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DOE OSTI2021

Possible impacts of molten salt reactors on the International Monitoring System

Molten salt reactors (MSRs) are gaining support as many countries look for ways to increase power generation and replace aging nuclear energy production facilities. MSRs have inherently safe designs, are scalable in size, can burn transuranic wastes from traditional solid fuel nuclear reactors, can store excess heat in thermal reservoirs for water desalination, and can be used to produce medical isotopes as part of the real-time liquid-fuel recycling process. The ability to remove 135 Xe in real time from the fuel improves the power production in an MSR because 135 Xe is the most significant neutron-absorbing isotope generated by nuclear fission. Xenon-135, and other radioactive gases, are removed by sparging the fuel with an inert gas while the liquid fuel is recirculated from the reactor inner core through the heat exchangers. Without effective abatement technologies, large amounts of radioactive gas could be released during the sparging process. This work examines the potential impact of radioxenon releases on samplers used by the International Monitoring System (IMS) to detect nuclear explosions. Here, atmospheric transport simulations from seven hypothetical MSRs on different continents were used to evaluate the holdup time needed before release of radioxenon so IMS samplers would register few detections. Abatement technologies that retain radioxenon isotopes for at least 120 d before their release will be needed to mitigate the impacts from a molten salt breeder reactor used to replace a nuclear power plant. A holdup time of about 150 d is needed to reduce emissions to the average level of current nuclear power plants.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2021

Modeling of fission and activation products in molten salt reactors and their potential impact on the radionuclide monitoring stations of the International Monitoring System

Molten Salt Reactors (MSRs) are one of six Generation IV reactor designs currently under development around the world. Because of the unique operating conditions of MSRs, which include molten fuel and the continuous removal of gaseous fission products during operation, work was performed to analyze the potential impact of emissions on the International Monitoring System (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). Simulations were performed to predict the production of IMS-relevant radionuclides in four MSR designs operating under two scenarios: (1) a sealed reactor with releases only during operational shutdown, and (2) continuous reprocessing or sparging of the fuel salt. From these production estimates the radioxenon and radioiodine signatures were extracted and compared to three current reactor designs (Pressurized Water Reactor (PWR), BWR, RBMK). In cases where continuous reprocessing of the fuel salt occurred, both the radioxenon and radioiodine signatures were nearly indistinguishable from a nuclear explosion. Estimates were also made of the potential emission rate of radioxenon for three reactor designs and it was found that MSRs have the potential to emit radioxenon isotopes at a rate of 10^15-8×10^16 Bq/d for 133Xe if no abatement is used. An assessment was made of activation products using a candidate fuel salt (FLiBe) mixed with corrosion products for the Thorium Molten Salt Reactor (TMSR-LF1).

Johnson, Christine M.↗

DOE OSTI2023

Dirty bomb source term characterization and downwind dispersion: Review of experimental evidence

Dirty bombs are considered one of the easiest forms of radiological terrorism, a form of terrorism based on the deliberate use of radiological material to cause adverse effects in a target population. One U.S. Government official has even described a dirty bomb attack as “all but inevitable”. While people in the vicinity of the blast may experience acute radiation effects, people downwind may unknowingly be contaminated by the radioactive airborne particulate and face increased long-term cancer risk. The likelihood of increased cancer risk depends on the radionuclide used and its specific activity, its aerosolization potential, the particle sizes generated in the blast, and where a person is with respect to the detonation. Different studies have reported that plausible radionuclides for dirty bomb include 60 Co, 90 Sr, 137 Cs, 192 Ir, 241 Am based on their availability in commercial sources as well as safeguards, the amount needed for adverse health effects, previous mishandling of radionuclides and malicious uses. In order to have increased long-term cancer risk, the radionuclide would have to deposit inside the body by entering the respiratory tract and then possibly migrate to other organs or bones (ground shine is not considered in this paper because areas affected by the event will likely become inaccessible). This implies that the particles will have to be smaller than 10 μm to be inhaled. Experiments involving the detonation of dirty bombs have shown that particles or droplets smaller than 10 μm are generated, independently from the initial radionuclide or its state (e.g., powder, solution). Atmospheric tests have shown that in unobstructed terrain, the radionuclide laden cloud can travel kilometers downwind even for relatively small amounts of explosives. Furthermore, buildings in the path of the cloud can change the dose rate. For instance, in one experiment with a single building, the dose rate was 1–2 orders of magnitude lower behind the obstacle compared to its front face. For people walking around, the amount of particulate deposited on them and inhaled will depend on their path relative to the cloud, resulting in the counterintuitive result that the closer people may actually not be the ones more at risk because they could simply miss the bulk of the cloud in their wandering. In summary, the long-term cancer risk for people caught in a dirty bomb cloud away from the detonation requires considering where and when the people are, which radionuclide was used, and the layout of the obstacles (e.g., buildings, vegetation) in the path of the cloud.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

