Nuclear Forensics-by-Design for Material Security: Research Strategies and Outcomes
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11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
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Results for “Molten salt reactors”
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High-Temperature Ferrofluids Based on Molten Salts
Molten metal chloride salts are promising candidates for advanced heat transfer fluids in generation IV nuclear reactors and beyond. However, research on the magnetic properties of suspended metallic nanoparticles at elevated temperatures is scarce, and there have been no attempts to develop a high-temperature, molten salt based ferrofluid. Such a ferrofluid would enable in situ manipulation of both the physical and thermal properties of the fluid via an external magnetic field. This study examines molten salt based ferrofluids comprised of metallic cobalt nanoparticles dispersed in molten metal chloride salts. High-temperature magnetometry and magneto-thermogalvometric measurements were conducted to evaluate the magnetic characteristics of the ferrofluid. Further analysis was conducted through a combination of microscopy, spectroscopy, solubility tests, and diffraction measurements. Furthermore, the metallic cobalt nanoparticles exhibited a notable degree of chemical stability and sustained magnetism from 25 to 800 °C when suspended in NaCl–MgCl 2 and KCl–ZnCl 2 mixtures.
Cobalt↗
Data-Driven RANS Turbulence Closures for Forced Convection Flow in Reactor Downcomer Geometry
Recent progress in data-driven turbulence modeling has shown its potential to enhance or replace traditional equation-based Reynolds-averaged Navier-Stokes (RANS) turbulence models. Here, this work utilizes invariant neural network (NN) architectures to model Reynolds stresses and turbulent heat fluxes in forced convection flows (when the models can be decoupled). As the considered flow is statistically one dimensional, the invariant NN architecture for the Reynolds stress model reduces to the linear eddy viscosity model. To develop the data-driven models, direct numerical and RANS simulations in vertical planar channel geometry mimicking a part of the reactor downcomer are performed. Different conditions and fluids relevant to advanced reactors (sodium, lead, unitary-Prandtl-number fluid, and molten salt) constitute the training database. The models enabled accurate predictions of velocity and temperature, and compared to the baseline k–τ turbulence model with the simple gradient diffusion hypothesis, do not require tuning of the turbulent Prandtl number. The data-driven framework is implemented in the open-source graphics processing unit–accelerated spectral element solver nekRS and has shown the potential for future developments and consideration of more complex mixed convection flows.
21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
Modeling and Experimental Verification of Thermal Energy Storage Systems to Enable Load Following Capability for Nuclear Reactors
NEUP Final Technical Report outlines experimental and modeling efforts to characterize performance of thermal energy storage systems with molten salt as the phase change material.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
Direct Measurement of Cl − Activity in Metal Chloride Molten Salts using a Cl 2 /Cl − Electrode
Molten metal chloride salts are promising candidates for advanced heat transfer fluids in generation IV nuclear reactors and beyond. The activity of the chloride ion in the salt has a large influence on the redox characteristics of the corresponding molten salt. There exists a knowledge gap for the direct measurement of chlorobasicity (Lewis basicity) in molten-salt mixtures. Here, the focus of this work was to develop a Cl 2 /Cl − electrode for the direct measurement of chloride activity in molten metal-chloride salt mixtures. The LiCl–KCl eutectic system was utilized as the reference melt to determine the change in chloride ion activity as increasing concentrations of MgCl 2 are added to the LiCl–KCl eutectic working electrode. The results of the measurements indicated a reduction in chloride ion activity as the concentration of magnesium chloride increased, consistent with the complexation of free chlorides by Lewis acidic magnesium cationic species. The Temkin model was used to estimate the thermodynamic properties of MgCl 4 2− complex.
