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DOE OSTI2024

Density functional theory (DFT) study of UF 6 hydrolysis: reaction pathways, spectroscopy, and chemical kinetics

Depleted uranium hexafluoride (UF 6 ), a stockpiled byproduct of the nuclear fuel cycle, reacts readily with atmospheric humidity, but the gas-phase reaction mechanism and associated chemical kinetics are poorly understood. During the performance period we undertook development of a state-of-the-art ab initio gas-phase chemical kinetics simulation workflow to model the hydrolysis of uranium hexafluroride (UF 6 ). In doing so, we addressed several outstanding issues in the theoretical treatment of uranium-containing systems. At the outset it was unclear how to generate accurate estimates of kinetic and thermodynamic data for U-containing chemical reactions. Generation of such data has been made routine. Prior to our work, the literature associated with UF 6 hydrolysis were disparate and inaccurate. This body of work provides a modern and comprehensive theoretical assessment of the reaction mechanism, molecular clustering towards deposition, and chemical kinetics. New methodological implementations and software integrations resulting from this work are also highlighted. As much as possible, our predictions were validated against experimental data including particle morphologies, vibrational spectroscopy, atomization enthalpies, and kinetic rate constants. Nevertheless, we were unable to reconcile kinetic measurements with high-accuracy simulations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Nuclear-Driven Integrated Energy Systems: A State-of-the-Art Review

Because of the growing concerns regarding climate change and energy sustainability, a transition toward a modern energy sector that reduces environmental effects while promoting social and economic growth has gained traction in recent years. Sustainable energy solutions, which include renewable and low-carbon sources such as nuclear energy and natural gas, could minimize emissions of greenhouse gases, enhance air and water quality, and encourage energy independence. Yet, the shift to a sustainable energy industry is fraught with difficulties, including governmental and regulatory obstacles, technological and economic limits, and societal acceptability hurdles. Addressing these issues would necessitate the development of long-term, durable, and cost-effective energy systems containing nuclear energy and associated with the generation of both electricity and other by-products required by industry. Integrated energy systems (IES) are a novel way to maximize the use of various energy resources and technologies in order to deliver dependable, efficient, and sustainable energy services. IES entail the integration of various energy systems, such as electricity, heating, cooling, and transportation, in respect to energy sustainability and a system’s resilience and flexibility. Their development and implementation require the cooperation of several parties, including energy providers and policymakers. This study provides a state-of-the-art literature review of the most creative nuclear-driven hybrid energy system applications and methodologies, from which the research challenges and prospects for effective IES implementation emerge.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2020

Nearby Quintuple Systems κ Tucanae and ξ Scorpii

Architecture and parameters of two wide, nearby hierarchical systems containing five solar-type stars each, κ Tuc and ξ Sco, are studied. Using Gaia astrometry and photometry, masses are determined from visual orbits and isochrones, and effective temperatures from spectra or colors. Both systems are ∼2 Gyr old. Their spatial motion corresponds to a young disk but does not match any known kinematic group. Internal proper motions relative to the center of mass and radial velocities show that wide ∼8 kau outer pairs are bound. No correlation between orbit orientations in the inner subsystems is observed. All masses except one are confined to the narrow range from 0.8 to 1.5 solar. Strongly correlated masses and wide orbits can be explained if those systems formed by fragmentation in relative isolation and their components accreted gas from a common source, as expected in a hierarchical collapse. Young moving groups could be formed in similar environments, and many of them contain high-order hierarchies.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Evaluation of Safety Standards for Fuel System and Fuel Container Integrity of Alternative Fuel Vehicles

There are two Federal Motor Vehicle Safety Standards (FMVSS) in place that specify requirements for integrity of the fuel system and fuel container on compressed natural gas (CNG) fuel vehicles. These are FMVSS Nos. 303, “Fuel system integrity of compressed natural gas vehicles,” and FMVSS No. 304, “CNG fuel container integrity.” At this time, no FMVSS are defined for the fuel system and fuel container integrity of propane and liquefied natural gas (LNG) vehicles or fuel system integrity requirements for heavy-duty CNG vehicles on the road. However, there are voluntary industry design standards and best practices, as well as regulations defined in other countries. FMVSS No. 303 specifies requirements for the integrity of the CNG fuel system of light-duty vehicles and school buses, and FMVSS No. 304 specifies requirements for fuel container integrity on all CNG vehicles. FMVSS No. 304 applies to containers used for vehicle propulsion, whereas containers used to transport CNG and transportation of CNG containers are regulated by the DOT Pipeline and Hazardous Materials Safety Administration. FMVSS Nos. 303 and 304 are performance-based standards to consistently test and validate equipment and are not design restrictive. Despite the increasing number of natural gas and propane medium- and heavy-duty vehicles on the road, there are no FMVSS fuel system integrity requirements beyond light-duty and school buses for CNG vehicles and no FMVSS fuel system integrity requirements for propane vehicles. NHTSA is researching fuel system safety for medium- and heavy-duty natural gas and propane vehicles to update FMVSS Nos. 303 and 304. NHTSA is also researching current best practices and standards for high pressure fuel tanks in motor vehicles as they may apply to FMVSS No. 304.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2024