DOE OSTI2023

Review of particle deposition to and removal from clothing, skin, and hair after a radioactive airborne dispersal event

Explosive Radiological Dispersal Devices (RDD) – aka dirty bombs – are seen as a credible method to carry out a radiological terror attack. After exploding a radioactive source, the radionuclide-laden plume will be blown downwind of ground zero, with particles falling out and potentially depositing on people caught in and under the cloud. Some of these people may not show any sign of radiation sickness and therefore not realize they have been contaminated and may take the radioactive particulate with them on their daily activities, thus spreading the radioactive particulate outside the initially contaminated area. This paper reviews the scientific literature to better understand the rate at which particulate deposits on and is removed from the different “surfaces” of a person, i.e., hair, skin, and clothing. Prior research indicates that: 1) particle deposition is usually higher on skin than on hair and clothing; 2) particle deposition is greater for a person with higher skin moisture, 3) stronger wind increases the deposition flux onto a person, and 4) the fraction of particulate deposited on the hair, skin, and clothing respectively depends on the length of the hair, assuming all the hair surface is available for deposition. The studies taken into consideration show that the largest uncertainty in particulate deposition onto a person is due to clothing type because of the different possible weave arrangements and tightness which translate into differences in actual surface area and surface roughness. A factor of 2-to-20 variation in deposition rate was found. Removal of the particulate from the contaminated person may be due to wind, a person's movement, and/or contact transfer, i.e., by touching a different clean surface. Experiments show that the majority of the particulate is resuspended within 2–6 h mostly depending on the intensity of physical activity. The largest uncertainty in particulate removal from skin depends on the skin moisture, transfer rate of single-contact, and how many objects/people a person touches per hour. No data for hair were found for particle removal and resuspension. The studies considered did not utilize radionuclides directly; however, data on adhesion of radioactive vs. their non-radioactive counterpart have shown that the uncertainty due to the radioactivity of the particles is lower than that due to other factors. In conclusion, an idealized scenario involving a single building in the path of the cloud showed the impact of building-influenced flow on the cloud transport path and mixing, which affects the radiological dose the downwind population is exposed to and consequently the health effects.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

DOE OSTI2024

Impacts of future nuclear power generation on the international monitoring system

Many countries are considering nuclear power as a means of reducing greenhouse gas emissions, and the IAEA (IAEA, 2022) has forecasted nuclear power growth rates up to 224% of the 2021 level by 2050. Nuclear power plants release trace quantities of radioxenon, an inert gas that is also monitored under international agreements as a signature of nuclear weapons tests. To better understand how nuclear energy growth (and resulting Xe emissions) could affect this global nonproliferation architecture, we modeled daily releases of radioxenon isotopes used for nuclear explosion detection in the International Monitoring System (IMS) that is part of the Comprehensive Nuclear Test-Ban Treaty: 131m Xe, 133 Xe, 133m Xe, and 135 Xe to examine the change in the number of radioxenon detections as compared to the 2021 detection levels. If a 40-station IMS network is used, the detections of 133 Xe in 2050 would range from 82% for the low-power scenario to 195% for the high-power scenario, compared to the detections in 2021. If an 80-station IMS network is used, the detections of 133 Xe in 2050 would range from 83% of the 2021 detection rate for the low-power scenario to 209% for the high-power scenario. Essentially no detections of 131m Xe and 133m Xe are expected. The high growth scenario could lead to a six-fold increase in 135 Xe detections, but the total number of detections is still small (on the order of 1 detection per day in the entire network).

