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538 records · Page 30

Global Properties of Local Star Forming Galaxies (ADP 2000)

We performed an archival study of the Hopkins Ultraviolet Telescope (HUT) Astro-2 database. Nineteen spectra of star-forming regions and starburst galaxies were retrieved, reprocessed, and analyzed. The spectra cover the wavelength region 912- 1800 A, providing access to the domain of peak luminosity from a young stellar population. We created an atlas of galaxy spectra documenting the continuum and line properties with an emphasis on the relatively unexplored spectral region below 1200 A. The dust obscuration law was derived from a comparison of the HUT spectra with synthetic population models. The law is similar to the commonly adopted starburst reddening curve at longer wavelengths and approaches the Milky Way law near the Lyman break. A simple power-law parameterization is given, which allows users to express the reddening law in terms of the stellar or nebular color excess at ultraviolet or optical wavelengths. We studied the effect of time-dependent dust obscuration on synthetic ultraviolet line profiles of a young stellar population. If the youngest and most massive stars are more obscured than the older, less massive stars, the C IV 1550 and other stellar wind lines are significantly diluted with respect to a simple foreground screen model for the dust. We propose to use stellar wind lines as a probe of the dust-obscuration model instead of the previously employed nebular emission lines. Since purely stellar diagnostics are utilized, uncertain assumptions on the nebular properties are unnecessary. Photoionization models demonstrate that the C IV 1550 emission is typically dominated by stellar winds and nebular contamination is negligible. A first comparison with the galaxy sample observed with the Hopkins Ultraviolet Telescope favors a dust geometry affecting ionizing and nonionizing stars equally. We point out the need for higher quality data for a more rigorous comparison. The Hubble Space Telescope is capable of obtaining such data in the future.

Leitherer, Claus↗

Iodine Retention of Long-chain Organic Iodides on Silver-based Sorbents under DOG and VOG Conditions

The aqueous reprocessing of used nuclear fuel releases four key volatile radionuclides ( 3 H, 14 C, 85 Kr, and 129 I) from the used fuel into the off-gas streams of a reprocessing facility. Some semi-volatile radionuclides such as 106 Ru may also be released into the gas streams. Compliance with US regulations may require removal of these radionuclides from the off-gas streams before their discharge to the environment (Jubin et al. 2017). Iodine is released during multiple unit operations within a plant and can be found in gas streams such as the shear off-gas, dissolver off-gas, vessel off-gas (VOG), and waste solidification off-gas. To achieve DFs >1,000, treatment of the plant off-gas streams must include, at minimum, removal of both the dissolver off-gas and VOG. A 2015 analysis showing that the speciation of iodine in the VOG is primarily composed of organic alkyl iodides and that abatement technology for organic iodides is not well developed has produced increased interest in removing iodine from VOG. The lack of knowledge surrounding iodine removal from the VOG prompted the Office of Nuclear Energy within the US Department of Energy to initiate experimental efforts targeted at understanding organic iodide removal from prototypic VOG streams. In 2018 a joint test plan was developed and issued by Oak Ridge National Laboratory and Idaho National Laboratory. This test plan is intended to guide a multiyear experimental effort that will provide substantial amounts of information about the removal of organic iodides from VOG streams. This document reports on the progress of Idaho National Laboratory and Oak Ridge National Laboratory in the execution of the joint test plan as of the end of fiscal year 2019. Silver-based sorbents are the primary removal technology being characterized, and this report includes data on iodine adsorption by reduced silver-exchanged mordenite (also called silver-exchanged zeolite [AgZ]) (as a baseline iodine sorbent) and silver-functionalized silica aerogel (AgAero or Ag Aerogel) (as an advanced iodine sorbent). Conclusions are preliminary in nature and reflect the ongoing execution of the test plan through close collaboration between the two laboratories.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Re-evaluation of the Gamma Radiolysis Radiation Chemistry of Neptunium

The reprocessing of spent nuclear fuel by solvent extraction techniques starts with dissolving fuel in concentrated nitric acid (HNO{sub 3}). The resulting radioactive liquor is subjected to multiple stages of solvent extraction to partition desired metal ions (e.g. uranium, plutonium, and neptunium) into an organic phase using specialized extractants. Under process conditions the solvent system is continuously exposed to a high intensity radiation field, which induces radiolytic degradation of both the diluent and extractants. This degradation occurs through the formation of radicals, as well as degradation products. Moreover, both radicals and degradation products can undergo redox chemistry with metal ions within the solvent system. This can be particularly problematic for metals such as neptunium which depend on the maintenance of a particular valence state amenable to complexation by extractants such as tributylphosphate in the PUREX (Plutonium Uranium Redox Extraction) process. Neptunium (Np) is well extracted when it is Np(IV) and Np(VI) but almost unextractable when Np(V). A recently study showed that the radiolysis of Np (VI) in acidic (4 M HNO{sub 3}) solution underwent reduction to Np(V). This reduction only occurred after sufficient production of nitrous acid (HNO{sub 2}) which countered the action of radiolytically-produced oxidizing free radicals (nitrate radical, NO{sub 3}{sup .} and hydroxyl radical, {sup .}OH). This radiation-induced chemistry was successfully modeling using a simplified kinetic model, that included a reaction set for water radiolysis, plus published rate constants for the reactions of free radicals with Np(VI) and Np(V). The most sensitive reaction rate constants were identified in this model, and optimization of the five most sensitive was performed to get excellent model agreement with the experimental data. No Np(IV) was observed or predicted by the model under these conditions. The present research re-evaluates this radiation chemistry of neptunium in aerated aqueous solutions of HNO; by using a far more comprehensive FACSIMILE code. We have also extended this modeling to study the radiolytically-induced Np redox chemistry occurring under multiple other nitric acid acidities, to fully characterize the importance of the oxidizing radical and reducing nitrous acid reactions under a range of conditions relevant to large-scale process conditions. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The Effect of Kr-85 Decay to Rb-85 on Waste Forms - 17105