Automated Calibration for Rapid Optical Spectroscopy Sensor Development for Online Monitoring

An automated platform has been developed to assist researchers in the rapid development of optical spectroscopy sensors to quantify species from spectral data. This platform performs calibration and validation measurements simultaneously. Real-time, in situ monitoring of complex systems through optical spectroscopy has been shown to be a useful tool; however, building calibration models requires development time, which can be a limiting factor in the case of radiological or otherwise hazardous systems. While calibration time can be reduced through optimized design of experiments, this study approached the challenge differently through automation. The ATLAS (Automated Transient Learning for Applied Sensors) platform used pneumatic control of stock solutions to cycle flow profiles through desired calibration concentrations for multivariate model construction. Additionally, the transients between desired concentrations based on flow calculations were used as validation measurements to understand model predictive capabilities. This automated approach yielded an incredible 76% reduction in model development time and a 60% reduction in sample volume versus estimated manual sample preparation and static measurements. The ATLAS system was demonstrated on two systems: a three-lanthanide system with Pr/Nd/Ho representing a use case with significant overlap or interference between analyte signatures and an alternate system containing Pr/Nd/Ni to demonstrate a use case in which broad-band corrosion species signatures interfered with more distinct lanthanide absorbance profiles. Both systems resulted in strong model prediction performance (RMSEP < 9%). Lastly, ATLAS was demonstrated as a tool to simulate process monitoring scenarios (e.g., column separation) in which models can be further optimized to account for day-to-day changes as necessary (e.g., baseline correction). Ultimately, ATLAS offers a vital tool to rapidly screen monitoring methods, investigate sensor fusion, and explore more complex systems (i.e., larger numbers of species).

47 OTHER INSTRUMENTATION↗

DOE OSTI1988

Nuclear Safety [Vol. 29, No. 3, July-September 1988]

Nuclear Safety is a review journal that covers significant developments in the field of nuclear safety. Its scope includes the analysis and control of hazards associated with nuclear energy, operations involving fissionable materials, and the products of nuclear fission and their effects on the environment. Primary emphasis is on safety in reactor design, construction, and operation; however, the safety aspects of the entire fuel cycle, including fuel fabrication, spent-fuel processing, nuclear waste disposal, handling of radioisotopes, and environmental effects of these operations, are also treated. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 259 Fifteenth Water Reactor Safety Information Meeting by E. G. Silver; CONTROL AND INSTRUMENTATION: 284 Reliability Technology to Improve and/or Maintain Emergency Diesel Generator Performance by S. Karimian and J. H. Taylor, 293 A Noise Diagnostics System for Operator Advice by G. Hessel, P. Liewers, P. Schumann, W. Schmitt, and F.-P. Weiss; PLANT SAFETY FEATURES: 307 A Passive Containment System for Advanced Light-Water Reactors by O. B. Falls, Jr., and F. W. Kleimola; ENVIRONMENTAL EFFECTS: 318 Data Base Construction for a Computerized Radiological Risk Investigation System by L. M. Hively, J. E. Nyquist, J. L. Bledsoe, and A. L. Sjoreen, 326 Erratum to "Radiation Hormesis and Nuclear Safety," Vol. 29, No. 1; OPERATING EXPERIENCES: 327 Operational Safety Experience and Passive Safety Testing at the Fast Flux Text Facility by Q. L. Baird, J. L. Rathbun, D. D. Stepnewski, R. L. Stover, and A. E. Waltar, 344 Backfilling of Independent Residual Heat Removal Systems in West Germany and Switzerland by G. Eckert and Y. Salomon, 353 Reactor Shutdown Experience Compiled by J. W. Cletcher, 356 Selected Safety-Related Events Compiled by G. A. Murphy, 363 Operating U.S. Power Reactors Compiled by E. G. Silver; RECENT DEVELOPMENTS: 384 General Administrative Activities Compiled by E. G. Silver, 390 Reports, Standards, and Safety Guides by D. S. Queener, 395 Status of Power-Reactor Projects Undergoing Licensing Review Compiled by E. G. Silver, 400 Proposed Rule Changes as of Mar. 31,1988; ANNOUNCEMENTS: 283 International ENS/ANS Conference on Thermal Reactor Safety "NUCSAFE 88", 317 Northwestern University Short Course on Radiation Safety, 407 Second International Seminar on Small- and Medium-Sized Nuclear Reactors, 407 International Workshop on New Developments in Occupational Dose Control and ALARA Implementation at Nuclear Power Plants and Similar Facilities, 408 Fourth International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-4), 404 The Authors.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Identification of uncommon objects in containers