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2025

Deployment of portable, modular gas samplers as part of an atmospheric tracer experiment

Underground nuclear explosions release noble gases into the atmosphere that can be detected to support international monitoring efforts. Atmospheric transport models help predict the movement of these gases over long distances, but struggle to predict the movement in the atmosphere local to the release. A field experiment was designed to monitor the movement of 127 Xe within a 5-km radius. Four gas samplers were deployed as part of this experiment to collect atmospheric samples at various distances from the release point. In conclusion, these samples were then analyzed in a near-field lab using a NaI detector and in an off-site lab using gamma-gamma coincidence and beta-gamma coincidence counting.

Radioxenon↗

DOE OSTI2025

Quantifying fission gas adsorption onto natural clinoptilolite in the presence of environmental air and water

Adsorption of noble gas fission products onto naturally occurring minerals is of interest for its potential to retain or retard emissions from nuclear fuel reprocessing operations or underground nuclear explosions. However, experimental studies of trace noble gas adsorption in the presence of air and water have largely focused on synthetic materials, such as activated carbon or metal-organic frameworks. Here, in this study, adsorption of Kr and Xe onto the naturally occurring zeolitic mineral clinoptilolite is studied in the presence of nitrogen and water. By varying the composition of the gas phase and monitoring the change in the combined adsorbate mass, the adsorbed concentration of noble gas is calculated gravimetrically. For dry clinoptilolite, the concentration of adsorbed Kr and Xe is linearly correlated with noble gas pressure and Henry's Law appears satisfactory, despite the presence of nitrogen at atmospheric pressures. However, the presence of water significantly reduces the adsorbed concentration of both Kr and Xe, which is typical in nanoporous sorbents. Here, an empirical bivariate model is presented, combining the Henry's Law adsorption model for a dry adsorbent with the exponential reduction in the presence of water, as reported by Lungu and Underhill in 1999. This model provides a means to estimate the adsorbate concentration at the trace partial pressures and higher water contents relevant to field-scale modeling of fission gas transport through the vadose zone.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Incorporating civilian radioxenon background estimates in anomaly detection

A nuclear explosion screening exercise in 2023 (Maurer et al., 2023) found challenges with discerning anomalous radioxenon activity concentrations relative to elevated background concentrations. Research has continued into methods to detect anomalous radioxenon concentrations by comparing samples to estimates of atmospheric radioxenon background concentrations caused by releases at nuclear reactors or medical isotope production facilities. A new approach estimates the sample concentrations using time-varying radioxenon release rates obtained using optimization techniques that constrain the facility release rates to plausible amounts based on historical data or facility knowledge. The purpose of the optimization is to determine whether any combination of plausible release rates from emitting facilities can explain a series of radioxenon measurements at one or more sampling stations. A case study uses radioxenon data collected at three locations in western Europe for a month in 2021 and considers releases from 77 locations. Fewer samples are identified as being anomalous using a simplistic flagging rule than from an application of the current International Monitoring System (IMS) activity concentration-level rule.