Krypton-85 (Kr-85) is a volatile radionuclide released during the reprocessing of used nuclear fuel (UNF). Prior to discharge of process off-gas streams to the environment, removal of Kr-85 is required to meet emission regulations. Once removed from the off-gas streams, Kr (containing stable Kr in addition to Kr-85) must be placed in storage until the Kr-85 has decayed to levels such that its potential release would meet regulatory guidelines. The current method of storage is high-pressure metal canisters. Historically, concerns have been expressed that the decay product of Kr-85, Rubidium-85 (Rb-85), could cause corrosion and weakening in the canisters that would ultimately lead to premature failure and release of Kr-85. Alternate methods and materials, such as matrix isolation in a vapor deposited metal and immobilization in zeolites, have been investigated as storage approaches for Kr. However, even these storage methods may become compromised due to the chemical effects of Rb-85 arising from the decay of Kr-85. A review was conducted of the available literature to examine topics relevant to the effects of Rb on the long-term storage of Kr-85, examine the source terms in the context of this concern, and suggest a path forward to resolve outstanding knowledge gaps. In the course of this analysis, several knowledge gaps were identified. Examples include: o The use of solid sorbents to potentially permit more Kr-85-bearing gas to be loaded into canisters, either at the pressures used in the current method or at significantly lower pressures. o A cost-to-benefit analysis is needed to ascertain the practicality of manufacturing waste forms for Kr-85 storage with solid sorbents. o The effects of radiation and chemical transmutation in solid sorbents or matrices for this application are virtually unknown. o Fundamental data are needed on corrosion rates and mechanisms as functions of Rb concentration, storage temperature, etc., for various storage approaches (e.g., as compressed gas or encapsulated in a getter material) and storage container materials. The present analysis focused on the available information regarding storage of Kr-85 in high-pressure containers. It was judged unlikely that such containers would be compromised by corrosion from the Rb decay product, especially if the Kr recovery operations result in a gas composition with very low oxygen content. However, this conclusion should be revisited based on preliminary data gathered from analysis of legacy Kr waste forms. These legacy waste forms are a result of experiments conducted at Idaho National Laboratory over 30 y ago and have been stored for more than three Kr-85 half-lives. Evaluation of these forms indicates significant corrosion, the cause of which has not been conclusively determined. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Near-Surface Phytoplankton Pigment from the Coastal Zone Color Scanner in the Subantarctic Region Southeast of New Zealand

Primarily based on satellite images, the phytoplankton concentration southeast (down- stream) of New Zealand in the High Nitrate - Low Chlorophyll (HNLC) Subantarctic water between the Subtropical Convergence (STC) and the Polar Front (PF) is believed to be higher than in the remainder of the Pacific Sector. Iron enrichment is assumed to be the reason, To study the question, near-surface phytoplankton pigment estimates from the Coastal Zone Color Scanner for up to 7 yr were reprocessed with particular attention to interference by clouds. Monthly mean images were created for the U,S. JGOFS Box along 170 deg W and means for individual dates calculated for 7 large areas between 170 deg E and 160 deg W, 45 deg and 58 deg S, well offshore of New Zealand and principally between and away from the STC and PF. The areal means are about as low as in other HNLC regions (most values between 0.1 and 0.4 or 0.5 mg/ sq m, with very few winter images; median of seasonal means, 0.26 mg/sq m) except at times near the STC, The higher means tend to occur in late summer and autumn, However, contrary to expectations, neither the PF nor the environs of the Subantarctic Front are distinguished by a zone of increased pigment. Also, of 24 spring-summer images of oceanic islands in mostly pigment-poor water, 17 yielded no recognizable elevated pigment; islands were 5 times surrounded by approximately doubled concentrations (ca 100 km in diameter), and 2 cases may have been associated with an extensive bloom. Inspection of offshore images showed concentrations of 1 greater than or equal to(up to 5) mg/sq m in rare patches of 65 to 200 km size on approximately one-tenth of the dates; such patches were not seen in Sub-antarctic waters of the eastern Pacific Sector. A case is made for Australian airborne iron supply being the cause that, presumably, would enhance large-celled phytoplankton. Since, however, the putative iron supply from the seabed around the oceanic islands or the near-by Campbell Plateau normally does not lead to phytoplankton increase, patches of neritic mesozooplankton advected from the shelves might be another mechanism that generates blooms of small-cetled phytoplankton, but there are no data. These alternatives can easily be field-tested from concentration and size composition of the phytoplankton.

