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At least 361 records · Page 20

Signature Analysis Utilizing a Dynamic Molten Salt Reactor Model for MC&A

Moving from traditional fixed fuel nuclear reactor systems to a mobile, dynamic fuel system that has dissolved special nuclear material in a molten salt is a paradigm shift in several respects. One major consideration is how to develop effective nuclear material controls and accounting for these novel reactor systems. The Molten Salt Reactor Experiment is one example of a critical molten salt system and provided a significant reference library based on the documented effort. But it was low thermal power that was not intended to reflect a commercial scale electricity production design. Therefore, to facilitate and assist vendors with domestic licensing considerations, research is underway to identify methods that could be used for domestic safeguards approaches for these novel reactor systems. This research presents the results of a signature analysis of data generated from three simulated scenarios using the molten salt demonstration reactor model defined in the Transient Simulation Framework of Reconfigurable Modules. Each scenario provides 1 hour isotope inventories over a 180 day period. The scenarios investigated provide test cases to examine if direct gamma-ray spectroscopy of the fuel can be used to identify changes comparing a base case (no reactivity control and fixed fission contribution) to an insertion of reactivity (10 pcm no change in fission composition) and a change in fission composition. The analysis demonstrates that monitoring the total count rate in a highly collimated high-resolution photon energy spectrum is sensitive to perturbations imposed into the reactor model. The total photon count rate changes ≈2% for the fission composition change and ≈4.5% for the reactivity insertion compared to the base case. However, both scenarios show an increase in the total photon count rate. The total photon count rate can be used to identify changes due to power (number of fissions) but not due to a change in the material undergoing fission. To distinguish between the two cases of increased power, the photon spectrum would require an intensive analysis technique. A photon peak count rate ratio analysis could be used to identify changes in the fissile material fission generation in the core through identification of a static peak that shows little variation to the source of fission and a highly varying peak. The photon peak strength will ultimately be determined by the isotope’s fission yield. A preliminary analysis investigating the coupling of the isotope’s fission yield and its concentration in the fuel salt derived from the modeling has been performed. A ratio analysis of the photon peak count rates of 140 La to 99 Mo demonstrated that the reactivity insertion creates a distinct difference in the ratio compared to the fission composition change scenario.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Refinement of Salt Dissolution Inhibitor Requirements (Final Report)

At Savannah River Site (SRS), High-Level Waste is stored in below-grade carbon steel tanks. This waste in part consists of sludge, salt cake, and/or supernate. Preparation of this waste for future processing involves dissolution of the salt cake layer. The salt dissolution process can create conditions that leave the carbon steel tanks susceptible to localized corrosion. The salt to be dissolved contains high concentrations of nitrate, that once released, create an environment that may be conducive to pitting corrosion and/or stress corrosion cracking (SCC) of carbon steel. The salt dissolution process also liberates interstitial liquid trapped between the salt crystals. This liquid is initially high in nitrite and hydroxide concentration. High pH and greater ratios of nitrite to nitrate act as inhibitors to minimize corrosion of carbon steel in high nitrate environments. However, as dissolution proceeds, the concentration of nitrate will increase, while the hydroxide and nitrite concentration of the interstitial liquid will deplete and become insufficient to prevent the onset of corrosion attack. Tank blending and addition of inhibitors are used to ensure adequate concentrations of hydroxide and nitrite. However, this is not desirable during salt dissolution as it can reduce process efficiency and increase the amount of waste that needs processing. It has been proposed that these corrosion control limits be revisited to evaluate the corrosion susceptibility of carbon steel in environments that more closely resemble current operating conditions at SRS. An experimental matrix was designed to evaluate the use of the pitting factor for supernate chemistries characteristic to SRS, particularly during the salt dissolution process. Two electrochemical methods were identified to determine the susceptibility of A537 and A285 low-carbon steels to pitting corrosion with this chemistry envelope at temperatures up to 75 °C. The predominant electrochemical test method was Cyclic Potentiodynamic Polarization (CPP) studies. Through CPP, the pitting factor was used, based on Hanford Site corrosion studies, to accurately identify pitting susceptibility within the compositional range studied with some conservatism. Additionally, sulfate was determined to have no statistically significant influence, at concentrations up to 0.6 M, on pitting behavior in more concentrated solutions where other aggressive species govern pitting susceptibility. Where CPP was inconclusive, Modified ASTM G192 was successfully used to evaluate pitting susceptibility conditions and allowed for a pass/fail result to be determined. In all cases, the pitting factor was determined to be applicable to the simulants tested, with this metric accurately predicting incidences in which pitting occurred. Based upon the findings in this work, a pitting factor of 1.2 is being proposed to build in a safety factor and remain consistent with the Hanford Site approach. Additionally, a minimum pH limit of 12 is proposed to ensure carbon steel passivity and localized corrosion the primary degradation mechanism. Susceptibility to SCC was evaluated using a reduced matrix of tests at 75 °C. No failures due SCC were observed at open circuit. In addition, tests polarized anodically by 200 mV only resulted in failures for trials with pitting factors less than 0.86. However, a test with a passing condition based upon the pitting factor metric (pitting factor = 1.40) did exhibit a failure with an applied potential of +300 mV vs. OCP. This result is contrary to the prediction based upon the pitting factor, however, a polarization of 300 mV, or even 200 mV, from open circuit is substantial. The relationship between these testing parameters and service environment/conditions and the desired level of conservatism in the metric should be further evaluated in the determination of the significance of this result. While the pitting factor accurately predicted susceptibility to SCC at temperatures up to 75 °C and with positive overpotentials up to 200 mV, the relatively small sample matrix and failure of a passing pitting factor with a 300 mV polarization resulted in an inconclusive determination of whether the pitting factor may be used for predicting susceptibility to SCC at temperatures between 50 °C and 75 °C. As such, additional testing is recommended to evaluate the validity of the pitting factor for SCC susceptibility prediction at temperatures between 50 °C and 75 °C.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Slow Strain Rate Testing of A537 Tank Wall Material