A system for identifying in an image an object that is commonly found in a collection of images and for identifying a portion of an image that represents an object based on a consensus analysis of segmentations of the image. The system collects images of containers that contain objects for generating a collection of common objects within the containers. To process the images, the system generates a segmentation of each image. The image analysis system may also generate multiple segmentations for each image by introducing variations in the selection of voxels to be merged into a segment. The system then generates clusters of the segments based on similarity among the segments. Each cluster represents a common object found in the containers. Once the clustering is complete, the system may be used to identify common objects in images of new containers based on similarity between segments of images and the clusters.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2022

Four new deeply eclipsing white dwarfs in Zwicky Transient Facility

ABSTRACT We present the results of a search for deeply eclipsing white dwarfs in the Zwicky Transient Facility (ZTF) Data Release 4 (DR4). We identify nine deeply eclipsing white dwarf candidates, four of which we followed up with high-cadence photometry and spectroscopy. Three of these systems show total eclipses in the ZTF data and our follow-up Apache Point Observatory 3.5 m telescope observations. Even though the eclipse duration is consistent with sub-stellar companions, our analysis shows that all four systems contain a white dwarf with low-mass stellar companions of ∼0.1 M⊙. We provide mass and radius constraints for both stars in each system based on our photometric and spectroscopic fitting. Finally, we present a list of 41 additional eclipsing WD+M candidates identified in a preliminary search of ZTF DR7, including 12 previously studied systems. We identify two new candidate short-period, eclipsing, white dwarf–brown dwarf binaries within our sample of 41 WD+M candidates based on Pan-STARRS colours.

Kosakowski, A. (ORCID:0000000298781647)↗

DOE OSTI2021

Rules of Use Report Engineering evaluations of nuclear material storage containers against the packaging requirements at TA-55

A set of obligations in the yearly storage container surveillance program, ensures that a retrospective approach is applied with loaded containers in inventory to confirm compliance with all “users” to ensure nuclear material storage container requirements are being followed. Validation that packaged containers are properly used, within a specific set of container types prescribed “bounding conditions of use,” is based on meeting requirements as identified in operating procedures associated with TA55-DOP-091, TA-55 Nuclear Material Packaging, and PA-RD-01022, Nuclear Material Packaging Requirements. The surveillance plan obligation requires the application of local area nuclear material accountability software or (LANMAS) to produce queries. The data queries are used to assess attributes of containers in storage these investigations are conducted on a bi-annual basis. This rules of use (ROU) compliance process ensures proper usage of storage containers as containment systems and therefore provides effective worker protection. It is structured as a supporting effort by implementing aspects of PA-AP-01207, Nuclear Material Container Safety Management at TA-55.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Engineering evaluations of nuclear material storage containers against the packaging requirements at TA-55 (FY22 Rules of Use Report)

36 MATERIALS SCIENCE↗

DOE OSTI2021

Parallel Battery: The Framework and Process for an Intelligent and Ecological Battery System and Related Services

The concept, framework, process methodology and applications of parallel battery were proposed from both virtual and real aspects.The parallel battery was an application of ACP-based parallel intelligence in battery and related energy system areas.The real battery system was running with its equivalent, and the artificial battery system was in a virtual space, in a parallel and interactive manner.The artificial battery system contained the descriptive, predictive, and prescriptive functions on the real battery and related energy systems.There was a closed-loop workflow between the real battery system and the artificial battery system, which iteratively optimizes the battery and related energy systems, leading to a new paradigm of intelligent and ecological parallel battery system management.