Banse, Karl↗

West Valley Demonstration Project (WVDP) Annual Site Environmental Report (ASER) for Calendar Year 2025

The report, prepared for the U.S. Department of Energy West Valley Demonstration Project office (DOE-WVDP), summarizes the environmental protection program at the WVDP for calendar year (CY) 2025. Monitoring and surveillance of the facilities used by the DOE are conducted to verify protection of public health and safety and the environment. The report is a key component of the DOE’s effort to keep the public informed of environmental conditions at the WVDP. The quality assurance protocols applied to the environmental monitoring program ensure the validity and accuracy of the monitoring data. In addition to demonstrating compliance with environmental laws, regulations, and directives, the evaluation of data collected in 2025 continued to indicate that WVDP activities posed no threat to public health or safety, or to the environment.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Iodine Capture and Mechanical Stability of Modified Silver-Functionalized Silica Aerogel

Silver-functionalized silica aerogel (AgAero) is a material proposed for use in the removal of iodine from the off-gas streams arising from nuclear fuel reprocessing. This material was developed by Pacific Northwest National Laboratory and has been shown to adsorb up to 300 mg of iodine per gram of AgAero. One of the challenges noted for AgAero as an iodine sorbent is its mechanical stability. Its initial particle size is >0.85 mm, but previous testing has shown that extended exposure to heated gas streams results in the degradation of the material such that the sorbent bed is compacted with a substantial amount of fines produced. The observed mechanical degradation prompted an effort to reengineer the silica aerogel to improve the mechanical stability of the material without compromising its iodine capture characteristics. Pacific Northwest National Laboratory has modified the material with the intention of strengthening the aerogel backbone and improving mechanical durability. This reengineered material was transferred to Oak Ridge National Laboratory for extended testing to assess its mechanical durability. Modified AgAero was continuously exposed to a CH 3 I-bearing humid gas stream for 84 days. Testing was performed at 150°C with a superficial gas velocity of 10 m/min., a CH 3 I concentration of 554 ppb, and an inlet dew point of 10°C. The density of the AgAero increased by 16% during testing, and the height of the column was observed to decrease by 11%. The fines produced by the material were comparable to that of previously supplied material. Additionally, iodine loading of a thin bed of modified AgAero was performed at 150°C with a superficial gas velocity of 10 m/min. and a CH 3 I concentration of 50 ppm (balance dry air) with a total test duration of 1 week. The CH 3 I capture capacity of the reengineered material was 225 mg iodine per gram AgAero, as compared to a CH 3 I capacity of 250 mg iodine per gram AgAero for the original material. The primary data collected were visual observations, density measurements before and after testing, and the extent of column compaction during testing. Additionally, the material was tested to ensure that the iodine capacity of the material was not adversely impacted by the alternative methods used in the production of the reengineered material. Based on these criteria, no distinguishable improvements were observed between the material produced in fiscal years 2017 and 2019 and the mechanical stability of the aerogel in prototypic off-gas conditions remains a challenge to large-scale deployment.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The x ray variability of NGC6814: Power spectra

Simulation techniques are used to obtain the X-ray variability power spectrum of unevenly sampled GINGA data from NGC6814. A simple power law is not an adequate description of the power spectrum, with the residuals showing excess power on timescales consistent with the periodicity seen in EXOSAT observations of this object. However the shape of the folded lightcurve is very different, with 3 main peaks, two of which are separated by an extremely sharp dip instead of the single peak and small harmonic structure observed by EXOSAT. Using the dip as a fiducial mark, a second GINGA observation of this source taken one year later is found to be consistent with being completely periodic and phase coherent with this first GINGA observation. Thus the period is consistent with being constant over a period of 6 years, but phase coherence is only maintained on timescales of approximately 1 year. Over 75 percent of the total source variability is due to the periodic component (r.m.s. amplitude of 36 percent). The residual variability can be described as the more usual 'flicker noise' f(exp -1.1) powerlaw. This shows no apparent high frequency break on timescales greater than 300 seconds. Subtle differences in the shape of the folded light curve with energy, and the very large amount of power in the periodic component suggest occultation as its origin, though amplification of variability from an X-ray emitting 'hot spot' at the disk inner radius through gravitational lensing is also possible. The former suffers from the very arbitrary nature of the periodic timescale, while the latter is unattractive as it cannot simply explain the lack of high frequency break in the residual power. That these models probably fail to provide an adequate explanation may be due to the added complexity of anisotropy of the X-ray emission, suggested by the discrepancy between the lack of soft photons implied by the flat spectrum and the copious source of soft photons available from reprocessing in the iron line producing material.