At Savannah River Site (SRS), High-Level Waste is stored in below-grade carbon steel tanks. This waste in part consists of sludge, salt cake, and/or supernate. Preparation of this waste for future processing involves dissolution of the salt cake layer. The salt dissolution process can create conditions that leave the carbon steel tanks susceptible to localized corrosion. The salt to be dissolved contains high concentrations of nitrate, that once released, create an environment that may be conducive to pitting corrosion and/or stress corrosion cracking (SCC) of carbon steel. The salt dissolution process also liberates interstitial liquid trapped between the salt crystals. This liquid is initially high in nitrite and hydroxide concentration. High pH and greater ratios of nitrite to nitrate act as inhibitors to minimize corrosion of carbon steel in high nitrate environments. However, as dissolution proceeds, the concentration of nitrate will increase, while the hydroxide and nitrite concentration of the interstitial liquid will deplete and become insufficient to prevent the onset of corrosion attack. Tank blending and the addition of inhibitors are used to ensure adequate concentrations of hydroxide and nitrite. However, this is not desirable during salt dissolution as it can reduce process efficiency and increase the amount of waste that needs processing. This testing program was designed to examine the risk of SCC associated with utilizing the pitting factor (PF) and nitrite/nitrate (NO 2 - /NO 3 - ) ratio limits for handling dissolved salt solutions at an elevated temperature in the carbon steel waste tanks. The previously identified limits are a PF of 1.2 and an NO 2 - /NO 3 - ratio of 0.15. The results indicate that as long as the NO 2 - /NO 3 - ratio exceeds 0.1 and the PF is above approximately 0.8, there is a discernible safety margin between the open circuit potential (OCP) and the critical cracking potential (CCP) observed during applied potential testing. However, this margin, defined by the difference between the OCP and CCP, is relatively narrow, ranging from 0.1 to 0.25 volts. This small margin raises concerns about potential shifts in OCP during waste retrieval operations, which could inadvertently increase the risk of SCC if the OCP approaches or exceeds the CCP. These results confirm that dissolved salt solutions provide a potent chemistry that, under certain conditions, makes carbon steel susceptible to SCC. The next question to consider is the influence these results have on decisions for storage and retrieval of waste from the tanks. For Type III/IIIA waste tanks, the risk of SCC remains very low. First, and most importantly, the post-weld stress relief of the tanks has reduced the residual stress near the welds. Thus, without the stress component, SCC risk is minimized. The material of construction (A537 Carbon steel) for the Type III/IIIA tanks is superior to the steel in its resistance to SCC than the steel that was utilized for the Type I, II, and IV tanks (A285 carbon steel). From a chemistry control standpoint for a Type III/IIIA tank directly involved with handling dissolved salt solutions, the PF and NO 2 - /NO 3 - ratio limits may be utilized wherein chemistry control provides an extra layer of defense against SCC. Chemistry control for a Type III/IIIA tank minimizes the risk for a tank that may receive the dissolved salt solution, particularly if that tank is a Type I, II, or IV waste tank. On the other hand, if the dissolved salt solution is handled by a Type I, II, or IV waste tank the risk of SCC is real. The potent chemistry, absence of stress relief, and inferior material result in a condition that is conducive to cracking. Efforts should be made to either avoid transferring waste that may not meet the PF and NO 2 - /NO 3 - ratio criteria to one of these tanks or if it is unavoidable, take measures to minimize the consequences of a leak. As shown by these tests, even if the PF and NO 2 - /NO 3 - ratio criteria are met, there is a risk that the tank potential may be disturbed in the positive direction and the risk of SCC increase.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Synthesis and characterization of uranium trichloride in alkali-metal chloride media

