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186 records · Page 11

Experimental Investigation of Uranium Volatility during Vapor Condensation

The predictive models that describe the fate and transport of radioactive materials in the atmosphere following a nuclear incident (explosion or reactor accident) assume that uranium-bearing particulates would attain chemical equilibrium during vapor condensation. Here, we show that kinetically driven processes in a system of rapidly decreasing temperature can result in substantial deviations from chemical equilibrium. This can cause uranium to condense out in oxidation states (e.g., UO 3 vs UO 2 ) that have different vapor pressures, significantly affecting uranium transport. To demonstrate this, we synthesized uranium oxide nanoparticles using a flow reactor under controlled conditions of temperature, pressure, and oxygen concentration. The atomized chemical reactants passing through an inductively coupled plasma cool from ~5000 to 1000 K within milliseconds and form nanoparticles inside a flow reactor. The ex situ analysis of particulates by transmission electron microscopy revealed 2–10 nm crystallites of fcc-UO 2 or α-UO 3 depending on the amount of oxygen in the system. α-UO 3 is the least thermodynamically preferred polymorph of UO 3 . The absence of stable uranium oxides with intermediate stoichiometries (e.g., U 3 O 8 ) and sensitivity of the uranium oxidation states to local redox conditions highlight the importance of in situ measurements at high temperatures. Therefore, we developed a laser-based diagnostic to detect uranium oxide particles as they are formed inside the flow reactor. Our in situ measurements allowed us to quantify the changes in the number densities of the uranium oxide nanoparticles (e.g., UO 3 ) as a function of oxygen gas concentration. Our results indicate that uranium can prefer to be in metastable crystal forms (i.e., α-UO 3 ) that have higher vapor pressures than the refractory form (i.e., UO 2 ) depending on the oxygen abundance in the surrounding environment. This demonstrates that the equilibrium processes may not dominate during rapid condensation processes, and thus kinetic models are required to fully describe uranium transport subsequent to nuclear incidents.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Morphological Characterization of Uranyl Fluoride Particles via Atomic Force Microscopy

Uranium hexafluoride (UF 6 ) undergoes a rapid hydrolysis reaction when exposed to atmospheric water. In addition to producing hazardous HF gas, the hydrolysis reaction produces uranyl fluoride (UO 2 F 2 ), a radioactive solid phase particulate material. Because of the technological utility of UF 6 in the nuclear fuel cycle, understanding the transport properties of UO 2 F 2 aerosol produced via UF 6 hydrolysis is important for accident scenarios. Moreover, the fundamental chemical and physical properties of the UF 6 hydrolysis reaction are not completely understood. Recently, several experiments on the aerosol phase properties of UO 2 F 2 produced in this way have shown that under most relevant conditions, the particle size distribution (PSD) of UO 2 F 2 can be extremely small, approximately 3 to 5 nm, which is well below the threshold that can be routinely observed via scanning electron microscopy (SEM). Although readily observable in the aerosol phase, observation of nanometer-sized particles in the condensed phase (i.e. deposited on surfaces) remains a challenge. Here, in this study, we have used atomic force microscopy (AFM) to study the PSD and morphological characteristics of UO 2 F 2 deposited at low and high concentrations under different humidity conditions, a primary variable in the hydrolysis reaction. Here, we find strong agreement between PSD measured in the aerosol phase via scanning mobility particle sizing and PSD measured via AFM, with particle sizes peaked below 4 nm for low-humidity conditions. At higher humidity, the distribution is centered around 5 to 10 nm but extends up to 20 nm. These results are in stark contrast to previous measurements using SEM that show PSD on the order of 300- to 1000-nm particle sizes; moreover, these are the first direct measurements of individual particles of UO 2 F 2 having been produced via UF 6 hydrolysis deposited on surfaces. These measurements, therefore, open a new avenue for collecting and detecting UO 2 F 2 in the condensed phase and further refine the PSD, which is critical for environmental transport determinations.