Chloride↗
Complete Optimization of LPBF Ni-Based Alloys Down-Selected from FY23 Candidate Materials Including, Thermodynamic Modeling, Sample Fabrication and Microstructure Characterization
The goal of the Advanced Materials and Manufacturing Technologies (AMMT) program is to accelerate the incorporation of new materials and manufacturing technologies into advanced nuclear-related systems. Although 316H stainless steel fabricated by laser powder bed fusion (LPBF) has already been identified as an alloy that could have a significant effect on various reactor technologies, many other materials and manufacturing techniques are being evaluated. Nickel-based alloys typically offer higher-temperature capabilities compared with advanced stainless steels, and previous reports looked at three Ni-based alloy categories: low-Co alloys with a potential use close to the reactor core; high-temperature, high-strength alloys; and molten salt–compatible alloys. In the first category, alloy 718 was studied in 2023, and creep testing at 600°C and 650°C revealed that the alloy exhibited great creep strength after the appropriate annealing but had low ductility. Advanced characterization was recently conducted to highlight the presence of strengthening γ' and γ" precipitates after creep testing and to show that brittle phases at grain boundaries might explain the low ductility of LPBF 718 compared with wrought 718. For the high-temperature, high-strength alloys, previously purchased powders of alloys 617, 230, and 625 were used to assess the printability of these three solution-strengthened alloys. Hot cracking could not be suppressed for alloy 617 and 230, and it was shown that these cracks, which were elongated along the build direction (BD), had a drastic effect on the ductility of alloy 230 at room temperature when specimens were machined perpendicular to the BD. On the contrary, LPBF printing of crack-free alloy 625 was achieved using similar printing parameters, and the alloy looked like a promising candidate for various reactor technologies. The fabrication of alloy 282 by LPBF, a γ'-strengthened alloy with great creep strength up to 800°C, was performed in 2023, and x-ray computed tomography (XCT) scans of the alloy before and after creep testing at 750°C were carried out to assess the effect of flaws on the alloy’s creep behavior. Correlation between the flaws’ volume fraction, creep ductility, and creep lifetime could be established, and future work on LPBF 625 will take full advantage of in situ printing data and ex situ XCT scans to accelerate the alloy qualification. Finally, single track experiments were performed on the two alloys previously identified as good molten salt–resistant, Ni-based candidates: Hastelloy N and 244. Various laser parameters were considered, and cracking was not observed for either of the two alloys. Wrought 244 offers better creep strength and molten salt compatibility than alloy 625, and future work will aim to establish the alloy LPBF processing window.
36 MATERIALS SCIENCE↗
Ab initio Molecular Dynamics Assessment of Thermodynamic and Transport Properties in (K,Li)Cl and (K, Na)Cl Molten Salt Mixtures
Molten salt mixtures are integral part of highly important technological applications such as nuclear reactors. However, due to inherent difficulties associated with experiment at high temperatures and the intrinsic complexity of liquid-phase multi-component systems, understanding their properties at a molecular level remains a challenge. Here, we report on an ab initio molecular dynamics investigation on structural, electronic, transport, and thermal properties of two common molten salt mixtures, (K, Li)Cl and (K,Na)Cl, at five different compositions and three temperatures. Most of the properties were found to depend on both composition and temperature. While properties, like atomic charges, show additive behaviors, other properties, such as electrical conductivity, show considerable deviations from additivity. We shall show that the mixing of the molten salt mixtures is mainly driven by entropy, and that the KCl and LiCl mix better than KCl and NaCl. Our computational results are in general consistent with available experimental data. Comparison with available theoretical data is also provided.
Nguyen, Manh Thuong↗
Geometric Optimization of an Electrochemical Purification Cell to Prevent Corrosion in CSP Plants During Operation
When exposed to moisture or oxygen, molten chloride salts produce corrosive impurities which degrade containment alloys. As a result, this can significantly decrease the lifetime and increase costs of molten-salt-based systems. To overcome this barrier, we designed and modeled an electrochemical purification cell to remove the corrosive impurity MgOH+. Various reactor architectures, including constant stirred tank reactors (CSTRs) and plug flow reactors (PFRs) were investigated. Steady-state thermoelectric properties were evaluated, allowing assessment of the effects of structure and design parameters such as flow rate, cell length, and cross-sectional area of molten salt. The results suggest that our design could most effectively increase reliability and decrease costs of molten-chloride-salt-based systems by protecting them during continuous operation using an annular plug flow reactor.