Given a growing interest in uranium salts for pyrochemical processing of used fuel and uranium-fueled molten salt reactors, the synthesis of uranium trichloride in alkali-metal chloride media was investigated in a series of four experiments. Specifically, uranium metal powder and uranium hydride powder were prepared and separately blended with ammonium chloride and lithium chloride – potassium chloride eutectic in two runs, while the same powders were separately blended with ammonium chloride and sodium chloride in two additional runs. Each of the lithium chloride – potassium chloride containing blends was slowly heated to 923 K, while those containing sodium chloride were heated to 1123 K. During each heat up, the ammonium chloride sublimed into gaseous ammonia and hydrogen chloride, leading to the chlorination of uranium metal or uranium hydride and the formation of molten salt solutions of the respective chlorides. Experimental conditions were incorporated in the runs to promote formation of uranium trichloride over uranium tetrachloride in the respective media. Molten samples of each run product were taken and characterized via chemical analyses, diffractometry, and microscopy. The final products from each run were dark dense ingots of the respective salt systems with uranium concentrations ranging from 44 to 51 wt%. Finally, chemical analyses and diffractometry identified the predominant presence of uranium trichloride in these systems; however, a possible minor presence of uranium tetrachloride could not be conclusively dismissed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Structure of Diisobutylene Maleic Acid Copolymer (DIBMA) and Its Lipid Particle as a “Stealth” Membrane-Mimetic for Membrane Protein Research

The study of membrane proteins remains challenging, especially in a native membrane environment. Recently, major progress has been made using maleic acid copolymers, such as styrene maleic acid, to purify membrane proteins and study them directly with native lipids associated with the membrane. Additional maleic acid copolymers, such as diisobutylene maleic acid (DIBMA) membrane-mimetic systems, are being developed and found to have improved spectroscopic properties and pH stability. We studied DIBMA and its lipid particles in solution to better understand its assembly, without and with the lipids, to provide an insight regarding how to use it in solution for better membrane extraction. Using small-angle neutron and X-ray scattering (SANS/SAXS), we show that DIBMA organizes into structures of different size scales at various concentrations and ionic strengths. The polymer performed reasonably well under most solvent conditions except in very low concentrations and high-salt conditions that could result in limited interaction with lipids. To explore DIBMA lipid particles as a suitable membrane-mimetic system for neutron scattering studies of membrane proteins, we measured and determined the contrast-matching point of DIBMA to be ~12% (v/v) D 2 O — similar to that of most protiated lipid molecules but distinct from that of regular protiated proteins — providing a natural contrast for separating their neutron scattering signals. Using SANS contrast variation, we demonstrated that the scattering from the whole lipid particle can be annihilated. Further, we determined that a well-defined lipid nanodisc structure with DIBMA was contrast-matched. These results demonstrate that the DIBMA lipid particle is an outstanding “stealth” membrane-mimetic for membrane proteins. The results provide a structural framework for understanding the organization and assembly process of the polymer itself and the lipid molecules. Such an understanding is imperative for structural techniques such as cryo-electron microscopy, nuclear magnetic resonance, small-angle scattering, and other biophysical techniques.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Molecular design for electrolyte solvents enabling energy-dense and long-cycling lithium metal batteries

Electrolyte engineering is critical for developing Li metal batteries. While recent works improved Li metal cyclability, a methodology for rational electrolyte design remains lacking. In this study, we propose a design strategy for electrolytes that enable anode-free Li metal batteries with single-solvent single-salt formations at standard concentrations. Rational incorporation of –CF 2 – units yields fluorinated 1,4-dimethoxylbutane as the electrolyte solvent. Paired with 1 M lithium bis(fluorosulfonyl)imide, this electrolyte possesses unique Li–F binding and high anion/solvent ratio in the solvation sheath, leading to excellent compatibility with both Li metal anodes (Coulombic efficiency ~ 99.52% and fast activation within five cycles) and high-voltage cathodes (~6 V stability). Fifty-μm-thick Li|NMC batteries retain 90% capacity after 420 cycles with an average Coulombic efficiency of 99.98%. Industrial anode-free pouch cells achieve ~325 Wh kg –1 single-cell energy density and 80% capacity retention after 100 cycles. Our design concept for electrolytes provides a promising path to high-energy, long-cycling Li metal batteries.