Done, C.↗

West Valley Demonstration Project (WVDP) Annual Site Environmental Report (ASER) for Calendar Year 2024

The report, prepared for the U.S. Department of Energy West Valley Demonstration Project office (DOE-WVDP), summarizes the environmental protection program at the WVDP for calendar year (CY) 2024. Monitoring and surveillance of the facilities used by the DOE are conducted to verify protection of public health and safety and the environment. The report is a key component of DOE’s effort to keep the public informed of environmental conditions at the WVDP. The quality assurance protocols applied to the environmental monitoring program ensure the validity and accuracy of the monitoring data. In addition to demonstrating compliance with environmental laws, regulations, and directives, evaluation of data collected in 2024 continued to indicate that WVDP activities pose no threat to public health or safety, or to the environment.

54 ENVIRONMENTAL SCIENCES↗

Predicting cutoff L-shells of solar protons using the GPPSn particle dataset

Solar energetic protons (SEPs) arriving at the Earth trigger severe radiation storms in the near-Earth space, directly impacting space missions operating at various altitudes. Therefore, monitoring SEP events and predicting the penetration depths of solar protons are critical for aerospace sectors. Building on previous efforts, here we demonstrate the feasibility of using proton measurements from the Global Prompt Proton Sensor network (GPPSn), enabled by Los Alamos National Laboratory developed combined X-ray dosimeters aboard GPS satellites, to characterize and predict the penetration of solar protons into the geomagnetic field. The inclined medium-Earth-orbits (MEOs) of the global GPS constellation offer a unique advantage of allowing simultaneous measurements of penetrating solar protons inside both open- and closed-field line regions. Therefore, the L-profiles of ∼10s–100 MeV solar protons and their associated cutoff L-shells can be determined from the GPPSn dataset, using predefined threshold proton flux values rather than traditional flux ratios. After examining a list of SEP event intervals across solar cycles 23, 24 and 25—including the 2024 Mother’s Day superstorm, we showcase how the latest GPPSn proton dataset (release v1.10), reprocessed and calibrated, can not only be used to monitor solar proton distributions inside the dynamic geomagnetic field for individual events, but also to derive a new empirical model linking cutoff L-shells with several key space weather parameters. This newly developed SEPCL-MEO model demonstrates high predictive performance; for example, predictions for > 30 MeV solar protons yield a correlation coefficient of 0.85 and performance efficiency of 0.67 when validated against GPPSn observations. Results from this pilot study underscores the scientific and operational value of the GPPSn dataset, and this dataset—when paired with machine-learning techniques—can play a critical role in observing and predicting the effects of future incoming SEP events, including extreme ones.

58 GEOSCIENCES↗

Developing a new criticality methodology to support decommissioning of legacy plutonium facilities

To decommission a legacy plutonium finishing facility, a number of gloveboxes need to be disposed of. These gloveboxes have been in place since the 1960's and were operational until the 1980's. A period of initial clean out and decommissioning took place in the 1990's and the first gloveboxes were removed from the line in the early 2000's. Compliance with downstream waste handling facility requirements meant that the gloveboxes needed to be removed using intensive 'hands-on' methods in order to size reduce them to fit into 200 litre (55 gallon) drums. This is the standard approach for handling waste items known as Plutonium Contaminated Material (PCM) on the Sellafield site and was credited in the criticality safety case for the decommissioning of the gloveboxes as it allowed each waste drum to be individually assayed such that the fissile content of the waste could be known. Not only was this approach time-consuming and laborious but as it involved operators working with cutting tools in a highly contaminated area it was challenged as being overly restrictive to operations and potentially hazardous to the workers. In order to decommission the remaining nine gloveboxes in the facility, a new decommissioning approach and associated criticality methodology has been developed. Instead of intensive size reduction and waste drum assay, the gloveboxes will be removed with little or no size reduction and put into storage crates without assay. The criticality assessor will review the operational history of each glovebox, along with the decommissioning records and relevant plant data, to make an evidence-based judgement that the crated glovebox represents no greater a residual criticality risk than would have been realised from the equivalent number of PCM drums that the standard decommissioning approach would have generated. This method identifies, in conjunction with the plant personnel, a number of review points to ensure that before the glovebox is removed any bulk residue material has been recovered and no more than a safe amount of moderating material (fixative) has been added to fix any remaining fissile contamination. Finally, once these review points have been confirmed to be complete - through a stakeholder meeting with criticality safety, plant operators and project managers - the glovebox will be placed in a crate, and this crate will be declared a Low Criticality Risk crate. No formal assay will be required prior to exporting the crate to the downstream waste handling facility and no fissile mass value will be assigned to the contents of the crate. No further intrusive work will be required on the crate and it can be safely stored without any spacing requirements, pending final disposal. (author)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Initial Assessment of TeF 6 Adsorption