ACP approach↗

DOE OSTI2019

Ion–ion interactions enhance aluminum solubility in alkaline suspensions of nano-gibbsite (α-Al(OH) 3 ) with sodium nitrite/nitrate

Despite widespread industrial importance, predicting metal solubilities in highly concentrated, multicomponent aqueous solutions is difficult due to poorly understood ion–ion and ion–solvent interactions. Aluminum hydroxide solid phase solubility in concentrated sodium hydroxide (NaOH) solutions is one such case, with major implications for ore refining, as well as processing of radioactive waste stored at U.S. Department of Energy legacy sites, such as the Hanford Site, Washington State. The solubility of gibbsite (α-Al(OH) 3 ) is often not well predicted because other ions affect the activity of hydroxide (OH – ) and aluminate (Al(OH) 4 – ) anions. In the study reported herein, we systematically examined the influence of key anions, nitrite (NO 2 – ) and nitrate (NO 3 – ), as sodium salts on the solubility of α-Al(OH) 3 in NaOH solutions taking care to establish equilibrium from both under- and oversaturation. Rapid equilibration was enabled by use of a highly pure and crystalline synthetic nano-gibbsite of well-defined particle size and shape. Measured dissolved aluminum concentrations were compared with those predicted by an α-Al(OH) 3 solubility model derived for simple Al(OH) 4 – /OH – systems. Specific anion effects were expressed as an enhancement factor (Al enhc ) conveying the excess of dissolved aluminum. At 45 °C, NaNO 2 and NaNO 3 -containing systems exhibited Al enhc values of 2.70 and 1.88, respectively, indicating significant enhancement. The solutions were examined by Raman and high-field 27 Al NMR spectroscopy, indicating specific interactions including Al(OH) 4 – –Na + contact ion pairing and Al(OH) 4 – –NO 2 – /NO 3 – ion–ion interactions. Dynamic evolution of the α-Al(OH) 3 particles including growth and agglomeration was observed revealing the importance of dissolution/reprecipitation in establishing equilibrium. These studies indicate that incomplete ion hydration, as a result of the low water activity in these concentrated electrolytes, results in: (i) enhanced reactivity of the hydroxide ion with respect to α-Al(OH) 3 ; (ii) increased concentrations of Al(OH) 4 – in solution; and (iii) stronger ion–ion interactions that act to stabilize the supersaturated solutions. This information on the mechanisms by which α-Al(OH) 3 becomes supersaturated is essential for more energy-efficient aluminum processing technologies, including the treatment of millions of gallons of Al(OH) 4 – -rich high-level radioactive waste.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Raman Lidar (RL) Instrument Handbook

The Raman lidar at the ARM Climate Research Facility (ACRF) Southern Great Plains (SGP) Central Facility (SGPRL) is an active, ground-based laser remote sensing instrument that measures height and time resolved profiles of water vapor mixing ratio and several cloud- and aerosol-related quantities. The system is a non-commercial custom-built instrument developed by Sandia National Laboratories specifically for the ARM Program. It is fully computer automated, and will run unattended for many days following a brief (~5-minute) startup period. The self-contained system (requiring only external electrical power) is housed in a climate-controlled 8’x8’x20’ standard shipping container.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Multi-fluid, earth battery energy systems and methods

The present disclosure relates to a system for storing and time shifting at least one of excess electrical power from an electrical power grid, excess electrical power from the power plant itself, or heat from a heat generating source, in the form of pressure and heat, for future use in assisting with a production of electricity. An oxy-combustion furnace is powered by a combustible fuel source, plus excess electricity, during a charge operation to heat a reservoir system containing a quantity of a thermal storage medium. During a discharge operation, a discharge subsystem has a heat exchanger which receives heated CO 2 from the reservoir system and uses this to heat a quantity of high-pressure, supercritical CO 2 (sCO 2 ) to form very-high-temperature, high-pressure sCO 2 at a first output thereof. The very-high-temperature, high-pressure sCO 2 is used to drive a Brayton-cycle turbine, which generates electricity at a first output thereof for transmission to a power grid. The Brayton-cycle turbine also outputs a quantity of sCO 2 which is reduced in temperature and pressure to a heat recuperator subsystem. The heat recuperator subsystem circulates the sCO 2 and re-heats and re-pressurizes the sCO 2 before feeding it back to the heat exchanger to be even further reheated, and then output to the Brayton-cycle turbine as a new quantity of very-high-temperature, high-pressure sCO 2 , to assist in powering the Brayton-cycle turbine.