25 ENERGY STORAGE↗

Insights into lithium ion deposition on lithium metal surfaces

Lithium metal is among the most promising anodes for the next generation of batteries due to its high theoretical energy density and high capacity. Challenges such as extreme reactivity and lithium dendrite formation have kept lithium metal anodes away from practical applications. However, the underlying mechanisms of Li ion deposition from the electrolyte solution onto the anode surface are still poorly understood due to their inherent complexity. In this work, density functional theory calculations and thermodynamic integration via constrained molecular dynamics simulations are conducted to study the electron and ion transfer between lithium metal slab and the electrolyte in absence of an external field. Here, we explore the effect of the solvent chemistry and structure, distance of the solvated complex from the surface, anion–cation separation, and concentration of Li-salts on the deposition of lithium ions from the electrolyte phase onto the surface. Ethylene carbonate (EC), 1,2-dimethoxyethane (DME), 1,3-dioxolane (DOL), and mixtures of them are used as solvents. These species compete with the salt anion and the Li cation for electron transfer from the surface. It is found that the structure and properties of the solvation shell around the lithium cation has a great influence on the ability of the cation to diffuse as well as on its surrounding electron environment. DME molecules allow easier motion of the lithium ion compared with EC and DOL molecules. The slow growth approach allows the study of energy barriers for the ion diffusion and desolvation during the deposition pathway. This method helps elucidating the underlying mechanisms on lithium-ion deposition and provides a better understanding of the early stages of Li nucleation.

25 ENERGY STORAGE↗

Fabrication, Modeling, and Testing of a Prototype Thermal Energy Storage Containment

Increasing penetration of variable renewable energy resources requires the deployment of energy storage at a range of durations. Long-duration energy storage (LDES) technologies will fulfill the need to firm variable renewable energy resource output year round; lithium-ion batteries are uneconomical at these durations. Thermal energy storage (TES) is one promising technology for LDES applications because of its siting flexibility and ease of scaling. Particle-based TES systems use low-cost solid particles that have higher temperature limits than the molten salts used in traditional concentrated solar power systems. A key component in particle-based TES systems is the containment silo for the high-temperature (>1100 degrees C) particles. This study combined experimental testing and computational modeling methods to design and characterize the performance of a particle containment silo for LDES applications. A laboratory-scale silo prototype was built and validated the congruent transient finite element analysis (FEA) model. The performance of a commercial-scale silo was then characterized using the validated model. The commercial-scale model predicted a storage efficiency above 95% after 5 days of storage with a design storage temperature of 1200 degrees C. Insulation material and concrete temperature limits were considered as well. The validation of the methodology means the FEA model can simulate a range of scenarios for future applications. This work supports the development of a promising LDES technology with implications for grid-scale electrical energy storage, but also for thermal energy storage for industrial process heating applications.

clean energy↗

Fabrication, Modeling, and Testing of a Prototype for Particle Thermal Energy Storage Containment

Increasing penetration of variable renewable energy resources requires the deployment of energy storage at a range of durations. Long-duration energy storage (LDES) technologies will fulfill the need to firm variable renewable energy resource output throughout the year. Conventional electrochemical batteries (e.g., lithium-ion) are uneconomical in this role due to high energy capacity costs. Thermal energy storage (TES) is one promising technology for LDES applications because of its siting flexibility and ease of scaling. Particle-based TES systems use low-cost solid particles that have higher temperature limits than the molten salts used in traditional concentrated solar power systems. A key component in particle-based TES systems is the containment silo for the high-temperature (> 1100 degrees C) particles. This study combined experimental testing and computational modeling methods to design and characterize the performance of a particle containment silo for LDES applications. A containment silo prototype was built at a laboratory scale and used to validate a congruent transient finite element analysis (FEA) model. The validation compared the actual and predicted temperature profile through the prototype over six days as the particles cooled from their initial temperature. The performance of a commercial scale (> 5 GWhth) was then characterized using the validated model. The transient FEA model was subject to several charge-discharge cycles to mimic a possible operating schedule. The commercial-scale model predicted a storage efficiency in excess of 95% after five days of storage with a design storage temperature of 1200 degrees C. Insulation material and concrete temperature limits were considered as well. The validation of the methodology means the FEA model can simulate a range of scenarios for future applications. This work supports the development of a promising LDES technology with implications for grid-scale electrical energy storage, but also for thermal energy storage for industrial process heating applications.