Uranium hexafluoride↗

Milestone 1.2.15: Feasibility of In Situ Accelerated Aluminum Coupon Radiolysis by Synchrotron X-Rays

Extended dry storage of aluminum-clad spent nuclear fuel (ASNF) requires an assessment of the radiolytic generation of molecular hydrogen gas (H2) from the ASNF’s corrosion layers. H2 accumulation can potentially lead to storage canister embrittlement/rupture and the accumulation of flammable gas mixtures in accident scenarios. To date, computational models have been developed for the prediction of radiolytic H2 generation from samples exposed to lower absorbed dose regimes (up to ~3 MGy). However, greater accuracy is needed for higher absorbed doses (> 25 MGy) where the concentration of H2 ultimately reaches a steady-state. Data in this area is limited due to the amount of time taken (months) to accumulate such high gamma doses. Furthermore, a recent study observed radiation-induced damage to the surface of pre-corroded aluminum alloy coupons at high absorbed gamma doses. Despite this observation and its implications, there is currently no computational connection between the radiolytic formation of H2 and changes in the composition and morphology of the cladding’s corrosion layers with absorbed dose. To develop a better understanding of the processes and effects described above, the present study aimed to evaluate the feasibility of leveraging synchrotron x-ray capabilities for coupled accelerated irradiation and in situ surface characterization of ASNF alloys. To that end, National Synchrotron Light Source II (NSLS-II) beamtime was secured and a series of aluminum alloy 1100 (AA1100) wires, prepared under a variety of conditions, were interrogated using ex situ x-ray diffraction (XRD) and scanning electron microscopy (SEM) techniques at Idaho National Laboratory (INL) and ex situ and in situ XRD capabilities at the NSLS-II x-ray powder diffraction (XPD) beamline. Results indicated that performing synchrotron XRD using the available XPD beamline configuration can provide sufficient radiation dose but cannot discern changes in the composition and morphology of sample corrosion layers. Additionally, ex situ XRD and SEM data from Idaho National Laboratory (INL) indicated that the pre-corrosion of AA1100 wires did not generate an appreciably thick corrosion layer, as compared with previous aluminum coupon studies. These thinner surface corrosion layers were not sufficient for detection by both ex situ and in situ synchrotron XRD, specifically under consideration of the NSLS-II XPD beamline’s configuration primarily capturing information from the sample’s bulk material, i.e., aluminum metal. In summary, the use of the NSLS-II XPD beamline for promoting accelerated radiolysis and in situ surface characterization is not appropriate for this program’s goals.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DeFault: DEep‐Learning‐Based FAULT Delineation Using the IBDP Passive Seismic Data at the Decatur CO2 Storage Site

Abstract The carbon capture, utilization, and storage (CCUS) framework is an essential component in reducing greenhouse gas emissions, with its success hinging on the comprehensive knowledge of subsurface geology and geomechanics. Passive seismic event relocation and fault detection offer vital insights into subsurface structures and the ability to monitor fluid migration pathways. Accurate identification and localization of seismic events, however, face significant challenges, including the necessity for high‐quality seismic data and advanced computational methods. To address these challenges, we introduce a novel deep learning method, , specifically designed for passive seismic source relocation and fault delineating for passive seismic monitoring projects. By leveraging data domain‐adaptation, allows us to train a neural network with labeled synthetic data and apply it directly to field data. Using , the passive seismic sources are automatically clustered based on their recording time and spatial locations, and subsequently, faults and fractures are delineated accordingly. We demonstrate the efficacy of on a field case study involving injection related microseismic data from Decatur, Illinois area. Our approach accurately and efficiently relocated passive seismic events, identified faults and could aid in potential damage induced by seismicity. Our results highlight the potential of as a valuable tool for passive seismic monitoring, emphasizing its role in ensuring CCUS project safety. This research bolsters the understanding of subsurface characterization in CCUS, illustrating machine learning’s capacity to refine these methods. Ultimately, our work has significant implications for CCUS technology deployment, an essential strategy in combating climate change. Plain Language Summary In our quest to tackle climate change, we use a strategy known as carbon capture, utilization, and storage (CCUS) to keep greenhouse gases out of the atmosphere. This strategy relies heavily on our ability to understand what's happening deep under the earth's surface. To make sure we store super critical safely, we need to accurately map out the geological structure, especially faults, but this is tough without high‐quality data and complex computer programs. We've developed a new tool called “DeFault,” which uses advanced machine learning to improve how we find and map these underground features. “DeFault” is smart enough to learn from numerically simulated data and then apply what it’s learned to real‐world situations. It groups together seismic activity—tiny tremors and shifts in the earth—based on when and where they happen, which helps us spot where there might be cracks or faults. We tested “DeFault” in Illinois, where CO 2 is injected underground, and it successfully pinpointed where these tremors occurred and mapped out the faults, helping to prevent accidents accurately in the future. Our study shows that “DeFault” will be a powerful ally in making CCUS safer and more effective, especially for the Illinois Basin Decatur Project. Key Points Faults and fractures introduced by carbon storage can be monitored by passive seismicity DeFault algorithm enables an automatic process for accurate and efficient passive seismic event locating and clustering