Research and development that supports the management of off-gases from nuclear fuel reprocessing has historically been focused on the off-gas streams that arise from aqueous reprocessing technology. However, as Gen-IV reactor development pathways move toward deployment, alternative spent nuclear fuel (SNF) processing and disposition pathways have been considered more actively. This work is focused upon aspects of fluoride volatility (FV) processing. The versatility of this method for deployment against multiple types of spent fuel encourages the continued advancement of both the primary separations processes and the secondary processes, including waste treatment, material control and accountability, and engineering designs. Recent work noted that TeF 6 , the most highly volatile fluorinated compound produced during FV processing, did not have a clear abatement technology recommended in the literature. Thus, this work performed scoping tests on activated alumina and copper shot to assess whether they could be used to remove TeF 6 from gas streams that bear F 2 . Previous work on this topic was not well described in the literature and was not performed with excess F 2 in the stream as would be typical of spent fuel processing via FV. To support an understanding of the concentration of TeF 6 contacting the adsorbent beds, a series of preliminary testing identified the TeF 6 production rate and the equilibrium concentration of TeF 6 in the gas stream contacting the adsorbent. Excess F 2 was determined to not affect the ability of activated alumina to remove TeF 6 from the gas stream quickly and completely. A determination of whether excess F 2 affected the distribution depth of Te in the sorbent bed is still pending analysis of the used sorbent. Literature suggests that when activated alumina is near saturation, TeF 6 could migrate from the sorbent bed. Future testing should investigate this possibility. Copper metal did not adsorb TeF 6 in the presence of F 2 across the sorbent temperature range of 50 to 335°C. F 2 was fully removed by the copper bed. Although preliminary thermodynamics would indicate adsorption to be energetically favorable, other factors that impact adsorption (e.g., slow kinetics, excess fluorine on the copper surface, an unfavorable transition state) are likely preventing the adsorption of TeF 6 at an easily measurable rate. The work also investigated TeF 6 production from multiple forms of Te in the temperature range of 100 to 250°C. No previous study had assessed the initial reaction rates for this process. A carefully designed study allowed determination of the activation energy for the production of TeF 6 from Te metal. The substantial amount of data collected during this study merits analysis beyond what is described here. A more in-depth kinetic analysis will be pursued. Additional analytical results will provide the ability to benchmark adsorption coefficients for TeF 6 , understand the distribution of TeF 6 within the alumina bed, and better understand the effect of F 2 partial pressure on Te fluorination. The data from this report, as supplemented by these additional analyses, will be submitted to a peer-reviewed journal.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Development and Optimization of Voltammetric Methods for Real Time Analysis of Electrorefiner Salt with High Concentrations of Actinides and Fission Products

This project addresses the problem of achieving accurate material control and accountability (MC&A) around pyroprocessing electrorefiner systems. Spent nuclear fuel pyroprocessing poses a unique challenge with respect to reprocessing technology in that the fuel is never fully dissolved in the process fluid. In this case, the process fluid is molten, anhydrous LiCl-KCl salt. Therefore, there is no traditional input accountability tank. However, electrorefiners (ER) accumulate very large quantities of fissile nuclear material (including plutonium) and should be well safeguarded in a commercial facility. Idaho National Laboratory (INL) currently operates a pyroprocessing facility for treatment of spent fuel from Experimental Breeder Reactor-II with two such ER systems. INL implements MC&A via a mass tracking model in combination with periodic sampling of the salt and other materials followed by destructive analysis. This approach is projected to be insufficient to meet international safeguards timeliness requirements. A real time or near real time monitoring method is, thus, direly needed to support commercialization of pyroprocessing. A variety of approaches to achieving real time monitoring for ER salt have been proposed and studied to date—including a potentiometric actinide sensor for concentration measurements, a double bubbler for salt depth and density measurements, and laser induced breakdown spectroscopy (LIBS) for concentration measurements. While each of these methods shows some promise, each also involves substantial technical complexity that may ultimately limit their implementation. Yet another alternative is voltammetry —a very simple method in theory that has previously been tested for this application to a limited extent. The equipment for a voltammetry system consists of off-the-shelf components (three electrodes and a potentiostat), which results in substantial benefits relative to cost and robustness. Based on prior knowledge of electrochemical reduction potentials for each of the species of interest, voltammetry can be used to quantify concentrations of a variety of elemental species—including uranium, plutonium, minor actinides, and rare earths. Various methods have been tested by other researchers to date—including cyclic voltammetry, square wave voltammetry, normal pulse voltammetry, etc. In most cases, it has been observed that there is a very limited concentration range for which the output can be readily correlated with concentration in the salt. Furthermore, testing to date has been limited to simple ternary salts with only a single element being quantified. While incomplete for application to MC&A for pyroprocessing, these results lead us to believe that voltammetry can be optimized based on salt properties and fundamental electrochemical rate processes to yield a highly accurate and robust method. This project is divided into four tasks jointly executed by three university research groups. This includes experimental measurement of key physical data on the systems of interest, development of a predictive voltammetry model, experimental validation of the voltammetry model, and design/verification of an optimized measurement method. This project supports the goals of the US-ROK Joint Fuel Cycle Study in addition to the NA-24 Office of the National Nuclear Security Agency and the International Atomic Energy Agency (IAEA).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Innovative Approach to SCC Inspection and Evaluation of Canister in Dry Storage