ENERGY STORAGE↗

Technology Strategy Assessment: Findings from Storage Innovations 2030 Bidirectional Hydrogen Storage

Hydrogen is the most common element in the universe, comprising nearly 75% of all normal matter, and it has been used by scientists for centuries, but it was not fully recognized as an element until 1766, when it was isolated by Henry Cavendish. Early work focused on the generation of hydrogen through the oxidation of metals in water, which released hydrogen gas. Hydrogen’s lighter-than-air and flammable properties were immediately used in engines, zeppelins, and as feedstock for a wide variety of chemical reactions. Several approaches were developed for the production of hydrogen with the most common being associated with the production and conversion of hydrocarbon-based fuels. Coal gasification, steam methane reforming, and other reformation processes provide the majority of current hydrogen production due to the relatively low cost of hydrogen produced through these processes. More than 95% of hydrogen production is used for industrial processes rather than energy storage. To facilitate affordable decarbonization of these industrial processes and to advance the use of hydrogen as a fuel in transportation, DOE launched the Hydrogen Shot as part of the Energy Earthshots Initiative. The goal of the Hydrogen Shot is to reduce the cost of clean hydrogen by 80% to $1/kg of clean hydrogen production within one decade (known as the “1 1 1” goal). This is distinct from the Long-Duration Storage Shot, which is the primary focus of this report; however, it is intrinsically linked to bidirectional hydrogen storage. Several important chemical synthesis processes are dependent upon hydrogen, and the production and use of hydrogen is generally driven by its connection to one of these markets. For example, ammonia is one of the most highly produced chemicals in the world and it depends chiefly on hydrogen. Ammonia is primarily used for agricultural fertilizer and is considered to be largely responsible for a doubling of agricultural production per unit of land over the last century. Another one of hydrogen’s primary uses is as a catalyst in petroleum refining during the desulfurization process. Beyond chemical production, hydrogen is used as a reductant in the production of steel and has been demonstrated as a substitute for metallurgical coal in the production of raw iron. It is even used in the hydrogenation reaction for food products to create more shelf-stable semi-solid fats. However, while hydrogen is produced on the order of 100 million metric tons/year globally to feed these industries, more than 95% of hydrogen is produced from hydrocarbons that emit CO2 during the process. Conversely, electrolysis is a process by which electricity is used to separate hydrogen and oxygen in water molecules, usually across a membrane. Hydrogen production via electrolysis lowers the carbon intensity of produced hydrogen when coupled with low-carbon electricity. Currently, global electrolysis capacity is on the order of 1 GW, which equates to about 500 metric tons/day of hydrogen production. To support large-scale industrial decarbonization, capacity will likely need to increase by two to three orders of magnitude. Electrolysis technology is broadly separated into groups that are defined by the electrolyte used, with further subdivision based on the operating characteristics. The majority of commercial electrolyzer systems are based around three main technology groups: liquid alkaline, proton exchange membrane, and solid oxide. Liquid Alkaline (LA) electrolysis is the oldest, most mature, least expensive, and most common commercial technology, with 400 plants in operation by 1902. Its hydrogen output is low relative to the size of the system due to a low current density. LA electrolysis utilizes a liquid potassium hydroxide solution as the electrolyte. Proton exchange membrane (PEM) electrolysis (also known as polymer electrolyte membrane electrolysis), described in 1960, relies on an acid-impregnated polymer membrane as the electrolyte and typically offers three to six times higher hydrogen production per unit cell area than LA electrolysis. Solid oxide electrolysis, or high-temperature electrolysis, utilizes a ceramic cell as the electrolyte and operates on steam rather than liquid water, enabling electrical efficiencies of more than 90%, which is up from 60% with PEM. Two pre-commercial electrolyzer technologies to note are alkaline exchange membrane (AEM) and proton-conducting solid oxide electrolysis cell (SOEC). AEM potentially has the advantages of both LA and PEM technologies in that it is able to use low-cost materials like LA but with the ability to operate at higher output pressures with a smaller footprint like PEM. Proton-conducting SOEC is similar to commercial SOEC, which uses an oxide-conducting ceramic; however, it uses a proton-conducting ceramic that has the potential to operate at lower temperatures and has lower capital costs. Each of these technologies is experiencing a rapid improvement in performance and a reduction in installed cost, and each appears to be well suited to specific applications. Besides differences in the type of electrolyzer used, the main difference in the architecture of bidirectional hydrogen systems is how the hydrogen is stored. Currently, the most cost-effective way to store large amounts of hydrogen gas is underground, such as in large salt caverns that have been hollowed out. These salt caverns are geographically concentrated in small portions of the United States and are not generally near large metropolitan areas; however, other subsurface architectures are being investigated to expand this reach. A more widely deployable option is aboveground pressurized tanks. These systems are about 10 times as expensive because of the materials and safety margins required to hold hydrogen at high pressures. A third option is using materials-based storage, such as liquid organic hydrogen carriers. By reversibly attaching the produced hydrogen to other molecules, it can be stored at near atmospheric pressure and room temperature. This has the potential to reduce the material cost of storage but may result in a reduction in the efficiency of the process because there are both hydrogen uptake and release processes. While materials-based storage has not been used extensively for large-scale hydrogen storage in the past, there is currently significant activity regarding developing materials and processes for use in large-scale hydrogen storage applications. Electrolysis-produced hydrogen offers an unusual opportunity for energy storage applications. Unlike more conventional energy storage approaches, such as batteries, which operate entirely within electrical markets, hydrogen is a valuable product beyond the electric market and can be directed to the most lucrative use. Hydrogen also can be directly converted back to electricity using either a fuel cell or turbine, or it can be sold to other markets, such as chemical synthesis, steel production, or even export. In this way, excess electricity can be upgraded to the most valuable product. Finally, its use can be actively managed between multiple off-takers; for example, local hydrogen storage can provide a specific amount of stored electricity and any excess can be exported to ammonia production. This flexibility is amplified by the fact that hydrogen storage has fully decoupled power and energy components, which allows for affordable scaling options. Together, this allows a substantial amount of creativity to enable the economic utilization of variable power resources while supporting decarbonization of the industry.