58 GEOSCIENCES↗

AGR-5/6/7 Final Release-to-Birth Ratio Data Analysis

AGR-5/6/7 is the last of a series of Advanced Gas Reactor (AGR) experiments conducted in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) in support of development and qualification of tristructural isotropic (TRISO) low-enriched fuel for use in the high-temperature gas cooled reactor (HTGR). AGR configuration and irradiation conditions are based on prismatic HTGR technology that is distinguished primarily through the use of helium coolant, a low-power-density ceramic core capable of withstanding very high temperatures, and TRISO-coated particle fuel. The AGR tests provide valuable irradiation-performance data to support fuel process development, qualify fuel for normal operation and accident conditions, and support development and validation of fuel performance and fission-product (FP) transport models and codes. Each AGR test consists of multiple independently controlled and monitored capsules containing fuel compacts placed in a graphite cylinder shrouded by a steel shell. Release-to-birth ratios (R/B) for fission-gas isotopes released from each capsule are calculated from release rates, measured by germanium detectors in the Fission Product Monitoring System (FPMS) installed downstream from each capsule, and birth rates calculated using numerical models of FG generation. The R/Bs are a critical measure of the ability of the fuel kernel, the particle coating layers, and the compact matrix to retain fission-gas atoms, preventing their release into the sweep-gas flow, and the impact of initially defective particles and/or particle-coating failures that occur during irradiation. For fission-gas isotopes, particle failure is defined as failure of all coating layers, allowing gaseous fission atoms to escape from a particle. During the first five cycles (162B ? 165A), R/Bs were stable in the 10-8?10-6 range, and no in-pile particle failures were observed, based on the gross gamma counts. The maximum R/B value of around 2 ? 10-6 for Kr-85m resulted from the presence of as-fabricated exposed kernels (based on the high exposed kernel fraction), the dispersed uranium, and high fuel particle temperatures in Capsule 1. Comparison of capsule-measured R/Bs from these early cycles to predictions using the previously developed AGR R/B model demonstrated FG release from the AGR-5/6/7 TRISO fuel was comparable to that of previous experiments. In addition, the Kr-85m R/B per-exposed-kernel values are comparable to R/B values obtained in AGR-3/4 irradiation experiment and four irradiation experiments performed during 1980s: (1) HRB-17/18, (2) COMEDIE-BD1, (3) HFR B1, and (4) HRB-21. In contrast, all measured R/B values are lower than predictions by the commonly used Richards and German models, which are intentionally conservative. A large number of in-pile particle failures occurred in Capsule 1 by the end of Cycle 166A. During the final four cycles (166A ? 168A), apparent damage to the Capsule 1 gas line appeared to cause FG leakage from that capsule into the other four capsules, resulting in an increase in fission gas (FG) detected in the effluent for all capsules. Isolation of the Capsule 1 gas line during the last three cycles also prevented measurement of its FG release. Thus, R/Bs in all capsules after Cycle 166A are highly uncertain because of undefined amount of leakage from Capsule 1, especially for long-lived isotopes. A few hundred in-pile particle failures were estimated for Capsule 1 before the end of Cycle 166A, but the total number of failures is unknown due to the lack of FG release data in the later cycles. Based primarily on evidence from the gross gamma counts during Cycle 168A, approximately 15 particles failed in Capsule 3 and four particles failed in Capsule 2. In-pile failures in Capsule 3 were anticipated because this capsule was designed to operate beyond the HTGR normal operating temperature range. In contrast, no in-pile failures were identified in the top two capsules (4 and 5) based on the absence of the typical spikes in gross gamma counts and low failure estimates using the AGR model, developed in INL/EXT-14-32970, for R/B of the short-lived isotopes (Kr-89 and Xe-137) with minimal leakage from Capsule 1.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Space Biology and Medicine: Space and Its Exploration - Volume I

