAD imaging. At HFEF’s NRAD facility, both thermal and epithermal neutrons can be used for NRAD imaging. Irradiated nuclear fuels emit high levels of γ radiation that can easily darken X-ray films, so direct exposure NRAD cannot be used to image them. Instead, an indirect NRAD imaging method was developed at HFEF’s NRAD facility. In this method, foils made of materials that can be activated by neutrons (i.e., with large neutron absorption cross section) are used to collect transmitted neutron signals. Then the activated foils are then placed against X-ray films and enclosed in a vacuum cassette so that the γ decay from the activated foils can produce images on the X-ray films. Then, general X-ray film processing procedures are used to digitize and store the images. By using different foil materials, different energy neutrons can be used for NRAD imaging. At the HFEF NRAD station, two types of films are commonly used: dysprosium (Dy) foils with thickness of 130 microns are used to capture thermal neutron signal, while indium (In) foils with thickness of 130 microns are used to capture epithermal neutron signal. A cadmium or gadolinium foil is put before the indium foil to work as a thermal neutron filter. The thermal and epithermal NRAD images can be taken simultaneously by using a Dy/Cd/In sandwiched foil combination. The typical NRAD exposure time is approximately 20 minutes. Then the exposed foils are transferred to film vacuum cassettes. The vacuum ensures that there is no gap between the foil and the film. The foil-to-film exposure time is at least three half-lives of the corresponding radioisotopes, which are 3 hours for In and 7.5 hours for Dy, respectively. Exposed films are processed using an automatic film processor to produce completed NRAD images.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Sister Rod Destructive Examinations (FY22) Appendix J: Leaching of High Burnup Used Nuclear Fuel in Deionized Water

The leaching experiment aims to understand the trends in the radiolysis-enhanced dissolution of HBU SNF when exposed to water (e.g., in-reactor or in-pool cladding failures). Specimens from a baseline M5-clad rod and a heat-treated M5 rod were cut from the fractured CIRFT specimens and placed in 100 mL deionized water for a period of 128 days. Both radial and axial sections were cut to provide different surface areas of fuel in contact with the leachate. During the four-month exposure period, aliquot samples of the leachate were analyzed using gamma spectroscopy and inductively coupled plasma - mass spectrometry (ICP-MS). The analysis quantified the amount of fuel leached into the solutions and provided individual isotopic release fractions (of 30+ isotopes) which were compared as a function of time and surface area of the fuel exposed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Modeling DOE Standard Canister Configurations with Updated Surface Chemistry

Road-ready and final disposition packaging configurations for the advanced test reactor (ATR) fuel currently specifies storage within helium backfilled DOE sealed standard canisters. The aluminum cladding of the ATR fuel contains an oxyhydroxide layer of boehmite/bayerite that generates hydrogen when subjected to irradiation. Understanding the effect of this hydrogen buildup over time to important for long term storage considerations. Previous modeling efforts have built a coupled CFD-chemical model to simulate the temperature gas phase concentrations within the DOE sealed standard canisters. These models have coupled the temperature conditions to both the gas phase radiolysis chemistry and the surface chemistry associated with the oxyhydroxide layer. Continued experimental work has identified trends for aluminum surrogate samples with oxyhydroxide layers for tests done at higher dose rates. At low initial doses a fast generation rate of hydrogen occurs which starts to roll over to a lower generation rate as the total dose applied in increased. A previous study created a small-scale chemical model was built to replicate a mini-canister surrogate system at SRNL as well as for the smaller capsule tests performed at INL. The previous iteration of the model utilized step function for its G-values for the hydrogen generation over a 200-year period. This model makes an update to the surface chemistry to account for theorized surface chemistry reactions allowing for oxygen to remain bounded to the oxyhydroxide layer. As additional experiments continue, the kinetic fits may be adjusted to adapt to new data. Three canister configurations are modeled – the base 18-inch, 15-foot DOR standard canister with 30 ATR fuel elements, an 18-inch, 10-foot DOE standard canister with 32 ATR fuel elements and a 24-inch, 10-foot DOE standard canister with 40 ATR fuel elements. In previous reports, the primary sensitivity of the canister conditions was identified as the decay heat of the fuel and the dried condition of the fuel. Only these parameters are studied in the report. For the nominal case with dried fuel, the hydrogen generation is only about 2%, so it is even less than the flammability limit if it were exposed to oxygen. For the densely packed 18-inch case the total hydrogen concentration is only around 4% with the nominal decay heat. For the densely packed 24-inch case the total hydrogen concentration is only 2.5%, roughly 20% higher than the original packing design, and still under flammability conditions if exposed to oxygen.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Summary Report for the 2019 Radiation Detection for Nuclear Security Summer School

The Pacific Northwest National Laboratory (PNNL) hosted students from across the United States at the 6th Radiation Detection for Nuclear Security Summer School 17-28 June 2019. The summer school provided students with a unique understanding of nuclear security challenges faced in the field and exposed them to the technical foundations, analyses, and insight that will be required by future leaders in technology development and implementation. The course heavily emphasized laboratory and field demonstrations including measurements of special nuclear material. Student evaluations and feedback from student advisors indicates that the summer school achieved its objectives of 1) exposing students to the range of nuclear security applications for which radiation detection is necessary, 2) articulating the relevance of student research into the broader context, and 3) growing student interest in careers in nuclear security.

61 RADIATION PROTECTION AND DOSIMETRY↗