08 HYDROGEN↗

Synthesis and characterization of uranium trichloride in alkali-metal chloride media

Given a growing interest in uranium salts for pyrochemical processing of used fuel and uranium-fueled molten salt reactors, the synthesis of uranium trichloride in alkali-metal chloride media was investigated in a series of four experiments. Specifically, uranium metal powder and uranium hydride powder were prepared and separately blended with ammonium chloride and lithium chloride – potassium chloride eutectic in two runs, while the same powders were separately blended with ammonium chloride and sodium chloride in two additional runs. Each of the lithium chloride – potassium chloride containing blends was slowly heated to 923 K, while those containing sodium chloride were heated to 1123 K. During each heat up, the ammonium chloride sublimed into gaseous ammonia and hydrogen chloride, leading to the chlorination of uranium metal or uranium hydride and the formation of molten salt solutions of the respective chlorides. Experimental conditions were incorporated in the runs to promote formation of uranium trichloride over uranium tetrachloride in the respective media. Molten samples of each run product were taken and characterized via chemical analyses, diffractometry, and microscopy. The final products from each run were dark dense ingots of the respective salt systems with uranium concentrations ranging from 44 to 51 wt%. Chemical analyses and diffractometry identified the predominant presence of uranium trichloride in these systems; however, a possible minor presence of uranium tetrachloride could not be conclusively dismissed.

D Herrmann, Steven↗

Integration of Nuclear Material Accounting Data and Process Monitoring Data for Improvement on Detection Probability in Safeguarding Electrochemical Processing Facilities (Final Technical Report)

The KAERI advanced spent fuel conditioning process (ACP) process is a critical component of the US- South Korean nuclear cooperation and the following “123 Agreement.” Its development has received considerable attention in both countries. The ACP is an electrochemical processing (pyroprocessing) that recycles over 96% of the used nuclear fuel (UNF). It is also intrinsically proliferation-resistant in theory. In normal operation, the U/TRU product is very hot radiologically. In addition, the Cm provides a high level of spontaneous neutrons, making the product unsuitable for weapon use. However, as pointed in some study, “the need for safeguards to protect against the diversion and misuse of separated plutonium applies essentially equally to all grades of plutonium.” As pointed by many studies, the well-established traditional Nuclear Material Accounting (NMA) approach cannot be directly applied to electrochemical processing because of the lack of an input accountability tank, the non-continuous material flow, and the unsatisfactory level of confidence in sampling methods. Therefore, nuclear safeguards remain a grand challenge in the developing of commercial electrochemical separations facilities, especially around the heart of such facilities, the electrorefiner (ER) systems. In contrast to NMA data, process monitoring (PM) data is normally an indirect measurement of the SNM and is acquired much more frequently. In a broad sense, PM includes monitoring by various types of equipment, e.g. radiation detectors, cameras, voltage, current sensors. Because it is already being collected by the operator, the additional cost to safeguards is low. It has long been believed that PM data can supplement NMA data and help improve safeguards, although the benefits are hard to quantify. The U.S. DOE’s Material Protection, Accounting, and Control Technology (MPACT) campaign has made substantial investments into innovative PM sensor technology and predictive model development for real- or near real-time measurement and prediction of molten salt density and level, salt composition and actinide concentration especially Pu, the cell voltage, and the cell current to supplement traditional NMA. For aqueous-based reprocessing facilities, it is reported that PM, integrated with traditional NMA, have a high detection probability for specific diversions. For electrochemical reprocessing, preliminary studies have shown that PM data can support traditional NMA in various ways by providing a basis to estimate some of the in-processing nuclear material inventories. Despite early success, further studies on fusion of PM data and NMA data are still needed, which is the goal of this proposed work.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Development of High Temperature (>700°C) molten Salt Pump Technology for Gen3 Solar Power Tower Systems