Environmental sciences↗

DOE OSTI2025

Fission gas trapped in Chornobyl fuel microparticles reveals details of reactor operations

The isotopic ratios of fission gas would provide important source information of a nuclear fuel sample found in the environment. However, it is believed that during a reactor accident like Chornobyl all fission gas is lost and that the radioactive particles found in the Chornobyl Exclusion Zone today are depleted in gases by the initial explosion and subsequent fire. We disprove this hypothesis by detection and analysis of trapped krypton and xenon in these particles. Our analysis of krypton and xenon isotopes by noble gas mass spectroscopy in combination with resonance ionization mass spectrometry establishes that important information about reactor operations like age, neutron flux and plutonium fission fraction can still be reconstructed from individual micrometer-sized particles even after decades of weathering in the environment.

Chornobyl↗

DOE OSTI2021

Determining processing behaviour of pure Cu in laser powder bed fusion using direct micro-calorimetry

We report copper is challenging to process by laser powder bed fusion (LPBF) given its high reflectivity at common infrared laser diode wavelengths and high thermal conductivity. Successful deposition of copper in a predictable and repeatable fashion relies on understanding the development of the keyhole melting regime, as well as heating, melting, boiling and vapour formation behaviour when interacting with a laser beam within an LPBF environment. In this study, in situ optical absorptivity measurements are used to clarify the complex physics of the laser material interaction. Absorptivity of laser energy is measured using direct micro-calorimetry and compared to melt pool depth in correlation to processing parameters. The measured absorptivity for a 100 μm layer thickness of powder was found to be approximately four times higher than that of the bare polished discs. It was also shown that high laser power above 500 W and scan speed up to 150 mm/s are appropriate for effective melting of the powder layer, with these parameters overcoming the threshold required to achieve keyhole melting. This is explained by multiple reflections withing the powder particles and the lower thermal conductivity of packed powder in comparison to bare discs. Melt pool formation was found to be highly unstable and an explosive behavior was observed when in the keyhole regime, caused by high fluctuations in absorptivity values. This work demonstrates calorimetry can be used to monitor melting behaviour in a real-time fashion during processing for this challenging to process material, thereby avoiding unnecessary parametric optimisation. In addition, the parametric window for optimum processing revealed here can inform future work.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Energy and environmental aspects in recycling lithium-ion batteries: Concept of Battery Identity Global Passport

The emergence and dominance of lithium-ion batteries in expanding markets such as consumer electronics, electric vehicles, and renewable energy storage are driving enormous interests and investments in the battery sector. The explosively growing demand is generating a huge number of spent lithium-ion batteries, thereby urging the development of cost-effective and environmentally sustainable recycling technologies to manage end-of-life batteries. Currently, the recycling of end-of-life batteries is still in its infancy, with many fundamental and technological hurdles to overcome. Here in this paper, the authors provide an overview of the current state of battery recycling by outlining and evaluating the incentives, key issues, and recycling strategies. The authors highlight a direct recycling strategy through discussion of its benefits, processes, and challenges. Perspectives on the future energy and environmental science of this important field is also discussed with respect to a new concept introduced as the Battery Identity Global Passport (BIGP).

25 ENERGY STORAGE↗

DOE OSTI2023

Assessing the vulnerability of solar inverters to EMPs: Port testing, PCI modeling, and protection strategies

Renewable energy sources are becoming an ever-larger contributor to the power grid. These renewable energy sources depend upon the power electronic devices, specifically inverters, being essential for connecting Photovoltaic (PV) generation to the grid. However, the Electromagnetic Pulses (EMPs) caused by the high-altitude nuclear explosions can generate fast broad-band pulses with nanosecond rise time, potentially causing damage or destruction to electronic components. To assess the vulnerability of PV inverters to high-altitude EMPs, the port testing and Pulsed Current Injection (PCI) modeling schemes are proposed based on the port impedance analysis. Wide-band frequency measurements are achieved by fusing impedance results from three vector network analyzers. Then, a PCI model is used to simulate the induced response to EMP, with two typical immunity levels of EC5 and EC8 tested. Here, the experiment successfully excites the induced voltage and current under EMP, where the voltage and current can reach 1500V/40A and 8000V/150Aunder EC5 andEC8, respectively. The port vulnerability analysis results demonstrate that only some ports can survive under EC5. To defend against the impact of EMP, three protection strategies are discussed.