chloride salts↗
Multi-Sourced Collaboration for the Production and Refining of Rare Elements and Critical Metals (Final Technical Report)
The project objective was to develop a feasible and cost-effective method for recovering rare earth elements (REEs) and critical materials (CMs) from coal and coal byproducts, resulting in high-purity individually separated REEs and CMs. The targeted REEs included Y, Pr, Nd, Gd, Dy, and Sm, with a purity of over 99.5%, while the CMs included Co, Mn, Ga, Sr, Li, Ni, Zn, and Ge, with a purity of over 90%. The project aimed to design a prototype facility capable of producing 1-3 tonnes/day of high-purity REO mixes. The work was divided into four designated circuits: 1) REE extraction and concentration, 2) REE separation and purification, 3) RE metal production, and 4) CM production. To achieve these goals, the project involved 11 tasks, including technology reviews, research, process flow diagram development, mass balance estimation, and preliminary technical-economic analysis. The project team included researchers from the University of Kentucky, University of Alabama and Virginia Tech as well as process specialists from Argonne National Laboratory. MP Materials provided technical support regarding rare earth markets and processing while Alliance Coal performed resource assessment. The project included a market analysis for Nd/Pr, Tb, Dy, Gd, Y, Co, Mn, Li, Sr, Ga, Ni, Zn, and Ge. These analyses provided insights into the supply and demand trends as well as historic and future projections of market price relative to purity requirements for these elements. Two coal resources were selected for the project: the West Kentucky No. 13 (Baker) Seam and an undisclosed lignite resource in the Illinois coal basin. The estimated quantities of REEs in these resources were calculated based on production samples and drilling data. It was estimated that there is adequate supply for an operation producing one metric ton daily of higher purity mixed rare earth oxides (MREO) for approximately 20 years at a site located in western Kentucky. In Circuit 1, project data was obtained from a pilot heap leach and REE concentration facility. It was concluded that the existing circuit, which generated a MREO concentrate, two types of CM mixed products, and Li- and Sr-containing waters, would be suitable feed for circuits 2-4. Data from the first-of-its-kind coal coarse refuse heap leach pilot pad played a crucial role in estimating reliable elemental concentrations of the pregnant leaching solution (PLS). The average total REE concentration in the PLS was found to be 28.6 ppm. In Circuit 2, several concepts were explored including a novel process referred to as solvent-assisted chromatography (SAC). This concept involved a novel columnar reactor that incorporated multiple mixer/settlers, thereby enabling the operation of counter-flowing aqueous and organic phases. Unfortunately, due to project time constraints, a complete fundamental modeling analysis could not be completed to fully evaluate the technology. Molten salt electrowinning was considered as an alternative for circuit 3 following circuit 2 purification circuit utilizing the novel SAC process. A mass and energy balance of Nd reduction to metal in a fluoride containing molten salt electrolyte was conducted. Comparisons were made with the current state of Asian molten salt electrorefining, and potential improvements in siphoning rare earth metals (REM) from the reactor were presented. A cost estimate was performed for the production of 1 tonne per day, which yielded a total of $2.29 million for the nine electrowinning (EW) cells required. The selected option for circuits 2 and 3 was a plasma distillation process, which initially separates rare earth elements (REEs) from other elements. This is followed by selective electrowinning in various ionic liquids. The selection was made on the basis of thermodynamic modeling and experimental data previously published by a project partner. The combination offers an innovative approach to integrated refining and RE metal production. For Circuit 4, an extensive literature review was conducted for the processing of the CMs. The ultimate decision was to utilize a combined plasma and ionic liquid process as well to produce individual high-purity concentrates of Zn, Ni, Co, Mn, and Mg. A separate flowsheet for Li and Sr was recommended, which would yield carbonates of these elements. Due to the lack of suitable experimental data at this time, a process recommendation could not be provided but several methods have been proposed for consideration. Lastly, a techno-economic analysis (TEA) was conducted to assess the effectiveness of the proposed process for further investigation. The TEA results revealed a capital expense (CapEx) of $737 million and an annual operational expense (OpEx) of $220 million. Due to the selected elements, the hypothetical heap leach pad can produce 1 metric tonne per day of REO equivalent, but a conscious decision was made to only treat targeted REEs, resulting in the production of 0.4 metric tonne of REM. An estimated annual revenue of $90.87 million was projected based on standard market pricing information provided by the funding agency. During the TEA, ten different modules were evaluated for costing purposes. The precipitation circuit was identified as the largest single operational expense, followed by the Mg/Mn process due to the amount of treated metal. In terms of capital expenditures, the heap leach process incurred the highest cost, followed by the Mg/Mn process. The scalability of the plasma process is a crucial consideration since the reactors cannot be scaled beyond the largest demonstrated size due to their reliance on surface area of the slag and vapor phase. The purity estimate for the REEs are generally 98%±2% to produce a metal. The purity level being lower than the project objective was due to the lack of specific experimental data needed to tighten the tolerance of the estimates. Based on literature and previous experience, the CMs are estimated as follows; Ga (95%+, metal), Sr (95%+, carbonate), Li (95%+, carbonate), Ni (98%±2%, metal), Zn (95%+, metal sponge), Ge (95%+, metal), Co (98%±2%, metal), and Mn (98%±2%, metal).