This final report is summarized four years of work of awarded project number DE-NE0008442\IRP-15-9318, title as: “Innovative Approach to SCC Inspection and Evaluation of Canister in Dry” supported by Nuclear Energy University Program\Integrated Research Program, NEUP\IRP, where last year is an extension of no cost project. This research work is focused on the possible degradation of dry storage canister holding used nuclear fuel (UNF), due to exposure of marine atmospheric environment. The canister usually designed from a welded austenitic stainless-steel of types 304 or 316, encased in a concrete shell known as an overpack. This canister designed and licensed for 20 years with an extension period need to be determined, in addition 20 years or more. These casks are located throughout the country in Independent Spent Fuel Storage Installations (IFSFIs) often on the site close to nuclear power plants, that are often located in coastal or lake-side regions where a marine atmospheric salt air environment exist. As a result of several recent decisions, such as not pursuing Yucca Mountain as a long-term geologic repository storage facility for UNF and the cancellation of the construction of a reprocessing facility in the 1980s due to proliferation risks, interim dry storage facilities for long-term storage are vital option for the immediate future of nuclear energy technology. One of the primary concerns with respect to the long-term performance of the storage casks is the potential for corrosion initiation due to deliquescence of salts deposited on the canister surface as aerosols; in regions of high residual weld stresses, this may lead to localized stress corrosion cracking (SCC). Dust and aerosols in the air being drawn though ventilation openings in the overpacks of passively ventilated dry canister storage systems may be deposited on the stainless-steel canister outer surfaces. Under these conditions, localized corrosion attack can occur. Chlorides ions deliquescence on the canister surface, a process by which the salts essentially pull moisture out of the air, creating a concentrated salt brine on the canister surface. Chloride-induced stress corrosion cracking (CISCC) of welded zones is of special concern, as it a well-documented mode of attack for austenitic stainless steels marine environments, and many independent spent fuel storage installations (ISFSIs) are located in coastal areas. Recent canister inspections have shown that chloride salts are present on the surface of in-service canisters at near-marine settings. However, canister surface inspections of satisfactory resolution to detect SCC have never been carried out in details, because access to the canister surfaces through vents in the overpacks is extremely limited, and high radiation fields make removal of the canisters from the overpacks undesirable. Although no significant corrosion damage has not been detected up to date, there is concern that this may lead to pitting corrosion, which could in turn develop into stress corrosion cracking, causing canister structural failure. The initiation and propagation of pitting corrosion has been widely studied in full immersion conditions, but limited studies have been done on marine atmospheric conditions, which is a focus of this work, these includes laboratory and field experimentally and propagation rate modeling of pitting and transition to crack, and crack propagation rate. It is known, however, that the rate of atmospheric corrosion can be affected by variations in relative humidity (RH), salt density, salt type, droplet area, temperature and stainless-steel microstructure and residual stress particularly in welded zones of canisters. The integrated research program has identified potential deterioration mechanisms for the stainless-steel canisters containing the UNF in dry storage that require detailed research and investigation and will have an impact on the performance of long-term interim storage under the normal and extreme environmental conditions experienced during the duration of this storage. The prediction and monitoring of canister corrosion processes while in storage can provide important data for the assessment of interim storage performance and the safety to the public. This report comprises of mainly the published results in different journals and covering a wide range spectrum from susceptible stainless-steel types 304\316 microstructural analysis through the implant test at atmospheric environment, residual stress analysis of mockup canister and simulation, inspection methodology includes nonlinear ultrasound and vibro-thermography and stochastic modeling and simulation of pits propagation rates and transition to cracks. Description of field specimens installed at ISFSI of Main Yankee is given in the following chapters and will be analyzed in the coming future and serves as an important data for a stochastic analysis as it was drawn from the publications and reports described in this report. The purpose of this report is to bring together the project efforts that includes improving in our understanding of structural aging performance at current dry storage casks fleet at ISFSIs in the context of remedial maintenance and inspection applications technologies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Comparison of Extended and Accelerated VOG Tests