42 ENGINEERING↗

DOE OSTI2020

Sensitivity of pore collapse heating to the melting temperature and shear viscosity of HMX

A multiscale modeling strategy is used to quantify factors governing the temperature rise in hot spots formed by pore collapse from supported and unsupported shock waves in the high explosive HMX (octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine). Two physical aspects are examined in detail, namely the melting temperature and liquid shear viscosity. All-atom molecular dynamics simulations of phase coexistence are used to predict the pressure-dependent melting temperature up to 5 GPa. Equilibrium simulations and the Green–Kubo formalism are used to obtain the temperature- and pressure-dependent liquid shear viscosity. Starting from a simplified continuum-based grain-scale model of HMX, in this study we systematically increase the complexity of treatments for the solid–liquid phase transition and liquid shear viscosity in simulations of pore collapse. Using a realistic pressure-dependent melting temperature completely suppresses melting for supported shocks, which is otherwise predicted when treating it as a constant determined at atmospheric pressure. Alternatively, melt pools form around collapsed pores when the pressure (and melting temperature) are reduced during the release stage of unsupported shocks. Capturing the pressure dependence of the shear viscosity increases the peak temperature of melt pools by hundreds of Kelvin through viscous work. The complicated interplay of the solid-phase plastic work, solid–liquid phase transition, and liquid-phase viscous work identified here motivate taking a systematic approach to building increasingly complex grain-scale models.

36 MATERIALS SCIENCE↗

DOE OSTI2025

A review of quantum imaging methods and enabling technologies

The field of quantum imaging has recently seen an explosion of new methods and techniques. At the heart of most quantum imaging approaches are three enabling technologies: the source of the quantum light, the detectors that turn sensing into imaging, and the method by which the quantum nature of light is leveraged to improve the desired measurement. This review addresses the dominant and emerging technologies in each of these components as well as details concerning the implementations of various quantum imaging methods.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Electrode roughness dependent electrodeposition of sodium at the nanoscale

Na metal is an attractive anode material for rechargeable Na ion batteries, however, the dendritic growth of Na can cause serious safety issues. Along with modifications of solid-electrolyte interphase (SEI), engineering the electrode has been reported to be effective in suppressing Na dendritic growth, likely by reducing localized current density accumulation. However, fundamental understanding of Na growth at the nanoscale is still limited. Here, we report an in-situ study of Na electrodeposition in electrochemical liquid cells with the electrodes in different surface roughness, e.g., flat or sharp curvature. Real time observation using transmission electron microscopy (TEM) reveals the Na electrodeposition with remarkable details. Relatively large Na grains (in the micrometer scale) are achieved on the flat electrode surface. The local SEI thickness variations impact the growth rate, thus the morphology of individual grains. In contrast, small Na grains (in tens of nanometers) grow explosively on the electrode at the point with sharp curvature. The newly formed Na grains preferentially deposit at the base of existing grains close to the electrode. Further studies using continuum-based computational modeling suggest that the growth mode of an alkali metal (e.g. Na) is strongly influenced by the transport properties of SEI. Our direct observation of Na deposition in combination with the theoretical modeling provides insights for comprehensive understanding of electrode roughness and SEI effects on Na electrochemical deposition.