01 COAL, LIGNITE, AND PEAT↗
Evaluation of Directed Energy Deposition and Laser Powder Bed Fusion Nickel-Based Alloys Process Application Envelopes Based on Performance, Process Economics, Supply Chain Risks, and Reactor-Specific Targeted Components
The goal of the Advanced Materials and Manufacturing Technologies (AMMT) program is to accelerate the deployment of new materials and manufacturing technologies into advanced nuclear-related systems. Although 316H stainless steel fabricated by laser powder bed fusion (LPBF) has already been identified as an alloy that could have a significant effect on various reactor technologies, many other materials and manufacturing techniques are being evaluated. Nickel-based alloys typically offer higher-temperature capabilities compared with advanced stainless steels, and previous reports looked at three Ni-based alloy categories: low-Co alloys with a potential use close to the reactor core; high-temperature, high-strength alloys; and molten salt–compatible alloys. Due to the increasing interest in the low Co 625 alloy for nuclear applications, the alloy was compared at the Oak Ridge National Laboratory (ORNL) with 617, 230, two high-temperature, high-strength solution-strengthened alloys. Hot cracking could not be suppressed for alloy 230, and it was shown that these cracks, which were elongated along the build direction (BD), had a drastic effect on the ductility of alloy 230 at room temperature when specimens were machined perpendicular to the BD. Cracking was not as significant for alloy 617, but still led to significant variation in ductility at room temperature along the build direction. On the contrary, LPBF printing of crack-free alloy 625 was achieved using similar printing parameters, and the alloy looks like a very promising candidate for various reactor technologies.
36 MATERIALS SCIENCE↗
Versatile Cell Design for Molten Fluoride Salt Spectroscopy: Investigating Metal-Ion Speciation in Molten Fluoride Salts
Fluoride-based molten salts are widely used in industrial applications including aluminum production, thermal energy storage, optical crystal growth, and advanced nuclear reactor designs. Despite the wide range of uses, fundamental understandings of coordination chemistry and methods for probing molten fluorides are scarce, likely due to the difficulty of probing fluoride melts with spectroscopic techniques. Performing spectroscopic measurements of fluoride-based salts is challenging due to the highly corrosive nature of these salts, which can degrade many common optical materials. Here, in this work, we present a versatile optical cell design that enables spectroscopic measurements of corrosive melts. This innovative cell design overcomes the challenges posed by the corrosive nature of the salts, allowing for an accurate and consistent spectroscopic analysis. This work reports temperature-dependent absorption measurements for Co 2+ , Ni 2+ , and Cr 3+ analytes in LiF-NaF-KF eutectic salt (i.e., FLiNaK), which are common corrosion products originating from structural alloys in molten-fluoride handling. Absorption spectra were used to understand interactions of these analytes with FLiNaK, particularly ligand field coordination. The analysis of absorption spectra was complemented by structural analyses using ab initio molecular dynamics (AIMD) simulations, providing deeper insights into the behavior of the analytes in FLiNaK. Our findings indicate that the analytes studied in this work exist in octahedral or near-octahedral coordination states that remain stable across the temperature range of 500–600 °C. This work not only highlights an applied solution to performing optical spectroscopy in corrosive, high-temperature melts but also provides important fundamental insight on coordination behavior of transition-metal species in molten fluorides.