The reprocessing of used nuclear fuel would release volatile radionuclides into the off-gas streams of a processing plant, including ¹²⁹I. The dissolver off-gas and more dilute vessel off-gas streams (VOG) must both be targeted when mitigating ¹²⁹I environmental release because each contains some amount of iodine. Iodine-129 will likely be found as elemental iodine (I₂) and methyl iodide (CH₃I) in these off-gas streams. Reduced silver-exchanged mordenite (AgZ or Ag⁰Z) has been investigated as a potential sorbent for iodine abatement and is studied here under prototypic VOG conditions. Because of the relatively low iodine abundance and high flow rates of the VOG, total iodine concentrations are expected to be in the parts per billion range. Thus, VOG experiments need to run for extended durations at low concentrations to reach sorbent saturation. Because the sorbent will be exposed to oxidizing gas streams for extended periods of time, aging effects and sorbent degradation need to be considered when designing a sorbent-based abatement system. Three sets of experiments were performed with the aim of determining how the adsorption of iodine by AgZ is affected by differing test durations and gas compositions. The first tested the capacity of sorbent aged for 8 months under a humid air stream. The second tested differences in sorbent capacity and mass transfer zone (MTZ) length during high-concentration (1200 ppb v ) CH₃I loading in a humid nitrogen gas (N₂) stream and a humid air gas stream over 28 days. The third tested sorbent capacity and MTZ length during low concentration (< 200 ppb v ) CH₃I and I₂ loading in a humid air stream over 9 months. The results of these tests suggest that AgZ capacity drops by ~50% after 1 month of aging, by ~60% after 2 months of aging, and then does not continue to decrease significantly at up to 8 months of aging. One-month aging tests that compared N₂ and air as the gas stream diluent resulted in similar maximum loading capacities and overall loading curves, indicating that the effects of aging cannot be mitigated by avoiding air as the balance gas. The 9-month extended VOG tests did not result in clear sorbent saturation at the inlet, but it can be inferred using an assumption of a maximum capacity of 45 mg I/g AgZ. Applying this assumption, then the MTZ of CH₃I is 12.8 cm, and the MTZ of I₂ is 12.4 cm. These results are similar to previous tests. Comparisons to tests completed at Idaho National Laboratory suggest that the CH₃I MTZ may be dependent on concentration. Future work should re-evaluate the design of the VOG iodine capture system with this updated data and should seek to understand fundamental characteristics of CH₃I adsorption by AgZ, such as the effect of concentration, gas velocity, and gas composition.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

On the 2018 Outburst of the Accreting Millisecond X-Ray Pulsar Swift J1756.9-2508 As Seen with NICER