Perhaps one of the greatest gifts that has been given to the people of the world in the last few hundred years has been an emerging sense of the place of our planet and its inhabitants within the context of the vast universe. Our knowledge of the rest of the universe has not come quickly, nor was the process of attaining it only recently begun; however, the unprecedented acceleration of that process has benefitted from a fundamental new aspect of our species that has only manifested itself in the last 30 years or so, the ability to travel in space. Before the space age, the Universe was studied only through observations from the Earth. All that has changed with the beginning of the space age. Machines built by humans have flown to all but one of the nine planets that revolve around our Sun, have ventured billions of miles from the Earth and looked back, and have landed on three other worlds. Spacecraft in orbit around the Earth have viewed the sky at a vast number of electromagnetic wavelengths, detecting the shape of the galaxy and the universe, and even measuring the remnants of the universe's beginning. Human explorers have ventured forth, first for short stays in orbit, then, later, walking upon the Moon and living for long periods in space. As they did so, billions of people on the Earth came to view the Earth in a fundamentally different way, not just as the familiar day to- day backdrop for their lives, but as a small oasis suspended in the night sky above an alien landscape. It is this new view of the Earth that is the true gift of space exploration. Space exploration has at once given us a new perspective on the value of our world, and a new perspective from which to understand how it operates. It has shown us that the Earth is by far the most precious place in the solar system in terms of supporting human life, while revealing that other destinations may still be compelling. The exploration of space has at once become a challenge for humanity to overcome and a path to our common future. But for humanity to embark on this path, we need to understand ourselves in a new environment. As such, an understanding of the biological consequences of and opportunities in space flight is essential. In this, the first volume of a joint U.S./Russian series on space biology and medicine, we describe the current status of our understanding of space and present general information that will prove useful when reading subsequent volumes. Since we are witnesses to the beginning of a new era of interplanetary travel, a significant portion of the first volume will concentrate on the physical and ecological conditions that exist in near and outer space, as well as heavenly bodies from the smallest ones to the giant planets and stars. While space exploration is a comparatively recent endeavor, its foundations were laid much more than 30 years ago, and its history has been an eventful one. In the first part of this volume, Rauschenbach, Sokolskiy, and Gurjian address the "Historical Aspects of Space Exploration" from its beginnings to a present-day view of the events of the space age. The nature of space itself and its features is the focus of the second section of the volume. In the first chapter of the part, "Stars and Interstellar Space," the origin and evolution of stars, and the nature of the portions of space most distant from Earth are described by Galeev and Marochnik. In Chapter 2, Pisarenko, Logachev, and Kurt in "The Sun and Interplanetary Space" bring us to the vicinity of our own solar system and provide a description and discussion of the nearest star and its influence on the space environment that our Earth and the other planets inhabit. In our solar system there are many fascinating objects, remnants of the formation of a rather ordinary star in a rather obscure portion of the galaxy. Historical accident has caused us to be much more curious (and knowledgeable) about "The Inner Planets of the Solar System" than about any of these other objects. In Chapter 3, Marov describes the planets Mercury, Venus, Earth, and Mars, their history and origin, and their environmental conditions, and in Chapter 4 Owen provides similar information about Jupiter, Saturn, Uranus, Neptune, and Pluto, "The Outer Planets of the Solar System." Morrison provides a thorough discussion of "Asteroids, Comets, and Other Small Bodies" in Chapter 5. The understanding of these relics of the formation of the solar system may form the center of our ability to understand the origin of solar systems in general, and of the critical role that the beginning of the solar system had on the prospects for the origin of life and its continued survival and evolution in the face of their recurrent impacts on Earth. In Chapter 6, the first chapter of the third part, Rummel describes the area of "Exobiology," the study of the origin, evolution, and distribution of life in the context of the origin and evolution of the universe. The same processes that have given rise to life on Earth may have given rise to life elsewhere. In Chapter 7, the "Earth and the Biosphere," the nature and function of the Earth are discussed as a specific instance of planetary and biological evolution. The effects of biological processes on the Earth under the influence of human activities are also addressed by Moore and Bartlett in Chapter 7. The final chapter in this section concerns the prospects that life in the universe may be widespread; "SETI," the Search for Extraterrestrial Intelligence, by Billingham and Tarter, presents the arguments for conducting a search for evidence of life elsewhere in the galaxy, and describes the various methods proposed for conducting such a search. While SETI has a distinctly exploration al character, more direct means are available for exploring the solar system around us. The fourth part of the volume addresses this subject of space exploration. Considering the prospects for research on space biology and medicine, the means of providing "Access to Space" are described by Feoktistov and Briggs in Chapter 9. This chapter addresses carriers and launch systems, the unmanned and manned spacecraft that they loft into space, and the task of mission operations by which these precious vessels are monitored, navigated, and controlled. Despite the successes of the past and the capabilities of the present, it is clear that the study of space biology and medicine will be even more rewarding in the future than it has been to date. The work of the next few years that will be undertaken by the U.S. and Russia, both independently and jointly, will focus first on enabling greater capabilities in the exploration of space, and then on using the unique characteristics of the space environment to provide insight and greater understanding into biological systems, their behavior, development, and origin. The chapters of the first volume were written by leaders in their fields from the U.S. and Russia. The material presented summarizes our current understanding of space and its exploration. We understand that the first volume will be of interest not only to medical personnel and biologists, but also to general readers who want information about space beyond their own particular fields of expertise.

Nicogossian, Arnauld E.↗