Fluoride salt spectroscopy↗
Computational and experimental analysis of structural and Thermophysical properties of LiX-KX (X = chloride, iodide, or bromide) molten salts
Molten salts containing lithium (Li) and potassium (K) halides, including chlorides (Cl), bromides (Br), and iodides (I), are pivotal in advanced technological applications including nuclear reactor technologies, thermal batteries, and industrial pyrochemical processes. Despite their significance, the availability of the temperature-dependent structural and thermophysical properties of these molten salts remain scarce. Here, this study addresses this knowledge gap by predicting and measuring the key properties such as coordination number, radial distribution function, density, heat capacity, and volumetric thermal expansion of molten LiI-KI, LiBr-KBr and LiCl-KCl eutectic mixtures. Utilizing ab initio molecular dynamics (AIMD) simulations, we predict these properties of LiX-KX (X=Br,I, Cl) across various temperatures, with chlorides as a benchmark. Experimental measurements using Archimedes methods and Differential Scanning Calorimetry validate the densities and heat capacities of these molten salts. Our comprehensive analysis of the structural and thermophysical properties provides critical insights into the behavior of these molten salts at various temperatures, enhancing the understanding necessary for their application in advanced technologies.
36 - MATERIALS SCIENCE↗
Need for research and training reactors for advanced reactor designs
Full text of publication follows. Research and training reactors have served a valuable role in helping train workforce for currently operating fleet of light water reactors. These research and training reactors have been used in reactor laboratory classes to familiarize the students with such vital concepts as approach to criticality, reactor period, neutron moderation, reactivity, flux distribution and leakage, etc. As the industry moves toward advanced non-light-water reactor designs, it is critical that research and training reactors be developed and deployed at university campuses to help train the new generation of nuclear and non-nuclear engineers who are likely to design, build, and operate these advanced reactors. Among the designs currently being pursued for nuclear power generation include molten salt, sodium cooled, and gas cooled designs, with options for various fuel forms. Thus, industry and DOE in collaboration with academic institutions should devise plans on how to familiarize the next generation of nuclear workforce with hands-on experience necessary for such designs. These research and training reactors will play a vital role in familiarizing the future workforce with hands-on experience with concepts associated with fast spectrum reactors, gas cooled reactors, and other features not associated with light water reactors. In addition to classical nuclear engineering concepts, these advanced research and training reactors can also be used for hands-on training as well as for research on features being considered in the design of GEN-IV reactors: cyber security for digital control room operations, hybrid energy system, hydrogen generation, district heating, autonomous control... (author)
21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
UF6 breeder reactor power plants for electric power generation
The reactor concept analyzed is a U-233F6 core surrounded by a molten salt (Li(7)F, BeF2, ThF4) blanket. Nuclear survey calculations were carried out for both spherical and cylindrical geometries. Thermodynamic cycle calculations were performed for a variety of Rankine cycles. A conceptual design is presented along with a system layout for a 1000 MW stationary power plant. Advantages of the gas core breeder reactor (GCBR) are as follows: (1) high efficiency; (2) simplified on-line reprocessing; (3) inherent safety considerations; (4) high breeding ratio; (5) possibility of burning all or most of the long-lived nuclear waste actinides; and (6) possibility of extrapolating the technology to higher temperatures and MHD direct conversion.