We report on the coherent timing analysis of the 182 Hz accreting millisecond X-ray pulsar SwiftJ1756.92508during its 2018 outburst as observed with the Neutron Star Interior Composition Explorer (NICER). Combiningour NICER observations with Rossi X-ray Timing Explorer observations of the 2007 and 2009 outbursts, we alsostudied the long-term spin and orbital evolution of this source. We find that the binary system is well describedby a constant orbital period model, with an upper limit on the orbital period derivative of Pb < 7.4 ´ 10-13 ss1.Additionally, we improve upon the source coordinates through astrometric analysis of the pulse arrival times,finding R.A.=17h56m57 18±0 08 and decl.=25°0627 8±3 5, while simultaneously measuring thelong-term spin frequency derivative as n = -7.3 ´ 10-16 Hzs1. We briefly discuss the implications of thesemeasurements in the context of the wider population of accreting millisecond pulsars. We reported on the coherent timing analysis of the 2018 outburst of Swift J1756 as observed with NICER. Consistent with analyses of the previous outbursts (Krimm et al. 2007b; Patruno et al. 2010), we find that the X-ray pulsations have energy dependent amplitudes; the fractional amplitude of the fundamental increases with energy, whereas the fractional amplitude of the harmonic shows a slight decline with energy. This energy dependent behavior is not unusual in AMXPs (Patruno & Watts 2012) and can be interpreted in terms of the thermal emission from the stellar hotspot and reprocessing in the accretion column (e.g., Gierliński et al. 2002; Ibragimov & Poutanen 2009). The pulse arrival times of the 2018 outburst are well described by a timing model consisting of a circular orbit with a constant spin frequency. The pulse phases with respect to this model do not show spurious residuals with time or orbital phase, and no evidence is found that the pulse arrival times exhibit an additional delay associated with passing through the gravitational well of the companion star (Shapiro delay). We note, however, that the expected Shapiro delay is given as (Shapiro et al. 1971) Equation (5) where Φ is the orbital phase, G is the gravitational constant, c is the speed of light, and i is the inclination. Even for the maximum allowed companion mass, ${M}_{C}=0.030\,{M}_{\odot }$ (Krimm et al. 2007b, but see Section 4.2 for more details) and an inclination of 90°, the largest delay we can expect is only 4 μs. As this time-delay is smaller than the uncertainty on our phase residuals by nearly two orders of magnitude (see Figure 1), we are not sensitive to Shapiro delays in Swift J1756. Comparing our measurements for the 2018 outburst with those of the 2007 and 2009 outbursts as observed with RXTE, we analyzed the long-term evolution of this source. We found that the binary system is consistent with having a constant orbital period and that the pulsar shows a spin frequency derivative of $\dot{\nu }=-7.3\times {10}^{-16}\,\mathrm{Hz}\,{{\rm{s}}}^{-1}$. 4.1. Spin-down Evolution The long-term spin frequency derivative measured in Swift J1756 is of the same order as the spin frequency derivatives measured in other AMXPs (Hartman et al. 2008; Patruno 2010; Riggio et al. 2011). This frequency change is most likely driven by the neutron star's loss of rotational energy. If so, then the spin-down luminosity is given as Equation (6) where I represents the neutron star moment of inertia. The long-term spin-down of a neutron star is usually assumed to be dominated by the braking torque associated with a spinning magnetic field. Assuming this mechanism is responsible for the observed spin-down in Swift J1756, we can compute the magnetic dipole moment as (Spitkovsky 2006) Equation (7) where α is the misalignment angle between the rotational and magnetic poles. Considering α = 0°–90°, we then find a magnetic field strength of $B\simeq (4\mbox{--}6)\times {10}^{8}$ G at the stellar magnetic poles. This magnetic field strength estimate is in line with those obtained for other accreting millisecond pulsars (see Mukherjee et al. 2015 and references therein). 4.2. Orbit Evolution The observed long-term binary evolution of Swift J1756 is consistent with this source having a constant orbital period and a lower limit on the evolutionary timescale of Equation (8) Binary evolution theory predicts that systems of this type evolve due to angular momentum loss through gravitational radiation (Kraft et al. 1962; Rappaport et al. 1982; Verbunt 1993). For conservative mass transfer, the binary period derivative is given by di Salvo et al. (2008), Equation (9) where MNS is the neutron star mass, $q={M}_{C}/{M}_{\mathrm{NS}}$ is the binary mass ratio, and −1/3 < n < 1 is the mass–radius index of the companion star. Depending on the source inclination, Krimm et al. (2007b) derived a companion mass of ${M}_{C}\,=0.007\mbox{--}0.022\,{M}_{\odot }$ for a neutron star mass of 1.4 ${M}_{\odot }$. For a neutron star mass of 2.2 ${M}_{\odot }$, the allowed range increased to ${M}_{C}=0.009\mbox{--}0.030\,{M}_{\odot }$. In both cases, they assumed an upper limit on the inclination of i < 85°, motivated by the fact that Swift J1756 does not show eclipses in its light curve. Accounting for the extreme cases of stellar masses and n, the binary may either be contracting or expanding. In either case, however, the rate of change is limited to $| {\dot{P}}_{b}| \lesssim 7\times {10}^{-14}$ s s−1, which is well below the upper limit obtained in this work. Although the binary evolution timescale we obtain for Swift J1756 is consistent with theory, it is worth noting that this is not generally true for low-mass X-ray binaries (see Patruno et al. 2017, for a comprehensive discussion). The AMXP SAX J1808.4–3658, in particular, has been found to evolve on a much shorter timescale, with a first derivative on the orbital period of $3.5\times {10}^{-12}$ s s−1 (Hartman et al. 2008; Patruno et al. 2012; Sanna et al. 2017a). Two models have been proposed to explain this discrepancy: highly nonconservative mass transfer due to irradiation of the companion star by the pulsar (di Salvo et al. 2008; Burderi et al. 2009), and spin–orbit coupling in the companion star (Hartman et al. 2008, 2009). While the latter depends on the companion star, and may vary from source to source, the former should operate in all AMXPs (see also Patruno 2017; Sanna et al. 2017c), including Swift J1756. The spin-down luminosity impinging on the companion star can be estimated as Equation (10) where ${\dot{E}}_{\mathrm{abl}}$ is the ablation luminosity, RL2 is the Roche lobe radius of the companion (Eggleton 1983), and a the binary separation. The irradiation fraction is $f={\dot{E}}_{\mathrm{abl}}/{\dot{E}}_{\mathrm{sd}}$, which, accounting for the range of allowed neutron star and companion masses, evaluates to f = 0.15%–0.35%. The associated mass loss for the companion is given by Equation (11) such that, assuming an efficiency of η = 100%, ${\dot{M}}_{C}\,\sim -3\times {10}^{-10}\,{M}_{\odot }$ yr−1. The effect of this mass loss on the orbital period follows through the relation (Frank et al. 2002) Equation (12) giving a period derivative due to mass loss of ${\dot{P}}_{b,\mathrm{ML}}\,=5\times {10}^{-12}$ s s−1. This value is well above our limit on the period derivative. Hence, in order for this mechanism to be consistent with our observations of Swift J1756, the efficiency at which the companion star converts the incident luminosity into mass loss must be η < 15%. This value is very different from the 40% required in SAX J1808.4–3658 (Patruno et al. 2016) and is instead in line with the <5% efficiency determined for IGR J00291+5934 (Patruno 2017). This work was supported by NASA through the NICER mission and the Astrophysics Explorers Program, and made use of data and software provided by the High Energy Astrophysics Science Archive Research Center (HEASARC). P.B. was supported by an NPP fellowship at NASA Goddard Space Flight Center. D.A. acknowledges support from the Royal Society.

Bult, Peter↗