Buschek, Thomas A.↗

DOE OSTI2022

The high-pressure lithium-palladium and lithium-palladium-hydrogen systems

The lithium-palladium and lithium-palladium-hydrogen systems are investigated at high pressures at and above room temperature. Two novel lithium-palladium compounds are found below 18.7 GPa. An ambient temperature phase is tentatively assigned as $F\bar{4}3m$ Li 17 Pd 4 , with a = 17.661(1) Å at 8.64 GPa, isostructural with Li 17 Sn 4 . The other phase occurs at high-temperature and is $I\bar{4}3m$ Li 11 Pd 2 , a = 9.218(1) Å at 3.88 GPa and 200 °C, similar to Li 11 Pt 2 , which is also known at high pressure. The presence of hydrogen in the system results in an $I\bar{4}3m$ structure with a = 8.856(1) Å at 9.74 GPa. This persists up to 13.3 GPa, the highest pressure studied. Below 2 GPa an fcc phase with a large unit cell, a = 19.324(1) Å at 0.39 GPa, is also observed in the presence of hydrogen. On heating the hydrogen containing system at 4 GPa the $I\bar{4}3m$ phases persists to the melting point of lithium. In both systems melting the lithium results in the loss of crystalline diffraction from palladium containing phases. This is attributed to dissolution of the palladium in the molten lithium, and on cooling the palladium remains dispersed.

Frost, Mungo↗

DOE OSTI2019

Quantum engineered Kondo lattices

Abstract Atomic manipulation techniques have provided a bottom-up approach to investigating the unconventional properties and complex phases of strongly correlated electron materials. By engineering artificial systems containing tens to thousands of atoms with tailored electronic or magnetic properties, it has become possible to explore how quantum many-body effects emerge as the size of a system is increased from the nanoscale to the mesoscale. Here we investigate both theoretically and experimentally the quantum engineering of nanoscale Kondo lattices – Kondo droplets – exemplifying nanoscopic replicas of heavy-fermion materials. We demonstrate that by changing a droplet’s real-space geometry, we can not only create coherently coupled Kondo droplets whose properties asymptotically approach those of a quantum-coherent Kondo lattice, but also markedly increase or decrease the droplet’s Kondo temperature. Furthermore we report on the discovery of a new quantum phenomenon – the Kondo echo – a signature of droplets containing Kondo holes functioning as direct probes of spatially extended, quantum-coherent Kondo cloud correlations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2026

Effects of PLA/PHB Blend Ratio and Wood Flour Loading on the Melt Rheology and Thermomechanical Properties of Biobased Polymer Composites

The development of sustainable, biobased polymer composites is crucial for reducing supply chain dependence on fossil fuels. A major challenge lies in understanding and predicting the processability of these sustainable material alternatives, which directly impacts large-scale manufacturing. Here, this study systematically investigates the effect of poly(lactic acid) (PLA)/polyhydroxybutyrate (PHB) blend ratios and wood flour (WF) loadings on the thermal, rheological, and mechanical properties of the composites. Composites were prepared via melt compounding and characterized by using differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), oscillatory shear melt rheology, tensile testing, and scanning electron microscopy. Results showed that increasing the PHB content lowered the glass transition temperature, while higher PHB and WF loadings decreased thermal stability. Complex viscosity decreased with increasing PHB in 0 and 10% WF, whereas it increased in 20% and 30% WF for PHB-rich blends (80/20 and 70/30 PLA/PHB) due to stronger filler interactions with flexible PHB chains. At 30% WF, PHB-containing composites also showed elastic dominance with G′ higher than G″. This behavior was confirmed by van Gurp–Palmen plots, where the phase angle decreased with increasing PHB and WF loadings. WF addition also shifted Cole–Cole plots away from semicircular terminal relaxation, while time–temperature superposition validity was maintained, confirming that polymer chain dynamics continue to dominate melt behavior. Young’s modulus increased with WF loading, while tensile strength and toughness decreased due to weaker interfacial adhesion between the matrix and the filler. Interestingly, 10% WF systems containing PHB exhibited the highest toughness among all of the filled systems, indicating synergistic reinforcement from WF fillers and PHB-induced ductility. Overall, melt rheology effectively captured the internal structure and stiffness of the composites as the formulation changed, reinforcing the concept that the PLA/PHB ratio and WF content can be tuned to adjust melt elasticity and balance mechanical property trade-offs for targeted applications.

melt rheology↗

DOE OSTI2021

Dynamic Phasor Modeling of Multi-Converter Systems

Generalized form of Dynamic Phasor (DP)-based modeling of multi-converter systems containing high order harmonics has not been proposed in the literature yet due to the complexity and large number of variables that should be included in the model. In this work a generalized form of a system-level model comprising high number of single-phase converters is presented. The proposed method can be applied to any number of single-phase voltage source converters (VSIs). Test cases of this modeling method containing 5 to 100 parallel connected single-phase voltage source inverters are modeled and simulation times are recorded. The results of the proposed method are compared and validated with conventional average models as well as detailed switching models. A systematic approach for comparing the accuracy and timestep between dynamic phasor modeling method and detailed switching model is illustrated. Advantage of DP models over conventional average models for stability assessment are also discussed at the end of the paper.

Xue, Yaosuo↗