Rust, J. H.↗
Final Report
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21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
Assessment of RELAP5-3D Code with Molten Salt Heat Transfer Experiments
The accurate thermal-hydraulic assessment of thermal storage systems is crucial for addressing the integrity and performance of the storage system design. This is particularly important for thermal storage systems using molten salts as a heat transport and storage medium, as the chemical corrosion and erosion by the high-temperature molten salts can cause serious damage to the structural components of the storage system. To understand these effects for TerraPower’s Natrium® Demonstration Reactor design, the system thermal-hydraulic analysis code, RELAP5-3D, is utilized to analyze the thermal storage system. This study evaluates two heat transfer correlations implemented in the RELAP5-3D code—the Dittus-Boelter and Gnielinski correlations—using selected benchmark cases from two molten salt heat transfer experiments conducted at Xi’an Jiao Tong University and the German Aerospace Center. The Nusselt numbers calculated using the Gnielinski correlation agree with the experimental data within ±5% of the relative deviations at 300°C and 400°C. With the increasing Reynolds numbers, the Dittus-Boelter correlation underestimates the Nusselt numbers by up to 22% compared to the Gnielinski correlation. Comparison of the RELAP5-3D calculation results with experimental data at a high temperature of 550°C revealed that the thermo-chemical characteristics of solar salt at high temperatures surpassing the decomposition temperatures of nitrate salts reduce the accuracy of heat transfer model of the RELAP5-3D code. Specifically, it has been observed that the temperatures of the wall surface and liquid near the wall can surpass the decomposition temperatures, even though the bulk temperature of molten salts remains significantly lower than these decomposition temperatures. In summary, this study recommends the use of the Gnielinski correlation for the heat transfer analysis of molten salt, rather than the Dittus-Boelter correlation.
21 - SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLAN↗
SSR APPLIED – Automated Power Plants: Intelligent, Efficient and Digitised (V.2)
This report describes work undertaken during the SSR APPLIED project. The focus of the project has been on the development of digital twins to de-risk licensing of improved operating and maintenance practices. The operation of a bespoke flowing separate effects molten salt loop at ANL, with realistic temperature gradients, will provide invaluable data for computer codes validation. Three digital twins of aspects of the SSR-W have been successfully developed using ANL expertise and software. These digital twins have demonstrated optimization of the fuel cycle, the ability to model transients using an integrated coupled neutronic – thermal-hydraulic model with a model of the fuel expansion feedback so important to the inherent safety of the SSR-W. Advanced machine learning techniques have been developed and demonstrated for optimization of heat exchanger operation and maintenance.
21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
New High-Strength Ni-based Alloys for High Temperature Service in Liquid Fluoride Salt Environments
The ever-increasing demand for higher system thermal efficiency necessitates the operation of power generation cycles and heat conversion systems for chemical processes at progressively higher temperatures. As the system operating temperature increases, fewer and fewer materials are available with the required mechanical properties and environmental compatibility. This dearth of materials is particularly acute in structural applications at temperatures above 700°C in liquid Fluoride Salt Cooled High-Temperature Reactors (FHRs) and Concentrated Solar Power (CSP) systems where liquid fluoride and/or liquid chloride salts are used for their high thermal capacity and low thermal conductivity to store and transport heat. It has been shown that fluorides and chlorides can degrade the properties of the material used for storage and transport due to corrosive effects thus affecting the performance and lifetime characteristics. Thus, materials used for storage and transport for fluoride/chloride-salt must at the minimum have good compatibility with the salt by exhibiting low corrosion rates at the required temperatures. In addition, since many of the components will be subject to stresses in service, they need to have sufficient strength to resist plastic deformation, and the resistance to time dependent creep deformation at these temperatures, and stress levels. Achieving the combination of these properties required for higher temperatures is particularly challenging considering traditionally, the expected lifetime of some of the components used in these systems are from 30 years (CSP) to 80 years (FHRs). Although 316 stainless steel and associated redox corrosion reduction techniques are being considered for use in the first generational systems, use of 316SS is limited to operating temperatures up to ~ 650°C, thereby resulting in lower reactor efficiencies. Hastelloy ® N, developed at ORNL in the 1950s-60s for molten salt service is currently the leading candidate FHR structural alloy but has inadequate creep properties at high temperatures. Using a computationally-guided approach, Oak Ridge National Laboratory had developed new high strength alloys strengthened by γ’ precipitates (about 2X the strength of Hastelloy ® N) in small laboratory-scale heats that show good resistance to corrosion by fluorides and improved creep rupture life at temperatures up to 850°C (U.S. Patent Application No. 13/833,357 entitled “High Strength Alloys for High Temperature Service in Liquid-Salt Cooled Energy Systems”- granted U. S. Patent No. 9,540,714).
22 GENERAL STUDIES OF NUCLEAR REACTORS↗