25 ENERGY STORAGE↗

DOE OSTI2022

Combustion machine learning: Principles, progress and prospects

Progress in combustion science and engineering has led to the generation of large amounts of data from large-scale simulations, high-resolution experiments, and sensors. This corpus of data offers enormous opportunities for extracting new knowledge and insights—if harnessed effectively. Machine learning (ML) techniques have demonstrated remarkable success in data analytics, thus offering a new paradigm for data-intense analyses and scientific investigations through combustion machine learning (CombML). While data-driven methods are utilized in various combustion areas, recent advances in algorithmic developments, the accessibility of open-source software libraries, the availability of computational resources, and the abundance of data have together rendered ML techniques ubiquitous in scientific analysis and engineering. This article examines ML techniques for applications in combustion science and engineering. Starting with a review of sources of data, data-driven techniques, and concepts, we examine supervised, unsupervised, and semi-supervised ML methods. Various combustion examples are considered to illustrate and to evaluate these methods. Next, we review past and recent applications of ML approaches to problems in combustion, spanning fundamental combustion investigations, propulsion and energy-conversion systems, and fire and explosion hazards. Challenges unique to CombML are discussed and further opportunities are identified, focusing on interpretability, uncertainty quantification, robustness, consistency, creation and curation of benchmark data, and the augmentation of ML methods with prior combustion-domain knowledge.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2024

Recent advances in combustion science related to hydrogen safety

Hydrogen is a key pillar in the global Net Zero strategy. Rapid scaling up of hydrogen production, transport, distribution and utilization is expected. This entails that hydrogen, which is traditionally an industrial gas, will come into proximity of populated urban areas and in some situations handled by the untrained public. To realize all their benefits, hydrogen and its technologies must be safely developed and deployed. The specific properties of hydrogen involving wide flammability range, low ignition energy and fast flame speed implies that any accidental release of hydrogen can be easily ignited. Comparing with conventional fuels, combustion systems fueled by hydrogen are also more prone to flame instability and abnormal combustion. This paper aims to provide a comprehensive review about combustion research related to hydrogen safety. It starts with a brief introduction which includes some overview about risk analysis, codes and standards. The core content covers ignition, fire, explosions and deflagration to detonation transition (DDT). Considering that DDT leads to detonation, and that detonation may also be induced directly under special circumstances, the subject of detonation is also included for completeness. The review covers laboratory, medium and large-scale experiments, as well as theoretical analysis and numerical simulation results. While highlights are provided at the end of each section, the paper closes with some concluding remarks highlighting the achievements and key knowledge gaps.

08 HYDROGEN↗

DOE OSTI2021

Rayleigh–Taylor and Richtmyer–Meshkov instabilities: A journey through scales

Hydrodynamic instabilities such as Rayleigh–Taylor (RT) and Richtmyer–Meshkov (RM) instabilities usually appear in conjunction with the Kelvin–Helmholtz (KH) instability and are found in many natural phenomena and engineering applications. They frequently result in turbulent mixing, which has a major impact on the overall flow development and other effective material properties. This can either be a desired outcome, an unwelcome side effect, or just an unavoidable consequence, but must in all cases be characterized in any model. The RT instability occurs at an interface between different fluids, when the light fluid is accelerated into the heavy. The RM instability may be considered a special case of the RT instability, when the acceleration provided is impulsive in nature such as that resulting from a shock wave. Here in this pedagogical review, we provide an extensive survey of the applications and examples where such instabilities play a central role. First, fundamental aspects of the instabilities are reviewed including the underlying flow physics at different stages of development, followed by an overview of analytical models describing the linear, nonlinear and fully turbulent stages. RT and RM instabilities pose special challenges to numerical modeling, due to the requirement that the sharp interface separating the fluids be captured with fidelity. These challenges are discussed at length here, followed by a summary of the significant progress in recent years in addressing them. Examples of the pivotal roles played by the instabilities in applications are given in the context of solar prominences, ionospheric flows in space, supernovae, inertial fusion and pulsed-power experiments, pulsed detonation engines and Scramjets. Progress in our understanding of special cases of RT/RM instabilities is reviewed, including the effects of material strength, chemical reactions, magnetic fields, as well as the roles the instabilities play in ejecta formation and transport, and explosively expanding flows. The article is addressed to a broad audience, but with particular attention to graduate students and researchers who are interested in the state-of-the-art in our understanding of the instabilities and the unique issues they present in the applications in which they are prominent.

42 ENGINEERING↗