Generation 3 Concentrating Solar Power (CSP) Systems require thermal energy storage that can efficiently receive solar heat and deliver it to a working fluid at temperatures greater than 700°C. For liquid systems, the thermal transfer fluid must be phase stable over large temperature ranges. High temperature molten salts meet this criteria, but are difficult liquids to handle. The high heat and salt content can be very corrosive to several different materials that are wetted by the liquid salt. For power tower collectors, the molten salt must be pumped under high pressure to the top of the collector tower. These pumps have impellers and shafts as part of their rotating elements, and under load, require bearings to control shaft movement while rotating. These high temperature pumps require submerged bearings, and thus bearing materials that can withstand the temperature and molten salt contact over long periods of time. This is essential for keeping pump maintenance costs low, and downtime to a minimum. Long running bearing materials is an enabling technology for integrated liquid systems in Generation 3 CSP Systems. Keeping costs low and systems reliable are critical for the broad adoption of Gen 3 CSP Systems. Hayward Tyler, Inc (HTI) proposed development of journal bearing materials for use in vertical pumps designed for pumping high temperature molten salt on both the hot and cold sides of the solar power tower. To complete this objective, HTI utilized the testing capabilities of Oak Ridge National Laboratory (ORNL) and High Temperature System Design (HTSD). Materials would first be selected for static corrosion testing, then downselected for tribological testing. Successful tribologically tested materials would then be downselected for use in additional test regimes. Ten samples were selected for static corrosion testing. Three passed the static testing regime. Two of these materials were downselected for ball material in tribological testing against three metallic alloys: Sintered Y2O3 Partially Stabilized Zirconia YTZP and Silicon Nitride, Grade 147-31N. HTI also proposed collecting data from a thorough bearing test regime using a test rig designed and built as part of this project, and also a conceptual design for a high temperature molten salt vertical pump. HTI withdrew from the project prior to completion of this work and this report reflects only the work completed prior to withdrawal. The completed work produced two papers, one manuscript submitted for publication, and one paper published in the journal Solar Energy Materials and Solar Cells. The papers are: “Tribological behavior of ceramic-alloy bearing contacts in molten salt lubrication for concentrating solar power” and “Material Selection and Corrosion Studies Of Candidate Bearing Materials For Use In Molten Chloride Salt."

14 SOLAR ENERGY↗

Refinement of Salt Dissolution Inhibitor Requirements (Interim Report)

At Savannah River Site, High-Level Waste is stored in below-grade carbon steel tanks. This waste in part consists of sludge, salt cake, and/or supernate. Preparation of this waste for future processing involves dissolution of the salt cake layer. The salt dissolution process can create conditions that leave the carbon steel tanks susceptible to localized corrosion. The salt to be dissolved contains high concentrations of nitrate, that once released, create an environment that may be conducive to pitting corrosion or stress corrosion cracking (SCC) of carbon steel. The salt dissolution process also liberates interstitial liquid trapped between the salt crystals. This liquid is initially high in nitrite and hydroxide concentration. High pH and greater ratios of nitrite to nitrate act as inhibitors to minimize corrosion of carbon steel in high nitrate environments. However, as dissolution proceeds, the concentration of nitrate increases while the hydroxide and nitrite concentration of the interstitial liquid depletes and becomes insufficient to prevent the onset of corrosion attack. While tank blending and the addition of inhibitors are used to ensure adequate concentrations of hydroxide and nitrite during normal operation, this is not desirable during salt dissolution as it can reduce process efficiency and increase the amount of waste that needs processed.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Concentration-dependent ion correlations impact the electrochemical behavior of calcium battery electrolytes.

Ion interactions strongly determine the solvation environments of multivalent electrolytes even at concentrations below that required for practical battery-based energy storage. This statement is particularly true of electrolytes utilizing ethereal solvents due to their low dielectric constants. These solvents are among the most commonly used for multivalent batteries based on reactive metals (Mg, Ca) due to their reductive stability. Recent developments in multivalent electrolyte design have produced a variety of new salts for Mg2+ and Ca2+ that test the limits of weak coordination strength and oxidative stability. Such electrolytes have great potential for enabling full-cell cycling of batteries based on these working ions. However, the ion interactions in these electrolytes exhibit significant and non-intuitive concentration relationships. In this work, we investigate a promising exemplar, calcium tetrakis(hexafluoroisopropoxy)borate (Ca(BHFIP)(2)), in the ethereal solvents 1,2-dimethoxyethane (DME) and tetrahydrofuran (THF) across a concentration range of several orders of magnitude. Surprisingly, we find that effective salt dissociation is lower at relatively dilute concentrations (e.g. 0.01 M) than at higher concentrations (e.g. 0.2 M). Combined experimental and computational dielectric and X-ray spectroscopic analyses of the changes occurring in the Ca2+ solvation environment across these concentration regimes reveals a progressive transition from well-defined solvent-separated ion pairs to de-correlated free ions. This transition in ion correlation results in improvements in both conductivity and calcium cycling stability with increased salt concentration. Comparison with previous findings involving more strongly associating salts highlights the generality of this phenomenon, leading to important insight into controlling ion interactions in ether-based multivalent battery electrolytes.

Hahn, Nathan T.↗

Performance of alloy 600 in flowing commercial Cl salt at 600°-750°C

For the next generation of concentrating solar power (CSP) plants, K-Mg-Na chloride salts are being explored as a potential higher temperature thermal storage medium. However, there are concerns about compatibility of structural alloys with the salt. To move beyond simple static pot compatibility experiments while a pumped salt loop is being constructed, thermal convection loops were constructed from ~16wt.%Cr Ni-based alloy 600 and operated for 100-1000 h with peak temperatures of 700° and 750°C. These experiments indicated that alloy 600 was compatible up to 700°C with purified (i.e. low O2-) or dried (low H2O) industrial-sourced Mg-K-Na chloride salt with <10 µm/yr loss. Mass transfer was observed from the hot leg to the cold leg in each experiment and more surface deposits were observed with the dried salt. Post-exposure room temperature tensile tests showed minimal degradation of alloy 600 under these conditions.

Pint, Bruce↗

Elucidating the Transition of 3D Morphological Evolution of Binary Alloys in Molten Salts with Metal Ion Additives

Molten salts serve as effective high-temperature heat transfer fluids and thermal storage media used in a wide range of energy generation and storage facilities, including concentrated solar power plants, molten salt reactors and high-temperature batteries. However, at the salt–metal interfaces, a complex interplay of charge-transfer reactions involving various metal ions, generated either as fission products or through corrosion of structural materials, takes place. Simultaneously, there is a mass transport of ions or atoms within the molten salt and the parent alloys. The precise physical and chemical mechanisms leading to the diverse morphological changes in these materials remain unclear. Here, to address this knowledge gap, this work employed a combination of synchrotron X-ray nanotomography and electron microscopy to study the morphological and chemical evolution of Ni-20Cr in molten KCl-MgCl 2 , while considering the influence of metal ions (Ni 2+ , Ce 3+ , and Eu 3+ ) and variations in salt composition. Our research suggests that the interplay between interfacial diffusivity and reactivity determines the morphological evolution. The summary of the associated mass transport and reaction processes presented in this work is a step forward toward achieving a fundamental comprehension of the interactions between molten salts and alloys. Overall, the findings offer valuable insights for predicting the diverse chemical and structural alterations experienced by alloys in molten salt environments, thus aiding in the development of protective strategies for future applications involving molten salts.

36 - MATERIALS SCIENCE↗

Cation valency in water-in-salt electrolytes alters the short- and long-range structure of the electrical double layer

Highly concentrated aqueous electrolytes (termed water-in-salt electrolytes, WiSEs) at solid-liquid interfaces are ubiquitous in myriad applications including biological signaling, electrosynthesis, and energy storage. This interface, known as the electrical double layer (EDL), has a different structure in WiSEs than in dilute electrolytes. Here, we investigate how divalent salts [zinc bis(trifluoromethylsulfonyl)imide, Zn(TFSI) 2 ], as well as mixtures of mono- and divalent salts [lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) mixed with Zn(TFSI) 2 ], affect the short- and long-range structure of the EDL under confinement using a multimodal combination of scattering, spectroscopy, and surface forces measurements. Raman spectroscopy of bulk electrolytes suggests that the cation is closely associated with the anion regardless of valency. Wide-angle X-ray scattering reveals that all bulk electrolytes form ion clusters; however, the clusters are suppressed with increasing concentration of the divalent ion. To probe the EDL under confinement, we use a Surface Forces Apparatus and demonstrate that the thickness of the adsorbed layer of ions at the interface grows with increasing divalent ion concentration. Multiple interfacial layers form following this adlayer; their thicknesses appear dependent on anion size, rather than cation. Importantly, all electrolytes exhibit very long electrostatic decay lengths that are insensitive to valency. It is likely that in the WiSE regime, electrostatic screening is mediated by the formation of ion clusters rather than individual well-solvated ions. This work contributes to understanding the structure and charge-neutralization mechanism in this class of electrolytes and the interfacial behavior of mixed-electrolyte systems encountered in electrochemistry and biology.

Science & Technology - Other Topics↗